TW202030236A - 具有熱塑性基質之複合物 - Google Patents
具有熱塑性基質之複合物 Download PDFInfo
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- TW202030236A TW202030236A TW108133604A TW108133604A TW202030236A TW 202030236 A TW202030236 A TW 202030236A TW 108133604 A TW108133604 A TW 108133604A TW 108133604 A TW108133604 A TW 108133604A TW 202030236 A TW202030236 A TW 202030236A
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Classifications
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- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L27/00—Compositions of homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by a halogen; Compositions of derivatives of such polymers
- C08L27/02—Compositions of homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by a halogen; Compositions of derivatives of such polymers not modified by chemical after-treatment
- C08L27/12—Compositions of homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by a halogen; Compositions of derivatives of such polymers not modified by chemical after-treatment containing fluorine atoms
- C08L27/16—Homopolymers or copolymers or vinylidene fluoride
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- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/06—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material
- B32B27/08—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/18—Layered products comprising a layer of synthetic resin characterised by the use of special additives
- B32B27/20—Layered products comprising a layer of synthetic resin characterised by the use of special additives using fillers, pigments, thixotroping agents
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/30—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers
- B32B27/304—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers comprising vinyl halide (co)polymers, e.g. PVC, PVDC, PVF, PVDF
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/30—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers
- B32B27/308—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers comprising acrylic (co)polymers
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/34—Layered products comprising a layer of synthetic resin comprising polyamides
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
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Abstract
本發明係關於具有改質PVDF的基質之連續纖維強化複合物。該複合物可為半成品或產品或由其製造的製成零件。根據本發明之產物為粒狀長纖維材料,而根據本發明的製成零件尤其是熱塑性複合物管。
Description
本發明係關於具有改質PVDF的基質之連續纖維強化複合物。該複合物可為半成品或產品或由其製造的製成零件。根據本發明之產物為粒狀長纖維材料,而根據本發明的製成零件尤其是熱塑性複合物管。
具有PVDF基質之複合物為已知的;具有玻璃纖維或碳纖維強化材料的對應類型為市售。然而,纖維與PVDF基質之間的黏著不令人滿意,其導致不足的機械性能。另一個缺點為在複合物和複合物中包括的組分之間不能達到直接黏著。US 2011/0166278和WO 2016/142630描述具有PVDF基質的複合物,其係藉由製備PVDF和不飽和單體的混合物,用高能輻射對其進行照射及接著除去不飽和單體的未反應部分來製造。然而,此製備模式不方便且昂貴及不能容易地轉化為生產規模。
基本問題之一態樣在於提供更容易製造的具有PVDF基質和良好纖維-基質黏著的複合物。
由於PVDF的阻燃作用,此種複合物非常受關注,例如用於飛機或機動車輛結構。彼等用作熱塑性複合物管(TCP)中的強化層也特別受關注,因為彼等從環境或所輸送的介質中所吸收之烴、水或甲醇比具有聚醯胺基質之複合物少,且在該等物質的存在下特別是也可承受較高的熱應力。相較於具有聚烯烴基質之複合物,情況也類似。
撓性熱塑性複合物管至少由熱塑性聚合物的內襯墊管、施加至其上的已浸漬有熱塑性基質之連續纖維膠帶的多層纏繞層、以及熱塑性材料的外保護層所組成。若這些層彼此黏結地黏合,則此也稱為黏合複合物撓性管。該等管通常用於離岸石油生產。尤其是使用於大水深處,且也用於將該等管可靠地連接至各個連接元件(例如端部配件)以及用於組裝和鋪設操作,將所述層全部彼此黏結性黏合是非常有利的。
TCP係描述例如於WO 1995/007428和WO 1999/067561中。其製造係另外揭示於WO 2002/095281、WO 2006/ 107196、WO 2012/118378、WO 2012/118379和WO 2013/ 188644中。在現有的TCP中,內襯墊管的材料(或在多層襯墊的情況下為外襯墊層的材料),膠帶的基質材料和外保護層的材料(“外套”或“覆蓋片”)通常由相同的聚合物組成,以便因此能夠達到纏繞層彼此之間以及與襯墊和保護層之很好的融合和黏著。取決於最高使用溫度和應用,這些通常為基於聚乙烯、聚丙烯或PA12/PA11之TCP。在低使用溫度(例如低於50℃)下,通常使用聚烯烴,及上述PA11或PA12。在要引導的流體之溫度超過80℃的應用中,在高達約135℃的溫度下通常使用PVDF均聚物或PVDF共聚物作為襯墊。若使用聚合物內層的限制不是由操作溫度而是由聚合物的化學穩定性引起的,則只有對流體穩定的薄內保護層通常就足以作為襯墊,其同樣可由PVDF均-或共聚物組成。
