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Title: Assessing Long-Term Cycling Stability of Single-Crystal Versus Polycrystalline Nickel-Rich NCM in Pouch Cells with 6 mAh cm-2 Electrodes

Journal Article · · Small
ORCiD logo [1];  [2];  [3];  [4];  [5];  [1];  [1];  [1]; ORCiD logo [4];  [1];  [4];  [4];  [3]; ORCiD logo [2];  [1]
  1. Swiss Federal Laboratories for Materials Science and Technology (Empa), Dübendorf (Switzerland)
  2. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
  3. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  4. Central South University, Changsha (China)
  5. Yanshan University, Qinhuangdao (China)
+ Show Author Affiliations

Lithium-ion batteries based on single-crystal LiNi1-x-yCoxMnyO2 (NCM, 1-x-y ≥ 0.6) cathode materials are gaining increasing attention due to their improved structural stability resulting in superior cycle life compared to batteries based on polycrystalline NCM. However, an in-depth understanding of the less pronounced degradation mechanism of single-crystal NCM is still lacking. Here, a detailed postmortem study is presented, comparing pouch cells with single-crystal versus polycrystalline LiNi0.60Co0.20Mn0.20O2 (NCM622) cathodes after 1375 dis-/charge cycles against graphite anodes. The thickness of the cation-disordered layer forming in the near-surface region of the cathode particles does not differ significantly between single-crystal and polycrystalline particles, while cracking is pronounced for polycrystalline particles, but practically absent for single-crystal particles. Transition metal dissolution as quantified by time-of-flight mass spectrometry on the surface of the cycled graphite anode is much reduced for single-crystal NCM622. Similarly, CO2 gas evolution during the first two cycles as quantified by electrochemical mass spectrometry is much reduced for single-crystal NCM622. Benefitting from these advantages, graphite/single-crystal NMC622 pouch cells are demonstrated with a cathode areal capacity of 6 mAh cm-2 with an excellent capacity retention of 83% after 3000 cycles to 4.2 V, emphasizing the potential of single-crystalline NCM622 as cathode material for next-generation lithium-ion batteries.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
National Natural Science Foundation of China (NSFC); Swiss Competence Center for Energy Research (SCCER); USDOE Office of Science (SC), Biological and Environmental Research (BER)
Grant/Contract Number:
AC05-76RL01830
OSTI ID:
1987547
Report Number(s):
PNNL-SA-169057
Journal Information:
Small, Journal Name: Small Journal Issue: 14 Vol. 18; ISSN 1613-6810
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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36 MATERIALS SCIENCE
cracking
excellent capacity retention
gas evolution
single-crystal NCM
transition metal dissolution