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 .
Election/Restrictions
Applicant's election with traverse of Group I, claims 1-17 in the reply filed on 12/12/2025 is acknowledged. The traversal is on the ground(s) that the shared technical feature is the method of claim 1 and that there would not be additional burden for the Examiner to search all of the claims. This is not found persuasive for the following reasons.
Applicant primarily argues:
“Respectfully, Groups I and II have unity of invention because they both require a method for producing a carrier-free oxygen reduction catalyst containing the indicated sequence of steps specifically defined in claim 1, which is not taught or suggested by Tran cited in the Office Action.”
Remarks, p. 2
The examiner respectfully traverses as follows:
While Group II, claims 18-19 recites “produced as claimed in claim 1”, this is a product-by-process limitation and does not limit the claim. Rather, any carrier-free oxygen reduction catalyst would meet the limitation of claim 18. Therefore, the method of claim 1 is not required by Group II and the shared technical feature between Groups I and II is a carrier-free oxygen reduction catalyst.
Applicant further argues:
“Still further, as non-elected claim 18-19 require all of the limitations of claim 1, it would additionally not be a burden for the Examiner to examine said claims once claim 1 is found allowable.”
Remarks, p. 2
The examiner respectfully traverses as follows:
This is not found persuasive because the instant application is a national stage entry filed under 35 U.S.C. 371 and is therefore not subject to US restriction practice but rather subject to lack of unity practice, see MPEP 1893.03(d). It is noted that undue search burden is not a criterion in lack of unity analysis. The test is whether or not special technical features can be established. It is noted that inventions listed as Groups I and II do not relate to a single general inventive concept under PCT Rule 13.1 because, under PCT Rule 13.2, they lack the same or corresponding special technical features as set forth on page 4 of the previous Office Action.
Therefore, given that the Examiner has properly established that Groups I and II lack unity as set forth in page 4 of the Office Action mailed 11/12/2025, it is the Examiner's position that the restriction is proper.
The requirement is still deemed proper and is therefore made FINAL.
Claims 18-19 are withdrawn from further consideration pursuant to 37 CFR 1.142(b), as being drawn to a nonelected invention, there being no allowable generic or linking claim. Applicant timely traversed the restriction (election) requirement in the reply filed on 12/12/2025.
Claim Objections
Claims 3-4, 8, and 17 are objected to because of the following informalities:
In order to ensure proper antecedent basis, it is suggested to amend “the molar ratio” to “a molar ratio” in line 2 of each of claims 3 and 4.
In order to ensure proper antecedent basis, it is suggested to amend “the weight ratio” to “a weight ratio” in claim 8, line 2.
In order to ensure proper Markush group language, it is suggested to amend “is selected from N2/H2, H2, CO2, NH3” to “is selected from the group consisting of N2/H2, H2, CO2, and NH3” in claim 17, lines 3.
Appropriate correction is required.
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 5, 7, 13 and 15 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.
Regarding claim 5, the phrase “in particular” renders the claim indefinite because it is unclear whether the limitation(s) following the phrase are part of the claimed invention. See MPEP § 2173.05(d).
Regarding claim 7, the phrases “in particular” and "preferably" render the claim indefinite because it is unclear whether the limitation(s) following the phrase are part of the claimed invention. See MPEP § 2173.05(d).
Regarding claim 13, the phrase “in particular” renders the claim indefinite because it is unclear whether the limitation(s) following the phrase are part of the claimed invention. See MPEP § 2173.05(d).
Regarding claim 15, the phrases “such as” and "for example" render the claim indefinite because it is unclear whether the limitation(s) following the phrase are part of the claimed invention. See MPEP § 2173.05(d).
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.
