CN117487225A - Packaging material with hygroscopicity and preparation method and application thereof - Google Patents

Packaging material with hygroscopicity and preparation method and application thereof Download PDF

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Publication number
CN117487225A
CN117487225A CN202311495476.2A CN202311495476A CN117487225A CN 117487225 A CN117487225 A CN 117487225A CN 202311495476 A CN202311495476 A CN 202311495476A CN 117487225 A CN117487225 A CN 117487225A
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packaging material
parts
moisture absorption
polyvinyl alcohol
polyethylene glycol
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张丽娟
于建平
葛萍花
陈建军
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Jiangsu Daya New Packaging Material Co ltd
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Jiangsu Daya New Packaging Material Co ltd
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    • 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
    • C08J7/00—Chemical treatment or coating of shaped articles made of macromolecular substances
    • C08J7/04—Coating
    • C08J7/0427—Coating with only one layer of a composition containing a polymer binder
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B65—CONVEYING; PACKING; STORING; HANDLING THIN OR FILAMENTARY MATERIAL
    • B65D—CONTAINERS FOR STORAGE OR TRANSPORT OF ARTICLES OR MATERIALS, e.g. BAGS, BARRELS, BOTTLES, BOXES, CANS, CARTONS, CRATES, DRUMS, JARS, TANKS, HOPPERS, FORWARDING CONTAINERS; ACCESSORIES, CLOSURES, OR FITTINGS THEREFOR; PACKAGING ELEMENTS; PACKAGES
    • B65D65/00—Wrappers or flexible covers; Packaging materials of special type or form
    • B65D65/38—Packaging materials of special type or form
    • B65D65/42—Applications of coated or impregnated materials
    • 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
    • C08J7/00—Chemical treatment or coating of shaped articles made of macromolecular substances
    • C08J7/12—Chemical modification
    • 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
    • C08J7/00—Chemical treatment or coating of shaped articles made of macromolecular substances
    • C08J7/12—Chemical modification
    • C08J7/123—Treatment by wave energy or particle radiation
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L67/00—Compositions of polyesters obtained by reactions forming a carboxylic ester link in the main chain; Compositions of derivatives of such polymers
    • C08L67/02—Polyesters derived from dicarboxylic acids and dihydroxy compounds
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
    • C09D129/00—Coating compositions based on homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by an alcohol, ether, aldehydo, ketonic, acetal, or ketal radical; Coating compositions based on hydrolysed polymers of esters of unsaturated alcohols with saturated carboxylic acids; Coating compositions based on derivatives of such polymers
    • C09D129/02—Homopolymers or copolymers of unsaturated alcohols
    • C09D129/04—Polyvinyl alcohol; Partially hydrolysed homopolymers or copolymers of esters of unsaturated alcohols with saturated carboxylic acids
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
    • C09D5/00—Coating compositions, e.g. paints, varnishes or lacquers, characterised by their physical nature or the effects produced; Filling pastes
    • C09D5/14—Paints containing biocides, e.g. fungicides, insecticides or pesticides
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
    • C09D7/00—Features of coating compositions, not provided for in group C09D5/00; Processes for incorporating ingredients in coating compositions
    • C09D7/40—Additives
    • C09D7/60—Additives non-macromolecular
    • C09D7/61—Additives non-macromolecular inorganic
    • C09D7/62—Additives non-macromolecular inorganic modified by treatment with other compounds

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
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  • Polymers & Plastics (AREA)
  • Health & Medical Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Materials Engineering (AREA)
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Abstract

The invention belongs to the technical field of packaging materials, and relates to a packaging material with hygroscopicity, wherein the packaging material comprises a PET (polyethylene terephthalate) base film layer and a moisture absorption layer; the surface of the PET base film layer, which is in contact with the moisture absorption layer, is subjected to polyethylene glycol surface modification, the moisture absorption layer comprises moisture absorption coating liquid, and the coating liquid comprises the following raw materials in parts by weight: 30-35 parts of polyvinyl alcohol; 10-20 parts of modified diatomite; 3-8 parts of an antibacterial agent; 5-10 parts of ethanol; 35-60 parts of water. The invention also discloses a preparation method of the packaging material with hygroscopicity, and the obtained packaging material has excellent hygroscopicity, good interlayer adhesion, difficult falling off and good antibacterial property. When the packaging material is used for preserving foods, particularly fruits and vegetables, water vapor generated in food preservation can be absorbed by the packaging material in time, and can not form condensation on the foods, so that the foods are easy to deteriorate, the storage time of the foods is effectively prolonged, and the coating of the packaging material is firmly bonded, so that the coating can not fall off to influence the safety of the foods.

Description

Packaging material with hygroscopicity and preparation method and application thereof
Technical Field
The invention belongs to the technical field of packaging materials, and particularly relates to a packaging material with hygroscopicity, and a preparation method and application thereof.
Background
In the field of food engineering, many fresh foods are very sensitive to humidity and easy to lose water, when the humidity in the package is condensed and exceeds the standard, microorganisms are bred in the environment with higher humidity, and deterioration and decay of food materials are accelerated. Especially when the packages of fresh vegetables, fruits and other foods are stored, the problems are particularly remarkable, and the freshness and the storage life of the foods are seriously affected. The dry storage environment can improve the storage quality, the existing treatment mode is often used for moisture absorption and prevention by adding a drying agent into food materials, and the method is inconvenient and unsafe, and has low moisture absorption efficiency on the inner wall of the package.
Thermoplastic resin, especially polyethylene terephthalate PET, has excellent mechanical properties, oil resistance, high solvent resistance, excellent high temperature resistance and low temperature resistance, and has little influence on the mechanical properties at high and low temperatures, and is nontoxic and tasteless, and is commonly used for food packaging. However, PET materials have low surface energy, poor hygroscopicity, and low surface adhesion, and are difficult to combine with other materials, so how to obtain a PET packaging material with excellent hygroscopicity for packaging humidity-sensitive foods is a problem to be solved.
