Exploring Self-Doped Conjugated Polyelectrolytes for All-Polymer Solid-State Supercapacitors

Ha N.-T. Yip B.R.P. Kusherbayev A. Bui Thi Thu T. Pham T.T. Bazan G.C. Nguyen-Dang T.
22 December 2025 American Chemical Society

ACS Applied Energy Materials
2025 #8 Issue 24 18346 - 18354 pp.

In this work, we explore the application of self-doped conjugated polyelectrolytes (CPEs) in all-polymer solid-state supercapacitors, aiming to develop safe, flexible, and environmentally friendly energy storage systems. Using poly[2,6-(4,4-bis-potassium butanylsulfonate-4H-cyclopenta-[2,1-b; 3,4-b′]-dithiophene)-alt-4,7-(2,1,3-benzothiadiazole)] (commonly referred to as CPE-K) as the electrode material, we fabricated both symmetric and asymmetric supercapacitor devices. A biodegradable poly(vinyl alcohol)/sulfuric acid (PVA/H₂SO₄) gel served as the electrolyte in both configurations, while poly(3,4-ethylenedioxythiophene):poly(styrenesulfonic acid) (PEDOT:PSS) was employed as the anode in the asymmetric setup. Electrochemical characterization showed that symmetric CPE-K devices achieved a specific capacitance of 28.13 F g^–1, an energy density of 1.41 Wh kg^–1, and operated within a voltage window of 0.6 V. In contrast, the asymmetric devices extended the voltage window to 1.6 V, delivering a maximum energy density of 6.01 Wh kg^–1 at a current density of 1 A g^–1, surpassing the performance of symmetric PEDOT:PSS-based devices. Both configurations demonstrated excellent cycling stability and Coulombic efficiency. Mechanical and thermal abuse tests confirmed the robustness of the solid-state architecture with capacitance enhancements under compressive pressures up to 8 MPa and stable operation at temperatures up to 100 °C. These findings underscore the potential of conjugated polyelectrolyte-based supercapacitors for next-generation energy storage applications that demand mechanical resilience and thermal safety.

conjugated polyelectrolytes , energy storage , organic mixed ionic–electronic conductors , solid state , supercapacitor

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Center for Environmental Intelligence, VinUniversity, Gia-Lam, Hanoi, 100000, Viet Nam
College of Engineering and Computer Science, VinUniversity, Gia-Lam, Hanoi, 100000, Viet Nam
Departments of Chemistry and Chemical & Biomolecular Engineering, National University of Singapore, Singapore, 119077, Singapore
Department of Biology, School of Sciences and Humanities, Nazarbayev University, Astana, 010000, Kazakhstan

Center for Environmental Intelligence
College of Engineering and Computer Science
Departments of Chemistry and Chemical & Biomolecular Engineering
Department of Biology

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