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IC4 FUNDED PROJECTS of membrane bundles have now undergone testing at Linde. The materials demonstrated a reversible CO2 absorption capacity previously unattained for polymer-based systems and could be processed to yield defect-free ho- mogeneous films. The thin polyelectrolyte films on TPSE support membra- nes exhibited highly competitive CO2 flow rates and ideal CO2/N2 selectivi- ty values of up to 67.7. In order to achieve a more tightly packed, selective membrane material attempts were made to achieve the stereoregular poly- merisation of 4-vinyl phenol. However, it was not possible to achieve any si- gnificant stereoregularity within the polymer chain even under the mildest reaction conditions. Characterisation of the membrane technology under realistic operational conditions (mixed gases and presence of water vapour), ideally under permanent loading and with the system in its steady state, was accomplished while the membrane module (Fraunhofer IGB) and the pilot plant (Linde AG) were under construction. The COOMeth subproject was central to the collaborative research project iC4 and was concerned with developing high-efficiency catalysts as well as a hydrogenation strategy that was compatible with the overall process. Both of these objectives were met. At the end of the subproject, the team had de- veloped a catalytic process with optimised catalysts and a customised reac- tor that enables the continuous conversion of CO2 to methane with yields of over 96% and that is characterised by simple reactor throughput, high selec- tivity and a long service life. One of the achievements of the subproject was the development of effi- cient nickel catalysts for the methanation of carbon dioxide that exhibited high thermal stability and good resistance to high concentrations of water vapour. The properties of more than 500 candidate catalysts were examined under realistic conditions; the catalysts were tested with the aid of a paral- lel reactor system operated by WACKER Chemie AG. The experiments were planned and evaluated using concepts from DOE (design of experiments) methodology and multivariate data analysis. The nickel-supported catalysts fabricated using a variety of impregnation methods showed only moderate activity in the Sabatier (methanation) reac- tion. However, the experimental data indicates that by optimising the calci- nation process, catalysts of satisfactory activity with moderate metal loading can be produced. The addition of small amounts of promoters can signifi- cantly increase the activity of the nickel catalysts. Certain promoters also help to increase the stability of the catalyst in the harsh reaction conditions that arise in large-scale industrial applications. The promoter-doped fully impregnated nickel catalysts achieved the maximum possible conversion of CO2 at the relatively low temperature of 250 °C and a GHSV of 35,000 h-1. The methane yield with these systems was always above 95%. 157PDF Image | Chemical Processes and Use of CO2
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