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 .
Priority
Receipt is acknowledged of certified copies of papers required by 37 CFR 1.55.
Information Disclosure Statement
The information disclosure statement (IDS) submitted on 05/09/2024, 06/09/2025 and 09/17/2025 are in compliance with the provisions of 37 CFR 1.97. Accordingly, the information disclosure statement is being considered by the examiner.
Drawings
The drawings received September, 05 2024 are acceptable.
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 3 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 3 recites the limitation "the nitrogen precursor" in the 13. There is insufficient antecedent basis for this limitation in the claim as “a nitrogen precursor” is introduced in claim 2 and this claim is dependent on claim 1. For the purpose of examination, it will be assumed that claim 3 is dependent on claim 1.
Claim Rejections - 35 USC § 102
The following is a quotation of the appropriate paragraphs of 35 U.S.C. 102 that form the basis for the rejections under this section made in this Office action:
A person shall be entitled to a patent unless –
(a)(1) the claimed invention was patented, described in a printed publication, or in public use, on sale, or
otherwise available to the public before the effective filing date of the claimed invention.
Claims 1, 2, 6, 7, 8 and 13 are rejected under 35 U.S.C. 102(a)(1) as being anticipated by Kim (WO 2019132281 A1, disclosed in IDS citations from enclosed machine translation) hereinafter referred to as KIM.
Regarding Claim 1, KIM teaches A catalyst for a fuel cell, (p. 2, [0001], lines 10-11) comprising: a second composite in which a plurality of first composites (Figs. 1-4; 1& 2) comprising a support (carrier, 1) and metal catalyst particles (2) supported on the support (Fig. 1; p.8, [0011], lines 1-5), are aggregated; (Figs. 1-4) and a nitrogen-containing protective layer (p. 29, [0061], lines 26-29) coated on the surface of the second composite (Fig. 4; p.28, [0059], lines 27-29).
Regarding Claim 2, KIM teaches the catalyst for a fuel cell of claim 1 (see above), wherein the nitrogen-containing protective layer is derived from a nitrogen precursor phthalocyanine or M-phthalocyanine (Fig. 4; p.28, [0059], lines 27-29).
Regarding Claim 6, KIM teaches the catalyst for a fuel cell of claim 1 (see above), wherein the nitrogen-containing protective layer is prepared using anyone selected from the group consisting of a ball mill, a powder mixer, a resonant acoustic mixer (RAM), and a combination thereof (p. 42, [0083], lines 25-26).
Regarding Claim 7, KIM teaches A method for preparing a catalyst for a fuel cell (p. 39, [0078], line 29), comprising: (S1) preparing a first mixture by adding a first composite (metal particle supported on a carrier) and a nitrogen precursor (phthalocyanine, M-phthalocyanine) to a reaction container and stirring them (ps. 39-40, [0078]); and (S2) heat-treating the stirred first mixture (p. 47, [0091], lines 15-18) wherein the first composite comprises a support and metal catalyst particles supported on the support (p. 50, [0096], lines 1-5).
Regarding Claim 8, KIM teaches the method of claim 7 (see above), and Kim further teaches wherein the step (S1) is a step where any one selected from the group consisting of a ball mill, a powder mixer, a resonant and a combination thereof is used (p. 42, [0083], lines 25-26).
Regarding Claim 13, KIM teaches A catalyst layer 30, 30’ (Fig. 5; p. 73, [0138], line 10) comprising the catalyst for a fuel cell (p. 76, [0143], lines 15-16) according to claim 1 (see above); and an ionomer (p. 62, [0116], lines 1-1) as an electrode assembly.
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.
Claim 3 is rejected under 35 U.S.C. 103 as being unpatentable over KIM as applied to claim 1 above, and further in view of Shul et al. (KR 20170054145 A, disclosed in IDS citations from enclosed machine translation) hereinafter referred to as SHUL.
Regarding Claim 3, KIM teaches the catalyst for a fuel cell of claim 1 (Figs. 1-4; ps. 8-9, [0011-0013]).
KIM does not explicitly teach an alternative to the nitrogen precursor, besides different components of M-phthalocyanine and the selection of the transition metal M (p. 11, [0019], lines 16-17).
