Fe3O4修饰的Pt-Ru/C纳米催化剂的制备及其在无溶剂条件下邻氯硝基苯选择性加氢的催化性能

doi:10.3866/PKU.WHXB201308151

Abstract

Abstract:

Aseries of Fe₃O₄-modified Pt-Ru/C nanocomposite catalysts were prepared by impregnation and hydrazine hydrate reduction of Pt and Ru precursors. Various Pt/Ru mass ratios of the catalysts were examined in terms of catalytic activity. They were characterized by transmission electron microscopic measurements (TEM), energy dispersive X-ray spectroscopy (EDX), X-ray photoelectron spectroscopy (XPS), and X-ray diffraction (XRD). The average diameters of the catalysts with different mass ratios of Pt/Ru were in a range of 2.2-2.5 nmwith narrowsize distributions. The valence states of the nanoparticles indicate strong interactions between the Pt and the carbon support or with Fe₃O₄. The XRDpatterns of the 8Pt-1Ru/Fe₃O₄/C, 6Pt-1Ru/Fe₃O₄/ C, 4Pt-1Ru/Fe₃O₄/C, and 2Pt-1Ru/Fe₃O₄/Ccatalysts have similar profiles, which are attributed to the cubic phase of pure Fe₃O₄ (i.e., no Pt or Ru present). These catalysts selectively hydrogenate ortho-chloronitrobenzene (o-CNB) to the corresponding ortho-chloroaniline (o-CAN) under solvent-free conditions that not only allowed high substrate concentrations promoting the hydrogenation reaction, but also enabled easy product separation and purification. They exhibited excellent catalytic activity (turnover frequency (TOF) range: 0.98-2.09 mol·mol^-1·s^-1) and up to 100% o-CAN selectivity, which was composition-dependent. The o-CAN yield selectivity monotonically increased with the proportion of Ru; however, the catalytic activity decreased. The high catalytic activity and selectivity of Pt-Ru/Fe₃O₄/Cnanoparticles are attributed to electron transfer between the two metals and Fe₃O₄.

Key words: Selective hydrogenation, Solvent-free, Chloronitrobenzene, Chloroaniline, Ferroferric oxide, Platinum, Ruthenium

MSC2000:

O643

WANG Ya-Nan, YANG Yu-Xia, LI Yong-Wen, LAI Jun-Hua, SUN Kun-Peng. Preparation of Fe₃O₄ Modified Pt-Ru/C Nanocatalysts and Their Catalytic Properties for the Selective Hydrogenation of ortho-Chloronitrobenzene under Solvent-Free Conditions[J].Acta Phys. -Chim. Sin., 2013, 29(10): 2239-2244.

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Preparation of Fe₃O₄ Modified Pt-Ru/C Nanocatalysts and Their Catalytic Properties for the Selective Hydrogenation of ortho-Chloronitrobenzene under Solvent-Free Conditions

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Preparation of Fe3O4 Modified Pt-Ru/C Nanocatalysts and Their Catalytic Properties for the Selective Hydrogenation of ortho-Chloronitrobenzene under Solvent-Free Conditions

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Preparation of Fe₃O₄ Modified Pt-Ru/C Nanocatalysts and Their Catalytic Properties for the Selective Hydrogenation of ortho-Chloronitrobenzene under Solvent-Free Conditions