Introduction:

Polyurethanes (PUs) are versatile polymers which have traditionally been produced from
petroleum (Avar et al., 2012). As Polyurethanes PU, first synthesized by Otto Bayer in Germany
in 1937, forms a wide range of polymers with urethane linkage. The reaction of isocyanate
groups (–N=C=O) with polyhydroxyl groups yields PUs containing urethane group (–NH–CO–
O–) and functional groups such as ester, ether, urea, and amide Fig 1 (Calvo-Correas et al., 2016;
Dabb, 2011) . The structure consists of a soft part formed by polyols and a hard part formed by
isocyanate and chain extenders Fig 2. These starting materials are mostly derived from
petroleum-based building blocks (Engels et al., 2013) as a source of monomer for the polymer
synthesis. It has been recognized that the long term dependence on petroleum as a source of
monomers for the polymer synthesis is at risk (Schneiderman & Hillmyer, 2017; Tawade et al.,
2017). The PU products can be divided mainly into elastomers (Petrović et al., 2013), adhesives
(Bahattab et al. 2011), coatings (Chattopadhyay & Raju, 2007), and foams (Narine et al., 2007).
However, growing concerns about biodegradability, sustainability, carbon dioxide emissions,
and other environmental problems are driving the search of renewable sources (Petrovic, 2008)
which can replace fossil fuel that can be turned into viable polymeric materials (Lligadas et al.,
2010; Tan & Chow, 2010). Several biobased materials, including cellulose, starch, natural oil,
and sugar, have been utilized as starting materials for PUs (Gandini, 2008; Zhang et al., 2014;
Luo et al., 2013). A biobased polyurethane (BPU) polymer was derived from liquefied starch and
used as the coating material for CRU Fig.3. Vegetable oils are among the most promising,
because they are an inexpensive, readily available, and renewable resource.
Vegetable oils and related products (e.g., free fatty acids) are non-toxic, non-volatile, renewable,
and biodegradable resources which represent the main biomaterial for the synthesis of bio-
polyols and other chemicals (Grishchuk & KargerKocsis, 2011; Islam et al., 2014; Liu et al.,
2012b). Vegetable oils are triglycerides of saturated and unsaturated fatty acids. The six most
common fatty acids are palmitic (C16:0), stearic (C 18:0), oleic (C 18:1), linoleic (C 18:2),
linolenic (C 18:3), and ricinoleic (C18:1 OH) acids (in this notation, the first number represents
the number of carbon atoms, the second number represents the number of carbon− carbon double
bonds, and OH represents hydroxyl groups in the fatty acid) (Zhang et al., 2015).
Lot of reports available on vegetable oil based polymeric resins such as soybean oil (Lu &
Larock, 2008), castor oil (Zhang et al., 2013), neem oil (Chaudhari et al., 2013), sunflower oil
(Xia & Larock, 2010), linseed oil (Alam et al., 2009), jatropha oil (Alam & Alandis, 2011),
cottonseed oil (Meshram et al., 2013), mahua oil (Yemul et al., 2013), etc.
There are several methods to prepare vegetable oil-based polyols: thiolene coupling reaction
(Samuelsson et al., 2004), ozonolysis (Petrović et al., 2005), hydroformylation (Petrović et al.,
2008), transesterification (Tavares et al., 2016), etc., being the epoxidation of the double bonds
and their further hydrolysis the most important path way(Miao et al., 2014).Different functional
groups, such as ester (Fridrihsone et al., 2013), acyl (Sharma et al., 2008), azide (de Haro et al.,
2016b), or amine groups (Biswas et al., 2005), have been incorporated into bio-polyols using this
route. Among the different vegetable oils, grape seed oil is a highly unsaturated one which can
be obtained by pressing or solvent Extraction from grape seeds (DaPorto et al., 2013;
Venkitasamy et al., 2014). Despite that it is an edible oil, it can be considered as a by-product of
winemaking industry since the potential production of grape seed oil is huge compared with its
average consumption as edible oil (Ng et al. 2015).
PU shows versatile and excellent physical, chemical and mechanical properties, which has
increased their demand in various fields such as foam, elastomers, adhesive, ink, paints, and
coatings applications (Petrović ET AL., 2013; Rajput et al., 2014). Applications of PU in the
coating industry are due to their excellent scratch resistance, stiffness, chemical, and corrosion
resistances, low temperature flexibility, and a wide range of mechanical strength (Xu et al.,
2008). Chemically all fats and oils are esters of glycerol and fatty acids, while physical
properties and structures of natural oils (triglycerides), and fatty acids vary for each oil Fig.3.
Fatty acid composition of cottonseed oil is as oleic acid (18:1) 17.6%, linoleic acid (18:2) 54%,
linolenic acid (18:3) 0.3%, and myristic acid less than 1% (Gunstone, 2011), while karanja oil,
contains oleic acid (18:1) 44–72%, linoleic acid (18:2) 10–18%, and linolenic (18:3) and
myristic acids are absent (Atabani et al., 2013). Among the natural oils, Cashew nut shell liquid
(CNSL) and their compositions is an important renewable resource and widely used as a starting
material for many industrial products (Phani Kumar et al., 2002). Cashew nut shell liquid is
organic aromatic oil which contains various types of natural phenolic components including
around 90 % anacardic acid and 10 % cardol shown in Fig. 4 (Das et al., 2004). Cardanol is a
renewable resource of immense potential can be obtained by the decarboxylation of anacardic
acid (Gandhi et al., 2012). Generally, cardanol is consider as the major component for the
manufacturing of PU foams and castor oil based foams due to their low thermal conductivity and
high insulation effect mostely used in construction, refrigeration and industrial application
(Ogunleye et al., 2008).. Renewable resources as a source of polyols in the preparation of PU
foam has also been widely studied (Petrović, 2008; Tan et al., 2011).. Most commercial polyols
are derived from petroleum resources which are diminishing rapidly. The current research is
being focused on developing newer technologies from renewable resources (Narine et al., 2007;
Sultania et al., 2010).

