Effect of the size and distribution of supported Ru nanoparticles on their activity in ammonia synthesis under mild reaction conditions

•A larger size of Ru nanoparticles leads to a higher (TOF).•Heterogeneous distribution of the size of Ru nanoparticles favors higher TOF.•Homogeneous distribution of size of Ru nanoparticles leads to lower TOF. Ru/γ-Al2O3 catalysts were prepared using three different methods: wet impregnation, collo...

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Vydané v:	Applied catalysis. A, General Ročník 474; číslo SI; s. 194 - 202
Hlavní autori:	Fernández, Camila, Sassoye, Capucine, Debecker, Damien P., Sanchez, Clément, Ruiz, Patricio
Médium:	Journal Article
Jazyk:	English
Vydavateľské údaje:	Kidlington Elsevier B.V 22.03.2014 Elsevier
Predmet:	Activation Ammonia Catalysis Catalysts Catalytic cooperation Chemical Sciences Chemistry Colloidal state and disperse state Exact sciences and technology General and physical chemistry Low-temperature ammonia synthesis Material chemistry Nanoparticle Nanoparticles Physical and chemical studies. Granulometry. Electrokinetic phenomena Ru supported catalyst Size distribution Surface chemistry Synthesis Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry X-ray photoelectron spectroscopy Catalytic cooperation Size distribution Ru supported catalyst Nanoparticle Low-temperature ammonia synthesis Ammonia Heterogeneous catalysis Catalytic reaction Synthesis Support Supported catalyst Low temperature
ISSN:	0926-860X, 1873-3875
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Abstract	•A larger size of Ru nanoparticles leads to a higher (TOF).•Heterogeneous distribution of the size of Ru nanoparticles favors higher TOF.•Homogeneous distribution of size of Ru nanoparticles leads to lower TOF. Ru/γ-Al2O3 catalysts were prepared using three different methods: wet impregnation, colloidal method and microemulsion. Ru-supported nanoparticles with different average sizes and distribution of sizes were obtained. The catalysts were tested in ammonia synthesis under mild reaction conditions, namely low temperature (100°C) and low pressure (4bar), and characterized by N2 adsorption, XRD, XPS, TEM and TPR techniques. The results indicate that a good catalytic performance can be achieved by Ru supported nanoparticles fulfilling two requirements: (i) a relatively high average size (despite the usual assertion that only small particles are required) and (ii) a broad distribution of sizes that ensures the presence of both small particles, containing highly active sites, and large nanoparticles, which are shown to promote the reaction on small particles. This promotion results from a cooperative effect between small and large nanoparticles in good contact, which also allows keeping a highly reduced surface of ruthenium. It is proposed that, under mild reaction conditions, large Ru nanoparticles promote the ammonia synthesis reaction by allowing a more effective activation and transfer of hydrogen atoms, able to hydrogenate strongly adsorbed nitrogen atoms, and thus to release active sites for the activation of N2.
AbstractList	Ru/ gamma -Al sub(2)O sub(3) catalysts were prepared using three different methods: wet impregnation, colloidal method and microemulsion. Ru-supported nanoparticles with different average sizes and distribution of sizes were obtained. The catalysts were tested in ammonia synthesis under mild reaction conditions, namely low temperature (100 C) and low pressure (4 bar), and characterized by N sub(2) adsorption, XRD, XPS, TEM and TPR techniques. The results indicate that a good catalytic performance can be achieved by Ru supported nanoparticles fulfilling two requirements: (i) a relatively high average size (despite the usual assertion that only small particles are required) and (ii) a broad distribution of sizes that ensures the presence of both small particles, containing highly active sites, and large nanoparticles, which are shown to promote the reaction on small particles. This promotion results from a cooperative effect between small and large nanoparticles in good contact, which also allows keeping a highly reduced surface of ruthenium. It is proposed that, under mild reaction conditions, large Ru nanoparticles promote the ammonia synthesis reaction by allowing a more effective activation and transfer of hydrogen atoms, able to hydrogenate strongly adsorbed nitrogen atoms, and thus to release active sites for the activation of N sub(2). Ru/gamma-Al2O3 catalysts were prepared using three different methods: wet impregnation, colloidal method and microemulsion. Ru-supported nanoparticles with different average sizes and distribution of sizes were obtained. The catalysts were tested in ammonia synthesis under mild reaction conditions, namely low temperature (100 degrees C) and low pressure (4 bar), and characterized by N-2 adsorption, XRD, XPS, TEM and TPR techniques. The results indicate that a good catalytic performance can be achieved by Ru supported nanoparticles fulfilling two requirements: (i) a relatively high average size (despite the usual assertion that only small particles are required) and (ii) a broad distribution of sizes that ensures the presence of both small particles, containing highly active sites, and large nanoparticles, which are shown to promote the reaction on small particles. This promotion results from a cooperative effect between small and large nanoparticles in good contact, which also allows keeping a highly reduced surface of ruthenium. It is proposed that, under mild reaction conditions, large Ru nanoparticles promote the ammonia synthesis reaction by allowing a more effective activation and transfer of hydrogen atoms, able to hydrogenate strongly adsorbed nitrogen atoms, and thus to release active sites for the activation of N2. (c) 2013 Elsevier B.V. All rights reserved. •A larger size of Ru nanoparticles leads to a higher (TOF).