Cnotrolled synthesis of hollow carbon ring incorporated g-C₃N₄ tubes for boosting photocatalytic H₂O₂ Production

Authors：Hao Luo, Tianshang Shan, Jianwen Zhou, Liulian Huang, Lihui Chen, Rongjian Sa*, Yusuke Yamauchi*, Jungmok You, Yusuke Asakura, Zhanhui Yuan* and He Xiao*

Abstract:H₂O₂ production through solar-driven photocatalytic route has received increasing attention. Herein, a carbon ring incorporated hollow g-C₃N₄ tubes (CHCN) was successfully fabricated via a novel supramolecular self-assembly strategy, co-inducing by hydrogen bond and covalent bond. The optimum H₂O₂ yield over the CHCN-0.02 reached up to 1.58 mmol L⁻¹ h⁻¹ (AQE= 28.10%, 420 nm), which was 5.4 times significantly higher than that of bulk g-C₃N₄ (0.29 mmol L⁻¹ h⁻¹) under visible light irradiation. Experimental and density functional theory (DFT) calculations revealed that the CHCNs not only expedited the charge carrier transfer/separation but also favored molecular oxygen adsorption and regulated bandgap structure under the in-plane electronic field induced by continuous π-conjugated Cring, which boosted the ORR efficiency for photocatalytic H₂O₂ synthesis. The optimized CHCN catalyst demonstrated adequate hybrid ORR routes, consisting of a dominated selective one-step two-electron ORR pathway and highly efficient two-step single-electron ORR for H₂O₂ production. Therefore, this work not only provides a new strategy for an efficient H₂O₂ formation using a g-C₃N₄-based photocatalyst but also explores the functionary mechanism of the ORR process and enlightens the way to highly efficient H₂O₂ generation.

Keywords:Carbon nitridePhotocatalyticHydrogen peroxideCarbon rings

DOI:https://doi.org/10.1016/j.apcatb.2023.122933