Currently, enhancing the catalytic activity of Zero-Valent Iron (ZVI) and improving the mineralization rate of pollutants remain significant challenges in ZVI application. In this study, the s-Fe0@Cu-Pd catalysts were synthesized using six different copper sources to activate peroxymonosulfate (PMS) for norfloxacin (NOR) degradation. SEM images revealed morphology variations in the s-Fe0@Cu-Pd trimetals, with the T-Cl (synthesized using CuCl2) exhibiting the largest specific surface area and pore volume. XPS characterization and DFT analyses indicated that anions significantly influenced the Cu(I)/Cu(II) ratio in s-Fe0@Cu-Pd trimetals. Raman spectroscopy confirmed the generation of CuCl and Cu2O on the catalyst surface in the presence of chloride ions, with copper valence state was effectively modulated by increasing the amount of chloride ion during synthesis. Among the six s-Fe0@Cu-Pd/PMS systems, T-Cl/PMS demonstrated the highest catalytic activity, achieving a 96.25 % NOR removal efficiency under optimized conditions. EPR characterization and radical scavenging experiments elucidated the coexistence of SO4•−, •OH, O2•− and 1O2, with SO4•− was identified as the predominant active radical. Furthermore, mechanism investigations into NOR degradation by the T-Cl/PMS system facilitated the proposal of potential degradation pathways. The s-Fe0@Cu-Pd/PMS system demonstrates considerable potential for the advanced treatment of recalcitrant pollutants in aqueous environments.

中文翻译：

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通过氯改性铁基三金属有效激活 PMS 以实现诺氟沙星解毒和矿化：对铜价态的深度调节


目前，提高零价铁 （ZVI） 的催化活性和提高污染物矿化速率仍然是零价铁应用中的重大挑战。在本研究中，使用六种不同的铜源合成了 s-Fe0@Cu-Pd 催化剂，以活化过氧一硫酸盐 （PMS） 用于诺氟沙星 （NOR） 降解。SEM 图像揭示了 s-Fe0@Cu-Pd 三金属的形态变化，其中 T-Cl（使用 CuCl2 合成）表现出最大的比表面积和孔体积。XPS 表征和 DFT 分析表明，阴离子显著影响 s-Fe0@Cu-Pd 三金属中的 Cu（I）/Cu（II） 比值。拉曼光谱证实，在氯离子存在下，催化剂表面生成了 CuCl 和 Cu2O，在合成过程中通过增加氯离子的量有效地调节了铜价态。在 6 个 s-Fe0@Cu-Pd/PMS 系统中，T-Cl/PMS 表现出最高的催化活性，在优化条件下实现了 96.25% 的 NOR 去除效率。EPR 表征和自由基清除实验阐明了 SO4•-、•OH、O2•- 和 1O2 共存，其中 SO4•− 被确定为主要的活性自由基。此外，T-Cl/PMS 系统对 NOR 降解的机制研究促进了潜在降解途径的提出。s-Fe0@Cu-Pd/PMS 系统在先进处理水性环境中的顽固污染物方面显示出相当大的潜力。