Special Issue Article

Journal of Intelligent Material Systems

and Structures
2021, Vol. 32(13) 1420–1431
Capacitance creep and recovery Ó The Author(s) 2020
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DOI: 10.1177/1045389X20969911

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Yuqin Fan1*, Hong Qin2, Chuan Lu3, Changrong Liao2 ,

Xianping Chen2, Jiabing Yu2 and Lei Xie2*

Abstract
As a novel conductive elastomer, magnetorheological elastomers (MREs) featuring both high sensitivity and wide working
range have been employed as a new sensing material for flexible tactile sensors. Their sensing mechanism, that is, the spa-
tial distribution rearrangement of particles under compression, completely differs from their conventional counterparts.
The piezo-capacitive effect of MREs resulting from the unique mechanism of particles rearrangement is actually a response
to the microscopic mechanical movement of particles. This nature brings a core concern on the intrinsic relationship
between their mechanical and electrical properties. This study illuminates them from the perspective of electrical creep
and recovery behavior of MREs. We give a meaningful analysis for the capacitance creep-recovery mechanism. The experi-
mental fact strongly demonstrated that the particles rearrangement was the direct cause, while the strain creep was an
indirect cause. All the behaviors were well interpreted by an evolution mechanism of the particles rearrangement driven
by the mechanical strain creep of the flexible matrix under constant pressure. In simpler terms, the electrical creep was
induced by the mechanical creep. We further explored the creep effect in practical applications and found a ‘‘self-healing’’
behavior, which indicated that the MRE sensors could obtain a stable sensing capability after a pre-processing.

Keywords
electrical creep, capacitance creep, particles rearrangement, time dependence, magnetorheological elastomer

1. Introduction (Fan et al., 2017, 2018). Specifically, induced by com-

In recent years, flexible tactile sensors (such as elec-
tronic skins) (An et al., 2017; Cao et al., 2018; Khalili
et al., 2018; Yan et al., 2019) have become a research
hotspot for intelligent robots, rehabilitation therapy
and many other applications. Sensitivity and working
range are the two key parameters for flexible tactile
sensors, but a trade-off usually exists. Lately, research-
ers (Arenhart et al., 2016; Fan et al., 2017, 2018;
Mysiukiewicz et al., 2017) have employed micron-/
nano- particles-filled conductive elastomers (hereinafter
referred to as PFCEs) as the sensing materials for the
relevant sensors; their unique piezo-resistive and piezo-
capacitive mechanism produces good sensitivity as well
as wide working range up to hundreds of kPa. The
piezo-resistive/-capacitive mechanism of these PFCEs
completely differs from those of traditional counter-
parts. Such a piezo-resistive/-capacitive behavior is a
macroscopic reflection of how well the dispersed parti-
cles change their spatial distributions (and hence the
dielectric constant) under compression (i.e. called parti-
cles rearrangement, a schematic shown in Figure 1(a))
pression, the adjacent particles that constitute micro-
capacitors pair with new neighbors into new micro-
capacitors (piezo-capacitive effect) (Fan et al., 2017,
2018), or establish new conductive paths (piezo-resis-
tive effect) (Rui and Ying, 2018; Zhou et al., 2017).
Inspired by these, some researchers proposed the
1
College of Mathematics and Physics, Chongqing University of Science
and Technology, Chongqing, China
2
Key Laboratory of Optoelectronic Technology & Systems (Chongqing
University), Education Ministry of China, Chongqing, China
3
Science and Technology on Reactor System Design Technology
Laboratory, Nuclear Power Institute of China, Chengdu, Sichuan
Province, China
* These authors contributed equally to this work.
Corresponding author:
Lei Xie, Key Laboratory of Optoelectronic Technology & Systems
(Chongqing University), Education Ministry of China, Room#1103, Main
Teaching Building, Campus A, Chongqing University, Chongqing 400044,
China.
Email: lxie@cqu.edu.cn
Fan et al. 1421

Figure 1. (a) Schematic of particles rearrangement for the piezo-capacitive effect of MRE, (a.1) for instance, particle #6 pairs with
#2 and #10 into two micro-capacitors between the two electrodes in the initial state, (a.2) upon application of a normal pressure,
the particles rearrange their spatial distribution, and particle #6 separates from #2 and #10 but repairs with #1 into a new micro-
capacitor; also, particles #2 and #10 become repaired even though there is a relatively wider inter-particle gap, (b) SEM images
showing the internal microstructures of MRE, and (c) typical strain creep-recovery curve of viscoelastic materials under a constant
pressure.

magnetorheological elastomers (hereinafter MREs) as The piezo-resistive/-capacitive effect of MREs con-

