11332939 (B.P.A.I. Dec. 7, 2009)

Ex Parte Botros

Board of Patent Appeals and InterferencesDec 7, 2009

11332939 (B.P.A.I. Dec. 7, 2009)

UNITED STATES PATENT AND TRADEMARK OFFICE ____________________ BEFORE THE BOARD OF PATENT APPEALS AND INTERFERENCES ____________________ Ex parte MAGED G. BOTROS ____________________ Appeal 2009-013212 Application 11/332,939 U.S. Patent Publication 2007/0167596 Technology Center 1700 ____________________ Decided: December 7, 2009 Before FRED E. McKELVEY, Senior Administrative Patent Judge, and RICHARD E. SCHAFER and JAMESON LEE, Administrative Patent Judges. McKELVEY, Senior Administrative Patent Judge. DECISION ON APPEAL A. Statement of the case 1 Equistar Chemicals, L.P. [hereinafter Equistar], the real party in 2 interest, seeks review under 35 U.S.C. Â§ 134(a) of a final rejection (mailed 3 10 April 2008). 4 The application was filed on 17 January 2006. 5 Claims 1-18 are on appeal. 6 The following prior art was cited by the Examiner: 7 Appeal 2009-013212 Application 11/332,939 2 Hattori U.S. Patent 5,591,792 7 Jan. 1997 Lee U.S. Patent 6,184,298 6 Feb. 2001 1 Equistar cites and discusses the following reference: 2 Goto U.S. Patent 5,709,953 20 Jan. 1998 3 We refer to the following reference: 4 Lindquist U.S. Patent 5,916,959 29 Jun. 1999 5 Hattori, Lee, Goto, and Lindquist are prior art under 35 U.S.C. 6 Â§ 102(b). 7 We have jurisdiction under 35 U.S.C. Â§ 134(a). 8 B. Findings of fact 9 The following findings of fact are supported by at least a 10 preponderance of the evidence. 11 References to the specification are to U.S. Patent Publication 12 2007/0167569 (19 July 2007). 13 Additional findings as necessary may appear in the Discussion portion 14 of the opinion. 15 Claims on appeal 16 Claims 1-18 are on appeal. 17 With respect to a rejection of claim 1-11 over Lee, Equistar does not 18 argue the separate patentability of claims 2-11. 19 With respect to a rejection of claims 1-18 over Hattori, Equistar does 20 not argue the separate patentability of claims 2-18. 21 Appeal 2009-013212 Application 11/332,939 3 Accordingly, we will decide the appeal on the basis of claim 1. 1 37 C.F.R. Â§ 41.37(c)(1)(vii) (2009). 2 Claim 1, which we reproduce from the Claim Appendix of the 3 Amended Appeal Brief filed 31 October 2008, reads [bracketed matter, 4 italics, and some indentation added]: 5 An adhesive composition consisting essentially of: 6 (a) 35 to 75 wt.%, based on the total weight of the [adhesive] 7 composition, ethylene-butene-1 linear low density copolymer 8 having 9 [1] a density from 0.912 to 0.925 g/cm3 and 10 [2] melt index from 0.5 to 15 g/10 min; 11 (b) 15 to 45 wt.%, based on the total weight [of the adhesive 12 composition], styrene-isoprene-styrene triblock copolymer 13 having 14 [1] a styrene content greater than 35 wt%, 15 [2] melt flow rate greater than 25 g/10 min and 16 [3] containing less that 1 wt.% diblock; and 17 (c) 1 to 25 wt.%, based on the total weight [of the adhesive 18 composition], [of a polymer selected from] 19 [1] ethylene homopolymer or 20 [2] ethylene C4-8 Î±-olefin copolymer, 21 grafted with 0.5 to 5 wt.% of maleic anhydride. 22 Relevant to this appeal, there are several kinds of polymers. See 23 generally, Malcolm P. Stevens, Polymer Chemistry, 7-8, 3d ed., Oxford 24 University Press, 1999 (ISBN 0-19-512444-8). 25 Appeal 2009-013212 Application 11/332,939 4 A homopolymer is one made from a single monomer, e.g., where the 1 monomer is A: 2 AAAAAAAA. 3 A random copolymer is one made from two monomer having a 4 random structure. If the two monomers are A and B, the copolymer 5 structure will be a random mixture of A and B, e.g.: 6 AABABBAABABA. 7 A block copolymer is one having groups of consecutive monomers 8 followed by consecutive groups of a different monomer, e.g., 9 AAAAABBBBB or AAAAABBBBBAAAAA. 10 as well as other possible blocks of consecutive monomers. 11 A triblock copolymer is a block copolymer having three groups of 12 consecutive monomers, e.g., where the two monomers are A and B: 13 AAAAABBBBBAAAAA. 14 A diblock copolymer is a block copolymer having two groups of 15 consecutive monomers, e.g.: 16 AAAAABBBBB. 17 A graft copolymers is one where a second monomer is grafted onto a 18 backbone of a first monomer, e.g., 19 AAAAAAAAA 20 â”‚ 21 BBBBBB. 22 23 The phrase "low density" in (a) would appear to be redundant given 24 that specific densities are recited in (a)[1]. 25 Appeal 2009-013212 Application 11/332,939 5 The claim transition phrase consisting essentially of has a well-1 defined meaning in patent law: in a composition claim the presence of 2 consisting essentially of leaves the scope of the claim open only to the 3 inclusion of unspecified ingredients which do not materially affect the basic 4 and novel characteristics of the composition. In re Janakirama-Rao, 5 50 CCPA 1312, 1314, 317 F.2d 951, 952 (CCPA 1963), citing Ex parte 6 Davis, 80 USPQ 448, 450 (Bd. App. 1948). 7 The Equistar invention 8 (1) General nature of the Equistar's invention 9 Equistar's invention relates to "tie-layer" adhesive blend compositions 10 and their use for coextruded multi-layer films and sheets having one or more 11 styrene polymer layers. Specification, Â¶ 0002. 12 The adhesive blend compositions are said to be an improvement over 13 prior art compositions. Specification, Â¶ 0002. 