CN104822870B - 用于纸或非织造网的交联/功能化系统 - Google Patents

用于纸或非织造网的交联/功能化系统 Download PDF

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CN104822870B
CN104822870B CN201480003241.XA CN201480003241A CN104822870B CN 104822870 B CN104822870 B CN 104822870B CN 201480003241 A CN201480003241 A CN 201480003241A CN 104822870 B CN104822870 B CN 104822870B
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nonwoven web
functionalizers
crosslinking agent
paper
acid
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CN104822870A (zh
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贝恩德·塞格尔
耶格·库恩
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Glatfelter Gernsbach GmbH and Co KG
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Abstract

本发明涉及一种纸或非织造网，包含纤维和至少一种交联剂或功能化剂，所述交联剂或功能化剂选自羧酸、卤代杂芳环化合物及其盐，其中所述至少一种交联剂或功能化剂具有不超过1000g/mol的分子量，且其中所述交联剂或功能化剂的至少一部分结合到所述纤维上，本发明还涉及用于生产所述纸或非织造网的方法，以及所述交联剂或功能化剂在纸或非织造网中的用途。

Description

用于纸或非织造网的交联/功能化系统
技术领域
本发明涉及包含纤维和特定交联剂或功能化剂的纸或非织造网(non-wovenweb)、用于生产所述纸或非织造网或气流成网(air-laid web)的方法以及所述交联剂或功能化剂在纸或非织造网中的用途。
背景技术
纸或非织造网可以用于各种目的。其实例包括用作包装材料，如用于食品包装；过滤材料，如用于注入饮料例如茶和咖啡，或用于油过滤；复合层压材料，如覆盖纸；适用于标签或包装的镀金属纸；非织造气流成网(air laid non-woven web)，如卫生和个人护理产品、家庭护理产品例如湿巾、毛巾、餐巾和桌布，特种纸例如墙纸(wallcovering,wallpaper)、床垫和家具垫料，仅举几例。
根据其用途，纸或非织造网必须满足多种性能，如干燥状态和/或潮湿状态下的抗张强度、孔隙度、附着性、润湿性、亲水性/疏水性。使用后，可能有必要或有利的是，纸或非织造网可被分解。因此，生物可降解性是纸或非织造网的常需的另一特性。
纸或非织造网通常包含主要构成网的纤维，其可以是天然纤维或合成纤维。为了赋予纸或非织造网所需的性能，通常需要改变其组成。
EP 0943731A1描述了一种过滤材料，其通过使用两亲化合物如羧甲基纤维素(CMC)或亲水性和疏水性化合物如苯乙烯/丙烯酸酯共聚物的添加剂来控制润湿性和吸水性。
