Co-Intercalation-Free Graphite Anode Enabled by an Additive Regulated Interphase in an Ether-Based Electrolyte for Low-Temperature Lithium-Ion Batteries

ACS Appl Mater Interfaces. 2024 Feb 28;16(8):10116-10125. doi: 10.1021/acsami.3c17844. Epub 2024 Feb 21.

Abstract

Graphite (Gr) anode, which is endowed with high electronic conductivity and low volume expansion after Li-ion intercalation, establishes the basis for the success of rocking-chair Li-ion batteries (LIBs). However, due to the high barrier of the Li-ion desolvation process, sluggish transport of Li ions through the solid electrolyte interphase (SEI) and the high freezing points of electrolytes, the Gr anode still suffers from great loss of capacity and severe polarization at low temperature. Here, 1,2-diethoxyethane (DEE) with an intrinsically wide liquid region and weak solvation ability is applied as an electrolyte solvent for LIBs. By rationally designing the additives of electrolytes, an intact SEI with fast Li-ion conductivity is constructed, enabling the co-intercalation-free Gr anode with long-term stability (91.8% after 500 cycles) and impressive low-temperature characteristics (82.6% capacity retention at -20 °C). Coupled with LiFePO4 and LiNi0.8Mn0.1Co0.1O2 cathodes, the optimized electrolyte also demonstrates low polarization under -20 °C. Our work offers a feasible approach to enable ether-based electrolytes for low-temperature LIBs.

Keywords: ether-based electrolyte; graphite anode; interphase design; lithium-ion batteries; low temperature.