The
application of flexible, robust, and low-cost solid polymer
electrolytes in next-generation all-solid-state lithium metal batteries
has been hindered by the low room-temperature ionic conductivity of
these electrolytes and the small critical current density of the batteries.
Both issues stem from the low mobility of Li+ ions in the
polymer and the fast lithium dendrite growth at the Li metal/electrolyte
interface. Herein, Mg(ClO4)2 is demonstrated
to be an effective additive in the poly(ethylene oxide) (PEO)-based
composite electrolyte to regulate Li+ ion transport and
manipulate the Li metal/electrolyte interfacial performance. By combining
experimental and computational studies, we show that Mg2+ ions are immobile in a PEO host due to coordination with ether oxygen
and anions of lithium salts, which enhances the mobility of Li+ ions; more importantly, an in-situ formed Li+-conducting Li2MgCl4/LiF
interfacial layer homogenizes the Li+ flux during plating
and increases the critical current density up to a record 2 mA cm–2. Each of these factors contributes to the assembly
of competitive all-solid-state Li/Li, LiFePO4/Li, and LiNi0.8Mn0.1Co0.1O2/Li cells,
demonstrating the importance of surface chemistry and interfacial
engineering in the design of all-solid-state Li metal batteries for
high-current-density applications.
Knowledge about degradation and failure of Li-ion batteries (LIBs) is of paramount importance especially because failure can be accompanied by severe hazards. To contribute to the understanding of such phenomena synchrotron in-line phase contrast Xray tomography was employed to investigate internal cell deformation and degradation caused by an internal short circuit (ISC). The tomographic images taken from an uncycled Li/Li cell and a short-circuited Li/Li cell reveal how lithium microstructures (LmS) develop during electrochemical stripping and plating during discharge and charge and how the three-layer separator used is damaged by growing LmSs and delaminates and melts as a consequence of an ISC. Previously unknown insights into the internal cell degradation and deformation mechanisms caused by an ISC are obtained and provide hints of how the properties of the separator could be modified in order to improve the reliability and safety of current and next-generation LIBs.
Limited
understanding of the lithium (Li) nucleation and growth
mechanism has hampered the implementation of Li-metal batteries. Herein,
we unravel the evolution of the morphology and inner structure of
Li deposits using focused ion beam scanning electron microscopy (FIB/SEM).
Ball-shaped Li deposits are found to be widespread and stack up at
a low current density. When the current density exceeds the diffusion-limiting
current, bush-shaped deposition appears that consists of Li-balls,
Li-whiskers, and bulky Li. Cryogenic transmission electron microscopy
(cryo-TEM) further reveals that Li-balls are primarily amorphous,
whereas the Li-whiskers are highly crystalline. Additionally, the
solid electrolyte interface (SEI) layers of the Li-balls and whiskers
show a difference in structure and composition, which is correlated
to the underlying deposition mechanism. The revealed Li nucleation
and growth mechanism and the correlation with the nanostructure and
chemistry of the SEI provide insights toward the practical use of
rechargeable Li-metal batteries.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.