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Inhibition of telomerase activity and SK-OV-3/DDP cell apoptosis by rhodium(III) and iron(III) complexes with 4′-(3-thiophenecarboxaldehyde)-2,2′:6′,2″-terpyridine

Inorganic Chemistry Communications 102 (2019) 180–184 ContentslistsavailableatScienceDirect Inorganic Chemistry Communications journal homepage: www.elsevier.com/locate/inoche Short communication Inhibition of telomerase activity and SK-OV-3/DDP cell apoptosis by T rhodium(III) and iron(III) complexes with 4′-(3-thiophenecarboxaldehyde)- 2,2′:6′,2″-terpyridine Qing-Min Weia,1, Zhen-Feng Wanga,1, Qi-Pin Qina,⁎ , Shu-Long Wanga, Ming-Xiong Tana,⁎ , Bi-Qun Zoub,d,⁎⁎ , Peng-Fei Yaoc,⁎ , Hong Liangd aGuangxiKeyLaboratoryofAgriculturalResources,ChemistryandBiotechnology,CollegeofChemistryandFoodScience,YulinNormalUniversity,1303Jiaoyudong Road,Yulin537000,China bDepartmentofChemistry,GuilinNormalCollege,9FeihuRoad,Gulin541001,China cGuangxiCollegesandUniversitiesKeyLaboratoryofRegionalEcologicalEnvironmentAnalysisandPollutionControlofWestGuangxi,CollegeofChemistryand EnvironmentalEngineering,BaiseUniversity,Baise,Guangxi533000,China dStateKeyLaboratoryfortheChemistryandMolecularEngineeringofMedicinalResources,SchoolofChemistryandPharmacy,GuangxiNormalUniversity,15Yucai Road,Guilin541004,China GRAPHICAL ABSTRACT tpatpy-Rhinhibitedtelomerasebydown-regulationofc-mycandhTERT,aswellasinducedSK-OV-3/DDPcellarrestintheSphase. ARTICLE INFO ABSTRACT Keywords: Tworhodium(III)andiron(III)complexesof4′-(3-thiophenecarboxaldehyde)-2,2′:6′,2″-terpyridine(tpatpy):[Rh 4′-(3-Thiophenecarboxaldehyde)-2,2′:6′,2″- (tpatpy)Cl3]·CH3OH (tpatpy-Rh) and [Fe(tpatpy)Cl3] (tpatpy-Fe) have been prepared and characterized. terpyridine Tpatpy-Rh(5.03±1.15μM)andtpatpy-Fe(18.02±0.45μM)exhibitedgreatercytotoxicitythanthetpatpy Rhodium(III)complex ligand(70.11±0.28μM)andcisplatin(61.21±1.39μM)againstSK-OV-3/DDPcells.Inaddition,tpatpy-Rh Cellapoptosis inhibitedtelomerasebydown-regulationofc-mycandhTERT,aswellasinducedSK-OV-3/DDPcellarrestinthe Telomeraseactivity Sphase. In1978cisplatin(cis-[PtCl2(NH3)2])wasthefirstapprovedbythe applicabilitywaslimitedatsometimes[1–4].Therefore,thenon‑pla- FDAasananti-tumormetaldrugforclinicaltreatment[1–3].However, tinum(II/IV)transitionmetalcomplexeshavereceivedrecentinterestat cisplatinanditsderivativeshavealsoshownsideeffects/drawbacksin presentduetotheirhavehighspecificitytobindtoproteinmolecules, the clinical treatment, including nephrotoxicity, ototoxicity, and ac- telomeraseandDNA,etc.[5–14]AlthoughlesswidelystudiedthanPt quired resistance or cisplatin-resistant tumor cells, etc., thus their (II/IV) compounds, complexes based on Fe(III) and Rh(III) have ⁎Correspondingauthors. ⁎⁎Correspondenceto:B.-Q.Zou,DepartmentofChemistry,GuilinNormalCollege,9FeihuRoad,Gulin541001,China. E-mailaddresses:qpqin2018@126.com(Q.-P.Qin),mxtan2018@126.com(M.-X.Tan),zoubiqun@163.com(B.-Q.Zou),yaopengfei1986@163.com(P.-F.Yao). 1Theseauthorscontributedequallytothiswork. https://doi.org/10.1016/j.inoche.2019.02.030 Received9January2019;Receivedinrevisedform18February2019;Accepted18February2019 Available online 20 February 2019 1387-7003/ © 2019 Elsevier B.V. All rights reserved. Q.