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 .
Response to Arguments
The applicant’s arguments in regards to Klose-Schubert failing to teach “wherein the carrier metal oxide on the first oxygen lattice sites is doped with at least one element from the group consisting of nitrogen, carbon and boron” have been considered but are moot because the new ground of rejection in regards to said feature does not rely solely on Klose-Schubert teaching said limitation.
Applicant's arguments filed October 7, 2025 have been fully considered but they are not persuasive.
In regards to the applicant’s amendment to claim 1 to specify “wherein the first metallic elements in the carrier metal oxide are each present in a same solid stoichiometric compound or a same solid homogenous solution, and the at least one second metallic element in the catalyst material are each present in a same solid stoichiometric compound or a same solid homogenous solution”, the applicant asserts that the discussion of the previous rejection of record indicates that the prior art of record fails to teach said structure. This argument has been fully considered, but has not been found to be persuasive.
The text cited by the applicant from the previous office action of record reads: “It is noted that the instant claim does not require structure where the carrier metal oxide and catalyst material are present in the same solid stoichiometric compound or solid homogenous solution, but instead requires that they are “each present in a solid stoichiometric compound or solid homogeneous solution”> Accordingly, if they are each present in individual solid stoichiometric compounds or solid homogeneous solutions, said structure would read upon the limitations of the instant claim”.
This statement indicates that the claim as written does not require the carrier metal oxide and catalyst material are required to be in a singular same solid stoichiometric compound or singular same solid homogeneous solution. The applicant’s amendments to the claims, presented in the amendment of October 7, 2025, do not require this structure as well.
The applicant’s amendment requires structure “wherein the first metallic elements in the carrier metal oxide are each present in a same solid stoichiometric compound or a same solid homogenous solution” and “the at least one second metallic element in the catalyst material are each present in a same solid stoichiometric compound or a same solid homogenous solution”. Here, for the carrier metal oxide the applicant has introduced a new first same solid stoichiometric compound or a first same solid homogenous solution, and then separately for the catalyst material, has introduced another new same solid stoichiometric compound or same homogenous solution, which are accordingly not the same as the compound or solution introduced for the carrier metal oxide. Accordingly, the claims as written require that the carrier metal oxide’s metallic elements are present in a same solution or same compound, and that separately, the catalyst material’s metallic elements are present in their own same solution or same compound, without a requirement that the catalyst material and carrier metal oxide’s metallic elements be both present in a single same solid stoichiometric solution or single same solid stoichiometric compound.
As discussed in the previous office action of record, and presented below, the metallic elements of the carrier metal oxide are present in their own solid homogenous solution, and the metallic elements of the carrier metal oxide are present in their own solid stoichiometric compound.
Additionally, in regards to the amended limitation of claim 17 which requires that the carrier metal oxide on the first oxygen lattice sites is doped with carbon, the applicant asserts that Klose-Schubert is directed towards a carbon-free electrocatalyst for fuel cells, and that accordingly Klose-Schubert cannot reasonably be combined with any other reference to realize the claimed doping with carbon. This argument has been fully considered but has not been found to be persuasive.
Klose-Schubert does discuss their invention within the context of being carbon-free, however the omission of carbon is specifically discussed in regards to carbon-containing supports, with the goal being the avoidance of corrosion of carbon supports (Paragraph 0021, “As opposed to conventional electrocatalysts with C-containing supports, no corrosion of the carbon support takes place. The electrocatalysts according to the invention are free from carbon, i.e., C-free.”). Therefore, it would be appropriate to consider the inclusion of carbon in the invention of Klose-Schubert in the context of non-support structure carbon. If carbon is introduced in a context other than being a part of a support structure, Klose-Schubert’s goal of avoiding the corrosion of carbon supports can still be maintained. Additionally, this does not discount the use of carbon materials which are directly disclosed as having the functionality of avoiding corrosion, as discussed below in regards to Wakizaka.
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.
Claims 1-6, 8-9, and 19 are 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 1 is indefinite as a result of the language “wherein the first metallic elements in the carrier metal oxide are each present in a same solid stoichiometric compound or a same solid homogeneous solution, and the at least one second metallic element in the catalyst material are each present in a same solid stoichiometric compound or a same solid homogeneous solution,”, where the claim introduces a same solid stoichiometric compound and a same solid homogenous solution, and then introduces a second new same solid stoichiometric compound and a second new same solid homogenous solution. Based on the language of the claim, it is unclear if the second same solid stoichiometric compound and second same solid homogenous solution are new and distinct, or if they are the same compound and solution respectively as the ones introduced earlier in the claim. Accordingly, the claim is rendered indefinite.
Claims 2-6 and 8-9 are indefinite as a result of their dependence on indefinite claim 1.
Claim 19 is indefinite as a result of the language “wherein the first metallic elements in the carrier metal oxide are each present in a same solid stoichiometric compound or a same solid homogeneous solution, and the at least one second metallic element in the catalyst material are each present in a same solid stoichiometric compound or a same solid homogeneous solution,”, where the claim introduces a same solid stoichiometric compound and a same solid homogenous solution, and then introduces a second new same solid stoichiometric compound and a second new same solid homogenous solution. Based on the language of the claim, it is unclear if the second same solid stoichiometric compound and second same solid homogenous solution are new and distinct, or if they are the same compound and solution respectively as the ones introduced earlier in the claim. Accordingly, the claim is rendered indefinite.
