Abstract
Hard magnetic particle–based magnetorheological elastomers are novel magnetoactive materials in which, unlike the soft particle–based magnetorheological elastomers, the particles provide magnetic poles inside the elastomeric medium. Therefore, the stiffness of the hard magnetic particle–based magnetorheological elastomers can be increased or decreased by applying the magnetic field in the same or opposite direction as the magnetic poles, respectively. In the present work, the viscoelastic properties of hard magnetic particle–based magnetorheological elastomers operating in shear mode have been experimentally characterized. For this purpose, hard magnetic particle–based magnetorheological elastomers with 15% volume fraction of NdFeB magnetic particles have been fabricated and then tested under oscillatory shear motion advanced rotational magneto-rheometer to investigate their viscoelastic behavior under varying excitation frequency and magnetic flux density. The influence of the shear strain amplitude and driving frequency is examined under various levels of applied magnetic field ranging from −0.2 to 1.0 T. Finally, a field-dependent phenomenological model has been proposed to predict the variation of storage and loss moduli of hard magnetic particle–based magnetorheological elastomers under varying excitation frequency and applied magnetic flux density. The results show that the proposed model can accurately predict the viscoelastic behavior of hard magnetic particle–based magnetorheological elastomers under various working conditions.
Keywords
1. Introduction
Magnetorheological elastomers (MREs) are an emerging class of smart materials that their properties can be changed in a reversible manner under the application of an external magnetic field (Dargahi et al., 2019). The viscoelastic properties of MREs, namely, the storage and loss moduli, can be controlled in a rapid, continuous, and reversible manner by applying an external magnetic field (Ginder et al., 1999; Woods et al., 2007). MREs are used in various applications such as adaptive tuned vibration absorber (Qian et al., 2017), smart material–based isolators (Li et al., 2013), vehicle seat suspension (Du et al., 2011), microcantilevers (Lee et al., 2014), microvibrations (Ying et al., 2013), sensors (Wang et al., 2009), touch-screen displays (Chen et al., 2019), magnetometers (Du and Chen 2012), prosthetic devices (Jonsdottir et al., 2015), noise barrier systems (Farshad and Le Roux 2004), sandwich beams (Zhou and Wang, 2005), negative changing stiffness isolators (Sun et al., 2015), bumper of a vehicle (Bogdanov et al., 2009), and particularly in shifting the fundamental frequency of controlled devices.
MREs consist of an elastomeric matrix such as silicon rubber impregnated with micron-sized iron particles and can be classified according to several parameters like particle types, matrix, structure, and distribution of particles. In terms of distribution of particles, MREs divided into isotropic and anisotropic (Asadi Khanouki et al., 2019; Lu et al., 2012). Curing the mixture of the elastomer and iron particles in the absence and presence of the applied magnetic field results in isotropic and anisotropic MREs, respectively. In terms of particle types, particles are divided into soft and hard magnetic particles. Soft magnetic particles, such as carbonyl iron (CI) powders, have been widely used in magnetorheological (MR) materials, because of their high saturation magnetization and low remanence (Zhao et al., 2017). Recently, particles of high-coercivity ferromagnetic materials, or hard magnetic materials, such as neodymium–iron–boron (NdFeB) have been embedded in soft matrices. The high remnant characteristics of hard magnetic materials allow them to retain high residual magnetic flux density even in the absence of magnetic fields once they are magnetically saturated (Wen et al., 2017). One of the main problem with soft MREs is that their storage modulus can be only increased by applying external magnetic field irrespective of the applied magnetic field direction which limits their potential applications in adaptive MRE–based devices such as MRE-based vibration absorbers and isolators in which the reduction in the stiffness (or natural frequency) may be required to enhance their control authority. In order to alleviate this issue, an initial magnetic field may be applied either by electromagnet or permanent magnet (Yang et al., 2014) so that the stiffness could be decreased from the initial value by decreasing the applied magnetic field. However, this approach is not effective due to the added cost, weight, and power consumption associated with generation of the initial magnetic field (Wen et al., 2017). Thus, hard magnetic particle–based MREs (H-MREs) capable of providing negative MR effect and reducing their stiffness seem to be a viable technology to considerably enhance the bandwidth of the MRE-based adaptive devices.
