Fluorous-Core Nanoparticle-Embedded Hydrogel Synthesized via Tandem Photo-Controlled Radical Polymerization: Facilitating the Separation of Perfluorinated Alkyl Substances from Water
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摘要: 全氟和多氟化合物，特别是全氟辛酸（PFOA）和全氟辛烷磺酸（PFOS）对多个国家和地区的水资源造成了污染。目前这类有机污染物处理技术在成本和效率方面存在的局限性，促使人们开发更高选择性和高亲和力的吸附剂。近期，复旦大学陈茂研究员团队报道了一种通过可见光催化的无金属串联光控自由基聚合得到的多氟纳米颗粒镶嵌的水凝胶吸附剂。这种吸附剂材料对于各种电性的全氟或多氟化小分子均表现出了优异的吸附性能，且在没有明显性能损耗的基础上可完成5次以上的吸附-解吸附循环。该方法为去除水中的PFOA、PFOS等全氟或多氟化小分子提供了新策略。Abstract: Per- and polyfluorinated alkyl substances (PFASs), notably perfluorooctanoic acid (PFOA), contaminate many ground and surface waters and are environmentally persistent. The cost and performance limitations of current PFAS removal technologies motivate efforts to develop adsorbents with high selectivity and affinity. Recently, Chen’s group at Fudan University reported a fluorous-core nanoparticle-embedded hydrogel (FCH) synthesized by the metal-free tandem photo-controlled radical polymerization under visible-light irradiation. This FCH material exhibits outstanding adsorption performance on PFASs with different electronic characteristics including neutral, anionic, cationic and zwitterionic ones. Moreover, the adsorption performance of the FCH material is barely affected even after more than five adsorption-desorption cycles. These results demonstrate the promise of the FCH material for treating PFAS-contaminated water.
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图 1 （a）两步串联photo-CRP过程的合成路线；（b）室温下水膨胀纳米氟核水凝胶（FCH）材料的应力-应变曲线；（c）拉伸性能，包括拉伸强度、断裂伸长率和杨氏模量；（d）拉伸多氟化钠米粒子嵌入的水凝胶(FCH2)的光学图像[5]
Figure 1. （a） Synthetic route of the two-step tandem photo-CRP process; （b） Stress-strain curves of the water-swollen FCH materials measured at room temperature; （c） Tensile properties including tensile strength, elongation at break and Young’s modulus; （d） Optical images of stretching FCH2[5]
图 2 用FCH2去除水溶液中的PFASs：（a）不同条件下从水溶液中以及正癸酸（DA）和无机盐离子IOSs（包括MgSO4，KNO3和NaCl）中去除PFOA；（b）不同浓度PFOA条件下，用FCH2和聚丙烯酰胺水凝胶（PAAH）去除PFOA（#1表示ρ（PFOA）=1 μg/L，ρ（DA）=20 mg/L，ρ（IOSs）=100 mg/L）；（c）FCH2对不同PFASs的去除[5]
Figure 2. Removal of PFASs from aqueous solutions with FCH2: （a） Removal of PFOA from aqueous solutions at different conditions（DA is decanoic acid.IOSs is inorganic salts,including MgSO4，KNO3 and NaCl ); （b） Removal of PFOA with FCH2 and poly（acrylamide） hydrogel （PAAH） at diffferent concentrations of PFOA(#1 represents ρ（PFOA）=1 μg/L，ρ（DA）=20 mg/L，ρ（IOSs）=100 mg/L); （c） Removal of different PFASs with FCH2[5]
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[1] GONG H, GU Y, ZHAO Y, et al. Precise synthesis of ultra-high-molecular-weight fluoropolymers enabled by chain-transfer-agent differentiation under visible-light irradiation [J]. Angew Chem Int Ed,2020,59(2):919-927. doi: 10.1002/anie.201914768 [2] GONG H, ZHAO Y, SHEN X, et al. Organocatalyzed photocontrolled radical polymerization of semifluorinated (meth)acrylates driven by visible light [J]. Angew Chem Int Ed,2018,57(1):333-337. doi: 10.1002/anie.201712460 [3] JIANG K, HAN S, MA M, et al. Photoorganocatalyzed reversible-deactivation alternating copolymerization of chlorotrifluoroethylene and vinyl ethers under ambient conditions: facile access to main-chain fluorinated copolymers [J]. J Am Chem Soc,2020,142(15):7108-7115. [4] QUAN Q, GONG H, CHEN M. Preparation of semifluorinated poly(meth)acrylates by improved photo-controlled radical polymerization without the use of a fluorinated RAFT agent: Facilitating surface fabrication with fluorinated materials [J]. Polymer Chemistry,2018,9(30):4161-4171. [5] QUAN Q, WEN H, HAN S, et al. Fluorous-core nanoparticle-embedded hydrogel synthesized via tandem photo-controlled radical polymerization: Facilitating the separation of perfluorinated alkyl substances from water [J]. ACS Appl Mater Interfaces,2020,12(21):24319-24327. doi: 10.1021/acsami.0c04646 -
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