硅酸锌催化臭氧氧化水中痕量对氯硝基苯

3211Vol．32№．11201111JournalofHarbinEngineeringUniversityNov．2011doi10．3969/j．issn．1006－7043．2011．11．01412222221．4500072．150090pCNBpCNB．N2、、．mO3/mpCNBpCNB．．pCNB47%25%．pCNB6200mg·L－1/pCNB．X703．1A1006-7043201111-1474-05Zincsilicatecatalyzedozonationforremovingp-chloronitrobenzenepCNBfromdrinkingwaterLIUYue12CHENZhonglin2LIUYu2HANYing2WANGHe2SHENJimin21．SchoolofEnergyandEnvironmentEngineeringZhongyuanUniversityofTechnologyZhengzhou450007China2．SchoolofMunicipalandEnvironmentalEngineeringHarbinInstituteofTechnologyHarbin150090ChinaAbstractLaboratorysynthesizedzincsilicatewastestedforitsactivityincatalyticozonationoftracep-chloronitro-benzenepCNBinaqueoussolutions．ThephysicochemicalfeaturesincludingspecificsurfaceareatotalporevolumedistributionofporesizeandfunctionalgroupsofthecatalystswerecharacterizedbyN2adsorptionandFou-rierTransformInfraredFTIRspectrumanalysis．EffectsofthemassratioofO3andpCNBcatalystdoseandconcentrationofbicarbonateionandhumicacidonpCNBremovalwerealsoinvestigated．TheresultsshowthatthezincsilicatewasactivatedincatalyticozonationfordegradationofpCNBnotonlyindistilledwaterbutalsointapwater．ComparedwiththeozonealoneindeionizedwaterconditionscatalyzedozonationcanenhancetheremovalefficiencyofpCNBby47%intapwaterconditionscatalyzedozonationcanenhancetheremovalefficiencyofpCNBby25%．InthepresentexperimentalconditionstheoptimalmassratioofO3andpCNBalongwiththecata-lystdosagewere6and200mgL－1respectively．Theconcentrationsofbicarbonate/carbonateandhumicacidinwatercansignificantlyreducethedegradationefficiencyofpCNBinanaqueoussolution．Keywordscatalyticozonatio[e-mail][e-mail]．．pCNB、、．1．pCNBpCNB2．．3．212、．4-5．Al2O3、6-8．9-1112．．．11．1、pH、、0．1～0．5mm．XXRDXXPS．1．2CF-G-3-010g0～10g/h．、．1．2L．1LpHO3/O2pCNB0、1、3、5、1015min．0．1mol·L－1Na2S2O3．pCNB100mgpCNB1L100mgL－1pCNB．．－24h．1．313．pCNB120080∶201．0mL·min－1C18275nmpCNB．MicromeriticsASAP-2020．-Barrett-Joyner-HalendaBJH．Perkin-ElmerSpectrum2000FT-IR．Zn2+Perkin-ElmerOptima5300DV．22．1、．1aN2－1b－．387．8m2/g8．4nm2～200nm．．1c．．490cm－1Zn-O16383448cm－1H-O-HOH．1380cm－1C-O-C920cm－1Si-O-Zn．aN2·5741·11b-c1Fig．1Thespectraforthesurfaceofzincsilicate2．2pCNB2．0．6mg·L－115minpCNB52%pCNB．pCNB1minpCNB61%15minpCNB．10minpCNB99%．pCNB．pCNB15minpCNB1．5%．pCNBpCNB．pCNBpCNB、2．pCNB．TOC3．4mg·L－1TOCpCNBpCNB．pCNB1%25pCNB．pH=6．9O30=0．6mg·L－1100mg·L－1pCNB0=100g·L－1．2pCNBFig．2ZincsilicatecatalyzedozonationofpCNB2．3mO3/mpCNBpCNB3mO3/mpCNBpCNB．3pCNBmO3/mpCNB．4mO3/mpCNBmO3/mpCNB=6pCNBpCNB58%．mO3/mpCNBmO3/mpCNB=6．