TW202017442A - 積層體 - Google Patents
積層體 Download PDFInfo
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- TW202017442A TW202017442A TW108132102A TW108132102A TW202017442A TW 202017442 A TW202017442 A TW 202017442A TW 108132102 A TW108132102 A TW 108132102A TW 108132102 A TW108132102 A TW 108132102A TW 202017442 A TW202017442 A TW 202017442A
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- TW
- Taiwan
- Prior art keywords
- plating
- layer
- catalyst
- resin
- laminate
- Prior art date
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- 229910052763 palladium Inorganic materials 0.000 claims description 19
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- TZIHFWKZFHZASV-UHFFFAOYSA-N methyl formate Chemical compound COC=O TZIHFWKZFHZASV-UHFFFAOYSA-N 0.000 description 2
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- 238000004611 spectroscopical analysis Methods 0.000 description 2
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- LJGHYPLBDBRCRZ-UHFFFAOYSA-N 3-(3-aminophenyl)sulfonylaniline Chemical compound NC1=CC=CC(S(=O)(=O)C=2C=C(N)C=CC=2)=C1 LJGHYPLBDBRCRZ-UHFFFAOYSA-N 0.000 description 1
- TYKLCAKICHXQNE-UHFFFAOYSA-N 3-[(2,3-dicarboxyphenyl)methyl]phthalic acid Chemical compound OC(=O)C1=CC=CC(CC=2C(=C(C(O)=O)C=CC=2)C(O)=O)=C1C(O)=O TYKLCAKICHXQNE-UHFFFAOYSA-N 0.000 description 1
- UCFMKTNJZCYBBJ-UHFFFAOYSA-N 3-[1-(2,3-dicarboxyphenyl)ethyl]phthalic acid Chemical compound C=1C=CC(C(O)=O)=C(C(O)=O)C=1C(C)C1=CC=CC(C(O)=O)=C1C(O)=O UCFMKTNJZCYBBJ-UHFFFAOYSA-N 0.000 description 1
- DKKYOQYISDAQER-UHFFFAOYSA-N 3-[3-(3-aminophenoxy)phenoxy]aniline Chemical compound NC1=CC=CC(OC=2C=C(OC=3C=C(N)C=CC=3)C=CC=2)=C1 DKKYOQYISDAQER-UHFFFAOYSA-N 0.000 description 1
- UCQABCHSIIXVOY-UHFFFAOYSA-N 3-[4-[4-(3-aminophenoxy)phenyl]phenoxy]aniline Chemical group NC1=CC=CC(OC=2C=CC(=CC=2)C=2C=CC(OC=3C=C(N)C=CC=3)=CC=2)=C1 UCQABCHSIIXVOY-UHFFFAOYSA-N 0.000 description 1
- ICNFHJVPAJKPHW-UHFFFAOYSA-N 4,4'-Thiodianiline Chemical compound C1=CC(N)=CC=C1SC1=CC=C(N)C=C1 ICNFHJVPAJKPHW-UHFFFAOYSA-N 0.000 description 1
- YBRVSVVVWCFQMG-UHFFFAOYSA-N 4,4'-diaminodiphenylmethane Chemical compound C1=CC(N)=CC=C1CC1=CC=C(N)C=C1 YBRVSVVVWCFQMG-UHFFFAOYSA-N 0.000 description 1
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Images
Classifications
