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-C3N4) is uniformly coated on the
LiNi0.8Co0.1Mn0.1O2
(denoted as NCM811@CN) using a facile chemical vaporization-assisted
synthesis method. As an ideal protective layer, the
g-C3N4 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-C3N4 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-1 and capacity retention of 84.6% at 0.5 C and 55
°C after 400 cycles and 95.7 mAh g-1 at 10 C, which is
greatly superior to the uncoated NCM811 (i.e. 129.3 mAh
g-1 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-1 and the capacity retention of
88.1% at 0.1 C and 30 °C after 200 cycles and 95.3 mAh
g-1 at 1 C.