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Kinking Matters: meta-Terphenyl Improves Hydroxide Conductivity of Mechanically Robust Fluorine-Free Poly(arylene piperidinium) Copolymers for Anion Exchange Membranes

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Title: Kinking Matters: meta-Terphenyl Improves Hydroxide Conductivity of Mechanically Robust Fluorine-Free Poly(arylene piperidinium) Copolymers for Anion Exchange Membranes
Authors: Mazumder, Kajari, Nederstedt, Hannes, Weber, Richard, Haraguchi, Shuichi, 1983, Neubert, Richard, Plamper, Felix A., Müller, Christian, 1980, Sommer, M.
Source: ACS Applied Materials & Interfaces. 17(29):41978-41990
Subject Terms: polymer electrolyte membranes, hydroxide conductivity, anion exchange membranes, fluorine-free polymers, meta-terphenyl polymers, poly(arylene piperidinium) copolymers
Description: Poly(arylene piperidinium) (PAP) polymers have emerged as promising candidates for applications as anion exchange membranes (AEMs) and have seen some commercial use in the form of PiperION by Versogen; however, PiperION contains fluorinated units to balance its ionic content. Fluorine-free variants are environmentally more friendly alternatives as recycling is facilitated. Herein, we report a series of four fluorine-free PAP membranes that are mechanically robust and feature moderate water uptake yet high ionic conductivity. p-Quaterphenyl (pQP) is copolymerized with either m- or p-terphenyl (m/pTP) and N-methyl-4-piperidone under superacid-catalyzed polyhydroxyalkylation conditions. The molar ratios of the reactants are adjusted to maintain a balance of solubility and flexibility of the polymers and to reach ion exchange capacities between 2.53 and 2.66 mequiv g -1 . The polymers exhibit thermal stability of Td,95 > 260 °C, Young’s moduli between 0.7 and 1.0 GPa, and ultimate tensile stresses of 50-60 MPa in the dry state. Additionally, under submersion tensile deformation, the Young’s moduli and ultimate tensile stresses are in the range 200-320 MPa and 15-22 MPa, respectively. The sample with an equimolar ratio of pQP and mTP was found to exhibit a robust nature with elongation up to 170% when subjected to submersion tensile deformation, thus showing attractive mechanical properties under relevant working conditions. Wet membranes show an ionomer SAXS peak in the range of 5 nm, suggesting clustering of water and ionic parts of the chain. High hydroxide conductivity of up to 197 mS cm -1 at 80 °C is observed. Such behavior is promising considering their water uptake of 85% at 80 °C as an upper limit, resulting in moderate areal and through-plane swellings of 100% and 55%, respectively. The results demonstrate that fluorine-free PAPs can be tuned to match important criteria of AEMs, including low water uptake, high dimensional and alkaline stability, and high hydroxide conductivity.
