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Lightweight polymer-carbon composite current collector for lithium-ion batteries

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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Electrical and melt rheological characterization of PC and co-continuous PC/SAN blends filled with CNTs: Relationship between melt-mixing parameters, filler dispersion, and filler aspect ratio

2018, Liebscher, Marco, Domurath, Jan, Krause, Beate, Saphiannikova, Marina, Heinrich, Gert, Pötschke, Petra

Electrical and melt rheological properties of melt-mixed polycarbonate (PC) and co-continuous PC/poly(styrene–acrylonitrile) (SAN) blends with carbon nanotubes (CNTs) are investigated. Using two sets of mixing parameters, different states of filler dispersion are obtained. With increasing CNT dispersion, an increase in electrical resistivity near the percolation threshold of PC–CNT composites and (PC + CNT)/SAN blends is observed. This suggests that the higher mixing energies required for better dispersion also result in a more severe reduction of the CNT aspect ratio; this effect was proven by CNT length measurements. Melt rheological studies show higher reinforcing effects for composites with worse dispersion. The Eilers equation, describing the melt viscosity as function of filler content, was used to fit the data and to obtain information about an apparent aspect ratio change, which was in accordance with measured CNT length reduction. Such fitting could be also transferred to the blends and serves for a qualitatively based discussion. © 2017 Wiley Periodicals

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Extruded polycarbonate/Di-Allyl phthalate composites with ternary conductive filler system for bipolar plates of polymer electrolyte membrane fuel cells

2019, Naji, Ahmed, Krause, Beate, Pötschke, Petra, Ameli, Amir

Here, we report multifunctional polycarbonate (PC)-based conductive polymer composites (CPCs) with outstanding performance manufactured by a simple extrusion process and intended for use in bipolar plate (BPP) applications in polymer electrolyte membrane (PEM) fuel cells. CPCs were developed using a ternary conductive filler system containing carbon nanotube (CNT), carbon fiber (CF), and graphite (G) and by introducing di-allyl phthalate (DAP) as a plasticizer to PC matrix. The samples were fabricated using twin-screw extrusion followed by compression molding and the microstructure, electrical conductivity, thermal conductivity, and mechanical properties were investigated. The results showed a good dispersion of the fillers with some degree of interconnection between dissimilar fillers. The addition of DAP enhanced the electrical conductivity and tensile strength of the CPCs. Due to its plasticizing effect, DAP reduced the processing temperature by 75 °C and facilitated the extrusion of CPCs with filler loads as high as 63 wt% (3 wt% CNT, 30 wt% CF, 30 wt% G). Consequently, CPCs with the through-plane electrical, in-plane electrical and thermal conductivities and tensile strength of 4.2 S cm-1, 34.3 S cm-1, 2.9 W m-1 K-1, and 75.4 MPa, respectively, were achieved. This combination of properties indicates the potential of PC-based composites enriched with hybrid fillers and plasticizers as an alternative material for BPP application.

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Melt-mixed thermoplastic composites containing carbon nanotubes for thermoelectric applications

2016, Luo, Jinji, Krause, Beate, Pötschke, Petra

Flexible thermoelectric materials are prepared by melt mixing technique, which can be easily scaled up to industrial level. Hybrid filler systems of carbon nanotubes (CNTs) and copper oxide (CuO), which are environmental friendly materials and contain abundant earth elements, are melt mixed into a thermoplastic matrix, namely polypropylene (PP). With the CNT addition, an electrical network could be built up inside the insulating PP for effective charge transport. The effect of CuO addition is determined by the corresponding CNT concentration. At high CNT concentration, largely above the percolation threshold (φc, ca. 0.1 wt%), the change in the TE properties is small. In contrast, at CNT concentration close to φc, the co-addition of CuO could simultaneously increase the electrical conductivity and Seebeck coefficient. With 5 wt% CuO and 0.8 wt% CNTs where a loose percolated network is formed, the Seebeck coefficient was increased from 34.1 µV/K to 45 µV/K while the electrical conductivity was from 1.6 × 10−3 S/cm to 3.8 × 10−3 S/cm, leading to a power factor of 9.6 × 10−4 µW/mK2 (cf. 1.8 × 10−4 µW/mK2 for the composite with only 0.8 wt% CNTs).

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Influence of talc with different particle sizes in melt-mixed LLDPE/MWCNT composites

2013, Müller, Michael Thomas, Dreyße, Janine, Häußler, Liane, Krause, Beate, Pötschke, Petra

Linear low-density polyethylene (LLDPE) was melt-mixed with multiwalled carbon nanotubes (MWCNTs) and varying amounts of three different kinds of talc (phyllo silicate), each with a different particle size distribution, to examine the effect of these filler combinations with regards to the electrical percolation behavior. The state of the filler dispersion was assessed using transmission light microscopy and electron microscopy. The use of talc as a second filler during the melt mixing of LLDPE/MWCNT composites resulted in an improvement in the dispersion of the MWCNTs and a decrease of the electrical percolation threshold. Talc with lower particle sizes showed a more pronounced effect than talc with larger particle sizes. However, the improvement in dispersion was not reflected in the mechanical properties. Modulus and stress values increase with both, MWCNT and talc addition, but not in a synergistic manner. The crystallization behavior of the composites was studied by differential scanning calorimetry to determine its potential influence on the electrical percolation threshold. It was found that the crystallinity of the matrix increased slightly with the addition of talc but no further increments were observed with the incorporation of the MWCNTs. © 2013 Wiley Periodicals, Inc.

