Electrochemical and structural characterization of lithiation in spray deposited ordered mesoporous titania as an...

Ordered mesoporous titania, prepared via low-temperature spray deposition, was examined as an anode material for lithium ion batteries. The material exhibits an exceptionally high electrochemical capacity of 680 mA h g^-1 during the first discharge, which rapidly decreases over the following cycles. The capacity stabilizes at around 170 mA h g^-1 after 50 cycles and the material delivers 83 mA h g^-1 at high charge/discharge rates (10C). A combination of electrochemical and structural characterization techniques were used to study the charge/discharge behavior of the material and the origin of the irreversible capacity. To determine the effect of cycling on the structure of the material, X-ray absorption spectroscopy (XAS) and energy filtered TEM were carried out on pristine and cycled samples in intercalated and deintercalated states. Titanium K-edge XAS measurements showed that intercalated lithium affects the NEXAFS region. By comparing peak intensity ratios, we propose a method to quantify the amount of lithium inserted into the titania structure and to differentiate between lithium bound in close proximity to titanium, and lithium bound further away from titanium. Additionally, we suggest that the irreversible loss in capacity is due to the formation of phases that are stable, and thereby electrochemically inactive, over the electrochemical cycling conditions applied.