CN111073526A - Fast-positioning two-component acrylate structural adhesive and preparation and use methods thereof - Google Patents
Fast-positioning two-component acrylate structural adhesive and preparation and use methods thereof Download PDFInfo
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- CN111073526A CN111073526A CN201911335720.2A CN201911335720A CN111073526A CN 111073526 A CN111073526 A CN 111073526A CN 201911335720 A CN201911335720 A CN 201911335720A CN 111073526 A CN111073526 A CN 111073526A
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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
- C09J4/00—Adhesives based on organic non-macromolecular compounds having at least one polymerisable carbon-to-carbon unsaturated bond ; adhesives, based on monomers of macromolecular compounds of groups C09J183/00 - C09J183/16
- C09J4/06—Organic non-macromolecular compounds having at least one polymerisable carbon-to-carbon unsaturated bond in combination with a macromolecular compound other than an unsaturated polymer of groups C09J159/00 - C09J187/00
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
- C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
- C08G59/40—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the curing agents used
- C08G59/50—Amines
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
- C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
- C08G59/40—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the curing agents used
- C08G59/66—Mercaptans
-
- 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
- C09J11/04—Non-macromolecular additives inorganic
Abstract
The invention discloses a fast-positioning two-component acrylate structural adhesive and a preparation and use method thereof, wherein the adhesive comprises A, B two components, acrylate structural adhesive and epoxy structural adhesive are organically combined together in a blending mode, and thiol curing agents, epoxy resin and epoxy latent curing agents are added into different components to promote the reaction of the three components. When the A, B components are mixed according to the volume ratio of 10:1, the mixture is used, the storage is stable at normal temperature, and the operation time is long; the thiol curing agent of the component A can be initiated to react with the epoxy resin of the component B by low-temperature heating, so that the rapid positioning effect is achieved, the generated heat further initiates an acrylic acid system to react to form an interpenetrating network structure, the acrylate structural adhesive and the epoxy structural adhesive are organically combined, the adjustable range of the raw materials is large, and the structural adhesive with excellent comprehensive performance is obtained by blending modification.
Description
Technical Field
The invention belongs to the field of acrylic acid structural adhesives, and particularly relates to a fast-positioning two-component acrylate structural adhesive.
Background
The second generation acrylate structural adhesive can be cured at room temperature, has simple and convenient operation process and wide bonding range, is suitable for bonding most metals and non-metallic materials, has low surface treatment requirement and can even be bonded on oil surface. 100 percent of solid content, small curing shrinkage, high peeling strength, impact resistance and better weather resistance strength, and structurally bonds the halogen-free metal structural adhesive. Because the solvent-free halogen-free structural adhesive is solvent-free, the adhesive is widely applied to bonding and fixing electronic assemblies, handheld products, communication equipment, automobile manufacturing, rail transit, elevators, ships, mobile phone/notebook shells and tablet computers. Along with the rapid development of the electronic communication industry in recent years, the application of the shell of the mobile phone/notebook computer is increasingly wide. In order to respond to national energy-saving and high-efficiency requirements, reduce the heat damage to precision components at high temperature and accelerate the assembly efficiency, the requirement on the positioning speed of glue is higher and higher, and the low-temperature rapid positioning becomes a new requirement of the industry.
The conventional method for accelerating positioning usually adopts high-activity monomers or resins with active groups, but under the condition of improving the positioning speed, the room-temperature operation time is correspondingly shortened, and the operation difficulty is increased.
Disclosure of Invention
In order to solve the problems, the invention provides the two-component acrylate adhesive which has long room temperature operation time, is quickly heated and positioned and has higher bonding strength after being cured.
In order to realize the technical effects, the invention discloses a fast-positioning two-component acrylate structural adhesive which comprises A, B two components,
wherein the component A comprises the following components in percentage by mass:
the component B comprises the following components in percentage by mass:
furthermore, the latent curing agent in the component B is an ultralow-temperature latent curing agent of modified amines.
Further, the epoxy curing agent in the component A is as follows: a thiol curing agent.
Further, the acrylate monomer is selected from: two or more of methyl methacrylate, hydroxyethyl methacrylate, hydroxypropyl methacrylate, tetrahydrofurfuryl acrylate, cyclohexyl acrylate, dicyclopentadiene acrylate, cyclotrimethylolpropane methylal acrylate, trimethylolpropane triacrylate dipentaerythritol pentaacrylate triethylene glycol dimethacrylate and ethoxylated trimethylolpropane triacrylate;
the functional monomer is selected from: one of methacrylic acid, acrylic acid and maleic acid.
