High-rate lithium cycling in a scalable trilayer Li-garnet-electrolyte architecture

Gregory T. Hitz, Dennis W. McOwen, Lei Zhang, Zhaohui Ma, Zhezhen Fu, Yang Wen, Yunhui Gong, Jiaqi Dai, Tanner R. Hamann, Liangbing Hu, Eric D. Wachsman

Research output: Contribution to journalArticlepeer-review

235 Scopus citations


Solid-state lithium batteries promise to exceed the capabilities of traditional Li-ion batteries in safety and performance. However, a number of obstacles have stood in the path of solid-state battery development, primarily high resistance and low capacity. In this work, these barriers are overcome through the fabrication of a uniquely microstructured solid electrolyte architecture based on a doped Li 7 La 3 Zr 2 O 12 (LLZ) ceramic Li-conductor. Specifically, a porous-dense-porous trilayer structure was fabricated by tape casting, a scalable roll-to-roll manufacturing technique. The dense (>99%) center layer can be fabricated as thin as ∼10 μm and blocks dendrites over hundreds of cycles. The microstructured porous layers serve as electrode supports and increase the mechanical strength by ∼9× making the cells strong enough to handle with ease. Additionally, the porous layers multiply the electrode–electrolyte interfacial surface area by >40× compared to a typical planar interface. Lithium symmetric cells based on the trilayer architecture were cycled at room temperature and achieved area-specific resistances (∼7 Ω-cm 2 ) dramatically lower, and current densities dramatically higher (10 mA/cm 2 ), than previously reported literature results. Moreover, to demonstrate scalability a large-format cell was fabricated with lithium metal in one porous layer and a sulfur electrode with conductive carbon and an ionic liquid interface in the other, achieving 1244 mAh/g S utilization and 195 Wh/kg based on total cell mass, showing a promising path to commercially viable, intrinsically safe lithium batteries with high specific energy and high energy density.

Original languageEnglish (US)
Pages (from-to)50-57
Number of pages8
JournalMaterials Today
StatePublished - Jan 1 2019

All Science Journal Classification (ASJC) codes

  • General Materials Science
  • Condensed Matter Physics
  • Mechanics of Materials
  • Mechanical Engineering


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