Lithium argyrodites electrolyte with high ionic conductivity and relatively lower cost show great potential as candidates for solid-state batteries. Further improvement of their conductivities can accelerate their applications. One of the means to significantly promote the conductivity of Li-ion is dual doping. Herein, Ag/Br dual-doping strategy is applied on Li 6 PS 5 Br (2.76 mS cm −1 ) to boast its conductivity to 6.15 mS cm −1 for Li 5.55 Ag 0.05 PS 4.6 Br 1.4 . The structural variations and chemical/electrochemical stability of the obtained electrolyte are carefully investigated. Li 3 InCl 6 electrolyte is introduced in the new battery configuration to mitigate the interfacial instability with LiNi 0.6 Mn 0.2 Co 0.2 O 2 active material enabling good electrochemical performances . The assembled battery delivers a discharge capacity of 160.8 mAh g −1 for the 1st cycle and maintains 85.9% of the initial value after 50 cycles at 0.5C. This modification strategy was proved effective for increasing the conductivity of sulfide electrolytes in this work.
Composite solid polymer electrolytes (CSPEs) with inorganic
fillers
are of great interest for advanced all-solid-state lithium–metal
batteries (ASSLMBs), enabling high energy density and enhanced safety.
Despite increasing interest, the effects of different inorganic fillers
on the interface between CSPEs and the lithium metal anode (LMA) remain
not fully understood. Herein, we systematically study the contact
behavior between the LMA and CSPEs containing PEO, LiTFSI, as well
as oxide- (Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 ), sulfide- (Li 6 PS 5 Cl), and halide-based
(Li 3 InCl 6 ) fillers by evaporating lithium metal
stepwise onto CSPE thin films under ultrahigh vacuum conditions, followed
by in-system X-ray photoelectron spectroscopy (XPS)
analysis. XPS results demonstrate that halide-based fillers can facilitate
the formation of electron-rich Li–O and Li–S species
at the interfaces, acting as a passivation layer, which can prevent
further decomposition of the CSPE and thus improve interfacial stability.
In contrast, the incorporation of oxide- and sulfide-based fillers
does not promote the interfacial reactions. Impedance spectroscopy
as a function of resting time also shows that the incorporation of
a halide-based filler reduces the CSPE/LMA interfacial impedance,
which is beneficial for increasing the critical current density for
lithium dendrite formation. The incorporation of active inorganic
fillers to induce protective interphases offers a novel strategy for
interfacial engineering of ASSLMBs.
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