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Cytotoxicity Studies of Cyclometallated Ruthenium(II) Compounds: New Applications for Ruthenium Dyes

2176 Organometallics 2010, 29, 2176–2179 DOI: 10.1021/om100106e NMR Chemical Shifts of Trace Impurities: Common Laboratory Solvents, Organics, and Gases in Deuterated Solvents Relevant to the Organometallic Chemist Gregory R. Fulmer,*,† Alexander J. M. Miller,‡ Nathaniel H. Sherden,‡ Hugo E. Gottlieb,§ Abraham Nudelman,§ Brian M. Stoltz,‡ John E. Bercaw,‡ and Karen I. Goldberg† Department of Chemistry, University of Washington, Box 351700, Seattle, Washington 98195-1700, Arnold and Mabel Beckman Laboratories of Chemical Synthesis and Caltech Center for Catalysis and Chemical Synthesis, Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, and §Department of Chemistry, Bar Ilan University, Ramat Gan 52900, Israel † ‡ Received February 11, 2010 Tables of 1H and 13C NMR chemical shifts have been compiled for common organic compounds often used as reagents or found as products or contaminants in deuterated organic solvents. Building upon the work of Gottlieb, Kotlyar, and Nudelman in the Journal of Organic Chemistry, signals for common impurities are now reported in additional NMR solvents (tetrahydrofuran-d8, toluene-d8, dichloromethane-d2, chlorobenzene-d5, and 2,2,2-trifluoroethanol-d3) which are frequently used in organometallic laboratories. Chemical shifts for other organics which are often used as reagents or internal standards or are found as products in organometallic chemistry are also reported for all the listed solvents. Hanging above the desk of most every chemist whose work relies heavily on using NMR spectroscopy1 is NMR Chemical Shifts of Common Laboratory Solvents as Trace Impurities by Gottlieb, Kotlyar, and Nudelman.2 By compiling the chemical shifts of a large number of contaminants commonly encountered in synthetic chemistry, the publication has become an essential reference, allowing for easy identification of known impurities in a variety of deuterated organic solvents. However, despite the utility of Gottlieb et al.’s work,3 the chemical shifts of impurities in a number of NMR solvents often used by organometallic chemists were not included. Tetrahydrofuran-d8 (THF-d8), toluene-d8, dichloromethane-d2 (CD2Cl2), chlorobenzene-d5 (C6D5Cl), and 2,2,2-trifluoroethanol-d3 (TFE-d3) are commonplace in laboratories practicing inorganic syntheses. Therefore, we have expanded the spectral data compilation with the inclusion of chemical shifts of common impurities recorded in the deuterated solvents heavily employed in our organometallic laboratories. The chemical shifts of various gases (hydrogen, methane, ethane, propane, *To whom correspondence should be addressed. E-mail: fulmerg@ u.washington.edu. (1) For general information on 1H and 13C{1H} NMR spectroscopy, see: Balcı, M. Basic 1H- and 13C-NMR Spectroscopy; Elsevier: Amsterdam, 2005. (2) Gottlieb, H. E.; Kotlyar, V.; Nudelman, A. J. Org. Chem. 1997, 62, 7512. (3) According to ACS Publications as of December 2009 (http://pubs. acs.org/), Gottlieb et al.’s publication2 is the most downloaded Journal of Organic Chemistry article over the preceding 12 months. pubs.acs.org/Organometallics Published on Web 04/16/2010 ethylene, propylene, and carbon dioxide) often encountered as reagents or products in organometallic reactions, along with organic compounds relevant to organometallic chemists (allyl acetate, benzaldehyde, carbon disulfide, carbon tetrachloride, 18-crown-6, cyclohexanone, diallyl carbonate, dimethyl carbonate, dimethyl malonate, furan, Apiezon H grease, hexamethylbenzene, hexamethyldisiloxane, imidazole, pyrrole, and pyrrolidine), have also been added to this expanded list. Experimental Section All deuterated solvents were obtained commercially through Cambridge Isotope Laboratories, Inc. NMR spectra were recorded at 298 K using 300, 500, or 600 MHz spectrometers (13C{1H} NMR frequencies of 75.5, 126, or 151 MHz, respectively). Adopting the previously reported strategy,2 standard solutions of mixtures of specific impurities were used to reduce the number of necessary individual NMR experiments. The combinations of organic compounds were chosen in a way in which intermolecular interactions and resonance convolution would be minimized. Unless otherwise stated, the standard solutions were prepared with qualitatively equal molar amounts of the following compounds: (solution 1) acetone, dimethylformamide, ethanol, toluene; (solution 2) benzene, dimethyl sulfoxide, ethyl acetate, methanol; (solution 3) acetic acid, chloroform, diethyl ether, 2-propanol, tetrahydrofuran; (solution 4) acetonitrile, dichloromethane, 1,4-dioxane, n-hexane, hexamethylphosphoramide (HMPA); (solution 5) 1,2-dichloroethane, n-pentane, pyridine, hexamethylbenzene; (solution 6) tert-butyl alcohol, 2,6-di-tert-butyl-4-methylphenol (BHT), cyclohexane, r 2010 American Chemical Society Article Organometallics, Vol. 29, No. 9, 2010 2177 Table 1. 1H NMR Dataa proton solvent residual signals mult THF-d8 CD2Cl2 CDCl3 toluene-d8 C6D6 1.72 3.58 5.32 7.26 2.08 6.97 7.01 7.09 7.16 C6D5Cl (CD3)2CO (CD3)2SO CD3CN 6.96 6.99 7.14 2.05 2.50 1.94 TFE-d3 5.02 3.88 CD3OD D2O 3.31 4.79 OH s 2.46 1.52 1.56 0.43 0.40 1.03 2.84b 3.33b 2.13 3.66 4.87 CH3 s 1.89 2.06 2.10 1.57 1.52 1.76 1.96 1.91 1.96 2.06 1.99 2.08 s 2.05 2.12 2.17 1.57 1.55 1.77 2.09 2.09 2.08 2.19 2.15 2.22 CH3 s 1.95 1.97 2.10 0.69 0.58 1.21 2.05 2.07 1.96 1.95 2.03 2.06 CH3 CH s 7.31 7.35 7.36 7.12 7.15 7.20 7.36 7.37 7.37 7.36 7.33 s 1.15 1.24 1.28 1.03 1.05 1.12 1.18 1.11 1.16 1.28 1.40 1.24 CH3 OH sc 3.16 0.58 0.63 1.30 4.19 2.18 2.20 chloroform CH s 7.89 7.32 7.26 6.10 6.15 6.74 8.02 8.32 7.58 7.33 7.90 18-crown-6 CH2 s 3.57 3.59 3.67 3.36 3.39 3.41 3.59 3.51 3.51 3.64 3.64 3.80 s 1.44 1.44 1.43 1.40 1.40 1.37 1.43 1.40 1.44 1.47 1.45 cyclohexane CH2 1,2-dichloroethane CH2 s 3.77 3.76 3.73 2.91 2.90 3.26 3.87 3.90 3.81 3.71 3.78 s 5.51 5.33 5.30 4.32 4.27 4.77 5.63 5.76 5.44 5.24 5.49 dichloromethane CH2 diethyl ether CH3 t, 7 1.12 1.15 1.21 1.10 1.11 1.10 1.11 1.09 1.12 1.20 1.18 1.17 CH2 q, 7 3.38 3.43 3.48 3.25 3.26 3.31 3.41 3.38 3.42 3.58 3.49 3.56 m 3.43 3.57 3.65 3.43 3.46 3.49 3.56 3.51 3.53 3.67 3.61 3.67 diglyme CH2 CH2 m 3.53 3.50 3.57 3.31 3.34 3.37 3.47 3.38 3.45 3.62 3.58 3.61 s 3.28 3.33 3.39 3.12 3.11 3.16 3.28 3.24 3.29 3.41 3.35 3.37 OCH3 dimethylformamide CH s 7.91 7.96 8.02 7.57 7.63 7.73 7.96 7.95 7.92 7.86 7.97 7.92 CH3 s 2.88 2.91 2.96 2.37 2.36 2.51 2.94 2.89 2.89 2.98 2.99 3.01 CH3 s 2.76 2.82 2.88 1.96 1.86 2.30 2.78 2.73 2.77 2.88 2.86 2.85 s 3.56 3.65 3.71 3.33 3.35 3.45 3.59 3.57 3.60 3.76 3.66 3.75 1,4-dioxane CH2 DME CH3 s 3.28 3.34 3.40 3.12 3.12 3.17 3.28 3.24 3.28 3.40 3.35 3.37 CH2 s 3.43 3.49 3.55 3.31 3.33 3.37 3.46 3.43 3.45 3.61 3.52 3.60 s 0.85 0.85 0.87 0.81 0.80 0.79 0.83 0.82 0.85 0.85 0.85 0.82 ethane CH3 ethanol CH3 t, 7 1.10 1.19 1.25 0.97 0.96 1.06 1.12 1.06 1.12 1.22 1.19 1.17 d q, 7 3.51 3.66 3.72 3.36 3.34 3.51 3.57 3.44 3.54 3.71 3.60 3.65 CH2 c,d OH s 3.30 1.33 1.32 0.83 0.50 1.39 3.39 4.63 2.47 s 1.94 2.00 2.05 1.69 1.65 1.78 1.97 1.99 1.97 2.03 2.01 2.07 ethyl acetate CH3CO CH2CH3 q, 7 4.04 4.08 4.12 3.87 3.89 3.96 4.05 4.03 4.06 4.14 4.09 4.14 CH2CH3 t, 7 1.19 1.23 1.26 0.94 0.92 1.04 1.20 1.17 1.20 1.26 1.24 1.24 s 5.36 5.40 5.40 5.25 5.25 5.29 5.38 5.41 5.41 5.40 5.39 5.44 ethylene CH2 e ethylene glycol CH2 s 3.48 3.66 3.76 3.36 3.41 3.58 3.28 3.34 3.51 3.72 3.59 3.65 CH3 m 0.85-0.91 0.84-0.90 0.84-0.87 0.89-0.96 0.90-0.98 0.86-0.92 0.90 0.82-0.88 0.88-0.94 0.86-0.93 H greasef CH2 br s 1.29 1.27 1.25 1.33 1.32 1.30 1.29 1.24 1.33 1.29 s 2.18 2.20 2.24 2.10 2.13 2.10 2.17 2.14 2.19 2.24 2.19 hexamethylbenzene CH3 n-hexane CH3 t, 7 0.89 0.89 0.88 0.88 0.89 0.85 0.88 0.86 0.89 0.91 0.90 CH2 m 1.29 1.27 1.26 1.22 1.24 1.19 1.28 1.25 1.28 1.31 1.29 s 0.07 0.07 0.07 0.10 0.12 0.10 0.07 0.06 0.07 0.08 0.07 0.28 HMDSO CH3 HMPA CH3 d,9.5 2.58 2.60 2.65 2.42 2.40 2.47 2.59 2.53 2.57 2.63 2.64 2.61 s 4.55 4.59 4.62 4.50 4.47 4.49 4.54 4.61 4.57 4.53 4.56 hydrogen H2 imidazole CH(2) s 7.48 7.63 7.67 7.30 7.33 7.53 7.62 7.63 7.57 7.61 7.67 7.78 CH(4,5) s 6.94 7.07 7.10 6.86 6.90 7.01 7.04 7.01 7.01 7.03 7.05 7.14 methane CH4 s 0.19 0.21 0.22 0.17 0.16 0.15 0.17 0.20 0.20 0.18 0.20 0.18 sg 3.27 3.42 3.49 3.03 3.07 3.25 3.31 3.16 3.28 3.44 3.34 3.34 methanol CH3 c,g OH s 3.02 1.09 1.09 1.30 3.12 4.01 2.16 nitromethane CH3 s 4.31 4.31 4.33 3.01 2.94 3.59 4.43 4.42 4.31 4.28 4.34 4.40 t, 7 0.89 0.89 0.88 0.87 0.87 0.84 0.88 0.86 0.89 0.90 0.90 n-pentane CH3 CH2 m 1.31 1.30 1.27 1.25 1.23 1.23 1.27 1.27 1.29 1.33 1.29 t, 7.3 0.90 0.90 0.90 0.89 0.86 0.84 0.88 0.87 0.90 0.90 0.91 0.88 propane CH3 CH2 sept, 7.3 1.33 1.32 1.32 1.32 1.26 1.26 1.31 1.29 1.33 1.33 1.34 1.30 d, 6 1.08 1.17 1.22 0.95 0.95 1.04 1.10 1.04 1.09 1.20 1.50 1.17 2-propanol CH3 CH sept, 6 3.82 3.97 4.04 3.65 3.67 3.82 3.90 3.78 3.87 4.05 3.92 4.02 propylene CH3 dt, 6.4, 1.5 1.69 1.71 1.73 1.55 1.55 1.58 1.68 1.68 1.70 1.70 1.70 1.70 dm, 10 4.89 4.93 4.94 4.92 4.95 4.91 4.90 4.94 4.93 4.93 4.91 4.95 CH2(1) CH2(2) dm, 17 4.99 5.03 5.03 4.98 5.01 4.98 5.00 5.03 5.04 5.03 5.01 5.06 CH m 5.79 5.84 5.83 5.70 5.72 5.72 5.81 5.80 5.85 5.87 5.82 5.90 pyridine CH(2,6) m 8.54 8.59 8.62 8.47 8.53 8.51 8.58 8.58 8.57 8.45 8.53 8.52 CH(3,5) m 7.25 7.28 7.29 6.67 6.66 6.90 7.35 7.39 7.33 7.40 7.44 7.45 CH(4) m 7.65 7.68 7.68 6.99 6.98 7.25 7.76 7.79 7.73 7.82 7.85 7.87 pyrrole NH br t 9.96 8.69 8.40 7.71 7.80 8.61 10.02 10.75 9.27 CH(2,5) m 6.66 6.79 6.83 6.43 6.48 6.62 6.77 6.73 6.75 6.84 6.72 6.93 CH(3,4) m 6.02 6.19 6.26 6.27 6.37 6.27 6.07 6.01 6.10 6.24 6.08 6.26 h pyrrolidine CH2(2,5) m 2.75 2.82 2.87 2.54 2.54 2.64 2.67 2.75 3.11 2.80 3.07 CH2(3,4) m 1.59 1.67 1.68 1.36 1.33 1.43 1.55 1.61 1.93 1.72 1.87 s 0.11 0.09 0.07 0.26 0.29 0.14 0.13 -0.06 0.08 0.16 0.10 silicone grease CH3 tetrahydrofuran CH2(2,5) m 3.62 3.69 3.76 3.54 3.57 3.59 3.63 3.60 3.64 3.78 3.71 3.74 m 1.79 1.82 1.85 1.43 1.40 1.55 1.79 1.76 1.80 1.91 1.87 1.88 CH2(3,4) toluene CH3 s 2.31 2.34 2.36 2.11 2.11 2.16 2.32 2.30 2.33 2.33 2.32 CH(2,4,6) m 7.10 7.15 7.17 6.96-7.01 7.02 7.01-7.08 7.10-7.20 7.18 7.10-7.30 7.10-7.30 7.16 CH(3,5) m 7.19 7.24 7.25 7.09 7.13 7.10-7.17 7.10-7.20 7.25 7.10-7.30 7.10-7.30 7.16 triethylamine CH3 t, 7 0.97 0.99 1.03 0.95 0.96 0.93 0.96 0.93 0.96 1.31 1.05 0.99 q,7 2.46 2.48 2.53 2.39 2.40 2.39 2.45 2.43 2.45 3.12 2.58 2.57 CH2 water acetic acid acetone acetonitrile benzene tert -butyl alcohol a Except for the compounds in solutions 8-10, as well as the gas samples, hexamethylbenzene, and the corrected values mentioned in the Supporting Information, all data for the solvents CDCl3, C6D6, (CD3)2CO, (CD3)2SO, CD3CN, CD3OD, and D2O were previously reported in ref 2. b A signal for HDO is also observed in (CD3)2SO (3.30 ppm) and (CD3)2CO (2.81 ppm), often seen as a 1:1:1 triplet (2JH,D = 1 Hz). c Not all OH signals were observable. d In some solvents, the coupling interaction between the CH2 and the OH protons may be observed (J = 5 Hz). e In CD3CN, the OH proton was seen as a multiplet at 2.69 ppm, as well as extra coupling to the CH2 resonance. f Apiezon brand H grease. g In some solvents, a coupling interaction between the CH3 and the OH protons may be observed (J = 5.5 Hz). h Pyrrolidine was observed to react with (CD3)2CO. 2178 Organometallics, Vol. 29, No. 9, 2010 Fulmer et al. Table 2. 13C{1H} NMR Dataa carbon solvent signals acetic acid acetone acetonitrile benzene tert -butyl alcohol carbon dioxide carbon disulfide carbon tetrachloride chloroform 18-crown-6 cyclohexane 1,2-dichloroethane dichloromethane diethyl ether diglyme dimethylformamide 1,4-dioxane DME ethane ethanol ethyl acetate ethylene ethylene glycol H greaseb hexamethylbenzene n-hexane HMDSO HMPAc imidazole methane methanol nitromethane n-pentane propane 2-propanol propylene pyridine pyrrole pyrrolidinee silicone grease tetrahydrofuran toluene triethylamine CO CH3 CO CH3 CN CH3 CH (CH3)3C (CH3)3C CO2 CS2 CCl4 CH CH2 CH2 CH2 CH2 CH3 CH2 CH3 CH2 CH2 CH CH3 CH3 CH2 CH3 CH2 CH3 CH3 CH2 CH3CO CO CH2 CH3 CH2 CH2 CH2 C CH3 CH3 CH2(2,5) CH2(3,4) CH3 CH3 CH(2) CH(4,5) CH4 CH3 CH3 CH3 CH2(2,4) CH2(3) CH3 CH2 CH3 CH CH3 CH2 CH CH(2,6) CH(3,5) CH(4) CH(2,5) CH(3,4) CH2(2,5) CH2(3,4) CH3 CH2(2,5) CH2(3,4) CH3 C(1) CH(2,6) CH(3,5) CH(4) CH3 CH2 THF-d8 CD2Cl2 CDCl3 toluene- d8 C6D6 C6D5Cl (CD3)2CO (CD3)2SO CD3CN TFE-d3 CD3OD 67.21 25.31 53.84 77.16 137.48 128.87 127.96 125.13 20.43 128.06 134.19 129.26 128.25 125.96 29.84 206.26 39.52 1.32 118.26 61.50 126.28 49.00 171.69 20.13 204.19 30.17 116.79 0.45 128.84 67.50 30.57 125.69 193.37 96.89 79.24 71.34 27.58 44.64 54.67 15.49 66.14 58.72 71.17 72.72 161.96 35.65 30.70 67.65 58.72 72.58 6.79 18.90 57.60 20.45 170.32 60.30 14.37 123.09 64.35 30.45 131.88 16.71 14.22 23.33 32.34 1.83 36.89 135.72 122.20 -4.90 49.64 62.49 14.18 23.00 34.87 16.60 16.82 25.70 66.14 19.27 115.74 134.02 150.57 124.08 135.99 118.03 107.74 45.82 26.17 1.20 68.03 26.19 21.29 138.24 129.47 128.71 125.84 12.51 47.18 175.85 20.91 206.78 31.00 116.92 2.03 128.68 69.11 31.46 125.26 192.95 96.52 77.99 70.47 27.38 44.35 54.24 15.44 66.11 58.95 70.70 72.25 162.57 36.56 31.39 67.47 59.02 72.24 6.91 18.69 58.57 21.15 171.24 60.63 14.37 123.20 64.08 30.14 132.09 16.93 14.28 23.07 32.01 1.96 36.99 135.76 122.16 -4.33 50.45 63.03 14.24 22.77 34.57 16.63 16.63 25.43 64.67 19.47 115.70 134.21 150.27 124.06 136.16 117.93 108.02 47.02 25.83 1.22 68.16 25.98 21.53 138.36 129.35 128.54 125.62 12.12 46.75 175.99 20.81 207.07 30.92 116.43 1.89 128.37 69.15 31.25 124.99 192.83 96.34 77.36 70.55 26.94 43.50 53.52 15.20 65.91 59.01 70.51 71.90 162.62 36.50 31.45 67.14 59.08 71.84 6.89 18.41 58.28 21.04 171.36 60.49 14.19 123.13 63.79 29.71 132.21 16.98 14.14 22.70 31.64 1.97 36.87 135.38 122.00 -4.63 50.41 62.50 14.08 22.38 34.16 16.63 16.37 25.14 64.50 19.50 115.74 133.91 149.90 123.75 135.96 117.77 107.98 46.93 25.56 1.19 67.97 25.62 21.46 137.89 129.07 128.26 125.33 11.61 46.25 175.30 20.27 204.00 30.03 115.76 0.03 128.57 68.12 30.49 124.86 192.71 96.57 77.89 70.86 27.31 43.40 53.47 15.47 65.94 58.62 70.92 72.39 161.93 35.22 30.64 67.17 58.63 72.25 6.94 18.78 57.81 20.46 170.02 60.08 14.23 122.92 64.29 30.31 131.72 16.84 14.34 23.12 32.06 1.99 36.80 135.57 122.13 -4.34 49.90 61.14 14.27 22.79 34.54 16.65 16.63 25.24 64.12 19.32 115.89 133.61 150.25 123.46 135.17 117.61 108.15 47.12 25.75 1.37 67.75 25.79 21.37 137.84 129.33 128.51 125.66 12.39 46.82 175.82 20.37 204.43 30.14 116.02 0.20 128.62 68.19 30.47 124.76 192.69 96.44 77.79 70.59 27.23 43.59 53.46 15.46 65.94 58.66 70.87 72.35 162.13 35.25 30.72 67.16 58.68 72.21 6.96 18.72 57.86 20.56 170.44 60.21 14.19 122.96 64.34 30.22 131.79 16.95 14.32 23.04 31.96 2.05 36.88 135.76 122.16 -4.29 49.97 61.16 14.25 22.72 34.45 16.66 16.60 25.18 64.23 19.38 115.92 133.69 150.27 123.58 135.28 117.78 108.21 46.86 25.65 1.38 67.80 25.72 21.10 137.91 129.33 128.56 125.68 12.35 46.77 175.67 20.40 204.83 30.12 115.93 0.63 128.38 68.19 31.13 126.08 192.49 96.38 77.67 70.55 26.99 43.60 53.54 15.35 65.79 