陆强1,
韩健1,
杨江毅1,2,
李文艳2,
杨勇平1
1.华北电力大学生物质发电成套设备国家工程实验室,北京 102206
2.华北电力大学能源动力与机械工程学院,北京 102206
基金项目: 国家重点基础研究发展计划(973)项目(2015CB251501)
北京科技新星计划项目(Z171100001117064)
Effect of preparation technology on De-NOx performance of V2O5/TiO2 SCR catalysts
LI Hui1,2,LU Qiang1,
HAN Jian1,
YANG Jiangyi1,2,
LI Wenyan2,
YANG Yongping1
1.National Engineering Laboratory for Biomass Power Generation Equipment, North China Electric Power University, Beijing 102206, China
2.School of Energy Power and Mechanical Engineering, North China Electric Power University, Beijing 102206, China
-->
摘要
HTML全文
图
参考文献
相关文章
施引文献
资源附件
访问统计
摘要:围绕SCR脱硝催化剂制备工艺中活性组分负载顺序和钒助溶剂2个关键因素,分别制备了钒钨体系和钒钼体系催化剂,比较了不同条件下制备的催化剂的脱硝活性,并利用X射线光电子能谱分析(XPS)、程序升温还原(H2-TPR)和程序升温脱附(NH3-TPD)等手段进行表征。结果表明,活性组分与助剂同时负载制备的催化剂,其低价钒和化学吸附氧的比例最高,钒的还原温度最低,酸性位数量最多,表现出最好的脱硝活性;相较于常规助溶剂单乙醇胺,以草酸为助溶剂制备的催化剂,其低价钒和化学吸附氧比例更高,氧化还原性能和表面酸性更强,脱硝活性更好。
关键词: SCR催化剂/
烟气脱硝/
负载顺序/
助溶剂/
催化活性
Abstract:V-W and V-Mo catalysts were prepared focusing on the two key points during the preparation process of SCR denitrification catalyst, i.e., the active components loading sequences and the cosolvents of vanadium. The denitrification activities of the catalysts prepared with different methods were compared, and the catalysts were also characterized by X-ray photoelectron spectroscopy (XPS), temperature-programmed reduction (H2-TPR) and temperature programmed desorption (NH3-TPD). The results showed that the catalysts prepared via simultaneous loading of the active component and promoter exhibited the highest proportions of low valence vanadium and chemisorbed oxygen, the lowest reduction temperature of vanadium, largest amount of acid sites, and thus, possessing the best denitrification activity. In addition, compared to conventional cosolvent monoethanolamine, the catalysts prepared with oxalic acid showed higher proportions of low valence vanadium and chemisorbed oxygen, better oxidation-reduction performance as well as stronger surface acidity, resulting in better denitrification activity.
Key words:SCR catalyst/
flue gas denitrification/
loading sequence/
cosolvent/
catalytic activity.
[1] | 喻明娥,李彩亭,王琰,等. 以改性TiO2-SnO2为载体的SCR脱硝催化剂性能[J]. 环境工程学报,2016,10(7):3733-3738 10.12030/j.cjee.201502049 |
[2] | 陶莉,张旭楠,李彩亭,等. 选择性催化还原催化剂氧化脱除烟气中单质汞[J]. 环境工程学报,2015,9(6):2925-2932 |
[3] | 石晓燕,丁世鹏,贺泓,等. 改进钒基SCR脱硝催化剂的抗碱金属中毒性能[J]. 环境工程学报,2014,8(5):2031-2034 |
[4] | BURKARDT A, WEIWEILER W, VAN DEN TILLAART J, et al.Influence of the V2O5 loading on the structure and activity of V2O5/TiO2 SCR catalysts for vehicle application[J].Topics in Catalysis,2001,16(1):369-375 10.1023/A:1016673418398 |
[5] | TANG F S,ZHUANG K,YANG L L, et al.Effect of dispersion stte and surface properties of supported vanadia on the activity of V2O5/TiO2 catalysts for the selective catalytic reduction of NO by NH3[J].Chinese Journal of Catalysis,2012,33(6):933-940 10.1016/S1872-2067(11)60365-3 |
[6] | GAN L,GUO F,YU J, et al.Improved low-temperature activity of V2O5-WO3/TiO2 for denitration using different vanadium precursors[J].Journal of Catalysis,2016,6(2):25-39 10.3390/catal6020025 |
