Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – From carboxylic acid or derivative thereof
Reexamination Certificate
2001-06-08
2004-04-27
Sergent, Rabon (Department: 1711)
Synthetic resins or natural rubbers -- part of the class 520 ser
Synthetic resins
From carboxylic acid or derivative thereof
C528S190000, C528S288000, C528S354000, C528S359000, C525S413000, C525S054300, C428S411100, C428S480000, C428S035100
Reexamination Certificate
active
06727342
ABSTRACT:
The present invention relates to the use of biodegradable polyester resins in the production of formed articles having good properties as barriers to water vapour.
The water-vapour barrier properties of biodegradable polymers developed in recent years are quite poor.
For example, polyesters such as polyhydroxybutyrate-valerate, polylactic acid, polyglycolic acid, polycaprolactone, polybutylene succinate, copolymers such as polybutylene adipate-co-terephthalate, polyester-amides such as polybutylene adipate-co-caprolactam, polyvinyl alcohol, ethylene-vinyl alcohol copolymers, polyesters-urethanes, and esters of cellulose and regenerated cellulose have permeabilities to water vapour greater than 300 g×30 &mgr;m/m
2
per day at 38° C. and 90% relative humidity (RH) (Lyssy method).
The poor barrier properties can be related to the fact that these polymers have good biodegradability which, in order for the bacterial action to be performed advantageously, means that the polymer should be wettable and hence contains polar groups in its structure with a consequent reduction in its water-vapour barrier properties since the polar groups increase the solubility of water in the polymer and hence its permeability to water vapour.
High permeability to water vapour considerably limits the fields of use of biodegradable polymers such as the above-mentioned aliphatic polyesters or copolyesters, particularly where good biodegradability and low permeability to water would be very desirable.
Fields of use in which there is a particular need for biodegradable materials having good water-vapour barrier properties are, for example, the hygiene field (so-called non-breathable nappies, that is to say, nappies with a low transpiration value, similar to the nappies which are in use with a backsheet of polyethylene and non-woven polypropylene fabric), multi-layer and non-multi-layer food packaging based on laminated milk cartons, mulching of soils where the evaporation of water through materials is to be as limited as possible, containers for soil for growing plants in greenhouses, sacks for collecting grass cuttings which require reduced biodegradation rates by virtue of a lower wettability of the biodegradable film of which the sack is made, non-woven, fabric which can provide a dry feel for nappies, fishing nets which must not undergo significant alterations due to water during the period of use, expanded products for packaging which requires moisture protection whilst remaining biodegradable, irrigation pipes for agriculture, products in contact with liquid foodstuffs, such as fast-food cups, plates and drinking straws, expanded trays for foodstuffs, blister packs for pharmaceutical products, nursery plant-pots through which moisture must not be able to pass and which must have a degradation process which does not interfere with the growth of the plants, hygiene products such as colostomy bags and the like, or blood containers, fibres for disposable products which can withstand water and a few washings, for disposable hosiery and garments, etc.
It has now been found, unexpectedly—in view of the outstanding permeability of aliphatic polyesters such as polybutylene adipate, polybutylene succinate, polyhexamethylene adipate and polybutylene adipate-co-terephthalate to water vapour—that the polyester resins defined below have good water-vapour barrier properties and, at the same time, are sufficiently biodegradable in normal composting conditions and are therefore usable in applications in which such properties are required.
The polyester resins usable in the applications of the invention are formed by recurring units X=[O—(CH
2
)
n
—OCO—(CH
2
)
m
—CO] and/or Y=[O—(CH
2
)
k
—CO], where the half-sum of n+m is equal to or greater than 6 and k is a number equal to or greater than 6, or by copolymers comprising units and/or sequences having the formula x
i
[O—(CH
2
)
ni
—OCO—(CH
2
)
mi
CO]; y
j
[O—(CH
2
)
k
—CO] where:
i,j
=1-5
; n
i
=2-22
; m
i
=0-20
; k
j
=1=21;
∑
i
=
1
5
x
i
+
∑
j
=
1
5
y
j
+
1
and x
i
and y
j
vary between 0 and 1 and are molar fractions of the various units such that
∑
i
=
1
5
x
i
·
(
n
i
+
m
i
2
)
+
∑
j
=
1
5
y
j
·
k
j
≥
6
,
or by recurring units
Z=[O—(CH
2
)
a
—OCO—(CH
2
)
b
—CO] where a=2-3 and b=7-11, present in sufficient quantity to ensure good barrier properties and biodegradability of the resins in the production of products in which a permeability to water vapour of less than 350 g×30 &mgr;m/m
2
per day at 38° C. and 90% RH and biodegradability in composting or burial conditions are required.
The products which can be produced from the polyesters as defined above can ensure permeability to water vapour of less than 350, more particularly less than 300, g×30 &mgr;m/m
2
per day at 38° C. and 90% RH.
The biodegradability of the products during composting or burial is sufficient to bring about their decomposition within the required periods of time.
More particularly, in the case of the products produced from the preferred polyester resins, the biodegradability is less than 30% in one month and more than 60% in six months, in accordance with DIN 54900, part II, or decomposition on 30 &mgr;m film of less than 10% in 14 days and more than 90% in 6 months, in accordance with the method described in “Journal of Environmental Polymer Degradation”, Vol. 4, No. 1, 1996, p. 55-63, or in accordance with the burial test described in “Biodegradable Plastics, Practices and Test Methods” ASTM Subsection D-20.96.1 of Environmental Degradable Plastics, Version 4.0 Dec. 6, 1990.
The polyester resins usable according to the invention have a mean numeral molecular weight greater than 10000 and a melting point (acceptable for industrial applications) of between 60 and 110° C.
Polyester resins with a mean numeral molecular weight of between 45000 and 70000 have been found particularly advantageous for use according to the invention.
There is not the slightest reference in the literature either to the barrier properties, particularly to water vapour, of the polyester resins falling within the general formula given above, or to their good biodegradability by decomposition.
The use of the above-mentioned polyester resins in applications which require a low permeability to water vapour (below the value indicated above) combined with a biodegradability during composting compatible with the standards in use is novel and constitutes the subject of the present invention.
Examples of applications in which the polyester resins according to the invention are particularly useful are:
coatings produced by extrusion-coating with good water-barrier properties, particularly for the packaging of fresh milk and diary products, of meat, and of foods with high water content,
multi-layer laminates with layers of paper, plastics material or paper/plastics material, aluminium and metallized films in general,
films as such, and multi-layer films with other polymer materials,
sacks for organic refuse and for grass cuttings with periods of use Longer than 1 week,
single-layer and multi-layer food packaging, particularly containers for milk, yoghurt, cheeses, meat and beverages, in which the layer in contact with the food or beverage is formed by the polyester,
composites with gelatinized starch, destructured starch, native starch in the form of a filler, or complexed starch,
mono-directional or bi-directional films,
semi-expanded and expanded products produced by physical and/or chemical means, by extrusion, injection, or agglomeration of pre-expanded particles, from materials constituted by the polyester as such, from blends, or from filled materials,
expanded sheet and expanded containers for foods, (fruit, vegetables, meat, cheeses) for drugs, and for fast-food,
fibres, fabrics and non-woven fabrics in the hygiene, sanitary and clothing fields,
outer non-woven fabric and/or film, front tapes for increasing the
Bastioli Catia
Cella Giandomenico
Farachi Fernanda
Floridi Giovanni
Foa' Marco
Bryan Cave LLP
Ministero Dell'Universita'E Della Ricerca Scientifica
Rajguru U. K.
Sergent Rabon
LandOfFree
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