14 (2) Background prior art 15 Multi-layer films and sheets are widely used for food packaging 16 applications. Specification, Â¶ 0004. 17 According to Equistar, depending on the intended end-use application, 18 the number and arrangement of resin layers and the type of resins employed 19 will vary. Specification, Â¶ 0004. 20 For example, polyethylene (PE) resins are often included as one of the 21 layers for their food contact and sealing properties. Ethylene-vinyl alcohol 22 (EVOH) copolymers and polyamides (nylons) are widely used as oxygen 23 and flavor barrier layers. Styrene polymers are commonly included as 24 structural layers. Styrene polymers which contain rubber, such as high 25 Appeal 2009-013212 Application 11/332,939 6 impact polystyrene (HIPS), are said to be especially useful for this purpose 1 [i.e., as structural layers]. Specification, Â¶ 0005. 2 According to Equistar, a continuing problem said to exist within the 3 industry is how to adhere the dissimilar resin layers within such multi-layer 4 constructions. Specification, Â¶ 0006. 5 While numerous tie-layer adhesive compositions containing modified, 6 i.e., functionalized, polyolefins are known to effectively adhere to polyolefin 7 and barrier resins, adhesion to styrene resins is said to be problematic. 8 Specification, Â¶ 0006. 9 Equistar tells us that it would be highly advantageous if adhesive 10 blends which provided superior adhesion to styrene polymers without 11 sacrificing adhesion to other polymer types employed in multi-layer 12 constructions were available. Specification, Â¶ 0007. 13 Various prior art adhesives are described in the Equistar specification. 14 One prior art example of a tie-layer is said to be described by Goto, 15 U.S. Patent 5,709,953. Specification, Â¶ 0012. 16 Equistar characterizes the Goto invention as follows (Specification, 17 Â¶Â¶ 0012-0013): 18 [Goto] . . . discloses adhesive compositions comprised of 19 35-65 weight percent (wt. %) ethylene polymer fraction and 20 35-65 wt. % styrene/aliphatic/styrene triblock elastomer 21 fraction. [Goto] . . . . discloses that all or a portion of the 22 ethylene polymer fraction can be grafted with an unsaturated 23 carboxylic acid or anhydride. For one embodiment where an 24 ethylene polymer fraction having relative low density is 25 Appeal 2009-013212 Application 11/332,939 7 desired, the reference suggests mixing a relatively small amount 1 of high density polyethylene (HDPE) grafted with a significant 2 amount of maleic anhydride (MAH) and a relatively large 3 amount of LLDPE [linear low density polyethylene]. 4 While [Goto] . . . generally discloses adhesive blends for 5 styrene polymers comprised of ethylene polymers, styrene 6 triblock elastomers and maleic anhydride grafts, styrene-7 butadiene-styrene (SBS) triblock elastomers are indicated to be 8 preferred. [According to Equistar,] [i]nconsistent results [are 9 said to] have been observed with adhesive blends of the types 10 disclosed . . . [Goto] formulated using styrene-isoprene-styrene 11 (SIS) triblock polymers, particularly when the ethylene polymer 12 is LLDPE. 13 (3) Goto 14 The Goto invention is directed to extrudable adhesives and 15 particularly to extrudable adhesives for bonding a layer of a polystyrene 16 resin to a layer of a second resin. Col. 1:4-6. 17 Many food packaging applications utilize a container formed from a 18 multi-layer, extruded laminate. One typical type of single-service, 19 shelf-stable container is formed of an extruded laminate of 20 polystyrene/adhesive/ethylene vinyl alcohol (EVOH)/adhesive/polyethylene. 21 The polystyrene is desirable as an outer layer in that it is very heat-formable, 22 being formable in a non-molten state at a temperature above a glass 23 transition temperature. Polyethylene is a desirable inner layer in that it is 24 Appeal 2009-013212 Application 11/332,939 8 inert, has desirable organoleptics (taste/odor properties) and often serves as 1 an effective heat-seal layer. EVOH (saponified ethylene vinyl acetate) as an 2 intermediate layer is known for its excellent gas barrier properties. 3 Furthermore EVOH acts as a chemical barrier, inhibiting the flow of 4 chemicals, such as polystyrene-plasticizing oils, from the contained food to 5 the polystyrene layer. Col. 1:9-24. 6 The Goto invention relates to an extrudable adhesive composition for 7 bonding polystyrene resin to a second resin such as EVOH and 8 polyethylene. Col. 1:53-57. 9 The extrudable adhesive comprises an A) polymer and a B) polymer. 10 The A) polymer is an ethylene polymer. 11 The adhesive has an ethylene polymer fraction at between about 35 12 and about 65 wt percent relative to the total of A) plus B). Col. 1:58-60. 13 The ethylene polymer fraction comprises an ethylene polymer or 14 copolymer, the ethylene polymer fraction A) being formed, in total, of at 15 least about 65 weight percent ethylene monomers, balance, other 16 copolymerizable monomers. Col. 1:60-67. 