WO2008091067A1 - Petg based decorative sheet having forming ability similar with pvc - Google Patents

Petg based decorative sheet having forming ability similar with pvc Download PDF

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Publication number
WO2008091067A1
WO2008091067A1 PCT/KR2008/000025 KR2008000025W WO2008091067A1 WO 2008091067 A1 WO2008091067 A1 WO 2008091067A1 KR 2008000025 W KR2008000025 W KR 2008000025W WO 2008091067 A1 WO2008091067 A1 WO 2008091067A1
Authority
WO
WIPO (PCT)
Prior art keywords
resin
petg
decorative sheet
pvc
sheet according
Prior art date
Application number
PCT/KR2008/000025
Other languages
French (fr)
Inventor
Young-Sun An
Min-Ho Lee
Original Assignee
Lg Chem, Ltd.
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Lg Chem, Ltd. filed Critical Lg Chem, Ltd.
Priority to JP2009546314A priority Critical patent/JP2010516833A/en
Priority to EP08704566A priority patent/EP2121815A4/en
Priority to CN2008800027346A priority patent/CN101583654B/en
Publication of WO2008091067A1 publication Critical patent/WO2008091067A1/en

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Classifications

    • 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
    • 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
    • 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
    • C08L67/03—Polyesters derived from dicarboxylic acids and dihydroxy compounds the dicarboxylic acids and dihydroxy compounds having the carboxyl- and the hydroxy groups directly linked to aromatic rings
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L71/00—Compositions of polyethers obtained by reactions forming an ether link in the main chain; Compositions of derivatives of such polymers
    • C08L71/02—Polyalkylene oxides
    • 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
    • C08J2367/02—Polyesters derived from dicarboxylic acids and dihydroxy compounds
    • 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
    • C08J2367/02—Polyesters derived from dicarboxylic acids and dihydroxy compounds
    • C08J2367/03—Polyesters derived from dicarboxylic acids and dihydroxy compounds the dicarboxylic acids and dihydroxy compounds having the hydroxy and the carboxyl groups directly linked to aromatic rings
    • 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
    • C08J2371/00—Characterised by the use of polyethers obtained by reactions forming an ether link in the main chain; Derivatives of such polymers
    • C08J2371/02—Polyalkylene oxides
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J2467/00—Characterised by the use of polyesters obtained by reactions forming a carboxylic ester link in the main chain; Derivatives of such polymers
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J2467/00—Characterised by the use of polyesters obtained by reactions forming a carboxylic ester link in the main chain; Derivatives of such polymers
    • C08J2467/02—Polyesters derived from dicarboxylic acids and dihydroxy compounds
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2203/00—Applications
    • C08L2203/16—Applications used for films
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2205/00—Polymer mixtures characterised by other features
    • C08L2205/02—Polymer mixtures characterised by other features containing two or more polymers of the same C08L -group

