CN113784997A - 适合用作板绝热材料的硬质聚氨酯泡沫 - Google Patents
适合用作板绝热材料的硬质聚氨酯泡沫 Download PDFInfo
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- CN113784997A CN113784997A CN202080032218.9A CN202080032218A CN113784997A CN 113784997 A CN113784997 A CN 113784997A CN 202080032218 A CN202080032218 A CN 202080032218A CN 113784997 A CN113784997 A CN 113784997A
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- isocyanate reactive
- reactive composition
- polyol
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Abstract
公开的是聚氨酯泡沫形成组合物、硬质聚氨酯泡沫及其制备方法,以及包含夹在饰面基材之间的这种泡沫的复合制品,包括这种复合元件用于冷藏牵引拖车的地板绝热元件的用途。该硬质聚氨酯泡沫由包含(1)多元醇共混物;(2)氢氯氟烯烃;和(3)叔胺催化剂组合物的异氰酸酯反应性组合物制备。
Description
技术领域
本说明书总体上涉及硬质聚氨酯泡沫形成组合物、硬质聚氨酯泡沫及其制备方法,以及涉及包含夹在饰面基材之间的这种泡沫的复合制品,包括这种复合元件用于冷藏牵引拖车的地板绝热元件的用途。硬质聚氨酯泡沫由异氰酸酯反应性组合物制备,该异氰酸酯反应性组合物包含:(1)多元醇共混物;(2)氢氯氟烯烃(hydrochlorofluoroolefin)("HCFO");和(3)叔胺催化剂组合物。
背景技术
硬质聚氨酯泡沫用于许多行业中。其是通过使合适的多异氰酸酯与异氰酸酯反应性化合物(通常是多元醇)在发泡剂的存在下反应来制备的。这种泡沫的一种用途是作为冷藏储存设备的结构中的绝热介质。闭孔硬质泡沫的绝热性能取决于多种因素,包括平均泡孔大小和泡孔内容物的导热性。由于氯氟烃(“CFC”)的蒸气热导率格外低,其通常用作发泡剂来制备这些泡沫。然而,CFC目前已知是平流层中臭氧消耗的原因之一,并且因此已经颁布了禁止其使用的法令。
起初,CFC的最有前途的替代物似乎是含氢氯氟烃(HCFC)。虽然HCFC诸如HCFC141b已经被用作CFC的替代物,但其也被发现具有一些臭氧消耗的可能性。因此,需要找到HCFC以及CFC的替代品。
替代的发泡剂,如氢氟烃(“HFC”),也替代了CFC。然而,该化合物是温室气体。还使用了诸如戊烷异构体等烃类,但是这些化合物易燃并且能量效率较低。含氢卤代烯烃化合物(如,HCFO)是作为HFC的替代物的可能候选者,因为其在较低层大气中的化学不稳定性提供了低的全球变暖潜势和零臭氧消耗或近零臭氧消耗。
然而,在令人满意的异氰酸酯基泡沫的制备中,作为发泡剂的一些HCFO的缺点是保存期限问题。发泡剂通常与多元醇和其他组分诸如一种或多种表面活性剂和一种或多种催化剂混合,以形成所谓“B方”预混物,该预混物在与“A方”异氰酸酯组分混合形成泡沫之前可能贮藏长达若干月。使用某些HCFO的体系的缺点是B方组合物的保存期限。如果B方组合物在与多异氰酸酯混合之前老化,则泡沫可能具有较低的质量并且甚至可能在形成期间塌陷。不良泡沫结构被认为是归因于某些催化剂与这些HCFO的反应,该反应导致发泡剂的部分分解并因此导致硅酮表面活性剂不合期望的改变,导致不良的泡沫结构和质量。
用于生产不连续板绝热材料(诸如用于冷藏拖车地板的绝热物)的泡沫形成组合物必须展现出严格的性能组合。举例来说,除良好的绝热性能之外,其必须展现出有益于所使用的制造设备和制造方法的目标胶凝时间,并且其必须展现出长的保存期限,这意味着在泡沫形成组合物各组分长期(数月或更久)储存之后——甚至是在以基于异氰酸酯反应性组合物的总重量计,2重量%或更多的量来使用水作为发泡剂组分时——该胶凝时间也不会发生大幅度改变。其还必须展现出良好的尺寸稳定性(低的泡沫收缩率)——甚至在自由发泡泡沫具有1.4至1.7lb/ft3(22.4to 27.2kg/m3)的相对低的密度时亦是如此。此外,重要的是,泡沫与通常用于冷藏拖车地板应用中的饰面基材(如,铝)粘附良好。而且,因为拖车地板部件经常在没有压力的情况下发泡,因此在发泡期间泡沫不产生高压可能是重要的。最后,重要的是泡沫表现出低脆性,即,对易破碎或破碎成小块的倾向低,同时保持良好的尺寸稳定性(尺寸稳定性通常随着体系官能度的增加而改善,但通常这会以脆性增加为代价)。降低泡沫脆性可以改善泡沫对饰面基材的粘附力,这允许更早地脱模,从而提高生产率。
因此,能够满足这些要求中的大多数(甚至全部)、同时又使用含HCFO发泡剂的组合物将是非常符合期望的。
发明内容
在某些方面,本公开涉及异氰酸酯反应性组合物。这些异氰酸酯反应性组合物包含:(a)多元醇共混物;(b)发泡剂组合物;和(c)叔胺催化剂组合物。多元醇共混物包含:(1)基于多元醇共混物总重量计,30至98重量%的糖引发的聚醚多元醇,该糖引发的聚醚多元醇具有200至600mg KOH/g的OH值和4至6的官能度;(2)基于多元醇共混物总重量计,1至40重量%的聚环氧烷二醇,该聚环氧烷二醇具有1.9至2.0的官能度和20至120mg KOH/g的OH值;和(3)基于多元醇共混物的总重量计,1至20重量%的烷醇胺引发的聚醚多元醇,该烷醇胺引发的聚醚多元醇具有至少500mg KOH/g的OH值和2.5至4的官能度。发泡剂组合物包括:(1)HCFO;和(2)产生二氧化碳的化学发泡剂。
本说明书还涉及由这种组合物制备的硬质聚氨酯泡沫、制备这种硬质泡沫的方法、包括这种硬质泡沫的复合制品、包括这种复合元件作为地板绝热物的冷藏拖车,以及相关的泡沫形成组合物。
具体实施方式
