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Title: Structural phase transformation and Fe valence evolution in FeOxF2-x/C nanocomposite electrodes during lithiation and de-lithiation processes

Abstract

In this study, the structural changes of FeOxF2-x/C during the first discharge and recharge cycles were studied by ex situ electron microscopy techniques including annular dark field scanning transmission electron microscopy (DF-STEM) imaging, selected area electron diffraction (SAED) and electron energy loss spectroscopy (EELS) as well as by in situ X-ray absorption spectroscopy (XAS). The evolution of the valence state of Fe was determined by combined EELS using the Fe-L edge and XAS using the Fe-K edge. The results of this investigation show that the conversion reaction path during 1st lithiation is very different from the re-conversion path during 1st delithiation. During lithiation, intercalation is first observed followed by conversion into a lithiated rocksalt (Li–Fe–O–F) structure, and metallic Fe and LiF phases. During delithiation, the rocksalt phase does not disappear, but co-exists with an amorphous (rutile type) phase formed initially by the reaction of LiF and Fe. However, a de-intercalation stage is still observed at the end of reconversion similar to a single phase process despite the coexistence of these two (rocksalt and amorphous) phases.

Authors:
; ; ; ; ; ;
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Northeastern Center for Chemical Energy Storage (NECCES)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1382483
DOE Contract Number:  
SC0001294
Resource Type:
Journal Article
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 1; Journal Issue: 38; Related Information: NECCES partners with Stony Brook University (lead); Argonne National Laboratory; Binghamton University; Brookhaven National University; University of California, San Diego; University of Cambridge, UK; Lawrence Berkeley National Laboratory; Massachusetts Institute of Technology; University of Michigan; Rutgers University; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; energy storage (including batteries and capacitors); defects; charge transport; materials and chemistry by design; synthesis (novel materials)

Citation Formats

Sina, M., Nam, K. -W., Su, D., Pereira, N., Yang, X. -Q., Amatucci, G. G., and Cosandey, F. Structural phase transformation and Fe valence evolution in FeOxF2-x/C nanocomposite electrodes during lithiation and de-lithiation processes. United States: N. p., 2013. Web. doi:10.1039/C3TA12109G.
Sina, M., Nam, K. -W., Su, D., Pereira, N., Yang, X. -Q., Amatucci, G. G., & Cosandey, F. Structural phase transformation and Fe valence evolution in FeOxF2-x/C nanocomposite electrodes during lithiation and de-lithiation processes. United States. doi:10.1039/C3TA12109G.
Sina, M., Nam, K. -W., Su, D., Pereira, N., Yang, X. -Q., Amatucci, G. G., and Cosandey, F. Tue . "Structural phase transformation and Fe valence evolution in FeOxF2-x/C nanocomposite electrodes during lithiation and de-lithiation processes". United States. doi:10.1039/C3TA12109G.
@article{osti_1382483,
title = {Structural phase transformation and Fe valence evolution in FeOxF2-x/C nanocomposite electrodes during lithiation and de-lithiation processes},
author = {Sina, M. and Nam, K. -W. and Su, D. and Pereira, N. and Yang, X. -Q. and Amatucci, G. G. and Cosandey, F.},
abstractNote = {In this study, the structural changes of FeOxF2-x/C during the first discharge and recharge cycles were studied by ex situ electron microscopy techniques including annular dark field scanning transmission electron microscopy (DF-STEM) imaging, selected area electron diffraction (SAED) and electron energy loss spectroscopy (EELS) as well as by in situ X-ray absorption spectroscopy (XAS). The evolution of the valence state of Fe was determined by combined EELS using the Fe-L edge and XAS using the Fe-K edge. The results of this investigation show that the conversion reaction path during 1st lithiation is very different from the re-conversion path during 1st delithiation. During lithiation, intercalation is first observed followed by conversion into a lithiated rocksalt (Li–Fe–O–F) structure, and metallic Fe and LiF phases. During delithiation, the rocksalt phase does not disappear, but co-exists with an amorphous (rutile type) phase formed initially by the reaction of LiF and Fe. However, a de-intercalation stage is still observed at the end of reconversion similar to a single phase process despite the coexistence of these two (rocksalt and amorphous) phases.},
doi = {10.1039/C3TA12109G},
journal = {Journal of Materials Chemistry. A},
issn = {2050-7488},
number = 38,
volume = 1,
place = {United States},
year = {2013},
month = {1}
}

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