CN114174066A - 用于运输或储存氢的多层结构体 - Google Patents

用于运输或储存氢的多层结构体 Download PDF

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Publication number
CN114174066A
CN114174066A CN202080055439.8A CN202080055439A CN114174066A CN 114174066 A CN114174066 A CN 114174066A CN 202080055439 A CN202080055439 A CN 202080055439A CN 114174066 A CN114174066 A CN 114174066A
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CN
China
Prior art keywords
polymer
multilayer structure
layer
structure according
bact
Prior art date
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Pending
Application number
CN202080055439.8A
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English (en)
Inventor
G.霍克斯泰特
P.当
T.萨瓦特
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Arkema France SA
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Arkema France SA
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Publication of CN114174066A publication Critical patent/CN114174066A/zh
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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
    • B32B1/00—Layered products having a non-planar shape
    • B32B1/08—Tubular products
    • 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
    • B32B1/00—Layered products having a non-planar shape
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29B—PREPARATION OR PRETREATMENT OF THE MATERIAL TO BE SHAPED; MAKING GRANULES OR PREFORMS; RECOVERY OF PLASTICS OR OTHER CONSTITUENTS OF WASTE MATERIAL CONTAINING PLASTICS
    • B29B15/00—Pretreatment of the material to be shaped, not covered by groups B29B7/00 - B29B13/00
    • B29B15/08—Pretreatment of the material to be shaped, not covered by groups B29B7/00 - B29B13/00 of reinforcements or fillers
    • B29B15/10—Coating or impregnating independently of the moulding or shaping step
    • B29B15/12—Coating or impregnating independently of the moulding or shaping step of reinforcements of indefinite length
    • 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
    • B29C48/00—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor
    • B29C48/03—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor characterised by the shape of the extruded material at extrusion
    • B29C48/07—Flat, e.g. panels
    • 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
    • B29C48/00—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor
    • B29C48/03—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor characterised by the shape of the extruded material at extrusion
    • B29C48/09—Articles with cross-sections having partially or fully enclosed cavities, e.g. pipes or channels
    • 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
    • B29C48/00—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor
    • B29C48/15—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor incorporating preformed parts or layers, e.g. extrusion moulding around inserts
    • 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
    • B29C48/00—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor
    • B29C48/25—Component parts, details or accessories; Auxiliary operations
    • B29C48/92—Measuring, controlling or regulating
    • 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
    • B29C53/00—Shaping by bending, folding, twisting, straightening or flattening; Apparatus therefor
    • B29C53/56—Winding and joining, e.g. winding spirally
    • 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
    • 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
    • B29C65/14—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using wave energy, i.e. electromagnetic radiation, or particle radiation
