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Investigations on the selective deoxygenation of sugar alcohols over heterogeneous catalysts

Kühne, Benjamin Bernhard (2018):
Investigations on the selective deoxygenation of sugar alcohols over heterogeneous catalysts.
Darmstadt, Technische Universität, [Online-Edition: http://tuprints.ulb.tu-darmstadt.de/7559],
[Ph.D. Thesis]

Abstract

In this PhD thesis, the industrial potential for selective deoxygenation (-C-O- bond cleavage) of biomass-derived polyols was investigated over heterogeneous catalysts. Standard commercial hydrogenation catalysts based on Ru, Ni and Cu were applied for the hydrogenolysis of various sugars and sugar alcohols, including sucrose, glucose, sorbitol, mannitol, and xylitol. The effect of the active metal and support material were investigated with regards to compare -C-O- vs. -C-C- bond cleavage properties.

For this purpose, reaction intermediates were identified and isolated to better understand the mechanisms involved in the selective -C-O- bond cleavage over Cu catalysts. Furthermore, different reaction pathways for -C-C- bond cleavage (degradation of the carbon chain) were evaluated such as retro-aldol reactions, decarbonylation and decarboxylation.

Finally, the separation of deoxygenated C6 polyols from short-chain compounds such as glycols and glycerol were investigated by comparing standard industrial downstream processes: ion-exchange chromatography and liquid-liquid extraction using non-soluble polar solvents.

Item Type: Ph.D. Thesis
Erschienen: 2018
Creators: Kühne, Benjamin Bernhard
Title: Investigations on the selective deoxygenation of sugar alcohols over heterogeneous catalysts
Language: English
Abstract:

In this PhD thesis, the industrial potential for selective deoxygenation (-C-O- bond cleavage) of biomass-derived polyols was investigated over heterogeneous catalysts. Standard commercial hydrogenation catalysts based on Ru, Ni and Cu were applied for the hydrogenolysis of various sugars and sugar alcohols, including sucrose, glucose, sorbitol, mannitol, and xylitol. The effect of the active metal and support material were investigated with regards to compare -C-O- vs. -C-C- bond cleavage properties.

For this purpose, reaction intermediates were identified and isolated to better understand the mechanisms involved in the selective -C-O- bond cleavage over Cu catalysts. Furthermore, different reaction pathways for -C-C- bond cleavage (degradation of the carbon chain) were evaluated such as retro-aldol reactions, decarbonylation and decarboxylation.

Finally, the separation of deoxygenated C6 polyols from short-chain compounds such as glycols and glycerol were investigated by comparing standard industrial downstream processes: ion-exchange chromatography and liquid-liquid extraction using non-soluble polar solvents.

Place of Publication: Darmstadt
Divisions: 07 Department of Chemistry
07 Department of Chemistry > Fachgebiet Technische Chemie
07 Department of Chemistry > Fachgebiet Technische Chemie > Technische Chemie I
Date Deposited: 12 Aug 2018 19:55
Official URL: http://tuprints.ulb.tu-darmstadt.de/7559
URN: urn:nbn:de:tuda-tuprints-75598
Referees: Vogel, Prof. Dr. Herbert and Kunz, Prof. Dr. Markwart
Refereed / Verteidigung / mdl. Prüfung: 11 April 2018
Alternative Abstract:
Alternative abstract Language
In dieser Dissertation wurde das industrielle Potenzial für die selektive Deoxygenierung (-C-O-Bindungsspaltung) von bio-basierten Polyolen an heterogene Katalysatoren untersucht. Handelsübliche Hydrierkatalysatoren auf der Basis von Ru, Ni und Cu wurden für die Hydrogenolyse verschiedener Zucker und Zuckeralkohole, einschließlich Saccharose, Glucose, Sorbitol, Mannitol und Xylitol, eingesetzt. Die Wirkung des aktiven Metalls und des Trägermaterials wurde im Hinblick auf den Vergleich von -C-O- und -C-C-Bindungsspaltungseigenschaften untersucht. Zu diesem Zweck wurden bisher unbekannte Reaktionsintermediate aus dem Produktgemisch identifiziert und isoliert, um die Mechanismen der selektiven -C-O- Bindungsspaltung besser zu verstehen. Für Cu-Katalsatoren wurde ein Mechanismus zur Entstehung von diversen deoxygenierten Zuckeralkoholen postuliert. Darüber hinaus wurden verschiedene Reaktionswege für die -C-C- Bindungsspaltung (Abbau der Kohlenstoffkette) wie retro-Aldol Reaktionen, Decarbonylierung und Decarboxylierung untersucht. Abschließend wurde die Abtrennung von deoxygenierten C6-Polyolen von kurzkettigen Verbindungen wie Glykolen und Glycerin durch einen Vergleich industrieller Downstream-Prozesse untersucht: Ionenaustauschchromatographie und Flüssig-Flüssig-Extraktion mit nicht-löslichen polaren Lösungsmitteln.German
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