脉冲电晕放电等离子体去除污染土壤热脱附尾气中的DDTs
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摘要
为探索新型产业化应用热脱附尾气处理技术,采用脉冲电晕放电等离子体技术对含DDTs的热脱附尾气进行处理,考察了工艺参数如脉冲电压、脉冲频率、ρ(DDTs)和停留时间对DDTs处理效果的影响,分析了DDTs经低温等离子体处理后的分解产物.结果表明,DDTs的去除率随脉冲电压的升高、脉冲频率的增大和停留时间的延长而增加,随进气中ρ(DDTs)的升高而降低,但去除量随进气中ρ(DDTs)的升高而增大.进气中的ρ(DDTs)为30.0 mg/m~3,停留时间为10 s,脉冲电压为30.0 kV,脉冲频率为50 Hz时,DDTs的去除率为82.5%.低温等离子体处理后,尾气中的ρ(p,p'-DDT)、ρ(o,p'-DDT)和ρ(p,p'-DDD)降低,ρ(p,p'-DDE)反而升高,另有微量的二苯甲烷、二苯甲醇、4,4'-二氯二苯甲烷、2,4'-二氯苯甲酮和1,1-双(对氯苯)-2-氯乙烯等分解产物被检出.研究显示,脉冲放电等离子体技术具有去除效率高等特点,可有效去除含DDTs的热脱附尾气.
In order to explore a new industrial application of thermal desorption off-gas treatment technique,pulsed corona discharge plasma was applied to remove DDTs in thermal desorption off-gas.The effects of pulse peak voltage,pulse frequency,inlet concentrations and residence time on DDTs removal rate were investigated.The degradation products of DDTs after the treatment were also analyzed.The DDTs removal rate increased with the increase of the pulse peak voltage,the pulse frequency and the gas residence time.The DDTs removal rate decreased with the increase of ρ( DDTs),but the removal quantities of DDTs increased with the increase of ρ( DDTs) in the feed gas.DDTs removal efficiency was 82.5% when 30.0 mg/m~3 of ρ( DDTs) in off-gas was treated for 10 s at pulse voltage of 30.0 kV and pulse frequency of 50 Hz.After treatment,ρ( p,p'-DDT),ρ( o,p'-DDT) and ρ( p,p'-DDD) in off-gas decreased,but ρ( p,p'-DDE)increased.In addition,DM,BH,DDM,DBP and DDMU with low contents were detected as the degradation products of DDTs.In conclusion,the pulsed discharge plasma is characterized as high removal efficiency,which can effectively remove thermal desorption offgas containing DDTs.
In order to explore a new industrial application of thermal desorption off-gas treatment technique,pulsed corona discharge plasma was applied to remove DDTs in thermal desorption off-gas.The effects of pulse peak voltage,pulse frequency,inlet concentrations and residence time on DDTs removal rate were investigated.The degradation products of DDTs after the treatment were also analyzed.The DDTs removal rate increased with the increase of the pulse peak voltage,the pulse frequency and the gas residence time.The DDTs removal rate decreased with the increase of ρ( DDTs),but the removal quantities of DDTs increased with the increase of ρ( DDTs) in the feed gas.DDTs removal efficiency was 82.5% when 30.0 mg/m~3 of ρ( DDTs) in off-gas was treated for 10 s at pulse voltage of 30.0 kV and pulse frequency of 50 Hz.After treatment,ρ( p,p'-DDT),ρ( o,p'-DDT) and ρ( p,p'-DDD) in off-gas decreased,but ρ( p,p'-DDE)increased.In addition,DM,BH,DDM,DBP and DDMU with low contents were detected as the degradation products of DDTs.In conclusion,the pulsed discharge plasma is characterized as high removal efficiency,which can effectively remove thermal desorption offgas containing DDTs.
引文
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[33]LAL R,SAXENA D M.Accumulation,metabolism,and effects of organochlorine insecticides on microorganisms[J].Microbiological Reviews,1982,46(1):95-127.
[34]US Environmental Protection Agency.Microbial decomposition of chlorinated aromatic compounds[R].Washington DC:Office of Research and Development,1986:138-145.
[35]VANDENBROUCKE A M,DINH M T N,NUNS N,et al.Combination of non-thermal plasma and Pd/La Mn O3for dilute trichloroethylene abatement[J].Chemical Engineering Journal,2016,283(1):668-675.
[36]陈杰,翁扬,袁细宁,等.活性炭吸附协同介质阻挡放电降解甲硫醚[J].高校化学工程学报,2011,25(3):495-5 0 0.CHEN Jie,WENG Yang,YUAN Sining,et al.Decomposition of dimethyl sulfide in dielectric barrier plasma discharge assisted by active carbon[J].Journal of Chemical Engineering of Chinese Universities,2 0 1 1,2 5(3):4 9 5-5 0 0.
