From metal-organic frameworks to porous carbons: heterogeneous catalysis by carbon-supported Pd nanoparticles

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2016-01-01
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Tesfagaber, Daniel
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Wenyu Huang
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Chemistry
Abstract

The last decade has seen a significant increase in research on biomass conversion to fuels and chemicals to address the limited supply of fossil fuels and to mitigate global warming. Numerous reactions and processes have been explored to upgrade biomass-derived platform chemicals to value-added products. The search for recyclable heterogeneous catalysts that remain stable and selective to desired products remains a key component for effective utilization of biomass. This thesis describes the synthesis of ultrasmall palladium nanoparticles supported on porous carbon derived from a sacrificial Al-MIL-101-NH2 metal-organic framework (MOF) template. Although three different Pd precursors were examined, potassium tetrachloropalladate (II) was found to yield the smallest monodisperse Pd nanoparticles. The synthesized Pd catalyst was found to have excellent activity, recyclability and selectivity for the selective hydrogenation of furfural to furfuryl alcohol in mild conditions. Compared to industrial conditions, our catalyst required much lower temperature and pressure, and showed no sign of leaching of active Pd species.

Finally, we also attempted to synthesize intermetallic compounds by using this model system, but we were not able to achieve monodisperse nanoparticles. With further screening and testing, this simple method however still holds promise for the development of new carbon-supported catalysts which can be utilized for the transformation of platform biomass feedstocks to value-added products.

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Fri Jan 01 00:00:00 UTC 2016