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This content will become publicly available on February 7, 2019

Title: Identifying the chemical and structural irreversibility in LiNi 0.8 Co 0.15 Al 0.05 O 2 – a model compound for classical layered intercalation

In this work, we extracted 95% of the electrochemically available Li from LiNi 0.8Co 0.15Al 0.05O 2 (NCA) by galvanostatically charging the NCA/MCMB full cell to 4.7 V. Joint powder X-ray and neutron diffraction (XRD & ND) studies were undertaken for NCA at highly charged states at the first cycle, and discharged states at different cycles. The results indicate that the bulk structure of NCA maintains the O3 structure up to the extraction of 0.90 Li per formula unit. In addition, we found that the transition metal layer becomes more disordered along the c-axis than along the a- and b-axes upon charging. This anisotropic disorder starts to develop no later than 4.3 V on charge and continues to grow until the end of charge. As Li is re-inserted during discharge, the structure that resembles the pristine NCA is recovered. The irreversible loss of Li and the migration of Ni to the Li layer have been quantified by the joint XRD and ND refinement and the results were further verified by solid state 7Li NMR and magnetic measurements. Thus, our work clearly demonstrates that the NCA bulk retains a robust, single phase O3 structure throughout the wide delithiation range (up tomore » 0.9 Li per formula unit of NCA) and is suitable for higher energy density usage with proper modifications.« less
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [2] ; ORCiD logo [3] ;  [1] ;  [5] ;  [5] ;  [1] ;  [2] ;  [2] ; ORCiD logo [6] ; ORCiD logo [6] ; ORCiD logo [6] ;  [2] ; ORCiD logo [2] ;  [4] ;  [3] ; ORCiD logo [1]
  1. Univ. of California, San Diego, CA (United States). Dept. of NanoEngineering
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS). X-ray Science Division
  3. Univ. of Cambridge (United Kingdom). Dept. of Chemistry
  4. State Univ. of New York (SUNY), Binghamton, NY (United States). Inst. for Materials Research
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division
  6. Chinese Academy of Sciences (CAS) Ningbo Inst. of Materials Technology and Engineering (NIMTE), Ningbo (China). Advanced Li-ion Battery Engineering Lab. and Key Lab. of Graphene Technologies and Applications
Publication Date:
Grant/Contract Number:
AC05-00OR22725; SC0012583; AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 6; Journal Issue: 9; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS); Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE; 25 ENERGY STORAGE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1427639