The present invention relates to a method for improving the airtightness of buildings or rooms in buildings using a vapor barrier membrane, comprising a biopolymer-based hydrophilic middle layer and two relatively more hydrophobic outer layers than the middle layer.
Humidity-regulator or humidity-regulating vapor barrier membranes, the water vapor permeability of which varies according to the humidity of the air, have been known for many years. For reasons explained, for example, in application WO96/33321, it is sought to obtain membranes that allow water vapor to pass easily when relative humidity (RH) is high (70% to 100% RH) and which effectively block it at low relative humidity (50% RH and less).
Such membranes, when they are arranged on the inner face of a thermal insulation material (the face turned toward the interior of a building or room), prevent as much as possible during the cold and dry season the water vapor from entering from the interior of the building into the space between the membrane and the wall and to condense on the latter (cold wall). Conversely, at the hot season, the high permeability of the membrane allows the humidity potentially present in the structural elements of the frame to be evacuated toward the inside of the building. This property is particularly important in the case of new construction where, during installation, certain elements may have a very high water content due to their storage conditions, but also in the case of water ingress into existing structures. In both cases, it is important to be able to let the entire structure dry in an effective manner in summer, towards the outside and inside of the building. This need is crucial in particular if the elements making up the system are conducive to the proliferation of microorganisms.
Such vapor barrier membranes having differentiated behavior as a function of the relative humidity conditions surrounding them are frequently referred to as “smart vapor retarder” (SVR) membranes. In the present application, the expressions “humidity-regulator”, “humidity-regulating” and “smart” are used as synonyms when they describe the variation in water vapor permeability of the vapor barrier membranes.
It is common to express the water vapor permeability of a membrane in terms of “equivalent air layer thickness” for the diffusion of water vapor (Sd). This thickness is expressed in meters and corresponds to the thickness of the air layer that would oppose a resistance equivalent to the diffusion of water vapor. Consequently, the greater the equivalent air layer thickness, the less permeable the membrane is to water vapor. The equivalent air layer thickness (Sd) can be determined in accordance with standards EN1931 and EN ISO12572.
A humidity-regulating vapor barrier membrane is generally considered to be all the more beneficial and effective as its equivalent air layer thickness is high at low relative humidity and low at high relative humidity.
The humidity-regulating vapor barrier membranes available on the market and described in the state of the art are generally based on synthetic organic polymers manufactured from petroleum monomers.
The most frequently described and used polymers are polyamides, in particular polycaprolactam, polyvinyl alcohol (PVOH), copolymers of ethylene and vinyl acetate and/or of vinyl alcohol (EVA and EVOH). The most hydrophilic polymers (PVOH, EVOH) may be combined, in multilayer structures, with more hydrophobic thin layers, in particular based on polyolefins, such as polyethylene, polypropylene and ethylene and propylene copolymers.
By way of examples of documents describing such “smart” vapor barrier membranes documents WO2007/010388, WO2006/034381, WO2005/110892, U.S. Pat. Nos. 7,008,890, 6,808,772 and 6,878,455 may be cited.
The purpose of the research, which resulted in the present invention, was to replace the humidity-regulating vapor barrier membranes of the prior art based on petroleum-sourced polymers, which are generally non-biodegradable, with humidity-regulating vapor barrier membranes based on biosourced and/or biodegradable polymers. These biosourced and/or biodegradable polymers will be referred to hereinafter as “biopolymers”. The biopolymers are preferably biosourced, that is based on a short-term renewable biological origin materials. In a particularly preferred embodiment, the biopolymers used in the membranes of the present application are both biosourced and biodegradable.
Biosourced biopolymers encompass both the natural organic polymers, present as such in biomass, the organic polymers obtained by physical and/or chemical modification of these natural polymers, and synthetic organic polymers obtained by polymerization of biosourced ingredients.
Membranes based on such biopolymers, for example based on cellulose, chitosan or even based on poly (3-hydroxybutyrate) (PHB) are known and have been used, as replacements for films based on petrosourced synthetic polymers, in particular in the field of food packaging where membranes generally are required to supply water vapor permeability that is relatively independent of the humidity and temperature conditions. Furthermore, in the field of food packaging, the service life of packaging films is quite limited and generally ranges from a few days to a few weeks, at most to a few months. In the field of vapor barrier membranes, on the contrary, a long lifetime of at least several years, or even several decades, is sought.
