10204306 (P.T.A.B. Feb. 26, 2013)

Ex Parte Hasenzahl et al

Patent Trial and Appeal BoardFeb 26, 2013

10204306 (P.T.A.B. Feb. 26, 2013)

UNITED STATES PATENT AND TRADEMARK OFFICE 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 APPLICATION NO. FILING DATE FIRST NAMED INVENTOR ATTORNEY DOCKET NO. CONFIRMATION NO. 10/204,306 10/15/2002 Steffen Hasenzahl 032301.306 9698 441 7590 02/26/2013 SMITH, GAMBRELL & RUSSELL 1130 CONNECTICUT AVENUE, N.W., SUITE 1130 WASHINGTON, DC 20036 EXAMINER HOFFMANN, JOHN M ART UNIT PAPER NUMBER 1741 MAIL DATE DELIVERY MODE 02/26/2013 PAPER 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. PTOL-90A (Rev. 04/07) UNITED STATES PATENT AND TRADEMARK OFFICE ____________ BEFORE THE PATENT TRIAL AND APPEAL BOARD ____________ Ex parte STEFFEN HASENZAHL and RALF JANTKE ____________ Appeal 2011-013390 Application 10/204,306 Technology Center 1700 ____________ Before CHUNG K. PAK, LINDA M. GAUDETTE, and KAREN M. HASTINGS, Administrative Patent Judges. PAK, Administrative Patent Judge DECISION ON APPEAL The named inventors (hereinafter “Appellants”)1 appeal under 35 U.S.C. § 134(a) from the Examiner’s final rejection of claims 1 through 12 and 18. We have jurisdiction under 35 U.S.C. § 6(b). STATEMENT OF THE CASE 1 Appellants identify the real party in interest as “EVONIK DEGUSSA GMBH, RELLINGHAUSER STRASSE 1-11, ESSEN, GERMANY 45128.” (See Appeal Brief filed April 1, 2011 (“App. Br.”) at 2-3. Appeal 2011-013390 Application 10/204,306 2 The subject matter on appeal is directed to “a process for the production of a titanium silicalite shaped article.” (Spec. 1, ll. 4-5.) This appealed subject matter is different from the subject matter in Appeal No. 2006-1903 (Application No. 10/204,306), for it is directed to a process rather than a product, i.e., a titanium silicalite shaped article. (See the Decision mailed July 31, 2006 (“Decision”) on Appeal No. 2006-1906, p. 2.) Details of the appealed subject matter are recited in illustrative independent process claims 1 and 8 reproduced below from the “CLAIMS APPENDIX” in the Appeal Brief: 1. Process for the production of a titanium silicalite shaped article comprising: a) preparing a synthesis gel containing a SiO2 source, a TiO2 source selected from the group consisting of tetraalkylorthotitanates and silicon-titanium mixed oxides obtainable by flame hydrolysis of a mixture of SiC14 and TiC14, a template compound and water, b) crystallizing the synthesis gel under hydrothermal conditions to obtain a crystal suspension containing titanium silicalite, c) drying the titanium silicalite from step b) at a temperature below the decomposition temperature of the template compound, Appeal 2011-013390 Application 10/204,306 3 d) preparing a formable mass containing a binder, a paste- forming agent and product from step c), said product being non- calcined and containing said template compound, e) forming of the mass from step d) into a green shaped article, said mass being not yet calcined, f) optionally drying, and g) calcining the green shaped article to thereby remove said template compound, characterized in that the template compound is chosen in a way that the titanium silicalite obtained by step b) exhibits MFI, MEL or p-zeolite structure and the calcination step takes place after the formation of the green shaped article. 8. Process for the production of a titanium silicalite shaped article comprising: a) preparing a synthesis gel containing a SiO2 source, a TiO2 source selected from the group consisting of tetraalkylorthotitanates and silicon-titanium mixed oxides obtainable by flame hydrolysis of a mixture of SiC14 and TiC14, a template compound and water, Appeal 2011-013390 Application 10/204,306 4 b) crystallizing the synthesis gel under hydrothermal conditions to obtain a crystal suspension containing titanium silicalite, c) concentrating the crystal suspension from step b) to form a concentrated crystal suspension, d) preparing a formable mass containing