Real Time Tracking of Nanoconfined Water‐Assisted Ion Transfer in Functionalized Graphene Derivatives Supercapacitor Electrodes

Abstract Water molecules confined in nanoscale spaces of 2D graphene layers have fascinated researchers worldwide for the past several years, especially in the context of energy storage applications. The water molecules exchanged along with ions during the electrochemical process can aid in wetting and stabilizing the layered materials resulting in an anomalous enhancement in the performance of supercapacitor electrodes. Engineering of 2D carbon electrode materials with various functionalities (oxygen (─O), fluorine (─F), nitrile (─C≡N), carboxylic (─COOH), carbonyl (─C═O), nitrogen (─N)) can alter the ion/water organization in graphene derivatives, and eventually their inherent ion storage ability. Thus, in the current study, a comparative set of functionalized graphene derivatives—fluorine‐doped cyanographene (G–F–CN), cyanographene (G–CN), graphene acid (G–COOH), oxidized graphene acid (G‐COOH (O)) and nitrogen superdoped graphene (G–N) is systematically evaluated toward charge storage in various aqueous‐based electrolyte systems. Differences in functionalization on graphene derivatives influence the electrochemical properties, and the real‐time mass exchange during the electrochemical process is monitored by electrochemical quartz crystal microbalance (EQCM). Electrogravimetric assessment revealed that oxidized 2D acid derivatives (G–COOH (O)) are shown to exhibit high ion storage performance along with maximum water transfer during the electrochemical process. The complex understanding of the processes gained during supercapacitor electrode charging in aqueous electrolytes paves the way toward the rational utilization of graphene derivatives in forefront energy storage applications.