Thickness Dependency of Battery Anode Properties in Multilayer Graphene

With the development of practical thin-film batteries, multilayer graphene (MLG) is being actively investigated as an anode material. Therefore, research on determining a technique to fabricate thick MLG on arbitrary substrates at low temperatures is essential. In this study, we formed an MLG with controlled thickness at low temperatures using a layer exchange (LE) technique and evaluated its anode properties. The LE technique enabled the formation of a uniform MLG with a wide range of thicknesses (25-500 nm) on Ta foil. The charge/discharge characterization using coin-type cells revealed that the total capacity, which corresponded to Li intercalation into the MLG interlayer, increased with increasing MLG thickness. In contrast, cross-sectional transmission electron microscopy showed a metal oxide formed at the MLG/Ta interface during annealing, which had small Li capacity. MLG with sufficient thickness (500 nm) exhibited an excellent Coulombic efficiency and capacity retention compared to bulk graphite formed at high temperatures. These results have led to the development of inexpensive and reliable rechargeable thin-film batteries.