TY - JOUR A1 - Goebel, Ronald A1 - Xie, Zai-Lai A1 - Neumann, Mike A1 - Günter, Christina A1 - Loebbicke, Ruben A1 - Kubo, Shiori A1 - Titirici, Maria-Magdalena A1 - Giordano, Cristina A1 - Taubert, Andreas T1 - Synthesis of mesoporous carbon/iron carbide hybrids with unusually high surface areas from the ionic liquid precursor [Bmim][FeCl4] JF - CrystEngComm N2 - Mesoporous carbon/iron carbide hybrid materials with surface areas reaching 800 m(2) g(-1) were synthesized via an exotemplating route using monolithic mesoporous silica as template and the ionic liquid 1-butyl-3-methylimidazolium tetrachloridoferrate(III) [Bmim][FeCl4] as carbon and iron source. After heat treatment (750 degrees C under argon) of the [Bmim][FeCl4] precursor confined within the silica matrix, the silica exotemplate was removed with HF leaving the mesoporous C/Fe3C hybrid behind. The surface areas and the pore sizes depend on the exotemplate and the surface areas a significantly larger than any other surface area reported for C/Fe3C hybrid materials so far. The approach is thus a prototype for the synthesis of high-surface area iron carbide-based hybrid materials with potential application in catalysis. Y1 - 2012 U6 - https://doi.org/10.1039/c2ce25064k SN - 1466-8033 VL - 14 IS - 15 SP - 4946 EP - 4951 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR A1 - Goebel, Ronald A1 - Hesemann, Peter A1 - Weber, Jens A1 - Moeller, Eléonore A1 - Friedrich, Alwin A1 - Beuermann, Sabine A1 - Taubert, Andreas T1 - Surprisingly high, bulk liquid-like mobility of silica-confined ionic liquids N2 - Mesoporous silica monoliths were prepared by the sol - gel technique and. lled with 1-ethyl-3-methyl imidazolium [Emim]-X (X = dicyanamide [N(CN)(2)], ethyl sulfate [EtSO4], thiocyanate [SCN], and triflate [TfO]) ionic liquids (ILs) using a methanol-IL exchange technique. The structure and behavior of the ILs inside the silica monoliths were studied using X-ray scattering, nitrogen sorption, IR spectroscopy, solid-state NMR, and thermal analysis. DSC finds shifts in both the glass transition temperature and melting points (where applicable) of the ILs. Glass transition and melting occur well below room temperature. There is thus no conflict with the NMR and IR data, which show that the ILs are as mobile at room temperature as the bulk (not confined) ILs. The very narrow line widths of the NMR spectra suggest that the ILs in our materials have the highest mobility reported for confined ILs so far. As a result, our data suggest that it is possible to generate IL/silica hybrid materials (ionogels) with bulk-like properties of the IL. This could be interesting for applications in, e.g., the solar cell or membrane fields. Y1 - 2009 UR - http://xlink.rsc.org/jumptojournal.cfm?journal_code=CP U6 - https://doi.org/10.1039/B821833a SN - 1463-9076 ER - TY - JOUR A1 - Kind, Lucy A1 - Plamper, Felix A. A1 - Goebel, Ronald A1 - Mantion, Alexandre A1 - Mueller, Axel H. E. A1 - Pieles, Uwe A1 - Taubert, Andreas A1 - Meier, Wolfgang P. T1 - Silsesquioxane/polyamine nanoparticle-templated formation of star- or raspberry-like silica nanoparticles N2 - Silica is an important mineral in biology and technology, and many protocols have been developed for the synthesis of complex silica architectures. The current report shows that silsesquioxane nanoparticles carrying polymer arms on their surface are efficient templates for the fabrication of silica particles with a star- or raspberry-like morphology. The shape of the resulting particles depends on the chemistry of the polymer arms. With poly(N,N- dimethylaminoethyl methacrylate) (PDMAEMA) arms, spherical particles with a less electron dense core form. With poly {[2- (methacryloyloxy)ethyl] trimethylammonium iodide} (PMETAI), star- or raspberry-like particles form. Electron microscopy, electron tomography, and small-angle X-ray scattering show that the resulting silica particles have a complex structure, where a silsequioxane nanoparticle carrying the polymer arms is in the center. Next is a region that is polymer-rich. The outermost region of the particle is a silica layer, where the outer parts of the polymer arms are embedded. Time- resolved zeta-potential and pH measurements, dynamic light scattering, and electron microscopy reveal that silica formation proceeds differently if PDMAEMA is exchanged for PMETAI. Y1 - 2009 UR - http://pubs.acs.org/journal/langd5 U6 - https://doi.org/10.1021/La900229n SN - 0743-7463 ER - TY - JOUR A1 - Delahaye, Emilie A1 - Goebel, Ronald