Improving the Performance of Supported Ionic Liquid Phase Catalysts for the Ultra-Low-Temperature Water Gas Shift Reaction Using Organic Salt Additives

Wolf, Patrick; Wick, Christian R.; Mehler, Julian; Blaumeiser, Dominik; Schötz, Simon; Bauer, Tanja; Libuda, Jörg; Smith, David M.; Smith, Ana-Sunčana; Haumann, Marco (2022) Improving the Performance of Supported Ionic Liquid Phase Catalysts for the Ultra-Low-Temperature Water Gas Shift Reaction Using Organic Salt Additives. ACS Catalysis, 12 (9). pp. 5661-5672. ISSN 2155-5435

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Abstract

The water gas shift reaction (WGSR) is catalyzed by supported ionic liquid phase (SILP) systems containing homogeneous Ru complexes dissolved in ionic liquids (ILs). These systems work at very low temperatures, that is, between 120 and 160 °C, as compared to >200 °C in the conventional process. To improve the performance of this ultra-low-temperature catalysis, we investigated the influence of various additives on the catalytic activity of these SILP systems. In particular, the application of methylene blue (MB) as an additive doubled the activity. Infrared spectroscopy measurements combined with density functional theory (DFT) calculations excluded a coordinative interaction of MB with the Ru complex. In contrast, state-of-the-art theoretical calculations elucidated the catalytic effect of the additives by non-covalent interactions. In particular, the additives can significantly lower the barrier of the rate-determining step of the reaction mechanism via formation of hydrogen bonds. The theoretical predictions, thereby, showed excellent agreement with the increase of experimental activity upon variation of the hydrogen bonding moieties in the additives investigated.

Item Type:	Article
Uncontrolled Keywords:	water gas shift reaction ; supported ionic liquid phase ; ruthenium ; methylene blue ; electronic interaction
Subjects:	NATURAL SCIENCES > Physics > Condensed Matter Physics NATURAL SCIENCES > Chemistry > Physical Chemistry NATURAL SCIENCES > Interdisciplinary Natural Sciences
Divisions:	Division of Physical Chemistry
Depositing User:	Ana Sunčana Smith
Date Deposited:	05 Jul 2022 09:46
URI:	http://fulir.irb.hr/id/eprint/7452
DOI:	10.1021/acscatal.1c05979

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