Disclosure of Invention
In order to solve the problem of poor hygroscopicity of PET packaging materials, the invention provides a packaging material with hygroscopicity, and a preparation method and application thereof.
In a first aspect, the present invention provides a packaging material having hygroscopicity, which adopts the following technical scheme:
a packaging material with hygroscopicity comprises a PET base film layer and a hygroscopic layer, wherein the contact surface of the PET base film layer and the hygroscopic layer is subjected to polyethylene glycol surface modification before the PET base film layer and the hygroscopic layer are bonded.
The inventor finds that the PET film is firstly subjected to surface modification by polyethylene glycol and then is coated with a moisture absorption liquid, so that the moisture absorption layer can achieve excellent adhesion effect on the PET, the moisture absorption and moisture resistance of the PET film can be maintained for a long time, the polyethylene glycol is a hydrophilic polymer, the moisture absorption and adhesion of the PET film are good, the moisture absorption effect of a packaging material can be enhanced, and the PET film also has a certain antistatic property, so that the PET film is also beneficial to food packaging.
In a specific embodiment, the step of surface modification of the PET base film layer is: polyethylene glycol is coated on one side surface of the PET film, and after plasma treatment, ungrafted polyethylene glycol is removed, and the PET film is dried.
The plasma treatment is a surface treatment technology, and the plasma has high-charge particles, excites and ionizes to destroy molecules, generates new active species such as ions, electrons or free radicals, and the like, can react with functional groups on the surface of the material, and improves the surface performance of the material. Plasma treatment techniques have been used for various surface treatments to improve material properties, with increased interfacial hydrophilicity following treatment consistent with the goals sought by the present invention, and enhanced surface recombination adhesion following plasma treatment also facilitates coating non-shedding, so that the present invention is particularly suitable when hygroscopicity and coating adhesion are sought. According to the invention, polyethylene glycol is coated on one side surface of the PET film, and then plasma treatment is carried out on the surface, in the plasma treatment, part of chemical bonds on the PET surface are opened to form active free radicals, and part of chemical bonds on the polyethylene glycol are opened to form free radicals, and the two are combined to form new chemical bonds, so that polyethylene glycol is grafted on the PET surface, and the polyethylene glycol has excellent hydrophilicity and contains active hydroxyl groups, so that multiple possibilities of bonding of the composite coating can be given.
In a specific embodiment, the polyethylene glycol used for grafting has an average molecular weight of 200 to 1000. The polyethylene glycol has too low molecular weight and toxicity, is not suitable for food packaging, and when the polyethylene glycol has too high molecular weight, the inventor finds that the hygroscopicity and the adhesiveness between film layers of the packaging material are reduced, which may be caused by the fact that when the polyethylene glycol chain segment is too long, on the one hand, the hydroxyl content is low, so that the hygroscopicity is reduced and the influence of hydrogen bonds on heat setting is reduced, so that the adhesiveness is affected; on the other hand, the polyethylene glycol chain segment which is too long is enriched on the surface of PET, the hydroxyl of polyethylene glycol is at the tail end, and the molecular chain side chain does not have hydroxyl, which is unfavorable for the adhesion of the moisture absorption layer on the surface of PET, so the moisture absorption effect and the adhesion effect realized in the molecular weight range of the polyethylene glycol are best.
In a specific embodiment, the hygroscopic layer comprises a hygroscopic coating liquid comprising the following raw materials in parts by weight: 30-35 parts of polyvinyl alcohol; 10-20 parts of modified diatomite; 3-8 parts of an antibacterial agent; 5-10 parts of ethanol; 35-60 parts of water.
When the inventors sought for a material of the moisture absorption layer, it was desired that the moisture absorption coating liquid not only brings about good moisture absorption and barrier properties, but also can keep food dry, mask off-flavors, and avoid tainting, and also that it has excellent adhesion to the PET base film, while ensuring that the prepared packaging composite film can be used for a long time without causing the coating to fall off, affecting the food in the package, and that the main film-forming resin of the coating liquid can have environmental protection characteristics such as non-toxicity, non-odor, etc., so that it can be safely applied to food packaging. Polyvinyl alcohol is a polyhydroxy polymer, has excellent hygroscopicity, high compactness and good barrier property, has good solubility in water, and can form a uniform and continuous hygroscopic layer film after drying, so that the polyvinyl alcohol is coated on a PET base film to form a hygroscopic film for packaging food. The PET surface treated by the plasma is favorable for bonding resin, and the hydroxyl of the polyvinyl alcohol and the hydroxyl of polyethylene glycol grafted on the PET surface can form a hydrogen bond when the polyvinyl alcohol is cured, so that the adhesive force of the polyvinyl alcohol moisture absorption layer and the PET film is further improved. In the prior art, the barrier property and long-term use effect of the polyvinyl alcohol are enhanced by carrying out hydrophobic treatment on the polyvinyl alcohol, and the invention seeks the self water absorption, so that the water absorption and durable use resistance of the polyvinyl alcohol are further improved by matching with other components.
The diatomite is a very good moisture absorbent, has a porous structure and a larger surface area, is favorable for the diffusion and storage of moisture in the diatomite, has static charges on the surface, can absorb water molecules to fix the diatomite in the diatomite, realizes the moisture absorption effect, is nontoxic and harmless, has long moisture absorption service life and stable moisture absorption performance, and can be repeatedly used. Therefore, when the inventor pursues better hygroscopicity, diatomite is selected to be added into the polyvinyl alcohol coating liquid to improve the moisture absorption effect of the whole material. In food preservation, the antibacterial agent can inhibit bacterial growth, but the antibacterial agent is not necessary, and can be added into the coating liquid according to the actual use environment requirements, and under the application requirements of certain products, the antibacterial agent is also added into the coating liquid so as to achieve a certain antibacterial effect.