17 If the resin layer to which the polystyrene layer is to be bonded is 18 substantially non-polar, such as polyethylene, the ethylene polymer fraction 19 A) may contain no polar graft moieties. However, if the second resin layer 20 to which the polystyrene layer is to be bonded contains oxygen, e.g., 21 ethylene vinyl alcohol (EVOH), the ethylene polymer fraction comprises 22 between about 0.1 and 100 wt % of graft ethylene polymer having grafted 23 thereto an unsaturated carboxylic acid or anhydride, balance (if any) an 24 unmodified ethylene polymer, such that the ethylene polymer fraction A) 25 Appeal 2009-013212 Application 11/332,939 9 comprises, in total, between about 0.01 and about 5 wt %, graft monomers 1 having carboxylic acid or carboxylic acid anhydride functionality. 2 Col. 2:1-14. 3 The extrudable adhesive also comprises B) between about 35 and 4 about 65 wt %, relative to total of A) plus B), of a styrene/aliphatic/styrene 5 triblock elastomer, between about 20 and about 60 wt % of the triblock 6 elastomer B) comprising styrene monomers. Col. 2:14-18. 7 According to Goto, in order to provide good adhesion to polystyrene, 8 MI2(SB)2 /MI2(PE) should be about 1.0 or above, preferably about 9 4.0 or above. Col. 2:18-21. MI is melt index. 10 Goto believes that the relation between the melt indices 11 promotes co-continuous phases of the ethylene polymer fraction A) and the 12 styrene/aliphatic/styrene triblock elastomer B) of the extrudable adhesive 13 composition, whereby there is substantial molecular contact of the elastomer 14 B) with the polystyrene resin layer and substantial molecular contact of the 15 ethylene polymer fraction A) with the second resin layer to which the 16 polystyrene layer is adhered. Col. 2:21-29. 17 The triblock elastomer is formed of sufficient styrene content and 18 utilized in sufficient amount so that the styrene blocks promote excellent 19 adhesion to polystyrene. Thus, says Goto, the styrene/aliphatic/styrene 20 triblock elastomer is formed from between about 20 and about 60 wt % 21 styrene monomers (i.e. has a styrene monomer content of between about 20 22 and about 60 wt %), balance aliphatic monomers, and the triblock elastomer 23 B) comprises between about 35 and about 65 wt % of the total of 24 polyethylene fraction A) plus triblock elastomer B). The aliphatic middle 25 Appeal 2009-013212 Application 11/332,939 10 block of the triblock elastomer may be unsaturated, such as a polybutadiene 1 block or a polyisoprene block, polybutadiene being the currently preferred 2 middle block. Also, the middle block may be saturated, e.g., 3 styrene/ethylene-butene/styrene rubber, or only partially unsaturated, such as 4 may be provided by hydrogenation or partial hydrogenation of an 5 unsaturated middle block. Col. 2:63 through col. 3:12. 6 Contrary to Equistar's statement in Â¶ 0006 of the Specification, the 7 adhesive compositions of the Goto invention are said to adhere well to any 8 polystyrene resin composition. Col. 2:39-40. 9 Data in Goto Table 1 (col. 5:22-35) and Table 2 (col. 5: 42-56) 10 support Goto's findings. 11 According to Goto, Examples 1A to 4B show that a MI2SB/MIPE 12 greater than 1.0 is necessary for good adhesion to PS (preferably greater than 13 3.0). Col. 5:33-35. 14 Further according to Goto, examples of 5-10 show that the range of 15 SB for good adhesion to both EVOH and PS is 35-65% SB (optimum being 16 said to be about 40%). Col. 5:54-56. 17 (4) Specific need said to exist 18 According to Equistar, "[t]here is a continuing need for adhesive 19 compositions which provide improved adhesion to styrene polymer layers in 20 coextruded multi-layer films and sheets comprised of one or more styrenic 21 layers." Specification, Â¶ 0014. 22 Further according to Equistar, "[i]t would be even more advantageous 23 if adhesive blends derived from LLDPE and SIS which provided superior 24 adhesion to styrenic polymers were available." Specification, Â¶ 0014. 25 Appeal 2009-013212 Application 11/332,939 11 (5) Equistar's solution to supposed need 1 The need and advantage are said to be realized with the adhesive 2 blends of the Equistar invention which utilize specific LLDPE and SIS 3 components in combination with a functionalized ethylene polymer to 4 supposedly achieve unexpectedly high adhesion. Specification, Â¶ 0014. 5 To support its position with respect to advantageous results said to be 6 achieved with the Equistar invention, Equistar relies on Examples 1-8. 7 Specification, Â¶Â¶ 0043 through 0052. 8 According to the examples, tie-layer adhesive blend compositions 9 prepared and utilized in the examples were pelletized prior to use by dry 10 blending all of the components and then melt blending the mixture in a 11 Warner-Pfleiderer ZSK-30 twin screw extruder equipped with a multi-hole 12 (1/8 inch diameter) die connected to a strand cutter. The extruder screw 13 speed was 250 rpm. Temperatures in the extruder ranged from 180 ÂºC to 14 200 ÂºC. The melt temperature at the extruder die was 209 ÂºC. Specification, 15 Â¶ 0040. 16 To evaluate adhesion of the tie-layer compositions, 24 mil multi-layer 17 cast sheets were prepared by coextrusion. The five-layer coextruded sheets 18 had an A/B/C/B/A layer structure where B represents the tie-layer 19 composition, C represents EVOH and A represents polystyrene layers. 20 Specification, Â¶ 0041. 21 Appeal 2009-013212 Application 11/332,939 12 Graphically, the 5-layer sheet is illustrated below. 