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Ru on N‐doped Carbon for the Selective Hydrogenolysis of Sugars and Sugar Alcohols

Beine, Anna Katharina ; Ludovicy, Jil ; Chai, Jiachun ; Hofmann, Jan P. ; Glotzbach, Christoph ; Hausoul, Peter J. C. ; Palkovits, Regina (2022)
Ru on N‐doped Carbon for the Selective Hydrogenolysis of Sugars and Sugar Alcohols.
In: ChemCatChem, 2022, 14 (11)
doi: 10.26083/tuprints-00022448
Article, Secondary publication, Publisher's Version

Abstract

Glycols are accessible via metal‐catalyzed hydrogenolysis of sugar alcohols such as xylitol obtained from hemicellulose. Ru‐based catalysts are highly active but also catalyze side‐reactions such as decarbonylation and deoxygenation. To achieve high selectivity, these reactions need to be suppressed. In our study, we introduce heteroatom doped carbon materials as catalyst supports providing high selectivity. Heteroatom doping with nitrogen and oxygen was achieved by treating activated carbon with HNO₃, NH₃ and H₂ or carbonization of organic precursors. For all N‐doped materials a high glycol selectivity of ∼ 80 % for sorbitol and xylitol and 44 % for xylose and glucose was reached. XPS analysis confirms the presence of different nitrogen species at the carbon surface and varying ligand effects for oxygen and nitrogen. Oxygen has an electron withdrawing effect on ruthenium and leads to a decreased activity. Nitrogen has weaker electron withdrawing properties, resulting in an enhanced selectivity.

Item Type: Article
Erschienen: 2022
Creators: Beine, Anna Katharina ; Ludovicy, Jil ; Chai, Jiachun ; Hofmann, Jan P. ; Glotzbach, Christoph ; Hausoul, Peter J. C. ; Palkovits, Regina
Type of entry: Secondary publication
Title: Ru on N‐doped Carbon for the Selective Hydrogenolysis of Sugars and Sugar Alcohols
Language: English
Date: 2022
Place of Publication: Darmstadt
Year of primary publication: 2022
Publisher: Wiley-VCH
Journal or Publication Title: ChemCatChem
Volume of the journal: 14
Issue Number: 11
Collation: 8 Seiten
DOI: 10.26083/tuprints-00022448
URL / URN: https://tuprints.ulb.tu-darmstadt.de/22448
Corresponding Links:
Origin: Secondary publication DeepGreen
Abstract:

Glycols are accessible via metal‐catalyzed hydrogenolysis of sugar alcohols such as xylitol obtained from hemicellulose. Ru‐based catalysts are highly active but also catalyze side‐reactions such as decarbonylation and deoxygenation. To achieve high selectivity, these reactions need to be suppressed. In our study, we introduce heteroatom doped carbon materials as catalyst supports providing high selectivity. Heteroatom doping with nitrogen and oxygen was achieved by treating activated carbon with HNO₃, NH₃ and H₂ or carbonization of organic precursors. For all N‐doped materials a high glycol selectivity of ∼ 80 % for sorbitol and xylitol and 44 % for xylose and glucose was reached. XPS analysis confirms the presence of different nitrogen species at the carbon surface and varying ligand effects for oxygen and nitrogen. Oxygen has an electron withdrawing effect on ruthenium and leads to a decreased activity. Nitrogen has weaker electron withdrawing properties, resulting in an enhanced selectivity.

Uncontrolled Keywords: Activated Carbon, Glycols, Hydrogenolysis, N-doping, Ruthenium
Status: Publisher's Version
URN: urn:nbn:de:tuda-tuprints-224489
Additional Information:

This article also appears in: 55. Jahrestreffen Deutscher Katalytiker

Classification DDC: 600 Technology, medicine, applied sciences > 660 Chemical engineering
Divisions: 11 Department of Materials and Earth Sciences
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences > Material Science > Surface Science
Date Deposited: 10 Oct 2022 12:49
Last Modified: 11 Oct 2022 05:18
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