Synthetic Nuances to Maximize n-Type Organic Electrochemical Transistor and Thermoelectric Performance in Fused Lactam Polymers

Adam Marks*, Xingxing Chen*, Ruiheng Wu, Reem B. Rashid, Wenlong Jin, Bryan D. Paulsen, Maximilian Moser, Xudong Ji, Sophie Griggs, Dilara Meli, Xiaocui Wu, Helen Bristow, Joseph Strzalka, Nicola Gasparini, Giovanni Costantini, Simone Fabiano, Jonathan Rivnay, Iain McCulloch

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

38 Citations (Scopus)

Abstract

A series of fully fused n-type mixed conduction lactam polymers p(g7NCnN), systematically increasing the alkyl side chain content, are synthesized via an inexpensive, nontoxic, precious-metal-free aldol polycondensation. Employing these polymers as channel materials in organic electrochemical transistors (OECTs) affords state-of-the-art n-type performance with p(g7NC10N) recording an OECT electron mobility of 1.20 × 10-2 cm2 V-1 s-1 and a μC figure of merit of 1.83 F cm-1 V-1 s-1. In parallel to high OECT performance, upon solution doping with (4-(1,3-dimethyl-2,3-dihydro-1H-benzoimidazol-2-yl)phenyl)dimethylamine (N-DMBI), the highest thermoelectric performance is observed for p(g7NC4N), with a maximum electrical conductivity of 7.67 S cm-1 and a power factor of 10.4 μW m-1 K-2. These results are among the highest reported for n-type polymers. Importantly, while this series of fused polylactam organic mixed ionic-electronic conductors (OMIECs) highlights that synthetic molecular design strategies to bolster OECT performance can be translated to also achieve high organic thermoelectric (OTE) performance, a nuanced synthetic approach must be used to optimize performance. Herein, we outline the performance metrics and provide new insights into the molecular design guidelines for the next generation of high-performance n-type materials for mixed conduction applications, presenting for the first time the results of a single polymer series within both OECT and OTE applications.

Original languageEnglish
Pages (from-to)4642-4656
Number of pages15
JournalJournal of the American Chemical Society
Volume144
Issue number10
Early online date8 Mar 2022
DOIs
Publication statusPublished - 16 Mar 2022

Bibliographical note

Funding Information:
A.M., M.M., S.G., H.B., X.C., and I.M. acknowledge financial support from KAUST, including Office of Sponsored Research (OSR) award nos. OSR-2018-CRG/CCF-3079, OSR-2019-CRG8-4086, and OSR-2018-CRG7-3749. The authors acknowledge funding from ERC Synergy Grant SC2 (610115), the European Union’s Horizon 2020 Research and Innovation Programme under grant agreement no. 952911, project BOOSTER and grant agreement no. 862474, project RoLA-FLEX, as well as EPSRC Project EP/T026219/1 and NSF DMR-1751308. R.W., B.D.P., and J.R. gratefully acknowledge support from the National Science Foundation Grant No. NSF DMR-1751308. B.D.P., R.B.R., X.J., D.M., and J.R. also acknowledge the KAUST CRG. This research used resources of the Advanced Photon Source; a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. This work made use of the Keck-II facility of Northwestern University’s NUANCE Center, which has received support from the SHyNE Resource (NSF ECCS-1542205), the IIN, and Northwestern’s MRSEC program (NSF DMR-1720139). S.F. and W.J. acknowledge financial support from the Swedish Research Council (2020-03243), the European Commission through the Marie Sklodowska-Curie project HORATES (GA-955837), and the Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linköping University (Faculty Grant SFO-Mat-LiU 2009-00971). X.W. acknowledges funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement no. 945380.

Publisher Copyright:
© 2022 American Chemical Society.

ASJC Scopus subject areas

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

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