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具有显著增强的可见光光催化活性用于四环素降解和析氢的Ag@AgCl/g-CN/沸石复合材料的合理设计

Rational design of Ag@AgCl/g-CN/zeolite composite with significantly enhanced visible-light photocatalytic activity for tetracycline degradation and hydrogen evolution.

作者信息

Gao Sihang, Hu Xiaolong, Wu Kexin, Hou Runa, Song Junying, Wang Li, Qian Weimin, Wu Sana, Lu Qing, Guo Qingbin, Gao Dengzheng

机构信息

College of Energy and Mining Engineering, Shandong University of Science and Technology, Qingdao, 266590, China.

College of Energy and Mining Engineering, Shandong University of Science and Technology, Qingdao, 266590, China; Huzhou Xinkaiyuan Detritus Co., Ltd., Huzhou, Zhejiang, 313002, China.

出版信息

Environ Res. 2025 Jul 8;285(Pt 1):122325. doi: 10.1016/j.envres.2025.122325.

DOI:10.1016/j.envres.2025.122325
PMID:40639598
Abstract

In the case of increasingly scarce global energy resources and worsening environmental problems, it is particularly important to explore effective ways to alleviate the environmental and energy crises. In this paper, a ternary Ag@AgCl/g-CN/zeolite photocatalyst was prepared for effective degradation of tetracycline (TC) and H production under visible light. Under visible light irradiation, the Ag@AgCl/g-CN/zeolite-25 photocatalyst demonstrates a remarkable degradation efficiency of 97.2 % for TC in 120 min and the maximum H production rate with 962.9 μmol h•g which is 13.0 and 4.5 times that of g-CN and Ag@AgCl. The significant improvement of photocatalytic activity is mainly attributed to the construction of Ag@AgCl/g-CN heterojunction, the introduction of zeolite carrier with good dispersion effect and the surface plasmon resonance (SPR) effect of Ag particles in composite. Furthermore, the degradation process of TC was investigated using three-dimensional fluorescence spectroscopy (3D EEM). The intermediate product was characterized using HPLC-MS analysis, and a degradation pathway for TC was proposed. The toxicity of the intermediate product was assessed using the TEST method. Moreover, a detailed reaction mechanism was proposed. This work provides a promising catalyst and a new strategy for efficient photocatalytic H evolution and wastewater treatment based on the construction of plasmonic heterojunction structure on mineral carrier.

摘要

在全球能源资源日益稀缺和环境问题不断恶化的情况下,探索缓解环境和能源危机的有效途径尤为重要。本文制备了一种三元Ag@AgCl/g-CN/沸石光催化剂,用于在可见光下有效降解四环素(TC)和产氢。在可见光照射下,Ag@AgCl/g-CN/沸石-25光催化剂在120分钟内对TC的降解效率高达97.2%,最大产氢速率为962.9 μmol h•g,分别是g-CN和Ag@AgCl的13.0倍和4.5倍。光催化活性的显著提高主要归因于Ag@AgCl/g-CN异质结的构建、具有良好分散效果的沸石载体的引入以及复合材料中Ag颗粒的表面等离子体共振(SPR)效应。此外,利用三维荧光光谱(3D EEM)研究了TC的降解过程。通过HPLC-MS分析对中间产物进行了表征,并提出了TC的降解途径。使用TEST方法评估了中间产物的毒性。此外,还提出了详细的反应机理。这项工作基于在矿物载体上构建等离子体异质结结构,为高效光催化产氢和废水处理提供了一种有前景的催化剂和新策略。

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