-M.Wei,etal. Inorganic Chemistry Communications 102 (2019) 180–184 Scheme1.Syntheticrouteoftpatpyligandanditstpatpy-Rhandtpatpy-Fecompexes.Reagentsandsolventsareasfollows:(a)ethanol,25%NH3·H2O(aq),KOH; (b)RhCl3·3H2OorFeCl3·6H2O(1.0mmol),3.5mLCH3OHand0.5mLCH2Cl2,85°C,2days. attractedrecentinterestfortheir interestinganti-tumoractivityprop- CH3OH/CH2Cl2 (2.5mL: 0.1mL) generated [Rh(tpatpy)Cl3]·CH3OH erties [11,15,16], such as phenanthroline Rh(III) complex [Rh (tpatpy-Rh, Yield: 85.12%) and [Fe(tpatpy)Cl3] (tpatpy-Fe, Yield: (phq)2(MOPIP)]+ (phq=2-phenylquinoline and MOPIP=2-(4-meth- 77.03%),respectively.Thestructuresoftpatpy-Rhandtpatpy-Fewere oxyphenyl)-1H-imidazo[4,5-f][1, 10]phenanthroline) [11], octahedral determined by elemental analysis and X-ray crystallography (Table Rh(III) complexes [16], the antibiotic platensimycin Fe(III) complex S1–S6,Figs.1and2).AsshownintheFigs.1and2,theRh(III)andFe [15,17], 4-chloro-2-phenylquinoline rhodium(III) complexes [18], (III)centerintpatpy-Rhandtpatpy-Feadoptedasix-coordinatedoc- piano-stool dipyrrinato Rh(III) complex [19], 2-phenylbenzimidazole tahedralgeometry.Inaddition,theRheNandNeFebondlengthswere rhodium(III)complex[20],andmore. intherangeof1.935(3)–2.045(3)Åand2.108(7)–2.151(7)Å,respec- Ontheotherhand,alargenumberoftribipyridinederivativesand tively.Inaddition,thehighestpeakswith2.38eÅ−3oftpatpy-Feinthe theirmetalcomplexes,suchasPdII,ZnII,IrIII,FeII,PtII,CuII,RuII,AuIII, residualelectrondensityarelocated0.02ÅfromatomCl(1).Thedee- VIIIandOsIIIcomplexes[21–51],havebeenreportedtostudyfortheir pestholewith−2.59eÅ−3oftpatpy-Feintheresidualelectronden- DNAbindingability[21–40],inhibittelomerasebydown-regulationof sityarelocated0.04ÅfromatomS(1). c-mycandhTERT[41–51],inducetumorcellcyclearrestandstabilize To gain information about the anti-tumor activity of the tpatpy thetelomere(HTG21)andproto-oncogene(c-Myc)G-quadruplexDNA ligand,tpatpy-Rh,tpatpy-Fe,cisplatin,RhCl3·3H2OandFeCl3·6H2O, [21–51].However,therhodium(III)andiron(III)complexeswith4′-(3- MTTassaywasperformedandtheIC50valuesweredeterminedforSK- thiophenecarboxaldehyde)-2,2′:6′,2″-terpyridine (tpatpy) have not OV-3, SK-OV-3/DDP, T-24, HeLa cancer cells and HL-7702 normal been reported in the literature [50,51], and the detailed anti-tumor cellsexposedtoeachofcompound(Table1).Theresultsshowedthat activitymechanismsofitsRh(III)andFe(III)complexesstillneedtobe tpatpy-Rh was the most active complex against SK-OV-3/DDP cells, explored. with the lowest IC50 value was 5.03 ± 1.15μM, which it was Herein,wereportedtworhodium(III)andiron(III)complexesof4′- 3.6–14.0foldsmoreactivethanthetpatpyligand(70.11 ± 0.28μM), (3-thiophenecarboxaldehyde)-2,2′:6′,2″-terpyridine (tpatpy): [Rh tpatpy-Fe (18.02 ± 0.45μM), and cisplatin (61.21 ± 1.39μM), re- (tpatpy)Cl3]·CH3OH (tpatpy-Rh) and [Fe(tpatpy)Cl3] (tpatpy-Fe). In spectively. Compared with the selected four tumor cells, tpatpy-Rh addition, we explored tpatpy-Rh in vitro anti-tumor activity and in- andtpatpy-FedisplayedlowinhibitoryratesagainstHL-7702normal vestigateditsactionmechanisms. cells,indicatingtheselectivityoftpatpy-Rhandtpatpy-FeonSK-OV- The 4′-(3-thiophenecarboxaldehyde)-2,2′:6′,2″-terpyridine (tpatpy) 3/DDPcells.Becauseoftheweakantitumoractivityoftpatpy-Fein was synthesized via the synthetic routes shown in Scheme 1, starting MTT assay, thus, only tpatpy-Rh (5.03μM) was selected for further from 2-acetylpyridine and 2-thenaldehyde, which was synthesized by assays. using modified method reported procedures [48,50,51]. In addition, Telomerase is transcriptionally repressed in most human normal the reactions of RhCl3·3H2O and FeCl3·6H2O with 4′-(3-thiophene- cellswhilebeingover-expressedinabout85%oftumorcells[56,57]. carboxaldehyde)-2,2′:6′,2″-terpyridine (tpatpy) in the presence of This activity by chemical complexes or compounds leads to the Fig.1.Molecularstructureoftpatpy-Rh(A)andtpatpy-Fe(B),respectively. 181 Q.-M.Wei,etal. Inorganic Chemistry Communications 102 (2019) 180–184 Fig.2.Modulationoftelomeraseactivitybytpatpy-Rh(5.03μM)inSK-OV-3/DDPcellsfor24h.