光催化
光化学
材料科学
吸附
带隙
制氢
电子转移
共价键
催化作用
化学工程
共轭体系
密度泛函理论
氢键
纳米技术
化学
有机化学
光电子学
计算化学
分子
聚合物
复合材料
工程类
作者
Hao Luo,Tianshang Shan,Jianwen Zhou,Liulian Huang,Lihui Chen,Rongjian Sa,Yusuke Yamauchi,Jungmok You,Yusuke Asakura,Zhanhui Yuan,He Xiao
标识
DOI:10.1016/j.apcatb.2023.122933
摘要
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.
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