Journal of Magnetism and Magnetic Materials 279 (2004) 184–194

Characterization, electrical and magnetic properties of PVDF films filled with FeCl3 and MnCl2 mixed fillers
M. Abdelaziz
Department of Physics, Faculty of Science, Mansoura University, P.O. Box 19, 35516 Mansoura, Egypt Received 11 November 2003

Abstract Polyvinylidene fluoride (PVDF)/(x) FeCl3 (20Àx) MnCl2 films, where x=0.0%, 1%, 5%, 10%, 15%, 19%, and 20%, were prepared by the casting technique. Their thermal and crystalline structure, electric and magnetic properties, and ESR were examined. For thermal measurements, with increasing FeCl3 content, the melting temperature rarely changed while the thermal degradation temperature decreased. X-ray diffraction and infrared analysis show that the crystalline structure of PVDF changed drastically on addition of FeCl3, indicating that there are interactions between the PVDF matrix and FeCl3 and MnCl2. The optical and electrical measurements revealed a nearly monotonic behavior of optical gap and electrical resistivity as FeCl3 content increased. The direct current (DC) magnetic susceptibility indicates a predominantly ferromagnetic interaction between the magnetic ions at lower temperatures for all samples. The ESR spectra indicate the aggregated forms of Fe3+ and Mn2+ ions that confirm the results obtained from optical measurements and DC magnetic susceptibility. r 2004 Elsevier B.V. All rights reserved.
PACS: 71.20.R; 72.80.L; 75.50.P Keywords: Polyvinylidene fluoride; FeCl3–MnCl2 mixed fillers; Optical spectra; DC electric conduction; DC magnetic susceptibility and ESR

1. Introduction Polyvinylidene fluoride (PVDF) is a polycrystalline polymer started drawing scientific interest in the seventies, because of its extraordinary pyroend piezoelectric properties. These properties combined with both high elasticity and processing ability lend this material numerous technological applications [1]. Another feature that distinguishes PVDF from other polymers is its polymorphism, that is, it may present at least five crystalline phases,
E-mail address: (M. Abdelaziz).

namely a, b, d, g, and e [2]. Moreover, an increasing interest has been devoted to PVDF as electric and/or magnetic field sensors. For this application, PVDF was filled with transition metal halides [3]. Fillers are used in polymers for a variety of reasons: cost reduction, improved processing, density control, optical effect, thermal conductivity, control of thermal expansion, electrical properties, magnetic properties, flame retardancy and hardness, and tear resistance [4]. For example, in optical, electrical and magnetic applications, fillers such as FeCl3 and MnCl2 are used to provide better optical, electrical and magnetic properties.

0304-8853/$ - see front matter r 2004 Elsevier B.V. All rights reserved. doi:10.1016/j.jmmm.2004.01.091

