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原位漫反射傅里叶变换红外光谱研究锰铁基催化剂上低温选择性催化还原反应机理
  • ISSN号:0253-9837
  • 期刊名称:《催化学报》
  • 时间:0
  • 分类:O6[理学—化学]
  • 作者机构:[1]上海交通大学动力机械及工程教育部重点实验室,上海200240
  • 相关基金:国家自然科学基金(51176118,51306115);中国博士后科学基金(2012M520894,2013T60445).
中文摘要:

采用自蔓延燃烧法制备了Ti0.9Mn0.05Fe0.05O2-δ催化剂,运用原位漫反射傅里叶变换红外光谱对该催化剂的NO和NH3稳态吸附以及NO和NH3瞬态反应进行了详细地分析与讨论.结果表明,相比于Lewis酸性位,150℃时Bronsted酸性位吸附的NH3更具有SCR活性;与双齿硝酸盐和桥式硝酸盐相比, NO吸附产生的单齿硝酸盐是主要的中间物种;该SCR反应遵循Eley-Rideal和Langmuir-Hinshelwood机理,但以后者为主.另外, O2的存在有利于NO的氧化和配位态NH3的活化.

英文摘要:

To investigate the mechanism of selective catalytic reduction (SCR) of NOx with NH3, Ti0.9Mn0.05Fe0.05O2-δ catalyst was prepared by self-propagating high-temperature synthesis (SHS) method and evaluated at 25-450 ℃. The catalyst was characterized by X-ray diffraction (XRD) and transmission electron microscopy (TEM). The possible SCR mechanism over Ti0.9Mn0.05Fe0.05O2-δ was studied by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). Ti0.9Mn0.05Fe0.05O2-δ showed both high SCR activity and N2 selectivity over a broad temperature win-dow of 100-350 ℃. The XRD and TEM results indicated that the active components of Mn and Fe were in a highly dispersed state and in an amorphous form on TiO2. The DRIFTS results revealed that Bronsted acid sites were the active centers for NO removal and monodentate nitrates were the key intermediate in the SCR reaction. At 150 ℃, both Langmuir-Hinshelwood and Eley-Rideal mechanisms are involved in the SCR reaction, while the former one mechanism dominates the cata-lytic activity of Ti0.9Mn0.05Fe0.05O2-δ. Additionally, the presence of O2 significantly affects NO oxidation and coordinated NH3 activation.

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期刊信息
  • 《催化学报》
  • 北大核心期刊(2011版)
  • 主管单位:中国科学院
  • 主办单位:中国化学会 中国科学院大连化学物理研究所
  • 主编:李灿 张涛
  • 地址:大连市沙河口区中山路457号
  • 邮编:116023
  • 邮箱:chxb@dicp.ac.cn
  • 电话:0411-84379240
  • 国际标准刊号:ISSN:0253-9837
  • 国内统一刊号:ISSN:21-1195/O6
  • 邮发代号:8-93
  • 获奖情况:
  • 第三届国家期刊奖提名奖,中国科协精品科技期刊示范项目
  • 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,美国剑桥科学文摘,美国科学引文索引(扩展库),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),英国英国皇家化学学会文摘,中国北大核心期刊(2000版)
  • 被引量:19199