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Title: Intergranular Cracking as a Major Cause of Long-Term Capacity Fading of Layered Cathodes

Capacity fading has limited commercial layered Li-ion battery electrodes to <70% of their theoretical capacity. Higher capacities can be achieved initially by charging to higher voltages, however, these gains are quickly eroded by a faster fade in capacity. In-creasing lifetimes and reversible capacity is contingent on identifying the origin of this capacity fade to inform electrode design and synthesis. We must understand how the battery reactions change following capacity loss after long-term cycling. Using operando X-ray diffraction, we followed the reaction of a LiNi 0.8Co 0.15Al 0.05O 2 (NCA) electrode after months of charge-discharge cycles. Furthermore, the heterogeneous reaction kinetics observed during extended cycles quantitatively explain the capacity loss, which is ultimately attributed to inter-granular fracturing that degrades the connectivity of sub-surface grains within the polycrystalline NCA aggregate.
ORCiD logo [1] ;  [2] ;  [3] ;  [4] ; ORCiD logo [3] ; ORCiD logo [2] ;  [1] ;  [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Univ. of Illinois, Chicago, IL (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Univ. of Illinois, Chicago, IL (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Report Number(s):
Journal ID: ISSN 1530-6984; 132046
Grant/Contract Number:
AC02-06CH11357; SC0012704
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 17; Journal Issue: 6; Journal ID: ISSN 1530-6984
American Chemical Society
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States); Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 25 ENERGY STORAGE; batteries; Capacity fading; intergranular cracking; operando X-ray diffraction; 77 NANOSCIENCE AND NANOTECHNOLOGY; inter-granular cracking; Center for Functional Nanomaterials
OSTI Identifier:
Alternate Identifier(s):
OSTI ID: 1389236