Claims 1-8, 10 and 15-16 are rejected under 35 U.S.C. 103 as being unpatentable over Tran et al. (“Iron–polypyrrole electrocatalyst with remarkable activity and stability for ORR in both alkaline and acidic conditions: a comprehensive assessment of catalyst preparation sequence”, 2016) (Tran) in view of Shen et al. (“In situ doping polymerization of pyrrole with sulfonic acid as a dopant”, 1998) (Shen).
Regarding claims 1 and 2, Tran teaches a method for producing an iron-polypyrrole electrocatalyst with remarkable activity and stability for oxygen reduction reactions for use in proton exchange membrane fuel cell and alkaline polymer electrolyte fuel cells known for their low operation temperature (Tran, Abstract; Introduction, Paragraph 1; p. 8646, 2.1 Material preparation) (i.e., for use in low-temperature fuel cells), wherein in the instant application “carrier-free” is defined as no carbon-based carrier materials are used, such as, for example, carbon nanotubes, graphene, graphite, carbon fibers, carbon aerogel or carbon black. Only the conductive polymer is required as a carbon source for the catalyst according to the invention with an M-N-C (i.e., metal-nitrogen-carbon) structure (Specification, [0031]). Therefore, the iron-polypyrrole electrocatalyst for oxygen reduction reactions of Tran corresponds to the carrier-free oxygen reduction catalyst for use in low-temperature fuel cells.
Tran teaches the method comprises (Tran, p. 8646, 2.1 Material preparation):
dissolving the monomer pyrrole (i.e., claim 2, nitrogenous aromatic monomer is pyrrole) in an HCl solution (i.e., producing a solution of a nitrogenous aromatic monomer which leads to conductive polymers);
adding an FeCl3 solution slowly to the mixture as an oxidant for pyrrole polymerization and stirring for 12 hours (i.e., producing a solution of an oxidizing agent, mixing the solutions and allowing the mixture to stand to produce a conductive polymer, wherein the solutions are mixed with one or more transition metal salts in order to directly obtain a precursor mixture), wherein the there would necessarily be a period of time between stirring and filtering the mixture (i.e., allowing the mixture to stand);
drying the product and then heating the product to 800, 900, and 1000°C for 1 h at a heating rate of 10°C/min in an argon atmosphere for carbonization and graphitization (i.e., pyrolysis of the precursor mixture in an inert gas atmosphere for producing the catalyst);
leaching the pyrolyzed product in 0.5 M H2SO4 (i.e., mineral acid in a solvent) followed by washing several times with ethanol (i.e., performing an acid etching step with a mixture of a mineral acid and a solvent for producing an etched catalyst);
pyrolyzing the leached product again using the same conditions (i.e., pyrolysis of the etched catalyst in an inert gas atmosphere).
However, Tran does not explicitly teach the nitrogenous aromatic monomer solution includes an aromatic sulfonic acid.
With respect to the difference, Shen teaches doping polymerization of pyrrole with sulfonic acid, including naphthalene sulfonic acid (Shen, Abstract) (i.e., claim 2, aromatic sulfonic acid is naphthalenesulfonic acid).
As Shen expressly teaches, the polypyrrole prepared by in situ doping polymerization in the presence of naphthalene sulfonic acid shows high conductivity (Shen, p. 127, Col. 2, Paragraph 2).
Shen is analogous art as it is drawn to the polymerization of the monomer pyrrole (Shen, Abstract).
In light of the motivation of doping the pyrrole with naphthalene sulfonic acid as disclosed by Shen, it therefore would have been obvious to one of ordinary skill in the art to modify the method of Tran by doping the polymerizing the pyrrole with the doping agent naphthalene sulfonic acid in order to increase the conductivity, and thereby arrive at the claimed invention.
Regarding claim 3, Tran, in view of Shen, teaches the method as claimed in claim 1, wherein the molar ratio of nitrogenous aromatic monomer to aromatic sulfonic acid is 14 mmol: 14mmol (i.e., 1:1 molar ratio) (Shen, p. 128, Col. 1, Paragraph 2), which falls within the claimed range.
