Two-dimensional graphitic carbon-nitride (g-C3N4)-coated LiNi0.8Co0.1Mn0.1O2 cathodes for high-energy-density and long-life lithium batteries

Abstract

High-capacity nickel-rich layered oxides are promising cathode materials for high-energy-density lithium batteries. However, the poor structural stability and severe side reactions at the electrode/electrolyte interface result in unsatisfactory cycle performance. Herein, the thin layer of two-dimensional (2D) graphitic carbon-nitride (g-CN) is uniformly coated on the LiNiCoMnO (denoted as NCM811@CN) using a facile chemical vaporization-assisted synthesis method. As an ideal protective layer, the g-CN layer effectively avoids direct contact between the NCM811 cathode and the electrolyte, preventing harmful side reactions and inhibiting secondary crystal cracking. Moreover, the unique nano-pore structure and abundant nitrogen vacancy edges in g-CN facilitate the adsorption and diffusion of lithium ions, which enhances the lithium deintercalation/intercalation kinetics of the NCM811 cathode. As a result, the NCM811@CN-3wt% cathode exhibits 161.3 mAh g and capacity retention of 84.6% at 0.5 C and 55 °C after 400 cycles and 95.7 mAh g at 10 C, which is greatly superior to the uncoated NCM811 (i.e. 129.3 mAh g and capacity retention of 67.4% at 0.5 C and 55 °C after 220 cycles and 28.8 mAh g-1 at 10 C). The improved cycle performance of the NCM811@CN-3wt% cathode is also applicable to solid-liquid-hybrid cells composed of PVDF:LLZTO electrolyte membranes, which show 163.8 mAh g and the capacity retention of 88.1% at 0.1 C and 30 °C after 200 cycles and 95.3 mAh g at 1 C.