CN107540951A - A kind of preparation method of the transparent polypropylene composition with low-temperature impact property - Google Patents
A kind of preparation method of the transparent polypropylene composition with low-temperature impact property Download PDFInfo
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Abstract
The invention discloses a kind of preparation method of the transparent polypropylene composition with low-temperature impact property, belongs to new material technology field, and its preparation method is the polypropene composition each component that will be pre-dried, and is well mixed in super mixer；Said mixture is added into double screw extruder in 160 DEG C~250 DEG C melting extrusions；Extrusion material strip passes through hauling machine quick traction, and the draw ratio measured by the ratio between mouth mold/monofilament cross-sectional area is 2~40, and the type of cooling is water cooling；By extrudate, heat is dried in baking oven.The polypropene composition has higher rigidity and low-temperature flexibility, while is also equipped with the good transparency.
Description
Technical field
The invention belongs to new material technology field, and in particular to a kind of transparent low temperature impact prolylene polymer composition and its
Preparation method.
Background technology
Transparent PP it is excellent the transparency and surface gloss can with typical transparent material, such as makrolon, polyester
(PET), polystyrene etc. compares favourably, thus can be widely applied to household supplies and packaging field.The heat resistance ratio of transparent PP
General PP is high, utensil that is high and using or sterilize at high temperature is required especially suitable for the transparency, such as injector for medical purpose, micro-wave oven
Cooker, baby bottles, disposable fast food apparatus etc..With the fast development of China PP industry, transparent PP turns into be increased in PP products
One of most fast kind of speed.
Improving the PP transparencys typically has three kinds of approach：(1) nucleator is added, i.e., is carried by adding different types of nucleator
Crystalline rate, crystallization temperature, refinement spherocrystal or the change crystal formation of high polymer, and then improve transparency, the lustrous surface of product
Degree, rigidity, heat distortion temperature, impact strength and shortening molding cycle；(2) it is polymerization process production random copolymerization product [4-7],
I.e. by using the Natta of forth generation Ziegler one (Z/N) catalyst or metallocene catalyst, directly produced on device binary or
Ternary atactic copolymer, improve PP crystal property；(3) it is that blending is anti-reflection, i.e., is blended in process by several raw materials,
Change PP crystallization behavior, reduce spherulite size.Since the 1990s, with changing for PP catalyst and polymerization technique technology
Enter, developed a variety of transparent PPs with high added value, they are widely applied by rigidity/toughness/transparent sexual balance
Key areas is waited with medical in packaging, has widened PP application significantly.
Chinese patent application 200780030588.3 discloses a kind of polypropene composition and its product, by the way that fusing point is low
It is blended to obtain in 160 DEG C, propylene copolymer of the bending modulus less than 1000MPa and ethylene-propylene rubber, said composition has machine
The optimum balance of tool performance and transparency.But the rigidity of the material is poor.
Chinese patent application 200610051053.1 discloses one kind with Nano silica sol and organic phosphoric acid salt form polypropylene
The method that nucleator compounding prepares transparent polypropylene.It is high using transparent polypropylene bending modulus made from this method, but material
The transparency is relatively low, and mist degree is higher, and impact strength is low.
Chinese patent application 02104405.8 discloses a kind of preparation method of transparent polypropylene, by adding in polypropylene
Add clarifier and dyes of anthraquinone, the clear acrylic with good appearance form and aspect is obtained after melting extrusion, can be effective
Solves transparent polypropylene product yellowing phenomenon.But it is still a kind of conventional anti-reflection method.
Chinese Patent Application No. 200710202436.9 discloses a kind of preparation method of nontoxic colored transparent polypropylene, its
Using nontoxic coloured silicasol as transparent nucleater and colouring agent, it is added to melt pelletization in polypropylene and obtains.But due into
Core antireflective effect is limited, and the combination property of material is still undesirable.
Chinese Patent Application No. 200710084361.9 discloses a kind of transparent polypropylene sheet with radiation resistant
Molding composition, it is by 100 parts by weight of polypropylene homopolymers, the propylene-ethylene random copolymerization that ethylene contents are 5% or less
Thing or their resin compound, the phosphorus antioxidants of 0.01~0.125 parts by weight, the hindered amine of 0.01~0.1 parts by weight
The calcium stearate of class compound and 0.01~0.1 parts by weight forms.Composition is similar to conventional addition nucleating agent compositions, only increases
Anti- x ray irradiation x antioxidant system has been added to be formed.
