DETAILED ACTION
Notice of Pre-AIA or AIA Status
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
Continued Examination Under 37 CFR 1.114
A request for continued examination under 37 CFR 1.114, including the fee set forth in 37 CFR 1.17(e), was filed in this application after final rejection. Since this application is eligible for continued examination under 37 CFR 1.114, and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114. Applicant's submission filed on 3/23/2026 has been entered.
Response to Arguments
Applicant's arguments filed 3/23/2026 have been fully considered but they are not persuasive.
Regarding claims 1-2, 4-5, 7-17, 20, 26-28, 34-35, 50, 55, and 57-58, Applicant argues in the Remarks at Page 15 that the combination of cited references does not teach or suggest where the first acid is a halogen acid. This argument is unpersuasive since Scadden is cited for teaching a first acid comprising HCl for oxidizing and dissolving Mo metal to form molybdate.
Regarding claims 18-19, 21-25, 29-30, 39-40, 42-45, 47-49 and 73, Applicant argues that Monroy-Guzman teaches away from the claimed invention because Monroy-Guzman teaches post-irradiation of his synthesized gel product. This argument is unpersuasive because Monroy-Guzman is relied upon only for teaching the use of a titanium chloride salt for forming a molybdate where Varnadoe and Evans are silent with respect to suitable salts. Furthermore, modification of the process according to Varnadoe and Evans with titanium chloride would not render the titanium molybdate unsatisfactory for its intended purpose since both Varnadoe and Evans suggest the processes that can be used having irradiated molybdenum compound or non-radioactive molybdenum compound (see Varnado, Page 1 and Evans, Abstract). Even if Monroy-Guzman suggests that titanium molybdate avoid special equipment for synthesis of radioactive material and reduced process time, Monroy-Guzman does not teach that using titanium chloride salt would be incompatible to form a pre-irradiated molybdate. Therefore, the Office maintains that the process for producing titanium molybdate comprising titanium chloride would still have been obvious. Shafiq et al (CHARACTERISTICS AND BEHAVIOR OF A 99Mo/99mTc GENERATOR USING IRRADIATED TITANIUM MOLYBDATE AS COLUMN MATRIX, J. RADIOANAL.NUCL.CHEM., LETTERS 199 (3) (1995) 173-181) is also prior art pre-dating Monroy-Guzman by twelve years and teaches the precipitation of titanium molybdate for a Tc generator using titanium chloride that neither states any benefits for post-irradiation of the molybdate nor criticizes a pre-irradiated molybdenum compound.
Regarding Applicant’s arguments with respect to claims 3 and 72, the argument is unpersuasive since Monroy-Guzman is cited for teaching titanium chloride to form titanium molybdate. Furthermore, the arguments that Monroy-Guzman teaches away from the invention are unpersuasive for the same reasons given above.
Regarding Applicant’s arguments with respect to claims 6 and 53, the argument is unpersuasive since Scadden is cited for teaching a halogen acid and Monroy-Guzman is cited for teaching titanium chloride to form titanium molybdate.
Regarding Applicant’s arguments with respect to claims 31-33 and 38 the argument is unpersuasive since Scadden is cited for teaching a halogen acid and Monroy-Guzman is cited for teaching titanium chloride to form titanium molybdate.
Regarding Applicant’s arguments with respect to claims 36-37 the argument is unpersuasive since Scadden is cited for teaching a halogen acid and Monroy-Guzman is cited for teaching titanium chloride to form titanium molybdate.
Regarding Applicant’s arguments with respect to claim 41 the argument is unpersuasive since Scadden is cited for teaching a halogen acid and Monroy-Guzman is cited for teaching titanium chloride to form titanium molybdate. Furthermore, the arguments that Monroy-Guzman teaches away from the invention are unpersuasive for the same reasons given above.
Regarding Applicant’s arguments with respect to claim 46 the argument is unpersuasive since Scadden is cited for teaching a halogen acid and Monroy-Guzman is cited for teaching titanium chloride to form titanium molybdate. Furthermore, the arguments that Monroy-Guzman teaches away from the invention are unpersuasive for the same reasons given above.
Regarding Applicant’s arguments with respect to claims 73-74 and 77-78 the argument that Monroy-Guzman teaches away from the invention are unpersuasive for the same reasons given above.
Regarding Applicant’s argument with respect to claim 79, the argument is unpersuasive as not being addressed since claim 79 is the independent claim.
In response to applicant's argument that the examiner has combined an excessive number of references, reliance on a large number of references in a rejection does not, without more, weigh against the obviousness of the claimed invention. See In re Gorman, 933 F.2d 982, 18 USPQ2d 1885 (Fed. Cir. 1991). Here, the Office maintains that this claim is the mere collection of known and obvious elements as supported by the cited references. For example, the current amendment to a “solid” target for irradiation is the mere addition of a limitation to something unstated in the previously cited references but is a well-known and obvious technique for irradiating a molybdenum metal target as supported by Wilson (US 20140029710).
Regarding Applicant’s arguments with respect to claims 80-82 the argument that Monroy-Guzman teaches away from the invention are unpersuasive for the same reasons given above.
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(b):
(b) CONCLUSION.—The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the inventor or a joint inventor regards as the invention.
The following is a quotation of 35 U.S.C. 112 (pre-AIA ), second paragraph:
The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the applicant regards as his invention.
Claim 4 is rejected under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), second paragraph, as being indefinite for failing to particularly point out and distinctly claim the subject matter which the inventor or a joint inventor (or for applications subject to pre-AIA 35 U.S.C. 112, the applicant), regards as the invention.
