TW201803922A - 熱塑性樹脂薄膜與其製造方法、及積層體 - Google Patents
熱塑性樹脂薄膜與其製造方法、及積層體 Download PDFInfo
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Abstract
提供一種熱塑性樹脂薄膜,其係至少一側的薄膜面為印刷性優異,內部霧度夠小,且能夠展現良好的消光外觀。本發明之熱塑性樹脂薄膜係由熱塑性樹脂組成物(C)所構成且至少一側的薄膜面滿足下式(1)及(2),該熱塑性樹脂組成物(C)包含至少1種的熱塑性樹脂(R)、及體積平均粒徑為0.5~15μm且與熱塑性樹脂(R)之折射率差為0.02以上的微粒子(P)。GL≧60…(1)、GL-35≦GH≦GL-10…(2)(其中,上式(1)、(2)中,GL係在20℃的60°光澤度(%),GH係以比熱塑性樹脂組成物(C)的玻璃轉移溫度高10℃的溫度加熱30分鐘之後,冷卻至20℃之後的60°光澤度(%))。
Description
本發明係有關於熱塑性樹脂薄膜與其製造方法。本發明還有關於使用了此熱塑性樹脂薄膜的印刷樹脂薄膜、消光樹脂薄膜與其製造方法、裝飾用薄膜、建材用薄膜、積層薄膜、及積層體。
於汽車的內裝構件及外裝構件、家庭用電器的外裝構件、家具的外裝構件、以及壁材等之用途,係有使用於具有表面無光澤的無光風格(消光)之外觀的樹脂薄膜(消光樹脂薄膜)的情形。進而,按照用途等,係有為了高級感及深度感等之設計性的賦予或者裝飾性的賦予等,而於消光樹脂薄膜的至少一側的薄膜面施行印刷的情形。此情形,對於消光樹脂薄膜,係謀求良好的消光外觀與良好的印刷性。
以往,就消光樹脂薄膜的製造方法而言,可舉出將一種於透明性樹脂中分散具有消光效果之微粒子(消光
劑)的樹脂組成物成形成薄膜狀的方法(專利文獻1~4等)、及將不含/或者含有具有消光效果之微粒子(消光劑)的樹脂(組成物)成形成薄膜狀之後,壓印於表面具有微細之凹凸的壓花輥,而對表面賦予微細之凹凸的方法(專利文獻5、6等)。
再者,於本說明書中,「樹脂(組成物)」係意味樹脂或樹脂組成物。
專利文獻1中揭示一種將包含熱塑性聚合物、含橡膠之聚合物及消光劑的樹脂組成物進行薄膜化而獲得之消光樹脂薄膜(請求項1)。就消光劑而言,係舉出有粒徑1~20μm之具有交聯結構的樹脂微粒子、雲母微粒子、及滑石微粒子(請求項2)。專利文獻1中,作為消光樹脂薄膜的製造方法而舉出有T字模法、充氣法、及壓延(calendaring)法(第0028段)。
專利文獻2中揭示一種作為要施行印刷之消光樹脂薄膜,而將包含熱塑性聚合物、含橡膠之聚合物及消光劑的樹脂組成物進行薄膜化而獲得的消光樹脂薄膜(請求項1、10)。就消光劑而言,係舉出有平均粒徑0.5~20μm之無機粒子及/或有機交聯粒子、及含氫氧基之聚合物(請求項2、3)。專利文獻2中記載著藉由上述構成,而可提供一種具有高級感及深度感優異的表面消光外觀且不回復光澤的消光樹脂薄膜(第0069段)。
一般而言,無關於作為消光劑之微粒子的使用之有無,消光樹脂薄膜係有因其表面凹凸而印刷性低且容易產生印刷遺漏的傾向(請參照專利文獻3的第0006段)。如此地,一般而言,於消光樹脂薄膜中,消光外觀與印刷性係互相違背之特性。若印刷遺漏產生,則無法獲得所期望的印刷效果(設計性或者裝飾性等之賦予),製造之收率也就會降低。
可是,於藉由熔融擠出之熱塑性樹脂薄膜的製造方法中,為了薄膜的厚度控制及薄膜的表面外觀提升,一般係將原料之樹脂(組成物)熔融而從T字模擠出成薄膜狀之後,以一對冷卻輥來挾持使其硬化。然而,在由分散了作為消光劑之微粒子的樹脂組成物所構成之消光樹脂薄膜,為了要獲得消光外觀,而需要使作為消光劑之微粒子由薄膜面突出。但是,於消光樹脂薄膜的製造方法中,若是實施將分散了作為消光劑之微粒子的樹脂組成物擠出成薄膜狀且以一對冷卻輥來挾持之步驟,則微粒子被擠壓進薄膜內部,會有消光外觀會受損之顧慮。此外,不實施將分散了作為消光劑之微粒子的樹脂組成物擠出成薄膜狀且以一對冷卻輥來挾持之步驟的情形,則薄膜的厚度控制困難,會有所獲得之薄膜的厚度不均變大的傾向。此外,會有於薄膜面發生條紋等而薄膜的表面外觀受損之顧慮。
專利文獻3中揭示了薄膜表背的60°表面光澤度的差為5%以上之消光樹脂薄膜(請求項1)。於專利文獻3中,就原料的樹脂組成物而言,係舉出有一種包含熱塑性聚合物、含橡膠之聚合物及消光劑的樹脂組成物(請求項5)。就消光劑而言,係舉出有含氫氧基之聚合物(請求項6)。專利文獻3中,係揭示了將樹脂組成物熔融擠出之後,以鏡面輥、與由橡膠輥或附壓紋的輥所構成之非鏡面輥來挾持熔融物的方法,作為消光樹脂薄膜之製造方法(請求項13、14)。在專利文獻3所記載的製造方法,係以一對的輥來挾持熔融物,所以可抑制厚度不均及條紋的發生。在專利文獻3所記載的方法,係鏡面會被轉印在密接於鏡面輥之薄膜面上,所以該面的表面光澤度高,且可藉由在該面施行印刷而減少印刷遺漏(專利文獻3的第0090段)。另一方面,密接於非鏡面輥之薄膜面的表面光澤度低,且可呈現消光外觀(專利文獻3的第0090段)。
專利文獻4中揭示了一種擠出之墊片(mat sheet)的製造方法,其係將分散了微粒子之樹脂組成物以熔融狀態由模具擠出,並以一方為高剛性之金屬輥而另一方為於外周部具備了金屬製薄膜的彈性輥之一對冷卻輥來夾住而進行成形(請求項1)。
在專利文獻4所記載的製造方法,係以一對冷卻輥來挾持熔融物,所以可抑制厚度不均及條紋的發生(專利文獻4的第0009段)。專利文獻4中記載了,藉由金屬
彈性輥的使用,而抑制作為消光劑之微粒子被擠壓進透明性樹脂中,且抑制消光外觀受損(專利文獻4的第0011段)。然而,金屬彈性輥的表面通常藉由鏡面處理而為平滑面,難以使作為消光劑之微粒子突出於薄膜面,並無法說消光外觀的展現為充分的。
專利文獻5、6中揭示了一種消光樹脂薄膜的製造方法,其係將透明性樹脂由T字模熔融擠出,並以由橡膠輥或金屬彈性輥所構成之第1冷卻輥、與由在外周面形成有凹凸形狀的金屬輥所構成之第2冷卻輥來挾持熔融物,而轉印第2冷卻輥的凹凸形狀(專利文獻5的請求項1、專利文獻6的請求項1)。在專利文獻5、6,並不使用作為消光劑之微粒子,係將第2冷卻輥的凹凸形狀轉印於熔融物的表面,以於薄膜面獲得消光外觀。
專利文獻1~6所記載的以往之技術,係任一者皆為於薄膜之製造時以某種的手段而對薄膜表面賦予凹凸之物,與在製造被一度冷卻硬化的薄膜之後,藉由加熱處理而使良好的消光外觀展現之技術無關。
此外,一般而言,在使用了作為消光劑之微粒子的熱塑性樹脂薄膜,係因微粒子的存在,而有內部霧度變大的傾向。內部霧度過大時,於印刷後對組件等貼附薄膜之際的定位會變得困難。所以,於使用了作為消光劑之微粒子的熱塑性樹脂薄膜中亦較佳為內部霧度要夠小。
再者,於本說明書中,「內部霧度」係排除了表面及背面之凹凸的影響之霧度,以後述之方法進行測定。
專利文獻1 日本特開平06-073199號公報(專利第3307989號公報)
專利文獻2 日本特開平10-237261號公報
專利文獻3 日本特開2002-361712號公報(專利第3964234號公報)
專利文獻4 日本特開2009-143174號公報(專利第5108487號公報)
專利文獻5 日本特開2009-202382號公報(專利第5118506號公報)
專利文獻6 日本特開2009-196327號公報(專利第5143587號公報)
本發明係鑒於上述狀況而進行者,係以提供一種熱塑性樹脂薄膜與其製造方法為目的,該熱塑性樹脂薄膜係至少一側的薄膜面為印刷性優異,內部霧度夠小,且能夠展現良好的消光外觀。
再者,本發明之熱塑性樹脂薄膜,係可於薄膜製造後藉由加熱處理而展現良好的消光外觀。
本發明係提供以下的熱塑性樹脂薄膜與其製造方法、印刷樹脂薄膜、消光樹脂薄膜與其製造方法、裝飾用薄膜、建材用薄膜、積層薄膜、及積層體。
本發明之熱塑性樹脂薄膜係由熱塑性樹脂組成物(C)所構成,且至少一側的薄膜面滿足下式(1)及(2),該熱塑性樹脂組成物(C)包含至少1種的熱塑性樹脂(R)、及體積平均粒徑為0.5~15μm且與熱塑性樹脂(R)之折射率差為0.02以上的微粒子(P)。
GL≧60…(1),GL-35≦GH≦GL-10…(2)
(其中,上式(1)、(2)中,GL係在20℃的60°光澤度(%),GH係以比熱塑性樹脂組成物(C)的玻璃轉移溫度高10℃的溫度加熱30分鐘之後,冷卻至20℃之後的60°光澤度(%)。)
本發明之熱塑性樹脂薄膜較佳為進一步滿足下式(3-1)。
10/d≦W≦30/d…(3-1)
(其中,上式(3-1)中,d係微粒子(P)的體積平均粒徑(μm),W係熱塑性樹脂薄膜中之微粒子(P)的含量(質量%)。)
於本發明之熱塑性樹脂薄膜中,較佳為外部霧度小於內部霧度。
熱塑性樹脂(R)較佳為包含甲基丙烯酸系樹脂。
熱塑性樹脂(R)較佳為包含丙烯酸系多層結構聚合物粒子(A),其至少1層之內層為主成分單體單元係具有碳數1~8的烷基之丙烯酸烷酯單體單元及/或共軛二烯系單體單元的交聯彈性聚合物層,且最外層為主成分單體單元係具有碳數1~8的烷基之甲基丙烯酸烷酯單體單元的熱塑性聚合物層。
丙烯酸系多層結構聚合物粒子(A)較佳為包含3層結構聚合物粒子(AX),其從中心側起包含:第1層,係包含含有30~98.99質量%之甲基丙烯酸甲酯單元、1~70質量%之具有碳數1~8的烷基之丙烯酸烷酯單元及0.01~2質量%之多官能性單體單元的交聯聚合物層;第2層,係包含含有70~99.9質量%之具有碳數1~8的烷基之丙烯酸烷酯單元、0~30質量%之甲基丙烯酸甲酯單元及0.1~5質量%之多官能性單體單元的交聯彈性聚合物層;及第3層,係包含含有80~99質量%之甲基丙烯酸甲酯單元、及1~20質量%之具有碳數1~8的烷基之丙烯酸烷酯單元的硬質熱塑性聚合物層。
丙烯酸系多層結構聚合物粒子(A)之粒徑較佳為0.05~0.20μm。
熱塑性樹脂(R)較佳為包含甲基丙烯酸系樹脂(B),其包含80質量%以上的甲基丙烯酸甲酯單元,且極限黏度為0.3~1.0dl/g。
本發明之印刷樹脂薄膜,係於上述的本發明之熱塑性樹脂薄膜的至少一側的薄膜面施行有印刷者。
本發明之消光樹脂薄膜,係上述的本發明之熱塑性樹脂薄膜或上述的本發明之印刷樹脂薄膜被加熱處理所獲得者。
本發明之裝飾用薄膜包含上述的本發明之熱塑性樹脂薄膜、上述的本發明之印刷樹脂薄膜、或上述的本發明之消光樹脂薄膜。
本發明之建材用薄膜包含上述的本發明之熱塑性樹脂薄膜、上述的本發明之印刷樹脂薄膜、或上述的本發明之消光樹脂薄膜。
本發明之積層薄膜包含上述的本發明之熱塑性樹脂薄膜、上述的本發明之印刷樹脂薄膜、或上述的本發明之消光樹脂薄膜。
本發明之積層體係於基材上積層有上述的本發明之熱塑性樹脂薄膜、上述的本發明之印刷樹脂薄膜、上述的本發明之消光樹脂薄膜、或上述的本發明之積層薄膜。
