USH1518H - Impact modification of polypropylene with styrene/isoprene triblock copolymers - Google Patents

Impact modification of polypropylene with styrene/isoprene triblock copolymers Download PDF

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Publication number
USH1518H
USH1518H US08/304,974 US30497494A USH1518H US H1518 H USH1518 H US H1518H US 30497494 A US30497494 A US 30497494A US H1518 H USH1518 H US H1518H
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Prior art keywords
polypropylene
polystyrene
weight
composition
polymer components
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Abandoned
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US08/304,974
Inventor
Lie K. Djiauw
Michael J. Modic
Richard Gelles
Glenn R. Himes
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Kraton Polymers US LLC
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Shell Oil Co
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Priority to US08/304,974 priority Critical patent/USH1518H/en
Assigned to SHELL OIL COMPANY reassignment SHELL OIL COMPANY ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: DJIAUW, LIE KHONG, GELLES, RICHARD, HIMES, GLENN ROY, MODIC, MICHAEL JOHN
Application granted granted Critical
Publication of USH1518H publication Critical patent/USH1518H/en
Assigned to UBS AG, STAMFORD BRANCH reassignment UBS AG, STAMFORD BRANCH SECURITY INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: KRATON POLYMERS U.S. LLC
Assigned to KRATON POLYMERS U.S. LLC reassignment KRATON POLYMERS U.S. LLC AFFIDAVIT OF NAME CHANGE Assignors: SHELL ELASTOMERS LLC
Assigned to SHELL ELASTOMERS LLC reassignment SHELL ELASTOMERS LLC CHANGE OF NAME (SEE DOCUMENT FOR DETAILS). Assignors: SHELL OIL COMPANY
Assigned to KRATON POLYMERS U.S. LLC reassignment KRATON POLYMERS U.S. LLC RELEASE BY SECURED PARTY (SEE DOCUMENT FOR DETAILS). Assignors: UBS AG, STAMFORD BRANCH
Assigned to KRATON POLYMERS U.S. LLC reassignment KRATON POLYMERS U.S. LLC CORRECTIVE ASSIGNMENT TO CORRECT THE INCORRECT PATENT NUMBER 7720798 AND REPLACE WITH PATENT NUMBER 7220798 PREVIOUSLY RECORDED ON REEL 025845 FRAME 0795. ASSIGNOR(S) HEREBY CONFIRMS THE RELEASE BY SECURED PARTY. Assignors: USB AG, STAMFORD BRANCH
Abandoned legal-status Critical Current

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    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
    • C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
    • C08L23/10—Homopolymers or copolymers of propene
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L53/00—Compositions of block copolymers containing at least one sequence of a polymer obtained by reactions only involving carbon-to-carbon unsaturated bonds; Compositions of derivatives of such polymers
    • C08L53/02—Compositions of block copolymers containing at least one sequence of a polymer obtained by reactions only involving carbon-to-carbon unsaturated bonds; Compositions of derivatives of such polymers of vinyl-aromatic monomers and conjugated dienes

