@inproceedings{MuellerHoffmannbeckKirneretal., author = {M{\"u}ller, Klaus and Hoffmannbeck, David and Kirner, Georg and St{\"a}dter, Matthias and Schmeißer, Dieter}, title = {CO2-Methanation by Catalytic Conversion}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, abstract = {The utilization of CO2 as raw material is an important component of a program for CO2 reduction. A possibility is the production of methane. At a moderate temperature of around 350°C, hydrogenation of CO2 to methane is possible by the Sabatier reaction CO2 + 4H2 ->CH4 +2H2O. Prerequisite for an efficient kinetics of the Sabatier reaction is the application and optimization of catalysts. In this contribution, we present investigations of Ru and Ni catalysts on different substrates. For Ru/Al2O3 catalysts, we found stable operation without degradation within 500 hours with a conversion rate of 80\% at 350°C. For NiO/SiO2 catalysts, a conversion rate of 90\% was found for temperatures of 350-405°C. We also show the investigation of cross sensitivities against SOx and NOx, which are typical contaminations of CO2, generated by the industrial oxyfuel process. In our work the morphology (REM, AFM, specific surface), chemical composition (FTIR, XPS) and phase composition (XRD) of the catalysts are characterized. In addition, we report on thermodesorption (TDS) measurements at atmospheric pressure to determine the amount of adsorbed CO2 under real conditions. The project is funded by the German Ministry of Research and Education (BMBF-GeoEn).}, language = {en} } @inproceedings{StaedterSchmeisser, author = {St{\"a}dter, Matthias and Schmeißer, Dieter}, title = {AP-TDS characterization of CO2 methanation catalysts}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft, Reihe 6, Bd. 47}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft, Reihe 6, Bd. 47}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, abstract = {Development of new catalysts and their characterization by TDS (thermal desorption spectroscopy) is used in a wide field of applications. In our group we focus on catalysts usable to convert CO2 towards methane by the Sabatier reaction (CO2 + 4H2 → CH4 + 2H2O at 375∘C). For measuring large numbers of samples we designed an AP-TDS (ambient pressure TDS) chamber where various desorption experiments can be performed without bringing the catalyst into vacuum. The well-defined reaction chamber, in terms of temperature, pressure and gas composition (Ar atmosphere), is separated by a pin hole (∅ = 6 µ m) from an external UHV chamber. Evolving species and their composition are monitored by a mass spectrometer attached to the UHV chamber. Our first measurement results on commercially available NiO/SiO2 and Ru/Al2O3 based catalysts, with focus on the identification and enumeration of different adsorption sites for CO2, will be presented. CO2 saturated samples were heated from RT to 1100∘C (heating rate β = 0.3 K/s) while measuring the evolution of the CO2 content. Our measurements show large numbers of different adsorption sites for NiO (200-750∘C) whereas Ru shows only few different sites around 440∘C. For both catalysts, most of the formerly adsorbed CO2 remains at the surface (at 375∘C) available for methanation.}, language = {en} } @inproceedings{TallaridaMichlingDasetal., author = {Tallarida, Massimo and Michling, Marcel and Das, Chittaranjan and Friedrich, Daniel and St{\"a}dter, Matthias and Schmeißer, Dieter}, title = {Role of substrate chemistry in ALD revealed by in-situ techniques}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft, Reihe 6, Bd. 47}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft, Reihe 6, Bd. 47}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, abstract = {We show recent results of our in-situ investigations where the role of substrate chemistry in ALD is outlined. While the usual strategy to develop new properties of ALD films is to find new precursors or new procedures, the influence of substrate chemistry on the growth properties of ALD films has been often underestimated. This has principally a technical reason, as the usual characterization methods (QMS, FTIR, ellipsometry) are only weakly sensitive to the substrate, and a characterization of substrates before ALD is often not possible. Thanks to the use of in-situ characterization methods, including photoemission and X-ray absorption spectroscopy with synchrotron radiation, we are able to determine chemical properties of substrates before ALD and after either half or complete ALD cycles. The substrate chemistry influences the standard Al2O3 ALD with TMA and water [1,2], as well as the TiO2 ALD with TTIP and either water, O2 or O2-plasma. [1] M. Tallarida, K. Kukli, M. Michling, M. Ritala, M. Leskel{\"a} and D. Schmeisser, Chem. Mater. 23, 3159 (2011); [2] M. Tallarida, C. Adelmann, A. Delabie, S. van Elshocht, M. Caymax, and D. Schmeisser, Appl. Phys. Lett. 92, 042906 (2011).}, language = {en} }