Membrane separation:
Nowadays, membrane technologies are becoming more frequently used for separation of wide
varying mixtures in the petrochemical-related industries and can compete successfully with
traditional schemes. Membrane separations find many applications because they have many
advantages like cost effectiveness, easy operation and a high pre-concentration factor with a high
degree of selectivity. The pre-concentration is useful for determining the metal ions present at
concentrations much lower than the detection limit of a particular instrument. Pre-concentration
associated with selectivity helps eliminate interference of matrix elements. Membrane
separations are also used for treatment of large volumes of low-level radioactive effluents
generated at the various stages of fuel reprocessing in the nuclear industry, wherein significant
volume reduction is achieved by membrane separation before processing by conventional
methods (Ramkumar et al., 2012).
Membrane is defined essentially as a barrier, which separates two phases and restricts transport
of various chemicals in a selective manner. A membrane can be homogenous or heterogeneous,
symmetric or asymmetric in structure, solid or liquid; can carry a positive or negative charge or
be neutral or bipolar. Transport through a membrane can be affected by convection or by
diffusion of individual molecules, induced by an electric field or concentration, pressure or
temperature gradient. The membrane thickness may vary from as small as 10 microns to few
hundred micrometers. The types membrane can be classified as below (Baker, 2004; Kargari et
al., 2004; Kargari et al., 2004):
 Isotropic membranes
o Microporous membranes
o Nonporous, dense membranes
o Electrically charged membranes
 Anisotropic membranes
 Ceramic, metal and liquid membranes
Membrane processes: Transport through the membrane takes place when a driving force is
applied to the components in the feed. In most of the membrane processes, the driving force is a
pressure difference or a concentration (or activity) difference across the membrane ( Kujawska et
al., 2015). Parameters such as pressure, concentration (or activity) and even temperature may be
included in one parameter, the chemical potential μ. Another driving force in membrane
separations is the electrical potential difference. This driving force only influences the transport
of charged particles or molecules (Scarazzato et al., 2017).
Biobased Polyurethane Membrane:
Some biobased polyurethane membrane for separation technique are mentioned below.
1. Anti-microbial microporous polyurethane membrane:
The purpose of this research was to design a multifunctional membrane material, which
possesses antimicrobial properties and maintains the balance between comfort and protection, i.e.
water vapor transport and barrier protection (Lee & Obendorf, 2007). Antimicrobial materials
can be chemically engineered by adding functional antimicrobial agents onto the surface or
within the matrix to either kill or inhibit the growth of microorganisms. Commonly used
antimicrobial agents, such as antibiotics, to protect the substrates from biological activities (Tan
& Obendorf, 2007)

