Formulating the Electrolyte Towards High-Energy and Safe Rechargeable Lithium-Metal Batteries

Angew Chem Int Ed Engl. 2021 Jul 19;60(30):16554-16560. doi: 10.1002/anie.202103850. Epub 2021 Jun 15.

Abstract

Rechargeable lithium-metal batteries with a cell-level specific energy of >400 Wh kg-1 are highly desired for next-generation storage applications, yet the research has been retarded by poor electrolyte-electrode compatibility and rigorous safety concerns. We demonstrate that by simply formulating the composition of conventional electrolytes, a hybrid electrolyte was constructed to ensure high (electro)chemical and thermal stability with both the Li-metal anode and the nickel-rich layered oxide cathodes. By employing the new electrolyte, Li∥LiNi0.6 Co0.2 Mn0.2 O2 cells show favorable cycling and rate performance, and a 10 Ah Li∥LiNi0.8 Co0.1 Mn0.1 O2 pouch cell demonstrates a practical specific energy of >450 Wh kg-1 . Our findings shed light on reasonable design principles for electrolyte and electrode/electrolyte interfaces toward practical realization of high-energy rechargeable batteries.

Keywords: hybrid electrolytes; in situ polymerization; interfacial chemistry; rechargeable lithium-metal batteries.