SHUL does teach the limitations, wherein the nitrogen precursor is anyone selected from the group consisting of melamine, 2-cyanoguanidine (an alternative name for dicyandiamide or DCDA), and a combination thereof where the protective layer can be formed using one or more of dicyandiamide (DCDA), tetrazol, aminotetrazole, methylamine, guanidine, methyl hydrazine, acetonitrile, triazole, dimethylamine, ethylamine, dimethyl hydrazine, ethylenediamine, triazine, acrylonitrile, pyrazole, melamine, pyrrole, and pyridine (p. 15, [0030], 10-13). Shul further teaches that the protective layer comprising of nitrogen-doped carbon using ethylenediamine serves to improve the dispersion of catalyst particles, wettability and hydrophilicity of the carbon support (p. 16, [0032], lines 1-4).
SHUL does not explicitly teach cyanamide or urea, but a skilled artisan would find it obvious that DCDA is a dimer of cyanamides and one can substitute any manner of disclosed nitrogen compounds for urea as it is a simple amide of carbamic acid. The substitution of compounds would serve the same purpose to form the nitrogen protective layer.
Further, both KIM and SHUL are considered analogous in the art as both inventions are directed towards catalysts comprising a support, metal particles and a nitrogen containing protective layer.
Therefore, it would have been obvious before the effective filing date of the claimed invention to one of ordinary skill in the art to take the catalyst construction of KIM already utilizing phthalocyanine as the nitrogen source and to try the nitrogen precursors taught by Shul. Further, a skilled artisan would find it obvious to try: 1) to use cyanamide, as the dimeric form (DCDA) is already being used and 2) substitute, the smaller nitrogen compounds (guanidine or acrylonitrile) with urea to improve the effective catalytic active area and the durability of the catalyst as a whole (p. 16, [0032], lines 4-6) as the physical characteristics (hydrophilicity/hydrophobicity/heat of vaporization/etc.) of the nitrogen containing compounds are known.
Claim 4 is rejected under 35 U.S.C. 103 as being unpatentable over KIM as applied to claim 1 above, and further in view of NUKUI et al. (JP 2009125693 A, citations from enclosed machine translation) hereinafter referred to as NUKUI.
Regarding Claim 4, KIM teaches the catalyst for a fuel cell of claim 1 (Figs. 1-4; ps. 8-9, [0011-0013]), wherein a thickness of the nitrogen-containing protective layer is 5 nm to 70 nm. That is the coating layer and is 0.1 nm to 7 nm (p. 11, [0020], line 30). KIM further teaches by making the thickness of the coating layer as thin as possible the durability of the catalyst can be improved without reducing activity of the catalyst (p. 36, [0071], lines 7-12).
In the alternative, NUKUI does teach that when the surface irregularities of the particles the coating layer thickness via polymer is 50 nm or less is preferable, and 20 nm or less is even better (p. 27, [0039], lines 10-11). NUKUI further teaches that although in a particulate or fibrous catalyst the thickness of the nitrogen layer’s conductivity is enhanced by carbonization treatment that ideally the thinner the layer the better for maintaining high conductivity (p. 27, [0039], lines 5-7).
Further KIM and NUKUI are considered analogous in the art as both inventions are directed towards a catalyst prepared with a nitrogen protective layer that undergoes heating treatments to enhance/preserve the catalysts’ conductivity.
Therefore, before the effective filing date of the claimed invention to one of ordinary skill in the art it would have been obvious to try to modify the range taught by KIM in view of the more closely overlapping range of NUKUI, through a matter of routine experimentation to account for the variances in surface irregularities of the materials and to maintain sufficient conductivity and protection of the catalyst.
Claim 5 is rejected under 35 U.S.C. 103 as being unpatentable over KIM as applied to claim 1 above, and further in view of LEE et al. (Applied Catalysis B: Environmental 237 (2018) 318–326, disclosed in IDS) hereinafter referred to as LEE ‘18.
Regarding Claim 5, KIM teaches the catalyst for a fuel cell of claim 1 (Figs. 1-4; ps. 8-9, [0011-0013]).
KIM does not teach the composition of a nitrogen precursor besides M-phthalocyanine or phthalocyanine.