Claim Rejections - 35 USC § 103
In the event the determination of the status of the application as subject to AIA 35 U.S.C. 102 and 103 (or as subject to pre-AIA 35 U.S.C. 102 and 103) is incorrect, any correction of the statutory basis (i.e., changing from AIA to pre-AIA ) for the rejection will not be considered a new ground of rejection if the prior art relied upon, and the rationale supporting the rejection, would be the same under either status.
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.
Claim(s) 1-6, and 8-9 is/are rejected under 35 U.S.C. 103 as being unpatentable over Klose-Schubert (US 20140349203) and in view of Kumta (US 20170233879 A1), Naito (US 20160186335 A1), Raiford (US 20070212593 A1), and Ghanem (US 20160298245 A1).
Regarding Claim 1, Klose-Schubert discloses a catalyst system (Abstract, “The invention relates to a carbon-free electrocatalyst for fuel cells,”) comprising an electrically conductive carrier metal oxide (Abstract, “containing an electrically conductive substrate”) which Klose-Schubert discloses to be a multicomponent support material OX1-OX2 (Paragraph 0025, “The multicomponent support material OX1-OX2”). Here, the multicomponent support material is disclosed as preferably having a conductivity greater than 1 S/cm (Paragraph 0025, “The multicomponent support material OX1-OX2 has an electrical conductivity in the range of >0.01 S/cm, preferably >0.1 S/cm and more preferably in the range of >1 S/cm.”), where Klose-Schubert further discloses a specific embodiment which has an electronic conductivity of 80 S/cm (Paragraph 0087, “Electrical conductivity: 80 S/cm (at 50 MPa)”), where high electronic conductivity is a desirable attribute in an electrically conductive carrier metal oxide, thereby making obvious the range of the instant claim, where the electrical conductivity of the electrically conductive carrier metal oxide is at least 10 S/cm.
Additionally, Klose Schubert discloses structure where the carrier metal oxide has at least two metallic elements selected from the group of non-precious elements (Paragraph 0048-0056, “Suitable OX2 precursor compounds for preparing the conductive oxides of the type include for example: […] For Sb/Sn oxide: SnCl4-5H2O…”), further disclosing a specific embodiment which comprises Sb/SnOx-TiO2 (Paragraph 0096, “10 wt % of Pt on Sb/SnOx--TiO2”).
Additionally, in regards to the limitation where the carrier metal oxide has a structure comprising oxide grains with a grain size of at least 30 nm, Klose-Schubert fails to disclose the grain size of the carrier metal oxide. Therefore, we look to Naito, which discloses structure which includes an electrode which comprises inorganic oxide particles (Abstract, “containing an inorganic oxide and provided on the first surface of the first electrode to cover the first surface and the through-holes.”). Here, Naito further discloses structure where their electrode comprises oxide particles (Paragraph 0039, “Various materials may be used for the inorganic oxide. For example, titanium oxide, silicon oxide, aluminum oxide, niobium oxide, zirconium oxide, tantalum oxide, nickel oxide, tungsten oxide, zircon or zeolite may be used.”) that have a grain size of 50 nm (Paragraph 0112, “An aqueous dispersion containing titanium oxide nanoparticles having a grain size of 50 nm is applied to the first surface 21a of the first electrode 20 by screen printing.”). Here, Naito discloses that titanium oxide facilitates cation-exchange (Paragraph 0040, “easily have a negative zeta potential in an alkaline region and therefore exhibit a cation-exchange function.”). As Naito discloses this benefit, and further discloses that a specific grain size that achieves this benefit to be 50 nm, it would be obvious to one ordinarily skilled in the art to apply this grain size of Naito to the invention of Klose-Schubert, to achieve said benefit where Klose-Schubert is otherwise silent in regards to grain size, thereby reading upon the limitations of the instant claim wherein the carrier metal, has a structure comprising oxide grains with a grain size of at least 30 nm.
Additionally, Klose-Schubert discloses structure which comprises the carrier metal oxide having a first crystal lattice structure comprising first oxygen lattice sites and first metal lattice sites (Paragraph 0096, “10 wt % of Pt on Sb/SnOx--TiO2”), here being tin oxide.
Additionally, in regards to the limitation of the instant claim which requires structure wherein the carrier metal oxide on the first oxygen lattice sites is doped with at least one element from the group consisting of nitrogen, carbon, or boron, Klose-Schubert fails to disclose said structure.
Therefore we look to Ghanem, which discloses a titanium oxide catalyst which is doped with nitrogen (Abstract, “The electrochemical method of producing hydrogen peroxide using a titanium oxide nanotube catalyst is an electrochemical process for producing hydrogen peroxide using a cathode formed as a nanostructured titania (TiO.sub.2) electrode surface treated with nitrogen.”).
Here, Ghanem discloses the use of nitrogen atmosphere annealing to introduce nitrogen into the crystal lattice of a titanium oxide (Paragraph 0033, “The TiO.sub.2 nanotube array forming the cathode 104 is treated with nitrogen, either by annealing the array in nitrogen atmosphere, doping the array with nitrogen plasma, or any other suitable process for modifying the surface of the titania with nitrogen. It should be understood that nitrogen may be replaced by any other suitable dopant which creates defects within the TiO.sub.2 nanotubes crystal lattice.”). Additionally, Ghanem discloses that the annealing in a nitrogen atmosphere which results in nitrogen doping causes an electrical conductivity increase between three and ten times greater than samples annealed in air or carbon. Here, where a significant increase in conductivity is a desirable attribute for a carrier metal oxide, it would therefore be obvious to one ordinarily skilled in the art to make use of the nitrogen annealing doping teaching of Ghanem, thereby resulting in structure wherein the carrier metal oxide on the first oxygen lattice sites is doped with unbonded nitrogen.
