CO Oxidation Promoted by Gold Atoms Loosely Attached in AuFeO3(-) Cluster Anions

J Phys Chem Lett. 2014 May 1;5(9):1585-90. doi: 10.1021/jz500509j. Epub 2014 Apr 17.

Abstract

Time-of-flight mass spectrometry experiment shows that upon the interactions with carbon monoxide, the mass-selected AuFeO3(-) oxide cluster anions can evaporate neutral gold atoms in a hexapole collision cell and oxidize CO into CO2 in an ion trap reactor. The computational studies identify that the gold atom is loosely attached in the AuFeO3(-) cluster, and the different reaction channels can be attributed to different cluster velocities. The structure of the AuFeO3(-) cluster is very flexible, and the approach of CO induces significant geometrical and electronic structure changes of AuFeO3(-), which facilitates the exposure of the positively charged gold atom to trap and oxidize CO. The CO oxidation by the AuFeO3(-) cluster follows the Au-assisted Mars-van Krevelen mechanism, in which the direct participation of the surface lattice oxygen (O(2-)) is proposed.

Keywords: CO oxidation; atomic clusters; density functional calculations; gold; mass spectrometry.