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Title: Phase transformation mechanism in lithium manganese nickel oxide revealed by single-crystal hard X-ray microscopy

Abstract

Understanding the reaction pathway and kinetics of solid-state phase transformation is critical in designing advanced electrode materials with better performance and stability. Despite the first-order phase transition with a large lattice mismatch between the involved phases, spinel LiMn 1.5Ni 0.5O 4 is capable of fast rate even at large particle size, presenting an enigma yet to be understood. The present study uses advanced two-dimensional and three-dimensional nano-tomography on a series of well-formed LixMn 1.5Ni 0.5O 4 (0 ≤ x ≤ 1) crystals to visualize the mesoscale phase distribution, as a function of Li content at the sub-particle level. Inhomogeneity along with the coexistence of Li-rich and Li-poor phases are broadly observed on partially delithiated crystals, providing direct evidence for a concurrent nucleation and growth process instead of a shrinking-core or a particle-by-particle process. As a result, superior kinetics of (100) facets at the vertices of truncated octahedral particles promote preferential delithiation, whereas the observation of strain-induced cracking suggests mechanical degradation in the material.

Authors:
 [1];  [2]; ORCiD logo [3];  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States); Donghua Univ., Shanghai (China)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1347552
Alternate Identifier(s):
OSTI ID: 1379708
Grant/Contract Number:
AC02-76SF00515; AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; energy; imaging studies

Citation Formats

Kuppan, Saravanan, Xu, Yahong, Liu, Yijin, and Chen, Guoying. Phase transformation mechanism in lithium manganese nickel oxide revealed by single-crystal hard X-ray microscopy. United States: N. p., 2017. Web. doi:10.1038/ncomms14309.
Kuppan, Saravanan, Xu, Yahong, Liu, Yijin, & Chen, Guoying. Phase transformation mechanism in lithium manganese nickel oxide revealed by single-crystal hard X-ray microscopy. United States. doi:10.1038/ncomms14309.
Kuppan, Saravanan, Xu, Yahong, Liu, Yijin, and Chen, Guoying. Wed . "Phase transformation mechanism in lithium manganese nickel oxide revealed by single-crystal hard X-ray microscopy". United States. doi:10.1038/ncomms14309. https://www.osti.gov/servlets/purl/1347552.
@article{osti_1347552,
title = {Phase transformation mechanism in lithium manganese nickel oxide revealed by single-crystal hard X-ray microscopy},
author = {Kuppan, Saravanan and Xu, Yahong and Liu, Yijin and Chen, Guoying},
abstractNote = {Understanding the reaction pathway and kinetics of solid-state phase transformation is critical in designing advanced electrode materials with better performance and stability. Despite the first-order phase transition with a large lattice mismatch between the involved phases, spinel LiMn1.5Ni0.5O4 is capable of fast rate even at large particle size, presenting an enigma yet to be understood. The present study uses advanced two-dimensional and three-dimensional nano-tomography on a series of well-formed LixMn1.5Ni0.5O4 (0 ≤ x ≤ 1) crystals to visualize the mesoscale phase distribution, as a function of Li content at the sub-particle level. Inhomogeneity along with the coexistence of Li-rich and Li-poor phases are broadly observed on partially delithiated crystals, providing direct evidence for a concurrent nucleation and growth process instead of a shrinking-core or a particle-by-particle process. As a result, superior kinetics of (100) facets at the vertices of truncated octahedral particles promote preferential delithiation, whereas the observation of strain-induced cracking suggests mechanical degradation in the material.},
doi = {10.1038/ncomms14309},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {Wed Feb 01 00:00:00 EST 2017},
month = {Wed Feb 01 00:00:00 EST 2017}
}

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Cited by: 6works
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