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Title: Localized concentration reversal of lithium during intercalation into nanoparticles

Nanoparticulate electrodes, such as Li xFePO 4, have unique advantages over their microparticulate counterparts for the applications in Li-ion batteries because of the shortened diffusion path and access to nonequilibrium routes for fast Li incorporation, thus radically boosting power density of the electrodes. However, how Li intercalation occurs locally in a single nanoparticle of such materials remains unresolved because real-time observation at such a fine scale is still lacking. We report visualization of local Li intercalation via solid-solution transformation in individual Li xFePO 4 nanoparticles, enabled by probing sub-angstrom changes in the lattice spacing in situ. The real-time observation reveals inhomogeneous intercalation, accompanied with an unexpected reversal of Li concentration at the nanometer scale. The origin of the reversal phenomenon is elucidated through phase-field simulations, and it is attributed to the presence of structurally different regions that have distinct chemical potential functions. Furthermore, the findings from this study provide a new perspective on the local intercalation dynamics in battery electrodes.
Authors:
ORCiD logo [1] ; ORCiD logo [2] ; ORCiD logo [1] ; ORCiD logo [3] ; ORCiD logo [4] ; ORCiD logo [5] ; ORCiD logo [1] ;  [6] ;  [7] ; ORCiD logo [5] ;  [5] ;  [8] ; ORCiD logo [1] ; ORCiD logo [6] ; ORCiD logo [7] ; ORCiD logo [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Univ. of Michigan, Ann Arbor, MI (United States); Michigan State Univ., East Lansing, MI (United States)
  3. Univ. of Cambridge, Cambridge (United Kingdom); Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  5. Chinese Academy of Sciences, Ningbo (People's Republic of China)
  6. Univ. of Michigan, Ann Arbor, MI (United States)
  7. Univ. of Cambridge, Cambridge (United Kingdom)
  8. Univ. of California, Berkeley, CA (United States)
Publication Date:
Report Number(s):
BNL-203647-2018-JAAM
Journal ID: ISSN 2375-2548
Grant/Contract Number:
SC0012704
Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 4; Journal Issue: 1; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Energy Frontier Research Centers (EFRC) (United States). Northeastern Center for Chemical Energy Storage (NECCES); Energy Frontier Research Centers (EFRC) (United States). Center for Mesoscale Transport Properties (m2M)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE
OSTI Identifier:
1438434

Zhang, Wei, Yu, Hui -Chia, Wu, Lijun, Liu, Hao, Abdellahi, Aziz, Qiu, Bao, Bai, Jianming, Orvananos, Bernardo, Strobridge, Fiona C., Zhou, Xufeng, Liu, Zhaoping, Ceder, Gerbrand, Zhu, Yimei, Thornton, Katsuyo, Grey, Clare P., and Wang, Feng. Localized concentration reversal of lithium during intercalation into nanoparticles. United States: N. p., Web. doi:10.1126/sciadv.aao2608.
Zhang, Wei, Yu, Hui -Chia, Wu, Lijun, Liu, Hao, Abdellahi, Aziz, Qiu, Bao, Bai, Jianming, Orvananos, Bernardo, Strobridge, Fiona C., Zhou, Xufeng, Liu, Zhaoping, Ceder, Gerbrand, Zhu, Yimei, Thornton, Katsuyo, Grey, Clare P., & Wang, Feng. Localized concentration reversal of lithium during intercalation into nanoparticles. United States. doi:10.1126/sciadv.aao2608.
Zhang, Wei, Yu, Hui -Chia, Wu, Lijun, Liu, Hao, Abdellahi, Aziz, Qiu, Bao, Bai, Jianming, Orvananos, Bernardo, Strobridge, Fiona C., Zhou, Xufeng, Liu, Zhaoping, Ceder, Gerbrand, Zhu, Yimei, Thornton, Katsuyo, Grey, Clare P., and Wang, Feng. 2018. "Localized concentration reversal of lithium during intercalation into nanoparticles". United States. doi:10.1126/sciadv.aao2608. https://www.osti.gov/servlets/purl/1438434.
@article{osti_1438434,
title = {Localized concentration reversal of lithium during intercalation into nanoparticles},
author = {Zhang, Wei and Yu, Hui -Chia and Wu, Lijun and Liu, Hao and Abdellahi, Aziz and Qiu, Bao and Bai, Jianming and Orvananos, Bernardo and Strobridge, Fiona C. and Zhou, Xufeng and Liu, Zhaoping and Ceder, Gerbrand and Zhu, Yimei and Thornton, Katsuyo and Grey, Clare P. and Wang, Feng},
abstractNote = {Nanoparticulate electrodes, such as LixFePO4, have unique advantages over their microparticulate counterparts for the applications in Li-ion batteries because of the shortened diffusion path and access to nonequilibrium routes for fast Li incorporation, thus radically boosting power density of the electrodes. However, how Li intercalation occurs locally in a single nanoparticle of such materials remains unresolved because real-time observation at such a fine scale is still lacking. We report visualization of local Li intercalation via solid-solution transformation in individual LixFePO4 nanoparticles, enabled by probing sub-angstrom changes in the lattice spacing in situ. The real-time observation reveals inhomogeneous intercalation, accompanied with an unexpected reversal of Li concentration at the nanometer scale. The origin of the reversal phenomenon is elucidated through phase-field simulations, and it is attributed to the presence of structurally different regions that have distinct chemical potential functions. Furthermore, the findings from this study provide a new perspective on the local intercalation dynamics in battery electrodes.},
doi = {10.1126/sciadv.aao2608},
journal = {Science Advances},
number = 1,
volume = 4,
place = {United States},
year = {2018},
month = {1}
}