部分氟化大分子捕获PFAS:氟化基团结构的影响

IF 5.2 1区 化学 Q1 POLYMER SCIENCE
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,&nbsp;Xiao Tan,&nbsp;Chunrong Yu,&nbsp;Kehan Liu,&nbsp;Chen Zhou,&nbsp;Yutong Zhu,&nbsp;Lam Leung,&nbsp;Stepen Breske,&nbsp;Timothy E. Hopkins,&nbsp;Attila Tottszer,&nbsp;Andrew Matheson,&nbsp;Andrew K. Whittaker and Cheng Zhang*,&nbsp;","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 &gt;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 &gt;93% in the landfill leachate and &gt;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,&nbsp;Xiao Tan,&nbsp;Chunrong Yu,&nbsp;Kehan Liu,&nbsp;Chen Zhou,&nbsp;Yutong Zhu,&nbsp;Lam Leung,&nbsp;Stepen Breske,&nbsp;Timothy E. Hopkins,&nbsp;Attila Tottszer,&nbsp;Andrew Matheson,&nbsp;Andrew K. Whittaker and Cheng Zhang*,&nbsp;\",\"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 &gt;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 &gt;93% in the landfill leachate and &gt;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\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Macromolecules\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.macromol.5c01012\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"POLYMER SCIENCE\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Macromolecules","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.macromol.5c01012","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"POLYMER SCIENCE","Score":null,"Total":0}
引用次数: 0

摘要

在这项工作中,我们制备并评估了四种具有不同氟化段的离子交换树脂,用于去除全氟和多氟烷基物质(PFAS)(即基于PFAS的Sorb-PFPE+(全氟聚醚)和Sorb-NFN+(十一氟-1-癸醇)以及非基于PFAS的Sorb-PFS+(五氟苯乙烯)和Sorb-DFE+(2,2-二氟乙醇)),特别感兴趣的是去除(超)短链PFAS。在所有这些类型的氟化吸附剂中,Sorb-PFS+达到了与先前报道的高效Sorb-PFPE+吸附剂相当的去除性能。Sorb-PFS+显示所有测试的PFAS去除率为90%,包括(超)短链全氟丙酸(PFPrA, 97.7%)、全氟-2-甲氧基乙酸(PFMOAA, 98.8%)、全氟-2-甲氧基丙酸(PMPA, 99.1%)和二氟乙酸(DFA, 92.2%)。进一步的吸附动力学试验证明了它在5分钟内快速、有效和不可逆地去除(超)短链PFAS。使用Langmuir模型估计了吸附量,DFA、PFPrA、PFMOAA和PMPA分别达到275.2、357.4、475.7和758.7 mg/g。在5个重复的吸附和解吸循环中,没有观察到吸附剂性能的显著下降,验证了Sorb-PFS+的再生和可重复使用性。在两种实际水基质中,Sorb-PFS+也表现出了令人满意的性能,在垃圾渗滤液中对PFMOAA和PMPA的去除率达到93%,在污水中达到99%,优于市售的PFA694E吸附剂。这项工作为氟化但非pfas吸附剂的发展提供了重要见解,强调了非pfas替代品在满足未来监管要求的同时保留氟-氟相互作用的好处的潜力,从而有助于实现更绿色和更可持续的未来。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Capturing PFAS with Partly Fluorinated Macromolecules: The Influence of the Fluorinated Group Structure

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.

求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
Macromolecules
Macromolecules 工程技术-高分子科学
CiteScore
9.30
自引率
16.40%
发文量
942
审稿时长
2 months
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.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信