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.

CdS has been widely used in photocatalytic water splitting due to its advantages of easy excitation by visible light and low cost. However, the applications of CdS are limited by...