Dual-Salt Electrolytes to Effectively Reduce Impedance Rise of High-Nickel Lithium-Ion Batteries

ACS Appl Mater Interfaces. 2021 Sep 1;13(34):40502-40512. doi: 10.1021/acsami.1c08478. Epub 2021 Aug 20.

Abstract

Simply mixing several lithium salts in one electrolyte to obtain blended salt electrolytes has been demonstrated as a promising strategy to formulate advanced electrolytes for lithium metal batteries (LMBs) and lithium-ion batteries (LIBs). In this study, we report the use of dual-salt electrolytes containing lithium hexafluorophosphate (LiPF6) and lithium difluorophosphate (LiDFP) in ethylene carbonate/ethyl methyl carbonate (EC/EMC) mixture and tested them in layered high-nickel LIB cells. LiNi0.94Co0.06O2 was synthesized through a coprecipitation method and was used as a representative high-nickel cathode for the U.S. DOE realizing next-generation cathode (RNGC) deep dive program. The ionic conductivity of dual-salt electrolytes can be maintained by controlling the amount of LiDFP. Techniques including 1H Nuclear Magnetic Resonance (NMR), X-ray photoelectron spectroscopy (XPS), inductively coupled plasma-mass spectrometry (ICP-MS), and differential voltage analysis (DVA) were used to understand the improved performance. The multifaceted benefits of using the dual-salt electrolytes include (1) reduced transesterification, (2) formation of a stable cathode electrolyte interface, and (3) mitigation of cathode degradation at high voltages, especially stabilization of oxide particles during the H2 ↔ H3 transformation.

Keywords: dual-salt electrolytes; high-nickel lithium-ion batteries; impedance rise; ionic conductivity; transesterification and transition-metal dissolution.