然而，本发明人已发现，在EP 0943731A1中提出的作为两亲性或亲水性化合物的多糖(polysaccharide)单独提供的纤维-纤维交联键在干燥状态下是稳定的，但在潮湿状态下稳定性不足。而在EP 0943731A1中提出的疏水性化合物，如苯乙烯/丙烯酸酯共聚物，提供更好的湿强度性能(wet-strength property)，它们基于矿物油，因此从资源保护和可生物降解性的观点看，这些化合物是不理想的。
发明目的
本发明的目的是提供一种纸或非织造网，其根据需要提供特定的性能，并在生物学基础和/或可生物降解性方面具有生态优势。
特别是，本发明的目的在于提供一种交联/功能化系统，如交联剂或功能化剂，其赋予纸或非织造网所需特定性能，同时比迄今已知的油基化合物对环境更加友好。
发明概述
本发明涉及一种纸或非织造网，其包含纤维和至少一种交联剂或功能化剂，所述交联剂或功能化剂选自羧酸、卤代杂芳环化合物及其盐。
本发明人已发现，本文所述的交联剂或功能化剂适合取代迄今已知的油基化合物，并可赋予纸或非织造网所需的特定性能，如在干燥和潮湿两种状态下，甚至在恶劣条件下例如极端pH下的高抗张强度。纸或非织造网的孔隙度、附着性、润湿性或亲水性/疏水性可以通过适当选择如本文所述的特定交联剂或功能化剂及其量，或通过将其与其它添加剂如多糖添加剂例如羧甲基纤维素(CMC)结合来容易地控制到所需的性能。
因此，本发明进一步涉及本文中所描述的交联剂或功能化剂在纸或非织造网中的用途。
此外，本发明涉及用于生产纸或非织造网的方法，其特征在于，应用至少一种本文所述的交联剂或功能化剂。
附图说明
图1是根据本发明在纸或非织造网中使用和/或结合本文所述的交联剂或功能化剂的可能性的示意图。
图2是显示测定本发明和现有技术的纸或非织造网的抗张强度的实验结果的图。
发明详述
在下文中将描述本发明的细节及其进一步的特征和优点。但是，本发明不限于下列具体的描述和实施方案，其仅用于说明的目的。
而且，本文中所作出的有关纸或非织造网的任何公开或示例性实施方案也可适用于如本文所述的用于生产纸或非织造网的方法和如本文所述的交联剂或功能化剂的用途中，反之亦然。
本发明提供了一种包含纤维的纸或非织造网，其特征在于，其包含至少一种如本文所述的交联剂或功能化剂。
所述至少一种交联剂或功能化剂的分子量特别不超过1000g/mol，特别不超过750g/mol，特别不超过600g/mol，特别不超过500g/mol，特别不超过400g/mol，特别不超过300g/mol，且通常超过50g/mol，特别是超过75g/mol。换言之，所述至少一种交联剂或功能化剂尤其不是聚合物。
特别是，所述纸或非织造网优选不包含聚合物(合成)粘合剂，如丙烯酸酯聚合物粘合剂。
本发明的纸或非织造网可以例如为包装材料，如用于食品包装的包装材料；过滤材料，如用于注入饮料例如茶和咖啡的过滤材料，或用于油过滤的过滤材料；复合层压材料，如覆盖纸；镀金属纸，如适用于标签或包装的镀金属纸；非织造气流成网，如卫生和个人护理产品、家庭护理产品例如湿巾、毛巾、餐巾和桌布，特种纸例如墙纸、床垫和家具垫料。优选的是，本发明的纸或非织造网是用于茶和咖啡的过滤材料。
本发明的纸或非织造网可以特别是气流成网或湿法成网(wet-laid web)。
本文所用的表述“包含(comprising)”或“包含(comprise)”不仅包括“包含”的含义，还包括“基本由…所组成的(consisting essentially of)”或“基本由…所组成(consist essentially of)”以及“由…所组成的(consisting of)”或“由…所组成(consist of)”的含义。
术语“交联剂或功能化剂”表示能够优选通过共价键结合到纤维上并能够形成交联键或使纤维功能化的化合物。