58.42 70.56 72.07 162.01 35.45 30.71 66.95 58.31 71.81 6.91 18.55 57.63 20.50 170.20 60.06 14.07 122.95 64.03 30.11 131.54 16.68 14.18 22.86 31.77 1.92 36.64 135.50 121.96 -4.33 49.66 61.68 14.10 22.54 34.26 16.56 16.48 25.14 64.18 19.32 115.86 133.57 149.93 123.49 135.32 117.65 108.03 46.75 25.59 1.09 67.64 25.68 21.23 137.65 129.12 128.31 125.43 11.87 46.36 172.31 20.51 205.87 30.60 117.60 1.12 129.15 68.13 30.72 125.81 193.58 96.65 79.19 71.25 27.51 45.25 54.95 15.78 66.12 58.77 71.03 72.63 162.79 36.15 31.03 67.60 58.45 72.47 6.88 18.89 57.72 20.83 170.96 60.56 14.50 123.47 64.26 171.93 20.95 206.31 30.56 117.91 1.03 128.30 66.88 30.38 124.21 192.63 95.44 79.16 69.85 26.33 45.02 54.84 15.12 62.05 57.98 69.54 71.25 162.29 35.73 30.73 66.36 58.03 71.17 6.61 18.51 56.07 20.68 170.31 59.74 14.40 123.52 62.76 173.21 20.73 207.43 30.91 118.26 1.79 129.32 68.74 30.68 125.89 193.60 96.68 79.17 71.22 27.63 45.54 55.32 15.63 66.32 58.90 70.99 72.63 163.31 36.57 31.32 67.72 58.89 72.47 6.99 18.80 57.96 21.16 171.68 60.98 14.54 123.69 64.22 177.96 20.91 32.35 214.98 118.95 1.00 129.84 72.35 31.07 126.92 196.26 97.74 78.83 70.80 28.34 45.28 54.46 15.33 67.55 59.40 73.05 71.33 166.01 37.76 30.96 68.52 59.52 72.87 7.01 18.11 59.68 21.18 175.55 62.70 14.36 124.08 64.87 175.11 20.56 209.67 30.67 118.06 0.85 129.34 69.40 30.91 126.31 193.82 97.21 79.44 71.47 27.96 45.11 54.78 15.46 66.88 59.06 71.33 72.92 164.73 36.89 31.61 68.11 59.06 72.72 6.98 18.40 58.26 20.88 172.89 61.50 14.49 123.46 64.30 132.22 16.86 14.34 23.28 32.30 2.01 37.04 135.89 122.31 -5.33 49.77 63.21 14.29 22.98 34.83 16.68 16.78 25.67 63.85 19.42 116.03 134.34 150.67 124.57 136.56 117.98 108.04 131.10 16.60 13.88 22.05 30.95 1.96 36.42 135.15 121.55 -4.01 48.59 63.28 13.28 21.70 33.48 16.34 15.67 25.43 64.92 19.20 116.07 133.55 149.58 123.84 136.05 117.32 107.07 46.51 25.26 132.61 16.94 14.43 23.40 32.36 2.07 37.10 136.33 122.78 -4.61 49.90 63.66 14.37 23.08 34.89 16.73 16.91 25.55 64.30 19.48 116.12 134.78 150.76 127.76 136.89 118.47 108.31 47.57 26.34 67.03 25.14 20.99 137.35 128.88 128.18 125.29 11.74 45.74 68.33 26.27 21.50 138.90 129.94 129.23 126.28 12.38 47.10 134.04 17.04 14.63 24.06 33.17 2.09 37.21 136.58 122.93 -5.88 50.67 63.17 14.54 23.75 35.76 16.93 17.46 25.21 66.69 19.63 116.38 136.00 149.76 126.27 139.62 119.61 108.85 47.43 25.73 2.87 69.53 26.69 21.62 139.92 130.58 129.79 126.82 9.51 48.45 132.53 16.90 14.45 23.68 32.73 1.99 37.00 136.31 122.60 -4.90 49.86 63.08 14.39 23.38 35.30 16.80 17.19 25.27 64.71 19.50 116.04 134.61 150.07 125.53 138.35 118.28 108.11 47.23 26.29 2.10 68.83 26.48 21.50 138.85 129.91 129.20 126.29 11.09 46.96 1.40 68.07 26.15 21.46 138.48 129.76 129.03 126.12 12.49 47.07 D2O 177.21 21.03 215.94 30.89 119.68 1.47 70.36 30.29 197.25 96.73 70.14 14.77 66.42 58.67 70.05 71.63 165.53 37.54 32.03 67.19 58.67 71.49 17.47 58.05 21.15 175.26 62.32 13.92 63.17 2.31 36.46 136.65 122.43 49.50d 63.22 24.38 64.88 149.18 125.12 138.27 119.06 107.83 46.83 25.86 68.68 25.67 9.07 47.19 a Except for the compounds in solutions 8-10, as well as the gas samples, hexamethylbenzene, and the corrected values mentioned in the Supporting Information, all data for the solvents CDCl3, C6D6, (CD3)2CO, (CD3)2SO, CD3CN, CD3OD, and D2O were previously reported in ref 2. b Apiezon brand H grease. c Phosphorus coupling was observed (2JPC = 3 Hz). d Internal reference; see text. e Pyrrolidine was observed to react with (CD3)2CO. Article 1,2-dimethoxyethane (DME), nitromethane, poly(dimethylsiloxane) (silicone grease), triethylamine; (solution 7) diglyme, dimethylacetamide, ethylene glycol, ethyl methyl ketone; (solution 8) allyl acetate, 2,6-di-tert-butyl-4-methoxyphenol (BHA), longchain, linear aliphatic hydrocarbons from pump oil;4 (solution 9) benzaldehyde, carbon disulfide, carbon tetrachloride, cyclohexanone, dimethyl malonate, furan, Apiezon H grease (H grease); (solution 10) 18-crown-6, diallyl carbonate, dimethyl carbonate, hexamethyldisiloxane (HMDSO), imidazole, pyrrole, pyrrolidine.5 In the case of TFE-d3, nitromethane was omitted from solution 6 and run separately, since the protons of nitromethane exchange with deuterium from TFE-d3 in the presence of triethylamine. In the case of (CD3)2CO, pyrrolidine was omitted from solution 10, since the two compounds were observed to react with each other. The gases used in this study included hydrogen, methane, ethane, propane, ethylene, propylene, and carbon dioxide. Before examining the various standard contaminant solutions by 1H NMR spectroscopy, solvent residual signals6 and chemical shifts for H2O7 for each NMR solvent were referenced against tetramethylsilane (TMS, δ 0 ppm) and reported. Before collecting 13C{1H} NMR spectral data, solvent signals6 were recorded with reference to the signal of a TMS internal standard. For D2O, 1H NMR spectra were referenced to the methyl signal (δ 0 ppm) of sodium 3-(trimethylsilyl)propanesulfonate,8,9 and 13C{1H} NMR spectra were referenced to the signal for the methyl group of methanol (one drop, added as an internal standard), which was set to 49.50 ppm.2 In a typical experiment for collecting 1H NMR spectral data, a 3 μL sample of a standard contaminant solution was added to an NMR tube containing approximately 0.4 mL of a deuterated solvent. For 13C{1H} NMR spectral data collection, an approximately 50 μL sample of the standard contaminant solution was added. When there was any uncertainty in the assignment of a resonance, the solution was spiked with an additional 1-2 μL of the impurity in question to accurately identify its chemical shift. In cases where the chemical shifts of resonances were highly dependent on the concentration of the impurities present, ambiguous resonances were instead resolved via gradient(4) VWR brand vacuum pump oil #19. (5) The components of solution 10 were stable together in dilute solution but unstable when neat mixtures were prepared. In general, it was observed that the nitrogen-containing compounds and possibly 18-crown-6 catalyzed the hydrolysis of the carbonates, reacted directly with them, or both. Therefore, for the purpose of storage, the solution was partitioned into two subsolutions: (solution 10A) 18-crown-6, imidazole, pyrrole, pyrrolidine; (solution 10B) diallyl carbonate, dimethyl carbonate, hexamethyldisiloxane. These subsolutions were stable for long periods as neat mixtures and were combined to form solution 10 by adding equal portions to an NMR tube containing the desired deuterated solvent. (6) For 1H NMR spectra, the solvent residual signals arise from the proton of isotopomers containing one less deuterium atom than the perdeuterated solvent: e.g., CDHCl2 in CD2Cl2. For 13C NMR spectra, the solvent signals arise from the 13C atoms at natural abundance in the perdeuterated solvent. (7) The chemical shift for H2O can vary depending on the temperature, [H2O], and the solutes present: e.g., a downfield shift may be observed in the presence of any hydrogen bond acceptors. For more information see page 75 of ref 1. (8) Harris, R. K.; Becker, E. D.; Cabral de Menezes, S. M.; Granger, P.; Hoffman, R. E.; Zilm, K. W. Pure Appl. Chem. 2008, 80, 59. (9) For information on the temperature dependence of HDO chemical shifts in D2O, see ref 2. Organometallics, Vol. 29, No. 9, 2010 2179 selected heteronuclear single-quantum coherence (gs-HSQC) and gradient-selected heteronuclear multiple-quantum coherence (gs-HMQC) NMR spectroscopies. For the experiments involving gases, a J. Young NMR tube containing approximately 0.4 mL of NMR solvent was first degassed with three freeze-pump-thaw cycles. Using a vacuum line equipped with a gas manifold, 1 atm of the desired gas was added to the tube. Each gas was run separately, degassing between each gas sample. Results and Discussion Chemical shifts for each of the impurities are reported in the tables: 1H and 13C{1H} NMR spectral data of all substrates are presented in Tables 1 and 2, respectively. Notably, physically larger tables, containing all the data from Tables 1 and 2 as well as the chemical shifts of additional organic compounds, are provided in the Supporting Information. Unless noted otherwise, coupling constants (reported in Hz) and resonance multiplicities (abbreviated as follows: s = singlet, d = doublet, t = triplet, q = quartet, p = pentet, sept = septet, m = multiplet, br = broad) were observed to be solvent-independent. It was noted that the amount of gas dissolved in solution gave 1H NMR signal integrations that were qualitatively comparable to those for the solutions made with the 3 μL additions of the liquid or solid contaminants. However, typically in order to observe signals for the gas samples by 13C{1H} NMR spectroscopy, additional time for data collection was required. The solubility of each gas in D2O was extremely limited, making 13C detection impractical. Of all the gases, methane required the most number of transients in order to obtain an observable signal by 13C{1H} NMR spectroscopy. In most cases, the 13C chemical shift of methane was acquired through the use of gs-HMQC NMR spectroscopy to provide enhanced sensitivity. In order to reflect what would be observed in typical NMR-scale experiments, 13C detection was not pursued with isotopically enriched gases. A number of misreported values were discovered in the years since the original publication10 and in the preparation of this paper. These are detailed in the Supporting Information, and the values are now correctly listed in Tables 1 and 2. Acknowledgment. G.R.F. and K.I.G. thank the Department of Energy (Contract No. DE-FG02-06ER15765) for support. A.J.M.M. and J.E.B. thank the Moore Foundation for support. N.H.S. and B.M.S. thank Abbott Laboratories, Amgen, Merck, Bristol-Myers Squibb, Boehringer Ingelheim, the Gordon and Betty Moore Foundation, and Caltech for financial support. Supporting Information Available: Large-format tables of the all the NMR data. This material is available free of charge via the Internet at http://pubs.acs.org. (10) The misreported value for acetonitrile in C6D6 from the original paper2 was also pointed out by Dr. Jongwook Choi, to whom we are grateful. Supporting Information NMR Chemical Shifts of Trace Impurities: Common Laboratory Solvents, Organics, and Gases in Deuterated Solvents Relevant to the Organometallic Chemist Gregory R. Fulmer,*,1 Alexander J. M. Miller,2 Nathaniel H. Sherden,2 Hugo E. Gottlieb,3 Abraham Nudelman,3 Brian M. Stoltz,2 John E. Bercaw,2 and Karen I. Goldberg1 1 2 Department of Chemistry, University of Washington, Box 351700, Seattle, Washington 98195-1700; Arnold and Mabel Beckman Laboratories of Chemical Synthesis, and Caltech Center for Catalysis and Chemical Synthesis, Division of Chemistry and Chemical Engineering California Institute of Technology, Pasadena, California 91125; 3 Department of Chemistry, Bar Ilan University, Ramat Gan 52900, Israel. Corrections and Comments ........................................................................................................ S2 1 H NMR Data (Table S1) ............................................................................................................ S3 13 C NMR Data (Table S2) ........................................................................................................... S5 Individual Solvent Tables – NMR Data Sorted by Chemical Shift (Tables S3–S26) ............ S7 References .................................................................................................................................. S19 S1 Corrections and Comments In the preparation of this manuscript, several errors were discovered in the original paper1 and are reported herein. While comparing the 1H NMR spectral data obtained in toluene-d8 to that in C6D6, it was discovered that the 1H NMR chemical shifts for acetic acid (CH3), acetonitrile (CH3) and tert-butyl alcohol (OH) in C6D6 had each been misreported at 1.55 ppm in the original paper; the values have now been correctly listed as 1.52, 0.58, and 0.63 ppm, respectively. The original paper's assignments for BHT's C(3,5) and C(4) in C6D6, (CD3)2CO, (CD3)2SO, CD3CN, and CD3OD were reversed and are now corrected. The resonances for 1,2-dimethoxyethane (CH2) in (CD3)2CO, silicone grease (CH3) in CDCl3, and 2-propanol (CH3) in CD3OD have been corrected and are reported as 72.47, 1.04, and 1.15 ppm, respectively. No other significant differences were discovered when comparing our data to that which had been previously reported; however, we have additionally provided the OH resonance for ethanol in C6D6 (0.50 ppm), the CH3 resonance for silicone grease in (CD3)2SO (–0.06 ppm), and replaced the “grease” entry (formerly motor oil1) with VWR vacuum pump oil #19, which is now reported in each deuterated solvent. S2 Table S1. 1H NMR Data2 proton mult THF-d 8 1.72 3.58 CD2Cl2 5.32 s s s s ddt ddt ddt ddd s s m m m s s s5 s s5 s s s s5 s s s s s t m m ddt ddt ddt ddd s s t, 7 q, 7 m m s s s s s s s s s s s s s s s t, 7 q, 76 s5,6 s q, 7 t, 7 s q, 7 t, 7 s s7 dd dd m br s s s 2.46 1.89 2.05 1.95 5.90 5.27 5.15 4.50 1.98 9.98 7.86–7.88 7.51–7.55 7.60–7.64 7.31 1.15 3.16 6.68 5.64 3.68 1.40 6.92 5.81 2.21 1.40 7.89 3.57 1.44 2.24 1.77–1.82 1.68–1.71 5.92 5.31 5.19 4.58 3.77 5.51 1.12 3.38 3.43 3.53 3.28 3.28 3.43 1.94 2.95 2.82 3.69 3.65 3.35 7.91 2.88 2.76 2.45 3.56 0.85 1.10 3.51 3.30 1.94 4.04 1.19 2.03 2.39 0.96 5.36 3.48 7.48 6.37 0.85–0.91 1.29 2.18 0.07 1.52 2.06 2.12 1.97 5.92 5.31 5.22 4.55 2.05 10.01 7.87–7.89 7.53–7.57 7.63–7.67 7.35 1.24 6.73 4.76 3.73 1.42 6.97 5.00 2.25 1.42 7.32 3.59 1.44 2.29 1.81–1.87 1.69–1.72 5.95 5.35 5.26 4.61 3.76 5.33 1.15 3.43 3.57 3.50 3.33 3.34 3.49 2.02 2.97 2.87 3.75 3.72 3.37 7.96 2.91 2.82 2.55 3.65 0.85 1.19 3.66 1.33 2.00 4.08 1.23 2.09 2.43 1.00 5.40 3.66 7.46 6.41 0.84–0.90 1.27 2.20 0.07 solvent residual signals water acetic acid acetone acetonitrile allyl acetate OH CH3 CH3 CH3 CH CH2 CHCH 2(1) CHCH 2(2) CH2 CH3 benzaldehyde HCO CH(2,6) CH(3,5) CH(4) benzene CH CH3 tert -butyl alcohol OH BHA ArH OH ArOCH3 ArC(CH3)3 BHT ArH OH ArCH3 ArC(CH3)3 chloroform CH CH2 18-crown-6 CH2 cyclohexane CH2(2,6) cyclohexanone CH2(3,5) CH2(4) CH CH2 diallyl carbonate CHCH 2(1) CHCH 2(2) CH2 CH2 1,2-dichloroethane CH2 dichloromethane CH3 diethyl ether CH2 CH2 diglyme CH2 OCH3 CH3 1,2-dimethoxyethane CH2 CH3CO dimethylacetamide NCH3 NCH3 CH3 dimethyl carbonate CH3 dimethyl malonate CH2 dimethylformamide CH CH3 CH3 CH3 dimethyl sulfoxide CH2 1,4-dioxane CH3 ethane CH3 ethanol CH2 OH CH3CO ethyl acetate CH 2CH3 CH2CH 3 CH3CO ethyl methyl ketone CH 2CH3 CH2CH 3 CH2 ethylene CH2 ethylene glycol furan CH(2,5) CH(3,4) CH3 H grease8 CH2 CH3 hexamethylbenzene CH3 hexamethyldisiloxane S3 CDCl3 7.26 toluene-d 8 C6D6 2.08 7.16 6.97 7.01 7.09 1.56 0.43 0.40 2.10 1.57 1.52 2.17 1.57 1.55 2.10 0.69 0.58 4 5.67 5.684 5.93 5.32 5.05 5.06 5.24 4.94 4.94 4.57 4.34 4.38 2.09 1.63 1.63 10.03 9.57 9.64 7.88–7.91 7.45–7.47 7.49–7.53 7.51–7.57 6.95–6.99 6.93–6.99 7.61–7.65 7.03–7.07 7.01–7.07 7.36 7.12 7.15 1.28 1.03 1.05 0.58 0.63 6.76 6.83 6.93 4.76 4.45 4.53 3.77 