WO2016152974A1 - 熱可塑性樹脂フィルム積層体、及び熱可塑性樹脂フィルム積層体を含む成形品 - Google Patents

熱可塑性樹脂フィルム積層体、及び熱可塑性樹脂フィルム積層体を含む成形品 Download PDF

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Publication number
WO2016152974A1
WO2016152974A1 PCT/JP2016/059387 JP2016059387W WO2016152974A1 WO 2016152974 A1 WO2016152974 A1 WO 2016152974A1 JP 2016059387 W JP2016059387 W JP 2016059387W WO 2016152974 A1 WO2016152974 A1 WO 2016152974A1
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WIPO (PCT)
Prior art keywords
thermoplastic resin
resin film
welding
molded product
film
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/JP2016/059387
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English (en)
French (fr)
Inventor
黒川　晴彦
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Mitsubishi Gas Chemical Co Inc
MGC Filsheet Co Ltd
Original Assignee
Mitsubishi Gas Chemical Co Inc
MGC Filsheet Co Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Mitsubishi Gas Chemical Co Inc, MGC Filsheet Co Ltd filed Critical Mitsubishi Gas Chemical Co Inc
Priority to KR1020177027781A priority Critical patent/KR102427367B1/ko
Priority to JP2017508421A priority patent/JP6718863B2/ja
Priority to US15/559,184 priority patent/US20180071995A1/en
Priority to CN201680015816.9A priority patent/CN107405890B/zh
Publication of WO2016152974A1 publication Critical patent/WO2016152974A1/ja
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
    • B29C66/50—General aspects of joining tubular articles; General aspects of joining long products, i.e. bars or profiled elements; General aspects of joining single elements to tubular articles, hollow articles or bars; General aspects of joining several hollow-preforms to form hollow or tubular articles
    • B29C66/51—Joining tubular articles, profiled elements or bars; Joining single elements to tubular articles, hollow articles or bars; Joining several hollow-preforms to form hollow or tubular articles
    • B29C66/53—Joining single elements to tubular articles, hollow articles or bars
    • B29C66/534—Joining single elements to open ends of tubular or hollow articles or to the ends of bars
    • B29C66/5346—Joining single elements to open ends of tubular or hollow articles or to the ends of bars said single elements being substantially flat
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C65/00—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor
    • B29C65/02—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure
    • B29C65/08—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using ultrasonic vibrations
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C66/01—General aspects dealing with the joint area or with the area to be joined
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    • B29C66/3022—Particular design of joint configurations the area to be joined comprising melt initiators said melt initiators being integral with at least one of the parts to be joined
    • B29C66/30223—Particular design of joint configurations the area to be joined comprising melt initiators said melt initiators being integral with at least one of the parts to be joined said melt initiators being rib-like
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    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
    • B29C66/50—General aspects of joining tubular articles; General aspects of joining long products, i.e. bars or profiled elements; General aspects of joining single elements to tubular articles, hollow articles or bars; General aspects of joining several hollow-preforms to form hollow or tubular articles
    • B29C66/51—Joining tubular articles, profiled elements or bars; Joining single elements to tubular articles, hollow articles or bars; Joining several hollow-preforms to form hollow or tubular articles
    • B29C66/53—Joining single elements to tubular articles, hollow articles or bars
    • B29C66/534—Joining single elements to open ends of tubular or hollow articles or to the ends of bars
    • B29C66/5346—Joining single elements to open ends of tubular or hollow articles or to the ends of bars said single elements being substantially flat
    • B29C66/53461—Joining single elements to open ends of tubular or hollow articles or to the ends of bars said single elements being substantially flat joining substantially flat covers and/or substantially flat bottoms to open ends of container bodies
    • B29C66/53462—Joining single elements to open ends of tubular or hollow articles or to the ends of bars said single elements being substantially flat joining substantially flat covers and/or substantially flat bottoms to open ends of container bodies joining substantially flat covers and substantially flat bottoms to open ends of container bodies
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
    • B29C66/70—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material
    • B29C66/71—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the composition of the plastics material of the parts to be joined
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
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    • B29C66/73—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the intensive physical properties of the material of the parts to be joined, by the optical properties of the material of the parts to be joined, by the extensive physical properties of the parts to be joined, by the state of the material of the parts to be joined or by the material of the parts to be joined being a thermoplastic or a thermoset
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    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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Definitions

  • the present invention relates to a resin laminate obtained by ultrasonic welding of a thin thermoplastic resin film and a thermoplastic resin molded product.
  • Examples of other joining methods such as molded products include ultrasonic welding methods using friction between molded products described in Patent Documents 2 and 3.
  • ultrasonic welding methods using friction between molded products described in Patent Documents 2 and 3.
  • bonding between resins by the ultrasonic welding method generally bonding between thick injection molded products is the mainstream, and when performing a welding test between a film and a thick injection molded product, There is a problem that appearance defects are likely to occur due to welding marks when contacting the molded product.
  • An object of the present invention is to provide a thermoplastic resin film laminate having an excellent appearance with high welding strength and few welding marks by ultrasonic welding of a thermoplastic resin film and a thermoplastic resin molded product.
  • thermoplastic resin film As a result of repeated studies to solve the above problems, the present inventors have found that the difference in heat deformation temperature between the thermoplastic resin film and the thermoplastic resin molded product, and the welding allowance (energy director) installed on the surface of the thermoplastic resin molded product. ), It was possible to achieve both the good appearance and the welding strength of the film welded product, which was difficult in the past.
  • the present invention relates to a thermoplastic resin film laminate in which the following thermoplastic resin film and a thermoplastic resin molded article are ultrasonically welded.
  • the thermoplastic resin molded article (B) has at least one opening of 3 cm 2 or more, and the thermoplastic resin film (A) covers at least a part of the opening [1] to [ [3] The thermoplastic resin film resin laminate according to any one of [3].
  • thermoplastic resin film laminate of the present invention obtained by ultrasonically welding a thermoplastic film and a thermoplastic resin molded product has excellent welding strength and good appearance.
  • the thermoplastic resin film laminate of the present invention can be suitably used as, for example, a casing for electric / electronic OA equipment, a battery pack casing, and a transparent window / window frame integrated molded product.
  • thermoplastic resin film and a thermoplastic resin molded product.
  • a plan view showing a state in which the thermoplastic resin film covers the opening of the thermoplastic resin molded article, and a thermoplastic resin cut along the line II-II in FIG. 2 (A).
  • FIG. 2 (B) sectional drawing
  • FIG. 2 (B) shows the side shape of a molded article.
  • FIG. 2 (B) shows the side shape of a molded article.
  • thermoplastic resin film A
  • thermoplastic resin molded product B
  • thermoplastic resin molded product welding allowance energy director
  • the styrenic resin examples include homopolymers such as styrene and ⁇ -methylstyrene, copolymers thereof, and copolymers with unsaturated monomers copolymerizable therewith.
  • GPPS general-purpose polystyrene
  • HIPS impact-resistant polystyrene
  • HPS heat-resistant polystyrene
  • ABS acrylonitrile / butadiene / styrene copolymer
  • ABS Acrylonitrile-butadiene-styrene- ⁇ -methylstyrene copolymer
  • ⁇ -methylstyrene heat-resistant ABS acrylonitrile-butadiene-styrene-phenylmaleimide copolymer (phenylmaleimide heat-resistant ABS), acrylonitrile-styrene copolymer ( AS), acrylonitrile-chlorin
  • polyphenylene ether resin examples include homopolymers such as poly (2,6-dimethyl-1,4-phenylene) ether and poly (2-methyl-6-ethyl-1,4-phenylene) ether. It is also possible to use those modified with a styrene resin.
