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    Lightweight polymer-carbon composite current collector for lithium-ion batteries
    (Basel : MDPI, 2020) Fritsch, Marco; Coeler, Matthias; Kunz, Karina; Krause, Beate; Marcinkowski, Peter; Pötschke, Petra; Wolter, Mareike; Michaelis, Alexander
    A hermetic dense polymer-carbon composite-based current collector foil (PCCF) for lithium-ion battery applications was developed and evaluated in comparison to state-of-the-art aluminum (Al) foil collector. Water-processed LiNi0.5Mn1.5O4 (LMNO) cathode and Li4Ti5O12 (LTO) anode coatings with the integration of a thin carbon primer at the interface to the collector were prepared. Despite the fact that the laboratory manufactured PCCF shows a much higher film thickness of 55 µm compared to Al foil of 19 µm, the electrode resistance was measured to be by a factor of 5 lower compared to the Al collector, which was attributed to the low contact resistance between PCCF, carbon primer and electrode microstructure. The PCCF-C-primer collector shows a sufficient voltage stability up to 5 V vs. Li/Li+ and a negligible Li-intercalation loss into the carbon primer. Electrochemical cell tests demonstrate the applicability of the developed PCCF for LMNO and LTO electrodes, with no disadvantage compared to state-of-the-art Al collector. Due to a 50% lower material density, the lightweight and hermetic dense PCCF polymer collector offers the possibility to significantly decrease the mass loading of the collector in battery cells, which can be of special interest for bipolar battery architectures. © 2020 by the authors. Licensee MDPI, Basel, Switzerland.
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    High-Performance, Lightweight, and Flexible Thermoplastic Polyurethane Nanocomposites with Zn2+-Substituted CoFe2O4 Nanoparticles and Reduced Graphene Oxide as Shielding Materials against Electromagnetic Pollution
    (Washington, DC : ACS Publications, 2021-10-11) Anju; Yadav, Raghvendra Singh; Pötschke, Petra; Pionteck, Jürgen; Krause, Beate; Kuřitka, Ivo; Vilcakova, Jarmila; Skoda, David; Urbánek, Pavel; Machovsky, Michal; Masař, Milan; Urbánek, Michal; Jurca, Marek; Kalina, Lukas; Havlica, Jaromir
    The development of flexible, lightweight, and thin high-performance electromagnetic interference shielding materials is urgently needed for the protection of humans, the environment, and electronic devices against electromagnetic radiation. To achieve this, the spinel ferrite nanoparticles CoFe2O4 (CZ1), Co0.67Zn0.33Fe2O4 (CZ2), and Co0.33Zn0.67Fe2O4 (CZ3) were prepared by the sonochemical synthesis method. Further, these prepared spinel ferrite nanoparticles and reduced graphene oxide (rGO) were embedded in a thermoplastic polyurethane (TPU) matrix. The maximum electromagnetic interference (EMI) total shielding effectiveness (SET) values in the frequency range 8.2-12.4 GHz of these nanocomposites with a thickness of only 0.8 mm were 48.3, 61.8, and 67.8 dB for CZ1-rGO-TPU, CZ2-rGO-TPU, and CZ3-rGO-TPU, respectively. The high-performance electromagnetic interference shielding characteristics of the CZ3-rGO-TPU nanocomposite stem from dipole and interfacial polarization, conduction loss, multiple scattering, eddy current effect, natural resonance, high attenuation constant, and impedance matching. The optimized CZ3-rGO-TPU nanocomposite can be a potential candidate as a lightweight, flexible, thin, and high-performance electromagnetic interference shielding material.
