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Title: In Situ Probing and Synthetic Control of Cationic Ordering in Ni-Rich Layered Oxide Cathodes

Ni-rich layered oxides (LiNi 1-xM xO 2; M=Co, Mn, …) are appealing alternatives to conventional LiCoO 2 as cathodes in Li-ion batteries for automobile and other large-scale applications due to their high theoretical capacity and low cost. However, preparing stoichiometric LiNi 1-xM xO 2 with ordered layer structure and high reversible capacity, has proven difficult due to Ni 2+/Li + cation mixing in octahedral sites. Herein, we report on in-situ studies of synthesis reactions and the associated structural ordering in preparing LiNiO 2 and the Co-substituted variant, LiNi 0.8Co 0.2O 2, thereby gaining insights into synthetic control of the structure and electrochemical properties of Ni-rich layered oxides. Results from this study indicate a direct transformation of the intermediate from the rock salt structure into hexagonal phase, and during the process, Co substitution facilities the nucleation of a Co-rich layered phase at low temperatures and subsequent growth and stabilization of solid solution Li(Ni, Co)O 2 upon heat treatment in a highly oxidation environment. Optimal conditions were identified from the in-situ studies and utilized in obtaining stoichiometric LiNi 0.8Co 0.2O 2 that exhibits high capacity of about 200 mAh/g with excellent retention. The findings shed light on designing Ni-rich layered oxide cathodesmore » with enhanced electrochemical properties through synthetic control of the structural ordering in the materials.« less
 [1] ;  [1] ;  [2] ;  [3] ;  [4] ;  [4] ;  [1] ;  [1] ;  [5] ;  [5] ;  [6] ;  [1] ;  [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Alfred Univ., NY (United States)
  4. Louisiana State Univ., Baton Rouge, LA (United States)
  5. Argonne National Lab. (ANL), Argonne, IL (United States)
  6. Peking Univ. Shenzhen Graduate School, Shenzhen (China)
Publication Date:
Report Number(s):
Journal ID: ISSN 1614-6832
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 7; Journal Issue: 3; Journal ID: ISSN 1614-6832
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
OSTI Identifier:
Alternate Identifier(s):
OSTI ID: 1401242