CN115093647A - EPDM flame-retardant foaming sealing strip for energy product line cabinet - Google Patents
EPDM flame-retardant foaming sealing strip for energy product line cabinet Download PDFInfo
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- C08J9/00—Working-up of macromolecular substances to porous or cellular articles or materials; After-treatment thereof
- C08J9/04—Working-up of macromolecular substances to porous or cellular articles or materials; After-treatment thereof using blowing gases generated by a previously added blowing agent
- C08J9/06—Working-up of macromolecular substances to porous or cellular articles or materials; After-treatment thereof using blowing gases generated by a previously added blowing agent by a chemical blowing agent
- C08J9/10—Working-up of macromolecular substances to porous or cellular articles or materials; After-treatment thereof using blowing gases generated by a previously added blowing agent by a chemical blowing agent developing nitrogen, the blowing agent being a compound containing a nitrogen-to-nitrogen bond
- C08J9/102—Azo-compounds
- C08J9/103—Azodicarbonamide
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- C08J9/00—Working-up of macromolecular substances to porous or cellular articles or materials; After-treatment thereof
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- C08J9/00—Working-up of macromolecular substances to porous or cellular articles or materials; After-treatment thereof
- C08J9/0014—Use of organic additives
- C08J9/0023—Use of organic additives containing oxygen
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- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J9/00—Working-up of macromolecular substances to porous or cellular articles or materials; After-treatment thereof
- C08J9/0061—Working-up of macromolecular substances to porous or cellular articles or materials; After-treatment thereof characterized by the use of several polymeric components
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- C08J9/0066—Use of inorganic compounding ingredients
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- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J2203/00—Foams characterized by the expanding agent
- C08J2203/04—N2 releasing, ex azodicarbonamide or nitroso compound
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- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J2323/00—Characterised by the use of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Derivatives of such polymers
- C08J2323/02—Characterised by the use of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Derivatives of such polymers not modified by chemical after treatment
- C08J2323/16—Ethene-propene or ethene-propene-diene copolymers
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- C08J2471/00—Characterised by the use of polyethers obtained by reactions forming an ether link in the main chain; Derivatives of such polymers
- C08J2471/02—Polyalkylene oxides
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- C08J2491/00—Characterised by the use of oils, fats or waxes; Derivatives thereof
- C08J2491/06—Waxes
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Abstract
The invention discloses an EPDM flame-retardant foaming sealing strip for an energy product line cabinet, which comprises the following raw materials in parts by weight: 100-120 parts of ethylene propylene diene monomer; quickly extruding out 20-40 parts of carbon black N550; 130 portions of flame retardant agent and 150 portions of flame retardant agent; 20-40 parts of paraffin oil; 5-7 parts of active zinc oxide; 1-3 parts of stearic acid; 1-3 parts of a flow aid; 1-3 parts of polyethylene glycol; 1-3 parts of a vulcanizing agent; 8-10 parts of an accelerator; 9-11 parts of a foaming agent; 1-3 parts of a foaming auxiliary agent. By adopting the formula of the EPDM flame-retardant foaming sealing strip for the cabinet of the energy product line, better material physical properties, lower density and higher flame-retardant grade can be obtained, and the EPDM flame-retardant foaming sealing strip can meet the requirement of self-extinguishing in a short time after being away from fire, thereby meeting the flame-retardant requirement of a sealing system of the cabinet of the energy product line and having high safety.
Description
Technical Field
The invention relates to the field of sealing strip materials, in particular to an EPDM flame-retardant foaming sealing strip for an energy product line cabinet.
Background
The EPDM flame-retardant foaming sealing strip for the energy product line cabinet is mainly used for a sealing system of the energy product line cabinet, the base material of the sealing strip is EPDM synthetic rubber with high ENB content, and the processing technology of the sealing strip is a microwave vulcanization extrusion technology. EPDM belongs to nonpolar slightly unsaturated rubber, has excellent ozone resistance, thermal aging resistance, water resistance and corrosion resistance, and is high-elasticity rubber with excellent electrical insulating property. But applied to the field of cabinets of energy product lines, in addition to excellent aging resistance and excellent electrical insulation, high flame retardancy is required to prevent fires. EPDM does not have the fire resistance, one or more fire retardants are required to be filled to enable the EPDM to have the fire resistance, and the existing energy product line cabinet sealing system has an increasing demand on the flame-retardant foamed EPDM sealing strip, so that the research on the EPDM flame-retardant foamed sealing strip is a demand in the field of energy product line cabinet sealing.
