燃煤电站多污染物一体化脱除研究进展
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摘要
燃煤电站排放的SO_2、NO和Hg等污染物对生态环境造成严重破坏,严格控制燃煤电站的污染物排放意义重大。由于目前燃煤电站采用的污染物单独脱除技术存在占地面积大、运行费用高等问题,经济高效的多污染物一体化脱除技术成为污染物控制领域的研究热点。本研究对燃煤电站多污染物一体化脱除技术进行概述,对吸附剂法、气相氧化法、湿法氧化和气固催化氧化法的技术原理、研究现状、技术优缺点及今后的发展方向进行了分析总结。
SO_2,NO and Hg pollutants released from coal-fired power plants have seriously damaged to ecological environment,so it is of great significance to strictly control the pollutants from coal-fired power plants. The separate removal technology of pollutants in coal-fired power plants has many shortcomings,such as large floor area and high operating costs. Therefore,the economic and efficient simultaneous removal technology of multiple pollutants has become a hot research topic. This review summarized the simultaneous removal technology of multi-pollutants. The technical principle,research status,technical advantages and disadvantages and development potential of adsorbent method,gas-phase oxidation,wet air oxidation and gas-solid catalytic oxidation method were summarized and analyzed. Furthermore,the key technology and development directions of these methods were pointed out.
SO_2,NO and Hg pollutants released from coal-fired power plants have seriously damaged to ecological environment,so it is of great significance to strictly control the pollutants from coal-fired power plants. The separate removal technology of pollutants in coal-fired power plants has many shortcomings,such as large floor area and high operating costs. Therefore,the economic and efficient simultaneous removal technology of multiple pollutants has become a hot research topic. This review summarized the simultaneous removal technology of multi-pollutants. The technical principle,research status,technical advantages and disadvantages and development potential of adsorbent method,gas-phase oxidation,wet air oxidation and gas-solid catalytic oxidation method were summarized and analyzed. Furthermore,the key technology and development directions of these methods were pointed out.
引文
[1] 惠霂霖,张磊,王祖光,等. 中国燃煤电厂汞的物质流向与汞排放研究[J]. 中国环境科学,2015(8):2241-2250.HUI Mu-lin,ZHANG Lei,WANG Zu-guang,et al. The mercury mass flow and emissions of coal-fired power plants in China[J].China Environmental Science,2015(8):2241-2250.
[2] 《中国电力年鉴》委员会. 中国电力年鉴[M].北京:中国电力出版社2016.China electric power yearbook[M].Beijing:China Electric Power Press,2016.
[3] ZHENG C,XU C,ZHANG Y,et al. Nitrogen oxide absorption and nitrite/nitrate formation in limestone slurry for WFGD system[J]. Applied Energy,2014(129):187-194.
[4] CHI G,SHEN B,YU R,et al. Simultaneous removal of NO and Hg0 over Ce-Cu modified V2O5/TiO2 based commercial SCR catalysts[J]. Journal of hazardous materials,2017,330:83-92.
[5] TONG L,YUE T,ZUO P,et al. Effect of characteristics of KI-impregnated activated carbon and flue gas components on Hg0 removal[J]. Fuel,2017,197:1-7.
[6] LIU Y,ZHOU J,ZHANG Y,et al. Removal of Hg0 and simultaneous removal of Hg0/SO2/NO in flue gas using two Fenton-like reagents in a spray reactor[J]. Fuel,2015,145:180-188.
[7] MA Z,WU X,FENG Y,et al. Low-temperature SCR activity and SO2 deactivation mechanism of Ce-modified V2O5-WO3/TiO2 catalyst[J].Progress in Natural Science: Materials International,2015,25(4):342-352.
[8] 常林,杨建平,余学海,等.WFGD系统中 pH对Hg2+还原释放机理的实验研究[J]. 工程热物理学报,2017,38(4):885-889.CHANG Lin,YANG Jian-ping,YU Xue-hai,et al.The experimental study on the effect of pH value on Hg2+ reduction mechanism in the wet flue gas desulphurization system[J]. Journal of Engineering Thermophysics,2017,38(4):885-889.
[9] DEHGHAN R,ANBIA M. Zeolites for adsorptive desulfurization from fuels: review[J]. Fuel Processing Technology,2017,167:99-116.
[10] CHEN W,MA Y,YAN N,et al. The co-benefit of elemental mercury oxidation and slip ammonia abatement with SCR-Plus catalysts[J]. Fuel,2014,133:263-269.
