Incompatibility of electrolytes with Li anode impedes the application of solid-state batteries. Aluminum with appropriate potential, high-capacity, and electronic conductivity can alloy with Li spontaneously and is proposed herein as a carbon-free and binder-free anode of an all-solid-state Li-S battery (LSB). A biphasic lithiation reaction of Al with modest volume change was revealed by in situ characterization. The Li
0.8
Al alloy anode showed excellent compatibility toward the Li
10
GeP
2
S
12
(LGPS) electrolyte, as verified by the steady Li
0.8
Al-LGPS-Li
0.8
Al cell operation for over 2500 hours at 0.5 mA cm
−2
. An all-solid-state LSB comprising Li
0.8
Al alloy anode and melting-coated S composite cathode functioned steadily for over 200 cycles with a capacity retention of 93.29%. Furthermore, a Li-S full cell with a low negative-to-positive ratio of 1.125 delivered a specific energy of 541 Wh kg
−1
. This work provides an applicable anode selection for all-solid-state LSBs and promotes their practical procedure.
Lithium−sulfur (Li−S) batteries have received intense interest as next-generation electrochemical energy storage systems because of their high specific energy and natural abundance potential. However, its practical reality is seriously limited by the safety concerns from heterogeneous lithium deposition and the so-called "shuttle effect". Herein, this work reports a novel gel−polymer−inorganic separator specifically for the lithium−sulfur battery, which could enable homogeneous lithium deposition and inhibit the diffusion of polysulfides, simultaneously. The composite separator exhibits a superior electrochemical performance up to 500 cycles at 0.5 C with a capacity retention of 718.2 mA h g −1 . It is worth noting that the corresponding fade rate for 1000 cycles was 0.04%/cycle even tested at 2 C. This outstanding cycling stability can be attributed to the strong anchoring effect of polar carboxymethylcellulose sodium to polysulfides, which is confirmed by the permeation experiments and X-ray photoelectron spectroscopy analyses. Besides, the Al 2 O 3 coating layer on the anode side could achieve relatively uniform lithium deposition and inhibit the growth of dendrite to some extent. As a result, this study may provide a novel strategy for the effective design of separators toward the practical reality of the high-performance lithium−sulfur battery.
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