TW202110636A - 附底漆之熱塑性樹脂材及樹脂－樹脂接合體 - Google Patents

附底漆之熱塑性樹脂材及樹脂－樹脂接合體 Download PDF

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TW202110636A
TW202110636A TW109126432A TW109126432A TW202110636A TW 202110636 A TW202110636 A TW 202110636A TW 109126432 A TW109126432 A TW 109126432A TW 109126432 A TW109126432 A TW 109126432A TW 202110636 A TW202110636 A TW 202110636A
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thermoplastic resin
resin material
functional
primer
aforementioned
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TW109126432A
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TWI810475B (zh
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大谷和男
沼尾臣二
高橋信行
新林良太
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日商昭和電工股份有限公司
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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
    • C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
    • C09D5/00—Coating compositions, e.g. paints, varnishes or lacquers, characterised by their physical nature or the effects produced; Filling pastes
    • C09D5/002—Priming paints
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C65/00—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor
    • B29C65/02—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure
    • B29C65/04—Dielectric heating, e.g. high-frequency welding, i.e. radio frequency welding of plastic materials having dielectric properties, e.g. PVC
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C65/00—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor
    • B29C65/02—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure
    • B29C65/06—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using friction, e.g. spin welding
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C65/02—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure
    • B29C65/08—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using ultrasonic vibrations
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C65/02—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure
    • B29C65/14—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using wave energy, i.e. electromagnetic radiation, or particle radiation
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Abstract

一種附底漆(primer)之熱塑性樹脂材，其係具有熱塑性樹脂材，與層合於前述熱塑性樹脂材之1層或複數層之底漆層，且前述底漆層之至少1層係使原位聚合型組成物在前述熱塑性樹脂材之上聚合而成之原位聚合型組成物層。

Description

附底漆之熱塑性樹脂材及樹脂－樹脂接合體
本發明係關於在強固熔接同種或異種之熱塑性樹脂材之用途上所適宜之附底漆之熱塑性樹脂材及其之製造方法、使用前述附底漆之熱塑性樹脂材之樹脂-樹脂接合體及其製造方法。
近年來基於製品之輕量化及低成本化等之觀點，從而頻繁地進行將汽車零件、醫療機器、家電製品等、各種領域之零件予以樹脂化而作成樹脂成形品。又，基於樹脂成形品之高生產性化等之觀點，諸多係採用預先將樹脂成形品分割成複數進行成形，並將該等之分割成形品互相接合之手段。
作為將由此種樹脂所構成之分割成形品互相接合之手段，係使用如機械性接合、接著劑接合、熔接。其中，熔接尤其係高信賴性且生產性有用之接合法。熔接係根據加熱樹脂構件之方法而有各種方法，具體而言，如有超音波熔接或振動熔接、熱熔接、熱風熔接、感應熔接、射出熔接等。
熔接一般係使用於接合同種熱塑性樹脂材之接合法，但接合強度則會根據熔接法或樹脂種類而有無法充分展現的情況。由於熔接時之母材損傷之影響，諸多情況例如只有原本母材強度之5~8成程度。因此，進行熔接法之改良。
關於同種之熱塑性樹脂材之接合，例如，專利文獻1已揭示藉由預先對聚丙烯進行電暈放電處理，而接合聚丙烯彼此之技術。
又，熔接也能可使用在接合溶解度參數(以下SP值)相近之異種之熱塑性樹脂材。 關於異種之熱塑性樹脂材之接合，例如，專利文獻2、3已揭示、在使熱塑性樹脂組成物成形而成之成形體，及，與前述成形體之熱塑性樹脂為異種之熱塑性樹脂之間隔著具有官能基之熱塑性片材與強化纖維束進行超音波熔接之技術。又，專利文獻4已揭示藉由在被熔接構件之間插入中間層並將該中間層固定在超音波共振器號角(ultrasonic resonator horn)上並使其振動來將兩被熔接構件進行超音波熔接之技術。 [先前技術文獻] [專利文獻]
[專利文獻1] 日本特開平8-126823號公報 [專利文獻2] 日本特開2017-202667號公報 [專利文獻3] 日本特開2017-206014號公報 [專利文獻4] 日本特開2008-284862號公報
[發明所欲解決之課題]
前述同種之熱塑性樹脂材之接合中，即使以專利文獻1之方法仍也無法確保充分之接合強度。
又，熔接之強度係藉由接合界面之分子擴散所成之分子糾纏與結晶化來展現。因此，以往在異種熱塑性樹脂材之接合中，熔接仍有無法取得充足接合強度的問題。
