CN1100035A - 复合薄膜 - Google Patents

复合薄膜 Download PDF

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CN1100035A
CN1100035A CN93121255A CN93121255A CN1100035A CN 1100035 A CN1100035 A CN 1100035A CN 93121255 A CN93121255 A CN 93121255A CN 93121255 A CN93121255 A CN 93121255A CN 1100035 A CN1100035 A CN 1100035A
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film
resin
glue
particle board
roll web
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CN1039212C (zh
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F·M·莫迪德
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Casco Adhesives AB
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Casco Nobel AB
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Abstract

本发明公开了一种适于在制造叠层颗粒板的过 程中连续覆盖颗粒板的薄膜，该薄膜可透过水蒸汽并 浸有半固化的浸渍树脂，在其一表面涂有部分固化的 胶层，另一面有一完全固化的漆层，该薄膜可以透过 在制造叠层颗粒板过程中产生的气体。本发明还公 开了一种制造这种薄膜的方法和用连续直接叠层工 艺制造叠层颗粒板的方法。

Description

本发明涉及一种适用于制造叠层颗粒板的薄膜，一种制造这种薄膜的方法以及使用这种薄膜制造叠层颗粒板的方法。
在制造装饰箔时一般使用未经处理的重量在每平方米40至140g之间的纤维纸。纸可以用密胺热固性树脂浸渍或不经处理。这种箔需要用粘结剂进行叠层。浸渍的程度和使用树脂的百分比对纸的内部结合强度有着直接的影响，而且对其孔隙度，切割质量及机加工性能也有影响。基本上未处理过的纸可能含有少量的树脂（2-3%），这一般是在制造过程中加入的。纸在传送时可以带有上表面涂漆层或是在叠层后再涂上表面漆层。
预浸渍纸是在造纸的过程中用一种树脂体系处理过的纸，树脂体系包括例如密胺或脲甲醛，通常是与两烯酸一起使用，这可以使纸在树脂完全固化后保持其柔性。通过一个精整体机和或在造纸机上或是其后进行砑光来供入树脂。砑光为树脂提供了一个优良的可印刷表面，而且这种表面很容易涂覆。这种纸可以用化学法糙化，而且也可以预涂热熔粘结剂。
纸也可以在它们制造出来以后再用上述类似的树脂体系进行处理，这就是所谓后浸渍纸。在这些纸中，纸的纤维被树脂包封，而且纸中的孔隙和空隙也被树脂充满。这些纸的上表面可以有涂层，也可以带有在制造点施涂的热熔性粘结剂。
在按现有技术制造叠层颗粒板时，首先要压制颗粒板或附聚物，在最后的压制工序之后送去形成平滑的表面，然后涂一层胶，再覆盖上一层如上所述的薄膜或箔片，最后加热并压紧层压板。按照现有技术，这种制造叠层颗粒板的方法可以是连续进行或是分步进行。
用现有技术的箔或薄膜在直接叠层加工时颗粒板产生的气体将会封闭在板内，这会造成在薄膜和颗粒板之间形成气泡，这种气泡可能导致薄膜损坏。
本发明的一个目的是提供一种薄膜，通过利用这种薄膜将会克服上述现有技术的缺陷。
本发明的另一个目的是提供一种方法，通过利用这种方法获得一种具有适当性能的薄膜，这些性能使其特别适于用连续法制造又叠层颗粒板。