在目前正在開發的TCP中,較佳地使用PA12或PEEK的單層襯墊,且具有相同聚合物之基質的玻璃或碳纖維膠帶與此等組合。然而,由於其特殊性質以及由於高材料成本,PEEK僅使用在對熱和化學穩定性有極高要求的地方。在中等溫度範圍內,使用由PVDF或PA12組成的襯墊以及具有PA12基質的膠帶。然而,PA12膠帶不容易以必要的黏合力黏著至PVDF襯墊。此問題可藉由製造例如具有PVDF內層、助黏著劑層和PA12外層的多層襯墊來解決。然而,在該類結構的情況下,產生三層界面(PVDF/助黏著劑、助黏著劑/PA12、PA12/膠帶),彼等在極端操作條件下會成為弱點(參見,尤其,DNV-GL Recommended Practice RP F119 “Thermoplastic Composite Pipes”)。目標因此必須為將在該類TCP中的關鍵層界面之數目減至最少。
基本問題的另一態樣因此在於提供一種熱塑性複合物管,其具有與易於製造的具有PVDF基質和良好纖維-基質黏著的複合物之一或多層強化層的最少層界面。
根據本發明之複合物、包含根根據本發明之複合物的根據本發明之成形體(例如熱塑性複合物管(TCP)、及根據本發明之用途以舉例的方式描述在下文中,而無意將本發明限於此等說明性實施例中。當化合物之範圍、通式或類別指定於下文時,此等意欲不僅涵蓋明確提及的化合物之對應範圍或群組,而且也包括可省略各個值(範圍)或化合物而獲得之化合物的所有子範圍和子群組。在本說明書的上下文中引用文件的情況下,其全部內容意欲作為本發明揭示的一部分。除非另有說明,否則在下文中給出百分比數字時,這些數字均為重量百分比。在組成物的情況下,除非另有說明,否則百分比數字以整體組成物為基準計。在下文中給出平均值的情況下,除非另有說明,否則此等為質量平均值(重量平均值)。在下文中給出測量值的情況下,除非另有說明,否則此等測量值係在101 325 Pa的壓力和25℃的溫度下測定。
藉由本申請案之標的解決基本問題之第一態樣,本申請案之標的為一種複合物,其由聚合物基質和嵌入其中的連續纖維組成,
其中該聚合物基質組成至少80重量%的程度,較佳為至少85重量%的程度,更佳為至少90重量%的程度及尤佳為至少95重量%的程度之包含下列成分的混合物:
a) 作為主成分之低黏度PVDF,即達到至少50重量份的程度,及
b) 1至50重量份,較佳為1.5至40重量份,更佳為2至30重量份,特佳為2.5至20重量份及尤佳為3至10重量份的丙烯酸酯共聚物,其中該丙烯酸酯共聚物含有1重量%至30重量%,較佳為2重量%至25重量%,更佳為4重量%至20重量%及尤佳為5重量%至15重量%的具有羧酸酐單元之單元,
其中a)和b)的重量份之總和為100,及
其中複合物中連續纖維的體積比例另外為10%至80%,較佳為15%至75%,更佳為20%至70%,甚至更佳為25%至65%,特佳為30%至60%,及尤佳為35%至55%;
其中聚合物基質的百分比和連續纖維的百分比各自以複合物的總質量或總體積為基準計。
EP 0673762A2 (US 5554426A)揭示PVDF和丙烯酸酯共聚物為相容的且彼此均勻地互溶的,並且呈摻合物、對聚醯胺層具有良好的黏著性。其中也提及可使此模塑料(moulding compound)導電,特別是藉由添加炭黑、碳纖維等等。導電添加劑不用於強化;在實施例中僅使用炭黑。沒有纖維-基質黏著之揭示。EP 0673762A2中所討論的層因此不為就本發明意義而言之複合物。
根據本發明之複合物為纖維複合物材料,其可為半成品之形式,或由其製造的製成零件。製造後直接的半成品為可具有任何所需幾何形狀的股形式。其可為例如片、膠帶、板、圓形輪廓、矩形輪廓或複雜輪廓。
連續纖維為具有大於50 mm之長度者。通常,彼等明顯更長。在本發明的情況下,彼等係以粗紗或編織的形式使用。原則上,適當纖維為具有足夠長度的所有纖維,其具有高於約250℃的基質模塑料之加工溫度的軟化溫度和熱穩定性;可能使用無機纖維、聚合物纖維和天然纖維,以及彼此的組合。適當纖維的實例為金屬纖維、玻璃纖維(較佳為S1玻璃、S2玻璃的玻璃纖維)、碳纖維、金屬化碳纖維、硼纖維、陶瓷纖維(例如Al2
O3
或SiO2
之陶瓷纖維)、玄武岩纖維、碳化矽纖維、鈦酸鉀纖維、聚芳醯胺纖維、液晶聚酯之纖維、聚丙烯腈纖維和聚合物諸如聚醯亞胺、聚醚醯亞胺、聚伸苯硫醚、聚對伸苯基苯并雙唑(PBO)、聚醚酮、聚醚醚酮等等之纖維。玻璃纖維較佳應不含任何氧化硼或二氧化鈦,因為此等可導致PVDF的自催化降解。較佳同樣排除含具有相似性質的物質之玻璃纖維。
