Supported single Au(Ⅲ) ion catalysts for high performance in the reactions of 1, 3-dicarbonyls with alcohols
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Aijun Duan(
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The high cost and poor atom utilization efficiency of noble metal catalysts have limited their industrial applications. Herein, we designed CeO2-supported single Au(Ⅲ) ion catalysts with ultra-low gold loading that can enhance the utilization efficiency of gold atoms and bridge the gap between homogeneous and heterogeneous gold catalysis. These catalysts were highly active and reusable for the reaction of 1, 3-dicarbonyls with alcohols. The catalytic turnover number of CeO2-supported single Au(Ⅲ) ion catalysts was much higher than that of the homogeneous catalyst NaAuCl4. In addition, the effects of gold loading and the drying method for the catalysts on the organic reactions were systematically explored. In-depth investigation of the structure–property relationship by highresolution transmission electron microscopy, hydrogen temperature-programmed reduction, X-ray absorption near edge structure analysis, UV–vis diffuse reflectance spectroscopy, and X-ray photoelectron spectroscopy revealed that the isolated Au(Ⅲ) ions were related to the active sites for the synthesis of β-substituted cyclohexenone and that CeO2 was responsible for yielding ketonic ester.
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Supported single Au(Ⅲ) ion catalysts for high performance in the reactions of 1, 3-dicarbonyls with alcohols
), Aijun Duan(
)
Abstract
The high cost and poor atom utilization efficiency of noble metal catalysts have limited their industrial applications. Herein, we designed CeO2-supported single Au(Ⅲ) ion catalysts with ultra-low gold loading that can enhance the utilization efficiency of gold atoms and bridge the gap between homogeneous and heterogeneous gold catalysis. These catalysts were highly active and reusable for the reaction of 1, 3-dicarbonyls with alcohols. The catalytic turnover number of CeO2-supported single Au(Ⅲ) ion catalysts was much higher than that of the homogeneous catalyst NaAuCl4. In addition, the effects of gold loading and the drying method for the catalysts on the organic reactions were systematically explored. In-depth investigation of the structure–property relationship by highresolution transmission electron microscopy, hydrogen temperature-programmed reduction, X-ray absorption near edge structure analysis, UV–vis diffuse reflectance spectroscopy, and X-ray photoelectron spectroscopy revealed that the isolated Au(Ⅲ) ions were related to the active sites for the synthesis of β-substituted cyclohexenone and that CeO2 was responsible for yielding ketonic ester.
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Acknowledgements
This work was financially supported by the National Natural Science Foundation of China (Nos. 21173269 and 21276277), the Ministry of Science and Technology of China (No. 2011BAK15B05), the Specialized Research Fund for the Doctoral Program of Higher Education (No. 20130007110003).
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