•Heterogeneous distribution of the size of Ru nanoparticles favors higher TOF.•Homogeneous distribution of size of Ru nanoparticles leads to lower TOF. Ru/γ-Al2O3 catalysts were prepared using three different methods: wet impregnation, colloidal method and microemulsion. Ru-supported nanoparticles with different average sizes and distribution of sizes were obtained. The catalysts were tested in ammonia synthesis under mild reaction conditions, namely low temperature (100°C) and low pressure (4bar), and characterized by N2 adsorption, XRD, XPS, TEM and TPR techniques. The results indicate that a good catalytic performance can be achieved by Ru supported nanoparticles fulfilling two requirements: (i) a relatively high average size (despite the usual assertion that only small particles are required) and (ii) a broad distribution of sizes that ensures the presence of both small particles, containing highly active sites, and large nanoparticles, which are shown to promote the reaction on small particles. This promotion results from a cooperative effect between small and large nanoparticles in good contact, which also allows keeping a highly reduced surface of ruthenium. It is proposed that, under mild reaction conditions, large Ru nanoparticles promote the ammonia synthesis reaction by allowing a more effective activation and transfer of hydrogen atoms, able to hydrogenate strongly adsorbed nitrogen atoms, and thus to release active sites for the activation of N2.
Author	Sanchez, Clément Fernández, Camila Sassoye, Capucine Debecker, Damien P. Ruiz, Patricio
Author_xml	– sequence: 1 givenname: Camila surname: Fernández fullname: Fernández, Camila email: camila.fernandez@uclouvain.be organization: Institute of Condensed Matter and Nanosciences – IMCN, Division “Molecules, Solids and Reactivity-MOST”, Université catholique de Louvain, Croix du Sud 2, 1348 Louvain-la-Neuve, Belgium – sequence: 2 givenname: Capucine surname: Sassoye fullname: Sassoye, Capucine organization: Laboratoire de Chimie de la Matière Condensée de Paris, Collège de France, Paris 75005, France – sequence: 3 givenname: Damien P. surname: Debecker fullname: Debecker, Damien P. organization: Institute of Condensed Matter and Nanosciences – IMCN, Division “Molecules, Solids and Reactivity-MOST”, Université catholique de Louvain, Croix du Sud 2, 1348 Louvain-la-Neuve, Belgium – sequence: 4 givenname: Clément surname: Sanchez fullname: Sanchez, Clément organization: Laboratoire de Chimie de la Matière Condensée de Paris, Collège de France, Paris 75005, France – sequence: 5 givenname: Patricio surname: Ruiz fullname: Ruiz, Patricio email: ruiz@cata.ucl.ac.be organization: Institute of Condensed Matter and Nanosciences – IMCN, Division “Molecules, Solids and Reactivity-MOST”, Université catholique de Louvain, Croix du Sud 2, 1348 Louvain-la-Neuve, Belgium
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Keywords	Catalytic cooperation Size distribution Ru supported catalyst Nanoparticle Low-temperature ammonia synthesis Ammonia Heterogeneous catalysis Catalytic reaction Synthesis Support Supported catalyst Low temperature
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Snippet	•A larger size of Ru nanoparticles leads to a higher (TOF).•Heterogeneous distribution of the size of Ru nanoparticles favors higher TOF.•Homogeneous... Ru/ gamma -Al sub(2)O sub(3) catalysts were prepared using three different methods: wet impregnation, colloidal method and microemulsion. Ru-supported... Ru/gamma-Al2O3 catalysts were prepared using three different methods: wet impregnation, colloidal method and microemulsion. Ru-supported nanoparticles with...
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SubjectTerms	Activation Ammonia Catalysis Catalysts Catalytic cooperation Chemical Sciences Chemistry Colloidal state and disperse state Exact sciences and technology General and physical chemistry Low-temperature ammonia synthesis Material chemistry Nanoparticle Nanoparticles Physical and chemical studies. Granulometry. Electrokinetic phenomena Ru supported catalyst Size distribution Surface chemistry Synthesis Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry X-ray photoelectron spectroscopy
Title	Effect of the size and distribution of supported Ru nanoparticles on their activity in ammonia synthesis under mild reaction conditions
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