TW201730315A - 接著劑組成物、使用其之黏附體之接合方法、以及積層體之製造方法 - Google Patents
接著劑組成物、使用其之黏附體之接合方法、以及積層體之製造方法 Download PDFInfo
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- TW201730315A TW201730315A TW105125412A TW105125412A TW201730315A TW 201730315 A TW201730315 A TW 201730315A TW 105125412 A TW105125412 A TW 105125412A TW 105125412 A TW105125412 A TW 105125412A TW 201730315 A TW201730315 A TW 201730315A
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- Prior art keywords
- adhesive composition
- adhesive
- polyfunctional
- present
- meth
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Links
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Classifications
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J163/00—Adhesives based on epoxy resins; Adhesives based on derivatives of epoxy resins
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B15/00—Layered products comprising a layer of metal
- B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
- B32B15/08—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B32B15/00—Layered products comprising a layer of metal
- B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
- B32B15/08—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
- B32B15/085—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin comprising polyolefins
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B15/00—Layered products comprising a layer of metal
- B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
- B32B15/08—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
- B32B15/09—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin comprising polyesters
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/06—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material
- B32B27/08—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/28—Layered products comprising a layer of synthetic resin comprising synthetic resins not wholly covered by any one of the sub-groups B32B27/30 - B32B27/42
- B32B27/281—Layered products comprising a layer of synthetic resin comprising synthetic resins not wholly covered by any one of the sub-groups B32B27/30 - B32B27/42 comprising polyimides
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/32—Layered products comprising a layer of synthetic resin comprising polyolefins
- B32B27/325—Layered products comprising a layer of synthetic resin comprising polyolefins comprising polycycloolefins
