纳米零价铁基催化剂对二氧化氯漂白废水中氯代化合物的还原脱氯治理
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摘要
本论文阐述了二氧化氯漂白废水中氯代化合物产生的根源、种类及环境危害。论述了现有二级生物处理和高级氧化技术对氯代化合物的非针对性及局限性。重点介绍了利用纳米零价铁及其改性物实现氯代化合物,尤其是氯代芳香族组分的高效还原脱氯,降解为低氯甚至无氯产品。论文还探讨了造纸白水中细小纤维作为催化剂绿色水凝胶载体的可行性。
This paper expounds the origin,types and the environmental hazards of chlorinated compounds contained in Cl O2 bleaching effluent,and discusses the limitations of the existing secondary biological wastewater treatment,and the advanced oxidation technologies to oxidize chlorinated compounds without selectivity. A method of using nano zero-valent iron( NZVI) nanoparticle and the NZVI-based materials has been introduced to dechlorinate chlorinated compounds stepwise,especially resistant chlorinated aromatic components,until the less chlorination products,or even products without chlorine was converted. This high reductive dechlorination treatment can be adopted to reduce the environment pollution resulted by high content of chlorinated compounds,and may realize the sustainable development of the pulp and paper industry. Paper also put forward the feasibility of fine recycled in white water during papermaking process as the green hydrogel carrier for NZVI-based catalyst.
This paper expounds the origin,types and the environmental hazards of chlorinated compounds contained in Cl O2 bleaching effluent,and discusses the limitations of the existing secondary biological wastewater treatment,and the advanced oxidation technologies to oxidize chlorinated compounds without selectivity. A method of using nano zero-valent iron( NZVI) nanoparticle and the NZVI-based materials has been introduced to dechlorinate chlorinated compounds stepwise,especially resistant chlorinated aromatic components,until the less chlorination products,or even products without chlorine was converted. This high reductive dechlorination treatment can be adopted to reduce the environment pollution resulted by high content of chlorinated compounds,and may realize the sustainable development of the pulp and paper industry. Paper also put forward the feasibility of fine recycled in white water during papermaking process as the green hydrogel carrier for NZVI-based catalyst.
引文
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[3]李军,何水淋,李智,等.蔗渣浆ECF短序漂白流程的对比[J].华南理工大学学报(自然科学版),2014,42(2):14-20.
[4]Manoj,Kumar,Ghosh,et al.Minimization of Phenols and Phenolic Compounds in Pulp and Paper Industries:Biological Approaches[J].J.Chem.Chem.Eng.2011,(5):595-601.
[5]Solomon K,Bergman H,Huggett R,et al.A review and assessment of the ecological risks associated with the use of chlorine dioxide for the bleaching of pulp[R],Report prepared for the Alliance for Environmental Technology,1993.
[6]EPA,Priority Pollutant List[EB/OL].http://www.epa.gov/safewater,2004.
[7]J Dorica.Removal of AOX from Bleach Plant Effluents by Alkaline Hydrolysis[J].Journal of Pulp and Paper Science,1992,18(6):231-237.
[8]Schnell A,Steel P,Melcer H,et a1.Enhanced biological treatment of bleached kraft mill effluents-I.Removal of chlorinated organic compounds and toxicity[J],Water Research,2000,34(2):493-500.
[9]Deshmukh N S,Lapsiya K L,Savant D V,et a1.Upflow anaerobic filter for the degradation of adsorbable organic halides(AOX)from bleach composite wastewater of pulp and paper industry[J].Chemosphere,2009,75(9):1179-1185.
[10]Majumder P S,Gupta S K.Effect of carbon sources and shock loading on the removal of chlorophenols in sequential anaerobicaerobic reactors[J].Bioresource Technology,2008,99(8):2930-2937.
