期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 26, 页码 14563-14570出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202102887
关键词
cluster compounds; CO2 reduction; heterogeneous catalysis; reaction mechanism; S ligands
资金
- Carbon-to-X Project through the National Research Foundation (NRF) of Korea -Ministry of Science and ICT, Republic of Korea [2020M3H7A1096344, 2021M3H7A1026177]
- NRF grant [NRF-2017R1A2B3006651]
- Korea Electric Power Corporation [R20XO02-23]
This study successfully identified active sites using gold nanoclusters as model catalysts in the electrochemical CO2 reduction reaction. The research showed that dethiolated Au sites are the active sites, and the CO2RR activity is determined by the number of active sites on the cluster surface.
Accurate identification of active sites is critical for elucidating catalytic reaction mechanisms and developing highly efficient and selective electrocatalysts. Herein, we report the atomic-level identification of active sites using atomically well-defined gold nanoclusters (Au NCs) Au-25, Au-38, and Au-144 as model catalysts in the electrochemical CO2 reduction reaction (CO2RR). The studied Au NCs exhibited remarkably high CO2RR activity, which increased with increasing NC size. Electrochemical and X-ray photoelectron spectroscopy analyses revealed that the Au NCs were activated by removing one thiolate group from each staple motif at the beginning of CO2RR. In addition, density functional theory calculations revealed higher charge densities and upshifts of d-states for dethiolated Au sites. The structure-activity properties of the studied Au NCs confirmed that dethiolated Au sites were the active sites and that CO2RR activity was determined by the number of active sites on the cluster surface.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据