    • B29C65/1403—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using wave energy, i.e. electromagnetic radiation, or particle radiation characterised by the type of electromagnetic or particle radiation
    • B29C65/1412—Infrared [IR] radiation
    • 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
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    • B29C65/02—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure
    • B29C65/14—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using wave energy, i.e. electromagnetic radiation, or particle radiation
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    • B29C65/1435—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using wave energy, i.e. electromagnetic radiation, or particle radiation characterised by the way of heating the interface at least passing through one of the parts to be joined, i.e. transmission welding
    • 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
    • B29C65/14—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using wave energy, i.e. electromagnetic radiation, or particle radiation
    • B29C65/16—Laser beams
    • B29C65/1629—Laser beams characterised by the way of heating the interface
    • B29C65/1635—Laser beams characterised by the way of heating the interface at least passing through one of the parts to be joined, i.e. laser transmission welding
    • 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
    • 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
    • B29C65/14—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using wave energy, i.e. electromagnetic radiation, or particle radiation
    • B29C65/16—Laser beams
    • B29C65/1677—Laser beams making use of an absorber or impact modifier
    • 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
    • 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
    • B29C65/34—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using heated elements which remain in the joint, e.g. "verlorenes Schweisselement"
    • B29C65/36—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using heated elements which remain in the joint, e.g. "verlorenes Schweisselement" heated by induction
    • B29C65/3604—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using heated elements which remain in the joint, e.g. "verlorenes Schweisselement" heated by induction characterised by the type of elements heated by induction which remain in the joint
    • B29C65/3608—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using heated elements which remain in the joint, e.g. "verlorenes Schweisselement" heated by induction characterised by the type of elements heated by induction which remain in the joint comprising single particles, e.g. fillers or discontinuous fibre-reinforcements
    • 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
    • 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
    • B29C65/34—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using heated elements which remain in the joint, e.g. "verlorenes Schweisselement"
    • B29C65/36—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using heated elements which remain in the joint, e.g. "verlorenes Schweisselement" heated by induction
    • B29C65/3672—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using heated elements which remain in the joint, e.g. "verlorenes Schweisselement" heated by induction characterised by the composition of the elements heated by induction which remain in the joint
    • B29C65/3676—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure using heated elements which remain in the joint, e.g. "verlorenes Schweisselement" heated by induction characterised by the composition of the elements heated by induction which remain in the joint being metallic
    • 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
