Metal-organic framework boosts heterogeneous electron donor–acceptor catalysis

Jiaxin Lin, Jing Ouyang, Tianyu Liu, Fengxing Li, Herman Ho-Yung Sung, Ian Williams and Yangjian Quan ()
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Jiaxin Lin: The Hong Kong University of Science and Technology (HKUST)
Jing Ouyang: The Hong Kong University of Science and Technology (HKUST)
Tianyu Liu: The Hong Kong University of Science and Technology (HKUST)
Fengxing Li: The Hong Kong University of Science and Technology (HKUST)
Herman Ho-Yung Sung: The Hong Kong University of Science and Technology (HKUST)
Ian Williams: The Hong Kong University of Science and Technology (HKUST)
Yangjian Quan: The Hong Kong University of Science and Technology (HKUST)

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Metal-organic framework (MOF) is a class of porous materials providing an excellent platform for engineering heterogeneous catalysis. We herein report the design of MOF Zr-PZDB consisting of Zr6-clusters and PZDB (PZDB = 4,4’-(phenazine-5,10-diyl)dibenzoate) linkers, which served as the heterogeneous donor catalyst for enhanced electron donor–acceptor (EDA) photoactivation. The high local concentration of dihydrophenazine active centers in Zr-PZDB can promote the EDA interaction, therefore resulting in superior catalytic performance over homogeneous counterparts. The crowded environment of Zr-PZDB can protect the dihydrophenazine active center from being attacked by radical species. Zr-PZDB efficiently catalyzes the Minisci-type reaction of N-heterocycles with a series of C-H coupling partners, including ethers, alcohols, non-activated alkanes, amides, and aldehydes. Zr-PZDB also enables the coupling reaction of aryl sulfonium salts with heterocycles. The catalytic activity of Zr-PZDB extends to late-stage functionalization of bioactive and drug molecules, including Nikethamide, Admiral, and Myristyl Nicotinate. Systematical spectroscopy study and analysis support the EDA interaction between Zr-PZDB and pyridinium salt or aryl sulfonium salt, respectively. Photoactivation of the MOF-based EDA adduct triggers an intra-complex single electron transfer from donor to acceptor, giving open-shell radical species for cross-coupling reactions. This research represents the first example of MOF-enabled heterogeneous EDA photoactivation.

Date: 2023
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DOI: 10.1038/s41467-023-43577-5

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