纖維的橫截面可為例如圓形、矩形、卵形、橢圓形或繭形。直徑較佳為5 μm至25 μm。特佳者為具有5至25 mm直徑的圓形橫截面之纖維。
使用橫截面偏離圓形的纖維(例如平板玻璃纖維),可能在製成零件中達成較高的纖維填充程度,從而獲得更高的強度。市售纖維通常在彼等表面上含有膠料(size),其提供黏合至聚合物基質的官能基。為了本發明之目的,膠料可能是有幫助的,但是原則上不是必需的。較佳者為使用上膠纖維;該膠料更佳對聚合物基質具有反應性。碳纖維是較佳的;上膠碳纖維為更佳的。尤佳上膠碳纖維為其中膠料含有環氧基者。
更佳地,複合物包括以複合物為基準計為20體積%至60體積%,特佳為30體積%至55體積%及尤佳為40體積%至50體積%的碳纖維。甚至更佳地,複合物包括以複合物為基準計為30體積%至55體積%的具有環氧膠料(size)之碳纖維。
熟習該技術者已知PVDF為聚偏二氟乙烯且可以各種類型商購獲得。PVDF可為均聚物或共聚物。根據本發明,所使用之聚偏二氟乙烯可為基於偏二氟乙烯之共聚物,其包括最多40重量%的衍生自下列單體之單元:三氟乙烯、氯三氟乙烯、乙烯、丙烯和六氟丙烯。較佳地,聚偏二氟乙烯為偏二氟乙烯之均聚物。
PVDF較佳為低黏度PVDF;低黏度PVDF較佳為具有18至50克/10 min之熔體流動指數(MFI),較佳為20至45克/10 min,使用2.16 kg (230℃),及根據ASTM D1238-13測定MFI。
具有較低MFI之PVDF導致纖維材料的浸漬較差並導致聚合物基質的孔隙率增加。此外,在複合物中只能達成較小比例的纖維材料。總體而言,較低的MFI因此導致複合物的機械性質惡化。例如,利用ASTM D2344-16可測定這些性質。
丙烯酸酯共聚物b)較佳含有下列單元:
I. 14重量%至80重量%,較佳為20重量%至70重量%,更佳為30重量%至65重量%及尤佳為40重量%至60重量%的下式之酯單元
且R = 甲基、乙基、丙基或丁基,R1
= 氫或甲基;
II. 10重量%至75重量%,較佳為20重量%至65重量%,更佳為25重量%至50重量%及尤佳為30重量%至40重量%的下式之醯亞胺單元
且R4
= 獨立地具有1至8個碳原子,較佳具有1至4個碳原子的脂族或脂環族基團,更佳氫或甲基,及
R3
= 獨立地甲基、乙基、丙基、丁基或苯基;
較佳地R3
和R4
皆為甲基;
m = 0或1;
III. 1重量%至20重量%,更佳為1.5重量%至15重量%及尤佳為2重量%至5重量%的下式之酸單元
且R2
= 氫或甲基;
IV. 1重量%至30重量%,較佳為2重量%至25重量%,更佳為4重量%至20重量%及尤佳為5重量%至15重量%的下式之酸酐單元
且R5
= 獨立地具有1至8個碳原子,較佳具有1至4個碳原子的脂族或脂環族基團,更佳為氫或甲基;
n = 0或1;
其中該等單元I、II、III和IV加起來總共100重量%。
丙烯酸酯共聚物b)可另外含有其他單元,例如彼等衍生自下列者:順丁烯二酯、反丁烯二酯、衣康酯、乙酸乙烯酯、乙烯基吡咯啶酮、氯乙烯、丙烯腈、丙烯醯胺、苯乙烯或乙烯,其先決條件為此不會顯著損害與PVDF的相容性和所需的黏著促進效應。
限制取代基R1
、R2
、R4
和R5
的鏈長的原因為較長的烷基導致玻璃轉移溫度降低並因此耐熱變形性降低。此在個別情況下可能被接受;該等實施態樣至少在本發明的等效範圍內。
酯單元I衍生自例如丙烯酸甲酯、丙烯酸乙酯、丙烯酸正丁酯、甲基丙烯酸甲酯、甲基丙烯酸正丙酯或甲基丙烯酸異丁酯,較佳者為甲基丙烯酸甲酯。
醯亞胺單元II,在m = 0的情況下,衍生自隨意地經取代之順丁烯二醯亞胺類諸如順丁烯二醯亞胺、N-甲基順丁烯二醯亞胺、N-乙基順丁烯二醯亞胺、N-苯基順丁烯二醯亞胺或N-甲基檸檬烯二醯亞胺。在m = 1的情況下,彼等衍生自聚合物中相鄰的二個式I或III單元與氨或一級胺以形成醯亞胺之反應。
酸單元III衍生自丙烯酸或甲基丙烯酸。
酐單元IV(當n = 0時)較佳衍生自不飽和二羧酸酐諸如順丁烯二酐、甲基丙烯酐和丙烯酐,更佳衍生自甲基丙烯酐。在n = 1的情況下,彼等衍生自具有閉環之聚合物中二個相鄰單元III中除去水。
其他酐單元可衍生自衣康酐和鳥頭酸。
更佳地,丙烯酸酯共聚物b)僅具有單元I、II、III和IV。
較佳地,丙烯酸酯共聚物中的R1
、R2
、R4
和R5
基團全部相同,更佳全部為甲基。