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- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C18/00—Chemical coating by decomposition of either liquid compounds or solutions of the coating forming compounds, without leaving reaction products of surface material in the coating; Contact plating
- C23C18/16—Chemical coating by decomposition of either liquid compounds or solutions of the coating forming compounds, without leaving reaction products of surface material in the coating; Contact plating by reduction or substitution, e.g. electroless plating
- C23C18/1601—Process or apparatus
- C23C18/1633—Process of electroless plating
- C23C18/1646—Characteristics of the product obtained
- C23C18/165—Multilayered product
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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
- B32B27/18—Layered products comprising a layer of synthetic resin characterised by the use of special additives
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Abstract
一種積層體,包括:基材;以及鍍敷形成層,配置於所述基材的兩面中的至少一面,含有熱塑性樹脂及鍍敷觸媒,所述鍍敷形成層更滿足下述(1)及/或(2)的條件:
(1)所述鍍敷形成層含有分散所述鍍敷觸媒的分散劑;
(2)所述鍍敷形成層的表面側中所述鍍敷觸媒的存在量大於所述鍍敷形成層的所述基材側中所述鍍敷觸媒的存在量。
Description
本發明是有關於一種積層體。
近年來,隨著半導體電路的高積體化,要求於印刷配線板中形成更微細的配線電路。為了形成微細的配線電路,需要減薄配線的厚度。然而,即便是薄的金屬箔,亦有2 μm的厚度,因此微細電路形成性不充分,而存在生產性下降的問題。
針對此種問題,於專利文獻1中揭示了:將高分子膜、含有具有結晶性的熱塑性樹脂的鍍敷形成層、及鍍敷層依次積層而成的積層體是能夠形成微細電路的材料,進而可提高鍍敷形成層與鍍敷層的接著性及焊料耐熱性。
[現有技術文獻]
[專利文獻]
[專利文獻1]WO2009075212號手冊
[發明所欲解決之課題]
然而,對於專利文獻1的積層體,要求均衡地進一步提高常態下的接著性與焊料耐熱性。
因此,本發明提供一種能夠均衡地提高常態下的接著性與焊料耐熱性的積層體。
[解決課題之手段]
本發明者們為了解決所述課題而進行了積極研究,結果發現藉由使一種包括基材以及配置於所述基材的兩面中的至少一面,含有熱塑性樹脂及鍍敷觸媒的鍍敷形成層的積層體中,鍍敷形成層滿足特定的條件,可解決所述課題,從而完成了本發明。
即,本發明如下。
〔1〕
一種積層體,包括:
基材;以及
鍍敷形成層,配置於所述基材的兩面中的至少一面,含有熱塑性樹脂及鍍敷觸媒,
所述鍍敷形成層更滿足下述(1)及/或(2)的條件:
(1)所述鍍敷形成層含有分散所述鍍敷觸媒的分散劑;
(2)所述鍍敷形成層的表面側中所述鍍敷觸媒的存在量大於所述鍍敷形成層的所述基材側中所述鍍敷觸媒的存在量。
〔2〕
如〔1〕所述的積層體,其中所述分散劑是與所述鍍敷觸媒中所含的金屬原子相互作用而進行鍵結的化合物。
〔3〕
如〔2〕所述的積層體,其中所述化合物的末端基為含有氮原子的官能基。
〔4〕
如〔1〕至〔3〕中任一項所述的積層體,其中所述鍍敷形成層包括:樹脂層,含有所述熱塑性樹脂;以及觸媒層,配置於所述樹脂層上,含有所述鍍敷觸媒。
〔5〕
如〔4〕所述的積層體,其中所述觸媒層含有所述分散劑。
〔6〕
如〔4〕或〔5〕所述的積層體,其中所述鍍敷形成層更包括配置於所述樹脂層與所述觸媒層之間,於熱塑性樹脂中滲透有所述鍍敷觸媒及所述分散劑的邊界層。
〔7〕
如〔1〕至〔6〕中任一項所述的積層體,其中所述基材為熱硬化性聚醯亞胺樹脂。
〔8〕
如〔1〕至〔7〕中任一項所述的積層體,其中所述熱塑性樹脂為熱塑性聚醯亞胺樹脂。
〔9〕
如〔1〕至〔8〕中任一項所述的積層體,其中所述鍍敷觸媒含有鈀及/或銀。
〔10〕
如〔1〕至〔9〕中任一項所述的積層體,其更包括配置於所述鍍敷形成層上的金屬鍍敷層。
[發明的效果]
根據本發明,可提供一種能夠均衡地進一步提高常態下的接著性與焊料耐熱性的積層體。
以下,對用以實施本發明的形態(以下,稱為「本實施形態」)進行詳細記載。再者,本發明並不限定於以下的實施形態,可於其主旨的範圍內進行各種變形而加以實施。
