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利用X射线吸收光谱（XAS）和漫反射红外傅里叶变换光谱（DRIFT）光谱来理解负载型铑原子和团簇在氢甲酰化反应和CO加氢反应中的作用。

Understanding the role of supported Rh atoms and clusters during hydroformylation and CO hydrogenation reactions with / XAS and DRIFT spectroscopy.

作者信息

Sarma Bidyut Bikash, Neukum Dominik, Doronkin Dmitry E, Lakshmi Nilayam Ajai Raj, Baumgarten Lorena, Krause Bärbel, Grunwaldt Jan-Dierk

机构信息

Institute for Chemical Technology and Polymer Chemistry, Karlsruhe Institute of Technology (KIT) Engesserstraße 20 76131 Karlsruhe Germany.

Institute of Catalysis Research and Technology, KIT Hermann-von Helmholtz Platz 1 76344 Eggenstein-Leopoldshafen Germany.

出版信息

Chem Sci. 2024 Jul 10;15(31):12369-12379. doi: 10.1039/d4sc02907k. eCollection 2024 Aug 7.

DOI:10.1039/d4sc02907k
PMID:39118611
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11304778/
Abstract

Supported Rh single-atoms and clusters on CeO, MgO, and ZrO were investigated as catalysts for hydroformylation of ethylene to propionaldehyde and CO hydrogenation to methanol/ethanol with / diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and X-ray absorption spectroscopy (XAS). Under hydroformylation reaction conditions, spectroscopic investigations unravel the presence of both single atoms and clusters and detected at first propanal and then methanol. We find that the formation of methanol is associated with CO hydrogenation over Rh clusters which was further confirmed under CO hydrogenation conditions at elevated pressure. The activity of catalysts synthesized a precipitation (PP) method over various supports towards the hydroformylation reaction follows the order: Rh/ZrO > Rh/CeO > Rh/MgO. Comparing Rh/CeO catalysts synthesized different methods, catalysts prepared by flame spray pyrolysis (FSP) showed catalytic activity for the hydroformylation reaction at lower temperatures (413 K), whereas catalysts prepared by wet impregnation (WI) showed the highest stability. These results not only provide fundamental insights into the atomistic level of industrially relevant reactions but also pave the way for a rational design of new catalysts in the future.

摘要

通过漫反射红外傅里叶变换光谱（DRIFTS）和X射线吸收光谱（XAS），研究了负载在CeO、MgO和ZrO上的Rh单原子和团簇作为乙烯氢甲酰化制丙醛以及CO加氢制甲醇/乙醇的催化剂。在氢甲酰化反应条件下，光谱研究揭示了单原子和团簇的存在，并首先检测到丙醛，然后是甲醇。我们发现甲醇的形成与Rh团簇上的CO加氢有关，这在高压下的CO加氢条件下得到了进一步证实。通过沉淀（PP）法在各种载体上合成的催化剂对氢甲酰化反应的活性顺序为：Rh/ZrO＞Rh/CeO＞Rh/MgO。比较通过不同方法合成的Rh/CeO催化剂，通过火焰喷雾热解（FSP）制备的催化剂在较低温度（413K）下对氢甲酰化反应表现出催化活性，而通过湿浸渍（WI）制备的催化剂表现出最高的稳定性。这些结果不仅为工业相关反应的原子水平提供了基本见解，也为未来新型催化剂的合理设计铺平了道路。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f0af/11304778/639861213b8f/d4sc02907k-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f0af/11304778/3a9ed117db4b/d4sc02907k-f1.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f0af/11304778/567230fd008a/d4sc02907k-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f0af/11304778/bcab228c1511/d4sc02907k-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f0af/11304778/2c40e1cac444/d4sc02907k-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f0af/11304778/681b32e36843/d4sc02907k-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f0af/11304778/639861213b8f/d4sc02907k-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f0af/11304778/3a9ed117db4b/d4sc02907k-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f0af/11304778/80a7af055a56/d4sc02907k-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f0af/11304778/567230fd008a/d4sc02907k-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f0af/11304778/bcab228c1511/d4sc02907k-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f0af/11304778/2c40e1cac444/d4sc02907k-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f0af/11304778/681b32e36843/d4sc02907k-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f0af/11304778/639861213b8f/d4sc02907k-f7.jpg

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本文引用的文献

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Low-temperature hydroformylation of ethylene by phosphorous stabilized Rh sites in a one-pot synthesized Rh-(O)-P-MFI zeolite.通过一锅法合成的Rh-(O)-P-MFI沸石中磷稳定的Rh位点实现乙烯的低温氢甲酰化反应。
Nat Commun. 2023 Nov 7;14(1):7174. doi: 10.1038/s41467-023-42938-4.
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Ethene Hydroformylation Catalyzed by Rhodium Dispersed with Zinc or Cobalt in Silanol Nests of Dealuminated Zeolite Beta.
铑与锌或钴分散在脱铝β沸石硅醇巢中催化乙烯氢甲酰化反应
J Am Chem Soc. 2023 Feb 8;145(5):2911-2929. doi: 10.1021/jacs.2c11075. Epub 2023 Jan 30.
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