CN103756133A - Fly ash-modified polypropylene composition and preparation method thereof - Google Patents
Fly ash-modified polypropylene composition and preparation method thereof Download PDFInfo
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- CN103756133A CN103756133A CN201310738141.9A CN201310738141A CN103756133A CN 103756133 A CN103756133 A CN 103756133A CN 201310738141 A CN201310738141 A CN 201310738141A CN 103756133 A CN103756133 A CN 103756133A
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K13/00—Use of mixtures of ingredients not covered by one single of the preceding main groups, each of these compounds being essential
- C08K13/02—Organic and inorganic ingredients
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C48/00—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor
- B29C48/03—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor characterised by the shape of the extruded material at extrusion
- B29C48/04—Particle-shaped
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29B—PREPARATION OR PRETREATMENT OF THE MATERIAL TO BE SHAPED; MAKING GRANULES OR PREFORMS; RECOVERY OF PLASTICS OR OTHER CONSTITUENTS OF WASTE MATERIAL CONTAINING PLASTICS
- B29B9/00—Making granules
- B29B9/02—Making granules by dividing preformed material
- B29B9/06—Making granules by dividing preformed material in the form of filamentary material, e.g. combined with extrusion
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C48/00—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor
- B29C48/25—Component parts, details or accessories; Auxiliary operations
- B29C48/36—Means for plasticising or homogenising the moulding material or forcing it through the nozzle or die
- B29C48/395—Means for plasticising or homogenising the moulding material or forcing it through the nozzle or die using screws surrounded by a cooperating barrel, e.g. single screw extruders
- B29C48/40—Means for plasticising or homogenising the moulding material or forcing it through the nozzle or die using screws surrounded by a cooperating barrel, e.g. single screw extruders using two or more parallel screws or at least two parallel non-intermeshing screws, e.g. twin screw extruders
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C48/00—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor
- B29C48/25—Component parts, details or accessories; Auxiliary operations
- B29C48/78—Thermal treatment of the extrusion moulding material or of preformed parts or layers, e.g. by heating or cooling
- B29C48/875—Thermal treatment of the extrusion moulding material or of preformed parts or layers, e.g. by heating or cooling for achieving a non-uniform temperature distribution, e.g. using barrels having both cooling and heating zones
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C48/00—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor
- B29C48/25—Component parts, details or accessories; Auxiliary operations
- B29C48/92—Measuring, controlling or regulating
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/18—Oxygen-containing compounds, e.g. metal carbonyls
- C08K3/20—Oxides; Hydroxides
- C08K3/22—Oxides; Hydroxides of metals
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/34—Silicon-containing compounds
- C08K3/36—Silica
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C2948/00—Indexing scheme relating to extrusion moulding
- B29C2948/92—Measuring, controlling or regulating
- B29C2948/92504—Controlled parameter
- B29C2948/92514—Pressure
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C2948/00—Indexing scheme relating to extrusion moulding
- B29C2948/92—Measuring, controlling or regulating
- B29C2948/92504—Controlled parameter
- B29C2948/92561—Time, e.g. start, termination, duration or interruption
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C2948/00—Indexing scheme relating to extrusion moulding
- B29C2948/92—Measuring, controlling or regulating
- B29C2948/92504—Controlled parameter
- B29C2948/92704—Temperature
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C2948/00—Indexing scheme relating to extrusion moulding
- B29C2948/92—Measuring, controlling or regulating
- B29C2948/92819—Location or phase of control
- B29C2948/92857—Extrusion unit
- B29C2948/92876—Feeding, melting, plasticising or pumping zones, e.g. the melt itself
- B29C2948/92895—Barrel or housing
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/18—Oxygen-containing compounds, e.g. metal carbonyls
- C08K3/20—Oxides; Hydroxides
- C08K3/22—Oxides; Hydroxides of metals
- C08K2003/2227—Oxides; Hydroxides of metals of aluminium
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K2201/00—Specific properties of additives
- C08K2201/002—Physical properties