[積層體]
本實施形態的積層體包括:基材;以及鍍敷形成層,配置於所述基材的兩面中的至少一面,含有熱塑性樹脂及鍍敷觸媒。鍍敷形成層更滿足下述(1)及/或(2)的條件。
(1)鍍敷形成層含有分散鍍敷觸媒的分散劑
(2)鍍敷形成層的表面側中鍍敷觸媒的存在量(Ca
)大於所述鍍敷形成層的所述基材側中所述鍍敷觸媒的存在量(Cb
)
藉由使鍍敷形成層滿足所述(1)及/或(2)的條件,包含其的積層體可均衡地提高常態下的接著性與焊料耐熱性,例如於設想到長期可靠性的接著性方面優異。此處,設想到長期可靠性的接著性例如是指即便進行150℃的加熱處理,亦充分抑制接著性的下降的性質。
藉由使鍍敷形成層滿足(1)及/或(2)的條件,積層體可均衡地提高常態下的接著性、設想到長期可靠性的接著性及焊料耐熱性的主要原因考慮如下。
印刷配線板用材料等中所使用的積層體包括:基材;鍍敷形成層,形成於基材的單面,含有熱塑性樹脂及鍍敷觸媒;以及金屬鍍敷層,形成於鍍敷形成層上。此處,此種積層體的接著性(常態下的接著性、設想到長期可靠性的接著性)及焊料耐熱性不充分的主要原因被認為是由於在鍍敷形成層與金屬鍍敷層的界面附近,鍍敷觸媒中所含的金屬(觸媒金屬)的存在量小。於是,為了加大所述界面附近觸媒金屬的存在量,而於鍍敷形成層中包含用於分散鍍敷觸媒的分散劑,或控制對鍍敷形成層中的鍍敷觸媒的存在量。由此,鍍敷金屬與觸媒金屬接觸的比例變大。其結果,觸媒金屬與鍍敷金屬容易接觸,從而認為積層體的接著性(常態下的接著性、設想到長期可靠性的接著性)及焊料耐熱性提高。
但是,主要因素並不限定於此。
(基材)
作為基材中的樹脂並無特別限定,例如可列舉:熱硬化性聚醯亞胺樹脂、液晶聚合物、聚苯硫醚、間規聚苯乙烯、聚對苯二甲酸乙二酯、聚萘二甲酸乙二酯、聚碳酸酯、聚對苯二甲酸丁二酯、聚醚醚酮、聚醚碸、聚苯醚、及氟系樹脂。該些樹脂可單獨使用一種,或者將兩種以上組合而使用。於該些中,就機械特性、熱特性及加熱時的尺寸穩定性更優異的觀點而言,樹脂較佳為熱硬化性聚醯亞胺樹脂。另外,於傳送高頻訊號的可撓性印刷配線板中,就介電特性的觀點而言,作為樹脂,較佳為液晶聚合物、或氟系樹脂。再者,液晶聚合物、及氟系樹脂的吸水率低,因此耐濕熱特性、高濕下的尺寸穩定性、及吸濕處理後的剝離強度亦變良好。
(熱硬化性聚醯亞胺樹脂)
熱硬化性聚醯亞胺樹脂例如是指300℃下的彈性係數相對於30℃下的彈性係數而保持為20%以上的聚醯亞胺樹脂。彈性係數例如是藉由動態黏彈性測定(Dynamic Mechanical Analysis,DMA)法而求出。作為熱硬化性聚醯亞胺樹脂,並無特別限定,例如可列舉藉由使酸二酐與二胺進行共聚而獲得的縮合型聚醯亞胺樹脂、雙馬來醯亞胺樹脂、及馬來醯亞胺樹脂。
作為酸二酐及二胺,例如脂肪族化合物、脂環式化合物、芳香族化合物均可使用。就耐熱性的觀點而言,作為酸二酐,較佳為芳香族四羧酸二酐,作為二胺,較佳為芳香族二胺。
作為酸二酐,例如可列舉:均苯四甲酸二酐、2,3,6,7-萘四羧酸二酐、3,3',4,4'-聯苯四羧酸二酐、1,2,5,6-萘四羧酸二酐、2,2',3,3'-聯苯四羧酸二酐、3,3',4,4'-二苯甲酮四羧酸二酐、4,4'-氧基二鄰苯二甲酸二酐、2,2-雙(3,4-二羧基苯基)丙烷二酐、3,4,9,10-苝四羧酸二酐、雙(3,4-二羧基苯基)丙烷二酐、1,1-雙(2,3-二羧基苯基)乙烷二酐、1,1-雙(3,4-二羧基苯基)乙烷二酐、雙(2,3-二羧基苯基)甲烷二酐、雙(3,4-二羧基苯基)乙烷二酐、雙(3,4-二羧基苯基)碸二酐、對苯雙(偏苯三甲酸單酯酸酐)、乙烯雙(偏苯三甲酸單酯酸酐)、及雙酚A雙(偏苯三甲酸單酯酸酐)。該些酸二酐可單獨使用一種,或者將兩種以上組合而使用。於該些中,就耐熱性及尺寸穩定性的觀點而言,較佳為選自由均苯四甲酸二酐、2,3,6,7-萘四羧酸二酐、2,2',3,3'-聯苯四羧酸二酐、3,3',4,4'-聯苯四羧酸二酐、及3,3',4,4'-二苯甲酮四羧酸二酐所組成的群組中的至少一種酸二酐。
作為二胺,例如可列舉:4,4'-二胺基二苯基丙烷、4,4'-二胺基二苯基甲烷、聯苯胺、3,3'-二氯聯苯胺、3,3'-二甲基聯苯胺、2,2'-二甲基聯苯胺、3,3'-二甲氧基聯苯胺、2,2'-二甲氧基聯苯胺、4,4'-二胺基二苯基硫醚、3,3'-二胺基二苯基碸、4,4'-二胺基二苯基碸、4,4'-氧二苯胺、3,3'-氧二苯胺、3,4'-氧二苯胺、1,5-二胺基萘、2,6-二胺基萘、4,4'-二胺基二苯基二乙基矽烷、4,4'-二胺基二苯基矽烷、4,4'-二胺基二苯基乙基氧化膦、4,4'-二胺基二苯基N-甲基胺、4,4'-二胺基二苯基N-苯基胺、1,4-二胺基苯(對苯二胺)、1,3-二胺基苯、1,2-二胺基苯、雙{4-(4-胺基苯氧基)苯基}碸、雙{4-(3-胺基苯氧基)苯基}碸、4,4'-雙(4-胺基苯氧基)聯苯、4,4'-雙(3-胺基苯氧基)聯苯、1,3-雙(3-胺基苯氧基)苯、1,3-雙(4-胺基苯氧基)苯、1,4-雙(4-胺基苯氧基)苯、3,3'-二胺基二苯甲酮、4,4'-二胺基二苯甲酮、及2,2-雙[4-(4-胺基苯氧基)苯基]丙烷。該些二胺可單獨使用一種,或者將兩種以上組合而使用。於該些中,就耐熱性及尺寸穩定性的觀點而言,較佳為含有選自由3,3'-二甲基聯苯胺、2,2'-二甲基聯苯胺、3,3'-二甲氧基聯苯胺、2,2'-二甲氧基聯苯胺、1,5-二胺基萘、及1,4-二胺基苯(對苯二胺)所組成的群組中的至少一種二胺。