the sensing material. The MREs are a magnetically
structured PFCE, which includes micron-sized soft
magnetic particles regulated by magnetic field during
the solidification of MRE due to the magnetorheologi-
cal effect (Liu et al., 2013; Mietta et al., 2016). The
authors (Fan et al., 2018) found that the MRE was
capable of inducing a large-scale particles rearrange-
ment under compression owing to the locally concen-
trated particles (i.e. particle-chains structures, see
Figure 1(b)) in the polymer matrix. This structured
MRE was able to not only achieve an extremely high
sensitivity (up to 460/kPa) which is one to two orders
of magnitude higher than those of the conventional
counterparts, but also maintain a very wide working
range (around 200 kPa) (Fan et al., 2018). Therefore,
MREs as a new candidate provide a promising candi-
date for flexible tactile sensors.
tributed by the unique effect of particles rearrangement
is, in other words, a response to the mechanical move-
ment of particles under compression. This nature
brings us a core concern on the intrinsic relationship
between the mechanical and electrical properties of
MREs. In general, polymer materials exhibit both solid
and fluid properties, which are commonly referred to
as viscoelasticity—a synthesis of elasticity and viscosity.
For MREs, the addition of particles inevitably makes
this property more complicated. For example, the
Young’s modulus is generally significantly enhanced,
and so is the viscosity because of the friction between
the dispersed particles and the matrix. Although viscoe-
lasticity is a mechanical property, it is intrinsically
related to the electrical behaviors of MREs. When sub-
jected to external force, MREs deform from their initial
state to another (compressed) along with the transition
1422
of microscopic polymer structure and particles spatial
distribution. Such a process of strain responding to
pressure takes a certain time, resulting in a phenom-
enon where strain increases with the loading time of
pressure, which is called strain creep (Li et al., 2010; Qi
et al., 2016). Since the piezo-resistive/-capacitive effect
of MREs is dominated by the microscopic spatial dis-
tribution of particles (Fan et al., 2017, 2018), an electri-
cal creep-recovery behavior will arise from the
mechanical strain creep and recovery. In addition, the
intrinsic mechanism of many properties of MREs such
as repeatability, stability, memory effect etc. could also
be further understood on the basis of this connection.
The electrical creep and recovery of MREs are a
phenomenon of the dependence of capacitance/resis-
tance on time when loading and unloading a constant
pressure (Wang, 2018; Wang et al., 2013; Wang and
Han, 2013; Zhu et al., 2018). In practical applications,
flexible tactile sensors sometimes need to accommodate
a long-term application of constant force (e.g. a manip-
ulator holding an object), or operation with varying
forces for a long period of time. In these cases, the
creep could be triggered, causing the input-output rela-
tionship of the sensor to differ over time. Especially,
the capacitance/resistance after creep would change
because of the residual effect in the recovery phase,
which produces abnormal output and further affects
the stability and repeatability of the sensors. These
characteristics are of significance for the practical
applications of the MRE-based flexible tactile sensors.
Therefore, it is a vital necessity to investigate their elec-
trical creep-recovery behaviors.
The mechanical creep and recovery knowledge of
viscoelastic materials can be meaningful inspiration for
the study of the electrical creep-recovery behavior of
MREs. As shown in Figure 1(c), the typical strain creep
process is divided into three phases: instantaneous
strain, primary creep and secondary creep, correspond-
ing to the instantaneous recovery strain, delayed elastic
strain and viscous flow strain in the recovery process,
respectively (Yao et al., 2013). For an ideal linear vis-
coelastic material, the instantaneous strain is the instan-
taneous elastic response of the material to the pressure.
It can completely recover after the pressure is removed,
which is equal to the instantaneous recovery strain in
the recovery phase. Primary creep is an unsteady creep
phase characterized by a large creep rate de/dt decreas-
ing with time. It takes a certain amount of time to fully
recover, therefore corresponding to the delayed elastic
strain. Secondary creep is the steady creep phase where
the strain slowly increases at a rate proportional to
time. Since secondary creep produces viscous strain, it
is irreversible (Li et al., 2010) and results in the residual
strain in the recovery phase (i.e. viscous flow strain).
Researchers had reported the resistance time-
dependent behavior of conductive polymers (Wang and
Han, 2013; Wang et al., 2013), including studies on the
Journal of Intelligent Material Systems and Structures 32(13)
constitutive equation and the sample compositions.
However, there are few reports on the capacitance
creep and recovery of conductive elastomers (especially
MREs). An exception is that Wang et al. conducted a
study on the carbon black filled elastomers, that is, the
capacitance creep/relaxation under ‘‘constant strain’’
(Wang, 2018; Zhu et al., 2018), but the microscopic
mechanism has not been thoroughly elaborated. In our
previous modeling and experiments, it has been con-
cluded that the particles spatial rearrangement is the
microscopic mechanism that dominates the extraordi-
nary piezo-capacitive effect of MREs (Fan et al., 2017,
2018) (schematic see Figure 1(a)). When compressed,
