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Polymer Testing 96 (2021) 107115

Contents lists available at ScienceDirect

Polymer Testing
journal homepage: http://www.elsevier.com/locate/polytest

A review on polymer-based materials for underwater sound absorption


Yifeng Fu a, *, Imrana I. Kabir a, Guan Heng Yeoh a, b, Zhongxiao Peng a
a
School of Mechanical and Manufacturing Engineering, University of New South Wales, Sydney, NSW2052, Australia
b
Australian Nuclear Science and Technology Organisation (ANSTO), Locked Bag 2001, Kirrawee DC, NSW, 2232, Australia

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

In some cases, underwater sound absorption materials will be

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)

1 air 1.23 340 418 [7]


2 Water 1053 1490 1.56 × 106 [28]
3 Cork 0.24 530 1.27 × 105 [29]
4 Aluminum 2690 6420 1.73 × 107 [30]
5 Steel 7860 5950 4.64 × 107 [30]
6 PDMS 969 1119 1.08 × 106 [28]
7 PU 1528 1040 1.59 × 106 [31]
8 Epoxy 1180 2490 2.95 × 106 [32]
9 Hydrogel 1000 1600 1.60 × 106 [33]
10 Ecoflex 1070 989 1.06 × 106 [34]
Fig. 1. Schematic of sound propagation.