Definitions

  • the present invention relates to a decorative sheet. More specifically, the present invention relates to a polyethylene terephthalate glycol (PETG)-based decorative sheet with formability comparable to polyvinylchloride (PVC).
  • PETG polyethylene terephthalate glycol
  • PVC polyvinylchloride
  • PETG decorative sheets for forming-purposes exhibit superior surface quality, but have a narrow range of high forming temperatures, as compared to polyvinylchloride (PVC). That is to say, in spite of superior surface quality and formability, PETG decorative sheets have a narrow range of forming temperature, thus making it difficult to perform secondary subsequent processing (i.e. forming). At low forming temperatures, the edge of articles may be cracked, or the adhesion force of the articles may be deteriorated. At high forming temperatures, there are problems in that the edges of articles may droop or sag, and surface quality is deteriorated in proportion to forming quality.
  • Japanese Patent Laid-open Publication No. 2003-246916 discloses a composition for a flexible cosmetic polyester sheet having a specific melt volume- flow rate, comprising a specific mix ratio of three polyester resins that differ from one another in glass transition temperature.
  • No. 2005-298715 discloses a composition with flame-retardancy employing the flexible polyester sheet and inorganic filler. Such prior art is different from the present invention that aims to lower forming temperatures at which a PETG resin is available and widen the range thereof.
  • a decorative sheet comprising a polyethylene terephthalate glycol (PETG) alloy resin prepared by alloying a PETG resin with an ester resin or an elastomer resin.
  • the PETG alloy resin of the present invention has a glass transition temperature (Tg) of 75 ⁇ 3 0 C which is lower than that of a general PETG resin by 3 to 7°C; and therefore, it is applicable to forming processes at low temperatures similar to those of PVC.
  • the PETG alloy resin of the present invention is applicable to forming processes at 60 to 80 0 C. This range is wide, similar to that of PVC.
  • PETG resins are generally applicable to forming processes at 7O 0 C to 85 0 C.
  • the ester resin used as the alloy ingredient in the present invention is polybutylene terephthalate (PBT) and may be prepared by liquid- or solid polymerization.
  • the elastomer resin used in the present invention may be a copolymer of a PBT resin and polyether glycol.
  • the content of the ester resin or the elastomer resin may be 5 to 20 parts by weight, based on 100 parts by weight of the PETG.
  • Tg and forming temperature of the alloy resin cannot be lowered to a desired level.
  • Tg and forming temperature of the alloy resin are excessively low, compound-property and sheet-extrudability are deteriorated and sheet-processibility is thus degraded due to characteristics of PBT and elastomer resins during processing. At this time, due to resistant-chemical properties of the PBT resin, surface-processibility and adhesion force of sheets are deteriorated.
  • the PETG resin by alloying the PETG resin with an ester resin or elastomer resin and thus lowering Tg by 3 to 7°C and gradually sloping down the decreasing rate of elastic modulus, it is possible to prepare a compound having thermal behaviors similar to PVC.
  • decorative sheets applicable to forming processes in a wide range of low temperatures may be prepared from this compound.
  • one of representative methods for evaluating the formability is to measure variation in elastic modulus employing dynamic mechanical analysis (DMA).
  • DMA dynamic mechanical analysis
  • FIG. 1 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Example 1 ;
  • FIG. 2 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Example 2;
  • FIG. 3 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Example 3;
  • FIG. 4 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Example 4; and FIG. 5 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Comparative Example.
  • a PETG resin was subjected to extrusion-sheeting in a thickness of 0.5 mm.
  • the glass transition temperature of a conventional PETG mirrored decorative sheet begins to decrease at around 74°C and is then minimized at around 84 0 C.
  • FIG. 1 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Example 1 (PETG + PBT alloy resin, content of alloy ingredient: 10 phr). As apparent from FIG. 1, Tg is 76°C and storage modulus begins to decrease at 65 0 C.
  • FIG. 2 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Example 2 (PETG + PBT alloy resin, content of alloy ingredient: 20 phr). As apparent from FIG. 2, Tg is 74°C and storage modulus begins to decrease at 63 0 C.
  • FIG. 3 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Example 3 (PETG + PBT copolymer elastomer alloy resin, content of alloy ingredient: 10 phr). As apparent from FIG. 3, Tg is 77°C and storage modulus begins to decrease at 65 0 C.
  • FIG. 4 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Example 4 (PETG + PBT copolymer elastomer alloy resin, content of alloy ingredient: 20 phr). As apparent from FIG. 4, Tg is 73 °C and storage modulus begins to decrease at 6O 0 C.
  • FIG. 5 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Comparative Example (PETG resin). As apparent from FIG. 5, Tg is 83 0 C and storage modulus begins to decrease at 73°C.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Manufacturing & Machinery (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Laminated Bodies (AREA)
  • Manufacture Of Macromolecular Shaped Articles (AREA)
  • Polyesters Or Polycarbonates (AREA)

Abstract

Disclosed herein is a polyethylene terephthalate glycol (PETG)-based decorative sheet with formability similar to polyvinylchloride (PVC). The decorative sheet comprises a polyethylene terephthalate glycol (PETG) alloy resin prepared by alloying a PETG resin with an ester resin or an elastomer resin.

