基于自旋态调谐优化 LaCoO3 的三维电子结构,提高四环素降解过程中的光-芬顿活性

IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Journal of Colloid and Interface Science Pub Date : 2024-09-06 DOI:10.1016/j.jcis.2024.09.024
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引用次数: 0

摘要

滥用抗生素造成的水污染对环境和人类健康产生了重大危害。光-芬顿过程是目前去除水中抗生素最有效的方法,但它面临着对可见光响应不足、光生电子的产量和利用率低、电子传输慢等挑战。本研究在光-芬顿过程中引入了自旋态调节,通过掺杂 Ce 置换来调节 Co3+ 的自旋态。在光-芬顿体系中,中间自旋态的 Ce-LaCoO3 在 120 分钟内可降解 91.6% 的四环素,比低自旋态的 LaCoO3 高出 15.2%。降解效果提高的原因在于中旋态的 Ce-LaCoO3 具有更低的带隙、更好的电荷转移能力和更强的 H2O2 吸附能力,可以加速 Co2+/Co3+ 的氧化还原循环,促进 -OH 的生成。这项研究为合成高效光-芬顿材料以有效处理抗生素废水提供了一种独特的策略。
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Optimizing 3d electronic structure of LaCoO3 based on spin state tuning for enhancing photo-Fenton activity on tetracycline degradation

The water pollution caused by the abuse of antibiotics has significant harmful effects on the environment and human health. The photo-Fenton process is currently the most effective method for removing antibiotics from water, but it encounters challenges such as inadequate response to visible light, low yield and utilization of photogenerated electrons, and slow electron transport. In this study, spin state regulation was introduced into the photo-Fenton process, and the spin state of Co3+ was regulated through Ce displacement doping. The intermediate-spin state Ce-LaCoO3 could degrade 91.6 % of tetracycline within 120 min in the photo-Fenton system, which is 15.2 % higher than that of low-spin state LaCoO3. The improved degradation effect is attributed to the reasons that Ce-LaCoO3 in the intermediate-spin state have lower band gap, better charge transfer ability, and stronger adsorption capacity of H2O2, which can accelerate the redox cycle of Co2+/Co3+ and promote the generation of ·OH. This study presents a unique strategy for synthesizing efficient photo-Fenton materials to treat antibiotic wastewater effectively.

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来源期刊
CiteScore
16.10
自引率
7.10%
发文量
2568
审稿时长
2 months
期刊介绍: The Journal of Colloid and Interface Science publishes original research findings on the fundamental principles of colloid and interface science, as well as innovative applications in various fields. The criteria for publication include impact, quality, novelty, and originality. Emphasis: The journal emphasizes fundamental scientific innovation within the following categories: A.Colloidal Materials and Nanomaterials B.Soft Colloidal and Self-Assembly Systems C.Adsorption, Catalysis, and Electrochemistry D.Interfacial Processes, Capillarity, and Wetting E.Biomaterials and Nanomedicine F.Energy Conversion and Storage, and Environmental Technologies
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