Dataset Information

Understanding the Surface Regeneration and Reactivity of Garnet Solid-State Electrolytes.

ABSTRACT: Garnet solid-electrolyte-based Li-metal batteries can be used in energy storage devices with high energy densities and thermal stability. However, the tendency of garnets to form lithium hydroxide and carbonate on the surface in an ambient atmosphere poses significant processing challenges. In this work, the decomposition of surface layers under various gas environments is studied by using two surface-sensitive techniques, near-ambient-pressure X-ray photoelectron spectroscopy and grazing incidence X-ray diffraction. It is found that heating to 500 °C under an oxygen atmosphere (of 1 mbar and above) leads to a clean garnet surface, whereas low oxygen partial pressures (i.e., in argon or vacuum) lead to additional graphitic carbon deposits. The clean surface of garnets reacts directly with moisture and carbon dioxide below 400 and 500 °C, respectively. This suggests that additional CO₂ concentration controls are needed for the handling of garnets. By heating under O₂ along with avoiding H₂O and CO₂, symmetric cells with less than 10 Ωcm² interface resistance are prepared without the use of any interlayers; plating currents of >1 mA cm^-2 without dendrite initiation are demonstrated.

SUBMITTER: Vema S

PROVIDER: S-EPMC10425971 | biostudies-literature | 2023 Aug

REPOSITORIES: biostudies-literature

ACCESS DATA

Publications

Understanding the Surface Regeneration and Reactivity of Garnet Solid-State Electrolytes.

Vema Sundeep S Sayed Farheen N FN Nagendran Supreeth S Karagoz Burcu B Sternemann Christian C Paulus Michael M Held Georg G Grey Clare P CP

ACS energy letters 20230720 8

Garnet solid-electrolyte-based Li-metal batteries can be used in energy storage devices with high energy densities and thermal stability. However, the tendency of garnets to form lithium hydroxide and carbonate on the surface in an ambient atmosphere poses significant processing challenges. In this work, the decomposition of surface layers under various gas environments is studied by using two surface-sensitive techniques, near-ambient-pressure X-ray photoelectron spectroscopy and grazing incide ...[more]

PMID: 37588018

Similar Datasets

Project description:Ionic transport in solid electrolytes can often be approximated as ions performing a sequence of hops between distinct lattice sites. If these hops are uncorrelated, quantitative relationships can be derived that connect microscopic hopping rates to macroscopic transport coefficients; i.e. tracer diffusion coefficients and ionic conductivities. In real materials, hops are uncorrelated only in the dilute limit. At non-dilute concentrations, the relationships between hopping frequency, diffusion coefficient and ionic conductivity deviate from the random walk case, with this deviation quantified by single-particle and collective correlation factors, f and fI, respectively. These factors vary between materials, and depend on the concentration of mobile particles, the nature of the interactions, and the host lattice geometry. Here, we study these correlation effects for the garnet lattice using lattice-gas Monte Carlo simulations. We find that, for non-interacting particles (volume exclusion only), single-particle correlation effects are more significant than for any previously studied three-dimensional lattice. This is attributed to the presence of two-coordinate lattice sites, which causes correlation effects intermediate between typical three-dimensional and one-dimensional lattices. Including nearest-neighbour repulsion and on-site energies produces more complex single-particle correlations and introduces collective correlations. We predict particularly strong correlation effects at xLi=3 (from site energies) and xLi=6 (from nearest-neighbour repulsion), where xLi=9 corresponds to a fully occupied lithium sublattice. Both effects are consequences of ordering of the mobile particles. Using these simulation data, we consider tuning the mobile-ion stoichiometry to maximize the ionic conductivity, and show that the 'optimal' composition is highly sensitive to the precise nature and strength of the microscopic interactions. Finally, we discuss the practical implications of these results in the context of lithium garnets and other solid electrolytes.

Dataset Information

Understanding the Surface Regeneration and Reactivity of Garnet Solid-State Electrolytes.

Publications

Understanding the Surface Regeneration and Reactivity of Garnet Solid-State Electrolytes.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets