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The direct synthesis of methanol [CO2+3H2->CH3OH+H2O]
represent a possibility to reduce the global CO2-emission by recycling the CO2 and also to store excess energy from renewable energy sources into a common fuel or chemical feedstock (Power-to-Liquid). For an acceptable conversion rate of CO2 a catalyst is needed, together with
high temperatures (>200°C) and high pressure (50-200bar). Methanol is normally produced form synthesis gas, a mixture of CO and H2. By directly using CO2 for the exothermic reaction, we avoid the conversion of CO2 to CO by the reversed water gas shift reaction. We also present
new concepts for the conversion from CO2-rich flue gases, eliminating the need for a separation of the CO2. The concept is backed up by
measurements in laboratory scale. Here we use a Cu−ZnO
catalyst on a ZrO2 substrate prepared by impregnation and compare the results with commercially available catalysts. We achieved a conversion of around 7% and a selectivity of 60% at a temperature of 240°C and
45bar. The reaction is thermodynamically limited with a maximum conversion rate of 15% at 250°C and 50bar. The conversion and the
selectivity towards methanol is highly influenced by the catalyst used, the temperature, the pressure as well as the flow rate of the reactants.
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.
Sabatier-Based Direct Synthesis of Methane and Methanol Using CO2 from Industrial Gas Mixtures
(2021)
For a complete transition from fossil to CO₂ neutral energy supply new energy storage concepts are needed that allow energy supply in times of absence of regenerative power production as during dark doldrums. A promising renewable energy storage approach is the power to gas (to power) technique based on the production of synthetic natural gas (also called e-methane) by methanation of CO₂ with H₂. The latter is usually produced by electrolysis. In any power to gas concept, electrolysis is a very critical part, due to its high costs, stability issues, or limited power of required electrolysers.
As an alternative source of hydrogen, we investigate the methanation of coke oven gas (COG). COG is a byproduct of the carbon rich coke production from coal for the steel industry, with a high amount of hydrogen (~60vol%). Coke oven gas furthermore contains CH₄(~25vol%), CO (5-8vol%), and CO₂(1-3vol%), making it an attractive feedstock for the production of synthetic energy carriers like methane. In the present study, the authors investigate the direct conversion of CO and CO₂ from COG into e-methane. Compared to stoichiometric conversion, the COG hydrogen content is too high for catalytic methanation of CO₂. In order to achieve a higher methane yield, the addition of CO₂ from air, flue gas, or coal gasification can compensate the surplus of hydrogen in the coke oven gas. The process is evaluated by the conversion of CO and CO₂, the catalyst selectivity towards higher hydrocarbons for varying temperatures, and the CH₄ yield.
The combustion of fossil fuels results in CO2 emission, which is one of the primary causes of global warming. An important approach for solving this problem is the fixation, the chemical utilization and the recycling of CO2. Therefore, we investigate the catalytic conversion of CO2 with H2 into methane (CH4) with an upscaled test station at a brown coal power plant. In a completely new strategy, we realize the direct conversion of the CO2 content of the flue gas, without a cleaning process like amine scrubbing or optimized combustion like oxyfuel. Our experiments are performed in matters of catalytic performance, heat production and stability of the catalytic Sabatier process, as a function of the gas flow rate. The catalytic performance is investigated with a simulated composition of flue gas and under real conditions directly at the power plant. The CH4 production by the Sabatier process is realized with a maximum input flow rate of near 50Nm3/h, with 30Nm3/h flue gas and 20Nm3/h hydrogen. For these values, the necessary power scale for hydrogen generation by electrolysis is around 100kW. With synthetic and real flue gas, a conversion up to 99% (for hydrogen surplus) with 100% selectivity is stabilized. The reaction operates in thermal steady state equilibrium without any external energy supply. In consequence, the process of CO2 recycling could be integrated directly as a post combustion process of conventional power plants, without an expensive capturing step, for example.
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.
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%.
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.
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.
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.