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

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms14309· OSTI ID:1347552
 [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)

© 2017 The Author(s). 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 1.5 Ni 0.5 O 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 Li x Mn 1.5 Ni 0.5 O 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. 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.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Grant/Contract Number:
AC02-76SF00515; AC02-05CH11231
OSTI ID:
1347552
Alternate ID(s):
OSTI ID: 1379708
Journal Information:
Nature Communications, Vol. 8; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 92 works
Citation information provided by
Web of Science

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Cited By (23)

Identifying the Origin and Contribution of Surface Storage in TiO 2 (B) Nanotube Electrode by In Situ Dynamic Valence State Monitoring journal July 2018
Review of Recent Development of In Situ/Operando Characterization Techniques for Lithium Battery Research journal May 2019
Quantification of Heterogeneous Degradation in Li‐Ion Batteries journal May 2019
Kathodenmaterialien für wiederaufladbare Lithiumbatterien journal November 2019
Advances in the Cathode Materials for Lithium Rechargeable Batteries journal February 2020
Ultra-Thin Coating and Three-Dimensional Electrode Structures to Boosted Thick Electrode Lithium-Ion Battery Performance journal November 2018
Application of Acrylic‐Rubber‐Based Latex Binder to High‐Voltage Spinel Electrodes of Lithium‐Ion Batteries journal August 2019
In Situ Probing Multiple-Scale Structures of Energy Materials for Li-Ion Batteries journal May 2019
Propagation topography of redox phase transformations in heterogeneous layered oxide cathode materials journal July 2018
Three-dimensional atomic-scale observation of structural evolution of cathode material in a working all-solid-state battery journal August 2018
Charge distribution guided by grain crystallographic orientations in polycrystalline battery materials journal January 2020
High-voltage positive electrode materials for lithium-ion batteries journal January 2017
Graphene aerogels for efficient energy storage and conversion journal January 2018
Chemomechanical behaviors of layered cathode materials in alkali metal ion batteries journal January 2018
Thermally driven mesoscale chemomechanical interplay in Li 0.5 Ni 0.6 Mn 0.2 Co 0.2 O 2 cathode materials journal January 2018
Thermally-driven mesopore formation and oxygen release in delithiated NCA cathode particles journal January 2019
Probing and quantifying cathode charge heterogeneity in Li ion batteries journal January 2019
Long-term chemothermal stability of delithiated NCA in polymer solid-state batteries journal January 2019
New molten salt synthesis of LiNi 0.5 Mn 1.5 O 4 cathode material journal July 2018
P2-type Na 2/3 Ni 1/3 Mn 2/3 O 2 Cathode Material with Excellent Rate and Cycling Performance for Sodium-Ion Batteries journal January 2019
Particle-Scale Path-Dependent Behavior of Li x Ni 0.5 Mn 1.5 O 4 Electrode in Li-Ion Batteries: Part I. Experimental Study journal January 2019
Long-Term Chemothermal Stability of Delithiated NCA in Polymer Solid-State Batteries text January 2019
Correlated X-Ray 3D Ptychography and Diffraction Microscopy Visualize Links between Morphology and Crystal Structure of Lithium-Rich Cathode Materials journal January 2019

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