Oxygen permeation studies in surface Pd-activated asymmetric Ce0.9Gd0.1O1.95 membranes for application in CO2 and CH4 environments

Julio Garcia-Fayos, Martin Søgaard, Andreas Kaiser, Jose M. Serra*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

Oxygen Transport Membranes (OTMs) present a high potential for being considered in the integration of O2 supply systems in oxyfuel installations, as well as for the conduction of chemical reactions when operating Catalytic Membrane Reactors (CMRs). Several solutions are being prospected for overcoming the main drawbacks regarding materials stability and membrane performance. A highly stable material such as Ce0.9Gd0.1O1.95 (CGO) doped with 2% mol. Co was studied as a 40 μm-thick CGO supported CGO membrane. This membrane was characterized by studying its performance as oxygen permeation membrane for the production of oxygen under oxyfuel conditions and for the conduction of chemical reactions involving CH4. In order to improve oxygen surface reactions and consequently, the oxygen permeation, the membrane was surface activated with the addition of Pd nanoparticles. A broad characterization consisting of the study of O2 production under different environments simulating real application conditions was conducted by subjecting the membrane to Ar, CO2 and CH4 environments in the temperature range of 750 to 1000 °C. A peak oxygen flux of 7.8 ml·min−1·cm−2 was obtained at 1000 °C when using a sweep consisting of 75% CH4 in Ar. This flux corresponds to a 16-fold improvement in the O2 permeation at 1000 °C when sweeping with Ar, with an oxygen flux of 0.47 ml·min−1·cm−2. An oxygen flux of 1.2 ml·min−1·cm−2 was obtained at 1000 °C when feeding with pO2 = 1 atm in feed side. Membrane performance under CO2-containing environments showed a positive effect of CO2 on permeation at 1000–900 °C, reaching up to 0.59 ml·min−1·cm−2 O2 at 1000 °C. A continuous exposure of CO2 during 48 h at 750 °C resulted in a slight J(O2) increase, with a reversible reduction in performance when returning to clean conditions, thus demonstrating high stability of CGO membranes.
Original languageEnglish
JournalSeparation and Purification Technology
Volume216
Pages (from-to)58-64
ISSN1383-5866
DOIs
Publication statusPublished - 2019

Keywords

  • Cerium gadolinium oxide
  • Supported membrane
  • Catalyst
  • Tape casting
  • MIEC
  • Syngas
  • Oxyfuel

Cite this

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title = "Oxygen permeation studies in surface Pd-activated asymmetric Ce0.9Gd0.1O1.95 membranes for application in CO2 and CH4 environments",
abstract = "Oxygen Transport Membranes (OTMs) present a high potential for being considered in the integration of O2 supply systems in oxyfuel installations, as well as for the conduction of chemical reactions when operating Catalytic Membrane Reactors (CMRs). Several solutions are being prospected for overcoming the main drawbacks regarding materials stability and membrane performance. A highly stable material such as Ce0.9Gd0.1O1.95 (CGO) doped with 2{\%} mol. Co was studied as a 40 μm-thick CGO supported CGO membrane. This membrane was characterized by studying its performance as oxygen permeation membrane for the production of oxygen under oxyfuel conditions and for the conduction of chemical reactions involving CH4. In order to improve oxygen surface reactions and consequently, the oxygen permeation, the membrane was surface activated with the addition of Pd nanoparticles. A broad characterization consisting of the study of O2 production under different environments simulating real application conditions was conducted by subjecting the membrane to Ar, CO2 and CH4 environments in the temperature range of 750 to 1000 °C. A peak oxygen flux of 7.8 ml·min−1·cm−2 was obtained at 1000 °C when using a sweep consisting of 75{\%} CH4 in Ar. This flux corresponds to a 16-fold improvement in the O2 permeation at 1000 °C when sweeping with Ar, with an oxygen flux of 0.47 ml·min−1·cm−2. An oxygen flux of 1.2 ml·min−1·cm−2 was obtained at 1000 °C when feeding with pO2 = 1 atm in feed side. Membrane performance under CO2-containing environments showed a positive effect of CO2 on permeation at 1000–900 °C, reaching up to 0.59 ml·min−1·cm−2 O2 at 1000 °C. A continuous exposure of CO2 during 48 h at 750 °C resulted in a slight J(O2) increase, with a reversible reduction in performance when returning to clean conditions, thus demonstrating high stability of CGO membranes.",
keywords = "Cerium gadolinium oxide, Supported membrane, Catalyst, Tape casting, MIEC, Syngas, Oxyfuel",
author = "Julio Garcia-Fayos and Martin S{\o}gaard and Andreas Kaiser and Serra, {Jose M.}",
year = "2019",
doi = "10.1016/j.seppur.2019.01.068",
language = "English",
volume = "216",
pages = "58--64",
journal = "Separation and Purification Technology",
issn = "1383-5866",
publisher = "Pergamon Press",

}

Oxygen permeation studies in surface Pd-activated asymmetric Ce0.9Gd0.1O1.95 membranes for application in CO2 and CH4 environments. / Garcia-Fayos, Julio; Søgaard, Martin; Kaiser, Andreas; Serra, Jose M.