[11] MACHADO B F,SERP P. Graphene-based materials for catalysis[J]. Catal Sci Technol,2012,2(1):54-75.
[12] TSUJI K,SHIRAISHI I. Combined desulfurization,denitrification and reduction of air toxics using activated coke: 2. Process applications and performance of activated coke[J]. Fuel,1997,76(6):555-560.
[13] TANG Qiang,ZHANG Zhi-gang,ZHU Wen-pei,et al.SO2 and NO selective adsorption properties of coal-based activated carbons[J]. Fuel,2005,84(4):461-465.
[14] LIU Z S. Adsorption of SO2 and NO from incineration flue gas onto activated carbon fibers[J]. Waste Management,2008,28(11):2329-2335.
[15] FANG C,ZHANG D,SHI L,et al. Highly dispersed CeO2 on carbon nanotubes for selective catalytic reduction of NO with NH3[J]. Catal Sci Technol,2013,3(3):803-811.
[16] ZHU Chun,DUAN Yu-feng,WU Chang-yu,et al.Mercury removal and synergistic capture of SO2/NO by ammonium halides modified rice husk char[J]. Fuel,2016,172:160-169.
[17] 高洪亮,周劲松,骆仲泱,等. 改性活性炭对模拟燃煤烟气中汞吸附的实验研究[J]. 中国电机工程学报,2007(8):26-30.GAO Hong-liang,ZHOU Jin-song,LUO Zhong-yang,et al. Experimental study on Hg vapor adsorption of modified activated carbons in simulated flue gas[J].Proceedings of Electric Machine Engineering,2007(8):26-30.
[18] LIU J,CHENEY M A,WU F,et al. Effects of chemical functional groups on elemental mercury adsorption on carbonaceous surfaces[J].Journal of Hazardous Materials,2011,186(1):108-113.
[19] XU H,QU Z,ZONG C,et al. MnOx/Graphene for the catalytic oxidation and adsorption of elemental mercury[J]. Environmental Science & Technology,2015,49(11):6823-6830.
[20] 严金英,郑重,于国峰,等. 燃煤烟气多污染物一体化控制技术研究进展[J]. 热力发电,2011(11):9-13.YAN Jin-ying,ZHENG Zhong,YU Guo-feng,et al. Progress in study on multi-pullutant control technology for coal-fired flue gas[J].Thermal Power Generation,2011(11):9-13.
[21] PAVLISH J H,SONDREAL E A,MANN M D,et al. Status review of mercury control options for coal-fired power plants[J]. Fuel Processing Technology,2003,82(2):89-165.
[22] WANG Z,ZHOU J,ZHU Y,et al. Simultaneous removal of NOx,SO2 and Hg in nitrogen flow in a narrow reactor by ozone injection: Experimental results[J]. Fuel Processing Technology,2007,88(8):817-823.
[23] DING J,ZHONG Q,ZHANG S. Simultaneous desulfurization and denitrification of flue gas by catalytic ozonation over Ce-Ti catalyst[J]. Fuel Processing Technology,2014,128:449-455.
[24] G?OMBA M,KORDYLEWSKI W. Simultaneous removal of NOx,SO2,CO and Hg from flue gas by ozonation. Pilot plant studies[J]. Environment Protection Engineering,2014,40(3):113-125.
[25] TSENG C-H,KEENER T C,LEE J-Y,et al.Enhanced effect of in-situ generated ammonium salts aerosols on the removal of NOx from simulated flue gas[J].Environmental Science & Technology,2001,35(15):3219-3224.
[26] VAN VELDHUIZEN E M,ZHOU L M,RUTGERS W R.Combined effects of pulsed discharge removal of NO,SO2,and NH3 from flue gas[J].Plasma Chemistry and Plasma Processing,1998,18(1):91-111.
[27] 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.
[28] NIU Q,LUO J,SUN S,et al. Effects of flue gas components on the oxidation of gaseous Hg0 by dielectric barrier discharge plasma[J]. Fuel,2015,150:619-624.
[29] 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,2013,34(1):217-228.
[30] NIST,http://kinetics.nist.gov/kinetics/index.jsp.
[31] BAI M,ZHANG Z,BAI M. Simultaneous desulfurization and denitrification of flue gas by .OH radicals produced from O2+ and water vapor in a duct[J]. Environmental Science & Technology,2012,46(18):10161-10168.
[32] LUO J,NIU Q,XIA Y,et al. Investigation of gaseous elemental mercury oxidation by non-thermal plasma injection method[J]. Energy & Fuels,2017,31(10): 11013-11018.
