Effect of Cu-Doped Co-Mn Spinel for Boosting Low-Temperature NO Reduction by CO: Exploring the Structural Properties, Performance, and Mechanisms.

ACS applied materials & interfaces(2023)

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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 CoMnO catalysts and apply to NO reduction by CO. The CuCoMnO exhibited superior catalytic performance, reaching 100% NO conversion and 80% N 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 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 → *O + CO), facilitating the desorption of the CO 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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关键词
Cu-doped CoMn2O4 spinel,DFT calculations,NO reduction by CO,cycle of oxygen vacancy,synergistic effect
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