采用溶胶一凝胶法结合等体积浸渍法制备了一系列不同Mo负载量的K—Co-Mo/CNTs催化剂.通过X射线衍射、N2等温吸脱附,透射电子显微镜和H2-TPD表征了催化剂结构,并研究了碳纳米管催化剂使用合成气合成低碳醇的催化性能.所制备的催化剂颗粒在CNTs载体的外表面和内表面上具有低结晶度和高分散性.CNTs载体的均匀介孔结构增加了反应物和产物的扩散速率,从而促进了反应转化.此外,CNTs载体的引入促进了氢的吸附和活化,而且和解离H物种的相互作用较弱,易于H的溢流,并促进了烷基的形成,烷基是形成醇产物和碳链增长的重要中间体.受益于这些特征,与传统的活性炭催化剂相比,CNTs负载的K—Co—Mo催化剂显示出更加优异的合成醇性能.
A series of carbon nanotubes-supported K-Co-Mo catalysts were prepared by a sol-gel method combined with incipient wetness impregnation. The catalyst structures were characterized by X-ray diffraction, N2 adsorption-desorption, transmission electron microscopy and H2-TPD, and its catalytic performance toward the synthesis of higher alcohols from syngas was investigated. The as-prepared catalyst particles had a low crystallization degree and high dispersion on the outer and inner surface of CNTs. The uniform mesoporous structure of CNTs increased the diffusion rate of reactants and products, thus promoting the reaction conversion. Furthermore, the incorporation of CNTs support led to a high capability of hydrogen absorption and spillover and promoted the formation of alkyl group, which served as the key intermediate for the alcohol formation and carbon chain growth. Benefiting from these characteristics, the CNTs supported Mo-based catalyst showed the excellent catalytic performance for the higher alcohols synthesis as compared to the unsupported catalyst and activated carbon supported catalyst.