Claim 4 contains the limitation wherein the first acid is selected from the group consisting of hydrochloric acid, nitric acid, sulfuric acid, and combinations thereof. The scope of this claim is indefinite since claim 1 which it depends on states that the first acid is a halogen acid while nitric acid and sulfuric acid are not halogen acids.
The following is a quotation of 35 U.S.C. 112(d):
(d) REFERENCE IN DEPENDENT FORMS.—Subject to subsection (e), a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
The following is a quotation of pre-AIA 35 U.S.C. 112, fourth paragraph:
Subject to the following paragraph [i.e., the fifth paragraph of pre-AIA 35 U.S.C. 112], a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
Claim 4 is rejected under 35 U.S.C. 112(d) or pre-AIA 35 U.S.C. 112, 4th paragraph, as being of improper dependent form for failing to further limit the subject matter of the claim upon which it depends, or for failing to include all the limitations of the claim upon which it depends. Claim 4 contains the limitation wherein the first acid is selected from the group consisting of hydrochloric acid, nitric acid, sulfuric acid, and combinations thereof. The claim therefore expands the scope of claim 1 which limits the first acid to a halogen acid while nitric acid and sulfuric acid are not halogen acids. Applicant may cancel the claim(s), amend the claim(s) to place the claim(s) in proper dependent form, rewrite the claim(s) in independent form, or present a sufficient showing that the dependent claim(s) complies with the statutory requirements.
Claim Rejections - 35 USC § 103
The following is a quotation of 35 U.S.C. 103 which forms the basis for all obviousness rejections set forth in this Office action:
A patent for a claimed invention may not be obtained, notwithstanding that the claimed invention is not identically disclosed as set forth in section 102, if the differences between the claimed invention and the prior art are such that the claimed invention as a whole would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to which the claimed invention pertains. Patentability shall not be negated by the manner in which the invention was made.
The factual inquiries for establishing a background for determining obviousness under 35 U.S.C. 103 are summarized as follows:
1. Determining the scope and contents of the prior art.
2. Ascertaining the differences between the prior art and the claims at issue.
3. Resolving the level of ordinary skill in the pertinent art.
4. Considering objective evidence present in the application indicating obviousness or nonobviousness.
This application currently names joint inventors. In considering patentability of the claims the examiner presumes that the subject matter of the various claims was commonly owned as of the effective filing date of the claimed invention(s) absent any evidence to the contrary. Applicant is advised of the obligation under 37 CFR 1.56 to point out the inventor and effective filing dates of each claim that was not commonly owned as of the effective filing date of the later invention in order for the examiner to consider the applicability of 35 U.S.C. 102(b)(2)(C) for any potential 35 U.S.C. 102(a)(2) prior art against the later invention.
Claims 1-2, 4-5, 7-17, 19-25, 26-30, 34-35, 39-40, 42-45, 47-50, 55, and 57-58 and 72 are rejected under 35 U.S.C. 103 as being unpatentable over Varnadoe et al (CA 2735612) in further view of Evans (US 4,280,053 submitted in the IDS filed 7/23/2018) and in further view of Jonsson (US 4,440,729 submitted in the IDS filed 10/22/2020) and in further view of Scadden et al (“
Regarding Claim 1, Varnadoe discloses a method for preparing a system for eluting radioactive material, the method comprising:
(1) irradiating molybdenum metal
(2) forming titanium molybdate after irradiation (see Page 1, Paragraph 3).
Varnadoe does not disclose the method for forming the titanium molybdate from the irradiated metal molybdenum comprising reacting the metal molybdenum in a liquid medium with a first acid to provide a Mo composition, combining the Mo composition with a titanium source to provide a Ti-Mo composition; and pH adjusting the Ti-Mo composition with a base to precipitate a plurality of Ti-Mo particulates.
Evans discloses a method for producing a metal-molybdate technetium-99m (Tc-99m) generator comprising: (1) mixing solutions containing molybdate obtained by dissolving MoO3 with ammonium hydroxide (i.e., a Mo composition) and zirconium salts or salts of other cations (i.e., metal source) in strongly acidic solution; (2) increasing the pH of the solution by addition of an alkali to precipitate the metal molybdate (see Col 3, Ln 37-42). Evans also discloses where besides zirconium molybdate, similar techniques are used to make titanium molybdate (see Col 3, LN 45-50). Evans further discloses that the molybdate precipitates are particles (see Abstract and Examples). Evans further discloses that the particles can be packed in finely divided form into a column as a generator (see Abstract) and where the generator is convenient and simple to use (see Col 2, Ln 38-42). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the method for preparing a Tc-99m generator as disclosed by Varnadoe where the Ti-Mo is precipitated by combining a molybdate solution (a Mo composition) with a titanium salt solution to provide a Ti-Mo composition; and pH adjusting the Ti-Mo composition with a base to precipitate a plurality of Ti-Mo particulates as disclosed by Evans as a known method for forming molybdate where the result would predictably be suitable for Tc-99m generators.
Regarding reacting a metal molybdenum material with acid, Jonsson discloses that when molybdenum metal is dissolved by nitric acid and sulfuric acid the molybdenum is dissolved as molybdic acid (see Col 1, Ln 51-60). Jonsson further discloses the molybdic acid converted to MoO3 (see Col 5, Ln 20-23). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform a method as disclosed by Varnadoe and Evans where the molybdate solution is obtained by first dissolving metal molybdate with acid to prepare molybdate as disclosed by Jonsson as a known method for obtaining MoO3. A person of ordinary skill in the art would reasonably predict that combining Evans and Jonsson would result in the production of Ti-Mo because the molybdate produced by Jonsson has identical chemical composition (i.e., MoO3) and Jonsson suggests that the recovered molybdenum is commercially useful.
