摘要
Hydrogen peroxide(H_(2)O_(2))is a clean disinfectant,bleaching agent,and value-added fuel in various systems and is industrially produced through multistep energy-intensive hydrogenation/oxidation using H_(2)and O_(2).The exploitation of metal-free catalysts for alternative H_(2)O_(2)photoconversion is limited by their limited activity and selectivity,especially for the continuous H_(2)O_(2)production using only air,water,and solar light.Now,a cheap and robust polymer,poly(4,4′,4″-(1,3,5-triazine-2,4,6-triyl)triphenyl pyromellitimide)(PTTPI)was rationally synthesized by thermal structure-defect control under relatively low temperature(80-190℃),and the resulting metal-free material with a concisely refined band structure functioned as an efficient and ultra-stable photocatalyst for H_(2)O_(2)production over a wide pH range.The PTTPI photocatalyst with an optimized defective degree(0.51)and moderate bandgap(2.3 eV)exhibited a H_(2)O_(2)production yield rate of 16.6μg h^(−1) mg_(cat)^(−1) and a high apparent quantumefficiency of 16.2%.By merging the well-designed PTTPI catalyst with the water transport path of natural cotton,a zero-emission and sunlightonly input system is constructed for continuous H_(2)O_(2)production from air and water in the natural environment.The design of the polyimide-based catalyst reveals a sustainable future toward efficient H_(2)O_(2)synthesis with sunlight-only energy input,enabling its implementation in other photocatalytic systems and on-site processing communities.
基金
This research was made possible by a generous grant from the National Natural Science Foundation of China(grant nos.21931005,21720102002,21737002,and 22071146)
Shanghai Science and Technology Committee(grant nos.19JC1412600 and 20520711600)and the SJTU-MPI partner group.
