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Highly water-dispersible magnetite-supported Pd nanoparticles and single atoms as excellent catalysts for Suzuki and hydrogenation reactions

机译:高度水分散的磁铁矿支撑的PD纳米颗粒和单个原子作为铃木和氢化反应的优异催化剂

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摘要

The molecule 4-(diphenylphosphino) benzoic acid (dpa) anchored on the surface of magnetite nanoparticles permits the easy capture of palladium ions that are deposited on the surface of the magnetite nanoparticles after reduction with NaBH4. Unexpectedly, a significant fraction of dpa is removed in this process. Samples of Fe(3)O(4)dpa@Pdx containing different Pd loadings (x = 0.1, 0.3, 0.5 and 1.0 wt%) were prepared, and their catalytic efficiency for the Suzuki C-C coupling reaction was studied. The best catalyst was Fe(3)O(4)dpa@Pd-0.5, which gave the highest TOF published to date for the reaction of bromobenzene with phenylboronic acid in a mixture of ethanol/water (1/1). Interestingly, the same reaction carried out in water also produced excellent yields of the resulting C-C coupling product. The behaviour of other bromide aryl molecules was also investigated. The best catalytic results for the aqueous phase reduction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) were obtained using Fe(3)O(4)dpa@Pd-0.1. The presence of Pd SACs (single atom catalysts) seems to be responsible for this performance. In contrast, the same Fe(3)O(4)dpa@Pd-0.1 catalyst is absolutely inactive for the hydrogenation of styrene in ethanol.
机译:在磁铁矿纳米粒子表面上锚定的分子4-(二苯基膦基)苯甲酸(DPA)允许易于捕获沉积在用NaBH4还原后沉积在磁铁矿纳米颗粒表面上的钯离子。出乎意料地,在该过程中除去了大部分DPA。制备了含有不同PD载荷(X = 0.1,0.3,0.5和1.0wt%)的Fe(3)O(4)DPA @ PDX的样品,研究了铃木C-C偶联反应的催化效率。最佳催化剂是Fe(3)O(4)DPA@pd-0.5,其迄今为止溴苯与苯基硼酸在乙醇/水(1/1)的混合物中发布的最高TOF。有趣的是,在水中进行的相同反应也产生了优异的得到C-C偶联产物的产率。还研究了其他溴芳基分子的行为。使用Fe(3)O(4)DPA@pd-0.1获得4-硝基苯酚(4-NP)至4-氨基酚(4-AP)的最佳催化结果。 PD SACS(单原子催化剂)的存在似乎是这种性能的原因。相反,相同的Fe(3)O(4)DPA@pd-0.1催化剂绝对不活性乙醇苯乙烯的氢化。

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  • 来源
    《RSC Advances》 |2016年第73期|共10页
  • 作者单位

    Univ Barcelona Dept Quim Inorgan &

    Organ Seccio Quim Inorgan Marti &

    Franques 1-11 E-08028 Barcelona Spain;

    Univ Barcelona Dept Quim Inorgan &

    Organ Seccio Quim Inorgan Marti &

    Franques 1-11 E-08028 Barcelona Spain;

    Univ Barcelona Dept Quim Inorgan &

    Organ Seccio Quim Inorgan Marti &

    Franques 1-11 E-08028 Barcelona Spain;

    Univ Politecn Cataluna Inst Tecn Energet Diagonal 647 Barcelona 08028 Spain;

    Univ Barcelona Dept Quim Inorgan &

    Organ Seccio Quim Inorgan Marti &

    Franques 1-11 E-08028 Barcelona Spain;

    Univ Barcelona Dept Quim Inorgan &

    Organ Seccio Quim Inorgan Marti &

    Franques 1-11 E-08028 Barcelona Spain;

    Empa Swiss Fed Labs Mat Sci &

    Technol Electron Microscopy Ctr Uberlandstr 129 CH-8600 Dubendorf Switzerland;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 化学;
  • 关键词

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