Further, the toughening agent is selected from: two or more of ABS, MBS, hydrogenated nitrile rubber, hydroxyl-terminated nitrile rubber, rosin resin, epoxy modified acrylic resin, polyurethane modified acrylic resin, styrene-butadiene rubber and polyacrylate rubber are mixed;
the promoter is selected from: one or more of N, N-dimethyl-p-toluidine, N-diethyl-p-toluidine, N-dihydroxyethyl-p-toluidine, vinyl thiourea and tetramethyl thiourea;
the auxiliary accelerator is selected from: one or more of triphenylphosphine, zinc diethyldithiocarbamate, zinc acrylate and zinc methacrylate;
the stabilizer is selected from: one or more of hydroquinone, benzoquinone, naphthoquinone, EDTA-Na, p-hydroxyanisole, 2-tert-butylhydroquinone and 2, 6-di-tert-butyl-4-methylphenol;
the auxiliary agent is selected from: one or more of PM-2, PM1590 PM2010SP 4051.
Further, the initiator of the component B is benzoyl peroxide;
the component B plasticizer is selected from: one or more of dipropylene glycol dibenzoate, diethylene glycol dibenzoate, dipropylene glycol dibenzoate, dioctyl adipate and dioctyl sebacate;
the component B epoxy resin is selected from: one of bisphenol A epoxy resin, bisphenol F epoxy resin and polyfunctional group modified epoxy resin.
The invention also discloses a preparation method of the fast-positioning two-component acrylate structural adhesive, which comprises the following steps: in that A, B components are prepared separately;
preparation of the component A: accurately weighing an acrylate monomer, a functional monomer and a stabilizer, and uniformly mixing; then adding a toughening agent, and stirring to completely dissolve the toughening agent; adding the accelerant, the promoter, the auxiliary agent and the epoxy curing agent, stirring uniformly, carrying out vacuum pressure maintaining defoaming, and discharging to obtain the component A.
B, preparation of a component: accurately weighing the plasticizer, the initiator and the epoxy resin, fully stirring to completely dissolve the plasticizer, the initiator and the epoxy resin, adding the latent curing agent and the pigment, uniformly stirring, finally defoaming in vacuum, and discharging to obtain the component B.
In addition, the invention also discloses a use method of the fast-positioning two-component acrylate structural adhesive, which comprises the following steps: and evenly mixing the A, B components according to the volume ratio of 10:1 to obtain the acrylate structure adhesive.
It is further characterized by the use of low temperature heating to initiate the curing reaction.
The invention has the beneficial effects that:
the acrylate structural adhesive and the epoxy structural adhesive are organically combined together by adopting a blending mode, a thiol curing agent, epoxy resin and an epoxy latent curing agent are added into different components, so that the three components are mutually promoted to react, the modified amine ultralow-temperature latent curing agent is used as the epoxy resin latent curing agent and is also a curing accelerator, and active hydrogen on the molecular structure of the curing accelerator has the function of curing catalyst functional groups. When A, B components are mixed, the storage is stable at normal temperature, and the operation time is long; the thiol curing agent of the component A can be initiated to react with the epoxy resin of the component B by low-temperature heating, so that the rapid positioning effect is achieved, the generated heat further initiates an acrylic acid system to react to form an interpenetrating network structure, the acrylate structural adhesive and the epoxy structural adhesive are organically combined, the adjustable range of the raw materials is large, and the structural adhesive with excellent comprehensive performance is obtained by blending modification.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the embodiments of the present invention. It is to be understood that the embodiments described are only a few embodiments of the present invention, and not all embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Example 1
Component A
B component
| Name of the component | Component amounts |
| Diethylene glycol dibenzoate | 30 |
| Benzoyl peroxide | 32 |
| Bisphenol A epoxy resin | 30 |
| Modified amine latent curing agent | 5 |
| Pigment (I) | 3 |
The preparation process comprises the following steps:
preparation of the component A: accurately weighing methyl methacrylate, hydroxyethyl methacrylate, tetrahydrofuran acrylate, methacrylic acid, hydroquinone and EDTA-Na, and uniformly mixing; then adding ABS resin and hydrogenated nitrile rubber, and stirring to completely dissolve the ABS resin and the hydrogenated nitrile rubber; adding polyurethane modified acrylic resin, N-dimethyl-p-toluidine, zinc diethyldithiocarbamate, PM-2 and mercaptan curing agent, stirring uniformly, adding fumed silica, stirring uniformly, vacuum pressure maintaining and defoaming, and discharging to obtain the component A.
