Longi, In re

Citation225 USPQ 645,759 F.2d 887
Decision Date11 April 1985
Docket NumberNo. 84-1561,84-1561
PartiesIn re Paolo LONGI, et al. Appeal
CourtUnited States Courts of Appeals. United States Court of Appeals for the Federal Circuit

Ellsworth H. Mosher, Stevens, Davis, Miller & Mosher, of Alexandria, Virginia, argued for appellants.

Harris A. Pitlick, Associate Solicitor, of U.S. Patent & Trademark Office, Arlington, Va., argued for appellee. With him on the brief were Joseph F. Nakamura, Sol. and John W. Dewhirst, Associate Sol., Washington, D.C.

Before FRIEDMAN and DAVIS, Circuit Judges, and SKELTON, Senior Circuit Judge.

DAVIS, Circuit Judge.

This is an appeal from a decision of the Patent and Trademark Office Board of Appeals (Board) affirming the examiner's final rejection of appellants' claims 17-34 in application Serial No. 543,520, (January 23, 1975) entitled "Polymerization Catalyst." The Board's affirmance was based upon a holding of obviousness-type double patenting over the claims of three commonly-owned applications, in view of four prior art patents to others. We affirm.

I. BACKGROUND
A. The Application.

Appellants claim certain highly active catalysts used in the polymerization of ethylene. The application discloses that the polymerization of ethylene has been aided by "Ziegler" catalysts which are complexes of transition metal halides (the transition metal being titanium, and the halide being a chloride, for example) with organometallic compounds of metals belonging to Groups I, II, or III of the Periodic Table. The invention claimed in the application relates to a titanium-based Ziegler catalyst obtained by contacting the titanium compound described below, with an anhydrous magnesium dihalide support under conditions such that the compound is preactivated or becomes activated.

Claim 17 is illustrative of the claims on appeal:

Polymerization catalysts obtained by mixing

(A) a catalyst-forming component which is a hydride or organometallic compound of a metal belonging to Groups I to III inclusive of the Mendelyeev Periodic System

with

(B) a catalyst-forming component which is the product obtained by dispersing a titanium compound having the general formula

(NR4 )p Tim X(n.m)+p

in which the Rs represent hydrogen or hydrocarbon radicals; the X(n.m) substituents are halogen atoms or in part OR' groups in which R' is an organic radical; n is the titanium valency and m and p are the whole numbers 1, 2 or 3; on a carrier essentially consisting of an anhydrous magnesium dihalide in an active form characterized in that in its X-rays spectrum the diffraction line of highest intensity that appears in the X-rays spectrum of the normal magnesium dihalide decreases in intensity and in its place a halo appears.

Also claimed is the method of preparing the catalysts and the process of polymerization using the claimed catalysts. It is asserted that unexpected results are obtained when the titanium compound is combined with an activated anhydrous magnesium dihalide which serves as a support for the titanium compound.

B. The Commonly-Owned Applications and Patent

Appellants' application (the applicants are Longi, Giannini and Mazzocchi) has been assigned to Montedison S.p.A., an Italian company based in Milan, Italy. The Galli claims polymerization catalysts obtained by mixing (a) the product obtained by contacting a titanium oxyhalide with a support composed, as in Mayr I, of an anhydrous magnesium dihalide in an active form, with (b) a Group I, II, or III hydride or organometallic compound. As in Mayr I, the dihalide is either preactivated or "cogrinded" with the titanium compound, converting the dihalide to an active form.

                assignee also owns the following related applications:  Serial Nos. 267,624 (Mayr I) (applicants Mayr, Susa, and Giachetti);  524,380 (Galli) (applicants Galli, Susa, Di Drusco); 1  and 622,550 (Mayr II) (applicants Mayr, Susa, and Giachetti).  Mayr I claims polymerization catalysts obtained by mixing a hydride or organometallic compound with a product obtained by contacting a titanium or vanadium halide in which the metal has a valence lower than 4, with an active form of anhydrous magnesium dihalide.  Specifically, catalysts in which the transition metal halide is titanium trichloride (TiCl3  ) are claimed.  Also claimed is the method of preparing the catalyst by cogrinding the titanium halide with an anhydrous magnesium dihalide, thereby converting the dihalide to an active form
                

On November 3, 1981, a patent was granted on the Mayr II application (filed October 14, 1975), entitled "Catalysts for the Polymerization of Olefins," U.S. Patent No. 4,298,718. The Mayr II patent claims a catalyst with an active magnesium dihalide support, obtained in the same manner as claimed in Mayr I and Galli. Here, a titanium tetrahalide (TiCl4 , for example) is combined with the support magnesium dihalide and mixed with a hydride or organometallic compound. Claim 11 is illustrative:

