尖晶石
催化作用
材料科学
锰
氧气
化学
选择性催化还原
纳米颗粒
氧化还原
无机化学
氧化态
活化能
选择性
冶金
纳米技术
物理化学
有机化学
生物化学
作者
Yu Qin,Shiying Fan,Xinyong Li,Guoqiang Gan,Liang Wang,Zhifan Yin,Xuecheng Guo,Moses O. Tadé,Shaomin Liu
出处
期刊:ACS applied nano materials
[American Chemical Society]
日期:2021-11-12
卷期号:4 (11): 11969-11979
被引量:32
标识
DOI:10.1021/acsanm.1c02546
摘要
Manganese–copper spinel is a kind of efficient catalyst for NO reduction by CO; however, its unsatisfactory low-temperature catalytic performance and poor N2 selectivity limit its application. Here, peanut-shaped Cu0.75Mn2.25O4 nano-hollow spinel (Cu0.75Mn2.25O4-NH) was prepared by a one-pot solvothermal method and applied in NO reduction by CO. The structure and physicochemical properties of catalysts were researched by comprehensive characterizations. Compared with Cu0.75Mn2.25O4 nanoparticles (Cu0.75Mn2.25O4-NP), Cu0.75Mn2.25O4-NH displayed excellent low-temperature catalytic performance, achieving 90% NO conversion at 200 °C, and possessed a lower apparent activation energy (36.4 kJ·mol–1). Importantly, the unique nanostructure with more exposed active sites enhanced the redox properties and oxygen mobility of the Cu0.75Mn2.25O4-NH catalyst. In addition, a synergistic effect between different metal ions in the Cu0.75Mn2.25O4-NH catalyst promoted the formation of oxygen vacancies and more low-oxidation-state species, which were conducive to the N–O bond scission at low temperatures. Combining the in situ DRIFTS results and DFT calculations, the dispersed species of Cuy+-O-Mnx+ could be reduced to the main reactive species of Cu(y–1)+-□-Mn(x–1)+. Moreover, the formation of oxygen vacancies optimized NO adsorption and activation ability, which improved the catalytic performance in NO reduction by CO.
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