EP0166451A2 — Para-phenylene sulfide block copolymers; process …

Claim 1

Independent Claim 129 words

A para-phenylene sulfide block copolymer consisting essentially of a recurring unit (A) and a recurring unit (B) said recurring units (A) being present in the form of a block of 20 to 5,000 units of (A) on the average in the molecular chain, the mol fraction of the recurring units (A) being in the range of 0.50 to 0.98, the block copolymer having a melt viscosity (n * ) of 50 to 100,000 poise as determined at 310°C at a shear rate of 200 sec 1 and having: (a) a glass transition temperature (Tg) of 20 to 80°C, (b) a crystalline melting point (Tm) of 250 to 285°C, and (c) a crystallization index (Ci) of 15 to 45, this value being that of the heat-treated, but not stretch-oriented copolymer.

Claim 2

Dependent Claim 129 words

A para-phenylene sulfide block copolymer consisting essentially of a recurring unit (A) and a recurring unit (B) said recurring units (A) being present in the form of a block of 20 to 5,000 units of (A) on the average in the molecular chain, the mol fraction of the recurring units (A) being in the range of 0.50 to 0.98, the block copolymer having a melt viscosity (n * ) of 50 to 100,000 poise as determined at 310°C at a shear rate of 200 sec 1 and having: (a) a glass transition temperature (Tg) of 20 to 80°C, (b) a crystalline melting point (Tm) of 250 to 285°C, and (c) a crystallization index (Ci) of 15 to 45, this value being that of the heat-treated, but not stretch-oriented copolymer.

Claim 3

Dependent Claim 246 words

A process for producing a p-phenylene sulfide block copolymer which comprises a first step of heating an aprotic polar organic solvent containing a p-dihalobenzene and an alkali metal sulfide to form a reaction liquid (C) containing a p-phenylene sulfide polymer of recurring units (A) and a second step of adding a dihaloaromatic compound consisting essentially of a m-dihalobenzene to the reaction liquid (C) and heating the mixture in the presence of an alkali metal sulfide and an aprotic polar organic solvent to form a block copolymer consisting essentially of a block consisting essentially of recurring units (A) and a block consisting essentially of recurring units (B) , the reaction in the first step being carried out until the degree of polymerization of the recurring units (A) has become 20 to 5,000 of (A) on the average; the reaction in the second step being carried out until the mol fraction (X) of the recurring units (A) in the resulting block copolymer has become 0.50 to 0.98; and the reactions in these steps being carried out so that the resulting p-phenylene sulfide block copolymer will have a melt viscosity (n * ) measured under conditions of 310°C/ 200 sec 1 of 50 to 100,000 poise and have: (a) a glass transition temperature (Tg) of 20 to 80°C, (b) a crystalline melting point (Tm) of 250 to 285°C, and (c) a crystallization index (Ci) of 15 to 45, this value being that of the heat-treated, but not stretch-oriented copolymer.

Claim 4

Dependent Claim 246 words

A process for producing a p-phenylene sulfide block copolymer which comprises a first step of heating an aprotic polar organic solvent containing a p-dihalobenzene and an alkali metal sulfide to form a reaction liquid (C) containing a p-phenylene sulfide polymer of recurring units (A) and a second step of adding a dihaloaromatic compound consisting essentially of a m-dihalobenzene to the reaction liquid (C) and heating the mixture in the presence of an alkali metal sulfide and an aprotic polar organic solvent to form a block copolymer consisting essentially of a block consisting essentially of recurring units (A) and a block consisting essentially of recurring units (B) , the reaction in the first step being carried out until the degree of polymerization of the recurring units (A) has become 20 to 5,000 of (A) on the average; the reaction in the second step being carried out until the mol fraction (X) of the recurring units (A) in the resulting block copolymer has become 0.50 to 0.98; and the reactions in these steps being carried out so that the resulting p-phenylene sulfide block copolymer will have a melt viscosity (n * ) measured under conditions of 310°C/ 200 sec 1 of 50 to 100,000 poise and have: (a) a glass transition temperature (Tg) of 20 to 80°C, (b) a crystalline melting point (Tm) of 250 to 285°C, and (c) a crystallization index (Ci) of 15 to 45, this value being that of the heat-treated, but not stretch-oriented copolymer.

Claim 5

Dependent Claim 37 words

A process according to Claim 2 wherein the dihaloaromatic compound consisting essentially of a m-dihalobenzene is used in the form of a liquid mixture (D) thereof with the aprotic polar organic solvent containing the alkali metal sulfide.

