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Designing bifunctional heterogeneous catalysts for the upgrading of bioderived alcohols

Jones, Kennedy R. 2023. Designing bifunctional heterogeneous catalysts for the upgrading of bioderived alcohols. PhD Thesis, Cardiff University.
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Abstract

The development of sustainable alternatives to traditional fossil fuels is of paramount importance. Ethanol has become a mainstream fuel additive in the UK, however, storage issues, low energy density and corrosion to engines are all issues when using this alternative fuel. A substitute for this has been identified; butanol possesses properties closer to that of petrol. One synthesis method being explored is the Guerbet reaction, which upgrades bioderived ethanol to n-butanol and isobutanol by alcohol coupling. Homogeneous catalysts for this reaction perform well but require a high amount of added base and often cannot be recovered. The heterogeneous catalysts studied previously, largely require high temperatures to achieve high ethanol conversions. Additionally, they do not provide good control over the reaction, resulting in a low selectivity to the desired product. Therefore, there is much scope to develop on the current literature. Herein, it was established that bimetallic 1% RuPd/TiO2 was significantly more active than its monometallic counterparts. Catalytic testing and characterisation of the catalysts showed that this was likely due to the synergy between the two metals. The metals supported by titanium dioxide were altered to develop a more sustainable alternative to the noble metals. A highly active 1% CuPd/TiO2 catalyst was synthesised that could provide high levels of ethanol conversion and isobutanol yield without added sodium methoxide. Further development, however, could not reproduce this catalyst. The effect of changing the support was studied with the view of understanding the acidity and basicity of each catalyst and how this relates to the observed catalytic performance. Finally, a proof of concept was shown for the use of microwave reactors with heterogeneous catalysts for this reaction.

Item Type: Thesis (PhD)
Date Type: Completion
Status: Unpublished
Schools: Chemistry
Date of First Compliant Deposit: 1 May 2024
Last Modified: 01 May 2024 12:59
URI: https://orca.cardiff.ac.uk/id/eprint/168559

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