CN114456563B - PLA-based heat shrinkable film and preparation method thereof - Google Patents

PLA-based heat shrinkable film and preparation method thereof Download PDF

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CN114456563B
CN114456563B CN202210260172.7A CN202210260172A CN114456563B CN 114456563 B CN114456563 B CN 114456563B CN 202210260172 A CN202210260172 A CN 202210260172A CN 114456563 B CN114456563 B CN 114456563B
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pla
film
eea
based heat
temperature
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CN114456563A (en
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宋璐
李娟�
罗珊珊
高成涛
孙静
黄绍文
张黎
王彦文
李剑
单艳茹
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Guizhou Material Industrial Technology Research Institute
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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
    • C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
    • C08J5/18—Manufacture of films or sheets
    • 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
    • C08J3/00—Processes of treating or compounding macromolecular substances
    • C08J3/24—Crosslinking, e.g. vulcanising, of macromolecules
    • C08J3/246—Intercrosslinking of at least two polymers
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J2367/00—Characterised by the use of polyesters obtained by reactions forming a carboxylic ester link in the main chain; Derivatives of such polymers
    • C08J2367/04—Polyesters derived from hydroxy carboxylic acids, e.g. lactones
    • 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
    • C08J2423/00—Characterised by the use of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Derivatives of such polymers
    • C08J2423/02—Characterised by the use of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Derivatives of such polymers not modified by chemical after treatment
    • C08J2423/04—Homopolymers or copolymers of ethene
    • C08J2423/08—Copolymers of ethene
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
    • Y02W90/00—Enabling technologies or technologies with a potential or indirect contribution to greenhouse gas [GHG] emissions mitigation
    • Y02W90/10—Bio-packaging, e.g. packing containers made from renewable resources or bio-plastics

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Materials Engineering (AREA)
  • Shaping By String And By Release Of Stress In Plastics And The Like (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Biological Depolymerization Polymers (AREA)

Abstract

The invention discloses a PLA-based heat shrinkable film and a preparation method thereof, wherein the PLA-based heat shrinkable film comprises, by mass, 85-90 parts of PLA, 5-15 parts of EEA, 0.1-0.5 part of an opening agent, 0.1-0.5 part of a light stabilizer and 0.2-0.4 part of a cross-linking agent. The invention mixes PLA, EEA, cross linker and so on, makes PLA and EEA generate chemical reaction, improves the interface performance between PLA and EEA, thus improves the shrinkage performance and shock resistance of PLA, keeps the transparency of PLA at the same time, expands the application of biodegradable plastic PLA in the field of heat shrinkage film.