[11]Atuanya E I,Purohit H J,Chakrabarti T.Anaerobic and aerobic biodegradation of chlorophenols using UASB and ASG bioreactors[J].World Journal of Microbiology&Biotechnology,2000,16(1):95-98.
[12]Parilti N B,Akten D.Optimization of Ti O2/Fe(III)/solar UV conditions for the removal of organic contaminants in pulp mill effluents[J].Desalination,201l,265(1-3):37-42.
[13]Gaya U I,Abdullah A H,Hussein M Z,et al.Photocatalytic removal of 2,4,6-trichlorophenol from water exploiting commercial Zn O powder[J],Desalination,2010,263(1-3):176-182.
[14]Ugurlu Mehmet,Karaoglu M Hamdi.Removal of AOX,total nitrogen and chlorinated lignin from bleached Kraft mill effluents by UV oxidation in the presence of hydrogen peroxide utilizing Ti O2as photocatalyst[J],Environmental Science and Pollution Research.2009,16(3):265-273.
[15]Chaparro T R,Botta C M,Pires,E C.Toxicity and recalcitrant compound removal from bleaching pulp plant effluents by an integrated system:anaerobic packed-bed bioreactor and ozone[J].Water Science and Technology,2010,6l(1):199-205.
[16]Sweeny K H.American water works association research foundation[R].Water Reuse Symposium,1979,(2):1487-1491.
[17]Rabideau A J,Shen P L,Khandelwal A.Feasibility of amending slurry walls with zero-valent iron[J].Journal of Geotechnical and Geoenvironmental Engineering,1999,125(4):330-333.
[18]Zhang W X,Wang C B,Lien H L.Treatment of chlorinated organic contaminants with nanoscale bimetallic particles[J].Catalysis Today,1998,40(4):387-395.
[19]Lien H L,Zhang W X.Transformation of chlorinated methanes by nanoscale iron particles[J].Journal of Environmental Engineering-Asce,1999,125(11):1042-1047.
[20]Lien H L,Zhang W X.Nanoscale iron particles for complete reduction of chlorinated ethenes[J].Colloids and Surfaces aPhysicochemical and Engineering Aspects,2001,191(1-2):97-105.
[21]卫建军.纳米级Pd-Fe双金属对水中氯酚的催化脱氯研究[D].浙江:浙江大学,2004.
[22]He F,Zhao D.Preparation and characterization of a new class of starch-stabilized bimetallic nanoparticles for degradation of chlorinated hydrocarbons in water[J].Environmental Science&Technology,2005,39(9):3314-3320.
[23]He F,Zhao D.Manipulating the size and dispersibility of zerovalent iron nanoparticles by use of carboxymethyl cellulose stabilizers[J].Environmental Science&Technology,2007,41(17):6216-6221.
[24]Liu T,Zhao L,Sun D,et al.Entrapment of nanoscale zerovalent iron in chitosan beads for hexavalent chromium removal from wastewater[J].Journal of Hazardous Materials,2010,184(1-3):724-730.
[25]Tiraferri A,Sethi R.Enhanced transport of zerovalent iron nanoparticles in saturated porous media by guar gum[J].Journal of Nanoparticle Research,2009,11(3),635-645.
[26]Zhou H Y,Han J,Baig S A,et al.Dechlorination of 2,4-dichlorophenoxyacetic acid by sodium carboxymethyl cellulose-stabilized Pd/Fe nanoparticles[J].Journal of Hazardous Materials,2011,198:7-12.
[27]Ma H,Huang Y,Shen M,et al.Enhanced dechlorination of trichloroethylene using electrospun polymer nanofibrous mats immobilized with iron/palladium bimetallic nanoparticles[J].Journal of Hazardous Materials,2012,211:349-356.
[28]Huang K C,Ehrman S H.Synthesis of iron nanoparticles via chemical reduction with palladium ion seeds[J].Langmuir,2007,23(3):1419-1426.