Definitions

  • the invention relates to compositions that contain polyolefin resins and elastomeric block copolymers. More specifically, the invention relates to polypropylene molding compositions that have improved impact resistance.
  • Polypropylene molding compositions containing low or medium flow polypropylene have good impact resistance when the composition includes a high molecular weight styrenic block copolymer having the structure polystyrene-hydrogenated polybutadiene-polystyrene, e.g. KRATON® G1650 thermoplastic elastomer.
  • the impact strengths are suitable for use of the molding compositions in large automotive parts.
  • polypropylene molding compositions for large automotive parts must also have improvements in rigidity, heat deformation resistance, low temperature impact resistance, and surface appearance.
  • High flow polypropylene molding compositions that are suitable for large automotive parts except for inferior low temperature impact strength and inferior high temperature heat deformation are produced by blending low molecular weight polystyrene with low molecular weight diblock copolymers of polystyrene-hydrogenated butadiene.
  • a blend of the triblock and diblock copolymers is commercially available as KRATON® G1657 elastomer which is available from Shell.
  • U.S. Pat. No. 5,045,589 describes much improved polypropylene molding compositions comprising a crystalline ethylene/propylene block copolymer, an amorphous polypropylene copolymer, and a thermoplastic elastomer which can be a polystyrene-hydrogenated polybutadiene-polystyrene elastomer, e.g. KRATON® G1650 elastomer, or a polystyrene-hydrogenated polyisoprene-polystyrene elastomer.
  • the present invention provides a high flow polypropylene molding composition that is excellent for large automobile parts, the polypropylene composition containing a low molecular weight polystyrene-hydrogenated polyisoprene-polystyrene elastomer which is superior to butadiene based elastomers for improving low temperature impact strength and high temperature heat distortion.
  • the isoprene based triblock polymers are also excellent modifiers for blends containing ethylene/propylene block polymers.
  • Polypropylene molding compositions comprising 60-95%, preferably 80-95%, by weight of the polymer components of a high flow polypropylene homopolymer or copolymer and 40-5%, preferably 20-5%, by weight of the polymer components of a low molecular weight polystyrene-hydrogenated polyisoprene-polystyrene block copolymer have excellent physical and appearance properties including superior low temperature impact strength and superior high temperature heat deformation.
  • the peak molecular weight of the block copolymers ranges from 58,000 to 82,000 with a polystyrene content from 13% to 20%.
  • the high flow propylene polymer can be (i) a homopolymer of propylene, (ii) a random copolymer of propylene and an olefin selected from ethylene and C 4 -C 10 alpha-olefins, or (iii) a random terpolymer of propylene with two alpha-olefins selected from the group consisting of ethylene and C 4 -C 10 alpha olefin, provided that the propylene polymer has a melt flow higher than 30 dg/min as measured by ASTM Method D 1238-82 (230° C./5 kg).
  • the polypropylene has a melt flow from 50 to 80 dg/min.
  • the C 4 -C 10 alpha-olefins include linear and branched C 4 -C 10 alpha-olefins such as 1-butene, 1-pentene, 4-methyl-pentene-1, 3-methyl-1-butene, 1-hexene, 3-4-dimethyl-1-butene, 1-heptene, 3-methyl-1-hexene, 1-octene and the like.
  • the elastomeric block copolymers employed in the molding compositions of the present invention have two polystyrene endblocks and one hydrogenated isoprene midblock in a linear arrangement (S-EP-S).
  • the polystyrene endblocks each preferably have a peak molecular weight from 4,500 to 8,000, most preferably from 5,000 to 5,500, which results in formation of weak polystyrene domains and low melt viscosity.
  • polypropylene molding compositions could further contain polyethylene-polypropylene block copolymers as described in U.S. Pat. No. 5,045,589 which is incorporated by reference herein.
  • Fillers and reinforcing agents e.g. carbon black and glass fibers, as well as inorganic powders such as calcium carbonate, talc, mica, and glass, may be included in the composition of the invention at concentration levels up to about 80 parts by weight per 100 parts by weight of the total polymer components. In addition to the economic benefit such fillers afford, greater stiffness and a higher heat distortion temperature can be attained.
  • the components of the composition can be blended or admixed in any conventional mixing apparatus, such as an extruder or a Banbury mixer.
  • test methods used to evaluate the molded specimens were ASTM D-256 (notched Izod impact at room temperature), ASTM D-638 (tensile strength), ASTM D-790 (flexural modulus), and ASTM-648 (Heat Distortion Temperature at 1820 kPa).
  • the propylene polymer used in the preparation of the molding compositions was a pelletized polypropylene resin, commercially available from UBE (UBE ZT772), a nominal melt flow rate (ASTM Method D 1238-82, 230° C./5 kg) of 66 dg/min.
  • the block copolymers are further described in Table I and the polypropylene molding compositions and results of the evaluations performed on the Example 1-2 compositions and the two control compositions are shown in Table II.

Abstract

Compositions consisting essentially of from 60% to 95% by weight of the polymer components of a high flow polypropylene and from 40% to 5% by weight of a polystyrene-hydrogenated polyisoprene-polystyrene block copolymer have excellent low temperature impact strength and high heat distortion temperature for molding large automobile parts.