The actuation capability and viscoelastic properties of H-MREs have been recently investigated. Koo et al. (2012) concluded that H-MREs are capable of being used as bending-type actuators. They also measured the block force and tip displacement of the samples to characterize actuation properties of H-MREs. Borin et al. (2013) experimentally determined the tensile modulus of H-MREs and considered the influence of the remanence magnetization on the tensile modulus. The viscoelastic properties of H-MREs also investigated by Stepanov et al. (2012, 2014), and it was shown that the modulus could be changed in two ways (to increase and decrease) by applying the magnetic field in opposite directions. Moreover, they concluded that the MR effect of such material is lower than that in magnetically soft composites. Stepanov et al. (2017a) also investigated the mechanism of the re-magnetization of the magnetoactive elastomers with hard magnetic fillers. They explained that this mechanism depends on the re-magnetizing of the magnetic filler and mechanical rotation of particles inside the polymer matrix. Moreover, they investigate the potential of the hybrid magnetic elastomers as active and passive dampers (Stepanov et al., 2017b). Kramarenko et al. (2015) synthesized MREs based on a silicone matrix with magnetically hard NdFeB particles, and they concluded that the response of MRE samples depends on the mutual orientation of the external magnetic field and the internal sample magnetization. Moreover, it was noted that the loss factor increases abruptly when the magnetic field is turned on in the opposite direction to that of sample magnetization due to the particle rotation within the polymer matrix. The loss factor then decreased with time. Moreover, examining the dynamic properties of both isotropic and anisotropic MREs (soft and hard) showed that the anisotropic MREs are stiffer (Anderson et al., 2015). The influence of soft and stiff elastomer matrices on the magnetization hysteresis loops of NdFeB-based MREs was compared by Kalina et al. (2017) in order to investigate the influence of the matrix material on the rotation of hard magnetic particle. Moreover, they presented microscale model to analyze the macroscopic behavior of H-MREs as a function of the rotation of the embedded particles. In another study conducted by Zhao et al. (2017), the storage modulus of both soft and NdFeB-based MR plastomers was analyzed. They demonstrated that unlike soft MR plastomers, the storage modulus of hard MR plastomers kept increasing when the magnetic field decreased and in general the hard MR plastomers presented more complex viscoelastic behavior. Becker et al. (2018) investigated the material properties and vibration of magnetic hybrid elastomer beams fabricated using elastic composite with hard and soft particles aiming to evaluate the potential of magnetic hybrid elastomers to be used in acceleration sensor systems. Hybrid magnetoactive elastomers also have been studied by Borin et al. (2019). They compared the behavior of hybrid magnetoactive elastomers under dynamic axial loading with those of the conventional elastomers. It was shown that both the passive and active state properties of the hybrid elastomer can be tuned using the pre-magnetization of the magnetically hard particles and applied external magnetic field (up to B = 240 mT), respectively.
While there are a number of studies on H-MREs and their quasi-static modeling using the microscale approach, to the best of our knowledge, no studies have been reported on characterization of H-MREs under wide range of operating conditions, particularly on the effect of excitation frequency and negative magnetic field. Considering this, the present study aims to investigate the dynamic behavior of H-MREs operating in oscillatory shear mode. For this purpose, H-MRE samples with 15% volume fraction of hard magnetic particles, NdFeB, were fabricated and their storage and loss moduli were measured performing oscillatory shear tests. The moduli are evaluated under various loading conditions including shear strain amplitude, driving frequency as well as the applied magnetic flux density, and their influence on the shear properties of the H-MRE is investigated. A phenomenological model is then developed to predict the moduli as a function of applied magnetic flux density and excitation frequency. The proposed model is then validated comparing the predicted results with those obtained experimentally.
2. Experimental characterization of H-MREs
In this section, first the procedure to fabricate the isotropic H-MRE samples is briefly explained. This is then followed by the description of the experimental test setup and experimental tests that have been conducted.
2.1. Fabrication of isotropic H-MRE samples
The H-MRE samples with 15% volume fraction of hard magnetic particles were fabricated in the laboratory by mixing hard magnetic particles and silicone rubber matrix. The hard magnetic particles used were unmagnetized NdFeB with a mean particles size of approximately 50 μm. The silicone rubber (Ecoflex 00-50; Smooth On) was used as the matrix of H-MRE. First, the NdFeB particles and the silicone rubber were mixed thoroughly for about 5 min to obtain a homogeneous mixture. The mixture was then degassed in a vacuum chamber under −28 in-Hg for about 5 min. Afterward, the mixture was poured into a transparent plexi-glass mold and left for 24 h at room temperature to be cured. Finally, the cured material was cut into 20-mm diameter cylindrical samples. The samples were then magnetized using a double-yoke adjustable electromagnet under 2.7 T magnetic flux density with applied magnetic field along the axis of the cylindrical samples. The distance between the yokes is set according to the total thickness of H-MRE specimen (2 mm). Figure 1 shows the microstructure image of the H-MRE with two different scales. It is noted that fabricated H-MRE samples are isotropic (no external magnetic field has been applied during the curing process); therefore, the hard particles (white spots in microstructure images) were distributed randomly.

