NZ626602B2 - Biodegradable sheet - Google Patents
Biodegradable sheet Download PDFInfo
- Publication number
- NZ626602B2 NZ626602B2 NZ626602A NZ62660212A NZ626602B2 NZ 626602 B2 NZ626602 B2 NZ 626602B2 NZ 626602 A NZ626602 A NZ 626602A NZ 62660212 A NZ62660212 A NZ 62660212A NZ 626602 B2 NZ626602 B2 NZ 626602B2
- Authority
- NZ
- New Zealand
- Prior art keywords
- layer
- biodegradable
- sheet
- pbsa
- biodegradable sheet
- Prior art date
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Abstract
Disclosed is a biodegradable sheet comprising a gas barrier material of nanoclay (nano-kaolin) and/or polyvinyl alcohol (PVOH). The biodegradable films have low oxygen transmittance (OTR) and water transmittance (WVTR) and are suitable as packaging materials for long term storage of food or liquids. (...)
Description
BIODEGRADABLE SHEET
FIELD OF THE INVENTION
This invention is directed to a composition for biodegradable sheets sing a gas
barrier material. The invention relates to the use of nanoclays and/or PVOH as gas barriers.
OUND OF THE INVENTION
The use of radable materials has grown over the past years due to the
biodegradable materials’ environmentally friendly properties. The use of such materials is
read and includes various types of plastic bags, diapers, balloons and even sunscreen. In
response to the demand for more environmentally friendly packaging materials, a number of
new biopolymers have been developed that have been shown to biodegrade when discarded into
the environment. Some of the larger players in the biodegradable plastics market include such
well-known chemical companies as DuPont, BASF, Cargill-Dow Polymers, Union Carbide,
Bayer, Monsanto, Mitsui and n Chemical. Each of these companies has developed one or
more classes or types of biopolymers. For example, both BASF and Eastman Chemical have
developed biopolymers known as "aliphatic-aromatic" copolymers, sold under the trade names
ECOFLEX and EASTAR BIO, tively. Bayer has developed polyesteramides under the
trade name BAK. Du Pont has developed BIOMAX, a modified polyethylene terephthalate
(PET). Cargill—Dow has sold a variety of biopolymers based on polylactic acid (PLA). Monsanto
ped a class of polymers known as polyhydroxyalkanoates (PHA), which include
polyhydroxybutyrates (PHB), polyhydroxyvalerates (PHV), and polyhydroxybutyrate-
hydroxyvalerate copolymers (PHBV). Union Carbide ctures polycaprolactone (PCL)
under the trade name TONE.
Each of the foregoing biopolymers has unique properties, benefits and weaknesses. For
e, biopolymers such as BIOMAX, BAK, PHB and PLA tend to be strong but are also
quite rigid or even brittle. This makes them poor candidates when flexible sheets or films are
desired, such as for use in making wraps, bags and other packaging materials requiring good
bend and g capability. In the case of BIOMAX, DuPont does not presently e
specifications or conditions suitable for blowing films therefrom, thus indicating that it may not
be presently believed that films can be blown from BIOMAX and similar polymers.
On the other hand, biopolymers such as PHBV, ECOFLEX and EASTAR BIO are
many times more flexible compared to the more rigid biopolymers sed above. However,
they have relatively low melting points such that they tend to be self adhering and unstable when
'JI0525
newly processed and/or exposed to heat. To prevent self-adhesion (or ”blocking") of such films,
it is typically necessary to incorporate a small amount (e.g. 0.15% by weight) of silica, talc or
other fillers.
Further, due to the limited number of biodegradable polymers, it is often difficult, or
even impossible, to identify one single polymer or copolymcr that meets all, or even most, of the
desired performance criteria for a given application. For these and other reasons, biodegradable
polymers are not as widely used in the area of food ing materials, particularly in the field
ofliquid receptacles, as desired for ical s.
In addition, the biodegradable sheets known today are mostly opaque, having low light
transmittance and high haze. Further, the known biodegradable sheets either do not include
barriers or include amounts and types of barriers that cause the sheets to be generally highly
ble to gases, having both a high oxygen transmission rate and a high water vapor
transmission rate, and thus they cannot serve as long term food or drink receptacles.
Additionally, the physical strength of known biodegradable sheets, measured by ters
such as stress at maximum load, strain at break and Young’s Modulus, is lacking and, therefore,
is deficient when used as packaging, particularly when it is ble to package liquids.
Therefore, there is a need in the art for a biodegradable sheet that is ally strong,
though flexible, and r, has low gas permeability, a high light transmittance and low
haze. Such a biodegradable sheet could be used as a long term receptacle.
Further, although many liquid receptacles are used in the food and drink industry,
biodegradable receptacles are not widely used. United States Patent No. 6,422,753 discloses a
separable beverage receptacle packaging for potable and freezable liquids, wherein the
packaging comprises a plurality of individual ge receptacle units aligned in a side by
side n relative to one another. Each beverage receptacle unit has an interior fluid
r defined by a lower heat weld, an upper heat weld and two vertical heat welds that
are formed on opposed sheets of plastic. The heat welds between the intermediate beverage
receptacle units are provided with ated strips and the upper end of each receptacle unit
is provided with an upper horizontal heat weld disposed above a tapered crimp with a gap
that defines an integral drinking solubility spout when the tear strip above the perforated line
is removed from the individual beverage receptacle units. r, this packaging is not
environmental ly.
United States Patent No. 5,756,194 discloses water—resistant starch products useful in
the food industry that comprise an inner core of gelatinized starch, an intermediate layer of
natural resin and an outer layer of water resistant biodegradable polyester. The gelatinized
PCT/ILZOlZ/OSOSZS
starch can be made resistant by coating with biodegradable polyesters such as
poly(beta-hydroxybutyrate-co-valerate) (PHBV), poly(laetie acid) (PLA), and poly(.di-elect
caprolactone) (PCL). Adherence ofthe two dissimilar materials is achieved through the
use of an intervening layer of a resinous al such as shellac or rosin which possesses a
solubility parameter (hydrophobicity) intermediate to that of the starch and the polyesters.
Coating is achieved by spraying an alcoholic solution of the shellac or rosin onto the starch-
based article and subsequently coating with a on of the polyester in an appropriate
solvent. However, these products are not optimally designed for allowing a user to carry them
easily while being in a physical activity. In addition, they are not designed to provide
different liquid volumes that can be consumed according to instant needs.
All of the aforementioned prior art constructions are deficient with t to their
failure to provide a simple, efficient, and practical packaging arrangement for liquids that will
provide the user with easy access to flexible compartmented packaging for liquids.
uently, there is a need for a new and improved type of a biodegradable liquid
acle.
SUMMARY OF THE INVENTION
One embodiment of the invention is ed to a biodegradable sheet comprising a
gas barrier al. According to some ments, the gas barrier material is a nanoclay,
according to other embodiments, the gas barrier material is polyvinyl alcohol (PVOI—l), and
according to further embodiments, the gas barrier material is a combination of a nanoclay and
PVOH.
Another embodiment of the invention is directed to a receptacle unit ed from a
biodegradable sheet that ses a gas barrier material, wherein the receptacle unit
comprises a compartment for storing liquids and a means by which the liquids are removed
rom. According to some embodiments, the receptacle unit comprises a hanger.
BRIEF DESCRIPTION OF THE GS
The above and other characteristics and advantages of the invention will be better
understood through the following illustrative and non-limitative detailed description of
preferred embodiments thereof, with reference to the appended drawings, wherein:
Fig. 1 illustrates the construction of an array of receptacle units of different volume,
according to an embodiment of the invention;
PCT/ILZOlZ/OSOSZS
Fig. 2A illustrates the layout ofa single receptacle units, according to an embodiment
of the invention;
[00l6] Figs. 2B and 2C illustrate using a single receptacle units, according to another
embodiment of the invention;
Fig. 2D illustrates the layout of an internal straw segment, according to an
embodiment ofthe invention;
Fig. 2E illustrates a sectional view of a sealed internal straw segment, according
to an embodiment of the invention;
Figs. 3A to 3F rate the layout of an array of six acle units, ing to an
embodiment of the invention;
Figs. 4A to 4C illustrate the layout ofa single receptacle units with a mating cover,
according to another embodiment of the invention;
Fig. 4D is a cross-sectional view of the top cover sealing arrangement, according to
another embodiment of the invention;
[0022] Figs. 5A and 5B illustrate the layout of a single receptacle units with a pivotally
foldable straw, ing to another embodiment ofthe invention;
Figs. 6A-D illustrate an array of four receptacle units, according to an embodiment of
the ion, wherein all of the receptacle units are closed (, Fig. 6A is an overview of the
array, Fig. 6B is a front view ofthe array, Fig. 6C is a side view ofthe array and Fig. 6D is a
top view of the array);
Figs. 7A-D illustrate an array of four receptacle units, according to an embodiment of
the invention, wherein all of the receptacle units are opened (Fig. 7A is an overview of the
array, Fig. 7B is a front view ofthe array, Fig. 7C is a side View of the array and Fig. 7D is a
top view ofthe array); and
Figure 8 is a graph g the radability of a three layered sheet prepared
ing to an embodiment of the invention.
