Stable and solubilized active Au atom clusters for selective epoxidation of cis-cyclooctene with molecular oxygen

Linping Qian, Zhen Wang, Evgeny V. Beletskiy, Jingyue Liu, Haroldo J. dos Santos, Tiehu Li, Maria do C. Rangel, Mayfair C. Kung () and Harold H. Kung ()
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Linping Qian: Fudan University
Zhen Wang: Northwestern University
Evgeny V. Beletskiy: Northwestern University
Jingyue Liu: Arizona State University
Haroldo J. dos Santos: Northwestern University
Tiehu Li: School of Materials Science and Engineering, Northwestern Polytechnical University
Maria do C. Rangel: Instituto de Química, Universidade Federal da Bahia
Mayfair C. Kung: Northwestern University
Harold H. Kung: Northwestern University

Nature Communications, 2017, vol. 8, issue 1, 1-9

Abstract: Abstract The ability of Au catalysts to effect the challenging task of utilizing molecular oxygen for the selective epoxidation of cyclooctene is fascinating. Although supported nanometre-size Au particles are poorly active, here we show that solubilized atomic Au clusters, present in ng ml−1 concentrations and stabilized by ligands derived from the oxidized hydrocarbon products, are active. They can be formed from various Au sources. They generate initiators and propagators to trigger the onset of the auto-oxidation reaction with an apparent turnover frequency of 440 s−1, and continue to generate additional initiators throughout the auto-oxidation cycle without direct participation in the cycle. Spectroscopic characterization suggests that 7–8 atom clusters are effective catalytically. Extension of work based on these understandings leads to the demonstration that these Au clusters are also effective in selective oxidation of cyclohexene, and that solubilized Pt clusters are also capable of generating initiators for cyclooctene epoxidation.

Date: 2017
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DOI: 10.1038/ncomms14881

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