2. Poly(ethylene glycol)/poly(tetra methylene glycol) based polyurethane membrane:

The effect of the structure of polyether-based polyurethane (PU) membranes on their gas
separation properties has been investigated. PU membranes were prepared by thermal phase
inversion method. The permeability of pure N2, O2, CH4 and CO2 gases were determined
(Talakesh et al., 2012).
3. Polyether-based polyurethane–silica nanocomposite membranes:
Scientists investigated the effect of silica particles on the gas separation properties of high
performance polyimides. They showed that, incorporation of silica particles into the polymer
matrix mainly improved the gas separation properties of polymer–silica membranes, especially
in the case of O2/N2 separation (Sadeghi et al., 2011).
4. polyurethane and polyurethane urea membranes with different soft segments:
Dense membranes with 30–40μm in thickness prepared by casting 20wt.% N,N-
dimethylformamide (DMF) solutions onto glass plate were examined for the separation of
toluene vapor from nitrogen stream. The use of polyurethane or polyurethane urea membranes
with single and mixed soft segments for the separation of toluene/N2 .

Fig.1 Schematic diagram of PU synthesis.

Source: (Olcay et al., 2020).

Structures of (a) diphenyl-methylene diisocyanata (b) Hexamethylene diisocyanate
(c) Naphthalene 1,5-diisocyanate
(a)

O C N

N C O

(a) diphenylmethylene diisocyanate

Chemical structure of diphenyl-methylene diisocyanate.
(b)
O
C N
N C
O
hexamethylene diisocyanate
Chemical structure of hexamethylene diisocyanate.

(c)
O
C
N

N
C
O
naphthalene 1,5-diisocyanate
Chemical structure of naphthalene 1,5-diisocyanate

Fig.2 Soft and hard segments of Polyurethane.

Source: (Olcay et al., 2020).

Fig.3 (a) Liquidation Mechanism of Starch and Reaction Mechanism of the Biobased (b)
Polyurethane
Fig.4 Systematic representation of triglyceride structure of vegetable oil.

Source: (Noreen et al., 2016).

Fig.5 composition of cashew nut shell liquid.

Source: (Rwahwire et al., 2019)

Review:
Isfahani et al., 2020 observed that In this study, we report highly selective CO2 polyurethane
incorporated with cured epoxy nanoparticles. PU–epoxy composite membranes were prepared
via solution casting method. The obtained SEM micrographs confirmed the nano-scale
distribution of epoxy particles in the polymer matrix. DSC and FTIR spectra showed different
phase separation for the PU composites compared to the pure PU. The effect of epoxy
nanoparticles on the gas permeability of CO2, CH4, O2 and N2 was studied at 25 8C and 10 bar.
The selectivity of CO2/N2 increased from 25 for the pure PU membrane to 55.5 for the PU–
EP10, while the CO2 permeability was unchanged.

Aframehr et al., 2020 reported that for the first time the fabrication of a glassy polymer/nickel
oxide hybrid membrane as a gas separation membrane. A PI (Matrimid) is used as a continuous
phase, and nickel oxide nanoparticles (NiO) were utilized as a dispersed phase. The structure of
mixed matrix (MMMs) and pure Matrimid membranes are investigated by employing various
characterization techniques including scanning electron microscopy (SEM), Fourier transforms
infrared (FT-IR), differential scanning calorimetry (DSC), X-ray diffraction (XRD), and tensile
stress-strain to characterize the NiO nanoparticles. The effect of NiO nanoparticles content (0–5
wt%) on gas permeability of pure CO2, CH4, O2, and N2 gases at different operating
temperatures (24–40 ◦C) and feed pressures (1–5 bar) were surveyed. The results revealed that
the CO2 permeability almost did not change and CO2/CH4 selectivity of PI was enhanced with
low-level loadings of NiO while the gas permeability of N2, CH4, and O2 was reduced. Our
results indicated that since NiO nanoparticles have high interaction with CO2 as Lewis pairs,
they have high potential to improve the gas permeability properties of polymer-based
membranes. This approach allows predicting the gas transport properties, structure/solubility
quantitative relationships of different gases, especially CO2 through the MMMs system

