Enhanced Electrochemical Performance of Disordered Rocksalt Cathodes in a Localized High‐Concentration Electrolyte

Ahmed, Ridwan A.; Koirala, Krishna P.; Lee, Gi‐Hyeok; Li, Tianyu; Zhao, Qian; Fu, Yanbao; Zhong, Lirong; Daddona, Joseph D.; Zuba, Mateusz; Siu, Carrie; Kahvecioglu, Ozgenur; Battaglia, Vincent S.; Clément, Raphaële J.; Yang, Wanli; Wang, Chongmin; Xu, Wu

doi:10.1002/aenm.202400722

Enhanced Electrochemical Performance of Disordered Rocksalt Cathodes in a Localized High‐Concentration Electrolyte

Journal Article · Tue May 14 00:00:00 EDT 2024 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202400722· OSTI ID:2350733

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Energy and Environment Directorate Pacific Northwest National Laboratory Richland WA 99354 USA
Physical and Computational Sciences Directorate Pacific Northwest National Laboratory Richland WA 99354 USA
Advanced Light Source Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
Materials Department and Materials Research Laboratory University of California Santa Barbara CA 93106 USA
Environmental Molecular Sciences Laboratory Pacific Northwest National Laboratory Richland WA 99354 USA
Energy Storage and Distributed Resources Division Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
National Security Directorate Pacific Northwest National Laboratory Richland WA 99354 USA
Applied Materials Division Argonne National Laboratory Lemont IL 60439 USA

Abstract

Lithium (Li)‐rich transition metal oxide cathodes with a cation disordered rock salt structure (DRX) are increasingly gaining popularity for advanced Li batteries as they offer high capacity and cost benefits over the commonly used layered Li transition metal oxide cathodes. However, the performance of DRX cathodes and their applications are limited by severe side reactions between the cathode and the state‐of‐the‐art carbonate‐based electrolytes at high voltage of 4.8 V, transition metal dissolution, and structural instability of the cathode particles. In this work, an advanced localized high‐concentration electrolyte (LHCE) is developed to form a stable cathode‐electrolyte interphase and mitigate structural instability of the Li _1.13 Mn _0.66 Ti _0.21 O ₂ (LMTO) DRX during electrochemical cycling. Li||LMTO half cells with the LHCE demonstrate increased capacity, cycling stability, and superior rate capability compared with cells containing a conventional carbonate electrolyte. For instance, the Li||LMTO cells cycled in LHCE show a higher initial capacity of 205.2 mAh g ⁻¹ and a better capacity retention of 72.5% after 200 cycles at a current density of 20 mA g ⁻¹ than those with the conventional electrolyte (initial capacity of 187.7 mAh g ⁻¹ and capacity retention of 19.9%). This work paves the way to the development of practical DRX cathode‐based high‐energy Li batteries.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC02-05CH11231; AC05-76RL01830

OSTI ID:: 2350733

Alternate ID(s):: OSTI ID: 2350734
OSTI ID: 2405904
OSTI ID: 2406222

Report Number(s):: PNNL-SA--194465; 2400722

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials; ISSN 1614-6832

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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25 ENERGY STORAGE
cathode-electrolyte interphase
disordered rock salt cathode
electrolyte
lithium metal
structural integrity

Enhanced Electrochemical Performance of Disordered Rocksalt Cathodes in a Localized High‐Concentration Electrolyte

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