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- ItemHighly active and selective photochemical reduction of CO2 to CO using molecular-defined cyclopentadienone iron complexes(Cambridge : Soc., 2015) Rosas-Hernández, Alonso; Alsabeh, Pamela G.; Barsch, Enrico; Junge, Hernrik; Ludwig, Ralf; Beller, MatthiasHerein, we report highly active (cyclopentadienone)iron–tricarbonyl complexes for CO2 photoreduction using visible light with an Ir complex as photosensitizer and TEOA as electron/proton donor. Turnover numbers (TON) of ca. 600 (1 h) with initial turnover frequencies (TOF) up to 22.2 min−1 were observed. Operando FTIR measurements allowed for the proposal of a plausible mechanism for catalyst activation.
- ItemTowards a methanol economy based on homogeneous catalysis: methanol to H2 and CO2 to methanol(Cambridge : Soc., 2015) Alberico, E.; Nielsen, M.The possibility to implement both the exhaustive dehydrogenation of aqueous methanol to hydrogen and CO2 and the reverse reaction, the hydrogenation of CO2 to methanol and water, may pave the way to a methanol based economy as part of a promising renewable energy system. Recently, homogeneous catalytic systems have been reported which are able to promote either one or the other of the two reactions under mild conditions. Here, we review and discuss these developments.
- ItemHighly selective visible light-induced Ti–O bond splitting in an ansa-titanocene dihydroxido complex(Cambridge : Soc., 2015) Godemann, Christian; Dura, Laura; Hollmann, Dirk; Grabow, Kathleen; Bentrup, Ursula; Jiao, Haijun; Schulz, Axel; Brückner, Angelika; Beweries, TorstenIrradiation of a substituted ansa-titanocene(IV) dihydroxido complex with visible light induces Ti–O bond dissociation. In contrast to previous studies on structurally similar unbridged complexes, no side reactions are observed and formation of the Ti(III) species is highly selective. The formation of OH radicals was proved using a biradicaloid species.
- ItemCorrection: A flow cytometer-based whole cell screening toolbox for directed hydrolase evolution through fluorescent hydrogels(Cambridge : Soc., 2015) Lülsdorf, Nina; Pitzler, Christian; Biggel, Michael; Martinez, Ronny; Vojcic, Ljubica; Schwaneberg, UlrichCorrection for ‘A flow cytometer-based whole cell screening toolbox for directed hydrolase evolution through fluorescent hydrogels’ by Nina Lülsdorf et al., Chem. Commun., 2015, 51, 8679–8682.
- ItemA neutral low-coordinate heterocyclic bismuth-tin species(Cambridge : Soc., 2015) Hering-Junghans, C.; Schulz, A.; Villinger, A.The reaction of distannadiazane bearing bulky RAr*-groups (RAr* = C6H2{C(H)Ph2}2R-2,6,4; R = iPr, tBu) with ECl3 (E = Sb, Bi) was studied resulting in the isolation of previously unknown N,N-bis(dichloropnictino)amines (3) and a novel heterocyclic carbenoid bismuth species (4) bearing a Bi(III) and a Sn(IV) center. The structure and bonding was investigated by means of X-ray structure elucidations and DFT calculations.
- ItemAccessing heavy allyl-analogous [(TerN)2E]− (E = Sb, Bi) ions and their reactivity towards ECl3(Cambridge : Soc., 2015) Hinz, Alexander; Schulz, Axel; Villinger, AlexanderThe attempted preparation of the biradicaloid [E(μ-NTer)]2 (E = Sb, Bi) yielded salts of the anion [(TerN)2E]−. These heteroatom allyl analogues could be further utilized in the reaction with pnictogen(III) chlorides to form the first 1,3-dichloro-1-bisma-3-stiba-2,4-diazane [ClSb(μ-NTer)2BiCl].
- ItemEnantio- and diastereoselective synthesis of γ-amino alcohols(Cambridge : Soc., 2015) Verkade, Jorge M. M.; Quaedflieg, Peter J. L. M.; Verzijl, Gerard K. M.; Lefort, Laurent; van Delft, Floris L.; de Vries, Johannes G.; Rutjes, Floris P. J. T.The γ-amino alcohol structural motif is often encountered in drugs and natural products. We developed two complementary catalytic diastereoselective methods for the synthesis of N-PMP-protected γ-amino alcohols from the corresponding ketones. The anti-products were obtained through Ir-catalyzed asymmetric transfer hydrogenation, the syn-products via Rh-catalyzed asymmetric hydrogenation.
- ItemSingle molecule level plasmonic catalysis – a dilution study of p-nitrothiophenol on gold dimers(Cambridge : Soc., 2015) Zhang, Zhenglong; Deckert-Gaudig, Tanja; Singh, Pushkar; Deckert, VolkerSurface plasmons on isolated gold dimers can initiate intermolecular reactions of adsorbed p-nitrothiophenol. At the single molecule level when dimerization is not possible an intramolecular reaction can be observed. Experimental evidence indicates that plasmon-induced hot electrons provide the required activation energy.
- ItemNickel cobalt oxide hollow nanosponges as advanced electrocatalysts for the oxygen evolution reaction(Cambridge : Soc., 2015) Zhu, Chengzhou; Wen, Dan; Leubner, Susanne; Oschatz, Martin; Liu, Wei; Holzschuh, Matthias; Simon, Frank; Kaskel, Stefan; Eychmüller, AlexanderA class of novel nickel cobalt oxide hollow nanosponges were synthesized through a sodium borohydride reduction strategy. Due to their porous and hollow nanostructures, and synergetic effects between their components, the optimized nickel cobalt oxide nanosponges exhibited excellent catalytic activity towards oxygen evolution reaction.
- ItemLabel-free monitoring of plasmonic catalysis on the nanoscale(Cambridge : Soc., 2015) Zhang, Zhenglong; Deckert-Gaudig, Tanja; Deckert, VolkerPlasmonics is the description of specific light matter interactions of metallic structures. In general the size of such structures is well in the nanometer regime and also determines such specific characteristics as color, field confinement etc. Plasmon-induced hot electrons play a vital role in so-called plasmonic catalysis, a field that has recently attracted attention as a new reaction platform. Current reports introduce such nanoscale catalysis as an effective approach to concentrate the energy of visible light and direct it to adsorbed molecules, thereby increasing the chemical reaction rate, and controlling the reaction selectivity. In this review, we present various plasmon-catalyzed reactions specifically monitored with Raman spectroscopy, namely surface-enhanced Raman scattering (SERS), remote SERS (Re-SERS) and tip-enhanced Raman scattering (TERS). These techniques utilize the signal enhancing effect of the metal nanoparticles. However, at the same time they can be used to control the actual reactivity. In the first part, the mechanism of plasmonic catalysis is introduced. Then it is shown how catalytic reactions can be spectroscopically investigated far beyond the diffraction limit using TERS. Finally, the sensitivity of the methods is discussed.