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Ce doping to Cu-SAPO-18: Enhanced catalytic performance for the NH3-SCR of NO in simulated diesel exhaust
Microporous and Mesoporous Materials ( IF 4.8 ) Pub Date : 2018-09-27 , DOI: 10.1016/j.micromeso.2018.09.027
Shuai Han , Jin Cheng , Qing Ye , Shuiyuan Cheng , Tianfang Kang , Hongxing Dai

The Ce-Cu-SAPO-18 catalysts were prepared by the ion exchange method. The Ce-Cu-SAPO-18-2 catalyst with a Ce content of 1.24 wt% showed the excellent NH3-SCR activity. Characterization results demonstrated that the Ce-Cu-SAPO-18-2 catalyst possessed strong redox ability and high reactive nitrate and NH3 species, which were responsible for the remarkable SCR performance. The best-performing Ce-Cu-SAPO-18-2 catalyst displayed a broad operation temperature window, a result possibly due to the improvement of physicochemical properties and acceleration of reaction rate in the Langmuir−Hinshelwood (L−H) and Eley−Rideal (E−R) mechanisms. The higher amounts of isolated Cu2+ species and acid sites in Ce-Cu-SAPO-18-2 promoted the adsorption and activation of NO, and facilitated the reaction between the adsorbed NOx species and the gas-phase NH3 molecules according to the L−H mechanism. For the E−R mechanism, the NH3 (L) species were the crucial initial intermediates for NH3 activation, and the more amount of Lewis acid sites in the Ce-Cu-SAPO-18-2 sample originated from its coordinatively unsaturated cationic sites benefited the reaction between the adsorbed NH3 species and NO molecules. Based on the results of in situ DRIFTS characterization, we believe that the L−H mechanism dominated the NH3-SCR reaction at low temperatures, and the doping of Ce in the catalyst improved the L−H and E−R reactions at low temperatures.



中文翻译:

Ce对Cu-SAPO-18的掺杂:增强了模拟柴油机废气中NO的NH 3 -SCR的催化性能

通过离子交换法制备了Ce-Cu-SAPO-18催化剂。Ce含量为1.24wt%的Ce-Cu-SAPO-18-2催化剂显示出优异的NH 3 -SCR活性。表征结果表明,Ce-Cu-SAPO-18-2催化剂具有较强的氧化还原能力和较高的反应性硝酸盐和NH 3种类,这是SCR性能优异的原因。表现最佳的Ce-Cu-SAPO-18-2催化剂显示出较宽的操作温度范围,其结果可能是由于Langmuir-Hinshelwood(L-H)和Eley-Rideal的理化性质和反应速率的提高所致(ER)机制。分离出的Cu 2+的量更高根据L-H机理,Ce-Cu-SAPO-18-2中的碳原子类型和酸位促进了NO的吸附和活化,并促进了吸附的NO x物种与气相NH 3分子之间的反应。对于E-R机理,NH 3(L)物种是NH 3活化的关键初始中间体,并且Ce-Cu-SAPO-18-2样品中更多的路易斯酸位源自其配位不饱和阳离子这些位点有利于吸附的NH 3物种与NO分子之间的反应。根据原位DRIFTS表征的结果,我们认为L-H机制主导了NH 3低温下的-SCR反应以及催化剂中Ce的掺杂改善了低温下的LH和E-R反应。

更新日期:2018-09-27
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