Additionally, Klose-Schubert discloses structure which comprises an electrically conductive metal-oxide catalyst material, specifically the use of noble metal-containing alloy particles (Paragraph 0042, “In a particular embodiment, noble metal-containing alloy particles may be used as the catalytically active particles. Such alloys comprise alloys of the noble metals with one another (for example platinum/ruthenium or platinum/gold) or those with base metals selected from the group vanadium, chromium, manganese, iron, cobalt, nickel, copper and zinc.”). Here, Klose-Schubert discloses that the noble metal alloy particles are dried following their deposition onto the support substrate (Paragraph 0067, “Once the noble metal particles or noble metal alloy particles have been deposited, the resulting electrocatalyst is dried. Drying is preferably effected in the range from 50 to 100 C.”) where drying of an alloy which includes oxidizable metal atoms will result in oxidation, thereby inherently directing the catalytically active particles of Klose-Schubert towards a metal-oxide catalyst material.
Additionally, in regards to the limitation which requires structure where the at least one first metallic element in the carrier metal oxide is present in a solid stoichiometric compound or solid homogeneous solution, Klose-Schubert discloses structure wherein the catalyst material is presented in a solution (Paragraph 0097, “17.25 g of SbCl3 (Merck) and 1.0 l of an HCl solution (37%, Merck) diluted with DM water to 18% (m/m), are added to 238.6 g of SnCl4.5H2O (Sigma-Aldrich) in order to obtain an Sb/Sn solution having the molar composition 1:9.”), where said solution is further added with stirring, and a subsequent drying process (Paragraph 0097, “While keeping the pH constant, the Sb/Sn solution is added with stirring. After a further 15 minutes of stirring, the solid is filtered off and washed with DM water, subsequently dried in a drying cabinet, and calcined in air at 500.degree. C.”). Accordingly, where Klose-Schubert discloses stirring, said stirring results in a homogeneous mixture, and where said process includes a drying of the solution to produce a final product characterized by relative wt% (Paragraph 0098-0100, “The support material has the following characteristics: Sb/SnOx content: 95.0 wt % TiO2 content: 5 wt %”), the product of Klose-Schubert therefore includes structure where the at least one first metallic elements are present in a solid homogeneous solution, where the first metallic elements are Sb and Sn.
Here, where the first metallic elements are present in a solid homogeneous solution, they therefore read upon the limitation of the instant claim which requires that the at the first metallic elements in the carrier metal oxide are each present in a same solid homogenous solution.
Additionally, Klose Schubert further presents that their invention teaches structure evidenced by an embodiment which comprises Pt nanoparticles deposited on the surface of the support material (Paragraph 0103, “To deposit the Pt particles, 6.75 g (dry mass) of the solid obtained is dispersed in 600 ml of DM water, and the dispersion is heated to 80° C. and admixed dropwise with 7.78 g of bis(ethanolamine)Pt(IV)(OH)6 (9.63 wt % Pt; Umicore, Hanau). Subsequently, 36 ml of buffer solution (sodium acetate/acetic acid, see ex. 1) are added in order to bring the mixture to a pH of 5.”). Here, where the material of the nanoparticles of the catalytically active material is purely that of the metal of the catalytically active material (Paragraph 0103, “The mean particle size of the Pt particles is 4 nm (measured using XRD).”), the composition of the deposited catalytically active particles can be understood to be a solid stoichiometric compound, having a stoichiometric ratio that is purely the catalytically active metal material, thereby representing structure which comprises the at least one second metallic element present in a solid stoichiometric compound.
Here, where the second metallic element is present in a solid stoichiometric compound, it is therefore present in a same solid stoichiometric compound as itself, reading upon the limitation of the instant claim which requires that the at least one second metallic element in the catalyst material be present in a same solid stoichiometric compound.
Here, though Klose-Schubert is silent in regards to the conductivity of the catalytically active material, where their invention is directed towards an electrocatalyst comprising an electrically conductive substrate (Abstract, “containing an electrically conductive substrate and a catalytically active species,) it would be obvious to one ordinarily skilled in the art to select a catalytically active material which has a conductivity at least equal to the conductivity of the carrier material, as discussed above, thereby reading upon and making obvious the scope of the instant limitation. Additionally, Klose-Schubert discloses structure where the catalyst material has at least one second metallic element from the group of non-precious metals (Paragraph 0042, “Such alloys comprise alloys of the noble metals with one another (for example platinum/ruthenium or platinum/gold) or those with base metals selected from the group vanadium, chromium, manganese, iron, cobalt, nickel, copper and zinc.”). Here, the catalyst material and the carrier material differ from each other in their composition, where the carrier material is a combination of multiple oxides, as discussed above, while the catalyst material is an oxidized alloy.
Additionally, Klose-Schubert fails to disclose structure where the carrier metal oxide and the catalyst material are each stabilized with fluorine. Therefore, we look to Kumta, which discloses electrocatalyst compositions (Abstract, “The invention provides electro-catalyst compositions”). Here, Kumta discloses that doping the crystal structure of their catalyst material with fluorine has a positive impact on the electrical activity of the solid material, and further improves the electronic conductivity and the electrochemical stability (Paragraph 0221, “The binding energy of Ir4f, Sn3d and O1s core level increased by ˜0.5V, an indirect reflection of the stronger binding likely due to the higher electro-negativity of fluorine incorporated into the lattice. F incorporation clearly had a net positive impact on the electrochemical activity of (Sn,Ir)O2:F solid solution most likely attributed to the improved electronic conductivity and the electrochemical stability.”). Accordingly, it would be obvious to one ordinarily skilled in the art to introduce fluorine dopants to the invention of Klose-Schubert in both the carrier material and the catalytically active material, to improve stability and increase the electronic conductivity.
