CN101454258A - 制造石颗粒和聚酯树脂的聚结体的板或块的方法 - Google Patents

制造石颗粒和聚酯树脂的聚结体的板或块的方法 Download PDF

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CN101454258A
CN101454258A CNA2007800199070A CN200780019907A CN101454258A CN 101454258 A CN101454258 A CN 101454258A CN A2007800199070 A CNA2007800199070 A CN A2007800199070A CN 200780019907 A CN200780019907 A CN 200780019907A CN 101454258 A CN101454258 A CN 101454258A
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卢卡·通切利
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Abstract

在根据所谓布莱通斯通技术制造板状或块状制品时，使用不含反应性溶剂的、通过环氧化的甘油三酯与至少一种羧酸酐之间的反应形成的聚酯树脂。

Description

制造石颗粒和聚酯树脂的聚结体的板或块的方法
本发明涉及聚结体制品的制造，更具体涉及以包含粒状石材等和树脂基粘合剂的混合物为原料制造板和块的方法。
前述类型的块状和板状制品的制造方法多年来已为人所知，并已知其通用名为布莱通斯通(Bretonstone)技术，在该技术中，制备初始混合物，该初始混合物由具有所选粒度的粒状石材或者无机或有机石类材料、以及可硬化树脂基粘合剂构成。
将该混合物沉积在临时载体上或具有最终制品尺寸的模具中，并进行真空压制步骤，同时以预设频率施加的振动。
然后将所得粗制品转移到硬化步骤中，在该步骤的最后，其具有所需机械特性。
然后将可由块状物锯得的板送往精加工(上胶、平滑化、抛光等)。
关于布莱通斯通技术的更多信息和技术细节，应该考查以MarcelloToncelli的名义提交的欧洲专利786325和相同申请人提交的国际专利申请PCT/EP2006/062120，两者均经此引用并入本文。
在根据布莱通斯通技术制造基于石或石类颗粒的聚结产品时，可以使用结构型树脂。这些包括聚酯树脂、丙烯酸类树脂、环氧树脂等。
在布莱通斯通技术中使用这些树脂，可以获得具有显著的特有规格的优质产品。
最普遍的产品是包含用反应性合成单体(例如苯乙烯)稀释的邻苯二甲酸基聚酯树脂的聚结体。
要注意的是，聚酯树脂是衍生自油的合成产品，其问题是公知的。
此外，苯乙烯单体作为反应性溶剂存在于聚酯树脂中并因此存在于该混合物中，造成了数个不同的环境问题，这些问题与其有害性质和由高挥发性引起的爆炸危险相关；实际上，必须使用复杂昂贵的设备收集和除去苯乙烯蒸气，以符合日益严格的排放法规。
迄今未解决的另一问题在于，当暴露在紫外线中时，(由含溶剂的聚酯树脂获得的)制品相当明显地变黄。显然，这种长期问题，尤其是对用作建筑物外覆物的制品而言，影响了制品的美观特性。
因此，本发明的目的是根据布莱通斯通技术制造制品，其中保持了使用前述粘合剂树脂可获得的机械和美观特性，同时克服了上述问题；特别消除了混合物中苯乙烯的存在。
使用前述类型的方法实现了该目的，该方法的特征在于，在最终制品中，粘合剂树脂是不含反应性溶剂、并通过至少一种环氧化的甘油三酯与至少一种羧酸酐之间的反应形成的聚酯树脂。
因此，这是首次用在布莱通斯通技术领域中的一种聚酯树脂类型，其中至少50重量％获自可再生来源、特别是植物来源的原材料，例如环氧化的甘油三酯，和获自至少一种羧酸酐。
关于本发明中所用的聚酯树脂的详细信息，可以参看公开的德国专利申请DE 10148672 A1。
关于该第一上述组分，几个进一步规定是适当的。
天然产品，尤其是植物来源的那些，含有大量被甘油酯化的脂肪酸以形成甘油三酯，其可以通过已知技术提取。
在性质上，脂肪酸几乎从不自由存在，而是与醇、甘油结合。甘油可以结合1至3个脂肪酸：因此存在脂肪酸的甘油单酯、甘油二酯和甘油三酯。
脂肪酸由键合到氢原子上的碳原子链构成，该链通常具有含有氧(O)或氢和氧(OH)的端键。
脂肪酸被分成短链脂肪酸(4至8个碳原子)、中链脂肪酸(8至14个碳原子)和长链碳原子(14至24个碳原子)，以及被分成饱和脂肪、单不饱和脂肪和多不饱和脂肪。
