低温SCR脱硝催化剂研究进展（英文）
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摘要
氮氧化物NOx(NO, NO_2和N_2O)是全球大气污染的主要污染物之一,引起光化学烟雾、酸雨、臭氧层破坏等环境问题,严重影响人们的生存环境和生活质量,引起了世界各国的广泛关注。针对固定源和移动源燃烧排放,各国制定了日益严格的排放标准。目前主要的脱硝技术分为选择性催化还原(SCR)、选择性非催化还原(SNCR)、氧化脱硝和活性炭吸附脱硝等。SNCR的应用有较高的条件,影响其成功运行的主要因素有温度、氨氮比、氨气在烟气中的分布和停留时间等,故SNCR的工业应用存在一定的局限性。SCR脱硝技术比其它脱硝技术应用更广泛,其中脱硝多安排于除尘脱硫后,此时温度多处于100～250℃之间。为提高SCR脱硝性能,低温SCR脱除NOx是目前研究最热门的烟气脱硝技术。本工作综述了近年来低温SCR脱硝催化剂的研究进展,介绍了锰基催化剂、钒基催化剂及碳基催化剂的发展现状,对单组分Mn基催化剂、负载型Mn基催化剂和复合型Mn基催化剂进行了综述,从V基催化剂的制备对脱销的影响和脱硝机理进行了表述,综述了过渡金属掺杂对C基催化剂的影响,阐述了烟气中H2O和SO2对催化反应的影响及低温SCR反应的脱硝机理,对低温SCR催化剂进行了总结并对其未来发展进行了展望。
Nitrogen oxide NOx(NO, NO_2, and N_2O) is one of the major pollutants in the air pollution, it can cause environmental problems such as photochemical smog, acid rain, and ozone layer destruction, which has posed threat to people's living environment and quality of life, and attracted great attention from the world. Countries made stricter emission standards for burning emissions from both fixed and mobile sources. The major denitrification technologies include selective catalytic reduction(SCR), selective non-catalytic reduction(SNCR), oxidative denitrification, and activated carbon adsorption and denitrification at present. The SNCR has higher conditions in industrial applications, the main factors affecting successful operation are temperature, ammonia-nitrogen ratio, distribution of ammonia gas in the flue gas and residence time, so there were certain limitations in industrial application of SNCR. Compared with other denitrification technologies, SCR denitration technology is more widely used in industrial application, in which denitration is mostly arranged after dust removal and desulfurization, at this time, the temperature is mostly between 100~250 ℃. The performance of SCR denitrification in low-temperature must be improved, which is one of the most promising flue gas DeNOx technology. In this paper, the recent works on low-temperature SCR catalysts were reviewed on manganese-based catalysts, vanadium-based catalysts and carbon-based catalysts. Single-component Mn-based catalysts, supported Mn-based catalysts and composite Mn-based catalysts were reviewed, the effects of preparation of V-based catalysts on the de-dumping and denitrification mechanisms were described. The effect of transition metal doping on C-based catalysts was reviewed. The influence of H_2O and SO_2 resistance on low-temperature NH_3-SCR catalytic activity and reaction mechanism were also discussed. Finally, the virtues advantages and defects of low temperature SCR catalysts were summarized, and the future development direction was also given out.
Nitrogen oxide NOx(NO, NO_2, and N_2O) is one of the major pollutants in the air pollution, it can cause environmental problems such as photochemical smog, acid rain, and ozone layer destruction, which has posed threat to people's living environment and quality of life, and attracted great attention from the world. Countries made stricter emission standards for burning emissions from both fixed and mobile sources. The major denitrification technologies include selective catalytic reduction(SCR), selective non-catalytic reduction(SNCR), oxidative denitrification, and activated carbon adsorption and denitrification at present. The SNCR has higher conditions in industrial applications, the main factors affecting successful operation are temperature, ammonia-nitrogen ratio, distribution of ammonia gas in the flue gas and residence time, so there were certain limitations in industrial application of SNCR. Compared with other denitrification technologies, SCR denitration technology is more widely used in industrial application, in which denitration is mostly arranged after dust removal and desulfurization, at this time, the temperature is mostly between 100~250 ℃. The performance of SCR denitrification in low-temperature must be improved, which is one of the most promising flue gas DeNOx technology. In this paper, the recent works on low-temperature SCR catalysts were reviewed on manganese-based catalysts, vanadium-based catalysts and carbon-based catalysts. Single-component Mn-based catalysts, supported Mn-based catalysts and composite Mn-based catalysts were reviewed, the effects of preparation of V-based catalysts on the de-dumping and denitrification mechanisms were described. The effect of transition metal doping on C-based catalysts was reviewed. The influence of H_2O and SO_2 resistance on low-temperature NH_3-SCR catalytic activity and reaction mechanism were also discussed. Finally, the virtues advantages and defects of low temperature SCR catalysts were summarized, and the future development direction was also given out.
