Ex Parte Jewson et alDownload PDFBoard of Patent Appeals and InterferencesAug 24, 200610435175 (B.P.A.I. Aug. 24, 2006) Copy Citation The opinion in support of the decision being entered today was not written for publication and is not binding precedent of the Board. UNITED STATES PATENT AND TRADEMARK OFFICE ____________ BEFORE THE BOARD OF PATENT APPEALS AND INTERFERENCES ____________ Ex parte JENNIFER D. JEWSON C. ANDREW JONES and RALPH M. DESSAU ____________ Appeal No. 2006-1750 Application No. 10/435,175 ____________ ON BRIEF ____________ Before GARRIS, KRATZ and TIMM, Administrative Patent Judges. KRATZ, Administrative Patent Judge. DECISION ON APPEAL This is a decision on appeal from the examiner's final rejection of claims 12-18, which are all of the claims pending in this application.1 BACKGROUND 1 This application is a divisional of Application No. 09/507,842, now abandoned. In the parent application, we entered a decision affirming an obviousness rejection that was before us in Appeal No. 2003-0630. Appellants' invention relates to a method for preparing a titanium zeolite catalyst using impregnation to add palladium and gold compounds. The catalyst is disclosed as being useful in Appeal No. 2006-1750 Application No. 10/435,175 Παγε 2 epoxidation reactions. See, e.g., pages 3 through 5 of appellants’ specification. A further understanding of the invention can be derived from a reading of exemplary claim 12, which is reproduced below. A method for preparing a catalyst comprising the steps of: (a) impregnating a titanium zeolite with a solution of a palladium compound and a gold compound in a solvent; (b) removing the solvent from the impregnated titanium zeolite; and (c) drying the impregnated titanium zeolite. The prior art references of record relied upon by the examiner in rejecting the appealed claims are: Muller et al. (Muller) 5,859,265 Jan. 12, 1999 Bowman et al. (Bowman) 6,031,116 Feb. 29, 2000 Grosch et al. (Grosch) WO 99/52626 Oct. 21, 1999 Appeal No. 2006-1750 Application No. 10/435,175 Παγε 3 (published International Pat. Appl. No. PCT/EP99/02355)2 2 Our references to Grosch are to U.S. Patent No. 6,551,546, which patent is employed as an English language equivalent (translation) of WO 99/52626 by the examiner. See page 5, line 3 of the answer. Appellants do not dispute the examiner’s reliance on U.S. Patent No. 6,551,546 as an acceptable English language equivalent (translation) of the disclosure of WO 99/52626. Claims 12-16 and 18 stand rejected under 35 U.S.C. § 103(a) as being unpatentable over Grosch in view of Muller. Claim 17 stands rejected under 35 U.S.C. § 103(a) as being unpatentable over Grosch in view of Muller and Bowman. We refer to the brief and reply brief and to the answer for a complete exposition of the opposing viewpoints expressed by appellants and the examiner concerning the issues before us on this appeal. OPINION Appeal No. 2006-1750 Application No. 10/435,175 Παγε 4 Having carefully considered each of appellants’ arguments set forth in the brief and reply brief and the specification evidence relied on in support thereof, appellants have not persuaded us of reversible error on the part of the examiner. Accordingly, we affirm the examiner’s rejections for substantially the reasons set forth by the examiner in the answer. We add the following for emphasis. Rejection of claims 12-16 and 18 Appellants do not argue claims 12-16 and 18 separately. Thus, we consider these claims as a group and select claim 12 as the representative claim on which we decide this appeal as to this ground of rejection. The examiner has determined that Grosch discloses a method of preparing a zeolite (titanium silicalite) catalyst body wherein one or more noble metals selected from ruthenium, rhodium, palladium, osmium, iridium, platinum, rhenium, gold and silver are added to the catalyst via an impregnation technique that employs a solvent. Grosch teaches that the catalyst is subjected to a drying step, as noted by the examiner at page 3 of the answer. See, e.g., column 8, line 62 through column 9, line 30 of Grosch. Grosch discloses, inter alia, that the product catalysts can be used as oxidation catalysts, including as a Appeal No. 2006-1750 Application No. 10/435,175 Παγε 5 catalyst for epoxidizing olefins. See, e.g., column 10, lines 1-36 of Grosch. Muller teaches a catalyst comprising titanium having a zeolite structure, a platinum group metal such as palladium, and optionally modified with an additional metal selected from among iron, cobalt, nickel rhenium, silver and gold. The catalyst may be employed in an epoxidation process. See, e.g., column 1, lines 25-63 and column 2, lines 33-36 of Muller. Muller teaches that the catalyst can be prepared by impregnating a titanium zeolite structure with platinum metal salt solution, subjecting the impregnated zeolite structure to evaporation (ostensibly to remove solvent) followed by heating (drying) to