Additionally, Klose-Schubert discloses that the pH of the carrier metal oxide solution prior to mixing with the catalyst material falls within a range of 6 to 10 (Paragraph 0083, “The suspension is then heated to 70 to 100° C. and IrO2 is subsequently precipitated out by controlled addition of aqueous alkali metal hydroxide solution, whereby the pH has to be adjusted within a range from 6 to 10.”), where the pH of the solution would be the pH of the solid material if it were returned to a form at which pH could be measured, that being the most recent form of the material from which a pH value could be obtained. Klose-Schubert further discloses structure where the pH of the catalyst material solution has a pH of 5 (Paragraph 0088, “Subsequently, about 3.6 ml of a buffer solution (prepared from 108.8 g of sodium acetate trihydrate, 252.2 g of acetic acid (100%) and 4.64 l of DM water) are added in order to bring the mixture to a pH of 5.”), where the pH of the solution would be the pH of the solid material if it were returned to a form at which pH could be measured, that being the most recent form of the material from which a pH value could be obtained. Therefore, the near-surface pH value, where the near-surface pH value is a pH value obtained through the solvation of a sample of the surface of the material, would differ between the carrier material and the catalyst material. Additionally, as discussed above, the catalyst material has a pH is 5, thereby reading upon the scope of the instant limitation, wherein said value of either the carrier metal oxide or the catalyst material is at most 5.
Additionally, in regards to the limitation which requires structure wherein the pH of the catalyst material or carrier metal is at most 5, Klose-Schubert fails to disclose said structure, disclosing that the carrier metal oxide has a pH of 7.5 (Paragraph 0083, “After 4 hours of stirring at 70° C., the suspension is titrated to pH 7.5 with 20% HCl solution”).
Accordingly, we look to Raiford, which discloses structure which comprises a proton exchange membrane comprising a catalyst system (Abstract, “A proton exchange membrane and a membrane electrode assembly for an electrochemical cell such as a fuel cell are provided. A catalytically active component is disposed within the membrane electrode assembly. The catalytically active component comprises particles containing a metal oxide such as silica, metal or metalloid ions such as ions that include boron, and a catalyst.”). Here, Raiford further discloses that their process comprises a pH less than 5 (Paragraph 0053, “The pH of the solution was measured to be approximately 10.2. With continued pH monitoring, small amounts of the acid-state ion-exchange resin were added, while allowing the pH to stabilize in between additions. Additional resin was added in small portions until the pH had dropped to pH 1.90-2.20.”), where said pH is a pH measured before a doping step, occurring in step 1 of Raiford’s manufacturing process, where doping occurs in step 2 of their manufacturing process (Paragraph 0055, “For each example, the metal salt specified in Table 1 for Examples (1-6) was added to one of the beakers under agitation to form a dispersion of bimetallic surface-modified silica.”). Additionally, Raiford discloses that their examples discussed in figure 1 comprise a significantly reduced fluoride emission, their other examples, as displayed in their table 3, correlated with the pH of the composition. Accordingly, where the combination of Klose-Schubert and Kumta discussed above comprises fluoride components which facilitate stability, it would therefore be obvious to one ordinarily skilled in the art to select the pH of the Raiford throughout their process, maintaining a low pH, so as to minimize the emission of fluoride components, thereby preserving the stability benefits of the fluoride components, accordingly making obvious to one ordinarily skilled in the art structure wherein the pzzp value of either the carrier metal or the catalyst material is at most pH=5.
Klose-Schubert discloses structure where the catalyst material and the carrier metal oxide form an at least two-phase disperse oxide composite (Abstract, “The multi-component substrate material 0X1-0X2 has an electrical conductivity in the range ≥0.01 S/cm and is coated with catalytically active particles”), as depicted in Klose-Schubert’s figure 1, which demonstrates a three-phase composite.
Regarding Claim 2, modified Klose-Schubert makes obvious the invention of Claim 1. Additionally, Klose-Schubert discloses structure where the first metallic elements are formed by at least two metals from the group consisting of tin, tantalum, and niobium (Paragraph 0051, “[0051] For Sb/Sn oxide: SnCl4.5H2O, Sn acetate, tin(II) nitrate, SbCl3, antimony(III) nitrate, antimony(III) acetate, etc.”; Paragraph 0055, “For Nb oxide: ammonium niobate(V) oxalate”; Paragraph 0056, “For tantalum oxide: ammonium tantalate(V) oxalate”).
Regarding Claim 3, modified Klose-Schubert makes obvious the invention of Claim 2. Additionally, Klose-Schubert discloses structure wherein the first metallic elements are formed by tin and furthermore by tantalum and niobium, as discussed above (Paragraph 0051, “[0051] For Sb/Sn oxide: SnCl4.5H2O, Sn acetate, tin(II) nitrate, SbCl3, antimony(III) nitrate, antimony(III) acetate, etc.”; Paragraph 0055, “For Nb oxide: ammonium niobate(V) oxalate”; Paragraph 0056, “For tantalum oxide: ammonium tantalate(V) oxalate”).
Regarding Claim 4, modified Klose-Schubert makes obvious the invention of Claim 1. Here, Klose-Schubert discloses structure where the at least one second metallic element is formed by titanium (Paragraph 0096, “10 wt % of Pt on Sb/SnOx--TiO2”), where titanium oxide comprises the second metallic element.
