Mitigating Interfacial Mismatch between Lithium Metal and Garnet-Type Solid Electrolyte by Depositing Metal Nitride Lithiophilic Interlayer

Baniya, Abiral; Gurung, Ashim; Pokharel, Jyotshna; Chen, Ke; Pathak, Rajesh; Lamsal, Buddhi Sagar; Ghimire, Nabin; Bobba, Raja Sekhar; Rahman, Sheikh Ifatur; Mabrouk, Sally; Smirnova, Alevtina L.; Xu, Kang; Qiao, Quinn

doi:10.1021/acsaem.1c03157

Mitigating Interfacial Mismatch between Lithium Metal and Garnet-Type Solid Electrolyte by Depositing Metal Nitride Lithiophilic Interlayer

Journal Article · Fri Jan 07 00:00:00 EST 2022 · ACS Applied Energy Materials

DOI:https://doi.org/10.1021/acsaem.1c03157· OSTI ID:2469980

^[1]; Gurung, Ashim ^[2]; Pokharel, Jyotshna ^[2]; ^[2]; Pathak, Rajesh ^[3]; Lamsal, Buddhi Sagar ^[2]; ^[2]; Bobba, Raja Sekhar ^[1]; ^[2]; Mabrouk, Sally ^[1]; ^[4]; Xu, Kang ^[5]; ^[1]

Syracuse Univ., NY (United States)
South Dakota State Univ., Brookings, SD (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
South Dakota School of Mines and Technology, Rapid City, SD (United States)
Army Research Lab., Adelphi, MD (United States)

Solid-state lithium batteries are generally considered as the next-generation battery technology that benefits from inherent nonflammable solid electrolytes and safe harnessing of high-capacity lithium metal. Among various solid-electrolyte candidates, cubic garnet-type Li₇La₃Zr₂O₁₂ ceramics hold superiority due to their high ionic conductivity (10^–3 to 10^–4 S cm^-1) and good chemical stability against lithium metal. However, practical deployment of solid-state batteries based on such garnet-type materials has been constrained by poor interfacing between lithium and garnet that displays high impedance and uneven current distribution. Herein, we propose a facile and effective strategy to significantly reduce this interfacial mismatch by modifying the surface of such garnet-type solid electrolyte with a thin layer of silicon nitride (Si₃N₄). This interfacial layer ensures an intimate contact with lithium due to its lithiophilic nature and formation of an intermediate lithium–metal alloy. The interfacial resistance experiences an exponential drop from 1197 to 84.5 Ω cm². Lithium symmetrical cells with Si₃N₄-modified garnet exhibited low overpotential and long-term stable plating/stripping cycles at room temperature compared to bare garnet. Furthermore, a hybrid solid-state battery with Si₃N₄-modified garnet sandwiched between lithium metal anode and LiFePO₄ cathode was demonstrated to operate with high cycling efficiency, excellent rate capability, and good electrochemical stability. This work represents a significant advancement toward use of garnet solid electrolytes in lithium metal batteries for the next-generation energy storage devices.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2469980

Journal Information:: ACS Applied Energy Materials, Journal Name: ACS Applied Energy Materials Journal Issue: 1 Vol. 5; ISSN 2574-0962

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
interfacial resistance
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Mitigating Interfacial Mismatch between Lithium Metal and Garnet-Type Solid Electrolyte by Depositing Metal Nitride Lithiophilic Interlayer

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