form the catalyst. See column 2, line 48 through column 3, line 17 and Example 2 of Muller. As for the optional additional iron, cobalt, nickel rhenium, silver or gold elements suggested by Muller, Muller does not exemplify how any of those metals are added but does state a desire for easy preparation of the catalyst. See column 1, lines 25-28 of Muller. It follows that one of ordinary skill in the art would have been led to add such an additional metal, including gold, via a conventional method, such as the impregnation method as taught by Muller (and Grosch) for the palladium metal addition. Appeal No. 2006-1750 Application No. 10/435,175 Παγε 6 Based on that similarity of catalyst composition, catalyst utility, and method of preparation taught by Grosch and Muller, we agree with the examiner’s reasonable determination that the appellants’ catalyst preparation method, including the use of impregnation, solvent removal and drying as set forth in representative claim 12, is reasonably suggested by the combined teachings of the applied references in a manner that would have rendered the claimed subject matter prima facie obvious to one of ordinary skill in the art. In this regard, the selection of palladium and gold as the additives for the titanium zeolite catalyst of Grosch would have been well within the level of ordinary skill in the art, especially given the relatively small list of additive ingredients suggested by each of Grosch and Muller. Appellants maintain that “Grosch does not teach the required impregnation of a titanium zeolite with a solution of a palladium and a gold compound in a solvent” (brief, page 3). Also, appellants argue that Muller (brief, pages 3-5) does not teach how and why the optional elements, including gold are incorporated in the zeolite catalyst. In this regard, appellants assert (brief, pages 6-8 and reply brief, page 1) that the claimed method requires that a zeolite is simultaneously Appeal No. 2006-1750 Application No. 10/435,175 Παγε 7 impregnated with a solution of a palladium compound and a gold compound in a solvent. We do not find appellants’ arguments persuasive for reasons set forth in the answer, and as further explained herein. Representative claim 12 does not require the simultaneous addition of gold and palladium via impregnation, as argued. In this regard, representative claim 12 recites “... impregnating a titanium zeolite with a solution of a palladium compound and a gold compound in a solvent ....” Thus, the zeolite is required to be impregnated with a solution of a palladium compound and the zeolite is required to be impregnated with a gold compound in a solvent. However, representative claim 12 does not require that the palladium compound and the gold compound are incorporated into the same solution and that such a solution is used for simultaneously impregnating the zeolite with both additives. In this regard, the conjunctive term “and”, as employed in claim 12, does not clearly require that the solution contains both compounds. Indeed, the claim phrase “gold compound in a solvent” is inclusive of an embodiment wherein a solution of gold compound (gold compound in a solvent) that is distinct from the solution of a palladium compound is employed in the impregnation in either a serial or concurrent manner. Thus, representative claim 12 Appeal No. 2006-1750 Application No. 10/435,175 Παγε 8 does not require the disclosed option of simultaneous addition of the compounds. Moreover, even if we could agree with appellants that representative claim 12 requires the concurrent impregnation addition of palladium and gold to the zeolite, such a limitation, by itself, would not patentably distinguish appellants’ method over the method suggested by the applied references. This is so since Muller is concerned with using a catalyst for the oxidation that is easy to prepare. Muller fully describes how platinum group metals, such as palladium, may be incorporated into the catalyst by impregnation using a solvent and a salt form of the metal. Clearly, one of ordinary skill in the art would have been led to incorporate one of the additional disclosed metals, such as gold, via a similar impregnation method with a reasonable expectation of success in so doing.3 Thus, one of ordinary skill 3 Muller does not explicitly disclose a separate reason for additionally modifying a catalyst with one or more elements selected from iron, cobalt, nickel, rhenium, silver and gold, as disclosed as column 2, lines 33-39 of the patent. However, the lack of express disclosure of a separate reason for incorporating those additional additives taught by Muller does not militate against the use of one or more of those additional catalyst modifiers to achieve a desirable catalyst as taught by Muller. Indeed, Muller teaches that the catalyst is not only easy to prepare but does not suffer disadvantages associated with prior art catalysts. See column 1, lines 20-43 