Regulating charge dynamics in covalent organic frameworks for efficient solar-driven hydrogen peroxide production

Abstract

Solar-driven hydrogen peroxide (H₂O₂) production offers a green and sustainable alternative to the energy-intensive anthraquinone process, utilizing water and oxygen as feedstock and solar energy as the sole input. Covalent organic frameworks (COFs), owing to their well-defined crystalline structures and tunable electronic properties, have emerged as a compelling platform for photocatalytic H₂O₂ synthesis. However, the efficiency of H₂O₂ photosynthesis remains limited by sluggish charge separation and rapid carrier recombination. Regulating charge dynamics, encompassing photogenerated exciton dissociation, carrier transport, and interfacial redox kinetics, is therefore central to unlocking the full potential of COF-based photocatalysts. In this Feature Article, we review recent progress in regulating charge dynamics within COFs for efficient solar-driven H₂O₂ production. We discuss key material design strategies including donor–acceptor engineering, functional group modification, molecular doping, topological control, regioisomeric design, and heterostructure construction. By correlating structural features with exciton binding energy, charge mobility, and photocatalytic performances, we highlight how molecular-level design translates into photocatalytic performance. Finally, we outline current challenges and propose future research directions to accelerate the development of high-efficiency COF-based materials for solar fuel generation.