Preparation, structure, and electrochemistry of layered polyanionic hydroxysulfates: LiMSO4OH (M = Fe, Co, Mn) electrodes for Li-ion batteries

Chinmayee V. Subban, Mohamed Ati, Gwenaëlle Rousse, Artem M. Abakumov, Gustaaf Van Tendeloo, Raphaël Janot, Jean Marie Tarascon

Research output: Contribution to journalArticlepeer-review

61 Citations (Scopus)

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+/Li0, 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 +/Li0. Besides, these compounds can be easily made at temperatures near 200 C via a synthesis process that enlists a new intermediate phase of composition M3(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.

Original languageEnglish
Pages (from-to)3653-3661
Number of pages9
JournalJournal of the American Chemical Society
Volume135
Issue number9
DOIs
Publication statusPublished - 6 Mar 2013
Externally publishedYes

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