JP5788978B2 - 連続繊維と長い繊維を含む熱可塑性プリプレグ - Google Patents
連続繊維と長い繊維を含む熱可塑性プリプレグ Download PDFInfo
- Publication number
- JP5788978B2 JP5788978B2 JP2013516736A JP2013516736A JP5788978B2 JP 5788978 B2 JP5788978 B2 JP 5788978B2 JP 2013516736 A JP2013516736 A JP 2013516736A JP 2013516736 A JP2013516736 A JP 2013516736A JP 5788978 B2 JP5788978 B2 JP 5788978B2
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- Prior art keywords
- prepreg
- thermoplastic
- fibers
- continuous
- long fibers
- 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.)
- Expired - Fee Related
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Images
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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Landscapes
- Engineering & Computer Science (AREA)
- Mechanical Engineering (AREA)
- Chemical & Material Sciences (AREA)
- Composite Materials (AREA)
- Physics & Mathematics (AREA)
- Thermal Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Materials Engineering (AREA)
- Health & Medical Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Medicinal Chemistry (AREA)
- Polymers & Plastics (AREA)
- Organic Chemistry (AREA)
- Reinforced Plastic Materials (AREA)
- Moulding By Coating Moulds (AREA)
Description
[0001]本出願は仮特許出願61/357301号(2010年6月22日提出)の優先権を主張し、その内容の全てが参考文献としてここに取り込まれる。
I.連続繊維
[0026]「連続繊維」という用語は、繊維、フィラメント、糸、またはロービング(例えば、繊維の束)であって、部材の長さだけによって概ね限定される長さを有するものを指す。例えば、そのような繊維は約25ミリメートルを超える長さを有し、ある態様においては約50ミリメートル以上であり、またある態様においては約100ミリメートル以上である。連続繊維は当分野で知られたあらゆる慣用の材料から形成されてもよく、それには例えば、金属繊維、ガラス繊維(例えば、Eガラス、Aガラス、Cガラス、Dガラス、ARガラス、Rガラス、S1ガラス、S2ガラス)、炭素繊維(例えば、黒鉛)ホウ素繊維、セラミック繊維(例えば、アルミナまたはシリカ)、アラミド繊維(例えば、E. I. duPont de Nemours(デラウェア州、ウィルミントン)によって市販されているケブラー(Kevlar)(登録商標))、合成有機繊維(例えば、ポリアミド、ポリエチレン、パラフェニレン、テレフタルアミド、ポリエチレンテレフタレートおよびポリフェニレンスルフィド)、および熱可塑性樹脂配合物を強化するものとして知られているその他の様々な天然または合成の無機繊維材料または有機繊維材料がある。ガラス繊維と炭素繊維は連続繊維において用いるのに特に望ましい。このような繊維は約4〜約35マイクロメートルの公称直径を有することが多く、ある態様においては約9〜約35マイクロメートルである。