A CO and CO₂ tolerating (La_0.9Ca_0.1)₂(Ni_0.75Cu_0.25)O_4+d Ruddlesden-Popper membrane for oxygen separation

Abstract

A series of novel dense mixed conducting ceramic membranes based on K₂NiF₄-type (La_1–xCa_x)₂ (Ni_0.75Cu_0.25)O_4+δ was successfully prepared through a sol-gel route. Their chemical compatibility, oxygen permeability, CO and CO₂ tolerance, and long-term CO₂ resistance regarding phase composition and crystal structure at different atmospheres were studied. The results show that higher Ca contents in the material lead to the formation of CaCO₃. A constant oxygen permeation flux of about 0.63 mL·min⁻¹·cm⁻² at 1173 K through a 0.65 mm thick membrane was measured for (La_0.9Ca_0.1)₂ (Ni_0.75Cu_0.25)O_4+δ, using either helium or pure CO₂ as sweep gas. Steady oxygen fluxes with no sign of deterioration of this membrane were observed with increasing CO₂ concentration. The membrane showed excellent chemical stability towards CO₂ for more than 1360 h and phase stability in presence of CO for 4 h at high temperature. In addition, this membrane did not deteriorate in a high-energy CO₂ plasma. The present work demonstrates that this (La_0.9Ca_0.1)₂(Ni_0.75Cu_0.25)O_4+δ membrane is a promising chemically robust candidate for oxygen separation applications.

Key words： K₂NiF₄ structure; oxygen permeation membrane; CO₂ and CO resistances; CO₂ plasma resistance; long-term robustness

Acknowledgments

This work is part of the project “Plasma-induced CO₂-conversion” (PiCK, project number: 03SFK2S3B) and financially supported by the German Federal Ministry of Education and Research in the framework of the “Kopernikus projects for the Energiewende”. The authors are thankful to B.Sc. Laura Steinle (University of Stuttgart) for her assistance during the CO stability tests, and Christine Stefani and Prof. Dr. Robert Dinnebier (Max Planck Institute for Solid State Research, Stuttgart) for the in situ PXRD measurements, respectively. G. C. thanks Frank Hack and Dr. Angelika Veziridis for their kind support during experiments and discussions.

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11705-019-1886-0 and is accessible for authorized users.

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