新型FeS@LH材料的制备及其活化过二硫酸盐(PDS)降解吡虫啉(IMI)的效能和机制研究

谢祎林; 董鲁钰; 王云飞; 张渺; 胡志欣; 王雪丽

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中国环境科学 ›› 2025, Vol. 45 ›› Issue (10) : 5525-5538.

水污染与控制

新型FeS@LH材料的制备及其活化过二硫酸盐(PDS)降解吡虫啉(IMI)的效能和机制研究

谢祎林¹, 董鲁钰¹, 王云飞¹, 张渺¹, 胡志欣¹, 王雪丽^1,2

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Preparation of novel FeS@LH materials and their efficiency and mechanism of activation of imidacloprid (IMI) degradation by perdisulfite (PDS)

XIE Yi-lin¹, DONG Lu-yu¹, WANG Yun-fei¹, ZHANG Miao¹, HU Zhi-xin¹, WANG Xue-li^1,2

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摘要

合成了一种新型铁基纳米复合木质素水凝胶(FeS@LH),并将其应用于过二硫酸盐(PDS)的活化.通过材料表征,发现该木质素水凝胶独特的三维(3D)结构有助于硫化纳米零价铁颗粒(FeS颗粒)的分散,增加FeS的暴漏位点.这种3D结构不仅为FeS、PDS和污染物提供了更多附着位点,还加速了FeS与PDS之间的电子转移,从而促进污染物降解.实验结果表明,FeS@LH在PDS活化方面表现出优异性能,在0.1g/L催化剂和1mmol/LPDS的条件下,120min内可完全降解10mg/L的吡虫啉(IMI).淬灭实验和电子自旋共振(ESR)光谱分析表明,在FeS@LH/PDS体系中,SO4·-和OH·是IMI降解的主要活性物种.此外,FeS@LH在存在无机阴离子和天然有机质(HA)的条件下仍能有效活化PDS降解IMI.通过液质联用(UPLC-MS-MS)系统鉴定了IMI的降解产物,并提出了两种可能的降解路径.毒性预测结果表明,IMI最终可转化为无毒产物.FeS@LH在3次循环测试后仍能保持一定的降解效率,同时表现出较低金属浸出特性.研究结果为开发高效降解农药类污染物提供了新的思路.

Abstract

In this paper, a novel iron-based nanocomposite lignin hydrogel (FeS@LH) was synthesized and applied to the activation of perdisulfate (PDS). Through the characterization of the material, it is found that the unique three-dimensional (3D) structure of the lignin hydrogel is helpful to the dispersion of sulfide nano-zero-valent iron particles (FeS particles) and increase the leakage site of FeS. This three-dimensional structure not only provides more attachment sites for FeS, PDS and pollutants, but also accelerates the electron transfer between FeS and PDS, thus promoting the degradation of pollutants. The experimental results show that FeS@LH has excellent performance in PDS activation. Under the condition of 0.1g/L catalyst and 1mmol/L PDS, 10mg/L IMI (100mL) can be completely degraded in 120minutes. Quenching experiments and electron spin resonance (ESR) spectra show that SO₄^·- and OH· are the main active species for IMI degradation in FeS@LH/PDS system. In addition, FeS@LH can effectively activate PDS to degrade IMI in the presence of inorganic anions and natural organic matter (HA).The degradation products of IMI were identified by liquid chromatography-mass spectrometry (UPLC-MS-MS) system, and two possible degradation pathways were proposed. The toxicity prediction results show that IMI can eventually be converted into a non-toxic product. FeS@LH was able to maintain a certain degradation efficiency after three cycles of testing, while exhibiting low metal leaching characteristics. Study results provide new ideas for the development of efficient degradation of pesticide pollutants.

导出引用

谢祎林, 董鲁钰, 王云飞, 张渺, 胡志欣, 王雪丽. 新型FeS@LH材料的制备及其活化过二硫酸盐(PDS)降解吡虫啉(IMI)的效能和机制研究[J]. 中国环境科学. 2025, 45(10): 5525-5538

XIE Yi-lin, DONG Lu-yu, WANG Yun-fei, ZHANG Miao, HU Zhi-xin, WANG Xue-li. Preparation of novel FeS@LH materials and their efficiency and mechanism of activation of imidacloprid (IMI) degradation by perdisulfite (PDS)[J]. China Environmental Science. 2025, 45(10): 5525-5538

中图分类号： X703

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