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INTRODUCTION
kitchenware, toys, and resilient flooring to name a few, and are extensively employed in many
such key industries as automobile, aerospace, electrical, and medical industries (Richardson,
2005).
Useful as they are, plastics are disposed constantly by people, and eventually
accumulate to large piles along with other wastes. Various efforts have been addressed in
response to the problem: the creation of sanitary landfills in strategically located places,
adoption of selective collecting and recycling programs, and active government and civic
participation (Vilpoux and Averous, 2004); still, people resort to quicker, short-term solutions
such as incineration and waste burning at household levels, aggravating the effects of global
biodegradable plastics, which currently exist in the market. Biodegradable plastics refer to
Biodegradable plastics have used starch as fillers in the 1970’s in response to the rise
of petroleum prices, the latter being the prime component of plastics manufacture (Curvelo, et
al., 2001; Garth and Kowal, 2001). Starch-based polymers are made from starch, which is a
linkages in the C1 and C4 positions (Whistler and Hilbert, 1984). Made up of two polymers,
the linear-chain amylose and the branched-chain amylopectin, the alpha linkage of amylose
allows it to be flexible and digestible, hence giving it the ability to be converted to starch-
found in several forms due to the origin of its raw material (Lawter and Fischer, 2000).
Although easily obtained from such agricultural commodities as corn, potatoes, and tapioca,
starch production and extraction has been done in expense of food production and
A superlative substitute could be sago starch from the sago palm, a crop widely
cultivated in peat soil land in tropical areas (Shibata et al., 2006). The palm exhibits large
a notable starch source, and alleviating extensively the problem of accruing atmospheric
greenhouse gases. The palm, in addition, is abundant here in the Philippines, specifically in
Starch-based plastics have starch contents from 10% to 90% and can be any one of
thermoplastic starch materials (Garth and Kowal, 2001); thermoplastic starch blends with
synthetic aliphantic polysters such as poly-ε -caprolactone (PCL), poly-lactic acid (PLA),
and polybutylene succinate adipate (PBSA); several others are also existent nowadays
(Nolan-ITU Pty, 2002). Nonetheless, of these categories, the thermoplastic starch materials
gained attention since the high amount of starch, 70 to 100 percent, engenders a material with
continuous supply of thermomechanical energy. More often than not, this combination of
thermal and mechanical input can obtained by extrusion. In this process, starch, along with
This study basically aimed to utilize sago starch as the main substrate for
successful;
1.3 Hypothesis
H0: There is no significant difference on the mean tensile strength of the TPS exposed
to different treatments.
Tensile Strength
Water Disintegration
For this study, the molten product was evaluated by its tensile strength and
degradability only. The extrusion processing part of the study took place in University of the
This study serves to find alternative ways of controlling the problem on accumulation
of plastics in the environment. The production of thermoplastic starch from sago starch can be
of great help in reducing plastics in the environment since they are composed of degradable
polymers, and will eventually degrade into substances that are less harmful to the
environment. Furthermore, this study will help in minimizing the factors that contribute to
global warming, since it is degradable unlike any other common plastics that require burning
for decomposition.
Glycerol -A syrupy, sweet, colorless or yellowish liquid, C3H8O3, obtained from fats
Starch -A naturally abundant nutrient carbohydrate, (C6H10O5)n, found chiefly in the seeds,
fruits, tubers, roots, and stem pith of plants, notably in corn, potatoes, wheat,
tearing.
