Details
Original language | English |
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Article number | 117082 |
Journal | Journal of membrane science |
Volume | 590 |
Early online date | 5 May 2019 |
Publication status | Published - 15 Nov 2019 |
Abstract
Most of the currently used perovskite-based oxygen-transporting membranes have insufficient resistance towards CO2 and high material costs that potentially limit their commercial applications. In the present work, a highly CO2-tolerant oxygen permeation membrane based on La0.6Ca0.4Co1–xFexO3−δ (x = 0, 0.3, 0.5, 0.7, 1) was designed and prepared by a scalable reverse co-precipitation method. The oxygen permeation flux through the dense membranes was evaluated and found to be highly dependent on the Co/Fe ratio. La0.6Ca0.4Co0.3Fe0.7O3−δ possessed the highest permeation flux among the investigated samples, achieving 0.76 ml min−1 cm−2 under an Air/He gradient and 0.5 ml min−1 cm−2 under an Air/CO2 gradient at 1173 K for a 1 mm thick membrane. A combination study of first principles calculations and experimental measurements was conducted to advance the understanding of Co/Fe ratio effects on the oxygen migration behavior in La0.6Ca0.4Co1–xFexO3−δ. The observed oxygen permeability is three times higher than that reported in literature under similar conditions. The presented results demonstrate that this highly CO2-tolerant membrane is a promising candidate for high temperature oxygen separation applications.
Keywords
- CO resistance, DFT, Oxygen permeation membrane, Oxygen vacancy formation energy, Oxygen vacancy migration energy, Perovskite
ASJC Scopus subject areas
- Biochemistry, Genetics and Molecular Biology(all)
- Biochemistry
- Materials Science(all)
- General Materials Science
- Chemistry(all)
- Physical and Theoretical Chemistry
- Chemical Engineering(all)
- Filtration and Separation
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In: Journal of membrane science, Vol. 590, 117082, 15.11.2019.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - High flux and CO2-resistance of La0.6Ca0.4Co1–xFexO3−δ oxygen-transporting membranes
AU - Chen, Guoxing
AU - Liu, Wenmei
AU - Widenmeyer, Marc
AU - Ying, Pingjun
AU - Dou, Maofeng
AU - Xie, Wenjie
AU - Bubeck, Cora
AU - Wang, Ling
AU - Fyta, Maria
AU - Feldhoff, Armin
AU - Weidenkaff, Anke
N1 - Funding Information: The financial support of the Federal Ministry of Education and Research of Germany in the framework of the Kopernikus projects for the Energiewende within the project ?Plasma-induced CO2-conversion? (PiCK, project number: 03SFK2S3B) is highly acknowledged. G. Chen is grateful to Frank Hack, Dr. Angelika Veziridis, Dr. Dirk Rothenstein and M. Sc. Binjie Tang for their kind supports during the experiments and discussions. The simulations presented in this work were performed on the computational resource For HLR II funded by the Ministry of Science, Research and the Arts Baden-W?rttemberg and the Deutsche Forschungsgemeinschaft.
PY - 2019/11/15
Y1 - 2019/11/15
N2 - Most of the currently used perovskite-based oxygen-transporting membranes have insufficient resistance towards CO2 and high material costs that potentially limit their commercial applications. In the present work, a highly CO2-tolerant oxygen permeation membrane based on La0.6Ca0.4Co1–xFexO3−δ (x = 0, 0.3, 0.5, 0.7, 1) was designed and prepared by a scalable reverse co-precipitation method. The oxygen permeation flux through the dense membranes was evaluated and found to be highly dependent on the Co/Fe ratio. La0.6Ca0.4Co0.3Fe0.7O3−δ possessed the highest permeation flux among the investigated samples, achieving 0.76 ml min−1 cm−2 under an Air/He gradient and 0.5 ml min−1 cm−2 under an Air/CO2 gradient at 1173 K for a 1 mm thick membrane. A combination study of first principles calculations and experimental measurements was conducted to advance the understanding of Co/Fe ratio effects on the oxygen migration behavior in La0.6Ca0.4Co1–xFexO3−δ. The observed oxygen permeability is three times higher than that reported in literature under similar conditions. The presented results demonstrate that this highly CO2-tolerant membrane is a promising candidate for high temperature oxygen separation applications.
AB - Most of the currently used perovskite-based oxygen-transporting membranes have insufficient resistance towards CO2 and high material costs that potentially limit their commercial applications. In the present work, a highly CO2-tolerant oxygen permeation membrane based on La0.6Ca0.4Co1–xFexO3−δ (x = 0, 0.3, 0.5, 0.7, 1) was designed and prepared by a scalable reverse co-precipitation method. The oxygen permeation flux through the dense membranes was evaluated and found to be highly dependent on the Co/Fe ratio. La0.6Ca0.4Co0.3Fe0.7O3−δ possessed the highest permeation flux among the investigated samples, achieving 0.76 ml min−1 cm−2 under an Air/He gradient and 0.5 ml min−1 cm−2 under an Air/CO2 gradient at 1173 K for a 1 mm thick membrane. A combination study of first principles calculations and experimental measurements was conducted to advance the understanding of Co/Fe ratio effects on the oxygen migration behavior in La0.6Ca0.4Co1–xFexO3−δ. The observed oxygen permeability is three times higher than that reported in literature under similar conditions. The presented results demonstrate that this highly CO2-tolerant membrane is a promising candidate for high temperature oxygen separation applications.
KW - CO resistance
KW - DFT
KW - Oxygen permeation membrane
KW - Oxygen vacancy formation energy
KW - Oxygen vacancy migration energy
KW - Perovskite
UR - http://www.scopus.com/inward/record.url?scp=85066309566&partnerID=8YFLogxK
U2 - 10.1016/j.memsci.2019.05.007
DO - 10.1016/j.memsci.2019.05.007
M3 - Article
AN - SCOPUS:85066309566
VL - 590
JO - Journal of membrane science
JF - Journal of membrane science
SN - 0376-7388
M1 - 117082
ER -