Artificially regulated interphase on natural graphite realizes rapid charge and durable high-temperature cycling of Li-ion batteries

Abstract

Natural graphite (NG) is a strong competitor in the anode market of Li-ion batteries because of its low cost, rich resource, low energy consumption and low carbon dioxide emission during production. The main problems inhibiting its universal application are its high surface area and the attendant unstable solid/electrolyte interphase (SEI), leading to unsatisfactory cycling and rate performance. In this work, a Li+-conductive, thermally and mechanically stable organic polymer layer is successfully constructed on NG surface by virtue of the simultaneous polymerization and crosslinking reactions of chitosan (CS) and acrylic acid (AA). With controllable thickness, the polymer layer denoted as CSAA significantly decreases the specific surface area of NG, works as an inner SEI substrate greatly mitigating the decomposition of electrolyte, and induces the formation of a LiF-rich SEI outer layer. The SEI resistance and activation energy for charge-transfer reactions are considerably reduced. Benefiting from the superior properties of CSAA-derived SEI, the NG@CSAA anodes exhibit a high initial coulombic efficiency of 94.1 %, fast charge/discharge capability and prolonged cycle life at both 25 °C and 45 °C in the LiFePO4 cathodes-based full cells.