Accounting for liquid solvent effects on the solutes adsorption of liquid/metal interfaces is a grand challenge in many research fields, such as heterogeneous catalysis, electrochemistry, corrosion, or biomedicine. The characterization of solvent effects is challenging because of configurational disorder in the solvent structure. Our group previously developed a sampling strategy—based-on molecular dynamics (MD)—for simulating configurational influences to the adsorption of solute species to solid surfaces under liquid solvent. This method allows us to calculate the encounter sticking coefficient (SE) and the adsorption rate for solutes adsorbing to a solid surface. However, once the solute molecule is close to the surface, our method does not account for the bonding energy contribution between the adsorbed species and the surface; which could influence the adsorption rate. Herein, we investigate how bonding energy contributions of adsorbate species influence their adsorption under liquid solvent conditions. To do this, we develop a force field (FF) that can capture chemical bonding between the catalytic species and the catalyst surface. Specifically, we derive the MePt-FF, which can model CH3OH adsorption to Pt(111). To map the CH3OH-Pt potential energy surface, we construct a set of 600 frames by dragging the CH3OH to and over the Pt(111) surface. Partial optimizations of the CH3OH are performed using the VASP code. We demonstrate the use of MePt-FF in calculating the adsorption of CH3OH under liquid solvent and compare it with our prior method to elucidate the influence of liquid solvent conformational changes on the CH3OH/Pt(111) system.

Free Energies calculations of CH3OH-Pt(111) under Liquid Solvent: Development and Assessment Interfacial Force Field

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