SCR装置对焦炉煤气燃烧废气中PCDD/Fs、PCBs和PCNs的协同脱除
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摘要
研究了某大型焦化厂的选择性催化还原(SCR)装置对焦炉煤气燃烧废气中典型非故意产生持久性有机污染物(UPPOPs)的脱除效果,对SCR装置入口和出口废气和SCR装置降尘中二英(PCDD/Fs)、多氯联苯(PCBs)和多氯萘(PCNs)的全部异构体进行了分析.结果表明,SCR装置对总PCDD/Fs的脱除效率最高,为94.6%,对总PCBs和总PCNs的脱除率分别为74.7%和78.4%.SCR装置入口和出口废气中UP-POPs同系物的分布模式明显不同,入口处以高氯取代为主,出口处以低氯取代为主.SCR装置对高氯取代UP-POPs有更好的脱除效果.催化还原和催化氧化降解同时发生是SCR装置脱除废气中UP-POPs的重要机制.
The removal efficiencies of typical unintentionally produced persistent organic pollutants(UP-POPs) from flues gases from coke gas burning were obtained using selective catalytic reduction(SCR) equipment installed in a large coking plant.The total congeners of polychlorinated dibenzo-p-dioxins/dibenzofurans(PCDD/Fs),polychlorinated biphenyls(PCBs),and polychlorinated naphthalenes(PCNs) in the flue gases at the inlet and outlet of the SCR equipment and the dustfall were analyzed.The results show that the removal efficiency of the total PCDD/Fs was the highest(94.6%).The removal efficiencies of total PCBs and total PCNs were74.7% and 78.4%,respectively.The homologue profile of UP-POPs in the flue gases at the inlet of the SCR equipment notably differed from that at the outlet.Highly chlorinated UP-POPs predominated over the homologue profile of UP-POPs in the inlet flue gas,while low-chlorinated UP-POPs were predominant in the outlet flue gas.The SCR equipment achieved a better removal efficiency with respect to highly chlorinated UP-POPs.Catalytic reduction and catalytic oxidation degradation are both important mechanisms for the removal of UP-POPs from flue gas using SCR equipment.
The removal efficiencies of typical unintentionally produced persistent organic pollutants(UP-POPs) from flues gases from coke gas burning were obtained using selective catalytic reduction(SCR) equipment installed in a large coking plant.The total congeners of polychlorinated dibenzo-p-dioxins/dibenzofurans(PCDD/Fs),polychlorinated biphenyls(PCBs),and polychlorinated naphthalenes(PCNs) in the flue gases at the inlet and outlet of the SCR equipment and the dustfall were analyzed.The results show that the removal efficiency of the total PCDD/Fs was the highest(94.6%).The removal efficiencies of total PCBs and total PCNs were74.7% and 78.4%,respectively.The homologue profile of UP-POPs in the flue gases at the inlet of the SCR equipment notably differed from that at the outlet.Highly chlorinated UP-POPs predominated over the homologue profile of UP-POPs in the inlet flue gas,while low-chlorinated UP-POPs were predominant in the outlet flue gas.The SCR equipment achieved a better removal efficiency with respect to highly chlorinated UP-POPs.Catalytic reduction and catalytic oxidation degradation are both important mechanisms for the removal of UP-POPs from flue gas using SCR equipment.
引文
[1]Liu G R,Zheng M H,Lv P,et al.Estimation and characterization of polychlorinated naphthalene emission from coking industries[J].Environmental Science&Technology,2010,44(21):8156-8161.
[2]Liu G R,Zheng M H,Ba T,et al.A preliminary investigation on emission of polychlorinated dibenzo-p-dioxins/dibenzofurans and dioxin-like polychlorinated biphenyls from coke plants in China[J].Chemosphere,2009,75(5):692-695.
[3]Liu G R,Zheng M H,Liu W B,et al.Atmospheric emission of PCDD/Fs,PCBs,hexachlorobenzene,and pentachlorobenzene from the coking industry[J].Environmental Science&Technology,2009,43(24):9196-9201.
[4]Liu G R,Liu W B,Cai Z W,et al.Concentrations,profiles,and emission factors of unintentionally produced persistent organic pollutants in fly ash from coking processes[J].Journal of Hazardous Materials,2013,261:421-426.
[5]孙鹏程,李晓璐,成钢,等.焦炉烟气中二英类物质排放水平研究[J].环境科学,2014,35(7):2515-2519.Sun P C,Li X L,Cheng G,et al.Preliminary investigation on emission of PCDD/Fs and DL-PCBs through flue gas from coke plants in china[J].Environmental Science,2014,35(7):2515-2519.
[6]Hsu W T,Liu M C,Hung P C,et al.PAH emissions from coal combustion and waste incineration[J].Journal of Hazardous Materials,2016,318:32-40.
[7]Mokhtar M M,Taib R M,Hassim M H.Measurement of PCDD/Fs emissions from a coal-fired power plant in Malaysia and establishment of emission factors[J].Atmospheric Pollution Research,2014,5(3):388-397.
