All-solid-state lithium-based batteries with inorganic solid electrolytes are considered a viable option for electrochemical energy storage applications. However, the application of lithium metal is hindered by issues associated with the growth of mossy and dendritic Li morphologies upon prolonged cell cycling and undesired reactions at the electrode/solid electrolyte interface. In this context, alloy materials such as lithium-indium (Li-In) alloys are widely used at the laboratory scale because of their (electro)chemical stability, although no in-depth investigations on their morphological stability have been reported yet. In this work, we report the growth of Li-In dendritic structures when the alloy material is used in combination with a Li6PS5Cl solid electrolyte and Li(Ni0.6Co0.2Mn0.2)O2 positive electrode active material and cycled at high currents (e.g., 3.8 mA cm−2) and high cathode loading (e.g., 4 mAh cm−2). Via ex situ measurements and simulations, we demonstrate that the irregular growth of Li-In dendrites leads to cell short circuits after room-temperature long-term cycling. Furthermore, the difference between Li and Li-In dendrites is investigated and discussed to demonstrate the distinct type of dendrite morphology.
Fe-based multiphase nanocrystallized ribbons (CR-II) prepared by annealing of metallic glasses show unexpected high performance for Orange II degradation.
A stable electrode–electrolyte interface is the
key for
the application of high-energy all-solid-state lithium metal batteries,
but the nanoscale behavior of the interface remains mysterious. Herein,
utilizing cryogenic transmission electron microscopy, we investigate
the nanostructure of the interphase layer between a single Li dendrite
and sulfide electrolyte (SE) at various temperatures. It is found
that a single-crystal Li2S layer with ∼12 nm thickness
is formed at 25 °C with good passivation on the interface, while
at 60 °C, the interphase is composed of polycrystalline Li2S accompanied by a disorder–order phase transition.
The increased grain boundaries and enlarged thickness of interphase
at elevated temperature lead to ultra-high interface resistance. The
temporal evolution of the atom-scale structure was further elucidated
by reactive dynamics simulations to assist in understanding the kinetics.
Our study provides new insight on the nanoscale interphase of the
Li-SE interface and will offer valuable guidance for the future design
and engineering of interfaces.
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