气体氛围对低温等离子体协同控制汞和二噁英的影响
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摘要
为了控制垃圾焚烧烟气中排放的汞和二噁英类物质,利用窄脉冲电源放电,通过自行设计的实验装置系统,以1,2,4–三氯苯作为二噁英类似物(TCB),考察了气体氛围对低温等离子体协同控制汞和二噁英的影响。实验结果表明:NO、SO_2、HCl 3种酸性气体对消除降解TCB存在竞争作用,SO_2和HCl对TCB消除竞争影响更加显著;比较无/全NO、SO_2、HCl 3种酸性气体综合氛围,Hg~0氧化率受气体氛围影响变化明显,各气体组分对Hg0氧化作用复杂,NO对降解效果的影响比较关键;在"酸性气体+Hg~0+TCB"的烟气氛围中,Hg~0氧化和TCB降解消除相互影响效果不同,各种烟气成分对结果贡献复杂,系统协同控制效果还能够继续提升;根据生成产物反推,·OH在TCB降解消除两大步历程中作用关键。该研究将为焚烧行业烟气协同控制新技术提供数据支持。
By utilizing a narrow pulse power discharge, synergistic control of mercury and dioxins was studied by using 1,2,4-trichlorobenzene(TCB) as a dioxin analogue through a self-designed experimental system in order to control the emission of mercury and dioxin substances in waste incineration flue gas. The competitive effects of NO, SO_2 and HCl on the TCB removal by non-thermal plasma were discussed. In the three sour gas atmospheres, the oxidation of Hg~0 decreased by about 10%, the oxidation of Hg~0 by each gas component was complex, and the effect of NO on the degradation was relatively crucial. In the flue gas atmosphere of ‘acid gas + Hg~0 + TCB', the interaction between Hg~0 oxidation and TCB degradation was different. The contribution of various flue gas components to the results was complicated, but the overall experimental results show that the synergistic control effect of the system can continue to improve. According to the reversion of generated products, ·OH plays an important role in the synergistic control of the degradation of Hg~0 and TCB. This work should provide basic research data for flue gas synergetic control in incineration industry.
By utilizing a narrow pulse power discharge, synergistic control of mercury and dioxins was studied by using 1,2,4-trichlorobenzene(TCB) as a dioxin analogue through a self-designed experimental system in order to control the emission of mercury and dioxin substances in waste incineration flue gas. The competitive effects of NO, SO_2 and HCl on the TCB removal by non-thermal plasma were discussed. In the three sour gas atmospheres, the oxidation of Hg~0 decreased by about 10%, the oxidation of Hg~0 by each gas component was complex, and the effect of NO on the degradation was relatively crucial. In the flue gas atmosphere of ‘acid gas + Hg~0 + TCB', the interaction between Hg~0 oxidation and TCB degradation was different. The contribution of various flue gas components to the results was complicated, but the overall experimental results show that the synergistic control effect of the system can continue to improve. According to the reversion of generated products, ·OH plays an important role in the synergistic control of the degradation of Hg~0 and TCB. This work should provide basic research data for flue gas synergetic control in incineration industry.
引文
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[14]KYUNG B K,BYUN Y,CHO M,et al.Influence of gas components on the oxidation of elemental mercury by positive pulsed corona discharge[J].Main Group Chemistry,2008,7(3):191-204.
[15]WANG Z H,JIANG S D,ZHU Y Q,et al.Investigation on elemental mercury oxidation mechanism by non-thermal plasma treatment[J].Fuel Processing Technology,2010,91(11):1395-1400.
[16]WANG M,ZHU T,LUO H,et al.Oxidation of gaseous elemental mercury in a high voltage discharge reactor[J].Journal of Environmental Sciences,2009,21(12):1652-1657.
[17]AN J T,SHANG K F,LU N,et al.Oxidation of elemental mercury by active species generated from a surface dielectric barrier discharge plasma reactor[J].Plasma Chemistry and Plasma Processing,2014,34(1):217-228.
[18]赵蔚欣,段钰锋,张君,等.低温等离子体耦合氯化钙模拟烟气脱汞实验研究[J].中国电机工程学报,2016,36(4):1002-1008.ZHAO Weixin,DU Yufeng,ZHANG Jun,et al.Experimental study on mercury removal by non-thermal plasma coupled with Ca Cl2[J].Proceddings of the CSEE,2016,36(4):1002-1008.
[19]王勇.滑动弧等离子体降解氯苯类有机污染物的实验研究[D].杭州:浙江大学,2013.WANG Yong.Experimental research of the degradation of chlorobenzenes with gliding arc plasma[D].Hangzhou,China:Zhejing University,2013.
