Ex Parte Mertens et alDownload PDFPatent Trial and Appeal BoardSep 30, 201612477826 (P.T.A.B. Sep. 30, 2016) Copy Citation UNITED STA TES p A TENT AND TRADEMARK OFFICE APPLICATION NO. FILING DATE 12/477,826 0610312009 23455 7590 10/04/2016 EXXONMOBIL CHEMICAL COMPANY 5200 BA YW A Y DRIVE P.O. BOX 2149 BAYTOWN, TX 77522-2149 FIRST NAMED INVENTOR Machteld M. Mertens UNITED STATES DEPARTMENT OF COMMERCE United States Patent and Trademark Office Address: COMMISSIONER FOR PATENTS P.O. Box 1450 Alexandria, Virginia 22313-1450 www .uspto.gov ATTORNEY DOCKET NO. CONFIRMATION NO. 2008EM181/2 8257 EXAMINER ENG, ELIZABETH ART UNIT PAPER NUMBER 1762 NOTIFICATION DATE DELIVERY MODE 10/04/2016 ELECTRONIC Please find below and/or attached an Office communication concerning this application or proceeding. The time period for reply, if any, is set in the attached communication. Notice of the Office communication was sent electronically on above-indicated "Notification Date" to the following e-mail address( es): chem.law. prosecution@exxonmobil.com PTOL-90A (Rev. 04/07) UNITED STATES PATENT AND TRADEMARK OFFICE BEFORE THE PATENT TRIAL AND APPEAL BOARD Ex parte MACHTELD M. MERTENS and GUANG CAO Appeal2015-003629 Application 12/477,826 Technology Center 1700 Before ADRIENE LEPIANE HANLON, TERRY J. OWENS, and JENNIFER R. GUPTA, Administrative Patent Judges. GUPTA, Administrative Patent Judge. DECISION ON APPEAL Appellants 1 appeal under 35 U.S.C. § 134(a) from the Examiner's decision2 finally rejecting claims 33--41. 3 We have jurisdiction under 35 U.S.C. § 6(b). We affirm. The claims are directed to a method of synthesizing a silicoaluminophosphate molecular sieve having 90% or greater CHA 1 Appellants identify the real party in interest as ExxonMobil Chemical Patents Inc. Appeal Brief filed October 14, 2014 ("App. Br."), 1. 2 Final Office Action mailed July 22, 2014 ("Final Act."). 3 In a Response under 37 C.F.R. § 1.116 filed August 15, 2015, Appellants amended claim 33 to include the limitations of claims 42 and 43. As a result claims 42 and 43 were cancelled .. Appeal2015-003629 Application 12/477,826 framework-type character. Spec. if 26. Claim 33, reproduced below, is illustrative of the claims on appeal. 33. A method of preparing a silicoaluminophosphate molecular sieve, the method comprising: (a) providing a synthesis mixture comprising a source of aluminum, a source of phosphorus, a source of silicon, and N,N-dimethylcyclohexylamine organic template, wherein the synthesis mixture exhibits a Si/Ab ratio less than 0.33; and (b) inducing crystallization of a silicoaluminophosphate molecular sieve, which exhibits 90% or greater CHA framework type character, from said synthesis mixture at a crystallization temperature of at least 165°C for a crystallization time from about 5 minutes to about 350 hours, wherein the alumina and phosphoric acid are first combined to form a synthesis mixture, followed by addition of the organic template and tetraalkylorthosilicate, and the synthesis mixture is aged at a temperature of between 0°C and 5 0°C, and for an aging time of at least 5 minutes; wherein (i) the crystallized silicoaluminophosphate molecular sieve exhibits a Si/ Ab ratio less than 0.33, (ii) the crystallized silicoaluminophosphate molecular sieve exhibits a Si/ Ab ratio not more than 0 .10 greater than the Si/ Ab ratio of the synthesis mixture, or (iii) both (i) and (ii); and wherein the crystallized silicoaluminophosphate molecular sieve is recovered from step (b) in a yield that is at least 2.0% greater than a yield obtained by recovering a silicoaluminophosphate molecular sieve crystallized from an identical synthesis mixture at a crystallization temperature of l 60°C or less for a crystallization time from about 5 minutes to about 3 5 0 hours. App. Br. 13 (Claims Appendix) (emphasis added to highlight key limitations). 2 Appeal2015-003629 Application 12/477,826 REJECTIONS ON APPEAL 4 1. Claims 33-35, 37, and 39 stand rejected under 35 U.S.C. § 103(a) as unpatentable over Cao et al. (US 2004/0253163 Al, published Dec. 16, 2004) (hereinafter "Cao") in view of Davis et al. (US 5,374,411, issued Dec. 20, 1994) (hereinafter "Davis"); 5 and 2. Claims 36, 38, 40, and 41 stand rejected under 35 U.S.C. § 103(a) as unpatentable over Cao in view of Davis, and further in view of Verduijn et al. (US 6,974,889 Bl, issued Dec. 13, 2005) (hereinafter "Verduijn"). ANALYSIS Appellants' arguments focus on limitations that appear in claim 33. Appellants do not present separate arguments for the patentability of the dependent claims, including separately rejected claims 36, 38, 40, and 41. Consequently, we confine our discussion to claim 33, and claims 34--41 will stand or fall with claim 33. 