  • polystyrene resin typically, homopolymers of ⁇ -olefins such as ethylene, propylene, butene-1, 3-methylbutene-1, 3-methylpentene-1, 4-methylpentene-1, or the like are used. Examples thereof include copolymers and copolymers of these with other copolymerizable unsaturated monomers.
  • Typical examples are high density polyethylene, medium density polyethylene, low density polyethylene, linear low density polyethylene, ultrahigh molecular weight polyethylene, ethylene / vinyl acetate copolymer, ethylene / ethyl acrylate copolymer, ethylene / octene- Polyethylenes such as metallocene ethylene / ⁇ -olefin copolymers such as 1 copolymer, atactic polypropylene, syndiotactic polypropylene, isotactic polypropylene, or polypropylenes such as propylene / ethylene block copolymer or random copolymer, Examples thereof include polymethylpentene-1.
  • polyvinyl chloride resin examples include vinyl chloride homopolymers and copolymers with unsaturated monomers copolymerizable with vinyl chloride. Specifically, vinyl chloride / acrylic acid ester copolymer, vinyl chloride / methacrylic acid ester copolymer, vinyl chloride / ethylene copolymer, vinyl chloride / propylene copolymer, vinyl chloride / vinyl acetate copolymer, And vinyl chloride / vinylidene chloride copolymer. In addition, those obtained by chlorinating these polyvinyl chloride resins to increase the chlorine content can also be used.
  • polyamide resin examples include those obtained by ring-opening polymerization of a cyclic aliphatic lactam represented by 6-nylon (polyamide 6) or 12-nylon, 6,6-nylon, 6,10-nylon, 6 , 12-nylon or the like, and those obtained by polycondensation of aliphatic diamine and aliphatic dicarboxylic acid, or those obtained by copolycondensation of aromatic diamine and aromatic dicarboxylic acid in some cases.
  • polyamide 6 cyclic aliphatic lactam represented by 6-nylon (polyamide 6) or 12-nylon, 6,6-nylon, 6,10-nylon, 6 , 12-nylon or the like
  • PA polyamide resin
  • polyester resins include those obtained by polycondensation of aromatic dicarboxylic acids and alkylene glycols such as ethylene glycol, propylene glycol, and butylene glycol. Specific examples include polyethylene terephthalate (PET), polypropylene terephthalate (PPT), polybutylene terephthalate (PBT), and the like.
  • polycarbonate resin examples include 4,4′-dihydroxydiarylalkane polycarbonate.
  • specific examples include bisphenol A polycarbonate (PC), modified bisphenol polycarbonate, copolymers thereof, and the like.
  • acrylic resin examples include methacrylic acid esters, acrylic acid ester homopolymers or copolymers thereof, and copolymers of these with other copolymerizable unsaturated monomers.
  • methacrylic acid ester and acrylic acid ester monomers include methyl, ethyl, n-propyl, isopropyl and butyl esters of methacrylic acid or acrylic acid.
  • a typical example is poly (methyl) methacrylate (PMMA).
  • the thickness of the thermoplastic resin film (A) is 0.4 mm or less. This means that in the thermoplastic resin film, the surface area of the region having a thickness of 0.4 mm or less is 70% or more of the surface area of the entire film.
  • the preferred thickness of the thermoplastic resin film (A) is from 0.01 mm to 0.4 mm, more preferably from 0.1 mm to 0.4 mm, and most preferably from 0.2 mm to 0.3 mm.
  • thermoplastic resin film (A) of this invention can use the film manufactured from the melt extrusion method using a T die, the solvent cast method, and the blow molding method.
  • thermoplastic resin molded product (B) has an average thickness of 0.5 mm or more.
  • examples of the molding method of the thermoplastic resin molded product (B) include injection molded products, press molded products, blow molded products, extruded molded products, vacuum molded products, and compressed air molded products. A molded article is preferably used.
  • the shape of the thermoplastic resin molded product (B) is not limited to a flat plate, but may be a three-dimensional shape.
  • the thermoplastic resin molded product (B) is a three-dimensional molded product having an opening of 3 cm 2 or more, for example, a housing, and the opening is made of the thermoplastic resin film (A).
  • the coating configuration is preferably used in the present invention.
  • thermoplastic resin molded product (energy director) (C) The welding allowance (energy director) (C) is installed on the welding surface of the thermoplastic resin molded product (B) in order to join the thermoplastic resin film (A) and the thermoplastic resin molded product (B).
  • ultrasonic welding As a bonding method, ultrasonic welding is used. In ultrasonic welding, ultrasonic energy concentrates on the welding allowance (energy director) installed in the thermoplastic resin molded product (B), and the welding allowance (C) and thermoplasticity of the thermoplastic resin molded product (B). The melted welding allowance (energy director) and the thermoplastic resin film (A) are joined by heat generated by friction with the resin film (A).
  • the energy director has a convex shape toward the thermoplastic resin film (A) to be joined, that is, upward, and the film thickness cross section is triangular.
  • the film thickness cross section is triangular.
  • an energy director with a vertex angle of 40 degrees to 120 degrees is used, preferably the vertex angle is 50 to 70 degrees, most preferably 60 degrees. That is, it is particularly preferable that the cross-sectional shape is an equilateral triangle.
  • the cross-sectional shape of the welding allowance (energy director) (C) is a triangle, particularly a regular triangle, it is possible to concentrate the ultrasonic energy at the upper end, that is, the apex of the triangle in ultrasonic welding.
  • thermoplastic resin molded product (B) side it is possible to sufficiently secure the welding margin region on the thermoplastic resin molded product (B) side, that is, on the bottom side of the triangle.
  • a quadrangle should be avoided as a cross-sectional shape of the welding allowance (energy director) (C), and it is preferable to avoid a circular shape.
  • the shape of the welding allowance (energy director) (C) can be imparted by a method of transferring from injection molding or hot press molding with a mold, machining of the molded product, processing by printing, and the like.
  • welding allowance (C) is arrange
  • the welding allowance (C) is preferably provided in a row on the welding surface of the thermoplastic resin molded product (B). This is because when a plurality of rows of welding allowances (C), for example, a plurality of parallel rows are provided on the welding surface of the thermoplastic resin molded product (B), ultrasonic energy is dispersed in the plurality of rows.
  • the length 24H is preferably 72% to 130% of the thickness 10T of the thermoplastic resin film (A) 10. That is, when the thickness of the thermoplastic resin film (A) is A (mm) and the welding allowance (C) is C (mm), The value of C (mm) / A (mm) ⁇ 100 (%) is preferably 72% to 130%, The value of (1-C (mm) / A (mm)) ⁇ 100 (%) is preferably ⁇ 28% to 30%.
  • the height 24H of the welding allowance 24 is 75 to 125%, more preferably 80 to 120%, particularly preferably 85 to 115% of the thickness 10T of the thermoplastic resin film (A) 10.
  • the height 24H of the welding allowance (energy director) exceeds the upper limit, the welding strength can be obtained, but there may be a problem that appearance defects are likely to occur due to the pushing of the energy director.
  • the height 24H of the welding allowance (energy director) does not satisfy the lower limit, a laminate having a good appearance can be obtained, but there may be a problem that the welding strength is lowered. As shown in FIG.