[20]林文锋,张斌,侯文慧,等.低温等离子体促进烟气中单质汞氧化的特性分析[J].中国电机工程学报,2010,30(2):72-76.LIN Wenfeng,ZHANG Bin,HOU Wenhui,et al.Enhanced oxidation of elemental Mercury in simulated FLUE gas by non-thermal plasma[J].Proceedings of the CSEE,2010,30(2):72-76.
[21]BYUN Y,KOH D J,SHIN D N.Removal mechanism ofelemental mercury by using non-thermal plasma[J].Chemosphere,2011,83(1):69-75.
[22]郑光明,朱承驻,张仁熙,等.平行板双介质阻挡放电处理水相中氯酚的脱氯机理[J].环境科学学报,2004,24(6):962-968.ZHENG Guangming,ZHU Chengzhu,ZHANG Renxi,et al.Dechlorination mechanism of chlorophenol in aqueous solution using lowtemperature plasma[J].Acta Scientiae Circumstantiae,2004,24(6):962-968.
[23]杜长明.滑动弧放电等离子体降解气相及液相中有机污染物的研究[D].杭州:浙江大学,2006.DU Changming.Study on the degradation of organic pollutants in gas phase and liquid phase by sliding arc discharge plasma[D].Hangzhou,China:Zhejiang University,2006.
[24]CHU W,KWAN C Y.The direct and indirect photolysis of 4,4'-dichlorobiphenyl in various surfactant/solvent-aided systems[J].Water Research,2002,36(9):2187-2194.
[25]周波,林文峰,余刚,等.脉冲介质阻挡放电条件下NO/O2/N2/Hg0体系反应动力学模拟[J].工程热物理学报,2009,30(2):343-346.ZHOU Bo,LIN Wenfeng,YU Gang,et al.Kinetic simulation of NO/O2/N2/Hg0 streamer under dielectric barrier discharge[J].Journal of Engineering Thermophysics,2009,30(2):343-346.
[2]竹涛,和娴娴,陈锐,等.低温等离子体反应器去除挥发性有机化合物的能效分析[J].高电压技术,2014,40(10):2986-2990.ZHU Tao,HE Xianxian,CHEN Rui,et al.Energy efficiency analysis of nonthermal plasma reactor for VOCs decomposition[J].High Voltage Engineering,2014,40(10):2986-2990.
[3]杨国清,曹一崧,邵朱夏,等.碱液协同介质阻挡放电处理含氮氧化物废气[J].高电压技术,2018,44(12):4013-4019.YANG Guoqing,CAO Yisong,SHAO Zhuxia,et al.Lye synergy dielectric barrier discharge on removing NOx of exhaust[J].High Voltage Engineering,2018,44(12):4013-4019..
[4]吴祖良,郑欣丹,谢德援,等.介质阻挡放电协同催化萘降解[J].高电压技术,2017,43(8):2660-2665.WU Zuliang,ZHENG Xindan,XIE Deyuan,et al.Naphthalene degradation by dielectric barrier discharge coupling catalyst[J].High Voltage Engineering,2017,43(8):2660-2665.
[5]竹涛,马名烽,李冉冉,等.等离子体联合动力波技术协同控制铅锌冶炼烟气中Hg、SO2、NOx实验研究[J].高电压技术,2016,42(2):384-391.ZHU Tao,MA Mingfeng,LI Ranran,et al.Experimental research on synergistic control technology of Hg,SO2 and NOx in lead and zinc smelting fume by plasma with dynamic wave technology[J].High Voltage Engineering,2016,42(2):384-391.
[6]姚水良,毛灵爱,张霞,等.等离子体复合微量贵金属催化反应器催化氧化苯的机理分析[J].高电压技术,2017,43(12):3973-3980.YAO Shuiliang,MAO Lingai,ZHANG Xia,et al.Mechanism analysis of benzene catalytic oxidation using plasma reactor with micro-level noble catalysts[J].High Voltage Engineering,2017,43(12):3973-3980.
[7]张丽军.低温等离子体协同处理含汞废气和二恶英的研究[D].北京:华北电力大学,2017.ZHANG Lijun.Research on simultaneous removal mercury and dioxinsfrom flue gas with non-thermal plasma[D].Beijing,China:North China Electric Power University,2017.
[8]俞明锋,付建英,詹明秀,等.生活废弃物焚烧处置烟气中二噁英排放特性研究[J].环境科学学报,2018,38(5):1983-1988.YU Mingfeng,FU Jianying,ZHAN Mingxiu,et al.The research of PCDD/Fs emission characteristics in flue gas from municipal solid waste incinerations[J].Acta Scientiae Circumstantiae,2018,38(5):1983-1988.
[9]任咏.滑动弧等离子体降解二噁英类有机污染物的基础研究[D].杭州:浙江大学,2015.REN Yong.Basic study on degradation of dioxin organic pollutants by sliding arc plasma[D].Hangzhou,China:Zhejing University,2015.