Biopolymer-based membranes are most often rather hydrophilic and their permeability to water vapor is high. The equivalent air layer thickness of these membranes is generally less than 1 m and its absolute value varies little with the relative humidity of the atmosphere surrounding them. These membranes therefore remain extremely permeable to water vapor regardless of the surrounding conditions.
Without wishing to be bound by any theory, it is believed that the low variation in water vapor permeability of these rather hydrophilic membranes can be attributed to the plasticizing effect of the water which “dissolves” in the membrane, even at low humidity. The higher the ambient humidity, the more the material of the membrane is plasticized by water and the more easily the water molecules diffuse within the membrane.
The main drawback of these membranes consisting of biopolymers, for the purpose of their possible use as humidity-regulating vapor barriers, therefore lies in the fact that their permeability to water vapor remains overall too high at low relative humidity for them to be able to operate satisfactorily during the cold, dry season. A membrane consisting only of cellulose would thus not form a sufficient barrier to the water vapor coming from the inside of the building and would not prevent efficiently enough the water vapor from entering the space between the membrane and the wall and condensing in the insulating material and on the inner face of the outer wall.
In summary biopolymer-based hydrophilic membranes used in the field of food packaging remain too permeable to water vapor under low relative humidity (cold-season) conditions. They are therefore not “smart” enough to be able to operate properly as a vapor barrier in the field of thermal insulation of buildings, in particular to improve airtightness and the management of water vapor flows in buildings.
The present invention is based on the surprising discovery that it is possible to very significantly increase the “smartness” of biopolymer-based membranes and thus makes them compatible with use as a vapor barrier membrane in the field of construction, by applying on each of their two faces a very thin layer of a polyester, less permeable to water vapor.
This discovery was even more surprising given that the fairly hydrophobic polyesters deposited on both faces of the biopolymer membrane have a water vapor permeability which is independent of the ambient relative humidity. In other words, membranes consisting only of these hydrophobic polymers would not have any humidity-regulating nature. It was therefore impossible to predict that the deposition of these same hydrophobic polyesters on the faces of a membrane made of hydrophilic biopolymer(s) would greatly increase the “smartness” thereof by allowing it to have extremely low permeability to water vapor during the dry season and high permeability to water vapor during the wet season.
The present application thus relates to a humidity-regulating vapor barrier membrane comprising an active portion comprising
It also concerns a method for improving the airtightness of a building or room in a building comprising the use of a vapor barrier membrane on the inner face of the walls of said building or said room in a building, characterized in that the vapor barrier membrane is a humidity-regulating vapor barrier membrane comprising an active portion comprising:
The active portion of the membrane is preferably a three-layer structure made up of a middle layer and two outer layers as defined above.
The permeability coefficients P1 and P2 are those of the polymers respectively forming the middle layer and the outer layers. They correspond to the ratio of the water vapor mass flow (Q) which passes through an area (A) of a membrane of the polymer to be tested having a given thickness (E), under the effect of a water vapor pressure difference (dP) existing on either side of the membrane.
They are determined according to the experimental protocol described in detail below and are expressed in “Barrers”, that is the mass flow Q is expressed in cm3 (normal pressure and temperature) per second, the thickness E is expressed in cm, the area A of the area traversed is expressed in cm2, and the water vapor pressure difference (dP) is expressed in cm Hg (see in particular S. A. Stern, Journal of Polymer Science Part A-2, vol. 6 (1968), pages 1933-1934).
The membrane of the present invention therefore includes a relatively thick layer based on a hydrophilic biopolymer (middle layer), coated on both its faces of a continuous layer of a hydrophobic polymer (outer layers).
The two outer layers generally have a thickness smaller than that of the middle layer. The ratio of the thickness of the middle layer to the thickness of each of the outer layers is advantageously between 1.5/1 and 1000/1, preferably between 2/1 and 500/1, in particular between 3/1 and 200/1.
The two outer layers are preferably directly in contact with the middle layer, that is, the interface between the layers is preferably free of adhesive.
