Roland A. Fischer

Nanjing University of Technology, Nan-ching, Jiangsu Sheng, China

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Publications (429)2253.97 Total impact

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    ABSTRACT: Copper(II) oxide thin films were grown by atomic layer deposition (ALD) using bis-(dimethylamino-2-propoxide)copper [Cu(dmap)2] and ozone in a temperature window of 80-140 °C. A thorough characterization of the films was performed using x-ray diffraction, x-ray reflectivity, UV Vis spectrophotometry, atomic force microscopy, field emission scanning electron microscopy, x-ray photoelectron spectroscopy, and time-of-flight elastic recoil detection analysis techniques. The process was found to produce polycrystalline copper(II) oxide films with a growth rate of 0.2-0.3 Å per cycle. Impurity content in the films was relatively small for a low temperature ALD process.
    Journal of Vacuum Science & Technology A Vacuum Surfaces and Films 01/2016; 34(1). DOI:10.1116/1.4933089 · 2.32 Impact Factor
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    ABSTRACT: A variety of strategies have been developed to adsorb and separate light hydrocarbons in metal-organic frameworks. Here, we present a new approach in which the pores of a framework are lined with four different C3 sidechains that feature various degrees of branching and saturation. These pendant groups, which essentially mimic a low-density solvent with restricted degrees of freedom, offer tunable control of dispersive host-guest interactions. The performance of a series of frameworks of the type Zn2 (fu-bdc)2 (dabco) (fu-bdc(2-) =functionalized 1,4-benzenedicarboxylate; dabco=1,4-diazabicyclo[2.2.2]octane), which feature a pillared layer structure, were investigated for the adsorption and separation of methane, ethane, ethylene, and acetylene. The four frameworks exhibit low methane uptake, whereas C2 hydrocarbon uptake is substantially higher as a result of the enhanced interaction of these molecules with the ligand sidechains. Most significantly, the adsorption quantities and selectivity were found to depend strongly upon the type of sidechains attached to the framework scaffold.
    Chemistry - A European Journal 11/2015; DOI:10.1002/chem.201503685 · 5.73 Impact Factor
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    ABSTRACT: Flexible metal-organic frameworks (MOFs) can undergo fascinating structural transitions triggered by external stimuli, such as adsorption/desorption of specific guest molecules or temperature changes. In this detailed study we investigate the potentials and limitations of tuning framework flexibility systematically by exploiting the powerful concept of mixed-linker solid solutions. We chose the prototypical family of functionalized pillared-layer MOFs of the general type Zn2(fu(1)-bdc)2x(fu(2)-bdc)2-2xdabco (with x = 1.00, 0.75, 0.50, 0.25 and 0.00; fu-bdc = 2,5-dialkoxy-1,4-benzenedicarboxylate with varying alkoxy chain length, dabco = 1,4-diazabicyclo[2.2.2]octane) and examined their guest responsive, as well as intrinsic temperature dependent structural flexibility by X-ray diffraction, gas physisorption and calorimetric measurements. The ratio of the different fu-bdc linkers can be adjusted freely, offering opportunity for a targeted design of these functional materials by modulating their key features, such as magnitude of framework contraction upon guest removal, breathing behaviour upon CO2 adsorption/desorption, thermoresponsive phase behaviour, and their general thermal expansivity, by the careful choice of fu-bdc linkers and their combination.
    Dalton Transactions 11/2015; DOI:10.1039/c5dt03825a · 4.20 Impact Factor
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    ABSTRACT: Titania exhibits unique photophysical and -chemical properties and can be used for potential applications in the field of photocatalysis. The control of TiO2 in terms of phase, shape, morphology, and especially nanoscale synthesis of TiO2 particles still remains a challenge. Ti-containing metal-organic frameworks (MOFs), such as MIL-125, can be used as sacrificial precursors to obtain TiO2 materials with diverse phase compositions, morphologies, sizes, and surface areas. MIL-125 is composed of Ti/O clusters as the secondary building units (SBUs) bridged by 1,4-benzenedicarboxylate (bdc). In this study, preformed and surfactant-stabilized gold nanoparticles (GNPs) were deposited onto the surface of amino functionalized NH2-MIL-125 during solvothermal synthesis. Targeted gold/titania nanocomposites, GNP/TiO2, were fabricated through the pyrolysis of GNP/NH2-MIL-125 nanocrystals. The modification of TiO2 with GNPs significantly increased the photocatalytic activity of the MOF derived TiO2 material for the reduction of CO2 to CH4 as compared to TiO2 reference samples such as P-25 and AUROlite (Au/TiO2). The new materials GNP/TiO2 and TiO2 derived by the MOF precursor route were thoroughly characterized by PXRD, FTIR and Raman, TEM, and N2 adsorption studies.