In: Separation and Purification Technology, Vol. 216, 2019, p. 58-64.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Oxygen permeation studies in surface Pd-activated asymmetric Ce0.9Gd0.1O1.95 membranes for application in CO2 and CH4 environments

AU - Garcia-Fayos, Julio

AU - Søgaard, Martin

AU - Kaiser, Andreas

AU - Serra, Jose M.

PY - 2019

Y1 - 2019

N2 - Oxygen Transport Membranes (OTMs) present a high potential for being considered in the integration of O2 supply systems in oxyfuel installations, as well as for the conduction of chemical reactions when operating Catalytic Membrane Reactors (CMRs). Several solutions are being prospected for overcoming the main drawbacks regarding materials stability and membrane performance. A highly stable material such as Ce0.9Gd0.1O1.95 (CGO) doped with 2% mol. Co was studied as a 40 μm-thick CGO supported CGO membrane. This membrane was characterized by studying its performance as oxygen permeation membrane for the production of oxygen under oxyfuel conditions and for the conduction of chemical reactions involving CH4. In order to improve oxygen surface reactions and consequently, the oxygen permeation, the membrane was surface activated with the addition of Pd nanoparticles. A broad characterization consisting of the study of O2 production under different environments simulating real application conditions was conducted by subjecting the membrane to Ar, CO2 and CH4 environments in the temperature range of 750 to 1000 °C. A peak oxygen flux of 7.8 ml·min−1·cm−2 was obtained at 1000 °C when using a sweep consisting of 75% CH4 in Ar. This flux corresponds to a 16-fold improvement in the O2 permeation at 1000 °C when sweeping with Ar, with an oxygen flux of 0.47 ml·min−1·cm−2. An oxygen flux of 1.2 ml·min−1·cm−2 was obtained at 1000 °C when feeding with pO2 = 1 atm in feed side. Membrane performance under CO2-containing environments showed a positive effect of CO2 on permeation at 1000–900 °C, reaching up to 0.59 ml·min−1·cm−2 O2 at 1000 °C. A continuous exposure of CO2 during 48 h at 750 °C resulted in a slight J(O2) increase, with a reversible reduction in performance when returning to clean conditions, thus demonstrating high stability of CGO membranes.

AB - Oxygen Transport Membranes (OTMs) present a high potential for being considered in the integration of O2 supply systems in oxyfuel installations, as well as for the conduction of chemical reactions when operating Catalytic Membrane Reactors (CMRs). Several solutions are being prospected for overcoming the main drawbacks regarding materials stability and membrane performance. A highly stable material such as Ce0.9Gd0.1O1.95 (CGO) doped with 2% mol. Co was studied as a 40 μm-thick CGO supported CGO membrane. This membrane was characterized by studying its performance as oxygen permeation membrane for the production of oxygen under oxyfuel conditions and for the conduction of chemical reactions involving CH4. In order to improve oxygen surface reactions and consequently, the oxygen permeation, the membrane was surface activated with the addition of Pd nanoparticles. A broad characterization consisting of the study of O2 production under different environments simulating real application conditions was conducted by subjecting the membrane to Ar, CO2 and CH4 environments in the temperature range of 750 to 1000 °C. A peak oxygen flux of 7.8 ml·min−1·cm−2 was obtained at 1000 °C when using a sweep consisting of 75% CH4 in Ar. This flux corresponds to a 16-fold improvement in the O2 permeation at 1000 °C when sweeping with Ar, with an oxygen flux of 0.47 ml·min−1·cm−2. An oxygen flux of 1.2 ml·min−1·cm−2 was obtained at 1000 °C when feeding with pO2 = 1 atm in feed side. Membrane performance under CO2-containing environments showed a positive effect of CO2 on permeation at 1000–900 °C, reaching up to 0.59 ml·min−1·cm−2 O2 at 1000 °C. A continuous exposure of CO2 during 48 h at 750 °C resulted in a slight J(O2) increase, with a reversible reduction in performance when returning to clean conditions, thus demonstrating high stability of CGO membranes.

KW - Cerium gadolinium oxide

KW - Supported membrane

KW - Catalyst

KW - Tape casting

KW - MIEC

KW - Syngas

KW - Oxyfuel

U2 - 10.1016/j.seppur.2019.01.068

DO - 10.1016/j.seppur.2019.01.068

M3 - Journal article

VL - 216

SP - 58

EP - 64

JO - Separation and Purification Technology

JF - Separation and Purification Technology

SN - 1383-5866

ER -