CN106752994A - Self-adhesive film/diaphragm thickening masterbatch - Google Patents
Self-adhesive film/diaphragm thickening masterbatch Download PDFInfo
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- CN106752994A CN106752994A CN201611106765.9A CN201611106765A CN106752994A CN 106752994 A CN106752994 A CN 106752994A CN 201611106765 A CN201611106765 A CN 201611106765A CN 106752994 A CN106752994 A CN 106752994A
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- self
- adhesive film
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J7/00—Adhesives in the form of films or foils
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J11/00—Features of adhesives not provided for in group C09J9/00, e.g. additives
- C09J11/02—Non-macromolecular additives
- C09J11/06—Non-macromolecular additives organic
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J11/00—Features of adhesives not provided for in group C09J9/00, e.g. additives
- C09J11/08—Macromolecular additives
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J123/00—Adhesives based on homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Adhesives based on derivatives of such polymers
- C09J123/02—Adhesives based on homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Adhesives based on derivatives of such polymers not modified by chemical after-treatment
- C09J123/18—Homopolymers or copolymers of hydrocarbons having four or more carbon atoms
- C09J123/20—Homopolymers or copolymers of hydrocarbons having four or more carbon atoms having four to nine carbon atoms
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J153/00—Adhesives based on block copolymers containing at least one sequence of a polymer obtained by reactions only involving carbon-to-carbon unsaturated bonds; Adhesives based on derivatives of such polymers
- C09J153/02—Vinyl aromatic monomers and conjugated dienes
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2201/00—Properties
- C08L2201/10—Transparent films; Clear coatings; Transparent materials
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2203/00—Applications
- C08L2203/16—Applications used for films
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2205/00—Polymer mixtures characterised by other features
- C08L2205/02—Polymer mixtures characterised by other features containing two or more polymers of the same C08L -group
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2205/00—Polymer mixtures characterised by other features
- C08L2205/03—Polymer mixtures characterised by other features containing three or more polymers in a blend
- C08L2205/035—Polymer mixtures characterised by other features containing three or more polymers in a blend containing four or more polymers in a blend
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2205/00—Polymer mixtures characterised by other features
- C08L2205/06—Polymer mixtures characterised by other features having improved processability or containing aids for moulding methods
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2207/00—Properties characterising the ingredient of the composition
- C08L2207/04—Thermoplastic elastomer
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- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Processes Of Treating Macromolecular Substances (AREA)
- Adhesives Or Adhesive Processes (AREA)
Abstract
The invention belongs to technical field of chemical synthesis, and in particular to a kind of diaphragm or self-adhesive film thickening masterbatch, it is made up of the raw material of following weight hundred：Polyisobutene 10 60%；Adhesion promoting component 10 60%；Plasticizer 2 30%；The 48%EVA5 30% of thermoplastic elastomer (TPE) 8；Antioxidant 0.1 3%；Impact resilience auxiliary agent 5 30%.Obtained product active constituent content of the invention is high, stable performance, and excellent, and the reduction of production process energy consumption, meets the effects of energy saving and emission reduction of country.
Description
Technical field
The invention belongs to technical field of chemical synthesis, and in particular to a kind of diaphragm or self-adhesive film thickening masterbatch.
Background technology
With the increasingly raising of people's living standard, people also become more and more fastidious to the quality lived, therefore self-adhesion
The application of film or adhesive protecting film is just more and more extensive, and self-adhesive film is also known as adhesive protecting film, its wherein one side surface
Tack coat with stickiness.Self-adhesive film is widely used in the electric appliance and electronic such as mobile phone, computer equipment and plastics, glass, building materials etc.
