Acceptorless Dehydrogenation of Methanol to Carbon Monoxide and Hydrogen using Molecular Catalysts
The acceptorless dehydrogenation of methanol to carbon monoxide and hydrogen was investigated using homogeneous molecular complexes. Complexes of ruthenium and manganese comprising the MACHO ligand framework showed promising activities for this reaction. The molecular ruthenium complex [RuH(CO)(BH4)...
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| Published in: | Angewandte Chemie International Edition Vol. 60; no. 51; pp. 26500 - 26505 |
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| Main Authors: | , , , |
| Format: | Journal Article |
| Language: | English |
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Weinheim
Wiley Subscription Services, Inc
13-12-2021
John Wiley and Sons Inc |
| Edition: | International ed. in English |
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| Abstract | The acceptorless dehydrogenation of methanol to carbon monoxide and hydrogen was investigated using homogeneous molecular complexes. Complexes of ruthenium and manganese comprising the MACHO ligand framework showed promising activities for this reaction. The molecular ruthenium complex [RuH(CO)(BH4)(HN(C2H4PPh2)2)] (Ru‐MACHO‐BH) achieved up to 3150 turnovers for carbon monoxide and 9230 turnovers for hydrogen formation at 150 °C reaching pressures up to 12 bar when the decomposition was carried out in a closed vessel. Control experiments affirmed that the metal complex mediates the initial fast dehydrogenation of methanol to formaldehyde and methyl formate followed by subsequent slow decarbonylation. Depending on the catalyst and reaction conditions, the CO/H2 ratio in the gas mixture thus varies over a broad range from almost pure hydrogen to the stoichiometric limit of 1:2.
Homogeneous catalysts based on ruthenium and manganese enable the generation of gaseous CO and H2 (syngas) from conveniently storable and easily transportable methanol. Conversion/time profiles and kinetic isotope effects together with spectroscopically detected intermediates indicate rapid dehydrogenation followed by two possible catalytic pathways via formaldehyde or methyl formate for decarbonylation as mechanistic manifold. |
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| AbstractList | The acceptorless dehydrogenation of methanol to carbon monoxide and hydrogen was investigated using homogeneous molecular complexes. Complexes of ruthenium and manganese comprising the MACHO ligand framework showed promising activities for this reaction. The molecular ruthenium complex [RuH(CO)(BH
4
)(HN(C
2
H
4
PPh
2
)
2
)] (Ru‐MACHO‐BH) achieved up to 3150 turnovers for carbon monoxide and 9230 turnovers for hydrogen formation at 150 °C reaching pressures up to 12 bar when the decomposition was carried out in a closed vessel. Control experiments affirmed that the metal complex mediates the initial fast dehydrogenation of methanol to formaldehyde and methyl formate followed by subsequent slow decarbonylation. Depending on the catalyst and reaction conditions, the CO/H
2
ratio in the gas mixture thus varies over a broad range from almost pure hydrogen to the stoichiometric limit of 1:2. The acceptorless dehydrogenation of methanol to carbon monoxide and hydrogen was investigated using homogeneous molecular complexes. Complexes of ruthenium and manganese comprising the MACHO ligand framework showed promising activities for this reaction. The molecular ruthenium complex [RuH(CO)(BH4)(HN(C2H4PPh2)2)] (Ru‐MACHO‐BH) achieved up to 3150 turnovers for carbon monoxide and 9230 turnovers for hydrogen formation at 150 °C reaching pressures up to 12 bar when the decomposition was carried out in a closed vessel. Control experiments affirmed that the metal complex mediates the initial fast dehydrogenation of methanol to formaldehyde and methyl formate followed by subsequent slow decarbonylation. Depending on the catalyst and reaction conditions, the CO/H2 ratio in the gas mixture thus varies over a broad range from almost pure hydrogen to the stoichiometric limit of 1:2. The acceptorless dehydrogenation of methanol to carbon monoxide and hydrogen was investigated using homogeneous molecular complexes. Complexes of ruthenium and manganese comprising the MACHO ligand framework showed promising activities for this reaction. The molecular ruthenium complex [RuH(CO)(BH 4 )(HN(C 2 H 4 PPh 2 ) 2 )] (Ru‐MACHO‐BH) achieved up to 3150 turnovers for carbon monoxide and 9230 turnovers for hydrogen formation at 150 °C reaching pressures up to 12 bar when the decomposition was carried out in a closed vessel. Control experiments affirmed that the metal complex mediates the initial fast dehydrogenation of methanol to formaldehyde and methyl formate followed by subsequent slow decarbonylation. Depending on the catalyst and reaction