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Title: Ternary metal fluorides as high-energy cathodes with low cycling hysteresis

In this study, transition metal fluorides are an appealing alternative to conventional intercalation compounds for use as cathodes in next-generation lithium batteries due to their extremely high capacity (3–4 times greater than the current state-of-the-art). However, issues related to reversibility, energy efficiency and kinetics prevent their practical application. Here we report on the synthesis, structural and electrochemical properties of ternary metal fluorides (M1yM21-yFx: M1, M2 = Fe, Cu), which may overcome these issues. By substituting Cu into the Fe lattice, forming the solid–solution CuyFe1-yF2, reversible Cu and Fe redox reactions are achieved with surprisingly small hysteresis (<150 mV). This finding indicates that cation substitution may provide a new avenue for tailoring key electrochemical properties of conversion electrodes. In conclusion, although the reversible capacity of Cu conversion fades rapidly, likely due to Cu+ dissolution, the low hysteresis and high energy suggest that a Cu-based fluoride cathode remains an intriguing candidate for rechargeable lithium batteries.
Authors:
 [1] ;  [1] ;  [2] ;  [3] ;  [1] ;  [4] ;  [5] ;  [5] ;  [6]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Sustainable Energy Technologies Dept.
  2. Seoul National Univ. (Korea, Republic of). Dept. of Materials Science and Engineering; Seoul National Univ. (Korea, Republic of). Center for Nanoparticle Research
  3. Seoul National Univ. (Korea, Republic of). Dept. of Materials Science and Engineering; Seoul National Univ. (Korea, Republic of). Center for Nanoparticle Research
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  5. HRL Laboratories, LLC, Malibu, CA (United States)
  6. Brookhaven National Lab. (BNL), Upton, NY (United States). Sustainable Energy Technologies Dept.; HRL Laboratories, LLC, Malibu, CA (United States)
Publication Date:
OSTI Identifier:
1229444
Report Number(s):
BNL--111520-2015-JA
Journal ID: ISSN 2041-1723
Grant/Contract Number:
SC0012704; SC0001060; SC0001294; AC02- 98CH10886
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
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
Language:
English
Subject:
36 MATERIALS SCIENCE