Fe掺杂Mn-Ce/AC催化剂的制备及其低温脱硝
|
摘要
以活性炭为载体,采用浸渍法制备了一系列Fe掺杂Mn-Ce/AC催化剂,研究了Fe的添加量、焙烧温度对催化剂低温脱硝活性的影响;采用了XRD、SEM和N2吸附-脱附技术对催化剂进行了表征。结果表明,Fe的添加能有效提高Mn-Ce/AC的低温脱硝活性,当Fe的添加量为Fe/Mn(摩尔比)为0.1时,催化剂比表面积大,活性组分的分散程度较高,催化剂低温脱硝性能最优,添加量大于0.1时,更多的Fe沉积在载体表面,催化剂活性降低。焙烧温度影响负载氧化物的价态和晶体的分散度,在400℃温度下焙烧时,催化剂低温脱硝性能最佳,此时催化剂孔隙结构较优,活性组分的分散程度也较高。
Fe-doped Mn-Ce / AC catalysts were prepared via a wet impregnation method and characterized through N2adsorption-desorption,X-ray diffraction,and scanning electron microscopy. The effects of the amount of Fe added and calcination temperature were studied. The NO removal activity of the Mn-Ce / AC catalyst increased clearly after the addition of Fe. When the amount of Fe added was 0. 1( molar ratio between Mn and Fe),the catalyst exhibited the highest NO reduction activity,with a high surface area and widely dispersed active components. The catalytic activity of the samples decreased when the Fe loading was greater than 0. 1. The calcination temperature influenced the valence of the oxides and the dispersion of crystals,and the optimal catalyst calcination temperature was 400 ℃,because the catalyst calcined at 400 ℃ had a superior pore structure and the active components showed better dispersion on the carbon surface.
Fe-doped Mn-Ce / AC catalysts were prepared via a wet impregnation method and characterized through N2adsorption-desorption,X-ray diffraction,and scanning electron microscopy. The effects of the amount of Fe added and calcination temperature were studied. The NO removal activity of the Mn-Ce / AC catalyst increased clearly after the addition of Fe. When the amount of Fe added was 0. 1( molar ratio between Mn and Fe),the catalyst exhibited the highest NO reduction activity,with a high surface area and widely dispersed active components. The catalytic activity of the samples decreased when the Fe loading was greater than 0. 1. The calcination temperature influenced the valence of the oxides and the dispersion of crystals,and the optimal catalyst calcination temperature was 400 ℃,because the catalyst calcined at 400 ℃ had a superior pore structure and the active components showed better dispersion on the carbon surface.
引文
[1]马倩,胡将军,李闯,等.Ce O2-Co O/ACF低温SCR烟气脱氮性能的研究[J].环境工程学报,2010,4(4):899-903
[2]KARAMI A,SALEHI V.The influence of chromium substitution on an iron-titanium catalyst used in the selective catalytic reduction of NO[J].Journal of Catalysis,2012,292:32-43
[3]SHEN Boxiong,CHEN Jianhong,YUE Shiji,et al.A comparative study of modified cotton biochar and activated carbon based catalysts in low temperature SCR[J].Fuel,2015,156:47-53
[4]KLINIK J,SAMOJEDE B,GRZYBEK T,et al.Nitrogen promoted activated carbons as De NOxcatalysts.2.The influence of water on the catalytic performance[J].Catalysis Today,2011,176(1):303-308
[5]SHEN Boxiong,LIU Tong,ZHAO Ning,et al.Iron-doped Mn-Ce/Ti O2catalyst for low temperature selective catalytic reduction of NO with NH3[J].Journal of Environmental Sciences,2010,22(9):1447-1454
[6]WU Zhongbiao,JIN Ruiben,LIU Yue,et al.Ceria modified Mn Ox/Ti O2as a superior catalyst for NO reduction with NH3at low-temperature[J].Catalysis Communications,2008,9(13):2217-2220
[7]QI Gongshi,YANG R T.Performance and kinetics study for low-temperature SCR of NO with NH3over Mn Ox-Ce O2catalyst[J].Journal of Catalysis,2003,217(2):434-441
[8]金瑞奔.负载型Mn-Ce系列低温SCR脱硝催化剂制备、反应机理及抗硫性能研究[D].杭州:浙江大学,2010
[9]ZHOU Guangying,ZHONG Biaocheng,WANG Wenhui,et al.In situ DRIFTS study of NO reduction by NH3over Fe-Ce-Mn/ZSM-5 catalysts[J].Catalyst Today,2011,175(1):157-163
[10]GRZYBEK T,KLINIK J,MOTAK M,et al.Nitrogen-promoted active carbons as catalytic supports:2.The influence of Mn promotion on the structure and catalytic properties in SCR[J].Catalysis Today,2008,137(2/3/4):235-241
