纳米团簇
二氧化碳重整
催化作用
热重分析
化学
物理吸附
甲烷
合成气
吸附
催化剂载体
X射线光电子能谱
化学工程
无机化学
物理化学
有机化学
工程类
作者
Subhasis Das,Sharvani Thakur,Arijit Bag,Manveer Singh Gupta,Prasenjit Mondal,Ankur Bordoloi
标识
DOI:10.1016/j.jcat.2015.06.010
摘要
Surface-tuned mesoporous alumina has been prepared using a template-assisted solvo thermal method, and Ni nanoclusters (4–5 nm) have been synthesized on this support using a very facile organic matrix decomposition approach to dry reforming of methane. The catalyst system demonstrates very good catalytic activity toward CH4 and CO2 conversion (>90%), with a H2/CO ratio in syngas of almost unity, remarkable stability for more than 100 h, and is proven to be a very interesting catalyst system in dry reforming with methane. Both fresh and spent catalyst have been thoroughly characterized using different techniques such as N2 physisorption studies, X-ray diffraction, X-ray photoelectron spectroscopy, high-resolution transmission electron microscopy, temperature-programmed reduction, scanning electron microscopy, energy-dispersive X-ray spectroscopy, and thermogravimetric analysis to determine the structure–activity relationship. Characterization results show that Ni nanoclusters are highly dispersed on the surface of modified alumina. In addition, an excellent metal-support interaction evolves that clearly enhances the stability of the Ni clusters, providing better resistivity toward sintering. The presence of balanced acidic and basic sites in the surface-modified alumina drastically lowers coke formation and enhances the catalyst lifetime. The structures of adsorbed methane and carbon dioxide on the catalyst surface and the corresponding energy of adsorption have been computed using density functional theory calculations. It has been found that CO2 is adsorbed and dissociated into CO and O, while methane is adsorbed as CH3∗ and H∗ on the catalyst system.
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