Propylene polymer compositions

Abstract

A propylene polymer composition is prepared by mixing propylene home- or co-polymer (A) obtained using a transition metal catalyst compound (h), defined herein, with a co-catalyst, e.g., organoaluminum oxy compound, with an olefin elastomer (D) and another olefin polymer (E), e.g., polyethylene. Alternatively, the combination of propylene polymer (A), olefin elastomer (D) and olefin polymer (E) is prepared by a multi-stage polymerization method. In both cases, the propylene homo- or copolymer (A) may include a second propylene homo- or co-polymer (A′) wherein the ratio of intrinsic viscosities of propylene polymers (A) and (A′) is in the range of 3 to 30. These propylene polymer compositions are excellent in heat resistance, mechanical strength, tensile elongation at break, etc., and can be used in the fabrication of structural materials, films and sheets.

What is claimed:  
     
         1 . A propylene polymer composition which is the product obtained by she process comprising: 
 polymerizing propylene or copolymerizing propylene and at least one olefin selected from the group consisting of ethylene and a-olefins of 4 to 20 carbon atoms in the presence of an olefin polymerization catalyst comprising 
 (i) a transition metal compound (h) represented by the following formula:  
                     
  wherein 
 M is zirconium;  
 R 1  is an alkyl group of 2 to 6 carbon atoms;  
 R 2  is an aryl group selected from the group consisting of phenyl, naphthyl, anthracenyl and phenanthryl, wherein the aryl group is unsubstituted or substituted with a halogen atom or a hydrocarbon group of 1 to 20 carbon atoms;  
 X 1  and X 2  are each a hydrogen atom, a halogen atom, a hydrocarbon group of 1 to 20 carbon atoms, a halogenated hydrocarbon group of 1 to 20 carbon atoms, an oxygen-containing group or a sulfur-containing group; and  
 Y is a divalent silicon-containing group selected from the group consisting of dialkylsilylene, alkylarylsilylene and diarylsilylene; and  
 
 (ii) at least one compound selected from the group consisting of 
 an organoaluminum oxy-compound, and  
 a compound which reacts with the transition metal compound (h) to form an ion pair,  
 to prepare a propylene homo- or co-polymer (A);  
 
   polymerizing or copolymerizing at least one monomer selected from the group consisting of olefins of 2 to 20 carbon atoms and polyenes of 5 to 20 carbon atoms in the presence of an olefin polymerization catalyst which may be the same or different from the aforementioned olefin polymerization catalyst to prepare an olefin elastomer (D) which contains constituent units derived from ethylene, propylene, butene or 4-methyl-1-pentene in an amount of less than 90% by mol, and has a glass transition temperature (Tg) of not higher than 10° C.;    polymerizing one monomer selected from the group consisting of ethylene, butene and 4-methyl-1-pentene or copolymerizing said one monomer with at least one additional monomer selected from the group consisting of olefins of 2 to 20 carbon atoms other than said one monomer and polyenes of 5 to 20 carbon atoms, in the presence of an olefin polymerization catalyst which may be the same as or different from the aforementioned olefin polymerization catalyst to prepare an olefin polymer (E) which contains constituent units derived from said one monomer in an amount of not less than 90% by mol; and    mixing 5 to 95% by weight of the propylene homo- or co-polymer (A), not more than 95% by weight of the olefin elastomer (D), and not more than 95% by weight of the olefin polymer (E).    
     
     
         2 . A propylene polymer composition which is the product obtained by a multi-stage polymerization method comprising the steps of: 
 polymerizing propylene or copolymerizing propylene and at. least one olefin selected from the group consisting of ethylene and α-olefins of 4 to 20 carbon atoms in the presence of an olefin polymerization catalyst comprising 
 (i) a transition metal compound (h) represented by the following formula:  
                     
  wherein 
 M is zirconium;  
 R 1  is an alkyl group of 2 to 6 carbon atoms;  
 R 2  is an aryl group selected from the group consisting of phenyl, naphthyl, anthracenyl and phenanthryl, wherein the aryl group is unsubstituted-or substituted with a halogen atom or a hydrocarbon group of 1 to 20 carbon atoms;  
 X 1  and X 2  are each a hydrogen atom, a halogen atom, a hydrocarbon group of 1 to 20 carbon atoms, a halogenated hydrocarbon group of 1 to 20 carbon atoms, an oxygen-containing group or a sulfur-containing group; and  
 Y is a divalent silicon-containing group selected from the group consisting of dialkylsilylene, alkylarylsilylene and diarylsilylene; and  
 
