Both LiCoO2 and LiNi1/3Mn1/3Co1/3O2 layered cathode materials are investigated in our studies. P3 phase of CoO2, the end member of the LixCoO2, is found in both chemically and electrochemically delithiated materials. Delithiated LixCoO2 specimens decompose into fine Co3O4 and LiCoO2 particles starting at around 200 °C. This decomposing reaction is proved by in-situ X-ray diffraction and in-situ transmission electron microscopy investigations. The structures of pristine and cycled LiNi1/3Mn1/3Co1/3O2 are investigated by electron diffraction. Single and polycrystalline crystals are found in this material. The partial substitution of Co by Ni and Mn in LiNi1/3Mn1/3Co1/3O2 opens up the possibility of different cation configurations in the crystal lattice. Both 3Rm symmetry and superlattices are identified in this material. The number of particles with superlattices in pristine material (40%) is much bigger than cycled material at discharge state (10%).

The rechargeable secondary Lithium ion (Li-ion) battery is expected to grow to more than $6.3 billion by 2012 from ~$4.6 billion in 2006. With the development of personnel electronics, hybrid and electric vehicles, Li-ion batteries will be more in demand. However, Li-ion batteries are not widely recycled because it is not economically justifiable (in contrast, at present more than 97% Lead-acid batteries are recycled). So far, no commercial methods are available to recycle different chemical Li-ion batteries economically and efficiently. Considering our limited resources, environmental impact, and national security, Li-ion batteries must be recycled. A new methodology with low temperature and high efficiency is proposed in order to recycle Li-ion batteries economically and with industrial viability. The separation and synthesis of cathode materials (most valuable in Li-ion batteries) from recycled components are the main focus of the proposed research. The analytical results showed that the recycling process is practical and has high recovery efficiency, create great commercial value as well.