Advancing oxygen separation: insights from experimental and computational analysis of La0.7Ca0.3Co0.3Fe0.6M0.1O3–δ (M = Cu, Zn) oxygen transport membranes

doi:10.1007/s11705-024-2421-5

2024, Vol. 18

Issue (6) : 62 https://doi.org/10.1007/s11705-024-2421-5

Advancing oxygen separation: insights from experimental and computational analysis of La_0.7Ca_0.3Co_0.3Fe_0.6M_0.1O_3–δ (M = Cu, Zn) oxygen transport membranes

Guoxing Chen¹(

), Wenmei Liu², Marc Widenmeyer³, Xiao Yu¹, Zhijun Zhao⁴, Songhak Yoon¹, Ruijuan Yan³, Wenjie Xie^1,³, Armin Feldhoff⁴, Gert Homm¹, Emanuel Ionescu^1,³, Maria Fyta^5,⁶(

), Anke Weidenkaff^1,³

¹. Fraunhofer Research Institution for Materials Recycling and Resource Strategies IWKS, Alzenau 63755, Germany
². Electrochemistry Laboratory, Paul Scherrer Institute, Villigen PSI 5232, Switzerland
³. Department of Materials and Earth Sciences, Materials and Resources, Technical University of Darmstadt, Darmstadt 64287, Germany
⁴. Institute of Physical Chemistry and Electrochemistry, Leibniz University Hannover, Hannover 30167, Germany
⁵. Institute for Computational Physics, University of Stuttgart, Stuttgart 70569, Germany
⁶. Computational Biotechnology, RWTH Aachen, Aachen 52074, Germany

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Abstract

In this study, perovskite-type La_0.7Ca_0.3Co_0.3Fe_0.6M_0.1O_3–δ (M = Cu, Zn) powders were synthesized using a scalable reverse co-precipitation method, presenting them as novel materials for oxygen transport membranes. The comprehensive study covered various aspects including oxygen permeability, crystal structure, conductivity, morphology, CO₂ tolerance, and long-term regenerative durability with a focus on phase structure and composition. The membrane La_0.7Ca_0.3Co_0.3Fe_0.6Zn_0.1O_3–δ exhibited high oxygen permeation fluxes, reaching up to 0.88 and 0.64 mL·min⁻¹·cm⁻² under air/He and air/CO₂ gradients at 1173 K, respectively. After 1600 h of CO₂ exposure, the perovskite structure remained intact, showcasing superior CO₂ resistance. A combination of first principles simulations and experimental measurements was employed to deepen the understanding of Cu/Zn substitution effects on the structure, oxygen vacancy formation, and transport behavior of the membranes. These findings underscore the potential of this highly CO₂-tolerant membrane for applications in high-temperature oxygen separation. The enhanced insights into the oxygen transport mechanism contribute to the advancement of next-generation membrane materials.

Keywords perovskite oxygen permeation membrane oxygen ions diffusion oxygen vacancy formation energy energy barrier

Corresponding Author(s): Guoxing Chen,Maria Fyta

About author:

Li Liu and Yanqing Liu contributed equally to this work.

Just Accepted Date: 04 February 2024 Issue Date: 22 April 2024

Cite this article:

Guoxing Chen,Wenmei Liu,Marc Widenmeyer, et al. Advancing oxygen separation: insights from experimental and computational analysis of La_0.7Ca_0.3Co_0.3Fe_0.6M_0.1O_3–δ (M = Cu, Zn) oxygen transport membranes[J]. Front. Chem. Sci. Eng., 2024, 18(6): 62.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-024-2421-5
https://academic.hep.com.cn/fcse/EN/Y2024/V18/I6/62

Fig.1 (a) A ball and stick model of the LCCFM perovskite structure with alternating layers of AO⁺ and

BO 2 ?

, where A stands for La/Ca, and B stands for Fe/Co/Cu/Zn (the La, Ca, Fe, Co, M = Fe/Cu/Zn, and O atoms are colored purple, green, orange, blue, cyan, and red, respectively). (b) We consider three types of oxygen vacancy locations a, b, and c, which are coordination-dependent and represented as V_a, V_b, and V_c, respectively.

Fig.2 Rietveld refinements of XRD patterns of the investigated perovskite-type powders at room temperature: (a) LCCFFe, (b) LCCFCu, and (c) LCCFZn.

Fig.3 SEM micrographs of fresh membranes: (a) LCCFFe, (b) LCCFCu, and (c) LCCFZn.

Fig.4 TG-curves of the fresh membranes under (a) Ar, (b) air, and (c) CO₂ atmospheres.

Fig.5 XRD patterns of the investigated membranes after exposure to CO₂ at 1173 K for various times: (a) LCCFFe, (b) LCCFCu, and (c) LCCFZn. (d) XRD patterns of the studied membranes after exposure to CO₂ plasma at 1173 K for 3 h.

Fig.6 Temperature dependence of (a) the total conductivity and (b) its Arrhenius plot of fresh membranes.

Fig.7 (a) Oxygen permeation fluxes through LCCFM membranes under air/He gradient, air/CO₂ gradient, and 80% air-20% CO₂/He gradient; (b) oxygen permeation flux through LCCFZn membrane under (100–x)% air-x% CO₂/He gradient.

Fig.8 The formation energy of a single oxygen vacancy in LCCFM with respect to their environment and increasing distance to M. The coordination of corresponding atoms is represented by a, b, and c (see Fig. 1).

Fig.9 Barrier energy of oxygen migration to next-neighbor (N) sites of LCCFM (M = Fe, Cu, and Zn). The cases corresponding to the largest/lowest barriers are indicated by the circular red/cyan regions.

Fig.10 Potential pathways of oxygen migration in (a) LCCFZn, (b) LCCFFe, and (c) LCCFCu (TS: transition state).

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