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New homogenous and heterogenised catalysts for bioethanol upgrading to advanced biofuels

Sama, Folasade Josephine 2021. New homogenous and heterogenised catalysts for bioethanol upgrading to advanced biofuels. PhD Thesis, Cardiff University.
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Abstract

Biofuels obtained from biomass sources have attracted increasing attention due to their economic and environmental benefits. Shifting society’s dependence away from gasoline to biofuels is an important contributor to sustainable development and effective management of greenhouse gas emissions. Particular attention has been given to bioethanol as an alternative to gasoline in past few decades. With the limitations of bioethanol as fuel and the sought for better substitutes for gasoline, the focus of this work is geared towards upgrading bioethanol to 1-butanol and iso-butanol whose fuel properties are similar to that of gasoline and, are thus termed “advanced biofuels”. Such transformation processes require the employment of suitable catalysts for acceptable productivity and selectivity. Ruthenium complexes have shown great catalytic activity in borrowed hydrogen chemistry which is advantageous to this system. In this study, special interest is given to the design of Ru-catalysts with combined homogeneous and heterogeneous properties in order to preclude the degradation of metal complexes and promote the recoverability and reusability of the catalysts. A two distinct classes of ruthenium-diphosphine has been synthesised and employed in the upgrading of ethanol to advanced biofuels. The first class, ruthenium-PNP with remote functionalities, displayed reasonable activity in the conversion of ethanol to 1-butanol and iso-butanol. With this baseline activity, the heterogenisation of the ruthenium-PNP catalysts was performed and variety of characterisation techniques confirmed the process was successful. The utilisation of the heterogeneous catalysts for ethanol-methanol upgrading to iso-butanol gave moderate yield and selectivity of iso-butanol with good recoverability. The other class of catalysts, ruthenium-PP, showed remarkable activity towards ethanol-methanol upgrading to iso-butanol with good productivity and excellent selectivity.

Item Type: Thesis (PhD)
Date Type: Completion
Status: Unpublished
Schools: Chemistry
Date of First Compliant Deposit: 22 June 2021
Last Modified: 22 Jun 2022 14:23
URI: https://orca.cardiff.ac.uk/id/eprint/142142

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