Understanding and Promoting the Rapid Preparation of the Triplite- Phase of LiFeSO4F for Use as a Large-Potential Fe Cathode - CNRS - Centre national de la recherche scientifique Accéder directement au contenu
Article Dans Une Revue Journal of the American Chemical Society Année : 2012

Understanding and Promoting the Rapid Preparation of the Triplite- Phase of LiFeSO4F for Use as a Large-Potential Fe Cathode

Résumé

The development of new electrode materials, which are composed of Earth-abundant elements and that can be made via eco-efficient processes, is becoming absolutely necessary for reasons of sustainable production. The 3.9 V triplite-phase of LiFeSO4F, compared to the 3.6 V tavorite-phase, could satisfy this requirement provided the currently complex synthetic pathway can be simplified. Here, we present our work aiming at better understanding the reaction mechanism that govern its formation as a way to optimize its preparation. We first demonstrate, using complementary X-ray diffraction and transmission electron microscopy studies, that triplite-LiFeSO4F can nucleate from tavorite-LiFeSO4F via a reconstructive process whose kinetics are significantly influenced by moisture and particle morphology. Perhaps the most spectacular finding is that it is possible to prepare electrochemically active triplite-LiFeSO4F from anhydrous precursors using either reactive spark plasma sintering (SPS) synthesis in a mere 20 min at 320 °C or room-temperature ball milling for 3 h. These new pathways appear to be strongly driven by the easy formation of a disordered phase with higher entropy, as both techniques trigger disorder via rapid annealing steps or defect creation. Although a huge number of phases adopts the tavorite structure-type, this new finding offers both a potential way to prepare new compositions in the triplite structure and a wealth of opportunities for the synthesis of new materials which could benefit many domains beyond energy storage.
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Dates et versions

hal-00794750 , version 1 (26-02-2013)

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Mohamed Ati, Mariyappan Sathiya, Sylvain Boulineau, Marine Reynaud, Artem Abakumov, et al.. Understanding and Promoting the Rapid Preparation of the Triplite- Phase of LiFeSO4F for Use as a Large-Potential Fe Cathode. Journal of the American Chemical Society, 2012, 134, pp.18380-18387. ⟨10.1021/ja3074402⟩. ⟨hal-00794750⟩
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