Varnadoe, Evans, and Jonsson do not disclose a method where the titanium salt is titanium chloride.
Monroy-Guzman discloses a method for producing a titanium-molybdate (Ti-Mo) for a molybdenum-99/technetium-99m (Mo-99/Tc-99m) generator comprising:
(1) dissolving MoO3 in NH4OH to form a molybdate solution and adjusting the pH to 4.5 by adding HCl and adding the molybdate solution dropwise to a solution containing TiCl3 or TiCl4 dissolved in HCl to provide a Ti-Mo composition;
(2) adjusting the pH of the Ti-Mo gel with NH4OH; and drying and crushing the resulting gel; and
(3) irradiating the Ti-Mo gel (see Page 11-12, Experimental Section).
It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the process for preparing a titanium molybdate by precipitation as disclosed by Varnadoe, Jonsson, and Evans where the titanium source is a TiCl3 or TiCl4 as disclosed by Monroy-Guzman with the predictable result that titanium molybdate can be precipitated from molybdate and titanium chloride since Monroy-Guzman suggests that titanium molybdate suitable for generators can be produced from coprecipitation with titanium chloride.
Varnadoe, Jonsson, and Evans do not disclose dissolving the metal molybdenum with a halogen acid.
Scadden discloses dissolving metallic molybdenum with dilute nitric acid, warm aqua regia (i.e., nitric acid and hydrochloric acid), or hot concentrated sulfuric acid which produces solutions with molybdenum in solution as an oxygenated anion (i.e., molybdate) (see Page 2, Bottom). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform a method as disclosed by Varnadoe, Jonsson, Evans, Monroy-Guzman and Courty where a warm aqua regia (i.e. a nitric acid and hydrochloric acid is used to dissolved the metallic molybdenum, as disclosed by Scadden, as the mere substitution of one known equivalent for dissolving molybdenum for another with a reasonable expectation that the warm aqua regia would dissolve the molybdenum as suggested by Scadden.
Regarding Claims 2 and 4, Jonsson discloses a method comprising a nitric acid and sulfuric acid (i.e., mineral acids).
Regarding Claim 5, Jonsson discloses a method comprising water (see Col 1, Ln 11).
Regarding Claim 7, Jonsson discloses a method where reacting the metal Mo material subjects the material to an oxidation and a dissolution (see Col 2, Ln 23-34).
Regarding Claim 8, Evans discloses the method where MoO3 is dissolved (see Col 3, Ln 17-18).
Regarding Claim 9, Jonsson discloses a method for chemical dissolution of molybdenum comprising acid dissolving molybdenum where heat is removed from the reaction because the reaction is exothermic and NO2 gases generated from the reaction with nitric acid can react with oxygen and condense as nitric acid (see Col 1, Ln 50-60 and Col 6, Ln 3 to Col 7, Ln 15).
Regarding Claims 10-14, Jonsson discloses that a temperature of 50°C is desirable for maintaining reaction velocity (see Col 7, Ln 16-43).
Regarding Claim 15, Jonsson also discloses that temperatures between 30°C and 40°C is the best condition for promoting the reforming of nitric acid (see Col 7, Ln 37-40). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention perform a method to prepare the metal molybdate gel with a step for acid dissolving metal molybdenum as disclosed in Evans, Jonsson, and Evans where the temperature is maintained between 30°C and 40°C if preventing NO2 generation is more desired than reaction velocity for environmental reasons.
Regarding Claims 16-17, Evans discloses a method where the reagents are combined and precipitation is performed with constant stirring (i.e., mechanical agitation) (see Col 3, Ln 21 and Col 5, Ln 10-18).
Regarding Claim 20, Evans discloses a method where during preparation of a zirconium molybdate the molybdate solution is added to the zirconium salt solution (see Examples 1-3). However, it has been held that absent unexpected results it is obvious to change the order of adding ingredients. Therefore, it would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the method as disclosed by Varnadoe, Jonsson, and Evans where a molybdate solution and titanium salt solution are added in any order including the titanium source solution to the molybdate solution absent evidence of unexpected results.
Regarding Claim 21, Monroy-Guzman discloses a method where the molar ratio of the Ti:Mo is 1:2 to 2:1 (see Page 12, ¶2 and Table 1, Series B). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the process for preparing a titanium molybdate by precipitation as disclosed by Varnadoe, Jonsson, and Evans where the Ti:Mo ratio is 1:2 to 2:1 as disclosed by Monroy-Guzman with the predictable result that titanium molybdate will be precipitated from molybdate and titanium chloride since Monroy-Guzman suggests that titanium molybdate suitable for generators can be produced from coprecipitation with titanium chloride.
Regarding Claim 22, Monroy-Guzman discloses combining the molybdate solution to the titanium source in the form of drops (see Page 11, Experimental Section). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the process for preparing a titanium molybdate by precipitation as disclosed by Varnadoe, Jonsson, and Evans where the molybdate solution is added to the titanium source in the form of drops as disclosed by Monroy-Guzman with the predictable result that titanium molybdate will be precipitated from molybdate and titanium chloride since Monroy-Guzman suggests that titanium molybdate suitable for generators can be produced from coprecipitation with titanium chloride.