基材於不阻礙本發明的作用效果的範圍內,可含有樹脂以外的成分,亦可不含有。
基材較佳為樹脂膜,更佳為樹脂膜為熱硬化性聚醯亞胺樹脂膜。熱硬化性聚醯亞胺樹脂膜可使用藉由公知的方法而製備的製備品,亦可使用市售品。作為市售品,可列舉東麗杜邦(Toray-Dupont)股份有限公司製品「卡普頓(Kapton)EN系列」、「卡普頓(Kapton)H系列」、「卡普頓(Kapton)V系列」、鐘淵化學(kaneka)股份有限公司製品「阿皮卡路(Apical)HP系列」、「阿皮卡路(Apical)NPI系列」、及宇部興產股份有限公司製品「尤皮萊庫斯(Upilex)S」。
就搬送性、絕緣性、及耐熱性等觀點而言,基材的積層方向的厚度較佳為5 μm〜500 μm。就同樣的觀點而言,厚度更佳為7.5 μm〜300 μm,進而佳為10 μm〜100 μm。
(鍍敷形成層)
鍍敷形成層只要配置於基材的兩面中的其中一面即可,亦可配置於基材的兩面。鍍敷形成層包含熱塑性樹脂及鍍敷觸媒。
(熱塑性樹脂)
熱塑性樹脂例如是指由於在玻璃轉移溫度(以下,亦稱為Tg)以上進行加熱時會軟化而具有軟化點溫度的樹脂。熱塑性樹脂可為未硬化的形態,亦可為硬化後的形態。作為熱塑性樹脂,例如可列舉:熱塑性聚醯亞胺樹脂、芳香族聚醚酮、聚苯硫醚、聚乙烯、聚丙烯、聚丁烯、結晶性聚丁二烯、聚甲基戊烯、聚醯胺、聚酯、聚胺基甲酸酯、液晶聚合物、聚苯乙烯等。該些熱塑性樹脂單獨使用一種,或者將兩種以上組合而使用。於該些中,就進一步提高焊料耐熱性的觀點而言,較佳為熱塑性聚醯亞胺樹脂。熱塑性聚醯亞胺樹脂例如是指300℃下的彈性係數相對於30℃下的彈性係數未滿20%的聚醯亞胺樹脂。
於本實施形態的積層體中,較佳為基材為熱硬化性聚醯亞胺樹脂,鍍敷形成層中所含的熱塑性樹脂為熱塑性聚醯亞胺樹脂。藉此,存在基材與鍍敷形成層的密接性進一步提高的傾向。
作為熱塑性聚醯亞胺樹脂,例如可列舉藉由使酸二酐與二胺共聚而獲得的聚醯亞胺樹脂。作為酸二酐及二胺,可列舉與所述熱硬化性聚醯亞胺樹脂中所使用者相同的酸二酐及二胺。
相對於鍍敷形成層整體而言的熱塑性樹脂的含量例如為1質量%~99質量%,較佳為20質量%~95質量%,更佳為40質量%~90質量%。
(鍍敷觸媒)
鍍敷觸媒含有貴金屬。作為鍍敷觸媒,只要為鍍敷處理(例如,無電解鍍敷處理)中通常所使用的觸媒即可。作為貴金屬,例如可列舉:鈀、銀、鉑、鎳、金及該些的合金。該些貴金屬亦可以離子的形態存在於鍍敷形成層中。該些貴金屬可單獨使用一種,或者將兩種以上組合而使用。於該些中,貴金屬較佳為鈀及/或銀。藉由使用此種貴金屬,當於鍍敷形成層上形成金屬鍍敷層(例如,銅鍍敷層)時,可減小金屬鍍敷層的厚度來進行鍍敷,因此存在可形成更微細的電路的傾向。
就使鍍敷層於接著層的表面均勻地析出的觀點而言,鍍敷觸媒理想的是貴金屬以膠體狀或均勻地分散於溶媒中。作為溶媒,並無特別限定,可列舉為了使貴金屬的粒子分散而通常所使用者,例如,可列舉:水、甲醇、乙醇、異丙醇等醇、己烷、環己酮、甲基乙基酮、丙酮、N-甲基-2-吡咯啶酮、N,N-二甲基乙醯胺、N,N-二甲基甲醯胺、甲苯、二乙醚、四氫呋喃(THF)、及該些的混合溶媒。
貴金屬的粒子的平均粒徑(D50)例如亦可為2 nm〜40 nm左右。平均粒徑為體積基準的平均粒徑,例如藉由基於動態光散射法(Dynamic Light Scattering,DLS)的粒徑分佈測定裝置而求出。再者,所謂D50是指體積累計50%的位置。
於貴金屬的粒子的平均粒徑(D50)為40 nm以下的情況下,貴金屬的表面積增加,觸媒活性上升。藉此,存在鍍敷的反應性提高的傾向。
相對於鍍敷形成層整體而言的鍍敷觸媒的含量例如為1質量%〜99質量%,較佳為5質量%〜80質量%,更佳為10質量%〜60質量%。
(分散劑)
鍍敷形成層含有分散鍍敷觸媒的分散劑。但是,只要鍍敷形成層滿足「(2)鍍敷形成層的表面側中鍍敷觸媒的存在量(Ca
)大於所述鍍敷形成層的所述基材側中所述鍍敷觸媒的存在量(Cb
)」的條件,則分散劑未必是必須的。分散劑較佳為與鍍敷觸媒中所含的金屬原子(觸媒金屬)相互作用而進行鍵結的化合物,更佳為該化合物是化合物的末端基為含有氮原子的官能基的化合物、具有不飽和鍵的化合物。作為鍵結形態,例如可為配位鍵結、離子鍵結、共價鍵結等。藉由使用此種分散劑,觸媒金屬均勻地分散於鍍敷形成層中。並且,藉由此分散,觸媒金屬與鍍敷金屬接觸的比例進一步變大,因此鍍敷金屬的析出性提高。其結果,於鍍敷形成層中,針孔的發生大幅減少。
相對於鍍敷形成層整體而言的分散劑的含量例如為1質量%~99質量%,較佳為10質量%~80質量%,更佳為20質量%~60質量%。
於將鍍敷形成層的表面側中鍍敷觸媒的存在量設為Ca
,並將鍍敷形成層的基材側中鍍敷觸媒的存在量設為Cb
時,鍍敷形成層滿足Ca
>Cb
。但是,鍍敷形成層於滿足所述(1)的條件的情況下,未必需要滿足Ca
>Cb
。Ca
及Cb
是使用X射線光電子分光分析裝置而求出。即。於鍍敷觸媒中所含的貴金屬為鈀(Pd)的情況下,鍍敷形成層的表面側中觸媒的存在量(鈀存在量(Pd)存在量)是使用X射線光電子分光分析裝置自表面側進行測定,並根據所檢測出的Pd的atomic%濃度求出。具體而言,將鈀(Pd)的atomic%濃度除以碳(C)的atomic%濃度而得的數值設為觸媒的存在量(鈀存在量(Pd存在量))Ca
。鍍敷形成層的基材側中觸媒的存在量是自鍍敷形成層的表面側藉由氬離子進行處理並處理至規定的部位後,使用X射線光電子分光分析裝置藉由與所述同樣的手法求出鍍敷形成層的基材側中鍍敷觸媒的存在量(鈀存在量(Pd存在量))Cb
