TW201522591A - Sealing thermosetting-resin sheet and hollow-package manufacturing method - Google Patents

Sealing thermosetting-resin sheet and hollow-package manufacturing method Download PDF

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Publication number
TW201522591A
TW201522591A TW103138715A TW103138715A TW201522591A TW 201522591 A TW201522591 A TW 201522591A TW 103138715 A TW103138715 A TW 103138715A TW 103138715 A TW103138715 A TW 103138715A TW 201522591 A TW201522591 A TW 201522591A
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TW
Taiwan
Prior art keywords
thermosetting resin
resin sheet
sealing
sheet
resin
Prior art date
Application number
TW103138715A
Other languages
Chinese (zh)
Inventor
Eiji Toyoda
Takashi Habu
Tomoaki Ichikawa
yusaku Shimizu
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Nitto Denko Corp
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Application filed by Nitto Denko Corp filed Critical Nitto Denko Corp
Publication of TW201522591A publication Critical patent/TW201522591A/en

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    • H—ELECTRICITY
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    • H01L21/50—Assembly of semiconductor devices using processes or apparatus not provided for in a single one of the subgroups H01L21/06 - H01L21/326, e.g. sealing of a cap to a base of a container
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    • H03H—IMPEDANCE NETWORKS, e.g. RESONANT CIRCUITS; RESONATORS
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  • Engineering & Computer Science (AREA)
  • Power Engineering (AREA)
  • Computer Hardware Design (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • General Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • Physics & Mathematics (AREA)
  • Manufacturing & Machinery (AREA)
  • Structures Or Materials For Encapsulating Or Coating Semiconductor Devices Or Solid State Devices (AREA)
  • Encapsulation Of And Coatings For Semiconductor Or Solid State Devices (AREA)
  • Surface Acoustic Wave Elements And Circuit Networks Thereof (AREA)
  • Micromachines (AREA)
  • Manufacture Of Macromolecular Shaped Articles (AREA)
  • Laminated Bodies (AREA)
  • Compositions Of Macromolecular Compounds (AREA)

Abstract

This invention provides a sealing thermosetting-resin sheet and a hollow-package manufacturing method whereby it is difficult for the material constituting said sealing thermosetting-resin sheet to flow into gaps between an adherend and an electronic device. This invention pertains to a sealing thermosetting-resin sheet that is used to manufacture a hollow package. When cured, said sealing thermosetting-resin sheet has a domain-matrix structure comprising a matrix part consisting primarily of a first resin component and domain parts consisting primarily of a second resin component, with the matrix part being softer than the domain parts.

Description

密封用熱硬化性樹脂薄片及中空封裝(hollow package)之製造方法 Thermosetting resin sheet for sealing and method for producing hollow package

本發明係關於密封用熱硬化性樹脂薄片及中空封裝之製造方法。 The present invention relates to a thermosetting resin sheet for sealing and a method for producing a hollow package.

電子裝置封裝之製作中，代表性係採用以密封樹脂將透過凸塊等固定於基板等之1個或複數個電子裝置予以密封，並視需要以成為電子裝置單位之封裝之方式切割密封體之程序。作為該密封樹脂係使用薄片狀之密封樹脂。 In the production of the electronic device package, one or a plurality of electronic devices that are fixed to the substrate by a bump or the like by a sealing resin are used for sealing, and the sealing body is cut as a package of the electronic device unit as needed. program. A sheet-shaped sealing resin is used as the sealing resin.

近年來，與半導體封裝並列，已進展SAW(表面聲波(Surface Acoustic Wave))濾波器、或CMOS(互補式金屬氧化物半導體(Complementary Metal Oxide Semiconductor)感測器、加速度感測器等之稱為MEMS之微小電子裝置之開發。密封該等電子裝置之封裝分別具有用以確保一般之表面彈性波之傳播或光學系統之維持、電子裝置可動構件之可動性等之中空構造。該中空構造大多設置為基板與元件間之空隙。密封時，必須以確保可動構 件之作動信賴性或元件之連接信賴性之方式一面維持中空構造一面密封。例如，專利文獻1中記載使用凝膠狀之硬化性樹脂薄片對功能元件進行中空模製之技術。 In recent years, in parallel with semiconductor packages, SAW (Surface Acoustic Wave) filters, or CMOS (Complementary Metal Oxide Semiconductor) sensors, acceleration sensors, etc. have been developed. Development of microelectronic devices for MEMS. The packages for sealing these electronic devices each have a hollow structure for ensuring propagation of a general surface acoustic wave or maintenance of an optical system, mobility of an movable member of an electronic device, and the like. It is the gap between the substrate and the component. When sealing, it must be ensured to be movable. The method of making the reliability or the connection reliability of the components is sealed while maintaining the hollow structure. For example, Patent Document 1 describes a technique of performing hollow molding of a functional element using a gel-like curable resin sheet.

[先前技術文獻] [Previous Technical Literature]

[專利文獻] [Patent Literature]

[專利文獻1]日本特開2006-19714號公報 [Patent Document 1] Japanese Patent Laid-Open Publication No. 2006-19714

關於中空封裝之製造方法，藉由例如包含下述步驟之方法可製造中空封裝：使具備被黏著體與安裝於被黏著體上之電子裝置之裝置安裝體、以及配置於裝置安裝體上之密封用熱硬化性樹脂薄片之層合體進行加壓，形成具備被黏著體、安裝於被黏著體上之電子裝置及包覆電子裝置之密封用熱硬化性樹脂薄片之密封體之步驟，藉加熱密封體使密封用熱硬化性樹脂薄片硬化，形成硬化體之步驟。該製造方法中，期望不使構成樹脂薄片之材料流入被黏著體與電子裝置間之空隙。 Regarding the manufacturing method of the hollow package, a hollow package can be manufactured by, for example, a method including the following steps: a device mounting body including an adherend and an electronic device mounted on the adherend, and a seal disposed on the device mounting body Pressing a laminate of a thermosetting resin sheet to form a sealing body having an adherend, an electronic device mounted on the adherend, and a thermosetting resin sheet for sealing covering the electronic device, and sealing by heat The step of curing the thermosetting resin sheet for sealing to form a hardened body. In this manufacturing method, it is desirable that the material constituting the resin sheet does not flow into the gap between the adherend and the electronic device.

本發明係鑑於上述課題而完成者，其目的係提供一種難以使構成密封用熱硬化性樹脂薄片之材料流入被黏著體與電子裝置間之空隙的密封用熱硬化性樹脂薄片及中空封裝之製造方法。 The present invention has been made in view of the above-described problems, and an object of the invention is to provide a thermosetting resin sheet for sealing and a hollow package in which it is difficult to cause a material constituting a thermosetting resin sheet for sealing to flow into a gap between an adherend and an electronic device. method.

本發明係關於用於製造中空封裝所使用之密封用熱硬化性樹脂薄片。本發明之密封用熱硬化性樹脂薄片之硬化物具備包含第1樹脂成分作為主成分之基質(matrix)部及包含第2樹脂成分作為主成分之區域(domain)部之海島構造，且基質部比區域部更柔軟。 The present invention relates to a thermosetting resin sheet for sealing used for manufacturing a hollow package. The cured product of the thermosetting resin sheet for sealing of the present invention has a matrix portion including a matrix portion containing a first resin component as a main component and a domain portion including a second resin component as a main component, and a matrix portion. It is softer than the area.

本發明之密封用熱硬化性樹脂薄片難以使構成密封用熱硬化性樹脂薄片之材料流入到被黏著體與電子裝置之間之空隙。其理由雖不清楚，但推測藉由對使用本發明之密封用熱硬化性樹脂薄片而得之密封體加熱，而進行包含區域部與比區域部柔軟之基質部之海島構造之形成，故不會使構成密封用熱硬化性樹脂薄片之材料過度流動之故。 In the thermosetting resin sheet for sealing of the present invention, it is difficult for the material constituting the thermosetting resin sheet for sealing to flow into the gap between the adherend and the electronic device. Though the reason for this is not clear, it is presumed that the sealing body obtained by using the thermosetting resin sheet for sealing of the present invention is heated, and the island structure including the region portion and the matrix portion which is softer than the region portion is formed. The material constituting the thermosetting resin sheet for sealing is excessively flowed.

硬化物較好進一步包含分散於基質部中之填料。據此，使構成密封用熱硬化性樹脂薄片之材料更難流入到被黏著體與電子裝置之間之空隙。 The cured product preferably further comprises a filler dispersed in the matrix portion. According to this, it is more difficult for the material constituting the thermosetting resin sheet for sealing to flow into the gap between the adherend and the electronic device.

本發明之密封用熱硬化性樹脂薄片較好含有熱可塑性樹脂及熱硬化性樹脂。基於使構成密封用熱硬化性樹脂薄片之材料難以流入被黏著體與電子裝置間之空隙之理由，較好第1樹脂成分為熱可塑性樹脂，第2樹脂成分為熱硬化性樹脂。 The thermosetting resin sheet for sealing of the present invention preferably contains a thermoplastic resin and a thermosetting resin. The reason why it is difficult for the material constituting the thermosetting resin sheet for sealing to flow into the gap between the adherend and the electronic device is that the first resin component is a thermoplastic resin, and the second resin component is a thermosetting resin.

區域部之最大粒徑較好為0.01μm~5μm。據此，使構成密封用熱硬化性樹脂薄片之材料更難流入到被黏著體與電子裝置之間之空隙。其原因為相對於構成位在 空隙附近之密封用熱硬化性樹脂薄片之材料，可賦予如觸變性般作用，而可限制構成密封用熱硬化性樹脂薄片之材料之流動所致。 The maximum particle diameter of the region portion is preferably from 0.01 μm to 5 μm. According to this, it is more difficult for the material constituting the thermosetting resin sheet for sealing to flow into the gap between the adherend and the electronic device. The reason is relative to the composition The material of the thermosetting resin sheet for sealing in the vicinity of the void can impart a thixotropic action and can restrict the flow of the material constituting the thermosetting resin sheet for sealing.

熱可塑性樹脂之酸價較好為1mgKOH/g~100mgKOH/g。酸價為1mgKOH/g~100mgKOH/g時，可容易地形成最大粒徑為0.01μm~5μm之區域部。 The acid value of the thermoplastic resin is preferably from 1 mgKOH/g to 100 mgKOH/g. When the acid value is from 1 mgKOH/g to 100 mgKOH/g, a region having a maximum particle diameter of from 0.01 μm to 5 μm can be easily formed.

本發明另關於一種中空封裝之製造方法，其包含使具備被黏著體及具備安裝於前述被黏著體之電子裝置之裝置安裝體、以及配置於裝置安裝體上之密封用熱硬化性樹脂薄片之層合體進行加壓，形成具備前述被黏著體、安裝於被黏著體之電子裝置及覆蓋電子裝置之密封用熱硬化性樹脂薄片之密封體之步驟。 Further, the present invention relates to a method of manufacturing a hollow package, comprising: a device mounting body including an adherend and an electronic device mounted on the adherend; and a thermosetting resin sheet for sealing disposed on the device mounting body. The laminate is pressurized to form a sealing body including the adherend, the electronic device attached to the adherend, and the sealing thermosetting resin sheet covering the electronic device.

2‧‧‧裝置安裝體 2‧‧‧Device installation

11‧‧‧熱硬化性樹脂薄片 11‧‧‧ thermosetting resin sheet

12‧‧‧隔膜 12‧‧‧Separator

22‧‧‧基板 22‧‧‧Substrate

23‧‧‧SAW晶片 23‧‧‧SAW chip

24‧‧‧突起電極 24‧‧‧ protruding electrode

25‧‧‧中空部 25‧‧‧ Hollow

26‧‧‧硬化樹脂 26‧‧‧ hardened resin

31‧‧‧層合體 31‧‧‧Layer

32‧‧‧密封體 32‧‧‧ Sealing body

33‧‧‧硬化體 33‧‧‧ hardened body

34‧‧‧中空封裝 34‧‧‧ hollow package

41‧‧‧下側加熱板 41‧‧‧lower heating plate

42‧‧‧上側加熱板 42‧‧‧Upper heating plate

圖1係熱硬化性樹脂薄片之概略剖面圖。 Fig. 1 is a schematic cross-sectional view showing a thermosetting resin sheet.

圖2係硬化物之剖面之TEM觀察像。下段之觀察像為上段之觀察像之部分放大像。 Fig. 2 is a TEM observation image of a cross section of a cured product. The observation of the lower section is a partial enlarged image of the observation image of the upper section.

圖3係硬化物之剖面之AFM相位像。為了清晰地顯示海島構造，而觀察使包含環氧樹脂、酚樹脂、熱可塑性樹脂及硬化促進劑，不含填料及顏料之熱硬化性樹脂薄片硬化所得之硬化物。 Figure 3 is an AFM phase image of the section of the cured product. In order to clearly show the sea-island structure, a cured product obtained by curing an epoxy resin, a phenol resin, a thermoplastic resin, a curing accelerator, and a thermosetting resin sheet containing no filler or pigment was observed.

圖4係硬化物之剖面TEM觀察像。為了清晰地顯示海島構造，而觀察包含環氧樹脂、酚樹脂、熱可塑性樹脂 及硬化促進劑，不含填料及顏料之熱硬化性樹脂薄片硬化所得之硬化物。 Fig. 4 is a cross-sectional TEM observation image of a cured product. In order to clearly show the structure of the island, it is observed that it contains epoxy resin, phenol resin, thermoplastic resin. And a hardening accelerator, a cured product obtained by hardening a thermosetting resin sheet containing no filler or pigment.

圖5係顯示將層合體配置於下側加熱板與上側加熱板之間之狀態之概略的剖面圖。 Fig. 5 is a schematic cross-sectional view showing a state in which a laminate is placed between a lower heating plate and an upper heating plate.

圖6係顯示以平行平板方式熱壓製層合體之樣態之概略剖面圖。 Fig. 6 is a schematic cross-sectional view showing a state in which a laminate is thermally pressed in a parallel flat plate manner.

