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Identification of an Intermediate Phase, Li1/2FeSO4F, Formed during Electrochemical Cycling of Tavorite LiFeSO4F

Sobkowiak, Adam (author)
Uppsala universitet,Strukturkemi
Roberts, Matthew R. (author)
Uppsala universitet,Strukturkemi
Häggström, Lennart (author)
Uppsala universitet,Strukturkemi
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Ericsson, Tore (author)
Uppsala universitet,Strukturkemi
Andersson, Anna M. (author)
ABB
Edström, Kristina (author)
Uppsala universitet,Strukturkemi
Gustafsson, Torbjörn (author)
Uppsala universitet,Strukturkemi
Björefors, Fredrik (author)
Uppsala universitet,Strukturkemi
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 (creator_code:org_t)
2014-07-24
2014
English.
In: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 26:15, s. 4620-4628
  • Journal article (peer-reviewed)
Abstract Subject headings
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  • Many compounds adopting the tavorite-type crystal structure have attracted considerable attention as cathode materials for lithium ion batteries due to the favorable structural characteristics, facilitating promising electrochemical performance. Recent reports have highlighted the complex mechanism of lithium insertion/extraction in some of these compounds, such as the stabilization of intermediate phases in the LiFeSO4OH and LiVPO4F systems. In the case of tavorite LiFeSO4F, reported density functional theory (DFT) calculations have suggested the possibility of a similar behavior, but thus far, no experimental verification of such a process has, to the best of our knowledge, been successfully demonstrated. In this work, we investigate the structural evolution of LiFeSO4F upon extraction/insertion of lithium ions from/into the host framework. By thorough ex situ characterizations of chemically and electrochemically prepared LixFeSO4F-samples (0 ≤ x ≤ 1), we demonstrate the stabilization of an intermediate phase, Li1/2FeSO4F, for which one possible structural model is proposed. However, results indicating charge ordering on the iron-sites, suggesting the formation of a super structure with a larger unit cell, are also highlighted. Moreover, the degree of formation of Li1/2FeSO4F is shown to be highly dependent on the rate of lithium extraction as a result of an exceptionally small potential separation (similar to 15 mV during charging) of the two subsequently occurring biphasic processes, LiFeSO4F/Li1/2FeSO4F and Li1/2FeSO4F/FeSO4F. Finally, the intermediate phase is shown to be formed both on charge and discharge during battery cycling, even though an apparent asymmetrical electrochemical trace suggests the contrary.

Subject headings

NATURVETENSKAP  -- Fysik (hsv//swe)
NATURAL SCIENCES  -- Physical Sciences (hsv//eng)
NATURVETENSKAP  -- Kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences (hsv//eng)

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