A1 - Loebbicke, Ruben A1 - Guillot, Regis A1 - Sieber, Christoph A1 - Taubert, Andreas T1 - Silica ionogels for proton transport JF - Journal of materials chemistry N2 - A number of ionogels - silica-ionic liquid (IL) hybrid materials - were synthesized and studied for their ionic conductivity. The materials are based on a sulfonated IL, 1-methyl-3-(3-sulfopropyl-)-imidazolium p-toluenesulfonate, [PmimSO(3)H][PTS], which contains a sulfonic acid/sulfonate group both in the IL anion and in the side chain of the IL cation. By way of the sulfonate-sulfonic acid proton transfer, the IL imparts the ionogel with a high ionic conductivity of ca. 10(-2) S cm(-1) in the as-synthesized state at 120 degrees C and 10(-3) S cm(-1) in the dry state at 120 degrees C. The ionogels are stable up to ca. 150 degrees C in dynamic thermogravimetric analysis. This suggests that these materials, which are relatively cheap and easily fabricated, could find application in fuel cells in intermediate temperature ranges where many other membrane materials are not suitable. Y1 - 2012 U6 - https://doi.org/10.1039/c2jm00037g SN - 0959-9428 VL - 22 IS - 33 SP - 17140 EP - 17146 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR A1 - Goebel, Ronald A1 - White, Robin J. A1 - Titirici, Maria-Magdalena A1 - Taubert, Andreas T1 - Carbon-based ionogels tuning the properties of the ionic liquid via carbon-ionic liquid interaction JF - Physical chemistry, chemical physics : a journal of European Chemical Societies N2 - The behavior of two ionic liquids (ILs), 1-ethyl-3-methylimidazolium dicyanamide [Emim][DCA] and 1-ethyl-3-methylimidazolium triflate [Emim][TfO], in (meso) porous carbonaceous hosts was investigated. Prior to IL incorporation into the host, the carbon matrix was thermally annealed between 180 and 900 degrees C to control carbon condensation and surface chemistry. The resulting materials have an increasing "graphitic'' carbon character with increasing treatment temperature, reflected in a modified behavior of the ILs when impregnated into the carbon host. The two ILs show significant changes in the thermal behavior as measured from differential scanning calorimetry; these changes can be assigned to anion-pi interaction between the IL anions and the pore wall surfaces of these flexible carbonaceous support materials. Y1 - 2012 U6 - https://doi.org/10.1039/c2cp23929a SN - 1463-9076 VL - 14 IS - 17 SP - 5992 EP - 5997 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR A1 - Goebel, Ronald A1 - Hesemann, Peter A1 - Friedrich, Alwin A1 - Rothe, Regina A1 - Schlaad, Helmut A1 - Taubert, Andreas T1 - Modular thiol-ene chemistry approach towards mesoporous silica monoliths with organically modified pore walls JF - Chemistry - a European journal N2 - The surface modification of mesoporous silica monoliths through thiol-ene chemistry is reported. First, mesoporous silica monoliths with vinyl, allyl, and thiol groups were synthesized through a sol-gel hydrolysis-poly-condensation reaction from tetramethyl orthosilicate (TMOS) and vinyltriethoxysilane, allyltriethoxysilane, and (3-mercaptopropyl) trimethoxysilane, respectively. By variation of the molar ratio of the comonomers TMOS and functional silane, mesoporous silica objects containing different amounts of vinyl, allyl, and thiol groups were obtained. These intermediates can subsequently be derivatized through radical photoaddition reactions either with a thiol or an olefin, depending on the initial pore wall functionality, to yield silica monoliths with different pore-wall chemistries. Nitrogen sorption, small-angle X-ray scattering, solid-state NMR spectroscopy, elemental analysis, thermogravimetric analysis, and redox titration demonstrate that the synthetic pathway influences the morphology and pore characteristics of the resulting monoliths and also plays a significant role in the efficiency of functionalization. Moreover, the different reactivity of the vinyl and allyl groups on the pore wall affects the addition reaction, and hence, the degree of the pore-wall functionalization. This report demonstrates that thiol-ene photoaddition reactions are a versatile platform for the generation of a large variety of organically modified silica monoliths with different pore surfaces. KW - mesoporous materials KW - photochemistry KW - sol-gel processes KW - surface chemistry Y1 - 2014 U6 - https://doi.org/10.1002/chem.201403982 SN - 0947-6539 SN - 1521-3765 VL - 20 IS - 52 SP - 17579 EP - 17589 PB - Wiley-VCH CY - Weinheim ER -