    Chemistry of Materials 10/2015; 27(21):151019122835009. DOI:10.1021/acs.chemmater.5b03017 · 8.35 Impact Factor
  • Jiyeon Kim · Markus Halbherr · Christian Gemel · Roland A Fischer ·
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    ABSTRACT: Uncommon Ni(I) cationic complexes were synthesized by treating [Ni(ECp*)2(PPh3)2] (E = Al, Ga; Cp* = pentamethylcyclopentadienyl) with 1 equiv of [FeCp2][BAr4(F)]. All compounds have been prepared readily in high yield. The paramagnetic compounds were characterized by single-crystal X-ray crystallography, mass spectrometry, elemental analysis, magnetic susceptibility, and electron paramagnetic resonance spectroscopy.
    Inorganic Chemistry 10/2015; 54(20). DOI:10.1021/acs.inorgchem.5b01215 · 4.76 Impact Factor
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    ABSTRACT: Nanostructure engineering has been demonstrated to improve the electrochemical performance of iron oxide based electrodes in Li-ion batteries (LIBs). However, the synthesis of advanced functional materials often requires multiple steps. Herein, we present a facile one-pot synthesis of carbon-coated nanostructured iron oxide on few-layer graphene through high-pressure pyrolysis of ferrocene in the presence of pristine graphene. The ferrocene precursor supplies both iron and carbon to form the carbon-coated iron oxide, while the graphene acts as a high-surface-area anchor to achieve small metal oxide nanoparticles. When evaluated as a negative-electrode material for LIBs, our composite showed improved electrochemical performance compared to commercial iron oxide nanopowders, especially at fast charge/discharge rates.
    Chemistry - A European Journal 09/2015; 21(45). DOI:10.1002/chem.201501935 · 5.73 Impact Factor
  • Zhenlan Fang · Bart Bueken · Dirk E. De Vos · Roland A. Fischer ·
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    ABSTRACT: Review: overview of defects in coordination network compounds (CNCs) (including their classification and characterizations) and applications of defective CNCs/MOFs; 133 refs.
    ChemInform 08/2015; 46(31). DOI:10.1002/chin.201531257
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    ABSTRACT: A controlled secondary building unit approach (CSA) was employed to obtain a series of ruthenium metal-organic frameworks (MOFs) of the general formula [Ru3(BTC)2Xx]·Gg (BTC = 1,3,5-benzenetricarboxylate; X = counter-anion, G = guest molecules) which are structural analogues of [M3(BTC)2] (M = Cu, Zn, Ni, Cr, Mo). The compounds [Ru2(OOCR)4X] and [Ru2(OOCCH3)4]Y were varied as Ru sources for CSA; namely strong coordinating X (Cl–) and weakly coordinating Y ([BF4]– or [BPh4]–) as well as the alkyl groups at the carboxylate ligand [R = CH3 or C(CH3)3] were utilized. Four phase-pure Ru-MOFs were obtained: [Ru3(BTC)2Cl0.5(OH)]·(AcOH)1.5 (1), [Ru3(BTC)2Cl1.2(OH)0.3]·(H3BTC)0.15(AcOH)2.4(PivOH)0.45 (2), [Ru3(BTC)2F0.5(OH)]·(AcOH)1.0 (3) and [Ru3(BTC)2(OH)1.5]·(H3BTC)0.5·(AcOH)1.4 (4) {AcOH = CH3COOH, PivOH = (CH3)3CCOOH}. The series of characterization data support the analytical composition and isostructural nature of 1–4, i.e. powder X-ray diffraction (PXRD), IR- and 1H-NMR spectroscopy, thermal gravimetric analysis (TGA) and N2 sorption were employed. The valence state of the Ru-sites were studied by X-ray absorption spectroscopy (XAS). The chosen precursors for CSA and optimized synthesis, work-up and activation protocols allowed improvement of the overall crystallinity, purity (i.e., residual solvent molecules) and surface area of the Ru-MOF materials.
