Rong Shen*a,
Rui Liua,
De Wangab,
Ke Chena,
Gang Suna and
Kunquan Lua
aBeijing National Laboratory for Condensed Matter Physics, CAS Key Laboratory of Soft Matter and Biological Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China. E-mail: rshen@iphy.ac.cn
bNational Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, China
First published on 11th November 2014
It is known that in traditional dielectric electrorheological (ER) fluid the shear stress decreases or increases with the frequency of the AC electric field. However, for giant ER fluid, which is based on the principle of the polar molecule dominated electrorheological (PM-ER) effect, how shear stress varies with the frequency of the AC electric field is still not clear. In the present paper, we systematically studied the frequency dependence of PM-ER fluid by measuring the shear stresses of PM-ER fluids consisting of CTO nanoparticles under a sinusoidal electric field in a wide frequency range. It is found that the shear stress decreases with the increase of frequency when an AC electric field is applied. In PM-ER fluids there are nonuniform phase shifts appearing in shear stresses with respect to the sinusoidal electric field. These phase shifts become more pronounced as the frequency increases, which leads to the decrease of the amplitudes of the shear stresses. When the frequency is high enough, the oscillations of shear stresses smear out and the amplitudes of shear stresses reduce to a single low value. This behavior in PM-ER fluids is different from that in conventional ER fluids. For a comparison with PM-ER fluid, the response of a traditional ER fluid to frequency in an AC field is also studied, in which the particles possess high dielectric constant. The origin of different frequency responses in two types of ER fluids has been discussed and explained.
In recent years, the researchers in the field of ER fluids focus on the giant ER fluids which is based on the principle of polar molecule dominated electrorheological (PM-ER) effect.14–19 The yield stress of PM-ER fluids can reach more than 100 kPa under a field strength of 5 kV mm−1, which is orders of magnitude higher than that of conventional ER fluids. Another character of giant ER fluids is the linear dependence of yield stress upon the electric field, rather than quadratic as for the dielectric ER fluids.14–16 It is obvious that the PM-ER fluids are distinct from conventional ER fluids.14–19 However it is still unknown how the PM-ER fluids behave under AC fields and what is the relation between the shear stress of PM-ER fluid and the frequency.
In this paper, by measuring the shear stresses under sinusoidal electric field at different frequencies, the frequency response of PM-ER fluids is systematically studied. The results show that the amplitude of shear stress for PM-ER fluid should decrease with increasing field frequency due to response decay. For a comparison with PM-ER fluids the response of a traditional ER fluid on frequency in AC field is also studied. As an example, this traditional ER fluid consisted of the particles with high dielectric constant shows a behaviour that the shear stress increases with the frequency. The origin of different frequency responses in two types of ER fluids has been discussed.
The frequency response measurements were performed with a home-made system which mainly consists of three units. (a) A concentric cylinder-cup rheometer for measuring the shear stress, in which the surfaces of electrodes were both coated with diamond grain layers to avoid sliding.21 The shear stresses were transferred from the recorded values of a torque sensor (0154 RW shaft end version, Dr Staiger Mohilo + CoGmbH, Germany). (b) A high voltage amplifier (Trek 10/40A), which was driven by Rigol DG1011 functional generator, supplied high voltage with slew rate ∼700 V μs−1. (c) A data collection unit with sampling rate up to 4k per second was used for data collection. During the experiment, purely sinusoidal or biased sinusoidal AC fields were employed for different measurements. The sample was sufficiently stirred after each measurement to ensure in a homogeneous state. All the measurements were performed at room temperature with a fixed shear rate of 50 s−1.