本说明书中描述和示例说明了各种实施方案来提供对所公开的发明的结构、功能、性能以及用途的全面理解。要理解的是,本说明书中所说明的各种实施方案是非限制性且非穷举的。因此,本发明不被本说明书中对各种非限制性且非穷举的实施方案的说明所限制。结合各种实施方案来说明的特征和特性可以与其他实施方案的特征和特性组合。这样的改变和变化意在被包括在本说明书的范围内。同样,可以修改权利要求来记述本说明书中清楚地或内在地描述的、或以其他方式清楚地或内在地得到本说明书支持的任何特征或特性。而且,申请人拥有修改权利要求以肯定地放弃可能在现有技术中存在的特征或特性的权利。因此,任何这样的修改都符合35U.S.C.§112和35U.S.C.§132(a)要求。本说明书中公开和说明的各种实施方案可包括本文多方面描述的特征和特性、由本文多方面描述的特征和特性组成,或者基本上由本文多方面描述的特征和特性组成。
除非另有说明,本文所提及的任何专利、出版物或其他公开材料通过引用而以其整体并入本说明书中,但仅限于所并入的材料不与现行定义、声明或本说明书中所提出的其他公开材料发生抵触的程度。同样,且在必要的程度上,本说明书中所述的明确公开内容代替任何发生抵触的、通过引用而被并入本文的材料。据称是通过引用被并入本说明书、但与现行定义、声明或本文中所提出的其他公开材料相抵触的任何材料或其部分仅以并入的材料与现有公开材料之间不存在抵触的程度被并入。申请人拥有修改本说明书以明确记述通过引用被并入本文的任何发明主题或其部分的权利。
在本说明书中,除了另有说明之处,所有数值参数在任何情况下均应被理解为是以术语“约”来开头和修饰的,其中数值参数具有用于确定参数数值的基础测量技术的固有的可变特性。至少,并且不试图限制等同原则应用于权利要求的范围,在本说明书中描述的每个数值参数应至少根据所报告的有效数字的量值并通过应用普通的舍入技术来解释。
并且,本说明书中所列举的任何数值范围意在包括被归入所列举范围内的同一数值精确度的所有子范围。例如,范围“1.0至10.0”意在包括所列举的最小值1.0和所列举的最大值10.0之间(并包括所列举的最小值1.0和所列举的最大值10.0)的所有子范围,即具有大于等于1.0的最小值和小于等于10.0的最大值,比如,2.4至7.6。本说明书中所列举的任何最大限值旨在包括其中所包含的所有较小限值,并且本说明书中所列举的任何最小限值旨在包括其中所包含的所有较大限值。因此,申请人拥有修改该说明书——包括权利要求书——以明确记述包含在本文中所明确记述的各个范围之内的任何子范围的权利。所有这样的范围意在固有地描述于本说明书中,从而明确记述任何这样的子范围的修改都将符合35U.S.C.§112和35U.S.C.§132(a)的规定。
除非另有说明,如本说明书中所使用的文法上的冠词“一个”、“一种”、和“所述/该”意在包括“至少一个/种”或“一个/种或多个/种”。因此,本说明书中使用冠词来指代一个/种或多于一个/种(即,指代“至少一个/种”)该冠词在文法上的宾语。举例来说,“一种组分”意为一种或多种组分,并且因此可能的是,多于一种组分被设想并可能在所描述的实施方案的实现中被采用或使用。而且,使用单数名词包括复数,并且使用复数名词包括单数,除非该用法的上下文中另有要求。
如本文中所使用的,术语“官能度”是指每分子正在被描述的多元醇或多元醇共混物所存在的反应性羟基(–OH)的平均数。在聚氨酯泡沫的制备中,羟基与连接于多异氰酸酯的异氰酸酯基团(–NCO)反应。术语“羟值”是指可供反应的反应性羟基数,并且被表述为等同于一克多元醇的羟基含量的氢氧化钾毫克数(ASTM D4274-16)。术语“当量”是指化合物重量除以其化合价。对于多元醇,当量是与异氰酸酯基团化合的多元醇的重量,并且可通过多元醇的摩尔质量除以其官能度来计算。多元醇的当量还可通过56,100除以多元醇的羟值来计算——当量(g/eq)=(56.1x 1000)/OH值。
正如所说明的,本说明书的某些实施方案涉及制备硬质泡沫。硬质泡沫的特征在于,抗压强度与拉伸强度之比为至少0.5:1,伸长率小于10%,以及变形恢复率低且弹性限度低,正如在“Polyurethanes:Chemistry and Technology,Part II Technology”,J.H.Saunders&K.C.Frisch,Interscience Publishers,1964,第239页中所述。
在一些实施方案中,本说明书涉及包括多元醇共混物的异氰酸酯反应性组合物。更特别地,在某些实施方案中,多元醇共混物包括基于所述多元醇共混物的总重量计,30至98重量%,如40至98重量%,50至98重量%,60至90重量%,或者,在一些情况下,70至90%的糖引发的聚醚多元醇,该糖引发的聚醚多元醇具有200至600mg KOH/g的OH值和4至6的官能度。
如本文中所使用的,“糖引发的聚醚多元醇”是指通过使至少一种环氧烷烃与一种或多种合适的引发剂化合物在合适的催化剂的存在下反应来制备的聚醚多元醇,其中引发剂化合物包括一种或多种糖。合适的环氧烷烃的例子包括环氧乙烷、环氧丙烷、环氧丁烷、氧化苯乙烯、表氯醇或其混合物等。合适的糖引发剂的一些例子是蔗糖、山梨糖醇、麦芽糖醇及其混合物,以及其他单糖、二糖、三糖和多糖。其他引发剂化合物经常与糖引发剂一起使用来制备糖引发的聚醚多元醇。糖可以与例如,诸如水、丙二醇、甘油、乙二醇、乙醇胺、二乙二醇的化合物及其混合物共引发,以形成糖引发的聚醚多元醇。正如将被理解的,可以将多种单独的引发剂化合物彼此组合使用,其中单独的引发剂化合物的官能度不落入本文中所述的官能度,前提是引发剂化合物的混合物的平均官能度能满足本文所公开的总官能度范围。
可使用的合适的催化剂的一些例子包括碱性催化剂(诸如,氢氧化钠或氢氧化钾,或叔胺如甲基咪唑)和双金属氰化物(DMC)催化剂。
在一些实施方案中,糖引发的聚醚多元醇具有200至600mg KOH/g,如300至550mgKOH/g,如350至450mg KOH/g,或者在一些情况下,360至400mg KOH/g的OH值,和4至6,如4至5,或4.0至4.5的官能度。
如前文所述,本说明书的异氰酸酯反应性组合物中所包括的多元醇共混合物的实施方案还包括,基于多元醇共混物总重量计,1至40重量%,如1至20重量%,或者,在一些情况下,10至20重量%的聚环氧烷二醇,该聚环氧烷二醇官能度为1.9至2.0,如1.98至2.00,且OH值为20至120mg KOH/g,如20至80mg KOH/g,20至40mg KOH/g,或20至30mg KOH/g。这样的聚环氧烷二醇还可具有例如1000至5600g/mol,如2800至5600g/mol或3700至5600g/mol的数均分子量。
