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Title: Chemomechanical interplay of layered cathode materials undergoing fast charging in lithium batteries

Journal Article · · Nano Energy
 [1];  [2];  [2];  [3];  [4];  [5];  [4];  [6]; ORCiD logo [3]; ORCiD logo [2];  [4]
  1. Nanjing University of Science and Technology, Jiangsu (China); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
  3. CAS, Beijing (China)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  5. Nanjing University of Science and Technology, Jiangsu (China)
  6. Purdue Univ., West Lafayette, IN (United States)

Morphological defects contribute to chronic and acute failures of batteries. The development of these morphological defects entails the multiscale chemo-mechanical coupling associated with internal mechanical stress. The mechanical stress, caused by anisotropic structural, chemical and state of charge (SOC) heterogeneities, is released through crack formation, undermining the continuous diffusion pathways of electrons and ions and creating fresh surfaces for electrode–electrolyte side reactions. The understanding of chemomechanical interplay has remained at the descriptive level, thus, the quantification or model to fingerprint these processes is highly desired. Herein, we systematically investigate the mesoscale morphological defects within LiNi0.6Mn0.2Co0.2O2 secondary particles that have gone through fast-charging conditions. With the advanced synchrotron X-ray tomography, we nondestructively pierce the internal volume of secondary particles and quantify the morphological outcomes of the crack formation, such as porosity and internal surface area. We then develop a numerical model to predict the crack-induced diffusion deterrent of electrons and lithium ions. The mismatch between the local ionic and electronic conductivity can lead to highly heterogeneous SOC distribution in secondary particles, which exponentially deteriorates as the current density increases. In conclusion, our incisive investigation of chemomechanical interplay and fast-charging can inform a knowledge base to accelerate the discovery of advanced materials that are resilient against chemomechanical failures.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
Grant/Contract Number:
2017YFB0102004; 51822211; DMR-1832613; DMR-1832707; AC02-76SF00515
OSTI ID:
1490861
Alternate ID(s):
OSTI ID: 1637160
Journal Information:
Nano Energy, Vol. 53, Issue C; ISSN 2211-2855
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 141 works
Citation information provided by
Web of Science

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Cited By (8)

Quantification of Heterogeneous Degradation in Li‐Ion Batteries journal May 2019
Probing and quantifying cathode charge heterogeneity in Li ion batteries journal January 2019
Chemomechanical behaviors of layered cathode materials in alkali metal ion batteries journal January 2018
Charge distribution guided by grain crystallographic orientations in polycrystalline battery materials journal January 2020
Enhanced High‐Temperature Electrochemical Performance of Layered Nickel‐Rich Cathodes for Lithium‐Ion Batteries after LiF Surface Modification journal October 2019
Real-time monitoring of stress development during electrochemical cycling of electrode materials for Li-ion batteries: overview and perspectives journal January 2019
Challenges and opportunities towards fast-charging battery materials journal June 2019
Charge distribution guided by grain crystallographic orientations in polycrystalline battery materials journal January 2020

Figures / Tables (6)