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.

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.

2019, Pötschke; Petra, Krause, Beate, Luo, Jinji

Composites were prepared with polypropylene (PP) as the matrix and singlewalled CNTs (SWCNTs) of the type TUBALL from OCSiAl Ltd. as the conducting component by melt processing in a small-scale twin-screw compounder. In order to switch the typical p-type behavior of such composites from positive Seebeck coefficients (S) into n-type behavior with negative Seebeck coefficients, a non-ionic surfactant polyoxyethylene 20 cetyl ether (Brij58) was used and compared with a PEG additive, which was shown previously to be able to induce such switching. For PP-2 wt% SWCNT composites Brij58 is shown to result in n-type composites. The negative S values (up to −48.2 µV/K) are not as high as in the case of previous results using PEG (−56.6 µV/K). However, due to the more pronounced effect of Brij58 on the electrical conductivity, the achieved power factors are higher and reach a maximum of 0.144 µW/(m·K2) compared to previous 0.078 µW/(m·K2) with PEG. Dispersion improvement depends on the type of SWCNTs obtained by using varied synthesis/treatment conditions. Solution prepared composites of PEG with SWCNTs also have negative S values, indicating the donation of electrons from PEG to the SWCNTs. However, such composites are brittle and not suitable as thermoelectric materials.

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.

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

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.

2017, Socher, Robert, Krause, Beate, Pötschke, Petra

The aim of this study was to decrease the electrical percolation threshold of multiwalled carbon nanotubes (MWCNTs) in a polyamide 12 matrix by the use of additives. Different kinds of additives were selected which either interact with the π-system of the MWCNTs (imidazolium based ionic liquid (IL) and perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA)) or improve the MWCNT wettability (cyclic butylene terephthalate, CBT). The composites were melt mixed using a DACA microcompounder. The electrical percolation threshold for PA12/MWCNT without additives, measured on compression molded plates, was found between 2.0 and 2.25 wt%. With all used additives, a significant reduction of the electrical percolation threshold could be achieved. Whereas the addition of IL and CBT resulted in MWCNT percolation at around 1.0 wt%, a slightly higher percolation threshold between 1.0 and 1.5 wt% was found for PTCDA as an additive. Interestingly, the electrical resistivity at higher loadings was decreased by nearly two decades when using CBT and one decade after application of PTCDA, whereas IL did not contribute to lower values in this range. In all cases macrodispersion as assessed by light microscopy was not improved and even worse as compared to non-modified composites. In summary, the results illustrate that these kinds of additives are able to improve the performance of PA12 based MWCNT nanocomposites.

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.

2014, Krause, Beate, Pötschke, Petra, Gohs, U.

Polymer modification with high energy electrons (EB) is well established in different applications for many years. It is used for crosslinking, curing, degrading, grafting of polymeric materials and polymerisation of monomers. In contrast to this traditional method, electron induced reactive processing (EIReP) combines the polymer modification with high energy electrons and the melt mixing process. This novel reactive method was used to prepare polymer blends and composites. In this study, both methods were used for the preparation of polyethylene (PE)/ multiwalled carbon nanotubes (MWCNT) composites in the presence of a coupling agent. The influence of MWCNT and type of electron treatment on the gel content, the thermal conductivity, rheological, and electrical properties was investigated whereby as-grown and oxidised MWCNT were used. In the presence of a coupling agent and at an absorbed dose of 40 kGy, the gel content increased from 57 % for the pure PE to 74 % or 88 % by the addition of as-grown (Baytubes® C150P) or oxidised MWCNT, respectively. In comparison to the composites containing the as-grown MWCNTs, the use of the oxidised MWCNTs led to higher melt viscosity and higher storage modulus due to higher yield of filler polymer couplings. The melt viscosity increased due to the addition of MWCNT and crosslinking of PE. The thermal conductivity increased to about 150 % and showed no dependence on the kind of MWCNT and the type of electron treatment. In contrast, the lowest value of electrical volume resistivity was found for the non-irradiated samples and after state of the art electron treatment without any influence of the type of MWCNT. In the case of EIReP, the volume resistivity increased by 2 (as-grown MWCNT) or 3 decades (oxidised MWCNT) depending on the process parameters. © 2014 American Institute of Physics.

2017, Krause, Beate, Cohnen, A., Pötschke, Petra, Hickmann, T., Koppler, D., Proksch, B., Kersting, T., Hopmann, C.

In this study, composites based on polypropylene (PP) and different graphite fillers were melt mixed using small scale microcompounder Xplore DSM15 as well as lab-scale co-rotating twin screw extruder Coperion ZSK26Mc. The measurements of the electrical and thermal conductivity as well as mechanical properties of the composites were performed on pressed plates. It was found that the addition of graphite powders having different particle size distributions leads to different increases of the thermal conductivity. For synthetic graphite, the PP composites filled with TIMCAL Timrex® KS500 reached the highest value of thermal conductivity of 0.52 W/(m·K) at 10 vol% loading, whereas this composite was not electrical conductive. Furthermore, the influence of a styrene-ethylene-butylene-styrene block copolymer (SEBS) based impact modifier on the mechanical properties of PP filled with 80 wt% of different synthetic graphites was investigated. For that the proportion of SEBS in the PP component was varied systematically. The conductivities were influenced by the type of graphite and the content of impact modifier. The results indicate that the impact strength of the composite containing TIMCAL Timrex® KS300-1250 can be increased by approx. 100 % when replacing 50 wt% of the PP component by SEBS.