In Situ Investigation of Methane Dry Reforming on Metal/Ceria(111) Surfaces: Metal–Support Interactions and C−H Bond Activation at Low Temperature
Zongyuan LiuPablo G. LustembergRamón A. GutiérrezJohn J. CareyRobert M. PalominoMykhailo VorokhtaDavid C. GrinterPedro J. RamírezVladimı́r MatolínMichael NolanM. V. Ganduglia-PirovanoSanjaya D. SenanayakeJosé A. Rodríguez
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Abstract Studies with a series of metal/ceria(111) (metal=Co, Ni, Cu; ceria=CeO 2 ) surfaces indicate that metal–oxide interactions can play a very important role for the activation of methane and its reforming with CO 2 at relatively low temperatures (600–700 K). Among the systems examined, Co/CeO 2 (111) exhibits the best performance and Cu/CeO 2 (111) has negligible activity. Experiments using ambient pressure X‐ray photoelectron spectroscopy indicate that methane dissociates on Co/CeO 2 (111) at temperatures as low as 300 K—generating CH x and CO x species on the catalyst surface. The results of density functional calculations show a reduction in the methane activation barrier from 1.07 eV on Co(0001) to 0.87 eV on Co 2+ /CeO 2 (111), and to only 0.05 eV on Co 0 /CeO 2− x (111). At 700 K, under methane dry reforming conditions, CO 2 dissociates on the oxide surface and a catalytic cycle is established without coke deposition. A significant part of the CH x formed on the Co 0 /CeO 2− x (111) catalyst recombines to yield ethane or ethylene.Keywords:
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Abstract The mitigation and utilization of greenhouse gases, such as carbon dioxide and methane, are among the most important challenges in the area of energy research. Dry reforming of CH 4 (DRM), which uses both CO 2 and CH 4 as reactants, is a potential method to utilize the greenhouse gases in the atmosphere. Natural gas containing high concentrations of CO 2 and CH 4 could therefore be utilized for hydrogen and synthesis gas (syngas) production in the near future, without need for the removal of CO 2 from the source gas. Thus, the DRM reaction is a suitable process to convert CH 4 and CO 2 to syngas, which is a raw material for liquid fuel production, through the Fischer–Tropsch process. Herein, the development of CO 2 reforming for syngas production is reviewed, covering process chemistry, catalyst development, and process technologies as well as the potential future direction for this process.
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Abstract The dry reforming of shale gas (methane and ethane with an average ratio of 4 : 1) with carbon dioxide (DRS) is considered to be a promising way to produce syngas, which widens the utilization of shale gas and mitigates carbon dioxide emission. In this paper, Ce modified Ni‐based catalysts were developed and the corresponding catalytic performances for DRS were investigated with a fixed bed reactor. Results showed that the catalyst containing 5 wt% of Ni and 5 wt% of Ce performed a best catalytic effect, including the selectivity of syngas and the carbon resistance performance, which is due to the good metal dispersion, strong interaction between Ni and Ce, and the formation of Ni‐CeO x solid solution. The electron transfer between Ni and Ce, substitution of Ni for Ce, and the sequential oxygen vacancies or defects, play significant roles in activating CH 4 , C 2 H 6 and CO 2 . The conversion of reactant gas increased with temperature, while the selectivity of syngas is little affected with temperature. In addition, the desired catalyst containing 5 wt% of Ni and 5 wt% of Ce showed good stability in the long‐time operation, which indicates that the Ce modified Ni‐based catalyst is a promising one for the dry reforming of shale gas.
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The propose CO2 reforming solution has improved CO2 conversion efficiency by developing a new double helix type plasma generator (DHTPG) to preheat the discharge gas and increase residence time of CO2 at DHTPG. In addition, injecting CH4 independently allows for a stable increase in the temperature of the CO2 plasma in the microwave plasma generator compared with other conventional methods. To verify the performance of the DHTPG, we experimentally investigated the distribution of the plasma gas temperature using an enthalpy probe system as a function of the specific energy input, which is a key parameter for understanding the mechanisms of CO2 reforming of CH4. We performed the CO2 reforming of CH4 using the newly designed plasma generator and a comparative analysis of its characteristics with those of other plasma generators. Without catalyst materials, our method significantly enhanced the CO2 conversion efficiency to 91.4% with an energy efficiency of 67% at a specific energy input of 245 kJ/mol. The main advantage of our method is an increase in energy-consumption selectivity, in which the energy injected through the plasma decomposes CO2 rather than CH4. In addition, it reduces the energy required to stably maintain the plasma to improve energy efficiency.
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