[8]Wang H C,Hwang J F,Chi K H,et al.Formation and removal of PCDD/Fs in a municipal waste incinerator during different operating periods[J].Chemosphere,2007,67(9):S177-S184.
[9]Van Caneghem J,De Greef J,Block C,et al.NOxreduction in waste incinerators by selective catalytic reduction(SCR)instead of selective non catalytic reduction(SNCR)compared from a life cycle perspective:a case study[J].Journal of Cleaner Production,2016,112(Pt 5):4452-4460.
[10]Liu X L,Wang J,Wang X,et al.Simultaneous removal of PCDD/Fs and NOxfrom the flue gas of a municipal solid waste incinerator with a pilot plant[J].Chemosphere,2015,133:90-96.
[11]Gallastegi-Villa M,Aranzabal A,Gonzalez-Marcos J A,et al.Tailoring dual redox-acid functionalities in VOx/Ti O2/ZSM5catalyst for simultaneous abatement of PCDD/Fs and NOxfrom municipal solid waste incineration[J].Applied Catalysis B:Environmental,2017,205:310-318.
[12]Chang M B,Chi K H,Chang S H,et al.Destruction of PCDD/Fs by SCR from flue gases of municipal waste incinerator and metal smelting plant[J].Chemosphere,2007,66(6):1114-1122.
[13]Chang M B,Chi K H,Chang-Chien G P.Evaluation of PCDD/F congener distributions in MWI flue gas treated with SCRcatalysts[J].Chemosphere,2004,55(11):1457-1467.
[14]Dvorˇák R,Chlápek P,Jecha D,et al.New approach to common removal of dioxins and NOxas a contribution to environmental protection[J].Journal of Cleaner Production,2010,18(9):881-888.
[15]Ji L J,Cao X,Lu S Y,et al.Catalytic oxidation of PCDD/F on a V2O5-WO3/Ti O2catalyst:effect of chlorinated benzenes and chlorinated phenols[J].Journal of Hazardous Materials,2018,342:220-230.
[16]Gallastegi-Villa M,Aranzabal A,Gonzalez-Marcos J A,et al.Metal-loaded ZSM5 zeolites for catalytic purification of dioxin/furans and NOxcontaining exhaust gases from MWI plants:effect of different metal cations[J].Applied Catalysis B:Environmental,2016,184:238-245.
[17]Yu M F,Li W W,Li X D,et al.Development of new transition metal oxide catalysts for the destruction of PCDD/Fs[J].Chemosphere,2016,156:383-391.
[18]Busca G,Baldi M,Pistarino C,et al.Evaluation of V2O5-WO3-Ti O2and alternative SCR catalysts in the abatement of VOCs[J].Catalysis Today,1999,53(4):525-533.
[19]Liljelind P,Unsworth J,Maaskant O,et al.Removal of dioxins and related aromatic hydrocarbons from flue gas streams by adsorption and catalytic destruction[J].Chemosphere,2001,42(5-7):615-623.
[20]Goemans M,Clarysse P,Joannès J,et al.Catalytic NOx reduction with simultaneous dioxin and furan oxidation[J].Chemosphere,2003,50(4):489-497.
[21]HJ 77.2-2008,环境空气和废气二英类的测定同位素稀释高分辨气相色谱-高分辨质谱法[S].HJ 77.2-2008,Ambient air and waste gas Determination of polychlorinated dibenzo-p-dioxins(PCDDs)and polychlorinated dibenzofurans(PCDFs)Isotope dilution HRGC-HRMS[S].
[22]GB 18485-2014,生活垃圾焚烧污染控制标准[S].GB 18485-2014,Standard for pollution control on the municipal solid waste incineration[S].
[23]Jones J,Ross J R H.The development of supported vanadia catalysts for the combined catalytic removal of the oxides of nitrogen and of chlorinated hydrocarbons from flue gases[J].Catalysis Today,1997,35(1-2):97-105.
[24]Debecker D P,Delaigle R,Hung P C,et al.Evaluation of PCDD/F oxidation catalysts:confronting studies on model molecules with tests on PCDD/F-containing gas stream[J].Chemosphere,2011,82(9):1337-1342.
[25]Wang Q L,Hung P C,Lu S Y,et al.Catalytic decomposition of gaseous PCDD/Fs over V2O5/Ti O2-CNTs catalyst:effect of NOand NH3addition[J].Chemosphere,2016,159:132-137.
[2]Liu G R,Zheng M H,Ba T,et al.A preliminary investigation on emission of polychlorinated dibenzo-p-dioxins/dibenzofurans and dioxin-like polychlorinated biphenyls from coke plants in China[J].Chemosphere,2009,75(5):692-695.
[3]Liu G R,Zheng M H,Liu W B,et al.Atmospheric emission of PCDD/Fs,PCBs,hexachlorobenzene,and pentachlorobenzene from the coking industry[J].Environmental Science&Technology,2009,43(24):9196-9201.
[4]Liu G R,Liu W B,Cai Z W,et al.Concentrations,profiles,and emission factors of unintentionally produced persistent organic pollutants in fly ash from coking processes[J].Journal of Hazardous Materials,2013,261:421-426.