    Berichte der deutschen chemischen Gesellschaft 07/2015; 2015(23). DOI:10.1002/ejic.201500478 · 2.94 Impact Factor
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    ABSTRACT: Host-guest inclusion properties of UiO-66 and UiO-67 metal-organic frameworks have been studied using ferrocene (FeCp2) as probe molecule. According to variable-temperature solid-state 1H and 13C CP-MAS-NMR, two different environments exist for adsorbed FeCp2 inside UiO-66 and UiO-67, which have been assigned to octahedral and tetrahedral cavities. At room temperature, a rapid exchange between these two adsorption sites occurs in UiO-67, while at –80 °C the intracrystalline traffic of FeCp2 through the triangular windows is largely hindered. In UiO-66, FeCp2 diffusion is already impeded at room temperature, in agreement with the smaller pore windows. Palladium nanoparticles (Pd NPs) encapsulated inside UiO-66 and UiO-67 have been prepared by chemical vapor infiltration of (allyl)Pd(Cp) followed by UV light irradiation. Infiltration must be carried out at low temperature (–10 °C) to avoid uncontrolled decomposition of the organometallic precursor and formation of Pd NPs at the external surface of the MOF. The resulting Pd-MOFs are shape selective catalysts, as shown for the hydrogenation of carbonyl compounds with different steric hindrance.
    Berichte der deutschen chemischen Gesellschaft 07/2015; 2015(23). DOI:10.1002/ejic.201500299 · 2.94 Impact Factor
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    ABSTRACT: Copper sulfide nanocrystals (Cu2-xS NCs) consisting of earth-abundant and nontoxic elements have attracted attention for optoelectronic and plasmonic applications due to their tunable light absorption and emission properties. In this work, we present a study of the electronic changes induced in organic-capped Cu2-xS NCs by surface modification treatments using charge transport and optical spectroscopy measurements. We have investigated surface treatments yielding ligand exchange and also ligand removal as well as changes in electronic defect density. The structural and morphological changes induced by the treatments were monitored by infrared spectroscopy, electron microscopy, and electron paramagnetic resonance. Untreated Cu2-xS NCs exhibit a strong absorption band arising from a localized surface plasmon resonance (LSPR). We found that using a ligand exchange procedure (ethanedithiol treatment), the electrical conductivity in films of Cu2-xS NCs can be enhanced by 5 orders of magnitude, while maintaining other electronic properties of the individual NCs like optical absorption and LSPR. The improvements in the electrical conductivity were attributed to the reduction of the inter-NC separation in the films, as revealed by the structural and morphological studies. We also have observed that ligand removal treatments such as thermal annealing and hydrazine treatment yield a LSPR red-shift, while the electrical conductivity increases by up to 5 and 7 orders of magnitude, respectively. We proposed a model for the surface reactions taking place during these treatments. Our work highlights the potential of simple chemical or thermal treatments in tailoring the electronic properties of Cu2-xS NCs, making thermally treated Cu2-xS NCs interesting for tunable plasmonic and optoelectronic applications.
    The Journal of Physical Chemistry C 07/2015; 119(28-28):16276-16285. DOI:10.1021/acs.jpcc.5b01078 · 4.77 Impact Factor
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    Zhenlan Fang · Bart Bueken · Dirk E. De Vos · Roland A. Fischer ·
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    ABSTRACT: Defect engineering in metal-organic frameworks (MOFs) is an exciting concept for tailoring material properties, which opens up novel opportunities not only in sorption and catalysis, but also in controlling more challenging physical characteristics such as band gap as well as magnetic and electrical/conductive properties. It is challenging to structurally characterize the inherent or intentionally created defects of various types, and there have so far been few efforts to comprehensively discuss these issues. Based on selected reports spanning the last decades, this Review closes that gap by providing both a concise overview of defects in MOFs, or more broadly coordination network compounds (CNCs), including their classification and characterization, together with the (potential) applications of defective CNCs/MOFs. Moreover, we will highlight important aspects of "defect-engineering" concepts applied for CNCs, also in comparison with relevant solid materials such as zeolites or COFs. Finally, we discuss the future potential of defect-engineered CNCs. © 2015 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the Creative Commons Attribution Non-Commercial NoDerivs License, which permits use and distribution in any medium, provided the original work is properly cited, the use is non-commercial and no modifications or adaptations are made.