the particles change their spatial distribution within the
polymer matrix. Thus, the adjacent particles constitut-
ing original micro-capacitors are separated, and paired
with new neighbors into new micro-capacitors. Such a
mechanism alters the overall number of micro-
capacitors connected in series and in parallel, which
gives rise to the macroscopic piezo-capacitive effect.
Therefore, the research on the capacitance creep and
recovery of MREs will not only provide knowledge on
the dependence of capacitance on time, but also a fur-
ther understanding of the unique mechanism of parti-
cles rearrangement.
In this study, five different groups of MRE samples
were prepared and experiments were carried out using
a testing system to investigate the capacitance creep-
recovery behavior of MRE. The effects of sample pre-
paration parameters (such as curing magnetic field
strength, particles volume fraction, particle size, and
the polymer matrix flexibility), level of constant pres-
sure and the loading time of pressure on the capaci-
tance creep and recovery were investigated. The impact
of capacitance creep on the piezo-capacitive sensing
properties of MRE was also studied by directly com-
paring the piezo-capacitive data acquired before and
after creeps. Especially, a microscopic analysis was per-
formed on the particle scale for the capacitance creep-
recovery mechanism as well as the experimental results
mentioned above.
2. Experimental details
2.1. Raw materials and sample preparation
The flexible matrix for the MRE samples was synthe-
sized from two-component room temperature vulca-
nized (RTV-2) silicone rubber, dimethyl silicone oil and
curing agent (1.5%) (Hong Ye-Jie Technology, China).
Spherical nickel particles with various average dia-
meters of 0.5, 6.5, 30 mm (Lord Metallurgical Powder
Factory, China) were used as the soft magnetic parti-
cles and meanwhile the conductive phase. Surface pre-
treatment was performed for the particles using silane
coupling agents (KH550, Lord Metallurgical Powder
Factory, China) in order to improve the adhesion
Fan et al.
Table 1. Configuration parameters of MRE samples.
Group Curing magnetic Volume fraction Particle
field flux density (T) (vol%) size (mm)
A 0, 0.2, 0.4, 0.6 10 6.5
B 0.6 5, 10, 15 6.5
C 0.6 10 0.5, 6.5, 30
D 0.6 10 6.5
E 0.6 10 6.5
between the nickel particles and silicone matrix. By
adjusting the weight ratio of the RTV-2 silicone rubber
to the silicone oil, the Young’s modulus of the MRE
could be controlled, so that they could have a bionic
flexibility as well as significant piezo-capacitive effect.
There were mainly three steps in preparing the MRE
samples. Firstly, surface pretreatment of the nickel par-
ticles was performed by thoroughly mixing them with
an appropriate amount of the silane coupling agent, fol-
lowed by drying the mixture in a vacuum oven at 120°C
for 2 h. Secondly, the RTV-2 silicone rubber and the
silicone oil at a given mass ratio were mixed and stirred
evenly. Then, surface-pretreated particles were added at
a designed volume fraction. The mixture was stirred for
1 h by a mechanic stirrer to obtain an isotropic suspen-
sion. Finally, curing agent was added into the suspen-
sion with vigorously stirring for 10 min. Then, it was
poured into a cylindrical mold (diameter = 20 mm and
depth = 2.6 mm) and placed in a magnetic field for
solidification and magnetization for 30 min. Thus, the
MRE samples were obtained after demolding. More
details for the sample preparation were described in our
previous work (Fan et al., 2018).
Five groups of cylindrical MRE samples (shown in
Table 1) were prepared for investigation of the influen-
cing factors on the capacitance creep-recovery behavior.
The main sample parameters were: particle volume frac-
tion = 10 vol% (corresponding to the weight fraction of
50 wt%), particles size = 6.5 mm, mass ratio of silicone
oil to RTV-2 silicone rubber = 0.25:1, and the curing
magnetic field flux density (denoted as Bcuring) = 0.6 T in
the axial/normal direction. All the samples in Groups
A;D were based on the above parameters, but in each
group, there was one specific parameter with various val-
ues so that its influence could be investigated. For exam-
ple, in Group A, samples prepared with Bcuring = 0, 0.2,
0.4, and 0.6 T were made for the effect of curing field
strength on the capacitance creep-recovery behavior.
2.2. Measurement
Figure 2(a) shows a schematic of the capacitance creep-
recovery test system. It consists of standard weights,
MRE based piezo-capacitive sensing unit, pressure
1423
Mass ratio of Influencing
silicone oil to factors
RTV-2 silicone rubber
0.25 Curing field strength
0.25 Particles Volume fraction
0.25 Particle size
0.19, 0.25, 0.32 Matrix flexibility
0.25 Pressure level and
loading time; repeatability
sensor (JHBM-7, Bengbu Sensor System Engineering
Co., Ltd., China), LCR meter (UC2656B, Changzhou
Youce Electronic Technology, China) and computer.
The flexible tactile sensing unit is structured as a sand-
wich, where MRE is placed between two flexible elec-
trode plates (thickness ;100 mm each). Hard glass
sheets were placed on/below the electrode plates so as
to produce a uniform pressure on the MRE sample.
The standard weight was instantaneously applied to
load a step normal pressure, maintained for 180 s to
fully observe the capacitance creep process. At 180 s,
the pressure was instantly unloaded, and the capaci-
tance recovery process was recorded. A force sensor
was placed below the sensing unit to monitor the nor-
mal pressure versus time. The LCR meter (1 kHz, 1 V
a.c.) recorded the real time response of capacitance to
pressure and saved the data in the computer. Except
