KR100807895B1 - 올레핀 중합 촉매용 구형 담체의 제조방법 - Google Patents
올레핀 중합 촉매용 구형 담체의 제조방법 Download PDFInfo
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- KR100807895B1 KR100807895B1 KR1020060082595A KR20060082595A KR100807895B1 KR 100807895 B1 KR100807895 B1 KR 100807895B1 KR 1020060082595 A KR1020060082595 A KR 1020060082595A KR 20060082595 A KR20060082595 A KR 20060082595A KR 100807895 B1 KR100807895 B1 KR 100807895B1
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- South Korea
- Prior art keywords
- weight
- olefin polymerization
- carrier
- metal magnesium
- alcohol
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- 150000001336 alkenes Chemical class 0.000 title claims abstract description 15
- JRZJOMJEPLMPRA-UHFFFAOYSA-N olefin Natural products CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 title claims abstract description 15
- 239000002685 polymerization catalyst Substances 0.000 title claims abstract description 10
- 238000002360 preparation method Methods 0.000 title claims description 3
- 238000000034 method Methods 0.000 title abstract description 20
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims abstract description 40
- 229910052749 magnesium Inorganic materials 0.000 claims abstract description 33
- 239000011777 magnesium Substances 0.000 claims abstract description 33
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 claims abstract description 32
- 229910052751 metal Inorganic materials 0.000 claims abstract description 24
- 239000002184 metal Substances 0.000 claims abstract description 24
- 238000006243 chemical reaction Methods 0.000 claims abstract description 20
- IJGRMHOSHXDMSA-UHFFFAOYSA-N nitrogen Substances N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims abstract description 19
- -1 nitrogen halogen compound Chemical class 0.000 claims abstract description 16
- 229910052757 nitrogen Inorganic materials 0.000 claims abstract description 15
- 239000003999 initiator Substances 0.000 claims abstract description 12
- 150000001875 compounds Chemical class 0.000 claims abstract description 6
- 238000004519 manufacturing process Methods 0.000 claims description 11
- 229910052739 hydrogen Inorganic materials 0.000 claims description 10
- 239000001257 hydrogen Substances 0.000 claims description 10
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 9
- 229910052736 halogen Inorganic materials 0.000 claims description 9
- 125000000217 alkyl group Chemical group 0.000 claims description 8
- 125000003118 aryl group Chemical group 0.000 claims description 6
- 150000001298 alcohols Chemical class 0.000 claims description 2
- 125000004432 carbon atom Chemical group C* 0.000 claims description 2
- 125000005843 halogen group Chemical group 0.000 claims 4
- 239000002245 particle Substances 0.000 abstract description 59
- 238000009826 distribution Methods 0.000 abstract description 15
- 239000000047 product Substances 0.000 description 12
- 238000006116 polymerization reaction Methods 0.000 description 11
- JRNVZBWKYDBUCA-UHFFFAOYSA-N N-chlorosuccinimide Chemical compound ClN1C(=O)CCC1=O JRNVZBWKYDBUCA-UHFFFAOYSA-N 0.000 description 10
