CHAPTER

Formulations and
properties: comparative
review of aromatic
polyurea vs aliphatic
1
polyurea
Khanisya Palaniandy1, Sheik Ambarine Banon Auckloo1, Eng-Seng Chan2,
Pooria Pasbakhsh3
1
Mechanical Engineering Discipline, School of Engineering, Monash University Malaysia, Subang
Jaya, Selangor, Malaysia; 2Chemical Engineering Discipline, School of Engineering, Monash
University Malaysia, Subang Jaya, Selangor, Malaysia; 3Advance Engineering Platform,
Mechanical Engineering Discipline, School of Engineering, Monash University Malaysia,
Subang Jaya, Selangor, Malaysia

1.1 Introduction
Polyurea is a polymer consisting of urea linkages ðNH2 Þ2CO. It is derived from a
step-growth (addition) polymerization of diisocyanate (NCO) polymer and amine
(NH2) resin blend. It exhibits elastomeric properties as it consists of polymer chains
that are connected to a network structure (crosslinking segments) and have a high
level of flexibility [1e4]. Polyurea is a chemically crosslinked random copolymer
that has a phase-separated microstructure consisting of both hard segments (HS)
and soft segments (SS) due to thermodynamic incompatibility [5,6].
Polyureas consist of a mixture of crystalline and amorphous domains, hard and
soft domains, respectively, which govern the mechanical properties. Usually, the
hard segments orient themselves to connect to each other via hydrogen bonding.
This could be achieved via monodentate hydrogen bonding (disordered) or bidentate
hydrogen bonding (ordered) depending on various factors such as index, gel time,
and fabrication method. Ordered and disordered bonds are particularly for the amine
and carbonyl regions of urea groups. These bonds can be detected from Fourier-
transform infrared spectroscopy (FTIR) peaks at around 1722/cm (disordered
hydrogen-bonded carbonyl group), 1711/cm (ordered hydrogen-bonded carbonyl
group), 3340/cm (hydrogen bonded NeH group) [7]. These bonded hard segments
form hard domains which act as bridges and as filler particles that reinforce the soft
segment matrix.
There are two types of polyurea; aromatic and aliphatic depending on the type of
the diisocyanate structure. By changing the type or structure of the diisocyanate, a

Polyurea. https://doi.org/10.1016/B978-0-323-99450-7.00011-3 3
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4 CHAPTER 1 Formulations and properties

wide variety of elastomers with different physical properties, productivity, and per-
formance of polyurea coating can be achieved [8]. Aromatic polyurea is derived
from aromatic diisocyanates containing aromatic rings which provide maximum
chemical stability and low reactivity. Aliphatic polyurea, on the other hand, was first
introduced in the 90s as there were challenges in the polyurethane coating industry
to offer a highly flexible, UV-stable coating system especially to meet the paint and
powder coatings industry [9,10]. Combination of aromatic and aliphatic co-
polyureas can be referred semi-aromatic or semi-aliphatic depending on the ratio
of the diisocyanate structures in the formulation. Apart from these two commonly
known polyurea, hybrid systems are another upcoming polymer technology devel-
oped by combining polyurea and other polymer(s) by physical or chemical means
to add to the properties and functionalities.

1.2 Aromatic polyurea

Aromatic polyurea became popular quickly since its introduction in the 80s in the
paint and coating industry. A commonly used aromatic prepolymer is diphenylme-
thane diisocyanate (MDI) [11]. Polyurea is employed in exterior applications that
are exposed to extreme environmental conditions, abrasion, and corrosion [12].
Environmental conditions such as ultraviolet (UV) radiation exposure could be
detrimental to the mechanical properties of materials gradually over some time.
Recent studies done on aromatic polyurea [12e16] as summarized in Table 1.1
have shown that UV radiation not only reduces the overall color stability, it reduces
yield strength, incurring crazing and microscopic cracks too. Polyurea macromole-
cules contain chromophores in the form of carbonyl groups that interact with oxygen
resulting in free radicals and this, in turn, causes surface embrittlement [12,13].
These effects suggest that where significant exposure to UV is expected, aliphatic
polyurea may be used as a top coat to protect the underlying aromatic coating or pig-
ments and UV absorbers can be added to reduce the UV effects. Hence, an aromatic-
based polyurea system is limited to be used in water or wastewater systems where
UV treatments are standard, concrete coating technology as well as in high pigment
loading content environments [17].