[33] XU F,LUO Z,CAO W,et al. Simultaneous oxidation of NO,SO2 and Hg0 from flue gas by pulsed corona discharge[J].Journal of Environmental Sciences,2009,21(3):328-332.
[34] MA S,ZHAO Y,YANG J,et al. Research progress of pollutants removal from coal-fired flue gas using non-thermal plasma[J]. Renewable and Sustainable Energy Reviews,2017,67:791-810.
[35] 康新园. 燃煤烟气脱硫脱硝一体化技术研究进展[J].洁净煤技术,2014(6):115-118.KANG Xin-yuan. Research progress of coal-fired flue gas simultaneous desulfurization and denitrification[J].Clean Coal Technology,2014(6):115-118.
[36] 赵毅,韩静,马天忠. 活性炭纤维负载TiO2同时脱硫脱硝实验研究[J]. 中国电机工程学报,2009(11):44-49.ZHAO Yi,HAN Jing,MA Tian-zhong.Experimental study on simultaneous desulfurization and denitrification by supporting TiO2 on activated carbon fiber[J]. Proceedings of Electric Machine Engineering,2009(11):44-49.
[37] YUAN Y,ZHANG J,LI H,et al. Simultaneous removal of SO2,NO and mercury using TiO2-aluminum silicate fiber by photocatalysis[J]. Chemical Engineering Journal,2012,192:21-28.
[38] SU C,RAN X,HU J,et al. Photocatalytic process of simultaneous desulfurization and denitrification of flue gas by TiO2-polyacrylonitrile nanofibers[J]. Environmental Science & Technology,2013,47(20):11562-11568.
[39] ZHAO Y,HAN Y,GUO T,et al. Simultaneous removal of SO2,NO and Hg0 from flue gas by ferrate (VI) solution[J]. Energy,2014,67:652-658.
[40] ZHAO Y,HAO R,YUAN B,et al. Simultaneous removal of SO2,NO and Hg0 through an integrative process utilizing a cost-effective complex oxidant[J].Journal of Hazardous Materials,2016,301:74-83.
[41] HAO R,YANG S,ZHAO Y,et al. Follow-up research of ultraviolet catalyzing vaporized H2O2 for simultaneous removal of SO2 and NO: absorption of NO2 and NO by Na-based WFGD byproduct (Na2SO3)[J]. Fuel Processing Technology,2017,160:64-69.
[42] LI H,WANG S,WANG X,et al. Catalytic oxidation of Hg0 in flue gas over Ce modified TiO2 supported Co-Mn catalysts: Characterization,the effect of gas composition and co-benefit of NO conversion[J]. Fuel,2017,202:470-482.
[43] LI H,WANG S,WANG X,et al. Activity of CuCl2-modified cobalt catalyst supported on Ti-Ce composite for simultaneous catalytic oxidation of Hg0 and NO in a simulated pre-sco process[J]. Chemical Engineering Journal,2017,316:1103-1113.
[44] LI L,SHEN Q,CHENG J,et al. Catalytic oxidation of NO over TiO2 supported platinum clusters I. Preparation,characterization and catalytic properties[J]. Applied Catalysis B:Environmental,2010,93(3/4):259-266.
[45] CR.Mercury removal in an on-thermal plasma-based multi-pollutant control technology for utility boilers[R].FC26-01NT41182,Powerspan CorporationUS2004 Contract.
[2] 《中国电力年鉴》委员会. 中国电力年鉴[M].北京:中国电力出版社2016.China electric power yearbook[M].Beijing:China Electric Power Press,2016.
[3] ZHENG C,XU C,ZHANG Y,et al. Nitrogen oxide absorption and nitrite/nitrate formation in limestone slurry for WFGD system[J]. Applied Energy,2014(129):187-194.
[4] CHI G,SHEN B,YU R,et al. Simultaneous removal of NO and Hg0 over Ce-Cu modified V2O5/TiO2 based commercial SCR catalysts[J]. Journal of hazardous materials,2017,330:83-92.
[5] TONG L,YUE T,ZUO P,et al. Effect of characteristics of KI-impregnated activated carbon and flue gas components on Hg0 removal[J]. Fuel,2017,197:1-7.
[6] LIU Y,ZHOU J,ZHANG Y,et al. Removal of Hg0 and simultaneous removal of Hg0/SO2/NO in flue gas using two Fenton-like reagents in a spray reactor[J]. Fuel,2015,145:180-188.
