Scalable Multilayer Printing of Graphene Interfacial Layers for Ultrahigh Power Lithium-Ion Storage

A low resistance graphene-based interfacial layer is developed for multilayered lithium-ion capacitor electrodes using a layer-by-layer printing approach, with the goal of boosting energy storage performance at ultrafast charge/discharge rates (>= 100 C). The electrochemical behavior of spray printed Li4Ti5O12-based heterostructure electrodes is investigated as a thin, discrete graphene layer is placed: 1) at the base of the Li4Ti5O12 (at the electrode/current collector interface); 2) on the top of the Li4Ti5O12 (at the electrode/separator junction); and 3) both at the base and on the top of the Li4Ti5O12 (sandwich configuration), with marked improved electrode performance at >50 C when the graphene layer is interleaved at the Li4Ti5O12/current collector interface. This best performing heterostructure negative electrode is then coupled with a spray printed activated carbon positive electrode in a lithium-ion capacitor configuration, showing an attractive power density of approximate to 8000 W kg(-1) at 350 C. The fabrication of double-sided graphene/Li4Ti5O12 multilayered heteroelectrodes is successfully demonstrated over areas of 20 cm x 15 cm and in various patterned configurations.