In a specific embodiment, the modified diatomaceous earth is polyvinyl alcohol grafted diatomaceous earth, comprising the following preparation steps: adding diatomite into an ethanol water solution, regulating the pH value, adding a silane coupling agent, heating to 70-100 ℃, and reacting for 3-6 hours; washing with an organic solvent, and drying to obtain silane coupling agent modified diatomite; adding the silane coupling agent modified diatomite into a polyvinyl alcohol aqueous solution, heating to 70-100 ℃, reacting for 0.5-6h, centrifuging, filtering, washing with an organic solvent, and drying to obtain the polyvinyl alcohol grafted diatomite.
Through the scheme, the diatomite is grafted through the polyvinyl alcohol, and the hydroxyl groups which are not grafted by the polyvinyl alcohol can participate in solidification, so that the stability and the dispersion effect of the diatomite in a coating film are improved, and the improvement of the moisture absorption performance of the packaging material is facilitated. The polyvinyl alcohol grafted diatomite can be any feasible mode, and the diatomite is modified by silane and then reacts with the polyvinyl alcohol, so that the dispersing effect of the diatomite is further improved by the silane. According to the prior art, the inventor finds that when only polyvinyl alcohol is used in the hygroscopic liquid or the polyvinyl alcohol is completely replaced by the polyvinyl alcohol grafted diatomite obtained in the mode, the hygroscopicity is not good because the two components are mixed and used, and the diatomite is grafted to the polyvinyl alcohol, so that the porous structure of the diatomite can be stably attached and better arranged in a three-dimensional network-shaped crosslinked structure formed by crosslinking the polyvinyl alcohol by means of grafting with resin after solidification, and the space for storing water is increased. The polyvinyl alcohol content is preferably 30-35 parts, the grafted modified diatomite content is preferably 10-20 parts, the mixed use effect of the grafted modified diatomite and the modified diatomite is further improved, the diatomite content is too low, the polyvinyl alcohol content is too high, and enough stably dispersed diatomite in the polyvinyl alcohol film is not used for absorbing and storing water, so that the hygroscopicity of the material is poor, and when the modified diatomite content is too high and the polyvinyl alcohol content is too low, the adhesion effect is also affected by the reduction of the hydroxyl groups of the polyvinyl alcohol, so that the optimal mixed use ratio of the grafted modified diatomite and the modified diatomite is realized in the range of the invention.
In a specific embodiment, the antimicrobial agent is a hydroxycyclodextrin coated antimicrobial agent.
The cyclodextrin has a hollow annular structure, so that the cyclodextrin can be included, the antibacterial agent can be slowly released when the cyclodextrin is added into the moisture absorption layer, and the durable antibacterial effect of food packaging is realized, therefore, the cyclodextrin coated antibacterial agent is a relatively mature technology for realizing the slow release of the antibacterial agent, when the conventional slow release antibacterial agent is added, the inventor prefers the hydroxy cyclodextrin, the hydroxy cyclodextrin is selected to have excellent hydrophilicity, the hydroxy on the surface of the hydroxy cyclodextrin participates in the solidification of the hydroxy on the PET surface and the hydroxy on the polyvinyl alcohol, and the stable dispersion of the antibacterial agent in the packaging material is further improved, and the hygroscopicity and the integral adhesive force are more facilitated while the integral antibacterial effect is improved.
In a specific embodiment, the step of preparing the hydroxycyclodextrin coated antibacterial agent comprises: adding hydroxy cyclodextrin into the hot alkaline solution to obtain cyclodextrin solution; adding an antibacterial agent into an alcohol solvent to obtain an antibacterial agent solution; adding the prepared antibacterial agent solution into cyclodextrin solution, heating in 50-80deg.C water bath, performing rotary evaporation after reaction, and oven drying to obtain hydroxy cyclodextrin coated antibacterial agent.
The conventional way for coating the antibacterial agent can be used for coating the antibacterial agent by using the hydroxy cyclodextrin, and the coating way has simple process and low cost.
In a second aspect, the present invention provides a method for producing a packaging material having hygroscopicity, comprising the steps of:
(1) Coating polyethylene glycol on one side surface of a PET base film, removing ungrafted polyethylene glycol after plasma treatment, and drying;
(2) And (3) coating the surface modified by the polyethylene glycol in the step (1) with a hygroscopic coating liquid, and curing to obtain the hygroscopic packaging material.
The PET base film is subjected to plasma polyethylene glycol modification treatment, so that on one hand, the surface energy of the PET base film is increased, the adhesion performance is enhanced, the adhesion with a moisture absorption layer is facilitated, and the durable use and the safety of the packaging material are improved; on the other hand, polyethylene glycol grafted on the surface participates in the solidification of the moisture absorption layer, so that the binding force of the moisture absorption layer and the PET film is further improved. The coating of the moisture absorption layer enables one side of the PET base film to have excellent moisture absorption effect, can be used for packaging foods such as vegetables and fruits, and can maintain longer storage time of the foods.
In a specific embodiment, the method for producing a packaging material having hygroscopicity further comprises the step (3): a hydrophobic layer and/or an oleophobic layer is arranged on one side of the PET base film far away from the hygroscopic layer.
The packaging material needs to have a moisture absorption effect on the contact surface of food to maintain the dryness of the food, and for the air contact surface (PET outer side film), a corresponding functional layer can be designed according to application requirements, when the application scene expects that the outer side of the PET packaging material has certain hydrophobicity or oleophobicity to prevent water vapor in the air or the external environment from entering and prevent greasy dirt, a hydrophobic coating and an oleophobic coating can be coated on one side of the PET film far away from the moisture absorption layer, and both the hydrophobic and oleophobic coatings for packaging can be used for realizing the hydrophobicity and oleophobicity of the other side film of the PET base film.
In a third aspect, the present invention provides the use of a packaging material having hygroscopicity in the packaging and storage of food.
