Bi‐affinity Electrolyte Optimizing High‐Voltage Lithium‐Rich Manganese Oxide Battery via Interface Modulation Strategy

The practical implementation of high-voltage lithium-rich manganese oxide (LRMO) cathode is limited by the formation of dendrites, unanticipated electrolyte decomposition, and dissolution of transition metal ions. The present study proposes a bi-affinity electrolyte formulation, wherein the sulfonyl group of ethyl vinyl sulfone (EVS) imparts a highly adsorptive nature to LRMO, while fluoroethylene carbonate (FEC) exhibits a reductive nature towards Li metal. This interface modulation strategy involves the synergistic use of EVS and FEC as additives to form robust interphase layers on the electrode. As-formed S-endorsed but LiF-assisted configuration cathode electrolyte interphase with a more dominant -SO2- component may promote the interface transport kinetics and prevent the dissolution of transition metal ions. Furthermore, the incorporation of S component into the solid electrolyte interphase and the reduction of its poorly conducting component can effectively inhibit the growth of lithium dendrites. Therefore, a 4.8 V LRMO/Li cell with optimized electrolyte may demonstrate a remarkable retention capacity of 97% even after undergoing 300 cycles at 1 C.