Interaction of C₆₀ with water: first-principles modeling and environmental implications

The nature of fullerene-water interactions has been the subject of much research and debate. Specifically, the presence of a stabilizing, negative surface potential on colloidal aggregates of C60 in water is unexpected, given the neutral nature of pure carbon, and is not well understood. Previous simulation efforts have focused on the C60-water interaction using molecular dynamics simulations that lacked the ability to account for charge transfer and distribution interactions. In this study, first-principles density functional theory was used to analyze the fundamental electronic interactions to elucidate the polarization and charge transfer between water and C60. Simulations show that charge is inductively transferred to the C60 from water molecules, with subsequent polarization of the C60 molecule. In a case with two neighboring C60 molecules, the charge polarization induces a charge onto the second C60. Simulation suggests that this charge transfer and polarization may contribute at least partly to the observed negative surface potential of fullerene aggregates and, combined with hydrogen bonding network formation around C60, provides a fundamental driving force for aggregate formation in water.