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- ItemEngineering Micropatterned Dry Adhesives: From Contact Theory to Handling Applications(Weinheim : Wiley-VCH, 2018) Hensel, René; Moh, Karsten; Arzt, EduardReversible adhesion is the key functionality to grip, place, and release objects nondestructively. Inspired by nature, micropatterned dry adhesives are promising candidates for this purpose and have attracted the attention of research groups worldwide. Their enhanced adhesion compared to nonpatterned surfaces is frequently demonstrated. An important conclusion is that the contact mechanics involved is at least as important as the surface energy and chemistry. In this paper, the roles of the contact geometry and mechanical properties are reviewed. With a focus on applications, the effects of substrate roughness and of temperature variations, and the long-term performance of micropatterned adhesives are discussed. The paper provides a link between the current, detailed understanding of micropatterned adhesives and emerging applications.
- ItemMagnetic Nanoparticle Chains in Gelatin Ferrogels: Bioinspiration from Magnetotactic Bacteria(Weinheim : Wiley-VCH, 2019) Sturm, Sebastian; Siglreitmeier, Maria; Wolf, Daniel; Vogel, Karin; Gratz, Micha; Faivre, Damien; Lubk, Axel; Büchner, Bernd; Sturm, Elena V.; Cölfen, HelmutInspired by chains of ferrimagnetic nanocrystals (NCs) in magnetotactic bacteria (MTB), the synthesis and detailed characterization of ferrimagnetic magnetite NC chain-like assemblies is reported. An easy green synthesis route in a thermoreversible gelatin hydrogel matrix is used. The structure of these magnetite chains prepared with and without gelatin is characterized by means of transmission electron microscopy, including electron tomography (ET). These structures indeed bear resemblance to the magnetite assemblies found in MTB, known for their mechanical flexibility and outstanding magnetic properties and known to crystallographically align their magnetite NCs along the strongest <111> magnetization easy axis. Using electron holography (EH) and angular dependent magnetic measurements, the magnetic interaction between the NCs and the generation of a magnetically anisotropic material can be shown. The electro- and magnetostatic modeling demonstrates that in order to precisely determine the magnetization (by means of EH) inside chain-like NCs assemblies, their exact shape, arrangement and stray-fields have to be considered (ideally obtained using ET). © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemElectron beam induced dehydrogenation of MgH2 studied by VEELS(Cham : Springer International Publishing AG, 2016) Surrey, Alexander; Schultz, Ludwig; Rellinghaus, BerndNanosized or nanoconfined hydrides are promising materials for solid-state hydrogen storage. Most of these hydrides, however, degrade fast during the structural characterization utilizing transmission electron microscopy (TEM) upon the irradiation with the imaging electron beam due to radiolysis. We use ball-milled MgH2 as a reference material for in-situ TEM experiments under low-dose conditions to study and quantitatively understand the electron beam-induced dehydrogenation. For this, valence electron energy loss spectroscopy (VEELS) measurements are conducted in a monochromated FEI Titan3 80–300 microscope. From observing the plasmonic absorptions it is found that MgH2 successively converts into Mg upon electron irradiation. The temporal evolution of the spectra is analyzed quantitatively to determine the thickness-dependent, characteristic electron doses for electron energies of both 80 and 300 keV. The measured electron doses can be quantitatively explained by the inelastic scattering of the incident high-energy electrons by the MgH2 plasmon. The obtained insights are also relevant for the TEM characterization of other hydrides.
- ItemCorrection: Interface-engineered reliable HfO2-based RRAM for synaptic simulation (Journal of Materials Chemistry C (2019) DOI: 10.1039/c9tc04880d)(London [u.a.] : RSC, 2019) Wang, Qiang; Niu, Gang; Roy, Sourav; Wang, Yankun; Zhang, Yijun; Wu, Heping; Zhai, Shijie; Bai, Wei; Shi, Peng; Song, Sannian; Song, Zhitang; Xie, Ya-Hong; Ye, Zuo-Guang; Wenger, Christian; Meng, Xiangjian; Ren, WeiThere was an error in the author list of this published article. The corresponding authors for this paper are Gang Niu (gangniu@xjtu.edu.cn) and Wei Ren (wren@mail.xjtu.edu.cn). The footnote indicating that Qiang Wang and Gang Niu contributed equally to the work was not intended. The corrected author list and notations are shown here. The Royal Society of Chemistry apologises for these errors and any consequent inconvenience to authors and readers. © The Royal Society of Chemistry 2019.
