Multiscale Mechanistic Insights of Shaped Catalyst Body Formulations and Their Impact on Catalytic Properties - Archive ouverte HAL
Article Dans Une Revue ACS Catalysis Année : 2019

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

Gareth T Whiting
  • Fonction : Auteur
Sang-Ho Chung
  • Fonction : Auteur
Abhishek Dutta Chowdhury
  • Fonction : Auteur
Lars I van Der Wal
  • Fonction : Auteur
Donglong Fu
  • Fonction : Auteur
Arnaud Travert
Klaartje Houben
  • Fonction : Auteur
Bert M Weckhuysen
  • Fonction : Auteur
Abhishek Dutta Chowdhury
  • Fonction : Auteur

Résumé

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.

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Catalyse
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hal-02160853 , version 1 (20-06-2019)

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Gareth T Whiting, Sang-Ho Chung, Dusan Stosic, Abhishek Dutta Chowdhury, Lars I van Der Wal, et al.. Multiscale Mechanistic Insights of Shaped Catalyst Body Formulations and Their Impact on Catalytic Properties. ACS Catalysis, 2019, 9 (6), pp.4792-4803. ⟨10.1021/acscatal.9b00151⟩. ⟨hal-02160853⟩
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