Multiscale Sampling of a Heterogeneous Water/Metal Catalyst Interface using Density Functional Theory and Force-Field...

Area of Science:

• Computational Chemistry
• Chemical Engineering
• Materials Science

Background:

• Heterogeneously-catalyzed chemical processes often occur in liquid environments, posing simulation challenges due to solvent interactions.
• Accurately modeling bond breaking/forming in these systems requires quantum chemical methods, complicated by solvent molecule thermal motion.

Purpose of the Study:

• To present a protocol for generating and sampling liquid water configurations around catalytic species on metal surfaces.
• To balance chemical accuracy with computational efficiency in simulating liquid-phase catalysis.

Main Methods:

• Utilizing force field molecular dynamics (FFMD) to generate configurations of liquid water molecules.
• Employing quantum mechanics-based methods, such as density functional theory (DFT) or ab initio molecular dynamics, on FFMD-generated configurations.

Main Results:

• The protocol was applied to catalytic intermediates in glycerol decomposition.
• Calculated enthalpies of solvation for catalytic species and identified water molecule roles in decomposition pathways.

Conclusions:

• The developed protocol effectively generates configurations for accurate simulation of liquid-phase catalytic processes.
• This approach aids in understanding solvent effects and water participation in heterogeneous catalysis.