$ CO_{2} $ Activation and Hydrogenation: A Comparative DFT Study of $ Ru_{10} $/$ TiO_{2} $ and $ Cu_{10} $/$ TiO_{2} $ Model Catalysts
Abstract Using DFT+U calculations with inclusion of van-der-Waals (vdW) forces, we studied $ CO_{2} $ activation and the initial steps of $ CO_{2} $ hydrogenation over $ Cu_{10} $ and $ Ru_{10} $ clusters supported on the $ TiO_{2} $ anatase (101) surface. $ CO_{2} $ is readily adsorbed and activate...
Ausführliche Beschreibung
Gespeichert in:
| Autor*in: |
Schlexer, Philomena [verfasserIn] |
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| Format: |
Artikel |
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| Sprache: |
Englisch |
| Erschienen: |
2017 |
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| Schlagwörter: |
valorization < processes and reactions |
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| Systematik: |
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| Anmerkung: |
© Springer Science+Business Media, LLC 2017 |
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| Übergeordnetes Werk: |
Enthalten in: Catalysis letters - Springer US, 1988, 147(2017), 8 vom: 07. Juni, Seite 1871-1881 |
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| Übergeordnetes Werk: |
volume:147 ; year:2017 ; number:8 ; day:07 ; month:06 ; pages:1871-1881 |
| Links: |
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| DOI / URN: |
10.1007/s10562-017-2098-1 |
|---|
| Katalog-ID: |
OLC2040193081 |
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| 245 | 1 | 0 | |a $ CO_{2} $ Activation and Hydrogenation: A Comparative DFT Study of $ Ru_{10} $/$ TiO_{2} $ and $ Cu_{10} $/$ TiO_{2} $ Model Catalysts |
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| 520 | |a Abstract Using DFT+U calculations with inclusion of van-der-Waals (vdW) forces, we studied $ CO_{2} $ activation and the initial steps of $ CO_{2} $ hydrogenation over $ Cu_{10} $ and $ Ru_{10} $ clusters supported on the $ TiO_{2} $ anatase (101) surface. $ CO_{2} $ is readily adsorbed and activated on the Ru cluster where direct $ CO_{2} $ dissociation proceeds with a barrier of 0.8 eV. When H atoms are co-adsorbed on the Ru cluster, H-addition to $ CO_{2} $ becomes preferred, as the best Ru sites for $ CO_{2} $ dissociation are blocked. A H atom is added to the $ CO_{2} $ molecule with formation of a formate [HCOO] species and an activation barrier of 1.2 eV. On $ Cu_{10} $/$ TiO_{2} $, only weak adsorption modes of the $ CO_{2} $ molecule are found, whereas $ H_{2} $ readily adsorbs on the Cu cluster. A reduction of the titania support does not significantly change this picture. Therefore, the only viable pathway for the $ CO_{2} $ hydrogenation over $ Cu_{10} $/$ TiO_{2} $ is the addition of a pre-adsorbed H atom to $ CO_{2} $ coming from the gas phase. This corresponds to an Eley–Rideal mechanism for the H-association to $ CO_{2} $. The work shows the importance to consider the hydrogen coverage on the metal cluster as an important variable in modeling the $ CO_{2} $ hydrogenation reaction. Graphical Abstract | ||
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| 650 | 4 | |a valorization < processes and reactions | |
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| 650 | 4 | |a CO | |
| 650 | 4 | |a hydrogenation | |
| 650 | 4 | |a Nanoparticles < nanotechnology | |