引文
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[24]Cha W,Chin S M,Park E,et al.Effect of V2O5 loading of V2O5/TiO2 catalysts prepared via CVC and impregnation methods on NOx removal[J].Applied Catalysis B:Environmental,2013,140:708-715.
[25]Boningari T,Koirala R,Smirniotis P G.Low-temperature catalytic reduction of NO by NH3 over vanadia-based nanoparticles prepared by flame-assisted spray pyrolysis:Influence of various supports[J].Applied Catalysis B:Environmental,2013,140:289-298.
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[28]Chen M Y,Zhao M M,Tang F S,et al.Effect of Ce doping into V2O5-WO3/TiO2 catalysts on the selective catalytic reduction of NOx by NH3[J].Journal of Rare Earths,2017,35:1206-1215.
[29]Liu Z M,Li Y,Zhu T L,et al.Selective catalytic reduction of NOx by NH3 over Mn-promoted V2O5/TiO2 catalyst[J].Industrial and Engineering Chemistry Research,2014,53(33):12964-12970.
[30]Chen L,Li J H,Ge M F.The poisoning effect of alkali metals doping over nano V2O5-WO3/TiO2 catalysts on selective catalytic reduction of NOx by NH3[J].Chemical Engineering Journal,2011,170:531-537.
[31]Busca G,Lietti L,Ramis G,et al.Chemical and mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts:a review[J].Applied Catalysis B:Environmental,1998,18(1/2):1-36.
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[33]Vargas M A L,Casanova M,Trovarelli A,et al.An IR study of thermally stable V2O5-WO3-TiO2 SCR catalysts modified with silica and rare-earths(Ce,Tb,Er)[J].Applied Catalysis B:Environmental,2007,75(3/4):303-311.
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[35]Li Q,Yang H S,Qiu F M,et al.Promotional effects of carbon nanotubes on V2O5/TiO2 for NOx removal[J].Journal of Hazardous Materials,2011,192(2):915-921.
[36]Fan X Y,Qiu F M,Yang H S,et al.Selective catalytic reduction of NOx with ammonia over Mn-Ce-Ox/TiO2-carbon nanotube composites[J].Catalysis Communications,2011,12:1298-1301.
[37]Zhang L,Zhang D S,Zhang J P,et al.Design of meso-TiO2@MnOx-CeOx/CNTs with a core-shell structure as De NOx catalysts:promotion of activity,stability and SO2-tolerance[J].Nanoscale,2013,20:9821-9829.
[38]Zhang Y B,Zheng Y Y,Wang X,et al.Preparation of Mn-FeOx/CNTs catalysts by redox co-precipitation and application in low-temperature no reduction with NH3[J].Catalysis Communications,2015,62:57-61.
[39]Huang B C,Huang R,Jin D J,et al.Low temperature SCR of NOwith NH3 over carbon nanotubes supported vanadium oxides[J].Catalysis Today,2007,126(3/4):279-283.
[40]Huang Z G,Zhu Z P,Liu Z Y.Combined effect of H2O and SO2 on V2O5/AC catalysts for NO reduction with ammonia at lower temperatures[J].Applied Catalysis B:Environmental,2002,39(4):361-368.
[41]Huang Z G,Zhu Z P,Liu Z Y.Formation and reaction of ammonium sulfate salts on V2O5/AC catalyst during selective catalytic reduction of nitric oxide by ammonia at low temperatures[J].Journal of Catalysis,2003,214(2):213-219.
[42]Huang Z G,Liu Z Y,Zhang X L,et al.Inhibition effect of H2O on V2O5/AC catalyst for catalytic reduction of NO with NH3 at low temperature[J].Applied Catalysis B:Environmental,2006,63(3/4):260-265.
[43]Wu Z B,Jin R B,Wang H Q,et al.Effect of ceria doping on SO2resistance of Mn/TiO2 for selective catalytic reduction of NO with NH3 at low temperature[J].Catalysis Communications,2009,10(6):935-939.
[44]Sun D K,Liu Q Y,Liu Z Y,et al.An in situ drifts study on SCR of NO with NH3 over V2O5/AC surface[J].Catalysis Letters,2009,132(1/2):122-126.
