Recycling
graphite from spent lithium-ion batteries plays a significant
role in relieving the shortage of graphite resources and environmental
protection. In this study, a novel method was proposed to regenerate
spent graphite (SG) via a combined sulfuric acid curing, leaching,
and calcination process. First, we conducted a sulfuric acid curing–acid
leaching experiment and systematically investigated the effects of
various operation conditions on the removal of impurities. Regenerated
graphite was obtained after a sequential calcination at 1500 °C,
and its morphology and structure were characterized by using X-ray
diffraction, Raman spectroscopy, and spherical aberration electron
microscopy analysis. The results show that the impurity removal efficiency
by sulfuric acid curing–acid leaching is much higher than that
by direct acid leaching, and the purity of the regenerated graphite
can reach 99.6%. Additionally, the regenerated graphite displays favorable
characteristics in morphology and structure, which are close to that
of a commercial unused material. The regenerated graphite exhibits
good electrochemical performance in charge capacity and cycle. The
initial charge capacity and retention rate are 349 mA h/g and 98.8%,
respectively. This recycle method has the advantages of low energy
consumption and low waste acid discharge and can be performed by easily
available equipment, so it may have great prospect for the industrial-scale
recycling of SG.