后一种细分非常重要，因为脂肪酸根据不饱和度具有不同的物理和化学性质。
如果甘油三酯主要由饱和脂肪酸(棕榈酸和硬脂酸)或单不饱和酸(油酸)构成，这些化合物在室温下是固体，并且被称作“脂肪”，且特别为动物来源(猪油、牛油)。
如果甘油三酯主要由不饱和脂肪酸构成，例如单不饱和(棕榈油酸、油酸、顺式-9二十碳烯酸)或多不饱和酸(亚油酸、亚麻酸)，这些化合物在室温下是液体并且被称作“油”，且特别为植物来源(橄榄籽油、亚麻籽油、大豆油、玉米油)。
饱和脂肪酸具有线型空间构造，这使得它们可以以有序方式排列：这种排列促进分子相互作用(氢桥)，因此，它们具有高熔点。
单不饱和和多不饱和脂肪酸由于造成静电失衡的双键，没有线型分子，而是弯曲的分子，因此，由于它们自身不能以有序方式排列，分子间的键较少，因此熔融温度较低。双键的数越大，熔融温度越低。
为了用在本发明中，如下列示意图所示，这些油经过所存在的双键的环氧化反应(本身公知的反应)：
Figure A200780019907D00061
[Trigliceride di acidi grassi polinsaturi＝多不饱和脂肪酸的甘油三酯；Acido Formico＝甲酸；Trigliceride di acidi grassi epossidati＝环氧化脂肪酸的甘油三酯]
对于酸酐组分，这些酸酐的化学性质(脂族或芳族)影响操作参数，并因此也影响所得树脂的最终特性。例如，下面列出两种酸酐的化学式，即脂族酸酐或饱和二羧酸的酸酐、和获自不饱和二羧酸的芳族酸酐：
Figure A200780019907D00071
[Anidride Alifatica＝脂族；Anidride Aromatica＝芳族酸酐]
为了本发明的目的，可以使用下列酸酐(作为非限制性实例指出)：苯均四酸酐、马来酸酐、琥珀酸酐、六氢邻苯二甲酸酐、邻苯二甲酸酐、降冰片烯二甲酸酐、己二酐、戊二酐、甲基邻苯二甲酸酐、1，2-环己烷二甲酸酐、3-甲基-1，2-环己烷二甲酸酐、4-甲基-1，2-环己烷二甲酸酐、3-甲基-1，2-环己烷二甲酸酐和4-甲基-1，2-环己烷二甲酸酐的混合物、甲基-四氢邻苯二甲酸酐、四氢邻苯二甲酸酐、甲基-5-降冰片烯-2，3-二甲酸酐、十二烷基-琥珀酸酐及其混合物。
环氧化脂肪酸与一种或多种酸酐的混合物在引发剂存在下和根据所用添加剂在80-180℃的温度下固化和硬化。
反应图如下所示：
Figure A200780019907D00081
[Iniziatore＝引发剂；Calore＝热；Resina Indurita＝硬化树脂]
如反应图中所示，在形成树脂的方法中，需要存在催化剂引发剂，其根据性质和量通过降低反应时间和工艺温度来发挥作用。
下面可以列出可能的引发剂：碱金属的卤化物，铝、锌和锡的有机金属化合物，季铵的卤化物，脂族和芳族胺，硼和钛基络合物。
含硅质或钙质粒子的树脂的硬化产生了聚结产品，从化学和物理角度看，其特性都与使用溶解在反应性合成单体中的聚酯树脂获得的那些相当。
在本发明的优选实施方案中，由于环氧化的油几乎完全饱和，优选使用脂族酸酐，因为所得聚酯树脂特别可抵抗由紫外线引起的变黄。
在本发明的优点中，必须强调使用可大量获自天然来源的原材料——天然脂肪酸的甘油三酯，因此从经济角度看，本发明的方法也是有利的。
下列非限制性实例例示了本发明的方法：
根据布莱通斯通技术制造按体积计具有下列组成的板：
■树脂：                        19％
■325目石英填料：               23％
■0.1至1.2毫米石英颗粒：        58％
树脂的按重量计的组成为：
■环氧化的亚麻籽油：            55％
■甲基环己烷二甲酸酐：          20％
■降冰片烯-二甲酸酐：           21％
■在醇溶液中的1-甲基咪唑：      4％
将板在炉中在140℃处理40分钟。冷却后，确定了下列物理特性：
■弯曲强度：                 59N/mm2
■深磨损耐受性：             225mm3
■UV处理500小时：            不变黄
要指出的是，这些机械特性相当于由含有苯乙烯的传统合成聚酯树脂制成的类似制品。
此外，与由含有苯乙烯的传统合成聚酯树脂制成的类似制品不同，该制品在紫外线下暴露500小时不会变黄。
应该指出的是，布莱通斯通技术也能够制造块状制品，然后像从采石场中开采的正常天然石块那样送往锯切和精加工操作。本发明，如所附权利要求中定义的，同样适用于这类块状物的制造。

