超临界水氧化去除含酚废水TOC的动力学研究

TOCX,,,,,,(,300071):,,(P=30MPa,T=400,440,480,520),TOC10,TOC2.15171.7kJ/mol,A2.991011:;;;:X703:A:1002-1264(1999)04-0001-031(Supercriticalwateroxidation,SCWO),,,(T374,P22MPa),CO2H2ON2,,[1],,,,SCWOTesteretal.[2]SCWOTester[3-5]250,COCH4NH3,(TOC),TOC21,,28mL,;30%,(TOC400-450mg/L),,,20min,TOC[6](GB13193-91)10,30MPa,400440480520,112419998URBANENVIRONMENT&URBANECOLOGYVol12,No.4Aug.1999X(No.973606511):1999-06-241234567133.1TOC(X):X=1-TOC/TOC0(1):TOCTOC,mg/L;TOC0TOC,mg/L(t),:t=V0/Fr=V0/Finin/r(2):t-,(s);V0,(cm3);Fr,cm3/s;Fin,cm3/s;in,cm3/g;r,cm3/gH2O2,[7],:CiHjOk+(2i+j/2-k)H2O2iCO2+(2i+j-k)H2O(3)TOC,,:-d[TOC]/dt=k[TOC]a[H2O2]b(4):t,s;kTOCx,(1)(4):dx/dt=k(1-x)a[TOC]a-10[H2O2]b(5),H2O210,[H2O2],[H2O2]bt=0,x=0,5:(1-x)1-a-1=(a-1)k[TOC]0a-1t(a1)(6)ln(1-x)=-kt(a=1)(7)3.2130MPa,1(6)a2.15,k(2)130MPa,TOCT(K)[TOC]0(mg/L)[TOC](mg/L)t(s)TOCX(%)673.2436.149.111.888.7436.154.912.687.4436.166.412.884.8436.156.813.187.0436.151.413.388.2436.165.314.285.0436.159.115.186.4436.153.716.287.7436.156.817.687.0436.156.819.187.0436.155.720.387.2436.153.423.487.8436.148.425.788.9436.148.830.288.8436.150.333.588.5436.146.437.189.4436.137.647.991.4436.121.168.595.2436.114.681.796.7713.2412.958.35.585.9412.963.06.084.8412.944.56.989.2412.961.48.085.1412.960.79.485.3412.953.011.687.2412.931.915.592.3412.96.523.598.4412.91.240.799.7753.2412.93.573.099.9412.93.838.699.9412.913.126.399.8412.96.119.498.5412.94.215.599.0412.92.713.499.3412.90.010.998.9412.95.010.098.8412.913.48.696.7793.2412.93.164.899.9412.93.832.199.9412.93.817.199.7412.90.013.899.3412.95.011.199.3412.90.09.899.1412.91.98.498.8412.97.77.598.12kT(K)k673.20.006865713.20.2018753.20.6251793.20.7322212419993.3,:dlnk/dT=-Ea/RT2(8):k=Aexp(-Ea/RT)(9)lnk=-Ea/RT+lnA(10)lnk1/TEa=171.7kJ/mol,A=2.991011TOC:(1-x)-1.15-1=3.441011exp(-171.7/RT)[TOC]01.15t(11)[5],,,2TOC,(11)TOC,10%22,4,H2O2,TOC,(H2O2)10,TOC2.15,,,Ea171.7kJ/mol,A=2.991011[1]..,1998;11(3):8-11[2]TesterTWetal.Supercriticalwateroxidationtechnology:processdevelopmentandfundamentalresearch.ACSSymp.Ser.1993;518:35[3]HellingRKandTesterJW.OxidationkineticsofCarbonmonoxideinsupercriticalwater.Energy&Fuels.1981;1:417[4]HellingRKandTesterJW.Oxidationofsimplecom2poundsandmixturesinsupercriticalwater:CarbonMonoxide,AmmoniaandEthanol,Environ.Sci.Tech2nol.1988;22:1319[5]HolgateHRetal.Fundamentalkineticsandmochanismsofhydrogenoxidationinsupercriticalwater.Combust.Sci.andTech.1993;88:369-397[6].1996.1,:,1996:477-480[7]..:,1989:182-193:,1973,,5GlobalKineticsforSupercriticalWaterOxidationofPhenolWastewaterLIHui,ZHUANGYuan2yi,YANGKe2lian,YUANYou2cai,GUWen2xin,YANLi,LIYang(DepartmentofEnvironmentalScience,NankaiUniversity,Tianjin300071)Abstract:Supercriticalwateroxidation(SCWO)hasbecomeawell-knowntreatmenttechnologyforaqueouswaste.Thispaperfocusedonthetreatmentofphenolwastewaterbyusingaself2madecontinuous2flowreactorsys2tem.Dilutedaqueoussolutionsofphenolwereoxidizedat400,440,480,520at30MParespectively.Theglobalkineticsfortotalorganiccarbon(TOC)disappearancewasdescribedbyapower2law,thatwas2.15orderinTOC.Theactivationenergywas171.7kJ/mol,andtheArrheniuspre-exponentialfactorwas2.991011.Keywords:phenolwastewater;supercriticalwater;oxidation;kinetics3TOC