本研究使用正負離子對單體(META, AMPS)、兩性分子單體(SBMA)及其線性聚合物Poly(SBMA)於自由基反應合成三種聚合物：由META、AMPS共聚為MA、反應中額外添加Poly(SBMA)為MAPS、使SBMA取代離子對單體與Poly(SBMA)進行聚合為SPS；再摻入NaClO4 (aq)電解液分析其準固態電解質與和超級電容器的電化學行為。聚合物電解質經導入12m NaClO4 (aq) 後可達最大離子導電率(MA, MAPS, SPS: 81.87, 91.03, 110.51 mS/cm)，同樣為離子對所構成，SPS有規律的電荷分布使之表現最佳，MAPS相較MA的優異表現則為Poly(SBMA)貢獻；兩性材料中的電荷間是否有效地提供作用可經由高溫下分子行為比較，如同電解質對於鹽類解離、離子移動的影響，SPS結構中穩定的交互作用力需要更高的溫度才可破壞。電解液中含有的大量離子使研究採用對稱式組裝的水性超級電容器在1.5V下運作無產生水電解反應，擴展電化學視窗可讓裝置於安全操作下發揮優異的儲能表現(c-MA, c-MAPS, c-SPS: 122.2, 131.4, 142.5 F/g)，c-SPS的突出表現歸功於電解質的低阻抗、良好的電解質/電極介面、以及快速的離子傳遞行為；在改變CV電位掃描速率與GCD施加電流等不同工作條件下c-SPS均擁有三者中最佳的比電容值，為高能量密度(41.0 Wh/kg)、高功率密度(4770.8 W/kg)的超級電容器。

The study demonstrates three different ways of fabricating polymer matrix using pair-ions and linear poly(sulfobetaine methacrylate), Poly(SBMA), via copolymerization, the properties of each type acted as gel electrolyte in presence of sodium perchlorate (NaClO4) salt and the performances within carbon-based symmetric supercapacitor are presented in the letter. MA, polymer derived from random polymerization of single-charged monomer, MAPS, an interpenetrating network of MA with Poly(SBMA), and SPS, MAPS-like structure constructed by SBMA monomer instead, which could reach the highest ionic conductivity of 81.87, 91.03, 110.51 mS cm-1, respectively, with 12m NaClO4 (aq) intake. Furthermore, supercapacitors containing gel electrolyte (c-MA, c-MAPS, c-SPS) all possessed wide electrochemical potential window of 1.5 V and high specific capacitance of 122.2, 131.4, 142.5 F g-1, respectively, under 1 A g-1. Among three items, c-SPS with well-designed, regular-immobilized pair-ions polymer structure showed superior performance by delivering high energy density of 41.0 Wh kg-1, and high power density of 4770.8 W kg-1.

Oyedotun, K.O. et al., (2023). Advances in Supercapacitor Development: Materials, Processes, and Applications. J. Electron. Mater., Vol. 52, pp. 96-129
Molahalli, V. et al., (2023). Past decade of supercapacitor research – Lessons learned for future innovations. J. Energy Storage, Vol. 70, No. 15, 108062
Mahala, S., Khosravinia, K., & Kiani, A., (2023). Unwanted degradation in pseudocapacitors: Challenges and opportunities. J. Energy Storage, Vol. 67, No. 1, 107558
Loganathan, N.N. et al., (2022). Recent studies on polymeric materials for supercapacitor development. J. Energy Storage, Vol. 49, 104149
Liew, S.Q., & Jun, H.K., (2022). Fundamentals, Mechanism, and Materials for Hybrid Supercapacitors. In: Thomas, S. , Gueye, A.B., & Gupta, R.K. (Eds.), Nanostructured Materials for Supercapacitors, pp. 71-100. Cham, Switzerland: Springer
Gebbie, M.A. et al., (2023). Linking Electric Double Layer Formation to Electrocatalytic Activity. ACS Catal., Vol. 13, pp. 16222-116239
Helmholtz, H., (1853). Ueber einige Gesetze der Vertheilung elektrischer Ströme in körperlichen Leitern mit Anwendung auf die thierisch-elektrischen Versuche. Ann. Phys.,Vol. 165, No. 6, pp. 211-233
Gouy, M., (1910). Sur la constitution de la charge électrique á la surface d'un électrolyte. J. Phys.: Theor. Appl., Vol. 9, No. 1, pp. 457-468
Chapman, D.L., (1913). A Contribution to the Theory of Electrocapillarity. Philos. Mag., Vol. 25, No. 148, pp. 475-481
Stern, O., (1924). Zur Theorie Der Elektrolytischen Doppelschicht. Z. Elektrochem. Angew. Phys. Chem., Vol. 30, pp. 508-516
Grahame, D.C., (1947). The Electrical Double Layer and the Theory of Electrocapillarity. Chem. Rev., Vol. 41, No. 3, pp. 441-501
Wu, J.Z., (2022). Understanding the Electric Double-Layer Structure, Capacitance, and Charging Dynamics. Chem. Rev., Vol. 122, pp. 10821-10859
Alipoori, S. et al., (2020). Review of PVA-based gel polymer electrolytes in flexible solid-state supercapacitors: Opportunities and challenges. J. Energy Storage, Vol. 27, 101072
Liu, Z.L. et al., (2023). Insights into quasi solid-state polymer electrolyte: The influence of succinonitrile on polyvinylene carbonate electrolyte in view of electrochemical applications. Battery Energy, Vol. 2, No. 3
Ren, W. et al., (2021). Advanced gel polymer electrolytes for safe and durable lithium metal batteries: Challenges, strategies, and perspectives. Energy Storage Mater., Vol. 34, pp. 515-535
Lee, H. et al., (2023). A flexible, high-energy density, and temperature-tolerant asymmetric supercapacitor based on water-in-salt gel electrolyte. J. Alloys Compd., Vol. 960
Qu, K. et al., (2022). Structures, properties, and applications of zwitterionic polymers. ChemPhysMatter, Vol. 1, No. 4, pp. 294-309
Li, W.C. et al., (2022). Superior performances of supercapacitors and lithium-ion batteries with carboxymethyl cellulose bearing zwitterions as binders. J. Taiwan Inst. Chem. Eng., Vol. 133, 104263
Willcock, H. et al., (2014). One-pot synthesis of responsive sulfobetaine nanoparticles by RAFT polymerisation: the effect of branching on the UCST cloud point. Polym. Chem., Vol. 5, No. 3, pp. 1023-1030
Shao, Y.L. et al., (2018). Design and Mechanisms of Asymmetric Supercapacitors. Chem. Rev., Vol. 118, No. 18, pp. 9233-9280
Lalani, R, & Liu, L, (2011). Synthesis, characterization, and electrospinning of zwitterionic poly(sulfobetaine methacrylate). Polymer, Vol. 52, pp. 5344-5354
Finney, A.R. et al., (2019). Ion Association in Lanthanide Chloride Solutions. Chem. Eur. J., Vol. 25, No. 37, pp. 8725-8740
Laschuk, N.O., Easton, E.B., & Zenkina, O.V., (2021). Reducing the resistance for the use of electrochemical impedance spectroscopy analysis in materials chemistry. RSC Adv., Vol. 11, No. 45, pp. 27925-27936
Wang, Y.H. et al., (2021). In situ Raman spectroscopy reveals the structure and dissociation of interfacial water. Nature, Vol. 600, pp. 81-85