According to the current main stream approach for improving polypropylene transparent, for existing HOPP, random copolymerization poly- third
Alkene and impact polypropylene are modified.In three kinds of materials, HOPP is rigidly optimal, the transparency between it is other therebetween,
But toughness is minimum；The atactic copolymerized polypropene transparency is optimal, toughness between it is other therebetween, but rigidity is minimum；Anti-impact poly- third
Alkene toughness is optimal, rigidity between it is other therebetween, but the transparency it is worst.There is presently no one kind to have good low temperature shock resistance
The clear acrylic of performance.Therefore, current present situation is, it is still desirable to provides a kind of clear acrylic, it is having
While having good transparency, the rigidity and toughness that also balance, particularly low-temperature flexibility, led for low temperature packaging material etc.
Domain.
The content of the invention
In order to solve the above problems, the present invention provides a kind of transparent polypropylene combination with good low temperature shock resistance
Thing, the polypropene composition has higher rigidity and low-temperature flexibility, while is also equipped with the good transparency.
A kind of preparation method of the transparent polypropylene composition with low-temperature impact property, including following basic step：
(1) the polypropene composition each component that will be pre-dried, it is well mixed in super mixer；
(2) said mixture is added into double screw extruder in 160 DEG C~250 DEG C melting extrusions；
(3) extrusion material strip passes through hauling machine quick traction, and the draw ratio measured by the ratio between mouth mold/monofilament cross-sectional area is 2
~40, the type of cooling is water cooling；
(4) by extrudate, heat is dried 30 minutes in baking oven.
Described transparent polypropylene composition by weight for example under：
Described prolylene polymer composition, described acrylic polymers are the ecosystem polypropylene for being not added with any auxiliary agent
Powder, it may be selected from HOPP or atactic copolymerized polypropene that melt flow rate (MFR) is 0.1~10g/10min.
Described randomly acrylic polymers altogether, comonomer be ethene, 1- butylene, 1- hexenes and one kind in 1- octenes or
A variety of, the content of comonomer is no more than 12wt%.
Described thermoplastic elastomer (TPE) may be selected from EP rubbers, ethylene propylene diene rubber, SBS, SEBS and POE (ethylene-octene
Copolymer) etc..
Described primary antioxidant may be selected from β-positive octadecanol ester of (4- hydroxyls -3,5- di-tert-butyl-phenyl) propionic acid, four [β -
(3,5- di-tert-butyl-hydroxy phenyl) propionic acid] pentaerythritol ester.
Described auxiliary anti-oxidant may be selected from (2,4- di-tert-butyl-phenyl) tris phosphite, pentaerythritol bis-phosphite two
(2,4- di-tert-butyl phenyl) ester.
Described halogen-absorber may be selected from the one or more of calcium stearate, zinc stearate and hydrated magnesium silicate, preferably
Calcium stearate.
Described crosslinking agent, which can be selected from organic peroxide, can enumerate hydroperoxides, dialkyl peroxide, two
Acyl peroxide.
Specifically, hydroperoxides can be selected from tert-butyl peroxide, cumyl peroxide, diisopropyl peroxidating
Hydrogen, the hydroperoxy hexane of 2,5- dimethyl -2,5- bis-, the hydroperoxy -3- hexins of 2,5- dimethyl -2,5- bis- and firpene base peroxide
Change hydrogen etc..
Dialkyl peroxide, di-tert-butyl peroxide, two t-amyl peroxy compounds, butyl-cumyl mistake can be selected from
Oxide, peroxide diisopropylbenzene (DIPB), 2,5- dimethyl -2,5- bis- (tert-butyl peroxy base) hexane, 2,5- dimethyl -2,5- bis-
Double (the tert-butyl peroxy bases) -3 of (tert-butyl peroxy base) hexin, 1,1-, double (the tert-butyl peroxy bases)-penta of 3,5- trimethyl-cyclohexanes, 4,4-
Double (4, the 4- bis- tert-butyl peroxy butylcyclohexyl) propane of sour N-butyl, 2,2-, 2,2- double (tert-butyl peroxy base) butane, (uncles of 1,1- bis-
Butyl peroxy base) hexamethylene and α, α '-bis- (tert-butyl peroxy bases) diisopropylbenzene (DIPB) etc..
