Multifunctional PdAg@MIL-101 for One-Pot Cascade Reactions: Combination of Host-Guest Cooperation and Bimetallic Synergy in Catalysis
Multifunctional PdAg@MIL-101 for One-Pot Cascade Reactions: Combination of Host-Guest Cooperation and Bimetallic Synergy in Catalysis
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用于一锅级联反应的多功能 PdAg@MIL-101：催化中主客体合作和双金属协同的结合
DOI：
10.1021/cs501953d
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发表时间：
2015-04-01
期刊：
影响因子：
12.9
通讯作者：
Jiang, Hai-Long
中科院分区：
文献类型：
--
作者：
Chen, Yu-Zhen;Zhou, Yu-Xiao;Jiang, Hai-Long
由金属有机骨架（MOF）稳定的金属纳米粒子（NP）在催化方面非常有前景，但关于它们协同催化级联反应的报道却非常罕见。在这项工作中，Pd NPs 结合到 MOF MIL-101 中，共同完成了基于 MOF Lewis 酸性和 Pd NPs 的串联反应。随后，超细 PdAg 合金纳米粒子（类似于 1.5 nm）被封装到 MIL-101 中。所获得的多功能PdAg@MIL-101基于主客体合作和双金属协同作用，在温和条件下的级联反应中表现出良好的催化活性和选择性，其中MIL-101提供路易斯酸性，Pd提供加氢活性，而Ag大大提高了对目标产物的选择性。据我们所知，这是第一个将双金属NP@MOF作为多功能催化剂的工作，具有多个活性位点（MOF酸性和双金属物质），发挥各自的功能并协同催化一锅级联反应。
Metal nanoparticles (NPs) stabilized by metal-organic frameworks (MOFs) are very promising for catalysis, while reports on their cooperative catalysis for a cascade reaction have been very rare. In this work, Pd NPs incorporated into a MOF, MIL-101, have jointly completed a tandem reaction on the basis of MOF Lewis acidity and Pd NPs. Subsequently, ultrafine PdAg alloy NPs (similar to 1.5 nm) have been encapsulated into MIL-101. The obtained multifunctional PdAg@MIL-101 exhibits good catalytic activity and selectivity in cascade reactions under mild conditions, on the basis of the combination of host-guest cooperation and bimetallic synergy, where MIL-101 affords Lewis acidity and Pd offers hydrogenation activity while Ag greatly improves selectivity to the target product. As far as we know, this is the first work on bimetallic NP@MOFs as multifunctional catalysts with multiple active sites (MOF acidity and bimetallic species) that exert respective functions and cooperatively catalyze a one-pot cascade reaction.