期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 26, 期 18, 页码 4143-4149出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201904619
关键词
alloys; AuCu; carbon dioxide reduction; electrocatalysis; electrochemistry; nanoporous alloys; self-supported
资金
- National Natural Science Foundation of China [21771137, 21773288]
- Key Project of Natural Science Foundation of Tianjin [18JCZDJC97200]
- Training Project of Innovation Team of Colleges and Universities in Tianjin [TD13-5020]
The key to the electrochemical conversion of CO2 lies in the development of efficient electrocatalysts with ease of operation, good conductivity, and rich active sites that fulfil the desired reaction direction and selectivity. Herein, an oxidative etching of Au20Cu80 alloy is used for the synthesis of a nanoporous Au3Cu alloy, representing a facile strategy for tuning the surface electronic properties and altering the adsorption behavior of the intermediates. HRTEM, XPS, and EXAFS results reveal that the curved surface of the synthesized nanoporous Au3Cu is rich in gold with unsaturated coordination conditions. It can be used directly as a self-supported electrode for CO2 reduction, and exhibits high Faradaic efficiency (FE) of 98.12 % toward CO at a potential of -0.7 V versus the reversible hydrogen electrode (RHE). The FE is 1.47 times that over the as-made single nanoporous Au. Density functional theory reveals that *CO has a relatively long distance on the surface of nanoporous Au3Cu, making desorption of CO easier and avoiding CO poisoning. The Hirshfeld charge distribution shows that the Au atoms have a negative charge and the Cu atoms exhibit a positive charge, which separately bond to the C atom and O atom in the *COOH intermediate through a bidentate mode. This affords the lowest *COOH adsorption free energy and low desorption energy for CO molecules.
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