期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 24, 页码 13388-13393出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202101559
关键词
CO2 reduction reaction; dual-atom site catalyst; electron transfer; palladium; single-atom site catalysts
资金
- National Key R&D Program of China [2018YFA0702003]
- National Natural Science Foundation of China [21890383, 21871159]
- Science and Technology Key Project of Guangdong Province of China [2020B010188002]
- Beijing Municipal Science & Technology Commission [Z191100007219003]
- China Postdoctoral Science Foundation [2020M670355]
Dual-atom site catalysts (DACs) have shown significant potential in heterogeneous catalysis, with Pd-2 DAC demonstrating superior catalytic performance and stability in the electrochemical CO2 reduction reaction (CO2RR) due to electron transfer between dimeric Pd sites.
Dual-atom site catalysts (DACs) have emerged as a new frontier in heterogeneous catalysis because the synergistic effect between adjacent metal atoms can promote their catalytic activity while maintaining the advantages of single-atom site catalysts (SACs), like 100 % atomic utilization efficiency and excellent selectivity. Herein, a supported Pd-2 DAC was synthesized and used for electrochemical CO2 reduction reaction (CO2RR) for the first time. The as-obtained Pd-2 DAC exhibited superior CO2RR catalytic performance with 98.2 % CO faradic efficiency at -0.85 V vs. RHE, far exceeding that of Pd-1 SAC, and coupled with long-term stability. The density functional theory (DFT) calculations revealed that the intrinsic reason for the superior activity of Pd-2 DAC toward CO2RR was the electron transfer between Pd atoms at the dimeric Pd sites. Thus, Pd-2 DAC possessed moderate adsorption strength of CO*, which was beneficial for CO production in CO2RR.
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