Regarding Claim 23-25, Monroy-Guzman further discloses adding HCl to adjust the pH of the molybdate solution (see Page 12 ¶1). Monroy-Guzman also discloses a method where the titanium chloride is dissolved in water and HCl and further diluted in HCl (see Page 12, ¶1). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the process for preparing a titanium molybdate by precipitation as disclosed by Varnadoe, Jonsson, and Evans where HCl is further added as disclosed by Monroy-Guzman with the predictable result that titanium molybdate will be precipitated from molybdate and titanium chloride since Monroy-Guzman suggests that titanium molybdate suitable for generators can be produced from coprecipitation with titanium chloride.
Regarding Claim 26, it would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the method as disclosed by Varnadoe, Jonsson, and Evans where the combination of molybdate solution and titanium salt solution and HCl are added in any order including the titanium source solution to the molybdate solution absent evidence of unexpected results.
Regarding Claim 27, Evans discloses a method where the molybdate salt solution and metal salt solution is combined in a strongly acidic solution (see Col 3, Ln 40). Evans also discloses the alternative method in the examples where an acidic solution with pH of 1 is added to a molybdate solution with higher pH to precipitate the metal molybdate particles (see Examples 1 and 2). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform a method to prepare the metal molybdate gel with a step for combining the salt solutions in strong acid solution as disclosed in Varnadoe, Jonsson, and Evans where the pH of the mixture is 1 since this solution keeps the ions in solution until precipitation as suggested by Evans.
Regarding Claim 28, Evans also discloses where an acidic solution with pH of 1 is added to a molybdate solution with higher pH of 4 to 5.5 to precipitate the metal molybdate particles (see Examples 1 and 2). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform a method to prepare the metal molybdate gel with a step for precipitating by gradually increasing the pH by adding alkali as disclosed in Varnadoe, Jonsson, and Evans where adjusting the pH is 4 or 5.5 since this pH precipitates the metal molybdate as suggested by Evans.
Regarding Claim 29, Monroy-Guzman discloses a method comprising adjusting pH with ammonium hydroxide (see Page 12, ¶2). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the process for preparing a titanium molybdate by precipitation as disclosed by Varnadoe, Jonsson, and Evans where the pH is adjusted with ammonium hydroxide as disclosed by Monroy-Guzman with the predictable result that titanium molybdate will be precipitated from molybdate and titanium chloride since Monroy-Guzman suggests that titanium molybdate suitable for generators can be produced from coprecipitation with titanium chloride.
Regarding Claim 30, Evans discloses precipitating the molybdate by gradually increasing the pH of the solution by the addition of alkali (see Col 3, LN 40-42). Monroy-Guzman discloses a method where reagents are combined by dropwise introduction (see Page 11, Experimental Section). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to prepare the metal molybdate by gradually increasing the pH with an alkali as disclosed by Varnadoe, Jonsson, and Evans where the ammonium hydroxide is added dropwise as a typical method for gradually adding ingredients as suggested by Monroy-Guzman.
Regarding Claim 34, Evans further discloses a method where separating comprises filtering to retain the particles (see Col 5, Ln 11-20).
Regarding Claim 35, Evans discloses a method where separating comprises filtering to retain the particles (see Col 5, Ln 11-20).
Regarding Claims 39, Monroy-Guzman discloses the Ti-Mo gel subjected to heat energy to dry using an infrared lamp at 40-60 °C (see Page 12, ¶2). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the process for preparing a titanium molybdate by precipitation as disclosed by Varnadoe, Jonsson, and Evans where drying comprises an infrared lamp at 40-60°C as disclosed by Monroy-Guzman with the predictable result that titanium molybdate will dry since Monroy-Guzman suggests that titanium molybdate suitable for generators can be produced from coprecipitation with titanium chloride.
Regarding Claim 40, Monroy-Guzman discloses the method where the Ti-Mo gel is dried using an infrared lamp (see Page 12, ¶2).
Regarding Claims 42-43, Monroy-Guzman discloses the Ti-Mo gel comprising crystalline ammonium chloride in the pores of a matrix (see Page 15, Effect of gel washing and Figure 2).
Regarding Claim 44, Monroy-Guzman discloses the Ti-Mo gel crushed in an agate mortar (i.e., milled) (see Page 12, ¶2). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the process for preparing a titanium molybdate by precipitation as disclosed by Varnadoe, Jonsson, and Evans where the titanium molybdate is milled as disclosed by Monroy-Guzman with the predictable result that titanium molybdate with suitable size for generators will be produced since Monroy-Guzman suggests that titanium molybdate suitable for generators can be produced with milling.
Regarding Claim 45, Monroy-Guzman discloses the Ti-Mo gel subjected to heat to dry (see Page 12, ¶2). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the process for preparing a titanium molybdate by precipitation as disclosed by Varnadoe, Jonsson, and Evans where the titanium molybdate is heated to dry as disclosed by Monroy-Guzman with the predictable result that a dry titanium molybdate suitable for loading in generators will be produced since Monroy-Guzman suggests that titanium molybdate suitable for generators can be produced after drying with heat.
Regarding Claims 47-48, Evans discloses a method where the particles are sieved to a size between 150-500 µm before packing into the generator. It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the process for producing metal molybdate gel as disclosed by Varnadoe, Jonsson, and Evans where milling produces a particle in the range of 150 µm to 500 µm to make the particle suitable for loading into the column of a generator.
Regarding Claim 49, Monroy-Guzman discloses washing the Ti-Mo gel (see Page 12, ¶2). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the process for preparing a titanium molybdate by precipitation as disclosed by Varnadoe, Jonsson, and Evans where the titanium molybdate is washed as disclosed by Monroy-Guzman with the predictable result that titanium molybdate suitable for generators will be produced since Monroy-Guzman suggests drying titanium molybdate for a generator.
Regarding Claim 50, Evans discloses drying molybdate gels (see Example 1). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to dry the molybdate gel as disclosed by Evans so that it can be used to form the generator.
