CN101314660A - Method for preparing high impact modified material with waste and old polystyrene plastics - Google Patents
Method for preparing high impact modified material with waste and old polystyrene plastics Download PDFInfo
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Abstract
The invention discloses a method for preparing high-impact modified material from waste polystyrene plastic, which comprises the following steps: uniformly mixing 60 to 80 parts of waste polystyrene, 5 to 10 parts of polyethylene, 10 to 30 parts of elastomer, compatibilizer, etc. by stirring, adding to a screw extruder, and melting and blending at 150 to 210 DEG C, wherein the melt index ratio of polyethylene to polystyrene is equal to or less than 0.5. Due to the addition of small amount of polyethylene, the viscosity ratio of polyethylene to polystyrene and the crystallization behavior and the phase size of polyethylene can be controlled by restricting the melt index of waste polystyrene and polyethylene, so that the obtained modified material has a notched impact strength 8 to 10 times as high as that of original waste polystyrene and can maintain or even improve the tensile strength of polystyrene. The prepared modified polystyrene can be used for producing parts of middle- and high-level household appliances such as computer and air conditioner as the substitute of high-impact polystyrene new material, thus achieving remarkable social and economic benefits.
Description
Technical field
The invention belongs to waste and old polystyrol and reclaim the modification technology field, be specifically related to a kind of method of utilizing waste and old polystyrene plastics to prepare high impact modified material.
Background technology
That polystyrene (PS) has is transparent, good moldability, good rigidly, easy dyeing, agent of low hygroscopicity and advantage such as cheap, has obtained widespread use in industries such as packing, electronics, building, automobile, household electrical appliances, instrument, daily necessities and toys.Yet because polystyrene is difficult to degraded, cause waste materials such as polystyrene and polystyrene foamed to increase day by day, this not only causes serious pollution to environment, and resource has been formed great waste, especially in today of oil worsening shortages.
In order to solve the waste and old polystyrene plastics pollution on the environment, and make full use of resource, at present utilize the approach of waste and old polystyrene plastics to be broadly divided into two classes both at home and abroad: a class is to make industrial chemicals (W.Kaminsky such as fuel products such as gasoline, kerosene, diesel oil and vinylbenzene, benzene, toluene by thermo-cracking, M.Predel, A.Sadiki.Feedstock recycling of polymers by pyrolysis in a fluidised bed.Polymer Degradationand Stability, 85 (2004): 1045-1050; Paul T.Williamsn, y and Ranbir Bagri.Hydrocarbongases and oils from the recycling of polystyrene waste by catalytic pyrolysis.ENERGYRESEARCH, 28 (2004): 31-44).One class is to prepare new product by modification mode: (1) preparation polystyrene series tackiness agent or coating.But the glued membrane poor adhesive force that these tackiness agent or coating form, easily come off, as it is carried out modification, and no matter be physically modified or chemical modification, waste polystyrene plastic must be dissolved in benzene or the toluene solvant, this will produce secondary pollution (Chen Lijun etc. to environment again, utilize waste and old polystyrene plastics to prepare tailor-(made) coating .2005,5:16-20; Li Cuizhen etc., the waste old polystyrene foamed plastic application in coating, coatings industry, 2005,35 (4): 35-37; What is newly fast etc., the development of waste and old polystyrol modified adhesive, Packaging Engineering, 2005,26 (3): 38-40).(2) directly pulverize back and cement mixing and make light-weight building material.But the density of matrix and polystyrene foamed base-material differs greatly in the light concrete product of making, laminated segregation (the Huang Farong that in preparation process, causes this material easily, Chen Tao, Shen Xuening. the recycle of macromolecular material. Beijing: Chemical Industry Press, 2002:195-196).(3) system flocculation agent.This flocculation agent is to adopt the method for introducing sulfonic acid on the PS phenyl ring to make its modification and have water-soluble, thereby processing (the Imene Bekri-Abbesa that is used for sewage, Sami Bayoudh, MohamedBaklouti.A technique for purifying wastewater with polymeric flocculant produced fromwaste plastic.Desalination, 204 (2007): 198-203), but the waste and old polystyrol amount that this method reclaims is less.Above-mentioned recycling approach exists that regeneration times is limited, resource utilization is low, can produce secondary pollution problems.
