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Activated-carbon-supported K-Co-Mo catalysts for synthesis of higher alcohols from syngas

机译:激活的碳支持的K-CO-MO催化剂,用于合成Syngas的较高醇

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A series of activated-carbon-supported K-Co-Mo catalysts (K-Co-Mo/AC) were prepared by using a solgel method combined with incipient wetness impregnation. The catalyst structure was characterized by X-ray diffraction (XRD), N-2 adsorption-desorption, X-ray absorption fine structure spectroscopy and X-ray photoelectron spectroscopy, and their catalytic performance toward synthesis of higher alcohols from syngas was investigated. The large surface area and pore volume of the support facilitated the distribution of metal particles and high dispersion of metals. At low Mo loading, the Mo atoms on the activated carbon surface were mainly tetrahedrally coordinated Mo6+ species. With an increase in the Mo loading, the coordination environment of the surface Mo atoms gradually transformed from tetrahedrally coordinated Mo6+ to octahedrally coordinated Mo4+, indicating that an increase in the Mo loading promoted the reduction of Mo6+ species to Mo4+ species. After reduction, it was observed that a type of a lower state Mo delta+ (1 < delta < 4) species was present on the surface, which is suggested to be responsible for alcohol synthesis. Compared to the unsupported catalyst, K-Co-Mo/AC exhibited a significantly higher activity for alcohol formation. In particular, the C2+ alcohol content increased significantly. This can be attributed to the fact that the supported catalysts have a high active surface area, and the mesoporous structure is suggested to prolong the residence time of intermediates to form alcohols in the pores to some extent, thus promoting the formation of higher alcohols. Under the conditions of a Mo/AC weight ratio of 40% and a reduction temperature of 798 K, the K-Co-Mo/AC catalyst exhibited the highest activity for alcohol formation, which may be attributed to the high content of Mo delta+ (1 < delta < 4) species on the surface.
机译:通过使用溶胶液和初期湿度浸渍的溶胶方法制备了一系列活化的碳支持的K-CO-MO催化剂(K-CO-MO/AC)。催化剂结构的特征是X射线衍射(XRD),N-2吸附 - 解吸收,X射线吸收良好的结构光谱和X射线光电子光谱,并研究了其促进Syngas中较高酒精的催化性能。支撑的较大表面积和孔体积促进了金属颗粒的分布和金属的高分布。在低MO负载下,活化碳表面上的MO原子主要是四面体配位的MO6+物种。随着MO载荷的增加,表面MO原子的配位环境逐渐从四面体配位的MO6+转变为八面体配位的MO4+,表明MO载荷的增加促进了MO6+物种的减少到MO4+物种。还原后,观察到表面上存在一种较低状态的mo delta+(1

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