CN113232397A - Recyclable packaging material and preparation method thereof - Google Patents
Recyclable packaging material and preparation method thereof Download PDFInfo
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- CN113232397A CN113232397A CN202110684900.2A CN202110684900A CN113232397A CN 113232397 A CN113232397 A CN 113232397A CN 202110684900 A CN202110684900 A CN 202110684900A CN 113232397 A CN113232397 A CN 113232397A
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- polyester film
- modified
- packaging material
- recyclable packaging
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/36—Layered products comprising a layer of synthetic resin comprising polyesters
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C69/00—Combinations of shaping techniques not provided for in a single one of main groups B29C39/00 - B29C67/00, e.g. associations of moulding and joining techniques; Apparatus therefore
- B29C69/001—Combinations of shaping techniques not provided for in a single one of main groups B29C39/00 - B29C67/00, e.g. associations of moulding and joining techniques; Apparatus therefore a shaping technique combined with cutting, e.g. in parts or slices combined with rearranging and joining the cut parts
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B33/00—Layered products characterised by particular properties or particular surface features, e.g. particular surface coatings; Layered products designed for particular purposes not covered by another single class
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B38/00—Ancillary operations in connection with laminating processes
- B32B38/14—Printing or colouring
- B32B38/145—Printing
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B7/00—Layered products characterised by the relation between layers; Layered products characterised by the relative orientation of features between layers, or by the relative values of a measurable parameter between layers, i.e. products comprising layers having different physical, chemical or physicochemical properties; Layered products characterised by the interconnection of layers
- B32B7/04—Interconnection of layers
- B32B7/10—Interconnection of layers at least one layer having inter-reactive properties
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
- C08J5/18—Manufacture of films or sheets
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2307/00—Properties of the layers or laminate
- B32B2307/30—Properties of the layers or laminate having particular thermal properties
- B32B2307/31—Heat sealable
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J2367/00—Characterised by the use of polyesters obtained by reactions forming a carboxylic ester link in the main chain; Derivatives of such polymers
- C08J2367/06—Unsaturated polyesters
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J2467/00—Characterised by the use of polyesters obtained by reactions forming a carboxylic ester link in the main chain; Derivatives of such polymers
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- Engineering & Computer Science (AREA)
- Chemical & Material Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Materials Engineering (AREA)
- Health & Medical Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Medicinal Chemistry (AREA)
- Polymers & Plastics (AREA)
- Organic Chemistry (AREA)
- Mechanical Engineering (AREA)
- Wrappers (AREA)
- Laminated Bodies (AREA)
Abstract
The invention belongs to the technical field of packaging materials, and particularly discloses a recyclable packaging material and a preparation method thereof, wherein the recyclable packaging material comprises a polyester film, a modified polyester film and a pattern layer; the pattern layer is arranged on the surface of the polyester film or the modified polyester film and is positioned between the polyester film and the modified polyester film; the polyester film and the modified polyester film are compounded through hot pressing; the raw material modified polyester of the modified polyester film is prepared by blending pure polyester slices and third monomer modified slices, wherein the third monomer modified slices are formed by polymerizing terephthalic acid, ethylene glycol and a third monomer. The recyclable packaging material is easy to recycle, the use of an adhesive is omitted, and the films are firmly combined; the product can be prepared by printing and hot-pressing compounding, and the process is simple.
Description
Technical Field
The invention relates to the technical field of packaging materials, in particular to a recyclable packaging material and a preparation method thereof.
Background
The traditional composite packaging products are often compounded by a plurality of different materials (such as PET/PA/PE, PET/AL/PE, BOPP/PE and the like), and because different materials have different characteristics, the recovery processing is very inconvenient, good separation effect is difficult to ensure, the recovery cost is very high, and no one is willing to recycle, so that white pollution is caused; and the different materials need to use the gluing agent usually when compounding, the solvent in the gluing agent can volatilize when processing, not only endanger operating personnel's health, also can cause adverse effect to the environment, the packaging material of producing in addition also can give off the peculiar smell because of remaining solvent, if be used for packing food, can pollute food, therefore the safety in utilization is poor.
