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Title: Structural Transformation of LiFePO 4 during Ultrafast Delithiation

The prolific lithium battery electrode material lithium iron phosphate (LiFePO 4) stores and releases lithium ions by undergoing a crystallographic phase change. Nevertheless, it performs unexpectedly well at high rate and exhibits good cycling stability. Here we investigate here the ultrafast charging reaction to resolve the underlying mechanism while avoiding the limitations of prevailing electrochemical methods by using a gaseous oxidant to deintercalate lithium from the LiFePO 4 structure. Oxidizing LiFePO 4 with nitrogen dioxide gas reveals structural changes through in situ synchrotron X-ray diffraction and electronic changes through in situ UV/vis reflectance spectroscopy. This study clearly shows that ultrahigh rates reaching 100% state of charge in 10 s does not lead to a particle-wide union of the olivine and heterosite structures. An extensive solid solution phase is therefore not a prerequisite for ultrafast charge/discharge.
Authors:
ORCiD logo [1] ;  [1] ;  [1] ;  [1] ; ORCiD logo [2] ;  [3] ;  [1]
  1. Univ. of Quebec, Montreal, QC (Canada). Dept. de chimie
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  3. Johnson Matthey Battery Materials Ltd, Candiac, QC (Canada)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 8; Journal Issue: 24; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Natural Sciences and Engineering Research Council of Canada (NSERC)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 25 ENERGY STORAGE; lithium-ion; In-Situ; Uv-vis; XRD; biphasic; electronic structure; reaction mechanism; structural analysis
OSTI Identifier:
1425270

Kuss, Christian, Trinh, Ngoc Duc, Andjelic, Stefan, Saulnier, Mathieu, Dufresne, Eric M., Liang, Guoxian, and Schougaard, Steen B.. Structural Transformation of LiFePO4 during Ultrafast Delithiation. United States: N. p., Web. doi:10.1021/acs.jpclett.7b02569.
Kuss, Christian, Trinh, Ngoc Duc, Andjelic, Stefan, Saulnier, Mathieu, Dufresne, Eric M., Liang, Guoxian, & Schougaard, Steen B.. Structural Transformation of LiFePO4 during Ultrafast Delithiation. United States. doi:10.1021/acs.jpclett.7b02569.
Kuss, Christian, Trinh, Ngoc Duc, Andjelic, Stefan, Saulnier, Mathieu, Dufresne, Eric M., Liang, Guoxian, and Schougaard, Steen B.. 2017. "Structural Transformation of LiFePO4 during Ultrafast Delithiation". United States. doi:10.1021/acs.jpclett.7b02569. https://www.osti.gov/servlets/purl/1425270.
@article{osti_1425270,
title = {Structural Transformation of LiFePO4 during Ultrafast Delithiation},
author = {Kuss, Christian and Trinh, Ngoc Duc and Andjelic, Stefan and Saulnier, Mathieu and Dufresne, Eric M. and Liang, Guoxian and Schougaard, Steen B.},
abstractNote = {The prolific lithium battery electrode material lithium iron phosphate (LiFePO4) stores and releases lithium ions by undergoing a crystallographic phase change. Nevertheless, it performs unexpectedly well at high rate and exhibits good cycling stability. Here we investigate here the ultrafast charging reaction to resolve the underlying mechanism while avoiding the limitations of prevailing electrochemical methods by using a gaseous oxidant to deintercalate lithium from the LiFePO4 structure. Oxidizing LiFePO4 with nitrogen dioxide gas reveals structural changes through in situ synchrotron X-ray diffraction and electronic changes through in situ UV/vis reflectance spectroscopy. This study clearly shows that ultrahigh rates reaching 100% state of charge in 10 s does not lead to a particle-wide union of the olivine and heterosite structures. An extensive solid solution phase is therefore not a prerequisite for ultrafast charge/discharge.},
doi = {10.1021/acs.jpclett.7b02569},
journal = {Journal of Physical Chemistry Letters},
number = 24,
volume = 8,
place = {United States},
year = {2017},
month = {12}
}