High-performance Li/LiNi0.8Co0.1Mn0.1O2 batteries enabled by optimizing carbonate-based electrolyte and electrode interphases via triallylamine additive

Lithium (Li) metal batteries (LMBs), paired with high-energy-density cathode materials, are promising to meet the ever-increasing demand for electric energy storage. Unfortunately, the inferior electrode-electrolyte interfaces and hydrogen fluoride (HF) corrosion in the state-of-art carbonate-based electrolytes lead to dendritic Li growth and unsatisfactory cyclability of LMBs. Herein, a multifunctional electrolyte additive triallylamine (TAA) is proposed to circumvent those issues. The TAA molecule exhibits strong nucleophilicity and contains three unsaturated carbon-carbon double bonds, the former for HF elimination, the later for in-situ passivation of aggressive electrodes. As evidenced theoretically and experimentally, the preferential oxidation and reduction of carbon-carbon double bonds enable the successful regulation of components and morphologies of electrode interfaces, as well as the binding affinity to HF effectively blocks HF corrosion. In particular, the TAA-derived electrode interfaces are packed with abundant lithium-containing inorganics and oligomers, which diminishes undesired parasitic reactions of electrolyte and detrimental degradation of electrode materials. When using the TAA-containing electrolyte, the cell configuration with Li anode and nickel-rich layered oxide cathode and symmetrical Li cell deliver remarkably enhanced electrochemical performance with regard to the additive-free cell. The TAA additive shows great potential in advancing the development of carbonate-based electrolytes in LMBs.