TW202222859A - 馬來酰亞胺系共聚物 - Google Patents
馬來酰亞胺系共聚物 Download PDFInfo
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- TW202222859A TW202222859A TW110135124A TW110135124A TW202222859A TW 202222859 A TW202222859 A TW 202222859A TW 110135124 A TW110135124 A TW 110135124A TW 110135124 A TW110135124 A TW 110135124A TW 202222859 A TW202222859 A TW 202222859A
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- mass
- maleimide
- resin
- tert
- copolymer
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- 229920001577 copolymer Polymers 0.000 title claims abstract description 88
- 239000002245 particle Substances 0.000 claims abstract description 48
- PEEHTFAAVSWFBL-UHFFFAOYSA-N Maleimide Chemical compound O=C1NC(=O)C=C1 PEEHTFAAVSWFBL-UHFFFAOYSA-N 0.000 claims description 94
- 229920005989 resin Polymers 0.000 claims description 59
- 239000011347 resin Substances 0.000 claims description 59
- 229920000122 acrylonitrile butadiene styrene Polymers 0.000 claims description 17
- 239000011342 resin composition Substances 0.000 claims description 17
- 239000000155 melt Substances 0.000 claims description 16
- 238000004519 manufacturing process Methods 0.000 claims description 12
- 229920006015 heat resistant resin Polymers 0.000 claims description 7
- 230000009477 glass transition Effects 0.000 claims description 6
- 238000002156 mixing Methods 0.000 claims description 4
- 238000004898 kneading Methods 0.000 abstract description 17
- 238000001125 extrusion Methods 0.000 abstract description 7
- 239000000178 monomer Substances 0.000 description 91
- PPBRXRYQALVLMV-UHFFFAOYSA-N Styrene Chemical compound C=CC1=CC=CC=C1 PPBRXRYQALVLMV-UHFFFAOYSA-N 0.000 description 50
- 238000000034 method Methods 0.000 description 42
- ZWEHNKRNPOVVGH-UHFFFAOYSA-N 2-Butanone Chemical compound CCC(C)=O ZWEHNKRNPOVVGH-UHFFFAOYSA-N 0.000 description 33
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 27
- 238000006116 polymerization reaction Methods 0.000 description 25
- NLHHRLWOUZZQLW-UHFFFAOYSA-N Acrylonitrile Chemical compound C=CC#N NLHHRLWOUZZQLW-UHFFFAOYSA-N 0.000 description 20
- 229920000578 graft copolymer Polymers 0.000 description 19
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- -1 peroxide tert-butyl benzoate Chemical class 0.000 description 12
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Images
Classifications
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- B29C48/022—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor characterised by the choice of material
