Lithium Ion-Channel Polymer Electrolyte for Lithium Metal Anode Rechargeable Batteries
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Reducing the electrolyte amount is critical for high practical specific energy of Li-S batteries. The lean electrolyte condition raises a complex situation for sulfur redox reactions since they rely on the electrolyte mediation. The insulating nature of discharge product Li 2 S and its uncontrollable accumulation (passivation) at the cathode interface is one of the major challenges for stable cycling of a Li-S battery under lean electrolyte condition. Here, we present that the NH 4 TFSI additive in electrolyte solution greatly alleviates the passivation issue in Li-S batteries under lean electrolyte condition. The ammonium additive enhances the solvation between sulfide anion and NH 4 + cation, and greatly reduces the amount of large insoluble and insulting Li 2 S particles in the sulfur cathodes, which greatly facilitates the reversible and sustainable redox reactions of sulfur. Therefore, the cycle life of Li-S battery under lean electrolyte condition was greatly improved. In addition, we found that the morphology of Li anode is dependent on the cathode structures. Ammonium additive enables a homogeneous surface of cathode and Li anode and extended cycle life.
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Abstract The solid‐state Li battery is a promising energy‐storage system that is both safe and features a high energy density. A main obstacle to its application is the poor interface contact between the solid electrodes and the ceramic electrolyte. Surface treatment methods have been proposed to improve the interface of the ceramic electrolytes, but they are generally limited to low‐capacity or short‐term cycling. Herein, an electron/ion dual‐conductive solid framework is proposed by partially dealloying the Li–Mg alloy anode on a garnet‐type solid‐state electrolyte. The Li–Mg alloy framework serves as a solid electron/ion dual‐conductive Li host during cell cycling, in which the Li metal can cycle as a Li‐rich or Li‐deficient alloy anode, free from interface deterioration or volume collapse. Thus, the capacity, current density, and cycle life of the solid Li anode are improved. The cycle capability of this solid anode is demonstrated by cycling for 500 h at 1 mA cm −2 , followed by another 500 h at 2 mA cm −2 without short‐circuiting, realizing a record high cumulative capacity of 750 mA h cm −2 for garnet‐type all‐solid‐state Li batteries. This alloy framework with electron/ion dual‐conductive pathways creates the possibility to realize high‐energy solid‐state Li batteries with extended lifespans.
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