本发明的再一个目的是提供一种利用这种薄膜以连续制造叠层颗粒板的方法。
在附图中：
图1是根据本发明的制造薄膜的方法的示意图；
图2是根据本发明的直接叠层方法的示意图；
图3是本发明薄膜和现在使用的标准膜的水蒸汽透过率（3a）和水蒸汽渗透度（3b）与时间之间的曲线图。
本发明的薄膜包括一层30至150g/cm2重量的基纸，基纸浸有几乎完全固化的并能够透过在制造叠层颗粒板过程中颗粒板（附聚物）内形成的气体的树脂。进一步讲，该薄膜的朝向颗粒板一面有一个部分固化的胶层，薄膜的上表面有一完全固化的漆或清漆层。这就是说完成后的薄膜包括一层可渗透气体的完全固化的漆层，一层浸渍树脂混合物层，它也能渗透气体和处于半固化状况的和至少95%固化的，以及一层部分固化的胶层。
本发明薄膜的重要特性是它的对水蒸汽的透过性和对水蒸汽的可渗透性。这些特性可根据ASTM E-96标准测定。在制造叠层板时，本发明的薄膜的水蒸汽透过性和水蒸汽渗透性都要高于现有技术中使用的标准膜的相应特性。图3和表1中所示的是根据ASTM E-96进行测定的，这些特性的测定值作为时间的函数，其中示出了对本发明的薄膜和现有技术标准膜测得的透过和渗透值。此外，测量了没有胶层的本发明薄膜的这些特性，由于事实上在叠层加工中所述的胶在连续压力机中是熔融状态，固此在所述加压过程中不会对水蒸汽的透过性或渗透性造成任何实质程度的影响。在所述测量中所用的薄膜组成如下：
1、本发明薄膜：
-纸基 70g/m2
-浸渍树脂：    脲甲醛树脂    38%
丙烯酸    38%
水    24%
-树脂饱和度：    26%
固化度：    97%
-胶：    蜜胺树脂＋聚乙烯醇
-胶层： 15g/m2，干的
固化度：    93%
-漆：    聚酯/甲氧甲基蜜胺
-漆层： 10g/m2，干的
2、无胶的本发明薄膜：
与1相同但没有15g/m2的干胶层。
3、在现有技术中使用的标准薄膜：
-纸基 71g/m2
-浸渍树脂    脲甲醛树脂    80%
丙烯酸    12%
水    6%
固化度：    完全固化
-树脂饱和度：    33%
-漆1：    丙烯酸
-漆1层： 8g/m2
-漆2：    聚酯/甲氧甲基蜜胺
-漆2层： 10g/m2
湿度                50％面积              18.1cm2温度             25.5℃蒸气压            24.5mmHg
表1
标准膜  本发明薄膜  未涂胶的本发明薄膜
时间,
水蒸汽  渗透  水蒸汽  渗透  水蒸汽透过
小时  渗透率
透过率  率  透过率  率  率
24  9.21  0.75  13.35  1.09  19.11  1.56
48  10.47  0.86  13.24  1.08  17.03  1.39
53  10.95  0.89  14.18  1.16  17.72  1.45
72  10.74  0.88  12.74  1.04  15.19  1.24
89  10.86  0.89  12.11  0.99  14.28  1.17
96  11.22  0.92  12.37  1.01  14.39  1.17
160  10.19  0.83  11.57  0.94  13.81  1.13
168  10.36  0.85  11.67  0.95  13.48  1.10
192  10.22  0.83  11.65  0.95  13.52  1.10
216  9.85  0.80  11.64  0.95  13.30  1.09
240  9.78  0.80  11.63  0.95  13.35  1.09
%