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- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F222/00—Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by a carboxyl radical and containing at least one other carboxyl radical in the molecule; Salts, anhydrides, esters, amides, imides, or nitriles thereof
- C08F222/36—Amides or imides
- C08F222/40—Imides, e.g. cyclic imides
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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
- C08F212/00—Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by an aromatic carbocyclic ring
- C08F212/02—Monomers containing only one unsaturated aliphatic radical
- C08F212/04—Monomers containing only one unsaturated aliphatic radical containing one ring
- C08F212/06—Hydrocarbons
- C08F212/08—Styrene
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- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
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- C08F8/32—Introducing nitrogen atoms or nitrogen-containing groups by reaction with amines
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- C—CHEMISTRY; METALLURGY
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- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F8/00—Chemical modification by after-treatment
- C08F8/48—Isomerisation; Cyclisation
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Abstract
本發明的課題為,提供一種熔融擠出混煉時的分散性優異的馬來酰亞胺系共聚物。根據本發明可提供一種平均粒子直徑為75μm以上,1000μm的篩子上小於5質量%的粉狀的馬來酰亞胺系共聚物(A)。
Description
本發明涉及熔融擠出混煉時的分散性優異的馬來酰亞胺系共聚物。
ABS樹脂是以丙烯腈、丁二烯、苯乙烯為主成分的熱塑性樹脂,憑藉其優異的機械強度、外觀、耐化學性、成型性等被廣泛應用於汽車、家電、OA設備、住宅建材、日用品等領域。但在汽車內裝材料等要求耐熱性的用途中,耐熱性可能會不足。作為提高耐熱性的技術,可使用馬來酰亞胺系共聚物或α-甲基苯乙烯系共聚物等(專利文獻1、2)。此外,近年來,在雙軸擠出機的高扭矩化和螺桿深槽化方面取得了進展,使得高排出量成為可能。此外,已知在熔融混煉的初期階段種固體樹脂的塑化進行,但固體樹脂引發可塑化需要除去固體樹脂周圍存在的空氣相,並壓縮直至接近真正的固體密度。因此,已知熔融混煉粉末時,必須有效消除空氣相引發可塑化,必須施加高混煉壓力以增加堆積密度。
[現有技術文獻]
[專利文獻]
專利文獻1:日本特開2003-41080號公報
專利文獻2: WO2010/082617號公報
[發明要解決的課題]
本發明的課題在於提供熔融擠出混煉時的分散性優異的馬來酰亞胺系共聚物。
[解決課題的技術手段]
(1)平均粒子直徑為75μm以上,在1000μm的篩子上小於5質量%的粉狀的馬來酰亞胺系共聚物(A)。
(2)如(1)所述的馬來酰亞胺系共聚物(A),其玻璃化轉變溫度為170~210℃。
(3)如(1)或(2)所述的馬來酰亞胺系共聚物(A),其在260℃、剪切速度120/sec下的熔融黏度為1000Pa・s以上。
(4)一種耐熱性樹脂組合物的製造方法,使用擠出機將(1)~(3)中任一項所述的馬來酰亞胺系共聚物(A)和選自ABS樹脂、ASA樹脂、AES樹脂、SAN樹脂中的至少一種的樹脂(B)熔融混煉。
[發明效果]
本發明的馬來酰亞胺系共聚物由於馬來酰亞胺系共聚物的分散性優異,因此在ABS樹脂等樹脂中的分散性也充分。因此,即使在使用分散性稍差的深槽螺桿的高排出量條件下,也可以獲得馬來酰亞胺系共聚物的分散狀態良好且無外觀缺陷的成型品。
<術語說明>
本說明書中,例如“A~B”這樣的記載是指A以上且B以下。
以下對本發明的實施方式進行詳細說明。以下所示的實施方式可以相互組合。