圖7係顯示自熱壓製所得之密封體剝離隔膜之樣態之概略剖面圖。 Fig. 7 is a schematic cross-sectional view showing a state in which the sealing body of the sealing body obtained by the hot pressing is peeled off.

圖8係藉加熱密封體所得之硬化體之概略剖面圖。 Fig. 8 is a schematic cross-sectional view showing a hardened body obtained by heating a sealing body.

圖9係使硬化體單片化所得之中空封裝之概略剖面圖。 Fig. 9 is a schematic cross-sectional view showing a hollow package obtained by singulating a hardened body.

圖10係實施例1之試驗片之TEM觀察像。 Fig. 10 is a TEM observation image of the test piece of Example 1.

圖11係比較例1之試驗片之TEM觀察像。 Fig. 11 is a TEM observation image of the test piece of Comparative Example 1.

以下揭示實施形態詳細說明本發明，但本發明並非僅限於該等實施形態。 Hereinafter, the present invention will be described in detail with reference to the embodiments, but the present invention is not limited to the embodiments.

[實施形態1] [Embodiment 1]

(熱硬化性樹脂薄片11) (thermosetting resin sheet 11)

針對熱硬化性樹脂薄片11加以說明。 The thermosetting resin sheet 11 will be described.

如圖1所示，熱硬化性樹脂薄片11之形態為薄片狀。熱硬化性樹脂薄片11代表性為以配置於聚對苯二甲酸乙二酯(PET)薄膜等隔膜12上之狀態提供。為使樹 脂薄片11可容易地自隔膜12剝離，隔膜12較好施以脫模處理。 As shown in FIG. 1, the form of the thermosetting resin sheet 11 is a sheet shape. The thermosetting resin sheet 11 is typically provided in a state of being disposed on a separator 12 such as a polyethylene terephthalate (PET) film. For the tree The lipid sheet 11 can be easily peeled off from the separator 12, and the separator 12 is preferably subjected to a release treatment.

熱硬化性樹脂薄片11具備熱硬化性。 The thermosetting resin sheet 11 is provided with thermosetting properties.

熱硬化性樹脂薄片11係藉硬化反應而誘發相分離。亦即，熱硬化性樹脂薄片11係藉硬化反應而誘發海島構造之形成。 The thermosetting resin sheet 11 induces phase separation by a hardening reaction. In other words, the thermosetting resin sheet 11 induces the formation of an island structure by a hardening reaction.

圖2系顯示以透過型電子顯微鏡(TEM)觀察熱硬化性樹脂薄片11之硬化物所得之觀察像。配置於上段左邊之觀察像中，觀察像之上部可確認基質部的顏色深之部分、與區域部的顏色淡之部分。配置於上段右邊之觀察像中，於觀察像之上部亦可確認基質部的顏色深之部分、與區域部的顏色淡之部分。又，圓形物體為填料。 2 is an observation image obtained by observing a cured product of the thermosetting resin sheet 11 by a transmission electron microscope (TEM). In the observation image arranged on the left side of the upper section, the portion where the color of the matrix portion is deep and the portion of the region portion is light is observed. In the observation image disposed on the right side of the upper section, the portion where the color of the matrix portion is deep and the portion where the color of the region portion is light can be confirmed in the upper portion of the observation image. Also, the circular object is a filler.

如圖2所示，熱硬化性樹脂薄片11之硬化物包含含有基質部(以下亦稱為海相)及分散於基質部中之區域部(亦下亦稱為島相)之海島構造，與分散於基質部中之填料。基質部比區域部柔軟。 As shown in Fig. 2, the cured product of the thermosetting resin sheet 11 includes an island structure including a matrix portion (hereinafter also referred to as a sea phase) and a region portion (also referred to as an island phase) dispersed in the matrix portion, and a filler dispersed in the matrix portion. The matrix portion is softer than the region portion.

又，硬化物係藉由例如使熱硬化性樹脂薄片11在150℃加熱1小時硬化而獲得。 Moreover, the cured product is obtained by, for example, heating the thermosetting resin sheet 11 at 150 ° C for 1 hour.

熱硬化性樹脂薄片11難以使構成熱硬化性樹脂薄片11之材料流入被黏著體與電子裝置之間之空隙。其理由雖不清楚，但推測藉由將使用熱硬化性樹脂薄片11所得之密封體加熱，而進行含有區域部及比區域部柔軟之基質部之海島構造之形成，故不會使構成熱硬化性樹脂薄片11之材料過度流動。 It is difficult for the thermosetting resin sheet 11 to flow the material constituting the thermosetting resin sheet 11 into the gap between the adherend and the electronic device. Though the reason is not clear, it is presumed that the sealing body obtained by using the thermosetting resin sheet 11 is heated to form a sea-island structure including a region portion and a matrix portion which is softer than the region portion, so that the thermosetting is not caused. The material of the resin sheet 11 is excessively flowed.

基質部及區域部之柔軟性可藉由例如原子力顯微鏡(AFM)得知。 The softness of the matrix portion and the region portion can be known by, for example, atomic force microscopy (AFM).

圖3中，顏色淡之部分(非黑色部分)為相位延遲較小之部分。相位延遲較小之部分吸附性低，為硬的部分。另一方面，顏色深的部分為相位延遲較大的部分。相位延遲較大的部分吸附性高，為柔軟之部分。 In Fig. 3, the light color portion (non-black portion) is a portion having a small phase delay. The portion with a small phase retardation is low in adsorption and is a hard portion. On the other hand, the portion deep in color is a portion having a large phase delay. The part with a large phase retardation has high adsorptivity and is a soft part.

基質部包含第1樹脂成分作為主成分。區域部包含第2樹脂成分作為主成分。 The matrix portion contains a first resin component as a main component. The region portion contains the second resin component as a main component.

基於難以使構成熱硬化性樹脂薄片11之材料流入被黏著體與電子裝置間之空隙中之理由，基質部較好包含熱可塑性樹脂作為主成分。亦即，第1樹脂成分較好為熱可塑性樹脂。區域部較好包含熱硬化性樹脂作為主成分。亦即，第2樹脂成分較好為熱硬化性樹脂。 The matrix portion preferably contains a thermoplastic resin as a main component for the reason that it is difficult to cause the material constituting the thermosetting resin sheet 11 to flow into the gap between the adherend and the electronic device. That is, the first resin component is preferably a thermoplastic resin. The region portion preferably contains a thermosetting resin as a main component. That is, the second resin component is preferably a thermosetting resin.

藉由對照硬化物之AFM之觀察結果與透過型電子顯微鏡(TEM)之觀察結果，可明瞭基質部包含熱可塑性樹脂作為主成分。可明瞭區域部包含熱硬化性樹脂作為主成分。 From the observation results of the AFM of the cured cured product and the observation results of the transmission electron microscope (TEM), it was confirmed that the matrix portion contains the thermoplastic resin as a main component. It is understood that the region portion contains a thermosetting resin as a main component.

圖4顯示圖3中使用之硬化物之TEM觀察像作為參考。顏色深的部分為低亮度區域，係包含熱可塑性樹脂作為主成分之部分。 Fig. 4 shows a TEM observation image of the cured product used in Fig. 3 as a reference. The dark portion is a low-luminance region and contains a thermoplastic resin as a main component.

關於海島構造之形成，可藉由調整熱可塑性樹脂之官能基種類、熱可塑性樹脂含量等，獲得可形成包含區域部及比區域部柔軟之基質部之海島構造的熱硬化性樹脂薄片11。 In the formation of the island structure, the thermosetting resin sheet 11 which can form the sea-island structure including the region portion and the substrate portion which is softer than the region portion can be obtained by adjusting the type of the functional group of the thermoplastic resin, the content of the thermoplastic resin, and the like.

藉由使熱可塑性樹脂之含量增量，可容易地形成比區域部柔軟之基質部。例如，藉由以使填料以外之總成分100重量%中之熱可塑性樹脂含量為10重量%以上之方式調配熱可塑性樹脂，可獲得可形成包含區域部及比區域部柔軟之基質部之海島構造的熱硬化性樹脂薄片11。 By increasing the content of the thermoplastic resin, it is possible to easily form a matrix portion which is softer than the region portion. For example, by formulating the thermoplastic resin so that the content of the thermoplastic resin in 100% by weight of the total component other than the filler is 10% by weight or more, it is possible to obtain an island structure capable of forming a matrix portion including a region portion and a softer region portion. Thermosetting resin sheet 11.

基於可容易地形成海島構造之理由，熱可塑性樹脂之官能基列舉為羧基(-COOH)、環氧基、羥基、胺基、巰基等。 The functional group of the thermoplastic resin is exemplified by a carboxyl group (-COOH), an epoxy group, a hydroxyl group, an amine group, a fluorenyl group or the like, for the reason that the sea-island structure can be easily formed.

區域部之最大粒徑較好為0.01μm以上，更好為0.03μm以上，又更好為0.05μm以上。為0.01μm以上時，可限制成型時之材料流動。另一方面，區域部之最大粒徑較好為5μm以下，更好為4μm以下，又更好為3μm以下，再更好為1μm以下，最好為0.8μm以下，又最好為0.5μm以下。為5μm以下時，可對於位在空隙附近之構成熱硬化性樹脂薄片11之材料賦予如觸變性般之作用，而可限制構成熱硬化性樹脂薄片11之材料之流動。 The maximum particle diameter of the region portion is preferably 0.01 μm or more, more preferably 0.03 μm or more, and still more preferably 0.05 μm or more. When it is 0.01 μm or more, the flow of the material during molding can be restricted. On the other hand, the maximum particle diameter of the region portion is preferably 5 μm or less, more preferably 4 μm or less, still more preferably 3 μm or less, still more preferably 1 μm or less, more preferably 0.8 μm or less, still more preferably 0.5 μm or less. . When it is 5 μm or less, it is possible to impart a thixotropic action to the material constituting the thermosetting resin sheet 11 located in the vicinity of the void, and the flow of the material constituting the thermosetting resin sheet 11 can be restricted.

區域部之最大粒徑可藉由熱可塑性樹脂之官能基之量控制。例如，藉由調配官能基量較多之熱可塑性樹脂，可使區域部之最大粒徑變小。又，熱硬化性樹脂與熱可塑性樹脂之相溶性對區域部之最大粒徑亦有影響。但，熱可塑性樹脂之官能基之量對區域部之最大粒徑有較大影響。 The maximum particle size of the zone portion can be controlled by the amount of functional groups of the thermoplastic resin. For example, by blending a thermoplastic resin having a large amount of functional groups, the maximum particle diameter of the region portion can be made small. Further, the compatibility of the thermosetting resin and the thermoplastic resin also affects the maximum particle diameter of the region portion. However, the amount of the functional group of the thermoplastic resin has a large influence on the maximum particle diameter of the region portion.

又，區域部之最大粒徑在以透過型電子顯微 鏡(TEM)觀察之觀察像中，為區域部之輪廓上之2點間距離中最大之距離。區域部之最大粒徑可藉觀察100個區域部所得之測定值予以平均而算出。集合或凝聚複數個區域部而存在時，係將輪廓連續者作為一個區域部予以處理。具體而言可藉實施例之方法測定。 Permeable electron microscopy In the observation image observed by the mirror (TEM), it is the largest distance between the two points on the contour of the area portion. The maximum particle size of the area portion can be calculated by averaging the measured values obtained by observing the 100 area parts. When a plurality of regions are aggregated or aggregated, the contour continuation is treated as one region. Specifically, it can be measured by the method of the examples.

硬化物之Tg(玻璃轉移溫度)較好為100℃以上，更好為120℃以上。硬化物之Tg較好為200℃以下，又更好為170℃以下。若為上述範圍內，則在溫度循環試驗、回焊試驗等各種信賴性試驗中可獲得良好的信賴性。 The Tg (glass transition temperature) of the cured product is preferably 100 ° C or higher, more preferably 120 ° C or higher. The Tg of the cured product is preferably 200 ° C or less, and more preferably 170 ° C or less. When it is in the above range, good reliability can be obtained in various reliability tests such as a temperature cycle test and a reflow test.

又，Tg可藉實施例中記載之方法測定。 Further, Tg can be measured by the method described in the examples.

硬化物之Tg可藉交聯密度控制。例如，可藉由使用分子中官能基數較多之熱硬化性樹脂而提高Tg。 The Tg of the hardened material can be controlled by the crosslink density. For example, Tg can be improved by using a thermosetting resin having a large number of functional groups in the molecule.

硬化物之Tg以下之線膨脹係數(CTE1)較好為20ppm/K以下，更好為17ppm/K以下。為20ppm/K以下時，可降低硬化物之翹曲。另一方面，硬化物之CTE1下限並無特別限制。例如，硬化物之CTE1為5ppm/K以上、8ppm/K以上等。 The coefficient of linear expansion (CTE1) below the Tg of the cured product is preferably 20 ppm/K or less, more preferably 17 ppm/K or less. When it is 20 ppm/K or less, the warpage of the hardened material can be reduced. On the other hand, the lower limit of the CTE1 of the cured product is not particularly limited. For example, the CTE1 of the cured product is 5 ppm/K or more and 8 ppm/K or more.

又，線膨脹係數可藉實施例中記載之方法測定。 Further, the coefficient of linear expansion can be measured by the method described in the examples.

硬化物之線膨脹係數可藉無機填充材之含量等控制。例如，可藉由增加無機填充材之含量而減小線膨脹係數。 The linear expansion coefficient of the hardened material can be controlled by the content of the inorganic filler or the like. For example, the coefficient of linear expansion can be reduced by increasing the content of the inorganic filler.

