Yutong He, Xiao Tan, Chunrong Yu, Kehan Liu, Chen Zhou, Yutong Zhu, Lam Leung, Stepen Breske, Timothy E. Hopkins, Attila Tottszer, Andrew Matheson, Andrew K. Whittaker and Cheng Zhang*,
{"title":"部分氟化大分子捕获PFAS:氟化基团结构的影响","authors":"Yutong He, Xiao Tan, Chunrong Yu, Kehan Liu, Chen Zhou, Yutong Zhu, Lam Leung, Stepen Breske, Timothy E. Hopkins, Attila Tottszer, Andrew Matheson, Andrew K. Whittaker and Cheng Zhang*, ","doi":"10.1021/acs.macromol.5c01012","DOIUrl":null,"url":null,"abstract":"<p >In this work, we prepare and evaluate four ion exchange resins with varying fluorinated segments for per- and polyfluoroalkyl substance (PFAS) removal (i.e., PFAS-based <i>Sorb-PFPE+</i> (perfluoropolyether) and <i>Sorb-NFN+</i> (nonadecafluoro-1-decanol) as well as non-PFAS-based <i>Sorb-PFS+</i> (pentafluorostyrene) and <i>Sorb-DFE+</i> (2,2-difluoroethanol)), with a particular interest being the removal of (ultra)short-chain PFAS. Among all these types of fluorinated sorbents, <i>Sorb-PFS+</i> achieves removal performance comparable to the previously reported highly efficient <i>Sorb-PFPE+</i> sorbent. <i>Sorb-PFS+</i> demonstrates >90% removal of all tested PFAS, including (ultra)short-chain perfluoropropionic acid (PFPrA, 97.7%), perfluoro-2-methoxyacetic acid (PFMOAA, 98.8%), perfluoro-2-methoxypropanoic acid (PMPA, 99.1%), and difluoroacetic acid (DFA, 92.2%). A further sorption kinetic trial evidenced its rapid, efficient, and nonreversible removal of (ultra)short-chain PFAS within 5 min. Sorption capacity was estimated using the Langmuir model, with DFA, PFPrA, PFMOAA, and PMPA achieving 275.2, 357.4, 475.7, and 758.7 mg/g, respectively. No significant drop in sorbent performance was observed over five repeated sorption and desorption cycles, validating the great regeneration and reusability of <i>Sorb-PFS+</i>. In two real water matrices, <i>Sorb-PFS+</i> also demonstrates commendable performance, with the removal of PFMOAA and PMPA achieving >93% in the landfill leachate and >99% in sewage water, outperforming the commercially available PFA694E sorbent. This work provides important insights into the development of fluorinated but non-PFAS sorbents, emphasizing the potentials of non-PFAS alternatives to meet future regulatory requirements while retaining the benefits of fluorine–fluorine interactions, thus contributing to a greener and more sustainable future.</p>","PeriodicalId":51,"journal":{"name":"Macromolecules","volume":"58 14","pages":"7050–7061"},"PeriodicalIF":5.2000,"publicationDate":"2025-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Capturing PFAS with Partly Fluorinated Macromolecules: The Influence of the Fluorinated Group Structure\",\"authors\":\"Yutong He, Xiao Tan, Chunrong Yu, Kehan Liu, Chen Zhou, Yutong Zhu, Lam Leung, Stepen Breske, Timothy E. Hopkins, Attila Tottszer, Andrew Matheson, Andrew K. Whittaker and Cheng Zhang*, \",\"doi\":\"10.1021/acs.macromol.5c01012\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >In this work, we prepare and evaluate four ion exchange resins with varying fluorinated segments for per- and polyfluoroalkyl substance (PFAS) removal (i.e., PFAS-based <i>Sorb-PFPE+</i> (perfluoropolyether) and <i>Sorb-NFN+</i> (nonadecafluoro-1-decanol) as well as non-PFAS-based <i>Sorb-PFS+</i> (pentafluorostyrene) and <i>Sorb-DFE+</i> (2,2-difluoroethanol)), with a particular interest being the removal of (ultra)short-chain PFAS. Among all these types of fluorinated sorbents, <i>Sorb-PFS+</i> achieves removal performance comparable to the previously reported highly efficient <i>Sorb-PFPE+</i> sorbent. <i>Sorb-PFS+</i> demonstrates >90% removal of all tested PFAS, including (ultra)short-chain perfluoropropionic acid (PFPrA, 97.7%), perfluoro-2-methoxyacetic acid (PFMOAA, 98.8%), perfluoro-2-methoxypropanoic acid (PMPA, 99.1%), and difluoroacetic acid (DFA, 92.2%). A further sorption kinetic trial evidenced its rapid, efficient, and nonreversible removal of (ultra)short-chain PFAS within 5 min. Sorption capacity was estimated using the Langmuir model, with DFA, PFPrA, PFMOAA, and PMPA achieving 275.2, 357.4, 475.7, and 758.7 mg/g, respectively. No significant drop in sorbent performance was observed over five repeated sorption and desorption cycles, validating the great regeneration and reusability of <i>Sorb-PFS+</i>. In two real water matrices, <i>Sorb-PFS+</i> also demonstrates commendable performance, with the removal of PFMOAA and PMPA achieving >93% in the landfill leachate and >99% in sewage water, outperforming the commercially available PFA694E sorbent. 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Capturing PFAS with Partly Fluorinated Macromolecules: The Influence of the Fluorinated Group Structure
In this work, we prepare and evaluate four ion exchange resins with varying fluorinated segments for per- and polyfluoroalkyl substance (PFAS) removal (i.e., PFAS-based Sorb-PFPE+ (perfluoropolyether) and Sorb-NFN+ (nonadecafluoro-1-decanol) as well as non-PFAS-based Sorb-PFS+ (pentafluorostyrene) and Sorb-DFE+ (2,2-difluoroethanol)), with a particular interest being the removal of (ultra)short-chain PFAS. Among all these types of fluorinated sorbents, Sorb-PFS+ achieves removal performance comparable to the previously reported highly efficient Sorb-PFPE+ sorbent. Sorb-PFS+ demonstrates >90% removal of all tested PFAS, including (ultra)short-chain perfluoropropionic acid (PFPrA, 97.7%), perfluoro-2-methoxyacetic acid (PFMOAA, 98.8%), perfluoro-2-methoxypropanoic acid (PMPA, 99.1%), and difluoroacetic acid (DFA, 92.2%). A further sorption kinetic trial evidenced its rapid, efficient, and nonreversible removal of (ultra)short-chain PFAS within 5 min. Sorption capacity was estimated using the Langmuir model, with DFA, PFPrA, PFMOAA, and PMPA achieving 275.2, 357.4, 475.7, and 758.7 mg/g, respectively. No significant drop in sorbent performance was observed over five repeated sorption and desorption cycles, validating the great regeneration and reusability of Sorb-PFS+. In two real water matrices, Sorb-PFS+ also demonstrates commendable performance, with the removal of PFMOAA and PMPA achieving >93% in the landfill leachate and >99% in sewage water, outperforming the commercially available PFA694E sorbent. This work provides important insights into the development of fluorinated but non-PFAS sorbents, emphasizing the potentials of non-PFAS alternatives to meet future regulatory requirements while retaining the benefits of fluorine–fluorine interactions, thus contributing to a greener and more sustainable future.
期刊介绍:
Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.