Graphene in Water is Hardly Ever Neutral

Abstract Graphene in water is electrically charged in most conditions. The level of charge can be large enough to stabilize single (or few) layer graphene colloidal dispersions in water, without the need of using any other additive. In this work, potentiometric titration, isothermal titration calorimetry, electrokinetic measurements, Density Functional Theory calculations, Raman Spectroscopy, and direct force measurements using Atomic Force Microscopy to investigate this charge and explore its origin are combined. The body of data collected suggests that this charge is a consequence of the interaction between water ions (hydroxide and hydronium) and graphene, and can be conveniently tuned (in magnitude and sign) by changing the pH of water.