Diacyl peroxide, caprylyl peroxide, lauroyl peroxide, stearoyl, peroxidating amber can be selected from
Amber acid, benzoyl peroxide, chloro benzoyl peroxide and peroxidating 2,4- dichloro-benzoyls etc..
The organic peroxide can be used alone, and a variety of can also be used in mixed way.Wherein preferred dialkyl group peroxide
Compound, most preferably further preferred di-tert-butyl peroxide and cumyl peroxide, di-tert-butyl peroxide.
Described assistant crosslinking agent may be selected from triallyl cyanurate (TAC), iso-cyanuric acid triallyl ester
(TAIC), trimethylol-propane trimethacrylate (TMPTMA), the meta-phenylene bismaleimide of N, N mono- (PDM), trimerization
The one or more of thiocyanic acid (TCY).
Described nucleator may be selected from Sorbitol Nucleator agent (DBS classes), if dibenzal sorbitol (DBS), two are (to second
The benzal of base two) sorbierite, two (to the benzal of methyl two) sorbierites (MDBS) and two (benzal of 3,4- dimethyl two) sorbierites etc.；Carboxylic
Acid and its esters nucleator such as two rings [2,2,1] heptane dicarboxylate salts (HPN-68) and two rings [2,2,1] heptane -2,3- dicarboxylic acids
Sodium salt (HPN-68L)；Nucleator in organic phosphate class such as NA-10, NA-11, NA-21 etc..It is preferred that Sorbitol Nucleator.
Described primary antioxidant, auxiliary anti-oxidant, crosslinking agent, assistant crosslinking agent and nucleator etc. can be added in the form of pure substance
Enter, can also masterbatch or the addition of compound additive form.
Described twin-screw double screw extruder be draw ratio between 35~45, preferably draw ratio be 40 it is parallel double in the same direction
Screw extruder.
Beneficial effect
It is a discovery of the invention that using the manufacture method of transparent polypropylene composition provided by the present invention, using simply connecting
Continuous extrusion reaction method, passes through melt drawn so that rubber mutually exists in 1-dimention nano fibers form, in crosslinking agent and helps crosslinking
In the presence of agent, process is dried by hot-stretch and follow-up heat, the nanofibrous structures of rubber phase are solidified, when partial rubber is mutually fine
Size is tieed up less than after visible wavelength, it is seen that light can be directed through, so as to greatly improve the polyacrylic transparency, simultaneously
Pass through additional nucleator so that the HOPP component crystal particle diameter in impact polypropylene raw material greatly reduces, further
The transparency of composition is improved, while remains in that good shock resistance.
Compared with other melt-mixing methods, using transparent polypropylene composition preparation method provided by the present invention, make
With impact polypropylene raw material, resulting transparent polypropylene composition has good rigidity-toughness balance quality, preferably simultaneously
The transparency and low-temperature impact performance, it is even lower that mist degree can be reduced to 13% from 102%.And this method is prepared simply, is applicable
Manufactured in industrial-scale, be especially suitable for low temperature packaging material application.
Embodiment
With reference to specific embodiment, the present invention will be described in detail.Protection scope of the present invention is not with specific implementation
Mode is limited, but is defined in the claims.
Explanation is of the invention in further detail with reference to embodiments, but the invention is not restricted to these embodiments.
Melt flow rate (MFR) (MFR) measure reference standard GB/T 3682-2008 are carried out, and condition determination is 230 DEG C and 2.16
Kilogram load；Tensile property is tested by GB/T1040-2006, draw speed 50mm/min；Impact property presses GB/T
1843-2008 is tested；Bending property is tested by GB/T 9341-2008, and mist degree is tested according to GB/T2410-2008.
