School of Materials Science and Engineering, Georgia Institute of Technology , Atlanta, Georgia 30332, United States.
School of Metallurgy and Environment, Central South University , Changsha, 410083, P.R. China.
ACS Nano. 2016 Jan 26;10(1):1333-40. doi: 10.1021/acsnano.5b06716. Epub 2015 Dec 14.
Lithium sulfide (Li2S) with a high theoretical specific capacity of 1166mAh g(-1) is a promising cathode material for next-generation Li-S batteries with high specific energy. However, low conductivity of Li2S and polysulfide dissolution during cycling are known to limit the rate performance and cycle life of these batteries. Here, we report on the successful development and application of a nanocomposite cathode comprising graphene covered by Li2S nanoparticles and protected from undesirable interactions with electrolytes. We used a modification of our previously reported low cost, scalable, and high-throughput solution-based method to deposit Li2S on graphene. A dropwise infiltration allowed us to keep the size of the heterogeneously nucleated Li2S particles smaller and more uniform than what we previously achieved. This, in turn, increased capacity utilization and contributed to improved rate performance and stability. The use of a highly conductive graphene backbone further increased cell rate performance. A synergetic combination of a protective layer vapor-deposited on the material during synthesis and in situ formed protective surface layer allowed us to retain ∼97% of the initial capacity of ∼1040 mAh gs(-1) at C/2 after over 700 cycles in the assembled cells. The achieved combination of high rate performance and ultrahigh stability is very promising.
硫化锂(Li2S)具有 1166mAh g(-1) 的高理论比容量,是下一代具有高比能量的锂硫电池的有前途的阴极材料。然而,Li2S 的导电性低和多硫化物在循环过程中的溶解,已知会限制这些电池的倍率性能和循环寿命。在这里,我们报告了一种由石墨烯覆盖的 Li2S 纳米粒子组成的纳米复合材料阴极的成功开发和应用,该阴极可防止与电解质发生不良相互作用。我们使用了我们之前报道的低成本、可扩展和高通量的基于溶液的方法的改进版本,将 Li2S 沉积在石墨烯上。滴注允许我们使异质成核的 Li2S 颗粒的尺寸更小且更均匀,这比我们之前的方法要好。这反过来又提高了容量利用率,并有助于提高倍率性能和稳定性。高导电性石墨烯骨架的使用进一步提高了电池的倍率性能。在合成过程中在材料上蒸镀的保护层和原位形成的保护层的协同组合使我们能够在组装好的电池中经过 700 多次循环后,在 C/2 时保留约 97%的初始容量,约为 1040 mAh gs(-1)。实现的高倍率性能和超高稳定性的组合非常有前景。