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Titel: The quantitative impact of fluid vs. solid interfaces on the catalytic performance of pickering emulsions
VerfasserIn: Stock, Sebastian
Schlander, Annika
Kempin, Maresa
Geisler, Ramsia
Stehl, Dmitrij
Spanheimer, Kai
Hondow, Nicole
Micklethwaite, Stuart
Weber, Ariane
Schomäcker, Reinhard
Drews, Anja
Gallei, Markus
von Klitzing, Regine
Sprache: Englisch
Titel: Physical chemistry, chemical physics : PCCP
Bandnummer: 23
Heft: 3
Startseite: 2355
Endseite: 2367
Verlag/Plattform: RSC
Erscheinungsjahr: 2020
DDC-Sachgruppe: 540 Chemie
Dokumenttyp: Journalartikel / Zeitschriftenartikel
Abstract: Pickering emulsions (PEs), i.e. particle stabilized emulsions, are used as reaction environments in biphasic catalysis for the hydroformylation of 1-dodecene into tridecanal using the catalyst rhodium (Rh)-sulfoxantphos (SX). The present study connects the knowledge about particle-catalyst interactions and PE structure with the reaction results. It quantifies the efficiency of the catalytic performance of the catalyst localized in the voids between the particles (liquid-liquid interface) and the catalyst adsorbed on the particle surface (liquid-solid interface) using a new numerical approach. First, it is ensured that the overall packing density and geometry at the droplet interface and the size of the water droplets of the resulting w/o PEs are predictable. Second, it is shown that approximately all particles assemble at the droplet surface after emulsion preparation and neither the packing parameter nor the droplet size change with the particle surface charge or size when the total particle cross section is kept constant. Third, studies on the influence of the catalyst on the emulsion structure reveal that irrespective of the particle charge the surface active and negatively charged catalyst Rh-SX reduces the PE droplet size significantly and decreases the particle packing parameter from s = 0.91 (hexagonal packing in 2D) to s = 0.69 (shattered structure). In this latter case, large voids of the free w/o interface form and become covered with the catalyst. With a deep knowledge about the PE structure the reaction efficiencies of the liquid-liquid vs. the solid-liquid interface are quantified. By excluding any other influence factors, it is shown that the activity of the catalyst is the same at the fluid and solid interface and the performance of the reaction is explained by the geometry of the system. After the reaction, the catalyst retention via membrane filtration is shown to be successfully achieved without damaging the emulsions. This enables the continuous recovery of the catalyst, i.e. the most expensive compound in PE-based catalytic reactions, being a crucial criterion for industrial applications.
DOI der Erstveröffentlichung: 10.1039/d0cp06030e
URL der Erstveröffentlichung: https://pubs.rsc.org/en/content/articlelanding/2021/cp/d0cp06030e
Link zu diesem Datensatz: urn:nbn:de:bsz:291--ds-371172
hdl:20.500.11880/33691
http://dx.doi.org/10.22028/D291-37117
ISSN: 1463-9084
1463-9076
Datum des Eintrags: 30-Aug-2022
Fakultät: NT - Naturwissenschaftlich- Technische Fakultät
Fachrichtung: NT - Chemie
Professur: NT - Prof. Dr. Markus Gallei
Sammlung:SciDok - Der Wissenschaftsserver der Universität des Saarlandes

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