[29]Wang X,Li F,Yang J.Polyvinyl pyrrolidone-modified Pd/Fe nanoparticles for enhanced dechlorination of 2,4-dichlorophenal[J].Desalination and Water Treatment,2014,52(40-42):7925-7936.
[30]Dhar P,Kumar A,Katiyar V.Fabrication of cellulose nanocrystal supported stable Fe(0)nanoparticles:A sustainable catalyst for dye reduction,organic conversion and chemo-magnetic propulsion[J].Cellulose,2015,22(6):3755-3771.
[31]Su J,Lin S.,Chen,Z,et al.Dechlorination of p-chlorophenol from aqueous solution using bentonite supported Fe/Pd nanoparticles:Synthesis,characterization and kinetics[J],Desalination,2011,280(1-3):167-173.
[32]Babu N S,Lingaiah N,Kumar J V,et al.Studies on alumina supported Pd-Fe bimetallic catalysts prepared by deposition-precipitation method for hydrodechlorination of chlorobenzene[J].Applied Catalysis a-General,2009,367(1–2):70-76.
[33]Zheng T,Zhan J,He J,et al.Reactivity characteristics of nanoscale zerovalent iron-silica composites for trichloroethylene remediation[J].Environmental Science&Technology,2008,42(12):4494-4499.
[34]Busch J,Meissner T,Potthoff A,et al.A field investigation on transport of carbon-supported nanoscale zero-valent iron(n ZVI)in groundwater[J].Journal of Contaminant Hydrology,2015,181:59-68.
[35]Yang L,Lv L,Zhang S,et al.Catalytic dechlorination of monochlorobenzene by Pd/Fe nanoparticles immobilized within a polymeric anion exchanger[J].Chemical Engineering Journal,2011,178:161-167.
[36]Xu J,Lv X,Li J,et al.Simultaneous adsorption and dechlorination of 2,4-dichlorophenol by Pd/Fe nanoparticles with multiwalled carbon nanotube support[J].Journal of Hazardous Materials,2012,225:36-45.
[37]Wang X,Chen C,Liu H,et al.Preparation and characterization of PAA/PVDF membrane-immobilized Pd/Fe nanoparticles for dechlorination of trichloroacetic acid[J].Water Research,2008,42(18):4656-4664.
[38]Ozay H,Kubilay S,Aktas N,et al.Utilization of Environmentally Benign Hydrogels and Their Networks as Reactor Media in the Catalytic Reduction of Nitrophenols[J].International Journal of Polymeric Materials,2011,60(2):163-173.
[39]Sahiner N.In situ metal particle preparation in cross-linked poly(2-acrylamido-2-methyl-1-propansulfonic acid)hydrogel networks[J].Colloid and Polymer Science,2006,285(3):283-292.
[40]Andarini M,Lazim A.Nata De Coco(NDC)Hydrogel as Nanoreactors for Preparation Iron Nanoparticles(Fe Nps)from Ferrocenium Reduction[C].AIP Conference Proceedings,2014,1614,414-418.
[2]Ali M,Sreekrishnan T R.Aquatic toxicity from pulp and paper mill effluents:a review[J].Advances in Environmental Research,2001,5(2):175-196.
[3]李军,何水淋,李智,等.蔗渣浆ECF短序漂白流程的对比[J].华南理工大学学报(自然科学版),2014,42(2):14-20.
[4]Manoj,Kumar,Ghosh,et al.Minimization of Phenols and Phenolic Compounds in Pulp and Paper Industries:Biological Approaches[J].J.Chem.Chem.Eng.2011,(5):595-601.
[5]Solomon K,Bergman H,Huggett R,et al.A review and assessment of the ecological risks associated with the use of chlorine dioxide for the bleaching of pulp[R],Report prepared for the Alliance for Environmental Technology,1993.
[6]EPA,Priority Pollutant List[EB/OL].http://www.epa.gov/safewater,2004.
