Gallium-promoted Ni/SiO2-ZrO2 catalysts for hydrogen-rich syngas production via methane partial oxidation
摘要
The partial oxidation of methane into syngas may protect the environment by consuming potential greenhouse gas, CH4, and yield hydrogen-rich synthetic feedstock to industries. Herein, in the target of developing POM catalyst, silica-zirconia (SZ) is used as support, 5 wt.% Ni as an active metal site and 0.25–1 wt.% Ga as a promoter. Catalysts are characterized by X-ray diffraction study, surface area-porosity, Raman spectroscopy, thermogravimetry, and temperature-programmed reduction–oxidation-reduction cyclic experiments. The Ga-promoted Ni-based catalysts attain a higher concentration of “strongly interacted reducible NiO” than “weakly interacted reducible NiO” in the presence of oxygen and hydrogen. 0.25 wt.% Ga-promoted 5Ni/SZ attains the initial highest concentration of “strongly interacted reducible NiO,” its concentration remains higher even against the molecular oxygen. 5Ni0.25 Ga/SZ catalyzes 51% CH4 to yield 50% H2 (H2/CO = 2.5) through POM, whereas a 35% CO2 yield is also noticed through parallel participation of the TOM reaction. 675 °C reaction temperature, 8000 ccg⁻1 h⁻1 gas hourly space velocity, and 1.50 CH4/O2 ratio are set over 5Ni0.25 Ga/YZ by statistically predicted models like response surface methodology under center composite design. Under these predicted conditions, 83% CH4 conversion, 81% H2 yield, and 2.5 H2/CO ratio are constantly obtained up to 30 h on stream. Such a high catalytic activity on optimized reaction conditions makes 5Ni0.25 Ga/YZ a highly potent catalyst in achieving the hydrogen energy goal at the expense of CH4 depletion.
Graphical Abstract