Optimized Magnetodielectric Coupling on High-Temperature Polymer

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Optimized Magnetodielectric Coupling on HighTemperature Polymer-Based Nanocomposites Alberto Maceiras, Tiago Marinho, Jose Luis Vilas, Enrique CarboArgibay, Yury V. Kolen'ko, Senentxu Lanceros-Méndez, and Pedro Martins J. Phys. Chem. C, Just Accepted Manuscript • DOI: 10.1021/acs.jpcc.7b09395 • Publication Date (Web): 28 Nov 2017 Downloaded from http://pubs.acs.org on November 29, 2017

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The Journal of Physical Chemistry

Optimized Magnetodielectric Coupling On HighTemperature Polymer-Based Nanocomposites A. Maceirasa#, T. Marinhob#, José Luis Vilasa,c, Enrique Carbó-Argibayc, Yury Kolen'kod, P. Martinsb*, and S. Lanceros-Mendeza,e a. BCMaterials, Parque Científico y Tecnológico de Bizkaia, 48160-Derio, Spain. b. Centro/Departamento de Física, Universidade do Minho, 4710-057 Braga, Portugal. c. Macromolecular Chemistry Research Group (LABQUIMAC). Dept. of Physical Chemistry. Faculty of Science and Technology. University of the Basque Country (UPV/EHU), Spain. d. INL- International Iberian Nanotechnology Laboratory, Avenida Mestre José Veiga s/n 4715-330 Braga, Portugal e. IKERBASQUE, Basque Foundation for Science, 48013 Bilbao, Spain.

ACS Paragon Plus Environment

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ABSTRACT: CoFe2O4 (CFO) ferrite nanoparticles with an average size of 15 nm were synthesized by a hydrothermal method and used to develop magnetodielectric (MD) composites with the piezoelectric diamine 2CN/diamine 0CN as polymer matrix. It is shown that the dielectric constant, dielectric loss, and saturation magnetization values of the composites increase with the increasing CFO content, being 4.4, 0.01, and 12 emu.g-1, respectively, for the sample with 20 weight percentage (wt.%) of ferrite. Additionally the large MD effect response (MDE(%)=10.15) and magnetodielectric coefficient (γ)=5.8x10-2) allows a new physical insight on the magneto-mechano-electrical interaction between magnetostrictive CFO and the polymer matrix. Such high MD response, the highest reported for polymer-based composite materials, can support innovative applications in the areas of sensors, actuators, and filters, among others.


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1. Introduction Aromatic polyimides (PI) are characterized by a high dielectric response, thermal stability, and chemical/radiation resistance1. They are widely used as high-temperature insulators (T≤200ºC), circuit boards, packaging materials and dielectric interlayers in microelectronics. In addition, they are also applied in fuel cells or battery separation membranes. Another interesting feature is related to their photo-physical properties (absorption and fluorescence), with many applications in photovoltaic, electrochromic, photochromic, thermo-optical, and/or electroluminescent devices2-5. However, aromatic polyimides show certain characteristics such as stiffness, toughness, low resistance to fire/ignition and also their barrier properties that are inadequate unless they are modified through the addition of fillers leading to the development of composite or nanocomposite materials6. In particular, nanoparticles have been proved to be effective additives for introducing useful new properties or characteristics in aromatic polyimides 7. The variety of polyimide nanocomposites reported in the literature is very wide, due to the high number of potential applications. It is possible to find examples with carbon nanotubes (CNTs)8, clays9, graphene10 and with nanoparticles, such as copper (Cu)11, silver (Ag)7, barium titanate BaTiO

12

silicon dioxide SiO ,

13

titanium oxide TiO

14

or calcium carbonate CaCO

15

.