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/36—Layered products comprising a layer of synthetic resin comprising polyesters
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/38—Layered products comprising a layer of synthetic resin comprising epoxy resins
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Abstract
本發明係一種接著劑組成物、使用其之黏附體之接合方法及積層體之製造方法,該接著劑組成物係含有下述通式(A)所表示之聚環氧烷加成多官能環氧化合物(a)、多官能(甲基)丙烯酸酯單體(b)及光酸產生劑(c)而成。□(上述式中,R表示低級伸烷基(例如碳數1~4之伸烷基),X表示具有環狀結構之碳數6~20之二價之連結基或低級伸烷基(例如碳數1~4之伸烷基);m及n分別獨立地為0以上之整數)。
Description
本發明係關於一種接著劑組成物、使用其之黏附體之接合方法及積層體之製造方法。
於近年之顯示器領域中,因顯示器之輕量化或薄厚化、樹脂化等技術之進展,正不斷推進即便掉落亦不易破裂之顯示器、可彎折/捲取之顯示器、可拉伸之顯示器等之開發。
例如,作為可彎折之顯示器,可列舉液晶顯示器或有機EL顯示器、電子紙等。該等顯示器係對顯示器基板貼合觸控面板或保護膜、偏光板等構件而製作。因此,作為將顯示器基板或各構件貼合之接著劑,提出有以高柔軟性或耐撓曲性為特徵之接著材料。
然而,於用於偏光板之光學膜中,為了防止液晶或偏光膜不受紫外線劣化而摻合有紫外線吸收劑(例如,參照專利文獻1)。因此,將藉由紫外線照射而硬化之光硬化型丙烯酸接著劑用於將偏光板與顯示器基板貼合之用途中而表現出所需之接著特性有困難性。
即,即便於偏光板或顯示器基板塗佈光硬化型丙烯酸接著劑,並於所塗佈之接著劑上重疊顯示器基板或偏光板後,自偏光板側進行紫外線照
射,亦因偏光板中之紫外線吸收劑而紫外線被吸收,光硬化型丙烯酸接著劑未充分硬化。
另一方面,於將偏光板與顯示器基板重疊並自顯示器基板側進行紫外線照射之情形時,顯示器基板必需為透明,即便為透明,亦有因強力之紫外線而使彩色濾光片等中所含之色素分解、或劣化之虞。
又,即便對光硬化型丙烯酸接著劑照射紫外線後,欲將偏光板與顯示器基板重疊而接合,光硬化型丙烯酸接著劑之硬化反應亦迅速地完成,並固化。因此,有變得無法將偏光板與顯示器基板接合之問題。
由於光硬化型丙烯酸接著劑具有上述問題點,故而正研究使用感壓型黏著劑之方法。由於感壓型黏著劑為低彈性模數,故而可藉由常溫且短時間之加壓而接著,亦可不進行硬化而將偏光板與顯示器基板貼合。然而,於該情形時,若將可彎折之顯示器之撓曲次數增加,則有撓曲部之接著劑(感壓型黏著劑)之厚度因低彈性模數而變動之可能性。因此,亦提出有如下之光硬化型接著片:藉由事先利用可見光進行聚合之丙烯酸黏著劑成分,而即便為初期狀態亦顯示出充分之感壓接著性,並藉由貼合時之紫外光照射,未反應之環氧化合物硬化,表現出充分之接著強度(例如,參照專利文獻2)。
此外,亦正研究使用液狀接著劑之方法。然而,液狀接著劑於輥貼合時剩餘之接著劑溢出而污損設備等。又,產生氣泡之捲入或難以取得接著劑層之厚度之均勻性等問題點。因此,為了防止因加熱或撓曲等導致之龜裂之產生,亦提出有含有多官能陽離子聚合性低聚物、分子量超過10萬之陽離子聚合性聚合物、及硬化劑的硬化性樹脂片(例如,參照專
利文獻3)。
[先前技術文獻]
[專利文獻]
[專利文獻1]日本特開2015-180968號公報
[專利文獻2]日本特開平10-306140號公報
[專利文獻3]國際公開第15/087807號
本發明之課題在於提供一種滿足用以將具有遮光性(尤其是紫外線遮光性)之構件貼合於可彎折之顯示器之各種性能的接著劑組成物、使用其之黏附體之接合方法及積層體之製造方法。
即,提供一種可於塗佈接著劑組成物時藉由噴霧或噴墨塗佈等各種方法而塗佈於黏附體,且所塗佈之接著劑組成物對黏附體之凹凸追隨性優異的接著劑組成物。又,提供一種塗佈後藉由紫外線照射而抑制接著劑組成物之滴液或塗佈厚度之變動,確保充分之適用時間(利用光照射之接著劑組成物之硬化開始後,可作業之時間)的接著劑組成物。進而,本發明之課題在於提供一種於硬化後追隨於各種黏附體而彎曲、不剝離之接著劑組成物。本發明之課題在於進而提供一種藉由使用上述各種性能優異之接著劑組成物,而於顯示器等可彎折之構件之製作中,可有效率地進行各種黏附體(尤其是具有遮光性之構件)之接合的黏附體之接合方法及將黏附體接合而成之積層體之製造方法。
本發明者等人發現:含有作為特定化合物之聚環氧烷(polyalkylene oxide)加成多官能環氧化合物及多官能(甲基)丙烯酸酯單體以及光酸產生劑(photo acid generator)的接著劑組成物,可於將具有遮光性之構件貼合於可彎折之顯示器時較佳地使用。即,發現:由於為液狀之接著劑組成物,故而可藉由各種塗佈法而塗佈於黏附體及對黏附體之凹凸追隨性優異,藉由塗佈後之光照射而抑制接著劑組成物之滴液或塗佈厚度之變動及可確保充分之適用時間,且硬化完成後之接著劑組成物追隨於各種黏附體而彎曲、不剝離。本發明係基於該等見解而成者。
