Lithium metal is known to possess a very high theoretical capacity of 3,842 mAh g À 1 in lithium batteries. However, the use of metallic lithium leads to extensive dendritic growth that poses serious safety hazards. Hence, lithium metal has long been replaced by layered lithium metal oxide and phospho-olivine cathodes that offer safer performance over extended cycling, although significantly compromising on the achievable capacities. Here we report the defect-induced plating of metallic lithium within the interior of a porous graphene network. The network acts as a caged entrapment for lithium metal that prevents dendritic growth, facilitating extended cycling of the electrode. The plating of lithium metal within the interior of the porous graphene structure results in very high specific capacities in excess of 850 mAh g À 1 . Extended testing for over 1,000 charge/discharge cycles indicates excellent reversibility and coulombic efficiencies above 99%.

Conventional graphitic anodes in lithium-ion batteries cannot provide high-power densities due to slow diffusivity of lithium ions in the bulk electrode material. Here we report photoflash and laser-reduced free-standing graphene paper as high-rate capable anodes for lithium-ion batteries. Photothermal reduction of graphene oxide yields an expanded structure with micrometer-scale pores, cracks, and intersheet voids. This open-pore structure enables access to the underlying sheets of graphene for lithium ions and facilitates efficient intercalation kinetics even at ultrafast charge/discharge rates of >100 C. Importantly, photothermally reduced graphene anodes are structurally robust and display outstanding stability and cycling ability. At charge/discharge rates of ~40 C, photoreduced graphene anodes delivered a steady capacity of ~156 mAh/g(anode) continuously over 1000 charge/discharge cycles, providing a stable power density of ~10 kW/kg(anode). Such electrodes are envisioned to be mass scalable with relatively simple and low-cost fabrication procedures, thereby providing a clear pathway toward commercialization.

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In this study, we report a novel route via microwave irradiation to synthesize a bio-inspired hierarchical graphene--nanotube--iron three-dimensional nanostructure as an anode material in lithium-ion batteries. The nanostructure comprises vertically aligned carbon nanotubes grown directly on graphene sheets along with shorter branches of carbon nanotubes stemming out from both the graphene sheets and the vertically aligned carbon nanotubes. This bio-inspired hierarchical structure provides a three-dimensional conductive network for efficient charge-transfer and prevents the agglomeration and restacking of the graphene sheets enabling Li-ions to have greater access to the electrode material. In addition, functional iron-oxide nanoparticles decorated within the three-dimensional hierarchical structure provides outstanding lithium storage characteristics, resulting in very high specific capacities. The anode material delivers a reversible capacity of ~1024 mA · h · g(-1) even after prolonged cycling along with a Coulombic efficiency in excess of 99%, which reflects the ability of the hierarchical network to prevent agglomeration of the iron-oxide nanoparticles.