The surface protection of object, tack coat fits in protected object body surface face when using, with it is easy to attach, easily open, open rear object
The advantage of surface noresidue bonding material.Self-adhesive film can be using gluing method, casting method, the production of coextrusion film blowing method；
Because market lacks inner additive type self-adhesive film or diaphragm thickening masterbatch, the adhesive protecting film seen currently on the market
Based on the production of gluing method.The method production self-adhesive film/diaphragm Product Process route be：
Plastic raw materials → blown film → sided corona treatment → finished film → unreel → gluing dilution agent or melting → coating → heating
Drying → trimming → winding → finished product.Its complex process is cumbersome, and energy waste is serious, it is often more important that, alcohol is molten or the molten type glue of benzene
Glutinous agent environmental pollution is serious, and developed country is superseded or strict control is used, based on ater-soluble adhesive, but it is water-soluble
Type adhesive application field is not extensive enough, relatively costly to limit it and widely use.
Self-adhesive film or diaphragm thickening masterbatch produce self-adhesive film and diaphragm using interior additive process, and finished product process route is：
Plastic raw materials → thickening masterbatch → blown film/curtain coating → finished film.
Process is simple, non-secondary pollution, viscosity is arbitrarily adjusted, low production cost, belongs to environmentally friendly product.
Certainly, this thickening masterbatch is also widely used for other self-adhesive foils such as industry winding film, diaphragm, preservative film
Deng.However, the country does not retrieve the Patents of the thickening masterbatch for adhesive protecting film at present.Only some self-adhesive films,
The Patents of diaphragm.Such as：CN200610049175.7 discloses a kind of adhesive protecting film, each composition by weight percent
For：Low density polyethylene (LDPE)：28%~34%, LLDPE：25%~26%, EVA：10%~38%, polyethylene
Elastomer：4%~22%, antistatic master granule：3%~4%, stabilizing additive：2%~6%.Thickening in the formula mainly makes
With EVA and polyethylene elastomer, viscosity is limited, after being only used for some product outputs, temperature industry higher, using scope very
Narrow, such as PC sunlight boards temperature after extruder is extruded is general in 80 degree or so, the product of CN200610049175.7 productions
Can just be clung by heat, when temperature is less than 50 degree, will not touched.
A kind of Publication No. CN204820560U viscous adhesive protecting film self-adhesive layers high are by 90% modified SEBS and 10%
LLDPE is prepared from a kind of viscous adhesive protecting films high of Publication No. CN105500859A and preparation method thereof institute
Self-adhesive layer is stated to be prepared from by 80%~90% modified SEBS and 10%~20% LLDPE.The two are special
Profit is all directly to make adhesion coating using SEBS plus polyethylene blend, and its viscosity is single, and is too dependent on the viscosity of SEBS, no
Can adjustment it is just viscous and hold viscous peel strength, high cost, using being limited in scope.
Self-adhesive film or diaphragm thickening masterbatch, can make according to the viscosity of film requirement and any ratio blending of polyethylene
With simple, Efficient Adhesive Promotion is good, with low cost, it is easy to use the features such as.
The content of the invention
Not enough according to prior art, the technical problems to be solved by the invention are：A kind of diaphragm is provided or self-adhesive film increases
Viscous masterbatch, active constituent content is high, and properties of product are excellent, is formulated excellent.
Diaphragm of the present invention or self-adhesive film thickening masterbatch, are made up of the raw material of following percentage by weight：
Described polyisobutene molecular weight is 600-60 ten thousand.
Described adhesion promoting component is terpene resin, C 5 petroleum resin, C 9 petroleum resin, the resin of hydrogenated carbon five, rosin
Resin, hydrogenated rosin resin, the copolymer resins of light dydrocarbon carbon nine, rosin, hydrogenated rosin, newtrex, ester gum, ancient road tree
One or more in fat, modified rosin and dicyclopentadiene (DCPD) resin.
Described plasticizer is one or more in naphthenic oil, white oil and DOP, DBP.
Described thermoplastic elastomer (TPE) is one or more in SBS, SEBS, SIS and SEPS.
The weight content of VA is 8-48% in described EVA.
Described antioxidant is one or more in 2246,2246S, 168,1010 and 1076.
Described impact resilience auxiliary agent is one or more in EEA, EAA, LDPE, LLDPE, MLDPE and POE.