。
藉此,鍍敷金屬與觸媒金屬接觸的比例變大。其結果,觸媒金屬與鍍敷金屬容易接觸,從而認為積層體的接著性(常態下的接著性、設想到長期可靠性的接著性)及焊料耐熱性提高。
作為滿足Ca
>Cb
的方法,例如可列舉於基材上形成含有熱塑性樹脂的樹脂層,並於所述樹脂層上積層含有所述分散劑的觸媒層等。
鍍敷形成層的厚度例如為10 nm~10 μm,就更有效且切實地收到本發明的作用效果的觀點而言,較佳為30 nm~8 μm,更佳為50 nm~6 μm。
鍍敷形成層可具有單層結構,亦可具有多層結構。於鍍敷形成層具有多層結構的情況下,就進一步提高接著性及焊料耐熱性的觀點而言,多層結構較佳為包括含有熱塑性樹脂的樹脂層及含有鍍敷觸媒的觸媒層,觸媒層較佳為更含有所述分散劑。於鍍敷形成層具有所述多層結構的情況下,例如於基材上配置(形成)有樹脂層,並於樹脂層上配置(形成)有觸媒層。
(樹脂層)
作為樹脂層中所含的熱塑性樹脂,可列舉與所述鍍敷形成層中所使用者相同的熱塑性樹脂。
樹脂層的厚度例如為10 nm~10 μm,就更有效且切實地收到本發明的作用效果的觀點而言,較佳為30 nm~8 μm,更佳為50 nm~6 μm。
(觸媒層)
觸媒層中所含的鍍敷觸媒及分散劑分別可列舉鍍敷形成層的項中例示的鍍敷觸媒及分散劑。
觸媒層的厚度例如為5 nm~300 nm,就更有效且切實地收到本發明的作用效果的觀點而言,較佳為10 nm~200 nm,更佳為20 nm~100 nm。
多層結構可僅包括樹脂層及觸媒層,亦可包括樹脂層、觸媒層、以及樹脂層及觸媒層以外的一種以上的其他層。
於該些中,鍍敷形成層較佳為更包括樹脂層、觸媒層以及配置於樹脂層與觸媒層之間的邊界層。邊界層例如是藉由在樹脂層的表面滲透鍍敷觸媒及分散劑而形成。藉由包括此種邊界層,樹脂層與觸媒層的層間密接性提高,其結果,存在剝離強度更優異的傾向。
邊界層的厚度例如為0.5 nm~300 nm,就更有效且切實地收到本發明的作用效果的觀點而言,較佳為1 nm~200 nm,更佳為2 nm~100 nm。
本實施形態的積層體可含有配置於鍍敷形成層上的鍍敷層,亦可不含有。
(鍍敷層)
作為鍍敷層,例如可列舉藉由金屬鍍敷處理而形成的金屬鍍敷層,作為金屬鍍敷層,可列舉:銅鍍敷層、金鍍敷層、錫鍍敷層、鎳鍍敷層、銀鍍敷層、鈀鍍敷層、焊料鍍敷層及無鉛焊料鍍敷層。
就更有效且切實地收到本發明的作用效果的觀點而言,鍍敷層的厚度較佳為0.05 μm〜35 μm,更佳為0.1 μm〜18 μm,進而佳為0.1 μm〜12 μm。
本實施形態的積層體可具有於基材的單面側依次積層有鍍敷形成層及鍍敷層的形態,亦可具有於基材的兩面側依次積層有鍍敷形成層及鍍敷層的形態。於本實施形態的積層體具有於基材的兩面側依次積層有鍍敷形成層及鍍敷層的形態的情況下,鍍敷形成層例如具有形成於基材的兩面中的其中一面的第一鍍敷形成層及形成於基材的兩面中的另一面的第二鍍敷形成層,鍍敷層具有形成於第一鍍敷形成層的表面上的第一鍍敷層及形成於第二鍍敷形成層的表面上的第二鍍敷層。第一鍍敷形成層與第二鍍敷形成層可相同亦可不同。
(特性)
本實施形態的積層體於常態下的接著性方面優異,90度方向剝離下的剝離強度例如為5.0 N/cm以上(例如,5.0 N/cm〜8.0 N/cm),較佳為6.0 N/cm以上,更佳為6.5 N/cm以上。
另外,本實施形態的積層體於設想到長期可靠性的接著性方面優異。因此,於溫度150℃的乾燥機中投入240小時後的剝離強度於90度剝離方向上,例如為5.0 N/cm以上(例如,5.0 N/cm〜8.0 N/cm),較佳為6.0 N/cm以上,更佳為6.5 N/cm以上。另外,於溫度85℃、濕度85%的恆溫恆濕器中投入240小時後的剝離強度於90度方向剝離下例如為5.0 N/cm以上(例如,5.0 N/cm〜8.0 N/cm),較佳為6.0 N/cm以上,更佳為6.5 N/cm以上。
(用途)
本實施形態的積層體可較佳地用於要求形成微細的配線電路的可撓性印刷配線板用材料。可撓性印刷配線板例如可較佳地用作積體電路(integrated circuit,IC)晶片安裝用的所謂晶片搭載可撓性印刷配線板、高密度電路形成用的可撓性印刷配線板。
[積層體的製造方法]
本實施形態的積層體的製造方法例如包括:鍍敷形成層形成步驟,於基材的至少一面上塗佈熱塑性樹脂及視需要含有所述分散劑的鍍敷觸媒原料,並進行乾燥,藉此形成鍍敷形成層,亦可更包括:鍍敷層形成步驟,於鍍敷形成層的與基材為相反側的面上進行鍍敷處理,藉此形成鍍敷層。本實施形態的製造方法藉由包括所述構成,而存在可提高所獲得的積層體的常態下的接著性及焊料耐熱性的傾向。
(鍍敷形成層形成步驟)
鍍敷形成層形成步驟是藉由在基材上塗佈熱塑性樹脂及鍍敷觸媒原料並進行乾燥而形成鍍敷形成層的步驟。
作為基材,並無特別限定,例如可列舉作為積層體的項中的基材而例示者。
作為熱塑性樹脂,並無特別限定,例如可列舉作為積層體的項中的熱塑性樹脂而例示者。於鍍敷形成層形成步驟中,例如熱塑性樹脂是以溶解或分散於有機溶媒中的形態來使用。作為有機溶媒,只要為能夠溶解或分散熱塑性樹脂的溶媒,則並無特別限定,例如可列舉:醇類(例如,甲醇、乙醇、丙醇、丁醇、戊醇、甘油、乙二醇、二乙二醇、三乙二醇、聚乙二醇、丙二醇、二丙二醇、三羥甲基乙烷、及三羥甲基丙烷)、醚類(例如,丁基乙醚等烷基醚、乙二醇單正丁醚等多元醇烷基醚類、及乙二醇單苯醚等多元醇芳醚類)、酮類(例如,甲基乙基酮、甲基異丁基酮、及環戊酮)、酯類(例如,乙酸丁酯、丙酸丙酯、及甲醚乙酸酯)、醯胺類(例如,N,N-二甲基甲醛、N,N-二甲基乙醯胺)、胺類(例如,單乙醇胺及二乙醇胺)、芳香族烴類(例如,甲苯及二甲苯)、含硫化合物(例如,二甲基亞碸)、及含氮雜環化合物(例如,N-甲基-2-吡咯啶酮、γ-丁內酯)。該些有機溶媒可單獨使用一種,或者將兩種以上組合而使用。有機溶媒中的熱塑性樹脂的濃度例如亦可為0.1質量%〜20質量%左右。