本發明的馬來酰亞胺系共聚物的平均粒子直徑為70μm以上,篩子上1000μm以上的小於5質量%。
馬來酰亞胺系共聚物(A)是具有馬來酰亞胺係單體單元、苯乙烯係單體單元的共聚物。在本發明中,還可以具有丙烯腈係單體單元、不飽和二羧酸酐係單體單元。
馬來酰亞胺係單體單元例如為N-甲基馬來酰亞胺、N-丁基馬來酰亞胺、N-環己基馬來酰亞胺等N-烷基馬來酰亞胺;以及N-苯基馬來酰亞胺、N-氯苯基馬來酰亞胺、N-甲基苯基馬來酰亞胺、N-甲氧基苯基馬來酰亞胺、N-三溴苯基馬來酰亞胺等。其中優選N-苯基馬來酰亞胺。馬來酰亞胺係單體單元可以單獨使用也可以將2種以上並用。馬來酰亞胺係單體單元例如可以使用由馬來酰亞胺係單體組成的原料。或者可通過使用氨或伯胺將由不飽和二羧酸單體單元組成的原料酰亞胺化來獲得。
馬來酰亞胺系共聚物(A)優選在馬來酰亞胺系共聚物(A)100質量%中含有馬來酰亞胺係單體單元40~70質量%,更優選含有45~60質量%。馬來酰亞胺係單體單元的含量具體而言例如為40、41、42、43、44、45、50、55、60或70質量%,也可以是任意2個所例示數值之間的範圍內。如果馬來酰亞胺係單體單元的含量在該範圍內,則可提高與下文中選自ABS樹脂、ASA樹脂、AES樹脂、SAN樹脂中的至少一種樹脂(B)的相容性,樹脂組合物的衝擊強度優異。馬來酰亞胺係單體單元的含量為由13C-NMR測得的值。
苯乙烯係單體單元為苯乙烯、鄰甲基苯乙烯、間甲基苯乙烯、對甲基苯乙烯、2,4-二甲基苯乙烯、乙基苯乙烯、對叔丁基苯乙烯、α-甲基苯乙烯、α-甲基-對甲基苯乙烯等。其中,優選苯乙烯。苯乙烯係單體單元可以單獨使用也可以將2種以上並用。
馬來酰亞胺系共聚物(A)100質量%中優選含有苯乙烯係單體單元20~60質量%,更優選含有35~55質量%。具體而言例如為20、30、40、45、46、47、48、49、50、55或60質量%,也可以是任意2個所例示數值之間的範圍內。如果苯乙烯係單體單元的含量在該範圍內,則可提高與下文中選自ABS樹脂、ASA樹脂、AES樹脂、SAN樹脂中的至少一種樹脂(B)的相容性,樹脂組合物的衝擊強度優異。苯乙烯係單體單元的含量是採用13C-NMR測得的值。
丙烯腈係單體單元為丙烯腈、甲基丙烯腈、乙基丙烯腈、富馬腈等。其中,優選丙烯腈。丙烯腈係單體單元可以單獨使用也可以將2種以上並用。
馬來酰亞胺系共聚物(A)100質量%中優選含有丙烯腈係單體單元0~20質量%,更優選含有0~15質量%。具體而言例如為0、5、6、7、8、9、10、15或20質量%,也可以是任意2個所例示數值之間的範圍內。如果丙烯腈係單體單元的含量在該範圍內,則樹脂組合物的耐化學性優異。丙烯腈係單體單元的含量是採用13C-NMR測得的值。
不飽和二羧酸酐係單體單元為馬來酸酐、衣康酸酐、檸康酸酐、烏頭酸酐等。其中優選馬來酸酐。不飽和二羧酸酐係單體單元可以單獨使用也可以將2種以上並用。
馬來酰亞胺系共聚物(A)100質量%中優選含有不飽和二羧酸酐係單體單元0~10質量%,更優選含有0~5質量%。具體而言例如為0、1、2、3、4、5、6、7、8、9或10質量%,也可以是任意2個所例示數值之間的範圍內。如果不飽和二羧酸酐係單體單元的含量在該範圍內,則馬來酰亞胺系共聚物的熱穩定性優異。不飽和二羧酸酐係單體單元的含量是採用滴定法測得的值。
本發明的一個方式中的馬來酰亞胺系共聚物(A)100質量%中優選含有馬來酰亞胺係單體單元40~70質量%、苯乙烯係單體單元20~60質量%、丙烯腈係單體單元0~20質量%、不飽和二羧酸酐係單體單元0~10質量%。馬來酰亞胺系共聚物(A)100質量%中更優選含有馬來酰亞胺係單體單元45~60質量%、苯乙烯係單體單元35~55質量%、丙烯腈係單體單元0~15質量%、不飽和二羧酸酐係單體單元0~5質量%。若構成單元在上述範圍內,則馬來酰亞胺系共聚物(A)的流動性、耐熱性、熱穩定性優異。
從有效提高選自後述的ABS樹脂、ASA樹脂、AES樹脂、SAN樹脂的至少1種樹脂(B)的耐熱性的方面考慮,馬來酰亞胺系共聚物(A)的玻璃化轉變溫度(Tmg)優選為170~210℃,更優選為185~205℃。玻璃化轉變溫度是採用DSC,在下述測得條件下測得的測定值。
裝置名:Seiko Instruments株式會社制的Robot DSC6200
升溫速度:10℃/分鐘
馬來酰亞胺系共聚物(A)的重均分子量(Mw)優選為6萬~15萬,更優選為7萬~14萬。具體而言例如為6、7、8、9、10、11、12、13、14或15萬,也可以是任意2個所例示數值之間的範圍內。若馬來酰亞胺系共聚物(A)的重均分子量(Mw)為上述範圍內,則通過與後述的樹脂(B)熔融混煉而得到的樹脂組合物的流動性和衝擊強度的平衡優異。。為了控制馬來酰亞胺系共聚物(A)的重均分子量(Mw),除了調整聚合溫度、聚合時間以及聚合引髮劑添加量之外,還有調整溶劑濃度和鏈轉移劑添加量等的方法。馬來酰亞胺系共聚物(A)的重均分子量是採用凝膠滲透色譜(GPC)測得的聚苯乙烯換算值,在以下條件下測定。
裝置名:SYSTEM-21 Shodex(昭和電工株式會社制)
柱:PL gel MIXED-B 3根串聯
溫度:40℃
檢測:差示折射率
溶劑:四氫呋喃
濃度:2質量%
標準曲線:使用標準聚苯乙烯(PS)(PL公司製)繪製。
作為馬來酰亞胺系共聚物(A)的製造方法,可採用公知方法。例如有如下方法:將由苯乙烯係單體、馬來酰亞胺係單體、不飽和二羧酸酐係單體、其他可共聚的單體構成的單體混合物共聚;或者將由苯乙烯係單體、不飽和二羧酸酐係單體、其他可共聚的單體構成的單體混合物共聚後,使不飽和二羧酸酐係單體單元的一部分與氨或伯胺反應進行酰亞胺化而轉變為馬來酰亞胺係單體單元(以下稱為“後酰亞胺化法”)。