When the packaging material is used for preserving foods, particularly fruits and vegetables, water vapor generated in food preservation can be absorbed by the packaging material in time, and can not form coagulation on the foods, so that the foods are easy to deteriorate, the storage time of the foods is effectively prolonged, the coating of the packaging material is firmly adhered, and the coating can not fall off to influence the safety of the foods.
Advantageous effects
1. According to the invention, the polyethylene glycol plasma is used for modifying the surface of one side of the PET, so that the surface energy and wettability of the PET are improved, the bonding force between the PET and the moisture absorption layer is enhanced, and the polyethylene glycol grafting modification on the surface of the PET improves the moisture absorption property of the PET film and can participate in the solidification of the moisture absorption layer, so that the bonding force between the PET film and the moisture absorption layer is further improved; meanwhile, the average molecular weight of polyethylene glycol is controlled, so that the film layer has better bonding effect, and the packaging material has better hygroscopicity;
2. according to the invention, the polyvinyl alcohol coating liquid is coated on the PET modified surface to form the moisture absorption layer, so that the moisture absorption of one side of PET is improved, meanwhile, the polyvinyl alcohol modified diatomite is added, the moisture absorption of the modified diatomite is further improved, the moisture absorption effect is further improved through the combined action of the polyvinyl alcohol and the modified diatomite, and the preferable moisture absorption of the packaging material and the adhesive force of the film layer are realized through controlling the content of the polyvinyl alcohol and the modified diatomite in the system.
3. According to the invention, the cyclodextrin coated antibacterial agent is added into the moisture absorption layer, so that the lasting release of the antibacterial agent is realized, meanwhile, the hydroxyl cyclodextrin has hydrophilicity, participates in the solidification of polyethylene glycol grafted on the surfaces of polyvinyl alcohol and PET, the dispersion of the antibacterial agent in the system is improved, the antibacterial effect is further improved, and the moisture absorption of the packaging material is facilitated.
Detailed Description
The present invention will be described in detail with reference to the following examples, so that those skilled in the art can better understand the present invention, but the present invention is not limited to the following examples.
The polymerization degree of the polyvinyl alcohol is 1700 and the alcoholysis degree is 99 percent; diatomaceous earth was purchased from the company of chemical industry, inc. in the south of the Ji's century and had a particle size of 800 mesh.
Antibacterial agent epsilon-polylysine hydrochloride antibacterial agent from source biotechnology limited of Jiangsu origin; the other raw materials are all conventional commercial products or can be prepared in a conventional preparation mode in the field.
Preparation example 1
Preparation of silane coupling agent modified diatomite: adding 20g of diatomite into 1L of ethanol water solution with the mass concentration of 50%, mixing, performing ultrasonic dispersion for half an hour, adding acetic acid under magnetic stirring (the rotating speed is 350 r/min) to adjust the pH to 4.6, adding 15g of methyltriethoxysilane, heating to 80 ℃, and continuously stirring for reacting for 4 hours; and after the reaction is finished, standing and cooling, filtering, washing with ethanol for 3 times, and drying at 60 ℃ to obtain the silane coupling agent modified diatomite.
Preparation example 2
Preparation of polyvinyl alcohol grafted diatomite: dissolving 20g of polyvinyl alcohol in 500mL of pure water at 95 ℃ to obtain a polyvinyl alcohol solution, adding 6g of the silane coupling agent modified diatomite prepared in preparation example 1 into 50mL of ethanol, stirring for half an hour to obtain a dispersion, adding the dispersion into the polyvinyl alcohol solution, adjusting the temperature to 80 ℃, adding acetic acid to adjust the pH to 4.6, stirring at the rotating speed of 350r/min for 4 hours, cooling after the reaction, centrifuging, filtering, washing with ethanol for 3 times, and drying at 60 ℃ to obtain the polyvinyl alcohol grafted diatomite.
Preparation example 3
Preparation of a hydroxycyclodextrin coated antibacterial agent: 3g of the hydroxy cyclodextrin is added into 100mL of hot alkali solution (preparation: potassium hydroxide 4 g/pure water 1L) with 90 ℃ and stirred for half an hour to obtain cyclodextrin solution; adding 2g of an antibacterial agent into 100mL of ethanol solution, and stirring for half an hour to obtain an antibacterial agent solution; adding the prepared antibacterial agent solution into cyclodextrin solution, heating to 70 ℃ in water bath, performing rotary steaming for 2 hours after reaction, and drying at 60 ℃ to obtain the hydroxyl cyclodextrin coated antibacterial agent.
Example 1
(1) Preparing an ethanol solution (60% of polyethylene glycol by mass) of PEG1000, coating the solution on one side surface of a PET base film for 3 times, standing for 2 hours, drying at 60 ℃, then placing the solution into a plasma treatment device for plasma treatment with the treatment power of 200W for 20min, washing with pure water for 5 times, and drying at 70 ℃;
(2) And coating a moisture absorption coating liquid on one side surface of the grafted polyethylene glycol, and drying and curing at 70 ℃ to obtain the packaging material. The moisture absorption coating liquid comprises the following components: 30 parts of polyvinyl alcohol and 20 parts of diatomite; 3 parts of antibacterial agent, 10 parts of ethanol and 37 parts of pure water; the mixing mode is as follows: adding 30g of polyvinyl alcohol into 37g of pure water, heating to 95 ℃, mixing and stirring for half an hour at a stirring speed of 200r/min, adding 20g of 800-mesh diatomite, stirring for 1 hour, cooling to 45 ℃, adding 3g of antibacterial epsilon-polylysine hydrochloride and 10g of ethanol, and stirring for half an hour to obtain the moisture absorption coating liquid.