即,根據本發明,提供以下之手段。
[1]
一種接著劑組成物,其係含有下述通式(A)所表示之環氧烷加成多官能環氧化合物(a)、多官能(甲基)丙烯酸酯單體(b)及光酸產生劑(c)而成:
(上述式中,R表示碳數1~4之伸烷基,X表示具有環狀結構之碳數6~20之二價之連結基或碳數1~4之伸烷基;m及n分別獨立地為0或正數)。
[2]
如[1]所記載之接著劑組成物,其中,上述接著劑組成物中之上述多官
能(甲基)丙烯酸酯單體(b)之含量為20質量%以下。
[3]
如[1]或[2]所記載之接著劑組成物,其係含有具有環氧乙烷環以外之環狀結構的單官能環氧化合物(d)而成。
[4]
一種黏附體A與B之接合方法,其依序包含下述步驟A及B:步驟A:於上述黏附體A塗佈[1]至[3]中任一項所記載之接著劑組成物之步驟;及步驟B:(i)藉由照射使上述光酸產生劑(c)活化之光,而使上述接著劑組成物之於25℃之黏度增黏至1Pa.s以上之步驟,及(ii)於上述經增黏之接著劑組成物上貼合上述黏附體B之步驟。
[5]
一種將黏附體A與B接合而成之積層體之製造方法,其依序包含下述步驟A及B:步驟A:於上述黏附體A塗佈[1]至[3]中任一項所記載之接著劑組成物之步驟;及步驟B:(i)藉由照射使上述光酸產生劑(c)活化之光,而使上述接著劑組成物之於25℃之黏度增黏至1Pa.s以上之步驟,及(ii)於上述經增黏之接著劑組成物上貼合上述黏附體B之步驟。
於本說明書中,所謂(甲基)丙烯酸酯,可為甲基丙烯酸酯及丙烯酸酯之任一種,係以該等之總稱而使用。因此,亦包括甲基丙烯酸酯及丙烯酸酯之任一者之情形或該等之混合物。
於本說明書中,於以特定之符號所表示之取代基或連結基等存在複數個時,或將複數個取代基等(取代基個數之規定亦同樣)同時或選取其一而規定時,各取代基等可彼此相同亦可不同。
於本說明書中,使用「~」所表示之數值範圍係指包含於「~」前後所記載之數值作為下限值及上限值之範圍。
本發明之接著劑組成物係於塗佈接著劑組成物時,可藉由噴霧或噴墨塗佈等各種方法而塗佈於黏附體,且所塗佈之接著劑組成物對黏附體之凹凸追隨性優異。塗佈後藉由紫外線照射而抑制接著劑組成物之滴液或塗佈厚度之變動。進而可提供於硬化後追隨於各種黏附體而彎曲、不剝離之接著劑組成物。又,本發明藉由使用上述各種性能優異之接著劑組成物,而可提供可於顯示器等可彎折之構件之製作中,有效率地進行各種黏附體之接合的黏附體之接合方法及將黏附體接合而成之積層體之製造方法。
關於本發明之上述及其他特徵及優點,將適宜參照隨附之圖式由下述之記載而變得更明確。
1‧‧‧經接著之膜
2‧‧‧構件(黏附體A)
3‧‧‧硬化體(硬化完成後之接著劑組成物)
4‧‧‧構件(黏附體B)
5‧‧‧鐵軸
圖1係表示於本發明之實施例中所製作之經接著之膜之縱剖面圖。
圖2係於本發明之實施例中進行[試驗例3]撓曲強度之評價之心軸撓曲試驗之說明圖。於該圖中,圖2(a)係表示自鐵軸之軸線方向觀察沿著鐵
軸將試驗用膜對半彎折之狀態之側面圖,圖2(b)係表示立體圖。
<接著劑組成物>
本發明之接著劑組成物含有聚環氧烷加成多官能環氧化合物(a)、多官能丙烯酸酯單體(b)及光酸產生劑(c)。
由於本發明之接著劑組成物於光(較佳為紫外線,於下文中亦相同)照射前為低黏度,故而可藉由噴霧或噴墨塗佈等各種方法而塗佈於黏附體。又,所塗佈之接著劑組成物對黏附體之凹凸追隨性優異。進而,由於本發明之接著劑組成物係藉由紫外線照射而開始之硬化反應緩慢進行(即,具有延遲硬化性)之延遲硬化型接著劑,故而於紫外線照射後亦可確保充分之適用時間(利用光照射之接著劑組成物之硬化開始後,可作業之時間),且可藉由加熱而加快硬化反應。因此,例如可於在顯示器基板表面塗佈本發明之接著劑組成物後對接著劑組成物進行紫外線照射,其後,將偏光板與進行了紫外線照射之接著材組成物貼合,進而進行加熱,藉此將兩者貼合。因此,可實現透光性較低之基板或構件之貼合。又,亦可將本發明之接著劑組成物塗佈於貼合用構件,進行使光酸產生劑活化之光照射後,於其適用時間內將構件貼合於顯示器基板,故而於構件貼合時顯示器暴露於紫外線或熱下之程度減輕,可減輕對顯示器基板造成之損傷。
以下,對本發明之接著劑組成物中之各成分進行說明。
(聚環氧烷加成多官能環氧化合物(a))
本發明中所使用之聚環氧烷加成多官能環氧化合物(a)係以下述通式
(A)所表示。
(上述式中,R表示低級伸烷基(例如較佳為碳數1~4之伸烷基),X表示具有環狀結構之碳數6~20之二價之基或低級伸烷基(例如較佳為碳數1~4之伸烷基);m及n分別獨立地為0或正數)
R之碳數更佳為2或3,最佳為2。作為R之碳數1~4之伸烷基,例如可列舉:亞甲基、伸乙基、1,2-伸丙基、1,3-伸丙基、1,4-伸丁基、2,4-伸丁基,較佳為伸乙基、1,3-伸丙基,更佳為伸乙基。
R為伸乙基之聚環氧乙烷加成環氧化合物可表現出良好之延遲硬化性。R為1,3-伸丙基之聚丙二醇加成環氧化合物係藉由甲基之立體效應而表現出低於聚環氧乙烷加成環氧化合物之延遲硬化性。
此處,本發明中所使用之聚環氧烷加成多官能環氧化合物(a)亦可為環氧烷結構之重複數不同之上述通式(A)所表示之化合物之混合物。於該情形時,由於將上述通式(A)所表示之化合物1分子中之環氧烷結構之推定平均重複數表示為m+n,故而有m+n不取整數之情況。再者,推定平均重複數可藉由利用不易引起試樣之破碎之柔軟之離子化的質量分析法(例如,FAB(fast atom bombardment)質量分析法)而算出。
