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. This study provides insight into the specific effects of aggregation on electrochemistry through a multiscale view of mechanisms for magnetite composite electrodes.
Bock, David C., et al. "Dispersion of Nanocrystalline Fe <sub>3</sub> O <sub>4</sub> within Composite Electrodes: Insights on Battery-Related Electrochemistry." ACS Applied Materials and Interfaces, vol. 8, no. 18, Apr. 2016. https://doi.org/10.1021/acsami.6b01134
Bock, David C., Pelliccione, Christopher J., Zhang, Wei, Wang, Jiajun, Knehr, K. W., Wang, Jun, Wang, Feng, West, Alan C., Marschilok, Amy C., Takeuchi, Kenneth J., & Takeuchi, Esther S. (2016). Dispersion of Nanocrystalline Fe <sub>3</sub> O <sub>4</sub> within Composite Electrodes: Insights on Battery-Related Electrochemistry. ACS Applied Materials and Interfaces, 8(18). https://doi.org/10.1021/acsami.6b01134
Bock, David C., Pelliccione, Christopher J., Zhang, Wei, et al., "Dispersion of Nanocrystalline Fe <sub>3</sub> O <sub>4</sub> within Composite Electrodes: Insights on Battery-Related Electrochemistry," ACS Applied Materials and Interfaces 8, no. 18 (2016), https://doi.org/10.1021/acsami.6b01134
@article{osti_1354336,
author = {Bock, David C. 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, Kenneth J. and others},
title = {Dispersion of Nanocrystalline Fe <sub>3</sub> O <sub>4</sub> within Composite Electrodes: Insights on Battery-Related Electrochemistry},
annote = {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. 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},
url = {https://www.osti.gov/biblio/1354336},
journal = {ACS Applied Materials and Interfaces},
issn = {ISSN 1944-8244},
number = {18},
volume = {8},
place = {United States},
publisher = {American Chemical Society (ACS)},
year = {2016},
month = {04}}
Energy Frontier Research Centers (EFRC) (United States). Center for Mesoscale Transport Properties (m2mt); Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI ID:
1354336
Report Number(s):
BNL--112852-2016-JA
Journal Information:
ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 18 Vol. 8; ISSN 1944-8244
Basinski, Zbigniew Stanislaw; Hume-Rothery, William; Sutton, A. L.
Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences, Vol. 229, Issue 1179, p. 459-467https://doi.org/10.1098/rspa.1955.0102