Decoupling ion size from electrochemistry: cation-size-independent accommodation of Li+ to Cs+ in an amorphous sulfonamide coordination polymer
(2026) Chemical Science — Vol. 17, n° 14, p. 6924-6930 (2026)
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- Abstract
- Understanding how cation identity governs charge storage is critical for next-generation batteries beyond lithium. Here we show that the amorphous Ca–Zn–PTtSA coordination polymer functions as a universal host for reversible electrochemical storage of all alkali-metal cations from Li+ to Cs+, including the rare case of reversible Rb+ and Cs+ electrochemical cycling in a positive electrode material. Despite the large variation in ionic radius, all cations yield nearly identical redox potentials, full material utilization (∼95 mAh g−1), and low hysteresis. Elemental and spectroscopic analyses confirm a cation storage mechanism without solvent co-intercalation. This behavior originates from the framework's amorphous flexibility and the delocalized electronic structure of the conjugated sulfonamide ligand, which together enable weak, reversible metal–ligand interactions and fast cation transport (D ≈ 10−9 cm2 s−1). Consequently, M2–Zn–PTtSA delivers high-rate capability and long-term cycling stability across the entire alkali-metal series, providing a platform that decouples ion size from electrochemical performance and supports “cation-of-choice” battery chemistries.
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Markowski, R., Darsi Rambabu, Ramackers, A., & Vlad, A. (2026). Decoupling ion size from electrochemistry: cation-size-independent accommodation of Li+ to Cs+ in an amorphous sulfonamide coordination polymer. Chemical Science, 17(14), 6924-6930. https://doi.org/10.1039/D6SC00585C (Original work published 2026)