The Role of Reduced Graphite Oxide in Transition Metal Oxide Nanocomposites Used as Li Anode Material: An Operando...

A composite consisting of CoFe₂ O₄ spinel nanoparticles and reduced graphite oxide (rGO) is studied as an anode material during Li uptake and release by applying synchrotron operando X-ray diffraction (XRD) and operando X-ray absorption spectroscopy (XAS), yielding a comprehensive picture of the reaction mechanisms. In the early stages of Li uptake, a monoxide is formed as an intermediate phase containing Fe²⁺ and Co²⁺ ions; this observation is in contrast to reaction pathways proposed in the literature. In the fully discharged state, metallic Co and Fe nanoparticles are embedded in an amorphous Li₂ O matrix. During charge, metallic Co and Fe are oxidized simultaneously to Co²⁺ and Fe³⁺ , respectively, thus enabling a high and stable capacity to be achieved. Here, evidence is presented that the rGO acts as a support for the nanoparticles and prevents the particles from contact loss. The operando investigations are complemented by TEM, Raman spectroscopy, galvanostatic cycling, and cyclic voltammetry.