Ex Parte Bull et alDownload PDFPatent Trials and Appeals BoardMar 25, 201912612142 - (D) (P.T.A.B. Mar. 25, 2019) Copy Citation UNITED STA TES p A TENT AND TRADEMARK OFFICE APPLICATION NO. FILING DATE 12/612,142 11/04/2009 109171 7590 03/27/2019 WOMBLE BOND DICKINSON (US) LLP Attn: IP Docketing P.O. Box 7037 Atlanta, GA 30357-7037 FIRST NAMED INVENTOR Ivor Bull 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. B248 2260US.l (0108.4) 3835 EXAMINER DA VIS, SHENG HAN ART UNIT PAPER NUMBER 1732 NOTIFICATION DATE DELIVERY MODE 03/27/2019 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): IPDocketing@wbd-us.com PTOL-90A (Rev. 04/07) UNITED STATES PATENT AND TRADEMARK OFFICE BEFORE THE PATENT TRIAL AND APPEAL BOARD Ex parte IVOR BULL, AHMAD MOINI, and MUKTA RAI Appeal2018-002220 Application 12/612, 142 Technology Center 1700 Before BRADLEY R. GARRIS, KAREN M. HASTINGS, and MICHAEL P. COLAIANNI, Administrative Patent Judges. COLAIANNI, Administrative Patent Judge. DECISION ON APPEAL Appeal2018-002220 Application 12/612, 142 Appellants 1 appeal under 35 U.S.C. § 134 the final rejection of claims 1, 4, 5, 8-13, 15-23, 28, and 29. We have jurisdiction over the appeal pursuant to 35 U.S.C. § 6(b ). We AFFIRM. Appellants' invention is directed to a selective catalytic article that includes zeolites that have a chabazite (CHA) crystal structure. (Claim 1; Spec. ,r 3). Claim 1 is illustrative: 1. A selective catalytic reduction catalytic article comprising a natural or synthetic aluminosilicate zeolite, the zeolite having exchange sites and a CHA crystal structure and the zeolite promoted at the exchange sites with one or more metal cations selected from iron, copper and combinations thereof, the zeolite being disposed on a substrate, the article effective to reduce NOx in exhaust streams from diesel and gasoline engines, wherein the zeolite has a mole ratio of silica to alumina of less than 15 and has an alkali content of less than about 0.5 weight percent, and wherein the catalytic article exhibits the selective catalytic reduction ofNOx with ammonia exceeding at least about 50% in exhaust gas streams at 250° C. Appellants appeal the following rejections: 1. Claims 1, 4, 5, 8, and 29 are rejected under 35 U.S.C. § 103 as unpatentable over Maeshima (US 4,046,888, issued Sept. 6, 1977) in view of Maher (US 3,402,996, issued Sept. 24, 1968), Famos (US 5,589,147, issued Dec. 31, 1996), and Ward (US 3,945,943, issued Mar. 23, 1976). 1 The Appeal Brief on page 1 indicates that "BASF Corporation" is the assignee of record. 2 Appeal2018-002220 Application 12/612, 142 2. Claim 9 is rejected under 35 U.S.C. § 103 as unpatentable over Maeshima in view of Maher, Famos, Ward, and further in view of Hubig (US 2007/0081934 Al, published Apr. 12, 2007). 3. Claim 10 is rejected under 35 U.S.C. § 103 as unpatentable over Maeshima in view Maher, Famos, Ward and in further view of Li '095 (US 2009/0048095 Al, published Feb. 19, 2009) and Li '362 (US 2010/0092362 Al, published Apr. 15, 2010). 4. Claims 11, 12, 13, 17, 18, 19, and 23 are rejected under 35 U.S.C. § I03(a) as unpatentable over Maeshima in view of Maher, Famos, Ward, and Beutel (US 2008/0045405 Al, published Feb. 21, 2008). 5. Claims 15, 16, 28, and 29 are rejected under 35 U.S.C. § I03(a) as unpatentable over Maeshima in view of Maher, Famos, Ward, and in further view ofHubig, and Gaffney (EP 0391351 A2, published Oct. 10, 1990). 6. Claims 20 and 22 are rejected under 35 U.S.C. § I03(a) as unpatentable over Maeshima in view of Maher, Famos, Ward, Beutel, and further in view of Wei (US 2009/0031710 Al, published Feb. 5, 2009). 7. Claim 21 is rejected under 35 U.S.C. § I03(a) as unpatentable over Maeshima in view of Maher, Famos, Ward, Beutel, Wei, and Long (R.Q. Long et al., "Selective Catalytic Oxidation (SCO) of Ammonia to Nitrogen over Fe-Exchanged Zeolites" J. of Catalysis 201, 145-152 (2001)). [ Appellants' arguments focus on the subject matter of claim 1 only (App. Br. 3-17). Any claim not argued separately will stand or fall with our analysis of the rejection of claim 1. 