Description

PLA-based heat shrinkable film and preparation method thereof
Technical Field
The invention belongs to the technical field of plastic film packaging, and particularly relates to a PLA-based heat shrinkable film and a preparation method thereof.
Background
The heat shrinkable film is a packaging film which generates a shrinking force to wrap goods after being heated, thereby achieving the effect of protecting the packaged goods. The shrinking mechanism of the heat shrinkable film is mainly that after the high polymer is completely plasticized and extruded to form a film, the film is stretched in a certain proportion along the longitudinal direction and the transverse direction between the glass transition temperature and the viscous flow temperature to enable molecular chains of the polymer to be oriented along the stretching direction, and then the film is quenched to enable strain generated by stretching orientation to be 'frozen'; when the film is re-applied
When the film is heated to the thawing temperature, the oriented molecular chains are subjected to disorientation and are recovered to the folding chains in a relaxed state before orientation, so that the heat shrinkable film is endowed with good shrinkage performance. The heat shrinkable film has good sealing, moisture-proof, pollution-proof, puncture-proof, heat-sealing, transparency and portability, and is active in various packaging markets. The current mainstream heat shrinkable films in the market comprise PE, PETG, PET, PVC, PS, PP and the like, which are traditional petroleum-based materials and have the problems of shortage of petroleum resources, aggravation of environmental pollution and the like, so that the environment-friendly bio-based degradable plastic has become the current development trend.
Among biodegradable plastics, polylactic acid (PLA) is one of the most valuable biodegradable polymers in the market, which has good mechanical properties and excellent optical clarity. However, as application of heat shrinkable films, improvement of heat shrinkability and impact strength is required, and blending with flexible polymers or elastomeric polymers is one of effective methods for developing polylactic acid applications.
The patent CN108822515A discloses a preparation method of a PLA heat shrinkable film, which takes PLA as a main raw material, adopts dibutyl diglycol adipate to compound polyethylene oxide with a specific molecular weight as a heat shrinkage modifier, changes the high-temperature motion capability of a polylactic acid molecular chain, and improves the high-temperature heat shrinkage capability of a polylactic acid film.
The patent CN113789039A discloses a biodegradable polyester heat-shrinkable film and a preparation method thereof, PLA and PBAT are used as main base materials, glycidyl methacrylate grafting and function-adjusting degradable master batches are introduced, so that the improvement of the orientation movement capability of a base material molecular chain is facilitated, and the film material has good heat-shrinkage.
However, the heat shrinkable films obtained by the above prior art still have problems of poor impact resistance and heat shrinkage properties.
Disclosure of Invention
This section is for the purpose of summarizing some aspects of embodiments of the invention and to briefly introduce some preferred embodiments. In this section, as well as in the abstract and the title of the invention of this application, simplifications or omissions may be made to avoid obscuring the purpose of the section, the abstract and the title, and such simplifications or omissions are not intended to limit the scope of the invention.
The present invention has been made in view of the above and/or the problems of the prior art that PLA is used for heat shrinkable films to have poor impact resistance and heat shrinkage properties.
One of the purposes of the present invention is to provide a PLA-based heat-shrinkable film, which is prepared by adding EEA transparent masterbatch, a cross-linking agent, a light stabilizer, an opening agent, etc. to PLA as a base material, and has high transparency, good heat-shrinkability and impact resistance.
In order to solve the technical problems, the invention provides the following technical scheme: a heat shrinkable film based on PLA comprises, by mass, 85-90 parts of PLA, 5-15 parts of EEA, 0.1-0.5 part of an opening agent, 0.1-0.5 part of a light stabilizer and 0.2-0.4 part of a cross-linking agent.
As a preferable aspect of the PLA-based heat shrinkable film of the present invention, wherein: the EA content in the EEA is one or more of 15.0%, 18.5% and 19.5%.
As a preferable aspect of the PLA-based heat shrinkable film of the present invention, wherein: the opening agent is one or more of oleamide, talcum powder and silicon dioxide.
As a preferable aspect of the PLA-based heat shrinkable film of the present invention, wherein: the light stabilizer is one or more of Chimassorb 2020FDL, Chimassor 944 and TINUVIN 326.
As a preferable aspect of the PLA-based heat shrinkable film of the present invention, wherein: the cross-linking agent is one or the combination of BIPB and TMAIC.
It is another object of the present invention to provide a method for preparing a PLA-based heat shrinkable film as set forth in any one of the above, comprising,
drying the PLA and EEA;
mixing PLA, EEA, an opening agent, a cross-linking agent and a light stabilizer in proportion to obtain a mixed material;
extruding, bracing, cooling and dicing the mixed material to prepare PLA modified resin particles;
blowing, cooling and rolling the PLA modified resin particles to prepare a modified PLA film;
the modified PLA film is stretched and immediately cooled, maintaining the shape and size of the stretched film.
As a preferable aspect of the preparation method of the PLA-based heat shrinkable film of the present invention, wherein: the PLA and the EEA are dried at the drying temperature of 60 ℃ for 6 hours.
As a preferable aspect of the preparation method of the PLA-based heat shrinkable film of the present invention, wherein: and extruding the mixed material, and adding the mixed material into a double-screw extruder, wherein the temperature of a feed inlet of the double-screw extruder is 90-120 ℃, and the temperature of two to five zones is 160-195 ℃.
