The Keto‐Switched Photocatalysis of Reconstructed Covalent Organic Frameworks for Efficient Hydrogen Evolution

Abstract The keto‐switched photocatalysis of covalent organic frameworks (COFs) for efficient H 2 evolution was reported the first time by engineering, at a molecular level, local structure and component skeletal building blocks. A series imine‐linked BT‐COFs were synthesized Schiff‐base reaction 1, 3, 5‐benzenetrialdehyde with diamines to demonstrate structural reconstruction enol keto configurations alkaline catalysis. groups blocks served as active injectors, where hot π‐electrons provided Pt nanoparticles (NPs) across polyvinylpyrrolidone (PVP) insulting layer. characterization results, together density functional theory calculations, indicated clearly that formation keto‐injectors not only made conduction band level more negative, but also led an inhomogeneous charge distribution in donor‐acceptor form strong intramolecular built‐in electric field. As result, visible‐light TP‐COFs‐1 one group successfully enabled achieved impressive rate high 0.96 mmol g −1 h . Also, photocatalytic rates reconstructed BT‐COFs‐2 ‐3 two three significantly enhanced post‐treatment.