1 Layer A = polystyrene Layer B = tie-layer (adhesive of the invention) Layer C = EVOH Layer B = tie-layer (adhesive of the invention) Layer A = polystyrene 2 Depicted is a 5-layer extruded sheet 3 The sheets were produced on a Killion laboratory scale film line using 4 three 1 inch extruders in an A/B/C/B/A feedblock configuration. Sheets 5 were extruded using a 10 inch flat die to produce continuous 8 inch wide 6 samples. Specification, Â¶ 0042. The Killion laboratory scale film extruder 7 is not otherwise described, but we assume it is a commercial product. 8 Adhesion values reported in the examples were determined in 9 accordance with ASTM D 1876-93. Adhesion values are reported for both 10 tie-layer/styrene interfaces since it was observed that, for the 24 mil cast 11 sheet prepared in this manner, adhesion on the side which contacted the chill 12 roll was consistently higher than adhesion on the side which did not contact 13 the chill roll. An average value is also reported. EVOH/tie-layer adhesion 14 was determined after separation and removal of the styrene polymer layers. 15 According to Equistar, separation at only one EVOH/tie-layer interface was 16 possible due to the thinness of the remaining structure. Specification, 17 Â¶ 0042. 18 Appeal 2009-013212 Application 11/332,939 13 Set out below is data based on Example 1 (representing the invention) 1 and Examples 2 and 3 (not representing the invention because an 2 ethylene/hexane-1 copolymer was used in place of an ethylene/butene-1 3 copolymer). 4 5 Example 1 2 3 Invention Comparison Comparison Polymer (a) 59.83% 59.83% 59.83% Ethylene- butene-1 Ethylene- hexene-1 Ethylene- hexene-1 Density 0.918 0.918 0.918 Melt index (g/10 min) 2 7 2 Polymer (b) 30% 30% 30% S-I-S S-I-S S-I-S % styrene 44 44 44 Melt index (g/10 min) 40 40 40 % diblock <1 <1 <1 Polymer (c) (graft) 10% 10% 10% HDPE + MA HDPE + MA HDPE + MA % MA 1.9% 1.9% 1.9% Other ingredients 0.17% 0.17% 0.17% Adhesion strength (lbs/in) Near chill roll 3.48 0.23 0.95 Away chill roll 1.95 0.4 0.25 Average 2.17 0.31 0.6 Appeal 2009-013212 Application 11/332,939 14 1 See generally Table 1 in Â¶ 0047. 2 S-I-S means styrene-isoprene-styrene triblock polymer. 3 HDPE means high density polyethylene. 4 MA means maleic anhydride. 5 We do not know what weight to give "average" adhesion strength 6 because the specification fails to reveal its significance. 7 Nor do we know what weight to give "near chill roll" versus "away 8 chill roll" since the specification fails to reveal the significance of one versus 9 the other. 10 Equistar maintains that the data shows an improvement using an 11 ethylene/butene-1 polymer (a) versus an ethylene/hexane-1 polymer (a) 12 (Specification Â¶ 0048): 13 It is apparent from the data provided in Table 1 that adhesion 14 obtained at the styrene polymer/tie-layer interface with the 15 adhesive compositions of the invention which utilize an 16 ethylene-butene-1 LLDPE resin with a SIS copolymer and 17 MAH graft component are significantly higher than that of 18 either of the comparative formulations which have an ethylene-19 hexene-1 LLDPE copolymer as the base resin. Furthermore, it 20 should be mentioned that the remarkable improvement in 21 adhesion at the styrenic polymer/tie-layer interface was 22 accomplished without sacrificing adhesion at the barrier 23 resin/tie-layer interface. Adhesion values obtained at the 24 barrier resin/tie-layer interface using the adhesive blends of 25 Appeal 2009-013212 Application 11/332,939 15 Example 1, Comparative Example 2 and Comparative Example 1 3 all ranged from about 0.8 to 1 lbs/in. 2 Set out below is data based on Example 4 (invention) and comparative 3 Examples 5 and 6 (not invention because an ethylene/hexene-1 copolymer is 4 used in place of an ethylene/butene-1 copolymer). 5 Example 4 differs from Example 1 in that the Example 4 composition 6 also contains a "commercially available ethylene-propylene-diene rubber" 7 comprising 60 wt. % ethylene, 0.5 wt. % ethylidenenorbornene, and 8 presumably the remainder propylene. 9 Appeal 2009-013212 Application 11/332,939 16 1 Example 4 5 6 Invention Comparative Comparative Polymer (a) (random) 49.83% 49.83% 49.83% Ethylene-butene-1 Ethylene-hexene-1 Ethylene-hexene-1 Density (g/cm3) 0.918 0.918 0.918 Melt (g/10 min) 2 7 2 Polymer (b) (block) 30% 30% 30% S-I-S S-I-S S-I-S % styrene 44 44 44 Melt index (g/10 min) 40 40 40 % diblock <1 <1 <1 Polymer (c) (graft) 10% 10% 10% HDPE + MA HDPE + MA HDPE + MA % MA 1.9% 1.9% 1.9% Polymer (d) (optional) 10% 10% 10% Viscosity (Mooney) 20 20 20 Ethylene % 60 60 60 Propylene 39.5 39.5 39.5 Ethylnidene- orborene 0.5 0.5 0.5 Other ingredients 0.17% 0.17% 0.17% Adhesion strength (lbs/in) Near chill roll 3.65 0.95 2.76 Away chill roll 0.95 0.25 0.6 Average 1.56 0.87 1.22 2 According to Equistar, the improvement in adhesion to the styrenic 3 polymer layer obtained with the adhesive blends of the invention is readily 4 Appeal 2009-013212 Application 11/332,939 17 apparent from the data. It should be noted that while the addition of 1 elastomer [i.e., polymer (d),] to the comparative blends formulated using the 2 ethylene-hexene-1 LLDPE base resin improves adhesion (see Comparative 3 Example 5 versus Comparative Example 2 and Comparative Example 6 4 versus Comparative Example 3), the adhesion results are still significantly 5 lower than achieved with adhesive blends of the invention formulated using 6 ethylene-butene-1 LLDPE base resin. Specification, Â¶ 0050. 