    • B29C66/01—General aspects dealing with the joint area or with the area to be joined
    • B29C66/05—Particular design of joint configurations
    • B29C66/10—Particular design of joint configurations particular design of the joint cross-sections
    • B29C66/11—Joint cross-sections comprising a single joint-segment, i.e. one of the parts to be joined comprising a single joint-segment in the joint cross-section
    • B29C66/112—Single lapped joints
    • B29C66/1122—Single lap to lap joints, i.e. overlap joints
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C66/40—General aspects of joining substantially flat articles, e.g. plates, sheets or web-like materials; Making flat seams in tubular or hollow articles; Joining single elements to substantially flat surfaces
    • B29C66/41—Joining substantially flat articles ; Making flat seams in tubular or hollow articles
    • 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
    • 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
    • B29C66/712—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 the composition of one of the parts to be joined being different from the composition of the other part
    • 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
    • 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
    • B29C66/72—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 structure of the material of the parts to be joined
    • B29C66/721—Fibre-reinforced materials
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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
    • B29C66/70—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
    • B29C66/72—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 structure of the material of the parts to be joined
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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
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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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    • B29C66/731—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 characterised by the intensive physical properties of the material of the parts to be joined
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    • B29C66/731—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 characterised by the intensive physical properties of the material of the parts to be joined
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Abstract

本发明涉及多层结构体，其选自储罐、管道或管路，其用于运输、分配、或储存氢，其从内侧至外侧包含至少一个密封层和至少一个复合增强层，所述最内的复合增强层熔接至所述最外的相邻的密封层，所述密封层由如下组合物组成：该组合物主要包含至少一种半结晶热塑性聚合物P1i(i＝1至n，n为密封层数)，其根据ISO 11357‑3:2013测量的Tf小于280℃、特别地小于265℃，其中各密封层的所述至少一种热塑性聚合物可为相同或不同的，并且所述复合增强层的至少一个由呈连续纤维形式的纤维状材料组成，所述纤维状材料浸渍有如下组合物：该组合物主要包含至少一种热塑性聚合物P2j，(j＝1至m，m为增强层数)，其特别地是半结晶的，所述热塑性聚合物P2j具有根据ISO 11357‑3:2013测量的大于所述结构体的最大使用温度(Tu)的Tg，其中Tg≥Tu+20℃，Tu大于50℃、特别地大于100℃。

Description

用于运输或储存氢的多层结构体
技术领域
本专利申请涉及用于运输、分配、或储存氢的多层复合结构体，及制造其的方法。
背景技术
在机动车领域中寻求的目标之一是提出污染越来越少的车辆。因而，包含电池的电动或混动车辆旨在逐步取代内燃机车辆，诸如汽油或柴油车辆。已经表明，电池是相对复杂的车辆零件。取决于电池在车辆中的定位，可必要的是保护其免于冲击和外部环境(其可具有极端温度和可变湿度)。还必要的是避免任何燃烧的风险。
此外，为了不损坏电池的单元电池和为了保全其寿命，重要的是其运行温度不超过55℃。相反地，例如在冬天，可必要的是提高电池温度，以优化其运行。
此外，电动车辆如今仍然遭受若干问题，即电池续航里程(范围，range)，在这些电池中使用其资源并非取之不尽的稀土，以及各国电力生产能否给电池充电的问题。
因此，氢是对供电电池(electric battery)的替代，因为氢可借助燃料电池转化为电力，并从而为电动车辆供能。
然而，由于氢非常低的摩尔质量和非常低的液化温度，氢的储存在技术上是困难的并且成本高昂，尤其是当涉及移动储存时。然而，为了高效，储存必须以小体积实施，鉴于车辆使用时的温度，这意味着氢必须被保持在高压下。对于燃料电池混动道路车辆而言情况尤为如此，所述车辆的目标是除了电池供能的电动基础之外对于基本上城市用途约600至700km、或甚至更少的续航里程。
氢储罐通常是由必须防止氢漏出的金属衬垫制成的。此第一衬垫必须自身被第二衬垫(通常由复合材料制成)保护，该第二衬垫设计成承受储罐的内部压力(例如700巴)、并且承受任何冲击或热源。阀门系统也必须是安全的。
根据法国氢和燃料电池联合会(AFHYPAC)氢备忘录4.2(2016年12月版)，加压氢储存和分配很多年来已经是标准实践，其中圆柱形钢瓶或瓶组装件充气至20或25MPa(I和II型)。此储存方法的缺点是尺寸——在20MPa和常温(21℃)下为仅14kg/m3(相比之下，甲烷为100kg/m3)——和最重要的重量，其由为了避免氢脆变(hydrogen embrittlement)问题而使用低应力钢所导致。随着复合储罐(被称为III或IV型)技术的出现，情况已发生根本改变。其基本原理是将密封和机械强度两项基本功能分离，并且对它们彼此独立地进行管理(控制，manage)。在此类型的储罐中，将由树脂(热固性或热塑性)制成的囊(亦称为衬垫(或密封鞘(sheath)))与由纤维(玻璃、芳纶、碳)构成的增强结构体(亦称为增强层或套管)组合，其允许储罐在高得多的压力下操作并同时降低其质量和避免在严重外部侵蚀的情况下爆炸性破裂的风险。因而，70MPa(700巴)已经实际上变成当前标准。