4 In response to the Final Office Action, Appellants deleted the recitation "having a controlled acid site density" from claim 33, and the recitation "step ( c )" from claim 38. See Response under 37 C.F .R. § 1.116 filed August 15, 2014, 2-3. The Examiner's Advisory Action mailed September 16, 2014 indicates that for purposes of appeal, the amendments will be entered. Thus, the rejection of claims 33--43 under§ 112, second paragraph set forth by the Examiner in the Final Office Action is effectively moot in view of the amendments to claims 33 and 38, despite the Examiner's Answer not identifying the rejection as having been withdrawn. See Examiner's Answer mailed February 9, 2015 ("Ans."), generally. 5 The Examiner does not identify claim 34 in the statement of rejection. Ans. at 2. We consider this harmless error, however, because the Examiner explicitly addresses claim 34 in the body of the rejection. Id. at 5. 3 Appeal2015-003629 Application 12/477,826 Cao discloses a method of preparing a silicoaluminophosphate molecular sieve with 90% or greater CHA framework type (Cao i-fi-f l and 56). The method of Cao includes providing a synthesis mixture comprising an aluminum component (preferably alumina), a phosphorus component (preferably phosphoric acid), a silicon component (e.g., tetraalkylorthosilicate ), and a templating agent (preferably N,N- dimethylcyclohexylamine ), where the synthesis mixture has a Si/ Ah ratio of less than 0.33 (Cao i-fi-138, 61, 74, 126-127). Cao teaches that the components of the mixture are sequentially and slowly combined with stirring to form a uniform gel-first adding alumina to phosphoric acid, and then adding the silicon component and the templating agent (Cao i-fi-f 126- 127; see also US 4,440,871 (issued Apr. 3, 1984) to Lok et al. (hereinafter "Lok"), 9:39-52 (Example 1), which is incorporated by reference at Cao i1 61 ). The gel is then heated to induce crystallization at a temperature of 180 QC for 3 to 7 days (72 to 168 hours) (Cao i-f 127). Davis discloses a method of preparing crystalline silicoaluminophosphate compositions with VPI-5 structures by first mixing a phosphorus source and an aluminum source together while stirring to ensure a homogenous mixture, aging the precursor mixture at room temperature for a period of from about 1 to about 5 hours for the pH to stabilize, and then adding a silicon source (preferably tetraethylorthosilicate ), and an organic template (e.g., tetrabutylammonium hydroxide) (Davis 7:7--44 and 8:10-25). The Examiner finds that Cao teaches the steps for preparing a silicoaluminophosphate molecular sieve as recited in claim 33 including combining the components sequentially (Cao i-f 127). Ans. 2-3. The Examiner, however, acknowledges that Cao' s method differs from the 4 Appeal2015-003629 Application 12/477,826 method recited in claim 33 in two respects: ( 1) first combining alumina and phosphoric acid to form a synthesis mixture and then aging the mixture of at room temperature for at least 5 minutes (see claim 33, first wherein clause), and (2) recovering the crystallized silicoaluminophosphate molecular sieve after crystallization at a temperature of at least 165 QC for about 5 minutes to about 350 hours in a yield that is at least 2.0% greater than the yield obtained by recovering a silicoaluminophosphate molecular sieve crystallized from an identical synthesis mixture at a crystallization temperature of 160 QC or less for a crystallization time from about 5 minutes to about 350 hours (see claim 33, last wherein clause). Ans. 2--4. With regard to (1 ), the Examiner finds that Davis teaches a method for forming silicoaluminophosphate compositions that includes first combining a phosphorous source and an aluminum source while stirring to ensure a homogenous mixture, aging the mixture at room temperature for a period of from about 1 to about 5 hours to stabilize pH of the mixture, and then adding an organic template and a silicon source (Davis 7:24--38; 13:42-52 (Example 9) ). Ans. 3. The Examiner finds that one of ordinary skill in the art would have been motivated, based on Davis, to age Cao' s primary mixture of alumina and phosphoric acid at room temperature for from about 1 to about 5 hours to stabilize the pH of the mixture prior to adding the organic template and tetraalkylorthosilicate. Ans. at 4. With regard to (2), the Examiner finds that because Cao teaches the identical synthesis mixture as recited in claim 33, and crystallizing the synthesis mixture at a temperature of 180 QC for 3 days (72 hours), which is within the temperature and time ranges recited in claim 33, one of ordinary skill in the art would reasonably expect to recover the crystallized 5 Appeal2015-003629 Application 12/477,826 silicoaluminophosphate molecular sieve in a yield that is at least 2.0% greater than a yield obtained by recovering a silicoaluminophosphate molecular sieve crystallized from an identical synthesis mixture at a crystallization temperature of 160 QC or less for a crystallization time from about 5 minutes to about 350 hours. Ans. at 4--5. Appellants argue that Cao and Davis are directed to solving different problems by different means, and thus there would have been no motivation to combine the references. App. Br. 6. 