[7] MA Z,WU X,FENG Y,et al. Low-temperature SCR activity and SO2 deactivation mechanism of Ce-modified V2O5-WO3/TiO2 catalyst[J].Progress in Natural Science: Materials International,2015,25(4):342-352.
[8] 常林,杨建平,余学海,等.WFGD系统中 pH对Hg2+还原释放机理的实验研究[J]. 工程热物理学报,2017,38(4):885-889.CHANG Lin,YANG Jian-ping,YU Xue-hai,et al.The experimental study on the effect of pH value on Hg2+ reduction mechanism in the wet flue gas desulphurization system[J]. Journal of Engineering Thermophysics,2017,38(4):885-889.
[9] DEHGHAN R,ANBIA M. Zeolites for adsorptive desulfurization from fuels: review[J]. Fuel Processing Technology,2017,167:99-116.
[10] CHEN W,MA Y,YAN N,et al. The co-benefit of elemental mercury oxidation and slip ammonia abatement with SCR-Plus catalysts[J]. Fuel,2014,133:263-269.
[11] MACHADO B F,SERP P. Graphene-based materials for catalysis[J]. Catal Sci Technol,2012,2(1):54-75.
[12] TSUJI K,SHIRAISHI I. Combined desulfurization,denitrification and reduction of air toxics using activated coke: 2. Process applications and performance of activated coke[J]. Fuel,1997,76(6):555-560.
[13] TANG Qiang,ZHANG Zhi-gang,ZHU Wen-pei,et al.SO2 and NO selective adsorption properties of coal-based activated carbons[J]. Fuel,2005,84(4):461-465.
[14] LIU Z S. Adsorption of SO2 and NO from incineration flue gas onto activated carbon fibers[J]. Waste Management,2008,28(11):2329-2335.
[15] FANG C,ZHANG D,SHI L,et al. Highly dispersed CeO2 on carbon nanotubes for selective catalytic reduction of NO with NH3[J]. Catal Sci Technol,2013,3(3):803-811.
[16] ZHU Chun,DUAN Yu-feng,WU Chang-yu,et al.Mercury removal and synergistic capture of SO2/NO by ammonium halides modified rice husk char[J]. Fuel,2016,172:160-169.
[17] 高洪亮,周劲松,骆仲泱,等. 改性活性炭对模拟燃煤烟气中汞吸附的实验研究[J]. 中国电机工程学报,2007(8):26-30.GAO Hong-liang,ZHOU Jin-song,LUO Zhong-yang,et al. Experimental study on Hg vapor adsorption of modified activated carbons in simulated flue gas[J].Proceedings of Electric Machine Engineering,2007(8):26-30.
[18] LIU J,CHENEY M A,WU F,et al. Effects of chemical functional groups on elemental mercury adsorption on carbonaceous surfaces[J].Journal of Hazardous Materials,2011,186(1):108-113.
[19] XU H,QU Z,ZONG C,et al. MnOx/Graphene for the catalytic oxidation and adsorption of elemental mercury[J]. Environmental Science & Technology,2015,49(11):6823-6830.
[20] 严金英,郑重,于国峰,等. 燃煤烟气多污染物一体化控制技术研究进展[J]. 热力发电,2011(11):9-13.YAN Jin-ying,ZHENG Zhong,YU Guo-feng,et al. Progress in study on multi-pullutant control technology for coal-fired flue gas[J].Thermal Power Generation,2011(11):9-13.
[21] PAVLISH J H,SONDREAL E A,MANN M D,et al. Status review of mercury control options for coal-fired power plants[J]. Fuel Processing Technology,2003,82(2):89-165.
[22] WANG Z,ZHOU J,ZHU Y,et al. Simultaneous removal of NOx,SO2 and Hg in nitrogen flow in a narrow reactor by ozone injection: Experimental results[J]. Fuel Processing Technology,2007,88(8):817-823.
[23] DING J,ZHONG Q,ZHANG S. Simultaneous desulfurization and denitrification of flue gas by catalytic ozonation over Ce-Ti catalyst[J]. Fuel Processing Technology,2014,128:449-455.
[24] G?OMBA M,KORDYLEWSKI W. Simultaneous removal of NOx,SO2,CO and Hg from flue gas by ozonation. Pilot plant studies[J]. Environment Protection Engineering,2014,40(3):113-125.
[25] TSENG C-H,KEENER T C,LEE J-Y,et al.Enhanced effect of in-situ generated ammonium salts aerosols on the removal of NOx from simulated flue gas[J].Environmental Science & Technology,2001,35(15):3219-3224.
