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

IF 7.4 2区 工程技术 Q1 ENGINEERING, CHEMICAL Journal of Environmental Chemical Engineering Pub Date : 2024-09-17 DOI:10.1016/j.jece.2024.114172
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引用次数: 0

摘要

光催化产生 H2O2 和裂解木质素 C-C 键是可持续发展的典型策略。遗憾的是,这两个反应的光催化效率仍面临巨大挑战。本文合成了一种具有硫-氯共同掺杂的三嗪和七嗪结构的氮化碳光催化剂(tri/hep-CN)。该催化剂可同时用于光催化 H2O2 生成和木质素 C-C 键裂解。在空气气氛中,向溶剂中加入 β-1 木质素模型 1,2-二苯基乙醇(Dpol)后,H2O2 的产率达到 1171.9 μmol-g-1-h-1。与不添加 Dpol 相比,H2O2 的产量增加了 20 倍。三/六氯化萘具有优异的光生载流子分离效率和正价电位,从而提高了光催化产生 H2O2 和木质素 C-C 键裂解的性能。值得注意的是,将光催化产生 H2O2 与木质素 C-C 键裂解耦合起来,充分利用光生电子和空穴,对于获得出色的光催化性能也非常重要。机理研究表明,光催化产生 H2O2 遵循间接反应机理。同时,木质素 C-C 键的裂解遵循 Cβ 自由基机制和单电子转移机制。这项工作对同时进行光催化产生 H2O2 和木质素 C-C 键裂解的研究很有启发。
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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.

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来源期刊
Journal of Environmental Chemical Engineering
Journal of Environmental Chemical Engineering Environmental Science-Pollution
CiteScore
11.40
自引率
6.50%
发文量
2017
审稿时长
27 days
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.
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