1.3 Aliphatic polyurea

Polyaspartic esters were used as coreactant of aliphatic isocyanates to curb the chal-
lenges faced in coating technology in 1990 [18]. Polyaspartic ester provides an addi-
tional layer of protection against the destructive effects of saltwater and prevents
discoloration of the polyurea intermediate coat, which is sensitive to UV light
[18]. The reactivity of polyaspartic esters depends on the carbon chain length and
structure of the component. Cyclic components take a longer time to react with
the isocyanate group fully. Johnston’s work [19] discovered that by optimizing
the percentage of polyaspartic ester in polyurea formulations, the properties of the
 1.4 Aromatic polyurea versus aliphatic polyurea 5

Table 1.1 Past studies on Isonate 143 L/P1000 polyurea as an aromatic

polyurea using 1:4 stoichiometry to investigate the effect of UV radiation on the
properties of polyurea.
Exposure Property
References time investigated Results

Brinson [15] 15 weeks Elastic Elastic modulus increased by 23.9%

modulus (11.7e90.2 MPa).
Whitten 15 weeks Acoustic Resistance to small strains decreased.
et al. [16] Shear attenuation decreased slightly at
the end of the exposure duration.
Youssef 18 weeks Dynamic Creep strain increased to 23% at 1000s
et al. [13] loading time; with higher deformation
resistance, the material became stiffer.
Creep strain increased up to 36% at high
temperatures, and the coloration of the
material significantly changed from
yellow to opaque tan.
Youssef 15 weeks Hyperelastic Remain unchanged.
et al. [12] behavior
Shaik [14] 15 weeks Segmental The surface of polyurea changed from
evolution having microvoids to crazing
microstructure.

resulting polyurea can be adjusted such that too high NCO content of the polyas-
partic ester may cause the polyurea to be brittle.
House et al. [20] investigated the effect of UV light on a series of aliphatic for-
mulations which resulted in cracks after exposure to a Xenon-lamp-based weather-
ometer for 200 h. This experiment proved that color stability in polyurea coating
does not necessarily guarantee excellent mechanical properties, although this argu-
ment is varied depending on the environment of the end product. Youssef et al. [12]
mentioned that the oxygen concentration in surroundings and ambient temperature,
pressure, and the existence of prestress all affect the growth of the UV-degraded sur-
face layer.

1.4 Aromatic polyurea versus aliphatic polyurea

Polyurea consists of a network structure that is “set” or hardened by thermally
induced crosslinking reactions, which makes it a thermoset elastomer. Most polyur-
eas are thermosetting elastomers that do not melt when heated below 200 C due to
their strong covalent cross-links. However, thermoplastic polyurea is also available
through physical crosslinking or by including susceptible chain extenders that
induce physical crosslinking during polymerization. Boenig et al. [21] showed
6 CHAPTER 1 Formulations and properties

that aliphatic polyurea is exceptionally meltable at a temperature ranging from 210

to 300 C, depending on the reactive isocyanate component. Taking this nature of
aliphatic polyurea into account, Kang et al. [22] synthesized melt-processible
aliphatic polyurea and successfully retained the original tensile strength (TS) and
elongation at break (εB ) by introducing hydrogen accepting chain extenders
(HACEs) to reduce the flow temperature. Fig. 1.1 shows the color change observed
at a higher temperature on aromatic polyurea (Isonate 143L: Versalink P650 of 1:4
mixing ratio) and aliphatic polyurea samples investigated for the present review
article. The aliphatic polyurea sample was prepared according to the PU PURE
formulation from our previous work [23]. While both aromatic and aliphatic poly-
urea began to show changes in color at 150 C, aromatic polyurea resulted in cracks
on the surface. The creation of cracks could be accelerated due to the presence of
internal voids that were produced during the sample preparation. Aliphatic polyurea
started to melt at 250 C releasing a toxic smell and resulting in cracks on its surface.
Both aromatic and aliphatic polyurea are greatly useful for diverse engineering
applications. Table 1.2 summarizes the comparison between the aromatic polyurea
and aliphatic polyurea. It shows that aromatic polyurea is generally stronger and
aliphatic polyurea is more stable and crack-free on exposure to light. Aliphatic poly-
urea is usually used as a topcoat of aromatic polyurea to provide an additional layer
of protection to the system. The high rigidity of aromatic polyurea prevents the
coating from breaking, while the light stability of aliphatic polyurea maintains its
color for longer usage.