Disclosure of Invention
The invention aims to overcome the defects of the prior art and provide the EPDM flame-retardant foaming sealing strip for the energy product line cabinet, which has the advantages of novel and reliable technology, high flame retardance, good tensile property and high vulcanization efficiency.
In order to achieve the above purpose, the technical scheme adopted by the invention is as follows: an EPDM flame-retardant foaming sealing strip for an energy product line cabinet comprises the following raw materials in parts by weight: 100-120 parts of ethylene propylene diene monomer; quickly extruding 20-40 parts of carbon black N550; 130 portions of flame retardant agent and 150 portions of flame retardant agent; 20-40 parts of paraffin oil; 5-7 parts of active zinc oxide; 1-3 parts of stearic acid; 1-3 parts of a flow aid; 1-3 parts of polyethylene glycol; 1-3 parts of a vulcanizing agent; 8-10 parts of an accelerator; 9-11 parts of a foaming agent; 1-3 parts of a foaming auxiliary agent.
Preferably, the flame retardant comprises the following raw materials in parts by weight: 40-60 parts of decabromodiphenylethane, 20-40 parts of magnesium hydroxide, 20-40 parts of zinc borate and 20-40 parts of antimony trioxide.
Preferably, the ethylene-propylene-diene monomer has an Ethylidene Norbornene (ENB) content of 8.9%, a Mooney viscosity ML (1+4) at 125 ℃ of 82, and an ethylene content of 57.5%.
Preferably, the production process comprises the steps of:
s1, firstly, adding ethylene propylene diene monomer, active zinc oxide, stearic acid, a flow aid and polyethylene glycol into an internal mixer for pressure plastication for 40-60 s;
s2, adding the quick-extrusion carbon black, the flame retardant and the paraffin oil, pressurizing to a cleaning temperature, opening a material door, cleaning an upper top plug and the residual materials around a hopper opening to an internal mixing chamber;
s3, pressurizing and mixing to exhaust temperature, and half opening the upper top plug to exhaust once; continuously pressurizing and banburying to the glue discharging temperature and then discharging glue;
s4, transferring the rubber material discharged by the internal mixer into an open mill for roll wrapping, rubber cutting and disc falling, then wrapping the roll again for rubber turning for 140-160s to obtain the rubber material;
s5, adding the hinge material, the vulcanizing agent, the accelerator, the foaming agent and the foaming auxiliary agent into an internal mixer for pressurization mixing for 120 s;
s6, transferring the rubber material discharged by the internal mixer into an open mill for roll wrapping, rubber cutting and disc falling, then wrapping the roll again for rubber turning for 170-190 seconds to obtain the rubber material;
s7, rolling and discharging the rubber material to obtain the finished product, wherein the sheet discharging width is 140-150mm, and cooling by air cooling.
Preferably, the cleaning temperature is 105-115 ℃, the exhaust temperature is 125-135 ℃, and the gel discharge temperature is 145-155 ℃.
Preferably, in the step S1, the temperature in the internal mixer is less than 115 ℃ when the charging temperature is higher.
The invention has the beneficial effects that: the EPDM flame-retardant foaming sealing strip for the energy product line cabinet has the advantages of good flame retardance, good stretchability and the like. And the invention adopts a high-promotion low-sulfur vulcanization system, which can ensure rapid vulcanization and compensate the adverse factor of vulcanization speed reduction caused by adding a flame retardant in the formula, so that the vulcanization speed of the invention can be ensured on the premise of flame resistance, which is beneficial to improving efficiency and is suitable for microwave vulcanization extrusion process. In addition, the invention adopts the foaming agent, is characterized by large gas evolution, and can greatly reduce the density of the sealing strip by decomposing a large amount of gas through the microwave high-temperature hot air vulcanizing tank. By adopting the formula of the EPDM flame-retardant foaming sealing strip for the cabinet of the energy product line, better material physical properties, lower density and higher flame-retardant grade can be obtained, and the EPDM flame-retardant foaming sealing strip can meet the requirement of self-extinguishing in a short time after being away from fire, thereby meeting the flame-retardant requirement of a sealing system of the cabinet of the energy product line and having high safety.
