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镁掺杂的镍 - 铜/钴改性稻壳衍生介孔二氧化硅上的一氧化碳甲烷化反应

CO methanation on Mg-doped Ni-Cu/Co modified mesoporous SiO derived from rice husks.

作者信息

Popova Margarita, Dimitrov Momtchil, Oykova Manuela, Shestakova Pavletta, Kovacheva Daniela, Atanasova Genoveva, Szegedi Ágnes

机构信息

Institute of Organic Chemistry With Centre of Phytochemistry, Bulgarian Academy of Sciences, 1113, Sofia, Bulgaria.

Institute of General and Inorganic Chemistry, Bulgarian Academy of Sciences, 1113, Sofia, Bulgaria.

出版信息

Environ Sci Pollut Res Int. 2025 Feb 10. doi: 10.1007/s11356-025-35931-5.

Abstract

Mesoporous silica (SiO) was prepared using a simple procedure from rice husks without the application of a template. Incipient wetness impregnation method was employed to prepare magnesium-doped nickel-copper- and nickel-cobalt-containing SiO catalysts. The obtained materials were characterized by X-ray powder diffraction (XRD), N physisorption, transmission electron microscopy (TEM), temperature-programmed reduction (TPR-TGA), and NMR and XPS spectroscopies. The study demonstrated the significant influence of Ni and Co/Cu content, as well as the sequence of Mg promotion (before or after the nickel-copper- and nickel-cobalt-modification) on the physico-chemical properties of the catalysts. The peculiar properties of the mesoporous carrier positively influenced the formation of finely dispersed nickel and/or copper/cobalt oxide species, which were readily reducible at temperatures below 600 °C. XPS analysis revealed that the surface of Mg-doped Ni-Co supported SiO catalysts was rich in nickel. All the prepared catalysts were active in CO hydrogenation to methane. The Mg-doped Ni-Co supported SiO catalysts showed higher catalytic activity compared to their Mg-doped Ni-Cu counterparts. The 1.5Mg10Ni5Co/SiO catalyst demonstrated 82% CO conversion and 99.5% selectivity to methane. The activity and selectivity of this catalyst was maintained at 400 °C for a reaction time of 4 h.

摘要

介孔二氧化硅(SiO)采用简单的方法由稻壳制备而成,无需使用模板。采用初湿浸渍法制备了镁掺杂的含镍 - 铜和含镍 - 钴的SiO催化剂。通过X射线粉末衍射(XRD)、N物理吸附、透射电子显微镜(TEM)、程序升温还原(TPR - TGA)以及NMR和XPS光谱对所得材料进行了表征。研究表明,镍和钴/铜含量以及镁促进顺序(在镍 - 铜和镍 - 钴改性之前或之后)对催化剂的物理化学性质有显著影响。介孔载体的特殊性质对细分散的镍和/或铜/钴氧化物物种的形成产生了积极影响,这些物种在低于600℃的温度下易于还原。XPS分析表明,镁掺杂的Ni - Co负载的SiO催化剂表面富含镍。所有制备的催化剂在CO加氢制甲烷反应中均具有活性。镁掺杂的Ni - Co负载的SiO催化剂比其镁掺杂的Ni - Cu对应物表现出更高的催化活性。1.5Mg10Ni5Co/SiO催化剂表现出82%的CO转化率和99.5%的甲烷选择性。该催化剂在400℃下反应4小时,活性和选择性得以保持。

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