Nevertheless, it is difficult to find reports on the use of ferrite nanoparticles in polyimides for magnetism-based applications16-19. This type of composites is of particular interest, since ferrites are important magnetic materials with applications in the areas of sensors, electronics, communication, magnetic recording, microwave absorption-based devices, electrical and


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automobile industries as well as an increasing applicability in the biomedical and biotechnology fields20-23. Interestingly, ferrites can be used as a magnetostrictive phase in magnetoelectric (ME) composites, due to their high magnetostrictive coefficient (up to 200 ppm) and the high Curie (≈550ºC) temperatures among magnetic oxides24-26. A ME material is characterized by the variation of the electrical polarization as a response to an applied magnetic field or by the variation of the magnetization by the application of an electric field27. Since ME materials show an interesting interplay between the magnetic and electric properties of matter28-29, those materials have drawn increasing interest due to its potential applications in areas such as information storage, spintronics, sensors and actuators, among others.24, 30-31 ME materials can also reveal an important magnetodielectric (MD) coupling32, allowing the control of the dielectric properties by an applied magnetic field, expanding the range of applications to tunable filters or four-state memories, among others17, 33. In this work, composite films with 0–3 connectivity were prepared via in-situ polymerization, using spherical cobalt ferrite nanoparticles CoFe O as fillers and amorphous copolyimides, 3bis(3-aminophenoxy)benzene

(diamine

0CN)

and

1,3-bis-2-cyano-3-(3-

aminophenoxy)phenoxybenzene (diamine 2CN), as polymer matrix (Figure 1).


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Figure 1. Schematic representation of the two repetitive units of the copolyimide with the polar groups (above) and of a cobalt ferrite nanoparticle (below).

Such composition has been chosen to tackle the main challenge of the polymer-based nanocomposite with the highest magnetodielectric response reported in the literature17, namely, to increase the temperature range of application above 100ºC1, 17. The amorphous copolyimide, 2CN/2CN can be used as an alternative to the semicrystalline poly(vinylidene fluoride), PVDF, and family polymers34, allowing the use of polymer-based MD materials in high-temperature applications. Such polymer-based MD material can be used in a variety of forms, such as thin sheets or moulded shapes, and can exhibit improved mechanical properties. Those are obvious advantages when compared to ceramic-based materials24.

2. Experimental Details All chemicals were used as received from the suppliers, while CFO nanoparticles were synthesized as reported elsewhere35. The CFO particles are characterized by diameter=15±8nm, saturation magnetization of 61 emu·g-1 and ≈200 ppm magnetostriction25, 35.

2.1 Synthesis CFO/0CN2CN films were prepared from 4,4'-oxydiphthalic anhydride (ODPA) and a mixture of two aromatic diamines, 1,3-bis-2-cyano-3-(3-aminophenoxy)phenoxybenzene (diamine 2CN) and 1,3-Bis(3-aminophenoxy)benzene (diamine 0CN) with cobalt ferrite magnetic nanoparticles CoFe O , CFO following the procedure schematically indicated in Figure 2. Firstly (step 1), the nanoparticles were introduced into a vial containing dimethylacetamide (DMAc), and the vial


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was placed in an ultrasonic dispersion reactor for 60 min to ensure the uniform dispersion of the CFO on DMAc. Then (step 2), a mixture of the two aromatic diamines (50% mole percentage) was added and stirred until the complete dissolution of the diamines. The content of ferrite nanoparticles ranged from 0 to 20 weight percentage (wt.%).


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Figure 2. Schematic representation of the polyimide based nanocomposites fabrication procedure.

Later, 4,4'-oxydiphthalic anhydride (ODPA) was introduced to the mixture and (step 3) stirred at room temperature for 24h in a dry nitrogen atmosphere resulting in a viscous polyamic acid (PAA) solution containing CFO nanoparticles (Figure 3). Finally, (step 4), the mixture was cast in 150 µm thick films and (step 5) thermally imidizated1 according to the thermal treatment presented in Figure 3.

Copolyimide

200

Temperature (ºC)

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60


150 ∆ -H2O

100

Thermal imidization

50

Co(polyamic acid)

0

a)

24h

48h

25

50

48h

75

100

24h

125

150

Time (h)

b)

Figure 3. a) Thermal treatment used in the preparation of the CFO/P0CN2CN ME nanocomposites. b) TEM image of the synthesized CFO nanoparticles.

