Carbon molecular sieve membranes for water separation in CO2 hydrogenation reactions: Effect of the carbonization temperature

Carbon membranes are a potentially attractive candidate for the in-situ removal of water vapor in CO2 hydrogenation reactions. Their hydrophilicity and pore structure can be tuned by properly adjusting the synthesis procedure. Herein, we assess the effect of the carbonization temperature (450–750 °C...

Descripción completa

Detalles Bibliográficos
Autores: Poto, Serena, Aguirre, A., Huigh, F., Llosa-Tanco, Margot Anabell, Pacheco-Tanaka, David Alfredo, Gallucci, Fausto, Neira d'Angelo, M. Fernanda
Tipo de recurso: artículo
Fecha de publicación:2023
País:España
Institución:TECNALIA Research & Innovation
Repositorio:TECNALIA Publications
Idioma:inglés
OAI Identifier:oai:dsp.tecnalia.com:11556/5214
Acceso en línea:https://hdl.handle.net/11556/5214
Access Level:acceso abierto
Palabra clave:Adsorption-diffusion
CO hydrogenation
Carbon membranes
Carbonization temperature
Hydrophilicity
Molecular sieving
Water separation
Biochemistry
General Materials Science
Physical and Theoretical Chemistry
Filtration and Separation
SDG 13 - Climate Action
Descripción
Sumario:Carbon membranes are a potentially attractive candidate for the in-situ removal of water vapor in CO2 hydrogenation reactions. Their hydrophilicity and pore structure can be tuned by properly adjusting the synthesis procedure. Herein, we assess the effect of the carbonization temperature (450–750 °C) on the performance of supported CMSM in terms of vapor/gas separation, in correlation with changes in their surface functionality and porous structure. FTIR spectra showed that the nature of the functional groups changes with the evolution of the carbonization step, leading to a gradual loss in hydrophilicity (i.e., OH stretching disappears at Tcarb ≥ 600 °C). The extent of water adsorption displays an optimum at Tcarb of 500 °C, with the membrane carbonized at 650 °C being the least hydrophilic. We found that the pore size distribution strongly influences the water permeance. At all Tcarb, adsorption-diffusion (AD) is the dominant transport mechanisms. However, as soon as ultra-micropores appear (Tcarb: 600–700 °C) molecular sieving (MS) contributes to an increase in the water permeance, despites a loss in hydrophilicity. At Tcarb ≥ 750 °C, MS pores disappear, causing a drop in the water permeance. Finally, the permeance of different gases (N2, H2, CO, CO2) is mostly affected by the pore size distribution, with MS being the dominant mechanism over the AD, except for CO2. However, the extent and mechanism of gas permeation drastically change as a function of the water content in the feed, indicating that gas/vapor molecules need to compete to access the pores of the membranes.