Materials that are consumed by microorganisms such as bacteria, fungi, and algae are
polymer chain and consume the material through several methods. Biodegradable plastics can
the material and on the constitution of the final product, not just on the raw materials used
for its production. Therefore, biodegradable plastics can be based on natural or synthetic
resins. Natural biodegradable plastics are based primarily on renewable resources (such as
7
starch) and can be either naturally produced or synthesized from renewable resources. Non-
product must meet the performance requirements of its intended function, many natural
biodegradable plastics are blended with synthetic polymers to produce plastics which meet
Because the oil embargo in the early 1970s caused the price of plastics to almost
double, researchers began to look for less expensive, non-plastic filler. The result of their
search was starch-based polymers. Since that time, starch-based polymers have remained
the most commonly used and lowest-costing ingredient of all biodegradable polymers
Starch-based biodegradable plastics may have starch contents ranging from 10% to
greater than 90%. Starch based polymers can be based on crops such as corn (maize), wheat
or potatoes. Starch content needs to exceed 60% before significant material breakdown
occurs. As the starch content is increased, the polymer composites become more
biodegradable and leave less recalcitrant residues. Often, starch-based polymers are blended
achieve the necessary performance properties for different applications (Averous, 2004;
glucosidic linkages between the sugar groups leading to a reduction in chain length and the
splitting off of sugar units (monosaccharides, disaccharides and oligosaccharides) which are
At lower starch contents (less than 60%) the starch particles act as weak links in
plastic matrix and are sites for biological attack. This allows the polymer matrix to
disintegrate into small fragments, but not for the entire polymer structure to actually
thermoplastic starch products; starch synthetic aliphatic polyester blends; starch PBS/PBSA
than 70% and are based on gelatinized vegetable starch, and with the use of specific
blended with other materials to form useful mechanical properties. Importantly, such TPS
content plastics are highly hydrophilic and readily disintegrate on contact with water. This
can be overcome through blending, as the starch has free hydroxyl groups which readily
(Averous, 2002).
The Cooperative Research Center (CRC) for the International Food Manufacture
and Packaging Science Australia has developed its own version of TPS biodegradable
plastics. These natural vegetable starch polymers have amylose content greater than 70%.
Trials have been successfully performed using maize starch polymers as mulch film, and
the material was found to perform as well as polyethylene film, with the added advantage
that after harvest, the film can be simply ploughed into soil. These natural starch polymers
are now being commercialized through a new company called Plantic Technologies Ltd.
shopping bags, bread bags, bait bags, over wrap, ‘flushable’ sanitary product backing
material, and mulch film. Foam loose fill packaging and injected molded products such as
takeaway containers are also potential applications. Foamed polystyrene can be substituted
by starch foams that are readily biodegradable in some loose-fill packaging and foam tray
9
applications. Foamed starch loose-fills are rather easy products to produce and this area has
become an early market for biodegradable plastics. During its, preparation, raw starch is
premixed with 25 to 50 weight percent water and fed into an extruder capable of imparting
intensive shear and operating at high temperature (higher than the boiling point of water,
i.e., 150-180°C). Under these conditions of shear and temperature, starch breaks down,
loses its crystallinity, and gets plasticized with water, resulting in a homogenous amorphous
mass. When this gelatinized starch/water mixture exits the extruder, the water that is present
in the mass that is present in the mass at a temperature higher than its boiling point expands
into steam due to a sudden drop in pressure, and the foam is formed. Generally a plasticizer
(such as glycerol) and other polymer (such as polyvinyl alcohol) impart more reproducible
properties to starch foam. Along with the biodegradation of the polymers by sugar
molecules, certain TPS grades are also fully water solube (Averous, 2004).
The TPS is a relatively new concept and, today, it is one of the main research hints
for the manufacturing of biodegradable materials (Curvelo, et al., 2001). The starch is not a
real thermoplastic, but, in the presence of a plasticizer (water, glycerin, sorbitol,etc.), high
temperatures (90-180°C) shearing, it melts and fluidizes, enabling its use in injection,
extrusion and blowing equipment, such as those for synthetic plastics. So as to obtain a
thermoplastic starch, it is necessary that the starch maintain its semi-crystal granular
structure and that it behaves in a way similar to that of a melted thermoplastic, obtained
through a mono- or twin-screw extrusion with the use of mechanical and thermal energy
The water added to formula plays two roles: it is an agent that breaks the structure
of the native granule, breaking the bonds of hydrogen chains, and it is a plasticizer.
which will be only slightly influenced by the atmospheric conditions in the sorption-
desorption mechanism, and that will allow a melting phase at a temperature lower than that
of the starch degradation (Averous, 2002). During starch extrusion, the combining of
material (Averous et al., 2001). Afterwards this material can be transformed by means of
mechanical properties under humid conditions affect the use of starch. Starch derivatives
present a high permeability to moisture and degrade rapidly for many types of applications.