The ferrite nanoparticles (15 nm diameter, Figure 3)) content varied from 0 to 20 in weight percent (wt.%), 0 to 0.1 in volume fraction aiming to avoid losses in the flexibility of the material, large agglomerates and increased fragility.


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2.2 Characterization Transmission electron microscopy (TEM) images were obtained with a Titan ChemiSTEM transmission electron microscope (FEI Company), operated at 200 kV and having a resolution of 0.24 nm. The sample was prepared by dropping ultrasonically dispersed NPs onto a holey Cu carbon grid, followed by the evaporation of the solvent. Measurements of the electrical capacity and dielectric loss (tan δ) were performed with an automatic Quadtech 1929 Precision LCR meter with an applied voltage of 0.5 V in the frequency range from 1 Hz to 1 MHz. Such frequency range was selected to contain the resonance frequency of the polymer-based nanocomposites. In order to obtain a plane parallel condenser geometry, Au contacts with 5 mm diameter were deposited on both sides of the samples using a Polaron SC502 sputter coater. The real part of the dielectric constant, ε´, was determined from the electrical capacity (C) taking into account the geometry of the sample (thickness (d) and electrode area (A)) (equation 1):

ε' =

C×d A

(1)


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Room-temperature magnetic hysteresis loops were measured at room temperature using a Microsense 2.2 Tesla Vibrating Sample Magnetometer. With the purpose of obtaining the out-of-plane MD coefficient, a DC magnetic field was applied by an electromagnet, with a maximum value of 0.5 T, along the perpendicular direction of the electric polarization of the aromatic polyamides, i.e., parallel the surface of the composites. The induced change in the dielectric response of the composites was measured with an automatic Quadtech 1929 Precision LCR meter. The MD coupling was studied in magnetic fields up to 0.5 T, once for higher fields the piezomagnetic coefficient of CoFe2O4 decreases35, leading to a decrease in the MD response.

3. Results and discussion

The dielectric response and magnetic properties were studied first to investigate the effect of CFO loading within the nanocomposite (Figure 4). 5.2

0CN/2CN 5 wt.% 10 wt.% 20 wt.%

a)

4.4 4.0

4.5

0.0100

b)

ε'

4.0

3.6

tanδ

4.8

ε'

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60


0.0075

3.5

3.2 3.0

2.8 10k

100k

log10freq. (Hz)

1M

0

5

10

CFO wt.%

15

20

0.0050


9


-1

-1

c)

40

0

CFO powder 5 wt% 10 wt.% 20 wt.%

-40

-80 -2

MagnetizationSAT(emu.g )

80

Magnetization (emu.g )

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

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-1

0

uoH (T)

1

2

60

d)

40

20

0 0

20

40

60

80

100

CFO wt.% Figure 4. a) Frequency-dependent dielectric response for CFO/0CN2CN nanocomposites and; b) Room-temperature variation of the dielectric constant (squares) and dielectric loss (tanδ - circles) of the polymeric composites as a function of CFO content for a frequency of 5 kHz; c) Room temperature hysteresis loops for the pure ferrite nanoparticle powder and the CFO/0CN2CN nanocomposites; (d) Saturation magnetization values as a function of CFO content.

Figure 4a shows that the dielectric constant first fast decreases with increasing frequency, and, later, remains almost constant for frequencies higher than 10 kHz. This behaviour at the lower frequency range can be explained by the Maxwell–Wagner type polarization, in agreement with Koop's phenomenological models36. For all measured frequencies, it is observed an increase of the real part of the dielectric permittivity for the composites with respect to the neat 0CN2CN, reaching the maxim value in the composite with 20 wt.% of CFO. The dielectric losses also increases with increasing nanoparticle content reaching the maximum value 0.01 at 5 kHz in the 20 wt.% composite sample. Figure 4b exhibits the variation of the dielectric properties to the nanocomposites with CoFe2O4 wt.% at a frequency of 5 kHz and reveals that the addition of CFO nanoparticles in the