The beneficial effects of the invention are as follows：
1st, obtained product active constituent content is high, stable performance, and excellent；
2nd, production process energy consumption reduction, meets the effects of energy saving and emission reduction of country；
3rd, preparation method is simple and easy to apply, the carrying out of convenient reaction；
4th, the properties of product for preparing are excellent, and consumption is few, low cost, easily production, and viscosity is high, and adhesion coating is uniform, not degumming, not residual
Staying can strengthen film-strength, transparency etc..
Specific embodiment
The present invention is described further with reference to embodiments.
Embodiment 1
A kind of diaphragm or self-adhesive film thickening masterbatch, are made up of the raw material of following percentage by weight：
Described polyisobutene molecular weight is 30000-60000.
Described adhesion promoting component be terpene resin,.
Described plasticizer is the part by weight that naphthenic oil and DOP respectively account for 50%.
Described thermoplastic elastomer (TPE) is SBS.
The weight content of VA is 8% in described EVA.
Described antioxidant is the part by weight at 2246 and 1076 each stations 50%.
Described impact resilience auxiliary agent is EEA.
Through banbury after above-mentioned material mixing, last extruding pelletization is obtained product, and the properties of product of preparation are excellent, consumption
Few, low cost, easily production, viscosity are high, and adhesion coating is uniform, can strengthen film-strength, transparency etc., outside the thickening master batch product of preparation
See：Transparent or semitransparent spherical particle, density：0.925g/cm3, moisture be less than 0.05%, melting means：10g/10min.
Embodiment 2
A kind of diaphragm or self-adhesive film thickening masterbatch, are made up of the raw material of following percentage by weight：
Described polyisobutene molecular weight is 1400-2400.
For terpene resin and C 9 petroleum resin, (mixed weight ratio is 2 to described adhesion promoting component:3).
Described plasticizer is white oil.
Described thermoplastic elastomer (TPE) is SBS and SEPS.
The weight content of VA is 48% in described EVA.
Described antioxidant is 1010.
Described impact resilience auxiliary agent mixes for the weight fraction of EEA and POE each 50%.
Through banbury after above-mentioned material mixing, last extruding pelletization is obtained product, and the properties of product of preparation are excellent, consumption
Few, low cost, easily production, viscosity are high, and adhesion coating is uniform, can strengthen film-strength, transparency etc., outside the thickening master batch product of preparation
See：Transparent or semitransparent spherical particle, density：0.920g/cm3, moisture be less than 0.05%, melting means：12g/10min.
Embodiment 3
A kind of described diaphragm or self-adhesive film thickening masterbatch, are made up of the raw material of following percentage by weight：
Described polyisobutene molecular weight is 1-2 ten thousand.
Described adhesion promoting component be C 5 petroleum resin,
Described plasticizer is one or more in naphthenic oil, white oil and DOP.
Described thermoplastic elastomer (TPE) is SEPS.
The weight content of VA is 30% in described EVA.
Described antioxidant is 1076.
Described impact resilience auxiliary agent is that (weight ratio is 1 for EEA, EAA and POE:1:2).
Through banbury after above-mentioned material mixing, last extruding pelletization is obtained product, and the properties of product of preparation are excellent, consumption
Few, low cost, easily production, viscosity are high, and adhesion coating is uniform, can strengthen film-strength, transparency etc., outside the thickening master batch product of preparation
See：Transparent or semitransparent spherical particle, density：0.922g/cm3, moisture be less than 0.5%, melting means：15g/10min.
Embodiment 4
A kind of described diaphragm or self-adhesive film thickening masterbatch, are made up of the raw material of following percentage by weight：
Described polyisobutene molecular weight is 15-16 ten thousand.
Described adhesion promoting component is terpene resin.
Described plasticizer is naphthenic oil.
Described thermoplastic elastomer (TPE) is SBS kinds.
The weight content of VA is 28% in described EVA.
Described antioxidant is 2246.