6 Cao teaches synthesizing silicoaluminophosphates of the CHA framework type by first adding a phosphorus source into a homogenizer, and then adding Catapal™ (Ab03), Cabosil™ (silica), and N,N-dimethylcyclohexylamine sequentially to form a uniform gel. Cao i-fi-f 126-12 7 (Example 1).7 Because the last three ingredients are added sequentially, the phosphorus source and the aluminum source are contacted first, which are then contacted with silicon source and the organic template as claimed. See also Lok 9:37-52 (Example 1) 6 Appellants also argue that a person in the art would not look to V erduijn to combine with Cao as it is solving a different problem in a different manner. App. Br. 6. Verduijn, however, is not relied upon by the Examiner in the rejection of claim 33. Additionally, the scope of analogous art includes references "from the same field of endeavor, regardless of the problem addressed" and references not within the inventor's field endeavor, but "still ... reasonably pertinent to the particular problem with which the inventor is involved." In re Klein, 647 F.3d 1343, 1348 (Fed. Cir. 2011). Verduijn, like Appellants, is focused on preparing silicoaluminophosphate molecular sieves of the CHA structure. Compare Spec. i1 2 with Verduijn 2: 12-17. Accordingly, one of ordinary skill in the art would have looked to Verduijn to combine with Cao. 7 Although silica is used as the silicon source in Cao' s Example 1, Cao teaches tetraethylorthosilicate as another advantageous silicon source. Cao i174. 6 Appeal2015-003629 Application 12/477,826 (preparing a silicoaluminophosphates by first mixing phosphoric acid and alumina until homogeneous, followed by addition of a source of silicon and a templating agent). Davis, like Cao, is directed to preparing crystalline silicoaluminophosphate compositions albeit with a different crystalline structure. Davis, like Cao, teaches first mixing the phosphorus and aluminum sources while stirring to ensure homogeneity, and then adding a source of silicon and a templating agent. Davis 7:20-8: 17. In addition, Davis teaches aging the phosphorus/aluminum precursor mixture to stabilize pH of the mixture, preferably at room temperature from about 1 to about 5 hours, prior to adding the silicon source and templating agent. Id. at 7:32- 8: 12; see also Lok 56:53-58 (teaching aging a silicoaluminophosphate gel composition at low temperatures). Appellants have not explained why a person of skill in the art would not have been motivated, based on the teachings of Davis, to age the Cao' s precursor mixture of alumina and phosphoric acid to sufficiently stabilize pH of the mixture prior to adding the tetraalkylorthosilicate and N ,N-dimethylcyclohexylamine organic template. There must be articulated reasoning with some rational underpinning to support the legal conclusion of obviousness. In re Kahn, 441 F .3d 977, 988 (Fed. Cir. 2006). In this instance, the Examiner has provided such reasoning (Ans. 3--4), and Appellants do not explain why the Examiner's reasoning is erroneous. Thus, Appellants' argument is not persuasive of reversible error in the Examiner's rejection. Appellants argue that the art of synthesizing molecular sieves is much too unpredictable to simply combine disparate references with no regard for what problem was being solved and what kind of product is being generated, and to do so is at best hindsight. App. Br. 8; see also Reply Brief filed 7 Appeal2015-003629 Application 12/477,826 February 16, 2015 ("Reply Br."), 3. To support this argument, Appellants rely on a number of publications of record including Verheyen, Davis & Lobo, Wilson. See App. Br. at 8-11. These publications merely show that the art in question possesses some degree of unpredictability. Obviousness, however, cannot be avoided simply by a showing of some degree of unpredictability in the art. "Only a reasonable expectation of success, not absolute predictability, is necessary for a conclusion of obviousness." In re Langi, 759 F.2d 887, 897 (Fed.Cir.1985). Appellants have not explained why one of ordinary skill in the art would not have had a reasonable expectation that Davis' step of aging the alumina and phosphoric acid mixture prior to adding the source