Grafting anthraquinone on ultrathin C3N4 for selective toluene photooxidation

IF 7.4 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Science China Materials Pub Date : 2024-11-11 DOI:10.1007/s40843-024-3105-1

Xiong Wang (, ), Guang-Hui Chen (, ), Yang Li (, ), Sheng Tian (, ), Bing-Hao Wang (, ), Biao Hu (, ), Xing-Sheng Hu (, ), Chao Peng (, ), Lang Chen (, ), Shuang-Feng Yin (, )

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Abstract

Anthraquinone (AQ), an effective hydrogen atom transfer catalyst, is limited in photocatalytic applications due to its dimerization. In this study, a simple 3-(3-(dimethylamino) propyl)-1-ethylcarbodiimide hydrochloride/N-hydroxysuccinimide (EDC/HNS) assisted linking strategy was developed to covalently graft AQ–COOH onto C₃N₄ (CN). Using this method, we successfully synthesized amide-bonded CN–AQ ultrathin nanosheets. The amide covalent bond formed between C₃N₄ and AQ facilitates efficient electron migration from C₃N₄ to AQ. As a result, charge carrier recombination is prevented and the hydrogen atom transfer capacity of AQ is enhanced. The CN–AQ photocatalyst exhibits high activity and selectivity with a toluene conversion rate of 10274 (mol g⁻¹ h⁻¹ and 85% selectivity for benzaldehyde, which is 31 times and 1.7 times higher than those of pristine C₃N₄ and AQ–COOH, respectively. Owing to the strong covalent bond in CN–AQ composite, the stability of AQ–COOH was greatly enhanced. This approach provides a new pathway to improve catalytic efficiency and solve the dimerization problem of AQ.

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超薄C3N4接枝蒽醌选择性光氧化甲苯

蒽醌（AQ）是一种有效的氢原子转移催化剂，但其二聚性限制了其光催化应用。本研究建立了一种简单的3-（3-（二甲氨基）丙基）-1-乙基碳二亚胺盐酸盐/ n -羟基琥珀酰亚胺（EDC/HNS）辅助连接策略，将AQ-COOH共价接枝到C3N4 （CN）上。利用这种方法，我们成功地合成了酰胺键合的CN-AQ超薄纳米片。C3N4与AQ之间形成酰胺共价键，促进了电子从C3N4向AQ的高效迁移，从而阻止了载流子的重组，增强了AQ的氢原子转移能力。CN-AQ光催化剂对甲苯的转化率为10274 (mol g−1 h−1)，对苯甲醛的选择性为85%，分别是原始C3N4和AQ-COOH的31倍和1.7倍。由于CN-AQ复合材料中存在较强的共价键，因此大大增强了AQ-COOH的稳定性。该方法为提高催化效率和解决二聚化问题提供了新的途径。

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 Materials Materials Science-General Materials Science

CiteScore

11.40

自引率

7.40%

发文量

949

期刊介绍： Science China Materials (SCM) is a globally peer-reviewed journal that covers all facets of materials science. It is supervised by the Chinese Academy of Sciences and co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China. The journal is jointly published monthly in both printed and electronic forms by Science China Press and Springer. The aim of SCM is to encourage communication of high-quality, innovative research results at the cutting-edge interface of materials science with chemistry, physics, biology, and engineering. It focuses on breakthroughs from around the world and aims to become a world-leading academic journal for materials science.