A synergistic modification strategy for enhancing the cycling stability and rate capacity of single-crystal nickel-rich cathode materials

Abstract

Ni-rich layered LiNi0.8Co0.1Mn0.1O2 (NCM811) is considered to be one of the most promising cathode materials due to its advantages of high specific capacity, lower cost and environmental friendliness. However, the relatively high nickel content in the LiNi0.8Co0.1Mn0.1O2 layered cathode materials leads to the instability of the internal structure and surface of the materials during long-term cycling, which results in the deterioration of electrochemical performance. In this study, single-crystal NCM811 (SNCM811) was prepared using a convenient solid-state method. By doping Al into SNCM811 (SNCMAl) and purposefully low-temperature surface treatment with a small amount of LiPF6, a Ni-rich single-crystal NCM811 modified by both Al bulk doping and LiF surface coating (SNCMAl@LiF) was obtained. The reversible capacity of SNCMAl@LiF with a cutoff voltage of 2.7–4.3 V at 0.1C is 200.3 mAh·g−1. And the capacity retention of the single-crystal cathode materials is 92.4 % with capacity of 171.07 mAh·g−1 after 100 cycles at 1C. Even at high rate of 10C, the discharge specific capacity maintains 148.8 mAh·g−1, demonstrating excellent electrochemical performance. The dual-modified single-crystal material has the lowest potential difference and electrochemical impedance without intragranular cracks and crystal slips after 100 cycles. Stronger AlO bond in single crystals reduced the degree of cation mixing and maintained the stability of the layered structure. LiF-modified surface can promote the transfer of Li+, maintain the stability of the electrode/electrolyte interface and then improve the electrochemical performance of cathode materials. Al-doping and LiF-coating provides a guidance on how to enhance the electrochemical performance of Ni-rich single-crystal cathode materials.