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This investigation demonstrates the feasibility to fabricate high quality ceramic–carbonate membranes based on mixed-conducting ceramics. Specifically, it is reported the simultaneous CO2/O2 permeation and stability properties of membranes constituted by a combination of ceramic and carbonate phases, wherein the microstructure of the ceramic part is composed, in turn, of a mixture of fluorite and perovskite phases. These ceramics showed ionic and electronic conduction, and at the operation temperature, the carbonate phase of the membranes is in liquid state, which allows the transport of CO32– and O2– species via different mechanisms. To fabricate the membranes, the ceramic powders were uniaxially pressed in a disk shape. Then, an incipient sintering treatment was carried out in such a way that a highly porous ceramic was obtained. Afterwards, the piece is densified by the infiltration of molten carbonate. Characterization of the membranes was accomplished by SEM, XRD, and gas permeation techniques among others. Thermal and chemical stability under an atmosphere rich in CO2 was evaluated. CO2/O2 permeation and long-term stability measurements were conducted between 850 and 940 ℃. The best permeation–separation performance of membranes of about 1 mm thickness, showed a maximum permeance flux of about 4.46×10–7 mol∙m–2∙s–1∙Pa–1 for CO2 and 2.18×10–7 mol∙m–2∙s–1∙Pa–1 for O2 at 940 ℃. Membranes exhibited separation factor values of 150–991 and 49–511 for CO2/N2 and O2/N2 respectively in the studied temperature range. Despite long-term stability test showed certain microstructural changes in the membranes, no significant detriment on the permeation properties was observed along 100 h of continuous operation.


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Mixed-conducting ceramic–carbonate membranes exhibiting high CO2/O2 permeation flux and stability at high temperatures

Show Author's information R. ORTEGA-LUGOaJ. A. FABIÁN-ANGUIANOaO. OVALLE-ENCINIAbC. GÓMEZ-YÁÑEZaB. H. ZEIFERTaJ. ORTIZ-LANDEROSa( )
Instituto Politécnico Nacional, Escuela Superior de Ingeniería Química e Industrias Extractivas, Departamento de Ingeniería en Metalurgia y Materiales, UPALM-Zacatenco, IPN Avenue, Mexico City 07738, Mexico
Chemical Engineering School for Engineering of Matter, Transport and Energy, Arizona State University, Tempe, AZ 85287-6106, USA

Abstract

This investigation demonstrates the feasibility to fabricate high quality ceramic–carbonate membranes based on mixed-conducting ceramics. Specifically, it is reported the simultaneous CO2/O2 permeation and stability properties of membranes constituted by a combination of ceramic and carbonate phases, wherein the microstructure of the ceramic part is composed, in turn, of a mixture of fluorite and perovskite phases. These ceramics showed ionic and electronic conduction, and at the operation temperature, the carbonate phase of the membranes is in liquid state, which allows the transport of CO32– and O2– species via different mechanisms. To fabricate the membranes, the ceramic powders were uniaxially pressed in a disk shape. Then, an incipient sintering treatment was carried out in such a way that a highly porous ceramic was obtained. Afterwards, the piece is densified by the infiltration of molten carbonate. Characterization of the membranes was accomplished by SEM, XRD, and gas permeation techniques among others. Thermal and chemical stability under an atmosphere rich in CO2 was evaluated. CO2/O2 permeation and long-term stability measurements were conducted between 850 and 940 ℃. The best permeation–separation performance of membranes of about 1 mm thickness, showed a maximum permeance flux of about 4.46×10–7 mol∙m–2∙s–1∙Pa–1 for CO2 and 2.18×10–7 mol∙m–2∙s–1∙Pa–1 for O2 at 940 ℃. Membranes exhibited separation factor values of 150–991 and 49–511 for CO2/N2 and O2/N2 respectively in the studied temperature range. Despite long-term stability test showed certain microstructural changes in the membranes, no significant detriment on the permeation properties was observed along 100 h of continuous operation.

Keywords: CO2 separation, O2 separation, ceramic–carbonate membrane, selectivity

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Publication history
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Publication history

Received: 25 June 2019
Revised: 24 September 2019
Accepted: 26 September 2019
Published: 05 February 2020
Issue date: February 2020

Copyright

© The author(s) 2019

Acknowledgements

This work was supported by Proyectos de Investigación Científica y Desarrollo Tecnológico SIP-IPN No. 20190014. J. A. Fabián thanks to Proyectos de Desarrollo Tecnológico o Innovación para Alumnos 2019, SIP-IPN. Finally, the authors wish to express their appreciation for the SIBE-IPN, EDI-IPN, BEIFI-IPN, and PNPC-CONACYT programs.

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