Microstructure images of fabricated H-MRE sample taken by confocal microscopy: (a) scale = 200 μm (10× zoom); (b) scale = 100 μm (20× zoom).
2.2. Test setup
The viscoelastic properties of the H-MRE with 15% volume fraction of hard particles were measured using an advanced rotary rheometer (Discovery HR-3, TA instrument) equipped with magnetorheology accessory. The accessory is capable of applying magnetic field ranging from −1.0 to 1.0 T along the central axis of the H-MRE sample. In the present study, the applied magnetic field is addressed as positive or negative when it is in the same or opposite direction compared to the direction of the magnetic poles inside the H-MRE sample, respectively. The test sample (20-mm diameter and 2-mm thickness) was placed between the rotating and fixed parallel geometries. The samples were initially subjected to 30 N axial compression load in order to ensure that there is no slippage between the geometries and the sample, and then the gap was maintained constant during all the tests. In other words, the tests have been done under constant pre-strain corresponding to 30 N axial load. The applied magnetic field provided by the magnetorheology accessory is perpendicular to the circular cross section of the sample. The temperature of the sample was kept constant during the tests at 20°C by circulating cooling fluid through the magnetorheology accessory.
2.3. Design of experiments
The viscoelastic properties of H-MREs depend on the various operating conditions including the strain amplitude, excitation frequency, and applied magnetic flux density. In the present study, two sets of experiments were performed in order to investigate the dynamic viscoelastic behavior of H-MREs operating in different loading conditions. First, the storage and loss moduli of the H-MRE sample were evaluated by sweeping the shear strain amplitude between 0.01% and 5%, while the driving frequency was kept steady. The tests were conducted under different levels of applied magnetic flux density, and the linear viscoelastic region in which the H-MRE operates independent from the shear strain amplitude was identified. Then, the influence of the excitation frequency on the storage and loss moduli of the H-MRE was investigated through sweep frequency tests. For this purpose, the oscillatory shear test was performed at linear shear strain amplitude of 0.01% while the excitation frequency was swept from 0.1 to 50 Hz. It should be noted that all the tests have been performed under both positive and negative applied magnetic flux densities and the effect of negative magnetic field on the storage and loss moduli of the H-MRE samples was evaluated.
3. Experimental results and discussion
The obtained data were analyzed in the following sections to investigate the effect of different loading conditions including the shear strain amplitude, excitation frequency, and magnetic flux density on the viscoelastic properties of H-MREs.
3.1 Effect of shear strain amplitude
In order to investigate the influence of shear strain amplitude on the storage and loss moduli of H-MRE’s, the oscillatory shear test was performed by sweeping the strain amplitude in the range of 0.01%–5% while the driving frequency and the temperature maintained steady at 1 Hz and 20°C, respectively. The tests were implemented under various levels of positive and negative applied magnetic flux density varied from B = −0.2 T to B = 1 T to study the effect of applied magnetic field on the mechanical properties of the H-MRE. The variation of the storage modulus with respect to the shear strain amplitude is shown in Figure 2. As it can be realized, the storage modulus is independent of strain amplitude for excitations with strain amplitudes below 0.1% and further increase in the strain amplitude decreases the modulus demonstrating the nonlinear viscoelastic behavior. The region in which the storage modulus is independent of the strain amplitude is called linear viscoelastic region, and the associated strain amplitude is represented as