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10.1007/s10562-017-2098-1 doi (DE-627)OLC2040193081 (DE-He213)s10562-017-2098-1-p DE-627 ger DE-627 rakwb eng 540 660 VZ VA 2890 VZ rvk Schlexer, Philomena verfasserin aut $ CO_{2} $ Activation and Hydrogenation: A Comparative DFT Study of $ Ru_{10} $/$ TiO_{2} $ and $ Cu_{10} $/$ TiO_{2} $ Model Catalysts 2017 Text txt rdacontent ohne Hilfsmittel zu benutzen n rdamedia Band nc rdacarrier © Springer Science+Business Media, LLC 2017 Abstract Using DFT+U calculations with inclusion of van-der-Waals (vdW) forces, we studied $ CO_{2} $ activation and the initial steps of $ CO_{2} $ hydrogenation over $ Cu_{10} $ and $ Ru_{10} $ clusters supported on the $ TiO_{2} $ anatase (101) surface. $ CO_{2} $ is readily adsorbed and activated on the Ru cluster where direct $ CO_{2} $ dissociation proceeds with a barrier of 0.8 eV. When H atoms are co-adsorbed on the Ru cluster, H-addition to $ CO_{2} $ becomes preferred, as the best Ru sites for $ CO_{2} $ dissociation are blocked. A H atom is added to the $ CO_{2} $ molecule with formation of a formate [HCOO] species and an activation barrier of 1.2 eV. On $ Cu_{10} $/$ TiO_{2} $, only weak adsorption modes of the $ CO_{2} $ molecule are found, whereas $ H_{2} $ readily adsorbs on the Cu cluster. A reduction of the titania support does not significantly change this picture. Therefore, the only viable pathway for the $ CO_{2} $ hydrogenation over $ Cu_{10} $/$ TiO_{2} $ is the addition of a pre-adsorbed H atom to $ CO_{2} $ coming from the gas phase. This corresponds to an Eley–Rideal mechanism for the H-association to $ CO_{2} $. The work shows the importance to consider the hydrogen coverage on the metal cluster as an important variable in modeling the $ CO_{2} $ hydrogenation reaction. Graphical Abstract CO valorization < processes and reactions Methanation Methanol synthesis CO hydrogenation Nanoparticles < nanotechnology Titania Ru Cu Chen, Hsin-Yi Tiffany aut Pacchioni, Gianfranco aut Enthalten in Catalysis letters Springer US, 1988 147(2017), 8 vom: 07. Juni, Seite 1871-1881 (DE-627)130436550 (DE-600)644234-1 (DE-576)025720724 1011-372X nnns volume:147 year:2017 number:8 day:07 month:06 pages:1871-1881 https://doi.org/10.1007/s10562-017-2098-1 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_OLC SSG-OLC-TEC SSG-OLC-CHE GBV_ILN_70 VA 2890 AR 147 2017 8 07 06 1871-1881 |
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10.1007/s10562-017-2098-1 doi (DE-627)OLC2040193081 (DE-He213)s10562-017-2098-1-p DE-627 ger DE-627 rakwb eng 540 660 VZ VA 2890 VZ rvk Schlexer, Philomena verfasserin aut $ CO_{2} $ Activation and Hydrogenation: A Comparative DFT Study of $ Ru_{10} $/$ TiO_{2} $ and $ Cu_{10} $/$ TiO_{2} $ Model Catalysts 2017 Text txt rdacontent ohne Hilfsmittel zu benutzen n rdamedia Band nc rdacarrier © Springer Science+Business Media, LLC 2017 Abstract Using DFT+U calculations with inclusion of van-der-Waals (vdW) forces, we studied $ CO_{2} $ activation and the initial steps of $ CO_{2} $ hydrogenation over $ Cu_{10} $ and $ Ru_{10} $ clusters supported on the $ TiO_{2} $ anatase (101) surface. $ CO_{2} $ is readily adsorbed and activated on the Ru cluster where direct $ CO_{2} $ dissociation proceeds with a barrier of 0.8 eV. When H atoms are co-adsorbed on the Ru cluster, H-addition to $ CO_{2} $ becomes preferred, as the best Ru sites for $ CO_{2} $ dissociation are blocked. A H atom is added to the $ CO_{2} $ molecule with formation of a formate [HCOO] species and an activation barrier of 1.2 eV. On $ Cu_{10} $/$ TiO_{2} $, only weak adsorption