    Angewandte Chemie International Edition 06/2015; 54(25). DOI:10.1002/anie.201411540 · 11.26 Impact Factor
  • Zhenlan Fang · Bart Bueken · Dirk E. De Vos · Roland A. Fischer ·
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    ABSTRACT: Die gezielte Manipulation Metall-organischer Gerüste (MOFs) ist ein interessantes Konzept zur Entwicklung maßgeschneiderter Materialeigenschaften, das nicht nur in den Gebieten der Sorption und Katalyse neue Möglichkeiten schafft, sondern auch bei der Kontrolle anspruchsvollerer physikalischer Merkmale wie der Bandlücke sowie magnetischer und elektrischer Eigenschaften. Bisher gab es wenig Bemühungen, die intrinsischen oder absichtlich geschaffenen Defekte verschiedenster Art zu charakterisieren. Basierend auf Veröffentlichungen aus den letzten Jahrzehnten schließt dieser Aufsatz die Lücke, indem er einen prägnanten Überblick über Defekte in MOFs, oder weiter gefasst in Koordinationsnetzwerk-Verbindungen (CNCs), gibt und deren Klassifikation und Charakterisierung sowie (mögliche) Anwendungen der defekthaltigen CNCs/MOFs einschließt. Außerdem werden wir wichtige Aspekte des Konzepts der “Defektmanipulation” in Anwendung an CNCs hervorheben, auch in Gegenüberstellung mit relevanten Feststoffen wie Zeolithen oder kovalenten organischen Gerüsten (COFs). Zuletzt werden wir das Potenzial der defektmanipulierten CNCs für die Zukunft diskutieren.
    Angewandte Chemie 06/2015; 127(25). DOI:10.1002/ange.201411540
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    Min Tu · Suttipong Wannapaiboon · Kira Khaletskaya · Roland A. Fischer ·
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    ABSTRACT: Thin films of sodalite-type zeolitic-imidazolate frameworks (ZIFs, ZIF-7, 8, 9, 67, 90, and ZIF-65-Zn) with different metal centers and functional moieties are fabricated on SiO2 coated quartz crystal microbalance (QCM) substrates using automatic program controlled repeated direct growth method. The repeated direct growth procedure manipulated here shows great applicability for rapid growth of uniform ZIF thin films with controllable thickness. The fabricated ZIF/QCM devices are used to detect vapor phase volatile organic compounds including alcohol/water, BTEX compounds (benzene, toluene, ethylbenzene and xylene isomers), and hexane isomers. The ZIF/QCM devices exhibit selective detection behavior upon exposure to these chemical vapors. The effects of ZIF pore size, limited pore diameter, surface functionality, and structural flexibility on the sensing performances of ZIF/QCM devices are systematically investigated, which would be beneficial for the practical application of ZIF sensors based on array-sensing technology. Furthermore, the selective adsorption behavior suggests that these ZIF materials have great potentials in the applications of biofuel recovery and the separation of benzene/cyclohexane, xylene, and hexane isomers.
    Advanced Functional Materials 06/2015; 25(28):n/a-n/a. DOI:10.1002/adfm.201500760 · 11.81 Impact Factor
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    ABSTRACT: A new titanium precursor, [Ti(OPri)2(deacam)2] (deacam = N,N-diethylacetoacetamide), was developed by the reaction of the parent Ti alkoxide with the β-ketoamide. The compound, obtained as a monomeric six-coordinated complex, was used in metal organic chemical vapor deposition (MOCVD) of TiO2 both as a single source precursor (SSP) and in the presence of oxygen. The high thermal stability of [Ti(OPri)2(deacam)2] enabled the fabrication of TiO2 films over a wide temperature range, with steady growth rates between 500 and 800 °C. The microstructure of the obtained systems was analyzed by X-ray diffraction (XRD) and Raman spectroscopy, whereas atomic force microscopy (AFM) and field emission-scanning electron microscopy (FE-SEM) measurements were performed to investigate the surface morphology and nanoorganization. Film composition was investigated by complementary techniques like Rutherford backscattering spectrometry (RBS), nuclear reaction analysis (NRA), X-ray photoelectron spectroscopy (XPS), and secondary ion mass spectrometry (SIMS). The electrical properties of the layers were investigated by performing capacitance voltage (C–V) and leakage current measurements.