Regarding claim 4, Tran, in view of Shen, teaches the method as claimed in claim 1, wherein the oxidizing agent is the 10 mL solution of FeCl3 with a 0.74 mol/L concentration, and the nitrogenous aromatic monomer is the 3.00 mL of pyrrole. Therefore, the moles of FeCl3 are 0.74 mol/L x 0.01 L (i.e., 10 mL) = 0.0074 mol oxidizing agent; and the moles of pyrrole are calculated as follows using the density of pyrrole at room temperature which is 0.967 g/mL and the molecular weight which is 67.09 g/mol: (3 mL pyrrole x 0.967 g/mL)/(67.09 g/mol) = 0.04 mol. Therefore, the molar ratio of oxidizing agent to pyrrole is 0.0074:0.04 which is approximately 1:5, which falls within the claimed range.
Regarding claims 5 and 7, Tran, in view of Shen, teaches the method as claimed in claim 1, wherein the oxidizing agent is FeCl3 (Tran, p. 8646, 2.1 Material Preparation) (i.e., claim 5, oxidizing agent is a trivalent iron salt; claim 7, the transition metal salt in steps c and d is Fe).
Regarding claim 6, Tran, in view of Shen, teaches the method as claimed in claim 1, wherein adding the oxidant to the pyrrole solution occurs at room temperature (i.e., between 20-25°C) (Tran, p. 8646, 2.1 Material Preparation), which falls within the claimed range.
Further, although there are no disclosures on the amounts of time the mixture is left to stand as presently claimed, it has long been an axiom of United States patent law that it is not inventive to discover the optimum or workable ranges of result-effective variables by routine experimentation. In re Peterson, 315 F.3d 1325, 1330 (Fed. Cir. 2003) ("The normal desire of scientists or artisans to improve upon what is already generally known provides the motivation to determine where in a disclosed set of percentage ranges is the optimum combination of percentages."); In re Boesch, 617 F.2d 272, 276 (CCPA 1980) ("[D]iscovery of an optimum value of a result effective variable in a known process is ordinarily within the skill of the art."); In re Aller, 220 F.2d 454, 456 (CCPA 1955) ("[W]here the general conditions of a claim are disclosed in the prior art, it is not inventive to discover the optimum or workable ranges by routine experimentation."). "Only if the 'results of optimizing a variable' are 'unexpectedly good' can a patent be obtained for the claimed critical range." In re Geisler, 116 F.3d 1465, 1470 (Fed. Cir. 1997) (quoting In re Antonie, 559 F.2d 618, 620 (CCPA 1977)).
At the time of the invention, it would have been obvious to one of ordinary skill in the art to vary the amounts of standing time, including over the amounts presently claimed, in order to ensure the pyrrole is fully polymerized.
Regarding claim 8, Tran, in view of Shen, teaches the method as claimed in claim 1, wherein the weight of the pyrrole is calculated using the density of pyrrole at room temperature which is 0.967 g/mL: 3 mL pyrrole x 0.967 g/mL = 2.901 g pyrrole. Further, the weight of FeCl3 is calculated using the molar mass of FeCl3 which is 162.2 g/mol: 0.74 mol/L FeCl3 x 162.2 g/mol x 0.01 L (i.e., 10 mL) = 1.2 g FeCl3. Therefore, the weight ratio of pyrrole to FeCl3 is 2.901 g: 1.2 g which equals 1: 0.4, which falls within the claimed range.
Regarding claim 10, Tran, in view of Shen, teaches the method as claimed in claim 1, wherein the pyrolysis step is heating at a rate of 10 °C/min which equals 600°C/h, which falls within the claimed range, to a temperature of 800, 900, and 1000°C for 1 hour, which falls within the claimed ranges, and is followed by cooling to room temperature (i.e., between 20-25°C), which falls within the claimed range (Tran, p. 8646, 2.1 Material Preparation).