Detailed Description
The claimed invention will now be described in further detail with reference to the following examples.
Example one
The EPDM flame-retardant foaming sealing strip for the energy product line cabinet in the embodiment comprises the following raw materials in parts by weight:
100 parts of ethylene propylene diene monomer, KEP-2480 and Jinhu chemical;
quickly extruding carbon black N55020 parts, N550 parts, and Boo, Qingzhou;
20 parts of paraffin oil, LD-300, Guangzhou Ligen;
5 parts of active zinc oxide, T-40, Shuiyilongxin zinc;
1 part of stearic acid, SA1801, Forster;
1 part of flow additive, RL-20 and Forster;
1 part of polyethylene glycol, PEG-4000 and Jinnuo chemical industry;
1 part of vulcanizing agent, IS-60, and the balance;
8 parts of accelerator, M/BZ/EZ/TRA/TDEC-75, product and;
9 parts of foaming agent, AC-75 parts and Achrom;
1 part of foaming auxiliary agent, K5, and permanently mixing chemical engineering;
60 parts of decabromodiphenylethane, RDT-3, chemical engineering of Shouguang Weidong;
20 parts of magnesium hydroxide, FM-20 parts of Artemex;
20 parts of zinc borate, 777 parts of gold and Yingtai chemical industry;
30 parts of antimony trioxide, Jinshan brand and Yingcheng mineral chemical industry;
the ethylene-propylene-diene monomer rubber has the ethylidene norbornene content of 8.9 percent, the Mooney viscosity ML (1+4) at 125 ℃ of 82 percent and the ethylene content of 57.5 percent.
The production process in this example comprises the following steps:
s1, firstly, adding ethylene propylene diene monomer, activated zinc oxide, stearic acid, a flow assistant and polyethylene glycol into a 75L internal mixer for pressure plastication, wherein the temperature in the internal mixer is less than 115 ℃ at the feeding temperature, and the plastication time is 40-60 s.
S2, adding the fast extrusion carbon black, decabromodiphenylethane, magnesium hydroxide, zinc borate, antimony trioxide and paraffin oil, pressurizing to a cleaning temperature of 105-.
S3, pressurizing and mixing until the exhaust temperature is 125-; continuously pressurizing and banburying until the rubber discharge temperature is reached, and then discharging the rubber at 145-155 ℃.
And S4, transferring the rubber material discharged from the internal mixer into an open mill for roll wrapping, rubber cutting and disc falling, and then wrapping the roll again for rubber turning for 140-160 seconds to obtain the rubber material.
S5, adding the hinge material, the vulcanizing agent, the accelerator, the foaming agent and the foaming auxiliary agent into an internal mixer for pressurization mixing for 120 s.
S6, transferring the rubber material discharged from the internal mixer into an open mill for roll wrapping, rubber cutting and disc falling, then wrapping the roll again for rubber turning for 170-190 seconds, and obtaining the rubber material.
S7, rolling and discharging the rubber material to obtain the finished product, wherein the sheet discharging width is 140-150mm, and cooling by air cooling.
