1 s2.0 S0142941821000659 Main
1 s2.0 S0142941821000659 Main
1 s2.0 S0142941821000659 Main
Polymer Testing
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A R T I C L E I N F O A B S T R A C T
Keywords: Greater demands for underwater sound absorption materials have been growing due to the concern about un
Polymer-based derwater noise control in water. Among the range of existing materials, polymer-based materials are increasingly
Acoustic property being utilized as underwater sound absorption materials. In this paper, different kinds of polymer-based mate
Underwater sound absorption
rials for underwater sound absorption with regards to key factors associated with sound absorption properties,
measurements, applications, and mechanisms are reviewed and summarized. Commonly used polymers for
underwater sound comprise, in general, interpenetrating polymer networks (IPN), polymer foams, and gradient
polymers. To further improve underwater sound absorption performance, different types of inclusions that are
introduced into the polymer matrix to transform the polymers as underwater sound absorption materials via air
voids, solid inclusions, nanofillers, and phononic crystals are discussed. Challenges for further development of
better polymer-based acoustic materials to meet requirements of current and future underwater applications are
also presented.
1. Introduction materials and passive materials [10]. Compared with active materials,
passive materials have received more attention and wider applications
Noise pollution affects not only the well-being of humans on land but because of their high performance-cast ratio, easy fabrication, and
also marine life of aquatic species and sanctuaries residing in the earth’s reliable service [11]. Passive underwater sound absorption materials
vast oceans. Worldwide human activities and the globalization of the can be metal-based [12–14], wood-based [15] and polymer-based [16].
economy have certainly led to increasing maritime traffic and anthro Theoretical research indicates that underwater sound absorption
pogenic noise [1] which, in turn, have impacted much of the marine life materials should satisfy two important principles: (I) The characteristic
in oceans [2–4]. Nevertheless, much effort has also been directed to impedance should match with the water impedance to decrease the
wards the development of underwater vehicles (such as submarines) to reflection of incident sound waves; and (II) the attenuation properties of
be undetected through the sonar system [5]. Essentially, there are two materials should be high enough to absorb the penetrated sound waves
main types of applications for underwater sound absorption materials: [7,17,18]. Polymer materials usually have close acoustic impedance
(i) reduction of noise radiated from underwater vehicles and (ii) with water, and some have damping property, so most underwater
reduction of acoustic target strength of underwater vehicles. For the first sound absorption materials are polymer-based. Besides, polymer mate
type applications, the sound absorption frequency range is audio from rials have excellent weather & abrasion resistance, very good resistance
50 Hz to 10,000 Hz [6]. For the second type, the frequency range is to corrosion, water, heat, ozone & oxidation, good thermal/electrical
determined by the sonar system, and the advanced sonar system has a insulation properties, low cost, and easy fabrication, which also make
wide working frequency range from 1 kHz to 30 kHz [7]. Because of the them very suitable for underwater applications [19,20]. Commonly used
wide interests and concerns about underwater sound absorption mate polymers for underwater sound absorption include interpenetrating
rials [3,8], many materials have been used for underwater sound ab polymer networks (IPN), polymer foams, and gradient polymers. In
sorption [9]. However, different from airborne sound absorption order to further improve the underwater sound absorption performance,
materials, underwater sound absorption materials are required to different types of inclusions are introduced into the polymer matrix.
withstand harsher environment, especially beneath the depths of the Typical inclusions are air voids and solid inclusions. With the develop
ocean. Underwater sound absorption materials include both active ment of nanotechnology and local resonances, nanofiller and phonoic
* Corresponding author.
E-mail address: [email protected] (Y. Fu).
https://doi.org/10.1016/j.polymertesting.2021.107115
Received 24 August 2020; Received in revised form 29 December 2020; Accepted 2 February 2021
Available online 6 February 2021
0142-9418/© 2021 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
Y. Fu et al. Polymer Testing 96 (2021) 107115
crystals are applied to improve the underwater sound absorption per seen as electric current. The acoustic impedance Z can be calculated as:
formance [21–23].
Although sound absorption in water is an important topic for both Z = p/v (2)
research and application, few reviews have been written on this topic. The unit of Z is Pa ⋅ s/m or Rayl (1 Rayl = 1 Pa s/m). For ideal
Bajram et al. [24] reviewed measurement and testing of the underwater medium with infinite thickness and one-dimensional sound, character
acoustic properties of materials. In Ref. [25] acoustic metamaterials and istic specific acoustic impedance Z0 is used.
underwater acoustics applications were introduced in chapter 5.
Recently, one conference paper gave a brief summary of underwater Z0 = ρc (3)
sound absorption materials [26]. However, to the best knowledge of us,
Where ρ is the volumetric mass density of the medium, and c is the speed
there is no relevant review paper on a systematic review about under
of the sound waves travelling in the medium.
water sound absorption from the aspect of polymer-based materials
To minimize sound reflection on the interface, two materials should
although they are commonly used for sound absorption in water. This
have similar impedance values. The impedance of water is 1.56 × 106
review attempts to gather the state of art about polymer-based materials
Rayl, which is much higher than that of air. As a result of impedance
for underwater sound absorption. It is expected that this work can
mismatch, most sound absorption materials in air cannot work in water.
benefit the studies for underwater sound absorption materials.
Many materials’ characteristic specific acoustic impedances are given in
This paper, focusing on polymer-based materials, is organized as
Table 1. Compared to other common materials (e.g., cork, aluminum,
follows:
steel), impedances of most polymers (e.g., polydimethylsiloxane
(PDMS), polyurethane (PU), Epoxy, hydrogel) are much closer to that of
• Introducing the characteristics, key factors, measurements of un
water [27]. Therefore, these polymer materials have been used as the
derwater sound absorption materials inSections 2 and 3;
matrix for underwater acoustic applications.
