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

Author:

Chang Wen1,Qi Bo1,Wang Ruoyu1,Liu Huijie1,Chen Guangbo2,Hu Guicong1,Li Zixian1,Sun Jie1,Peng Yung‐Kang3,Li Guangchao4,Kong Xianggui15,Song Yu‐Fei16,Zhao Yufei156ORCID

Affiliation:

1. State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology Beijing 100029 P. R. China

2. Center for Advancing Electronics Dresden (Cfaed) and Faculty of Chemistry and Food Chemistry Technische Universita¨t Dresden 01062 Dresden Germany

3. Department of Chemistry City University of Hong Kong Hong Kong Hong Kong SAR 999077 P. R. China

4. Department of Applied Physics The Hong Kong Polytechnic University Hong Kong 999077 P. R. China

5. Qingyuan Innovation Laboratory Quanzhou Fujian 362801 P. R. China

6. Quzhou Institute for Innovation in Resource Chemical Engineering Quzhou Zhejiang 324000 P. R. China

Abstract

AbstractDeveloping 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.

Funder

National Natural Science Foundation of China

National Key Research and Development Program of China

Fundamental Research Funds for the Central Universities

Publisher

Wiley

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