Changes to remedy these problems make the final product more expensive, what limits any
solutions (Lawter and Fischer, 2000). According to Averous et al. (2001), besides being
susceptible to moisture, starch biopolymers have mechanical properties that change as time
goes by, apart from their low resistance to impacts. Moreover, in the case of thermoformed
products, the thinness of formed products limits the use of starch derivatives. According to
Levesque (2001), the use of starch and its derivatives as the only component of
objects), which, however, evolve rapidly due to the atmospheric humidity. It is necessary to
properties to plastify the starch. This material can be processed in the same way as synthetic
materials: extrusion, injection, etc. According to Lourdin et al. (1999), a plasticizer such as
glycerol and sorbitol is added in a ratio ranging from 20% to 40% to the starch weight. The
plasticizer content is directly related to the mechanical properties and glassy transition of
the material. The use of plasticizer also allows for a lower water activity, limiting the
plasticizing power, the material behavior changes according to the relative humidity of the
air (Averous, 2002), through a sorption-desorption mechanism. The higher the plasticizer
content (polyol), the higher is the moisture content. At the same time, the properties of the
material evolve as time goes by, even when moisture and temperature are controlled,
translating into a lower elongation breaking and higher rigidness. So as to improve the
blended with the starch or applied to multilayered films, with an internal layer of starch and
two external layers of impermeable polymer. According to Averous et al. (2001) and Martin
et al. (2001), starch films can complecting with thermoplastic polyesters, such as
traditional plastics. As regards biodegrabadle films, the industrial process reaches a yield
The multilayered structure is more difficult to be produced than the blended one
(Averous, 2001). The main manufacturing technique is the co-extrusion (with a flat die) for
the production of a film that can be thermoformed for the manufacturing of, for example,
trays. Hot compression can also be applied to the films, but, in this case, there are fewer
adherences among the layers. Not all materials are compatible among themselves, and they
can come unstuck. In this case, compatibilizers are added (Averous, 2002). In the case of
According to Martin et al. (2001), the adherence among the films diminishes through the
adding synthetic polymers, cross-linked agents, such as Ca and Zn, salts, or lignin. TPS
properties vary according to the type of starch used, emphasizing the amylose content. The
almost linear increase of breaking forces and elongation according to the amylose content
can be explained through the larger agglomeration capacity of linear macromolecules while
ramified structures of amylopectin originate nodules. The amylose-rich corn starch (70% of
manufacturing of these materials. However, even that the values of maximum forces for
breaking are acceptable (30 to 60 MPa), materials are fragile due to their low deformation
(approximately 6%). This property explains the reason why it is necessary to add other
components, such as plasticizers, able to enhance the plastic behavior (Lourdin et al., 1999).
.According to Lourdin et al. (1995 and 1999), the effect of the amylase content is
considered a favorable factor when there is no plasticizer. When plasticizers are added,
12
there is a reverse effect, since films with a larger content of amylase content can be
preferable. Besides the blend of starch with other polymers and the use of plasticizers,
many surveys have been conducted regarding the possibility of modifying the starch so that
the TPS can acquire the desirable properties with regards to both mechanical and moisture
Starch-based films found in the market are made mainly from starch complected
biodegradable products (Bastioli, 2000). When used for the manufacturing of bags for the
recycling of organic waster (composting), packaging, hygienic items and agriculture, the
properties of these films are similar to those of low density polyethylene. The more
common products of starch-based films are: purchase bags; consumer goods packaging;
food packaging; composting bags; hygiene and cosmetics; and funerary goods.
Purchase bags were introduced in the market in 1999 and started being used in
many supermarkets in Scandinavia and in the Mediterranean Coast. They were introduced
in places where collecting of organic wastes already existed and where they were accepted
as biodegradable compost bags. Bastioli (2000) stated that these bags have a behavior
similar to the bags made with LDPE with regards to the maximum weight and most of its
performances.
In consumer goods packaging, the main market is that of silk paper, but there are
markets for magazines’ wrapping and bubble films, mainly for electronic goods (Basioli,
2000).
It was further added that in food packaging, the main markets are those of bags for
fruit, vegetables and bakery products. The high cost of biodegradable products limits this
market, but starch films have an advantage against traditional plastics, that is to say, they
Meanwhile, composting bags are used in the selective collecting of organic waste,
which will be treated to produce a compound. Million of Europeans already use these bags
(Bastioli, 2000)
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In hygiene business lines, biodegradable polymers are found in diapers, swabs and
compliance with the rules on the use of biodegradable materials (Thouzeau, 2001).
