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活性炭负载金簇上葡萄糖高效有氧氧化制葡萄糖酸

Efficient Aerobic Oxidation of Glucose to Gluconic Acid over Activated Carbon-Supported Gold Clusters.

作者信息

Liu Chao, Zhang Junying, Huang Jiahui, Zhang Chaolei, Hong Feng, Zhou Yang, Li Gao, Haruta Masatake

机构信息

Gold Catalysis Research Centre, State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, P. R. China.

出版信息

ChemSusChem. 2017 May 9;10(9):1976-1980. doi: 10.1002/cssc.201700407. Epub 2017 Apr 11.

Abstract

The catalytic performance of the atomically precise gold cluster-Au (PET) (PET=2-phenylethanethiolate), immobilized on activated carbon (AC), was investigated for the aerobic oxidation of glucose to gluconic acid. The Au (PET) /AC-120 catalysts, annealed at 120 °C in air, exhibited high catalytic activity and significantly better performance than the corresponding catalysts Au /AC-150 and Au /AC-300 (treated at 150 and 300 °C to remove the protecting thiolate ligands). The high activity of the robust Au cluster was a result of the partial ligand removal, providing catalytically active sites, which were evidenced by TEM, X-ray photoelectron spectroscopy, thermogravimetric analysis, and Fourier-transform IR spectroscopy. Au (PET) /AC-120 also showed excellent recyclability (up to seven cycles). The turnover frequency for the Au (PET) /AC-120 catalyst was 5440 h , which is higher than for the Pd/AC, Pd-Bi/AC, and Au/AC under identical reaction conditions. This new ultra-small gold nanomaterial is expected to find wide application in other catalytic oxidations.

摘要

研究了负载在活性炭(AC)上的原子精确金簇-Au(PET)(PET = 2-苯乙硫醇盐)对葡萄糖有氧氧化生成葡萄糖酸的催化性能。在空气中120°C退火的Au(PET)/AC-120催化剂表现出高催化活性,并且比相应的催化剂Au /AC-150和Au /AC-300(在150和300°C处理以去除保护硫醇盐配体)具有明显更好的性能。坚固的金簇的高活性是部分配体去除的结果,提供了催化活性位点,这通过透射电子显微镜(TEM)、X射线光电子能谱、热重分析和傅里叶变换红外光谱得到证实。Au(PET)/AC-120还显示出优异的可回收性(高达七个循环)。在相同反应条件下,Au(PET)/AC-120催化剂的周转频率为5440 h⁻¹,高于Pd/AC、Pd-Bi/AC和Au/AC。这种新型超小金纳米材料有望在其他催化氧化中得到广泛应用。

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