担载型过渡金属催化剂上甲烷和乙烯的同系化反应

STUDIES OF HOMOLOGATION OF ETHYLENE WITH METHANE ON SUPPORTED TRANSITION METAL CATALYSTS

利用程序升温脉冲反应技术较系统地考察了担载型过渡金属催化剂上甲烷与乙烯同系聚合制丙烯和丙烷的反应．通过分步反应，即首先进行甲烷分解，然后引入乙烯与甲烷分解产生的表面碳物种反应，可以克服甲烷与乙烯同系聚合反应的动力学限制，使该反应能在较为温和的条件下进行．还系统地探讨了影响该反应的各种因素．结果表明，Ｐｔ，Ｃｏ．催化剂表现出较为优越的催化性能．

he homologation of ethylene with methane on supported transition metal catalysts was investigated by using transient response characterization (TRC), temperature programmed pulse reaction (TPPR) and constant temperature pulse reaction (CTPR) of probe molecule CH3I. The different factors which greatly affect the reaction were also studied. A tentative approachwas to split the overall reaction into two steps occurring under moderate conditions. At first, methane decomposed to form carbonaceous species on thesurface of the transition metals, then ethylene was introduced to homologatewith the surface carbonaceous species. In such a two-step route, the kineticlimitation can be overcome and the homologation of ethylene with methanemay be practically achieved, Platinum and cobalt catalysts favor the homologation of ethylene with methane.