3 Appeal2018-002220 Application 12/612, 142 FINDINGS OF FACT & ANALYSIS The Examiner's findings and conclusions with respect to claim 1 are located on pages 7 to 9 of the Final Action. The Examiner finds that Maeshima discloses a selective catalyst reduction (SCR) catalyst made of aluminosilicate obtained by exchanging an alkali metal ion with a metal for the reduction ofNOx (Final Act. 7). The Examiner finds that Maeshima discloses that the metal can be iron or copper and the silica to alumina ratio (SAR) is 2 or more (Final Act. 7). The Examiner finds that Maeshima teaches that the zeolite can have a chabazite crystal structure (Final Act. 7). The Examiner finds that Maeshima does not teach the following: 1) the alkali content is less than 0.5 wt. %, 2) the zeolite is disposed on a substrate, 3) the zeolite is used in a gasoline or diesel engine, and 4) the NOx reduction when ammonia is used is at least 50% in the exhaust gas stream at 250°C (Final Act. 7). The Examiner finds that Maher discloses reducing sodium ion concentrations in an ion exchange zeolite using ammonium exchange (Final Act. 7). The Examiner finds that the level of sodium in the zeolite can be reduced to below 0.5% (Final Act. 7). The Examiner finds that Ward teaches improving zeolite aluminosilicate catalysts that may be used in a denitrification reaction by lowering the alkali metal levels to as low as 0.5% to enhance thermal stability and tolerance to high temperatures (Final Act. 7-8). The Examiner concludes that it would have been obvious to reduce the sodium levels to below 0.5 wt.% as taught by Maher by performing additional exchange steps because Ward teaches that reduced sodium levels improve hydrothermal stability and tolerance to high temperatures (Final Act. 8). 4 Appeal2018-002220 Application 12/612, 142 The Examiner finds that Famos discloses a SCR catalyst usable in an engine that is coated on a substrate and can be a natural zeolite (Final Act. 8). The Examiner further finds that the engine in Famos would have been either gasoline or diesel as they are standard in the art (Final Act. 8). The Examiner concludes that it would have been obvious to coat the catalyst on a substrate for use in a gasoline or diesel engine, as taught by Famos, for use with Maeshima, Maher and Ward because it is known to coat SCR catalysts on a substrate for use with engines to reduce NOx in these exhaust gas streams (Final Act. 8-9). The Examiner finds that because the catalysts are the same it is reasonable to expect that each catalyst has the same NOx reducing property (Final Act. 9). Appellants argue that they surprisingly discovered that chabazite (CHA) zeolite materials exhibit strong ammonia SCR activity even after hydrothermal aging (App. Br. 6). Appellants contend that the declaration of one of the present inventors, Ahmad Moini (hereinafter "Moini Declaration"), is evidence that one of ordinary skill in the art would not have used a chabazite catalyst with a SAR ( silica to alumina ratio) below 15 (App. Br. 6). Appellants argue that as explained in the Moini Declaration, the patent to Bull (US 7,601,662) and the pre-grant publication to Li '060 (US 2008/0241060) each demonstrate that one of ordinary skill in the art would not have used a chabazite zeolite with a SAR less than 15 (App. Br. 6). Appellants contend that Bull and Li '060 teach away from using chabazite zeolites having a SAR below 15 due to the instability of the lower SAR catalysts at high temperatures ( e.g., 700°C) found in exhaust gases (App. Br. 6). Appellants contend that Bull and Li '060 teach away from chabazite catalysts with SAR values below 15 in ammonia applications and 5 Appeal2018-002220 Application 12/612, 142 instead teach to use chabazite catalysts with a preferred SAR range from 25 to 40 (App. Br. 6, 7). Appellants contend that Li teaches that the "low-silica chabazite" with a SAR of 6.3 as shown in Table 1 was largely destroyed after aging at 700°C due to the precipitous drop in surface area of the catalyst (App. Br. 7). Regarding Maeshima, Appellants argue that Maeshima