• Reviewing and comparing critical and commonly used polymer
materials with and without inclusions for underwater sound ab
sorption as well as the mechanisms and applications in Sections 4 2.2. Dynamic modulus
and 5;
• Summarizing challenges and outlook of underwater sound absorp Sound can only propagate through elastic materials. With the irri
tion materials in Section 6. tation of sound waves, the polymer chains will be compressed and
elongated alternatively in micro/nano scale. Under this cyclic dynamic
2. Key factors of underwater sound absorption process, the strain will lag the stress with a phase angle, δ, that is be
tween 0 and π/2 radians [16]. The ratio of imaginary part to real part is
Accurate evaluations of underwater sound absorbing properties of the tangent of the phase angle δ, which is usually defined as the loss
acoustical elements are essential to underwater acoustic researches factor. High loss factor is critical for underwater sound absorption
[24]. As shown in Fig. 1, underwater sound absorption is defined as ratio materials.
of absorbed energy to incident energy noting the amount of sound being tanδ = E ’’/E ’ (4)
absorbed by a material.
E* = E ‘ + E ’’ j (5)
α = 1 − Ir/Ii − It/Ii (1)
Where E is the storage modulus, E is the loss modulus, and E * is
’ ’’
Where α, Ii, Ir, It are the sound absorption coefficient, intensity of the complex dynamic modulus. E’ is a measure of the energy stored elasti
incident sound, intensity of the reflected sound and intensity of the cally, while E’’ represents the equivalent energy loss (as heat) during the
transmitted sound, respectively. The underwater sound absorption collision.
properties are usually determined by materials’ acoustic impedance and The dynamic mechanical property E * can be used to evaluate the
loss factor. For applications in deep water, compressive strength is also a damping and absorption capability. The loss factor can be measured by
critical parameter. using Dynamic Mechanical Analysis (DMA) [35]. The higher the mate
rial’s loss factor tanδ, the better the damping property. As shown in
2.1. Acoustic impedance Table 2, polymer materials usually have high loss factors compared with
other materials (e.g., metal, glass) because of their long-chain
Acoustic impedance is a key parameter in the field of acoustics, molecules.
which is analogous to resistance in the field of electricity. Sound pres
sure p can be seen as voltage, while sound speed v in the material can be 2.3. Compressive strength
Table 1
Characteristic specific acoustic impedances of polymer materials in comparison
to some common materials.
No. Materials Density (kg/ Sound speed Impedance Ref.
m3) (m/s) (Rayl)
2
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3
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4
Y. Fu et al. Polymer Testing 96 (2021) 107115
Table 7
Polymers used for underwater acoustic matrix materials.
Category Materials Ref.
Rubber Butyl rubber, nitrile butadiene rubber, styrene-butadiene rubber (SBR), silicon rubber (PDMS, Ecoflex) [9,19,28,34,81]
PU elastomer TDI- and IPDI-type PU, Ezecast PU and Encap PU [68,78,82]
Foam SiC foam, PU foam, expanded polystyrene foam [14,83–85]
Others Epoxy, hydrogel (PVA) [33,79,80]
Fig. 2. The influence of different type of epoxy resin and different type of isocyanate on the underwater acoustic properties of the EPU/EP = 70/30 IPN: (a)
fabrication, (b) acoustic absorption coefficient. (EPU1 TDI-type epoxyurethane, EPU2 IPDI-type epoxyurethane, E− 51 type Epoxy resin, E− 44 type Epoxy resin) [82].
5
Y. Fu et al. Polymer Testing 96 (2021) 107115
Fig. 3. (a) Photograph of Si foam sample, (b) SEM photographs of the cell structure, (c) triangular cross-section of hollow skeleton, (d) and micropores throughout
the strut of foam skeleton, (e) underwater acoustic absorption coefficient [83].
underwater applications. More recently, a new aerogel-graphite poly materials, which have equal impedance with water in the first layer, and
urethane spray foam composite shows the potential for absorbing the impedance rises with the increase of the layers [18]. Such a design
thermal and sound energy [94]. By using new production process, the realizes the multi-physics coupling requirement. A three-layer structure
foams’ microstructure can be adjusted, which can be a new way for the of different polyurethanes showed high sound absorption coefficient
design of polymer-based underwater sound absorption materials. from 2 kHz to 30 kHz [71]. Liu et al. [95] fabricated multilayer samples,
and the results showed that multilayer materials can have good broad
band absorption characteristics in different incident angles. However,
4.3. Gradient polymers the multilayer materials have high requirements on the fabrication
technology. The layers should be arranged in a specific order, and the air
To overcome the limitations of homogeneous materials, gradient bubbles between each layer are also required to be avoided.
impedance polymers have been proposed. As shown in Fig. 4, there are The other kind of gradient impedance materials are wedge materials,
two kinds of gradient impedance polymers. The first kind is multilayer
Fig. 4. Gradient impedance materials: (a) multilayer material, (b) wedge material.
