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Structural control of mixed ionic and electronic transport in conducting polymers.

ABSTRACT: Poly(3,4-ethylenedioxythiophene) doped with poly(styrenesulfonate),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 toPSS 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 inPSS 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. These findings may pave the way for the rational design of polymeric materials and processing routes to enhance devices reliant on mixed conduction.

SUBMITTER: Rivnay J

PROVIDER: S-EPMC4838877 | biostudies-other | 2016

REPOSITORIES: biostudies-other

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Structural control of mixed ionic and electronic transport in conducting polymers.

Rivnay Jonathan J Inal Sahika S Collins Brian A BA Sessolo Michele M Stavrinidou Eleni E Strakosas Xenofon X Tassone Christopher C Delongchamp Dean M DM Malliaras George G GG

Nature communications 20160419

Poly(3,4-ethylenedioxythiophene) doped with poly(styrenesulfonate),<h4>Pedot</h4>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<h4>Pedot</h4>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 wh ...[more]

PMID: 27090156

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Project description:The commercially available polyelectrolyte complex poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) is ubiquitous in organic and hybrid electronics. As such, it has often been used as a benchmark material for fundamental studies and the development of new electronic devices. Yet, most studies on PEDOT:PSS have focused on its electronic conductivity in dry environments, with less consideration given to its ion transport, coupled ionic-electronic transport, and charge storage properties in aqueous environments. These properties are essential for applications in bioelectronics (sensors, actuators), charge storage devices, and electrochromic displays. Importantly, past studies on mixed ionic-electronic transport in PEDOT:PSS neglected to consider how the molecular structure of PSS affects mixed ionic-electronic transport. Herein, we therefore investigated the effect of the molecular weight and size distribution of PSS on the electronic properties and morphology of PEDOT:PSS both in dry and aqueous environments, and overall performance in organic electrochemical transistors (OECTs). Using reversible addition-fragmentation chain transfer (RAFT) polymerization with two different chain transfer agents, six PSS samples with monomodal, narrow (Đ = 1.1) and broad (Đ = 1.7) size distributions and varying molecular weights were synthesized and used as matrices for PEDOT. We found that using higher molecular weight of PSS (M n = 145 kg mol-1) and broad dispersity led to OECTs with the highest transconductance (up to 16 mS) and [μC * ] values (~140 F·cm-1V-1s-1) in PEDOT:PSS, despite having a lower volumetric capacitance (C * = 35 ± 4 F cm-3). The differences were best explained by studying the microstructure of the films by atomic force microscopy (AFM). We found that heterogeneities in the PEDOT:PSS films (interconnected and large PEDOT- and PSS-rich domains) obtained from high molecular weight and high dispersity PSS led to higher charge mobility (μ OECT ~ 4 cm2V-1s-1) and hence transconductance. These studies highlight the importance of considering molecular weight and size distribution in organic mixed ionic-electronic conductor, and could pave the way to designing high performance organic electronics for biological interfaces.

Dataset Information

Structural control of mixed ionic and electronic transport in conducting polymers.

Publications

Structural control of mixed ionic and electronic transport in conducting polymers.

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