High-pressure advantages in stoichiometric hydrogenation of carbon dioxide to methanol
<p> Interplay between three important reaction parameters (pressure, temperature, and space velocity) in stoichiometric hydrogenation of carbon dioxide (CO<sub>2</sub>:H<sub>2</sub>=1:3) was systematically investigated using a commercial Cu/ZnO/Al<sub>2</sub>...
| Autores: | , , |
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| Tipo de recurso: | artículo |
| Fecha de publicación: | 2016 |
| País: | España |
| Institución: | Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya) |
| Repositorio: | Recercat. Dipósit de la Recerca de Catalunya |
| OAI Identifier: | oai:recercat.cat:2072/305873 |
| Acceso en línea: | http://hdl.handle.net/2072/305873 https://doi.org/10.1016/j.jcat.2016.02.005 |
| Access Level: | acceso abierto |
| Palabra clave: | CO2 hydrogenation methanol synthesi high-pressure kinetics thermodynamics Cu/ZnO/Al2O3 |
| Sumario: | <p> Interplay between three important reaction parameters (pressure, temperature, and space velocity) in stoichiometric hydrogenation of carbon dioxide (CO<sub>2</sub>:H<sub>2</sub>=1:3) was systematically investigated using a commercial Cu/ZnO/Al<sub>2</sub>O<sub>3</sub> catalyst. Their impacts on reaction performance and important ranges of process conditions towards full one-pass conversion of CO<sub>2</sub> to methanol at high yield were rationalized based on the kinetics and thermodynamics of the reaction. Under high-pressure condition above a threshold temperature, the reaction overcomes kinetic control, entering thermodynamically controlled regime. Ca. 90% CO<sub>2</sub> conversion and >95% methanol selectivity was achieved with a very good yield (0.9-2.4 g<sub>MeOH</sub> g<sub>cat</sub><sup>-1</sup> h<sup>-1</sup>) at 442 bar. Such high-pressure condition induces the formation of highly dense phase and consequent mass transfer limitation. When this limitation is overcome, the advantage of high-pressure conditions can be fully exploited and weight time yield as high as 15.3 g<sub>MeOH</sub> g<sub>cat</sub><sup>-1</sup> h<sup>-1</sup> could be achieved at 442 bar. Remarkable advantages of high-pressure conditions in the terms reaction kinetics, thermodynamics, and phase behavior in the aim to achieve better methanol yield are discussed.</p> |
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