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首页> 外文期刊>Chemistry: A European journal >Palladium Nanoparticles Bonded to Two-Dimensional Iron Oxide Graphene Nanosheets: A Synergistic and Highly Reusable Catalyst for the Tsuji-Trost Reaction in Water and Air
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Palladium Nanoparticles Bonded to Two-Dimensional Iron Oxide Graphene Nanosheets: A Synergistic and Highly Reusable Catalyst for the Tsuji-Trost Reaction in Water and Air

机译：结合到二维氧化铁石墨烯纳米片上的钯纳米粒子：在水中和空气中的Tsuji-Trost反应的协同和高度可重复使用的催化剂

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Low cost, high activity and selectivity, convenient separation, and increased reusability are the main requirements for noble-metal-nanocatalyst-catalyzed reactions. Despite tremendous efforts, developing noble-metal nanocatalysts to meet the above requirements remains a significant challenge. Here we present a general strategy for the preparation of strongly coupled Fe_3O_4 and palladium nanoparticles (PdNPs) to graphene sheets by employing polyethyleneimine as the coupling linker. Transmission electron microscopic images show that Pd and Fe_3O_4 nanoparticles are highly dispersed on the graphene surface, and the mean particle size of Pd is around 3 nm. This nanocatalyst exhibits synergistic catalysis by Pd nanoparticles supported on reduced graphene oxide (rGO) and a tertiary amine of polyethyleneimine (Pd/Fe_3O_4/PEI/rGO) for the Tsuji-Trost reaction in water and air. For example, the reaction of ethyl acetoacetate with allyl ethyl carbonate afforded the allylated product in more than 99% isolated yield, and the turnover frequency reached 2200 h~(-1). The yield of allylated products was 66% for Pd/rGO without polyethyleneimine. The catalyst could be readily recycled by a magnet and reused more than 30 times without appreciable loss of activity. In addition, only about 7.5% of Pd species leached off after 20 cycles, thus rendering this catalyst safer for the environment.
机译：低成本，高活性和选择性，方便的分​​离以及增加的可重复使用性是贵金属-纳米催化剂催化反应的主要要求。尽管付出了巨大的努力，开发满足上述要求的贵金属纳米催化剂仍然是一项重大挑战。在这里，我们介绍了通过使用聚乙烯亚胺作为偶联连接剂，制备强耦合的Fe_3O_4和钯纳米颗粒（PdNPs）与石墨烯片的一般策略。透射电子显微镜图像显示，Pd和Fe_3O_4纳米颗粒高度分散在石墨烯表面，Pd的平均粒径约为3 nm。该纳米催化剂通过负载在还原的氧化石墨烯（rGO）和聚乙烯亚胺的叔胺（Pd / Fe_3O_4 / PEI / rGO）上的Pd纳米颗粒在水和空气中的Tsuji-Trost反应表现出协同催化作用。例如，乙酰乙酸乙酯与碳酸烯丙酯的反应得到的烯丙基化产物的分离收率超过99％，周转频率达到2200h〜（-1）。没有聚乙烯亚胺的Pd / rGO的烯丙基化产物的产率为66％。催化剂可以很容易地被磁铁回收，并可以重复使用30次以上，而活性却没有明显下降。此外，在20个循环后，仅约有7.5％的Pd沉淀出来，因此使该催化剂对环境更安全。

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