According to Van Tuil et al. (2000), multi layered biodegradable films can be used
as food packaging with either controlled atmosphere or gas. Starch packaging boast the
characteristics of being an excellent barrier to O2 and CO2, facing problems only with water
and water vapor. The application of layers of biopolymers resistant to water in the ratio of
10% allowed Van Tuil et al. (2000) to obtain films resistant to water with a thickness from
30 to 100 μm. This material is currently commercialized by AVEBE under the name of
Paragon® and can be processed by means of blowing and used in multilayer’s with PLA or
1.8.4 Starch
Starch is the major carbohydrate reserve in plant tubers and seed endosperm where it is found
as granules (Buléon et al., 1998). It consists of two types of molecules: amylose (normally 20-
30%) and amylopectin (normally 70-80%). Both consist of polymers of α-D-glucose units in
the 4C1 conformation. In amylose these are linked -(14)-, with the ring oxygen atoms all on
the same side, whereas in amylopectin about one residue in every twenty or so is also linked -
(16)- branch-points both depend on the source of the starch, for example, amylomaizes
contain over 50% amylose whereas 'waxy' maize has almost none (Li and Yeh, 2001; Singh et
al., 2003). The representative partial structures of the two components of starch are shown in
Figure 1.
14
A
15
Fig. 1. Representative partial structures of (A), amylose and (B), amylopectin (Lifted from
Chaplin, 2008).
lower molecular weight with a relatively extended shape whereas amylopectin has huge but
compact molecules. Although α-(14) links are capable of relatively free rotation, hydrogen
bonding between the O3' and O2 oxygen atoms of sequential residues tends to encourage a
helical conformation. These helical structures are relatively stiff and may impart adjacent
(14)-D-glucose units dependent on source (a very few α-16 branches and linked
phosphate groups may be found (Hoover, 2001), but these have little influence on the
molecule's behavior (Buléon et al., 1998). Hydrogen bonding between aligned chains causes
retrogradation and releases some of the bound water (syneresis). The aligned chains may then
form double stranded crystallites that are resistant to amylases. These possess extensive inter-
16
solubility. The amylose content of starches is thus the major cause of resistant starch
enzymes that leave each chain with up to 30 glucose residues. Each amylopectin molecule
contains a million or so residues, about 5% of which form the branch points. There are
usually slightly more 'outer' unbranched chains (called A-chains) than 'inner' branched chains
(called B-chains). There is only one chain (called the C-chain) containing the single reducing
Sago is a powdery starch made from the processed pith found inside the trunks of
the Metroxylon sagu palm, a pinnate-leaved palm occurring in the hot humid tropics of
Southeast Asia and Oceania. The palm is soboliferous; it produces tillers or suckers. Once
planted, a regular succession of suckers is produced from the lowest part of the trunk,
sago yields are exceptionally high. Under good conditions the range is from 15 to possibly
The sago palm is a promising source of carbohydrate. In areas where the sago palm
grows, sago pith is used for human consumption and livestock feeding. The palms are
harvested at the age of 7 to 15 years just before they flower. They only flower and fruit
once before they die. When harvested the stems are full of the stored starch which would
otherwise be used for flowering and fruiting. The trunks are cut into sections and into
halves and the starch is beaten or otherwise extracted from the heartwood, and in some
17
traditional methods it is collected when it settles out of water. One palm yields 150 to 300
noodles, white bread, and sago pearls (similar to tapioca). In India pearl sago (a form of
sago) is called Sabudana, and is used in a variety of dishes including khichdi, wafers and
biodegradable plastics and in producing fuel alcohol and ethanol (PCARRD, 2001).
Sago starch contains 27% amylose, the linear polymer, and 73% amylopectin, the
branched polymer (Ito et al., 1979). Kawabata et al., (1984), however, give the amylose
content of sago starch as 21.7%. A grain size distribution of 16.0-25.4 mm was found. Jong
(1995), however, found a mean length of almost twice as much, about 40 mm. It is probable
that the grain size increases with age of the trunk, until initiation of the inflorescence.
temperature is 70°C. Viscosity decreases with deterioration of the starch quality, owing to
microbial activity (Cecil et al., 1986). In the modern starch industry, starches can be
modified to quite an extent. Provided there is a regular supply of cheap, clean and non-
corroded starch, sago will be clearly competitive to all other starches, and for some
1.8.6 Extrusion
Extrusion plays a significant part on the plastic industry. The process is performed
conveyed down an electrically heated barrel by a rotating screw. As it proceeds down the
barrel, the compound melts and is forced through a die, which imparts the said compound’s
shape. The formed item is generally cooled and solidified in a water bath (Wikipedia, 2008;
Rosen, 1982).