Description

This is a continuation of application Ser. No. 08/150,654, filed Nov. 3, 1993, now abandoned.
FIELD OF THE INVENTION
The invention relates to compositions that contain polyolefin resins and elastomeric block copolymers. More specifically, the invention relates to polypropylene molding compositions that have improved impact resistance.
BACKGROUND OF THE INVENTION
Polypropylene molding compositions containing low or medium flow polypropylene have good impact resistance when the composition includes a high molecular weight styrenic block copolymer having the structure polystyrene-hydrogenated polybutadiene-polystyrene, e.g. KRATON® G1650 thermoplastic elastomer. The impact strengths are suitable for use of the molding compositions in large automotive parts. However, research has established that polypropylene molding compositions for large automotive parts must also have improvements in rigidity, heat deformation resistance, low temperature impact resistance, and surface appearance.
High flow polypropylene molding compositions that are suitable for large automotive parts except for inferior low temperature impact strength and inferior high temperature heat deformation are produced by blending low molecular weight polystyrene with low molecular weight diblock copolymers of polystyrene-hydrogenated butadiene. A blend of the triblock and diblock copolymers is commercially available as KRATON® G1657 elastomer which is available from Shell.
U.S. Pat. No. 5,045,589 describes much improved polypropylene molding compositions comprising a crystalline ethylene/propylene block copolymer, an amorphous polypropylene copolymer, and a thermoplastic elastomer which can be a polystyrene-hydrogenated polybutadiene-polystyrene elastomer, e.g. KRATON® G1650 elastomer, or a polystyrene-hydrogenated polyisoprene-polystyrene elastomer.
SUMMARY OF THE INVENTION
The present invention provides a high flow polypropylene molding composition that is excellent for large automobile parts, the polypropylene composition containing a low molecular weight polystyrene-hydrogenated polyisoprene-polystyrene elastomer which is superior to butadiene based elastomers for improving low temperature impact strength and high temperature heat distortion. The isoprene based triblock polymers are also excellent modifiers for blends containing ethylene/propylene block polymers.
DETAILED DESCRIPTION OF THE INVENTION
Polypropylene molding compositions comprising 60-95%, preferably 80-95%, by weight of the polymer components of a high flow polypropylene homopolymer or copolymer and 40-5%, preferably 20-5%, by weight of the polymer components of a low molecular weight polystyrene-hydrogenated polyisoprene-polystyrene block copolymer have excellent physical and appearance properties including superior low temperature impact strength and superior high temperature heat deformation. The peak molecular weight of the block copolymers ranges from 58,000 to 82,000 with a polystyrene content from 13% to 20%.
The high flow propylene polymer can be (i) a homopolymer of propylene, (ii) a random copolymer of propylene and an olefin selected from ethylene and C4 -C10 alpha-olefins, or (iii) a random terpolymer of propylene with two alpha-olefins selected from the group consisting of ethylene and C4 -C10 alpha olefin, provided that the propylene polymer has a melt flow higher than 30 dg/min as measured by ASTM Method D 1238-82 (230° C./5 kg). Preferably, the polypropylene has a melt flow from 50 to 80 dg/min. The C4 -C10 alpha-olefins include linear and branched C4 -C10 alpha-olefins such as 1-butene, 1-pentene, 4-methyl-pentene-1, 3-methyl-1-butene, 1-hexene, 3-4-dimethyl-1-butene, 1-heptene, 3-methyl-1-hexene, 1-octene and the like.
The elastomeric block copolymers employed in the molding compositions of the present invention have two polystyrene endblocks and one hydrogenated isoprene midblock in a linear arrangement (S-EP-S). The polystyrene endblocks each preferably have a peak molecular weight from 4,500 to 8,000, most preferably from 5,000 to 5,500, which results in formation of weak polystyrene domains and low melt viscosity.
The hydrogenated isoprene blocks have a residual unsaturation less that 5%, preferably less than 2%, and may have from 30% to 100% 1,4-addition of the isoprene. The block copolymers are readily prepared by anionic polymerization and selective hydrogenation processes known in the art to give polymers having low polydispersity.
The polypropylene molding compositions could further contain polyethylene-polypropylene block copolymers as described in U.S. Pat. No. 5,045,589 which is incorporated by reference herein.
Fillers and reinforcing agents, e.g. carbon black and glass fibers, as well as inorganic powders such as calcium carbonate, talc, mica, and glass, may be included in the composition of the invention at concentration levels up to about 80 parts by weight per 100 parts by weight of the total polymer components. In addition to the economic benefit such fillers afford, greater stiffness and a higher heat distortion temperature can be attained.
The components of the composition can be blended or admixed in any conventional mixing apparatus, such as an extruder or a Banbury mixer.
EXAMPLES
The following examples, presented for illustrative purposes, describe various embodiments of the polypropylene molding composition of the invention.
In all of the examples and control experiments, the polypropylene and the S-EP-S block copolymer, as well as any other modifier used in comparison, were mixed and extruded in a single pass through a co-rotating twin-screw extruder. A stabilizer composition (0.08 weight%), known as Irganox 1010, was added to all batches before compounding to minimize oxidation. The extruder temperature was in the 200°-245° C. range. The extruded blends were molded into test specimens.
The test methods used to evaluate the molded specimens were ASTM D-256 (notched Izod impact at room temperature), ASTM D-638 (tensile strength), ASTM D-790 (flexural modulus), and ASTM-648 (Heat Distortion Temperature at 1820 kPa).
EXAMPLES 1-2
Two polypropylene molding compositions of the invention were made and tested as described above. In these compositions the block copolymer was a S-EP-S block copolymer. Two control compositions containing known styrene/butadiene block copolymers also were made and tested in the same manner.
The propylene polymer used in the preparation of the molding compositions was a pelletized polypropylene resin, commercially available from UBE (UBE ZT772), a nominal melt flow rate (ASTM Method D 1238-82, 230° C./5 kg) of 66 dg/min.
The block copolymers are further described in Table I and the polypropylene molding compositions and results of the evaluations performed on the Example 1-2 compositions and the two control compositions are shown in Table II.
                                  TABLE I                                 
__________________________________________________________________________
             Comparison Example No.                                       
                           Example No.                                    
             A.sup.(a)                                                    
                    B.sup.(b)                                             
                           1      2                                       
__________________________________________________________________________
Triblock/Diblock in                                                       
             100% S-EB-S                                                  
                    70% S-EB-S                                            
                           100% S-EP-S                                    
                                  100% S-EP-S                             
Block Copolymer (wt %)                                                    
                    30% S-EB                                              
Molecular Weight (peak)                                                   
             71,000 82,000 62,000 59,000                                  
Triblock/Diblock    41,000                                                
Polystyrene (wt %).sup.(c)                                                
             30     13     18     19                                      
Melt Flow dg/min.sup.(d)                                                  
             No Flow                                                      
                    20-29  14     29                                      
Tensile strength psi                                                      
             3,100  2,550  3,100  3,125                                   
__________________________________________________________________________
 .sup.(a) Commercially availableKRATON ® G1650 elastomer from Shell.  
 .sup.(b) Commercially availableKRATON ® G1657 elastomer from Shell.  
 .sup.(c) Measured prior to hydrogenation.                                
 .sup.(d) ASTM D1238 (230° C./5 kg).                               