从图3和表中可见本发明薄膜根据ASTM E-96测得的水蒸汽透过率大于11.5g.h-1.m-2，水蒸汽渗透率至少为0.94kg.pa-1.s-1.m-2。没有胶层的本发明薄膜的水蒸汽透过率至少为13.3，水蒸汽渗透率至少为1.09。现有技术的标准膜的相应值为：水蒸汽透过率低于11.2，水蒸汽渗透率低于0.92。从比较可清楚地看到本发明薄膜的水蒸汽透过率和水蒸汽渗透率更优于现有技术薄膜。因此，本发明薄膜在有胶层时应当具有至少11g.h-1.m-2的水蒸汽透过率，最好是至少12.5，在没有胶层时至少为13g.h-1.m-2，并且其水蒸汽渗透率在有胶层时至少为0.9kg.pa-1.s-1.m-2，最好至少1.05，在没有胶层时至少应为1.1kg.pa-1.s-1.m-2
与现有技术使用的预浸渍箔相比本发明薄膜有较大的厚度和硬度。这些特性使该薄膜能较好地掩饰板表面的不规则性，这意味着在叠层加工前对送交的颗粒板的要求不像现有技术方法那样苛刻。
用于制造薄膜的漆必须完全符合具有良好耐热性的条件。适用的漆是那些含有聚酯或丙烯酸树脂作为粘合剂和醚化的蜜胺，例如甲氧甲基蜜胺，或甲氧基脲作为交联剂。用一种强酸作为固化反应的催化剂。在使用丙烯酸类似或聚酯漆时，还可以用紫外线辐射固化。使用聚氨基甲酸乙酯（饱和的）漆中可能的，但是很贵。
脲-甲醛树脂和丙烯酸乳化液的组合物适于用作浸渍树脂。脲-甲醛树和丙烯酸乳化液之间的适当重量比是从75∶25至40∶60，最好是从70∶30至50∶50，这要取决于丙烯酸乳化液的硬度。浸渍后树脂半固化至95%以上的固化度，最好为96至98%。
适用于本发明薄膜的胶为蜜胺-甲醛和/或脲-甲醛树脂。热固性丙烯酸树脂也可以作为胶使用。胶用已知的方法部分固化，适宜的固化度为90-95%，最好为91-94%。
在制造本发明薄膜时必须注意某些参数。未经浸渍的纸的孔隙率应当在某种范围之内，例如，8-20秒/100ml的Gurley孔隙率，最好是10-13秒/100ml，其平滑度根据Bendtsen为80-150ml/分，最好是90-110ml/分。未处理过的纸的基本重量为从30至150g/m2，适宜的重量为70-80g/m2。按照本发明一种适用的本发明的薄膜（箔）的例子，其终重量为115-120g/m2，其中涂漆的干重量为10-12g/m2，浸渍树脂的重量为22-24g/m2，这意味着当基纸重量为70g/m2时树脂饱和百分比为24至26%。
浸渍树脂的重量最好不要低于某个限度，即18%。
制造薄膜的方法，这是本发明的另一个目的，包括如下基本步骤：
a）用能使颗粒板中产生的气体透过的树脂浸渍卷筒基纸的纤维素基底，纸的重量为70-80g/m2
b）将浸渍了树脂的卷筒纸通过一个炉子，使浸渍树脂半固化，
c）半固化的浸渍卷筒纸通过一个胶槽，为其提供一胶层，
d）将涂了胶的部分固化的浸渍卷筒纸通过一个炉子，使其进一步固化和干燥，
e）将卷筒纸通过一漆槽，为其上表面提供漆层，然后，
f）将涂过漆和带有胶层的浸渍卷筒纸通过一个炉子，进一步固化和干燥，由此获得完成的薄膜。
如果在使用丙烯酸或聚酯漆时，固化由紫外线辐射完成，炉子之前需设置紫外线隧道。
完成的薄膜可以输入颗粒板生产线，该生产线用于直接连续制造叠层板，其中颗粒板是由浸胶木屑块构成的。在这一步骤可以向木屑块输入一条或两条薄膜以便覆盖木屑块的一面或两面。
在这个叠层阶段，薄膜可以渗过水蒸汽是致关重要的，因为在加压时胶冷凝，并会产生水，这水必须通过薄膜逸出，以避免产生气泡或/和爆破。从压力机输出后获得的颗粒板可直接用于装饰目的。
刚才提到的叠层阶段应当与为获得同样产品的标准方法相比较。在标准制造的最后加压阶段中，被送出的是制造的粗颗粒板（木屑块）（其厚度必须标准）。在此之后把胶涂在板的叠加薄膜的那个表面，并把板和标准膜一起加压以便干燥和固化胶。这种按照现有技术的方法比本发明的直接叠层法更麻烦和要花费更多的时间。
在图1中，带有颜色的纸（1）的卷筒用作薄膜的基纸。（2）是盛有适宜的浸渍树脂组合物的树脂槽，（3）是把卷筒纸导向树脂槽的导向辊，在树脂槽的（4）和（5）区，由于毛细作用树脂浸透卷筒纸。当离开槽（2）时，两刮板（6）刮削卷筒纸以除去过量的树脂。
