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Boosting the interfacial superionic conduction of halide solid electrolytes for all-solid-state batteries
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Boosting the interfacial superionic conduction of halide solid electrolytes for all-solid-state batteries
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Journal Article
Boosting the interfacial superionic conduction of halide solid electrolytes for all-solid-state batteries
2023
Overview
Designing highly conductive and (electro)chemical stable inorganic solid electrolytes using cost-effective materials is crucial for developing all-solid-state batteries. Here, we report halide nanocomposite solid electrolytes (HNSEs) ZrO
2
(-ACl)-A
2
ZrCl
6
(A = Li or Na) that demonstrate improved ionic conductivities at 30 °C, from 0.40 to 1.3 mS cm
−1
and from 0.011 to 0.11 mS cm
−1
for Li
+
and Na
+
, respectively, compared to A
2
ZrCl
6
, and improved compatibility with sulfide solid electrolytes. The mechanochemical method employing Li
2
O for the HNSEs synthesis enables the formation of nanostructured networks that promote interfacial superionic conduction. Via density functional theory calculations combined with synchrotron X-ray and
6
Li nuclear magnetic resonance measurements and analyses, we demonstrate that interfacial oxygen-substituted compounds are responsible for the boosted interfacial conduction mechanism. Compared to state-of-the-art Li
2
ZrCl
6
, the fluorinated ZrO
2
−2Li
2
ZrCl
5
F HNSE shows improved high-voltage stability and interfacial compatibility with Li
6
PS
5
Cl and layered lithium transition metal oxide-based positive electrodes without detrimentally affecting Li
+
conductivity. We also report the assembly and testing of a Li-In||LiNi
0.88
Co
0.11
Mn
0.01
O
2
all-solid-state lab-scale cell operating at 30 °C and 70 MPa and capable of delivering a specific discharge of 115 mAh g
−1
after almost 2000 cycles at 400 mA g
−1
.
Compositional tuning is a standard procedure to improve the ionic conductivity of inorganic superionic conductors. Here, the authors report (electro)chemical stable composite halide solid electrolytes applying a nanostructure approach that promotes interfacial superionic conductivity.