7 Set out below is data from Example 7 (not the invention due to the 8 amount of styrene (18%) in the S-I-S block copolymer) and Example 8 (not 9 the invention due to the amount of styrene (30%) in the S-I-S block 10 copolymer). 11 Appeal 2009-013212 Application 11/332,939 18 1 Example 7 8 Comparative Comparison Polymer (a) 64.83% 64.83% Ethylene-butene-1 Ethylene-butene-1 Density (g/cm3) 0.918 0.918 Melt Index (g/10 min) 2 7 Polymer (b) 25% 25% S-I-S S-I-S % styrene (S) 18% 30% Melt index (g/10 min) 12 13 % diblock <1 <1 Polymer (c) (graft) 10% 10% HDPE + MA HDPE + MA % MA 1.9% 1.9% Other ingredients 0.17% 0.17% Adhesion strength Near chill roll (lbs/in) 0.04 0.29 Away chill roll 0.01 0.23 Average Not reported Not reported 2 According to Equistar, adhesion at the styrenic polymer/tie-layer 3 interface obtained with the Comparative 7 adhesive blend was only 0.04 4 lbs/in at the interface nearest the chill roll and 0.01 at the interface away 5 from the chill roll--significantly lower than obtained with the blend of 6 Example 1 (44 % styrene). Specification, Â¶ 0051. 7 Further according to Equistar, while adhesion values with 8 Comparative Example 8 were somewhat improved over Comparative 9 Appeal 2009-013212 Application 11/332,939 19 Example 7 (adhesion at the interface nearest the chill roll was 0.29 lbs/in and 1 0.23 lbs/in at the interface away from the chill roll), the results were still 2 orders of magnitude less than obtained with the adhesive blend of Example 1 3 formulated using the high styrene content, high MI SIS copolymers. 4 Prior art 5 (1) Hattori 6 The invention described by Hattori is broader than the invention 7 defined by claim 1. 8 Reproduced below is Equistar claim 1 with references to the column 9 and line of Hattori inserted therein. Cf. Ex parte Braeken, 54 USPQ2d 1110, 10 1112-13 (B.P.A.I. 1999) 11 An adhesive composition [col. 1:7-8] consisting essentially of: 12 (a) 35 to 75 wt.% [col. 8:35â€”more preferably 40% to 70%], 13 based on the total weight of the [adhesive] composition, 14 ethylene-butene-1 [col. 3:49 and 52] linear [col. 3:34] low 15 density [col. 3:44] copolymer having 16 [1] a density from 0.912 to 0.925 g/cm3 [col. 3:60â€”17 preferably 0.89 to 0.94 g/cm3]and 18 [2] melt index from 0.5 to 15 g/10 min [col. 3:61-64â€”19 more preferably 0.1 to 30 g/10 min]; 20 (b) 15 to 45 wt.% [col. 8:38â€”more preferably 5% to 40%], 21 based on the total weight [of the adhesive composition], 22 styrene-isoprene-styrene [col. 6:38 (preferably styrene)] and 23 [col. 6:30-31 and 41 (isoprene)] triblock [col. 6:27-28â€”24 A-B-A]copolymer having 25 Appeal 2009-013212 Application 11/332,939 20 [1] a styrene content greater than 35 wt% [col. 6:46â€”1 preferably 10% to 70%], 2 [2] melt flow rate greater than 25 g/10 min [number 3 average molecular weight between 10,000 and 4 400,000â€”we understand that melt flow rate is an 5 indirect measure of molecular weight, high melt flow 6 rate corresponding to low molecular weight] and 7 [3] containing less that 1 wt.% diblock [col. 7:7-8â€”8 preferably A-B-A, which is not a diblock A-B]; and 9 (c) 1 to 25 wt.% [Col. 15, Table 1, Example 1â€”polymer A2 10 present in an amount of 10%], based on the total weight [of 11 the adhesive composition], [of a polymer selected from] 12 [1] ethylene homopolymer [col. 4:26] or 13 [2] ethylene C4-8 Î±-olefin copolymer [col. 3:49-52 and 14 col. 4:22], 15 grafted [col. 4:21] with 0.5 to 5 wt.% [col. 4:61â€”more 16 preferably 0.1 to 5 wt. %]of maleic anhydride [col. 4:51-52]. 17 Hattori teaches those skilled in the art the following. 18 First, if the density of polymer A1 (corresponding to Equistar's 19 polymer (a)) is less than 0.88 g/cm3, the resultant resin composition exhibits 20 poor adhesive strength at 60 ÂºC, where the postforming for a laminate is 21 carried out. On the other hand, if the density is over 0.945 g/cm3, the 22 resultant composition shows impaired adhesive strength at ordinary 23 temperatures and higher temperatures. Col. 4:4-9. Equistar's density falls 24 within the range of those said by Hattori to be acceptable. 25 Appeal 2009-013212 Application 11/332,939 21 Second, if the MFR of the polymer is outside of the range specified 1 above [more preferably 0.1 to 30 g/10 min], the resultant composition 2 exhibits lower or higher melt viscosity, and therefore possess low 3 processability. Col. 10-12. The claimed melt flow index for Equistar's 4 polymer (a) (0.5 to 15 g/10 min) falls within the range of those said to be 5 acceptable by Hattori. 6 Third, grafting less than 0.01 wt % unsaturated carboxylic acid or 7 derivative thereof, e.g., maleic anhydride, leads to the decrease in adhesion 8 of the resultant resin composition to EVOH; whereas a grafting amount of 9 over 10 wt % not only causes the partially crosslinking during the graft 10 polymerization process, resulting in decrease in moldability of the resultant 11 resin composition, but also causes the generation of fisheyes and lumps, 12 resulting in deterioration in appearance of the finished article, and further 13 leads to the deterioration in adhesion to other resins. Col. 4:58 through 14 col. 5:3. The amount of maleic anhydride graft of Equistar's polymer (c) is 15 consistent with Hattori. 