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1. Carbonylation Reactions Using Single‐Atom Catalysts.

Author

Jurado, Lole, Posada‐Pérez, Sergio, and Axet, M. Rosa

Subjects
HETEROGENEOUS catalysts, CARBONYLATION, HYDROFORMYLATION, METHYL ether, CATALYSTS, ETHANOL
Abstract

The development of highly efficient and selective catalysts for carbonylation reactions represents a significant challenge in catalysis. Single‐atom catalysts (SACs) have postulated as promising candidates able to combine the strengths of both homogeneous and heterogeneous catalysts. In this paper, we review recent advances in tailoring solid supports for SACs to enhance their catalytic performance in carbonylation reactions. We first discuss the effect of supports on the hydroformylation reaction catalysed by SACs, followed by recent advances for methanol, ethanol, and dimethyl ether carbonylation reactions, focusing on the design of halide‐free catalysts with improved activity and stability. Finally, oxidative carbonylation is discussed. Overall, this review highlights the importance of tailoring solid supports for SACs to achieve highly active and selective catalysts in carbonylation reactions, paving the way for future developments in sustainable catalysis. [ABSTRACT FROM AUTHOR]

Published
2024
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2. Colloidal Bimetallic RuNi Particles and their Behaviour in Catalytic Quinoline Hydrogenation.

Author

Cardona‐Farreny, Miquel, Ishikawa, Hiroya, Odufejo Ogoe, Abolanle Olatilewa, Mallet‐Ladeira, Sonia, Coppel, Yannick, Lecante, Pierre, Esvan, Jerome, Philippot, Karine, and Axet, M. Rosa

Subjects
STABILIZING agents, BIMETALLIC catalysts, METAL nanoparticles, HETEROGENEOUS catalysis, PRECIOUS metals, RUTHENIUM catalysts
Abstract

Colloidal metal nanoparticles exhibit interesting catalytic properties for the hydrogenation of (hetero)arenes. Catalysts based on precious metals, such as Ru and Rh, promote this reaction efficiently under mild reaction conditions. In contrast, heterogeneous catalysts based on earth‐abundant metals can selectively hydrogenate (hetero)arenes but require harsher reaction conditions. Bimetallic catalysts that combine precious and earth‐abundant metals are interesting materials to mitigate the drawbacks of each component. To this end, RuNi nanoparticles bearing a phosphine ligand were prepared through the decomposition of [Ru(η4‐C8H12)(η6‐C8H10)] and [Ni(η4‐C8H12)2] by H2 at 85 °C. Wide angle X‐ray scattering confirmed a bimetallic segregated structure, with Ni predominantly on the surface. Spectroscopic analyses revealed that the phosphine ligand coordinated to the surface of both metals, suggesting, as well, a partial Ni shell covering the Ru core. The RuNi‐based nanomaterials were used as catalysts in the hydrogenation of quinoline to assess the impact of the metallic composition and of the stabilizing agent on their catalytic performance. [ABSTRACT FROM AUTHOR]

Published
2024
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5. Highly dispersed Rh single atoms over graphitic carbon nitride as a robust catalyst for the hydroformylation reaction

Author

Instituto de Salud Carlos III, Centre National de la Recherche Scientifique (France), Agencia Estatal de Investigación (España), Ministerio de Ciencia e Innovación (España), European Commission, Jurado, Lole[0000-0003-1908-899X], Luque-Álvarez, Ligia A[0000-0002-3998-580X], Bobadilla, Luis F.[0000-0003-0085-9811], Odriozola, José Antonio[0000-0002-8283-0459], Poater, Albert[0000-0002-8997-2599], Comas-Vives, Aleix[0000-0002-7002-1582], Axet, M Rosa[0000-0002-2483-1533], Jurado, Lole, Esvan, Jerome, Luque-Álvarez, Ligia A, Bobadilla, Luis F, Odriozola, José Antonio, Posada-Pérez, Sergio, Poater, Albert, Comas-Vives, Aleix, Axet, M Rosa, Instituto de Salud Carlos III, Centre National de la Recherche Scientifique (France), Agencia Estatal de Investigación (España), Ministerio de Ciencia e Innovación (España), European Commission, Jurado, Lole[0000-0003-1908-899X], Luque-Álvarez, Ligia A[0000-0002-3998-580X], Bobadilla, Luis F.[0000-0003-0085-9811], Odriozola, José Antonio[0000-0002-8283-0459], Poater, Albert[0000-0002-8997-2599], Comas-Vives, Aleix[0000-0002-7002-1582], Axet, M Rosa[0000-0002-2483-1533], Jurado, Lole, Esvan, Jerome, Luque-Álvarez, Ligia A, Bobadilla, Luis F, Odriozola, José Antonio, Posada-Pérez, Sergio, Poater, Albert, Comas-Vives, Aleix, and Axet, M Rosa