2
Y. Fu et al. Polymer Testing 96 (2021) 107115

Table 2 3.1.1. Water-filled impedance tube


Loss factor of polymer materials in comparison to some common materials. Water-filled impedance tubes are widely used to measure the un­
No. Materials Loss factor Ref. derwater acoustic properties of materials. One-dimensional plane waves
travelling in normal direction are propagated towards the test speci­
1 Glass ≈0.002 [7]
2 Wood ≈0.13 [7] mens. Although this method does not represent a real three-dimensional
3 Aluminum 0.3 ~ 10 × 10− 5 [36] sound field, it is cost-effective, and pressure and temperature in the tube
4 Steel 0.2 ~ 3 × 10− 4 [36] can be easily controlled to simulate different underwater environment.
5 Copper 2 ~ 7 × 10− 4 [36] Depending on different setups, there are three standardized methods
6 Acrylic [37]
including standing wave ratio method [42], transfer function method
≈0.1
7 PDMS ≈0.15 [38]
8 Epoxy ≈0.039 [39] [43,44] and active cancellation approaches [45].
9 Neoprene rubber ≈1.12 [37] The standing wave ratio method (the pulse tube) is the oldest and
10 Nanocomposite ≈0.5 ~ 0.9 [37] simplest method [46,47]. In the setup, a loudspeaker placed at one end
of the tube generates the incident plane sinusoidal sound wave. The
other end of the tube is terminated with the test sample backed with a
applied in different water depth, so the compressive strength will
hard reflective end [48]. During testing, there is a standing wave in the
determine the underwater sound absorption performance under
tube, so there are only plane incident and reflected waves propagating
different hydrostatic pressures. High compressive strength can guar­
along the tube axis in the test section of the tube. By measuring the
antee stable underwater sound absorption performance at different hy­
pressure maximum and minimum, the standing wave ratio can be
drostatic pressures due to variable water depths. These commonly used
calculated, which deduces the sound absorption coefficient. B&K (Nor­
polymer materials and their Young’s modulus are given in Table 3. It can
cross, GA, USA) designs a commercial apparatus (Standing Wave
be seen that the modulus can vary in a large range from 0.125 MPa to
Apparatus Type 4002) for air tests, which is used for specific acoustic
1300 MPa. For application under high hydrostatic pressure, the polymer
impedance of circular cut samples of sound absorbing materials in the
matrix materials should consider high Young’s modulus (>1000 MPa).
frequency range from 90 Hz to 6500 Hz. In order to measure in a rela­
To further improve the compressive strength, hard frame structure can
tively wide frequency range, the Standing Wave Apparatus is supplied
be embedded into the polymer matrix material [14].
with two measuring tubes with different diameters (ϕ). The large one ϕ
= 100 mm is for low frequency from 90 Hz to 1800 Hz, and the smaller
3. Testing of polymer-based underwater sound absorption
one ϕ = 30 mm is used for high frequency from 800 Hz to 6500 Hz.
materials
When the data overlap, the results of the large tube are adopted because
of being more accurate. Naval Undersea Warfare Center of Beijing [49,
To evaluate polymer-based underwater sound absorption materials,
50] and the Pennsylvania State University [10,51] adopted this method
corresponding testing instruments can be applied. Acoustic impedance
for underwater tests. For the standing wave ratio method, only one given
and sound absorption coefficient are obtained by underwater acoustic
frequency can be tested at one time, which is not entirely efficient.
test. Dynamic modulus, which has significant effect on sound absorp­
Different from the standing wave ratio method, the transfer function
tion, can be measured by dynamic mechanical test. Compressive test is
method can test a broad frequency at one time [52], so it is more effi­
important to measure whether a polymer material can maintain its
cient. Instead of measuring the pressure maximum and minimum, sound
sound absorption property under high hydrostatic pressure conditions.
pressures at any positions are measured, and then transfer function can
More details are given below.
be calculated. According to the number of hydrophones, the transfer
function method can be divided into different measurement ways. The
3.1. Underwater acoustic test
typical transfer function method uses two hydrophones. The setup of the
impedance tube is almost the same with the standing wave ratio method.
Based on different requirements and purposes, there are corre­
In contrast, the speaker generates broadband, stationary random sound
sponding underwater acoustic testing methods to obtain underwater
waves which propagate as plane waves and reflect after hitting the
sound absorption properties [40]. Full sea trial is the ideal testing
sample [53]. Ayub et al. [54] have provided details about the setup,
method for practical applications. It can use sonar system to analyze
repeatability and reproducibility tests, and error analysis about the
large scale samples. However, this method is often prohibitively
transfer function method. Wilson et al. [55] from Boston University also
expensive, so it is best used for final stage testing of a complete system.
reported a transfer function water-filled impedance tube with improved
For lab tests, the most widely used acoustic testing facilities are water
measurement accuracy and precision. The tube was below 50 cm in
filled impedance tube and acoustic tank. Both methods can carry out
length and 5.178 cm in diameter. The working frequency range was
multitude of tests for small samples, allowing possible changes in design
from 5000 Hz to 9000 Hz. However, the accuracy of the transfer func­
and selection of materials. It is worth noting that the use of water for
tion method has been found to be as accurate as the standing wave ratio
these lab tests should be softened to prevent lime precipitation, and it is
method.
required to be frequently degassed to avoid trapped air bubbles which
Active cancellation method is seldom used. The standing wave ratio
are known to absorb sound [41].
method and transfer function method have to involve backing the
sample with other material (hard backing and soft backing), avoiding
the influence of unwanted reflections from the tube end especially for
high hydrostatic pressure. However, the absorption coefficient
Table 3 measured in this manner is characteristic not only for the sample, but
Compressive strength of widely used polymer materials. also of the backing material. This will become worse when frequency is
lower. Active cancellation method is proposed to solve this problem
No. Materials Young’s modulus Ref.
(MPa) [56]. In this method, the setup is different from the above two methods.
In one study [45], the sample was placed near the tube’s center. Two
1 Ecoflex 0.125 [34]
2 Hydrogel (90% water and 10% Poly (vinyl 0.3 [33]
ends of the tube were fitted with projector arrays consisting of 14
alcohol)) pressure-compensated transducers. There were six hydrophones moun­
3 PDMS 1.3 [28] ted along the upper interior length of the tube. It can acquire the mea­
4 PU 3.59 [31] surements over the full range of ocean environmental conditions in the
5 Epoxy 1300 [32]
frequency range of 100 Hz–1750 Hz.

