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    Correction: 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, Wei
    There 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.
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    A size dependent evaluation of the cytotoxicity and uptake of nanographene oxide
    (London [u.a.] : RSC, 2015) Mendes, Rafael Gregorio; Koch, Britta; Bachmatiuk, Alicja; Ma, Xing; Sanchez, Samuel; Damm, Christine; Schmidt, Oliver G.; Gemming, Thomas; Eckert, Jürgen; Rümmeli, Mark H.
    Graphene oxide (GO) has attracted great interest due to its extraordinary potential for biomedical application. Although it is clear that the naturally occurring morphology of biological structures is crucial to their precise interactions and correct functioning, the geometrical aspects of nanoparticles are often ignored in the design of nanoparticles for biological applications. A few in vitro and in vivo studies have evaluated the cytotoxicity and biodistribution of GO, however very little is known about the influence of flake size and cytotoxicity. Herein, we aim at presenting an initial cytotoxicity evaluation of different nano-sized GO flakes for two different cell lines (HeLa (Kyoto) and macrophage (J7742)) when they are exposed to samples containing different sized nanographene oxide (NGO) flakes (mean diameter of 89 and 277 nm). The obtained data suggests that the larger NGO flakes reduce cell viability as compared to smaller flakes. In addition, the viability reduction correlates with the time and the concentration of the NGO nanoparticles to which the cells are exposed. Uptake studies were also conducted and the data suggests that both cell lines internalize the GO nanoparticles during the incubation periods studied.
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    Design of high-performance antimony/MXene hybrid electrodes for sodium-ion batteries
    (London [u.a.] : RSC, 2022) Arnold, Stefanie; Gentile, Antonio; Li, Yunjie; Wang, Qingsong; Marchionna, Stefano; Ruffo, Riccardo; Presser, Volker
    Due to their versatile properties and excellent electrical conductivity, MXenes have become attractive materials for alkali metal-ion batteries. However, as the capacity is limited to lower values due to the intercalation mechanism, these materials can hardly keep up in the ever-fast-growing community of battery research. Antimony has a promisingly high theoretical sodiation capacity characterized by an alloying reaction. The main drawback of this type of battery material is related to the high volume changes during cycling, often leading to electrode cracking and pulverization, resulting in poor electrochemical performance. A synergistic effect of combing antimony and MXene can be expected to obtain an optimized electrochemical system to overcome capacity fading of antimony while taking advantage of MXene charge storage ability. In this work, variation of the synthesis parameters and material design strategy have been dedicated to achieving the optimized antimony/MXene hybrid electrodes for high-performance sodium-ion batteries. The optimized performance does not align with the highest amount of antimony, the smallest nanoparticles, or the largest interlayer distance of MXene but with the most homogeneous distribution of antimony and MXene while both components remain electrochemically addressable. As a result, the electrode with 40 mass% MXene, not previously expanded, etched with 5 mass% HF and 60% antimony synthesized on the surfaces of MXene emerged as the best electrode. We obtained a high reversible capacity of 450 mA h g−1 at 0.1 A g−1 with a capacity retention of around 96% after 100 cycles with this hybrid material. Besides the successful cycling stability, this material also exhibits high rate capability with a capacity of 365 mA h g−1 at 4 A g−1. In situ XRD measurements and post mortem analysis were used to investigate the reaction mechanism.
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    The natural critical current density limit for Li7La3Zr2O12 garnets
    (London [u.a.] : RSC, 2020) Flatscher, Florian; Philipp, Martin; Ganschow, Steffen; Wilkening, H. Martin R.; Rettenwander, Daniel
    Ceramic batteries equipped with Li-metal anodes are expected to double the energy density of conventional Li-ion batteries. Besides high energy densities, also high power is needed when batteries have to be developed for electric vehicles. Practically speaking, so-called critical current densities (CCD) higher than 3 mA cm-2 are needed to realize such systems. As yet, this value has, however, not been achieved for garnet-type Li7La3Zr2O12 (LLZO) being one of the most promising ceramic electrolytes. Most likely, CCD values are influenced by the area specific resistance (ASR) governing ionic transport across the Li|electrolyte interface. Here, single crystals of LLZO with adjusted ASR are used to quantify this relationship in a systematic manner. It turned out that CCD values exponentially decrease with increasing ASR. The highest obtained CCD value was as high as 280 µA cm-2. This value should be regarded as the room-temperature limit for LLZO when no external pressure is applied. Concluding, for polycrystalline samples either stack pressure or a significant increase of the interfacial area is needed to reach current densities equal or higher than the above-mentioned target value. This journal is © The Royal Society of Chemistry.