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Y. Fu et al. Polymer Testing 96 (2021) 107115
which have gradually increasing volume weight from the exterior to the reptation back and forth along their length at Tg. When the sound fre
interior [96,97]. They are widely used in anechoic water tanks because quency equals the natural frequency of the polymer chain, an absorption
they have high sound absorption coefficient in broadband, especially peak is reached. The energy is converted into molecular motion (i.e.,
low frequency [7]. The shapes of the wedge have significant effect on the heat). As mentioned above, loss factor can be used to represent the
underwater sound absorption performance. These shapes can be distri damping ability. The frequency of excitation, temperature, molecular
butions of pyramids, cones with linear, optimally curved sides, a simple structure of polymers, and chemical cross-linking systems all affect the
liner run with a saw-tooth cross section, or even flat slabs of material of damping properties [16]. However, it is difficult to achieve high sound
various width extending out from the surface. Since the material re absorption coefficient only by the intrinsic damping properties. To
quirements for the wedge are not very restrictive, it can be constructed further improve the sound absorption properties, other mechanisms
using many commercially available materials. For example, wooden need to be introduced.
wedges are particularly low in cost and their fabrication is simple [98].
More generally, wedges are made of simple polymeric materials. These 4.4.2. Scattering and reflection
are typically more compact and more easily mounted but they are more Sound scattering is the specular reflection of waves from small seg
costly. It needs to be mentioned that air cavities have also been ments of a rough surface. Here it refers in particular to the scattering
embedded in wedge designs, so significant cost savings at low fre inside the material, so sound energy can be absorbed more in this pro
quencies can be achieved [99]. However, the thickness of the wedge cess compared with one-way propagation. For heterogeneous polymers,
material usually needs to be rather large, so their applications are very the impedances of different parts can be quite different, so sound waves
limited [100]. A summary of studies on the gradient impedance mate will be scattered on the interfaces of inhomogeneities in the matrix
rials for underwater sound absorption is listed in Table 9. These material. The benefit of scattering is the increase of the propagation
wedge-shaped samples in big size were measured in the acoustic water distance. In general, the thicker the sound absorption materials are, the
tank. better sound absorption performance they have. The thickness of the
sound absorption materials is very limited, and thick materials are more
costly or not practical for some applications. By scattering, the sound
4.4. Underwater sound absorption mechanisms
can propagate inside the material for longer distance and time, and thus
the sound can become easier to be absorbed, especially for polymer
Polymers absorb underwater sound mainly based on their intrinsic
foams [106]. As an analogy, tortuosity is used to quantify the effect for
properties and geometrical spreading. The mechanisms of sound ab
polymer foams as defined below [107].
sorption are discussed as following.
L
α∞ = (6)
4.4.1. Intrinsic absorption C
For homogenous polymers, the energy of sound waves can be con
verted from vibration into random thermal motion or heat by molecular where L is the propagated length, and C is the straight-line distance.
relaxation, usually with a negligible rise in temperature of the solid. Underwater sound absorption materials are usually attached with
According to the theory of polymer motion, the chains undergo backing materials, so the reflection occurs on these interfaces. It is
noteworthy that the direct reflection from the interface of air and water
brings a π phase shift, while the reflection from the interface of the steel
Table 9
and water has a zero-phase difference. Consequently, there is destructive
A summary of studies on the gradient impedance materials for underwater sound
absorption.
interference between the two paths. This can be used to transform a
perfect reflector into a perfect absorber [108].
No. Material and Sample size Frequency Sound Ref.
structure range absorption
coefficient
a
4.5. Applications
1 Different PU in 56 mm 2–30 kHz 0.85 [71]
each layer diameter
and 58 mm Quiet underwater environment is desired not only in the ocean but
thickness also in some underwater lab situations. The underwater noise pollution
2 Gradient PU 208 mm 1400–4000 0.7 [101] has attracted more attention from both scientific community and gov
a
diameter Hz ernment. High level impulsive sound waves may cause injuries or
3 Different layers 56.5 mm 3–7 kHz 0.7 [102]
of epoxy resin diameter
auditory troubles. This may happen particularly for active sonar pulses,
and 70 mm underwater air guns used for oil and gas explorations at sea, and marine
thickness pile driving (e.g., during the installation of offshore wind turbines);
4 Gradient 55 mm 2–10 kHz 0.8 [95] lower level but continuous sound has chronic effects. For example, the
composite with thickness
marine animals may not be injured by the sound source, but the inad
multiphase
5 SOAB wedges 100 mm 14-30 KHz – [103] equate soundscape can lead to auditory masking or behavior changes,
with width 25 thickness resulting in the long term to negative damages. This is the scenario for
