Cooperative Brønsted Acid-Single Atom Photocatalysis in Metal–Organic Framework
Enzymes, composed of earth-abundant elements, outperform conventional heterogeneous photocatalysts in hydrogen production due to the dual-site cooperation between adjacent active metal sites and proton-transferring ligands. However, the realization of such dual-site cooperation in heterogeneous catalytic systems is hindered by the challenges in the precise construction of cooperative active sites. In this study, we present the design of a structurally tuned metal-organic framework (MOF) photocatalyst that incorporates cooperative Brønsted acid-single atom catalytic sites. By grafting Co single-atom sites onto the Ti-oxo clusters and introducing Brønsted acidic P-OH moieties in tandem within the MOF-based catalyst structure, we achieved a visible-light-activated photocatalytic H<sub>2</sub> production rate of 6.6 mmol g<sup>-1</sup> h<sup>-1</sup>, which is 6.6 times higher than that of a Pt nanoparticle-based cocatalyst, emphasizing the significance of incorporating cooperative Brønsted acid-single atom catalytic sites.
Authors
- Jeongin Moon (ORCID: https://orcid.org/0000-0002-1190-8837)
- Jinsol Bok (ORCID: https://orcid.org/0000-0002-9003-1091)
- Jaeyune Ryu
- Chan Woo Lee (ORCID: https://orcid.org/0000-0002-9358-6893)
- Taeghwan Hyeon (ORCID: https://orcid.org/0000-0001-5959-6257)
- Wonjae Ko (ORCID: https://orcid.org/0000-0002-8806-6789)
- Megalamane S. Bootharaju (ORCID: https://orcid.org/0000-0002-8276-6987)
- Hyeon Seok Lee (ORCID: https://orcid.org/0000-0003-2605-2266)
- Minho Kim (ORCID: https://orcid.org/0000-0002-5886-2469)
- Jae Wook Lee (ORCID: https://orcid.org/0000-0002-8756-0195)
- Kangjae Lee (ORCID: https://orcid.org/0000-0002-2494-2372)
- Byoung‐Hoon Lee (ORCID: https://orcid.org/0000-0002-0482-2859)
- Yunjae Yu
- Yoon Jung (ORCID: https://orcid.org/0009-0006-2786-8602)
Institutions
- Seoul National University (KR)
- Korea University (KR)
- Kyung Hee University (KR)
- Institute for Basic Science (KR)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2024-12-31
- DOI
- https://doi.org/10.1021/jacs.4c13057
- Citations
- 25
- Primary Topic
- Advanced Photocatalysis Techniques
- Type
- article
- Field-Weighted Citation Impact
- 2.56
Funders
- National Research Foundation of Korea
- Institute for Basic Science