Embodiment 1
By 100 parts by weight (2000 grams) acrylic polymers powder (Propylene-ethylene random copolymer, ethylene copolymer amount
12wt%) it is added in super mixer, and by the POE of 10 parts by weight, 0.05 parts by weight (1.0 grams) primary antioxidant β-(4- hydroxyls
Base -3,5- di-tert-butyl-phenyl) the positive octadecanol ester of propionic acid, (2,4- di-tert-butyl-phenyl) phosphorous of 0.1 parts by weight (2.0 grams)
Sour three esters, 0.05 parts by weight (1.0 grams) halogen-absorber calcium stearate, the cumyl peroxide of 0.1 parts by weight (2 grams), 1.0
The assistant crosslinking agent iso-cyanuric acid triallyl ester of parts by weight (20 grams) and the nucleator two of 0.05 parts by weight (1.0 grams) are (to first
The benzal of base two) after sorbierite is mutually mixed, it is added in moderate-speed mixers and is stirred, speed of agitator is 250 revs/min, is stirred
Incorporation time is mixed as 10 minutes.Discharged after the completion of mixing, the premix is added to the double spiral shells of Haake for having set temperature immediately
Melt mixed extruding pelletization is carried out in bar extruder.170~210 DEG C of double screw extruder design temperature, screw speed 40-
120rpm, port mould diameter 0.5mm.Extrusion material strip through water-bath cooling and draws winding, rolling speed 10m/min.Mouth mold/monofilament is horizontal
The draw ratio that the ratio between sectional area is measured is 38.
Polypropene composition can be shown in Table 1.
Embodiment 2
By 100 parts by weight (2000 grams) acrylic polymers powder (ethylene-propylene random copolymer, ethylene copolymer amount
8wt%) it is added in super mixer, and by the glue of second third of 8 parts by weight, 0.1 parts by weight (2 grams) primary antioxidant four [β-(3,5-
Di-tert-butyl-hydroxy phenyl) propionic acid] pentaerythritol ester, the pentaerythritol bis-phosphite two (2,4- of 0.2 parts by weight (4 grams)
Di-tert-butyl phenyl) ester, 0.1 parts by weight (2 grams) halogen-absorber (calcium stearate), the diisopropyl of 1.3 parts by weight (26 grams)
Hydrogen peroxide, the assistant crosslinking agent trimethylol propane trimethyl propylene of 1.5 parts by weight (30 grams) and 0.1 parts by weight (3 grams) into
After core agent two (to the benzal of ethyl two) sorbierite is mutually mixed, it is added in moderate-speed mixers and is stirred, speed of agitator 250
Rev/min, the time is stirred as 10 minutes.Discharged after the completion of mixing, the premix is added to has set temperature immediately
Haake double screw extruder in carry out melt mixed extruding pelletization.180~220 DEG C of double screw extruder design temperature, screw rod
Rotating speed 40-120rpm, port mould diameter 0.5mm.Extrusion material strip through water-bath cooling and draws winding, rolling speed 9m/min.Mouth mold/
The draw ratio that the ratio between monofilament cross-sectional area is measured is 30.
Polypropene composition can be shown in Table 1.
Embodiment 3
100 parts by weight (2000 grams) Propylene-ethylene random copolymer powder (ethylene copolymer amount 5wt%) is added at a high speed
In blender, and by 20 parts by weight (400 grams) ethylene-propylene diene copolymer, 0.1 parts by weight (2.0 grams) primary antioxidant β-(4- hydroxyls -3,5-
Di-tert-butyl-phenyl) the positive octadecanol ester of propionic acid, 0.2 parts by weight (4.0 grams) (2,4- di-tert-butyl-phenyl) tris phosphite,
0.1 parts by weight (2.0 grams) halogen-absorber (zinc stearate), di-tert-butyl peroxide, 0.05 weight of 2.5 parts by weight (50 grams)
Measure the assistant crosslinking agent acid esters triallyl cyanurate of part (1.0 grams) and the nucleator two (3,4- bis- of 0.5 parts by weight (10 grams)
The benzal of methyl two) after sorbierite is mutually mixed, it is added in moderate-speed mixers and is stirred, speed of agitator is 250 revs/min,
The time is stirred as 10 minutes.Discharged after the completion of mixing, the premix is added to the Haake pair for having set temperature immediately
Melt mixed extruding pelletization is carried out in screw extruder.180~230 DEG C of double screw extruder design temperature, screw speed 20-
120rpm, port mould diameter 0.5mm.Extrusion material strip through water-bath cooling and draws winding, rolling speed 4.5m/min.Mouth mold/monofilament
The draw ratio that the ratio between cross-sectional area is measured is 7.0.
Polypropene composition can be shown in Table 1.