As a preferable aspect of the preparation method of the PLA-based heat shrinkable film of the present invention, wherein: and blowing the PLA modified resin particles by using a single-screw film blowing machine, wherein the temperature of a feed inlet of the single-screw film blowing machine is 135-140 ℃, and the temperature of the rest temperature sections is 165-195 ℃.
As a preferable aspect of the preparation method of the PLA-based heat shrinkable film of the present invention, wherein: the modified PLA film was stretched by a uniaxial stretcher having a draw ratio of 4 at 80 ℃.
Compared with the prior art, the invention has the following beneficial effects:
the invention takes PLA as a substrate material, and EEA transparent master batch, cross-linking agent, light stabilizer, opening agent and the like are added to prepare the packaging film with high transparency, good heat shrinkage and impact resistance, wherein EEA is ethylene-ethyl acrylate copolymer, has good toughness, flexibility, bending resistance and high-temperature heat stability, and can also be used for food contact; the EEA and the PLA are melt blended, and chemical crosslinking is performed between the EEA and the PLA, so that the interfacial property between the PLA and the EEA is improved to a certain extent, the impact strength and the heat shrinkage property of the PLA are further improved, and the application of polylactic acid in the field of heat shrinkage films is expanded.
Detailed Description
In order to make the aforementioned objects, features and advantages of the present invention more comprehensible, embodiments accompanying the present invention are described in detail below with reference to examples.
In the following description, numerous specific details are set forth in order to provide a thorough understanding of the present invention, but the present invention may be practiced in other ways than those specifically described and will be readily apparent to those of ordinary skill in the art without departing from the spirit of the present invention, and therefore the present invention is not limited to the specific embodiments disclosed below.
Furthermore, reference herein to "one embodiment" or "an embodiment" means that a particular feature, structure, or characteristic described in connection with the embodiment is included in at least one implementation of the invention. The appearances of the phrase "in one embodiment" in various places in the specification are not necessarily all referring to the same embodiment, nor are separate or alternative embodiments mutually exclusive of other embodiments.
The raw materials used in the examples were all purchased commercially unless otherwise specified.
Example 1
(1) Drying 87 parts of PLA and 12 parts of EEA (EA content 18.5%) at 60 ℃ for 6 h;
(2) then adding the mixture, 0.4 part of opening agent, 0.4 part of light stabilizer and 0.2 part of cross-linking agent into a mixer, and stirring for 5min at 500rmp to obtain a mixed material;
(3) adding the mixed material into a feeding port of a double-screw extruder, wherein the temperature of the feeding port is 110 ℃, the temperature of two to five zones is 190 ℃, and extruding, drawing strips, cooling and cutting into granules to obtain PLA modified resin granules;
(4) adding the PLA modified particles into a single-screw film blowing machine, and performing film blowing to obtain a PLA film, wherein the temperature of a feed inlet of the single-screw film blowing machine is 135 ℃, and the temperatures of the rest sections are 175-195 ℃;
(5) the modified PLA film was subjected to uniaxial stretching at a temperature of 80 ℃ and a stretching ratio of 4 using a hot stretcher (model HY-0230, Shanghai) and then immediately cooled to maintain the shape and size of the stretched film.
Example 2
(1) PLA 91 parts and EEA 8(EA content 18.5%) parts are dried at 60 ℃ for 6 h;
(2) then adding the mixture, 0.4 part of opening agent, 0.4 part of light stabilizer and 0.2 part of cross-linking agent into a mixer, and stirring for 5min at 500rmp to obtain a mixed material;
(3) adding the mixed material into a feeding port of a double-screw extruder, wherein the temperature of the feeding port is 100 ℃, the temperature of two to five zones is 190 ℃, and extruding, drawing strips, cooling and cutting into granules to obtain PLA modified resin granules;
(4) adding the PLA modified particles into a single-screw film blowing machine, and performing film blowing to obtain a PLA film, wherein the temperature of a feed inlet of the single-screw film blowing machine is 135 ℃, and the temperatures of the rest sections are 175-190 ℃;
(5) the subsequent hot stretching conditions were the same as in example 1.
Example 3
(1) Drying 94 parts of PLA and 5 parts of EEA (two EEAs with EA content of 15% and 19.5% are mixed at a ratio of 5: 5) at 60 deg.C for 6 h;
(2) then adding the mixture, 0.4 part of opening agent, 0.4 part of light stabilizer and 0.2 part of cross-linking agent into a mixer, and stirring for 5min at 500rmp to obtain a mixed material;
(3) adding the mixed material into a feeding port of a double-screw extruder, wherein the temperature of the feeding port is 100 ℃, the temperature of two to five zones is 190 ℃, and extruding, drawing strips, cooling and cutting into granules to obtain PLA modified resin granules;
(4) adding PLA modified particles into a single-screw film blowing machine, and cooling the PLA modified particles to a PLA film through film blowing, wherein the temperature of a feed inlet of the single-screw film blowing machine is 135 ℃, and the temperatures of the rest sections are 175-190 ℃;
(5) the subsequent hot stretching conditions were the same as in example 1.
Example 4
(1) Drying 87 parts of PLA and 12 parts of EEA (EA content 18.5%) at 60 ℃ for 6 h;
(2) then adding the mixture, 0.3 part of an opening agent, 0.3 part of a light stabilizer and 0.4 part of a cross-linking agent into a mixer, and stirring for 5min at 500rmp to obtain a mixed material;
(3) adding the mixed material into a feeding port of a double-screw extruder, wherein the temperature of the feeding port is 110 ℃, the temperature of two to five zones is 190 ℃, and extruding, drawing strips, cooling and cutting into granules to obtain PLA modified resin granules;
(4) adding PLA modified particles into a single-screw film blowing machine, and cooling the PLA modified particles to a PLA film through film blowing, wherein the temperature of a feed inlet of the single-screw film blowing machine is 135 ℃, and the temperatures of the rest sections are 175-195 ℃;
(5) the subsequent hot stretching conditions were the same as in example 1.
Example 5