contains a broad disclosure for aluminosilicates having a SAR of 2 or greater but Maeshima does not teach specifically that chabazites should have a SAR value of 2 or greater (App. Br. 8-9). Appellants argue that Maeshima's disclosure is directed to faujasite/zeolite frameworks with a SAR below 15, not to chabazite zeolites (App. Br. 9). Appellants contend that Famos teaches that exhaust gas temperatures can be as high as 1000°C and Maeshima's upper temperature limit for the zeolite catalysts is half the temperature disclosed by Famos (i.e., 500°C) (App. Br. 10). Appellants argue that one of ordinary skill in the art would have been aware of the problems associated with using chabazite zeolites with low SAR values at high temperatures and would not have used Maeshima's chabazite zeolite in an exhaust gas system as taught by Famos (App. Br. 10). These arguments are not persuasive of reversible error. Although claim 1 recites the intended use for the catalyst article in exhaust streams from diesel and gasoline engines, claim 1 does not recite any particular temperature of the exhaust gases. Appellants contend that Famos teaches that exhaust gases may have a temperature as high as 1000°C, but Famos also teaches that the exhaust gases may be as low as 200°C, which overlaps with the temperature range disclosed by Maeshima (Famos col. 4, 11. 40-42; Maeshima col. 3, 11. 23-25). Maeshima discloses 6 Appeal2018-002220 Application 12/612, 142 treating exhaust gas maintained at a temperature of 200 to 500°C with ammonia and a zeolite to reduce NOx (Maeshima col. 2, 11. 47-50). Maeshima further discloses that the exhaust gas temperature is adjusted to a temperature of 200 to 500°C and discloses using an economizer ( e.g., a heat exchanger) to achieve the desired exhaust gas temperature (Maeshima, col. 2, 11. 48-53; col. 7, 11. 20-23). Maeshima provides means to maintain and achieve the desired exhaust gas temperature. Claim 1 uses the open-ended transitional claim language comprising and so does not exclude using Maeshima's economizer to maintain the desired exhaust gas temperature. Maeshima' s teaching to maintain the exhaust temperature between 200 and 500°C undercuts Appellants' argument that Bull and Li teach away from using chabazite zeolites in high temperature exhaust gas. Bull teaches that at temperatures higher than 500°C the activity of metal-promoted zeolites begins to decline (col. 1, 11. 35-38). Appellants allege that Li '060 shows that Comparative Example 1 that uses low-SAR chabazite zeolites having a SAR of 6.3 is destroyed after hydrothermal aging at 700°C because the surface area drops precipitously (App. Br. 6). The nature of Bull and Li '060's disclosures do not teach away from using chabazite zeolites with a low-SAR in Maeshima. In re Gurley, 27 F.3d 551, 553 (Fed. Cir. 1994) ("Although a reference that teaches away is a significant factor to be considered in determining unobviousness, the nature of the teaching is highly relevant, and must be weighed in substance."). Rather, teachings in Maeshima, Bull and Li '060 would have suggested cooling the exhaust gas to within a temperature range of 200 to 500°C before treating with zeolite that may include chabazite zeolites encompassed by the claim. As noted 7 Appeal2018-002220 Application 12/612, 142 above, claim 1 does not exclude using a heat exchanger to control the exhaust gas temperature. Maeshima may include a broad disclosure of suitable zeolites having a SAR of 2 or more. Nevertheless, Maeshima discloses zeolites having a chabazite crystal structure and a SAR of 2 to 6. Maeshima's disclosure is not limited to the preferred embodiments that use the faujasite zeolites. All of Maeshima's disclosures, including the non-preferred embodiments, must be considered. In re Lamberti, 545 F.2d 747, 750 (CCPA 1976). Appellants argue that Maher, Gaffney and Hubig are non-analogous art (App. Br. 11-12). Appellants contend that the field of Appellants' endeavor is selective catalytic reduction (SCR) catalytic articles and exhaust gas treatment systems and methods using