Theoretical studies on metal thioarsenites and thioantimonides synergistic interactions between transition metals and heavy metalloids 英文参考文献.docVIP

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Theoretical studies on metal thioarsenites and thioantimonides synergistic interactions between transition metals and heavy metalloids 英文参考文献.doc

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Theoretical studies on metal thioarsenites and thioantimonides synergistic interactions between transition metals and heavy metalloids 英文参考文献

Theoreticalstudiesonmetalthioarsenitesandthioantimonides: synergisticinteractionsbetweentransitionmetalsandheavy metalloids J.A.Tossell Article DepartmentofChemistryandBiochemistry,UniversityofMaryland,CollegeParkMD 20742,USA Received15thApril2000,Accepted5thMay2000 PublishedontheWeb15thMay2000 Recentlyweestablishedthattheternarycomplex,CuAsS(SH)(OH)hasanunusuallyhighstabilityandmakesa largecontributiontothetotalconcentrationsofbothCuandAsinsul?dicsolutionsequilibratedwithCuand Assul?deminerals.Thisternarycomplexhasanunusualstructure,containingabondwhichisformallyCu()± I As( III ),alongwithabrokenAs±Sbond.Wehavenowfoundthatcomplexeswithsimilarstructuresexistfor Au+andTl+coordinatedtoAsS(SH)(OH)2.However,suchadirectmetal±metalloidbondisnotarequirement forstability.Infact,TlAsS(SH)(OH)isunstablewhileAuAsS(SH)(OH)ishighlystable(comparedtotheaquo ion).Zn2+,Cd2+,Hg2+ andPb2+ alsoformbondstotheAsofAsS(SH)(OH),butwithoutbreakinganyAs±S bonds,andHgAsS(SH)(OH)+andPbAsS(SH)(OH)+areparticularlystablecomplexes.Calculatedstructures areshownforthesecomplexes,gas-phaseenergiesarecalculated,andformationconstantsinaqueoussolution areestimated.TheSbS(SH)(OH)2ionformsanalogouscomplexes,withsimilarstabilities.However,theAu+ complexofSbS(SH)(OH)2isslightlylessstablethantheCu+complex,oppositetotheorderfoundforthe AsS(SH)(OH)2ligand.TheAu+andAuSHcomplexesofAsSSHOH2orAsS(SH)22maybeimplicatedin invisiblegoldinarsenianpyrites.VibrationalfrequenciesaregivenfortheAuAsS(SH)32complexandthe XANESenergiesofthiscomplexandAu(SH)22arecompared.Theexistenceofsuchstrongcomplexesmay explainthemanycorrelationsobservedbetweentheconcentrationsofcoinagemetalsandmetalloids. beofgreateststabilityinaqueoussolutionandsuggeststargets formoreaccuratecomputationalstudiesandforexperimental studies. Introduction In determining the solubilities of minerals in solution one generally examines the mineral by itself in contact with a solutionwhichcontainsonlynoncoordinatingions.1However, in nature minerals do not occur