Facile immobilization of Ni nanoparticles into mesoporous MCM-41 channels for efficient methane dry reforming

ABSTRACT Development of dry reforming of methane and carbon dioxide is an effective route to convert in-dustrial waste gases such as coke-oven gas and coal-to-oil gas into platform syngas. However, this process encounters severe problems of metal particle sintering and coke formation at high tem-peratures. In this work, we developed a new synthetic method for preparing confined Ni/MCM-41 catalysts, which impede the sintering of metal nanoparticles (NPs) and coke deposition at high temperatures, enabling them to be successfully applied to methane dry reforming . The method results in high activity and stability of the catalyst at 700 °C for 200 h. The Ni precursor is immersed in ethanol and impregnated into MCM-41 by the peculiar capillary action of hexagonal straight mesopores . By this method, 10 wt% Ni NPs (d = 2 nm) is equably confined to the mesoporous channels with strong metal-support interactions, as confirmed by HRTEM, TEM mapping, H2-TPR, and XRD measurements. Such a confined structure has a significant effect on the inhibition of metal NP agglomeration and carbon deposition during methane dry reforming, as evidenced by TEM, Raman, TGA, and TPO measurements of used Ni/MCM-41 catalysts. In contrast, unconfined Ni/MCM-41 catalysts, with Ni NPs located on the pore exteriors, are rapidly deactivated after 12 h due to the blocked contact between the active metal centers and the gas feedstock. Additionally, a fast increase in the Ni NP size and the formation of substantial carbon nanotubes on the unconfined catalyst surface are seen. This work offers a facile approach for the synthesis of anti-sintering, car-bon-resistant confined Ni catalysts that can operate at high temperatures