本發明係有鑑於該技術背景所完成者，其課題在於提供一種在強固地熔接同種之熱塑性樹脂材或異種之熱塑性樹脂材之用途所適宜之附底漆之熱塑性樹脂材及其之關聯技術。前述關聯技術係意指前述附底漆之熱塑性樹脂材之製造方法、使用前述附底漆之熱塑性樹脂材之樹脂-樹脂接合體及其之製造方法。 [用以解決課題之手段]
本發明為了達成前述目的，提供以下之手段。 尚且，本說明書中，接合係意指將物與物予以連接，且接著及熔接則為其之下位概念。接著係意指隔著膠帶或接著劑之各種有機材(熱硬化性樹脂或熱塑性樹脂等)，將2個被連接材(所欲接著者)作成接合狀態。熔接係意指藉由熱來熔融被連接材之熱塑性樹脂等之表面，並藉由接觸加壓與冷卻來利用由分子擴散所成之糾纏與結晶化而作成接合狀態。
(附底漆之熱塑性樹脂材) [1] 一種附底漆之熱塑性樹脂材，其係具有：熱塑性樹脂材，與層合於前述熱塑性樹脂材之1層或複數層之底漆層， 且前述底漆層之至少1層為使原位聚合型組成物在前述熱塑性樹脂材之上進行聚合而成之原位聚合型組成物層。 [2] 如[1]之附底漆之熱塑性樹脂材，其中前述原位聚合型組成物層係與前述熱塑性樹脂材直接接觸之層。 [3] 如[1]或[2]之附底漆之熱塑性樹脂材，其中前述原位聚合型組成物含有下述(1)~(7)之至少一種； (1)2官能異氰酸酯化合物與二醇之組合、 (2)2官能異氰酸酯化合物與2官能胺基化合物之組合、 (3)2官能異氰酸酯化合物與2官能硫醇化合物之組合、 (4)2官能環氧化合物與二醇之組合、 (5)2官能環氧化合物與2官能羧基化合物之組合、 (6)2官能環氧化合物與2官能硫醇化合物之組合、 (7)單官能自由基聚合性單體。 [4] 如[1]或[2]之附底漆之熱塑性樹脂材，其中前述原位聚合型組成物為一組成物包含：含有下述(1)~(7)之至少一種之組成物，以及，無水馬來酸改質聚丙烯或改質聚苯醚； (1)2官能異氰酸酯化合物與二醇之組合、 (2)2官能異氰酸酯化合物與2官能胺基化合物之組合、 (3)2官能異氰酸酯化合物與2官能硫醇化合物之組合、 (4)2官能環氧化合物與二醇之組合、 (5)2官能環氧化合物與2官能羧基化合物之組合、 (6)2官能環氧化合物與2官能硫醇化合物之組合、 (7)單官能自由基聚合性單體。 [5] 如[1]或[2]之附底漆之熱塑性樹脂材，其中前述原位聚合型組成物為一組成物包含：含有下述(1)~(7)之至少一種之組成物，以及，與構成前述熱塑性樹脂材之熱塑性樹脂為異種之熱塑性樹脂； (1)2官能異氰酸酯化合物與二醇之組合、 (2)2官能異氰酸酯化合物與2官能胺基化合物之組合、 (3)2官能異氰酸酯化合物與2官能硫醇化合物之組合、 (4)2官能環氧化合物與二醇之組合、 (5)2官能環氧化合物與2官能羧基化合物之組合、 (6)2官能環氧化合物與2官能硫醇化合物之組合、 (7)單官能自由基聚合性單體。 [6] 如[1]或[2]之附底漆之熱塑性樹脂材，其中前述原位聚合型組成物為一組成物包含：含有下述(1)~(7)之至少一種之組成物、無水馬來酸改質聚丙烯或改質聚苯醚，以及，與構成前述熱塑性樹脂材之熱塑性樹脂為異種之熱塑性樹脂； (1)2官能異氰酸酯化合物與二醇之組合、 (2)2官能異氰酸酯化合物與2官能胺基化合物之組合、 (3)2官能異氰酸酯化合物與2官能硫醇化合物之組合、 (4)2官能環氧化合物與二醇之組合、 (5)2官能環氧化合物與2官能羧基化合物之組合、 (6)2官能環氧化合物與2官能硫醇化合物之組合、 (7)單官能自由基聚合性單體。 [7] 如[3]~[6]中任一項之附底漆之熱塑性樹脂材，其中前述原位聚合型組成物含有前述(4)，且前述(4)之二醇為2官能酚化合物。 [8] 如[1]、[3]~[7]中任一項之附底漆之熱塑性樹脂材，其中前述底漆層係在前述原位聚合型組成物層與前述熱塑性樹脂材之間具有熱硬化性樹脂層，該熱硬化性樹脂層係由包含熱硬化性樹脂之組成物所形成而成。 [9] 如[8]之附底漆之熱塑性樹脂材，其中前述熱硬化性樹脂為選自由胺基甲酸酯樹脂、環氧樹脂、乙烯基酯樹脂及不飽和聚酯樹脂所成群之至少1種。
(附底漆之熱塑性樹脂材之製造方法) [10] 一種如[1]之附底漆之熱塑性樹脂材之製造方法，其係將已溶解於溶劑之前述原位聚合型組成物塗佈於前述熱塑性樹脂材之表面，並使前述原位聚合型組成物進行聚合。
(樹脂-樹脂接合體) [11] 一種樹脂-樹脂接合體，其係使如[1]~[9]中任一項之附底漆之熱塑性樹脂材之底漆層，與其他熱塑性樹脂材熔接而成。 [12] 如[11]之樹脂-樹脂接合體，其中前述其他熱塑性樹脂材為如[1]~[9]中任一項之附底漆之熱塑性樹脂材，並且係使各自之底漆層熔接而成。 [13] 如[11]或[12]之樹脂-樹脂接合體，其中構成前述其他熱塑性樹脂材之熱塑性樹脂且係構成該熱塑性樹脂之單體中佔最大含量之單體，與，構成如[1]~[9]中任一項之附底漆之熱塑性樹脂材之熱塑性樹脂且係構成該熱塑性樹脂之單體中佔最大含量之單體為相同，且該單體之含量皆為70質量%以上。
(樹脂-樹脂接合體之製造方法) [14] 一種如[11]~[13]中任一項之樹脂-樹脂接合體之製造方法，其係對前述附底漆之熱塑性樹脂材之底漆層，以選自由超音波熔接法、振動熔接法、電磁感應法、高頻法、雷射法、及熱壓法所成群之至少1種方法來熔接其他熱塑性樹脂材。 [15] 一種如[11]~[13]中任一項之樹脂-樹脂接合體之製造方法，其係對前述附底漆之熱塑性樹脂材之底漆層，以射出成形法來射出熔接其他熱塑性樹脂材。 [發明效果]
根據本發明，可提供在強固地熔接同種之熱塑性樹脂材或異種之熱塑性樹脂材之用途上所適宜之附底漆之熱塑性樹脂材及其之關聯技術。
詳述關於本發明之附底漆之熱塑性樹脂材及其之關聯技術。 尚且，本說明書中，「(甲基)丙烯醯基」係意指丙烯醯基及/或甲基丙烯醯基，又，「(甲基)丙烯酸酯」係意指丙烯酸酯及/或甲基丙烯酸酯。
[附底漆之熱塑性樹脂材] 如圖1所示，本實施形態之附底漆之熱塑性樹脂材1為具有熱塑性樹脂材2，與，層合於前述熱塑性樹脂材上之1層或複數層之底漆層3的層合體。圖1之情況，前述底漆層3之至少1層為使原位聚合型組成物在前述熱塑性樹脂材2之上進行聚合而成之原位聚合型組成物層31。 本發明中，原位聚合型組成物係意指藉由使特定之2官能化合物之組合在原位，即各種材料上，在觸媒存在下進行加成聚合反應，或，藉由特定單官能單體之自由基聚合反應，而形成熱塑性構造，即，線性聚合物構造之組成物。與在進行聚合時會構成由交聯構造所成之3次元網路的熱硬化性樹脂相異，原位聚合型組成物不會構成由交聯構造所成之3次元網路，而仍具有熱塑性。 前述原位聚合型組成物層31係以由包含原位聚合型苯氧基樹脂之組成物所形成而成之層為佳。原位聚合型苯氧基樹脂係指亦稱為熱塑性環氧樹脂，或原位硬化型苯氧基樹脂、原位硬化型環氧樹脂等之樹脂，藉由使2官能環氧樹脂與2官能酚化合物在觸媒存在下進行加成聚合反應而形成熱塑性構造，即，線性聚合物構造。
本發明中，如後述之圖3所示般，前述底漆層係指在將熱塑性樹脂材2，與另一方之接合對象物即其他熱塑性樹脂材5予以接合一體化而取得樹脂-樹脂接合體之際，存在於熱塑性樹脂材2與其他熱塑性樹脂材5之間，而使熱塑性樹脂材2對其他熱塑性樹脂材5之接合強度提升之層者。
本發明在前述其他熱塑性樹脂材5係為包含與構成前述熱塑性樹脂材2之熱塑性樹脂為同種熱塑性樹脂之熱塑性樹脂材時，則係適宜於將熱塑性樹脂材2與其他熱塑性樹脂材5予以強固熔接之用途上。又，在前述其他熱塑性樹脂材5係為包含與構成前述熱塑性樹脂材2之熱塑性樹脂為異種熱塑性樹脂之熱塑性樹脂材時，一般而言，熱塑性樹脂材2與其他熱塑性樹脂材5之SP值會遠離之情況為多，但仍也係適宜於將此種異種之熱塑性樹脂材予以強固熔接之用途上。 在此，本說明書中，「同種熱塑性樹脂」係意指構成熱塑性樹脂之單體中，佔最大含量之單體為相同，該單體之含量皆為70質量%以上之熱塑性樹脂。又，「異種熱塑性樹脂」係意指「同種熱塑性樹脂」以外之熱塑性樹脂，具體而言，意指不存在共通之單體之熱塑性樹脂、構成熱塑性樹脂之單體中佔最大含量之單體為相異之熱塑性樹脂，或，佔最大含量之單體為相同且至少一者之佔最大含量之單體含量為未滿70質量%之熱塑性樹脂。
