@misc{MuellerFleigeRachowetal., author = {M{\"u}ller, Klaus and Fleige, Michael and Rachow, Fabian and Schmeißer, Dieter}, title = {Sabatier based CO2-methanation of flue gas emitted by conventional power plants}, series = {Energy Procedia}, volume = {40}, journal = {Energy Procedia}, issn = {1876-6102}, doi = {10.1016/j.egypro.2013.08.028}, pages = {240 -- 248}, abstract = {The hydrogenation CO2+ 4H2 ->CH4 + 2H2O discovered by Paul Sabatier nowadays is discussed as "Power-to-approach" to utilize excess energy from renewable electricity generation. In a laboratory scale, we investigate the Sabatier process in a simulated flue gas atmosphere of conventional base load power plants. The reaction is investigated with regard to conversion rates, yield, selectivity and long-term stability. Using a catalyst based on nickel,we extract selectivities near 100\% with a conversion around 85\%. Beside the influence of oxygen, we investigate further typical contaminations like NO2 and SO2.}, language = {en} } @misc{MuellerStaedterRachowetal., author = {M{\"u}ller, Klaus and St{\"a}dter, Matthias and Rachow, Fabian and Hoffmannbeck, David and Schmeißer, Dieter}, title = {Sabatier-based CO2-methanation by catalytic conversion}, series = {Environmental Earth Sciences}, volume = {70}, journal = {Environmental Earth Sciences}, number = {8}, issn = {1866-6280}, doi = {10.1007/s12665-013-2609-3}, pages = {3771 -- 3778}, abstract = {The catalytic conversion of CO2is an important component for the reintegration of secondary products like CO2 or H2 into the energy supply. An example is the "power to gas'" concept with a conversion of CO2 into CH4. The CO2 is transferred into a carrier of chemical energy, with the possibility to feed the produced CH4 into the existing network of natural gas. At temperatures of around 350 °C, hydrogenation of CO2 to CH4 is possible by the Sabatier reaction CO2+4H2->CH4+H2O. One prerequisite for efficient kinetics of the Sabatier reaction is the application and optimization of catalysts. The focus of catalyst development is given to their performance under the conditions to be expected in the special application. As a part of the project Geoenergy-Research (GeoEn), we address questions related to the catalytic utilization of CO2 produced in the course of the oxyfuel combustion of lignite. In this contribution, we report on the experimental setup in laboratory scale, which enables an advanced characterization of the catalytic performance, including thermodesorption measurements at atmospheric pressure in order to determine the amount of adsorbed CO2 under real conditions. We also show data for activation energies, the catalytic performance as function of temperature and the long time stability of a commercial Ru-based catalyst.}, language = {en} } @misc{StaedterMuellerRachowetal., author = {St{\"a}dter, Matthias and M{\"u}ller, Klaus and Rachow, Fabian and Richter, Matthias and Schmeißer, Dieter}, title = {Ambient pressure thermal desorption spectroscopy (AP-TDS) of NiO/SiO2 catalysts}, series = {Environmental Earth Sciences}, volume = {70}, journal = {Environmental Earth Sciences}, number = {8}, issn = {1866-6280}, doi = {10.1007/s12665-013-2835-8}, pages = {3779 -- 3784}, abstract = {The Sabatier reaction is a key process in the "power-to-gas" application which is considered to con-tribute to future chemical energy storage systems. In this contribution we focus on the catalytic active sites of a NiO catalyst supported on SiO2(NiO/SiO2) which is commonly used in the Sabatier reaction. A novel technique for the characterization of the active sites is presented and dis-cussed using thermal desorption spectroscopy at ambient pressure. This analytical tool is operated under reaction conditions and allows element specific measurements during the catalytic process of CO2 reforming towards methane. Beside the desorption experiments, XPS and XAS measurements of pristine and catalytically used samples are performed to determine the influence of the Sabatier reaction conditions on the surface structure of the catalyst.}, language = {en} } @inproceedings{FleigeMuellerSchmeisser, author = {Fleige, Michael and M{\"u}ller, Klaus and Schmeißer, Dieter}, title = {Sabatier based CO2-Methanation of flue gas in conventional power plants}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, abstract = {Already discovered by Paul Sabatier in 1902 the Hydrogenation according to CO2 + 4H2 ->CH4 + 2H2O nowadays is discussed in the course of the 'Power-to-Gas' approach to utilize excess energy from renewable electricity generation in times of oversupply of electricity. We investigate the behavior of this process in a simulated flue gas atmosphere of conventional base load power plants, which could be used as constant sources of the reactant CO2. Therefore the influence of different flue gas compositions such as varying contents of nitrogen and residual oxygen are tested in a laboratory scale. The heterogeneous catalysis process is investigated with regard to conversion rates, yield and selectivity and long-term stability of the Ni-catalyst. Earlier results of stable operating conditions in a 1:1 mixture of nitrogen and reactants, which is a typical ratio for flue gas in conventional power plants, could be confirmed in a first step.}, language = {en} } @inproceedings{IsraelMuellerRachowetal., author = {Israel, Johannes and M{\"u}ller, Klaus and Rachow, Fabian and Beuckert, Guido and Schmeißer, Dieter}, title = {Reaction kinetics of the Sabatier Reaction in a demonstration plant}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, abstract = {We currently build up a demonstration plant for the direct catalytic conversion of CO2 into methane according to the Sabatier reaction CO2+4H2→CH4+2H2O. We have already reached conversion rates higher than 90\% and a selectivity close to unity in our laboratory experiments with NiO based catalysts. A good long term stability was obtained with a reactant gas flow density of 0.8 l/min cm2· at 350∘C. We will study the process now on a larger scale with a factor 10000. The process is controlled via mass flow controllers with a throughput of 20m3/h H2 and 5m3/h CO2 at an inlet gas pressure of up to 15 bar, the temperature is regulated by a PID multichannel controller. As water is a by-product we use an efficient cooling trap for its separation form the obtained methane. The reaction products are analyzed by a quadrupole mass spectrometer under reaction conditions. We start our experiments in using clean CO2 and H2. Later experiments will involve industrial quality (oxy-fuel) conditions also. Goal of this project is to determine the performance of the catalytic process under conditions which enable an industrial implementation in energy storage concepts. In this contribution we report of the design of a demonstration plant and on first experiments concerning the kinetics within the system.}, language = {en} } @inproceedings{RachowMuellerSchmeisser, author = {Rachow, Fabian and M{\"u}ller, Klaus and Schmeißer, Dieter}, title = {Sabatier based Methanation of carbon dioxide and Catalyst stability against contaminations}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, abstract = {The Sabatier-Reaction [CO2+4H2→CH4+2H2O] represents a possible way for the reduction and utilization of CO2 produced in the oxy-fuel combustion process. While using different ruthenium and nickel based catalysts we studied the catalytic performance with quadrupole mass spectroscopy and IR-spectroscopy in terms of conversion of CO2,yield of CH4, selectivity and stability. Conversions of up to 90\% and a selectivity of well above 95\% could be achieved. Further studies focus on the long term stability, especially with the influence of contaminations like SOx and NOx as they may occur in oxy-fuel or flue gas and could greatly reduce the life time of a catalyst. We investigate the limits of Ni based catalysts for those additives. However, technical oxy-fuel gas seems to have no particular effect on the activity of a commonly used NiO-catalyst when compared to quasi pure CO2 , showing only a small drop of performance after five days with a constant conversion rate of over 80\% at the end.}, language = {en} }