通过构建三嗪-七嗪基氮化碳和偶联木质素CC键裂解提高H2O2产光催化性能

IF 2 3区 化学 Q4 CHEMISTRY, PHYSICAL
Man Liu , Jie Xu , Jihuang Zhang , Shixi Bao , Chang Ge
{"title":"通过构建三嗪-七嗪基氮化碳和偶联木质素CC键裂解提高H2O2产光催化性能","authors":"Man Liu ,&nbsp;Jie Xu ,&nbsp;Jihuang Zhang ,&nbsp;Shixi Bao ,&nbsp;Chang Ge","doi":"10.1016/j.chemphys.2025.112799","DOIUrl":null,"url":null,"abstract":"<div><div>Photocatalytic H<sub>2</sub>O<sub>2</sub> production and lignin C<img>C bond cleavage have a positive effect on promoting green and sustainable development. At present, the photocatalytic efficiency of these two reactions can yet be greatly enhanced. Herein, a series of carbon nitride-based photocatalysts with triazine and heptazine units were synthesized. The ratio of triazine and heptazine units was successfully adjusted by changing the ratio of raw materials (urea and melem). When the mass ratio of urea to melem was 1:1, the synthesized photocatalyst 1 U/M-CN had the best photocatalytic performance for H<sub>2</sub>O<sub>2</sub> production. The amount of H<sub>2</sub>O<sub>2</sub> production was increased by 14 times via the addition of 1,2-diphenylethanol (Dpol, β-1 lignin model) to induce the oxidative half-reaction. Under optimal conditions, the concentration of H<sub>2</sub>O<sub>2</sub> production and the cleavage efficiency of lignin C<img>C bonds in Dpol reached 1126.1 μmol/g and 91.2 %, respectively. Mechanistic studies show that the electron transfer pathway in 1 U/M-CN follows the S-Scheme mechanism. The photocatalytic production of H<sub>2</sub>O<sub>2</sub> conforms to the indirect reaction pathway, and the photocatalytic lignin C<img>C bond cleavage follows the C<sub>β</sub> radical mechanism. This work provides a new idea for simultaneous photocatalytic H<sub>2</sub>O<sub>2</sub> production and lignin C<img>C bond cleavage by constructing triazine-heptazine-based carbon nitride photocatalysts.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"597 ","pages":"Article 112799"},"PeriodicalIF":2.0000,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhancing photocatalytic performance for H2O2 production by constructing triazine-heptazine-based carbon nitride and coupling lignin CC bond cleavage\",\"authors\":\"Man Liu ,&nbsp;Jie Xu ,&nbsp;Jihuang Zhang ,&nbsp;Shixi Bao ,&nbsp;Chang Ge\",\"doi\":\"10.1016/j.chemphys.2025.112799\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Photocatalytic H<sub>2</sub>O<sub>2</sub> production and lignin C<img>C bond cleavage have a positive effect on promoting green and sustainable development. At present, the photocatalytic efficiency of these two reactions can yet be greatly enhanced. Herein, a series of carbon nitride-based photocatalysts with triazine and heptazine units were synthesized. The ratio of triazine and heptazine units was successfully adjusted by changing the ratio of raw materials (urea and melem). When the mass ratio of urea to melem was 1:1, the synthesized photocatalyst 1 U/M-CN had the best photocatalytic performance for H<sub>2</sub>O<sub>2</sub> production. The amount of H<sub>2</sub>O<sub>2</sub> production was increased by 14 times via the addition of 1,2-diphenylethanol (Dpol, β-1 lignin model) to induce the oxidative half-reaction. Under optimal conditions, the concentration of H<sub>2</sub>O<sub>2</sub> production and the cleavage efficiency of lignin C<img>C bonds in Dpol reached 1126.1 μmol/g and 91.2 %, respectively. Mechanistic studies show that the electron transfer pathway in 1 U/M-CN follows the S-Scheme mechanism. The photocatalytic production of H<sub>2</sub>O<sub>2</sub> conforms to the indirect reaction pathway, and the photocatalytic lignin C<img>C bond cleavage follows the C<sub>β</sub> radical mechanism. This work provides a new idea for simultaneous photocatalytic H<sub>2</sub>O<sub>2</sub> production and lignin C<img>C bond cleavage by constructing triazine-heptazine-based carbon nitride photocatalysts.</div></div>\",\"PeriodicalId\":272,\"journal\":{\"name\":\"Chemical Physics\",\"volume\":\"597 \",\"pages\":\"Article 112799\"},\"PeriodicalIF\":2.0000,\"publicationDate\":\"2025-05-29\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemical Physics\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0301010425002009\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q4\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Physics","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0301010425002009","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q4","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0