＜熱塑性樹脂材2＞ 熱塑性樹脂材2之形態並無特別限定，可為塊狀亦可為薄膜狀。 構成熱塑性樹脂材2之熱塑性樹脂並非係受到特別限定者。 作為熱塑性樹脂，可舉出例如，聚丙烯(PP，SP值：8.0(J/cm3 )1/2 )、聚醯胺6(PA6，SP值：12.7-13.6(J/cm3 )1/2 )、聚醯胺66(PA66，SP值：13.6(J/cm3 )1/2 )、改質聚苯醚(m-PPE)、聚苯硫醚(PPS，SP值：19.8(J/cm3 )1/2 )、聚醚醯亞胺(PEI)、聚碳酸酯(PC，SP值：9.7(J/cm3 )1/2 )、聚對酞酸丁二酯(PBT，SP值：20.5(J/cm3 )1/2 )等。
在此，溶解度參數(SP值)係指、根據由希德布郎所導入之正規溶液理論來定義之提供材料間之相互作用程度之預測數值的值(δ)。 已提出有各種SP值之算出方法，例如，由Fedors (Polym.Eng.Sci.1974年,14卷,p147)所提出之手法，可使用下述式(1)來求出。 δ=(ΣEcoh /ΣV)1/2 ・・・(1) 在此，δ表示溶解度參數(J0.5 /cm1.5 )，Ecoh 表示凝聚能密度(J/mol)、V表示莫耳分子容積(cm3 /mol)，Σ係指對於構成單體之全部原子團，將賦予至各個原子團之該等數值取總和之意義。各個原子團之Ecoh 或V之數值係例舉在例如“聚合物物性，第3完整改版(Properties of Polymers, Third completely revised edition)”之Table7.3等。
＜底漆層3＞ 底漆層係層合在熱塑性樹脂材2之上而成。
[原位聚合型組成物層31] 如前述般，底漆層之至少1層係為使原位聚合型組成物在前述熱塑性樹脂材之上進行聚合而成之原位聚合型組成物層31。 原位聚合型組成物層31係可將溶解於溶劑之前述原位聚合型組成物塗佈於前述熱塑性樹脂材2之表面後，使前述原位聚合型組成物滲透於因前述溶劑之滲透而膨潤之前述熱塑性樹脂材2之表層上，使前述溶劑揮發並使前述原位聚合型組成物進行聚合而得。又，原位聚合型組成物層31係也可將包含前述原位聚合型組成物之乳液或包含前述原位聚合型組成物之粉體塗料塗佈於前述熱塑性樹脂材2之上，並在前述熱塑性樹脂材2之上使前述原位聚合型組成物進行聚合而得。並且，原位聚合型組成物層31係也可將溶解於溶劑之前述原位聚合型組成物，以乾燥後之厚度成為1~100μm之薄膜狀之方式塗布在離型薄膜上，在室溫~40℃之環境下放置，使溶劑揮發並同時使反應些許地進行並B階化，將取得之薄膜之與離型薄膜為反對側之面配置於前述熱塑性樹脂材2之上，從前述已B階化之薄膜剝離離型薄膜後，在40~150℃下進行加熱反應1~30分鐘，使前述已B階化之薄膜進行聚合來取得。 關於前述粉體塗料，能藉由在前述熱塑性樹脂材2之上，以厚度成為1~100μm之方式，將粉碎前述已B階化之薄膜者予以層合，而直接使用作為粉體塗料狀底漆。又，關於前述乳液，若使用乳化劑，將前述粉體塗料狀底漆予以後乳化，並將此以厚度成為1~100μm之方式塗佈於前述熱塑性樹脂材2之上，即能使用作為乳液化(水系化)底漆。
前述原位聚合型組成物層31係以包含使前述原位聚合型組成物進行聚合而成之原位聚合型樹脂50~100質量%為佳，以包含70~100質量%為較佳。
前述原位聚合型組成物係以含有下述(1)~(7)之至少一種為佳，以含有下述(4)為較佳，以含有2官能環氧樹脂予2官能酚化合物之組合為更佳。 (1)2官能異氰酸酯化合物與二醇之組合 (2)2官能異氰酸酯化合物與2官能胺基化合物之組合 (3)2官能異氰酸酯化合物與2官能硫醇化合物之組合 (4)2官能環氧化合物與二醇之組合 (5)2官能環氧化合物與2官能羧基化合物之組合 (6)2官能環氧化合物與2官能硫醇化合物之組合 (7)單官能自由基聚合性單體
(1)中之2官能異氰酸酯化合物與二醇之摻合量比係以設定成異氰酸酯基對羥基之莫耳當量比成為0.7~1.5為佳，較佳作成0.8~1.4，更佳作成0.9~1.3。 (2)中之2官能異氰酸酯化合物與2官能胺基化合物之摻合量比係以設定成異氰酸酯基對胺基之莫耳當量比成為0.7~1.5為佳，較佳作成0.8~1.4，更佳作成0.9~1.3。 (3)中之2官能異氰酸酯化合物與2官能硫醇化合物之摻合量比係以設定成異氰酸酯基對巰基之莫耳當量比成為0.7~1.5為佳，較佳作成0.8~1.4，更佳作成0.9~1.3。 (4)中之2官能環氧化合物與二醇之摻合量比係以設定成環氧基對羥基之莫耳當量比成為0.7~1.5為佳，較佳作0.8~1.4，更佳作成0.9~1.3。 (5)中之2官能環氧化合物與2官能羧基化合物之摻合量比係以設定成環氧基對羧基之莫耳當量比成為0.7~1.5為佳，較佳作成0.8~1.4，更佳作成0.9~1.3。 (6)中之2官能環氧化合物與2官能硫醇化合物之摻合量比係以設定成環氧基對巰基之莫耳當量比成為0.7~1.5為佳，較佳作成0.8~1.4，更佳作成0.9~1.3。
作為前述原位聚合型組成物，可例示例如，下述原位聚合型組成物(A)~(D)。 原位聚合型組成物(A)：含有前述(1)~(7)之至少一種之組成物。 原位聚合型組成物(B)：包含含有前述(1)~(7)之至少一種之組成物，與無水馬來酸改質聚丙烯或改質聚苯醚的組成物。 原位聚合型組成物(C)：包含含有前述(1)~(7)之至少一種之組成物，及，與構成熱塑性樹脂材2之熱塑性樹脂為異種之熱塑性樹脂的組成物。 原位聚合型組成物(D)：包含含有前述(1)~(7)之至少一種之組成物、無水馬來酸改質聚丙烯或改質聚苯醚、及，與構成熱塑性樹脂材2之熱塑性樹脂為異種之熱塑性樹脂的組成物。
藉由在前述熱塑性樹脂材2上層合原位聚合型組成物層31作為底漆層3，而能在前述熱塑性樹脂材2上強固地熔接同種之熱塑性樹脂材或異種之熱塑性樹脂材。尤其，前述原位聚合型組成物層31係以與前述熱塑性樹脂材2直接接觸之層為佳。 尚且，作為前述原位聚合型組成物，以選擇包含與構成前述熱塑性樹脂材2之熱塑性樹脂類似之熱塑性樹脂的組成物為佳。例如，前述熱塑性樹脂材2為聚烯烴之情況，藉由使用包含無水馬來酸改質聚烯烴之原位聚合型組成物，而變得能更加強固性熔接。又，前述熱塑性樹脂材2為改質聚苯醚之情況，藉由使用包含改質聚苯醚之原位聚合型組成物，而變得能更加強固性熔接。
也能以包含前述原位聚合型組成物層31之複數層來構成前述底漆層3。前述底漆層3為包含複數層之情況，必須之原位聚合型組成物層31係以層合在與前述熱塑性樹脂材2為反對側之最表面上為佳。於此情況，原位聚合型組成物並非係在熱塑性樹脂材2之表面，而係變得在原位聚合型組成物層31之正下方之層表面上進行聚合。
(原位聚合型組成物層A) 原位聚合型組成物層A包含前述原位聚合型組成物(A)之聚合物。 原位聚合型組成物層A係可使含有前述(1)~(6)之至少一種之組成物在觸媒存在下進行加成聚合反應而得。作為加成聚合反應用之觸媒，適宜使用例如，三乙基胺、2,4,6-參(二甲基胺基甲基)酚等之3級胺-三苯基膦等之磷系化合物等。前述加成聚合反應雖也係根據組成物之組成而不同，但以在常溫~200℃下加熱5~120分鐘來進行為佳。在此，本說明書中，常溫係指5~35℃，以15~25℃為佳。 具體而言，例如，原位聚合型組成物層A係可藉由將含有前述(1)~(6)之至少一種之組成物溶解於溶劑並塗佈於前述熱塑性樹脂材2之上後，適宜使溶劑揮發，其後加熱來進行加成聚合反應，而形成經強固結合之原位聚合型組成物層。原位聚合型組成物層A係也可藉由將使含有前述(1)~(6)之至少一種之組成物B階化後之薄膜配置於前述熱塑性樹脂材2上，加熱前述薄膜使其進行加成聚合反應來形成。
