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稀土—钴簇桥联配合物的合成与表征及F-T催化性能评价
Preparation and Fischer-Tropsch Performance of Bridging Complexes of Cobalt Cluster and Lanthanide
【作者】 王晶;
【导师】 苏海全;
【作者基本信息】 内蒙古大学 , 无机化学, 2009, 硕士
【摘要】 本文将不同核数的钴羰基簇合物和稀土(Yb、Sm、Eu)构造桥联配合物作为F-T合成催化剂前驱体的设计思路应用到F-T合成领域当中,以Co2(CO)8为原料,合成出带有羧基的四面体型钴羰基簇合物,并用此簇合物分别和稀土(Yb、Sm和Eu)的三氟乙酸盐反应构造桥联配合物;并将上述合成出来的配合物作为F-T合成反应的前驱体,并以γ-Al2O3为载体,制备催化剂,对催化剂进行F-T催化性能评价。具体工作如下:1.依照文献合成出带有羧基的四面体型钴羰基簇合物(CO)9Co3CCOOH,(CO)6Co2CHCCOOH,以它们为母体簇合物,分别和稀土(Yb、Sm、Eu)的三氟乙酸盐反应得到系列新的稀土-钴簇桥联配合物,并对它们进行了元素分析,红外光谱分析,电感耦合等离子发射光谱,X-单晶衍射分析以及热重分析,确定一种新的配合物的结构,Yb4-O{Co3(CO)9COO}6,其结构为:四个稀土原子通过氧原子连结,稀土原子周围通过六个钴羰基簇进行配位。2.将合成出来的配合物作为催化剂前驱体负载到γ-Al2O3上,制备不同的催化剂并对催化剂进行了F-T催化性能评价。
【Abstract】 In this paper, bridging complexes, which can be used as the precursor of F-T synthesis, contain both cobalt carbonyl cluster and lanthanide were designed to use as the precursor of F-T synthesis. First, Tetrahedron-cobalt carbonyl cluster with carboxyl was synthesized use Co2(CO)8 as the raw material and the cluster was used to react with lanthanide (Yb、Sm、Eu) trifluoroacetate to construct bridging complexes. Then, a series of catalysts were prepared by impregnating the complexes synthesized onγ-Al2O3 support for the first time, and F-T catalytic performance was evaluated. Concrete work as follows:1. Cluster (CO)9Co3CCOOH, (CO)6Co2CHCCOOH, was used to react with lanthanide (Yb、Sm、Eu) trifluoroacetate respectively, and a series of bridging complexes contained lanthanide and cobalt clusters were synthesized and characterized by IR,ICP,C/H element analysis ,X-ray diffraction and thermal analysis, Cluster1 was Yb4-O{Co3(CO)9COO}6 determined by X-ray single crystal diffraction analysis. The structure of the complexes were speculated as: four lanthanide atom were bridging with O, cobalt carbonyl clusters were coordinated to the lanthanide atom to form a Steady structure. Since dicobalt carbonyl clusters’ crystallization conditions difficult to control, crystal training work remains to be further explored.2. A series of catalysts were prepared by impregnating the complexes synthesized onγ-Al2O3 support, and characterized by surface area analysis (BET), and thermal analysis (TGA).
【Key words】 cobalt carbonyl cluster; rare earth complexes; bridging complex; F-T synthesis;
- 【网络出版投稿人】 内蒙古大学 【网络出版年期】2010年 04期
- 【分类号】O643.3
- 【下载频次】176