·6741·32pH=6．9100mg·L－1pCNB0=100g·L－115min3mO3/mpCNBpCNBFig．3EffectofmO3/mpCNBonremovaleffi-ciencyofpCNB2．4pCNB4pCNB．41min50mgpCNB54%pCNB100mgpCNB87%500mgpCNB94%·OH．15min5pCNB．200mg·L．pH=7．0O30=0．6mg·L－1pCNB0=100g·L－14pCNBFig．4EffectofcatalystdoseonremovalefficiencyofpCNB2．5CO2－3/HCO－3pCNB．．pHHCO－3HCO－37．9×107Lmol·s－1HCO－350～200mg·L－1．NaHCO3HCO－3pCNB5．HCO－3pCNBHCO－3．NaHCO350mg·L－116%．NaHCO3200mg·L－1pCNB61%．pCNB．pH=6．9O30=0．6mg·L－1100mg·L－1pCNB0=100g·L－1．5pCNBFig．5EffectofHCO－3onremovalefficiencyofpCNB2．6pCNB、14．pCNB6．61．08mg·L－13．6mg·L－115minpCNBpCNB．1．08mg·L－13．6mg·L－1．·7741·11pCNB．5．4mg·L－1pCNBpCNB．．pCNBpCNB．pH=6．9O30=0．6mg·L－1100mg·L－1pCNB0=100g·L－1．6pCNBFig．6EffectofhumicacidsonremovalefficiencyofpCNB2．7．1．0mg·L－1．pCNB．100mg·L－10．03mg·L－11000mg·L－10．4mg·L－1．3pCNB．pCNBmO3/mpCNB．/pCNB．pCNB．1．ZnOOH/O3J．200738112550．CHENZhonglinXUZhenzhenBENYueetal．Effectandmechanismofremovaloftracep-ChloronitrobenzeneinaqueoussolutionbyZnOOH/O3J．EnvironmentalSci-ence200738112550．2．La2O3CeO2J．200941477-80．YEMiaomiaoCHENZhonglinSHENJiminetal．Syn-thesisoflanthanumoxideandceriumoxideandozonationcatalyticactivitiesofp-chloronitrobenzeneJ．JournalofHarbinInstituteofTechnology200941477-80．3．J．2006222399-102．SUIMinghaoMAJunSHENGLI．Roleofadsorptioninhetero-geneouscatalyticozonationprocessfordegradationoforganicsinwaterJ．ChinaWater＆Wastewater2006222399-102．4GRACIARARAGUESJLOVELLEIROJL．MnⅡ-catalysedozonationofrawEbroriverwateranditsozonationby-productsJ．WaterResearch199832157-62．5MAJunGRAHAMNJD．Degradationofatrazinebyman-ganese-catalyzedozonationinfluenceofhumicsubstrancesJ．WaterResearch1999333785-793．6QIFeiXUBingbingCHENZhonglinetal．Influenceofaluminumoxidessurfacepropertiesoncatalyzedozonationof246-trichloroanisoleJ．SeperationPurificationMeth-ods2009662405-410．7ZHAOLeiMAJunSUNZhizhongetal．MechanismofheterogeneouscatalyticozonationofnitrobenzeneinaqueoussolutionwithmodifiedceramichoneycombJ．AppliedCa-talysisBEnvironmental2009893/4326-334．8YINCYAROUAMKASHRIWMetal．ReviewofmodificationsofactivatedcarbonforenhancingcontaminantuptakesfromaqueoussolutionsJ．SeperationPurificationMethods2007523403-415．9ZENGYBPARKJB．Characterizationandcoagulationper-formanceofanovelinorganicpolymercoagulant-poly-zinc-sili-cate-sulfateJ．ColloidsandSurfacesAPhysicochemicalandEngineeringAspects20093341/2/3147-154．10TZOUPANOSNDZOUBOULISAITSOLERIDISCA．Asystematicstudyforthecharacterizationofanovelcoag-ulantpolyaluminiumsilicatechlorideJ．ColloidsandSurfacesAPhysicochemicalandEng