1.5 Hybrid polyurea

Hybrid polyurea is another milestone of the polyurea system as a step to enhance the
properties of polyurea and give versatility to its features. Hybrids of polyurea are
usually employed to reduce the cost of the coatings as the second component in
the system is usually of low-price value such as polyurethane, epoxy, or acrylic.
Hybrid polyurea are mainly employed in wastewater systems’ corrosion mitigation
and roof coating applications [26] for their high adhesion performance [27]. Poly-
urea hybrid is typically a blend or combination of polyurea and other contemporary
polymers or monomers such as polyurethane, epoxy, polyamide, polyaniline, poly-
dimethylsiloxane, formaldehyde, polycarbonate, etc.
Hybrid polyurea is a result of combining it with one or more other polymers in
the backbone to reflect the advantages of all the polymers that have been physically
or chemically combined. This technology goes beyond just mixing two or more
liquid polymers together via in-situ or bulk polmyerization. By coreacting the poly-
mers during the synthesis stage, the resultant cured product could exhibit high per-
formance in the final applications as the drawbacks of a single polymer are
compensated with addition of one or more other polymers.
A summary of types of hybrid polyurea, their structure and properties, as well
as their applications are presented in Table 1.3. A poly(urea-urethane) hybrid is a
 (a)
Room temperature 50°C 100°C 150°C 200°C 250°C

(b)
Room temperature 50°C 100°C 150°C 200°C 250°C

1.5 Hybrid polyurea

FIGURE 1.1
Color change in polyurea with increasing temperature; (A) aromatic polyurea (isonate 143 L/Versalink P650), (B) aliphatic polyurea from the
formulation from our previous work.

7
 8
CHAPTER 1 Formulations and properties
Table 1.2 Comparison of aromatic polyurea with aliphatic polyurea.
Examples of
Type of polyurea isocyanate UV stability Properties Applications

Aromatic Methylene Discoloration and Tensile strength Automotive parts and ballistic protective
diphenyl crazing form on the (TS): 35e60 MPa coatings.
diisocyanate surface. Elongation at
(MDI) Formation of break (εB ): Over
Toluene microvoids and 400% [24,25].
diisocyanate surface
(TDI) irregularities.
Aliphatic Isophorene Very slow TS: 2.2 They are used as topcoats where high
diisocyanate degradation of e31.1 MPa UV exposure is expected especially for
(IPDI) color. εB : 293% roofing and flooring.
Hexamethylene e1000% [22,23]
diisocyanate The melting point
(HDI) is above 210 C.
Table 1.3 Summary of hybrid polyurea systems.
Synthesis Interaction Potential
Type method(s) mechanism Notable results applications References

Poly (urea-urethane) Bulk two-step H-bonding between urea Gas permeability up to 128 Gas separation [28,29]
polymerization and urethane linkages barrer.a membranes,
resulting in ordered, Breaking strength microcapsules,
disordered bonds increased from 39.5 to reprocessability
45.0 MPa through 5 cycles
of molding
Polyurea/poly (urea- In situ Weak Van der Waals Enhanced thermal stability, Microcapsules for [30]
formaldehyde) polymerization, forces between two high self-healing efficiency, self-reparable
atomic layer polymer chains and simulatenous coatings,
deposition (ALD) corrosion protection anticorrosion
performance for
metal substrates
Polyurea/ In situ- H-bonding between Up to 16% loss in heavy Adsorbent for heavy [31,32]
polydimethylsiloxane polymerization silicone hard segment metal (Cr, Co, Pb) metals (Cr, Co, Pb
and urea adsorption ions) uptake for
wastewater
purification
Poly (urea- In situ- Exchange reaction High mechanical Reprocessable or [33]
carbonate) polymerization between allophanate.b properties recycling of polyurea,
crosslinkers and free Ew70MPa; sy w13MPa; shape memory

1.5 Hybrid polyurea

hydroxyl groups εB w350%Þ
Polyurea/epoxy Interfacial Epoxy-urea bond from Damping coefficients Damping and [34,35]
reaction via (epoxide) þ (amine epoxy increased at higher vibration capability
condensation hardener) þ (isocyanate) excitation frequencies for structural
polymerization ( > 100 Hz) for fast curing materials
epoxies ( < 2.5 h)
Continued

