Effect of doping, microstructure, and CO{sub 2} on La{sub 2}NiO{sub 4+{delta}}-based oxygen-transporting materials

Journal Article · Thu Dec 15 04:00:00 EST 2011 · Journal of Solid State Chemistry

DOI:https://doi.org/10.1016/j.jssc.2011.10.019· OSTI ID:21612833

Klande, Tobias ^[1]; Efimov, Konstantin ^[1]; Cusenza, Salvatore; Becker, Klaus-Dieter ^[2]; Feldhoff, Armin ^[1]

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1. Institute of Physical Chemistry and Electrochemistry, Leibniz Universitaet Hannover, Callinstr. 3-3a, D-30179 Hannover (Germany)
2. Institute of Physical and Theoretical Chemistry, Technische Universitaet Braunschweig, Hans-Sommer-Str. 10, D-38106 Braunschweig (Germany)

Alkaline earth-free La{sub 2}NiO{sub 4+{delta}} based materials were synthesized by a sol-gel method and studied by X-ray diffraction (XRD), scanning electron microscopy (SEM) and transmission electron microscopy (TEM) techniques as well as oxygen permeation experiments. Effects of doping the nickel position with a variety of cations (Al, Co, Cu, Fe, Mg, Ta, and Zr) were investigated with regards to oxygen flux and microstructure. Doping was always found to diminish the oxygen flux as compared to the reference composition. However, larger grains, which were achieved by longer annealing times at 1723 K have a minor negative impact on oxygen permeation flux in case of La{sub 2}NiO{sub 4+{delta}} and La{sub 2}Ni{sub 0.9}Fe{sub 0.1}O{sub 4+{delta}} system. Moessbauer spectroscopy shows that the iron-doped system exhibits a secondary phase, which was identified by high-resolution transmission electron microscopy (HRTEM) as a higher Ruddlesden-Popper phase. In-situ XRD in an atmosphere containing 50 vol% CO{sub 2} and long-term oxygen permeation experiments using pure CO{sub 2} as the sweep gas revealed a high tolerance of the materials towards CO{sub 2}. - Graphical Abstract: The vibrational polished La{sub 2}Ni{sub 0.9}Fe{sub 0.1}O{sub 4+{delta}} membrane revealed formation of secondary phases, which were confirmed by Moessbauer spectroscopy. Highlights: Black-Right-Pointing-Pointer La{sub 2}NiO{sub 4+{delta}} systematically doped with different valent cations. Black-Right-Pointing-Pointer Large grains have a negative impact on oxygen-permeation performance. Black-Right-Pointing-Pointer CO{sub 2}-stability proved by in-situ XRD in 50 vol% CO{sub 2}. Black-Right-Pointing-Pointer Constant long-term permeation in presence of CO{sub 2}. Black-Right-Pointing-Pointer Moessbauer and TEM reveal multiple phases in La{sub 2}Ni{sub 0.9}Fe{sub 0.1}O{sub 4+{delta}} system.

• OSTI ID: 21612833
• Journal Information: Journal of Solid State Chemistry, Journal Name: Journal of Solid State Chemistry Journal Issue: 12 Vol. 184; ISSN 0022-4596; ISSN JSSCBI
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CARBON COMPOUNDS
CARBON DIOXIDE
CARBON OXIDES
CATIONS
CHALCOGENIDES
CHARGED PARTICLES
COHERENT SCATTERING
DIFFRACTION
DOPED MATERIALS
ELECTRON MICROSCOPY
ELEMENTS
IONS
IRON
MATERIALS
MEMBRANES
METALS
MICROSCOPY
MICROSTRUCTURE
MOESSBAUER EFFECT
NICKEL
NONMETALS
OXIDES
OXYGEN
OXYGEN COMPOUNDS
SCANNING ELECTRON MICROSCOPY
SCATTERING
SOL-GEL PROCESS
STABILITY
TRANSITION ELEMENTS
TRANSMISSION ELECTRON MICROSCOPY
X-RAY DIFFRACTION