硬化物之25℃之拉伸儲存彈性模數較好為1GPa以上，更好為3GPa以上。若為1GPa以上，則可在形成硬化物後抑制硬化物回到常溫時產生之翹曲。硬化物 之25℃之拉伸儲存彈性模數較好為15GPa以下，更好為10GPa以下。若為15GPa以下，則可使因硬化物回到常溫時產生之變形而發生之硬化樹脂之應力減小，可抑制因對於被黏著體之應力集中造成之剝離或龜裂。 The tensile storage elastic modulus of the cured product at 25 ° C is preferably 1 GPa or more, more preferably 3 GPa or more. When it is 1 GPa or more, warpage which occurs when a hardened material returns to normal temperature can be suppressed after formation of a hardened material. Hardened material The tensile storage elastic modulus at 25 ° C is preferably 15 GPa or less, more preferably 10 GPa or less. When the pressure is 15 GPa or less, the stress of the cured resin which is generated by the deformation of the cured product when it returns to normal temperature can be reduced, and peeling or cracking due to stress concentration on the adherend can be suppressed.

又，拉伸儲存彈性模數可藉實施例中記載之方法測定。 Further, the tensile storage elastic modulus can be measured by the method described in the examples.

硬化物之拉伸儲存彈性模數主要可藉無機填充材之含量控制。例如，可藉由增加無機填充材之含量而提高拉伸儲存彈性模數。 The tensile storage elastic modulus of the cured product can be mainly controlled by the content of the inorganic filler. For example, the tensile storage elastic modulus can be increased by increasing the content of the inorganic filler.

關於熱硬化性樹脂薄片11，在60℃~130℃下之最低熔融黏度較好為2000Pa．s以上，更好為5000Pa．s以上。若為2000Pa．s以上，則難以使構成熱硬化性樹脂薄片11之材料流入中空部。另一方面，熱硬化性樹脂薄片11之在60℃~130℃下之最低熔融黏度較好為20000Pa．s以下，更好15000Pa．s以下。若為20000Pa．s以下，則可容易地使電子裝置埋入於熱硬化性樹脂薄片11內，故可減低孔洞。 Regarding the thermosetting resin sheet 11, the lowest melt viscosity at 60 ° C to 130 ° C is preferably 2000 Pa. Above s, better for 5000Pa. s above. If it is 2000Pa. When it is s or more, it is difficult to cause the material constituting the thermosetting resin sheet 11 to flow into the hollow portion. On the other hand, the lowest melt viscosity of the thermosetting resin sheet 11 at 60 ° C to 130 ° C is preferably 20000 Pa. s below, better 15000Pa. s below. If it is 20000Pa. In the case of s or less, the electronic device can be easily embedded in the thermosetting resin sheet 11, so that the hole can be reduced.

又，最低熔融黏度可藉實施例中記載之方法測定。 Further, the lowest melt viscosity can be measured by the method described in the examples.

熱硬化性樹脂薄片11較好包含熱硬化性樹脂及熱可塑性樹脂。 The thermosetting resin sheet 11 preferably contains a thermosetting resin and a thermoplastic resin.

熱硬化性樹脂薄片11中熱硬化性樹脂與熱可塑性樹脂較好相溶。若相溶，則不會產生熱硬化性樹脂之偏析或熱可塑性樹脂之偏析，故可減低硬化物之翹曲。 The thermosetting resin in the thermosetting resin sheet 11 is preferably compatible with the thermoplastic resin. When it is compatible, segregation of the thermosetting resin or segregation of the thermoplastic resin does not occur, so that the warpage of the cured product can be reduced.

又，所謂熱硬化性樹脂與熱可塑性樹脂相溶意指以透 過型電子顯微鏡(TEM)觀察之觀察像中，未觀察到熱硬化性樹脂與熱可塑性樹脂之相分離構造。 Moreover, the term "thermosetting resin" is compatible with the thermoplastic resin means In the observation image observed by a electron microscope (TEM), the phase separation structure of the thermosetting resin and the thermoplastic resin was not observed.

熱硬化性樹脂並無特別限制，但較好為環氧樹脂、酚樹脂。 The thermosetting resin is not particularly limited, but is preferably an epoxy resin or a phenol resin.

環氧樹脂並無特別限制。可使用例如三苯基甲烷型環氧樹脂、甲酚酚醛清漆型環氧樹脂、聯苯型環氧樹脂、改質雙酚A型環氧樹脂、雙酚A型環氧樹脂、雙酚F型環氧樹脂、改質雙酚F型環氧樹脂、二環戊二烯型環氧樹脂、酚酚醛清漆型環氧樹脂、苯氧樹脂等各種環氧樹脂。該等環氧樹脂可單獨使用亦可併用2種以上。 The epoxy resin is not particularly limited. For example, a triphenylmethane type epoxy resin, a cresol novolak type epoxy resin, a biphenyl type epoxy resin, a modified bisphenol A type epoxy resin, a bisphenol A type epoxy resin, a bisphenol F type can be used. Epoxy resin, modified bisphenol F type epoxy resin, dicyclopentadiene type epoxy resin, phenol novolac type epoxy resin, phenoxy resin and other epoxy resins. These epoxy resins may be used alone or in combination of two or more.

就確保環氧樹脂之反應性之觀點而言，以環氧當量150~250、軟化點或熔點為50~130℃之在常溫為固態者較佳。其中，就信賴性之觀點而言，較好為三苯基甲烷型環氧樹脂、甲酚酚醛清漆型環氧樹脂、聯苯型環氧樹脂。此外，基於可對熱硬化性樹脂薄片11賦予可撓性之理由，以雙酚F型環氧樹脂較佳。 From the viewpoint of ensuring the reactivity of the epoxy resin, it is preferred that the epoxy resin has an epoxy equivalent of 150 to 250, a softening point or a melting point of 50 to 130 ° C at room temperature. Among them, from the viewpoint of reliability, a triphenylmethane type epoxy resin, a cresol novolak type epoxy resin, and a biphenyl type epoxy resin are preferable. Moreover, it is preferable to use a bisphenol F type epoxy resin for the reason that the thermosetting resin sheet 11 can be provided with flexibility.

酚樹脂只要是可與環氧樹脂之間引起硬化反應者即無特別限制。可使用例如酚酚醛清漆樹脂、酚芳烷基樹脂、聯苯芳烷基樹脂、二環戊二烯型酚樹脂、甲酚酚醛清漆樹脂、間苯二酚樹脂等。該等酚樹脂可單獨使用，亦可併用2種以上。 The phenol resin is not particularly limited as long as it can cause a hardening reaction with the epoxy resin. For example, a phenol novolak resin, a phenol aralkyl resin, a biphenyl aralkyl resin, a dicyclopentadiene type phenol resin, a cresol novolak resin, a resorcin resin, or the like can be used. These phenol resins may be used singly or in combination of two or more.

作為酚樹脂，就與環氧樹脂之反應性之觀點而言，較好使用羥基當量為70~250，軟化點為50~110℃者。其中就硬化反應性高之觀點而言，可較好地使用酚酚 醛清漆樹脂。且，就信賴性之觀點而言，亦可較好地使用如酚酚醛清漆樹脂或聯苯芳烷基樹脂之低吸濕性者。 As the phenol resin, from the viewpoint of reactivity with an epoxy resin, those having a hydroxyl group equivalent of 70 to 250 and a softening point of 50 to 110 ° C are preferably used. Among them, in terms of high hardening reactivity, phenol can be preferably used. Aldehyde varnish resin. Further, from the viewpoint of reliability, a low hygroscopic property such as a phenol novolak resin or a biphenyl aralkyl resin can be preferably used.

環氧樹脂與酚樹脂之調配比例，就硬化反應性之觀點而言，較好以使酚樹脂中之羥基之合計相對於環氧樹脂中之環氧基1當量成為0.7~1.5當量之方式加以調配，更好為0.9~1.2當量。 The ratio of the epoxy resin to the phenol resin is preferably such that the total amount of the hydroxyl groups in the phenol resin is 0.7 to 1.5 equivalents per equivalent of the epoxy group in the epoxy resin from the viewpoint of the curing reactivity. The blending is preferably 0.9 to 1.2 equivalents.

填料以外之總成分100重量%中之熱硬化性樹脂之含量較好為70重量%以上，更好為75重量%以上，又更好為80重量%以上。若為70重量%以上，則可使硬化物之CTE1值變小。另一方面，熱硬化性樹脂之含量較好為95重量%以下，更好為92重量%以下，又更好為90重量%以下，最好為88重量%以下。 The content of the thermosetting resin in 100% by weight of the total component other than the filler is preferably 70% by weight or more, more preferably 75% by weight or more, still more preferably 80% by weight or more. When it is 70% by weight or more, the CTE1 value of the cured product can be made small. On the other hand, the content of the thermosetting resin is preferably 95% by weight or less, more preferably 92% by weight or less, still more preferably 90% by weight or less, and most preferably 88% by weight or less.

熱硬化性樹脂薄片11較好包含硬化促進劑。 The thermosetting resin sheet 11 preferably contains a curing accelerator.

硬化促進劑若為能使環氧樹脂與酚樹脂之硬化進行者即無特別限制，列舉為例如2-甲基咪唑(商品名：2MZ)、2-十一烷基咪唑(商品名：C11-Z)、2-十七烷基咪唑(商品名：C17Z)、1,2-二甲基咪唑(商品名：1.2DMZ)、2-乙基-4-甲基咪唑(商品名：2E4MZ)、2-苯基咪唑(商品名：2PZ)、2-苯基-4-甲基咪唑(商品名：2P4MZ)、1-苄基-2-甲基咪唑(商品名：1B2MZ)、1-苄基-2-苯基咪唑(商品名：1B2PZ)、1-氰基乙基-2-甲基咪唑(商品名：2MZ-CN)、1-氰基乙基-2-十一烷基咪唑(商品名：C11Z-CN)、1-氰基乙基-2-苯基咪唑鎓偏苯三酸鹽(商品名：2PZCNS-PW)、2,4-二胺基-6-[2'-甲基咪唑基-(1’)]-乙 基-s-三嗪(商品名：2MZ-A)、2,4-二胺基-6-[2'-十一烷基咪唑基-(1')]-乙基-s-三嗪(商品名：C11Z-A)、2,4-二胺基-6-[2'-乙基-4’-甲基咪唑基-(1’)]-乙基-s-三嗪(商品名：2E4MZ-A)、2,4-二胺基-6-[2'-甲基咪唑基-(1’)]-乙基-s-三嗪異氰尿酸加成物(商品名：2MA-OK)、2-苯基-4,5-二羥基甲基咪唑(商品名：2PHZ-PW)、2-苯基-4-甲基-5-羥基甲基咪唑(商品名：2P4MHZ-PW)等咪唑系硬化促進劑(均為四國化成工業(股)製)。 The hardening accelerator is not particularly limited as long as it can cure the epoxy resin and the phenol resin, and is exemplified by, for example, 2-methylimidazole (trade name: 2MZ) and 2-undecylimidazole (trade name: C11- Z), 2-heptadecylimidazole (trade name: C17Z), 1,2-dimethylimidazole (trade name: 1.2DMZ), 2-ethyl-4-methylimidazole (trade name: 2E4MZ), 2-phenylimidazole (trade name: 2PZ), 2-phenyl-4-methylimidazole (trade name: 2P4MZ), 1-benzyl-2-methylimidazole (trade name: 1B2MZ), 1-benzyl group -2-phenylimidazole (trade name: 1B2PZ), 1-cyanoethyl-2-methylimidazole (trade name: 2MZ-CN), 1-cyanoethyl-2-undecylimidazole (commercial product Name: C11Z-CN), 1-cyanoethyl-2-phenylimidazolium trimellitate (trade name: 2PZCNS-PW), 2,4-diamino-6-[2'-methyl Imidazolyl-(1')]-B Base-s-triazine (trade name: 2MZ-A), 2,4-diamino-6-[2'-undecylimidazolyl-(1')]-ethyl-s-triazine ( Trade Name: C11Z-A), 2,4-Diamino-6-[2'-ethyl-4'-methylimidazolyl-(1')]-ethyl-s-triazine (trade name: 2E4MZ-A), 2,4-Diamino-6-[2'-methylimidazolyl-(1')]-ethyl-s-triazine isocyanuric acid adduct (trade name: 2MA-OK) ), 2-phenyl-4,5-dihydroxymethylimidazole (trade name: 2PHZ-PW), 2-phenyl-4-methyl-5-hydroxymethylimidazole (trade name: 2P4MHZ-PW), etc. Imidazole hardening accelerator (all manufactured by Shikoku Chemical Industry Co., Ltd.).

其中，基於硬化促進能力良好且獲得高Tg之硬化樹脂之理由以咪唑系硬化促進劑較佳，更好為2-苯基-4,5-二羥基甲基咪唑、2,4-二胺基-6-[2’-乙基-4’-甲基咪唑-(1’)]-乙基-s-三嗪，又更好為2-苯基-4,5-二羥基甲基咪唑。 Among them, an imidazole-based hardening accelerator is preferred for the purpose of obtaining a hardening resin having a high Tg-promoting ability and obtaining a high Tg, and more preferably 2-phenyl-4,5-dihydroxymethylimidazole or 2,4-diamino group. -6-[2'-ethyl-4'-methylimidazolium-(1')]-ethyl-s-triazine, more preferably 2-phenyl-4,5-dihydroxymethylimidazole.

硬化促進劑之含量相對於環氧樹脂及酚樹脂之合計100重量份較好為0.2重量份以上，更好為0.5重量份以上，又更好為0.8重量份以上。硬化促進劑之含量相對於環氧樹脂及酚樹脂之合計100重量份，較好為5重量份以下，更好為2重量份以下。 The content of the curing accelerator is preferably 0.2 parts by weight or more, more preferably 0.5 parts by weight or more, and still more preferably 0.8 parts by weight or more based on 100 parts by weight of the total of the epoxy resin and the phenol resin. The content of the curing accelerator is preferably 5 parts by weight or less, more preferably 2 parts by weight or less based on 100 parts by weight of the total of the epoxy resin and the phenol resin.

熱硬化性樹脂薄片11較好包含熱可塑性樹脂。熱可塑性樹脂較好為可作為彈性體功能者。 The thermosetting resin sheet 11 preferably contains a thermoplastic resin. The thermoplastic resin is preferably one which can function as an elastomer.

