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From plants to plastics: continuous catalytic routes for the production of renewable monomers

Yakabi Diosdado, Laura 2018. From plants to plastics: continuous catalytic routes for the production of renewable monomers. PhD Thesis, Cardiff University.
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Moving towards a more sustainable chemical society requires the discovery and development of alternative catalytic routes to replace the current petrochemical industry. In this respect, the valorisation of biomass into commodity compounds, such as polymers, represents a great challenge. In order to tackle this challenge, various key points call for attention, including: i) the quest of identifying a suitable catalyst, ii) optimising operational conditions to obtain high levels of selectivity towards the desired product, and iii) studying potential process intensification. This thesis provides a detailed investigation of two catalytic routes to produce renewable monomers: the Baeyer-Villiger oxidation (BVO) reaction of substituted cyclohexanones, and the selective hydrogenation of succinic acid to give rise to the corresponding lactones. This work begins in Chapter 3, with the full elucidation of the kinetic, mechanistic and lifetime aspects of the BVO reaction of cyclohexanone to caprolactone, studied as a model reaction, using Sn-β as catalyst, and hydrogen peroxide as green oxidant. Taking the knowledge gained from the study of this model reaction, the substrate scope is broadened to various substituted cyclohexanones in Chapter 4, where various kinetic, steric, electronic, and thermodynamic elements of this transformation are investigated in greater detail than previously achieved. Additionally, the intensification of this process in continuous flow, and the production of polymer-grade lactone monomers, are also evaluated. Following this, Chapter 5 is focused on the coupling of in situ hydrogen peroxide production with the BVO system, in order to potentially upgrade the sustainability of this process. Subsequently, selective hydrogenation of succinic acid to γ-butyrolactone over various metal supported nanoparticles is discussed in Chapter 6, showing how the choice of metal, support and operational conditions determines the product distribution and catalytic activity obtained. In closing, Chapter 7 evaluates the consequences of the findings of this research, and the pertaining challenges that these findings open.

Item Type: Thesis (PhD)
Date Type: Completion
Status: Unpublished
Schools: Chemistry
Subjects: Q Science > QD Chemistry
Funders: Engineering and Physical Sciences Research Council
Date of First Compliant Deposit: 22 March 2019
Last Modified: 04 Aug 2022 01:56

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