Journal
ACS APPLIED ENERGY MATERIALS
Volume 3, Issue 7, Pages 6775-6784Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsaem.0c00905
Keywords
solid-state electrolyte; garnet electrolyte; h-BN; moisture stability; dendrite suppression; in-situ Raman; lithium metal anode
Funding
- National Science Foundation [1751472]
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [1751472] Funding Source: National Science Foundation
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All-solid-state batteries using garnet-type solid-state electrolytes (SSEs) are promising candidates for safe, high energy density batteries due to their wide electrochemical stability window, high lithium-ion conductivity at room temperature, and the use of a lithium metal anode. However, garnet-type SSEs exhibit formidable challenges, including their instability in a moisture-containing atmosphere, high interfacial resistance, and the formation of lithium dendrites. Though several strategies have been deployed to alleviate the issues related to garnet-type SSEs against metallic lithium, most of the approaches fail to solve all the challenges. Herein, we demonstrate a surface modification strategy of the Li6.5La3Zr1.5Ta0.5O12 (LLZT) garnet electrolyte by two-dimensional hexagonal boron nitride (h-BN) nanosheets to solve the interfacial issues. Detailed spectroscopic evidence elucidates that the h-BN interlayer effectively protects the LLZT from moisture-induced chemical degradation and suppresses the formation of adverse carbonate species for over 120 h in an open atmosphere. The h-BN-coated garnet SSE interface has shown a nearly 10-fold reduction in interfacial resistance value compared to the uncoated one and it exhibits stable lithium plating/stripping behavior for over 1400 cycles at 0.2 mA cm(-2). Advanced in situ Raman analysis reveals that the h-BN interlayers remain stable during cycling and inhibit the structural transformation of LLZT at the interface.
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