Abstract

Rhodium-catalysed hydroformylation, effective tool in bulk and fine-chemical synthesis, predominantly uses soluble metal complexes. For that reason, the metal leaching and the catalyst recycling are still the major drawbacks of this process. Single-atom catalysts have emerged as a powerful tool to combine the advantages of both homogeneous and heterogeneous catalysts. Since using an appropriate support material is key to create stable, finely dispersed, single-atom catalysts, here we show that Rh atoms anchored on graphitic carbon nitride are robust catalysts for the hydroformylation reaction of styrene.

Published
2023

9. Colloidal ruthenium catalysts for selective quinaldine hydrogenation: Ligand and solvent effects.

Author

Colliere, Vincent, Verelst, Marc, Lecante, Pierre, and Axet, M. Rosa

Subjects
RUTHENIUM catalysts, CATALYST selectivity, HYDROGENATION, STABILIZING agents, CATALYTIC hydrogenation, CATALYSTS
Abstract

Colloidal Ru nanoparticles (NP) display interesting catalytic properties for the hydrogenation of (hetero)arenes as they proceed efficiently in mild reaction conditions. In this work, a series of Ru based materials was used in order to selectively hydrogenate quinaldine and assess the impact of the stabilizing agent on their catalytic performances. Ru nanoparticles stabilized with polyvinylpyrrolidone (PVP) and 1‐adamantanecarboxylic acid (AdCOOH) allowed to obtain 5,6,7,8‐tetrahydroquinaldine with a remarkable selectivity in mild reaction conditions by choosing the suitable solvent. The presence of a carboxylate ligand on the surface of the Ru NP led to an increase in the activity when compared to Ru/PVP catalyst. The stabilizing agent had also an impact on the selectivity, as carboxylate ligand modified catalysts promoted the selectivity towards 1,2,3,4‐tetrahydroquinaldine, with bulky carboxylate displaying the highest ones. [ABSTRACT FROM AUTHOR]

Published
2024
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11. Highly Dispersed Rh Single Atoms over Graphitic Carbon Nitride as a Robust Catalyst for the Hydroformylation Reaction

Author

Universidad de Sevilla. Departamento de Química Inorgánica, Ministerio de Ciencia e Innovación (MICIN). España, European Commission. Fondo Social Europeo (FSO), European Union (UE), Jurado, Lole, Esvan, Jerome, Luque Álvarez, Ligia Amelia, Bobadilla Baladrón, Luis Francisco, Odriozola Gordón, José Antonio, Posada Pérez, Sergio, Poater, Albert, Comas Vives, Aleix, Axet, M. Rosa, Universidad de Sevilla. Departamento de Química Inorgánica, Ministerio de Ciencia e Innovación (MICIN). España, European Commission. Fondo Social Europeo (FSO), European Union (UE), Jurado, Lole, Esvan, Jerome, Luque Álvarez, Ligia Amelia, Bobadilla Baladrón, Luis Francisco, Odriozola Gordón, José Antonio, Posada Pérez, Sergio, Poater, Albert, Comas Vives, Aleix, and Axet, M. Rosa

Abstract

Rhodium-catalysed hydroformylation, effective tool in bulk and fine-chemical synthesis, predominantly uses soluble metal complexes. For that reason, the metal leaching and the catalyst recycling are still the major drawbacks of this process. Single-atom catalysts have emerged as a powerful tool to combine the advantages of both homogeneous and heterogeneous catalysts. Since using an appropriate support material is key to create stable, finely dispersed, single-atom catalysts, here we show that Rh atoms anchored on graphitic carbon nitride are robust catalysts for the hydroformylation reaction of styrene.