When a unbiased sinusoidal electric field E = E0sin(2πft) with E0 = 4 kV mm−1 is applied at different frequencies ranged from f = 1 Hz to 100 Hz, the response curves of shear stress on E can be obtained for each specified frequency. Some selected response curves of shear stress vs. E = E0
sin(2πft) at f = 1 Hz, 10 Hz, 50 Hz and 100 Hz and at shear rate of 50 s−1 are shown in Fig. 3. It can be seen that the behaviors of shear stress varying with E in the regions of 0–π and π–2π are same, due to the equal response of shear stress in both positive and negative electric field. However the maximum magnitude of shear stress at low frequency is large and decreases with increased frequency. It is clear in Fig. 3 that the maximum magnitude of shear stress can reach up to about 20 kPa in a field of f = 1 Hz, while the induced oscillation causes the shear stress almost being smeared out to about 5 kPa in same field E with f = 100 Hz. This will be clearly demonstrated in an inset of Fig. 5(b) presented later on, which shows the maximum and minimum values of shear stress in a region of f from 1 Hz to 100 Hz. This phenomenon is due to the response decay of shear stress on E in PM-ER fluids. Obviously there are phase shifts for the shear stress corresponding to E and the shifts augment gradually as the frequency increases. Therefore, the shear stress in a sinusoidal electric field can be expressed as τ(E) = τm(E0)
sin[2πft + δ(f,t)] + τ0(f), where τm(E0) and δ(f,t) are the amplitude of shear stress and phase shift respectively, τ0(f) is residual stress. δ(f,t) is not a constant for a fixed frequency in a period from 0 to 2π and τ0(f) is a function of frequency.
In order to give a distinct picture, the response of shear stress in a sinusoidal electric field with bias Eb is carefully studied in a wide frequency range of f = 0.5–1000 Hz. Using a biased sinusoidal electric field E = E0sin(2πft) + Eb, an advantage is only one maximum of shear stress in the period from −π to π as E changing from 0 kV mm−1 to E0 + Eb. The dependences of magnitude and phase shift of shear stress on frequency of electric field are intuitional in this configuration.
Fig. 4 shows how the shear stresses of PM-ER fluids respond to a field of E = E0sin(2πft) + Eb for f = 0.5 Hz, 15 Hz, 50 Hz and 100 Hz, where E0 = 2 kV mm−1 and Eb = 2 kV mm−1. The relations of shear stress vs. time and shear stress vs. E are illustrated in left and right columns of Fig. 4, respectively. When the frequency is low, f = 0.5 Hz for instance, the shear stress varies sinusoidally with quite large amplitudes from 2 kPa to 20 kPa as shown in Fig. 4(a)-1. However, there are some slight time delays of shear stress τ(E) comparing to the field E and hence an asynchronism in the relation of τ(E) and E in Fig. 4(a)-2 appears. Obviously there is an uneven phase shift on shear stress in a period of sine wave. When the frequency of the field is high, the shear stress tends to a constant value and their wave patterns vary no longer with any sinusoidal shape. From all measured curves of τ(E) = τm
sin[2πft + δ(f,t)] + τ0(f) in the field of E = (2 kV mm−1)sin(2πft) + (2 kV mm−1) from f = 0.5 Hz to f = 1000 Hz, the phase shifts and the amplitudes of shear stresses varying with frequencies are drawn in Fig. 5(a) and (b) respectively. Fig. 5(a) shows the phase shifts of τ(E) for some selected frequencies in a cycle from −π to π. It can be seen that the phase shift δ(f,t) is small at low frequency and increases with f. Furthermore, for a fixed f, δ(t) is not a constant in the period from −π to π. For instance, in the case of f = 0.5 Hz, δ ≈ 0.16π at −π/2 and δ ≈ 0.03π at π/2. As f ≥ 100 Hz, the phase shift δ even reaches up to π with nonuniform variation in the cycle from −π to π. Such large and nonuniform phase shift must smear out the amplitude variation of shear stress in sinusoidal field and thus cause τ(E) approaching a stable value around 5 kPa. A Fourier transform of τ(E) function for f = 100 Hz, as shown in the upper right inset of Fig. 4(d)-2, demonstrates that there are many frequency components contained in τ(E), which makes the amplitude of τ(E) reduced.
As described above the traditional ER effect is derived from the particle polarization, in which the mismatch factor β plays a crucial role. In the polarization process the polarizing time is fast enough to response the change of AC field in frequency range to 103 Hz. Thus β2 increases with increased frequency and can enhance the attractive forces between particles in the ER fluid consisted of the particles with high dielectric constant, i.e. the shear stress increases monotonically. Although the shear stress of such type ER fluid is low, the enhancement factor can be as large as a factor of 102 from a DC field to an AC field of 103 Hz, correspondingly the shear stress increases from few Pascal to hundreds of Pascal.
