催化作用
尖晶石
钴
共沉淀
化学
分解
氧化物
一氧化二氮
氧气
密度泛函理论
热分解
化学工程
无机化学
材料科学
计算化学
有机化学
冶金
工程类
作者
Bingzhi Li,Xiaoxiao Duan,Ting Zhao,Ben Niu,Ganggang Li,Zeyu Zhao,Zhenwen Yang,Dongmei Liu,Fenglian Zhang,Jie Cheng,Zhengping Hao
标识
DOI:10.1021/acs.est.3c09741
摘要
Nitrous oxide (N2O) has a detrimental impact on the greenhouse effect, and its efficient catalytic decomposition at low temperatures remains challenging. Herein, the cobalt-based high-entropy oxide with a spinel-type structure (Co-HEO) is successfully fabricated via a facile coprecipitation method for N2O catalytic decomposition. The obtained Co-HEO catalyst displays more remarkable catalytic performance and higher thermal stability compared with single and binary Co-based oxides, as the temperature of 90% N2O decomposition (T90) is 356 °C. A series of characterization results reveal that the synergistic effect of multiple elements enhances the reducibility and augments oxygen vacancy in the high-entropy system, thus boosting the activity of the Co-HEO catalyst. Moreover, density functional theory (DFT) calculations and the temperature-programmed surface reaction (TPSR) with isotope labeling demonstrate that N2O decomposition on the Co-HEO catalyst follows the Langmuir–Hinshelwood (L-H) mechanism with the promotion of abundant oxygen vacancies. This work provides a fundamental understanding of the synergistic catalytic effect in N2O decomposition and paves the way for the novel environmental catalytic applications of HEO.
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