mm noise footprints related to commercial ship traffic [2], offshore wind
6 Stepped – – – [104] farms [109], and marine renewable energy systems in operation [25].
converging
wedge-shaped
Especially, high energy demand has led to the increasing number of
duct offshore wind farms with high-power turbines, and many of them are
7 Wedges on a 800 mm 0.5–10 kHz – [105] being planned for the shallow water of the world’s marine habitats. Both
compound plate thickness construction and operation have severe impact on the marine environ
and cylindrical
ment [110,111]. To control the underwater noise, the European Com
shell structure
8 Multilayer 250 mm 3–25 kHz 0.9 [98] munity adopted Marine Strategy Framework Directive (MSFD) in 2008
absorber and thickness require the member states to take actions to achieve good ocean envi
wedge coating ronment status by 2020 [112]. Underwater sound absorption polymers
for water tanks can be applied on ship hulls, underwater operation platform, and un
a
Having good underwater sound absorption performance under high hydro derwater pipes to reduce the underwater noise. The abovementioned
static pressure. underwater noise is generally in the frequency range from 10 Hz to 10
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Y. Fu et al. Polymer Testing 96 (2021) 107115
cially, gradient polymer materials have been widely used in anechoic 1 Doubly periodic 40 mm 5–15 kHz 0.5–0.8 [118]
water tanks. The working frequency range of anechoic water tanks is cylinders with a thickness
diameter of 1.5 cm, a
usually broad, varying from several Hz to several kHz. Simulating ocean
height of 2 cm and a
depths can go down to 700 m (e.g., 7 MPa) or more [62], and some spacing 5 cm
gradient polymer materials with good compressive strength can be 2 Super ellipsoidal 20 mm 8–22 kHz 0.9 [119]
employed. In addition, some underwater acoustic sensors also require cavities in mm with thickness
careful integration during installation, so underwater sound absorption mixed sizes and
global optimal size
polymers are needed. 3 Cylindrical cavities 50 mm 1–2 kHz 0.9 [123]
of 15 mm height, 20 thickness
5. Improvement of sound absorption performance using mm diameter and a
inclusions grating spacing 30
mm
4 Cylinder with a 50 mm 500–1200 0.8 [124]
To further improve underwater sound absorption properties, diameter of 1.2 cm thickness Hz
different inclusions are embedded into the matrix materials. The first and a height of 3 cm
applied inclusion is air cavity or voids, which is a particularly simple backed by a rib-
resonator and well known to couple strongly with water-borne acoustic stiffened plate
5 Cavity with different 40 mm 2–25 kHz 0.9 [125]
waves [108]. While air voids are soft inclusions, so the poor compression material distribution thickness
resistant capability limits their applications. Some solid inclusions have configuration
been proposed to replace the soft inclusions [113]. These solid in 6 Three different 50 mm 1–10 kHz 0.6 [120]
clusions include steel cylinder, hollow glass sphere and carbon fiber, etc. shaped cavities thickness
(cylinder, cone and
With the development of nanotechnology, nanofillers are introduced to
horn)
underwater acoustics. Nanofillers have large specific surface area 7 Cylindrical cavities 35.9 mm 1.3–10 kHz 0.9 [121]
compared to traditional fillers; low loading fractions up to 0.1 wt% can of mixed sizes in mm thickness
significantly improve the materials’ properties [114]. To control sub 8 Two lossy nitrile – – – [126]
wavelength waves at low frequencies, localized resonances in phononic polymer layers the
base layer contained
crystals have been introduced to improve the low-frequency acoustic
cylindrical holes
absorption of viscoelastic materials [115].
8
Y. Fu et al. Polymer Testing 96 (2021) 107115
Fig. 5. Schematic of (a) traditional Alberich anechoic material and sound absorption performance [122], (b) Alberich anechoic material with mix sizes and sound
absorption performance from computational calculations (solid lines-total absorption cross section, dashed lines-the losses suffered within a surrounding sphere with
radius 10 mm) [119], (c) Alberich anechoic material with different shapes and sound absorption performance [120].
composite material resistant to pressure and substantially increases the Other researchers used steel cylinders as solid inclusion to replace air
shock resistance. In addition, HGS have small and controllable size as cylinders [113]. Sharma et al. [130] investigated underwater sound
shown in Fig. 6 (a). Therefore, HGS have attracted many attentions. Yu absorption of rubber coatings with periodic air voids and steel inclusions
et al. [127] studied underwater sound absorption of visco-elastic com as shown in Fig. 6(b). This combination was found to exhibit high sound
posites coating containing micro-spherical glass shell. It was found that absorption in a broad frequency range, which was not achieved using
the multilayer micro-spherical glass shells can improve sound absorp the corresponding designs comprising only voids or solid inclusions.
tion at low frequencies (2–4 kHz) and maintain the sound absorption Besides, steel spheres and aluminum spheres can also be successfully
coefficients above 0.7 at high frequencies (above 7 kHz). A patent for an employed as scattering effects to reduce acoustic reflections [131]. The
anechoic coating has been proposed, which comprised of a rubber ma results also showed the sound absorption performance had a close
trix having inclusions of glass spheres encapsulated rubber-like cores relationship with the sphere size and coating thickness. Solid inclusions
instead of air voids [128]. The resonance of the rubber cores with ferrite attached on the surface of the elastic coating can also realize sound
loading in combination with the matrix material dissipates acoustic absorption. Zhang et al. [132] found that steels periodically attached to
energy directed toward the composite material. As a result, better un the top surface of the elastic coating plays an important role in modi
derwater sound absorption performance can be obtained. Stainless steel fying the sound absorption, especially at low frequencies and/or the
hollow spheres were also studied [129]. 316L stainless steel hollow resonance frequencies of the trapped modes of the plate.
spheres (316L HS) were mixed with polyurethane and silicone rubber Some small particles can also enhance underwater sound absorption
matrix materials. It was found that silicone rubber with better molecular capability. For example, carbon fibers are also widely used to improve
flexibility was easier to reflect sound waves than polyurethane, while PU underwater sound absorption property, because they are already used to
was better at sound absorption. PU with 316L HS had better sound ab enhance mechanical properties of rubbers. Jung et al. [19,133] inves
sorption coefficient than silicone rubber with 316L HS. Its maximum tigated underwater acoustic properties of nitrile butadiene rubber (NBR)
sound absorption coefficient was 0.74 at 2650 Hz. specimens with carbon black and found that modified NBR can be a
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Y. Fu et al. Polymer Testing 96 (2021) 107115
Fig. 6. Schematic of (a) Epoxy resin/hollow glass microsphere composite acoustic materials and SEM images [134], (b) Steel and air inclusions and underwater
sound absorption coefficient (solid lines-analytical model, dashed lines-numerical simulation) [130].
