Tracking charge dynamics in a silver single-atom catalyst during the light-driven oxidation of benzyl alcohol to benzaldehyde
Author(s)
Type
Journal Article
Abstract
Understanding charge transfer in light-driven processes is crucial for optimizing the efficiency and performance of a photocatalyst, as charge transfer directly influences the separation and migration of photogenerated charge carriers and determines the overall reaction rate and product formation. However, achieving this understanding remains challenging in the context of single-atom photocatalysis. This study addresses this gap and investigates an Ag-based single-atom catalyst (Ag1@CN x ) in the photocatalytic oxidation of benzyl alcohol to benzaldehyde. Comprehensive characterization was conducted using a battery of diffractive, textural, spectroscopic, and microscopic methods, confirming the catalyst crystallinity, porosity, elemental composition, and atomic dispersion of silver atoms. This material displayed efficient performance in the selective oxidation of benzyl alcohol to benzaldehyde. Density functional theory calculations were used to rationalize the catalyst structure and elucidate the reaction mechanism, unveiling the role of the photogenerated holes in lowering the reaction energy barriers. Time-resolved transient spectroscopic studies were used to monitor the dynamics of photogenerated charges in the reaction, revealing the lifetimes and behaviors of excited states within the catalyst. Specifically, the introduction of silver atoms led to a significant enhancement in the excited state lifetime, which favors the hole-transfer in the presence of the benzyl alcohol. This indicated that the photoexcited carriers were effectively transferred to the reactant, thereby driving the oxidation process in the presence of oxygen. These mechanistic insights are pivotal in spectroscopically elucidating the reaction mechanism and can be practically applied to design single-atom photocatalysts more rationally, targeting materials that combine both rapid reductive quenching and efficient charge transfer to the metal.
Date Issued
2025-04-04
Date Acceptance
2025-01-29
Citation
ACS Catalysis, 2025, 15 (7), pp.5601-5613
ISSN
2155-5435
Publisher
American Chemical Society
Start Page
5601
End Page
5613
Journal / Book Title
ACS Catalysis
Volume
15
Issue
7
Copyright Statement
© 2025 The Authors. Published by American Chemical Society. This publication is licensed under CC-BY 4.0 .
License URL
Identifier
https://www.ncbi.nlm.nih.gov/pubmed/40207072
Publication Status
Published
Coverage Spatial
United States
Date Publish Online
2025-03-21