Regarding Claim 5, modified Klose-Schubert makes obvious the invention of Claim 1. Additionally, Klose-Schubert is silent in regards to disclosing structure wherein the catalyst material has a structure comprising oxide grains with a grain size in the range from 1 nm to 50 nm. Therefore, we look to Naito, which discloses structure which includes an electrode which comprises inorganic oxide particles (Abstract, “containing an inorganic oxide and provided on the first surface of the first electrode to cover the first surface and the through-holes.”). Here, Naito further discloses structure where their electrode comprises oxide particles (Paragraph 0039, “Various materials may be used for the inorganic oxide. For example, titanium oxide, silicon oxide, aluminum oxide, niobium oxide, zirconium oxide, tantalum oxide, nickel oxide, tungsten oxide, zircon or zeolite may be used.”) that have a grain size of 50 nm (Paragraph 0112, “An aqueous dispersion containing titanium oxide nanoparticles having a grain size of 50 nm is applied to the first surface 21a of the first electrode 20 by screen printing.”). Here, Naito discloses that titanium oxide facilitates cation-exchange (Paragraph 0040, “easily have a negative zeta potential in an alkaline region and therefore exhibit a cation-exchange function.”). As Naito discloses this benefit, and further discloses that a specific grain size that achieves this benefit to be 50 nm, it would be obvious to one ordinarily skilled in the art to apply this grain size of Naito to the invention of Klose-Schubert, to achieve said benefit where Klose-Schubert is otherwise silent in regards to grain size, thereby reading upon the limitations of the instant claim wherein the catalyst material, which includes titanium dioxide, has a structure comprising oxide grains with a grain size in the range from 1 nm to 50 nm.
Regarding Claim 6, modified Klose-Schubert makes obvious the invention of Claim 1. Here, Klose-Schubert discloses structure where the carrier metal oxide has a first crystal lattice structure comprising first oxygen lattice sites and first metal lattice sites, here tin oxide, (Paragraph 0096, “10 wt % of Pt on Sb/SnOx--TiO2”), where the carrier metal oxide on the first metal site is doped with a coating of platinum.
Regarding Claim 8, modified Klose-Schubert makes obvious the invention of Claim 1. Here, Klose-Schubert discloses structure where the catalyst material on the second metal lattice sites is doped with titanium, where the second metal site material is titanium oxide (Paragraph 0096, “10 wt % of Pt on Sb/SnOx--TiO2”), and additionally the entire catalyst material is doped with platinum.
Regarding Claim 9, modified Klose-Schubert makes obvious the invention of Claim 1. Additionally, Klose-Schubert discloses structure where the catalyst system has platinum applied to the surface of the catalyst particles (Paragraph 0088, “Depositing the Noble Metal-Containing Particles”). Here, Klose-Schubert discloses the application of 7.78 g of a platinum-containing compound which contains 9.63% platinum (Paragraph 0103, “admixed dropwise with 7.78 g of bis(ethanolamine)Pt(IV)(OH)6 (9.63 wt % Pt; Umicore, Hanau)”) to 6.75 g of the dry mass of catalyst (Paragraph 0103, “To deposit the Pt particles, 6.75 g (dry mass) of the solid obtained”), which has a specific surface area of 78 m2/g (Paragraph 0101, “Specific surface area (BET): 78 m2/g.”). Accordingly, there are at most 0.749 grams of platinum used to coat 6.75 grams of the dry mass of the catalyst, which has a surface area of 526.6 m2. Assuming that the total mass of platinum is applied to the surface of the catalyst, there would be 0.749 grams Pt/526.6 m2 catalyst surface area, where 0.749 g/526.6 m2 = 0.00142 g/m2. Accordingly, converting the units to mg/cm2, 0.00142 g/m2 * 1000 mg/1 g * 1 m2/10,000 cm2 = 0.000142 mg/cm2. Accordingly, where this represents a situation where 100% of the platinum is applied to the surface of the catalyst material, and there may be less than complete use of the platinum, there is accordingly structure where at most 0.000142 mg/cm2 is applied to the surface of the catalyst, which reads upon the limitation of the instant claim, which requires that the platinum content is applied to the surface of the catalyst system in an amount of at most 0.1 mg/cm2.
Claim(s) 17-19 is/are rejected under 35 U.S.C. 103 as being unpatentable over Klose-Schubert (US 20140349203) and in view of Kumta (US 20170233879 A1), Naito (US 20160186335 A1), Raiford (US 20070212593 A1), and Wakizaka (US 20110183234 A1).
Regarding Claims 17, Klose-Schubert discloses a catalyst system (Abstract, “The invention relates to a carbon-free electrocatalyst for fuel cells,”) comprising an electrically conductive carrier metal oxide (Abstract, “containing an electrically conductive substrate”) which Klose-Schubert discloses to be a multicomponent support material OX1-OX2 (Paragraph 0025, “The multicomponent support material OX1-OX2”). Here, the multicomponent support material is disclosed as preferably having a conductivity greater than 1 S/cm (Paragraph 0025, “The multicomponent support material OX1-OX2 has an electrical conductivity in the range of >0.01 S/cm, preferably >0.1 S/cm and more preferably in the range of >1 S/cm.”), where Klose-Schubert further discloses a specific embodiment which has an electronic conductivity of 80 S/cm (Paragraph 0087, “Electrical conductivity: 80 S/cm (at 50 MPa)”), where high electronic conductivity is a desirable attribute in an electrically conductive carrier metal oxide, thereby making obvious the range of the instant claim, where the electrical conductivity of the electrically conductive carrier metal oxide is at least 10 S/cm.