在IV型储罐中，衬垫和增强层是由不同材料制成的，其具有在衬垫和增强层之间存在粘附不足的缺点，当既存在气体在衬垫和复合物之间的界面处积聚又存在储罐的内部压力下降时，该缺点导致衬垫崩溃的问题。
此问题已经导致开发V型储罐，该储罐基于使用相同聚合物用于衬垫和复合物基体，以保证衬垫和复合物之间卓越且耐久的粘附。
当借助刚性或柔性管道运输或分配氢时，还优选的是，氢处于低体积且因此高压力，以确保足够的流动。因而，就储存、运输、或分配氢而言，使用如下复合管道是令人关注的：其由被复合材料制成的外层所增强的密封鞘构成(确保气密性和化学耐受性)，其是由以相继的层沉积在衬垫上的单向(UD)带(tape)通过长丝(filament)卷绕而制造的。当期望使此管道柔性时，一种可能性是将UD带以相对于管道轴一个或多个取向角度卷绕，使得复合增强物可支撑复合管道在其使用期间的变形。所述复合增强物允许管道承受由被运输的流体所产生的内部压力。
至于储存储罐，必要的是密封鞘抵抗崩溃，尤其是在导致压力突然下降的生产停止期间。当鞘未粘附至复合增强物且气体可存在于密封鞘和复合增强物之间时，存在该崩溃风险。为了避免此现象，一种解决方案是向压力夹套添加称为骨架的内部增强物：此增强物(通常是金属的)被穿孔以使其为柔性的，并且因此其对于被运输的流体不是密封的。其对于柔性管道增加了重量、复杂性和成本。此外，为了降低复合管道的重量或甚至消除复合管道的内部骨架，必要的是所述复合增强物粘附至密封鞘，如在V型储存储罐的情形中那样。
此外，密封鞘必须能够被连续挤出，可能挤出在如上文所描述的内部骨架支撑体上。此密封鞘必须足够化学稳定，使得其机械和密封特性在所述储罐或柔性管道的寿命期间不以禁止性的方式恶化。
在具有内部金属骨架的柔性管道的情形中，密封衬垫还必须能够承受制成其的材料的蠕变效应(由于管道的内部压力在密封鞘上产生应力而引起)。当管道受到被运输的流出物的压力时，蠕变在其上有衬垫的金属铠装(armoring)(例如自锁的Z或T几何形状)之间的接头(空隙或间隙)中发生，从而生成材料突起，其产生应力集中且因此对于密封鞘是优先的失效区(failure zone)：构成密封鞘的材料因此还必须承受这些应力集中。
例如，Airborne已经开发了多种柔性管道，其不具有内部骨架并且具有粘附至复合增强物的密封鞘，所述柔性管道包含：具有PA11 FC复合物的PA11衬垫(JIP于2011年完成)或者具有PA12 FC复合物的PA12衬垫，或者甚至具有PVDF FC复合物的PVDF衬垫。然而，所有这些结构体都具有如下缺点：复合增强物的基体具有比管道的使用温度Tu低的玻璃化转变温度Tg；即，在基于PA11或PA12的管道的情形中，干燥状态中的Tg为50℃，而管道使用温度Tu为60至80℃；以及在PVDF的情形中，Tg为-40℃，而在连续操作中的使用温度为100℃以上并且通常接近130℃。在特定的PVDF情形中，基体的硬度(刚度，stiffness)(模量)在其Tg以上保持为高的，直至其达到在100℃左右的另一转变(α转变)，超出该转变之后基体的行为变成纯橡胶状的。因而，在TP基体复合管道的所有以上工业和商业情形中，复合增强物的基体在复合管道使用温度Tu下均处于完全橡胶化的状态。
为了解决此问题和为了使其基体具有高于最大使用温度的Tg的复合增强物在使用温度(在此情形中为130℃)下不处于橡胶化状态，Kutting&Total、然后是Vitrex和Magma已经开发了如下解决方案：由PEEK密封鞘(或衬垫)构成，其通过具有PEEK基体的复合物增强。PEEK的Tg为140℃，并且因此满足高刚度(rigidity)的要求，因为此Tg高于最大使用温度。缺点是，结果，所述密封鞘也是非常刚性的，这可限制其疲劳寿命，并且对于生产柔性管道而言是主要缺点。此外，此类型的密封套管的加工温度非常高(典型地380-400℃)，并且这在常见的转变工艺(其为管路挤出)的情形中在工具作业和工艺控制方面造成了主要困难。
此外，Ticona(Celanese)与Airborne一道提供了具有PPS FC增强物和PPS密封鞘的复合管道。
对于Tu>90℃，此结构体对于复合物基体造成了与基于PVDF的解决方案相同的问题(即，Tg<Tu)，并且另外存在转变温度的问题(对于PPS和PVDF，典型地分别为350℃对250℃)。
对于Tu<90℃，PPS是适合于复合物基体的，但是密封衬垫挤出温度的问题仍然存在，以及其高刚度的问题(其限制了复合管道的柔韧性)。
氢储罐的情形造成了相似的技术问题，因为其快速被氢填充导致储罐温度由于氢的压缩而提高，尤其是在约110℃，在复合物的基体具有低于此温度的Tg的情形中，这要求复合物是超尺寸的(特大尺寸的，oversized)。
因而，仍要在一方面优化复合物的基体，以优化其在高温下的机械强度，并且在另一方面优化构成密封衬垫的材料，以优化其应用温度而不使复合增强物对密封衬垫的粘附劣化。因而，为了确保与复合物的基体的至少部分混溶性而将做出的对构成密封衬垫的材料的组成进行的改变不应当导致该衬垫的制造温度(挤出-吹塑、注射、滚塑、等等)与如今聚酰胺和PVDF所实践的温度相比显著增加。
这些问题通过提供本发明的多层结构体而得以解决，所述多层结构体为完全结合的、“双材料”复合管道或储罐，并且是由高强度复合增强物(即包含高Tg基体)沉积(特别地通过长丝卷绕)在事先在相对低的温度下挤出的衬垫上而构成的。复合物和衬垫之间的粘附非常良好。
在整个本说明书中，术语“衬垫”、“密封鞘”和“压力夹套”具有相同的含义。
因而，本发明涉及如下的多层结构体：其选自旨在运输或储存氢的储罐、管道或管路(管，tube)，其从内侧至外侧包含至少一个密封层和至少一个复合增强层，
所述最内的复合增强层熔接至所述最外的相邻密封层，
所述密封层由如下组合物组成：该组合物主要包含至少一种半结晶热塑性聚合物P1i(i＝1至n，n为密封层数)，其根据ISO 11357-3:2013测量的Tm小于280℃、特别地小于265℃，
各密封层的所述至少一种热塑性聚合物可为相同或不同的，并且所述复合增强层的至少一个由呈连续纤维形式的纤维状材料组成，所述纤维状材料浸渍有如下组合物：该组合物主要包含至少一种热塑性聚合物P2j(j＝1至m，m为增强层数)，所述热塑性聚合物P2j特别地为半结晶的，所述热塑性聚合物P2j具有根据ISO 11357-3:2013测量的大于所述结构体的最大使用温度(Tu)的Tg，其中Tg≥Tu+20℃、特别地Tg≥Tu+30℃，Tu大于50℃、特别地大于100℃。
因而，发明人预料之外地发现，对于复合物基体和衬垫使用不同聚合物，并且特别地：
复合增强物的基体是由如下聚合物构成的：该聚合物具有显著大于储罐或管道的最大使用温度Tu的Tg(典型地，Tg>Tu+20℃、特别地Tg≥Tu+30℃)，以仍然在其玻璃态区中并且具有高刚度，从而使得复合物能够具有高机械强度，
构成衬垫的半结晶聚合物具有低熔点Tm，从而允许其在对于本领域技术人员常见的中等温度下，相对于此聚合物的Tm(小于280℃、优选地小于265℃)通过挤出、挤出吹塑、滚塑、注射或者通过卷绕纯树脂膜(视情况而定)加工。目前已知的低Tm的半结晶聚合物也具有低Tg，该Tg在大多数情况下将在最大使用温度以下。结果，构成衬垫的聚合物将在其橡胶化区中工作，并且因此将是非常柔性的并且因此对于疲劳非常耐受。其半结晶性质确保对于化学侵蚀、磨损和蠕变的良好耐受性，
并且，两种前述聚合物(构成复合物基体的聚合物和构成衬垫的聚合物)是彼此足够能混溶的，以确保复合物对衬垫的可熔接性以及因而在衬垫和复合物之间卓越的粘附。粘附的耐久性将通过构成在该两种材料的界面处(即在熔接接头中)的混合物的材料的耐久性而得以保证。该两种聚合物的混溶性是通过如下表达的：优选地通过单一Tg；或者当无法那样时，通过部分均相混合物的特性标记(characteristic signature)，例如通过对该两种纯聚合物的Tg存在两个中间的Tg值。
两种聚合物的不混溶性导致在该两种聚合物的混合物中存在两个Tg，其对应于分开取的纯聚合物的各自的Tg。
“多层结构体”意为，例如，包含若干层特别地两层、或者由其组成的储罐、管道、或管路。
与作为最外层的复合增强层相比，密封层(一个或多个)是最内层。
密封层是与氢接触的，即便存在用以形成所述骨架的更内的且因而最内的非密封金属层时也是如此，所述非密封金属层通过螺旋卷绕的异型金属条带诸如经切断的条带而形成，在其上通过挤出包覆所述密封层(一个或多个)。