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[2]罗飞,宋静,潘云雨,等.典型滴滴涕废弃生产场地污染土壤的人体健康风险评估研究[J].土壤学报,2012,49(1):26-35.LUO Fei,SONG Jing,PAN Yunyu,et al.Human health risk assessment of contaminated soil:a case study of a former DDTmanufacturing site[J].Acta Pedologica Sinica,2012,49(1):26-35.
[3]SONG Qinqin,CHEN Hao,LI Yuhu,et al.Toxicological effects of benzo(a)pyrene,DDT and their mixture on the green mussel Perna viridis revealed by proteomic and metabolomic approaches[J].Chemosphere,2016,144:214-224.
[4]SUN Yuxin,HAO Qing,ZENG Xiaobo,et al.PCBs and DDTs in light-vented bulbuls from Guangdong Province,South China:levels,geographical pattern and risk assessment[J].Science of the Total Environment,2014,490:815-821.
[5]United States Navy.Overview of thermal desorption technology[R].California:Naval Facilities Engineering Services Center,1998.
[6]PERCIN P R D.Application of thermal desorption technologies to hazardous waste sites[J].Journal of Hazardous Materials,1995,40(2):203-209.
[7]ARESTA M,DIBENEDETTO A,FRAGALE C,et al.Thermal desorption of polychlorobiphenyls from contaminated soils and their hydrodechlorination using Pd-and Rh-supported catalysts[J].Chemosphere,2008,70(6):1052-1058.
[8]GAO Yanfei,YANG Hong,ZHAN Xinhua,et al.Scavenging of BHCs and DDTs from soil by thermal desorption and solvent washing[J].Environmental Science and Pollution Research,2013,20(3):1482-1492.
[9]US Environmental Protection Agency.Superfund remedy report 14th Edition[R].Washington DC:Office of Solid Waste and Emergency Response,2013.
[10]US Environmental Protection Agency.Reference guide to noncombustion technologies for remediation of persistent organic pollutants in soil,2ndEdition[R].Washington DC:Office of Solid Waste and Emergency Response,2010:18-42.
[11]ADDINK R,BAKKER W C M,OLIE K.Influence of HCl and Cl2on the formation of polychlorinated dibenzo-p-dioxins/dibenzofurans in a carbon/fly ash mixture[J].Environmental Science&Technology,1995,29(8):2055-2058.
[12]HIROTA K,SAKAI H,WASAKAZU W,et al.Application of electron beams for the treatment of VOC streams[J].Industrial&Engineering Chemistry Research,2004,43(5):1185-1191.
[13]CHANG J S.Physics and chemistry of plasma pollution control technology[J].Plasma Sources Science and Technology,2008,17(4):969-977.
[14]VANDENBROUCKE A M,MORENT R,DE GEYTER N,et al.Non-thermal plasmas for non-catalytic and catalytic VOC abatement[J].Journal of Hazardous Materials,2011,195:30-54.
[15]CHANG J S,CHAKRABARTI A,MYINT T A,et al.The effect of corona wire geometries on the destruction of volatile organic compounds in air by a pulsed corona discharge plasma reactoradsorbent hybrid system[J].Journal of Advanced Oxidation Technologies,1999,4(3):297-304.
[16]TETSUJI O,TADASHI T,KEI Y.Nonthermal plasma processing for dilute VOCs decomposition[J].IEEE Transactions on Industry Applications,2002,38(3):873-878.
[17]聂勇.脉冲放电等离子体治理有机废气放大试验研究[D].杭州:浙江大学,2004:9-12.
[18]CHANG J,LAWLESS P A,YAMAMOTO T.Corona discharge processes[J].IEEE Transactions on Plasma Science,1991,19(6):1152-1166.
[19]DURME J V,DEWULF J,SYSMANS W,et al.Abatement and degradation pathways of toluene in indoor air by positive corona discharge[J].Chemosphere,2007,68(10):1821-1829.
[20]赵雷,周中平.低温等离子体技术净化空气中的甲苯[J].环境科学研究,2006,19(4):70-73.ZHAO Lei,ZHOU Zhong ping.Purification of toluene in the air by nonthermal plasma technique[J].Research of Environmental Sciences,2006,19(4):70-73.
