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At least 163 records · Page 9

Transferring Liquid Metal to form a Hybrid Solid Electrolyte via a Wettability-Tuning Technology for Lithium-Metal Anodes

Integrating solid-state electrolyte (SSE) into Li-metal anodes has demonstrated great promise to unleash the high energy density of rechargeable Li-metal batteries. However, fabricating a highly cyclable SSE/Li-metal anode remains a major challenge because the densification of the SSE is usually incompatible with the reactive Li metal. Here, a liquid-metal-derived hybrid solid electrolyte (HSE) is proposed, and a facile transfer technology to construct an artificial HSE on the Li metal is reported. By tuning the wettability of the transfer substrates, electron- and ion-conductive liquid metal is sandwiched between electron-insulating and ion-conductive LiF and oxides to form the HSE. The transfer technology renders the HSE continuous, dense, and uniform. The HSE, having high ion transport, electron shut-off, and mechanical strength, makes the composite anode deliver excellent cyclability for over 4000 h at 0.5 mA cm(-2) and 1 mAh cm(-2) in a symmetrical cell. When pairing with LiFePO4 and sulfur cathodes, the HSE-coated Li metal dramatically enhances the performance of full cells. Therefore, this work demonstrates that tuning the interfacial wetting properties provides an alternate approach to build a robust solid electrolyte, which enables highly efficient Li-metal anodes.

li-metal anodes↗

Elucidating Interfacial Stability between Lithium Metal Anode and Li Phosphorus Oxynitride via In Situ Electron Microscopy

Li phosphorus oxynitride (LiPON) is one of a very few solid electrolytes that have demonstrated high stability against Li metal and extended cyclability with high Coulombic efficiency for all solid-state batteries (ASSBs). However, theoretical calculations show that LiPON reacts with Li metal. Here, we utilize in situ electron microscopy to observe the dynamic evolutions at the LiPON–Li interface upon contacting and under biasing. We reveal that a thin interface layer (~60 nm) develops at the LiPON–Li interface upon contact. This layer is composed of conductive binary compounds that show a unique spatial distribution that warrants an electrochemical stability of the interface, serving as an effective passivation layer. Our results explicate the excellent cyclability of LiPON and reconcile the existing debates regarding the stability of the LiPON–Li interface, demonstrating that, though glassy solid electrolytes may not have a perfect initial electrochemical window with Li metal, they may excel in future applications for ASSBs.

25 ENERGY STORAGE↗

Elucidating the Effects of LiF on Lithium Metal Anodes

LiF is widely recognized as a crucial component of a solid-electrolyte interphase (SEI) for Li metal anodes. However, the roles of LiF in the SEI remain elusive. Herein, we examined the evolution of SEI influenced by LiF and identified distinct features that elucidate functional characteristics of LiF for Li metal anodes. Through comprehensive empirical and theoretical analyses, we found that LiF enriches Li2O within the SEI, forms LiF/Li2O interfaces, exhibits non-negligible solubility with spontaneous dissolution-reprecipitation behavior in the electrolyte, and works synergistically with Li2O. These findings shed light on the effects of LiF on Li metal anodes and the arrangement characteristic of LiF within the SEI. By integrating key discoveries regarding LiF, a projected working mechanism for LiF is illustrated. Overall, our study on LiF provides valuable insights that advance the understanding of the SEI and interphase nanostructures, contributing to the development of more reliable and practical Li metal batteries.

Kim, Mun Sek↗

Dissolution of the Solid Electrolyte Interphase and Its Effects on Lithium Metal Anode Cyclability

At >95% Coulombic efficiencies, most of the capacity loss for Li metal anodes (LMAs) is through the formation and growth of the solid electrolyte interphase (SEI). However, the mechanism through which this happens remains unclear. One property of the SEI that directly affects its formation and growth is the SEI’s solubility in the electrolyte. Here, in this work, we systematically quantify and compare the solubility of SEIs derived from ether-based electrolytes optimized for LMAs using in-operando electrochemical quartz crystal microbalance (EQCM). A correlation among solubility, passivity, and cyclability established in this work reveals that SEI dissolution is a major contributor to the differences in passivity and electrochemical performance among battery electrolytes. Together with our EQCM, X-ray photoelectron spectroscopy (XPS), and nuclear magnetic resonance (NMR) spectroscopy results, we show that solubility depends on not only the SEI’s composition but also the properties of the electrolyte. This provides a crucial piece of information that could help minimize capacity loss due to SEI formation and growth during battery cycling and aging.

25 ENERGY STORAGE↗