[10]吴彦,占部武生.脉冲放电法消除汞蒸气的实验研究[J].环境科学学报,1996,16(2):221-225.WU Yan,ZHANBU Wusheng.Removal of mercury vapor by pulsed corona discharge[J].Acta Scientiae Circumstantiae.1996,16(2):221-225.
[11]林文锋,张斌,侯文慧,等.低温等离子体促进烟气中单质汞氧化的特性分析[J].中国电机工程学报,2010,30(2):72-76.LIN Wenfeng,ZHANG Bin,HOU Wenhui,et al.Enhanced oxidation of elemental mercury in simulated flue gas by non-thermal plasma[J].Proceedings of the CSEE,2010,30(2):72-76.
[12]KO K B,BYUN Y,CHO M,et al.Influence of HCl on oxidation of gaseous elemental Mercury by dielectric barrier discharge process[J].Chemosphere,2008,71(9):1674-1682.
[13]KO K B,BYUN Y,CHO M,et al.Pulsed corona discharge for oxidation of gaseous elemental mercury-article no.251503[J].Applied Physics Letters,2008,92(25):4048-4244.
[14]KYUNG B K,BYUN Y,CHO M,et al.Influence of gas components on the oxidation of elemental mercury by positive pulsed corona discharge[J].Main Group Chemistry,2008,7(3):191-204.
[15]WANG Z H,JIANG S D,ZHU Y Q,et al.Investigation on elemental mercury oxidation mechanism by non-thermal plasma treatment[J].Fuel Processing Technology,2010,91(11):1395-1400.
[16]WANG M,ZHU T,LUO H,et al.Oxidation of gaseous elemental mercury in a high voltage discharge reactor[J].Journal of Environmental Sciences,2009,21(12):1652-1657.
[17]AN J T,SHANG K F,LU N,et al.Oxidation of elemental mercury by active species generated from a surface dielectric barrier discharge plasma reactor[J].Plasma Chemistry and Plasma Processing,2014,34(1):217-228.
[18]赵蔚欣,段钰锋,张君,等.低温等离子体耦合氯化钙模拟烟气脱汞实验研究[J].中国电机工程学报,2016,36(4):1002-1008.ZHAO Weixin,DU Yufeng,ZHANG Jun,et al.Experimental study on mercury removal by non-thermal plasma coupled with Ca Cl2[J].Proceddings of the CSEE,2016,36(4):1002-1008.
[19]王勇.滑动弧等离子体降解氯苯类有机污染物的实验研究[D].杭州:浙江大学,2013.WANG Yong.Experimental research of the degradation of chlorobenzenes with gliding arc plasma[D].Hangzhou,China:Zhejing University,2013.
[20]林文锋,张斌,侯文慧,等.低温等离子体促进烟气中单质汞氧化的特性分析[J].中国电机工程学报,2010,30(2):72-76.LIN Wenfeng,ZHANG Bin,HOU Wenhui,et al.Enhanced oxidation of elemental Mercury in simulated FLUE gas by non-thermal plasma[J].Proceedings of the CSEE,2010,30(2):72-76.
[21]BYUN Y,KOH D J,SHIN D N.Removal mechanism ofelemental mercury by using non-thermal plasma[J].Chemosphere,2011,83(1):69-75.
[22]郑光明,朱承驻,张仁熙,等.平行板双介质阻挡放电处理水相中氯酚的脱氯机理[J].环境科学学报,2004,24(6):962-968.ZHENG Guangming,ZHU Chengzhu,ZHANG Renxi,et al.Dechlorination mechanism of chlorophenol in aqueous solution using lowtemperature plasma[J].Acta Scientiae Circumstantiae,2004,24(6):962-968.
[23]杜长明.滑动弧放电等离子体降解气相及液相中有机污染物的研究[D].杭州:浙江大学,2006.DU Changming.Study on the degradation of organic pollutants in gas phase and liquid phase by sliding arc discharge plasma[D].Hangzhou,China:Zhejiang University,2006.
[24]CHU W,KWAN C Y.The direct and indirect photolysis of 4,4'-dichlorobiphenyl in various surfactant/solvent-aided systems[J].Water Research,2002,36(9):2187-2194.
[25]周波,林文峰,余刚,等.脉冲介质阻挡放电条件下NO/O2/N2/Hg0体系反应动力学模拟[J].工程热物理学报,2009,30(2):343-346.ZHOU Bo,LIN Wenfeng,YU Gang,et al.Kinetic simulation of NO/O2/N2/Hg0 streamer under dielectric barrier discharge[J].Journal of Engineering Thermophysics,2009,30(2):343-346.