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首页> 外文期刊>Catalysis science & technology >Highly stable Pd2+ species anchoring on ethylenediamine-grafted-MIL-101(Cr) as a robust oxidation catalyst
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Highly stable Pd2+ species anchoring on ethylenediamine-grafted-MIL-101(Cr) as a robust oxidation catalyst

机译：高度稳定的PD2+种类锚定在乙二胺 - 移植米尔-101（CR）上的物种作为强大的氧化催化剂

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摘要

Highly stable Pd2+ species were anchored on ethylenediamine-grafted MIL-101(Cr). Ethylenediamine (0.3–1.2 mmol g−1) was first grafted onto MIL-101(Cr), then Pd2+ (0.03–0.2 mmol Pd per g) was incorporated by double-solvent adsorption. Fourier transform infrared, inductively coupled plasma-optical emission spectroscopy, transmission electron microscopy and CHN analysis confirmed the incorporation of ethylenediamine and Pd2+ in MIL-101(Cr). X-ray photoelectron and Raman spectroscopy suggested that one amino moiety of ethylenediamine coordinated with the Cr3+ nodes of MIL-101(Cr). The other served as an anchoring site for the incorporated Pd2+ species. In situ X-ray absorption near-edge structure analysis showed that the strong interaction between Pd2+ and ethylenediamine, within the confinement of the MIL-101(Cr) structure, effectively prevented reduction to Pd0, even in the presence of H2 at 150 °C. At relatively low temperatures, the catalysts with ethylenediamine : Pd2+ molar ratios of 10 provided a higher activity for styrene oxidation (TOF ∼30 h−1), as compared to previous reports. The presence of ethylenediamine as an anchoring ligand also inhibited the reduction of Pd2+ by the feed (styrene) and minimized leaching of the active Pd2+ species under oxidizing and acidic conditions. The Pd2+ species anchoring on ethylenediamine-grafted-MIL-101(Cr) exhibited an improved catalytic activity and stability, as compared to typical liquid-phase oxidation catalysts.
机译：高度稳定的PD2+物种锚定在乙二胺移植的MIL-101（CR）上。首先将乙二胺（0.3–1.2 mmol G-1）接枝到MIL-101（CR）上，然后通过双溶剂吸附掺入PD2+（0.03-0.2 mmol PD）。傅立叶变换红外，电感耦合等离子光光谱，透射电子显微镜和CHN分析证实了在MIL-101（CR）中掺入乙二胺和PD2+。 X射线光电子和拉曼光谱法表明，乙二胺的一个氨基部分与MIL-101（CR）的CR3+节点协调。另一个是掺入PD2+物种的锚定位点。原位X射线吸收接近边缘结构分析表明，在MIL-101（CR）结构的限制内，PD2+和乙二胺之间的强相互作用有效地阻止了PD0的降低，即使在150°C下H2也存在下来。在相对较低的温度下，与先前的报道相比，乙二胺：PD2+摩尔比为10的催化剂为苯乙烯氧化（TOF约30 h -1）提供了更高的活性。在氧化和酸性条件下，乙二胺作为一种锚定配体的存在也抑制了饲料（苯乙烯）的降低（苯乙烯），并最大程度地减少活性PD2+物种的浸出。与典型的液相相氧化催化剂相比，锚定在乙二胺氨基氨基氨基氨基氨基氨基氨基-101（CR）上的PD2+物种表现出改善的催化活性和稳定性。

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