DETAILED DESCRIPTION OF THE INVENTION
In the following detailed description, us specific details are set forth in order to
provide a thorough understanding of the invention. However, it will be understood by those
skilled in the art that the present invention may be practiced without these specific details. In
other instances, well-known methods, procedures, and components have not been described in
detail so as not to obscure the present invention.
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The term “biodegradable” as used herein is to be understood to include any polymers
that degrade through the action of living organisms, light, air, water or any combinations thereof
Such biodegradable polymers include various synthetic polymers, such as polyesters, ter
amides, polycarbonates, etc. Naturally—derived semi—synthetic ters (e.g., from
fermentation) may also be included in the term “biodegradable”. Biodegradation ons are
typically enzyme-catalyzed and generally occur in the presence of moisture. l
macromolecules containing hydrolyzable linkages, such as protein, cellulose and starch, are
generally susceptible to biodegradation by the hydrolytic enzymes of microorganisms. A few
man-made polymers, r, are also biodegradable. The hydrophilic/hydrophobic character
of polymers greatly affects their biodegradability, with more polar polymers being more readily
biodegradable as a general rule. Other important polymer characteristics that affect
biodegradability include crystallinity, chain flexibility and chain length.
The term “sheet” as used herein is to be understood as having its customary meanings as
used in the thermoplastic and packaging arts. The biodegradable compositions according to the
ion can be used to manufacture a wide variety of articles of manufacture, including
articles useful to e solid and liquid substances, including food substances. Thus, the
sheets according to this invention include sheets having a wide variety of thicknesses (both
measured and ated).
The term “about” as used herein is to be understood to refer to a 10% deviation in the
value related to.
The terms cle” or "particulate filler" should be interpreted broadly to e filler
particles having any of a variety of different shapes and aspect ratios. In general, ”particles" are
those solids having an aspect ratio (i.e., the ratio of length to thickness) of less than about 10:1.
Solids having an aspect ratio r than about 10:1 may be better understood as "fibers", as
that term will be d and discussed hereinbelow.
The term “fibers” should be interpreted as a solid having an aspect ratio greater than at
least about 10:1. Therefore, fibers are better able to impart strength and toughness than
particulate fillers. As used herein, the terms "fibers" and "fibrous material" include both
inorganic fibers and organic fibers.
Besides being able to biodegrade, it is often important for a polymer or r blend to
exhibit certain physical properties. The intended application of a particular polymer blend will
often dictate which properties are ary in order for a particular polymer blend, or article
manufactured there from, to exhibit the desired performance criteria. When relating to
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radable sheets for use as packaging als, particularly as liquid receptacles, desired
performance criteria may include strain at break, Young’s modulus and stress at maximum load.
In order to define the physical properties ofthe biodegradable sheets ofthis invention,
several measurements were used. Stress at m load, Young’s Modulus and the strain at
break were measured using the ASTM D882-10 Standard Test Method for Tensile Properties
of Thin Plastic Sheeting. The light transmittance and the haze were measured using the
ASTM D1003 - 07el Standard Test Method for Haze and Luminous Transmittance of
Transparent Plastics. The oxygen permeability of the radable sheets was measured
using the ASTM D3985 - 05(2010)e1 rd Test Method for Oxygen Gas Transmission
Rate Through Plastic Film and Sheeting Using a Coulometric . The water vapor
bility of the biodegradable sheets of the ion was measured using the ASTM
E398 — 03(2009)el Standard Test Method for Water Vapor Transmission Rate of Sheet
Materials Using Dynamic Relative Humidity Measurement.
In an embodiment of the invention, this invention provides a biodegradable sheet
having a stress at maximum load of at least 15 Mpa. According to other embodiments, this
invention provides a biodegradable sheet having a stress at maximum load of at least 30 Mpa.
According to some embodiments of the invention, the stress at maximum load is in the range
of 15-50 Mpa. According to some embodiments of the invention, the stress at maximum load
is in the range of 15-20 Mpa. According to some embodiments of the invention, the stress at
maximum load is in the range of 20—25 Mpa. ing to some embodiments of the
invention, the stress at maximum load is in the range of 25-30 Mpa. According to some
embodiments of the invention, the stress at maximum load is in the range of 30-35 Mpa.
According to some embodiments of the invention, the stress at maximum load is in the range
of35-40 Mpa. According to some embodiments of the invention, the stress at maximum load
is in the range of 40-45 Mpa. According to some embodiments of the invention, the stress at
maximum load is in the range of 45-50 Mpa. According to further embodiments of the
ion, the stress at maximum load is in the range of 24-26 Mpa. According to further
embodiments of the ion, the stress at m load is in the range of 46-48 Mpa.
According to further embodiments of the invention, the stress at maximum load is in the
range of 32-34 Mpa. According to some embodiments of the invention, the stress at
maximum load is in the range of 19-21 Mpa. According to some ments of the
invention, the stress at maximum load is in the range of 29—31 Mpa.
The biodegradable sheet of this invention has a strain at break of at least 280%.
According to further embodiments, the strain at break is at least 300%. According to some
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embodiments, the strain at break is in the range of 400—600%. According to some
embodiments, the strain at break is in the range of 280—850%. According to some
embodiments, the strain at break is in the range of 280-350%. According to further
embodiments, the strain at break is in the range of 350-450%. According to further
embodiments, the strain at break is in the range of 450-550%. According to further
embodiments, the strain at break is in the range of 550-650%. ing to further
embodiments, the strain at break is in the range of 650-750%. According to further
embodiments, the strain at break is in the range of 750-850%. According to further
ments, the strain at break is in the range of 410-420%. According to further
embodiments, the strain at break is in the range of 725-735%. According to further
embodiments, the strain at break is in the range of 575-585%. ing to r
embodiments, the strain at break is in the range of SSS-565%. According to further
embodiments, the strain at break is in the range of 615-625%.
The Young‘s Modulus of the biodegradable sheet of this invention is at least 200
Mpa. ing to some embodiments of the invention, Young’s Modulus is in the range of
200-800Mpa. According to further ments of the invention, Young’s Modulus is in the
range of 400—600 Mpa. ing to further embodiments, Young’s s is in the range
of 300-350 Mpa. According to further embodiments, s Modulus is in the range of
350—400 Mpa. According to further ments, Young’s Modulus is in the range of 400—
450 Mpa. According to further embodiments, Young’s Modulus is in the range of 0
Mpa. According to further embodiments, Young’s Modulus is in the range of 500-550 \/lpa.
According to further embodiments, Young‘s Vlodulus is in the range of 550—600 lea.
According to further embodiments, Young’s Vlodulus is in the range of 600—650 lea.
According to further ments, Young‘s us is in the range of 650-700 lea.
According to r embodiments, Young‘s Vlodulus is in the range of 700—750 lea.
According to further embodiments, Young’s Vlodulus is in the range of 750-800 lea.
According to further embodiments, Young‘s Vlodulus is in the range of 5 lea.
According to further embodiments, Young’s Vlodulus is in the range of 565—575 lea.
According to further embodiments, Young‘s Vlodulus is in the range of 600-610 lea.
According to further embodiments, Young’s Vlodulus is in the range of 670—680 lea.
According to r embodiments, Young’s Modulus is in the range of385-395 Mpa.
According to some embodiments of the invention, the light transmittance of the
biodegradable sheet of the invention is at least 75%. According to further embodiments, the
light transmittance is in the range of 75-95%. According to further embodiments, the light
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transmittance is in the range of 75-80%. According to further ments, the light
transmittance is in the range of 80-85%. According to r embodiments, the light
transmittance is in the range of 85-90%. According to further embodiments, the light
transmittance is in the range of 90-95%. According to further embodiments, the light
transmittance is above 95%.
According to some embodiments of the invention, the oxygen transmission rate ofthe
biodegradable sheet of the invention is lower than 8500 cc/m2/24 hours. According to further
embodiments, the oxygen transmission rate is in the range of 0 ec/m2/24 hours.
According to further embodiments, the oxygen ission rate is in the range of 100-1000
cc/m2/24 hours. According to further ments, the oxygen transmission rate is in the
range of 1000-2000 cc/m2/24 hours. According to further embodiments, the oxygen
transmission rate is in the range of 2000—3000 ec/m2/24 hours. According to further
embodiments, the oxygen transmission rate is in the range of 3000-4000 cc/m2/24 hours.
According to further embodiments, the oxygen transmission rate is in the range of 4000—5000
cc/m2/24 hours. According to further embodiments, the oxygen transmission rate is in the
range of 5000-6000 cc/m2/24 hours. According to further embodiments, the oxygen
transmission rate is in the range of 6000—7000 cc/m2/24 hours. According to further
embodiments, the oxygen transmission rate is in the range of 7000-8000 cc/m2/24 hours.
According to some embodiments of the invention, the water vapor transmission rate
of the biodegradable sheet of the invention is lower than 30gr/m2/day. According to further
embodiments of the invention, the water vapor transmission rate is lower than 20gr/m2/day.