[7] | DONG G J,ZHANG Y F,ZHAO Y, et al.Effect of the pH value of precursor solution on catalytic performance of V2O5-WO3/TiO2 in the low temperature NH3-SCR of NOx [J].Journal of Fuel Chemistey and Technology,2014,42(12):1455-1463 10.1016/S1872-5813(15)60003-2 |
[8] | PUTLURU S S R,SCHILL L,GARDINI D, et al.Superior DeNOx activity of V2O5–WO3/TiO2 catalysts prepared by deposition–precipitation method[J].Journal of Materials Science,2014,49(7):2705-2713 10.1007/s10853-013-7926-0 |
[9] | ZHU L,ZHONG Z P,YONG H, et al.Effect of MoO3 on vanadium based catalysts for the selective catalytic reduction of NOx with NH3 at low temperature[J].Journal of Environmental Sciences,2017,56(6):169-179 10.1016/j.jes.2016.08.025 |
[10] | 高慧聪.V4+/V5+比值调变与SCR脱硝活性及催化剂性能[D]. 哈尔滨: 哈尔滨工程大学,2013 |
[11] | 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 10.1016/j.cej.2016.02.094 |
[12] | TOPOSE N,DUMESIC J,TOPOSE H, et al.Vanadia-titania catalysts for selective catalytic reduction of nitric-oxide by ammonia: I.I.Studies of active sites and formulation of catalytic cycles[J].Journal of Catalysis,1995,151(1):241-252 10.1006/jcat.1995.1025 |
[13] | TOPOSE N,TOPOSE H,DUMESIC J, et al.Vanadia/titania catalysts for selective catalytic reduction (SCR) of nitric-oxide by ammonia: I.Combined temperature-programmed in-situ FTIR and on-line mass-spectroscopy studies[J].Journal of Catalysis,1995,151(1):226-240 10.1006/jcat.1995.1024 |
[14] | RAMIS G,YI L,BUSCA G, et al.Adsorption, activation, and oxidation of ammonia over SCR catalysts[J].Journal of Catalysis,1995,157(2):523-535 10.1006/jcat.1995.1316 |
[15] | CIAMBELLI P,BAGNASCO G,LISI L, et al.Vanadium oxide catalysts supported on laser-synthesized titania powders: Characterization and catalytic activity in the selective reduction of nitric oxide[J].Applied Catalysis B:Environmental,1992,1(2):61-77 10.1016/0926-3373(92)80033-V |
[16] | 赵乐乐,王守信,王远洋,等.V2O5-WO3/TiO2催化剂的制备及其烟气脱硝性能[J]. 工业催化,2015,23(11): 874-881 |
[17] | 吕汉清. 负载型钒钨脱硝催化剂的制备及其脱硝性能[D]. 重庆: 重庆大学,2011 |
[18] | LIETTI L,NOVA I,RAMIS G, et al.Characterization and reactivity of V2O5-MoO3/TiO2 De-NOx SCR catalysts[J].Journal of Catalysis,1999,187(2):419-435 10.1006/jcat.1999.2603 |
[19] | KOBAYSHI M,KUMA R,MORITA A, et al.Low temperature selective catalytic reduction of NO by NH3 over V2O5 supported on TiO2-SiO2-MoO3[J].Catalysis Letters,2006,112(1):37-44 10.1007/s10562-006-0161-4 |
[20] | CASANOVA M,LLORCA J,SAGAR A, et al.Mixed iron-erbium vanadate NH3-SCR catalysts[J].Catalysis Today,2015,241:159-168 10.1016/j.cattod.2014.03.051 |
[21] | KANG M,PARK E D,KIM J M, et al.Manganese oxide catalysts for NOx reduction with NH3 at low temperatures[J].Applied Catalysis A:General,2007,327(2):261-269 10.1016/j.apcata.2007.05.024 |
[22] | ZHAO K,HAN W,TANG Z, et al.Investigation of coating technology and catalytic performance over monolithic V2O5-WO3/TiO2 catalyst for selective catalytic reduction of NOx with NH3[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2016,503:53-60 10.1016/j.colsurfa.2016.05.014 |
