Photocatalytic Methanol Dehydrogenation Promoted Synergistically by Atomically Dispersed Pd and Clustered Pd
Supported metal in the form of single atoms, clusters, and particles can individually or jointly affect the activity of supported heterogeneous catalysts. While the individual contribution of the supported metal to the overall activity of supported photocatalysts has been identified, the joint activity of mixed metal species is overlooked because of their different photoelectric properties. Here, atomically dispersed Pd (Pd<sub>1</sub>) and Pd clusters are loaded onto CdS, serving as oxidation and reduction sites for methanol dehydrogenation. The Pd<sub>1</sub> substitutes Cd<sup>2+</sup>, forming hole-trapping states for methanol oxidation and assisting the dispersion of photodeposited Pd clusters. Therefore, methanol dehydrogenation on CdS with supported Pd<sub>1</sub> and Pd clusters exhibits the highest turnover frequency of 1.14 s<sup>-1</sup> based on the Pd content and affords H<sub>2</sub> and HCHO with a similar apparent quantum yield of 87 ± 1% at 452 nm under optimized reaction conditions. This work highlights the synergistic catalysis of supported metal for improved photocatalytic activity.
Authors
- Junju Mu (ORCID: https://orcid.org/0000-0002-7382-2182)
- Nengchao Luo (ORCID: https://orcid.org/0000-0002-6137-292X)
- Tiziano Montini (ORCID: https://orcid.org/0000-0001-9515-566X)
- Feng Wang (ORCID: https://orcid.org/0000-0002-9167-8743)
- Paolo Fornasiero (ORCID: https://orcid.org/0000-0003-1082-9157)
- Emiliano Fonda (ORCID: https://orcid.org/0000-0001-6584-4587)
- Zhuyan Gao (ORCID: https://orcid.org/0000-0001-5965-3901)
Institutions
- University of Trieste (IT)
- Dalian Institute of Chemical Physics (CN)
- Chinese Academy of Sciences (CN)
- Synchrotron soleil (FR)
- Dalian National Laboratory for Clean Energy (CN)
- University of Chinese Academy of Sciences (CN)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2024-08-20
- DOI
- https://doi.org/10.1021/jacs.4c06573
- Citations
- 75
- Primary Topic
- Catalytic Processes in Materials Science
- Type
- article
- Field-Weighted Citation Impact
- 8.79
Funders
- Dalian High-Level Talent Innovation Program
- European Commission
- National Natural Science Foundation of China
- Chinese Academy of Sciences
- China Postdoctoral Science Foundation
- Youth Innovation Promotion Association of the Chinese Academy of Sciences
- National Key Research and Development Program of China
- Fundamental Research Funds for the Central Universities
- Youth Innovation Promotion Association
- High-end Foreign Experts Recruitment Plan of China
- HORIZON EUROPE Widening Participation and Strengthening the European Research Area
- HORIZON EUROPE European Innovation Council