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Title: Operando Lithium Dynamics in the Li-Rich Layered Oxide Cathode Material via Neutron Diffraction

Journal Article · · Advanced Energy Materials
 [1];  [2];  [3];  [1];  [1];  [1]
  1. Univ. of California, San Diego, CA (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Envia Systems, Newark, CA (United States)
+ Show Author Affiliations

Neutron diffraction under operando battery cycling is used to study the lithium and oxygen dynamics of high Li‐rich Li(Li x /3 Ni (3/8‐3 x /8) Co (1/4‐ x /4) Mn (3/8+7 x /24) O 2 ( x = 0.6, HLR) and low Li‐rich Li(Li x /3 Ni (1/3‐ x /3) Co (1/3‐ x /3) Mn (1/3+ x /3) O 2 ( x = 0.24, LLR) compounds that exhibit different degrees of oxygen activation at high voltage. The measured lattice parameter changes and oxygen position show largely contrasting changes for the two cathodes where the LLR exhibits larger movement of oxygen and lattice contractions in comparison to the HLR that maintains relatively constant lattice parameters and oxygen position during the high voltage plateau until the end of charge. Density functional theory calculations show the presence of oxygen vacancy during the high voltage plateau; changes in the lattice parameters and oxygen position are consistent with experimental observations. Lithium migration kinetics for the Li‐rich material is observed under operando conditions for the first time to reveal the rate of lithium extraction from the lithium layer, and transition metal layer is related to the different charge and discharge characteristics. At the beginning of charging, the lithium extraction predominately occurs within the lithium layer. Once the high voltage plateau is reached, the lithium extraction from the lithium layer slows down and extraction from the transition metal layer evolves at a faster rate.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1261356
Alternate ID(s):
OSTI ID: 1785873
Journal Information:
Advanced Energy Materials, Vol. 6, Issue 7; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 106 works
Citation information provided by
Web of Science

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Cited By (18)

Oxygen Release and Surface Degradation of Li- and Mn-Rich Layered Oxides in Variation of the Li 2 MnO 3 Content journal January 2018
Tuning Oxygen Redox Chemistry in Li‐Rich Mn‐Based Layered Oxide Cathodes by Modulating Cation Arrangement journal September 2019
Tracing Phase Transformation and Lattice Evolution in a TRIP Sheet Steel under High-Temperature Annealing by Real-Time In Situ Neutron Diffraction journal September 2018
Event-based processing of neutron scattering data at the Spallation Neutron Source journal May 2018
Nucleation of dislocations and their dynamics in layered oxide cathode materials during battery charging journal July 2018
In Situ Probing Multiple-Scale Structures of Energy Materials for Li-Ion Batteries journal May 2019
RHEGAL: Resistive heating gas enclosure loadframe for in situ neutron scattering journal September 2018
Controlled Atomic Solubility in Mn‐Rich Composite Material to Achieve Superior Electrochemical Performance for Li‐Ion Batteries journal December 2019
Surface modification of Li-rich manganese-based cathode materials by chemical etching journal January 2019
Understanding Rechargeable Battery Function Using In Operando Neutron Powder Diffraction journal September 2019
Native Vacancy Enhanced Oxygen Redox Reversibility and Structural Robustness journal December 2018
Feasibility of Cathode Surface Coating Technology for High-Energy Lithium-ion and Beyond-Lithium-ion Batteries journal March 2017
Review—Recent Advances and Remaining Challenges for Lithium Ion Battery Cathodes: II. Lithium-Rich, xLi journal January 2017
Direct observation of layered-to-spinel phase transformation in Li 2 MnO 3 and the spinel structure stabilised after the activation process journal January 2017
Interface Engineering for Garnet-Based Solid-State Lithium-Metal Batteries: Materials, Structures, and Characterization journal October 2018
Editors' Choice—State of Charge Dependent Resistance Build-Up in Li- and Mn-Rich Layered Oxides during Lithium Extraction and Insertion journal January 2019
A suite-level review of the neutron powder diffraction instruments at Oak Ridge National Laboratory journal September 2018
Nucleation of dislocations and their dynamics in layered oxide cathode materials during battery charging text January 2018

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