3
Y. Fu et al. Polymer Testing 96 (2021) 107115

3.1.2. Acoustic water tank Table 5


Analogous to the reverberation room for airborne acoustic tests, a Review on DMA tests for different samples.
water tank for similar underwater measurements is commonly adopted Facility Frequency Temperature range Heating rate Ref.
[57]. The acoustic water tank can simulate a three-dimensional sound (Hz) (◦ C) (◦ C/min)
field, which is akin to a real sound environment compared with the DMA Q800 1 0 to 100 3 [66]
one-dimensional sound field in the water-filled impedance tube. DMA Metravib 10 − 30 to 60 3 [67]
Generally, there are two kinds of water tanks. The first type is for a DMA Q800 0.3 to 20 − 40 to 40 – [68]
narrow frequency range under normal pressure. This kind of water tank DMA Q800 1 − 30 to 100 3 [69]
DMA Q800 1 − 100 to 100 3 [70]
is cost-effective, so has been widely adopted to test small panel in lab­ DMA Eerkin- – − 100 to 100 3 [71]
oratory. Leroy et al. [58,59] constructed a tank (60 × 60 × 120 cm3) to Elmer
investigate the sound absorption of air bubbles from 30 kHz to 400 kHz.
Feng et al. [60] built a water tank (180 × 80 × 80 cm3) to study an
underwater acoustic absorption metasurface from 50 kHz to 250 kHz. 800.
A more complex water tank is the ability to modify the hydrostatic
pressure and the temperature conditions while testing. To avoid the 3.3. Compressive test
reflected sound disturbing the sound field, anechoic tiles are applied on
the wall of the tank. For example, Alex [61] has used this kind of water Some applications are under high hydrostatic pressure, so it is
tank to test anechoic rubber coatings applied to water-immersed steel necessary to test the compression performance. The latest combat sub­
plates introducing both variable water temperature from 8 to 20 ◦ C and marines are built to reach depths as great as 600 m (translating into
ambient pressure from 0 to 20 bar. Victor et al. [62] used a parametric hydrostatic pressure of 6 MPa) [72]. Corresponding, the quasi-static
array in this kind of water tank capable of simulating ocean depths down compression tests should be conducted in the pressure range 0–6 MPa,
to 700 m and water temperatures from 2 to 35 ◦ C. Compared with real using mechanical testing apparatus [14]. During the compression test,
ocean trials, a water tank can simulate water or ocean environment. the compression of the thickness and volume with the pressure can be
However, the water tank test may suffer from problems that arise due to obtained. The decrease of thickness may contribute to the reduction of
the finite size of the panel under test. In particular, diffraction of the underwater sound absorption performance. In addition, the compressed
acoustic field from the edges of the panel leads to signals that arrive at volume will suppress the polymer molecular structure, which can
the hydrophones at times only marginally different from those of the further weaken the damping property. The recoverability of the
reflected and transmitted signals [62]. When test frequency is lowered, polymer-based materials can also be evaluated by compressive tests.
panel size must be increased to avoid the disturbing influence of waves Table 6 summarizes some compressive tests.
originating at the panel edges. As a summary, the comparison of
different underwater acoustic testing methods is given in Table 4. 4. Commonly used polymers for underwater sound absorption
Different methods are made comparison, and advantages and disad­
vantages are highlighted for each method [24,44,47,63]. The choice of a Polymer materials have, in general, densities that are close to water,
suitable method to be adopted depends on the requirements for the and are easy to design and modify for their specific underwater acoustic
specimens to be tested (i.e., different frequency range and accuracy). functions [75]. Some polymers are naturally damping, so they can be
suitable candidates for underwater sound absorption materials. Polymer
3.2. Dynamic mechanical test materials for underwater sound absorption are listed in Table 7. The
most widely used polymers are rubber including butyl rubber, nitrile
Dynamic mechanical test (or dynamic mechanical analysis, DMA) is nutadiene rubber, silicon rubber (e.g., PDMS) [76,77]. Polyurethane
the technique of applying a stress or strain to one sample at controlled (PU) elastomer is also adopted because of higher damping property and
frequencies and analyzing the response to obtain phase angle and mechanical strength [68,78]. Some foams are used in some underwater
deformation data [64]. Based on this data, loss factor and complex situations. Other polymers are hydrogel and epoxy [79,80].
modulus can be calculated. Besides, DMA of polymer-based materials
can be tested in a large temperature range, so glass transition temper­ 4.1. Interpenetrating polymer networks (IPN)
ature (Tg) can be obtained. At that temperature, thermosetting polymers
change from a “glassy” state (e.g., rigid or hard) to a “rubbery” state (e. Most homogeneous polymers have limited performance for under­
g., damping or pliable) [65]. For underwater sound absorption appli­ water sound absorption because of matched impedance but low loss
cations, it is desirable to make Tg close to the working temperature factor. For example, tanδ of PDMS is below 0.225 [86], tanδ of epoxy is
range, so high damping properties can be fully utilized. Table 5 sum­ about 0.38 [87] and tanδ of PU is slightly higher up to about 0.5 [88]. To
marizes different DMA tests. The most widely used facility is DMA Q further improve the sound absorption property, a new synthetically
macromolecule composed two or more polymers with a physical circle
Table 4 connected by a cross network, namely interpenetrating polymer net­
Comparison of different underwater acoustic testing methods. works (IPN), is introduced. A summary of studies about IPN for under­
Facility (sound Method Advantage Disadvantage water sound absorption is given in Table 8. As shown in Fig. 2, IPN of
field)

