Atomically Dispersed Gold Nanoclusters and Single Atoms Coexisting Chiral Electrode for High-Performance Enantioselective Electrosynthesis using H2o as Hydrogen Source

Wen Chang, Bo Qi*, Ruoyu Wang, Huijie Liu, Guangbo Chen, Guicong Hu, Zixian Li, Jie Sun, Yung-Kang Peng, Guangchao Li, Xianggui Kong, Yu-Fei Song*, Yufei Zhao*

*Corresponding author for this work

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

3 Citations (Scopus)

Abstract

Developing chiral electrode catalysts for enantioselective electrosynthesis is a great challenge, as it requires catalysts that possess both high activity and enantioselectivity. Precise synthesis of nanoclusters and single atoms coexisting chiral catalysts provide a promising pathway for enhancing asymmetric catalytic performance. Herein, chiral electrode catalysts are fabricated comprising gold clusters (R-AuC) and single atoms (R-AuS) on graphene oxide (R-AuC/S@GO) through an assembly-irradiation strategy. Thereinto, the R-Aus is in situ generated from R-AuC under light irradiation. The monoatomization process can be precisely regulated by changing the wavelength of the light, resulting in four Au-based chiral electrode (R-Au@GO) catalysts with different ratios of nanoclusters and single atoms. These chiral electrodes are applied in the electrocatalytic enantioselective hydrogenation of methyl benzoylformate (MB) to chiral methyl mandelate (S-MM), and the R-AuC/S-2@GO with ≈26% R-AuC and 74% R-AuS achieve the highest catalytic activity (35 µmol cm−2 h−1 productivity) and enantioselectivity [97% enantiomeric excess (ee)]. Detailed experimental analysis and density functional theory calculations reveal that the R-AuS on GO promotes the in situ generation of H* species, and R-AuC mainly drives the enantioselective conversion of MB by transferring the H* species to the carbonyl group of MB, ultimately yielding chiral S-MM. © 2024 Wiley-VCH GmbH.
Original languageEnglish
Article number2315675
JournalAdvanced Functional Materials
Volume34
Issue number28
Online published28 Jan 2024
DOIs
Publication statusPublished - 10 Jul 2024

Research Keywords

  • chiral electrode
  • heterogeneous catalysis
  • heterogeneous enantioselective electrosynthesis asymmetric catalysis
  • nanoclusters
  • single atoms

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