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Title: Dispersion of nanocrystalline Fe 3O 4 within composite electrodes: Insights on battery-related electrochemistry

Aggregation of nanosized materials in composite lithium-ion-battery electrodes can be a significant factor influencing electrochemical behavior. In this study, aggregation was controlled in magnetite, Fe 3O 4, composite electrodes via oleic acid capping and subsequent dispersion in a carbon black matrix. A heat treatment process was effective in the removal of the oleic acid capping agent while preserving a high degree of Fe 3O 4 dispersion. Electrochemical testing showed that Fe 3O 4 dispersion is initially beneficial in delivering a higher functional capacity, in agreement with continuum model simulations. However, increased capacity fade upon extended cycling was observed for the dispersed Fe 3O 4 composites relative to the aggregated Fe 3O 4 composites. X-ray absorption spectroscopy measurements of electrodes post cycling indicated that the dispersed Fe 3O 4 electrodes are more oxidized in the discharged state, consistent with reduced reversibility compared with the aggregated sample. Higher charge-transfer resistance for the dispersed sample after cycling suggests increased surface-film formation on the dispersed, high-surface-area nanocrystalline Fe 3O 4 compared to the aggregated materials. Furthermore, this study provides insight into the specific effects of aggregation on electrochemistry through a multiscale view of mechanisms for magnetite composite electrodes.
Authors:
;  [1] ;  [2] ;  [2] ;  [2] ;  [3] ;  [2] ;  [2] ;  [3] ;  [1] ;  [1]
  1. Stony Brook Univ., Stony Brook, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Columbia Univ., New York, NY (United States)
Publication Date:
Report Number(s):
BNL-112124-2016-JA
Journal ID: ISSN 1944-8244
Grant/Contract Number:
SC00112704
Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 8; Journal Issue: 18; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society
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; magnetite; composite; aggregate; EXAFS; lithium-ion battery; electrochemical impedance spectroscopy; TXM
OSTI Identifier:
1287086

David C. Bock, Takeuchi, Kenneth J., Pelliccione, Christopher J., Zhang, Wei, Wang, Jiajun, Knehr, K. W., Wang, Jun, Wang, Feng, West, Alan C., Marschilok, Amy C., and Takeuchi, Esther S.. Dispersion of nanocrystalline Fe3O4 within composite electrodes: Insights on battery-related electrochemistry. United States: N. p., Web. doi:10.1021/acsami.6b01134.
David C. Bock, Takeuchi, Kenneth J., Pelliccione, Christopher J., Zhang, Wei, Wang, Jiajun, Knehr, K. W., Wang, Jun, Wang, Feng, West, Alan C., Marschilok, Amy C., & Takeuchi, Esther S.. Dispersion of nanocrystalline Fe3O4 within composite electrodes: Insights on battery-related electrochemistry. United States. doi:10.1021/acsami.6b01134.
David C. Bock, Takeuchi, Kenneth J., Pelliccione, Christopher J., Zhang, Wei, Wang, Jiajun, Knehr, K. W., Wang, Jun, Wang, Feng, West, Alan C., Marschilok, Amy C., and Takeuchi, Esther S.. 2016. "Dispersion of nanocrystalline Fe3O4 within composite electrodes: Insights on battery-related electrochemistry". United States. doi:10.1021/acsami.6b01134. https://www.osti.gov/servlets/purl/1287086.
@article{osti_1287086,
title = {Dispersion of nanocrystalline Fe3O4 within composite electrodes: Insights on battery-related electrochemistry},
author = {David C. Bock and Takeuchi, Kenneth J. and Pelliccione, Christopher J. and Zhang, Wei and Wang, Jiajun and Knehr, K. W. and Wang, Jun and Wang, Feng and West, Alan C. and Marschilok, Amy C. and Takeuchi, Esther S.},
abstractNote = {Aggregation of nanosized materials in composite lithium-ion-battery electrodes can be a significant factor influencing electrochemical behavior. In this study, aggregation was controlled in magnetite, Fe3O4, composite electrodes via oleic acid capping and subsequent dispersion in a carbon black matrix. A heat treatment process was effective in the removal of the oleic acid capping agent while preserving a high degree of Fe3O4 dispersion. Electrochemical testing showed that Fe3O4 dispersion is initially beneficial in delivering a higher functional capacity, in agreement with continuum model simulations. However, increased capacity fade upon extended cycling was observed for the dispersed Fe3O4 composites relative to the aggregated Fe3O4 composites. X-ray absorption spectroscopy measurements of electrodes post cycling indicated that the dispersed Fe3O4 electrodes are more oxidized in the discharged state, consistent with reduced reversibility compared with the aggregated sample. Higher charge-transfer resistance for the dispersed sample after cycling suggests increased surface-film formation on the dispersed, high-surface-area nanocrystalline Fe3O4 compared to the aggregated materials. Furthermore, this study provides insight into the specific effects of aggregation on electrochemistry through a multiscale view of mechanisms for magnetite composite electrodes.},
doi = {10.1021/acsami.6b01134},
journal = {ACS Applied Materials and Interfaces},
number = 18,
volume = 8,
place = {United States},
year = {2016},
month = {4}
}