腐殖质电子传递机制及其环境效应研究进展李丽

35220162ENVIＲONMENTALCHEMISTＲYVol．35No．2February20162015710ＲeceivedJuly102015．*51325804．SupportedbytheChinaNationalFundsforDistinguishedYoungScientists51325804．＊＊[e-mail][e-mail]10．7524/j．issn．0254-6108．2016．02．2015071002．J．2016352254-266LILiTANWenbingWANGGuoanetal．ElectrontransfermechanismsofhumicsubstancesandtheirenvironmentalimplicationsAreviewJ．EnvironmentalChemistry2016352254-266*1231＊＊23231．1001932．1000123．100012．、．．、．、．．．ElectrontransfermechanismsofhumicsubstancesandtheirenvironmentalimplicationsAreviewLILi1TANWenbing23WANGGuoan1＊＊HEXiaosong23XIBeidou231．DepartmentofEnvironmentalSciencesandEngineeringCollegeofＲesourcesandEnvironmentalSciencesChinaAgriculturalUniversityBeijing100193China2．StateKeyLaboratoryofEnvironmentalCriteriaandＲiskAssessmentChineseＲesearchAcademyofEnvironmentalSciencesBeijing100012China3．StateEnvironmentalProtectionKeyLaboratoryofSimulationandControlofGroundwaterPollutionChineseＲesearchAcademyofEnvironmentalSciencesBeijing100012ChinaAbstractHumicsubstancesHScanserveaselectronshuttlesthatpromotetheelectrontransferfrommicroorganismstoextracellularelectronacceptors．TheelectrontransfercapacityofHScouldbeinfluencedbymanyfactorsincludingmolecularstructuresourceandenvironmentalconditions．HScannotonlyacceleratetheprocessofelectrontransferbutalsohavestablestructureandchemicalpropertiesandthisiswhyHScanbeusedasanidealelectronshuttleinthenaturalenvironments．ComparedwithdissolvedHSwhichareextractedandpurifiedbychemicalreagentsthesolidphaseHScouldbetterreflecttheelectrontransferprocessesintherealenvironment．InthisreviewarticlewehighlightrecentadvancesintheunderstandingoftheapplicationsofHSontheremediationofsoilpollutionthemitigationofgreenhouseeffectandthetreatmentofwaterpollution．AlthoughmanyresearcheshavebeenconductedonelectrontransferviaHSsomeissueswithrespecttotheelectrontransfermechanismofHSanditsenvironmentimplicationsshouldbeaddressedfurther．2255Keywordshumicsubstanceselectronshuttleselectrontransfermechanismenvironmentalimplications．、、、．、31．2-3、、4．、5-6．7849、、、．FeⅢ．1FeⅢ．10-11．12-13、1415．FeⅢ2．4FeⅢ、249．．1．11a1bFeⅢ．16．116Fig．1Humicsubstancesactingasredoxmediatorsduringanaerobicbiotransformationofelectron-acceptingcontaminants16．2517-19．6182563520-22．．———23．Aeschbacher24H+．．FeⅢ25-27c2．c25c．AQDS29-30．AQDS．AQDS25-272ac31．Voordeckers27G．sulfurreducensAQDS．26-27FeⅢ32-33．2FeⅢ28OMIMNADH1/NADHMQcytFig．