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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.
- 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.