The lithium storage properties of graphene nanosheet (GNS) materials as high capacity anode materials for rechargeable lithium secondary batteries (LIB) were investigated. Graphite is a practical anode material used for LIB, because of its capability for reversible lithium ion intercalation in the layered crystals, and the structural similarities of GNS to graphite may provide another type of intercalation anode compound. While the accommodation of lithium in these layered compounds is influenced by the layer spacing between the graphene nanosheets, control of the intergraphene sheet distance through interacting molecules such as carbon nanotubes (CNT) or fullerenes (C60) might be crucial for enhancement of the storage capacity. The specific capacity of GNS was found to be 540 mAh/g, which is much larger than that of graphite, and this was increased up to 730 mAh/g and 784 mAh/g, respectively, by the incorporation of macromolecules of CNT and C60 to the GNS.

Recently, battery technology has come to require a higher rate capability. The main difficulty in high-rate charge-discharge experiments is kinetic problems due to the slow diffusion of Li-ions in electrodes. Nanosizing is a popular way to achieve a higher surface area and shorter Li-ion diffusion length for fast diffusion. However, while various nanoelectrodes that provide excellent high-rate capability have been synthesized, a size-controlled synthesis and a systematic study of nanocrystalline LiCoO2 have not been carried out because of the difficulty in controlling the size. We have established the size-controlled synthesis of nanocrystalline LiCoO2 through a hydrothermal reaction and, for the first time, clarified the structural and electrochemical properties of this intercalation cathode material. Lattice expansion in nanocrystalline LiCoO2 was found from powder X-ray diffraction measurements and Raman spectroscopy. Electrochemical measurements and theoretical analyses on nanocrystalline LiCoO2 revealed that extreme size reduction below 15 nm was not favorable for most applications. An excellent high-rate capability (65% of the 1 C rate capability at 100 C) was observed in nanocrystalline LiCoO2 with an appropriate particle size of 17 nm.

The effect of crystallite size on Li-ion insertion in electrode materials is of great interest recently because of the need for nanoelectrodes in higher-power Li-ion rechargeable batteries. We present a systematic study of the effect of size on the electrochemical properties of LiMn(2)O(4). Accurate size control of nanocrystalline LiMn(2)O(4), which is realized by a hydrothermal method, significantly alters the phase diagram as well as Li-ion insertion voltage. Nanocrystalline LiMn(2)O(4) with extremely small crystallite size of 15 nm cannot accommodate domain boundaries between Li-rich and Li-poor phases due to interface energy, and therefore lithiation proceeds via solid solution state without domain boundaries, enabling fast Li-ion insertion during the entire discharge process.