Promoting CO2-to-CO Electroreduction via the Active-Site Engineering of Atomically Precise Silver Nanoclusters

Hoeun Seong, Minji Choi, Sojung Park, Hyun Woo Kim, Jiyoung Kim, Wooyul Kim, Jong Suk Yoo, Dongil Lee

Research output: Contribution to journalArticlepeer-review

22 Scopus citations

Abstract

Atomically precise metal nanoclusters (NCs) are promising catalysts for the electrochemical CO2reduction reaction (CO2RR) and are effective model catalysts for the identification of active sites. We report the metal-dependent CO2RR activities of Au25(SR)18and Ag25(SR)18(SR = thiolate). While both NCs produced CO as a main CO2RR product, the Au25NC exhibited a significantly higher CO2RR activity than the Ag25NC. Theoretical and operando studies revealed that the CO2RR limiting potential for the Au25NC was significantly smaller than that for the Ag25NC, while both NCs contained the partially dethiolated metal sites as the active sites. Active-site engineering was performed by replacing the Ag12(SR)18shell of the Ag25(SR)18NC with the Au12(SR)18shell to generate a core-shell AuAg12@Au12(SR)18NC, which exhibited dramatically enhanced CO2RR activity compared with the Ag25(SR)18NC. The AuAg12@Au12NCs exhibited stable CO2-to-CO electroreduction at a commercially relevant current density of 200 mA/cm2and a full-cell potential of 2.1 V in a zero-gap CO2electrolyzer.

Original languageEnglish
Pages (from-to)4177-4184
Number of pages8
JournalACS Energy Letters
Volume7
Issue number12
DOIs
StatePublished - 9 Dec 2022

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