Description

PETG BASED DECORATIVE SHEET HAVING FORMING ABILITY SIMILAR WITH PVC
Technical Field
The present invention relates to a decorative sheet. More specifically, the present invention relates to a polyethylene terephthalate glycol (PETG)-based decorative sheet with formability comparable to polyvinylchloride (PVC).
Background Art
Polyethylene terephthalate glycol (PETG)-based decorative sheets for forming-purposes exhibit superior surface quality, but have a narrow range of high forming temperatures, as compared to polyvinylchloride (PVC). That is to say, in spite of superior surface quality and formability, PETG decorative sheets have a narrow range of forming temperature, thus making it difficult to perform secondary subsequent processing (i.e. forming). At low forming temperatures, the edge of articles may be cracked, or the adhesion force of the articles may be deteriorated. At high forming temperatures, there are problems in that the edges of articles may droop or sag, and surface quality is deteriorated in proportion to forming quality.
Japanese Patent Laid-open Publication No. 2003-246916 discloses a composition for a flexible cosmetic polyester sheet having a specific melt volume- flow rate, comprising a specific mix ratio of three polyester resins that differ from one another in glass transition temperature. Japanese Patent Laid-open Publication
No. 2005-298715 discloses a composition with flame-retardancy employing the flexible polyester sheet and inorganic filler. Such prior art is different from the present invention that aims to lower forming temperatures at which a PETG resin is available and widen the range thereof.
Disclosure Technical Problem
It is an aspect of the present invention to provide a PETG decorative sheet for forming-purposes having formability in a narrow range of low forming temperatures comparable to those of PVC.
Technical Solution
In accordance with an aspect of the present invention for achieving the above problem, there is provided a decorative sheet comprising a polyethylene terephthalate glycol (PETG) alloy resin prepared by alloying a PETG resin with an ester resin or an elastomer resin. The PETG alloy resin of the present invention has a glass transition temperature (Tg) of 75 ± 30C which is lower than that of a general PETG resin by 3 to 7°C; and therefore, it is applicable to forming processes at low temperatures similar to those of PVC.
In addition, the PETG alloy resin of the present invention is applicable to forming processes at 60 to 800C. This range is wide, similar to that of PVC.
PETG resins are generally applicable to forming processes at 7O0C to 850C.
Preferably, the ester resin used as the alloy ingredient in the present invention is polybutylene terephthalate (PBT) and may be prepared by liquid- or solid polymerization. The elastomer resin used in the present invention may be a copolymer of a PBT resin and polyether glycol.
Preferably, the content of the ester resin or the elastomer resin may be 5 to 20 parts by weight, based on 100 parts by weight of the PETG.
When the content of the alloy ingredient is lower than 5 phr, Tg and forming temperature of the alloy resin cannot be lowered to a desired level. When the content of the alloy ingredient exceeds 20 phr, Tg and forming temperature of the alloy resin are excessively low, compound-property and sheet-extrudability are deteriorated and sheet-processibility is thus degraded due to characteristics of PBT and elastomer resins during processing. At this time, due to resistant-chemical properties of the PBT resin, surface-processibility and adhesion force of sheets are deteriorated.
According to the present invention, by alloying the PETG resin with an ester resin or elastomer resin and thus lowering Tg by 3 to 7°C and gradually sloping down the decreasing rate of elastic modulus, it is possible to prepare a compound having thermal behaviors similar to PVC. Thus, decorative sheets applicable to forming processes in a wide range of low temperatures may be prepared from this compound.
For the reference, one of representative methods for evaluating the formability is to measure variation in elastic modulus employing dynamic mechanical analysis (DMA).
Description of Drawings
The above and other aspects, features and other advantages of the present invention will be more clearly understood from the following detailed description taken in conjunction with the accompanying drawings, in which:
FIG. 1 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Example 1 ;
FIG. 2 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Example 2;
FIG. 3 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Example 3;
FIG. 4 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Example 4; and FIG. 5 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Comparative Example.
Best Mode
[Example 1]
10 phr of a PBT resin was added to a PETG resin and the blend was extrusion-compounded and then subjected to extrusion-sheeting in a thickness of 0.5 mm.
[Example 2]
20 phr of a PBT resin was added to a PETG resin and the blend was extrusion-compounded and then subjected to extrusion-sheeting in a thickness of 0.5 mm. [Example 3]
10 phr of a PBT copolymer elastomer resin was added to a PETG resin and the blend was extrusion-compounded and then subjected to extrusion-sheeting in a thickness of 0.5 mm.
[Example 4]
20 phr of a PBT copolymer elastomer resin was added to a PETG resin and the blend was extrusion-compounded and then subjected to extrusion-sheeting in a thickness of 0.5 mm.
[Comparative Example]
A PETG resin was subjected to extrusion-sheeting in a thickness of 0.5 mm.
As can be seen from FIG. 5, the glass transition temperature of a conventional PETG mirrored decorative sheet begins to decrease at around 74°C and is then minimized at around 840C.
[Experimental Example]
For the decorative sheets of Examples 1 to 4 and Comparative Example, variations in glass transition temperature and storage modulus were measured by
DMA.
FIG. 1 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Example 1 (PETG + PBT alloy resin, content of alloy ingredient: 10 phr). As apparent from FIG. 1, Tg is 76°C and storage modulus begins to decrease at 650C.
FIG. 2 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Example 2 (PETG + PBT alloy resin, content of alloy ingredient: 20 phr). As apparent from FIG. 2, Tg is 74°C and storage modulus begins to decrease at 630C. FIG. 3 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Example 3 (PETG + PBT copolymer elastomer alloy resin, content of alloy ingredient: 10 phr). As apparent from FIG. 3, Tg is 77°C and storage modulus begins to decrease at 650C.
FIG. 4 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Example 4 (PETG + PBT copolymer elastomer alloy resin, content of alloy ingredient: 20 phr). As apparent from FIG. 4, Tg is 73 °C and storage modulus begins to decrease at 6O0C.
FIG. 5 is a graph showing variations in glass transition temperature and storage modulus of a decorative sheet according to Comparative Example (PETG resin). As apparent from FIG. 5, Tg is 830C and storage modulus begins to decrease at 73°C.
Industrial Applicability
As apparent from the above description, according to the present invention, by alloying a PETG resin with an ester resin or an elastomer resin, it is possible to prepare a PETG decorative sheet that maintains surface quality and exhibits formability in a wide range of temperature which is 3 to 1O0C lower than conventional PETG decorative sheets.