Example 2
(1) Preparing an ethanol solution (60% of polyethylene glycol by mass) of PEG1000, coating the solution on one side surface of a PET base film for 3 times, standing for 2 hours, drying at 60 ℃, then placing the solution into a plasma treatment device for plasma treatment with the treatment power of 200W for 20min, washing with pure water for 5 times, and drying at 70 ℃;
(2) And coating a moisture absorption coating liquid on one side surface of the grafted polyethylene glycol, and drying and curing at 70 ℃ to obtain the packaging material. The moisture absorption coating liquid comprises the following components: 35 parts of polyvinyl alcohol and 10 parts of diatomite; 8 parts of antibacterial agent, 5 parts of ethanol and 42 parts of pure water; the mixing mode is as follows: adding 35g of polyvinyl alcohol into 42g of pure water, heating to 95 ℃, mixing and stirring for half an hour at a stirring speed of 200r/min, adding 10g of 800-mesh diatomite, stirring for 1 hour, cooling to 45 ℃, adding 8g of antibacterial agent epsilon-polylysine hydrochloride and 5g of ethanol, and stirring for half an hour to obtain the moisture absorption coating liquid.
Example 3
(1) Preparing an ethanol solution (60% of polyethylene glycol by mass) of PEG1000, coating the solution on one side surface of a PET base film for 3 times, standing for 2 hours, drying at 60 ℃, then placing the solution into a plasma treatment device for plasma treatment with the treatment power of 200W for 20min, washing with pure water for 5 times, and drying at 70 ℃;
(2) And coating a moisture absorption coating liquid on one side surface of the grafted polyethylene glycol, and drying and curing at 70 ℃ to obtain the packaging material. The moisture absorption coating liquid comprises the following components: 32 parts of polyvinyl alcohol and 16 parts of diatomite; 5 parts of antibacterial agent, 7 parts of ethanol and 40 parts of pure water; the mixing mode is as follows: adding 32g of polyvinyl alcohol into 40g of pure water, heating to 95 ℃, mixing and stirring for half an hour at the stirring speed of 200r/min, adding 16g of 800-mesh diatomite, stirring for 1 hour, cooling to 45 ℃, adding 5g of antibacterial agent epsilon-polylysine hydrochloride and 7g of ethanol, and stirring for half an hour to obtain the moisture absorption coating liquid.
Example 4
(1) Preparing an ethanol solution (60% of polyethylene glycol by mass) of PEG1000, coating the solution on one side surface of a PET base film for 3 times, standing for 2 hours, drying at 60 ℃, then placing the solution into a plasma treatment device for plasma treatment with the treatment power of 200W for 20min, washing with pure water for 5 times, and drying at 70 ℃;
(2) And coating a moisture absorption coating liquid on one side surface of the grafted polyethylene glycol, and drying and curing at 70 ℃ to obtain the packaging material. The moisture absorption coating liquid comprises the following components: 32 parts of polyvinyl alcohol and 16 parts of silane coupling agent modified diatomite of preparation example 1; 5 parts of antibacterial agent, 7 parts of ethanol and 40 parts of pure water; the mixing mode is as follows: adding 32g of polyvinyl alcohol into 40g of pure water, heating to 95 ℃, mixing and stirring for half an hour at a stirring speed of 200r/min, adding 16g of silane coupling agent modified diatomite of preparation example 1, stirring for 1 hour, cooling to 45 ℃, adding 5g of antibacterial agent epsilon-polylysine hydrochloride and 7g of ethanol, and stirring for half an hour to obtain the moisture absorption coating liquid.
Example 5
(1) Preparing an ethanol solution (60% of polyethylene glycol by mass) of PEG1000, coating the solution on one side surface of a PET base film for 3 times, standing for 2 hours, drying at 60 ℃, then placing the solution into a plasma treatment device for plasma treatment with the treatment power of 200W for 20min, washing with pure water for 5 times, and drying at 70 ℃;
(2) And coating a moisture absorption coating liquid on one side surface of the grafted polyethylene glycol, and drying and curing at 70 ℃ to obtain the packaging material. The moisture absorption coating liquid comprises the following components: 32 parts of polyvinyl alcohol and 16 parts of polyvinyl alcohol grafted diatomite of preparation example 2; 5 parts of antibacterial agent, 7 parts of ethanol and 40 parts of pure water; the mixing mode is as follows: adding 32g of polyvinyl alcohol into 40g of pure water, heating to 95 ℃, mixing and stirring for half an hour at a stirring speed of 200r/min, adding 16g of polyvinyl alcohol grafted diatomite of preparation example 2, stirring for 1 hour, cooling to 45 ℃, adding 5g of antibacterial agent epsilon-polylysine hydrochloride and 7g of ethanol, and stirring for half an hour to obtain the moisture absorption coating liquid.
Example 6
(1) Preparing an ethanol solution (60% of polyethylene glycol by mass) of PEG1000, coating the solution on one side surface of a PET base film for 3 times, standing for 2 hours, drying at 60 ℃, then placing the solution into a plasma treatment device for plasma treatment with the treatment power of 200W for 20min, washing with pure water for 5 times, and drying at 70 ℃;
(2) And coating a moisture absorption coating liquid on one side surface of the grafted polyethylene glycol, and drying and curing at 70 ℃ to obtain the packaging material. The moisture absorption coating liquid comprises the following components: 48 parts of polyvinyl alcohol, 5 parts of an antibacterial agent, 7 parts of ethanol and 40 parts of pure water; the mixing mode is as follows: 48g of polyvinyl alcohol is added into 40g of pure water, heated to 95 ℃, mixed and stirred for half an hour, the stirring speed is 200r/min, cooled to 45 ℃, 5g of antibacterial agent epsilon-polylysine hydrochloride and 7g of ethanol are added, and the mixture is stirred for half an hour to obtain the moisture absorption coating liquid.
