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Metal-incorporated beta zeolites: A versatile class of catalysts for continuous glucose upgrading

Botti, Luca 2020. Metal-incorporated beta zeolites: A versatile class of catalysts for continuous glucose upgrading. PhD Thesis, Cardiff University.
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Glucose upgrading to chemical commodities is an essential step to employ biomass as a novel and renewable source of carbon for chemical production. Sn-Beta zeolite is known to efficiently catalyse the upgrading of glucose to several commodities such as fructose, a-hydroxy esters and furanic compounds. Nonetheless, Sn- Beta is a catalyst of academic interest only; the lack of knowledge on its stability and selectivity over continuous processes represent an important drawback to its application in the chemical industry. During my PhD studies I focused on tackling this problem investigating and improving the kinetic performance of Sn-Beta zeolite during glucose upgrading to fructose and a-hydroxy esters, five experimental chapters are presented in the manuscript, from chapter 2 to chapter 6. In chapter 2 the causes of Sn-Beta deactivation in methanol were explored, and small traces of water in the feed of reaction were found to increment the stability of the processes carried out by Sn-Beta zeolite. In the third chapter it was shown how the activity and stability of this material are strongly affected by the methodology of preparation, and how the hydrothermal synthesis leads to the most performant material. In chapter 4 the “pre-activation” protocol of Sn-Beta was unveiled, this new treatment enhanced the performances of Sn-Beta for glucose upgrading by tuning the active site and the textural properties of the material. In chapter 5, a new Hf-incorporated Beta zeolite was discovered as a more selective catalyst for glucose isomerisation to fructose, achieving over 50 % yield in fructose with no loss of substrate. In the last experimental chapter of the manuscript the experience gained throughout the whole project allowed to expand the scope of operando UV-Vis glucose upgrading, benchmarking the different interactions between the substrate and the catalyst. In this chapter different UVVis interactions between catalyst and sugars were attributed to different chemical pathway, generating therefore a powerful methodology to monitor the catalyst deactivation during sugars upgrading. Throughout this project a better understanding of the performances of Sn-Beta zeolite in continuous conditions was achieved, important developments were brought to the field and new issues were raised suggesting the next challenges to tackle.

Item Type: Thesis (PhD)
Date Type: Completion
Status: Unpublished
Schools: Chemistry
Date of First Compliant Deposit: 9 November 2020
Last Modified: 09 Nov 2020 13:24

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