 (ii) at least one compound selected from the group consisting of 
 an organoaluminum oxy-compound, and  
 a compound which reacts with the transition metal compound (h) to form an ion pair  
 to prepare a propylene homo- or co-polymer (A);  
 
   polymerizing or copolymerizing at least one monomer selected from the group consisting of olefins of 2 to 20 carbon atoms and polyenes of 5 to 20 carbon atoms in the presence of an olefin polymerization catalyst which may be the same as or different from the aforementioned olefin polymerization catalyst to prepare olefin elastomer (D) which contains constituent units derived from ethylene, propylene, butene or 4-methyl-1-pentene in an amount of less than 90% by mol, and has a glass transition temperature (Tg) of not higher than 10° C.;    polymerizing one monomer selected from the group consisting of ethylene, butene and 4-methyl-1-pentene or copolymerizing said one monomer with at least one additional monomer selected from the group consisting of olefin of 2 to 20 carbon atoms other than said one monomer and polyenes of 5 to 20 carbon atoms in the presence of an olefin polymerization catalyst which may be the same as or different from the aforementioned olefin polymerization catalyst to prepare an olefin polymer (E) which contains constituent units derived from said one monomer in an amount of not less than 90% by mol; and    wherein the steps of preparing the propylene homo- or co-polymer (A), preparing the olefin elastomer (D) and preparing the olefin polymer (E) are conducted in an arbitrary order; and the amount of the propylene homo- or co-polymer (A) is 5 to 95% by weight, and the amount of the olefin elastomer (D) is not more than 95% by weight, and the amount of the olefin polymer (E) is not more than 95% by weight.    
     
     
         3 . A propylene polymer composition which is the product obtained by the process comprising: 
 polymerizing propylene or copolymerizing propylene and at least one olefin selected from the group consisting of ethylene and α-olefins of 4 to 20 carbon atoms in the presence of an olefin polymerization catalyst comprising 
 (i) a transition metal compound (h) represented by the following formula:  
                     
  wherein 
 M is zirconium;  
 R 1  is an alkyl group of 2 to 6 carbon atoms;  
 R 2  is an aryl group selected from the group consisting of phenyl, naphthyl, anthracenyl and phenanthryl, wherein the aryl group is unsubstituted or substituted with a halogen atom or a hydrocarbon group of 1 to 20 carbon atoms;  
 X 1  and X 2  are each a hydrogen atom, a halogen atom, a hydrocarbon group of 1 to 20 carbon atoms, a halogenated hydrocarbon group of 1 to 20 carbon atoms, an oxygen-containing group or a sulfur-containing group; and  
 Y is a divalent silicon-containing group selected from the group consisting of dialkylsilylene, alkylarylsilylene and diarylsilylene; and  
 
 (ii) at least one compound selected from the group consisting of 
 an organoaluminum oxy-compound, and  
 a compound which reacts with the transition metal compound (h) to form an ion pair,  
 to prepare a propylene homo- or co-polymer (A);  
 
   polymerizing propylene or copolymerizing propylene and not more than 10% by mol of at least one olefin selected, from the group consisting of ethylene and α-olefins of 4 to 20 carbon atoms in the presence of an olefin polymerization catalyst comprising a metallocene compound or an olefin polymerization catalyst comprising (d) a solid titanium catalyst component and (e) an organometallic compound catalyst component    to prepare a propylene homo- or co-polymer (A′) which contains constituent units derived from propylene in an amount of not less than 90% by mol and is different from the propylene homo- or co-polymer (A),    wherein, the ratio of the intrinsic viscosity (nA) of the propylene homo- or co-polymer (A) and the intrinsic viscosity (η A′ ) of the propylene homo- or co-polymer (A′), measured in decalin at 135° C., (η A /η A′ ) or (η A′ /η A ) is in the range of 3 to 30;    polymerizing or copolymerizing at least one monomer selected from the group consisting of olefins of 2 to 20 carbon atoms and polyenes of 5 to 20 carbon atoms in the presence of an olefin polymerization catalyst which may be the same as or different from the aforementioned olefin polymerization catalyst to prepare an olefin elastomer (D) which contains constituent units derived from ethylene, propylene, butene or 4-methyl-1-pentene in an amount of less than 90% by mol, and has a glass transition temperature (Tg) of not higher than 10° C.;    polymerizing one monomer selected from the group consisting of ethylene, butene and 4-methyl-1-pentene or copolymerizing said one monomer with at least one additional monomer selected from the group consisting of olefins of 2 to 20 carbon atoms other than said one monomer and polyenes of 5 to 20 carbon atoms in the presence of an olefin polymerization catalyst, which may be the same as or different from the aforementioned olefin polymerization catalyst, to prepare an olefin polymer (E) which contains constituent units derived from said one monomer in an amount of not less than 90% by mol; and    mixing 5 to 95% by weight of the propylene homo- or co-polymer (A), not more than 95% by weight of the propylene homo- or co-polymer (A′), not more than 95% by weight of the olefin elastomer (D), and not more than 95% by weight of the olefin polymer (E).    
     
