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基于集成凝胶混凝-自发浮选工艺的高效、快速和低碳去除微塑料的机制。

Efficient, quick, and low-carbon removal mechanism of microplastics based on integrated gel coagulation-spontaneous flotation process.

机构信息

School of Chemistry and Materials Science, Jiangsu Normal University, Xuzhou 221110, China.

Department of Life Science, Imperial College London, Silwood Park Campus, Berks SL5 7PY, United Kingdom.

出版信息

Water Res. 2024 Aug 1;259:121906. doi: 10.1016/j.watres.2024.121906. Epub 2024 Jun 7.

Abstract

To address the problems of unstable efficiency, long treatment period, and high energy consumption during microplastics (MPs) removal by traditional coagulation-flotation technology, a gel coagulation-spontaneous flotation (GCSF) process is proposed that employs laminarin (LA) as the crosslinker and polyaluminum chloride (PAC)/polyaluminum ferric chloride (PAFC) as the coagulant to remove MPs. Herein, the effects of GCSF chemical conditions on microplastic-humic acid composite pollutants (MP-HAs) removal were investigated, and the removal mechanisms were analyzed through theoretical calculations and floc structure characterization. Results showed that an LA to PAC/PAFC ratio of 2.5:1 achieved the highest removal of HA (86 %) and MPs (93 %-99 %) in short coagulation (< 1 min) and spontaneous flotation (< 9 min) period. PAC-LA exhibited strong removal ability for MP-HAs while PAFC-LA induced fast flotation speed. The peak intensity and peak shift in Fourier-transformed infrared and X-ray photo-electron spectra indicated that the removal mechanisms of MPs include hydrogen bond adsorption and the sweeping effect, mainly relying on -OH/-C = O on the MPs surface and entrapment of gel flocs with a high degree of aggregation, respectively. The extended Derjaguin-Landau-Verwey-Overbeek calculation also revealed that interactions between PAC/PAFC-LA and MP-HAs were mainly polar interaction (hydrogen bonding) and intermolecular attraction interaction (Lifshitz-van der Waals force), and the sweep effect was reflected by intermolecular interaction. In addition, density function theory calculations indicated that -OH in LA mainly adsorbs DO through a double hydrogen bond configuration, and the crosslinking ligand FeO/AlO assists in DO absorption by -OH.

摘要

为解决传统混凝浮选技术去除微塑料(MPs)时效率不稳定、处理周期长、能耗高的问题,提出了一种利用海藻酸钠(LA)作为交联剂、聚合氯化铝(PAC)/聚合氯化铁(PAFC)作为混凝剂的凝胶混凝-自然浮选(GCSF)工艺去除 MPs。在此,考察了 GCSF 化学条件对微塑料-腐殖酸复合污染物(MP-HAs)去除的影响,并通过理论计算和絮体结构表征分析了去除机制。结果表明,LA 与 PAC/PAFC 的比例为 2.5:1 时,在短混凝(<1 min)和自然浮选(<9 min)时间内,对 HA(86%)和 MPs(93%-99%)的去除效果最佳。PAC-LA 对 MP-HAs 具有较强的去除能力,而 PAFC-LA 则诱导快速浮选速度。傅里叶变换红外和 X 射线光电子能谱的峰强度和峰位移表明, MPs 的去除机制包括氢键吸附和清扫效应,主要依赖于 MPs 表面的-OH/-C=O 和高聚合度凝胶絮体的捕获。扩展的德加古因-朗道-维尔韦尔-奥弗贝克计算也表明,PAC/PAFC-LA 与 MP-HAs 之间的相互作用主要是极性相互作用(氢键)和分子间吸引相互作用(Lifshitz-van der Waals 力),清扫效应则反映了分子间相互作用。此外,密度泛函理论计算表明,LA 中的-OH 主要通过双氢键构型吸附 DO,交联配体 FeO/AlO 辅助-OH 吸收 DO。

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