原位聚合型組成物層A係也能以含有前述(7)之單官能自由基聚合性單體之組成物之自由基聚合反應來取得。前述自由基聚合反應雖也係根據組成物之組成而不同，但以在常溫~200℃下加熱5~90分鐘來進行為佳。又在光硬化之情況，照射紫外線或可見光來進行聚合反應。 具體而言，例如，原位聚合型組成物層A係可藉由將使含有前述(7)之單官能自由基聚合性單體之組成物溶解於溶劑並塗佈在前述熱塑性樹脂材2之上後，進行加熱或光照射來進行自由基聚合反應，而形成經強固結合之原位聚合型組成物層。原位聚合型組成物層A係也可藉由將薄膜配置於前述熱塑性樹脂材2上，對前述薄膜進行加熱或光照射使其進行自由基聚合反應來形成，其中該薄膜係使含有前述(7)之單官能自由基聚合性單體之組成物B階化者。
(2官能異氰酸酯化合物) 前述2官能異氰酸酯化合物為具有2個異氰酸基之化合物，可舉出例如，六亞甲基二異氰酸酯、四亞甲基二異氰酸酯、二聚物酸二異氰酸酯、2,4-或2,6-伸甲苯基二異氰酸酯(TDI)或其混合物、p-伸苯基二異氰酸酯、伸茬基二異氰酸酯、二苯基甲烷二異氰酸酯(MDI)等之二異氰酸酯化合物。其中從底漆強度之觀點，以TDI或MDI等為佳。
(二醇) 前述二醇為具有2個羥基之化合物，可舉出例如，乙二醇、丙二醇、二乙二醇、1,6己二醇等之脂肪族二醇、雙酚A、雙酚F、雙酚S等之雙酚類。其中從底漆強靭性之觀點，以丙二醇、二乙二醇等為佳。
(2官能胺基化合物) 前述2官能胺基化合物為具有2個胺基之化合物，可舉出例如，2官能之脂肪族二胺、芳香族二胺。作為脂肪族二胺，可舉出如，乙二胺、1,2-丙二胺、1,3-丙二胺、1,4-二胺基丁烷、1,6-六亞甲基二胺、2,5-二甲基-2,5-己二胺、2,2,4-三甲基六亞甲基二胺、異佛爾酮二胺、雙(4-胺基-3-甲基環己基)甲烷、1,3-二胺基環己烷、N-胺基乙基哌嗪等，作為芳香族二胺，可舉出如二胺基二苯基甲烷、二胺基二苯基丙烷等。其中從底漆強靭性之觀點，以1,3-丙二胺、1,4-二胺基丁烷、1,6-六亞甲基二胺等為佳。
(2官能硫醇化合物) 前述2官能硫醇化合物為分子內具有2個巰基之化合物，可舉出例如，2官能2級硫醇化合物之1,4-雙(3-巰基丁醯氧基)丁烷(例如，昭和電工股份有限公司製「Karenz MT(註冊商標) BD1」)。
(2官能環氧化合物) 前述2官能環氧化合物為1分子中具有2個環氧基之化合物。可舉出例如，雙酚A型環氧樹脂、雙酚F型環氧樹脂、雙酚S型環氧樹脂、聯酚型環氧樹脂、萘型2官能環氧樹脂等之芳香族環氧樹脂或1,6-己二醇二環氧丙基醚等脂肪族環氧化合物。 該等之中，可單獨使用1種，亦可併用2種以上。 具體地可舉出如三菱化學股份有限公司製「jER(註冊商標)828」、同「jER(註冊商標)834」、同「jER(註冊商標)1001」、同「jER(註冊商標)1004」、同「jER(註冊商標)YX-4000」等。其他，只要2官能者，也可使用特殊構造之環氧化合物。該等之中，可單獨使用1種，亦可併用2種以上。
(2官能羧基化合物) 作為前述2官能羧基化合物，只要係具有2個羧基之化合物即可，可舉出例如，草酸、丙二酸、琥珀酸、戊二酸、己二酸、馬來酸、富馬酸、異酞酸、對酞酸等。其中從底漆之強度或強靭性之觀點，以異酞酸、對酞酸、己二酸等為佳。
(單官能自由基聚合性單體) 前述單官能自由基聚合性單體為具有1個乙烯性不飽和鍵之單體。例如，苯乙烯單體；苯乙烯之α-,o-,m-,p-烷基、硝基、氰基、醯胺、酯衍生物；氯苯乙烯、乙烯基甲苯、二乙烯基苯等之苯乙烯系單體；(甲基)丙烯酸乙酯、(甲基)丙烯酸甲酯、(甲基)丙烯酸-n-丙基、(甲基)丙烯酸-i-丙基、(甲基)丙烯酸己基、(甲基)丙烯酸2-乙基己基酯、(甲基)丙烯酸月桂基酯、(甲基)丙烯酸十二基酯、(甲基)丙烯酸環戊基酯、(甲基)丙烯酸環己基酯、(甲基)丙烯酸四氫呋喃基酯、乙醯乙醯氧基乙基(甲基)丙烯酸酯、二環戊烯氧基乙基(甲基)丙烯酸酯及苯氧基乙基(甲基)丙烯酸酯、環氧丙基(甲基)丙烯酸酯等之(甲基)丙烯酸酯類。前述化合物之中，可使用1種，亦可使用2種以上。其中從底漆之強度或強靭性之觀點，以苯乙烯、(甲基)丙烯酸甲酯、(甲基)丙烯酸2-乙基己基酯、苯氧基乙基(甲基)丙烯酸酯之中之一種，或2種以上之組合為佳。 含有自由基聚合性單體之組成物為了使自由基聚合反應充分進行而形成所欲之原位聚合型組成物層，亦可包含溶劑，或因應必要之著色劑等之添加劑。此時，前述組成物之溶劑以外之含有成分中，以前述單官能自由基聚合性單體係主成分為佳。前述主成分係意指前述單官能自由基聚合性單體之含有率為50~100質量%。前述含有率係以60質量%以上為佳，較佳為80質量%以上。 作為自由基聚合反應用之聚合起始劑，可適宜使用例如，公知之有機過氧化物或光起始劑等。也可使用對有機過氧化物組合鈷金屬鹽或胺類而成之常溫自由基聚合起始劑。作為有機過氧化物，可舉出如被分類在過氧化酮、過氧化縮酮、氫過氧化物、二烯丙基過氧化物、二醯基過氧化物、過氧化酯、過氧化二碳酸酯者。作為光起始劑，以使用在從紫外線至可見光線下能開始聚合開始者為理想。 自由基聚合反應雖也係根據反應化合物等之種類而不同，但以在常溫~200℃下加熱5~90分鐘來進行為佳。又在光硬化之情況，照射紫外線或可見光來進行聚合反應。具體而言，可藉由塗佈前述組成物後，進行加熱、或光照射來進行自由基聚合反應，而形成包含前述自由基聚合性化合物之原位聚合型組成物層。
(原位聚合型組成物層B) 原位聚合型組成物層B包含前述原位聚合型組成物(B)之聚合物。 原位聚合型組成物層B係可在無水馬來酸改質聚丙烯或改質聚苯醚之溶液中，使前述(1)~(6)之至少一種在觸媒存在下進行加成聚合反應而得。作為加成聚合反應用之觸媒，適宜使用例如，三乙基胺、2,4,6-參(二甲基胺基甲基)酚等之3級胺-三苯基膦等之磷系化合物等。前述加成聚合反應係也係根據組成物之組成而不同，但以在常溫~200℃下加熱5~120分鐘來進行為佳。 具體而言，例如，原位聚合型組成物層B係可藉由使無水馬來酸改質聚丙烯或改質聚苯醚，與含有前述(1)~(6)之至少一種之組成物溶解於溶劑並塗佈於前述熱塑性樹脂材2之上後，適宜使溶劑揮發，其後加熱來進行加成聚合反應而形成。又，原位聚合型組成物層B係也可藉由將薄膜配置於前述熱塑性樹脂材2上，並加熱前述薄膜來進行加成聚合反應而形成，其中該薄膜係使無水馬來酸改質聚丙烯或改質聚苯醚與含有前述(1)~(6)之至少一種之組成物之混合物B階化者。
原位聚合型組成物層B係也可使含有前述(7)之單官能自由基聚合性單體之組成物在無水馬來酸改質聚丙烯或改質聚苯醚之溶液中進行自由基聚合反應而得。前述自由基聚合反應係也係根據組成物之組成而不同，但以在常溫~200℃下加熱5~90分鐘來進行為佳。又在光硬化之情況，照射紫外線或可見光來進行聚合反應。 具體而言，例如，原位聚合型組成物層B係可藉由使無水馬來酸改質聚丙烯或改質聚苯醚，與含有前述(7)之單官能自由基聚合性單體之組成物溶解於溶劑並塗佈於前述熱塑性樹脂材2之上後，進行加熱或光照射來進行自由基聚合反應而形成。又，原位聚合型組成物層B係也可藉由將薄膜配置於前述熱塑性樹脂材2上，對前述薄膜進行加熱或光照射來進行自由基聚合反應而形成，其中該薄膜係使無水馬來酸改質聚丙烯或改質聚苯醚與含有前述(7)之單官能自由基聚合性單體之組成物之混合物B階化者。
(無水馬來酸改質聚丙烯) 無水馬來酸改質聚丙烯為以無水馬來酸來接枝改質之聚丙烯。如有化藥AKZO公司製Kayabrid 002PP、002PP-NW、003PP、003PP-NW、三菱化學公司製Modic系列等。 又亦可併用BYK公司製SCONA TPPP2112GA、TPPP8112GA、TPPP9212GA作為以無水馬來酸來機能化之聚丙烯添加劑。
(改質聚苯醚) 作為前述改質聚苯醚，可使用公知者。 改質聚苯醚為對聚苯醚摻合聚苯乙烯、聚醯胺、聚苯硫醚、聚丙烯等而成者，如有SABIC公司製NORYL系列(PPS/PS)：731、7310、731F、7310F，旭化成化學公司製Zylon系列(PPE/PS、PP/PPE、PA/PPE、PPS/PPE、PPA/PPE)、三菱工程塑料公司製Iupiace系列、Lemalloy系列(PPE/PS、PPE/PA)。
