An, Xiaoqiang;
Wei, Tingcha;
Ding, Peijia;
Liu, Li-Min;
Xiong, Lunqiao;
Tang, Junwang;
Ma, Jiani;
... Qu, Jiuhui; + view all
(2023)
Sodium-Directed Photon-Induced Assembly Strategy for Preparing Multisite Catalysts with High Atomic Utilization Efficiency.
Journal of the American Chemical Society
, 145
(3)
pp. 1759-1768.
10.1021/jacs.2c10690.
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Abstract
Integrating different reaction sites offers new prospects to address the difficulties in single-atom catalysis, but the precise regulation of active sites at the atomic level remains challenging. Here, we demonstrate a sodium-directed photon-induced assembly (SPA) strategy for boosting the atomic utilization efficiency of single-atom catalysts (SACs) by constructing multifarious Au sites on TiO2 substrate. Na+ was employed as the crucial cement to direct Au single atoms onto TiO2, while the light-induced electron transfer from excited TiO2 to Au(Na+) ensembles contributed to the self-assembly formation of Au nanoclusters. The synergism between plasmonic near-field and Schottky junction enabled the cascade electron transfer for charge separation, which was further enhanced by oxygen vacancies in TiO2. Our dual-site photocatalysts exhibited a nearly 2 orders of magnitude improvement in the hydrogen evolution activity under simulated solar light, with a striking turnover frequency (TOF) value of 1533 h-1 that exceeded other Au/TiO2-based photocatalysts reported. Our SPA strategy can be easily extended to prepare a wide range of metal-coupled nanostructures with enhanced performance for diverse catalytic reactions. Thus, this study provides a well-defined platform to extend the boundaries of SACs for multisite catalysis through harnessing metal-support interactions.
| Type: | Article |
|---|---|
| Title: | Sodium-Directed Photon-Induced Assembly Strategy for Preparing Multisite Catalysts with High Atomic Utilization Efficiency |
| Location: | United States |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/jacs.2c10690 |
| Publisher version: | https://doi.org/10.1021/jacs.2c10690 |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | Bottom-up assembly; single-atom catalysts; atomic utilization efficiency; water splitting; metal-support interactions |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering |
| URI: | https://discovery-pp.ucl.ac.uk/id/eprint/10164362 |
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