the influencing factor of constant pressure, 50 kPa
(within the linear visco-elastic range of all samples) was
used for all factors affecting the capacitance creep-
recovery behavior in this study.
Both the piezo-capacitive property (i.e. capacitance
versus pressure) and repeatability were tested by an elec-
tronic universal testing machine (ETM503B, Wance
Test Equipment Co., Ltd., China). The test was a quasi-
static response process with a loading rate of 4 mm/min,
in a pressure range of 0–150 kPa. The repeatability test
adopted a loading rate of 30 mm/min and an unloading
rate of 80 mm/min to approximate the effect of instan-
taneous loading (150 kPa) and unloading (0 kPa). The
pressure (150 kPa) was loaded for 15 s and the zero-
pressure state after unloading lasted 30 s. All experi-
ments were carried out at room temperature (25°C).
3. Results and discussion
3.1. Capacitance creep-recovery characteristics of
MRE
From Figure 2(b.1), we can clearly observe the capaci-
tance creep and recovery phenomenon of MRE (sam-
ple of Group E, constant pressure = 100 kPa). Note
that the ordinate is the fractional capacitance change
(i.e. DC/C0). Comparing Figure 2(b.1) with 1(c), they
1424
Figure 2. (a) Schematic of experimental setup for capacitance creep-recovery measurement, (b) capacitance creep-recovery curves
for MRE (Group E) when loading and unloading, (b.1) a constant pressure of 100 kPa, and (b.2) a constant strain of 22%
(corresponding to initial pressure of 100 kPa).
indicate that the capacitance (electrical) creep and
recovery process has a very similar profile with the
strain (mechanical) counterpart (Yao et al., 2013).
This manifests an intrinsic relation between the electri-
cal and mechanical creep-recovery behaviors. Based on
the typical strain creep and recovery process of viscoe-
lastic materials in Figure 1(c), we also divide the capa-
citance creep process of MRE into three stages:
the instantaneous responsive capacitance, capacitance
primary creep, and capacitance secondary creep.
Correspondingly, the recovery process includes the
instantaneous recovery capacitance, elastic recovery
capacitance and residual capacitance. All the stages are
labeled in Figure 2(b.1). At the instant of loading the
pressure, the capacitance responds very quickly with a
rapid rise (instantaneous responsive capacitance, DC/
C0 = 2.80). Then, it grows more and more slowly with
time (capacitance primary creep DC/C0 = 3.05), and
finally tends to increase linearly (capacitance secondary
creep, DC/C0 = 0.20). When unloading the pressure,
the capacitance drastically dropped first (instantaneous
recovery capacitance, DC/C0 = 5.65) and then tends to
be stable (elastic recovery capacitance, DC/C0 = 0.25).
However, the capacitance is slightly higher than its ini-
tial zero value (residual capacitance, DC/C0 = 0.15)
due to the unrecoverable creep. According to the creep
phase in Figure 2(b.1), it is worth mentioning that, the
capacitance of the MRE sensors has a significant time
dependence, which may restrict their applications on
situations where long-term pressure is imposed.
However, the slight residual capacitance in the recovery
phase indicates that the irreversible damage caused by
creep to the performance of the sensors could be negli-
gible, which will be discussed in more detail later.
3.2. Role of effect of particles rearrangement
In our earlier research (Fan et al., 2017, 2018), it has
been known that the piezo-capacitive effect of MRE
Journal of Intelligent Material Systems and Structures 32(13)
mainly comes from the spatial redistribution of parti-
cles (i.e. particles rearrangement) during the compres-
sion and decompression. This is described in detail as,
the micro-capacitors constituted by adjacent particles
separate and repair, which further changes the number
of micro-capacitors connected in series and in parallel
between the electrode plates. Since the dielectric con-
stant of silicone rubber matrix is invariable, it is the
particles rearrangement within the matrix that varies
the dielectric constant and, hence, dominates the piezo-
capacitive effect (Fan et al., 2017, 2018). Further, the
compressibility of the solid particles is negligible, while
the silicone rubber has a significant viscoelasticity.
Therefore, our hypothesis arises, that is, the strain creep
of MRE could be attributed to the deformation of the
silicone rubber matrix under a constant pressure, but
the capacitance creep should be directly dominated by
the particles rearrangement.
Overall, it is reasonable to confirm that two factors
could be responsible for the capacitance creep under
constant pressure: the strain creep of matrix and/or the
particles rearrangement. However, we cannot distin-
guish their contributions since the strain creep and
capacitance creep occur simultaneously during loading
a constant pressure. Therefore, it is necessary to design
an appropriate experiment to separate these two fac-
tors. When loading a constant strain, the impact of
strain creep of the silicone rubber matrix can be elimi-
nated in spite of stress relaxation. Thus, the capacitance
creep measurement at a constant strain is meaningful
to verify whether the particles rearrangement promotes
the capacitance creep of MRE. Figure 2(b.2) presents
the data (sample of Group E), where significant capaci-
tance creep was still observed at the constant strain of
22% (corresponding to initial pressure of 100 kPa).
This fact strongly demonstrates that the particles rear-
rangement of MRE should be the direct cause of the
capacitance creep. Because, in the condition of constant
strain, only the process in which the spatial distribution
Fan et al. 1425