Impedance tube Standing High accuracy Time-consuming Table 6


(one- wave ratio High efficiency Low accuracy Review on DMA tests for different samples.
dimensional Transfer Avoiding interference Complicated
Facility Sample size Pressure range Ref.
sound filed) function from backing material
(MPa)
Active
cancellation WDW-100 universal testing Diameter 56.5 mm and 0–10 [29]
Acoustic tank Simple setup Cost-effective Limited testing machine thickness 50
(three- Complex Simulating real ocean conditions, CMT4305 mechanical Diameter 35 mm and 0–6 [14]
dimensional setup environment (variable interference from testing apparatus thickness 20
sound filed) temperature, water the reflected sound Universal testing machine – 0–6 [73]
depth), no reflected Complicated, large Instron universal testing 152 mm × 100 mm × 50 0.3 [74]
sound interference space, high cost machine mm

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]

4.2. Polymer foams


Table 8
A summary of studies on the damping rubbers for underwater sound absorption.
Foams are the most widely used sound absorption materials in air
No. Materials Sample size Frequency Sound Ref. because of the low density and a high ratio of acoustic energy dissipation
range absorption
to treatment weight [91–93]. However, when it comes to the under­
coefficient
water sound absorption, foams usually have poor performance. It is
1 Polypropylene glycol 2–25 kHz 0.7 [70]

difficult for the sound to enter the porous material from water because of
as soft segment,
toluene diisocyanate the impedance mismatch between of the porous material and water.
and triethanolamine While metal materials have much higher acoustic impedance, so metal
as hard segments forms can have close impedance with water. Aluminum foam is the most
2 PU, epoxy, 57 mm 2–12 kHz 0.6–0.8 [89] popular metal foam for underwater sound absorption, but the thin
unsaturated diameter
aluminum foam cannot absorb sound, and the corrosion and poor sound
polyester resin (UPR) and 50 mm
and PDMS thickness absorption performance at low frequency are also a problem. To over­
3 PU and PDMS 49.5 mm 2–15 kHz 0.68–0.84 [90] come these issues, compliant PU and stiff PU were filled into the pores of
diameter aluminum foam [14]. Result showed that this structure had high un­
and 25 mm
derwater sound absorption coefficients over 0.9 in 12–30 kHz. More­
thickness
4 Epoxyurethane and 56.2 mm 2–12 kHz 0.75 [82] over, the quasi-static compressive test indicated that it has a
epoxy diameter compressive strength over 5 MPa which is crucial for deep water
and 40 mm applications.
thickness Recently, Xu et al. [83,84] studied porous SiC foam with or without
silicon oil or water filling using finite element method (FEM) and
eopxyurethane (EPU) and EP was fabricated and investigated. It was experimental tests in a water-filled impedance tube. The air-saturated
found that both ratio of EPU/EP and molecular weight have effect on the SiC foam exhibited great potential underwater sound absorption prop­
underwater sound absorption performance. By adapting the combina­ erties over a broad frequency regime, especially over 1000 Hz as shown
tion, high sound absorption coefficient above 0.9 can be achieved in a in Fig. 3 (a) and (f). The behavior can be attributed to the high flow
broad frequency range. Luo et al. [89] also used PU, epoxy, polyester resistance resulting from the complex channel structure combined with
resin and PDMS blend to make IPN. The sound absorption coefficient unique fine morphology of porous skeletons formed by micro-sized
around 0.8 can be achieved from 2 kHz to 12 kHz. Jayakumari et al. [90] sub-channels as shown in Fig. 3 (b)–(d). In a further study, the SiC
also found only PU and PDMS blend can have good underwater sound foam was partially or fully saturated by water. The partially saturated
absorption performance for both modelling and testing in a water-filled SiC foam still demonstrated enhanced sound absorbency at low fre­
pulse tube. Some researchers studied the effect of different hard segment quency. However, the sound absorbency was lost for fully saturated SiC
contents on underwater acoustic properties of PU [70]. The hard and due to the low magnitude of kinematic viscosity of water which led to
soft segments are analogical to the mass-spring system. By modifying the weak drag force exerted by the foam skeleton surfaces. If the foam was
hard segment contents, the underwater acoustic properties can be filled with silicon oil, a high magnitude of absorption coefficient across
improved significantly. the frequency band could be achieved because of the high kinematic
viscosity of silicon oil. The use of foams remains challenging for

