Membrane-based oxy-combustion is a promising technology for energy efficient combustion of carboncontaining fuels with the simultaneous opportunity to capture CO2 from the resulting exhaust gas.However, oxy-combustion conditions result in special demands on the design of the ceramic membrane components due to the high pressure and temperature applied. Therefore, we have developed a planar membrane design for 4-end operation using asymmetric membranes of La0.6Sr0.4Co0.2Fe0.8O3-δ. FEM and CFD simulations have been performed in order to develop an internal channel structure that allows withstanding pressures of 5 bar on the feed side while achieving the desired O2 concentrations of 27 % in the sweep gas, i.e. CO2, and an oxygen recovery rate from the feed gas of 86 % at the same time.Due to the symmetric design of the membrane components, they are scalable and adaptable in size. This design has been realized in a process chain from powder to the final component consisting of thin 20 µm Membrane layer, support with 38 % porosity, an inner channelled architecture and a thin (3-5 µm) porous activation layer. Particular emphasis was laid on scalable manufacturing processes in order to ensure transferability to industrial scale. The process chain is also applicable to other membrane materials suitable for any application of interest. Finally, the reproducible processing was successfully demonstrated by the fabrication of membrane components in lengths of 100 mm and widths of 70 mm.

The present work is focused on the investigation of the performance and long-term stability of two composite palladium membranes under different operating conditions. One membrane (Pd/porous stainless steel (PSS)) is characterized by a ~10 µm-thick palladium layer on a porous stainless steel substrate, which is pretreated by means of surface modification and oxidation; the other membrane (Pd/Al2O3) is constituted by a ~7 µm-thick palladium layer on an asymmetric microporous Al2O3 substrate. The operating temperature and pressure ranges, used for studying the performance of these two kinds of membranes, are 350–450 °C and 200–800 kPa, respectively. The H2 permeances and the H2/N2 selectivities of both membranes were investigated and compared with literature data. At 400 °C and 200 kPa as pressure difference, Pd/PSS and Pd/Al2O3 membranes exhibited an H2/N2 ideal selectivity equal to 11700 and 6200, respectively, showing stability for 600 h. Thereafter, H2/N2 selectivity of both membranes progressively decreased and after around 2000 h, dropped dramatically to 55 and 310 for the Pd/PSS and Pd/Al2O3 membranes, respectively. As evidenced by Scanning Electron Microscope (SEM) analyses, the pinholes appear on the whole surface of the Pd/PSS membrane and this is probably due to release of sulphur from the graphite seal rings.

Powders of constant morphology and quality are indispensable for reproducible ceramic manufacturing. In this study, commercially available powders were characterized regarding their microstructural properties and screened for a reproducible membrane manufacturing process, which was done by sequential tape casting. Basing on this, the slurry composition and ratio of ingredients were systematically varied in order to obtain flat, crack-free green tapes suitable for upscaling of the manufacturing process. Debinding and sintering parameters were adjusted to obtain defect-free membranes with diminished bending. The crucial parameters are the heating ramp, sintering temperature, and dwell time. The microstructure of the asymmetric membranes was investigated, leading to a support porosity of approximately 35% and a membrane layer thickness of around 20 µm. Microstructure and oxygen flux are comparable to asymmetric La0.6Sr0.4Co0.2Fe0.8O3−δ (LSCF) membranes manufactured from custom-made powder, showing an oxygen flux of > 1 mL⋅cm−2⋅min at 900 °C in air/Ar gradient.

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