Trends in Plastics Coatings
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`2. Primers and tie-coats
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`3. Adhesion promoters
`a. covalent bonding
`1). chemical similarity
`c. other forces of attraction — hydrogen bonding, electrostatic, van der Waals
`4. Corona and plasma treatment
`5. Surface roughening
`
`A. Solvent and co-solvent composition of the coating fluid:
`Plastics of low surface energy present difficult surfaces for coating adhesion. Also, as discussed above, plastics
`may have a polymer conformation that is not conducive to good coating adhesion. To accommodate these types
`of plastics, one approach to promoting adhesion is through careful formulation of the coating composition. In
`doing so, significant emphasis should be given to the balance of solvents and/or cosolvents used in the
`formulation. Consideration of the demands of environmental regulations, to reduce volatile organic compound
`(V. O. C.) usage, presents a significant challenge to the forrnulator.
`
`The primary action that must take place is to relax or partially solubilize the surface polymer molecules, thus.
`providing the potential for coating polymer or binder resin to penetrate the plastic surface and form an
`interpolymer entanglement. Temperature will also improve this action, especially if the temperature can be
`elevated to a point well above the Tg of the plastic without detrimental effects on the plastic or coating
`composition. This solvent/temperature action will result in exceptional adhesion of the coating.
`
`In practice, the formulator must consider the solubility parameters of the solvent used in the coating composition
`and both the coating polymer or binder resin and the plastic or poiymer substrate. Solubility parameter theory3
`provides numeric three dimensional coordinates for solvents according to Equation 4.
`
`502 = 5,12 + 5P2 + 5h2
`
`Eq. 4
`
`Where:
`
`50 = Solubiiity parameter
`
`5d = Component due to dispersive forces
`
`8p = Component due to polar forces
`5,, = Component due to hydrogen bonding
`
`It is, however, common practice to use only a two dimensional approach to permit easy plotting of parameter
`coordinates according to standard X-Y graphing. The most frequently used parameters used in such plots are the
`polar (Sp) and the hydrogen bonding (Sh) according to the Hanson solubility parameter theory3. A solvent will
`be located at a specific point according to its parameter value, but polymers will have a range of solubility and
`will cover an area within a plot of 8p vs. 831. The center of the polymer solubility area may be designated the
`solubility parameter average and may be used to determine those solvents that are most likely to exhibit high
`potential for dissolution of the polymer based on proximity to the polymers’ average value.
`
`Also it is important to recognize that binary, tertiary, etc. mixtures or blends of solvents will exhibit a summed
`solubility parameter value based on the weight fraction of each solvent in the mixture according to Equation 5.
`H
`H
`Fl
`
`5
`
`0 mixture
`
`31 ZW, 5diEi+ Zwiajl + Zw,8h,2
`
`Eq. 5
`
`Where:
`
`Declaration of Robert A. Iezzi, Ph.D.
`(cid:39)(cid:72)(cid:70)(cid:79)(cid:68)(cid:85)(cid:68)(cid:87)(cid:76)(cid:82)(cid:81)(cid:3)(cid:82)(cid:73)(cid:3)(cid:53)(cid:82)(cid:69)(cid:72)(cid:85)(cid:87)(cid:3)(cid:36)(cid:17)(cid:3)(cid:44)(cid:72)(cid:93)(cid:93)(cid:76)(cid:15)(cid:3)(cid:51)(cid:75)(cid:17)(cid:39)(cid:17)(cid:3)
`AppEND|X K_9
`(cid:36)(cid:51)(cid:51)(cid:40)(cid:49)(cid:39)(cid:44)(cid:59)(cid:3)(cid:46)(cid:16)(cid:28)
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`http://www.vtcoatings.com/plasticshtrn
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`Wavelock
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`Exhibit 1017
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`Trends in Plastics Coatings
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`And:
`
`W, = Weight fraction of solvent i
`
`Cdi = Component due to dispersive forces of solvent i
`
`8pi = Component due to polar forces of solvent i
`5m = Component due to hydrogen bonding of solvent 1
`
`i’)
`
`5
`
`p mixture
`I1
`
`=ZWfiw
`
`8
`
`fl—Zw@m
`h mixture _—
`
`will provide the parameters for two dimensional plotting of the solvent mixture or blend. Furthermore, as the
`solvent mixture of the coating composition begins to evaporate during drying and cure, the parameter values will
`shift in the direction of the solvent(s) having the lowest rate of evaporation. This leads to a very important
`realization. The solvent having the lowest rate of evaporation (the last one out of the coating during drying)
`should be a very good solvent for the coating polymer or binder resin and for the polymer constituting that of the
`plastic substrate. This will promote the best conditions for coating adhesion.