熱可塑性樹脂列舉為例如丙烯酸系彈性體、胺基甲酸酯系彈性體、聚矽氧系彈性體、聚酯系彈性體等。其中，就容易獲得可撓性、與環氧樹脂之分散性良好之觀點，較好為丙烯酸系彈性體。 The thermoplastic resin is exemplified by, for example, an acrylic elastomer, an urethane elastomer, a polyoxynene elastomer, a polyester elastomer, or the like. Among them, from the viewpoint of easy flexibility and good dispersibility with an epoxy resin, an acrylic elastomer is preferred.

丙烯酸系彈性體並無特別限制，列舉為以具有碳數30以下，尤其是碳數4~18之直鏈或分支之烷基之丙烯酸或甲基丙烯酸之酯類之1種或2種以上作為成分之聚合物(丙烯酸共聚物)等。烷基列舉為例如甲基、乙基、丙基、異丙基、正丁基、第三丁基、異丁基、戊基、異戊基、己基、庚基、環己基、2-乙基己基、辛基、異辛基、壬基、異壬基、癸基、異癸基、十一烷基、月桂基、十三烷基、十四烷基、硬脂基、十八烷基、或十二烷基等。 The acrylic elastomer is not particularly limited, and one or two or more kinds of esters of acrylic acid or methacrylic acid having a carbon number of 30 or less, particularly a linear or branched alkyl group having 4 to 18 carbon atoms are used. A polymer of a component (acrylic acid copolymer) or the like. The alkyl group is exemplified by, for example, methyl, ethyl, propyl, isopropyl, n-butyl, t-butyl, isobutyl, pentyl, isopentyl, hexyl, heptyl, cyclohexyl, 2-ethyl Hexyl, octyl, isooctyl, decyl, isodecyl, decyl, isodecyl, undecyl, lauryl, tridecyl, tetradecyl, stearyl, octadecyl, Or dodecyl and the like.

且，形成聚合物之其他單體並無特別限制，列舉為例如丙烯酸、甲基丙烯酸、丙烯酸羧基乙酯、丙烯酸羧基戊酯、衣康酸、馬來酸、富馬酸或巴豆酸等之含羧基之單體、如馬來酸酐或衣康酸酐等之酸酐單體、如(甲基)丙烯酸2-羥基乙酯、(甲基)丙烯酸2-羥基丙酯、(甲基)丙烯酸4-羥基丁酯、(甲基)丙烯酸6-羥基己酯、(甲基)丙烯酸8-羥基辛酯、(甲基)丙烯酸10-羥基癸酯、(甲基)丙烯酸12-羥基月桂酯或(4-羥基甲基環己基)-甲基丙烯酸酯等之含羥基之單體、如苯乙烯磺酸、烯丙基磺酸、2-(甲基)丙烯醯胺-2-甲基丙烷磺酸、(甲基)丙烯醯胺丙烷磺酸、(甲基)丙烯酸磺丙酯或(甲基)丙烯醯氧基萘磺酸等之含磺酸基之單體、或如2-羥基乙基丙烯醯基磷酸酯等含磷酸之單體。其中，基於可與環氧樹脂反應，提高熱硬化性樹脂薄片11之黏度之觀點，較好包含含羧基之單體、含縮水甘油基(環氧基)之單體、含羥基之單體中之至少一者。 Further, the other monomer forming the polymer is not particularly limited, and is exemplified by, for example, acrylic acid, methacrylic acid, carboxyethyl acrylate, carboxy amyl acrylate, itaconic acid, maleic acid, fumaric acid or crotonic acid. a monomer of a carboxyl group, an anhydride monomer such as maleic anhydride or itaconic anhydride, such as 2-hydroxyethyl (meth)acrylate, 2-hydroxypropyl (meth)acrylate, 4-hydroxyl (meth)acrylate Butyl ester, 6-hydroxyhexyl (meth)acrylate, 8-hydroxyoctyl (meth)acrylate, 10-hydroxydecyl (meth)acrylate, 12-hydroxylauryl (meth)acrylate or (4- a hydroxyl group-containing monomer such as hydroxymethylcyclohexyl)-methacrylate, such as styrenesulfonic acid, allylsulfonic acid, 2-(methyl)acrylamido-2-methylpropanesulfonic acid, a sulfonic acid group-containing monomer such as methyl acrylamide sulfonium sulfonic acid, sulfopropyl (meth) acrylate or (meth) propylene phthaloxy naphthalene sulfonic acid, or such as 2-hydroxyethyl acrylonitrile A phosphate-containing monomer such as a phosphate ester. Among them, from the viewpoint of being able to react with an epoxy resin and increasing the viscosity of the thermosetting resin sheet 11, it is preferable to contain a monomer having a carboxyl group, a monomer having a glycidyl group (epoxy group), and a monomer having a hydroxyl group. At least one of them.

熱可塑性樹脂較好具有官能基。基於可容易形成海島構造之理由，官能基較好為羧基、環氧基、羥基、胺基、巰基，更好為羧基。 The thermoplastic resin preferably has a functional group. The functional group is preferably a carboxyl group, an epoxy group, a hydroxyl group, an amine group or a mercapto group, and more preferably a carboxyl group, for the reason that the sea-island structure can be easily formed.

熱可塑性樹脂之酸價較好為1mgKOH/g以上，更好為3mgKOH/g以上，又更好為10mgKOH/g以上。若為1mgKOH/g以上，則可使區域部減小，而限制構成熱硬化性樹脂11之材料之流動。另一方面，熱可塑性樹脂之酸價較好為100mgKOH/g以下，更好為60mgKOH/g以下，又更好為50mgKOH/g以下，最好為40mgKOH/g以下。若為100mgKOH/g以下，則可比較良好地保持因酸價之影響造成之熱硬化性樹脂薄片11之保存安定性。 The acid value of the thermoplastic resin is preferably 1 mgKOH/g or more, more preferably 3 mgKOH/g or more, and still more preferably 10 mgKOH/g or more. When it is 1 mgKOH/g or more, the area portion can be reduced, and the flow of the material constituting the thermosetting resin 11 can be restricted. On the other hand, the acid value of the thermoplastic resin is preferably 100 mgKOH/g or less, more preferably 60 mgKOH/g or less, still more preferably 50 mgKOH/g or less, and most preferably 40 mgKOH/g or less. When it is 100 mgKOH/g or less, the storage stability of the thermosetting resin sheet 11 due to the influence of the acid value can be relatively favorably maintained.

又，酸價可藉JIS K 0070-1992中規定之中和滴定法測定。 Further, the acid value can be measured by the titration method as specified in JIS K 0070-1992.

熱可塑性樹脂之重量平均分子量較好為50萬以上，更好為80萬以上。若為50萬以上，則由於熱可塑性樹脂之黏度不會過低，故調配時之操作變容易。另一方面，熱可塑性樹脂之重量平均分子量較好為200萬以下，更好為150萬以下。若為200萬以下，則熱可塑性樹脂之黏度不會太高，故調配時之操作變容易。 The weight average molecular weight of the thermoplastic resin is preferably 500,000 or more, more preferably 800,000 or more. If it is 500,000 or more, since the viscosity of the thermoplastic resin is not too low, the operation at the time of preparation becomes easy. On the other hand, the weight average molecular weight of the thermoplastic resin is preferably 2,000,000 or less, more preferably 1.5,000,000 or less. If it is 2,000,000 or less, the viscosity of the thermoplastic resin is not too high, so the operation at the time of preparation becomes easy.

又，重量平均分子量係以GPC(凝膠滲透層析儀)測定，以聚苯乙烯換算算出之值。 Further, the weight average molecular weight is measured by GPC (gel permeation chromatography) and is calculated in terms of polystyrene.

熱可塑性樹脂之Tg較好為-70℃以上，更好為-50℃以上。若為-70℃以上，則聚合物設計容易，且成 型溫度之彈性率不會過低，故成形時之埋入性易於控制。另一方面，熱可塑性樹脂之Tg較好為20℃以下，更好為0℃以下。若為20℃以下，則成型溫度下之彈性率不會過度變高，成型時之埋入性易於控制。 The thermoplastic resin has a Tg of preferably -70 ° C or higher, more preferably -50 ° C or higher. If it is above -70 ° C, the polymer design is easy and The modulus of elasticity of the type temperature is not too low, so the embedding property at the time of molding is easy to control. On the other hand, the thermoplastic resin has a Tg of preferably 20 ° C or lower, more preferably 0 ° C or lower. When it is 20 ° C or less, the modulus of elasticity at the molding temperature does not become excessively high, and the embedding property at the time of molding can be easily controlled.

本說明書中，熱可塑性樹脂之玻璃轉移溫度係指以Fox式求出之理論值。 In the present specification, the glass transition temperature of the thermoplastic resin means a theoretical value obtained by the Fox equation.

且，求出玻璃轉移溫度之其他方法亦有根據利用示差掃描熱量計(DSC)測定之最大熱吸收波峰時之溫度，求出熱可塑性樹脂之玻璃轉移溫度之方法。具體而言，使用示差掃描熱量計(TA Instruments公司製之「Q-2000」)在比預測之試料之玻璃轉移溫度(預測溫度)高約50℃之溫度加熱測定試料10分鐘後，冷卻至比預測溫度低50℃之溫度進行前處理，隨後在氮氣環境下，以升溫速度5℃/分鐘升溫而測定吸熱開始溫度，以此作為玻璃轉移溫度。 Further, another method for determining the glass transition temperature is to determine the glass transition temperature of the thermoplastic resin based on the temperature at the maximum heat absorption peak measured by a differential scanning calorimeter (DSC). Specifically, the sample was heated and measured for 10 minutes at a temperature higher than the glass transition temperature (predicted temperature) of the predicted sample by a differential scanning calorimeter ("Q-2000" manufactured by TA Instruments Co., Ltd.), and then cooled to a ratio. The pretreatment was carried out at a temperature at which the temperature was lowered by 50 ° C, and then the endothermic onset temperature was measured by raising the temperature at a temperature increase rate of 5 ° C / min in a nitrogen atmosphere as the glass transition temperature.

填料以外之總成分100重量%中之熱可塑性樹脂之含量較好為5重量%以上，更好為10重量%以上，又更好為11重量%以上，再更好為12重量%以上，最好為13重量%以上。若為5重量%以上，則可形成海島構造。且，若為10重量%以上，則可容易形成海島構造。另一方面，熱可塑性樹脂之含量較好為30重量%以下，更好為20重量%以下。若為30重量%以下，則熱硬化性樹脂薄片11之儲存彈性模數不會變得過高，可兼具埋入性與流動限制。 The content of the thermoplastic resin in 100% by weight of the total component other than the filler is preferably 5% by weight or more, more preferably 10% by weight or more, still more preferably 11% by weight or more, still more preferably 12% by weight or more, most preferably It is preferably 13% by weight or more. If it is 5% by weight or more, an island structure can be formed. Moreover, when it is 10 weight% or more, an island structure can be formed easily. On the other hand, the content of the thermoplastic resin is preferably 30% by weight or less, more preferably 20% by weight or less. When it is 30% by weight or less, the storage elastic modulus of the thermosetting resin sheet 11 does not become excessively high, and both the embedding property and the flow restriction can be achieved.

熱硬化性樹脂薄片11較好包含填料。藉由調 配填料，可使熱膨脹係數α減小。填料較好為例如無機填充材。 The thermosetting resin sheet 11 preferably contains a filler. By tune With the filler, the coefficient of thermal expansion α can be reduced. The filler is preferably, for example, an inorganic filler.

無機填充材列舉為例如石英玻璃、滑石、二氧化矽(熔融二氧化矽或結晶性二氧化矽等)、氧化鋁(alumina)、氮化硼、氮化鋁、碳化矽等。其中基於可良好遞減低熱膨脹係數之理由，以二氧化矽較佳。基於流動性優異之理由，二氧化矽較好為熔融二氧化矽，更好為球狀二氧化矽。此外，基於提高熱傳導率之理由，較好為熱傳導性填料，更好為氧化鋁、氮化硼、氮化鋁。又，無機填充材較好為電絕緣性者。 The inorganic filler is exemplified by quartz glass, talc, cerium oxide (melting cerium oxide or crystalline cerium oxide, etc.), alumina, boron nitride, aluminum nitride, tantalum carbide or the like. Among them, cerium oxide is preferred because of the reason that the coefficient of thermal expansion is well degraded. The reason for the excellent fluidity is that the cerium oxide is preferably molten cerium oxide, more preferably spherical cerium oxide. Further, it is preferably a thermally conductive filler for the reason of improving the thermal conductivity, and more preferably alumina, boron nitride or aluminum nitride. Further, the inorganic filler is preferably electrically insulating.

填料之平均粒徑較好為0.5μm以上，更好為1μm以上。若為0.5μm以上，則容易獲得熱硬化性樹脂薄片11之可撓性、柔軟性。填料之平均粒徑較好為30μm以下，更好為10μm以下。若為30μm以下，則填料容易高填充。 The average particle diameter of the filler is preferably 0.5 μm or more, more preferably 1 μm or more. When it is 0.5 μm or more, the flexibility and flexibility of the thermosetting resin sheet 11 are easily obtained. The average particle diameter of the filler is preferably 30 μm or less, more preferably 10 μm or less. When it is 30 μm or less, the filler is easily filled.

又，平均粒徑可使用任意自母集團抽取之試料，藉由使用雷射繞射散射式粒度分佈測定裝置測定而導出。 Further, the average particle diameter can be derived by using a sample extracted from the parent group and measuring by using a laser diffraction scattering type particle size distribution measuring apparatus.

填料之粒度分佈中，較好至少存在波峰A及波峰B。具體而言，較好於0.01μm~10μm之粒徑範圍存在波峰A，於1μm~100μm之粒徑範圍存在波峰B。據此，在形成波峰B之填料之間可填充形成波峰A之填料，使填料可高填充。 In the particle size distribution of the filler, it is preferred that at least the peak A and the peak B exist. Specifically, it is preferable that the peak A exists in the particle diameter range of 0.01 μm to 10 μm, and the peak B exists in the particle diameter range of 1 μm to 100 μm. Accordingly, the filler forming the peak A can be filled between the fillers forming the peak B, so that the filler can be highly filled.