It is to make full use of recyclable resource, reduce the pollution of waste or used plastics to environment that blending and modifying reclaims polystyrene, expand the regenerated polystyrene material and provide a valid approach, and the low cost of waste or used plastics also can be enterprise and brings considerable economic in the application of wide spectrum more.Polystyrene (PS) and the formed PS particle of polystyrene foamed (EPS) reclaimed materials matter is crisp, resistance to impact shock is low, coming the impact property of modified polystyrene with blend rubber is one of effective, the most most economical method of improving plastics performance that grows up nearly decades (Huang Farong, Chen Tao, Shen Xuening. the macromolecular material recycle. Beijing: Chemical Industry Press, 2002:204～206).Yet being added in of rubber improves the material impact flexible simultaneously, but greatly reduces the rigidity and the intensity of material, makes the waste and old polystyrol that reclaims after rubber toughened modification at present can only be used to make low-end products such as wrapping material, articles for daily use.
How little amplitude reduces rigidity and intensity when increasing waste and old polystyrol impelling strength, can also reduce the cost of material simultaneously, becomes the focus of this area science and technology research worker to the research of waste and old polystyrol blending and modifying.
Summary of the invention
The objective of the invention is problem, provide a kind of technology simply to utilize waste and old polystyrene plastics to prepare the method for high impact modified material at the prior art existence.
The method of utilizing waste and old polystyrene plastics to prepare high impact modified material provided by the invention is on the basis of having furtherd investigate plastic toughening mechanism, utilize rubber and the polyethylene mode of toughness reinforcing waste and old polystyrol simultaneously, and recently regulate viscosity ratio between them by prescription being designed simultaneously with waste and old polystyrol and poly melting index, thereby reach poly crystallization behavior of control and phase morphology, to obtain to replace fully the modified waste old polystyrene material of high-impact polystyrene.
The method of utilizing waste and old polystyrene plastics to prepare high impact modified material provided by the invention, this method is earlier 60～80 parts of waste and old polystyrols, 5～10 parts of polyethylene, 10～30 parts on elastomerics, 4～10 parts of expanding materials and oxidation inhibitor to be mixed for 0.001～0.004 part, put into screw extrusion press then, obtain at 150～210 ℃ of following melt blendings of temperature, used umber is weight part in this method prescription, and the melting index of used polyethylene and polystyrene is than≤0.5.
The melting index of used waste and old polystyrol is 10～25g/10min in the aforesaid method, and poly melting index is 0.05～6g/10min.
Used polyethylene is any in ultrahigh molecular weight polyethylene(UHMWPE), high density polyethylene(HDPE) or their reclaimed materials in the aforesaid method.
Used elastomerics is any in ethylene-octene copolymer elastomerics POE, ethylene-propylene rubber(EPR), styrene-butadiene rubber(SBR), cis-1,4-polybutadiene rubber, the natural rubber in the aforesaid method.Therein ethylene-octene copolymer elastomerics POE is meant that U.S. DuPontDOW chemical company adopts the POE of constrained geometry catalyst technology and relevant INSITE process exploitation.
Used expanding material is any in styrene-ethylene copolymers, styrene-butadiene copolymer, SIS/SEBS, styrene-isoprene-phenylethene thermoplastic elastomer, the styrene-butadiene-styrene synthetic rubber in the aforesaid method.
Used oxidation inhibitor is the conventional oxidation inhibitor that use this area in the aforesaid method, specifically can be antioxidant 1010,136,1076,300,264 etc.