本文使用的术语“交联(crosslinking)”或“交联键(crosslinkage)”不仅包括两种纤维或纤维与另外的添加剂如将会在下面进一步详细描述的多糖添加剂的连接，还包括在一种纤维内的交联。本文使用的术语“交联”或“交联键”特别包括纸或非织造网内在内部中)的连接(例如两种纤维的连接、纤维和另外的添加剂的连接，和/或在一种纤维内的交联)，且特别不仅是在纸或非织造网表面上的连接。
本文使用的术语“功能化(functionalization)”表示提供给纸或非织造网特定的一种功能或特定的多种功能，如亲水性、疏水性、润湿性、附着性、稳定性、抗张强度以及抗性等。
在本发明的纸或非织造网中，至少一部分交联剂或功能化剂结合到，特别是共价结合到纤维上。本文所用的术语“至少一部分(at least a part of)”可以表示在如将会在下面进一步详细描述的羧酸化合物和次磷酸盐化合物的组合的情况中，羧酸化合物和次磷酸盐化合物中的至少一种类型的化合物结合到纤维上，例如至少羧酸结合到纤维上。本文所用的术语“至少一部分”也可以表示在纸或非织造网中含有的交联剂或功能化剂的至少5％、特别是至少10％、特别是至少20％、特别是至少30％、特别是至少40％、特别是至少50％、特别是至少60％、特别是至少70％、特别是至少80％、特别是至少90％、以及特别是至少100％的量结合到纤维上。
本发明的交联剂或功能化剂选自羧酸、卤代杂芳环化合物及其盐。
羧酸优选选自二羧酸、聚羧酸、氨基酸及其盐，更优选选自脂肪族二羧酸、脂肪族聚羧酸、脂肪族氨基酸及其盐。
二羧酸特别优选是马来酸、富马酸、草酸、丙二酸、丁二酸、己二酸及其盐。
聚羧酸特别优选是柠檬酸、丁烷四羧酸、亚氨基二琥珀酸及其盐。
氨基酸特别优选是天冬氨酸、谷氨酸及其盐。
羧酸最优选是柠檬酸及其钠盐、丁烷四羧酸特别是丁烷1,2,3,4-四羧酸及其钠盐、以及天冬氨酸。
卤代杂芳环化合物可含有一个或多个卤原子，彼此独立地选自F、Cl、Br和I。
卤代杂芳环化合物优选是卤代含氮杂芳环化合物及其盐，更优选是氯代含氮杂芳环化合物及其盐。
卤代杂芳环化合物特别优选是卤代三嗪化合物及其盐，特别是氯代三嗪化合物及其盐。
卤代杂芳环化合物最优选是4,6-二氯-1,3,5-三嗪-2-醇及其钠盐(NHDT)。
本发明最优选的交联剂或功能化剂是柠檬酸和4,6-二氯-1,3,5-三嗪-2-醇及其钠盐(NHDT)。
本发明人已发现，在交联剂或功能化剂包含羧酸的情况下，该羧酸为其酸式形式是有利的。换言之，羧酸的盐可能是次优选的。
本发明人已发现，在交联剂或功能化剂包含羧酸如二羧酸或聚羧酸，特别是柠檬酸的情况下，包含额外至少一种次磷酸盐化合物是有利的。所述至少一种次磷酸盐(phosphinate)化合物可以特别是次磷酸(phosphinic acid,H3PO2)的盐，特别是其钠盐，如次磷酸钠(sodium phosphinate,NaH2PO2)。由此，本发明的纸或非织造网在可生物降解性和抗张强度方面显示出特别有利的性能。基于纸或非织造网的总重量，在纸或非织造网中次磷酸盐化合物试剂的含量优选为0.1-10wt％，特别是0.2-5.0wt％，特别是0.3-4.0wt％，特别是0.4-3.0wt％，特别是0.5-2.5wt％。
基于纸或非织造网的总重量，在本发明的纸或非织造网中交联剂或功能化剂的含量优选高至50wt％，更优选0.01-40wt％，还更优选0.02-30wt％，还更优选0.03-25wt％，还更优选0.04-20wt％，还更优选0.05-15wt％，且最优选0.1-10wt％，特别是0.5-10wt％，特别是1.0-10wt％，如1.0-5.0wt％或2.0-10wt％。这些含量值应被理解为包括所述至少一种次磷酸盐化合物(如果存在的话)的含量。
例如，纸或非织造网可以包含1.0-5.0wt％的羧酸(如柠檬酸)和0.5-2.5wt％的至少一种次磷酸盐化合物(如次磷酸钠)，所有含量基于纸或非织造网的总重量。
