Huilan
Jing‡
ab,
Letian
Hua‡
a,
Fei
Long
ac,
Bojin
Lv
ab,
Bing
Wang
ab,
Hewen
Zhang
a,
Xunye
Fan
a,
Hongru
Zheng
a,
Chengyi
Chu
a,
Gaojie
Xu
a,
Jianjun
Guo
*a,
Aihua
Sun
*a and
Yuchuan
Cheng
*ab
aZhejiang Key Laboratory of Additive Manufacturing Materials, Ningbo Institute of Materials Technology & Engineering, Chinese Academy of Sciences, Ningbo 315201, P. R. China. E-mail: jjguo@nimte.ac.cn; sunaihua@nimte.ac.cn; yccheng@nimte.ac.cn
bCenter of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, P. R. China
cDepartment of Mechanical, Materials and Manufacturing Engineering, University of Nottingham Ningbo China, Ningbo 315100, P. R. China
First published on 7th August 2023
Soft robots have drawn a lot of attention due to their soft materials that make them highly flexible and adaptable to complex environments. However, these also make soft robots not suited to high-load tasks, and achieving controllable material stiffness variation is still a challenge. Herein, we designed a soft structure with variable stiffness based on electrorheological fluids, which presented the advantages of continuously variable stiffness and fast response. The structure exhibited a stiffness of up to 1065 mN mm−1 when the electric field strength was 4.5 kV mm−1 (displacement of 1 mm). When varying the electric field strength (0 to 4.5 kV mm−1), the rate of stiffness variation was over 1500%. According to the load cycle experiments, it was shown that the structure's response time to a change in load was less than 65 ms, and that the structure changes could be made repeatedly. In addition, we demonstrated the functions of stiffness adjustment, shape memory, and motion locking of the structure. This work has potential applications in the fields of soft robotics and artificial muscles.
The inherent softness of flexible materials not only makes dexterous and safe interactions possible to prevent damage to the environment and the physical body, but it also makes soft robots unsuitable for tasks that require a high load capacity.8 Therefore, stiffness tuning is crucial to allow the actuator to perform both flexible movements and rigid load carrying and is a way for soft robots to interact effectively with humans and environment. Inspired by nature, where organisms can adjust the stiffness of their tissues to resist external changes, stiffness variation has been introduced into mechanical systems9,10 and can be used to tune mechanical properties of flexible actuators. Researchers have explored a variety of stiffness-tunable materials to prepare soft robots.11–13 Among these, temperature-sensitive phase-change materials have received particular attention,14 including shape-memory alloys,15 thermoplastic polymers,16 and low-melting-point alloys.17 These materials have the advantages of a wide range of stiffness variation, but usually can only switch between rigid and flexible states, and it is difficult for them to achieve multistage and continuous control of stiffness, and they cannot achieve active invertible stiffness, while their response speed is usually slow.
Electrorheological (ER) fluids are a kind of smart materials whose rheological performance can be adjusted by an external electric field.18,19 ER fluids are typically composed of electrically polarizable particles dispersed in an insulating fluid. In the absence of an electric field, the particles are uniformly distributed in the insulating liquid and the material is fluid-like. When an electric field is applied, however, the particles form a chain or columnar structure along the direction of the electric field as a result of the attractive forces between the polarized particles. At that moment, the viscosity of ER fluids changes significantly, transforming from fluid-like to solid-like in milliseconds. This viscosity conversion is reversible, and when the electric field is withdrawn, the particles return to their original fluid state.20–22 The macroscopic performance of ER fluids involves a reversible change between liquid and solid states, as well as a reversible shift in its apparent viscosity. Based on the properties of ER fluids, they have a range of engineering applications, such as dampers,23 clutches,24 and valves.25
A lot of researchers have studied the properties of the stiffness variation due to the ER effect. Tonazzini et al. proposed an ER fluid-based multilayer valve, in which the ER fluid acted as an actuation fluid and a control medium.26 By applying an ON–OFF electric signal to the rigid electrode plates, fast switching between the liquid and solid state of the ER fluid could be achieved. However, the materials used for encapsulating and the electrodes used for powering ER fluids were rigid, making it difficult to achieve a flexible structure. Wei et al. proposed a cantilever sandwich beam with ER elastomers, where the elastomer was used as a viscoelastic damping material to control the vibration of the cantilever beam.27 The results showed that with the increase in the applied electric field strength, the natural frequency of the ER elastomer sandwich beam increased and the vibration amplitude at the natural frequency decreased. Although the ER elastomer was flexible, the ER particles were embedded in the elastomer and could not move, leading to a low stiffness rate and weak electric field response. Fast variable stiffness of flexible devices remains a challenge.
