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

dc.contributor.authorDing, Bowen
dc.contributor.authorLe, Vianna
dc.contributor.authorYu, Hang
dc.contributor.authorWu, Guanchen
dc.contributor.authorMarsh, Adam V.
dc.contributor.authorGutiérrez-Fernández, Edgar
dc.contributor.authorRamos, Nicolás
dc.contributor.authorRimmele, Martina
dc.contributor.authorMartín, Jaime
dc.contributor.authorNelson, Jenny
dc.contributor.authorPaterson, Alexandra F.
dc.contributor.authorHeeney, Martin
dc.contributor.departmentPhysical Sciences and Engineering Division (PSE) King Abdullah University of Science and Technology (KAUST) Thuwal 23955–6900 Saudi Arabia
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.contributor.departmentKAUST Solar Center (KSC)
dc.contributor.departmentChemical Science Program
dc.contributor.institutionDepartment of Chemistry and Centre for Processable Electronics Imperial College London Molecular Sciences Research Hub (White City Campus) 80 Wood Lane Shepherd's Bush London W12 0BZ UK
dc.contributor.institutionDepartment of Chemical and Materials Engineering, and Centre for Applied Energy Research University of Kentucky Lexington KY4050 USA
dc.contributor.institutionDepartment of Physics and Centre for Processable Electronics Imperial College London South Kensington Campus London SW7 2AZ UK
dc.contributor.institutionPOLYMAT and Polymer Science and Technology Department Faculty of Chemistry University of the Basque Country UPV/EHU Manuel de Lardizabal 3 20018 Donostia–San Sebastián Spain
dc.contributor.institutionCampus Industrial de Ferrol, CITENI Universidade da Coruña Campus Esteiro S/N Ferrol 15403 Spain
dc.date.accessioned2024-01-25T07:23:21Z
dc.date.available2024-01-25T07:23:21Z
dc.date.issued2024-01-23
dc.description.abstractFour 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.
dc.description.sponsorshipThe 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.
dc.eprint.versionPublisher's Version/PDF
dc.identifier.doi10.1002/aelm.202300580
dc.identifier.issn2199-160X
dc.identifier.issn2199-160X
dc.identifier.journalAdvanced Electronic Materials
dc.identifier.urihttp://hdl.handle.net/10754/696808
dc.publisherWiley
dc.relation.urlhttps://onlinelibrary.wiley.com/doi/10.1002/aelm.202300580
dc.rightsArchived with thanks to Advanced Electronic Materials under a Creative Commons license, details at: http://creativecommons.org/licenses/by/4.0/
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/
dc.titleDevelopment of Synthetically Accessible Glycolated Polythiophenes for High-Performance Organic Electrochemical Transistors
dc.typeArticle
display.details.left<span><h5>License</h5>http://creativecommons.org/licenses/by/4.0/<br><br><h5>Type</h5>Article<br><br><h5>Authors</h5><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.author=Ding, Bowen,equals">Ding, Bowen</a><br><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.author=Le, Vianna,equals">Le, Vianna</a><br><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.author=Yu, Hang,equals">Yu, Hang</a><br><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.author=Wu, Guanchen,equals">Wu, Guanchen</a><br><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.author=Marsh, Adam V.,equals">Marsh, Adam V.</a><br><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.author=Gutiérrez-Fernández, Edgar,equals">Gutiérrez-Fernández, Edgar</a><br><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.author=Ramos, Nicolás,equals">Ramos, Nicolás</a><br><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.author=Rimmele, Martina,equals">Rimmele, Martina</a><br><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.author=Martín, Jaime,equals">Martín, Jaime</a><br><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.author=Nelson, Jenny,equals">Nelson, Jenny</a><br><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.author=Paterson, Alexandra F.,equals">Paterson, Alexandra F.</a><br><a href="https://repository.kaust.edu.sa/search?query=orcid.id:0000-0001-6879-5020&spc.sf=dc.date.issued&spc.sd=DESC">Heeney, Martin</a> <a href="https://orcid.org/0000-0001-6879-5020" target="_blank"><img src="https://repository.kaust.edu.sa/server/api/core/bitstreams/82a625b4-ed4b-40c8-865a-d6a5225a26a4/content" width="16" height="16"/></a><br><br><h5>KAUST Department</h5><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.department=Physical Sciences and Engineering Division (PSE) King Abdullah University of Science and Technology (KAUST) Thuwal 23955–6900 Saudi Arabia,equals">Physical Sciences and Engineering Division (PSE) King Abdullah University of Science and Technology (KAUST) Thuwal 23955–6900 Saudi Arabia</a><br><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.department=Physical Science and Engineering (PSE) Division,equals">Physical Science and Engineering (PSE) Division</a><br><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.department=KAUST Solar Center (KSC),equals">KAUST Solar Center (KSC)</a><br><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.department=Chemical Science Program,equals">Chemical Science Program</a><br><br><h5>Date</h5>2024-01-23</span>
display.details.right<span><h5>Abstract</h5>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.<br><br><h5>Acknowledgements</h5>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.<br><br><h5>Publisher</h5><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.publisher=Wiley,equals">Wiley</a><br><br><h5>Journal</h5><a href="https://repository.kaust.edu.sa/search?spc.sf=dc.date.issued&spc.sd=DESC&f.journal=Advanced Electronic Materials,equals">Advanced Electronic Materials</a><br><br><h5>DOI</h5><a href="https://doi.org/10.1002/aelm.202300580">10.1002/aelm.202300580</a><br><br><h5>Additional Links</h5>https://onlinelibrary.wiley.com/doi/10.1002/aelm.202300580</span>
kaust.acknowledged.supportUnitKAUST baseline funding
kaust.acknowledged.supportUnitstudentship support
kaust.personMarsh, Adam V.
kaust.personHeeney, Martin
orcid.authorDing, Bowen
orcid.authorLe, Vianna
orcid.authorYu, Hang
orcid.authorWu, Guanchen
orcid.authorMarsh, Adam V.
orcid.authorGutiérrez-Fernández, Edgar
orcid.authorRamos, Nicolás
orcid.authorRimmele, Martina
orcid.authorMartín, Jaime
orcid.authorNelson, Jenny
orcid.authorPaterson, Alexandra F.
orcid.authorHeeney, Martin::0000-0001-6879-5020
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