在一个优选实施方案中，本发明的纸或非织造网还包含至少一种多糖添加剂。多糖添加剂的优选实例包括羧甲基纤维素(CMC)、淀粉、海藻酸或海藻酸盐、果胶及其混合物，特别是羧甲基纤维素(CMC)。多糖添加剂优选通过交联剂或功能化剂连接(结合，如共价结合)到纸或非织造网的纤维上。
除包含交联剂或功能化剂外，通过包含至少一种多糖添加剂可赋予本发明的纸或非织造网其它功能，并且可进一步提高本发明的纸或非织造网的抗张强度。
基于纸或非织造网的总重量，在本发明的纸或非织造网中的至少一种多糖添加剂的含量优选高达30wt％，特别为0.1-20wt％，特别为0.25-15wt％，特别为0.5-10wt％，特别为0.75-5.0wt％，特别为1.0-3.0wt％。
例如，纸或非织造网可以包含1.0-5.0wt％的羧酸(如柠檬酸)、0.5-2.5wt％的至少一种次磷酸盐化合物(如次磷酸钠)和1.0-3.0wt％的至少一种多糖添加剂(如CMC)，所有含量基于纸或非织造网的总重量。
取决于纸或非织造网的预期用途，本发明的纸或非织造网中可以含有其它添加剂。特别是当用作覆盖纸时，例如可以含有耐磨粒子或硬质材料粒子，如刚玉或玻璃珠。
在本发明的纸或非织造网中含有的纤维并没有特别限制，只要其可以结合至交联剂或功能化剂即可。
适合的纤维是天然纤维或纤维素纤维。优选的实例包括纤维素、粘胶、莱赛尔、棉、大麻、马尼拉、黄麻、剑麻、人造纤维和蕉麻的纤维以及其它纤维，并且还包括软木浆和硬木浆的纤维。
其它适合的纤维是合成纤维或可热封纤维。优选的实例包括聚乙烯(PE)、聚丙烯(PP)、聚酯如聚对苯二甲酸乙二醇酯(PET)和聚(乳酸)(PLA)的纤维。其它优选实例包括双组分纤维，优选皮-芯型双组分纤维。双组分纤维是由具有不同物理和/或化学性质，特别是不同熔化性质的两种类型的聚合物组成。皮-芯型双组分纤维通常具有较高熔点成分的芯和较低熔点成分的皮。适用于本发明的双组分纤维的实例包括PET/PET纤维，PE/PP纤维、PET/PE纤维和PLA/PLA纤维。
还可使用上述纤维的混合物，如两种或多种天然纤维的混合物、两种或多种合成纤维或可热封纤维的混合物、天然纤维和合成纤维或可热封纤维的混合物以及其任意组合。
纸或非织造网的每平方米克重没有特别限制。通常，纸或非织造网的每平方米克重为5-2000g/m2，优选50-600g/m2或8.5-120g/m2。
纤维的长度和粗度(coarseness)没有特别限制。纤维的粗度被定义为纤维的每单位长度的重量。通常，天然纤维或纤维素纤维的长度为1-15mm，优选3-10mm。通常，天然纤维或纤维素纤维的粗度为30-300mg/km，优选70-150mg/km。通常，合成纤维和可热封纤维的长度为1-15mm，优选2-12mm。适用于本发明的可热封纤维的粗度通常为0.1-5分特(dtex)，优选0.3-3分特。
图1是根据本发明在纸或非织造网中使用和/或结合交联剂或功能化剂的可能性的示意图。
在实施例A中，在一种纤维内通过交联剂或功能化剂发生交联，这增强了纤维的机械稳定性，如耐磨性或树脂织缩(resin take-up)抗性。
在实施例B中，使交联剂或功能化剂结合到纤维上，由此赋予纤维特定的一种功能或特定的多种功能。例如，当聚羧酸或氨基酸，如柠檬酸、丁烷四羧酸、天冬氨酸或其盐用作交联剂或功能化剂时，本发明的纸或非织造网的亲水性和润湿性可得到提高。当卤代杂芳环化合物如4,6-二氯-1,3,5-三嗪-2-醇或其钠盐(NHDT)用作交联剂或功能化剂时，本发明的纸或非织造网特别是在碱性条件下的疏水性和湿抗张强度可得到提高。而且，纤维的耐磨性可得到增强。
