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

Journal article
(Original article)


Publication Details

Author(s): Bauer T, Stepic R, Wolf P, Kollhoff F, Karawacka W, Wick C, Haumann M, Wasserscheid P, Smith DM, Smith AS, Libuda J
Journal: Catalysis: Science and Technology
Publication year: 2018
Volume: 8
Journal issue: 1
Pages range: 344-357
ISSN: 2044-4753
Language: English


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 Authors / FAU Editors

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.
Physics Underlying Life Science
Stepic, Robert
Physics Underlying Life Science
Wasserscheid, Peter Prof. Dr.
Lehrstuhl für Chemische Reaktionstechnik
Wick, Christian Dr.
Physics Underlying Life Science
Wolf, Patrick
Lehrstuhl für Chemische Reaktionstechnik


Additional Organisation
Exzellenz-Cluster Engineering of Advanced Materials


External institutions with authors

Institute Ruđer Bošković


Research Fields

D Catalytic Materials
Exzellenz-Cluster Engineering of Advanced Materials
A3 Multiscale Modeling and Simulation
Exzellenz-Cluster Engineering of Advanced Materials


How to cite

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(1), 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 8.1 (2018): 344-357.

BibTeX: 

Last updated on 2019-20-02 at 18:38