DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Native lattice strain induced structural earthquake in sodium layered oxide cathodes

Journal Article · · Nature Communications

Abstract High-voltage operation is essential for the energy and power densities of battery cathode materials, but its stabilization remains a universal challenge. To date, the degradation origin has been mostly attributed to cycling-initiated structural deformation while the effect of native crystallographic defects induced during the sophisticated synthesis process has been significantly overlooked. Here, using in situ synchrotron X-ray probes and advanced transmission electron microscopy to probe the solid-state synthesis and charge/discharge process of sodium layered oxide cathodes, we reveal that quenching-induced native lattice strain plays an overwhelming role in the catastrophic capacity degradation of sodium layered cathodes, which runs counter to conventional perception—phase transition and cathode interfacial reactions. We observe that the spontaneous relaxation of native lattice strain is responsible for the structural earthquake (e.g., dislocation, stacking faults and fragmentation) of sodium layered cathodes during cycling, which is unexpectedly not regulated by the voltage window but is strongly coupled with charge/discharge temperature and rate. Our findings resolve the controversial understanding on the degradation origin of cathode materials and highlight the importance of eliminating intrinsic crystallographic defects to guarantee superior cycling stability at high voltages.

Sponsoring Organization:
USDOE
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1842355
Alternate ID(s):
OSTI ID: 1879851
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 13; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United Kingdom
Language:
English

References (64)

