Tuning the Anode–Electrolyte Interface Chemistry for Garnet-Based Solid-State Li Metal Batteries

Deng, Tao; Ji, Xiao; Zhao, Yang; Cao, Longsheng; Li, Shuang; Hwang, Sooyeon; Luo, Chao; Wang, Pengfei; Jia, Haiping; Fan, Xiulin; Lu, Xiaochuan; Su, Dong; Sun, Xueliang; Wang, Chunsheng; Zhang, Ji‐Guang

doi:10.1002/adma.202000030

Title: Tuning the Anode–Electrolyte Interface Chemistry for Garnet-Based Solid-State Li Metal Batteries

Journal Article · Mon May 04 00:00:00 EDT 2020 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202000030· OSTI ID:1631926

Deng, Tao ^[1]; Ji, Xiao ^[2]; Zhao, Yang ^[3]; Cao, Longsheng ^[2]; Li, Shuang ^[4];

^[4]; Luo, Chao ^[5]; Wang, Pengfei ^[2]; Jia, Haiping ^[6]; Fan, Xiulin ^[2]; Lu, Xiaochuan ^[7]; Su, Dong ^[4]; Sun, Xueliang ^[3];

^[2]; Zhang, Ji‐Guang ^[6]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. of Maryland, College Park, MD (United States)
Univ. of Maryland, College Park, MD (United States)
Univ. of Western Ontario, London, ON (Canada)
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
George Mason Univ., Fairfax, VA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
North Carolina A & T State Univ., Greensboro, NC (United States)

Lithium (Li) metal anode is a promising candidate for high energy density solid-state batteries. However, the interface issues, including large interfacial resistance and Li dendrite generation, have always frustrated the attempt to commercialize solid-state Li metal batteries (SSLBs). Here, we report that infusing the garnet-type solid electrolytes (GSEs) with air-stable electrolyte Li₃PO₄ (LPO) dramatically reduces the interfacial resistance to ~1 Ω cm² and achieves a high critical current density of 2.2 mA cm^-2 under ambient condition due to enhanced interfacial stability to Li metal anode. The coated and infused LPO electrolytes not only improve the mechanical strength and Li-ion conductivity of grain boundaries, but also form a stable Li-ion conductive but electron-insulating LPO-derived solid-electrolyte interphase between Li metal and GSEs, and consequently eliminates the Li dendrites growth and prevents the direct reduction of GSEs by Li metal over a long cycle life. This interface engineering approach together with grain-boundary modification on GSEs represents a promising strategy to revolutionize the anode-electrolyte interface chemistry for SSLBs and provides new design strategy for other-types of solid-state batteries.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: SC0012704; AC02‐05CH11231

OSTI ID:: 1631926

Alternate ID(s):: OSTI ID: 1617070

Report Number(s):: BNL-215968-2020-JAAM

Journal Information:: Advanced Materials, Vol. 32, Issue 23; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 130 works

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Title: Tuning the Anode–Electrolyte Interface Chemistry for Garnet-Based Solid-State Li Metal Batteries

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