Hydrogenation of arenes, alkenes and alkynes catalyzed by a sol-gel entrapped mixture of [Rh(cod)Cl]2 and Na[HRu3(CO)11]

Raed Abu-Reziq; Margarita Shenglof; Liza Penn; Tomer Cohen; Jochanan Blum

doi:10.1016/j.molcata.2008.05.002

Hydrogenation of arenes, alkenes and alkynes catalyzed by a sol-gel entrapped mixture of [Rh(cod)Cl]₂ and Na[HRu₃(CO)₁₁]

Raed Abu-Reziq^*, Margarita Shenglof, Liza Penn, Tomer Cohen, Jochanan Blum

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

10 Scopus citations

Abstract

A sol-gel entrapped 1:3 mixture of [Rh(cod)Cl]₂ and Na[HRu₃(CO)₁₁] catalyzes the hydrogenation of various unsaturated substrates by two distinguishable mechanisms. Under 13.8 bar H₂ and 20 °C methylated arenes react rapidly to give cycloalkane derivatives. XRD and TEM studies showed that under these conditions the hydrogenation proceeds without the generation of free metal particles. The hydrogenation of non-methylated arenes, as well as that of alkenes and alkynes, require a temperature of 80-120 °C at which the entrapped complexes form metallic nano-particles of 3-5 nm. Chloroarenes are also hydrodechlorinated at 120 °C, but require a hydrogen pressure of ≥25 bar. At both temperature ranges the catalysts are reusable at least four times. The high efficiency of the hydrogenation process at 20 °C is rationalized by a synergistic effect between the two different metal atoms of the combined catalyst. This may be related to a remote control model through a hydrogen spillover mechanism.

Original language	American English
Pages (from-to)	30-34
Number of pages	5
Journal	Journal of Molecular Catalysis A: Chemical
Volume	290
Issue number	1-2
DOIs	https://doi.org/10.1016/j.molcata.2008.05.002
State	Published - 1 Jul 2008
Externally published	Yes

Bibliographical note

Funding Information:
We thank Dr. Inna Popov and Dr. Vladimir Uvarov from the Unit for Nanoscopic Characterization (The HUJI Center for Nanoscience and Nanotechnology) for the performance of the XRD and TEM-EDS measurements, as well as the Israel Science Foundation (ISF) for the financial support of this study through Grant No. 296/06.

Keywords

Heterogeneous hydrogenation
Rhodium
Ruthenium
Sol-gel
Synergism

Access to Document

10.1016/j.molcata.2008.05.002

Cite this

@article{bcbc2e142be3490992218699e7448406,

title = "Hydrogenation of arenes, alkenes and alkynes catalyzed by a sol-gel entrapped mixture of [Rh(cod)Cl]2 and Na[HRu3(CO)11]",

abstract = "A sol-gel entrapped 1:3 mixture of [Rh(cod)Cl]2 and Na[HRu3(CO)11] catalyzes the hydrogenation of various unsaturated substrates by two distinguishable mechanisms. Under 13.8 bar H2 and 20 °C methylated arenes react rapidly to give cycloalkane derivatives. XRD and TEM studies showed that under these conditions the hydrogenation proceeds without the generation of free metal particles. The hydrogenation of non-methylated arenes, as well as that of alkenes and alkynes, require a temperature of 80-120 °C at which the entrapped complexes form metallic nano-particles of 3-5 nm. Chloroarenes are also hydrodechlorinated at 120 °C, but require a hydrogen pressure of ≥25 bar. At both temperature ranges the catalysts are reusable at least four times. The high efficiency of the hydrogenation process at 20 °C is rationalized by a synergistic effect between the two different metal atoms of the combined catalyst. This may be related to a remote control model through a hydrogen spillover mechanism.",

keywords = "Heterogeneous hydrogenation, Rhodium, Ruthenium, Sol-gel, Synergism",

author = "Raed Abu-Reziq and Margarita Shenglof and Liza Penn and Tomer Cohen and Jochanan Blum",

note = "Funding Information: We thank Dr. Inna Popov and Dr. Vladimir Uvarov from the Unit for Nanoscopic Characterization (The HUJI Center for Nanoscience and Nanotechnology) for the performance of the XRD and TEM-EDS measurements, as well as the Israel Science Foundation (ISF) for the financial support of this study through Grant No. 296/06.",

year = "2008",

month = jul,

day = "1",

doi = "10.1016/j.molcata.2008.05.002",

language = "American English",

volume = "290",

pages = "30--34",

journal = "Journal of Molecular Catalysis A: Chemical",

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TY - JOUR

T1 - Hydrogenation of arenes, alkenes and alkynes catalyzed by a sol-gel entrapped mixture of [Rh(cod)Cl]2 and Na[HRu3(CO)11]

AU - Abu-Reziq, Raed

AU - Shenglof, Margarita

AU - Penn, Liza

AU - Cohen, Tomer

AU - Blum, Jochanan

N1 - Funding Information: We thank Dr. Inna Popov and Dr. Vladimir Uvarov from the Unit for Nanoscopic Characterization (The HUJI Center for Nanoscience and Nanotechnology) for the performance of the XRD and TEM-EDS measurements, as well as the Israel Science Foundation (ISF) for the financial support of this study through Grant No. 296/06.

PY - 2008/7/1

Y1 - 2008/7/1

N2 - A sol-gel entrapped 1:3 mixture of [Rh(cod)Cl]2 and Na[HRu3(CO)11] catalyzes the hydrogenation of various unsaturated substrates by two distinguishable mechanisms. Under 13.8 bar H2 and 20 °C methylated arenes react rapidly to give cycloalkane derivatives. XRD and TEM studies showed that under these conditions the hydrogenation proceeds without the generation of free metal particles. The hydrogenation of non-methylated arenes, as well as that of alkenes and alkynes, require a temperature of 80-120 °C at which the entrapped complexes form metallic nano-particles of 3-5 nm. Chloroarenes are also hydrodechlorinated at 120 °C, but require a hydrogen pressure of ≥25 bar. At both temperature ranges the catalysts are reusable at least four times. The high efficiency of the hydrogenation process at 20 °C is rationalized by a synergistic effect between the two different metal atoms of the combined catalyst. This may be related to a remote control model through a hydrogen spillover mechanism.

AB - A sol-gel entrapped 1:3 mixture of [Rh(cod)Cl]2 and Na[HRu3(CO)11] catalyzes the hydrogenation of various unsaturated substrates by two distinguishable mechanisms. Under 13.8 bar H2 and 20 °C methylated arenes react rapidly to give cycloalkane derivatives. XRD and TEM studies showed that under these conditions the hydrogenation proceeds without the generation of free metal particles. The hydrogenation of non-methylated arenes, as well as that of alkenes and alkynes, require a temperature of 80-120 °C at which the entrapped complexes form metallic nano-particles of 3-5 nm. Chloroarenes are also hydrodechlorinated at 120 °C, but require a hydrogen pressure of ≥25 bar. At both temperature ranges the catalysts are reusable at least four times. The high efficiency of the hydrogenation process at 20 °C is rationalized by a synergistic effect between the two different metal atoms of the combined catalyst. This may be related to a remote control model through a hydrogen spillover mechanism.

KW - Heterogeneous hydrogenation

KW - Rhodium

KW - Ruthenium

KW - Sol-gel

KW - Synergism

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