Atomically Precise Gold Nanoclusters as Model Catalysts for Identifying Active Sites for Electroreduction of CO2

Hoeun Seong, Vladimir Efremov, Gibeom Park, Hyunwoo Kim, Jong Suk Yoo, Dongil Lee

Research output: Contribution to journalArticlepeer-review

3 Citations (Scopus)

Abstract

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) Au25, Au38, and Au144 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.

Original languageEnglish
Pages (from-to)14563-14570
Number of pages8
JournalAngewandte Chemie - International Edition
Volume60
Issue number26
DOIs
Publication statusPublished - 2021 Jun 21

Bibliographical note

Funding Information:
This work was supported by the Carbon‐to‐X Project (No. 2020M3H7A1096344 and 2021M3H7A1026177) through the National Research Foundation (NRF) of Korea funded by the Ministry of Science and ICT, Republic of Korea, the NRF grant (NRF‐2017R1A2B3006651), and the Korea Electric Power Corporation (grant No. R20XO02‐23). The DFT calculations were performed using the computational resources in the Korea Institute of Science and Technology Information (KSC‐2021‐CRE‐0101).

Funding Information:
This work was supported by the Carbon-to-X Project (No. 2020M3H7A1096344 and 2021M3H7A1026177) through the National Research Foundation (NRF) of Korea funded by the Ministry of Science and ICT, Republic of Korea, the NRF grant (NRF-2017R1A2B3006651), and the Korea Electric Power Corporation (grant No. R20XO02-23). The DFT calculations were performed using the computational resources in the Korea Institute of Science and Technology Information (KSC-2021-CRE-0101).

Publisher Copyright:
© 2021 Wiley-VCH GmbH

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)

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