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, Harold H. Kung

Research output: Contribution to journalArticle

14 Citations (Scopus)

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 440s-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.

Original languageEnglish (US)
Article number14881
JournalNature Communications
Volume8
DOIs
StatePublished - Mar 28 2017

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epoxidation
Epoxidation
Molecular oxygen
initiators
Hydrocarbons
Particle Size
Oxygen
Ligands
Atoms
Oxidation
oxidation
oxygen
atoms
atomic clusters
cycles
Demonstrations
hydrocarbons
actuators
Particle size
catalysts

ASJC Scopus subject areas

  • Chemistry(all)
  • Biochemistry, Genetics and Molecular Biology(all)
  • Physics and Astronomy(all)

Cite this

Stable and solubilized active Au atom clusters for selective epoxidation of cis-cyclooctene with molecular oxygen. / Qian, Linping; Wang, Zhen; Beletskiy, Evgeny V.; Liu, Jingyue; Dos Santos, Haroldo J.; Li, Tiehu; Rangel, Maria Do C; Kung, Mayfair C.; Kung, Harold H.

In: Nature Communications, Vol. 8, 14881, 28.03.2017.

Research output: Contribution to journalArticle

Qian, Linping ; Wang, Zhen ; Beletskiy, Evgeny V. ; Liu, Jingyue ; Dos Santos, Haroldo J. ; Li, Tiehu ; Rangel, Maria Do C ; Kung, Mayfair C. ; Kung, Harold H. / Stable and solubilized active Au atom clusters for selective epoxidation of cis-cyclooctene with molecular oxygen. In: Nature Communications. 2017 ; Vol. 8.
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AU - Dos Santos, Haroldo J.

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AU - Rangel, Maria Do C

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