modes of the $ CO_{2} $ molecule are found, whereas $ H_{2} $ readily adsorbs on the Cu cluster. A reduction of the titania support does not significantly change this picture. Therefore, the only viable pathway for the $ CO_{2} $ hydrogenation over $ Cu_{10} $/$ TiO_{2} $ is the addition of a pre-adsorbed H atom to $ CO_{2} $ coming from the gas phase. This corresponds to an Eley–Rideal mechanism for the H-association to $ CO_{2} $. The work shows the importance to consider the hydrogen coverage on the metal cluster as an important variable in modeling the $ CO_{2} $ hydrogenation reaction. Graphical Abstract CO valorization < processes and reactions Methanation Methanol synthesis CO hydrogenation Nanoparticles < nanotechnology Titania Ru Cu Chen, Hsin-Yi Tiffany aut Pacchioni, Gianfranco aut Enthalten in Catalysis letters Springer US, 1988 147(2017), 8 vom: 07. Juni, Seite 1871-1881 (DE-627)130436550 (DE-600)644234-1 (DE-576)025720724 1011-372X nnns volume:147 year:2017 number:8 day:07 month:06 pages:1871-1881 https://doi.org/10.1007/s10562-017-2098-1 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_OLC SSG-OLC-TEC SSG-OLC-CHE GBV_ILN_70 VA 2890 AR 147 2017 8 07 06 1871-1881 |
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10.1007/s10562-017-2098-1 doi (DE-627)OLC2040193081 (DE-He213)s10562-017-2098-1-p DE-627 ger DE-627 rakwb eng 540 660 VZ VA 2890 VZ rvk Schlexer, Philomena verfasserin aut $ CO_{2} $ Activation and Hydrogenation: A Comparative DFT Study of $ Ru_{10} $/$ TiO_{2} $ and $ Cu_{10} $/$ TiO_{2} $ Model Catalysts 2017 Text txt rdacontent ohne Hilfsmittel zu benutzen n rdamedia Band nc rdacarrier © Springer Science+Business Media, LLC 2017 Abstract Using DFT+U calculations with inclusion of van-der-Waals (vdW) forces, we studied $ CO_{2} $ activation and the initial steps of $ CO_{2} $ hydrogenation over $ Cu_{10} $ and $ Ru_{10} $ clusters supported on the $ TiO_{2} $ anatase (101) surface. $ CO_{2} $ is readily adsorbed and activated on the Ru cluster where direct $ CO_{2} $ dissociation proceeds with a barrier of 0.8 eV. When H atoms are co-adsorbed on the Ru cluster, H-addition to $ CO_{2} $ becomes preferred, as the best Ru sites for $ CO_{2} $ dissociation are blocked. A H atom is added to the $ CO_{2} $ molecule with formation of a formate [HCOO] species and an activation barrier of 1.2 eV. On $ Cu_{10} $/$ TiO_{2} $, only weak adsorption modes of the $ CO_{2} $ molecule are found, whereas $ H_{2} $ readily adsorbs on the Cu cluster. A reduction of the titania support does not significantly change this picture. Therefore, the only viable pathway for the $ CO_{2} $ hydrogenation over $ Cu_{10} $/$ TiO_{2} $ is the addition of a pre-adsorbed H atom to $ CO_{2} $ coming from the gas phase. This corresponds to an Eley–Rideal mechanism for the H-association to $ CO_{2} $. The work shows the importance to consider the hydrogen coverage on the metal cluster as an important variable in modeling the $ CO_{2} $ hydrogenation reaction. Graphical Abstract CO valorization < processes and reactions Methanation Methanol synthesis CO hydrogenation Nanoparticles < nanotechnology Titania Ru Cu Chen, Hsin-Yi Tiffany aut Pacchioni, Gianfranco aut Enthalten in Catalysis letters Springer US, 1988 147(2017), 8 vom: 07. Juni, Seite 1871-1881 (DE-627)130436550 (DE-600)644234-1 (DE-576)025720724 1011-372X nnns volume:147 year:2017 number:8 day:07 month:06 pages:1871-1881 https://doi.org/10.1007/s10562-017-2098-1 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_OLC SSG-OLC-TEC SSG-OLC-CHE GBV_ILN_70 VA 2890 AR 147 2017 8 07 06 1871-1881 |