LEE ‘18 does teach wherein the nitrogen-containing protective layer comprises graphitic carbon nitride (p. 318, abstract). Lee ’18 further teaches that the a support made of amorphous carbon black (a-CB) is susceptible to electrochemical corrosion in the operating conditions of PEMFCs where the surface defects and catalyst support interactions are the most influential factors and as such, a more electrochemically stable support can be achieved with the preparation of thin, layered polymeric graphitic carbon nitride (pg-CN) coatings (pgs. 318-319, Introduction, paragraphs 4-6).
Further, the disclosure of LEE ‘18 and KIM are considered analogous in the art as they are both directed towards the carbon support of a fuel cell catalyst molecule and the nitrogen-protective layer coating.
Therefore, it would have been obvious before the effective filing date of the claimed invention to one of ordinary skill in the art to substitute the phthalocyanine of KIM with the graphitic carbon nitride of Lee ’18 to produce a more electrochemically stable support despite surface defects that arise from synthesis and manufacture.
Claims 9 and 12 are rejected under 35 U.S.C. 103 as being unpatentable over KIM as applied to claim 7 above, and further in view of Lee et al. (US 20210359311 A1) hereinafter referred to as LEE ‘21.
Regarding Claim 9, KIM teaches the method of claim 7 (see above) of wherein the step (S2) comprises a first heat treatment step for carbonization of the coating layer (p. 16, [0030]) with a temperature range of 400 °C to 800 °C (p. 53, [0102], lines 20-21). KIM further teaches that the thickness of the coating layer and the length, diameter, and structure of any of the carbon supports and mixtures can be controlled by changing the type, content, heat treatment temperature/time/atmosphere of any of the group of nitrogen precursors and mixtures thereof (p. 51, [0098]).
Kim does not teach a second heat treatment step or the parameters thereof.
In the same field of endeavor, LEE ’21 does teach a second heat treatment step S5 (Tertiary Heat Treatment, Fig. 5), which is different from the first heat treatment step S2 (Primary Heat Treatment, Fig. 5). Where the three different heat treatment steps are necessary to prepare a catalyst by first preparing a carbon support with the precursor, subject the support to a second heat treatment, purify/acid treat the support and prepare a composite catalyst with the third heat treatment (p. 1, [0017]).
A skilled artisan would find it obvious to include another heat treatment step as an improvement on the preparation of the nitrogen protective layer catalyst of KIM, as a different range of time and temperature would affect the nitrogen protective layer and the catalyst as whole. Further the omission of the second heat treatment step of LEE ’21 would be obvious if the catalyst does not require a purification or acid wash step, but additional heat treatment steps could be applied as necessary.
Regarding Claim 12 KIM teaches the method of claim 7 (p. 39, [0078], line 29).
KIM does not teach content of the nitrogen precursor is 80 to 200 parts by weight based on 100 parts by weight of the support; KIM only teaches that the overall content of the coating layer may be 5% to 30% by weight with respect to the total weight of the catalyst (p. 36, [0072], 25-26). Kim further teaches that the content of the coating layer is important as less than the range would result in uncoated areas and if the weight percentage is higher than the thickness of the coating layer may be too thick, inhibiting the activity of the catalyst (pgs. 36-37, [0072]).
LEE ’21 does teach the limitation, in particular LEE ’21 teaches the weight ratio of the support (100), and the nitrogen precursor is 1:1 to 1:3 which corresponds to 100 to 300 parts of nitrogen based on 100 parts of support (p. 4, [0082], lines 17-19). A skilled artisan would find it obvious that the ratio would depend on the molecular weight/composition of the precursor and the desired thickness.
Further, LEE ’21 is considered analogous in the art to KIM both inventions are directed towards a catalyst for a fuel cell that has a nitrogen protective layer and the method for preparing the same.
Therefore, it would have been obvious before the effective filing date of the claimed invention to one of ordinary skill in the art to combine the final weight percentages of nitrogen coating the support as taught by KIM and the range of as taught by LEE ’21. Further, it would be obvious to try to determine the optimal ratio of precursor to support as taught by LEE ’21 by routine experimentation of adjusting both composition of the precursor or the amount of precursor added to achieve a final nitrogen weight percentage of the coating layer to adequately cover the metal particles and maintain conductivity.
