In this study, dendrite growth at the anode-electrolyte interface was simulated using an Extended Butler-Volmer Smoothed Particle Hydrodynamics (eBV-SPH) model implemented in LAMMPS. While a constant current (CC) charging protocol has been standard, recent studies have shown that a pulse plating (PP) charging protocol is effective at reducing dendrite growth and improving cycle life. The formation of dendrites on lithium electrodes presents safety and cycling challenges for the development of high-performance, rechargeable lithium metal batteries. We expect that this article will help boost more efforts in exploring advanced surface coatings via ALD and MLD to successfully mitigate the issues of alkali metal anodes. In this review, we have made a thorough survey on surface coatings via ALD and MLD, and comparatively analyzed their effects on improving the safety and stability of alkali metal anodes. Consequently, ALD and MLD have paved a novel route for tackling the issues of alkali metal anodes. ALD and MLD enable a variety of inorganic, organic, and even inorganic-organic hybrid materials, featuring accurate nanoscale controllability, low process temperature, and extremely uniform and conformal coverage. Among them, atomic and molecular layer deposition (ALD and MLD) have been drawing more and more efforts, owing to a series of their unique capabilities. Many technical strategies have been developed for addressing these two issues in the past decades. Two commonly experienced issues, however, have hindered them from commercialization: the dendritic growth of alkali metals during plating and the formation of solid electrolyte interphase due to contact with liquid electrolytes. We propose further studies on the fundamental understanding of cationic and anionic redox mixing and the effect of transition metals on redox behavior to excite the full energy potential of Li-rich layered cathodes.Īlkali metals (lithium, sodium, and potassium) are promising as anodes in emerging rechargeable batteries, ascribed to their high capacity or abundance. We highlight that not only the type of transition metals but also the composition of transition metals strongly affects redox behavior. The case-by-case redox evolution processes of Li-rich 3d/4d/5d transition metal O3 type layered cathodes are discussed. Various synchrotron X-ray spectroscopy methods which can identify charge compensation by cations and anions are summarized. In this review, we present the general redox evolution of Li-rich layered cathodes upon activation of reversible oxygen redox. Therefore, advanced characterization techniques have been developed to explore the fundamental understanding underlying their unusual phenomenon, such as the redox evolution of these materials. However, they exhibit different electrochemical profiles before and after oxygen redox activation. Li-rich layered oxides utilizing reversible oxygen redox are promising cathodes for high-energy-density lithium-ion batteries. As a result, when the amount of CuO is 0.5 wt%, LLZO-Ga shows the highest room-temperature ionic conductivity and the lowest activation energy, which are 1.111 mS/cm and 0.27 eV, respectively. It is found that adding a small amount of CuO as an additive can reduce the sintering temperature from 1100 ℃ to about 1000 ℃. Herein, we synthesized garnet-type solid electrolytes of Li6.1Ga0.3La3Zr2O12 (LLZO-Ga) with x wt% CuO (x = 0, 0.2, 0.5, 1, 2) by the traditional solid-state reaction method, in which CuO was introduced as a sintering aid to reduce the sintering temperature of LLZO-Ga and increase its Li-ion conductivity. Therefore, it is an important issue how to reduce the synthesis temperature of LLZO and simultaneously increase its ionic conductivity. However, the synthesis of LLZO often requires a high temperature, which may lead to the evaporation of the lithium and result in a decrease in ionic conductivity. Garnet-type Li7La3Zr2O12 (LLZO) is considered as a promising solid electrolyte.
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