Supported Sulfide Cluster Catalysts for Hydrodesulfurization

这个小企业创新研究（SBIR）第一阶段项目是在分析和表面化学的一般领域以及多相催化的子领域。这项活动的重点是对用于加氢脱硫的金属硫化物簇-氧化物支撑系统（HDS）的基础研究。尽管对加氢脱硫进行了广泛的研究，但人们对加氢脱硫仍然知之甚少。簇衍生催化剂在HDS中的应用代表了一种识别HDS活性位点和了解其物理化学性质的新方法。与传统制备的HDS催化剂相比，这种类型的催化剂也具有更好的活性和选择性。在该项目的研究计划执行中，Thompson博士将研究同核硫化物簇Cp2Mo2(uS)2(uSH)2, Fe2(uS)2(CO)6和Co6(u3S)2(CO)12的行为。由于这些簇含有桥接硫化物配体，因此它们的金属框架在HDS反应条件下非常坚固和稳定。这些团簇将在部分去羟基化的γ - al2o3和MgO上合成和支撑。纯催化剂和负载催化剂将通过各种分析技术进行表征，包括红外光谱、表面积分析、x射线衍射和x射线光电子能谱。从这些研究中获得的对HDS反应的机理见解将作为这一重要催化过程模型的基础。

This Small Business Innovation Research (SBIR) Phase I project is in the general area of analytical and surface chemistry and in the subfield of heterogeneous catalysis. The thrust of this activity focusses on fundamental investigations of metal sulfide cluster-oxide support systems for hydrodesulfurization (HDS). Hydrodesulfurization remains a poorly understood reaction despite very extensive study. The use of cluster-derived catalysts for HDS represents a novel approach to identifying the active site for HDS and understanding its physicochemical nature. This type of catalyst could also have improved activity and selectivity relative to conventionally prepared HDS catalysts. In the execution of the research plan of this project, Dr. Thompson will investigate the behavior of the homonuclear sulfide clusters Cp2Mo2(uS)2(uSH)2, Fe2(uS)2(CO)6,and Co6(u3S)2(CO)12. Because these clusters contain bridging sulfide ligands, their metal frameworks are expected to be very robust and stable under HDS reaction conditions. These clusters will be synthesized and supported on partially dehydroxylated gamma-Al2O3 and MgO. The pure and supported catalysts will be characterized by a variety of analytical techniques including infrared spectroscopy, surface area analysis, X-ray diffraction, and X-ray photoelectron spectroscopy. Mechanistic insights into the HDS reaction garnered from these studies will be used as the basis for a model of this important catalytic process.