We found a match
Your institution may have access to this item. Find your institution then sign in to continue.
- Title
Atomically Dispersed Gold Nanoclusters and Single Atoms Coexisting Chiral Electrode for High‐Performance Enantioselective Electrosynthesis using H<sub>2</sub>o as Hydrogen Source.
- Authors
Chang, Wen; Qi, Bo; Wang, Ruoyu; Liu, Huijie; Chen, Guangbo; Hu, Guicong; Li, Zixian; Sun, Jie; Peng, Yung‐Kang; Li, Guangchao; Kong, Xianggui; Song, Yu‐Fei; Zhao, Yufei
- 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.
- Subjects
ELECTROSYNTHESIS; GOLD clusters; HYDROGENATION; ATOMS; ELECTRODES; CATALYTIC activity; DENSITY functional theory; CARBONYL group
- Publication
Advanced Functional Materials, 2024, Vol 34, Issue 28, p1
- ISSN
1616-301X
- Publication type
Article
- DOI
10.1002/adfm.202315675