Dynamic sampling of liquid metal structures for theoretical studies on catalysis

Area of Science:

• Catalysis
• Materials Science
• Computational Chemistry

Background:

• Liquid metals are emerging as superior catalysts compared to solid catalysts for various reactions.
• Current theoretical models struggle to accurately simulate adsorbate interactions with dynamic liquid metal surfaces.

Purpose of the Study:

• To develop and validate a novel computational approach for modeling liquid metal catalysts.
• To accurately capture adsorbate-surface dynamics on liquid metals at operating temperatures.

Main Methods:

• Utilized *ab initio* molecular dynamics (AIMD) to simulate adsorbate behavior on liquid metal surfaces.
• Analyzed time-resolved structures and adsorption energies for formate on liquid Ga-In and methanol oxidation intermediates on Ga-Pt.

Main Results:

• Developed a method to account for the dynamic motion of liquid metal surfaces in catalytic simulations.
• Identified unstable intermediates in the methanol oxidation pathway on Ga-Pt, suggesting a revised reaction mechanism involving H desorption.
• Calculated accessible adsorption energies reflecting real-time surface dynamics.

Conclusions:

• The proposed AIMD approach provides a more accurate representation of liquid metal catalysis than static models.
• This method is crucial for advancing the understanding and design of efficient liquid metal catalysts.
• Highlights the importance of dynamic surface effects in catalytic reaction pathways.