conditions, the CO/H 2 ratio in the gas mixture thus varies over a broad range from almost pure hydrogen to the stoichiometric limit of 1:2. Homogeneous catalysts based on ruthenium and manganese enable the generation of gaseous CO and H 2 (syngas) from conveniently storable and easily transportable methanol. Conversion/time profiles and kinetic isotope effects together with spectroscopically detected intermediates indicate rapid dehydrogenation followed by two possible catalytic pathways via formaldehyde or methyl formate for decarbonylation as mechanistic manifold. The acceptorless dehydrogenation of methanol to carbon monoxide and hydrogen was investigated using homogeneous molecular complexes. Complexes of ruthenium and manganese comprising the MACHO ligand framework showed promising activities for this reaction. The molecular ruthenium complex [RuH(CO)(BH4)(HN(C2H4PPh2)2)] (Ru‐MACHO‐BH) achieved up to 3150 turnovers for carbon monoxide and 9230 turnovers for hydrogen formation at 150 °C reaching pressures up to 12 bar when the decomposition was carried out in a closed vessel. Control experiments affirmed that the metal complex mediates the initial fast dehydrogenation of methanol to formaldehyde and methyl formate followed by subsequent slow decarbonylation. Depending on the catalyst and reaction conditions, the CO/H2 ratio in the gas mixture thus varies over a broad range from almost pure hydrogen to the stoichiometric limit of 1:2. Homogeneous catalysts based on ruthenium and manganese enable the generation of gaseous CO and H2 (syngas) from conveniently storable and easily transportable methanol. Conversion/time profiles and kinetic isotope effects together with spectroscopically detected intermediates indicate rapid dehydrogenation followed by two possible catalytic pathways via formaldehyde or methyl formate for decarbonylation as mechanistic manifold. The acceptorless dehydrogenation of methanol to carbon monoxide and hydrogen was investigated using homogeneous molecular complexes. Complexes of ruthenium and manganese comprising the MACHO ligand framework showed promising activities for this reaction. The molecular ruthenium complex [RuH(CO)(BH4 )(HN(C2 H4 PPh2 )2 )] (Ru-MACHO-BH) achieved up to 3150 turnovers for carbon monoxide and 9230 turnovers for hydrogen formation at 150 °C reaching pressures up to 12 bar when the decomposition was carried out in a closed vessel. Control experiments affirmed that the metal complex mediates the initial fast dehydrogenation of methanol to formaldehyde and methyl formate followed by subsequent slow decarbonylation. Depending on the catalyst and reaction conditions, the CO/H2 ratio in the gas mixture thus varies over a broad range from almost pure hydrogen to the stoichiometric limit of 1:2. |
| Author | Chatterjee, Basujit Leitner, Walter Werlé, Christophe Kaithal, Akash |
| AuthorAffiliation | 3 Institut für Technische und Makromolekulare Chemie RWTH Aachen University Worringer Weg 2 52074 Aachen Germany 1 Max Planck Institute for Chemical Energy Conversion Stiftstraße 34–36 45470 Mülheim a.d. Ruhr Germany 2 Ruhr University Bochum Universitätsstr. 150 44801 Bochum Germany |
| AuthorAffiliation_xml | – name: 1 Max Planck Institute for Chemical Energy Conversion Stiftstraße 34–36 45470 Mülheim a.d. Ruhr Germany – name: 3 Institut für Technische und Makromolekulare Chemie RWTH Aachen University Worringer Weg 2 52074 Aachen Germany – name: 2 Ruhr University Bochum Universitätsstr. 150 44801 Bochum Germany |
| Author_xml | – sequence: 1 givenname: Akash orcidid: 0000-0003-3328-3003 surname: Kaithal fullname: Kaithal, Akash organization: Max Planck Institute for Chemical Energy Conversion – sequence: 2 givenname: Basujit orcidid: 0000-0003-3539-089X surname: Chatterjee fullname: Chatterjee, Basujit organization: Max Planck Institute for Chemical Energy Conversion – sequence: 3 givenname: Christophe orcidid: 0000-0002-2174-2148 surname: Werlé fullname: Werlé, Christophe organization: Ruhr University Bochum – sequence: 4 givenname: Walter orcidid: 0000-0001-6100-9656 surname: Leitner fullname: Leitner, Walter email: walter.leitner@cec.mpg.de organization: RWTH Aachen University |
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| Snippet | The acceptorless dehydrogenation of methanol to carbon monoxide and hydrogen was investigated using homogeneous molecular complexes. Complexes of ruthenium and... |
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| SubjectTerms | carbon dioxide Carbon monoxide Catalysts Communication Communications Coordination compounds decarbonylation Dehydrogenation Gas mixtures Hydrogen Manganese Methanol Methyl formate Ruthenium Ruthenium compounds |
| Title | Acceptorless Dehydrogenation of Methanol to Carbon Monoxide and Hydrogen using Molecular Catalysts |
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