  Advanced supercapacitors have great potential to transform how we store and
utilize energy, leading to more efficient and sustainable energy systems. This
study reveals the structural features influencing the interfacial thermal
transport and electrical performances of supercapacitors, using the constant
potential and constant charge molecular dynamics simulation techniques. Thermal
and electrical properties were calculated for graphene/carbon nanotube
composite electrodes and ionic liquid electrolytes with different nanotube
diameter, number, layers, and alignments of the nanotubes. The effect of
application of a constant potential on the Kapitza resistance is determined for
the first time. The vertically aligned CNT structures exhibited higher
electrical performance, while the horizontal arrangement showed better thermal
performance. Optimum electrode configurations were identified by considering
thermal and electrical performance, along with other design factors, such as
structural stability, ease of manufacturing, and scalability. After considering
all these factors, the horizontally stacked multi-layer CNT arrangement emerged
as the optimal electrode structure. The insights gained from this study aid in
comprehending the effects of variations in electrode structure, thereby
enabling efficient supercapacitor electrode design.
