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Porosity and Structure of Hierarchically Porous Ni/Al₂O₃ Catalysts for CO₂ Methanation

Weber, Sebastian ; Abel, Ken L. ; Zimmermann, Ronny T. ; Huang, Xiaohui ; Bremer, Jens ; Rihko-Struckmann, Liisa K. ; Batey, Darren ; Cipiccia, Silvia ; Titus, Juliane ; Poppitz, David ; Kübel, Christian ; Sundmacher, Kai ; Gläser, Roger ; Sheppard, Thomas L. (2024)
Porosity and Structure of Hierarchically Porous Ni/Al₂O₃ Catalysts for CO₂ Methanation.
In: Catalysts, 2020, 10 (12)
doi: 10.26083/tuprints-00017428
Artikel, Zweitveröffentlichung, Verlagsversion

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Kurzbeschreibung (Abstract)

CO₂ methanation is often performed on Ni/Al₂O₃ catalysts, which can suffer from mass transport limitations and, therefore, decreased efficiency. Here we show the application of a hierarchically porous Ni/Al₂O₃ catalyst for methanation of CO₂. The material has a well-defined and connected meso- and macropore structure with a total porosity of 78%. The pore structure was thoroughly studied with conventional methods, i.e., N₂ sorption, Hg porosimetry, and He pycnometry, and advanced imaging techniques, i.e., electron tomography and ptychographic X-ray computed tomography. Tomography can quantify the pore system in a manner that is not possible using conventional porosimetry. Macrokinetic simulations were performed based on the measures obtained by porosity analysis. These show the potential benefit of enhanced mass-transfer properties of the hierarchical pore system compared to a pure mesoporous catalyst at industrially relevant conditions. Besides the investigation of the pore system, the catalyst was studied by Rietveld refinement, diffuse reflectance ultraviolet-visible (DRUV/vis) spectroscopy, and H₂-temperature programmed reduction (TPR), showing a high reduction temperature required for activation due to structural incorporation of Ni into the transition alumina. The reduced hierarchically porous Ni/Al₂O₃ catalyst is highly active in CO₂ methanation, showing comparable conversion and selectivity for CH₄ to an industrial reference catalyst.

Typ des Eintrags: Artikel
Erschienen: 2024
Autor(en): Weber, Sebastian ; Abel, Ken L. ; Zimmermann, Ronny T. ; Huang, Xiaohui ; Bremer, Jens ; Rihko-Struckmann, Liisa K. ; Batey, Darren ; Cipiccia, Silvia ; Titus, Juliane ; Poppitz, David ; Kübel, Christian ; Sundmacher, Kai ; Gläser, Roger ; Sheppard, Thomas L.
Art des Eintrags: Zweitveröffentlichung
Titel: Porosity and Structure of Hierarchically Porous Ni/Al₂O₃ Catalysts for CO₂ Methanation
Sprache: Englisch
Publikationsjahr: 15 Januar 2024
Ort: Darmstadt
Publikationsdatum der Erstveröffentlichung: 2020
Ort der Erstveröffentlichung: Basel
Verlag: MDPI
Titel der Zeitschrift, Zeitung oder Schriftenreihe: Catalysts
Jahrgang/Volume einer Zeitschrift: 10
(Heft-)Nummer: 12
Kollation: 22 Seiten
DOI: 10.26083/tuprints-00017428
URL / URN: https://tuprints.ulb.tu-darmstadt.de/17428
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Herkunft: Zweitveröffentlichung DeepGreen
Kurzbeschreibung (Abstract):

CO₂ methanation is often performed on Ni/Al₂O₃ catalysts, which can suffer from mass transport limitations and, therefore, decreased efficiency. Here we show the application of a hierarchically porous Ni/Al₂O₃ catalyst for methanation of CO₂. The material has a well-defined and connected meso- and macropore structure with a total porosity of 78%. The pore structure was thoroughly studied with conventional methods, i.e., N₂ sorption, Hg porosimetry, and He pycnometry, and advanced imaging techniques, i.e., electron tomography and ptychographic X-ray computed tomography. Tomography can quantify the pore system in a manner that is not possible using conventional porosimetry. Macrokinetic simulations were performed based on the measures obtained by porosity analysis. These show the potential benefit of enhanced mass-transfer properties of the hierarchical pore system compared to a pure mesoporous catalyst at industrially relevant conditions. Besides the investigation of the pore system, the catalyst was studied by Rietveld refinement, diffuse reflectance ultraviolet-visible (DRUV/vis) spectroscopy, and H₂-temperature programmed reduction (TPR), showing a high reduction temperature required for activation due to structural incorporation of Ni into the transition alumina. The reduced hierarchically porous Ni/Al₂O₃ catalyst is highly active in CO₂ methanation, showing comparable conversion and selectivity for CH₄ to an industrial reference catalyst.

Freie Schlagworte: methanation, carbon dioxide, hierarchical porosity, nickel, alumina, tomography, porosity analysis
Status: Verlagsversion
URN: urn:nbn:de:tuda-tuprints-174281
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This article belongs to the Special Issue Design of Heterogeneous Catalysts and Adsorbents

Sachgruppe der Dewey Dezimalklassifikatin (DDC): 500 Naturwissenschaften und Mathematik > 540 Chemie
600 Technik, Medizin, angewandte Wissenschaften > 660 Technische Chemie
Fachbereich(e)/-gebiet(e): 11 Fachbereich Material- und Geowissenschaften
11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft
11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft > In-Situ Elektronenmikroskopie
Hinterlegungsdatum: 15 Jan 2024 13:49
Letzte Änderung: 16 Jan 2024 07:22
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