馬來酰亞胺系共聚物(A)的聚合方式例如有溶液聚合、本體聚合等。從通過一邊分批添加一邊聚合可得到聚合組成更均勻的馬來酰亞胺系共聚物(A)的觀點考慮,優選溶液聚合。溶液聚合的溶劑從不易產生副產物、不良影響小的觀點考慮優選為非聚合性。例如為丙酮、甲乙酮、甲基異丁基酮、苯乙酮等酮類;四氫呋喃、1,4-二噁烷等醚類;苯、甲苯、二甲苯、氯苯等芳香族烴;N,N-二甲基甲酰胺、二甲基亞砜、N-甲基-2-吡咯烷酮等。從對馬來酰亞胺系共聚物(A)進行脫揮回收時容易去除溶劑的觀點考慮,優選甲乙酮、甲基異丁基酮。對於聚合工藝,連續聚合式、批次式(分批式)、半分批式均可適用。聚合方法沒有特別限定,但從可通過簡單的工藝生產率良好地進行製造的觀點考慮,優選自由基聚合。
溶液聚合或本體聚合中可使用聚合引髮劑、鏈轉移劑。聚合溫度優選為80~150℃的範圍。聚合引髮劑例如為偶氮二異丁腈、偶氮二環己基甲腈、偶氮二甲基丙腈、偶氮二甲基丁腈等偶氮系化合物;過氧化苯甲酰、過氧化苯甲酸叔丁酯、1,1-二(叔丁基過氧化)環己烷、叔丁基過氧化異丙基單碳酸酯、過氧化-2-乙基己酸叔丁酯、二叔丁基過氧化物、過氧化二異丙苯、乙基-3,3-二(叔丁基過氧化)丁酸酯等過氧化物類。可以使用其中1種也可以將2種以上組合使用。從控制聚合反應速度和聚合率的觀點考慮,優選使用10小時半衰期為70~120℃的偶氮系化合物或有機過氧化物。聚合引髮劑的使用量沒有特別限定,相對於全部單體單元100質量%優選使用0.1~1.5質量%,進一步優選為0.1~1.0質量%。如果聚合引髮劑的使用量為0.1質量%以上,則可得到足夠的聚合速度,因而優選。如果聚合引髮劑的使用量為1.5質量%以下,則可抑制聚合速度,因此容易控制反應,容易得到目標分子量。鏈轉移劑例如有正辛硫醇、正十二烷基硫醇、叔十二烷基硫醇、α-甲基苯乙烯二聚體、巰基乙酸乙酯、檸檬烯、萜品油烯等。鏈轉移劑量的使用量只要可得到目標分子量就沒有特別限定,但相對於全部單體單元100質量%優選為0.1~0.8質量%,更優選為0.15~0.5質量%。如果鏈轉移劑的使用量為0.1質量%~0.8質量%,則可容易得到目標分子量。
馬來酰亞胺系共聚物(A)的馬來酰亞胺係單體單元的導入有使馬來酰亞胺係單體共聚的方法和後酰亞胺化法。後酰亞胺化法由於馬來酰亞胺系共聚物(A)中的殘留馬來酰亞胺係單體量少而優選。後酰亞胺化法是將由苯乙烯係單體、不飽和二羧酸酐係單體、其他可共聚單體構成的單體混合物共聚後,使不飽和二羧酸酐係單體單元的一部分與氨或伯胺反應進行酰亞胺化而轉變為馬來酰亞胺係單體單元的方法。作為伯胺,例如有甲胺、乙胺、正丙胺、異丙胺、正丁胺、正戊胺、正己胺、正辛胺、環己胺、癸胺等烷基胺類以及氯或溴取代的烷基胺;苯胺、甲苯胺、萘胺等芳香族胺,其中優選苯胺。這些伯胺可以單獨使用也可以將2種以上並用。採用後酰亞胺化時,在伯胺與不飽和二羧酸酐係單體單元的反應中,為了提高脫水閉環反應可使用催化劑。催化劑例如為三甲胺、三乙胺、三丙胺、三丁胺、N,N-二甲基苯胺、N,N-二乙基苯胺等叔胺。後酰亞胺化的溫度優選為100~250℃,更優選為120~200℃。如果後酰亞胺化反應的溫度為100℃以上,則可提高反應速度,從生產率的觀點考慮優選。如果酰亞胺化反應的溫度為250℃以下,則能夠抑制馬來酰亞胺系共聚物(A)的熱劣化導致的物性下降,因而優選。
馬來酰亞胺系共聚物(A)的溶液聚合結束後的溶液或酰亞胺化結束後的溶液去除溶液聚合所使用的溶劑和未反應單體等揮發成分的方法(脫揮方法)可採用公知方法。例如可使用帶加熱器的真空脫揮槽或者帶排氣孔的脫揮擠出機。經脫揮的熔融狀態的馬來酰亞胺系共聚物(A)被轉移至造粒步驟,從多孔模呈繩狀擠出,採用冷切方式、空中熱切方式、水中熱切方式加工成顆粒狀。
顆粒狀的馬來酰亞胺系共聚物(A)可以使用公知的粉碎機加工成粉末狀。粉碎機例如可列舉篩網式微粉碎機和衝擊型粉碎機。
馬來酰亞胺系共聚物(A)是粉末狀,其平均粒子直徑為75μm以上,優選為80~300μm,更優選為100~250μm。具體而言例如為75、80、95、100、110、120、130、140、150、160、170、180、190、200、210、220、230、240、250、260、270、280、290或300μm,也可以是任意2個所例示數值之間的範圍內。通過使其呈現粉末狀,熔融擠出混煉時的分散性大幅提高,但平均粒子直徑小於75μm時,當從料斗進料時,擠出機供應區可能會堵塞。它還增加了粉塵爆發性的風險。粉末的平均粒子直徑可使用JIS Z 8801的試驗篩子測定。使用網孔為1000、850、500、355、250、150、106、75、50μm的篩子,將噴灑抗靜電劑混合的馬來酰亞胺系共聚物的粉末50g放入網孔最大的篩子中蓋上蓋子,將篩子置於搖床上,搖晃20分鐘後,測定包含粉末的各篩子的質量,減去篩子的質量,即可計算出篩子上的粒度分佈。從粒度分佈的結果來看,質量從網孔大的開始依次相加,平均粒子直徑是從夾住累積質量50%的兩點網孔(粒子直徑)和50%的交點求出的粒子直徑。例如,使用篩網式微粉碎機時,平均粒子直徑可根據篩網直徑和旋轉數調節。
粉狀的馬來酰亞胺系共聚物(A)的1000μm的篩子上小於5質量%,優選為小於3質量%。本發明中馬來酰亞胺系共聚物的粒子量規定的“篩子上”是指一種積酸分佈,表示特定粒子直徑以上的粒子量佔整體的百分比。
另外,本發明中馬來酰亞胺系共聚物的粒子量規定的“篩子下” 是指一種積酸分佈,表示特定粒子直徑以下的粒子量佔整體的百分比。具體而言例如為,1000μm的篩子上小於5、4、3、2或1質量%,也可以是任意2個所例示數值之間的範圍內。若1000μm的篩子上大於5質量%,則即使是粉末狀熔融擠出混煉時的分散性也會變差。1000μm的篩子上的含量可通過粉碎條件和粉碎後的分級調節。另外,75μm的篩子上至850μm的篩子下的含量優選為60~90質量%,更優選65~90質量%。具體而言例如為60、65、70、75、80、85或90質量%,也可以是任意2個所例示數值之間的範圍內。
