Amorphous Sn(HPO4)2-derived phosphorus-modified Sn/SnOx core/shell catalyst for efficient CO2 electroreduction to formate

JOURNAL OF ENERGY CHEMISTRY(2023)

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摘要
Simultaneously achieving high activity, selectivity and stability for electrochemical CO2 reduction reac-tion (CO2RR) remains great challenges. Herein, a phosphorus-modified Sn/SnOx core/shell (P-Sn/SnOx) catalyst, derived from in situ electrochemical reduction of an amorphous Sn(HPO4)2 pre-catalyst, exhibits high CO2RR performance. The total Faradaic efficiency (FE) of C1 products is close to 100% in a broad potential range from-0.49 to-1.02 V vs. reversible hydrogen electrode, and a total current density of 315.0 mA cm-2 is achieved. Moreover, the P-Sn/SnOx catalyst maintains a formate FE of-90% for 120 h. Density functional theory calculations suggest that the phosphorus-modified Sn/SnOx core/shell structure effectively facilitates formate production by enhancing CO2 adsorption and improving free energy profile of formate formation. (c) 2022 SOCIETY. Published by ELSEVIERCOMPANY All rights reserved.
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关键词
CO2 electroreduction, Structural evolution, Reaction intermediate, Phosphorus modification, Stability
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