All-solid-state lithium sulfur batteries (ASLSB) have many advantages over liquid electrolyte-based lithium sulfur batteries such as high sulfur utilization, low electrolyte-to-sulfur ratio and low self-discharge. However, the kinetics of all-solid-state sulfur cathodes is not well understood, which is critical to achieve their full potential. In this work, we determine the contributions of different processes to the overall kinetics of sulfur electrodes using Electrochemical Impedance Spectroscopy (EIS) and Gravimetric Intermittent Titration Technique (GITT). We show that the impedance of sulfur electrodes can be well described by the Transmission Line Model (TLM). It is found that the kinetics of the sulfur electrode is determined primarily by ionic migration at the electrode level and diffusion within the sulfur active materials. Based on this understanding, we compared kinetics of sulfur electrodes with different solid electrolytes and mixing methods. Electrodes using amorphous sulfide solid electrolyte and impregnated S/C composites display the best kinetics. ASLSB possess high capacities at moderate rates at room temperature, and can operate even at 120 °C. Combined with the negligible self-discharge over a year, we believe that ASLSB is a promising candidate for as high-energy primary batteries.

与基于液体电解质的锂硫电池相比，全固态锂硫电池（ASLSB）具有许多优势，例如硫利用率高，电解质硫比低和自放电率低。但是，对全固态硫阴极的动力学还没有很好的了解，这对于实现其全部潜力至关重要。在这项工作中，我们使用电化学阻抗谱（EIS）和重力间歇滴定技术（GITT）确定了不同过程对硫电极整体动力学的贡献。我们表明，硫电极的阻抗可以通过传输线模型（TLM）很好地描述。发现硫电极的动力学主要由电极水平上的离子迁移和硫活性材料内的扩散决定。基于这种理解，我们比较了具有不同固体电解质和混合方法的硫电极的动力学。使用非晶态硫化物固体电解质和浸渍的S / C复合材料的电极表现出最佳的动力学性能。ASLSB在室温下具有中等速率的高容量，甚至可以在120°C下运行。结合一年以来微不足道的自放电，我们认为ASLSB是高能一次电池的有前途的候选者。