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10.1007/s10562-017-2098-1 doi (DE-627)OLC2040193081 (DE-He213)s10562-017-2098-1-p DE-627 ger DE-627 rakwb eng 540 660 VZ VA 2890 VZ rvk Schlexer, Philomena verfasserin aut $ CO_{2} $ Activation and Hydrogenation: A Comparative DFT Study of $ Ru_{10} $/$ TiO_{2} $ and $ Cu_{10} $/$ TiO_{2} $ Model Catalysts 2017 Text txt rdacontent ohne Hilfsmittel zu benutzen n rdamedia Band nc rdacarrier © Springer Science+Business Media, LLC 2017 Abstract Using DFT+U calculations with inclusion of van-der-Waals (vdW) forces, we studied $ CO_{2} $ activation and the initial steps of $ CO_{2} $ hydrogenation over $ Cu_{10} $ and $ Ru_{10} $ clusters supported on the $ TiO_{2} $ anatase (101) surface. $ CO_{2} $ is readily adsorbed and activated on the Ru cluster where direct $ CO_{2} $ dissociation proceeds with a barrier of 0.8 eV. When H atoms are co-adsorbed on the Ru cluster, H-addition to $ CO_{2} $ becomes preferred, as the best Ru sites for $ CO_{2} $ dissociation are blocked. A H atom is added to the $ CO_{2} $ molecule with formation of a formate [HCOO] species and an activation barrier of 1.2 eV. On $ Cu_{10} $/$ TiO_{2} $, only weak adsorption modes of the $ CO_{2} $ molecule are found, whereas $ H_{2} $ readily adsorbs on the Cu cluster. A reduction of the titania support does not significantly change this picture. Therefore, the only viable pathway for the $ CO_{2} $ hydrogenation over $ Cu_{10} $/$ TiO_{2} $ is the addition of a pre-adsorbed H atom to $ CO_{2} $ coming from the gas phase. This corresponds to an Eley–Rideal mechanism for the H-association to $ CO_{2} $. The work shows the importance to consider the hydrogen coverage on the metal cluster as an important variable in modeling the $ CO_{2} $ hydrogenation reaction. Graphical Abstract CO valorization < processes and reactions Methanation Methanol synthesis CO hydrogenation Nanoparticles < nanotechnology Titania Ru Cu Chen, Hsin-Yi Tiffany aut Pacchioni, Gianfranco aut Enthalten in Catalysis letters Springer US, 1988 147(2017), 8 vom: 07. Juni, Seite 1871-1881 (DE-627)130436550 (DE-600)644234-1 (DE-576)025720724 1011-372X nnns volume:147 year:2017 number:8 day:07 month:06 pages:1871-1881 https://doi.org/10.1007/s10562-017-2098-1 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_OLC SSG-OLC-TEC SSG-OLC-CHE GBV_ILN_70 VA 2890 AR 147 2017 8 07 06 1871-1881 |
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10.1007/s10562-017-2098-1 doi (DE-627)OLC2040193081 (DE-He213)s10562-017-2098-1-p DE-627 ger DE-627 rakwb eng 540 660 VZ VA 2890 VZ rvk Schlexer, Philomena verfasserin aut $ CO_{2} $ Activation and Hydrogenation: A Comparative DFT Study of $ Ru_{10} $/$ TiO_{2} $ and $ Cu_{10} $/$ TiO_{2} $ Model Catalysts 2017 Text txt rdacontent ohne Hilfsmittel zu benutzen n rdamedia Band nc rdacarrier © Springer Science+Business Media, LLC 2017 Abstract Using DFT+U calculations with inclusion of van-der-Waals (vdW) forces, we studied $ CO_{2} $ activation and the initial steps of $ CO_{2} $ hydrogenation over $ Cu_{10} $ and $ Ru_{10} $ clusters supported on the $ TiO_{2} $ anatase (101) surface. $ CO_{2} $ is readily adsorbed and activated on the Ru cluster where direct $ CO_{2} $ dissociation proceeds with a barrier of 0.8 eV. When H atoms are co-adsorbed on the Ru cluster, H-addition to $ CO_{2} $ becomes