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    Thermal annealing to influence the vapor sensing behavior of co-continuous poly(lactic acid)/polystyrene/multiwalled carbon nanotube composites
    (Amsterdam [u.a.] : Elsevier Science, 2020) Li, Yilong; Pionteck, Jürgen; Pötschke, Petra; Voit, Brigitte
    With the main purpose of being used as vapor leakage detector, the volatile organic compound (VOC) vapor sensing properties of conductive polymer blend composites were studied. Poly(lactic acid)/polystyrene/multi-walled carbon nanotube (PLA/PS/MWCNT) based conductive polymer composites (CPCs) in which the polymer components exhibit different interactions with the vapors, were prepared by melt mixing. CPCs with a blend composition of 50/50 wt% resulted in the finest co-continuous structure and selective MWCNT localization in PLA. Therefore, these composites were selected for sensor tests. Thermal annealing was applied aiming to maintain the blend structure but improving the sensing reversibility of CPC sensors towards high vapor concentrations. Different sensing protocols were applied using acetone (good solvent for PS and PLA) and cyclohexane (good solvent for PS but poor solvent for PLA) vapors. Increasing acetone vapor concentration resulted in increased relative resistance change (Rrel) of CPCs. Saturated cyclohexane vapor resulted in lower response than nearly saturated acetone vapor. The thermal annealing at 150 °C did not change the blend morphology but increased the PLA crystallinity, making the CPC sensors more resistant to vapor stimulation, resulting in lower Rrel but better reversibility after vapor exposure.
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    MWCNT induced negative real permittivity in a copolyester of Bisphenol-A with terephthalic and isophthalic acids
    (Bristol : IOP Publ., 2020) Özdemir, Zeynep Güven; Daşdan, Dolunay Şakar; Kavak, Pelin; Pionteck, Jürgen; Pötschke, Petra; Voit, Brigitte; SüngüMısırlıoğlu, Banu
    In the present study, the negative real permittivity behavior of a copolyester of bisphenol-A with terephthalic acid and isophthalic acid (PAr) containing 1.5 to 7.5 wt% multi-walled carbon nanotubes (MWCNTs) have been investigated in detail. The structural and morphological analysis of the melt-mixed composites was performed by Fourier transform infrared spectroscopy using attenuated total reflection (FTIR-ATR), atomic force microscopy (AFM), X-ray diffraction (XRD), and light microscopy. The influences of the MWCNT filler on the AC impedance, complex permittivity, and AC conductivity of the PAr polymer matrix were investigated at different operating temperatures varied between 296 K and 373 K. The transition from a negative to positive real permittivity was observed at different crossover frequencies depending on the MWCNT content of the composites whereas pure PAr showed positive values at all frequencies. The negative real permittivity characteristic of the composites was discussed in the context of Drude model. © 2020 The Author(s). Published by IOP Publishing Ltd.
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    The Localization Behavior of Different CNTs in PC/SAN Blends Containing a Reactive Component
    (Basel : MDPI, 2021-3-1) Gültner, Marén; Boldt, Regine; Formanek, Petr; Fischer, Dieter; Simon, Frank; Pötschke, Petra
    Co-continuous blend systems of polycarbonate (PC), poly(styrene-co-acrylonitrile) (SAN), commercial non-functionalized multi-walled carbon nanotubes (MWCNTs) or various types of commercial and laboratory functionalized single-walled carbon nanotubes (SWCNTs), and a reactive component (RC, N-phenylmaleimide styrene maleic anhydride copolymer) were melt compounded in one step in a microcompounder. The blend system is immiscible, while the RC is miscible with SAN and contains maleic anhydride groups that have the potential to reactively couple with functional groups on the surface of the nanotubes. The influence of the RC on the localization of MWCNTs and SWCNTs (0.5 wt.%) was investigated by transmission electron microscopy (TEM) and energy-filtered TEM. In PC/SAN blends without RC, MWCNTs are localized in the PC component. In contrast, in PC/SAN-RC, the MWCNTs localize in the SAN-RC component, depending on the RC concentration. By adjusting the MWCNT/RC ratio, the localization of the MWCNTs can be tuned. The SWCNTs behave differently compared to the MWCNTs in PC/SAN-RC blends and their localization occurs either only in the PC or in both blend components, depending on the type of the SWCNTs. CNT defect concentration and surface functionalities seem to be responsible for the localization differences.
