Novel A–D–A Type Naphthalenediimide Supramolecule for H<sub>2</sub>O<sub>2</sub> Photosynthesis with Solar‐to‐Chemical Conversion 1.03%
Rong Ji, Yuming Dong, Xinyu Sun, Pengken Li, Renbao Zhang, Chengsi Pan, Hui Zhao, Yongfa Zhu
Abstract
Abstract Organic supermolecules have shown great promise for photocatalytic hydrogen peroxide (H 2 O 2 ) production. However, the limitation of intramolecular charge separation efficiency is still a crucial scientific problem. In this study, a novel acceptor–donor–acceptor (A–D–A) type naphthalenediimide supramolecule (SA‐NDI) is successfully designed for overcoming fundamental issues in organic supermolecule. Composed of one electron‐rich core (naphthalenediimide) and two electron‐poor units (aminopyridine), the supramolecule possesses strong intramolecular charge transfer ability. Meanwhile, the SA‐NDI has an obviously stronger internal electric field, which is 2.83 times higher than that of D–A type supramolecule. The A–D–A type SA‐NDI efficiently accelerates charge separation, so that the intramolecular electron quickly migrates to the acceptor for a two‐electron oxygen reduction reaction. The SA‐NDI supramolecule shows excellent H 2 O 2 accumulation ability (13.7 m m ) and stable cyclic time above 120 h. Meanwhile, the catalyst exhibits a superior solar‐to‐chemical conversion efficiency of 1.03% under simulated solar irradiation. This work provides an entirely new idea to design an organic supramolecule with an efficient intramolecular charge transfer monomer.