the concentrated crystal suspension from step c) and a binder, e) forming of the formable mass from step d) into a green shaped article, said mass being not yet calcined, f) optionally drying, and g) calcining the green shaped article to thereby remove the template compound, characterized in that the template compound is chosen in a way that the titanium silicalite obtained by step b) exhibits MFI, MEL or β-zeolite structure and the titanium silicalite is not calcined prior to formation of the green shaped article. [(Emphasis added.)] Appellants seek review of the Examiner’s rejection of claims 1 through 12 and 18 under 35 U.S.C. § 103(b) as unpatentable over Giusti 2 in 2 U.S. Patent 4,831,201 issued to Giusti et al. on May 16, 1989. Appeal 2011-013390 Application 10/204,306 5 view of Faraj,3 Smith4, and Parker5 maintained in the Answer mailed May 4, 2011 (“Ans.”). (See App. Br. 6.) As evidence of non-obviousness of the subject matter claimed, Appellants relied upon the following literature: Flanigen, Nature 271:512-516, “Silicalite, A New Hydrophobic Crystalline Silica Molecular Sieve,” (February 9, 1978). Notari, Surf. Sci, Catal., 37:413-425, “Synthesis and Catalytic Properties of Titanium Containing Zeolites,” (1998). U.S. Patent 6,008,389 issued to Grosch et al., (“Grosch”) on December 28, 1999. DISCUSSION Giusti discloses a process for producing a titanium-iron-silicalite shaped article useful as a catalyst for oligomerizing light olefins. (See Abstract and col. 1, ll. 28-58.) Giusti exemplifies preparing and crystallizing a mixture containing a SiO2 source, a TiO2 source, an iron source, and tetrapropylammonium hydroxide (the template compound defined at page 7 of Appellants’ Specification) and water to form a suspension containing titanium-iron-silicalite and then filtering, washing, drying and calcining the resulting titanium-iron-silicalite. (See col. 4, ll. 9- 3 U.S. Patent 5,977,009 issued to Faraj on November 2, 1999. 4 U.S. Patent 5,958,366 issued to Smith et al. on September 28, 1999. 5 U.S. Patent 4,054,510 issued to Parker on October 18, 1977. Appeal 2011-013390 Application 10/204,306 6 32, Example 1, and col. 2, l. 40 to col. 3, l. 21.) The titanium-iron-silicalite can then be “pelletized or extruded according to the techniques known in the art” and then calcined at a temperature of 500o to 600oC. (See col. 3, ll. 17- 38.) Recognizing that the claims on appeal preclude calcination of the titanium-iron-silicalite containing a template compound prior to pelletizing or extruding it, the Examiner states at page 6 of the Answer that: Giusti does not explicitly state that “the material obtained” (col. 3, line 33) has not been calcined, neither does it state that it was calcined…. … See Parker 4054510 (col. 4, lines 8-22) that teaches zeolites are pelleted prior to being calcined. Smith seems to indicate (at col. 6, lines 53-57) that the crystals can be calcined, but that when making an extruded catalysts [(sic.)], it isn’t even necessary to calcine the crystal before forming. Thus[,] it would have been obvious [to] not calcine the crystals prior to forming, especially when they will be eventually calcined when one creates the final (extruded body).” On the other hand, Appellants contend that the collective teachings of Giusti, Parker and Smith would not have led one of ordinary skill in the art to exclude the calcination step for the titanium-iron-silicalite containing a template compound and to pelletize or extrude the uncalcined titanium-iron- silicalite containing a template compound in the process taught by Giusti. (App. Br. 16-21.) In support of this position, Appellants also refer to the disclosures of Grosch, Flanigen, and Notari. (Id.) Appeal 2011-013390 Application 10/204,306 7 Thus, the dispositive question is: Has the Examiner reversibly erred in determining that the collective teachings of Giusti, Parker and Smith would have led one of ordinary skill in the art to extrude or pelletize an uncalcined