- ItemOn the anomalous optical conductivity dispersion of electrically conducting polymers: Ultra-wide spectral range ellipsometry combined with a Drude-Lorentz model(London [u.a.] : RSC, 2019) Chen, Shangzhi; Kühne, Philipp; Stanishev, Vallery; Knight, Sean; Brooke, Robert; Petsagkourakis, Ioannis; Crispin, Xavier; Schubert, Mathias; Darakchieva, Vanya; Jonsson, Magnus P.Electrically conducting polymers (ECPs) are becoming increasingly important in areas such as optoelectronics, biomedical devices, and energy systems. Still, their detailed charge transport properties produce an anomalous optical conductivity dispersion that is not yet fully understood in terms of physical model equations for the broad range optical response. Several modifications to the classical Drude model have been proposed to account for a strong non-Drude behavior from terahertz (THz) to infrared (IR) ranges, typically by implementing negative amplitude oscillator functions to the model dielectric function that effectively reduce the conductivity in those ranges. Here we present an alternative description that modifies the Drude model via addition of positive-amplitude Lorentz oscillator functions. We evaluate this so-called Drude-Lorentz (DL) model based on the first ultra-wide spectral range ellipsometry study of ECPs, spanning over four orders of magnitude: from 0.41 meV in the THz range to 5.90 eV in the ultraviolet range, using thin films of poly(3,4-ethylenedioxythiophene):tosylate (PEDOT:Tos) as a model system. The model could accurately fit the experimental data in the whole ultrawide spectral range and provide the complex anisotropic optical conductivity of the material. Examining the resonance frequencies and widths of the Lorentz oscillators reveals that both spectrally narrow vibrational resonances and broader resonances due to localization processes contribute significantly to the deviation from the Drude optical conductivity dispersion. As verified by independent electrical measurements, the DL model accurately determines the electrical properties of the thin film, including DC conductivity, charge density, and (anisotropic) mobility. The ellipsometric method combined with the DL model may thereby become an effective and reliable tool in determining both optical and electrical properties of ECPs, indicating its future potential as a contact-free alternative to traditional electrical characterization. © The Royal Society of Chemistry 2019.
- ItemNiobium carbide nanofibers as a versatile precursor for high power supercapacitor and high energy battery electrodes(London [u.a.] : RSC, 2016) Tolosa, Aura; Krüner, Benjamin; Fleischmann, Simon; Jäckel, Nicolas; Zeiger, Marco; Aslan, Mesut; Grobelsek, Ingrid; Presser, VolkerThis study presents electrospun niobium carbide/carbon (NbC/C) hybrid nanofibers, with an average diameter of 69 ± 30 nm, as a facile precursor to derive either highly nanoporous niobium carbide-derived carbon (NbC–CDC) fibers for supercapacitor applications or niobium pentoxide/carbon (Nb2O5/C) hybrid fibers for battery-like energy storage. In all cases, the electrodes consist of binder-free and free-standing nanofiber mats that can be used without further conductive additives. Chlorine gas treatment conformally transforms NbC nanofiber mats into NbC–CDC fibers with a specific surface area of 1508 m2 g−1. These nanofibers show a maximum specific energy of 19.5 W h kg−1 at low power and 7.6 W h kg−1 at a high specific power of 30 kW kg−1 in an organic electrolyte. CO2 treatment transforms NbC into T-Nb2O5/C hybrid nanofiber mats that provide a maximum capacity of 156 mA h g−1. The presence of graphitic carbon in the hybrid nanofibers enabled high power handling, maintaining 50% of the initial energy storage capacity at a high rate of 10 A g−1 (64 C-rate). When benchmarked for an asymmetric full-cell, a maximum specific energy of 86 W h kg−1 was obtained. The high specific power for both systems, NbC–CDC and T-Nb2O5/C, resulted from the excellent charge propagation in the continuous nanofiber network and the high graphitization of the carbon structure.
- ItemEffects of PNDIT2 end groups on aggregation, thin film structure, alignment and electron transport in field-effect transistors(London [u.a.] : RSC, 2016) Matsidik, Rukiya; Luzio, Alessandro; Hameury, Sophie; Komber, Hartmut; McNeill, Christopher R.; Caironi, Mario; Sommer, MichaelTo develop greener protocols toward the sustainable production of conjugated polymers, we combine the advantages of atom-economic direct arylation polycondensation (DAP) with those of the green solvent 2-methyltetrahydrofuran (MeTHF). The n-type copolymer PNDIT2 is synthesized from unsubstituted bithiophene (T2) and 2,6-dibromonapthalene diimide (NDIBr2) under simple DAP conditions in MeTHF. Extensive optimization is required to suppress nucleophilic substitution of NDIBr end groups, which severely limits molar mass. Different carboxylic acids, bases, palladium precursors and ligands are successfully screened to enable quantitative yield and satisfyingly high molar masses up to Mn,SEC ∼ 20 kDa. In contrast to PNDIT2 made via DAP in toluene with tolyl-chain termini, nucleophilic substitution of NDIBr chain ends in MeTHF finally leads to NDI-OH termination. The influence of different chain termini on the optical, thermal, structural and electronic properties of PNDIT2 is investigated. For samples with identical molecular weight, OH-termination leads to slightly reduced aggregation in solution and bulk crystallinity, a decreased degree of alignment in directionally deposited films, and a consequently reduced, but not compromised, electron mobility with promising values still close to 0.9 cm2 V−1 s−1.