such catalytic articles to reduce NOx in a gas stream (App. Br. 11-12). Appellants argue that Gaffney is directed to zeolites used in a completely different field of use (i.e., removal of trace gases from argon) (App. Br. 12). Appellants contend that Ward's denitrogenation disclosure would not be understood by one of ordinary skill in the art to refer to SCR reactions for use in treating exhaust gas streams but rather another form of hydrocarbon conversion (App. Br. 12). Appellants argue that Ward is directed to hydrogenative hydrocarbon conversion, which is not a SCR reaction to reduce NOx species in an exhaust gas (App. Br. 13). Appellants contend that Maher is directed to the same general field as Ward, hydrocarbon conversion, which is non-analogous to the field of endeavor of the claimed invention (App. Br. 13). Appellants contend that neither Ward, Maher, nor Gaffney is reasonably pertinent to Appellants' problem (App. Br. 14). Appellants argue that the problem solved by their invention is enabling use of a low SAR 8 Appeal2018-002220 Application 12/612, 142 chabazite material to reduce efficiently NOx in a gaseous exhaust stream via a SCR reaction under hydrothermal conditions (App. Br. 14). Appellants contend that Gaffney is not directed to NOx reduction reactions of any kind (App. Br. 14). Appellants argue that Ward and Maher are directed to hydrocarbon conversion processes not NOx reduction of an exhaust gas stream using SCR reaction (App. Br. 14). Prior art is considered analogous if it is either ( 1) from the same field of endeavor, regardless of problem addressed, or (2) if not from the same field of endeavor the reference still is reasonably pertinent to the particular problem with which the inventor was involved. In re Clay, 966 F.2d 656, 659 (Fed. Cir. 1992). The Supreme Court directs us to construe the scope of analogous art broadly, stating "familiar items may have obvious uses beyond their primary purposes, and a person of ordinary skill often will be able to fit the teachings of multiple patents together like pieces of a puzzle." Wyers v. Master Lock Co., 616 F.3d 1231, 1238 (Fed. Cir. 2010) citing KSR Int'! Co. v. Teleflex, Inc., 550 U.S. 398, 402 (2007). The Specification describes the "technical field" as chabazite zeolite catalysts, methods for their preparation, and their use in exhaust gas treatment systems (Spec. ,r 3). Claim 1 is directed to a selective catalytic reduction catalytic article comprising a natural or synthetic aluminosilicate zeolite, the zeolite having exchange sites and a chabazite crystal structure having a ratio of silica to alumina (SAR) less than 15 and an alkali content of less than about 0.5 weight percent with the intended use of the catalytic article to reduce NOx in exhaust systems of diesel and gasoline engines. Claim 1 further recites a property of the catalytic article where the article exhibits the selective catalytic reduction ofNOx with ammonia exceeding at 9 Appeal2018-002220 Application 12/612, 142 least about 50% in exhaust gas streams at 250°C. Based on claim 1 and the Specification, the field of endeavor is broadly directed to chabazite zeolite catalysts that may be used to treat exhaust gas. A chabazite zeolite catalyst possessing the same structure and composition as recited in claim 1 would reasonably be expected to have the recited property. In other words, the field of endeavor includes zeolites generally including the chabazite crystal structure with a SAR less than 15 and alkali content of less than 0.5% and their use in exhaust systems with the attendant property being a characteristic of the zeolite. Based on these findings regarding the field of endeavor, we find that Maher, Gaffney, and Ward are in the same field of endeavor. All three references are concerned with zeolite catalysts and their use in catalyzing nitrogen removal. Gaffney is directed to chabazite zeolites and improving adsorption of nitrogen in the zeolite (Gaffney 2:4--6). Although Appellants argue that one of ordinary skill in the art would not find Gaffney useful in selecting zeolite material for SCR processes (Reply Br. 5) that argument is premised on the erroneous argument that the field of endeavor is limited solely to ammonia-SCR processes. Ward is directed to crystalline aluminosilicate zeolite catalysts that may be used in denitrogenation reactions ( col. 6, 1. 