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Graphite modified epoxy-based adhesive for joining of aluminium and PP/graphite composites

2020, Rzeczkowski, P., Pötschke, Petra, Fischer, M., Kühnert, I., Krause, Beate

A graphite-modified adhesive was developed in order to simultaneously enhance the thermal conductivity and the strength of an adhesive joint. The thermal conductivity through the joint was investigated by using highly filled PP/graphite composite substrates, which were joined with an epoxy adhesive of different layer thicknesses. Similar measurements were carried out with a constant adhesive layer thickness, whilst applying an epoxy adhesive modified with expanded graphite (EG) (6, 10, and 20 wt%). By reducing the adhesive layer thickness or modifying the adhesive with conductive fillers, a significant increase of the thermal conductivity through the joint was achieved. The examination of the mechanical properties of the modified adhesives was carried out by tensile tests (adhesive only), lap-shear tests, and fracture energy tests (mode 1) with aluminium substrates. Modification of the adhesive with EG led to an increase of the tensile lap-shear strength and the adhesive fracture energy (mode 1) of the joint. In addition, burst pressure tests were performed to determine the strength of the joint in a complex component. The strength of the joint increased with the graphite content in the PP substrate and in the epoxy adhesive.

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Aspect ratio effects of multi-walled carbon nanotubes on electrical, mechanical, and thermal properties of polycarbonate/MWCNT composites

2014, Guo, Jiaxi, Liu, Yanjun, Prada-Silvy, Ricardo, Tan, Yongqiang, Azad, Samina, Krause, Beate, Pötschke, Petra, Grady, Brian P.

Two multi-walled carbon nanotubes (MWCNTs) having relatively high aspect ratios of 313 and 474 with approximately the same diameter were melt mixed with polycarbonate (PC) in a twin-screw conical micro compounder. The effects of aspect ratio on the electrical, mechanical, and thermal properties of the PC/MWCNT composites were investigated. Electrical conductivities and storage moduli of the filled samples are found to be independent of the starting aspect ratio for these high aspect ratio tubes; although the conductivities and storage moduli are still significantly higher than values of composites made with nanotubes having more commercially common aspect ratios of ∼100. Transmission electron microscopy results suggest that melt-mixing reduces these longer nanotubes to the same length, but still approximately two times longer than the length of commercially common aspect ratio tubes after melt-mixing. Molecular weight measurements show that during melt-mixing the longer nanotubes significantly degrade the molecular weight of the polymer as compared to very similar nanotubes with aspect ratio ∼100. Because of the molecular weight reduction glass transition temperatures predictably show a large decrease with increasing nanotube concentration. © 2013 Wiley Periodicals, Inc.

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Electrically conductive and piezoresistive polymer nanocomposites using multiwalled carbon nanotubes in a flexible copolyester: Spectroscopic, morphological, mechanical and electrical properties

2022, Dhakal, Kedar Nath, Khanal, Santosh, Krause, Beate, Lach, Ralf, Grellmann, Wolfgang, Le, Hai Hong, Das, Amit, Wießner, Sven, Heinrich, Gert, Pionteck, Jürgen, Adhikari, Rameshwar

Nanocomposites of multiwalled carbon nanotubes (MWCNTs) with poly(butylene adipate-co-terephthalate) (PBAT), a flexible aromatic–aliphatic copolyester, were prepared by melt mixing followed by compression moulding to investigate their spectroscopic, morphological, mechanical and electrical properties. A comparison of the Fourier transform infrared (FTIR) spectra of the neat polymer matrix and the composites showed no difference, implying a physical mixing of the matrix and the filler. A morphological investigation revealed the formation of a continuous and interconnected MWCNT network embedded in the polymer matrix with partial agglomeration. Increasing Martens hardness and indentation modulus and decreasing maximum indentation depth with increasing filler concentration demonstrated the reinforcement of the polymer by the MWCNTs. A volume resistivity of 4.6 × 105 Ω cm of the materials was achieved by the incorporation of only 1 wt.-% of the MWCNTs, which confirmed a quite low percolation threshold (below 1 wt.-%) of the nanocomposites. The electrical volume resistivity of the flexible nanocomposites was achieved up to 1.6 × 102 Ω cm, depending on the filler content. The elongation at the break of the nanocomposites at 374% and the maximum relative resistance changes (ΔR/R0) of 20 and 200 at 0.9 and 7.5% strains, respectively, were recorded in the nanocomposites (3 wt.-% MWCNTs) within the estimated volume resistivity range. A cyclic strain experiment shows the most stable and reproducible ΔR/R0 values in the 2%–5% strain range. The electrical conductivity and piezoresistivity of the investigated nanocomposites in correlation with the mechanical properties and observed morphology make them applicable for low-strain deformation-sensing.

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Experimental and computational analysis of thermoelectric modules based on melt-mixed polypropylene composites

2023, Doraghi, Qusay, Żabnieńska-Góra, Alina, Norman, Les, Krause, Beate, Pötschke, Petra, Jouhara, Hussam

Researchers are constantly looking for new materials that exploit the Seebeck phenomenon to convert heat into electrical energy using thermoelectric generators (TEGs). New lead-free thermoelectric materials are being investigated as part of the EU project InComEss, with one of the anticipated uses being converting wasted heat into electric energy. Such research aims to reduce the production costs as well as the environmental impact of current TEG modules which mostly employ bismuth for their construction. The use of polymers that, despite lower efficiency, achieve increasingly higher values of electrical conductivity and Seebeck coefficients at a low heat transfer coefficient is increasingly discussed in the literature. This article presents two thermoelectric generator (TEG) models based on data previously described in the literature. Two types of designs are presented: consisting of 4- and 49-leg pairs of p- and n-type composites based on polypropylene melt-mixed with single-walled carbon nanotubes. The models being developed using COMSOL Multiphysics software and validated based on measurements carried out in the laboratory. Based on the results of the analysis, conductive polymer composites employing insulating matrices can be considered as a promising material of the future for TEG modules.