[45]Jiang B Q,Deng B Y,Zhang Z Q,et al.Effect of Zr addition on the low-temperature SCR activity and SO2 tolerance of Fe-Mn/Ti catalysts[J].Journal of Physical Chemistry C,2014,118(27):14866-14875.
[46]Zhu Z P,Liu Z Y,Niu H X,et al.Promoting effect of SO2 on activated carbon-supported vanadia catalyst for NO reduction by NH3 at low temperatures[J].Journal of Catalysis,1999,187(1):245-248.
[47]Gálvez M E,Boyano A,Lázaro M J,et al.A study of the mechanisms of NO reduction over vanadium loaded activated carbon catalysts[J].Chemical Engineering Journal,2008,144(1):10-20.
[48]Ettireddy P R,Ettireddy N,Boningari T,et al.Investigation of the selective catalytic reduction of nitric oxide with ammonia over Mn/TiO2 catalysts through transient isotopic labeling and in situ FT-IR studies[J].Journal of Catalysis,2012,292:53-63.
[49]Yang S J,Wang C Z,Li J H,et al.Low temperature selective catalytic reduction of NO with NH3 over Mn-Fe spinel:performance,mechanism and kinetic study[J].Applied Catalysis B:Environmental,2011,110:71-80.
[50]Wang Y L,Ge C Z,Zhan L,et al.MnOx-CeO2/activated carbon honeycomb catalyst for selective catalytic reduction of NO with NH3at low temperatures[J].Industrial and Engineering Chemistry Research,2012,51(36):11667-11673.
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[52]Tronconi E,Nova I,Ciardelli C,et al.Redox features in the catalytic mechanism of the―standard‖and―fast‖NH3-SCR of NOx over a V-based catalyst investigated by dynamic methods[J].Journal of Catalysis,2007,245(1):1-10.
[53]Wang J P,Yan Z,Liu L L,et al.In situ drifts investigation on the SCR of NO with NH3 over V2O5 catalyst supported by activated semi-coke[J].Applied Surface Science,2014,313:660-669.
[2]Qiu Y,Liu B,Du J,et al.The monolithic cordierite supported V2O5-MoO3/TiO2 catalyst for NH3-SCR[J].Chemical Engineering Journal,2016,294:264-272.
[3]Li J H,Chang H Z,Ma L,et al.Low-temperature selective catalytic reduction of NOx with NH3 over metal oxide and zeolite catalysts-a review[J].Catalysis Today,2011,175(1):147-156.
[4]Fang N J,Guo J X,Shu S,et al.Enhancement of low-temperature activity and sulfur resistance of Fe0.3Mn0.5Zr0.2 catalyst for NOremoval by NH3-SCR[J].Chemical Engineering Journal,2017,325:114-123.
[5]Xia Q,Qin Z.Investigation of selective catalytic reduction of NOx with V2O5/TiO2 as catalysts[J].Journal of Safety and Environmental,2004,4:16-18.
[6]Tian W,Yang H S,Fan X Y,et al.Catalytic reduction of NOx with NH3 over different-shaped MnO2 at low temperature[J].Journal of Hazardous Materials,2011,188(1/3):105-109.
[7]Tang X L,Hao J M,Xu W G,et al.Low temperature selective catalytic reduction of NOx with NH3 over amorphous MnOx catalysts prepared by three methods[J].Catalysis Communications,2007,8(3):329-334.
[8]Wu Z B,Jin R B,Liu Y,et al.Ceria modified MnOx/TiO2 as a superior catalyst for NO reduction with NH3 at low-temperature[J].Catalysis Communications,2008,9(13):2217-2220.
[9]Thirupathi B,Smirniotis P.Effect of nickel as dopant in Mn/TiO2catalysts for the low-temperature selective reduction of NO with NH3[J].Catalysis Letters,2011,141(10):1399-1404.
[10]Thirupathi B,Smirniotis P.Nickel-doped Mn/TiO2 as an efficient catalyst for the low-temperature SCR of NO with NH3:catalytic evaluation and characterizations[J].Journal of Catalysis,2012,288:74-83.
[11]Shen B X,Liu T,Zhao N,et al.Iron-doped Mn-Ce/TiO2 catalyst for low temperature selective catalytic reduction of NO with NH3[J].Journal of Environmental Sciences,2010,22(9):1447-1454.
[12]Luo S P,Zhou W T,Xie A J,et al.Effect of MnO2 polymorphs structure on the selective catalytic reduction of NOx with NH3 over TiO2-palygorskite[J].Chemical Engineering Journal,2016,286:291-299.