45). Appellants contend that Ward's denitrogenation is directed to a hydrocarbon conversion reaction, not SCR using ammonia (Reply Br. 5). Appellants' argument is not persuasive because Ward's denitrogenation would still include removing nitrogen from the hydrocarbon. Moreover, Ward teaches that the aluminosilicate zeolites have better thermal stability in basic environments including "ammoniacal solutions" or ammonia atmospheres (Ward, col. 6, 11. 10 Appeal2018-002220 Application 12/612, 142 10-20). Additionally, Ward is also reasonably pertinent to Appellants' problem of improving thermal stability of aluminosilicate zeolites, including chabazite zeolites, by, inter alia, reducing the alkali content of the zeolite. Maher is directed to improving the thermal stability of aluminosilicate zeolites which would appear to be in a similar field of endeavor as Appellants' chabazite zeolite. Nevertheless, Maher appears to be reasonably pertinent to Appellants' problem of improving the thermal stability of aluminosilicate zeolites. Maher teaches improving the thermal stability in aluminosilicate zeolites by reducing the sodium ion concentration ( col. 1, 11. 45-50). Appellants question the Examiner's reliance on Ward for teaching that reducing sodium levels improve thermal stability of the zeolite (App. Br. 14). The Examiner provides multiple citations to Ward where it is taught to reduce alkali metal levels and that so doing produces a zeolite with improved thermal stability (Final Act. 7-8). Appellants do not specifically show error with the Examiner's finding regarding Ward's teaching to reduce alkali metal content of the zeolite. Maher teaches reducing sodium in zeolites improves thermal stability (col. 1, 11. 45-50). In other words, the combined teachings of the references would have suggested reducing the sodium content of a zeolite to improve thermal stability of the zeolite. Appellants contend that the Moini Declaration explains that the evidence in the Specification establishes that it was surprising and unexpected that by reducing the sodium content of the chabazite zeolite with a silica to alumina ratio (SAR) of less than 15 would have good hydrothermal stability for use in treating exhaust gas (App. Br. 15). Appellants contend that as shown in Li '060 the low-silica chabazite zeolite 11 Appeal2018-002220 Application 12/612, 142 with a SAR of 6.3 is completely destroyed after aging at 700°C (App. Br. 16). Although Appellants allege that evidence in the Specification establishes unexpected results, no evidence in the Specification has been cited or explained by Appellants. The Moini Declaration in paragraph 8 refers to "experimental results set forth in the present application" but does not direct us to the specific evidence or explain such evidence. Moreover, Appellants have not compared the claimed invention with the closest prior art (i.e., Maeshima). Appellants' argument of unexpected results is premised on the low SAR chabazite catalyst being destroyed when used in a high temperature exhaust gas (App. Br. 16). Claim 1, however, does not require any temperature for the exhaust gas. As noted earlier in this decision, Maeshima's economizer to lower the exhaust gas temperature to a temperature between 200 and 500°C is not excluded by claim 1. Appellants' Moini Declaration is not sufficient to overcome strong evidence of obviousness provided by the Examiner. On this record, we affirm the Examiner's § 103 rejection over Maeshima in view of Maher, Famos and Ward. We further affirm the Examiner's § 103 rejections (2) to (7) for the same reasons. DECISION The Examiner's decision is 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). See 37 C.F.R. § 1.136(a)(l )(iv). AFFIRMED 12 Copy with citationCopy as parenthetical citation