Patent CN213157258U discloses a recoverable compound blow molding or plastic uptake packaging material, including surface course, middle supporting layer, sealed inlayer and with the two-layer adhesive layer of each layer complex together, the material of surface course is polyethylene terephthalate (PET), the material of middle supporting layer is amorphous polyethylene terephthalate (APET), the material of sealing layer is PET and ethylene-vinyl alcohol's multilayer coextrusion thing, wherein surface course and middle supporting layer chemical composition are the same, physical properties are different, and account for more than 90% of total sheet quality, can directly retrieve the degradation and use. This patent effectively reduces the packaging material and retrieves the degree of difficulty through adopting the same chemical structure quality to account for the material more than 90%, but still need use the gluing agent, can't solve the problem that aforementioned adhesive exists.
Disclosure of Invention
One of the objects of the present invention is to provide a recyclable packaging material, which is easily recyclable, eliminates the use of adhesives, and has firm bonding between films.
In order to achieve the purpose, the invention adopts the following specific technical scheme:
a recyclable packaging material comprises a polyester film, a modified polyester film and a pattern layer; the pattern layer is arranged on the surface of the polyester film or the modified polyester film and is positioned between the polyester film and the modified polyester film; the polyester film and the modified polyester film are compounded through hot pressing; the raw material modified polyester of the modified polyester film is prepared by blending pure polyester slices and third monomer modified slices, wherein the third monomer modified slices are formed by polymerizing terephthalic acid, ethylene glycol and a third monomer, and the third monomer is one or more of dicarboxylic acids, hydroxycarboxylic acids, glycols, trimellitic acid, trimesic acid, trimethylolpropane and glycerol. Wherein the polyester film is a PET film; when the modified polyester is prepared by blending, the modified slices of the third monomer of the raw material can be one or more; the weight of the third monomer accounts for 1-40% of the total weight of the blend.
In order to reduce the recycling difficulty, the packaging material is made of a single polyester material, and on the basis, in order to overcome the problems of the adhesive in the traditional composite packaging material, the film is bonded by adopting the effect of hot-pressing compounding to replace an adhesive layer. The hot-press lamination is a process of heating to make the surface of a film in a molten state and laminating the film by using the mutual adhesive force between the films in the molten state, and although the process is a common lamination process between the films, the application range is limited, and a film material with good mutual adhesive force in the molten state needs to be searched. If the two PET films are common, the two PET films can not be bonded by hot pressing, but the modified polyester film can effectively solve the problem, the modified polyester prepared by blending the pure polyester slices and the third monomer modified slices is firstly similar to the polyester and is easy to recycle; the packaging material has good thermal bonding performance with polyester, good thermal bonding performance with printing ink (a pattern layer is formed by printing ink mostly), and good self-heat sealability, so that the packaging material can realize bonding between films by utilizing hot-pressing compounding, the bonding effect is firmer than that of an adhesive, the adhesive is omitted, the release of harmful solvents is avoided, the bonding strength between the films is ensured, and the advantages are obvious.
Preferably, the pattern layer is formed by printing ink on the polyester film. The surface of the modified polyester film is in a molten state during hot pressing, and if the pattern layer is printed on the modified polyester film, the printed pattern is likely to be damaged during hot pressing; the surface state of the polyester film is relatively stable during hot pressing, and the pattern layer printed on the polyester film cannot be damaged during hot pressing, so that the hot-pressing compounding is ensured not to influence the printing effect.
Preferably, the ink contains ink resin, the ink resin is one or more of polyurethane, polyester and polyamide, the bonding effect of the ink resin and the modified polyester film is better, and the commercially available products are listed as follows: UNIVERSAL E series available from DIC, GSA series available from Cercis chinensis, GTK series available from Cercis chinensis, and GV-NT series available from Cercis chinensis.
Preferably, the dicarboxylic acids are aliphatic dicarboxylic acids, aromatic dicarboxylic acids, alicyclic dicarboxylic acids, or ester derivatives thereof; the hydroxycarboxylic acid is hydroxycarboxylic acid or an ester derivative of hydroxycarboxylic acid; the diol is aliphatic diol, aromatic diol, ethylene oxide adduct of aromatic diol, diethylene glycol, triethylene glycol, dimer diol, or 1,4 cyclohexanedimethanol. More specifically, the aliphatic dicarboxylic acid such as oxalic acid, succinic acid, adipic acid, glutaric acid, sebacic acid, maleic acid, dimer acid, and the like; such as isophthalic acid, phthalic acid, 2,6 naphthalene dicarboxylic acid, diphenyl-4, 4-dicarboxylic acid, diphenoxyethanedicarboxylic acid, etc.; the alicyclic dicarboxylic acids such as cyclohexanedicarboxylic acid and the like; such as hydroxycaproic acid, p-hydroxybenzoic acid and the like; such as propylene glycol, 1, 2-propanediol, 1, 3-propanediol, butanediol, neopentyl glycol, and the like.