波峰A更好存在於0.1μm以上之粒徑範圍。波峰A更好存在於1μm以下之粒徑範圍。 The peak A is more preferably present in a particle size range of 0.1 μm or more. The peak A is more preferably present in a particle size range of 1 μm or less.

波峰B更好存在於3μm以上之粒徑範圍。波峰B更好存在於10μm以下之粒徑範圍。 The peak B is preferably present in a particle size range of 3 μm or more. The peak B is preferably present in a particle size range of 10 μm or less.

填料之粒度分佈中，亦可存在波峰A及波峰B以外之波峰。 In the particle size distribution of the filler, peaks other than the peak A and the peak B may also exist.

又，填料之粒度分佈可藉以下方法測定。 Further, the particle size distribution of the filler can be measured by the following method.

填料之粒度分佈之測定方法 Method for determining particle size distribution of filler

將熱硬化性樹脂薄片11導入坩堝中，經強熱使熱硬化性樹脂薄片11灰化。將所得灰分分散於純水中並經超音波處理10分鐘，使用雷射繞射式粒度分佈測定裝置(Beckman Coulter公司製，「LS 13 320」；濕式法)求出粒度分佈(體積基準)。 The thermosetting resin sheet 11 is introduced into a crucible, and the thermosetting resin sheet 11 is ashed by intense heat. The obtained ash was dispersed in pure water and ultrasonicated for 10 minutes, and a particle size distribution (volume basis) was determined using a laser diffraction type particle size distribution measuring apparatus ("LS 13 320", manufactured by Beckman Coulter Co., Ltd.; wet method). .

無機填充材亦可經矽烷偶合劑處理(前處理)。藉此，可提高與樹脂之潤濕性，且可提高無機填充材之分散性。 The inorganic filler can also be treated with a decane coupling agent (pretreatment). Thereby, the wettability with the resin can be improved, and the dispersibility of the inorganic filler can be improved.

矽烷偶合劑為分子中具有水解性基及有機官能基之化合物。 The decane coupling agent is a compound having a hydrolyzable group and an organic functional group in the molecule.

水解性基列舉為例如甲氧基、乙氧基等碳數1~6之烷氧基、乙醯氧基、2-甲氧基乙氧基等。其中，基於容易去除因水解產生之醇等之揮發性成分之理由，較好為甲氧基。 The hydrolyzable group is, for example, an alkoxy group having 1 to 6 carbon atoms such as a methoxy group or an ethoxy group, an ethoxy group, a 2-methoxyethoxy group or the like. Among them, a methoxy group is preferred because it is easy to remove a volatile component such as an alcohol produced by hydrolysis.

有機官能基列舉為乙烯基、環氧基、苯乙烯基、甲基丙烯醯基、丙烯醯基、胺基、脲基、巰基、硫醚基、異氰酸酯基等。其中，基於與環氧樹脂、酚樹脂反應容易之理由，較好為環氧基。 The organic functional group is exemplified by a vinyl group, an epoxy group, a styryl group, a methacryloyl group, an acryloyl group, an amine group, a urea group, a fluorenyl group, a thioether group, an isocyanate group or the like. Among them, an epoxy group is preferred because it is easily reacted with an epoxy resin or a phenol resin.

矽烷偶合劑列舉為例如乙烯基三甲氧基矽烷、乙烯基三乙氧基矽烷等含有乙烯基之矽烷偶合劑；2-(3,4-環氧基環己基)乙基三甲氧基矽烷、3-縮水甘油氧基丙基甲基二甲氧基矽烷、3-縮水甘油氧基丙基三甲氧基矽烷、3-縮水甘油氧基丙基甲基二乙氧基矽烷、3-縮水甘油氧基丙基三乙氧基矽烷等含環氧基之矽烷偶合劑；對-苯乙烯基三甲氧基矽烷等含苯乙烯基之矽烷偶合劑；3-甲基丙烯醯氧基丙基甲基二甲氧基矽烷、3-甲基丙烯醯氧基丙基三甲氧基矽烷、3-甲基丙烯醯氧基丙基甲基二乙氧基矽烷、3-甲基丙烯醯氧基丙基三乙氧基矽烷等含甲基丙烯醯基之矽烷偶合劑；3-丙烯醯氧基丙基三甲氧基矽烷等含丙烯醯基之矽烷偶合劑；N-(2-胺基乙基)-3-胺基丙基甲基二甲氧基矽烷、N-2-(胺基乙基)-3-胺基丙基三甲氧基矽烷、3-胺基丙基三甲氧基矽烷、3-胺基丙基三乙氧基矽烷、3-三乙氧基矽烷基-N-(1,3-二甲基-亞丁基)丙胺、N-苯基-3-胺基丙基三甲氧基矽烷、N-(乙烯基苄基)-2-胺基乙基-3-胺基丙基三甲氧基矽烷等含胺基之矽烷偶合劑；3-脲基丙基三乙氧基矽烷等含脲基之矽烷偶合劑；3-巰基丙基甲基二甲氧基矽烷、3-巰基丙基三甲氧基矽烷等含巰基之矽烷偶合劑；雙(三乙氧基矽烷基丙基)四硫醚等含硫醚基之矽烷偶合劑；3-異氰酸酯基丙基三乙氧基矽烷等含異氰酸酯基之矽烷偶合劑等。 The decane coupling agent is exemplified by a vinyl group-containing decane coupling agent such as vinyl trimethoxy decane or vinyl triethoxy decane; 2-(3,4-epoxycyclohexyl)ethyltrimethoxy decane, 3 - glycidoxypropylmethyldimethoxydecane, 3-glycidoxypropyltrimethoxydecane, 3-glycidoxypropylmethyldiethoxydecane, 3-glycidoxy An epoxy group-containing decane coupling agent such as propyltriethoxysilane; a styrene-based decane coupling agent such as p-styryltrimethoxydecane; 3-methylpropenyloxypropylmethyl dimethyl Oxydecane, 3-methylpropenyloxypropyltrimethoxydecane, 3-methylpropenyloxypropylmethyldiethoxydecane, 3-methylpropenyloxypropyltriethoxylate a decane coupling agent containing a methacrylonitrile group such as a decane or a decane coupling agent containing an acrylonitrile group such as 3-propenyloxypropyltrimethoxydecane; N-(2-aminoethyl)-3-amine Propylmethyldimethoxydecane, N-2-(aminoethyl)-3-aminopropyltrimethoxydecane, 3-aminopropyltrimethoxydecane, 3-aminopropyl Triethoxy decane , 3-triethoxydecyl-N-(1,3-dimethyl-butylene)propylamine, N-phenyl-3-aminopropyltrimethoxydecane, N-(vinylbenzyl) An amine group-containing decane coupling agent such as 2-aminoethyl-3-aminopropyltrimethoxydecane; a urea group-containing decane coupling agent such as 3-ureidopropyltriethoxysilane; 3-mercapto group a decane-containing decane coupling agent such as propylmethyldimethoxydecane or 3-mercaptopropyltrimethoxydecane; a thioether-containing decane coupling agent such as bis(triethoxydecylpropyl)tetrasulfide An isocyanate group-containing decane coupling agent such as 3-isocyanatepropyltriethoxydecane.

以矽烷偶合劑處理無機填充材之方法並無特別限制，列舉為將無機填充材與矽烷偶合劑於溶劑中混合 之濕式法、在氣相中處理無機填充材與矽烷偶合劑之乾式法等。 The method for treating the inorganic filler by the decane coupling agent is not particularly limited, and is exemplified by mixing the inorganic filler with the decane coupling agent in a solvent. The wet method, the dry method of treating the inorganic filler and the decane coupling agent in the gas phase, and the like.

矽烷偶合劑之處理量並無特別限制，但相對於未處理之無機填充材100重量份較好處理0.1重量份~1重量份之矽烷偶合劑。 The treatment amount of the decane coupling agent is not particularly limited, but is preferably 0.1 part by weight to 1 part by weight of the decane coupling agent per 100 parts by weight of the untreated inorganic filler.

熱硬化性樹脂薄片11中之填充劑含量較好為60體積%以上，更好為70體積%以上。若為60體積%以上，則可使硬化物之CTE1變小。另一方面，填料之含量較好為90體積%以下，更好為80體積%以下。若為90體積%以下，則薄片成型容易。 The filler content in the thermosetting resin sheet 11 is preferably 60% by volume or more, more preferably 70% by volume or more. When it is 60% by volume or more, the CTE1 of the cured product can be made small. On the other hand, the content of the filler is preferably 90% by volume or less, more preferably 80% by volume or less. When it is 90 volume% or less, sheet formation is easy.

填料之含量亦可以「重量%」作為單位說明。針對代表性之二氧化矽含量，以「重量%」為單位加以說明。 The content of the filler can also be expressed in terms of "% by weight". The representative cerium oxide content is described in terms of "% by weight".

二氧化矽通常比重為2.2g/cm3，故二氧化矽之含量(重量%)之較佳範圍例如如下。 The cerium oxide usually has a specific gravity of 2.2 g/cm 3 , so the preferred range of the content (% by weight) of cerium oxide is as follows, for example.

亦即，熱硬化性樹脂薄片11中之二氧化矽含量較好為75重量%以上，更好為80重量%以上。另一方面，熱硬化性樹脂薄片11中之二氧化矽含量較好為95重量%以下，更好為90重量%以下。 That is, the content of cerium oxide in the thermosetting resin sheet 11 is preferably 75% by weight or more, more preferably 80% by weight or more. On the other hand, the content of cerium oxide in the thermosetting resin sheet 11 is preferably 95% by weight or less, more preferably 90% by weight or less.

氧化鋁通常比重為3.9g/cm3，故氧化鋁之含量(重量%)之較佳範圍例如如下。 The alumina generally has a specific gravity of 3.9 g/cm 3 , so a preferred range of the content (% by weight) of alumina is as follows, for example.

亦即，熱硬化性樹脂薄片11中之氧化鋁含量較好為85重量%以上，更好為90重量%以上。另一方面，熱硬化性樹脂薄片11中之氧化鋁含量較好為97重量%以下， 更好為95重量%以下。 That is, the alumina content in the thermosetting resin sheet 11 is preferably 85% by weight or more, more preferably 90% by weight or more. On the other hand, the alumina content in the thermosetting resin sheet 11 is preferably 97% by weight or less. More preferably, it is 95% by weight or less.

熱硬化性樹脂薄片11除前述成分以外，亦可適當含有密封樹脂之製造中一般使用之調配劑，例如顏料等。 The thermosetting resin sheet 11 may contain, in addition to the above components, a preparation agent generally used in the production of a sealing resin, such as a pigment.

顏料並無特別限制，列舉為碳黑等。 The pigment is not particularly limited and is exemplified by carbon black or the like.

熱硬化性樹脂薄片11之製造方法並無特別限制，藉由將用於形成熱硬化性樹脂薄片11之樹脂等溶解、分散於適當之溶劑中調整漆料，且以成為特定厚度之方式將該漆料塗佈於隔膜12上形成塗佈膜後，在特定之條件下使塗佈膜乾燥，可獲得熱硬化性樹脂薄片11。塗佈方法並無特別限制，列舉為例如輥塗佈、網版塗佈、凹版塗佈等。此外，乾燥條件係在例如乾燥溫度70~160℃、乾燥時間1~30分鐘之範圍內進行。且，將漆料塗佈於與隔膜12不同之隔膜上形成塗佈膜，使塗佈膜乾燥而形成熱硬化性樹脂薄片11後，將熱硬化性樹脂薄片11貼合於隔膜12上之方法亦較佳。熱硬化性樹脂薄片11尤其在包含熱可塑性樹脂、環氧樹脂、酚樹脂時，藉由使該等全部溶解於溶劑中，經塗佈、乾燥。藉此，可提高熱硬化性樹脂薄片11之黏度，可抑制樹脂成分進入到中空部。作為溶劑可列舉為甲基乙基酮、乙酸乙酯、甲苯等。 The method for producing the thermosetting resin sheet 11 is not particularly limited, and the resin or the like for forming the thermosetting resin sheet 11 is dissolved and dispersed in a suitable solvent to adjust the paint, and the resin is adjusted to have a specific thickness. After the paint is applied onto the separator 12 to form a coating film, the coating film is dried under specific conditions to obtain a thermosetting resin sheet 11. The coating method is not particularly limited, and examples thereof include roll coating, screen coating, gravure coating, and the like. Further, the drying conditions are carried out, for example, at a drying temperature of 70 to 160 ° C and a drying time of 1 to 30 minutes. Further, a method of applying a paint to a separator different from the separator 12 to form a coating film, drying the coating film to form the thermosetting resin sheet 11, and then bonding the thermosetting resin sheet 11 to the separator 12 Also preferred. When the thermosetting resin sheet 11 contains a thermoplastic resin, an epoxy resin, or a phenol resin, it is coated and dried by dissolving all of them in a solvent. Thereby, the viscosity of the thermosetting resin sheet 11 can be increased, and the resin component can be prevented from entering the hollow portion. The solvent may, for example, be methyl ethyl ketone, ethyl acetate or toluene.

熱硬化性樹脂薄片11較好以混練擠出製造。據此，可容易地形成薄片狀，可獲得孔洞少、厚度均勻之熱硬化性樹脂薄片11。以混練擠出予以製造之方法較好為例如將混練前述各成分(例如，熱硬化性樹脂、硬化促 進劑、熱可塑性樹脂及填料等)所得之混練物塑性加工成薄片狀之方法。據此，可使填料高填充，可設計熱膨脹係數較低。 The thermosetting resin sheet 11 is preferably produced by kneading extrusion. According to this, the sheet shape can be easily formed, and the thermosetting resin sheet 11 having a small number of pores and a uniform thickness can be obtained. The method of producing by kneading extrusion is preferably, for example, kneading the above-mentioned respective components (for example, thermosetting resin, hardening promotion) A method of plastically processing a kneaded material obtained by a flux, a thermoplastic resin, a filler, or the like into a flake. According to this, the filler can be made highly filled, and the coefficient of thermal expansion can be designed to be low.