preferred, as the best Ru sites for $ CO_{2} $ dissociation are blocked. A H atom is added to the $ CO_{2} $ molecule with formation of a formate [HCOO] species and an activation barrier of 1.2 eV. On $ Cu_{10} $/$ TiO_{2} $, only weak adsorption modes of the $ CO_{2} $ molecule are found, whereas $ H_{2} $ readily adsorbs on the Cu cluster. A reduction of the titania support does not significantly change this picture. Therefore, the only viable pathway for the $ CO_{2} $ hydrogenation over $ Cu_{10} $/$ TiO_{2} $ is the addition of a pre-adsorbed H atom to $ CO_{2} $ coming from the gas phase. This corresponds to an Eley–Rideal mechanism for the H-association to $ CO_{2} $. The work shows the importance to consider the hydrogen coverage on the metal cluster as an important variable in modeling the $ CO_{2} $ hydrogenation reaction. Graphical Abstract CO valorization < processes and reactions Methanation Methanol synthesis CO hydrogenation Nanoparticles < nanotechnology Titania Ru Cu Chen, Hsin-Yi Tiffany aut Pacchioni, Gianfranco aut Enthalten in Catalysis letters Springer US, 1988 147(2017), 8 vom: 07. Juni, Seite 1871-1881 (DE-627)130436550 (DE-600)644234-1 (DE-576)025720724 1011-372X nnns volume:147 year:2017 number:8 day:07 month:06 pages:1871-1881 https://doi.org/10.1007/s10562-017-2098-1 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_OLC SSG-OLC-TEC SSG-OLC-CHE GBV_ILN_70 VA 2890 AR 147 2017 8 07 06 1871-1881 |
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Schlexer, Philomena ddc 540 rvk VA 2890 misc CO misc valorization < processes and reactions misc Methanation misc Methanol synthesis misc hydrogenation misc Nanoparticles < nanotechnology misc Titania misc Ru misc Cu $ CO_{2} $ Activation and Hydrogenation: A Comparative DFT Study of $ Ru_{10} $/$ TiO_{2} $ and $ Cu_{10} $/$ TiO_{2} $ Model Catalysts |
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$ CO_{2} $ Activation and Hydrogenation: A Comparative DFT Study of $ Ru_{10} $/$ TiO_{2} $ and $ Cu_{10} $/$ TiO_{2} $ Model Catalysts |
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$ CO_{2} $ Activation and Hydrogenation: A Comparative DFT Study of $ Ru_{10} $/$ TiO_{2} $ and $ Cu_{10} $/$ TiO_{2} $ Model Catalysts |
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$ co_{2} $ activation and hydrogenation: a comparative dft study of $ ru_{10} $/$ tio_{2} $ and $ cu_{10} $/$ tio_{2} $ model catalysts |
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$ CO_{2} $ Activation and Hydrogenation: A Comparative DFT Study of $ Ru_{10} $/$ TiO_{2} $ and $ Cu_{10} $/$ TiO_{2} $ Model Catalysts |
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Abstract Using DFT+U calculations with inclusion of van-der-Waals (vdW) forces, we studied $ CO_{2} $ activation and the initial steps of $ CO_{2} $ hydrogenation over $ Cu_{10} $ and $ Ru_{10} $ clusters supported on the $ TiO_{2} $ anatase (101) surface. $ CO_{2} $ is readily adsorbed and activated on the Ru cluster where direct $ CO_{2} $ dissociation proceeds with a barrier of 0.8 eV. When H atoms are co-adsorbed on the Ru cluster, H-addition to $ CO_{2} $ becomes preferred, as the best Ru sites for $ CO_{2} $ dissociation are blocked. A H atom is added to the $ CO_{2} $ molecule with formation of a formate [HCOO] species and an activation barrier of 1.2 eV. On $ Cu_{10} $/$ TiO_{2} $, only weak adsorption modes of the $ CO_{2} $ molecule are found, whereas $ H_{2} $ readily adsorbs on the Cu cluster. A