In –Situ Spectroscopic Investigation of Immobilized Organometallic Catalysts

Davis, Robert, J.

关键词: ABSORPTION SPECTROSCOPY;    AMINES;    CATALYSIS;    CATALYSTS;    COMMUNITIES;    DEACTIVATION;    EPOXIDES;    HETEROGENEOUS CATALYSIS;    KINETICS;    LEACHING;    PROBES;    RESOLUTION;    SILICA;    TRANSITION ELEMENTS;    ZEOLITES ca;   

DOI  :  10.2172/919527
RP-ID  :  DOE/ER/15460
PID  :  OSTI ID: 919527
Others  :  TRN: US200821%%343

学科分类：化学（综合）

美国|英语

来源: SciTech Connect

【 摘 要 】

Immobilized organometallic catalysts, in principle, can give high rates and selectivities like homogeneous catalysts with the ease of separation enjoyed by heterogeneous catalysts. However, the science of immobilized organometallics has not been developed because the field lies at the interface between the homogeneous and heterogeneous catalysis communities. By assembling an interdisciplinary research team that can probe all aspects of immobilized organometallic catalyst design, the entire reacting system can be considered, where the transition metal complex, the complex-support interface and the properties of the support can all be considered simultaneously from both experimental and theoretical points of view. Researchers at Georgia Tech and the University of Virginia are studying the fundamental principles that can be used to understand and design future classes of immobilized organometallic catalysts. In the framework of the overall collaborative project with Georgia Tech, our work focused on (a) the X-ray absorption spectroscopy of an immobilized Pd-SCS-O complex (b) the mode of metal leaching from supported Pd catalysts during Heck catalysis and (c) the mode of deactivation of Jacobsen’s Co-salen catalysts during the hydrolytic kinetic resolution of terminal epoxides. Catalysts containing supported Pd pincer complexes, functionalized supports containing mercapto and amine groups, and oligomeric Co-salen catalysts were synthesized at Georgia Tech and sent to the University of Virginia. Incorporation of Pd onto several different kinds of supports (silica, mercapto-functionalized silica, zeolite Y) was performed at the University of Virginia.