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Multiscale Mechanistic Insights of Shaped Catalyst Body Formulations and Their Impact on Catalytic Properties

Authors :
Whiting, Gareth T.
Chung, Sang Ho
Stosic, Dusan
Chowdhury, Abhishek Dutta
Van Der Wal, Lars I.
Fu, Donglong
Zecevic, Jovana
Travert, Arnaud
Houben, Klaartje
Baldus, Marc
Weckhuysen, Bert M.
NMR Spectroscopy
Inorganic Chemistry and Catalysis
Sub Inorganic Chemistry and Catalysis
Sub NMR Spectroscopy
Institut de recherches sur la catalyse et l'environnement de Lyon (IRCELYON)
Université Claude Bernard Lyon 1 (UCBL)
Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Inorganic Chemistry and Catalysis, Department of Chemistry
Utrecht University [Utrecht]
Laboratoire catalyse et spectrochimie (LCS)
Centre National de la Recherche Scientifique (CNRS)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN)
Normandie Université (NU)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Université de Caen Normandie (UNICAEN)
Normandie Université (NU)
Institut de biologie et chimie des protéines [Lyon] (IBCP)
Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)
NMR Spectroscopy
Inorganic Chemistry and Catalysis
Sub Inorganic Chemistry and Catalysis
Sub NMR Spectroscopy
Source :
ACS Catalysis, ACS Catalysis, American Chemical Society, 2019, 9 (6), pp.4792-4803. ⟨10.1021/acscatal.9b00151⟩, ACS Catalysis, 9(6), 4792. American Chemical Society
Publication Year :
2019
Publisher :
HAL CCSD, 2019.

Abstract

International audience; Zeolite-based catalysts are globally employed in many industrial processes, such as in crude-oil refining and in the production of bulk chemicals. However, to be implemented in industrial reactors efficiently, zeolite powders are required to be shaped in catalyst bodies. Scale-up of zeolite catalysts into such forms comes with side effects to its overall physicochem-ical properties and to those of its constituting components. Although fundamental research into "technical" solid catalysts is scarce, binder effects have been reported to significantly impact their catalytic properties and lifetime. Given the large number of additional (in)organic components added in the formulation, it is somehow surprising to see that there is a distinct lack of research into the unintentional impact organic additives can have on the properties of the zeolite and the catalyst bodies in general. Here, we systematically prepared a series of alumina-bound zeolite ZSM-5-based catalyst bodies, with organic additives such as peptizing, plasticizing, and lubricating agents, to rationalize their impacts on the physicochemical properties of the shaped catalyst bodies. By utilizing a carefully selected arsenal of bulk and high-spatial resolution multiscale characterization techniques, as well as specifically sized bioinspired fluorescent nanoprobes to study pore accessibility, we clearly show that, although the organic additives achieve their primary function of a mechanically robust material, uncontrolled processes are taking place in parallel. We reveal that the extrusion process can lead to zeolite dealumination (from acid peptizing treatment, and localized steaming upon calcination); meso-and macropore structural rearrangement (via burning-out of organic plasticizing and lubricating agents upon calcination); and abating of known alumina binder effects (via scavenging of Al species via chelating lubricating agents), which significantly impact catalytic performance. Understanding the mechanisms behind such effects in industrial-grade catalyst formulations can lead to enhanced design of these important materials, which can improve process efficiency in a vast range of industrial catalytic reactions.

Details

Language :
English
ISSN :
21555435
Database :
OpenAIRE
Journal :
ACS Catalysis, ACS Catalysis, American Chemical Society, 2019, 9 (6), pp.4792-4803. ⟨10.1021/acscatal.9b00151⟩, ACS Catalysis, 9(6), 4792. American Chemical Society
Accession number :
edsair.doi.dedup.....73cb4e84004c15ff39525707bede1335
Full Text :
https://doi.org/10.1021/acscatal.9b00151⟩