合适的聚环氧烷二醇包括可通过一种或多种环氧烷烃如环氧乙烷、环氧丙烷、环氧丁烷等与一种或多种二醇如乙二醇、二乙二醇、丙二醇以及乙二醇和/或丙二醇的其他低聚物之间的加成聚合所获得的产物。在一些实施方案中,环氧烷烃包括环氧丙烷和/或环氧乙烷或者在一些情况下由环氧丙烷和/或环氧乙烷组成,和/或二醇包括丙二醇或者在一些情况下由丙二醇组成。
在一些实施方案中,聚环氧烷二醇,如聚环氧丙烷二醇,是用双金属氰化物催化剂(DMC催化剂)而并非通常的氢氧化钾来制备的,并且因此,在一些情况下,可比使用氢氧化钾作为催化剂制得的那些聚环氧烷二醇呈现出更大的OH官能度和更低的一元醇含量。
这样的聚醚多元醇可通过在DMC催化剂如六氰钴酸锌的存在下,于130℃,例如使用WO 97/29,146(实施例1至5)中所述的方法,逐步加入引发剂而制备。
在某些实施方案中,上述糖引发的聚醚多元醇和上述聚环氧烷二醇以至少2:1,如2:1至10:1,3:1至7:1,或者4:1至6:1的重量比存在于多元醇共混物中。
如前文所述,本说明书的异氰酸酯反应性组合物的多元醇共混物包括烷醇胺引发的聚醚多元醇。如本文所使用的,“烷醇胺引发的聚醚多元醇”是指在合适的催化剂存在下,通过至少一种环氧烷与一种或多种合适的引发剂化合物反应制备的聚醚多元醇,其中引发剂化合物包括一种或多种烷醇胺。合适的催化剂包括碱性催化剂(如,氢氧化钠或氢氧化钾,或叔胺如甲基咪唑)和DMC催化剂。本文所述的多元醇共混物中,所述聚醚多元醇——包括“烷醇胺引发的聚醚多元醇”和“脂族胺引发的聚醚多元醇”——各自是彼此不同的。
如本文所使用的,术语“烷醇胺”是指由下式表示的化合物:
NH2—Z—OH
其中Z表示二价基团,该二价基团是具有2至6个碳原子的直链或支链的亚烷基、具有4至6个碳原子的亚环烷基,或具有4至6个碳原子的二亚烷基醚基。该二亚烷基醚基可由如下化学式表示:
—R—O—R—
其中每个R表示具有2至3个碳原子的烃基。
可用于制备烷醇胺引发的聚醚多元醇的合适的烷醇胺的具体例子包括单乙醇胺、1-氨基-2-丙醇、2-氨基-l-丙醇、3-氨基-l-丙醇、1-(2-氨基乙氧基)乙醇、1-氨基-2-丁醇、2-氨基-3-丁醇、2-氨基-2-甲基丙醇、5-氨基戊醇、3-氨基-2,2-二甲基丙醇、4-氨基环己醇,以及其两种以上的混合物。
为制备烷醇胺引发的聚醚多元醇,使烷醇胺与环氧烷烃反应。合适的环氧烷烃包括环氧乙烷、环氧丙烷、环氧丁烷、氧化苯乙烯和表氯醇,以及其任意两种以上的混合物。
在一些实施方案中,烷醇胺引发的聚醚多元醇具有具有至少500mg KOH/g,如500至900mg KOH/g,600至800mg KOH/g,或在一些情况下,680至720mg KOH/g的OH值,和2.5至4,如2.5至3.5的官能度。
在一些实施方案中,烷醇胺引发的聚醚多元醇以1至20重量%,如1至10重量%或2至10重量%的量使用,基于所述多元醇共混物的总重量计。
在一些实施方案中,上述糖引发的聚醚多元醇和烷醇胺引发的聚醚多元醇以至少5:1,如10:1至25:1或15:1至25:1的重量比存在于多元醇共混物中。在某些实施方案中,聚环氧烷二醇和烷醇胺引发的聚醚多元醇以至少1:1,如1:1至10:1,1:1至5:1,或在一些情况下2:1至4:1的重量比存在于所述多元醇共混物中。
出乎意料地发现,在本说明书中所述的异氰酸酯反应性组合物中以上述范围之内的量包括烷醇胺引发的聚醚多元醇,能够制备保存期限稳定的异氰酸酯反应性组合物,该异氰酸酯反应性组合物可以制备这样的硬质聚氨酯泡沫:与由不包含此类烷醇胺引发的聚醚多元醇的类似异氰酸酯反应性组合物生产的泡沫相比,该硬质聚氨酯泡沫的脆性大大降低(导致饰面粘附力大大提高)。目前认为,这样的改善的饰面粘附力允许更快的脱模,从而提高生产率。
如果需要,多元醇共混物可包括含异氰酸酯反应性基团的另外的化合物。举例来说,在一些实施方案中,多元醇共混物还可包括脂族三醇引发的聚醚多元醇,所述脂族三醇引发的聚醚多元醇具有100至500mg KOH/g,如200至400mgKOH/g,200至300mg KOH/g,200至250mg KOH/g,230至250mg KOH/g或233至243mg KOH/g的OH值,和大于2至4,如2.5至3.5,或在一些情况下,3.0的官能度。
这样的聚醚多元醇可通过使合适的脂族二价、三价和/或多价醇(例如,乙二醇、1,2-丙二醇和1,3-丙二醇、二乙二醇、二丙二醇、1,4-丁二醇、1,6-己二醇和甘油)发生反应来制备,条件是使用至少一种脂族三价醇(如,甘油)。在一些实施方案中,多价醇引发剂包括甘油,或者在一些情况下由甘油组成,并且环氧烷烃包括环氧丙烷,或者在一些情况下,由环氧丙烷组成。
如果需要,多元醇共混物可包括具有异氰酸酯反应性基团的其他化合物,如扩链剂和/或交联剂,以及上文未述及的更高分子量的聚醚多元醇和聚酯多元醇。扩链剂和/或交联剂包括,例如,乙二醇、丙二醇、丁二醇、甘油、二乙二醇、二丙二醇、二丁二醇、三羟甲基丙烷、季戊四醇、乙二胺和二乙基甲苯二胺。聚酯多元醇可由例如,具有2至12个碳原子的有机二羧酸如具有4至6个碳原子的脂族二羧酸,和多价醇如具有2至12个碳原子的二醇或三醇来制备。二羧酸的例子是琥珀酸、戊二酸、己二酸、辛二酸、壬二酸、癸二酸、癸二羧酸、马来酸、富马酸、邻苯二甲酸、间苯二甲酸和对苯二甲酸。作为游离二羧酸的替代,可以使用相应的二羧酸衍生物,如由具有1至4个碳原子的醇酯化制备的二羧酸单酯或二酯或者二羧酸酸酐。
在某些实施方案中,多元醇共混物具有4至6,如4.5至4.5或4.5至5.0的加权平均官能度,和/或300至500mg KOH/g,如300至400mg KOH/g,或320至360mg KOH/g的加权平均羟值,和/或大于800至1600g/mol,如1000至1400g/mol或1200至1300g/mol的加权平均分子量。
如所述,本说明书的异氰酸酯反应性组合物还包括发泡剂组合物。发泡剂组合物包括:(1)包括HCFO的物理发泡剂;和(2)产生二氧化碳的化学发泡剂。
合适的HCFO包括1-氯-3,3,3-三氟丙烯(HCFO-1233zd,E和/或Z异构体)、2-氯-3,3,3-三氟丙烯(HCFO-1233xf)、HCFO1223、1,2-二氯-1,2-二氟乙烯(E和/或Z异构体)、3,3-二氯-3-氟丙烯、2-氯-1,1,1,4,4,4-六氟-2-丁烯(E和/或Z异构体)、2-氯-1,1,1,3,4,4,4-七氟-2-丁烯(E和/或Z异构体)。在一些实施方案中,HCFO在大气压下的沸点是至少-25℃,至少-20℃,或在一些情况下,至少-19℃,以及40℃或更低,如35℃或更低,或在一些情况下33℃或更低。HCFO在大气压下可具有例如-25℃至40℃,或-20℃至35℃,或-19℃至33℃的沸点。