作為馬來酰亞胺系共聚物(A),從賦予樹脂(B)耐熱性的觀點出發,可以使用含有大量馬來酰亞胺係單體單元的共聚物。此時,伴隨馬來酰亞胺係單體單元的含量的增加,馬來酰亞胺系共聚物(A)的熔融黏度提高,與樹脂(B)熔融混煉時會導致分散性的問題。在本發明所涉及的馬來酰亞胺系共聚物(A)的情況下,從賦予樹脂(B)耐熱性的觀點出發,即使採用含有大量馬來酰亞胺係單體單元的共聚物,與樹脂(B)熔融混煉時的分散性也優異。
從賦予樹脂(B)耐熱性的觀點出發,使用含有大量馬來酰亞胺係單體單元的馬來酰亞胺系共聚物(A)時,馬來酰亞胺系共聚物(A)在260℃、剪切速度120/sec下的熔融黏度優選為1000Pa・s以上,在260℃、剪切速度120/sec下的熔融黏度更優選為1000Pa・s以上,且在280℃、剪切速度120/sec下的熔融黏度為500Pa・s以上。馬來酰亞胺系共聚物(A)的熔融黏度越高,熔融擠出混煉時的分散性變差,通過將其製成粉末狀而提高分散性的效果也增加。另外,從分散性的觀點出發,馬來酰亞胺系共聚物(A)在280℃、剪切速度120/sec下的熔融黏度優選為3000Pa・s以下,更優選為2000Pa・s以下。熔融黏度是使用毛細管流變儀,用L=40mm、D=1mm的毛細管模測定的值。
樹脂(B)只要是選自ABS樹脂、ASA樹脂、AES樹脂、SAN樹脂,可以使用1種也可以使用2種以上。
ABS樹脂、ASA樹脂、AES樹脂是使橡膠狀聚合物至少與苯乙烯係單體和丙烯腈係單體接枝共聚而成的接枝共聚物。例如,使用聚丁二烯、苯乙烯-丁二烯共聚物等丁二烯系橡膠作為橡膠狀聚合物時為ABS樹脂;使用由丙烯酸丁酯或丙烯酸乙酯等構成的丙烯酸系橡膠時為ASA樹脂;使用乙烯-α-烯烴共聚物等乙烯系橡膠時為AES樹脂。進行接枝共聚時,可以組合使用這些橡膠狀聚合物中的2種以上。
作為ABS樹脂等的接枝共聚物的製造方法,可採用公知方法。例如可舉出採用乳化聚合或連續本體聚合的製造方法。採用乳化聚合的方法容易調整最終樹脂組合物中的橡膠狀聚合物的含量,因而優選。
採用乳化聚合的接枝共聚物的製造方法是使橡膠狀聚合物的乳膠與苯乙烯係單體和丙烯腈係單體乳化接枝聚合的方法(以下稱為“乳化接枝聚合法”)。採用乳化接枝聚合法可得到接枝共聚物的乳膠。
乳化接枝聚合法中,使用水、乳化劑、聚合引髮劑、鏈轉移劑,聚合溫度優選為30~90℃的範圍。乳化劑例如有陰離子表面活性劑、陽離子表面活性劑、兩性表面活性劑等。聚合引髮劑例如有異丙苯過氧化氫、過氧化二異丙苯、過氧化乙酸叔丁酯、過氧化苯甲酸叔己酯、過氧化苯甲酸叔丁酯等有機過氧化物;過硫酸鉀、過硫酸銨等過硫酸鹽類;偶氮二異丁腈等偶氮系化合物;鐵離子等還原劑;甲醛次硫酸氫鈉等二次還原劑;以及乙二胺四乙酸二鈉等螯合劑等。鏈轉移劑例如有正辛硫醇、正十二烷基硫醇、叔十二烷基硫醇、α-甲基苯乙烯二聚體、巰基乙酸乙酯、檸檬烯、萜品油烯等。
接枝共聚物的乳膠可採用公知方法凝固並回收接枝共聚物。例如向接枝共聚物的乳膠中加入凝固劑使其凝固,使用脫水機清洗脫水,經過乾燥步驟得到粉末狀的接枝共聚物。
從抗衝擊性的觀點考慮,採用乳化接枝聚合法得到的接枝共聚物中橡膠狀聚合物的含量優選為40~70質量%,更優選為45~65質量%。橡膠狀聚合物的含量例如可通過在乳化接枝聚合時調整苯乙烯係單體和丙烯腈係單體相對於橡膠狀聚合物的使用比例來調整。
從抗衝擊性或耐化學性的觀點考慮,除了採用乳化接枝聚合法得到的接枝共聚物的橡膠狀聚合物之外的構成單元優選為苯乙烯係單體單元65~85質量%、丙烯腈係單體單元15~35質量%。
接枝共聚物的凝膠成分優選為粒子狀。凝膠成分為苯乙烯係單體與丙烯腈係單體接枝共聚合而成的橡膠狀聚合物的粒子,是不溶於甲乙酮、甲苯等有機溶劑,可通過離心而分離的成分。有時可形成為在橡膠狀聚合物的粒子內部呈粒子狀內包有苯乙烯-丙烯腈系共聚物的包藏結構。若將接枝共聚物與苯乙烯-丙烯腈共聚物熔融共混,則凝膠成分以粒子狀作為分散相存在於苯乙烯-丙烯腈共聚物的連續相中。凝膠成分是將質量W的接枝共聚物溶解在甲乙酮中,使用離心機以20000rpm離心沉澱不溶物,傾析除去上清液,得到不溶成分,由真空乾燥後乾燥的不溶成分的質量S,根據式凝膠成分(質量%)=(S/W)×100計算出的值。此外,凝膠成分可以通過同樣地將接枝共聚物和苯乙烯-丙烯腈共聚物熔融共混的樹脂組合物溶解在甲乙酮中並離心來計算。
從抗衝擊性和成型品外觀的觀點考慮,接枝共聚物的凝膠成分的體積平均粒徑優選為0.10~1.0μm的範圍,更優選為0.15~0.50μm。體積平均粒徑是如下計算得到的值:將接枝共聚物與苯乙烯-丙烯腈共聚物熔融共混得到樹脂組合物的顆粒,從該顆粒切出超薄切片,使用透射電子顯微鏡(TEM)進行觀察,根據分散於連續相的粒子的圖像解析進行計算。體積平均粒徑例如可通過調整乳化接枝聚合時使用的橡膠狀聚合物的乳膠粒徑來調整。橡膠狀聚合物的乳膠粒徑可通過在乳化聚合時調整乳化劑的添加方法或水的使用量等來調整,但為了得到優選的範圍需要延長聚合時間而生產率降低,因此可採用如下方法:使粒徑0.1μm左右的橡膠狀聚合物短時間聚合,再採用化學凝集法或物理凝集法使橡膠粒子肥大化。
從抗衝擊性的觀點考慮,接枝共聚物的接枝率優選為10~100質量%,更優選為20~70質量%。接枝率是由凝膠成分(G)與橡膠狀聚合物的含量(RC)採用接枝率(質量%)=[(G-RC)/RC]×100計算得到的值。接枝率表示每單位質量橡膠狀聚合物中含有的通過接枝而鍵合的苯乙烯-丙烯腈共聚物和粒子中內包的苯乙烯-丙烯腈共聚物的量。接枝率例如可通過在乳化接枝聚合時調整單體與橡膠狀聚合物的比例、引髮劑的種類和量、鏈轉移劑量、乳化劑量、聚合溫度、投料方法(一次性/多次/連續)、單體的添加速度等來調整。