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    Bio-inspired deposition of electrochemically exfoliated graphene layers for electrical resistance heating applications
    (Bristol : IOP Publishing, 2020-12-4) Utech, Toni; Pötschke, Petra; Simon, Frank; Janke, Andreas; Kettner, Hannes; Paiva, Maria; Zimmerer, Cordelia
    Electrochemically exfoliated graphene (eeG) layers possess a variety of potential applications, e.g. as susceptor material for contactless induction heating in dynamic electro-magnetic fields, and as flexible and transparent electrode or resistivity heating elements. Spray coating of eeG dispersions was investigated in detail as a simple and fast method to deposit both, thin conducting layers and ring structures on polycarbonate substrates. The spray coating process was examined by systematic variation of dispersion concentration and volume applied to heated substrates. Properties of the obtained layers were characterized by UV-VIS spectroscopy, SEM and Confocal Scanning Microscopy. Electrical conductivity of eeG ring structures was measured using micro-four-point measurements. Modification of eeG with poly(dopamine) and post-thermal treatment yields in the reduction of the oxidized graphene proportion, an increase in electrical conductivity, and mechanical stabilization of the deposited thin layers. The chemical composition of modified eeG layer was analyzed via x-ray photoelectron spectroscopy pointing to the reductive behavior of poly(dopamine). Application oriented experiments demonstrate the direct electric current heating (Joule-Heating) effect of spray-coated eeG layers.
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    Blend Structure and n-Type Thermoelectric Performance of PA6/SAN and PA6/PMMA Blends Filled with Singlewalled Carbon Nanotubes
    (Basel : MDPI, 2021-4-28) Krause, Beate; Liguoro, Alice; Pötschke, Petra
    The present study investigates how the formation of melt-mixed immiscible blends based on PA6/SAN and PA6/PMMA filled with single walled nanotubes (SWCNTs) affects the thermoelectric (TE) properties. In addition to the detailed investigation of the blend morphology with compositions between 100/0 wt.% and 50/50 wt.%, the thermoelectric properties are investigated on blends with different SWCNT concentrations (0.25–3.0 wt.%). Both PA6 and the blend composites with the used type of SWCNTs showed negative Seebeck coefficients. It was shown that the PA6 matrix polymer, in which the SWCNTs are localized, mainly influenced the thermoelectric properties of blends with high SWCNT contents. By varying the blend composition, an increase in the absolute Seebeck coefficient, power factor (PF), and figure of merit (ZT) was achieved compared to the PA6 composite which is mainly related to the selective localization and enrichment of SWCNTs in the PA6 matrix at constant SWCNT loading. The maximum PFs achieved were 0.22 µW/m·K2 for PA6/SAN/SWCNT 70/30/3 wt.% and 0.13 µW/m·K2 for PA6/PMMA/SWCNT 60/40/3 wt.% compared to 0.09 µW/m·K2 for PA6/3 wt.% SWCNT which represent increases to 244% and 144%, respectively. At higher PMMA or SAN concentration, the change from matrix-droplet to a co-continuous morphology started, which, despite higher SWCNT enrichment in the PA6 matrix, disturbed the electrical conductivity, resulting in reduced PFs with still increasing Seebeck coefficients. At SWCNT contents between 0.5 and 3 wt.% the increase in the absolute Seebeck coefficient was compensated by lower electrical conductivity resulting in lower PF and ZT as compared to the PA6 composites.
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    Boron doping of SWCNTs as a way to enhance the thermoelectric properties of melt‐mixed polypropylene/SWCNT composites
    (Basel : MDPI, 2020) Krause, Beate; Bezugly, Viktor; Khavrus, Vyacheslav; Ye, Liu; Cuniberti, Gianaurelio; Pötschke, Petra
    Composites based on the matrix polymer polypropylene (PP) filled with single‐walled carbon nanotubes (SWCNTs) and boron‐doped SWCNTs (B‐SWCNTs) were prepared by melt‐mixing to analyze the influence of boron doping of SWCNTs on the thermoelectric properties of these nanocomposites. It was found that besides a significantly higher Seebeck coefficient of B‐SWCNT films and powder packages, the values for B‐SWCNT incorporated in PP were higher than those for SWCNTs. Due to the higher electrical conductivity and the higher Seebeck coefficients of B‐SWCNTs, the power factor (PF) and the figure of merit (ZT) were also higher for the PP/B‐SWCNT composites. The highest value achieved in this study was a Seebeck coefficient of 59.7 μV/K for PP with 0.5 wt% B‐SWCNT compared to 47.9 μV/K for SWCNTs at the same filling level. The highest PF was 0.78 μW/(m∙K2) for PP with 7.5 wt% B‐SWCNT. SWCNT macro‐ and microdispersions were found to be similar in both composite types, as was the very low electrical percolation threshold between 0.075 and 0.1 wt% SWCNT. At loadings between 0.5 and 2.0 wt%, B‐SWCNT‐based composites have one order of magnitude higher electrical conductivity than those based on SWCNT. The crystallization behavior of PP is more strongly influenced by B‐SWCNTs since their composites have higher crystallization temperatures than composites with SWCNTs at a comparable degree of crystallinity. Boron doping of SWCNTs is therefore a suitable way to improve the electrical and thermoelectric properties of composites. © 2020 by the authors.