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Y. Fu et al. Polymer Testing 96 (2021) 107115
unclear. Ayub et al. [54] studied the acoustic properties of CNTs forest. graphene, Gu et al. [78] studied the underwater acoustic properties of
It was found that a 3 mm thick layer of CNTs could provide up to 10% PU/CNTs nanocomposites. Measurement revealed that the underwater
acoustic absorption within the frequency range 0.125–4 kHz. The mo sound absorption coefficient of PU/CNTs nanocomposite increased as
lecular simulation studies based on CNTs found that acoustic absorption the content of CNTs increased to 1 wt%. Recently, PDMS/MWCNT
is associated with molecular interactions between acoustic waves and nanocomposite films also have been proven to have improved under
nanomaterials, and these interactions occur even at high frequency (GHz water sound absorption property [140]. It was found that MWCNT can
range) [139]. change the internal structure of PDMS. The introduced micro air bubbles
When it comes to underwater applications, it was also found that also made contribution to enhance the sound absorption performance
nanofillers can enhance underwater sound absorption property. As [141]. For other applications, the enhanced attenuation of sound in
mentioned above, some fillers in micro-size are found to improve un agar-gel phantoms was observed by introducing magnetic nanoparticles
derwater sound absorption including carbon fiber [10,68], hollow glass [142]. The obtained results can be used for modelling ultrasound
microspheres [134,135], etc. Furthermore, Li et al. [69] proved that propagation and heating in human tissues. Recently, natural bio-based
graphene/rubber nanocomposites exhibited excellent underwater sound Eucommia ulmoides gum (EUG) was dispersed in the SBR matrix as
absorption performance. The fabrication procedure of graphene/SBR nanocrystallites by two-roll mill mixing method. These nanocrystallites
nanocomposites via the spray-drying method is given in Fig. 7 (a). acted as physical crosslinking points and made SBR/EUG composites
Enhanced interface interaction between the fillers and fillers can be have two dynamic mechanical loss peaks. SBR/EUG composites pre
achieved. As shown in Fig. 7 (b), graphene sheets and rubber particles sented excellent pressure resistance and sound absorption capacity in
formed together, and were distributed in the rubber matrix evenly and the low-frequency region (3–8 kHz) [143]. The studies that focused on
continuously to form a network, which brought about multiple scat polymers with nanofillers for underwater sound absorption are sum
tering and wave-mode conversions to enhance sound absorption per marized in Table 12.
formance. Notably, average absorption coefficient > 0.8 was exhibited
at 6–30 kHz as displayed in Fig. 7 (c), and the performance could be
maintained under high hydrostatic pressure up to 3 MPa. Another 5.4. Polymer with phononic crystals
experiment indicated that graphene nanoplatelet modified
acrylonitrile-butadiene rubber based materials exhibited excellent Polymers with phononic crystals, also known as metamaterials, are
damping and underwater sound absorption properties [67]. Besides artificially created structures from cells with small wave dimensions that
can have effective properties not encountered in nature. Compared with
Fig. 7. Graphene/SBR nanocomposites: (a) fabrication procedure, (b) SEM images with changing filler content at different magnifications, (c) underwater absorption
coefficient [69].
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Y. Fu et al. Polymer Testing 96 (2021) 107115
Table 12 Table 13
A summary of studies on the polymers with nanofillers for underwater sound A summary of studies on the polymers with phononic crystals for underwater
absorption. sound absorption.
No. Nanofillers Sample size Frequency Sound Ref. No. Phononic crystals Sample Frequency Sound Ref.
range absorption size range absorption
coefficient coefficient
1 Nano-SiO2 57 mm 2–12 kHz 0.85 [89] 1 Steel cores (diameter 118 mm 800–1200 0.8 [150]
diameter 10 mm) with silicone diameter Hz
and 50 mm rubber embedded in and 55
thickness a viscoelastic mm
2 Reduced graphene 120 mm 6–30 kHz 0.8 [69] polymer thickness
a
oxide with diameter 2 Polyoxymethylene 1.8 mm 2–5 kHz 0.9 [151]
thickness and 25 mm (POM) sheet with thickness
3.4 nm thickness holes of diameter 8.6
3 Graphene 57 mm 2–30 kHz 0.73 [67] mm drilled through
nanoplatelets with diameter 3 A single layer of gas 0.23 mm 1–7 MHz 0.7 [108]
diameter 50 and 40 mm inclusions in PDMS thickness
− 65 nm and surface thickness 4 Sphere core with 20 mm 100–900 – [152]
area 206 m2/g radius 5 mm and thickness Hz
4 Carbon nanotubes – 2–6 kHz 0.5 [78] coating with radius
with diameter 20 8.5 mm
nm and length 10 5 Spiral-based local 4 mm 0.8–6 kHz 0.54 [153]
a
μm resonators with thickness
5 Carboxyl- 120 mm 1.5–7 kHz 0.9 [140] diameter 5 mm,
functionalized diameter length 22 mm
multi-walled and 10 mm 6 Helix metal in 210 mm 100–1000 0.8 [154]
carbon nanotube thickness viscoelastic damping thickness Hz
with diameter rubber
10–20 nm and 7 Epoxy as matrix, 50 mm 2–20 kHz 0.7 [79]
length 10–30 μm multilayer scatterers thickness
6 Fe3O4 nanoparticles – – – [142] made of soft rubber
with diameter and steel
64.9 nm 83.7 nm 8 Phononic glass in the 56 12–30 kHz 0.9 [14] a
a interpenetrating diameter
Having good underwater sound absorption performance under high hydro network structure of and 10
static pressure. a metal skeleton and mm
PU infillings thickness
other sound absorption materials, metamaterials have attracted signif a
Having good underwater sound absorption performance under high hydro
icant attention [23,144,145]. The concept of metamaterial originates static pressure.