浸渍后的卷筒纸穿过炉子（7），在其中被加热，以便干燥和部分固化浸渍树脂。然后用水冷辊冷却卷筒纸。
在这炉处理之后，浸渍后的卷筒纸通过一个盛有适宜的胶或胶的混合物的胶槽（8），利用一个与卷筒纸运动方向逆向旋转的辊子把胶涂在卷筒纸上。涂胶的量用螺纹杆（10）测量，接着卷筒纸通过炉（11）热处理，之后用吹风机（12）吹冷风冷却。
用一个类似物涂胶的系统为卷筒纸的上表面在一个漆槽（13）中涂漆，在漆槽（13）中辊子（14）以逆着卷筒纸运动的方向旋转，涂漆的量由螺纹杆（15）测量。
应当注意的是，如需要，上述涂漆步骤可以置于涂胶步骤之前进行，这意味着涂胶和漆可以以任意顺序进行，即或是在涂漆之前涂胶，或是在上胶之前涂漆。
图2显示了一种本发明的直接叠层的方法，利用这种方法制造一种叠层颗粒板，在其中浸有胶的木屑块（17）的两侧都覆盖了本发明的薄膜（18，19），两个薄膜可以是相同组成或不同组成。两侧都覆盖了薄膜的颗粒板在连续压力机（20）中挤压，连续压力机（20）包括：两条最好是经过渗铬处理的不锈钢带张紧在上下两对大尺寸辊筒之间，并以相反的方向旋转。钢带辊筒安装在机架上并被加热。两个外进料辊一般由直流驱动单元驱动。两条钢带彼此相向，穿过加热区和加压区，在这里从前方插入的木屑块上的浸胶被固化。
下面的实施例显示了本发明的薄膜及其制造方法（实施例1），和用本发明的薄膜直接叠层加工的方法（实施例2）。这些实施例仅用作说明，其意图不是对发明进行任何限制。
实施例1
在一如图1所示结构的装置中以下述的方式制造本发明薄膜。
一卷作为薄膜基底的染有颜色的重量为70g/m2的卷筒纸（ⅰ）通过导辊（3）送至盛有树脂组合物的槽（2），树脂组合物包括：
Ⅰ）脲-甲醛，801，95kg，脲-甲醛的分子比为1∶2，
Ⅱ）一种丙烯酸乳化液，601，63.6kg，例如Rohm和Hass生产的Primal FS-100，和
Ⅲ）一种丙烯酸乳化液，201，21.1kg，例如Primal HA-12。
浸渍树脂组合物在区域（4）和（5）通过毛细作用施加。用两刮板（6）除去任何过量的树脂。必须施加正确量的树脂，以便为薄膜提供必要的机械性能和为完成后薄膜提供必要的可透气性。浸渍槽也盛有851的水和一种乳化剂。
在浸渍槽之后，卷筒纸通过炉（7），在炉中卷筒纸在90至120℃温度之间被加热15秒，以及到固化度大约为97%的半固化树脂。
然后用水冷辊冷却卷筒纸，其后使其通过胶槽（8），在此用与卷筒纸运动方向逆向旋转的辊（9）涂胶。胶包括蜜胺/甲醛的分子比为1∶1.8的蜜胺/甲醛树脂，和一种部分皂化的聚乙烯醇。这种部分皂化的聚乙烯醇改善胶对浸渍后基纸的渗透性。
施胶量是用螺纹杆（10）控制的，以使完成后的薄膜每平方米的干胶在13和15g之间。
接着使卷筒纸通过炉（11），在温度为100和150℃之间行进7秒，其后用吹风机（12）吹冷空气冷却。得到大约93%的固化度。
接下来使卷筒纸通过一个与涂胶类似的系统为卷筒纸在漆槽（13）中涂漆，在漆槽中辊（14）的旋转方向与卷筒纸运动方向相反，用螺纹杆（15）控制涂漆量。
最后使薄膜通过炉（16）在120和170℃之间温度干燥和固化大约15秒，其后用水冷辊冷却薄膜。
实施例2
一个浸有22-24g/m2重量的浸渍树脂混合物的，一面有一干重最重为13-15g/m2的胶层。另一面有一重量为10-12g/m2漆层的，最终重量为115-120g/m2的本发明的薄膜被用来在如图2所示的装置中制造本发明的叠层颗粒板。包括浸有胶液木屑的块状物的颗粒板（17）与用来覆盖块状物两面的如实施例那样制备的两条薄膜一起送入用来制造颗粒板的连续压机中。薄膜可以透过水蒸汽，这样在压制过程中胶凝结并产生水时，水可以通过薄膜逸出，避免了产生气泡或/和爆破。在压机的出口处获得两面都被覆盖的颗粒板，这种板可以直接用于装饰目的。在压制时所用压制速度为10m/分，带温为165℃。
图3：-■-现有技术的标准薄膜
-□-按照本发明的薄膜
-◆-按照本发明不带胶层的薄膜