Figure 3. Illustration of mechanism of the capacitance creep and recovery behavior of MRE. The intrinsic secret of capacitance
creep of MRE is the viscously-delayed time-dependent elastic deformation of the insulating flexible matrix that motivates the
movement of the dispersed conducting particles (i.e. particles rearrangement that dominates dielectric constant of MRE). The elastic
effect of flexible matrix between adjacent particles is depicted by spring elements. (a) Initial state without external pressure. The
initial longitudinal interparticle gap (wi) is equal to the initial horizontal interparticle gap (li). (b) Moment after loading a step pressure.
wm is forced to suddenly decrease by the step pressure, and wm would be smaller than lm due to anisotropic internal stress.
Meanwhile, particles number nm in column becomes reduced but columns mm grows, indicating that particles rearrangement takes
place. (c) Duration of maintaining the constant pressure. There is a spontaneous trend that the interparticle gaps tend to be finally
equal, and thus, wp tends to approach lp. In this process, particles rearrangement happens when particles number np in column
declines and columns mp grows. (d) Approximately recovered initial distribution of particles as the pressure is released, leaving an
unrecovered residual strain and residual capacitance. Note that the viscous damping effect between particles and matrix is very
important and reflected in these figures but the dashpot elements are not presented for simplification.

of the particles changes with time exists. Furthermore,
the capacitance creep under constant pressure in Figure
2(b.1) is relatively more pronounced than the one under
constant strain in Figure 2(b.2). Since the strain creep
of silicone rubber matrix takes place in the sample of
Figure 2(b.1) but not in that of Figure 2(b.2) where the
constant strain was maintained, we can infer that the
strain has another effect on the capacitance creep as
well. It is this strain creep that enhances the particles
rearrangement because it strengthens the normal com-
pression as well as the transverse expansion for the
position self-adjustment of the dispersed particles in
MRE. In brief, particles rearrangement is the direct
cause of the capacitance creep, while the strain creep is
an indirect cause contributing by enhancing the parti-
cles rearrangement.
It should be noted that since MRE is a sensing mate-
rial used for flexible tactile sensors, it is the response of
the material to external forces that matters. Hence, this
study will not focus on the situations under constant
strain hereinafter.
3.3. Qualitative mechanism of capacitance creep-
recovery behavior of MRE
The strain creep of polymer materials subjected to
external force primarily comes from the following two
deformations: the elastic deformation due to the exten-
sion or compression of molecular chains by the seg-
ments movement, and the viscous deformation due to
the relative slip between molecular chains (Trantina,
1986). Viscoelastic models for polymer composites are
typically described by combination of spring and dash-
pot, such as Maxwell model (Jiménez et al., 2002) and
Kelvin model (Alzoubi et al., 2016; Schutter, 1999). As
discussed above, the particles rearrangement that domi-
nates the dielectric constant of MRE is the direct cause
of the capacitance creep, while the strain creep of sili-
cone rubber matrix is an indirect cause by inducing the
particles rearrangement. In other words, the electrical
creep is induced by the mechanical strain creep under
constant pressure. The next step is to further under-
stand the relationship between these two factors.
The capacitance creep of MRE displays the depen-
dence of capacitance on time, then the particles rearran-
gement should also have a time dependent behavior,
which microscopically is the mechanical movement of
particles under compression. Besides, it is within the
flexible silicone rubber matrix that the dispersed parti-
cles move. Thus, to understand the capacitance creep
and recovery, we need to look into the microscopic
state of the mixture during loading a constant pressure.
Figure 3 illustrates a mechanism of the capacitance
creep and recovery behavior of MRE. For simplifica-
tion, the particles are ideally aligned into chain-like
structures between the electrode plates due to the mag-
netorheological effect during solidification of MRE
(Romeis et al., 2019; Semisalova et al., 2013). Suppose
there are n particles in each column, m columns between
the electrode plates, and the matrix viscosity could be
ignored, we employ an ideal spring model to character-
ize the elasticity of silicone rubber matrix. However,
there is viscous effect existing in the polymer matrix in
reality, and especially between the particles and matrix.
1426
As a matter of fact, it is the viscous effect that causes
the inertia of elasticity (i.e. delayed deformation) of the
silicone rubber matrix. Since the dispersed particles are
separated by the matrix, the movement of particles are
actually driven by the elasticity of matrix. To illustrate
the mechanism of the creep and recovery behavior of
MRE more clearly, the model in Figure 3 does not pres-
ent the dashpot elements. But, it is worth again pointing
out that the model already reflects their effect.
In Figure 3, the elastic effect of silicone rubber
matrix between adjacent particles is depicted by the
spring elements. Figure 3(a) shows the initial state with-
out external pressure. There are ni particles connected
in series in each column and these columns further con-
nect in parallel, which lay the foundation for the macro
capacitance evaluation (Fan et al., 2017). Assuming
that the particles are uniformly distributed, the initial
longitudinal interparticle gap (wi) is equal to the initial
horizontal interparticle gap (li). Note that wi and li also
denote the length of springs between the adjacent parti-
cles. Besides, Li and Wi denote the macroscopic length/
diameter and width of MRE, respectively. The initial
fractional capacitance change is very small because
there is no particles rearrangement (i.e. very small ini-
tial dielectric constant of MRE) (Fan et al., 2017,
2018).
Figure 3(b) presents the situation after loading a step
pressure P. At this moment, a MRE sample is suddenly
compressed (i.e. Wm \ Wi), and the MRE should be
horizontally expanded (i.e. Lm . Li) because it tends to
remain the initial overall volume. Therefore, the parti-
cles number nm in each column diminishes (i.e. nm \ ni)
