The Effect of Selected Metal Oxides Over Ni Supported on SiO2+ZrO2 Catalysts Towards Dry Reforming of Methane
摘要
The work systematically investigated the promotional effects of La2O3, CeO2, and WO3 on 5 wt.% Ni supported over SiO2+ZrO2 mixed oxide (10SiZr) catalysts for the dry reforming of methane (DRM) reaction. The synthesized catalysts of physicochemical properties were comprehensively characterized using several techniques to elucidate structure–activity relationships. The addition of promoters is found to enhance covalency in oxygen of M-O-M′ bonding in metal oxide matrix, to improve the reducibility and to enhance the basicity of moderate and strong strength. The ceria promoter reduces the crystallinity of catalyst to a minimum inducing high dispersion of the metal oxide’s matrix of support and oxidizing coke effectively over a long time on stream. The 5Ni+1Ce–10SiZr catalyst achieved 75% CH4 conversion and 81% CO2 conversion with an H2/CO ratio of 0.86, maintaining stable catalytic activity over 20 h time-on-stream. As expected for the endothermic DRM reaction, conversions increased with reaction temperature. The Ce-promoted catalyst had minimum 48.82 kJ/mol apparent activation energy for CH4 conversion, indicating favourable reaction kinetics. The less availability of active sites over highly crystalline 5Ni+1La-10SiZr catalyst turns into least catalytic activity among rest catalysts. The WO3-promoted catalyst exhibited high crystallinity, deposit of thermally stable carbonates and lower activity than the Ce-promoted catalyst. 1 wt.% ceria promotion effectively optimizes the structural and surface properties of the 5 wt.%Ni–10SiZr catalyst, enhancing DRM activity and stability through improved metal dispersion, balanced basicity, and strengthened metal–support interactions.
Graphical Abstract