本發明之熱塑性樹脂薄膜的製造方法係上述的本發明之熱塑性樹脂薄膜的製造方法,具有將熱塑性樹脂組成物(C)由T字模熔融擠出成薄膜狀之步驟、與將擠出成薄膜狀之熔融物以雙方為金屬剛體輥之一對冷卻輥、或是一方為金屬剛體輥而另一方為金屬彈性輥之一對冷卻輥來挾持之步驟。
於本發明之熱塑性樹脂薄膜的製造方法中,較佳為前述一對冷卻輥之中,將一方的冷卻輥之表面溫度設為T1,將另一方的冷卻輥之表面溫度設為T2(其中,T2≧T1。),將熱塑性樹脂組成物(C)的玻璃轉移溫度設為TgC時,滿足下式(4)。
10≦|TgC-T2|≦40…(4)
本發明之消光樹脂薄膜的製造方法,係將上述的本發明之熱塑性樹脂薄膜進行加熱處理。此外,本發明之消光樹脂薄膜的製造方法,係於上述的本發明之熱塑性樹脂薄膜的至少一側的薄膜面施行印刷,進行加熱處理。
通常,厚度為5~250μm的情形,係主要被分類為「薄膜」,而比250μm厚的情形,則主要被分類為「薄片」,但在本說明書,並不明確地區別薄膜與薄片,將二者一起稱為「薄膜」。
於本說明書中,只要無特別述明,則熱塑性樹脂(R)的折射率係設為以以下的方法測定之值。
利用壓製成形而將熱塑性樹脂(R)加工為縱3cm×橫3cm×厚度3mm的薄片,使用Shimadzu Device Corporation製「Kalnew精密折射計KPR-200」,於23℃以波長587.6nm(d線)測定折射率。
於本說明書中,只要無特別述明,則微粒子(P)的折射率係設為使用顯微鏡而藉由浸漬法(貝克線法)所測定之值。
於本說明書中,只要無特別述明,則微粒子(P)的體積平均粒徑係設為以以下的方法所測定之值。
使用微型追蹤粒徑分布測定裝置(NIKKISO CO.,LTD.製「MK-3300」),藉由雷射繞射.散射法而測定微粒子(P)的體積平均粒徑。
於本說明書中,只要無特別述明,則薄膜之整體霧度、內部霧度、及外部霧度係以以下的方法測定之值。
依據JIS K 7136而測定測定對象之薄膜的整體霧度(如通常之霧度測定)。此外,準備2張厚度為相同程度且霧度為0.2以下之輔助測定用的透明樹脂薄膜。將測定對象之薄膜的兩面以水滴弄濕之後,使輔助測定用的薄膜分別對於各面密接。可藉此而消除測定對象之薄膜的表面凹凸之影響。在此狀態依據JIS K 7136而進行霧
度測定,並將所得之值當作內部霧度。求出上述整體霧度與上述內部霧度之差分作為外部霧度。
薄膜的整體霧度較佳為10~20%,更佳為13~16%。內部霧度較佳為6~13%,更佳為8~10%,進一步較佳為8~9%。外部霧度較佳為2~8%,更佳為3~7%。
於本說明書中,只要無特別述明,則「樹脂(組成物)的玻璃轉移溫度(Tg)」係設為以以下的方法測定之值。
依據JIS K 7121而測定樹脂(組成物)的玻璃轉移溫度(Tg)。使用示差掃描量熱測定裝置(島津製作所公司製「DSC-50」),將試樣一旦升溫至230℃而冷卻至室溫之後,再度以由室溫至230℃以10℃/分鐘之升溫速度使其升溫之條件來測定DSC曲線。將由所得之DSC曲線所求出的中點當作玻璃轉移溫度(Tg)。再者,自室溫至230℃之範圍中出現複數中點的情形,係將其中點之中來自含量最多之樹脂的中點當作玻璃轉移溫度(Tg)。
於本說明書中,只要無特別述明,則熱塑性樹脂薄膜的「gloss(光澤度)」為60°光澤度,係設為以以下的方法測定之值。
就光澤度計而言,係使用日本電色工業公司製「VG7000」。起初,於熱塑性樹脂薄膜上,針對兩薄膜面分別依據JIS Z 8741的光澤度測定,以20℃、以60°反射條件來測定光澤度。此值為GL。
進一步使用烘箱,而將薄膜以Tg+10℃的溫度加熱30分鐘,並自然冷卻至20℃之後,針對兩薄膜面與上述同樣地進行而再度測定光澤度。此值為GH。
於本說明書中,只要無特別述明,則包含丙烯酸系多層結構聚合物粒子(A)之乳膠中的丙烯酸系多層結構聚合物粒子(A)之粒徑,係設為使用堀場製作所股份有限公司製的「LA-300」而測定之值。
於薄膜製造的過程中,有丙烯酸系多層結構聚合物粒子(A)的非交聯之最外層等熔融而形成基質(matrix)的情形。此情形,薄膜中之丙烯酸系多層結構聚合物粒子(A)的粒徑會變得比原料的聚合物粒子之粒徑還小。
於本說明書中,只要無特別述明,則薄膜中之丙烯酸系多層結構聚合物粒子(A)的粒徑係設為藉由利用穿透式電子顯微鏡(TEM)之截面觀察而求出者。具體而言,係切下薄膜的一部分,在凍結條件下利用薄片切片機於厚度方向進行切斷,並將所得之切片以氧化釕水溶液染色之後,以TEM觀察經染色之橡膠粒子的截面。將100個粒子的平均值當作丙烯酸系多層結構聚合物粒子(A)之粒徑。
若根據本發明,則可提供一種熱塑性樹脂薄膜與其製造方法,該熱塑性樹脂薄膜係至少一側的面為印刷性優異,內部霧度夠小,且能夠展現良好的消光外觀。
再者,本發明之熱塑性樹脂薄膜係能夠於薄膜製造後藉由加熱處理而展現良好的消光外觀者。
1‧‧‧薄膜製造裝置
110‧‧‧擠出成形手段
111‧‧‧原料投入部
112‧‧‧螺旋部
113‧‧‧T字模
113A‧‧‧吐出口
120‧‧‧冷卻輥單元
121‧‧‧第1冷卻輥
122‧‧‧第2冷卻輥
123‧‧‧第3冷卻輥
124‧‧‧第4冷卻輥
210‧‧‧樹脂薄膜
210M‧‧‧樹脂組成物
R1‧‧‧第1製造室
R2‧‧‧第2製造室
圖1係顯示有關本發明之一實施形態的薄膜製造裝置的概略圖。
本發明之熱塑性樹脂薄膜,係於薄膜製造後藉由加熱處理而展現良好的消光外觀者。
再者,本發明之熱塑性樹脂薄膜可為未拉伸薄膜,亦可為拉伸薄膜。只要無特別述明,則薄膜係意味未拉伸薄膜。
以下,「熱塑性樹脂薄膜」係有簡略為「樹脂薄膜」或「薄膜」之情形。
本發明之熱塑性樹脂薄膜包含熱塑性樹脂(R)、與一般被稱為消光劑或光擴散劑之微粒子(P)。
熱塑性樹脂(R)係可作為構成本發明之熱塑性樹脂薄膜的熱塑性樹脂組成物(C)之主成分,例如較佳為構成熱塑性樹脂薄膜的50質量%以上,更佳為80質量%以上,特佳為90質量%以上之熱塑性樹脂。
一般而言,在包含作為消光劑之微粒子(P)的熱塑性樹脂薄膜,係被認為為了得到消光外觀,而需要使作為消光劑之微粒子(P)由薄膜面充分地突出,但因此而會有印刷性降低之情形。
在本發明,於薄膜的製造階段中,並不需要具有良好的消光外觀,作為消光劑之微粒子(P)不需要由薄膜面突出。在本發明,可於薄膜製造後,藉由加熱處理使薄膜軟化,以使作為消光劑之微粒子(P)突出於薄膜面,而展現良好的消光外觀。
再者,一般而言,薄膜的表背並不明確。所以,於本說明書中,「薄膜面」係薄膜的表面或背面。
於本發明中,微粒子(P)係體積平均粒徑為0.5~15μm,與熱塑性樹脂(R)之折射率差為0.02以上,較佳為0.03以上,更佳為0.04以上。微粒子(P)的體積平均粒徑小於0.5μm時,係無法於將熱塑性樹脂薄膜加熱處理之後良好地得到由微粒子(P)所致之光擴散效果,難以展現良好的消光外觀。微粒子(P)的體積平均粒徑超過15μm時,熱塑性樹脂薄膜的內部霧度變大,會有於印刷後將薄膜貼附於組件等之際的定位變困難之顧慮。此外,會有於微粒子(P)的凝集物產生之時,成為外觀上的缺陷之顧慮。熱塑性樹脂(R)與微粒子(P)之折射率差小於0.02時,係無法於加熱處理後充分地得到由微粒子(P)所致之光擴散效果,而難以展現良好的消光外觀。藉由使用體積平均粒徑為0.5~15μm且與熱塑性樹脂
(R)之折射率差為0.02以上的微粒子(P),而可於加熱處理後良好地得到由微粒子(P)所致之光擴散效果,可得到良好的消光外觀。微粒子(P)較佳為體積平均粒徑為0.5~10μm,更佳為3~7μm,較佳為與熱塑性樹脂(R)之折射率差為0.03以上。
於本發明中,微粒子(P)的長寬比較佳為5以上,更佳為10以上,特佳為20以上。藉由使用具有該長寬比的微粒子(P),而可於加熱處理後良好地得到由微粒子(P)所致之光擴散效果,可得到良好的消光外觀。長寬比的上限並未特別限定,通常為200左右。
1個微粒子中的「長寬比」,係以(最大長徑/厚度)所定義之表示微粒子的形狀之指數。
通常,微粒子(P)係包含長寬比具有分布之複數的微粒子。
於本說明書中,只要無特別述明,則長寬比係設為如以下地進行測定而得到之值。以電子顯微鏡觀察100個以上的微粒子,並於所得之顯微鏡像中求出各個微粒子的長寬比,得到顯示微粒子的個數(縱軸)與長寬比(橫軸)之關係的分布。將該分布之中個數成為波峰之長寬比當作中心,而求出包括全微粒子之50%的長寬比之範圍來作為長寬比的數據。
長寬比的數據亦可採用型錄值(catalogue value)。
本發明之熱塑性樹脂薄膜,係至少一側的薄膜面滿足下式(1)、(2)。
GL≧60…(1),GL-35≦GH≦GL-10…(2)
(其中,上式(1)、(2)中,GL係在20℃的60°光澤度(%),GH係以熱塑性樹脂組成物(C)的玻璃轉移溫度(Tg)+10℃的溫度加熱30分鐘之後,冷卻至20℃之後的60°光澤度(%)。)
GL係在常溫(加熱處理前)之光澤性的指標。另一方面,GH係加熱處理後之光澤性及消光性的指標。
於本說明書中,「用於GH測定之加熱處理」,只要無特別述明,則設為使用烘箱(Yamato Scientific Co.,Ltd.公司製「safety精密恆溫器DF411S」)進行者。
薄膜面滿足上式(1)之情形(薄膜面的GL為60%以上之情形),此薄膜面係在常溫具有高光澤,且表面平滑性高,因此印刷遺漏被抑制,且具有良好的印刷性。薄膜面的GL小於60%之情形,此薄膜面在常溫光澤低,且微粒子(P)突出於薄膜面的可能性高,會有不具有良好的印刷性之顧慮。若薄膜面的GL過高,則於加熱處理後突出於薄膜面之微粒子(P)的量會不充分,會有無法得到良好的消光外觀之顧慮。由於至少一側的薄膜面在常溫具有高光澤而具有良好的印刷性,且可於加熱處理後可獲得良好的消光外觀,至少一側的薄膜面之GL較佳為
60~99%,更佳為70~99%,進一步較佳為80~99%,特佳為90~99%。
再者,一對的薄膜面之GL值不同的情形,從能夠進行更高品質的印刷來看,較佳為於GL值較高的面施行印刷。
以玻璃轉移溫度(Tg)+10℃的溫度加熱30分鐘之後的60°光澤度之降低小於10%的情形(GL-GH<10),難以於加熱處理後使其展現良好的消光外觀。另一方面,以玻璃轉移溫度(Tg)+10℃的溫度加熱30分鐘之後的60°光澤度之降低超過35%的情形(GL-GH>35),於加熱處理後會展現消光外觀,但突出於薄膜面之微粒子(P)的量多,會有表面外觀惡化之顧慮。薄膜面係滿足上式(2)之情形(10≦GL-GH≦35),可於加熱處理後得到良好的消光外觀與良好的表面外觀。
