MnO2的晶相结构和表面性质对低温NH3-SCR反应的影响

采用水热法合成了两种具有相同形貌但是不同物相结构的MnO2纳米棒,分别为隧道状和层状结构。考察其低温NH。选择性催化还原NOx(NH3-SCR)的性能.结果表明MnO2纳米棒的比表面积不是影响活性的主要因素,催化剂的晶相结构和表面性质对催化活性有很大影响,隧道状a-MnO2纳米棒的低温NH3-SCR活性明显高于层状5-MnO2纳米棒.结构分析和NH。程序升温脱附(NH3-TPD)实验表明,a-MnO2纳米棒的暴露晶面(110)面存在大量的配位不饱和Mn离子,形成较多的Lewis酸性位点,而且a-MnO2较弱的Mn—O键和隧道结构都有利于NH。的吸附:而δ-MnO2纳米棒的暴露晶面(001)面上...

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Bibliographic Details
Published in物理化学学报 Vol. 28; no. 7; pp. 1771 - 1776
Main Author 戴韵 李俊华 彭悦 唐幸福
Format Journal Article
LanguageChinese
Published 清华大学环境学院,环境模拟与污染控制国家重点联合实验室,北京100084%复旦大学环境科学与工程系,上海,200433 2012
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ISSN1000-6818
DOI10.3866/PKU.WHXB201204175

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Summary:采用水热法合成了两种具有相同形貌但是不同物相结构的MnO2纳米棒,分别为隧道状和层状结构。考察其低温NH。选择性催化还原NOx(NH3-SCR)的性能.结果表明MnO2纳米棒的比表面积不是影响活性的主要因素,催化剂的晶相结构和表面性质对催化活性有很大影响,隧道状a-MnO2纳米棒的低温NH3-SCR活性明显高于层状5-MnO2纳米棒.结构分析和NH。程序升温脱附(NH3-TPD)实验表明,a-MnO2纳米棒的暴露晶面(110)面存在大量的配位不饱和Mn离子,形成较多的Lewis酸性位点,而且a-MnO2较弱的Mn—O键和隧道结构都有利于NH。的吸附:而δ-MnO2纳米棒的暴露晶面(001)面上的Mn离子已达到配位饱和,所以其表面Lewis酸性位点较少.X射线光电子能谱(XPS)和热重(TG)分析表明a-MnO2纳米棒的表面更有利于NH3和NOX的活化.具有有利于吸附NH3和活化NH3和N0x的表面性质和晶型结构,是a-MnO:纳米棒活性高的主要原因.
Bibliography:11-1892/06
DAI Yun, LI Jun-Hua, PENG Yue,TANG Xing-Fu (1.State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beo'ing 100084, P. R. China; 2.Department of Environmental Science and Engineering, Fudan University, Shanghai 200433, P. R. China)
Two manganese oxides with the same nanorod-shaped morphology but different crystal structures, tunnel and layer structures, were synthesized and investigated for selective catalytic reduction of NOx with NH3 (NH3-SCR) at low temperature. Tunneled e-MnO2 had much higher catalytic activity than layered δ-MnO2 under the same reaction conditions. Experiment results revealed that the surface area was not the main factor to affect the NH3-SCR activities over the MnO2 nanorods and that the activities were structure sensitive. Structure analysis and temperature-programmed desorption experiments of NH3 (NH~-TPD) suggested that the exposed (110) plane of e-MnO2 had many Mn cations in coordinatively unsaturated environ
ISSN:1000-6818
DOI:10.3866/PKU.WHXB201204175