鍍敷觸媒原料含有貴金屬。作為貴金屬,並無特別限定,例如可列舉:鈀、銀、金、鉑、鎳及該些的合金。該些貴金屬可單獨使用一種,或者將兩種以上組合而使用。
鍍敷觸媒原料可直接添加貴金屬,亦可添加貴金屬化合物、與用以使貴金屬化合物還原而獲得貴金屬的還原劑,於鍍敷觸媒原料中藉由還原反應而使貴金屬析出。作為貴金屬化合物,並無特別限定,例如可列舉:鈀化合物(例如,氯化鈀、氟化鈀、溴化鈀、碘化鈀、硝酸鈀、硫酸鈀、氧化鈀、及硫化鈀)、銀化合物(例如,硝酸銀、氟化銀、氧化銀、及乙酸銀)、金化合物(例如,氰化金、三氯化金、三溴化金、氯化金鉀、氰化金鉀、氯化金鈉、及氰化金鈉)、鉑化合物(例如,氯化鉑、及硫酸鉑)、及鎳化合物(例如,氯化鎳、及硫酸鎳)。該些貴金屬化合物可單獨使用一種,或者將兩種以上組合而使用。
作為還原劑,並無特別限定,例如可列舉:氫化硼金屬鹽(例如,氫化硼鈉及氫化硼鉀)、氫化鋁鹽(例如,氫化鋁鋰、氫化鋁鉀、氫化鋁銫、氫化鋁鈹、氫化鋁鎂、及氫化鋁鈣)、肼化合物、羧酸類(例如,檸檬酸、甲酸、乙酸、富馬酸、蘋果酸、琥珀酸、抗壞血酸及該些的鹽)、一級或二級醇類(例如,甲醇、乙醇、異丙醇、及多元醇)、三級胺類(例如,三甲胺、三乙胺、二異丙基乙胺、二乙基甲胺、四甲基乙二胺[TMEDA]、及乙二胺四乙酸[EDTA])、羥基胺、酮類(例如,丙酮、及甲基乙基酮)、醚類(例如,二乙醚)、醛類(例如,甲醛、及乙醛)、酯類(例如,甲酸甲酯、乙酸甲酯、及乙酸乙酯)、及膦類(例如,三正丙基膦、三正丁基膦、三環己基膦、三苄基膦、三苯基膦、三乙氧基膦、1,2-雙(二苯基膦基)乙烷[DPPE]、1,3-雙(二苯基膦基)丙烷[DPPP]、1,1'-雙(二苯基膦基)二茂鐵[DPPF]、及2,2'-雙(二苯基膦基)-1,1'-聯萘[BINAP])。該些還原劑可單獨使用一種,或者將兩種以上組合而使用。
還原劑的使用量並無特別限定,例如亦可相對於貴金屬化合物100質量份而為10質量份〜1000質量份左右。
作為分散劑,例如可列舉作為積層體的項中的分散劑而例示者。於鍍敷形成層形成步驟中,例如分散劑以溶解或分散於有機溶媒中的形態來使用。作為有機溶媒,例如可列舉作為能夠溶解或分散熱塑性樹脂的溶媒而例示者。有機溶媒中的分散劑的濃度例如亦可為0.1質量%~10質量%左右。
於鍍敷形成層形成步驟中,可藉由將混合有熱塑性樹脂、鍍敷觸媒原料及視需要的分散劑的混合原料塗佈於基材的至少一面上並進行乾燥,而形成鍍敷形成層。另外,於鍍敷形成層形成步驟中,亦可藉由將熱塑性樹脂塗佈於基材的至少一面上並進行乾燥,而形成樹脂層,藉由將鍍敷觸媒原料及視需要的分散劑塗佈於樹脂層的表面上並進行乾燥,而形成觸媒層。於該情況下,鍍敷形成層包括樹脂層與觸媒層。
於鍍敷形成層形成步驟中,作為分別塗佈熱塑性樹脂、鍍敷觸媒原料及視需要的分散劑的方法,並無特別限定,例如可列舉:輥塗方式、吻式輥塗方式、凹版塗佈方式、反塗方式、輥刷方式、噴霧塗佈方式、浸漬輥塗方式、棒塗方式、刮刀塗佈方式、氣刀塗佈方式、簾幕式塗佈方式、模唇塗佈方式、及模塗機方式。
關於鍍敷形成層形成步驟中的乾燥條件,可根據使用的有機溶劑來適當設定乾燥溫度及時間。作為乾燥溫度的範圍,例如為60℃~300℃左右,作為乾燥時間,例如為5分鐘〜60分鐘左右。乾燥溫度可階段性地變化,亦可維持為固定。
(鍍敷層形成步驟)
鍍敷層形成步驟是藉由在接著層的與基材為相反側的面上進行鍍敷處理而形成鍍敷層的步驟。作為鍍敷處理,可列舉:無電解鍍敷處理、電氣鍍敷處理及將該些組合的處理。若於該些鍍敷處理中使用無電解鍍敷處理,則可應用於作為圖案形成方法之一的半加成法,可應對兩面窄間距化,故較佳。
作為無電解鍍敷處理及電氣鍍敷處理的各處理條件,可使用公知的處理條件。更詳細而言,可使用實施例中記載的處理條件。
再者,本說明書中的各物性只要無特別標明,則可依據以下的實施例中所記載的方法來測定。
實施例
以下,藉由實施例及比較例來對本發明進行更具體的說明,但本發明並不僅僅限定於該些實施例。
以下,對本發明的樹脂層的原料即熱塑性樹脂的合成例進行具體的說明,但本發明並不僅僅限定於該些合成例。
熱塑性樹脂的合成中使用的酸二酐、二胺及溶劑如下。
p-PDA:對苯二胺(關東化學股份有限公司製造)
BAPP:2,2-雙(4-胺基苯氧基苯基)異丙烷(和歌山精化工業股份有限公司製造)
TPE-R:1,3-雙(4-胺基苯氧基)苯(和歌山精化工業股份有限公司製造)
4,4'-DPE:4,4'-二胺基二苯基醚(和歌山精化工業股份有限公司製造)
BPDA:3,4,3',4'-聯苯基四羧酸二酐(宇部興產股份有限公司製造)
DMAc:N,N-二甲基乙醯胺(關東化學股份有限公司製造)
NMP:N-甲基-2-吡咯啶酮(關東化學股份有限公司製造)
[合成例1]
向反應容器之中添加DMAc 85 g、BAPP 1.034 g(0.003 mol)及TPE-R 6.628 g(0.023 mol)後,於室溫下進行攪拌,使BAPP、TPE-R溶解於DMAc中。向所獲得的溶液中緩慢地添加BPDA 7.338 g(0.025 mol)。其後,藉由在室溫下攪拌3小時而獲得樹脂組成物(聚醯胺酸溶液)。以所獲得的聚醯胺酸溶液的固體成分濃度成為2質量%的方式利用DMAc進行稀釋,獲得聚醯胺酸溶液A。