B, preparation of a component: accurately weighing diethylene glycol dibenzoate, benzoyl peroxide and bisphenol A epoxy resin, fully stirring to completely dissolve the diethylene glycol dibenzoate, adding the modified amine latent curing agent and the pigment, uniformly stirring, finally defoaming in vacuum, and discharging to obtain the component B.
And evenly mixing A, B components according to the volume ratio of 10:1 to obtain the acrylate structural adhesive.
Example 2
Component A
B component
| Name of the component | Component amounts |
| Dioctyl adipate | 30 |
| Benzoyl peroxide | 32 |
| Bisphenol F epoxy resin | 30 |
| Modified amine latent curing agent | 5 |
| Pigment (I) | 3 |
The preparation process comprises the following steps:
preparation of the component A: accurately weighing methyl methacrylate, hydroxypropyl methacrylate, tetrahydrofuran acrylate, methacrylic acid, 2-tert-butylhydroquinone and EDTA-Na, and uniformly mixing; then adding MBS resin and polyacrylate rubber, and stirring to completely dissolve the MBS resin and the polyacrylate rubber; adding epoxy modified acrylic resin, N-dihydroxyethyl p-toluidine, triphenylphosphine, PM-2010SP and mercaptan, stirring uniformly, finally adding fumed silica, stirring uniformly, carrying out vacuum pressure maintaining defoaming, and discharging to obtain the component A.
B, preparation of a component: accurately weighing dioctyl adipate, benzoyl peroxide and bisphenol F epoxy resin, fully stirring to completely dissolve the dioctyl adipate, the benzoyl peroxide and the bisphenol F epoxy resin, adding the modified amine latent curing agent and the pigment, uniformly stirring, finally defoaming in vacuum, and discharging to obtain the component B. And evenly mixing A, B components according to the volume ratio of 10:1 to obtain the acrylate structural adhesive.
Comparative example one:
component A
B component
| Name of the component | Component amounts |
| Diethylene glycol dibenzoate | 32 |
| Benzoyl peroxide | 34 |
| Bisphenol A epoxy resin | 31 |
| Pigment (I) | 3 |
The preparation process comprises the following steps:
preparation of the component A: accurately weighing methyl methacrylate, hydroxyethyl methacrylate, cyclotrimethylolpropane methylal acrylate, tetraethyleneglycol dimethacrylate, methacrylic acid, hydroquinone and EDTA-Na, and uniformly mixing; then adding ABS resin and chloroprene rubber, stirring to make them completely dissolve; adding polyurethane modified acrylic resin, N-dimethyl-p-toluidine, zinc diethyldithiocarbamate and PM-2, stirring uniformly, finally adding fumed silica, stirring uniformly, carrying out vacuum pressure maintaining defoaming, and discharging to obtain the component A.
B, preparation of a component: accurately weighing diethylene glycol dibenzoate, benzoyl peroxide and bisphenol A epoxy resin, fully stirring to completely dissolve the diethylene glycol dibenzoate, adding pigment, uniformly stirring, finally performing vacuum defoaming, and discharging to obtain the component B.
And evenly mixing A, B components according to the volume ratio of 10:1 to obtain the acrylate structural adhesive.
Comparative example two:
component A
B component
| Name of the component | Component amounts |
| Dioctyl adipate | 32 |
| Benzoyl peroxide | 34 |
| Bisphenol F epoxy resin | 31 |
| Pigment (I) | 3 |
The preparation process comprises the following steps:
preparation of the component A: accurately weighing methyl methacrylate, hydroxypropyl methacrylate, dipentaerythritol pentaacrylate, ethoxylated trimethylolpropane triacrylate, 2-tert-butyl hydroquinone and EDTA-Na, and uniformly mixing; then adding MBS resin and polyacrylate rubber, and stirring to completely dissolve the MBS resin and the polyacrylate rubber; adding epoxy modified acrylic resin, N-dihydroxyethyl-p-toluidine, triphenylphosphine and PM-2010SP, stirring uniformly, finally adding fumed silica, stirring uniformly, carrying out vacuum pressure maintaining defoaming, and discharging to obtain the component A.