but columns number mm grows (i.e. mm . mi), indicat-
ing that particles rearrangement takes place. In this
stage, the particles are instantaneously rearranged to
remarkably increase the dielectric constant so that the
macro capacitance leaps. This stage corresponds to the
instantaneous responsive capacitance phase in Figure
2(b.1). However, the internal stress within the MRE at
this moment may be anisotropic due to the viscous
damping effect, that is, the internal longitudinal stress
should be greater than the horizontal stress. The reason
is that the longitudinal springs are compressed more
intensively and are not able to recover instantaneously
because of viscous damping effect. Therefore, the longi-
tudinal interparticle gap wm is decreased (i.e. wm \ wi)
and it should be smaller than the horizontal one (i.e.
wm \ lm).
As time goes on, the internal stress becomes isotropic
spontaneously, that is, the interparticle gaps in different
directions tend to be finally equal. Thus, as shown in
Figure 3(c), wp tends to increase (i.e. wp . wm) and
approach lp (i.e. wp!lp). Namely, some longitudinal
springs might become horizontally oriented in order to
release their concentrated stress. In this process, some
particles may move out of their previous columns and
into new columns (i.e. np \ nm and mp . mm). Particles
Journal of Intelligent Material Systems and Structures 32(13)
rearrangement happens and leads to the primary and
the secondary creep phases of capacitance in Figure
2(b.1). Meanwhile, because the internal longitudinal
stress is being released and some particles are moving
horizontally, the maintained external constant pressure
will impose a little further compression on the MRE
(i.e. Wp \ Wm and Lp . Lm). This effect will also
enhance the particles rearrangement in this process.
In the final stage, upon releasing the pressure, all the
springs recovers rapidly (a little irreversible strain
remained) and, hence, the particles approximately
return to their initial distribution. Therefore, the macro
capacitance drops (see Figure 2(b.1)) due to the disap-
pearance of particles rearrangement or the recovered
dielectric constant. However, the unrecoverable viscous
strain, which makes the particles unable to return to
their exact original positions, results in a small amount
of residual capacitance.
In summary, the capacitance creep behavior of
MRE can be well interpreted by the evolution of parti-
cles rearrangement which is driven by the mechanical
strain creep of the flexible matrix. In simpler terms, the
electrical creep is induced by the mechanical creep. The
intrinsic secret is the viscously-delayed time-dependent
elastic deformation of the insulating flexible matrix that
motivates the movement of the dispersed conducting
particles which dominates the dielectric constant of
MRE. It is worth noting that the varying longitudinal
interparticle gaps will also affect the capacitance (Fan
et al., 2017), but only the dominant particles rearrange-
ment is considered here for simplification.
3.4. Factors affecting the capacitance creep-recovery
behavior of MRE
From the above analysis we have known that the parti-
cles rearrangement is the direct cause of the capacitance
creep-recovery behavior. In fact, the particles rearran-
gement is indirectly influenced by the sample’s config-
uration parameters and the test conditions. Here we
focus on the following influencing factors, that is, the
curing magnetic field flux density, particles volume frac-
tion, particle size, matrix flexibility, constant pressure
level, and loading time of pressure. Investigation of
these influencing factors will give further understanding
of the mechanisms.
3.4.1. Effect of curing field strength. Figure 4(a) shows the
effect of the curing field strength Bcuring on the capaci-
tance creep-recovery behavior (samples from Group
A). It can be clearly seen from the creep stage in Figure
4(a) that the greater the curing field Bcuring, the higher
the curves. This apparently indicates that the piezo-
capacitive effect is positively affected by Bcuring (Fan
et al., 2018). Secondly, from the slope of the creep
curves, the capacitance has a slight tendency to
Fan et al.
(a)
(d)
Figure 4. Factors affecting capacitance creep-recovery behavior: (a) curing magnetic field flux density Bcuring, (b) particles volume
fraction, (c) particle size, (d) matrix flexibility, (e) pressure level, and (f) loading time of pressure.
strengthen with Bcuring. It is ascertained in our previous
research that as Bcuring increases, the particles form lon-
ger and thicker chains, and the initial average inter-
particle gap decreases, leading to a stronger piezo-
capacitive effect (Fan et al., 2018). In the instantaneous
response phase, the instantaneous responsive capaci-
tance significantly jumps with Bcuring because of the
instantaneously strengthened particles rearrangement
(see Figure 3). In the creep stage, the internal stress
tends to be isotropic, resulting in continued particles
rearrangement, and hence, the capacitance grows over
time. After unloading the external pressure, all the sam-
ples recovered rapidly, but the ones cured at stronger
magnetic fields have relatively poorer recovery ability.
Specifically, the residual capacitance values were 0.05,
0.05, 0.06, 0.08 for Bcuring at 0, 0.2, 0.4, 0.6 T, respec-
tively. This could be due to that, larger Bcuring increases
the local particles volume fraction in the microscopic
particle chains. Thus, there is a higher possibility that
some particles cannot return to their initial positions
after the creep due to the complex mutual interference.
3.4.2. Effect of particles volume fraction. Figure 4(b) corre-
sponds to the effect of particles volume fraction on the
creep and recovery of MRE (samples from Group B).
Similar to the effect of curing field strength, the larger
1427
(b) (c)
(e) (f)
the particles volume fraction, the more the piezo-
capacitive effect is enhanced. The reason could be
described as, smaller initial inter-particle gaps are
established as the particles volume fraction or concen-
tration increases, which is advantageous for particles
rearrangement to occur on a larger scale (Fan et al.,
2017). To be specific, more particles participate in the
particles rearrangement at the moment of loading pres-
sure, which features a more rapidly increasing instanta-
neous responsive capacitance. This trend would also
work for the creep phases. After unloading the pres-
sure, more particles in the MRE with a larger concen-