在一些实施方案中,HCFO以至少10重量%,如10至30重量%,或10至20重量%的量使用,基于所述异氰酸酯反应性组合物的总重量计。
在一些实施方案中,异氰酸酯反应性组合物包括一种或多种其他物理发泡剂,如其他卤代发泡剂,诸如CFC、HCFC和/或HFC,和/或烃类发泡剂,诸如丁烷、正戊烷、环戊烷、己烷和/或异戊烷(即2-甲基丁烷)。在其他实施方案中,异氰酸酯反应性组合物基本不含或在一些情况下完全不含其他物理发泡剂,如其他卤代发泡剂(诸如CFC、HCFC和/或HFC)和/或烃类发泡剂(诸如丁烷、正戊烷、环戊烷、己烷和/或异戊烷(即2-甲基丁烷))。如本文中所使用的,术语“基本不含”在用于提及这些发泡剂时,意为发泡剂(如果有的话)是以基于发泡剂组合物的总重量计,少于10重量%,如少于1重量%的量存在的。
如上文所述,异氰酸酯反应性组合物包括产生二氧化碳的化学发泡剂,如水,和/或甲酸酯封端的胺。
在一些这样的实施方案中,产生二氧化碳的化学发泡剂,如水,以0.5至5.0重量%,如1至4重量%,或1.0至3.0重量%,或2.0至3.0重量%的量使用,基于所述异氰酸酯反应性组合物的总重量计。
在一些实施方案中,发泡剂组合物包括HCFO和产生二氧化碳的化学发泡剂,如水,其中HCFO和产生二氧化碳的化学发泡剂以至少90重量%,至少95重量%,或在一些情况下至少99重量%的量存在,基于所述异氰酸酯反应性组合物的总重量计。在一些实施方案中,HCFO和产生二氧化碳的化学发泡剂以至少2:1,如至少4:1,如4:1至10:1,或6:1至10:1的重量比存在于所述发泡剂组合物中。
如果需要,发泡剂组合物可包括其他物理发泡剂,如(a)其他氢氟烯烃(HFO),如五氟丙烷、四氟丙烷、2,3,3,3-四氟丙烷、1,2,3,3-四氟丙烷、三氟丙烷、四氟丁烷、五氟丁烷、六氟丁烷、七氟丁烷、七氟丙烷、八氟丙烷和九氟丙烷;(b)氢氟烃;(c)烃,如任何戊烷异构体和丁烷异构体;(d)氢氟醚(HFE);(e)C1至C5醇、C1至C4醛、C1至C4酮、C1至C4醚和二氧化碳。美国专利申请公开No.US 2014/0371338 A1在[0051]和[0053]记载了这样的发泡剂的具体例子,其引用部分通过引证并入本文。
在一些实施方案中,异氰酸酯反应性组合物还包括表面活性剂。可使用任何合适的表面活性剂,包括有机硅化合物,如聚硅氧烷-聚烯烃-嵌段共聚物,如聚醚改性的聚硅氧烷。其他有用的表面活性剂包括长链醇的聚乙二醇醚、长链烷基酸硫酸酯、烷基磺酸酯或烷基芳基磺酸的叔胺或烷醇胺盐。以这样的量来使用这样的表面活性剂:该量足以稳定发泡反应混合物,以免坍塌和形成大而不均匀的泡孔。在一些实施方案中,表面活性剂以基于异氰酸酯反应性组合物的总重量计,0.2至5.0重量%,如1至3重量%的量来使用。
如前文所述,异氰酸酯反应性组合物还包括叔胺催化剂组合物。正如将理解的,叔胺催化剂被称为“发泡催化剂”,因为它们对水-多异氰酸酯发泡反应起到较大作用。在一些实施方案中,叔胺催化剂包括吗啉和/或咪唑。此外,在一些实施方案中,叔胺催化剂组合物包括:(i)基于叔胺催化剂组合物总重量计,80至99重量%,如90至99重量%,或者在一些情况下95至98重量%或97至98重量%的吗啉;和(ii)基于叔胺催化剂组合物总重量计,1至20重量%,如1至10重量%,或者在一些情况下2至5重量%或2至3重量%的咪唑。
合适的吗啉催化剂包括,例如,二吗啉二乙醚、二吗啉二甲醚、N-乙基吗啉和N-甲基吗啉。合适的咪唑催化剂包括,例如,咪唑、N-甲基咪唑和1,2-二甲基咪唑。在一些实施方案中,吗啉催化剂包括两种以上吗啉催化剂的混合物,如二吗啉二乙醚与N-甲基吗啉的混合物,其中例如基于吗啉催化剂的总重量用量计,二吗啉二乙醚以30至80重量%,如40至80重量%的量使用,而N-甲基吗啉以20至70重量%,如20至60重量%的量使用。
在某些实施方案中,叔胺催化剂组合物不包括酸封端的胺催化剂。在某些实施方案中,异氰酸酯反应性组合物不包括金属催化剂和/或不为叔胺催化剂的任何其他催化剂。
在某些实施方案中,异氰酸酯反应性组合物中所使用的叔胺催化剂的总量为基于异氰酸酯反应性组合物的总重量计,1至5重量%,如1.0至3.0%或1.5至2.5重量%。
可以可选地包括在本发明的泡沫形成组合物中的另外的原料包括:颜料、着色剂、填料、抗氧化剂、阻燃剂和稳定剂。适用于本发明的泡沫形成组合物的示例性的阻燃剂包括,但不限于,基于反应性溴的化合物和氯化磷酸酯,包括但不限于磷酸三(2-氯乙基)酯(TECP)、磷酸三(1,3-二氯-2-丙基)酯、磷酸三(1-氯-2-丙基)酯(TCPP)和二甲基丙基磷酸酯(DMPP)。
正如将被理解的,本说明书的其他实施方案涉及硬质聚氨酯泡沫形成组合物,其包括:(a)二异氰酸酯和/或多异氰酸酯(统称为“多异氰酸酯”);和(b)上述类型的异氰酸酯反应性组合物。
可使用已知的有机多异氰酸酯、改性多异氰酸酯或由任何已知有机异氰酸酯制得的异氰酸酯封端的预聚物中的任一者。合适的有机异氰酸酯包括芳族、脂族和脂环族多异氰酸酯及其组合。有用的多异氰酸酯包括:二异氰酸酯,如间苯二异氰酸酯、对苯二异氰酸酯、2,4-甲苯二异氰酸酯、2,6-甲苯二异氰酸酯、1,6-己二异氰酸酯、1,4-己二异氰酸酯、1,3-环己烷二异氰酸酯、1,4-环己烷二异氰酸酯、六氢甲苯二异氰酸酯的各种异构体、异氟尔酮二异氰酸酯、二环己基甲烷二异氰酸酯、1,5-萘二异氰酸酯、4,4′-二苯基甲烷二异氰酸酯、2,4′-二苯基甲烷二异氰酸酯、4,4′-联苯二异氰酸酯、3,3′-二甲氧基-4,4′-联苯二异氰酸酯和3,3′-二甲基二苯基丙烷-4,4′-二异氰酸酯;三异氰酸酯,如2,4,6-甲苯三异氰酸酯;和多异氰酸酯,如4,4′-二甲基二苯基甲烷-2,2′,5,5′-四异氰酸酯和多亚甲基多苯基多异氰酸酯。
也可使用未经蒸馏的或粗多异氰酸酯。由甲苯二胺混合物光气化获得的粗甲苯二异氰酸酯和由粗二苯基甲烷二胺光气化获得的粗二苯基甲烷二异氰酸酯(聚合MDI)是合适的粗多异氰酸酯的例子。合适的未经蒸馏的或粗多异氰酸酯公开在U.S.Pat.No.3,215,652中。
改性的多异氰酸酯由多异氰酸酯的化学反应获得。有用的改性多异氰酸酯包括,但不限于,含有酯基、脲基、缩二脲基、脲基甲酸酯基、碳二亚胺基、异氰脲酸酯基、缩脲二酮基和/或尿烷基的那些。改性多异氰酸酯的例子包括含有NCO基并具有25至35重量%(如,29至34重量%)的NCO含量的预聚物,诸如基于聚醚多元醇或聚酯多元醇与二苯基甲烷二异氰酸酯的那些预聚物。
