电絮凝法同步去除氨氮和磷的模拟试验

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26220132ResearchofEnvironmentalSciencesVol.26No.2Feb.2013.J.2013262181-187.LANGLinZHANGLiuZHUYanetal.SimultaneousremovalofnitrogenandphosphorusbyelectrocoagulationprocessJ.ResearchofEnvironmentalSciences2013262181-187.2012-09-302012-12-082011ZX07303-001PCRRF100162011HGQC10291988-langlin0829@163.com.*1981-jingweifeng@hfut.edu.cn12311111*1.2300092.2300013.200092.Redlich-PetersonGibbs-20~0kJmolR20.98pH.0.15~0.500.02~0.04kW·hg.X788A1001-6929201302-0181-07SimultaneousRemovalofNitrogenandPhosphorusbyElectrocoagulationProcessLANGLin1ZHANGLiu23ZHUYan1CHENPei1ZHUDan1SHIChao1FENGJing-wei11.SchoolofCivilEngineeringHefeiUniversityofTechnologyHefei230009China2.AnhuiInstituteofEnvironmentScienceHefei230001China3.KeyLaboratoryofYangtzeAquaticEnvironmentMinistryofEducationCollegeofEnvironmentalScienceandEngineeringTongjiUniversityShanghai200092ChinaAbstractElectrocoagulationwithstainlesssteelelectrodesandaluminumelectrodeswereadoptedforremovalofammonianitrogenandphosphorus.Thethermodynamicskineticsandtheeffectofdifferentparametersonammonianitrogenandphosphorusremovalwerestudied.Theresultsshowedthatstainlesssteelelectrodeweremoresuitableforremovalofammonianitrogenandphosphorusfromaqueoussolutionscomparedwithaluminumelectrodes.ThephosphorusadsorptionprocesscouldbedepictedprimarilybyRedlich-Petersonfunctionandthehighertemperaturewashelpfulforitsadsorptionwhichwasaspontaneousandendothermalprocess.ThechangesofGibbsfreeenergyrangesfrom-20kJmolto0kJmol.ThecorrelationcoefficientR2wasgreaterthan0.98andthisindicatedthatthekineticdataofphosphorusadsorptionwerebetterfittedwiththepseudo-second-orderkineticmodel.Theremovalefficiencyofammonianitrogenandphosphorusincreasedwithincreasingelectriccurrentdensity.AlowerammonianitrogenremovalrateunderstrongalkalineconditionswasalsoobservedandtheremovalefficiencyofphosphoruswasthebestunderacidconditionswhileitdecreasedwiththeincreasingpH.Thepowervalueswere0.15-0.50and0.02-0.04kW·hgrespectivelywhichwererequiredforammonianitrogenandphosphorusremovalduringelectrochemicalprocesses.Keywordselectrocoagulationnitrogenremovalphosphorusremoval1.DOI10.13198/j.res.2013.02.70.langl.01226、、2-5.pH、6-7.2.8Al→Al3++3e-.3H2O+3e-→32H2+3OH-.Al3+OH-AlOH3.9Fe→Fe2++2e-2Fe2++5H2O+12O2→2FeOH3+4H+Fe2++2OH-→FeOH2.2H2O+2e-→2OH-+H2..10..Ikematsu11PtIrFePtIr.FENG12TiRuO2、、CODCr90%..11.1..ρρρ-13.0.45μm.pH.1.210cm×10cm×17cm1L.66500cm25mmρ100mgLρ50mgL.ρ253.4mgL..3.0A1.15minρ.15minρρ.HHρ286、293、303K15min15min0.45μmρ.