titanium-iron-silicalite containing a template compound from a crystallization step (without any intermediate calcination) in the process taught by Giusti within the meaning of 35 U.S.C. § 103(a)? On this record, we answer this question in the affirmative. As indicated supra, Giusti teaches filtering, washing, drying and calcining for 4 to 8 hours the titanium-iron-silicalite containing a template compound from a crystallization step, pelletizing or extruding the calcined titanium-iron-silicalite to form a shaped article, and then calcining the titanium-iron-silicalite shaped article. Giusti’s intermediate calcination step, according to column 2, lines 4 7-48 of Grosch relied upon by Appellants at page 19 of the Appeal Brief, is used for removing an organic nitrogen base (the template compound). Both Giusti and Grosch teach employing both the intermediate and final calcination steps in forming their titanium-silicalite shaped articles (catalysts) with their intermediate calcination being used for removing the template compound in their titanium-silicalite zeolite crystals containing such template compound prior to shaping and calcining the resulting shaped titanium-silicalite zeolite article. The Examiner’s reliance on Smith and Parker does not support obviousness of excluding Giusti’s intermediate calcination step for removing Appeal 2011-013390 Application 10/204,306 8 the template compound in the titanium-iron-silicalite zeolite crystals. As correctly stated by Appellants at pages 19 and 20 of the Appeal Brief, Smith’s disclosure relied upon by the Examiner is consistent with the teachings of Giusti in that it teaches employing an intermediate calcination step for removing a template compound from zeolite crystals prior to extruding them. On this record, the Examiner has not identified any teaching in Smith that would have prompted one of ordinary skill in the art to exclude Giusti’s intermediate calcination step for removing the template compound in its titanium-iron-silicalite crystals. Unlike Smith, Parker teaches pelletizing and then calcining the pelletized alumino-silicate zeolite crystals, without any intermediate calcination, as indicated by the Examiner. However, Parker is not directed to silicalite zeolite crystals having a template compound. As correctly indicated by Appellants at page 19 of the Appeal Brief: [T]he zeolites of Parker are not titanium silicalites according to the present invention [and the invention of Giusti]. Instead, the zeolites of Parker are alumino-silicates which are made by a process which does not use a template compound. See col. 3, lines 18 to col. 4, line 7. As no template compound is used [in Parker], calcining to remove the template compound is not required. [(Emphasis original)] In other words, Parker does not teach or suggest excluding Giusti’s intermediate calcination step for removing the template compound in its titanium-iron-silicalite zeolite crystals. Thus, on this record, we are constrained to agree with Appellants that Appeal 2011-013390 Application 10/204,306 9 the Examiner has reversibly erred in determining that the collective teachings of Giusti, Parker and Smith would have led one of ordinary skill in the art to extrude or pelletize the uncalcined titanium-iron-silicalite containing a template compound from a crystallization step in the process taught by Giusti (without any intermediate calcination) within the meaning of 35 U.S.C. § 103(a).6 ORDER Upon consideration of the record, and for the reasons given above, it is ORDERED that the decision of the Examiner rejecting claims 1 through 12 and 18 under 35 U.S.C. § 103(a) as unpatentable over Giusti in view of Faraj, Smith, and Parker is REVERSED. REVERSED tc 6 Since we determine that the Examiner has not established a prima facie case of obviousness regarding the claimed subject matter, we need not reach the issue of the sufficiency of the Rule 132 declarations of record. In re Geiger, 815 F.2d 686, 688 (Fed. Cir. 1987).