由於單元II的存在,該等共聚物稱為聚丙烯醯亞胺或聚甲基丙烯醯亞胺,或者有時也稱為聚戊二醯亞胺(polyglutarimide)。此等為從其中二個相鄰的羧酸酯基已轉化成環醯亞胺(cyclic acid imide)的聚丙烯酸烷酯或聚甲基丙烯酸烷酯開始的產物。醯亞胺形成較佳在水存在下用氨或一級胺(例如甲胺)進行,同時藉由水解伴隨形成單元III和IV。
產物及其製備為已知的(Hans R. Kricheldorf, Handbook of Polymer Synthesis, Part A, Verlag Marcel Dekker Inc. New York-Basle-Hong Kong, p. 223 ff.; H. G. Elias, Makromoleküle [Macromolecules], Hüthig und Wepf Verlag Basle-Heidelberg-New York; US 2 146 209, US 4 246 374)。
丙烯酸酯共聚物較佳具有40重量%至60重量%的單元I、30重量%至40重量%的單元II、2重量%至5重量%的單元III、及5重量%至15重量%的單元IV。
該聚合物基質較佳含有低黏度PVDF和以聚合物基質為基準計為2重量%至30重量%,更佳2.5重量%至20重量%及尤佳3重量%至10重量%的丙烯酸酯共聚物,其中該丙烯酸酯共聚物包括40重量%至60重量%的單元I、30重量%至40重量%的單元II、2重量%至5重量%的單元III和5重量%至15重量%的單元IV,且單元I、II、III和IV總計100。
較佳地,在由低黏度均-PVDF和以聚合物基質為基準計為5重量%至10重量%的丙烯酸酯共聚物所組成之聚合物基質中,根據本發明之複合物包括以複合物為基準計為30體積%至55體積%的具有環氧樹脂膠料(size)之碳纖維,其中該丙烯酸酯共聚物包括40重量%至60重量%的單元I、30重量%至40重量%的單元II、2重量%至5重量%的單元III和5重量%至15重量%的單元IV,且單元I、II、III和IV總計100。
該聚合物基質除了低黏度PVDF和丙烯酸酯共聚物之外,可含有習知助劑和添加劑,例如衝擊改質劑(例如丙烯酸酯橡膠)、阻燃劑、穩定劑、塑化劑、加工助劑、染料、顏料或類似物。所述試劑的量應計量加入,以使所需的性質(尤其是關於纖維材料與基質的黏合)沒有明顯受損。
該聚合物基質係以習知和已知的方法藉由在有效捏合的混合單元(例如雙螺桿擠出機)中於依據成分的熔點之溫度(通常介於200和300℃之間)下將成分的熔體混合而製得。
根據本發明之複合物可藉由先前技技術方法製造。單向連續纖維強化帶的製造係詳細描述於例如EP 0056703A1、US 5002712A、US 4883625A、US 2014/ 0191437A1、US 2013/0333788A1和WO 2014/140025中。從粗紗或織物開始的可能製造方法為例如熔融施用、用聚合物溶液浸漬及除去溶劑、薄膜浸漬或粉末浸漬(US 2018001516A1、WO 2016/156222、WO 2016/173886)。
於適當形式的以此方式獲得之複合物可已為最終產品。在其他情況下,其為半成品,可借助於適當成形方法進一步加工而產生製成零件。說明性的製成零件為飛機、火箭或機動車輛的構造零件,或含有該類複合物作為強化層的熱塑性複合物管。
此外,複合物可能切割為股以產生具有4至60 mm,較佳為5至50 mm,特佳為6至40 mm,尤佳為5至30 mm及非常特佳為6至25 mm的長度之伸長長纖維強化粒。在此等伸長長纖維強化粒中,強化纖維沿軸向配置並從第一切割面延伸到第二切割面。
接著可利用射出成形、擠出、壓縮成形或其他熟悉的成形方法而將這些顆粒用於製造模製品,且在此以溫和的加工方法達成特別好的模製品性質。在此情況下,術語“溫和”應理解尤其意為在很大程度上避免不當的纖維斷裂和隨之而來的纖維長度之嚴重減少。在射出成形的情況下,此意味著較佳使用大直徑和低壓縮比的螺桿,以及大尺寸的(generously dimensioned)噴嘴通道和澆口通道。應確保的補充條件為借助於高筒溫(接觸加熱)伸長顆粒迅速熔融,及纖維不會因不當的剪切程度而被過度粉碎。當觀察這些測量時,所得模製品的平均纖維長度高於由短纖維強化模製組成物所製造的可比較模製品。此達成性質(特別是拉伸彈性模數、極限拉伸強度和耐缺口衝擊性)之顯著改良。