2. Tw . Abdelaziz / Journal of Magnetism and Magnetic Materials 279 (2004) 184–194 185 Most studies considered the FeCl3 filler as an efficient electron acceptor and this was attributed to the formation of Fe2Cl2À [5]. 15% and 20%. at Tm peak is calculated using the Kissinger method [12] and the values of n. The order of reaction.ARTICLE IN PRESS M. 100 C. Differential thermal analysis The thermal behavior of PVDF films filled with (x) FeCl3 (20Àx) MnCl2. a nonlinear (even nonmonotonic) filling level (FL) dependence of the contents of the active structural forms was found. 10.2%. using an autorange multimeter (Keithley 175) with an accuracy of 0. we investigated the physical properties of PVDF films filled with FeCl3 [8] and MnCl2 [9]. the small endothermic peaks. 1. Sample preparation Films of PVDF filled with (x) FeCl3 (20Àx) MnCl2 were prepared by the casting method. by the twoprobe method. electrical and magnetic properties. The exothermic peak at Tc B100 C is attributed to the relaxation associated with the crystalline region. it was thought to use the intrasubstituted (x) FeCl3 (20Àx) MnCl2 mixed fillers. Results and discussion 3. 2. UV/VIS absorption spectra were measured in the wavelength range of 200–900 nm using a spectrometer (Perkin Elmer UV/VIS). An endothermic peak is observed at Tm B175 C which is attributed to the PVDF melting.0%. the optical absorption and magnetic properties of PVDF. observed at temperature 2. Different concentrations of the fillers were obtained. n. 5. The DC magnetic susceptibility was measured using the Faraday pendulum balance technique that provides an accuracy of better than 3. Mixtures of the dissolved polymer with mixed halides was placed in a glass dish and kept in a dry atmosphere at 323 K for 2 weeks to remove the solvent traces.1. where x=0%. Measurements DTA was carried out using an equipment type (Shimadzu DTA–50) with a measuring temperature . Experimental 2. However. The direct current (DC) electrical resistivity was measured. in a fair FL range. 1. From this figure. ESR spectra were measured with an X-band ESR spectrometer (Bruker. Therefore.1. 19 and 20 wt%. This exerted a strong influence on the electrical and magnetic properties of the filled PVDF films. In our previous works. was studied by DTA in the temperature range of 20–400 C. range of 20–400 C and a heating rate of 5 C minÀ1. The observed transitions can be assigned as follows: the Tw B30 C endotherm is due to the small amount of water that is always present in the conventional polymer unless it is carefully vacuum dried [11]. EMX) at room temperature using standard rectangular cavity (4102 ST) operating at 9. 5%. 175 C. 15. These investigations revealed that the used fillers modified the electric and magnetic properties of PVDF. the present work was devoted to investigate the effect of filling PVDF with a mixture of FeCl3 and MnCl2 on crystal structure. The X-ray diffraction (XRD) scans were obtained using a Seimens type F diffractometer with CuKa radiation and LiF monochromator. 10%. Manganese is well 4 known as a magneto-active multivalent element. The thickness of films was in the range of 100–150 mm. we observe that the filled PVDF films displayed three transitions at about 30 C. In addition. MnCl2 is considered as a good candidate for oneor two-dimensional phenomena [6] and for optical memory device [7]. another endothermic peak at B275 C is related to the thermal degradation of the polymer [10]. The infrared (IR) spectrophotometer (Perkin Elmer 883) was used for measuring the IR spectra in the wavenumber range of 4000–400 cmÀ1. Tc Tm and Td are listed in Table 1. see Fig. On the other hand. thus its halides can be used as fillers to modify the electric conduction. While searching for a linear (or monotonic) FL dependence of the electrical and magnetic properties. Dimethylformamide was used to dissolve the used materials. optical. where x ¼ 0:0. For x ¼ 0:0.7 GHz with a 100 kHz modulation frequency. 3.

3. 2.2 173. This indicates that all the reactants melted at Tm : It can be observed from Table 1 that the values of thermal degradation temperature Td decrease as the FeCl3 content increases.9 Tm ( C) 176.02 1. Table 1 FL dependence of: water (Tw ). Some of the observed band positions and their assignments are given in Table 3.4 31. Abdelaziz / Journal of Magnetism and Magnetic Materials 279 (2004) 184–194 3. ð1Þ Fig. It is clearly seen that all samples under investigation contain b. .3. 2.7 Td ( C) 375. It is suggested that the addition of FeCl3 decreases the thermal stability.2.8 n 1.02 oTm .02 1.2 174. The assignments [16] of these crystalline peaks are listed in Table 2. 1.7 99. are assigned to the ferroelectric to paraelectric phase transitions [13].5 330 310. X-ray diffraction XRD patterns of the present system are shown in Fig. for x ¼ 10% there are two endothermic peaks at B217 C and 253 C that may be attributed to the dehydration of MnCl2 Á 4H2O and/or FeCl3 Á H2O [15].5 32. The values of n were B1.4 103. XRD patterns of PVDF films with various mass fractions of (x) FeCl3 (20Àx) MnCl2.1 1.2 109.4 Tc ( C) 95.ARTICLE IN PRESS 186 M. the absorption coefficient aðnÞ at various frequency (n) values was calculated using the following formula: aðnÞ ¼ ln½t1 ðnÞ=t2 ðnފ=ðd1 À d2 Þ. The bands in the range of 370–500 nm are due to crystal field transitions of the tetrahedral isolated Fe3+ ions [17].0 5 10 15 20 Tw ( C) 43. This agrees with the results obtained by Zidan [14].06 1.9 31. Fig. Optical absorption The optical absorption spectra are carried out for PVDF films filled with two mixed fillers FeCl3 and MnCl2 and are shown in Fig. melting (Tm ) and thermal degradation (Td ) temperatures and order of reaction (n) FeCl3 (wt%) 0. Moreover. 3. Obviously.6 29. only the sample at x ¼ 10% contains a higher content of crystallinity.5 175.4 — 267.and a-crystalline phases except at x ¼5% and 20% contain the a-phase only. Interestingly. The DTA thermograms of PVDF filled with (x) FeCl3 (20Àx) MnCl2. crystalline (Tc ).6 173. the XRD patterns indicate the presence of a semicrystalline structure.5 112. Moreover.