- 239000003054 catalyst Substances 0.000 description 9
- 239000000843 powder Substances 0.000 description 7
- 238000010992 reflux Methods 0.000 description 7
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 6
- 239000012265 solid product Substances 0.000 description 6
- 150000002367 halogens Chemical class 0.000 description 5
- XDKQUSKHRIUJEO-UHFFFAOYSA-N magnesium;ethanolate Chemical compound [Mg+2].CC[O-].CC[O-] XDKQUSKHRIUJEO-UHFFFAOYSA-N 0.000 description 5
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 4
- LRHPLDYGYMQRHN-UHFFFAOYSA-N N-Butanol Chemical compound CCCCO LRHPLDYGYMQRHN-UHFFFAOYSA-N 0.000 description 4
- 230000032683 aging Effects 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 4
- 230000001186 cumulative effect Effects 0.000 description 4
- 239000010419 fine particle Substances 0.000 description 4
- 239000002002 slurry Substances 0.000 description 4
- 238000003756 stirring Methods 0.000 description 4
- 238000012662 bulk polymerization Methods 0.000 description 3
- 238000012685 gas phase polymerization Methods 0.000 description 3
- VLKZOEOYAKHREP-UHFFFAOYSA-N n-Hexane Chemical compound CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 description 3
- 229920000642 polymer Polymers 0.000 description 3
- ZCYVEMRRCGMTRW-UHFFFAOYSA-N 7553-56-2 Chemical compound [I] ZCYVEMRRCGMTRW-UHFFFAOYSA-N 0.000 description 2
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 2
- TWRXJAOTZQYOKJ-UHFFFAOYSA-L Magnesium chloride Chemical compound [Mg+2].[Cl-].[Cl-] TWRXJAOTZQYOKJ-UHFFFAOYSA-L 0.000 description 2
- AMQJEAYHLZJPGS-UHFFFAOYSA-N N-Pentanol Chemical compound CCCCCO AMQJEAYHLZJPGS-UHFFFAOYSA-N 0.000 description 2
- PCLIMKBDDGJMGD-UHFFFAOYSA-N N-bromosuccinimide Chemical compound BrN1C(=O)CCC1=O PCLIMKBDDGJMGD-UHFFFAOYSA-N 0.000 description 2
- 229910002092 carbon dioxide Inorganic materials 0.000 description 2
- 239000001569 carbon dioxide Substances 0.000 description 2
- 238000001816 cooling Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000000635 electron micrograph Methods 0.000 description 2
- 150000002366 halogen compounds Chemical class 0.000 description 2
- PNDPGZBMCMUPRI-UHFFFAOYSA-N iodine Chemical compound II PNDPGZBMCMUPRI-UHFFFAOYSA-N 0.000 description 2
- 229910052740 iodine Inorganic materials 0.000 description 2
- 239000011630 iodine Substances 0.000 description 2
- ZXEKIIBDNHEJCQ-UHFFFAOYSA-N isobutanol Chemical compound CC(C)CO ZXEKIIBDNHEJCQ-UHFFFAOYSA-N 0.000 description 2
- BDERNNFJNOPAEC-UHFFFAOYSA-N propan-1-ol Chemical compound CCCO BDERNNFJNOPAEC-UHFFFAOYSA-N 0.000 description 2
- 239000011949 solid catalyst Substances 0.000 description 2
- 239000012798 spherical particle Substances 0.000 description 2
- 238000001694 spray drying Methods 0.000 description 2
- APQIUTYORBAGEZ-UHFFFAOYSA-N 1,1-dibromoethane Chemical compound CC(Br)Br APQIUTYORBAGEZ-UHFFFAOYSA-N 0.000 description 1
- YRIZYWQGELRKNT-UHFFFAOYSA-N 1,3,5-trichloro-1,3,5-triazinane-2,4,6-trione Chemical compound ClN1C(=O)N(Cl)C(=O)N(Cl)C1=O YRIZYWQGELRKNT-UHFFFAOYSA-N 0.000 description 1