3.48 3.48 1.44 1.34 1.41 6.98 6.99 7.05 5.01 4.72 4.79 2.27 2.23 2.24 1.43 1.36 1.38 7.26 6.10 6.15 3.67 3.36 3.39 1.43 1.40 1.40 2.33 1.95 1.98 1.84–1.86 1.33–1.39 1.28–1.37 1.71–1.73 1.16–1.20 1.08–1.16 5.94 5.63 5.65 5.37 5.09 5.09 5.27 4.92 4.92 4.64 4.34 4.38 3.73 2.91 2.90 5.30 4.32 4.27 1.21 1.10 1.11 3.48 3.25 3.26 3.65 3.43 3.46 3.57 3.31 3.34 3.39 3.12 3.11 3.40 3.12 3.12 3.55 3.31 3.33 2.09 1.59 1.60 3.02 2.56 2.57 2.94 2.11 2.05 3.79 3.31 3.30 3.75 3.24 3.23 3.40 2.92 2.97 8.02 7.57 7.63 2.96 2.37 2.36 2.88 1.96 1.86 2.62 1.64 1.68 3.71 3.33 3.35 0.87 0.80 0.81 1.25 0.97 0.96 3.72 3.36 3.34 1.32 0.83 0.50 2.05 1.69 1.65 4.12 3.87 3.89 1.26 0.94 0.92 2.14 1.59 1.58 2.46 1.82 1.81 1.06 0.84 0.85 5.40 5.25 5.25 3.76 3.41 3.36 7.13 7.45 7.10 6.08 6.40 6.07 0.84–0.87 0.89–0.96 0.90–0.98 1.32 1.25 1.33 2.24 2.13 2.10 0.07 0.12 0.10 C6D5Cl 6.96 6.99 7.14 (CD3)2CO (CD3)2SO 2.05 2.50 CD3CN 1.94 TFE-d 3 5.02 3.88 CD3OD 3.31 D2O 4.79 1.03 1.76 1.77 1.21 5.77 5.15 5.04 4.44 1.80 9.77 7.59–7.61 7.15–7.19 7.24–7.28 7.20 1.12 1.30 6.83 4.62 3.61 1.37 6.97 5.50 2.20 1.37 6.74 3.41 1.37 2.08 1.48–1.53 1.33–1.37 5.75 5.17 5.03 4.46 3.26 4.77 1.10 3.31 3.49 3.37 3.16 3.17 3.37 1.74 2.65 2.42 3.48 3.41 3.15 7.73 2.51 2.30 2.03 3.45 0.79 1.06 3.51 1.39 1.78 3.96 1.04 1.78 2.06 0.89 5.29 3.58 7.24 6.19 0.86–0.92 1.30 2.10 0.10 2.843 1.96 2.09 2.05 5.92 5.29 5.18 4.53 2.02 10.05 7.92–7.94 7.59–7.63 7.69–7.73 7.36 1.18 6.72 5.65 3.72 1.41 6.96 2.22 1.41 8.02 3.59 1.43 2.27 1.79–1.83 1.70–1.74 5.96 5.35 5.23 4.62 3.87 5.63 1.11 3.41 3.56 3.47 3.28 3.28 3.46 1.97 3.00 2.83 3.72 3.68 3.42 7.96 2.94 2.78 2.52 3.59 0.83 1.12 3.57 3.39 1.97 4.05 1.20 2.07 2.45 0.96 5.38 3.28 7.56 6.43 0.90 1.29 2.17 0.07 2.13 1.96 2.08 1.96 5.93 5.29 5.21 4.53 2.02 10.01 7.89–7.91 7.57–7.61 7.67–7.71 7.37 1.16 2.18 6.73 4.98 3.72 1.40 6.97 5.20 2.22 1.39 7.58 3.51 1.44 2.27 1.79–1.84 1.67–1.72 5.96 5.34 5.25 4.61 3.81 5.44 1.12 3.42 3.53 3.45 3.29 3.28 3.45 1.97 2.96 2.83 3.72 3.68 3.38 7.92 2.89 2.77 2.50 3.60 0.85 1.12 3.54 2.47 1.97 4.06 1.20 2.06 2.43 0.96 5.41 3.51 7.52 6.44 2.19 0.07 3.66 2.06 2.19 1.95 5.93 5.32 5.25 4.58 2.07 9.88 7.90–7.92 7.56–7.59 7.68–7.72 7.36 1.28 2.20 6.87 3.79 1.44 7.06 2.24 1.43 7.33 3.64 1.47 2.38 1.87–1.92 1.75–1.78 5.92 5.35 5.28 4.62 3.71 5.24 1.20 3.58 3.67 3.62 3.41 3.40 3.61 2.09 3.05 2.94 3.77 3.76 3.41 7.86 2.98 2.88 2.63 3.76 0.85 1.22 3.71 2.03 4.14 1.26 2.16 2.49 1.05 5.40 3.72 7.44 6.42 0.88–0.94 1.33 2.24 0.08 4.87 1.99 2.15 2.03 5.94 5.30 5.21 4.56 2.05 10.00 7.90–7.93 7.56–7.60 7.66–7.70 7.33 1.40 6.71 4.85 3.72 1.41 6.92 2.21 1.40 7.90 3.64 1.45 2.34 1.85–1.87 1.74–1.76 5.94 5.34 5.25 4.61 3.78 5.49 1.18 3.49 3.61 3.58 3.35 3.35 3.52 2.07 3.31 2.92 3.74 3.72 3.44 7.97 2.99 2.86 2.65 3.66 0.85 1.19 3.60 2.01 4.09 1.24 2.12 2.50 1.01 5.39 3.59 7.49 6.40 0.86–0.93 1.29 2.19 0.07 2.08 2.22 2.06 5.99 5.37 5.30 4.62 2.13 9.96 7.97–7.99 7.57–7.66 7.76–7.80 1.24 3.80 2.40 1.85–1.90 1.70–1.75 5.99 5.40 5.32 4.69 1.17 3.56 3.67 3.61 3.37 3.37 3.60 2.08 3.06 2.90 3.69 3.78 3.60 7.92 3.01 2.85 2.71 3.75 0.82 1.17 3.65 2.07 4.14 1.24 2.19 3.18 1.26 5.44 3.65 7.57 6.51 0.28 3.333 1.91 2.09 2.07 5.91 5.29 5.20 4.52 2.03 10.02 7.91–7.93 7.61–7.67 7.69–7.75 7.37 1.11 4.19 6.62 6.52 3.66 1.36 6.87 6.65 2.18 1.36 8.32 3.51 1.40 2.25 1.74–1.78 1.64–1.66 5.93 5.33 5.25 4.61 3.90 5.76 1.09 3.38 3.51 3.38 3.24 3.24 3.43 1.96 2.94 2.78 3.69 3.65 3.53 7.95 2.89 2.73 2.54 3.57 0.82 1.06 3.44 4.63 1.99 4.03 1.17 2.07 2.43 0.91 5.41 3.34 7.67 6.47 0.82–0.88 1.24 2.14 0.06 n -hexane HMPA hydrogen imidazole methane methanol nitromethane n -pentane propane 2-propanol propylene pump oil pyridine pyrrole pyrrolidine10 silicone grease tetrahydrofuran toluene triethylamine 0.88 0.89 0.85 CH3 t, 7 0.89 0.89 0.88 0.88 1.26 1.24 1.19 CH2 m 1.29 1.27 1.22 1.28 2.65 2.40 2.47 CH3 d, 9.5 2.58 2.60 2.42 2.59 4.62 4.47 4.49 H2 s 4.55 4.59 4.50 4.54 7.67 7.33 7.53 CH(2) s 7.48 7.63 7.30 7.62 7.10 6.90 7.01 CH(4,5) s 6.94 7.07 6.86 7.04 0.22 0.16 0.15 CH4 s 0.19 0.21 0.17 0.17 9 3.49 3.07 3.25 CH3 3.27 3.42 3.03 3.31 s 1.09 1.30 OH 3.02 1.09 3.12 s5,9 4.33 2.94 3.59 CH3 s 4.31 4.31 3.01 4.43 0.88 0.87 0.84 CH3 t, 7 0.89 0.89 0.87 0.88 1.27 1.23 1.23 CH2 m 1.31 1.30 1.25 1.27 0.90 0.86 0.84 CH3 t, 7.3 0.90 0.90 0.89 0.88 1.32 1.26 1.26 CH2 sept, 7.3 1.33 1.32 1.32 1.31 1.22 0.95 1.04 CH3 d, 6 1.08 1.17 0.95 1.10 4.04 3.67 3.82 CH sept, 6 3.82 3.97 3.65 3.90 1.73 1.55 1.68 CH3 dt, 6.4, 1.5 1.69 1.71 1.55 1.58 4.94 4.95 4.90 CH2(1) dm, 10 4.89 4.93 4.92 4.91 5.03 5.01 5.00 CH2(2) dm, 17 4.99 5.03 4.98 4.98 5.83 5.72 5.81 CH m 5.79 5.84 5.70 5.72 CH3 m 0.86–0.90 0.84–0.89 0.83–0.89 0.88–0.96 0.91–0.97 0.88–0.91 0.87 1.31 CH2 br s 1.29 1.27 1.26 1.30 1.37 1.29 8.51 CH(2,6) m 8.54 8.59 8.62 8.47 8.53 8.58 6.90 CH(3,5) m 7.25 7.28 7.29 6.67 6.66 7.35 7.25 CH(4) m 7.65 7.68 7.68 6.99 6.98 7.76 8.61 NH br t 9.96 8.69 8.40 7.71 7.80 10.02 6.62 CH(2,5) m 6.66 6.79 6.83 6.43 6.48 6.77 6.27 CH(3,4) m 6.02 6.19 6.26 6.27 6.37 6.07 CH2(2,5) m 2.75 2.82 2.87 2.54 2.54 2.64 1.43 CH2(3,4) m 1.59 1.67 1.68 1.36 1.33 0.14 CH3 s 0.11 0.09 0.07 0.26 0.29 0.13 3.59 CH2(2,5) m 3.62 3.69 3.76 3.54 3.57 3.63 1.55 CH2(3,4) m 1.79 1.82 1.85 1.43 1.40 1.79 2.16 CH3 s 2.31 2.34 2.36 2.11 2.11 2.32 7.01–7.08 7.10–7.20 CH(2,4,6) m 7.10 7.15 7.17 6.96–7.01 7.02 7.10–7.17 7.10–7.20 CH(3,5) m 7.19 7.24 7.25 7.09 7.13 0.93 CH3 t, 7 0.97 0.99 1.03 0.95 0.96 0.96 2.39 CH2 q, 7 2.46 2.48 2.53 2.39 2.40 2.45 S4 0.86 1.25 2.53 4.61 7.63 7.01 0.20 3.16 4.01 4.42 0.86 1.27 0.87 1.29 1.04 3.78 1.68 4.94 5.03 5.80 0.74 1.15 8.58 7.39 7.79 10.75 6.73 6.01 2.67 1.55 –0.06 3.60 1.76 2.30 7.18 7.25 0.93 2.43 0.91 0.90 0.89 1.31 1.29 1.28 2.63 2.64 2.57 4.53 4.56 4.57 7.61 7.67 7.57 7.03 7.05 7.01 0.18 0.20 0.20 3.44 3.34 3.28 2.16 4.28 4.34 4.31 0.90 0.90 0.89 1.33 1.29 1.29 0.90 0.91 0.90 1.33 1.34 1.33 1.20 1.15 1.09 4.05 3.92 3.87 1.70 1.70 1.70 4.93 4.91 4.93 5.03 5.01 5.04 5.87 5.82 5.85 0.85 0.99 0.86–0.91 1.27 1.41 1.29 8.45 8.57 8.53 7.40 7.33 7.44 7.82 7.73 7.85 9.27 6.84 6.75 6.72 6.24 6.10 6.08 2.75 2.80 3.11 1.93 1.61 1.72 0.16 0.08 0.10 3.78 3.64 3.71 1.91 1.80 1.87 2.33 2.33 2.32 7.10–7.30 7.10–7.30 7.16 7.10–7.30 7.10–7.30 7.16 1.31 0.96 1.05 3.12 2.45 2.58 2.61 7.78 7.14 0.18 3.34 4.40 0.88 1.30 1.17 4.02 1.70 4.95 5.06 5.90 8.52 7.45 7.87 6.93 6.26 3.07 1.87 3.74 1.88 0.99 2.57 Table S2. 13C{1H} NMR Data2 carbon solvent signals acetic acid acetone acetonitrile allyl acetate benzaldehyde benzene tert -butyl alcohol BHA BHT carbon dioxide carbon disulfide carbon tetrachloride chloroform 18-crown-6 cyclohexane cyclohexanone diallyl carbonate 1,2-dichloroethane dichloromethane diethyl ether diglyme 1,2-dimethoxyethane dimethylacetamide dimethyl carbonate dimethyl malonate dimethylformamide dimethyl sulfoxide 1,4-dioxane ethane ethanol CO CH3 CO CH3 CN CH3 CO C HCH2 CHC H2 CH2 CH3 HCO C(1) CH(2,6) CH(3,5) CH (4) CH (CH3)3C (C H3)3C C(1) C(2,6) CH(3,5) C(4) CH3O (C H3)3C (CH3)3C C(1) C(2,6) CH(3,5) C(4) CH3Ar (C H3)3C (CH3)3C CO2 CS2 CCl4 CH CH2 CH2 CO CH2(2,6) CH2(3,5) CH2(4) CO C HCH2 CHC H2 CH2 CH2 CH2 CH3 CH2 CH3 CH2 CH2 CH3 CH2 CH3 CO NCH3 NCH3 CO CH3 CO2 CH3 CH2 CH CH3 CH3 CH3 CH2 CH3 CH3 CH2 S5 THF-d 8 67.21 25.31 CD2Cl2 53.84 CDCl3 77.16 171.69 20.13 204.19 30.17 116.79 0.45 170.14 133.90 117.58 65.31 20.45 191.95 137.78 129.98 129.56 134.67 128.84 67.50 30.57 154.07 148.62 110.94 140.07 55.39 30.65 35.51 152.48 137.93 125.71 128.64 21.21 31.55 34.91 125.69 193.37 96.89 79.24 71.34 27.58 208.79 42.17 27.69 25.76 155.36 133.08 117.70 68.58 44.64 54.67 15.49 66.14 58.72 71.17 72.72 58.72 72.58 21.15 169.77 34.60 37.56 156.91 54.58 167.14 52.07 41.15 161.96 35.65 30.70 41.21 67.65 6.79 18.90 57.60 175.85 20.91 206.78 31.00 116.92 2.03 170.83 132.94 118.00 65.36 21.06 192.61 136.98 129.98 129.42 134.79 128.68 69.11 31.46 153.05 148.06 110.93 137.77 55.88 30.37 34.91 151.92 136.32 125.84 128.73 21.27 30.54 34.56 125.26 192.95 96.52 77.99 70.47 27.38 211.82 42.31 27.47 25.42 155.15 132.24 118.75 68.76 44.35 54.24 15.44 66.11 58.95 70.70 72.25 59.02 72.24 21.64 171.05 35.23 38.22 156.73 55.09 167.32 52.75 41.48 162.57 36.56 31.39 41.33 67.47 6.91 18.69 58.57 175.99 20.81 207.07 30.92 116.43 1.89 170.81 132.33 118.34 65.28 21.02 192.67 136.58 129.91 129.16 134.64 128.37 69.15 31.25 152.57 147.85 110.69 137.36 55.70 30.32 34.72 151.55 135.87 125.55 128.27 21.20 30.33 34.25 124.99 192.83 96.34 77.36 70.55 26.94 212.57 41.97 27.00 24.97 154.88 131.58 118.96 68.55 43.50 53.52 15.20 65.91 59.01 70.51 71.90 59.08 71.84 21.53 171.07 35.28 38.13 156.45 54.89 167.18 52.57 41.11 162.62 36.50 31.45 40.76 67.14 6.89 18.41 58.28 toluene-d 8 137.48 128.87 127.96 125.13 20.43 175.30 20.27 204.00 30.03 115.76 0.03 169.44 132.98 117.49 64.87 20.21 191.09 137.12 129.61 128.68 133.88 128.57 68.12 30.49 153.50 148.06 110.99 137.34 55.04 30.30 34.69 152.06 136.12 125.79 128.44 21.42 31.39 34.39 124.86 192.71 96.57 77.89 70.86 27.31 208.60 41.78 27.05 25.15 155.15 132.30 118.04 68.20 43.40 53.47 15.47 65.94 58.62 70.92 72.39 58.63 72.25 21.05 169.65 34.58 36.98 156.61 54.13 166.49 51.76 40.88 161.93 35.22 30.64 40.41 67.17 6.94 18.78 57.81 C6D6 128.06 C6D5Cl 134.19 129.26 128.25 125.96 (CD3)2CO 29.84 206.26 (CD3)2SO 39.52 CD3CN 1.32 118.26 TFE-d 3 61.50 126.28 CD3OD 49.00 D2O - 175.82 20.37 204.43 30.14 116.02 0.20 169.67 132.90 117.64 64.92 20.37 191.43 137.05 129.65 128.95 133.95 128.62 68.19 30.47 153.62 148.13 111.15 137.50 55.27 30.35 34.72 152.05 136.08 125.83 128.52 21.40 31.34 34.35 124.76 192.69 96.44 77.79 70.59 27.23 209.10 41.83 27.00 25.03 155.24 132.18 118.22 68.28 43.59 53.46 15.46 65.94 58.66 70.87 72.35 58.68 72.21 21.16 169.95 34.67 37.03 156.71 54.30 166.66 51.86 41.04 162.13 35.25 30.72 40.03 67.16 6.96 18.72 57.86 175.67 20.40 204.83 30.12 115.93 0.63 169.59 132.69 117.63 64.86 20.40 191.24 136.78 129.49 128.87 134.02 128.38 68.19 31.13 153.19 147.87 110.84 137.29 55.08 30.21 34.56 151.69 135.92 125.58 128.26 21.10 30.19 34.11 126.08 192.49 96.38 77.67 70.55 26.99 209.30 41.79 27.02 25.07 154.87 131.93 118.22 68.19 43.60 53.54 15.35 65.79 58.42 70.56 72.07 58.31 71.81 21.03 169.79 34.59 37.13 156.36 54.23 166.51 51.89 40.93 162.01 35.45 30.71 40.27 66.95 6.91 18.55 57.63 172.31 20.51 205.87 30.60 117.60 1.12 170.61 133.76 117.81 65.28 20.68 192.95 137.66 130.23 129.90 135.14 129.15 68.13 30.72 153.97 148.48 111.00 140.32 55.51 30.64 35.45 152.51 138.19 126.03 129.05 21.31 31.61 35.00 125.81 193.58 96.65 79.19 71.25 27.51 210.36 42.24 27.68 25.59 155.48 133.16 118.53 68.78 45.25 54.95 15.78 66.12 58.77 71.03 72.63 58.45 72.47 21.51 170.61 34.89 37.92 157.04 54.95 167.58 52.47 41.43 162.79 36.15 31.03 41.23 67.60 6.88 18.89 57.72 171.93 20.95 206.31 30.56 117.91 1.03 169.97 132.71 117.64 64.32 20.54 193.08 136.20 129.45 129.10 134.52 128.30 66.88 30.38 152.53 147.44 109.80 141.16 54.89 30.30 34.76 151.47 139.12 124.85 127.97 20.97 31.25 34.33 124.21 192.63 95.44 79.16 69.85 26.33 210.63 41.32 26.46 24.32 154.16 132.18 118.32 67.86 45.02 54.84 15.12 62.05 57.98 69.54 71.25 58.03 71.17 21.29 169.54 34.42 37.38 155.76 54.63 166.91 52.08 40.72 162.29 35.73 30.73 40.45 66.36 6.61 18.51 56.07 173.21 20.73 207.43 30.91 118.26 1.79 171.32 133.83 118.06 65.55 21.02 193.64 137.62 130.42 130.07 135.40 129.32 68.74 30.68 154.02 148.39 111.35 140.20 55.94 30.55 35.48 152.42 138.13 126.38 129.61 21.23 31.50 35.05 125.89 193.60 96.68 79.17 71.22 27.63 211.99 42.44 27.80 25.62 155.66 133.20 118.86 69.09 45.54 55.32 15.63 66.32 58.90 70.99 72.63 58.89 72.47 21.76 171.31 35.17 38.26 157.26 55.39 168.07 52.95 41.77 163.31 36.57 31.32 41.31 67.72 6.99 18.80 57.96 177.96 20.91 32.35 214.98 118.95 1.00 175.98 133.33 119.39 67.61 21.10 197.63 137.84 131.78 130.82 137.17 129.84 72.35 31.07 153.74 150.52 112.90 140.23 57.55 30.80 36.07 153.46 138.59 127.11 130.62 21.34 31.01 35.69 126.92 196.26 97.74 78.83 70.80 28.34 221.30 43.16 28.56 26.00 157.39 132.72 120.15 70.69 45.28 54.46 15.33 67.55 59.40 73.05 71.33 59.52 72.87 21.40 175.74 36.28 39.06 159.04 56.17 170.88 54.00 42.13 166.01 37.76 30.96 40.06 68.52 7.01 18.11 59.68 175.11 20.56 209.67 30.67 118.06 0.85 172.41 133.71 118.22 66.14 20.71 194.11 137.96 130.64 130.12 135.60 129.34 69.40 30.91 154.34 149.04 111.30 141.36 55.96 30.82 35.83 152.85 139.09 126.11 129.49 21.38 31.15 35.36 126.31 193.82 97.21 79.44 71.47 27.96 214.69 42.61 28.16 25.86 156.28 133.25 118.74 69.35 45.11 54.78 15.46 66.88 59.06 71.33 72.92 59.06 72.72 21.32 173.32 35.50 38.43 157.91 55.25 168.70 52.83 41.60 164.73 36.89 31.61 40.45 68.11 6.98 18.40 58.26 177.21 21.03 215.94 30.89 119.68 1.47 174.78 132.48 119.03 66.52 21.00 191.67 136.11 130.09 129.48 134.70 70.36 30.29 197.25 96.73 70.14 221.22 42.02 27.50 24.77 157.78 132.76 118.75 68.81 14.77 66.42 58.67 70.05 71.63 58.67 71.49 21.09 174.57 35.03 38.76 163.96 55.81 170.12 53.65 42.13 165.53 37.54 32.03 39.39 67.19 17.47 58.05 C H3CO CO CH2 CH3 C H3CO ethyl methyl ketone CO C H2CH3 CH2C H3 CH2 ethylene CH2 ethylene glycol furan CH(2,5) CH(3,4) CH2 H grease8 hexamethylbenzene C CH3 CH3 hexamethyldisiloxane CH3 n -hexane CH2(2,5) CH2(3,4) HMPA11 CH3 imidazole CH(2) CH(4,5) CH4 methane CH3 methanol CH3 nitromethane CH3 n -pentane CH2(2,4) CH2(3) CH3 propane CH2 CH3 2-propanol CH CH3 propylene CH2 CH CH2 pump oil pyridine CH(2,6) CH(3,5) CH(4) pyrrole CH(2,5) CH(3,4) pyrrolidine10 CH2(2,5) CH2(3,4) CH3 silicone grease CH2(2,5) tetrahydrofuran CH2(3,4) CH3 toluene C(1) CH(2,6) CH(3,5) CH(4) CH3 triethylamine CH2 ethyl acetate S6 20.45 170.32 60.30 14.37 28.92 207.05 36.59 7.87 123.09 64.35 143.26 109.88 30.45 131.88 16.71 1.83 14.22 23.33 32.34 36.89 135.72 122.20 –4.90 49.64 62.49 14.18 23.00 34.87 16.60 16.82 25.70 66.14 19.27 115.74 134.02 30.63 150.57 124.08 135.99 118.03 107.74 45.82 26.17 1.20 68.03 26.19 21.29 138.24 129.47 128.71 125.84 12.51 47.18 21.15 171.24 60.63 14.37 29.55 209.57 37.01 7.94 123.20 64.08 142.98 109.86 30.14 132.09 16.93 1.96 14.28 23.07 32.01 36.99 135.76 122.16 –4.33 50.45 63.03 14.24 22.77 34.57 16.63 16.63 25.43 64.67 19.47 115.70 134.21 30.13 150.27 124.06 136.16 117.93 108.02 47.02 25.83 1.22 68.16 25.98 21.53 138.36 129.35 128.54 125.62 12.12 46.75 21.04 171.36 60.49 14.19 29.49 209.56 36.89 7.86 123.13 63.79 142.71 109.57 29.71 132.21 16.98 1.97 14.14 22.70 31.64 36.87 135.38 122.00 –4.63 50.41 62.50 14.08 22.38 34.16 16.63 16.37 25.14 64.50 19.50 115.74 133.91 29.84 149.90 123.75 135.96 117.77 107.98 46.93 25.56 1.19 67.97 25.62 21.46 137.89 129.07 128.26 125.33 11.61 46.25 20.46 170.02 60.08 14.23 28.74 206.31 36.32 7.89 122.92 64.29 142.65 109.63 30.31 131.72 16.84 1.99 14.34 23.12 32.06 36.80 135.57 122.13 –4.34 49.90 61.14 14.27 22.79 34.54 16.65 16.63 25.24 64.12 19.32 115.89 133.61 30.33 150.25 123.46 135.17 117.61 108.15 47.12 25.75 1.37 67.75 25.79 21.37 137.84 129.33 128.51 125.66 12.39 46.82 20.56 170.44 60.21 14.19 28.56 206.55 36.36 7.91 122.96 64.34 142.73 109.67 30.22 131.79 16.95 2.05 14.32 23.04 31.96 36.88 135.76 122.16 –4.29 49.97 61.16 14.25 22.72 34.45 16.66 16.60 25.18 64.23 19.38 115.92 133.69 30.24 150.27 123.58 135.28 117.78 108.21 46.86 25.65 1.38 67.80 25.72 21.10 137.91 129.33 128.56 