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Hybrid Catalyst Coupling Zn Single Atoms and CuN x Clusters for Synergetic Catalytic Reduction of CO 2

Reverse water‐gas shift (RWGS) reaction is the initial and necessary step of CO 2 hydrogenation to high value‐added products, and regulating the selectivity of CO is still a fundamental challenge. In the present study, an efficient catalyst (CuZnN x @C‐N) composed by Zn single atoms and Cu clusters...

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Bibliographic Details
Published in:Advanced functional materials 2023-04, Vol.33 (16)
Main Authors: Hu, Xiaosong, Liu, Xinyu, Hu, Xin, Zhao, Chaoyue, Guan, Qingxin, Li, Wei
Format: Article
Language:English
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Summary:Reverse water‐gas shift (RWGS) reaction is the initial and necessary step of CO 2 hydrogenation to high value‐added products, and regulating the selectivity of CO is still a fundamental challenge. In the present study, an efficient catalyst (CuZnN x @C‐N) composed by Zn single atoms and Cu clusters stabilized by nitrogen sites is reported. It contains saturated four‐coordinate Zn‐N 4 sites and low valence CuN x clusters. Monodisperse Zn induces the aggregation of pyridinic N to form Zn‐N 4 and N 4 structures, which show strong Lewis basicity and has strong adsorption for *CO 2 and *COOH intermediates, but weak adsorption for *CO, thus greatly improves the CO 2 conversion and CO selectivity. The catalyst calcined at 700 °C exhibits the highest CO 2 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 CO 2 . In the catalytic process, CuN x not only adsorbs and activates H 2 , but also cooperates with the adjacent Zn‐N 4 and N 4 structures to jointly activate CO 2 molecules and further promotes the hydrogenation of CO 2 . This synergistic mechanism will provide new insights for developing efficient hydrogenation catalysts.
ISSN:1616-301X
1616-3028
DOI:10.1002/adfm.202214215