在实施例C中，两种纤维通过交联剂或功能化剂交联，由此改善本发明的纸或非织造网的特性，如干燥和潮湿状态下的抗张强度、疏水/亲水润湿性和树脂织缩抗性。
在实施例D中，交联剂或功能化剂通过自身将多糖添加剂结合到纤维上，由此赋予本发明的纸或非织造网其它功能，并进一步提高了本发明的纸或非织造网的特性如抗张强度。
在实施例E中，两种纤维通过交联剂或功能化剂以及多糖添加剂进行交联，由此进一步改善了本发明的纸或非织造网的特性如抗张强度。
当然，除上述示例性的实施例A至E外，其它可能性和组合也是可以的，且本发明的纸或非织造网可以包括上述示例性的实施例A至E以及所述其它可能性和组合的任意组合。
本发明的交联剂或功能化剂优选具有至少两个能够结合到纤维上以及任选的多糖添加剂上的部分(moiety)。
例如，作为本发明优选的交联剂或功能化剂的柠檬酸和丁烷四羧酸分别包含三个和四个羧酸部分，其能够例如与纤维和/或任选的多糖添加剂的羟基形成酯键。没有必要使这些交联剂或功能化剂的所有羧酸部分都进行反应，任何余留的未反应羧酸部分可有助于本发明的纸或非织造网的进一步功能化。
作为本发明其它优选的交联剂或功能化剂，4,6-二氯-1,3,5-三嗪-2-醇钠盐(NHDT)包含两个可被独立地取代的氯原子。而且，通过NHDT的氮原子可以形成键。
作为示例性的说明，4,6-二氯-1,3,5-三嗪-2-醇钠盐(NHDT)与纤维素纤维(OH-Cell)和/或羧甲基纤维素(CMC)的一些典型反应式如下所示：
(1)
(2)
(3)
本发明的纸或非织造网可以通过常规造纸方法使用造纸机，优选斜网造纸机(inclined wire paper machine)，或通过干法成型气流成网非织造制造方法(dry-forming air-laid non-woven manufacturing process)进行制备，其中额外应用如本文限定的至少一种交联剂或功能化剂。在例如US2004/0129632A1中描述了一种常规造纸方法，其公开内容通过引用并入本文。在例如US 3905864中描述了一种适合的干法成型气流成网非织造制造方法，其公开内容通过引用并入本文。
本发明的用于生产纸或非织造网的方法的特征在于，应用至少一种如本文所限定的交联剂或功能化剂。
交联剂或功能化剂的优选应用方式如下：
尽管在下列优选应用方式的描述中用NHDT作为本发明的交联剂或功能化剂的实例以及CMC作为本发明的任选的多糖添加剂的实例，但这些优选的应用方式不应被解释为限于这些具体的实施例，而是可以适用于本发明的其它交联剂或功能化剂、纤维和任选的多糖添加剂。
(1)在单独的步骤中应用NHDT和CMC：
(a)将NHDT应用于纤维素纤维，以产生Cell-O-NHMT(pH、温度)
(b)冲洗
(c)将CMC应用于Cell-O-NHMT，以产生Cell-O-NHMT-CMC(pH、温度)
(d)任选地冲洗
(2)在一个步骤中应用NHDT和CMC的混合物：
(a)将NHDT和CMC应用于纤维素纤维
(b)任选地冲洗
(3)应用先前功能化的CMC
(a)将先前功能化的CMC(NHDT-CMC)应用于纤维素纤维，以产生CMC-NHT-O-Cell
(b)任选地冲洗
后一种方法即应用方式(3)，在下列方面特别有利，即对于任何剩余的过量NHDT的冲洗步骤不是必需的。
其各种变型是可行的，例如交联剂或功能化剂和任选的多糖添加剂可在应用于造纸机之前加到纤维上，由此，交联剂或功能化剂和纤维以及任选的多糖添加剂全部(in-mass)发生反应。
