Avoiding CO 2 Improves Thermal Stability at the Interface of Li 7 La 3 Zr 2 O 12 Electrolyte with Layered Oxide Cathodes

Kim, Younggyu; Waluyo, Iradwikanari; Hunt, Adrian; Yildiz, Bilge

doi:10.1002/aenm.202102741

Avoiding CO ₂ Improves Thermal Stability at the Interface of Li ₇ La ₃ Zr ₂ O ₁₂ Electrolyte with Layered Oxide Cathodes

Journal Article · Thu Feb 17 00:00:00 EST 2022 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202102741· OSTI ID:1845582

^[1]; Waluyo, Iradwikanari ^[2]; Hunt, Adrian ^[2]; Yildiz, Bilge ^[1]

Laboratory for Electrochemical Interfaces Department of Nuclear Science and Engineering Massachusetts Institute of Technology Cambridge MA 02139 USA, Department of Materials Science and Engineering Massachusetts Institute of Technology Cambridge MA 02139 USA
National Synchrotron Light Source II Brookhaven National Laboratory Upton NY 11973 USA

Abstract

Solid‐state batteries promise higher energy densities and better safety than Li‐ion batteries with liquid electrolytes. However, the interface between solid electrolyte and cathode is unstable at the elevated temperatures that are needed while sintering to achieve good bonding between ceramic components. Here, the hypothesis is that, the gas environment, especially the presence of CO _2, is critical in determining the stability of the solid electrolyte–cathode interface. The effect of gas species on the interface is systematically probed, by a using Li ₇ La ₃ Zr ₂ O ₁₂ (LLZO) solid electrolyte with a thin film LiNi _0.6 Mn _0.2 Co _0.2 O ₂ cathode as a model system to enable interface sensitivity. Detrimental phases formed at the interface and their onset conditions are identified by X‐ray absorption spectroscopy, X‐ray diffraction, and Gibbs free energy analysis. As a result, removing CO ₂ and minimizing H ₂ O(g) during sintering is necessary to obtain good contact at the LLZO|cathode interface without forming secondary phases. Sintering in O ₂ is ideal, yielding excellent chemical stability and low interfacial resistance. Secondary phases also do not form in N _2, but oxygen loss occurs at elevated temperatures. The interfacial resistance obtained upon sintering in pure O ₂ is comparable to the lowest values at LLZO interfaces with protective coatings, but here without the need for interface coatings.

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

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)' US Army Research Office

Grant/Contract Number:: SC0012704

OSTI ID:: 1845582

Alternate ID(s):: OSTI ID: 1845584
OSTI ID: 1887538
OSTI ID: 23130442

Report Number(s):: BNL-223302-2022-JAAM; 2102741

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 13 Vol. 12; ISSN 1614-6832

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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