較佳半成品為膠帶;此等較佳具有已用連續纖維單向強化。較佳地,膠帶具有5至600 mm的寬度及較佳地具有8至300 mm的寬度,而厚度通常在從0.05至2 mm之範圍,較佳在從0.1至1 mm之範圍,更佳在從0.125至0.5 mm之範圍及特佳在從0.15至0.35 mm之範圍。
較佳複合物由連續纖維強化膠帶層組成,具有1至100,更佳5至90個別層之許多個別層,其中該複合物係藉由施加壓力和升高溫度,更佳藉由固結來形成,如實施例中所示,且個別層可具有任何所需的纖維取向。
本發明之另一部分標的解決基本問題之第二態樣,本發明之另一部分標的為一種熱塑性複合物管(TCP),其由內而外包括下列組件:
I. 具有一或多層的管狀襯墊,其外表面由聚醯胺模塑料(moulding compound)或PVDF模塑料組成;
II. 由複合物組成的強化層,該複合物由聚合物基質和嵌入其中的連續纖維組成,其中該聚合物基質組成至少80重量%的程度,較佳為至少85重量%的程度,更佳為至少90重量%的程度及尤佳為至少95重量%的程度之包含下列成分的混合物:
a) 作為主成分之低黏度PVDF,即達到至少50重量份的程度,及
b) 1至50重量份,較佳為1.5至40重量份,更佳為2至30重量份,特佳為2.5至20重量份及尤佳為3至10重量份的丙烯酸酯共聚物,其中該丙烯酸酯共聚物含有1重量%至30重量%,較佳為2重量%至25重量%,更佳為4重量%至20重量%及尤佳為5重量%至15重量%的具有羧酸酐基團之單元,
其中a)和b)的重量份之總和為100,
及其中複合物中連續纖維的體積比例另外為10%至80%,較佳為15%至75%,更佳為20%至70%,甚至更佳為25%至65%,特佳為30%至60%,及尤佳為35%至55%,
其中聚合物基質的百分比和連續纖維的百分比各自以強化層的總質量或總體積為基準計;
III. 隨意地由聚醯胺基質和嵌入其中的連續纖維組成之複合物的其他強化層,
其中該聚醯胺基質組成至少80重量%的程度,較佳為至少85重量%的程度,更佳為至少90重量%的程度及尤佳為至少95重量%的程度之聚醯胺,
及其中複合物中連續纖維的體積比例另外為10%至80%,較佳為15%至75%,更佳為20%至70%,甚至更佳為25%至65%,特佳為30%至60%,及尤佳為35%至55%,
其中聚醯胺基質的百分比和連續纖維的百分比各自以強化層的總質量或總體積為基準計;
IV. 隨意地由聚合物材料組成之外覆蓋層。
較佳地,層II為由如上所述的根據本發明之複合物所組成的強化層。
管狀襯墊通常具有在從10至500 mm之範圍,較佳在從12至425 mm之範圍及更佳在從15至300 mm之範圍的內直徑。其壁厚一般在從2至40 mm之範圍,較佳在從2.5至30 mm之範圍及更佳在從3至20 mm之範圍。襯墊可具有單層或多層。
在TCP的製造中,以施加接觸壓力將膠帶形式的根據本發明之複合物施加至襯墊的外表面上。必要的接觸壓力可透過繞取張力或利用接觸體來達成。在此,在一實施態樣中,例如利用紅外輻射、熱空氣、熱氣體、雷射輻射、微波輻射或直接藉由接觸加熱而在表面上將二個接觸面熔融。接著將部分熔融的接觸表面彼此壓在一起。然後應保持接觸壓力,直到熔融區固化。在另一實施態樣中,將膠帶纏繞,及接著利用可加熱的接觸體間接地或直接地從外部熔融。必須校準加熱輸出,以使襯墊在此處的外表面也開始熔融。之後,保持接觸壓力直到熔融區固化。膠帶的纏繞和任何其他膠帶層的纏繞為先前技術。隨意地可能以相同的方式將一或多層具有聚醯胺基質的膠帶層施加至由此獲得的結構上。在一些情況下,這是可取的,因為TCP的外區域較小程度暴露於要輸送的介質及其溫度且以此方式可保持較低的材料成本,並使整個管道更輕。熟習該項技術者已知聚醯胺為非常耐衝擊的聚合物並因此提供較佳和額外的保護以抵抗環境影響;此外,聚醯胺具有低於PVDF的密度。
整個複合物層,即所有膠帶層的總和,在此係在從1至100 mm之範圍,較佳在從5至90 mm之範圍及更佳在從10至80 mm之範圍。對於不同的膠帶層,可能使用不同的膠帶幾何形狀和纏繞角度。所使用的膠帶可具有任何適當的橫截面。
為了保護外膠帶層,可能隨意地最終施加聚合物材料的外覆蓋層。此為熱塑性模塑料或熱塑性或可交聯或交聯彈性體。覆蓋層較佳牢固地黏著於外膠帶層。在此情況下,覆蓋層可例如利用十字頭擠壓模施加且因此黏結地黏合於膠帶層。黏著也可藉由可交聯彈性體的交聯產生。
