Controlling swelling in mixed transport polymers through alkyl side-chain physical cross-linking

Author:

Siemons Nicholas12ORCID,Pearce Drew1,Yu Hang1,Tuladhar Sachetan M.1,LeCroy Garrett S.2,Sheelamanthula Rajendar3ORCID,Hallani Rawad K.3,Salleo Alberto2,McCulloch Iain3ORCID,Giovannitti Alexander24,Frost Jarvist M.5ORCID,Nelson Jenny1ORCID

Affiliation:

1. Department of Physics, Imperial College, London, South Kensington, London SW7 2AZ, United Kingdom

2. Department of Materials Science and Engineering, Stanford University, Stanford, CA 94305

3. King Abdullah University of Science and Technology Solar Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal 23955, Saudi Arabia

4. Department of Chemistry and Chemical Engineering, Chalmers University of Technology, Göteborg 412 96, Sweden

5. Department of Chemistry, Imperial College, London, South Kensington, London SW7 2AZ, United Kingdom

Abstract

Semiconducting conjugated polymers bearing glycol side chains can simultaneously transport both electronic and ionic charges with high charge mobilities, making them ideal electrode materials for a range of bioelectronic devices. However, heavily glycolated conjugated polymer films have been observed to swell irreversibly when subjected to an electrochemical bias in an aqueous electrolyte. The excessive swelling can lead to the degradation of their microstructure, and subsequently reduced device performance. An effective strategy to control polymer film swelling is to copolymerize glycolated repeat units with a fraction of monomers bearing alkyl side chains, although the microscopic mechanism that constrains swelling is unknown. Here we investigate, experimentally and computationally, a series of archetypal mixed transporting copolymers with varying ratios of glycolated and alkylated repeat units. Experimentally we observe that exchanging 10% of the glycol side chains for alkyl leads to significantly reduced film swelling and an increase in electrochemical stability. Through molecular dynamics simulation of the amorphous phase of the materials, we observe the formation of polymer networks mediated by alkyl side-chain interactions. When in the presence of water, the network becomes increasingly connected, counteracting the volumetric expansion of the polymer film.

Funder

China Scholarship Council

EC | ERC | HORIZON EUROPE European Research Council

Royal Society

DOE | Idaho Operations Office, U.S. Department of Energy

King Abdullah University of Science and Technology

Publisher

Proceedings of the National Academy of Sciences

Subject

Multidisciplinary

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