Jiefei Cao, Siyuan Feng, Alireza Arhami Dolatabad, Yue Zhi, Baolin Deng, Caihong Liu, Xueyan Lyu, Charlotte S.Q. Christensen, Joseph J. Pignatello, Pan Ni, Shihong Lin, Zongsu Wei, Feng Xiao
{"title":"颗粒活性炭从反渗透和纳滤盐水中去除PFAS:盐度效应的热力学见解","authors":"Jiefei Cao, Siyuan Feng, Alireza Arhami Dolatabad, Yue Zhi, Baolin Deng, Caihong Liu, Xueyan Lyu, Charlotte S.Q. Christensen, Joseph J. Pignatello, Pan Ni, Shihong Lin, Zongsu Wei, Feng Xiao","doi":"10.1016/j.watres.2025.123758","DOIUrl":null,"url":null,"abstract":"We explored an underexplored area in water treatment by examining the removal of per- and polyfluoroalkyl substances (PFAS) from reverse osmosis/nanofiltration (RO/NF) brine. We first compared multiple RO/NF membranes, revealing that DK and NF270 showed sub-optimal removal (<90%) of C4−C8 PFAS, SW30 had low flux (<15 L/m<sup>2</sup>/h at 8 bar), and NFX exhibited significant adsorption of perfluorosulfonic acids (e.g., 8 µmol/m<sup>2</sup>). To address the PFAS-enriched brine generated from membrane treatment, we further evaluated activated carbon (GAC) and anion-exchange (AIX) resin, both of which efficiently removed moderate- and long-chain PFAS from brine. Although AIX outperformed GAC, the ion exchange contribution was small for short-chain PFAS like perfluorobutanoic acid (PFBA, C4) but increased with chain length, driven by the hydrophobic effect facilitating the migration to near-surface regions of resins. Equilibrium batch experiments and thermodynamic modeling revealed a disproportionate salinity impact on PFAS adsorption by GAC, with short-chain PFAS (e.g., PFBA) experiencing more pronounced adsorption reduction than longer-chained homologs as NaCl concentrations increased. This reduction was driven by a significant change in a free energy component unrelated to the hydrophobic or electrostatic interactions, likely due to the competitive adsorption of Cl<sup>−</sup> ions and short-chain PFAS anions or the formation of hydration shells around Na<sup>+</sup> and Cl<sup>−</sup> ions, obstructing the pathways for weakly hydrophobic PFAS (e.g., PFBA) within the GAC pore network. The salting-out effect was found to be unimportant. This study provides new insights into salinity-dependent sorptive removal of PFAS from high-ionic-strength water such as RO/NF brine.","PeriodicalId":443,"journal":{"name":"Water Research","volume":"43 1","pages":""},"PeriodicalIF":11.4000,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"PFAS Removal from Reverse Osmosis and Nanofiltration Brine by Granular Activated Carbon: Thermodynamic Insights into Salinity Effects\",\"authors\":\"Jiefei Cao, Siyuan Feng, Alireza Arhami Dolatabad, Yue Zhi, Baolin Deng, Caihong Liu, Xueyan Lyu, Charlotte S.Q. Christensen, Joseph J. Pignatello, Pan Ni, Shihong Lin, Zongsu Wei, Feng Xiao\",\"doi\":\"10.1016/j.watres.2025.123758\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"We explored an underexplored area in water treatment by examining the removal of per- and polyfluoroalkyl substances (PFAS) from reverse osmosis/nanofiltration (RO/NF) brine. We first compared multiple RO/NF membranes, revealing that DK and NF270 showed sub-optimal removal (<90%) of C4−C8 PFAS, SW30 had low flux (<15 L/m<sup>2</sup>/h at 8 bar), and NFX exhibited significant adsorption of perfluorosulfonic acids (e.g., 8 µmol/m<sup>2</sup>). To address the PFAS-enriched brine generated from membrane treatment, we further evaluated activated carbon (GAC) and anion-exchange (AIX) resin, both of which efficiently removed moderate- and long-chain PFAS from brine. Although AIX outperformed GAC, the ion exchange contribution was small for short-chain PFAS like perfluorobutanoic acid (PFBA, C4) but increased with chain length, driven by the hydrophobic effect facilitating the migration to near-surface regions of resins. Equilibrium batch experiments and thermodynamic modeling revealed a disproportionate salinity impact on PFAS adsorption by GAC, with short-chain PFAS (e.g., PFBA) experiencing more pronounced adsorption reduction than longer-chained homologs as NaCl concentrations increased. This reduction was driven by a significant change in a free energy component unrelated to the hydrophobic or electrostatic interactions, likely due to the competitive adsorption of Cl<sup>−</sup> ions and short-chain PFAS anions or the formation of hydration shells around Na<sup>+</sup> and Cl<sup>−</sup> ions, obstructing the pathways for weakly hydrophobic PFAS (e.g., PFBA) within the GAC pore network. The salting-out effect was found to be unimportant. 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PFAS Removal from Reverse Osmosis and Nanofiltration Brine by Granular Activated Carbon: Thermodynamic Insights into Salinity Effects
We explored an underexplored area in water treatment by examining the removal of per- and polyfluoroalkyl substances (PFAS) from reverse osmosis/nanofiltration (RO/NF) brine. We first compared multiple RO/NF membranes, revealing that DK and NF270 showed sub-optimal removal (<90%) of C4−C8 PFAS, SW30 had low flux (<15 L/m2/h at 8 bar), and NFX exhibited significant adsorption of perfluorosulfonic acids (e.g., 8 µmol/m2). To address the PFAS-enriched brine generated from membrane treatment, we further evaluated activated carbon (GAC) and anion-exchange (AIX) resin, both of which efficiently removed moderate- and long-chain PFAS from brine. Although AIX outperformed GAC, the ion exchange contribution was small for short-chain PFAS like perfluorobutanoic acid (PFBA, C4) but increased with chain length, driven by the hydrophobic effect facilitating the migration to near-surface regions of resins. Equilibrium batch experiments and thermodynamic modeling revealed a disproportionate salinity impact on PFAS adsorption by GAC, with short-chain PFAS (e.g., PFBA) experiencing more pronounced adsorption reduction than longer-chained homologs as NaCl concentrations increased. This reduction was driven by a significant change in a free energy component unrelated to the hydrophobic or electrostatic interactions, likely due to the competitive adsorption of Cl− ions and short-chain PFAS anions or the formation of hydration shells around Na+ and Cl− ions, obstructing the pathways for weakly hydrophobic PFAS (e.g., PFBA) within the GAC pore network. The salting-out effect was found to be unimportant. This study provides new insights into salinity-dependent sorptive removal of PFAS from high-ionic-strength water such as RO/NF brine.
期刊介绍:
Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include:
•Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management;
•Urban hydrology including sewer systems, stormwater management, and green infrastructure;
•Drinking water treatment and distribution;
•Potable and non-potable water reuse;
•Sanitation, public health, and risk assessment;
•Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions;
•Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment;
•Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution;
•Environmental restoration, linked to surface water, groundwater and groundwater remediation;
•Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts;
•Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle;
•Socio-economic, policy, and regulations studies.