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.

6
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

kHz [109], and the water depth range is limited. Table 10


In anechoic water tanks, the quiet underwater environment is also A summary of studies on polymers with air voids for underwater sound
important. During acoustic tests, the reflected sound will disturb the absorption.
sound field, which can significantly affect the testing results. To avoid No. Air voids Sample Frequency Sound Ref.
the reflected sound waves, underwater sound absorption polymers can size range absorption
be applied on the wall of the tank to absorb the emitted sound. Espe­ coefficient

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].

5.1. Polymers with air voids bandwidth of the absorption.


Recently, some improvements have been achieved by studying the
For polymer foams, the pores are difficult to control, and the effi­ attenuation performance of both random and periodic air bubbles
ciency is not high. Then polymer matrix embedded periodic air cavities immersed in a soft elastic polymer matrix [58]. And the size of air
is proposed, which is also called Alberich anechoic material. It is the first bubbles is in micrometer, and the absorbed sound is in MHz (i.e., ul­
practical underwater sound absorption material for navy, named after trasound). Ultrasonic measurements were carried out in a large water
Alberich, a king famous for his magical cloak of invisibility in Germanic tank. Sub-wavelength sound absorption and even some broadband
mythology [116]. German Navy used this name to show their high super-absorption can be achieved. For example, a bubbly soft elastic
expectation of stealthy submarines to counter the British ASDIC (active material, PDMS with two-dimensional periodic air bubbles (diameter
sonar). This anechoic coating can mute sonar reflection up to 15% at the 78 μm, height 50 μm) showed high absorption around 0.8 MHz [77].
frequency range from 10 kHz to 18 kHz. Currently, Alberich anechoic With the steel backing, it was further found that even 4 mm thin film
material is still the standard anechoic device for modern underwater with periodic arrangement of 14 μm bubbles can obtain 35 dB reduction
vessels [117]. over the 8–22 kHz frequency range [108]. However, there are still two
A summary of studies on polymers with air voids is listed in Table 10. challenges for polymers with air voids. Firstly, the active sonar system
Hladky-Hennion et al. [118] applied a finite element approach for becomes much better in low frequency, which means the sample must
modelling the acoustical behavior of doubly periodic structures, and the increase in thickness. For example, the thickness will increase to 1 m for
result has good agreement with measurements. As shown in Fig. 5 (a), several Hz to hundred Hz, which is not practical to apply on ship hulls.
one layer of air cavities with the same size is difficult to achieve the The second challenge is that the submarine can go down to deep water
broadband absorption. Ivansson [119] numerically designed Alberich because of increasing significant drag. Therefore, polymers with air
anechoic material using the layer-multiple-scattering (LMS) method and voids cannot perform stably at all diving depths because of the defor­
differential evolution algorithms. It was proven that the broadband mation of embedded air cavities under different hydrostatic pressure.
performance can be improved by mixing air cavities of different sizes
and using rubbers with compressional and shear wave absorptions as 5.2. Polymers with solid inclusions
shown in Fig. 5 (b). Further, air cavities in different shapes were also
investigated [120]. It was found that horn holes have the best sound Different from polymers with air voids, some underwater sound
absorption performance at relatively low frequencies as shown in Fig. 5 absorption materials replace the air voids by solid inclusions, which
(c). The backing material also has a significant effect on Alberich have the ability to absorb sound waves of different frequency range and
anechoic materials’ performance. Alberich anechoic materials are usu­ simultaneously enhance their compressive strength [75]. One disad­
ally immersed in water with steel backing, so Zhao et al. [121] studied vantage of air voids is that they will deform under pressure, but air voids
the optimization and mechanisms of Alberich anechoic materials on encapsulated in hollow glass spheres (HGS) can overcome this issue. The
steel plate. It has been validated that laying different coatings on both spherical shells are made from glass and therefore acoustically trans­
surfaces of the steel plate can effectively enhance the low frequency and parent. The stiffness and spherical shape of the inclusions make the