Example two
120 parts of ethylene propylene diene monomer, KEP-2480 and Jinhu chemistry;
quickly extruding carbon black N55040 parts, N550 parts, and Boo, Qingzhou;
40 parts of paraffin oil, LD-300, Guangzhou Liben;
7 parts of active zinc oxide, T-40, Shuiylongxin zinc industry;
3 parts of stearic acid, SA1801, Forster;
3 parts of a flow aid, RL-20 and Forster;
3 parts of polyethylene glycol, PEG-4000, Jinnuo chemical industry;
3 parts of vulcanizing agent, IS-60, and the balance;
10 parts of accelerator, M/BZ/EZ/TRA/TDEC-75, and the balance;
11 parts of foaming agent, AC-75 parts and Achrom;
3 parts of foaming auxiliary agent, K5, and permanently mixing chemical engineering;
40 parts of decabromodiphenylethane, RDT-3, chemical engineering of Shouguangdongdong;
40 parts of magnesium hydroxide, FM-20 parts of Artemex;
40 parts of zinc borate, 777 parts of gold and Tai chemical engineering;
20 parts of antimony trioxide, Jinshan brand and Yingcheng mineral chemical industry;
the ethylene-propylene-diene monomer rubber has the ethylidene norbornene content of 8.9 percent, the Mooney viscosity ML (1+4) at 125 ℃ of 82 percent and the ethylene content of 57.5 percent.
The production process in this example comprises the following steps:
s1, firstly, ethylene propylene diene monomer, activated zinc oxide, stearic acid, a flow aid and polyethylene glycol are put into a 75L internal mixer for pressure plastication, the temperature in the internal mixer is less than 115 ℃ when the feeding temperature is high, and the plastication time is 40-60 s.
S2, quickly extruding the carbon black, the decabromodiphenylethane, the magnesium hydroxide, the zinc borate, the antimony trioxide and the paraffin oil, pressurizing to a cleaning temperature of 105-.
S3, pressurizing and mixing to exhaust temperature of 125-; continuously pressurizing and banburying until the rubber discharge temperature is reached, and then discharging the rubber at 145-155 ℃.
And S4, transferring the rubber material discharged from the internal mixer into an open mill for roll wrapping, rubber cutting and disc falling, and then wrapping the roll again for rubber turning for 140-160 seconds to obtain the rubber material.
S5, adding the hinge material, the vulcanizing agent, the accelerator, the foaming agent and the foaming auxiliary agent into an internal mixer for pressurization mixing for 120 s.
S6, transferring the rubber material discharged from the internal mixer into an open mill for roll wrapping, rubber cutting and disc falling, and then re-wrapping the roll for rubber turning for 170-190 seconds to obtain the rubber material.
S7, rolling and discharging the rubber material to obtain the finished product, wherein the sheet discharging width is 140-150mm, and cooling by air cooling.
EXAMPLE III
110 parts of ethylene propylene diene monomer, KEP-2480 and Jinhu chemical;
quickly extruding carbon black N55030 parts, N550 parts, and Boo, Qingzhou;
30 parts of paraffin oil, LD-300, Guangzhou Liben;
6 parts of active zinc oxide, T-40, Shuiyilongxin zinc;
2 parts of stearic acid, SA1801, forster;
2 parts of a flow aid, RL-20 and Forster;
2 parts of polyethylene glycol, PEG-4000, Jinnuo chemical industry;
2 parts of vulcanizing agent, IS-60, and the balance;
9 parts of accelerator, M/BZ/EZ/TRA/TDEC-75, and the product;
10 parts of foaming agent, AC-75 parts and Achrom;
2 parts of foaming auxiliary agent, K5, and permanently mixing chemical engineering;
50 parts of decabromodiphenylethane, RDT-3, chemical engineering of Shouguangdongdong;
30 parts of magnesium hydroxide, FM-20 parts of Artemex;
30 parts of zinc borate, 777 parts of gold and Yingtai chemical industry;
40 parts of antimony trioxide, Jinshan brand and Yinheng mineral chemical industry;
the ethylene-propylene-diene monomer rubber has the ethylidene norbornene content of 8.9 percent, the Mooney viscosity ML (1+4) at 125 ℃ of 82 percent and the ethylene content of 57.5 percent.
The production process in this example comprises the following steps:
s1, firstly, ethylene propylene diene monomer, activated zinc oxide, stearic acid, a flow aid and polyethylene glycol are put into a 75L internal mixer for pressure plastication, the temperature in the internal mixer is less than 115 ℃ when the feeding temperature is high, and the plastication time is 40-60 s.
S2, adding the fast extrusion carbon black, decabromodiphenylethane, magnesium hydroxide, zinc borate, antimony trioxide and paraffin oil, pressurizing to a cleaning temperature of 105-.