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  Label: Title
  Group: Ti
  Data: Kinking Matters: meta-Terphenyl Improves Hydroxide Conductivity of Mechanically Robust Fluorine-Free Poly(arylene piperidinium) Copolymers for Anion Exchange Membranes
– Name: Author
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  Data: <searchLink fieldCode="AR" term="%22Mazumder%2C+Kajari%22">Mazumder, Kajari</searchLink><br /><searchLink fieldCode="AR" term="%22Nederstedt%2C+Hannes%22">Nederstedt, Hannes</searchLink><br /><searchLink fieldCode="AR" term="%22Weber%2C+Richard%22">Weber, Richard</searchLink><br /><searchLink fieldCode="AR" term="%22Haraguchi%2C+Shuichi%22">Haraguchi, Shuichi</searchLink>, 1983<br /><searchLink fieldCode="AR" term="%22Neubert%2C+Richard%22">Neubert, Richard</searchLink><br /><searchLink fieldCode="AR" term="%22Plamper%2C+Felix+A%2E%22">Plamper, Felix A.</searchLink><br /><searchLink fieldCode="AR" term="%22Müller%2C+Christian%22">Müller, Christian</searchLink>, 1980<br /><searchLink fieldCode="AR" term="%22Sommer%2C+M%2E%22">Sommer, M.</searchLink>
– Name: TitleSource
  Label: Source
  Group: Src
  Data: <i>ACS Applied Materials & Interfaces</i>. 17(29):41978-41990
– Name: Subject
  Label: Subject Terms
  Group: Su
  Data: <searchLink fieldCode="DE" term="%22polymer+electrolyte+membranes%22">polymer electrolyte membranes</searchLink><br /><searchLink fieldCode="DE" term="%22hydroxide+conductivity%22">hydroxide conductivity</searchLink><br /><searchLink fieldCode="DE" term="%22anion+exchange+membranes%22">anion exchange membranes</searchLink><br /><searchLink fieldCode="DE" term="%22fluorine-free+polymers%22">fluorine-free polymers</searchLink><br /><searchLink fieldCode="DE" term="%22meta-terphenyl+polymers%22">meta-terphenyl polymers</searchLink><br /><searchLink fieldCode="DE" term="%22poly%28arylene+piperidinium%29+copolymers%22">poly(arylene piperidinium) copolymers</searchLink>
– Name: Abstract
  Label: Description
  Group: Ab
  Data: Poly(arylene piperidinium) (PAP) polymers have emerged as promising candidates for applications as anion exchange membranes (AEMs) and have seen some commercial use in the form of PiperION by Versogen; however, PiperION contains fluorinated units to balance its ionic content. Fluorine-free variants are environmentally more friendly alternatives as recycling is facilitated. Herein, we report a series of four fluorine-free PAP membranes that are mechanically robust and feature moderate water uptake yet high ionic conductivity. p-Quaterphenyl (pQP) is copolymerized with either m- or p-terphenyl (m/pTP) and N-methyl-4-piperidone under superacid-catalyzed polyhydroxyalkylation conditions. The molar ratios of the reactants are adjusted to maintain a balance of solubility and flexibility of the polymers and to reach ion exchange capacities between 2.53 and 2.66 mequiv g -1 . The polymers exhibit thermal stability of Td,95 > 260 °C, Young’s moduli between 0.7 and 1.0 GPa, and ultimate tensile stresses of 50-60 MPa in the dry state. Additionally, under submersion tensile deformation, the Young’s moduli and ultimate tensile stresses are in the range 200-320 MPa and 15-22 MPa, respectively. The sample with an equimolar ratio of pQP and mTP was found to exhibit a robust nature with elongation up to 170% when subjected to submersion tensile deformation, thus showing attractive mechanical properties under relevant working conditions. Wet membranes show an ionomer SAXS peak in the range of 5 nm, suggesting clustering of water and ionic parts of the chain. High hydroxide conductivity of up to 197 mS cm -1 at 80 °C is observed. Such behavior is promising considering their water uptake of 85% at 80 °C as an upper limit, resulting in moderate areal and through-plane swellings of 100% and 55%, respectively. The results demonstrate that fluorine-free PAPs can be tuned to match important criteria of AEMs, including low water uptake, high dimensional and alkaline stability, and high hydroxide conductivity.
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RecordInfo BibRecord:
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      – Type: doi
        Value: 10.1021/acsami.5c08476
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      – Text: English
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        PageCount: 13
        StartPage: 41978
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      – SubjectFull: polymer electrolyte membranes
        Type: general
      – SubjectFull: hydroxide conductivity
        Type: general
      – SubjectFull: anion exchange membranes
        Type: general
      – SubjectFull: fluorine-free polymers
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      – SubjectFull: meta-terphenyl polymers
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      – SubjectFull: poly(arylene piperidinium) copolymers
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      – TitleFull: Kinking Matters: meta-Terphenyl Improves Hydroxide Conductivity of Mechanically Robust Fluorine-Free Poly(arylene piperidinium) Copolymers for Anion Exchange Membranes
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              Y: 2025
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