可藉由使用體積平均粒徑為0.5~15μm,較佳為0.5~10μm,且與熱塑性樹脂(R)之折射率差為0.02以上的微粒子(P),並且至少一側的薄膜面係滿足上式(1)、(2),而提供一種熱塑性樹脂薄膜,其係至少一側的薄膜面為高光澤且印刷性優異,內部霧度夠小,且能夠於加熱處理後展現良好的消光外觀。
於本發明中,微粒子(P)的體積平均粒徑d(μm)及熱塑性樹脂薄膜中之微粒子(P)的含量W(質量%)較佳為滿
足下式(3-1),更佳為滿足下式(3-2),進一步較佳為滿足下式(3-3)。
10/d≦W≦30/d…(3-1)
10/d≦W≦20/d…(3-2)
13/d≦W≦17/d…(3-3)
微粒子(P)的含量W過少(小於10/d)時,熱塑性樹脂薄膜無法於加熱處理後良好地得到由微粒子(P)所致之光擴散效果,會有變得難以展現充分的消光外觀之顧慮。微粒子(P)的含量W過多(超過30/d)時,在製造熱塑性樹脂薄膜之時間點,突出於薄膜面之微粒子(P)的量多,會有變得薄膜面的光澤性不充分且印刷性不充分之顧慮。此外,會有內部霧度變大之顧慮。微粒子(P)的含量W較佳為滿足上式(3-1),更佳為滿足(3-2),進一步較佳為滿足(3-3)之時,可更安定地提供一種熱塑性樹脂薄膜,其係至少一側的薄膜面為高光澤且印刷性優異,內部霧度夠小,且能夠於加熱處理後展現良好的消光外觀。
就熱塑性樹脂(R)而言,並未特別限定,較佳為能夠熔融加工的透明性樹脂。
熱塑性樹脂(R)可為通用的樹脂,亦可為所謂的工程塑膠。熱塑性樹脂(R)可為非橡膠狀聚合物,亦可為橡膠狀聚合物。熱塑性樹脂(R)可使用1種或2種以上。
就作為熱塑性樹脂(R)所使用之非橡膠狀聚合物而言,可舉出例如聚乙烯、聚丙烯、聚丁烯-1、聚-4-甲基戊烯-1、及聚降莰烯等之烯烴系樹脂;甲基丙烯酸甲酯樹脂、及甲基丙烯酸甲酯-苯乙烯樹脂等之甲基丙烯酸系樹脂:聚苯乙烯、苯乙烯-順丁烯二酸酐共聚合物、耐衝擊聚苯乙烯、丙烯腈-苯乙烯(AS)系樹脂、丙烯腈-丁二烯-苯乙烯(ABS)系樹脂、丙烯腈.乙烯-丙烯-二烯.苯乙烯(AES)系樹脂、丙烯酸酯-丙烯腈-苯乙烯(AAS)系樹脂、丙烯腈-氯化乙烯-苯乙烯(ACS)系樹脂、及甲基丙烯酸酯丁二烯苯乙烯(MBS)樹脂等之苯乙烯系樹脂;聚對苯二甲酸乙二酯、及聚對苯二甲酸丁二酯等之酯系樹脂;耐綸6、及耐綸66等之醯胺系樹脂;以及,聚氯乙烯、聚偏二氯乙烯、聚偏二氟乙烯、聚乙烯醇、乙烯-乙酸乙烯酯系樹脂、乙酸纖維素系樹脂、丙烯酸酯-氯化乙烯系樹脂、縮醛系樹脂、氟系樹脂、芳香族碳酸酯系樹脂、碸系樹脂、醚碸系樹脂、甲基戊烯系樹脂、芳酯系樹脂、含有含脂環結構的乙烯性不飽和單體單元的樹脂、苯硫醚(phenylene sulfide)系樹脂、苯醚(phenylene oxide)系樹脂、二醚酮(ether ether ketone)系樹脂、乙烯-丙烯酸乙酯系樹脂、氯化乙烯系樹脂、胺基甲酸酯系樹脂、改質聚苯醚、及聚矽氧改質樹脂等。
就作為熱塑性樹脂(R)所使用之橡膠狀聚合物而言,可舉出SEPS、SEBS、及SIS等之苯乙烯系熱塑性彈性體;IR、EPR、及EPDM等之烯烴系橡膠;丙烯酸
系熱塑性彈性體;氯乙烯系熱塑性彈性體;胺基甲酸酯系熱塑性彈性體;酯系熱塑性彈性體;醯胺系熱塑性彈性體;離子聚合物(ionomer)系樹脂;苯乙烯.丁二烯嵌段共聚合物;乙烯-丙烯橡膠;丁二烯系樹脂;丙烯酸系橡膠;聚矽氧橡膠;丙烯酸系多層結構聚合物等。
由於可獲得具有充分的彎曲強度,且於藉由輥對輥(Roll to Roll)製程之連續生產中對輥上的捲繞為容易之薄膜,熱塑性樹脂(R)較佳為包含至少1種的橡膠狀聚合物。此外,藉由使用橡膠狀聚合物,亦可獲得熱塑性樹脂薄膜之耐衝擊性的提升效果。
就橡膠狀聚合物而言,上述例示之中,較佳為包含至少1層之橡膠層的多層結構粒子(所謂的核/殼結構橡膠粒子)及嵌段共聚合物等。其中,從耐衝擊性等之觀點,特佳為丙烯酸系多層結構聚合物。
就丙烯酸系多層結構聚合物而言,可使用公知之物。從耐衝擊性等之觀點,就丙烯酸系多層結構聚合物而言,較佳為丙烯酸系多層結構聚合物粒子(A),其至少1層的內層(比最外層內側之層)係主成分單體單元為具有碳數1~8的烷基之丙烯酸烷酯單體單元及/或共軛二烯系單體單元的交聯彈性聚合物層,而最外層係主成分單體單元為具有碳數1~8的烷基之甲基丙烯酸烷酯單體單元的熱塑性聚合物層。
於本說明書中,只要無特別述明,則「主成分單體單元」係定義為50質量%以上的單體單元。
丙烯酸系多層結構聚合物粒子(A),係所謂的核/殼結構橡膠粒子,其藉由最外層的熱塑性聚合物層,而覆蓋包含至少1層的交聯彈性聚合物層之1層或複數層的內層。
丙烯酸系多層結構聚合物粒子(A),較佳為構成最外層除外的至少1層之內層的交聯彈性聚合物層之分子鏈、與鄰接之層中之分子鏈是藉由共價結合而被結合的接枝共聚合物。
就交聯彈性聚合物層中所使用之具有碳數1~8的烷基之丙烯酸烷酯而言,可舉出例如丙烯酸甲酯、丙烯酸乙酯、丙烯酸丁酯、丙烯酸2-乙基己酯、及丙烯酸丙酯等。從耐衝擊性之點,較佳為丙烯酸正丁酯。就交聯彈性聚合物層中所使用之共軛二烯系單體而言,可舉出例如1,3-丁二烯、及異戊二烯等。
交聯彈性聚合物層中,除了具有碳數1~8的烷基之丙烯酸烷酯及/或共軛二烯系單體之外,亦可使用能夠與該等共聚合的乙烯系單體。就能夠共聚合的乙烯系單體而言,可舉出例如甲基丙烯酸甲酯、甲基丙烯酸乙酯、甲基丙烯酸丁酯、及甲基丙烯酸環己酯等之甲基丙烯酸酯;苯乙烯、對甲基苯乙烯、及α-甲基苯乙烯等之芳香
族乙烯化合物;N-丙基順丁烯二醯亞胺、N-環己基順丁烯二醯亞胺、及N-鄰氯苯基順丁烯二醯亞胺等之順丁烯二醯亞胺系化合物;乙二醇二甲基丙烯酸酯、丙二醇二甲基丙烯酸酯、三乙二醇二甲基丙烯酸酯、己二醇二丙烯酸酯、乙二醇二丙烯酸酯、丙二醇二丙烯酸酯、三乙二醇二丙烯酸酯、甲基丙烯酸烯丙酯、及三聚異氰酸三烯丙酯等之多官能性單體等。
再者,於本說明書中,「多官能性單體」係具有2以上之聚合性官能基的單體。
從本發明之熱塑性樹脂薄膜的耐衝擊性等之觀點,交聯彈性聚合物層中之具有碳數1~8的烷基之丙烯酸烷酯單元及/或共軛二烯系單體單元的含量,較佳為60質量%以上,更佳為70質量%以上,進一步較佳為80質量%以上,特佳為90質量%以上。
於丙烯酸系多層結構聚合物粒子(A)中,就最外層的熱塑性聚合物層中所使用之具有碳數1~8的烷基之甲基丙烯酸烷酯而言,可舉出例如甲基丙烯酸甲酯、甲基丙烯酸乙酯、甲基丙烯酸丙酯、甲基丙烯酸丁酯、及甲基丙烯酸環己酯等。熱塑性聚合物層中之甲基丙烯酸烷酯單體單元的含量,從丙烯酸系多層結構聚合物粒子(A)的分散性之點,較佳為70質量%以上,更佳為80質量%以上。
丙烯酸系多層結構聚合物粒子(A)的層數並未特別限定,係2層、3層、或4層以上。在熱安定性及生產性之點,丙烯酸系多層結構聚合物粒子(A)特佳為3層結構。
就丙烯酸系多層結構聚合物粒子(A)而言,較佳為3層結構聚合物粒子(AX),其從中心側起包含:第1層,係包含含有30~98.99質量%之甲基丙烯酸甲酯單元、1~70質量%之具有碳數1~8的烷基之丙烯酸烷酯單元、及0.01~2質量%之多官能性單體單元的交聯聚合物層;第2層,係包含含有70~99.9質量%之具有碳數1~8的烷基之丙烯酸烷酯單元、0~30質量%之甲基丙烯酸甲酯單元(任意成分)、及0.1~5質量%之多官能性單體單元的交聯彈性聚合物層;第3層(最外層),係包含含有80~99質量%之甲基丙烯酸甲酯單元、及1~20質量%之具有碳數1~8的烷基之丙烯酸烷酯單元的硬質熱塑性聚合物層。
於3層結構聚合物粒子(AX)中,各層的比率並未特別限定,較佳為第1層是5~40質量%,第2層是20~55質量%,第3層(最外層)是40~75質量%。
丙烯酸系多層結構聚合物粒子(A)的粒徑並未特別限定,但較佳為0.05~0.20μm之範圍內,更佳為0.07~0.15μm,特佳為0.08~0.10μm。丙烯酸系多層結構
聚合物粒子(A)的粒徑小於0.05μm時,則會有丙烯酸系多層結構聚合物粒子(A)的操作性降低之傾向。丙烯酸系多層結構聚合物粒子(A)的粒徑超過0.20μm時,則會有本發明之熱塑性樹脂薄膜於被施加應力時白化而透射率容易降低(抗應力白化性惡化)之傾向。從抗應力白化性之觀點,丙烯酸系多層結構聚合物粒子(A)的粒徑較佳為0.15μm以下。
丙烯酸系多層結構聚合物粒子(A)的聚合法並未特別限定,較佳為乳化聚合法。首先,使1種或2種以上的原料單體乳化聚合而得到核粒子之後,使其他的1種或2種以上之單體於核粒子的存在下乳化聚合,而使核粒子的周圍形成殼。接著因應需要,而於包含核與殼之粒子的存在,進一步使1種或2種以上之單體乳化聚合而使別的殼形成。可藉由反覆進行這種聚合反應,而製造目的之丙烯酸系多層結構聚合物粒子(A)作為乳化乳膠。於所得之乳膠中,通常除了丙烯酸系多層結構聚合物粒子(A)以外,存在具有甲基丙烯酸甲酯單元之直鏈的甲基丙烯酸系樹脂。
就乳化聚合中所使用之乳化劑而言,並未特別限定,可舉出陰離子系乳化劑、非離子系乳化劑、及非離子.陰離子系乳化劑等。該等乳化劑可使用1種或2種以上。
就陰離子系乳化劑而言,可舉出例如磺琥珀酸鈉二辛酯、及磺琥珀酸鈉二月桂酯等之磺琥珀酸鹽二烷酯;十二烷基苯磺酸鈉等之烷基苯磺酸鹽;十二烷基硫酸鈉等之烷基硫酸鹽等。
就非離子系乳化劑而言,可舉出例如聚氧乙烯烷基醚、及聚氧乙烯壬基苯基醚等。
就非離子.陰離子系乳化劑而言,可舉出例如聚氧乙烯壬基苯基醚硫酸鈉等之聚氧乙烯壬基苯基醚硫酸鹽;聚氧乙烯烷基醚硫酸鈉等之聚氧乙烯烷基醚硫酸鹽;聚氧乙烯十三烷基醚醋酸鈉等之烷基醚羧酸鹽等。
為了使乳化劑的起泡性不會極端地變大,非離子系乳化劑或非離子.陰離子系乳化劑的例示化合物中之氧乙烯單元的加成莫耳數,一般為30莫耳以下,較佳為20莫耳以下,特佳為10莫耳以下。
乳化聚合中所使用的聚合起始劑並未特別限定,可舉出例如過硫酸鉀及過硫酸銨等之過硫酸鹽系起始劑;過次硫酸鹽(persulfoxylate)/有機過氧化物及過硫酸鹽/亞硫酸鹽等之氧化還原系起始劑等。
乳化聚合中,可因應需要而使用鏈轉移劑。就鏈轉移劑而言,可舉出例如正辛硫醇、正十二硫醇、正月桂硫醇、三級十二硫醇、及二級丁硫醇等之烷硫醇。
在各層的乳化聚合之際,單體、乳化劑、聚合起始劑、及鏈轉移劑等之原料之對聚合反應系的添加,係可藉由統一添加法、批次添加法、及連續添加法等之公知的任意之方法來進行。
各層的聚合反應溫度,係任一者皆較佳為30~120℃,更佳為50~100℃。各層的聚合反應時間亦因所使用之聚合起始劑及乳化劑的種類與使用量、及聚合溫度而不同,但各層都通常為0.5~7小時。單體與水的質量比(單體/水比)較佳為1/20~1/1。
藉由乳化聚合所獲得之聚合物乳膠中包含的丙烯酸系多層結構聚合物粒子(A)為粒狀。其粒徑較佳為0.05~0.2μm。可將包含丙烯酸系多層結構聚合物粒子(A)之乳膠用於本發明之熱塑性樹脂薄膜的製造。