就表現出良好之延遲硬化之觀點而言,m+n較佳為12以下,更佳為10以下,進而較佳為8以下。又,就表現出硬化完成後之接著劑組成物(以下,簡稱為硬化體)之良好之撓曲性之觀點而言,m+n較佳為2以上,更
佳為4以上,進而較佳為6以上。
作為X之碳數1~4之伸烷基,可較佳地應用R之碳數1~4之伸烷基之記載。
X之具有環狀結構之碳數6~20之二價之連結基之碳數較佳為6~18,更佳為6~15。又,作為構成原子,可列舉碳原子、氧原子、氮原子等,較佳為碳原子。
作為環狀結構,亦可為芳香族環及脂肪族環中之任一種。作為芳香族環,較佳為碳數6~14,例如較佳為苯環。作為脂肪族環,較佳為碳數3~14,例如較佳為環己烷環。
作為X之具有環狀結構之碳數6~20之二價之連結基,就硬化體中之自由體積較大,可形成較大空隙之方面而言,較佳為具有環己烷結構、下述通式(Aa)所表示之雙酚型結構、二環戊二烯結構、及其等之氫化體結構的連結基。
(上述式中,R1表示烷基(碳數較佳為1~10,更佳為1~3,進而較佳為1),R2表示氫原子、烷基(碳數較佳為1~5,更佳為1~3,進而較佳為1)或環烷基(碳數較佳為3~5,更佳為3);p為0~4之整數(較佳為0或1,更佳為0);*表示鍵結部)
其中,於上述通式(Aa)中,較佳為R2為甲基且p為0之
二價之連結基,即雙酚-A型之連結基。
此處,作為環氧系接著劑而廣泛使用之雙酚A二環氧丙醚或雙酚F二環氧丙醚等由於不具有聚環氧烷結構,故而使用該等之接著劑組成物之硬化體不會顯示出充分之撓曲性,且接著劑組成物不表現出延遲硬化。
就提高本發明之接著劑組成物及硬化體對黏附體之追隨性之觀點而言,聚環氧烷加成多官能環氧化合物(a)之分子量或重量平均分子量較佳為1,000以下,更佳為800以下,進而較佳為600以下。下限值並無特別限制,較佳為300以上,更佳為400以上。
再者,重量平均分子量例如可使用Waters公司製造之GPC系統(管柱:昭和電工公司製造之「Shodex K-804(商品名)」(聚苯乙烯凝膠),移動相:氯仿),藉由凝膠滲透層析法(GPC)以聚苯乙烯換算之分子量之形式而測定(或算出)。
作為可當作市售品而獲得之聚環氧烷加成多官能環氧化合物(a),例如可列舉:新日本理化公司製造之商品名「RIKARESIN BPO-20E(分子量457)」、「RIKARESIN BEO-60E(分子量541)」等「RIKARESIN」系列。
接著劑組成物中之聚環氧烷加成多官能環氧之含量較佳為5質量%~90質量%。就硬化體之良好之耐撓曲性之觀點而言,更佳為20質量%以上,進而較佳為35質量%以上。又,就對黏附體之塗佈性之觀點而言,更佳為70質量%以下,進而較佳為60質量%以下。
(多官能(甲基)丙烯酸酯單體(b))
本發明中所使用之多官能(甲基)丙烯酸酯單體(b)係於1分子中具有
兩個以上之聚合性基。因此,本發明之接著劑組成物顯示出由光照射所得之較高增黏性。此處,所謂聚合性基,意指可藉由光酸產生劑(c)而進行光自由基聚合之基,具體可列舉乙烯基、(甲基)丙烯醯基等具有碳-碳不飽和雙鍵之基。再者,單官能之(甲基)丙烯酸酯單體無法獲得由光(紫外線)照射所得之充分之增黏效果。
多官能(甲基)丙烯酸酯單體1分子中之聚合性基之個數較佳為2~4個,更佳為2或3個,進而較佳為2個。其中,尤佳為於1分子中具有2個(甲基)丙烯醯基之多官能(甲基)丙烯酸酯單體。
又,多官能(甲基)丙烯酸酯單體亦較佳為於分子中具有體積大之結構。作為體積大之結構,可列舉:環己烷骨架或二環戊二烯骨架、雙酚-A骨架、及其等之氫化體等。上述具有體積大之結構之多官能(甲基)丙烯酸酯單體即便為少量,增黏效果亦較大。
另一方面,1,6-己二醇二丙烯酸酯或1,9-壬二醇二丙烯酸酯等不含體積大之結構且於分子內具有直鏈烯烴結構之多官能(甲基)丙烯酸酯單體係由光(紫外線)照射所得之增黏效果較小,照射後之黏度上升平穩。再者,與上述不具有體積大之結構且於分子內具有直鏈烯烴結構之多官能(甲基)丙烯酸酯單體相比,上述於分子內具有體積大之結構之多官能(甲基)丙烯酸酯單體對聚環氧烷加成多官能環氧化合物(a)之相容性良好,故而較佳。若對聚環氧烷加成多官能環氧化合物(a)之相容性良好,則可抑制硬化體中之相分離。
又,關於本發明中所使用之多官能(甲基)丙烯酸酯單體,就提高儲藏穩定性之方面而言,較佳為與環氧基為非反應性之化合物。即,
不具有容易與環氧基反應之羥基、羧基或酸酐骨架之情況下,藉由長期保管而可抑制接著劑組成物之黏度上升,故而較佳。
關於接著劑組成物中之多官能(甲基)丙烯酸酯單體之含量,就藉由光(紫外線)照射後之增黏而製備成不引起滴液之黏度之方面而言,下限值較佳為1質量%以上。就於塗佈後藉由多官能(甲基)丙烯酸酯單體之效果而抑制接著劑組成物之厚度變動之方面而言,更佳為2質量%以上,進而較佳為5質量%以上。又,就抑制硬化體中之相分離之產生之方面而言,上限值較佳為20質量%以下。就確保對黏附體之充分之凹凸追隨性之方面而言,上限值較佳為20質量%以下,更佳為15質量%以下。若多官能(甲基)丙烯酸酯單體之含量為上述較佳之上限值內,則可製備接著劑組成物不因紫外線照射而立即硬化、於光照射後可確保充分之適用時間之延遲硬化型之接著劑組成物。
關於多官能(甲基)丙烯酸酯單體之分子量,就與其他構成材料之相容性之觀點而言,較佳為150以上,更佳為200以上。就接著劑組成物之黏度之觀點而言,較佳為500以下,更佳為350以下。
(光酸產生劑(c))
可認為本發明中所使用之光酸產生劑係藉由光照射而吸收能量,由此光酸產生劑分解而產生布氏酸或路易斯酸、及自由基,(甲基)丙烯酸酯單體藉由該自由基而進行聚合,環氧基藉由陽離子而進行聚合。因此,於本發明中為了使(甲基)丙烯酸酯成分聚合,可於不進一步添加自由基產生劑之情況下使(甲基)丙烯酸酯成分聚合。