Herein, we propose a stiffness-tunable soft device with a “sandwich” structure of a PDMS/electrode-ER fluid-electrode/PDMS (Fig. 1a). The ER materials used, which were prepared via a precipitation process, offered the advantages of a high yield stress and low leakage current density, while the chosen encapsulating material and electrodes were both flexible. The ER fluid was in a liquid state without the electric field, providing the structure with good compliance and the ability to be deformed. Once the electric field was applied, the ER fluid solidified, keeping the structure in its temporary shape. The stiffness variation rate of the structure was over 1500% (0 to 4.5 kV mm−1). Benefiting from the fast polarization and depolarization of ER particles, the soft structure demonstrated an outstanding response speed, within 65 ms for load changes. Based on the advantages of the continuously variable stiffness and fast response of this structure, we demonstrated the functions of variable stiffness, shape memory, and motion locking.
Fig. 1 (a) Structure of the stiffness-tunable soft structure. (b) Fabrication process of the stiffness-tunable soft structure. |
The ER fluids were formed by mixing the CTO particles with silicone oil. Before the experiment, the silicone oil was dried at 120 °C for 4 h. The CTO particles and silicone oil were mixed by ball milling in different proportions after cooling to obtain the desired concentration. The concentration of the ER fluids is denoted as the ratio of the nanoparticle weight to the silicone oil volume. For example, 1 g of CTO particles mixed with 1 mL of silicone oil is denoted as 1 g mL−1.
A range of concentrations of CTO ER fluids were prepared to evaluate their ER behavior under different electric fields. When the concentration was increased to 3.5 g mL−1, the fluid was clay-like and lacked fluidity, making it difficult to inject into the silicone rubber shell (Fig. S3, ESI†). Therefore, we only investigated the ER properties of the ER fluids with concentrations ≤ 3 g mL−1. As shown in Fig. 2d, the yield stress conformed to a positive dependence on the electric field strength, which was due to the tendency of the polarized particles to aggregate into tighter and thicker fibrous or columnar chains when the electric field strength was raised. This positive correlation was not obvious in the electric field strength region of 0–1.5 kV mm−1, which was due to the fact that the ER fluid constructed a polarization layer in this region. In addition, the ER performance increased as the ER fluid concentration increased, which could be explained by the fact that as the concentration increased, more dielectric particles became involved in the polarization process in the system and more polarization chains were generated between the electrodes, thus reflecting a higher yield stress at the macro level. According to the experimental values in Fig. 2d, when the concentration was 3 g mL−1, the ER fluid exhibited a significantly high capacity with yield stresses up to 125 kPa. Therefore, the ER fluid with a concentration of 3 g mL−1 was selected for injection into the flexible shell to prepare the stiffness-tunable structure. Also, the concentration refers to 3 g mL−1 from here on unless otherwise noted.
The leakage current density is also an important consideration when assessing ER fluids. The leakage current density has a noticeable impact on an ER fluids system's power consumption and heat production. Moreover, greater leakage currents might result in a breakdown, which would greatly affect the lifespan and application performance of ER fluids systems. As shown in Fig. 2e, the leakage current density of the ER fluid increased with the rising electric field strength, and the maximum leakage current density was 12.73 μA cm−2 (4.5 kV mm−1). This shows the superior operational safety and reduced energy usage caused by Joule heating of the prepared ER fluids. It has been reported that the wettability between the ER particles and the insulating oil determines the leakage current density.30 In a well-infiltrated ER fluid, the charge transfer between the particles is hindered by the insulating oil, which modifies the current flow.
To acquire a deeper comprehension of the CTO ER fluids, the dynamic rheological properties were also assessed (Fig. 2f). The maximum shear stress at 4.5 kV mm−1 was around 125 kPa, which was equivalent to the yield stress under the same conditions. It is generally accepted that the shear field-induced hydrodynamic and electric field-induced electrostatic interactions determine the rheological behavior of ER fluids, whereby the hydrodynamic interactions tend to destroy the ER particles’ structures and facilitate flow while the electric field-induced interactions cause the reorganization of the ER particles’ structures and obstruct flow. For high concentrations of ER fluids, the shear stress tends to decrease as the electric field strength increases after peaking. This is a common phenomenon in parallel plate measuring instruments; in fact, for all parallel plate measuring instruments, when the concentration of ER fluids is relatively high, the suspension is easily discharged from the central region of the test instrument. This is because once the particles have formed a chain, there is a significant density difference between them and the fluid, and the centrifugal force produced by the plate measuring instrument's rotation drives the chain to move to the plate's edge.31
ΔLoadmax = LoadE, max − LoadE0, max | (1) |
In the small deformation region (0–1 mm), the load as a function of bending displacement at different electric field strengths is depicted in Fig. 3c. The load variation of the structure was little affected by the electric field at a lower electric field strength because the lower strengths were insufficient to provide a strong enough polarization force to chain the ER particles. When the electric field strength was 0.5 kV mm−1, the yield pressure of the ER fluid was about 2 kPa (Fig. 2d), and the maximum load at the bending displacement of 1 mm was 0.11 N. In this case, the structure had almost no resistance to external pressure. When the electric field strength was 4.5 kV mm−1, the yield pressure of the ER fluids was 125 kPa (Fig. 2d), and the maximum load at 1 mm displacement reached 0.97 N, which was approximately 9 times the load at 0.5 kV mm−1. To quantify the ability of the structure to cope with tensile deformation, the stiffness k is defined as:
k = P/δ | (2) |
In the large deformation region (1–6 mm), the load as a function of displacement at various electric fields is shown in Fig. 3e and the stiffness versus electric field is shown in Fig. 3f, respectively. When the electric field strength was 4.5 kV mm−1, the maximum load at a displacement of 6 mm was 2.24 N, and the stiffness was 259 mN mm−1, which had increased by nearly 200% compared with the case in the absence of an electric field. It can be seen that the increased amplitude in stiffness was lower than that in the small deformation region.