Variation of storage modulus with respect to the shear strain amplitude at the excitation frequency of 1.0 Hz for various applied magnetic flux densities.
Figure 3 shows the variation of the loss modulus with respect to the strain amplitude. Results show that the loss modulus is generally less sensitive to strain amplitude compared with the storage modulus. Figure 3 also shows that regardless of the orientation of the magnetization, applying magnetic field causes the loss modulus of the H-MRE to increase. Increasing the applied magnetic field in positive direction increases the loss modulus; however, this increment is very slight compared with that of storage modulus. On the other hand, the effect of negative field on the loss modulus is in contrary with that on the storage modulus as presented in Figure 2. This is mainly due to the fact that applying negative magnetic field causes the magnetized particles to rotate in the matrix which enhances the energy dissipation capacity of the H-MRE and, subsequently, its loss modulus. Moreover, it is clear in Figure 3 that the loss modulus is almost strain-independent for the strain amplitude range of 0.01%–5% regardless of the applied magnetic flux density.

Variation of loss modulus with respect to the shear strain amplitude at the frequency of 1.0 Hz for various applied magnetic flux densities.
3.2. Effect of excitation frequency
Sweep frequency tests have been performed in order to investigate the effect of excitation frequency on the behavior of H-MREs operating in shear mode. For this purpose, the oscillatory shear test was conducted under constant strain amplitude (0.01%), while the frequency was swept in the range of 0.1–60 Hz. The test was performed under various magnitudes of applied magnetic flux densities ranging from B = −0.2 T to B = 0.85 T in order to investigate the effect of both negative and positive magnetic field on the dynamic behavior of H-MREs. Figures 4 and 5 show the variation of the storage and loss moduli with respect to the excitation frequency for different levels of applied magnetic flux densities. Results presented in Figure 4 show that the storage modulus increases by increasing driving frequency. Results show that the storage modulus increases almost exponentially at low frequencies between 0.1 and 10 Hz (region (a)) and the rate of increase in storage modulus reduces noticeably in this region. Further examination of results reveals that the rate of increase in storage modulus becomes constant and the modulus increases almost linearly beyond 10 Hz (region (b)), so that one can assume linear variation of the storage modulus with respect to the excitation frequency in this region. This behavior could be due to the fact that by increasing the driving frequency, the measurement duration becomes less than the lifetime of the bonding between the matrix chains as well as the silicone rubber matrix and hard magnetic particles. Therefore, the effective bonding increases at higher frequencies which contributes to higher storage modulus of the H-MRE. In addition, Figure 4 shows that apart from the driving frequency, the storage modulus increases by increasing the magnetic flux density and the trend of increment is quite similar over the observed frequency range.

Storage modulus with respect to the driving frequency for different applied magnetic flux densities in both linear and logarithmic scales.

Loss modulus with respect to the driving frequency for different applied magnetic flux densities in both linear and logarithmic scales.
Figure 5 shows the variation of the loss modulus versus frequency for different magnetic flux densities. Increasing the excitation frequency rises the intermolecular heat generated inside the H-MRE sample, and consequently the energy dissipation in the H-MRE increases by increasing the excitation frequency. This phenomenon appears as the growth in the loss modulus with respect to the frequency. As shown in Figure 5, the trend of variation in loss modulus with respect to the driving frequency is similar to that of the storage modulus. The loss modulus increases almost linearly in frequencies higher than 10 Hz (region b), whereas the loss modulus increases almost exponentially for frequencies lower than 10 Hz (region (a)). With respect to the influence of the applied magnetic flux density, as discussed before unlike the storage modulus, applying magnetic field in the opposite direction as the direction of the magnetization does not reduce the loss modulus. Results show that the level of the loss modulus is almost the same for −0.2 and 0.2 T applied magnetic flux density. For instance, for 60 Hz excitation frequency, the loss modulus is 23.68 and 23.2 kPa in presence of −0.2 and 0.2 T applied magnetic flux density, respectively. Moreover, the influence of the applied magnetic field on the loss modulus is not significant compared to its effect on the storage modulus and only applying significant amount of magnetic field (e.g. 0.85 T) causes a slight enhancement in the loss modulus.
3.3. Effect of applied magnetic field
Variation of the storage modulus of the H-MRE with respect to the applied magnetic flux density is shown in Figure 6. Results are generated at various levels of shear strain amplitudes ranging from 0.01% to 5% at driving frequency of 1 Hz. Results clearly show that as expected the storage modulus increases with an increase in the applied magnetic flux density up to saturation limit of almost 0.8 T and further enhancement of the field does not noticeably affect the modulus. This can be attributed to the magnetic saturation of the particles above 0.8 T. Moreover, results again confirm that by applying magnetic field in the opposite direction to that of magnetization direction of hard particles, storage modulus reduces.

Dependence of storage modulus on the magnetic field at the frequency of 1.0 Hz for different shear strain amplitudes.
4. Model formulation
Phenomenological-based mathematical models are developed to predict the viscoelastic properties of the H-MRE with respect to the applied magnetic flux density and excitation frequency. The model is developed for H-MREs operating in shear mode at linear viscoelastic region (
Through examination of results presented in Figures 4 and 5, one can realize that variation of the storage and loss moduli of the H-MRE with respect to the driving frequency can be represented by power functions. This observation stems from the fact that the storage and loss moduli increase almost linearly versus excitation frequency in the logarithmic scale as shown in these figures. The mathematical models for the storage and loss moduli are, thus, proposed to be in the following form
where
in which subscripts
Field-dependent parameters in the developed models at various applied magnetic flux densities.
Figure 7 shows the variation of the obtained parameters with respect to the applied magnetic flux density. Examination of Figure 7 suggests that a second-order polynomial function can be effectively utilized to quantify these parameters as a function of applied magnetic flux density as follows
where B is the applied magnetic flux density in T.