於具代表性之三芳基鋶鹽之情形時,可認為光酸產生劑之光
分解機制係藉由下述式而進行。下述式(1)及(2)表示光酸產生劑吸收光而發生分解之反應。下述式(3)及(4)表示自下述式(2)中所產生之Ar2S+‧烷烴類中奪取氫而產生酸之反應。下述式(5)及(6)表示下述式(2)中所產生之Ar‧之反應。再者,於下述式中,Ar表示芳基,X表示陰離子成分,YH表示烷烴類。
2Ar‧ → Ar-Ar (5)
Ar‧+YH → ArH+Y‧ (6)
尤其推測:本發明之接著劑組成物含有上述通式(A)所表示之聚環氧烷加成多官能環氧化合物(a)、多官能(甲基)丙烯酸酯單體(b)及光酸產生劑(c),故而藉由光照射而進行以下之反應,由此可確保充分之適用時間。
即,藉由光照射而光酸產生劑(c)分解,由此生成自由基與陽離子,自由基促進多官能(甲基)丙烯酸酯單體(b)之聚合,陽離子促進聚環氧烷加成多官能環氧化合物(a)或下述具有環氧乙烷環以外之環狀結構之單官能環氧化合物(d)之聚合。此處,多官能(甲基)丙烯酸酯單體(b)係因利用光照射之自由基聚合極速進行而高分子量化。因此,使本發明之接著劑組成物之黏度適度上升。另一方面,聚環氧烷加成多官能環氧化合物(a)
由於陽離子聚合於常溫下緩慢進行,故而並不會較大地有助於本發明之接著劑組成物之黏度上升。因此,本發明之接著劑組成物可確保充分之適用時間。
進而推測:多官能(甲基)丙烯酸酯單體(b)藉由光照射而進行自由基聚合,藉由將塗佈有滴液或厚度變動得到抑制之本發明之接著劑組成物的黏附體、與其他黏附體貼合後進行加熱,而促進聚環氧烷加成多官能環氧化合物(a)之陽離子聚合而進行聚合、硬化,使黏附體接合。
光酸產生劑較佳為於本發明之接著劑組成物中含有0.1~10質量%。為了獲得充分之硬化度,較佳為0.5質量%以上。又,於要求透明性之用途中,就抑制由光酸產生劑所致之著色之方面而言,較佳為5質量%以下。
光酸產生劑係主要由鎓離子(陽離子成分)與非親核性之陰離子成分構成之鹽。
作為陽離子成分,例如可列舉:銨化合物離子、吡啶鎓化合物離子、三苯基鏻化合物離子等週期表第15族元素之離子,鋶化合物離子(包括三芳基鋶離子、芳香族鋶化合物離子、脂肪族鋶化合物離子等)、硒鎓化合物離子等第16族元素之離子,二芳基氯化合物離子、溴鎓離子、錪離子等第17族元素之離子及鐵-芳烴(arene)錯合物。
其中,較佳為錪離子、鋶化合物離子、銨化合物離子等離子成分,更佳為鋶化合物離子,就作為鹽之熱穩定性優異之方面而言,進而較佳為三芳基鋶離子。
鋶鹽系光陽離子聚合起始劑之光吸收範圍於甲醇溶液中為
360nm附近為止。因此,藉由在使本發明之接著劑組成物進行硬化時,將360nm以上之紫外線阻斷而進行光照射,可降低對吸收360nm以上之波長之色素之影響,而較佳。
作為陰離子成分,可列舉:BF4 -、B(C6F5)4 -、Ga(C6F5)4 -、PF6 -、PF1Rf(6-1) -(Rf:全氟烷基,1=0~5之整數)、AsF6 -、SbF6 -等週期表第13族及第15族元素之過氟化物(超強酸之陰離子殘基)。
其中,較佳為SbF6 -、PF6 -、PF1Rf(6-1) -及Ga(C6F5)4 -。
由於光酸產生劑為鹽,故而就對有機化合物之溶解性之觀點而言,較佳為芳基鋶鹽,更佳為於陰離子成分中使用過氟化物(尤佳為PF1Rf(6-1) -)而成之光酸產生劑。
作為光酸產生劑之市售品,可列舉:CPI-100P、CPI-101A、CPI-110S、CPI-200K、CPI-210S及CPI-500K(均為商品名,三芳基鋶鹽,SAN-APRO公司製造),Adeka Optomer SP系列(商品名,芳香族鋶鹽,ADEKA公司製造),CP系列(商品名,脂肪族鋶鹽,ADEKA公司製造),K-PURE(註冊商標)TAG及CXC系列(均為商品名,KING INDUSTRIES公司製造),San-Aid SI系列、SI-150L、SI-110L、SI-60L、SI-80L及SI-100L(均為商品名,芳香族鋶鹽,三新化學工業公司製造)。
(具有環氧乙烷環以外之環狀結構之單官能環氧化合物(d))
本發明之接著劑組成物進而含有:具有環氧乙烷環以外之環狀結構之單官能環氧化合物(d)亦就提高剝離接著力之觀點而言較佳。
該具有環氧乙烷環以外之環狀結構之單官能環氧化合物(d)之分子量
較佳為150以上。上限值並無特別限制,較佳為1,000以下,由於接著劑組成物之黏度降低,故而更佳為500以下。
作為環氧乙烷環以外之環狀結構,亦可為單環式化合物、多環式化合物之任一種,更佳為多環式化合物。又,亦較佳為含有雜原子(例如氧原子、氮原子、硫原子、硒原子)作為構成環狀結構之原子,具有雜環式化合物之結構作為環氧乙烷環以外之環狀結構之情況下,藉由雜原子而接著力提高,故而較佳。
構成環狀結構之原子數較佳為3~20,更佳為5~18,進而較佳為6~16。
具體可列舉:苯環、聯苯環、鄰苯二甲酸骨架等。
作為此種具有環氧乙烷環以外之環狀結構之單官能環氧化合物(d),可列舉:日油股份有限公司製造之「EPIOL TB(對第三丁基苯基環氧丙醚;分子量206)」,阪本藥品工業股份有限公司製造之「PGE(苯基環氧丙醚;分子量152)」、「SY-OCG(鄰甲酚基環氧丙醚;分子量180」、「m,p-CGE(間對甲酚基環氧丙醚;分子量165)」及「SY-OPG(鄰苯基苯酚環氧丙醚;分子量230)」,三光股份有限公司製造之「OPP-G(2-苯基苯酚環氧丙醚;分子量226)」,Nagase chemtex股份有限公司製造之「EX-142(2-苯基苯酚環氧丙醚;分子量226)」及「EX-731(N-環氧丙基鄰苯二甲醯亞胺;分子量203)」等。此處,「 」表示商品名,( )表示化合物名。
