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Open AccessArticle

Metal-Support Synergy of Supported Gold Nanoclusters in Selective Oxidation of Alcohols

1
Hangzhou Institute of Advanced studies, Zhejiang Normal University, Hangzhou 311231, China
2
CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
3
Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
4
The State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
*
Authors to whom correspondence should be addressed.
These authors contributed equally to this work and should be considered as the co-first authors.
Catalysts 2020, 10(1), 107; https://doi.org/10.3390/catal10010107
Received: 25 December 2019 / Revised: 6 January 2020 / Accepted: 8 January 2020 / Published: 11 January 2020
(This article belongs to the Section Nanostructured Catalysts)
Gold catalysts have been reported to exhibit good performance in aerobic oxidation of alcohols, but the intrinsic origin of the catalytic reactivity is still illusive. The catalyst preparation method, the morphology of the gold particles, and even the support might be key factors that determine the activity. Here, we prepared a series of gold catalysts with different supports, i.e., the hydrotalcite (HT), ZnO, MgO, Al2O3, and SiO2, by using the atomically controlled Au25 nanoclusters (NCs) as the gold precursor. The characterization results of the X-ray diffraction (XRD), UV-vis and transmission electron microscopy (TEM) show that the gold particles were mostly uniformly distributed on the supports, with a mean particle size within 3 nm. In aerobic oxidation of benzyl alcohol, the MgAl-HT- and Al2O3-supported Au25 NCs display good performances, with turnover frequency (TOF) values of ~2927 and 2892 h−1, respectively, whereas the SiO2-, MgO-, and ZnO-supported analogues show much inferior activity. The high resolution TEM and X-ray photoelectron spectra (XPS) results suggest that the interactions between gold and the supports in different samples are differing, which influences the morphology and the nature of gold. Our results further point to the importance of acid-base property of the support and the metal-support synergy rather than the gold particle size alone in achieving high-performance in selective alcohol oxidation. Moreover, this work provided a good way to design gold catalysts with controllable sizes that is crucial for understanding the reaction process in aerobic oxidation of alcohol. View Full-Text
Keywords: gold nanocluster; supported catalysts; aerobic oxidation of alcohols; support effect; size effect gold nanocluster; supported catalysts; aerobic oxidation of alcohols; support effect; size effect
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Liu, L.; Li, H.; Tan, Y.; Chen, X.; Lin, R.; Yang, W.; Huang, C.; Wang, S.; Wang, X.; Liu, X.Y.; Zhao, M.; Ding, Y. Metal-Support Synergy of Supported Gold Nanoclusters in Selective Oxidation of Alcohols. Catalysts 2020, 10, 107.

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