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      Tuning the degree of oxidation and electron delocalization of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) with solid-electrolyte

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      Author(s)
      Vempati, Sesha
      Ertaş, Yelda
      Çelebioğlu, Aslı
      Uyar, Tamer
      Date
      2017-10
      Source Title
      Applied Surface Science
      Print ISSN
      0169-4332
      Publisher
      Elsevier
      Volume
      419
      Pages
      770 - 777
      Language
      English
      Type
      Article
      Item Usage Stats
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      Abstract
      We report on the effects of ionic interaction on the electronic structure of PEDOT:PSS where the oxidation state of PEDOT is an import aspect for various applications. Additional ionic interactions are introduced and controlled by varying the fraction of poly(ethylene oxide) (PEO). These interactions are balanced against the inherent cohesive forces within each of the polymers constituting intertwined networks. Raman spectra evidenced a peak-shift as high as ∼14 cm−1 for C[dbnd]C vibrational region which suggested increasing degree of oxidation of PEDOT for higher PEO fractions. Changes to the single and bipolaronic absorption bands support the results from the Raman spectra. For highest PEO fraction neutral-PEDOT and lowered bipolaron density is attributed to localization of PEDOT chains within PEO matrix. Interestingly, for higher PEO fractions the electronic density of states (DOS) of HOMO and core-levels (S2p, C1s and O1s) suggested increased degree of oxidation and electron localization on PEDOT. Near and below (∼12 eV) Fermi level, contribution to the O2p and C2p atomic orbitals depicted significantly different DOS. Also we note energetic shift for O2s/C2s and bonding σCC atomic and molecular DOS, respectively. The correlation between some surface and bulk-related properties suggests the uniformity of the blend material which might be vital for the application in electrochemical devices.
      Keywords
      HOMO structure
      Ionic interaction and intertwined polymer network
      XPS
      Conducting polymers
      Electrolytes
      Electronic density of states
      Electronic structure
      Ethylene
      Oxidation
      Polyethylene oxides
      Polymers
      Quantum chemistry
      Raman scattering
      X ray photoelectron spectroscopy
      Degree of oxidations
      Electrochemical devices
      Electron delocalization
      Electron localizations
      Electronic density
      Poly (ethylene oxide) (PEO)
      Poly(3 ,4-ethylenedioxythiophene):poly(styrenesulfonate)
      Polymer networks
      Solid electrolytes
      Permalink
      http://hdl.handle.net/11693/37435
      Published Version (Please cite this version)
      https://doi.org/10.1016/j.apsusc.2017.05.049
      Collections
      • Institute of Materials Science and Nanotechnology (UNAM) 2098
      • Nanotechnology Research Center (NANOTAM) 1125
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