全 文 ：生态科学2()03年05月第22卷第2期 坠旦!竺望!!兰!!翌!!竺!!!!!!!i：!!、!’!!!!二!旦
汽油添加剂甲基叔丁基醚(MTBE)污染的植物修复
于晓章，TRAPPStefan(丹麦技术大学环境与资源研究中心DK．2800gs．Lyngh弘丹麦
【摘要】 甲基叔丁基醚(MTBE)是北美燃料市场最常用的汽油添加剂。由于其在土壤中的不吸附肚和极高的水溶
性，MTBE已成为一种蔓延性的地下水污染物。本实验用一自行设计的植物反应器来观察和测定在不同温度条件卜概】
树‘妇，打日￡妇)对MTBE污染水溶液的修复潜力．长出新根须和嫩叶的柳树枝条在一容积500mL的锥型瓶中生长12d(其
中M113E溶液450rIlL)来观察舢E对柳树生长的影响，同时测定柳树对MTBE的吸收和降解。MTBE及其丰要降斛
产物叔J基醇(11；A)用气相色谱来检测。本实验结果表明在为期12d的时间内．水溶液中24．84～5327％MTBEHJ
以通过柳树的蒸腾作用去除。同时在15℃、一25℃的温度范围内．MrBE的去除率(％)和柳树的蒸腾量‘g)之间存扣
着明显的线性关系。由于没有发现TBA和其它可能的降解产物，植物挥发是MTBE植物修复技术中主要的作用机理
尽管植物在MTBE污染的修复过程中只是起着中间传输媒介的作用，大量的MTBE通过植物的燕腾作用以气态的形式
释放到天气中，但由于MTBE在气态下的光氧化非常．快，MTBE不会造成空气污染。我们认为植物修复技术对MTBE—i
染的土壤和地F水仍不失为一个有效的修复手段．
关键词：甲基叔了_基醚(MTBE)；植物修复；叔丁醇(11jA)；温度；柳树
中图分类号：x173 文献标识码：A 文章编号：1008罐873【2003)P2一109一I】5
Thepotent蹦forphytonIⅡemaⅡonofmethyl枷-butyIether(MTBE)，Yuxiao—zh如g卸dTRAPPstef抽(En“ronment
＆Resollrces，1hhnicalUnivefsityofDenmark．DK·2800Kgs．L和窖bHDenmark)
AbslractMe山yl把n岫utyle h口(MTBB)诂t11cmos【commonlyusedgasolineoxygenateintheNonhAme^call’sfucJ
indusⅡyDuetoitshighsolubilityinwat盯柚dlowsorpdonte d肋cy洫soils，MTBEhasbecomeoneofthemostcommon
con协11inantsinurban窟roundwa魄．T11ispaperxa血ncdⅡlc口otendalforphytoremedia60nofMTBEwithinacarefullv
des垃nedbioreac【。fPre．rootedwdIowtrees∞血d佑d)wer℃k印tinanErIenmeyernaskof500n儿wi恤450InLs讲ked
aqueoussolu石onfor12dMTBE如dtIlem越nmetabolite1BAw remeasuredbyG(珊．W11low骶euptaket stsiⅡdicaL酣
thattheremoval0fMTBEmassinaqu。0uss01嘶0nthroughwillow订ceac廿videswafoundirItherangeof248 一，5327％at
15—25·overa12一dav口嘶odofexposure．The行acdonofMTBE(％)re【noved厅Dmtlleaqueoussolu石onbywⅢowⅡ℃es
wasposinvelycorrelatcdtoⅡ∞缸锄spira石on(rng)．Nei出erTBA，noranyotherpossiblemetaboUtefmBEwas口ackedm
thistest．indica缸ngphvtovoladhzadonis山edorflin如tⅡ佗chanismforph邶remedi8donofMTBE．Resultsof山ebench*sc甜e
studjesndicatcdⅡ1ata1arge仔acdonofMTBEwasrele船edi工Itothea打州【hout粕yconv盯酊onthmughwillow玳霉sovera
s咖p嘶odofdme，h0、ⅣevcrMTBE耐Ilbesuscep曲letopho∞oxid撕onaIldoesnotbecomeanairqualityconcer【!