具體而言，以混練輥、加壓式捏合機、擠出機等之習知混練機將熱硬化性樹脂、硬化促進劑、熱可塑性樹脂及填料等熔融混練，而調製混練物，將所得混練物塑性加工成薄片狀。至於混練條件，溫度之上限較好為140℃以下，更好為130℃以下。溫度之下限較好為上述各成分之軟化點以上，例如為30℃以上，較好為50℃以上。混練時間較好為1~30分鐘。且，混練較好在減壓條件下(減壓環境下)進行，減壓條件下之壓力為例如1×10-4~0.1kg/cm2。 Specifically, a thermosetting resin, a curing accelerator, a thermoplastic resin, a filler, and the like are melt-kneaded by a conventional kneading machine such as a kneading roll, a pressure kneader, or an extruder to prepare a kneaded product, and the resulting kneaded product is kneaded. The material is plastically processed into flakes. As for the kneading conditions, the upper limit of the temperature is preferably 140 ° C or lower, more preferably 130 ° C or lower. The lower limit of the temperature is preferably at least the softening point of each of the above components, and is, for example, 30 ° C or higher, preferably 50 ° C or higher. The mixing time is preferably 1 to 30 minutes. Further, the kneading is preferably carried out under reduced pressure (under reduced pressure), and the pressure under reduced pressure is, for example, 1 × 10 -4 to 0.1 kg/cm 2 .

熔融混練後之混練物較好不進行冷卻而在高溫狀態下直接塑性加工。塑性加工之方法並無特別限制，列舉為平板壓製法、T模嘴擠出法、螺旋擠出法、輥壓延法、輥混練法、吹塑擠出法、共擠出法、軋光成形法等。塑性加工溫度較好為上述各成分之軟化點以上，考慮環氧樹脂之熱硬化性及成形性時，為例如40~150℃，較好為50~140℃，更好為70~120℃。 The kneaded material after the melt kneading is preferably directly subjected to plastic working at a high temperature without cooling. The method of plastic working is not particularly limited, and is exemplified by a flat press method, a T die extrusion method, a spiral extrusion method, a roll calendering method, a roll kneading method, a blow molding method, a coextrusion method, and a calender forming method. Wait. The plastic working temperature is preferably at least the softening point of each of the above components, and is, for example, 40 to 150 ° C, preferably 50 to 140 ° C, more preferably 70 to 120 ° C in consideration of thermosetting properties and moldability of the epoxy resin.

熱硬化性樹脂薄片11之厚度並無特別限制，較好為100μm以上，更好為150μm以上。此外，熱硬化性樹脂薄片11之厚度較好為2000μm以下，更好為1000μm以下。若為上述範圍內，則可良好地密封電子裝置。 The thickness of the thermosetting resin sheet 11 is not particularly limited, but is preferably 100 μm or more, and more preferably 150 μm or more. Further, the thickness of the thermosetting resin sheet 11 is preferably 2000 μm or less, more preferably 1000 μm or less. If it is in the above range, the electronic device can be satisfactorily sealed.

熱硬化性樹脂薄片11係為了製造中空封裝而使用。中空封裝列舉為例如感知器封裝、MEMS(微機電系統(Micro Electro Mechanical Systems))封裝、SAW(表面聲波(Surface Acoustic Wave))濾波器。 The thermosetting resin sheet 11 is used for manufacturing a hollow package. Hollow packages are listed, for example, as perceptron packages, MEMS (Micro Electro Mechanical Systems) packages, SAW (Surface Acoustic Wave) filters.

中空封裝具備例如基板、安裝於基板上之電子裝置及被覆電子裝置之硬化樹脂。電子裝置與基板之間設置中空部。至於基板列舉為例如印刷配線基板、LTCC(低溫共燒陶瓷(Low Temperature Co-fired Ceramics))基板(以下亦稱為低溫同時燒成陶瓷基板)、陶瓷基板、矽基板、金屬基板等。電子裝置列舉為感知器、MEMS、SAW晶片等。其中，可較好地使用壓力感知器、振動感知器、SAW晶片，最好可使用SAW晶片。硬化樹脂係藉由使熱硬化性樹脂薄片11硬化形成。 The hollow package includes, for example, a substrate, an electronic device mounted on the substrate, and a cured resin covering the electronic device. A hollow portion is disposed between the electronic device and the substrate. The substrate is exemplified by, for example, a printed wiring board, a LTCC (Low Temperature Co-fired Ceramics) substrate (hereinafter also referred to as a low-temperature simultaneous firing ceramic substrate), a ceramic substrate, a tantalum substrate, a metal substrate, or the like. Electronic devices are listed as perceptrons, MEMS, SAW wafers, and the like. Among them, a pressure sensor, a vibration sensor, and a SAW wafer can be preferably used, and a SAW wafer can be preferably used. The cured resin is formed by hardening the thermosetting resin sheet 11.

使用熱硬化性樹脂薄片11製造中空封裝之方法代表為例如將電子裝置埋入到熱硬化性樹脂薄片11中之方法。 The method of manufacturing a hollow package using the thermosetting resin sheet 11 is represented by, for example, a method of embedding an electronic device in the thermosetting resin sheet 11.

熱硬化性樹脂薄片11可作為用於保護電子裝置及其所隨附之元件免受外部環境影響之密封樹脂之功能。 The thermosetting resin sheet 11 functions as a sealing resin for protecting the electronic device and the components attached thereto from the external environment.

(中空封裝之製造方法) (Manufacturing method of hollow package)

如圖5所示，層合體31係配置在下側加熱板41與上述加熱板42之間。層合體31具備裝置安裝體2、配置於裝置安裝體2上之熱硬化性樹脂薄片11及配置於熱硬化 性樹脂薄片11上之隔膜12。 As shown in FIG. 5, the laminated body 31 is arrange|positioned between the lower side heating board 41 and the said heating board 42. The laminate 31 includes a device mounting body 2, a thermosetting resin sheet 11 disposed on the device mounting body 2, and a thermosetting resin sheet. The separator 12 on the resin sheet 11.

裝置安裝體2具備基板22及安裝於基板22上之SAW晶片23。藉由以習知方法晶片切割形成有特定梳形電極之壓電結晶而單片化，可獲得SAW晶片23。可使用覆晶黏晶機、固晶機等習知裝置，將SAW晶片23配置於基板22上。SAW晶片23與基板22係透過凸塊等突起電極24電性連接。此外，SAW晶片23與基板22之間係以不妨礙SAW濾波器表面之表面彈性波傳播之方式維持中空部25。SAW晶片23與基板22間之距離(以下亦稱為中空部25之寬度)可適當設定，一般為10μm~100μm左右。亦即，裝置安裝體2具備基板22、配置於基板22上之突起電極24及配置於突起電極24上之SAW晶片23。 The device mounting body 2 includes a substrate 22 and a SAW wafer 23 mounted on the substrate 22. The SAW wafer 23 can be obtained by wafer-cutting a piezoelectric crystal formed with a specific comb-shaped electrode by a conventional method. The SAW wafer 23 can be placed on the substrate 22 by a conventional device such as a flip chip bonding machine or a die bonding machine. The SAW wafer 23 and the substrate 22 are electrically connected to each other through the bump electrodes 24 such as bumps. Further, the hollow portion 25 is maintained between the SAW wafer 23 and the substrate 22 so as not to interfere with the surface elastic wave propagation of the surface of the SAW filter. The distance between the SAW wafer 23 and the substrate 22 (hereinafter also referred to as the width of the hollow portion 25) can be appropriately set, and is generally about 10 μm to 100 μm. That is, the device mounting body 2 includes the substrate 22, the bump electrodes 24 disposed on the substrate 22, and the SAW wafer 23 disposed on the bump electrodes 24.

如圖6所示，藉由使用下側加熱板41及上側加熱板42之平行平板方式熱加壓層合體31，形成密封體32。 As shown in FIG. 6, the sealing body 32 is formed by thermally pressing the laminated body 31 by using the parallel flat plate of the lower side heating plate 41 and the upper side heating plate 42.

熱加壓之溫度較好為40℃以上，更好為50℃以上，又更好為60℃以上。若為40℃以上，則可良好地密封。熱加壓溫度較好為150℃以下，更好為90℃以下，又更好為80℃以下。若為150℃以下，則藉熱加壓成型前，硬化反應不會過度進行，故可良好地密封。 The temperature of the hot pressurization is preferably 40 ° C or more, more preferably 50 ° C or more, and still more preferably 60 ° C or more. If it is 40 ° C or more, it can seal well. The heat pressurization temperature is preferably 150 ° C or lower, more preferably 90 ° C or lower, and still more preferably 80 ° C or lower. When it is 150 ° C or less, the hardening reaction does not proceed excessively before the hot press molding, so that it can be satisfactorily sealed.

熱加壓層合體31之壓力較好為0.1MPa以上，更好為0.5MPa以上，又更好為1MPa以上。此外，熱加壓層合體1之壓力較好為10MPa以下，更好為8MPa以下。若為10MPa以下，則不會對SAW晶片23造成大 的損傷。 The pressure of the heat-pressure laminated body 31 is preferably 0.1 MPa or more, more preferably 0.5 MPa or more, and still more preferably 1 MPa or more. Further, the pressure of the heat-pressure laminated body 1 is preferably 10 MPa or less, more preferably 8 MPa or less. If it is 10 MPa or less, it will not cause a large SAW wafer 23 Damage.

熱加壓時間較好為0.3分鐘以上，更好為0.5分鐘以上。且，熱加壓時間較好為10分鐘以下，更好為5分鐘以下。 The hot pressurization time is preferably 0.3 minutes or more, more preferably 0.5 minutes or more. Further, the hot pressurization time is preferably 10 minutes or shorter, more preferably 5 minutes or shorter.

熱加壓較好在減壓環境下進行。藉由在減壓環境下熱加壓，可減低孔洞，可良好地埋入凹凸。減壓條件為壓力例如0.01kPa~5kPa，較好為0.1Pa~100Pa。 The hot pressurization is preferably carried out under a reduced pressure environment. By heat-pressurizing in a reduced pressure environment, the holes can be reduced, and the unevenness can be buried well. The pressure reduction condition is, for example, 0.01 kPa to 5 kPa, preferably 0.1 Pa to 100 Pa.

藉由熱加壓層合體31所得之密封體32具備基板22、安裝於基板22上之SAW晶片23及被覆SAW晶片23之熱硬化性樹脂薄片11。於密封體32上配置隔膜12。 The sealing body 32 obtained by thermally pressing the laminate 31 includes a substrate 22, a SAW wafer 23 mounted on the substrate 22, and a thermosetting resin sheet 11 covering the SAW wafer 23. The diaphragm 12 is disposed on the sealing body 32.

如圖7所示，自密封體32剝離隔膜12。 As shown in FIG. 7, the separator 12 is peeled off from the sealing body 32.

藉加熱密封體32使熱硬化性樹脂薄片11硬化，形成硬化體33。 The thermosetting resin sheet 11 is cured by the heat sealing body 32 to form a hardened body 33.

加熱溫度較好為100℃以上，更好為120℃以上。另一方面，加熱溫度之上限較好為200℃以下，更好為180℃以下。加熱時間較好為10分鐘以上，更好為30分鐘以上。另一方面，加熱時間之上限較好為180分鐘以下，更好為120分鐘以下。較好在加壓環境下加熱密封體32，壓力較好為0.1Mpa以上，更好為0.5MPa以上。另一方面，上限較好為10MPa以下，更好為5MPa以下。在大氣壓下加熱密封體32亦較佳。 The heating temperature is preferably 100 ° C or higher, more preferably 120 ° C or higher. On the other hand, the upper limit of the heating temperature is preferably 200 ° C or lower, more preferably 180 ° C or lower. The heating time is preferably 10 minutes or longer, more preferably 30 minutes or longer. On the other hand, the upper limit of the heating time is preferably 180 minutes or shorter, more preferably 120 minutes or shorter. The sealing body 32 is preferably heated in a pressurized environment, and the pressure is preferably 0.1 MPa or more, more preferably 0.5 MPa or more. On the other hand, the upper limit is preferably 10 MPa or less, more preferably 5 MPa or less. It is also preferred to heat the sealing body 32 at atmospheric pressure.

如圖8所示，硬化體33具備基板22、安裝於基板22上之SAW晶片23及被覆SAW晶片23之硬化樹 脂26。 As shown in FIG. 8, the hardened body 33 includes a substrate 22, a SAW wafer 23 mounted on the substrate 22, and a hardened tree covering the SAW wafer 23. Grease 26.

如圖9所示，硬化體33經單片化(晶片切割)獲得中空封裝34。據此，可獲得SAW晶片23單位之中空封裝34。中空封裝34具備基板22、安裝於基板22上之SAW晶片23及被覆SAW晶片23之硬化樹脂26。 As shown in FIG. 9, the hardened body 33 is singulated (wafer cut) to obtain a hollow package 34. According to this, a hollow package 34 of 23 units of the SAW wafer can be obtained. The hollow package 34 includes a substrate 22, a SAW wafer 23 mounted on the substrate 22, and a cured resin 26 covering the SAW wafer 23.

亦可於中空封裝34上形成凸塊，使之安裝於另外基板(未圖示)上。中空封裝34對基板之安裝可使用覆晶黏晶機或固晶機等習知裝置。 A bump may also be formed on the hollow package 34 to be mounted on another substrate (not shown). A conventional device such as a flip chip bonder or a die bonder can be used for mounting the hollow package 34 to the substrate.