According to further embodiments, the water vapor transmission rate is in the range of 15—
20gr/n12/day. According to r embodiments, the water vapor transmission rate is in the
range of 20-25gr/m2/day. According to further embodiments, the water vapor transmission
rate is in the range of 25—30gr/m2/day.
The invention is further directed to a biodegradable sheet comprising any riate
amounts of any appropriate biodegradable polymers, capable of providing the biodegradable
sheet with the d physical properties, as ed above. According to some
embodiments, the biodegradable sheet of the invention is recyclable, i.e., the material from
which it is prepared may be reused (after appropriate ent, i.e., ng when necessary,
grinding, heating, etc.) to prepare additional articles of cture.
According to r embodiments, the biodegradable sheet of the invention is
compostable.
According to some embodiments, the biodegradable sheet comprises synthetic
polyesters, semi—synthetic polyesters made by fermentation (e.g., PHB and PHBV), polyester
amides, polycarbonates, and polyester urethanes. In other embodiments the biodegradable
sheet of the invention includes at least one of a variety of natural polymers and their
derivatives, such as polymers comprising or derived from , cellulose, other
polysaccharides and proteins.
According to some embodiments, the biodegradable sheet ses polylactic acids
(PLA) or derivatives f related to as CPLA, polybutylene suecinate (PBS), polybutylene
suecinate adipate (PBSA), polyethylene suecinate (PES), poly(tetramethylene-adipate-
coterephthalate (PTAT), polyhydrozyalkanoates (PHA), poly(butylene adipate-coterephthalate
, thermoplastic starch (TPS), polyhydroxyburates (PHB),
polyhydroxyvalerates (PHV), polyhydroxybutyrate-hydroxyvalerate copolymers (PHBV),
polycaprolactone (PCL), x®, an aliphatic-aromatic mer, Eastar Bio®, another
aliphatic-aromatic copolymer, BaktR) comprising polesteramides, Biomax<R>, which is a
modified polyethylene terephathalate, novamont®, or any combination thereof.
According to some embodiments, the biodegradable sheet comprises ctic acids
(PLA) or derivatives thereof related to as CPLA and/or tylene suecinate (PBS)
together with any one of tylene suecinate adipate (PBSA), polyethylene suecinate
(PES), poly(tetramethylene-adipate-coterephthalate (PTAT), polyhydrozyalkanoates (PHA),
poly(butylene adipate—co-terephthalate (PBAT), thermoplastic starch (TPS),
polyhydroxyburates (PHB), droxyvalerates (PHV), polyhydroxybutyratehydroxyvalerate
copolymers (PHBV), polycaprolactone (PCL), ecoflextR), an aliphatic—
aromatic mer, Eastar Bio®, another aliphatic-aromatic copolymer, Bak® comprising
polesteramides, Biomaxtli), which is a ed polyethylene terephathalate, novamont®, or
any combination thereof.
According to some embodiments, the PLA is a homopolymer. According to further
embodiments, the PLA is copolymerized with glycolides, lactones or other monomers. One
ularly attractive feature of sed polymers is that they are derived from ble
agricultural products. Further, since lactic acid has an asymmetric carbon atom, it exists in
several isomeric forms. The PLA used according to some ments of the invention
includes poly-L-lactide, poly-D-lactide, poly-DL-lactide or any combination thereof.
According to some embodiments, the biodegradable sheet of the invention further
comprises any appropriate additives. According to one embodiment, the additive softens the
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biodegradable polymer. The softeners used may be selected from the group comprising
paraloid®, sukano®, tributyl acetyl citrate (A4®) or any combination thereof.
ing to some embodiments, the biodegradable sheet of the invention ses
at least one nanoclay and/or at least one nano-composite. The addition of the nanoclay and/or
the nano—eomposite lowers the water vapor ission rate and the oxygen transmission
rate of the biodegradable sheet of the ion, thus acting as barriers in the sheet. Further,
according to certain embodiments of this invention, the nanoclays and the nano-eomposites
added to the biodegradable sheet are naturally occurring materials, and therefore, the sheets
remain biodegradable. According to one embodiment, montmorillonite, vermiculite or any
combination thereof are added to the composition of the biodegradable sheet.
According to one embodiment, nanoclays based on montmorrilonite with polar
philie based surface treatment and/or nanoclays based on vermiculite, heat treated and
polar organophilie base surface treated are added to the biodegradable composition in order
to create a well dispersed material. According to one ment, the nanoclay based gas
barrier is dispersed in the bulk of the biodegradable composition, preferably added during the
melt compounding process. The sment of nanoclay platelets creates a tortuous path in
the bulk of the composition, thus leading to a reduction in gas permeation rates though the
biodegradable sheet produced. According to another embodiment, the nanoclay based gas
r is implemented as an internal gas barrier layer in a ayer biodegradable sheet,
wherein the barrier layer reduces the gas permeation rate.
According to one embodiment, the nanoclay added to the biodegradable sheet creates
a tortuous structure that resists the penetration of moisture, oil, grease and gases, such as
oxygen, nitrogen and carbon dioxide. According to one embodiment of the invention, the
nanoclay is based on nano-kaolin. According to another embodiment, the nanoclay added to
the biodegradable sheet is based on bentonite, which is an absorbent aluminium
phyllosilicate. According to one embodiment, the nanoclay is based on CloisitetR). According
to one embodiment, a mixture of any appropriate nanoclays may be added to the
biodegradable sheet.
According to one embodiment, the nanoclay is dispersed in the bulk of the
biodegradable composition, resulting in the dispersment of the ay in at least one layer
of the biodegradable sheet. According to some ments, the nanoclay is added during
the melt compounding process. According to another embodiment, the ay is added to
the biodegradable sheet in a separate layer, together with a biodegradable polymer, thus
forming a omposite layer. ing to one embodiment, the nanoclay layer in the
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multilayer biodegradable sheet is an internal layer, i.e., is not d to the outside
atmosphere.
According to one embodiment, the nanoclay is dispersed in the bulk of the
biodegradable composition, forming a neus dispersion, using polymer conjugation to
the nano clay e. In an embodiment of the invention, the nanoclay particles contain
siloxy and hydroxyl groups, and are used as a functional anchoring between the inorganic
nanoclay particle and the organic polymer. According to some embodiments of the invention,
the polymer can be conjugated using a hertobifunctional molecule, such as, isocyanatoproyl
oxy silane, where the ethoxysilane condensate to form silicone bonding to the nanoclay
surface, and the isocyanate group r react with the hydroxyl or amine group of the
polymer.
According to some embodiments of the invention the nanoclay particles are exfoliated
using 3-(Dimethylamino)propylamine (DMPA), where the tertiary amine, is conjugated to
the hydroxyls on the surface, and the primary amine is free for further reaction. In the next
step, a bifunctional nate such as Hexamethylene diisocyanate (HDI), methylene
diphenyl diisocyanate (MDI) or toluene diisocyanate (TDI), can conjugate to the amine on
the nanoclay surface, g urethane linkage, and the other free isocyanate can further
react we the r hydroxyl end group.
According to some ments of the invention, the nanoclay hydroxyl groups are
used as nucleation sites for ring g polymerization, which are further reacted to open
es, such as, L-lactide, D-lactide, D,L-lactide and epsilon-caprolacton. The polymer
conjugation to the nanoclay surface form polymer brushes perpendicular to the nanoclay
particle surface; contribute to stable exfoliation of the particles, as well as to homogeneous
particles sion through r processing, by extrusion.
According to one embodiment, the amount of the nanoclay is about 20—30% w/W of
the nano-composite layer. According to one embodiment, the amount of the nanoclay is about
—20% W/W of the omposite layer. According to one embodiment, the amount of the
nanoclay is about 10—15% w/w of the nano—composite layer. According to one embodiment,
the amount of the nanoclay is about 5-10% w/w of the nano-composite layer. According to
one embodiment, the amount of the nanoclay is about 1-5% w/w of the nano-composite layer.
According to one embodiment, the amount of the nanoclay is less than about 20% w/w of the
nano—composite layer. According to one embodiment, the amount of the nanoclay is less than
about 15% w/w of the nano-composite layer.
According to one ment, the biodegradable sheet of the invention includes at
least one external layer that is a multilayer laminate, based on biodegradable blends.
According to further embodiments, the biodegradable sheet of the invention includes at least
one internal biodegradable nanocomposite layer. According to some embodiments, the
biodegradable sheet includes at least one al core layer of a gas barrier material, such as
polyvinyl alcohol (PVOH). According to some embodiments, the biodegradable sheet
es two or more al core layers of a gas barrier material, such as PVOH. A highly
polar gas r material, such as PVOH, exhibits weak interaction with low polarity gases,
such as oxygen and carbon dioxide, which, together with the crystalline regions in the sheet,
reduce the permeability rate of gases through the sheet.
According to some embodiments of the invention, the biodegradable sheet includes
PVOH and a nanoclay dispersed in one or more of the layers as described above.
According to some embodiments, the biodegradable sheet comprises an al
laminate layer, an internal nanocomposite layer and an internal core layer. Such a
biodegradable sheet provides low permeability rate of gases.
According to one embodiment, a compatibilizer is added to the biodegradable sheet.
