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Nanoscale Hybrid Amorphous/Graphitic Carbon as Key Towards Next‐Generation Carbon‐Based Oxidative Dehydrogenation Catalysts

Herold, Felix ; Prosch, Stefan ; Oefner, Niklas ; Brunnengräber, Kai ; Leubner, Oliver ; Hermans, Yannick ; Hofmann, Kathrin ; Drochner, Alfons ; Hofmann, Jan P. ; Qi, Wei ; Etzold, Bastian J. M. (2021):
Nanoscale Hybrid Amorphous/Graphitic Carbon as Key Towards Next‐Generation Carbon‐Based Oxidative Dehydrogenation Catalysts. (Publisher's Version)
In: Angewandte Chemie International Edition, 60 (11), pp. 5898-5906. Wiley, ISSN 1433-7851, e-ISSN 1521-3773,
DOI: 10.26083/tuprints-00019350,
[Article]

Abstract

A new strategy affords “non-nano” carbon materials as dehydrogenation catalysts that perform similarly to nanocarbons. Polymer-based carbon precursors that combine a soft-template approach with ion adsorption and catalytic graphitization are key to this synthesis strategy, thus offering control over macroscopic shape, texture, and crystallinity and resulting in a hybrid amorphous/graphitic carbon after pyrolysis. From this intermediate the active carbon catalyst is prepared by removing the amorphous parts of the hybrid carbon materials via selective oxidation. The oxidative dehydrogenation of ethanol was chosen as test reaction, which shows that fine-tuning the synthesis of the new carbon catalysts allows to obtain a catalytic material with an attractive high selectivity (82 %) similar to a carbon nanotube reference, while achieving 10 times higher space–time yields at 330 °C. This new class of carbon materials is accessible via a technically scalable, reproducible synthetic pathway and exhibits spherical particles with diameters around 100 μm, allowing unproblematic handling similar to classic non-nano catalysts.

Item Type: Article
Erschienen: 2021
Creators: Herold, Felix ; Prosch, Stefan ; Oefner, Niklas ; Brunnengräber, Kai ; Leubner, Oliver ; Hermans, Yannick ; Hofmann, Kathrin ; Drochner, Alfons ; Hofmann, Jan P. ; Qi, Wei ; Etzold, Bastian J. M.
Origin: Secondary publication service
Status: Publisher's Version
Title: Nanoscale Hybrid Amorphous/Graphitic Carbon as Key Towards Next‐Generation Carbon‐Based Oxidative Dehydrogenation Catalysts
Language: English
Abstract:

A new strategy affords “non-nano” carbon materials as dehydrogenation catalysts that perform similarly to nanocarbons. Polymer-based carbon precursors that combine a soft-template approach with ion adsorption and catalytic graphitization are key to this synthesis strategy, thus offering control over macroscopic shape, texture, and crystallinity and resulting in a hybrid amorphous/graphitic carbon after pyrolysis. From this intermediate the active carbon catalyst is prepared by removing the amorphous parts of the hybrid carbon materials via selective oxidation. The oxidative dehydrogenation of ethanol was chosen as test reaction, which shows that fine-tuning the synthesis of the new carbon catalysts allows to obtain a catalytic material with an attractive high selectivity (82 %) similar to a carbon nanotube reference, while achieving 10 times higher space–time yields at 330 °C. This new class of carbon materials is accessible via a technically scalable, reproducible synthetic pathway and exhibits spherical particles with diameters around 100 μm, allowing unproblematic handling similar to classic non-nano catalysts.

Journal or Publication Title: Angewandte Chemie International Edition
Journal volume: 60
Number: 11
Publisher: Wiley
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: 25 Aug 2021 12:09
DOI: 10.26083/tuprints-00019350
Official URL: https://tuprints.ulb.tu-darmstadt.de/19350
URN: urn:nbn:de:tuda-tuprints-193504
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