`
`One last concept in the use of solvents is the fact that, as solvent evaporation progresses during drying, the surface
`tension of the coating or fluid layer may drift and present problems with uniformity and adhesion. Consideration
`of the surface tension of the solvent of lowest rate of evaporation is also important to maintain the optimum
`coating performance.
`
`B. Primers and Tie—Coats:
`There are many times where the coating chemistry desired will never be compatible with the plastic surface, even
`in consideration of the solvents used. Under these circumstances, primers or tie—coats serve to act as an
`intermediate layer for adhesion purposes. The basic premise is to apply a coating to the plastic surface that
`exhibits good adhesion and will also act as a compatible intermediate surface for the final topcoat composition.
`
`It is often seen that primers and tie«coats can be specific for the type of topcoat composition to be applied to a
`particular plastic. “Universal” primers have been claimed with some materials but caution is warranted when
`examining them for any application.
`
`Primers may be clear or filled to provide added surface area or roughness for maximum adhesion. Tie—coats are
`typically ciear and may simply be an adhesion promoting agent solubilized or dispersed in low concentration in a
`particular solvent or water. These will be addressed in the next section.
`
`C. Adhesion Promoters:
`Adhesion promoters may be added to either the primer, tie-coat, or coating compositions and are primarily of
`three main types, those that bond covalently, those that bond by other forces of attraction, and those that promote
`adhesion by chemical similarity (“like—sticks to-like”). In all instances, these types of adhesion promoters use the
`described mode of adhesion to the plastic substrate. They all, additionally, possess specific functional groups that
`are presented to the coating for subsequent bonding or binding of that layer. In application, it is typical to use a
`very low concentration of an adhesion promoter, thus, providing a near mono—mo1ecular layer over the surface of
`the plastic. Effectiveness may decrease with greater applied thickness of the adhesion promoter. It is, therefore,
`essential to fully discuss and/or review the performance mechanism of the adhesion promoter through respective
`vendor communications.
`
`In the use of adhesion promoters, the adhesion promoter must look for chemical functionality in the plastic to
`bond or bind to. With thermoset surfaces, the best performance of an adhesion promoter will be when there is a
`fair level of residual functionality remaining and available for binding. Polymers of low or no residual
`Declaration of Robert A. Iezzi, Ph.D.
`(cid:39)(cid:72)(cid:70)(cid:79)(cid:68)(cid:85)(cid:68)(cid:87)(cid:76)(cid:82)(cid:81)(cid:3)(cid:82)(cid:73)(cid:3)(cid:53)(cid:82)(cid:69)(cid:72)(cid:85)(cid:87)(cid:3)(cid:36)(cid:17)(cid:3)(cid:44)(cid:72)(cid:93)(cid:93)(cid:76)(cid:15)(cid:3)(cid:51)(cid:75)(cid:17)(cid:39)(cid:17)(cid:3)
`APPEND|x K-1o
`(cid:36)(cid:51)(cid:51)(cid:40)(cid:49)(cid:39)(cid:44)(cid:59)(cid:3)(cid:46)(cid:16)(cid:20)(cid:19)
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`http://wwwvtcoatings.com/plasticshtm
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`Exhibit 1017
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`Trends in Plastics Coatings
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`functionality will remain more problematic to promote adhesion, but nonetheless, there are some options
`available.
`
`A very popular class of adhesion promoters are silanes and several are available for specific combinations of
`plastics and coatings. For these types of adhesion promoters to find such functionality certain conditions must be
`met4. First, the plastic must have appropriate functional groups-. Second, the adhesion promoter must be mobile
`enough in the primer or coating composition for the time necessary to migrate to and find the appropriate
`functionality on the surface of the plastic. This implies careful formulation of the solvent balance of the coating
`composition and an appropriate surface activity in the adhesion promoter itself. Third, there should be minimal
`competition between the plastic functionality and the coating polymer or binder resin so that the effectiveness of
`the adhesion promoter is not diminished. Fourth, the adhesion promoter must be soluble in the coating
`composition and miscible with the polymer of the plastic.