The inventive method designs interpolation polyethylene a small amount of and polystyrene melting index coupling in prescription be the key that obtains high impact modified material.Find that under study for action the Tc of the Tc of PE and pure PE is compared almost constant (see figure 1) in the mixed system when the melting index ratio of polyethylene and polystyrene is less than or equal to 0.5.This explanation polyethylene disperses the particle diameter in the polystyrene matrix bigger, and the heterogeneous nucleation agent that comprises is more, and polyethylene can heterogeneous nucleation crystallization under lower condensate depression, so can keep higher Tc; And because the also big (see figure 2) of the dispersed phase size of polyethylene in the polystyrene matrix, form easily and keep a kind of filamentary structure (see figure 3).The polyethylene of this filamentary structure is when being subjected to surging force, can playing in crazing or crackle on the one hand puts up a bridge does in order to cracking that stops crazing and the effect of playing the termination crackle, lot of energy on the other hand can dissipate in fiber is pulled out process with unsticking, thereby improved the shock strength of material greatly, made the notched Izod impact strength that records with this mixed system gained material can reach 9.3KJ/m
2But when the melting index of polyethylene and polystyrene than greater than 0.5 the time, poly Tc just will descend greatly in this mixed with polymers system, drops to 80 ℃ of left and right sides (see figure 1)s for about 117 ℃ from the Tc of pure PE.This shows that the polyethylene under this melting index is dispersed into small droplets easily in the polystyrene matrix, and small droplets does not contain or contain effective heterogeneous nucleation agent seldom, and polyethylene can only homogeneous nucleation crystallization under higher condensate depression; And because the relative viscosity of polyethylene in polystyrene is less, the too small (see figure 4) of dispersed phase size in the polystyrene matrix, not only do not have the effect that stops the crazing cracking and stop crazing, also can become focal point of stress and induce initiation crazing (see figure 5), make with the notched Izod impact strength of this mixed system gained material intensity (6.0KJ/m more toughness reinforcing than gum
2) also low, have only 3.7KJ/m
2
In addition, because the present invention also defines the melting index of waste and old polystyrol in the above technical solution that provides should be at 10～25g/10min, poly melting index should be at 0.05～6g/10min, and the melting index of polyethylene and polystyrene ratio is less than or equal to 0.5.The viscosity that can reflect polymkeric substance according to melt index indirectly, and its viscosity and their melting index (MFI) are the characteristics of inverse relation, so just can control their viscosity indirectly by limiting polystyrene and poly melting index, promptly the melting index by reducing polyethylene and polystyrene is than (MFI
PE/ MFI
PS≤ 0.5) enlarges their viscosity ratio, when the increase of the relative viscosity of polyethylene in the polystyrene matrix can stop the homogeneous phase crystallization behavior of a small amount of polyethylene in the polystyrene matrix and the formation of minimum PE particle, thereby guaranteed that the dispersed phase size of polyethylene in the polystyrene matrix increases, and makes it to form and kept this polyethylene fibre structure.
The present invention has following advantage:
1, because the present invention is adding a small amount of polyethylene in the rubber plastic blend toughening modifying waste and old polystyrol system usually, and by limiting viscosity ratio and poly crystallization behavior and the poly phase morphology that polystyrene and poly melting index are controlled both, thereby the notched Izod impact strength of the toughening modifying waste and old polystyrol material that obtains is more than 8～10 times of former waste and old polystyrol, and when the green strength of waste and old polystyrol during less than 23MPa, its tensile strength also can be brought up to more than the 23MPa when its toughness increases, sees Table 1.
2, because the polyethylene that the present invention adds can be with elastomerics coordination plasticizing waste and old polystyrol, the shock strength of the material that obtains is increased greatly, and poly adding can keep even improve the tensile strength of polystyrene, thereby the invention solves prior art with the single problem that tensile strength sharply descends when shock strength improves that exists when toughness reinforcing of elastomerics.
3, since the present invention added melting index with respect to the less polyethylene of polystyrene after, this full-bodied polyethylene has formed a kind of fibrous texture in the polystyrene matrix, when this fibrous polyethylene is subjected to surging force, can play in crazing or crackle puts up a bridge does in order to cracking that stops crazing and the effect of playing the termination crackle, and the lot of energy that can in this fiber is pulled out process with unsticking, dissipate, thereby improved the shock strength of material greatly, even the notched Izod impact strength that also surpasses the special high-impact polystyrene for preparing sees Table 21 times more.
4, because the present invention has introduced polyethylene in toughened system, the elastomerics consumption is reduced, and the present invention also can use waste and old high density polyethylene(HDPE), the ultrahigh molecular weight polyethylene(UHMWPE) of melting index between 0.05～6g/10min, thereby can further reduce the cost of the modified waste old polystyrene material that obtains.
5, method provided by the invention is simple, technology controlling and process is easy, the high-impact waste and old polystyrol modifying material that is obtained can substitute the high-impact polystyrene virgin material and be used for middle and high end household electrical appliance parts such as scheduler, air-conditioning, refrigerator, colour TV, both solved problem of environmental pollution, started a new approach for recycling waste and old polystyrol again, had broad application prospects and economic results in society.
The mechanical property of waste and old PS of table 1 and modified system of the present invention relatively
| Material | Molten refer to (g/10min) of PE | Molten refer to (g/10min) of PS | Izod notched Izod impact strength (KJ/m 2) | Tensile strength (MPa) |
| Waste and old polystyrol | 0 | 15～25 | 0.97～1.02 | 18.1～32.3 |
| PS/ elastomerics/PE/ expanding material | 0.05～6 | 15～25 | 8.12～10.5 | 23.1～26.6 |
The mechanical property of typical HIPS of table 2 and modified system of the present invention relatively
| Mechanical property | Polystyrene after toughness reinforcing | HIPS |
| Tensile strength (MPa) | 23～26 | 21 |
| Izod notched Izod impact strength (KJ/m 2) | 8.12～10.5 | 4.5 |
The HIPS performance data derives from document in this table: Ostromislensky II.US Pat.1,613,673.