125.68 12.35 46.77 20.50 170.20 60.06 14.07 28.82 206.87 36.39 7.79 122.95 64.03 142.49 109.64 30.11 131.54 16.68 1.92 14.18 22.86 31.77 36.64 135.50 121.96 –4.33 49.66 61.68 14.10 22.54 34.26 16.56 16.48 25.14 64.18 19.32 115.86 133.57 30.11 149.93 123.49 135.32 117.65 108.03 46.75 25.59 1.09 67.64 25.68 21.23 137.65 129.12 128.31 125.43 11.87 46.36 20.83 170.96 60.56 14.50 29.30 208.30 36.75 8.03 123.47 64.26 143.49 110.24 132.22 16.86 2.01 14.34 23.28 32.30 37.04 135.89 122.31 –5.33 49.77 63.21 14.29 22.98 34.83 16.68 16.78 25.67 63.85 19.42 116.03 134.34 30.36 150.67 124.57 136.56 117.98 108.04 1.40 68.07 26.15 21.46 138.48 129.76 129.03 126.12 12.49 47.07 20.68 170.31 59.74 14.40 29.26 208.72 35.83 7.61 123.52 62.76 142.82 109.62 131.10 16.60 1.96 13.88 22.05 30.95 36.42 135.15 121.55 –4.01 48.59 63.28 13.28 21.70 33.48 16.34 15.67 25.43 64.92 19.20 116.07 133.55 29.33 149.58 123.84 136.05 117.32 107.07 46.51 25.26 67.03 25.14 20.99 137.35 128.88 128.18 125.29 11.74 45.74 21.16 171.68 60.98 14.54 29.60 209.88 37.09 8.14 123.69 64.22 143.74 110.49 132.61 16.94 2.07 14.43 23.40 32.36 37.10 136.33 122.78 –4.61 49.90 63.66 14.37 23.08 34.89 16.73 16.91 25.55 64.30 19.48 116.12 134.78 30.86 150.76 127.76 136.89 118.47 108.31 47.57 26.34 68.33 26.27 21.50 138.90 129.94 129.23 126.28 12.38 47.10 21.18 175.55 62.70 14.36 29.64 218.31 38.23 8.29 124.08 64.87 144.22 111.06 134.04 17.04 2.09 14.63 24.06 33.17 37.21 136.58 122.93 –5.88 50.67 63.17 14.54 23.75 35.76 16.93 17.46 25.21 66.69 19.63 116.38 136.00 31.85 149.76 126.27 139.62 119.61 108.85 47.43 25.73 2.87 69.53 26.69 21.62 139.92 130.58 129.79 126.82 9.51 48.45 20.88 172.89 61.50 14.49 29.39 212.16 37.34 8.09 123.46 64.30 143.68 110.33 132.53 16.90 1.99 14.45 23.68 32.73 37.00 136.31 122.60 –4.90 49.86 63.08 14.39 23.38 35.30 16.80 17.19 25.27 64.71 19.50 116.04 134.61 31.35 150.07 125.53 138.35 118.28 108.11 47.23 26.29 2.10 68.83 26.48 21.50 138.85 129.91 129.20 126.29 11.09 46.96 21.15 175.26 62.32 13.92 29.49 218.43 37.27 7.87 63.17 143.57 110.23 2.31 36.46 136.65 122.43 49.5012 63.22 24.38 64.88 149.18 125.12 138.27 119.06 107.83 46.83 25.86 68.68 25.67 9.07 47.19 Table S3. THF-d8 (1H NMR data by chemical shift in ppm) shift 0.07 0.11 0.19 0.85 0.85–0.91 0.86–0.90 0.89 0.89 0.90 0.96 0.97 1.08 1.10 1.12 1.15 1.19 1.29 1.29 1.29 1.31 1.33 1.40 1.40 1.44 1.59 1.68–1.71 1.69 1.72 1.77–1.82 1.79 1.89 1.94 1.94 1.95 1.98 2.03 2.05 2.18 mult proton s CH3 s CH3 s CH4 s CH3 m CH3 m CH3 t, 7 CH3 t, 7 CH3 t, 7.3 CH3 t, 7 CH2CH3 t, 7 CH3 d, 6 CH3 t, 7 CH3 t, 7 CH3 s CH3 t, 7 CH2CH3 br s CH2 m CH2 br s CH2 m CH2 sept, 7.3 CH2 s ArC(CH3)3 s ArC(CH3)3 s CH2 m CH2(3,4) m CH2(4) dt, 6.4, 1.5 CH3 m CHD(3,4) m CH2(3,5) m CH2(3,4) s CH3 s CH3CO s CH3CO s CH3 s CH3 s CH3CO s CH3 s CH3 impurity shift mult proton impurity shift mult proton impurity hexamethyldisiloxane silicone grease methane ethane H grease8 pump oil n-hexane n-pentane propane ethyl methyl ketone triethylamine 2-propanol ethanol diethyl ether tert-butyl alcohol ethyl acetate H grease8 n-hexane pump oil n-pentane propane BHA BHT cyclohexane pyrrolidine cyclohexanone propylene THF-d8 residual cyclohexanone tetrahydrofuran acetic acid dimethylacetamide ethyl acetate acetonitrile allyl acetate ethyl methyl ketone acetone hexamethylbenzene 2.21 2.24 2.31 2.39 2.45 2.46 2.46 2.58 2.75 2.76 2.82 2.88 2.95 3.02 3.16 3.27 3.28 3.28 3.30 3.35 3.38 3.43 3.43 3.48 3.51 3.53 3.56 3.57 3.58 3.62 3.65 3.68 3.69 3.77 3.82 4.04 4.31 s t s q, 7 s s q, 7 d, 9.5 m s s s s s9 s s9 s s s6 s q, 7 m s s q, 76 m s s m m s s s s sept, 6 q, 7 s ArCH3 CH2(2,6) CH3 CH2CH3 CH3 OH CH2 CH3 CH2(2,5) CH3 NCH3 CH3 NCH3 OH OH CH3 OCH3 CH3 OH CH2 CH2 CH2 CH2 CH2 CH2 CH2 CH2 CH2 CHD(2,5) CH2(2,5) CH3 ArOCH3 CH3 CH2 CH CH2CH3 CH3 BHT cyclohexanone toluene ethyl methyl ketone dimethyl sulfoxide water triethylamine HMPA pyrrolidine dimethylformamide dimethylacetamide dimethylformamide dimethylacetamide methanol tert-butyl alcohol methanol diglyme 1,2-dimethoxyethane ethanol dimethyl malonate diethyl ether diglyme 1,2-dimethoxyethane ethylene glycol ethanol diglyme 1,4-dioxane 18-crown-6 THF-d8 residual tetrahydrofuran dimethyl malonate BHA dimethyl carbonate 1,2-dichloroethane 2-propanol ethyl acetate nitromethane 4.50 4.55 4.58 4.89 4.99 5.15 5.19 5.27 5.31 5.36 5.51 5.64 5.79 5.81 5.90 5.92 6.02 6.37 6.66 6.68 6.92 6.94 7.10 7.19 7.25 7.31 7.48 7.48 7.51–7.55 7.60–7.64 7.65 7.86–7.88 7.89 7.91 8.54 9.96 9.98 ddd s ddd dm, 10 dm, 17 ddt ddt ddt ddt s s s m s ddt ddt m dd m s s s m m m s dd s m m m m s s m br t s CH2 H2 CH2 CH2(1) CH2(2) CHCH2(2) CHCH2(2) CHCH2(1) CHCH2(1) CH2 CH2 OH CH OH CHCH2 CHCH2 CH(3,4) CH(3,4) CH(2,5) ArH ArH CH(4,5) CH(2,4,6) CH(3,5) CH(3,5) CH CH(2,5) CH(2) CH(3,5) CH(4) CH(4) CH(2,6) CH CH CH(2,6) NH HCO allyl acetate hydrogen diallyl carbonate propylene propylene allyl acetate diallyl carbonate allyl acetate diallyl carbonate ethylene dichloromethane BHA propylene BHT allyl acetate diallyl carbonate pyrrole furan pyrrole BHA BHT imidazole toluene toluene pyridine benzene furan imidazole benzaldehyde benzaldehyde pyridine benzaldehyde chloroform dimethylformamide pyridine pyrrole benzaldehyde Table S4. THF-d8 (13C{1H} NMR data by chemical shift in ppm) shift carbon impurity shift carbon impurity shift carbon impurity shift carbon impurity –4.90 0.45 1.20 1.83 6.79 7.87 12.51 14.18 14.22 14.37 15.49 16.60 16.71 16.82 18.90 19.27 20.13 20.45 20.45 21.15 21.21 21.29 23.00 23.33 25.31 (p) 25.70 25.76 26.17 26.19 27.58 27.69 28.92 CH4 CH3 CH3 CH3 CH3 CH2CH3 CH3 CH3 CH3 CH3 CH3 CH3 CH3 CH2 CH3 CH3 CH3 CH3 CH3CO CH3 CH3Ar CH3 CH2(2,4) CH2(2,5) CD2(3,4) CH3 CH2(4) CH2(3,4) CH2(3,4) CH2 CH2(3,5) CH3CO methane acetonitrile silicone grease hexamethyldisiloxane ethane ethyl methyl ketone triethylamine n-pentane n-hexane ethyl acetate diethyl ether propane hexamethylbenzene propane ethanol propylene acetic acid allyl acetate ethyl acetate dimethylacetamide BHT toluene n-pentane n-hexane THF-d8 signal 2-propanol cyclohexanone pyrrolidine tetrahydrofuran cyclohexane cyclohexanone ethyl methyl ketone 30.17 30.45 30.57 30.63 30.65 30.70 31.55 32.34 34.60 34.87 34.91 35.51 35.65 36.59 36.89 (d) 37.56 41.15 41.21 42.17 44.64 45.82 47.18 49.64 52.07 54.58 54.67 55.39 57.60 58.72 58.72 60.30 62.49 CH3 CH2 (CH3)3C CH2 (CH3)3C CH3 (CH3)3C CH2(3,4) NCH3 CH2(3) (CH3)3C (CH3)3C CH3 CH2CH3 CH3 NCH3 CH2 CH3 CH2(2,6) CH2 CH2(2,5) CH2 CH3 CH3 CH3 CH2 CH3O CH2 CH3 CH3 CH2 CH3 acetone H grease8 tert-butyl alcohol pump oil BHA dimethylformamide BHT n-hexane dimethylacetamide n-pentane BHT BHA dimethylformamide ethyl methyl ketone HMPA11 dimethylacetamide dimethyl malonate dimethyl sulfoxide cyclohexanone 1,2-dichloroethane pyrrolidine triethylamine methanol dimethyl malonate dimethyl carbonate dichloromethane BHA ethanol diglyme 1,2-dimethoxyethane ethyl acetate nitromethane 64.35 65.31 66.14 66.14 67.21 (p) 67.50 67.65 68.03 68.58 71.17 71.34 72.58 72.72 79.24 96.89 107.74 109.88 110.94 115.74 116.79 117.58 117.70 118.03 122.20 123.09 124.08 125.69 125.71 125.84 128.64 128.71 128.84 CH2 CH2 CH2 CH CD2(2,5) (CH3)3C CH2 CH2(2,5) CH2 CH2 CH2 CH2 CH2 CH CCl4 CH(3,4) CH(3,4) CH(3,5) CH2 CN CHCH2 CHCH2 CH(2,5) CH(4,5) CH2 CH(3,5) CO2 CH(3,5) CH(4) C(4) CH(3,5) CH ethylene glycol allyl acetate diethyl ether 2-propanol THF-d8 signal tert-butyl alcohol 1,4-dioxane tetrahydrofuran diallyl carbonate diglyme 18-crown-6 1,2-dimethoxyethane diglyme chloroform carbon tetrachloride pyrrole furan BHA propylene acetonitrile allyl acetate diallyl carbonate pyrrole imidazole ethylene pyridine carbon dioxide BHT toluene BHT toluene benzene 129.47 129.56 129.98 131.88 133.08 133.90 134.02 134.67 135.72 135.99 137.78 137.93 138.24 140.07 143.26 148.62 150.57 152.48 154.07 155.36 156.91 161.96 167.14 169.77 170.14 170.32 171.69 191.95 193.37 204.19 207.05 208.79 CH(2,6) CH(3,5) CH(2,6) C CHCH2 CHCH2 CH CH (4) CH(2) CH(4) C(1) C(2,6) C(1) C(4) CH(2,5) C(2,6) CH(2,6) C(1) C(1) CO CO CH CO2 CO CO CO CO HCO CS2 CO CO CO toluene benzaldehyde benzaldehyde hexamethylbenzene diallyl carbonate allyl acetate propylene benzaldehyde imidazole pyridine benzaldehyde BHT toluene BHA furan BHA pyridine BHT BHA diallyl carbonate dimethyl carbonate dimethylformamide dimethyl malonate dimethylacetamide allyl acetate ethyl acetate acetic acid benzaldehyde carbon disulfide acetone ethyl methyl ketone cyclohexanone S7 Table S5. CD2Cl2 (1H NMR data by chemical shift in ppm) shift mult 0.07 0.09 0.21 0.84–0.89 0.84–0.90 0.85 0.89 0.89 0.90 0.99 1.00 1.09 1.15 1.17 1.19 1.23 1.24 1.27 1.27 1.27 1.30 1.32 1.33 1.42 1.42 1.44 1.52 1.69–1.72 1.67 1.71 1.81–1.87 1.82 1.97 2.00 2.02 2.05 2.06 proton s CH3 s CH3 s CH4 m CH3 m CH3 s CH3 t, 7 CH3 t, 7 CH3 t, 7.3 CH3 t, 7 CH3 t, 7 CH2CH3 s9 OH t, 7 CH3 d, 6 CH3 t, 7 CH3 t, 7 CH2CH3 s CH3 br s CH2 m CH2 br s CH2 m CH2 sept, 7.3 CH2 s6 OH s ArC(CH3)3 s ArC(CH3)3 s CH2 s OH m CH2(4) m CH2(3,4) dt, 6.4, 1.5 CH3 m CH2(3,5) m CH2(3,4) s CH3 s CH3CO s CH3CO s CH3 s CH3 impurity shift mult proton impurity shift mult proton impurity hexamethyldisiloxane silicone grease methane pump oil H grease8 ethane n-hexane n-pentane propane triethylamine ethyl methyl ketone methanol diethyl ether 2-propanol ethanol ethyl acetate tert-butyl alcohol H grease8 n-hexane pump oil n-pentane propane ethanol BHA BHT cyclohexane water cyclohexanone pyrrolidine propylene cyclohexanone tetrahydrofuran acetonitrile ethyl acetate dimethylacetamide allyl acetate acetic acid 2.09 2.12 2.20 2.25 2.29 2.34 2.43 2.48 2.55 2.60 2.82 2.82 2.87 2.91 2.97 3.33 3.34 3.37 3.42 3.43 3.49 3.50 3.57 3.59 3.65 3.66 3.66 3.69 3.72 3.73 3.75 3.76 3.97 4.08 4.31 4.55 4.59 s s s s t s q, 7 q, 7 s d, 9.5 s m s s s s s s s9 q, 7 s m m s s q, 76 s m s s s s sept, 6 q, 7 s ddd s CH3CO CH3 CH3 ArCH3 CH2(2,6) CH3 CH2CH3 CH2 CH3 CH3 CH3 CH2(2,5) NCH3 CH3 NCH3 OCH3 CH3 CH2 CH3 CH2 CH2 CH2 CH2 CH2 CH2 CH2 CH2 CH2(2,5) CH3 ArOCH3 CH3 CH2 CH CH2CH3 CH3 CH2 H2 ethyl methyl ketone acetone hexamethylbenzene BHT cyclohexanone toluene ethyl methyl ketone triethylamine dimethyl sulfoxide HMPA dimethylformamide pyrrolidine dimethylacetamide dimethylformamide dimethylacetamide diglyme 1,2-dimethoxyethane dimethyl malonate methanol diethyl ether 1,2-dimethoxyethane diglyme diglyme 18-crown-6 1,4-dioxane ethanol ethylene glycol tetrahydrofuran dimethyl malonate BHA dimethyl carbonate 1,2-dichloroethane 2-propanol ethyl acetate nitromethane allyl acetate hydrogen 4.61 4.76 4.93 5.00 5.03 5.22 5.26 5.31 5.32 5.33 5.35 5.40 5.84 5.92 5.95 6.19 6.41 6.73 6.79 6.97 7.07 7.15 7.24 7.28 7.32 7.35 7.46 7.53–7.57 7.63 7.63–7.67 7.68 7.87–7.89 7.96 8.59 8.69 10.01 ddd s dm, 10 s dm, 17 ddt ddt ddt t s ddt s m ddt ddt m dd s m s s m m m s s dd m s m m m s m br t s CH2 OH CH2(1) OH CH2(2) CHCH2(2) CHCH2(2) CHCH2(1) CDHCl2 CH2 CHCH2(1) CH2 CH CHCH2 CHCH2 CH(3,4) CH(3,4) ArH CH(2,5) ArH CH(4,5) CH(2,4,6) CH(3,5) CH(3,5) CH CH CH(2,5) CH(3,5) CH(2) CH(4) CH(4) CH(2,6) CH CH(2,6) NH HCO diallyl carbonate BHA propylene BHT propylene allyl acetate diallyl carbonate allyl acetate CD2Cl2 residual dichloromethane diallyl carbonate ethylene propylene allyl acetate diallyl carbonate pyrrole furan BHA pyrrole BHT imidazole toluene toluene pyridine chloroform benzene furan benzaldehyde imidazole benzaldehyde pyridine benzaldehyde dimethylformamide pyridine pyrrole benzaldehyde Table S6. CD2Cl2 (13C{1H} NMR data by chemical shift in ppm) shift carbon impurity shift carbon impurity shift carbon impurity shift carbon impurity –4.33 1.22 1.96 2.03 6.91 7.94 12.12 14.24 14.28 14.37 15.44 16.63 16.63 16.93 18.69 19.47 20.91 21.06 21.15 21.27 21.53 21.64 22.77 23.07 25.42 25.43 25.83 25.98 27.38 27.47 29.55 30.13 CH4 CH3 CH3 CH3 CH3 CH2CH3 CH3 CH3 CH3 CH3 CH3 CH3 CH2 CH3 CH3 CH3 CH3 CH3 CH3CO CH3Ar CH3 CH3 CH2(2,4) CH2(2,5) CH2(4) CH3 CH2(3,4) CH2(3,4) CH2 CH2(3,5) CH3CO CH2 methane silicone grease hexamethyldisiloxane acetonitrile ethane ethyl methyl ketone triethylamine n-pentane n-hexane ethyl acetate diethyl ether propane propane hexamethylbenzene ethanol propylene acetic acid allyl acetate ethyl acetate BHT toluene dimethylacetamide n-pentane n-hexane cyclohexanone 2-propanol pyrrolidine tetrahydrofuran cyclohexane cyclohexanone ethyl methyl ketone pump oil 30.14 30.37 30.54 31.00 31.39 31.46 32.01 34.56 34.57 34.91 35.23 36.56 36.99 (d) 37.01 38.22 41.33 41.48 42.31 44.35 46.75 47.02 50.45 52.75 53.84 (p) 54.24 55.09 55.88 58.57 58.95 59.02 60.63 63.03 CH2 (CH3)3C (CH3)3C CH3 CH3 (CH3)3C CH2(3,4) (CH3)3C CH2(3) (CH3)3C NCH3 CH3 CH3 CH2CH3 NCH3 CH3 CH2 CH2(2,6) CH2 CH2 CH2(2,5) CH3 CH3 CD2Cl2 CH2 CH3 CH3O CH2 CH3 CH3 CH2 CH3 H grease8 BHA BHT acetone dimethylformamide tert-butyl alcohol n-hexane BHT n-pentane BHA dimethylacetamide dimethylformamide HMPAi ethyl methyl ketone dimethylacetamide dimethyl sulfoxide dimethyl malonate cyclohexanone 1,2-dichloroethane triethylamine pyrrolidine methanol dimethyl malonate CD2Cl2 signal dichloromethane dimethyl carbonate BHA ethanol diglyme 1,2-dimethoxyethane ethyl acetate nitromethane 64.08 64.67 65.36 66.11 67.47 68.16 68.76 69.11 70.47 70.70 72.24 72.25 77.99 96.52 108.02 109.86 110.93 115.7 116.92 117.93 118.00 118.75 122.16 123.20 124.06 125.26 125.62 125.84 128.54 128.68 128.73 129.35 CH2 CH CH2 CH2 CH2 CH2(2,5) CH2 (CH3)3C CH2 CH2 CH2 CH2 CH CCl4 CH(3,4) CH(3,4) CH(3,5) CH2 CN CH(2,5) CHCH2 CHCH2 CH(4,5) CH2 CH(3,5) CO2 CH(4) CH(3,5) CH(3,5) CH C(4) CH(2,6) ethylene glycol 2-propanol allyl acetate diethyl ether 1,4-dioxane tetrahydrofuran diallyl carbonate tert-butyl alcohol 18-crown-6 diglyme 1,2-dimethoxyethane diglyme chloroform carbon tetrachloride pyrrole furan BHA propylene acetonitrile pyrrole allyl acetate diallyl carbonate imidazole ethylene pyridine carbon dioxide toluene BHT toluene benzene BHT toluene 129.42 129.98 132.09 132.24 132.94 134.21 134.79 135.76 136.16 136.32 136.98 137.77 138.36 142.98 148.06 150.27 151.92 153.05 155.15 156.73 162.57 167.32 170.83 171.05 171.24 175.85 192.61 192.95 206.78 209.57 211.82 CH(3,5) CH(2,6) C CHCH2 CHCH2 CH CH (4) CH(2) CH(4) C(2,6) C(1) C(4) C(1) CH(2,5) C(2,6) CH(2,6) C(1) C(1) CO CO CH CO2 CO CO CO CO HCO CS2 CO CO CO benzaldehyde benzaldehyde hexamethylbenzene diallyl carbonate allyl acetate propylene benzaldehyde imidazole pyridine BHT benzaldehyde BHA toluene furan BHA pyridine BHT BHA diallyl carbonate dimethyl carbonate dimethylformamide dimethyl malonate allyl acetate dimethylacetamide ethyl acetate acetic acid benzaldehyde carbon disulfide acetone ethyl methyl ketone cyclohexanone S8 Table S7. CDCl3 (1H NMR data by chemical shift in ppm) shift mult 0.07 0.07 0.22 0.83–0.89 0.84–0.87 0.87 0.88 0.88 0.90 1.03 1.06 1.09 1.21 1.22 1.25 1.25 1.26 1.26 1.26 1.27 1.28 1.32 1.32 1.43 1.43 1.44 1.56 1.68 1.71–1.73 1.73 1.84–1.86 1.85 2.05 2.09 2.09 2.10 2.10 proton s CH3 s CH3 s CH4 m CH3 m CH3 s CH3 t, 7 CH3 t, 7 CH3 t, 7.3 CH3 t, 7 CH3 t, 7 CH2CH3 s9 OH t, 7 CH3 d, 6 CH3 t, 7 CH3 br s CH2 t, 7 CH2CH3 m CH2 br s CH2 m CH2 s CH3 s6 OH sept, 7.3 CH2 s ArC(CH3)3 s CH2 s ArC(CH3)3 s OH m CH2(3,4) m CH2(4) dt, 6.4, 1.5 CH3 m CH2(3,5) m CH2(3,4) s CH3CO s CH3 s CH3CO s CH3 s CH3 impurity