Covalently Linked Organic–Inorganic Hybrid Assemblies for Enhanced Photocatalytic Water Splitting

This work presents an experimentally viable synthetic approach for developing visible light-active water-splitting photocatalysts based on organic semiconductors with tunable bandgaps. Chromophore–catalyst dyad assemblies were synthesized by covalently linking catalytic units to donor–acceptor conjugated organic semiconductors. These ensembles demonstrate photocatalytic activity, with hydrogen evolution rates of 1.12 mmol g–1 h–1 and oxygen evolution rates of 420 μmol g–1 h–1 during 12-h studies. Computational analyses indicate that the improved performance results from advantageous energy level alignment between the chromophore and catalytic unit, promoting efficient charge transfer. This research illustrates the feasibility of organic semiconductor photocatalysts for sustainable hydrogen generation and offers mechanistic insights to inform future advancements in clean energy technology.