Revealing the Na storage behavior of graphite anodes in low-concentration imidazole-based electrolytes

Abstract

The thermodynamic instability of Na⁺-intercalated compounds is an important factor limiting the application of graphite anodes in sodium-ion batteries. Although solvent co-intercalation is recognized as a simple and effective strategy, the challenge lies in the lack of durable electrolytes. Herein, we successfully apply low-concentration imidazole-based electrolytes to graphite anodes for sodium-ion batteries. Specifically, low concentrations ensure high ionic conductivity while saving on costs. Methylimidazole molecules can be co-intercalated with Na⁺, and a small amount of unreleased solvated Na⁺ serves the dual purpose of providing support to the graphite layer and preventing peeling off. The interphase formed in imidazole is more uniform and dense compared with that in ether electrolytes, which reduces side reactions and the risk of internal short circuits. The obtained battery demonstrates a long cycle life of 1800 cycles with a capacity retention of 84.6%. This success extends to other imidazole-based solvents such as 1-propylimidazole and 1-butylimidazole.