The compatibilizer is added in order to enhance the on between the different layers of
the multilayer biodegradable sheet. According to one embodiment, the ibilizer is
based on PBSA grafted with maleic ide, which is a monomer known for grafting used
mainly for modifying efins. According to one embodiment, the PBSA is grafted with
the maleic anhydride in a twin-screw extruder, using a continuous flow of nitrogen.
According to one embodiment the grafting is ted by an initiator, such as dieumyl
peroxide, benzoyl de and 2,2-azobis(isobutyronitrile). According to one embodiment, a
mixture of PBSA, about 3% maleic anhydride and about 1% dicumyl peroxide is extruded in
order to obtain PBSA grafted with maleic anhydrideanhydride.
According to one embodiment, a mixture of PVOH, about 1% maleic anhydride and
about 0.3% 2,2—azobis(isobutyronitrile) is extruded in order to obtain PVOH grafted with
maleic anhydride. According to one embodiment, a mixture of PVOH, about 0.5% maleic
anhydride and about 0.1% 2,2-azobis(isobutyronitri1e) is extruded in order to obtain PVOH
grafted with maleic anhydride.
According to one embodiment, a mixture of PVOH with highly branched PBS and
about 1% maleic anhydride and about 0.3% 2,2—azobis(isobutyronitri1e) is extruded in order
to obtain PVOH grafted with maleic anhydride, nd with PBS. According to one
embodiment, a e of PVOH with highly branched PBS and about 0.5% maleic
PCT/ILZOIZ/OSOSZS
anhydride and about 0.1% 2,2-azobis(isobutyronitrile) is ed in order to obtain PVOH
d with maleic anhydride compound with PBS.
ing to one embodiment, the amount of compatibilizer added to the PBSA layer
is up to 10% w/w. According to one embodiment, the amount of compatibilizer added to the
PBSA layer is up to 5% w/w. According to another embodiment, the amount of ibilier
added to the PBSA layer is up to 4%. According to r embodiment, the amount of
compatibilier added to the PBSA layer is up to 3%. According to another embodiment, the
amount of compatibilier added to the PBSA layer is up to 2%. According to another
embodiment, the amount of compatibilier added to the PBSA layer is up to 1%. According to
another embodiment, the amount of compatibilier added to the PBSA layer is in the range of
2-4%.
According to one embodiment, the amount of compatibilizer added to the PVOH
layer is up to 10% w/w. According to one embodiment, the amount of compatibilizer added
to the PVOH layer is up to 5% w/w. According to another embodiment, the amount of
compatibilier added to the PVOH layer is up to 4%. According to another embodiment, the
amount of compatibilier added to the PVOH layer is up to 3%. ing to r
embodiment, the amount of compatibilier added to the PVOH layer is up to 2%. According to
another embodiment, the amount of compatibilier added to the PVOH layer is up to 100.
According to another embodiment, the amount of compatibilier added to the PVOH layer is
in the range of 2—40 0.
According to some embodiments, the biodegradable sheet of the invention further
comprises nic particulate s, fibers, organic fillers or any combination thereof, in order
to decrease self—adhesion, lower the cost, and increase the modulus of elasticity (Young's
modulus) ofthe polymer blends.
Examples of nic particulate flllers include crushed rock, bauxite, granite,
, gravel,
limestone, sandstone, glass beads, aerogels, xerogels, mica, clay, alumina, silica, kaolin,
microspheres, hollow glass spheres, porous c spheres, gypsum ate, insoluble salts,
calcium carbonate, magnesium carbonate, calcium hydroxide, m aluminatc, ium
carbonate, titanium dioxide, talc, ceramic materials, pozzolanic materials, salts, zirconium
compounds, xonotlite (a crystalline calcium silicate gel), lightweight expanded clays, perlite,
vermiculite, hydrated or ated hydraulic cement particles, pumice, zeolites, exfoliated
rock, ores, minerals, and other geologic materials. A wide variety of other inorganic fillers may
be added to the polymer blends, including materials such as metals and metal alloys (e.g.,
stainless steel, iron, and copper), balls or hollow spherical materials (such as glass, polymers,
PCT/ILZOIZ/OSOUI25
and metals), filings, pellets, flakes and powders (such as microsilica) as well as any combination
thereof.
Examples of organic fillers include seagel, cork, seeds, gelatins, wood fiour, saw dust,
milled polymeric materials, ased materials, native starch granules, pregelatinized and
dried starch, expandable particles, as well as ation f. Organic fillers may also
include one or more appropriate synthetic polymers.
Fibers may be added to the moldable mixture to increase the lity, ductility,
bendability, cohesion, elongation ability, deflection ability, toughness, and re energy, as
well as the flexural and tensile strengths of the resulting sheets and articles. Fibers that may be
incorporated into the polymer blends include naturally occurring c fibers, such as
cellulosic fibers extracted from wood, plant leaves, and plant stems. In addition, inorganic fibers
made from glass, graphite, , ceramic, rock wool, or metal materials may also be used.
Preferred fibers include cotton, wood fibers (both hardwood or softwood fibers, examples of
which include rn hardwood and southern pine), flax, abaca, sisal, ramie, hemp, and
bagasse because they readily decompose under normal ions. Even recycled paper fibers
can be used in many cases and are extremely inexpensive and plentiful. The fibers may include
one or more filaments, fabrics, mesh or mats, and which may be ruded, or otherwise
blended with or impregnated into, the polymer blends of the present invention.
According to further embodiments, plasticizers may be added to impart desired
softening and elongation properties as well as to improve processing, such as extrusion.
al plasticizers that may be used in accordance with the present invention include, but
are not limited to, soybean oil caster oil, TWEEN 20, TWEEN 40, TWEEN 60, TWEEN 80,
TWEEN 85, sorbitan monolaurate, sorbitan monooleate, sorbitan lmitate, sorbitan
trioleate, sorbitan monostearate, PEG, derivatives of PEG, N,N-ethylene bis-stearamide, N,N—
ethylene bis-oleamide, polymeric plasticizers such as poly(l,6-hexamethylene adipate), and
other compatible low lar weight polymers.
According to some embodiments, lubricants, such as salts of fatty acids, e.g.,
magnesium stearate, may also be incorporated into the biodegradable sheets of the invention.
According to additional embodiments, the radable sheets of this invention may
be embossed, crimped, d or otherwise textured to improve their physical properties.
The biodegradable sheet of this invention is composed of any appropriate number of
layers. According to one embodiment, the biodegradable sheet of this invention ses
one layer. According to another embodiment, the biodegradable sheet of this invention
comprises two layers. According to another embodiment, the biodegradable sheet of this
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ion comprises three layers. According to another embodiment, the biodegradable sheet
of this invention ses four . According to another embodiment, the biodegradable
sheet ofthis invention comprises five layers.
According to some embodiments, the biodegradable sheets of this invention have any
desired thickness. According to some embodiments, the thickness of the sheets ranges from
-300 s. The measured thickness will typically be between 10-100% larger than the
ated thickness when the sheets are prepared from compositions that have a relatively
high concentration of particulate filler particles, which can protrude from the surface of the
sheet. This phenomenon is especially pronounced when significant quantities of filler
particles, having a particle size diameter that is larger than the thickness of the polymer
, are used.
According to some embodiments, the thickness of a one layer sheet is about 40—60
microns. According to some embodiments, the thickness of a one layer sheet is about 50
microns. According to some embodiments, the thickness of a three layer sheet is about 90—
110 microns. According to some embodiments, the thickness of a three layer sheet is about
100 microns. According to some ments, the biodegradable sheets of the invention
have a low haze.
The biodegradable sheet of this invention may be prepared using any appropriate
means. According to certain embodiments, the biodegradable polymers used according to this
invention are extruded (using mono or co—extrusion methods), blown, cast or otherwise
formed into sheets for use in a wide variety of packaging materials, or they may be molded
into shaped articles. ing to some embodiments, known , extrusion, blowing,
injection molding, and blow molding tus known in the thermoplastic art are suitable
for use in forming the biodegradable sheets of this invention. In an embodiment of the
invention, the sheet may be blown into various shapes including a shape of a bottle.
According to one embodiment of the ion, the biodegradable sheet is prepared by
compounding the raw biopolymers and possible additives and then preparing a sheet in a cast
extruder. Once the biodegradable sheet is prepared, it is post—treated by heat sealing,
according to some embodiments, to join two parts ofthe same sheet or two separate , in
order to prepare pockets, s etc. According to further embodiments, the biodegradable
sheets of this invention are coated with any riate coating, while ensuring that the end
product remains biodegradable.
According to further embodiments, the one d biodegradable sheet of the
invention comprises about 20% w/w PLA and about 80% w/w PBS. According to further
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embodiments, the biodegradable sheet of the invention comprises about 20% w/w PLA,
about 40% w/w PBS and about 40% w/w novamont CF. According to further embodiments,
the biodegradable sheet of the ion comprises about 33% w/w PLA, about 33% w/w
PBS and about 33% w/w Ecoflex.
