Enhancing Electron Donor–Acceptor Complex Photoactivation with a Stable Perylene Diimide Metal–Organic Framework
Electron donor-acceptor complexes are commonly employed to facilitate photoinduced radical-mediated organic reactions. However, achieving these photochemical processes with catalytic amounts of donors or acceptors can be challenging, especially when aiming to reduce catalyst loadings. Herein, we have unveiled a framework-based heterogenization approach that significantly enhances the photoredox activity of perylene diimide species in radical addition reactions with alkyl silicates by promoting faster and more efficient electron donor-acceptor complex formation. Besides offering broad substrate scope in alkene hydroalkylation, the newly developed heterogeneous photocatalysis substantially improves the catalyst turnover numbers in comparison to previous homogeneous photocatalytic systems and demonstrates outstanding catalyst recyclability. These research findings pave the way for the advancement of various efficient and practical organic transformations using framework-supported organocatalysts.
Authors
- Xiao Xiong (ORCID: https://orcid.org/0000-0002-0433-0328)
- Dongyi Liu (ORCID: https://orcid.org/0000-0002-7990-5018)
- Kun Wu (ORCID: https://orcid.org/0000-0002-2357-3288)
- Jun Guo (ORCID: https://orcid.org/0000-0003-4170-2853)
- Tianyu Liu (ORCID: https://orcid.org/0000-0002-0093-8993)
- Ming Cui (ORCID: https://orcid.org/0000-0002-0755-0123)
- Ri‐Qin Xia (ORCID: https://orcid.org/0000-0003-2962-2113)
- Puxin Weng (ORCID: https://orcid.org/0000-0003-1819-2090)
- Yong‐Liang Huang (ORCID: https://orcid.org/0000-0003-1569-014X)
- Jian Feng He (ORCID: https://orcid.org/0000-0002-3388-3239)
- Dan Li (ORCID: https://orcid.org/0000-0002-4936-4599)
- Zekun Li (ORCID: https://orcid.org/0000-0002-7976-039X)
- Xia Wu (ORCID: https://orcid.org/0000-0002-1496-8800)
Institutions
- Jinan University (CN)
- Shantou University (CN)
- Key Laboratory of Guangdong Province (CN)
- Shantou University Medical College (CN)
- State Key Laboratory of Synthetic Chemistry (CN)
- University of Hong Kong (HK)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2025-01-27
- DOI
- https://doi.org/10.1021/jacs.4c16021
- Citations
- 16
- Primary Topic
- Metal-Organic Frameworks: Synthesis and Applications
- Type
- article
- Field-Weighted Citation Impact
- 8.60
Funders
- Croucher Foundation
- National Natural Science Foundation of China
- Innovation and Technology Commission
- University of Hong Kong