@inproceedings{IsraelRachowSchwiertzetal., author = {Israel, Johannes and Rachow, Fabian and Schwiertz, Carola and Charlafti, Evgenia and M{\"u}ller, Klaus and Schmeißer, Dieter}, title = {Self restriction oft the Sabatier reaction in large scale}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, abstract = {A main goal for a sustainable energy supply is a long term energy storage system. One opportunity in this research field is the power to gas concept, where the produced gas can be fed in the existing network of natural gas. Here we show in a technical scale how the direct CO2 conversion to methane according the Sabatier reaction, CO2 + 4 H2 → CH4 + 2H2O , is self organized. At a certain limit of gas flow, a steady state equilibrium of exothermic heat production and thermal flow is reached and the reaction needs no further external annealing. We find for the maximum volume rate at the steady state equilibirum a shift of around 250 ∘C above the optimized temperature of the catalytic supported chemical equilibrium. It is shown that also with this setup the used catalyst works with a stable conversion higher than 80 \% under the reached temperature and given pressure conditions.}, language = {en} } @inproceedings{RachowIsraelSchwiertzetal., author = {Rachow, Fabian and Israel, Johannes and Schwiertz, Carola and Charlafti, Evgenia and M{\"u}ller, Klaus and Schmeißer, Dieter}, title = {CO2 Methanation with different gas mixtures}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, pages = {S. 539}, abstract = {A key issue in the Energiewende in Germany is the storage of excess energy, as it enables energy management systems to react to fluctuating sources and enhances the flexibility of an energy mix. Power to Gas may be the most reasonable approach to store the energy in the form of hydrogen or synthetic natural gas. We study the direct conversion of CO2 by the Sabatier reaction to gain a methane based mixture which can replace natural gas in CHP plants and gas motors and can help to partially reduce the CO2 emission. In laboratory scale we investigated the performance (with IR and QMS) of Ni-based catalyst for different sources of CO2 like clean CO2, CO2 emitted as flue gas from an Oxyfuel power plant or a synthetic mixture with O2, N2 and SO2 in concentration typical for conventional power plants. Measurements from an up-scaled system are also presented, showing data important for a technical application. Here, we are able to convert more than 200kg CO2/day with conversion rates up to 90\%.}, 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} } @inproceedings{IsraelRachowSchwiertzetal., author = {Israel, Johannes and Rachow, Fabian and Schwiertz, Carola and Charlafti, Evgenia and M{\"u}ller, Klaus and Schmeißer, Dieter}, title = {Direct CO2-Methanation of flue gas emitted by conventional power plants}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, pages = {S. 255}, abstract = {The catalytic conversion of CO2 with H2 into CH4 is possible by the Sabatier reaction CO2+4H2→CH4+2H2O. Using excess energy from renewable electricity generation, this approach offers an opportunity for recycling of CO2 as synthetic natural gas. In a new concept, we investigate the performance of the Sabatier reaction as direct methanation of flue gas, emitted by conventional power plants. We investigate the Sabatier process in an upscaled system, with a maximum input flow rate of 45 Nm3/h Gas. The performance is investigated in a simulated composition of flue gas and under real conditions at a lignite power plant in Schwarze Pumpe, Brandenburg, Germany. We can achieve a CO2-conversion of up to 90\%, with approx. 100\% selectivity towards CH4. Under flue gas conditions and at a certain limit of gas flow the system is operated at an autothermal running modus, a steady state equilibrium of exothermic heat production and thermal flow that needs neither external annealing nor cooling.}, language = {en} }