According to further embodiments, the one layered radable sheet of the
invention consists of about 20% w/w PLA and about 80% w/w PBS. According to further
embodiments, the biodegradable sheet of the invention consists of about 20% w/w PLA,
about 40% w/w PBS and about 40% w/w novamont CF. According to further embodiments,
the radable sheet of the invention consists of about 33% w/w PLA, about 33% w/w
PBS and about 33% w/w Ecoflex.
According to further embodiments, the multi-layered biodegradable sheet of the
invention comprises the following three layers, wherein layer 2 is sandwiched n layers
1 and 3 so that layers 1 and 3 are on the e of the sheet, in direct contact with the outside
atmosphere, while layer 2 is oned between them:
Layer 1: comprising about 33.3% w/w PLA, 33.3% w/w PBS and 33.3% w/w Ecoflex;
Layer 2: sing about 100% w/w PHA; and
Layer 3: comprising about 33.3% w/w PLA, 33.3% w/w PBS and 33.3% w/w Ecoflex.
According to further embodiments, the multi-layered biodegradable sheet of the
invention comprises the following three layers:
Layer 1: comprising about 33.3% w/w PLA, 33.3% w/w PBSA and 33.3% w/w PBAT;
Layer 2: comprising about 100% w/w PBAT; and
Layer 3: comprising about 33.3% w/w PLA, 33.3% w/w PBSA and 33.3% w/w PBAT.
According to further embodiments, the multi—layered biodegradable sheet of the
ion consists the following three layers:
Layer 1: consisting about 33.3% w/w PLA, 33.3% w/w PBS and 33.3% w/w ;
Layer 2: consisting about 100% w/w PHA; and
Layer 3: consisting about 33.3% w/w PLA, 33.3% w/w PBS and 33.3% w/w Eeoflex.
According to further embodiments, the multi—layered biodegradable sheet of the
invention consists the following three layers:
Layer 1: consisting about 33.3% w/w PLA, 33.3% w/w PBSA and 33.3% w/w PBAT;
Layer 2: consisting about 100% w/w PBAT; and
Layer 3: consisting about 33.3% w/w PLA, 33.3% w/w PBSA and 33.3% w/w PBAT.
According to further ments, the monolayer biodegradable sheet consists of
about 75% PBSA and about 25% PLA. According to some embodiments embodiments, the
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multi-layered biodegradable sheet of the invention consists of the following three, five or
more layers. ing to some embodiments thc al layers consist of about 25% w/w
PLA and about 75% w/w PBSA. According to some embodiments, PVOH layer is included
as a core layer, sandwiched between the biodegradable polymer layers and any existing
nanocomposite . According to some cmbodiments, at lcast one layer consisting of
100% biodegradable polymers, e.g., PBSA is ed. According to some embodiments, the
biodegradable sheet includes at least one internal layer consisting of PBSA and about 10-15%
w/w nanoclays. According to some embodiments, the biodegradable sheet includes at least
one internal layer consisting of PBSA and about 5—10% w/w nanoclays. According to some
embodimcnts, thc biodegradable sheet includcs at lcast onc intcmal laycr consisting of PBSA
and about 0-5% w/w nanoclays. According to some embodiments, the radable sheet
includes at least one intcrnal laycr consisting of PBSA and about 15—20% w/w nanoclays.
ing to some ments, the biodegradable sheet includes at least one internal layer
consisting of PBSA and about 20—25% w/w nanoclays. According to further embodiments,
the PBSA may be replaced with any appropriate biodegradable polymer blend. According to
further embodiments, the multi-layered biodegradable sheet of the ion consists the
following threc laycrs:
Layer 1: consisting about 25% w/w PLA and about 75% w/w PBSA;
Layer 2: consisting about 100% w/w PBSA; and
Laycr 3: consisting about 25% w/w PLA and about 75% w/w PBSA.
According to further embodiments, the multi-layered radable sheet of the
invention consists the following three layers:
Layer 1: consisting about 75% w/w PLA and about 25% w/w PBSA;
Layer 2: consisting about 100% w/w PBSA; and
Laycr 3: consisting about 75% w/w PLA and about 25% w/w PBSA.
According to one ment, the thickness of all three layers is the same.
According to further embodiments, the multi—layered biodegradable sheet of the
ion consists the following five laycrs:
Layer 1: consisting about 25% w/w PLA and about 75% w/w PBSA;
Laycr 2: consisting about 100% w/w PBSA;
Layer 3: consisting about 100% w/w PVOH;
Layer 4: consisting about 100% w/w PBSA; and
Laycr 5: consisting about 25% w/w PLA and about 75% w/w PBSA.
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According to one embodiment, the ess of layers 1 and 5 is about 30% of the
total thickness of thc sheet, and the thickness of layers 2 and 4 is about 15% of the total
thickness ofthe sheet and the thickness oflayer 3 is about 10% of the total sheet.
According to further ments, the multi—layered biodegradable sheet of the
invention consists the following fivc layers:
Layer 1: ting about 25% w/w PLA and about 75% w/w PBSA;
Layer 2: consisting of about 90—85% PBSA and about 10—15% w/w nanoclays;
Layer 3: consisting of about 100% w/w PVOH;
Layer 4: consisting of about 90—85% PBSA and about 10—15% w/w nanoclays; and
Layer 5: consisting of about 25% w/w PLA and about 75% w/w PBSA.
Although c examples for mono-layered, three-layered and five-layered sheets
were given herein, embodimcnts of the invention are ed to biodegradable sheets
including any possible number of layers.
According to another embodiment, the biodegradable compositions of this invention
are suitable for injection molding. Injection molding is used according to this invention to
prepare any riate shape, including a means for removing liquid from a beverage
receptacle, such as a spout, a straw, an opening covered by a cap, etc. The physical and
mechanical properties of the injection moldcd biodegradable matcrial according to this
invention are as follows:
ic Gravity 1.0—1.5 ASTM D792
Melt volume rate (1900C/2.l6 kg) [ems/10 min] 3.0 — 8.0 ASTM D1238
Melt flow rate (190002.16 kg) [g/10 min] 4.0 4 9.0 ASTM D1238
Tensilc Strength & Brcak, (MPa) 30 - 50 ASTM D882
Tensile Modulus, (MPa) 800 - l200 ASTM D882
Tcnsilc Elongation, % 200 - 400 ASTM D882
According to some embodiments ofthe invention, the biodegradable ition that
is molded by injection is prepared from 75% PBSA and 25% PLA. The physical and
mechanical ties of this composition arc as s:
Specific Gravity 1.25 ASTM D792
Melt volumc rate (190°C/2.16 kg) [ems/10 min] 3.9 ASTM D1238
Melt flow rate (190°C/2.l6 kg) [g/10 min] 4.2 ASTM D1238
Tensile Strength (gt, Break, (MPa) 32 ASTM D882
Tcnsilc Modulus, (MPa) 894 ASTM D882
Tensile Elongation, % 339 ASTM D882
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The biodegradable sheet of the invention may be used for any ation requiring
such a sheet. According to one embodiment, the biodegradable sheet of the invention is used
in the preparation of a receptacle for liquids, including water, beverages and liquid food
matter.
According to one embodiment of the ion, there is provided a separable
beverage receptacle ing comprising a plurality of receptacle units possible of ent
volume, formed in a contiguous fashion, wherein each can be torn-off on demand. The
separable beverage receptacle packaging may be made from a biodegradable material. In an
embodiment of the invention, the separable beverage receptacle packaging is made from the
biodegradable sheet described herein. According to one ment, the receptacle units are
attached to one r in a side by side arrangement. According to another embodiment, the
receptacle units are attached to one another so that the bottom of one unit is attached to the
top of the other unit. According to further embodiments, the separable beverage receptacle
packaging of the present invention comprises a ity of receptacle units, any number of
which may have a different volume and shape. ing to further embodiments, at least
two of the acle units have a different volume. According to one embodiment, at least
one of the receptacle units is asymmetrical. According to further embodiments more than one
ofthe receptacle units is asymmetrical.
Each receptacle (e.g., a pouch, a bag or any other type of essentially flexible
receptacle) includes two sheets of flexible and sufficiently impermeable biodegradable
material, such as the biodegradable compositions detailed herein. ing to one
embodiment, the radable sheets are heat sealed along d lines to create the
individual receptacle units, which are separated from one another by a line of scored
perforations that allows the individual receptacle units to be physically separated from one
another. According to some embodiments, the perforation lines are adapted to provide
receptacle units with different volumes that correspond to the amount of s regularly
consumed by family members. According to one embodiment, the perforations between each
two acle units are such that once detached there is no wasted material, i.e., there is no
excess material found between the receptacle units that is not part of the receptacle unit itself
The plurality of receptacle units, which are connected to one another, is related to
herein as an array. The array of this invention comprises any number of receptacle units, any
number of which may be of different shape and/or volume. According to one embodiment,
the volume of each receptacle unit ranges from 100-500ml. According to a further
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embodiment, the volume of each receptacle unit ranges from 200-350ml. ing to one
embodiment, the shape of at least one acle unit is triangular. According to another
embodiment, the shape of at least one receptacle unit is pyramidal.