繊維は撚られていても、あるいは真っ直ぐなものであってもよい。所望により、繊維は単一の繊維タイプの繊維または異なるタイプの繊維を含むロービング(例えば、繊維の束)の形態のものであってもよい。異なる繊維が個々のロービングの中に含まれていてもよく、あるいは各々のロービングが異なる繊維タイプを含んでいてもよい。例えば、一つの態様において、特定のロービングが連続炭素繊維を含んでいて、一方、他のロービングがガラス繊維を含んでいてもよい。各々のロービングの中に含まれる繊維の数は一定であっても、あるいはロービングどうしで異なっていてもよい。典型的に、ロービングは約1000本〜約50000本の個々の繊維を含んでいてもよく、ある態様においては約2000本〜約40000本の繊維を含んでいてもよい。
II.長い繊維
[0027]「長い繊維」という用語は一般に、連続していない繊維、フィラメント、糸、またはロービングであって、約0.5〜約25ミリメートルの長さを有するものを指し、ある態様においては約0.8〜約15ミリメートル、またある態様においては約1〜約12ミリメートルである。長い繊維は、連続繊維について上で説明したいずれの材料、形状、および/またはサイズのものから形成されていてもよい。ガラス繊維と炭素繊維は長い繊維として用いるのに特に望ましい。
III.熱可塑性のマトリックス
[0028]中に連続繊維と長い繊維が埋め込まれる熱可塑性樹脂のマトリックスを形成するために、任意の様々な熱可塑性ポリマーを用いることができる。本発明において用いるのに適当な熱可塑性ポリマーとしては、例えば、ポリオレフィン(例えば、ポリプロピレン、プロピレン−エチレンコポリマーなど)、ポリエステル(例えば、ポリブチレンテレフタレート(PBT))、ポリカーボネート、ポリアミド(例えば、ナイロン(商標))、ポリエーテルケトン(例えば、ポリエーテルエーテルケトン(PEEK))、ポリエーテルイミド、ポリアリーレンケトン(例えば、ポリフェニレンジケトン(PPDK))、液晶ポリマー、ポリアリーレンスルフィド(例えば、ポリフェニレンスルフィド(PPS))、フルオロポリマー(例えば、ポリテトラフルオロエチレン−ペルフルオロメチルビニルエーテルポリマー、ペルフルオロ−アルコキシアルカンポリマー、ペトラフルオロエチレンポリマー、エチレン−テトラフルオロエチレンポリマーなど)、ポリアセタール、ポリウレタン、ポリカーボネート、スチレン系ポリマー(例えば、アクリロニトリルブタジエンスチレン(ABS))などがある。ABSは特に適当な熱可塑性ポリマーである。
IV.プリプレグの形成
[0030]上で述べたように、プリプレグは概して、長い繊維をランダムに配置することのできる方法で形成される。これは様々なやり方で達成できるだろう。例えば、一つの特定の態様において、長い繊維を含む熱可塑性樹脂のペレットを押出し装置のホッパーに供給し、次いで、連続繊維と溶融混合する。押出しプロセスの圧力と力により、得られるプリプレグの中での長い繊維の所望のランダムな配向が生じる。図1を参照すると、例えば、そのような押出し装置の一態様が示されている。詳細には、装置は、バレル122の内部に取り付けられたスクリューシャフト124を含む押出し機120を有する。ヒーター130(例えば、抵抗加熱ヒーター)がバレル122の外側に取り付けられている。使用する間、熱可塑性ポリマーの供給原料127がホッパー126を通して押出し機120に供給される。この特定の態様において、供給原料127は長い繊維も含んでいる。例えば、長い繊維は供給原料の約5重量%から約60重量%を構成していてもよく、ある態様においては約10重量%から約50重量%、またある態様においては約20重量%から約40重量%を構成している。あるいは、供給原料127は長い繊維を含んでいなくてもよく、そのような繊維は、例えばホッパー126よりも下流および/または他の供給口のような、別の位置(図示せず)において供給されてもよい。
Vf=100×(ρt−ρc)/ρt
ここで、
Vfはパーセントでの気孔率;
ρcは複合材料の密度であり、液体比重壜または気体比重壜(例えば、ヘリウム比重壜)を用いるもののような公知の技術を用いて測定される;
ρtは複合材料の理論密度であり、次の式によって決定される;
ρt=1/[Wf/ρf+Wm/ρm]
ρmは(例えば、適当な結晶化度における)熱可塑性樹脂マトリックスの密度;