B, preparation of a component: accurately weighing dioctyl adipate, benzoyl peroxide and bisphenol F epoxy resin, fully stirring to completely dissolve, uniformly stirring pigment, finally defoaming in vacuum, and discharging to obtain the component B.
And evenly mixing A, B components according to the volume ratio of 10:1 to obtain the acrylate structural adhesive.
According to the GB/T7124-2008 tensile shear test standard, the tensile shear strength of the aluminum alloy and the aluminum alloy, the aluminum alloy and the PC (containing 30 percent of glass fiber) are tested.
The positioning time testing method comprises the following steps: and placing the rear shell of the mobile phone and a PC (containing 30% of glass fiber) sample piece for testing at the positioning temperature to be measured, and pre-baking for 30 min. Setting a hot press machine to be the positioning temperature to be measured, installing a glue outlet (No. 20 needle head) on the filled finished product, dispensing on a mobile phone rear shell (dispensing amount is 0.05g) by using an automatic dispenser, quickly covering a PC (containing 30% of glass fiber), pressing by the hot press machine, and measuring the time when the thrust is more than 10kg, namely the positioning time.
The operation time testing method comprises the following steps: and (3) gluing the finished product with the glue outlet nozzle, using a glue gun to spray a small amount of glue to ensure that A, B components are uniformly mixed, putting the glue into a 25 ℃ oven, and simultaneously pressing a stopwatch to start timing. And recording the time when the glue can not be applied, namely the operation time of the glue mixing head.
The test data are shown in the following table:
note: examples 1 and 2 are acrylate structural adhesives according to the present invention, and comparative examples 1 and 2 are conventional acrylate structural adhesives.
As can be seen from the data in the table: the acrylate structural adhesive has the advantages that the room temperature operation time is long while the high tensile and shearing strength is kept, the positioning time is obviously faster than that of a certain brand sold in comparative examples 1-2 and domestic markets within the temperature range of 50-90 ℃, and the positioning is faster than that of a certain brand known internationally at certain temperature. The assembling efficiency can be obviously improved, and the heat damage to the precise element device at high temperature is reduced.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents, improvements and the like made within the spirit and principles of the present invention are within the scope of the present invention.
Claims (9)
1. A fast-positioning two-component acrylate structural adhesive is characterized in that: comprises A, B two components, namely a water-soluble polymer,
wherein the component A comprises the following components in percentage by mass:
the component B comprises the following components in percentage by mass:
2. the fast-positioning two-component acrylate structural adhesive according to claim 1, wherein: the latent curing agent in the component B is an ultralow-temperature latent curing agent of modified amines.
3. The fast-positioning two-component acrylate structural adhesive according to claim 1, wherein: the epoxy curing agent in the component A is as follows: a thiol curing agent.
4. The fast-positioning two-component acrylate structural adhesive according to claim 1, wherein:
the acrylic ester monomer is selected from: two or more of methyl methacrylate, hydroxyethyl methacrylate, hydroxypropyl methacrylate, tetrahydrofurfuryl acrylate, cyclohexyl acrylate, dicyclopentadiene acrylate, cyclotrimethylolpropane methylal acrylate, trimethylolpropane triacrylate dipentaerythritol pentaacrylate triethylene glycol dimethacrylate and ethoxylated trimethylolpropane triacrylate;
the functional monomer is selected from: one of methacrylic acid, acrylic acid and maleic acid.
5. The fast-positioning two-component acrylate structural adhesive according to claim 1, wherein: the toughening agent is selected from: two or more of ABS, MBS, hydrogenated nitrile rubber, hydroxyl-terminated nitrile rubber, rosin resin, epoxy modified acrylic resin, polyurethane modified acrylic resin, styrene-butadiene rubber and polyacrylate rubber are mixed;
the promoter is selected from: one or more of N, N-dimethyl-p-toluidine, N-diethyl-p-toluidine, N-dihydroxyethyl-p-toluidine, vinyl thiourea and tetramethyl thiourea;
the auxiliary accelerator is selected from: one or more of triphenylphosphine, zinc diethyldithiocarbamate, zinc acrylate and zinc methacrylate;
the stabilizer is selected from: one or more of hydroquinone, benzoquinone, naphthoquinone, EDTA-Na, p-hydroxyanisole, 2-tert-butylhydroquinone and 2, 6-di-tert-butyl-4-methylphenol;
the auxiliary agent is selected from: one or more of PM-2, PM1590 PM2010SP 4051.
