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颗粒活性炭对全氟烷基化学品的吸附:评估粒径对平衡参数的影响以及相关的快速小尺度柱试验缩放假设。

Perfluoroalkyl chemical adsorption by granular activated carbon: Assessment of particle size impact on equilibrium parameters and associated rapid small-scale column test scaling assumptions.

作者信息

Abulikemu Gulizhaer, Pressman Jonathan G, Sorial George A, Sanan Toby T, Haupert Levi M, Burkhardt Jonathan B, Smith Samantha J, Kleiner Eric J, Stebel Eva K, Gray Brooke N, Gastaldo Cameron X, Hughes Esther W, Pedigo Sophia G, Wahman David G

机构信息

Pegasus Technical Services, Inc., Cincinnati, OH 45268, USA; Department of Chemical and Environmental Engineering, University of Cincinnati, Cincinnati, OH 45221, USA.

Center for Environmental Solutions & Emergency Response, U.S. Environmental Protection Agency, Cincinnati, OH 45268, USA.

出版信息

Water Res. 2025 Mar 1;271:122977. doi: 10.1016/j.watres.2024.122977. Epub 2024 Dec 13.

Abstract

Single-solute batch kinetic and isotherm experiments were conducted in Type 1 (18.2 MΩ·cm resistivity) water supplemented with 10 mM carbonate buffer (pH 7.75, 25 °C) for nine drinking water relevant perfluoroalkyl chemicals and three bituminous-coal based granular activated carbons (GACs). Except for perfluorooctane sulfonic acid (PFOS), mass transfer was well represented by a film diffusion model, which estimated a film diffusion coefficient (k). For PFOS, a batch pore and surface diffusion model better represented the data and allowed estimation of both k and a surface diffusion coefficient (D). Adsorption was well described by the Freundlich isotherm, and for a given perfluoroalkyl chemical at equilibrium, the three GACs showed similar solid phase density (q) for a given liquid concentration (c). For each GAC and at c ≤ 1000 ng/L, log q increased linearly with perfluoroalkyl chemical carbon chain length for both perfluoroalkyl carboxylic acids (PFCAs) and perfluoroalkane sulfonic acids (PFSAs). GenX, a perfluoroalkyl ether carboxylic acid containing six carbon atoms, showed similar adsorption with the PFCA perfluorohexanoic acid. The impact of particle size (d) on kinetic and isotherm parameters was investigated: (i) for PFOS, D increased with increasing d, with some overlap in confidence intervals; (ii) for PFSAs, Freundlich K and 1/n showed decreasing and increasing trends, respectively, with increasing d. Potential implications of the d impact were explored with PFOS breakthrough simulations under different rapid small-scale column test conditions where carbon usage rate estimations varied by -49 % to 6 % from the baseline simulation, depending on the d and scaling approach.

摘要

针对9种与饮用水相关的全氟烷基化学品和3种烟煤基颗粒活性炭(GAC),在添加了10 mM碳酸盐缓冲液(pH 7.75,25°C)的1型水(电阻率为18.2 MΩ·cm)中进行了单溶质间歇动力学和等温线实验。除全氟辛烷磺酸(PFOS)外,传质过程可用膜扩散模型很好地描述,该模型可估算膜扩散系数(k)。对于PFOS,间歇孔和表面扩散模型能更好地拟合数据,并可同时估算k和表面扩散系数(D)。吸附过程可用Freundlich等温线很好地描述,对于给定的全氟烷基化学品,在平衡状态下,三种GAC在给定的液相浓度(c)下表现出相似的固相密度(q)。对于每种GAC且在c≤1000 ng/L时,全氟烷基羧酸(PFCA)和全氟烷磺酸(PFSA)的log q均随全氟烷基化学品的碳链长度线性增加。含有6个碳原子的全氟烷基醚羧酸GenX与PFCA全氟己酸表现出相似的吸附特性。研究了粒径(d)对动力学和等温线参数的影响:(i)对于PFOS,D随d的增加而增加,置信区间存在一些重叠;(ii)对于PFSA,Freundlich K和1/n分别随d的增加呈下降和上升趋势。在不同的快速小规模柱试验条件下,通过PFOS穿透模拟探讨了d影响的潜在意义,根据d和缩放方法的不同,碳使用率估计值与基线模拟相比变化范围为-49%至6%。

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