Ag3PO4 enables the generation of long-lived radical cations for visible light-driven [2 + 2] and [4 + 2] pericyclic reactions

Lirong Guo, Rongchen Chu, Xinyu Hao, Yu Lei, Haibin Li, Dongge Ma, Guo Wang, Chen-Ho Tung and Yifeng Wang ()
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Lirong Guo: School of Chemistry and Chemical Engineering Shandong University Jinan
Rongchen Chu: School of Chemistry and Chemical Engineering Shandong University Jinan
Xinyu Hao: School of Chemistry and Chemical Engineering Shandong University Jinan
Yu Lei: Institute of Chemistry Chinese Academy of Sciences Beijing
Haibin Li: School of Chemistry and Chemical Engineering Shandong University Jinan
Dongge Ma: College of Chemistry and Materials Engineering Beijing Technology and Business University Beijing
Guo Wang: Department of Chemistry Capital Normal University Beijing
Chen-Ho Tung: School of Chemistry and Chemical Engineering Shandong University Jinan
Yifeng Wang: School of Chemistry and Chemical Engineering Shandong University Jinan

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Photocatalytic redox reactions are important for synthesizing fine chemicals from olefins, but the limited lifetime of radical cation intermediates severely restricts semiconductor photocatalysis efficiency. Here, we report that Ag3PO4 can efficiently catalyze intramolecular and intermolecular [2 + 2] and Diels-Alder cycloadditions under visible-light irradiation. The approach is additive-free, catalyst-recyclable. Mechanistic studies indicate that visible-light irradiation on Ag3PO4 generates holes with high oxidation power, which oxidize aromatic alkene adsorbates into radical cations. In photoreduced Ag3PO4, the conduction band electron (eCB−) has low reduction power due to the delocalization among the Ag+-lattices, while the particle surfaces have a strong electrostatic interaction with the radical cations, which considerably stabilize the radical cations against recombination with eCB−. The radical cation on the particle’s surfaces has a lifetime of more than 2 ms, 75 times longer than homogeneous systems. Our findings highlight the effectiveness of inorganic semiconductors for challenging radical cation-mediated synthesis driven by sunlight.

Date: 2024
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DOI: 10.1038/s41467-024-45217-y

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