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MIL-101笼内铂纳米粒子的原子层沉积:一种温和且可循环使用的氢化催化剂。

Atomic Layer Deposition of Pt Nanoparticles within the Cages of MIL-101: A Mild and Recyclable Hydrogenation Catalyst.

作者信息

Leus Karen, Dendooven Jolien, Tahir Norini, Ramachandran Ranjith K, Meledina Maria, Turner Stuart, Van Tendeloo Gustaaf, Goeman Jan L, Van der Eycken Johan, Detavernier Christophe, Van Der Voort Pascal

机构信息

Department of Inorganic and Physical Chemistry, Center for Ordered Materials, Organometallics and Catalysis (COMOC), Ghent University, Krijgslaan 281-S3, B-9000 Ghent, Belgium.

Department of Solid State Sciences, Conformal Coatings on Nanomaterials (CoCooN), Ghent University, Krijgslaan 281-S1, B-9000 Ghent, Belgium.

出版信息

Nanomaterials (Basel). 2016 Mar 9;6(3):45. doi: 10.3390/nano6030045.

Abstract

We present the synthesis of Pt nanoparticles within MIL-101-Cr (MIL = Materials Institute Lavoisier) by means of atomic layer deposition (ALD). The obtained Pt@MIL-101 materials were characterized by means of N₂ adsorption and X-ray powder diffraction (XRPD) measurements, showing that the structure of the metal organic framework was well preserved during the ALD deposition. X-ray fluorescence (XRF) and transmission electron microscopy (TEM) analysis confirmed the deposition of highly dispersed Pt nanoparticles with sizes determined by the MIL-101-Cr pore sizes and with an increased Pt loading for an increasing number of ALD cycles. The Pt@MIL-101 material was examined as catalyst in the hydrogenation of different linear and cyclic olefins at room temperature, showing full conversion for each substrate. Moreover, even under solvent free conditions, full conversion of the substrate was observed. A high concentration test has been performed showing that the Pt@MIL-101 is stable for a long reaction time without loss of activity, crystallinity and with very low Pt leaching.

摘要

我们通过原子层沉积(ALD)法在MIL-101-Cr(MIL = 拉瓦锡材料研究所)中合成了铂纳米颗粒。通过N₂吸附和X射线粉末衍射(XRPD)测量对所得的Pt@MIL-101材料进行了表征,结果表明在ALD沉积过程中金属有机骨架的结构得到了很好的保留。X射线荧光(XRF)和透射电子显微镜(TEM)分析证实了高度分散的铂纳米颗粒的沉积,其尺寸由MIL-101-Cr的孔径决定,并且随着ALD循环次数的增加,铂负载量也增加。对Pt@MIL-101材料在室温下用于不同线性和环状烯烃氢化反应的催化剂性能进行了研究,结果表明每种底物都能实现完全转化。此外,即使在无溶剂条件下,也观察到底物的完全转化。进行了高浓度测试,结果表明Pt@MIL-101在长时间反应中保持稳定,没有活性损失、结晶度损失,并且铂的浸出率非常低。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f53a/5302512/3b3e7f0d3ea3/nanomaterials-06-00045-g001.jpg

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