丙烯酸系多層結構聚合物粒子(A)係可因應需要,而對於藉由乳化聚合所製造之聚合物乳膠,藉由公知方法而實施凝固、脫水、及乾燥等,來作為粉末狀等之聚合物而進行回收。就粉末狀等之丙烯酸系多層結構聚合物粒子(A)的分離回收方法而言,可舉出鹽析凝固法、凍結凝固法、及噴霧乾燥法等。其中,從將雜質藉由水洗而可容易地除去之點,較佳為鹽析凝固法及凍結凝固法。再者,較佳為於凝固步驟之前,以除去混入乳膠中之異物為目的,使用孔徑50μm以下的金屬絲網等而實施過濾之步驟。
於本發明中使用的熱塑性樹脂組成物(C)中,丙烯酸系多層結構聚合物粒子(A)的含量較佳為40~80質量%,更佳為50~70質量%,特佳為62~67質量%。
再者,丙烯酸系多層結構聚合物粒子(A)的含量,係設為使用丙酮而以以下的方法求出者。
將熱塑性樹脂組成物(C)充分乾燥而除去水分之後,測定其質量(W1)。其次,將此熱塑性樹脂組成物(C)放入試管,加入丙酮而進行溶解,除去丙酮可溶部分。然後,使用真空加熱乾燥機除去丙酮,得到殘留物。由此殘留物分離微粒子,其次測定所得之殘留物的質量(W2)。根據下式,而求出丙烯酸系多層結構聚合物粒子(A)的含量。
[丙烯酸系多層結構聚合物粒子(A)的含量]=(W2/W1)×100(%)
熱塑性樹脂(R)較佳為與丙烯酸系多層結構聚合物粒子(A)一起,而進一步包含含有80質量%以上之甲基丙烯酸甲酯單元且極限黏度為0.3~1.0dl/g之甲基丙烯酸系樹脂(B)。於甲基丙烯酸系樹脂(B)中,從耐熱性之點,甲基丙烯酸甲酯單元的含量更佳為85質量%以上,特佳為90質量%以上。甲基丙烯酸系樹脂(B)可使用1種或2種以上。
甲基丙烯酸系樹脂(B)係透明性高,且藉由使用其,而容易調整熱塑性樹脂(R)與微粒子(P)之折射率差,而較佳。
甲基丙烯酸系樹脂(B)可與甲基丙烯酸甲酯單元合計,因應需要而包含20質量%以下之能夠共聚合的乙烯系單體單元。就乙烯系單體而言,並未特別限定,可舉出例如丙烯酸甲酯、丙烯酸乙酯、丙烯酸丁酯、丙烯酸丙酯、丙烯酸己酯、丙烯酸環己酯、丙烯酸2-乙基己酯、丙烯酸苯酯、及丙烯酸苄酯等之丙烯酸酯單體;甲基丙烯酸乙酯、甲基丙烯酸丁酯、甲基丙烯酸丙酯、甲基丙烯酸己酯、甲基丙烯酸環己酯、甲基丙烯酸苯酯、及甲基丙烯酸苄酯等之甲基丙烯酸酯;醋酸乙烯酯、苯乙烯、對甲基苯乙烯、鄰甲基苯乙烯、間甲基苯乙烯、α-甲基苯乙烯、及乙烯基萘等之芳香族乙烯化合物;丙烯腈、及甲基丙烯腈等之腈類;丙烯酸、甲基丙烯酸、巴豆酸等之α、β-不飽和羧酸;N-乙基順丁烯二醯亞胺及N-環己基順丁烯二醯亞胺等之順丁烯二醯亞胺化合物等。該等可使用1種或2種以上。
甲基丙烯酸系樹脂(B)的極限黏度為0.3~1.0dl/g。當甲基丙烯酸系樹脂(B)的極限黏度小於0.3dl/g時,則將包含熱塑性樹脂(R)與微粒子(P)的熱塑性樹脂組成物(C)熔融成形之際的黏著強度會降低,而不佳。當甲基丙烯酸系樹脂(B)的極限黏度超過1.0dl/g時,則將熱塑性樹脂組成物(C)熔融成形之際的流動性會降低,而不佳。
相對於丙烯酸系多層結構聚合物粒子(A)100質量份之甲基丙烯酸系樹脂(B)的摻合量並未特別限定,較佳為1~100質量份,更佳為5~70質量份,特佳為15~45質量份,最佳為20~30質量份。甲基丙烯酸系樹脂(B)的摻合量超過100質量份時,會有本發明之熱塑性樹脂薄膜的抗應力白化性降低之傾向及熱塑性樹脂薄膜變硬之傾向,而不佳。在另一方面,若甲基丙烯酸系樹脂(B)的摻合量為1質量份以上,則將熱塑性樹脂薄膜進行製膜之時的加工性安定,所以較佳。
甲基丙烯酸系樹脂(B)可使用市售品或ISO8257-1之規格品。
甲基丙烯酸系樹脂(B)可藉由公知方法來進行聚合而使用。此處,甲基丙烯酸系樹脂(B)的聚合法並未特別限定,可舉出例如乳化聚合法、懸浮聚合法、塊狀聚合法、及溶液聚合法等。
於本發明之熱塑性樹脂薄膜所分散的微粒子(P),係一般被被稱為消光劑或光擴散劑之微粒子。微粒子(P)可為無機粒子,亦可為有機粒子。微粒子(P)可使用1種或2種以上。
就微粒子(P)而言,可舉出例如碳酸鈣、碳酸鎂、硫酸鋇、氧化鈦、氧化鎂、氧化鋅、氧化鋯、氧化鋁、氫氧化鋁、矽石(二氧化矽)、鍛燒矽酸鈣、鍛燒高嶺土、水合矽酸鈣、矽酸鋁、矽酸鎂、磷酸鈣、玻璃、滑石、黏土、雲母、碳黑、及白碳等之無機粒子;交聯苯乙烯系樹脂粒子、高分子量苯乙烯系樹脂粒子、及交聯矽氧烷系樹脂粒子等之樹脂粒子等。微粒子(P)亦可為對於上述例示之粒子使用脂肪酸等而進行了表面處理之粒子。上述之中,又較佳為雲母等。雲母可為合成雲母與天然雲母之任一者。
本發明之熱塑性樹脂薄膜可於上述之成分以外,在無損本發明之目的的範圍,因應需要而包含1種或2種以上的任意成分。
就任意成分而言,可舉出例如抗氧化劑、熱劣化防止劑、紫外線吸收劑、光安定劑、塑化劑、潤滑劑、脫模劑、高分子加工助劑、抗靜電劑、阻燃劑、染顏料、有機色素、耐衝擊性改質劑、起泡劑、填充劑、及螢光體等之各種添加劑等。
上述任意成分的添加時機並未特別限定,例如可於至少1種的熱塑性樹脂(R)的聚合時添加,亦可添加於被聚合之至少1種的熱塑性樹脂(R),亦可於至少1種的熱塑性樹脂(R)、微粒子(P)、及因應需要之任意成分的混鍊時或者混鍊後添加。
抗氧化劑,係於氧存在下,以其單體而對樹脂的氧化劣化防止具有效果者。可舉出例如磷系抗氧化劑、受阻酚系抗氧化劑、及硫醚系抗氧化劑等。就抗氧化劑而言,亦可使用於同一分子中包含具有磷系抗氧化劑的效果之部分及具有受阻酚系抗氧化劑的效果之部分的抗氧化劑。該等的抗氧化劑可使用1種或2種以上。其中,從因著色所導致之光學特性的劣化防止效果之觀點,較佳為磷系抗氧化劑及受阻酚系抗氧化劑等,更佳為磷系抗氧化劑與受阻酚系抗氧化劑的併用。併用磷系抗氧化劑與受阻酚系抗氧化劑之情形,磷系抗氧化劑的使用量:受阻酚系抗氧化劑的使用量係以質量比而較佳為1:5~2:1,更佳為1:2~1:1。
就磷系抗氧化劑而言,較佳為例如亞磷酸2,2-亞甲雙(4,6-二(三級丁基)苯基)辛基酯(ADEKA公司製;商品名:ADK STAB HP-10)、亞磷酸三(2,4-二(三級丁基)苯基)酯(BASF公司製;商品名:IRGAFOS168)、及3,9-雙(2,6-二(三級丁基)-4-甲基苯氧基)-2,4,8,10-四氧-3,9-二磷螺[5.5]十一烷(ADEKA公司製;商品名:ADK STAB PEP-36)等。
就受阻酚系抗氧化劑而言,較佳為例如新戊四醇肆[3-(3,5-二(三級丁基)-4-羥苯)丙酸]酯(BASF公司製;商
品名IRGANOX1010)、及3-(3,5-二(三級丁基)-4-羥苯)丙酸十八酯(BASF公司製;商品名IRGANOX1076)等。
就於同一分子中包含具有磷系抗氧化劑的效果之部分及具有受阻酚系抗氧化劑的效果之部分的抗氧化劑而言,較佳為例如6-[3-(3-三級丁基-4-羥-5-甲基)丙氧基]-2,4,8,10-四-三級丁基二苯[d,f][1,3,2]-二氧磷環庚烷(dioxaphosphepin)(住友化學工業公司製;商品名:Sumilizer GP)等。
熱劣化防止劑,係藉由捕捉在實質上無氧的狀態下被放置於高熱時所產生的高分子自由基,而可防止樹脂的熱劣化者。就熱劣化防止劑而言,較佳為例如丙烯酸2-三級丁基-6-(3’-三級丁基-5’-甲基-羥苄基)-4-甲苯酯(住友化學公司製;商品名Sumilizer GM)、及丙烯酸2,4-二三級戊基-6-(3’,5’-二三級戊基-2’-羥-α-甲苄基)苯酯(住友化學公司製;商品名Sumilizer GS)等。
紫外線吸收劑係具有吸收紫外線之能力的化合物。紫外線吸收劑係主要被稱為具有將光能轉換為熱能之機能的化合物。就紫外線吸收劑而言,可舉出例如二苯基酮類、苯并三唑類、三類、苯甲酸酯類、水楊酸酯類、氰基丙烯酸酯類、草酸醯胺苯類、丙二酸酯類、及甲脒
類等。該等可使用1種或2種以上。上述之中,又較佳為苯并三唑類、三類、或於波長380~450nm之莫耳吸光係數的最大值εmax為1200dm3.mol-1cm-1以下之紫外線吸收劑。
苯并三唑類,係抑制因被照射紫外線所導致之著色等之光學特性降低的效果高。就苯并三唑類而言,較佳為例如2-(2H-苯并三唑-2-基)-4-(1,1,3,3-四甲基丁基)苯酚(BASF公司製;商品名TINUVIN329)、2-(2H-苯并三唑-2-基)-4,6-雙(1-甲基-1-苯基乙基)苯酚(BASF公司製;商品名TINUVIN234)、及2,2’-亞甲雙[6-(2H-苯并三唑-2-基)-4-三級辛基苯酚](ADEKA公司製;LA-31)等。
於波長380~450nm之莫耳吸光係數的最大值εmax為1200dm3.mol-1cm-1以下之紫外線吸收劑,可抑制所獲得之熱塑性樹脂薄膜的偏黃。而就這種紫外線吸收劑言,可舉出例如2-乙基-2’-乙氧基-草醯苯胺(Clariant Japan Co.,Ltd.製;商品名SANDEYUBOA VSU)等。
在上述之紫外線吸收劑之中,從所謂可抑制因被照射紫外線所導致之樹脂劣化的觀點,較佳使用苯并三唑類等。
此外,欲有效率地吸收波長380nm附近的波長之情形,係較佳使用三類的紫外線吸收劑。就這種紫外線
吸收劑而言,可舉出例如2,4,6-參(2-羥-4-己氧基-3-甲基苯基)-1,3,5-三(ADEKA公司製;LA-F70)、及其類似物的羥苯三系紫外線吸收劑(BASF公司製;TINUVIN477-D或TINUVIN460或TINUVIN479)等。
進一步欲特別有效地吸收380~400nm之波長的光之情形,較佳為使用國際公開第2011/089794號公報、國際公開第2012/124395號公報、日本特開2012-012476號公報、日本特開2013-023461號公報、日本特開2013-112790號公報、日本特開2013-194037號公報、日本特開2014-62228號公報、日本特開2014-88542號公報、及日本特開2014-88543號公報等中所揭示之具有雜環結構之配位子的金屬錯合物(例如以下式(A)所表示之結構的化合物等)作為紫外線吸收劑。
式(A)中,M為金屬原子。Y1、Y2、Y3及Y4係分別獨立地為碳原子以外的二價基(氧原子、硫原子、NH、
及NR5等)。此處,R5為烷基、芳基、雜芳基、雜芳烷基、及芳烷基等之取代基。此取代基係亦可於此取代基進一步具有取代基。Z1及Z2係分別獨立地為三價基(氮原子、CH、及CR6等)。此處,R6為烷基、芳基、雜芳基、雜芳烷基、及芳烷基等之取代基。此取代基係亦可於此取代基進一步具有取代基。R1、R2、R3及R4係分別獨立地為氫原子、烷基、羥基、羧基、烷氧基、鹵基、烷磺醯基、啉磺醯基、六氫吡啶磺醯基、硫代啉磺醯基、及哌磺醯基等之取代基。此取代基係亦可於此取代基進一步具有取代基。a、b、c及d分別表示R1、R2、R3及R4的數量,係分別為1~4之任一整數。
