Graphene versus concentrated aqueous electrolytes: the role of the electrochemical double layer in determining the screening length of an electrolyte

Understanding the performance of graphene devices in contact with highly concentrated aqueous electrolytes is key to integrating graphene into next-generation devices operating in sea water environments, biosensors, and high-density energy production/storage units. Despite significant efforts toward interpreting the structure of the electrochemical double layer at high concentrations, the interface between graphene-based materials and concentrated aqueous solutions has remained vaguely described. In this study, we demonstrate the use of graphene-based chemiresistors as a technique to indirectly quantify the experimental screening length of concentrated electrolytes that could clarify the interpretation of electrochemical measurements conducted at low ionic strength. We report a breakdown of the Debye–Hückel theory in the proximity of graphene surfaces at lower concentrations (10–50 mM) than previously reported for other systems, depending on cation size, dissolved oxygen concentration, and degree of graphene defectivity.