Embodiment 4
100 parts by weight (2000 grams) homo-polypropylene powder is added in super mixer, and by 3 parts by weight (60 grams)
SEBS, 0.15 parts by weight (3 grams) primary antioxidant four [β-(3,5- di-tert-butyl-hydroxy phenyl) propionic acid] pentaerythritol ester,
Pentaerythritol bis-phosphite two (2,4- di-tert-butyl phenyl) ester, 0.08 parts by weight (1.6 grams) halogen of 0.3 parts by weight (6 grams)
Plain absorbent (calcium stearate), the benzoyl peroxide of 4.0 parts by weight (80 grams), the assistant crosslinking agent N, N of 3.0 parts by weight (60 grams)
After one meta-phenylene bismaleimide (PDM) and the nucleator dibenzal sorbitol of 0.3 parts by weight (15 grams) are mutually mixed, add
Enter and be stirred into moderate-speed mixers, speed of agitator is 250 revs/min, is stirred the time as 10 minutes.After the completion of mixing
Discharging, the premix is added to progress melt mixed extrusion in the Haake double screw extruder for set temperature immediately and made
Grain.180~250 DEG C, screw speed 20-120rpm, port mould diameter 0.5mm of double screw extruder design temperature.Extrude material strip warp
Water-bath cooling simultaneously draws winding, rolling speed 3m/min.The draw ratio that the ratio between mouth mold/monofilament cross-sectional area is measured is 2.
Polypropene composition can be shown in Table 1.
Comparative example
100 parts by weight (2000 grams) Propylene-ethylene random copolymer powder (ethylene contents 8wt%) is added to mixed at a high speed
In clutch, and by 10 parts by weight (200 grams) POE, 0.12 parts by weight (2.4 grams) primary antioxidant four [β-(3,5- di-t-butyl -4-
Hydroxy phenyl) propionic acid] pentaerythritol ester, (2,4- di-tert-butyl-phenyl) tris phosphite of 0.2 parts by weight (4.0 grams), 0.08
Parts by weight (1.6 grams) halogen-absorber (calcium stearate), the di-tert-butyl peroxide of 2.5 parts by weight (50 grams), 2.0 parts by weight
The assistant crosslinking agent iso-cyanuric acid triallyl ester of (40 grams) and the nucleator two of 0.2 parts by weight (4 grams) (to the benzal of methyl two)
After sorbierite is mutually mixed, it is added in moderate-speed mixers and is stirred, speed of agitator is 250 revs/min, is stirred the time
For 10 minutes.Discharge, be immediately added to the premix in the Haake double screw extruder for having set temperature after the completion of mixing
Carry out melt mixed extruding pelletization.180~250 DEG C, screw speed 20-120rpm of double screw extruder design temperature, mouth mold is straight
Footpath 0.5mm.Extrusion material strip obtains through water-bath cooling and pelletizing.
Polypropene composition can be shown in Table 1.
The Polypropylene compositions physical performance of table 1
From the result of table 1, compared with comparative example, the polypropene composition transparency prepared using the inventive method is had
Significantly lifted, and can guarantee that bending modulus is suitable, simply supported beam notch impact strength does not decline level substantially.Also, use
Atactic copolymerized polypropene matrix and raising stretching ratio, the mist degree of composition are on a declining curve.
Claims (10)
1. a kind of preparation method of the transparent polypropylene composition with low-temperature impact property, it is characterised in that including as follows
Step：
(1) the polypropene composition each component that will be pre-dried, it is well mixed in super mixer；
(2) said mixture is added into double screw extruder in 160 DEG C~250 DEG C melting extrusions；
(3) extrusion material strip passes through hauling machine quick traction, and the draw ratio measured by the ratio between mouth mold/monofilament cross-sectional area is 2~40,
The type of cooling is water cooling；
(4) by extrudate, heat is dried in baking oven；
Described polypropene composition by weight for example under：
It selected from melt flow rate (MFR) is 0.1~10g/10min that described HOPP or atactic copolymerized polypropene polymer, which are,.
2. preparation method according to claim 1, it is characterised in that described atactic copolymerized polypropene, wherein copolymerization is single
Body is the one or more in ethene, 1- butylene, and the content of comonomer is 0-12wt%.
3. preparation method according to claim 1, it is characterised in that described thermoplastic elastomer (TPE) be selected from EP rubbers,
The one of which of ethylene propylene diene rubber, SBS, SEBS or POE (ethylene-octene copolymer).