Claims 10 and 11 are rejected under 35 U.S.C. 103 as being unpatentable over KIM modified by LEE ‘21 as applied to claim 9 above, and further in view of LEE '18.
Regarding Claim 10 KIM teaches the method of claim 9 (p. 16, [0030]) and in a first non-reactive gas atmosphere argon or argon-hydrogen atmosphere (p. 16, [0032], lines 33-34). KIM also teaches a temperature range, 400 – 800 °C, and time range, 5 – 60 minutes. KIM further teaches that the thickness of the coating layer and the length, diameter, and structure of any of the carbon supports and mixtures can be controlled by changing the type, content, heat treatment temperature/time/atmosphere of any of the group of nitrogen precursors and mixtures thereof (p. 51, [0098]).
KIM does not teach wherein the first heat treatment step is a step of heat treatment at 150 °C to 250 °C for 0.5 to 3 hours or a second heating step and the parameters thereof.
LEE ’21, teaches these parameters, specifically the temperature range of the first heat treatment step of 140 °C to 180 °C and the time range of 30 min (0.5) to 5 hours (p. 4, [0083], line 21). A skilled artisan would find it obvious to adjust the temperature and the time of heating to achieve a coating with the desired thickness on the carbon support.
LEE ’21 further teaches and the second heat treatment step (p. 5, [0109], lines 13-15) but does not explicitly teach the claimed time and temperature but a much shorter time of heating and a broader temperature range, 10 to 60 min and 300 – 600 °C respectively.
LEE ’18 teaches a step of heat treatment at 500°C to 600°C 550 °C for 1 to 5 hours 4 hours in a second non-reactive gas atmosphere argon gas (p. 319, Results and Discussion, paragraph 1). It is noted that where the claimed ranges overlap or lie inside ranges disclosed by the prior art, a prima facie case of obviousness exists. See MPEP 2144.05.
Further KIM, LEE ’21, and LEE ’18 are analogous to the claimed invention as all three are directed towards catalysts of a carbon support with a metal particle and nitrogen protective layer.
Therefore, it would have been obvious before the effective filing date of the claimed invention to one of ordinary skill in the art to take the multiple heat treatment steps of LEE ’21, including the second heat treating step of LEE ’18 and apply them to the method of mixing and preparation of KIM. Further, a skilled artisan would find it obvious to adjust heating temperatures, times, and nitrogen precursor through routine experimentation to achieve a nitrogen-protective layer of appropriate thickness.
Regarding Claim 11 KIM modified by LEE ’21 & LEE ‘18 teaches the method of claim 10 (see above rejection). KIM further teaches the first non-reactive gas and the second non-reactive gas are each independently any one selected from the group consisting of nitrogen, argon, helium, and a combination thereof the above inert gas may be any one selected from the group consisting of nitrogen, helium, argon, neon, krypton, xenon, radon, and mixtures thereof, and the above reducing gas may be a hydrogen mixture (p. 51, [0099]). As stated above KIM teaches that the atmosphere of the heating step can affect the thickness of the coating layer (p. 51, [0098], line 5) and further that an argon hydrogen mixed atmosphere the heteroparticles of a transition metal may be partially doped into the carbon depending on the transition metal of M-phthalocyanine (p. 52, [0100], lines 12-15).
Thus, it would be obvious to independently select a non-reactive gas mixture for each discrete heating step as the substitution of inert gases and mixtures thereof as a skilled artisan would find it obvious to try the combinations to control the type of particles in the protective layer.
Conclusion
The prior art made of record and not relied upon is considered pertinent to applicant's disclosure. Long et al. (CN 110729495 A).
Any inquiry concerning this communication or earlier communications from the examiner should be directed to WAYNE WALTER VIGIL JR whose telephone number is (571)270-7652. The examiner can normally be reached Monday - Friday 8:30 am - 5:00 pm.
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If attempts to reach the examiner by telephone are unsuccessful, the examiner’s supervisor, Abbas Rashid can be reached at (571) 270-7457. The fax phone number for the organization where this application or proceeding is assigned is 571-273-8300.
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/WAYNE WALTER VIGIL/Examiner, Art Unit 1748
/Abbas Rashid/Supervisory Patent Examiner, Art Unit 1748
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