Efficient photocatalytic H2 evolution over tubular mesoporous carbon nitride with N-vacancy by microwave-assisted synthesis

IF 10.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Science China Chemistry Pub Date : 2025-01-02 DOI:10.1007/s11426-024-2237-1

Yuanlong Pan, Qiang Zhang, Guangzheng Huang, Yannan Luo, Honglin Gao

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Abstract

Modifying the microstructure of photocatalysts while simultaneously introducing vacancies has shown significant potential in enhancing their performance for hydrogen production. Herein, a novel tubular mesoporous carbon nitride (TMCN) with nitrogen vacancies was fabricated using a microwave-assisted synthesis strategy, employing melamine-cyanuric acid supramolecular (MC-S) as the precursor. The optimized TMCN exhibited an outstanding H₂ production rate, approximately 29 times higher than that of pristine g-C₃N₄. The N-vacancies serve as sites for reactant adsorption and activation, leading to enhanced delocalization of HOMO-LUMO. Furthermore, the porous structures of TMCN facilitate the reactant diffusion, while its tubular architectures promote the oriented transfer of charge carriers. Crucially, the markedly improved photocatalytic performance of TMCN can be predominantly attributed to the synergistic effects arising from its superior structure and N-vacancy defects. This work opens new possibilities for the simultaneous formation of surface defect states as photocatalytic reaction sites and distinctive structures conducive to charge carrier transport.

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微波辅助合成具有n空位的管状介孔氮化碳上的高效光催化析氢

改变光催化剂的微观结构，同时引入空位，在提高其制氢性能方面显示出巨大的潜力。本文以三聚氰胺-三聚氰尿酸超分子（MC-S）为前驱体，采用微波辅助合成策略制备了一种新型的具有氮空位的管状介孔氮化碳（TMCN）。优化后的TMCN产氢率比原始的g-C3N4高约29倍。n -空位作为反应物吸附和活化的位点，导致HOMO-LUMO的离域增强。此外，TMCN的多孔结构促进了反应物的扩散，而其管状结构促进了载流子的定向转移。重要的是，TMCN的光催化性能的显著提高主要归因于其优越的结构和n空位缺陷所产生的协同效应。这项工作为同时形成表面缺陷状态作为光催化反应位点和有利于载流子传输的独特结构开辟了新的可能性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Science China Chemistry CHEMISTRY, MULTIDISCIPLINARY-

CiteScore

14.40

自引率

7.30%

发文量

3787

审稿时长

2.2 months

期刊介绍： Science China Chemistry, co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China and published by Science China Press, publishes high-quality original research in both basic and applied chemistry. Indexed by Science Citation Index, it is a premier academic journal in the field. Categories of articles include: Highlights. Brief summaries and scholarly comments on recent research achievements in any field of chemistry. Perspectives. Concise reports on thelatest chemistry trends of interest to scientists worldwide, including discussions of research breakthroughs and interpretations of important science and funding policies. Reviews. In-depth summaries of representative results and achievements of the past 5–10 years in selected topics based on or closely related to the research expertise of the authors, providing a thorough assessment of the significance, current status, and future research directions of the field.