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0CN2CN matrix lead to a gradual increase of the real part of dielectric constant (from 2.8 to 4.4) and dielectric losses (from 0.006 to 0.010). The observed increase of both the dielectric constant and the dielectric losses related to the accumulation of interfacial charges in the nanoparticlepolymer interface, which is known as the Maxwell–Wagner–Sillars interfacial polarization phenomenon37-38. Regarding magnetic properties, all CFO/0CN2CN composite develop a ferromagnetic hysteresis loop with a coercivity of ≈0.20 T. Moreover an increase of the remanence and saturation magnetization values with increasing CFO loading is observed. The saturation magnetization values and shape of the measured hysteresis loops for the CFO/0CN2CN composite (Figure 4c) demonstrate that magnetic particles are randomly oriented within the polymer matrix. Additionally, the measured maximum magnetization of 12 emu·g−1 reveals that CoFe2O4 nanoparticles are well distributed and dispersed in the 0CN2CN matrix and that the maximum magnetization value is directly proportional to the amount of nanoparticles loaded into the polymer-based composite. The simultaneous existence of dielectric and ferromagnetic orders allows the coupling between electric polarization and magnetization. The coupling was measured by monitoring the variation of the dielectric constant with increasing magnetic field for the different composites (Figure 5).


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6

a)

4.0

OCN/2CN 5 wt.% 10 wt.% 20 wt.%

f=500 Hz 5

b) B=500mT

ε'

ε'

3.9 4

3.8 3 -500

-250

0

HDC (mT)

250

1k

500

20

25

c) 15

10k

100k

log10freq. (Hz)

d)

MDE (%)

10

B=400mT f=500 Hz

5

-19

15

10

CFO wt.%

15

-4 2

y=-0.85-7.4x10 x+1.1x10 x 2 r =0.93

10

f=500 Hz

0 5

10M

5

0 0

1M

Polynomial fit 20 wt.%

20

MDE (%)

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

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20

-500

-250

0

HDC (mT)

250

500

Figure 5. a) Dielectric constant as a function of the DC magnetic field at 500 Hz; b) MD (%) as a function of the frequency ; c) MD (%) as a function of the CFO content at 400 mT and 500 Hz; and d) Parabolic curve fitting of the MD (%) as a function of the DC magnetic field.

Figure 5a shows a decrease of the dielectric constant with increasing DC magnetic field modulus that reflects a decrease of the dipolar mobility as a consequence of increasing hardness of the composite resulting from the mechanical compressing induced by the magnetostrictive strain25. Similar to what happens to ME composites, there is an electromechanical resonance frequency at which the magnetodielectric effect (MD)


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coupling is optimized24, that was found to be 500 Hz (Figure 5b) for the CFO/0CN2CN MD composites. Such variation in the dielectric response with the applied magnetic field is usually quantified by the MD constant, defined as MD (%)=(|eH-e0|/ e0)x100, where eH and e0 are the dielectric constants with and without the applied magnetic fields, respectively17. The additional mechanical force that emerges from the magnetostrictive response of the CFO nanoparticles and decreases the dielectric response of the composite films is higher for higher CFO loadings, resulting in the increase of the MD (%) from 15.6 (for the wt.% sample) to 19.2 (for the 20 wt.% sample). The obtained MD(%) vs HDC curves (Figure 5d) can be fitted with a parabolic equation wherein the MD is proportional to the P2M2 term in a symmetry-allowed Ginzburg−Landau free energy (P and M are the electrical polarization and magnetization, respectively)39. Such quadratic dependence is observed in many ME materials39, where their thermodynamic potential (φ) can be written as:

β β' φ = φ0 + αP2 + P4 − PE+ α' M2 + M4 − MH+ γP2M2 2 2

(3)

where α, β, α’, β’ and γ are coupling coefficients39. A ferroelectromagnet material is described by a potential φ that can be used to quantify the effect of magnetic ordering on the dielectric susceptibility, and the term representing the exchange MD interaction γP2M2 is allowed in any ferroelectromagnet

33, 40

. In this way, the change of the relative

dielectric constant will be proportional to the square of the magnetic order parameter, i.e., ∆ε ≈ γM2 (Figure 6).