Claim 6

Dependent Claim 262 words

A process for producing a p-phenylene sulfide block copolymer comprising a first step of heating an aprotic polar organic solvent containing a dihaloaromatic compound consisting essentially of a m-dihalobenzene and an alkali metal sulfide to form a reaction liquid (E) containing a m-phenylene sulfide polymer consisting essentially of recurring units (B) and a second step of adding a p-dihalo- benzene to the reaction liquid (E) ana heating tne mixture in the presence of an alkali metal sulfide and an aprotic polar organic solvent to form a block copolymer consisting essentially of the recurring units (B) and recurring units (A) , the reaction in the first step being carried out until the average degree of polymerization of at least 2 and in the range of to wherein X represents a mol fraction of the recurring units (A) in the resulting block copolymer which is in the range of 0.50 to 0.98 has been obtained; the reaction in the second step being carried out until the mol fraction (X) of the recurring units (A) in the resulting block copolymer has become 0.50 to 0.98; and the reactions in these steps being carried out so that the resulting p-phenylene sulfide block copolymer will have a melt viscosity (n * ) measured under conditions of 310°C/200 sec 1 of 50 to 100,000 P and have: (a) a glass transition temperature (Tg) of 20 to 80°C, (b) a crystalline melting point (Tm) of 250 to 285°C, and (c) a crystallization index (Ci) of 15 to 45, this value being that of the heat-treated, but not stretch-oriented copolymer.

Claim 7

Dependent Claim 262 words

A process for producing a p-phenylene sulfide block copolymer comprising a first step of heating an aprotic polar organic solvent containing a dihaloaromatic compound consisting essentially of a m-dihalobenzene and an alkali metal sulfide to form a reaction liquid (E) containing a m-phenylene sulfide polymer consisting essentially of recurring units (B) and a second step of adding a p-dihalo- benzene to the reaction liquid (E) ana heating tne mixture in the presence of an alkali metal sulfide and an aprotic polar organic solvent to form a block copolymer consisting essentially of the recurring units (B) and recurring units (A) , the reaction in the first step being carried out until the average degree of polymerization of at least 2 and in the range of to wherein X represents a mol fraction of the recurring units (A) in the resulting block copolymer which is in the range of 0.50 to 0.98 has been obtained; the reaction in the second step being carried out until the mol fraction (X) of the recurring units (A) in the resulting block copolymer has become 0.50 to 0.98; and the reactions in these steps being carried out so that the resulting p-phenylene sulfide block copolymer will have a melt viscosity (n * ) measured under conditions of 310°C/200 sec 1 of 50 to 100,000 P and have: (a) a glass transition temperature (Tg) of 20 to 80°C, (b) a crystalline melting point (Tm) of 250 to 285°C, and (c) a crystallization index (Ci) of 15 to 45, this value being that of the heat-treated, but not stretch-oriented copolymer.

Claim 8

Dependent Claim 31 words

A process according to Claim 4 wherein the p-dihalobenzene is used in the form of a liquid mixture (F) thereof with the aprotic polar organic solvent containing the alkali metal sulfide.

Claim 9

Dependent Claim 322 words

A process for producing a p-phenylene sulfide block copolymer comprising a first step of heating an aprotic polar organic solvent containing a p-dihalobenzene and an alkali metal sulfide to form a reaction liquid (C) containing a p-phenylene sulfide polymer consisting essentially of recurring units (A) , a second step of heating an aprotic polar organic solvent containing a dihaloaromatic compound consisting essentially of a m-dihalobenzene and an alkali metal sulfide to form a reaction liquid (E) containing a m-phenylene sulfide polymer consisting essentially of recurring units (B) , and a third step of mixing the reaction liquids (C) and (E) thus obtained and heating the mixture to form a p-phenylene sulfide block copolymer consisting essentially of blocks of said recurring units (A) and the recurring units (B), the reaction in the first step being carried out until the average degree of polymerization of 20 to 5,000 recurring units (A) on the average has been obtained; the reaction in the second step being carried out until the average degree of polymerization of at least 2 and in the range of to wherein X represents a mol fraction of the recurring units (A) in the resulting block copolymer which is in the range of 0.50 to 0.98 has been obtained; the reaction in the third step being carried out so that the mol fraction (X) of the recurring units (A) in the resulting block copolymer will be in the range of 0.50 to 0.98; and the reactions in these steps being carried out so that the resulting p-phenylene sulfide block copolymer will have a melt viscosity (n * ) measured under conditions of 3l0°C/200 sec -1 of 50 to 100,000 poise and have: (a) a glass transition temperature (Tg) of 20 to 80°C, (b) a crystalline melting point (Tm) of 250 to 285°C, and (c) a crystallization index (Ci) of 15 to 45, this value being that of the heat-treated, but not stretch-oriented copolymer.