It can be observed in Fig. S4 (ESI†) that the stiffness k was divided into two zones with increasing deformation displacement, and that the inflection point occurred at 1 mm from the displacement. This phenomenon can be explained as follows: two factors contribute to the increase in the structure stiffness under an electric field. On the one hand, the ER fluid in the structure forms polarization chains when an electric field is applied, and these chains will hinder the shear behavior, and thus the viscosity of the ER fluid increases. On the other hand, when an external force is applied, there is friction between the CTO particles and the electrode surface, which also leads to an increase in viscosity. As shown in Fig. 4a, the bending deformation undergoes no-slip and slip processes. Fig. 4b describes the stiffness variation of the whole structure under the electric field, as well as the microstructure of the particles in the no-slip process and slip process. In the non-slip process, the applied pressure is less than the yield stress of the ER fluid and the friction between the CTO–CTO particles, and between the CTO–electrodes. At this time, there is no relative displacement between the CTO particles, or between the ER fluid and the electrode surface. The ER fluid and the electrode layer can be regarded as a single entity to withstand external pressure, and the polarization chains are not damaged, so there will be greater stiffness. With the increase in external pressure, the structure generates large deformation and enters the slip process. The external pressure at this time is larger than the yield stress of the ER fluid, and the space for the formation of particle chains decreases, resulting in the slip and miss-cutting of particles, which damages the particle chain segment, and decreases the interparticle forces. Therefore, the increase in stiffness is less than that in the small deformation process.
To further demonstrate the versatility of the structure, we demonstrated the stiffness variation and shape-memory functions. Pictures of the stiffness variation of the structure are shown in Fig. 5a. When a 100 g weight was applied to the structure without applying an electric field, the structure produced a large bending deformation. Also, when the same weight was applied with an electric field, it can be seen that the deformation was significantly reduced. This implies that the load to be carried became greater, and the stiffness of the structure became larger. We demonstrate the shape-memory function of the structure in Fig. 5b and Movie S1 (ESI†). The principles of the shape-memory behavior and the microstructural changes of the elastic shell and ER fluid in the process of shape memory are also described in Fig. 5b. Initially, the structure was in its original stress-free state without an electric field. After adding a 100 g weight, the structure bent due to the external stresses and deformed into a temporary shape. Here, the elastic shell of the structure generated restored the stress, while the ER fluid remained in its unstressed state. Upon the application of an electric field with an intensity of 2.8 kV mm−1, the ER fluid solidified in a nearly stress-free state, while the elastic shell was unaffected. When the yield stress of the ER fluid was much larger than the resilience of the elastomer, the structure could maintain a profile close to its programmed shape. Thus, with the applied electric field maintained, the restoring stress of the elastomer was counteracted by the stiffness of the ER fluid after the external pressure was released. When the electric field was removed, the ER fluid became fluid again, restoring the elastomer to its original remembered shape. The shape memory was fully rewritable, so a new cycle could be repeated.
Considering the fast-response properties of the ER fluid, motion locking was designed by switching the electric field to adjust the stiffness of the soft structure (Fig. 6b). As can be seen in Fig. 6c and Movie S2 (ESI†), when no electric field was applied, a nudge on the top clip of the structure disrupted its equilibrium and then it bent, which was an accelerated motion caused by gravity. At the moment when the electric field is applied, the motion was locked due to the stiffness of the structure increasing. After the electric field was removed, the structure continued to bend down under the effect of gravity. The response of the structure was very sensitive to switching the electric field.
Footnotes |
† Electronic supplementary information (ESI) available. See DOI: https://doi.org/10.1039/d3tc01563g |
‡ Huilan Jing and Letian Hua contributed equally to this work. |
This journal is © The Royal Society of Chemistry 2023 |