[合成例2]
向反應容器之中添加DMAc 85 g、BAPP 5.645 g(0.014 mol)及TPE-R 2.680 g(0.009 mol)後,於室溫下進行攪拌,使BAPP、TPE-R溶解於DMAc中。向所獲得的溶液中緩慢地添加BPDA 6.675 g(0.023 mol)。其後,藉由在室溫下攪拌3小時而獲得樹脂組成物(聚醯胺酸溶液)。以所獲得的聚醯胺酸溶液的固體成分濃度成為2質量%的方式利用DMAc進行稀釋,獲得聚醯胺酸溶液B。
[合成例3]
向反應容器之中添加DMAc 85 g、p-PDA 4.061 g(0.038 mol)後,於40℃下進行攪拌,使p-PDA溶解於DMAc中。向所獲得的溶液中緩慢地添加BPDA 10.939 g(0.037 mol)。其後,藉由在室溫下攪拌3小時而獲得樹脂組成物(聚醯胺酸溶液)。以所獲得的聚醯胺酸溶液的固體成分濃度成為2質量%的方式利用DMAc進行稀釋,獲得聚醯胺酸溶液C。
[實施例1]
使用棒塗機將合成例1中合成的熱塑性聚醯亞胺樹脂的前驅物樹脂溶液即2質量%聚醯胺酸溶液A塗佈於作為基材的具有38 μm的厚度的熱硬化性聚醯亞胺樹脂膜(東麗杜邦(Toray-Dupont)股份有限公司製品「卡普頓(Kapton)150EN-C,線熱膨脹係數13 ppm,玻璃轉移溫度320℃,Ra為0.03 μm」)的單面,於60℃〜250℃、10分鐘左右的乾燥條件下進行乾燥,藉此形成具有150 nm的厚度的樹脂層(樹脂層形成步驟)。其次,使用棒塗機將含有Pd作為鍍敷觸媒且含有具有銨基的分散劑的藥劑A(日產化學股份有限公司製造CP系列)塗佈於樹脂層表面,於120℃下乾燥10分鐘左右,進而於250℃下乾燥15分鐘左右,藉此形成具有50 nm的厚度的觸媒層(觸媒層形成步驟)。將如此形成的形成體於奧野製藥工業股份有限公司製品OPC copper HFS(初期Cu濃度2.5 g/l,浴容積500 ml,40℃,40分鐘)中浸漬5分鐘左右,於觸媒層的表面形成具有0.3 μm的厚度的金屬鍍敷層(化學鍍敷步驟)。進而,藉由電解鍍敷處理而將金屬鍍敷層的厚度製成0.3 μm至12 μm(電解鍍敷步驟)。藉此,獲得積層體。使用掃描型電子顯微鏡觀察所獲得的積層體的剖面圖,可知積層體於樹脂層與觸媒層之間形成了邊界層。將所獲得的積層體的剖面圖示於圖1。如圖1中所示,此積層體於基材上依次積層有樹脂層、邊界層、觸媒層。
[實施例2]
於樹脂層形成步驟中,使用合成例2中合成的熱塑性聚醯胺樹脂的前驅物樹脂溶液即2質量%聚醯胺酸溶液B代替合成例1中合成的熱塑性聚醯亞胺樹脂的前驅物樹脂溶液即2質量%聚醯胺酸溶液A,除此以外以與實施例1同樣的方式獲得積層體。
[比較例1]
於樹脂層形成步驟中,使用合成例3中合成的熱硬化性聚醯亞胺樹脂的前驅物樹脂溶液即2質量%聚醯胺酸溶液C代替合成例1中合成的熱塑性聚醯亞胺樹脂的前驅物樹脂溶液即2質量%聚醯胺酸溶液A,除此以外以與實施例1同樣的方式獲得積層體。
[比較例2]
不進行樹脂層形成步驟,於觸媒層形成步驟中,將所述藥劑A塗佈於基材的單面,除此以外以與實施例1同樣的方式獲得積層體。
[實施例3]
使用棒塗機將以質量比10:1混合合成例1中合成的熱塑性聚醯亞胺樹脂的前驅物樹脂溶液即2質量%聚醯胺酸溶液A與實施例1的藥劑A而成的溶液(樹脂濃度為0.5質量%、Pd濃度為0.136質量%)塗佈於基材的單面,於120℃下乾燥10分鐘左右,進而於250℃下乾燥15分鐘左右,藉此形成具有100 nm的厚度的鍍敷形成層。將如此形成的形成體於奧野製藥工業股份有限公司製品OPC copper HFS(初期Cu濃度2.5 g/l,浴容積500 ml,40℃,40分鐘)中浸漬5分鐘左右,於觸媒層的表面形成具有0.3 μm的厚度的金屬鍍敷層(化學鍍敷步驟)。進而,藉由電解鍍敷處理而將金屬鍍敷層的厚度製成0.3 μm至12 μm(電解鍍敷步驟)。藉此,獲得積層體。
[實施例4]
作為基材,將於熱硬化性樹脂層的兩面具有熱塑性聚醯亞胺樹脂層的25 μm的黏合片(bond ply)膜:鐘淵化學(kaneka)股份有限公司製品「皮庫西奧(Pixeo)FRS-142、線膨脹係數20 ppm」於40℃的10重量%(wt%)KOH水溶液中浸漬60分鐘左右使聚醯亞胺樹脂層膨潤後,於其單面使用棒塗機將含有Pd作為鍍敷觸媒,且含有具有銨基的分散劑的藥劑A塗佈於基材表面,於120℃下乾燥10分鐘左右,進而於250℃下乾燥15分鐘左右,藉此形成具有50 nm的厚度的觸媒層。針對如此形成的形成體以與實施例1同樣的方式獲得積層體。
[實施例5]
於作為基材的、於熱硬化性樹脂層的兩面具有熱塑性聚醯亞胺樹脂層的25 μm的黏合片(bond ply)膜:鐘淵化學(kaneka)股份有限公司製品「皮庫西奧(Pixeo)FRS-142、線膨脹係數20 ppm」的單面,使用棒塗機將含有Pd作為鍍敷觸媒,且含有具有銨基的分散劑的藥劑A塗佈於基材表面,於120℃下乾燥10分鐘左右,進而於氮環境下300℃下乾燥30分鐘左右,藉此形成具有50 nm的厚度的觸媒層。針對如此形成的形成體以與實施例1同樣的方式獲得積層體。