從抗衝擊性和成型品外觀的觀點考慮,接枝共聚物的甲苯膨潤度優選為5~20倍。甲苯膨潤度表示橡膠狀聚合物的粒子的交聯度,通過如下方式算出:將接枝共聚物溶解於甲苯,將不溶成分離心或過濾分離,由用甲苯膨潤後的狀態的質量與真空乾燥去除甲苯後的干燥狀態的質量之比算出。甲苯膨潤度例如收到乳化接枝聚合時使用的橡膠狀聚合物的交聯度的影響,可通過在橡膠狀聚合物的乳化聚合時添加引髮劑、乳化劑、調整聚合溫度、添加二乙烯基苯等多官能單體來調整。
SAN樹脂是具有苯乙烯係單體單元和丙烯腈係單體單元的共聚物,例如有苯乙烯-丙烯腈共聚物。
作為SAN樹脂的其他可共聚單體,可使用甲基丙烯酸甲酯等(甲基)丙烯酸酯係單體、丙烯酸丁酯、丙烯酸乙酯等丙烯酸酯係單體、甲基丙烯酸等(甲基)丙烯酸係單體、丙烯酸等丙烯酸係單體、N-苯基馬來酰亞胺等N-取代馬來酰亞胺係單體。
SAN樹脂的構成單元優選為苯乙烯係單體單元60~90質量%、乙烯基氰單體單元10~40質量%,更優選為苯乙烯係單體單元65~80質量%、乙烯基氰單體單元20~35質量%。如果構成單元為上述範圍內,則所得樹脂組合物的衝擊強度與流動性的平衡優異。苯乙烯係單體單元、乙烯基氰單體單元的含量是採用13C-NMR測得的值。
作為SAN樹脂的製造方法,可採用公知方法。例如可採用本體聚合、溶液聚合、懸浮聚合、乳化聚合等來製造。作為反應裝置的操作方法,連續式、分批式(批次式)、半批次式均可適用。從品質和生產率的方面考慮,優選本體聚合或溶液聚合,優選連續式。作為本體聚合或溶液聚合的溶劑,例如有苯、甲苯、乙苯和二甲苯等烷基苯類;丙酮、甲乙酮等酮類;己烷、環己烷等脂肪族烴等。
SAN樹脂的本體聚合或溶液聚合中可使用聚合引髮劑、鏈轉移劑,聚合溫度優選為120~170℃的範圍。聚合引髮劑例如有1,1-二(叔丁基過氧化)環己烷、2,2-二(叔丁基過氧化)丁烷、2,2-二(4,4-二叔丁基過氧化環己基)丙烷、1,1-二(叔戊基過氧化)環己烷等過氧縮醛類、異丙苯過氧化氫、叔丁基過氧化氫等氫過氧化物類、過氧化乙酸叔丁酯、過氧化苯甲酸叔戊酯等烷基過氧化物類、叔丁基過氧化異丙苯、二叔丁基過氧化物、過氧化二異丙苯、二叔己基過氧化物等二烷基過氧化物類、過氧化乙酸叔丁酯、過氧化苯甲酸叔丁酯、叔丁基過氧化異丙基單碳酸酯等過氧化物酯類、叔丁基過氧異丙基碳酸酯、聚醚四(叔丁基過氧碳酸酯)等過氧碳酸酯類、N,N’-偶氮雙(環己烷-1-腈)、N,N’-偶氮雙(2-甲基丁腈)、N,N’-偶氮雙(2,4-二甲基戊腈)、N,N’-偶氮雙[2-(羥甲基)丙腈]等,可使用其中1種或者將2種以上組合使用。鏈轉移劑例如有正辛硫醇、正十二烷基硫醇、叔十二烷基硫醇、α-甲基苯乙烯二聚體、巰基乙酸乙酯、檸檬烯、萜品油烯等。
從SAN樹脂聚合結束後的溶液中去除未反應單體或用於溶液聚合的溶劑等揮發成分的脫揮方法可採用公知方法。例如可使用帶預熱器的真空脫揮槽或帶排氣口的脫揮擠出機。經脫揮的熔融狀態的SAN樹脂可被移送至造粒步驟,由多孔模呈繩狀擠出,採用冷切方式、空中熱切方式、水中熱切方式加工成顆粒狀。
從樹脂組合物的抗衝擊性和成型性的觀點考慮,SAN樹脂的重均分子量優選為5萬~25萬,更優選為7萬~20。具體而言例如為5、6、7、8、9、10、11、12、13、14、15、16、17、18、19或20萬,也可以是任意2個所例示數值之間的範圍內。SAN樹脂的重均分子量是使用凝膠滲透色譜(GPC)在THF溶劑中測定得到的聚苯乙烯換算值,是採用與馬來酰亞胺系共聚物(A)相同的方法測定得到的值。重均分子量可通過調整聚合時鏈轉移劑的種類和量、溶劑濃度、聚合溫度、聚合引髮劑的種類和量來調整。
作為樹脂(B),例如可舉出使用採用乳化聚合法得到的粉末狀ABS樹脂以及採用連續式本體聚合法得到的顆粒狀SAN樹脂這兩種樹脂的方法。另外可舉出將採用乳化聚合法得到的粉末狀ABS樹脂和採用連續本體聚合得到的顆粒狀SAN樹脂用擠出機等熔融混合後,製成顆粒狀的ABS樹脂的方法。
使用擠出機將馬來酰亞胺系共聚物(A)和選自ABS樹脂、ASA樹脂、AES樹脂、SAN樹脂中的至少一種的樹脂(B)熔融混煉的方法可採用公知方法。擠出機可使用公知的裝置,例如可舉出雙螺桿擠出機、單螺桿擠出機、多螺桿擠出機、帶雙軸轉子的連續混煉機等。優選使用雙軸擠出機,更優選被廣泛使用的嚙合式同向雙螺桿擠出機。
作為本發明的實施方式中雙軸擠出機的螺桿,從生產性的觀點來看優選使用螺桿深溝比大的。螺桿深溝比由螺桿外徑(D)和谷徑(d)之比D/d規定。螺桿深溝比在整個螺桿上可以是均勻的,也可以在每個區域中不同。本發明的混煉部中螺桿深溝比是指,混煉熔融混煉的材料的區域中,配置有混合元件溫度最高的區域的螺桿深溝比。本發明的實施方式中,從生產性的觀點考慮,雙軸擠出機的混煉部中螺桿深溝比優選為1.55以上。
熔融混煉優選在抗氧化劑(C)的存在下進行。抗氧化劑優選使用受阻酚系抗氧化劑,也可並用磷系抗氧化劑。
受阻酚系抗氧化劑是在其基本骨架中具有酚性羥基的抗氧化劑。受阻酚系抗氧化劑例如可列舉,十八烷基-3-(3,5-二叔丁基-4-羥基苯基)丙酸酯、亞乙基雙(氧乙烯基)雙〔3-(5-叔丁基-4-羥基-間-甲苯基)丙酸酯〕、3,9-雙[2-〔3-(3-叔丁基-4-羥基-5-甲基苯基)丙酰氧基〕-1,1-二甲基乙基]-2,4,8,10-四氧雜螺[5.5]十一烷、季戊四醇四[3-(3,5-二叔丁基-4-羥基苯基)丙酸酯]、4,6-雙(辛基硫甲基)-鄰甲酚、4,6-雙〔(正十二烷硫基)甲基〕-鄰甲酚、2,4-二甲基-6-(1-甲基十五烷基)酚、四〔亞甲基-3-(3,5-二-叔丁基-4-羥基苯基)丙酸〕甲烷、4,4’-硫代雙(6-叔丁基-3-甲基酚)、1,1,3-三(2-甲基-4-羥基-5-叔丁基苯基)丁烷、4,4’-亞丁基雙(3-甲基-6-叔丁基酚)、雙-[3,3-雙-(4’-羥基-3’-tert―丁基苯基)-丁酸]-乙二醇酯、2-叔丁基-6-(3-叔丁基-2-羥基-5-甲基芐基)-4-甲基苯基丙烯酸酯、2-〔1-(2-羥基-3,5-二-叔戊基苯基)乙基〕-4,6-二-叔戊基苯基丙烯酸酯等。優選為,十八烷基-3-(3,5-二叔丁基-4-羥基苯基)丙酸酯、亞乙基雙(氧乙烯基)雙〔3-(5-叔丁基-4-羥基-間-甲苯基)丙酸酯〕、季戊四醇四[3-(3,5-二叔丁基-4-羥基苯基)丙酸酯]。更優選為,十八烷基-3-(3,5-二叔丁基-4-羥基苯基)丙酸酯。受阻酚系抗氧化劑可以單獨使用也可以組合2種以上來使用。
