Zeolite Coated Separators for Improved Performance and Safety of Lithium Metal Batteries

Abstract

Lithium (Li) metal batteries are attractive due to their high gravimetric and volumetric energy densities. However, they can fail catastrophically due to dendritic nucleation, growth, and penetration through the polypropylene (PP) or polyethylene (PE) separators. Poor electrolyte wetting and non-uniform Li ion flux are known to affect Li dendrite formation, especially since the PP/PE separators have non-uniform pore size distribution and typical organic electrolytes do not wet them well. In this work, we demonstrate that a porous zeolite coating on a commercial PP separator can improve electrolyte wettability and through plane ionic conductivity, giving rise to more uniform Li flux. Consequently, coated separator can delay dendrite penetration and enhance cell performance and safety. We tested Celgard 2400 (uncoated) and zeolite-coated separator (coated) in high energy NMC||Li cells for their rate capability and cycle life performance. Rate capability test for these cells shows that the additional resistance due to the zeolite coating can negatively impact the cell performance at high C-rates. However, cells with the coated separator outperform those with uncoated separator in the cycle life test with improved capacity retention. Symmetric cell studies performed to understand the differences in Li plating morphology indicate initial lower overpotential for the coated separator cells, revealing improved electrolyte wetting and relatively uniform Li flux. Scanning electron microscopy (SEM) reveals zeolite-coating microstructure with evenly distributed zeolite particles and cycled Li metal electrode morphologies. SEM images show much smoother Li plating morphology on Li metal surface in the cells with coated separators. This study highlights the potential of using zeolite-coated separators to enhance lithium metal battery (LMB) performance and safety.