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Energies 2019, 12, 469 13 of 15 Considering the target value of 10 ppm CO (XCO = 99.8%) in the product gas of the methanation reactor for an inlet temperature of 120 ◦C, 5.1 kg catalyst are needed, 1.05% CO2 are simultaneously converted and the gas outlet temperature is 217 ◦C. Taking into consideration that the target value of 100 ppm CO in the product gas of the methanation reactor has to be achieved, this corresponds to 98% CO conversion and 1.85% H2 conversion. The further rise in temperature and H2 consumption is caused by the unwanted CO2 methanation. The excess of H2 conversion is here characterized by the factor EH2 = XH2 /0.0185, which is the ratio of the actual H2 conversion to the minimum conversion of 1.85%, if only CO methanation takes place and the residual CO content of 100 ppm needed for PtRu-anodes is just reached. Table 4 indicates that an inlet temperature of 130 ◦C is an appropriate value to avoid very high outlet temperatures (>240 ◦C). In this case, 2.6 kg of catalyst (52 g Ru) would be needed. The outlet temperature is then 221 ◦C, which is a reasonable value to limit the RWGS and CO2 methanation. EH2 would then be 1.2, i.e., 20% more hydrogen (H2 conversion of 2.22% compared to 1.85%) is consumed compared to the ideal case without CO2 conversion instead of here 0.7%. In order to be on the safe side, a certain surplus of the reactor size is advisable. Therefore, Table 4 also shows the reactor parameters, if the reactor length and mass of catalyst would be by a factor 1.5 or 2 larger compared to 100 ppm residual CO content. For a factor of 1.5 (mcat = 3.9 kg) and Tin = 130 ◦C, the resulting values are XCO =99.95%(residualCOcontentof3ppm),XCO2 =1.6%,andEH2 =1.45.Thefeedgasofthefuelcell would then consist of 77.2% H2, 9.8% CO2, 10.8% H2O, and 2.1% CH4. The reactor size is then 7.8 L, e.g., a cylinder with a length of 44 cm and diameter of 15 cm. An option is also an increase of the Ru content (here 2 wt-%), which would decrease the size and mass of the reactor further. 4. Conclusions The activity and selectivity of a 2 wt% Ru supported on γ-Al2O3 egg-shell catalyst for CO methanation in CO2/H2 rich gases was investigated. A kinetic model based on a Langmuir-Hinshelwood approach for both reactions was determined. The agreement with measurements in a fixed bed reactor is very satisfactory. CO2 methanation is slow compared to CO methanation, at least at temperatures below 200 ◦C. CO2 is directly converted to methane; the indirect route via RWGS and CO methanation could be excluded by respective measurements and kinetic considerations. Pore diffusion may affect the CO conversion at high temperatures (>200 ◦C). The kinetic equations were applied to model an adiabatic fixed bed methanation reactor suitable for a fuel cell for household appliances. The catalyst mass needed to reach a residual CO content of 100 ppm for feed gas with 0.5% CO, 10% CO2, 10% H2O, and 79.5% H2 is about 3 kg, which seems to a reasonable value. The H2 consumption is 20% higher compared to the ideal case without any conversion of CO2. Author Contributions: C.K. conceived the present idea and methodology and was involved in planning providing critical feedback. P.G. planned and carried out the experiments, the simulation and the validation of the experimental data and data curation. A.J. was the project administrator, supervised the project and was in charge of the overall direction, planning and data curation. C.K. acquired the project funding and P.G. the publication funding. A.J. and P.G. wrote, reviewed and edited the manuscript. Funding: This work was funded by the Bavarian State Ministry of Education, Science and the Arts within the framework of the TechnologieAllianzOberfranken (TAO). This publication was funded by the German Research Foundation (DFG) and the University of Bayreuth in the funding programme Open Access Publishing. Acknowledgments: The authors gratefully acknowledge the support of TechnolgieAllianzOberfranken and Center for Energy and Technology and thank the German Research Foundation (DFG) and the University of Bayreuth in the funding programme Open Access Publishing for funding this publication. Conflicts of Interest: The authors declare no conflict of interest.PDF Image | Selective Methanation of CO over a Ru-y-AI2O3 Catalyst in CO2 H2
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