  • thermoplastic resin film 10 and the thermoplastic resin are formed by ultrasonic welding in which the thermoplastic resin film 10 and the thermoplastic resin molded product 20 are welded as indicated by an arrow in a state of facing each other.
  • a laminate with the molded product 20 is formed.
  • the welding allowance 24 is melted by ultrasonic welding and becomes a joint part melt-mixed with the thermoplastic resin film 10.
  • the surface of these members becomes substantially smooth, and the problem on an external appearance does not arise.
  • Thermal deformation temperature of thermoplastic resin film (A) and thermoplastic resin molded product (B) is the glass transition temperature when these resins are amorphous resins, and when these resins are crystalline resins. Is the melting point.
  • the heat distortion temperature can be measured by DSC (differential thermal scanning calorimetry). In the case of an incompatible polymer alloy material, the heat deformation temperature of the matrix resin is used.
  • a combination having a difference in heat distortion temperature of 20 ° C. or less is preferably used.
  • the difference in heat distortion temperature is 15 ° C. or less, and particularly preferably 10 ° C. or less.
  • the thermoplastic resin film (A) and the thermoplastic resin molded product (B) are preferably highly compatible or highly reactive.
  • the thermoplastic resin film (A) and the thermoplastic resin molded product (B) are formed of the same kind of resin material.
  • the same kind of material here refers to a thermoplastic resin material having the same resin system shown in the paragraph [0013] and the following, more specifically, a thermoplastic resin material having the same kind of chemical bond.
  • the same type of resin in the present invention can be used even if the molecular weight is different, the type of copolymerization, the copolymer composition ratio, and the amount of additives are different.
  • the difference in thermal deformation temperature between the thermoplastic resin film (A) and the thermoplastic resin molded product (B) exceeds 20 ° C., when the appearance is given priority, the resin welding strength becomes insufficient, and the welding strength is given priority. In some cases, since higher ultrasonic energy is required, there is a problem that the appearance of the obtained thermoplastic resin film laminate (molded article) is inferior.
  • thermoplastic resin film laminate In the method for producing a thermoplastic resin film laminate of the present invention, ultrasonic welding is used. That is, a thermoplastic resin film laminated body is manufactured by ultrasonically welding the above-mentioned thermoplastic resin film (A) and the welding margin (C) of the above-mentioned thermoplastic resin molded product (B). For example, by providing a welding allowance (C) around the opening of the thermoplastic resin molded product (B) and bonding the thermoplastic resin film (A) so as to cover the opening, the thermoplastic resin film laminate is obtained. can get.
  • the thickness of the thermoplastic resin film (A) is adjusted to a value within a predetermined range, and the welding allowance (C) having a predetermined height is further adjusted to the thermoplastic resin molded product (B).
  • the manufacturing method provided on the welding surface a laminate having good welding strength and appearance can be obtained, and further, the difference in thermal deformation temperature between the thermoplastic resin film (A) and the thermoplastic resin molded product (B) is obtained. By suppressing it, it is possible to ensure both high welding strength and good appearance.
  • thermoplastic resin composition used in the present invention may contain components other than those described above as necessary as long as desired physical properties are not significantly impaired.
  • other components include phosphates, heat stabilizers typified by phosphites, antioxidants typified by hindered phenol compounds, UV absorbers typified by benzotriazole compounds, antifogging agents, and anti-blocking agents.
  • One of these resin additives may be contained, or two or more thereof may be contained in any combination and ratio.
  • thermoplastic resin film 10 and the heat are so formed that the thermoplastic resin film 10 covers the opening 20H with respect to the thermoplastic resin molded article 20 having the opening 20H.
  • a laminate with the plastic resin molded product 20 can be formed.
  • the plastic resin molded product 20 is welded by ultrasonic welding.
  • a wider internal space 40A is formed compared to the case where the entire surface is formed by the wall member 20W of the thermoplastic resin molded product 20 having a thickness larger than that of the thermoplastic resin film 10. For example, a space for accommodating internal components such as a battery is increased.
  • the thermal deformation temperature (Tg) of the thermoplastic resin was measured with a differential thermal scanning calorimeter SSC-5200 (DSC) manufactured by Seiko Denshi Kogyo Co., Ltd. In the measurement, the temperature was raised to 20 ° C./min to a temperature at which the resin component melts in a nitrogen atmosphere (260 ° C.), rapidly cooled to ⁇ 30 ° C., and then again raised to 10 ° C./min (2nd run). The glass transition temperature and the melting point were determined from the obtained DSC curve by the starting point method.
  • DSC-5200 differential thermal scanning calorimeter SSC-5200
  • ⁇ Appearance evaluation> The appearance evaluation of the molded product laminate after ultrasonic welding of the film laminate was performed visually. Visual observation was performed from the film side. There is almost no surface damage due to the indentation of the welding allowance (energy director) on the film surface, particularly excellent conditions are excellent, there are few surface scratches, good conditions are good, surface defects are somewhat conspicuous, surface defects are somewhat poor, and surface damage is large A state inferior in appearance was regarded as defective.
  • the polycarbonate resin was compounded according to the formulation shown in Table 1, and a commercially available polybutylene terephthalate was used.
  • A-1 “Iupilon (registered trademark) S-3000F” manufactured by Mitsubishi Engineering Plastics Co., Ltd., bisphenol A type aromatic polycarbonate resin, heat distortion temperature (glass transition temperature) 145 ° C.
  • A-2) “Novaduran (registered trademark) 5020” manufactured by Mitsubishi Engineering Plastics Co., Ltd., polybutylene terephthalate resin, heat distortion temperature (melting point) 224 ° C.
  • the cylinder / die head temperature was set at 260 ° C. for polycarbonate and 235 ° C. for polybutylene terephthalate.
  • the film thickness shown in Table 1 was used.
  • the size of the film used for the ultrasonic welding test was cut to 150 mm ⁇ 40 mm to cover the thermoplastic resin molded product (B) shown in FIG.
  • thermoplastic resin molded product (B)> A 150 mm ⁇ 100 mm ⁇ 1.2 mm thick flat resin plate of the composition described in Table 1 was molded by injection molding. By cutting the obtained injection molded product, a thermoplastic resin molded product having a welding allowance (ED, energy type) (C) 24 having the dimensions shown in FIG. 3 and the shape schematically shown in FIG. (B) 20 was produced.
  • ED, energy type a welding allowance
  • C welding allowance
  • symbol in FIG. 3 and 4 shows the dimension (mm) of each member.
  • thermoplastic resin molded product (B) 20 and the thermoplastic resin film (A) 10 were integrated to produce a welding allowance integral type thermoplastic resin molded product.
  • the height of the welding allowance (ED, energy tyretor) (C) was set to a value of 0.1 to 0.4 mm shown in Table 1. Then, using the thermoplastic resin molded product (B) 20 having the shape shown in FIG. 3, the thermoplastic resin film 10 and the thermoplastic resin molded product 20 so that the thermoplastic resin film completely covers the two openings 20H. And were welded.
  • the thickness of the thermoplastic resin molded product (B) 20 is 1.0 mm, the vertical and horizontal lengths are 4.0 cm and 15.0 cm, respectively, and the vertical and horizontal lengths of each opening 20H are 1. 0 cm and 12.5 cm, and the area of each opening 20H was 12.5 cm 2 (see FIG. 3).
