Adsorption of O2 on Cationic Gold Clusters:Analyses on Bonding Strength and Extent of Activation
We explored the adsorption of O2 on cationic gold clusters by combining clus-ter reaction experiments and theoretical calculations.Under a mild condition,Au10+can readily adsorb one O2 molecule forming Au10O2+;Au2+and Au4+are low-reactive,while the argon complexes Au2ArO2+and Au4Ar1,2O2+can easily form;all other sizes are inactive.Theoreti-cal calculations indicate that the O2 on the linear or planar structures of Aun+(n=2-7)and the planar isomers of Au8+tends to be adsorbed in an end-on man-ner and non-activated,and so does the O2 on the large odd sizes of Aun+with n=9,11,and 13 determined to be three-dimensional struc-tures.In marked contrast,the O2 on the three-dimensional isomer of Au8+and the large even-numbered Aun+with n=10,12,and 14 tends to be adsorbed in a side-on manner and appar-ently activated.Observation of only Au2,4,10O2+,Au2ArO2+,and Au4ArO2+in the present experiments can be well rationalized using the calculated bonding strengths and the kinetic factors.
Cationic gold clusterTime-of-flight mass spectrometerDensity functional the-oryO2 activation
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