Title Understanding and promoting the rapid preparation of the triplite-phase of $LiFeSO_{4}F$ for use as a large-potential Fe cathode Author Ati, Mohamed Sathiya, Mariyappan Boulineau, Sylvain Reynaud, Marine Abakumov, Artem Rousse, Gwenaelle Melot, Brent Van Tendeloo, Gustaaf Tarascon, Jean-Marie Faculty/Department Faculty of Sciences. Physics Publication type article Publication 2012 Washington, D.C. , 2012 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. E-info http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000310720900041&DestLinkType=RelatedRecords&DestApp=ALL_WOS&UsrCustomerID=ef845e08c439e550330acc77c7d2d848 http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000310720900041&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=ef845e08c439e550330acc77c7d2d848 http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000310720900041&DestLinkType=CitingArticles&DestApp=ALL_WOS&UsrCustomerID=ef845e08c439e550330acc77c7d2d848 Handle