6. The fast-positioning two-component acrylate structural adhesive according to claim 1, wherein: the initiator of the component B is benzoyl peroxide;
the component B plasticizer is selected from: one or more of dipropylene glycol dibenzoate, diethylene glycol dibenzoate, dipropylene glycol dibenzoate, dioctyl adipate and dioctyl sebacate;
the component B epoxy resin is selected from: one of bisphenol A epoxy resin, bisphenol F epoxy resin and polyfunctional group modified epoxy resin.
7. The preparation method of the fast-positioning two-component acrylate structural adhesive according to any one of claims 1 to 6, which comprises the following steps: it is characterized in that A, B components are respectively prepared;
preparation of the component A: accurately weighing an acrylate monomer, a functional monomer and a stabilizer, and uniformly mixing; then adding a toughening agent, and stirring to completely dissolve the toughening agent; adding the accelerant, the promoter, the auxiliary agent and the epoxy curing agent, stirring uniformly, carrying out vacuum pressure maintaining defoaming, and discharging to obtain the component A.
B, preparation of a component: accurately weighing the plasticizer, the initiator and the epoxy resin, fully stirring to completely dissolve the plasticizer, the initiator and the epoxy resin, adding the latent curing agent and the pigment, uniformly stirring, finally defoaming in vacuum, and discharging to obtain the component B.
8. The use method of the fast-positioning two-component acrylate structural adhesive according to any one of claims 1 to 6 comprises the following steps: the acrylate structural adhesive is characterized in that A, B components are uniformly mixed according to the volume ratio of 10:1 to obtain the acrylate structural adhesive.
9. The use method of the fast-positioning two-component acrylate structural adhesive according to claim 8, wherein: the reaction of the epoxy system in the system is initiated by low-temperature heating to achieve the effect of quick positioning.
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Cited By (6)
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| CN112040387A (en) * | 2020-09-01 | 2020-12-04 | 昆山联滔电子有限公司 | Telephone receiver and preparation method thereof, and loudspeaker and preparation method thereof |
| CN112694839A (en) * | 2020-12-31 | 2021-04-23 | 烟台泰盛精化科技有限公司 | Low-odor acrylate structural adhesive and preparation method thereof |
| CN112778942A (en) * | 2021-01-29 | 2021-05-11 | 厦门韦尔通科技有限公司 | Bi-component acrylate structural adhesive capable of being rapidly cured by hot pressing and long in operable time after being mixed at normal temperature and preparation method thereof |
| CN114231185A (en) * | 2021-12-15 | 2022-03-25 | 武汉市科达云石护理材料有限公司 | Seam beautifying agent capable of quickly curing system and preparation method and application thereof |
| CN114231186A (en) * | 2021-12-15 | 2022-03-25 | 武汉市科达云石护理材料有限公司 | Fast-curing modified dry-hanging adhesive and preparation method and application thereof |
| CN115368849A (en) * | 2021-05-20 | 2022-11-22 | 中国科学院福建物质结构研究所 | Anisotropic conductive adhesive film and preparation method and application thereof |
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Cited By (8)
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| CN112040387A (en) * | 2020-09-01 | 2020-12-04 | 昆山联滔电子有限公司 | Telephone receiver and preparation method thereof, and loudspeaker and preparation method thereof |
| CN112694839A (en) * | 2020-12-31 | 2021-04-23 | 烟台泰盛精化科技有限公司 | Low-odor acrylate structural adhesive and preparation method thereof |
| CN112694839B (en) * | 2020-12-31 | 2023-01-31 | 烟台泰盛精化科技有限公司 | Low-odor acrylate structural adhesive and preparation method thereof |
| CN112778942A (en) * | 2021-01-29 | 2021-05-11 | 厦门韦尔通科技有限公司 | Bi-component acrylate structural adhesive capable of being rapidly cured by hot pressing and long in operable time after being mixed at normal temperature and preparation method thereof |
| CN115368849A (en) * | 2021-05-20 | 2022-11-22 | 中国科学院福建物质结构研究所 | Anisotropic conductive adhesive film and preparation method and application thereof |
| CN115368849B (en) * | 2021-05-20 | 2023-10-03 | 中国科学院福建物质结构研究所 | Anisotropic conductive adhesive film and preparation method and application thereof |
| CN114231185A (en) * | 2021-12-15 | 2022-03-25 | 武汉市科达云石护理材料有限公司 | Seam beautifying agent capable of quickly curing system and preparation method and application thereof |
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Application publication date: 20200428 |