`
`Of the types of plastics available, polyolefins and other hydrocarbon thermoplastics are difficult substrates for
`coating adhesion. When dealing with these substrates, polychlorinated polyolefin adhesion promoters5 have been
`used to bind the coating to the plastic surface by their chemical similarity. Additionally, being relatively
`hydrophobic, they tend to migrate to the coating/substrate interface and orient themselves with their pendant
`maleic anhydride and/or halogen groups toward the coating layer.
`
`D. Corona and Plasma Treatment;
`Corona and plasma treatment of plastic surfaces causes a change in the chemical nature of the surface through
`possible oxidation or possible microstructure formation so that subsequent coating adhesion is made maximum.
`These treatments are quite effective for a number of types of plastics and work well for most types of Coatings.
`particular, this form of treatment works remarkably well for polyester, polyolefin, and other hydrocarbon
`thermoplastics.
`
`In
`
`Corona discharge is made possible by high voltage across a gap through which the plastic substrate is passed.
`Current passes from an electrode to a grounded hardened steel support surface for the plastic. This hardened steel
`support may be ceramic coated for longer use. Plasma discharge is, in simple terms, a high temperature flame
`impinging on the surface of the plastic for a very short period of time. The effectiveness is not necessarily
`permanent and it is best to apply the desired coating shortly after treatment.
`
`E. Surface Roughening:
`As introduced earlier, rough surfaces are easier to coat and to adhere to. Although, the surface tension of the base
`plastic material does not change, microscopically the surface has varied angles causing the net contact angle that
`the coating makes appear exceptionally low. The increase in surface area coated also contributes to adhesion.
`When this option is acceptable in the overall process of producing the plastic article, it is advised to take
`advantage of it, especially in combination with other forms of adhesion promotion.
`
`Summary
`By no means are the concepts introduced above all inclusive for what the formulator needs to know about plastic
`surfaces for successful coating design. There are numerous other concepts and principles that interplay with the
`science of coating design for plastics. Obstacles always seem to occur, some of which may be insurmountable. If
`the coating cannot be modified to comply with requirements, perhaps the type of plastic can.
`It is always helpful
`to combine a coating formulators skill with that of a polymer or plastic engineer to design the best possible end
`product. The plastic coating formulator must always realize that the product is never a fluid composition but
`always an article composed of a coated plastic. The coating and the substrate must function synergisticly as a unit
`to satisfy the requirements of the final consumer.
`
`References
`
`1.. J. Brandrup, E. H. Immergut, Polymer Handbook, 3rd Ed., V1/411-426 (1989) John Wiley & Sons, inc.
`2. M. J. Rosen, Surfactants and lnterfacial Phenomenon, 2nd Ed., 240-255 (1989) John Wiley & Sons, Inc.
`3. C. M. Hanson, J. Paint Tech. 39 (505), 104-117, (1967).
`4. A Guide to Dow Corning Silane Coupling Agents, Dow Corning Corporation, Midland, MI (1990).
`5. Chlorinated Polyolefins, Eastman Chemical Company, Kingsport, TN (1995).
`
`Declaration of Robert A. Iezzi, Ph.D.
`(cid:39)(cid:72)(cid:70)(cid:79)(cid:68)(cid:85)(cid:68)(cid:87)(cid:76)(cid:82)(cid:81)(cid:3)(cid:82)(cid:73)(cid:3)(cid:53)(cid:82)(cid:69)(cid:72)(cid:85)(cid:87)(cid:3)(cid:36)(cid:17)(cid:3)(cid:44)(cid:72)(cid:93)(cid:93)(cid:76)(cid:15)(cid:3)(cid:51)(cid:75)(cid:17)(cid:39)(cid:17)(cid:3)
`APPENDIX K-11
`(cid:36)(cid:51)(cid:51)(cid:40)(cid:49)(cid:39)(cid:44)(cid:59)(cid:3)(cid:46)(cid:16)(cid:20)(cid:20)
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`http://WWW.vtcoatingscorn/plastics.htm
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`Exhibit1017
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`Trends in Plastics Coatings
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`Page 12 of 12
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`About the Author
`
`Lawrence C. Van Iseghem is the president and founder of Van Technologies, Inc. Van Technologies designs,
`formulates, and manufactures specialty industrial coatings with emphasis on environmentally compliant
`technology.