在某些实施方案中,归因于使聚氨酯交联的能力,多异氰酸酯包括亚甲基桥接的多苯基多异氰酸酯和/或亚甲基桥接的多苯基多异氰酸酯的预聚物,其平均官能度为每分子1.8至3.5(如2.0至3.1)个异氰酸酯部分且NCO含量为25至32重量%。
本说明书还涉及制备硬质聚氨酯泡沫的方法。在这样的方法中,有机多异氰酸酯与上文所述类型的异氰酸酯反应性组合物反应。在一些实施方案中,以90至140,如120至130的异氰酸酯指数混合异氰酸酯官能组分和异氰酸酯反应性组合物。
在某些实施方案中,在发泡剂、水、叔胺催化剂组合物、表面活性剂和任何其他可选组分的存在下,异氰酸酯反应性组合物的多元醇共混物与有机多异氰酸酯发生反应。硬质泡沫可通过将异氰酸酯反应性组合物的所有组分一起共混为相稳定混合物,然后将此混合物与有机多异氰酸酯以合适的比例混合而制备。或者,一种或多种组分,如表面活性剂,可在将有机多异氰酸酯与异氰酸酯反应性组合物混合之前与该有机多异氰酸酯组合。本发明其他可能的实施方案包括将一种或多种组分作为单独的料流,与多元醇共混物和有机多异氰酸酯一起加入。
许多发泡机被设计成调理并以合适比例混合仅有的两种组分。为使用这些机器,可有利地采用除多异氰酸酯之外的所有成分的预混物。根据两组分方法(组分A:多异氰酸酯;和组分B:异氰酸酯反应性组合物,通常包括多元醇共混物、发泡剂、水、催化剂和表面活性剂),各组分可在5至50℃,如15至35℃的温度下以合适比例混合,再被注入或倒入温度被控制在20至70℃,如35至60℃范围内的模具中。然后,混合物膨胀以使空腔充满硬质聚氨酯泡沫。这简化了形成聚氨酯泡沫形成混合物的各反应组分的计量和混合,但要求异氰酸酯反应性组合物是相稳定的。
此外,硬质聚氨酯泡沫可使用任何众所周知的发泡设备,通过一步法或准预聚物法,以分批或连续过程来制备。硬质聚氨酯泡沫可制备为以下形式:块状泡沫(slabstock)、模制品、型腔填充物、喷涂泡沫、沫状泡沫(frothed foam)或与作为饰面基材的其他材料(如,硬纸板、石膏板、塑料、纸张或金属)的层压板。
对于闭孔绝热泡沫,目的是将发泡剂保留在泡孔内,以保持绝热材料即硬质聚氨酯泡沫的低导热性。因此,泡沫中的闭孔含量高是期望的。根据本说明书的实施方案制备的泡沫具有如按照ASTM D6226-15测量的多于80%,通常多于85%,或多于88%的闭孔含量。此外,按照本说明书的不同实施方案制备的泡沫按照ASTM C518-17测量的导热性,针对来自3英寸厚的板的芯部的泡沫,在35°F(2℃)下测得为低于0.160BTU-in/h-ft2-°F。
该说明书还涉及本文所述的硬质聚氨酯泡沫用于绝热的用途。可将硬质泡沫例如用作复合元件的中间层或用于填充冰箱和冷冻机或冷藏拖车的中空空间。泡沫也可具有在建筑业中的用途或用于长距离加热管道和容器的绝热。
如此,本发明还提供包含夹在一个或多个饰面基材之间的如本文所公开的硬质聚氨酯泡沫的复合制品。在某些实施方案中,饰面基材可以是塑料(如,以连续双向玻璃纤维增强的聚丙烯树脂或纤维玻璃增强的聚酯共聚物)、纸、木头或金属(如,铝)。举例来说,在某些实施方案中,复合制品可为冷藏设备,如,具有金属外壳和塑料内衬的冰箱、冷冻机或冷却机。在某些实施方案中,冷藏设备可为拖车,并且复合制品可包含位于夹层复合材料中的本发明聚氨酯泡沫,该夹层复合材料用于拖车地板。
目前认为,本文所述的特定的异氰酸酯反应性组合物能够制备这样的硬质泡沫:其具有特定的性能组合,使其适合用在用于拖车地板的夹层复合材料中。
首先,针对来自3英寸厚的板的泡沫,在1.90至2.20lb/ft3(30.4至35.2kg/m3)的整体泡沫密度下,如按照ASTM D1622-14所测量的,即使在异氰酸酯反应性组合物中所使用的HCFO为基于异氰酸酯反应性组合物总重量计小于15重量%时,硬质泡沫在75°F(23.9℃)下测得的导热率仍可为小于0.160BTU-in/h-ft2-°F。其次,异氰酸酯反应性组合物具有长的保存期限。本文中,当说到异氰酸酯反应性组合物具有“长”保存期限时,意为在60℃下贮存异氰酸酯反应性组合物6天后,当异氰酸酯反应性组合物与多异氰酸酯混合时,即使在异氰酸酯反应性组合物包括1.5重量%或更多的水时,由此产生的泡沫的胶凝时间也保持在初始胶凝时间(刚制得并且没有将异氰酸酯反应性组分在60℃下贮存6天后的这种泡沫的胶凝时间)的10%之内。在一些情况下,该初始胶凝时间是120至240秒,这理想地适合于拖车地板应用。第三,硬质泡沫呈现出低收缩率,甚至密度为低至2.02lb/ft3时,这意味着,由本文所述的泡沫形成组合物制备的自由发泡密度泡沫,在环境条件的温度和压力(25℃和1大气压)下老化4周后,体积改变为小于14%。第四,泡沫呈现出对通常用于制造冷藏拖车地板绝热复合元件的饰面基材的优异粘附性,特别是铝饰面。第五,当在拖车地板部件的生产中无压发泡时,发泡期间泡沫可产生足够低的压力,以保持顶部地板挠曲小于0.5英寸。如本文中所使用的,“优异粘附性”意为硬质泡沫通过下文所述的格林强度粘附测试。
以下的非限制性且非穷举的实施例意在进一步说明各种非限制性且非穷举的实施方案,而不限制本说明书所述的实施方案的范围。
实施例
用表1所列出的成分和用量(以重量份计)制备泡沫形成组合物。使用了以下原料:
多元醇1:蔗糖、甘油、丙二醇和水引发的聚醚多元醇,OH值为398-422mg KOH/g且平均官能度为4.3;
多元醇2:蔗糖和水引发的聚醚多元醇,OH值为370-390mg KOH/g且平均官能度为5.33;
多元醇3:甘油引发的基于环氧丙烷的三醇,OH值为445-495mg KOH/g;
多元醇4:分子量4,000的基于聚环氧丙烷的二醇,羟值为26-30;
多元醇5:甘油引发的基于聚环氧丙烷的三醇,羟值为233-243mg KOH/g;
多元醇6:基于聚环氧丙烷的二醇,羟值为107.4-115.4(当量486-522);
多元醇7:蔗糖/水引发的聚醚多元醇,OH值为450-490mg KOH/g且平均官能度为5.52;
多元醇8:芳族胺引发的聚醚四醇,羟值为378-398mg KOH/g;
多元醇9:芳族胺引起的聚醚四醇,羟值为350-370mg KOH/g;
多元醇10:芳香族聚酯多元醇,OH值为230-250mg KOH/g,且25℃下粘度为2,000-4,000mPa·s;