測定各實施例及比較例的積層體的各物性。將測定結果示於表1。根據此測定結果,可知若基材側的樹脂層中鍍敷及鍍敷觸媒原料即金屬的存在少,則熱處理後或濕熱處理後的剝離強度的下降被抑制。作為其原因之一,雖是推測,但考慮是因樹脂層中的所述金屬的存在少,熱對樹脂產生的影響小。再者,各物性的測定方法是利用以下的方法進行。
各評價方法及測定方法如下。
[各層的厚度]
各層的厚度的測定是利用超薄切片機(ultramicrotome)EM UC6(徠卡(LEICA)公司製造)將樣品切削為50 nm~150 nm厚度,針對其剖面使用掃描型電子顯微鏡S-4800(日立公司製造)觀察剖面透射像,據此算出厚度。
[鈀存在量]
鈀存在量的測定是使用X射線光電子分光分析裝置來進行測定。更具體而言,鍍敷形成層的表面側中觸媒的存在量(鈀存在量(Pd存在量))是使用X射線光電子分光分析裝置自表面側進行測定,並根據所檢測出的Pd的atomic%濃度求出。更具體而言,將鈀(Pd)的atomic%濃度除以碳(C)的atomic%濃度而得的數值設為觸媒的存在量(鈀存在量(Pd存在量))。鍍敷形成層的基材側中觸媒的存在量是自基材側藉由氬離子進行處理並處理至規定的部位後,使用X射線光電子分光分析裝置藉由與所述同樣的手法求出鍍敷形成層的基材側中鍍敷觸媒的存在量(鈀存在量(Pd存在量))。
(評價基準)
〇:可確認到Pd的存在量為表面側>基材側(Ca
>Cb
)。
×:未能確認到Pd的存在量為表面側>基材側(Ca
>Cb
)。
[常態的剝離強度]
剝離強度的測定是依據JIS C6471來進行。更詳細而言,於各積層體的銅鍍敷層表面對3 mm寬度的蝕刻抗蝕劑進行圖案化後,藉由蝕刻來去除殘餘的銅鍍敷層,藉此獲得樣品。利用雙面膠帶將所獲得的樣品固定於增強板,將銅鍍敷層自增強板沿90°方向剝離並進行強度測定,藉此測定剝離強度。剝離速度是設為50 mm/分。表中的評價基準如下。
(評價基準)
○:剝離強度為5 N以上。
△:剝離強度為3 N以上且未滿5 N。
×:剝離強度未滿3 N。
[熱處理後的剝離強度]
於各積層體的銅鍍敷層表面以3 mm寬度對蝕刻抗蝕劑進行圖案化後,藉由蝕刻來去除殘餘的銅鍍敷層,藉此獲得樣品。將所述樣品於調整為溫度150℃的乾燥機中保存240小時。利用雙面膠帶將自乾燥機中取出的樣品固定於增強板,將銅鍍敷層自增強板沿90°方向剝離,測定剝離強度。剝離速度設為50 mm/分。表中的評價基準如下。
(評價基準)
○:剝離強度為5 N以上。
△:剝離強度為3 N以上且未滿5 N。
×:剝離強度未滿3 N。
[濕熱處理後的剝離強度]
於各積層體的銅鍍敷層表面以3 mm寬度對蝕刻抗蝕劑進行圖案化後,藉由蝕刻來去除殘餘的銅鍍敷層,藉此獲得樣品。將所述樣品於調整為溫度85℃濕度85%的濕熱機中保存240小時。利用雙面膠帶將自乾燥機中取出的樣品固定於增強板,將銅鍍敷層自增強板沿90°方向剝離,測定剝離強度。剝離速度設為50 mm/分。表中的評價基準如下。
(評價基準)
○:剝離強度為5 N以上。
△:剝離強度為3 N以上且未滿5 N。
×:剝離強度未滿3 N。
[焊料耐熱試驗]
將各積層體切為30 mm×30 mm。將各積層體的銅鍍敷層側設為焊料浴槽側,並進行60秒浮動處理。藉由目視確認處理後的外觀,並確認收縮、膨脹、及剝落的有無。自240℃至340℃以10℃為單位進行試驗,求出無收縮、膨脹、及剝落的最大溫度。再者,表1中,於240℃下發生收縮、膨脹、及剝落中的任一者的情況記載為「未滿240℃」,於340℃下看不到收縮、膨脹、及剝落中的任一者的情況記載為「340℃<」。
本申請案基於2018年9月5日向日本專利廳提出申請的日本專利申請案(日本專利特願2018-166271),其內容以參照的形式被併入本申請案中。
[產業上之可利用性]
本發明的積層體具有在產業上用作可撓性印刷配線板中所使用的材料的可能性。
無
圖1是表示實施例1中的、使用掃描型電子顯微鏡而觀察的積層體的剖面圖。
Claims (10)
- 一種積層體,包括: 基材;以及 鍍敷形成層,配置於所述基材的兩面中的至少一面,含有熱塑性樹脂及鍍敷觸媒, 所述鍍敷形成層更滿足下述(1)及/或(2)的條件: (1)所述鍍敷形成層含有分散所述鍍敷觸媒的分散劑; (2)所述鍍敷形成層的表面側中所述鍍敷觸媒的存在量大於所述鍍敷形成層的所述基材側中所述鍍敷觸媒的存在量。
- 如申請專利範圍第1項所述的積層體,其中所述分散劑是與所述鍍敷觸媒中所含的金屬原子相互作用而進行鍵結的化合物。
- 如申請專利範圍第2項所述的積層體,其中所述化合物的末端基為含有氮原子的官能基。
- 如申請專利範圍第1項至第3項中任一項所述的積層體,其中所述鍍敷形成層包括: 樹脂層,含有所述熱塑性樹脂;以及 觸媒層,配置於所述樹脂層上,含有所述鍍敷觸媒。
- 如申請專利範圍第4項所述的積層體,其中所述觸媒層含有所述分散劑。
- 如申請專利範圍第4項所述的積層體,其中所述鍍敷形成層更包括配置於所述樹脂層與所述觸媒層之間,於熱塑性樹脂中滲透有所述鍍敷觸媒及所述分散劑的邊界層。
- 如申請專利範圍第1項至第3項中任一項所述的積層體,其中所述基材為熱硬化性聚醯亞胺樹脂。
- 如申請專利範圍第1項至第3項中任一項所述的積層體,其中所述熱塑性樹脂為熱塑性聚醯亞胺樹脂。
- 如申請專利範圍第1項至第3項中任一項所述的積層體,其中所述鍍敷觸媒含有鈀及/或銀。
- 如申請專利範圍第1項至第3項中任一項所述的積層體,其更包括配置於所述鍍敷形成層上的金屬鍍敷層。
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