Multifunctional ion-conductive polymer coatings for high-performance sulfide solid-state batteries with Ni-rich cathodes
Pranav Karanth (TU Delft - ChemE/Materials for Energy Conversion and Storage, TU Delft - RST/Storage of Electrochemical Energy)
J.H. Prins (Student TU Delft)
A. Gautam (TU Delft - RST/Storage of Electrochemical Energy)
Zhu Cheng (TU Delft - RST/Storage of Electrochemical Energy)
Jef Canals (TU Delft - RST/Storage of Electrochemical Energy)
Swapna Ganapathy (TU Delft - RID/TS/Instrumenten groep, TU Delft - RST/Storage of Electrochemical Energy)
P. Ombrini (TU Delft - RST/Storage of Electrochemical Energy)
M Wagemaker (TU Delft - RST/Storage of Electrochemical Energy)
Fokko Mulder (TU Delft - ChemE/Materials for Energy Conversion and Storage)
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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−1 vs. 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.
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