在取得前述原位聚合型組成物層B時所用之前述(1)~(7)之合計量，在將無水馬來酸改質聚丙烯或改質聚苯醚設為100質量份時，以5~100質量份為佳，以5~60質量份為較佳，以20~40質量份為更佳。
(原位聚合型組成物層C) 原位聚合型組成物層C包含前述原位聚合型組成物(C)之聚合物。 原位聚合型組成物層C係可藉由在包含與構成熱塑性樹脂材2之熱塑性樹脂為異種之熱塑性樹脂之溶液中，使前述(1)~(6)之至少一種在觸媒存在下進行加成聚合反應而得。作為加成聚合反應用之觸媒，適宜使用例如，三乙基胺、2,4,6-參(二甲基胺基甲基)酚等之3級胺、三苯基膦等之磷系化合物等。前述加成聚合反應雖也係根據組成物之組成而不同，但以在常溫~200℃下加熱5~120分鐘來進行為佳。 具體而言，例如，原位聚合型組成物層C係可藉由使與構成熱塑性樹脂材2之熱塑性樹脂為異種之熱塑性樹脂，及含有前述(1)~(6)之至少一種之組成物溶解於溶劑並塗佈於前述熱塑性樹脂材2之上後，適宜使溶劑揮發，其後加熱來進行加成聚合反應而形成。又，原位聚合型組成物層C係也可藉由將薄膜配置於前述熱塑性樹脂材2上，加熱前述薄膜來進行加成聚合反應而形成，其中該薄膜係使與構成熱塑性樹脂材2之熱塑性樹脂為異種之熱塑性樹脂，與含有前述(1)~(6)之至少一種之組成物之混合物B階化者。
原位聚合型組成物層C係也可使含有前述(7)之單官能自由基聚合性單體之組成物，在包含與構成熱塑性樹脂材2之熱塑性樹脂為異種之熱塑性樹脂之溶液中進行自由基聚合反應而得。前述自由基聚合反應係也係根據組成物之組成而不同，但以在常溫~200℃下加熱5~90分鐘來進行為佳。又在光硬化之情況，照射紫外線或可見光來進行聚合反應。 具體而言，例如，原位聚合型組成物層C係可藉由使與構成熱塑性樹脂材2之熱塑性樹脂為異種之熱塑性樹脂，及含有前述(7)之單官能自由基聚合性單體之組成物溶解於溶劑並塗佈於前述熱塑性樹脂材2之上後，進行加熱或光照射來進行自由基聚合反應而形成。又，原位聚合型組成物層C係也可藉由將薄膜配置於前述熱塑性樹脂材2上，對前述薄膜進行加熱或光照射來進行自由基聚合反應而形成，其中該薄膜係使與構成熱塑性樹脂材2之熱塑性樹脂為異種之熱塑性樹脂，與含有前述(7)之單官能自由基聚合性單體之組成物之混合物B階化者。
(原位聚合型組成物層D) 原位聚合型組成物層D包含前述原位聚合型組成物(D)之聚合物。 原位聚合型組成物層D係可在無水馬來酸改質聚丙烯或改質聚苯醚之溶液中，使前述(1)~(6)之至少一種在觸媒存在下進行加成聚合反應後，將其混合於與構成熱塑性樹脂材2之熱塑性樹脂為異種之熱塑性樹脂中而得。或，也可在包含與構成熱塑性樹脂材2之熱塑性樹脂為異種之熱塑性樹脂之溶液中，也可使前述(1)~(6)之至少一種在觸媒存在下進行加成聚合反應後，再與無水馬來酸改質聚丙烯或改質聚苯醚進行混合而得。或，可使無水馬來酸改質聚丙烯或改質聚苯醚、與構成熱塑性樹脂材2之熱塑性樹脂為異種之熱塑性樹脂，及前述(1)~(6)之至少一種在觸媒存在下進行加成聚合反應而得。作為加成聚合反應用之觸媒，適宜使用例如，三乙基胺、2,4,6-參(二甲基胺基甲基)酚等之3級胺、三苯基膦等之磷系化合物等。前述加成聚合反應雖也係根據組成物之組成而不同，但以在常溫~200℃下加熱5~120分鐘來進行為佳。 具體而言，例如，原位聚合型組成物層D係可藉由使無水馬來酸改質聚丙烯或改質聚苯醚、與構成熱塑性樹脂材2之熱塑性樹脂為異種之熱塑性樹脂、及含有前述(1)~(6)之至少一種之組成物溶解於溶劑並塗佈於前述熱塑性樹脂材2之上後，適宜使溶劑揮發，其後進行加熱來進行加成聚合反應而形成。又，原位聚合型組成物層D係也可藉由將薄膜配置於前述熱塑性樹脂材2上，加熱前述薄膜來進行加成聚合反應而形成，其中該薄膜係使無水馬來酸改質聚丙烯或改質聚苯醚、與構成熱塑性樹脂材2之熱塑性樹脂為異種之熱塑性樹脂，及含有前述(1)~(6)之至少一種之組成物之混合物B階化者。
原位聚合型組成物層D係也可使含有前述(7)之單官能自由基聚合性單體之組成物，在包含無水馬來酸改質聚丙烯或改質聚苯醚，及，與構成熱塑性樹脂材2之熱塑性樹脂為異種之熱塑性樹脂之溶液中進行自由基聚合反應而得。前述自由基聚合反應係也係根據組成物之組成而不同，但以在常溫~200℃下加熱5~90分鐘來進行為佳。又在光硬化之情況，照射紫外線或可見光來進行聚合反應。 具體而言，例如，原位聚合型組成物層D係可藉由使無水馬來酸改質聚丙烯或改質聚苯醚、與構成熱塑性樹脂材2之熱塑性樹脂為異種之熱塑性樹脂，及含有前述(7)之單官能自由基聚合性單體之組成物溶解於溶劑中並塗佈於前述熱塑性樹脂材2之上後，進行加熱或光照射來進行自由基聚合反應而形成。又，原位聚合型組成物層D係也藉由將薄膜配置於前述熱塑性樹脂材2上，對前述薄膜進行加熱或光照射來進行自由基聚合反應而形成，其中該薄膜係使無水馬來酸改質聚丙烯或改質聚苯醚、與構成熱塑性樹脂材2之熱塑性樹脂為異種之熱塑性樹脂，及含有前述(7)之單官能自由基聚合性單體之組成物之混合物B階化者。
尚且，形成前述原位聚合型組成物層時所產生之反應方式則有多種方式，如無水馬來酸改質聚丙烯或改質聚苯醚與2官能環氧樹脂之反應、無水馬來酸改質聚丙烯或改質聚苯醚與2官能酚化合物之反應等，且，也無法包括性地表現基於該組合之具體態樣。因此，藉由構造或特性來直接特定前述原位聚合型組成物層可謂係不可能或不實際。
[熱硬化性樹脂層32] 以包含前述原位聚合型組成物層31之複數層來構成底漆層3之情況，如圖2所示般，底漆層3係也可在原位聚合型組成物層31與熱塑性樹脂材2之間包含由包含熱硬化性樹脂之組成物所形成而成之熱硬化性樹脂層32。 尚且，前述包含熱硬化性樹脂之組成物為了使前述熱硬化性樹脂之硬化反應充分進行而形成所欲之熱硬化性樹脂層，亦可包含溶劑，或因應必要之著色劑等之添加劑。於此情況，在前述組成物之溶劑以外之含有成分中，以前述熱硬化性樹脂為主成分為佳。前述主成分係意指前述熱硬化性樹脂之含有率為40~100質量%。前述含有率係以60質量%以上為佳，較佳為70質量%以上，更佳為80質量%以上。
作為前述熱硬化性樹脂，可舉出例如，胺基甲酸酯樹脂、環氧樹脂、乙烯基酯樹脂、不飽和聚酯樹脂。 熱硬化性樹脂層32係能以該等樹脂之中之單獨1種來形成，亦可混合2種以上來形成。又或，也能以複數層來構成熱硬化性樹脂層32，並使用包含相異種類之熱硬化性樹脂之組成物來形成各層。
藉由前述包含熱硬化性樹脂之單體之組成物來形成熱硬化性樹脂層32之塗覆方法並非係受到特別限定者，可舉出例如，噴塗法、浸漬法等。
尚且，本實施態樣所稱之熱硬化性樹脂係廣泛地意指交聯硬化之樹脂，而不受限於加熱硬化型，也係作為包括常溫硬化型或光硬化型者。前述光硬化型係藉由可見光或紫外線之照射而能達成短時間內之硬化者。亦可將前述光硬化型與加熱硬化型及/或常溫硬化型併用。作為前述光硬化型，可舉出例如，昭和電工股份有限公司製「Ripoxy(註冊商標)LC-760」、同「Ripoxy(註冊商標)LC-720」等之乙烯基酯樹脂。
(胺基甲酸酯樹脂) 前述胺基甲酸酯樹脂通常係藉由異氰酸酯化合物之異氰酸基與多元醇化合物之羥基之反應而得之樹脂，以該當於在ASTM D16中，定義成「包含不揮發媒液成分10wt%以上之聚異氰酸酯之塗料」者之胺基甲酸酯樹脂為佳。前述胺基甲酸酯樹脂可為單液型，亦可為二液型。
作為單液型胺基甲酸酯樹脂，可舉出例如，油改質型(藉由不飽和脂肪酸基之氧化聚合而進行硬化者)、濕氣硬化型(藉由異氰酸基與空氣中之水之反應而進行硬化者)、封端型(封端劑藉由加熱進行解離而再生之異氰酸基與羥基進行反應而硬化者)、漆(Lacquer)型(藉由溶劑進行揮發乾燥而進行硬化者)等。該等之中，從操作容易性等之觀點，適宜使用濕氣硬化型單液胺基甲酸酯樹脂。具體地可舉出如昭和電工股份有限公司製「UM-50P」等。
作為二液型胺基甲酸酯樹脂，可舉出例如，觸媒硬化型(異氰酸基與空氣中之水等在觸媒存在下反應而進行硬化者)、多元醇硬化型(藉由異氰酸基與多元醇化合物之羥基之反應而進行硬化者)等。