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    Large-area wet-chemical deposition of nanoporous tungstic silica coatings
    (London [u.a.] : RSC, 2015) Nielsen, K.H.; Wondraczek, K.; Schubert, U.S.; Wondraczek, L.
    We report on a facile procedure for synthesis of nanoporous coatings of tungstic silica through wet-chemical deposition and post-treatment of tungsten-doped potassium silicate solutions. The process relies on an aqueous washing and ion exchange step where dispersed potassium salt deposits are removed from a 150 nm silicate gel layer. Through an adjustment of the pH value of the washing agent within the solubility regime of a tungstic salt precursor, the tungsten content of the remaining nanostructured coating can be controlled. We propose this route as a universal approach for the deposition of large-area coatings of nanoporous silica with the potential for incorporating a broad variety of other dopant species. As for the present case, we observe, on the one hand, antireflective properties which enable the reduction of reflection losses from float glass by up to 3.7 percent points. On the other hand, the incorporation of nanoscale tungstic precipitates provides a lever for tailoring the coating hydrophilicity and, eventually, also surface acidity. This may provide a future route for combining optical performance with anti-fouling functionality.
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    On 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.
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    Niobium 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, Volker
    This 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.
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    Choosing the right carbon additive is of vital importance for high-performance Sb-based Na-ion batteries
    (London [u.a.] : RSC, 2020) Pfeifer, Kristina; Arnold, Stefanie; Budak, Öznil; Luo, Xianlin; Presser, Volker; Ehrenberg, Helmut; Dsoke, Sonia
    Electrodes based on alloying reactions for sodium-ion batteries (NIB) offer high specific capacity but require bespoken electrode material design to enable high performance stability. This work addresses that issue by systematically exploring the impact of carbon properties on antimony/carbon composite electrodes for NIBs. Since the Sb surface is covered by an insulating oxide layer, carbon additives are crucial for the percolation and electrochemical activity of Sb based anodes. Instead of using complex hybridization strategies, the ability of mechanical mixing to yield stable high-performance Sb/C sodium-ion battery (NIB) electrodes is shown. This is only possible by considering the physical, chemical, and structural features of the carbon phase. A comparison of carbon nanohorns, onion-like carbon, carbon black, and graphite as conductive additives is given in this work. The best performance is not triggered by the highest or lowest surface area, and not by highest or lowest heteroatom content, but by the best ability to homogenously distribute within the Sb matrix. The latter provides an optimum interaction between carbon and Sb and is best enabled by onion-like carbon. A remarkable rate performance is attained, electrode cracking caused by volume expansion is successfully prevented, and the homogeneity of the solid/electrolyte interphase is significantly improved as a result of it. With this composite electrode, a reversible capacity of 490 mA h g-1 at 0.1 A g-1 and even 300 mA g-1 at 8 A g-1 is obtained. Additionally, high stability with a capacity retention of 73% over 100 cycles is achieved at charge/discharge rates of 0.2 A g-1 This journal is © The Royal Society of Chemistry.
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    Targeting extracellular lectins of Pseudomonas aeruginosa with glycomimetic liposomes
    (London [u.a.] : RSC, 2021) Metelkina, Olga; Huck, Benedikt; O'Connor, Jonathan S.; Koch, Marcus; Manz, Andreas; Lehr, Claus-Michael; Titz, Alexander
    The antimicrobial resistance crisis requires novel approaches for the therapy of infections especially with Gram-negative pathogens. Pseudomonas aeruginosa is defined as priority 1 pathogen by the WHO and thus of particular interest. Its drug resistance is primarily associated with biofilm formation and essential constituents of its extracellular biofilm matrix are the two lectins, LecA and LecB. Here, we report microbial lectin-specific targeted nanovehicles based on liposomes. LecA- and LecB-targeted phospholipids were synthesized and used for the preparation of liposomes. These liposomes with varying surface ligand density were then analyzed for their competitive and direct lectin binding activity. We have further developed a microfluidic device that allowed the optical detection of the targeting process to the bacterial lectins. Our data showed that the targeted liposomes are specifically binding to their respective lectin and remain firmly attached to surfaces containing these lectins. This synthetic and biophysical study provides the basis for future application in targeted antibiotic delivery to overcome antimicrobial resistance.
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    Effects 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, Michael
    To 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.