2SchematicillustrationofthepathwayofelectronflowtopoorlysolubleFeⅢoxidesanddissolvedelectronshuttlesinFeⅢ-reducingbacteria28OMoutermembraneIMinnermembraneNADH1/NADHdehydrogenaseMQmenaquinonepoolcytcytochromeoftheelectrontransfersystem1b2b．FeⅢFeⅢ．．2434-352257．．．1．2、、202436．．37-38．．39．S．oneidensis40．AQDSS．oneidensisAQDS40．41．42．Aeschbacher24C/HＲatasukNanny34．．Hernández-Montoya42H2/PdpH=81360cm－1H2/PdpH=6．5．H2/PdpH=6．5pKa=9．9．ＲatasukNanny34pH=6．5H2/Pd．44%—58%3442．pH=6．5H2/PdG．sulfurreducens42．、3--、n-、1--25-43．44．．50—1000μeq·g－1HS618203544-452434243439．46．25835．Eh．pH=7．0Eh－0．3—+0．4VvsSHE1947-48．EhEh．Eh－225—－137mV45．FeⅢ．FeⅢ、21FeⅢEh．BauerKappler35Eh=－287mVEh=－274mVEh=+372mVEh=0mV．Liu49FeⅡAQDS．FeⅢ．．pH50-52．Gamage51AQSH2AQSH－AQSH－AQS2pKas．pH＜pKa1H+pKa1＜pH＜pKa2H+pH＞pKa2pH52．pH＜pKa2．GuChen53．、、MnⅣ、FeⅢ．Cervantes54、．2434-35．5522239．．22．1FeⅢ2nm2c56．AQDS．G．metallireducensS．alga2．20、、、57FeⅢ．JiangKappler62a2c272b2c7．．58-59．22592．2AQDS、JQ、NQ、AQCAQDS．60．Eh61ADQSEh45．AQDS．Wolf45AQDS28、．、344244AQDS．AQDS5AQDS．．———．．、H2、H2S、、、4062-652845．2．366-676869-70．68．．Kappler71＜1g·L－1．、、3．2nmAQDS．3、71Fig．3ElectronhoppingamongmicroorganismbiocharandFeⅢminerals713、．260351727374-7521．763、、．Ｒoden7G．sulfurreducenS．oneidensis．．281cm4．Nielsen77O2．．428Fig．4ElectrontransferfrommicrobiallyproducedreducedmetabolitesFeⅡS2－etc．toelectronacceptorswithamorepositiveredoxpotentiale．g．O2overmm-orevencm-longdistancesviaaconductivenetworkincludingredox-activedissolvedandsolid-phasehumicsubstancesinsedimentsorsoils28．、．ZhangKatayama8．8．、pH．226149．4．．4．178-83．FeⅢFeⅢFeⅢFeⅡ2．AgⅠCdⅥ84、HgⅡ8285、CrⅥ86．Wang87AQDSE．coliSeⅣ、TeⅣ．．Bradley88、．HAAQDS89-90．91、92．．1．14Table1Priorityorganicpollutantsbiodegradedwithhumicsubstancesorhumicsubstancesanaloguesservingasterminalelectronacceptor4PollutantsTerminalelectronacceptorInoculaＲeferences-AQDS88AQDSHA88AQDSHA89-90AQDSPseudomonasaeruginosa92AQDS93AQDS93AQDS94AQDSHA95AQDSGeobactersp．914．2CO2、N2OCH4CH4CO2．Bradley88CH4CO2CH4．5796．N2O97．．4．39．26235、、98-100、101-102．Ye1032000μmol·L－1AQDSC．beijerinckii1．94．104-105C．beijerinckii．．106107-108．．SeⅣ、TeⅣ、PbⅡSe0、Te0、Pb0109-110．520．．、．．．Ｒeferences1STEVENSONFJ．HumuschemistrygenesiscompositionreactionsM．2ndEdition．NewYorkWiley199417．2LOVLEYDＲCOATESJDBLUNT-HAＲＲISELetal．HumicsubstancesaselectronacceptorsformicrobialrespirationJ．Nature19963826590445-448．3PIEPENBＲOCKASCHＲDEＲCKAPPLEＲA．ElectrontransferfromhumicsubstancestobiogenicandabiogenicFeⅢoxyhydroxidemineralsJ．EnvironmentalScience＆Technology20144831656-1664．4MAＲTINEZCMALVAＲEZLHCELISLBetal．Humus-reducingmicroorganismsandtheirvaluablecontributioninenvironment