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0.075

5 wt.% y=0.058x-0.147

a)

r2=0.98 10 wt.% y=0.00508x-0.07

0.050

r2=0.990

20wt.% y=0.00114x-0.07 2

r =0.96

0.025

0.000

b)

γ (emu-2.g2)

0.075

(ε(H)-εε(0))//(ε(0))

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

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0.050

f=500 Hz 0.025

0.000

0

20

60

80

100

Magnetization2 (emu.g-1)2

0

5

10

15

CFO wt.%

20

Figure 6. (a) Variation of the dielectric constant versus (M)2 plot for the CFO/PVDF composites; (b) γ as a function of the CFO content at 500 mT and 5 kHz. Figure 6 shows that the resulting (|e(H)-e(0)|)/e(0) vs. M2 plots are properly fitted (r2≥0.96). The value of the MD interaction coefficient-γ- (slope of |(e(H) – e(0))| / e(0) vs. M2 plots) of the composite samples decreases from 0.058 emu2 g2 to 0.001 emu2 g2 with increasing ferrite content from 5 to 20 wt.%, suggesting a lower magnetodielectric coupling with increasing ferrite content. Similar decrease in the value of γ with the increasing filler content has already been reported in other polymer-based CFO MD composites, and is related to the increase of dielectric losses and the deterioration of mechanical connectivity with the increased ferrite loading that forms agglomerates.


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Table 1. Type of MD material, composition and highest coupling parameters found in the literature. Materials composition Type

Coupling (Temperature, HDC)

Ref.

Ferroelectric

Magnetic

MDE (%)

γ (emu-2.g2)

PVDF

CoFe2O4

4.2 (300 K, 0.5 T)

1.5x10-2

17

OCN2CN

CoFe2O4

19.15 (300K, 0.4T)

5.8 x10-2

Our

Polymer Composite

Table 1 compares the highest MD coupling parameters (MDE (%) and γ) reported in the literature with the ones reported in the present study. It was observed that the substitution of PVDF to OCN/2CN not only allows the use of the CFO/0CN2CN composite on hightemperature ( up to 200ºC)technological application but also shows improved MD effect (19.15% and 5.8×10–2 emu–2.g2). The high MD coupling leads to a high magnetic sensitivity that may promote the use of these materials on magnetic sensing-based applications, namely non-contacting location of moving objects, electronic guiding, aerospace and automotive industries41-42.

4. Conclusions Composite films were produced from dianhydride ODPA and a combination of two aromatic diamines, diamine 0CN and diamine 2CN, with 15 nm CFO magnetostrictive nanoparticles. The value of dielectric constant, dielectric loss and saturation magnetization of the polymer-based composites increase with increasing CFO content being maximized to 4.4, 0.01, and 12 emu.g-1, respectively, for the composite film with 20 wt.% of CFO. The linear fitting of the variation of the dielectric constant (∆ε) with the square of magnetization improved understanding of the MD physical process and allowed


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to determine the value of magnetoelectric interaction coefficient (γ)= 5.8x10-2, the highest reported on polymer-based MD materials. Thus, the large MD response and the thermal stability up to 200 ºC, as well as due to its simple processability and flexibility, makes this polymeric composite suitable for a wide range of applications such as magnetic field sensors, actuators and filters, among others.

AUTHOR INFORMATION Corresponding Author *P. Martins, Centro de Física, Universidade do Minho, 4710-057 Braga, Portugal; email: [email protected] Author Contributions The manuscript was written through contributions of all authors. All authors have given approval to the final version of the manuscript. ACKNOWLEDGMENT The authors thank the Portuguese Fundação para a Ciência e Tecnologia (FCT) for financial support under project PTDC/EEI-SII/5582/2014 and in the framework of the Strategic Funding UID/FIS/04650/2013. P. Martins acknowledges also support from FCT (SFRH/BPD/96227/2013 grant). Financial support from the Spanish Ministry of Economy and Competitiveness (MINECO) through the project MAT2016-76039-C4-3-R (AEI/FEDER, UE) (including the FEDER financial support) and from the Basque Government Industry Department under the ELKARTEK Program is also acknowledged.


