化工学报2025，Vol.76Issue(11)：5604-5616,13.DOI:10.11949/0438-1157.20250482
Mn/Ce共掺杂强化氧物种转化与稀薄甲烷催化燃烧机制研究
Mechanistic study of Mn/Ce co-doping for enhanced oxygen species conversion and catalytic combustion of dilute methane
摘要
Abstract
In this study,a series of Cu-based monolithic catalysts with different Mn/Ce doping ratios were synthesized and used for catalytic combustion activity testing of dilute methane.Among them,the 4Cu-3Mn-1Ce catalyst exhibited the best methane catalytic activity with a conversion of 85.0％at 550℃ and achieved complete conversion at 600℃.The mechanism of the effect of Mn/Ce doping on the physicochemical properties of Cu-based monolithic catalysts was investigated by characterization analysis,including in situ Fourier Transform infrared spectroscopy(in situ FTIR),and density functional theory(DFT)simulation calculations.The enhanced methane catalytic combustion activity of the Cu-based monolithic catalysts can be attributed to the following:Ce doping forming a Ce-Cu solid solution,weakening the Cu-O bond,and promoting lattice oxygen diffusion at high temperatures,thus enhancing high-temperature catalytic activity;and Mn doping promotes the adsorption of O2 on the catalysts,which strengthens methane oxidation at low temperatures;Mn/Ce co-doping strengthens the activation of O2 and its dissociation to *O,which fills the oxygen vacancies and regenerates into lattice oxygen,the co-doping strengthens the cycle of oxygen species and thus significantly improves the catalytic combustion activity of thin and dilute methane.关键词
催化/甲烷/活化/燃烧/掺杂Key words
catalysis/methane/activation/combustion/doping分类
化学化工引用本文复制引用
邱家齐,杨仲卿,张志刚,甘海龙,霍春秀,窦志帅,冉景煜..Mn/Ce共掺杂强化氧物种转化与稀薄甲烷催化燃烧机制研究[J].化工学报,2025,76(11):5604-5616,13.基金项目
国家自然科学基金项目(52276099) （52276099）
中煤科工集团科技计划项目(2024-TD-ZD020) （2024-TD-ZD020）
中煤科工集团重庆研究院有限公司自立项目(2024ZDYF19) （2024ZDYF19）