[11]吴海苗,王晓波,归柯庭.以活性炭为载体的负载型催化剂的SCR脱硝性能[J].东南大学学报(自然科学版),2013,43(4):814-818
[12]杨超,张俊丰,童志权,等.活性炭低温催化还原NOx影响因素及反应机理分析[J].环境科学研究,2006,19(4):86-90
[13]GUO Jiaxiu,QU Yifan,SHU Song,et al.Effects of preparation conditions on Mn-based activated carbon catalysts for desulfurization[J].New Journal of Chemistry,2015,39(8):5997-6015
[14]KHAN A,SMIRNIOTIS P G.Relationship between temperature-programmed reduction profile and activity of modified ferritebased catalysts for WGS reaction[J].Journal of Molecular Catalysis A:Chemical,2008,280(1/2):43-51
[15]曹伟.改性玻璃纤维负载复合铁锰铈氧化物低温选择性催化还原NO[D].上海:东华大学,2015
[16]LI Le,DIAO Yongfa,LIU Xin.Ce-Mn mixed oxides supported on glass-fiber for low-temperature selective catalytic reduction of NO with NH3[J].Journal of Rare Earths,2014,32(5):409-415
[17]KAPTEIJN F,SINGOREDJO L,ANDREINI A.Activity and selectivity of pure manganese oxides in the selective catalytic reduction of nitric oxide with ammonia[J].Applied Catalysis B:Environmental,1994,3(2/3):173-189
[18]张恒建.柱状凹凸棒石-活性炭负载锰氧化物低温SCR脱硝催化剂性能研究[D].合肥:合肥工业大学,2014
[2]KARAMI A,SALEHI V.The influence of chromium substitution on an iron-titanium catalyst used in the selective catalytic reduction of NO[J].Journal of Catalysis,2012,292:32-43
[3]SHEN Boxiong,CHEN Jianhong,YUE Shiji,et al.A comparative study of modified cotton biochar and activated carbon based catalysts in low temperature SCR[J].Fuel,2015,156:47-53
[4]KLINIK J,SAMOJEDE B,GRZYBEK T,et al.Nitrogen promoted activated carbons as De NOxcatalysts.2.The influence of water on the catalytic performance[J].Catalysis Today,2011,176(1):303-308
[5]SHEN Boxiong,LIU Tong,ZHAO Ning,et al.Iron-doped Mn-Ce/Ti O2catalyst for low temperature selective catalytic reduction of NO with NH3[J].Journal of Environmental Sciences,2010,22(9):1447-1454
[6]WU Zhongbiao,JIN Ruiben,LIU Yue,et al.Ceria modified Mn Ox/Ti O2as a superior catalyst for NO reduction with NH3at low-temperature[J].Catalysis Communications,2008,9(13):2217-2220
[7]QI Gongshi,YANG R T.Performance and kinetics study for low-temperature SCR of NO with NH3over Mn Ox-Ce O2catalyst[J].Journal of Catalysis,2003,217(2):434-441
[8]金瑞奔.负载型Mn-Ce系列低温SCR脱硝催化剂制备、反应机理及抗硫性能研究[D].杭州:浙江大学,2010
[9]ZHOU Guangying,ZHONG Biaocheng,WANG Wenhui,et al.In situ DRIFTS study of NO reduction by NH3over Fe-Ce-Mn/ZSM-5 catalysts[J].Catalyst Today,2011,175(1):157-163
[10]GRZYBEK T,KLINIK J,MOTAK M,et al.Nitrogen-promoted active carbons as catalytic supports:2.The influence of Mn promotion on the structure and catalytic properties in SCR[J].Catalysis Today,2008,137(2/3/4):235-241
[11]吴海苗,王晓波,归柯庭.以活性炭为载体的负载型催化剂的SCR脱硝性能[J].东南大学学报(自然科学版),2013,43(4):814-818
[12]杨超,张俊丰,童志权,等.活性炭低温催化还原NOx影响因素及反应机理分析[J].环境科学研究,2006,19(4):86-90
[13]GUO Jiaxiu,QU Yifan,SHU Song,et al.Effects of preparation conditions on Mn-based activated carbon catalysts for desulfurization[J].New Journal of Chemistry,2015,39(8):5997-6015
[14]KHAN A,SMIRNIOTIS P G.Relationship between temperature-programmed reduction profile and activity of modified ferritebased catalysts for WGS reaction[J].Journal of Molecular Catalysis A:Chemical,2008,280(1/2):43-51
[15]曹伟.改性玻璃纤维负载复合铁锰铈氧化物低温选择性催化还原NO[D].上海:东华大学,2015
[16]LI Le,DIAO Yongfa,LIU Xin.Ce-Mn mixed oxides supported on glass-fiber for low-temperature selective catalytic reduction of NO with NH3[J].Journal of Rare Earths,2014,32(5):409-415
[17]KAPTEIJN F,SINGOREDJO L,ANDREINI A.Activity and selectivity of pure manganese oxides in the selective catalytic reduction of nitric oxide with ammonia[J].Applied Catalysis B:Environmental,1994,3(2/3):173-189
[18]张恒建.柱状凹凸棒石-活性炭负载锰氧化物低温SCR脱硝催化剂性能研究[D].合肥:合肥工业大学,2014