Claims (9)

1.制造板状或块状制品的方法，其中制备初始混合物，该初始混合物由具有选择的粒度的任何石或石类颗粒材料以及形成可硬化树脂的粘合剂构成，将该混合物沉积在具有最终制品尺寸的临时载体上或模具中，进行真空压制步骤，并以预设频率施加振动，然后进行所述粘合剂树脂的硬化步骤，其特征在于使用不含反应性溶剂、并且能够通过至少一种环氧化的甘油三酯与至少一种羧酸酐之间的反应形成的聚酯树脂作为粘合剂。
2.根据权利要求1的制造板状或块状制品的方法，其特征在于所述初始混合物是通过将所述颗粒与形成所述聚酯树脂的组分混合而制备的，形成所述聚酯树脂的组分包含至少一种环氧化的甘油三酯和至少一种羧酸酐。
3.根据权利要求1或2的制造板状或块状制品的方法，其特征在于所述环氧化的甘油三酯选自在室温下是液体的单不饱和或多不饱和的不饱和脂肪酸的甘油三酯。
4.根据权利要求1或2的制造板状或块状制品的方法，其特征在于所述酸酐选自苯均四酸酐、马来酸酐、琥珀酸酐、六氢邻苯二甲酸酐、邻苯二甲酸酐、降冰片烯二甲酸酐、己二酸酐、戊二酸酐、甲基邻苯二甲酸酐、1，2-环己烷二甲酸酐、3-甲基-1，2-环己烷二甲酸酐、4-甲基-1，2-环己烷二甲酸酐、3-甲基-1，2-环己烷二甲酸酐和4-甲基-1，2-环己烷二甲酸酐的混合物、甲基-四氢邻苯二甲酸酐、四氢邻苯二甲酸酐、甲基-5-降冰片烯-2，3-二甲酸酐、十二烷基-琥珀酸酐以及它们的混合物。
5.根据权利要求1或2的制造板状或块状制品的方法，其特征在于将催化剂引发剂添加到环氧化的甘油三酯和酸酐的混合物中。
6.根据权利要求5的制造板状或块状制品的方法，其特征在于所述催化剂引发剂选自碱金属的卤化物，铝、锌和锡的有机金属化合物，季铵的卤化物，脂族和芳族胺，硼和钛基络合物。
7.根据权利要求1的制造板状或块状制品的方法，其特征在于所述形成聚酯树脂的反应和硬化步骤在80-180℃的温度范围进行。
8.根据权利要求7的制造板状或块状制品的方法，其特征在于所述形成聚酯树脂的反应和硬化在140℃的温度进行。
9.可通过各个前述权利要求的方法获得的板状或块状制品，其特征在于所述粘合剂是通过至少一种环氧化的甘油三酯与至少一种羧酸酐在催化剂引发剂存在下和在80-180℃的温度范围的反应获得的聚酯树脂。
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