16 Fourth, too small or too large amount of this polymer block (Hattori 17 polymer C and Equistar polymer (c)) disadvantageously leads to a decrease 18 in adhesive strength of the resultant resin composition. Col. 6:47-49. 19 Equistar's 15 to 45 wt % block falls within the preferably 10 to 70 wt. % 20 suggested by Hattori. 21 Fifth, larger or smaller molecular weights of Hattori polymer C 22 corresponding to Equistar's polymer (c) outside of a range of 10,000 to 23 400,000 leads to a decrease in adhesive strength of the resultant resin 24 composition. In addition, when a block copolymer having a number average 25 Appeal 2009-013212 Application 11/332,939 22 molecular weight of over 400,000 is used, the resulting composition 1 disadvantageously exhibits poor processability. Col. 6:58-63. 2 Sixth, when the Hattori resin composition is laminated onto an 3 EVOH, the resin composition should be blended with the component 4 A2 for increasing the adhesion to these resins. Hattori therefore tells one 5 skilled in the art that if you are adhering to EVOH, polymer A2 6 corresponding to Equistar's polymer (c) should be present. 7 Hattori explicitly indicates that its adhesive may be used to laminate 8 inter alia EVOH and PSâ€”polystyrene and high-impact polystyrene. 9 Col. 1:15-36. 10 (2) Lee 11 The invention described by Lee is broader than the invention defined 12 by claim 1. 13 Reproduced below is claim 1 with references to the column and line 14 of Lee inserted therein. 15 An adhesive composition [col. 3:2] consisting essentially of: 16 (a) 35 to 75 wt.% [col. 3:24-55 to85 wt. %], based on the total 17 weight of the [adhesive] composition, ethylene-butene-1 [col. 18 3:67 to col. 4:1 (ethylene) and col. 4:2 (butane-1)] linear low 19 density copolymer [col. 4:4-5 and col. 4:34-35] having 20 [1] a density from 0.912 to 0.925 g/cm3 [col. 3:26-0.86 21 to 0.97 g/cm3 overall and col. 4:27-28-0.91 to 0.935 22 g/cm3 for LLDPE] and 23 [2] melt index from 0.5 to 15 g/10 min [col. 12, Table 1, 24 melt index of 1.4 (LL1), 5 (LL3), and 12 (LL4)]; 25 Appeal 2009-013212 Application 11/332,939 23 (b) 15 to 45 wt.% [col. 6-15 to 45 wt. %], based on the total 1 weight [of the adhesive composition], styrene-isoprene-styrene 2 [col. 6:26 (styrene) and col. 6:9 (isoprene)] triblock [S-EB-S 3 triblock illustrated at col. 12, Table 1 (EL-4)] copolymer 4 having 5 [1] a styrene content greater than 35 wt% 6 [col. 6:34-37â€”preferred 10 to 50%], 7 [2] melt flow rate greater than 25 g/10 min [col. 6:39â€”8 melt index range of 0.001 to 100] and 9 [3] containing less that 1 wt.% diblock; and 10 (c) 1 to 25 wt.% [col. 6:12â€”modified and unmodified 11 preferably make up 60 to 80 wt. % of adhesive composition; 12 and col. 6:13-15â€”ratio modified to unmodified is 0-100 to 13 99-1 %], based on the total weight [of the adhesive 14 composition], [of a polymer selected from] 15 [1] ethylene homopolymer [col. 3:67 and col. 5:40-41] 16 or 17 [2] ethylene C4-8 Î±-olefin copolymer [col. 4:1-2 and 18 col. 5:40-41], 19 grafted [col. 6:1] with 0.5 to 5 wt.% [col. 6:3-4] of maleic 20 anhydride [col. 5:50]. 21 Lee reveals that the adhesive compositions in Table 3 were 22 coextruded between a layer of a propylene homopolymer of MFI 3 g/10 23 minutes, and a layer of an ethylene ionomer with a melt index of 1.7. 24 Col. 11:31-34. 25 Appeal 2009-013212 Application 11/332,939 24 Table 3 provides the following data for Examples C11, C25 and C26. 1 Col. 13. 2 Ex Unmodified polyethylene Grafted polyethylene Elastomer Wt. Peel Strength Code Wt. % Code Wt. % Code Wt. % grams per 25 mm C11 LL1 78 G3 12 EL-4 10 196 Â±14 C25 LL1 68 G3 12 EL-4 20 897Â±78 C26 LL1 58 G3 12 EL-4 30 1040Â±22 3 LL1 is a conventional LLDPE butane with a density of 0.024 g/cm3. 4 Col. 12, Table 1. 5 G3 is an ethylene/hexane copolymer grafted with 0.9 wt. % maleic 6 anhydride. Col. 12, Table 1. 7 EL-4 is a styrene-ethylene/butylene-styrene triblock with 29% styrene. 8 Col. 12. Table 1. 9 According to Lee, Comparative Example 11 shows that when the 10 styrene elastomer is below about 15% (10% or below), the adhesive 11 composition does not provide good peel strength. In contrast, Examples 25 12 and 26 which are identical in composition to Comparative example 11, 13 except that the styrene elastomer is above about 15%, demonstrate good peel 14 strength. 15 Appeal 2009-013212 Application 11/332,939 25 C. Discussion 1 1. Prima facie case of obviousness 2 Both Hattori and Lee appear to describe adhesive compositions which 3 encompass those of Equistar claim 1 on appeal. 4 The adhesives of Hattori and Lee are used to adhere layers of 5 polymers, with Hattori explicitly revealing adhesion of EVOH to styrene 6 polymer layers. 7 Under the circumstances, the Examiner has made out a prima facie 8 case of obviousness. In re Harris, 409 F.3d 1339, 1341 (Fed. Cir. 2005) (a 9 prima facie case of obviousness arises when the ranges of a claimed 10 composition overlap the ranges disclosed in the prior art); In re Peterson, 11 315 F.3d 1325, 1329 (Fed. Cir. 2003) (a prima facie case of obviousness 12 typically exists when the ranges of a claimed composition overlap the ranges 13 disclosed in the prior art); In re Boesch, 617 F.2d 272, 275 (CCPA 1980) 14 (where ranges overlap, a prima facie case of obviousness is made out). 15 Harris, Peterson, and Boesch foreclose Equistar's "wide range" 16 argument based on Hattori and Lee being "broad" inventions whereas the 17 claimed subject matter being a "narrower" invention. 