[26] VAN VELDHUIZEN E M,ZHOU L M,RUTGERS W R.Combined effects of pulsed discharge removal of NO,SO2,and NH3 from flue gas[J].Plasma Chemistry and Plasma Processing,1998,18(1):91-111.
[27] 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.
[28] NIU Q,LUO J,SUN S,et al. Effects of flue gas components on the oxidation of gaseous Hg0 by dielectric barrier discharge plasma[J]. Fuel,2015,150:619-624.
[29] 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,2013,34(1):217-228.
[30] NIST,http://kinetics.nist.gov/kinetics/index.jsp.
[31] BAI M,ZHANG Z,BAI M. Simultaneous desulfurization and denitrification of flue gas by .OH radicals produced from O2+ and water vapor in a duct[J]. Environmental Science & Technology,2012,46(18):10161-10168.
[32] LUO J,NIU Q,XIA Y,et al. Investigation of gaseous elemental mercury oxidation by non-thermal plasma injection method[J]. Energy & Fuels,2017,31(10): 11013-11018.
[33] XU F,LUO Z,CAO W,et al. Simultaneous oxidation of NO,SO2 and Hg0 from flue gas by pulsed corona discharge[J].Journal of Environmental Sciences,2009,21(3):328-332.
[34] MA S,ZHAO Y,YANG J,et al. Research progress of pollutants removal from coal-fired flue gas using non-thermal plasma[J]. Renewable and Sustainable Energy Reviews,2017,67:791-810.
[35] 康新园. 燃煤烟气脱硫脱硝一体化技术研究进展[J].洁净煤技术,2014(6):115-118.KANG Xin-yuan. Research progress of coal-fired flue gas simultaneous desulfurization and denitrification[J].Clean Coal Technology,2014(6):115-118.
[36] 赵毅,韩静,马天忠. 活性炭纤维负载TiO2同时脱硫脱硝实验研究[J]. 中国电机工程学报,2009(11):44-49.ZHAO Yi,HAN Jing,MA Tian-zhong.Experimental study on simultaneous desulfurization and denitrification by supporting TiO2 on activated carbon fiber[J]. Proceedings of Electric Machine Engineering,2009(11):44-49.
[37] YUAN Y,ZHANG J,LI H,et al. Simultaneous removal of SO2,NO and mercury using TiO2-aluminum silicate fiber by photocatalysis[J]. Chemical Engineering Journal,2012,192:21-28.
[38] SU C,RAN X,HU J,et al. Photocatalytic process of simultaneous desulfurization and denitrification of flue gas by TiO2-polyacrylonitrile nanofibers[J]. Environmental Science & Technology,2013,47(20):11562-11568.
[39] ZHAO Y,HAN Y,GUO T,et al. Simultaneous removal of SO2,NO and Hg0 from flue gas by ferrate (VI) solution[J]. Energy,2014,67:652-658.
[40] ZHAO Y,HAO R,YUAN B,et al. Simultaneous removal of SO2,NO and Hg0 through an integrative process utilizing a cost-effective complex oxidant[J].Journal of Hazardous Materials,2016,301:74-83.
[41] HAO R,YANG S,ZHAO Y,et al. Follow-up research of ultraviolet catalyzing vaporized H2O2 for simultaneous removal of SO2 and NO: absorption of NO2 and NO by Na-based WFGD byproduct (Na2SO3)[J]. Fuel Processing Technology,2017,160:64-69.
[42] LI H,WANG S,WANG X,et al. Catalytic oxidation of Hg0 in flue gas over Ce modified TiO2 supported Co-Mn catalysts: Characterization,the effect of gas composition and co-benefit of NO conversion[J]. Fuel,2017,202:470-482.
[43] LI H,WANG S,WANG X,et al. Activity of CuCl2-modified cobalt catalyst supported on Ti-Ce composite for simultaneous catalytic oxidation of Hg0 and NO in a simulated pre-sco process[J]. Chemical Engineering Journal,2017,316:1103-1113.
[44] LI L,SHEN Q,CHENG J,et al. Catalytic oxidation of NO over TiO2 supported platinum clusters I. Preparation,characterization and catalytic properties[J]. Applied Catalysis B:Environmental,2010,93(3/4):259-266.
[45] CR.Mercury removal in an on-thermal plasma-based multi-pollutant control technology for utility boilers[R].FC26-01NT41182,Powerspan CorporationUS2004 Contract.