弱激发水衍生自由基化学:进展与展望OA

Chemical reactions driven by water-derived redox radicals have garnered widespread attention across physics,chemis-try,medicine,and environmental science,owing to their distinct advantages of low energy consumption,environmental benignity,and catalyst-free systems.For decades,high-intensity excitation methods(e.g.,irradiation,plasma,ultrahigh temperature)have served as the primary energy sources to induce the formation of water-derived radicals.However,the experimental evidence in recent years has revealed that water-derived redox radicals can also be readily detected under mild reaction conditions,such as gas-liquid in-terfaces,bulk electrolytes,and light irradiation.Compared to high-intensity excitation systems,mild excitation with low energy input is more prevalent in practical applications,including energy conversion,chemical synthesis,and medical diagnosis,thereby offering broader application potential.Nevertheless,the generation pathways of water-derived radicals in mild excitation systems and their in-teraction mechanisms with reaction substrates cannot be reasonably elucidated solely from the perspectives of classic thermodynamic radical diffusion kinetic:this has become a critical bottleneck hampering the advancement and practical implementation of water-derived free radical chemistry.Herein,from the viewpoint of water microstructural evolution and solution environments,we systemati-cally propose the generation mechanisms of water-derived redox radicals modulated by interface,salt solution,organic solvent,and light irradiation.We also identify the key scientific challenges remaining in this field and explore the core research directions for the future.