The linear portion of Fig. (2 0 0) b (0 0 2) a (1 1 0) b. and 20%. 4. The spectra of all samples are nearly similar. It is clear that Eg exhibits a rapid increase up to x ¼ 5%: Then Eg increases linearly as FeCl3 content increases.8 20. in which the data can be fitted by the following relationship: Eg ¼ 0:01x þ 2:25.5 39.4. Main where t1 and t2 are the transmittances of two films (of the same concentration) with thicknesses d1 and d2 : Plotting ðahnÞ1=2 as a function of the photon . we obtain the curves shown in Fig.8 Assignments (1 1 0) b. Each curve exhibits a linear portion characterizing an optical gap Eg according to the Davis and Mott formula [18] aðnÞ ¼ B½ðhn À Eg Þ2 Š=hn. ð3Þ where x is the percent of FeCl3 content. 4 is used to obtain the value of the optical gap (namely Eg ). 10%. 5%.4 39. (2 0 0) b (0 0 2) a (0 0 2) a (1 1 0) b. IR transmittance Fig. 15%. where x=0%.0 39. Fig.0 2y (deg) 20. The UV/VIS absorption spectra of PVDF films filled with various FLs. The change of Eg may be attributed to the change of induced energy states due to the change of chilation mode at FL=5% [19].ARTICLE IN PRESS M.5 20. (2 0 0) b (0 0 2) a 15 20 (0 0 2) a 187 Table 3 The observed band positions and their assignments [17] for the tetrahedral Fe3+ FeCl3 (wt%) 5 Observed wavelength (nm) 307 370 409 398 361 409 295 358 397 424 316 364 406 Transitions 6A1g(S)4 4 5 10 T1g(P) T2g(D) 4 Eg(G) 4 4 10 15 T1g(P) T2g(D) 4 Eg(G) 4 4 T1g(P) T2g(D) 4 Eg(G) 4 A1g(G) 4 4 20 T1g(P) T2g(D) 4 Eg(G) energy hn (where h is Plank’s constant). Abdelaziz / Journal of Magnetism and Magnetic Materials 279 (2004) 184–194 Table 2 Assigned [16] X-ray diffraction peaks characterizing the crystalline PVDF phases FeCl3 (wt%) 0. 3.4 39. Fig. 3. 5 depicts the dependence of Eg on the FeCl3 content. 6 shows the plots of infrared absorption spectra for PVDF filled with (x) FeCl3 (20Àx) MnCl2.5 38. in the spectral range 4000–400 cmÀ1. ð2Þ where B is a constant.

temperature is shown as follows: r ¼ r0 expðEa =kTÞ. Fig. 8. The obtained results can be concluded as follows: (a) In Fig. the IR vibrational modes due to the aphase are 670. 5. (a. Further. Dependence of an optical energy gap Eg on FLs. The intensities of the bands at 840 cmÀ1 that refers to the b-phase. revealed a minimum value at x ¼ 10%: The change of the intensities of these certain IR absorption bands indicates a change of the chelation mode of FeCl3 and/or MnCl2 with the PVDF matrix. which refer to the g-phase and 1650 cmÀ1 that was . DC electrical resistivity As a function of temperature. Abdelaziz / Journal of Magnetism and Magnetic Materials 279 (2004) 184–194 Fig. It is noteworthy that the CQC mode and the h2h defects are suitable sites for polarons and/or bipolarons formation in the PVDF matrix. The IR vibrational modes due to the g-phase are identified at 950 cmÀ1 [20]. r.ARTICLE IN PRESS 188 M. 750 and 870 cmÀ1 and the vibrational modes due to the b-phase are 508 and 840 cmÀ1. The temperature dependence of the electrical resistivity was examined according to two basic existing theories. which refers to the head-to-head (h2h) and tail-to-tail (t2t) defects [22]. (2) 5%. and (5) 20%.5 vs. photon energy for various FLs: (1) 0. 950. 7. of the prepared samples was measured in the range 293–403 K. an Arrhenius plot of resistivity vs. (4) 15%. The structural modification can be identified by investigation of the FL dependence of certain IR absorption peaks 750. b) (ahn)0. 4. (3) 10%. T. 950 cmÀ1. ð4Þ characterizing peaks of PVDF can be noted. 3. the electrical resistivity.0%. and 1650 cmÀ1 depicted in Fig. which are Arrhenius and modified interpolaronhopping model. 840.5. assigned to the CQC stretching in the difluorinated alkenes [21] revealed minimum values at x ¼ 10%: The band at 750 cmÀ1.