9
 10
Table 1.3 Summary of hybrid polyurea systems.dcont’d

CHAPTER 1 Formulations and properties

Synthesis Interaction Potential
Type method(s) mechanism Notable results applications References
Polyurea/polyaniline Interfacial H-bonding via the Delay in rusting up to Self-healing, [36e38]
polymerization aromatic NeH bond 30 days in 10wt.% NaCl anticorrosion
present in both polymers solution, high impedance performance,
modulus (1011 U cm2) microcapsules,
wearable electronics
Polyurea/polyamide Interfacial Crosslinking between MgSO4 rejection retained Acid-resistant [39e41]
polymerization urea and amide bonds at > 98% for over 80 days nanofiltration
resulting in quadruple H- in 15 wt.% H2SO4 membranes,
bonding exposure hydrophobic
microcapsules,
aerogels for selective
CO2 sequestration
a
Barrer ¼ 1  1010 [cm3 (STP) cm/cm2/s cm Hg].
b
Allophanate group is C2H3N2O3.
 1.5 Hybrid polyurea 11

well known hybrid polyurea and has a composition that combines both polyurea
and polyurethane systems. The amine reacts with diisocyanate in a fast reaction
which doesn’t give enough time for the moisture reaction to happen therefore it
will reduce the level of moisture sensitivity, while polyol slows the reaction and
allows for a more reasonable price at the same time. Since both polymers are chem-
ically similar, they interact by forming H-bonding between opposite urea and ure-
thane linkages forming a crosslinked network. Similarly, epoxy interacts with
polyurea by forming H-bonding between the epoxide group and urea group. Ep-
oxies are known to be brittle and strong, resisting high vibration frequencies, hence
they are added into polyurea to bring the balance between damping and vibration
capabilities. Inventions on polyurea/polyurethane and polyurea/epoxy hybrid
products have been reported to be applied in industrial applications such as for
expansion joint sealants [42], extras service safety on battery boxes for hybrid elec-
tric vehicles [43], flexible and low-density foamed sponge for higher wet strength
and good load-bearing [44,45], the adhesive coating on oil, metal and glass sub-
strates, and hybrid microcapsules as a perfuming ingredient in detergents, or
body-care products.
Hybrids of polyurea with conductive polymers like polyaniline show prom-
ising results for wearable electronics, electronic structures, shape memory, and
smart materials that are self-repairing in case of crack due to mechanical abra-
sion or corrosion. The presence of viscous polyurea in the matrix may dampen
the conductivity nature of polyaniline due to the phase-separated structure that
flows on the latter during polymerization; however, addition of conductive fillers
could induce the flow of electrons through the path created by polyaniline
chains [39].
Some polymers are added into polyurea network through hybridization or
interfacial polymerization to enhance the chemical resisitivity, thermal stability
as well as self-healing efficiency such as polycarbonate, poly(urea-formal
dehye), and polyamide. These polymers have active bonds which dynamically
react again by forming H-bonding in case of minor cracks. Since the polyurea
and the above-mentioned polymers exhibit excellent chemical resistance, the
hybrid products are greatly useful for filtration and self-cleaning applications
(Figs. 1.2 and 1.3).

FIGURE 1.2
Chemical structure of an allophanate group.
12 CHAPTER 1 Formulations and properties

FIGURE 1.3
Example of a quadruple H-bonding between two polymers (polyurea and polyamide) [39].
Reprinted with permission from H.M. Park, M. Ismael, H. Takaba, Y.T. Lee, Acid-resistant thin-film composite
nanofiltration membrane prepared from polyamide-polyurea and the behavior of density functional theory study,
J. Membran. Sci. 645 (2022) 120175. https://doi.org/10.1016/j.memsci.2021.120175.

1.6 Conclusion
The three different types of polyurea systems; aromatic, aliphatic, and hybrid each
possess unique characteristics and properties. Aromatic polyureas are mechanically
strong, thermally stable as they are thermosets but they are weak UV-resisting coat-
ings, hence they are used as basecoats of the excellent UV-resisting aliphatic poly-
ureas. Though polyurea is an excellent viscoelastic elastomer, blending it with other
contemporary polymers has shown great possibilities for the extension of polyurea’s
applications to self-healing coatings, anticorrosion, and even conductive coatings. In
order to carefully design an excellent material to serve a specific application
requiring specific properties, extensive fundamental studies on the kinetics, chemi-
cal interactions of the different polymers in polyurea blends must be performed. On
top of that, it is also necessary to understand the packing and the segmental dy-
namics of the polymers when they are in a cross-linked network, especially for shape
memory, mechanical durability, and reprocessability applications of the material.

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