     
         4 . A propylene polymer composition which is the product obtained by a multi-stage polymerization method comprising the steps of: 
 polymerizing propylene or copolymerizing propylene and at least one olefin selected from the group consisting of ethylene and α-olefins of 4 to 20 carbon atoms in the presence of an olefin polymerization catalyst comprising 
 (i) a transition metal compound (h) represented by the following formula:  
                     
  wherein 
 M is zirconium;  
 R 1  is an alkyl group of 2 to 6 carbon atoms;  
 R 2  is an aryl group selected from the group consisting of phenyl, naphthyl, anthracenyl and phenanthryl, wherein the aryl group is unsubstituted or substituted with a halogen atom or a hydrocarbon group of 1 to 20 carbon atoms;  
 X 1  and X 2  are each a hydrogen atom, a halogen atom, a hydrocarbon group of 1 to 20 carbon atoms, a halogenated hydrocarbon group of 1 to 20 carbon atoms, an oxygen-containing group or a sulfur-containing group; and  
 Y is a divalent silicon-containing group selected from the group consisting of dialkylsilylene, alkylarylsilylene and diarylsilylene; and  
 
 (ii) at least one compound selected from the group consisting of 
 an organoaluminum oxy-compound, and  
 a compound which reacts with the transition metal compound (h) to form an ion pair,  
 to prepare a propylene homo- or co-polymer (A);  
 
   polymerizing propylene or copolymerizing propylene and not more than 10% by mol of at least one olefin selected from the group consisting of ethylene and α-olefins of 4 to 20 carbon atoms in the presence of an olefin polymerization catalyst comprising a metallocene compound or an olefin polymerization catalyst comprising (d) a solid titanium catalyst component and (e) an organometallic compound catalyst component,    to prepare a propylene homo- or co-polymer (A′) which contains constituent units derived from propylene in an amount of not less than 90% by mol and is different from the propylene homo- or co-polymer (A), wherein, the ratio of the intrinsic viscosity (η A ) of the propylene homo- or co-polymer (A) and the intrinsic viscosity (η A′ ) of the propylene homo- or co-polymer (A′), measured in decalin at 135° C., (η A /η A′ ) or (η A′ /η A ) is in the range of 3 to 30;    polymerizing or copolymerizing at least one monomer selected from the group consisting of olefins of 2 to 20 carbon atoms and polyenes of 5 to 20 carbon atoms in the presence of an olefin polymerization catalyst which may be the same as or different from the aforementioned olefin polymerization catalyst to prepare an olefin elastomer (D) which contains constituent units derived from ethylene, propylene, butene or 4-methyl-1-pentene in an amount of less than 90% by mol, and has a glass transition temperature (Tg) of not higher than 10° C.;    polymerizing one monomer selected from the group consisting of ethylene, butene and 4-methyl-1-pentene or copolymerizing said one monomer with at least one additional monomer selected from the group consisting of olefins of 2 to 20 carbon atoms other than said one monomer and polyenes of 5 to 20 carbon atoms in the presence of an olefin polymerization catalyst, which may be the same as or different from the aforementioned olefin polymerization catalyst, to prepare an olefin polymer (E) which contains constituent units derived from said one monomer in an amount of not less than 90% by mol; and    wherein the steps of preparing the propylene homo- or co-polymers (A) and (A′), preparing the olefin elastomer (D) and preparing the olefin polymer (E) are conducted in an arbitrary order; and the amount of the propylene homo- or co-polymer (A) is 5 to 95% by weight, the amount of the propylene homo- or co-polymer (A′) is not more than 95% by weight, the amount of the olefin elastomer (D) is not more than 95% by weight and the amount of the olefin polymer (E) is not more than 95% by weight.