无机材料学报2026,Vol.41Issue(1):87-95,中插8-中插10,12.DOI:10.15541/jim20250044
CeO2对MnOx催化剂低温脱硝性能的影响及其机理研究
Effect of CeO2 on Low-temperature Denitrification Performance of MnOx Catalysts and Its Mechanism
摘要
Abstract
Nitrogen oxides(NOx),as main atmospheric pollutants in China,are usually removed through ammonia selective catalytic reduction(NH3-SCR)technology to achieve ultra-low emissions.Low-temperature NH3-SCR has gained much attention due to its low energy consumption and cost.However,MnOx-based catalysts generally suffer from insufficient stability and are susceptible to SO2 and H2O poisoning at 120℃.To improve the denitrification performance of MnOx-based catalysts under low temperature and lean flue gas conditions,CeO2/MnOx catalysts were prepared by precipitation-calcination decomposition method in this study.Influence of CeO2 modification on structure,surface properties and low-temperature NH3-SCR performance of catalyst was systematically studied.Combining first principles calculations,influence of CeO2 modification on catalytic mechanism for reducing activation energy of the reaction was revealed at microscopic level.The results showed that addition of CeO2 refined micro particle size of catalyst,reduced proportion of main crystalline phase MnO2,significantly increased concentration of weak acid sites in the catalyst,augmented proportion of Mn3+/Mn and Oα/O,and improved surface acidity and redox performance of the catalyst.The prepared Mn10Ce3 and Mn10Ce5 catalysts achieved a NO conversion rate of over 98%,maintaining stability even at 120℃.Addition of CeO2 dispersed the aggregated MnOx and reduced concentration of Mn4+distribution,which to some extent hindered excessive oxidation of NH3 and NO by high valence Mn4+,thereby suppressing N2O formation and improving N2 selectivity of the catalyst.First principles calculations further confirmed that CeO2 modification reduced the activation energy of various intermediate states in reaction pathway,lowering the reaction temperature and improving the low-temperature NH3-SCR efficiency.关键词
低温氨气选择性催化还原/CeO2/MnOx催化剂/反应机理Key words
low-temperature ammonia selective catalytic reduction/CeO2/MnOx catalyst/reaction mechanism分类
资源环境引用本文复制引用
邬博宇,张深根,张生杨,刘波,张柏林..CeO2对MnOx催化剂低温脱硝性能的影响及其机理研究[J].无机材料学报,2026,41(1):87-95,中插8-中插10,12.基金项目
国家自然科学基金(52204414) (52204414)
国家节能低碳材料生产应用示范平台项目(TC220H06N)National Natural Science Foundation of China(52204414) (TC220H06N)
Low-Carbon Materials Production and Application Demonstration Platform Program(TC220H06N) (TC220H06N)