Additionally, Klose Schubert discloses structure where the carrier metal oxide has at least two metallic elements selected from the group of non-precious elements (Paragraph 0048-0056, “Suitable OX2 precursor compounds for preparing the conductive oxides of the type include for example: […] For Sb/Sn oxide: SnCl4.5H2O…”), further disclosing a specific embodiment which comprises Sb/SnOx-TiO2 (Paragraph 0096, “10 wt % of Pt on Sb/SnOx--TiO2”).
Additionally, in regards to the limitation where the carrier metal oxide has a structure comprising oxide grains with a grain size of at least 30 nm, Klose-Schubert fails to disclose the grain size of the carrier metal oxide. Therefore, we look to Naito, which discloses structure which includes an electrode which comprises inorganic oxide particles (Abstract, “containing an inorganic oxide and provided on the first surface of the first electrode to cover the first surface and the through-holes.”). Here, Naito further discloses structure where their electrode comprises oxide particles (Paragraph 0039, “Various materials may be used for the inorganic oxide. For example, titanium oxide, silicon oxide, aluminum oxide, niobium oxide, zirconium oxide, tantalum oxide, nickel oxide, tungsten oxide, zircon or zeolite may be used.”) that have a grain size of 50 nm (Paragraph 0112, “An aqueous dispersion containing titanium oxide nanoparticles having a grain size of 50 nm is applied to the first surface 21a of the first electrode 20 by screen printing.”). Here, Naito discloses that titanium oxide facilitates cation-exchange (Paragraph 0040, “easily have a negative zeta potential in an alkaline region and therefore exhibit a cation-exchange function.”). As Naito discloses this benefit, and further discloses that a specific grain size that achieves this benefit to be 50 nm, it would be obvious to one ordinarily skilled in the art to apply this grain size of Naito to the invention of Klose-Schubert, to achieve said benefit where Klose-Schubert is otherwise silent in regards to grain size, thereby reading upon the limitations of the instant claim wherein the carrier metal, has a structure comprising oxide grains with a grain size of at least 30 nm.
Additionally, Klose-Schubert discloses structure which comprises the carrier metal oxide having a first crystal lattice structure comprising first oxygen lattice sites and first metal lattice sites (Paragraph 0096, “10 wt % of Pt on Sb/SnOx--TiO2”), here being tin oxide.
Additionally, in regards to the limitation of the instant claim which requires structure wherein the carrier metal oxide on the first oxygen lattice sites is doped with at least one element from the group consisting of carbon, Klose-Schubert fails to disclose said structure.
Therefore, we look to Wakizaka, which discloses a metal oxycarbonitride catalyst which has excellent resistance and is not corroded in acidic electrolytes (Abstract, “The invention has an object of providing catalysts that are not corroded in acidic electrolytes or at high potential, have excellent durability and show high oxygen reducing ability. An aspect of the invention is directed to a process wherein metal carbonitride mixture particles or metal oxycarbonitride mixture particles are produced from an organometallic compound of a Group IV or V transition metal, a metal salt of a Group IV or V transition metal, or a mixture of these compounds using laser light as a light source.”). Here, Wakizaka discloses the use of metal oxycarbonitride which has oxygen atoms partially substituted with single atoms of carbon and nitrogen (Paragraph 0042, “or a mixture of a metal carbonitride and a compound having a structure of an oxide of the identical metal in which part of the oxygen atoms in the oxide are partially substituted with carbon and nitrogen.”). Here, Wakizaka further discloses that metal oxycarbonitride particles have benefits in regards to having a small and uniform particle size (Paragraph 00123, “ The carbonitride mixture particles or the oxycarbonitride mixture particles obtained by the production processes of the invention have small particle diameters of 1 to 100 nm and a uniform particle size distribution and a uniform composition distribution. The particles exhibit excellent properties as various catalysts, in particular fuel cell catalysts.”), as well as enabling excellent properties as catalysts.
Accordingly, it would therefore be obvious to one ordinarily skilled in the art to make use of the teachings of Wakizaka and introduce individual unbonded carbon atoms as a dopant on the first oxygen lattice sides of the carrier metal oxide, thereby making obvious the limitation of the instant claim.
Additionally, Klose-Schubert discloses structure which comprises an electrically conductive metal-oxide catalyst material, specifically the use of noble metal-containing alloy particles (Paragraph 0042, “In a particular embodiment, noble metal-containing alloy particles may be used as the catalytically active particles. Such alloys comprise alloys of the noble metals with one another (for example platinum/ruthenium or platinum/gold) or those with base metals selected from the group vanadium, chromium, manganese, iron, cobalt, nickel, copper and zinc.”). Here, Klose-Schubert discloses that the noble metal alloy particles are dried following their deposition onto the support substrate (Paragraph 0067, “Once the noble metal particles or noble metal alloy particles have been deposited, the resulting electrocatalyst is dried. Drying is preferably effected in the range from 50 to 100.degree. C.”) where drying of an alloy which includes oxidizable metal atoms will result in oxidation, thereby inherently directing the catalytically active particles of Klose-Schubert towards a metal-oxide catalyst material.
