Stock material or miscellaneous articles – Hollow or container type article – Polymer or resin containing
Reexamination Certificate
2002-05-08
2004-05-25
Nolan, Sandra M. (Department: 1772)
Stock material or miscellaneous articles
Hollow or container type article
Polymer or resin containing
C428S420000, C428S421000, C428S422000
Reexamination Certificate
active
06740375
ABSTRACT:
This application is the national phase under 35 U.S.C. § 371 of PCT International Application No. PCT/JP00/06126 which has an International filing date of Sep. 8, 2000, which designated the United States of America.
FIELD OF THE INVENTION
The present invention relates to a fluorine-containing adhesive material which can firmly adhere to various substrates comprising an organic material such as various synthetic resins or an inorganic material such as glass and metal. The present invention also relates to a laminate and a shaped article comprising the same as well as a process for producing the shaped article.
RELATED ART
A fluorine-containing polymer has hitherto been used in many uses since it is excellent in heat-resistance, chemical resistance, weatherability, surface properties (a low frictional property and the like), and electrical insulation. Because, particularly in view of solvent resistance, the fluorine-containing polymer is insoluble in most of solvents and has high resistance to impregnation and penetration of solvents, the fluorine-containing polymer is widely used for a tube or a pipe lining for transportation of fuels, paints and chemical liquids.
On the other hand, a fluorine-containing polymer is generally insufficient in the mechanical strength and dimensional stability, and is expensive.
Then, in order to utilize the advantages of a fluorine-containing polymer to a maximum degree and minimize the defects, it has been extensively studied to develop a composite such as adhesion or lamination between the fluorine-containing polymer and other organic materials or inorganic materials.
However, it is difficult to adhere a fluorine-containing polymer directly to other materials. Even when the adhesion was tried with heat fusing, the adhesion strength was insufficient and, even if adhered to some extent, the adhesion strength was widely varied, which frequently resulted in the insufficient reliance on the adherability.
As a method for adhering a fluorine-containing polymer to other materials,
(1) a method for physically roughing with a sandblaster treatment a surface of a shaped article comprising one or both materials,
(2) a method of subjecting a shaped article formed from a fluorine-containing polymer to a surface treatment such as sodium etching, plasma treatment and photochemical treatment, and
(3) a method of adhesion with an adhesive have been mainly studied. However, regarding the above-mentioned (1) and (2), a treating step is necessary and, additionally, the productivity is low due to the complicated step. In addition, a type and shape of a substrate are restricted. A problem on appearance of the resultant laminate (coloration and flaw) easily arises. Further, even if these treatments are conducted, significant improvement of adhesion strength cannot obtained.
The study on the adhesive described in the above-mentioned (3) has been variously conducted. Generally used adhesives based on hydrocarbon materials have the insufficient adherability, and laminates comprising these adhesives have an adhesive layer insufficient in heat resistance, chemical resistance and water resistance. Accordingly, the adhesion strength can not be retained by a change in temperature and a change in circumstances, leading to the lack of reliance. In addition, it is difficult to impart to the laminates the above-mentioned excellent properties possessed by the fluorine-containing polymer.
On the other hand, the adhesion with an adhesive or an adhesive composition comprising a fluorine-containing polymer having a functional group has been studied.
For example, there are a report on the use of, as an adhesive, a fluorine-containing polymers obtained by graft-polymerization of a fluorine-containing polymer with a hydrocarbon monomer having a carboxyl group, a carboxylic anhydride residue group, an epoxy group, or a hydrolyzable silyl group, such as maleic anhydride and vinyl trimethoxysilane (for example, JP-A-7-18035 (18035/1995), JP-A-7-25952 (25952/1995), JP-A-7-25954 (25954/1995), JP-A-7-173230 (173230/1995), JP-A-7-173446 (173446/1995) and JP-A-7-173447 (173447/1995)), and a report in which an adhesive composition comprising a fluorine-containing copolymer obtained by copolymerizing a hydrocarbon monomer containing a functional group such as a hydroxylalkyl vinyl ether with tetrafluoroethylene or chlorotrifluoroethylene, and an isocyanate curing agent are used as an adhesive between a vinyl chloride polymer and ETFE (an ethylene/tetrafluoroethylene polymer) treated with corona discharge (for example, JP-A-7-228848 (228848/1995)).
The adhesive or adhesive composition comprising a fluorine-containing polymer obtained by graft-polymerizing or copolymerizing a hydrocarbon functional group-containing monomer does not have sufficiently improved heat-resistance so that degradation and foaming are caused at the use of an elevated temperature, leading to decrease in the adhesion strength, peeling or coloration. In the case of using the above-mentioned adhesive composition described in the JP-A-7-228848 (228848/1995), the fluororesin (ETFE) uneconomically requires the previously conducted corona discharge treatment.
In addition, it is reported that a fluorine-containing polymer having a functional group obtained by copolymerizing a perfluorovinylether compound containing arboxylic acid or its derivative with a fluorine-containing monomer is used as an adhesive or an adhesive composition. U.S. Pat. No. 4,916,020 discloses a laminate comprising a fluorine-containing polymer having a functional group introduced by copolymerizing perfluorovinylether having carboxylic acid group or its derivative with tetrafluoroethylene and the like.
However, this is a laminate in which the aforementioned fluorine-containing polymer having carboxylic acid group or the like is laminated on a metal or the other substrate via an adhesive resin such as an epoxy resin and a urethane resin and not a laminate in which the polymer is directly adhered to a metal, glass or other resins. Thus, there is a problem on heat-resistance, chemical resistance and solvent resistance of an epoxy resin or an urethane resin upon use. This report does not explicitly describe a method for adhering directly the fluorine-containing polymer to a metal, glass or other resins.
SUMMARY OF THE INVENTION
An object of the present invention is to solve the aforementioned problems of the prior art and provide a fluorine-containing adhesive material which can impart the firm direct adhesion strength to substrates such as a metal, a glass and a resin while maintaining the excellent properties such as chemical resistance, solvent resistance, weatherability, soil releasability and unstickness, possessed by a fluorine-containing polymer, as well as a laminate and a shaped article comprising the same. Another object of the present invention is to provide a fluorine-containing adhesive material which can firmly adhere to the above-mentioned substrates by, particularly, a heat melting adhesion, as well as a laminate comprising the same.
A fluorine-containing adhesive material according to the present invention comprises a fluorine-containing polymer having a specified range of number of carbonate groups and/or carboxylic acid halide groups at polymer chain terminals or side chains. The present inventors discovered that when a carbonate group and/or a carboxylic acid halide group are introduced into a fluorine-containing ethylenic polymer, a fluorine-containing adhesive material has surprisingly strong adhesion strength to synthetic resins, metals, glass and other materials, without the surface treatment and adhesive resin (such as primer) coating treatment usually conducted for the adhesion of fluororesin.
In addition, the present inventors discovered that when a total number of carbonate groups and carboxylic acid halide groups in the fluorine-containing ethylenic polymer is limited to a certain range, the evolution of gas caused by a chemical change of carbonate groups or carboxylic acid halide groups associated with an adhesion operation can be restr
Arase Takuya
Inaba Takeshi
Kato Taketo
Sagisaka Shigehito
Shimizu Tetsuo
Daikin Industries Ltd.
Nolan Sandra M.
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