The global energy consumption is accelerating at an alarming rate and will soon exhaust all fossil fuel resources. Sustainable, renewable, and environmentally friendly technologies for energy generation, storage, and conversion are high on the agenda of public and private enterprises. Electrochemical capacitors, also called supercapacitors, are one of the energy storage modalities. In light of their excellent power density, fast charging rate, and extended cycle life, supercapacitors have immense application potential in portable electronics and electric vehicles [1], and thus have been attracting growing research interest in recent years. In general, two major types of supercapacitors exist depending on the underlying energy storage mechanism: electric double-layer capacitors (EDLCs) and pseudocapacitors [2][3][4]. EDLCs store energy by the electrostatic accumulation of charges in the electric double layer near the electrode/electrolyte interface, as shown in Figure 5.1. The electrode materials for EDLCs are generally carbonaceous materials, such as activated carbon (AC), mesoporous carbon, carbon nanotubes, and graphene. The electric double-layer (EDL) capacitance is closely dependent on the surface area, which can be calculated using the following equation [5]:where r and 0 are the relative dielectric constant and the dielectric constant of vacuum, respectively, A is the specific surface area of the electrode accessible to the electrolyte ions, and d is the effective thickness of the EDL. Because of the nature of energy storage mechanism of EDLCs, charges are not transferred between the electrode materials and the electrolyte. Thus, the EDLCs have good cycling stability, but do not exhibit a high enough energy density to meet the ever-growing need for peak-power assistance in electric vehicles. Pseudocapacitors use an energy storage mechanism similar to that of electrochemical batteries, but the fast and the reversible faradaic reactions for energy storage primarily occur at the interface or near the interface of Graphene-based Energy Devices, First Edition. Edited by A. Rashid bin Mohd Yusoff.