根據本發明之TCP的特定設計為例如:
a) 聚醯胺模塑料的襯墊/本發明PVDF複合物層/聚醯胺模塑料的覆蓋層;
b) PVDF模塑料的襯墊/本發明PVDF複合物層/PVDF模塑料的覆蓋層;
c) PVDF模塑料的襯墊/本發明PVDF複合物層/聚醯胺模塑料的覆蓋層;
d) 聚醯胺模塑料的襯墊/本發明PVDF複合物層/PVDF模塑料的覆蓋層;
e) 二層襯墊,具有聚醯胺模塑料之內層和PVDF之外層/丙烯酸酯共聚物摻合物/本發明PVDF複合物層/PVDF的層/丙烯酸酯共聚物摻合物/聚醯胺模塑料的覆蓋層;
f) 二層襯墊,具有聚醯胺模塑料之內層和PVDF之外層/丙烯酸酯共聚物摻合物/本發明PVDF複合物層/PVDF模塑料的覆蓋層;
g) PVDF或聚醯胺模塑料的襯墊/本發明PVDF複合物層/具有聚醯胺基質之複合物層/PVDF或聚醯胺模塑料的覆蓋層。
設計e和f中的丙烯酸酯共聚物在此與根據本發明之複合物的丙烯酸酯共聚物 b)具有相同的組成。
適當的聚醯胺為例如PA6、PA66、PA610、PA88、PA8、PA612、PA810、PA108、PA9、PA613、PA614、PA812、PA128、PA1010、PA10、PA814、PA148、PA1012、PA11、PA1014、PA1212和PA12、或基於此等聚醯胺之聚醚醯胺或聚醚酯醯胺,或聚酞醯胺,例如 PA66/6T、PA6/6T、PA6T/MPMDT(MPMD代表2-甲基五亞甲基二胺)、PA9T、PA10T、PA11T、PA12T、PA14T、PA6T/6I、PA6T/10T、PA6T/12、PA10T/11、PA10T/12或PA612/6T。
關於具有由根據本發明的複合物構成之強化物的根據本發明之TCP的優點在於:相較於聚烯烴或聚醯胺之基質,聚合物基質由於烴、水或甲醇的吸收而軟化之程度較小。因此,相較於由聚烯烴或聚醯胺製成之可比較的管,根據本發明之TCP具有較高的外抗壓強度。另外良好的纖維-基質黏著特別有利,其顯著有助於高強化和長壽命。纖維-基質黏著之測量可考慮為根據ASTM D2344-16之三點彎曲試驗,如實施例中所述。
根據本發明之TCP的另一優點為在根據本發明之PVDF複合物層與任何存在的聚醯胺層之間不需要額外的黏著促進。
根據本發明之TCP尤其適合於石油或天然氣生產中之離岸應用,例如用於將產物運輸到平台、用於連接鋼管、作為運輸管及尤其是作為臍狀帶(umbilical)、作為立管、作為跨接管線、作為流管線、作為介入管線、作為下管線、作為注入管線或作為壓力管線。其可用於運輸可能加壓的烴類或其混合物,諸如原油、粗煤氣(crude gas)、三相(即油/氣/水混合物)、加工油(已在海床部分處理)、加工氣、汽油或柴油、注入介質諸如水(例如以保持洞穴中的壓力)、油田化學品、甲醇或CO2
的運輸、或用於液壓油(例如用於海床的致動器)的傳導。另外,根據本發明之TCP也適合作為在陸上行業或其他工業應用中之壓力傳導管線,尤其是在彼等必須在管道和連接元件之間具有壓入配合黏合之軸管方向上傳遞較高的力者。
實施例:
從95重量%的低黏度均-PVDF(Solef 1006)與5重量%的丙烯酸酯共聚物混合製造由在聚合物基質中之45體積%的碳纖維(Grafil 34-700 D)組成之膠帶,該丙烯酸酯共聚物包括10.1重量%的酸酐(IV)、2.9重量%的酸基(III)、35重量%的醯胺基(II)和52重量%的甲基丙烯酸酯基(I),不含其他添加劑。
將上述膠帶的八個單向層固結以產生半成品後(10巴,240℃,保持時間5分鐘),發現根據ASTM D2344-16在平面試樣上測得的層間剪切強度為59 MPa。
直到指定的值為止,在試樣中都沒有觀察到基質與碳纖維的分離;此試驗因此提供關於基質與連續纖維之黏著性的陳述。
為了比較,類似於該工作例構造半成品,但是沒有使用丙烯酸酯共聚物。在可比較的半成品固結之後,發現根據ASTM D2344-16測得的層間剪切強度為17 MPa。
Claims (9)
- 一種複合物,其由聚合物基質和嵌入其中的連續纖維組成,其中該聚合物基質組成至少80重量%的程度之包含下列成分的混合物: a) 作為主成分之低黏度PVDF,即達到至少50重量份的程度,及 b) 1至50重量份的丙烯酸酯共聚物,其中該丙烯酸酯共聚物含有1重量%至30重量%的具有羧酸酐單元之單元, 其中a)和b)的重量份之總和為100,及 其中該複合物中該連續纖維的體積比例亦為10重量%至80重量%, 其中該聚合物基質的百分比和該連續纖維的百分比各自以該複合物的總質量或總體積為基準計。