formation of its glucose units, and must be modified and destructured to be converted and
used for other applications. To do this, starch must be gelatinized in the presence of water
and heat to disrupt the granular organization of the starch molecules. Such process results to
the reduction of the melting temperature and glass transition temperature of the starch,
Except for the purpose as filler to produce reinforced plastics, native starch must be
modified to find applications such as destructured starch. The destructuring agent is usually
water. Starch gelatinization can be obtained with the combination of water (high content)
and heat. Gelatinization, essentially, is the disruption of the granule organization. The
hydrogen links. A reduction of both, the melting temperature (Tm or Tf) and the glass
transition (Tg) is then obtained. According to the level of destructuration and the water
content, different products and applications can be obtained; for instance, expanded
structures can be produced with rather high water content. Such closed cells structures
(foams) have been developed to obtain shock absorbable and isothermal packaging. Most
decreasing the moisture content (20% w/w), the melting temperature tends to be close to the
degradation temperature. For instance, for pure dry starch Tm is 220-240°C (Russell, 1988),
(Shogren, 1992). To overcome this last issue, we add a non-volatile (at the process
temperature) plasticizer to decrease Tm, such as glycerol or other polyols (sorbitol, PEG,
etc.). A mixture of different polyols can also be held. Other compounds such as those
thermal and mechanical outputs can be obtained by extrusion. The process can be one or
19
two stages. In a one-stage process, the extruder, usually a twin-screw extruder is fed with
native starch. Along the barrel, water and liquid plasticizer are successively introduced. In a
two-stage process, the first stage is a dry blend preparation (Averous et al., 2000). Into a
turbo-mixer, under high speed, the plasticizer is added slowly in to the native starch until a
homogenous dispersion is obtained. Then, the mixture is placed in a vented oven allowing
the diffusion of the plasticizer into the granule. The plasticizer swells the starch. After
cooling, the right amount of water is added to the mixture using a turbo-mixer. This dry
blend is then introduced into an extruder. The different stages of the extrusion process are
given in Figure 4. The starch granules are fragmented. Under temperature and shearing,
starch is destructured, plasticized, melted but also partially depolymerized. After the
Fig. 2. Schematic diagram of starch extrusion processing (Lifted from Averous, 2004).
Parker et al., 1990; Pdmanabhan and Bhattacharya, 1991). Viscosity data and rheological
models that take into account these variables have been reported in literature. Martin et al.
(2003) have summarized the main rheological studies performed on starch, including the
measurement technique and models used. A thermoplastic like behavior of low hydrated
starch, with an Arrhenius dependence on temperature and similar for moisture content was
reported. Conversely, structural modifications of starch, which affect the viscosity of the
product, are reflected differently by specific mechanical energy (SME), by the screw speed,
20
or even by the extruder barrel pressure, which depend on the machine characteristics. This
discrepancy underlines the need to ascertain the dependence of starch melt viscosity upon
Lai and Kokini (1990) studied the rheological properties of high amylose (70%)
and high amylopectin (98%) cornstarches, and showed the strong influence of the
Wang (1994) identified the contribution of shear and thermal energies in the conversion of
waxy cornstarch. Della Valle et al. (1994) took into account the starch transformation and
intrinsic viscosity, by confirming the importance of the term noted β. This latter is reported
in the following equation, which presents a pseudo-plastic model with the pseudo-plastic
index (m) and the consistency (K). The influence of SME on the degradation of starch
products was evaluated by intrinsic viscosity [η] measurements. The gradual decrease of [η]
with increasing SME confirmed that macromolecular degradation occurred (Martin et al.,
2000)
where MC is the moisture content; GC is the glycerol content; α, α’, and β, are
dimensionless coefficients.
needed to obtain a homogeneous molten starch phase prior to measurement. This material
2003). Both, mechanical energy and temperature are required to obtain a molten material to
appropriate for the study of rheological behavior of low moisture starches. In that respect,
extruder-fed slit rheometry is well adapted (Senouci and Smith, 1988; Bastioli et al., 1994).
Martin et. al. (2000) have also shown great interest in combining capillary and slit dyes on
21
(shear rate, SME, and temperature) comparable to those used during the processing.