from the field of electrodynamics. As shown in Fig. 8, the developing
process of metamaterials is from electrodynamics to optics to air kHz in both theoretical and experimental results of metamaterial sam
acoustic to underwater acoustics [146]. For traditional materials, the ples [150]. The phenomenon can be explained as a mass-spring analogy
density and elastic moduli are positive, but for metamaterial the model. With lighter core, the absorption peak shifted to higher fre
occurrence of local resonances can lead to effective density and elastic quency. It suggested that the converted transverse waves enhanced the
moduli which are frequency-dependent (i.e., zero or negative at certain multiple scattering and absorption, which damped rapidly in visco
frequencies). In this case, metamaterials can be used to control sub elastic polymer and dominated the acoustic absorption. To reveal this
wavelength sound waves, which is not possible for traditional materials. absorption mechanism, both finite element method (FEM) and locally
According to Bragg’s reflection, band gaps can only occur at a frequency resonant sonic model (LRSM) were used to investigate a viscoelastic
for which the wavelength is twice of the spacing between the scatterers polymer slab embedded with spherical scatters [156]. According to the
[147]. At low frequency, traditional materials need to be much thicker, relationship between the resonance modes with the displacement con
which is not practical. Liu et al. firstly proved the subwavelength band tours and the corresponding absorption spectra, it was concluded that
gaps in locally resonant phononic crystals [148]. Some acoustic meta localized resonance led to the absorption peak, and the mode conversion
materials have been developed for underwater acoustics applications from longitudinal to transverse waves at the second absorption peak was
[25,149]. A summary of partial studies on polymers with phononic found to be more efficient than that at the first one. Although these
crystals for underwater sound absorption is given in Table 13. metamaterials have shown better sound absorption performance in the
Wen et al. [155] carried out a systematic investigation on meta low frequency band, the effective frequency range was considered to be
materials. In his book, the development, basic theory, calculation rather narrow.
method of band gap, mechanisms, 2D and 3D phononic structures were To overcome this issue, a new type of multilayered locally resonant
all summarized. For underwater sound applications, they experimen acoustic metamaterials (M-LRAM) is proposed. It was found that
tally and theoretically studied acoustic absorption of various viscoelastic multilayered locally resonant scatterers have obvious superiority in
polymer slabs embedded with locally resonant scatterers (i.e., heavy underwater sound absorption over the conventional LRAMs [79,157].
spheres coated by soft silicon rubber). As shown in Fig. 9, the samples As shown in Fig. 10, one layer locally resonant acoustic metamaterials
had a diameter of 118 mm and a thickness of 55 mm. The diameter of the gave the lowest absorption coefficients. When the layer increased to two
spherical core was 10 mm, and the lattice was 19.5 mm. Compared with or three, the absorption peaks moved to high frequency, and the overall
pure polymer samples, there was an obvious absorption peak around 1 sound absorption performance also increased. In addition, a woodpile
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Y. Fu et al. Polymer Testing 96 (2021) 107115
Fig. 9. Underwater sound absorption performance: (a) Pure polymer samples; (b) polymer samples embedded with heavy spheres coated by soft silicon rubber (solid
lines-computational results from layer-multiple-scattering method, dashed lines-experiment results from the water-filled impedance tube) [150].
Fig. 10. The sectional view of a unit cell of underwater sound absorption structure: (a) conventional LRSMs, (b) LRSMs with two resonators, (c) LRSMs with three
resonators, (d) underwater acoustic absorption coefficient [157].
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Y. Fu et al. Polymer Testing 96 (2021) 107115
structure inspired metamaterial also showed a strong capability of 5.5. Underwater sound absorption mechanisms
absorbing sound in a wide frequency range [158]. Three kinds of ma
terials with different elastic modulus were selected to produce the With the addition of these different inclusions, more underwater
locally resonant phononic woodpile (LRPW). The composite materials sound absorption mechanisms are introduced, which are summarized
comprised steel rods with three different sizes, soft PU and hard PU. below.
Hard PU of characteristic impedance matching with water was chosen as
matrix material, while soft PU and steel rods with a volume ratio of 3:1 5.5.1. Resonance
were LRPW. An average absorption coefficient over 0.8 in a wide fre Embedded inclusions in polymer matrix have their own natural
quency range, from 8 kHz to 30 kHz, was achieved. To achieve broad frequency and will resonate with incident waves near their natural
band underwater sound absorption, a gradient cavity shaped PU frequency. It has been proven that the peak values of the sound ab
composite array supported by carbon fiber honeycomb was designed sorption coefficient appear at the resonance frequency [123]. As shown
[159]. Different types of PU composites were integrated to fabricate the in Fig. 11 (a) and (b), when an incident wave dynamically excites such a
sound-permeable layer, the gradient resonant cavity layer and the configuration, the region around the cavity exhibits a typical deforma
viscoelastic bottom layer. The tested underwater sound absorption co tion consisting of two components. One is the radial, in-and-out motion
efficient was 0.9 in the frequency range of 2400–10000 Hz under the of the cavity wall, while the other is the drum like up-and-down motion
hydraulic pressure of 1.5 MPa, basing on the combined effects of cavity [160]. Because sound absorption can only occur around the resonance
resonance and impedance transition. frequency, the working frequency range is usually very narrow. To
broaden the band of high sound absorption coefficient, mixed sizes and
multi-layers of inclusions are used. Several sound absorption peaks can
Fig. 11. Schematic of resonances: (a) resonance of in-and-out, (b) resonance of up-and-down. Local resonances: (c) displacement amplitude field of transmission
coefficient model, (d) radiation model [152].
