The ubiquitous manufacturing of lithium-ion batteries
(LIBs) due
to high consumer demand produces inevitable e-waste that imposes severe
environmental and resource sustainability challenges. In this work,
the charge storage capability and Li-ion kinetics of the recovered
water-leached graphite (WG) anode from spent LIBs are enhanced by
using an optimized amount of recycled graphene nanoflakes (GNFs) as
an additive. The WG@GNF anode exhibits an initial discharge capacity
of 400 mAh g–1 at 0.5C with 88.5% capacity retention
over 300 cycles. Besides, it delivers an average discharge capacity
of 320 mAh g-1 at 500 mA g–1 over 1000
cycles, which is 1.5–2 times higher than that of WG. The sharp
increase in electrochemical performance is due to the synergistic
effects of Li-ion intercalation into the graphite layers and Li-ion
adsorption into the surface functionalities of GNF. Density functional
theory calculations reveal the role of functionalization behind the
superior voltage profile of WG@GNF. Besides, the unique morphology
of spherical graphite particles trapping into graphene nanoflakes
provides mechanical stability over long-term cycling. This work explains
an efficient strategy to upgrade the electrochemical compatibility
of recovered graphite anode from spent LIBs toward next-generation
high-energy-density LIBs.