Tbereforc，“istoconclude廿1atphyt饥emediationisa11effecdvememodto eall七hesoilandgmundwatercon【aITljnatedw；th
MTBE．
Kevwords：MTBE；PhytOremediadon：TBA：Tempera呲re：Willow虹_ces
Methylf已盯_butylether(MTBE)，witllits
introductionin }leIate1970s，isthemostf}equemJy
usedgas01ineoxygenateto reduceatIrlosphere
emissiOnsofcarbonmOnOxide．柚dtOincreasefuel
0ctanelevels．AnnualDfoductionofMTBEincreased
fmm1．38billionlbi 1984to24．1billjon1bi 1993，
thesecoJldon t}Ie血st ofor芎anicche埘cals
manufacturedinthUS⋯．ThecauseofMTBE
leakingt0the nvirOnmentis ainly砒埘butedtO
gasOlinespiUsandleaksf}ompipelines，under鲜Ound
andabo。导，．呼0undstoragetanks，andtransport
accidemsH．ThereisevidencethatMTBEhas
becomeone0ftl】emostcOmmonc tarninantsof
“ballgmundwaterin吐leUS⋯1．InEU，sinmar
Droblemsmi曲toccurinnearfuture．Duetoitslli曲
solubiUtynwaterandlowsorptionte dencyinsoils，
MTBEfacilelymovesiⅡto目oundwaterwithoutre ard
ontheaquiferma廿ixwhenspiUed，anditspersistence
ingmundwateris ofsigII讯cantconcem，which
providesamajorstimuIusfortheinVesIigationand
researchOntheremediationOfenvironInenlalsites
contaminatedwi山M盯BE．Itiswimthisinrnindthat
differentanemDtshavebeenmadetotreatthismobile
andpersistentcomp咖nd．NaturalttenuanOn．
en乐neeringtechnjquesandbioreme1jationarethree
altemativesforcleallin空M丌BE≮ontaITlinatedsites
FieldstIldieshaver Dortedthattllenaturalatten¨aⅡon
ofMTBEinaqllif打sis lowandinsomecases
undetectable，wi山halflivesofatleasttwoyears”1
Engine鲥ngr ethodsal ohaveindicatedlow
e佑ciencyandlli曲cost，andpotentialadversee仟 cts
基金项目：勘fap啊lc(_m面s啪n，田’gmm。fQud竹。F恤
f。U8Cr2000舶164】
作者简介：于晓章(1966一)．男，副教授研究^向为☆母污瓷物的植
物修复Bm缸l：yu^iaozh柚g@h咖血1．㈣
2003．O禾09收藕。2003．05．2l接受
万方数据
生态科学
oncc(’logicalsvstemsH1． Despiteevidencetbat
biode船丑dation”⋯
Phvtorellledia石onhasbe fM1BEinpure
cultures．enIic|lIIlent．andbatchrnjcrocosmsis
Dossible”)。⋯．theseresultsdonotshowt量latMTBE
biodeglada“onis si911ificantprocessinthefield
comearec(19nizedmcansofreclaimingenVirOnmental
sitesc()nlat面natedwi山varioushazardouschemicals
”“．Alar￡enumberOfstudieshavedemonstratedth
plaIltscanplavaroleinthedegradationofpersistent
organicconta蛐nants8ucha 砸chlomethyle玎e(TCE)，
tetrachloroet|lyiene(PCE)．arIdpolynucleararOmatic
hvdrocarbonsfI)AH)“1． HoweveLt|lereahtvof
phytoremediaⅡ0nasanin—situec心queforcleaning
MTBE。contaminateds“esis 矾ckysub{ecttoP丁asp．
Severalstudieshavebeendonetoinvesn髓tethe
feasibiIltvof口hvtoremediationofMTBE【2，12，13，14， ”．
Itisknownthata rangeofenvironmentalfac ors
af：fbctoralterthemechanismsofphytoremedianon．
Curremlv．thereisn(儿dataavailableontheresearchin
mepotentialforphytoremediationofM：TBEatvarious
temperatures．Tbmperaturecanaf!f色ctthemt sat
whjch￡hevariousmechaflismsofphvtorcmedianon
take口lace．T11ispaperxarIlinesMTBEupt{ll(eby
willowtreeswithinacarefu“vdesi娜edbiOreactorat
15一～25·andDrOvidesthewealthOfinformationto
developen砸neeredphytoremediationofMTBE．
1 MaterjalsandMetllods
