Application of Best

• Decision Date: 13 October 1977
• Docket Number: Patent Appeal No. 77-509.
• Citation: 562 F.2d 1252
• Court: U.S. Court of Customs and Patent Appeals (CCPA)
• Parties: APPLICATION OF DONALD FRANCIS BEST, Anthony Peter Bolton and Herbert Charles Shaw.

562 F.2d 1252

APPLICATION OF DONALD FRANCIS BEST, Anthony Peter Bolton and Herbert Charles Shaw.

Patent Appeal No. 77-509.

United States Court of Customs and Patent Appeals.

October 13, 1977.

Richard G. Miller, New York City, attorney of record, for appellants, James C. Arvantes, Arlington, Va., of counsel.

Joseph F. Nakamura, Washington, D. C., for the Commissioner of Patents, Gerald H. Bjorge, Washington, D. C., of counsel.

Before MARKEY, C. J., RICH, BALDWIN and LANE, JJ., and FORD, J., United States Customs Court.

MARKEY, Chief Judge.

Appeal from the decision of the Patent and Trademark Office (PTO) Board of Appeals (board) sustaining rejections of claims 1-7 under 35 U.S.C. § 102 or 35 U.S.C. § 103, and claims 3-7 under 35 U.S.C. § 112, of appellants' application serial No. 347,216, filed April 2, 1973, for "Catalyst for Hydrocarbon Conversion Processes and Process for Preparing Same."¹ We affirm.

The Invention

The invention relates to zeolitic molecular sieve catalyst compositions useful in hydrocarbon conversion and to a process for producing them. Claim 1 is illustrative of the product claims:

1. A crystalline zeolitic aluminosilicate having a SiO2/A12O3 molar ratio of from 4.6 to 5.4, a face centered cubic unit cell having an ao of greater than 24.45 to 24.55A, an Na2O/A12O3 molar ratio of not greater than 0.25, an adsorptive capacity in the dehydrated state for oxygen of at least 26 weight per cent at 100 mm Hg oxygen pressure and %ao183°C., an ion exchange capacity of from 0.15 to 0.35 and having the essential X-ray powder diffraction pattern of zeolite Y with the proviso that the d-spacing thereof having the Miller Indices 331 is at least as great in intensity as the line thereof having the Miller Indices 533.

Claim 3 is illustrative of the process claims:

3. Process for preparing a hydrolytically-stable zeolitic aluminosilicate which comprises providing an ion-exchanged zeolite Y having the following composition in terms of mole ratios of oxides

0.75 %ao 0.9(A)2O: 0.1 %ao 0.25 Na2O: A12O3: 4.6 %ao 5.4 SiO2: yH2O

wherein "A" represents H+ or NH4+ or a mixture thereof, and wherein y has a value of from zero to nine, heating the zeolite at a temperature between 550°C. and 800°C. for a period of at least 0.25 hours in an inert atmosphere comprising sufficient steam to prevent dehydroxylation of the zeolite, removing at least a major proportion of any ammonia generated by the heated zeolite from contact with the zeolite, and cooling the steamed zeolite to a temperature below 350°C. at a rate sufficiently rapid that the cooled zeolite exhibits an X-ray powder diffraction pattern having the d-spacing corresponding to the Miller Indices, hkl, of 331 at least as strong in intensity as that corresponding to the Miller Indices 533, prior to any post-steaming ion exchange treatment.

Claim 2 is restricted to a zeolite of claim 1 with a Na2O/A12O3 molar ratio of less than 0.038. Claims 4-7 add further process restrictions as to starting materials or process steps. All of the claims stand or fall with claims 1 and 3.

As recognized in the prior art, crystalline zeolitic aluminosilicates with high concentrations of sodium cations do not make good hydrocarbon conversion catalysts. For this reason sodium cations are replaced with non-metallic cations such as hydrogen or ammonium. The hydrogen or ammonium cations are removed by calcination, producing a decationized zeolite. Such decationized zeolites have poor hydrothermal stability, i. e., they lose their crystallinity upon reheating after contact with water.

The process of appealed claims 3-7 is a stabilization procedure for such low-sodium zeolites wherein a thermal treatment in the presence of steam is followed by a particular cool-down step. The zeolitic compositions of claims 1-2 represent the products of the claimed process.

                The 102/103 Rejections
                  The references relied upon were
                  Maher et al. (Maher)           3,293,192    Dec. 20, 1966
                  Hansford                       3,354,077    Nov. 21, 1967
                  McDaniel et al. (McDaniel)     3,449,070    June 10, 1969
                  Kerr et al (Kerr I)            3,493,519    Feb.  3, 1970
                  Kerr (Kerr II)                 3,513,108    May  19, 1970
                

All claims were rejected under 35 U.S.C. § 102 or 35 U.S.C. § 103 as unpatentable over Hansford. Claims 1-2 were additionally rejected in view of each of Maher, McDaniel, Kerr I, and Kerr II.²

Hansford discloses a method for producing a hydrothermally stable Y-sieve zeolite composition by calcining an ammonium zeolite Y for 2 or more hours in an atmosphere containing water vapor at a temperature of from 700°F to 1200°F (338°C-649°C). The starting material is disclosed by Hansford as having a SiO2/A12O3 molar ratio of 4 to 6 and a reduced Na2O content of 0.6% to 2.5% by weight (appellants claim 0.1 %ao 0.25 Na2O/A12O3 molar ratio and disclose 2.48% by weight in example 10 of their specification). In rejecting claims 1-7 on Hansford, the examiner asserted that a major portion of any ammonia generated during calcination would inherently be removed from contact with the zeolite, because the gaseous atmosphere disclosed by Hansford was in the form of a moving stream. Also with respect to Hansford, the examiner believed the cooling rate of the zeolite after stabilization to be within the terms of the appealed process claims. The claimed product being the unique result of the claimed process, the examiner, therefore, rejected both process and product claims as anticipated by Hansford, or, in any case, as obvious in view of Hansford.

In sustaining the rejection, the board added its view of Hansford.

All the positive process limitations are expressly disclosed except for the functionally expressed rate of cooling. However, there is nothing to indicate that this rate of cooling in any way differs from the normal rate resulting from removal of the heat source. Thus, the examiner's conclusion that those parameters of the resultant product which are recited in the appealed claims but are not expressly disclosed in the reference would be inherent is a reasonable one, absent convincing evidence to the contrary. Appellants have presented no such convincing evidence. No comparison has been made between appellants' process and product and the process and product disclosed in the Hansford patent. The comparative data contained in appellants' specification and in an affidavit under 37 CFR 1.132 do not relate to the reference but merely illustrate the result of deviating from appellants' process. Such deviations appear to be also outside the scope of the Hansford teaching.

OPINION

I. The Process Claims

The appellants urge that, because Hansford is silent on appellants' crucial cool-down step and on his apparatus, a direct comparison between the claimed process and that of Hansford is impossible. Appellants correctly state that indirect comparisons, based on established scientific principles, can validly be applied to distinguish a claimed chemical process or product from that disclosed in the prior art. In re Blondel, 499 F.2d 1311, 182 USPQ 294 (CCPA 1974). However, our analysis of the comparative data offered by appellants convinces us that the burden of rebutting the PTO's reasonable assertion of inherency under 35 U.S.C. § 102, or of prima facie obviousness under 35 U.S.C. § 103, has not been met.

Our reading of Hansford leads us to conclude, as did the board, that all process limitations of claim 3 are expressly disclosed by Hansford, except for the functionally expressed rate of...