单级自养脱氮污泥的厌氧氨氧化代谢特征郭劲松

第32卷第6期重庆大学学报Vol.32No.62009年6月JournalofChongqingUniversityJun.2009　　:1000-582X(2009)06-721-06郭劲松,杨国红,方　芳,秦　宇(重庆大学三峡库区生态环境教育部重点实验室,重庆400030):2009-02-17:(50608071);(308020);(200801A1A0180277):(1963-),,,,,(Tel)023-65120768;(E-mail)[e-mail]。　:以单级自养脱氮污泥为研究对象,采用批式试验的方式,分析在不同进水水质条件下系统内生成的中间产物的种类及其含量,研究了单级自养脱氮污泥的厌氧氨氧化反应的代谢特征。实验结果表明,单级自养脱氮污泥具有厌氧氨氧化反应功能。部分NH+4和NO-2是按照Graaf提出的厌氧氨氧化代谢途径去除的:NO-2首先被还原为NH2OH,生成的NH2OH则与系统内的NH+4反应生成N2H4,N2H4继续被转化为N2实现氮的去除。还有部分NH+4和NO-2是按照另外一条厌氧氨氧化反应代谢途径去除的:NH2OH与NO-2在缺氧条件下被转化为N2O,N2O则进一步被转化为N2而实现氮的去除,同时NH+4被氧化为NH2OH。该途径中NH+4转化为NH2OH的反应和N2O转化为N2的反应可能是相互耦合的过程,但关于这点还需进一步证实。:单级自养脱氮;厌氧氨氧化;中间产物;代谢途径　　:X703.1:AAnaerobicammoniumoxidationinaone-step,completelyautotrophicnitrogenremovalsystemGUOJin-song,YANGGuo-hong,FANGFang,QINYu(KeyLaboratoryoftheThreeGorgesReservoirRegion'sEco-environment,MinistryofEducation,ChongqingUniversity,Chongqing400030,P.R.China)Abstract:Weexplorethecharacteristicsofanaerobicammoniumoxidation(ANAMMOX)usingsludgedrawnfromaone-step,completelyautotrophicnitrogenremovalsystem.Batchexperimentsareadopted.Thequalityandquantityoftheintermediatesformedinthesystemareanalyzed.TheresultsshowthatthesludgepossessestheANAMMOXfunction.SomeoftheNH+4andNO-2areremovedintheANAMMOXmetabolicpathway.Thatistosay,NO-2firstisreducedtoNH2OH,andthenNH2OHreactswithNH+4toformN2H4,whichsubsequentlyisconvertedtoN2.OtherportionsoftheNH+4andNO-2areremovedinadifferentANAMMOXmetabolicpathwayinwhichtheNH2OHandNO-2areconvertedtoN2O,thentheN2OisconvertedtoN2,andNH+4isconvertedtoNH2OH.ThecouplingbetweentheNH+4toNH2OHconversionprocessandtheprocessofN2ObeingconvertedtoN2needsfurtherresearch.Keywords:one-stepcompletelyautotrophicnitrogenremoval;anaerobicammoniumoxidation(ANAMMOX);intermediates;metabolicpathway　　、N2,10[1-3],、、C/N[4-5]。,,[6-7]。,[8-10]。Graff[11]15N,NO-2。,Graff[12],1,NH2OHN2H4。Wood[13]Thauer[14],NH3NO-2N2ΔG0′=-358kJ·mol-1,NH3NH2OHΔG0′=-87kJ·mol-1,NH2OHNO-2N2OΔG0′=-270kJ·mol-1,N2ON2ΔG0′=-341.4kJ·mol-1。,,:NH3NH2OH,NH2OHNO-2N2O,N2ON2。1,NH2OHN2O,NH2OHNH3,NO-2NH2OHN2ON2。。1　Graaf,,,,,,,2。1　1.1　,500mL,300mL。,30℃130r/min,30℃,。,(,4L)NO、NO2、N2ON2。,30℃,Ar30min,N2O2,DOLDOTMHQ10(0.01mg/L)。Ar30min,,。Ar,4～6mL/min。12h,3,(,)。,NH+4、NO-2、NO-3、NH2OH、N2H4TN,。,,2h1,1。1.2　,(1),NaHCO3pH8.0(±0.2),(EDTA5.0g/L,CoCl2·6H2O1.6g/L,ZnSO4·7H2O2.2g/L,MnCl2·4H2O5.1g/L,CuSO4·5H2O1.6g/L,(NH4)6Mo7O24·4H2O1.1g/L,CaCl2·2H2O5.5g/L,FeSO4·7H2O5.0g/L)。722重庆大学学报　　　　　　　　　　　　　　　　　　　　第32卷1　/(mg·L-1)ⅠNH4HCO3(N,)NaNO23030NH3+NO-2※N2ⅡNaNO230NO-2※NH2OHGraafⅢNH4HCO3NH2OHCl3030NH3+NH2OH※N2H4GraafⅣN2H4·H2O30N2H4※N2GraafⅤNH4HCO330NH3※NH2OHⅥNH2OHClNaNO23030NH2OH+NO-2※N2O※N21.3　2SBBR[15-16],873.6mgMLSS/L。