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ABBREVIATIONS diamine 0CN , bis(3-aminophenoxy)benzene; diamine 2CN, 1,3-bis-2-cyano-3-(3aminophenoxy)phenoxybenzene; MD, Magnetodielectric; ME, Magnetoelectric. REFERENCES (1) Maceiras, A.; Martins, P.; Gonc¸alves, R.; Botelho, G.; Venkata Ramana, E.; Mendiratta, S. K.; San Sebastián, M.; Vilas, J. L.; Lanceros-Mendez, S.; León, L. M., High-Temperature Polymer Based Magnetoelectric Nanocomposites. Eur. Polym. J. 2015, 64, 224-228. (2) Mittal, K. L., Polyimides and Other High Temperature Polymers: Synthesis, Characterization and Applications. Volume 2; Taylor & Francis, 2003. (3) Luo, Y.; Sun, J.; Wang, J.; Jin, K.; He, F.; Fang, Q., A Novel Thermo-Polymerizable Aromatic Diamine: Synthesis and Application in Enhancement of the Properties of Conventional Polyimides. Macromol. Chem. Phys. 2016, 217, 856-862. (4) Zhao, Q.; Wang, X. Y.; Hu, Y. H., The Application of Highly Soluble Amine-Terminated Aromatic Polyimides with Pendent Tert-Butyl Groups as a Tougher for Epoxy Resin. Chin. J. Polym. Sci. (Eng. Ed.) 2015, 33, 1359-1372. (5) Zheng, F.; Van Sittert, C. G. C. E.; Lu, Q., A Computational Probe into the Dissolution Inhibitation Effect of Diazonaphthoquinone Photoactive Compounds on Positive Tone Photosensitive Polyimides. J. Phys. Chem. C 2017, 121, 1704-1714. (6) Alateyah, A. I.; Dhakal, H. N.; Zhang, Z. Y., Processing, Properties, and Applications of Polymer Nanocomposites Based on Layer Silicates: A Review. Adv. Polym. Tech. 2013, 32. (7) Wang, L.; Li, J.; Wang, D.; Wang, D.; Li, H., Preparation and Properties of Core–Shell Silver/Polyimide Nanocomposites. Polym. Bull. 2014, 71, 2661-2670. (8) Jiang, X.; Bin, Y.; Matsuo, M., Electrical and Mechanical Properties of PolyimideCarbon Nanotubes Composites Fabricated by in Situ Polymerization. Polymer 2005, 46, 74187424. (9) Tabatabaei-Yazdi, Z.; Mehdipour-Ataei, S., Poly(Ether-Imide) and Related Sepiolite Nanocomposites: Investigation of Physical, Thermal, and Mechanical Properties. Polym. Adv. Technol. 2015, 26, 308-314. (10) Ye, X.; Gong, P.; Wang, J.; Wang, H.; Ren, S.; Yang, S., Fluorinated Graphene Reinforced Polyimide Films with the Improved Thermal and Mechanical Properties. Compos. Part. A Appl. Sci. Manuf. 2015, 75, 96-103. (11) Choi, D. J.; Maeng, J. S.; Ahn, K. O.; Jung, M. J.; Song, S. H.; Kim, Y. H., Synthesis of Cu or Cu2o-Polyimide Nanocomposites Using Cu Powders and Their Optical Properties. Nanotechnology 2014, 25. (12) Hamciuc, E.; Hamciuc, C.; Bacosca, I.; Cristea, M.; Okrasa, L., Thermal and Electrical Properties of Nitrile-Containing Polyimide/Batio3 Composite Films. Polym. Compos. 2011, 32, 846-855. (13) Sakamoto, M.; Nohara, S.; Miyatake, K.; Uchida, M.; Watanabe, M.; Uchida, H., Effects of Incorporation of Sio2 Nanoparticles into Sulfonated Polyimide Electrolyte Membranes on Fuel Cell Performance under Low Humidity Conditions. Electrochim. Acta 2014, 137, 213-218.


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Optimized Magnetodielectric Coupling on High-Temperature Polymer

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