shift mult proton impurity shift mult proton impurity hexamethyldisiloxane silicone grease methane pump oil H grease8 ethane n-hexane n-pentane propane triethylamine ethyl methyl ketone methanol diethyl ether 2-propanol ethanol H grease8 ethyl acetate n-hexane pump oil n-pentane tert-butyl alcohol ethanol propane BHT cyclohexane BHA water pyrrolidine cyclohexanone propylene cyclohexanone tetrahydrofuran ethyl acetate allyl acetate dimethylacetamide acetic acid acetonitrile 2.14 2.17 2.24 2.27 2.33 2.36 2.46 2.53 2.62 2.65 2.87 2.88 2.94 2.96 3.02 3.39 3.40 3.40 3.48 3.49 3.55 3.57 3.65 3.67 3.71 3.72 3.73 3.75 3.76 3.76 3.77 3.79 4.04 4.12 4.33 4.57 4.62 s s s s t s q, 7 q, 7 s d, 9.5 m s s s s s s s q, 7 s9 s m m s s q, 79 s s s m s s sept, 6 q, 7 s ddd s CH3CO CH3 CH3 ArCH3 CH2(2,6) CH3 CH2CH3 CH2 CH3 CH3 CH2(2,5) CH3 NCH3 CH3 NCH3 OCH3 CH3 CH2 CH2 CH3 CH2 CH2 CH2 CH2 CH2 CH2 CH2 CH3 CH2 CH2(2,5) ArOCH3 CH3 CH CH2CH3 CH3 CH2 H2 ethyl methyl ketone acetone hexamethylbenzene BHT cyclohexanone toluene ethyl methyl ketone triethylamine dimethyl sulfoxide HMPA pyrrolidine dimethylformamide dimethylacetamide dimethylformamide dimethylacetamide diglyme 1,2-dimethoxyethane dimethyl malonate diethyl ether methanol 1,2-dimethoxyethane diglyme diglyme 18-crown-6 1,4-dioxane ethanol 1,2-dichloroethane dimethyl malonate ethylene glycol tetrahydrofuran BHA dimethyl carbonate 2-propanol ethyl acetate nitromethane allyl acetate hydrogen 4.64 4.76 4.94 5.01 5.03 5.24 5.27 5.30 5.32 5.37 5.40 5.83 5.93 5.94 6.26 6.40 6.76 6.83 6.98 7.10 7.17 7.25 7.26 7.26 7.29 7.36 7.45 7.51–7.57 7.61–7.65 7.67 7.68 7.88–7.91 8.02 8.40 8.62 10.03 ddd s dm, 10 s dm, 17 ddt ddt s ddt ddt s m ddt ddt m dd s m s s m m s s m s dd m m s m m s br t m s CH2 OHd CH2(1) OHd CH2(2) CHCH2(2) CHCH2(2) CH2 CHCH2(1) CHCH2(1) CH2 CH CHCH2 CHCH2 CH(3,4) CH(3,4) ArH CH(2,5) ArH CH(4,5) CH(2,4,6) CH(3,5) CH CH CH(3,5) CH CH(2,5) CH(3,5) CH(4) CH(2) CH(4) CH(2,6) CH NH CH(2,6) HCO diallyl carbonate BHA propylene BHT propylene allyl acetate diallyl carbonate dichloromethane allyl acetate diallyl carbonate ethylene propylene allyl acetate diallyl carbonate pyrrole furan BHA pyrrole BHT imidazole toluene toluene CDCl3 residual chloroform pyridine benzene furan benzaldehyde benzaldehyde imidazole pyridine benzaldehyde dimethylformamide pyrrole pyridine benzaldehyde Table S8. CDCl3 (13C{1H} NMR data by chemical shift in ppm) shift carbon impurity shift carbon impurity shift carbon impurity shift carbon impurity –4.63 1.19 1.89 1.97 6.89 7.86 11.61 14.08 14.14 14.19 15.20 16.37 16.63 16.98 18.41 19.50 20.81 21.02 21.04 21.20 21.46 21.53 22.38 22.70 24.97 25.14 25.56 25.62 26.94 27.00 29.49 29.71 CH4 CH3 CH3 CH3 CH3 CH2CH3 CH3 CH3 CH3 CH3 CH3 CH2 CH3 CH3 CH3 CH3 CH3 CH3 CH3CO CH3Ar CH3 CH3 CH2(2,4) CH2(2,5) CH2(4) CH3 CH2(3,4) CH2(3,4) CH2 CH2(3,5) CH3CO CH2 methane silicone grease acetonitrile hexamethyldisiloxane ethane ethyl methyl ketone triethylamine n-pentane n-hexane ethyl acetate diethyl ether propane propane hexamethylbenzene ethanol propylene acetic acid allyl acetate ethyl acetate BHT toluene dimethylacetamide n-pentane n-hexane cyclohexanone 2-propanol pyrrolidine tetrahydrofuran cyclohexane cyclohexanone ethyl methyl ketone H grease8 29.84 30.32 30.33 30.92 31.25 31.45 31.64 34.16 34.25 34.72 35.28 36.50 36.87 (d) 36.89 38.13 40.76 41.11 41.97 43.50 46.25 46.93 50.41 52.57 53.52 54.89 55.70 58.28 59.01 59.08 60.49 62.50 63.79 CH2 (CH3)3C (CH3)3C CH3 (CH3)3C CH3 CH2(3,4) CH2(3) (CH3)3C (CH3)3C NCH3 CH3 CH3 CH2CH3 NCH3 CH3 CH2 CH2(2,6) CH2 CH2 CH2(2,5) CH3 CH3 CH2 CH3 CH3O CH2 CH3 CH3 CH2 CH3 CH2 pump oil BHA BHT acetone tert-butyl alcohol dimethyl malonate n-hexane n-pentane BHT BHA dimethylacetamide dimethyl malonate HMPAi ethyl methyl ketone dimethylacetamide dimethyl sulfoxide dimethyl malonate cyclohexanone 1,2-dichloroethane triethylamine pyrrolidine methanol dimethyl malonate dichloromethane dimethyl carbonate BHA ethanol diglyme 1,2-dimethoxyethane ethyl acetate nitromethane ethylene glycol 64.50 65.28 65.91 67.14 67.97 68.55 69.15 70.51 70.55 71.84 71.90 77.16 (t) 77.36 96.34 107.98 109.57 110.69 115.74 116.43 117.77 118.34 118.96 122.00 123.13 123.75 124.99 125.33 125.55 128.26 128.27 128.37 129.07 CH CH2 CH2 CH2 CH2(2,5) CH2 (CH3)3C CH2 CH2 CH2 CH2 CDCl3 CH CCl4 CH(3,4) CH(3,4) CH(3,5) CH2 CN CH(2,5) CHCH2 CHCH2 CH(4,5) CH2 CH(3,5) CO2 CH(4) CH(3,5) CH(3,5) C(4) CH CH(2,6) 2-propanol allyl acetate diethyl ether 1,4-dioxane tetrahydrofuran diallyl carbonate tert-butyl alcohol diglyme 18-crown-6 1,2-dimethoxyethane diglyme CDCl3 signal chloroform carbon tetrachloride pyrrole furan BHA propylene acetonitrile pyrrole allyl acetate diallyl carbonate imidazole ethylene pyridine carbon dioxide toluene BHT toluene BHT benzene toluene 129.16 129.91 131.58 132.21 132.33 133.91 134.64 135.38 135.87 135.96 136.58 137.36 137.89 142.71 147.85 149.90 151.55 152.57 154.88 156.45 162.62 167.18 170.81 171.07 171.36 175.99 192.67 192.83 207.07 209.56 212.57 CH(3,5) CH(2,6) CHCH2 C CHCH2 CH CH (4) CH(2) C(2,6) CH(4) C(1) C(4) C(1) CH(2,5) C(2,6) CH(2,6) C(1) C(1) CO CO CH CO2 CO CO CO CO HCO CS2 CO CO CO benzaldehyde benzaldehyde diallyl carbonate hexamethylbenzene allyl acetate propylene benzaldehyde imidazole BHT pyridine benzaldehyde BHA toluene furan BHA pyridine BHT BHA diallyl carbonate dimethyl carbonate dimethylformamide dimethyl malonate allyl acetate dimethylacetamide ethyl acetate acetic acid benzaldehyde carbon disulfide acetone ethyl methyl ketone cyclohexanone S9 Table S9. Toluene-d8 (1H NMR data by chemical shift in ppm) shift mult 0.10 0.17 0.26 0.43 0.58 0.69 0.81 0.83 0.84 0.87 0.88 0.88–0.96 0.89 0.89–0.96 0.94 0.95 0.95 0.97 1.03 1.10 1.16–1.20 1.22 1.25 1.30 1.32 1.33 1.33–1.39 1.34 1.36 1.36 1.40 1.43 1.55 1.57 1.57 1.59 1.59 1.63 proton s CH3 s CH4 s CH3 s OH s OH s CH3 s CH3 s6 OH t, 7 CH2CH3 t, 7 CH3 t, 7 CH3 m CH3 t, 7.3 CH3 m CH3 t, 7 CH2CH3 d, 6 CH3 t, 7 CH3 t, 7 CH3 s CH3 t, 7 CH3 m CH2(4) m CH2 m CH2 br s CH2 sept, 7.3 CH2 br s CH2 m CH2(3,5) s ArC(CH3)3 s ArC(CH3)3 m CH2(3,4) s CH2 m CH2(3,4) dt, 6.4, 1.5 CH3 s CH3 s CH3 s CH3CO s CH3CO s CH3 impurity shift mult proton impurity shift mult proton impurity hexamethyldisiloxane methane silicone grease water tert-butyl alcohol acetonitrile ethane ethanol ethyl methyl ketone n-pentane n-hexane pump oil propane H grease8 ethyl acetate 2-propanol triethylamine ethanol tert-butyl alcohol diethyl ether cyclohexanone n-hexane n-pentane pump oil propane H grease8 cyclohexanone BHA BHT pyrrolidine cyclohexane tetrahydrofuran propylene acetic acid acetone dimethylacetamide ethyl methyl ketone allyl acetate 1.64 1.69 1.82 1.95 1.96 2.08 2.10 2.11 2.11 2.23 2.37 2.39 2.42 2.54 2.56 2.91 2.92 3.01 3.03 3.12 3.12 3.24 3.25 3.31 3.31 3.31 3.33 3.36 3.36 3.36 3.43 3.48 3.54 3.65 3.87 4.32 4.34 4.34 s s q, 7 t s p s s s s s q, 7 d, 9.5 m s s s s s9 s s s q, 7 m s s s s q, 76 s m s m sept, 6 q, 7 s ddd ddd CH3 CH3CO CH2CH3 CH2(2,6) CH3 CH3 CH3 NCH3 CH3 ArCH3 CH3 CH2 CH3 CH2(2,5) NCH3 CH2 CH2 CH3 CH3 OCH3 CH3 CH3 CH2 CH2 CH2 CH3 CH2 CH2 CH2 CH2 CH2 ArOCH3 CH2(2,5) CH CH2CH3 CH2 CH2 CH2 dimethyl sulfoxide ethyl acetate ethyl methyl ketone cyclohexanone dimethylformamide Toluene-d8 residual hexamethylbenzene dimethylacetamide toluene BHT dimethylformamide triethylamine HMPA pyrrolidine dimethylacetamide 1,2-dichloroethane dimethyl malonate nitromethane methanol diglyme 1,2-dimethoxyethane dimethyl malonate diethyl ether diglyme 1,2-dimethoxyethane dimethyl carbonate 1,4-dioxane 18-crown-6 ethanol ethylene glycol diglyme BHA tetrahydrofuran 2-propanol ethyl acetate dichloromethane allyl acetate diallyl carbonate 4.45 4.50 4.72 4.92 4.92 4.94 4.98 5.05 5.09 5.25 5.63 5.674 5.70 6.07 6.10 6.27 6.43 6.67 6.83 6.86 6.95–6.99 6.96–7.01 6.97 6.99 6.99 7.01 7.03–7.07 7.09 7.09 7.10 7.12 7.30 7.45–7.47 7.57 7.71 8.47 9.57 s s s ddt dm, 10 ddt dm, 17 ddt ddt s ddt t(nfo ABX) m dd s m m m s s m m p s m s m m m dd s s m s br t m s OH5 H2 OH5 CHCH2(2) CH2(1) CHCH2(2) CH2(2) CHCH2(1) CHCH2(1) CH2 CHCH2 CHCH2 CH CH(3,4) CH CH(3,4) CH(2,5) CH(3,5) ArH CH(4,5) CH(3,5) CH(2,4,6) CH(4) ArH CH(4) CH(2,6) CH(4) CH(3,5) CH(3,5) CH(2,5) CH CH(2) CH(2,6) CH NH CH(2,6) HCO BHA hydrogen BHT diallyl carbonate propylene allyl acetate propylene allyl acetate diallyl carbonate ethylene diallyl carbonate allyl acetate propylene furan chloroform pyrrole pyrrole pyridine BHA imidazole benzaldehyde toluene Toluene-d8 residual BHT pyridine Toluene-d8 residual benzaldehyde Toluene-d8 residual toluene furan benzene imidazole benzaldehyde dimethylformamide pyrrole pyridine benzaldehyde Table S10. Toluene-d8 (13C{1H} NMR data by chemical shift in ppm) shift carbon impurity shift carbon impurity shift carbon impurity shift carbon impurity –4.34 0.03 1.37 1.99 6.94 7.89 12.39 14.23 14.27 14.34 15.47 16.63 16.65 16.84 18.78 19.32 20.21 20.27 20.43 (sept) 20.46 21.05 21.37 21.42 22.79 23.12 25.15 25.24 25.75 25.79 27.05 27.31 28.74 30.03 CH4 CH3 CH3 CH3 CH3 CH2CH3 CH3 CH3 CH3 CH3 CH3 CH2 CH3 CH3 CH3 CH3 CH3 CH3 CD3 CH3CO CH3 CH3 CH3Ar CH2(2,4) CH2(2,5) CH2(4) CH3 CH2(3,4) CH2(3,4) CH2(3,5) CH2 CH3CO CH3 methane acetonitrile silicone grease hexamethyldisiloxane ethane ethyl methyl ketone triethylamine ethyl acetate n-pentane n-hexane diethyl ether propane propane hexamethylbenzene ethanol propylene allyl acetate acetic acid toluene-d8 signal ethyl acetate dimethylacetamide toluene BHT n-pentane n-hexane cyclohexanone 2-propanol pyrrolidine tetrahydrofuran cyclohexanone cyclohexane ethyl methyl ketone acetone 30.30 30.31 30.33 30.49 30.64 31.39 32.06 34.39 34.54 34.58 34.69 35.22 36.32 36.8 (d) 36.98 40.41 40.88 41.78 43.40 46.82 47.12 49.90 51.76 53.47 54.13 55.04 57.81 58.62 58.63 60.08 61.14 64.12 64.29 (CH3)3C CH2 CH2 (CH3)3C CH3 (CH3)3C CH2(3,4) (CH3)3C CH2(3) NCH3 (CH3)3C CH3 CH2CH3 CH3 NCH3 CH3 CH2 CH2(2,6) CH2 CH2 CH2(2,5) CH3 CH3 CH2 CH3 CH3O CH2 CH3 CH3 CH2 CH3 CH CH2 BHA H grease8 pump oil tert-butyl alcohol dimethylformamide BHT n-hexane BHT n-pentane dimethylacetamide BHA dimethylformamide ethyl methyl ketone HMPA11 dimethylacetamide dimethyl sulfoxide dimethyl malonate cyclohexanone 1,2-dichloroethane triethylamine pyrrolidine methanol dimethyl malonate dichloromethane dimethyl carbonate BHA ethanol diglyme 1,2-dimethoxyethane ethyl acetate nitromethane 2-propanol ethylene glycol 64.87 65.94 67.17 67.75 68.12 68.20 70.86 70.92 72.25 72.39 77.89 96.57 108.15 109.63 110.99 115.76 115.89 117.49 117.61 118.04 122.13 122.92 123.46 124.86 125.13 (t) 125.66 125.79 127.96 (t) 128.44 128.51 128.57 128.68 128.87 (t) CH2 CH2 CH2 CH2(2,5) (CH3)3C CH2 CH2 CH2 CH2 CH2 CH CCl4 CH(3,4) CH(3,4) CH(3,5) CN CH2 CHCH2 CH(2,5) CHCH2 CH(4,5) CH2 CH(3,5) CO2 CD(4) CH(4) CH(3,5) CD(3,5) C(4) CH(3,5) CH CH(3,5) CD(2,6) allyl acetate diethyl ether 1,4-dioxane tetrahydrofuran tert-butyl alcohol diallyl carbonate 18-crown-6 diglyme 1,2-dimethoxyethane diglyme chloroform carbon tetrachloride pyrrole furan BHA acetonitrile propylene allyl acetate pyrrole diallyl carbonate imidazole ethylene pyridine carbon dioxide toluene-d8 signal toluene BHT toluene-d8 signal BHT toluene benzene benzaldehyde toluene-d8 signal 129.33 129.61 131.72 132.30 132.98 133.61 133.88 135.17 135.57 136.12 137.12 137.34 137.48 137.84 142.65 148.06 150.25 152.06 153.50 155.15 156.61 161.93 166.49 169.44 169.65 170.02 175.30 191.09 192.71 204.00 206.31 208.60 CH(2,6) CH(2,6) C CHCH2 CHCH2 CH CH (4) CH(4) CH(2) C(2,6) C(1) C(4) C C(1) CH(2,5) C(2,6) CH(2,6) C(1) C(1) CO CO CH CO2 CO CO CO CO HCO CS2 CO CO CO toluene benzaldehyde hexamethylbenzene diallyl carbonate allyl acetate propylene benzaldehyde pyridine imidazole BHT benzaldehyde BHA toluene-d8 signal toluene furan BHA pyridine BHT BHA diallyl carbonate dimethyl carbonate dimethylformamide dimethyl malonate allyl acetate dimethylacetamide ethyl acetate acetic acid benzaldehyde carbon disulfide acetone ethyl methyl ketone cyclohexanone S10 Table S11. C6D6 (1H NMR data by chemical shift in ppm) shift mult 0.12 0.16 0.29 0.40 0.50 0.58 0.63 0.80 0.85 0.86 0.87 0.89 0.90–0.98 0.91–0.97 0.92 0.95 0.96 0.96 1.05 1.08–1.16 1.11 1.23 1.24 1.26 1.28–1.37 1.32 1.33 1.37 1.38 1.40 1.40 1.41 1.52 1.55 1.55 1.58 1.60 proton s CH3 s CH4 s CH3 s OH 6 s OH s CH3 s OH s CH3 t, 7 CH2CH3 t, 7.3 CH3 t, 7 CH3 t, 7 CH3 m CH3 m CH3 t, 7 CH2CH3 d, 6 CH3 t, 7 CH3 t, 7 CH3 s CH3 m CH2(4) t, 7 CH3 m CH2 m CH2 sept, 7.3 CH2 m CH2(3,5) br s CH2 m CH2(3,4) br s CH2 s ArC(CH3)3 s CH2 m CH2(3,4) s ArC(CH3)3 s CH3 s CH3 dt, 6.4, 1.5 CH3 s CH3CO s CH3CO impurity shift mult proton impurity shift mult proton impurity hexamethyldisiloxane methane silicone grease water ethanol acetonitrile tert-butyl alcohol ethane ethyl methyl ketone propane n-pentane n-hexane H grease8 pump oil ethyl acetate 2-propanol ethanol triethylamine tert-butyl alcohol cyclohexanone diethyl ether n-pentane n-hexane propane cyclohexanone H grease8 pyrrolidine pump oil BHT cyclohexane tetrahydrofuran BHA acetic acid acetone propylene ethyl methyl ketone dimethylacetamide 1.63 1.65 1.68 1.81 1.86 1.98 2.05 2.11 2.13 2.24 2.36 2.40 2.40 2.54 2.57 2.90 2.94 2.97 3.07 3.11 3.12 3.23 3.26 3.30 3.33 3.34 3.34 3.35 3.39 3.41 3.46 3.48 3.57 3.67 3.89 4.27 4.38 s s s q, 7 s t s s s s s d, 9.5 q, 7 m s s s s s9 s s s q, 7 s s m q, 76 s s s m s m sept, 6 q, 7 s ddd CH3 CH3CO CH3 CH2CH3 CH3 CH2(2,6) NCH3 CH3 CH3 ArCH3 CH3 CH3 CH2 CH2(2,5) NCH3 CH2 CH3 CH2 CH3 OCH3 CH3 CH3 CH2 CH3 CH2 CH2 CH2 CH2 CH2 CH2 CH2 ArOCH3 CH2(2,5) CH CH2CH3 CH2 CH2 allyl acetate ethyl acetate dimethyl sulfoxide ethyl methyl ketone dimethylformamide cyclohexanone dimethylacetamide toluene hexamethylbenzene BHT dimethylformamide HMPA triethylamine pyrrolidine dimethylacetamide 1,2-dichloroethane nitromethane dimethyl malonate methanol diglyme 1,2-dimethoxyethane dimethyl malonate diethyl ether dimethyl carbonate 1,2-dimethoxyethane diglyme ethanol 1,4-dioxane 18-crown-6 ethylene glycol diglyme BHA tetrahydrofuran 2-propanol ethyl acetate dichloromethane allyl acetate 4.38 4.47 4.53 4.79 4.92 4.94 4.95 5.01 5.06 5.09 5.25 5.65 5.684 5.72 6.08 6.15 6.37 6.48 6.66 6.90 6.93 6.93–6.99 6.98 7.01–7.07 7.02 7.05 7.13 7.13 7.15 7.16 7.33 7.49–7.53 7.63 7.80 8.53 9.64 ddd s s s ddt ddt dm, 10 dm, 17 ddt ddt s ddt t(nfo ABX) m dd s m m m s s m m m m s dd m s s s m s br t m s CH2 H2 OH5 OH5 CHCH2(2) CHCH2(2) CH2(1) CH2(2) CHCH2(1) CHCH2(1) CH2 CHCH2 CHCH2 CH CH(3,4) CH CH(3,4) CH(2,5) CH(3,5) CH(4,5) ArH CH(3,5) CH(4) CH(4) CH(2,4,6) ArH CH(2,5) CH(3,5) CH CH CH(2) CH(2,6) CH NH CH(2,6) HCO diallyl carbonate hydrogen BHA BHT diallyl carbonate allyl acetate propylene propylene allyl acetate diallyl carbonate ethylene diallyl carbonate allyl acetate propylene furan chloroform pyrrole pyrrole pyridine imidazole BHA benzaldehyde pyridine benzaldehyde toluene BHT furan toluene benzene C6D6 residual imidazole benzaldehyde dimethylformamide pyrrole pyridine benzaldehyde Table S12. C6D6 (13C{1H} NMR data by chemical shift in ppm) shift carbon impurity shift carbon impurity shift carbon impurity shift carbon impurity –4.29 0.20 1.38 2.05 6.96 7.91 12.35 14.19 14.25 14.32 15.46 16.60 