In this study, we investigate the effect of thermal treatment/calcination on the stability and activity of a Na-Mn-W/SiO2 catalyst for the oxidative coupling of methane reaction. The catalyst performance and...
A La−Sr/CaO catalyst was studied operando during the oxidative coupling of methane (OCM) reaction using the X-ray diffraction computed tomography technique. Full-pattern Rietveld analysis was performed in order to track the evolving solid-state chemistry during the temperature ramp, OCM reaction, as well as after cooling to room temperature. We observed a uniform distribution of the catalyst main components: La 2 O 3 , CaO−SrO mixed oxide, and the hightemperature rhombohedral polymorph of SrCO 3 . These were stable initially in the reaction; however, doubling the gas hourly space velocity resulted in the decomposition of SrCO 3 to SrO, which subsequently led to the formation of a second CaO−SrO mixed oxide. These two mixed CaO−SrO oxides differed in terms of the extent of Sr incorporation into their unit cell. By applying Vegard's law during the Rietveld refinement, it was possible to create maps showing the spatial variation of Sr occupancy in the mixed CaO−SrO oxides. The formation of the Srdoped CaO species is expected to have an important role in this system through the enhancement of the lattice oxygen diffusion as well as increased catalyst basicity.
A flexible combined heat, power and fuel production concept, FlexCHX, is being developed for managing the seasonal mismatch between solar energy supply and the demand for heat and power characteristic of Northern and Central Europe. The process produces an intermediate energy carrier (Fischer-Tropsch hydrocarbon product), which can be refined to transportation fuels using existing refineries. The FlexCHX process can be integrated into various combined heat and power production systems, both industrial CHPs and communal district heating units. In the summer season, renewable fuels are produced from biomass and hydrogen; the hydrogen is produced from water via electrolysis that is driven by low-cost excess electricity from the grid. In the dark winter season, the plant is operated only with biomass in order to maximize the production of the much-needed heat, electricity and FT hydrocarbons. Most of the invested plant components are in full use throughout the year with only the electrolysis unit being operated seasonally. The catalytic reformer plays a key role in this process by converting tars and light hydrocarbon gases into synthesis gas and by bringing the main gas constituents towards equilibrium. Developmental precious metal catalysts were used, and an optimal reformer concept was established and tested at pilot scale. Reforming results obtained at pilot gasification tests with commercial nickel catalysts and with the developed precious metal catalysts are presented.
This work presents multi-scale approaches to investigate 3D printed structured Mn–Na–W/SiO2 catalysts used for the oxidative coupling of methane (OCM) reaction. The performance of the 3D printed catalysts has been compared to their conventional analogues, packed beds of pellets and powder. The physicochemical properties of the 3D printed catalysts were investigated using scanning electron microscopy, nitrogen adsorption and X-ray diffraction (XRD). Performance and durability tests of the 3D printed catalysts were conducted in the laboratory and in a miniplant under real reaction conditions. In addition, synchrotron-based X-ray diffraction computed tomography technique (XRD-CT) was employed to obtain cross sectional maps at three different positions selected within the 3D printed catalyst body during the OCM reaction. The maps revealed the evolution of catalyst active phases and silica support on spatial and temporal scales within the interiors of the 3D printed catalyst under operating conditions. These results were accompanied with SEM-EDS analysis that indicated a homogeneous distribution of the active catalyst particles across the silica support.
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