According to one embodiment, the array is terminated with a hanger for efficient
storage (sec, e.g., Figs. 6A—D and 7A—D). According to one ment, such a hanger is
formed as a round hole in the array. According to this invention, each receptacle unit includes
a compartment for storing liquids and a means for removing the liquids therefrom. The means
for removing the liquids from the compartment include a straw (see, e.g., Figs. 1, 2A-C, 6A-
D and 7A—D), a conduit (see, e.g., Figs. 3A—E), a spout, an opening covered by a cap (see,
c.g., Figs 3F and 4A), an opening closed by a stopper and a foldable unit that when ed
creates an opening through which s can exit the compartment (see, e.g., Figs 5A and
SB). According to some embodiments, the compartment does not comprise an opening; but
rather an opening is formed by the movement of an element, such as a cap, attached to the
compartment.
[0094] According to some embodiments, each receptacle unit comprises a tment for
storing liquid and a straw. According to one embodiment, the straw is hermetically
sandwiched n the sheets of the compartment in such a way that it has two segments, an
internal segment that is found inside the compartment and an external segment that is found
outside the compartment. According to r embodiments, each receptacle unit further
comprises a sealing edge for sealing the external segment of the straw that is also
hermetically sandwiched between the sheets of the sealing edge. According to some
embodiments, a perforated line is placed between the sealing edge and the compartment,
which perforated line s tearing off the sealing edge and exposing the external segment
of the straw.
According to one embodiment of the invention, the straw includes two opposing
members positioned between the external segment and the internal segment of the straw.
These members are attached to the biodegradable sheets of the receptacle unit, e.g., by heat
sealing them between the two sheets, which, ore, prevent movements of the straw as
well as leaks from around the straw. According to one embodiment, the members are tapered
to as to ease their attachment to the acle unit.
ing to further embodiments, the receptacle unit includes a compartment for
storing liquids and a conduit, through which the s may be d from the
compartment. According to one embodiment, the conduit is formed from a continuation of
the biodegradable sheets forming the compartment. According to one embodiment, the
WO 88443 UI25
conduit is sealed at the end, e.g., by heat, and comprises a perforated line, which aids in
opening the t and removing the liquids from the compartment, when desired.
According to one embodiment, the conduit is folded over when not in use. According to a
further ment, the conduit is ed to the side of the compartment when not in use.
ing to the invention, the acle units are attached to one another at any
appropriate location on each receptacle unit. According to one embodiment of the invention,
the receptacle units are attached to one another in a side by side fashion, wherein the opening
of each unit is positioned in any appropriate ion. According to one embodiment, the
g of each receptacle unit is either upwards or downwards, when the receptacle units
are connected in a side by side fashion. ing to one embodiment, the openings of the
receptacle units ate, i.e., the first pointing up (or down) and the next pointing down (or
up). According to further embodiments, any number of openings is located on the side, front
or back of the receptacle unit. According to this invention, any such opening may comprise a
straw as detailed above.
[0098] According to another embodiment, the biodegradable sheets are used to manufacture
pouches of larger , to be used as substitute to larger plastic bottles for feeding purified
water dispensing appliances. In this case, the pouch will have a spout that perfectly matches
the inlet of the water dispensing appliance. The pouch will have hanging members that allow
for hanging ofthe pouch, such that the spout is the lowermost, in order to allow water to exit
the pouch by gravity. According to one embodiment, before use, the spout is sealed by
flexible material that may be pierced by a proper tip extending from the inlet of the water
dispensing appliance. Alternatively, the pouch may be inserted into an adapter which receives
the pouch, guides it s the piercing tip and holds it in place, as long as it is not empty.
Fig. 1 illustrates the construction of an exemplary array of receptacle units (related to
herein also as pouches) of different volume, formed in a contiguous side by side fashion
wherein each can be torn off on demand. The array 10 may include a plurality of pouches of
different volume (in this example, volumes of 200 ml, 250, 300 and 350 ml), such that the
entire array is delimited within a size of 20x37 cm. Each pouch is separated from its
neighboring pouches by a ated curved line, for allowing optimal division of the
delimited area between different pouches. Each individual pouch may be marked to show its
volume and content, such as pouch 101.
Fig. 2A illustrates the layout ofa single pouch, according to an embodiment of
the invention. The pouch 101, which is torn off from array 10, comprises a tment 102
for storing the liquid, an internal segment of straw 103 that is hermetically sandwiched
PCT/ILZOIZ/OSOUI25
between the sheets of the compartment 102 and a sealing edge 104 for sealing the external
segment of straw 103 that is also hermetically sandwiched between the sheets of the g
edge 104. A perforated line 105 is implemented between the sealing edge 104 and the
compartment 102.
The user can tear off the scaling edge 104 along the perforated line 105 and
remove the sealing edge 104 from the external segment of straw 103, as shown in Fig. 2B.
This enables the user to drink the fluid via the external segment of straw 103, as shown in
Fig. 2C.
Fig. 2D illustrates the layout of an internal straw segment, according to an
embodiment of the ion. The straw segment 103 has two opposing tapered members
103a and 103b extending outwardly, so as to be attached to (i.e., sandwiched between) the
biodegradable impermeable sheets that define the compartment.
] Fig. 2E rates a cross-sectional view of a sealed internal straw segment,
according to an embodiment of the invention. The two opposing tapered members 103a and
103b are pressed between the two opposing biodegradable impermeable sheets 200, so as to
obtain sealing pressure and prevent both movement of the straw and leaks from around it.
Fig. 3A rates the layout of an array of six pouches, according to an
embodiment of the invention. er needed, each pouch 300 can be torn-off from array
along the corresponding perforated line 105. The fluid e compartment 301 of each
single pouch 300 is terminated by a flat t 302 having a sealing edge 303 at its distal
end, as shown in Fig. 38 (front view). Before use, the flat conduit 302 is bent (e.g., to form a
U—shape) and the sealing edge 303 is attached to the side—wall of the pouch 300 (side view).
Thc perforated linc 105 may be of full length or of partial lcngth.
When the user wishes to drink, he first detaches the sealing edge 303 from the
side-wall and straightens the flat conduit 302, as shown in Fig. 3C. Then he tears-off the
sealing edge 303 along the perforated line 105 and removes the sealing edge 303 from the
distal end of flat conduit 302, thereby breaking the sealing and opening the distal end, to form
a straw segment, as shown in Fig. 3D. Now the user can drink the fluid via the distal cnd, as
shown in Fig. 3E. The straw segment, as well as the sealing edge 303, may be made from the
same biodegradable material that the pouch is made of.
[00l06] Fig. 3F illustrates an array of several receptacle units attached to one another
in a side by side fashion so that the openings thereof ate in an -downward
position. As shown in fig. 3F, only the middlc portion of the various receptacle units is
attached to one another.
ZOIZ/OSOSZS
Fig. 4A illustrates the layout of a single pouch, according to another
ment of the invention. The pouch 400 comprises a clipped compartment 401 for
storing the liquid, which is ated by a flat surface 402, from which a conduit segment
403 extends outwardly. The proximal end of conduit segment 103 is terminated with a
sealing disc (not shown) that is a part ofthe flat surface 402. The g disc also has several
niches formed therein, for receiving mating projections. The sealing disc is attached to the
edges of the conduit segment 403 by a relatively weak layer that seals the compartment 401,
but can be broken by applying a rotational shearing force on it. The shearing force may be
d by a top cover 404 that includes several projections 405. These projections 405 are
designed to mate the formed niches, such that when the cover 404 is attached to the distal end
of conduit t 403, the niches formed in the sealing disc receive the mating projections
405 and remain asably attached to them (e.g., by a unidirectional elastic connection).
According to this embodiment, when the user wishes to drink, he has to rotate the top cover
404, to thereby break the weak layer and disconnect the sealing disc from the edges of the
conduit segment 403. According to this ment, the scaling is broken and the user
removes the top cover along with the g disc that is now attached to the top cover. Thus,
the user can drink the fluid via the conduit segment 403, as shown in Fig. 48. Alternatively,
clipping of the tment may be eliminated by locating the top cover in the middle of the
ll, as shown in Fig. 4C. In this case, the pouch can be laid on any flat support. In both
configurations, the top cover may be reused (screwed), so as to seal the conduit segment 403.
[00l08] Fig. 4D is a cross-sectional view of the top cover sealing arrangement. In this
arrangement, the top cover 406 is screwed on top of the conduit segment 403, which is heat
welded to the edges of the biodegradable impermeable sheet 407, so as to obtain
impermeable sealing.
Figs. 5A and SB illustrate the layout of a single pouch with a pivotally
le straw, according to another embodiment ofthe invention. The pouch 500 comprises
a rigid arched member 501 attached to the edge of the pouch 500. Arched member 501
comprises an elongated groove 502 (cradle) for receiving a matching pivotally foldable rigid
straw 503, which has a tubular conduit for allowing fluid to flow. Arched member 501 also
comprises at its end a spherical tap (not shown) with an orifice into the pouch‘s cavity. This
spherical tap is also used as ajoint around which straw 503 can pivot. As long as the pouch is
stored, straw 503 lies within groove 502 (as shown in Fig. 5A) and the tubular conduit does
not overlap the orifice in the spherical tap. In this position the pouch is sealed. When the
straw 503 is lifted to its vertical position (as shown in Fig. SB), the tubular t overlaps
the orifice in the spherical tap and fluid can flow out of the pouch via straw 503 into the
user’s mouth. The pouch can be sealed again by folding straw 503 back into the cradle after
use. It is also possible to add a sealing sheet to the upper end of the orifice to increase the
sealing level before use and to include a puncturing tip at the end of straw 503, such that the
sealing sheet will be punctured when straw 503 is lifted to its vertical position.
