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Title: Galvanostatic interruption of lithium insertion into magnetite: Evidence of surface layer formation

Magnetite is a known lithium intercalation material, and the loss of active, nanocrystalline magnetite can be inferred from the open-circuit potential relaxation. Specifically, for current interruption after relatively small amounts of lithium insertion, the potential first increases and then decreases, and the decrease is hypothesized to be due to a formation of a surface layer, which increases the solid-state lithium concentration in the remaining active material. Comparisons of simulation to experiment suggest that the reactions with the electrolyte result in the formation of a thin layer of electrochemically inactive material, which is best described by a nucleation and growth mechanism. Simulations are consistent with experimental results observed for 6, 8 and 32-nm crystals. As a result, simulations capture the experimental differences in lithiation behavior between the first and second cycles.
Authors:
;  [1] ;  [2] ;  [3] ;  [2] ;  [3] ;  [3] ;  [3] ;  [2]
  1. Stony Brook Univ., Stony Brook, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Columbia Univ., New York, NY (United States)
  3. Stony Brook Univ., Stony Brook, NY (United States)
Publication Date:
Report Number(s):
BNL-112126-2016-JA
Journal ID: ISSN 0378-7753
Grant/Contract Number:
SC00112704
Type:
Accepted Manuscript
Journal Name:
Journal of Power Sources
Additional Journal Information:
Journal Volume: 321; Journal Issue: C; Journal ID: ISSN 0378-7753
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; galvanostatic; magnetite; surface layer formation
OSTI Identifier:
1287087
Alternate Identifier(s):
OSTI ID: 1345841

Nicholas W. Brady, Takeuchi, Esther S., Knehr, K. W., Cama, Christina A., Lininger, Christianna N., Lin, Zhou, Marschilok, Amy C., Takeuchi, Kenneth J., and West, Alan C.. Galvanostatic interruption of lithium insertion into magnetite: Evidence of surface layer formation. United States: N. p., Web. doi:10.1016/j.jpowsour.2016.04.117.
Nicholas W. Brady, Takeuchi, Esther S., Knehr, K. W., Cama, Christina A., Lininger, Christianna N., Lin, Zhou, Marschilok, Amy C., Takeuchi, Kenneth J., & West, Alan C.. Galvanostatic interruption of lithium insertion into magnetite: Evidence of surface layer formation. United States. doi:10.1016/j.jpowsour.2016.04.117.
Nicholas W. Brady, Takeuchi, Esther S., Knehr, K. W., Cama, Christina A., Lininger, Christianna N., Lin, Zhou, Marschilok, Amy C., Takeuchi, Kenneth J., and West, Alan C.. 2016. "Galvanostatic interruption of lithium insertion into magnetite: Evidence of surface layer formation". United States. doi:10.1016/j.jpowsour.2016.04.117. https://www.osti.gov/servlets/purl/1287087.
@article{osti_1287087,
title = {Galvanostatic interruption of lithium insertion into magnetite: Evidence of surface layer formation},
author = {Nicholas W. Brady and Takeuchi, Esther S. and Knehr, K. W. and Cama, Christina A. and Lininger, Christianna N. and Lin, Zhou and Marschilok, Amy C. and Takeuchi, Kenneth J. and West, Alan C.},
abstractNote = {Magnetite is a known lithium intercalation material, and the loss of active, nanocrystalline magnetite can be inferred from the open-circuit potential relaxation. Specifically, for current interruption after relatively small amounts of lithium insertion, the potential first increases and then decreases, and the decrease is hypothesized to be due to a formation of a surface layer, which increases the solid-state lithium concentration in the remaining active material. Comparisons of simulation to experiment suggest that the reactions with the electrolyte result in the formation of a thin layer of electrochemically inactive material, which is best described by a nucleation and growth mechanism. Simulations are consistent with experimental results observed for 6, 8 and 32-nm crystals. As a result, simulations capture the experimental differences in lithiation behavior between the first and second cycles.},
doi = {10.1016/j.jpowsour.2016.04.117},
journal = {Journal of Power Sources},
number = C,
volume = 321,
place = {United States},
year = {2016},
month = {4}
}