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Superior catalytic performance within H2O-vapor of W-modified CoMn2O4/TiO2 catalyst for selective catalytic reduction of NOx with NH3

催化作用 氮氧化物 选择性催化还原 选择性 化学 氧化还原 X射线光电子能谱 无机化学 吸附 尖晶石 化学工程 材料科学 燃烧 冶金 物理化学 有机化学 工程类
作者
Yuanyuan Liu,Fengyu Gao,Songjin Ko,Chengzhi Wang,Hengheng Liu,Xiaolong Tang,Honghong Yi,Yuansong Zhou
出处
期刊:Chemical Engineering Journal [Elsevier BV]
卷期号:434: 134770-134770 被引量:59
标识
DOI:10.1016/j.cej.2022.134770
摘要

Improving the resistance to H2O is crucial to promote industrial applications of Mn-based catalysts for selective catalytic reduction of NOx by NH3 (NH3-SCR). In this work, we reported the CoMn2O4/TiO2 catalyst, and W was introduced as a promoter to enhance the resistance to H2O at low-temperature. CoMn2O4/W-TiO2 catalyst exhibited remarkable H2O-resistance of above 95% NOx conversion and nearly 100% N2 selectivity at 150–250 °C in the presence of 10 vol% H2O. Further, the role of tungsten and the effect of water on the structure and chemical properties of CoMn2O4/W-TiO2 catalyst were revealed by various techniques of BET, XRD, Raman, H2-TPR, NH3-TPD, XPS and in-situ DRIFTS experiments. The superior performance was attributed to unique spinel structure, mesoporous structure, highly dispersed tungsten species, greater surface acidity. The electron cycle among Mn, Co, W and Ti was beneficial to maintain the Mn3+/Mn4+ and Co3+ at high concentrations and enhance lattice oxygen mobility. The SCR reaction mainly followed the Eley-Rideal (E-R) mechanism over two catalysts, but the poor water resistance of CoMn2O4/TiO2 was attributed to the suppression of NH3 activation and E-R mechanism, despite NH3 adsorption was enhanced. Both Lewis and Brønsted acid sites were created by the incorporation of tungsten in the presence of H2O, and enhanced NH3 adsorption, promoting E-R reaction pathway. Besides, N2 selectivity was significantly enhanced by H2O, which could be due to a decrease in the redox activity of both catalysts. This study opens up a new avenue for designing efficient and environment-friendly NH3-SCR catalysts and looks promising for practical application.
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