Example 7
(1) Preparing an ethanol solution (60% of polyethylene glycol by mass) of PEG1000, coating the solution on one side surface of a PET base film for 3 times, standing for 2 hours, drying at 60 ℃, then placing the solution into a plasma treatment device for plasma treatment with the treatment power of 200W for 20min, washing with pure water for 5 times, and drying at 70 ℃;
(2) And coating a moisture absorption coating liquid on one side surface of the grafted polyethylene glycol, and drying and curing at 70 ℃ to obtain the packaging material. The moisture absorption coating liquid comprises the following components: 48 parts of polyvinyl alcohol grafted diatomite of preparation example 2; 5 parts of antibacterial agent, 7 parts of ethanol and 40 parts of pure water; the mixing mode is as follows: 48g of polyvinyl alcohol grafted diatomite prepared in preparation example 2 is added into 40g of pure water, heated to 95 ℃, mixed and stirred for 1 hour, the stirring speed is 200r/min, the temperature is reduced to 45 ℃, 5g of antibacterial agent epsilon-polylysine hydrochloride and 7g of ethanol are added, and the mixture is stirred for half an hour to obtain the moisture absorption coating liquid.
Example 8
(1) Preparing an ethanol solution (60% of polyethylene glycol by mass) of PEG1000, coating the solution on one side surface of a PET base film for 3 times, standing for 2 hours, drying at 60 ℃, then placing the solution into a plasma treatment device for plasma treatment with the treatment power of 200W for 20min, washing with pure water for 5 times, and drying at 70 ℃;
(2) And coating a moisture absorption coating liquid on one side surface of the grafted polyethylene glycol, and drying and curing at 70 ℃ to obtain the packaging material. The moisture absorption coating liquid comprises the following components: 42 parts of polyvinyl alcohol and 6 parts of polyvinyl alcohol grafted diatomite of preparation example 2; 5 parts of antibacterial agent, 7 parts of ethanol and 40 parts of pure water; the mixing mode is as follows: adding 42g of polyvinyl alcohol into 40g of pure water, heating to 95 ℃, mixing and stirring for half an hour at a stirring speed of 200r/min, adding 6g of polyvinyl alcohol grafted diatomite of preparation example 2, stirring for 1 hour, cooling to 45 ℃, adding 5g of antibacterial agent epsilon-polylysine hydrochloride and 7g of ethanol, and stirring for half an hour to obtain the moisture absorption coating liquid.
Example 9
(1) Preparing an ethanol solution (60% of polyethylene glycol by mass) of PEG1000, coating the solution on one side surface of a PET base film for 3 times, standing for 2 hours, drying at 60 ℃, then placing the solution into a plasma treatment device for plasma treatment with the treatment power of 200W for 20min, washing with pure water for 5 times, and drying at 70 ℃;
(2) And coating a moisture absorption coating liquid on one side surface of the grafted polyethylene glycol, and drying and curing at 70 ℃ to obtain the packaging material. The moisture absorption coating liquid comprises the following components: 24 parts of polyvinyl alcohol and 24 parts of polyvinyl alcohol grafted diatomite of preparation example 2; 5 parts of antibacterial agent, 7 parts of ethanol and 40 parts of pure water; the mixing mode is as follows: adding 24g of polyvinyl alcohol into 40g of pure water, heating to 95 ℃, mixing and stirring for half an hour at a stirring speed of 200r/min, adding 24g of polyvinyl alcohol grafted diatomite of preparation example 2, stirring for 1 hour, cooling to 45 ℃, adding 5g of antibacterial agent epsilon-polylysine hydrochloride and 7g of ethanol, and stirring for half an hour to obtain the moisture absorption coating liquid.
Example 10
(1) Preparing an ethanol solution (60% of polyethylene glycol by mass) of PEG1000, coating the solution on one side surface of a PET base film for 3 times, standing for 2 hours, drying at 60 ℃, then placing the solution into a plasma treatment device for plasma treatment with the treatment power of 200W for 20min, washing with pure water for 5 times, and drying at 70 ℃;
(2) And coating a moisture absorption coating liquid on one side surface of the grafted polyethylene glycol, and drying and curing at 70 ℃ to obtain the packaging material. The moisture absorption coating liquid comprises the following components: 32 parts of polyvinyl alcohol and 16 parts of diatomite; 5 parts of the hydroxy cyclodextrin coated antibacterial agent prepared in preparation example 3, 7 parts of ethanol and 40 parts of pure water; the mixing mode is as follows: adding 32g of polyvinyl alcohol into 40g of pure water, heating to 95 ℃, mixing and stirring for half an hour at a stirring speed of 200r/min, adding 16g of 800-mesh diatomite, stirring for 1 hour, cooling to 45 ℃, adding 5g of the hydroxycyclodextrin coated antibacterial agent prepared in preparation example 3 and 7g of ethanol, and stirring for half an hour to obtain the moisture absorption coating liquid.
Example 11
(1) Preparing an ethanol solution (60% of polyethylene glycol by mass) of PEG1000, coating the solution on one side surface of a PET base film for 3 times, standing for 2 hours, drying at 60 ℃, then placing the solution into a plasma treatment device for plasma treatment with the treatment power of 200W for 20min, washing with pure water for 5 times, and drying at 70 ℃;
(2) And coating a moisture absorption coating liquid on one side surface of the grafted polyethylene glycol, and drying and curing at 70 ℃ to obtain the packaging material. The moisture absorption coating liquid comprises the following components: 32 parts of polyvinyl alcohol and 16 parts of polyvinyl alcohol grafted diatomite of preparation example 2; 5 parts of the hydroxy cyclodextrin coated antibacterial agent prepared in preparation example 3, 7 parts of ethanol and 40 parts of pure water; the mixing mode is as follows: adding 32g of polyvinyl alcohol into 40g of pure water, heating to 95 ℃, mixing and stirring for half an hour, stirring at a speed of 200r/min, adding 16g of polyvinyl alcohol grafted diatomite of preparation example 2, stirring for 1 hour, cooling to 45 ℃, adding 5g of the hydroxyl cyclodextrin coated antibacterial agent prepared in preparation example 3 and 7g of ethanol, and stirring for half an hour to obtain the moisture absorption coating liquid.