  • the welding allowance (C) 24 was provided in the position shown with the broken line so that the circumference
  • thermoplastic resin film (A) 10 is made into a thermoplastic resin molded product ( B) It can be firmly fixed to 20.
  • region I of the welding surface 20S the process which provides the welding margin becomes easy by providing the area
  • ⁇ Ultrasonic welding method> For ultrasonic welding, a Branson 2000Xdt (20 kHz 2200 W) manufactured by Nippon Emerson Co., Ltd. was used, and a welding horn made of a titanium alloy suitable for the shape of the molded product was used. The welding test is performed on the mirror surface side of the thermoplastic resin film (A) and the surface on which the welding allowance of the thermoplastic resin molded product (B) is formed, and the thermoplastic resin molded product (B) is thermoplastic on the upper horn side. The resin film (A) was fixed to the lower horn cradle and a welding test was performed.
  • thermoplastic resin film (A) In order to protect the mat pattern of the thermoplastic resin film (A), a test was conducted by bringing a protective film made of polyethylene having a thickness of 0.03 mm into contact with the film.
  • the parameter settings in the ultrasonic welding test are as follows. That is, an ultrasonic welding test was performed under the conditions of an irradiation time of 0.3 sec (0.45 sec for polybutylene terephthalate resin), a hold time of 0.3 sec, an air cylinder pressure of 200 kPa, a trigger force of 250 N, and an amplitude of 100%.

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Abstract

　熱可塑性樹脂フィルムと熱可塑性樹脂成形品の超音波溶着により、高い溶着強度及び溶着痕が少なく優れた外観を有する熱可塑性樹脂フィルム積層体を提供する。　厚み０．４ｍｍ以下の熱可塑性樹脂フィルム（Ａ）と、溶着代（Ｃ）を有する厚み０．５ｍｍ以上の熱可塑性樹脂成形品（Ｂ）の前記溶着代（Ｃ）とを超音波溶着して得られる熱可塑性樹脂積層体であって、該溶着代（Ｃ）の高さが該熱可塑性樹脂フィルム（Ａ）の厚みの７５～１２５％である熱可塑性樹脂フィルム積層体により、上記課題は解決される。

Description

熱可塑性樹脂フィルム積層体、及び熱可塑性樹脂フィルム積層体を含む成形品
　本発明は、薄肉の熱可塑性樹脂フィルムと、熱可塑性樹脂成形品とを超音波溶着して得られる樹脂積層体等に関する。
　近年、電気電子機器の部材には、製品の小形化と部品の薄肉化が進みつつあるため、さらなる高意匠性が求められている。なかでも小型充電池を内蔵した電池パック用の筐体は、高容量化を目的にプラスチック成形品の薄肉化が進んでいる。今後も部材の薄肉化が進むことで、電池パック用筐体の厚みは０．４ｍｍ以下の部分が成形品表面積中の４０％以上を占めることになるといわれている。
　このような薄肉の成形品を得る方法としてこれまでに採用されてきたものとしては、通常の射出成形法、及び特許文献１に記載のあらかじめ薄肉フィルムを金型内に設置し射出成形を行うインモールドフィルムを用いた射出成形法などが挙げられる。しかし通常の射出成形方法では、樹脂の薄肉部への充填が難しく、製品がショートショットとなる問題、また高射出圧力で充填した場合は成形品の薄肉部が反る問題があった。また、特許文献１に記載のインモールドフィルムによる射出成形法では、開口部を有する成形品の場合は、成形品とフィルムの接触部と非接触部との熱収縮の差により、開口部を覆うフィルムが撓んでしまう問題があった。
　また他に、接着剤や両面テープを介してフィルムと射出成形品を貼り合せる方法などがあるが、いずれの方法によっても、局部的に接着部の厚みが増加するため外観の良いものは得られなかった。
　成形品等の他の接合方法として、特許文献２、３に記載の成形品間の摩擦を利用した超音波溶着方法が挙げられる。しかし、超音波溶着方法による樹脂間の接合に関しては、一般的に肉厚の射出成形品同士での接合が主流であり、フィルムと肉厚のある射出成形品で溶着試験を行う場合は、フィルムが成形品に接触する際の溶着痕による外観不良が生じやすい問題があった。
特開２０１３－１２９０７７号公報 特許４５５８３７４ 特開昭６２－５４７５７号公報
　本発明の課題は、熱可塑性樹脂フィルムと熱可塑性樹脂成形品の超音波溶着により、高い溶着強度及び溶着痕が少なく優れた外観を有する熱可塑性樹脂フィルム積層体を提供することにある。
　本発明者らは上記課題を解決するべく検討を重ねた結果、熱可塑性樹脂フィルムと熱可塑性樹脂成形品の熱変形温度の差、及び熱可塑性樹脂成形品表面に設置する溶着代（エネルギーダイレクター）の高さに着目し、従来、困難であったフィルム溶着品の良好な外観と溶着強度との両立を可能とした。
