Layered article with improved microcrack resistance and method of making

• US 6,376,064 B1
• Filed: 08/07/2000
• Issued: 04/23/2002
• Est. Priority Date: 12/13/1999
• Status: Expired due to Term

• Current Assignee: Sabic Innovative Plastics IP BV (Government of Saudi Arabia)
• Original Assignee: General Electric Company
• Inventors: Gasworth, Steven Marc, Olson, Daniel Robert, Katsamberis, Dimitris
• Primary Examiner(s): Nakarani, D. S.
• Application Number:
  US09/633,714
• Time in Patent Office: 624 Days
• Field of Search: 427/407.1, 427/489, 428/331, 428/332, 428/334, 428/335, 428/336, 428/412, 428/447, 428/451, 428/448
• US Class Current: 428/331
• CPC Class Codes: B05D 1/62 Plasma-deposition of organic layers plasma deposition in general C23C14/00, C23C16/00
• CPC Class Codes: B05D 2201/02 Polymeric substrate
• CPC Class Codes: B05D 7/52 Two layers
• CPC Class Codes: B05D 7/56 Three layers or more
• CPC Class Codes: C08J 2369/00 Characterised by the use of polycarbonates; Derivatives of polycarbonates
• CPC Class Codes: C08J 2433/06 of esters containing only carbon, hydrogen, and oxygen, the oxygen atom being present only as part of the carboxyl radical
• CPC Class Codes: C08J 2483/00 Characterised by the use of macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing silicon with or without sulfur, nitrogen, oxygen, or carbon only; Derivatives of such polymers
• CPC Class Codes: C08J 7/042 with two or more layers, where at least one layer of a composition contains a polymer binder
• CPC Class Codes: C08J 7/0427 with only one layer of a composition containing a polymer binder with more layers C08J7/042
• CPC Class Codes: C08J 7/043 Improving the adhesiveness of the coatings per se, e.g. forming primers adhesives in the form of films or foils characterised by the primer layers between the polymer carriers and the adhesives C09J7/50
• CPC Class Codes: C08J 7/046 Forming abrasion-resistant coatings; Forming surface-hardening coatings
• CPC Class Codes: C08J 7/18 using wave energy or particle radiation
• CPC Class Codes: Y10T 428/259 Silicic material
• CPC Class Codes: Y10T 428/265 1 mil or less
• CPC Class Codes: Y10T 428/31663 As siloxane, silicone or silane
• CPC Class Codes: Y10T 428/31667 Next to addition polymer from unsaturated monomers, or aldehyde or ketone condensation product

Abstract

The invention relates to a multilayer article which includes a substrate, a first layer comprising a partial condensate of a diorganodiorganooxysilane having the formula R₂Si(OR′)₂ or an organotriorganooxysilane having the formula RSi(OR′)₃, or both, where R is independently selected from the group consisting of alkyl groups containing about 1-3 carbon atoms, aromatic groups containing about 6-13 carbon atoms, the vinyl radical, the 3,3,3-trifluoropropyl radical, the gamma-glycidoxypropyl radical and the gamma-methacryloxypropyl radical, and R′ is independently selected from the group consisting of alkyl groups containing about 1-8 carbon atoms, aromatic groups containing about 6-20 carbon atoms, and hydrogen; and a second layer deposited on the first layer, the second layer comprising an organosilicon material which has been polymerized and oxidized in a plasma, the second layer containing silicon, oxygen, carbon, and hydrogen.

Claims

1. A multilayer article comprising:

a substrate;

a first layer comprising an ultraviolet radiation absorbing material, the ultraviolet radiation absorbing material comprising at least one polybenzoylresorcinol, and a partial condensate of a diorganodiorganooxysilane having the formula R₂Si(OR′

)₂ or an organotriorganooxysilane having the formula RSi(OR′

)₃, or both, where R is independently selected from the group consisting of alkyl groups containing about 1-3 carbon atoms, aromatic groups containing about 6-13 carbon atoms, vinyl radical, 3,3,3-trifluoropropyl radical, gamma-glycidoxypropyl radical and gamma-methacryloxypropyl radical, and R′

is independently selected from the group consisting of alkyl groups containing about 1-8 carbon atoms, aromatic groups containing about 6-20 carbon atoms, and hydrogen; and

a second layer comprising a plasma polymerized organosilicon, the second layer being deposited at a power level of 10⁶-10⁸ J/Kg in the presence of excess oxygen.

2. A multilayer article comprising:

a substrate;

a first layer comprising an ultraviolet radiation absorbing material, the ultraviolet radiation absorbing material comprising at least one polybenzoylresorcinol, and a partial condensate of a diorganodiorganooxyslane having the formula R₂Si(OR′

)₂ or an organotriorganooxysilane having the formula RSi(OR′

)₃, or both, where R is independently selected from the group consisting of alkyl groups containing about 1-3 carbon atoms, aromatic groups containing 6-13 carbon atoms, vinyl radical, 3,3,3-trifluoropropyl radical, gamma-glycidoxypropyl radical and Gardena-methacryloxypropyl radical, and R′

is independently selected from the group consisting of alkyl groups containing about 1-8 carbon atoms, aromatic groups containing about 6-20 carbon atoms, and hydrogen; and

a second layer comprising a plasma polymerized organosilicon;

wherein the article remains substantially free of microcracks after being exposed to 6875 kJ/m² of radiation in an ASTM G26 cycle in a xenon arc weatherometer.

