Tailoring the Redox Reactions for High-Capacity Cycling of Cation-Disordered Rocksalt Cathodes

Yue, Yuan; Li, Ning; Ha, Yang; Crafton, Matthew J.; McCloskey, Bryan D.; Yang, Wanli; Tong, Wei

doi:10.1002/adfm.202008696

Tailoring the Redox Reactions for High-Capacity Cycling of Cation-Disordered Rocksalt Cathodes

Journal Article · Wed Jan 27 00:00:00 EST 2021 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.202008696· OSTI ID:1845100

Yue, Yuan ^[1]; Li, Ning ^[1]; Ha, Yang ^[1]; Crafton, Matthew J. ^[2]; McCloskey, Bryan D. ^[3]; Yang, Wanli ^[1]; ^[1]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)

Cation-disordered rocksalts (DRXs) have emerged as a new class of high-capacity Li-ion cathode materials. One unique advantage of the DRX chemistry is the structural flexibility that substantially lessens the elemental constraints in the crystal lattice, such as Li content, choice of transition metal redox center paired with appropriate d⁰ metal, and incorporation of F anion, which allows optimization of the key redox reactions. Herein, a series of the DRX oxyfluorides based on the Mn redox have been designed and synthesized. By tailoring the stoichiometry of the DRX compositions, high-capacity cycling by promoting the cationic Mn²⁺/Mn⁴⁺ redox reactions while suppressing those from anionic O is successfully demonstrated. A highly fluorinated DRX compound, Li_1.2Mn_0.625Nb_0.175O_1.325F_0.675 (M_0.625F_0.675), delivers a capacity of ≈170 mAh g^-1 at C/3 for 100 cycles. Furthermore, this work showcases the concept of balancing the cationic and anionic redox reactions in the DRX cathodes for improved electrochemical performance through the rational composition design.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515

OSTI ID:: 1845100

Alternate ID(s):: OSTI ID: 1785777
OSTI ID: 23116412

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 14 Vol. 31; ISSN 1616-301X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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