S3, pressurizing and mixing until the exhaust temperature is 125-; continuously pressurizing and banburying to the glue discharging temperature, and then discharging the glue at 145-155 ℃.
And S4, transferring the rubber material discharged from the internal mixer into an open mill for roll wrapping, rubber cutting and disc falling, and then wrapping the roll again for rubber turning for 140-160 seconds to obtain the rubber material.
S5, adding the hinge material, the vulcanizing agent, the accelerator, the foaming agent and the foaming auxiliary agent into an internal mixer for pressurization mixing for 120 s.
S6, transferring the rubber material discharged from the internal mixer into an open mill for roll wrapping, rubber cutting and disc falling, then wrapping the roll again for rubber turning for 170-190 seconds, and obtaining the rubber material.
S7, rolling and discharging the rubber material to obtain the finished product, wherein the sheet discharging width is 140-150mm, and cooling by air to obtain the finished product.
The ethylene propylene diene monomer used in the first, second and third examples was an ethylene propylene diene monomer (KEP-2480) having a high ENB content, a high molecular weight and a medium ethylene content, and had an ENB content of 8.9%, a Mooney viscosity ML (1+4) at 125 ℃ of 82 and an ethylene content of 57.5%. The high ENB content ensures that the rubber compound has higher vulcanization speed, the high molecular weight ensures that the rubber compound is not easy to collapse in the microwave vulcanization extrusion process, and the medium ethylene ensures that the rubber compound has good tensile property. The carbon black N550 is quickly extruded, which not only can endow the ethylene propylene diene monomer (KEP-2480) with poor self-reinforcement with certain reinforcement, but also can ensure that the extrusion surface of the rubber compound is smooth. The multi-element combination of the flame retardant mixture, decabromodiphenylethane, magnesium hydroxide, zinc borate and antimony trioxide can play a role in high flame-retardant synergistic effect and can meet the requirement of self-extinguishing in a short time after leaving fire. The ADC chemical foaming agent is characterized by large gas evolution quantity, and the density of the sealing strip can be greatly reduced by decomposing a large quantity of gas through a microwave high-temperature hot air vulcanizing tank.
Comparative example
260 parts of ethylene propylene diene monomer;
quickly extruding 30 parts of carbon black;
30 parts of paraffin oil;
6 parts of active zinc oxide;
2 parts of stearic acid;
2 parts of a flow aid;
2 parts of polyethylene glycol;
2 parts of a vulcanizing agent;
10 parts of a foaming agent;
2 parts of a foaming auxiliary agent;
the production process in this example comprises the following steps:
s1, firstly, ethylene propylene diene monomer, activated zinc oxide, stearic acid, a flow aid and polyethylene glycol are put into a 75L internal mixer for pressure plastication, the temperature in the internal mixer is less than 115 ℃ when the feeding temperature is high, and the plastication time is 40-60 s.
S2, adding the fast-extrusion carbon black and the paraffin oil, pressurizing to a cleaning temperature of 105-.
S3, pressurizing and mixing until the exhaust temperature is 125-; continuously pressurizing and banburying until the rubber discharge temperature is reached, and then discharging the rubber at 145-155 ℃.
And S4, transferring the rubber material discharged from the internal mixer into an open mill for roll wrapping, rubber cutting and disc falling, and then wrapping the roll again for rubber turning for 140-160 seconds to obtain the rubber material.
S5, adding the hinge material, the vulcanizing agent, the foaming agent and the foaming auxiliary agent into an internal mixer for pressurization mixing for 120 s.
S6, transferring the rubber material discharged from the internal mixer into an open mill for roll wrapping, rubber cutting and disc falling, then wrapping the roll again for rubber turning for 170-190 seconds, and obtaining the rubber material.
S7, rolling and discharging the rubber material to obtain the finished product, wherein the sheet discharging width is 140-150mm, and cooling by air cooling.