3. A multilayer article comprising:

a substrate;

a fist layer comprising an ultraviolet radiation absorbing material, the ultraviolet radiation absorbing material comprising at least one polybenzoylresorcinol, and a partial condensate of a diorganodiorganooxysilane having the formula R2Si(OR′

)2 or an organoiorganooxysilane having the formula RSi(OR′

)3, or both, where R is independently selected from the group consisting of alkyl groups containing about 1-3 carbon atoms, aromatic groups containing about 6-13 carbon atoms, vinyl radical, 3,3,3-trifluoropropyl radical, gamma-glycidoxypropyl radical and gamma-methacryloxypropyl radical, and R′

is independently selected from the group consisting of alkyl groups containing about 1-8 carbon atoms, aromatic groups containing about 6-20 carbon atoms, and hydrogen; and

a second layer deposited on the first layer, the second layer comprising an organosilicon material which has been polymerized and oxidized in a plasma, the second layer containing silicon, oxygen, carbon, and hydrogen.

4. The article of claim 3, wherein the diorganodiorganooxysilaned or the organotriorganooxysliane comprise a silanol of the formula R₂Si(OH)₂ or RSi(OH)₃, respectively, in which R is selected from the group consisting of alkyl radicals of 1 to 3 carbon atoms, vinyl radical, 3,3,3-trifluoropropyl radical, gamma-glycidoxypropyl radical and gamma-metbacryloxypropyl radical.

5. The article of claim 4, wherein the first layer further comprises colloidal silica.

6. The article of claim 5, wherein the colloidal silica comprises particles having a diameter of 10-30 nanometers.

7. The article of claim 5, wherein at least 70 weight percent of the silanol comprises CH₃Si(OH)₃ and (CH₃)₂Si(OH)₂.

8. The article of claim 5, wherein the first layer comprises 10 to 70 weight percent of the colloidal silica and 30 to 90 weight percent of the partial condensate.

9. The article of claim 5, wherein the first layer is applied by at least one of:

flowing, spraying, dipping, brushing, roll coating, and curtain coating.

10. The article of claim 5, wherein the second layer is formed by plasma enhanced chemical vapor deposition of an organosilicon monomer.

11. The article of claim 10, wherein the organosilicon monomer comprises at least one of:

tetramethyldisiloxane, hexamethyldisiloxane, and octamethylcyclotetrasiloxane.

12. The article of claim 5, further comprising a primer layer between the substrate and the first layer.

13. The article of claim 12, wherein the primer layer comprises a thermoplastic acrylic.

14. The article of claim 12, wherein the primer layer comprises a thermoset acrylic.

15. The article of claim 12, wherein the primer layer includes an ultraviolet radiation absorbing material.

16. The article of claim 12, wherein the primer layer has a thickness of 0.2-2.0 microns.

17. The article of claim 12, wherein the primer layer has a thickness of 0.6-1.0 microns.

18. The article of claim 5, wherein the first layer has a thickness of 1-15 microns.

19. The article of claim 5, wherein the first layer has a thickness of 5-10 microns.

20. The article of claim 5, wherein the second layer has a thickness of 0.5-5.0 microns.

21. The article of claim 5, wherein the second layer has a thickness of 2.0-3.0 microns.

22. The article of claim 3, wherein the second layer comprises a plasma polymerized and oxidized organosilicon material having a the formula SiOxCyHz, where 0.5<

x<

2.4;

0.3<

y<

1.0; and

0.7<

z<

4.0.

23. The article of claim 3, wherein the second layer is applied by plasma enhanced chemical vapor deposition.

24. The article of claim 23, wherein the second layer is deposited at a power level of 10⁶-10⁸ J/Kg in the presence of excess oxygen.

25. The article of claim 23, wherein the article remains substantially free of microcracks after being exposed to 6875 kJ/m² of radiation in an ASTM G26 cycle in a xenon arc weatherometer.

26. A method of forcing a multilayer article comprising:

N applying a first layer to a substrated, the first layer comprising an ultraviolet radiation absorbing material, the ultraviolet radiation absorbing material comprising at least one polybenzoylresorcinol, and a partial condensate of a diorganodiorganooxysilane having the formula R2Si(OR′

)2 or an organotriorganooxysilane having the formula RSi(OR′

)3, or both, where R is independently selected from the group consisting of alkyl groups containing about 1-3 carbon atoms, aromatic groups containing about 6-13 carbon atoms, vinyl radical, 3,3,3-trifluoropropyl radical, gamma-glycidoxypropyl radical and gamma-methacryloxypropyl radical, and R′

is independently selected from the group consisting of alkyl groups containing about 1-S carbon atoms, aromatic groups containing about 6-20 carbon atoms, and hydrogen; and

applying a second layer on the first layer by plasma polymerizing an organosilicon material in excess oxygen.

27. The method of claim 26, wherein the organosilicon material is plasma polymerized at a power density of 10⁶-10⁸ J/Kg.

28. The method of claim 26, wherein the second layer is applied by plasma enhanced chemical vapor deposition.

29. The method of claim 26, wherein the second layer comprises a polymerized and oxidized organosilicon material having the formula SiOxCyHz, where 0.5<

x<

2.4;

0.3<

y<

1.0; and

0.7<

z<

4.0.

30. The method of claim 26, wherein the first layer further comprises colloidal silica.

31. The method of claim 26, wherein the first layer is applied by at least one of:

flowing, spraying, dipping, brushing, roll coating, and curtain coating.

32. The method of claim 26, further comprising the step of curing the first layer.

33. The method of claim 26, wherein the article remains substantially free of microcracks after being exposed to 6875 kJ/m² of radiation in an ASTM G26 cycle in a xenon arc weatherometer.

34. The method of claim 26, further comprising the step of applying a primer layer between the substrate and the first layer.

35. The method of claim 34, wherein the primer layer comprises a thermoplastic acrylic material.

36. The method of claim 34, wherein the primer layer comprises a thermoset acrylic material.