1．1 Treesandexposllrere百lnes
WjldwjJ】ow姐eesf黝Z缸d舾d)weresampledhom
alakeinH—rshhOlm，Dlenmark．40c lOngwillOw
cut石ngswereutilized．andtIlenculturedinbuckets
withtapwaterat25℃，Anef曲正ee—week舀_owtll，
pre—rootedtreesweretransferredintoanErlenmeyer
naskOf500mL．a11dthen450mLofspikedaqueOus
soIutionwereadded．Theflaskswereallsealedwith
tefloncOatedcorkstoppers．Thesenaskwrapped
withalurninumfoilwereincubated￡hreedi抒erent
temDeratures(15℃，20℃and25℃)undefarti矗ciaI
li出lIModifiedISOnu埘entsolunonwasusedt0
supponwillowtreeg耳owtll⋯1．
FOurreplicates、verecOnducteda eachrangeOf
temDerature．oneconIrolwaswithMTBE，butwitllout
trees．andO ewithⅡees，butwithOutMTBE，to
quannfythe骶cIofvolamization，aIldtocheckthe
genemlgrowmofwillowtrces．Thewe谵htof
bioreacIOrwithwillowtreesandaqueoussOlutiOnwas
r℃cordedlomeasureth incl℃aseinwillow圩ee
bjomassndthechangein仃anspimnOnoVerthemire
pe^od(1ftests．
WillowtreeswerexposedtoMTBEaqueous
solutionwitht econcenⅡationsof4．8卜一7．97mg·Ll
ThepresenceofMTBEintlleaqueOussOludOnwas
measurcdDriorto thetests．afterwmcjllhe
concenIratiOnofMTBE，andtheoccurrenceofth
intemlediatef已疗-butvla cohol(TBA)andother
possibIeinte姗ediates(methan01．formaldehvdeaIld
othercompundstllatcanbedetecI∞bythcnlethod)
wastrackedineach3．dayperiod．Ansamplesw re
an vzedwithamaximumholdtimeofl davThe
duratjonofthetestswas12davs．
1．2 ChenⅡcalanalvsis
AnalvsisofMTBEandTBAintheaaueous
solutiOnwasdonebvaS“madzuGC．14Bwil}1FD，
combinedwithapurgeandtrapunit(Tekma卜LSC
2(100)．1()(HLwatersamplesw redirectIvinlected，
andthesamplewaspurgedfor4．5 minu据saI30‘C
(approxjmately)，fo儿owedbya drypurge^)r0．5
删nuteCompoundswerecollectedonthesorbent”ap
andthenpre—k俎tedto 150℃．Thedesorption
temDera“盯ewas160。Cforl minute．fbllowedbva
bakecvcleat200℃for3 n虹nutesThe1nitial
temDeratureofGCwas37℃for1 minute．increased
tothefinaltemDemtureof120℃at20C．仃Ⅱn。and
washeldat120℃for3111inutes．Standardsolutions
containjngchcmicals(MTBEandTBA)were
preparedintherangeof0．74一14．8mg·j。1for
MTBEandO．78～15．6m只·L1forTBAandusedfor
caⅡbration．MTBEandTBAwereidentified11vt11e
(jCfetentiontime门．3minforMTBEand26n讧nfor
TBA)．7nledet ctionl mitsforthetwocompounds
weredetefITlinedtobe0．2lg·LoandJlig·i．“for
MTBEandTBA，resDectivelv，
2 ResultsandDiscussion
2．1VolatilizatiOn0fMTBE
T11econ扭olwaswitllMTBE．butwithoutwillow
treestotestheD0tentialforvOlatilization0fMTBE
fromthedesignedbioreactoLEverythinges【’aping
fromthebioreactormustgothrou窖hthecorkstopperS
Atl5·，thepresenceofMTBEinaqueoussoIution
wasattenuatedfrOnl4．32mg·L
1
leveIsjnitialIylo
2．26m2·L1overa12_dayperiod．correspOndingt0a
47．69％reductionra eofMTBE．Thereductionrates
ofMTBEals0weredete衄inedtobe46．18％at20‘C
and44．99％at25 ，respectivelv．LittleornOjossof
waterwasfoundinalltestsduringa12一dayexposure
period．Resultsindicatedthatsignificantdi盯hence
(>lO％)inthev01atiliza廿on0fMTBEf如Inthe
aoueoussOlutionwasotobserved砒15～25【：overa