Description of drawings
Fig. 1 is the crystallization curve of PS/POE/SBS/HDPE (75/15/5/5) system of the present invention's preparation, wherein curve a is the crystallization curve of 0.05g/10minHDPE system for the melting index of adding, and b is the crystallization curve of 20g/10minHDPE system for the melting index of adding.
Fig. 2 is the face sem photograph absolutely of quenching of PS/POE/SBS/HDPE (75/15/5/5) system of the present invention's preparation, and the melting index of wherein used HDPE is 0.05g/10min, and the melting index of PS is 20g/10min.
Fig. 3 for the Impact Test of PS/POE/SBS/HDPE (75/15/5/5) system of the present invention preparation after profile scanning Electronic Speculum figure, the melting index of wherein used HDPE is 0.05g/10min, the melting index of PS is 20g/10min.
Fig. 4 is the face sem photograph absolutely of quenching of PS/POE/SBS/HDPE (75/15/5/5) system of the present invention's preparation, and the melting index of wherein used HDPE is 20g/10min, and the melting index of PS is 20g/10min.
Fig. 5 for the Impact Test of PS/POE/SBS/HDPE (75/15/5/5) system of the present invention preparation after profile scanning Electronic Speculum figure, the melting index of wherein used HDPE is 20g/10min, the melting index of PS is 20g/10min.
Embodiment
Also the invention will be further described to provide embodiment below.Be necessary to be pointed out that at this following examples can not be interpreted as limiting the scope of the invention; if the person skilled in the art in this field makes some nonessential improvement and adjustment according to the invention described above content to the present invention, still belong to protection domain of the present invention.
The used umber of each component is weight part in following examples.
In addition, Izod notched Izod impact strength that what deserves to be explained is product of the present invention is according to GB/T 1834-1996 test, and tensile strength is then tested according to GB/T 1040-92 standard.
Be that 10 parts in 72 parts of waste and old polystyrols, the styrene-butadiene rubber(SBR) of 20g/10min, 10 parts and 0.001 part antioxidant 1076 of 8 parts of high density polyethylene(HDPE)s, SIS/SEBS that melting index is 5.5g/10min mix with melting index earlier, put into twin screw extruder then, be respectively 150 ℃, 170 ℃, 190 ℃, 210 ℃, 210 ℃, 200 ℃ following melt blendings in each district's temperature and obtain toughening modifying waste and old polystyrol material.The notched Izod impact strength that this material records is 9.27KJ/m
2, tensile strength is 24.13MPa.
Embodiment 2
Be that 28 parts of 60 parts of waste and old polystyrols, the natural rubbers of 23g/10min, 7 parts and 0.002 part antioxidant 1010 of 5 parts of high density polyethylene(HDPE)s, styrene-isoprene-phenylethene thermoplastic elastomer that melting index is 3.0g/10min mix with melting index earlier, put into twin screw extruder then, be respectively 150 ℃, 170 ℃, 190 ℃, 210 ℃, 210 ℃, 200 ℃ following melt blendings in each district's temperature and obtain toughening modifying waste and old polystyrol material.The notched Izod impact strength that this material records is 10.22KJ/m
2, tensile strength is 23.12MPa.
Embodiment 3
80 parts of waste and old polystyrols, polyolefin elastomer POE10 part, the melting index that with melting index is 12g/10min earlier is that 4 parts and 0.003 part antioxidant 1010 of 6 parts of ultrahigh molecular weight polyethylene(UHMWPE) reclaimed materials, styrene-grafted ethylene copolymer of 6g/10min mixes, put into single screw extrusion machine then, be respectively 150 ℃, 170 ℃, 190 ℃, 210 ℃, 210 ℃, 200 ℃ following melt blendings in each district's temperature and obtain toughening modifying waste and old polystyrol material.The notched Izod impact strength that this material records is 8.12KJ/m
2, tensile strength is 25.55MPa.
