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比较无机硅和有机硅改性活性炭对全氟烷基物质的吸附性能。

Comparison of perfluoroalkyl substance adsorption performance by inorganic and organic silicon modified activated carbon.

机构信息

Key Laboratory of Drinking Water Science and Technology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, 100085, China; University of Chinese Academy of Sciences, Beijing, 100049, China.

Key Laboratory of Drinking Water Science and Technology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, 100085, China.

出版信息

Water Res. 2024 Aug 15;260:121919. doi: 10.1016/j.watres.2024.121919. Epub 2024 Jun 10.

Abstract

Owing to the persistence and increasingly stringent regulations of perfluoroalkyl substances (PFAS), it is necessary to improve their adsorption capacities using activated carbon (AC). However, their adsorption capacities are suppressed by dissolved organic matter (DOM). In this study, two ACs modified with organic silicon (C-OS) and inorganic silicon (C-IS) were synthesized and used for the adsorption of PFAS in raw water (RW). The results showed that the PFAS adsorption capacity of C-IS was much less influenced by DOM than that of the original AC (C-virgin). In RW, perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS) adsorption capacities on C-IS were 15.08 and 3.65 times higher than those on C-virgin, respectively. DOM had less influence on the PFOA and PFOS adsorption kinetics of C-IS than C-OS and C-virgin. Under multi-PFAS condition, C-IS also exhibited slower desorption of short-chain PFAS and breakthrough in batch and column tests, respectively. Characterization of the ACs before and after adsorption and independent gradient modelling indicated that hydrogen bond interactions between the O-Si of C-IS and the -COOH or -CSOH groups of PFAS contributed to PFAS adsorption. Density functional theory calculations demonstrated that the adsorption energy of C-IS was much lower than that of C-OS and C-virgin. The arrangement of PFAS molecules on C-OS was chaotic owing to the hydrophobic siloxane chain, whereas the arrangement of PFAS on C-IS was orderly in multi-layer or semi-micelle status and more favorable to PFAS adsorption. This study provides a new strategy for avoiding adverse effects of DOM on PFAS adsorption.

摘要

由于全氟烷基物质 (PFAS) 的持久性和日益严格的法规,有必要使用活性炭 (AC) 来提高它们的吸附能力。然而,它们的吸附能力会受到溶解有机物 (DOM) 的抑制。在这项研究中,合成了两种用有机硅 (C-OS) 和无机硅 (C-IS) 改性的活性炭,并将其用于原水 (RW) 中 PFAS 的吸附。结果表明,C-IS 的 PFAS 吸附能力受 DOM 的影响远小于原始 AC (C-virgin)。在 RW 中,C-IS 对全氟辛酸 (PFOA) 和全氟辛烷磺酸 (PFOS) 的吸附容量分别比 C-virgin 高 15.08 倍和 3.65 倍。DOM 对 C-IS 的 PFOA 和 PFOS 吸附动力学的影响小于 C-OS 和 C-virgin。在多 PFAS 条件下,C-IS 在批量和柱试验中也表现出较慢的短链 PFAS 解吸和穿透。AC 吸附前后的表征和独立梯度建模表明,C-IS 的 O-Si 与 PFAS 的 -COOH 或 -CSOH 基团之间的氢键相互作用有助于 PFAS 的吸附。密度泛函理论计算表明,C-IS 的吸附能远低于 C-OS 和 C-virgin。由于疏水性硅氧烷链,C-OS 上 PFAS 分子的排列混乱,而 C-IS 上 PFAS 的排列有序,呈多层或半胶束状态,更有利于 PFAS 的吸附。本研究为避免 DOM 对 PFAS 吸附的不利影响提供了一种新策略。

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