[7]J Dorica.Removal of AOX from Bleach Plant Effluents by Alkaline Hydrolysis[J].Journal of Pulp and Paper Science,1992,18(6):231-237.
[8]Schnell A,Steel P,Melcer H,et a1.Enhanced biological treatment of bleached kraft mill effluents-I.Removal of chlorinated organic compounds and toxicity[J],Water Research,2000,34(2):493-500.
[9]Deshmukh N S,Lapsiya K L,Savant D V,et a1.Upflow anaerobic filter for the degradation of adsorbable organic halides(AOX)from bleach composite wastewater of pulp and paper industry[J].Chemosphere,2009,75(9):1179-1185.
[10]Majumder P S,Gupta S K.Effect of carbon sources and shock loading on the removal of chlorophenols in sequential anaerobicaerobic reactors[J].Bioresource Technology,2008,99(8):2930-2937.
[11]Atuanya E I,Purohit H J,Chakrabarti T.Anaerobic and aerobic biodegradation of chlorophenols using UASB and ASG bioreactors[J].World Journal of Microbiology&Biotechnology,2000,16(1):95-98.
[12]Parilti N B,Akten D.Optimization of Ti O2/Fe(III)/solar UV conditions for the removal of organic contaminants in pulp mill effluents[J].Desalination,201l,265(1-3):37-42.
[13]Gaya U I,Abdullah A H,Hussein M Z,et al.Photocatalytic removal of 2,4,6-trichlorophenol from water exploiting commercial Zn O powder[J],Desalination,2010,263(1-3):176-182.
[14]Ugurlu Mehmet,Karaoglu M Hamdi.Removal of AOX,total nitrogen and chlorinated lignin from bleached Kraft mill effluents by UV oxidation in the presence of hydrogen peroxide utilizing Ti O2as photocatalyst[J],Environmental Science and Pollution Research.2009,16(3):265-273.
[15]Chaparro T R,Botta C M,Pires,E C.Toxicity and recalcitrant compound removal from bleaching pulp plant effluents by an integrated system:anaerobic packed-bed bioreactor and ozone[J].Water Science and Technology,2010,6l(1):199-205.
[16]Sweeny K H.American water works association research foundation[R].Water Reuse Symposium,1979,(2):1487-1491.
[17]Rabideau A J,Shen P L,Khandelwal A.Feasibility of amending slurry walls with zero-valent iron[J].Journal of Geotechnical and Geoenvironmental Engineering,1999,125(4):330-333.
[18]Zhang W X,Wang C B,Lien H L.Treatment of chlorinated organic contaminants with nanoscale bimetallic particles[J].Catalysis Today,1998,40(4):387-395.
[19]Lien H L,Zhang W X.Transformation of chlorinated methanes by nanoscale iron particles[J].Journal of Environmental Engineering-Asce,1999,125(11):1042-1047.
[20]Lien H L,Zhang W X.Nanoscale iron particles for complete reduction of chlorinated ethenes[J].Colloids and Surfaces aPhysicochemical and Engineering Aspects,2001,191(1-2):97-105.
[21]卫建军.纳米级Pd-Fe双金属对水中氯酚的催化脱氯研究[D].浙江:浙江大学,2004.
[22]He F,Zhao D.Preparation and characterization of a new class of starch-stabilized bimetallic nanoparticles for degradation of chlorinated hydrocarbons in water[J].Environmental Science&Technology,2005,39(9):3314-3320.
[23]He F,Zhao D.Manipulating the size and dispersibility of zerovalent iron nanoparticles by use of carboxymethyl cellulose stabilizers[J].Environmental Science&Technology,2007,41(17):6216-6221.
[24]Liu T,Zhao L,Sun D,et al.Entrapment of nanoscale zerovalent iron in chitosan beads for hexavalent chromium removal from wastewater[J].Journal of Hazardous Materials,2010,184(1-3):724-730.
