284114 In Situ and Operando Raman/IR/UV-Vis/MS Spectroscopic Studies of Propylene Metathesis by Supported Wox/SiO2 Catalysts

Thursday, November 1, 2012: 10:10 AM
317 (Convention Center )
Israel E. Wachs1, Soe Lwin1, Wu Zhou2, Chris K. Kiely3, Nikolaos Soultanidis4 and Michael S. Wong5, (1)Chemical Engineering, Lehigh University, Bethlehem, PA, (2)Mat. Sci. & Eng., Lehigh University, Bethlehem, PA, (3)Center for Advanced Materials and Nanotechnology, Lehigh University, Bethlehem, PA, (4)Chemical and Biomolecular Engineering, Rice University, Houston, TX, (5)Department of Chemical and Biomolecular Engineering, Rice University, Houston, TX

SiO2-supported tungsten oxide catalysts are used for high temperature (300-400 °C) metathesis of low molecular olefins such as production of ethylene and butene from propylene as well as the reverse reaction for production of propylene. Surprisingly, almost no characterization studies have been reported about olefin metathesis heterogeneous catalysts under reaction conditions. The objective of this investigation is to obtain fundamental insights about the catalytic active sites and surface reaction intermediates present during propylene metathesis over supported WO3/SiO2 catalysts.

The SiO2-supported catalysts were synthesized by conventional incipient-wetness impregnation of ammonium metatungstate (AMT), solvothermal reaction between AMT and oleylamine (NP) and controlling decomposition/reduction of AMT using trimethylamine N-oxide (sNP). The catalysts were characterized with operando Raman and UV-vis spectroscopy during propylene metathesis.

 The new insights generated with the operando spectroscopy experiments reveal for the first time the molecular structure-activity relationships of SiO2-supported tungsten oxide heterogeneous catalysts for propylene metathesis.  The dispersed surface WOx species are the selective catalytic active sites for propylene metathesis and the crystalline WO3 NPs are unselective for propylene metathesis.

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See more of this Session: In Situ and Operando Spectroscopy of Catalysts I
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