A controlled surface exfoliation method for graphite pencil electrodes using an environmentally friendly, low cost and scalable electrochemical process is reported. A simple direct current power supply in a neutral medium is used for inducing graphene formation on the electrode surface in a controlled manner. The electrochemical properties of the surface exfoliated electrode are characterized, displaying a >300× increase in the electrochemical surface area and >50× decrease in the electrode resistance after exfoliation. The surface graphene layer is characterized using electron microscopy, Raman, infrared, X-ray photoelectron, and energy dispersive X-ray spectroscopies and X-ray diffractometry showing a fully exfoliated surface, formation of surface defects and mild surface graphene oxidation while maintaining an intact graphitic crystal structure. The surface exfoliated electrode is tested as a supercapacitor demonstrating more than 2 orders of magnitude improvement over non-exfoliated electrode in both 3-electrode and 2-electrode setups and achieving a high areal capacitance of ∼54 mF cm-2. The benign nature, low cost, scalability of our controlled surface exfoliation methodology, and its significant impact on the electrochemical properties of the electrode make it very promising for further investigation in various applications such as energy storage and conversion, sensors, and catalysis.
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