Multiple Covalent/hydrogen Bonds Bridging Electron Transfer in Polymeric Carbon Nitride for Efficient Photocatalytic H2O2 Production

Photo-driven H 2 O 2 production by graphitic carbon nitride (g-C 3 N 4 ) using H 2 O and O 2 is a sustainable alternative to fossil fuels, but pristine g-C 3 N 4 is typically limited by inefficient charge transfer and separation. Many research works have focused on the construction of catalyst heterojunction, doping and defect engineering with electron migration for enhanced H 2 O 2 synthesis, while also damaging the intrinsic crystal structure of the catalysts. Herein, a "living " aldehyded cellulose nanofibers (CNF A ) are anchored onto g-C 3 N 4 with multiple hydrogen and covalent bonding. Moreover, the CNF A incorporation is found to dominantly increase the wettability of g-C 3 N 4 and promote the adsorption of molecular oxygen. Batch experiments and DFT calculations further confirm that high-quality interfacial hydrogen and covalent bonding between CNF A and g-C 3 N 4 with boosting transfer of photogenerated electrons, leading enhanced single-electron oxygen reduction reaction (ORR) for H 2 O 2 generation. The optimized photocatalytic H 2 O 2 of resultant MCN-CNF A is 67.44 mu mol/L, surpassing four-folds of pristine MCN. This work provides an eco-friendly design of active cellulose nanofibers, which efficiently tunes the intramolecular charge transfer of g-C 3 N 4-based photocatalysts for H 2 O 2 generation.