Board of Patent Appeals and Interferences
Patent and Trademark Office (P.T.O.)
*1 EX PARTE THOMAS G. ATTIG, KENNETH J. KURUC AND ROBERT K. GRASSELLI
Appeal No. 643-48
August 27, 1986
Application for Patent filed December 27, 1983, Serial No. 566,118. Ammoxidation of N-Butane to Acrylonitrile and Hydrogen Cyanide.
Debra L. Pawl for appellants
Primary Examiner--Joseph P. Brust
Before Sturtevant, Goldstein and Steiner
This is an appeal from the final rejection of all claims in the application, which are claims 1 through 12. Claims 1, 5 and 6 are reproduced here to illustrate the subject matter.
1. A process for the production of acrylonitrile by the ammoxidation of a reactant selected from the group consisting of n-butane, isobutane and propane, the process comprising contacting the gaseous reactant and ammonia with molecular oxygen at a temperature of 300<<degrees>> C to 700<<degrees>> C in the presence of a catalyst having the following formula:
where Ma (zeolite)
M is a Group VIII metal, Cu, Ag, Zn, W, Mo or Cr or oxides thereof;
zeolite is ZSM-5-type aluminosilicate zeolites, or aluminum-free ZSM-5-type zeolites; and
a is a number from 0.0001 to about 0.50.
5. The process of claim 1 wherein zeolite is selected from a group consisting of ZSM-5, ZSM-8, ZSM-11, ZSM-12, ZSM-21 and NU-1.
6. The process of claim 1 wherein zeolite is silicalite.
There are two issues before us on appeal. First is the examiner's rejection of all claims for failure to comply with 35 U.S.C. 112, both the first and second paragraphs. Second is the examiner's rejection of all claims as obvious under 35 U.S.C. 103 in view of prior art. As evidence of obviousness the examiner relies on the following references:
Jones 3,412,134 Nov. 19, 1966
Taylor 3,670,006 June 13, 1972
Taylor 3,670,008 June 13, 1972
Taylor 3,670,009 June 13, 1972
Reulet et al. 3,678,091 July 18, 1972
Chen et al. 3,700,585 Oct. 24, 1972
Argomer et al. 3,702,886 Nov. 14, 1972
Chu 3,709,979 Jan. 9, 1973
Tullman 3,746,737 July 17, 1973
Taylor 3,816,506 June 11, 1974
Rosinski et al. 3,832,449 Aug. 27, 1974
Knox et al. 3,833,638 Sep. 3, 1974
Gelbein 3,925,447 Dec. 9, 1975
Bonacci et al. 3,948,758 Apr. 6, 1976
Whittam et al. 4,060,590 Nov. 29, 1977
Grose et al. 4,061,724 Dec. 6, 1977
O'Rear et al. 4,251,348 Feb. 17, 1981
All of these references were made of record by appellants in their disclosure under 37 CFR 1.56 (paper no. 2) and are cited in their specification, particularly at pages 1, 2 and 4.
After careful review of the record we conclude that the examiner's rejection of the claims under the first paragraph of 35 U.S.C. 112 must be reversed. However, we affirm the rejection under 112, second paragraph, and the rejection under 103.
Before discussing the rejections per se, it is helpful in this instance to discuss briefly some of the patents relied on. The O'Rear et al. patent, as pointed out by appellants in their brief (paragraph bridging pages 3-4), in the claims defines the useful catalyst as 'a ZSM-5-type' and at col. 3, lines 46- 65, describes the ZSM-5-type catalyst as 'exemplified by' the same five ZSM catalysts listed in the Markush group of appeal claim 5. In this same paragraph, the catalyst is said to be usable in either the hydrogen form or in a metal cation form. Among the metals listed as useful are copper, silver and zinc, three of the metals in appeal claim 1. In the Chen et al. patent on the other hand, cited by appellants as teaching the ZSM-8 catalyst, as the paragraph bridging columns 3-4 the 'ZSM-5 type and ZSM-8 type zeolites' are carefully distinguished. Nor is the 8-type treated as within the 5-type zeolite anywhere else in the patent. Note also at column 8, lines 16-32, that well-nigh all the cations named in appeal claim 1 are taught as useful 'in intimate combination with' the zeolites. At column 7, lines 64-65, the Group II metals such as zinc and the Group VIII metals such as nickel are also taught. In the patent on the ZSM-5 family itself (3,702,886) there is this same teaching of utilizing 'replacing metallic cations' from Groups II and VIII (e.g., col. 6, lines 24-28). In patent 3,709,979, ZSM-11 is said to be 'similar to ZSM-5 and ZSM-8' but is distinguished from them (col. 3, lines 34-42). Here also the extensive disclosure of metallic cations found in the Chen et al. patent appears (see col. 3, lines 49-62 and col. 2, lines 60-63). The ZSM-12 patent (Rosinski et al., 3,832,449) speaks of the 'ZSM-12 family' (e.g., col. 5, line 20) but nowhere subsumes this family within the ZSM-5-type of zeolite. See also the same extensive disclosure of metallic cations at the paragraph bridging cols. 3-4. In the patent 3,948,758, cited by appellants as describing ZSM-21, ZSM-11 is clearly identified as within the 'ZSM-5 type,' but ZSM-12, ZSM-21 and zeolite beta are distinguished therefrom (col. 6, lines 8-13). In claim 1 the ZSM-12 and ZSM-21 are separately claimed from the 'type ZSM-5 zeolite.' The silicalite patent 4,061,724 clearly states that this zeolite is 'distinctly different' from the 'ZSM-5 family' (col. 5, lines 26-30). The Nu-1 patent 4,060,590, teaches no relationship of that zeolite to the ZSM series.