　すなわち、本発明は、以下に示す熱可塑性樹脂フィルムと熱可塑性樹脂成形品を超音波溶着した熱可塑性樹脂フィルム積層体に関するものであり、以下を要旨とする。
［１］厚み０．４ｍｍ以下の熱可塑性樹脂フィルム（Ａ）と、溶着代（Ｃ）を有する厚み０．５ｍｍ以上の熱可塑性樹脂成形品（Ｂ）の前記溶着代（Ｃ）とを超音波溶着して得られる熱可塑性樹脂積層体であって、該溶着代（Ｃ）の高さが熱可塑性樹脂フィルム（Ａ）の厚みの７２～１３０％であり、熱可塑性樹脂フィルム（Ａ）と熱可塑性樹脂成形品（Ｂ）の熱変形温度の差が２０℃以下である熱可塑性樹脂フィルム積層体。
［２］熱可塑性樹脂フィルム（Ａ）と熱可塑性樹脂成形品（Ｂ）とが同種の樹脂材料で形成されている［１］に記載の熱可塑性樹脂フィルム積層体。
［３］熱可塑性樹脂フィルム（Ａ）の厚みが０．２ｍｍから０．３ｍｍである、[１]又は［２］のいずれかに記載の熱可塑性樹脂フィルム積層体。
［４］熱可塑性樹脂成形品（Ｂ）が、３ｃｍ２以上の開口部を少なくとも１つ以上有し、開口部の少なくとも一部を熱可塑性樹脂フィルム（Ａ）が覆っている[１]～[３]のいずれかに記載の熱可塑性樹脂フィルム樹脂積層体。
［５］上記［１］～［４］のいずれかに記載の熱可塑性樹脂フィルム積層体を含有する成形品。
　熱可塑性フィルムと熱可塑性樹脂成形品を超音波溶着した本発明の熱可塑性樹脂フィルム積層体は、優れた溶着強度ならびに良好な外観を有する。このため、本発明の熱可塑性樹脂フィルム積層体は、例えば、電気電子ＯＡ機器用筐体、電池パック筐体、透明窓/窓枠一体型成形品として好適に使用できる。
熱可塑性樹脂フィルム及び熱可塑性樹脂成形品の簡略的な断面図である。 熱可塑性樹脂フィルムが、熱可塑性樹脂成形品の開口部を覆った状態を示す平面図（図２（Ａ））と、図２（Ａ）におけるII‐II線に沿って切断した、熱可塑性樹脂成形品の側面形状を示す断面図（図２（Ｂ））である 図２とは異なる熱可塑性樹脂成形品の平面図である。 図３における熱可塑性樹脂成形品の領域Ｉ及びＩＩを拡大して示す平面図である。
　以下、本発明を詳細に説明する。尚、本発明は、以下の実施の形態に限定されるものではなく、発明の効果を有する範囲において任意に変更して実施することができる。
［熱可塑性樹脂フィルム（Ａ）、熱可塑性樹脂成形品（Ｂ）及び熱可塑性樹脂成形品の溶着代（エネルギーダイレクター）（Ｃ）の組成］
　本発明の樹脂組成物に含まれる熱可塑性樹脂には、特に制限はなく、従来、成形材料として使用されているものから任意に選択して使用することができる。例えば、スチレン系樹脂、ポリフェニレンエーテル系樹脂、ポリオレフィン系樹脂、ポリ塩化ビニル系樹脂、ポリアミド系樹脂、ポリエステル系樹脂、ポリカーボネート系樹脂及びアクリル系樹脂等が挙げられる。
　スチレン系樹脂としては、例えばスチレン、α－メチルスチレン等の単独重合体又はこれらの共重合体、あるいはこれらと共重合可能な不飽和単量体との共重合体等が挙げられる。具体的には、一般用ポリスチレン（ＧＰＰＳ）、耐衝撃性ポリスチレン（ＨＩＰＳ）、耐熱性ポリスチレン（例えば、α－メチルスチレン重合体あるいは共重合体等）、アクリロニトリル・ブタジエン・スチレン共重合体（ＡＢＳ）、アクリロニトリル・ブタジエン・スチレン・α－メチルスチレン共重合体（α－メチルスチレン系耐熱ＡＢＳ）、アクリロニトリル・ブタジエン・スチレン・フェニルマレイミド共重合体（フェニルマレイミド系耐熱ＡＢＳ）、アクリロニトリル－スチレン共重合体（ＡＳ）、アクリロニトリル－塩素化ポリスチレン・スチレン系共重合体（ＡＣＳ）、アクリロニトリル・エチレンプロピレンゴム・スチレン共重合体（ＡＥＳ）、アクリルゴム・アクリロニトリル・スチレン共重合体（ＡＡＳ）、あるいはシンディオタクティクポリスチレン（ＳＰＳ）等が挙げられる。また、スチレン系樹脂は、ポリマーブレンドしたものであっても良い。
　ポリフェニレンエーテル系樹脂（ＰＰＥ）としては、例えばポリ（２，６－ジメチル－１，４－フェニレン）エーテル、ポリ（２－メチル－６－エチル－１，４－フェニレン）エーテル等のホモポリマーが挙げられ、これをスチレン系樹脂で変性したものを用いることもできる。
　ポリオレフィン系樹脂としては、代表的には、エチレン、プロピレン、ブテン－１、３－メチルブテン－１、３－メチルペンテン－１、４－メチルペンテン－１等のα－オレフィンの単独重合体又はこれらの共重合体、あるいはこれらと他の共重合可能な不飽和単量体との共重合体等が挙げられる。代表例としては、高密度ポリエチレン、中密度ポリエチレン、低密度ポリエチレン、直鎖状低密度ポリエチレン、超高分子量ポリエチレン、エチレン・酢酸ビニル共重合体、エチレン・アクリル酸エチル共重合体、エチレン・オクテン－１共重合体等のメタロセン系エチレン・αオレフィン共重合体等のポリエチレン類、アタクチックポリプロピレン、シンディオタクチックポリプロピレン、アイソタクチックポリプロピレンあるいはプロピレン・エチレンブロック共重合体又はランダム共重合体等ポリプロピレン類、ポリメチルペンテン－１等を挙げることができる。
　ポリ塩化ビニル系樹脂としては、例えば塩化ビニル単独重合体や塩化ビニルと共重合可能な不飽和単量体との共重合体が挙げられる。具体的には、塩化ビニル・アクリル酸エステル共重合体、塩化ビニル・メタクリル酸エステル共重合体、塩化ビニル・エチレン共重合体、塩化ビニル・プロピレン共重合体、塩化ビニル・酢酸ビニル共重合体、塩化ビニル・塩化ビニリデン共重合体等が挙げられる。また、これらのポリ塩化ビニル系樹脂を塩素化して塩素含有量を高めたものも使用できる。
　ポリアミド系樹脂（ＰＡ）としては、例えば６－ナイロン（ポリアミド６）あるいは１２－ナイロン等に代表される環状脂肪族ラクタムを開環重合したもの、６，６－ナイロン、６，１０－ナイロン、６，１２－ナイロン等の脂肪族ジアミンと脂肪族ジカルボン酸とを重縮合したもの、あるいは場合により芳香族ジアミン、芳香族ジカルボン酸を共重縮合したもの等を挙げることができる。
　ポリエステル系樹脂としては、例えば芳香族ジカルボン酸とエチレングリコール、プロピレングリコール、ブチレングリコール等のアルキレングリコールとを重縮合させたものが挙げられる。具体例としては、ポリエチレンテレフタレート（ＰＥＴ）、ポリプロピレンテレフタレート（ＰＰＴ）、ポリブチレンテレフタレート（ＰＢＴ）等が挙げられる。
　ポリカーボネート系樹脂としては、例えば４，４’－ジヒドロキシジアリールアルカン系ポリカーボネート等が挙げられる。具体例としては、ビスフェノールＡ系ポリカーボネート（ＰＣ）、変性ビスフェノール系ポリカーボネート、それらの共重合体等を挙げることができる。