- WDRFYIPWHMGQPN-UHFFFAOYSA-N 2-chloroisoindole-1,3-dione Chemical compound C1=CC=C2C(=O)N(Cl)C(=O)C2=C1 WDRFYIPWHMGQPN-UHFFFAOYSA-N 0.000 description 1
- WVDDGKGOMKODPV-UHFFFAOYSA-N Benzyl alcohol Chemical compound OCC1=CC=CC=C1 WVDDGKGOMKODPV-UHFFFAOYSA-N 0.000 description 1
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- 239000011954 Ziegler–Natta catalyst Substances 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 238000004220 aggregation Methods 0.000 description 1
- 230000002776 aggregation Effects 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 238000009835 boiling Methods 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 239000003426 co-catalyst Substances 0.000 description 1
- 238000010960 commercial process Methods 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- HPXRVTGHNJAIIH-UHFFFAOYSA-N cyclohexanol Chemical compound OC1CCCCC1 HPXRVTGHNJAIIH-UHFFFAOYSA-N 0.000 description 1
- XCIXKGXIYUWCLL-UHFFFAOYSA-N cyclopentanol Chemical compound OC1CCCC1 XCIXKGXIYUWCLL-UHFFFAOYSA-N 0.000 description 1
- 230000006378 damage Effects 0.000 description 1
- VRLDVERQJMEPIF-UHFFFAOYSA-N dbdmh Chemical compound CC1(C)N(Br)C(=O)N(Br)C1=O VRLDVERQJMEPIF-UHFFFAOYSA-N 0.000 description 1
- 230000000911 decarboxylating effect Effects 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- KZNICNPSHKQLFF-UHFFFAOYSA-N dihydromaleimide Natural products O=C1CCC(=O)N1 KZNICNPSHKQLFF-UHFFFAOYSA-N 0.000 description 1
- 238000001493 electron microscopy Methods 0.000 description 1
- 230000009969 flowable effect Effects 0.000 description 1
- 229940091173 hydantoin Drugs 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 238000002347 injection Methods 0.000 description 1
- 239000007924 injection Substances 0.000 description 1
- PHTQWCKDNZKARW-UHFFFAOYSA-N isoamylol Chemical compound CC(C)CCO PHTQWCKDNZKARW-UHFFFAOYSA-N 0.000 description 1
- 150000002680 magnesium Chemical class 0.000 description 1
- OTCKOJUMXQWKQG-UHFFFAOYSA-L magnesium bromide Chemical compound [Mg+2].[Br-].[Br-] OTCKOJUMXQWKQG-UHFFFAOYSA-L 0.000 description 1
- 229910001623 magnesium bromide Inorganic materials 0.000 description 1
- 229910001629 magnesium chloride Inorganic materials 0.000 description 1
- BLQJIBCZHWBKSL-UHFFFAOYSA-L magnesium iodide Chemical compound [Mg+2].[I-].[I-] BLQJIBCZHWBKSL-UHFFFAOYSA-L 0.000 description 1
- 229910001641 magnesium iodide Inorganic materials 0.000 description 1
- HONQAQNYJBKAMA-UHFFFAOYSA-L magnesium;ethyl carbonate Chemical compound [Mg+2].CCOC([O-])=O.CCOC([O-])=O HONQAQNYJBKAMA-UHFFFAOYSA-L 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- KPSSIOMAKSHJJG-UHFFFAOYSA-N neopentyl alcohol Chemical compound CC(C)(C)CO KPSSIOMAKSHJJG-UHFFFAOYSA-N 0.000 description 1
- 150000002894 organic compounds Chemical class 0.000 description 1
- 150000002896 organic halogen compounds Chemical class 0.000 description 1
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 1
- 125000004805 propylene group Chemical group [H]C([H])([H])C([H])([*:1])C([H])([H])[*:2] 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000001953 recrystallisation Methods 0.000 description 1
