A high capacity cathode based on silicates material for advanced lithium batteries

Silicate materials have been proposed as alternative cathodes for Li-ion battery applications. A novel mixture of silicates, labelled Li6MnSi5, based on the molar ratio among the Li / Mn / Si precursors, with promising electrochemical properties as positive electrode material is synthesized through a solid-state reaction. The results indicate the proposed synthetic method as effective for preparation of nanostructured silicate owders with average particle diameter of 30 nm. Structural morphology of the samples was determined using X-ray powder diffraction (XRPD), XPS and FESEM analysis. A joint analysis by XRPD data and by density unctional theory (DFT) identified LiHMn4Si5O15, Li2Mn4Si5O15, Li2Si2O5 and Li0.125Mn0.875SiO4 as components of Li6MnSi5 mixture. The electrochemical performance of Li6MnSi5 was evaluated by charge/discharge testing at constant current mode. Li6MnSi5 discharge behaviour is characterized by high capacity value of 480 mA h g-1 , although such capacity fades gradually on cycling. Ex situ XPS studies carried out on the electrode in both full charged and discharged states, pointed out that Li2Si2O5 is decisive for achieving such high capacity. The discharge/charge plateau is most probably related to the change in the oxidation state of silicon at the surface of the silica material.