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    Probing Comonomer Selection Effects on Dioxythiophene-Based Aqueous-Compatible Polymers for Redox Applications

    Year: 2022

    Journal: Chem. Mat., Volume 34, MAY 24, page 4633–4645

    Authors: Advincula, Abigail A.; Jones, Austin L.; Thorley, Karl J.; Osterholm, Anna M.; Ponder, James F., Jr.; Reynolds, John R.

    Organizations: Department of the Navy, Office of Naval Research [N00014-20-1-2129]; Department of Defense (DoD) through the National Defense Science & Engineering Graduate Fellowship (NDSEG) Program; National Science Foundation [ECCS-1542174]

    Oligoether-functionalized dioxythiophene polymers are a promising classof materials for electrochemical applications requiring aqueous electrolytes with rapid,reversible redox behavior, high pseudocapacitance, and strong electrochromic contrast.By copolymerizing different monomers (EDOT, DMP, and PheDOT) with anoligoether-functionalized propylenedioxythiophene unit, we tune the redox properties,modulating the onsets of oxidation, redox kinetics, and conductance properties in anaqueous electrolyte (NaCl/H2O). Density functional theory calculations aresubsequently employed to establish a theoretical basis for the observed differences inenergy levels of the polymers. Polymerfilms demonstrate <1 s discharge rates, <1.5 selectrochromic switching times, and 90% charge retention after 1000 cycles. As these materials demonstrate rapid and reversibleredox behavior, we test the utility of these materials as electrochromes and as active layers in type I aqueous supercapacitors. In bothaqueous and organic electrolytes, these materials demonstrate high electrochromic contrasts, with comonomer selection altering thecolors of the resultant polymers. As active layers in supercapacitors, all polymers show relatively constant current response as afunction of cell voltage, and P(OE3)-E, in a test device, demonstrates high current retention after 15,000 charge/discharge cycles.This work demonstrates the broad utility of oligoether-functionalized dioxythiophenes for aqueous redox applications while detailingthe tuning of optical, electrochemical, and conductance properties through comonomer selection.
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