Additionally, in regards to the limitation which requires structure where the at least one first metallic element in the carrier metal oxide is present in a solid stoichiometric compound or solid homogeneous solution, Klose-Schubert discloses structure wherein the catalyst material is presented in a solution (Paragraph 0097, “17.25 g of SbCl3 (Merck) and 1.0 l of an HCl solution (37%, Merck) diluted with DM water to 18% (m/m), are added to 238.6 g of SnCl4.5H2O (Sigma-Aldrich) in order to obtain an Sb/Sn solution having the molar composition 1:9.”), where said solution is further added with stirring, and a subsequent drying process (Paragraph 0097, “While keeping the pH constant, the Sb/Sn solution is added with stirring. After a further 15 minutes of stirring, the solid is filtered off and washed with DM water, subsequently dried in a drying cabinet, and calcined in air at 500.degree. C.”). Accordingly, where Klose-Schubert discloses stirring, said stirring results in a homogeneous mixture, and where said process includes a drying of the solution to produce a final product characterized by relative wt% (Paragraph 0098-0100, “The support material has the following characteristics: Sb/SnOx content: 95.0 wt % TiO2 content: 5 wt %”), the product of Klose-Schubert therefore includes structure where the at least one first metallic element is present in a solid homogeneous solution, where the first metallic elements are Sb and Sn
Additionally, Klose Schubert further presents that their invention teaches structure evidenced by an embodiment which comprises Pt nanoparticles deposited on the surface of the support material (Paragraph 0103, “To deposit the Pt particles, 6.75 g (dry mass) of the solid obtained is dispersed in 600 ml of DM water, and the dispersion is heated to 80° C. and admixed dropwise with 7.78 g of bis(ethanolamine)Pt(IV)(OH)6 (9.63 wt % Pt; Umicore, Hanau). Subsequently, 36 ml of buffer solution (sodium acetate/acetic acid, see ex. 1) are added in order to bring the mixture to a pH of 5.”). Here, where the material of the nanoparticles of the catalytically active material is purely that of the metal of the catalytically active material (Paragraph 0103, “The mean particle size of the Pt particles is 4 nm (measured using XRD).”), the composition of the deposited catalytically active particles can be understood to be a solid stoichiometric compound, having a stoichiometric ratio that is purely the catalytically active metal material, thereby representing structure which comprises the at least one second metallic element present in a solid stoichiometric compound.
Here, though Klose-Schubert is silent in regards to the conductivity of the catalytically active material, where their invention is directed towards an electrocatalyst comprising an electrically conductive substrate (Abstract, “containing an electrically conductive substrate and a catalytically active species,) it would be obvious to one ordinarily skilled in the art to select a catalytically active material which has a conductivity at least equal to the conductivity of the carrier material, as discussed above, thereby reading upon and making obvious the scope of the instant limitation. Additionally, Klose-Schubert discloses structure where the catalyst material has at least one second metallic element from the group of non-precious metals (Paragraph 0042, “Such alloys comprise alloys of the noble metals with one another (for example platinum/ruthenium or platinum/gold) or those with base metals selected from the group vanadium, chromium, manganese, iron, cobalt, nickel, copper and zinc.”). Here, the catalyst material and the carrier material differ from each other in their composition, where the carrier material is a combination of multiple oxides, as discussed above, while the catalyst material is an oxidized alloy.
Additionally, Klose-Schubert fails to disclose structure where the carrier metal oxide and the catalyst material are each stabilized with fluorine. Therefore, we look to Kumta, which discloses electrocatalyst compositions (Abstract, “The invention provides electro-catalyst compositions”). Here, Kumta discloses that doping the crystal structure of their catalyst material with fluorine has a positive impact on the electrical activity of the solid material, and further improves the electronic conductivity and the electrochemical stability (Paragraph 0221, “The binding energy of Ir4f, Sn3d and O1s core level increased by ˜0.5V, an indirect reflection of the stronger binding likely due to the higher electro-negativity of fluorine incorporated into the lattice. F incorporation clearly had a net positive impact on the electrochemical activity of (Sn,Ir)O2:F solid solution most likely attributed to the improved electronic conductivity and the electrochemical stability.”). Accordingly, it would be obvious to one ordinarily skilled in the art to introduce fluorine dopants to the invention of Klose-Schubert in both the carrier material and the catalytically active material, to improve stability and increase the electronic conductivity.
Additionally, Klose-Schubert discloses that the pH of the carrier metal oxide solution prior to mixing with the catalyst material falls within a range of 6 to 10 (Paragraph 0083, “The suspension is then heated to 70 to 100° C. and IrO2 is subsequently precipitated out by controlled addition of aqueous alkali metal hydroxide solution, whereby the pH has to be adjusted within a range from 6 to 10.”), where the pH of the solution would be the pH of the solid material if it were returned to a form at which pH could be measured, that being the most recent form of the material from which a pH value could be obtained. Klose-Schubert further discloses structure where the pH of the catalyst material solution has a pH of 5 (Paragraph 0088, “Subsequently, about 3.6 ml of a buffer solution (prepared from 108.8 g of sodium acetate trihydrate, 252.2 g of acetic acid (100%) and 4.64 l of DM water) are added in order to bring the mixture to a pH of 5.”), where the pH of the solution would be the pH of the solid material if it were returned to a form at which pH could be measured, that being the most recent form of the material from which a pH value could be obtained. Therefore, the near-surface pH value, where the near-surface pH value is a pH value obtained through the solvation of a sample of the surface of the material, would differ between the carrier material and the catalyst material. Additionally, as discussed above, the catalyst material has a pH is 5, thereby failing to read upon the scope of the instant limitation, wherein said value of either the carrier metal oxide or the catalyst material is at most 3.
