Novel Rh catalytic systems based on microporous metal-organic framework MIL-53(Al) for “green” ethylene hydroformylation

IF 3.2 4区材料科学 Q2 CHEMISTRY, APPLIED

Journal of Porous Materials Pub Date : 2024-10-23 DOI:10.1007/s10934-024-01695-5

Vera I. Isaeva, Andrei L. Tarasov, Olga P. Tkachenko, Sergei V. Savilov, Nikolai A. Davshan, Vladimir V. Chernyshev, Leonid M. Kustov

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Abstract

Novel hybrid nanomaterials were synthesized using microporous metal-organic framework MIL-53(Al) as a support for rhodium nanoparticles (Rh NPs). In order to elucidate the factors that govern the dispersion and location of Rh, MIL-53(Al) samples were synthesized using two alternative strategies: conventional solvothermal procedure and microwave (MW) activation of the reaction mass. It was established that the use of different preparation conditions for the synthesis of the MIL-53(Al) carrier results in the spatial manipulation of the structural characteristics of the Rh@MIL-53(Al) nanohybrids. The structural study revealed also a pronounced confinement effect of the MIL-53(Al) porous matrix for the Rh nanoparticles. The novel Rh@MIL-53(Al) nanohybrids show high efficiency in “green” ethylene hydroformylation into propionic aldehyde (propanal) using syngas produced by CO₂ hydrogenation. Carbon dioxide hydrogenation (atmospheric pressure, 500^oC) was performed over cobalt nanoparticles deposited on the MIL-53(Al) nanomaterial obtained in MW fields. Exceptionally high thermal stability of the MIL-53(Al) matrix under conditions of the two-stage catalytic process was found. This work results demonstrate the new potential of the nanostructured catalysts based on the MIL-53(Al) carrier in the carbon dioxide conversion into value-added products.

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基于微孔金属-有机骨架MIL-53（Al）的新型Rh催化体系用于“绿色”乙烯氢甲酰化

以微孔金属-有机骨架MIL-53（Al）为载体，制备了新型杂化纳米材料。为了阐明影响Rh分散和定位的因素，采用常规溶剂热法和微波活化两种方法合成了MIL-53（Al）样品。结果表明，不同制备条件下MIL-53（Al）载体的合成会对Rh@MIL-53（Al）纳米杂化物的结构特性产生空间上的影响。结构研究还揭示了MIL-53（Al）多孔基质对Rh纳米颗粒的明显约束效应。新型Rh@MIL-53（Al）纳米杂化物在利用CO2加氢产生的合成气将乙烯氢甲酰化成丙醛方面表现出高效率。在MW场制备的MIL-53（Al）纳米材料上，对钴纳米颗粒进行了二氧化碳加氢（大气压，500℃）处理。发现MIL-53（Al）基体在两段催化条件下具有极高的热稳定性。这一研究结果显示了基于MIL-53（Al）载体的纳米结构催化剂在二氧化碳转化为增值产品方面的新潜力。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Journal of Porous Materials 工程技术-材料科学：综合

CiteScore

4.80

自引率

7.70%

发文量

203

审稿时长

2.6 months

期刊介绍： The Journal of Porous Materials is an interdisciplinary and international periodical devoted to all types of porous materials. Its aim is the rapid publication of high quality, peer-reviewed papers focused on the synthesis, processing, characterization and property evaluation of all porous materials. The objective is to establish a unique journal that will serve as a principal means of communication for the growing interdisciplinary field of porous materials. Porous materials include microporous materials with 50 nm pores. Examples of microporous materials are natural and synthetic molecular sieves, cationic and anionic clays, pillared clays, tobermorites, pillared Zr and Ti phosphates, spherosilicates, carbons, porous polymers, xerogels, etc. Mesoporous materials include synthetic molecular sieves, xerogels, aerogels, glasses, glass ceramics, porous polymers, etc.; while macroporous materials include ceramics, glass ceramics, porous polymers, aerogels, cement, etc. The porous materials can be crystalline, semicrystalline or noncrystalline, or combinations thereof. They can also be either organic, inorganic, or their composites. The overall objective of the journal is the establishment of one main forum covering the basic and applied aspects of all porous materials.