In Situ Self-Assembly of Hydrogen-Bonded Organic Frameworks for Organic Photoredox Catalysis

Structural self-assembly enables the hydrogen-bonded organic frameworks (HOFs) with facile synthesis, self-repair structures, and intriguing optoelectronic attributes. Herein, we report a strategy that directly employs the HOF monomer for efficient photoredox catalysis without involving the catalyst prefabrication. Remarkably, this simplified mode was equally effective as the prefabricated HOF catalysts, verified with high activity, selectivity, and generality in photocatalytic sulfide oxygenation. The complementary hydrogen (H) bonds of carboxy dimmers led to a fast in situ self-assembly of the HOF monomer into the target HOF framework. The yield enhancement of singlet oxygen (1O2) resulting from the excitonic effect and strong interlayer confinement of self-assembly frameworks accounted for the activity origin. This work offered a facile but efficient application approach to use HOF material for photoredox catalysis.

Automated summary

In this work, a strategy of directly using the hydrogen-bonded organic framework (HOF) monomer for efficient photoredox catalysis without catalyst prefabrication is reported. This simplified mode showed equal effectiveness as the prefabricated HOF catalysts, with high activity, selectivity, and generality in photocatalytic sulfide oxygenation. The in situ self-assembly of the HOF monomer into the target HOF framework was achieved through complementary hydrogen bonds of carboxy dimers. The enhanced yield of singlet oxygen (1O2) resulting from the excitonic effect and strong interlayer confinement of self-assembly frameworks explained the origin of activity. This work offers a facile yet efficient approach to utilize HOF material for photoredox catalysis.