Another object of the present invention is to provide a method for preparing the recyclable packaging material, comprising the steps of:
s1, printing: printing ink on the polyester film in a printing machine according to a design pattern by taking the polyester film as a base material;
s2, hot-pressing compounding: respectively preheating and quickly heating the modified polyester film and the printed polyester film, rolling and compounding the modified polyester film and the printed polyester film, and then cooling to obtain the recyclable packaging material. In practical application, the composite film compounded by hot pressing is cut into semi-finished products with specified width, and then the semi-finished products are made into corresponding bag shapes according to different requirements.
Preferably, in step S1, the thickness of the polyester film is 5 to 60 μm, the surface tension of the polyester film is 45 to 60 dynes, and the printing speed is 80 to 400 m/min.
Preferably, in step S2, the preheating temperature is 50-100 ℃, the instant heating temperature is 100-250 ℃, the rolling composite temperature is 100-250 ℃, and the cooling temperature is 10-60 ℃.
Preferably, in step S2, the conveying speed of the modified polyester film and the polyester film is 50-450m/min, and the pressure during rolling is 0.5-8 MPa.
Preferably, in step S2, the surface of the press roll used in the roll lamination is chrome-plated or fluorine-treated to form a release coating on the surface of the press roll to prevent the film from sticking to the press roll during the hot pressing.
The invention has the following beneficial effects:
1. the invention utilizes the compounding of the modified polyester film and the polyester film, adopts the single material of polyester, is easy to process and treat, can be recycled, effectively reduces the plastic pollution and saves the resources.
2. The modified polyester film, the polyester film and the ink layer have good thermal bonding performance and good self-heat sealability, are suitable for hot-pressing compounding, do not need adhesive bonding, avoid the release of harmful solvents, are green and energy-saving, and ensure the use safety.
3. The interlayer bonding effect of the packaging material prepared by hot-pressing compounding is obviously superior to that of the traditional composite packaging product using an adhesive: the peel strength of the traditional composite packaging product is generally 1-1.5N/15mm, the peel strength of the ink area of the packaging material is more than or equal to 2N/mm, and the non-ink area can not be peeled.
4. The packaging material can be expanded to a structure with more than three layers, has simple process and convenient transformation, and can meet various requirements.
Detailed Description
The present invention will be further described with reference to the following specific examples.
Example 1
A recyclable packaging material comprises a polyester film, a modified polyester film and a pattern layer; the pattern layer is positioned between the polyester film and the modified polyester film and is formed by printing ink on the polyester film; and the polyester film and the modified polyester film are compounded through hot pressing. In the embodiment, the raw material modified polyester of the modified polyester film is maleic acid modified slices obtained by polymerizing terephthalic acid, ethylene glycol and maleic acid, wherein the mass fraction of the maleic acid in the polymer is 20%, and the mass ratio of the phthalic acid to the ethylene glycol is 2: 1; and then pure polyester chips and maleic acid modified chips are blended to prepare the modified polyester resin, wherein the maleic acid modified chips account for 80% of the mixture by mass. The modified polyester film is prepared by mixing, re-melting and extruding pure polyester chips and maleic acid modified chips. The ink is polyurethane ink, namely ink containing polyurethane resin, and the specific model is cercis ocellata GSA 8210.
The preparation method of the recyclable packaging material comprises the following steps:
s1, printing: taking a polyester film as a base material, wherein the thickness of the polyester film is 30 mu m; printing ink on the polyester film in a gravure printing machine according to the design pattern in a color-by-color mode; the surface tension of the polyester film in the printing process was 50 dynes, and the printing speed was 200 m/min.
S2, hot-pressing compounding: respectively preheating the modified polyester film and the printed polyester film to 75 ℃ in hot-pressing compounding equipment; respectively and rapidly heating to 150 ℃; then drawing the modified polyester film and the polyester film between two press rolls with chrome-plated surfaces for rolling and compounding; the conveying speed of the film in the whole hot-pressing compounding process is 200m/min, the pressure during rolling is 4.5Mpa, and the rolling compounding temperature is 200 ℃; and cooling the composite film obtained after rolling and compounding to 30 ℃ by a cooling roller to obtain the recyclable packaging material.