[25]Tiraferri A,Sethi R.Enhanced transport of zerovalent iron nanoparticles in saturated porous media by guar gum[J].Journal of Nanoparticle Research,2009,11(3),635-645.
[26]Zhou H Y,Han J,Baig S A,et al.Dechlorination of 2,4-dichlorophenoxyacetic acid by sodium carboxymethyl cellulose-stabilized Pd/Fe nanoparticles[J].Journal of Hazardous Materials,2011,198:7-12.
[27]Ma H,Huang Y,Shen M,et al.Enhanced dechlorination of trichloroethylene using electrospun polymer nanofibrous mats immobilized with iron/palladium bimetallic nanoparticles[J].Journal of Hazardous Materials,2012,211:349-356.
[28]Huang K C,Ehrman S H.Synthesis of iron nanoparticles via chemical reduction with palladium ion seeds[J].Langmuir,2007,23(3):1419-1426.
[29]Wang X,Li F,Yang J.Polyvinyl pyrrolidone-modified Pd/Fe nanoparticles for enhanced dechlorination of 2,4-dichlorophenal[J].Desalination and Water Treatment,2014,52(40-42):7925-7936.
[30]Dhar P,Kumar A,Katiyar V.Fabrication of cellulose nanocrystal supported stable Fe(0)nanoparticles:A sustainable catalyst for dye reduction,organic conversion and chemo-magnetic propulsion[J].Cellulose,2015,22(6):3755-3771.
[31]Su J,Lin S.,Chen,Z,et al.Dechlorination of p-chlorophenol from aqueous solution using bentonite supported Fe/Pd nanoparticles:Synthesis,characterization and kinetics[J],Desalination,2011,280(1-3):167-173.
[32]Babu N S,Lingaiah N,Kumar J V,et al.Studies on alumina supported Pd-Fe bimetallic catalysts prepared by deposition-precipitation method for hydrodechlorination of chlorobenzene[J].Applied Catalysis a-General,2009,367(1–2):70-76.
[33]Zheng T,Zhan J,He J,et al.Reactivity characteristics of nanoscale zerovalent iron-silica composites for trichloroethylene remediation[J].Environmental Science&Technology,2008,42(12):4494-4499.
[34]Busch J,Meissner T,Potthoff A,et al.A field investigation on transport of carbon-supported nanoscale zero-valent iron(n ZVI)in groundwater[J].Journal of Contaminant Hydrology,2015,181:59-68.
[35]Yang L,Lv L,Zhang S,et al.Catalytic dechlorination of monochlorobenzene by Pd/Fe nanoparticles immobilized within a polymeric anion exchanger[J].Chemical Engineering Journal,2011,178:161-167.
[36]Xu J,Lv X,Li J,et al.Simultaneous adsorption and dechlorination of 2,4-dichlorophenol by Pd/Fe nanoparticles with multiwalled carbon nanotube support[J].Journal of Hazardous Materials,2012,225:36-45.
[37]Wang X,Chen C,Liu H,et al.Preparation and characterization of PAA/PVDF membrane-immobilized Pd/Fe nanoparticles for dechlorination of trichloroacetic acid[J].Water Research,2008,42(18):4656-4664.
[38]Ozay H,Kubilay S,Aktas N,et al.Utilization of Environmentally Benign Hydrogels and Their Networks as Reactor Media in the Catalytic Reduction of Nitrophenols[J].International Journal of Polymeric Materials,2011,60(2):163-173.
[39]Sahiner N.In situ metal particle preparation in cross-linked poly(2-acrylamido-2-methyl-1-propansulfonic acid)hydrogel networks[J].Colloid and Polymer Science,2006,285(3):283-292.
[40]Andarini M,Lazim A.Nata De Coco(NDC)Hydrogel as Nanoreactors for Preparation Iron Nanoparticles(Fe Nps)from Ferrocenium Reduction[C].AIP Conference Proceedings,2014,1614,414-418.