Variation of the parameters (a)
Identified parameters in equations (5)–(8).
As it can be seen in Figure 7, the proposed quadratic functions in equations (5)–(8) can accurately predict the variation of the parameters in the whole range of applied flux densities. Finally, by substituting equations (5) and (6) into equation (1) and equations (7) and (8) into equation (2) and using the parameters presented in Tables 2, the following equations are obtained for the storage and loss moduli of the H-MRE
In the following section, it has been shown that the proposed models can accurately predict the storage and loss moduli of the H-MRE under wide range of applied excitation frequency and magnetic flux densities.
5. Validation of the developed models
In this section, the results obtained using the developed phenomenological models are compared with those measured experimentally to evaluate the performance of the proposed models. Figures 8 and 9 show the results for the storage and loss moduli with respect to the applied magnetic flux density at various excitation frequencies, respectively. Results clearly show that the results obtained from the proposed models agree very well with those obtained experimentally and thus the proposed model can accurately predict the storage and loss moduli under different loading conditions. Comparing Figures 8 and 9 also confirms that that the dependency of the loss modulus on the applied magnetic flux density is negligible compared with the influence of the field variation on the storage modulus.

Comparison of the storage modulus predicted by the proposed model with those measured experimentally.

Comparison of the loss modulus predicted by the proposed model with those measured experimentally.
The variation of the storage and loss moduli with driving frequency are presented in Figures 10 and 11, respectively, in which the results obtained using proposed models are compared with those measured experimentally. As it can be realized, the proposed models can accurately capture the behavior of the H-MRE versus excitation frequency for both positive and negative magnetic fields. The model prediction is completely in accordance with the experimental results especially in the range of 1–20 Hz while slightly deviated from the experiential results at higher frequencies.

Comparison of the storage modulus versus frequency predicted by the proposed model with those measured experimentally.

Comparison of the loss modulus versus frequency predicted by the proposed model with those measured experimentally.
For further evaluation of the developed model, the coefficients of determination (
where G represents the storage or loss modulus of the H-MRE. It is noted that (
The coefficient of determination,
The percentage error is also employed to find the relative error between simulation and experimental results at different applied magnetic flux density and driving frequency. It is found that for majority of cases the average percentage error between the experimental and model results is below 3%.
5. Conclusion
A fundamental study has been conducted to investigate the viscoelastic behavior of the H-MRE under wide range of excitation and applied magnetic field. H-MRE sample with 15% fraction of NdFeB particles was fabricated. Oscillatory shear tests have been performed under different loading conditions including the various shear strain amplitudes, excitation frequencies, and applied magnetic flux densities. The storage and loss moduli were measured under both positive and negative magnetic fields, and the influence of field direction and magnitude on the moduli was investigated. The results illustrated that the storage modulus of the H-MREs is a function of the magnetic field and the strain amplitude as well as the excitation frequency. Enhancing the applied magnetic flux density increases the storage modulus; however, unlike the soft MREs, applying magnetic flux density in the direction opposite to the orientation of the magnetization reduces the storage modulus of the H-MRE. It was also shown that the loss modulus is almost independent of the shear strain amplitude and applied magnetic field. In addition, the influence of driving frequency on the viscoelastic properties of the H-MREs was investigated and it was shown that both moduli are frequency dependent and increasing the excitation frequency rises the moduli. Finally, phenomenological-based mathematical models were developed to predict the linear viscoelastic behavior of the H-MRE under varying operating conditions. Results show that the proposed models can accurately predict the variation of storage and loss moduli under wide range of excitation frequencies and in presence of both positive and negative magnetic fields.
Footnotes
Acknowledgements
Support from the Natural Sciences and Engineering Research Council of Canada (NSERC) is gratefully acknowledged.
Declaration of conflicting interests
The author(s) declared no potential conflicts of interest with respect to the research, authorship, and/or publication of this article.
Funding
The author(s) disclosed receipt of the following financial support for the research, authorship, and/or publication of this article: This research has been funded by NSERC, Grant No. RGPIN/6696-2016.
