CN1183422A - 聚氨酯泡沫塑料 - Google Patents

聚氨酯泡沫塑料 Download PDF

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CN1183422A
CN1183422A CN97102951A CN97102951A CN1183422A CN 1183422 A CN1183422 A CN 1183422A CN 97102951 A CN97102951 A CN 97102951A CN 97102951 A CN97102951 A CN 97102951A CN 1183422 A CN1183422 A CN 1183422A
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G·J·布莱斯
V·G·J·内扬斯
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Hentzman ICI Chemical Product Co., Ltd.
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Abstract

一种制备软质聚氨酯泡沫塑料的方法,该方法是使多异氰酸酯与多元醇组合物和水反应,所述多异氰酸酯含有至少85%(重量)4,4′－二苯甲烷二异氰酸酯或其液态变体,所述多元醇组合物含有至少一种聚(氧乙烯－氧化烯)多醇,该组合物的平均名义羟基官能度为2.5—6,数均羟基当量重量为1000—3000,平均氧乙烯含量为25%(重量)至小于50%(重量)。

Description

聚氨酯泡沫塑料
通过使有机多异氰酸酯(如甲苯二异氰酸酯(TDI)或二苯甲烷二异氰酸酯(MDI))与聚醚多醇及发泡剂反应制备软质聚氨酯泡沫塑料的方法是人们所公认的。聚醚多醇通常是由氧丙烯生成的聚氧丙烯多醇或由氧丙烯或氧乙烯的各种组合物生成的聚(氧丙烯-氧乙烯)多醇。其中氧乙烯基占氧化烯基总量的一少部分的氧乙烯封端的聚氧丙烯多醇因其与异氰酸酯的反应性提高而特别重要。
具有较高氧乙烯含量(例如50％(重量)或更高)的多元醇通常用作辅助添加剂以保证泡沫塑料具有开孔结构。
现已发现，如果使用基本上纯的4，4′-MDI或其液态衍生物作
为多异氰酸酯，可由含有具有中等氧乙烯含量的多元醇组合物的配方制得具有有用性能的软质泡沫塑料。
因此，本发明提供了一种通过使多异氰酸酯与多元醇组合物和水
反应制备软质聚氨酯泡沫塑料的方法，所述多异氰酸酯含有至少85％(重量)、优选至少90％(重量)、更优选至少95％(重量)4，4′-二苯甲烷二异氰酸酯或其液态变体，所述多元醇组合物含有至少一种聚(氧乙烯-氧化烯)多醇，平均名义羟基官能度为2.5-6、
优选2.5-3，数均羟基当量重量为1000-3000，平均氧乙烯含量为25％至小于50％(重量)、优选40％至小于50％(重量)。
本发明方法所用的多异氰酸酯组分可基本上由纯的4，4′-二苯甲烷二异氰酸酯或该异氰酸酯与一种或多种其它有机多异氰酸酯、特别是其它二苯甲烷二异氰酸酯异构体(如2，4′-异构体任选地与2，2′-异构体联用)的混合物组成。多异氰酸酯组分还可以是由含有至少85％(重量)4，4′-二苯甲烷二异氰酸酯的多异氰酸酯组合物衍生得到的MDI变体。MDI变体是本领域众所周知的，对于按照本发明的应用，还特别包括通过将uretonimine和/或碳化二亚胺基团引入所述多异氰酸酯组合物(如含有至多30％(重量)uretonimine和/或碳化二亚胺修饰的4，4′-MDr)和/或使这种组合物与一种或多种多元醇反应得到的液体(室温)产物。多元醇组合物中的多元醇是本领域已知的，可以按常规方法通过使氧乙烯和另一种氧化烯(优选氧丙烯)同时和/或按任何顺序依次与诸如水、多元醇、羟胺、多胺等具有2-6(优选2-3)个活性氢原子的引发剂反应而得到。优选的引发剂是乙二醇、二甘醇、丙二醇、双丙甘醇、甘油、三羟甲基丙烷、乙醇胺、二乙醇胺和三乙醇胺。
或者，多元醇组合物可含有两种或更多种聚氧化烯多醇的组合物以便使整个组合物具有所需的平均官能度、当量重量和氧乙烯含量。这种混合物中的聚氧化烯多醇优选为聚(氧乙烯-氧丙烯)多醇，但也可含有一种或多种聚氧乙烯多醇和/或聚氧丙烯多醇。
就数均羟基当量重量为1000-3000的聚醚多醇而言，优选的多元醇组合物由下述组分组成：
(a)50-100％(重量)含氧乙烯基的聚氧化烯多醇，所述多元醇组分的平均名义羟基官能度为2-6、优选2-3，数均羟基当量重量为1000-3000，平均氧乙烯含量为25％(重量)至小于50％(重量)，和