Regarding Claim 55, the claim limitations are met as applied above in Claim 1. Further regarding oxidizing, Jonsson discloses that dissolving molybdenum with acid produces molybdenum in solution as an H2MoO4 (i.e., oxidized).
Regarding Claim 57, the claim limitations are met as applied above in Claim 1.
Regarding Claim 58, the claim limitations are met as applied above in Claim 1.
Regarding Claim 72, Scadden teaches aqua regia (i.e., hydrochloric acid).
Claims 6 and 53 is/are rejected under 35 U.S.C. 103 as being unpatentable over Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden as applied to Claim 1 and in further view of Bennett (US 5,802,438 submitted in the IDS filed 10/22/2020).
As applied to Claim 1, Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden suggest a method for preparing titanium molybdate comprising irradiating a metal molybdenum and forming a titanium molybdate for Tc-99 generation where the metal molybdate is dissolved in halogen acid to form molybdate, and the titanium molybdate is precipitated from an acidic solution comprising molybdate and titanium chloride by adjusting the pH with a base.
Regarding Claim 6, Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden do not specifically disclose a molar ratio of the Mo material to the first acid in the range of 0.1:1 to about 10:1.
Bennett discloses a method for generating crystalline 99Mo comprising a step of dissolving 99Mo metal in an oxygen-containing primary solvent (acid) including HNO3, H2SO4, or H2O2 (see Col 16, Ln 4-25). Bennett further discloses the method where dissolving the acid comprises a 6-9M HNO3 and where the weight ratio of the metal and primary solvent is from 1-5 : 1-25 (see Col 16, Ln 22). Bennett therefore discloses a method comprising dissolving molybdenum metal where the molar ratio of the metal Mo to the acid is in a range overlapping with 0.1:1 to about 10:1. It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to prepare the titanium molybdate with a step for dissolving metal molybdenum as disclosed by Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden where the molar ratio of metal Mo and acid is in any range overlapping with Bennett’s molar ratio including the claimed range and expect to be able to dissolve the metal molybdenum and produce a molybdenum solution.
Regarding Claims 53, Bennett further discloses production of Mo-99 materials by irradiating Mo-99 metal which is subsequently converted to MoO3-99 (see Col 13, Ln 28-30). Bennett further discloses a method where the 99Mo is generated by irradiating a circular metal molybdenum target which is circular in configuration and has the thickness of 5-50 mm and diameter of 5-20 mm (i.e., discs or tubules) (see Col 14, Ln 12-15). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to prepare the titanium molybdate with a step for irradiating the metal molybdenum as disclosed by Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden where the targets are discs are tubules as disclosed by Bennett since it produces irradiated MoO3 which can be used for forming the Mo99 generator molybdate.
Claims 31-33 and 38 is/are rejected under 35 U.S.C. 103 as being unpatentable over Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden as applied to Claim 1 or 34 and in further view of Courty et al (US 4,141,861 submitted in the IDS filed 10/22/2020).
As applied to Claim 1, Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden suggest a method for preparing titanium molybdate comprising irradiating a metal molybdenum and forming a titanium molybdate for Tc-99 generation where the metal molybdate is dissolved in halogen acid to form molybdate, and the titanium molybdate is precipitated from an acidic solution comprising molybdate and titanium chloride salt by adjusting the pH with a base.
As applied to Claim 34, Evans further discloses a method where separating comprises filtering to retain the particles.
Varnadoe, Evans, and Jonsson do not disclose a temperature of the metal-Mo composition before precipitating and before filtering.
Regarding Claims 31-33, Courty discloses a method for producing an iron and molybdenum gel comprising reacting a solution of ferric salts and soluble molybdate (see Col 2, Ln 34-37). Courty further discloses a method where the temperature of the mixture is maintained between 0 and 15°C (see Col 4, Ln 15-22). Courty suggests that the process comprising mixing at the temperature between 0°C and 15°C produces a homogeneous product and avoids suspended solid particles of MoO3 (see Col 4, Ln 11-22 and Col 7, Ln 43-55). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform a method to prepare the metal molybdate gel with a step for precipitating the metal molybdate gel as disclosed in Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden n where the temperature throughout precipitation is in any workable or optimum range overlapping with 0 to 15°C as disclosed by Courty including 3 to 10°C and expect to produce homogeneous metal molybdate gel particles.
Regarding Claim 38, it would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform a method to prepare the metal molybdate gel with a step for precipitating the metal molybdate gel as disclosed in Varnadoe, Jonsson, and Evans where the temperature throughout precipitation is in any workable or optimum range overlapping with 0 to 15°C as disclosed by Courty including 3 to 10°C and expect to produce a homogeneous metal molybdate gel. It also would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform a method to prepare the metal molybdate gel with a step for separating after precipitating the metal molybdate gel as disclosed in Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden where there is no change in temperature after precipitation to simplify the process and expect to produce homogeneous metal molybdate gel particles.
Claims 36-37 is/are rejected under 35 U.S.C. 103 as being unpatentable over Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden as applied to Claim 35 and in further view of Jones et al (US 6,136,740 submitted in the IDS filed 10/22/2020).
As applied to Claim 35, Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden suggest a method for preparing titanium molybdate comprising irradiating a metal molybdenum and forming a titanium molybdate for Tc-99 generation where the metal molybdate is dissolved in halogen acid to form molybdate, and the titanium molybdate is precipitated from an acidic solution comprising molybdate and titanium chloride salt by adjusting the pH with a base and wherein the Ti-Mo particulates are separated with a filter to retain at least most of the metal-Mo particulates.