多元醇11:单乙醇胺引发的聚醚多元醇,OH值为685至715,官能度为3,且氮含量为5.8重量%,通过使单乙醇胺丙氧基化来制备;
FR:三(2-氯异丙基)磷酸酯(FyrolTM PCF,来自ICL Industrial Products);
表1
成分 | 1 | 2 | 3 | 4 | 5 | 6 | 7 |
多元醇1 | 52.08 | 52.37 | -- | -- | -- | -- | -- |
多元醇2 | -- | -- | -- | 26.19 | -- | -- | 34.91 |
多元醇3 | -- | -- | -- | -- | -- | 17.46 | -- |
多元醇4 | 18.01 | -- | -- | -- | -- | -- | -- |
多元醇5 | -- | 10.04 | 10.04 | 10.04 | 10.04 | 10.04 | 10.04 |
多元醇6 | -- | 9.02 | 9.02 | 9.02 | 9.02 | 9.02 | 9.02 |
多元醇7 | -- | -- | 52.37 | 26.18 | 26.19 | -- | -- |
多元醇8 | -- | -- | -- | -- | 26.18 | -- | -- |
多元醇9 | -- | -- | -- | -- | -- | 34.91 | -- |
多元醇10 | -- | -- | -- | -- | -- | -- | 17.46 |
SURF | 1.93 | 1.91 | 1.91 | 1.91 | 1.91 | 1.91 | 1.91 |
CAT 1 | 2.03 | 2.01 | 2.01 | 2.01 | 2.01 | 2.01 | 2.01 |
CAT 2 | 0.92 | 0.38 | 0.38 | 0.38 | 0.38 | 0.38 | 0.38 |
CAT 3 | 0.10 | -- | -- | -- | -- | -- | -- |
FR | 8.14 | 8.04 | 8.04 | 8.04 | 8.04 | 8.04 | 8.04 |
水 | 2.34 | 2.41 | 2.41 | 2.41 | 2.41 | 2.41 | 2.41 |
HCFO | 14.45 | 13.82 | 13.82 | 13.82 | 13.82 | 13.82 | 13.82 |
总计 | 100.00 | 100.00 | 100.00 | 100.00 | 100.00 | 100.00 | 100.00 |
ISO | 100.00 | 118.00 | 127.00 | 120.00 | 121.00 | 117.00 | 104.00 |
表1(续)
对于每一个实施例,多元醇、催化剂、表面活性剂、阻燃剂、水和HCFO均以表1中所述用量来混合。所有泡沫均在实验室用小型的实验室压机来制备。成功的实验室结果用Hennecke HK-100高压发泡机来制备。液体输出对于多元醇一方保持恒定在21℃,对于异氰酸酯一方保持恒定在27℃,输出范围为454至653克/秒,倾倒压力为103巴。由三块倒入尺寸为8英寸乘78.75英寸乘3英寸(20.3厘米x 200厘米x 7.6厘米)的控温模具(29.4℃)、而未将模具完全填满的板发泡来确定最小填充密度,然后使用线性回归确定计算出的最小板质量值。在最小填充密度确定之后,然后填塞泡沫以获得超过最小填充密度约8%至15%的期望密度。泡沫被夹在一个铝饰面和一个塑料饰面之间。在29.4℃下将泡沫保持在模具中180至240分钟然后脱模。根据ASTM D1622-14测量,每个泡沫的整体密度在2.01至2.17lb/ft3(32.2至34.8kg/m3)之间。
针对各种性能对泡沫进行测试,并且将结果列在表2中。对于k系数,针对来自3英寸厚的板的芯部的泡沫,根据ASTM C518-17进行测量,如果泡沫在75°F(23.9℃)测得的导热性为小于0.160BTU-in/h-ft2-°F,则认为泡沫“合格”。对于保存期限,如果在将异氰酸酯反应性组合物于60℃下贮存6天后,泡沫的胶凝时间在初始胶凝时间(立即而不是将异氰酸酯反应性组合物于60℃下贮存6天后才制备的这种泡沫的胶凝时间)的10%以内,则认为泡沫“合格”。对于尺寸稳定性,如果将泡沫于环境条件的温度和压力下(25℃和1大气压)老化4周后,自由发泡密度泡沫的体积改变小于14%,则认为泡沫“合格”。对于泡沫压力,如美国专利申请No.16/296,872的[00111]段中所述那样测量,如果所产生的压力低于1.0lb/in2,在一些情况下,低于0.95lb/in2,或者甚至低于0.85lb/in2,则认为泡沫“合格”。对于粘附性,当按照下文所述的格林强度粘附测试测量时,如果铝饰面粘在泡沫上并将胶带拉离压机,则认为泡沫“合格”。对于粘附性,当按照下文所述的格林强度粘附测试测量时,如果铝饰面与泡沫脱离并使胶带保持在压机,则认为泡沫“不合格”。
格林强度粘附测试如下:将框架内尺寸为26英寸高、13英寸宽和3英寸厚的立式实验室压机加热至85°F。将1英寸宽的遮蔽胶带粘到压机驱动侧上的0.04英寸厚的铝饰面的整个周长,使1/2"重叠在饰面上,而1/2"重叠在压机上。该饰面代替了尺寸为26英寸高、13英寸宽的框架的一侧。将脱模剂(来自Solar Corp.的1894-EX-S)应用于框架的其余部分并使其干燥至少2分钟。将框架封闭在压机内,并将所需量的泡沫形成组合物以达到所需密度的目标量倒入模具中。在泡沫到达模具顶部之前关闭模具顶部并夹紧。20分钟后,用手将框架部件固定就位,同时打开压机的驱动侧。
表2
从表2可以明显看出,本发明实施例8、9、12和14全部通过了尺寸稳定性测试并且表现出可接受的泡沫压力。本发明的实施例12和14也进行了粘附力测试并通过(虽然没有测试,但也认为实施例8和9将通过粘附力测试)。实施例14也经过了保存期限测试并通过(认为实施例8、9和12也会通过保存期限测试)。
尽管出于说明的目的在上文中对本发明进行了详细描述,但是应当理解,这种细节仅出于此目的,并且本领域技术人员可以在不脱离本发明的精神和范围的情况下在其中进行各种改变,除非本发明的精神和范围可受到权利要求书的限制。
Claims (40)
1.一种异氰酸酯反应性组合物,其包括:
(a)多元醇共混物,其包括:
(1)基于所述多元醇共混物的总重量计,30重量%至98重量%的糖引发的聚醚多元醇,所述糖引发的聚醚多元醇具有200至600mg KOH/g的OH值和4至6的官能度,