　アクリル系樹脂としては、例えばメタクリル酸エステル、アクリル酸エステル単独重合体又はこれらの共重合体、あるいはこれらと他の共重合可能な不飽和単量体との共重合体等が挙げられる。メタクリル酸エステル、アクリル酸エステル単量体としては、メタクリル酸あるいはアクリル酸のメチル、エチル、ｎ－プロピル、イソプロピル、ブチルの各エステル体等が挙げられる。代表的には、ポリ（メチル）メタアクリレート（ＰＭＭＡ）が挙げられる。
［熱可塑性樹脂フィルム（Ａ）］
　本発明において、熱可塑性樹脂フィルム（Ａ）の厚みは０．４ｍｍ以下である。これは熱可塑性樹脂フィルムにおいて、厚みが０．４ｍｍ以下である領域の表面積がフィルム全体の表面積の７０％以上であるものをいう。熱可塑性樹脂フィルム（Ａ）の厚みが０．４ｍｍより大きいと、通常、射出成形での成形が容易となり、また充分な厚みを有するためエネルギーダイレクターの押込による外観不良が観察されないことから、本発明の効果が充分に得られない。熱可塑性樹脂フィルム（Ａ）の好ましい厚みは０．０１ｍｍから０．４ｍｍ以下であり、さらに好ましくは０．１ｍｍから０．４ｍｍ、最も好ましくは０．２ｍｍから０．３ｍｍである。熱可塑性樹脂フィルム（Ａ）の厚みが０．０１ｍｍより小さいとフィルムが薄すぎるため、超音波溶着後の良好な外観が得られず、また筐体として用いた場合、内部部品の保護が不充分となる問題が生じ得る。なお、本発明の熱可塑性樹脂フィルム（Ａ）は、Ｔダイを用いた溶融押出法、溶剤キャスト法、ブロー成形法から製造されたフィルムを用いることができる。
［熱可塑性樹脂成形品（Ｂ）］
　本発明において、熱可塑性樹脂成形品（Ｂ）は、厚みの平均が０．５ｍｍ以上である。また、熱可塑性樹脂成形品（Ｂ）の成形方法は、射出成形品、プレス成形品、ブロー成形品、押出成形品、真空成形品、圧空成形品などが挙げられるが、生産性の観点から射出成形品が好ましく用いられる。
　本発明の熱可塑性樹脂フィルム積層体においては、熱可塑性樹脂成形品（Ｂ）の形状は平板に限らず、三次元形状であっても良い。特に効果的な形状としては、熱可塑性樹脂成形品（Ｂ）が３ｃｍ２以上の開口部を有する三次元の成形品、例えば、筐体であり、その開口部を熱可塑性樹脂フィルム（Ａ）で被覆する構成が本発明において好ましく用いられる。熱可塑性樹脂成形品（Ｂ）の開口部を熱可塑性樹脂フィルム（Ａ）で被覆することにより、部材の軽量化、例えば筐体である成形品（Ｂ）の内部において部品の高充填化が可能となる。
［熱可塑性樹脂成形品の溶着代（エネルギーダイレクター）（Ｃ）］
　溶着代（エネルギーダイレクター）（Ｃ）は、熱可塑性樹脂フィルム（Ａ）と熱可塑性樹脂成形品（Ｂ）を接合するために、熱可塑性樹脂成形品（Ｂ）の溶着面に設置される。接合法としては、超音波溶着が用いられる。超音波溶着においては、熱可塑性樹脂成形品（Ｂ）に設置された溶着代（エネルギーダイレクター）に超音波エネルギーが集中し、熱可塑性樹脂成形品（Ｂ）の溶着代（Ｃ）と熱可塑性樹脂フィルム（Ａ）との摩擦によって生じる発熱によって、溶融した溶着代（エネルギーダイレクター）と熱可塑性樹脂フィルム（Ａ）が接合される。
　エネルギーダイレクターは、接合される熱可塑性樹脂フィルム（Ａ）側、すなわち上側に向かって凸の形状であり、フィルム厚み断面の形状が三角形であることが好ましい。この断面の三角形については、頂点の角度が４０度から１２０度のエネルギーダイレクターが用いられ、好ましくは頂点の角度は５０～７０度、最も好ましくは６０度である。すなわち、断面形状が正三角形であることが特に好ましい。このように、溶着代（エネルギーダイレクター）（Ｃ）の断面形状が三角形、特に正三角形であれば、超音波溶着において、超音波エネルギーを上端部、すなわち三角形の頂点に集中させることを可能にしつつ、熱可塑性樹脂成形品（Ｂ）側、すなわち三角形の底辺側の溶着代の領域を十分に確保できる。このような観点から、溶着代（エネルギーダイレクター）（Ｃ）の断面形状として、四角形を回避すべきであり、円状も回避することが好ましい。溶着代（エネルギーダイレクター）（Ｃ）の形状は、射出成形又は熱プレス成形から金型で転写する方法、成形品の機械切削、印刷等による加工によって付与できる。
　なお、溶着代（Ｃ）は、熱可塑性樹脂成形品（Ｂ）の溶着面において、連なって列状（ライン状）に配置されていることが好ましい。特に、溶着代（Ｃ）は、熱可塑性樹脂成形品（Ｂ）の溶着面において一列に設けられていることが好ましい。熱可塑性樹脂成形品（Ｂ）の溶着面において溶着代（Ｃ）の複数の列、例えば、平行な複数の列を設けると、超音波エネルギーが複数の列に分散されるためである。
　溶着代（（Ｃ）エネルギーダイレクター）の高さ、すなわち、図１に示されるように、熱可塑性樹脂成形品（Ｂ）２０の溶着面２０Ｓから例えば断面が三角形である溶着代２４の頂点までの長さ２４Ｈは、熱可塑性樹脂フィルム（Ａ）１０の厚み１０Ｔの７２％～１３０％とすることが好ましい。すなわち、熱可塑性樹脂フィルム（Ａ）の厚みをＡ（ｍｍ）、溶着代（Ｃ）の高さをＣ（ｍｍ）としたときに、
　Ｃ（ｍｍ）／Ａ（ｍｍ）×１００（％）の値が、好ましくは７２％～１３０％であり、
　（１－Ｃ（ｍｍ）／Ａ（ｍｍ））×１００（％）の値が、好ましくは－２８％～３０％である。
　なお好ましくは、溶着代２４の高さ２４Ｈは、熱可塑性樹脂フィルム（Ａ）１０の厚み１０Ｔの７５～１２５％、より好ましくは８０～１２０％、特に好ましくは８５～１１５％である。溶着代（エネルギーダイレクター）の高さ２４Ｈが上限を超える場合は、溶着強度は得られるがエネルギーダイレクターの押込による外観不良が起こりやすいという問題が生じ得る。また溶着代（エネルギーダイレクター）の高さ２４Ｈが下限を満たさない場合は、良好な外観の積層体が得られるが、溶着強度が低下する問題が生じ得る。
　図１に示されるように、熱可塑性樹脂フィルム１０と熱可塑性樹脂成形品２０とを互いに対向させた状態で、矢印の示すように溶着させる超音波溶着により、熱可塑性樹脂フィルム１０と熱可塑性樹脂成形品２０との積層体が形成される。こうして得られる積層体の熱可塑性樹脂フィルム１０と熱可塑性樹脂成形品２０との間において、溶着代２４は、超音波溶着により溶けて熱可塑性樹脂フィルム１０と溶融混合された接合部となる。このため、製造された積層体における熱可塑性樹脂フィルム１０と熱可塑性樹脂成形品２０との接合領域では、これらの部材の表面はいずれも実質的に平滑になり、外観上の問題は生じない。
［熱可塑性樹脂フィルム（Ａ）、熱可塑性樹脂成形品（Ｂ）の熱変形温度］