reduction of the titania support does not significantly change this picture. Therefore, the only viable pathway for the $ CO_{2} $ hydrogenation over $ Cu_{10} $/$ TiO_{2} $ is the addition of a pre-adsorbed H atom to $ CO_{2} $ coming from the gas phase. This corresponds to an Eley–Rideal mechanism for the H-association to $ CO_{2} $. The work shows the importance to consider the hydrogen coverage on the metal cluster as an important variable in modeling the $ CO_{2} $ hydrogenation reaction. Graphical Abstract © Springer Science+Business Media, LLC 2017 |
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Abstract Using DFT+U calculations with inclusion of van-der-Waals (vdW) forces, we studied $ CO_{2} $ activation and the initial steps of $ CO_{2} $ hydrogenation over $ Cu_{10} $ and $ Ru_{10} $ clusters supported on the $ TiO_{2} $ anatase (101) surface. $ CO_{2} $ is readily adsorbed and activated on the Ru cluster where direct $ CO_{2} $ dissociation proceeds with a barrier of 0.8 eV. When H atoms are co-adsorbed on the Ru cluster, H-addition to $ CO_{2} $ becomes preferred, as the best Ru sites for $ CO_{2} $ dissociation are blocked. A H atom is added to the $ CO_{2} $ molecule with formation of a formate [HCOO] species and an activation barrier of 1.2 eV. On $ Cu_{10} $/$ TiO_{2} $, only weak adsorption modes of the $ CO_{2} $ molecule are found, whereas $ H_{2} $ readily adsorbs on the Cu cluster. A reduction of the titania support does not significantly change this picture. Therefore, the only viable pathway for the $ CO_{2} $ hydrogenation over $ Cu_{10} $/$ TiO_{2} $ is the addition of a pre-adsorbed H atom to $ CO_{2} $ coming from the gas phase. This corresponds to an Eley–Rideal mechanism for the H-association to $ CO_{2} $. The work shows the importance to consider the hydrogen coverage on the metal cluster as an important variable in modeling the $ CO_{2} $ hydrogenation reaction. Graphical Abstract © Springer Science+Business Media, LLC 2017 |
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Abstract Using DFT+U calculations with inclusion of van-der-Waals (vdW) forces, we studied $ CO_{2} $ activation and the initial steps of $ CO_{2} $ hydrogenation over $ Cu_{10} $ and $ Ru_{10} $ clusters supported on the $ TiO_{2} $ anatase (101) surface. $ CO_{2} $ is readily adsorbed and activated on the Ru cluster where direct $ CO_{2} $ dissociation proceeds with a barrier of 0.8 eV. When H atoms are co-adsorbed on the Ru cluster, H-addition to $ CO_{2} $ becomes preferred, as the best Ru sites for $ CO_{2} $ dissociation are blocked. A H atom is added to the $ CO_{2} $ molecule with formation of a formate [HCOO] species and an activation barrier of 1.2 eV. On $ Cu_{10} $/$ TiO_{2} $, only weak adsorption modes of the $ CO_{2} $ molecule are found, whereas $ H_{2} $ readily adsorbs on the Cu cluster. A reduction of the titania support does not significantly change this picture. Therefore, the only viable pathway for the $ CO_{2} $ hydrogenation over $ Cu_{10} $/$ TiO_{2} $ is the addition of a pre-adsorbed H atom to $ CO_{2} $ coming from the gas phase. This corresponds to an Eley–Rideal mechanism for the H-association to $ CO_{2} $. The work shows the importance to consider the hydrogen coverage on the metal cluster as an important variable in modeling the $ CO_{2} $ hydrogenation reaction. Graphical Abstract © Springer Science+Business Media, LLC 2017 |
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