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IEEE - ICSD 2010 Potsdam, Germany, 04-09 July 2010

DIELECTRIC PROPERTIES OF LDPE-SiO2 NANOCOMPOSITES


Florin Ciuprina1), Ilona Plesa1), Petru V. Notingher1),
Pascal Rain2),
Traian Zaharescu3) and Denis Panaitescu4)
1)

POLITEHNICA University of Bucharest, ELMAT, Splaiul Independentei 313, Bucharest, Romania, florin@elmat.pub.ro
2) Grenoble Electrical Engineering Laboratory (G2Elab), University of Grenoble, G-INP, CNRS, UJF Grenoble, France
3) ICPE-CA, Bucharest, Romania
4) National Institute of Research and Development in Chemistry and Petrochemistry, ICECHIM, Bucharest, Romania

GOAL

Dielectric spectroscopy
3.3

LDPE-SiO2 nanocomposites;

Plaques of square shape (10 x 10 cm2) with the thickness of 0.5-0.6 mm;
Manufacturing by direct mixing method;
Nanofiller: SiO2 nanoparticles of average diameter 15 nm and content
2, 5 and 10 wt.%;
Maleic anhydride graft polyethylene (MA-PE) used for a better dispersion
of the nanoparticles and for a better compatibility nanofiller - polymer
matrix.

0.05

T = 300 K

Unfilled
2% nano-SiO2
5% nano-SiO2
10% nano-SiO 2

3.1
3.0
2.9

Tan Delta

2.8
2.7
2.6
2.5
2.4
2.2

10

2.30

0.0030
300 K
310 K
320 K
330 K
340 K
350 K

44

Cristallinity index [%]

X-Ray Diffraction

42

2.5

10

10

10

10

LDPE unfilled
300 K
310 K
320 K
330 K
340 K
350 K

LDPE-SiO2
5 % filler concentration

300 K
310 K
320 K
330 K
340 K
350 K

0.020

2.4
2.3

0.015
0.010
0.005

2.2
2.1
10-3 10-2 10-1 100 101

102 103 104

105 106

3.2

107

0.000
10-3 10-2 10-1 100

Frequency [Hz]

300 K
310 K
320 K
330 K
340 K
350 K

3.0

101

102

103 104

105 106

LDPE-SiO2
10 % filler concentration

300 K
310 K
320 K
330 K
340 K
350 K

0.05
0.04

2.8
2.6

107

Frequency [Hz]
0.06

LDPE-SiO2
10 % filler concentration

0.03
0.02

2.4

0.01
2.2
102 103 104

105 106

107

0.00
-3
-2
-1
0
1
10 10 10 10 10

10

10

10

Frequency [Hz]

10

10

10

Fig. 6 Frequency variation of tan at temperatures


from 300 to 350 K with a step size of 10 K:
(a) unfilled LDPE, (b) LDPE-SiO2 with 5% filler
content, (c) LDPE-SiO2 with 10% filler content.

0.08

10

250 K
260 K
270 K
280 K
290 K
300 K

0.07
0.06

Tan Delta

6
-1

CL Intensity (Hz.g ) * 10

0.0010

0.05

0.04
0.03
0.02

0.01

0.00
-3
-2
-1
0
1
2
3
4
5
6
7
10 10 10 10 10 10 10 10 10 10 10

2
0

10

0.025

Tan Delta

Relative Permittivity (real part)

2.6

Unfilled
2 % nan o-SiO 2
5 % nan o-SiO 2
10 % na no-SiO 2

10

Frequency [Hz]

300 K
310 K
320 K
330 K
340 K
350 K

Fig. 2 Cristallinity index vs. SiO2 concentration


12

10

0.0015

0.030

LDPE-SiO2
5 % filler concentration

SiO2 concentration [%]

Chemiluminescence

10

0.0000
10-3 10-2 10-1 100 101 102 103 104 105 106 107

Fig. 5 Frequency variation of r' at temperatures


from 300 to 350 K with a step size of 10 K:
(a) unfilled LDPE, (b) LDPE-SiO2 with 5% filler
content, (c) LDPE-SiO2 with 10% filler content

36

0.0005

Frequency [Hz]

38

10

2.15

10-3 10-2 10-1 100 101

40

-1

0.0020

Tan Delta

RESULTS

10

0.0025

2.20

Relative Permittivity (real part)

LUMIPOL 3 (SAS, Slovak Republik);


Isothermal (180 0C) and nonisothermal conditions.

-2

10

Frequency [Hz]

LDPE unfilled

2.25

3.4

Chemiluminescence:

-3

Fig. 4 Frequency variation of r' (a) and of tan (b) for LDPE-SiO2 nanocomposites with
different filler concentrations, at 300 K.

2.7

Novocontrol ALPHA-A Analyzer in combination with ZGS Sample Cell;


Frequency range: 10-2 106 Hz;
Temperature range: 250 - 350 K.

0.02

Frequency [Hz]

Fig. 1 Setup for nanocomposite realization

Dielectric spectroscopy:

0.03

0.00

2.1
-3
-2
-1
0
1
2
3
4
5
6
7
10 10 10 10 10 10 10 10 10 10 10

Frequency [Hz]

DRON-2.0 diffractometer (CuK radiation, Ni filter);


Bragg-Brentano geometry (reflexion).

Unfilled
2% nano-SiO2
5% nano-SiO2
10% nano-SiO 2

0.01

2.3

2.10
10-3 10-2 10-1 100 101 102 103 104 105 106 107

X-Ray Diffraction:

T = 300 K

0.04

Tan Delta

Samples:

Relative Permittivity (real part)

EXPERIMENTAL

3.2

Relative Permittivity (real part)

Study of the dielectric behaviour of LDPE-SiO2 nanodielectrics, at


different frequencies and temperatures.

Frequency [Hz]
0

100

200
300
Time (min)

400

Fig. 7 Frequency variation of tan at temperatures from 250 to 300 K


with a step size of 10 K for LDPE-SiO2 naonocomposite with 10%
filler content.

500

Fig. 3 Isothermal chemiluminograms for


LDPE- SiO2 nanodielectrics

CONCLUSIONS
The results indicate an -relaxation process which is enhanced by the filler
concentration and shifted to higher frequencies with the increasing
temperature.

The absorbed water molecules in the LDPE-SiO2 nanocomposites influence


the relaxation frequency.

The charges at the nanofiller-polymer interface are thought to be the main


responsible for this behaviour.

The thermal stability of the polyethylene is improved by the nanosilica filler.

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