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Title: Disintegration of Meatball Electrodes for LiNi x Mn y Co z O 2 Cathode Materials

Mechanical degradation of Li-ion batteries caused by the repetitive swelling and shrinking of electrodes upon electrochemical cycles is now well recognized. Structural disintegration of the state-of-art cathode materials of a hierarchical structure is relatively less studied. In this paper, we track the microstructural evolution of different marked regimes in LiNi x Mn y Co z O 2 (NMC) electrodes after lithiation cycles. Decohesion of primary particles constitutes the major mechanical degradation in the NMC materials, which results in the loss of connectivity of the conductive network and impedance increase. We find that the structural disintegration is largely dependent on the charging rate – slow charging causes more damage, and is relatively insensitive to the cyclic voltage window. We use finite element modeling to study the evolution of Li concentration and stresses in a NMC secondary particle and employ the cohesive zone model to simulate the interfacial fracture between primary particles. Finally, we reveal that microcracks accumulate and propagate during the cyclic lithiation and delithiation at a slow charging rate.
 [1] ;  [1] ;  [1] ;  [2] ;  [1]
  1. Purdue Univ., West Lafayette, IN (United States). School of Mechanical Engineering
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Energy and Transportation Science Division
Publication Date:
Grant/Contract Number:
AC05-00OR22725; CBET-1603866
Accepted Manuscript
Journal Name:
Experimental Mechanics
Additional Journal Information:
Journal Volume: 58; Journal Issue: 4; Journal ID: ISSN 0014-4851
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Purdue Univ., West Lafayette, IN (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Science Foundation (NSF); Office of Naval Research (ONR) (United States)
Country of Publication:
United States
25 ENERGY STORAGE; 42 ENGINEERING; fracture; NMC; stresses; primary particles; Li-ion batteries
OSTI Identifier: