Solvent‐Free Mechano‐Thermal Synthesis of a Li‐Zn Phosphonate Cathode Framework
(2025) Batteries & Supercaps — Vol. 202500426 (2025)
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- Authors
Chanteux, Géraldine 
Kachmar, Andrii
- Abstract
- A key challenge in synthesizing alkali-ion metal–organic frameworks (MOFs) lies in the multistep procedures typically required, often involving solvothermal crystallization, desolvation, post-synthetic alkali-metalation, and controlled drying. To address this, a solvent-free mechano-thermal method is reported that combines solid-state grinding of precursors with thermal annealing under vacuum. This direct, scalable route offers a more sustainable alternative while enabling stoichiometric precision. We demonstrate this approach for the synthesis of Li4-Zn-p-DOBDP_mt (LZP3; p-DOBDP6− = 2,5-dioxido-1,4-benzenediphosphate), in which lithium is incorporated during MOF formation. The resulting material exhibits better crystallinity compared to its conventionally synthesized counterpart and retains its key functional properties, including a reversible capacity of 130 mAhg−1 at 3.2 V versus Li+/Li and a quasi-solid-state ionic conductivity of 10−6 S cm−1 at 303 K. These results underscore the viability of solid-state synthesis for constructing alkali-ion-containing organic electrode materials with reduced processing complexity.
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Citations
Ramackers, A., Darsi Rambabu, Goossens, T., Bakuru, V. R., Apostol, P., Markowski, R., Chanteux, G., Kachmar, A., Frano, V., Esser, G., Malherbe, N., Zhang, Y., Lucaccioni, F., Filinchuk, Y., & Vlad, A. (2025). Solvent‐Free Mechano‐Thermal Synthesis of a Li‐Zn Phosphonate Cathode Framework. Batteries & Supercaps, 202500426. https://doi.org/10.1002/batt.202500426 (Original work published 2025)