Chlorpyrifos (CPF) is one of the most widely used pesticides in the world, and its improper use will cause serious pollution to ecological safety and water environment. There is an urgent need for an efficient, environmental-friendly, and cost-effective removal technology. ZVI@Al (mixed zero-valent iron and aluminum) is a potential technology for degrading CPF by combining it with ZVI (zero-valent iron), ZVAl (zero-valent aluminum) and ZVI@Al (supported zero-valent iron and aluminum). This technology can efficiently degrade CPF, achieving a removal rate of 93.47% and a complete mineralization rate of 62.15% at the concentration of 10 mg/L, pH of 7.0, temperature of 25 °C, and ZVI@Al dosage of 0.30 g/L, and can effectively alleviate the interference of anions and HA in actual wastewater. The elemental evolution and solution composition of ZVI@Al indicates that the material has an activation effect on O in solution. The existence of •OH and O in the reaction and the degradation of CPF were confirmed by quenching experiments and electron spin resonance. In addition, Al provides electronic output for ZVI, which prolongs the life of ZVI and guarantees the sustainable degradation ability of ZVI@Al. The detection of pollutant degradation intermediates initially proposed two degradation pathways, the cleavage of C–O–P bonds, and the substitution of S and methyl groups. DFT calculation proves that pathway Ⅰ is more favorable in the reaction process, and the toxicity assessment also shows that the product toxicity of pathway Ⅰ is slightly lower than that of pathway Ⅱ. Finally, ZVI@Al has strong reusability, the removal rate of CPF in the fourth reuse process can still reach 80.91%, and the material recovery in the fifth time can still reach 80.46%. This study proposed a mechanism to degrade CPF using cheap bimetallic particles and confirmed its feasibility through practice and theory. These findings not only provide an efficient, green, and economical pollution control technology for the removal of organophosphorus pesticides in the wastewater but also provide new ideas for the application of ZVI-based bimetallic materials in the field of environmental governance.

中文翻译：

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协同混合 Fe–Al（ZVI@Almix）双金属粒子对毒死蜱的持续高效降解：性能与机理

毒死蜱（CPF）是世界上使用最广泛的农药之一，其使用不当会对生态安全和水环境造成严重污染。迫切需要一种高效、环保、经济的去除技术。 ZVI@Al（混合零价铁和铝）是一种潜在的降解 CPF 的技术，将其与 ZVI（零价铁）、ZVAl（零价铝）和 ZVI@Al（负载型零价铁和铝）相结合）。该技术可高效降解CPF，在浓度10 mg/L、pH 7.0、温度25℃、ZVI@Al用量0.30 g/时，去除率达93.47%，完全矿化率达62.15%。 L，并能有效减轻实际废水中阴离子和HA的干扰。 ZVI@Al的元素演化和溶液组成表明该材料对溶液中的O具有活化作用。通过猝灭实验和电子自旋共振证实了反应中•OH和O的存在以及CPF的降解。此外，Al为ZVI提供电子输出，延长了ZVI的寿命，保证了ZVI@Al的可持续降解能力。污染物降解中间体的检测最初提出了两种降解途径，即C-O-P键的断裂以及S和甲基的取代。 DFT计算证明途径Ⅰ在反应过程中更为有利，毒性评估也表明途径Ⅰ的产物毒性略低于途径Ⅱ。最后，ZVI@Al具有很强的可重复使用性，在第四次重复使用过程中CPF的去除率仍然可以达到80.91%，并且在第五次重复使用时材料回收率仍然可以达到80.46%。本研究提出了一种利用廉价双金属颗粒降解 CPF 的机制，并通过实践和理论证实了其可行性。这些发现不仅为废水中有机磷农药的去除提供了一种高效、绿色、经济的污染控制技术，而且为ZVI基双金属材料在环境治理领域的应用提供了新思路。