Metal-Organic Framework Supported Gold Nanoparticles as a Highly Active Heterogeneous Catalyst for Aerobic Oxidation of Alcohols
Metal-Organic Framework Supported Gold Nanoparticles as a Highly Active Heterogeneous Catalyst for Aerobic Oxidation of Alcohols
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金属有机框架负载金纳米颗粒作为醇类有氧氧化的高活性多相催化剂
DOI：
10.1021/jp105666f
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发表时间：
2010-08-12
影响因子：
3.7
通讯作者：
Jiang, Huanfeng
中科院分区：
文献类型：
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作者：
Liu, Hongli;Liu, Yaling;Jiang, Huanfeng
金属有机骨架（MOB）是一类新兴的多孔材料，其作为金纳米颗粒（NP）的载体的使用可能为开发用于各种催化反应的高活性非均相金催化剂带来新的机会。尽管目前已经报道了一些MOF负载的纳米颗粒Au的实例，在溶液中制备活性Au NPs沉积的MOP催化剂仍然是具有挑战性的研究目标。在这项研究中，我们报告了一种高效的非均相金催化剂，这是通过一个简单的胶体方法沉积在沸石型的MOF（MIL-101）与聚乙烯吡咯烷酮（PVP）作为保护剂，使用HAuCl 4作为Au的前体。所制备的Au/MIL-101（CD/PVP）催化剂对多种醇类的液相好氧氧化反应表现出极高的催化活性，甚至在无水或无碱的环境条件下也能有效地催化氧化。该催化剂易于回收，可重复使用多次，金属不会流失，活性不会降低。Au NPs在MIL-101载体大笼中的高度分散性和芳基环对Au NPs的电子供体效应被认为是Au/MIL-101（CD/PVP）催化剂在无碱条件下醇的有氧氧化中观察到的高活性的主要原因
The use of metal-organic frameworks (MOB), an emerging class of porous materials, as supports for gold nanoparticles (NPs) may bring new opportunities in the development of highly active heterogeneous gold catalysts for a variety of catalytic reactions Although currently a few examples of MOF-supported nanoparticulate Au have been reported, the preparation of an active Au NPs deposited MOP catalyst in solution is still a challenging research target. In this study, we report a highly efficient heterogeneous gold catalyst, which was deposited on a zeolite-type MOF (MIL-101) by a simple colloidal method with polyvinylpyrrolidone (PVP) as protecting agent using HAuCl4 as the Au precursor. The resulting Au/MIL-101 (CD/PVP) catalyst exhibited extremely high catalytic activities in liquid-phase aerobic oxidation of a wide range of alcohols, which could even efficiently catalyze the oxidation under ambient conditions in the absence of water or base. Moreover, the catalyst was easily recoverable and could be reused several times without leaching of metals or debasing of activity. The high dispersion of Au NPs and the electron donation effects of aryl rings to the Au NPs within the large cages of the MIL-101 support are suggested to be the main reasons for the observed high activities of the Au/MIL-101 (CD/PVP) catalyst in aerobic oxidation of alcohols under base-free conditions