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Y. Fu et al. Polymer Testing 96 (2021) 107115
contribute to a broad band. Another issue is that the resonance fre Fig. 12 shows sound attenuations of an example of 30% lead inclu
quency has a negative relationship with the size of the resonator. For low sion in epoxy. It is clear material with mode conversion has higher sound
frequency, the size will increase to an unrealistic size. Besides, the big attenuation than the sample without mode conversion. It is also found
resonator (usually air voids) is easily affected by high hydrostatic that mode conversion is stronger in the case of rigid inclusions in soft
pressure, so it is still difficult to overcome the “bottle-neck” in enhancing matrix materials [166]. Wen et al. [156] used finite element method to
the absorption at low frequency (i.e., in the range of several hundred verify this by modelling a unit cell with steel core coated by silicon
hertz) [156]. rubber. As shown in Fig. 13, it is obvious that longitudinal waves convert
To resolve these issues, the local resonance was introduced by Liu into shear waves on the interface. It is also noticed that shear waves
et al. as an effective way to control subwavelength sound waves at low dissipate rapidly in viscoelastic medium, which can also enhance the
frequencies [148]. Basically, this concept was first proposed in the field energy dissipation. Another benefit of the mode conversion is that only
of optics [161,162], and then adopted in the acoustic field. Currently, longitudinal waves can propagate into rubbers, while shear waves
most studies focus on sound absorption materials in air [144,163,164], cannot propagate back to water. The reason is that shear waves cannot
and not many studies are about underwater applications [165]. exist in water. Therefore, shear waves can only stay in the material
Different from traditional resonators, local resonators are inclusions dissipates in the form of heat.
with the soft coating layer and heavy core, which can lead to a band gap
at low frequency about two orders of magnitude lower than the value 5.5.3. Friction
predicted by Bragg’s theory [156]. In this case, the heavy core moves (as When surfaces in contact move relatively to each other, the friction
a whole) along the direction of the wave propagation, with large strain between the two surfaces converts kinetic energy into thermal energy (i.
at the heavy core-soft rubber coating layer interface. This low frequency e., it converts from work to heat). The friction can occur between matrix
resonance could be understood as an oscillation, in which the inner core material and inclusion surface or in the matrix material. For rubber
provides the heavy mass and the silicon rubber provides the soft spring. matrix with inclusions inside, the inclusions and the matrix have
Huang et al. [152] carried out numerical simulation to confirm this different displacements, which means there is friction on the interfaces.
phenomenon as shown in Fig. 11 (c) and (d). Another part contributing It has been found that carbon nanotube (CNT) and graphene can
to the sound absorption is the displacement of the heavy core [148]. significantly improve PDMS matrix’s sound absorption performance
However, most studies about local resonance are still limited in because of the friction between CNTs, graphene layers and interfaces as
analytical model or simulation, and the applications in real materials are shown in Fig. 14 (a). Rubbers themselves have hard section and soft
still challenging. Besides, the narrow bandwidth also needs to be tackled section in the molecular chain as shown in Fig. 14 (b). Being excited by
[79]. incident sound, they will vibrate in different extents. It is a kind of the
mass-spring system [167]. The hard section is the mass, while the soft
5.5.2. Mode conversion section is the spring. Some sound waves can be dissipated by the relative
Mode conversion generally refers to the concept of converting lon motions in the rubbers.
gitudinal waves to shear waves. Sound in water can only propagate as
longitudinal waves, but it can exist in forms of both longitudinal and
shear waves in solid materials. Therefore, there is mode conversion in 5.6. Applications
materials. For polymer materials, the longitudinal bulk modulus is one
or two orders of magnitude greater than the shear modulus, so the Sound waves can propagate in long distance underwater, which have
fraction of acoustic energy stored in the longitudinal strain is much positive or negative effects on environment, depending on sound level
higher than that of shear strain. In contrast, the loss factor of shear and frequency. For the negative effects, it is necessary to control these
modulus (tanδ ≈1) is much higher than that of the longitudinal bulk issues. Navy ships and submarines have machines and with propellers,
modulus (tanδ ≤ 0.1), so the fraction of acoustic energy lost by both which produce noise and vibration, emitting underwater sound waves
shear strain and longitudinal strain are small. To improve sound ab throughout the hull or directly. The sound emission is higher at low
sorption property, it is necessary to insert inclusions in polymers which frequencies (below 1000 Hz) and can propagate underwater at long
convert longitudinal waves to shear waves [10,141]. The inclusions distance, producing a sound field that can be detected by passive sonar.
include hollow glass microspheres, carbon materials, metal particles, In addition, another threat for underwater vehicles is active sonar,
etc. The size of the inclusion varies from centimeter to nanometer [166]. which can detect objects by radiating sound waves. Target strength
mainly depends on the size, shape and acoustic reflectivity of external
surfaces, as well as on the direction of incoming waves [25], but the
practical way is to change acoustic reflectivity of external surfaces.
Underwater sound absorption polymer-based materials can be applied
on the surface to absorb sound waves, so the acoustic target strength can
be reduced. Active sonar’s working frequency can be from 1 kHz to 30
kHz, and some advanced Sonar can work at 100 Hz or even lower fre
quency [7], which is highly challenging for underwater sound absorp
tion materials. For submarines, they can reach depths down to 600 m,
while most materials cannot resist high hydrostatic pressure. As sum
marized above, polymers with air voids have good performance at me
dium and high frequency, but their performance is not uniform at all
operating depths because of the deformation of air voids under varying
hydrostatic pressure. Polymers with solid inclusions have good perfor
mance at high frequency range, and some solid inclusions have been
proven to work well under high hydrostatic pressure. Polymers with
nanofillers have demonstrated good performance at low and medium
frequency, and the thickness is thinner than polymers with solid in
clusions. Polymers with phononic crystals have also shown good per
Fig. 12. The contribution of mode conversion to sound attenuation by spher formance at low and medium frequency, and they are very promising to
ical Pb inclusions in epoxy [166]. realize high sound absorption at low frequency with ultra-thin layers.
