Crystal Orientation-Dependent Reactivity of Oxide Surfaces in Contact with Lithium Metal

Connell, Justin G.; Zhu, Yisi; Zapol, Peter; Tepavcevic, Sanja; Sharafi, Asma; Sakamoto, Jeff; Curtiss, Larry A.; Fong, Dillon D.; Freeland, John W.; Markovic, Nenad M.

doi:10.1021/acsami.8b03078

Title: Crystal Orientation-Dependent Reactivity of Oxide Surfaces in Contact with Lithium Metal

Journal Article · 30 April 2018 · ACS Applied Materials and Interfaces

DOI: https://doi.org/10.1021/acsami.8b03078 · OSTI ID:1455046

^[1]; Zhu, Yisi ^[1];

^[1]; Tepavcevic, Sanja ^[1];

^[2]; Sakamoto, Jeff ^[2];

^[1]; Fong, Dillon D. ^[1]; Freeland, John W. ^[1]; Markovic, Nenad M. ^[1]

Argonne National Lab. (ANL), Argonne, IL (United States)
Univ. of Michigan, Ann Arbor, MI (United States)

Understanding ionic transport across interfaces between dissimilar materials and the intrinsic chemical stability of such interfaces is a fundamental challenge spanning many disciplines and is of particular importance for designing conductive and stable solid electrolytes for solid-state Li-ion batteries. In this work, we establish a surface science-based approach for assessing the intrinsic stability of oxide materials in contact with Li metal. Through a combination of experimental and computational insights, using Nb-doped SrTiO3 (Nb/STO) single crystals as a model system, we were able to understand the impact of crystallographic orientation and surface morphology on the extent of the chemical reactions that take place between surface Nb, Ti, and Sr upon reaction with Li. By expanding our approach to investigate the intrinsic stability of the technologically relevant, polycrystalline Nb-doped lithium lanthanum zirconium oxide (Li6.5La3Zr1.5Nb0.5O12) system, we found that this material reacts with Li metal through the reduction of Nb, similar to that observed for Nb/STO. These results clearly demonstrate the feasibility of our approach to assess the intrinsic (in)stability of oxide materials for solid-state batteries and point to new strategies for understanding the performance of such systems.

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1455046

Journal Information:: ACS Applied Materials and Interfaces, Vol. 10, Issue 20; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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