本發明之接著劑組成物中之具有環狀結構之單官能環氧化合物(d)之含量較佳為5質量%~70質量%。就防止撓曲時之剝離之觀點而言,更佳為15質量%以上,進而較佳為25質量%以上。就防止由添加單
官能環氧化合物(d)所致之硬化體之強度降低及凝集破壞之觀點而言,更佳為60質量%以下,進而較佳為50質量%以下。
(添加劑)
於本發明中,可進而以無損本發明之接著劑組成物之效果之範圍之量適宜使用各種添加劑。
例如,為了對硬化體賦予柔軟性,亦可適宜摻合分子量為1,000~100,000之聚丁二烯等聚烯烴末端經由胺酯鍵、酯鍵或醚鍵而(甲基)丙烯酸酯化之(甲基)丙烯酸酯化合物作為柔軟性賦予劑。關於該等聚烯烴之(甲基)丙烯酸酯化合物之含量,就相容性之觀點而言,較佳為本發明之接著劑組成物中30質量%以下。
作為市售之柔軟性賦予劑,例如可列舉:CN307、CN308、CN309、CN310及CN9014(均為商品名,Arkema公司製造),TEAI-1000、TE-2000及EMA3000(均為商品名,日本曹達公司製造),BAC-45及SPBDA-S30(均為商品名,大阪有機化學工業公司製造)、DENALEX R-45EPT(商品名,Nagase chemtex股份有限公司製造)。
進而,亦可適宜添加低分子之黏著賦予劑。
作為黏著賦予劑,可使用:天然樹脂之松香、萜烯樹脂或將松香進行聚合、改質而成之聚合松香、松香酯、氫化松香或石油樹脂等。
此外,亦可適宜摻合光自由基聚合起始劑、熱陽離子聚合起始劑、稀釋劑、塑化劑、交聯助劑、消泡劑、難燃劑、聚合抑制劑、填料、偶合劑等添加劑。
使用本發明之接著劑組成物時之硬化條件、適用時間可較佳
地應用下述黏附體之接合方法及積層體之製造方法中之記載。
本發明之接著劑組成物之製備方法並無特別限定,例如可藉由摻合上述通式(A)所表示之聚環氧烷加成多官能環氧化合物(a)、多官能(甲基)丙烯酸酯單體(b)及光酸產生劑(c)及添加劑,並攪拌直至變均勻等常法而製備。再者,為了防止光酸產生劑(c)之分解,較佳為於遮光條件下進行製備。
又,為了防止光酸產生劑(c)之分解,製備後之本發明之接著劑組成物亦較佳為進行遮光而保存。
<黏附體之接合方法>
使用本發明之接著劑組成物之黏附體A與B之接合方法依序包含下述步驟A及B。
步驟A:於黏附體A塗佈本發明之接著劑組成物之步驟
步驟B:(i)藉由照射使光酸產生劑(c)活化之光,而使接著劑組成物之於25℃之黏度增黏至1Pa.s以上之步驟,及(ii)於經增黏之接著劑組成物上貼合黏附體B之步驟
藉由本發明之黏附體之接合方法,可獲得具有黏附體A(2)/經硬化之接著劑組成物(硬化體3)/黏附體B(4)之積層結構的圖1之經接著之膜(1)。
<積層體之製造方法>
使用本發明之接著劑組成物將黏附體A與B接合而成之積層體之製造方法依序包含下述步驟A及B。
步驟A:於黏附體A塗佈本發明之接著劑組成物之步驟
步驟B:(i)藉由照射使光酸產生劑(c)活化之光,而使接著劑組成物之於25℃之黏度增黏至1Pa.s以上之步驟,及(ii)於經增黏之接著劑組成物上貼附黏附體B之步驟
藉由本發明之積層體之製造方法,可獲得具有黏附體A(2)/經硬化之接著劑組成物(硬化體3)/黏附體B(4)之積層結構的圖1之積層體(經接著之膜1)。
以下,對黏附體之接合方法及積層體之製造方法中記載之黏附體A及B以及步驟(A)及(B)詳細地說明。
作為黏附體A及B之構件,可藉由本發明之接合方法將由聚對苯二甲酸乙二酯(PET)、聚萘二甲酸乙二酯(PEN)、聚醯亞胺(PI)、環烯烴聚合物(COP)、環烯烴-共聚物(COC)、玻璃、金屬箔等原材料構成之構件或觸控面板、彩色濾光片、偏光板、保護膜、顯示器基板、軟性印刷基板、柔軟性電池等構件接著。其中,黏附體A及B為具有撓曲性之構件,於將遮光性之構件進行接合時,進一步發揮藉由使用本發明之接著劑組成物之接合方法及製造方法之效果,例如,可較佳地用於可彎折之顯示器基板與構件之接合及將該等接合而成之積層體之製造。
(步驟A)
對黏附體A之本發明之接著劑組成物之塗佈可藉由常法進行。尤其由於本發明之接著劑組成物為低黏度之液狀,故而可較佳地使用狹縫式塗佈或噴墨方式、噴霧方式、滴塗方式等。此處,所謂本發明之接著劑組成物為液狀,意指於5℃~200℃時為液狀(較佳為0.01Pa.s~50Pa.s)。又,就對黏附體A塗佈本發明之接著劑組成物後,於步驟B中貼合黏附體B之觀
點而言,所謂本發明之接著劑組成物為液狀,意指不含溶劑之狀態下之接著劑組成物為液狀。
本發明之接著劑組成物之塗佈厚度係根據目的而適宜選擇,於適合於以撓曲為目的之構件之情形時,塗佈厚度較薄之情況下,於撓曲之內側與外側產生之應力變形減小,不易剝離,故而較佳。具體而言,塗佈厚度較佳為100μm以下,更佳為50μm以下。又,就對黏附體A及B之凹凸追隨性之方面而言,較佳為塗佈厚度較厚。具體而言,較佳為2μm以上,更佳為10μm以上。
(步驟B)
(i)使光酸產生劑(c)活化之光之照射條件可根據接著劑組成物中之光酸產生劑(c)之含量、接著劑組成物之塗佈厚度、接著劑組成物中所含有之水分量等而適宜選擇,就可獲得充分之適用時間之方面而言,可較佳地列舉如下之條件。
即,較佳為將照射強度(光輸出)5~100mW/cm2、照射量100~5,000mJ/cm2之紫外線照射至塗佈於黏附體A之本發明之接著劑組成物。
