{"title":"构建硫-氯共同掺杂的三嗪/庚嗪均相结氮化碳光催化剂,用于同时产生 H2O2 和裂解木质素 C-C 键","authors":"","doi":"10.1016/j.jece.2024.114172","DOIUrl":null,"url":null,"abstract":"<div><p>Photocatalytic H<sub>2</sub>O<sub>2</sub> production and cleavage of lignin C-C bonds is a typical strategy that follows sustainable development. Unfortunately, the photocatalytic efficiency of these two reactions still faces significant challenges. Herein, a carbon nitride photocatalyst (tri/hep-CN) with sulfur-chloride co-doped triazine and heptazine structures was synthesized. It was simultaneously used for photocatalytic H<sub>2</sub>O<sub>2</sub> production and lignin C-C bond cleavage. In the air atmosphere, the yield of H<sub>2</sub>O<sub>2</sub> reached 1171.9 μmol•g<sup>−1</sup>•h<sup>−1</sup> after the addition of β-1 lignin model 1,2-diphenylethanol (Dpol) to the solvent. The yield of H<sub>2</sub>O<sub>2</sub> increased by 20 times compared with no addition of Dpol. The lignin C-C bond in Dpol is also efficiently broken, producing benzaldehyde and benzyl alcohol. tri/hep-CN has excellent photogenerated carrier separation efficiency and positive valence potential, which improves the photocatalytic H<sub>2</sub>O<sub>2</sub> production and lignin C-C bond cleavage performance. Notably, coupling photocatalytic H<sub>2</sub>O<sub>2</sub> production with lignin C-C bond cleavage to fully use photogenerated electrons and holes is also very important to obtain outstanding photocatalytic performance. Mechanistic studies have shown that photocatalytic H<sub>2</sub>O<sub>2</sub> production follows an indirect reaction mechanism. Meanwhile, the cleavage of lignin C-C bond follows the C<sub>β</sub> radical mechanism and the single electron transfer mechanism. This work is very instructive for simultaneous photocatalytic H<sub>2</sub>O<sub>2</sub> production and lignin C-C bond cleavage studies.</p></div>","PeriodicalId":15759,"journal":{"name":"Journal of Environmental Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":7.4000,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Construction of sulfur-chloride co-doped triazine/heptazine homojunction carbon nitride photocatalyst for simultaneous production of H2O2 and lignin C-C bond cleavage\",\"authors\":\"\",\"doi\":\"10.1016/j.jece.2024.114172\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Photocatalytic H<sub>2</sub>O<sub>2</sub> production and cleavage of lignin C-C bonds is a typical strategy that follows sustainable development. Unfortunately, the photocatalytic efficiency of these two reactions still faces significant challenges. Herein, a carbon nitride photocatalyst (tri/hep-CN) with sulfur-chloride co-doped triazine and heptazine structures was synthesized. It was simultaneously used for photocatalytic H<sub>2</sub>O<sub>2</sub> production and lignin C-C bond cleavage. In the air atmosphere, the yield of H<sub>2</sub>O<sub>2</sub> reached 1171.9 μmol•g<sup>−1</sup>•h<sup>−1</sup> after the addition of β-1 lignin model 1,2-diphenylethanol (Dpol) to the solvent. The yield of H<sub>2</sub>O<sub>2</sub> increased by 20 times compared with no addition of Dpol. The lignin C-C bond in Dpol is also efficiently broken, producing benzaldehyde and benzyl alcohol. tri/hep-CN has excellent photogenerated carrier separation efficiency and positive valence potential, which improves the photocatalytic H<sub>2</sub>O<sub>2</sub> production and lignin C-C bond cleavage performance. Notably, coupling photocatalytic H<sub>2</sub>O<sub>2</sub> production with lignin C-C bond cleavage to fully use photogenerated electrons and holes is also very important to obtain outstanding photocatalytic performance. Mechanistic studies have shown that photocatalytic H<sub>2</sub>O<sub>2</sub> production follows an indirect reaction mechanism. Meanwhile, the cleavage of lignin C-C bond follows the C<sub>β</sub> radical mechanism and the single electron transfer mechanism. This work is very instructive for simultaneous photocatalytic H<sub>2</sub>O<sub>2</sub> production and lignin C-C bond cleavage studies.</p></div>\",\"PeriodicalId\":15759,\"journal\":{\"name\":\"Journal of Environmental Chemical Engineering\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":7.4000,\"publicationDate\":\"2024-09-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Environmental Chemical Engineering\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2213343724023030\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Environmental Chemical Engineering","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2213343724023030","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Construction of sulfur-chloride co-doped triazine/heptazine homojunction carbon nitride photocatalyst for simultaneous production of H2O2 and lignin C-C bond cleavage
Photocatalytic H2O2 production and cleavage of lignin C-C bonds is a typical strategy that follows sustainable development. Unfortunately, the photocatalytic efficiency of these two reactions still faces significant challenges. Herein, a carbon nitride photocatalyst (tri/hep-CN) with sulfur-chloride co-doped triazine and heptazine structures was synthesized. It was simultaneously used for photocatalytic H2O2 production and lignin C-C bond cleavage. In the air atmosphere, the yield of H2O2 reached 1171.9 μmol•g−1•h−1 after the addition of β-1 lignin model 1,2-diphenylethanol (Dpol) to the solvent. The yield of H2O2 increased by 20 times compared with no addition of Dpol. The lignin C-C bond in Dpol is also efficiently broken, producing benzaldehyde and benzyl alcohol. tri/hep-CN has excellent photogenerated carrier separation efficiency and positive valence potential, which improves the photocatalytic H2O2 production and lignin C-C bond cleavage performance. Notably, coupling photocatalytic H2O2 production with lignin C-C bond cleavage to fully use photogenerated electrons and holes is also very important to obtain outstanding photocatalytic performance. Mechanistic studies have shown that photocatalytic H2O2 production follows an indirect reaction mechanism. Meanwhile, the cleavage of lignin C-C bond follows the Cβ radical mechanism and the single electron transfer mechanism. This work is very instructive for simultaneous photocatalytic H2O2 production and lignin C-C bond cleavage studies.
期刊介绍:
The Journal of Environmental Chemical Engineering (JECE) serves as a platform for the dissemination of original and innovative research focusing on the advancement of environmentally-friendly, sustainable technologies. JECE emphasizes the transition towards a carbon-neutral circular economy and a self-sufficient bio-based economy. Topics covered include soil, water, wastewater, and air decontamination; pollution monitoring, prevention, and control; advanced analytics, sensors, impact and risk assessment methodologies in environmental chemical engineering; resource recovery (water, nutrients, materials, energy); industrial ecology; valorization of waste streams; waste management (including e-waste); climate-water-energy-food nexus; novel materials for environmental, chemical, and energy applications; sustainability and environmental safety; water digitalization, water data science, and machine learning; process integration and intensification; recent developments in green chemistry for synthesis, catalysis, and energy; and original research on contaminants of emerging concern, persistent chemicals, and priority substances, including microplastics, nanoplastics, nanomaterials, micropollutants, antimicrobial resistance genes, and emerging pathogens (viruses, bacteria, parasites) of environmental significance.