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

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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 [Ru(CO)3Cl2]2/[C4C1C1Im]Cl/Al2O3 catalyst indicate splitting of the dimer induced by Cl. Subsequently, an equilibrium between several [Ru(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 [Ru(CO)3Cl2]2 is indeed [Ru(CO)3Cl3]. A smaller amount of [Ru(CO)2Cl3] and chloride-rich species [Ru(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.

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

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Publication details

The article was received on 26 Oct 2017, accepted on 27 Nov 2017 and first published on 28 Nov 2017


Article type: Paper
DOI: 10.1039/C7CY02199B
Citation: Catal. Sci. Technol., 2018, Advance Article
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    Dynamic equilibria in supported ionic liquid phase (SILP) catalysis: in situ IR spectroscopy identifies [Ru(CO)xCly]n species in water gas shift catalysis

    T. Bauer, R. Stepic, P. Wolf, F. Kollhoff, W. Karawacka, C. R. Wick, M. Haumann, P. Wasserscheid, D. M. Smith, A. Smith and J. Libuda, Catal. Sci. Technol., 2018, Advance Article , DOI: 10.1039/C7CY02199B

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