Engineering Synergistic Sites in a Cerium-Based Metal–Organic Framework for Photocatalytic CO2 Reduction
Abstract Photoreduction of CO2 to produce solar fuels is an important target. Redox-active Ce-based metal–organic frameworks (MOFs) are promising catalysts. Herein, we have synthesized an amino-functionalized Ce-based MOF, PKU-167 (PKU = Peking University). Upon introduction of Co(bpy)2Cl2 (bpy = 2,2′-bipyridine) to the skeleton of PKU-167, PKU-167-0.9Co achieved a high CO production rate of 18.4 mmol g–1 h–1 with a selectivity of 91.8% under visible-light irradiation and an apparent quantum yield of 1.97% at 425 nm. In situ characterizations and modeling reveal a synergistic adsorption–reduction mechanism, where amino groups enrich adsorption of CO2 for subsequent photoreduction on {Ce6} clusters and Co2+ sites in concert to achieve the optimal photocatalytic performance. This study will advance the rational design of redox-active Ce-based MOFs as efficient photocatalysts.
Authors
- Sarah J. Day (ORCID: https://orcid.org/0000-0003-1059-8475)
- Mark D. Frogley (ORCID: https://orcid.org/0000-0002-0742-5007)
- Luke L. Keenan (ORCID: https://orcid.org/0000-0001-9892-7864)
- Sihai Yang⧫ (ORCID: https://orcid.org/0000-0002-1111-9272)
- Xin Lian (ORCID: https://orcid.org/0009-0007-4504-5236)
- Siyu Zhou (ORCID: https://orcid.org/0000-0002-2427-6242)
- Tian Luo (ORCID: https://orcid.org/0000-0002-5788-5060)
- Xue Han (ORCID: https://orcid.org/0000-0002-0390-422X)
- B. Moore (ORCID: https://orcid.org/0009-0009-4227-170X)
- Jiarui Fan (ORCID: https://orcid.org/0009-0009-8504-3643)
- Lifei Lin
- Zhaozhao Hu
- Zhixin Wang
- Yuanjun Wang
- Yukun Ye
- Ruohan Li
- Jiangnan Li
Institutions
- Peking University (CN)
- Beijing Normal University (CN)
- Diamond Light Source (GB)
- University of Manchester (GB)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2026-11-03
- DOI
- https://doi.org/10.1021/jacs.6c16747
- Primary Topic
- Advanced Photocatalysis Techniques
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- Diamond Light Source
- National Natural Science Foundation of China
- Ministry of Education of the People's Republic of China
- China Postdoctoral Science Foundation
- Beijing Nova Program
- Beijing National Laboratory for Molecular Sciences