tration cannot return to their original positions, and
thus the residual capacitance slightly grows with this
factor (0.04, 0.08, 0.13, respectively).
3.4.3. Effect of particle size. The experimental results of
the effect of particle size on the creep-recovery behavior
of MRE (samples from Group C) are shown in Figure
4(c). It presents that the smaller the particle size, the
more pronounced the piezo-capacitive effect and the
more significant the capacitance creep. On one hand, at
the same particles volume fraction, a greater number of
particles are contained in the MRE with smaller-sized
particles. In other words, more particles forming more
micro-capacitors are involved in the particles
1428
rearrangement during compression. Because the parti-
cles rearrangement dominates the capacitance creep,
larger instantaneous responsive capacitance and more
distinct capacitance creep are attained. On the other
hand, the Young’s modulus of MRE having smaller-
sized particles tends to be smaller, which enlarges the
strain creep under the same constant pressure (50 kPa)
and, further induces a stronger particles rearrangement.
Similarly, after unloading the pressure, the residual
capacitance was observed to relatively increase with the
overall amount of particles, and they were calculated as
0.08, 0.08, and 1.20 respectively for samples filled with
30, 0.6, 0.5 mm particles.
3.4.4. Effect of matrix flexibility. The matrix composition
includes the silicone RTV-2 and silicone oil. During the
curing process of MRE, RTV-2 silicone rubber under-
goes chemical cross-linking reactions, and the molecu-
lar chains link each other to make the MRE transition
from fluid to viscoelastic solid. Silicone oil having low
molecular weight adjusts the Young’s modulus of
MRE for the best bionic flexibility (Fan et al., 2017).
The higher the silicone oil concentration, the lower the
silicone rubber matrix polymerization degree, and the
smaller the Young’s modulus of the MRE. It can be
found in Figure 4(d) (samples from Group D) that the
capacitance creep and recovery of MRE has an appar-
ent dependence on the matrix composition or flexibil-
ity. Similar to the result caused by smaller particle size,
with the increase of silicon oil content, the piezo-
capacitive effect becomes more significant and the
capacitance creep is stronger. The reason is that the
reduced Young’s modulus leads to the increase of strain
creep under the constant pressure, which enhances the
particles rearrangement. Moreover, the residual capaci-
tance also has the same trend, which are respectively
0.03, 0.08, and 0.12 in Figure 4(d).
3.4.5. Effect of the constant pressure. The constant pres-
sure could have an effect on the creep and recovery of
MRE. To investigate this, MREs (samples from Group
E) with particles volume fraction of 10 vol% (Bcuring =
0.6 T) was used for experiments under various constant
pressures. It is important to determine the pressure
range for the experiments. The upper pressure limit of
the effective working range of the MRE is approxi-
mately 200 kPa (Fan et al., 2018). When the pressure
exceeds the threshold of 200 kPa, some particles may
contact with their neighbors due to an excessive strain,
resulting in disappearance of some micro-capacitors
(Fan et al., 2018). Meanwhile, the silicone rubber
matrix undergoes an excessive viscous strain and, hence
many particles cannot return to their initial positions
after unloading the pressure. Therefore, we limited the
pressures to below 200 kPa, that is, 30, 50, 100, and
150 kPa, respectively. It can be seen from Figure 4(e)
Journal of Intelligent Material Systems and Structures 32(13)
that the constant pressure is an important factor affect-
ing the capacitance creep and recovery of MRE. It
serves as a positive role in promoting the creep as well
as the residual capacitance (0.08, 0.08, 0.15, and 0.30
with increasing the pressure, respectively). This is
because the magnitude of the pressure directly deter-
mines the strain level of MRE, and larger compression
further leads to a more pronounced particles rearrange-
ment. In Figure 4(e), all the residual capacitances,
which represent the irreversible damages of the creeps
to the sensing materials, are very small under such pres-
sures. This implies that the residual impact of the capa-
citance creep could be negligible even under long-term
application of pressure up to 150 kPa.
3.4.6. Effect of loading time of pressure. Figure 4(f) shows
the effect of loading time of pressure on the capacitance
creep-recovery behavior. The pressure of 150 kPa is
maintained for 150, 180, and 210 s, respectively. When
the pressure is instantly unloaded, the capacitance
drops immediately, and then tends to be stable.
However, the curve for 210 s tends to decline a little
more slowly and its residual capacitance is slightly
greater than those for 150 and 180 s. This should be
due to that more particles cannot recover their initial
distribution at a longer loading time of pressure, even-
tually leading to the unrecoverable creep.
It is worth pointing out that even though the creep
phases vary with the various factors above, the very
small residual capacitances in their recovery phases tell
that the irreversible damage caused by the creep to the
performance of the MRE sensors could be acceptable.
3.5. Effect of capacitance creep on piezo-capacitive
property of MRE
3.5.1. Irreversible effect of capacitance creep. As a sensing
material, the degree of variation of the piezo-capacitive
property of MRE caused by creep is of particular con-
cern. We performed an investigation by first testing the
piezo-capacitive curve (capacitance versus pressure) of
a sample from Group E so as to obtain a reference
(Figure 5(a)). Then, a new sample underwent a creep-
recovery test (capacitance versus time) at a constant
pressure of 150 kPa. This sample was then measured
again to obtain its piezo-capacitive curve (capacitance
versus pressure), which was further compared with the
reference. Considering that in Figure 4(e) the most resi-
dual capacitance occurred at 150 kPa, implying that it
should produce the most damage to the sample. Hence,
we here selected 150 kPa for the creep-recovery test to
investigate the maximum impact on the piezo-capacitive
property (shown in Figure 5(a)). It can be seen that the
two curves before and after creep do not overlap, indi-
cating that the creep has an irreversible effect to some
extent on the sensing property. A reason is that, during
Fan et al. 1429