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Y. Fu et al. Polymer Testing 96 (2021) 107115
10
Fig. 13. Total displacement ( × 10− m) contours of a unit cell with steel core coated by silicon rubber [156].
Fig. 14. Schematics of friction: (a) The damping of sound waves by interfacial sliding and friction between CNTs, graphene layers and interfaces [63]; (b) Structure
of the polymer molecular structure [29].
Although underwater sound absorption materials have been studied One main challenge for the development of underwater sound ab
for many years, there are still challenges and opportunities remain for sorption materials is to achieve broad frequency range, especially at low
broader and reliable applications. More specifically, important problems frequency. Underwater acoustics cover a wide frequency range of in
to be solved in this field include sound absorption at low frequency, terest. For example, ships or underwater platform generally involves
broad band, light weight, high pressure, multifunctionality for various systems operating with frequencies from a few kHz up to several hun
applications. dreds of kHz, whereas long-range detection Sonar systems use lower
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Y. Fu et al. Polymer Testing 96 (2021) 107115
frequencies to a few hundred Hz [57]. While different sound absorption 6.4. Multifunctionality
materials or mechanisms can only be effective in specific frequency
range. As summarized, most polymers with single size air voids have In many aspects, there is a driving force for materials shifting to
good performance around 8 kHz–18 kHz [7]. By mixing air cavities with wards multifunction. For underwater sound absorption materials, there
different size, significant absorption reduction from 1 kHz to 25 kHz can are also requirements about antifouling and drag reduction. Biofouling
be achieved [121]. However, it is challenging to further improve the remains a severe environmental problem and causes huge economic loss
frequency range, especially below 1000 Hz. Metamaterials have ad in the shipping industry [173]. For underwater sound absorption ma
vantages at low frequency, but the critical issue is the relatively narrow terials, the biofouling can totally cover the surface, which can signifi
band gaps, which limits the application of locally resonant acoustic cantly decrease the sound absorption performance [7]. The surface
metamaterials [168]. To overcome this drawback, multilayered locally roughness has a negative relationship with drag. If underwater sound
resonant acoustic metamaterials have been proposed. Results indicated absorption materials are not smooth, which can result in the increase of
coupled resonance can broaden band gaps and engender multiple band drag, so drag reduction should also be considered for underwater sound
gaps [79]. This could be an inspiration for other types of underwater absorption materials. It is difficult to resolve these issues using tradi
sound absorption materials. tional polymer-based underwater sound absorption materials. It is found
that nanofillers can not only introduce sound absorption properties, but
also make multifunction possible. For example, carbon nanotubes can
6.2. High pressure resistance enhance sound absorption, and improve antifouling and drag reduction
[174,175]. Therefore, nanofillers or other new types of inclusions
Most polymer-based materials still suffer under high hydrostatic require special attention when performing the design of underwater
pressure. With the increase of hydrostatic pressure, their underwater sound absorption materials.
sound absorption performance decreases or is completely suppressed in
some cases [169]. The reasons include the deformation of both matrix 7. Conclusion
material and inclusions, change of mechanical property under high
compression. Zhu et al. [7] found the sound absorption shifted to high In this review, we have examined different polymer-based materials
frequency with the increase of hydrostatic pressure because of the for underwater sound absorption regarding key factors of underwater
deformation of air voids. Wang [29] used the free volume theory to sound absorption, measurements, mechanisms, applications. Based on
explain. The movement of free volume was related to the chain structure polymers themselves, underwater sound absorption can be realized.
of polymer. Under high pressure, the chain structure was compressed, so These materials include IPN, polymer foams, and gradient polymers. To
the suppressed free volume weakened sound absorption capability. further improve the performance, different types of inclusions are
Different methods have been applied to improve the performance introduced to polymer matrix materials, including polymers with air
under high pressure. Some studies focus on improving the matrix ma voids, solid inclusions, nanofillers, and phononic crystals. The current
terials’ compression resistance capacity [29]. In this scenario, the harder challenges are low and broad frequency range, high pressure resistance,
matrix material’s impedance should remain close to water, so the un thin thickness, and multifunctionality. Although there are some chal
derwater sound absorption capability can be maintained, which could lenges remaining, a rapid development will be expected in future
be challenging for some matrix materials. Other method utilizes solid studies. Further promising research resolve those challenges may
inclusions which do not collapse and are able to contain their sound include the incorporation of two or more types of inclusions and
absorption function under high pressure [128,134,135]. Therefore, to structures.
choose a suitable hard inclusion for a specific application is still chal
lenging. Surface structures which can trap sound waves can also be. A Credit author statement
wedge-shaped sound-absorbing structure shows good performance
under high hydrostatic pressure [170,171]. However, the surface Yifeng Fu: Conceptualization, Methodology, Investigation, Writing
structures usually take a large space, which are not suitable for moving – original draft. Imrana I Kabir: Methodology, Writing – review &
objects. More effort should be directed to develop sound absorption editing. Guan Heng Yeoh: Supervision, Writing – review & editing.
materials with high pressure resistance. Zhongxiao Peng: Supervision, Writing – review & editing.
17
Y. Fu et al. Polymer Testing 96 (2021) 107115
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