Evans discloses filtering with a Buchner funnel (see Example 1). However, Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden do not specifically disclose where the filter is a metal filtering surface.
Jones discloses a method for making an inorganic particulate material comprising a step of separating an aqueous medium and acid from suspended particles by vacuum filtering rapidly in a stainless-steel Buchner funnel (see Col 7, Ln 3-14). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform a method to prepare the metal molybdate gel with a step for filtering to separate the metal-Mo particulates from the liquid medium as disclosed in Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden where the Buchner funnel comprises a stainless steel as disclosed in Jones and expect the stainless steel to be able to separate the particles from the aqueous medium as in Jones.
Claim 41 is/are rejected under 35 U.S.C. 103 as being unpatentable over Varnadoe, Evans, Jonsson, Monroy-Guzman, and Scadden as applied to Claim 40, and in further view of Nakahara et al (US 2010/0183045).
As applied to Claim 40, Varnadoe, Jonsson, Evans, Monroy-Guzman, and Scadden suggest a method for preparing titanium molybdate comprising irradiating a metal molybdenum and forming a titanium molybdate for Tc-99 generation where the metal molybdate is dissolved in halogen acid to form molybdate, the titanium molybdate precipitated from an acidic solution comprising molybdate and titanium chloride salt by adjusting the pH with a base and drying the Ti-Mo at 40-60°C using an infrared lamp.
Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden do not specifically disclose the wavelength of the infrared lamp.
Nakahara discloses a substrate temperature measuring apparatus comprising a heating source that heats a substrate where the heat source comprises an infrared lamp with a wavelength of 700 nm or more (see [0027] and [0029]). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the method to prepare the titanium molybdate gel as disclosed in Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden where the infrared heat lamp is in any working or optimum range overlapping with 700 nm or more as disclosed by Nakahara including the claimed range since this wavelength provides heat to substrates from the infrared lamp as suggested by Nakahara.
Claim 46 is/are rejected under 35 U.S.C. 103 as being unpatentable over Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden as applied to Claim 44, and in further view of Fukushima et al (US 2005/0156144 submitted in the IDS filed 10/22/2020).
As applied to Claim 44, Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden suggest a method for preparing titanium molybdate comprising irradiating a metal molybdenum and forming a titanium molybdate for Tc-99 generation where the metal molybdate is dissolved in halogen acid to form molybdate, and the titanium molybdate is precipitated from an acidic solution comprising molybdate and titanium chloride salt by adjusting the pH with a base and where the titanium molybdate gel is crushed in a mortar before being loaded into column as a generator (see Page 12) but does not specifically disclose wet milling.
Fukushima discloses a method for preparing gel compositions where wet milling is used instead of manual grinding in a mortar for mass production (see [0018]). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the method to prepare the titanium molybdate gel as disclosed in Varnadoe, Evans, Jonsson, Monroy-Guzman and Scadden where the precipitate is wet milling is used instead of a manual grinding in a mortar as disclosed by Fukushima to mass produce the product.
Claim(s) 73-74 and 77-78 are rejected under 35 U.S.C. 103 as being unpatentable over Varnadoe, Evans, Jonsson, Monroy-Guzman, and Courty.
Regarding Claim 73, Varnadoe discloses a method for preparing a system for eluting radioactive material, the method comprising:
(1) irradiating molybdenum metal
(2) forming titanium molybdate after irradiation (see Page 1, Paragraph 3).
Varnadoe does not disclose the method for forming the titanium molybdate from the irradiated metal molybdenum comprising reacting the metal molybdenum in a liquid medium with a first acid to provide a Mo composition, combining the Mo composition with a titanium chloride to provide a Ti-Mo composition; and pH adjusting the Ti-Mo composition with a base to precipitate a plurality of Ti-Mo particulates.
Evans discloses a method for producing a metal-molybdate technetium-99m (Tc-99m) generator comprising: (1) mixing solutions containing molybdate obtained by dissolving MoO3 with ammonium hydroxide (i.e., a Mo composition) and zirconium salts or salts of other cations (i.e., metal source) in strongly acidic solution; (2) increasing the pH of the solution by addition of an alkali to precipitate the metal molybdate (see Col 3, Ln 37-42). Evans also discloses where besides zirconium molybdate, similar techniques are used to make titanium molybdate (see Col 3, LN 45-50). Evans further discloses that the molybdate precipitates are particles (see Abstract and Examples). Evans further discloses that the particles can be packed in finely divided form into a column as a generator (see Abstract) and where the generator is convenient and simple to use (see Col 2, Ln 38-42). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the method for preparing a Tc-99m generator as disclosed by Varnadoe where the Ti-Mo is precipitated by combining a molybdate solution (a Mo composition) with a titanium salt solution to provide a Ti-Mo composition; and pH adjusting the Ti-Mo composition with a base to precipitate a plurality of Ti-Mo particulates as disclosed by Evans as a known method for forming molybdate where the result would predictably be suitable for Tc-99m generators.
Regarding reacting a metal molybdenum material with acid, Jonsson discloses that when molybdenum metal is dissolved by nitric acid and sulfuric acid the molybdenum is dissolved as molybdic acid (see Col 1, Ln 51-60). Jonsson further discloses the molybdic acid converted to MoO3 (see Col 5, Ln 20-23). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform a method as disclosed by Varnadoe and Evans where the molybdate solution is obtained by first dissolving metal molybdate with acid to prepare molybdate as disclosed by Jonsson as a known method for obtaining MoO3. A person of ordinary skill in the art would reasonably predict that combining Evans and Jonsson would result in the production of Ti-Mo because the molybdate produced by Jonsson has identical chemical composition (i.e., MoO3) and Jonsson suggests that the recovered molybdenum is commercially useful.
