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Ultrahigh Areal Capacity Li Electrodeposition at Metal-Solid Electrolyte Interfaces under Minimal Stack Pressures Enabled by Interfacial Na-K Liquids.

ABSTRACT: The need for higher energy density rechargeable batteries has generated interest in metallic electrodes paired with solid electrolytes. However, impedance growth at the Li metal-solid electrolyte interface due to void formation during cycling at practical current densities and areal capacities, e.g., greater than 0.5 mA cm^-2 and 1.5 mAh cm^-2 respectively, remains a significant barrier. Here, we show that introducing a wetting interfacial film of Na-K liquid between the Li metal and the Li_6.75La₃Zr_1.75Ta_0.25O₁₂ (LLZTO) solid electrolyte permits reversible stripping and plating of up to 150 μm of Li (30 mAh cm^-2), approximately 10 times the areal capacity of today's lithium-ion batteries, at current densities above 0.5 mA cm^-2 and stack pressures below 75 kPa, all with minimal changes in cell impedance. We further show that this increase in the accessible areal capacity at high stripping current densities is due to the presence of Na-K liquid at the Li stripping interface; this performance improvement is not enabled in the absence of the Na-K liquid. This design approach holds promise for overcoming interfacial stability issues that have heretofore limited the performance of solid-state metal batteries.

SUBMITTER: Park RJ

PROVIDER: S-EPMC10401566 | biostudies-literature | 2023 Aug

REPOSITORIES: biostudies-literature

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Ultrahigh Areal Capacity Li Electrodeposition at Metal-Solid Electrolyte Interfaces under Minimal Stack Pressures Enabled by Interfacial Na-K Liquids.

Park Richard J-Y RJ Fincher Cole D CD Badel Andres F AF Carter W Craig WC Chiang Yet-Ming YM

ACS applied materials & interfaces 20230719 30

The need for higher energy density rechargeable batteries has generated interest in metallic electrodes paired with solid electrolytes. However, impedance growth at the Li metal-solid electrolyte interface due to void formation during cycling at practical current densities and areal capacities, e.g., greater than 0.5 mA cm<sup>-2</sup> and 1.5 mAh cm<sup>-2</sup> respectively, remains a significant barrier. Here, we show that introducing a wetting interfacial film of Na-K liquid between the Li m ...[more]

PMID: 37468128

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Project description:We evaluate the influence of Li-salt doping on the dynamics, capacitance, and structure of three ionic liquid electrolytes, [pyr14][TFSI], [pyr13][FSI], and [EMIM][BF4], using molecular dynamics and polarizable force fields. In this respect, our focus is on the properties of the electric double layer (EDL) formed by the electrolytes at the electrode surface as a function of surface potential (Ψ). The rates of EDL formation are found to be on the order of hundreds of picoseconds and only slightly influenced by the addition of Li-salt. The EDLs of three electrolytes are shown to have different energy storage capacities, which we relate to the EDL formation free energy. The differential capacitance obtained from our computations exhibits asymmetry about the potential of zero charge and is consistent with the camel-like profiles noted from mean field theories and experiments on metallic electrodes. The introduction of Li-salt reduces the noted asymmetry in the differential capacitance profile. Complementary experimental capacitance measurements have been made on our three electrolytes in their neat forms and with Li-salt. The measurements, performed on glassy carbon electrodes, produce U-like profiles, and Li-salt doping is shown to strongly affect capacitance at high magnitudes of Ψ. Differences in the theoretical and experimental shapes and magnitudes of capacitance are rationalized in terms of the electrode surface and pseudocapacitive effects. In both neat and Li-doped liquids, the details of the computational capacitance profile are well described by Ψ-induced changes in the density and molecular orientation of ions in the molecular layer closest to the electrode. Our results suggest that the addition of Li+ induces disorder in the EDL, which originates from the strong binding of anions to Li+. An in-depth analysis of the distribution of Li+ in the EDL reveals that it does not readily enter the molecular layer at the electrode surface, preferring instead to be localized farther away from the surface in the second molecular layer. This behavior is validated through an analysis of the free energy of Li+ solvation as a function of distance from the electrode. Free energy wells are found to coincide with localized concentrations of Li+, the depths of which increase with Ψ and suggest a source of impedance for Li+ to reach the electrode. Finally, we make predictions of the specific energy at ideal graphite utilizing the computed capacitance and previously derived electrochemical windows of the liquids.

Dataset Information

Ultrahigh Areal Capacity Li Electrodeposition at Metal-Solid Electrolyte Interfaces under Minimal Stack Pressures Enabled by Interfacial Na-K Liquids.

Publications

Ultrahigh Areal Capacity Li Electrodeposition at Metal-Solid Electrolyte Interfaces under Minimal Stack Pressures Enabled by Interfacial Na-K Liquids.

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