(變形例1) (Modification 1)

實施形態1中，熱硬化性樹脂薄片11為單層構造，但變形例1中，熱硬化性樹脂薄片11為層合複數層熱硬化性樹脂層而成之多層構造。針對變形例1之熱硬化性樹脂薄片11，藉由使與電子裝置接觸之熱硬化性樹脂層硬化獲得之硬化層只要含有包含區域部及比區域部柔軟之基質部之海島構造與分散於基質部中之填料，則其他熱硬化性樹脂層並無特別限制。 In the first embodiment, the thermosetting resin sheet 11 has a single-layer structure. However, in the first modification, the thermosetting resin sheet 11 has a multilayer structure in which a plurality of layers of a thermosetting resin layer are laminated. In the thermosetting resin sheet 11 of the first modification, the hardened layer obtained by curing the thermosetting resin layer in contact with the electronic device includes an island structure including a region portion and a substrate portion which is softer than the region portion, and is dispersed in the matrix. In the filler in the portion, the other thermosetting resin layer is not particularly limited.

(變形例2) (Modification 2)

實施例1中，以平行平板方式加壓層合體31，但變形例2中係使用層合機加壓層合體31。 In the first embodiment, the laminate 31 was pressed in a parallel plate manner, but in the second modification, the laminate press laminate 31 was used.

(變形例3) (Modification 3)

實施例1中係熱加壓層合體31，但變形例3係熱加 壓具備裝置安裝體2及配置於裝置安裝體2上之熱硬化性樹脂薄片11之層合體(未圖示)。 In the first embodiment, the hot press laminate 31 is used, but the modification 3 is hot addition. A laminate (not shown) including the device mounting body 2 and the thermosetting resin sheet 11 disposed on the device mounting body 2 is pressed.

[實施例] [Examples]

以下，例示本發明之較佳實施例詳細說明。但，該實施例中記載之材料或調配量等，只要無特別限定記載，則本發明之範圍並非意指僅限於彼等者。 Hereinafter, a detailed description of the preferred embodiments of the present invention will be exemplified. However, the materials, the blending amounts, and the like described in the examples are not intended to limit the scope of the invention unless otherwise specified.

針對實施例1、實施例7~9及比較例1中使用之成分加以說明。 The components used in Example 1, Examples 7 to 9, and Comparative Example 1 will be described.

環氧樹脂：新日鐵化學公司製之YSLV-80XY(雙酚F型環氧樹脂，環氧當量：200g/eq.，軟化點：80℃) Epoxy resin: YSLV-80XY manufactured by Nippon Steel Chemical Co., Ltd. (bisphenol F epoxy resin, epoxy equivalent: 200 g/eq., softening point: 80 ° C)

酚樹脂：群榮化學公司製之LVR8210DL(酚醛清漆型酚樹脂，羥基當量：104g/eq.，軟化點：60℃) Phenol resin: LVR8210DL manufactured by Qun Rong Chemical Co., Ltd. (novolak type phenol resin, hydroxyl equivalent: 104 g/eq., softening point: 60 ° C)

熱可塑性樹脂1：根上工業公司製之ME-2000M(含羧基之丙烯酸酯共聚物，重量平均分子量：約60萬，Tg：-35℃，酸價：20mgKOH/g) Thermoplastic Resin 1: ME-2000M (Carboxy-containing acrylate copolymer, weight average molecular weight: about 600,000, Tg: -35 ° C, acid value: 20 mg KOH / g) manufactured by Kasei Kogyo Co., Ltd.

熱可塑性樹脂2：根上工業公司製之HME-2006(含羧基之丙烯酸酯共聚物，重量平均分子量：約84萬，Tg：-47℃，酸價：32mgKOH/g) Thermoplastic Resin 2: HME-2006 manufactured by Kasei Kogyo Co., Ltd. (carboxyl-containing acrylate copolymer, weight average molecular weight: about 840,000, Tg: -47 ° C, acid value: 32 mg KOH / g)

熱可塑性樹脂3：NAGASE CHEMTEX公司製之SG-280(含羧基之丙烯酸酯共聚物，重量平均分子量：約90萬，Tg：-29℃，酸價：30mgKOH/g) Thermoplastic Resin 3: SG-280 manufactured by NAGASE CHEMTEX Co., Ltd. (carboxyl-containing acrylate copolymer, weight average molecular weight: about 900,000, Tg: -29 ° C, acid value: 30 mg KOH / g)

熱可塑性樹脂4：根上工業公司製之NSC-010(含羧基之丙烯酸酯共聚物，重量平均分子量：約93萬，Tg：-13 ℃，酸價：5mgKOH/g) Thermoplastic Resin 4: NSC-010 (carboxyl-containing acrylate copolymer) manufactured by Kokusai Kogyo Co., Ltd., weight average molecular weight: about 930,000, Tg: -13 °C, acid value: 5mgKOH/g)

碳黑：三菱化學公司製之#20 Carbon black: #20 from Mitsubishi Chemical Corporation

填料1：電氣化學工業公司製之FB-5SDC(球狀二氧化矽，平均粒徑5μm) Filler 1: FB-5SDC (spherical cerium oxide, average particle size 5 μm) manufactured by Electrochemical Industry Co., Ltd.

填料2：ADAMTECH公司製之SO-25R(球狀二氧化矽，平均粒徑0.5μm) Filler 2: SO-25R (spherical cerium oxide, average particle size 0.5 μm) manufactured by ADAMTECH

硬化促進劑：四國化成工業公司製之2PHZ-PW(2-苯基-4,5-二羥基甲基咪唑) Hardening accelerator: 2PHZ-PW (2-phenyl-4,5-dihydroxymethylimidazole) manufactured by Shikoku Chemical Industry Co., Ltd.

[熱硬化性樹脂薄片之製作] [Production of thermosetting resin sheet]

依據表1所記載之調配比，將各成分溶解、分散於作為溶劑之甲基乙基酮中，獲得濃度90重量%之漆料。將該漆料塗佈於經聚矽氧脫模處理之厚度為38μm之由聚對苯二甲酸乙二酯薄膜所成之脫模處理薄膜上後，在110℃乾燥5分鐘。據此，獲得厚度65μm之薄片。層合4層該薄片獲得厚度260μm之熱硬化性樹脂薄片。 According to the mixing ratio described in Table 1, each component was dissolved and dispersed in methyl ethyl ketone as a solvent to obtain a paint having a concentration of 90% by weight. This paint was applied onto a release-treated film made of a polyethylene terephthalate film having a thickness of 38 μm which was subjected to polyfluorene stripping treatment, and then dried at 110 ° C for 5 minutes. According to this, a sheet having a thickness of 65 μm was obtained. Four sheets of this sheet were laminated to obtain a thermosetting resin sheet having a thickness of 260 μm.

[硬化物之製作] [Production of hardened material]

使用加熱烘箱，在150℃使熱硬化性樹脂薄片加熱1小時硬化而獲得硬化物。 The thermosetting resin sheet was cured by heating at 150 ° C for 1 hour using a heating oven to obtain a cured product.

[試驗片之製作] [Production of test piece]

除了未調配填料1、填料2及碳黑以外，餘以與熱硬化性樹脂薄片相同之方法，製作試驗用樹脂薄片。使用加 熱烘箱，在150℃使試驗用樹脂薄片加熱1小時硬化而獲得試驗片。 A test resin sheet was produced in the same manner as the thermosetting resin sheet except that the filler 1, the filler 2, and the carbon black were not prepared. Use plus In a hot oven, the test resin sheet was heated at 150 ° C for 1 hour to obtain a test piece.

又，製作試驗片之理由係為了觀察海島構造。觀察硬化物亦可確認海島構造，但藉由觀察試驗片可容易地確認海島構造。 Moreover, the reason for producing the test piece was to observe the island structure. The island structure can also be confirmed by observing the cured product, but the island structure can be easily confirmed by observing the test piece.

[評價] [Evaluation]

針對熱硬化性樹脂薄片、硬化物、試驗片進行以下評價。結果示於表1。 The following evaluation was performed on the thermosetting resin sheet, the cured product, and the test piece. The results are shown in Table 1.

(熱硬化性樹脂薄片之相分離) (phase separation of thermosetting resin sheets)

以TEM觀察熱硬化性樹脂薄片之切斷面，而確認有無相分離。 The cut surface of the thermosetting resin sheet was observed by TEM to confirm the presence or absence of phase separation.

(熱硬化性樹脂薄片之最低熔融黏度) (the lowest melt viscosity of the thermosetting resin sheet)

針對熱硬化性樹脂薄片，使用動態黏彈性測定裝置((TA Instruments公司製，ARES)，以間距1mm、平行板直徑25mm、測定頻率0.1Hz、應變(變形)0.1%、測定溫度範圍60℃~130℃、升溫速度10℃/min之測定條件測定所得之黏度之最低值作為最低黏度。 For the thermosetting resin sheet, a dynamic viscoelasticity measuring device (ARES) manufactured by TA Instruments Co., Ltd., having a pitch of 1 mm, a parallel plate diameter of 25 mm, a measurement frequency of 0.1 Hz, a strain (deformation) of 0.1%, and a measurement temperature range of 60 ° C were used. The lowest value of the viscosity obtained by measuring the measurement conditions of 130 ° C and a temperature increase rate of 10 ° C / min was taken as the lowest viscosity.

(硬化物之拉伸儲存彈性模數及Tg) (Stretch storage elastic modulus and Tg of hardened material)

以切割刀自硬化物切出長40mm、寬10mm、厚200μm之短條狀之試驗片。針對試驗片使用固體黏彈性測 定裝置(RSAIII，Rheometric Scientific(股)製)，測定-50℃~300℃下之儲存彈性模數及損失彈性模數。測定條件為頻率1Hz，升溫速度10℃/min。進而，藉由算出tanδ(G”(損失彈性模數/G’(儲存彈性模數))之值而獲得Tg。 A test piece having a length of 40 mm, a width of 10 mm, and a thickness of 200 μm was cut out from the cured product by a cutter. Solid viscoelasticity test for test pieces A fixed device (RSAIII, manufactured by Rheometric Scientific Co., Ltd.) was used to measure the storage elastic modulus and the loss elastic modulus at -50 ° C to 300 ° C. The measurement conditions were a frequency of 1 Hz and a temperature increase rate of 10 ° C/min. Further, Tg is obtained by calculating the value of tan δ (G" (loss elastic modulus / G' (storage elastic modulus)).

(硬化物之CTE1) (CTE1 of hardened material)

自硬化物切出長15mm、寬5mm、厚200μm之測定試料。將測定試料固定在熱機械分析裝置(Rigaku公司製之TMA8310)之薄膜拉伸測定用治具後，在-50℃~300℃之溫度區域，於拉伸荷重2g、升溫速度5℃/分鐘之條件下，由50℃~70℃之膨脹率算出CTE1。 A test sample having a length of 15 mm, a width of 5 mm, and a thickness of 200 μm was cut out from the cured product. After fixing the measurement sample to a jig for tensile measurement of a film in a thermomechanical analyzer (TMA8310, manufactured by Rigaku Co., Ltd.), the tensile load was 2 g and the temperature was raised at 5 ° C/min in a temperature range of -50 ° C to 300 ° C. Under the conditions, CTE1 was calculated from the expansion ratio of 50 ° C to 70 ° C.

(試驗片之相分離) (phase separation of test pieces)

以TEM觀察試驗片之切斷面，而確認有無相分離(參照圖10及圖11)。 The cut surface of the test piece was observed by TEM to confirm the presence or absence of phase separation (see Figs. 10 and 11).

(試驗片之AFM觀察) (AFM observation of the test piece)

以AFM觀察試驗片之切斷面，針對海相及島相確認熱硬化性樹脂及熱可塑性樹脂中何者為主成分。 The cut surface of the test piece was observed by AFM, and it was confirmed which of the thermosetting resin and the thermoplastic resin was the main component for the sea phase and the island phase.

(島相之最大粒徑) (the maximum particle size of the island phase)

以TEM觀察硬化物之切斷面。由觀察像求出島相之最大粒徑。 The cut surface of the cured product was observed by TEM. The maximum particle diameter of the island phase was obtained from the observation image.

(中空部之樹脂浸入量) (Resin impregnation amount in the hollow portion)

以下述黏晶條件將形成有鋁梳型電極之以下規格之SAW晶片安裝於陶瓷基板上，製作具備陶瓷基板及安裝於陶瓷基板之SAW晶片之SAW晶片安裝基板。SAW晶片與陶瓷基板間之間隙寬為20μm。 The SAW wafer of the following specifications in which the aluminum comb-type electrode was formed was mounted on a ceramic substrate under the following conditions, and a SAW wafer mounting substrate including a ceramic substrate and a SAW wafer mounted on the ceramic substrate was produced. The gap between the SAW wafer and the ceramic substrate is 20 μm wide.

〈SAW晶片〉 <SAW Wafer>

晶片尺寸：1.2mm見方(厚度150μm) Wafer size: 1.2mm square (thickness 150μm)

凸塊材質：Au(高度20μm) Bump material: Au (height 20μm)

凸塊數：6凸塊 Number of bumps: 6 bumps

晶片數：100個(10個×10個) Number of wafers: 100 (10 × 10)

〈黏晶條件〉 <Crystalline conditions>

裝置：Panasonic電工(股)製 Device: Panasonic Electrician (share) system

黏晶條件：200℃、3N、1秒、超音波輸出2W Bonding conditions: 200 ° C, 3 N, 1 second, ultrasonic output 2W

藉由將熱硬化性樹脂薄片配置於SAW晶片安裝基板上，獲得層合體。藉以下所示之加熱加壓條件，以平行平板方式真空加壓層合體，獲得密封體。 A laminate is obtained by disposing a thermosetting resin sheet on a SAW wafer mounting substrate. The laminate was vacuum-pressed in a parallel plate by the heating and pressurizing conditions shown below to obtain a sealed body.