ρ50mgL0.45μmρ.13.0AFig.1Voltagechangesatconstantcurrent3.0A22.12.2ρ100mgL60min.14.0.8A2812.815..pHpH.1—2—.2Fig.2Effectofelectrodematerialontheremovalrateofammonianitrogen3.310min295%.1—2—.3Fig.3Effectofelectrodematerialontheremovalrateofphosphorus、、16-17.、.2.2286、293、303K4.4qe.Langmuir、FreundlichRedlich-Peterson1.K1—2862—2933—303.4Fig.4Effectoftemperatureontheadsorptionofphosphorus1Redlich-PetersonLangmuirFreundlich.Langmuir18.Freundlich19.Redlich-Peterson20.2.3GibbsΔG0、ΔS0ΔH021ΔG0=ΔH0-TΔS0lnCe=lnqe-ΔS0R'+ΔH0R'TqemgCemgLR'8.314JK·molTK.381261Table1ParametersofisothermadsorptionequationsatdifferenttemperaturesKLangmuirFreundlichRedlich-Petersonq0mgbR2KFnR2KRαβR2286228.940.0640.948540.462.950.978637.560.550.760.9866293235.370.0850.944448.013.110.990667.140.960.750.9974303240.740.1190.925657.833.350.9935138.461.870.750.9989q0LangmuirmgbLangmuirR2KF、nFreundlichKR、αRedlich-PetersonβRedlich-Peterson.qeRedlich-PetersonCe1T、lnCe.ΔH0R'lnqe-ΔS0R'ΔH0、ΔS0ΔG02.2ΔG0-20~0kJmol|G|ΔH0.2、Table2ThermodynamicparametersevaluatedatdifferentequilibriumadsorptionamountsandtemperaturesqemgΔH0kJmolΔS0〔JK·mol〕ΔG0kJmol286K293K303K10033.8122135.3284-4.8917-5.8390-7.192315027.5676107.2667-3.1107-3.8616-4.934220024.680191.4525-1.4753-2.1155-3.03002.4.22lnqe-qt=lnqe-K1t22tqt=1K2qe2+tqeqttmgK1、K2.3.3R20.98qeqeqeqeR20.97.3Table3ParametersofkineticmodelsforadsorptionofphosphorusρmgLqemgK1R2qemgK2R212.57.80.26740.893614.50.03870.99442521.60.28850.969626.10.01680.99565058.40.37130.939763.30.00500.98372.5.5、60.5A3.0A.5.2.1.6..23-24..4minρ4812.、.Am21—0.772—1.543—4.62.5Fig.5EffectofcurrentdensityonammonianitrogenremovalrateAm21—0.772—1.543—3.084—4.62.6Fig.6Effectofcurrentdensityontheremovalrateofphosphorus2.6pHpH.7pH.40min.7pHFig.7EffectofinitialpHontheremovalrateofammonianitrogen7pH.25pH5~9.pH5pH26.HClOClO-27.ClO3-HClOClO-ClO3-28.8pH.8pH.pHFeOH30、FeOH4-、Fe2OH24+FeOH+、29.pH12FeOH4-30-32.pH.pH1—3.02—5.03—7.04—9.05—11.0.8pHFig.8EffectofinitialpHontheremovalrateofphosphoruspH9.9pHpHpH.2.7ρ10ρ.2.1ρρρ.10ρ.ρρρ58126pH1—3.02—5.03—7.04—9.05—11.0.9pHFig.9pHchangesduringelectrolysisρmgL1—253.42—500.03—750.0.1.54Am2.10ρFig.10Effectofchlorineionmassconcentrationontheremovalrateofammonianitrogen.11Fig.11Ammonianitrogenandphosphorusremovalamountvs.powerrequiredduringelectrocoagulation2.8.11.11.29.15gt4.3kW·h37.68gt0.86kW·h0.15~0.500.02~0.04kW·hg.3a、.b286、293、303KRedlich-PetersonLangmuirFreundlichGibbs-20~0kJmol|G|ΔH0.cpHpH.d0.15~0.500.02~0.04kW·hg.References1.M.2001131-202.2AKBALFCAMCS.Copperchromiumandnickelremovalfromme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