Affiliation:
1. College of Chemistry State Key Laboratory of Elemento‐Organic Chemistry Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Nankai University Tianjin 300071 P. R. China
2. Key Laboratory of 3D Micro/Nano Fabrication and Characterization of Zhejiang Province School of Engineering Westlake University Hangzhou Zhejiang Province 310024 P. R. China
Abstract
AbstractReverse water‐gas shift (RWGS) reaction is the initial and necessary step of CO2 hydrogenation to high value‐added products, and regulating the selectivity of CO is still a fundamental challenge. In the present study, an efficient catalyst (CuZnNx@C‐N) composed by Zn single atoms and Cu clusters stabilized by nitrogen sites is reported. It contains saturated four‐coordinate Zn‐N4 sites and low valence CuNx clusters. Monodisperse Zn induces the aggregation of pyridinic N to form Zn‐N4 and N4 structures, which show strong Lewis basicity and has strong adsorption for *CO2 and *COOH intermediates, but weak adsorption for *CO, thus greatly improves the CO2 conversion and CO selectivity. The catalyst calcined at 700 °C exhibits the highest CO2 conversion of 43.6% under atmospheric pressure, which is 18.33 times of Cu‐ZnO and close to the thermodynamic equilibrium conversion rate (49.9%) of CO2. In the catalytic process, CuNx not only adsorbs and activates H2, but also cooperates with the adjacent Zn‐N4 and N4 structures to jointly activate CO2 molecules and further promotes the hydrogenation of CO2. This synergistic mechanism will provide new insights for developing efficient hydrogenation catalysts.
Funder
National Natural Science Foundation of China
Natural Science Foundation of Tianjin City
Subject
Electrochemistry,Condensed Matter Physics,Biomaterials,Electronic, Optical and Magnetic Materials
Cited by
20 articles.
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