当存在若干密封层时，所述密封层的仅最内者与氢直接接触。
当仅存在密封层和复合增强层、从而导致两层的多层结构体时，则该两层被熔接并从而彼此粘附，彼此直接接触。
当存在若干密封层和/或若干复合增强层时，则所述密封层的最外层(且从而是和与氢接触的层相反的层)熔接至所述复合增强层的最内层，并从而彼此粘附，彼此直接接触。
其它复合增强层也是熔接在一起的。
其它密封层也是熔接在一起的。
关于密封层和热塑性聚合物P1i
可存在一个或多个密封层。
所述层的每一个均由如下组合物组成：该组合物主要包含至少一种热塑性聚合物P1i，i对应于存在的层数。i为1至10、特别地1至5、特别地1至3、优选地i＝1。
术语“主要(地)”意指所述至少一种聚合物是以超过50重量％存在的，相对于组合物的总重量计。
有利地，所述至少一种主要聚合物是以如下量存在的：大于60重量％、特别地大于70重量％、特别地大于80重量％、更特别地大于或等于90重量％，相对于组合物的总重量计。
所述组合物可进一步包含抗冲改性剂和/或添加剂。
所述添加剂可选自抗氧化剂、热稳定剂、UV吸收剂、光稳定剂、润滑剂、无机填料、阻燃剂、成核剂、增塑剂、染料、炭黑、和碳质纳米填料。
有利地，所述组合物主要由以下组成：所述热塑性聚合物P1i、0至5重量％的抗冲改性剂、0至5重量％的添加剂，所述组合物的成分的总和等于100％(基于最大90％P2i)。
各层中的所述至少一种主要聚合物可为相同或不同的。
在一种实施方式中，至少在熔接至复合增强层的密封层中存在单一主要聚合物。
热塑性聚合物P1i
热塑性塑料或热塑性聚合物指如下的半结晶材料：在环境温度下其一般为固体，并且在温度升高期间、特别是在超过其玻璃化转变温度(Tg)之后软化，并且在超过被称为其熔点(Tm)处可展现尖锐转变，并且当温度降低至其结晶温度以下时再次变为固体。
Tg、Tc和Tm分别是根据标准11357-2:2013和11357-3:2013通过差示扫描量热法(DSC)确定的。
所述热塑性聚合物的数均分子量Mn优选地在10000至40000、优选地12000至30000的范围中。这些Mn数值可对应于大于或等于0.8的特性粘度，如根据标准ISO 307:2007但是通过改变溶剂在间甲苯酚中确定的(使用间甲苯酚而不是硫酸，并且温度为20℃)。
本发明中合适的半结晶热塑性聚合物的实例包括：
聚酰胺，包括共聚物，例如聚酰胺-聚醚共聚物、聚酯、和PVDF、和PVDF/PEI共混物(其中PVDF是主要的)。
在所述半结晶聚合物之中更特别优选的是聚酰胺及其半结晶共聚物。
用以定义聚酰胺的命名法描述于ISO标准1874-1:2011“Plastiques--Matériauxpolyamides(PA)pour moulage et extrusion--Partie 1:Désignation”中，尤其是在第三页(表1和2)上，并且是技术人员所熟知的。
所述聚酰胺可为均聚酰胺、或共聚酰胺、或其混合物。
有利地，所述热塑性聚合物为长链脂族聚酰胺，即具有相对于每个氮原子大于8.5、优选地大于9的平均碳原子数的聚酰胺。
特别地，所述长链脂族聚酰胺选自：
聚酰胺11(PA11)、聚酰胺12(PA12)、聚酰胺1010(PA1010)、聚酰胺1012(PA1012)、聚酰胺1212(PA1012)、或其混合物或其共聚酰胺，特别地PA11和PA12。
有利地，所述热塑性聚合物为长链半芳族聚酰胺，即具有相对于每个氮原子大于8.5、优选地大于9的平均碳原子数和240至小于280℃的熔点的聚酰胺。
特别地，所述长链半芳族聚酰胺选自聚酰胺11/5T或11/6T或11/10T。在此情形中显而易见的是，应当小心选取11的比率，使得所述聚合物的Tm低于280℃、优选地低于265℃。
有利地，各密封层由如下组合物组成：该组合物包含相同类型的聚合物、特别地聚酰胺。
有利地，包含所述聚合物P1i的所述组合物颜色为黑色，并且能够吸收适合于熔接的辐射。
存在各种方法用于熔接热塑性聚合物部件(部分)。因而，可使用接触或非接触的加热刮刀(heating blade)、超声、红外、振动、将一个待熔接的元件相对于于另一个旋转、或甚至激光熔接。
热塑性聚合物元件的熔接(特别地通过激光熔接)要求待熔接的两个元件相对于辐射特别是激光辐射具有不同性质：元件之一必须是对辐射特别是激光辐射透明的，并且另一个必须吸收辐射特别是激光辐射。因而，辐射特别是激光辐射穿过透明部件并且随后到达吸收元件，在该处所述辐射被转化为热。这允许两个元件之间的接触区域熔融并且从而使熔接发生。
在一些应用中，期望的是，两个待熔接部件均为黑色，包括对激光辐射透明的部件。
为了使它们为能吸收的，已知的是添加各种添加剂，包括例如炭黑，其给予聚合物黑色并且允许其吸收适合于熔接的辐射。
在一种实施方式中，熔接是通过选自激光、红外(IR)加热、LED加热、感应或微波加热、或高频(HF)加热的系统进行的。
在其中熔接是通过激光熔接实施的情形中，则所述组合物P1i包含非附聚或非聚集的碳质填料。
在其中熔接是通过感应实施的情形中，则所述组合物P1i包含金属颗粒。
有利地，熔接是通过激光系统进行的。
关于复合增强层和热塑性聚合物P2j
可存在一个或多个复合增强层。
所述层的每一个均由如下组合物组成：该组合物主要包含至少一种热塑性聚合物P2j，j对应于存在的层数。
j包含1至10、特别地1至5、特别地1至3、优先地j＝1。
术语“主要(地)”意指所述至少一种聚合物以超过50重量％存在，相对于组合物的总重量计。
有利地，所述至少一种主要聚合物以大于60重量％、特别地大于70重量％、特别地大于80重量％、更特别地大于或等于90重量％存在，相对于组合物的总重量计。
所述组合物可进一步包含抗冲改性剂和/或添加剂。
所述添加剂可选自抗氧化剂、热稳定剂、UV吸收剂、光稳定剂、润滑剂、无机填料、阻燃剂、成核剂、增塑剂、和染料。
有利地，所述组合物主要由以下组成：所述热塑性聚合物P2j、0至5重量％的抗冲改性剂、0至5重量％的添加剂，组合物的成分的总和等于100％(基于最大90％的P2j)。
各层中的所述至少一种主要聚合物可为相同或不同的。
在一种实施方式中，至少在熔接至密封层的复合增强层中存在单一主要聚合物。
在一种实施方式中，各增强层包含相同类型的聚合物、特别地聚酰胺。
热塑性聚合物P2j
热塑性塑料或热塑性聚合物指如下的材料：在环境温度下其一般为固体，其可为半结晶或无定形的、特别地半结晶的，并且在温度升高期间、特别是在超过其玻璃化转变温度(Tg)之后软化，并且当其为无定形的时在更高温度下流动、或者当其为半结晶的时一超过其所谓的熔融温度(Tm)就可展现尖锐转变，并且当温度降低至其结晶温度以下(对于半结晶者)时或者其玻璃化转变温度以下(对于无定形者)时再次变为固体。
Tg、Tc、和Tm分别是根据标准11357-2:2013和11357-3:2013通过差示扫描量热法(DSC)确定的。
所述复合增强层的至少一个的组合物的聚合物P2j是这样的：其Tg大于所述结构体的最大使用温度(Tu)，并且特别地Tg≥Tu+20℃、尤其Tg≥Tu+30℃。
在一种实施方式中，聚合物P2j具有Tg≥Tu+20℃、特别地Tg≥Tu+30℃，无论所述所述增强层的位置如何。
在另一种实施方式中，由包含具有Tg≥Tu+20℃、尤其Tg≥Tu+30℃的聚合物P2j的组合物组成的所述增强层是熔接至所述密封层的层。
在一种实施方式中，所述复合增强层的至少一个的组合物的聚合物P2j是这样的：其Tg大于所述结构体的最大使用温度(Tu)，Tg≥Tu+20℃，并且由包含该聚合物P2j的组合物组成的所述增强层是熔接至所述密封层的层。
在一种实施方式中，所述复合增强层的至少一个的组合物的聚合物P2j是这样的：其Tg大于所述结构体的最大使用温度(Tu)，Tg≥Tu+30℃，并且由包含该聚合物P2j的组合物组成的所述增强层是熔接至所述密封层的层。
在另一种实施方式中，由包含具有Tg≥Tu+20℃、尤其Tg≥Tu+30℃的聚合物P2j的组合物组成的所述增强层是所述结构体的最外的增强层。所述热塑性聚合物的数均分子量Mn优选地在10000至40000、优选地12000至30000的范围中。这些Mn数值可对应于大于或等于0.8的特性粘度，如根据标准ISO 307:2007但是通过改变溶剂在间甲苯酚中确定的(使用间甲苯酚而不是硫酸，并且温度为20℃)。
本发明中合适的半结晶热塑性聚合物的实例包括：
聚酰胺，特别地包含芳族和/或脂环族结构的聚酰胺，包括共聚物，例如聚酰胺-聚醚共聚物、聚酯，
聚芳醚酮(PAEK)，
聚醚醚酮(PEEK)，
聚醚酮酮(PEKK)，
聚醚酮醚酮酮(PEKEKK)，
聚酰亚胺，特别地聚醚酰亚胺(PEI)或聚酰胺-酰亚胺，
聚砜(PSU)，特别地聚芳基砜，诸如聚苯砜(PPSU)，
聚醚砜(PES)。
