Boosting the power performance of multilayer graphene as lithium-ion battery anode via unconventional doping with in-situ formed Fe nanoparticles

Graphene is extensively investigated and promoted as a viable replacement for graphite, the state-of-the-art material for lithium-ion battery (LIB) anodes, although no clear evidence is available about improvements in terms of cycling stability, delithiation voltage and volumetric capacity. Here we report the microwave-assisted synthesis of a novel graphene-based material in ionic liquid (i.e., carved multilayer graphene with nested Fe3O4 nanoparticles), together with its extensive characterization via several physical and chemical techniques. When such a composite material is used as LIB anode, the carved paths traced by the Fe3O4 nanoparticles, and the unconverted metallic iron formed in-situ upon the 1st lithiation, result in enhanced rate capability and, especially at high specific currents (i.e., 5 A g−1), remarkable cycling stability (99% of specific capacity retention after 180 cycles), low average delithiation voltage (0.244 V) and a substantially increased volumetric capacity with respect to commercial graphite (58.8 Ah L−1 vs. 9.6 Ah L−1).