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金属有机框架作为催化剂载体：晶格无序对金属纳米颗粒形成的影响。

Metal-Organic Frameworks as Catalyst Supports: Influence of Lattice Disorder on Metal Nanoparticle Formation.

机构信息

Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584, CG, Utrecht, The Netherlands.

Aix-Marseille University, CNRS, MADIREL (UMR 7246), Centre de St Jérôme, 13013, Marseille Cedex, France.

出版信息

Chemistry. 2018 May 23;24(29):7498-7506. doi: 10.1002/chem.201800694. Epub 2018 Apr 30.

DOI:10.1002/chem.201800694
PMID:29709084
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6519236/
Abstract

Because of their high tunability and surface area, metal-organic frameworks (MOFs) show great promise as supports for metal nanoparticles. Depending on the synthesis route, MOFs may contain defects. Here, we show that highly crystalline MIL-100(Fe) and disordered Basolite® F300, with identical iron 1,3,5-benzenetricarboxylate composition, exhibit very divergent properties when used as a support for Pd nanoparticle deposition. While MIL-100(Fe) shows a regular MTN-zeotype crystal structure with two types of cages, Basolite® F300 lacks long-range order beyond 8 Å and has a single-pore system. The medium-range configurational linker-node disorder in Basolite® F300 results in a reduced number of Lewis acid sites, yielding more hydrophobic surface properties compared to hydrophilic MIL-100(Fe). The hydrophilic/hydrophobic nature of MIL-100(Fe) and Basolite® F300 impacts the amount of Pd and particle size distribution of Pd nanoparticles deposited during colloidal synthesis and dry impregnation methods, respectively. It is suggested that polar (apolar) solvents/precursors attractively interact with hydrophilic (hydrophobic) MOF surfaces, allowing tools at hand to increase the level of control over, for example, the nanoparticle size distribution.

摘要

由于其高度可调性和表面积，金属有机骨架（MOFs）作为金属纳米粒子的载体具有很大的应用前景。根据合成路线的不同，MOFs 可能含有缺陷。在这里，我们表明，高度结晶的 MIL-100(Fe) 和无序的 Basolite® F300，具有相同的铁 1,3,5-苯三甲酸酯组成，在用作 Pd 纳米粒子沉积的载体时表现出非常不同的性质。虽然 MIL-100(Fe) 具有两种笼型的规则 MTN-zeotype 晶体结构，但 Basolite® F300 的长程有序性超过 8 Å 后不存在，并且具有单孔系统。Basolite® F300 中的中程构象连接点无序导致路易斯酸位点数减少，与亲水性的 MIL-100(Fe) 相比，表面具有更多的疏水性。MIL-100(Fe) 和 Basolite® F300 的亲水性/疏水性影响胶体合成和干浸渍法期间沉积的 Pd 的量和 Pd 纳米粒子的粒径分布。有人认为，极性（非极性）溶剂/前体与亲水性（疏水性）MOF 表面具有吸引力，从而使我们手头的工具能够更好地控制例如纳米粒子的粒径分布。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/3330a51af78f/CHEM-24-7498-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/95df47000d20/CHEM-24-7498-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/aa8b42098f07/CHEM-24-7498-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/fbb522a0eff5/CHEM-24-7498-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/35a26677710d/CHEM-24-7498-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/32e5603d43cd/CHEM-24-7498-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/afaced0be098/CHEM-24-7498-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/b926adc0cb8e/CHEM-24-7498-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/54bebbcfb7b7/CHEM-24-7498-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/3330a51af78f/CHEM-24-7498-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/95df47000d20/CHEM-24-7498-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/aa8b42098f07/CHEM-24-7498-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/fbb522a0eff5/CHEM-24-7498-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/35a26677710d/CHEM-24-7498-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/32e5603d43cd/CHEM-24-7498-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/afaced0be098/CHEM-24-7498-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/b926adc0cb8e/CHEM-24-7498-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/54bebbcfb7b7/CHEM-24-7498-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fa/6519236/3330a51af78f/CHEM-24-7498-g009.jpg

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