16.66 16.95 18.72 19.38 20.37 20.37 20.56 21.10 21.16 21.40 22.72 23.04 25.03 25.18 25.65 25.72 27.00 27.23 28.56 30.14 CH4 CH3 CH3 CH3 CH3 CH2CH3 CH3 CH3 CH3 CH3 CH3 CH2 CH3 CH3 CH3 CH3 CH3 CH3 CH3CO CH3 CH3 CH3Ar CH2(2,4) CH2(2,5) CH2(4) CH3 CH2(3,4) CH2(3,4) CH2(3,5) CH2 CH3CO CH3 methane acetonitrile silicone grease hexamethyldisiloxane ethane ethyl methyl ketone triethylamine ethyl acetate n-pentane n-hexane diethyl ether propane propane hexamethylbenzene ethanol propylene acetic acid allyl acetate ethyl acetate toluene dimethylacetamide BHT n-pentane n-hexane cyclohexanone 2-propanol pyrrolidine tetrahydrofuran cyclohexanone cyclohexane ethyl methyl ketone acetone 30.22 30.24 30.35 30.47 30.72 31.34 31.96 34.35 34.45 34.67 34.72 35.25 36.36 36.88 (d) 37.03 40.03 41.04 41.83 43.59 46.77 46.86 49.97 51.86 53.46 54.30 55.27 57.86 58.66 58.68 60.21 61.16 64.23 CH2 CH2 (CH3)3C (CH3)3C CH3 (CH3)3C CH2(3,4) (CH3)3C CH2(3) NCH3 (CH3)3C CH3 CH2CH3 CH3 NCH3 CH3 CH2 CH2(2,6) CH2 CH2 CH2(2,5) CH3 CH3 CH2 CH3 CH3O CH2 CH3 CH3 CH2 CH3 CH H grease8 pump oil BHA tert-butyl alcohol dimethylformamide BHT n-hexane BHT n-pentane dimethylacetamide BHA dimethylformamide ethyl methyl ketone HMPA11 dimethylacetamide dimethyl sulfoxide dimethyl malonate cyclohexanone 1,2-dichloroethane triethylamine pyrrolidine methanol dimethyl malonate dichloromethane dimethyl carbonate BHA ethanol diglyme 1,2-dimethoxyethane ethyl acetate nitromethane 2-propanol 64.34 64.92 65.94 67.16 67.80 68.19 68.28 70.59 70.87 72.21 72.35 77.79 96.44 108.21 109.67 111.15 115.92 116.02 117.64 117.78 118.22 122.16 122.96 123.58 124.76 125.68 125.83 128.06 (t) 128.52 128.56 128.62 128.95 CH2 CH2 CH2 CH2 CH2(2,5) (CH3)3C CH2 CH2 CH2 CH2 CH2 CH CCl4 CH(3,4) CH(3,4) CH(3,5) CH2 CN CHCH2 CH(2,5) CHCH2 CH(4,5) CH2 CH(3,5) CO2 CH(4) CH(3,5) CD C(4) CH(3,5) CH CH(3,5) ethylene glycol allyl acetate diethyl ether 1,4-dioxane tetrahydrofuran tert-butyl alcohol diallyl carbonate 18-crown-6 diglyme 1,2-dimethoxyethane diglyme chloroform carbon tetrachloride pyrrole furan BHA propylene acetonitrile allyl acetate pyrrole diallyl carbonate imidazole ethylene pyridine carbon dioxide toluene BHT C6D6 signal BHT toluene benzene benzaldehyde 129.33 129.65 131.79 132.18 132.90 133.69 133.95 135.28 135.76 136.08 137.05 137.50 137.91 142.73 148.13 150.27 152.05 153.62 155.24 156.71 162.13 166.66 169.67 169.95 170.44 175.82 191.43 192.69 204.43 206.55 209.10 CH(2,6) CH(2,6) C CHCH2 CHCH2 CH CH (4) CH(4) CH(2) C(2,6) C(1) C(4) C(1) CH(2,5) C(2,6) CH(2,6) C(1) C(1) CO CO CH CO2 CO CO CO CO HCO CS2 CO CO CO toluene benzaldehyde hexamethylbenzene diallyl carbonate allyl acetate propylene benzaldehyde pyridine imidazole BHT benzaldehyde BHA toluene furan BHA pyridine BHT BHA diallyl carbonate dimethyl carbonate dimethylformamide dimethyl malonate allyl acetate dimethylacetamide ethyl acetate acetic acid benzaldehyde carbon disulfide acetone ethyl methyl ketone cyclohexanone S11 Table S13. C6D5Cl (1H NMR data by chemical shift in ppm) shift mult 0.10 0.14 0.15 0.79 0.84 0.84 0.85 0.86–0.92 0.88–0.91 0.89 0.93 1.03 1.04 1.04 1.06 1.10 1.12 1.19 1.21 1.23 1.26 1.30 1.30 1.30 1.31 1.33–1.37 1.37 1.37 1.37 1.39 1.43 1.48–1.53 1.55 1.58 1.74 1.76 1.77 1.78 proton s CH3 s CH3 s CH4 s CH3 t, 7 CH3 t, 7.3 CH3 t, 7 CH3 m CH3 m CH3 t, 7 CH2CH3 t, 7 CH3 s OH t, 7 CH2CH3 d, 6 CH3 t, 7 CH3 t, 7 CH3 s CH3 m CH2 s CH3 m CH2 sept, 7.3 CH2 s OH br s CH2 9 s OH br s CH2 m CH2(4) s ArC(CH3)3 s ArC(CH3)3 s CH2 6 s OH m CH2(3,4) m CH2(3,5) m CH2(3,4) dt, 6.4, 1.5 CH3 s CH3CO s CH3 s CH3 s CH3CO impurity shift mult proton impurity shift mult proton impurity hexamethyldisiloxane silicone grease methane ethane n-pentane propane n-hexane H grease8 pump oil ethyl methyl ketone triethylamine water ethyl acetate 2-propanol ethanol diethyl ether tert-butyl alcohol n-hexane acetonitrile n-pentane propane tert-butyl alcohol H grease8 methanol pump oil cyclohexanone BHA BHT cyclohexane ethanol pyrrolidine cyclohexanone tetrahydrofuran propylene dimethylacetamide acetic acid acetone ethyl acetate 1.78 1.80 2.03 2.06 2.08 2.10 2.16 2.20 2.30 2.39 2.42 2.47 2.51 2.64 2.65 3.15 3.16 3.17 3.25 3.26 3.31 3.37 3.37 3.41 3.41 3.45 3.48 3.49 3.51 3.58 3.59 3.59 3.61 3.82 3.96 4.44 4.46 4.49 s s s q, 7 t s s s s q, 7 s d, 9.5 s m s s s s s9 s q, 7 m s s s s s m q, 76 s s m s sept, 6 q, 7 ddd ddd s CH3CO CH3 CH3 CH2CH3 CH2(2,6) CH3 CH3 ArCH3 CH3 CH2 NCH3 CH3 CH3 CH2(2,5) NCH3 CH2 OCH3 CH3 CH3 CH2 CH2 CH2 CH2 CH2 CH3 CH2 CH3 CH2 CH2 CH2 CH3 CH2(2,5) ArOCH3 CH CH2CH3 CH2 CH2 H2 ethyl methyl ketone allyl acetate dimethyl sulfoxide ethyl methyl ketone cyclohexanone hexamethylbenzene toluene BHT dimethylformamide triethylamine dimethylacetamide HMPA dimethylformamide pyrrolidine dimethylacetamide dimethyl malonate diglyme 1,2-dimethoxyethane methanol 1,2-dichloroethane diethyl ether diglyme 1,2-dimethoxyethane 18-crown-6 dimethyl malonate 1,4-dioxane dimethyl carbonate diglyme ethanol ethylene glycol nitromethane tetrahydrofuran BHA 2-propanol ethyl acetate allyl acetate diallyl carbonate hydrogen 4.62 4.77 4.91 4.98 5.03 5.04 5.15 5.17 5.29 5.50 5.72 5.75 5.77 6.19 6.27 6.62 6.74 6.83 6.90 6.96 6.97 6.99 7.01 7.01–7.08 7.10–7.17 7.14 7.15–7.19 7.20 7.24 7.24–7.28 7.25 7.53 7.59–7.61 7.73 8.51 8.61 9.77 s s dm, 10 dm, 17 ddt ddt ddt ddt s s m ddt ddt dd m m s s m br. s s br. s s m m br. s m s dd m m s m s m br t s OH5 CH2 CH2(1) CH2(2) CHCH2(2) CHCH2(2) CHCH2(1) CHCH2(1) CH2 OH5 CH CHCH2 CHCH2 CH(3,4) CH(3,4) CH(2,5) CH ArH CH(3,5) CH(4) ArH CH(3,5) CH(4,5) CH(2,4,6) CH(3,5) CH(2,6) CH(3,5) CH CH(2,5) CH(4) CH(4) CH(2) CH(2,6) CH CH(2,6) NH HCO BHA dichloromethane propylene propylene diallyl carbonate allyl acetate allyl acetate diallyl carbonate ethylene BHT propylene diallyl carbonate allyl acetate furan pyrrole pyrrole chloroform BHA pyridine C6D5Cl residual BHT C6D5Cl residual imidazole toluene toluene C6D5Cl residual benzaldehyde benzene furan benzaldehyde pyridine imidazole benzaldehyde dimethylformamide pyridine pyrrole benzaldehyde Table S14. C6D5Cl (13C{1H} NMR data by chemical shift in ppm) shift carbon impurity shift carbon impurity shift carbon impurity shift carbon impurity –4.33 0.63 1.09 1.92 6.91 7.79 11.87 14.07 14.10 14.18 15.35 16.48 16.56 16.68 18.55 19.32 20.40 20.40 20.50 21.03 21.10 21.23 22.54 22.86 25.07 25.14 25.59 25.68 26.99 27.02 28.82 30.11 30.11 CH4 CH3 CH3 CH3 CH3 CH2CH3 CH3 CH3 CH3 CH3 CH3 CH2 CH3 CH3 CH3 CH3 CH3 CH3 CH3CO CH3 CH3Ar CH3 CH2(2,4) CH2(2,5) CH2(4) CH3 CH2(3,4) CH2(3,4) CH2 CH2(3,5) CH3CO CH2 CH2 methane acetonitrile silicone grease hexamethyldisiloxane ethane ethyl methyl ketone triethylamine ethyl acetate n-pentane n-hexane diethyl ether propane propane hexamethylbenzene ethanol propylene acetic acid allyl acetate ethyl acetate dimethylacetamide BHT toluene n-pentane n-hexane cyclohexanone 2-propanol pyrrolidine tetrahydrofuran cyclohexane cyclohexanone ethyl methyl ketone H grease8 pump oil 30.12 30.19 30.21 30.71 31.13 31.77 34.11 34.26 34.56 34.59 35.45 36.39 36.64 (d) 37.13 40.27 40.93 41.79 43.60 46.36 46.75 49.66 51.89 53.54 54.23 55.08 57.63 58.31 58.42 60.06 61.68 64.03 64.18 64.86 CH3 (CH3)3C (CH3)3C CH3 (CH3)3C CH2(3,4) (CH3)3C CH2(3) (CH3)3C NCH3 CH3 CH2CH3 CH3 NCH3 CH3 CH2 CH2(2,6) CH2 CH2 CH2(2,5) CH3 CH3 CH2 CH3 CH3O CH2 CH3 CH3 CH2 CH3 CH2 CH CH2 acetone BHT BHA dimethylformamide tert-butyl alcohol n-hexane BHT n-pentane BHA dimethylacetamide dimethylformamide ethyl methyl ketone HMPA11 dimethylacetamide dimethyl sulfoxide dimethyl malonate cyclohexanone 1,2-dichloroethane triethylamine pyrrolidine methanol dimethyl malonate dichloromethane dimethyl carbonate BHA ethanol 1,2-dimethoxyethane diglyme ethyl acetate nitromethane ethylene glycol 2-propanol allyl acetate 65.79 66.95 67.64 68.19 68.19 70.55 70.56 71.81 72.07 77.67 96.38 108.03 109.64 110.84 115.86 115.93 117.63 117.65 118.22 121.96 122.95 123.49 125.43 125.58 125.96 (t) 126.08 128.25 (t) 128.26 128.31 128.38 128.87 129.12 CH2 CH2 CH2(2,5) (CH3)3C CH2 CH2 CH2 CH2 CH2 CH CCl4 CH(3,4) CH(3,4) CH(3,5) CH2 CN CHCH2 CH(2,5) CHCH2 CH(4,5) CH2 CH(3,5) CH(4) CH(3,5) CD(4) CO2 CD(3,5) C(4) CH(3,5) CH CH(3,5) CH(2,6) diethyl ether 1,4-dioxane tetrahydrofuran tert-butyl alcohol diallyl carbonate 18-crown-6 diglyme 1,2-dimethoxyethane diglyme chloroform carbon tetrachloride pyrrole furan BHA propylene acetonitrile allyl acetate pyrrole diallyl carbonate imidazole ethylene pyridine toluene BHT C6D5Cl signal carbon dioxide C6D5Cl signal BHT toluene benzene benzaldehyde toluene 129.26 (t) 129.49 131.54 131.93 132.69 133.57 134.02 134.19 135.32 135.50 135.92 136.78 137.29 137.65 142.49 147.87 149.93 151.69 153.19 154.87 156.36 162.01 166.51 169.59 169.79 170.20 175.67 191.24 192.49 204.83 206.87 209.30 CD(2,6) CH(2,6) C CHCH2 CHCH2 CH CH (4) CCl CH(4) CH(2) C(2,6) C(1) C(4) C(1) CH(2,5) C(2,6) CH(2,6) C(1) C(1) CO CO CH CO2 CO CO CO CO HCO CS2 CO CO CO C6D5Cl signal benzaldehyde hexamethylbenzene diallyl carbonate allyl acetate propylene benzaldehyde C6D5Cl signal pyridine imidazole BHT benzaldehyde BHA toluene furan BHA pyridine BHT BHA diallyl carbonate dimethyl carbonate dimethylformamide dimethyl malonate allyl acetate dimethylacetamide ethyl acetate acetic acid benzaldehyde carbon disulfide acetone ethyl methyl ketone cyclohexanone S12 Table S15. (CD3)2CO (1H NMR data by chemical shift in ppm) shift mult 0.07 0.13 0.17 0.83 0.87 0.88 0.88 0.88 0.90 0.96 0.96 1.10 1.11 1.12 1.18 1.20 1.27 1.28 1.29 1.29 1.31 1.41 1.41 1.43 1.68 1.70–1.74 1.79 1.79–1.83 1.96 1.97 1.97 2.02 2.05 2.05 2.07 2.09 proton s CH3 s CH3 s CH4 s CH3 m CH3 t, 7 CH3 t, 7 CH3 t, 7.3 CH3 m CH3 t, 7 CH2CH3 t, 7 CH3 d, 6 CH3 t, 7 CH3 t, 7 CH3 s CH3 t, 7 CH2CH3 m CH2 m CH2 br s CH2 br s CH2 sept, 7.3 CH2 s ArC(CH3)3 s ArC(CH3)3 s CH2 dt, 6.4, 1.5 CH3 m CH2(4) m CH2(3,4) m CH2(3,5) s CH3 s CH3CO s CH3CO s CH3 s CH3 p CHD2 s CH3CO s CH3 impurity shift mult proton impurity shift mult proton impurity hexamethyldisiloxane silicone grease methane ethane pump oil n-hexane n-pentane propane H grease8 ethyl methyl ketone triethylamine 2-propanol diethyl ether ethanol tert-butyl alcohol ethyl acetate n-pentane n-hexane H grease8 pump oil propane BHA BHT cyclohexane propylene cyclohexanone tetrahydrofuran cyclohexanone acetic acid dimethylacetamide ethyl acetate allyl acetate acetonitrile (CD3)2CO residual ethyl methyl ketone acetone 2.17 2.22 2.27 2.32 2.45 2.45 2.52 2.59 2.78 2.83 2.843 2.94 3.00 3.12 3.28 3.28 3.28 3.31 3.39 3.41 3.42 3.46 3.47 3.56 3.57 3.59 3.59 3.63 3.68 3.72 3.72 3.87 3.90 4.05 4.43 4.53 s s t s q, 7 q, 7 s d, 9.5 s s s s s s9 s s s s9 s6 q, 7 s s m m q, 76 s s m s s s s sept, 6 q, 7 s ddd CH3 ArCH3 CH2(2,6) CH3 CH2CH3 CH2 CH3 CH3 CH3 NCH3 OH CH3 NCH3 OH OCH3 CH3 CH2 CH3 OH CH2 CH2 CH2 CH2 CH2 CH2 CH2 CH2 CH2(2,5) CH3 ArOCH3 CH3 CH2 CH CH2CH3 CH3 CH2 hexamethylbenzene BHT cyclohexanone toluene ethyl methyl ketone triethylamine dimethyl sulfoxide HMPA dimethylformamide dimethylacetamide water dimethylformamide dimethylacetamide methanol diglyme 1,2-dimethoxyethane ethylene glycol methanol ethanol diethyl ether dimethyl malonate 1,2-dimethoxyethane diglyme diglyme ethanol 18-crown-6 1,4-dioxane tetrahydrofuran dimethyl malonate BHA dimethyl carbonate 1,2-dichloroethane 2-propanol ethyl acetate nitromethane allyl acetate 4.54 4.62 4.90 5.00 5.18 5.23 5.29 5.35 5.38 5.63 5.65 5.81 5.92 5.96 6.07 6.43 6.72 6.77 6.96 7.04 7.10–7.20 7.10–7.20 7.35 7.36 7.56 7.59–7.63 7.62 7.69–7.73 7.76 7.92–7.94 7.96 8.02 8.58 10.02 10.05 s ddd dm, 10 dm, 17 ddt ddt ddt ddt s s s m ddt ddt m dd s m s s m m m s dd m s m m m s s m br t s H2 CH2 CH2(1) CH2(2) CHCH2(2) CHCH2(2) CHCH2(1) CHCH2(1) CH2 CH2 OH5 CH CHCH2 CHCH2 CH(3,4) CH(3,4) ArH CH(2,5) ArH CH(4,5) CH(2,4,6) CH(3,5) CH(3,5) CH CH(2,5) CH(3,5) CH(2) CH(4) CH(4) CH(2,6) CH CH CH(2,6) NH HCO hydrogen diallyl carbonate propylene propylene allyl acetate diallyl carbonate allyl acetate diallyl carbonate ethylene dichloromethane BHA propylene allyl acetate diallyl carbonate pyrrole furan BHA pyrrole BHT imidazole toluene toluene pyridine benzene furan benzaldehyde imidazole benzaldehyde pyridine benzaldehyde dimethylformamide chloroform pyridine pyrrole benzaldehyde Table S16. (CD3)2CO (13C{1H} NMR data by chemical shift in ppm) shift carbon impurity shift carbon impurity shift carbon impurity shift carbon impurity –5.33 1.12 1.40 2.01 6.88 8.03 12.49 14.29 14.34 14.50 15.78 16.68 16.78 16.86 18.89 19.42 20.51 20.68 20.83 21.31 21.46 21.51 22.98 23.28 25.59 25.67 26.15 27.51 27.68 29.30 29.84 (sept) 30.36 CH4 CH3 CH3 CH3 CH3 CH2CH3 CH3 CH3 CH3 CH3 CH3 CH3 CH2 CH3 CH3 CH3 CH3 CH3 CH3CO CH3Ar CH3 CH3 CH2(2,4) CH2(2,5) CH2(4) CH3 CH2(3,4) CH2 CH2(3,5) CH3CO CD3 CH2 methane acetonitrile silicone grease hexamethyldisiloxane ethane ethyl methyl ketone triethylamine n-pentane n-hexane ethyl acetate diethyl ether propane propane hexamethylbenzene ethanol propylene acetic acid allyl acetate ethyl acetate BHT toluene dimethylacetamide n-pentane n-hexane cyclohexanone 2-propanol tetrahydrofuran cyclohexane cyclohexanone ethyl methyl ketone (CD3)2CO signal pump oil 30.60 30.64 30.72 31.03 31.61 32.30 34.83 34.89 35.00 35.45 36.15 36.75 37.04 (d) 37.92 41.23 41.43 42.24 45.25 47.07 49.77 52.47 54.95 54.95 55.51 57.72 58.45 58.77 60.56 63.21 63.85 64.26 CH3 (CH3)3C (CH3)3C CH3 (CH3)3C CH2(3,4) CH2(3) NCH3 (CH3)3C (CH3)3C CH3 CH2CH3 CH3 NCH3 CH3 CH2 CH2(2,6) CH2 CH2 CH3 CH3 CH2 CH3 CH3O CH2 CH3 CH3 CH2 CH3 CH CH2 acetone BHA tert-butyl alcohol dimethylformamide BHT n-hexane n-pentane dimethylacetamide BHT BHA dimethylformamide ethyl methyl ketone HMPA11 dimethylacetamide dimethyl sulfoxide dimethyl malonate cyclohexanone 1,2-dichloroethane triethylamine methanol dimethyl malonate dichloromethane dimethyl carbonate BHA ethanol 1,2-dimethoxyethane diglyme ethyl acetate nitromethane 2-propanol ethylene glycol 65.28 66.12 67.60 68.07 68.13 68.78 71.03 71.25 72.47 72.63 79.19 96.65 108.04 110.24 111.00 116.03 117.60 117.81 117.98 118.53 122.31 123.47 124.57 125.81 126.03 126.12 129.03 129.05 129.15 129.76 129.90 CH2 CH2 CH2 CH2(2,5) (CH3)3C CH2 CH2 CH2 CH2 CH2 CH CCl4 CH(3,4) CH(3,4) CH(3,5) CH2 CN CHCH2 CH(2,5) CHCH2 CH(4,5) CH2 CH(3,5) CO2 CH(3,5) CH(4) CH(3,5) C(4) CH CH(2,6) CH(3,5) allyl acetate diethyl ether 1,4-dioxane tetrahydrofuran tert-butyl alcohol diallyl carbonate diglyme 18-crown-6 1,2-dimethoxyethane diglyme chloroform carbon tetrachloride pyrrole furan BHA propylene acetonitrile allyl acetate pyrrole diallyl carbonate imidazole ethylene pyridine carbon dioxide BHT toluene toluene BHT benzene toluene benzaldehyde 130.23 132.22 133.16 133.76 134.34 135.14 135.89 136.56 137.66 138.19 138.48 140.32 143.49 148.48 150.67 152.51 153.97 155.48 157.04 162.79 167.58 170.61 170.61 170.96 172.31 192.95 193.58 205.87 206.26 208.30 210.36 CH(2,6) C CHCH2 CHCH2 CH CH (4) CH(2) CH(4) C(1) C(2,6) C(1) C(4) CH(2,5) C(2,6) CH(2,6) C(1) C(1) CO CO CH CO2 CO CO CO CO HCO CS2 CO CO CO CO benzaldehyde hexamethylbenzene diallyl carbonate allyl acetate propylene benzaldehyde imidazole pyridine benzaldehyde BHT toluene BHA furan BHA pyridine BHT BHA diallyl carbonate