8 research outputs found

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

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    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

    Supraparticles for Bare‐Eye H2 Indication and Monitoring: Design, Working Principle, and Molecular Mobility

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    Abstract Indicators for H2 are crucial to ensure safety standards in a green hydrogen economy. Herein, the authors report micron‐scaled indicator supraparticles for real‐time monitoring and irreversible recording of H2 gas via a rapid eye‐readable two‐step color change. They are produced via spray‐drying SiO2 nanoparticles, AuPd nanoparticles, and indicator‐dye resazurin. The resulting gas‐accessible mesoporous supraparticle framework absorbs water from humid atmospheres to create a three‐phase‐system. In the presence of H2, the color of the supraparticle switches first irreversibly from purple to pink and further reversibly to a colorless state. In situ infrared spectroscopy measurements indicate that this color change originates from the (ir)reversible H2‐induced reduction of resazurin to resorufin and hydroresorufin. Further infrared spectroscopic measurements and molecular dynamics simulations elucidate that key to achieve this functionality is an established three‐phase‐system within the supraparticles, granting molecular mobility of resazurin. Water acts as transport medium to carry resazurin molecules towards the catalytically active AuPd nanoparticles. The advantages of the supraparticles are their small dimensions, affordable and scalable production, fast response times, straightforward bare‐eye detection, and the possibility of simultaneously monitoring H2 exposure in real‐time and ex post. Therefore, H2 indicator supraparticles are an attractive safety additive for leakage detection and localization in a H2 economy

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