12埘ayperiodofnme．Also，nophot lvsis，hydn’lysis，
and／Orde窖radationbyr icr00rganismswereound．
、blatiliz撕OnwastheonlVlossprocessforMTBE
mass行Omthecontrols．
2．2RemovalofMTBE丘omtheaqueousmediaby
willow扛eesThepoteInialofwiJdwillowu℃es￡of(move
万方数据
十晓章．等：汽油添加剂甲基叔丁基醚(MTBE)污染的植物修复
ThblcMeasu坤哇parameters垫垫!塑’11里垦竺旦塑堑塑!塑塑!!!!!!!竺!竺一，——
Parametcr Testl(15℃) Tesl2(20℃) Test3(2511)
Control1leatme力tControlTreatm曲tControl 1YeamlenI
2．21 2．03(O．65) 2．51 ：．10(0．41) 347 26S(O．5m
1 282I 152．49f4859) 20453 20726(8879) 29483 40929(466)
TTeebiomass(g)
TfanspiraIion(g)
MTBEreduction(％)0 7253(1252) O 7886(66()) 0 9R26(1{)6)
里艘堡l且!!鲎(丝! ! 堡幽!翌 ! 翌竺堕竺 ! 翌型。‘!生～
+Valueswi【hlnp{lrcnthesesrepresentthesLandardeViatiOn0fn)urmeasurements
MTBEfbTnLheaque()usmediaw stested砒15—25℃
overa J2一出ype一0d叫’exposu衅．CleEaijedr。s¨swer
sunlrn撕zedjnthetollo诵ngtable．
ThetotalreductionofMTBEmassinaqueous
sol嘶onwasdeteIminedtob 72．53～98．26％|dt15～
25℃．Ifa constantvola61izationr eofMTBEis
sub廿acted，theremovalofMTBEbvwillow扛佻scan
beestimatedtobe24_84～53．27％overa 12一dav
De『jodrexposI肿．Thjsjndicatedthata】argefractjon
ofMTBEmasscanbe removedfrOmthe
contaminatedrrlediat}Ⅱou时1wi儿owtreeactivities
withoutanvobservedanmeasuredimDactonwiUow
trees，in panicularunderanoptimal伊Owtll
tem口eratureof25℃．Thus．wiUowtreescanactas
or鼬nicpumpsforMTBE舡ansferfromcoman吐nated
mediato aIrMTBEintheatmosDherewillb
susceptibIeIophOto—oxidationbyvaporphaser action
w“hph(Ho—chemicallVproducedhy roxVlradicals
wichanesIimatedhalf．1ifeo 4davs”“．
2-3AccumulationofMTBEinwillowtreebiomass
AccumulatiOnOf c tarnjnantswitllin柚。e
biomassis oneof thekeymechanismsfor
Dhvtoremediation．Severalstudi8s11ustraIedthattrees
takeupMTBEffomthecomaIIlinatedmediathmugh
theirrOOtsaJldaccumulate山emtOasmallde嚣eein
theirbiomass．NewmaIl
“。1
re口0nedmat月∞r耐
p鲫肠坩wereabletOincorporateO．37％ofthedosed
MTBEintotheirbiomasswhile咖nspiring5．1％．
￡“cn劬∽incorporated0．4％oftheosedMTBEand
transpiredl6．52％．Hong”“foundthat2．2l％ofthe
radiOlabeledMTBEwasrecoveredwit|Iinpoplar仃ees
(pop“f“sdP打。耐即xn堙mDN一34，ImperialCa olina)．
Theseudiesindicatedthatonlva saTllIl锄ountof
MTBErnasswasrocOveredasinsolublefesiduewithjn
treebiomassn i IocOncludethataccumulatiOnof
contafIliantsintreebiomassisnotakevmechanims
forDhvtoremediationofMTBE．Therefore，int11istest
thereisnointentiOnlO仃ackCheaccumula“OnOf
MTBEwlthinwillowtreebiomass．
2．4MetaboIismofMTBEbvwillow仃ees
Enzvmesof 山e cvtocllrorr伦P_450
monooxvgenase(CYP450s)werefoundtobeableto
workonthede譬radationofMTBEinmicroorganisms，
humanlivers．andrniceUvers¨“’．Enzvmesofth
CYP450safemetvpicalenzvmeofvascularpallltsto
p】avac一“calro】ei力thep】ametabo“smlI⋯N—lher
TBA，nor0therpossibleintermediatcs(methanol’
fomlaldehyde)wastrackedduringthentireperIL)dof
tests．Asilimarresultalsowasfoundint11es“Hlvof
H0n2””NOtetIlatsOmewhatsurprisingresullwas
reponedbyTrapp”“，inthetestusjngplantrootsand
leavestocbaraclerizcMTBEde盯adation，morethan