ρfは繊維の密度;
Wfは繊維の重量分率;そして
Wmは熱可塑性樹脂マトリックスの重量分率である。
本発明の具体的態様は以下のとおりである。
[1]熱可塑性プリプレグであって、このプリプレグは:
実質的に縦方向に配向している複数の連続繊維、ここで、この連続繊維はプリプレグの約10重量%から約80重量%を構成している;
複数のランダムに配置された長い繊維、ここで、長い繊維の少なくとも一部は縦方向に対してある角度で配向していて、長い繊維はプリプレグの約2重量%から約35重量%を構成している;および
1種以上の熱可塑性ポリマーを含んでいて、中に連続繊維と長い繊維が埋め込まれている樹脂製のマトリックス、ここで、熱可塑性ポリマーはプリプレグの約10重量%から約80重量%を構成している;
を含み、横断方向におけるプリプレグの最大引張り応力に対する縦方向におけるプリプレグの最大引張り応力の比は約1から約40である、前記熱可塑性プリプレグ。
[2]横断方向におけるプリプレグの最大引張り応力に対する縦方向におけるプリプレグの最大引張り応力の比は約2から約30である、[1]に記載の熱可塑性プリプレグ。
[3]プリプレグは縦方向において約250から約3000メガパスカルの最大引張り応力を示す、[1]に記載の熱可塑性プリプレグ。
[4]プリプレグは横断方向において約0.5から約50メガパスカルの最大引張り応力を示す、[1]に記載の熱可塑性プリプレグ。
[5]連続繊維はプリプレグの約20重量%から約70重量%を構成している、[1]に記載の熱可塑性プリプレグ。
[6]長い繊維はプリプレグの約5重量%から約30重量%を構成している、[1]に記載の熱可塑性プリプレグ。
[7]連続繊維、長い繊維、またはこれら両者は、ガラス繊維、炭素繊維、またはガラス繊維と炭素繊維の組み合わせを含む、[1]に記載の熱可塑性プリプレグ。
[8]熱可塑性ポリマーには、ポリオレフィン、ポリエーテルケトン、ポリエーテルイミド、ポリアリーレンケトン、液晶ポリマー、ポリアリーレンスルフィド、フルオロポリマー、ポリアセタール、ポリウレタン、ポリカーボネート、スチレン系ポリマー、ポリエステル、ポリアミド、またはこれらの組み合わせが含まれる、[1]に記載の熱可塑性プリプレグ。
[9]プリプレグは約2%以下の気孔率を有する、[1]に記載の熱可塑性プリプレグ。
[10]長い繊維は連続繊維と混合されている、[1]に記載の熱可塑性プリプレグ。
[11]長い繊維はプリプレグの第一の層の中に存在し、そして連続繊維はプリプレグの第二の層の中に存在する、[1]に記載の熱可塑性プリプレグ。
[12]長い繊維の少なくとも一部は第二の層の中へ延びている、[11]に記載の熱可塑性プリプレグ。
[13][1]に記載のプリプレグを含む線状の形材。
[14]形材は、形材の表面を画定しているキャッピング層をさらに含む、[13]に記載の線状の形材。
[15][1]に記載のプリプレグを含む成形品。
[16]熱可塑性プリプレグを形成するための方法であって:
連続繊維と長い繊維を押出し装置に供給すること;
熱可塑性の供給原料を押出し装置に供給すること、このとき、その供給原料は少なくとも1種の熱可塑性ポリマーを含む;および
連続繊維と長い繊維と熱可塑性ポリマーを含浸用ダイの中で押し出すことによって押出し物を形成すること、このとき、この押出し物において連続繊維は長い繊維と混合され、そして熱可塑性ポリマーのマトリックスの中に埋め込まれる;
を含む、前記方法。
[17]供給原料は長い繊維を含む、[16]に記載の方法。
[18]ロールの間に画定されるニップを通して押出し物を引っ張り、それにより押出し物をシートの形に団結させることをさらに含む、[16]に記載の方法。
[19]連続繊維はプリプレグの約10重量%から約80重量%を構成していて、長い繊維はプリプレグの約2重量%から約35重量%を構成している、[16]に記載の方法。
[20]連続繊維、長い繊維、またはこれら両者は、ガラス繊維、炭素繊維、またはガラス繊維と炭素繊維の組み合わせを含む、[16]に記載の方法。
[21]熱可塑性ポリマーには、ポリオレフィン、ポリエーテルケトン、ポリエーテルイミド、ポリアリーレンケトン、液晶ポリマー、ポリアリーレンスルフィド、フルオロポリマー、ポリアセタール、ポリウレタン、ポリカーボネート、スチレン系ポリマー、ポリエステル、ポリアミド、またはこれらの組み合わせが含まれる、[16]に記載の方法。
