Ultrafast-Sintered Self-Standing LLZO Membranes for High Energy Density Li-Garnet Solid-State Batteries

When and Where

Apr 12, 2023
9:30am - 9:45am

Moscone West, Level 2, Room 2006

Presenter

Huanyu Zhang

Faruk Okur

Kostiantyn Kravchyk

Maksym Kovalenko

Co-Author(s)

Huanyu Zhang^1,2,Faruk Okur^1,2,Kostiantyn Kravchyk^1,2,Maksym Kovalenko^1,2

ETH Zürich¹,Empa–Swiss Federal Laboratories for Materials Science and Technology²

Abstract

Huanyu Zhang^1,2,Faruk Okur^1,2,Kostiantyn Kravchyk^1,2,Maksym Kovalenko^1,2

ETH Zürich¹,Empa–Swiss Federal Laboratories for Materials Science and Technology²

Towards building non-flammable and temperature-tolerant Li-ion batteries with high energy density, Li7La3Zr2O12 (LLZO) has recently attracted considerable attention as a compelling solid-state Li-ion electrolyte (SSE) due to its high thermal stability, Li-ion conductivity of up to 1 mS cm−1 (RT), and a wide electrochemical operation window of 0–6 V vs. Li+/Li.[1, 2] Additionally, unlike other Li-ion soft solid conductors such as those based on sulfides, LLZO SSE can be manufactured with a bilayer dense-porous microstructure, which prevents the issues of dynamic volume change of the Li anode and the formation of voids at the Li/SSE interface during cycling and thus eliminates the need for external pressure.[3, 4] Here we report a facile, ultrafast sintering methodology for the fabrication of LLZO solid-state electrolyte in the form of self-standing bilayer dense-porous LLZO membranes. The thickness of the produced dense and porous layers was ca. 8 µm and 55 µm, which hypothetically allows to achieve high gravimetric and volumetric energy densities of Li-garnet batteries of 202 Wh kg−1 and 715 Wh L−1 (in combination with an NMC111/LiFSI-Pyr13FSI cathode). Electrochemical measurements confirmed that produced LLZO membranes possess high critical current density up to 1.7 mA cm−2 and cycling stability of over 45 cycles at a current density of 0.1 mA cm−2. References [1] R. Dubey, J. Sastre, C. Cancellieri, F. Okur, A. Forster, L. Pompizii, A. Priebe, Y. E. Romanyuk, L. P. H. Jeurgens, M. V. Kovalenko, K. V. Kravchyk, Adv. Energy Mater. 2021, 2102086. [2] S. Afyon, K. V. Kravchyk, S. Wang, J. v. d. Broek, C. Hänsel, M. V. Kovalenko, J. L. M. Rupp, J. Mater. Chem. A 2019, 7, 21299. [3] K. V. Kravchyk, F. Okur, M. V. Kovalenko, ACS Energy Lett. 2021, 2202. [4] K.V. Kravchyk, H. Zhang, F. Okur, M.V. Kovalenko, Acc. Mater. Res., 2022, 3, 4, 411–415.