作為前述多元醇硬化型中之多元醇化合物，可舉出例如，聚酯多元醇、聚醚多元醇、酚樹脂等。 又，作為前述多元醇硬化型中之具有異氰酸基之異氰酸酯化合物，可舉出例如，六亞甲基二異氰酸酯(HDI)、四亞甲基二異氰酸酯、二聚物酸二異氰酸酯等之脂肪族異氰酸酯；2,4-或2,6-伸甲苯基二異氰酸酯(TDI)或其混合物、p-伸苯基二異氰酸酯、伸茬基二異氰酸酯、二苯基甲烷二異氰酸酯(MDI)或其多核體混合物之聚合型MDI等之芳香族異氰酸酯；異佛爾酮二異氰酸酯(IPDI)等之脂環族異氰酸酯等。 前述多元醇硬化型之二液型胺基甲酸酯樹脂中之前述多元醇化合物與前述異氰酸酯化合物之配合比在以羥基/異氰酸基之莫耳當量比計，以0.7~1.5之範圍為佳。
作為前述二液型胺基甲酸酯樹脂中所使用之胺基甲酸酯化觸媒，可舉出例如，三乙二胺、四甲基胍、N,N,N’,N’-四甲基己-1,6-二胺、二甲基醚胺、N,N,N’,N”,N”-五甲基二伸丙基-三胺、N-甲基嗎啉、雙(2-二甲基胺基乙基)醚、二甲基胺基乙氧基乙醇-三乙基胺等之胺系觸媒；二丁基錫二乙酸酯、二丁基錫二月桂酸酯、二丁基錫硫代羧酸鹽、二丁基錫二馬來酸鹽等之有機錫系觸媒等。 前述多元醇硬化型中，一般而言，相對於前述多元醇化合物100質量份，以摻合、前述胺基甲酸酯化觸媒0.01~10質量份為佳。
(環氧樹脂) 前述環氧樹脂為1分子中具有至少2個環氧基之樹脂。 作為前述環氧樹脂之硬化前之預聚物，可舉出例如，醚系雙酚型環氧樹脂、酚醛型環氧樹脂、聚酚型環氧樹脂、脂肪族型環氧樹脂、酯系之芳香族環氧樹脂、環狀脂肪族環氧樹脂、醚・酯系環氧樹脂等，該等之中係以適宜使用雙酚A型環氧樹脂。該等之中，可單獨使用1種，亦可併用2種以上。 作為雙酚A型環氧樹脂，具體地可舉出如三菱化學股份有限公司製「jER(註冊商標)828」、同「jER(註冊商標)1001」等。 作為酚醛型環氧樹脂，具體地可舉出如陶氏化學公司製「D.E.N.(註冊商標)438(註冊商標)」等。
作為前述環氧樹脂所使用之硬化劑，可舉出例如，脂肪族胺、芳香族胺、酸酐、酚樹脂、硫醇類、咪唑類、陽離子觸媒等之公知之硬化劑。前述硬化劑藉由與長鏈脂肪族胺或/及硫醇類之併用，而可取得伸長率大，且耐衝撃性優異之效果。 作為前述硫醇類之具體例，可舉出如，與作為後述之形成含官能基層用之硫醇化合物所例示者為相同之化合物。該等之中，從伸長率及耐衝撃性之觀點，以季戊四醇肆(3-巰基丁酸酯)(例如，昭和電工股份有限公司製「Karenz MT(註冊商標)PE1」)為佳。
(乙烯基酯樹脂) 前述乙烯基酯樹脂係使乙烯基酯化合物溶解於聚合性單體(例如，苯乙烯等)者。雖然也係稱為環氧基(甲基)丙烯酸酯樹脂，但前述乙烯基酯樹脂中也係作為包括胺基甲酸酯(甲基)丙烯酸酯樹脂者。 作為前述乙烯基酯樹脂，也可使用例如，「聚酯樹脂手冊」(日刊工業新聞社、1988年發行)、「塗料用語辭典」(色材協會、1993年發行)等記載者，又，具體地可舉出如昭和電工股份有限公司製「Ripoxy(註冊商標)R-802」、同「Ripoxy(註冊商標)R-804」、同「Ripoxy(註冊商標)R-806」等。
作為前述胺基甲酸酯(甲基)丙烯酸酯樹脂，可舉出例如，使異氰酸酯化合物與多元醇化合物反應後，再使含羥基之(甲基)丙烯醯基單體(及，因應必要之含羥基之烯丙基醚單體)反應而得之含自由基聚合性不飽和基之寡聚物。具體地可舉出如昭和電工股份有限公司製「Ripoxy(註冊商標)R-6545」等。
前述乙烯基酯樹脂係能以由在有機過氧化物等之觸媒存在下之加熱所成自由基聚合來使其硬化。 作為前述有機過氧化物，並非係受到特別限定者，可舉出例如，過氧化酮類、過氧化縮酮類、氫過氧化物類、二烯丙基過氧化物類、二醯基過氧化物類、過氧化酯類、過氧化二碳酸酯類等。藉由將該等與鈷金屬鹽等組合，從而也變得能在常溫下硬化。 作為前述鈷金屬鹽，並非係受到特別限定者，可舉出例如，環烷酸鈷、辛酸鈷、氫氧化鈷等。該等之中，以環烷酸鈷或/及辛酸鈷為佳。
(不飽和聚酯樹脂) 前述不飽和聚酯樹脂係使由多元醇化合物與不飽和多元酸(及，因應必要之飽和多元酸)之酯化反應而成之縮合生成物(不飽和聚酯)溶解於聚合性單體(例如，苯乙烯等)者。 作為前述不飽和聚酯樹脂，也可使用如「聚酯樹脂手冊」(日刊工業新聞社、1988年發行)、「塗料用語辭典」(色材協會、1993年發行)等記載者，又，具體地可舉出如昭和電工股份有限公司製「Rigolac(註冊商標)」等。
前述不飽和聚酯樹脂係能以由與關於前述乙烯基酯樹脂同樣之觸媒存在下之加熱所成自由基聚合來使其硬化。
[底漆層3之作用] 底漆層3係形成於熱塑性樹脂材之表面，或，熱塑性樹脂材之表面及表層。 熱塑性樹脂材之表面之底漆層3係意指將使形成底漆層之組成物溶解於溶劑者塗佈於熱塑性樹脂材之表面，並在熱塑性樹脂材之表面上使前述溶劑揮發而形成者。 熱塑性樹脂材之表層之底漆層3係意指將使形成底漆層之組成物溶解於溶劑者塗佈於熱塑性樹脂材之表面，並藉由前述溶劑之滲透而經膨潤之熱塑性樹脂材之表層上，使形成前述底漆層之組成物滲透，再使前述溶劑揮發而形成者。
藉由底漆層3，而能賦予與接合對象之其他熱塑性樹脂材之優異接合性。也能取得即使經過數個月間之長時間，仍能維持前述接合性之附底漆之熱塑性樹脂材。 又，藉由底漆層3，熱塑性樹脂材之表面受到保護，而能抑制污垢之附著或氧化等之變質。
[樹脂-樹脂接合體4] 如圖3所示，本發明之樹脂-樹脂接合體4係使附底漆之熱塑性樹脂材1之底漆層3，與其他熱塑性樹脂材5熔接而成。構成其他熱塑性樹脂材5之熱塑性樹脂係可為與構成前述附底漆之熱塑性樹脂材1之熱塑性樹脂為同種，亦可為異種。
在試圖接合2個熱塑性樹脂材之情況，構成一側之熱塑性樹脂材之熱塑性樹脂，與，構成另一側之熱塑性樹脂材之熱塑性樹脂即使為同種，在一側或兩側之熱塑性樹脂含有填料或纖維，或該熱塑性樹脂已摻合有其他熱塑性樹脂時，2個熱塑性樹脂材間之接合強度仍會有變得不充足之場合。但，根據本發明，仍能強固地熔接其他熱塑性樹脂材5與附底漆之熱塑性樹脂材1。
前述構成附底漆之熱塑性樹脂材1之熱塑性樹脂，與，前述構成其他熱塑性樹脂材5之熱塑性樹脂為同種之情況，在構成熱塑性樹脂之單體中，佔最大含量之單體之比例皆為70質量%以上，以70~100質量%為佳，較佳為80~100質量%，更佳為85~100質量%。
前述構成附底漆之熱塑性樹脂材1之熱塑性樹脂及/或前述構成其他熱塑性樹脂材5之熱塑性樹脂在含有選自由填料及纖維所成群之至少1種之情況，其含量係以5~50質量%為佳，較佳為5~40質量%，更佳為5~30質量%。前述含量在前述範圍內時，可提高前述其他熱塑性樹脂材5與前述附底漆之熱塑性樹脂材1之接合強度。
又，前述構成附底漆之熱塑性樹脂材1之熱塑性樹脂及/或前述構成其他熱塑性樹脂材5之熱塑性樹脂為主要之熱塑性樹脂與附隨之熱塑性樹脂之摻合物的情況，附隨之熱塑性樹脂之含有率係以5~40質量%為佳，較佳為5~30質量%，更佳為5~20質量%。前述含有率在前述範圍內時，可提高附底漆之熱塑性樹脂材1與其他熱塑性樹脂材5之接合強度。 尚且，前述含有率係可藉由下述式來求出。 含有率(質量%)=[B/(A+B)]×100 (式中，A為構成附底漆之熱塑性樹脂材之熱塑性樹脂及/或構成其他熱塑性樹脂材之熱塑性樹脂當中主要之熱塑性樹脂之質量(g)，B為構成附底漆之熱塑性樹脂材之熱塑性樹脂及/或構成其他熱塑性樹脂材之熱塑性樹脂當中附隨之熱塑性樹脂之質量(g)。)
本發明在即使前述構成其他熱塑性樹脂材5之熱塑性樹脂，與，前述構成附底漆之熱塑性樹脂材1之熱塑性樹脂為異種之情況，仍能強固地熔接其他熱塑性樹脂材5與附底漆之熱塑性樹脂材1。並且，前述構成其他熱塑性樹脂材5之熱塑性樹脂之SP值，與前述構成附底漆之熱塑性樹脂材1之熱塑性樹脂之SP值即使遠離之情況，仍能強固地熔接其他熱塑性樹脂材5與附底漆之熱塑性樹脂材1。
前述底漆層之厚度(乾燥後之厚度)雖也係根據附底漆之熱塑性樹脂材1及其他熱塑性樹脂材5之材質或接合部分之接觸面積而不同，從取得優異接合強度之觀點，以1μm~500μm為佳，較佳為3μm~100μm，更佳為5μm~70μm。又，原位聚合型組成物層之厚度(乾燥後之厚度)係以1~60μm為佳。 尚且，前述底漆層為複數層之情況，底漆層之厚度(乾燥後之厚度)係作為各層合計之厚度。