Claims (12)

1、一种可以用于颗粒板的，在直接连续法中制造叠层颗粒板的薄膜，其特征在于该薄膜可以透过水蒸汽，它包括一个重量为30至150g/m2的浸渍了树脂的基纸，该树脂的半固化度为大于95%并可以透过在制造叠层颗粒板过程中颗粒板内产生的气体，该薄膜与颗粒板接触的一面有一部分固化的胶层，其另一面，上表面，有一完全固化的漆层它可以使在制造叠层颗粒板过程中产生的气体透过。
2、如权利要求1所述的薄膜，其特征在于它的水蒸汽透过率根据ASTM E-96标准大于11g.h-1.m-2，其水蒸汽渗透率至少为0.9kg.pa-1.s-1.m-2
3、如权利要求2所述的薄膜，其特征在于使用脲-甲醛树脂和丙烯酸乳化液组合物作为浸渍树脂，其重量比为从75∶25至40∶60，最好是从70∶30至50∶50。
4、如权利要求1-3之一所述的薄膜，其特征在于使用的胶是蜜胺-甲醛树脂，这种胶使产品具有防水性。
5、如权利要求1-3之一所述的薄膜，其特征在于使用的胶是脲-甲醛树脂。
6、如权利要求1-3之一所述的薄膜，其特征在于使用的胶是热固性丙烯酸树脂。
7、如权利要求1-6之一所述的薄膜，其特征在于使用的上表面漆是聚酯/甲氧甲基蜜胺漆。
8、如权利要求1-7之一所述的薄膜，其特征在于使用的上表面漆是丙烯酸/甲氧甲基蜜胺漆。
9、如权利要求1-6之一所述的薄膜，其特征在于使用的上表面漆是用紫外线辐射固化的丙烯酸或聚酯漆。
10、制造可透过水蒸汽薄膜的方法，该薄膜可以用连续覆盖颗粒板的方式叠加在颗粒板上，其特征在于利用下述步骤获得该薄膜：
a）用浸渍树脂（2）浸渍纤维素卷筒纸（1），该树脂可以透过附聚物内产生的气体，
b）使浸渍过树脂的纤维素卷筒纸通过炉子（7）加热并半固化树脂，
c）使浸渍后半固化的纤维素卷筒纸通过胶槽（8），
d）使浸渍后，半固化并挂上胶层的纤维素卷筒纸通过炉子（11）使其部分固化，
e）使纤维素卷筒纸通过漆槽（13）使卷筒纸在上表面获得一油漆涂层，然后
f）使卷筒纸通过炉子（16）固化漆层，
在上述步骤中如果需要步骤e）可以在步骤c）和d）之前进行；通过以上步骤得到一个具有完全固化的上表面漆层的，浸渍了半固化浸渍树脂混合物的和部分固化的胶底层的，可透过水蒸汽的纤维素薄膜。
11、如权利要求10所述的方法，其特征在于当使用可用紫外线辐射固化的丙烯酸或聚酯漆作为上表面漆时，炉子（16）之前应设置一个紫外线隧道。
12、用连续直接叠层过程制造叠层颗粒板的方法，其特征在于在移动的浸胶木屑层的一面或两面覆盖一层能渗透蒸汽的薄膜，它包括浸渍了脲-甲醛树脂和丙烯酸乳化液组合物的浸渍树脂并半固化至大于95%固化度的纤维素卷筒纸，卷筒纸与木屑层接触的表面上涂有一层部分固化的甲醛基底胶，卷筒纸的另一面涂有一层完全固化的耐热漆层，它包含聚酯或丙烯酸树脂作粘合剂，在那里浸胶木屑层和薄膜一起送至连续压力机中加压，连续直接地制造叠层产品。
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AT (1) ATE137445T1 (zh)
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CN101709558A (zh) * 2009-12-11 2010-05-19 李忠良 一种浸渍装饰纸及其制作方法
CN104520080A (zh) * 2012-08-09 2015-04-15 瓦林格地板技术股份有限公司 粉末表面的单层散布
CN108018746A (zh) * 2017-12-04 2018-05-11 浙江盛龙装饰材料有限公司 一种水性涂布油漆纸及其生产工艺

