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Title: Essential Role of Spinel MgFe 2 O 4 Surfaces during Discharge

Abstract

Spinel magnesium ferrite (MgFe2O4) is a prospective anode material in lithium ion battery (LIB) due to its large theoretical capacity. Here, we employed Density Functional Theory (DFT) to study the contribution from diverse facets of three spinel systems of MgFe2O4, normal-spinel, mixed-spinel and inverse-spinel, to the initial discharge behaviors. The mixed-spinel (1 0 0) surface terminated by MgFeOx is found to be the most active among the diverse surfaces studied. It can provide the high capacity, the high voltage and facile Li+ transport during the initial discharge stage. The high performance is found to be associated with the high surface activity to capture Li+ ions, and the ability to accommodate a large amount of Li+ ions and facilitate the sequential smooth transport to subsurface. The DFT-estimated discharge voltages based on the mixed-spinel (1 0 0) surface terminated by MgFeOx are much higher than those using the stoichiometric bulk models and fit well with the corresponding experimental measurement at the initial stage. Our results develop new design strategies for optimization of particle morphologies, enabling the enhancement in stability and discharge performance of ferrite materials.

Authors:
; ; ; ; ; ; ORCiD logo
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Mesoscale Transport Properties (m2mt); Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1605952
Alternate Identifier(s):
OSTI ID: 1617291
Report Number(s):
BNL-215899-2020-JAAM
Journal ID: ISSN 1945-7111
Grant/Contract Number:  
SC0012704
Resource Type:
Published Article
Journal Name:
Journal of the Electrochemical Society (Online)
Additional Journal Information:
Journal Name: Journal of the Electrochemical Society (Online) Journal Volume: 167 Journal Issue: 9; Journal ID: ISSN 1945-7111
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Guo, Haoyue, Durham, Jessica L., Brady, Alexander B., Marschilok, Amy C., Takeuchi, Esther S., Takeuchi, Kenneth J., and Liu, Ping. Essential Role of Spinel MgFe 2 O 4 Surfaces during Discharge. United States: N. p., 2020. Web. https://doi.org/10.1149/1945-7111/ab7f89.
Guo, Haoyue, Durham, Jessica L., Brady, Alexander B., Marschilok, Amy C., Takeuchi, Esther S., Takeuchi, Kenneth J., & Liu, Ping. Essential Role of Spinel MgFe 2 O 4 Surfaces during Discharge. United States. https://doi.org/10.1149/1945-7111/ab7f89
Guo, Haoyue, Durham, Jessica L., Brady, Alexander B., Marschilok, Amy C., Takeuchi, Esther S., Takeuchi, Kenneth J., and Liu, Ping. Tue . "Essential Role of Spinel MgFe 2 O 4 Surfaces during Discharge". United States. https://doi.org/10.1149/1945-7111/ab7f89.
@article{osti_1605952,
title = {Essential Role of Spinel MgFe 2 O 4 Surfaces during Discharge},
author = {Guo, Haoyue and Durham, Jessica L. and Brady, Alexander B. and Marschilok, Amy C. and Takeuchi, Esther S. and Takeuchi, Kenneth J. and Liu, Ping},
abstractNote = {Spinel magnesium ferrite (MgFe2O4) is a prospective anode material in lithium ion battery (LIB) due to its large theoretical capacity. Here, we employed Density Functional Theory (DFT) to study the contribution from diverse facets of three spinel systems of MgFe2O4, normal-spinel, mixed-spinel and inverse-spinel, to the initial discharge behaviors. The mixed-spinel (1 0 0) surface terminated by MgFeOx is found to be the most active among the diverse surfaces studied. It can provide the high capacity, the high voltage and facile Li+ transport during the initial discharge stage. The high performance is found to be associated with the high surface activity to capture Li+ ions, and the ability to accommodate a large amount of Li+ ions and facilitate the sequential smooth transport to subsurface. The DFT-estimated discharge voltages based on the mixed-spinel (1 0 0) surface terminated by MgFeOx are much higher than those using the stoichiometric bulk models and fit well with the corresponding experimental measurement at the initial stage. Our results develop new design strategies for optimization of particle morphologies, enabling the enhancement in stability and discharge performance of ferrite materials.},
doi = {10.1149/1945-7111/ab7f89},
journal = {Journal of the Electrochemical Society (Online)},
number = 9,
volume = 167,
place = {United States},
year = {2020},
month = {1}
}

Journal Article:
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https://doi.org/10.1149/1945-7111/ab7f89

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