dimethyl carbonate dimethylformamide dimethyl malonate allyl acetate dimethylacetamide ethyl acetate acetic acid benzaldehyde carbon disulfide acetone (CD3)2CO signal ethyl methyl ketone cyclohexanone S13 Table S17. (CD3)2SO (1H NMR data by chemical shift in ppm) shift mult –0.06 0.06 0.20 0.74 0.82 0.82–0.88 0.86 0.86 0.87 0.91 0.93 1.04 1.06 1.09 1.11 1.15 1.17 1.24 1.25 1.27 1.29 1.36 1.36 1.40 1.55 1.64–1.66 1.68 1.74–1.78 1.76 1.91 1.96 1.99 2.03 2.07 2.07 2.09 2.14 proton s CH3 s CH3 s CH4 m CH3 s CH3 m CH3 t, 7 CH3 t, 7 CH3 t, 7.3 CH3 t, 7 CH2CH3 t, 7 CH3 d, 6 CH3 t, 7 CH3 t, 7 CH3 s CH3 br s CH2 t, 7 CH2CH3 br s CH2 m CH2 m CH2 sept, 7.3 CH2 s ArC(CH3)3 s ArC(CH3)3 s CH2 m CH2(3,4) m CH2(4) dt, 6.4, 1.5 CH3 m CH2(3,5) m CH2(3,4) s CH3 s CH3CO s CH3CO s CH3 s CH3 s CH3CO s CH3 s CH3 impurity shift mult proton impurity shift mult proton impurity silicone grease hexamethyldisiloxane methane pump oil ethane H grease8 n-hexane n-pentane propane ethyl methyl ketone triethylamine 2-propanol ethanol diethyl ether tert-butyl alcohol pump oil ethyl acetate H grease8 n-hexane n-pentane propane BHA BHT cyclohexane pyrrolidine cyclohexanone propylene cyclohexanone tetrahydrofuran acetic acid dimethylacetamide ethyl acetate allyl acetate acetonitrile ethyl methyl ketone acetone hexamethylbenzene 2.18 2.25 2.30 2.43 2.43 2.50 2.53 2.54 2.67 2.73 2.78 2.89 2.94 3.16 3.24 3.24 3.333 3.34 3.38 3.38 3.43 3.44 3.51 3.51 3.53 3.57 3.60 3.65 3.66 3.69 3.78 3.90 4.01 4.03 4.19 4.42 4.52 s t s q, 7 q, 7 p d, 9.5 s m s s s s s9 s s s s q, 7 m s q, 76 s m s s m s s s sept, 6 s s9 q, 7 s s ddd ArCH3 CH2(2,6) CH3 CH2CH3 CH2 CHD2 CH3 CH3 CH2(2,5) CH3 NCH3 CH3 NCH3 CH3 OCH3 CH3 OH CH2 CH2 CH2 CH2 CH2 CH2 CH2 CH2 CH2 CH2(2,5) CH3 ArOCH3 CH3 CH CH2 OH CH2CH3 OH CH3 CH2 BHT cyclohexanone toluene ethyl methyl ketone triethylamine (CD3)2SO residual HMPA dimethyl sulfoxide pyrrolidine dimethylformamide dimethylacetamide dimethylformamide dimethylacetamide methanol diglyme 1,2-dimethoxyethane water ethylene glycol diethyl ether diglyme 1,2-dimethoxyethane ethanol 18-crown-6 diglyme dimethyl malonate 1,4-dioxane tetrahydrofuran dimethyl malonate BHA dimethyl carbonate 2-propanol 1,2-dichloroethane methanol ethyl acetate tert-butyl alcohol nitromethane allyl acetate 4.61 4.61 4.63 4.94 5.03 5.20 5.25 5.29 5.33 5.41 5.76 5.80 5.91 5.93 6.01 6.47 6.52 6.62 6.65 6.73 6.87 7.01 7.18 7.25 7.37 7.39 7.61–7.67 7.63 7.67 7.69–7.75 7.79 7.91–7.93 8.32 8.58 10.02 10.75 ddd s s6 dm, 10 dm, 17 ddt ddt ddt ddt s s m ddt ddt m dd s s s m s s m m s m m s dd m m m s m s br t CH2 H2 OH CH2(1) CH2(2) CHCH2(2) CHCH2(2) CHCH2(1) CHCH2(1) CH2 CH2 CH CHCH2 CHCH2 CH(3,4) CH(3,4) OH5 ArH OH5 CH(2,5) ArH CH(4,5) CH(2,4,6) CH(3,5) CH CH(3,5) CH(3,5) CH(2) CH(2,5) CH(4) CH(4) CH(2,6) CH CH(2,6) HCO NH diallyl carbonate hydrogen ethanol propylene propylene allyl acetate diallyl carbonate allyl acetate diallyl carbonate ethylene dichloromethane propylene allyl acetate diallyl carbonate pyrrole furan BHA BHA BHT pyrrole BHT imidazole toluene toluene benzene pyridine benzaldehyde imidazole furan benzaldehyde pyridine benzaldehyde chloroform pyridine benzaldehyde pyrrole Table S18. (CD3)2SO (13C{1H} NMR data by chemical shift in ppm) shift carbon –4.01 1.03 1.96 6.61 7.61 11.74 13.28 13.88 14.40 15.12 15.67 16.34 16.60 18.51 19.20 20.54 20.68 20.95 20.97 20.99 21.29 21.70 22.05 24.32 25.14 25.26 25.43 26.33 26.46 29.26 29.33 30.30 CH4 CH3 CH3 CH3 CH2CH3 CH3 CH3 CH3 CH3 CH3 CH2 CH3 CH3 CH3 CH3 CH3 CH3CO CH3 CH3Ar CH3 CH3 CH2(2,4) CH2(2,5) CH2(4) CH2(3,4) CH2(3,4) CH3 CH2 CH2(3,5) CH3CO CH2 (CH3)3C S14 impurity shift methane 30.38 acetonitrile 30.56 hexamethyldisiloxane 30.73 ethane 30.95 ethyl methyl ketone 31.25 triethylamine 33.48 n-pentane 34.33 n-hexane 34.42 ethyl acetate 34.76 diethyl ether 35.73 propane 35.83 propane 36.42 (d) hexamethylbenzene 37.38 ethanol 39.52 (sept) propylene 40.45 allyl acetate 40.72 ethyl acetate 41.32 acetic acid 45.02 BHT 45.74 toluene 46.51 dimethylacetamide 48.59 n-pentane 52.08 n-hexane 54.63 cyclohexanone 54.84 tetrahydrofuran 54.89 pyrrolidine 56.07 2-propanol 57.98 cyclohexane 58.03 cyclohexanone 59.74 ethyl methyl ketone 62.05 pump oil 62.76 BHA carbon impurity shift carbon impurity shift carbon impurity (CH3)3C CH3 CH3 CH2(3,4) (CH3)3C CH2(3) (CH3)3C NCH3 (CH3)3C CH3 CH2CH3 CH3 NCH3 CD3 CH3 CH2 CH2(2,6) CH2 CH2 CH2(2,5) CH3 CH3 CH3 CH2 CH3O CH2 CH3 CH3 CH2 CH2 CH2 tert-butyl alcohol acetone dimethylformamide n-hexane BHT n-pentane BHT dimethylacetamide BHA dimethylformamide ethyl methyl ketone HMPA11 dimethylacetamide (CD3)2SO signal dimethyl sulfoxide dimethyl malonate cyclohexanone 1,2-dichloroethane triethylamine pyrrolidine methanol dimethyl malonate dimethyl carbonate dichloromethane BHA ethanol diglyme 1,2-dimethoxyethane ethyl acetate diethyl ether ethylene glycol 63.28 64.32 64.92 66.36 66.88 67.03 67.86 69.54 69.85 71.17 71.25 79.16 95.44 107.07 109.62 109.80 116.07 117.32 117.64 117.91 118.32 121.55 123.52 123.84 124.21 124.85 125.29 127.97 128.18 128.30 128.88 CH3 CH2 CH CH2 (CH3)3C CH2(2,5) CH2 CH2 CH2 CH2 CH2 CH CCl4 CH(3,4) CH(3,4) CH(3,5) CH2 CH(2,5) CHCH2 CN CHCH2 CH(4,5) CH2 CH(3,5) CO2 CH(3,5) CH(4) C(4) CH(3,5) CH CH(2,6) nitromethane allyl acetate 2-propanol 1,4-dioxane tert-butyl alcohol tetrahydrofuran diallyl carbonate diglyme 18-crown-6 1,2-dimethoxyethane diglyme chloroform carbon tetrachloride pyrrole furan BHA propylene pyrrole allyl acetate acetonitrile diallyl carbonate imidazole ethylene pyridine carbon dioxide BHT toluene BHT toluene benzene toluene 129.10 129.45 131.10 132.18 132.71 133.55 134.52 135.15 136.05 136.20 137.35 139.12 141.16 142.82 147.44 149.58 151.47 152.53 154.16 155.76 162.29 166.91 169.54 169.97 170.31 171.93 192.63 193.08 206.31 208.72 210.63 CH(3,5) CH(2,6) C CHCH2 CHCH2 CH CH (4) CH(2) CH(4) C(1) C(1) C(2,6) C(4) CH(2,5) C(2,6) CH(2,6) C(1) C(1) CO CO CH CO2 CO CO CO CO CS2 HCO CO CO CO benzaldehyde benzaldehyde hexamethylbenzene diallyl carbonate allyl acetate propylene benzaldehyde imidazole pyridine benzaldehyde toluene BHT BHA furan BHA pyridine BHT BHA diallyl carbonate dimethyl carbonate dimethylformamide dimethyl malonate dimethylacetamide allyl acetate ethyl acetate acetic acid carbon disulfide benzaldehyde acetone ethyl methyl ketone cyclohexanone Table S19. CD3CN (1H NMR data by chemical shift in ppm) shift mult 0.07 0.08 0.20 0.85 0.85 0.89 0.89 0.90 0.96 0.96 1.09 1.12 1.12 1.16 1.20 1.27 1.28 1.29 1.33 1.39 1.40 1.44 1.61 1.67–1.72 1.70 1.79–1.84 1.80 1.94 1.96 1.96 1.97 1.97 2.02 2.06 2.08 2.13 2.16 proton s CH3 s CH3 s CH4 s CH3 m CH3 t, 7 CH3 t, 7 CH3 t, 7.3 CH3 t, 7 CH2CH3 t, 7 CH3 d, 6 CH3 t, 7 CH3 t, 7 CH3 s CH3 t, 7 CH2CH3 br s CH2 m CH2 m CH2 sept, 7.3 CH2 s ArC(CH3)3 s ArC(CH3)3 s CH2 m CH2(3,4) m CH2(4) dt, 6.4, 1.5 CH3 m CH2(3,5) m CH2(3,4) p CHD2 s CH3 s CH3 s CH3CO s CH3CO s CH3 s CH3CO s CH3 s OH 9 s OH impurity shift mult proton impurity shift mult proton impurity hexamethyldisiloxane silicone grease methane ethane pump oil n-hexane n-pentane propane ethyl methyl ketone triethylamine 2-propanol diethyl ether ethanol tert-butyl alcohol ethyl acetate pump oil n-hexane n-pentane propane BHT BHA cyclohexane pyrrolidine cyclohexanone propylene cyclohexanone tetrahydrofuran CD3CN residual acetic acid acetonitrile dimethylacetamide ethyl acetate allyl acetate ethyl methyl ketone acetone water methanol 2.18 2.19 2.22 2.27 2.33 2.43 2.45 2.47 2.50 2.57 2.697 2.75 2.77 2.83 2.89 2.96 3.28 3.28 3.29 3.38 3.42 3.45 3.45 3.51 3.51 3.53 3.54 3.60 3.64 3.68 3.72 3.72 3.81 3.87 4.06 4.31 4.53 s s s t s q, 7 q, 7 s6 s d, 9.5 m7 m s s s s s s9 s s q, 7 m s s m7 m q, 76 s m s s s s sept, 6 q, 7 s ddd OH CH3 ArCH3 CH2(2,6) CH3 CH2CH3 CH2 OH CH3 CH3 OH7 CH2(2,5) CH3 NCH3 CH3 NCH3 CH3 CH3 OCH3 CH2 CH2 CH2 CH2 CH2 CH2 CH2 CH2 CH2 CH2(2,5) CH3 ArOCH3 CH3 CH2 CH CH2CH3 CH3 CH2 tert-butyl alcohol hexamethylbenzene BHT cyclohexanone toluene ethyl methyl ketone triethylamine ethanol dimethyl sulfoxide HMPA ethylene glycol7 pyrrolidine dimethylformamide dimethylacetamide dimethylformamide dimethylacetamide 1,2-dimethoxyethane methanol diglyme dimethyl malonate diethyl ether diglyme 1,2-dimethoxyethane 18-crown-6 ethylene glycol diglyme ethanol 1,4-dioxane tetrahydrofuran dimethyl malonate BHA dimethyl carbonate 1,2-dichloroethane 2-propanol ethyl acetate nitromethane allyl acetate 4.57 4.61 4.93 4.98 5.04 5.20 5.21 5.25 5.29 5.34 5.41 5.44 5.85 5.93 5.96 6.10 6.44 6.73 6.75 6.97 7.01 7.10–7.30 7.10–7.30 7.33 7.37 7.52 7.57 7.57–7.61 7.58 7.67–7.71 7.73 7.89–7.91 7.92 8.57 9.27 10.01 s ddd dm, 10 s dm, 17 s ddt ddt ddt ddt s s m ddt ddt m dd s m s s m m m s dd s m s m m m s m br t s H2 CH2 CH2(1) OH5 CH2(2) OH5 CHCH2(2) CHCH2(2) CHCH2(1) CHCH2(1) CH2 CH2 CH CHCH2 CHCH2 CH(3,4) CH(3,4) ArH CH(2,5) ArH CH(4,5) CH(2,4,6) CH(3,5) CH(3,5) CH CH(2,5) CH(2) CH(3,5) CH CH(4) CH(4) CH(2,6) CH CH(2,6) NH HCO hydrogen diallyl carbonate propylene BHA propylene BHT allyl acetate diallyl carbonate allyl acetate diallyl carbonate ethylene dichloromethane propylene allyl acetate diallyl carbonate pyrrole furan BHA pyrrole BHT imidazole toluene toluene pyridine benzene furan imidazole benzaldehyde chloroform benzaldehyde pyridine benzaldehyde dimethylformamide pyridine pyrrole benzaldehyde Table S20. CD3CN (13C{1H} NMR data by chemical shift in ppm) shift carbon impurity shift carbon impurity shift carbon impurity shift carbon impurity –4.61 1.32 (sept) 1.79 2.07 6.99 8.14 12.38 14.37 14.43 14.54 15.63 16.73 16.91 16.94 18.80 19.48 20.73 21.02 21.16 21.23 21.50 21.76 23.08 23.40 25.55 25.62 26.27 26.34 27.63 27.80 29.60 30.55 CH4 CD3 CH3 CH3 CH3 CH2CH3 CH3 CH3 CH3 CH3 CH3 CH3 CH2 CH3 CH3 CH3 CH3 CH3 CH3CO CH3Ar CH3 CH3 CH2(2,4) CH2(2,5) CH3 CH2(4) CH2(3,4) CH2(3,4) CH2 CH2(3,5) CH3CO (CH3)3C methane CD3CN signal acetonitrile hexamethyldisiloxane ethane ethyl methyl ketone triethylamine n-pentane n-hexane ethyl acetate diethyl ether propane propane hexamethylbenzene ethanol propylene acetic acid allyl acetate ethyl acetate BHT toluene dimethylacetamide n-pentane n-hexane 2-propanol cyclohexanone tetrahydrofuran pyrrolidine cyclohexane cyclohexanone ethyl methyl ketone BHA 30.68 30.86 30.91 31.32 31.50 32.36 34.89 35.05 35.17 35.48 36.57 37.09 37.10 (d) 38.26 41.31 41.77 42.44 45.54 47.10 47.57 49.90 52.95 55.32 55.39 55.94 57.96 58.89 58.90 60.98 63.66 64.22 64.30 (CH3)3C CH2 CH3 CH3 (CH3)3C CH2(3,4) CH2(3) (CH3)3C NCH3 (CH3)3C CH3 CH2CH3 CH3 NCH3 CH3 CH2 CH2(2,6) CH2 CH2 CH2(2,5) CH3 CH3 CH2 CH3 CH3O CH2 CH3 CH3 CH2 CH3 CH2 CH tert-butyl alcohol pump oil acetone dimethylformamide BHT n-hexane n-pentane BHT dimethylacetamide BHA dimethylformamide ethyl methyl ketone HMPA11 dimethylacetamide dimethyl sulfoxide dimethyl malonate cyclohexanone 1,2-dichloroethane triethylamine pyrrolidine methanol dimethyl malonate dichloromethane dimethyl carbonate BHA ethanol 1,2-dimethoxyethane diglyme ethyl acetate nitromethane ethylene glycol 2-propanol 65.55 66.32 67.72 68.33 68.74 69.09 70.99 71.22 72.47 72.63 79.17 96.68 108.31 110.49 111.35 116.12 118.06 118.26 118.26 118.47 118.86 122.78 123.69 125.89 126.28 126.38 127.76 129.23 129.32 129.61 129.94 CH2 CH2 CH2 CH2(2,5) (CH3)3C CH2 CH2 CH2 CH2 CH2 CH CCl4 CH(3,4) CH(3,4) CH(3,5) CH2 CHCH2 CN CN CH(2,5) CHCH2 CH(4,5) CH2 CO2 CH(4) CH(3,5) CH(3,5) CH(3,5) CH C(4) CH(2,6) allyl acetate diethyl ether 1,4-dioxane tetrahydrofuran tert-butyl alcohol diallyl carbonate diglyme 18-crown-6 1,2-dimethoxyethane diglyme chloroform carbon tetrachloride pyrrole furan BHA propylene allyl acetate CD3CN signal acetonitrile pyrrole diallyl carbonate imidazole ethylene carbon dioxide toluene BHT pyridine toluene benzene BHT toluene 130.07 130.42 132.61 133.20 133.83 134.78 135.40 136.33 136.89 137.62 138.13 138.90 140.20 143.74 148.39 150.76 152.42 154.02 155.66 157.26 163.31 168.07 171.31 171.32 171.68 173.21 193.60 193.64 207.43 209.88 211.99 CH(3,5) CH(2,6) C CHCH2 CHCH2 CH CH (4) CH(2) CH(4) C(1) C(2,6) C(1) C(4) CH(2,5) C(2,6) CH(2,6) C(1) C(1) CO CO CH CO2 CO CO CO CO CS2 HCO CO CO CO benzaldehyde benzaldehyde hexamethylbenzene diallyl carbonate allyl acetate propylene benzaldehyde imidazole pyridine benzaldehyde BHT toluene BHA furan BHA pyridine BHT BHA diallyl carbonate dimethyl carbonate dimethylformamide dimethyl malonate dimethylacetamide allyl acetate ethyl acetate acetic acid carbon disulfide benzaldehyde acetone ethyl methyl ketone cyclohexanone S15 Table S21. TFE-d3 (1H NMR data by chemical shift in ppm) shift mult 0.08 0.16 0.18 0.85 0.88–0.94 0.90 0.90 0.91 0.99 1.05 1.20 1.20 1.22 1.26 1.28 1.31 1.31 1.33 1.33 1.33 1.41 1.43 1.44 1.47 1.70 1.75–1.78 1.87–1.92 1.91 1.93 1.95 2.03 2.06 2.07 2.09 2.16 2.19 proton s CH3 s CH3 s CH4 s CH3 m CH3 t, 7 CH3 t, 7.3 CH3 t, 7 CH3 m CH3 t, 7 CH2CH3 t, 7 CH3 d, 6 CH3 t, 7 CH3 t, 7 CH2CH3 s CH3 m CH2 t, 7 CH3 br s CH2 m CH2 sept, 7.3 CH2 br s CH2 s ArC(CH3)3 s ArC(CH3)3 s CH2 dt, 6.4, 1.5 CH3 m CH2(4) m CH2(3,5) m CH2(3,4) m CH2(3,4) s CH3 s CH3CO s CH3 s CH3 s CH3CO s CH3CO s CH3 impurity shift mult proton impurity shift mult proton impurity hexamethyldisiloxane silicone grease methane ethane H grease8 n-pentane propane n-hexane pump oil ethyl methyl ketone diethyl ether 2-propanol ethanol ethyl acetate tert-butyl alcohol n-hexane triethylamine H grease8 n-pentane propane pump oil BHT BHA cyclohexane propylene cyclohexanone cyclohexanone tetrahydrofuran pyrrolidine acetonitrile ethyl acetate acetic acid allyl acetate dimethylacetamide ethyl methyl ketone acetone 2.20 2.24 2.24 2.33 2.38 2.49 2.63 2.63 2.88 2.94 2.98 3.05 3.11 3.12 3.40 3.41 3.41 3.44 3.58 3.61 3.62 3.64 3.66 3.67 3.71 3.71 3.72 3.76 3.76 3.77 3.78 3.79 3.88 4.05 4.14 4.28 s s s s t q, 7 s d, 9.5 s s s s m q, 7 s s s s q, 7 s m s s m s q, 7 s s s s m s tq sept, 6 q, 7 s OH ArCH3 CH3 CH3 CH2(2,6) CH2CH3 CH3 CH3 CH3 NCH3 CH3 NCH3 CH2(2,5) CH2 CH3 OCH3 CH2 CH3 CH2 CH2 CH2 CH2 OH CH2 CH2 CH2 CH2 CH3 CH2 CH3 CH2(2,5) ArOCH3 CDH CH CH2CH3 CH3 tert-butyl alcohol BHT hexamethylbenzene toluene cyclohexanone ethyl methyl ketone dimethyl sulfoxide HMPA dimethylformamide dimethylacetamide dimethylformamide dimethylacetamide pyrrolidine triethylamine 1,2-dimethoxyethane diglyme dimethyl malonate methanol diethyl ether 1,2-dimethoxyethane diglyme 18-crown-6 water diglyme 1,2-dichloroethane ethanol ethylene glycol dimethyl malonate 1,4-dioxane dimethyl carbonate tetrahydrofuran BHA TFE-d3 residual 2-propanol ethyl acetate nitromethane 4.53 4.58 4.62 4.93 5.02 5.03 5.24 5.25 5.28 5.32 5.35 5.40 5.87 5.92 5.93 6.24 6.42 6.84 6.87 7.03 7.06 7.10–7.30 7.10–7.30 7.33 7.36 7.40 7.44 7.56–7.59 7.61 7.68–7.72 7.82 7.86 7.90–7.92 8.45 9.88 s ddd ddd dm, 10 s dm, 17 s ddt ddt ddt ddt s m ddt ddt m dd m s s s m m s s m dd m s m m s m m s H2 CH2 CH2 CH2(1) OH CH2(2) CH2 CHCH2(2) CHCH2(2) CHCH2(1) CHCH2(1) CH2 CH CHCH2 CHCH2 CH(3,4) CH(3,4) CH(2,5) ArH CH(4,5) ArH CH(2,4,6) CH(3,5) CH CH CH(3,5) CH(2,5) CH(3,5) CH(2) CH(4) CH(4) CH CH(2,6) CH(2,6) HCO hydrogen allyl acetate diallyl carbonate propylene TFE-d3 residual propylene dichloromethane allyl acetate diallyl carbonate allyl acetate diallyl carbonate