(2)基于所述多元醇共混物的总重量计,1重量%至40重量%的聚环氧烷二醇,所述聚环氧烷二醇具有1.9至2.0的官能度和20至120mg KOH/g的OH值;和
(3)基于所述多元醇共混物的总重量计,1重量%至20重量%的烷醇胺引发的聚醚多元醇,所述烷醇胺引发的聚醚多元醇具有至少500mg KOH/g的OH值和2.5至4的官能度;
(b)发泡剂组合物,其包括:
(1)氢氯氟烯烃;和
(2)产生二氧化碳的化学发泡剂;和
(c)叔胺催化剂组合物。
2.根据权利要求1所述的异氰酸酯反应性组合物,其中,基于所述多元醇共混物的总重量计,所述糖引发的聚醚多元醇以40重量%至98重量%,50重量%至98重量%,60重量%至90重量%,或70重量%至90重量%的量存在。
3.根据权利要求1或权利要求2所述的异氰酸酯反应性组合物,其中,所述糖包括蔗糖、山梨糖醇或麦芽糖醇。
4.根据权利要求1至权利要求3中任一项所述的异氰酸酯反应性组合物,其中,所述糖引发的聚醚多元醇是至少一种环氧烷烃与一种或多种合适的引发剂化合物在合适的催化剂的存在下的反应产物,所述环氧烷烃包括环氧丙烷和/或环氧乙烷,其中所述引发剂化合物包括一种或多种糖和一种或多种共引发剂,所述共引发剂包括水、丙二醇、甘油、乙二醇、乙醇胺、二乙二醇的化合物及其混合物。
5.根据权利要求1至权利要求4中任一项所述的异氰酸酯反应性组合物,其中,所述糖引发的聚醚多元醇具有300至550mg KOH/g,350至450mg KOH/g或360至400mg KOH/g的OH值,和/或4至5或4.0至4.5的官能度。
6.根据权利要求1至权利要求5中任一项所述的异氰酸酯反应性组合物,其中,基于所述多元醇共混物的总重量计,所述多元醇共混物包括1至20重量%或10至20%的聚环氧烷二醇。
7.根据权利要求1至权利要求6中任一项所述的异氰酸酯反应性组合物,其中,所述聚环氧烷二醇具有1.98至2.00的官能度和/或20至80mg KOH/g,20至40mg KOH/g或20至30mgKOH/g的OH值。
8.根据权利要求1至权利要求7中任一项所述的异氰酸酯反应性组合物,其中,所述聚环氧烷二醇具有1000至5600g/mol,2800至5600g/mol或3700至5600g/mol的数均分子量。
9.根据权利要求1至权利要求8中任一项所述的异氰酸酯反应性组合物,其中,所述聚环氧烷二醇包括一种或多种环氧烷烃与一种或多种二醇的加成聚合产物,所述环氧烷烃包括环氧乙烷、环氧丙烷和/或环氧丁烷,所述二醇包括乙二醇、二乙二醇、丙二醇以及乙二醇和/或丙二醇的其他低聚物。
10.根据权利要求1至权利要求9中任一项所述的异氰酸酯反应性组合物,其中,所述糖引发的聚醚多元醇和所述聚环氧烷二醇以至少2:1、2:1至10:1、3:1至7:1或4:1至6:1的重量比存在于所述多元醇共混物中。
11.根据权利要求1至权利要求10中任一项所述的异氰酸酯反应性组合物,其中,所述烷醇胺引发的聚醚多元醇是至少一种环氧烷烃与一种或多种合适的引发剂化合物的反应产物,所述环氧烷烃包括环氧丙烷、环氧丁烷、氧化苯乙烯、表氯醇或其任意两种或更多种的混合物,所述引发剂化合物包括如下化学式所表示的烷醇胺:
NH2—Z—OH
其中Z表示二价基团,所述二价基团是具有2至6个碳原子的直链或支链的亚烷基、具有4至6个碳原子的亚环烷基,或如下化学式所表示的二亚烷基醚基:
—R—O—R—
其中每个R表示具有2至3个碳原子的烃基。
12.根据权利要求11所述的异氰酸酯反应性组合物,其中,所述烷醇胺包括单乙醇胺、1-氨基-2-丙醇、2-氨基-l-丙醇、3-氨基-l-丙醇、1-(2-氨基乙氧基)乙醇、1-氨基-2-丁醇、2-氨基-3-丁醇、2-氨基-2-甲基丙醇、5-氨基戊醇、3-氨基-2,2-二甲基丙醇、4-氨基环己醇或其任意两种或更多种的混合物。
13.根据权利要求1至权利要求12中任一项所述的异氰酸酯反应性组合物,其中,所述烷醇胺引发的聚醚多元醇具有500至900mg KOH/g,600至800mg KOH/g或680至720mg KOH/g的OH值,和/或2.5至3.5的官能度。
14.根据权利要求1至权利要求13中任一项所述的异氰酸酯反应性组合物,其中,基于所述多元醇共混物的总重量计,所述烷醇胺引发的聚醚多元醇以1重量%至10重量%或2重量%至10重量%的量存在。
15.根据权利要求1至权利要求14中任一项所述的异氰酸酯反应性组合物,其中,所述糖引发的聚醚多元醇和所述烷醇胺引发的聚醚多元醇以至少5:1,10:1至25:1或15:1至25:1的重量比存在于所述多元醇共混物中。
16.根据权利要求1至权利要求15中任一项所述的异氰酸酯反应性组合物,其中,所述聚环氧烷二醇和所述烷醇胺引发的聚醚多元醇以至少1:1,1:1至10:1,1:1至5:1,或2:1至4:1的重量比存在于所述多元醇共混物中。
17.根据权利要求1至权利要求16中任一项所述的异氰酸酯反应性组合物,其中,所述多元醇共混物还包括脂族三醇引发的聚醚多元醇,所述脂族三醇引发的聚醚多元醇具有100至500mg KOH/g,200至400mgKOH/g,200至300mg KOH/g,200至250mg KOH/g,230至250mgKOH/g或233至243mg KOH/g的OH值,和/或大于2至4,2.5至3.5,或3.0的官能度。
18.根据权利要求1至权利要求17中任一项所述的异氰酸酯反应性组合物,其中,所述多元醇共混物具有4至6,4.5至4.5或4.5至5.0的加权平均官能度,和/或300至500mg KOH/g,300至400mg KOH/g,或320至360mg KOH/g的加权平均羟值,和/或大于800至1600g/mol,1000至1400g/mol或1200至1300g/mol加权平均分子量。
19.根据权利要求1至权利要求18中任一项所述的异氰酸酯反应性组合物,其中,所述氢氯氟烯烃包括1-氯-3,3,3-三氟丙烯(HCFO-1233zd,E和/或Z异构体)、2-氯-3,3,3-三氟丙烯(HCFO-1233xf)、HCFO1223、1,2-二氯-1,2-二氟乙烯(E和/或Z异构体)、3,3-二氯-3-氟丙烯、2-氯-1,1,1,4,4,4-六氟-2-丁烯(E和/或Z异构体)、2-氯-1,1,1,3,4,4,4-七氟-2-丁烯(E和/或Z异构体),或其任意两种或更多种的混合物。