　本発明における熱可塑性樹脂フィルム（Ａ）と熱可塑性樹脂成形品（Ｂ）の熱変形温度は、これらの樹脂が非晶性樹脂の場合はガラス転移温度とし、これらの樹脂が結晶性樹脂の場合は融点とする。熱変形温度はＤＳＣ（示差熱走査熱量分析計）によって測定できる。非相溶系のポリマーアロイ材の場合は、マトリックス樹脂の熱変形温度とする。
　熱可塑性樹脂フィルム（Ａ）と熱可塑性樹脂成形品（Ｂ）の組合せは、好ましくは、熱変形温度の差が２０℃以下のものを用いる。より好ましくは、熱変形温度の差は１５℃以下であり、特に好ましくは１０℃以下である。なかでも熱可塑性樹脂フィルム（Ａ）と熱可塑性樹脂成形品（Ｂ）樹脂の種類は相溶性の高いもの、もしくは反応性の高いものが好ましく用いられる。特に、熱可塑性樹脂フィルム（Ａ）と熱可塑性樹脂成形品（Ｂ）を、同種の樹脂材料で形成することが好ましい。ここでいう同種の材料とは、段落［００１３］以下に示した樹脂の系統が同一のもの、より具体的には同種の化学結合を有する熱可塑性樹脂材料のことをいう。そのため、同種の分子構造を有する樹脂材料であれば、分子量が異なるもの、共重合の種類、共重合組成比、添加剤の配合量が異なっているものであっても、本発明における同種の樹脂材料と定義する。
　熱可塑性樹脂フィルム（Ａ）と熱可塑性樹脂成形品（Ｂ）の熱変形温度の差が２０℃を超える場合、外観を優先にした場合は樹脂溶着強度が不充分となり、その溶着強度を優先した場合はさらに高い超音波エネルギーが必要となるため、得られた熱可塑性樹脂フィルム積層体（成形品）の外観が劣るといった問題が生じ得る。
［熱可塑性樹脂フィルム積層体の製造方法］
　本発明の熱可塑性樹脂フィルム積層体の製造方法においては、超音波溶着が用いられる。すなわち、熱可塑性樹脂フィルム積層体は、上述の熱可塑性樹脂フィルム（Ａ）と、上述の熱可塑性樹脂成形品（Ｂ）の溶着代（Ｃ）とを超音波溶着することにより、製造される。例えば、熱可塑性樹脂成形品（Ｂ）の開口部の周囲に溶着代（Ｃ）を設け、開口部を覆うように熱可塑性樹脂フィルム（Ａ）を接合させることにより、熱可塑性樹脂フィルム積層体が得られる。
　以上のように、熱可塑性樹脂フィルム（Ａ）の厚さを所定の範囲内の値となるように調整し、さらに、所定の高さの溶着代（Ｃ）を熱可塑性樹脂成形品（Ｂ）の溶着表面上に設ける製法により、溶着強度及び外観の良好な積層体が得られるのであり、さらに、熱可塑性樹脂フィルム（Ａ）と熱可塑性樹脂成形品（Ｂ）との熱変形温度の差を抑制することにより、高い溶着強度と良好な外観との両立が確実に可能となる。
　本発明において用いられる熱可塑性樹脂組成物は、所望の諸物性を著しく損なわない限り、必要に応じて、上述したもの以外の成分を含有していてもよい。その他の成分としては、例えば、ホスフェート、ホスファイトを代表とする熱安定剤、ヒンダードフェノール化合物を代表とする抗酸化剤、ベンゾトリアゾール系化合物を代表とする紫外線吸収剤、防曇剤、アンチブロッキング剤、流動性改良剤、衝撃強度改良剤、摺動性改質剤、可塑剤、分散剤、抗菌剤、難燃剤、ガラス繊維、炭素繊維などの各種樹脂添加剤などが挙げられる。これらの樹脂添加剤は１種が含有されていてもよく、２種以上が任意の組み合わせ及び比率で含有されていても良い。
　図２に示される本発明の一実施形態においては、開口部２０Ｈを有する熱可塑性樹脂成形品２０に対して、熱可塑性樹脂フィルム１０が開口部２０Ｈを覆うように、熱可塑性樹脂フィルム１０と熱可塑性樹脂成形品２０との積層体を形成することができる。この場合、熱可塑性樹脂フィルム１０の溶着面１０Ｓと熱可塑性樹脂成形品２０の溶着面２０Ｓ（図１参照）とが接する領域、すなわち、図２では境界面３０Ｓにおいて、熱可塑性樹脂フィルム１０と熱可塑性樹脂成形品２０とを超音波溶着により溶着させる。
　こうして製造された筐体である積層体４０においては、厚みが熱可塑性樹脂フィルム１０よりも大きい熱可塑性樹脂成形品２０の壁部材２０Ｗにより全面を形成した場合に比べて、より広い内部空間４０Ａを確保することができ、例えば電池などの内部部品を収容するスペースが増すこととなる。
　以下、実施例を示して本発明について更に具体的に説明する。ただし、本発明は以下の実施例に限定されるものではなく、本発明の要旨を逸脱しない範囲において、任意に変更して実施することができる。
＜熱変形温度の測定＞
　熱可塑性樹脂の熱変形温度（Ｔｇ）は、示差熱走査熱量分析計セイコー電子工業（株）製のＳＳＣ－５２００（ＤＳＣ）で測定した。測定においては、窒素雰囲気下で樹脂成分が溶融する温度（２６０℃）に２０℃／ｍｉｎで昇温し、－３０℃まで急冷した後、再度１０℃／ｍｉｎで昇温（２ｎｄ　ｒｕｎ）した。得られたＤＳＣ曲線から始点法によってガラス転移温度及び融点を求めた。
＜溶着強度＞
　超音波溶着強度の評価として、フィルム積層体の溶着後の成形品の成形品穴開き部を、成形品側から指で押込み破壊した。
　特に良好：溶着部での破壊は見られなかった。
　良好：一部、溶着代での破壊が見られた。
　不良：溶着していたフィルムが剥離した。
＜外観評価＞
　フィルム積層体の超音波溶着後の成形品積層体の外観評価を目視にて行った。目視観察はフィルム側から行った。フィルム表面に溶着代（エネルギーダイレクター）の押込みによる表面傷がほとんどなく特に優れた状態を特に良好、表面傷が少なく良好な状態を良好、表面傷がやや目立つものをやや不良、表面傷が大きく外観に劣る状態を不良とした。
＜たわみ評価＞
　図３に示すように、２つの開口部を有し、図１及び２に示された成形品とは形状の異なる平板状の成形品にフィルム積層体を溶着させた後に、成形品積層のたわみの度合いを目視にて確認した。たわみがほとんどない状態を良好、たわみが大きい状態を不良とした。
［使用材料］
＜熱可塑性樹脂＞
　ポリカーボネート樹脂は表１の配合でコンパウンド化を実施、ポリブチレンテレフタレートは市販のものを用いた。
（ａ－１）三菱エンジニアリングプラスチックス（株）製「ユーピロン（登録商標）Ｓ－３０００Ｆ」、ビスフェノールＡ型芳香族ポリカーボネート樹脂、熱変形温度（ガラス転移温度）１４５℃
（ａ－２）三菱エンジニアリングプラスチックス（株）製「ノバデュラン（登録商標）５０２０」、ポリブチレンテレフタレート樹脂、熱変形温度（融点）２２４℃
（ａ－３）三菱エンジニアリングプラスチックス（株）製「ノバデュラン（登録商標）５５１０Ｓ」、ポリブチレンテレフタレート樹脂、熱変形温度（融点）２１９℃
＜難燃剤＞
（ｂ－１）大八化学工業（株）製　「ＰＸ－２００」、芳香族縮合リン酸エステル系難燃剤、１，３－フェニレンビス（ジ－２，６－キシレニルホスフェート）
［実施例１～１０、比較例１～４］
＜樹脂ペレットの製造＞