Figs. 6A, 6B, 6C and 6D illustrate an array of four receptacle units, all of
which are closed. Figure 6A is an overview of the array, which include four separable
receptacle units, separated from one another by perforated lines. Further, as shown in Fig.
6A, each of the receptacle units includes a straw at the top (closed in this figure) and a hole at
the , by which the receptacle unit can be hung from any type of hook, rope, twine, etc.
Fig. 6B is a front view of the array, Fig. 6C is a side view of the array and Fig. 6D is a top
view of the array.
Figs. 7A, 7B and 7C show the same array as shown in Figs 6A-D; r, in
Figures 7A-D, all of the receptacle units are opened, having a straw protruding from the top
of each unit. Specifically, Fig. 7A is an overview of the array, Fig. 7B is a front view of the
array, Fig. 7C is a side view ofthe array and Fig. 7D is a top view ofthe array.
According to another embodiment, the biodegradable sheets are made of two
laminated layers. The first layer is an inner layer, made of 10-50 H thick PLA that is in
contact with the liquid. The second layer is an outer layer, made of 50-150 u thick starch that
is d to the air. Both layers are attached to each other by an adhesive layer, the weight
of which is less that 1% of the total weight of the laminated layers. This combination is
unique, due to the fact that the laminated sheet is sufficiently impermeable to hold s,
while being sufficiently flexible to allow efficient and comfortable production ofpouches.
According to another embodiment, the biodegradable sheet, which is highly
flexible and transparent and is suitable for carrying s, is made of Polylactic Acid (PLA)
blended with additional radable polyesters, such as: tylene succinate (PBS),
polybutylene succinate adipate (PBSA), poly(tetramethylene adipate-eoterephthalate)
(PTAT), thermoplastic starch blends.
The Polylactic acids include poly(L—lactie acid), whose structural units are L-
lactide acid; -lactide acid), whose structural units are D-lactic acid; poly(DL-lactic
acid) which is a copolymer of ic acid and D-lactic acid; and any mixture f
Different combinations of the above mentioned polymers should be melt
compounded using a twin-screw extruder. The polymer blends are extruded in the form of
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s to form pellets. The pellets contain a physical mixture ) of the different
polymers used. The blends are then extruded in a cast or a blow ifilm extruder in order to
obtain films or sheets. In order to increase the barrier of the films and sheets, metalized
laminates of the above described polymers can be obtained using an aluminum film or
aluminum vapor deposition.
[001 16] Various aspects ofthe ion are described in greater detail in the following
Examples, which represent embodiments of this invention, and are by no means to be
interpreted as limiting the scope ofthis ion.
EXAMPLES
Example 1
Single layered biodegradable sheets
All ofthe single layered sheets d to herein were 50 microns thick.
18] Sheet #1: A single layered biodegradable sheet consisting of 33.3% w/w PLA,
33.3% w/w PBS and 33.3% w/w Ecoflex was prepared as follows:
A. Melt extrusion compounding stage:
1. 166.7gr PLA, 166.7gr PBS and 166.7gr Ecofiex were dried ght at a
temperature of 500C under vacuum;
2. the dried polymers were dry blended and placed in a two screw PRISM
compounder;
3. the rs were melt ed in the PRISM compounder set to the following
profile:
i) temperature profile: 170—175—180—185—1900C (the Die is set to 1900C);
ii) screw speed: 250rpm; and
iii) pressure: 15—25 bar.
B. Cast extrusion stage:
1. the melt extruded al was dried overnight at a temperature of 50°C under
vacuum;
2. the material was placed into a Randcastle Extruder set to the following profile:
i) 170—180—1900C — 180°C—Adaptor; 1850C —feedblock; Die—1850C;
ii) screw speed: 80rpm; and
iii) head pressure 590bar.
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The ed physical ties of Sheet #1 were as follows: Stress at
Maximum Load was 25Mpa, the Strain at Break was 415% and Young‘s Modulus was
679Mpa.
Sheet #2: A single layered biodegradable sheet consisting of 20% w/w PLA
and 80% w/w PBS was prepared using the same procedure described above for Sheet #1,
wherein the amounts of the polymers used were 100gr PLA and 400gr PBS. The measured
physical properties of Sheet #2 were as s: Stress at Maximum Load was 47Mpa, the
Strain at Break was 731% and Young’s Modulus was 569Mpa.
Sheet #3: A single layered biodegradable sheet ting of 20% w/w PLA,
40% w/w PBS and 40% Novamont CF was prepared using the same procedure described
above for Sheet #1, wherein the amounts of the polymers used were 100gr PLA, 200gr PBS
and 200gr Novamont. The measured physical properties of Sheet #3 were as follows: Stress
at Maximum Load was 33Mpa, the Strain at Break was 579% and Young’s s was
603Mpa.
[00122] Sheet #4: A single layered biodegradable sheet consisting of 60% w/w PLA
and 40% w/w PBS was prepared using the same procedure bed above for Sheet #1,
wherein the amounts of the polymers used were 300gr PLA and 200gr PBS. The measured
physical ties of Sheet #4 were as follows: Stress at Maximum Load was 40Mpa, the
Strain at Break was 240% and Young‘s Modulus was a.
Sheet #5: A single layered radable sheet consisting of 55% w/w PLA
and 45% w/w PBS was prepared using the same procedure described above for Sheet #1,
wherein the amounts of the polymers used were 275gr PLA and 225gr PBS. The measured
physical properties of Sheet #5 were as follows: Stress at Maximum Load was 45Mpa, the
Strain at Break was 4% and Young‘s Modulus was l4l4Mpa.
As evident from their physical properties, as detailed above, Sheets #1—3 are
advantageous one layered biodegradable sheets ing to this invention. Further, as
detailed above, although the composition of Sheets #4 and #5 is very similar, they highly
differ in their physical properties, particularly in their strain at break. Therefore, it is
obviously necessary to perform many ments in order reach the desired physical
properties.
Example 2
Three-layered biodegradable sheets
All ofthe three layered sheets related to herein were 100 microns thick.
Sheet #6: A three layered biodegradable sheet was prepared according to the
procedure described above for Sheet #1, wherein the weight of each layer constitutes a third
of the weight of the final sheet. The three layered Sheet #6 ts of the following three
layers:
Layer 1: 33.3% w/w PLA, 33.3% w/w PBS and 33.3% w/w Ecoflex
Layer 2: 100% w/w PHA
Layer 3: 33.3% w/w PLA, 33.3% w/w PBS and 33.3% w/w Ecoflex
The measured physical properties of Sheet #6 were as s: Stress at Maximum Load was
20Mpa, the Strain at Break was 558% and Young’s Modulus was 675Mpa.
[00127] Sheet #7: A three layered biodegradable sheet was prepared ing to the
procedure described above for Sheet #1, wherein the weight of each layer constitutes a third
of the weight of the final sheet. The three d Sheet #7 consists of the following three
layers:
Layer 1: 33.3% w/w PLA, 33.3% w/w PBSA and 33.3% w/w PBAT
Layer 2: 100% w/w PBAT
Layer 3: 33.3% w/w PLA, 33.3% w/w PBSA and 33.3% w/w PBAT
The measured physical properties of Sheet #7 were as s: Stress at Maximum Load was
30Mpa, the Strain at Break was 618% and Young’s Modulus was 391Mpa.
Sheet #8: A three d biodegradable sheet was prepared according to the
procedure described above for Sheet #1, wherein the weight of each layer tutes a third
of the weight of the final sheet. The three layered Sheet #8 consists of the following three
layers:
Layer 1: 100% w/w PBS
Layer 2: 60% w/w PLA and 40% w/w PBS
Layer 3: 100% W/w PBS
The measured physical properties of Sheet #8 were as follows: Stress at Maximum Load was
44Mpa, the Strain at Break was 4.1% and Young‘s Modulus was 1374Mpa.
Sheet #9: A three layered biodegradable sheet was prepared according to the
procedure described above for Sheet #1, wherein the weight of each layer constitutes a third
of the weight of the final sheet. The three layered Sheet #9 consists of the following three
Layer 1: 100%w/w Ecoflex
Layer 2: 50% w/w PLA and 50% w/w PBAT
Layer 3: 100% w/w Ecoflex
PCT/ILZOIZ/OSOUI25
The measured al properties of Sheet #9 were as follows: Stress at Maximum Load was
38Mpa, the Strain at Break was 559% and Young’s Modulus was 837Mpa.
As evident from their physical properties, as detailed above, Sheets #6-7 are
advantageous three layered biodegradable sheets according to this invention.