    Physica Status Solidi (A) Applications and Materials 05/2015; 212(7). DOI:10.1002/pssa.201532271 · 1.62 Impact Factor
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    ABSTRACT: Porosity switching in the crystalline solid state is a unique phenomenon observed only in a limited number of materials. The switching behavior of two metal-organic frameworks as well as their respective solid solutions of composition [Zn2(BME-bdc)x(DB-bdc)2-xdabco]n (x = 2; 1.5; 1.0; 0.5; 0) is studied in situ during the adsorption of CO2 and Xe using X-ray diffraction and NMR techniques. The diffraction data, measured during the adsorption suggest a direct one-step phase transition (switching) from the narrow pore phase to the large pore phase beyond the transition pressure. An intermediate phase was found only in one compound within a narrow pressure range around the phase transition pressure region. In situ high-pressure 13C NMR spectroscopy of adsorbed CO2 also allowed following the gating behavior of the studied materials by monitoring the signal of adsorbed CO2. The 13C NMR spectra exhibit a pronounced broadening indicating a certain degree of order for the adsorbed molecules inside the pores. This ordering effect and the resulting line broadening depend on the linker functionalization as could be confirmed by corresponding molecular dynamics (MD) simulations.
    Microporous and Mesoporous Materials 03/2015; DOI:10.1016/j.micromeso.2015.02.042 · 3.45 Impact Factor
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    Lars Heinke · Min Tu · Suttipong Wannapaiboon · Roland A. Fischer · Christof Wöll ·
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    ABSTRACT: Thin films of metal-organic frameworks (MOFs) enable various applications ranging from membrane separations over sensor techniques to potential (micro-) electronic uses. Recent progresses of thin and homogenous surface-mounted MOF (SURMOF) films, which are prepared in a well-defined layer-by-layer fashion on a solid substrate surface, are highlighted in this review. Various substrate surfaces, ranging from plain metal, metal-oxide and polymer surfaces over metal-oxide membranes to magnetic nanoparticles, can be coated with SURMOFs. Multilayered SURMOF films with either identical or different MOF lattice constants or even different MOF structures were prepared, enabling the preparation of functional surface coatings. This allows, by incorporating photoswitchable azobenzene in the MOF structure, the preparation of multilayered, nanoporous films with remote-controllable properties. By means of crosslinking the SURMOF structure employing post-synthetic modifications, water stable thin films, SURGELs, can be prepared. Their thin and homogenous morphology also makes SURMOFs perfectly suited as coatings for electrochemical and electronic applications, where the small dielectric constant k as well as the option to tune the conductivity by loading the pores are very promising features of these porous solids. Furthermore, SURMOFs are very well suited for investigations of MOF-specific properties, since e.g. photoelectron spectroscopies can be applied to these thin films in a straightforward fashion. In additions, mass transfer and diffusion properties in MOFs can be studied for such thin films with high precision using a quartz-crystal microbalance (QCM).
    Microporous and Mesoporous Materials 03/2015; 46(38). DOI:10.1016/j.micromeso.2015.03.018 · 3.45 Impact Factor
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    ABSTRACT: Die dreieckigen Cluster [Zn3Cp*3]+ und [Zn2CuCp*3] wurden durch Addition der in situ generierten, elektrophilen und isolobalen Spezies [ZnCp*]+ und [CuCp*] an das Carmona-Reagens [Cp*ZnZnCp*] synthetisiert, wobei die Zn-Zn-Bindung des Letzteren erhalten blieb. Die Verwendung von nichtkoordinierenden fluorierten aromatischen Lösungsmitteln ist dabei essenziell. Die Bindungssituation der ligandenstabilisierten Cluster wurde mit quantenchemischen Methoden untersucht, wobei sich ein hohes Maß an σ-Aromatizität zeigte, ähnlich der Bindungssituation im Triwasserstoffkation [H3]+. Die neuen Spezies dienen als molekulare Bausteine für CunZnm-Cluster (Nanomessing), die auch im LIFDI-Massenspektrum der neuen Verbindungen detektiert werden können.