of silicon and the organic template would have been successful in the method of Cao. Accordingly, Appellants' arguments is not persuasive of reversible error in the Examiner's rejection. Appellants argue that the Examiner reversibly erred in finding Cao discloses recovering the crystallized silicoaluminosphosphate molecular sieve after crystallization at a temperature of at least 165 QC for about 5 minutes to about 350 hours in a yield that is at least 2.0% greater than the yield obtained using an identical synthesis mixture at a crystallization temperature of 160 QC or less for 5 minutes to 350 hours (claim 33, last wherein clause). App. Br. 7-8. As discussed above, Cao teaches a synthesis mixture and sequence of mixing that are the same as recited in claim 3 3. In addition, Cao teaches crystallizing the synthesis mixture at a temperature of 180 QC for 3 days (72 hours), which is within the crystallization conditions recited in claim 33. As discussed above, Davis teaches aging the aluminum and phosphorus mixture prior to adding the silicon source and organic template as claimed in claim 33. Thus, the Examiner's finding on this 8 Appeal2015-003629 Application 12/477,826 record that one of ordinary skill in the art would expect the yield of crystallized silicoaluminosphosphate molecular sieve recovered in Cao' s method, as modified by Davis, after crystallization at a temperature of 180QC for 72 hours, would be at least 2.0% greater than the yield obtained using an identical synthesis mixture at a crystallization temperature of 160 QC or less for 5 minutes to 350 hours is reasonable. See Ex parte Obiaya, 227 USPQ 58, 60 (BP AI 1985) ("The fact that appellant has recognized another advantage which would flow naturally from following the suggestion of the prior art cannot be the basis for patentability when the differences would otherwise be obvious."). Finally, Appellants argue that the examples in the Specification (e.g., as shown in Figure 2) demonstrate that an unexpected result is achieved when using the claimed crystallization conditions. App. Br. 11. The burden of showing unexpected results rests on the person who asserts them by establishing that the difference between the claimed invention and the closest prior art was an unexpected difference. See In re Klosak, 455 F .2d 1077, 1080 (CCP A 1972). Appellants do not provide any objective evidence that the results of using the claimed crystallization conditions are actually unexpected. An attorney's arguments in a brief cannot take the place of evidence. See In re Schulze, 346 F .2d 600, 602 (CCP A 1965). In addition, the evidence of unexpected results relied upon by Appellants is not reasonably commensurate in scope with the claims. In re Grasselli, 713 F.2d 731, 743 (Fed. Cir. 1983) (concluding that unexpected results "limited to sodium only" were not commensurate in scope with claims to a catalyst having "an alkali metal"). Examples 1-8 were subjected to crystallization at about 170 C for about 24 hours, but the crystallization temperature and time 9 Appeal2015-003629 Application 12/477,826 recited in claim 33 is not so limited and covers crystallizing at a temperature of 165 QC or greater for about 5 minutes to about 350 hours. Appellants have not established that the results obtained at a crystallization temperature of about 170 C for a crystallization time of about 24 hours is representative of the results which would be obtained over the broad scope of crystallization temperatures and times covered by the claims. Nor have Appellants established that the comparative examples, which use a crystallization temperature of 160 QC (Spec. i-f 95), are necessarily representative of Cao' s method, which uses a crystallization temperature of 180 QC (Cao i-f 127). In re Baxter Travenol Labs., 952 F.2d 388, 392 (Fed. Cir. 1991) ("[W]hen unexpected results are used as evidence of nonobviousness, the results must be shown to be unexpected compared with the closest prior art."). Accordingly, based on the totality of the appeal record, including due consideration of Appellant's arguments and evidence, we determine that the preponderance of the evidence weighs most heavily in favor of obviousness of the subject matter recited in claims 33--41 within the meaning of 35 U.S.C. § 103(a). DECISION For the above reasons, the Examiner's rejection of claims 33-35, 37, and 39 under 35 U.S.C. § 103(a) over Cao in view of Davis, and the rejection of claims 36, 38, 40, and 41under35 U.S.C. § 103(a) over Cao in view of Davis, and further in view of Verduijn are affirmed. No time period for taking any subsequent action in connection with this appeal may be extended under 37 C.F.R. § 1.136(a). 10 Copy with citationCopy as parenthetical citation