半结晶聚合物是特别优选的，并且特别地聚酰胺及其半结晶共聚物。
用以定义聚酰胺的命名法描述于ISO标准1874-1:2011“Plastiques--Matériauxpolyamides(PA)pour moulage et extrusion--Partie 1:Désignation”中，尤其是在第三页(表1和2)上，并且是技术人员所熟知的。
聚酰胺可为均聚酰胺、或共聚酰胺、或其混合物。
有利地，所述半结晶聚酰胺为半芳族聚酰胺，尤其是如EP1505099中所描述的式X/YAr的半芳族聚酰胺，尤其是式A/XT的半芳族聚酰胺，其中A选自由氨基酸获得的单元、由内酰胺获得的单元、和对应于式(Ca二胺).(Cb二酸)的单元，其中a代表二胺的碳原子数并且b代表二酸的碳原子数，a和b各自在4和36之间、有利地在9和18之间，单元(Ca二胺)选自线型或支化的脂族二胺、脂环族二胺和烷基芳族二胺，并且单元(Cb二酸)选自线型或支化的脂族二酸、脂环族二酸和芳族二酸；
X.T表示由Cx二胺和对苯二甲酸的缩聚获得的单元，其中x代表Cx二胺的碳原子数，x在5和36之间、有利地在9和18之间，特别地具有式A/5T、A/6T、A/9T、A/10T、或A/11T的聚酰胺，A是如上文所定义的，特别地选自以下的聚酰胺：PA MPMDT/6T、PA11/10T、PA 5T/10T、PA 11/BACT、PA 11/6T/10T、PA MXDT/10T、PA MPMDT/10T、PA BACT/10T、PA BACT/6T、PA BACT/10T/6T、PA11/BACT/6T、PA 11/MPMDT/6T、PA 11/MPMDT/10T、PA 11/BACT/10T、PA11/MXDT/10T、11/5T/10T。
T对应于对苯二甲酸，MXD对应于间苯二甲二胺，MPMD对应于甲基五亚甲基二胺，并且BAC对应于双(氨基甲基)环己烷。如上文所定义的所述半芳族聚酰胺特别地具有大于或等于80℃的Tg。
有利地，各复合增强层由如下组合物组成：该组合物包含相同类型的聚合物、特别地聚酰胺。
有利地，包含所述聚合物P2j的所述组合物是对适合于熔接的辐射透明的。
出于熔接、尤其是激光熔接的目的，热塑性聚合物一般是透明的。碳质纳米填料使得可赋予包含热塑性聚合物的组合物的层黑色，并同时保持所述层的对激光辐射的透明性。
有利地，所述碳质纳米填料为非附聚或非聚集的。
有利地，所述碳质纳米填料以100ppm至500ppm、并且优选地100ppm至250ppm的量并入组合物中。
有利地，所述碳质纳米填料选自碳纳米管(CNT)、碳纳米纤维、石墨烯、纳米尺度炭黑、及其混合物。
有利地，所述碳质纳米填料不含纳米炭黑。
在一种实施方式中，熔接是通过选自激光、IR加热、或感应加热的系统进行的。
有利地，所述熔接是通过激光系统进行的。
有利地，激光辐射为红外激光辐射，并且优选地具有在700nm和1200nm之间、并且优选地在800nm和1100nm之间的波长。
关于结构体
因而，所述多层结构体包含熔接在一起的至少一个密封层和至少一个复合增强层。
在一种实施方式中，在所述多层结构体中，各密封层的各聚合物P1i是与相邻层的各聚合物P1i部分或完全能混溶的，各增强层的各聚合物P2j是与相邻层的各聚合物P2j部分或完全能混溶的，并且各聚合物P2j是与各聚合物P1i部分或完全能混溶的(当他们相邻时)，并且聚合物P21是与和其相邻的聚合物P11部分或完全能混溶的，
所述聚合物的完全或部分混溶性是通过两种树脂在混合物中的玻璃化转变温度的差异相对于两种树脂在混合之前的玻璃化转变温度的差异来定义的，并且当所述差异等于0时混溶性为完全的，并且当所述差异不同于0时混溶性为部分的，排除聚合物P2j与聚合物P1i的不混溶性。
当所述聚合物的混溶性为部分的时，所述差异为所述混溶性越大则所述差异越小。
有利地，当所述聚合物的混溶性为部分的时，所述差异小于30％、优选地小于20％，以绝对数值计。
在一种实施方式中，混合物的玻璃化转变温度，取决于混溶性为完全还是部分的，必然在所述聚合物于共混之前的玻璃化转变温度之间，并且与它们相差至少5℃、优选地至少10℃。
表述“完全能混溶(的)”意指：当例如两种聚合物P11和P12(其分别具有Tg11和Tg12)存在于两个相邻密封层或两个相邻增强层中时，则该两种聚合物的混合物仅具有一个Tg1112，其数值在Tg11和Tg12之间。
进而，此Tg1112数值比Tg11大至少5℃、特别地至少10℃，并且比Tg12低至少5℃、特别地至少10℃。
表述“部分能混溶(的)”意指：当例如两种聚合物P11和P12(其分别具有Tg11和Tg12)存在于两个相邻密封层或两个相邻增强层中时，则该两种聚合物的混合物具有两个Tg：Tg’11和Tg’12，其中Tg11<Tg’11<Tg’12<Tg12。
进而，这些Tg’11和Tg’12数值比Tg11大至少5℃、特别地至少10℃，并且比Tg12低至少5℃、特别地至少10℃。
两种聚合物的不混溶性导致在该两种聚合物的混合物中存在两个Tg：Tg11和Tg12，其对应于分开取的纯聚合物各自的Tg，Tg11和Tg12。
有利地，所述经熔接的密封层和增强层是由分别包含不同聚合物的组合物制成的。
尽管如此，所述不同聚合物可为相同类型的。
因而，若两个经熔接的复合增强层和密封层之一是由包含脂族聚酰胺的组合物制成的，则另一层是由包含如下聚酰胺的组合物制成的：其为非脂族的并且为例如半芳族聚酰胺，以具有高Tg聚合物作为复合增强物的基体。
所述多层结构体可包含最高达10个密封层和最高达10个复合增强层。
显而易见的是，所述多层结构体不必是对称的，并且因此其可包含相比复合层更多的密封层，或者反之。
有利地，所述多层结构体包含一个、两个、三个、四个、五个、六个、七个、八个、九个、或十个密封层，和一个、两个、三个、四个、五个、六个、七个、八个、九个、或十个复合增强层。
有利地，所述多层结构体包含一个、两个、三个、四个、或五个密封层，和一个、两个、三个、四个、或五个复合增强层。
有利地，所述多层结构体包含一个、两个、或三个密封层，和一个、两个、或三个复合增强层。
有利地，它们由分别包含不同聚合物的组合物组成。
有利地，它们由如下组合物组成：该组合物分别包含对应于聚酰胺P1i和P2j的聚酰胺。
有利地，它们由分别包含不同聚酰胺的组合物组成。
在一种实施方式中，所述多层结构体包含单一密封层和若干增强层，所述密封层是熔接至所述相邻增强层的。
在另一种实施方式中，所述多层结构体包含单一增强层和若干密封层，所述增强层是熔接至所述相邻密封层的。
在一种有利实施方式中，所述多层结构体包含熔接在一起的单一密封层和单一复合增强层。
因此，这两层的所有组合都在本发明的范围内，条件是：至少所述最内的复合增强层熔接至所述最外的相邻密封层，其它层熔接在一起或未熔接在一起。
有利地，在所述多层结构体中，各密封层由如下组合物组成：该组合物包含相同类型的聚合物P1i、特别地聚酰胺。
表述“相同类型的聚合物”意指，例如，取决于层可为相同或不同聚酰胺的聚酰胺。
有利地，所述聚合物P1i为聚酰胺并且所述聚合物P2j为聚酰胺。
有利地，聚酰胺P1i对于所有密封层都是相同的。
有利地，所述聚合物P1i为长链脂族聚酰胺，特别地PA1010、PA 1012、PA 1212、PA11、PA12，特别地PA 11或PA12。
有利地，所述聚酰胺P1i为长链半芳族聚酰胺，特别地PA 11/5T、PA 11/6T、或PA11/10T。在此情形中显而易见的是，必须小心选取11的比率，使得所述聚合物的Tm低于280℃、优选地265℃。
有利地，在所述多层结构体中，各增强层由如下组合物组成：该组合物包含相同类型的聚合物P2j、特别地聚酰胺。
有利地，聚酰胺P2j对于所有增强层都是相同的。
有利地，所述聚合物P2j为选自以下的半芳族聚酰胺：PA MXDT/6T、PA 11/10T、PA11/BACT、PA 5T/10T、PA 11/6T/10T、PA MXDT/10T、PA MPMDT/10T、PA BACT/10T、PA BACT/6T、PA BACT/10T/6T、PA 11/BACT/6T、PA 11/MPMDT/6T、PA 11/MPMDT/10T、PA 11/BACT/10T、PA 11/MXDT/10T、PA 5T/10T。
有利地，在所述多层结构体中，各密封层由包含相同类型的聚合物P1i、特别地聚酰胺的组合物组成，并且各增强层由包含相同类型的聚合物P2j、特别地聚酰胺的组合物组成，条件是：聚酰胺P1i和P2j是不同的，即，若密封层由包含长链脂族聚酰胺的组合物组成，则密封层由包含半芳族聚酰胺的组合物组成。