摘要

光催化H2O2生成和木质素CC键裂解对促进绿色可持续发展具有积极作用。目前,这两种反应的光催化效率还可以大大提高。本文合成了一系列氮化碳基三嗪基和七嗪基光催化剂。通过改变原料(尿素和甲醇)的比例,成功地调整了三嗪和七嗪单元的比例。当尿素与甲醇的质量比为1:1时,合成的光催化剂1 U/M-CN对H2O2的光催化性能最好。通过加入1,2-二苯乙醇(Dpol, β-1木质素模型)诱导氧化半反应,H2O2产量提高了14倍。在最佳条件下,Dpol中H2O2的生成浓度和木质素CC键的裂解效率分别达到1126.1 μmol/g和91.2%。机理研究表明,1 U/M-CN中的电子传递途径遵循S-Scheme机制。光催化生成H2O2符合间接反应途径,光催化木质素CC键裂解遵循Cβ自由基机制。本研究为构建三嗪-七嗪基氮化碳光催化剂同时催化H2O2生成和木质素CC键裂解提供了新思路。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Enhancing photocatalytic performance for H2O2 production by constructing triazine-heptazine-based carbon nitride and coupling lignin CC bond cleavage

Enhancing photocatalytic performance for H2O2 production by constructing triazine-heptazine-based carbon nitride and coupling lignin CC bond cleavage
Photocatalytic H2O2 production and lignin CC bond cleavage have a positive effect on promoting green and sustainable development. At present, the photocatalytic efficiency of these two reactions can yet be greatly enhanced. Herein, a series of carbon nitride-based photocatalysts with triazine and heptazine units were synthesized. The ratio of triazine and heptazine units was successfully adjusted by changing the ratio of raw materials (urea and melem). When the mass ratio of urea to melem was 1:1, the synthesized photocatalyst 1 U/M-CN had the best photocatalytic performance for H2O2 production. The amount of H2O2 production was increased by 14 times via the addition of 1,2-diphenylethanol (Dpol, β-1 lignin model) to induce the oxidative half-reaction. Under optimal conditions, the concentration of H2O2 production and the cleavage efficiency of lignin CC bonds in Dpol reached 1126.1 μmol/g and 91.2 %, respectively. Mechanistic studies show that the electron transfer pathway in 1 U/M-CN follows the S-Scheme mechanism. The photocatalytic production of H2O2 conforms to the indirect reaction pathway, and the photocatalytic lignin CC bond cleavage follows the Cβ radical mechanism. This work provides a new idea for simultaneous photocatalytic H2O2 production and lignin CC bond cleavage by constructing triazine-heptazine-based carbon nitride photocatalysts.
求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
Chemical Physics
Chemical Physics 化学-物理:原子、分子和化学物理
CiteScore
4.60
自引率
4.30%
发文量
278
审稿时长
39 days
期刊介绍: Chemical Physics publishes experimental and theoretical papers on all aspects of chemical physics. In this journal, experiments are related to theory, and in turn theoretical papers are related to present or future experiments. Subjects covered include: spectroscopy and molecular structure, interacting systems, relaxation phenomena, biological systems, materials, fundamental problems in molecular reactivity, molecular quantum theory and statistical mechanics. Computational chemistry studies of routine character are not appropriate for this journal.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信