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Pt修饰和反应气氛对富铝Cu-Beta分子筛NH3-SCR反应性能的影响
  • ISSN号:1001-3555
  • 期刊名称:《分子催化》
  • 时间:0
  • 分类:O643.3[理学—物理化学;理学—化学]
  • 作者机构:大连理工大学化工学院精细化工国家重点实验室,辽宁大连116024
  • 相关基金:国家自然科学基金(21173029,21373035,21603022)及中央高校基本科研业务费专项资金(DUT16RC(3)002)项目资助
中文摘要:

富铝Cu-Beta分子筛具有优异的低温NH3-SCR性能,在汽车尾气脱硝中具有潜在的应用前景.我们考察了H2O、CO2、丙烯等气氛对富铝Cu-Beta分子筛NH3-SCR反应性能的影响.发现H2O会降低催化剂的低温活性,CO2则提高低温活性,丙烯对中、低温活性均有明显抑制作用.固体13C核磁共振显示丙烯在分子筛上形成链状脂肪烃积碳,导致催化剂的活性降低.Pt修饰使丙烯存在下低温NH3-SCR活性有所提高,但在中高温度下会催化NH3氧化产生大量的N2O和NO,从而降低了NO转化率.电子顺磁共振(EPR)和紫外-可见(UV-Vis)光谱研究表明,Pt的引入使部分孤立铜离子转化为簇状多聚态铜离子,会进一步加剧高温NH3氧化反应的发生,进而降低了催化剂的活性.

英文摘要:

NOx emission arising from consumption brings serious impact on public's lives and health. of fossil fuels increases significantly during recent years, and Selective catalytic reduction of NO by NH3 (NH3-SCR) as the most effective technique has been widely used in NOx abatement. However, the commercial V2O5-WO3-ZiO2 catalyst used in stationary emission has intrinsic biological toxicity and narrow operating temperature window, which is restricted in mobile emissions. In this study, 4% Cu/Al-rich Beta zeolite (Si/Al = 4) was prepared by aqueous CuE+ ion-exchange with Al-rich Beta zeolite synthesized from organotemplate-free approach, which shows excellent catalytic performance at low temperature in NHa-SCR reaction with 100% NO conversion at 175 ℃. It is a promi- sing DeNOx catalyst for application in diesel engine exhaust treatment. In order to mimic the real working environ- ment as exhaust gas, the effects of co-feeding 5% (V/V) n20- 10% (V/V) CO2 and 300 ppm propene on NH3- SCR performance of Cu/Al-rich Beta were also investigated. It' s found that the low-temperature activity of Cu/A1- rich Beta was decreased in the presence of H2O, while CO2 enhanced the low-temperature activity, and propene in- hibited the catalytic activity significantly at both low and medium temperatures from 150 to 500 ℃. All the components had little effect on the high temperature activity. Solid-state lac magic angle spinning nuclear magnetic reso- nance (MAS NMR) indicated paraffin as deposited carbon was formed from the polymerization of propene in the pores of zeolite. Cu/Al-rieh Beta catalysts doped with different amount of Pt ranging from 0.03% to 0.8% were prepared by incipient wetness impregnation of Cu/Al-rich Beta with aqueous solution of H2PtCl6·6H2O, and pro- pene tolerance of Pt-Cu/Al-rich Beta catalysts were investigated. It' s found Pt modification can indeed enhance the low-temperature SCR performance by 10% at 150 ℃ in the presence of propene. However, combined with am-monia oxidation e

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期刊信息
  • 《分子催化》
  • 中国科技核心期刊
  • 主管单位:中国科学院
  • 主办单位:中国化学会 中国科学院兰州化学物理研究所
  • 主编:李树本
  • 地址:兰州市天水路18号
  • 邮编:730000
  • 邮箱:fzch@licp.cas.cn
  • 电话:0931-4968226
  • 国际标准刊号:ISSN:1001-3555
  • 国内统一刊号:ISSN:62-1039/O6
  • 邮发代号:54-69
  • 获奖情况:
  • 1992年获中国科学院优秀期刊三等奖,1992年获甘肃省第二届优秀科技期刊荣誉称号
  • 国内外数据库收录:
  • 俄罗斯文摘杂志,美国化学文摘(网络版),荷兰文摘与引文数据库,美国工程索引,日本日本科学技术振兴机构数据库,中国中国科技核心期刊,中国北大核心期刊(2004版),中国北大核心期刊(2008版),中国北大核心期刊(2011版),中国北大核心期刊(2014版),中国北大核心期刊(2000版)
  • 被引量:7932