有利地，所述聚合物P1i为长链脂族聚酰胺，特别为PA1010、PA 1012、PA 1212、PA11、PA12，尤其为PA 11或PA12，并且所述聚合物P2j为半芳族聚酰胺，特别地选自PAMPMDT/6T、PA PA11/10T、PA 11/BACT、PA 5T/10T、PA 11/6T/10T、PA MXDT/10T、PA MPMDT/10T、PA BACT/10T、PA BACT/6T,PA BACT/10T/6T、PA 11/BACT/6T,PA 11/MPMDT/6T,PA 11/MPMDT/10T,PA 11/BACT/10T、PA 11/MXDT/10T、和PA 5T/10T。
有利地，所述多层结构体由单一增强层和单一密封层组成，其中所述聚合物P1i为长链脂族聚酰胺，特别地PA1010、PA 1012、PA 1212、PA11、PA12，特别地PA 11或PA12；并且所述聚合物P2j为半芳族聚酰胺，特别地选自PA MPMDT/6T、PA PA11/10T、PA 11/BACT、PA11/6T/10T a PA MXDT/10T、PA MPMDT/10T、PA BACT/10T、PA BACT/6T、PA BACT/10T/6T、PA11/BACT/6T、PA 11/MPMDT/6T、PA 11/MPMDT/10T、PA 11/BACT/10T、PA 11/MXDT/10T。
根据一种实施方式，所述多层结构体为储罐。
根据另一种实施方式，所述多层结构体为柔性管道。
所述多层结构体的最大使用温度Tu为50℃以上、特别地100℃以上。
在一种实施方式中，上文所定义的所述多层结构体具有减压耐受性和干燥能力。
的确，当储存或运输氢时，由于密封层对运输或储存的氢的渗透性，氢可从管路或储罐的内部扩散通过密封层，到达最后的密封层和第一复合增强层之间的界面。氢在此位置的积聚可产生压力，其在管路或储罐的内部压力低于与复合增强物的界面处的压力时(这尤其可在以下情况下发生：当氢的泵送或运输在生产中断(停止，stoppage)期间停止、导致数百巴到大气压的压力下降时，或者当储存储罐空了时)将导致密封层的崩溃。这同样适用于储罐的内部水压测试：此水可能通过渗透迁移到复合增强物和最后的密封层之间的界面处，并且继而将非常难以移除，导致所述储存储罐(尤其是在真空下)的长且昂贵的干燥周期。
在另一种实施方式中，上文所定义的所述多层结构体进一步包含位于密封层内的金属骨架。
该金属骨架不是防漏的，并且是最内层。
有利地，所述多层结构体进一步包含至少一个外层，尤其是金属层，所述层为所述多层结构体的最外层。
所述外层为第二增强层，但是为金属而非复合(复合材料)的。
在结构体上还可存在聚合物型保护层(最外层)，其具有抗磨损作用，或者其允许在结构体上放置铭文(inscription)。
关于纤维状材料
关于构成所述纤维状材料的纤维，它们特别为矿物、有机或植物纤维。
有利地，所述纤维状材料可为施胶的或未施胶的。
因此，所述纤维状材料可包含最高达0.1重量％的被称为施胶剂(sizing)的有机材料(热固性或热塑性树脂型)。
所述矿物纤维包括例如碳纤维、玻璃纤维、玄武岩或基于玄武岩的纤维、二氧化硅纤维、或碳化硅纤维。有机纤维包括基于热塑性或热固性聚合物的纤维，例如半芳族聚酰胺纤维、芳纶纤维、或聚烯烃纤维。优选地，它们是基于无定形热塑性聚合物的，并且具有如下的玻璃化转变温度Tg：该Tg高于构成预浸渍基体的聚合物或热塑性聚合物混合物的Tg(当后者为无定形的时)，或者该Tg高于构成预浸渍基体的聚合物或热塑性聚合物混合物的Tm(当后者为半结晶的时)。有利地，它们是基于半结晶热塑性聚合物的，并且具有如下的熔融温度Tm：该Tm高于构成预浸渍基体的聚合物或热塑性聚合物混合物的Tg(当后者为无定形的时)，或者该Tm高于构成预浸渍基体的聚合物或热塑性聚合物混合物的Tm(当后者为半结晶的时)。因而，对于构成纤维状材料的有机纤维而言，在被最终复合物的热塑性基体浸渍期间，不存在熔融风险。所述植物纤维包括天然亚麻，苎麻(hemp)，木质素，竹，丝特别是蜘蛛丝，剑麻，和其它纤维素纤维、特别是粘胶纤维。这些植物纤维可如下使用：纯的，经处理的，或涂覆有涂覆层，以促进热塑性聚合物机体的附着和浸渍。
纤维状材料还可为织物、编织物、或用纤维织成的。
其还可对应于具有支撑线(support thread)的纤维。
这些组成纤维(组分纤维，component fiber)可单独或以混合物使用。因而，有机纤维可与矿物纤维混合，以用热塑性聚合物粉末预浸渍并且形成经预浸渍的纤维状材料。
有机纤维线股可具有若干克重。它们可进一步具有若干几何形状。纤维状材料的组成纤维可进一步呈现这些具有不同几何形状的增强纤维的混合物的形式。所述纤维是连续纤维。
优选地，所述纤维状材料由如下组成：连续碳或玻璃纤维或其混合物，特别地碳纤维。其以粗纱或若干粗纱的形式使用。
根据另一方面，本发明涉及制造如上文所定义的多层结构体的方法，其特征在于，其包含将如上文所定义的增强层熔接至如上文所定义的密封层的步骤。
有利地，熔接步骤是通过选自激光、红外(IR)加热、LED加热、感应或微波加热、或高频(HF)加热的系统进行的。
有利地，所述方法包含将所述密封层挤出至金属骨架上的步骤和将增强层熔接至密封层上的步骤。
根据另一方面，本发明涉及选自储罐或管道或管路的多层结构体用于制备运输、分配或储存氢的储罐或管道或管路的用途，该多层结构体从内侧至外侧包含至少一个如上文所定义的密封层和至少一个如上文所定义的复合增强层，
所述最内的复合增强层熔接至所述最外的相邻密封层，
所述密封层由如下组合物组成：该组合物主要包含至少一种半结晶热塑性聚合物P1i(i＝1至n，n为密封层数)，其根据ISO 11357-3:2013测量的Tm小于280℃、特别地小于265℃，
各密封层的所述至少一种热塑性聚合物可为相同或不同的，并且所述复合增强层的至少一个由呈连续纤维形式的纤维状材料组成，所述纤维状材料浸渍有如下组合物：该组合物主要包含至少一种热塑性聚合物P2j(特别是半结晶的)，(j＝1至m，m为增强层数)，所述热塑性聚合物P2j具有根据ISO11357-3:2013测量的大于所述结构体的最大使用温度(Tu)的Tg，其中Tg≥Tu+20℃、特别地Tg≥Tu+30℃，Tu大于50℃、特别地大于100℃。
实施例
在所有实施例中，储罐均是通过衬垫在如下温度下的滚塑而获得的：该温度适应于所使用的热塑性树脂的性质，但是在所有情形中均低于280℃。
在环氧的情形中，则使用湿法长丝卷绕工艺，其由将纤维卷绕在衬垫周围而组成，该纤维在液体环氧浴中预浸渍。随后使储罐在烘箱中聚合2小时。
在所有其它情形中，使用预先浸渍有热塑性树脂的纤维状材料(带)。此带是使用具有1500W激光加热器的自动机、以12m/min的速度通过长丝卷绕而沉积的，并且不存在聚合步骤。
实施例1(对比实施例)
IV型氢储存储罐，其由T700SC31E(Toray所生产)碳纤维环氧复合增强物(Tg 80℃)和PA6密封层构成：两种树脂之间无混溶性(见表1)，其阻碍纤维状增强物和密封层之间的任何熔接。
实施例2(对比实施例)
IV型氢储存储罐，其由T700SC31E(Toray所生产)碳纤维环氧复合增强物(Tg 80℃)和HDPE密封层构成：两种树脂之间无混溶性(见表1)，其阻碍纤维状增强物和密封层之间的任何熔接。
实施例3：IV或V型氢储存储罐，其由T700SC31E(Toray所生产)BACT/10T碳纤维复合增强物和PA6密封层构成：两种树脂之间良好的部分混溶性(见表1)，其允许纤维状增强物和密封层之间的良好熔接。
选择的BACT/10T组合物具有283℃的熔融温度Tm，250℃的结晶温度Tc，和164℃的玻璃化转变温度。
Tg、Tc、和Tm分别是根据标准11357-2:2013和11357-3:2013通过差示扫描量热法(DSC)确定的。
实施例4：IV或V型氢储存储罐，其由T700SC31E(Toray所生产)BACT/10T碳纤维复合增强物和PA66密封层构成：两种树脂之间良好的部分混溶性(见表I)，其允许纤维状增强物和密封层之间的良好熔接。选择的BACT/10T组合物具有283℃的熔融温度Tm，250℃的结晶温度Tc，和164℃的玻璃化转变温度。Tg、Tc、和Tm分别是根据标准11357-2:2013和11357-3:2013通过差示扫描量热法(DSC)确定的。
与实施例3中的PA6衬垫(220℃)相比PA66衬垫更高的熔点(268.8℃)促进储罐的包扎(taping)和制造。
实施例5：IV或V型氢储存储罐，其由CT24-5.0/270-T140(SGL Carbon所生产)11/BACT/10T碳纤维复合增强物和PA11密封层构成：两种树脂之间良好的部分混溶性(见表1)，其导致纤维状增强物和密封层之间的良好熔接。选择的11/BACT/10T组合物具有280℃的熔融温度Tm，220℃的结晶温度Tc，和160℃的玻璃化转变温度。Tg、Tc、和Tm分别是根据标准11357-2:2013和11357-3:2013通过差示扫描量热法(DSC)确定的。
