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ACS Appl Energy Mater ; 6(3): 1661-1672, 2023 Feb 13.
Artigo em Inglês | MEDLINE | ID: mdl-36817749


Most highly Li-conducting solid electrolytes (σRT > 10-3 S cm-1) are unstable against lithium-metal and suffer from detrimental solid-electrolyte decomposition at the lithium-metal/solid-electrolyte interface. Solid electrolytes that are stable against lithium metal thus offer a direct route to stabilize lithium-metal/solid-electrolyte interfaces, which is crucial for realizing all-solid-state batteries that outperform conventional lithium-ion batteries. In this study, we investigate Li5NCl2 (LNCl), a fully-reduced solid electrolyte that is thermodynamically stable against lithium metal. Combining experiments and simulations, we investigate the lithium diffusion mechanism, different synthetic routes, and the electrochemical stability window of LNCl. Li nuclear magnetic resonance (NMR) experiments suggest fast Li motion in LNCl, which is however locally confined and not accessible in macroscopic LNCl pellets via electrochemical impedance spectroscopy (EIS). With ab-initio calculations, we develop an in-depth understanding of Li diffusion in LNCl, which features a disorder-induced variety of different lithium jumps. We identify diffusion-limiting jumps providing an explanation for the high local diffusivity from NMR and the lower macroscopic conductivity from EIS. The fundamental understanding of the diffusion mechanism we develop herein will guide future conductivity optimizations for LNCl and may be applied to other highly-disordered fully-reduced electrolytes. We further show experimentally that the previously reported anodic limit (>2 V vs Li+/Li) is an overestimate and find the true anodic limit at 0.6 V, which is in close agreement with our first-principles calculations. Because of LNCl's stability against lithium-metal, we identify LNCl as a prospective artificial protection layer between highly-conducting solid electrolytes and strongly-reducing lithium-metal anodes and thus provide a computational investigation of the chemical compatibility of LNCl with common highly-conducting solid electrolytes (Li6PS5Cl, Li3YCl6, ...). Our results set a framework to better understand and improve highly-disordered fully-reduced electrolytes and highlight their potential in enabling lithium-metal solid-state batteries.

RSC Adv ; 10(40): 24108-24114, 2020 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-35517340


Carbon inverse opals (IOs) were prepared via a facile synthesis approach using a sucrose-based precursor and polystyrene (PS) spheres as a sacrificial template. During IO preparation, polymer spheres are typically removed by dispersion in organic solvents, such as toluene or tetrahydrofuran. In this study, carbon IOs are prepared with and without removal of PS spheres by toluene to determine the influence of template removal prior to high-temperature treatment on the morphology and chemistry of the resulting carbons. Properties of samples are compared through a systematic investigation by electron microscopy, Fourier-transform infrared spectroscopy and Raman spectroscopy. We demonstrate that a commonly used processing step-polymer sphere template chemical removal-does not make any significant difference to the IO morphology. A correlation of Raman spectroscopy with SEM imaging and TGA analysis indicates that carbon IOs prepared without the solvent-treatment step are more ordered than samples prepared with this processing step. The key finding of this report is the simplified IO synthesis procedure, which can be adapted to the preparation of IOs of other materials besides carbon.