Claim 10

Dependent Claim 322 words

A process for producing a p-phenylene sulfide block copolymer comprising a first step of heating an aprotic polar organic solvent containing a p-dihalobenzene and an alkali metal sulfide to form a reaction liquid (C) containing a p-phenylene sulfide polymer consisting essentially of recurring units (A) , a second step of heating an aprotic polar organic solvent containing a dihaloaromatic compound consisting essentially of a m-dihalobenzene and an alkali metal sulfide to form a reaction liquid (E) containing a m-phenylene sulfide polymer consisting essentially of recurring units (B) , and a third step of mixing the reaction liquids (C) and (E) thus obtained and heating the mixture to form a p-phenylene sulfide block copolymer consisting essentially of blocks of said recurring units (A) and the recurring units (B), the reaction in the first step being carried out until the average degree of polymerization of 20 to 5,000 recurring units (A) on the average has been obtained; the reaction in the second step being carried out until the average degree of polymerization of at least 2 and in the range of to wherein X represents a mol fraction of the recurring units (A) in the resulting block copolymer which is in the range of 0.50 to 0.98 has been obtained; the reaction in the third step being carried out so that the mol fraction (X) of the recurring units (A) in the resulting block copolymer will be in the range of 0.50 to 0.98; and the reactions in these steps being carried out so that the resulting p-phenylene sulfide block copolymer will have a melt viscosity (n * ) measured under conditions of 3l0°C/200 sec -1 of 50 to 100,000 poise and have: (a) a glass transition temperature (Tg) of 20 to 80°C, (b) a crystalline melting point (Tm) of 250 to 285°C, and (c) a crystallization index (Ci) of 15 to 45, this value being that of the heat-treated, but not stretch-oriented copolymer.

Claim 11

Dependent Claim 130 words

A molding of a p-phenylene sulfide block copolymer consisting essentially of recurring units (A) and recurring units (B) said recurring units (A) being present in the form of a block of 20 to 5,000 units of (A) on the average in the molecular chain, the mol fraction of the recurring units (A) being in the range of 0.50 to 0.98, and the copolymer having a melt viscosity (n * ) of 50 to 100,000 P as determined at 310°C at a shear rate of 200 sec 1 and having: (a) a glass transition temperature (Tg) of 20 to 80°C, (b) a crystalline melting point (Tm) of 250 to 285°C, and (c) a crystallization index (Ci) of 15 to 45, this value being that of the heat-treated, but not draw-oriented copolymer.

Claim 12

Dependent Claim 130 words

A molding of a p-phenylene sulfide block copolymer consisting essentially of recurring units (A) and recurring units (B) said recurring units (A) being present in the form of a block of 20 to 5,000 units of (A) on the average in the molecular chain, the mol fraction of the recurring units (A) being in the range of 0.50 to 0.98, and the copolymer having a melt viscosity (n * ) of 50 to 100,000 P as determined at 310°C at a shear rate of 200 sec 1 and having: (a) a glass transition temperature (Tg) of 20 to 80°C, (b) a crystalline melting point (Tm) of 250 to 285°C, and (c) a crystallization index (Ci) of 15 to 45, this value being that of the heat-treated, but not draw-oriented copolymer.

Claim 13

Dependent Claim 17 words

A molding comprising a p-phenylene sulfide block copolymer according to Claim 7 which is film or fiber.

Claim 14

Dependent Claim 23 words

A molding comprising a p-phenylene sulfide block copolymer according to Claim 7 which is an injection-molded product, extrusion-molded product or electric wire coating.

Claim 15

Dependent Claim 124 words

A printed wiring board composed of an insulating base which is a molded plate comprising a composite of 50 to 95 vol. % of a polymer comprising mainly a phenylene sulfide block copolymer and 5 to 50 vol. % of a fibrous reinforcing material and a metal layer of a circuit pattern formed on the surface of the base, said phenylene sulfide block copolymer comprising 20 to 5,000 recurring units on the average in the molecular chain, said recurring units having a mol fraction of 0.50 to 0.98 and said copolymer having a melt viscosity (n * ) of 300 to 50,000 poise as determined at 310°C at a shear rate of 200 sec 1 and a crystalline melting point of 200 to 350°C.

Claim 16

Dependent Claim 124 words

A printed wiring board composed of an insulating base which is a molded plate comprising a composite of 50 to 95 vol. % of a polymer comprising mainly a phenylene sulfide block copolymer and 5 to 50 vol. % of a fibrous reinforcing material and a metal layer of a circuit pattern formed on the surface of the base, said phenylene sulfide block copolymer comprising 20 to 5,000 recurring units on the average in the molecular chain, said recurring units having a mol fraction of 0.50 to 0.98 and said copolymer having a melt viscosity (n * ) of 300 to 50,000 poise as determined at 310°C at a shear rate of 200 sec 1 and a crystalline melting point of 200 to 350°C.