实施例6：IV或V型氢储存储罐，其由CT24-5.0/270-T140(SGL Carbon所生产)11/BACT/10T碳纤维复合增强物和PA11/10T密封层构成：两种树脂之间良好的部分混溶性(见表1)，其导致纤维状增强物和密封层之间的良好熔接。
选择的11/BACT/10T组合物具有280℃的熔融温度Tm，220℃的结晶温度Tc，和160℃的玻璃化转变温度。Tg、Tc、和Tm分别是根据标准11357-2:2013和11357-3:2013通过差示扫描量热法(DSC)确定的。
用于衬垫的11/10T组合物导致255℃的Tm。
使用具有255℃的熔点(接近用作复合物的基体的11/BACT/10T树脂的熔点)的11/10T衬垫促进储罐的加工。
实施例7：IV或V型氢储存储罐，其由CT24-5.0/270-T140(SGL Carbon所生产)11/BACT碳纤维复合增强物和PA11密封层构成：两种树脂之间良好的部分混溶性(见表1)，其导致纤维状增强物和密封层之间的良好熔接。选择的11/BACT组合物具有278℃的熔融温度Tm，210℃的结晶温度Tc，和157℃的玻璃化转变温度。Tg、Tc、和Tm分别是根据标准11357-2:2013和11357-3:2013通过差示扫描量热法(DSC)确定的。
使用缓慢结晶的11/BACT聚合物允许与此前实施例的11/BACT/10T相比更低的包扎温度，并且便于PA11衬垫的使用。
实施例8：IV或V型氢储存储罐，其由CT24-5.0/270-T140 T140(SGL Carbon所生产)11/BACT碳纤维复合增强物和PA11/10T密封层构成：两种树脂之间良好的部分混溶性(见表1)，其导致纤维状增强物和密封层之间的良好熔接。
选择的11/BACT组合物具有278℃的熔融温度Tm，210℃的结晶温度Tc，和157℃的玻璃化转变温度。Tg、Tc、和Tm分别是根据标准11357-2:2013和11357-3:2013通过差示扫描量热法(DSC)确定的。
用于衬垫的11/10T组合物导致255℃的Tm。
使用具有255℃的熔点(接近作为复合物的增强树脂的11/BACT)的11/10T衬垫促进储罐的实施。
在以下表1中的所有实施例中，为了评估树脂的混溶性，由具有约150μm的粒度的粉末在微型DSM上以在熔融之后1分钟的再流通时间制造混合物。所有混合物均在300℃下制造，环氧树脂-聚乙烯混合物除外，其是在220℃下制造的。
在混合过程结束时，将混合物注入模具中，以制造测试件，该测试件将在DMA中表征。
表1
Figure BDA0003495039790000191
Figure BDA0003495039790000201
***Tg测量是根据ISO 4664-1通过DMTA完成的
混溶性测试结果：
-第4列：各树脂在混合之前的玻璃化转变温度
-第5列：树脂在混合物中的玻璃化转变温度
-第6列：树脂在混合物中和在混合之前的玻璃化转变温度的差异之间的比率。
100％表明树脂的不混溶性，
<80％表明低混溶性，
<30％表明良好但是部分的混溶性，
0表明完全混溶性。

Claims (23)

1.多层结构体，其选自旨在运输、分配、或储存氢的储罐、管道或管路，其从内侧至外侧包含至少一个密封层和至少一个复合增强层，
所述最内的复合增强层熔接至所述最外的相邻的密封层，
所述密封层由如下组合物组成：该组合物主要包含至少一种半结晶热塑性聚合物P1i(i＝1至n，n为密封层数)，其根据ISO 11357-3:2013测量的Tm小于280℃、特别地小于265℃，
各密封层的所述至少一种热塑性聚合物可为相同或不同的，并且所述复合增强层的至少一个由呈连续纤维形式的纤维状材料组成，所述纤维状材料浸渍有如下组合物：该组合物主要包含至少一种热塑性聚合物P2j，(j＝1至m，m为增强层数)、特别是半结晶热塑性聚合物P2j，所述热塑性聚合物P2j具有根据ISO 11357-3:2013测量的大于所述结构体的最大使用温度(Tu)的Tg，其中Tg≥Tu+20℃、特别地Tg≥Tu+30℃，Tu大于50℃、特别地大于100℃。
2.根据权利要求1的多层结构体，其中各增强层的各聚合物P1i是与相邻层的各聚合物P1i部分或完全能混溶的，各增强层的各聚合物P2j是与相邻层的各聚合物P2j部分或完全能混溶的，并且聚合物P21是与和其相邻的聚合物P11部分或完全能混溶的，
所述聚合物的完全或部分混溶性是通过两种树脂在混合物中的玻璃化转变温度的差异相对于两种树脂在混合之前的玻璃化转变温度的差异来定义的，当所述差异等于0时混溶性为完全的，并且当所述差异不同于0时混溶性为部分的。
3.根据权利要求1或2之一的多层结构体，其特征在于，各密封层包含相同类型的聚合物、特别地聚酰胺。
4.根据权利要求1或2之一的多层结构体，其特征在于，各增强层包含相同类型的聚合物、特别地聚酰胺。
5.根据权利要求3或4之一的多层结构体，其特征在于，各密封层包含相同类型的聚合物、特别地聚酰胺，并且各增强层包含相同类型的聚合物、特别地聚酰胺。
6.根据权利要求1至5之一的多层结构体，其特征在于，其具有单一密封层和单一增强层。
7.根据权利要求1至6之一的多层结构体，其特征在于，所述结构体为储罐或柔性管道。
8.根据权利要求1至7之一的多层结构体，其特征在于，包含所述聚合物P1和P2的所述组合物还包含使得它们能够吸收适合于熔接的辐射的添加剂，诸如炭黑、碳纳米管(CNT)、或石墨烯。
9.根据权利要求1至8之一的多层结构体，其特征在于，包含所述聚合物P2j的所述组合物是对适合于熔接的辐射透明的。
10.根据权利要求8或9之一的多层结构体，其特征在于，熔接是通过选自激光、红外(IR)加热、LED加热、感应或微波加热、或高频(HF)加热的系统实施的。
11.根据权利要求1至10之一的多层结构体，其特征在于，所述聚合物P1i为聚酰胺。
12.根据权利要求1至10之一的多层结构体，其特征在于，所述聚合物P2j为聚酰胺。
13.根据权利要求11或12之一的多层结构体，其特征在于，所述聚合物P1i和所述聚合物P2j为聚酰胺。
14.根据权利要求11或13的多层结构体，其特征在于，所述聚合物P1i为长链脂族聚酰胺，特别地PA1010、PA 1012、PA 1212、PA11、PA12，尤其是PA 11或PA12；或者半芳族的，尤其是PA 11/5T、PA 11/6T、和PA11/10T。
15.根据权利要求12或13的多层结构体，其特征在于，所述聚合物P2j为半芳族聚酰胺，特别地选自PA MPMDT/6T、PA 11/10T、PA 11/BACT、PA 5T/10T、PA 11/6T/10T、PA MXDT/10T、PA MPMDT/10T、PA BACT/10T、PA BACT/6T、PA BACT/10T/6T、PA 11/BACT/6T、PA 11/MPMDT/6T、PA 11/MPMDT/10T、PA 11/BACT/10T、PA 11/MXDT/10T、PA11/5T/10T。
16.根据权利要求13至15之一的多层结构体，其特征在于，所述聚合物P1i为长链脂族聚酰胺，特别地PA1010、PA 1012、PA 1212、PA11、PA12，或者半芳族的，特别地PA 11/5T、或PA 11/6T、或PA 11/10T，尤其是PA11或PA12；并且所述聚合物P2j为半芳族聚酰胺，特别地选自PA MPMDT/6T、PA PA11/10T、PA 11/BACT、PA 5T/10T、PA 11/6T/10T、PA MXDT/10T、PAMPMDT/10T、PA BACT/10T、PA BACT/6T、PA BACT/10T/6T、PA 11/BACT/6T、PA 11/MPMDT/6T、PA 11/MPMDT/10T、PA 11/BACT/10T、PA 11/MXDT/10T、PA11/5T/10T。
17.根据权利要求1至16之一的多层结构体，其特征在于，其具有减压耐受性和干燥能力。
18.根据权利要求1至17之一的多层结构体，其特征在于，所述结构体进一步包含位于密封层内的金属骨架。
19.根据权利要求1至18之一的多层结构体，其特征在于，所述结构体进一步包含至少一个外层，特别是金属层，所述层为所述多层结构体的最外层。
20.根据权利要求1至19之一的多层结构体，其特征在于，所述纤维状材料选自玻璃纤维和碳纤维或玄武岩纤维或基于玄武岩的纤维。
21.用于制造如权利要求1至20之一中所定义的多层结构体的方法，其特征在于，其包含将如权利要求1中所定义的增强层熔接至如权利要求1中所定义的密封层的步骤。
22.根据权利要求21的方法，其特征在于，熔接步骤是通过选自激光、红外(IR)加热、LED加热、感应或微波加热、或高频(HF)加热的系统实施的。
23.根据权利要求21或22的方法，其特征在于，其包含将所述密封层挤出至金属骨架上的步骤和将增强层熔接至密封层上的步骤。
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