磷系抗氧化劑是三價磷化合物的亞磷酸酯類。磷系抗氧化劑例如可列舉,6-[3-(3-叔丁基-4-羥基-5-甲基苯基)丙氧基]-2,4,8,10-四-叔丁基苯[d,f][1,3,2]二噁磷雜庚英、3,9-雙(2,6-二-叔丁基-4-甲基苯氧基)-2,4,8,10-四氧雜-3,9-二磷雜螺〔5.5〕十一烷、雙(2,4-枯基苯基)季戊四醇二亞磷酸酯、2,2’-亞甲基雙(4,6-二-叔丁基-1-苯氧基)(2-乙基己氧基)磷、三(2,4-二-叔丁基苯基)亞磷酸酯、雙〔2,4-雙(1,1-二甲基乙基)-6-甲基苯基〕亞磷酸乙基酯、雙(2,4-二-叔丁基苯基)季戊四醇二亞磷酸酯、環辛戊烷四基雙(十八烷基亞磷酸酯)、雙(壬基苯基)季戊四醇二亞磷酸酯、4,4’-亞聯苯基二次磷酸四(2,4-二-叔丁基苯基)、9,10-二氫-9-氧雜-10-磷雜菲-10-氧化物、四(2,4-二-叔丁基-5-甲基苯基)-4,4’-聯苯二亞磷酸酯等。優選為,6-[3-(3-叔丁基-4-羥基-5-甲基苯基)丙氧基]-2,4,8,10-四-叔丁基苯[d,f][1,3,2]二噁磷雜庚英、3,9-雙(2,6-二-叔丁基-4-甲基苯氧基)-2,4,8,10-四氧雜-3,9-二磷雜螺〔5.5〕十一烷、雙(2,4-枯基苯基)季戊四醇二亞磷酸酯、2,2’-亞甲基雙(4,6-二-叔丁基-1-苯氧基)(2-乙基己氧基)磷、三(2,4-二-叔丁基苯基)亞磷酸酯、雙(2,4-二-叔丁基苯基)季戊四醇二亞磷酸酯。更優選為,6-[3-(3-叔丁基-4-羥基-5-甲基苯基)丙氧基]-2,4,8,10-四-叔丁基苯[d,f][1,3,2]二噁磷雜庚英、雙(2,4-枯基苯基)季戊四醇二亞磷酸酯、三(2,4-二-叔丁基苯基)亞磷酸酯、雙(2,4-二-叔丁基苯基)季戊四醇二亞磷酸酯,進一步優選為6-[3-(3-叔丁基-4-羥基-5-甲基苯基)丙氧基]-2,4,8,10-四-叔丁基苯[d,f][1,3,2]二噁磷雜庚英、雙(2,4-枯基苯基)季戊四醇二亞磷酸酯、雙(2,4-二-叔丁基苯基)季戊四醇二亞磷酸酯。磷系抗氧化劑可以單獨使用也可以組合2種以上來使用。
混煉部的氣缸溫度為290℃以上時,作為抗氧化劑(C)更有選使用游離基清除劑。作為游離基清除劑可列舉,2-叔丁基-6-(3'-叔丁基-5'-甲基-2'-羥基芐基)-4-甲基苯基丙烯酸酯、2,4ー二叔戊基ー6-[1-(3,5-二叔戊基-2-羥基苯基)乙基]苯基丙烯酸酯。
相對於馬來酰亞胺系共聚物(A)和樹脂(B)的總計100質量份,抗氧化劑(C)的添加量優選為0.1~0.5質量份,更優選為0.3~0.5質量份。具體而言例如為0.1、0.2、0.3、0.4或0.5質量份,也可以是任意2個所例示數值之間的範圍內。
將馬來酰亞胺系共聚物(A)和樹脂(B)的總量作為100質量%時,樹脂組合物中馬來酰亞胺系共聚物(A)的含量優選為5~45質量%,更優選為7~35質量%,進一步優選為10~30質量%。具體而言例如為5、10、15、20、21、22、23、24、25、26、27、28、29、30、35、40或45質量%,也可以是任意2個所例示數值之間的範圍內。馬來酰亞胺系共聚物(A)的含量過少,則樹脂組合物的耐熱性提高不充分。過多則流動性降低,成型性變差。應予說明,包含於樹脂組合物的樹脂實質上可以僅是馬來酰亞胺系共聚物(A)和樹脂(B)。
耐熱性樹脂組合物的製造中在不損害本發明效果的範圍內可以含有其他樹脂成分、抗衝擊改性劑、流動性改性劑、硬度改性劑、抗氧化劑、無機填充劑、消光劑、阻燃劑、阻燃助劑、防滴劑、滑動性賦予劑、放熱劑、電磁波吸收劑、增塑劑、潤滑劑、脫模劑、紫外線吸收劑、光穩定劑、抗菌劑、抗黴劑、抗靜電劑、炭黑、氧化鈦、顏料、染料等。
[實施例]
以下使用實施例對詳細內容進行說明,但本發明並不限定於以下實施例。
<馬來酰亞胺系共聚物(A-1)的製造例>
採用以下方法製造馬來酰亞胺系共聚物(A-1)。
向具備攪拌機的容積約120升的高壓釜中投入苯乙烯62質量份、馬來酸酐11質量份、2、4-二苯基-4-甲基-1-戊烯0.2質量份、甲乙酮31質量份,用氮氣對系內進行置換後,升溫至92℃,歷時7小時連續添加將馬來酸酐28質量份和過氧化-2-乙基己酸叔丁酯0.19質量份溶解於甲乙酮110質量份的溶液。添加之後升溫至120℃,使其反應30分鐘完成聚合。其後向聚合液加入苯胺35質量份、三乙胺0.6質量份在140℃反應7小時。將反應結束後的酰亞胺化反應液投入於排氣式擠出機,除去揮發成分得到了約3mm的顆粒狀的馬來酰亞胺系共聚物(A-1)。A-1的苯乙烯單元為48質量%、N-苯基馬來酰亞胺單元為51質量%、馬來酸酐單元為1質量%,重均分子量Mw為13萬,玻璃化轉變溫度Tmg為202℃。另外,在260℃、剪切速度120/sec下的熔融黏度為3420Pa・s,在280℃、剪切速度120/sec下的熔融黏度為1780Pa・s。
<馬來酰亞胺系共聚物(A-2~A-8)的製造例>