作為製造樹脂-樹脂接合體4之方法，可舉出如，對附底漆之熱塑性樹脂材1之底漆層3以選自由超音波熔接法、振動熔接法、電磁感應法、高頻法、雷射法、及熱壓法所成群之至少1種方法來熔接其他熱塑性樹脂材之方法，或，在附底漆之熱塑性樹脂材1之底漆層3之上，藉由射出成形來使其他熱塑性樹脂材成形之方法。 作為前述其他熱塑性樹脂材，也可使用與本發明之附底漆之熱塑性樹脂材相同構成之附底漆之熱塑性樹脂材，來熔接各自之底漆層。
構成附底漆之熱塑性樹脂材1之熱塑性樹脂與構成其他熱塑性樹脂材5之熱塑性樹脂可為同種，也可為異種，從強固熔接之觀點，以同種為佳。 [實施例]
其次，說明關於本發明之具體實施例，但本發明並非係受到該等實施例所特別限定者。
＜試驗片用熱塑性樹脂材＞ 在以下所示之表1之條件下，使用射出成形機(住友重機械工業股份有限公司製SE100V)，而取得拉伸試驗用之試驗片用熱塑性樹脂材(寬10mm、長度45mm、厚度3mm)：放有滑石之PP樹脂、放有玻璃纖維之PA6樹脂、放有玻璃纖維之PA66樹脂、m-PPE樹脂、PPS樹脂、PEI樹脂、PC樹脂、放有玻璃纖維之PBT樹脂。
Figure 02_image001
＜試驗片之製作：實施例1~3、比較例1＞ (底漆層形成用之原位聚合型組成物-1之製作) 取得使2官能環氧樹脂：三菱化學股份有限公司製「jER(註冊商標)1001」(雙酚A型環氧樹脂 分子量約900) 100g、雙酚S6.2g、及三乙基胺0.4g溶解於甲苯197g中而成之原位聚合型組成物-1(原位聚合型熱塑性環氧樹脂組成物)。
(底漆層之形成) 其次，在前述試驗片用熱塑性樹脂材之PBT、PC、PEI、PPS之單面表面上，以乾燥後之厚度成為80μm之方式，使用噴霧法來塗布原位聚合型組成物-1。藉由在空氣中常溫(23℃)下放置30分鐘而使溶劑揮發後，放置於150℃之爐中30分鐘來進行加成聚合反應，放置冷卻至常溫(23℃)，而取得將熱塑性環氧樹脂作為底漆層之試驗片PBT-1、PC-1、PEI-1、PPS-1。 以下，將試驗片中已形成底漆層之面稱為底漆面，將未形成底漆層之面稱為無底漆面。又，下述表2~4及6中，將具有底漆層之面標示為(有)，將不具有底漆層之面標示為(無)。
＜實施例1＞ (熔接) 在使PPS-1之底漆面與PEI-1之底漆面以接合部重疊且成為長度5mm、寬10mm之方式來疊合之狀態下，使用精電舍電子工業股份有限公司製超音波熔接機SONOPET-JII430T-M(28.5KHz)進行超音波熔接，而取得試驗片1(樹脂-樹脂接合體)。在此接合部係意指疊合試驗片用熱塑性樹脂材的場所。
(拉伸剪切強度) 對於試驗片1，在常溫(23℃)下放置1天後，根據ISO19095 1-4，使用拉伸試驗機(股份有限公司島津製作所製 萬能試驗機Autograph「AG-IS」；荷重元10kN、拉伸速度10mm/min、溫度23℃、50%RH)，進行拉伸剪切強度試驗，並測量接合強度。將測量結果展示於下述表2。
＜實施例2＞ (熔接) 使用與實施例1相同之操作順序來超音波熔接PBT-1之底漆面與PC-1之底漆面，而取得試驗片2(樹脂-樹脂接合體)。
(拉伸剪切強度) 對於試驗片2，使用與實施例1相同之手法來進行拉伸剪切強度試驗。將測量結果展示於下述表2。
＜實施例3＞ (熔接) 使用與實施例1相同之操作順序來超音波熔接PBT-1之底漆面與PC-1之無底漆面，而取得試驗片3(樹脂-樹脂接合體)。
(拉伸剪切強度) 對於試驗片3，使用與實施例1相同之手法來進行拉伸剪切強度試驗。將測量結果展示於下述表2。
＜實施例4＞ (熔接) 使用與實施例1相同之操作順序來超音波熔接PBT-1之底漆面與PPS-1之無底漆面，而取得試驗片4(樹脂-樹脂接合體)。
(拉伸剪切強度) 對於試驗片4，使用與實施例1相同之手法來進行拉伸剪切強度試驗。將測量結果展示於下述表2。
＜比較例1＞ 使用與實施例1相同之操作順序來嘗試超音波熔接PBT-1之無底漆面與PPS-1之無底漆面，但無法熔接。
Figure 02_image003
＜試驗片：實施例5~7、比較例2、3＞ (底漆層形成用之原位聚合型組成物-2之製作) 取得使二苯基甲烷二異氰酸酯(東曹股份有限公司製「Millionate MT」)100g、丙二醇54.7g、及4,4´-二胺基二苯基甲烷15.8g溶解於丙酮287g中而成之原位聚合型組成物-2(原位聚合型胺基甲酸酯樹脂組成物)。
(底漆層之形成) 其次，在前述試驗片用熱塑性樹脂材之PA6、PA66、PBT、PC之單面表面上，以乾燥後之厚度成為90μm之方式以噴霧法來塗佈原位聚合型組成物-2。藉由在空氣中常溫(23℃)下放置30分鐘而使溶劑揮發後，放置於150℃之爐中30分鐘來進行加成聚合反應，放置冷卻至常溫(23℃)，而取得將胺基甲酸酯樹脂作為底漆層之試驗片PA6-1、PA66-1、PBT-2、PC-2。
＜實施例5＞ (熔接) 在使PA6-1之底漆面與PBT-2之底漆面以接合部重疊且成為長度5mm、寬10mm之方式來疊合之狀態下，使用精電舍電子工業股份有限公司製超音波熔接機SONOPET-JII430T-M(28.5KHz)進行超音波熔接，而取得試驗片5(樹脂-樹脂接合體)。
(拉伸剪切強度) 對於試驗片5，使用與實施例1相同之手法來進行拉伸剪切強度試驗，並測量接合強度。將測量結果展示於下述表3。
＜實施例6、7＞ 與實施例5同樣地操作，以下述表3記載之組合，進行各試驗片之作成，及拉伸剪切強度試驗。將結果展示於下述表3。
＜比較例2＞ 使用與實施例5相同之操作順序來嘗試超音波熔接PA6-1之無底漆面與PBT-2之無底漆面，但無法熔接。
＜比較例3＞ 使用與實施例5相同之操作順序來嘗試超音波熔接PA66-1之無底漆面與PC-2之無底漆面，但無法熔接。
Figure 02_image005
＜試驗片：實施例8~10、比較例4、5＞ (底漆層形成用之原位聚合型組成物-3之製作) 使無水馬來酸改質聚丙烯(三菱化學股份有限公司製 Modic(註冊商標)ER321P)：5g、環氧樹脂(三菱化學股份有限公司製 jER(註冊商標)1001)：1.01g、雙酚A：0.24g溶解於熱二甲苯：95g後，添加觸媒之2,4,6-參(二甲基胺基甲基)酚：0.006g並急速冷卻，而取得原位聚合型組成物-3(原位聚合型含無水馬來酸之環氧樹脂組成物)。
(底漆層形成用之原位聚合型組成物-4之製作) 使改質聚苯醚(SABIC公司製 NOLYL731)：3.77g、2官能環氧樹脂(三菱化學股份有限公司製 jER(註冊商標) 1001)：1.0g、雙酚A：0.22g溶解於熱二甲苯：95g後，添加2,4,6-參(二甲基胺基甲基)酚：0.005g並急速冷卻，而取得原位聚合型組成物-4(原位聚合型含改質聚苯醚之環氧樹脂組成物)。
(底漆層之形成) 其次，在前述試驗片用熱塑性樹脂材之PP(滑石30質量%)、PBT之單面表面上，以乾燥後之厚度成為80μm之方式使用噴霧法來塗佈原位聚合型組成物-3。藉由在空氣中常溫(23℃)下放置30分鐘而使溶劑揮發後，放置於150℃之爐中30分鐘來進行加成聚合反應，放置冷卻至常溫(23℃)，而取得將含無水馬來酸之熱塑性環氧樹脂作為底漆層之試驗片PP-1、PBT-3。
其次，在前述試驗片用熱塑性樹脂材之m-PPE之單面表面上，以乾燥後之厚度成為80μm之方式使用噴霧法來塗佈原位聚合型組成物-4。藉由在空氣中常溫(23℃)下放置30分鐘而使溶劑揮發後，放置於150℃之爐中30分鐘來進行加成聚合反應，放置冷卻至常溫(23℃)，而取得將含有改質聚苯醚之環氧樹脂作為底漆層之試驗片m-PPE-1。
＜實施例8＞ (熔接) 在使PP-1之底漆面與m-PPE-1之底漆面以接合部重疊且成為長度5mm、寬10mm之方式來疊合之狀態下，使用精電舍電子工業股份有限公司製超音波熔接機SONOPET-JII430T-M(28.5KHz)進行超音波熔接，而取得試驗片8(樹脂-樹脂接合體)。