(a) (b)

(c) (d)
Figure 5. (a) Comparison of piezo-capacitive curves of MRE before and after a capacitance creep-recovery test, (b) compression
repeatability tests, (c) 200 impulsive loading/unloading repeatability tests of MRE after a creep test (constant pressure = 150 kPa), and
(d) comparison of capacitance creep-recovery behavior (150 kPa) before and after 200 impulse loading/unloading repeatability tests.

the creep triggered by long-term pressure, although
most particles move in the elastic ranges, there are still
a few particles failing to return to their original posi-
tions after the external force is removed. In Figure 5(a),
there is an extra reason why the curve after creep is
lower than the pre-creep one. Namely, the residual
capacitance after creep raised (was equal to) the new
zero-pressure capacitance, which simply reduced the
fractional capacitance changes in value.
3.5.2. ‘‘Self-healing’’ of MRE. Although there is an irrever-
sible effect of creep on the piezo-capacitive property of
MRE found in Figure 5(a), here we further explore its
effect in practical applications. Firstly, samples from
Group E were performed creep tests under the large
constant pressure of 150 kPa. Secondly, to simulate the
situation in reality, we performed compression repeat-
ability tests (Figure 5(b)) and impulsive loading/unload-
ing repeatability tests (Figure 5(c)) for the samples.
These two experiments represent the common working
situations in practice for continuous loading and
impulse loading. At last, we focused back on the varia-
tion in the creep-recovery behavior of MRE before and
after the repeatability tests.
As can be seen from Figure 5(b), the piezo-capacitive
curve after creep tends to decline with increase in the
cycles of continuous compression tests. Specifically, the
curves of the first 10 cycles show more downward trend,
while the curves of the 10th to 30th tests become closer
and closer until they almost overlap and no longer
change. In Figure 5(c), the peak of the fractional capa-
citance change (i.e. DC/C0) goes downwards notably
(;0.7) during 1 to 80 cycles, but then levels off from 80
through 200 cycles. Here the deviation D = (initial
value—stable value)/stable value is defined and it is
around 13% for the tests in Figure 5(c). The repeatabil-
ity tests present us that although the capacitance creep
has an effect on the piezo-capacitive sensing property, it
would recover and become stable after a certain time of
repeatability tests. This ability of ‘‘self-healing’’ means
1430
that the MRE sensors can obtain stable sensing capabil-
ity after an initial pre-processing at the factory.
Figure 5(d) exhibits two creep-recovery curves of the
sample before and after 200 impulse loading/unloading
repeatability tests in Figure 5(c). Apparently, the creep
slope and the residual capacitance of the latter are
smaller than those of the former, indicating that the
creep effect is reduced after the repeatability tests. This
behavior implies that the dispersed particles reach a
more stable distribution after the repeatability tests,
where the internal stress could be eliminated and the
particles find a ‘‘comfortable zone’’ with more linear
elasticity. In all, as long as the working range is not
exceeded, MRE can have a good repeatability and the
ability of ‘‘self-healing’’ is able to reduce the creep
effect.
4. Conclusion
MREs are emerging conductive elastomers filled with
micron-/nano-particles, which are a novel generation of
sensing material for flexible tactile sensors. The research
on the capacitance creep and recovery not only pro-
vides knowledge for MREs on their dependence of
capacitance on time, but also a further understanding
of the unique mechanism of particles rearrangement.
The capacitance creep and recovery have a very sim-
ilar profile to the strain counterpart. This manifests an
intrinsic relation between the electrical and mechanical
creep-recovery behaviors. All the influencing factors
(except particle size), that is, the curing magnetic field
flux density, particles volume fraction, matrix flexibil-
ity, constant pressure level and loading time of pressure
serve as positive roles in promoting the creep as well as
the residual capacitance. On the contrary, the smaller
the particle size, the more pronounced the capacitance
creep, and the more notable the residual capacitance.
There is a common mechanism for all such factors
enhancing the creep, that is, the particles rearrange-
ment directly strengthened by the factors or indirectly
strengthened by the increased strain creep. Besides, the
mechanism for the residual effect is that some particles
cannot return to their initial positions after the creep
due to complex mutual interference.
Although there is an irreversible effect of creep on
the piezo-capacitive property of MRE, the residual
capacitance, which represents the irreversible damage
of the creep to MRE, is always very small. This implies
that the irreversible damage caused by the creep to the
performance of the MRE sensors could be acceptable.
The creep effect is reduced after the repeatability tests,
exhibiting a ‘‘self-healing’’ behavior. This ability of
‘‘self-healing’’ indicates that the MRE sensors can
Journal of Intelligent Material Systems and Structures 32(13)
obtain stable sensing capability after an initial pre-
processing at the factory.
Especially, as a core contribution of this study, a
qualitative mechanism analysis was performed at the
micro level. The fact of the capacitance creep and
recovery phenomenon of MRE under constant strain
strongly demonstrates that the particles rearrangement
is the direct cause of the capacitance creep, while the
strain creep is an indirect cause by inducing the parti-
cles rearrangement. The elastic behavior of flexible
matrix between adjacent particles is elaborated through
the spring models. The viscous effect causes the elasti-
city inertia (i.e. delayed deformation) of the springs.
Since the particles are dispersed in the matrix sepa-
rately, the movement of them are actually driven by the
elasticity of matrix. The capacitance creep behavior of
MRE can be well interpreted by the evolution of the
particles rearrangement dominated by the mechanical
strain creep of the silicone rubber matrix. To put it sim-
ply, the electrical creep is induced by the mechanical
creep. The intrinsic secret is the viscously-delayed time-
dependent elastic deformation of the insulating flexible
matrix that motivates the movement of the dispersed
conducting particles which dominates the dielectric
constant of MRE. The detailed mechanism of the creep
behaviors obtained in this study provide us deep
insights into the time-dependent influencing factors.
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 sup-
port for the research, authorship, and/or publication of this
article: This research was financially supported by the
National Natural Science Foundation of China (11802046 &
11702040), and additionally supported by Fundamental
Research Funds for the Central Universities (2019CDJ
GFGD006), Chongqing Basic Research and Frontier
Exploration project (cstc2019jcyj-msxmX0483, cstc2018jcyj
AX0591, cstc2018jcyiAX0023), the Science and Technology
Research Program of Chongqing Municipal Education
Commission (KJQN201801510), National Training Program
of Innovation and Entrepreneurship for Undergraduates
(201910611040), and Chongqing Key Research and
Development Project on Major Themes of Artificial Intelligence
Technological Innovation (cstc2017rgzn-zdyfX0036).
ORCID iDs
Changrong Liao https://orcid.org/0000-0002-1837-1083
Lei Xie https://orcid.org/0000-0002-0775-7466
Fan et al.
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