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Power‐to‐methane (PtM) offers an efficient opportunity for surplus renewable energy storage, but heat management is a major challenge for conducting the highly exothermic methanation reaction. To address this challenge, this study presents the first successful demonstration of core‐shell catalyst pellets in a pilot‐scale reactor for CO2 methanation. Experiments in a wall‐cooled fixed‐bed reactor are conducted with diluted and undiluted reactant feed under systematic variation of cooling temperature and inlet gas flow rate. The results show that core‐shell catalyst pellets significantly reduce the hot‐spot temperature while maintaining comparable reactant conversions to uncoated catalyst pellets at the same conditions. Additionally, core‐shell catalyst pellets allow for undiluted reactant feed at comparably low hot‐spot temperatures (approx. 600 °C). [ABSTRACT FROM AUTHOR]

Cylindrical, cm‐sized monolithic Al2O3 xerogels with hierarchical meso‐/macropore system were prepared by sol‐gel synthesis. The influence of both solvent exchange and drying on monolith stability and the resulting pore system was studied following mass and volume of the monolith as well as by porosimetry and electron microscopy. Crack‐free drying of the monoliths requires a proper management of drying stress. This is achieved by adjusting the drying rate and solvent exchange procedure applied to the intermediate lyogels. Moreover, mainly through differences in capillary pressure, changing the pore fluid allows an adjustment of the mesopore width from 7.6 nm to 10.5 nm. Neither solvent exchange nor drying affect the macropores, the width of which stays at 1.5 μm. Finally, CO2 methanation over Ni‐impregnated Al2O3 monoliths reveals CO2 conversion and CH4 selectivity comparable to an industrial Ni/Al2O3 benchmark catalyst. [ABSTRACT FROM AUTHOR]

There is considerable motivation in the catalysis community and chemical industry to envision a future where rational catalyst design and targeted chemical process optimization become standard. Achieving this goal for heterogeneous catalysis requires a cultural shift centered around effective research data management. The core elements of modern catalysis research are synthesis, characterization, and testing, while all can be elevated by effective collection, correlation, interoperation, and exploitation of data between disciplines and stakeholders. Here, first steps are made towards a holistic picture of an industrial Ni/Al2O3 reference catalyst for CO2 methanation. A range of conventional and advanced characterization tools are applied to probe metal particle size and pore characteristics of the support, selected as crucial parameters for catalyst performance. Challenges are shown with respect to current reporting of characterization data and metadata, which ultimately influences the development and reliability of digital twins in catalysis research. Furthermore, the cooperation and combined expertise of diverse research groups from different fields is recognized as essential to deliver meaningful progress towards the digital future of catalysis research. [ABSTRACT FROM AUTHOR]

CO2 methanation is often performed on Ni/Al2O3 catalysts, which can suffer from mass transport limitations and, therefore, decreased efficiency. Here we show the application of a hierarchically porous Ni/Al2O3 catalyst for methanation of CO2. The material has a well-defined and connected meso- and macropore structure with a total porosity of 78%. The pore structure was thoroughly studied with conventional methods, i.e., N2 sorption, Hg porosimetry, and He pycnometry, and advanced imaging techniques, i.e., electron tomography and ptychographic X-ray computed tomography. Tomography can quantify the pore system in a manner that is not possible using conventional porosimetry. Macrokinetic simulations were performed based on the measures obtained by porosity analysis. These show the potential benefit of enhanced mass-transfer properties of the hierarchical pore system compared to a pure mesoporous catalyst at industrially relevant conditions. Besides the investigation of the pore system, the catalyst was studied by Rietveld refinement, diffuse reflectance ultraviolet-visible (DRUV/vis) spectroscopy, and H2-temperature programmed reduction (TPR), showing a high reduction temperature required for activation due to structural incorporation of Ni into the transition alumina. The reduced hierarchically porous Ni/Al2O3 catalyst is highly active in CO2 methanation, showing comparable conversion and selectivity for CH4 to an industrial reference catalyst. [ABSTRACT FROM AUTHOR]

Cylindrical, cm‐sized monolithic Al2O3 xerogels with hierarchical meso‐/macropore system were prepared by sol‐gel synthesis. The influence of both solvent exchange and drying on monolith stability and the resulting pore system was studied following mass and volume of the monolith as well as by porosimetry and electron microscopy. Crack‐free drying of the monoliths requires a proper management of drying stress. This is achieved by adjusting the drying rate and solvent exchange procedure applied to the intermediate lyogels. Moreover, mainly through differences in capillary pressure, changing the pore fluid allows an adjustment of the mesopore width from 7.6 nm to 10.5 nm. Neither solvent exchange nor drying affect the macropores, the width of which stays at 1.5 μm. Finally, CO2 methanation over Ni‐impregnated Al2O3 monoliths reveals CO2 conversion and CH4 selectivity comparable to an industrial Ni/Al2O3 benchmark catalyst. [ABSTRACT FROM AUTHOR]