- ItemVanadium pentoxide/carbide-derived carbon core-shell hybrid particles for high performance electrochemical energy storage(London [u.a.] : RSC, 2016) Zeiger, Marco; Ariyanto, Teguh; Krüner, Benjamin; Peter, Nicolas J.; Fleischmann, Simon; Etzold, Bastian J.M.; Presser, VolkerA novel, two step synthesis is presented combining the formation of carbide-derived carbon (CDC) and redox-active vanadium pentoxide (V2O5) in a core–shell manner using solely vanadium carbide (VC) as the precursor. In a first step, the outer part of VC particles is transformed to nanoporous CDC owing to the in situ formation of chlorine gas from NiCl2 at 700 °C. In a second step, the remaining VC core is calcined in synthetic air to obtain V2O5/CDC core–shell particles. Materials characterization by means of electron microscopy, Raman spectroscopy, and X-ray diffraction clearly demonstrates the partial transformation from VC to CDC, as well as the successive oxidation to V2O5/CDC core–shell particles. Electrochemical performance was tested in organic 1 M LiClO4 in acetonitrile using half- and asymmetric full-cell configuration. High specific capacities of 420 mA h g−1 (normalized to V2O5) and 310 mA h g−1 (normalized to V2O5/CDC) were achieved. The unique nanotextured core–shell architecture enables high power retention with ultrafast charging and discharging, achieving more than 100 mA h g−1 at 5 A g−1 (rate of 12C). Asymmetric cell design with CDC on the positive polarization side leads to a high specific energy of up to 80 W h kg−1 with a superior retention of more than 80% over 10 000 cycles and an overall energy efficiency of up to 80% at low rates.
- ItemMXene as a novel intercalation-type pseudocapacitive cathode and anode for capacitive deionization(London [u.a.] : RSC, 2016) Srimuk, Pattarachai; Kaasik, Friedrich; Krüner, Benjamin; Tolosa, Aura; Fleischmann, Simon; Jäckel, Nicolas; Tekeli, Mehmet C.; Aslan, Mesut; Suss, Matthew E.; Presser, VolkerIn this proof-of-concept study, we introduce and demonstrate MXene as a novel type of intercalation electrode for desalination via capacitive deionization (CDI). Traditional CDI cells employ nanoporous carbon electrodes with significant pore volume to achieve a large desalination capacity via ion electrosorption. By contrast, MXene stores charge by ion intercalation between the sheets of its two-dimensional nanolamellar structure. By this virtue, it behaves as an ideal pseudocapacitor, that is, showing capacitive electric response while intercalating both anions and cations. We synthesized Ti3C2-MXene by the conventional process of etching ternary titanium aluminum carbide i.e., the MAX phase (Ti3AlC2) with hydrofluoric acid. The MXene material was cast directly onto the porous separator of the CDI cell without added binder, and exhibited very stable performance over 30 CDI cycles with an average salt adsorption capacity of 13 ± 2 mg g−1.
- ItemLayered manganese bismuth tellurides with GeBi4Te7- and GeBi6Te10-type structures: Towards multifunctional materials(London : RSC Publ., 2019) Souchay, Daniel; Nentwig, Markus; Günther, Daniel; Keilholz, Simon; de Boor, Johannes; Zeugner, Alexander; Isaeva, Anna; Ruck, Michael; Wolter, Anja U.B.; Büchnerde, Bernd; Oeckler, OliverThe crystal structures of new layered manganese bismuth tellurides with the compositions Mn0.85(3)Bi4.10(2)Te7 and Mn0.73(4)Bi6.18(2)Te10 were determined by single-crystal X-ray diffraction, including the use of microfocused synchrotron radiation. These analyses reveal that the layered structures deviate from the idealized stoichiometry of the 12P-GeBi4Te7 (space group P3m1) and 51R-GeBi6Te10 (space group R3m) structure types they adopt. Modified compositions Mn1-xBi4+2x/3Te7 (x = 0.15-0.2) and Mn1-xBi6+2x/3Te10 (x = 0.19-0.26) assume cation vacancies and lead to homogenous bulk samples as confirmed by Rietveld refinements. Electron diffraction patterns exhibit no diffuse streaks that would indicate stacking disorder. The alternating quintuple-layer [M2Te3] and septuple-layer [M3Te4] slabs (M = mixed occupied by Bi and Mn) with 1 : 1 sequence (12P stacking) in Mn0.85Bi4.10Te7 and 2 : 1 sequence (51R stacking) in Mn0.81Bi6.13Te10 were also observed in HRTEM images. Temperature-dependent powder diffraction and differential scanning calorimetry show that the compounds are high-temperature phases, which are metastable at ambient temperature. Magnetization measurements are in accordance with a MnII oxidation state and point at predominantly ferromagnetic coupling in both compounds. The thermoelectric figures of merit of n-type conducting Mn0.85Bi4.10Te7 and Mn0.81Bi6.13Te10 reach zT = 0.25 at 375 °C and zT = 0.28 at 325 °C, respectively. Although the compounds are metastable, compact ingots exhibit still up to 80% of the main phases after thermoelectric measurements up to 400 °C. © The Royal Society of Chemistry 2019.