催化作用
材料科学
钴
密度泛函理论
尖晶石
空位缺陷
锰
选择性催化还原
解吸
选择性
化学工程
无机化学
傅里叶变换红外光谱
物理化学
化学
吸附
计算化学
结晶学
有机化学
冶金
工程类
作者
Yu Qin,Shiying Fan,Jinsuo Gao,Moses O. Tadé,Shaomin Liu,Xinyong Li
标识
DOI:10.1021/acsami.2c23120
摘要
Cobalt-manganese spinel catalysts performed unsatisfactory activity at low-temperature and narrow reaction temperature window, which greatly limited the application in NO reduction by CO. Herein, we synthesize a series of Cu-doped CoMn2O4 catalysts and apply to NO reduction by CO. The Cu0.3Co0.7Mn2O4 exhibited superior catalytic performance, reaching 100% NO conversion and 80% N2 selectivity at 250 °C. Detailed structural analysis showed that the introduced Cu replaces some Co in tetrahedral coordination to induce a strong synergistic effect between different metals. This endows the catalyst with the promotion of both electron transfer and oxygen vacancy generation on the catalyst surface. Importantly, the reaction mechanism and pathway were further revealed by in situ diffusion Fourier transform infrared spectroscopy (DRIFTS) and density functional theory (DFT) calculations. The results indicated that the cycle of oxygen vacancy mainly determines the catalytic activity of NO reduction by CO. Notably, Cu doping significantly lowered the energy barrier of the rate-determining step (*CO + O → *Ov + CO2), facilitating the desorption of the CO2 and exposing the active sites for efficient NO reduction with CO. This work offers an effective way for designing the catalyst in NO reduction by CO and provides a reference for exploring the catalytic mechanism of the reaction.
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