As a metal-free conjugated polymer, carbon nitride (CN) has attracted tremendous attention as a heterogeneous (photo)catalyst. By following the example of enzymes, making all of the catalytic sites accessible via homogeneous reactions is a promising approach toward maximizing CN activity, but hindered due to the poor solubility of CN. Herein, we report the dissolution of CN in environmentally friendly methanesulfonic acid, and homogeneous photocatalysis (two biomimetic/pharmaceutical photocatalytic oxidation reactions) driven by CN for the first time with the activity boosted up to 10-times compared to the heterogeneous counterparts. Moreover, facile recycling and reusability, the hallmarks of heterogeneous catalysts, were kept for the homogeneous CN photocatalyst via reversible precipitation using poor solvents. This study opens a new vista for CN in homogeneous catalysis and offers a successful example of a polymeric catalyst that bridges the gap between homo/heterogeneous catalysis.
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