Tailoring grain boundary structures and chemistry of Ni-rich layered cathodes for enhanced cycle stability of lithium-ion batteries journal June 2018
High‐Voltage‐Driven Surface Structuring and Electrochemical Stabilization of Ni‐Rich Layered Cathode Materials for Li Rechargeable Batteries journal May 2020
Direct Observation of Defect‐Aided Structural Evolution in a Nickel‐Rich Layered Cathode journal September 2020
Ti-Substituted NaNi 0.5 Mn 0.5- x Ti x O 2 Cathodes with Reversible O3−P3 Phase Transition for High-Performance Sodium-Ion Batteries journal March 2017
Surface-to-Bulk Redox Coupling through Thermally Driven Li Redistribution in Li- and Mn-Rich Layered Cathode Materials journal July 2019
Realizing Complete Solid‐Solution Reaction in High Sodium Content P2‐Type Cathode for High‐Performance Sodium‐Ion Batteries journal July 2020
Understanding the formation of antiphase boundaries in layered oxide cathode materials and their evolution upon electrochemical cycling journal December 2021
Charging Reactions Promoted by Geometrically Necessary Dislocations in Battery Materials Revealed by In Situ Single‐Particle Synchrotron Measurements journal August 2020
Building ultraconformal protective layers on both secondary and primary particles of layered lithium transition metal oxide cathodes journal May 2019
New Insights into the Performance Degradation of Fe-Based Layered Oxides in Sodium-Ion Batteries: Instability of Fe 3+ /Fe 4+ Redox in α-NaFeO 2 journal September 2015
Superstructure control of first-cycle voltage hysteresis in oxygen-redox cathodes journal December 2019
Nickel-Rich Layered Lithium Transition-Metal Oxide for High-Energy Lithium-Ion Batteries journal March 2015
Synthesis of full concentration gradient cathode studied by high energy X-ray diffraction journal January 2016
Trace doping of multiple elements enables stable battery cycling of LiCoO2 at 4.6 V journal June 2019
Atomistic mechanism of cracking degradation at twin boundary of LiCoO2 journal December 2020
Temperature Dependence of Oxygen Release from LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) Cathode Materials for Li-Ion Batteries journal January 2018
Challenges for Rechargeable Li Batteries journal February 2010
Degradation of High‐Nickel‐Layered Oxide Cathodes from Surface to Bulk: A Comprehensive Structural, Chemical, and Electrical Analysis journal August 2020
Challenges in Developing Electrodes, Electrolytes, and Diagnostics Tools to Understand and Advance Sodium-Ion Batteries journal February 2018
High-nickel layered oxide cathodes for lithium-based automotive batteries journal January 2020
Study on the Reversible Electrode Reaction of Na 1– x Ni 0.5 Mn 0.5 O 2 for a Rechargeable Sodium-Ion Battery journal May 2012
Progress in High-Voltage Cathode Materials for Rechargeable Sodium-Ion Batteries journal September 2017
Structural Evolution and Redox Processes Involved in the Electrochemical Cycling of P2–Na 0.67 [Mn 0.66 Fe 0.20 Cu 0.14 ]O 2 journal July 2017
Structural origin of the high-voltage instability of lithium cobalt oxide journal February 2021
Singlet oxygen evolution from layered transition metal oxide cathode materials and its implications for lithium-ion batteries journal October 2018
The effect of cooling process on the structure and charge/discharge capacities of Li-rich solid-solution layered oxide cathode materials for the Li-ion battery journal January 2021
Rock-Salt Growth-Induced (003) Cracking in a Layered Positive Electrode for Li-Ion Batteries journal October 2017
The interplay between thermodynamics and kinetics in the solid-state synthesis of layered oxides journal May 2020
Lithium-Doping Stabilized High-Performance P2–Na 0.66 Li 0.18 Fe 0.12 Mn 0.7 O 2 Cathode for Sodium Ion Batteries journal April 2019
Cooling Induced Surface Reconstruction during Synthesis of High‐Ni Layered Oxides journal October 2019
Stable cycling of high-voltage lithium metal batteries in ether electrolytes journal July 2018
Challenges and Strategies to Advance High‐Energy Nickel‐Rich Layered Lithium Transition Metal Oxide Cathodes for Harsh Operation journal September 2020
Nature of the “Z”-phase in layered Na-ion battery cathodes journal January 2019
The effect of morphology on the stability of retained austenite in a quenched and partitioned steel journal March 2013
How Synthetic Quench Rate and Composition Affect the Performance of Lithium Nickel Manganese Oxide Cathode Materials journal December 2020
Nonaqueous Sodium‐Ion Full Cells: Status, Strategies, and Prospects journal March 2019
Research Development on Sodium-Ion Batteries journal October 2014
Kinetic Study of Parasitic Reactions in Lithium-Ion Batteries: A Case Study on LiNi 0.6 Mn 0.2 Co 0.2 O 2 journal January 2016
Structure of the high voltage phase of layered P2-Na 2/3−z [Mn 1/2 Fe 1/2 ]O 2 and the positive effect of Ni substitution on its stability journal January 2015
Revisiting Primary Particles in Layered Lithium Transition‐Metal Oxides and Their Impact on Structural Degradation journal January 2019
Insights into the Improved High-Voltage Performance of Li-Incorporated Layered Oxide Cathodes for Sodium-Ion Batteries journal September 2018
Deciphering the Cathode-Electrolyte Interfacial Chemistry in Sodium Layered Cathode Materials journal October 2018
Chemical versus Electrochemical Electrolyte Oxidation on NMC111, NMC622, NMC811, LNMO, and Conductive Carbon journal September 2017
High‐Voltage Charging‐Induced Strain, Heterogeneity, and Micro‐Cracks in Secondary Particles of a Nickel‐Rich Layered Cathode Material journal March 2019
Multiscale Computational Model for Particle Size Evolution during Coprecipitation of Li-Ion Battery Cathode Precursors journal March 2019
Synthetic Control of Kinetic Reaction Pathway and Cationic Ordering in High-Ni Layered Oxide Cathodes journal August 2017
Insights into the structural effects of layered cathode materials for high voltage sodium-ion batteries journal January 2017
Approaching the capacity limit of lithium cobalt oxide in lithium ion batteries via lanthanum and aluminium doping journal June 2018
Bulk fatigue induced by surface reconstruction in layered Ni-rich cathodes for Li-ion batteries journal August 2020
Understanding the Capacity Fading Mechanisms of O3‐Type Na[Ni 0.5 Mn 0.5 ]O 2 Cathode for Sodium‐Ion Batteries journal July 2020
Controlling Surface Phase Transition and Chemical Reactivity of O3-Layered Metal Oxide Cathodes for High-Performance Na-Ion Batteries journal April 2020
Unlocking the Potential of Cation-Disordered Oxides for Rechargeable Lithium Batteries journal January 2014
Suppressing the P2-O2 Phase Transition of Na 0.67 Mn 0.67 Ni 0.33 O 2 by Magnesium Substitution for Improved Sodium-Ion Batteries journal May 2016
The Role of Intragranular Nanopores in Capacity Fade of Nickel-Rich Layered Li(Ni 1– xy Co x Mn y )O 2 Cathode Materials journal August 2019
Singlet Oxygen Reactivity with Carbonate Solvents Used for Li-Ion Battery Electrolytes journal October 2018
Phase transition induced cracking plaguing layered cathode for sodium-ion battery journal December 2018
Constructing Safe and Durable High‐Voltage P2 Layered Cathodes for Sodium Ion Batteries Enabled by Molecular Layer Deposition of Alucone journal March 2020
Phase Behavior during Electrochemical Cycling of Ni‐Rich Cathode Materials for Li‐Ion Batteries journal December 2020
Reactive boride infusion stabilizes Ni-rich cathodes for lithium-ion batteries journal March 2021
Synthesis, Structure, and Electrochemical Properties of the Layered Sodium Insertion Cathode Material: NaNi 1 / 3 Mn 1 / 3 Co 1 / 3 O 2 journal April 2012
High Voltage Mg-Doped Na 0.67 Ni 0.3– x Mg x Mn 0.7 O 2 ( x = 0.05, 0.1) Na-Ion Cathodes with Enhanced Stability and Rate Capability journal July 2016
Cyclic deterioration and its improvement for Li-rich layered cathode material Li[Ni0.17Li0.2Co0.07Mn0.56]O2 journal January 2010
Oxidatively stable fluorinated sulfone electrolytes for high voltage high energy lithium-ion batteries journal January 2017
Insights into Li/Ni ordering and surface reconstruction during synthesis of Ni-rich layered oxides journal January 2019