              TABLE II                                                    
______________________________________                                    
               Comparison                                                 
               Example No.                                                
                         Example No.                                      
Polypropylene Comp..sup.(a)                                               
                 A       B       1     2                                  
______________________________________                                    
Heat Distortion Temperature                                               
                 109.0   104.1   105.6 --                                 
(°C.)                                                              
Brittleness Temp. (°C.)                                            
                 -37.6   -40.8   -45.0 --                                 
Izod Impact (Kg-cm/cm.sup.2)                                              
                 15.8    21      38    57                                 
Melt Flow dg/min.sup.(b)                                                  
                 40      59      57    60                                 
Flex Modulus (Kg/cm.sup.2)                                                
                 12,450  12,070  12,040                                   
                                       11,410                             
______________________________________                                    
 .sup.(a) Contains 90% high flow polypropylene and 10% block copolymer wit
 0.08% Irganox 1010.                                                      
 .sup.(b) ASTM 1238 230° C./5 kg.

Claims (4)

What is claimed is:
1. A polypropylene molding composition, comprising:
from 60% to 95% by weight of the polymer components of a high flow polypropylene having a melt flow from 50 to 80 dg/min, wherein the polypropylene is selected from a group consisting of homopolymers of propylene, random copolymers of propylene and an olefin selected from ethylene and C4 -C10 alpha-olefins, and random terpolymers of propylene with two alpha-olefins selected from ethylene and C4 -C10 alpha-olefins; and
from 40% to 5% by weight of the polymer components of a polystyrene-hydrogenated polyisoprene-polystyrene block copolymer having a peak molecular weight from 4,500 to 8,000 for each polystyrene block and a polystyrene content from 13% to 20%.
2. The composition of claim 1, wherein each polystyrene block in the block copolymer has a peak molecular weight from 5,000 to 5,500.
3. The composition of claim 1, wherein the high flow polypropylene comprises from 80% to 95% of the polymer components.
4. The composition of claim 1, further comprising up to about 80 parts of a filler per 100 parts of the total polymer components.
US08/304,974 1993-11-03 1994-09-13 Impact modification of polypropylene with styrene/isoprene triblock copolymers Abandoned USH1518H (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
US08/304,974 USH1518H (en) 1993-11-03 1994-09-13 Impact modification of polypropylene with styrene/isoprene triblock copolymers