本文所述的交联剂或功能化剂可用于纸或非织造网，例如包装材料，如用于食品包装的包装材料；过滤材料，如用于注入饮料例如茶和咖啡的过滤材料，或用于油过滤的过滤材料；复合层压材料，如覆盖纸；镀金属纸，如适用于标签或包装的镀金属纸；非织造气流成网，如卫生和个人护理产品、家庭护理产品例如湿巾、毛巾、餐巾和桌布，特种纸例如墙纸、床垫和家具垫料。优选地，本文所述的交联剂或功能化剂可用于茶和咖啡的过滤材料。特别地，本文所述的交联剂或功能化剂可用来赋予纸或非织造网(在干燥状态下和/或在潮湿状态下的)抗张强度、多孔性、润湿性、亲水性/疏水性和/或附着性。此外，本文所述的交联剂或功能化剂可用来赋予纸或非织造网可生物降解性。
实施例
已制备软木和蕉麻纤维混合物的纸或非织造网(参考例)。
已向如在参考例中使用的混合物中加入如下所示的另外的化合物，以制备本发明的实施例和对比例的纸或非织造网：
实施例1：海藻酸盐/柠檬酸(9％)
实施例2：NHDT/海藻酸盐(9％)
实施例3：NHDT/果胶(9％)
实施例4：NHDT 7.3％
实施例5：柠檬酸10％
对比例1：CMC 2％
对比例2：苯乙烯/丙烯酸酯(6％)
确定参考例、本发明的实施例和对比例的样品在干燥状态、潮湿状态以及另外包含6％NaOH(即碱性条件下)的潮湿状态下的抗张强度。根据ISO 1924-2来确定干抗张强度，并根据ISO 3781确定湿抗张强度。
结果示于图2中。
由这些结果可见，相比于仅使用多糖添加剂如CMC的常规纸(对比例1)，本发明的纸或非织造网特别在湿抗张强度方面具有优异性能。而且，本发明的交联剂或功能化剂表现出适合替代常规油基化合物如苯乙烯/丙烯酸酯共聚物(对比例2)。
虽然已通过具体的实施方案和实施例的方式对本发明进行了详细描述，但本发明不限于此，且在不背离本发明范围的情况下，可作出各种变化和修改。

Claims (15)

1.一种纸或非织造网，其包含纤维和至少一种选自羧酸、卤代杂芳环化合物及它们的盐的交联剂或功能化剂，
其中所述至少一种交联剂或功能化剂具有不超过1000g/mol的分子量，且
其中所述交联剂或功能化剂的至少一部分结合到所述纤维上。
2.根据权利要求1所述的纸或非织造网，其是气流成网或湿法成网。
3.根据权利要求1或2所述的纸或非织造网，其中所述交联剂或功能化剂选自二羧酸、聚羧酸、氨基酸、卤代含氮杂芳环化合物及它们的盐。
4.根据权利要求1或2所述的纸或非织造网，其中所述交联剂或功能化剂选自脂肪族二羧酸、脂肪族聚羧酸、脂肪族氨基酸、氯代含氮杂芳环化合物及它们的盐。
5.根据权利要求1或2所述的纸或非织造网，其中所述交联剂或功能化剂选自柠檬酸、丁烷四羧酸、马来酸、富马酸、草酸、丙二酸、丁二酸、己二酸、天冬氨酸、谷氨酸、亚氨基二琥珀酸、氯代三嗪化合物及它们的盐。
6.根据权利要求1或2所述的纸或非织造网，其中所述交联剂或功能化剂是4,6-二氯-1,3,5-三嗪-2-醇或其钠盐。
7.根据权利要求1或2所述的纸或非织造网，其中所述交联剂或功能化剂是柠檬酸。
8.根据权利要求1或2所述的纸或非织造网，其中所述交联剂或功能化剂包括羧酸，且进一步包括至少一种次磷酸盐化合物。
9.根据权利要求1或2所述的纸或非织造网，进一步包含至少一种多糖添加剂。
10.根据权利要求9所述的纸或非织造网，其中所述多糖添加剂是选自由羧甲基纤维素、淀粉、海藻酸、海藻酸盐和果胶组成的组的至少一种。
11.根据权利要求9所述的纸或非织造网，其中所述多糖添加剂通过所述交联剂或功能化剂连接到所述纤维上。
12.根据权利要求1或2所述的纸或非织造网，其中所述纤维包括纤维素纤维。
13.根据权利要求1或2所述的纸或非织造网，其中所述纤维包括可热封纤维。
14.一种用于生产纸或非织造网的方法，其特征在于，应用至少一种权利要求1-8中任一项所限定的交联剂或功能化剂。
15.权利要求1-8中任一项所限定的交联剂或功能化剂在纸或非织造网中的用途。
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