- 根據請求項1之複合物,其中該PVDF為均聚物或共聚物。
- 根據前述請求項中任一項之複合物,其中該丙烯酸酯共聚物包含下列單元: I. 14重量%至80重量%的下式之酯單元 且R = 甲基、乙基、丙基或丁基,R1 = 氫或甲基; II. 10重量%至75重量%的下式之醯亞胺單元 且R4 = 獨立地具有1至8個碳原子,較佳具有1至4個碳原子的脂族或脂環族基團,更佳氫或甲基,及 R3 = 獨立地甲基、乙基、丙基、丁基或苯基; m = 0或1; III. 1重量%至20重量%的下式之酸單元 且R2 = 氫或甲基; IV. 1重量%至30重量%的下式之酸酐單元 且R5 = 獨立地具有1至8個碳原子的脂族或脂環族基團; n = 0或1; 其中該等單元I、II、III和IV加起來總共100重量%。
- 根據前述請求項中任一項之複合物,其為單向連續纖維強化帶。
- 一種具有長度為4至60 mm之伸長長纖維強化粒,其係藉由將股形式之根據前述請求項中任一項之複合物切割而製得。
- 一種熱塑性複合物管(TCP),其由內而外包括下列組件: I. 具有一或多層的管狀襯墊,其外表面由聚醯胺模塑料(moulding compound)或PVDF模塑料組成; II. 由複合物組成的強化層,該複合物由聚合物基質和嵌入其中的連續纖維組成,其中該聚合物基質組成至少80重量%的程度之包含下列成分的混合物: a) 50至99重量份的PVDF及 b) 1至50重量份的丙烯酸酯共聚物,其中該丙烯酸酯共聚物含有1重量%至30重量%的具有羧酸酐基團之單元, 其中a)和b)的重量份之總和為100,及 其中該複合物中該連續纖維的體積比例為10重量%至80重量%, 其中該聚合物基質的百分比和該連續纖維的百分比各自以該強化層的總質量或總體積為基準計; III. 隨意地由聚醯胺基質和嵌入其中的連續纖維組成之複合物的其他強化層,其中該聚醯胺基質組成至少80重量%的程度之聚醯胺及其中該複合物中該連續纖維的體積比例另外為10%至80%; 其中該聚醯胺基質的百分比和該連續纖維的百分比各自以該強化層的總質量或總體積為基準計; IV. 隨意地由聚合物材料組成之外覆蓋層。
- 根據請求項6項之熱塑性複合物管,其中該TCP的設計係選自下列群組: a) 聚醯胺模塑料的襯墊/本發明PVDF複合物層/聚醯胺模塑料的覆蓋層; b) PVDF模塑料的襯墊/本發明PVDF複合物層/PVDF模塑料的覆蓋層; c) PVDF模塑料的襯墊/本發明PVDF複合物層/聚醯胺模塑料的覆蓋層; d) 聚醯胺模塑料的襯墊/本發明PVDF複合物層/PVDF模塑料的覆蓋層; e) 二層襯墊,具有聚醯胺模塑料之內層和PVDF之外層/丙烯酸酯共聚物摻合物/本發明PVDF複合物層/PVDF的層/丙烯酸酯共聚物摻合物/聚醯胺模塑料的覆蓋層; f) 二層襯墊,具有聚醯胺模塑料之內層和PVDF之外層/丙烯酸酯共聚物摻合物/本發明PVDF複合物層/PVDF模塑料的覆蓋層; g) PVDF或聚醯胺模塑料的襯墊/本發明PVDF複合物層/具有聚醯胺基質之複合物層/PVDF或聚醯胺模塑料的覆蓋層。
- 根據請求項6和7中任一項之熱塑性複合物管,其中該TCP為臍狀帶(umbilical)、立管、跨接管線、流管線、介入管線、下管線、注入管線或壓力管線。
- 一種根據請求項6至8中任一項之熱塑性複合物管之用途,其用於原油、粗煤氣(crude gas)、三相、加工油、加工氣、汽油或柴油、注入介質的運輸、或用於液壓油的傳導。
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US20220041849A1 (en) | 2022-02-10 |
EP3626764B1 (de) | 2021-02-24 |
CA3112965C (en) | 2023-09-05 |
BR112021004961A2 (pt) | 2021-06-08 |
MX2021003211A (es) | 2021-09-23 |
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