　ポリカーボネート樹脂組成物のコンパウンド化には、１ベントを備えた日本製鋼所社製二軸押出機ＴＥＸ３０α（Ｃ１８ブロック）を用いた。そして、スクリュー回転数２００ｒｐｍ、吐出量２０ｋｇ／時間、バレル温度２７０℃の条件で各成分を混練し、ストランド状に押出した溶融樹脂を水槽にて急冷し、ペレタイザーを用いてペレット化してポリカーボネート樹脂組成物のコンパウンドを得た。
＜熱可塑性樹脂フィルム（Ａ）＞
　バレル直径３２ｍｍ、スクリューのＬ／Ｄ＝３５の二軸押出機からなるＴダイ溶融押出機を用い、吐出量２０ｋｇ／ｈ、スクリュー回転数２００ｒｐｍで幅４００ｍｍのシートを成形した。シリンダー・ダイヘッド温度の設定は、ポリカーボネートは２６０℃、ポリブチレンテレフタレートは２３５℃で行った。フィルムの表面は、一方が鏡面、もう一方には表面粗さＲａ＝１．５μｍのマット形状が転写されたものを用いた。フィルム厚みは表１に示したものを用いた。超音波溶着試験に用いたフィルムの大きさは、図３に示した熱可塑性樹脂成形品（Ｂ）を覆うため１５０ｍｍ×４０ｍｍにカットしたものを用いた。
＜熱可塑性樹脂成形品（Ｂ）＞
　表１に記載した組成品の１５０ｍｍ×１００ｍｍ×１．２ｍｍ厚平板の樹脂プレートを射出成形で成形した。得られた射出成形品を切削加工することによって、図３に示す寸法、及び図１に概略的に示した形状の溶着代（ＥＤ、エネルギータイレクター）（Ｃ）２４を有する熱可塑性樹脂成形品（Ｂ）２０を製造した。なお、図３及び４中の符号とは異なる数値は、各部材の寸法（ｍｍ）を示す。これらの数値は、各部材の寸法の一例であり、各部材の寸法を限定するものではない。
＜積層体を備えた樹脂成形品＞
　上述の熱可塑性樹脂成形品（Ｂ）２０と、熱可塑性樹脂フィルム（Ａ）１０とが一体となった溶着代一体型熱可塑性樹脂成形品を作製した。溶着代（ＥＤ、エネルギータイレクター）（Ｃ）の高さは、表１に示す０．１～０．４ｍｍの値とした。そして図３に示す形状を有する熱可塑性樹脂成形品（Ｂ）２０を用いて、熱可塑性樹脂フィルムが２つの開口部２０Ｈを完全に覆うように、熱可塑性樹脂フィルム１０と熱可塑性樹脂成形品２０とを溶着させた。熱可塑性樹脂成形品（Ｂ）２０の厚さは１．０ｍｍ、縦及び横の長さはそれぞれ４．０ｃｍ及び１５．０ｃｍであり、各開口部２０Ｈの縦及び横の長さはそれぞれ１．０ｃｍ及び１２．５ｃｍであり、各開口部２０Ｈの面積は１２．５ｃｍ２であった（図３参照）。そして、熱可塑性樹脂成形品（Ｂ）２０の溶着面２０Ｓ上に、開口部２０Ｈの周囲を囲むように、溶着代（Ｃ）２４を破線で示された位置に設けた。図４において、図３に示す溶着面２０Ｓの領域Ｉ及びＩＩを拡大して示す。
　このように、開口部２０Ｈの実質的に全周を囲むように溶着代（Ｃ）２４を設けて超音波溶着を行うことにより、熱可塑性樹脂フィルム（Ａ）１０を、熱可塑性樹脂成形品（Ｂ）２０に対して強固に固定することができる。なお、溶着面２０Ｓの領域Ｉにおいて、溶着代（Ｃ）２４の途切れている領域２０Ｄを設けることにより（図４参照）、溶着代を設ける加工が容易になる。
Figure JPOXMLDOC01-appb-T000001
＜インモールドフィルム成形＞
　成形品開口部を覆うフィルムのたわみ状態について、超音波溶着品とインモールドフィルムによる射出成形品との比較を行うため、インモールドフィルムによる射出成形品を成形した。あらかじめ超音波溶着用成形品と同寸法（１５０×４０ｍｍ）のポリカーボネート樹脂フィルムを金型内に設置、超音波溶着用金型の溶着代（Ｃ）の彫込がない金型にてポリカーボネート樹脂の射出成形を行った。以下の成形条件、すなわち、シリンダー温度３２０℃、金型温度９５℃の条件で成形した。インモールドフィルム成形で得られた結果を比較例４に示す。
Figure JPOXMLDOC01-appb-T000002
＜超音波溶着方法＞
　超音波溶着は、日本エマソン社製のＢｒａｎｓｏｎ　２０００Ｘｄｔ（２０ｋＨｚ　２２００Ｗ）を用い、成形品形状に合ったチタン合金製の溶着ホーンを使用した。溶着試験は熱可塑性樹脂フィルム（Ａ）の鏡面側と熱可塑性樹脂成形品（Ｂ）の溶着代が形成されている面とで行い、熱可塑性樹脂成形品（Ｂ）を上部ホーン側、熱可塑性樹脂フィルム（Ａ）を下部ホーン受け台に固定し溶着試験を行った。熱可塑性樹脂フィルム（Ａ）のマット柄の保護のため、フィルムに厚さ０．０３ｍｍのポリエチレン製の保護フィルムを接触させて試験を行った。超音波溶着試験におけるパラメータの設定は以下の通りである。すなわち、照射時間０．３ｓｅｃ（ポリブチレンテレフタレート樹脂では０．４５ｓｅｃ）、ホールド時間０．３ｓｅｃ、エアーシリンダ圧力２００ｋＰａ、トリガーフォース２５０Ｎ、及び振幅１００％の条件で超音波溶着試験を実施した。
　上記実施例１～１０においては、溶着強度、フィルムの外観及び形状のいずれもが良好以上であったのに対し、比較例１～４においては、少なくともいずれかの評価項目において実施例よりも劣る結果となった。以上より、熱可塑性樹脂成形品の溶着面に適当な大きさの溶着代を設け、熱可塑性樹脂フィルムと熱可塑性樹脂成形品を形成する樹脂の熱変形温度の差が小さくなるように調整した超音波溶着により、インモールド成形によるものよりも高い溶着強度及び優れた外観を有する積層体を製造できることが確認された。
１０　熱可塑性樹脂フィルム
１０Ｔ　熱可塑性樹フィルムの厚み
２０　熱可塑性樹脂成形品
２０Ｈ　開口部
２０Ｓ　溶着面
２４　溶着代
２４Ｈ　溶着代の高さ

Claims (5)

  1. 　厚み０．４ｍｍ以下の熱可塑性樹脂フィルム（Ａ）と、溶着代（Ｃ）を有する厚み０．５ｍｍ以上の熱可塑性樹脂成形品（Ｂ）の前記溶着代（Ｃ）とを超音波溶着して得られる熱可塑性樹脂積層体であって、
    　該溶着代（Ｃ）の高さが該熱可塑性樹脂フィルム（Ａ）の厚みの７２～１３０％であり、
    　前記熱可塑性樹脂フィルム（Ａ）と前記熱可塑性樹脂成形品（Ｂ）の熱変形温度の差が２０℃以下である熱可塑性樹脂フィルム積層体。
  2. 　前記熱可塑性樹脂フィルム（Ａ）と前記熱可塑性樹脂成形品（Ｂ）とが同種の樹脂材料で形成されている請求項１に記載の熱可塑性樹脂フィルム積層体。
  3. 　前記熱可塑性樹脂フィルム（Ａ）の厚みが０．２ｍｍ～０．３ｍｍである、請求項１又は２のいずれかに記載の熱可塑性樹脂フィルム積層体。
  4. 　前記熱可塑性樹脂成形品（Ｂ）が、３ｃｍ２以上の開口部を少なくとも１つ以上有し、前記開口部の少なくとも一部を前記熱可塑性樹脂フィルム（Ａ）が覆っている請求項１～３のいずれか一項に記載の熱可塑性樹脂フィルム積層体。
  5. 　請求項１～４のいずれか一項に記載の熱可塑性樹脂フィルム積層体を含有する成形品。
     
     
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