Quantum mechanical and molecular mechanical simulation approaches bridging length and time scales for simulation of interface reactions in realistic environments

Abstract

Computer-assisted design of functional materials requires methods that are able to simultaneously describe these with the necessary accuracy at the relevant time and length scales. One such possibility is the combination of classical interatomic force fields with density-functional based tight-binding (DFTB), an efficient and accurate quantum method. We employ this combination to study porous silicon dioxide functionalized with imidazole, which is used as an additive to polymer electrolyte membranes (PEM) for fuel cells applications. We analyze the water density and the dynamics of the functional groups at different temperatures by molecular dynamics simulation, whereas we calculate DFTB free energy barriers for proton transport reactions within the functionalized surface at different water contents. Combining both results, a macroscopic picture of the proton diffusion is drawn. Furthermore, we simulate the adsorption reactions of different components of an epoxide adhesive system on gamma alumina, using a direct coupling of DFTB and classical modeling. This yields direct chemical insight, how water and excess protons at the interface weaken the adhesion between epoxy polymers and natively oxidized aluminium.