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Title: Atomic Insight into the Layered/Spinel Phase Transformation in Charged LiNi0.80Co0.15Al0.05O2 Cathode Particles

Journal Article · · Journal of Physical Chemistry. C
ORCiD logo [1];  [2];  [3];  [3];  [4]; ORCiD logo [1]
  1. State Univ. of New York, Binghamton, NY (United States). Materials Science and Engineering Program, and Mechanical Dept.; State Univ. of New York, Binghamton, NY (United States). NorthEast Center for Chemical Energy Storage
  2. State Univ. of New York, Binghamton, NY (United States). NorthEast Center for Chemical Energy Storage; Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
  3. State Univ. of New York, Binghamton, NY (United States). NorthEast Center for Chemical Energy Storage
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
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Layered LiNi0.80Co0.15Al0.05O2 (NCA) holds great promise as a potential cathode material for high energy density lithium ion batteries. However, its high capacity is heavily dependent on the stability of its layered structure, which suffers from a severe structure degradation resulting from a not fully understood layered → spinel phase transformation. Using high-resolution transmission electron microscopy and electron diffraction, we probe the atomic structure evolution induced by the layered → spinel phase transformation in the NCA cathode. We show that the phase transformation results in the development of a particle structure with the formation of complete spinel, spinel domains, and intermediate spinel from the surface to the subsurface region. The lattice planes of the complete and intermediate spinel phases are highly interwoven in the subsurface region. The layered → spinel transformation occurs via the migration of transition metal (TM) atoms from the TM layer into the lithium layer. Incomplete migration leads to the formation of the intermediate spinel phase, which is featured by tetrahedral occupancy of TM cations in the lithium layer. Finally, the crystallographic structure of the intermediate spinel is discussed and verified by the simulation of electron diffraction patterns.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Northeastern Center for Chemical Energy Storage (NECCES)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0001294; SC0012583; AC02-98CH10886
OSTI ID:
1388616
Journal Information:
Journal of Physical Chemistry. C, Vol. 121, Issue 3; Related Information: NECCES partners with Stony Brook University (lead); Argonne National Laboratory; Binghamton University; Brookhaven National University; University of California, San Diego; University of Cambridge, UK; Lawrence Berkeley National Laboratory; Massachusetts Institute of Technology; University of Michigan; Rutgers University; ISSN 1932-7447
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 46 works
Citation information provided by
Web of Science

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Cited By (6)

Boron-doped single crystal LiNi0.6Mn0.2Co0.2O2 with improved electrochemical performance for lithium-ion batteries journal July 2019
Influence of Ni/Mn distributions on the structure and electrochemical properties of Ni-rich cathode materials journal January 2018
Enhanced rate performance and cycle stability of LiNi0.8Co0.15Al0.05O2 via Rb doping journal October 2018
Using in situ and operando methods to characterize phase changes in charged lithium nickel cobalt aluminum oxide cathode materials journal January 2020
Long-term chemothermal stability of delithiated NCA in polymer solid-state batteries journal January 2019
Long-Term Chemothermal Stability of Delithiated NCA in Polymer Solid-State Batteries text January 2019

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
36 MATERIALS SCIENCE
energy storage (including batteries and capacitors)
defects
charge transport
materials and chemistry by design
synthesis (novel materials)