於欲加快硬化速度之情形時,亦較佳為於紫外線照射後,於(ii)黏附體B之貼合後進而加熱,該形態亦係作為步驟B而較佳之態樣。加熱溫度較佳為50~150℃,加熱時間較佳為0.5~24小時。加熱可藉由常法而進行,例如可使用加熱爐進行加熱。
藉由將紫外線照射量設為上述範圍內,可於不使黏附體等之周邊材料劣化之情況下獲得充分硬度之硬化體,故而較佳。就排除存在於空氣中或黏附體表面之水分或具有硬化阻礙特性之物質之影響,穩定地獲得硬化體
之方面而言,照射量更佳為1,000mJ/cm2以上。
塗佈於黏附體A後之本發明之接著劑組成物係藉由光照射而使接著劑組成物之於25℃之黏度(以下,稱作黏度(25℃))增黏至1Pa.s以上。藉此,亦可於塗佈後之接著劑組成物之厚度不因由於接著劑組成物塗佈後之移動(搬送)等所產生之振動等而變動之情況下,均勻地保持黏附體A與B之貼合厚度。結束光照射後,0.5分鐘後(較佳為1分鐘後)之黏度(25℃)較佳為1Pa.s以上。就以良好之凹凸追隨性於黏附體B加熱貼合之觀點而言,結束光照射後,0.5分鐘後(較佳為1分鐘後)之黏度(25℃)較佳為1,000Pa.s以下,就不加熱而以良好之凹凸追隨性貼合於黏附體B之觀點而言,結束光照射後,0.5分鐘後(較佳為1分鐘後)之黏度(25℃)更佳為100Pa.s以下。再者,較佳為結束光照射後,至6小時後之黏度為上述上限值以下。
此處,所謂黏度,係指藉由實施例中記載之裝置、方法所測定之複黏度n*。
所謂本發明之接合方法及製造方法之適用時間(利用光照射之接著劑組成物之硬化開始後可作業之時間),即,係指結束步驟B之(i)光照射後至可進行(ii)黏附體B之貼合之時間。雖然根據光照射之條件、接著劑組成物之塗佈厚度而不同,但本發明之適用時間為0.5分鐘~6小時,可於黏附體A與B之貼合時確保良好之作業性。
(ii)於接著劑組成物上之黏附體B之貼合係於(i)藉由光照射而使塗佈於黏附體A之接著劑組成物增黏後進行。此處,於黏附體A及B之任一者為透光性之情形時,亦可於塗佈本發明之接著劑組成物後,
經由所塗佈之接著劑組成物將黏附體A與B貼合,自透光性黏附體側進行光照射,進行加熱而接著。
當然,於遮光性之構件、或含有光反應性之化合物之黏附體(構件)之貼合時,亦可較佳地應用。
根據本發明之黏附體之接合方法,亦可對具有黏附體A(2)/經硬化之接著劑組成物(硬化體3)/黏附體B(4)之積層結構的圖1之經接著之膜(1),於黏附體A及/或B上進而接合1個或2個以上之黏附體。
又,根據本發明之積層體之製造方法,亦可製造對具有黏附體A(2)/經硬化之接著劑組成物(硬化體3)/黏附體B(4)之積層結構的圖1之積層體(經接著之膜1),於黏附體A及/或B上進而經由硬化體3貼合1個或2個以上之黏附體而成之積層體。
[實施例]
以下,根據實施例進而詳細地說明本發明,但本發明並不限定於此。
[實施例1]
以表1之質量比摻合作為聚環氧烷加成多官能環氧化合物(a)之RIKARESIN BEO-60E(商品名,新日本理化公司製造)、作為多官能(甲基)丙烯酸酯單體(b)之A-NOD-N(商品名,新中村化學工業公司製造)、作為光酸產生劑(c)之CPI-200K(商品名,SAN-APRO公司製造),攪拌直至變均勻而製備接著劑組成物。
將所製備之接著劑組成物以成為厚度20μm之方式塗佈於厚度25μm之PET膜(商品名「G2」,Teijin Dupont股份有限公司製造),使用紫外線照
射裝置(商品名:US5-0151,EYE GRAPHICS公司製造),以50mW/cm2照射60秒(照射量:2000mJ/cm2)紫外線。進而,於結束紫外線照射後1小時後,於所塗佈之接著劑組成物上貼合厚度25μm之PET膜(商品名「G2」,Teijin Dupont股份有限公司製造)。將以如此之方式所獲得之經2片PET膜所夾持之接著劑組成物投入至90℃之加熱爐中60分鐘,獲得以硬化完成後之接著劑組成物(3)將2片PET膜接著而成之具有圖1中記載之構成之經接著之膜(1)。將以如此之方式所獲得之經接著之膜切割為25mm×100mm,用作以下之試驗用膜。
[實施例2~10、比較例1~3]
於實施例1中,將接著劑組成物之成分代替為下述表1中記載之種類、質量摻合比,除此以外,以與實施例1相同之方式,製備實施例2~10、比較例1~3之接著劑組成物。使用所獲得之接著劑組成物,除此以外,以與實施例1相同之方式,獲得具有圖1中記載之構成之經接著之膜(1)、及試驗用之膜。
此處,實施例1~10中所製備之接著劑組成物均於23℃為液狀。
[試驗例1]增黏特性評價
將上述所製備之接著劑組成物以厚度20μm塗佈於厚度25μm之PET膜(商品名「G2」,Teijin Dupont股份有限公司製造),使用紫外線照射裝置(商品名:US5-0151,EYE GRAPHICS公司製造),以50mW/cm2照射60秒(照射量:2000mJ/cm2)紫外線。對於紫外線照射後之接著劑組成物,於動態黏彈性測定裝置(裝置名「ARES」,Rheometric Scientific公司製造)中,使用圓錐直徑25mm、圓錐角度0.1rad之錐板,以剪切速度1s-1之角速度
於常溫(25℃)下結束紫外線照射後,測定1分鐘後之複黏度n*。將紫外線照射後之複黏度n*未達1Pa.s者評價為「×」,將因黏度上升而成為1Pa.s以上者評價為「○」。
[試驗例2]剝離接著強度之評價
上述試驗用膜之剝離接著強度係依據JIS K6854-3(接著劑-剝離接著強度試驗方法-第3部:T形剝離)而測定。剝離接著強度係以「N/25mm」之形式測定。於下表中,省略單位而記載。