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US6610358B1 (en) * 1999-03-12 2003-08-26 Premark Rwp Holdings, Inc. System and method for two sided sheet treating
CA2295416C (en) * 1999-03-12 2005-10-04 Premark Rwp Holdings, Inc. System and method for two sided sheet treating
DE19937759A1 (de) * 1999-08-10 2001-02-15 Basf Ag Verfahren zur Herstellung von Platten mit dekorativer Oberfläche
MC200022A1 (fr) * 1999-09-21 2001-03-28 Heller Ernst Systeme eco-decor traitement en phases muliples des papiers destines a la stratification des supports tels que les panneaux de particules les panneaux en fibres de bois les contreplaques ou autres
DE19963151A1 (de) * 1999-12-24 2001-07-05 Vits Maschinenbau Gmbh Anlage zum Imprägnieren von durchlaufenden Bahnen
US7074295B2 (en) * 2000-06-06 2006-07-11 Applied Extrusion Technologies, Inc. Labelling apparatus and method for correcting visual adhesive defects
US6551439B1 (en) 2000-06-06 2003-04-22 Applied Extrusion Technologies, Inc. Ultraviolet labeling apparatus and method
US6517661B2 (en) 2000-06-06 2003-02-11 Applied Extrusion Technologies, Inc. Labeling method employing radiation curable adhesive
US7229517B2 (en) * 2000-06-06 2007-06-12 Applied Extrusion Technologies, Inc. Labeling apparatus and method employing radiation curable adhesive
ES2339621B1 (es) * 2007-05-14 2011-01-04 Jesus Fco. Barberan Latorre Maquina de aplicacion de cola y barniz sobre laminas para cubrimientos.
EP2687373A1 (en) * 2007-11-16 2014-01-22 Välinge Photocatalytic AB Impregnation fluid and a method for manufacturing photocatalytic boards or panels using this fluid
NL1036705C2 (nl) * 2009-03-13 2010-09-14 Trespa Int Bv Werkwijze ter vervaardiging van een met hars geïmpregneerd decorpapier alsmede een decorpaneel.
PL2411141T3 (pl) 2009-03-23 2014-06-30 Vaelinge Photocatalytic Ab Wytwarzanie zawiesiny nanocząsteczek koloidalnych ditlenku tytanu z zachowaniem krystaliczności za pomocą młyna kulkowego z kulkami o rozmiarach mikrometrowych
IT1397259B1 (it) * 2009-12-04 2013-01-04 Max Canti Decorazione e smaltatura di protezione su biscotto ceramico o vetro in risparmio di energia; nobilitazione di altre superfici grezze di materiali diversi quali conglomerati legnosi o lapidei con contemporanea dotazione di finiture opache o lucide , o goffrate. processo , macchina , elementi ottenuti.
DE102010052044A1 (de) 2010-11-23 2012-05-24 Vits Technology Gmbh Verfahren und Anlage zum Imprägnieren und Trocknen einer durchlaufenden Papierbahn
RU2607558C2 (ru) * 2011-07-05 2017-01-10 Велинге Фотокаталитик Аб Изделия из древесины с покрытием и способ получения изделий из древесины с покрытием
AU2013235858B2 (en) 2012-03-20 2016-03-31 Valinge Photocatalytic Ab Photocatalytic compositions comprising titanium dioxide and anti-photogreying additives
US9375750B2 (en) 2012-12-21 2016-06-28 Valinge Photocatalytic Ab Method for coating a building panel and a building panel
EP3049485B1 (en) 2013-09-25 2019-04-10 Välinge Photocatalytic AB A method of applying a photo catalytic dispersion and a method of manufacturing a panel
PL4001504T3 (pl) * 2020-11-18 2024-03-11 Mm Kotkamills Absorbex Oy Papier bazowy, jego zastosowanie i struktura wielowarstwowa

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Cited By (3)

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Publication number Priority date Publication date Assignee Title
CN101709558A (zh) * 2009-12-11 2010-05-19 李忠良 一种浸渍装饰纸及其制作方法
CN104520080A (zh) * 2012-08-09 2015-04-15 瓦林格地板技术股份有限公司 粉末表面的单层散布
CN108018746A (zh) * 2017-12-04 2018-05-11 浙江盛龙装饰材料有限公司 一种水性涂布油漆纸及其生产工艺

Also Published As

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EP0670780A1 (en) 1995-09-13
ATE137445T1 (de) 1996-05-15
FI952478A (fi) 1995-05-22
MY109042A (en) 1996-11-30
DK0670780T3 (da) 1996-09-16
JPH08503748A (ja) 1996-04-23
JP2860707B2 (ja) 1999-02-24
US5714269A (en) 1998-02-03
CA2149910A1 (en) 1994-06-09
WO1994012347A1 (en) 1994-06-09
EP0670780B1 (en) 1996-05-01
CN1039212C (zh) 1998-07-22
GR3020427T3 (en) 1996-10-31
ES2087807T3 (es) 1996-07-16
BR9307507A (pt) 1999-06-01
FI952478A0 (fi) 1995-05-22
DE69302484T2 (de) 1996-09-19
KR950704115A (ko) 1995-11-17
KR0163470B1 (ko) 1998-12-15
DE69302484D1 (de) 1996-06-05

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