ethylene propylene diallyl carbonate allyl acetate pyrrole furan pyrrole BHA imidazole BHT toluene toluene chloroform benzene pyridine furan benzaldehyde imidazole benzaldehyde pyridine dimethylformamide benzaldehyde pyridine benzaldehyde Table S22. TFE-d3 (13C{1H} NMR data by chemical shift in ppm) shift carbon impurity shift carbon impurity shift carbon impurity shift carbon impurity –5.88 1.00 2.09 2.87 7.01 8.29 9.51 14.36 14.54 14.63 15.33 16.93 17.04 17.46 18.11 19.63 20.91 21.10 21.18 21.34 21.40 21.62 23.75 24.06 25.21 25.73 26.00 26.69 28.34 28.56 29.64 30.80 CH4 CH3 CH3 CH3 CH3 CH2CH3 CH3 CH3 CH3 CH3 CH3 CH3 CH3 CH2 CH3 CH3 CH3 CH3 CH3CO CH3Ar CH3 CH3 CH2(2,4) CH2(2,5) CH3 CH2(3,4) CH2(4) CH2(3,4) CH2 CH2(3,5) CH3CO (CH3)3C methane acetonitrile hexamethyldisiloxane silicone grease ethane ethyl methyl ketone triethylamine ethyl acetate n-pentane n-hexane diethyl ether propane hexamethylbenzene propane ethanol propylene acetic acid allyl acetate ethyl acetate BHT dimethylacetamide toluene n-pentane n-hexane 2-propanol pyrrolidine cyclohexanone tetrahydrofuran cyclohexane cyclohexanone ethyl methyl ketone BHA 30.96 31.01 31.07 31.85 32.35 33.17 35.69 35.76 36.07 36.28 37.21 (d) 37.76 38.23 39.06 40.06 42.13 43.16 45.28 47.43 48.45 50.67 54.00 54.46 56.17 57.55 59.40 59.52 59.68 61.5 (qp) 62.70 63.17 64.87 CH3 (CH3)3C (CH3)3C CH2 CO CH2(3,4) (CH3)3C CH2(3) (CH3)3C NCH3 CH3 CH3 CH2CH3 NCH3 CH3 CH2 CH2(2,6) CH2 CH2(2,5) CH2 CH3 CH3 CH2 CH3 CH3O CH3 CH3 CH2 CD2 CH2 CH3 CH2 dimethylformamide BHT tert-butyl alcohol pump oil acetone n-hexane BHT n-pentane BHA dimethylacetamide HMPAi dimethylformamide ethyl methyl ketone dimethylacetamide dimethyl sulfoxide dimethyl malonate cyclohexanone 1,2-dichloroethane pyrrolidine triethylamine methanol dimethyl malonate dichloromethane dimethyl carbonate BHA diglyme 1,2-dimethoxyethane ethanol TFE-d3 signal ethyl acetate nitromethane ethylene glycol 66.69 67.55 67.61 68.52 69.53 70.69 70.80 71.33 72.35 72.87 73.05 78.83 97.74 108.85 111.06 112.90 116.38 118.95 119.39 119.61 120.15 122.93 124.08 126.27 126.28 (q) 126.82 126.92 127.11 129.79 129.84 130.58 130.62 CH CH2 CH2 CH2 CH2(2,5) CH2 CH2 CH2 (CH3)3C CH2 CH2 CH CCl4 CH(3,4) CH(3,4) CH(3,5) CH2 CN CHCH2 CH(2,5) CHCH2 CH(4,5) CH2 CH(3,5) CF3 CH(4) CO2 CH(3,5) CH(3,5) CH CH(2,6) C(4) 2-propanol diethyl ether allyl acetate 1,4-dioxane tetrahydrofuran diallyl carbonate 18-crown-6 diglyme tert-butyl alcohol 1,2-dimethoxyethane diglyme chloroform carbon tetrachloride pyrrole furan BHA propylene acetonitrile allyl acetate pyrrole diallyl carbonate imidazole ethylene pyridine TFE-d3 signal toluene carbon dioxide BHT toluene benzene toluene BHT 130.82 131.78 132.72 133.33 134.04 136.00 136.58 137.17 137.84 138.59 139.62 139.92 140.23 144.22 149.76 150.52 153.46 153.74 157.39 159.04 166.01 170.88 175.55 175.74 175.98 177.96 196.26 197.63 214.98 218.31 221.30 CH(3,5) CH(2,6) CHCH2 CHCH2 C CH CH(2) CH (4) C(1) C(2,6) CH(4) C(1) C(4) CH(2,5) CH(2,6) C(2,6) C(1) C(1) CO CO CH CO2 CO CO CO CO CS2 HCO CH3 CO CO benzaldehyde benzaldehyde diallyl carbonate allyl acetate hexamethylbenzene propylene imidazole benzaldehyde benzaldehyde BHT pyridine toluene BHA furan pyridine BHA BHT BHA diallyl carbonate dimethyl carbonate dimethylformamide dimethyl malonate ethyl acetate dimethylacetamide allyl acetate acetic acid carbon disulfide benzaldehyde acetone ethyl methyl ketone cyclohexanone S16 Table S23. CD3OD (1H NMR data by chemical shift in ppm) shift mult 0.07 0.10 0.20 0.85 0.86–0.91 0.86–0.93 0.90 0.90 0.91 1.01 1.05 1.15 1.18 1.19 1.24 1.29 1.29 1.29 1.29 1.34 1.40 1.40 1.41 1.45 1.70 1.72 1.74–1.76 1.85–1.87 1.87 1.99 2.01 2.03 2.05 2.07 2.12 2.15 proton s CH3 s CH3 s CH4 s CH3 m CH3 m CH3 t, 7 CH3 t, 7 CH3 t, 7.3 CH3 t, 7 CH2CH3 t, 7 CH3 d, 6 CH3 t, 7 CH3 t, 7 CH3 t, 7 CH2CH3 br s CH2 m CH2 m CH2 br s CH2 sept, 7.3 CH2 s CH3 s ArC(CH3)3 s ArC(CH3)3 s CH2 dt, 6.4, 1.5 CH3 m CH2(3,4) m CH2(4) m CH2(3,5) m CH2(3,4) s CH3 s CH3CO s CH3 s CH3 s CH3CO s CH3CO s CH3 impurity shift mult proton impurity shift mult proton impurity hexamethyldisiloxane silicone grease methane ethane pump oil H grease8 n-hexane n-pentane propane ethyl methyl ketone triethylamine 2-propanol diethyl ether ethanol ethyl acetate H grease8 n-hexane n-pentane pump oil propane tert-butyl alcohol BHT BHA cyclohexane propylene pyrrolidine cyclohexanone cyclohexanone tetrahydrofuran acetic acid ethyl acetate acetonitrile allyl acetate dimethylacetamide ethyl methyl ketone acetone 2.19 2.21 2.32 2.34 2.50 2.58 2.64 2.65 2.80 2.86 2.92 2.99 3.31 3.31 3.34 3.35 3.35 3.44 3.49 3.52 3.58 3.59 3.60 3.61 3.64 3.66 3.71 3.72 3.72 3.74 3.78 3.92 4.09 4.34 4.56 s s s t q, 7 q, 7 d, 9.5 s m s s s p s s s s s q, 7 s m s q, 7 m s s m s s s s sept, 6 q, 7 s ddd CH3 ArCH3 CH3 CH2(2,6) CH2CH3 CH2 CH3 CH3 CH2(2,5) CH3 NCH3 CH3 CD2H NCH3 CH3 OCH3 CH3 CH2 CH2 CH2 CH2 CH2 CH2 CH2 CH2 CH2 CH2(2,5) ArOCH3 CH3 CH3 CH2 CH CH2CH3 CH3 CH2 hexamethylbenzene BHT toluene cyclohexanone ethyl methyl ketone triethylamine HMPA dimethyl sulfoxide pyrrolidine dimethylformamide dimethylacetamide dimethylformamide CD3OD residual dimethylacetamide methanol diglyme 1,2-dimethoxyethane dimethyl malonate diethyl ether 1,2-dimethoxyethane diglyme ethylene glycol ethanol diglyme 18-crown-6 1,4-dioxane tetrahydrofuran BHA dimethyl malonate dimethyl carbonate 1,2-dichloroethane 2-propanol ethyl acetate nitromethane allyl acetate 4.56 4.61 4.85 4.87 4.91 5.01 5.21 5.25 5.30 5.34 5.39 5.49 5.82 5.94 5.94 6.08 6.40 6.71 6.72 6.92 7.05 7.16 7.16 7.33 7.44 7.49 7.56–7.60 7.66–7.70 7.67 7.85 7.90 7.90–7.93 7.97 8.53 10.00 s ddd s s dm, 10 dm, 17 ddt ddt ddt ddt s s m ddt ddt m dd s m s s m m s m dd m m s m s m s m s H2 CH2 OHd OH CH2(1) CH2(2) CHCH2(2) CHCH2(2) CHCH2(1) CHCH2(1) CH2 CH2 CH CHCH2 CHCH2 CH(3,4) CH(3,4) ArH CH(2,5) ArH CH(4,5) CH(2,4,6) CH(3,5) CH CH(3,5) CH(2,5) CH(3,5) CH(4) CH(2) CH(4) CH CH(2,6) CH CH(2,6) HCO hydrogen diallyl carbonate BHA water propylene propylene allyl acetate diallyl carbonate allyl acetate diallyl carbonate ethylene dichloromethane propylene allyl acetate diallyl carbonate pyrrole furan BHA pyrrole BHT imidazole toluene toluene benzene pyridine furan benzaldehyde benzaldehyde imidazole pyridine chloroform benzaldehyde dimethylformamide pyridine benzaldehyde Table S24. CD3OD (13C{1H} NMR data by chemical shift in ppm) shift carbon –4.90 0.85 1.99 2.10 6.98 8.09 11.09 14.39 14.45 14.49 15.46 16.80 16.90 17.19 18.40 19.50 20.56 20.71 20.88 21.32 21.38 21.50 23.38 23.68 25.27 25.86 26.29 26.48 27.96 28.16 29.39 30.67 CH4 CH3 CH3 CH3 CH3 CH2CH3 CH3 CH3 CH3 CH3 CH3 CH3 CH3 CH2 CH3 CH3 CH3 CH3 CH3CO CH3 CH3Ar CH3 CH2(2,4) CH2(2,5) CH3 CH2(4) CH2(3,4) CH2(3,4) CH2 CH2(3,5) CH3CO CH3 S17 impurity shift methane 30.82 acetonitrile 30.91 hexamethyldisiloxane 31.15 silicone grease 31.35 ethane 31.61 ethyl methyl ketone 32.73 triethylamine 35.30 n-pentane 35.36 n-hexane 35.50 ethyl acetate 35.83 diethyl ether 36.89 propane 37.00 (d) hexamethylbenzene 37.34 propane 38.43 ethanol 40.45 propylene 41.60 acetic acid 42.61 allyl acetate 45.11 ethyl acetate 46.96 dimethylacetamide 47.23 BHT 49.00 (sept) toluene 49.86 n-pentane 52.83 n-hexane 54.78 2-propanol 55.25 cyclohexanone 55.96 pyrrolidine 58.26 tetrahydrofuran 59.06 cyclohexane 59.06 cyclohexanone 61.50 ethyl methyl ketone 63.08 acetone 64.30 carbon impurity shift carbon impurity shift carbon impurity (CH3)3C (CH3)3C (CH3)3C CH2 CH3 CH2(3,4) CH2(3) (CH3)3C NCH3 (CH3)3C CH3 CH3 CH2CH3 NCH3 CH3 CH2 CH2(2,6) CH2 CH2 CH2(2,5) CD3 CH3 CH3 CH2 CH3 CH3O CH2 CH3 CH3 CH2 CH3 CH2 BHA tert-butyl alcohol BHT pump oil dimethylformamide n-hexane n-pentane BHT dimethylacetamide BHA dimethylformamide HMPAi ethyl methyl ketone dimethylacetamide dimethyl sulfoxide dimethyl malonate cyclohexanone 1,2-dichloroethane triethylamine pyrrolidine CD3OD signal methanol dimethyl malonate dichloromethane dimethyl carbonate BHA ethanol diglyme 1,2-dimethoxyethane ethyl acetate nitromethane ethylene glycol 64.71 66.14 66.88 68.11 68.83 69.35 69.40 71.33 71.47 72.72 72.92 79.44 97.21 108.11 110.33 111.30 116.04 118.06 118.22 118.28 118.74 122.60 123.46 125.53 126.11 126.29 126.31 129.20 129.34 129.49 129.91 CH CH2 CH2 CH2 CH2(2,5) CH2 (CH3)3C CH2 CH2 CH2 CH2 CH CCl4 CH(3,4) CH(3,4) CH(3,5) CH2 CN CHCH2 CH(2,5) CHCH2 CH(4,5) CH2 CH(3,5) CH(3,5) CH(4) CO2 CH(3,5) CH C(4) CH(2,6) 2-propanol allyl acetate diethyl ether 1,4-dioxane tetrahydrofuran diallyl carbonate tert-butyl alcohol diglyme 18-crown-6 1,2-dimethoxyethane diglyme chloroform carbon tetrachloride pyrrole furan BHA propylene acetonitrile allyl acetate pyrrole diallyl carbonate imidazole ethylene pyridine BHT toluene carbon dioxide toluene benzene BHT toluene 130.12 130.64 132.53 133.25 133.71 134.61 135.60 136.31 137.96 138.35 138.85 139.09 141.36 143.68 149.04 150.07 152.85 154.34 156.28 157.91 164.73 168.70 172.41 172.89 173.32 175.11 193.82 194.11 209.67 212.16 214.69 CH(3,5) CH(2,6) C CHCH2 CHCH2 CH CH (4) CH(2) C(1) CH(4) C(1) C(2,6) C(4) CH(2,5) C(2,6) CH(2,6) C(1) C(1) CO CO CH CO2 CO CO CO CO CS2 HCO CO CO CO benzaldehyde benzaldehyde hexamethylbenzene diallyl carbonate allyl acetate propylene benzaldehyde imidazole benzaldehyde pyridine toluene BHT BHA furan BHA pyridine BHT BHA diallyl carbonate dimethyl carbonate dimethylformamide dimethyl malonate allyl acetate ethyl acetate dimethylacetamide acetic acid carbon disulfide benzaldehyde acetone ethyl methyl ketone cyclohexanone Table S25. D2O (1H NMR data by chemical shift in ppm) shift mult proton impurity shift mult proton impurity shift mult proton impurity 0.18 0.28 0.82 0.88 0.99 1.17 1.17 1.17 1.24 1.24 1.26 1.30 1.70 1.70–1.75 1.85–1.90 1.87 1.88 2.06 2.07 2.08 2.08 2.13 2.19 2.22 2.40 2.57 2.61 s s s t, 7.3 t, 7 t, 7 t, 7 d, 6 s t, 7 t, 7 sept, 7.3 dt, 6.4, 1.5 m m m m s s s s s s s t q, 7 d, 9.5 CH4 CH3 CH3 CH3 CH3 CH3 CH3 CH3 CH3 CH2CH3 CH2CH3 CH2 CH3 CH2(4) CH2(3,5) CH2(3,4) CH2(3,4) CH3 CH3CO CH3 CH3CO CH3 CH3CO CH3 CH2(2,6) CH2 CH3 methane hexamethyldisiloxane ethane propane triethylamine diethyl ether ethanol 2-propanol tert-butyl alcohol ethyl acetate ethyl methyl ketone propane propylene cyclohexanone cyclohexanone pyrrolidine tetrahydrofuran acetonitrile ethyl acetate acetic acid dimethylacetamide allyl acetate ethyl methyl ketone acetone cyclohexanone triethylamine HMPA 2.71 2.85 2.90 3.01 3.06 3.07 3.18 3.34 3.37 3.37 3.56 3.60 3.60 3.61 3.65 3.65 3.67 3.69 3.74 3.75 3.78 3.80 4.02 4.14 4.40 4.62 s s s s s m q, 7 s s s q, 7 s s m q, 7 s m s m s s s sept, 6 q, 7 s ddd CH3 CH3 NCH3 CH3 NCH3 CH2(2,5) CH2CH3 CH3 OCH3 CH3 CH2 CH2 CH2 CH2 CH2 CH2 CH2 CH3 CH2(2,5) CH2 CH3 CH2 CH CH2CH3 CH3 CH2 dimethyl sulfoxide dimethylformamide dimethylacetamide dimethylformamide dimethylacetamide pyrrolidine ethyl methyl ketone methanol diglyme 1,2-dimethoxyethane diethyl ether 1,2-dimethoxyethane dimethyl malonate diglyme ethanol ethylene glycol diglyme dimethyl carbonate tetrahydrofuran 1,4-dioxane dimethyl malonate 18-crown-6 2-propanol ethyl acetate nitromethane allyl acetate 4.69 4.79 4.95 5.06 5.30 5.32 5.37 5.40 5.44 5.90 5.99 5.99 6.26 6.51 6.93 7.14 7.45 7.57 7.57–7.66 7.76–7.80 7.78 7.87 7.92 7.97–7.99 8.52 9.96 ddd s dm, 10 dm, 17 ddt ddt ddt ddt s m ddt ddt m dd m s m dd m m s m s m m s CH2 HOD CH2(1) CH2(2) CHCH2(2) CHCH2(2) CHCH2(1) CHCH2(1) CH2 CH CHCH2 CHCH2 CH(3,4) CH(3,4) CH(2,5) CH(4,5) CH(3,5) CH(2,5) CH(3,5) CH(4) CH(2) CH(4) CH CH(2,6) CH(2,6) HCO diallyl carbonate D2O residual propylene propylene allyl acetate diallyl carbonate allyl acetate diallyl carbonate ethylene propylene allyl acetate diallyl carbonate pyrrole furan pyrrole imidazole pyridine furan benzaldehyde benzaldehyde imidazole pyridine dimethylformamide benzaldehyde pyridine benzaldehyde Table S26. D2O (13C{1H} NMR data by chemical shift in ppm) shift carbon impurity shift carbon impurity shift carbon impurity shift carbon impurity 1.47 2.31 7.87 9.07 13.92 14.77 17.47 21.00 21.03 21.09 21.15 24.38 24.77 25.67 25.86 27.50 29.49 30.29 30.89 32.03 35.03 CH3 CH3 CH2CH3 CH3 CH3 CH3 CH3 CH3 CH3 CH3 CH3CO CH3 CH2(4) CH2(3,4) CH2(3,4) CH2(3,5) CH3CO (CH3)3C CH3 CH3 NCH3 acetonitrile hexamethyldisiloxane ethyl methyl ketone triethylamine ethyl acetate diethyl ether ethanol allyl acetate acetic acid dimethylacetamide ethyl acetate 2-propanol cyclohexanone tetrahydrofuran pyrrolidine cyclohexanone ethyl methyl ketone tert-butyl alcohol acetone dimethylformamide dimethylacetamide 36.46 (d) 37.27 37.54 38.76 39.39 42.02 42.13 46.83 47.19 49.5012 53.65 55.81 58.05 58.67 58.67 62.32 63.17 63.22 64.88 66.42 66.52 CH3 CH2CH3 CH3 NCH3 CH3 CH2(2,6) CH2 CH2(2,5) CH2 CH3 CH3 CH3 CH2 CH3 CH3 CH2 CH2 CH3 CH CH2 CH2 HMPAi ethyl methyl ketone dimethylformamide dimethylacetamide dimethyl sulfoxide cyclohexanone dimethyl malonate pyrrolidine triethylamine methanol dimethyl malonate dimethyl carbonate ethanol diglyme 1,2-dimethoxyethane ethyl acetate ethylene glycol nitromethane 2-propanol diethyl ether allyl acetate 67.19 68.68 68.81 70.05 70.14 70.36 71.49 71.63 96.73 107.83 110.23 118.75 119.03 119.06 119.68 122.43 125.12 129.48 130.09 132.48 CH2 CH2(2,5) CH2 CH2 CH2 (CH3)3C CH2 CH2 CCl4 CH(3,4) CH(3,4) CHCH2 CHCH2 CH(2,5) CN CH(4,5) CH(3,5) CH(3,5) CH(2,6) CHCH2 1,4-dioxane tetrahydrofuran diallyl carbonate diglyme 18-crown-6 tert-butyl alcohol 1,2-dimethoxyethane diglyme carbon tetrachloride pyrrole furan diallyl carbonate allyl acetate pyrrole acetonitrile imidazole pyridine benzaldehyde benzaldehyde allyl acetate 132.76 134.70 136.11 136.65 138.27 143.57 149.18 157.78 163.96 165.53 170.12 174.57 174.78 175.26 177.21 191.67 197.25 215.94 218.43 221.22 CHCH2 CH (4) C(1) CH(2) CH(4) CH(2,5) CH(2,6) CO CO CH CO2 CO CO CO CO HCO CS2 CO CO CO diallyl carbonate benzaldehyde benzaldehyde imidazole pyridine furan pyridine diallyl carbonate dimethyl carbonate dimethylformamide dimethyl malonate dimethylacetamide allyl acetate ethyl acetate acetic acid benzaldehyde carbon disulfide acetone ethyl methyl ketone cyclohexanone S18 References (1) Gottlieb, H. E.; Kotlyar, V.; Nudelman, A. J. Org. Chem. 1997, 62, 7512. (2) Except for the compounds in solutions 8–10, as well as the gas samples, hexamethylbenzene, and the corrected values (vide supra), all data for the solvents CDCl3, C6D6, (CD3)2CO, (CD3)2SO, CD3CN, CD3OD, and D2O were previously reported in ref 1. (3) A signal for HDO is also observed in (CD3)2SO (3.30 ppm) and (CD3)2CO (2.81 ppm), often seen as a 1:1:1 triplet (2JH,D = 1 Hz). (4) Splitting pattern observed as a triplet of a non-first-order ABX pattern. (5) Not all OH signals were observable. (6) In some solvents, the coupling interaction between the CH2 and the OH protons may be observed (J = 5 Hz). (7) In CD3CN, the OH proton was seen as a multiplet at 2.69 ppm, as well as extra coupling to the CH2 peak. (8) Apiezon-brand H grease. (9) In some solvents, the coupling interaction between the CH3 and the OH protons may be observed (J = 5.5 Hz). (10) Pyrrolidine was observed to react with the solvent (CD3)2CO. (11) Phosphorus coupling was observed (2JPC = 3 Hz). (12) Internal reference; see Experimental Section in text. S19