Polymer-based solid-state electrolytes are shown to be highly promising for realizing low-cost, high-capacity, and safe Li batteries. One major challenge for polymer solid-state batteries is the relatively high operating temperature (60-80°C), which means operating such batteries will require significant ramp up time due to heating. On the other hand, as polymer electrolytes are poor thermal conductors, thermal variation across the polymer electrolyte can lead to nonuniformity in ionic conductivity. This can be highly detrimental to lithium deposition and may result in dendrite formation. Here, a polyethylene oxide-based electrolyte with improved thermal responses is developed by incorporating 2D boron nitride (BN) nanoflakes. The results show that the BN additive also enhances ionic and mechanical properties of the electrolyte. More uniform Li stripping/deposition and reversible cathode reactions are achieved, which in turn enable all-solid-state lithium-sulfur cells with superior performances.

An all-solid-state lithium–sulfur battery (ASSLSB) is a promising candidate for post-Li-ion battery technologies with high energy densities and good safety performance. However, the intrinsic insulating nature of sulfur requires triple-phase contact with an ionic conductor and an electronic conductor for electrochemical reactions, which decreases the amount of active surface and lowers the charge-transfer efficiency. In this work, a double-phase interface constructed from a mixed ionic/electronic conductor is proposed to enhance the solid-state electrochemical reaction of sulfur. By employing lithium lanthanum titanium oxide/carbon (LLTO/C) nanofibers with mixed ionic/electronic conductivity, enhanced charge-transfer behavior is realized at the sulfur–LLTO/C double-phase interface, compared to the traditional triple-phase interface. As a result, high sulfur utilization and excellent rate performance are achieved. And the facilitated charge transfer shows great potential to lower the operating temperature and improve the sulfur content for practical applications of ASSLSBs. Cycle performance is also enhanced due to the suppressed shuttle effect of polysulfides by the incorporation of the LLTO/C nanofibers.

The sluggish conversion reaction of sulfur and poor interfacial contact restrict electrochemical performance and practical application of all-solid-state Li–S batteries. Herein, we present a rational design of cell structure with a cathode-supported-electrolyte configuration to attain high-performance all-solid-state Li–S batteries. A mechanically robust sulfur cathode was constructed, and a slurry-based polymer electrolyte layer was subsequently cast on the cathode to form an intimate interfacial contact. The resulting battery shows a high specific capacity and good cycle performance. As a proof-of-concept, full cells with variable configurations, excellent flexibility, and safety features are demonstrated.

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