Ni@SBA-15 monoliths with up to 5 wt.% of Ni were successfully synthetized by means of an original and easy one-pot sol-gel method. Transmission Electron Microscopy (TEM), X-ray Photoelectron Spectroscopy (XPS), Temperature-Programmed Reduction (TPR), Pair Distribution Function (PDF) and X-Ray Diffraction (XRD) were used for the structural characterization of the samples. After H2-reduction, those solids exhibited small Ni 0 particles (between 1-3 nm) highly dispersed (one of the highest dispersion reported in the literature to date for 5 wt.% Ni/Silica materials) in strong interaction with the silica support. Scanning Transmission Electron Microscopy in the High Angle Annular Dark Field (STEM/HAADF) mode, chemical mapping by Energy Dispersive X-Ray (EDX) spectroscopy and electron tomography in STEM-HAADF mode highlighted the presence of Ni particles homogeneously distributed, especially in the mesopores. Such confined Ni nanoparticles were shown to be very selective and stable in the dry reforming of methane.
Supported nickel nanoparticles are promising catalysts for the methanation of CO2. The role of nickel particle size on activity and selectivity in this reaction is a matter of debate. We present a study of metal particle size effects on catalytic stability, activity and selectivity, using nickel on graphitic carbon catalysts. Increasing the Ni particle size from 4 to 8 nm led to a higher catalytic activity, both per gram of nickel and normalized surface area. However, the apparent activation energy remained the same (∼105 kJ mol−1). Comparing experiments at atmospheric to 30 bar pressure demonstrates the importance of testing under industrially relevant pressures; the highest selectivity is obtained at high CO2 conversions and pressures. Finally, the selectivity was particle size‐dependent. The largest particles were not only most active but also most selective to methane. With this work we contribute to the ongoing debate about Ni particle size effects in CO2 methanation.
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