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- ItemManganese-catalyzed selective C–H activation and deuteration by means of a catalytic transient directing group strategy(London : Royal Society of Chemistry (RSC), 2021) Kopf, Sara; Neumann, Helfried; Beller, MatthiasA novel manganese-catalyzed C-H activation methodology for selective hydrogen isotope exchange of benzaldehydes is presented. Using D2O as a cheap and convenient source of deuterium, the reaction proceeds with excellent functional group tolerance. Highortho-selectivity is achieved in the presence of catalytic amounts of specific amines, whichin situform a transient directing group. © The Royal Society of Chemistry 2021.
- ItemSelective Earth-Abundant System for CO2 Reduction: Comparing Photo- and Electrocatalytic Processes(Washington, DC : American Chemical Society, 2019) Steinlechner C.; Roesel A.F.; Oberem E.; Päpcke A.; Rockstroh N.; Gloaguen F.; Lochbrunner S.; Ludwig R.; Spannenberg A.; Junge H.; Francke R.; Beller M.The valorization of CO2 via photo- or electrocatalytic reduction constitutes a promising approach toward the sustainable production of fuels or value-added chemicals using intermittent renewable energy sources. For this purpose, molecular catalysts are generally studied independently with respect to the photo- or the electrochemical application, although a unifying approach would be much more effective with respect to the mechanistic understanding and the catalyst optimization. In this context, we present a combined photo- and electrocatalytic study of three Mn diimine catalysts, which demonstrates the synergistic interplay between the two methods. The photochemical part of our study involves the development of a catalytic system containing a heteroleptic Cu photosensitizer and the sacrificial BIH reagent. The system shows exclusive selectivity for CO generation and renders turnover numbers which are among the highest reported thus far within the group of fully earth-abundant photocatalytic systems. The electrochemical part of our investigations complements the mechanistic understanding of the photochemical process and demonstrates that in the present case the sacrificial reagent, the photosensitizer, and the irradiation source can be replaced by the electrode and a weak Brønsted acid. © 2019 American Chemical Society.
- ItemElectronic transitions and dielectric function tensor of a YMnO3 single crystal in the NIR-VUV spectral range(London [u.a.] : Royal Society of Chemistry, 2014) Schmidt-Grund, R.; Richter, S.; Ebbinghaus, S.G.; Lorenz, M.; Bundesmann, C.; Grundmann, M.We present optical properties in the near-infrared to vacuum-ultraviolet spectral range of hexagonal YMnO3. The high-quality (110)-oriented bulk single crystal was grown by the optical floating zone technique. We have determined the tensor of the dielectric function by means of Mueller matrix ellipsometry in the wide spectral range (0.5-9.15) eV. For the spectral range below 5.4 eV, we present much more precise data compared to previous reports. For higher energies no experimental reports were given previously. The experimental dielectric function of YMnO3 agrees generally with theoretical calculations. We found the well known transitions involving hybridized oxygen-Mn states and Mn-3d states to be spectrally localized with a homogeneous Lorentzian lineshape. At energies above these transitions, we observe pseudo-transparent points where for each of the principal diagonal elements of the dielectric function tensor the imaginary part approaches zero but at different photon energies. These are followed at the onset of the high-absorption spectral range by parabolic direct band-band transitions which have not been reported so far.