Oxygen vacancies promote the activation of O2 in transition metal oxide doped ε-MnO2 for low-temperature CO oxidation

Zilei Zhang, Dongxiang Zhang*, Dagang Li, Linfeng He, Zhiren Guo, Guma Yeli, Xu Zhang, Bing Liu, Haocun Tan, Fengqi Zhang, Xiaotong Chen*, Jinying Li, Xiyan Xu

*此作品的通讯作者

科研成果: 期刊稿件文章同行评审

2 引用 (Scopus)

摘要

Carbon monoxide (CO), a toxic pollutant usually formed from incomprehensive combustion especially at low temperature, has harmful effects on human health. Therefore, the catalytic oxidation of CO always receives widespread attention. Herein, we reported transition metal (Cu, Co, Ni, Fe) doped ε-MnO2 as CO catalysts using a hydrothermal-deposition method. Physiochemical properties for CO oxidation were meticulously analyzed employing characterization techniques such as SEM, XRD, BET, XPS, EPR, CO-TPR. The doped ε-MnO2 catalyst showed expanded BET surface area, increased oxygen vacancy defects, more active sites, enhanced adsorption, and faster electron transfer. Catalytic activity tests indicated that the ε-MnO2 catalyst doped with transition metals exhibited exceptionally high catalytic activity, with the Cu-doped catalyst showing the fastest chemical reaction rate and the lowest complete conversion reaction temperature (TOF of 9.92 × 10−3 s−1, at 65℃). Density Functional Theory (DFT) calculations indicated that Cu doping more effectively induced oxygen vacancy defects compared to Co, Ni, Fe, and raw ε-MnO2 catalysts. It identifies the CO oxidation reaction and improved the CO adsorption capacity of the catalyst. Furthermore, a novel potential reaction pathway for the M-vK mechanism in transition metal oxides was proposed.

源语言英语
文章编号128109
期刊Separation and Purification Technology
352
DOI
出版状态已出版 - 1 1月 2025

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Zhang, Z., Zhang, D., Li, D., He, L., Guo, Z., Yeli, G., Zhang, X., Liu, B., Tan, H., Zhang, F., Chen, X., Li, J., & Xu, X. (2025). Oxygen vacancies promote the activation of O2 in transition metal oxide doped ε-MnO2 for low-temperature CO oxidation. Separation and Purification Technology, 352, 文章 128109. https://doi.org/10.1016/j.seppur.2024.128109