18 2. The Hattori tackifier and consisting essentially of 19 Equistar maintains that Hattori fails as prior art because (1) Hattori 20 requires a tackifier and (2) claim 1 uses the claim transition phrase 21 "consisting essentially of" and does not call for a tackifier. 22 Equistar's adhesive compositions and Hattori's adhesive compositions 23 have a common utility. Both can be used to adhere EVOH to styrene 24 polymer films. 25 Appeal 2009-013212 Application 11/332,939 26 It is not apparent how the tackifier called for by Hattori would 1 materially affect the basic and novel characteristics of the claimed 2 composition. 3 Based on the Equistar specification, it is difficult to determine a 4 numerical peel strength which Equistar believes represents the "basic and 5 novel" characteristics of the Equistar invention. 6 We also note that no particular peel strength is recited in Equistar 7 claim 1. 8 3. S-I-S versus other block copolymers 9 Relying on Goto, Equistar maintains "that poor adhesion to styrenics 10 is obtained when certain SIS triblock polymers are combined with certain 11 LLDPE resins and grafted polyolefins." Appeal Brief, page 5. However, on 12 its face the sentence in the Appeal Brief suggests that poor adhesion will not 13 result when certain other SIS triblock polymers are combined certain other 14 LLDPE resins and grafted polyolefins. 15 In any event, the prior art teaches the use of several triblocks, 16 including (1) S-B-S (styrene-butadiene-styrene), (2) S-EB-S (styrene-17 ethylene/butylene-styrene) and (3) S-I-S (styrene-isoprene-styrene). 18 Equistar maintains that Lee does not describe S-I-S triblock 19 copolymers. A careful reading of Lee shows otherwise. Among the 20 "styrene-based elastomers" said to be useful by Lee are the KRAYTONÂ® 21 resinsâ€”actually the trademark is KRATONÂ®--including KRATON D. Lee, 22 col. 6:66. We understand the KRATON D series of polymers to be S-I-S 23 polymers. See, e.g., Lindquist, U.S. Patent 5,916,959 (29 June 1999), col. 9, 24 Appeal 2009-013212 Application 11/332,939 27 Table 1 referring to linear S-I-S block polymers identified as Kraton D-1112 1 and D-1107. 2 On this record, it is not apparent why one skilled in the art should not 3 be allowed to take, and would not have taken, advantage of known S-I-S 4 triblock polymer to be used for one of its intended purposes. 5 Equistar's use of a known S-I-S triblock polymer for its intended use 6 to achieve an expected result is evidence that the subject matter of claim 1 7 would have been obvious. KSR Int'l Co. v. Teleflex, Inc., 550 U.S. 398, 416 8 (2007) (combination of familiar elements according to known methods is 9 likely to be obvious when it does no more than yield predictable results). 10 4. The "discovery of a problem" evidence 11 Equistar maintains that it has discovered a problem in the art for 12 which it has an unexpected solution. Appeal Brief, page 6. 13 Goto, cited and discussed by Equistar, provides a different viewpoint. 14 According to Equistar, Goto is said to identify a poor adhesion problem with 15 use of S-I-S triblock polymers. Appeal Brief, page 5. 16 Equistar, therefore, has not identified a problem in the art. 17 Rather, Equistar has simply sought to find better adhesion solutionâ€”18 something which the prior art of record reveals those skilled in the art 19 continually seek to achieve. 20 5. The "unexpected" adhesion evidence 21 Generally, a showing of unexpected results must be commensurate in 22 scope with the breadth of the claims. In re Grasselli, 713 F.2d 731, 743 23 (Fed. Cir 1983) (objective evidence of non-obviousness must be 24 Appeal 2009-013212 Application 11/332,939 28 commensurate in scope with the claims which the evidence is offered to 1 support). 2 Moreover it is not enough to show results are obtained which differ 3 from those obtained in the prior artâ€”any difference must be shown to be an 4 unexpected difference. In re Klosak, 455 F.2d 1077, 1080 (CCPA 1972). 5 The Examiner found that the "unexpected results" data in the 6 specification is not commensurate in scope with the breadth of the claims. 7 Examiner's Answer, page 8. 8 The evidence supports the Examiner's finding. 9 As noted earlier, the significance of near chill roll and away chill roll 10 has not been explained. Likewise, not explained is the significance of the 11 "average" values reported for some of the examples. 12 The most that can be said for the data presented in Examples 1-8 is 13 that Equistar found that one particular combination may have provided what 14 Equistar would characterize as better adhesion than certain adhesives outside 15 the scope of claim 1. 16 However, it is not apparent how the one particular combination would 17 lead one skilled in the art to find that the adhesives of claim 1 generally 18 possess the properties said to have been found for the one particular 19 combination. 20 Equistar itself maintains that the results are unexpected. Why would 21 one skilled in the art be inclined to expect that the "unexpected" results said 22 to be shown in Examples 1 and 4 would result in other combinations of 23 polymers identified in claim 1? Equistar provides no cogent answer to this 24 question. For example, in Examples 1-3, only one density (0.918 g/cm3) 25 Appeal 2009-013212 Application 11/332,939 29 was tested. On what basis does Equistar maintain that a different density 1 would not show better results for an ethylene hexane-1 polymer (a)? 