(b)50-0％(重量)一种或多种其它多元醇，所述多元醇的平均名义官能度为2-6、优选2-3，数均当量重量为1000-
3000，氧乙烯含量小于25％(重量)、优选为10％(重量)至小于25％(重量)或者50％(重量)或更多、优选50-85％(重量)；该多元醇组合物的羟基官能度、当量重量和氧乙烯含量如上所述。
这里所用的术语“平均名义羟基官能度”是指在假定多元醇组合物中所含的聚氧化烯多醇的平均官能度与制备所述多元醇时所用的引发剂的平均官能度(每个分子中的活性氢原子数)相同的条件下多元醇组合物的平均官能度(每个分子的羟基数)，但实际上由于某些末端不饱和的情况，前者常常在某种程度上小于后者。
如果需要，多元醇组合物可含有分散的聚合物颗粒。这类聚合物改性的多元醇已在先有技术中详细描述，它们包括通过一种或多种乙烯基单体(例如丙烯腈和苯乙烯)在聚氧化烯多醇中原位聚合或通过使多异氰酸酯和氨基或羟基官能化合物(例如三乙醇胺)在聚氧化烯多醇中原位反应得到的产物。
本发明方法优选的发泡剂是水，且可任选地与物理发泡剂(如低沸点有机含氟化合物)结合使用。可用已知方法改变发泡剂的用量以便达到所要求的泡沫塑料密度。适宜的水量例如是多元醇组合物重量的0.25-20％，优选2-15％。优选仅用水作发泡剂。包括多元醇组合物、水和任何其它异氰酸酯反应性物质(例如扩链剂或交联剂)在内的反应体系的异氰酸酯指数可以是10-120，优选40-110。软质泡沫塑料的自由起发密度可以是15-100kg/m3优选20-80kg/m3。
发泡反应混合物可含有一种或多种用于制备软质泡沫塑料的添加剂。这类添加剂包括催化剂(如叔胺、锡化合物，优选碱金属或碱土金属羧酸盐，特别是羧酸钾)、表面活性剂和泡沫稳定剂(如硅氧烷-氧化烯共聚物)、扩链剂(如分子量为200-1000的低分子量二醇类，如乙二醇、丁二醇、二甘醇和聚乙二醇)、交联剂(如甘油、三羟甲基丙烷、二乙醇胺和三乙醇胺)、阻燃剂、有机和无机填料、颜料、用于抑制所谓沸泡(boiling-foam)效应的试剂(如聚二甲基硅氧烷)和内脱模剂。相对于100重量份数均羟基当量重量为1000-3000的聚醚多醇，扩链剂和/或交联剂的用量优选为2重量份或更少，更优选为1重量份或更少。
优选的羧酸盐催化剂可以选自具有1-10个碳原子的脂族羧酸盐，如乙酸盐、已酸盐、2-乙基己酸盐和辛酸盐。
羧酸盐还可以选自下式所示的羧酸盐：
R-E-A-COO-；其中，
A为具有1-6、优选1-3个碳原子的烃双基；
E为-O-或
Figure A9710295100061
R为X-R1-(OR2)n-，其中X为CH3-或OH-，R1为具有1-8、优选1-4个碳原子的烃双基，R2为具有2-4、优选2或3个碳原子的双基，n为0-10，优选0-5。
某些这类催化剂及其制备方法是已知的，例如参见EP 294161和
EP220697。
A可以选自诸如-CH2-、-CH2CH2-、-CH2CH2CH2-、-CH＝CH-CH2-、
Figure A9710295100062
、-CH＝CH-、
Figure A9710295100063
和
Figure A9710295100064
类的双基。最优选的双基是-CH＝CH-。
R1可以选自A的定义中提及的烃双基和由例如丁烷、戊烷、己烷和辛烷上去掉两个氢原子所得的基团。最优选的R1亚甲基、亚乙基、1，3-亚丙基、1，4-亚丁基和1，2-亚丙基。
R2可以选自亚乙基、1，3-亚丙基、1，4-亚丁基、乙基亚乙基和1，2-亚丙基。最优选的基团是亚乙基和亚丙基。
催化剂的实例有乙酸钠、乙酸钾、己酸钾、2-乙基己酸钾、乙氧基乙酸钾、乙氧基乙酸钠，马来酸与下列化合物的半酯的钾盐：乙氧基乙烷、乙氧基乙氧基乙烷、乙二醇、二甘醇、三甘醇、四甘醇、丙二醇、双丙甘醇、三丙甘醇、甲醇、乙醇、丙醇或丁醇，以及这类含羟基化合物与下列化合物的半酯的钾盐：丙二酸、丁二酸、戊二酸、己二酸或富马酸。
通过使用这种特殊类型的催化剂而不是常规的含叔胺催化剂，泡沫塑料不易发生因与添加剂(如抗氧剂)发生副反应而导致的色变、不易产生含人不快的气味、更易于回用且不易发生结雾。
相对于100重量份反应物，羧酸盐的用量为0.1-5重量份，优选0.2-3重量份。
因此，本发明的另一方面涉及一个反应体系，该体系包括：
(i)含有至少85％(重量)4，4′-二苯甲烷二异氰酸酯或其液态变体的多异氰酸酯；
(ii)含有至少一种聚(氧乙烯-氧化烯)多醇的多元醇组合物，该组合物的平均名义羟基官能度为2-6，数均羟基当量重量为1000-3000，平均氧乙烯含量为25％(重量)至小于50％(重量)；
(iii)包含水的发泡剂；和任选的
