Title
Understanding and promoting the rapid preparation of the triplite-phase of <tex>$LiFeSO_{4}F$</tex> for use as a large-potential Fe cathode Understanding and promoting the rapid preparation of the triplite-phase of <tex>$LiFeSO_{4}F$</tex> for use as a large-potential Fe cathode
Author
Faculty/Department
Faculty of Sciences. Physics
Publication type
article
Publication
Washington, D.C. ,
Subject
Chemistry
Source (journal)
Journal of the American Chemical Society. - Washington, D.C.
Volume/pages
134(2012) :44 , p. 18380-18387
ISSN
0002-7863
ISI
000310720900041
Carrier
E
Target language
English (eng)
Full text (Publishers DOI)
Affiliation
University of Antwerp
Abstract
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 degrees 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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