- C08K2201/003—Additives being defined by their diameter
Abstract
The invention relates to a fly ash-modified polypropylene composition and a preparation method thereof. The fly ash-modified polypropylene composition is prepared from the following raw materials by weight percent: 52-94% of polypropylene, 5-40% of fly ash, 0-3% of coupling agent, 0.1-2% of antioxidant, and 0-3% of other additives. The method comprises the steps of putting the raw materials into a high-speed mixer to carry out dry mixing for 3-5 minutes, and then putting the same into a twin-screw extruder; melt-extruding and granulating. The processes are as follows: the temperature of a first region is 200-210 DEG C, the temperature of a second region is 210-220 DEG C, the temperature of a third region is 210-220 DEG C, the temperature of a fourth region is 205-215 DEG C, the standing time is 1-2 minutes, and the pressure is 12-18MPa. The fly ash-modified polypropylene composition has the advantages that 1, the preparation method is simple in process, the cost is reduced by filling the modified polypropylene with the fly ash, and meanwhile, good overall performance of a composite material is kept; 2, the environmental pollution caused by the fly ash can be solved, the cost of the polypropylene material can be reduced, unification of the environmental benefits and the economic benefits is achieved, and a novel field is developed for comprehensive utilization of the fly ash.
Description
Technical field
The present invention relates to a kind of polypropene composition, be specifically related to a kind of flyash modified polypropene composition and preparation method thereof, polypropene composition of the present invention has the advantages such as technique is simple, cost is low, good combination property, can reduce the pollution of flyash to environment simultaneously.
Background technology
Polypropylene is important general-purpose plastics, and it not only has good physicals, chemical-resistant, and good processability, cheap, and these features make it be widely used in automobile, electrical equipment and field of furniture.But due to shortcomings such as polypropylene dimensional stability are poor, and thermotolerance and rigidity are lower, limited its application at engineering field.
Flyash is the flour of discharging from the flue of coal-fired power plant, is one of industrial waste of current quantity discharged maximum in the world.If it is not fully utilized, will inevitably cause serious pollution to the water surrounding in city, atmospheric environment etc.The rational exploitation and utilization of flyash is not only in order to meet the needs to the energy and resource, is also the needs that solve environmental pollution.How to become this objectionable impurities of flyash into being conducive to environment, be conducive to the useful thing of people's lives, become an important research topic in industry and field of Environment Protection.
The eighties in 20th century, China just started utilization of fly ash to carry out systematic study, and had in succession produced a large amount of Appropriate technologies.The comprehensive utilization of flyash mainly concentrates on it as material of construction, but along with deepening continuously of scientific research, to deepening constantly of flyash essence understanding, in the high-level development research of flyash, obtained certain progress, the range of application of flyash constantly expands.The main component of flyash is SiO
2and Al
2o
3, also have a small amount of CaO, MgO, K
2o, Na
2o, Fe
2o
3deng.In recent years, in view of the thin light weight of fine coal soot particle, the advantage such as mechanical property is high, active group is more, electrical property is good, make it be used as plastic filler for new field has been opened up in the comprehensive utilization of flyash.
The patent of flyash modified polypropylene aspect is less, and the Chinese patent of publication number CN1090236A has been announced the evaluation and exploration technology of a kind of flyash and polypropylene waste material.But owing to being the modified composite material of using waste woven bag and flyash, the poor-performings such as its stability, smell have been subject to a lot of restrictions in industrial circle.
Summary of the invention
The object of the invention is to develop the polypropene composition that a kind of technique is simple, cost is low, said composition has good over-all properties, and the present invention simultaneously can reduce the pollution of flyash to environment, benefits the nation and the people.
Another object of the present invention is to provide the preparation method of this polypropene composition.
