Quantitative determination of elemental sulfur at the arsenopyrite surface after oxidation by ferric iron mechanistic implications 英文参考文献.docVIP

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Quantitative determination of elemental sulfur at the arsenopyrite surface after oxidation by ferric iron mechanistic implications 英文参考文献.doc

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Quantitative determination of elemental sulfur at the arsenopyrite surface after oxidation by ferric iron mechanistic implications 英文参考文献

Quantitativedeterminationofelementalsulfuratthearsenopyrite surfaceafteroxidationbyferriciron:mechanisticimplications MollyM.McGuire,aJillianF.Ban?eldbandRobertJ.Hamers*a aDepartmentofChemistry,1101UniversityAve,UniversityofWisconsin—Madison, Madison,WI53706,USA.E-mail:rjhamers@facstaff.wisc.edu;Tel:(608)262-6371; Fax:(608)262-0453 bDepartmentofGeologyandGeophysics,1215W.DaytonSt,UniversityofWisconsin— Madison,Madison,WI53706,USA Article Received10thMay2001,Accepted13thJuly2001 PublishedontheWeb24thJuly2001Firstpublishedas anAdvancedArticleontheweb25thAugust2000 Theelementalsulfurformedatthearsenopyritesurfaceafteroxidationbyferricironwasquantitatively measuredbyextractioninperchloroethyleneandsubsequentquantitativeanalysisbyHPLC.Reactionswith ferricironinperchloricacidsolutionsorinsulfuricacidsolutions(bothatpH~1and42uC,which approximateextremeacidminedrainageconditions)producedelementalsulfurinquantitiesgreaterthan50% ofthetotalreactedsulfur.Thecontroversysurroundingthemechanismoftheoxidativedissolutionof arsenopyriteisdiscussedinlightofthesemeasurements.Basedontheobservationofgreaterthan50% productionofelementalsulfur,amechanismbywhichallthesulfurfromthemineralproceedsthrough thiosulfatecanbeeliminatedasapossibledescriptionofthedissolutionofarsenopyrite.Instead,itislikelythe otherconstituentsoftheminerallattice,FeandAs,areleachedout,leavingbehindaS0lattice.Nucleation reactionswillthenresultintheformationofstableS8rings. Introduction Incontrast,Ramanspectroscopicandchromatographicinves- tigations of arsenopyrite samples oxidized in ferric iron Arsenopyrite,FeAsS(aderivativeofthemarcasitestructure), isthemostcommonarsenic-bearingmineral.Underoxidizing conditions,eitheroccurringnaturallyorasaresultofmining processes, the mineral produces arsenite (AsO332), arsenate (AsO432), and sulfate (SO422),1–3 thus contributing to the acidi?cation of water as well as the release of soluble arsenic species. Despite the potential environmental and health hazards posed by the