就雜環結構之配位子而言,可舉出例如2,2’-亞胺雙苯并噻唑、2-(2-苯并噻唑基胺基)苯并唑、2-(2-苯并噻唑基胺基)苯并咪唑、(2-苯并噻唑基)(2-苯并咪唑基)甲烷、雙(2-苯并唑基)甲烷、雙(2-苯并噻唑基)甲烷、雙[2-(N-取代)苯并咪唑基]甲烷、及該等之衍生物等。
就金屬錯合物的中心金屬而言,較佳為使用銅、鎳、鈷、及鋅。
為了將金屬錯合物作為紫外線吸收劑使用,較佳為使金屬錯合物分散於低分子化合物或者聚合物等之介質媒體中。金屬錯合物的添加量,係相對於熱塑性樹脂100質量份,而較佳為0.01~5質量份,更佳為0.1~2質量份。由於金屬錯合物於380~400nm的波長之莫耳吸光係數
大,所以為了得到充分的紫外線吸收效果所添加之量,係少量即可。若添加量變少,則可抑制因滲出(bleed out)等所導致之薄膜外觀的惡化。此外,由於金屬錯合物係耐熱性高,所以製膜時的劣化或者分解少。進一步由於金屬錯合物係耐光性高,所以可長期間保持紫外線吸收性能。
再者,紫外線吸收劑之莫耳吸光係數的最大值εmax係如以下地進行來測定。於環己烷1L中添加紫外線吸收劑10.00mg並使其溶解,使在藉由目視之觀察無未溶解物。將此溶液注入1cm×1cm×3cm的石英玻璃槽,使用日立製作所公司製U-3410型分光光度計,測定在波長380~450nm的吸光度。從紫外線吸收劑的分子量(MUV)、與所測定之吸光度的最大值(Amax)藉由下式進行計算,算出莫耳吸光係數的最大值εmax。
εmax=[Amax/(10×10-3)]×MUV
光安定劑,係主要被稱為具有捕捉因光而導致之氧化所生成的自由基之機能的化合物。就適合的光安定劑而言,可舉出具有2,2,6,6-四烷基哌啶骨架的化合物等之受阻胺類等。
就潤滑劑而言,可舉出例如硬脂酸、蘿酸、硬脂醯胺酸、亞甲雙硬脂醯胺、三羥硬脂酸甘油脂、固體石蠟、酮蠟(ketone wax)、辛醇、及硬化油等。該等可使用1種或2種以上。
就脫模劑而言,可舉出例如鯨臘醇、硬脂醇等之高級醇類;硬脂酸單甘油酯、硬脂酸雙甘油酯等之高級脂肪酸甘油酯等。該等可使用1種或2種以上。
作為脫模劑,較佳為併用高級醇類與脂肪酸單甘油酯。併用高級醇類與脂肪酸單甘油酯之情形,其比例並未特別限定,但高級醇類的使用量:脂肪酸單甘油酯的使用量係以質量比而較佳為2.5:1~3.5:1,更佳為2.8:1~3.2:1。
就高分子加工助劑而言,係例如使用下述聚合物粒子,其係藉由乳化聚合法而被製造,且由60質量%以上之甲基丙烯酸甲酯單元及能夠與其共聚合的40質量%以下之乙烯系單體單元所構成,平均聚合度為3,000~40,000,具有0.05~0.5μm之粒徑。該聚合物粒子,可為包含單一組成及單一極限黏度之聚合物的單層粒子,亦可為包含組成或極限黏度不同的2種以上之聚合物的多層粒子。特佳為2層結構之粒子,其係於內層具有具較低極限黏度的聚合物層,且於外層具有具5dl/g
以上之較高極限黏度的聚合物層。高分子加工助劑較佳為極限黏度係3~6dl/g。極限黏度過小或者過大時,則會有製膜性降低之顧慮。具體而言,可舉出Mitsubishi Rayon公司製METABLEN-P系列、Rohm and Haas公司製、Dow Chemical公司製、及吳羽化學公司製的PARALOID系列等。本發明之熱塑性樹脂薄膜中所摻合之高分子加工助劑的量,係相對於熱塑性樹脂的總量100質量份,而較佳為0.1~5質量份。高分子加工助劑的摻合量小於0.1質量份時,會有成形性降低之顧慮,而超過5質量份時,會有熔融流動性降低之顧慮。
就有機色素而言,較佳為使用具有將紫外線轉換為可見光之機能的化合物等。
就螢光體而言,可舉出螢光顏料、螢光染料、螢光白色染料、螢光增白劑、及螢光漂白劑等。該等可使用1種或2種以上。
上述各種添加劑的總量並未特別限定,一般在熱塑性樹脂薄膜100質量%中為0.01~20質量%,較佳為0.05~1.5質量%。
於裝飾用薄膜等之用途中,本發明之熱塑性樹脂薄膜較佳為依據JIS Z 0208所測定之於溫度40℃及相對濕度90%之透濕度為80g/day/m2以下。透濕度滿足上述規定之情形,濕氣所導致之對基材的影響會被抑制而較佳。
本發明之熱塑性樹脂薄膜可使用含有熱塑性樹脂(R)、微粒子(P)、及因應需要之其他任意成分的熱塑性樹脂組成物(C)來製造。於熱塑性樹脂組成物(C)中,各成分較佳為近乎均勻地分散。
就熱塑性樹脂薄膜的製造方法而言,較佳為將含有熱塑性樹脂(R)與微粒子(P)之複數種的原料熔融混鍊而配製熱塑性樹脂組成物(C),將所得之熱塑性樹脂組成物(C)薄膜成形之方法。
本發明之熱塑性樹脂薄膜的製造方法,較佳為具有將熱塑性樹脂組成物(C)由T字模熔融擠出成薄膜狀之步驟、與將擠出成薄膜狀之熔融物(以下,有僅簡略為「熔融物」之情形。)以雙方為金屬剛體輥之一對冷卻輥、或是一方為金屬剛體輥而另一方為金屬彈性輥之一對冷卻輥來挾持之步驟。
包含熱塑性樹脂(R)與微粒子(P)之複數種的原料可統一而進行熔融混鍊,亦可分為複數次而進行熔融混
鍊。熔融混鍊可使用例如揑揉機(kneader ruder)、擠製機、混合輥、及班布里混合機等之熔融混鍊裝置來進行。混鍊溫度較佳為因應樹脂成分的熔融溫度而適當調節,通常為140℃~300℃之範圍內。於熔融混鍊時,關於熱塑性樹脂組成物(C)之剪切速率,較佳為100sec-1以上,更佳為200sec-1以上。
以上述溫度實施熔融混鍊之後,將所得之熔融混鍊物冷卻為120℃以下的溫度。冷卻係比起自然放冷而較佳為急速冷卻。就急速冷卻法而言,可舉出將熔融狀態的繩股浸漬於冷水槽之方法等。
藉由熔融混鍊所獲得之熱塑性樹脂組成物(C),係為了提高保存、運搬或成形時的便利性,而可製成團粒、顆粒、及粉末等之任意的形態。
就薄膜成形法而言,可舉出擠出成形法、溶液鑄造法、熔融鑄造法、充氣成形法、及吹塑成形法等。其中,又較佳為擠出成形法。若藉由擠出成形法,則能以比較高的生產性得到透明性高且厚度的均勻性良好而表面平滑性良好的薄膜。
在擠出成形法,較佳為使用附有T字模的擠製機。附有T字模的擠製機係具備:原料之熱塑性樹脂組成物(C)被投入的進料斗等之原料投入部、將被投入之熱塑性樹脂組成物(C)加熱熔融並送出至T字模側之螺旋部、及
將經加熱熔融之熱塑性樹脂組成物(C)擠出成薄膜狀之T字模。
於附有T字模的擠製機中,熔融樹脂較佳為使用齒輪泵來定量供給至T字模。可藉此而製造厚度精度高的薄膜。
熔融樹脂還較佳為藉由使用了高分子過濾器等的過濾而除去雜質之後,供給至T字模。附有T字模的擠製機的設定溫度並未特別限定,因應熱塑性樹脂組成物(C)之組成而設定,較佳為160~300℃,更佳為220~280℃,進一步較佳為240~270℃,特佳為250~260℃。此外,較佳為由擠製機的尖端到T字模之間也設定為同樣的溫度。再者,附有T字模的擠製機的設定溫度即為熱塑性樹脂組成物(C)的熔融溫度(加工溫度)。
在上述溫度成為熔融狀態的熱塑性樹脂組成物(C),係由T字模的吐出口向垂直下方被擠出成薄膜狀。T字模的溫度分布較佳為±15℃以下,更佳為±5℃以下,特佳為±1℃以下。T字模的溫度分布超過±15℃之情形,會有於熔融樹脂產生黏度不均,而於所獲得之薄膜產生因厚度不均、及應力不均所導致的扭曲等之顧慮,而不佳。
就由T字模擠出之熔融物的冷卻方法而言,可舉出軋輥(nip roll)方式、靜電施加方式、氣刀方式、壓延方
式、單面帶方式、兩面帶方式、及3支輥方式等。在本發明,較佳為軋輥方式。藉由軋輥方式而容易得到印刷性優異的薄膜。
在軋輥方式,由T字模擠出之熔融物係藉由冷卻輥單元而被加壓及冷卻,該冷卻輥單元係包含複數的冷卻輥(軋輥),該等係空出對應於熱塑性樹脂薄膜之期望厚度的分隔距離之分隔部,而互相鄰接地配置。
以下,於冷卻輥單元中,將自上游側起第n個(n為1以上之整數)的冷卻輥稱為「第n冷卻輥」。冷卻輥單元係至少包含於T字模之吐出口的下方具有分隔部之第1冷卻輥、與第2冷卻輥。冷卻輥的數量為2以上,較佳為3~4。
由T字模擠出之熔融物,係被挾持在第1冷卻輥與第2冷卻輥之間,並被加壓及冷卻而成為熱塑性樹脂薄膜。再者,熱塑性樹脂薄膜,僅以冷卻輥單元並不會被充分地冷卻,即使是在自最下游的冷卻輥離開之時間點,熱塑性樹脂薄膜係通常並未完全地硬化。自最下游的冷卻輥離開之後,熱塑性樹脂薄膜係一邊流下一邊被進一步冷卻下去。
於本發明中,第1冷卻輥及第2冷卻輥較佳為雙方為金屬剛體輥,或是一方為金屬剛體輥而另一方為金屬彈性輥。
金屬剛體輥係具有於薄膜製造中不會變形之高剛性的金屬輥。金屬剛體輥的表面為平滑面,較佳為鏡面。就金屬剛體輥而言,可使用自以往一般在擠出成形所使用之公知的金屬剛體輥。就金屬剛體輥而言,係例如使用雙重構造的金屬剛體輥,其係包含由鑽孔輥(drilled roll)或螺旋輥等之金屬製中空輥所構成的內輥、與表面平滑之金屬製的外筒,且冷卻流體會在內輥的內部及/或內輥與外筒之間流下。外筒的厚度,係具有至少不會於薄膜製造中變形之充分的厚度,例如20mm左右。內輥及外筒的材料並未特別限定,可舉出不銹鋼及鉻鋼等。
金屬彈性輥係於薄膜製造中表面能夠彈性變形的金屬輥。金屬彈性輥的表面為平滑面,較佳為鏡面。就金屬彈性輥而言,可使用自以往一般在擠出成形所使用之公知的金屬彈性輥。就金屬彈性輥而言,係例如使用雙重構造的金屬彈性輥,其係包含由金屬製中空輥所構成的內輥、與表面平滑而於薄膜製造中能夠彈性變形的金屬製的外筒,且冷卻流體會在內輥的內部及/或內輥與外筒之間流下。亦可使內輥與外筒之間有橡膠或非冷卻目的之任意的流體存在。外筒的厚度,係具有不會於薄膜製造中破裂而能夠彈性變形之充分薄的厚度,例如2~8mm左右。外筒較佳為無熔焊接合部的無接縫結構。內輥及外筒的材料並未特別限定,可舉出不銹鋼及鉻鋼等。
使用2支金屬剛體輥之情形,任一之輥皆外筒未變形,在截面視圖係對於熔融物為點接觸。相對於此,金屬彈性輥係隨著熔融物被壓印而會彈性變形。因此,使用至少1支金屬彈性輥之情形,在熔融物與金屬彈性輥之截面視圖的接觸長係相對地較長,且可在截面視圖線接觸,可將熔融物以更均勻的線壓力進行加壓。
藉由將熔融物以第1冷卻輥及第2冷卻輥來挾持,而薄膜的製膜性會成為良好,可抑制薄膜的厚度不均及條紋的發生。也能夠進行薄膜的薄膜化。
進一步,可藉由使用表面為平滑面,較佳為鏡面之金屬剛體輥或金屬彈性輥作為挾持熔融物的第1冷卻輥及第2冷卻輥,而使至少一側的薄膜面成為在常溫具有高光澤且具有良好的印刷性之面。基本上來說,可使兩薄膜面成為在常溫具有高光澤且具有良好的印刷性之面。
再者,如上所述,在本發明,於薄膜的製造階段中,並不需要具有良好的消光外觀,不需要使作為消光劑之微粒子(P)由薄膜面充分地突出。所以,即使將分散有作為消光劑之微粒子(P)的熱塑性樹脂組成物(C)成形成薄膜狀之後,將所得之熔融物以一對冷卻輥來挾持,而因此微粒子(P)被擠壓進薄膜內部,且消光外觀受損亦無妨。
