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可见光驱动的过一硫酸盐在坚固的 TiO2 基纳米颗粒上的活化用于磺胺甲恶唑的有效去除。

Visible-light-driven peroxymonosulfate activation by robust TiO-base nanoparticles for efficient removal of sulfamethoxazole.

机构信息

School of Transportation and Civil Engineering, Foshan University, Foshan, 528000, China.

School of Environmental and Chemical Engineering, Foshan University, Foshan, 528000, China.

出版信息

Environ Pollut. 2023 Oct 1;334:122150. doi: 10.1016/j.envpol.2023.122150. Epub 2023 Jul 8.

Abstract

In this study, a novel bimetallic Co-Mo-TiO nanomaterial was fabricated through a simple two-step method, and applied as photocatalyst to activate peroxymonosulfate (PMS) with high efficiency for sulfamethoxazole (SMX) removal under visible light. Nearly 100% of SMX was degraded within 30 min in Vis/Co-Mo-TiO/PMS system, and its kinetic reaction rate constant (0.099 min) was 24.8 times higher compare with the Vis/TiO/PMS system (0.014 min). Moreover, the quenching experiments and the electronic spin resonance analysis results confirmed that both O and SO were the dominant active species in the optimal system, and the redox cycles of Co/Co and Mo/Mo promoted the generation of the radicals during the PMS activation process. Additionally, the Vis/Co-Mo-TiO/PMS system exhibited a wide working pH range, superior catalytic performance toward different pollutants and excellent stability with 92.8% SMX removal capacity retention after three consecutive cycles. The result of density functional theory (DFT) suggested that Co-Mo-TiO exhibited a high affinity for PMS adsorption, as indicated by the length O-O bond from PMS and the E of the catalysts. Finally, the possible degradation pathway of SMX in optimal system was proposed through intermediate identification and DFT calculation, and a toxicity assessment of the by-products was also conducted.

摘要

在这项研究中,通过一种简单的两步法制备了一种新型的双金属 Co-Mo-TiO 纳米材料,并将其作为光催化剂应用于高效激活过一硫酸盐 (PMS) 以去除可见光下的磺胺甲恶唑 (SMX)。在 Vis/Co-Mo-TiO/PMS 体系中,SMX 在 30 分钟内几乎完全降解,其动力学反应速率常数 (0.099 min) 是 Vis/TiO/PMS 体系 (0.014 min) 的 24.8 倍。此外,猝灭实验和电子自旋共振分析结果证实,O 和 SO都是最佳体系中的主要活性物质,Co/Co 和 Mo/Mo 的氧化还原循环促进了 PMS 活化过程中自由基的生成。此外,Vis/Co-Mo-TiO/PMS 体系具有较宽的工作 pH 范围,对不同污染物表现出优异的催化性能和良好的稳定性,经过三次连续循环后,SMX 的去除率仍保持在 92.8%。密度泛函理论 (DFT) 的结果表明,Co-Mo-TiO 对 PMS 吸附具有很高的亲和力,这可以从 PMS 的 O-O 键长和催化剂的 E 来表示。最后,通过中间产物鉴定和 DFT 计算提出了最佳体系中 SMX 的可能降解途径,并对副产物进行了毒性评估。

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