废弃物水稻秸秆制备催化剂强化臭氧深度处理造纸废水的效能

20171CIESCJournal313January2017681Vol.68No.1DOI10.11949/j.issn.0438-1157.201609191,222231(131002323242003150090)FeFe3O414.25%1175.1m2g1Langmuir(R20.99)0.3gh11gL1pHCODBOD546175mgL118GB3544200820ESRX703.1A04381157201701031307Advancedtreatmentofpaper-makingwastewaterusingcatalyticozonationwithwastericestrawascatalystZHUANGHaifeng1,2,HUANGHaili2,XUKelong2,ZHANGYunjin2,HANHongjun3,SHANShengdao1(1KeyLaboratoryofRecyclingandEco-treatmentofWasteBiomassofZhejiangProvince,ZhejiangUniversityofScienceandTechnology,Hangzhou310023,Zhejiang,China;2ChangshanCountyRuralEnergyOffice,Quzhou324200,Zhejiang,China;3StateKeyLaboratoryofUrbanWaterResourceandEnvironment,HarbinInstituteofTechnology,Harbin150090,Heilongjiang,China)Abstract:Wastericestrawswereconvertedintoricestrawderivedactivatedcarbon(RSAC),whichsupportedferricoxides(Fe3O4,loadeddosageof14.25%)asozonecatalystwith1175.1m2g1ofspecificsurfacearea,andefficiencyofheterogeneouscatalyticozonationofbiologicallypretreatedpaper-makingwastewaterwereinvestigated.TheresultsindicatedthatRSACandcatalystallhadthegoodadsorptioncapacityofbiologicallypretreatedpaper-makingwastewater,andtheadsorptionisothermsfittedwellwiththeLangmuirmodel(R20.99).Theadditionofthepreparedcatalystsignificantlyenhancedthepollutantsremovalperformanceofozonationofrawwastewater,andtheCOD,BOD5,NH+4-Nandchromaticityinthetreatedeffluentwere46,17,5mgL1and18degreewhichallmetdischargestandardpaper-makingwastewater(GB35442008)withtheoptimal2016-07-042016-10-0619842016C33108LQ17E0800082015C02037Receiveddate:2016-07-04.Correspondingauthor:Dr.ZHUANGHaifeng,[e-mail]:supportedbythePublicWelfareTechnologyApplicationResearchProjectofZhejiangProvince,China(2016C33108),theZhejiangProvincialNaturalScienceFoundationofChina(LQ17E080008)andtheMajorProjectsforScienceandTechnologyDevelopmentofZhejiangProvince,China(2015C02037).68314operatingparameters(0.3gh1ofozonedosageand1gL1ofcatalystdosageandrawwastewaterpH).Moreover,thecatalysthadsuperiorstabilityandleachingofmetalironswereveryfewat20cycle’sutilization.ItwasdeducedthattheenhancementofcatalyticactivitywasresponsibleforgeneratingmoreradicalsbyradicalscavengerandESRdetection.Thus,thepreparedcatalystwithefficient,stableandeconomicaladvantageswassuitableforcatalyticozonationofbiologicallypretreatedpaper-makingwastewater.Keywords:adsorption;catalyticozonation;catalyst;radical;wastetreatment[1]GB35442008[2][3-4]•OH[4-6][7-8][9]FeSEMBETXRDXPSXRF11.113cm1006hCODBOD5210153551531108mgL1355pH7.00.51.2ZnCl23molL1Fe:ZnCl2:Fe=1:2:112h50rmin110012h200mlmin115s15003hHClpH12h1mmFeOx/FeOx/ricestrawderivedactivatedcarbon,FeOx/RSAC1.31.2L1m5%KI1315100μlNa2S2O30.45μmBOD5Na2S2O360min1.4CODBOD5Brunauer-Emmet-Teller(BET)ASAP-2020HELIOSNanoLab600iXXRFAXIOS-PW4400,HollandXXRDRigakuD/max-2000XXPSPHI-5700ICP-AES(Optima5300DU,PerkinElmerInc)N-(DMPO)(ESRBrukermodelESP300E)1.0L500ml3096h10e()ccVqm.(1)qmgg1c0cemgL1VLmgLangmuirFreundlichLangmuirFreundlich23Langmuir0ee1xQbCqmbC(2)Freundlich1/fenxqKCm(3)xmgQ0mgg1CemgL1bLangmuirLmg1KfnFreundlich22.11ZnCl212261Fig.1SEMimagesofpreparedcatalystandRSAC68316m2g10.335,0.232cm3g13.411nmFeFe0.74%14.25%XRF1CHN2aXRD2θ=23.5°30.5°35.8°43.5°57.5°63.3°JCPDSNo.19-0629220311400511440FeFe3O4XPSFe2+/Fe3+1:2Fe3O4[2b][10]1Table1PhysicochemicalpropertiesofpreparedcatalystParametersRSACFeOx/RSACSBET/m2g11226.61175.1Vmeso(macro)/cm3g10.3320.311Vmicro/cm3g10.2350.212poresize/nm4.4113.845Fe/%(mass)0.7414.25C/%(mass)55.2464.79H/%(mass)4.764.55N/%(mass)1.511.852.2RSACFeOx/RSAC3109.6102.1mgg1LangmuirFreundlich2RSACFeOx/RSACCODLangmuirR20.99Langmuir[11][12]2XRDaXPSbFig.2XRD(a)andXPS(b)spectrumofpreparedcatalyst3Fig.3Adsorptionisothermsofpreparedcatalyst2Table2IsothermparametersCatalystLangmuirFreundlichQ0/mgg1b/Lmg1R2Kf1/nR2RSAC109.60.060.9981523.944980.300190.94188FeOx/RSAC102.10.050.9942621.433860.304120.952012.32.3.113171gL1pH(7)4aCOD0.3gh1FeOx/RSACCOD0.15gh123%0.6gh1COD7%4Fig.4EffectsofprocessparametersontreatmentperformanceCOD[13]0.3gh14bCOD1gL1COD39%4gL16.7%•OH1gL1•OH[14]4cpHpH49FeOx/RSACCOD33%•OH[15]pHpH79COD7.8%pHpH70.3gh11gL1pH2.3.23CODBOD578.1%51.4%66.7%83.6%46517251mgL1183GB35442008He[16]Fe10COD56%683183Table3PollutantsevolutioninrawandtreatedwastewaterbycatalyticozonationParametersInfluentEffluentO3O3+RSACO3+FeOx/RSACCOD/mgL1210±15130±1079±846±5BOD5/mgL135±525±322±317±2NH+4-N/mgL115±314±311±25±1chromaticity/degree110±859±553±518±30.170.37[17]2.452060minCOD6.5%GB35442008Fe11.22mgL1200.85mgL1Fe[18]5Fig.5Stabilityofcatalystinsuccessivecatalyticozonationruns2.5•OH(80mgL1)[6a]COD28.6%40.6%RSAC+O349.2%(FeOx/RSAC+O3)FeOx/RSACCOD•OH6b1:2:2:14DMPO/•OHESRDMPO-•OOH/O2–••OH[19]FeOx/RSAC•OHESR[20]6Fig.6Mechanismdetection31Fe1319Fe3O414.25%1175.1m2g1Langmuir(R20.99)20.3gh11gL1pHCODBOD5203ESR4References[1]KAMALIM,KHODAPARASTZ.Reviewonrecentdevelopmentsonpulpandpapermillwastewatertreatment[J].EcotoxicologyandEnvironmentalSafety,2015,114:326-342.[2],,,.[J].,2010,23(4):504-509.YANGF,SHIHX,WANXK,etal.Screeningforpartic