The finished products obtained in the first, second and third examples and the comparative example were tested and compared, and the test results are as follows:
the above-described embodiments are merely preferred embodiments of the present invention, which is not intended to limit the present invention in any way. Those skilled in the art can make many changes and modifications to the disclosed embodiments, or modify equivalent embodiments to practice the disclosed embodiments, without departing from the scope of the disclosed embodiments. Therefore, equivalent variations made in accordance with the spirit of the present invention should be covered by the protection scope of the present invention without departing from the content of the technical scheme of the present invention.
Claims (6)
1. The EPDM flame-retardant foaming sealing strip for the energy product line cabinet is characterized by comprising the following raw materials in parts by weight: 100-120 parts of ethylene propylene diene monomer; quickly extruding 20-40 parts of carbon black N550; 150 parts of flame retardant 130; 20-40 parts of paraffin oil; 5-7 parts of active zinc oxide; 1-3 parts of stearic acid; 1-3 parts of a flow aid; 1-3 parts of polyethylene glycol; 1-3 parts of a vulcanizing agent; 8-10 parts of an accelerator; 9-11 parts of a foaming agent; 1-3 parts of a foaming auxiliary agent.
2. The EPDM flame retardant foaming sealing strip for the energy product line cabinet according to claim 1, which is characterized in that: the flame retardant comprises the following raw materials in parts by weight: 40-60 parts of decabromodiphenylethane, 20-40 parts of magnesium hydroxide, 20-40 parts of zinc borate and 20-40 parts of antimony trioxide.
3. The EPDM flame retardant foaming sealing strip for the energy product line cabinet according to claim 1, which is characterized in that: the ethylene-propylene-diene monomer rubber has the ethylidene norbornene content of 8.9 percent, the Mooney viscosity ML (1+4) at 125 ℃ of 82 percent and the ethylene content of 57.5 percent.
4. The EPDM flame retardant foaming sealing strip for the energy product line cabinet according to claim 1, which is characterized in that: the production process comprises the following steps:
s1, firstly, adding ethylene propylene diene monomer, active zinc oxide, stearic acid, a flow aid and polyethylene glycol into an internal mixer for pressure plastication for 40-60 s;
s2, adding the quick-extrusion carbon black, the flame retardant and the paraffin oil, pressurizing to a cleaning temperature, opening a material door, cleaning an upper top plug and the residual materials around a hopper opening to an internal mixing chamber;
s3, pressurizing and mixing to exhaust temperature, and half opening the upper top plug to exhaust once; continuously pressurizing and banburying until the rubber discharge temperature is reached, and then discharging rubber;
s4, transferring the rubber material discharged by the internal mixer into an open mill for roll wrapping, rubber cutting and disc falling, then wrapping the roll again for rubber turning for 140-160s to obtain the rubber material;
s5, adding the hinge material, the vulcanizing agent, the accelerator, the foaming agent and the foaming auxiliary agent into an internal mixer for pressurization mixing for 120 s;
s6, transferring the rubber material discharged by the internal mixer into an open mill for roll wrapping, rubber cutting and disc falling, then wrapping the roll again for rubber turning for 170-190 seconds to obtain the rubber material;
s7, rolling and discharging the rubber material to obtain the finished product, wherein the sheet discharging width is 140-150mm, and cooling by air cooling.
5. The EPDM flame retardant foaming sealing strip for the energy product line cabinet according to claim 4, wherein: the cleaning temperature is 105-115 ℃, the exhaust temperature is 125-135 ℃, and the glue discharging temperature is 145-155 ℃.
6. The EPDM flame retardant foaming sealing strip for the energy product line cabinet according to claim 4, wherein: in step S1, the charging temperature is set to a temperature less than 115 ℃.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115505215A (en) * | 2022-10-28 | 2022-12-23 | 江西奋发科技有限公司 | Low-smoke halogen-free flame-retardant rubber strip and preparation method thereof |
Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN1316453A (en) * | 2000-02-21 | 2001-10-10 | 住友化学工业株式会社 | Foamed rubber, its preparation method and composite containing the foamed rubber |
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| CN115505215A (en) * | 2022-10-28 | 2022-12-23 | 江西奋发科技有限公司 | Low-smoke halogen-free flame-retardant rubber strip and preparation method thereof |
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