Donor–Acceptor Solid Molecular Catalysts for Photocatalytic Hydrogen Peroxide Production

Solid molecular catalysts (SMCs) represent a promising class of photocatalysts. Here, we report the influence of distinct donor and acceptor moieties of terpyridine‐based SMCs on the photocatalytic hydrogen peroxide (H 2 O 2 ) production. An aromatic and linear donor proved to be advantageous due to its favorable optoelectrical properties, achieving an activity of 8.55 mmol g −1 h −1 under white light irradiation without any sacrificial agents. The variation of backbone functionalities (toluene (C), pyrrole (N), furan (O), and thiophene (S)) revealed the important role of charge stabilization in the acceptor units through inductive and mesomeric effects. Scaling up the reaction with the best performing SMC C2‐SP1 yielded a photocatalytic activity of 12.8 mmol g −1 h −1 (405 nm). To facilitate the transition from laboratory studies to practical applications, H 2 O 2 production has been successfully demonstrated under natural sunlight. Under optimized reaction conditions, concentrations of up to 108.3 mg L −1 were achieved, demonstrating the potential of SMCs for sustainable hydrogen peroxide generation.