In all of the above , layer 2 is sandwiched between layers 1 and 3 so that
layers 1 and 3 are on the outside of the three layered biodegradable sheet and have contact
with the outside atmosphere and layer 2 is positions between them so that it does not contact
the e atmosphere.
Example 3
Physical, mechanical, thermal and barrier properties of monolayer, layered and
five-layered biodegradable sheets
Sheet #10: A monolayered biodegradable sheet consisting of 25% w/w PLA
and 75% w/w PBSA was prepared using the same procedure bed above for Sheet #1,
wherein the amounts of the polymers used were 125gr PLA and 375gr PBS. The measured
physical, ical, thermal and barrier properties of Sheet #10 were as follows:
al Properties
Specific Gravity 1.25 ASTM D792
Melt volume rate (190002.16 kg) [cm3/10 min] 3.9 ASTM D1238
Melt flow rate (190 OC/2. 16 kg) [g/10 min] 4.2 ASTM D1238
Mechanical Properties
Tensile Strength (CZ; Break, (MPa) 32 ASTM D882
Tensile s, (MPa) 894 ASTM D882
Tensile tion, % 339 ASTM D882
Notched lzod Impact, (J/m) 536 ASTM D256
Thermal ties
Heat distortion temperature HDT [QC/18.5kg/cm2] 45 ASTM D648
Barrier properties
OTR (oxygen transmittance from bottle) 0.3 cc/pack/day
Sheet #11: A three layered biodegradable sheet was prepared according to the
procedure described above for Sheet #1, wherein the weight of each layer constitutes a third
of the weight of the final sheet. The three layered Sheet #11 consists of the following three
layers:
WO 88443
Layer 1: consisting about 25% w/w PLA and about 75% w/w PBSA;
Layer 2: consisting about 100% w/w PBSA; and
Layer 3: consisting about 25% w/w PLA and about 75% w/w PBSA.
The ed physical, ical and barrier properties of sheet #11 were as
follows:
Physical Properties
Light transmittance (%) 88
Mechanical Properties
Tensile Strength (a; Break, MD (MPa) 24 ASTM D882
Tensile Strength 6i; Break, TD (MPa) 22 ASTM D882
Tensile Modulus, MD (MPa) 527 ASTM D882
Tensile Modulus, TD (MPa) 392 ASTM D882
Tensile Elongation, MD 00 319 ASTM D882
Tensile Elongation, TD % 463 ASTM D882
r properties
WVTR [water transmittance, g,/(m2°d)] 48.4 ASTM E96
OTR [cm3/(m2'd-bar)] 54.1 ASTM D3985
Sheet #12: A five layered biodegradable sheet was prepared according to the
procedure described above for Sheet #1, wherein the ess of each of layers 1 and 5
constitutes about 30% of the total thickness, the thickness of each of layers 2 and 4
constitutes about 15% of the thickness final sheet, and the ess of layer 3 constitutes
about 10% of the thickness of the final sheet. It is noted that since the materials have
approximately the same density, the weight ratio is about the same as the thickness ratio. The
five layered Sheet #12 consists of the following five layers:
Layer 1: consisting about 25% w/w PLA and about 75% w/w PBSA;
Layer 2: consisting about 100% w/w PBSA;
Layer 3: consisting about 100% w/w PVOH;
Layer 4: consisting about 100% w/w PBSA; and
Layer 5: consisting about 25% w/w PLA and about 75% w/w PBSA.
The measured physical, mechanical and barrier properties of sheet #12 were as
follows:
Physical ties
Light transmittance (%‘) 88
Mechanical Properties
40 Tensile Strength @ Break, MD (MPa) 32 ASTM D882
e Strength @ Break, TD (MPa) 27 ASTM D882
Tensile Modulus, MD (MPa) 464 ASTM D882
Tensile Modulus, TD (MPa) 596 ASTM D882
Tensile Elongation, MD % 687 ASTM D882
Tensile Elongation, TD % 447 ASTM D882
Barrier ties
WVTR [g/(m2'd)] 57.0 ASTM E96
OTR [cm3/(m2-d-bar)] 2.2 ASTM D3985
Sheet #13: A five layered biodegradable sheet was prepared ing to the
procedure described above for Sheet #1, wherein the ess of each of layers 1 and 5
constitutes about 30% of the total thickness, the thickness of each of layers 2 and 4
constitutes about 15% of the thickness final sheet, and the thickness of layer 3 constitutes
about 10% of the thickness of the final sheet. It is noted that since the materials have
approximately the same density, the weight ratio is about the same as the thickness ratio The
five layered Sheet #13 consists ofthe following five :
Layer 1: consisting about 25% w/w PLA and about 75% w/w PBSA;
Layer 2: consisting ofPBSA and about 20% w/w nano-kaolin;
Layer 3: consisting about 100% w/w PVOH;
Layer 4: consisting of PBSA and about 20% w/w nano-kaolin; and
Layer 5: consisting about 25% w/w PLA and about 75% w/w PBSA.
The barrier ties of sheet #13 were as s:
Barrier properties
WVTR [g/(m2-d)] 30.0 ASTM E96
OTR [cm3/(m2-d-bar)] 2.0 ASTM D3985
As evident from the above results, the addition of PVOH to the biodegradable
sheet lowers the OTR and the further addition of nanoclays lowers the WVTR.
Example 4
Biodegradability
Sheet #14: A three layered biodegradable sheet was prepared according to the
procedure described above for Sheet #1, wherein the weight of each layer constitutes a third
of the weight of the final sheet. The three layered Sheet #14 consists of the ing three
layers:
Layer 1: consisting about 75% w/w PLA and about 25% w/w PBSA;
Layer 2: consisting about 100% w/w PBSA; and
Layer 3: consisting about 75% w/w PLA and about 25% w/w PBSA.
According to ISO 2 the rcfcrcncc material used was microcrystallinc
cellulose. The graph presented in figure 8 shows the percentage degree of degradation of
Sheet #14 (columns N1 and N2) in comparison to the reference (columns N3 and N4). Other
than the sheet in colunms N1 and N2 and thc rystallinc cellulose in columns N3 and
N4, the columns were filled with compost. Throughout this test, the temperature of the
columns was kept at 58°C.
While certain features of the invention have been illustrated and described
herein, many ations, substitutions, changes, and cquivalcnts will now occur to those
of ordinary skill in the art. It is, therefore, to be tood that the appended claims are
intcndcd to cover all such modifications and changes as fall within the true spirit of the
invention.
Claims (12)
1. A biodegradable sheet comprising a nanoclay and PVOH.
2. A biodegradable sheet comprising an inner layer, wherein said inner layer comprises PVOH, wherein the sheet is devoid of a fibrous substrate.
3. The biodegradable sheet according to claim 1, wherein the nanoclay is based on montmorrilonite, ulite, nano-kaolin, bentonite, or any combination thereof.
4. The biodegradable sheet according to claim 1, wherein the nanoclay is dispersed in the bulk of the biodegradable composition.
5. The biodegradable sheet ing to claim 1, wherein the nanoclay is added to the biodegradable sheet as a separate nanocomposite layer comprising a biodegradable polymer and the nanoclay.
6. The biodegradable sheet according to claim 5, wherein the separate nanocomposite layer is an internal layer.
7. The biodegradable sheet ing to claim 2, further comprising a compatibilizer.
8. The biodegradable sheet ing to claim 7, wherein the ibilizer is maleic anhydride, benzoyl peroxide or 2,2-azobis(isobutyronitrile).
9. The biodegradable sheet according to claim 2, consisting of the following five layers: Layer 1: consisting about 20-80% w/w PLA and about 80-20% w/w PBSA; Layer 2: consisting about 100% w/w PBSA; Layer 3: consisting about 100% w/w PVOH; Layer 4: consisting about 100% w/w PBSA; and Layer 5: ting about 20-80% w/w PLA and about 80-20% w/w PBSA.
10. The biodegradable sheet ing to claim 2, consisting of the following five layers: Layer 1: consisting about 20-80% w/w PLA and about 80-20% w/w PBSA; Layer 2: consisting of about 90-85% PBSA and about 10-15% w/w nanoclays; Layer 3: ting about 100% w/w PVOH; Layer 4: consisting of about 90-85% PBSA and about 10-15% w/w nanoclays; and Layer 5: consisting about 20-80% w/w PLA and about 80-20% w/w PBSA.
11. A receptacle unit prepared from the biodegradable sheet according to any one of claims 1 or 2, comprising a compartment for storing liquids and a means by which the liquids are removed therefrom.
12. The biodegradable sheet ing to any one of claims 1 or 2, wherein the biodegradable sheet further comprises an external laminate layer.
Applications Claiming Priority (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US201161570864P | 2011-12-15 | 2011-12-15 | |
US61/570,864 | 2011-12-15 | ||
PCT/IL2012/050525 WO2013088443A1 (en) | 2011-12-15 | 2012-12-13 | Biodegradable sheet |
Publications (2)
Publication Number | Publication Date |
---|---|
NZ626602A NZ626602A (en) | 2015-09-25 |
NZ626602B2 true NZ626602B2 (en) | 2016-01-06 |
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