In the less preferred case, where the outer layers are attached to the middle layer by means of an adhesive, the latter preferably would have a permeability coefficient P3 greater than P1 and P2. In other words, the adhesive should not offer resistance to the diffusion of the water vapor greater than the resistance from each of the layers constituting the membrane.
The layers defined above form the “active portion” of the membranes of the present invention. This part is preferably a membrane obtained in a known manner by co-extrusion of thermoplastic polymers forming the different layers, by heat bonding of films (outer layers) on the middle layer, or by deposition of a coating on both faces of the middle layer.
Although the active portion in principle has a mechanical strength allowing it to be used alone, that is to say without a support layer, it may be advantageous, in particular for active layers of small thickness (less than 50 μm), to reinforce it with a mechanical structure permeable to air and whose resistance to the diffusion of water vapor is therefore negligible compared with that of the active layer, which is impermeable to air.
In an advantageous embodiment, the vapor barrier membrane therefore further comprises an air-permeable reinforcing or protective layer, directly in contact with the active portion, that is to say with one of the outer layers. This support layer may be a grid, a perforated plate, an open-porosity foam or a woven or non-woven fabric, that is permeable to air. This is preferably an air-permeable textile, preferably a non-woven fabric. Mention may be made, as examples of particularly preferred support layers, of nonwovens made of polypropylene or polyester fibers or of glass fibers. The support layer(s) are preferably attached to the active membrane, or active layer, by bonding using a polyurethane adhesive. The present invention also encompasses membranes where a reinforcement structure, such as a grid or a non-woven, is incorporated into the active portion of the membrane and more particularly into the middle layer.
As explained in the introduction, the biopolymers forming the middle layer are biosourced and/or biodegradable organic polymers. They are preferably biosourced.
Biosourced biopolymers are preferably selected from the group consisting of
Osides encompass heterosides, the hydrolysis of which produces non-carbohydrate oses and compounds and holosides which are polymers consisting exclusively of oses.
Mention may be made, by way of examples of osides usable to form the middle layer of the vapor barrier of the present invention, of those chosen from the group consisting of alginate, carrageenan, cellulose, in particular regenerated cellulose (cellulose hydrate), chitin, chitosan, pectin, dextrin, starch, curdlan, FucoPol, gellan gum, pullulan and xanthan.
The proteins are advantageously selected from the group consisting of gluten, soy protein isolate, zein, whey proteins, casein, collagen and gelatin.
Most of these biosourced polymers, extracted from biomass, have a high affinity for water and dissolve or swell in water to form hydrogels.
It may consequently be advantageous, or even necessary, to chemically modify them in order to reduce their hydrophilic nature, in particular to crosslink them in order to make them insoluble in water.
Mention may be made, as examples of chemically modified biosourced biopolymers, of cellulose esters, in particular cellulose acetate, cellulose ethers (in particular ethylcellulose, hydroxyethylcellulose), nitrocellulose, starch esters and ethers.
The third category of biosourced biopolymers is formed by the polymers synthesized from biosourced monomers.
These polymers may be linear or branched, and therefore thermoplastic, or thermoset.
Mention may be made, as examples of synthetic polymers obtained from biosourced monomers, of those selected from the group consisting of polyhydroxyalkanoates (PHA), in particular polyhydroxybutyrate (PHB) and poly(hydroxybutyrate-co-hydroxyvalerate) (PHBV), poly(lactic acid) (PLA), poly(glycolic acid) (PGA), poly(lactide-co-glycolide) (PLGA), the polymers obtained by polymerization of lipid monomers, and the thermoset polymers obtained by reaction of monosaccharides, disaccharides, oligosaccharides and/or alditols with a polycarboxylic acid and/or a polyaldehyde.
The thermoset polymers obtained by reaction of monosaccharides, disaccharides, oligosaccharides and/or alditols with a polycarboxylic acid and/or a polyaldehyde are well known in the field of binders for mineral wools and are described in detail, for example in international applications WO2009/080938, WO2010/029266, WO2013/014399, WO2013/021112 and WO2015/132518 in the name of the Applicant.
As explained in the introduction, it is also possible to use polymers of petrochemical origin to form the middle layer of the membranes of the present invention when they are biodegradable within the meaning of the NF EN 13432 standard.