〈真空加壓條件〉 <Vacuum pressurization conditions>

溫度：60℃ Temperature: 60 ° C

加壓力：4MPa Pressure: 4MPa

真空度：1.6kPa Vacuum degree: 1.6kPa

加壓時間：1分鐘 Pressurization time: 1 minute

釋放至大氣壓後，在熱風乾燥機中，以150℃、1小時之條件加熱密封體，獲得硬化物。劈開所得硬化物之基板、密封樹脂界面，以KEYENCE公司製之商品名「數位顯微鏡」(200倍)，測定樹脂朝SAW晶片與陶瓷基板間之中空部之進入量。樹脂進入量係測定自SAW晶片之端部進入到中空部之樹脂最大到達距離，以此作為樹脂進入量。樹脂進入量為20μm以下時評價為「○」，超過20μm時評價為「×」。 After releasing to atmospheric pressure, the sealed body was heated in a hot air dryer at 150 ° C for 1 hour to obtain a cured product. The substrate and the sealing resin interface of the obtained cured product were separated, and the amount of penetration of the resin into the hollow portion between the SAW wafer and the ceramic substrate was measured under the trade name "Digital Microscope" (200 times) manufactured by KEYENCE. The resin entry amount was measured as the resin entry amount by measuring the maximum reach distance of the resin entering the hollow portion from the end portion of the SAW wafer. When the resin entering amount was 20 μm or less, the evaluation was "○", and when it was more than 20 μm, it was evaluated as "×".

針對實施例2中使用之成分加以說明。 The components used in Example 2 will be described.

環氧樹脂：新日鐵化學(股)製之YSLV-80XY(雙酚F型環氧樹脂，環氧當量200g/eq.，軟化點80℃) Epoxy resin: YSLV-80XY (bisphenol F type epoxy resin, epoxy equivalent 200g/eq., softening point 80 °C) made by Nippon Steel Chemical Co., Ltd.

酚樹脂：群榮化學製之LVR8210DL(酚醛清漆型酚樹脂，羥基當量104g/eq.，軟化點60℃) Phenol resin: LVR8210DL manufactured by Qunrong Chemicals (phenolic varnish type phenol resin, hydroxyl equivalent 104g/eq., softening point 60°C)

熱可塑性樹脂：含羧基之丙烯酸酯共聚物，重量平均分子量：約60萬，玻璃轉移溫度(Tg)：-35℃ Thermoplastic resin: carboxyl group-containing acrylate copolymer, weight average molecular weight: about 600,000, glass transition temperature (Tg): -35 ° C

填料1：電氣化學工業公司製之FB-9454FC(平均粒徑19μm) Filler 1: FB-9454FC (average particle size 19 μm) manufactured by Electrochemical Industry Co., Ltd.

碳黑：三菱化學公司製之#20 Carbon black: #20 from Mitsubishi Chemical Corporation

硬化促進劑：四國化成工業公司製之2PHZ-PW(2-苯基-4,5-二羥基甲基咪唑) Hardening accelerator: 2PHZ-PW (2-phenyl-4,5-dihydroxymethylimidazole) manufactured by Shikoku Chemical Industry Co., Ltd.

[熱硬化性樹脂薄片之製作] [Production of thermosetting resin sheet]

依據表2所記載之調配比，將各成分溶解、分散於作為溶劑之甲基乙基酮中，獲得濃度90重量%之漆料。將該漆料塗佈於經聚矽氧脫模處理之厚度為38μm之由聚對苯二甲酸乙二酯薄膜所成之脫模處理薄膜上後，在110℃乾燥5分鐘。藉此，獲得厚度65μm之薄片。層合4層該薄片獲得厚度260μm之熱硬化性樹脂薄片。 According to the mixing ratio described in Table 2, each component was dissolved and dispersed in methyl ethyl ketone as a solvent to obtain a paint having a concentration of 90% by weight. This paint was applied onto a release-treated film made of a polyethylene terephthalate film having a thickness of 38 μm which was subjected to polyfluorene stripping treatment, and then dried at 110 ° C for 5 minutes. Thereby, a sheet having a thickness of 65 μm was obtained. Four sheets of this sheet were laminated to obtain a thermosetting resin sheet having a thickness of 260 μm.

[硬化物之製作] [Production of hardened material]

使用加熱烘箱，在150℃使熱硬化性樹脂薄片加熱1小時硬化而獲得硬化物。 The thermosetting resin sheet was cured by heating at 150 ° C for 1 hour using a heating oven to obtain a cured product.

[評價] [Evaluation]

針對熱硬化性樹脂薄片、硬化物進行各種評價。結果示於表2。 Various evaluations were performed on the thermosetting resin sheet and the cured product. The results are shown in Table 2.

針對實施例3~4中使用之成分加以說明。 The components used in Examples 3 to 4 will be described.

環氧樹脂：新日鐵化學(股)製之YSLV-80XY(雙酚F型環氧樹脂，環氧當量200g/eq.，軟化點80℃) Epoxy resin: YSLV-80XY (bisphenol F type epoxy resin, epoxy equivalent 200g/eq., softening point 80 °C) made by Nippon Steel Chemical Co., Ltd.

酚樹脂：群榮化學公司製之LVR8210DL(酚醛清漆型酚樹脂，羥基當量104g/eq.，軟化點60℃) Phenol resin: LVR8210DL manufactured by Qun Rong Chemical Co., Ltd. (novolac type phenol resin, hydroxyl equivalent 104 g/eq., softening point 60 ° C)

熱可塑性樹脂：含羧基之丙烯酸酯共聚物，重量平均分子量：約60萬，玻璃轉移溫度(Tg)：-35℃ Thermoplastic resin: carboxyl group-containing acrylate copolymer, weight average molecular weight: about 600,000, glass transition temperature (Tg): -35 ° C

填料1：電氣化學工業公司製之FB-7SDC(平均粒徑6μm) Filler 1: FB-7SDC (average particle size 6 μm) manufactured by Electrochemical Industry Co., Ltd.

填料2：ADAMTECH公司製之SO-25R(平均粒徑0.5μm) Filler 2: SO-25R (average particle size 0.5 μm) manufactured by ADAMTECH

碳黑：三菱化學公司製之#20 Carbon black: #20 from Mitsubishi Chemical Corporation

硬化促進劑：四國化成工業公司製之2PHZ-PW(2-苯基-4,5-二羥基甲基咪唑) Hardening accelerator: 2PHZ-PW (2-phenyl-4,5-dihydroxymethylimidazole) manufactured by Shikoku Chemical Industry Co., Ltd.

[熱硬化性樹脂薄片之製作] [Production of thermosetting resin sheet]

依據表3所記載之調配比，將各成分溶解、分散於作為溶劑之甲基乙基酮中，獲得濃度90重量%之漆料。將該漆料塗佈於經聚矽氧脫模處理之厚度為38μm之由聚對苯二甲酸乙二酯薄膜所成之脫模處理薄膜上後，在110℃乾燥5分鐘。藉此，獲得厚度65μm之薄片。層合4層該薄片獲得厚度260μm之熱硬化性樹脂薄片。 According to the blending ratio described in Table 3, each component was dissolved and dispersed in methyl ethyl ketone as a solvent to obtain a paint having a concentration of 90% by weight. This paint was applied onto a release-treated film made of a polyethylene terephthalate film having a thickness of 38 μm which was subjected to polyfluorene stripping treatment, and then dried at 110 ° C for 5 minutes. Thereby, a sheet having a thickness of 65 μm was obtained. Four sheets of this sheet were laminated to obtain a thermosetting resin sheet having a thickness of 260 μm.

[硬化物之製作] [Production of hardened material]

使用加熱烘箱，在150℃使熱硬化性樹脂薄片加熱1小時硬化而獲得硬化物。 The thermosetting resin sheet was cured by heating at 150 ° C for 1 hour using a heating oven to obtain a cured product.

[評價] [Evaluation]

針對熱硬化性樹脂薄片、硬化物進行各種評價。結果 示於表3。 Various evaluations were performed on the thermosetting resin sheet and the cured product. result Shown in Table 3.

針對實施例5~6中使用之成分加以說明。 The components used in Examples 5 to 6 will be described.

環氧樹脂：新日鐵化學(股)製之YSLV-80XY(雙酚F型環氧樹脂，環氧當量200g/eq.，軟化點80℃) Epoxy resin: YSLV-80XY (bisphenol F type epoxy resin, epoxy equivalent 200g/eq., softening point 80 °C) made by Nippon Steel Chemical Co., Ltd.

酚樹脂：群榮化學製之LVR8210DL(酚醛清漆型酚樹脂，羥基當量104g/eq.，軟化點60℃) Phenol resin: LVR8210DL manufactured by Qunrong Chemicals (phenolic varnish type phenol resin, hydroxyl equivalent 104g/eq., softening point 60°C)

熱可塑性樹脂：含羧基之丙烯酸酯共聚物，重量平均分子量：約60萬，玻璃轉移溫度(Tg)：-35℃ Thermoplastic resin: carboxyl group-containing acrylate copolymer, weight average molecular weight: about 600,000, glass transition temperature (Tg): -35 ° C

填料1：球狀熔融二氧化矽(平均粒徑50μm) Filler 1: Spherical molten cerium oxide (average particle size 50 μm)

碳黑：三菱化學公司製之#20 Carbon black: #20 from Mitsubishi Chemical Corporation

硬化促進劑：四國化成工業公司製之2PHZ-PW(2-苯基-4,5-二羥基甲基咪唑) Hardening accelerator: 2PHZ-PW (2-phenyl-4,5-dihydroxymethylimidazole) manufactured by Shikoku Chemical Industry Co., Ltd.

[熱硬化性樹脂薄片之製作] [Production of thermosetting resin sheet]

依據表4所記載之調配比，將各成分溶解、分散於作為溶劑之甲基乙基酮中，獲得濃度90重量%之漆料。將該漆料塗佈於經聚矽氧脫模處理之厚度為38μm之由聚對苯二甲酸乙二酯薄膜所成之脫模處理薄膜上後，在110℃乾燥5分鐘。藉此，獲得厚度65μm之薄片。層合4層該薄片獲得厚度260μm之熱硬化性樹脂薄片。 According to the mixing ratio described in Table 4, each component was dissolved and dispersed in methyl ethyl ketone as a solvent to obtain a paint having a concentration of 90% by weight. This paint was applied onto a release-treated film made of a polyethylene terephthalate film having a thickness of 38 μm which was subjected to polyfluorene stripping treatment, and then dried at 110 ° C for 5 minutes. Thereby, a sheet having a thickness of 65 μm was obtained. Four sheets of this sheet were laminated to obtain a thermosetting resin sheet having a thickness of 260 μm.

[硬化物之製作] [Production of hardened material]

使用加熱烘箱，在150℃使熱硬化性樹脂薄片加熱1小時硬化而獲得硬化物。 The thermosetting resin sheet was cured by heating at 150 ° C for 1 hour using a heating oven to obtain a cured product.

[評價] [Evaluation]

針對熱硬化性樹脂薄片、硬化物進行各種評價。結果示於表4。 Various evaluations were performed on the thermosetting resin sheet and the cured product. The results are shown in Table 4.

11‧‧‧熱硬化性樹脂薄片 11‧‧‧ thermosetting resin sheet

12‧‧‧隔膜 12‧‧‧Separator

Claims (6)

一種密封用熱硬化性樹脂薄片，其係用以製造中空封裝所使用之密封用熱硬化性樹脂薄片，其特徵係前述密封用熱硬化性樹脂薄片之硬化物具備包含第1樹脂成分作為主成分之基質部及包含第2樹脂成分作為主成分之區域部之海島構造，前述基質部比前述區域部更柔軟。 A thermosetting resin sheet for sealing, which is used for producing a thermosetting resin sheet for sealing used in a hollow package, characterized in that the cured product of the thermosetting resin sheet for sealing has a first resin component as a main component. The seafloor structure of the matrix portion and the region portion including the second resin component as a main component, the matrix portion being softer than the region portion. 如請求項1之密封用熱硬化性樹脂薄片，其中前述硬化物進而包含分散於前述基質部中之填料。 The thermosetting resin sheet for sealing according to claim 1, wherein the cured product further contains a filler dispersed in the matrix portion. 如請求項1之密封用熱硬化性樹脂薄片，其包含熱可塑性樹脂及熱硬化性樹脂，前述第1樹脂成分為前述熱可塑性樹脂，前述第2樹脂成分為前述熱硬化性樹脂。 The thermosetting resin sheet for sealing according to claim 1, comprising a thermoplastic resin and a thermosetting resin, wherein the first resin component is the thermoplastic resin, and the second resin component is the thermosetting resin. 如請求項1之密封用熱硬化性樹脂薄片，其中前述區域部之最大粒徑為0.01μm~5μm。 The thermosetting resin sheet for sealing according to claim 1, wherein the maximum particle diameter of the region portion is 0.01 μm to 5 μm. 如請求項3之密封用熱硬化性樹脂薄片，其中前述熱可塑性樹脂之酸價為1mgKOH/g~100mgKOH/g。 The thermosetting resin sheet for sealing according to claim 3, wherein the thermoplastic resin has an acid value of from 1 mgKOH/g to 100 mgKOH/g. 一種中空封裝之製造方法，其包含使具備被黏著體及安裝於前述被黏著體之電子裝置之裝置安裝體、以及配置於前述裝置安裝體上之密封用熱硬化性樹脂薄片之層合體進行加壓，形成具備前述被黏著體、安裝於前述被黏著體之前述電子裝置及覆蓋前述電子裝置之前述密封用熱硬化性樹脂薄片之密封體之步驟，前述密封用熱硬化性樹脂薄片之硬化物具備 包含第1樹脂成分作為主成分之基質部及包含第2樹脂成分作為主成分之區域部之海島構造，前述基質部比前述區域部更柔軟。 A method of manufacturing a hollow package, comprising: laminating a device mounting body including an adherend and an electronic device mounted on the adherend, and a thermosetting resin sheet for sealing disposed on the device mounting body; a step of forming a sealing body comprising the above-mentioned adherend, the electronic device mounted on the adherend, and the thermosetting resin sheet for sealing covering the electronic device, and the cured product of the thermosetting resin sheet for sealing have The seafloor structure including a matrix portion in which the first resin component is a main component and a region portion including a second resin component as a main component, and the matrix portion is softer than the region portion.
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