Regarding the titanium salt comprising titanium chloride, Monroy-Guzman discloses a method for producing a titanium-molybdate (Ti-Mo) for a molybdenum-99/technetium-99m (Mo-99/Tc-99m) generator comprising:
(1) dissolving MoO3 in NH4OH to form a molybdate solution and adjusting the pH to 4.5 by adding HCl and adding the molybdate solution dropwise to a solution containing TiCl3 or TiCl4 dissolved in HCl to provide a Ti-Mo composition;
(2) adjusting the pH of the Ti-Mo gel with NH4OH; and drying and crushing the resulting gel; and
(3) irradiating the Ti-Mo gel (see Page 11-12, Experimental Section).
It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the process for preparing a titanium molybdate by precipitation as disclosed by Varnadoe, Jonsson, and Evans where the titanium source is a TiCl3 or TiCl4 as disclosed by Monroy-Guzman with the predictable result that titanium molybdate can be precipitated from molybdate and titanium chloride since Monroy-Guzman suggests that titanium molybdate suitable for generators can be produced from coprecipitation with titanium chloride.
Courty discloses a method for producing an iron and molybdenum gel comprising reacting a solution of ferric salts and soluble molybdate (see Col 2, Ln 34-37). Courty further discloses a method where the temperature of the mixture is maintained between 0 and 15°C (see Col 4, Ln 15-22). Courty suggests that the process comprising mixing at the temperature between 0°C and 15°C produces a homogeneous product and avoids suspended solid particles of MoO3 (see Col 4, Ln 11-22 and Col 7, Ln 43-55). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform a method to prepare the metal molybdate gel with a step for precipitating the metal molybdate gel as disclosed in Varnadoe, Evans, and Jonsson where the temperature throughout precipitation is cooled to 0 to 15°C as disclosed by Courty to produce homogeneous metal molybdate gel particles.
Regarding claim 74, Jonsson discloses a method comprising a nitric acid and sulfuric acid (i.e., mineral acids).
Regarding claim 77, Monroy-Guzman discloses TiCl3 or TiCl4.
Regarding claim 78, Monroy-Guzman discloses the Ti-Mo gel crushed in an agate mortar (i.e., milled) (see Page 12, ¶2).
Claim 75-76 are rejected under 35 U.S.C. 103 as being unpatentable over Varnadoe, Evans, Jonsson, Monroy-Guzman, and Courty as applied to Claim 73, and in further view of Scadden.
As applied to Claim 73, Varnadoe, Evans, Jonsson, Monroy-Guzman, and Courty suggest a method comprising all of the limitations of claim 73.
Regarding Claims 75-76, Varnadoe do not disclose dissolving the metal molybdenum with a halogen acid.
Scadden discloses dissolving metallic molybdenum with dilute nitric acid, warm aqua regia (i.e., nitric acid and hydrochloric acid), or hot concentrated sulfuric acid which produces solutions with molybdenum in solution as an oxygenated anion (i.e., molybdate) (see Page 2, Bottom). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform a method as disclosed by Varnadoe, Jonsson, Evans, Monroy-Guzman and Courty where a warm aqua regia (i.e. a nitric acid and hydrochloric acid is used to dissolved the metallic molybdenum, as disclosed by Scadden, as the mere substitution of one known equivalent for dissolving molybdenum for another with a reasonable expectation that the warm aqua regia would dissolve the molybdenum as suggested by Scadden.
Claim(s) 79 is rejected under 35 U.S.C. 103 as being unpatentable over Varnadoe, Evans, Jonsson, Courty, Scadden, and in further view of Wilson (US 20140029710).
Varnadoe discloses a method for preparing a system for eluting radioactive material, the method comprising:
(1) irradiating molybdenum metal
(2) forming titanium molybdate after irradiation (see Page 1, Paragraph 3).
Varnadoe does not disclose the method for forming the titanium molybdate from the irradiated metal molybdenum comprising reacting the metal molybdenum in a liquid medium with a first acid to provide a Mo composition, combining the Mo composition with a titanium chloride to provide a Ti-Mo composition; and pH adjusting the Ti-Mo composition with a base to precipitate a plurality of Ti-Mo particulates.
Evans discloses a method for producing a metal-molybdate technetium-99m (Tc-99m) generator comprising: (1) mixing solutions containing molybdate obtained by dissolving MoO3 with ammonium hydroxide (i.e., a Mo composition) and zirconium salts or salts of other cations (i.e., metal source) in strongly acidic solution; (2) increasing the pH of the solution by addition of an alkali to precipitate the metal molybdate (see Col 3, Ln 37-42). Evans also discloses where besides zirconium molybdate, similar techniques are used to make titanium molybdate (see Col 3, LN 45-50). Evans further discloses that the molybdate precipitates are particles (see Abstract and Examples). Evans further discloses that the particles can be packed in finely divided form into a column as a generator (see Abstract) and where the generator is convenient and simple to use (see Col 2, Ln 38-42). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the method for preparing a Tc-99m generator as disclosed by Varnadoe where the Ti-Mo is precipitated by combining a molybdate solution (a Mo composition) with a titanium salt solution to provide a Ti-Mo composition; and pH adjusting the Ti-Mo composition with a base to precipitate a plurality of Ti-Mo particulates as disclosed by Evans as a known method for forming molybdate where the result would predictably be suitable for Tc-99m generators.
