School of Transportation and Civil Engineering, Foshan University, Foshan, 528000, China.
School of Environmental and Chemical Engineering, Foshan University, Foshan, 528000, China.
Environ Pollut. 2023 Oct 1;334:122150. doi: 10.1016/j.envpol.2023.122150. Epub 2023 Jul 8.
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.
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。