Example 12
(1) Preparing an ethanol solution (60% of polyethylene glycol by mass) of PEG2000, coating the solution on one side surface of a PET base film for 3 times, standing for 2 hours, drying at 60 ℃, then placing the solution into a plasma treatment device for plasma treatment with the treatment power of 200W for 20min, washing with pure water for 5 times, and drying at 70 ℃;
(2) And coating a moisture absorption coating liquid on one side surface of the grafted polyethylene glycol, and drying and curing at 70 ℃ to obtain the packaging material. The moisture absorption coating liquid comprises the following components: 32 parts of polyvinyl alcohol and 16 parts of diatomite; 5 parts of antibacterial agent, 7 parts of ethanol and 40 parts of pure water; the mixing mode is as follows: adding 32g of polyvinyl alcohol into 40g of pure water, heating to 95 ℃, mixing and stirring for half an hour at the stirring speed of 200r/min, adding 16g of 800-mesh diatomite, stirring for 1 hour, cooling to 45 ℃, adding 5g of antibacterial agent epsilon-polylysine hydrochloride and 7g of ethanol, and stirring for half an hour to obtain the moisture absorption coating liquid.
Comparative example 1
And coating a moisture absorption coating liquid on one side surface of the PET base film, and drying and curing at 70 ℃ to obtain the packaging material. The moisture absorption coating liquid comprises the following components: 32 parts of polyvinyl alcohol and 16 parts of diatomite; 5 parts of antibacterial agent, 7 parts of ethanol and 40 parts of pure water; the mixing mode is as follows: 32g of polyvinyl alcohol was added to 40g of pure water and heated to
Mixing and stirring at 95 ℃ for half an hour at a stirring speed of 200r/min, adding 16g of 800-mesh diatomite, stirring for 1 hour, cooling to 45 ℃, adding 5g of antibacterial epsilon-polylysine hydrochloride and 7g of ethanol, and stirring for half an hour to obtain the moisture absorption coating liquid.
Comparative example 2
(1) Putting the PET film into a plasma treatment device for plasma treatment with the treatment power of 200W for 20min, washing with pure water for 5 times, and drying at 70 ℃;
(2) And coating a moisture absorption coating liquid on one side plasma treatment surface, and drying and curing at 70 ℃ to obtain the packaging material. The moisture absorption coating liquid comprises the following components: 32 parts of polyvinyl alcohol and 16 parts of diatomite; 5 parts of antibacterial agent, 7 parts of ethanol and 40 parts of pure water; the mixing mode is as follows: adding 32g of polyvinyl alcohol into 40g of pure water, heating to 95 ℃, mixing and stirring for half an hour at the stirring speed of 200r/min, adding 16g of 800-mesh diatomite, stirring for 1 hour, cooling to 45 ℃, adding 5g of antibacterial agent epsilon-polylysine hydrochloride and 7g of ethanol, and stirring for half an hour to obtain the moisture absorption coating liquid.
Comparative example 3
(1) Putting the PET film into a plasma treatment device for plasma treatment with the treatment power of 200W for 20min, washing with pure water for 5 times, and drying at 70 ℃;
(2) And coating a moisture absorption coating liquid on one side plasma treatment surface, and drying and curing at 70 ℃ to obtain the packaging material. The moisture absorption coating liquid comprises the following components: 32 parts of polyvinyl alcohol and 16 parts of polyvinyl alcohol grafted diatomite of preparation example 2; 5 parts of antibacterial agent, 7 parts of ethanol and 40 parts of pure water; the mixing mode is as follows: adding 32g of polyvinyl alcohol into 40g of pure water, heating to 95 ℃, mixing and stirring for half an hour at a stirring speed of 200r/min, adding 16g of polyvinyl alcohol grafted diatomite of preparation example 2, stirring for 1 hour, cooling to 45 ℃, adding 5g of antibacterial agent epsilon-polylysine hydrochloride and 7g of ethanol, and stirring for half an hour to obtain the moisture absorption coating liquid.
Comparative example 4
(1) Putting the PET film into a plasma treatment device for plasma treatment with the treatment power of 200W for 20min, washing with pure water for 5 times, and drying at 70 ℃;
(2) And coating a moisture absorption coating liquid on one side plasma treatment surface, and drying and curing at 70 ℃ to obtain the packaging material. The moisture absorption coating liquid comprises the following components: 32 parts of polyvinyl alcohol and 16 parts of polyvinyl alcohol grafted diatomite of preparation example 2; 5 parts of the hydroxy cyclodextrin coated antibacterial agent prepared in preparation example 3, 7 parts of ethanol and 40 parts of pure water; the mixing mode is as follows: adding 32g of polyvinyl alcohol into 40g of pure water, heating to 95 ℃, mixing and stirring for half an hour, stirring at a speed of 200r/min, adding 16g of polyvinyl alcohol grafted diatomite of preparation example 2, stirring for 1 hour, cooling to 45 ℃, adding 5g of the hydroxyl cyclodextrin coated antibacterial agent prepared in preparation example 3 and 7g of ethanol, and stirring for half an hour to obtain the moisture absorption coating liquid.
Performance test and test criteria:
peel strength test: the packaging materials prepared in examples 1-12 and comparative examples 1-4 were tested according to GB/T8808-1988 standard.
Water absorption test: the films prepared in examples 1 to 12 and comparative examples 1 to 4 were cut into film samples of 10cm×10cm, the Wq was weighed, the side of the film without the moisture absorption layer was physically fixed and attached to a conventional hydrophobic PET film, and then placed in a constant temperature and humidity cabinet at 25℃and 90% RH so that the moisture absorption layer was brought into contact with the oven environment, removed after 24 hours, and separated from the hydrophobic PET film, and the mass change of the film samples was measured and recorded as Wt, moisture absorption (%) = (Wt-Wq)/Wq×100%.
The results of the test for the hygroscopic packaging materials produced in each example and each comparative example are as follows.