Fig. The values of electrical resistivity. FL dependence of the IR peaks at: (a) 840 (J) and 1650 cmÀ1 (n). where r0 is the pre-exponential rate corresponding to 1=T ¼ 0:0. 6. (b) 750 (n) and 950 cmÀ1 (J). and activation energy Ea of the sample are determined through . Ea the activation energy for this thermal activated process and k the Boltzmann’s constant. IR transmission spectra of PVDF filled with various FLs. The variation in the logarithmic scale electrical resistivity values as a function of the reciprocal absolute temperature for samples is represented in Fig. 7. r0 . Abdelaziz / Journal of Magnetism and Magnetic Materials 279 (2004) 184–194 189 Fig.ARTICLE IN PRESS M. 8.

R0 ¼ ½3=ð4pCimp ފ1=3 is the typical separation between impurities whose concentration is Cimp . the electrical resistivity can be expressed as   kT R2 ðyp þ ybp Þ2 2BR0 0 r¼ exp . (4) 10%. monotonic decrease as FeCl3 content increases. the present results can be discussed on the basis of Kuivalainen et al. b) Reciprocal temperature dependence of log r on various FLs: (1) 0. Abdelaziz / Journal of Magnetism and Magnetic Materials 279 (2004) 184–194 Fig. 9.’s [24] modified interpolaron-hopping model. It can be clearly seen that all samples have semiconducting property because their resistivity decreases with an increase in temperature [23]. Bredas et al. (3) 5%. (a. Therefore. Dependence of activation energy Ea (J) and log r (n) on various FLs. the electrical activation energy of all samples has a positive value and has a maximum value at x ¼ 10%: Moreover.ARTICLE IN PRESS 190 M. In this temperature region. [25] reported that the extension of defect should be the same for polarons and bipolarons.0%. the logarithm of r0 shows a . (4) and are plotted in Fig. in which the conduction is attributed to phonon-assisted hopping between polaron and/or bipolaron-bound states in the polymer. B ¼ 1:39. 8. Fig. (6) 19%. z ¼ ðzJ z2 Þ1=3 is the average > decay length of a polaron and bipolaron wave function. (2) 1%. 9. respectively. respectively. yp and ybp are the concentrations of polarons and bipolarons. (b) The difluorinated alkenes (detected by IR analysis) indicating the presence of conjugated polyene and h2h defects may evidence the formation of polarons in the polymeric matrix. and (7) 20%. ð5Þ yp ybp x Ae2 gðTÞ2 x where A ¼ 0:45. According to this model. (5) 15%. and zJ and z> are the decay lengths parallel and perpendicular to the polymer chain. The electronic transition rate between polaron and bipolaron Eq.

6. The parameter zJ ¼ 1:06 nm while z> ¼ 0:22 nm [26]. shown in Table 4. (6) 19%. The FL dependences of meff are shown in Fig. can be noted in Fig. 10.6). (5) 15%. 13. It is remarkable that meff has a symmetric behavior for 0:0pxp10 and 10oxp20 which exhibits two minima at x ¼ 5% and 15% and a . equation meff ¼ 2:839½wm ðT À yp ފ1=2 ð8Þ where C is the Curie constant and yp is the paramagnetic Curie temperature. w. 11 shows the FL dependence of log r measured (and R0 calculated) at T ¼ 373 K. The log r and R0 have a slight change up to x ¼ 5% and a rapid decrease as FeCl3 content increases. using Eqs.0%. Abdelaziz / Journal of Magnetism and Magnetic Materials 279 (2004) 184–194 191 states can be expressed as gðTÞ ¼ 1:2  1017 ðT=300 KÞ11 : ð6Þ Using a computer-aided program. 10. indicating a semiconducting order. (2) 1%.9–4. On the other hand. 12.4 nm.ARTICLE IN PRESS M. Taking yp ¼ ybp for simplicity. (4) 10%.25 nm [28]). together with the to calculate the effective magnetic moment. which is an acceptable approximation [27]. for various FLs. meff . 3.7–9. (3) 5%. measured in the temperature range of 95–285 K for various FLs is shown in Fig. (a. ð7Þ Fig. It is clear that w obeys Curie–Weiss law [29] in which w ¼ C=ðT À yp Þ. we can obtain the values of the hopping distance R0 : A linear decrease of R0 as the temperature increases. Positive yp values. which depends on the interchain resonance energy and the interchain distance. and (7) 20%. This indicates that the concentration of thermally activated polarons (acting as hopping sites for the charge carriers) increases gradually as the temperature increases. the order of magnitude of r in the present system was adjusted with the impurity concentration Cimp . which were 4–18 times the monomer length (B0. which actually was the fitting parameter. Fig.b) Temperature dependence of hopping distance R0 for various FLs: (1) 0. The Curie–Weiss plots were used. where wm is the molar susceptibility of the used sample. This indicates that the electrical conduction is an interchain one-dimensional hopping type. the obtained values of R0 were in the range of 0. DC magnetic susceptibility The temperature dependence of the reciprocal values of the DC magnetic susceptibility.1. It is remarkable that the logarithm of resistivity is in the range of 6. (5. obtained for all samples under study suggest a ferromagnetic exchange interaction between the magnetic centers.

