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Title: Structural control of mixed ionic and electronic transport in conducting polymers

Poly(3,4-ethylenedioxythiophene) doped with poly(styrenesulfonate), PEDOT:PSS, has been utilized for over two decades as a stable, solution-processable hole conductor. While its hole transport properties have been the subject of intense investigation, recent work has turned to PEDOT:PSS as a mixed ionic/electronic conductor in applications including bioelectronics, energy storage and management, and soft robotics. Conducting polymers can efficiently transport both holes and ions when sufficiently hydrated, however, little is known about the role of morphology on mixed conduction. Here, we show that bulk ionic and electronic mobilities are simultaneously affected by processing-induced changes in nano- and meso-scale structure in PEDOT:PSS films. We quantify domain composition, and find that domain purification on addition of dispersion co-solvents limits ion mobility, even while electronic conductivity improves. We show that an optimal morphology allows for the balanced ionic and electronic transport that is critical for prototypical mixed conductor devices. As a result, these findings may pave the way for the rational design of polymeric materials and processing routes to enhance devices reliant on mixed conduction.
ORCiD logo [1] ;  [1] ;  [2] ;  [3] ;  [1] ;  [1] ;  [4] ;  [5] ;  [1]
  1. Ecole Nationale Superieure des Mines, CMP-EMSE, MOC, Gardanne (France)
  2. National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States); Washington State Univ., Pullman, WA (United States)
  3. Univ. de Valencia, Paterna (Spain)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  5. National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States)
Publication Date:
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Nature Publishing Group
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
36 MATERIALS SCIENCE; physical sciences; materials science; nanotechnology; physical chemistry
OSTI Identifier: