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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.
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.
Quantitatively Designing Porous Copper Current Collectors for Lithium Metal Anodes
Not provided.
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.
Engineering and characterization of interphases for lithium metal anodes
Different strategies of SEI engineering such as modification, additive application, and artificial SEI for electrolyte are summarized. Characterization techniques for SEI studies using X-ray, neutron, and electron as probing beams are discussed.
Identifying Limitations of the Lithium Metal Anode through Laser Plasma Focused Ion Beam Cross-Sectional Imaging.
Abstract not provided.
Understanding lithium metal anodes in batteries through cryogenic focused ion beam and electron microscopy techniques.
Abstract not provided.
Lithium Metal Anode Self Discharge
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Development of high energy density primary batteries 200 watt hours per pound total battery weight minimum third quarterly report, 10 dec. 1964 - 9 mar. 1965
Electrolyte and electrode studies for high energy lithium anode primary cells
A program to develop a high-energy density primary battery with a minimum of 200 watt hours per pound of total battery weight Sixth quarterly report, Oct. 1 - Dec. 31, 1965
Lithium anodes, inorganic and organic cathodes, vacuum-distilled solvents, and methods for sintering cupric fluoride on lightweight metal substrates - development of high energy battery
Conductive polymer binder for a novel silicon/graphene anode in lithium ion batteries
A composite electrode prepared from silicon-graphene material and conductive polymer binder poly (1-pyrenemethyl methacrylate-co-methacrylic acid) for use in lithium-ion batteries.
Semi-tubular carbon film for stable lithium metal anodes and methods of manufacture thereof
A method of forming a battery electrode by forming, on a first substrate, a polymer template comprising interconnected polymer fibers, forming, on the polymer template, a carbon coating to form a carbon-coated polymer template, removing the carbon-coated polymer template from the first substrate, subsequent to removing the carbon-coated polymer template from the first substrate, removing the polymer template from the carbon coating, and disposing the carbon coating on a second substrate. A solid electrolyte interphase layer (SEI) comprising the carbon coating produced via the method, a battery electrode comprising such an SEI layer, and a battery comprising such a battery electrode are also provided.
Anomalous Self-Optimizing Microporous Graphene-Based Lithium-ion Battery Anode from Laser Activation
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Large-Area Lithium Electrode Sub-Assemblies (LESAs) Protected by Self Forming Microstructured Polymer-Inorganic Single-Ion Conducting Composites (Final Report)
The aim of this project is to realize a low-cost, safe, reversible, high-areal capacity lithium metal electrode though the use of scalable, low-cost Lithium Electrode Sub-Assembly (LESA). At its core, the LESA applies novel polymer scaffolds to nanostructure inorganic ionic materials into high-conductivity composites that stabilize lithium anodes during high-rate, high-capacity cycling in lithium metal batteries. Fundamental investigations from this project identified a newly defined region of stability for composites with respect to the shear modulus and lithium molar volume ratio which have been broadly applied in the scientific literature for a multitude of different systems. The advancements achieved in this field have furthered the fundamental understanding of lithium metal electrode chemistry and degradation mechanisms and resulted in a lithium metal anode with improved cycle life.