Department of Mechanical Engineering, The Pennsylvania State University, University Park, PA, 16802, USA.
Department of Chemical Engineering, The Pennsylvania State University, University Park, PA, 16802, USA.
Nat Commun. 2023 Apr 5;14(1):1895. doi: 10.1038/s41467-023-37564-z.
Lithium-sulfur all-solid-state batteries using inorganic solid-state electrolytes are considered promising electrochemical energy storage technologies. However, developing positive electrodes with high sulfur content, adequate sulfur utilization, and high mass loading is challenging. Here, to address these concerns, we propose using a liquid-phase-synthesized LiPS-2LiBH glass-ceramic solid electrolyte with a low density (1.491 g cm), small primary particle size (~500 nm) and bulk ionic conductivity of 6.0 mS cm at 25 °C for fabricating lithium-sulfur all-solid-state batteries. When tested in a Swagelok cell configuration with a Li-In negative electrode and a 60 wt% S positive electrode applying an average stack pressure of ~55 MPa, the all-solid-state battery delivered a high discharge capacity of about 1144.6 mAh g at 167.5 mA g and 60 °C. We further demonstrate that the use of the low-density solid electrolyte increases the electrolyte volume ratio in the cathode, reduces inactive bulky sulfur, and improves the content uniformity of the sulfur-based positive electrode, thus providing sufficient ion conduction pathways for battery performance improvement.
使用无机固态电解质的锂硫全固态电池被认为是很有前途的电化学储能技术。然而，开发具有高硫含量、充分利用硫和高质量负载的正极是具有挑战性的。在这里，为了解决这些问题，我们提出使用液相合成的 LiPS-2LiBH 玻璃陶瓷固体电解质，其具有低密度（1.491 g/cm）、小初级粒径（~500nm）和室温下 6.0 mS cm 的体离子电导率，用于制造锂硫全固态电池。当在 Swagelok 电池配置中进行测试时，采用 Li-In 负电极和 60wt% S 正电极，施加平均堆叠压力约为 55 MPa，全固态电池在 167.5 mA g 和 60°C 下提供约 1144.6 mAh g 的高放电容量。我们进一步证明，使用低密度固体电解质增加了正极中电解质的体积比，减少了不活跃的大块硫，并提高了基于硫的正极的含量均匀性，从而为提高电池性能提供了足够的离子传导途径。