[23] | LIU F,HE H,ZHANG C, et al.Novel iron titanate catalyst for the selective catalytic reduction of NO with NH3 in the medium temperature range[J].Chemical Communications,2008,17:2043-2045 10.1039/B800143J |
[24] | SEO P W,LEE J Y,SHIM K S, et al.The control of valence state: How V/TiO2 catalyst is hindering the deactivation using the mechanochemical method[J].Journal of Hazardous Materials,2009,165(1/2/3):39-47 10.1016/j.jhazmat.2008.09.119 |
[25] | MEJRI I,AYARI F,MHAMDI M, et al.SCR of NO by NH3 catalyzed by Mo- and V-exchanged zeolite: Effect of Mo precursor salt[J].Microporous and Mesoporous Materials,2016,220:239-246 10.1016/j.micromeso.2015.09.014 |
Turn off MathJax -->
点击查看大图
计量
文章访问数:1092
HTML全文浏览数:830
PDF下载数:366
施引文献:0
出版历程
刊出日期:2018-07-26
-->
制备工艺对V2O5/TiO2 SCR催化剂脱硝性能的影响
李慧1,2,陆强1,
韩健1,
杨江毅1,2,
李文艳2,
杨勇平1
1.华北电力大学生物质发电成套设备国家工程实验室,北京 102206
2.华北电力大学能源动力与机械工程学院,北京 102206
基金项目: 国家重点基础研究发展计划(973)项目(2015CB251501) 北京科技新星计划项目(Z171100001117064)
关键词: SCR催化剂/
烟气脱硝/
负载顺序/
助溶剂/
催化活性
摘要:围绕SCR脱硝催化剂制备工艺中活性组分负载顺序和钒助溶剂2个关键因素,分别制备了钒钨体系和钒钼体系催化剂,比较了不同条件下制备的催化剂的脱硝活性,并利用X射线光电子能谱分析(XPS)、程序升温还原(H2-TPR)和程序升温脱附(NH3-TPD)等手段进行表征。结果表明,活性组分与助剂同时负载制备的催化剂,其低价钒和化学吸附氧的比例最高,钒的还原温度最低,酸性位数量最多,表现出最好的脱硝活性;相较于常规助溶剂单乙醇胺,以草酸为助溶剂制备的催化剂,其低价钒和化学吸附氧比例更高,氧化还原性能和表面酸性更强,脱硝活性更好。
English Abstract
Effect of preparation technology on De-NOx performance of V2O5/TiO2 SCR catalysts
LI Hui1,2,LU Qiang1,
HAN Jian1,
YANG Jiangyi1,2,
LI Wenyan2,
YANG Yongping1
1.National Engineering Laboratory for Biomass Power Generation Equipment, North China Electric Power University, Beijing 102206, China
2.School of Energy Power and Mechanical Engineering, North China Electric Power University, Beijing 102206, China
Keywords: SCR catalyst/
flue gas denitrification/
loading sequence/
cosolvent/
catalytic activity
Abstract:V-W and V-Mo catalysts were prepared focusing on the two key points during the preparation process of SCR denitrification catalyst, i.e., the active components loading sequences and the cosolvents of vanadium. The denitrification activities of the catalysts prepared with different methods were compared, and the catalysts were also characterized by X-ray photoelectron spectroscopy (XPS), temperature-programmed reduction (H2-TPR) and temperature programmed desorption (NH3-TPD). The results showed that the catalysts prepared via simultaneous loading of the active component and promoter exhibited the highest proportions of low valence vanadium and chemisorbed oxygen, the lowest reduction temperature of vanadium, largest amount of acid sites, and thus, possessing the best denitrification activity. In addition, compared to conventional cosolvent monoethanolamine, the catalysts prepared with oxalic acid showed higher proportions of low valence vanadium and chemisorbed oxygen, better oxidation-reduction performance as well as stronger surface acidity, resulting in better denitrification activity.