Shirvani et al., 2019 stated that the Polymer blending and mixed-matrix membranes are
well-known modification techniques for tuning the gas separation properties of polymer
membranes. Here, we studied the gas separation performance of mixed-matrix membranes
(MMMs) based on the polyurethane/poly(vinyl alcohol) (PU/PVA) blend containing silica
nanoparticles. Pure (CO2, CH4, N2, O2) and mixed-gas (CO2/N2 and CO2/CH4) permeability
experiments were carried out at 10 bar and 35 ◦C. Poly(vinyl alcohol) (PVA) with a molecular
weight of 200 kDa (PVA200) was blended with polyurethane (PU) to increase the CO2
solubility, while the addition of silica particles to the PU/PVA blend membranes augmented the
CO2 separation performance. The SEM images of the membranes showed that the miscibility of
the blend improved by increasing the PVA contents. The membrane containing 10 wt % of
PVA200 (PU/PVA200–10) exhibited the highest CO2/N2~32.6 and CO2/CH4~9.5 selectivities
among other blend compositions, which increased to 45.1 and 15.2 by incorporating 20 wt %
nano-silica particles.

Shirvani et al., 2018 observed that the prepared blend membranes were characterized by Fourier
transform infrared spectroscopy (FT-IR), X-ray Diffraction (XRD), and scanning electron
microscopy (SEM). The effects of molecular weight of PVA, and blend composition on the gas
transport properties of N2, O2, CO2 and CH4 were investigated. Obtained results show that the
permeability of gases decreased in blend membranes by poly(vinyl alcohol) (PVA) molecular
weights while their gas selectivity enhanced. Comparison of the gas separation performance of
the prepared membranes to Robeson upper bound, reveal the enhancement of membrane
performance by introducing PVA in PU matrix

Zhang et al., 2019 conducted that the Petroleum depletion and climate change have
inspired research on bio-based polymers and CO2 capture. Tung-oil-based polyols were applied
to partially replace polyether-type polyols from petroleum for sustainable polyurethane. Tung-
oil-based polyurethane (TBPU), was prepared via a two-step polycondensation, that is, bulk
prepolymerization and chain extension reaction. The graphene oxide (GO) was prepared via
Hummer’s method. Then, TBPU was composited with the GO at different ratios to form a
TBPU/GO hybrid film. The GO/TBPU films were characterized by fourier transform infrared
spectroscopy (FTIR), differential scanning calorimeter (DSC), thermal gravimetric analysis
(TGA) and scanning electron microscope (SEM), followed by the measurement of mechanical
properties and gas permeability. The results showed that the addition of tung-oil-based polyols
enhanced the glass transition temperature and thermal stability of TBPU. The mechanical
properties of the hybrid film were significantly improved, and the tensile strength and elongation
at break were twice as high as those of the bulk TBPU film. When the GO content was higher
than 2.0%, a brittle fracture appeared in the cross section of hybrid film. The increase of GO
content in hybrid films improved the selectivity of CO2/N2 separation. When the GO content
was higher than 0.35%, the resulting GO agglomeration constrained the gas separation and
permeation properties.
Recent advances in polyurethane applications
The general properties (physical and chemical) of any PU are dependent on the nature of the
individual reactants (especially the R1 and R2 groups) from which it is produced.
1.Building and construction applications:

Present day buildings need to meet certain requirements in terms of the use of construction
materials, including highperformance strong materials, light weight, easy to install, durable and
versatile. The use of PUs for construction and building applications is on the increase due to their
specifc properties, such as excellent heat insulation capacity, highly desirable strength-to-weight
ratio, versatility and durability. In the roofng application, the plastic coverings on the PU surface
can help to keep the house cool on the one hand, and help to reduce energy usage on the other
hand. Generally, PU materials help to add fexibility to new homes, such as the entry door and
garage doors, which contains panels with foam cores (Madbouly et al., 2006)