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    Surface modification of MWCNT and its influence on properties of paraffin/MWCNT nanocomposites as phase change material
    (Hoboken, NJ [u.a.] : Wiley InterScience, 2020) Avid, Arezoo; Jafari, Seyed Hassan; Khonakdar, Hossein Ali; Ghaffari, Mehdi; Krause, Beate; Pötschke, Petra
    Multiwalled carbon nanotubes (MWCNTs) were modified by an organo-silane in order to improve their dispersion state and stability in paraffin wax. A family of paraffin-based phase change material (PCM) composites filled with MWCNTs was prepared with different loadings (0, 0.1, 0.5, and 1 wt%) of pristine MWCNTs and organo-silane modified MWCNTs (Si-MWCNT). Structural analyses were performed by means of Fourier transform infrared (FTIR), scanning electron microscopy (SEM), and rheological studies using temperature sweeps. Moreover, phase change transition temperatures and heat of fusion as well as thermal and electrical conductivities of the developed PCM nanocomposites were determined. The SEM micrographs and FTIR absorption bands appearing at approximately 1038 and 1112 cm−1 confirmed the silane modification. Differential scanning calorimetery (DSC) results indicate that the presence of Si-MWCNTs leads to slightly favorable enhancement in the energy storage capacity at the maximum loading. It was also shown that the thermal conductivity of the PCM nanocomposites, in both solid and liquid phases, increased with increasing the MWCNT content independent of the kind of MWCNTs by up to about 30% at the maximum loading of MWCNTs. In addition, the modification of MWCNTs made the samples completely electrically nonconductive, and the electrical surface resistivity of the PCMs containing pristine MWCNTs decreased with increasing MWCNTs loading. Furthermore, the rheological assessment under consecutive cyclic phase change demonstrated that the samples containing modified MWCNTs are more stable compared to the PCM containing pristine MWCNTs. © 2019 Wiley
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    Nitrogen-Doped Carbon Nanotube/Polypropylene Composites with Negative Seebeck Coefficient
    (Basel : MDPI, 2020) Krause, Beate; Konidakis, Ioannis; Arjmand, Mohammad; Sundararaj, Uttandaraman; Fuge, Robert; Liebscher, Marco; Hampel, Silke; Klaus, Maxim; Serpetzoglou, Efthymis; Stratakis, Emmanuel; Pötschke, Petra
    This study describes the application of multi-walled carbon nanotubes that were nitrogen-doped during their synthesis (N-MWCNTs) in melt-mixed polypropylene (PP) composites. Different types of N-MWCNTs, synthesized using different methods, were used and compared. Four of the five MWCNT grades showed negative Seebeck coefficients (S), indicating n-type charge carrier behavior. All prepared composites (with a concentration between 2 and 7.5 wt% N-MWCNTs) also showed negative S values, which in most cases had a higher negative value than the corresponding nanotubes. The S values achieved were between 1.0 µV/K and −13.8 µV/K for the N-MWCNT buckypapers or powders and between −4.7 µV/K and −22.8 µV/K for the corresponding composites. With a higher content of N-MWCNTs, the increase in electrical conductivity led to increasing values of the power factor (PF) despite the unstable behavior of the Seebeck coefficient. The highest power factor was achieved with 4 wt% N-MWCNT, where a suitable combination of high electrical conductivity and acceptable Seebeck coefficient led to a PF value of 6.1 × 10−3 µW/(m·K2). First experiments have shown that transient absorption spectroscopy (TAS) is a useful tool to study the carrier transfer process in CNTs in composites and to correlate it with the Seebeck coefficient.