再者,相較於金屬剛體輥或金屬彈性輥,橡膠輥等之非金屬輥係表面平滑性低,難以得到高光澤的薄膜面。
在本發明之製造方法,係可於第1冷卻輥及第2冷卻輥的雙方使用金屬剛體輥。但是,如上所述,使用金屬彈性輥之情形,熔融物與金屬彈性輥之截面視圖的接觸長會相對地較長,且可將熔融物以更均勻的線壓力進行加壓。因此,可獲得薄膜中的殘留應力之減少效果及薄膜之薄膜化效果等。所以,較佳為一側的冷卻輥(第1冷卻輥或第2冷卻輥)使用金屬彈性輥。
再者,使用金屬彈性輥之情形,需要有會由相反側在截面視點支撐熔融物的金屬剛體輥。亦即,在本發明,特佳為第1冷卻輥及第2冷卻輥之中,一方使用金屬剛體輥,且另一方使用金屬彈性輥。
較佳為第1冷卻輥及第2冷卻輥之中至少一側被設計成輥兩端部的外徑比輥中央部的外徑還要稍微小。此情形,於外周面所形成之輥兩端部與輥中央部之間的高度差,較佳為0.5~1.0mm。若於至少一側的冷卻輥之外周面形成有上述高度差,則可使薄膜之兩端部的厚度比中央部還要厚一些,可抑制由兩端部發生切斷而生產性降低。上述高度差的形狀並未特別限定,可為垂直狀、錐體狀、及階梯狀的任一者。再者,比薄膜的中央部還稍微變厚之薄膜的兩端部,可因應需要而在後步驟切斷除去。
由第1冷卻輥及第2冷卻輥對熔融物施加之線壓力並未特別限定,從熔融物的均勻加壓之觀點,較佳為5kg/cm以上,更佳為10kg/cm以上,進一步較佳為20kg/cm以上,特佳為30kg/cm以上。由第1冷卻輥及第2冷卻輥對熔融物施加之線壓力的上限並未特別限定,從冷卻輥可彈性變形且可防止薄膜的破裂來看,為50kg/cm左右。
如上所述,在本發明之製造方法,較佳為將分散了微粒子(P)之熱塑性樹脂組成物(C)熔融擠出之後,以雙方為金屬剛體輥之一對冷卻輥,或是一方為金屬剛體輥而另一方為金屬彈性輥之一對冷卻輥(第1冷卻輥及第2冷卻輥)來挾持熔融物。
在此方法,熔融物對一對冷卻輥之密接性及剝離性良好,且可抑制微粒子(P)突出於薄膜面,可於製造時製造至少一側的薄膜面為高光澤且印刷性優異的熱塑性樹脂薄膜。
冷卻輥的表面溫度與熱塑性樹脂組成物(C)的玻璃轉移溫度(Tg)之差越小,則熔融物對冷卻輥之密接性提升,而所獲得之薄膜的表面平滑性及表面光澤性提升,但另一方面,會有熔融物自冷卻輥之剝離性降低之傾向。
於本發明之製造方法中,將第1冷卻輥及第2冷卻輥之中,將一方的冷卻輥的表面溫度設為T1,將另一方的冷卻輥的表面溫度設為T2(但是,T2≧T1。),且將熱
塑性樹脂組成物(C)的玻璃轉移溫度(Tg)設為TgC之時,較佳為滿足下式(4),更佳為滿足下式(5)。
10≦|TgC-T2|≦40…(4)
15≦|TgC-T2|≦20…(5)
用於本發明而適合的熱塑性樹脂組成物(C)的TgC,較佳為70~125℃,更佳為90~110℃。T2較佳為60~90℃,更佳為70~80℃。若T2為60~90℃,則薄膜的表面平滑性及表面光澤性、與熔融物自冷卻輥之剝離性的平衡會良好,而較佳。
由於熱塑性樹脂薄膜係藉由第1冷卻輥及第2冷卻輥而被充分地加壓及冷卻,因此冷卻輥單元包含第3以後之冷卻輥之情形,其材質並未特別限定。就第3以後之冷卻輥而言,較佳為金屬剛體輥。
此外,冷卻輥單元包含第3以後之冷卻輥之情形,該輥的表面溫度並未特別限定。第3以後之冷卻輥的表面溫度,較佳為50~90℃,更佳為60~80℃。
圖1係呈示藉由擠出成形法之薄膜製造裝置的一實施形態。
圖1係薄膜製造裝置的概略圖。
如圖1所示,薄膜製造裝置1係具備將原料之樹脂組成物210M(樹脂組成物(C))加熱熔融並擠出成薄膜狀之擠出成形手段110。於本實施形態中,擠出成形手段110為附有T字模的擠製機,其係具備原料之樹脂組成物210M被投入的進料斗等之原料投入部111、將樹脂組成物210M加熱熔融並擠出之螺旋部112、及包含將經加熱熔融之樹脂組成物210M吐出成薄膜狀之吐出口113A的T字模113。
薄膜製造裝置1還具有冷卻輥單元120,其係包含空出對應於樹脂薄膜210所期望的厚度之分隔距離的分隔部而互相鄰接地配置,且將藉由附有T字模的擠出成形手段110而被擠出之熔融物一邊加壓一邊冷卻之複數的冷卻輥。冷卻輥單元120至少包含:於T字模113之吐出口113A的下方具有分隔部之第1冷卻輥121與第2冷卻輥122。
由T字模113被擠出之熔融物,係被挾持在第1冷卻輥121與第2冷卻輥122之間,並被加壓及冷卻,而成為樹脂薄膜210。在此時間點,樹脂薄膜210未充分地被冷卻,並未完全地硬化。
在圖示的例子,冷卻輥單元120包含第1冷卻輥121、第2冷卻輥122、第3冷卻輥123、及第4冷卻輥124。被挾持在第1冷卻輥121與第2冷卻輥122之間並
且被加壓及冷卻所得之熔融物,係自第1冷卻輥121離開而一邊通過第2冷卻輥122的面上一邊被冷卻,被供給至第2冷卻輥122與第3冷卻輥123之間而被加壓。由熔融物所逐步地形成之樹脂薄膜210,係進一步自第2冷卻輥122離開而一邊通過第3冷卻輥123的面上一邊被冷卻,被供給至第3冷卻輥123與第4冷卻輥124之間而被加壓。再者,樹脂薄膜210亦可不在第2冷卻輥122與第3冷卻輥123之間、及/或第3冷卻輥123與第4冷卻輥124之間被加壓(省略圖示)。樹脂薄膜210係進一步自第3冷卻輥123離開而一邊通過第4冷卻輥124的面上一邊被冷卻之後,自第4冷卻輥124離開而朝向接下來的步驟。再者,在此時間點,樹脂薄膜210未充分地被冷卻,並未完全地硬化。
於本實施形態中,擠出成形手段110之T字模113及冷卻輥單元120係被配置於第1製造室R1內。第1製造室R1內的環境溫度並未被特別調整,因加熱熔融樹脂的存在而為比常溫(20~25℃)稍高的例如35~40℃左右。
於本實施形態中,第2製造室R2係鄰接第1製造室R1而設置。由於將藉由冷卻輥單元120而被加壓及冷卻所得之樹脂薄膜210進行徐冷,因此第2製造室R2內的環境溫度較佳為被調整於20~50℃的溫度範圍內。第2製造室R2內的環境溫度係使用公知的空調設備等來進行調整。
薄膜製造裝置1可因應需要而具有將樹脂薄膜210拉伸之公知的拉伸手段(省略圖示)。薄膜製造裝置1可因應需要而具有公知的保護薄膜黏貼手段(省略圖示),其係於所製造之樹脂薄膜210之至少一側的薄膜面黏貼保護薄膜。薄膜製造裝置1可因應需要而具有捲繞所製造之樹脂薄膜210的捲繞輥(省略圖示)。
熱塑性樹脂薄膜的厚度並未特別限定。
再者,如[用以解決課題之手段]之項所說明,通常厚度為5~250μm的情形係主要被分類為「薄膜」,而於比250μm厚的情形係主要被分類為「薄片」,但在本說明書,並未明確地區別薄膜與薄片而將二者一起稱為「薄膜」。
以上述製造方法所製造之未拉伸的熱塑性樹脂薄膜(未拉伸薄膜)的厚度,較佳為10~500μm,更佳為30~400μm,特佳為40~300μm,最佳為50~200μm。厚度小於10μm的薄膜,係有變得難以製造之傾向。若厚度比500μm厚,則會有積層性、操作性、切斷性、及沖壓性等之二次加工性降低,且每單位面積的材料成本也增大之傾向。
本發明之熱塑性樹脂薄膜可為拉伸薄膜。亦即,可對於上述未拉伸薄膜施行拉伸處理而製成拉伸薄膜。藉由拉伸處理而機械強度會升高,可獲得不易發生裂縫的
薄膜。拉伸方法並未特別限定,可舉出例如同時雙軸拉伸法、逐次雙軸拉伸法、及管式(tubular)拉伸法等。從所謂可均勻地拉伸且可獲得高強度的薄膜之觀點,拉伸溫度的下限較佳為比熱塑性樹脂組成物(C)的玻璃轉移溫度(Tg)高10℃的溫度,而拉伸溫度的上限較佳為比熱塑性樹脂組成物(C)的玻璃轉移溫度(Tg)高40℃的溫度。
本發明之印刷樹脂薄膜,係於上述的本發明之熱塑性樹脂薄膜之至少一側的薄膜面施行了印刷者。通常會於上述的本發明之熱塑性樹脂薄膜之一側的薄膜面施行印刷。由於上述的本發明之熱塑性樹脂薄膜於常溫中至少一側的薄膜面具有高光澤性,因此可藉由於具有高光澤性的薄膜面施行印刷,而提供印刷遺漏被抑制且具有良好的印刷外觀之印刷樹脂薄膜。
再者,如上所述,若按照上述的本發明之熱塑性樹脂薄膜的製造方法,則可製造兩薄膜面具有高光澤性的熱塑性樹脂薄膜。一對的薄膜面之GL值不同的情形,從能夠進行更高品質的印刷來看,較佳為於GL值較高的面施行印刷。
就印刷方法而言,並未特別限定,可使用例如凹版印刷法、柔版印刷法、及絲網印刷法等之公知的印刷方法。
再者,於基材上積層本發明之印刷樹脂薄膜之情形,從印刷面的保護及高級感的賦予之點,較佳為以印刷面與基材接觸的方式進行積層。
本發明之消光樹脂薄膜係上述的本發明之熱塑性樹脂薄膜被加熱處理所獲得者。熱塑性樹脂薄膜較佳為於至少一側的薄膜面有施行印刷者。
可藉由使用上述的本發明之熱塑性樹脂薄膜,而提供印刷遺漏被抑制而具有良好的印刷外觀,且具有良好的消光外觀之消光樹脂薄膜。
用於展現消光之加熱處理的溫度及時間,係被設定為至少一側的薄膜面及其附近的熱塑性樹脂組成物(C)充分地軟化,而充分之量的微粒子(P)突出於薄膜面,會展現良好的消光外觀之溫度。加熱處理溫度,係熱塑性樹脂組成物(C)的軟化溫度以上,較佳為Tg~Tg+50℃,更佳為Tg+10℃~Tg+20℃。加熱處理時間較佳為15分鐘~30分鐘。
加熱處理溫度越高、加熱處理時間越長,則微粒子(P)的薄膜面中之突出程度就變得越高,且會有消光的等級變高之傾向。本發明中,係能夠藉由調整薄膜製造後的加熱處理條件,而調整消光的等級。就加熱手段而言,可使用例如烘箱、乾燥機、及恆溫器等,但若為可保持所設定之溫度者,則不限定於該等。例如,於後述之積層、壓縮空氣成形、及真空成形等之後加工中,加熱熱塑性樹脂薄膜而使其軟化的步驟亦可兼任上述加熱處
理。但是,若對熱塑性樹脂薄膜使用表面平滑的壓機而藉由熱壓來進行加熱處理,則會有消光的等級降低之傾向,所以不佳。亦即,加熱處理可在加壓狀態進行,但較佳為在非加壓狀態進行。
本發明之積層薄膜,係具有包含樹脂層的複數個層的薄膜,該樹脂層包含上述的本發明之熱塑性樹脂薄膜、上述的本發明之印刷樹脂薄膜、或上述的本發明之消光樹脂薄膜。
可於上述的本發明之熱塑性樹脂薄膜、上述的本發明之印刷樹脂薄膜、或上述的本發明之消光樹脂薄膜的至少一側的薄膜面設置各種機能層。就機能層而言,可舉出例如硬塗層、抗眩光層、抗反射層、防黏層、擴散層、防眩層、靜電防止層、防污層、易接著層、及含微粒子等之易滑性層等。
上述的本發明之熱塑性樹脂薄膜、上述的本發明之印刷樹脂薄膜、或上述的本發明之消光樹脂薄膜,係與任意之熱塑性樹脂(組成物)之接著性優異,因此可於至少一側的薄膜面,積層樹脂組成不同之至少1層的熱塑性樹脂層。
積層薄膜的製造方法並未特別限定。
