Document Type
Article
Original Publication Date
2004
Journal/Book/Conference Title
The Journal of Chemical Physics
Volume
120
Issue
14
DOI of Original Publication
10.1063/1.1666009
Date of Submission
October 2015
Abstract
Experimental and theoretical evidence is presented for the nondissociative chemisorption of O2on free Au cluster anions (Au−n, n=number of atoms) with n=2, 4, 6 at room temperature, indicating that the stabilization of the activated di-oxygen species is the key for the unusual catalytic activities of Au-based catalysts. In contrast to Au−n with n=2, 4, 6, O2 adsorbs atomically on Aumonomer anions. For the Aumonomer neutral, calculations based on density functional theory reveal that oxygen should be molecularly bound. On Au dimer and tetramer neutrals, oxygen is molecularly bound with the O–O bond being less activated with respect to their anionic counterparts, suggesting that the excess electron in the anionic state plays a crucial role for the O–O activation. We demonstrate that interplay between experiments on gas phase clusters and theoretical approach can be a promising strategy to unveil mechanisms of elementary steps in nanocatalysis.
Rights
Sun, Q., Jena, P., Kim, Y. D., et al. Interactions of Au cluster anions with oxygen. The Journal of Chemical Physics 120, 6510 (2004). Copyright © 2004 AIP Publishing LLC.
Is Part Of
VCU Physics Publications
Comments
Originally published at http://dx.doi.org/10.1063/1.1666009