Issue 24, 2025

Multifunctional ion-conductive polymer coatings for high-performance sulfide solid-state batteries with Ni-rich cathodes

Abstract

Sulfide-based solid-state batteries (SSBs) are emerging as a top contender for next-generation rechargeable batteries with improved safety and higher energy densities. However, SSBs with Ni-rich cathode materials such as LiNi0.82Mn0.07Co0.11O2 (NMC82) exhibit several chemomechanical challenges at the cathode–electrolyte interface, such as contact loss and solid-electrolyte decomposition, resulting in poor interfacial Li+ ion transport. To overcome these challenges, we used polymerized ionic liquids (PIL) as coatings at the NMC82 cathode surface, with and without incorporating a lithium salt. The thin Li+ ion-conductive Li–PIL nanocoating shows excellent compatibility with sulfide solid electrolytes and enables efficient Li+ transfer over the cathode–solid electrolyte interface, as demonstrated by 2D solid-state exchange NMR. It also improves contact retention between the cathode–solid electrolyte particles and mitigates electrolyte oxidation-induced degradation. This is reflected in the electrochemical performance of coated NMC82 in sulfide SSBs, where both a higher rate performance (190 mA h g−1vs. 163 mA h g−1 for uncoated at 0.1C) and a remarkable capacity retention of 82.7% after 500 cycles at 0.2C and ambient conditions (20 °C) are observed. These results emphasize the effectiveness of PILs with Li salts as multifunctional coatings that enable high-performance sulfide-based SSBs with Ni-rich cathode materials at ambient temperature.

Graphical abstract: Multifunctional ion-conductive polymer coatings for high-performance sulfide solid-state batteries with Ni-rich cathodes

Supplementary files

Article information

Article type
Paper
Submitted
05 Mar 2025
Accepted
13 May 2025
First published
13 May 2025
This article is Open Access
Creative Commons BY license

J. Mater. Chem. A, 2025,13, 18518-18531

Multifunctional ion-conductive polymer coatings for high-performance sulfide solid-state batteries with Ni-rich cathodes

P. Karanth, J. H. Prins, A. Gautam, Z. Cheng, J. Canals-Riclot, S. Ganapathy, P. Ombrini, A. Ladam, S. Fantini, M. Wagemaker and F. M. Mulder, J. Mater. Chem. A, 2025, 13, 18518 DOI: 10.1039/D5TA01827G

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