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 , Jie Xu , Jihuang Zhang , Shixi Bao , 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 , Jie Xu , Jihuang Zhang , Shixi Bao , 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}
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.
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.