Journal
ACS MACRO LETTERS
Volume 10, Issue 8, Pages 1061-1067Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsmacrolett.1c00328
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Funding
- National Science Foundation (NSF CAREER Award) [1653909]
- Polymers Program at the National Science Foundation [1554957]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1653909] Funding Source: National Science Foundation
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1554957] Funding Source: National Science Foundation
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A new generation of polymers designed for OECTs successfully addressed the long-term performance and stability challenges, exhibiting high charge mobility and volumetric capacitance values. The PProDOT-DPP thin films demonstrated excellent electrochemical response and retained performance stability after multiple cycles and prolonged use.
Organic electrochemical transistors (OECTs) are oft-used for bioelectronic applications, and a variety of OECT channel materials have been developed in recent years. However, the majority of these materials are still limited by long-term performance and stability challenges. To resolve these issues, we implemented a next-generation design of polymers for OECTs. Specifically, diketopyrrolopyrrole (DPP) building blocks were copolymerized with propylene dioxythiophene-based (Pro-based) monomers to create a donor-acceptor-type conjugated polymer (PProDOT-DPP). These PProDOT-DPP macromolecules were synthesized using a straightforward direct arylation polymerization synthetic route. The PProDOT-DPP polymer thin film exhibited excellent electrochemical response, low oxidation potential, and high crystallinity, as evidenced by spectroelectrochemical measurements and grazing incidence wide-angle X-ray scattering measurements. Thus, the resultant polymer thin films had high charge mobility and volumetric capacitance values (i.e., mu C* as high as 310 F cm(-1) V-1 s(-1)) when they were used as the active layer materials in OECT devices, which places PProDOT-DPP among the highest performing accumulation-mode OECT polymers reported to date. The performance of the PProDOT-DPP thin films was also retained for 100 cycles and over 2000 s of ON-OFF cycling, indicating the robust stability of the materials. Therefore, this effort provides a clear roadmap for the design of electrochemically active macromolecules for accumulation-mode OECTs, where crystalline acceptor cores are incorporated into an all-donor polymer. We anticipate that this will ultimately inspire future polymer designs to enable OECTs with both high electrical performance and operational stability.
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