Biodegradable biopolymers may advantageously be selected from the group consisting of homopolymer alipathic polyesters such as poly(caprolactone) (PCL) and poly(butylene succinate) (PBS), aliphatic copolyesters such as and poly(butylene succinate-co-adipate), aromatic copolyesters such as poly(butylene adipate-co-terephthalate) (PBAT) and polyesteramides.
All the biopolymers constituting the middle layer have a permeability coefficient P1, determined at 23° C. under dry conditions (about 25% average relative humidity), greater than or equal to 600 Barrers, preferably between 600 and 50,000 Barrers, in particular between 700 and 30,000 Barrers, and ideally between 800 and 20,000 Barrers.
This permeability coefficient is determined as follows:
Five samples of the same membrane of thickness (E) are sealed by means of a sealing product above test cups containing a desiccant (CaCl2 powder imposing relative humidity in the cup of about 1%). A template is arranged on the surface of the films prior to the application of the sealing product, in order to create an exchange zone, free of any sealing product and of a defined zone (A). Various sealing products can be used. The sealing product is for example a mixture of 60% microcrystalline wax and 40% refined crystalline paraffin.
The cups thus produced are placed in a temperature-controlled test chamber (23° C.) and in relative humidity (50%), also called a climate chamber.
Due to the difference in partial pressure of vapor (dP) prevailing inside the test cups and in the chamber, water vapor migrates through the exchange zone of the membranes. Periodic weighings of the cups are carried out in order to determine the water vapor transmission flow rates (Q) in a steady state, then, by calculation, the water vapor permeability coefficient of the films considered, expressed in Barrers. The average of the permeabilities measured on the different assemblies is then calculated and corresponds to the aforementioned permeability coefficient P1.
The hydrophilic middle layer of the vapor barrier membrane of the present invention is covered on its two faces with a continuous layer of an organic polymer that is more hydrophobic and less permeable to water vapor than the middle layer. The term “continuous” here means that each of the outer layers completely covers one of the faces of the median membrane so that the latter is not in contact with the atmosphere. The two continuous layers may be of the same chemical nature and of the same thickness, or else of different chemical nature and/or thickness from each other. Each of them is preferably directly in contact with the middle layer.
The permeability coefficient P2 of each of the outer layers is between 105 and 550 Barrers, preferably between 110 and 520 Barrers, in particular between 120 and 500 Barrers. The permeability coefficient is determined in the same way as the coefficient P1.
The organic polymer constituting the outer layers is advantageously selected from the group consisting of the semi-aromatic polyesters obtained by polycondensation of aliphatic polyols and aromatic polyacids. The semi-aromatic polyesters are preferably thermoplastic polyesters obtained by polycondensation of aliphatic diols, such as ethylene glycol, propane-1,3-diol and butylene glycol, and of aromatic diacids such as terephthalic acid and naphthalic acid. They are preferably selected from the group consisting of poly(ethylene terephthalate) (PET), polybutylene terephthalate (PBT), poly(trimethylene terephthalate) (PTT), and poly(ethylene naphthalate) (PNE) and corresponding copolyesters.
The permeability coefficient P2 of aromatic polyesters decreases when the degree of crystallinity and therefore the degree of orientation of the polyester chains increases. However, it remains generally within the range indicated above. If necessary, it is thus possible to adjust the P2 by modifying the orientation of the chains within the polyester layers.
A vapor barrier membrane with a middle layer consisting of cellulose, in particular regenerated cellulose, and two outer layers constituted of semi-aromatic polyester, preferably poly(ethylene terephthalate), is a particularly preferred embodiment of the vapor barrier membrane used in the method of the present invention.
The active portion of the vapor barrier membrane used in the method of the present invention advantageously has a thickness between 5.0 μm and 240 μm, preferably between 10 μm and 120 μm, in particular between 15 and 80 μm, these values corresponding to the active portion (trilayer) of the membrane, but do not encompass a possible reinforcing and/or protective structure.
Preferably, the wall of the room or wall of the building the airtightness of which is to be improved are insulated, that is to say covered, by a thermal insulating material and the vapor barrier membrane is attached to the heat insulating material or incorporated in the heat insulating material. In one embodiment of the method for improving the airtightness of a building or room in a building, the vapor barrier membrane of the present invention consequently is applied in an internal position relative to the thermal insulation material, preferably in direct contact therewith. The attachment can be done by any suitable means that do not significantly reduce the airtightness of the membrane. It can be done for example by gluing, stapling or by means of a mechanical fastening system using hooks and textile loops (a hook-and-loop fastener of the Velcro® type).