[13]Huang J H,Tong Z Q,Huang Y,et al.Selective catalytic reduction of NO with NH3 at low temperatures over iron and manganese oxides supported on mesoporous silica[J].Applied Catalysis B:Environmental,2008,78(3/4):309-314.
[14]Guo J,Li C T,Pei L U,et al.Research on SCR denitrification of MnOx/Al2O3 modified by CeO2 and its mechanism at low temperature[J].Chinese Journal of Environmental Science,2011,32(8):2240-2246.
[15]Li Y,Li Y P,Wang P F,et al.Low-temperature selective catalytic reduction of NOx with NH3 over MnFeOx nanorods[J].Chemical Engineering Journal,2017,330:213-222.
[16]Zhang Y P,Zhao X Y,Xu H T,et al.Novel ultrasonic-modified MnOx/TiO2 for low-temperature selective catalytic reduction(SCR)of NO with ammonia[J].Journal of Colloid and Interface Science,2011,361(1):212-218.
[17]Lian Z H,Liu F D,He H,et al.Manganese-niobium mixed oxide catalyst for the selective catalytic reduction of NOx with NH3 at low temperatures[J].Chemical Engineering Journal,2014,250:390-398.
[18]Zuo J L,Chen Z H,Wang F R,et al.Low-temperature selective catalytic reduction of NOx with NH3 over novel Mn-Zr mixed oxide catalysts[J].Industrial and Engineering Chemistry Research,2014,53(7):2647-2655.
[19]Liu Z M,Liu Y X,Li Y,et al.WO3 promoted Mn-Zr mixed oxide catalyst for the selective catalytic reduction of NOx with NH3[J].Chemical Engineering Journal,2016,283:1044-1050.
[20]Lin L Y,Lee C Y,Zhang Y R,et al.Aerosol-assisted deposition of Mn-Fe oxide catalyst on TiO2 for superior selective catalytic reduction of NO with NH3 at low temperatures[J].Catalysis Communications,2018,111:36-41.
[21]Wan Y P,Zhao W R,Tang Y,et al.Ni-Mn bi-metal oxide catalysts for the low temperature SCR removal of NO with NH3[J].Applied Catalysis B:Environmental,2014,148:114-122.
[22]Wu Z B,Jiang B Q,Liu Y.Effect of transition metals addition on the catalyst of manganese/titania for low temperature selective catalytic reduction of nitric oxide with ammonia[J].Applied Catalysis B:Environmental,2008,79(4):347-355.
[23]Wu Z B,Jin R B,Wang H Q,et al.Effect of ceria doping on SO2resistance of Mn/TiO2 for selective catalytic reduction of NO with NH3 at low temperature[J].Catalysis Communications,2009,10(6):935-939.
[24]Cha W,Chin S M,Park E,et al.Effect of V2O5 loading of V2O5/TiO2 catalysts prepared via CVC and impregnation methods on NOx removal[J].Applied Catalysis B:Environmental,2013,140:708-715.
[25]Boningari T,Koirala R,Smirniotis P G.Low-temperature catalytic reduction of NO by NH3 over vanadia-based nanoparticles prepared by flame-assisted spray pyrolysis:Influence of various supports[J].Applied Catalysis B:Environmental,2013,140:289-298.
[26]Boningari T,Koirala R,Smirniotis P G.Low-temperature selective catalytic reduction of NO with NH3 over V/ZrO2 prepared by flame-assisted spray pyrolysis:structural and catalytic properties[J].Applied Catalysis B:Environmental,2012,127:255-264.
[27]Jiang Y,Gao X,Zhang Y X,et al.Effects of PbCl2 on selective catalytic reduction of NO with NH3 over vanadia-based catalysts[J].Journal of Hazardous Materials,2014,274:270-278.
[28]Chen M Y,Zhao M M,Tang F S,et al.Effect of Ce doping into V2O5-WO3/TiO2 catalysts on the selective catalytic reduction of NOx by NH3[J].Journal of Rare Earths,2017,35:1206-1215.
[29]Liu Z M,Li Y,Zhu T L,et al.Selective catalytic reduction of NOx by NH3 over Mn-promoted V2O5/TiO2 catalyst[J].Industrial and Engineering Chemistry Research,2014,53(33):12964-12970.
[30]Chen L,Li J H,Ge M F.The poisoning effect of alkali metals doping over nano V2O5-WO3/TiO2 catalysts on selective catalytic reduction of NOx by NH3[J].Chemical Engineering Journal,2011,170:531-537.
