Anion-enrichment interface enables high-voltage anode-free lithium metal batteries

Aggressive chemistry involving Li metal anode (LMA) and high-voltage LiNi0.8Mn0.1Co0.1O2 (NCM811) cathode is deemed as a pragmatic approach to pursue the desperate 400 Wh kg(-1). Yet, their implementation is plagued by low Coulombic efficiency and inferior cycling stability. Herein, we propose an optimally fluorinated linear carboxylic ester (ethyl 3,3,3-trifluoropropanoate, FEP) paired with weakly solvating fluoroethylene carbonate and dissociated lithium salts (LiBF4 and LiDFOB) to prepare a weakly solvating and dissociated electrolyte. An anion-enrichment interface prompts more anions' decomposition in the inner Helmholtz plane and higher reduction potential of anions. Consequently, the anion-derived interface chemistry contributes to the compact and columnar-structure Li deposits with a high CE of 98.7% and stable cycling of 4.6 V NCM811 and LiCoO2 cathode. Accordingly, industrial anode-free pouch cells under harsh testing conditions deliver a high energy of 442.5 Wh kg(-1) with 80% capacity retention after 100 cycles. The implementation of Li metal anode with high-voltage Ni/Co rich cathode is plagued by low coulombic efficiency and inferior cycling stability. Here authors propose an anion-enriched interface to facilitate the columnar-structure of Li deposits to solve this issue.

Automated summary

The authors propose an anion-enriched interface to facilitate the columnar-structure of Li deposits, solving the issue of low coulombic efficiency and inferior cycling stability between the Li metal anode and high-voltage Ni/Co rich cathode.