Reif, Phillip (2023)
Sustainable Production of Aromatics by Catalytic Aldol Condensation of Biomass-Derived Ketones.
Technische Universität Darmstadt
doi: 10.26083/tuprints-00026330
Dissertation, Erstveröffentlichung, Verlagsversion
Kurzbeschreibung (Abstract)
Achieving carbon neutrality and establishing a circular bioeconomy are major challenges of our time. Currently, polymers are predominantly derived from fossil resources. However, increasing demands for their sustainable production require the exploration of alternative pathways based on renewable biomass. For many monomers, aromatics are key precursors, but the large-scale production from biomass remains limited. Catalytic self-aldol condensation of biomass-derived alkyl methyl ketones over solid acid catalysts to aromatics is a promising, less explored pathway. The one-step reaction requires neither hydrogen nor precious metal catalysts. In this study, the aromatization of the model compound acetone was initially investigated under solvent-free batch and continuous flow conditions over commercially available catalysts. The goal was to identify acid catalysts with superior stability and activity and to elucidate structure-activity relationships. The most active catalyst under batch conditions proved to be unstable in the continuous flow reactor. Conversely, larger pore silica-alumina catalysts were observed to provide stable aromatization activity under flow conditions. Very high stability (> 50 h time-on-stream) combined with significant activity was found for the amorphous silica-alumina Siralox 30. The catalyst was also suitable for the aromatization of 2-butanone. Increased space-time-yield and energy-efficient product separation are feasible through solvent-free reaction conditions. Overcoming the challenges associated with catalyst deactivation represents a significant step toward the potential scale-up of the alkyl methyl ketone route and contributes to the transition to a fossil-free, renewable chemical industry.
| Typ des Eintrags: | Dissertation | ||||
|---|---|---|---|---|---|
| Erschienen: | 2023 | ||||
| Autor(en): | Reif, Phillip | ||||
| Art des Eintrags: | Erstveröffentlichung | ||||
| Titel: | Sustainable Production of Aromatics by Catalytic Aldol Condensation of Biomass-Derived Ketones | ||||
| Sprache: | Englisch | ||||
| Referenten: | Rose, Prof. Dr. Marcus ; Busch, Prof. Dr. Markus | ||||
| Publikationsjahr: | 4 Dezember 2023 | ||||
| Ort: | Darmstadt | ||||
| Kollation: | ix, 103 Seiten | ||||
| Datum der mündlichen Prüfung: | 13 November 2023 | ||||
| DOI: | 10.26083/tuprints-00026330 | ||||
| URL / URN: | https://tuprints.ulb.tu-darmstadt.de/26330 | ||||
| Kurzbeschreibung (Abstract): | Achieving carbon neutrality and establishing a circular bioeconomy are major challenges of our time. Currently, polymers are predominantly derived from fossil resources. However, increasing demands for their sustainable production require the exploration of alternative pathways based on renewable biomass. For many monomers, aromatics are key precursors, but the large-scale production from biomass remains limited. Catalytic self-aldol condensation of biomass-derived alkyl methyl ketones over solid acid catalysts to aromatics is a promising, less explored pathway. The one-step reaction requires neither hydrogen nor precious metal catalysts. In this study, the aromatization of the model compound acetone was initially investigated under solvent-free batch and continuous flow conditions over commercially available catalysts. The goal was to identify acid catalysts with superior stability and activity and to elucidate structure-activity relationships. The most active catalyst under batch conditions proved to be unstable in the continuous flow reactor. Conversely, larger pore silica-alumina catalysts were observed to provide stable aromatization activity under flow conditions. Very high stability (> 50 h time-on-stream) combined with significant activity was found for the amorphous silica-alumina Siralox 30. The catalyst was also suitable for the aromatization of 2-butanone. Increased space-time-yield and energy-efficient product separation are feasible through solvent-free reaction conditions. Overcoming the challenges associated with catalyst deactivation represents a significant step toward the potential scale-up of the alkyl methyl ketone route and contributes to the transition to a fossil-free, renewable chemical industry. |
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| Alternatives oder übersetztes Abstract: |
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| Freie Schlagworte: | Biomasse, Aromaten, Katalyse, Katalysatorstabilität, Rohrreaktor | ||||
| Status: | Verlagsversion | ||||
| URN: | urn:nbn:de:tuda-tuprints-263309 | ||||
| Sachgruppe der Dewey Dezimalklassifikatin (DDC): | 600 Technik, Medizin, angewandte Wissenschaften > 660 Technische Chemie | ||||
| Fachbereich(e)/-gebiet(e): | 07 Fachbereich Chemie 07 Fachbereich Chemie > Ernst-Berl-Institut > Fachgebiet Technische Chemie 07 Fachbereich Chemie > Ernst-Berl-Institut > Fachgebiet Technische Chemie > Technische Chemie II |
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| TU-Projekte: | PTJ|031B0680|BioAromatics | ||||
| Hinterlegungsdatum: | 04 Dez 2023 13:04 | ||||
| Letzte Änderung: | 05 Dez 2023 09:27 | ||||
| PPN: | |||||
| Referenten: | Rose, Prof. Dr. Marcus ; Busch, Prof. Dr. Markus | ||||
| Datum der mündlichen Prüfung / Verteidigung / mdl. Prüfung: | 13 November 2023 | ||||
| Export: | |||||
| Suche nach Titel in: | TUfind oder in Google | ||||
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