[5]孙鹏程,李晓璐,成钢,等.焦炉烟气中二英类物质排放水平研究[J].环境科学,2014,35(7):2515-2519.Sun P C,Li X L,Cheng G,et al.Preliminary investigation on emission of PCDD/Fs and DL-PCBs through flue gas from coke plants in china[J].Environmental Science,2014,35(7):2515-2519.
[6]Hsu W T,Liu M C,Hung P C,et al.PAH emissions from coal combustion and waste incineration[J].Journal of Hazardous Materials,2016,318:32-40.
[7]Mokhtar M M,Taib R M,Hassim M H.Measurement of PCDD/Fs emissions from a coal-fired power plant in Malaysia and establishment of emission factors[J].Atmospheric Pollution Research,2014,5(3):388-397.
[8]Wang H C,Hwang J F,Chi K H,et al.Formation and removal of PCDD/Fs in a municipal waste incinerator during different operating periods[J].Chemosphere,2007,67(9):S177-S184.
[9]Van Caneghem J,De Greef J,Block C,et al.NOxreduction in waste incinerators by selective catalytic reduction(SCR)instead of selective non catalytic reduction(SNCR)compared from a life cycle perspective:a case study[J].Journal of Cleaner Production,2016,112(Pt 5):4452-4460.
[10]Liu X L,Wang J,Wang X,et al.Simultaneous removal of PCDD/Fs and NOxfrom the flue gas of a municipal solid waste incinerator with a pilot plant[J].Chemosphere,2015,133:90-96.
[11]Gallastegi-Villa M,Aranzabal A,Gonzalez-Marcos J A,et al.Tailoring dual redox-acid functionalities in VOx/Ti O2/ZSM5catalyst for simultaneous abatement of PCDD/Fs and NOxfrom municipal solid waste incineration[J].Applied Catalysis B:Environmental,2017,205:310-318.
[12]Chang M B,Chi K H,Chang S H,et al.Destruction of PCDD/Fs by SCR from flue gases of municipal waste incinerator and metal smelting plant[J].Chemosphere,2007,66(6):1114-1122.
[13]Chang M B,Chi K H,Chang-Chien G P.Evaluation of PCDD/F congener distributions in MWI flue gas treated with SCRcatalysts[J].Chemosphere,2004,55(11):1457-1467.
[14]Dvorˇák R,Chlápek P,Jecha D,et al.New approach to common removal of dioxins and NOxas a contribution to environmental protection[J].Journal of Cleaner Production,2010,18(9):881-888.
[15]Ji L J,Cao X,Lu S Y,et al.Catalytic oxidation of PCDD/F on a V2O5-WO3/Ti O2catalyst:effect of chlorinated benzenes and chlorinated phenols[J].Journal of Hazardous Materials,2018,342:220-230.
[16]Gallastegi-Villa M,Aranzabal A,Gonzalez-Marcos J A,et al.Metal-loaded ZSM5 zeolites for catalytic purification of dioxin/furans and NOxcontaining exhaust gases from MWI plants:effect of different metal cations[J].Applied Catalysis B:Environmental,2016,184:238-245.
[17]Yu M F,Li W W,Li X D,et al.Development of new transition metal oxide catalysts for the destruction of PCDD/Fs[J].Chemosphere,2016,156:383-391.
[18]Busca G,Baldi M,Pistarino C,et al.Evaluation of V2O5-WO3-Ti O2and alternative SCR catalysts in the abatement of VOCs[J].Catalysis Today,1999,53(4):525-533.
[19]Liljelind P,Unsworth J,Maaskant O,et al.Removal of dioxins and related aromatic hydrocarbons from flue gas streams by adsorption and catalytic destruction[J].Chemosphere,2001,42(5-7):615-623.
[20]Goemans M,Clarysse P,Joannès J,et al.Catalytic NOx reduction with simultaneous dioxin and furan oxidation[J].Chemosphere,2003,50(4):489-497.
[21]HJ 77.2-2008,环境空气和废气二英类的测定同位素稀释高分辨气相色谱-高分辨质谱法[S].HJ 77.2-2008,Ambient air and waste gas Determination of polychlorinated dibenzo-p-dioxins(PCDDs)and polychlorinated dibenzofurans(PCDFs)Isotope dilution HRGC-HRMS[S].
[22]GB 18485-2014,生活垃圾焚烧污染控制标准[S].GB 18485-2014,Standard for pollution control on the municipal solid waste incineration[S].
[23]Jones J,Ross J R H.The development of supported vanadia catalysts for the combined catalytic removal of the oxides of nitrogen and of chlorinated hydrocarbons from flue gases[J].Catalysis Today,1997,35(1-2):97-105.
[24]Debecker D P,Delaigle R,Hung P C,et al.Evaluation of PCDD/F oxidation catalysts:confronting studies on model molecules with tests on PCDD/F-containing gas stream[J].Chemosphere,2011,82(9):1337-1342.
[25]Wang Q L,Hung P C,Lu S Y,et al.Catalytic decomposition of gaseous PCDD/Fs over V2O5/Ti O2-CNTs catalyst:effect of NOand NH3addition[J].Chemosphere,2016,159:132-137.
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