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可见光驱动的钒酸铜/生物炭纳米复合材料用于四环素的多相光催化降解:性能、机理及机器学习应用

Visible light-driven copper vanadate/biochar nanocomposite for heterogeneous photocatalysis degradation of tetracycline: Performance, mechanism, and application of machine learning.

作者信息

Chen Yuxuan, Zhao Chuanqi, Tan Wen, Gong Sinuo, Pan Honghui, Liu Xixiang, Huang Shiyong, Shi Qin

机构信息

Guangxi Colleges and Universities Key Laboratory of Environmental-friendly Materials and Ecological Remediation, Guangxi Key Laboratory of Advanced Structural Materials and Carbon Neutralization, School of Materials and Environment, Guangxi Minzu University, Nanning, 530006, China.

Guangxi Colleges and Universities Key Laboratory of Environmental-friendly Materials and Ecological Remediation, Guangxi Key Laboratory of Advanced Structural Materials and Carbon Neutralization, School of Materials and Environment, Guangxi Minzu University, Nanning, 530006, China; Guangxi Research Institute of Chemical Industry Co., Ltd., Nanning, 530001, China.

出版信息

Environ Res. 2025 Feb 15;267:120747. doi: 10.1016/j.envres.2024.120747. Epub 2024 Dec 31.

Abstract

Water pollution caused by antibiotics is considered a major and growing issue. To address this challenge, high-performance copper vanadate-based biochar (CuVO/BC) nanocomposite photocatalysts were prepared to develop an efficient visible light-driven photocatalytic system for the remediation of tetracycline (TC) contaminated water. The effects of photocatalyst mass, solution pH, pollutant concentration, and common anions on the TC degradation were investigated in detail. Analytical techniques indicated that the CuVO exhibited a nanobelt-like structure with a uniform distribution on the wrinkled biochar surface. The XRD spectrum confirmed that the as-prepared nanomaterial was composed of CuVO(OH)·2HO. Meanwhile, XPS analysis revealed that copper was present in two forms: monovalent and divalent, while vanadium remained pentavalent. The CuVO/BC exhibited excellent stability and high visible light photocatalytic activity towards TC degradation over a wide pH range. The presence of SO, HPO, CO, and citric acid inhibited the degradation process due to the consuming of photogenerated h and •OH, while Cl enhanced the efficiency of photocatalytic reactions due to generating chlorine oxidizing species. The CuVO/BC showed lower electron-hole recombination rate, more effective separation of photogenerated carriers, lower charge transfer resistance, and higher visible light absorption capacity comparing to pure CuVO by the addition of BC, thus improving the overall photocatalytic performance. In terms of oxidation mechanism, the EPR test and quenching experiment revealed that the contribution of the active species to the degradation of TC followed the order h > O > •OH > •O. Through the application of machine learning models to analyse the influencing factors of photocatalytic processes, it was discovered that the GBDT model exhibited optimal reliability for the photocatalytic system, and the simulation results were in agreement with the experimental findings.

摘要

抗生素造成的水污染被认为是一个重大且日益严重的问题。为应对这一挑战,制备了高性能的钒酸铜基生物炭(CuVO/BC)纳米复合光催化剂,以开发一种高效的可见光驱动光催化系统,用于修复四环素(TC)污染的水。详细研究了光催化剂质量、溶液pH值、污染物浓度和常见阴离子对TC降解的影响。分析技术表明,CuVO呈现出纳米带状结构,在起皱的生物炭表面均匀分布。XRD光谱证实,所制备的纳米材料由CuVO(OH)·2H₂O组成。同时,XPS分析表明铜以一价和二价两种形式存在,而钒保持五价。CuVO/BC在较宽的pH范围内对TC降解表现出优异的稳定性和高可见光光催化活性。SO₄²⁻、HPO₄²⁻、CO₃²⁻和柠檬酸的存在由于消耗光生空穴和•OH而抑制了降解过程,而Cl⁻由于产生氯氧化物种而提高了光催化反应效率。与纯CuVO相比,通过添加BC,CuVO/BC显示出更低的电子-空穴复合率、光生载流子更有效的分离、更低的电荷转移电阻和更高的可见光吸收能力,从而提高了整体光催化性能。在氧化机理方面,EPR测试和猝灭实验表明,活性物种对TC降解的贡献顺序为h⁺ > O₂ > •OH > •O₂⁻。通过应用机器学习模型分析光催化过程的影响因素,发现GBDT模型对光催化系统表现出最佳的可靠性,模拟结果与实验结果一致。

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