Enabling High-Performance Hybrid Solid-State Batteries by Improving the Microstructure of Free-Standing LATP/LFP Composite Cathodes
Martin Ihrig, Enkhtsetseg Dashjav, Philipp Odenwald, Christian Dellen, Daniel Grüner, Jürgen Peter Gross, Thi Tuyet Hanh Nguyen, Yu-Hsing Lin, Walter Sebastian Scheld, Changhee Lee, Ruth Schwaiger, Abdelfattah Mahmoud, Jürgen Malzbender, Olivier Guillon, Sven Uhlenbruck, Martin Finsterbusch, Frank Tietz, Hsisheng Teng, Dina Fattakhova‐Rohlfing
Abstract
High Resolution Image Download MS PowerPoint Slide The phosphate lithium-ion conductor Li 1.5 Al 0.5 Ti 1.5 (PO 4 ) 3 (LATP) is an economically attractive solid electrolyte for the fabrication of safe and robust solid-state batteries, but high sintering temperatures pose a material engineering challenge for the fabrication of cell components. In particular, the high surface roughness of composite cathodes resulting from enhanced crystal growth is detrimental to their integration into cells with practical energy density. In this work, we demonstrate that efficient free-standing ceramic cathodes of LATP and LiFePO 4 (LFP) can be produced by using a scalable tape casting process. This is achieved by adding 5 wt % of Li 2 WO 4 (LWO) to the casting slurry and optimizing the fabrication process. LWO lowers the sintering temperature without affecting the phase composition of the materials, resulting in mechanically stable, electronically conductive, and free-standing cathodes with a smooth, homogeneous surface. The optimized cathode microstructure enables the deposition of a thin polymer separator attached to the Li metal anode to produce a cell with good volumetric and gravimetric energy densities of 289 Wh dm –3 and 180 Wh kg –1, respectively, on the cell level and Coulombic efficiency above 99% after 30 cycles at 30 °C.