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>...

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Detalles Bibliográficos
Autores: Gaikwad, Rohit, Bansode, Atul, Urakawa, Atsushi
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
Descripción
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 &gt;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>