*3 This body of zeolite patents is the art that must particularly be considered in deciding the rejection of all the claims under 35 U.S.C. 112. In support of the rejection, the examiner first criticizes the use of the term 'type' in claim 1 as defining the useful zeolites. He then criticizes claims 5 and 6 as improperly dependent on claim 1 since the zeolite of claim 6 and all the zeolites of claim 5 except ZSM-5 itself he considers not to be within the genus of claim 1: 'ZSM-5-type aluminosilicate zeolites or aluminum-free ZSM-5- type zeolites.' It should be apparent from our above discussion of this art that we are in full agreement with the examiner that the 'type' term of claim 1 renders the claims indefinite and that claims 5 and 6 are not properly dependent on claim 1. It is true that the zeolites have been defined in various patents and claimed with the terminology 'ZSM . . . type.' However, clearly the art of record in this case, all of it cited by appellants themselves, in the aggregate serves to render the term indefinite rather than definite. Indeed, the improper dependency of claims 5 and 6 serves to illustrate the confused meaning of 'type' in claim 1 and thus supports the indefiniteness objection.
We cannot agree with the examiner's third and fourth points in support of his 112 rejection. Claim 1 describes the catalysts as having the 'formula' set forth. It is clear from this collection of zeolite patents that associating the metal cation chosen with the zeolite was well within the skill of the art at the time of appellants' invention. (Again see for instance the patent 3,700,585 at col. 8, lines 16-32.) With regard to enablement (first paragraph of 112) we are in agreement with appellants' position as set out in their brief at page 5. Thus we reverse the 112 rejection as based on the first paragraph of the statute section and we affirm the 112, second paragraph rejection on two of the three grounds stated by the examiner.
In support of his 103 rejection of all claims the examiner has cited all 16 of the references listed in his answer, i.e., all of those we have listed except the O'Rear et al. patent. While this may seem at first an undue proliferation of references, on this particular record we are in full agreement with the examiner's application of this art. He relies on the four Taylor patents, Knox et al., Reulet et al. and Tullman as the primary art teaching the same reaction as that of the claims on appeal and as teaching the metals of appeal claim 1, i.e., the useful cations. The group of patents we have hereinbefore discussed is relied on for the teaching of all of the particular zeolites recited in the claims on appeal, albeit in connection with other catalytic reactions. The Jones and Gelbein references are cited for their teachings of zeolites of various types as catalysts in the preparation of nitriles such as appellants' product by appellants' ammoxidation reaction, starting however with unsaturated hydrocarbons. Viewing this large body of prior art as a whole, and comparing it with the claimed subject matter as a whole, we are convinced that the person of average skill in this art at the time of appellants' invention would have found it clearly obvious, and would have been highly motivated, to employ the claimed group of zeolites in the ammoxidation of the claimed saturated hydrocarbons to produce acrylonitrile. As stated for instance in the Knox et al. patent at col. 1, lines 41-47, propane and isobutane are more desirable as starting materials than the corresponding unsaturated hydrocarbons because of their lower cost. The Tullman patent at col. 1, lines 53-59, points to the previous difficulties in the ammoxidation of saturated hydrocarbons. Tullman's solution and that of most of the other primary references, is to choose particular catalysts containing a wide variety of appellants' claimed metals to facilitate the reaction starting from the alkanes. With regard to appellants' argument that no reference teaches the numerous metal-zeolite combinations of the appealed claims (brief, page 6) we need only refer to our previous discussion of the zeolite patents, particularly Chen et al., Rosinski et al. and Chu. Respecting the other major arguments by appellants, we are in agreement with the examiner's response thereto in his answer at pages 5-6.
*4 The examiner's rejection of all claims under 35 U.S.C. 112, second paragraph, and his rejection of all claims under 35 U.S.C. 103 are affirmed. His rejection under 112, first paragraph, is reversed. His decision is affirmed.
Arthur J. Steiner