Superconcentrated electrolytes for a high-voltage lithium-ion battery

Abstract

Finding a viable electrolyte for next-generation 5 V-class lithium-ion batteries is of primary importance. A long-standing obstacle has been metal-ion dissolution at high voltages. The LiPF ₆ salt in conventional electrolytes is chemically unstable, which accelerates transition metal dissolution of the electrode material, yet beneficially suppresses oxidative dissolution of the aluminium current collector; replacing LiPF ₆ with more stable lithium salts may diminish transition metal dissolution but unfortunately encounters severe aluminium oxidation. Here we report an electrolyte design that can solve this dilemma. By mixing a stable lithium salt LiN(SO ₂F) ₂ with dimethyl carbonate solvent at extremely high concentrations, we obtain an unusual liquid showing a three-dimensional network of anions and solvent molecules that coordinate strongly to Li ⁺ ions. This simple formulation of superconcentrated LiN(SO ₂F) ₂/dimethyl carbonate electrolyte inhibits the dissolution of both aluminium and transition metal at around 5 V, and realizes a high-voltage LiNi _0.5Mn _1.5O ₄/graphite battery that exhibits excellent cycling durability, high rate capability and enhanced safety.

Abstract

Electrode degradation due to metal-ion dissolution in conventional electrolyte hampers the performance of 5 V-class lithium ion batteries. Here, the authors employ a high concentration electrolyte to inhibit metal-ion dissolution and realize a stable high voltage LiNi _0.5Mn _1.5O ₄/graphite battery.