[試驗例3]撓曲強度之評價
撓曲強度係利用心軸撓曲試驗進行評價。將上述25mm×100mm之試驗用膜以成為25mm×50mm之方式,如圖2般沿著直徑1mm之鐵軸對半彎折,觀察龜裂及剝離之產生。將有龜裂及剝離之試片評價為「×」,將無龜裂及剝離之試片評價為「○」。
將試驗例1~3之結果示於下表。
<表之備註>
(A)環氧化合物
‧聚環氧烷加成多官能環氧化合物(a)
RIKARESIN BEO-60E:商品名,新日本理化公司製造,雙酚A雙(三乙二醇環氧丙醚)醚,分子量541
RIKARESIN BPO-20E:商品名,新日本理化公司製造,雙酚A雙(丙二醇環氧丙醚)醚,分子量457
Epolight 200E:商品名,共榮社化學公司製造,聚乙二醇#200二環氧丙醚,分子量322
Epogosey PT(通常等級):商品名,共榮社化學公司製造,聚乙二醇二環氧丙醚,分子量870
‧不具有聚環氧烷結構之環氧化合物
Epikote 828:商品名,三菱化學公司製造,雙酚A二環氧丙醚,分子量340
(B)(甲基)丙烯酸酯單體
‧多官能(甲基)丙烯酸酯單體(b)
A-DCP:商品名,新中村化學工業公司製造,三環癸烷二甲醇二丙烯酸酯,分子量304
A-HD-N:商品名,新中村化學工業公司製造,1,6-己二醇二丙烯酸酯,分子量226
A-NOD-N:商品名,新中村化學工業公司製造,1,9-壬二醇二丙烯酸酯,分子量268
‧單官能(甲基)丙烯酸酯單體
PLACCEL FM2D:商品名,Daicel公司製造,(單官能)不飽和脂肪酸羥基烷基酯改質ε-己內酯,分子量358
(C)光酸產生劑(c)
CPI-200K:商品名,SAN-APRO公司製造,三芳基鋶鹽(碳酸丙烯酯50wt%溶液)
(D)單官能環氧化合物
‧具有環狀結構之單官能環氧化合物(d)
PGE:商品名,阪本藥品工業公司製造,苯基環氧丙醚,分子量152
EX-731:商品名,Nagase chemtex公司製造,N-環氧丙基鄰苯二甲醯亞胺,分子量203
EPIOL TB:商品名,日油公司製造,對第三丁基苯基環氧丙醚,分子量206
OPP-G:商品名,三光公司製造,2-苯基苯酚環氧丙醚,分子量226
‧不具有環狀結構之單官能環氧化合物
Epolight M-1230:商品名,共榮社化學公司製造,高級醇環氧丙醚,分子量295~320
上述各試驗例之結果為,於使用不具有聚環氧烷結構之多官能環氧化合物之比較例1中,撓曲強度不足,於使用單官能(甲基)丙烯酸酯單體之比較例2及不含多官能(甲基)丙烯酸酯單體之比較例3中,均未獲得充分之增黏特性。
相對於此,可知本發明之接著劑組成物係增黏特性、剝離接著強度及
撓曲強度均優異。又,可藉由使用本發明之接著劑組成物之黏附體之接合方法,將遮光性之構件或含有光反應性之化合物之構件進行接合。可藉由使用本發明之接著劑組成物之積層體之製造方法,製造將遮光性之構件或含有光反應性之化合物之構件接合而成之積層體。
於實施例1~10中,將經紫外線照射之接著劑組成物上之PET膜之貼合由結束紫外線照射後1小時後代替為結束紫外線照射後0.5分鐘後,除此以外,以與實施例1~10同樣之方式,獲得具有圖1中記載之構成之經接著之膜(1)、及試驗用膜。可知,於試驗例1~3之任一者中,與使用將成分設為相同之接著劑組成物之各實施例相比,均分別可獲得同等水準之結果。
又可知,即便於將結束紫外線照射後之時間設為6小時後之情形時,與上述設為0.5分鐘後之情形同樣地,於試驗例1~3之任一者中,與使用將成分設為相同之接著劑組成物之各實施例相比,均分別可獲得同等水準之結果。
將本發明與其實施態樣一併進行了說明,但只要我等並未特別指定,則不欲將我等之發明限定於說明之任何細部,可認為,應於不違反隨附之申請專利範圍所示之發明之精神與範圍之情況下廣泛地解釋。
本發明案主張基於2015年12月18日於日本提出專利申請之日本專利特願2015-247963之優先權,其係在此參照並將其內容作為本說明書之記載之一部分而併入。
1‧‧‧經接著之膜
2‧‧‧構件(黏附體A)
3‧‧‧硬化體(硬化完成後之接著劑組成物)
4‧‧‧構件(黏附體B)
Claims (5)
- 一種接著劑組成物,其係含有下述通式(A)所表示之聚環氧烷(polyalkylene oxide)加成多官能環氧化合物(a)、多官能(甲基)丙烯酸酯單體(b)及光酸產生劑(c)而成;
- 如申請專利範圍第1項之接著劑組成物,其中,上述接著劑組成物中之上述多官能(甲基)丙烯酸酯單體(b)之含量為20質量%以下。
- 如申請專利範圍第1或2項之接著劑組成物,其係含有具有環氧乙烷環以外之環狀結構的單官能環氧化合物(d)而成。
- 一種黏附體A與B之接合方法,其依序包含下述步驟A及B:步驟A:於上述黏附體A塗佈申請專利範圍第1至3項中任一項之接著劑組成物之步驟;及步驟B:(i)藉由照射使上述光酸產生劑(c)活化之光,而使該接著劑組成物之於25℃之黏度增黏至1Pa.s以上之步驟,及(ii)於上述經增黏之接著劑組成物上貼合上述黏附體B之步驟。
- 一種將黏附體A與B接合而成之積層體之製造方法,其依序包含下述步驟A及B:步驟A:於上述黏附體A塗佈申請專利範圍第1至3項中任一項之接著劑組成物之步驟;及 步驟B:(i)藉由照射使上述光酸產生劑(c)活化之光,而使該接著劑組成物之於25℃之黏度增黏至1Pa.s以上之步驟,及(ii)於上述經增黏之接著劑組成物上貼合上述黏附體B之步驟。
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