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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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Published in: | Advanced functional materials 2023-04, Vol.33 (16) |
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Main Authors: | , , , , , |
Format: | Article |
Language: | English |
Citations: | Items that this one cites Items that cite this one |
Online Access: | Get full text |
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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. |
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ISSN: | 1616-301X 1616-3028 |
DOI: | 10.1002/adfm.202214215 |