Ionic Liquid Designed for PEDOT:PSS Conductivity Enhancement.

Poly-3,4-ethylenedioxythiophene:polystyrenesulfonate (PEDOT:PSS) is a water-processable conducting polymer with promise for use in transparent flexible electrodes and thermoelectric devices, but its conductivity is not satisfactory. Its low conductivity is attributed to the formation of hydrophilic/...

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Published in:Journal of the American Chemical Society Vol. 140; no. 16; pp. 5375 - 5385
Main Authors: de Izarra, Ambroise, Seongjin Park, Jinhee Lee, Lansac, Yves, Yun Hee Jang
Format: Article
Published: American Chemical Society 4/25/2018
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Online Access:View this record in EBSCOhost
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        00027863
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      jtl: Journal of the American Chemical Society
      issn: 00027863
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    pubinfo:
      dt: 4/25/2018
      vid: 140
      iid: 16
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      pub: American Chemical Society
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        129345624
        10.1021/jacs.7b10306
      ppf: 5375
      ppct: 10
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        atl: Ionic Liquid Designed for PEDOT:PSS Conductivity Enhancement.
      aug:
        au:
          de Izarra, Ambroise
          Seongjin Park
          Jinhee Lee
          Lansac, Yves
          Yun Hee Jang
        affil:
          Department of Energy Science and Engineering, DGIST, Daegu 42988, Korea
          GREMAN, UMR 7347, CNRS, Université de Tours, 37200 Tours, France
          Laboratoire de Physique des Solides, CNRS, Université Paris-Sud, 91405 Orsay, France
      su:
        Ionic liquids
        Electric conductivity
        Conducting polymers
        Ion exchange (Chemistry)
        Electrodes
        Thermoelectric apparatus & appliances
        Density functional theory
      sug:
        subj:
          Ionic liquids
          Electric conductivity
          Conducting polymers
          Ion exchange (Chemistry)
          Electrodes
          Thermoelectric apparatus & appliances
          Density functional theory
      ab: Poly-3,4-ethylenedioxythiophene:polystyrenesulfonate (PEDOT:PSS) is a water-processable conducting polymer with promise for use in transparent flexible electrodes and thermoelectric devices, but its conductivity is not satisfactory. Its low conductivity is attributed to the formation of hydrophilic/insulating PSS outer layers encapsulating the conducting/hydrophobic p-doped PEDOT cores. Recently a significant conductivity enhancement has been achieved by adding ionic liquid (IL). It is believed that ion exchange between PEDOT:PSS and IL components helps PEDOT to decouple from PSS and to grow into large-scale conducting domains, but the exact mechanism is still under debate. Here we show through free energy calculations using density functional theory on a minimal model that the most efficient IL pairs are the least tightly bound ones with the lowest binding energies, which would lead to the most efficient ion exchange with PEDOT:PSS. This spontaneous ion exchange followed by nanophase segregation between PEDOT and PSS, with formation of a π-stacked PEDOT aggregate decorated by IL anions, is also supported by molecular dynamics performed on larger PEDOT:PSS models in solution. We also show that the most efficient IL anions would sustain the highest amount of charge carriers uniformly distributed along the PEDOT backbone to further enhance the conductivity, providing that they remain in the PEDOT domain after the ion exchange. Hence, our design principle is that the high-performance IL should induce not only an efficient ion exchange with PEDOT:PSS to improve the PEDOT morphology (to increase mobility) but also a uniform high-level p-doping of PEDOT (to enhance intrinsic conductivity). Based on this principle, a promising (electron-withdrawing, but bulky, soft, and hydrophobic) new IL pair is proposed.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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          year: 2018
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