The object of the invention is to be achieved through the following technical solutions:
A kind of flyash modified polypropene composition, is comprised of the raw material of following weight percent meter:
In above-mentioned flyash modified polypropene composition,
Described polypropylene is homo-polypropylene or block copolymerization propylene; Under 230 ℃, 2.16kg loading condiction, melt flow rate (MFR) is 2～60g/10min.
Wherein, the degree of crystallinity of homo-polypropylene is 70～100%, and degree of isotacticity is 99～100%; The comonomer of block copolymerization propylene is ethene, and vinyl monomer repeating unit molar content is 4～10%.
Described flyash is that relative density is 2.1～2.3g/cm
3, median size is the canescence meal of 1～10 micron, its main component is SiO
2and Al
2o
3, both total amounts are more than 85%.
Described coupling agent is the one in silane coupling agent, titanate coupling agent and aluminate coupling agent.
Described oxidation inhibitor comprises primary antioxidant and auxiliary anti-oxidant (auxiliary antioxidant).Wherein, described primary antioxidant is one or more mixing in hindered phenol and sulphur ester antioxidant; Auxiliary anti-oxidant is one or more mixing in phosphite and ester kind antioxidant.
Described other auxiliary agent comprises shades of colour additive, various ester lubricant or fatty acid lubricant etc.
The preparation method of above-mentioned flyash modified polypropene composition, its step is as follows:
(1) by above-mentioned weight proportion, take raw material;
(2) raw material is placed in to super mixer and is dry mixed 3～5 minutes;
(3) step (2) gained mixture is placed in to dual-screw-stem machine, through melt extruding, granulation, its technique is: 200～210 ℃, a district, two 210～220 ℃, districts, three 210～220 ℃, districts, four 205～215 ℃, districts; The residence time is 1～2 minute, and pressure is 12～18Mpa.
The invention has the advantages that:
1, the present invention is by flyash filled modified polypropylene, and this preparation method's technique is simple, reduces costs, and keeps the over-all properties that matrix material is good simultaneously.
2, the present invention can solve the pollution of flyash to environment, can reduce again the cost of polypropylene material, makes it to reach the unification of environment and economic benefit, for new field has been opened up in the comprehensive utilization of flyash.
Embodiment
Below in conjunction with specific embodiment, further set forth technical characterstic of the present invention.
In flyash modified polypropene composition of the present invention, comprise that quality percentage composition is that 52～95% melt flow rate (MFR) (test condition: 230 ℃, 2.16kg load) is that (comonomer of block copolymerization propylene is that its content of ethene is in the scope of 4～10mol% for the homo-polypropylene of 2～60g/10min or block copolymerization propylene; The degree of crystallinity of homo-polypropylene is more than 70%, and degree of isotacticity is greater than 99%); Quality percentage composition is 5～40%, relative density 2.1～2.3g/cm3, and median size is the flyash of 1～10 micron; Quality percentage composition is a kind of coupling agent in 0～3% silane coupling agent, titanate coupling agent or aluminate coupling agent.Also comprise and comprising with the primary antioxidant of one or more compositions in hindered phenol or sulphur ester antioxidant and the oxidation inhibitor take the auxiliary anti-oxidant of one or more compositions in phosphorite kind antioxidant as component, the mass percentage content of this oxidation inhibitor in polypropene composition of the present invention is 0.1～2%.Can also comprise that quality percentage composition is that other auxiliary agent of 0～3% comprises shades of colour additive, various ester class or fatty acid lubricant etc.
Before use, by said components and weight proportion, take raw material, in super mixer, be dry mixed 3～5 minutes; The raw material of mixing is placed in to dual-screw-stem machine, and through melt extruding, granulation, its technique is: 200～210 ℃, a district, two 210～220 ℃, districts, three 210～220 ℃, districts, four 205～215 ℃, districts; The residence time is 1～2 minute, and pressure is 12～18Mpa.
Mode below by embodiment further illustrates the present invention, does not therefore limit the present invention among described scope of embodiments.
