Tuning the degree of oxidation and electron delocalization of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) with solid-electrolyte
Date
2017-10Source Title
Applied Surface Science
Print ISSN
0169-4332
Publisher
Elsevier
Volume
419
Pages
770 - 777
Language
English
Type
ArticleItem Usage Stats
237
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185
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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 structureIonic 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/11693/37435Published Version (Please cite this version)
https://doi.org/10.1016/j.apsusc.2017.05.049Collections
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