Amorphous coordination polymers for versatile Mg2+, Ca2+, Sr2+, Ba2+, and Zn2+ cation storage

Guo, Xiaolong;Markowski, Robert;Black, Ashley;Apostol, Petru;Vlad, Alexandru;et.al.
(2025) Energy & Environmental Science — Vol. 18, n° 20, p. 9114-9124 (2025)

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Abstract
Divalent metal-ion batteries hold immense promise for electrochemical energy storage applications, offering advantages in terms of volumetric capacity, cost-efficiency, sustainability, and safety. Despite advances, the lack of high-voltage and high-performance positive electrode materials remains a critical obstacle. Here, we disclose a family of amorphous coordination polymers capable of reversibly storing Mg2+, Ca2+, Sr2+, Ba2+, and Zn2+ cations. For Ca2+ and Mg2+ systems, the highest reported working potentials of >3.2 V vs. Ca2+/Ca and 2.8 V vs. Mg2+/Mg are measured, along with fast, stable, and low-hysteresis storage without solvent or ion pair storage. These characteristics stem from the amorphous structure, delocalized anionic charge, and disordered, long bond-distance coordination, enabling weak binding and fast cation diffusion. Using sustainable elements and demonstrating universal divalent cation storage capacity by achieving the first-ever reversible storage of Sr2+ and Ba2+ ions, this work establishes key design principles for divalent cation storage materials and systems.
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Guo, X., Markowski, R., Black, A., Apostol, P., Darsi Rambabu, Lužanin, O., Pavčnik, T., Monti, D., Du, M., Tie, D., Lin, X., Bakuru, V. R., Delogne, R., Robeyns, K., Simonelli, L., Gohy, J.-F., Bitenc, J., Wang, J., Ponrouch, A., & Vlad, A. (2025). Amorphous coordination polymers for versatile Mg2+, Ca2+, Sr2+, Ba2+, and Zn2+ cation storage. Energy & Environmental Science, 18(20), 9114-9124. https://doi.org/10.1039/d5ee02567b (Original work published 2025)