Identification of Potential Electrolyte Additives via Density Functional Theory Analysis

Abstract With the ongoing progress in updating electrode materials and electrolyte components, the performance of lithium‐ion batteries (LIBs) has been greatly improved in the past decades. Specifically, density functional theory (DFT) calculations have emerged as a convenient and reliable strategy, especially to comprehend the origin for the improved electrochemical performances induced by certain reagent. Herein, DFT calculations have been utilized to analyze the plausibility of electrolyte additives for six groups of heterocyclic molecules (including N‐, O‐, S‐, N,O‐, S,N/O‐containing cyclic structures, and other cyclic ones, with 110 molecules in total). VC was used as the reference, as we aim to develop the additives with higher reductivity and high‐voltage stability etc . than that of VC. With the filter of LUMO, HOMO, HOMO‐LUMO gap, and Li + binding energies, 6 molecules were finally screened out. The synthesis of one sulfate‐containing structure (i. e. 85 ) and its improved electrochemical performance of LIBs supports the theoretical prediction.