Regarding claim 15, Tran, in view of Shen, teaches the method as claimed in claim 1, wherein leaching is performed using a 0.5 M solution of H2SO4, which falls within the claimed range, and is further washed several times with ethanol, i.e., organic solvent (Tran, p. 8646, 2.1 Material Preparation), wherein part of the washing is interpreted as part of the acid etching.
Although there are no disclosures on the volume ratio of mineral acid to solvent being 1:10 to 10:1 as presently claimed, it has long been an axiom of United States patent law that it is not inventive to discover the optimum or workable ranges of result-effective variables by routine experimentation. In re Peterson, 315 F.3d 1325, 1330 (Fed. Cir. 2003) ("The normal desire of scientists or artisans to improve upon what is already generally known provides the motivation to determine where in a disclosed set of percentage ranges is the optimum combination of percentages."); In re Boesch, 617 F.2d 272, 276 (CCPA 1980) ("[D]iscovery of an optimum value of a result effective variable in a known process is ordinarily within the skill of the art."); In re Aller, 220 F.2d 454, 456 (CCPA 1955) ("[W]here the general conditions of a claim are disclosed in the prior art, it is not inventive to discover the optimum or workable ranges by routine experimentation."). "Only if the 'results of optimizing a variable' are 'unexpectedly good' can a patent be obtained for the claimed critical range." In re Geisler, 116 F.3d 1465, 1470 (Fed. Cir. 1997) (quoting In re Antonie, 559 F.2d 618, 620 (CCPA 1977)).
At the time of the invention, it would have been obvious to one of ordinary skill in the art to vary the amounts of mineral acid to solvent, including over the amounts presently claimed, in order to effectively remove all redundant phases of unstable metallic iron and iron compounds (Tran, p. 8646, 2.1 Material Preparation).
Regarding claim 16, Tran, in view of Shen, teaches the method as claimed in claim 1, wherein following acid etching the pyrolyzed product is washed several times with deionized water and absolute ethanol and then dried (Tran, p. 8646, 2.1 Material Preparation), wherein the product is necessarily filtered in order to be washed and dried.
Further, although there are no disclosures on the amounts of time standing between acid etching and the steps of filtering, washing, and drying as presently claimed, it has long been an axiom of United States patent law that it is not inventive to discover the optimum or workable ranges of result-effective variables by routine experimentation. In re Peterson, 315 F.3d 1325, 1330 (Fed. Cir. 2003) ("The normal desire of scientists or artisans to improve upon what is already generally known provides the motivation to determine where in a disclosed set of percentage ranges is the optimum combination of percentages."); In re Boesch, 617 F.2d 272, 276 (CCPA 1980) ("[D]iscovery of an optimum value of a result effective variable in a known process is ordinarily within the skill of the art."); In re Aller, 220 F.2d 454, 456 (CCPA 1955) ("[W]here the general conditions of a claim are disclosed in the prior art, it is not inventive to discover the optimum or workable ranges by routine experimentation."). "Only if the 'results of optimizing a variable' are 'unexpectedly good' can a patent be obtained for the claimed critical range." In re Geisler, 116 F.3d 1465, 1470 (Fed. Cir. 1997) (quoting In re Antonie, 559 F.2d 618, 620 (CCPA 1977)).
At the time of the invention, it would have been obvious to one of ordinary skill in the art to vary the amounts of resting time, including over the amounts presently claimed, in order to ensure all redundant phases of unstable metallic iron and iron compounds are removed.
Claim 9 is rejected under 35 U.S.C. 103 as being unpatentable over Tran in view of Shen, as applied to claim 1 above, and further in view of Ratso et al. (“Effect of Ball-Milling on the Oxygen Reduction Reaction Activity of Iron and Nitrogen Co-doped Carbide-Derived Carbon Catalysts in Acid Media”, 2019) (Ratso).