24Dlanls丘om15farmliesinDenmarkwerefoundto
beunabletode盯adeMTBE．Theseresultsindicated
thatMTBEis recalcitrantothcattackofDlanl
enzyrrles．
2．4Heallhofwillow七rees
Withincer七ainconcentmtionranges，trcescan
loleratehazardouschernicals，thuslayingthe
fundationfortbephytoremedialionofconlammnted
siles．fhytoremediationmaybe nef!fectjVe，howeVeL
ifconcentr诅“onsofthecontan证nan“areei{hertoo
h蟾h(causingt9婪city)0rtoolow(resultinginpoor
bioavallabilitv)”⋯．A1aboratorvstu—indicatedIjttle
OrnOtOxjcitytOhybirdpOplarI eesalMTBE
cOncen伽Onslesst11anl OOOm卫·L¨。’“．Inthjslest，
willowtreeswerexDosedtOMTBEsolutionwith
c0Bcentradonsof4．8l～一7．97mg·L‘。．I】1deed，no
observedeff色cts“：仇on)j血ofleaves)wasfoundboth
incontrolsand廿eatedplantsOvermeenIireperi‘dOf
tests．Aslightdi圩色renceintreebiomassbetween
con“Olledantreatedplantswasdetected，prObably
resultingfromthefactmatit isvervha坩toselect
hOmo留eneouswmowcutlin窟s．Theseobserv¨【ions
indicatcdthatwillOwtreescankeepuptheirnormal
phVsi0109icalfunctloningw thinthedesigned
bioreactoL
2．5 Con-t；ladonoftherenlovalofMTBEl|lrnu曲
winowt『eestote坷【perature
1mef0110wingf 即reglvesas ani1Ius【衄tive
examDleth cOrrelation0ftheremovalofMTBE
”oughwi】】owtreesto Va—oustemperatures，
Temperatl玎eis oneof themostimportant
environmentalfac ors山at aHbctsheratesof
phytOrenlediatiOnbecausetemperatureandtrce
transDiration，andalsotheremovalofMTBEand
transDirationarecl setoeachotheLInchistesthe
fracⅡonfMTBEr％)removedfromtheaqueous
solutionbvw．1lowtreeswaspos{石velycorrelatedto
万方数据
生态科学
treetranspjra“onf譬)。asde行nedbythexpressjonfv=
()．108她+9．16l2 ¨thacorrelationcoef!ficientOf
()．9956．Notemathebiologicallegi廿macyoft11is
estimatewasmctlyconnnedtotheteJTIperaturenge
of】5、25。C．Theseresultsindicatedthat山ehimler
thetemDeraturethefastertheremovalofMTBE舶m
aqueoussolutjonbyw订10wtrees．
Resultsofthebench—scalestudiesndicated山ata
Iar空e疔acmnofM113Ecallberemoved仔omaqueous
1 00 200 300 400
Transpirationlg
med|aInrou助wljJOw∽es， lnpa巾cuJarm列eraI】
opnmalplant}=fow山temper¨tureof 25·．
Phvtovola【“izationis thedominantmechanjsmfor
phytoremediationofMTBE．Duetoamn足eofPxtemal
andintemalv撕ablesinv01vedinmeneldaDD】ica“on．
anactivemanagements廿ategyWithplanning．site
inVesdgationandassessment，dataaIlalysisa11d
monitoringisneededtoremediatethegroundwater
DIumecontanlinatedwithⅣ盯BE．
群
刻
Fig1 Plolof廿ee仃anspira60n(g)vs．refnov“ofMTBE(％)bywillow”ees
Acknowledgements
Thankst0Professor“aoBoH Ilforthepreview
andAndersTGundersenforhisengagedhelp．
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f81 SalanitmJRDiazLA，wiIliamsMPeta1．1994．】蛐lauon
ofabacL酣alculturethatde盯adesMcth“tcn_buIvlether
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汽油添加剂甲基叔丁基醚(MTBE)污染的植物修复
作者： 于晓章， Trapp Stefan
作者单位： 丹麦技术大学,环境与资源研究中心,DK-2800,Kgs.Lyngby,丹麦
刊名： 生态科学
英文刊名： ECOLOGIC SCIENCE
年，卷(期)： 2003,22(2)
被引用次数： 10次

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