Polymerization catalysts prepared by mixing

(a) a supported catalyst-forming component the essential support material of which is an active magnesium dihalide, said component being obtained by cogrinding a titanium tetrahalide with a normal, non-active anhydrous magnesium dihalide to obtain a component (a) the magnesium dihalide support material of which is activated and characterized in that it has one or both of the following properties (1) its X-rays powder spectrum does not show the most intense diffraction lines as they appear in the X-rays powder spectrum of normal, non-active magnesium dihalide, the spectrum of the activated magnesium dihalide showing a broadening of said most intense diffraction lines; (2) the surface area of the activated magnesium dihalide is greater than 3 m 2/g, with

(b) a hydride or organometallic compound of a metal belonging to one of Groups I to III inclusive of the Mendelyeev Periodic Table. 2

Considered together, the three other applications all claim catalysts obtained by mixing the product of a titanium compound and an activated magnesium dihalide with an organometallic compound. Mayr I claims a catalyst composed in part of a titanium halide with a valence less than 4 (i.e., TiCl3 ); Galli a titanium oxyhalide; and Mayr II a titanium tetrahalide. The application in issue claims catalysts obtained in a similar manner as Mayr I, Galli, and Mayr II, except that a titanium compound with a quaternary nitrogen group (NR4 ) is claimed.

C. The Prior Art

The prior art references relied on by the examiner are:

                Hewett      3,238,146  March, 1966
                Argabright  3,069,446   Dec., 1962
                Luft        2,981,725  April, 1961
                Nowlin      2,918,458   Dec., 1959
                

Hewett's patent, entitled "Catalysts and their Preparation," discloses the use of metal-containing catalysts, including titanium catalysts, for aiding polymerization of unsaturated monomers. The disclosure Nowlin's patent, entitled "Process and Catalyst for Production of Olefin Polymers," discloses the use of a polymerization catalyst comprised of an ammonium radical, a titanium, and a halogen, combined with a hydride or organometallic compound. The disclosed complex metal halide compounds include ammonium chlorotitonate ( (NH4 )2 TiCl6 ). The Argabright patent, entitled "Titanium Halide Derivatives", also teaches that nitrogen-containing titanium halide derivatives combined with an electron donor molecule perform as active catalysts. Thus, all together, the four references disclose that the titanium compounds claimed in the instant and prior applications are well-known components of Ziegler-catalyts.

teaches the use of metal salts such as magnesium chloride, as carriers for the catalysts. Luft's patent, entitled "Process for Polymerizing Olefins," teaches the use of promotors in conjunction with organometallic catalysts to improve the polymerization of ethylene. The use of an inert organic carrier, such as magnesium chloride, for the promotor and catalyst is specifically disclosed as useful in that it increases the accessible surface area of the catalyst, and thus lowers the amount of catalyst required to produce a given quantity of ethylene.

D. The Examiner's Rejection

On February 10, 1981, the examiner finally rejected the claimed subject matter in Longi's application as unpatentable on the ground of estoppel, reasoning that the titanium species claimed were either compounds known to be used in forming Ziegler-type catalysts or were obvious in light of the prior art. The claims were further rejected by the examiner as unpatentable over the claims of Mayr I, Galli and Mayr II in view of Nowlin, Argabright, Hewett and Luft, on the grounds of double patenting. The examiner suggested that the applicants might overcome this rejection by filing a disclaimer or having the patents issue on the same date.

Instead, appellants filed a declaration by Enrico Albizzati, a Montedison biologist researching catalysts used for olefin polymerization, which purports to outline the unexpected results obtained from the applicants' claimed invention. By comparing the results of four tests which he supervised, Albizzati concluded that the "compound (CH3 )4 NTi2 Cl9 [claimed in the instant application] used alone and in not supported form [sic] (Test 2) is a catalytic component having very low activity, as compared to TiCl3 ARA [claimed in Mayr I ] used in Test 3 or TiCl4 [claimed in Mayr II ] used in Test 4." The examiner, however, found the Albizzati declaration unpersuasive and in his final rejection, based on the grounds of estoppel and "obviousness type double patenting," stated:

It is certainly not surprising that the omission of the magnesium dichloride results in a catalyst that is far less active than the analogous catalyst based on titanium tetrachloride or titanium trichloride, i.e., Ziegler-type catalyst based on titanium tetrachloride or titanium trichloride were [sic] known to be more active than those of Nowlin et. al. The catalyst of Nowlin et. al., thus, would be a prime candidate for the activation...

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