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- ItemAn amino acid based system for CO2 capture and catalytic utilization to produce formates(Cambridge : RSC, 2021) Wei, Duo; Junge, Henrik; Beller, MatthiasHerein, we report a novel amino acid based reaction system for CO2 capture and utilization (CCU) to produce formates in the presence of the naturally occurring amino acid l-lysine. Utilizing a specific ruthenium-based catalyst system, hydrogenation of absorbed carbon dioxide occurs with high activity and excellent productivity. Noteworthy, following the CCU concept, CO2 can be captured from ambient air in the form of carbamates and converted directly to formates in one-pot (TON > 50 000). This protocol opens new potential for transforming captured CO2 from ambient air to C1-related products. © 2021 The Royal Society of Chemistry.
- ItemEfficient Synthesis of Novel Plasticizers by Direct Palladium-Catalyzed Di- or Multi-carbonylations(Weinheim : Wiley-VCH, 2022) Hu, Yuya; Sang, Rui; Vroemans, Robby; Mollaert, Guillaume; Razzaq, Rauf; Neumann, Helfried; Junge, Henrik; Franke, Robert; Jackstell, Ralf; Maes, Bert U. W.; Beller, MatthiasDiesters are of fundamental importance in the chemical industry and are used for many applications, e.g. as plasticizers, surfactants, emulsifiers, and lubricants. Herein, we present a straightforward and efficient method for the selective synthesis of diesters via palladium-catalyzed direct carbonylation of di- or polyols with readily available alkenes. Key-to-success is the use of a specific palladium catalyst with the “built-in-base” ligand L16 providing esterification of all alcohols and a high n/iso ratio. The synthesized diesters were evaluated as potential plasticizers in PVC films by measuring the glass transition temperature (Tg) via differential scanning calorimetry (DSC).
- ItemSite-Selective Real-Time Observation of Bimolecular Electron Transfer in a Photocatalytic System Using L-Edge X-Ray Absorption Spectroscopy(Weinheim : Wiley-VCH Verl., 2021) Britz, Alexander; Bokarev, Sergey I.; Assefa, Tadesse A.; Bajnóczi, Èva G.; Németh, Zoltán; Vankó, György; Rockstroh, Nils; Junge, Henrik; Beller, Matthias; Doumy, Gilles; March, Anne Marie; Southworth, Stephen H.; Lochbrunner, Stefan; Kühn, Oliver; Bressler, Christian; Gawelda, WojciechTime-resolved X-ray absorption spectroscopy has been utilized to monitor the bimolecular electron transfer in a photocatalytic water splitting system. This has been possible by uniting the local probe and element specific character of X-ray transitions with insights from high-level ab initio calculations. The specific target has been a heteroleptic [IrIII (ppy)2 (bpy)]+ photosensitizer, in combination with triethylamine as a sacrificial reductant and Fe3(CO)12 as a water reduction catalyst. The relevant molecular transitions have been characterized via high-resolution Ir L-edge X-ray absorption spectroscopy on the picosecond time scale and restricted active space self-consistent field calculations. The presented methods and results will enhance our understanding of functionally relevant bimolecular electron transfer reactions and thus will pave the road to rational optimization of photocatalytic performance.