In another embodiment of the method of the present invention, the vapor barrier membrane is integrated into the insulating material and attached to the wall of the room or building at the same time as the latter. The membrane is then oriented parallel to the two main surfaces of the insulating material and is preferably located closer to the main surface facing the inside of the room or building than to the main surface facing the wall.
The thermal insulation material may be any insulating material permeable to water vapor and notably encompasses foams and fiber-based materials. It is preferably made of mineral fibers (mineral wool) or of natural organic fibers (lignocellulosic fibers, cellulose wadding, animal wool), synthetic (polyester fibers) or artificial fibers. It is preferably made of mineral wool.
Four vapor barrier membranes were subjected to an evaluation of their permeability to water vapor under wet and dry conditions.
For this, each membrane was positioned so as to close an aluminum cup using as a jointing product molten paraffin wax (mixture of 60% microcrystalline wax and 40% refined crystalline paraffin) to ensure sealing. To measure water vapor permeability in dry conditions, calcium chloride is introduced into the cup before sealing it with the membrane to impose relative humidity of about 1% inside. The cup/membrane assembly is then introduced into a climate chamber wherein the relative humidity is set at 50% and the temperature at 23° C., so as to create a water vapor differential pressure (dP) on either side of the membrane. The flow of water vapor (Q) which passes through the zone (A) of the membrane with thickness (E) is determined by weighing the cups over time, and the permeability coefficient (expressed in Barrers) is calculated using the formula
The permeability coefficient P1 thus calculated corresponds to an average relative humidity of 25.5% ((1%+50%)/2).
To measure the water vapor permeability under wet conditions (90% average relative humidity), the procedure is analogous, except that liquid water is introduced into the cup in order to set the relative humidity to 100%, and the relative humidity in the climate chamber is set at 80%.
The equivalent air layer thickness (Sd) is also determined for each membrane in accordance with standard EN ISO12572.
The first membrane is a vapor barrier membrane according to the invention. It consists of a middle layer of cellulose with a thickness of 21.4 μm sandwiched between two layers of polyethylene terephthalate (PET) with a thickness of 800 nm each. The permeability coefficient P1 of the middle layer of cellulose is 5,600 Barrers at a relative humidity of 25.5% (23° C.) and 34,600 Barrers at a relative humidity of 90% (23° C.); the permeability coefficient P2 of the PET layers is 300 Barrers (23° C.). It varies little depending on relative humidity.
The second and third membranes consist solely of cellulose and have the same permeability coefficients P1 as the middle layer of the first membrane.
The fourth membrane is a membrane made up of a single active layer of polyamide 6 with a thickness of 40 μm attached to a polypropylene nonwoven. It is available on the market under the name Vario KM Duplex® (Saint-Gobain Isover)
The technical characteristics of the membranes (composition of the layers, thickness, equivalent air layer thickness under dry and wet conditions) are gathered in Table 1 below.
It can be seen that the difference between the equivalent air thickness of the three-layer vapor barrier membrane according to the invention (membrane 1) under dry and wet conditions is significantly stronger than that of all the comparative membranes (membranes 2 to 4).
The two cellulose membranes (membranes 2 and 3) have an equivalent air thickness (Sd) less than 1 m, whether in wet or dry conditions. They are not suitable as vapor barrier membranes since their humidity-regulating power is insufficient. During the dry and cold season, these membranes would let too much water into the space between the membrane and the wall of the building. This insufficiently “smart” behavior is efficiently corrected by the presence of the two thin PET layers.
It may also be noted that the membrane according to the invention (membrane 1) has a total thickness (23 μm) much lower than that of the active portion of the membrane sold by the Applicant, which is equal to 40 μm (Vario KM Duplex®). The excellent performance of the membrane according to the invention consequently makes it possible to reduce the raw materials and consequently the costs.
Number | Date | Country | Kind |
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2103507 | Apr 2021 | FR | national |
Filing Document | Filing Date | Country | Kind |
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PCT/FR2022/050635 | 4/5/2022 | WO |