A Novel Multi-Functional Electrolyte Additive for Ni-Rich Cathode Materials

Abstract

Ni-rich layer oxides Li[Ni x CoyMn1−x−y ]O2 (x ≥ 0.8, NCMs) are promising advanced cathode materials for high-energy Li-ion batteries because of their high specific capacity (≥ 200 mAh g−1) with an average discharge voltage of 3.8 V vs Li+/Li, as compared to the commercialized cathode materials (e.g. LiCoO2, LiFePO4).1 However, the instability of cathode–electrolyte interface causes the structural degradation of cathode active material and the electrolyte consumption, as well as gas evolution due to oxidative decomposition of electrolyte, resulting in a rapid capacity fading.2 Thus, improvement in the stability of cathode–electrolyte interphase is a key requirement to inhibit their structural degradation and enhance their electrochemical properties. The formation of a protective surface film via electrolyte additives is considered a cost-effective and reliable way to improve the cathode–electrolyte interfacial stability, as the stable surface film, uniformly distributed over the entire cathode surface, would prevent direct contact of oxide with the electrolyte, still allowing Li+ transport between the cathode and electrolyte.3 In this work, we report the high-performance NCM cathode through interfacial stabilization using a novel electrolyte additive. The details of surface film stability and formation mechanism, and their relation to gas evolution as well as cycling performance would be discussed.