Title
Preparation, structure, and electrochemistry of layered polyanionic hydroxysulfates : <tex>$LiMSO_{4}OH$</tex> (M = Fe, Co, Mn) electrodes for Li-Ion batteries
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
135(2013) :9 , p. 3653-3661
ISSN
0002-7863
ISI
000315936700056
Carrier
E
Target language
English (eng)
Full text (Publishers DOI)
Affiliation
University of Antwerp
Abstract
The Li-ion rechargeable battery, due to its high energy density, has driven remarkable advances in portable electronics. Moving toward more sustainable electrodes could make this technology even more attractive to large-volume applications. We present here a new family of 3d-metal hydroxysulfates of general formula LiMSO4OH (M = Fe, Co, and Mn) among which (i) LiFeSO4OH reversibly releases 0.7 Li+ at an average potential of 3.6 V vs Li+/Li-0, slightly higher than the potential of currently lauded LiFePO4 (3.45 V) electrode material, and (ii) LiCoSO4OH shows a redox activity at 4.7 V vs Li+/Li-0. Besides, these compounds can be easily made at temperatures near 200 degrees C via a synthesis process that enlists a new intermediate phase of composition M-3(SO4)(2)(OH)(2) (M = Fe, Co, Mn, and Ni), related to the mineral caminite. Structurally, we found that LiFeSO4OH is a layered phase unlike the previously reported 3.2 V tavorite LiFeSO4OH. This work should provide an impetus to experimentalists for designing better electrolytes to fully tap the capacity of high-voltage Co-based hydroxysulfates, and to theorists for providing a means to predict the electrochemical redox activity of two polymorphs.
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