Embodiment 1
Polypropene composition main ingredient of the present invention comprises 91.7% polypropylene, 5% flyash, 1% coupling agent, 0.1% antioxidant 3114 and 0.2% irgasfos 168 and 2% other auxiliary agent.
Embodiment 2
Polypropene composition main ingredient of the present invention comprises 86.7% polypropylene, 10% flyash, 1% coupling agent, 0.1% antioxidant 3114 and 0.2% irgasfos 168 and 2% other auxiliary agent.
Embodiment 3
Polypropene composition main ingredient of the present invention comprises 76.7% polypropylene, 20% flyash, 1% coupling agent, 0.1% antioxidant 3114 and 0.2% irgasfos 168 and 2% other auxiliary agent.
Embodiment 4
Polypropene composition main ingredient of the present invention comprises 66.7% polypropylene, 30% flyash, 1% coupling agent, 0.1% antioxidant 3114 and 0.2% irgasfos 168 and 2% other auxiliary agent.
Embodiment 5
Polypropene composition main ingredient of the present invention comprises 56.7% polypropylene, 40% flyash, 1% coupling agent, 0.1% antioxidant 3114 and 0.2% irgasfos 168 and 2% other auxiliary agent.
Above-described embodiment main component quality percentage composition is in Table 1.
Table 1 embodiment 1～5 main ingredient content (quality percentage composition)
| Embodiment numbering | 1 | 2 | 3 | 4 | 5 |
| Polypropylene | 91.7 | 86.7 | 76.7 | 66.7 | 56.7 |
| Flyash | 5 | 10 | 20 | 30 | 40 |
| Coupling agent | 1 | 1 | 1 | 1 | 1 |
| Antioxidant 3114 | 0.1 | 0.1 | 0.1 | 0.1 | 0.1 |
| Irgasfos 168 | 0.2 | 0.2 | 0.2 | 0.2 | 0.2 |
| Other auxiliary agent | 2 | 2 | 2 | 2 | 2 |
In the composite formula of above-described embodiment, polypropylene is homo-polypropylene, and melt flow rate (MFR) is 10g/10min.Described flyash, relative density is 2.2g/cm
3, median size is 2.5 microns.Described coupling agent is the silane coupling agent that U.S. Dow Corning company produces, and trade names are Z-6011.Described primary antioxidant 3114 is BASF AG's production, and trade names are Irganox3114, and chemical name is 3,5-di-tert-butyl-4-hydroxyl benzyl diethyl phosphoric acid; Auxiliary anti-oxidant 168 is BASF AG's production, and trade names are Irgafos168, and chemical name is three (2,4-di-tert-butyl-phenyl) phosphorous acid ester.
In above-described embodiment and comparative example, each resin and various additive are dry mixed 3～5 minutes in super mixer, then in twin screw extruder through melt extruding, granulation, its technique is: 190～200 ℃, a district, two 200～210 ℃, districts, three 210～220 ℃, districts, four 205～215 ℃, districts; The residence time is 1～2 minute, and pressure is 12～18Mpa.
The particulate material that completes as stated above granulation is dried to 2～3 hours in the convection oven of 90～100 ℃, and then dried particulate material is carried out on injection moulding machine to injection molding sample preparation, carry out performance test.
Tensile property test is undertaken by ISO527-2, and specimen size is 170 × 10 × 4mm, and draw speed is 50mm/min; Bending property test is undertaken by ISO178, and specimen size is 80 × 10 × 4mm, and rate of bending is 2mm/min; Shock strength is undertaken by ISO179/1eA, and specimen size is 80 × 10 × 4mm, and probe temperature is 23 ℃; Heat-drawn wire test is undertaken by ISO75-2, and specimen size is 80 × 10 × 4mm, and test load is 0.45MPa; Shore hardness test is undertaken by ISO868, and specimen size is ￠ 50 × 4mm, test duration 15s.