Regarding claim 9, Tran, in view of Shen, teaches the method as claimed in claim 1, but does not explicitly teach the mixing of precursors is a mechanical mixing and is performed in a ball mill.
With respect to the difference, Ratso teaches the effect of ball-milling on the oxygen reduction reaction activity of iron and nitrogen co-doped carbide-derived carbon catalysts in acid media (Ratso, Title; Abstract). Ratso specifically teaches ball-milling the precursors (Ratso, p. 7953, 2.1. Synthesis of Iron- and Nitrogen-Doped Catalysts).
As Ratso expressly teaches, ball-milling decreases the particle size of the material and disperses reagents into the pores (Ratso, p. 7960, Conclusion).
Ratso is analogous art as it is drawn to the preparation of iron and nitrogen co-doped catalysts for oxygen reduction reactions (Ratso, Abstract).
In light of the motivation of ball-milling precursors as disclosed by Ratso, it therefore would have been obvious to one of ordinary skill in the art to modify the method of Tran, in view of Shen, by ball-milling the precursors in order to decrease the particle size and disperse reagents into the pores more effectively, and thereby arrive at the claimed invention.
Claim 11 is rejected under 35 U.S.C. 103 as being unpatentable over Tran in view of Shen, as applied to claim 10 above, and further in view of Peera et al. (“Cumulative effect of transition metals on nitrogen and fluorine co-doped graphite nanofibers: an efficient and highly durable non-precious metal catalyst for the oxygen reduction reaction”, 2016) (Peera).
Regarding claim 11, Tran, in view of Shen, teaches the method as claimed in claim 10, but does not explicitly teach wherein the obtained catalyst is fluorinated and subsequently pyrolyzed again after the pyrolysis in step g) by reaction with a fluorinating agent.
With respect to the difference, Peera teaches doping oxygen reduction reaction catalysts comprising iron with fluorine (Peera, Abstract). Peera teaches doping with fluorine and then pyrolyzing (Peera, p. 14651, Col. 2, Paragraph 3).
As Peera expressly teaches, the formed catalysts exhibited excellent ORR activity and extraordinary durability in comparison with a commercial Pt/C catalyst and complete resistance to the methanol and CO species (Peera, p. 14662, Conclusion).
Peera is analogous art as it is drawn to oxygen reduction reaction catalysts in the form of N-M-C complexes (Peera, p. 14662, Conclusion).
In light of the motivation of fluorinating the catalyst as disclosed by Peera, it therefore would have been obvious to one of ordinary skill in the art to modify the method of Tran, in view of Shen, by doping with fluorine followed by pyrolysis in order to increase activity of the ORR catalyst and exhibit complete resistance to the methanol and CO species, and thereby arrive at the claimed invention.
Claim 14 is rejected under 35 U.S.C. 103 as being unpatentable over Tran in view of Shen, as applied to claim 1 above, and further in view of Zhang et al. (“Optimization of the acid leaching process by using an ultrasonic field for metallurgical grade silicon”, 2009) (Zhang).
Regarding claim 14, Tran, in view of Shen, teaches the method as claimed in claim 1, wherein the acid etching step is performed for 8 hours at 80°C, which falls within the claimed range (Tran, p. 8646, 2.1 Material preparation). Further, Tran teaches the argon atmosphere (i.e., inert atmosphere) is used for the two preceding steps and does not teach the atmosphere is changed for the acid etching step, therefore, a person of ordinary skill in the art would continue to use the argon atmosphere for the acid etching step.
However, Tran does not explicitly teach the acid etching is performed in an ultrasound bath.
With respect to the difference, Zhang teaches acid leaching under an ultrasonic field to remove impurities (Zhang, Abstract).
As Zhang expressly teaches, the acid leaching process under an ultrasonic field is more effective than the acid leaching under magnetic stirring (Zhang, Abstract).
Zhang is analogous art as it is drawn to the acid leaching of metal impurities (Zhang, Abstract).
