Nickel and potassium co-modified β-Mo2C catalysts were prepared and used for CO hydrogenation reaction. The major products over β-Mo2C were C1-C4 hydrocarbons, only few alcohols were obtained. Addition of potassium ...Nickel and potassium co-modified β-Mo2C catalysts were prepared and used for CO hydrogenation reaction. The major products over β-Mo2C were C1-C4 hydrocarbons, only few alcohols were obtained. Addition of potassium resulted in remarkable selectivity shift from hydrocarbons to alcohols at the expense of CO conversion over β-Mo2C. Moreover, it was found that potassium enhanced the ability of chain propagation with a higher C2+OH production. Modified by nickel,β-Mo2C showed a relatively high CO conversion, however, the products were similar to those of pure β-Mo2C. When co-modified by nickel and potassium,β-Mo2C exhibited high activity and selectivity towards mixed alcohols synthesis, and also the whole chain propagation to produce alcohols especially for the stage of C1 OH to C2OH was remarkably enhanced. It was concluded that the Ni and K had, to some extent, synergistic effect on CO conversion.展开更多
The X-ray photoelectron spectroscopy (XPS) was used to investigate the surface characteristic of potassium-promoted or un-promoted both β-Mo2C and α-MoC1-x pretreated by syngas at different temperatures,and the pr...The X-ray photoelectron spectroscopy (XPS) was used to investigate the surface characteristic of potassium-promoted or un-promoted both β-Mo2C and α-MoC1-x pretreated by syngas at different temperatures,and the promotional effect of potassium on the catalytic performance was also studied.XPS results revealed that the content of surface Mo and its valence distribution between β-Mo2C and α-MoC1-x were quite different.Promoted by potassium,the remarkable changes were observed for surface composition and valence of Mo distribution over β-Mo2C.Potassium had strong electronic effect on β-Mo2C,which led to a higher Mo4+ content.On the contrary,potassium had little electronic effect on α-MoC1-x,and K-Mo interaction was weak.Therefore,Mo0 and Mo2+ became the dominant species on the catalyst surface,and the Mo4+ content showed almost no increase as the pretreatment temperature enhanced.In terms of catalytic performance of molybdenum carbides,the increase in Mo0 most likely explained the increase in hydrocarbon selectivity,yet Mo4+ might be responsible for the alcohols synthesis.展开更多
Fe modified and un-modified K/Mo2C were prepared and investigated as catalysts for CO hydrogenation reaction. Compared with K/Mo2C catalyst, the addition of Fe increased the production of alcohols, especially the C2+...Fe modified and un-modified K/Mo2C were prepared and investigated as catalysts for CO hydrogenation reaction. Compared with K/Mo2C catalyst, the addition of Fe increased the production of alcohols, especially the C2+OH. Meanwhile, considerable amounts of C5+ hydrocar- bons and C2= -C4= were formed, whereas methane selectivity greatly decreased. Also, the activity and selectivity of the catalyst were readily affected by the reaction pressure and temperature employed. According to the XPS results, Mo4+ might be responsible for the production of alcohols, whereas the low valence state of Mo species such as Mo^0 and/or Mo^2+ might be account for the high activity and selectivity toward hydrocarbons.展开更多
基金supported by the National Key Project for Basic Research of China (973 Project) (No. 2005CB221400)
文摘Nickel and potassium co-modified β-Mo2C catalysts were prepared and used for CO hydrogenation reaction. The major products over β-Mo2C were C1-C4 hydrocarbons, only few alcohols were obtained. Addition of potassium resulted in remarkable selectivity shift from hydrocarbons to alcohols at the expense of CO conversion over β-Mo2C. Moreover, it was found that potassium enhanced the ability of chain propagation with a higher C2+OH production. Modified by nickel,β-Mo2C showed a relatively high CO conversion, however, the products were similar to those of pure β-Mo2C. When co-modified by nickel and potassium,β-Mo2C exhibited high activity and selectivity towards mixed alcohols synthesis, and also the whole chain propagation to produce alcohols especially for the stage of C1 OH to C2OH was remarkably enhanced. It was concluded that the Ni and K had, to some extent, synergistic effect on CO conversion.
文摘The X-ray photoelectron spectroscopy (XPS) was used to investigate the surface characteristic of potassium-promoted or un-promoted both β-Mo2C and α-MoC1-x pretreated by syngas at different temperatures,and the promotional effect of potassium on the catalytic performance was also studied.XPS results revealed that the content of surface Mo and its valence distribution between β-Mo2C and α-MoC1-x were quite different.Promoted by potassium,the remarkable changes were observed for surface composition and valence of Mo distribution over β-Mo2C.Potassium had strong electronic effect on β-Mo2C,which led to a higher Mo4+ content.On the contrary,potassium had little electronic effect on α-MoC1-x,and K-Mo interaction was weak.Therefore,Mo0 and Mo2+ became the dominant species on the catalyst surface,and the Mo4+ content showed almost no increase as the pretreatment temperature enhanced.In terms of catalytic performance of molybdenum carbides,the increase in Mo0 most likely explained the increase in hydrocarbon selectivity,yet Mo4+ might be responsible for the alcohols synthesis.
基金supported by the Key Project of Chinese National Programs for Fundamental Research and Development(973 Program-2005CB221400)
文摘Fe modified and un-modified K/Mo2C were prepared and investigated as catalysts for CO hydrogenation reaction. Compared with K/Mo2C catalyst, the addition of Fe increased the production of alcohols, especially the C2+OH. Meanwhile, considerable amounts of C5+ hydrocar- bons and C2= -C4= were formed, whereas methane selectivity greatly decreased. Also, the activity and selectivity of the catalyst were readily affected by the reaction pressure and temperature employed. According to the XPS results, Mo4+ might be responsible for the production of alcohols, whereas the low valence state of Mo species such as Mo^0 and/or Mo^2+ might be account for the high activity and selectivity toward hydrocarbons.