Claims

1. A decorative sheet comprising a polyethylene terephthalate glycol (PETG) alloy resin prepared by alloying a PETG resin with an ester resin or an elastomer resin.
2. The decorative sheet according to claim 1, wherein the PETG alloy resin has a glass transition temperature (Tg) of 75 ± 30C.
3. The decorative sheet according to claim 1, wherein the PETG alloy resin is applicable to a forming process at 60 to 800C.
4. The decorative sheet according to claim 1, wherein the ester resin is polybutylene terephthalate (PBT).
5. The decorative sheet according to claim 1, wherein the elastomer resin is a copolymer of polyether glycol and a polybutylene terephthalate (PBT) resin.
6. The decorative sheet according to claim 1, wherein the content of the ester resin or the elastomer resin is 5 to 20 parts by weight, based on 100 parts by weight of the PETG resin.
PCT/KR2008/000025 2007-01-23 2008-01-03 Petg based decorative sheet having forming ability similar with pvc WO2008091067A1 (en)

Priority Applications (3)

Application Number Priority Date Filing Date Title
JP2009546314A JP2010516833A (en) 2007-01-23 2008-01-03 PETG-type decorative panel for molding having moldability similar to PVC
EP08704566A EP2121815A4 (en) 2007-01-23 2008-01-03 Petg based decorative sheet having forming ability similar with pvc
CN2008800027346A CN101583654B (en) 2007-01-23 2008-01-03 Petg based decorative sheet having forming ability similar with pvc

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
KR1020070006824A KR101004614B1 (en) 2007-01-23 2007-01-23 PETG based decorative sheet having forming ability similar with PVC
KR10-2007-0006824 2007-01-23

Publications (1)

Publication Number Publication Date
WO2008091067A1 true WO2008091067A1 (en) 2008-07-31

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ID=39644625

Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/KR2008/000025 WO2008091067A1 (en) 2007-01-23 2008-01-03 Petg based decorative sheet having forming ability similar with pvc

Country Status (5)

Country Link
EP (1) EP2121815A4 (en)
JP (1) JP2010516833A (en)
KR (1) KR101004614B1 (en)
CN (1) CN101583654B (en)
WO (1) WO2008091067A1 (en)

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EP3476896B8 (en) 2017-10-24 2023-11-22 Youngil Co. Ltd Polybutylene terephthalate elastomer composition having excellent heat resistance
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KR102162574B1 (en) 2018-06-28 2020-10-07 이호영 A film composition for packaging which is recyclable and excellent in adhesion
KR102110131B1 (en) * 2018-07-17 2020-05-13 주식회사 케이에스씨 Synthetic resin composition for deco sheets
KR102167904B1 (en) 2018-12-13 2020-10-20 주식회사 케이씨씨 Composition for decoration sheet and decoration sheet prepared therefrom
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CN101583654B (en) 2012-07-04
JP2010516833A (en) 2010-05-20
KR101004614B1 (en) 2010-12-28
EP2121815A1 (en) 2009-11-25
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