In light of the motivation of acid leaching/etching under an ultrasonic field (i.e., ultrasound bath) as disclosed by Zhang, it therefore would have been obvious to one of ordinary skill in the art to modify the acid etching of Tran, in view of Shen, by using an ultrasonic field in order to have a more effective acid leaching of metal impurities, and thereby arrive at the claimed invention.
Claim 17 is rejected under 35 U.S.C. 103 as being unpatentable over Tran in view of Shen, as applied to claim 1 above, and further in view of Dominguez et al. (“Effect of the pyrolysis atmosphere and nature of iron precursor on the structure and activity of Fe/N based electrocatalysts for the oxygen reduction reaction”, 2016) (Dominguez).
Regarding claim 17, Tran, in view of Shen, teaches the method as claimed in claim 1, but does not explicitly teach wherein during pyrolysis after acid etching, the reactive gas is selected from N2/H2, H2, CO2, and NH3.
With respect to the difference, Dominguez teaches the effect of the pyrolysis atmosphere on the structure and activity of Fe/N based electrocatalysts for the oxygen reduction reaction (Dominguez, Title; Abstract). Dominguez specifically teaches using reactive NH3 gas during pyrolysis (Dominguez, Abstract).
As Dominguez expressly teaches, thermal treatments under reactive atmosphere with NH3 promote the formation of micropores in the final material and improve the incorporation of nitrogen atoms in the C-C structure (Dominguez, p. 22561, Col. 2, lines 4-7).
Dominguez is analogous art as it is drawn to synthesis of Fe/N based electrocatalysts for the oxygen reduction reaction including pyrolysis steps (Dominguez, Title; Abstract).
In light of the motivation of using an NH3 atmosphere for pyrolysis as disclosed by Dominguez, it therefore would have been obvious to one of ordinary skill in the art to modify the method of Tran in view of Shen by using an NH3 atmosphere for pyrolysis in order to promote the formation of micropores in the final material and improve the incorporation of nitrogen atoms in the C-C structure, and thereby arrive at the claimed invention.
Allowable Subject Matter
Claim 12 is objected to as being dependent upon a rejected base claim, but would be allowable if rewritten in independent form including all of the limitations of the base claim and any intervening claims.
Claim 13 would be allowable if rewritten to overcome the rejection(s) under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), 2nd paragraph, set forth in this Office action and to include all of the limitations of the base claim and any intervening claims.
Tran, in view of Shen and Peera, teaches the method as claimed in claim 1, but does not explicitly teach wherein the fluorinating agent comprises a fluoride compound with a primary amino group and a nitrite compound.
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to Catriona Corallo whose telephone number is (571)272-8957. The examiner can normally be reached Monday-Friday, 8am-5pm.
Examiner interviews are available via telephone, in-person, and video conferencing using a USPTO supplied web-based collaboration tool. To schedule an interview, applicant is encouraged to use the USPTO Automated Interview Request (AIR) at http://www.uspto.gov/interviewpractice.
If attempts to reach the examiner by telephone are unsuccessful, the examiner’s supervisor, Ching-Yiu Fung can be reached at (571)270-5713. The fax phone number for the organization where this application or proceeding is assigned is 571-273-8300.
Information regarding the status of published or unpublished applications may be obtained from Patent Center. Unpublished application information in Patent Center is available to registered users. To file and manage patent submissions in Patent Center, visit: https://patentcenter.uspto.gov. Visit https://www.uspto.gov/patents/apply/patent-center for more information about Patent Center and https://www.uspto.gov/patents/docx for information about filing in DOCX format. For additional questions, contact the Electronic Business Center (EBC) at 866-217-9197 (toll-free). If you would like assistance from a USPTO Customer Service Representative, call 800-786-9199 (IN USA OR CANADA) or 571-272-1000.
/C.M.C./Examiner, Art Unit 1732
/CORIS FUNG/Supervisory Patent Examiner, Art Unit 1732