(1) Drying 87 parts of PLA and 12 parts of EEA (EA content is 15%) at 60 ℃ for 6 h;
(2) then adding the mixture, 0.4 part of opening agent, 0.4 part of light stabilizer and 0.2 part of cross-linking agent into a mixer, and stirring for 5min at 500rmp to obtain a mixed material;
(3) adding the mixed material into a feeding port of a double-screw extruder, wherein the temperature of the feeding port is 110 ℃, the temperature of two to five zones is 190 ℃, and extruding, drawing strips, cooling and cutting into granules to obtain PLA modified resin granules;
(4) adding PLA modified particles into a single-screw film blowing machine, and cooling the PLA modified particles to a PLA film through film blowing, wherein the temperature of a feed inlet of the single-screw film blowing machine is 135 ℃, and the temperatures of the rest sections are 175-195 ℃;
(5) the subsequent hot stretching conditions were the same as in example 1.
Example 6
(1) PLA 87 parts and EEA 12(EA content 19.5%) parts are dried for 6h at 60 ℃;
(2) then adding the mixture, 0.4 part of an opening agent, 0.4 part of a light stabilizer and 0.2 part of a cross-linking agent into a mixer, and stirring for 5min at 500rmp to obtain a mixed material;
(3) adding the mixed material into a feeding port of a double-screw extruder, wherein the temperature of the feeding port is 110 ℃, the temperature of two to five zones is 190 ℃, and extruding, drawing strips, cooling and cutting into granules to obtain PLA modified resin granules;
(4) adding PLA modified particles into a single-screw film blowing machine, and cooling the PLA modified particles to a PLA film through film blowing, wherein the temperature of a feed inlet of the single-screw film blowing machine is 135 ℃, and the temperatures of the rest sections are 175-195 ℃;
(5) the subsequent hot stretching conditions were the same as in example 1.
Comparative example 1
(1) Drying 87 parts of PLA and 12 parts of EEA (EA content 18.5%) at 60 ℃ for 6 h;
(2) then adding the mixture, 0.5 part of an opening agent and 0.5 part of a light stabilizer into a mixer, and stirring for 5min at 500rmp to obtain a mixed material;
(3) adding the mixed material into a feeding port of a double-screw extruder, wherein the temperature of the feeding port is 110 ℃, the temperature of two to five zones is 190 ℃, and extruding, drawing strips, cooling and cutting into granules to obtain PLA modified resin granules;
(4) adding PLA modified particles into a single-screw film blowing machine, and cooling the PLA modified particles to a PLA film through film blowing, wherein the temperature of a feed inlet of the single-screw film blowing machine is 135 ℃, and the temperatures of the rest sections are 175-195 ℃;
(5) the subsequent hot stretching conditions were the same as in example 1.
Comparative example 2
(1) Drying 99 parts of PLA for 6 hours at 60 ℃;
(2) then adding the mixture, 0.4 part of opening agent, 0.4 part of light stabilizer and 0.2 part of cross-linking agent into a mixer, and stirring for 5min at 500rmp to obtain a mixed material;
(3) adding the mixed material into a feeding port of a double-screw extruder, wherein the temperature of the feeding port is 110 ℃, the temperature of two to five zones is 190 ℃, and extruding, drawing strips, cooling and cutting into granules to obtain PLA modified resin granules;
(4) adding PLA modified particles into a single-screw film blowing machine, and cooling the PLA modified particles to a PLA film through film blowing, wherein the temperature of a feed inlet of the single-screw film blowing machine is 135 ℃, and the temperatures of the rest sections are 175-195 ℃;
(5) the subsequent hot stretching conditions were the same as in example 1.
Performance testing
Performing shrinkage rate test according to BB/T0070-; the tensile strength test is carried out according to GB/T13022-1991 method for testing the tensile property of the plastic film; testing the light transmittance and the haze according to GB/T2410-2008 'determination of light transmittance and haze of transparent plastics'; testing the impact strength according to an ASTM D256 standard; the test results are shown in table 1.
TABLE 1
Figure BDA0003549846230000071
As can be seen from the above table, the addition of EEA has no great influence on the transparency of polylactic acid, the light transmittance is above 88%, and the haze is below 7.5%; with the increase of the content of EEA, the heat shrinkage rate and the impact strength of PLA are improved, and the possible reason is that chemical crosslinking occurs between EEA and PLA, so that the interface performance is improved; when the amount of the crosslinking agent is increased to 0.4 part, the heat shrinkage and impact strength of PLA are lowered because EEA is excessively crosslinked, particles of EEA are unevenly distributed, and the dispersibility in PLA is poor.
The effect of adding the opening agent is to improve the opening performance of the film; the light stabilizer is added to play a role in protecting PLA in the processing process and long-time illumination, so that yellowing is prevented, and good transparency is kept. In the test process, the opening performance is reduced due to the lack of the opening agent; the light stabilizer is absent, and the light transmittance is reduced; meanwhile, if the addition amount of the opening agent and the light stabilizer is too large, the heat shrinkage property is lowered.
In order to overcome the defect that the PLA is applied as the heat shrinkable film, the PLA, the EEA, the cross-linking agent and the like are melted and blended, so that the PLA and the EEA are subjected to chemical reaction, the interface performance between the PLA and the EEA is improved, the shrinkage performance and the impact resistance of the PLA are improved, the transparency of the PLA is kept, and the application of the biodegradable plastic PLA in the field of the heat shrinkable film is expanded.
It should be noted that the above-mentioned embodiments are only for illustrating the technical solutions of the present invention and not for limiting, and although the present invention has been described in detail with reference to the preferred embodiments, it should be understood by those skilled in the art that modifications or equivalent substitutions may be made on the technical solutions of the present invention without departing from the spirit and scope of the technical solutions of the present invention, which should be covered by the claims of the present invention.