[31]Busca G,Lietti L,Ramis G,et al.Chemical and mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts:a review[J].Applied Catalysis B:Environmental,1998,18(1/2):1-36.
[32]Koebel M,Madia G,Elsener M.Selective catalytic reduction of NOand NO2 at low temperatures[J].Catalysis Today,2002,73(3/4):239-247.
[33]Vargas M A L,Casanova M,Trovarelli A,et al.An IR study of thermally stable V2O5-WO3-TiO2 SCR catalysts modified with silica and rare-earths(Ce,Tb,Er)[J].Applied Catalysis B:Environmental,2007,75(3/4):303-311.
[34]Li Q,Yang H S,Ma Z X,et al.Selective catalytic reduction of NOwith NH3 over CuOx-carbonaceous materials[J].Catalysis Communications,2012,17:8-12.
[35]Li Q,Yang H S,Qiu F M,et al.Promotional effects of carbon nanotubes on V2O5/TiO2 for NOx removal[J].Journal of Hazardous Materials,2011,192(2):915-921.
[36]Fan X Y,Qiu F M,Yang H S,et al.Selective catalytic reduction of NOx with ammonia over Mn-Ce-Ox/TiO2-carbon nanotube composites[J].Catalysis Communications,2011,12:1298-1301.
[37]Zhang L,Zhang D S,Zhang J P,et al.Design of meso-TiO2@MnOx-CeOx/CNTs with a core-shell structure as De NOx catalysts:promotion of activity,stability and SO2-tolerance[J].Nanoscale,2013,20:9821-9829.
[38]Zhang Y B,Zheng Y Y,Wang X,et al.Preparation of Mn-FeOx/CNTs catalysts by redox co-precipitation and application in low-temperature no reduction with NH3[J].Catalysis Communications,2015,62:57-61.
[39]Huang B C,Huang R,Jin D J,et al.Low temperature SCR of NOwith NH3 over carbon nanotubes supported vanadium oxides[J].Catalysis Today,2007,126(3/4):279-283.
[40]Huang Z G,Zhu Z P,Liu Z Y.Combined effect of H2O and SO2 on V2O5/AC catalysts for NO reduction with ammonia at lower temperatures[J].Applied Catalysis B:Environmental,2002,39(4):361-368.
[41]Huang Z G,Zhu Z P,Liu Z Y.Formation and reaction of ammonium sulfate salts on V2O5/AC catalyst during selective catalytic reduction of nitric oxide by ammonia at low temperatures[J].Journal of Catalysis,2003,214(2):213-219.
[42]Huang Z G,Liu Z Y,Zhang X L,et al.Inhibition effect of H2O on V2O5/AC catalyst for catalytic reduction of NO with NH3 at low temperature[J].Applied Catalysis B:Environmental,2006,63(3/4):260-265.
[43]Wu Z B,Jin R B,Wang H Q,et al.Effect of ceria doping on SO2resistance of Mn/TiO2 for selective catalytic reduction of NO with NH3 at low temperature[J].Catalysis Communications,2009,10(6):935-939.
[44]Sun D K,Liu Q Y,Liu Z Y,et al.An in situ drifts study on SCR of NO with NH3 over V2O5/AC surface[J].Catalysis Letters,2009,132(1/2):122-126.
[45]Jiang B Q,Deng B Y,Zhang Z Q,et al.Effect of Zr addition on the low-temperature SCR activity and SO2 tolerance of Fe-Mn/Ti catalysts[J].Journal of Physical Chemistry C,2014,118(27):14866-14875.
[46]Zhu Z P,Liu Z Y,Niu H X,et al.Promoting effect of SO2 on activated carbon-supported vanadia catalyst for NO reduction by NH3 at low temperatures[J].Journal of Catalysis,1999,187(1):245-248.
[47]Gálvez M E,Boyano A,Lázaro M J,et al.A study of the mechanisms of NO reduction over vanadium loaded activated carbon catalysts[J].Chemical Engineering Journal,2008,144(1):10-20.
[48]Ettireddy P R,Ettireddy N,Boningari T,et al.Investigation of the selective catalytic reduction of nitric oxide with ammonia over Mn/TiO2 catalysts through transient isotopic labeling and in situ FT-IR studies[J].Journal of Catalysis,2012,292:53-63.
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[50]Wang Y L,Ge C Z,Zhan L,et al.MnOx-CeO2/activated carbon honeycomb catalyst for selective catalytic reduction of NO with NH3at low temperatures[J].Industrial and Engineering Chemistry Research,2012,51(36):11667-11673.
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