Embodiment 4
15 parts in 75 parts of waste and old polystyrols, the ethylene-propylene rubber(EPR), the melting index that with melting index are 10g/10min earlier are that 5 parts of 1.1g/10min ultrahigh molecular weight polyethylene(UHMWPE) reclaimed materials, 5 parts and 0.004 part antioxidant 300 of styrene-butadiene copolymer mix, put into single screw extrusion machine then, be respectively 150 ℃, 170 ℃, 190 ℃, 210 ℃, 210 ℃, 200 ℃ following melt blendings in each district's temperature and obtain toughening modifying waste and old polystyrol material.The notched Izod impact strength that this material records is 8.44KJ/m
2, tensile strength is 24.8MPa.
Embodiment 5
Be that 20 parts of 65 parts of waste and old polystyrols, the cis-1,4-polybutadiene rubbers of 25g/10min, 5 parts and 0.003 part oxidation inhibitor 136 of 10 parts of recovery high density polyethylene(HDPE)s, styrene-butadiene-styrene synthetic rubber that melting index is 0.2g/10min mix with melting index earlier, put into twin screw extruder then, be respectively 150 ℃, 170 ℃, 190 ℃, 210 ℃, 210 ℃, 200 ℃ following melt blendings in each district's temperature and obtain toughening modifying waste and old polystyrol material.The notched Izod impact strength that this material records is 9.2KJ/m
2, tensile strength is 23.45MPa.
Embodiment 6
75 parts of waste and old polystyrols, polyolefin elastomer POE15 part, the melting index that with melting index is 20g/10min earlier is that 5 parts and 0.002 part antioxidant 300 of 5 parts of high density polyethylene(HDPE) reclaimed materials, styrene-butadiene-styrene multipolymer of 0.05g/10min mixes, put into twin screw extruder then, be respectively 150 ℃, 170 ℃, 190 ℃, 210 ℃, 210 ℃, 200 ℃ following melt blendings in each district's temperature and obtain toughening modifying waste and old polystyrol material.The notched Izod impact strength that this material records is 8.80KJ/m
2, tensile strength is 24.3MPa.
Claims (8)
1, a kind of method of utilizing waste and old polystyrene plastics to prepare high impact modified material, this method is that first 4～10 parts of 10～30 parts on 5～10 parts of 60～80 parts of waste and old polystyrols, polyethylene, elastomerics, expanding materials and oxidation inhibitor of inciting somebody to action mixes for 0.001～0.004 part, put into screw extrusion press then, obtain at 150～210 ℃ of following melt blendings of temperature, used umber is weight part in this method prescription, and the melting index of used polyethylene and polystyrene is than≤0.5.
2, the method for utilizing waste and old polystyrene plastics to prepare high impact modified material according to claim 1, the melting index of used waste and old polystyrol is 10～25g/10min in this method, poly melting index is 0.05～6g/10min.
3, the method for utilizing waste and old polystyrene plastics to prepare high impact modified material according to claim 1 and 2, used polyethylene is any in ultrahigh molecular weight polyethylene(UHMWPE), high density polyethylene(HDPE) or their reclaimed materials in this method.
4, the method for utilizing waste and old polystyrene plastics to prepare high impact modified material according to claim 1 and 2, used elastomerics is any in ethylene-octene copolymer elastomerics POE, ethylene-propylene rubber(EPR), styrene-butadiene rubber(SBR), cis-1,4-polybutadiene rubber, the natural rubber in this method.
5, the method for utilizing waste and old polystyrene plastics to prepare high impact modified material according to claim 3, used elastomerics is any in ethylene-octene copolymer elastomerics POE, ethylene-propylene rubber(EPR), styrene-butadiene rubber(SBR), cis-1,4-polybutadiene rubber, the natural rubber in this method.
6, the method for utilizing waste and old polystyrene plastics to prepare high impact modified material according to claim 1 and 2, used expanding material is any in styrene-ethylene copolymers, styrene-butadiene copolymer, SIS/SEBS, styrene-isoprene-phenylethene thermoplastic elastomer, the styrene-butadiene-styrene multipolymer (SBS) in this method.
7, the method for utilizing waste and old polystyrene plastics to prepare high impact modified material according to claim 3, used expanding material is any in styrene-ethylene copolymers, styrene-butadiene copolymer, SIS/SEBS, styrene-isoprene-phenylethene thermoplastic elastomer, the styrene-butadiene-styrene synthetic rubber in this method.
8, the method for utilizing waste and old polystyrene plastics to prepare high impact modified material according to claim 5, used expanding material is any in styrene-ethylene copolymers, styrene-butadiene copolymer, SIS/SEBS, styrene-isoprene-phenylethene thermoplastic elastomer, the styrene-butadiene-styrene synthetic rubber in this method.
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