Abstract. Polymer matrix-TiO2 composites were prepared in three different filler concentrations. The electrical relaxation dynamics as well as the electrical conductivity of all samples were examined by means of Broadband Dielectric Spectroscopy (BDS) over a wide frequency and temperature range. The recorded relaxation response includes contributions from both the polymer matrix and the reinforcing phase. Two relaxation modes (β and γ) are observed in the low temperature region, which are attributed to the re-orientation of polar side groups of the matrix and rearrangement of small parts of the polymeric chain respectively. The α-relaxation and the Maxwell-Wagner-Sillars effect (MWS), attributed to the glassrubber transition of the polymeric matrix and to interfacial polarization phenomena respectively, are observed in the high temperature region. These two mechanisms are superimposed, thus a computer simulation procedure was followed in order to distinguish them. MWS effect becomes more pronounced with increasing concentration of the filler following an Arrhenius behaviour. The relaxation frequencies corresponding to α-mode follow the Vogel-Tamann-Fulcher (VTF) equation. An additional relaxation mode is recorded at relatively high temperatures and high frequencies. Its occurrence and dynamics are related to the presence and the concentration of the filler. Finally, the Direct Current (DC) conductivity follows the VTF equation.
The impact of nanomaterials and/or nanostructured materials is well known and well appreciated [1][2][3][4], mostly due to their potential applications based on their thermo-mechanical performance, flame resistance, electrical properties etc. Polymer matrix nanocomposites can be prepared by dispersing a small amount of nanometer size filler within the host medium. Rubber/Layered Silicate (LS) nanocomposites are increasingly attracting scientific and technological attention, because of the high reinforcing efficiency of the LS, even at very low loading. Polymer matrix/LS nanocomposites exhibit three different configurations: (a) microphase separated composites, where polymer matrix and layered silicates remain immiscible, (b) intercalated structures, where polymer molecules are inserted between the silicate layers, and (c) exfoliated structures, where individual silicate layers are dispersed in the polymer matrix. Polymer matrix nanocomposites are expected to be useful in replacing conventional insulating materials providing tailored performance, by simply controlling the type and the concentration of nanoinclusions [5][6][7][8]. 'Nanodielectrics' is a rather new term associating dielectrics with nanotechnology [9]. Nanoinclusions could be able to serve as inherent nanocapacitors. Charging and discharging 837 * Corresponding author, e-mail: G.C.Psarras@upatras.gr © BME-PT and GTE Abstract. Broadband Dielectric Spectroscopy (BDS) is employed in order to investigate relaxation phenomena occurring in natural rubber (NR), polyurethane rubber (PUR) and PUR/NR blend based nanocomposites, reinforced by 10 parts per hundred (phr) Layered Silicates (LS). Nanocomposites and matrices were examined under identical conditions in a wide frequency (10 -1 to 10 6 Hz) and temperature (-100 to 50°C) range. Experimental data are analyzed in terms of electric modulus formalism. The recorded relaxation phenomena include contributions from both the polymer matrices and the nanofiller. Natural rubber is a non-polar material and its performance is only slightly affected by the presence of layered silicates. Polyurethane rubber exhibits four distinct relaxation processes attributed, with ascending relaxation rate, to Interfacial Polarization (IP), glass/rubber transition (α-mode), local motions of polar side groups and small segments of the polymer chain (β, γ-mode). The same processes have been detected in all systems containing PUR. IP is present in all nanocomposites being the slowest recorded process. Finally, pronounced interfacial relaxation phenomena, occurring in the PUR+10 phr LS spectra, are attributed to nanoscale effects of intercalation and exfoliation.Keywords : polymer composites, nanocomposites, dielectric spectroscopy, relaxations, rubber eXPRESS Polymer Letters Vol.1, No.12 (2007) [837][838][839][840][841][842][843][844][845] Available online at www.expresspolymlett.com DOI: 10.3144/expresspolymlett.2007.116 under control the embedded in a matrix nanocapacitors, defines an energy storing procedure at the nanoscal...
The reduction in electronic recombination losses by the passivation of surfaces is a key factor enabling high‐efficiency solar cells. Here a strategy to passivate surface trap states of TiO2 films used as cathode interlayers in organic photovoltaics (OPVs) through applying alumina (Al2O3) or zirconia (ZrO2) insulating nanolayers by thermal atomic layer deposition (ALD) is investigated. The results suggest that the surface traps in TiO2 are oxygen vacancies, which cause undesirable recombination and high electron extraction barrier, reducing the open‐circuit voltage and the short‐circuit current of the complete OPV device. It is found that the ALD metal oxides enable excellent passivation of the TiO2 surface followed by a downward shift of the conduction band minimum. OPV devices based on different photoactive layers and using the passivated TiO2 electron extraction layers exhibit a significant enhancement of more than 30% in their power conversion efficiencies compared to their reference devices without the insulating metal oxide nanolayers. This is a result of significant suppression of charge recombination and enhanced electron extraction rates at the TiO2/ALD metal oxide/organic interface.
Polymer matrix‐ZnO microcomposites were prepared in different filler concentrations. The electrical relaxation dynamics of all samples was examined by means of broadband dielectric spectroscopy (BDS) over a wide temperature range. Two relaxation modes (namely β and γ), observed in the low temperature region, are attributed to the reorientation of small polar groups of the polymer matrix. Glass‐rubber transition (α‐mode) of the polymeric matrix and interfacial polarization phenomena are considered as responsible for the recorded relaxation processes in the high temperature region. An additional relaxation mode, named intermediate dipolar effect (IDE), is recorded at temperatures higher than −30 °C in all composites. Its occurrence and dynamics are related to the presence and concentration of the filler. IDE and α‐relaxation are observed in the same frequency and temperature range, leading to a mutual superposition. The two processes were distinguished following a simulation procedure employing the simultaneous fitting of two Havrilliak‐Negami terms and a third term describing the contribution of DC conductivity to dielectric losses. The temperature dependence of relaxation times for α‐mode follows the Vogel‐Tamann‐Fulcher equation, whereas IDE relaxation times follow unusual temperature dependence. The latter is discussed under the assumption of intrinsic interfacial polarization phenomena within ZnO crystal domains. © 2009 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 47: 445–454, 2009
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