Reversible Electrochemical Charging of n-Type Conjugated Polymer Electrodes in Aqueous Electrolytes

Anna A. Szumska, Iuliana P. Maria, Lucas Q. Flagg, Achilleas Savva, Jokubas Surgailis, Bryan D. Paulsen, Davide Moia, Xingxing Chen, Sophie Griggs, J. Tyler Mefford, Reem B. Rashid, Adam Marks, Sahika Inal, David S. Ginger, Alexander Giovannitti, Jenny Nelson

Research output: Contribution to journalArticlepeer-review

65 Scopus citations


Conjugated polymers achieve redox activity in electrochemical devices by combining redox-active, electronically conducting backbones with ion-transporting side chains that can be tuned for different electrolytes. In aqueous electrolytes, redox activity can be accomplished by attaching hydrophilic side chains to the polymer backbone, which enables ionic transport and allows volumetric charging of polymer electrodes. While this approach has been beneficial for achieving fast electrochemical charging in aqueous solutions, little is known about the relationship between water uptake by the polymers during electrochemical charging and the stability and redox potentials of the electrodes, particularly for electron-transporting conjugated polymers. We find that excessive water uptake during the electrochemical charging of polymer electrodes harms the reversibility of electrochemical processes and results in irreversible swelling of the polymer. We show that small changes of the side chain composition can significantly increase the reversibility of the redox behavior of the materials in aqueous electrolytes, improving the capacity of the polymer by more than one order of magnitude. Finally, we show that tuning the local environment of the redox-active polymer by attaching hydrophilic side chains can help to reach high fractions of the theoretical capacity for single-phase electrodes in aqueous electrolytes. Our work shows the importance of chemical design strategies for achieving high electrochemical stability for conjugated polymers in aqueous electrolytes.
Original languageEnglish (US)
JournalJournal of the American Chemical Society
StatePublished - Sep 1 2021

Bibliographical note

KAUST Repository Item: Exported on 2021-09-07
Acknowledged KAUST grant number(s): OSR-2018-CRG/CCF-3079, OSR-2018-CRG7-3749, OSR-2019-CRG8-4086
Acknowledgements: We thank Dr. Drew Pearce for assistance and advice with DFT calculations. A.G. acknowledges funding from the TomKat Center for Sustainable Energy at Stanford University. J.N., A.A.S., and A.G. acknowledge funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (grant agreement No. 742708, project CAPaCITy). D.M. and J.N. acknowledge support of the UK Engineering and Physical Sciences Research Council (EPSRC) via the Supersolar programme (grant no. EP/M025020/1). B.D.P and R.B.R. gratefully acknowledge financial support from King Abdullah University of Science and Technology (KAUST) Office of Sponsored Research (OSR) under award no. OSR-2019-CRG8-4086. I.P.M., X.C., and S.G. acknowledge financial support from KAUST, including Office of Sponsored Research (OSR) awards (no. OSR-2018-CRG/CCF-3079, OSR-2019-CRG8-4086, and OSR-2018-CRG7-3749), the ERC Synergy Grant SC2 (610115), the European Union’s Horizon 2020 research and innovation program under grant agreement No. 952911, project BOOSTER, and grant agreement No. 862474, project RoLA-FLEX, EPSRC Project EP/T026219/1, and NSF DMR-1751308. This work made use of the Keck-II and NUFAB facilities of Northwestern University’s NUANCE Center, which has received support from the SHyNE Resource (NSF ECCS-2025633), the IIN, and Northwestern’s MRSEC program (NSF DMR-1720139).

ASJC Scopus subject areas

  • Biochemistry
  • Colloid and Surface Chemistry
  • General Chemistry
  • Catalysis


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