Accordingly, we look to Raiford, which discloses structure which comprises a proton exchange membrane comprising a catalyst system (Abstract, “A proton exchange membrane and a membrane electrode assembly for an electrochemical cell such as a fuel cell are provided. A catalytically active component is disposed within the membrane electrode assembly. The catalytically active component comprises particles containing a metal oxide such as silica, metal or metalloid ions such as ions that include boron, and a catalyst.”). Here, Raiford further discloses multiple examples which present a pH value less than 3, depicted in their Table 1, where their examples 5, 6, and 8 have pH values of 2.0, 1.5, and 1.15 respectively. Additionally, Raiford discloses that these examples display significantly reduced fluoride emission compared to their other examples, as displayed in their table 3. Accordingly, where the combination of Klose-Schubert and Kumta discussed above comprises fluoride components which facilitate stability, it would therefore be obvious to one ordinarily skilled in the art to select the pH of Raiford, so as to minimize the emission of fluoride components, thereby preserving the stability benefits of the fluoride components, accordingly making obvious to one ordinarily skilled in the art structure wherein the pzzp value of either the carrier metal or the catalyst material is at most pH=3.
Klose-Schubert further discloses structure where the catalyst material and the carrier metal oxide form an at least two-phase disperse oxide composite (Abstract, “The multi-component substrate material 0X1-0X2 has an electrical conductivity in the range ≥0.01 S/cm and is coated with catalytically active particles”), as depicted in Klose-Schubert’s figure 1, which demonstrates a three-phase composite.
Regarding Claim 18, modified Klose-Schubert makes obvious the invention of Claim 17. As discussed above, Wakizaka makes obvious structure where the carrier metal oxide on the first oxygen lattice side is doped with unbonded carbon atoms, teaching the benefits of metal oxycarbonitrides (Abstract, “The invention has an object of providing catalysts that are not corroded in acidic electrolytes or at high potential, have excellent durability and show high oxygen reducing ability. An aspect of the invention is directed to a process wherein metal carbonitride mixture particles or metal oxycarbonitride mixture particles are produced from an organometallic compound of a Group IV or V transition metal, a metal salt of a Group IV or V transition metal, or a mixture of these compounds using laser light as a light source.”).
Regarding Claim 19, modified Klose-Schubert makes obvious the invention of Claim 17. Klose-Schubert discloses structure wherein the catalyst material is presented in a solution (Paragraph 0097, “17.25 g of SbCl3 (Merck) and 1.0 l of an HCl solution (37%, Merck) diluted with DM water to 18% (m/m), are added to 238.6 g of SnCl4.5H2O (Sigma-Aldrich) in order to obtain an Sb/Sn solution having the molar composition 1:9.”), where said solution is further added with stirring, and a subsequent drying process (Paragraph 0097, “While keeping the pH constant, the Sb/Sn solution is added with stirring. After a further 15 minutes of stirring, the solid is filtered off and washed with DM water, subsequently dried in a drying cabinet, and calcined in air at 500.degree. C.”). Accordingly, where Klose-Schubert discloses stirring, said stirring results in a homogeneous mixture, and where said process includes a drying of the solution to produce a final product characterized by relative wt% (Paragraph 0098-0100, “The support material has the following characteristics: Sb/SnOx content: 95.0 wt % TiO2 content: 5 wt %”), the product of Klose-Schubert therefore includes structure where the at least one first metallic elements are present in a solid homogeneous solution, where the first metallic elements are Sb and Sn.
Here, where the first metallic elements are present in a solid homogeneous solution, they therefore read upon the limitation of the instant claim which requires that the at the first metallic elements in the carrier metal oxide are each present in a same solid homogenous solution.
Additionally, Klose Schubert further presents that their invention teaches structure evidenced by an embodiment which comprises Pt nanoparticles deposited on the surface of the support material (Paragraph 0103, “To deposit the Pt particles, 6.75 g (dry mass) of the solid obtained is dispersed in 600 ml of DM water, and the dispersion is heated to 80° C. and admixed dropwise with 7.78 g of bis(ethanolamine)Pt(IV)(OH)6 (9.63 wt % Pt; Umicore, Hanau). Subsequently, 36 ml of buffer solution (sodium acetate/acetic acid, see ex. 1) are added in order to bring the mixture to a pH of 5.”). Here, where the material of the nanoparticles of the catalytically active material is purely that of the metal of the catalytically active material (Paragraph 0103, “The mean particle size of the Pt particles is 4 nm (measured using XRD).”), the composition of the deposited catalytically active particles can be understood to be a solid stoichiometric compound, having a stoichiometric ratio that is purely the catalytically active metal material, thereby representing structure which comprises the at least one second metallic element present in a solid stoichiometric compound.
Here, where the second metallic element is present in a solid stoichiometric compound, it is therefore present in a same solid stoichiometric compound as itself, reading upon the limitation of the instant claim which requires that the at least one second metallic element in the catalyst material be present in a same solid stoichiometric compound.
Conclusion
Applicant's amendment necessitated the new ground(s) of rejection presented in this Office action. Accordingly, THIS ACTION IS MADE FINAL. See MPEP § 706.07(a). Applicant is reminded of the extension of time policy as set forth in 37 CFR 1.136(a).
A shortened statutory period for reply to this final action is set to expire THREE MONTHS from the mailing date of this action. In the event a first reply is filed within TWO MONTHS of the mailing date of this final action and the advisory action is not mailed until after the end of the THREE-MONTH shortened statutory period, then the shortened statutory period will expire on the date the advisory action is mailed, and any nonprovisional extension fee (37 CFR 1.17(a)) pursuant to 37 CFR 1.136(a) will be calculated from the mailing date of the advisory action. In no event, however, will the statutory period for reply expire later than SIX MONTHS from the mailing date of this final action.
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/J.W.E./Examiner, Art Unit 1725
/BASIA A RIDLEY/Supervisory Patent Examiner, Art Unit 1725