Supramolecular Self-Assembly of Nitrogen-Deficient Ag/g‑C3N4 Nanofiber Films with Enhanced Charge Transfer Dynamics for Efficient Visible-Light Photocatalytic Activity

Molecular self-assembly of organic molecules through noncovalent interactions is a powerful strategy for designing functional materials. Herein, we fabricated a novel free-standing Ag/g-C3N4 nanofiber (Ag/CNNF) film via a water-based molecular engineering approach followed by pyrolysis using a cyanuric acid–melamine complex as the precursor. Uniform dispersion of plasmonic Ag nanoparticles and incorporation of nitrogen vacancies were synchronously introduced into the 3D highly interconnected porous CNNF framework. The resulting Ag/CNNF film with multilevel interlayer spacing distributions significantly expedited more sufficient charge transfer dynamics not only at Schottky junction sites but also throughout hierarchical CN by exciton dissociation. Benefiting from the synergistic enhancement in visible light harvesting capability and steered charge carrier transfer in a longitudinal direction, the Ag/CNNF film presented remarkably boosted photocatalytic ability both for hydrogen production and tetracycline degradation. The optimal Ag/CNNF-2 film exhibited a prominent photocatalytic hydrogen evolution rate of 1240 μmol g–1 h–1 without the Pt co-catalyst under visible light illumination, which was 10.3 times as high as that of bulk g-C3N4. Significantly, 1D Ag/g-C3N4 nanofibers self-assembled into an ordered and macroscopic film, which was more favorable in practical applications owing to good reusability and high processability. This work paved the way for the facile preparation of supramolecular self-assembled CN-based film photocatalysts.