Rapid Thermal Shutdown of Deep‐Eutectic‐Polymer Electrolyte Enabling Overheating Self‐Protection of Lithium Metal Batteries

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Safety concerns and uncontrollable dendrite growths have severely impeded the advancement of lithium-metal batteries. Herein, a safe deep-eutectic-polymer electrolyte with built-in thermal shutdown capability is proposed by utilizing hydrophobic association of methylcellulose within a novel deep-eutectic-solvent. Specifically, at elevated temperatures, methylcellulose chains aggregate to form dense polymer networks due to hydrophobic association and break the solvation structure equilibrium inside the deep-eutectic system through encapsulating Li⁺ in polymer matrix, leading to quick solidification of the electrolyte. The solidified electrolyte obstructs Li⁺ transports and terminates electrochemical processes, protecting LMBs from unstoppable exothermic chain reactions. The accelerating rate calorimeter tests of 1 Ah pouch cells demonstrate that the as-prepared electrolyte significantly improves the onset self-heating temperature from 73 °C for conventional electrolytes to 172 °C and prolongs the thermal runaway waiting time more than 20 hours. More impressively, benefiting from its favorable electrochemical performance, this polymer electrolyte enables LiNi0.8Mn0.1Co0.1O₂||Li batteries to retain 92% capacity over 200 cycles and LiFePO₄||Li batteries to maintain 90% capacity after 500 cycles. This research paves a promising avenue for enhancing both the safety and electrochemical performance of high-energy-density LMBs.