2 The "commensurate in scope" issue takes on particular significance in 3 this case given what the prior art tells us about the level of skill in this art. 4 Many of Equistar's Example 1-8 "data" findings are consistent with 5 suggestions in the prior art advising those skilled in the art concerning the 6 effect certain variables may have on ultimate adhesive properties. 7 Gotoâ€”cited by Equistarâ€”reveals that Goto adhesives are said to 8 adhere well to any polystyrene resin composition. Col. 2:39-40. 9 Data in Goto Table 1 (col. 5:22-35) and Table 2 (col. 5: 42-56) 10 support Goto's findings. 11 According to Goto, Examples 1A to 4B show that a MI2SB/MIPE 12 greater than 1.0, preferably greater than 3.0, is necessary for good adhesion 13 to PS (PS is polystyrene). Col. 5:33-35. Equistar's claimed compositions 14 are consistent with Goto's MI ratio teaching. 15 Further according to Goto, optimally the block copolymer should be 16 present in an amount of 40% to have good adhesion of EVOH to PS. 17 Col. 5:54-56. The Goto 40% falls squarely within Equistar's 15 to 45%. 18 According to Hattori, if the density of polymer A1 (corresponding to 19 Equistar's polymer (a)) is less than 0.88 g/cm3, the resultant resin 20 composition exhibits poor adhesive strength at 60 ÂºC. when the postforming 21 for a laminate is carried out. On the other hand, if the density is over 0.945 22 g/cm3, the resultant composition shows impaired adhesive strength at 23 ordinary temperatures and higher temperatures. Col. 4:4-9. Equistar's 24 density falls within the range of those said by Hattori to be acceptable. One 25 Appeal 2009-013212 Application 11/332,939 30 skilled in the art is taught the range of densities to consider. One skilled in 1 the art is not an automaton (KSR, 550 U.S. at 421). In our view, one skilled 2 in the art would have been able to determine an optimum density for any 3 particular combination of polymers. 4 Hattori reveals that if the MFR of polymer A1 is outside of a more 5 preferably 0.1 to 30 g/10 min range, the resultant composition exhibits lower 6 or higher melt viscosity, and therefore possess low processability. 7 Col. 10-12. The claimed melt flow index for Equistar's polymer (a) (0.5 to 8 15 g/10 min) falls within the range of those said to be acceptable by Hattori. 9 Hattori also reveals that grafting less than 0.01 wt % unsaturated 10 carboxylic acid or derivative thereof, e.g., maleic anhydride, leads to the 11 decrease in adhesion of the resultant resin composition to EVOH; whereas a 12 grafting amount of over 10 wt % not only causes the partially crosslinking 13 during the graft polymerization process, resulting in decrease in moldability 14 of the resultant resin composition, but also causes the generation of fisheyes 15 and lumps, resulting in deterioration in appearance of the finished article, 16 and further leads to the deterioration in adhesion to other resins. 17 Col. 4:58 through col. 5:3. The amount of maleic anhydride graft of 18 Equistar's polymer (c) is consistent with Hattori. 19 Like Goto, Hattori says that too small or too large amount of Hattori 20 polymer C (corresponding to Equistar polymer (c)) disadvantageously leads 21 to a decrease in adhesive strength of the resultant resin composition. 22 Col. 6:47-49. Equistar's 15 to 45 wt % block falls within the preferably 10 23 to 70 wt. % suggested by Hattori. One skilled in the art should therefore be 24 able to determine an appropriate percentage of Hattori polymer C. 25 Appeal 2009-013212 Application 11/332,939 31 When the Hattori resin composition is laminated onto an 1 EVOH, the resin composition should be blended with the component Hattori 2 polymer A2 for increasing the adhesion to these resins. Hattori therefore 3 tells one skilled in the art that if you are adhering to EVOH, polymer A2 4 corresponding to Equistar's polymer (c) should be present. 5 The evidence suggests that the level of ordinary skill in this art knows 6 a lot about the effect of one variable on the overall properties. The level of 7 skill in this art shows precisely why there is a need in this case for a showing 8 of unexpected results to be commensurate in scope with the claimed 9 invention. 10 Other arguments 11 We have considered Equistarâ€™s remaining arguments and find none 12 that warrant reversal of the Examinerâ€™s rejection(s). Cf. Hartman v. 13 Nicholson, 483 F.3d 1311, 1315 (Fed. Cir. 2007). 14 D. Decision 15 Upon consideration of the appeal, and for the reasons given herein, as 16 well as those given by the Examiner in the Examiner's Answer and the 17 Advisory Action entered 27 June 2008, it is 18 ORDERED that the decision of the Examiner rejecting 19 claims 1-18 over Hattori and Lee is affirmed. 20 FURTHER ORDERED that no time period for taking any 21 subsequent action in connection with this appeal may be extended under 22 37 C.F.R. Â§ 1.136(a)(1)(iv) (2008). 23 AFFIRMED Appeal 2009-013212 Application 11/332,939 32 rvb cc (via First Class mail) Mr. Shao-Hua Guo Lyondell Chemical Company 3801 West Chester Pike Newtown Square, PA 19073-2387