The Role of Pore Architect, Reducibility and Silica-Alumina Ratio over Ni-Containing Molecular Sieves for Methane Partial Oxidation
摘要
The catalytic conversion of CH4 by O2 into syngas (known as partial oxidation of methane; POM) is a practical approach for depleting CH4 concentration as well as achieving excellent H2 yield with high H2/CO ratio. The pentasil zeolite family having different SiO2/Al2O3 ratios 10, 20, 25, and 30 (abbreviated as CBV10A, CBV20A, CP810E, and CBV3024E) is found to be an excellent carrier for Ni. These Ni-containing molecular sieves are investigated for POM and characterized by X-ray diffraction, Raman-infrared spectroscopy, thermogravimetry, temperature-programmed techniques, and transmission electron microscopy. 5Ni/CBV3024E catalyst has smaller number of active sites, 5Ni/CP810E contains unstable active site and mordenite-based Ni catalysts (5Ni/CBV10A and 5Ni/CBV20A) attain higher metal-support interaction. 5Ni/CBV20A outperforms others due to the presence of reducible NiO under moderate and strong interaction. It shows an initial 40% H2 yield at 600 oC and 81% H2 yield at 750 oC. The high-temperature POM reaction limits the H2/CO ratio close to the stoichiometric value of POM (~ 2), indicating the direct pathways of POM reaction at high temperatures. The high POM activity with the option of a wide range of H2/CO (4.12–2.26) using Ni-containing molecular sieve may gain industrial-level attention in the coming future.
Graphical abstract