使用篩網式微粉碎機將馬來酰亞胺系共聚物(A-1)粉碎為粉末狀。用篩網直徑1mm,改變旋轉數得到了平均粒子直徑不同的A-2~A-5。A-6使用了除去A-4的篩子(850μm)上的。A-7僅使用了篩子(75μm)下的。A-8使用了混合了A-2 80質量%和A-6的篩子(1000μm)上 10質量%的。粉末的平均粒子直徑使用JIS Z 8801的試驗篩子測定。使用網孔為1000、850、500、355、250、150、106、75、50μm的篩子,將噴灑抗靜電劑混合的馬來酰亞胺系共聚物的粉末50g放入網孔最大的篩子中蓋上蓋子,將篩子置於搖床上,搖晃20分鐘。搖晃後,測定包含粉末的各篩子的質量,減去篩子的質量,即可計算出篩子上的粒度分佈。從粒度分佈的結果來看,質量從網孔大的開始依次相加,平均粒子直徑是從夾住累積質量50%的兩點網孔(粒子直徑)和50%的交點求出的粒子直徑。應予說明,因為用本測定法無法測定A-7的平均粒子直徑,因此為小於75μm,但通過激光衍射/散射法獲得的平均粒子直徑為37μm。
<馬來酰亞胺系共聚物(A-9)的製造例>
採用以下方法製造馬來酰亞胺系共聚物(A-9)。
向具備攪拌機的容積約120升的高壓釜中投入苯乙烯42質量份、丙烯腈10質量份、馬來酸酐4質量份、2、4-二苯基-4-甲基-1-戊烯0.03質量份、甲乙酮27質量份,用氮氣對氣相部進行置換後,攪拌同時歷時40分鐘升溫至92℃。升溫後維持92℃,歷時4.5小時連續添加將馬來酸酐21質量份和過氧化-2-乙基己酸叔丁酯0.15質量份溶解於甲乙酮85質量份的溶液以及苯乙烯20質量份。進一步,添加完馬來酸酐之後,歷時30分鐘連續添加將過氧化-2-乙基己酸叔丁酯0.02質量份溶解於甲乙酮9質量份的溶液以及苯乙烯3質量份。添加之後升溫至120℃,使其反應30分鐘完成聚合。後向聚合液中加入苯胺23質量份、三乙胺0.4質量份在140℃反應7小時。將反應結束後的酰亞胺化反應液投入於排氣式擠出機,除去揮發成分得到了顆粒狀的馬來酰亞胺系共聚物(A-9)進一步,與(A-2)~(A-8)相同的方式,使用篩網式微粉碎機將馬來酰亞胺系共聚物(A-9)粉碎為粉末狀。(A-9)的苯乙烯單元為52質量%、丙烯腈單元為8質量%、N-苯基馬來酰亞胺單元為39質量%、馬來酸酐單元為1質量%,重均分子量Mw為14萬、玻璃化轉變溫度Tmg為177℃。另外,在260℃、剪切速度120/sec下的熔融黏度為1660Pa・s,在280℃、剪切速度120/sec下的熔融黏度為710Pa・s。
<ABS樹脂(B-1)>
用市售的ABS樹脂(電化株式會社制 DENKAABS GR-3500)。
<SAN樹脂(B-2)>
使用市售的SAN樹脂(電化株式會社制 DENKAAS AS-EXS)。
<實施例・比較例>
使用擠出機按表1所示的配合以及條件將馬來酰亞胺系共聚物、ABS樹脂熔融混煉,進行了耐熱性樹脂組合物的製造。擠出機使用了L/D=48、螺桿深溝比1.56的雙螺桿擠出機(東芝機械株式會社制 TEM-26SX)。應予說明,作為抗氧化劑,相對於馬來酰亞胺系共聚物(A)和樹脂(B)的總量100質量份,混合了下述(C-1)0.3質量份(C-2)0.15質量份。評價結果示於表1。
(C-1)季戊四醇四[3-(3,5-二叔丁基-4-羥基苯基)丙酸酯](BASF日本株式會社製造 Irganox1010)
(C-2):三(2,4-二-叔丁基苯基)亞磷酸酯(BASF日本株式會社製造 Irganox168)
(熔體流動速率)
熔體流動速率基於JIS K7210在220℃以98N負載進行測定。
(維卡軟化溫度)
維卡軟化點基於JIS K7206,採用50法(負載50N、升溫速度50℃/小時)使用10mm×10mm、厚4mm的實驗片進行測定。應予說明,測定設備使用東洋精機製作所社制的HDT&VSPT試驗裝置。
(夏比衝擊強度)
夏比衝擊強度基於JIS K7111-1,使用帶缺口實驗片,打擊方向採用沿邊進行測定。應予說明,測定設備使用東洋精機製作所社制的數顯衝擊試驗機。
(分散等級)
使用射出成型機(東芝機械株式會社製造,IS-50EP),將在氣缸溫度220℃、模具溫度60℃的成型條件下成型的長90mm、寬55mm、厚2mm的鏡板,肉眼觀察馬來酰亞胺系共聚物的分散狀態。若馬來酰亞胺系共聚物的分散狀態差,則在成型品的表面觀察到沿樹脂流動的條紋。
分散等級5:外觀非常乾淨沒有瑕疵
分散等級4:可以看到細微的條紋
分散等級3:可以看到細微的條紋
分散等級2:存在導致明顯不良外觀的條紋。
分散等級1:有明顯被認為整體外觀較差的條紋。
由表1的結果可知,通過使用平均粒子直徑為75μm以上、1000μm的篩子上小於5質量%的粉狀的馬來酰亞胺系共聚物,可得到馬來酰亞胺系共聚物的分散性優異的耐熱性樹脂組合物。
應予說明,雖然沒有示於表1,但比較例2在製造耐熱性樹脂組合物時,馬來酰亞胺系共聚物在擠出機的供給區堵塞二工作效率差。
[產業上的可利用性]
根據本發明的馬來酰亞胺系共聚物,可以得到生產率高、馬來酰亞胺系共聚物的分散性優異的耐熱性樹脂組合物,其成型品的外觀也優異。
圖1是本發明的實施方式所涉及的雙軸擠出裝置的螺桿構成圖。
Claims (4)
- 一種馬來酰亞胺系共聚物(A),其平均粒子直徑為75μm以上,在1000μm的篩子上小於5質量%的粉狀的馬來酰亞胺系共聚物(A)。
- 如請求項1所述的馬來酰亞胺系共聚物(A),其玻璃化轉變溫度為170~210℃。
- 如請求項1或2所述的馬來酰亞胺系共聚物(A),其在260℃、剪切速度120/sec下的熔融黏度為1000Pa・s以上。
- 一種耐熱性樹脂組合物的製造方法, 使用擠出機將請求項1~3中任一項所述的馬來酰亞胺系共聚物(A)和選自ABS樹脂、ASA樹脂、AES樹脂、SAN樹脂中的至少一種的樹脂(B)熔融混煉。
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