`
`Declaration of Robert A. Iezzi, Ph.D.
`(cid:39)(cid:72)(cid:70)(cid:79)(cid:68)(cid:85)(cid:68)(cid:87)(cid:76)(cid:82)(cid:81)(cid:3)(cid:82)(cid:73)(cid:3)(cid:53)(cid:82)(cid:69)(cid:72)(cid:85)(cid:87)(cid:3)(cid:36)(cid:17)(cid:3)(cid:44)(cid:72)(cid:93)(cid:93)(cid:76)(cid:15)(cid:3)(cid:51)(cid:75)(cid:17)(cid:39)(cid:17)(cid:3)
`APPENDIX K-12
`(cid:36)(cid:51)(cid:51)(cid:40)(cid:49)(cid:39)(cid:44)(cid:59)(cid:3)(cid:46)(cid:16)(cid:20)(cid:21)
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`http://wwwvtcoatings.com/plastics.htm
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`|ngeoT"" Film Surface Treatment
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`G‘) Natur‘e\/\/Or‘|<s LLC
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`Figure 4.
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`Figure 5 shows untreated lngeo film does require more watt density to effectively increase the surface energy when compared
`to “bump” treatment, but not an unreasonable amount of watt density is required to be effective.
`Declaration of Robert A. lezzi, Ph.D.
`(cid:39)(cid:72)(cid:70)(cid:79)(cid:68)(cid:85)(cid:68)(cid:87)(cid:76)(cid:82)(cid:81)(cid:3)(cid:82)(cid:73)(cid:3)(cid:53)(cid:82)(cid:69)(cid:72)(cid:85)(cid:87)(cid:3)(cid:36)(cid:17)(cid:3)(cid:44)(cid:72)(cid:93)(cid:93)(cid:76)(cid:15)(cid:3)(cid:51)(cid:75)(cid:17)(cid:39)(cid:17)(cid:3)
`APPENDIX L-4
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`NatureWorks, lngeo and the lngeo logo are trademarks or registered trademarks in the USA and other countries.
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`Exhibit 1017
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`Page 173
`Page 4 of 5
`NWFS017_020111
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`FOR
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`Declaration of Robert A. Iezzi, Ph.D.
`(cid:39)(cid:72)(cid:70)(cid:79)(cid:68)(cid:85)(cid:68)(cid:87)(cid:76)(cid:82)(cid:81)(cid:3)(cid:82)(cid:73)(cid:3)(cid:53)(cid:82)(cid:69)(cid:72)(cid:85)(cid:87)(cid:3)(cid:36)(cid:17)(cid:3)(cid:44)(cid:72)(cid:93)(cid:93)(cid:76)(cid:15)(cid:3)(cid:51)(cid:75)(cid:17)(cid:39)(cid:17)(cid:3)
`APPENDIX M-1
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`Wavelock
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`Exhibit 1017
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`Page 175
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`C‘0p_\'tigltt
`
`I9‘)? ht‘ iohn Wiley 6°: Sons Ltd.
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`Library of Cangress Catalagittg-in-Publication Dam
`Modern fittoropolymcrs : high performance pOi_\“IT]6l'b for diverse
`applieiittons I edited by John Scheirs.
`p.
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`include»: bibliographical references and indexes.
`ISBN (J-47t~97t_l55~7 (itllvt. paper)
`1.
`i)01}l'Ilt3]'S.
`2. Orgitnofittorine Compounds.
`TA~i55.P5b’i\-I54
`1997
`53U.l")2 — dcll
`
`I. Scheirs. John.
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`9t:-49974
`Cl?
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`Brt'fi'sh Library’ C‘ata.t'oguz'tzg in Pttblication Data
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`ISBN tl—-—i»7l—97tl55 7
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