A self-assembly strategy to synthesize carbon doped carbon nitride microtubes with a large π-electron conjugated system for efficient H2 evolution

A self-assembly strategy to synthesize carbon doped carbon nitride microtubes with a large π-electron conjugated system for efficient H2 evolution
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DOI:
10.1016/j.cej.2022.137436
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发表时间:
2022
影响因子:
15.1
通讯作者:
Shuping Zhuo
Shuping Zhuo
中科院分区:
工程技术1区
文献类型:
--
作者:
Shuo Zhao;Yuepeng Liu;Yanyun Wang;Jiasheng Fang;Yiqiang Qi;Yuming Zhou;Lihong Liu;Shuping Zhuo

文献摘要

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• C doping g-C 3 N 4 tube with a large π-electron conjugated system is developed. • The unique tubular morphology endows g-C 3 N 4 the improved surface area. • The effective π delocalization facilitates the charge carrier transfer. • The CCN-10 catalyst displays outstanding photocatalytic activity. • The structure–activity relationship was elucidated. The combination of element doping into carbon nitride and developing a novel structure is charming in realizing outstanding photocatalytic performance. Herein, carbon-doped carbon nitride microtubes with a large π-electron conjugated system were developed via a facile self-assembly strategy. Glucosamine hydrochloride, a substance with abundant hydroxyl and amino, and melamine were applied as precursors based on the self-assembly behavior via hydrogen bonds. The glucosamine hydrochloride content and the formation of hydrogen bond have impacts on self-assembly behavior to fabricate a rod-shaped precursor. Afterwards, carbon-doped carbon nitride microtubes are synthesized after calcination. The effective π delocalization induced by C doping and unique tubular morphology facilitate charge carrier transfer, offer plentiful active sites as well as the improved visible light capture efficiency. Therefore, carbon-doped carbon nitride microtubes display an outstanding H 2 generation rate of 3888.9 μmol h −1 g −1 under λ > 400 nm, far beyond that of pure carbon nitride (886.3 μmol h −1 g −1 ). Experimental and density functional theory calculation demonstrate that carbon doping endows adjustable band structure, narrow band gap, enhanced π electron density and fast charge transfer rate, finally boosts photocatalytic activity. Our work gives a facial way for fabricating C doped carbon nitride with optimized structure and catalytic performance, which offers an efficient method to develop heteroatoms-doped carbon nitride.