- 238000001226 reprecipitation Methods 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 229960002317 succinimide Drugs 0.000 description 1
- 229950009390 symclosene Drugs 0.000 description 1
- 230000002194 synthesizing effect Effects 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 239000004711 α-olefin Substances 0.000 description 1
Images
Classifications
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F4/00—Polymerisation catalysts
- C08F4/02—Carriers therefor
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
- B01J21/10—Magnesium; Oxides or hydroxides thereof
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
- B01J35/51—Spheres
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F10/00—Homopolymers and copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F4/00—Polymerisation catalysts
- C08F4/06—Metallic compounds other than hydrides and other than metallo-organic compounds; Boron halide or aluminium halide complexes with organic compounds containing oxygen
- C08F4/10—Metallic compounds other than hydrides and other than metallo-organic compounds; Boron halide or aluminium halide complexes with organic compounds containing oxygen of alkaline earth metals, zinc, cadmium, mercury, copper or silver
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- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Organic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- Medicinal Chemistry (AREA)
- Polymers & Plastics (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Transition And Organic Metals Composition Catalysts For Addition Polymerization (AREA)
- Polymerization Catalysts (AREA)
Abstract
Description
입자모양 | 겉보기밀도(g/cc) | 평균입경(D50,㎛) | 입도분포지수 | |
실시예1 | 구형 | 0.32 | 37 | 0.78 |
실시예2 | 구형 | 0.33 | 28 | 0.75 |
실시예3 | 구형 | 0.31 | 32 | 0.77 |
실시예4 | 구형 | 0.30 | 31 | 0.83 |
실시예5 | 구형 | 0.32 | 35 | 0.88 |
비교예 | 구형 | 0.30 | 45 | 1.21 |
Claims (3)
- 반응개시제로서 다음의 일반식 I 내지 IV의 화합물로 이루어진 군에서 선택되는 질소 할로겐 화합물의 존재하에 금속 마그네슘과 알코올을 반응시키는 것을 포함하며, 상기 질소 할로겐 화합물은 상기 금속 마그네슘 1중량부에 대해 0.001~0.2중량부, 상기 알코올은 상기 금속 마그네슘 1중량부에 대해 5~50중량부가 사용되는 것을 특징으로 하는 올레핀 중합 촉매용 구형 담체의 제조방법:여기에서 X는 할로겐, R1, R2, R3, R4는 독립적으로 수소 또는 C1~12의 알킬 또는 아릴;여기에서 X는 할로겐;여기에서 X는 할로겐, R1, R2, R3, R4는 독립적으로 수소 또는 C1~12의 알킬 또는 아릴; 및여기에서 X는 할로겐, R1, R2는 독립적으로 수소 또는 C1~12의 알킬 또는 아릴.
- 삭제
- 제1항에 있어서, 상기 알코올은 일반식 ROH(여기에서, R은 탄소수 1~6의 알킬기이다)로 표시되는 지방족 알코올 및 방향족 알코올로 이루어진 군으로부터 선택된 1종류 이상의 알코올을 단독 또는 혼합하여 사용하는 것을 특징으로 하는 올레핀 중합 촉매용 구형 담체의 제조방법.
Priority Applications (7)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
KR1020060082595A KR100807895B1 (ko) | 2006-08-30 | 2006-08-30 | 올레핀 중합 촉매용 구형 담체의 제조방법 |
TW095139577A TWI331612B (en) | 2006-08-30 | 2006-10-26 | Method for preparation of spherical support for olefin polymerization catalyst |
DE602006012325T DE602006012325D1 (de) | 2006-08-30 | 2006-10-31 | Verfahren zur Herstellung von sphärischen Trägern für Polymerisationsatalystoren von Olefinen |
EP06022739A EP1905783B1 (en) | 2006-08-30 | 2006-10-31 | Method for preparation of spherical support for olefin polymerization catalyst |
JP2006300102A JP4662555B2 (ja) | 2006-08-30 | 2006-11-06 | オレフイン重合触媒用球形担体の製造方法 |