20.根据权利要求1至权利要求19中任一项所述的异氰酸酯反应性组合物,其中,所述氢氯氟烯烃在大气压下的沸点是至少-25℃,至少-20℃,或至少-19℃,以及40℃或更低,35℃或更低,或者33℃或更低,例如其中所述氢氯氟烯烃在大气压下具有-25℃至40℃,-20℃至35℃或-19℃至33℃的沸点。
21.根据权利要求1至权利要求20中任一项所述的异氰酸酯反应性组合物,其中,基于所述异氰酸酯反应性组合物的总重量计,所述氢氯氟烯烃以至少10重量%,10至30重量%,或10至20重量%的量存在。
22.根据权利要求1至权利要求21中任一项所述的异氰酸酯反应性组合物,其中,所述产生二氧化碳的化学发泡剂包括水和/或甲酸酯封端的胺。
23.根据权利要求1至权利要求22中任一项所述的异氰酸酯反应性组合物,其中,基于所述异氰酸酯反应性组合物的总重量计,所述产生二氧化碳的化学发泡剂以0.5重量%至5.0重量%,1重量%至4重量%,1.0重量%至3.0重量%,或2.0重量%至3.0重量%的量存在。
24.根据权利要求1至权利要求23中任一项所述的异氰酸酯反应性组合物,其中,基于所述异氰酸酯反应性组合物的总重量计,所述氢氯氟烯烃和所述产生二氧化碳的化学发泡剂以至少90重量%,至少95重量%,或至少99重量%的量存在。
25.根据权利要求1至权利要求24中任一项所述的异氰酸酯反应性组合物,其中,所述氢氯氟烯烃和产生二氧化碳的化学发泡剂以至少2:1,至少4:1,4:1至10:1,或6:1至10:1的重量比存在于所述发泡剂组合物中。
26.根据权利要求1至权利要求25中任一项所述的异氰酸酯反应性组合物,其中,所述异氰酸酯反应性组合物还包括表面活性剂,例如聚硅氧烷-聚烯烃-嵌段共聚物,例如聚醚改性的聚硅氧烷、长链醇的聚乙二醇醚、长链烷基酸硫酸酯、烷基磺酸酯或烷基芳基磺酸的叔胺或烷醇胺盐。
27.根据权利要求1至权利要求27中任一项所述的异氰酸酯反应性组合物,其中,所述叔胺催化剂组合物包括吗啉和/或咪唑,例如其中所述叔胺催化剂组合物包括:(i)80重量%至99重量%,90重量%至99重量%,95重量%至98重量%或97重量%至98重量%的吗啉,基于所述叔胺催化剂组合物的总重量计;和(ii)1重量%至20重量%,1重量%至10重量%,2重量%至5重量%,或2重量%至3重量%的咪唑,基于所述叔胺催化剂组合物的总重量计,例如其中吗啉催化剂包括二吗啉二乙醚、二吗啉二甲醚、N-乙基吗啉、N-甲基吗啉或其两种或更多种的混合物,并且所述咪唑催化剂包括咪唑、N-甲基咪唑、1,2-二甲基咪唑或其两种或更多种的混合物,例如其中所述吗啉催化剂包括二吗啉二乙醚与N-甲基吗啉的混合物,其中基于吗啉催化剂的总重量计,二吗啉二乙醚以30重量%至80重量%,或40重量%至80重量%的量存在,且N-甲基吗啉以20重量%至70重量%,或20重量%至60重量%的量存在。
28.一种硬质聚氨酯泡沫形成组合物,其包括:(a)多异氰酸酯;和(b)根据权利要求1至权利要求27中任一项所述的异氰酸酯反应性组合物。
29.根据权利要求28所述的硬质聚氨酯泡沫形成组合物,其中,所述多异氰酸酯包括芳族、脂族或脂环族多异氰酸酯、或其两种或更多种的混合物,例如亚甲基桥接的多苯基多异氰酸酯和/或亚甲基桥接的多苯基多异氰酸酯的预聚物,其平均官能度为每分子1.8至3.5、或2.0至3.1个异氰酸酯部分且NCO含量为25至32重量%。
30.一种由权利要求28或权利要求29所述的硬质聚氨酯泡沫形成组合物制备的硬质聚氨酯泡沫。
31.一种制备硬质聚氨酯泡沫的方法,包括将有机异氰酸酯与根据权利要求1至权利要求27中任一项所述的异氰酸酯反应性组合物以90至140或110至130的异氰酸酯指数混合。
32.根据权利要求31所述的方法,其中混合物被注入或倒入温度为20至70℃或35至60℃的模具中。
33.一种包含夹在一个或多个饰面基材之间的硬质聚氨酯泡沫的复合制品,所述硬质聚氨酯泡沫是根据权利要求28或权利要求29所述的硬质聚氨酯泡沫形成组合物的反应产物,或者所述硬质聚氨酯泡沫由根据权利要求31或权利要求32所述的方法制备,其中,所述饰面基材包括塑料,例如以连续双向玻璃纤维增强的聚丙烯树脂或纤维玻璃增强的聚酯共聚物、纸、木头或金属,例如铝。
34.根据权利要求33所述的复合制品,其中所述复合制品是冷藏设备。
35.根据权利要求34所述的复合制品,其中所述冷藏设备包括拖车,并且所述复合制品是用于拖车地板的夹层复合材料。
36.一种包含夹在饰面基材之间的硬质聚氨酯泡沫的复合制品,其中所述硬质聚氨酯泡沫包括反应混合物的反应产物,所述反应混合物包括(a)多异氰酸酯;(b)多元醇共混物;(c)发泡剂组合物,所述发泡剂组合物包括:(1)氢氯氟烯烃,和(2)产生二氧化碳的化学发泡剂;和(d)叔胺催化剂组合物,其中所述多元醇共混物包括:
(1)基于所述多元醇共混物的总重量计,40重量%至98重量%的糖引发的聚醚多元醇,所述糖引发的聚醚多元醇具有200至600mg KOH/g的OH值和4至6的官能度;
(2)基于所述多元醇共混物的总重量计,1重量%至40重量%的聚环氧烷二醇,所述聚环氧烷二醇具有1.9至2.0的官能度和20至120mg KOH/g的OH值;和
(3)基于所述多元醇共混物的总重量计,1重量%至20重量%的烷醇胺引发的聚醚多元醇,所述烷醇胺引发的聚醚多元醇具有至少500mg KOH/g的OH值和2.5至4的官能度。
37.根据权利要求36所述的复合制品,其中所述饰面基材包括铝饰面。
38.根据权利要求37所述的复合制品,其中所述复合制品体现为冷藏牵引拖车地板。
39.一种硬质聚氨酯泡沫形成组合物,其包括:
(a)多异氰酸酯;
(b)多元醇共混物,其包括:
(1)基于所述多元醇共混物的总重量计,40重量%至98重量%的糖引发的聚醚多元醇,所述糖引发的聚醚多元醇具有200至600mg KOH/g的OH值和4至6的官能度;
(2)基于所述多元醇共混物的总重量计,1重量%至40重量%的聚环氧烷二醇,所述聚环氧烷二醇具有1.9至2.0的官能度和20至120mg KOH/g的OH值;和
(3)基于所述多元醇共混物的总重量计,1重量%至20重量%的烷醇胺引发的聚醚多元醇,所述烷醇胺引发的聚醚多元醇具有至少500mg KOH/g OH值和2.5至4的官能度;
(c)发泡剂组合物,其包括:
(1)氢氯氟烯烃;和
(2)产生二氧化碳的化学发泡剂;和
(d)叔胺催化剂组合物。
40.一种由根据权利要求39所述的硬质聚氨酯泡沫形成组合物制备的硬质聚氨酯泡沫。
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