就包含上述的本發明之熱塑性樹脂薄膜的積層薄膜之製造方法而言,可舉出(1)將上述的本發明之熱塑性樹脂薄膜的原料樹脂組成物(C)、與其他的熱塑性樹脂(組成物)熔融共擠出,而製造積層薄膜之方法;(2)針對上述的本發明之熱塑性樹脂薄膜的原料樹脂組成物(C)、與其他的熱塑性樹脂(組成物)之任一者,預先得到薄膜,將另一者熔融擠出而對所得之薄膜進行覆蓋,而製造積層薄膜之方法;(3)針對上述的本發明之熱塑性樹脂薄膜的原料樹脂組成物(C)、與其他的熱塑性樹脂(組成物)之雙方,預先得到薄膜,將該等使用加壓(press)、壓縮空氣、真空等而進行熱壓接合之方法;(4)針對上述的本發明之熱塑性樹脂薄膜的原料樹脂組成物(C),預先得到薄膜,在所得之薄膜上使聚合性組成物聚合,而製造積層薄膜之方法等。
再者,於上述方法(3)中,在加壓熱壓接合的步驟,微粒子(P)不會突出於薄膜面,不會展現消光。
對於以上述(1)~(4)之中的任一方法所得之積層薄膜,於本發明之熱塑性樹脂薄膜的露出面施行印刷,藉此而獲得包含上述的本發明之印刷樹脂薄膜的積層薄膜。進一步,藉由將此積層薄膜進行加熱處理,而獲得包含上述的本發明之消光樹脂薄膜的積層薄膜。
就適於積層之其他的熱塑性樹脂而言,並未特別限定,可舉出例如碳酸酯系聚合物、氯乙烯系聚合物、偏二氟乙烯系聚合物、(甲基)丙烯酸系樹脂、ABS系樹脂、AES系樹脂、及AS系樹脂等。該等可使用1種或2種以上。
本發明之積層體,係於基材上積層有上述的本發明之熱塑性樹脂薄膜、上述的本發明之印刷樹脂薄膜、上述的本發明之消光樹脂薄膜、或上述的本發明之積層薄膜者。可藉由於基材上積層上述薄膜,而謀求基材的設計性提升。此外,亦可獲得基材保護的效果。
就基材的材質而言,並未特別限定,可舉出樹脂、鋼材、木材、玻璃、及該等之複合材料等。就基材中所使用的樹脂而言,並未特別限定,可舉出熱塑性樹脂或熱硬化性樹脂。就基材中所使用的熱塑性樹脂而言,可舉出碳酸酯系樹脂、對苯二甲酸乙二酯系樹脂、醯胺系樹脂、烯烴系樹脂、苯乙烯系樹脂、氯乙烯系樹脂、(甲基)丙烯酸系樹脂、及ABS系樹脂等。就基材中所使用的熱硬化性樹脂而言,可舉出環氧系樹脂、酚系樹脂、及三聚氰胺系樹脂等。
本發明之積層體的製造方法並未特別限定,可舉出接著、積層、壓縮空氣成形、真空成形、三維表面裝飾成形(Three dimension Overlay Method:TOM成形)、嵌入成形、及模內成形等。
於基材的材質為樹脂之情形,較佳為對於基材的表面,將本發明之熱塑性樹脂薄膜、本發明之印刷樹脂薄膜、或本發明之積層薄膜在加熱下進行真空成形、壓縮空氣成形、或壓縮成形之方法。其中又特佳為射出成形同時貼合法。射出成形同時貼合法,係於射出成形用之一對的公母模具間插入本發明之熱塑性樹脂薄膜、本發明之印刷樹脂薄膜、或本發明之積層薄膜之後,於模具內(薄膜的單面上)將熔融的熱塑性樹脂射出成形之方法。以此方法,而能夠於與射出成形體之製造同時,同時地實施薄膜之貼合。
於模具內所插入的薄膜,可為平坦者,亦可為以真空成形或壓縮空氣成形等預備成形而可獲得之凹凸形狀者。薄膜的預備成形,可在個別的成形機進行,亦可在射出成形同時貼合法中使用之射出成形機的模具內進行。再者,將薄膜預備成形之後,於其單面將熔融樹脂射出之方法,係被稱為嵌入成形法。
於基材的材質為樹脂之情形,也有將基材與要進行積層之薄膜進行共擠出成形之方法。
再者,在本發明之積層體,係為了使其展現良好的消光外觀,而使最外層為本發明之熱塑性樹脂薄膜。可藉由於上述成形後進一步進行加熱處理,而使其展現良好的消光外觀。藉此而可獲得包含本發明之消光樹脂薄膜的積層體。
可進一步在複合於基材的本發明之薄膜之上,賦予會藉由紫外線(UV)或電子束(EB)的照射而硬化而成之塗層。此情形,可更進一步提高設計性或基材保護性。
本發明之熱塑性樹脂薄膜、本發明之印刷樹脂薄膜、本發明之消光樹脂薄膜、本發明之積層薄膜、及本發明之積層體,係可使用於任意之用途,可較佳地利用於要求設計性之各種用途,適於謀求消光外觀之用途。
本發明之熱塑性樹脂薄膜、本發明之印刷樹脂薄膜、本發明之消光樹脂薄膜、及本發明之積層薄膜,係可較佳地利用於裝飾用薄膜及建材用薄膜等。
就適合的用途而言,可舉出例如家具、吊燈、及鏡子等之室內裝潢構件;及門、窗框、圓頂、安全窗玻璃、隔壁、階梯護牆板、露台護牆板、及休閒用建築物的屋頂等之建築用構件等。
就其他的用途而言,可舉出例如廣告塔、立架招牌、側懸式招牌、橫樑招牌、及屋頂招牌等之招牌構件或看板用薄膜(marking film);展示櫃、隔板、及店鋪展示等之展示構件;螢光燈罩、氣氛照明外罩、燈罩、發光頂板、光壁、及枝形吊燈等之照明構件;飛機風擋、飛行員用護目鏡、機車風擋、汽艇風擋、巴士用遮光板、汽車用側遮光板、後遮光板、頭燈殼、頭燈罩、汽車內裝
組件、及保險桿等之汽車外裝組件等的輸送機相關構件;音響影像用標牌、立體聲音響罩、電視保護罩、自動販賣機、行動電話、及個人電腦等之電子裝置構件;保溫箱、及X光構件等之醫療裝置構件;機械罩、計量儀器罩、實驗裝置、量尺、刻度盤、及觀察窗等之機器相關構件;太陽能電池的背襯薄膜、及可撓式太陽能電池用前面薄膜等之太陽能電池用構件;各種家電製品;交通標誌、指引板、彎道鏡、及隔音牆等之交通相關構件;溫室、大型水槽、箱型水槽、時鐘面板、浴缸等之浴室組件、衛浴設備、桌墊、娛樂構件、玩具、樂器、壁紙、及焊接時的臉部保護用面罩等之表面所設置的裝飾薄膜兼保護薄膜等。
於以下呈示實施例及比較例,以進一步地說明本發明,但本發明不因以下之實施例而受到任何限定。再者,於以下的記載中,只要無特別述明,「份」係代表「質量份」,「%」係代表「質量%」。
各種評價係藉由以下的方法進行。
微粒子(P)的體積平均粒徑,係以規定於[用以解決課題之手段]之項的方法進行測定。
熱塑性樹脂薄膜的整體霧度、內部霧度、及外部霧度,係以規定於[用以解決課題之手段]之項的方法進行測定。
樹脂(組成物)的玻璃轉移溫度(Tg),係以規定於[用以解決課題之手段]之項的方法進行測定。
熱塑性樹脂薄膜的光澤度GL、GH,係以規定於[用以解決課題之手段]之項的方法進行測定。
將熱塑性樹脂薄膜裝到凹版印刷機,對GL值高之側的薄膜面施行文字及圖樣的印刷。根據下述基準,而評價印刷性。
A(良):未觀察到印刷遺漏。
B(可):可些許觀察到印刷遺漏。
C(不可):可觀察到印刷遺漏。
(製造例1)丙烯酸系多層結構聚合物粒子(AX)的聚合:
(1)於具備有攪拌機、溫度計、氮氣體導入部、單體導入管及回流冷卻器的反應器內,進料去離子水200份、十二烷基苯磺酸鈉1份及碳酸鈉0.05份,將容器內以氮氣體充分地進行置換而使其成為實質上無氧的狀態
之後,將內溫設定為80℃。於此投入過硫酸鉀0.01份,並攪拌5分鐘之後,將包含甲基丙烯酸甲酯9.48份、丙烯酸正丁酯0.5份及甲基丙烯酸烯丙酯0.02份的單體混合物花費20分鐘來連續性地滴下供給,結束添加後,進一步進行30分鐘聚合反應使聚合率成為98%以上。
(2)接著,於同反應器內,投入過硫酸鉀0.03份而攪拌5分鐘之後,將包含甲基丙烯酸甲酯1.45份、丙烯酸正丁酯27.67份及甲基丙烯酸烯丙酯0.88份的單體混合物花費40分鐘來連續性地滴下供給。結束添加後,進一步進行30分鐘聚合反應使聚合率成為98%以上。
(3)其次,於同反應器內,投入過硫酸鉀0.06份而攪拌5分鐘之後,將含有甲基丙烯酸甲酯53.73份、丙烯酸正丁酯5.97份及正辛硫醇(鏈轉移劑)0.3份的單體混合物花費100分鐘來連續性地滴下供給,結束添加後,進一步進行60分鐘聚合反應使聚合率成為98%以上,得到包含丙烯酸系多層結構聚合物粒子(AX-1)之乳膠。平均粒徑為0.09μm。
接著,將包含丙烯酸系多層結構聚合物粒子(AX-1)之乳膠在-30℃花費4小時使其凍結。將凍結乳膠投入凍結之乳膠的2倍量的80℃溫水中,進行溶解而作成漿體之後,於80℃保持20分鐘之後,進行脫水,在70℃進行乾燥。
如上述地進行,而得到含有粉末狀的3層結構之丙烯酸系多層結構聚合物粒子(AX-1)與直鏈的甲基丙烯酸系樹脂之熱塑性樹脂組成物(AX-2)。進一步,以公知方法將此熱塑性樹脂組成物(AX-2)進行造粒化。使用丙酮來測定該熱塑性樹脂組成物(AX-2)中之丙烯酸系多層結構聚合物粒子(AX-1)的含量,結果為65質量%。此外,熱塑性樹脂組成物(AX-2)的玻璃轉移溫度為98℃,折射率為1.49。
使用在製造例1所得之包含丙烯酸系多層結構聚合物粒子(AX-1)之組成物(AX-2)的團粒作為原料,並使用微雲母(micromica)MK-100K(Co-op Chemical Co.,Ltd.製,折射率1.53,體積平均粒徑5μm,長寬比30~50)作為微粒子(P),藉由熔融擠出成形,而得到熱塑性樹脂薄膜。再者,微雲母MK-100K之長寬比係藉由平均粒徑/厚度所求得之型錄值。包含丙烯酸系多層結構聚合物粒子(AX-1)之組成物(AX-2)與微粒子(P)之質量比係設為97/3。
起初,使用附有T字模的單軸排氣擠製機,將包含上述原料之混合物的熱塑性樹脂組成物(C)熔融擠出成薄膜狀。熔融擠出條件係如下述。
擠製機的設定溫度(樹脂組成物的熔融溫度):260℃,螺旋徑:75mm,
T字模之寬:1850mm,T字模之模口開度:0.8mm,熔融樹脂自T字模的吐出速度:110kg/h。
其次,將擠出成薄膜狀之熔融物使用包含第1~第4冷卻輥(軋輥)的冷卻輥單元而進行加壓及冷卻。使用調整溫度為64℃之金屬彈性輥作為第1冷卻輥(以下,有簡略為「第1輥」之情形),並使用調整溫度為79℃之金屬剛體輥作為第2冷卻輥(以下,有簡略為「第2輥」之情形)。使用調整溫度為65℃之金屬剛體輥作為第3冷卻輥,並使用調整溫度為60℃之金屬剛體輥作為第4冷卻輥。再者,任一之冷卻輥,表面都為鏡面。此外,任一之輥間距離都設定為75μm,且於任一之輥間,對熔融物施加之線壓力都設為30kg/cm。將熔融物藉由上述冷卻輥單元而加壓及冷卻之後,以與公知方法同樣的方法,得到厚度75μm之未拉伸的熱塑性樹脂薄膜。針對所得之熱塑性樹脂薄膜,進行各種評價。將主要的製造條件與評價結果呈示於表1。
除了將使用之微粒子(P)設為YAMAGUCHI MICA CO.,LTD.製「SJ-010」(體積平均粒徑10μm,長寬比10~30),將其含量設為2質量%以外,係與實施例1同樣地進行,而得到厚度75μm之熱塑性樹脂薄膜。將主要的製造條件與評價結果呈示於表1。
除了在丙烯酸系多層結構聚合物粒子(AX-1)之外,還使用甲基丙烯酸系樹脂(B)(KURARAY CO.,LTD製「PARAPET EH」)作為熱塑性樹脂(R)以外,係與實施例1同樣地進行,而得到厚度75μm之熱塑性樹脂薄膜。包含丙烯酸系多層結構聚合物粒子(AX-1)之組成物(AX-2)、甲基丙烯酸系樹脂(B)、及微粒子(P)的質量比係設為77/20/3。將主要的製造條件與評價結果呈示於表1。
