在协同掺磷和缺陷工程石墨 C3N4 上用可见光光催化合成 H2O2

IF 4.4 3区 化学 Q2 CHEMISTRY, PHYSICAL Catalysis Science & Technology Pub Date : 2024-06-17 DOI:10.1039/d4cy00455h
Xiankui Xu , Zhonghai Zhang
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引用次数: 0

摘要

H2O2 是一种绿色氧化剂,广泛应用于化工生产、环境修复、可持续能源转换和医疗行业。传统的蒽醌法生产 H2O2 面临着潜在的安全隐患和环境污染等问题。因此,绿色和可持续生产 H2O2 的方法值得研究。g-C3N4 是一种非金属光催化剂,具有成本低、环保、稳定性高等优点。然而,g-C3N4 仍然面临着可见光响应范围窄、光生电子/空穴分离效率低、载流子寿命短等问题。g-C3N4 的聚合物特性有利于在三-s-三嗪结构的主体中引入外来原子。通过掺杂可以调整 g-C3N4 的电子结构和光学性质,从而显著提高 g-C3N4 的光催化性能。本研究采用简单的化学气相沉积法制备了掺磷 g-C3N4(P/g-C3N4)。掺杂过程还在 g-C3N4 的体相中引入了缺陷,从而克服了可见光捕获能力弱、电荷分离和转移效率低以及传质速率慢等缺点。此外,优化的导带位置进一步增强了光生电子的还原能力,使其光催化性能比纯 g-C3N4 提高了一个数量级。在可见光的驱动下,P/g-C3N4 通过光催化氧还原反应(ORR)在 2 小时内产生 H2O2,浓度高达 1460.22 μM,并且在三周期催化实验中保持了良好的催化重复性。P/g-C3N4 实现了高效、稳定和绿色合成 H2O2 的目标。
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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Visible light photocatalytic synthesis of H2O2 on synergistic phosphorus-doped and defect engineered graphite C3N4†

H2O2 is a green oxidant, which is widely used in chemical production, environmental remediation, sustainable energy conversion and the medical industry. The traditional anthraquinone method for producing H2O2 is facing issues, such as potential safety hazards and environmental pollution. Therefore, green and sustainable production of H2O2 is desirably investigated. Solar-driven photocatalytic synthesis of H2O2 is a promising method, which requires no additional energy input and will not produce new pollution. g-C3N4 is a kind of nonmetallic photocatalyst, which has the advantages of low cost, environmental friendliness and high stability. However, g-C3N4 still faces the problems of a narrow visible light response range, low photo-generated electron/hole separation efficiency and short carrier lifetime. The polymer properties of g-C3N4 are conducive to introducing foreign atoms into the main body of the tri-s-triazine structure. The electronic structure and optical properties of g-C3N4 can be adjusted by doping, which can significantly improve the photocatalytic performance of g-C3N4. In this work, phosphorus doped g-C3N4 (P/g-C3N4) is prepared by a simple chemical vapor deposition method. The doping process also introduced defects in the bulk phase of g-C3N4, which overcomes drawbacks such as weak visible light capturing ability, low charge separation and transfer efficiency, and a slow mass transfer rate. In addition, the optimized conduction band position further enhances the reduction ability of photo-generated electrons, making its photocatalytic performance magnify by one order of magnitude compared to that of pure g-C3N4. Driven by visible light, P/g-C3N4 produces H2O2 through the photocatalytic oxygen reduction reaction (ORR) in 2 h, reaching a high concentration of 1460.22 μM, and it also maintains good catalytic repeatability in three-cycle catalytic experiments. P/g-C3N4 achieves the goal of efficient, stable and green synthesis of H2O2.

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来源期刊
Catalysis Science & Technology
Catalysis Science & Technology CHEMISTRY, PHYSICAL-
CiteScore
8.70
自引率
6.00%
发文量
587
审稿时长
1.5 months
期刊介绍: A multidisciplinary journal focusing on cutting edge research across all fundamental science and technological aspects of catalysis. Editor-in-chief: Bert Weckhuysen Impact factor: 5.0 Time to first decision (peer reviewed only): 31 days
期刊最新文献
Back cover Inside back cover Outstanding Reviewers for Catalysis Science & Technology in 2023 Thermostable fatty acid hydroxylases from ancestral reconstruction of cytochrome P450 family 4 enzymes Catalytic processes for the selective hydrogenation of fats and oils: reevaluating a mature technology for feedstock diversification
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