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Title: Design Principles for High-Capacity Mn-Based Cation-Disordered Rocksalt Cathodes

Journal Article · · Chem
 [1];  [1];  [1];  [2];  [1];  [3];  [4];  [5];  [1];  [6];  [1];  [3];  [7];  [1]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  2. Univ. of California, Berkeley, CA (United States); Univ. of California, Santa Barbara, CA (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  4. Univ. of California, Berkeley, CA (United States)
  5. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  6. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  7. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Univ. of California, Santa Barbara, CA (United States)
+ Show Author Affiliations

Mn-based Li-excess cation-disordered rocksalt (DRX) oxyfluorides are promising candidates for next-generation rechargeable battery cathodes owing to their large energy densities, the earth abundance, and low cost of Mn. In this work, we synthesized and electrochemically tested four representative compositions in the Li-Mn-O-F DRX chemical space with various Li and F content. Although all compositions achieve higher than 200 mAh g-1 initial capacity and good cyclability, we show that the Li-site distribution plays a more important role than the metal-redox capacity in determining the initial capacity, whereas the metal-redox capacity is more closely related to the cyclability of the materials. We apply these insights and generate a capacity map of the Li-Mn-O-F chemical space, LixMn2-xO2-yFy (1.167 ≤ x ≤ 1.333, 0 ≤ y ≤ 0.667), which predicts both accessible Li capacity and Mn-redox capacity. This map provides the design of compounds that balance high capacity with good cyclability.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Science Foundation (NSF)
Grant/Contract Number:
AC02-05CH11231; AC02-06CH11357
OSTI ID:
1594944
Alternate ID(s):
OSTI ID: 1702270; OSTI ID: 1609125; OSTI ID: 1763076; OSTI ID: 1651140
Journal Information:
Chem, Journal Name: Chem Journal Issue: 1 Vol. 6; ISSN 2451-9294
Publisher:
Cell Press, ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (2)

Cation-disordered rocksalt transition metal oxides and oxyfluorides for high energy lithium-ion cathodes journal January 2020
Effect of Fluorination on Lithium Transport and Short‐Range Order in Disordered‐Rocksalt‐Type Lithium‐Ion Battery Cathodes journal March 2020

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Related Subjects

25 ENERGY STORAGE
cation-disordered rocksalt cathodes
Li-excess Mn-based oxyfluorides
short-range order
density functional theory
Monte Carlo simulation
Li percolation
fluorination