| Title: |
Synthetic Nuances to Maximize n-Type Organic Electrochemical Transistor and Thermoelectric Performance in Fused Lactam Polymers |
| Authors: |
Marks, Adam; Chen, Xingxing; Wu, Ruiheng; Rashid, Reem B.; Jin, Wenlong; Paulsen, Bryan D.; Moser, Maximilian; Ji, Xudong; Griggs, Sophie; Meli, Dilara; Wu, Xiaocui; Bristow, Helen; Strzalka, Joseph W.; Gasparini, Nicola; Costantini, Giovanni; Fabiano, Simone; Rivnay, Jonathan; McCulloch, Iain |
| Contributors: |
KAUST Solar Center (KSC); Physical Science and Engineering (PSE) Division; Department of Chemistry, University of Oxford, Oxford OX1 3TA, U.K.; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States; Department of Biomedical Engineering, Northwestern University, Evanston, Illinois 60208, United States; Laboratory of Organic Electronics, Department of Science and Technology, Linköping University, NorrköpingSE-60174, Sweden; Department of Material Science, Northwestern University, Evanston, Illinois 60208, United States; Department of Chemistry, University of Warwick, Coventry CV4 7AL, U.K.; X-ray Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States; Department of Chemistry and Centre for Processable Electronics, Imperial College London, London W12 0BZ, U.K. |
| Publisher Information: |
American Chemical Society (ACS) |
| Publication Year: |
2022 |
| Collection: |
King Abdullah University of Science and Technology: KAUST Repository |
| Description: |
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. ; 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 ... |
| Document Type: |
article in journal/newspaper |
| File Description: |
application/pdf; image/jpeg |
| Language: |
unknown |
| ISSN: |
0002-7863; 1520-5126 |
| Relation: |
http://liu.diva-portal.org/smash/get/diva2:1653559/FULLTEXT01; Marks, A., Chen, X., Wu, R., Rashid, R. B., Jin, W., Paulsen, B. D., Moser, M., Ji, X., Griggs, S., Meli, D., Wu, X., Bristow, H., Strzalka, J., Gasparini, N., Costantini, G., Fabiano, S., Rivnay, J., & McCulloch, I. (2022). Synthetic Nuances to Maximize n-Type Organic Electrochemical Transistor and Thermoelectric Performance in Fused Lactam Polymers. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.2c00735; 2-s2.0-85126592627; 10; Journal of the American Chemical Society; http://hdl.handle.net/10754/676476; 144 |
| DOI: |
10.1021/jacs.2c00735 |
| Availability: |
http://hdl.handle.net/10754/676476; https://doi.org/10.1021/jacs.2c00735 |
| Rights: |
© American Chemical Society. This is an open access article under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/ ; This file is an open access version redistributed from: http://liu.diva-portal.org/smash/get/diva2:1653559/FULLTEXT01 ; http://creativecommons.org/licenses/by-nc-nd/4.0/ |
| Accession Number: |
edsbas.68742161 |
| Database: |
BASE |