[22]熱可塑性の供給原料を押出し装置にマニホールドアセンブリーによって供給し、このマニホールドアセンブリーは、熱可塑性の供給原料が流れる枝分れしたランナーを有する、[16]に記載の方法。
[23]熱可塑性プリプレグを形成するための方法であって:
連続繊維を押出し装置に供給すること;
熱可塑性の供給原料を押出し装置に供給すること、このとき、その供給原料は少なくとも1種の熱可塑性ポリマーを含む;
連続繊維と供給原料を含浸用ダイの中で押し出すことによって押出し物を形成すること、このとき、この押出し物において連続繊維は熱可塑性ポリマーのマトリックスの中に埋め込まれる;
次いで、長い繊維を押出し物に付与することによって複合材料を形成すること;
を含む、前記方法。
[24]ロールの間に画定されるニップを通して複合材料を引っ張り、それにより複合材料をシートの形に団結させることをさらに含む、[23]に記載の方法。
[25]連続繊維はプリプレグの約10重量%から約80重量%を構成していて、長い繊維はプリプレグの約2重量%から約35重量%を構成している、[23]に記載の方法。
[26]連続繊維、長い繊維、またはこれら両者は、ガラス繊維、炭素繊維、またはガラス繊維と炭素繊維の組み合わせを含む、[23]に記載の方法。
[27]熱可塑性ポリマーには、ポリオレフィン、ポリエーテルケトン、ポリエーテルイミド、ポリアリーレンケトン、液晶ポリマー、ポリアリーレンスルフィド、フルオロポリマー、ポリアセタール、ポリウレタン、ポリカーボネート、スチレン系ポリマー、ポリエステル、ポリアミド、またはこれらの組み合わせが含まれる、[23]に記載の方法。
[28]熱可塑性の供給原料を押出し装置にマニホールドアセンブリーによって供給し、このマニホールドアセンブリーは、熱可塑性の供給原料が流れる枝分れしたランナーを有する、[23]に記載の方法。
Claims (18)
- 熱可塑性プリプレグであって、このプリプレグは:
実質的に縦方向に配向している複数の連続繊維、ここで、この連続繊維はプリプレグの約10重量%から約80重量%を構成している;
複数のランダムに配置された長い繊維、ここで、長い繊維の少なくとも一部は縦方向に対してある角度で配向していて、長い繊維はプリプレグの約2重量%から約35重量%を構成している;および
1種以上の熱可塑性ポリマーを含んでいて、中に連続繊維と長い繊維が埋め込まれている樹脂製のマトリックス、ここで、熱可塑性ポリマーはプリプレグの約10重量%から約80重量%を構成している;
を含み、
横断方向におけるプリプレグの最大引張り応力に対する縦方向におけるプリプレグの最大引張り応力の比は約1から約40であり;
長い繊維はプリプレグの第一の層の中に存在し、連続繊維はプリプレグの第二の層の中に存在し、そして、長い繊維の少なくとも一部は第二の層の中へ延びている、
前記熱可塑性プリプレグ。 - 横断方向におけるプリプレグの最大引張り応力に対する縦方向におけるプリプレグの最大引張り応力の比は約2から約30である、請求項1に記載の熱可塑性プリプレグ。
- プリプレグは縦方向において約250から約3000メガパスカルの最大引張り応力を示す、請求項1に記載の熱可塑性プリプレグ。
- プリプレグは横断方向において約0.5から約50メガパスカルの最大引張り応力を示す、請求項1に記載の熱可塑性プリプレグ。
- 連続繊維はプリプレグの約20重量%から約70重量%を構成している、請求項1に記載の熱可塑性プリプレグ。
- 長い繊維はプリプレグの約5重量%から約30重量%を構成している、請求項1に記載の熱可塑性プリプレグ。
- 連続繊維、長い繊維、またはこれら両者は、ガラス繊維、炭素繊維、またはガラス繊維と炭素繊維の組み合わせを含む、請求項1に記載の熱可塑性プリプレグ。
- 熱可塑性ポリマーには、ポリオレフィン、ポリエーテルケトン、ポリエーテルイミド、ポリアリーレンケトン、液晶ポリマー、ポリアリーレンスルフィド、フルオロポリマー、ポリアセタール、ポリウレタン、ポリカーボネート、スチレン系ポリマー、ポリエステル、ポリアミド、またはこれらの組み合わせが含まれる、請求項1に記載の熱可塑性プリプレグ。
- プリプレグは約2%以下の気孔率を有する、請求項1に記載の熱可塑性プリプレグ。
- 請求項1に記載のプリプレグを含む線状の形材。
- 形材は、形材の表面を画定しているキャッピング層をさらに含む、請求項10に記載の線状の形材。