Published
2023

12. Ruthenium Nanoparticles Stabilized with Methoxy-Functionalized Ionic Liquids:Synthesis and Structure–Performance Relations in Styrene Hydrogenation

Author

Krishnan, Deepthy, Schill, Leonhard, Axet, M. Rosa, Philippot, Karine, Riisager, Anders, Krishnan, Deepthy, Schill, Leonhard, Axet, M. Rosa, Philippot, Karine, and Riisager, Anders

Abstract

A series of ruthenium nanoparticles (RuNPs) were synthesized by the organometallic approach in different functionalized imidazolium ionic liquids (FILs). Transmission electron microscopy (TEM) showed well-dispersed and narrow-sized RuNPs ranging from 1.3 to 2.2 nm, depending on the IL functionalization. Thermal gravimetric analysis (TGA) and X-ray photoelectron spectroscopy (XPS) allowed the interaction between the RuNPs and the ILs to be studied. The RuNPs stabilized by methoxy-based FILs (MEM and MME) displayed a good balance between catalytic activity and stability when evaluated in the hydrogenation of styrene (S) under mild reaction conditions. Moreover, the catalysts showed total selectivity towards ethylbenzene (EB) under milder reaction conditions (5 bar, 30 °C) than reported in the literature for other RuNP catalysts.

Published
2023

22. Nanocatalysts for High Selectivity Enyne Cyclization: Oxidative Surface Reorganization of Gold Sub-2-nm Nanoparticle Networks

Author

Nasrallah, Houssein O., primary, Min, Yuanyuan, additional, Lerayer, Emmanuel, additional, Nguyen, Tuan-Anh, additional, Poinsot, Didier, additional, Roger, Julien, additional, Brandès, Stéphane, additional, Heintz, Olivier, additional, Roblin, Pierre, additional, Jolibois, Franck, additional, Poteau, Romuald, additional, Coppel, Yannick, additional, Kahn, Myrtil L., additional, Gerber, Iann C., additional, Axet, M. Rosa, additional, Serp, Philippe, additional, and Hierso, Jean-Cyrille, additional

Published
2021
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24. 2D and 3D Ruthenium Nanoparticle Covalent Assemblies for Phenyl Acetylene Hydrogenation

Author

Min, Yuanyuan, primary, Leng, Faqiang, additional, Machado, Bruno F., additional, Lecante, Pierre, additional, Roblin, Pierre, additional, Martinez, Hervé, additional, Theussl, Thomas, additional, Casu, Alberto, additional, Falqui, Andrea, additional, Barcenilla, María, additional, Coco, Silverio, additional, Martínez, Beatriz María Illescas, additional, Martin, Nazario, additional, Axet, M. Rosa, additional, and Serp, Philippe, additional

Published
2020
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27. 3D Ruthenium Nanoparticle Covalent Assemblies from Polymantane Ligands for Confined Catalysis

Author

Min, Yuanyuan, primary, Nasrallah, Houssein, additional, Poinsot, Didier, additional, Lecante, Pierre, additional, Tison, Yann, additional, Martinez, Hervé, additional, Roblin, Pierre, additional, Falqui, Andrea, additional, Poteau, Romuald, additional, del Rosal, Iker, additional, Gerber, Iann C., additional, Hierso, Jean-Cyrille, additional, Axet, M. Rosa, additional, and Serp, Philippe, additional

Published
2020
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33. Organometallic quinonoid linkers: a versatile tether for the design of panchromatic ruthenium(II) heteroleptic complexes

Author

Damas, Aurelie, Ventura, Barbara, Axet, M. Rosa, Esposti, Alessandra Degli, Chamoreau, Lise-Marie, Barbieri, Andrea, and Amouri, Hani

Subjects
Organometallic compounds -- Structure, Organometallic compounds -- Chemical properties, Pyridine -- Structure, Pyridine -- Chemical properties, Ruthenium -- Chemical properties, X-ray crystallography -- Usage, Chemistry
Published
2010

34. Carbon Nanotube Nanoreactors for Chemical Transformations

Author

Axet, M. Rosa, Serp, Philippe, Laboratoire de chimie de coordination (LCC), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie de Toulouse (ICT-FR 2599), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), and Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Confinement effects, Carbon nanotubes, [CHIM.COOR]Chemical Sciences/Coordination chemistry, Electronic effects, Spatial restriction, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, Gas and liquid diffusion, Catalysis
Abstract

International audience; The confinement of molecules or materials in carbon nanotubes (CNTs) may generate unique one-dimensional supramolecular nanostructures that may bring forth novel electronic, magnetic, and chemical properties. The nature of the confinement effects can be either physical or chemical. The physical nature is related to space restriction in the CNT channels. The chemical factors are related to the chemical nature of the pores, which influences the interaction of the confined phase with the pore wall. Apparently all of these effects can influence chemical transformations, catalytic or not, with the extent of the influence depending on the selected catalysts (if any), the diameter of CNTs, and the specific reactions being carried out. Although wide efforts have been made to assess the relative importance of each factor in order to gain fundamental insights, they are still, in most cases, rather difficult to clearly identify.

