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 language | English |
|---|---|
| Article number | 14881 |
| Journal | Nature Communications |
| Volume | 8 |
| DOIs | |
| Publication status | Published - Mar 28 2017 |
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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 journal › Article
}
TY - JOUR
T1 - Stable and solubilized active Au atom clusters for selective epoxidation of cis-cyclooctene with molecular oxygen
AU - Qian, Linping
AU - Wang, Zhen
AU - Beletskiy, Evgeny V.
AU - Liu, Jingyue
AU - Dos Santos, Haroldo J.
AU - Li, Tiehu
AU - Rangel, Maria Do C
AU - Kung, Mayfair C.
AU - Kung, Harold H
PY - 2017/3/28
Y1 - 2017/3/28
N2 - 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.
AB - 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.
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U2 - 10.1038/ncomms14881
DO - 10.1038/ncomms14881
M3 - Article
VL - 8
JO - Nature Communications
JF - Nature Communications
SN - 2041-1723
M1 - 14881
ER -