Unraveling the dipole field in ultrathin, porous, and defective carbon nitride nanosheets for record-high piezo-photocatalytic H2O2 production
Zhaoqiang Wang, Guixiang Ding, Hongwei Huang, Juntao Zhang, Qi Lv, Shuai Li, Yonghao Ni, Guangfu Liao
Abstract
Piezo-photocatalysis is capable of concerting mechanical vibration into chemical energy, portraying a promising alternative technology for H 2 O 2 production. However, low mechanical energy conversion efficiency and constrained surface active sites hinder its practical application. Herein, ultrathin porous carbon nitride nanosheets with controlled carbon vacancies and oxygen doping (OCN-X, where X represents the calcination temperature) are synthesized by thermal oxidation etching to achieve unprecedented piezo-photocatalytic H 2 O 2 production. The carbon vacancies and oxygen doping cause the formation of asymmetric structure of triazine unit with a strong dipole field, which creates spontaneous polarization field to speed up directional electron transfer to the nitrogen active sites for effective piezo-photocatalysis. Meanwhile, the ultrathin and porous structure formed by hot-oxygen etching enhances the mechanical energy conversion efficiency and collaboratively induces adsorbed oxygen via indirect two-electron oxygen reduction reaction (ORR) transfer pathway to effectively produce H 2 O 2 . Consequently, without any co-catalysts, the as-prepared OCN-460 displays record-high piezo-photocatalytic H 2 O 2 production rate of 19.30 mmol g −1 h −1 , far outdistancing those previously reported for piezo-photocatalysts. Furthermore, it also still maintains a notable piezo-photocatalytic activity of 2.87 mmol g −1 h −1 in the pure water system. This work offers some new insights for the future design of an effective piezo-photocatalytic H 2 O 2 production system. • Ultrathin porous g-C 3 N 4 nanosheets with carbon vacancies and oxygen doping were prepared. • Record-high piezo-photocatalytic H 2 O 2 production was achieved. • Dipole field in ultrathin, porous, and defective g-C 3 N 4 nanosheets was revealed. • Piezo-photocatalytic mechanism was revealed by state-of-the-art characterizations.