Applications Claiming Priority (2)

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US15065493A 1993-11-03 1993-11-03
US08/304,974 USH1518H (en) 1993-11-03 1994-09-13 Impact modification of polypropylene with styrene/isoprene triblock copolymers

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20150315377A1 (en) * 2014-04-30 2015-11-05 Exxonmobil Chemical Patents Inc. Polypropylene Compositions and Methods to Produce the Same

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP5240985B2 (en) * 2007-11-06 2013-07-17 旭化成ケミカルズ株式会社 Block copolymer composition and method for producing hydrogenated product thereof

Citations (11)

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JPS5829842A (en) * 1981-08-18 1983-02-22 Mitsubishi Petrochem Co Ltd Propylene polymer composition having improved coatability
EP0308001A2 (en) * 1987-09-04 1989-03-22 Shell Internationale Researchmaatschappij B.V. Polymeric composition
US5026752A (en) * 1987-04-03 1991-06-25 Minnesota Mining And Manufacturing Company Amorphous-polypropylene-based hot melt adhesive
US5045589A (en) * 1988-11-21 1991-09-03 Ube Industries, Ltd. Polypropylene composition
US5060818A (en) * 1988-08-08 1991-10-29 Japan Crown Cork Co., Ltd. Heat-resistant liner-provided vessel closure and process for preparation thereof
US5086109A (en) * 1989-12-01 1992-02-04 Ube Industries, Ltd. Polypropylene resin composition
JPH0570699A (en) * 1991-09-13 1993-03-23 Kuraray Co Ltd Thermoplastic resin composition
JPH05163394A (en) * 1991-12-12 1993-06-29 Mitsui Toatsu Chem Inc Polypropylene resin composition excellent in clarity and flexibility
US5256734A (en) * 1991-02-15 1993-10-26 Mitsui Toatsu Chemicals, Inc. Polypropylene resin composition and method for manufacturing coated molded article of the resin composition
US5374677A (en) * 1991-06-21 1994-12-20 Mitsubishi Petrochemical Company Limited Thermoplastic polymer composition
JPH09149939A (en) * 1995-12-01 1997-06-10 Tokai Rika Co Ltd Sensor for intra-corporeal medical instrument

Patent Citations (11)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS5829842A (en) * 1981-08-18 1983-02-22 Mitsubishi Petrochem Co Ltd Propylene polymer composition having improved coatability
US5026752A (en) * 1987-04-03 1991-06-25 Minnesota Mining And Manufacturing Company Amorphous-polypropylene-based hot melt adhesive
EP0308001A2 (en) * 1987-09-04 1989-03-22 Shell Internationale Researchmaatschappij B.V. Polymeric composition
US5060818A (en) * 1988-08-08 1991-10-29 Japan Crown Cork Co., Ltd. Heat-resistant liner-provided vessel closure and process for preparation thereof
US5045589A (en) * 1988-11-21 1991-09-03 Ube Industries, Ltd. Polypropylene composition
US5086109A (en) * 1989-12-01 1992-02-04 Ube Industries, Ltd. Polypropylene resin composition
US5256734A (en) * 1991-02-15 1993-10-26 Mitsui Toatsu Chemicals, Inc. Polypropylene resin composition and method for manufacturing coated molded article of the resin composition
US5374677A (en) * 1991-06-21 1994-12-20 Mitsubishi Petrochemical Company Limited Thermoplastic polymer composition
JPH0570699A (en) * 1991-09-13 1993-03-23 Kuraray Co Ltd Thermoplastic resin composition
JPH05163394A (en) * 1991-12-12 1993-06-29 Mitsui Toatsu Chem Inc Polypropylene resin composition excellent in clarity and flexibility
JPH09149939A (en) * 1995-12-01 1997-06-10 Tokai Rika Co Ltd Sensor for intra-corporeal medical instrument

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20150315377A1 (en) * 2014-04-30 2015-11-05 Exxonmobil Chemical Patents Inc. Polypropylene Compositions and Methods to Produce the Same
US10287431B2 (en) * 2014-04-30 2019-05-14 Exxonmobil Chemical Patents Inc. Polypropylene compositions and methods to produce the same

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JP3468879B2 (en) 2003-11-17
JPH07188480A (en) 1995-07-25

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