Described impact resilience auxiliary agent is LLDPE.
Through banbury after above-mentioned material mixing, last extruding pelletization is obtained product, and the properties of product of preparation are excellent, consumption
Few, low cost, easily production, viscosity are high, and adhesion coating is uniform, can strengthen film-strength, transparency etc., outside the thickening master batch product of preparation
See：Transparent or semitransparent spherical particle, density：0.926g/cm3, moisture be less than 0.05%, melting means：7g/10min.
Embodiment 5
A kind of described diaphragm or self-adhesive film thickening masterbatch, are made up of the raw material of following percentage by weight：
Described polyisobutene molecular weight is 59-60 ten thousand.
Described adhesion promoting component is light dydrocarbon.
Described plasticizer is naphthenic oil.
Described thermoplastic elastomer (TPE) is SIS.
The weight content of VA is 38% in described EVA.
Described antioxidant is 1076.
Described impact resilience auxiliary agent is MLDPE.
Through banbury after above-mentioned material mixing, last extruding pelletization is obtained product, and the properties of product of preparation are excellent, consumption
Few, low cost, easily production, viscosity are high, and adhesion coating is uniform, can strengthen film-strength, transparency etc., outside the thickening master batch product of preparation
See：Transparent or semitransparent spherical particle, density：0.927g/cm3, moisture be less than 0.1%, melting means：10g/10min.
Claims (8)
1. a kind of diaphragm or self-adhesive film viscosify masterbatch, it is characterised in that be made up of the raw material of following percentage by weight：
2. diaphragm according to claim 1 or self-adhesive film viscosify masterbatch, it is characterised in that described polyisobutene molecule
It is 600-60 ten thousand to measure.
3. diaphragm according to claim 1 or self-adhesive film viscosify masterbatch, it is characterised in that described adhesion promoting component is terpene
One or more in olefine resin, C 5 petroleum resin, rosin resin, the copolymerized petroleum resin of light dydrocarbon carbon nine.
4. diaphragm according to claim 1 or self-adhesive film viscosify masterbatch, it is characterised in that described plasticizer is cycloalkanes
One or more in oil, white oil and DOP.
5. diaphragm according to claim 1 or self-adhesive film viscosify masterbatch, it is characterised in that described thermoplastic elastomer (TPE)
It is one or more in SBS, SEBS, SIS and SEPS.
6. diaphragm according to claim 1 or self-adhesive film viscosify masterbatch, it is characterised in that the weight of VA in described EVA
Content is 8-48%.
7. diaphragm according to claim 1 or self-adhesive film thickening masterbatch, it is characterised in that described antioxidant be 2246,
One or more in 2246S, 168,1010 and 1076.
8. diaphragm according to claim 1 or self-adhesive film thickening masterbatch, it is characterised in that described impact resilience auxiliary agent is
One or more in EEA, EAA, LDPE, LLDPE, MLDPE and POE.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201611106765.9A CN106752994A (en) | 2016-12-06 | 2016-12-06 | Self-adhesive film/diaphragm thickening masterbatch |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201611106765.9A CN106752994A (en) | 2016-12-06 | 2016-12-06 | Self-adhesive film/diaphragm thickening masterbatch |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN106752994A true CN106752994A (en) | 2017-05-31 |
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| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN201611106765.9A Pending CN106752994A (en) | 2016-12-06 | 2016-12-06 | Self-adhesive film/diaphragm thickening masterbatch |