Claim 17

Dependent Claim 109 words

ll. A composition for sealing electronic parts comprising 100 parts by weight of a synthetic resin component and 20 to 300 parts by weight of an inorganic filler, characterized in that the synthetic resin component comprises mainly a phenylene sulfide block copolymer consisting essentially of recurring units and recurring units wherein the former recurring units form blocks have an average degree of polymerization of 20 to 2,000 bonded in the molecular chain and have a mol fraction in the range of 0.50 to 0.95, said copolymer having a melt viscosity of 10 to 1,500 P (as determined at 310°C and at a shear rate of 200 sec l ).

Claim 18

Dependent Claim 109 words

ll. A composition for sealing electronic parts comprising 100 parts by weight of a synthetic resin component and 20 to 300 parts by weight of an inorganic filler, characterized in that the synthetic resin component comprises mainly a phenylene sulfide block copolymer consisting essentially of recurring units and recurring units wherein the former recurring units form blocks have an average degree of polymerization of 20 to 2,000 bonded in the molecular chain and have a mol fraction in the range of 0.50 to 0.95, said copolymer having a melt viscosity of 10 to 1,500 P (as determined at 310°C and at a shear rate of 200 sec l ).

Claim 19

Dependent Claim 22 words

A composition for sealing electronic parts according to Claim 11 wherein the synthetic resin component comprises the phenylene sulfide block copolymer alone.

Claim 20

Dependent Claim 31 words

A composition for sealing electronic parts according to Claim 11 wherein the synthetic resin component is a phenylene sulfide block copolymer mixture comprising up to 40 wt.% of m-phenylene sulfide polymer.

Claim 21

Dependent Claim 32 words

A composition for sealing electronic parts according to Claim 11 wherein the synthetic resin component is a phenylene sulfide block copolymer mixture comprising up to 40 wt. % of p-phenylene sulfide polymer.

Claim 22

Dependent Claim 43 words

A composition for sealing electronic parts according to any of Claims 11 to 14 wherein the inorganic filler is a fibrous filler having a length of up to 0.5 mm or a non-fibrous filler having a particle diameter of up to 0.5 mm.

Claim 23

Dependent Claim 118 words

A process for sealing electronic parts characterized in that the electronic parts are sealed by an injection molding method with a sealing composition comprising 100 parts by weight of a synthetic resin component and 20 to 300 parts by weight of an inorganic filler wherein the synthetic resin component comprises mainly a phenylene sulfide block copolymer consisting essentially of recurring units and recurring units . in which the former recurring units form blocks have an average degree of polymerization of 20 to 2,000 bonded in the molecular chain and have a mol fraction in the range of 0.50 to 0.95, said copolymer having a melt viscosity of 10 to 1,500 P (310°C, shear rate: 200 sec -1 ).

Claim 24

Dependent Claim 118 words

A process for sealing electronic parts characterized in that the electronic parts are sealed by an injection molding method with a sealing composition comprising 100 parts by weight of a synthetic resin component and 20 to 300 parts by weight of an inorganic filler wherein the synthetic resin component comprises mainly a phenylene sulfide block copolymer consisting essentially of recurring units and recurring units . in which the former recurring units form blocks have an average degree of polymerization of 20 to 2,000 bonded in the molecular chain and have a mol fraction in the range of 0.50 to 0.95, said copolymer having a melt viscosity of 10 to 1,500 P (310°C, shear rate: 200 sec -1 ).

Claim 25

Dependent Claim 23 words

l7. The para-phenylene sulfide block copolymer as claimed in Claim 1, which copolymer is produced by the process as claimed in Claim 4.

Claim 26

Dependent Claim 24 words

The molding of a p-phenylene sulfide block copolymer as claimed in Claim'7, which copolymer is produced by the process as claimed in Claim 4.

Claim 27

Dependent Claim 23 words

The printed circuit board as claimed in Claim 10, in which the block copolymer is produced by the process claimed in Claim 4.

Claim 28

Dependent Claim 26 words

The process for sealing electronic parts as claimed in Claim 16, in which the block copolymer is produced by the process as claimed in Claim 4.

Claim 29

Dependent Claim 22 words

The para-phenylene sulfide block copolymer as claimed in Claim 1, which polymer is produced by the process as claimed in Claim 2.

Claim 30

Dependent Claim 25 words

The molding of a p-phenylene sulfide block copolymer as claimed in Claim 7, which copolymer is produced by the process as claimed in Claim 2.

Claim 31

Dependent Claim 23 words

The printed circuit board as claimed in Claim 10, in which the block copolymer is produced by the process claimed in Claim 2.

Claim 32

Dependent Claim 26 words

The process for sealing electronic parts as claimed in Claim 16, in which the block copolymer is produced by the process as claimed in Claim 2.

Para-phenylene sulfide block copolymers; process for the production of the same and use thereof

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