On the other hand, the polar molecules adsorbed on the particles dominate the PM-ER effect.14–16 When an electric field E is applied and then the particles will attract each other to form chains through the dielectric interaction as the traditional ER effect. In the gap between the particles the local electric field Eloc can be more than 102 times higher than E. Under a strong local electric field Eloc between particles, polar molecules are able to be orientated along the field direction and interact with the polarized charges on particles. Such interaction is 2–3 orders of magnitude stronger than that of polarized particles as in conventional ER fluids. So that the shear stress of PM-ER fluids can reach hundreds of kPa.
The adsorption energy Uad of the polar molecules on the particles is nearly KT, where K is Boltzmann constant and T is absolute temperature. As long as the interaction energy μEloc of Eloc and polar moment μ is larger than KT the polar molecules adsorbed on the particles can turn their directions. If the amplitude of E is smaller than a certain value in the period of applied sinusoidal field E = E0sin(2πft), the Eloc will be not large enough to satisfy the condition of μEloc > KT. The polar molecules adsorbed on the particles are unable to turn to the direction of electric field. Thus only the amplitude of sinusoidal field is higher and causes μEloc > KT, the polar molecules can be turned to the direction of electric field and result in the PM-ER effect. As E in a period of sinusoidal field is reduced to a value corresponding to Eloc < KT, the polar molecules will turn back to original adsorption configuration on the surface of particles, and then the PM-ER effect disappear. Fig. 6 illustrates how the adsorbed polar molecules affect in an AC field. The gray area of a sinusoidal field in Fig. 6(a) indicates the corresponding region of μ|Eloc| < KT where the adsorbed polar molecules are unable to responding the field as shown in Fig. 6(c). If μEloc > KT in the range of 0 to π or μ|−Eloc| > KT in π to 2π, the adsorbed polar molecules are able to turn their orientation as shown in Fig. 6(d) and (e) respectively, and then correspondingly the shear stress caused by PM-ER effect emerges. All these procedures must create a time delay of shear stress responding to the AC field. On the other hand the local electric field Eloc in between the particles is related to the particle size. The amplitudes of local field Eloc for various particles are different in a same applied field because of the unequal particle size in the suspension. Assuming the gap widths between particles are the same, the larger particles will induce larger Eloc. It means that in a E = E0
sin(2πft) field the local field Eloc are different for the particles with different size. Hence the gray area shown in Fig. 6(a) will vary with the sizes of the particles due to Eloc is related with the size of particle. Therefore in PM-ER fluids, turning and returning the orientations of polar molecules in an AC electric field cannot well follow the variation of the field and cause a complex phase shift. The behaviour is about the same by using an unbiased or biased sinusoidal field as shown in Fig. 5(b).
As described above the PM-ER effect cannot occur in the region of μ|Eloc| < KT and Eloc is related with the size of particles. This factor is also able to be employed to explain the phenomena usually observed that the shear stress of PM-ER fluids rises very gently in the region of low DC field strength. Because of the unequal size distribution of particles, the particles with larger size need lower field strength and that with small size need higher field strength for getting same Eloc. Therefore the number of responding particles gradually increases as the field strength increases. Once the strength of the applied field is high enough, all particles can contribute to PM-ER effect and then the shear stress increases linearly with field strength increasing.
The measured response time for PM-ER fluids is about 10 ms, which is longer at the rising edges of shear stress and shorter for its falling edges.22 The patterns of shear stress of PM-ER fluids shown in Fig. 5 indicate that the phase shift is larger in the first half cycle of −π to 0 in the case of using a sinusoidal field with bias. This means that the response delay on shear stress is longer in the rising region of the sinusoidal field. When frequency is enough high, i.e. f ≥ 100 Hz for our measured samples, the response delay spreads unequally in a cycle and phase shift can even reach to π. Therefore the amplitudes of shear stress of PM-ER fluids decrease with frequency increasing in an AC field. The dependence of response time on the volume fraction and electric field strength in an AC field will be presented elsewhere.22 The tendency of shear stress of PM-ER fluids decreasing with frequency increasing remains the same. Although based on the traditional ER effect at times the polarization force of particles can have a positive effect on the shear stress from increasing frequency as shown in Fig. 2(a), however the contributed values are as small as 102 Pa and can be neglected.
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