of Muller. Thus, one of ordinary skill of the art would be guided by these previously stated purposes in choosing to add such additional modifier(s). Appeal No. 2006-1750 Application No. 10/435,175 Παγε 9 in the art would have readily recognized that the impregnations could be conducted serially or simultaneously based on the combined teachings of Grosch and Muller. After all skill, and not the converse, is presumed on the part of those practicing in the art. See In re Sovish, 769 F.2d 738, 743, 226 USPQ 771, 774 (Fed. Cir. 1985); In re Jacoby, 309 F.2d 513, 516, 135 USPQ 317, 319 (CCPA 1962). Also, see the teachings of Grosch at column 8, line 62 through column 9, line 15 and as further referred to herein and in the answer. Appellants note the generic addition methods for catalyst modifiers as set forth in the applied references (brief, page 6), as if the other addition options disclosed therein detract from the teaching of impregnation set forth in Grosch and Muller. Such an argument is clearly unpersuasive in that the disclosure of each of the limited number of addition options set forth in the applied references, including impregnation, are clear and instructive to one of ordinary skill in the art as to how to add a metal promoter. Certainly, these teachings are not destructive Appeal No. 2006-1750 Application No. 10/435,175 Παγε 10 of each other. Moreover, we note that appellants’ specification undercuts such a line of argument in that appellants present several ways of incorporating the catalyst components other than impregnation while acknowledging that the manner of incorporating palladium into the catalyst is not critical. See page 4, line 12 through page 5, line 21 of appellants’ specification. As for appellants’ remarks regarding the lack of examples disclosing how to add palladium and gold in the applied references, it cannot be overemphasized that a reference must be considered in its entirety and that the disclosure of a reference is not limited to specific working examples contained therein. See In re Fracalossi, 681 F.2d 792, 794 n.1, 215 USPQ 569, 570 n.1 (CCPA 1982); In re Lamberti, 545 F.2d 747, 750, 192 USPQ 278, 280 (CCPA 1976). Appellants maintain that appellants’ claimed process is attended by unexpected results. Appellants (brief, page 8 and reply brief, pages 2 and 3) point to Example 4 and Example 7 of the specification wherein catalysts of Example 1 and Example 6, respectively, are employed in the epoxidation of propylene. Appellants assert that those examples demonstrate that “a simultaneous addition of palladium and gold results in significantly higher oxygen to POE selectivity and hydrogen to Appeal No. 2006-1750 Application No. 10/435,175 Παγε 11 POE selectivity compared to a catalyst in which a palladium- containing titanium zeolite is first formed followed by addition of gold” (reply brief, pages 2 and 3). The question as to whether unexpected advantages have been demonstrated is a factual question. In re Johnson, 747 F.2d 1456, 1460, 223 USPQ 1260, 1263 (Fed. Cir. 1984). Thus, it is incumbent upon appellants to supply the factual basis to rebut the prima facie case of obviousness established by the examiner. See, e.g., In re Klosak, 455 F.2d 1077, 1080, 173 USPQ 14, 16 (CCPA 1972). Appellants, however, do not refer to an adequate factual showing in the specification to support a conclusion of unexpected advantages. In this regard, we note that the catalyst employed in the Example 4 reaction test was prepared by a method that differs substantially from the method of preparation of the catalyst employed in Example 7. For example, the catalyst used in Example 4 was prepared using particular metal salts and long stirring times as detailed in the following steps of Example 1 of the specification: The pre-calcined TS-1 (20 g), [Pd (NH3)4] (NO3)2 (2.06 g of a 5 weight percent Pd solution in water), AuCl3 (0.0317 g), and distilled water (80 g) are placed in a 250-mL single-neck round-bottom flask forming a pale white mixture. The flask is connected to a 15- inch cold water condenser and then blanketed with Appeal No. 2006-1750 Application No. 10/435,175 Παγε 12 nitrogen at a 150 cc/min flow rate. The flask is inserted into an oil bath at 80 °C and the reaction slurry is stirred. After stirring for 24 hours, the slurry is transferred to a roto-vap and the water is removed by roto-evaporation under vacuum at 50 °C. The solid catalyst is then dried at 60 °C in a vacuum oven for 24 hours. Measured Pd loading of the catalyst is 0.40 wt.% and the measured Au loading is 0.09 wt.