(iv)一种或多种用于软质泡沫塑料配方的添加剂。
该反应体系用于制备软质泡沫塑料。术语“反应体系”定义为其中多异氰酸酯保存在与异氰酸酯反应性成分分开的容器中的体系。
在实施本发明的方法时，已知的一步法半预聚物和全预聚物技术可以与常规混合装置一起使用，泡沫塑料可以制成块料、模制品等。
上述多异氰酸酯(过量)与多元醇的反应产物-NCO值为5-30％(重量)的预聚物也构成本发明的一部分。预聚物本身的制备方法是本领域公知的。
用本发明方法制成的泡沫塑料具有有用的能量吸收性能，这使得它们可用于减弱声振动及装填用途。所述泡沫塑料的玻璃化转变温度(Tg)比由具有更高氧乙烯含量的多元醇制得的泡沫塑料低，本发明的泡沫塑料密度低、回弹性提高，同时保持由具有更高氧乙烯含量的多元醇制得的泡沫塑料的大部分优良性能，如撕裂强度、断裂伸长和压缩变形。
另外，本发明的泡沫塑料具有开孔或易于压垮的孔。
本发明用下述实施例说明，但不限于此。在实施例中，所有的份数、百分数和比例均按重量计。
除非另外指明，用下述材料的集注来确定反应组分。集注
多元醇1：EO/PO多醇，名义官能度为3，羟值为38.5mgKOH/g，EO含量为59％，末端EO含量为19％。
多元醇2：EO/PO多醇，名义官能度为3，羟值为36mg KOH/g，EO含量为39％，末端EO含量为10％。
多元醇3：EO/PO多醇，名义官能度为3，羟值为26mgKOH/g，EO含量为29％，末端EO含量为15％。
Dabco EG是Dabco在乙二醇中的33％溶液，由Air Products得到。Dabco是Air Products的商标。
多异氰酸酯：NCO含量为31.4％的MDI混合物，含有1.8％2，2′+2，4′-MII、84.6％4，4′-MDI和13.6％uretorimine修饰的4，4′-MDI。
DBDTL是二月桂酸二丁基锡。
A1是Niax A1：由Union Carbide得到的催化剂。Nias ix是Union Carbide的商标。
DELA：二乙醇胺。
Dabco EG：由Air Products得到的催化剂。
在发泡杯中，使多异氰酸酯在如表1所示的特定指数下与异氰酸酯反应性组合物(其具体组成连同一些物理性能示于表1中)反应。所有的量均为重量份数。表1
           指数     100     97     96     102
         多元醇1     50     20      -      -
         多元醇2     50     80     100      -
         多元醇3     -     -      -     100
            水     3     3     3     3
          DabcoEG    0.4    O.4    0.4    0.4
           DBTDL    0.1    0.15    0.15    0.15
          NiaxA 1    0.15    0.15    0.15    0.15
           DELA     -    0.7    0.9     1
   自由起发密度，kg/m3     38     39     41     36
回弹性，％(Iso 8307)     48     36     39     44
玻璃化转变温度，℃(动力机械热分析，PolymerLaboratories有限公司的DMT分析仪MKII)    -24     -    -25    -42

Claims (2)

1.一个反应体系，包括：
(i)含有至少85％(重量)4，4′-二苯甲烷二异氰酸酯或其液态变体的多异氰酸酯；
(ii)含有至少一种聚(氧乙烯-氧化烯)多醇的多元醇组合物，该组合物的平均名义羟基官能度为2.5-6，数均羟基当量重量为1000-3000，平均氧乙烯含量为25％(重量)至小于50％(重量)；
(iii)包含水的发泡剂；和任选的
(iv)一种或多种用于制备软质泡沫塑料的添加剂。
2.一种NCO值为5-30％(重量)的预聚物，该预聚物是通过使过量的多异氰酸酯与多元醇组合物反应得到的，所述多异氰酸酯含有至少85％(重量)4，4′-二苯甲烷二异氰酸酯或其液态变体，所述多元醇组合物含有至少一种聚(氧乙烯-氧化烯)多醇，该组合物的平均名义羟基官能度为2.5-6，数均羟基当量重量为1000-3000，平均氧乙烯含量为25％(重量)至小于50％(重量)。
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