摘要
费托合成提供了由非石油路线获取高附加值基础化学品的有效途径,随着后石油时代的临近,其重要性及战略意义日显突出。其中,费托合成制低碳烯烃(C_2~=-C_4~=)具有重要的应用价值,但目前仍面临着催化剂选择性低、稳定性差等问题。我们以氮掺杂碳纳米管(NCNTs)为载体,通过浸渍法构建了Fe/NCNTs催化剂,利用氮的锚定作用可方便地实现Fe纳米粒子的均匀负载,无需对载体做任何表面预处理。对比研究发现,NCNTs负载的催化剂在低碳烯的选择性、催化活性和稳定性方面均优于碳纳米管(CNTs)和活性炭(AC)负载的催化剂,其原因是N掺杂位有效促进了Fe物种的分散,且有利于其还原和碳化,从而有效提高了催化剂的活性和稳定性。
Iron-based Fischer-Tropsch synthesis(FTS) catalyst for lower olefins with high selectivity and stability is of great importance in post-petroleum era. By means of the anchoring effect and the intrinsic basicity of nitrogen-doped carbon nanotubes(NCNTs), iron nanoparticles were conveniently immobilized on NCNTs without surface pre-modification. The so-constructed Fe/NCNTs catalyst presents superb catalytic performance in FTS with high selectivity for lower olefins as well as high activity and stability. The excellent performance is well-correlated with enhanced dissociative CO adsorption, inhibition of secondary hydrogenation of lower olefins, and promoted formation of the active phase of χ-Fe_5C_2. All of these merits result from participation of the nitrogen. These results may lead to a new strategy for exploring advanced FTS catalysts with abundant N-doped carbon nanostructures.
引文
1.Lu J,Yang L,Xu B,Wu Q,Zhang D,Yuan S,Zhai Y,Wang X,Fan Y,Hu Z.ACS Catal.,2014,4(2):613-621.
2.Lu J,Hu R,Zhuo O,Xu B,Yang L,Wu Q,Wang X,Fan Y,Hu Z.Acta Chim.Sinica,2014,72,1017-1022.