Selective Catalytic Oxidation of Organosulfur Compounds to Valuable Chemical Intermediates

Wachs和Stenger教授建议研究有机硫化合物的催化氧化脱硫。 这一基本过程可应用于纸浆和造纸工业副产品的环境修复。 C1-有机硫化合物选择性氧化的基本动力学和机理将在负载型金属氧化物催化剂上进行研究，主要是V，Mo，Cr和Re的那些。 典型的反应是COS或CS2氧化成CO和SO2，CH 3SH氧化成H2 CO、SO2和H2O，以及生成衍生物甲醇和硫酸。 所述氧化物将负载在二氧化钛上直至单层覆盖，并用W或Nb以及K或P改性。固体的原位表征技术将包括拉曼、IR、UV-Vis DRS和固态NMR。 动力学测量将在微分反应器中进行，以及与程序升温反应光谱。 该研究将导致在理解的作用，如速率决定步骤，金属氧化物网站的活性合奏，电负性的支持配体，氧化支持网站的协调，和相互作用的共吸附物种的反应参数。 在实践中，它将导致硫化合物催化升级为有价值的化学中间体的改进工艺。

Professors Wachs and Stenger propose to investigate the catalytic oxidative desulfurizaiton of organosulfur compounds. This fundamental process finds applications in the environmental remediation of byproducts from pulp and paper industry. Fundamental kinetics and mechanisms of the selective oxidation of C1-organosulfur compounds will be studies on supported metal oxide catalysts, primarily those of V, Mo, Cr and Re. Typical reactions are the oxidation of COS or CS2 to CO and SO2, and the oxidaiton of CH3SH to H2CO, SO2, and H2O, as well as the production of derivatives methanol and sulfuric acid. The mentioned oxides will be supported on titania up to monolayer coverage and modified with W or Nb as well as K or P. In situ characterization techniques for the solid will include Raman, IR, UV-Vis DRS, and solid state NMR. Kinetics measurement will be performed in differential reactors as well as with temperature-programmed reactin spectroscopy. The research will result in understanding of the role of reaction parameters such as rate determining step, number of metal oxide sites in the active ensembles, electronegativity of the support ligands, coordination of the oxidic support site, and interaction of co-adsorbed species. In practice, it will lead to improved processes for the catalytic upgrade of sulfur compounds to valuable chemical intermediates.