一氧化碳加氢制碳氢化合物反应选择性的调控  

Selectivity tuning for the hydrogenation of carbon monoxide into hydrocarbons

作　　者：王野[1] 成康[1] 张庆红[1] 

机构地区：[1]厦门大学化学化工学院,厦门361005

出　　处：《中国科学：化学》2012年第4期363-375,共13页SCIENTIA SINICA Chimica

基　　金：国家自然科学基金(21173174,21033006,20923004);国家科技部973项目(2010CB732303)基金资助

摘　　要：合成气(即一氧化碳加氢)催化转化制碳氢化合物的费托合成反应是煤、甲烷和生物质等非油基碳资源间接转化制液体燃料或化学品的关键步骤.在传统的费托合成催化剂上,产物服从Anderson-Schulz-Flory分布,特定产物的选择性差.设计和制备高选择性费托合成催化剂,实现C–C偶联产物选择性的调控,是现代C1化学最具挑战性的课题.本文概述了近年来有关C–C偶联机理方面的理论研究进展,简要总结了影响费托合成产物选择性的几个关键因素,着重阐述了活性金属尺寸及所处微环境对产物选择性和催化活性的影响.本文还评述了既具有一氧化碳加氢制高碳烃又具有高碳烃加氢裂解能力的双功能费托合成催化剂体系,并提出通过控制加氢裂解等二次反应控制费托合成产物选择性的新策略.Fischer-Tropsch synthesis, i.e., the catalytic conversion of syngas （CO ＋ H2） into hydrocarbons, is a key step for the indirect transformation of non-petroleum carbon resources such as coal, methane, and biomass into liquid fuels and chemicals. The products follow the Anderson-Schulz-Flory distribution over cc,nventional Fischer-Tropsch catalysts, which is unselective for particular products. The design and preparation of highly selective Fischer-Tropsch catalysts and the realization of selectivity control for C-C coupling are the too：st challenging targets in the modem C1 chemistry. This review outlines recent advances in the theoretical studies on C-C coupling mechanism on the surfaces of typical Fischer-Tropsch catalysts, and briefly summarizes the key thctors affecting the product selectivity in Fischer-Tropsch synthesis with emphases on recent studies on the effects of the size and the microenvironment of active metal particles. This paper also highlights recent developments of bifunctional Fischer-Tropsch catalytic systems capable of catalyzing not only the hydrogenation of CO to heavy hydrocarbons but also the hydrocracking/ isomerization of heavy hydrocarbons. A new strategy for tuning the Fischer-Tropsch product selectivity by controlling the secondary reactions has been proposed.

关 键 词：费托合成碳氢化合物选择性调控碳纳米管介孔沸石分子筛 

分 类 号：TQ529.2[化学工程—煤化学工程]