Example 2
A recyclable packaging material comprises a polyester film, a modified polyester film and a pattern layer; the pattern layer is positioned between the polyester film and the modified polyester film and is formed by printing ink on the polyester film; and the polyester film and the modified polyester film are compounded through hot pressing. In this embodiment, the raw material modified polyester of the modified polyester film is a slice modified by 1,4 cyclohexanedimethanol obtained by polymerizing terephthalic acid, ethylene glycol and 1,4 cyclohexanedimethanol, wherein the 1,4 cyclohexanedimethanol accounts for 25% of the mass of the polymer, and the mass ratio of the phthalic acid to the ethylene glycol is 2: 1; and then blending pure polyester chips and 1,4 cyclohexanedimethanol modified chips, wherein the 1,4 cyclohexanedimethanol modified chips account for 60% of the mixture by mass. The modified polyester film is prepared by mixing, melting and extruding pure polyester chips and 1,4 cyclohexanedimethanol modified chips. The ink is polyester ink, namely ink containing polyester resin, and the specific model is cercis negundo GTK 8299F.
The preparation method of the recyclable packaging material comprises the following steps:
s1, printing: taking a polyester film as a base material, wherein the thickness of the polyester film is 5 mu m; printing ink on the polyester film in a gravure printing machine according to a design pattern in a color-by-color mode, wherein the surface tension of the polyester film in the printing process is 45 dynes, and the printing speed is 80 m/min.
S2, hot-pressing compounding: respectively preheating the modified polyester film and the printed polyester film to 50 ℃ in hot-pressing compounding equipment; respectively and rapidly heating to 100 ℃; then drawing the modified polyester film and the polyester film between two press rolls with chrome-plated surfaces for rolling and compounding; the conveying speed of the film in the whole hot-pressing compounding process is 50m/min, the pressure during rolling is 0.5Mpa, and the rolling compounding temperature is 150 ℃; and cooling the composite film obtained after rolling and compounding to 10 ℃ by a cooling roller to obtain the recyclable packaging material.
Example 3
A recyclable packaging material comprises a polyester film, a modified polyester film and a pattern layer; the pattern layer is positioned between the polyester film and the modified polyester film and is formed by printing ink on the polyester film; and the polyester film and the modified polyester film are compounded through hot pressing. In this embodiment, the raw material modified polyester of the modified polyester film is prepared by polymerizing terephthalic acid, ethylene glycol, isophthalic acid and propylene glycol to obtain an isophthalic acid-propylene glycol modified slice, wherein isophthalic acid accounts for 10% by mass of the total polymer, propylene glycol accounts for 8% by mass of the total polymer, and the mass ratio of phthalic acid to ethylene glycol is 2: 1; and then blending pure polyester chips and isophthalic acid-propylene glycol modified chips, wherein the isophthalic acid-propylene glycol modified chips account for 70% of the mixture by mass. The modified polyester film is prepared by mixing, re-melting and extruding pure polyester chips and m-phthalic acid-propylene glycol modified chips. The ink is polyamide ink, namely ink containing polyamide resin, and the specific model is GV6213P/NT of cercis chinensis.
The preparation method of the recyclable packaging material comprises the following steps:
s1, printing: taking a polyester film as a base material, wherein the thickness of the polyester film is 60 mu m; printing ink on the polyester film in a relief printing machine according to the design pattern in a color-by-color mode; the surface tension of the polyester film in the printing process was 60 dynes, and the printing speed was 400 m/min.
S2, hot-pressing compounding: respectively preheating the modified polyester film and the printed polyester film to 100 ℃ in hot-pressing compounding equipment; respectively and rapidly heating to 200 ℃; then drawing the modified polyester film and the polyester film between two press rolls with chrome-plated surfaces for rolling and compounding; the conveying speed of the film in the whole hot-pressing compounding process is 450m/min, the pressure during rolling is 8Mpa, and the rolling compounding temperature is controlled to be 250 ℃; and cooling the composite film obtained after rolling and compounding to 60 ℃ by a cooling roller to obtain the recyclable packaging material.
Comparative example 1
This comparative example provides a conventional composite packaging article, a PET/PE structure, adhesively compounded.
Comparative example 2
This embodiment provides a packaging material, which is a modified mylar-pattern layer-modified mylar structure, in which the modified mylar is used instead of the mylar of embodiment 1, and the pattern layer and the modified mylar are the same as those of embodiment 1.
