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Structure-activity relationship studies of supported metal catalysts for benzyl alcohol oxidation and propane dehydrogenation

Wang, Kai 2022. Structure-activity relationship studies of supported metal catalysts for benzyl alcohol oxidation and propane dehydrogenation. PhD Thesis, Cardiff University.
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Abstract

The recent discovery of a cooperative redox enhancement (CORE) effect provides a new route to the design of multicomponent heterogeneous catalysts. Following this, an investigation was performed to determine whether this CORE effect could be extended to the selective oxidation of benzyl alcohol, and the influence of Au/Pd molar ratios on CORE mechanism was also explored. A series of monometallic Aux/C and Pdy/C catalysts, Aux-Pdy/C alloy catalysts and physical mixture catalysts (Aux/C + Pdy/C) possessing various Au/Pd molar ratios were prepared and tested. The catalytic results showed that there did not appear to be a CORE effect in this system, which was likely due to the absence of solvent and base. Interestingly, the monometallic Pdy/C exhibited higher activity than Aux-Pdy/C alloy catalysts, regardless the Au/Pd ratios under investigation. The influence of thermal pre-treatment of carbon support on the catalytic performance of supported Pd nanoparticles for solvent-free benzyl alcohol oxidation was investigated. A promotional effect on catalytic activity was observed with increasing calcination temperature of carbon. This promotional effect was attributed to the more exposed active Pd atoms on the pre-calcined carbon, and more importantly, the promoted disproportionation reaction rate due to the introduced surface functionalities, in particular -COOH groups, during the calcination process. With the help of DFT calculations, a study was performed to investigate the effect of metal oxide supports on the catalytic behaviour of atomically dispersed Pt catalysts for oxidative and non-oxidative dehydrogenation of propane. A variety of atomically dispersed Pt catalysts supported on various metal oxides were prepared by wet impregnation with a rotavapor, followed with a calcination treatment. The CeO2 and tetragonal ZrO2 supported Pt catalysts were found to exhibit higher activity and selectivity towards propene in both reactions compared to other metal oxides under investigation.

Item Type: Thesis (PhD)
Date Type: Completion
Status: Unpublished
Schools: Chemistry
Date of First Compliant Deposit: 11 September 2023
Last Modified: 11 Sep 2023 10:42
URI: https://orca.cardiff.ac.uk/id/eprint/162363

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