A Bilayer Electrolyte Design to Enable High-Areal-Capacity Composite Cathodes in Polymer Electrolytes Based Solid-State Lithium Metal Batteries

Journal Article · 08 February 2022 · ACS Applied Energy Materials

DOI: https://doi.org/10.1021/acsaem.2c00050 · OSTI ID:1847517

Sahore, Ritu  ^[1]; Yang, Guang  ^[1]; Chen, Xi Chelsea  ^[1]; Tsai, Wan-Yu  ^[1]; Li, Jianlin  ^[1]; Dudney, Nancy J.  ^[1]; Westover, Andrew  ^[1]

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1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

High-areal-capacity cathodes are needed for energy-dense solid-state batteries. Here, we demonstrate a bilayer polymer electrolyte design for cycling 3–6 mAh/cm² NMC811 composite cathodes. In this work, the bilayer electrolyte comprises a cross-linked poly(ethylene oxide) (PEO)-based electrolyte layer and a linear-PEO-based electrolyte layer. The former provides dendritic resistance, and the latter provides a seamless interface with the cathode during cycling. Using a single layer of either membrane led to severe shorting or extremely low Coulombic efficiency (CE) in the first cycle. The general concept of a rigid dendrites-inhibiting electrolyte facing Li anode and a softer, cathode-integrated electrolyte that ensures contact with the cathodes during cycling may present a pattern for enabling high-energy-density cathodes.

• Research Organization: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
• Sponsoring Organization: USDOE Laboratory Directed Research and Development (LDRD) Program
• Grant/Contract Number: AC05-00OR22725
• OSTI ID: 1847517
• Journal Information: ACS Applied Energy Materials, Journal Name: ACS Applied Energy Materials Journal Issue: 2 Vol. 5; ISSN 2574-0962
• Publisher: American Chemical Society (ACS)Copyright Statement
• Country of Publication: United States
• Language: English