• Bresser, Dominic
• Zarrabeitia, Maider
• Chen, Zhen
• Liang, Haipeng
• Merz, Steffen
• Jovanovic, Sven
• Granwehr, Josef
• Passerini, Stefano

Abstract

<jats:title>Abstract</jats:title><jats:p>Single‐ion conducting polymer electrolytes are considered particularly attractive for realizing high‐performance solid‐state lithium‐metal batteries. Herein, a polysiloxane‐based single‐ion conductor (PSiO) is investigated. The synthesis is performed via a simple thiol‐ene reaction, yielding flexible and self‐standing polymer electrolyte membranes (PSiOM) when blended with poly(vinylidene fluoride‐<jats:italic>co</jats:italic>‐hexafluoropropylene) (PVdF‐HFP). When incorporating 57 wt% of organic carbonates, these polymer membranes provide a Li<jats:sup>+</jats:sup> conductivity of &gt;0.4 mS cm<jats:sup>−1</jats:sup> at 20 °C and a wide electrochemical stability window of more than 4.8 V. This excellent electrochemical stability allows for the highly reversible cycling of symmetric Li||Li cells as well as high‐energy Li||LiNi<jats:sub>0.6</jats:sub>Mn<jats:sub>0.2</jats:sub>Co<jats:sub>0.2</jats:sub>O<jats:sub>2</jats:sub> (NMC<jats:sub>622</jats:sub>) and Li||LiNi<jats:sub>0.8</jats:sub>Mn<jats:sub>0.1</jats:sub>Co<jats:sub>0.1</jats:sub>O<jats:sub>2</jats:sub> (NMC<jats:sub>811</jats:sub>) cells for several hundred cycles at relatively high discharge and charge rates. Remarkably, Li||NMC<jats:sub>811</jats:sub> cells with high mass loading cathodes provide more than 76% capacity retention at a high current density of 1.44 mA cm<jats:sup>−2</jats:sup>, thus rendering this polymer electrolyte suitable for high‐performance battery applications.</jats:p>

Topics

• density
• impedance spectroscopy
• mass spectrometry
• Lithium
• current density
• polymer blend