1. Molecular-Level Details about Liquid H2O Interactions with CO and Sugar Alcohol Adsorbates on Pt(111) Calculated Using Density Functional Theory and Molecular Dynamics
- Author
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Sapna Sarupria, Rachel B. Getman, and Cameron J. Bodenschatz
- Subjects
Work (thermodynamics) ,Hydrogen bond ,Aqueous two-phase system ,Surfaces, Coatings and Films ,Electronic, Optical and Magnetic Materials ,Catalysis ,chemistry.chemical_compound ,Molecular dynamics ,General Energy ,chemistry ,Computational chemistry ,Chemical physics ,Molecule ,Density functional theory ,Methanol ,Physics::Chemical Physics ,Physical and Theoretical Chemistry - Abstract
Catalytic fuel production and energy generation from biomass-derived compounds generally involve the aqueous phase, and water molecules at the catalyst interface have energetic and entropic consequences on the reaction free energies. These effects are difficult to elucidate, hindering rational catalyst design for these processes and inhibiting their widespread adoption. In this work, we combine density functional theory (DFT) and classical molecular dynamics (MD) simulations to garner molecular-level insights into H2O–adsorbate interactions. We obtain ensembles of liquid configurations with classical MD and compute the electronic energies of these systems with DFT. We examine CO, CH2OH, and C3H7O3 intermediates, which are critical in biomass reforming and direct methanol electrooxidation, on the Pt(111) surface under various explicit and explicit/implicit water configurations. We find that liquid H2O molecules arrange around surface intermediates in ways that favor hydrogen bonding, with larger and more h...
- Published
- 2015
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