%. Contrastingly, the catalyst employed in the Example 7 reaction test was prepared by a method that differed by more than the lack of simultaneous gold and palladium addition from the catalyst employed in Example 4 as evident by the use of different metal salts in different amounts, much shorter stirring times, and a hydrogen reduction step. See Examples 5 and 6 of the specification for the manner of preparing the catalyst used in Example 7. Not only is a catalyst composition that differs by more than the order of addition of palladium and gold used in Example 7 (as compared to the catalyst used in Example 4), but the reaction test employed in Examples 4 and 7 differ. For example, the relative amounts of propylene, hydrogen and oxygen employed in Examples 4 and 7 were not the same. Also, the pressure employed during the reactions of Example 4 and 7 differed. Moreover, in Example 4 both gas and liquid phase products are analyzed whereas in Example 7 only the exit-gas is Appeal No. 2006-1750 Application No. 10/435,175 Παγε 13 analyzed. The cause-and-effect relationship which appellants desire to show between step wise and simultaneous palladium and gold addition is lost in such a welter of unfixed variables. See In re Heyna, 360 F.2d 222, 228, 149 USPQ 692, 697 (CCPA 1966); In re Dunn, 349 F.2d 433, 439, 146 USPQ 479, 483 (CCPA 1965). Thus, a comparison between the PO equivalent products (POE), as referred to in Example 4 and the PO product (propylene oxide) as measured in Example 7 cannot be fairly made.4 Hence, we are not satisfied that the evidence of record that is offered for comparison, as discussed in the briefs, demonstrates results that are truly unexpected over the closest prior art for reasons set forth above and in the answer. Nor have appellants satisfied their burden of explaining how the results reported for the limited tests presented can be extrapolated to substantiate appellants’ contentions for the invention as broadly claimed. Thus, the examiner correctly notes (answer, pages 10 and 11) that appellants have not satisfied the well established criterium that the evidence relied on to establish unobviousness must be commensurate in scope with the claimed subject matter. See In re Kerkhoven, 626 F.2d 846, 851, 205 USPQ 1069, 1072-73 (CCPA 1980) 4 The POE products include not only PO but also PG (propylene glycol), DPG (diphenylguanidine) and acetol according to appellants. See Example 4 of the specification. Appeal No. 2006-1750 Application No. 10/435,175 Παγε 14 and In re Clemens, 622 F.2d 1029, 1035, 206 USPQ 289, 296 (CCPA 1980). Under the circumstances recounted above, it is our determination that the evidence of record for and against a conclusion of obviousness, reconsidered in light of the respective arguments and evidence advanced by appellants and the examiner, on balance, weighs most heavily in favor of an obviousness conclusion with respect to the rejection under consideration. Accordingly, we sustain the examiner's § 103(a) rejection of claims 12-16 and 18. Rejection of dependent claim 17 Dependent claim 17 requires that the gold compound employed is selected from halides, cyanides, hydroxides, and sulfides. In the separate rejection of dependent claim 17, the examiner additionally relies on the teachings of Bowman to show that a soluble gold compound, such as a gold cyanide is known to be useful in adding a gold promoter to a zeolite catalyst. See, e.g., column 9, lines 23-26 of Bowman.5 In addition to the arguments and evidence advanced against the examiner’s rejection of independent claim 12, which we find 5 Also, we note that Bowman (column 10, lines 25-33) discloses the simultaneous addition of multiple promoter metals as an option. Appeal No. 2006-1750 Application No. 10/435,175 Παγε 15 unpersuasive for reasons set forth above, appellants maintain that Bowman excludes palladium promoter in a preferred embodiment leaving little incentive to combine Bowman with Grosch and Muller. We disagree for reasons set forth by the examiner in the answer (page 11). In this regard, Grosch teaches that water soluble salts should be employed in adding metals, such as gold, to the catalyst. See, e.g., column 8, lines 62 through column 9, line 7 of Grosch. Nor is the teaching value of Bowman limited to one preferred embodiment thereof that would exclude palladium. It follows that, on this record, we affirm the examiner’s separate obviousness rejection of claim 17. CONCLUSION The decision of the examiner to reject claims 12-16 and 18 under 35 U.S.C. § 103(a) as being unpatentable over Grosch in view of Muller and to reject claim 17 under 35 U.S.C. § 103(a) as being unpatentable over Grosch in view of Muller and Bowman is affirmed. Appeal No. 2006-1750 Application No. 10/435,175 Παγε 16 No time period for taking any subsequent action in connection with this appeal may be extended under 37 CFR § 1.136(a)(1)(iv)(2004). AFFIRMED BRADLEY R. GARRIS ) Administrative Patent Judge ) ) ) ) ) BOARD OF PATENT PETER F. KRATZ ) APPEALS Administrative Patent Judge ) AND ) INTERFERENCES ) ) ) CATHERINE TIMM ) Administrative Patent Judge ) PFK/TF Appeal No. 2006-1750 Application No. 10/435,175 Παγε 17 LYONDELL CHEMICAL COMPANY 3801 WEST CHESTER PIKE NEWTOWN SQUARE, PA 19073 Comment [jvn1]: Type address Copy with citationCopy as parenthetical citation