Dynamic equilibria in supported ionic liquid phase (SILP) catalysis: in situ IR spectroscopy identifies [Ru(CO)xCly]n species in water gas shift catalysis

Beitrag in einer Fachzeitschrift
(Originalarbeit)


Details zur Publikation

Autor(en): Bauer T, Stepic R, Wolf P, Kollhoff F, Karawacka W, Wick C, Haumann M, Wasserscheid P, Smith DM, Smith AS, Libuda J
Zeitschrift: Catalysis: Science and Technology
Jahr der Veröffentlichung: 2018
Band: 8
Seitenbereich: 344-357
ISSN: 2044-4753
Sprache: Englisch


Abstract


Ru-based supported ionic liquid phase (SILP) systems efficiently catalyze the low-temperature water-gas


shift reaction (WGSR). While previous studies suggest that Ru-carbonyl species play an important role in


the mechanism, detailed knowledge on the catalytically active species is still missing. To identify these carbonyl


complexes, we apply in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) in


combination with density functional theory (DFT). Investigations of an as-prepared [R(CO)3Cl2]2/


[C4C1C1Im]Cl/Al2O3 catalyst indicate splitting of the dimer induced by Cl−. Subsequently, an equilibrium between


several [R(CO)xCly]n species is established, in which the IL serves as an effectively infinite Cl− reservoir.


We find that the major species in the system freshly-prepared from [R(CO)3Cl2]2 is indeed


[R(CO)3Cl3]−. A smaller amount of [R(CO)2Cl3]− and chloride-rich species [R(CO)2Cl4]2− or [RuCOCl4]2−


are also found in the SILP. Similar Ru-carbonyl species are observed during carbonylation of RuCl3/


[C4C1C1Im]Cl/Al2O3, another potential WGSR catalyst. The response of [Ru(CO)3Cl2]2/[C4C1C1Im]Cl/Al2O3


to heating and/or CO dosing was probed in situ and the results confirm the presence of the equilibrium


proposed above.


FAU-Autoren / FAU-Herausgeber

Haumann, Marco PD Dr.
Lehrstuhl für Chemische Reaktionstechnik
Kollhoff, Fabian
Lehrstuhl für Physikalische Chemie II
Libuda, Jörg Prof. Dr.
Professur für Physikalische Chemie
Smith, Ana-Suncana Prof. Dr.
Professur für Theoretische Physik
Stepic, Robert
Professur für Theoretische Physik
Wasserscheid, Peter Prof. Dr.
Lehrstuhl für Chemische Reaktionstechnik
Wick, Christian Dr.
Professur für Theoretische Physik
Wolf, Patrick
Lehrstuhl für Chemische Reaktionstechnik


Autor(en) der externen Einrichtung(en)
Institute Ruđer Bošković


Zitierweisen

APA:
Bauer, T., Stepic, R., Wolf, P., Kollhoff, F., Karawacka, W., Wick, C.,... Libuda, J. (2018). Dynamic equilibria in supported ionic liquid phase (SILP) catalysis: in situ IR spectroscopy identifies [Ru(CO)xCly]n species in water gas shift catalysis. Catalysis: Science and Technology, 8, 344-357. https://dx.doi.org/10.1039/C7CY02199B

MLA:
Bauer, Tanja, et al. "Dynamic equilibria in supported ionic liquid phase (SILP) catalysis: in situ IR spectroscopy identifies [Ru(CO)xCly]n species in water gas shift catalysis." Catalysis: Science and Technology 8 (2018): 344-357.

BibTeX: 

Zuletzt aktualisiert 2018-25-08 um 07:08