    Angewandte Chemie 02/2015; 127(14). DOI:10.1002/ange.201410737
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    ABSTRACT: The triangular clusters [Zn3 Cp*3 ](+) and [Zn2 CuCp*3 ] were obtained by addition of the in situ generated, electrophilic, and isolobal species [ZnCp*](+) and [CuCp*] to Carmona's compound, [Cp*ZnZnCp*], without splitting the ZnZn bond. The choice of non-coordinating fluoroaromatic solvents was crucial. The bonding situations of the all-hydrocarbon-ligand-protected clusters were investigated by quantum chemical calculations revealing a high degree of σ-aromaticity similar to the triatomic hydrogen ion [H3 ](+) . The new species serve as molecular building units of Cun Znm nanobrass clusters as indicated by LIFDI mass spectrometry. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
    Angewandte Chemie International Edition in English 02/2015; 54(14). DOI:10.1002/anie.201410737 · 13.45 Impact Factor
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    Hung Banh · Christian Gemel · Rüdiger W. Seidel · Roland A. Fischer ·
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    ABSTRACT: The synthesis and characterisation of the solvent-stabilized salt [Zn2(THF)6]2+[BAr4F]2− (1) is presented, which features the dizinc dication [Zn2]2+ as an analogue of the calomel dication [Hg2]2+. The labile tetrahydrofuran (THF) solvate molecules of 1 can be readily substituted by other ligands. Reaction with the strong donor ligand PMe3 (Me = CH3) leads to the Zn(II) complex [Zn(PMe3)4]2+[BAr4F]2− by disproportionation, while the π-acceptor-ligand phenylisocyanide (PhNC) gives the substitution product [Zn2(PhNC)6]2+[BAr4F]2− (2) with an intact Zn–Zn bond.
    Chemical Communications 01/2015; 51(11). DOI:10.1039/C4CC08850F · 6.83 Impact Factor
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    ABSTRACT: The synthesis and characterization of the cationic mixed metal Ga/Zn cluster [Zn2(GaCp*)6](2+) (1) is presented. The reaction of [Zn2Cp*2] with [Ga2Cp*][BAr4(F)] leads to the formation of the novel complex being the first example of a [Zn2](2+) core exclusively ligated by metalloid group-13 organyl-ligands. Compound 1 exhibits two different coordination modes: In the solid state, two of the six GaCp* ligands occupy bridging positions, whereas VT (1)H NMR indicates the coexistence of a second isomer in solution featuring six terminal GaCp* ligands. Quantum chemical calculations have been carried out to assign the gallium and zinc positions; the bonding situation in 1 is characterized and the importance of dispersion forces is discussed.
    Inorganic Chemistry 12/2014; 54(1). DOI:10.1021/ic502532g · 4.76 Impact Factor

Publication Stats

10k Citations
2,253.97 Total Impact Points


  • 2015
    • Nanjing University of Technology
      Nan-ching, Jiangsu Sheng, China
  • 1998-2015
    • Ruhr-Universität Bochum
      • • Inorganic Chemistry
      • • Faculty of Chemistry and Biochemistry
      Bochum, North Rhine-Westphalia, Germany
  • 1998-2014
    • Philipps University of Marburg
      • Faculty of Chemistry
      Marburg, Hesse, Germany
  • 1999
    • Hochschule Bochum
      Bochum, North Rhine-Westphalia, Germany
  • 1996-1997
    • Universität Heidelberg
      • Institute of Inorganic Chemistry
      Heidelburg, Baden-Württemberg, Germany
    • Technische Universität München
      • Walter Schottky Institut (WSI)
      München, Bavaria, Germany
  • 1980-1996
    • Deutsches Herzzentrum München
      München, Bavaria, Germany
  • 1988
    • Hochschuelerschaft an der Technischen Universitaet Graz
      FRG, New York, United States