1.4　NH+4:;NO-2:N-1--;NO-3TN:-;MLSS:[17]。NH2OHNH2NH2Frear[18]Yatslmlrsky[19]。NONO242CNO-NO-2-NOxAnalyzer(ThermoScientific,)。N2OECD5890(,)。N2TCDSC-6000(,)。pH:Sension2pH/ISE(Hach,);:LDOTMHQ10(Hach,)。2　2.1　1,Ar,,。,2。2　mgNH+4NO-2NO-3NH2OHN2H4NONO2N2ON2NH4HCO3/NaNO25.935.560.970.0770.0520.00150.000310.000565.06NaNO25.570.051.68NH4HCO3/NH2OHCl6.260.027—5.182.01N2H4·H2O2.24———5.58NH4HCO38.65—0.06———0.00076—NH2OHCl/NaNO22.990.090.910.0130.00281.235.93　　:,“—”,N2.2　NH+4NO-2Ⅰ,Ar。NH2OH、N2H4NO-3,5.06mgN2(2),,,NH+4NO-2N2。NO、NO2N2O。Wyffels[20]Graaf[21],。NO-2NO、NO2N2O,,。,,NO-2NO、NO2N2O。723第6期　　　　　　　　　　　　　郭劲松,等:单级自养脱氮污泥的厌氧氨氧化代谢特征2。NH+4NO-2,1∶1.12,Strous[22]NH+4NO-2,。2　Ⅰ2.3　2.3.1　Graaf等报道的厌氧氨氧化代谢途径Ⅱ、ⅢⅣ,Ar,Graaf[12]。1)NO-2※NH2OH,NO-2Ⅱ,12h1.68mgNH2OH。1NO-2、NO-3NH2OH3(a),NO-20.97mg/L·h,N,NH2OH(0.45mg/(L·h)2.16,NO-3,0.15mg/L。,NO-2NH2OH。NO-2(3.43mg)NH2OH(1.68mg),NH2OHNO-2N2ON2。2)NH3+NH2OH※N2H4NH+4NH2OHⅢ,N2H4,13.34mg/L。NH+4、NH2OH、N2H4NO-213(b),NH+4NH2OH,N2H4,NH+4NH2OHN2H4。NO-2,NH+4NH2OH(6.56mg)3　Ⅱ、ⅢⅤN2H4NO-2(4.02mg),。3)N2H4※N2N2H4Ⅳ,724重庆大学学报　　　　　　　　　　　　　　　　　　　　第32卷N2H4-N7.47mg/L。1N2H43(c),N2H4,1.99mg/(L·h),5.58mgN2,NO、NO2N2O,N2H4N2,NH+4NH2OH,N2。,Graaf[12],NH+4NO-2。2.3.2　厌氧氨氧化代谢途径研究ⅤⅥ,Ar,,Ⅰ,。1)NH3※NH2OHNH+4Ⅴ,Ar,DO(0.01mg/L),28.83mg/L,,NH2OHN2H4,0.35mgAr。,,。2)NH2OH+NO-2※N2O※N2NH2OHNO-2Ⅵ,Ar。2h1(4)。NH2OHNO-2,NH2OHNO-2,1∶1.27,NO-3,0.15mg/L。,NO、NO2、N2ON2,N2ON2,17.14%82.64%。NH2OHNaNO2,N2ON2。,,NH+4NO-21∶1.12,NH2OHN2O,NH2OHNO-21∶1.27,N2ON217.14%82.64%,。,NH+4NH2OHN2ON2,4　Ⅵ,,NH2OH,,N2ON2,。Zart[23],,NONO2NH3。,NH+4,NH+4。,NH+4NH2OHN2ON2,N2ON2NH+4NH2OH,2,5,NH+4NH2OHN2ON2。3　　,,,,,,:1)NH+4NO-2,Ar,(12h),NH+4NO-21∶1.12,5.06mgN2,。2)NH+4NO-2Graaf:NO-2NH2OH,NH2OHNH+4N2H4,N2H4N2。3)NH+4NO-2725第6期　　　　　　　　　　　　　郭劲松,等:单级自养脱氮污泥的厌氧氨氧化代谢特征:NH2OHNO-2N2O,N2ON2,NH+4NH2OH。NH+4NH2OHN2ON2,。:[1]SUNGZ,AUSTIND.Completelyautotrophicnitrogen-removalovernitriteinlab-scaleconstructedwetlands:Evidencefromamassbalancestudy[J].Chemosphere,2007,68(6):1120-1128.[2]SLIEKERSAO,DDEWORTHN,GOMEZJLC,etal.Completelyautotrophicnitrogenremovalovernitriteinonesinglereactor[J].WaterResearch,2002,36(10):2475-2482.[3]GONGZ,YANGFL,LIUST,etal.Feasibilityofamembrane-aeratedbiofilmreactortoachievesingle-stageautotrophicnitrogenremovalbasedonAnammox[J].Chemosphere,2007,69(5):776-784.[4]AHNYH,CHOIHC.Autotrophicnitrogenremovalfromsludgeliquidsinupflowsludgebedreactorwithexternalaeration[J].ProcessBiochemistry,2006,41(9):1945-1950.[5]DONGX,TOLLN