2.Automotive applications
The areas of PU application in the automotive industry are vast. Aside from its common use as a
foam to make vehicle seats more comfortable, it may also be used in car bodies, bumpers doors,
windows and ceiling sections. . PUs also help to provide better automobile mileage through
reduced weight, increased fuel economy, good insulation with proper sound absorption,
(Njuguna et al., 2011) great comfort for passengers (Deng et al., 2003) and high corrosion
resistance properties. Deng R. and his colleague opined that since a clear majority of vehicular
seats are mainly foams, the dynamic comfort of users may be controlled by modifying the foam
properties to obtain the desired quasi-static features (Njuguna et al., 2011). PU foams have been
reported to occupy the largest fraction of the global polymeric foam market (Deng et al., 2003)

3. Marine application
PU materials have contributed a large innovation to the recent development in boat technology.
PUs into various products for the specifc advantages they provide, including elasticity, durability
and ease of processing ability with good suitability for cable and wire coatings, drive belts,
hydraulic seals and hoses and engine tubing as well as ship construction. Some PUs can also be
used to recognize certain active materials, (Xiao et al., 2011) and for removing certain organic
substances from water bodies. Cyclodextrin PU, for example, has been reported to be effective
towards the removal of certain organic materials, such as paraben, from water (Chin et al., 2010).
A study was conducted over a long period (2 and 5 years) observing the polyether-based PU
materials under seawater and adverse conditions (Davies et al., 2007)
4.Coating applications
Over the years, there has been continuous research on suitable materials for coating applications.
PUs have been reported to possess great potential as paint and surface-coating materials (Dutta et
al., 2005 & Dutta et al., 2009) Research in this area saw the development of certain non-linear
hyperbranched polymers, which have metamorphosed into other hyperbranched PUs with gloss,
high solubility and fexible coating properties (Van Benthem & R. A. (2000) To modify these
hyperbranched materials for certain fame-retardant coating applications, compounds containing
nitrogen, halogen or phosphorus may be incorporated into them (Chen et al., 2010)

5.Medical applications
PUs are used in several medicine-related applications, including, but not limited to, general
purpose tubing, surgical drapes, catheters, hospital bedding, wound dressing and several other
injection-moulded equipment. They are used for these applications due to their availability, good
mechanical and physical properties and biocompatibility (Zhou et al., 2014 : Wang et al., 2012)
of PUs in medicine-related application helps to offer cost effectiveness and provides adequate
room for toughness and longevity of materials (Middleton et al., 2000) Furthermore, other
medical-application-based studies were performed, including studies on a chitosanbased PU for
antibacterial properties (Baheirae et al., 2014) and biodegradable electroactive PUs for cardiac
tissue engineering.

6.Appliances, fooring and packaging applications

Most of the appliances that consumers use these days are based on PUs. For fooring purposes,
PUs have several specifc applications, such as top coatings or as carpet underlay foams. They
can help to make floors more durable, aesthetically pleasing and easy to maintain.

7.Apparels applications
Initially when PU was discovered to be a good for apparels, where PUs are converted to thin
threads and incorporated into nylon to produce garments that are stretchable and lightweight.
Among the PU types, aqueous dispersions of WPUs have been widely incorporated into textile-
related applications.218 Among the PU types, aqueous dispersions of WPUs have been widely
incorporated into textile-related applications (Xinrong et al., 2014). The product was found to
offer great UV dyeing protection to cotton fabrics, and it also showed great suitability for several
other textile applications (Xinrong et al., 2014)
8Wood composite applications
PUs are very important inclusions in many present day materials, including wood composites
Recently PU-based composites were prepared by using activated carbon for electromagnetic
interference (EMI) shielding (Shaaban et al., 2015) In a different study, PU/wood composites
were prepared from wood wastes and polyols (Fornasieri et al., 2011) These changes were
associated with several factors, such as the glycerol content, condition of the reaction and the
stoichiometric ratio of the reactants (Patel et al., 2005) The significance behind the use of natural
fibres or wood for PU-based composites is that they are hydroxyl-enriched substances, which can
undergo chemical bonding easily with diisocyanate (Mohebb et al., 2009)

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