CN2006101624065A CN101134789B (zh) | 2006-08-30 | 2006-11-22 | 烯烃聚合催化剂用球形载体的制备方法 |
US11/614,390 US7767614B2 (en) | 2006-08-30 | 2006-12-21 | Method for preparation of spherical support for olefin polymerization catalyst |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
KR1020060082595A KR100807895B1 (ko) | 2006-08-30 | 2006-08-30 | 올레핀 중합 촉매용 구형 담체의 제조방법 |
Publications (1)
Publication Number | Publication Date |
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KR100807895B1 true KR100807895B1 (ko) | 2008-02-27 |
Family
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Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
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KR1020060082595A KR100807895B1 (ko) | 2006-08-30 | 2006-08-30 | 올레핀 중합 촉매용 구형 담체의 제조방법 |
Country Status (7)
Country | Link |
---|---|
US (1) | US7767614B2 (ko) |
EP (1) | EP1905783B1 (ko) |
JP (1) | JP4662555B2 (ko) |
KR (1) | KR100807895B1 (ko) |
CN (1) | CN101134789B (ko) |
DE (1) | DE602006012325D1 (ko) |
TW (1) | TWI331612B (ko) |
Cited By (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2010005164A3 (ko) * | 2008-07-11 | 2010-03-11 | 삼성토탈 주식회사 | 올레핀 중합 촉매용 구형 담체의 크기를 조절하는 방법 |
KR101140112B1 (ko) * | 2009-05-22 | 2012-04-30 | 삼성토탈 주식회사 | 올레핀 중합 촉매용 디알콕시마그네슘 담체의 제조 방법, 이를 이용한 올레핀 중합 촉매의 제조 방법 및 이를 이용한 올레핀 중합 방법 |
KR20240001338A (ko) | 2022-06-24 | 2024-01-03 | 한국에너지기술연구원 | 코어-쉘 전극촉매 자동화 제조시스템 |
Families Citing this family (7)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
KR100874089B1 (ko) * | 2007-04-25 | 2008-12-16 | 삼성토탈 주식회사 | 프로필렌 중합용 촉매의 제조방법 |
KR100954056B1 (ko) * | 2007-12-12 | 2010-04-20 | 삼성토탈 주식회사 | 올레핀 중합 촉매용 구형 담체의 제조방법 |
EP2194070B1 (en) | 2008-12-03 | 2012-08-22 | Süd-Chemie IP GmbH & Co. KG | Electron donor composition for a solid catalyst, solid catalyst composition used in the polymerisation of alpha-olefins, and process for the production of a polymer consisting of alpha-olefin units using the solid catalyst composition |
CN104592427B (zh) * | 2015-01-28 | 2017-09-15 | 任丘市利和科技发展有限公司 | 一种烯烃聚合催化剂载体、其制备方法及应用 |
CN108219040B (zh) * | 2018-01-09 | 2020-07-17 | 为信(深圳)材料科技有限公司 | 球形烷氧基镁颗粒的组份、制备方法及应用 |
CN113801253A (zh) * | 2020-06-17 | 2021-12-17 | 中化学科学技术研究有限公司 | 一种催化剂组分、固体钛催化剂、乙烯聚合催化剂及其应用和聚乙烯产品 |
CN115894174A (zh) * | 2022-11-22 | 2023-04-04 | 任国辉 | 一种用于烯烃聚合催化剂的二烷氧基镁载体的制备方法 |
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WO2010005164A3 (ko) * | 2008-07-11 | 2010-03-11 | 삼성토탈 주식회사 | 올레핀 중합 촉매용 구형 담체의 크기를 조절하는 방법 |
KR101140112B1 (ko) * | 2009-05-22 | 2012-04-30 | 삼성토탈 주식회사 | 올레핀 중합 촉매용 디알콕시마그네슘 담체의 제조 방법, 이를 이용한 올레핀 중합 촉매의 제조 방법 및 이를 이용한 올레핀 중합 방법 |
KR20240001338A (ko) | 2022-06-24 | 2024-01-03 | 한국에너지기술연구원 | 코어-쉘 전극촉매 자동화 제조시스템 |
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CN101134789B (zh) | 2010-10-27 |
US20080064589A1 (en) | 2008-03-13 |
TWI331612B (en) | 2010-10-11 |
CN101134789A (zh) | 2008-03-05 |
TW200811210A (en) | 2008-03-01 |
JP2008056885A (ja) | 2008-03-13 |
DE602006012325D1 (de) | 2010-04-01 |
JP4662555B2 (ja) | 2011-03-30 |
EP1905783B1 (en) | 2010-02-17 |
US7767614B2 (en) | 2010-08-03 |
EP1905783A1 (en) | 2008-04-02 |
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