In this study, the adsorption mechanism of different mixtures of monomers of polyvinylpyrrolidone (PVP)-based battery binders (polyvinylpyrrolidone:polyvinylidene difluoride, PVP:PVDF; polyvinylpyrrolidone:polyacrylic acid, PVP:PAA; and polyvinylpyrrolidone:lithiated polyacrylic acid, PVP:Li-PAA) on a graphene oxide (GO) nanoparticle was investigated using density functional theory (DFT), quantum theory of atoms in molecules (QTAIM) and molecular dynamics (MD) simulations in order to identify the thermodynamic, intermolecular forces and interfacial properties of these systems within the framework of battery applications employing LiPF6-EC-EMC electrolyte. Our work focuses into the short-range interactions and electronic properties of the adsorbed binder mixtures on the GO nanoparticle, and also into their interfacial properties (considering systems with and without the electrolyte, 1.2 M LiPF6 dissolved in EC/EMC 3/7, w/w), shedding light on the fundamental interactions that govern the mechanisms of GO (and also another 2D-nanomaterial such as graphite, for reference) enabling the physical adsorption of binders (and electrolyte compounds) for obtaining strongly adhered anode and cathode active substances in Li-ion battery applications. The results of this study advance the understanding of the adsorption mechanisms of binder mixtures and electrolyte compounds on carbon-based nanomaterials, and hold significant promise for the designing battery-optimized energy devices in lithium-ion batteries.
