A jigsaw-structured artificial solid electrolyte interphase for high-voltage lithium metal batteries

Lithium-metal batteries are hindered by their insufficient Coulombic efficiency and uncontrollable dendrite growth. Here, a multi-component jigsaw-like artificial solid electrolyte interphase was constructed that regulates lithium-ion transport and protects the reactive lithium metal. The practical application of lithium-metal batteries is hindered by insufficient lithium Coulombic efficiency and uncontrolled dendrite growth, bringing a challenge concerning how to create robust solid electrolyte interphases (SEIs) that can regulate Li+ transport and protect reactive lithium-metal. Here, we present the rational construction of a multi-component jigsaw-like artificial SEI by the integration of fluorine-containing silane and polyether-containing silane. The fluorine-donating group prevents the parasitic reaction and yields a dense structure for homogeneous lithium deposition. Additionally, the lithophilicity of ethylene glycol backbone facilitates the rapid transport of Li+ and the cross-linked network increases mechanical robustness of the SEI. With this artificial SEI, we show highly reversible lithium plating and stripping cycling for more than 500 hours. Moreover, we also demonstrate stable operation of high-voltage LiNi0.8Co0.1Mn0.1O2 cathode in both coin and pouch cells under high loading, limiting excess lithium, and lean electrolyte conditions, holding great prospects for the practical application of high-voltage lithium-metal batteries.