期刊
SCIENCE BULLETIN
卷 67, 期 14, 页码 1477-1485出版社
ELSEVIER
DOI: 10.1016/j.scib.2022.06.006
关键词
Sulfur regulation; Nickel clusters; Fully exposed metal sites; Carbon dioxide reduction reaction; Industrial current density
资金
- Alexander von Humboldt Foundation (Germany)
- National Key R&D Program of China [2020YFB1505603]
- National Natural Science Foundation of China [51925102]
- Key Research Program of the Chinese Academy of Sciences [ZDRW-CN-2021-3]
- Youth Innovation Promotion Association CAS [E1202002]
A facile method was developed to regulate the atomic dispersion of Ni species for efficient CO2 reduction. The obtained Ni catalyst exhibited excellent performance in electrocatalytic reactions, with high Faradaic efficiency and current density, as well as good stability.
Single-atom catalysts (SACs) have attracted increasing concerns in electrocatalysis because of their max-imal metal atom utilization, distinctive electronic properties, and catalytic performance. However, the isolated single sites are disadvantageous for reactions that require simultaneously activating different reactants/intermediates. Fully exposed metal cluster catalyst (FECC), inheriting the merits of SACs and metallic nanoparticles, can synergistically adsorb and activate reactants/intermediates on their multi -atomic sites, demonstrating great promise in electrocatalytic reactions. Here a facile method to regulate the atomic dispersion of Ni species from cluster to single-atom scale for efficient CO2 reduction was developed. The obtained Ni FECC exhibits high Faradaic efficiency of CO up to 99%, high CO partial current density of 347.2 mA cm(-2), and robust durability under 20 h electrolysis. Theoretical calculations illumi-nate that the ensemble of multiple Ni atoms regulated by sulfur atoms accelerates the reaction kinetics and thus improves CO production. (C) 2022 Science China Press. Published by Elsevier B.V. and Science China Press. All rights reserved.
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