TABLE 1
Peel strength (N/15 mm) Water absorption (%)
Example 1 5.4 19％
Example 2 5.7 20％
Example 3 5.5 22％
Example 4 5.6 23％
Example 5 6.3 26％
Example 6 6.8 17％
Example 7 5.6 21％
Example 8 6.5 22％
Example 9 5.8 24％
Example 10 5.7 23％
Example 11 6.7 29％
Example 12 4.6 20％
Comparative example 1 1.3 15％
Comparative example 2 3.2 18％
Comparative example 3 3.6 20％
Comparative example 4 3.8 21％
As can be seen from examples 1 to 12 and comparative examples 1 to 4, the packaging material prepared by the present invention combines a large interlayer adhesion and excellent hygroscopicity, and as can be seen from examples 3 and comparative example 1, the adhesion between the material layers is improved by plasma treatment of the surface of the PET base film, examples 3, 5, 11 and comparative examples 2 to 4, the surface adhesion after plasma grafting of polyethylene glycol is better, the resulting composite film has a large peel strength, is not liable to peel and fall off, and as can be seen from examples 3 and 12, the molecular weight of the modified polyethylene glycol can obtain better hygroscopicity and peel strength within the ranges defined in the present application;
the test results of examples 3 and 5 show that the polyvinyl alcohol modified diatomite can realize better moisture absorption effect within a low addition range. The test results of examples 5-9 are observed, and analysis shows that when the polyvinyl alcohol grafted diatomite and the polyvinyl alcohol are both present in the moisture absorption coating liquid, the moisture absorption of the material is better than that of the two components which are independently present, so that the beneficial effects of the mixed use of the modified diatomite and the polyvinyl alcohol are proved, and meanwhile, the optimal control of the proportion of the modified diatomite and the polyvinyl alcohol can be realized within the limit of the application. Examples 3, 5, 10 and 11 show that the coating of the antibacterial agent can also improve the peel strength and hygroscopicity to some extent, and the modification of the diatomite and the coating of the antibacterial agent act together to further improve the hygroscopicity and the layer adhesion of the packaging material. It can be found that, compared with the plasma treatment alone, the modified diatomite is modified by polyethylene glycol, so that the interlayer adhesive force of the modified diatomite to a material is improved more, and the interlayer adhesive force and the moisture absorption effect of the packaging material are improved by the combined action of the modification of the polyethylene glycol on the surface and the grafting of the diatomite.
The foregoing are all preferred embodiments of the present application, and are not intended to limit the scope of the present application in any way, therefore: all equivalent changes in structure, shape and principle of this application should be covered in the protection scope of this application.

Claims (10)

1. A packaging material having hygroscopicity, characterized in that: the packaging material at least comprises a PET base film layer and a moisture absorption layer, wherein the surface of the PET base film layer, which is contacted with the moisture absorption layer, is subjected to polyethylene glycol surface modification.
2. The packaging material with hygroscopicity according to claim 1, wherein the polyethylene glycol is surface-modified by the steps of: polyethylene glycol is coated on one side surface of the PET base film, and after plasma treatment, ungrafted polyethylene glycol is removed, and the PET base film is dried.
3. The packaging material having hygroscopicity as set forth in claim 2, wherein: the average molecular weight of the polyethylene glycol is 200-1000.
4. A packaging material having hygroscopicity as claimed in any one of claims 1 to 3, characterized in that: the moisture absorption layer is formed by coating moisture absorption coating liquid, and the moisture absorption coating liquid comprises the following raw materials in parts by weight: 30-35 parts of polyvinyl alcohol; 10-20 parts of modified diatomite; 3-8 parts of an antibacterial agent; 5-10 parts of ethanol; 35-60 parts of water.
5. The hygroscopic packaging material as recited in claim 4 wherein: the modified diatomite is polyvinyl alcohol grafted diatomite, and the preparation method comprises the following steps: adding diatomite into an ethanol water solution, regulating the pH value, adding a silane coupling agent, heating to 70-100 ℃, and reacting for 3-6 hours; washing with an organic solvent, and drying to obtain silane coupling agent modified diatomite; adding the modified diatomite into a polyvinyl alcohol aqueous solution, heating to 70-100 ℃, reacting for 0.5-6h, centrifuging, filtering, washing with an organic solvent, and drying to obtain the polyvinyl alcohol grafted diatomite.
6. The hygroscopic packaging material as recited in claim 4 wherein: the antibacterial agent is a hydroxyl cyclodextrin coated antibacterial agent.
7. The hygroscopic packaging material as recited in claim 6 wherein: the preparation method of the hydroxy cyclodextrin coated antibacterial agent comprises the following steps: adding hydroxy cyclodextrin into the hot alkaline solution to obtain cyclodextrin solution; adding an antibacterial agent into an alcohol solvent to obtain an antibacterial agent solution; adding the prepared antibacterial agent solution into cyclodextrin solution, heating in 50-80deg.C water bath, performing rotary evaporation after reaction, and oven drying to obtain hydroxy cyclodextrin coated antibacterial agent.
8. A method for producing a packaging material having hygroscopicity as set forth in any one of claims 1 to 7, comprising the steps of:
(1) Coating polyethylene glycol on one side surface of a PET base film, removing ungrafted polyethylene glycol after plasma treatment, and drying;
(2) And (3) coating the surface modified by the polyethylene glycol in the step (1) with a hygroscopic coating liquid, and curing to obtain the hygroscopic packaging material.
9. The method for producing a packaging material having hygroscopicity as claimed in claim 8, further comprising the step (3): a hydrophobic layer and/or an oleophobic layer is arranged on one side of the PET base film far away from the hygroscopic layer.
10. Use of a packaging material having hygroscopicity in packaging and storage of food, characterized in that: the packaging material is the packaging material having hygroscopicity as described in any one of claims 1 to 7.
CN202311495476.2A 2023-11-10 2023-11-10 Packaging material with hygroscopicity and preparation method and application thereof Pending CN117487225A (en)

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