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107698883A (en) * | 2017-10-30 | 2018-02-16 | 天津泽恒包装制品有限公司 | A kind of high viscous diaphragm thickening masterbatch preparation process of noresidue |
| CN109370039A (en) * | 2018-10-15 | 2019-02-22 | 佛山市南海区承欣塑料助剂有限公司 | A kind of thickening master batch and preparation method thereof |
| CN109535534A (en) * | 2018-11-06 | 2019-03-29 | 厦门聚富塑胶制品有限公司 | Viscosity discharges fast winding film and preparation method thereof under low temperature |
| CN111718500A (en) * | 2020-07-10 | 2020-09-29 | 贵州廿庆塑胶有限公司 | Filling master batch, preparation method and application thereof, and modified plastic |
| CN112061593A (en) * | 2020-10-12 | 2020-12-11 | 杭州空气盒子包装有限公司 | Multilayer protection inflatable packaging bag with self-adhesive film |
| CN112852313A (en) * | 2021-01-15 | 2021-05-28 | 东莞市金恒晟新材料科技有限公司 | Protective film convenient for adhesion |
| CN114525093A (en) * | 2021-12-31 | 2022-05-24 | 佛山南宝高盛高新材料有限公司 | Hot melt adhesive for non-woven fabric anti-skid floor mat and preparation method thereof |
| CN114805997A (en) * | 2022-05-12 | 2022-07-29 | 宁波鸿雁包装材料有限公司 | Antistatic packaging film and preparation method thereof |
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|---|---|---|---|---|
| CN103788887A (en) * | 2014-02-18 | 2014-05-14 | 周坤先 | Transparent non-adhesive protective film |
| CN104497426A (en) * | 2014-12-10 | 2015-04-08 | 淄博龙沙高分子材料科技有限公司 | Tackifying master batch and preparation method thereof |
| CN104497900A (en) * | 2014-12-01 | 2015-04-08 | 张家港康得新光电材料有限公司 | Self-adhering protecting film and application thereof in adhering protecting smooth-surfaced PC board |
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2016
- 2016-12-06 CN CN201611106765.9A patent/CN106752994A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103788887A (en) * | 2014-02-18 | 2014-05-14 | 周坤先 | Transparent non-adhesive protective film |
| CN104497900A (en) * | 2014-12-01 | 2015-04-08 | 张家港康得新光电材料有限公司 | Self-adhering protecting film and application thereof in adhering protecting smooth-surfaced PC board |
| CN104497426A (en) * | 2014-12-10 | 2015-04-08 | 淄博龙沙高分子材料科技有限公司 | Tackifying master batch and preparation method thereof |
Cited By (10)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107698883A (en) * | 2017-10-30 | 2018-02-16 | 天津泽恒包装制品有限公司 | A kind of high viscous diaphragm thickening masterbatch preparation process of noresidue |
| CN109370039A (en) * | 2018-10-15 | 2019-02-22 | 佛山市南海区承欣塑料助剂有限公司 | A kind of thickening master batch and preparation method thereof |
| CN109535534A (en) * | 2018-11-06 | 2019-03-29 | 厦门聚富塑胶制品有限公司 | Viscosity discharges fast winding film and preparation method thereof under low temperature |
| CN111718500A (en) * | 2020-07-10 | 2020-09-29 | 贵州廿庆塑胶有限公司 | Filling master batch, preparation method and application thereof, and modified plastic |
| CN111718500B (en) * | 2020-07-10 | 2024-02-27 | 贵州廿庆塑胶有限公司 | Filling master batch, preparation method and application thereof, and modified plastic |
| CN112061593A (en) * | 2020-10-12 | 2020-12-11 | 杭州空气盒子包装有限公司 | Multilayer protection inflatable packaging bag with self-adhesive film |
| CN112852313A (en) * | 2021-01-15 | 2021-05-28 | 东莞市金恒晟新材料科技有限公司 | Protective film convenient for adhesion |
| CN114525093A (en) * | 2021-12-31 | 2022-05-24 | 佛山南宝高盛高新材料有限公司 | Hot melt adhesive for non-woven fabric anti-skid floor mat and preparation method thereof |
| CN114525093B (en) * | 2021-12-31 | 2023-12-08 | 佛山南宝高盛高新材料有限公司 | Hot melt adhesive for non-woven fabric anti-slip floor mat and preparation method thereof |
| CN114805997A (en) * | 2022-05-12 | 2022-07-29 | 宁波鸿雁包装材料有限公司 | Antistatic packaging film and preparation method thereof |
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