4. preparation method according to claim 1, it is characterised in that described primary antioxidant is selected from β-(4- hydroxyls -3,5-
Di-tert-butyl-phenyl) the positive octadecanol ester of propionic acid, four [β-(3,5- di-tert-butyl-hydroxy phenyl) propionic acid] pentaerythritol esters
One of which.
5. preparation method according to claim 1, it is characterised in that described auxiliary anti-oxidant is selected from (2,4- di-t-butyls
Phenyl) tris phosphite, the one of which of pentaerythritol bis-phosphite two (2,4- di-tert-butyl phenyl) ester.
6. preparation method according to claim 1, it is characterised in that described halogen-absorber is selected from calcium stearate, hard
The one or more of resin acid zinc and hydrated magnesium silicate.
7. preparation method according to claim 1, it is characterised in that described crosslinking agent is selected from hydroperoxides, dioxane
The one or more of base peroxide, diacyl peroxide；
Described hydroperoxides are selected from tert-butyl peroxide, cumyl peroxide, diisopropyl hydrogen peroxide, 2,5- diformazans
The hydroperoxy hexane of base -2,5- bis-, the hydroperoxy -3- hexins of 2,5- dimethyl -2,5- bis- or firpene base hydrogen peroxide；
Dialkyl peroxide is selected from di-tert-butyl peroxide, two t-amyl peroxy compounds, tert-butyl cumyl peroxide, mistake
Oxide diisopropylbenzene (DIPB), 2,5- dimethyl -2,5- bis- (tert-butyl peroxy base) hexane, (tert-butyl peroxy of 2,5- dimethyl -2,5- bis-
Base) hexin, double (the tert-butyl peroxy bases) -3 of 1,1-, double (tert-butyl peroxy the base)-n-butyl pentanoates of 3,5- trimethyl-cyclohexanes, 4,4-,
2,2- double (4,4- bis- tert-butyl peroxy butylcyclohexyl) propane, 2,2- double (tert-butyl peroxy base) butane, 1,1- bis- (tert-butyl peroxy base)
Hexamethylene or α, α '-bis- (tert-butyl peroxy bases) diisopropylbenzene (DIPB)；
Diacyl peroxide is selected from caprylyl peroxide, lauroyl peroxide, stearoyl, succinic acid peroxide, peroxide
Change benzoyl, chloro benzoyl peroxide or peroxidating 2,4- dichloro-benzoyls.
8. preparation method according to claim 1, it is characterised in that described assistant crosslinking agent is selected from triallyl melamine
Acid esters (TAC), iso-cyanuric acid triallyl ester (TAIC), trimethylol-propane trimethacrylate (TMPTMA), N, N-
The one or more of meta-phenylene bismaleimide (PDM), trithiocyanuric acid (TCY).
9. preparation method according to claim 1, it is characterised in that described nucleator is selected from dibenzal sorbitol
(DBS), two (to the benzal of ethyl two) sorbierites, two (to the benzal of methyl two) sorbierites (MDBS), two (3,4- dimethyl dibenzyls
Fork) sorbierite, two rings [2,2,1] heptane dicarboxylate salts (HPN-68), two rings [2,2,1] heptane -2,3- dicarboxylic acids sodium salt (HPN-
68L), NA-10, NA-11, NA-21 one or more.
10. according to the preparation method described in claim 1 to 9 any one, it is characterised in that described double screw extruder is
Draw ratio is between 35~45.
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| CN114907643A (en) * | 2021-02-08 | 2022-08-16 | 中国石油化工股份有限公司 | Polypropylene composition, polypropylene material, preparation method and application thereof |
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| CN109851913B (en) * | 2018-12-18 | 2021-09-10 | 东华能源(宁波)新材料有限公司 | Toughened polypropylene material and preparation method thereof |
| CN114907643A (en) * | 2021-02-08 | 2022-08-16 | 中国石油化工股份有限公司 | Polypropylene composition, polypropylene material, preparation method and application thereof |
| CN114181452A (en) * | 2021-10-29 | 2022-03-15 | 金发科技股份有限公司 | Polypropylene composition and preparation method and application thereof |
| CN114181452B (en) * | 2021-10-29 | 2023-10-31 | 金发科技股份有限公司 | Polypropylene composition and preparation method and application thereof |
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Application publication date: 20180105 |