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

Title: Locking oxygen in lattice: A quantifiable comparison of gas generation in polycrystalline and single crystal Ni-rich cathodes

Journal Article · · Energy Storage Materials

High-energy Ni-rich NMC (LiNixMnyCo1-x-yO2, x ≥ 0.6) is a very promising cathode material in Li-ion batteries but the gas generation during cycling is a significant safety concern and becomes the major roadblock of the large-scale commercialization of Ni-rich NMC cathode materials. Micron-sized single crystal Ni-rich NMC has a potential to address the common issues that polycrystals have. However, it is unknown if gassing issue will be mitigated or even eliminated by using single crystals, not mentioning a quantifiable understanding of gas generation from single crystals and polycrystals. This work takes LiNi0.76Mn0.14Co0.1O2 (NMC76) as a model material to study the mechanism of gas generation from single crystal and polycrystalline NMC by using both coin cells and pouch cells, which provides different conclusions on the generated gases, highlighting the importance of using relevant testing conditions for fundamental diagnostic study on battery materials. Further, the information from single crystal NMC also provides critical insights from material perspective to enhance the safety attributes of Ni-rich NMC cathodes.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Grant/Contract Number:
AC05-76RL01830; LC-000L053; 76RL01830; AC05?; AC05–76RL01830
OSTI ID:
1963902
Alternate ID(s):
OSTI ID: 1846466
Report Number(s):
PNNL-SA-163635
Journal Information:
Energy Storage Materials, Vol. 47; ISSN 2405-8297
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (38)

Bulk fatigue induced by surface reconstruction in layered Ni-rich cathodes for Li-ion batteries journal August 2020
Effect of electrolyte composition on rock salt surface degradation in NMC cathodes during high-voltage potentiostatic holds journal January 2019
In Situ Investigation of the Electrochemical Reduction of Carbonate Electrolyte Solutions at Graphite Electrodes journal January 1998
A dual-functional gel-polymer electrolyte for lithium ion batteries with superior rate and safety performances journal January 2017
Increased Stability Toward Oxygen Reduction Products for Lithium-Air Batteries with Oligoether-Functionalized Silane Electrolytes journal December 2011
Tailoring grain boundary structures and chemistry of Ni-rich layered cathodes for enhanced cycle stability of lithium-ion batteries journal June 2018
Singlet oxygen evolution from layered transition metal oxide cathode materials and its implications for lithium-ion batteries journal October 2018
Gassing in Li4Ti5O12-based batteries and its remedy journal December 2012
Reactive boride infusion stabilizes Ni-rich cathodes for lithium-ion batteries journal March 2021
Origin of Carbon Dioxide Evolved during Cycling of Nickel-Rich Layered NCM Cathodes journal October 2018
Combinations of Ethylene Sulfite (ES) and Vinylene Carbonate (VC) as Electrolyte Additives in Li(Ni 1/3 Mn 1/3 Co 1/3 )O 2 /Graphite Pouch Cells journal January 2014
Beyond Doping and Coating: Prospective Strategies for Stable High-Capacity Layered Ni-Rich Cathodes journal March 2020
Suppressed oxygen extraction and degradation of LiNi x Mn y Co z O2 cathodes at high charge cut-off voltages journal September 2017
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
Origin of H 2 Evolution in LIBs: H 2 O Reduction vs. Electrolyte Oxidation journal January 2016
Achieving highly reproducible results in graphite-based Li-ion full coin cells journal May 2021
Effect of calcination temperature on the electrochemical properties of nickel-rich LiNi0.76Mn0.14Co0.10O2 cathodes for lithium-ion batteries journal July 2018
Twin Problems of Interfacial Carbonate Formation in Nonaqueous Li–O 2 Batteries journal March 2012
Unraveling the Cationic and Anionic Redox Reactions in a Conventional Layered Oxide Cathode journal October 2019
Low pressure carbon dioxide solubility in lithium-ion batteries based electrolytes as a function of temperature. Measurement and prediction journal June 2013
Reversible planar gliding and microcracking in a single-crystalline Ni-rich cathode journal December 2020
Online Continuous Flow Differential Electrochemical Mass Spectrometry with a Realistic Battery Setup for High-Precision, Long-Term Cycling Tests journal May 2015
Chemical versus Electrochemical Electrolyte Oxidation on NMC111, NMC622, NMC811, LNMO, and Conductive Carbon journal September 2017
Electrochemical Study of Functional Additives for Li-Ion Batteries journal January 2020
Investigation of the rechargeability of Li–O2 batteries in non-aqueous electrolyte journal July 2011
Combining In Situ Synchrotron X-Ray Diffraction and Absorption Techniques with Transmission Electron Microscopy to Study the Origin of Thermal Instability in Overcharged Cathode Materials for Lithium-Ion Batteries journal June 2012
Origin, Nature, and the Dynamic Behavior of Nanoscale Vacancy Clusters in Ni-Rich Layered Oxide Cathodes journal April 2021
Building ultraconformal protective layers on both secondary and primary particles of layered lithium transition metal oxide cathodes journal May 2019
Residual Lithium Carbonate Predominantly Accounts for First Cycle CO 2 and CO Outgassing of Li-Stoichiometric and Li-Rich Layered Transition-Metal Oxides journal November 2017
Oxygen, hydrogen, ethylene and CO2 development in lithium-ion batteries journal December 2007
Capacity Fading of Ni-Rich Li[Ni x Co y Mn 1– xy ]O 2 (0.6 ≤ x ≤ 0.95) Cathodes for High-Energy-Density Lithium-Ion Batteries: Bulk or Surface Degradation? journal January 2018
Impact of Microcrack Generation and Surface Degradation on a Nickel-Rich Layered Li[Ni 0.9 Co 0.05 Mn 0.05 ]O 2 Cathode for Lithium-Ion Batteries journal September 2017
Mesoscale-architecture-based crack evolution dictating cycling stability of advanced lithium ion batteries journal January 2021
Oxygen Release and Its Effect on the Cycling Stability of LiNi x Mn y Co z O 2 (NMC) Cathode Materials for Li-Ion Batteries journal January 2017
Structural Origin of Overcharge-Induced Thermal Instability of Ni-Containing Layered-Cathodes for High-Energy-Density Lithium Batteries journal September 2011
Comparison of the structural and electrochemical properties of layered Li[NixCoyMnz]O2 (x = 1/3, 0.5, 0.6, 0.7, 0.8 and 0.85) cathode material for lithium-ion batteries journal July 2013
Hierarchical Porous LiNi1/3Co1/3Mn1/3O2 Nano-/Micro Spherical Cathode Material: Minimized Cation Mixing and Improved Li+ Mobility for Enhanced Electrochemical Performance journal May 2016
Boosting Reaction Homogeneity in High‐Energy Lithium‐Ion Battery Cathode Materials journal August 2020

Figures / Tables (4)