Regarding reacting a metal molybdenum material with acid, Jonsson discloses that when molybdenum metal is dissolved by nitric acid and sulfuric acid the molybdenum is dissolved as molybdic acid (see Col 1, Ln 51-60). Jonsson further discloses the molybdic acid converted to MoO3 (see Col 5, Ln 20-23). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform a method as disclosed by Varnadoe and Evans where the molybdate solution is obtained by first dissolving metal molybdate with acid to prepare molybdate as disclosed by Jonsson as a known method for obtaining MoO3. A person of ordinary skill in the art would reasonably predict that combining Evans and Jonsson would result in the production of Ti-Mo because the molybdate produced by Jonsson has identical chemical composition (i.e., MoO3) and Jonsson suggests that the recovered molybdenum is commercially useful.
Regarding cooling the Ti-Mo composition, Courty discloses a method for producing an iron and molybdenum gel comprising reacting a solution of ferric salts and soluble molybdate (see Col 2, Ln 34-37). Courty further discloses a method where the temperature of the mixture is maintained between 0 and 15°C (see Col 4, Ln 15-22). Courty suggests that the process comprising mixing at the temperature between 0°C and 15°C produces a homogeneous product and avoids suspended solid particles of MoO3 (see Col 4, Ln 11-22 and Col 7, Ln 43-55). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform a method to prepare the metal molybdate gel with a step for precipitating the metal molybdate gel as disclosed in Varnadoe, Evans, and Jonsson where the temperature throughout precipitation is cooled to 0 to 15°C as disclosed by Courty to produce homogeneous metal molybdate gel particles.
Regarding the first acid comprising a mineral, halogen acid selected from the group consisting of hydrochloric acid, hydrofluoric acid, hydrobromic acid, hydroiodic acid and a combination thereof, Scadden discloses dissolving metallic molybdenum with dilute nitric acid, warm aqua regia (i.e., nitric acid and hydrochloric acid), or hot concentrated sulfuric acid which produces solutions with molybdenum in solution as an oxygenated anion (i.e., molybdate) (see Page 2, Bottom). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform a method as disclosed by Varnadoe, Jonsson, Evans, and Courty where a warm aqua regia (i.e. a nitric acid and hydrochloric acid is used to dissolved the metallic molybdenum, as disclosed by Scadden, as the mere substitution of one known equivalent for dissolving molybdenum for another with a reasonable expectation that the warm aqua regia would dissolve the molybdenum as suggested by Scadden.
Regarding irradiating a solid molybdenum metal target, Varnadoe does not explicitly teach that the metal molybdenum target is a solid. Wilson teaches a method for production of technetium from a molybdenum metal target formed from a pressed powder, metallic foil target, powder sintered into pellets (i.e., solids). Wilson further teaches that irradiation of metal molybdenum targets as opposed to molybdenum oxide is because they can withstand much higher beam currents which allows for production of much greater quantities of the technetium product (see [0025]). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform a method as disclosed by Varnadoe, Jonsson, Evans, Courty, and Scadden where the target is a solid metal molybdenum target as taught by Wilson so that irradiation can produce greater quantities of the technetium.
Claims 80-82 are rejected under 35 U.S.C. 103 as being unpatentable over Varnadoe, Evans, Jonsson, Courty, Scadden, and Wilson as applied to Claim 79, and in further view of Monroy-Guzman.
As applied to claim 79, Varnadoe, Evans, Jonsson, Courty, Scadden, and Wilson suggest a process for producing a titanium-molybdate comprising all of the limitations of claim 79.
Regarding Claims 80-81 Varnadoe, Evans, Jonsson, Courty, and Scadden do not disclose a method where the titanium salt is titanium chloride.
Monroy-Guzman discloses a method for producing a titanium-molybdate (Ti-Mo) for a molybdenum-99/technetium-99m (Mo-99/Tc-99m) generator comprising:
(1) dissolving MoO3 in NH4OH to form a molybdate solution and adjusting the pH to 4.5 by adding HCl and adding the molybdate solution dropwise to a solution containing TiCl3 or TiCl4 dissolved in HCl to provide a Ti-Mo composition;
(2) adjusting the pH of the Ti-Mo gel with NH4OH; and drying and crushing the resulting gel; and
(3) irradiating the Ti-Mo gel (see Page 11-12, Experimental Section).
It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the process for preparing a titanium molybdate by precipitation as disclosed by Varnadoe, Jonsson, and Evans where the titanium source is a TiCl3 or TiCl4 as disclosed by Monroy-Guzman with the predictable result that titanium molybdate can be precipitated from molybdate and titanium chloride since Monroy-Guzman suggests that titanium molybdate suitable for generators can be produced from coprecipitation with titanium chloride.
Regarding claim 81, Monroy-Guzman discloses TiCl3 or TiCl4.
Regarding claim 82, Monroy-Guzman discloses the Ti-Mo gel crushed in an agate mortar (i.e., milled) (see Page 12, ¶2).
Citation of Pertinent Art
The prior art made of record and not relied upon is considered pertinent to applicant's disclosure.
Shafiq et al (CHARACTERISTICS AND BEHAVIOR OF A 99Mo/99mTc GENERATOR USING IRRADIATED TITANIUM MOLYBDATE AS COLUMN MATRIX, J. RADIOANAL.NUCL.CHEM., LETTERS 199 (3) (1995) 173-181) teaches a method for preparing a titanium molybdate comprising dissolving TiCl4 in water, dissolving MoO3 in NH3 solution, adding ammonium molybdate solution to the TiCl4 solution and separating and washing the gel-like precipitate and sieving to get a particle size in the range of 320-555 mesh (See Page 174).
Conclusion
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/MICHAEL FORREST/Primary Examiner, Art Unit 1738
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