[21]叶招莲,宋潇潇,何锦丛,等.介质阻挡放电脱除模拟工业苯系物的可行性[J].环境科学学报,2008,28(12):2480-2486.YE Zhaolian,SONG Xiaoxiao,HE Jincong,et al.Feasibility of benzene series waste gas destruction with DBD technology[J].Acta Scientiae Circumstantiae,2008,28(12):2480-2486.
[22]VANDENBROUCKE A M,MORENT R,GEYTER N D,et al.Nonthermal plasmas for non-catalytic and catalytic VOC abatement[J].Journal of Hazardous Materials,2011,195(1):30-54.
[23]YAN Jianhua,PENG Zheng,LU Shengyong,et al.Destruction of PCDD/Fs by gliding arc discharges[J].Journal of Environmental Sciences,2007,19(11):1404-1408.
[24]REN Yong,LI Xiaodong,YU Liang,et al.Degradation of PCDD/Fs in fly ash by vortex-shaped gliding arc plasma[J].Plasma Chemistry and Plasma Processing,2013,33(1):293-305.
[25]WANG Tiecheng,LU Na,LI Jie,et al.Evaluation of the potential of pentachlorophenol degradation in soil by pulsed corona discharge plasma from soil characteristics[J].Environmental Science&Technology,2010,44(8):3105-3110.
[26]WANG Tiecheng,LU Na,LI Jie,et al.Degradation of pentachlorophenol in soil by pulsed corona discharge plasma[J].Journal of Hazardous Materials,2010,180(1/2/3):436-441.
[27]ZHANG Hao,MA Danyan,QIU Rongliang,et al.Non-thermal plasma technology for organic contaminated soil remediation:a review[J].Chemical Engineering Journal,2017,33:15.
[28]姜理英,曹书岭,朱润晔,等.介质阻挡放电对氯苯的降解特性及其产物分析[J].环境科学,2015(3):831-838.JIANG Liying,CAO Shuling,ZHU Runye,et al.Analysis of characteristics and products of chlorobenzene degradation with dielectric barrier discharge[J].Environmental Science,2015(3):831-838.
[29]曹静,杨建涛,陈杰,等.介质阻挡放电低温等离子体降解甲硫醚[J].高校化学工程学报,2007,21(6):1060-1064.CAO Jing,YANG Jiantao,CHEN Jie,et al.Decomposition of dimethyl sulfide with non-thermal plasma induced by dielectric barrier discharge[J].Journal of Chemical Engineering of Chinese Universities,2007,21(6):1060-1064.
[30]YU Liang,LI Xiaodong,TU Xin,et al.Decomposition of naphthalene by dc gliding arc gas discharge[J].Journal of Physical Chemistry A,2010,114(1):360-368.
[31]李战国,曹鹏,赵红杰.脉冲电晕等离子体降解有毒气体[J].环境化学,2012,31(6):869-873.LI Zhanguo,CAO Peng,ZHAO Hongjie.Decomposition of toxic gas by pulse corona plasma[J].Environmental Chemistry,2012,31(6):869-873.
[32]ALLAH Z A,WHITEHEAD J C,MARTINP.Remediation of dichloromethane(CH2Cl2)using non-thermal,atmospheric pressure plasma generated in a packed-bed reactor[J].Environmental Science&Technology,2014,48(1):558-565.
[33]LAL R,SAXENA D M.Accumulation,metabolism,and effects of organochlorine insecticides on microorganisms[J].Microbiological Reviews,1982,46(1):95-127.
[34]US Environmental Protection Agency.Microbial decomposition of chlorinated aromatic compounds[R].Washington DC:Office of Research and Development,1986:138-145.
[35]VANDENBROUCKE A M,DINH M T N,NUNS N,et al.Combination of non-thermal plasma and Pd/La Mn O3for dilute trichloroethylene abatement[J].Chemical Engineering Journal,2016,283(1):668-675.
[36]陈杰,翁扬,袁细宁,等.活性炭吸附协同介质阻挡放电降解甲硫醚[J].高校化学工程学报,2011,25(3):495-5 0 0.CHEN Jie,WENG Yang,YUAN Sining,et al.Decomposition of dimethyl sulfide in dielectric barrier plasma discharge assisted by active carbon[J].Journal of Chemical Engineering of Chinese Universities,2 0 1 1,2 5(3):4 9 5-5 0 0.
[37]叶招莲,曹长青,张仁熙,等.外置式联合等离子体光解技术去除苯乙烯气体[J].环境科学研究,2009,22(9):1083-1088.YE Zhaolian,CAO Changqing,ZHANG Renxi,et al.Decomposition of styrene gas with outer combined plasma photolysis(OCPP)technology[J].Research of Environmental Sciences,2009,22(9):1083-1088.