Development of Synthetically Accessible Glycolated Polythiophenes for High-Performance Organic Electrochemical Transistors

Abstract
Four glycolated polythiophene-based organic mixed ionic-electronic conductors (OMIECs), PE2gTT, PE2gT, PT2gTT, and PT2gT are prepared by atom-efficient direct arylation polymerization, avoiding the need for toxic organometallic precursors. PE2gT, PT2gTT, and PT2gT are operable in p-type accumulation mode organic electrochemical transistors (OECTs), with PT2gT displaying the best device performance with a µC* product figure-of-merit of 290 F cm−1 V−1 s−1. A record volumetric capacitance among p-type glycolated polythiophene OMIECs of 313 F cm−3 is observed for PE2gT, ascribed to the high proportionality of polar components in its materials design. The good OECT performance of PE2gT with µC* = 84.2 F cm−1 V−1 s−1, comparable with state-of-the-art poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) devices, coupled with its synthetic accessibility and favorable accumulation mode operation makes PE2gT an ideal glycolated alternative to PEDOT:PSS in bioelectronics. PE2gT with the least negative threshold voltage also displays the best OECT operational cycling stability, linked to better resistance of its oxidized state against parasitic redox side reactions . Shelf life stability of OECTs stored (without bias) is observed to be better for materials with a more negative threshold voltage and higher average molecular weight (PT2gT), that are less susceptible to ambient auto-oxidation and film delamination.

Acknowledgements
The authors thank the Engineering and Physical Sciences Research Council (EPSRC) (EP/T028513/1) and KAUST baseline funding for support. B.D. acknowledges funding via the President's PhD Scholarship Scheme. V.L. and A.F.P. thank the National Science Foundation (NSF) through cooperative agreement number 1849213 for financial support. H. Y. acknowledges the PhD studentship support from the China Scholarship Council (CSC). J.N. and H.Y. thank the European Research Council for support under the European Union's Horizon 2020 research and innovation program (Grant Agreement No. 742708). J.N. thanks the Royal Society for award of a Research Professorship.

Publisher
Wiley

Journal
Advanced Electronic Materials

DOI
10.1002/aelm.202300580

Additional Links
https://onlinelibrary.wiley.com/doi/10.1002/aelm.202300580

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