Finally, starch molts are commonly considered to exhibit viscoelastic behavior. The
measurement of elastic components of PLS molten phases, associated with the first normal
stress difference (N1), is not trivial because conventional rheometers do not allow to
study using plane-plate geometry, PLS was shown to behave mainly as a solid-like material,
alternative, Senouci and Smith (1988) related the entrance and exit pressure losses in a slit
viscometer dye to the elastic properties of potato starch-based materials. Entrance and exit
pressure effects have been also used to evaluate the elasticity of melt of plasticized wheat
starch.
1.8.8 Plasticizers
Occasionally they are used only to facilitate the processing of a polymer and are not meant
used so that it will evaporate once the final product is produced (Daniels, 1989). The smell
associated with new plastic is often caused by volatile plasticizers (Rosen, 1982).
polymer and interfere with the chain-chain secondary bonding (Nolan-ITU Pty, 2002). This
interference reduces inter-chain bonding strength and allows the chain segments greater
plasticizer is chosen for its solubility in the polymer, since a soluble plasticizer can
penetrate the polymer more easily than a non-soluble one. Plasticizers can also be of the
non-soluble type and merely mechanically dispersed throughout the polymer (Daniels,
1989).
Most liquid plasticizer are low molecular weight organic materials with a glass
transition temperature in the range of 125-225K. When this type of solvent as added to an
22
organic polymer the result is a weight averaging of the glass transition temperature between
that of polymer and that of plasticizer if they are miscible. The reduction of the glass
transition temperature of the polymer by the plasticizer under the above conditions is
ranging from 20% to 40% to the starch weight. The plasticizer content is directly related to
the mechanical properties and glassy transition of the material (Vilpoux and Averous,
2004).
the study, during the thermoplastic process, water in starch and other plasticizers play a
crucial role in that the plasticizer could form the hydrogen bonds with starch, taking the
place of the strong action between hydroxyl groups of starch molecules, plasticizing the
starch. In their study, formamide was first used as plasticizer, which thereby suppressed the
glycerol-plasticized thermoplastic starch. When urea was introduced, the retrogradation and
In the said authors’ another study regarding the role of plasticizers in the properties
of thermoplastic starch, they have emphasized the role of hydrogen bonding in the
groups were used. Such compounds were believed to form stronger hydrogen bonds with
the hydrogen in C-O-H bonds of starch, contrary to the belief that the oxygen
23
in such starch bonds would form hydrogen bonds with the plasticizers (Ma and Yu, 2004-
b).
thermoplastic starch blends have reported success. Results of the study have indicated that
both tensile strength and elongation of the blends decreased as the starch content increased.
Zhai et al. (2003) incorporated polyvinyl alcohol (PVA) in corn starch-based sheets under
successful, and were in fact patented in the United States of America as sausage casings and
food package from thermoplastic corn starch, with infusion of certain cross-linking agents
far, but esterification processes to alter the flexibility of gelatinized sago starch have been
done. A study by Igura et al. (2007) have reported that esterified sago starch extraction
residue containing a sizeable starch portion have been converted to biodegradable plant pots
Jeroen et al. (1995) have stated that thermoplastic starch materials have been
native starches with the addition of glycerol as plasticizer. Nonetheless, in a recent study,
Thunwall et al. (2007) have established the possible routes for film blowing thermoplastic
glycerol, and moisture content. However, difficulties such as sticky film surface formation,
It has been observed that sago starch materials plasticized with glycerol pose a
significant vulnerability to moisture. To address this, Carvalho et al. (2005) have treated
films with isocyanates, epoxy functions, and stearoyl chloride to lessen their sensitivity to
24
moisture. The results have showed that, in all instances, the polar contribution in the films
was considerably reduced, indicating the increase in surface hydrophobicity of the films.
In a study by Sitohy and Ramadan (2001), thermoplastic films were prepared from
Using a method by Fishman et al. (1996), films were cut into squares from a thin layer
plate, and were submerged in water at 25C that was continually stirred. It was found out
that the phosphorylated starches were easily disintegrated than the non-phosphorylated
Using a method by Fishman et al. (1996), films were cut into squares from a thin
layer plate, and were submerged in water at 25 degrees Celsius that was continually stirred.
It was found out that the phosphorylated starches were easily disintegrated than the non-