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一锅法合成用于 NH3 选择性催化还原 NO 的 CeO-CePO4 纳米棒复合材料:活性位与反应机理

One-pot synthesis of ceria and cerium phosphate (CeO-CePO) nanorod composites for selective catalytic reduction of NO with NH: Active sites and reaction mechanism.

机构信息

School of Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, PR China.

School of Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, PR China.

出版信息

J Colloid Interface Sci. 2018 Aug 15;524:8-15. doi: 10.1016/j.jcis.2018.04.003. Epub 2018 Apr 3.

Abstract

In this work, novel (CeO)-(CePO) (defined as CeP) nanorod composites were prepared by a simple co-precipitation method, and the influence of CeO on the catalytic performance of CePO for selective catalytic reduction of NO by NH (NH-SCR of NO) was investigated. The catalytic performance evaluation revealed that the CeP catalysts, especially CeP exhibited a much better catalytic activity and HO + SO resistance than CePO. Structure characterizations via high-resolution transmission electron microscope (HRTEM) and Brunauer-Emmett-Teller (BET) revealed that the introduction of CeO had a little effect on the shape of CePO nanorods and it could promote the formation of new mesoporous then significantly enhance the surface area of catalyst. The analysis results of active sites suggested that phosphorus was the main adsorption site for NH and the redox sites were controlled by CeO on CeP catalysts. Finally, reaction process study demonstrated that the NH-SCR over CeP was processed via Langmuir-Hinshelwood (L-H) mechanism. Combining the results of active sites and reaction mechanism analysis, it was drawn that the superior low temperature activity of CeP could be attributed to its excellent redox properties, which promoted the oxidation of NO then facilitated the process of NH-SCR via "fast SCR".

摘要

在这项工作中,通过简单的共沉淀法制备了新型(CeO)-(CePO)(定义为 CeP)纳米棒复合材料,并研究了 CeO 对 CePO 用于选择性催化还原 NO 的 NH(NO 的 NH-SCR)的催化性能的影响。催化性能评价表明,CeP 催化剂,尤其是 CeP 表现出比 CePO 更高的催化活性和抗 HO+SO 能力。通过高分辨率透射电子显微镜(HRTEM)和 Brunauer-Emmett-Teller(BET)进行的结构特征研究表明,CeO 的引入对 CePO 纳米棒的形状几乎没有影响,但可以促进新介孔的形成,从而显著提高催化剂的表面积。活性位分析结果表明,磷是 NH 的主要吸附位,而氧化还原位由 CeP 催化剂上的 CeO 控制。最后,反应过程研究表明,CeP 上的 NH-SCR 是通过 Langmuir-Hinshelwood(L-H)机制进行的。结合活性位和反应机理分析的结果,得出 CeP 具有优异的低温活性,这归因于其优异的氧化还原性能,促进了 NO 的氧化,然后通过“快速 SCR”促进了 NH-SCR 过程。

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