Claims (8)

1. A PLA-based heat shrink film characterized by: the adhesive comprises, by mass, 85-90 parts of PLA, 5-15 parts of EEA, 0.1-0.5 part of an opening agent, 0.1-0.5 part of a light stabilizer and 0.2-0.4 part of a cross-linking agent;
the EA content in the EEA is one or more of 15.0%, 18.5% and 19.5%;
the cross-linking agent is one or the combination of BIPB and TMAIC.
2. A PLA-based heat shrink film as in claim 1, wherein: the opening agent is one or more of oleamide, talcum powder and silicon dioxide.
3. A PLA-based heat shrink film as claimed in claim 1 or 2, wherein: the light stabilizer is one or more of Chimassorb 2020FDL, Chimassor 944 and TINUVIN 326.
4. A preparation method of a PLA-based heat shrinkable film as set forth in any one of claims 1 to 3, wherein: comprises the steps of (a) preparing a mixture of a plurality of raw materials,
drying the PLA and EEA;
mixing PLA, EEA, an opening agent, a cross-linking agent and a light stabilizer in proportion to obtain a mixed material;
extruding, bracing, cooling and dicing the mixed material to prepare PLA modified resin particles;
blowing, cooling and rolling the PLA modified resin particles to prepare a modified PLA film;
the modified PLA film is stretched and immediately cooled, maintaining the shape and size of the stretched film.
5. A method of making a PLA-based heat shrinkable film as set forth in claim 4, wherein: and drying the PLA and the EEA at the drying temperature of 50-60 ℃ for 5-8 h.
6. A process for the preparation of a PLA-based heat shrinkable film as set forth in claim 4 or 5, wherein: and extruding the mixed material, and adding the mixed material into a double-screw extruder, wherein the temperature of a feed inlet of the double-screw extruder is 90-120 ℃, and the temperature of two to five zones is 160-195 ℃.
7. A method of making a PLA-based heat shrink film as claimed in claim 6 wherein: and blowing the PLA modified resin particles by using a single-screw film blowing machine, wherein the temperature of a feed inlet of the single-screw film blowing machine is 135-140 ℃, and the temperature of the rest temperature sections is 165-195 ℃.
8. A process for the preparation of a PLA-based heat shrinkable film as claimed in any one of claims 4, 5, 7, wherein: the modified PLA film was stretched by a uniaxial stretcher having a draw ratio of 4 at 80 ℃.
CN202210260172.7A 2022-03-16 2022-03-16 PLA-based heat shrinkable film and preparation method thereof Active CN114456563B (en)

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JP5330740B2 (en) * 2007-06-06 2013-10-30 三菱樹脂株式会社 Polylactic acid resin composition, polylactic acid film, molded article using the film, stretched film, heat-shrinkable label, and container equipped with the label
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