Comparative example 3
This embodiment provides a packaging material, which uses a polyester film to replace the modified polyester film of embodiment 1, i.e. a polyester film-pattern layer-polyester film structure, wherein the pattern layer and the polyester film are the same as those of embodiment 1. The two layers of polyester films after hot-pressing compounding are separated, and obviously can not be bonded through hot-pressing compounding.
And (3) performance testing: the peel strength of the packaging materials of examples 1-3 and comparative examples 1-2 was tested according to GB/T21302-2007 composite film for packaging and general bag code, and the test results are shown in the following table:
therefore, the packaging material disclosed by the invention does not use an adhesive, but can obtain a better interlayer bonding effect than the traditional adhesive composite packaging product.
This detailed description is to be construed as illustrative only and is not to be taken as limiting the invention, as any changes that may be made by a person skilled in the art after reading the present specification will be protected by the patent laws within the scope of the appended claims.
Claims (9)
1. A recyclable packaging material, characterized by: comprises a polyester film, a modified polyester film and a pattern layer; the pattern layer is arranged on the surface of the polyester film or the modified polyester film and is positioned between the polyester film and the modified polyester film; the polyester film and the modified polyester film are compounded through hot pressing; the raw material modified polyester of the modified polyester film is prepared by blending pure polyester slices and third monomer modified slices, wherein the third monomer modified slices are formed by polymerizing terephthalic acid, ethylene glycol and a third monomer, and the third monomer is one or more of dicarboxylic acids, hydroxycarboxylic acids, glycols, trimellitic acid, trimesic acid, trimethylolpropane and glycerol.
2. The recyclable packaging material of claim 1, wherein: the pattern layer is formed by printing ink on the polyester film.
3. The recyclable packaging material of claim 2, wherein: the ink contains ink resin, and the ink resin is one or more of polyurethane, polyester and polyamide.
4. The recyclable packaging material of claim 1, wherein: the dicarboxylic acids are aliphatic dicarboxylic acids, aromatic dicarboxylic acids, ester ring dicarboxylic acids or ester derivatives thereof; the hydroxycarboxylic acid is hydroxycarboxylic acid or an ester derivative of hydroxycarboxylic acid; the diol is aliphatic diol, aromatic diol, ethylene oxide adduct of aromatic diol, diethylene glycol, triethylene glycol, dimer diol, or 1,4 cyclohexanedimethanol.
5. The method of producing a recyclable packaging material as described in any of claims 2-4, comprising the steps of:
s1, printing: printing ink on the polyester film in a printing machine according to a design pattern by taking the polyester film as a base material;
s2, hot-pressing compounding: respectively preheating and quickly heating the modified polyester film and the printed polyester film, rolling and compounding the modified polyester film and the printed polyester film, and then cooling to obtain the recyclable packaging material.
6. The method of making recyclable packaging material as defined in claim 5, wherein: in step S1, the thickness of the polyester film is 5-60 μm, the surface tension of the polyester film is 45-60 dyne, and the printing speed is 80-400 m/min.
7. The method of making recyclable packaging material as defined in claim 5, wherein: in step S2, the preheating temperature is 50-100 ℃, the instant heating temperature is 100-250 ℃, the rolling composite temperature is 100-250 ℃, and the cooling temperature is 10-60 ℃.
8. The method of making recyclable packaging material as defined in claim 5, wherein: in step S2, the conveying speed of the modified polyester film and the polyester film is 50-450m/min, and the pressure during rolling is 0.5-8 Mpa.
9. The method of making recyclable packaging material as defined in claim 5, wherein: in step S2, the surface of the press roll used for roll lamination is subjected to chrome plating or fluorine treatment.
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Citations (2)
Publication number | Priority date | Publication date | Assignee | Title |
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US20190337274A1 (en) * | 2017-01-11 | 2019-11-07 | Bostik, Inc. | Extrudable antifog copolyester heat seal resins |
JP2020183252A (en) * | 2019-04-27 | 2020-11-12 | 進栄化成株式会社 | Bag container, recycling method, and laminating method |
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Patent Citations (2)
Publication number | Priority date | Publication date | Assignee | Title |
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US20190337274A1 (en) * | 2017-01-11 | 2019-11-07 | Bostik, Inc. | Extrudable antifog copolyester heat seal resins |
JP2020183252A (en) * | 2019-04-27 | 2020-11-12 | 進栄化成株式会社 | Bag container, recycling method, and laminating method |
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