High-voltage spinel LiNi0.5Mn1.5O4 (LNMO) is a promising cathode material for next-generation
lithium-ion
batteries (LIBs), but its poor cycle performance has impeded its commercialization.
In this study, we developed highly stable LNMO cathode materials having
an octahedral morphology through a solid-state high-energy ball-mill–cum–spray-drying
method. We also developed a novel strategy for modifying this cathode
material with two kinds of carbon materials, thereby improving the
electrochemical cycling performance. Introducing single-walled carbon
nanotubes (SWCNTs) as a sub-carbon conductive additive during the
slurry preparation process improved the conductivity of electrons
between the particles of the cathode material. The LNMO electrode
modified with the SWCNT sub-carbon additives exhibited an average
Coulombic efficiency of 99.4% after 500 cycles at 1C, compared with
98.9% for the pristine LNMO-based electrode. Furthermore, we used
a wet-chemical method to coat graphene oxide (GO) onto the post-sintered
LNMO cathode material to act as a protective layer, preventing corrosion
induced by HF in the electrolyte. The capacity retention of the GO-coated
LNMO electrode after 500 cycles at 1C (91.8%) was higher than that
of the pristine LNMO (52.5%). The corresponding dual-modification
strategy, combining the SWCNTs and GO, provided LNMO cathode materials
exhibiting superior rate performance and cyclability, with an average
Coulombic efficiency of 99.3% and capacity retention of 92.9% after
500 cycles at 1C. Thus, the LNMO cathode materials prepared in this
study possessed excellent electrochemical properties favoring their
marketability, applicability, and competitiveness for application
in high-voltage LIBs.