The over-all properties of material is passed judgment on by tensile strength, modulus in flexure, shock strength, heat-drawn wire and the shore hardness D of test gained.The performance test results of the embodiment of the present invention 1～5 is in Table 2.
Table 2 embodiment 1～5 polypropene composition the performance test results
From the test result of embodiment 1～5, can find out, along with the increase of flyash filling content, the performances such as the tensile strength of polypropene composition, modulus in flexure, shock strength, heat-drawn wire all present the trend of first increases and then decreases, when the filling content of flyash is 20%, the over-all properties of polypropene composition is best.
Above specific embodiments of the invention be have been described in detail, but it is just as example, the present invention is not restricted to specific embodiment described above.To those skilled in the art, any equivalent modifications that the present invention is carried out and alternative also all among category of the present invention.Therefore, equalization conversion and the modification done without departing from the spirit and scope of the invention, all should contain within the scope of the invention.
Claims (8)
1. a flyash modified polypropene composition, is characterized in that: the raw material by following weight percent meter forms:
2. the flyash modified polypropene composition of one according to claim 1, is characterized in that: described polypropylene is homo-polypropylene or block copolymerization propylene; Under 230 ℃, 2.16kg loading condiction, melt flow rate (MFR) is 2～60g/10min.
3. the flyash modified polypropene composition of one according to claim 2, is characterized in that: during for homo-polypropylene, its degree of crystallinity is 70～100%, and degree of isotacticity is 99～100%; During for block copolymerization propylene, its comonomer is ethene, and vinyl monomer repeating unit molar content is 4～10%.
4. the flyash modified polypropene composition of one according to claim 1, is characterized in that: described flyash is that relative density is 2.1～2.3g/cm
3, median size is the canescence meal of 1～10 micron, its main component is SiO
2and Al
2o
3, both total amounts are more than 85%.
5. the flyash modified polypropene composition of one according to claim 1, is characterized in that: described coupling agent is the one in silane coupling agent, titanate coupling agent and aluminate coupling agent.
6. the flyash modified polypropene composition of one according to claim 1, is characterized in that: described oxidation inhibitor comprises primary antioxidant and auxiliary anti-oxidant; Wherein, primary antioxidant is one or more mixing in hindered phenol and sulphur ester antioxidant; Auxiliary anti-oxidant is one or more mixing in phosphite and ester kind antioxidant.
7. the flyash modified polypropene composition of one according to claim 1, is characterized in that: described other auxiliary agent comprises shades of colour additive, various ester lubricant and fatty acid lubricant.
8. the preparation method of flyash modified polypropene composition described in claim 1, is characterized in that: its step is as follows:
(1) by above-mentioned weight proportion, take each component;
(2) raw material is placed in to super mixer and is dry mixed 3～5 minutes;
(3) step (2) gained mixture is placed in to dual-screw-stem machine, through melt extruding, granulation, its technique is: 200～210 ℃, a district, two 210～220 ℃, districts, three 210～220 ℃, districts, four 205～215 ℃, districts; The residence time is 1～2 minute, and pressure is 12～18Mpa.
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Cited By (4)
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| CN104371313A (en) * | 2014-12-05 | 2015-02-25 | 中国纺织科学研究院 | Composition of polymer composite prepared through the use of dust and method therefor |
| CN104592627A (en) * | 2014-12-22 | 2015-05-06 | 上海普利特复合材料股份有限公司 | High-toughness high-shrinkage environmental-friendly modified polypropylene composition and preparation method thereof |
| CN106750889A (en) * | 2016-11-09 | 2017-05-31 | 中国神华能源股份有限公司 | A kind of residue of aluminum-extracted pulverized fuel ash/PP composite material and preparation method thereof |
| CN111205556A (en) * | 2020-02-26 | 2020-05-29 | 上海应用技术大学 | Polypropylene composite material and preparation method thereof |
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