Dynamic Activation of Ga Sites by Pt Dopant in Low-Temperature Liquid-Metal Catalysts

Liquid GaPt catalysts with Pt concentrations as low as 1x10(-4) atomic % have recently been identified as highly active for the oxidation of methanol and pyrogallol under mild reaction conditions. However, almost nothing is known about how liquid state catalysts support these significant improvements in activity. Here, ab initio molecular dynamics simulations are employed to examine GaPt catalysts in isolation and interacting with adsorbates. We find that persistent geometric features can exist in the liquid state, given the correct environment. We postulate that the Pt dopant may not be limited to direct involvement in catalysis of reactions, but rather that its presence can also enable Ga atoms to become catalytically active.

Automated summary

Liquid GaPt catalysts with Pt concentrations as low as 1x10(-4) atomic % have been found to exhibit high activity for the oxidation of methanol and pyrogallol under mild reaction conditions. However, the mechanism behind these significant improvements in activity is still unknown. In this study, ab initio molecular dynamics simulations are used to investigate the behavior of GaPt catalysts and their interaction with adsorbates. The results suggest that persistent geometric features can exist in the liquid state, and the presence of Pt dopant may enable the Ga atoms to become catalytically active.