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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].

potential anechoic-coating material. Compared to carbon black, carbon


Table 11
fiber shows better capability to improve underwater sound absorption
A summary of studies on the polymers embedded solid inclusions for underwater
property. Mental powders are considered as penitential fillers for un­
sound absorption.
derwater sound absorption materials. Sphere fillers TiO2, ZrO2, Al2O3
with diameter from 1.1 μm to 3000 μm were investigated [29]. It was No. Solid inclusions Sample size Frequency Sound Ref.
range absorption
found that fillers with smaller sizes usually have better underwater coefficient
sound absorption performance. A summary of studies of using different
1 Hollow glass 10 mm 20–100 0.68–0.9 [135]
solid inclusions is given in Table 11.
microspheres thickness kHz
(HGM) with
diameter 50 μm
5.3. Polymers with nanofillers 2 HGM with 20 mm 1 kHz-1 – [134]
diameter 30–120 diameter MHz
With the development of nanotechnology, nanofillers are used to μm and 80 mm
improve polymers’ properties due to their small scale and complex in­ thickness
3 Carbon fiber 64 mm 7–12 kHz 0.9 [10]
teractions of nanomaterials with polymers [136]. It has been proven that (diameter 7.2 μm, diameter
some carbon nanofillers can significantly improve the sound absorption length 6.35 mm) and 65 mm
properties of polymers. Verdejo et al. showed that by adding only 0.1 wt thickness
% [137] multiwalled carbon nanotubes (MWCNTs) into PU foams, the 4 Carbon fiber with 49.5 mm 500 Hz-15 ~ 0.9 [68]
a
diameter 7.2 diameter kHz
sound absorption coefficient can be dramatically improved. The intro­
μm and length 3–4 and 20 mm
duction of MWCNTs can change not only the inside structure of the mm thickness
foams, but also the material properties (i.e., dynamic mechanical 5 Sphere fillers TiO2, 56.5 mm 3–30 kHz 0.7 [29]
property). The authors did not attribute the sound absorption ZrO2, Al2O3 with diameter
improvement to increase in cell size, but to energy dissipation on the diameter from 1.1 and 50 mm
μm to 3000 μm thickness
large surface area at the polymer-CNT interface. However, they did not 6 Macro and micro – – – [57]
provide any evidence to support the statement. Bandarian et al. [138] inclusions
studied MWCNTs with different functionalized groups. MWCNTs with a
Having good underwater sound absorption performance under high hydro­
carboxyl group have the highest sound absorption coefficient. This al­
static pressure.
lows the carboxyl-modified nanotubes to be uniformly dispersed as well
as having stronger interfacial interaction with the polymer matrix.
However, the mechanism of the sound absorption of CNTs remains

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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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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

Fig. 8. Trend of the development of acoustic materials.

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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].

13
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.

15
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].

6. Challenges and outlook 6.1. Low and broad frequency range

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

16
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.

Declaration of competing interest


6.3. Thin thickness
There is no any kind of conflict of interest.
Perfect absorption can be easily realized if the material is thick
enough for all the energy to be dissipated. However, in practice, the Acknowledgements
underwater sound absorption materials are wanted to be as thin and
light as possible. Thin thickness is not only more cost-effective, but also The PhD scholarship is funded by the China Scholarship Council
decrease the sailing resistance in water. Minimizing the thickness of (Grant No. 201606950016).
underwater sound absorption materials and, ideally, reaching a sub­
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