- 請求項1に記載のプリプレグを含む成形品。
- 熱可塑性プリプレグを形成するための方法であって:
連続繊維を押出し装置に供給すること;
熱可塑性の供給原料を押出し装置に供給すること、このとき、その供給原料は少なくとも1種の熱可塑性ポリマーを含む;
連続繊維と供給原料を含浸用ダイの中で押し出すことによって押出し物を形成すること、このとき、この押出し物において連続繊維は熱可塑性ポリマーのマトリックスの中に埋め込まれる;
次いで、長い繊維を押出し物に付与することによって複合材料を形成すること;
を含み、
長い繊維はプリプレグの第一の層の中に存在し、連続繊維はプリプレグの第二の層の中に存在し、そして、長い繊維の少なくとも一部は第二の層の中へ延びている、
前記方法。 - ロールの間に画定されるニップを通して複合材料を引っ張り、それにより複合材料をシートの形に団結させることをさらに含む、請求項13に記載の方法。
- 連続繊維はプリプレグの約10重量%から約80重量%を構成していて、長い繊維はプリプレグの約2重量%から約35重量%を構成している、請求項13に記載の方法。
- 連続繊維、長い繊維、またはこれら両者は、ガラス繊維、炭素繊維、またはガラス繊維と炭素繊維の組み合わせを含む、請求項13に記載の方法。
- 熱可塑性ポリマーには、ポリオレフィン、ポリエーテルケトン、ポリエーテルイミド、ポリアリーレンケトン、液晶ポリマー、ポリアリーレンスルフィド、フルオロポリマー、ポリアセタール、ポリウレタン、ポリカーボネート、スチレン系ポリマー、ポリエステル、ポリアミド、またはこれらの組み合わせが含まれる、請求項13に記載の方法。
- 熱可塑性の供給原料を押出し装置にマニホールドアセンブリーによって供給し、このマニホールドアセンブリーは、熱可塑性の供給原料が流れる枝分れしたランナーを有する、請求項13に記載の方法。
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2011
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- 2011-06-22 CN CN201180029246.6A patent/CN102947076B/zh not_active Expired - Fee Related
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- 2011-06-22 US US13/698,382 patent/US9096000B2/en active Active
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Also Published As
Publication number | Publication date |
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JP2013531717A (ja) | 2013-08-08 |
CN102947076B (zh) | 2016-01-27 |
WO2011163365A2 (en) | 2011-12-29 |
BR112012033036A2 (pt) | 2016-12-20 |
EP2585279B8 (en) | 2016-07-27 |
RU2013102590A (ru) | 2014-07-27 |
MX2012014179A (es) | 2013-02-21 |
US9096000B2 (en) | 2015-08-04 |
RU2573674C2 (ru) | 2016-01-27 |
CN102947076A (zh) | 2013-02-27 |
US20150298400A1 (en) | 2015-10-22 |
EP2585279B1 (en) | 2016-06-08 |
KR20130088034A (ko) | 2013-08-07 |
CA2801081A1 (en) | 2011-12-29 |
US20130136890A1 (en) | 2013-05-30 |
EP2585279A2 (en) | 2013-05-01 |
WO2011163365A3 (en) | 2012-02-16 |
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