(A)Analysisofthetelomeraseactivity.(BandC)c-mycandhTRET proteinsintpatpy-Rh(5.03μM)treatedcellsweredetectedbywesternblot. Table1 IC50values(μM±SD)forthetpatpyligand,tpatpy-Rh,tpatpy-Fe,cisplatin,RhCl3·3H2OandFeCl3·6H2OagainstSK-OV-3,SK-OV-3/DDP,T-24,HeLacancercells andHL-7702normalcellsfor48hat37°C. Compounds SK-OV-3 SK-OV-3/DDP T-24 HeLa HL-7702 tpatpy 35.96±0.15 70.11±0.28 18.23±1.59 25.06±1.78 35.02±1.85 tpatpy-Rh 29.62±1.14 5.03±1.15 15.31±0.22 >100 40.11±1.91 tpatpy-Fe 32.06±0.72 18.02±0.45 27.03±1.09 >100 38.15±0.22 RhCl3·3H2O >150 >150 >150 >150 >100 FeCl3·6H2O >150 >150 >150 >150 >100 Cisplatina 15.02±1.43 61.21±1.39 12.36±1.11 16.25±0.31 15.58±1.56 a Cisplatin(1.0mM)wasdissolvedinNaClsolution(0.154M)[52–55]. decrease in the level of hTERT and c-myc proteins [58–66], conse- (Fig. 3B and C). Thus, those prompt us to study the percentages of quently inducing tumor cell cycle arrest and down-regulating the re- apoptosis cells (Q2+Q4), as shown in Fig. 4, SK-OV-3/DDP cells lated-proteins [58–66]. Remarkably, Western blot assay testified that treated with tpatpy-Rh (5.03μM), the populations of apoptosis cells tpatpy-Rh(5.03μM)inhibitedthetwoproteinslevelsofthehTERTand (Q2+Q4) was 54.40%, which suggested that tpatpy-Rh (5.03μM) c-mycexpressionsinSK-OV-3/DDPcells(Fig.2BandC).Becauseofthe couldcauseapoptosis. weak anti-tumor activity of tpatpy-Fe in MTT assay, only tpatpy-Rh In conclusion, we synthesized two Rh(III) and Fe(III) complexes, (5.03μM) was selected for TRAP‑silver staining assay. Consequently, [Rh(tpatpy)Cl3]·CH3OH (tpatpy-Rh) and [Fe(tpatpy)Cl3] (tpatpy-Fe), the inhibitory ratio (IR) forthe telomerase activity in cancercells in- with 4′-(3-thiophenecarboxaldehyde)-2,2′:6′,2″-terpyridine (tpatpy), duced by tpatpy-Rh (5.03μM) reached 47.71% (Fig. 2A), comparing respectively. By MTT assay, it was confirmed that tpatpy-Rh withthecontrol(5%DMSO),whichwasagreedwellwiththeresultsof (5.03 ± 1.15μM)andtpatpy-Fe(18.02 ± 0.45μM)exhibitedgreater Westernblotanalysis(Fig.2).AsshowninFig.3,treatedwithtpatpy- cytotoxicity than the tpatpy ligand (70.11 ± 0.28μM) and cisplatin Rh (5.03μM) for 24h, the populations of S-phase was approximately (61.21 ± 1.39μM)againstSK-OV-3/DDPcells.Inaddition,thesewere 35.89%,compared withthecontrol(21.74%), thesecan bedescribed thefirststudiestodemonstratethattpatpy-Rhinhibitedtelomeraseby thattpatpy-Rh(5.03μM)causedSphasearrest(Fig.3A),andledtothe down-regulationofc-mycandhTERT,aswellasinducedSK-OV-3/DDP decrease on the level of CDK2 and cyclin A by Western blot assay cellarrestintheSphase. 182 Q.-M.Wei,etal. Inorganic Chemistry Communications 102 (2019) 180–184 Fig.3.Thechangeofcellcycleandrelated- proteinsinSK-OV-3/DDPcellsaftertreated withtpatpy-Rh(5.03μM)for24h.(A)The cell cycle in SK-OV-3/DDP cells after treated with tpatpy-Rh (5.03μM) was analyzedbyflowcytometry.(BandC)The cell cycle related-proteins in tpatpy-Rh (5.03μM) treated cells were detected by westernblot. Fig.4.ApoptosisofSK-OV-3/DDPcellsaftertreatedwithtpatpy-Rh(5.03μM)for24h. Acknowledgements AppendixA. Supplementarymaterial This work was supported by the National Natural Science Inaddition,supplementarycrystallographicdatafortpatpy-Rhand Foundation of China (Nos. 21867017 and 21761033), the Natural tpatpy-Fe collected in this study can be found under CCDC Nos. Science Foundation of Guangxi (No. 2018GXNSFBA138021), the Key 1889618 and 1889619. These data include synthesis, materials and Foundation Project of Colleges and Universities in Guangxi (No. methods of the most important compounds described in this article. 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