FL dependence of log r (K) and R0 (J) at T ¼ 373 K.7. These findings support the results obtained from optical measurements. The main characterizing features of PVDF. maximum value is observed at x ¼ 10%: The values of meff were in the range of 2. [30]. which correlated to the existence of Fe3+ and Mn2+ [29]. The FL dependences of A and DH are Fig. (2) 1%. 11. which is the ratio between the two halves of the Lorentzian signal.2 BM. and (7) 20%. It may be seen that A shows a monotonic increase as FeCl3 content increases for xX5%: On the other hand. 12. for the case of x ¼ 0:0% and 1% the spectra are characterized by unresolved 6-weak hyperfine lines superimposed on the lower field side of the Lorentzian signal arising from the hyperfine structure of the manganese nucleus (I ¼ 5=2) with an unpaired electron. shown in Fig. 15. 14. previously reported in Ref. Moreover. 3. (3) 5%. (5) 15% (6) 19%. (4) 10%. The FL dependence of the filler local structural can be clarified more explicitly with the aid of peak-to-peak separation (DH) of the Lorentzian signal and the symmetry factor (A).8–4. ESR The ESR spectra of PVDF filled with various fractions of FeCl3 and MnCl2 are observed in Fig. Temperature dependence of the reciprocal magnetic susceptibility for variously filled PVDF films: (1) 0. Abdelaziz / Journal of Magnetism and Magnetic Materials 279 (2004) 184–194 Fig. DH also shows a monotonic increase as FeCl3 content increases for .ARTICLE IN PRESS 192 M. The PVDF hyperfine spectra disappeared and strong Lorentzian signals were observed which may be ascribed mainly to the Fe3+ and/or Mn2+ cluster coupled by strong spin–spin interaction. indicating isolated Mn2+ in the ionmer [31]. are not observed in the present spectra.0%.

ARTICLE IN PRESS M. Based on the results of the present work. 15. These films can be used as microwave sensors. ESR spectra of PVDF filled with various FLs. it could be concluded that the mixture of Fe3+ and Mn2+ ions enhanced the magnetoactivity of PVDF. 14. Eg . electrical resistivity (r0 ).u. Abdelaziz / Journal of Magnetism and Magnetic Materials 279 (2004) 184–194 Table 4 FL dependence of paramagnetic Curie temperature yP FeCl3 0.3 39. it can serve as a piezoelectric and paramagnetic semiconductor . The linear dependence of an optical gap. maximum content bphase. Conclusion Fig. The fair intrasubstituted range of 0:0oxo20% revealed a linear or monotonic FL dependence on most of the investigated parameters such as optical energy gap (Eg ).2 x(wt%) 20 193 (x)FeCl3(20-x)MnCl2 Intensity (a.5 41. activation energy (Ea ).6 37. indicating the increase of dipolar interactions between the magnetic ions [13].) 19 15 10 5 1 0 0 1000 2000 3000 4000 5000 6000 Magnetic field (Gauss) Fig. FL dependence of meff (n).5 1. tetrahedral Fe3+ and maximum effective magnetic moment meff : Thus. 13. on FL indicates the improvement of an optical response. PVDF+(x) FeCl3 (20Àx) MnCl2. Fig. asymmetry factor (A) and peakto-peak separation (DH). 4.0 1 5 10 15 19 20 yp (K) 45. FL dependence of A (J) and DH (n).2 34 59. x > 0%. The sample of x ¼ 10% contains minimum structural defects.

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