Organic π-conjugated polymers are promising heterogeneous photocatalysts that involve photoredox or energy transfer processes. In such settings, the materials are usually applied in the form of dispersion in liquid medium, which is bound to certain technological limits of applicability. Herein, we present an innovative approach using carbon nitride thin films prepared via chemical vapor deposition at different vessel walls and using them as batch and microfluidic photoreactors. This approach allows us not only to fabricate technologically relevant and reusable devices but also to improve photophysical properties of carbon nitride, such as the singlet–triplet energy gap and lifetime of triplet excited states, when the material is assembled in thin films. These morphological changes are employed to maximize the performance of the materials in photocatalytic reactions, in which the carbon nitride thin films show at least 1 order of magnitude higher activity per area unit compared to photocatalysis using suspended particles.
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