除了使第1冷卻輥與第2冷卻輥的雙方為金屬剛體輥以外,係與實施例1同樣地進行,而得到厚度75μm之熱塑性樹脂薄膜。將主要的製造條件與評價結果呈示於表1。
除了取代微粒子(P)而使用YAMAGUCHI MICA CO.,LTD.製「A-21S」(體積平均粒徑23μm,長寬比60~80)來作為比較用的微粒子(Q),並設其含量為1質量%以外,係與實施例1同樣地進行,而得到厚度75μm之熱塑性樹脂薄膜。將主要的製造條件與評價結果呈示於表2。
除了將微粒子(P)的含量以如表2呈示地分別變更為1質量%、10質量%以外,係與實施例1同樣地進行,而得到厚度75μm之熱塑性樹脂薄膜。將主要的製造條件與評價結果呈示於表2。
除了取代微粒子(P)而使用東洋紡(股)公司製的交聯性丙烯酸系樹脂粒子「TAFTIC(註冊商標)FH-S」(體積平均粒徑5μm,長寬比約1)來作為比較用的微粒子(Q)以外,係與實施例1同樣地進行,而得到厚度75μm之熱塑性樹脂薄膜。將主要的製造條件與評價結果呈示於表2。
除了使一對冷卻輥之中一方或雙方為矽橡膠輥以外,與實施例1同樣地進行,而得到厚度75μm之熱塑性樹脂薄膜。將主要的製造條件與評價結果呈示於表3。
在實施例1~4,係使用包含熱塑性樹脂(R)、及體積平均粒徑為0.5~15μm且與熱塑性樹脂(R)之折射率差為0.02以上的微粒子(P)之熱塑性樹脂組成物(C)。
在實施例1~4,係將上述的熱塑性樹脂組成物(C)由T字模熔融擠出之後,將擠出成薄膜狀之熔融物以雙方為金屬剛體輥之一對冷卻輥、或是一方為金屬剛體輥而
另一方為金屬彈性輥之一對冷卻輥來挾持,而製造熱塑性樹脂薄膜。
在實施例1~4,係得到至少一側的薄膜面滿足上式(1)、(2)之熱塑性樹脂薄膜。在實施例1~4,係得到一種熱塑性樹脂薄膜,其包含粒子(P),並且兩薄膜面於常溫中具有高光澤且具有良好的印刷性,內部霧度及整體霧度小,於加熱處理後會展現良好的消光外觀。
另一方面,在使用體積平均粒徑大的微粒子(Q)的比較例1,所得之熱塑性樹脂薄膜係內部霧度及整體霧度高。
在相對於實施例1而將微粒子(P)的添加量減少並使d.W之值小於10的比較例2,所得之熱塑性樹脂薄膜係於加熱處理之後光澤度未充分地降低,並未得到所期望的消光外觀。
在相對於實施例1而微粒子(P)的添加量增加並使d.W之值超過30的比較例3,所得之熱塑性樹脂薄膜在加熱處理前之時間點,兩薄膜面的光澤性低且印刷性亦些微惡劣。
在使用與熱塑性樹脂(R)之折射率差小的微粒子(Q)的比較例4,所得之熱塑性樹脂薄膜無法於加熱處理後得到充分的光擴散效果,無法得到良好的消光外觀。
在使一對冷卻輥之中一方或雙方為矽橡膠輥的比較例5、6,所得之熱塑性樹脂薄膜係兩薄膜面的表面凹凸大,在剛製造後之時間點呈現消光外觀,且印刷性不良。
本發明不被上述實施形態及實施例所限定,可在不脫離本發明之旨趣的情形下適當地變更設計。
此申請係主張以2016年2月15日所申請之日本申請之特願2016-025751號為基礎之優先權,於此引用其揭示之全文。
1‧‧‧薄膜製造裝置
110‧‧‧擠出成形手段
111‧‧‧原料投入部
112‧‧‧螺旋部
113‧‧‧T字模
113A‧‧‧吐出口
120‧‧‧冷卻輥單元
121‧‧‧第1冷卻輥
122‧‧‧第2冷卻輥
123‧‧‧第3冷卻輥
124‧‧‧第4冷卻輥
210‧‧‧樹脂薄膜
210M‧‧‧樹脂組成物
R1‧‧‧第1製造室
R2‧‧‧第2製造室
Claims (17)
- 一種熱塑性樹脂薄膜,其係由包含至少1種熱塑性樹脂(R)、及體積平均粒徑為0.5~15μm且與熱塑性樹脂(R)之折射率差為0.02以上之微粒子(P)的熱塑性樹脂組成物(C)所構成,且至少一側的薄膜面滿足下式(1)及(2):GL≧60…(1)、GL-35≦GH≦GL-10…(2)(其中,上式(1)、(2)中,GL係在20℃的60°光澤度(%),GH係以比熱塑性樹脂組成物(C)的玻璃轉移溫度高10℃的溫度加熱30分鐘之後,冷卻至20℃之後的60°光澤度(%))。
- 如請求項1之熱塑性樹脂薄膜,其進一步滿足下式(3-1):10/d≦W≦30/d…(3-1)(其中,上式(3-1)中,d為微粒子(P)的體積平均粒徑(μm),W為熱塑性樹脂薄膜中的微粒子(P)之含量(質量%))。
- 如請求項1或2之熱塑性樹脂薄膜,其外部霧度小於內部霧度。
- 如請求項1或2之熱塑性樹脂薄膜,其中,熱塑性樹脂(R)包含丙烯酸系多層結構聚合物粒子(A),其至少1層之內層為主成分單體單元係具有碳數1~8的烷基之丙烯酸烷酯單體單元及/或共軛二烯系單體單元的交聯彈性聚合物層,最外層為主成分單體單元係具有碳數1~8的烷基之甲基丙烯酸烷酯單體單元的熱塑性聚合物層。
- 如請求項4之熱塑性樹脂薄膜,其中,丙烯酸系多層結構聚合物粒子(A)包含3層結構聚合物粒子(AX),其從中心側起包含:第1層,其包含含有30~98.99質量%之甲基丙烯酸甲酯單元、1~70質量%之具有碳數1~8的烷基之丙烯酸烷酯單元及0.01~2質量%之多官能性單體單元的交聯聚合物層;第2層,其包含含有70~99.9質量%之具有碳數1~8的烷基之丙烯酸烷酯單元、0~30質量%之甲基丙烯酸甲酯單元及0.1~5質量%之多官能性單體單元的交聯彈性聚合物層;及第3層,其包含含有80~99質量%之甲基丙烯酸甲酯單元、及1~20質量%之具有碳數1~8的烷基之丙烯酸烷酯單元的硬質熱塑性聚合物層。
- 如請求項4之熱塑性樹脂薄膜,其中,丙烯酸系多層結構聚合物粒子(A)之粒徑為0.05~0.20μm。
- 如請求項4之熱塑性樹脂薄膜,其中,熱塑性樹脂(R)進一步包含甲基丙烯酸系樹脂(B),其包含80質量%以上的甲基丙烯酸甲酯單元且極限黏度為0.3~1.0dl/g。
- 一種印刷樹脂薄膜,其係於如請求項1之熱塑性樹脂薄膜的至少一側的薄膜面施行有印刷。
- 一種消光樹脂薄膜,其係將如請求項1之熱塑性樹脂薄膜、或於該熱塑性樹脂薄膜的至少一側的薄膜面施行有印刷的印刷樹脂薄膜,進行加熱處理所得。
- 一種裝飾用薄膜,其包含如請求項1或2之熱塑性樹脂薄膜、如請求項8之印刷樹脂薄膜、或如請求項9之消光樹脂薄膜。
- 一種建材用薄膜,其包含如請求項1或2之熱塑性樹脂薄膜、如請求項8之印刷樹脂薄膜、或如請求項9之消光樹脂薄膜。
- 一種積層薄膜,其包含如請求項1或2之熱塑性樹脂薄膜、如請求項8之印刷樹脂薄膜、或如請求項9之消光樹脂薄膜。
- 一種積層體,其係於基材上積層有如請求項1或2之熱塑性樹脂薄膜或包含該熱塑性樹脂薄膜之積層薄膜、如請求項8之印刷樹脂薄膜或包含該印刷樹脂薄膜之積層薄膜、或是如請求項9之消光樹脂薄膜或包含該消光樹脂薄膜之積層薄膜。
- 一種熱塑性樹脂薄膜的製造方法,其係如請求項1或2之熱塑性樹脂薄膜的製造方法,其具有:將熱塑性樹脂組成物(C)由T字模熔融擠出成薄膜狀之步驟、與將擠出成薄膜狀之熔融物以雙方為金屬剛體輥之一對冷卻輥、或是一方為金屬剛體輥而另一方為金屬彈性輥之一對冷卻輥來挾持之步驟。
- 如請求項14之熱塑性樹脂薄膜的製造方法,其中,前述一對冷卻輥之中,將一方的冷卻輥之表面溫度設為T1,將另一方的冷卻輥之表面溫度設為T2(其中,T2≧T1),將熱塑性樹脂組成物(C)的玻璃轉移溫度設為TgC時,滿足下式(4): 10≦|TgC-T2|≦40...(4)。
- 一種消光樹脂薄膜的製造方法,其係將如請求項1或2之熱塑性樹脂薄膜進行加熱處理。
- 一種消光樹脂薄膜的製造方法,其係於如請求項1或2之熱塑性樹脂薄膜的至少一側的薄膜面施行印刷,進行加熱處理。
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2017
- 2017-02-13 KR KR1020187023789A patent/KR20180109072A/ko not_active Application Discontinuation
- 2017-02-13 WO PCT/JP2017/005152 patent/WO2017141873A1/ja active Application Filing
- 2017-02-13 EP EP17753130.8A patent/EP3418326B1/en active Active
- 2017-02-13 CN CN201780011340.6A patent/CN108699266B/zh active Active
- 2017-02-13 JP JP2018500102A patent/JP7160676B2/ja active Active
- 2017-02-13 US US16/077,329 patent/US11052645B2/en active Active
- 2017-02-14 TW TW106104696A patent/TWI715722B/zh active
Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
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US11904411B2 (en) | 2019-01-23 | 2024-02-20 | Nitto Denko Corporation | Method for producing thin glass resin laminate piece |
TWI827849B (zh) * | 2019-05-28 | 2024-01-01 | 日商可樂麗股份有限公司 | 丙烯酸系橡膠粒子及甲基丙烯酸樹脂組成物 |
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CN108699266A (zh) | 2018-10-23 |
US11052645B2 (en) | 2021-07-06 |
JPWO2017141873A1 (ja) | 2018-12-06 |
JP7160676B2 (ja) | 2022-10-25 |
US20190055393A1 (en) | 2019-02-21 |
EP3418326A4 (en) | 2019-09-11 |
EP3418326B1 (en) | 2022-04-13 |
EP3418326A1 (en) | 2018-12-26 |
KR20180109072A (ko) | 2018-10-05 |
CN108699266B (zh) | 2021-07-16 |
WO2017141873A1 (ja) | 2017-08-24 |
TWI715722B (zh) | 2021-01-11 |
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