Published
2016

35. Hexakis [60]Fullerene Adduct‐Mediated Covalent Assembly of Ruthenium Nanoparticles and Their Catalytic Properties

Author

Leng, Faqiang, primary, Gerber, Iann C., additional, Lecante, Pierre, additional, Bentaleb, Ahmed, additional, Muñoz, Antonio, additional, Illescas, Beatriz M., additional, Martín, Nazario, additional, Melinte, Georgian, additional, Ersen, Ovidiu, additional, Martinez, Hervé, additional, Axet, M. Rosa, additional, and Serp, Philippe, additional

Published
2017
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39. Chemoselective reduction of quinoline over Rh–C60nanocatalystsElectronic supplementary information (ESI) available. See DOI: 10.1039/c9cy02025j

Author

Luo, Zhishan, Min, Yuanyuan, Nechiyil, Divya, Bacsa, Wolfgang, Tison, Yann, Martinez, Hervé, Lecante, Pierre, Gerber, Iann C., Serp, Philippe, and Axet, M. Rosa

Abstract

The design and engineering of heterogeneous nanocatalysts that are both highly active and selective for hydrogenation reactions constitute a crucial challenge. In that context, herein a series of Rh–C60nanocatalysts have been synthesized viathe decomposition of an organometallic rhodium complex in the presence of fullerene C60under a H2atmosphere. Rhodium atomically dispersed or rhodium nanoparticles on Rh–C60spherical fulleride particles were produced by tuning the Rh/C60molar ratio. Significant charge transfer between rhodium and C60was evidenced through Raman and X-ray photoelectron spectroscopy, which indicates electron-deficient Rh species. The resulting heterostructured nanomaterials were applied successfully in the catalytic hydrogenation of quinoline, exhibiting excellent activity and producing selectively the partially hydrogenated product, 1,2,3,4-tetrahydroquinoline. Density functional theory (DFT) calculations show that the hydride coverage of the Rh NPs plays a key role in the adsorption modes of quinoline and 1,2,3,4-tetrahydroquinoline on the surface of the NPs, and that these adsorption modes are modulated by the presence of fullerene C60, thus affecting the activity and selectivity obtained with this rhodium based catalyst.

Published
2019
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41. Gold Compounds Anchored to a Metalated Arene Scaffold: Synthesis, X-ray Molecular Structures, and Cycloisomerization of Enyne

Author

Dubarle-Offner, Julien, primary, Barbazanges, Marion, additional, Augé, Mylène, additional, Desmarets, Christophe, additional, Moussa, Jamal, additional, Axet, M. Rosa, additional, Ollivier, Cyril, additional, Aubert, Corinne, additional, Fensterbank, Louis, additional, Gandon, Vincent, additional, Malacria, Max, additional, Gontard, Geoffrey, additional, and Amouri, Hani, additional

Published
2013
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44. Metalated-Arene-Phosphino Ligands: A Novel Approach to Open-Sided Gold Compounds

Author

Axet, M. Rosa, primary, Barbazanges, Marion, additional, Augé, Mylène, additional, Desmarets, Christophe, additional, Moussa, Jamal, additional, Ollivier, Cyril, additional, Aubert, Corinne, additional, Fensterbank, Louis, additional, Gandon, Vincent, additional, Malacria, Max, additional, Chamoreau, Lise Marie, additional, and Amouri, Hani, additional

Published
2010
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46. Application of Chiral Amine-Imine Ligands in Palladium-Catalyzed Polyketone Synthesis: Effect of Ligand Backbone on the Polymer Stereochemistry

Author

Axet, M. Rosa, primary, Amoroso, Francesco, additional, Bottari, Giovanni, additional, D’Amora, Angela, additional, Zangrando, Ennio, additional, Faraone, Felice, additional, Drommi, Dario, additional, Saporita, Maria, additional, Carfagna, Carla, additional, Natanti, Paolo, additional, Seraglia, Roberta, additional, and Milani, Barbara, additional

Published
2009
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