(拉伸剪切強度) 對於試驗片8，使用與實施例1相同之手法來進行拉伸剪切強度試驗，並測量接合強度。將測量結果展示於下述表4。
＜實施例9、10＞ 與實施例8同樣地操作，以下述表4記載之組合，進行各試驗片之作成，及拉伸剪切強度試驗。將結果展示於下述表4。
＜比較例4＞ 與實施例8相同之操作順序來嘗試超音波熔接PP-1之無底漆面與PBT-3之無底漆面，但無法熔接。
＜比較例5＞ 與實施例8相同之操作順序來嘗試超音波熔接m-PPE-1之無底漆面與前述試驗片用熱塑性樹脂材之PC之單面(無底漆面)，但無法熔接。
Figure 02_image007
＜試驗片：實施例11＞ 將附底漆之熱塑性樹脂材PC-1、PBT-1、PEI-1、PPS-1、PA6-1、PA66-1、m-PPE-1、PP-1插入於射出成形用模具中，在與表1相同條件下，在底漆面上，射出成形表5記載之個別異種之熱塑性樹脂，而取得接合部重疊且長度5mm、寬10mm之試驗片(8種)。
(拉伸剪切強度) 對於各試驗片，使用與實施例1相同之手法來進行拉伸剪切強度試驗。將測量結果展示於下述表5。
Figure 02_image009
＜實施例12~14、比較例6＞ 在已施加電暈放電處理之PA6薄膜(東麗股份有限公司製，Rayfan(註冊商標)NO(1401)，厚度15μm)及PET薄膜(東麗股份有限公司製，Lumirror(註冊商標)＃25-S10，厚度12μm)之單面表面，將原位聚合型組成物-2以乾燥後之厚度成為1μm之方式來分別進行塗布，在60℃下放置10分鐘來進行溶劑之揮發與加成聚合反應，從而進行底漆層之形成。 結合表6記載之薄膜之底漆面，與薄膜之底漆面，在60℃下通過熱輥，更在60℃下保持5分鐘來貼合薄膜彼此。製作出根據ISO29862(2007)之180°剝離試驗用之試驗片：各樹脂薄膜接合體(24mm×300mm×28μm，接合部長度：275mm)，並進行剝離試驗。將測量結果展示於下述表6。
Figure 02_image011
[產業上之可利用性]
本發明之附底漆之熱塑性樹脂材係可與其他熱塑性樹脂材接合一體化而使用作為例如，門側板(door side panel)、罩蓋頂(bonnet roof)、尾板(tailgate)、轉向吊架(Steering hanger)、A柱、B柱、C柱、D柱、碰撞盒(crash box)、電源控制單元(PCU)殼、電動壓縮機構件(內壁部、吸入口部、排氣控制閥(ECV)挿入部、機架軸套(mount boss)部等)、鋰離子電池(LIB)隔件、電池盒、LED頭燈等之汽車用零件，或智慧型電話、筆記型個人電腦、平板個人電腦、智慧手錶、大型液晶電視(LCD-TV)、屋外LED照明之構造物等，並非係特別係受限至於該等例示之用途者。
1:附底漆之熱塑性樹脂材 2:熱塑性樹脂材 3:底漆層 31:原位聚合型組成物層 32:熱硬化性樹脂層 4:樹脂-樹脂接合體 5:其他熱塑性樹脂材
[圖1]展示本發明之一實施形態中之附底漆之熱塑性樹脂材之構成的說明圖。 [圖2]展示本發明之其他實施形態中之附底漆之熱塑性樹脂材之構成的說明圖。 [圖3]展示本發明之一實施形態中之樹脂-樹脂接合體之構成的說明圖。
1:附底漆之熱塑性樹脂材
2:熱塑性樹脂材
3:底漆層
31:原位聚合型組成物層

Claims (15)

  1. 一種附底漆之熱塑性樹脂材，其係具有：熱塑性樹脂材，與層合於前述熱塑性樹脂材之1層或複數層之底漆層， 且前述底漆層之至少1層為使原位聚合型組成物在前述熱塑性樹脂材之上進行聚合而成之原位聚合型組成物層。
  2. 如請求項1之附底漆之熱塑性樹脂材，其中前述原位聚合型組成物層係與前述熱塑性樹脂材直接接觸之層。
  3. 如請求項1或2之附底漆之熱塑性樹脂材，其中前述原位聚合型組成物含有下述(1)~(7)之至少一種； (1)2官能異氰酸酯化合物與二醇之組合、 (2)2官能異氰酸酯化合物與2官能胺基化合物之組合、 (3)2官能異氰酸酯化合物與2官能硫醇化合物之組合、 (4)2官能環氧化合物與二醇之組合、 (5)2官能環氧化合物與2官能羧基化合物之組合、 (6)2官能環氧化合物與2官能硫醇化合物之組合、 (7)單官能自由基聚合性單體。
  4. 如請求項1或2之附底漆之熱塑性樹脂材，其中前述原位聚合型組成物為一組成物包含：含有下述(1)~(7)之至少一種之組成物，以及，無水馬來酸改質聚丙烯或改質聚苯醚； (1)2官能異氰酸酯化合物與二醇之組合、 (2)2官能異氰酸酯化合物與2官能胺基化合物之組合、 (3)2官能異氰酸酯化合物與2官能硫醇化合物之組合、 (4)2官能環氧化合物與二醇之組合、 (5)2官能環氧化合物與2官能羧基化合物之組合、 (6)2官能環氧化合物與2官能硫醇化合物之組合、 (7)單官能自由基聚合性單體。
  5. 如請求項1或2之附底漆之熱塑性樹脂材，其中前述原位聚合型組成物為一組成物包含：含有下述(1)~(7)之至少一種之組成物，以及，與構成前述熱塑性樹脂材之熱塑性樹脂為異種之熱塑性樹脂； (1)2官能異氰酸酯化合物與二醇之組合、 (2)2官能異氰酸酯化合物與2官能胺基化合物之組合、 (3)2官能異氰酸酯化合物與2官能硫醇化合物之組合、 (4)2官能環氧化合物與二醇之組合、 (5)2官能環氧化合物與2官能羧基化合物之組合、 (6)2官能環氧化合物與2官能硫醇化合物之組合、 (7)單官能自由基聚合性單體。
  6. 如請求項1或2之附底漆之熱塑性樹脂材，其中前述原位聚合型組成物為一組成物包含：含有下述(1)~(7)之至少一種之組成物、無水馬來酸改質聚丙烯或改質聚苯醚，以及，與構成前述熱塑性樹脂材之熱塑性樹脂為異種之熱塑性樹脂； (1)2官能異氰酸酯化合物與二醇之組合、 (2)2官能異氰酸酯化合物與2官能胺基化合物之組合、 (3)2官能異氰酸酯化合物與2官能硫醇化合物之組合、 (4)2官能環氧化合物與二醇之組合、 (5)2官能環氧化合物與2官能羧基化合物之組合、 (6)2官能環氧化合物與2官能硫醇化合物之組合、 (7)單官能自由基聚合性單體。
  7. 如請求項3~6中任一項之附底漆之熱塑性樹脂材，其中前述原位聚合型組成物含有前述(4)，且前述(4)之二醇為2官能酚化合物。
  8. 3~7中任一項之附底漆之熱塑性樹脂材，其中前述底漆層係在前述原位聚合型組成物層與前述熱塑性樹脂材之間具有熱硬化性樹脂層，該熱硬化性樹脂層係由包含熱硬化性樹脂之組成物所形成而成。
  9. 如請求項8之附底漆之熱塑性樹脂材，其中前述熱硬化性樹脂為選自由胺基甲酸酯樹脂、環氧樹脂、乙烯基酯樹脂及不飽和聚酯樹脂所成群之至少1種。
  10. 一種如請求項1之附底漆之熱塑性樹脂材之製造方法，其係將已溶解於溶劑之前述原位聚合型組成物塗佈於前述熱塑性樹脂材之表面，並使前述原位聚合型組成物進行聚合。
  11. 一種樹脂-樹脂接合體，其係使如請求項1~9中任一項之附底漆之熱塑性樹脂材之底漆層，與其他熱塑性樹脂材熔接而成。
  12. 如請求項11之樹脂-樹脂接合體，其中前述其他熱塑性樹脂材為如請求項1~9中任一項之附底漆之熱塑性樹脂材，並且係使各自之底漆層熔接而成。
  13. 如請求項11或12之樹脂-樹脂接合體，其中構成前述其他熱塑性樹脂材之熱塑性樹脂且係構成該熱塑性樹脂之單體中佔最大含量之單體，與，構成如請求項1~9中任一項之附底漆之熱塑性樹脂材之熱塑性樹脂且係構成該熱塑性樹脂之單體中佔最大含量之單體為相同，且該單體之含量皆為70質量%以上。
  14. 一種如請求項11~13中任一項之樹脂-樹脂接合體之製造方法，其係對前述附底漆之熱塑性樹脂材之底漆層，以選自由超音波熔接法、振動熔接法、電磁感應法、高頻法、雷射法、及熱壓法所成群之至少1種方法來熔接其他熱塑性樹脂材。
  15. 一種如請求項11~13中任一項之樹脂-樹脂接合體之製造方法，其係對前述附底漆之熱塑性樹脂材之底漆層，以射出成形法來射出熔接其他熱塑性樹脂材。
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