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 .
DETAILED ACTION
This Office Action is in response to the communication filed on 5/21/26. Applicant’s arguments have been considered but do not overcome all the rejections of record. The amended claims necessitated new grounds of rejection. Claims 1, 5-10 and 12-15 are pending and remain rejected.
This Action is Non-FINAL.
Continued Examination Under 37 CFR 1.114
A request for continued examination under 37 CFR 1.114, including the fee set forth in 37 CFR 1.17(e), was filed in this application after final rejection. Since this application is eligible for continued examination under 37 CFR 1.114, and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114. Applicant's submission filed on 5/21/26 has been entered.
Claims Analysis
Claim 1 recites “wherein, at a relative pressure of a nitrogen adsorption isotherm of the metal-supported catalyst within a range of 0.4 or more and 0.6 or less, a maximum value of a ratio of a nitrogen adsorption amount of a desorption-side isotherm to a nitrogen adsorption amount of an adsorption-side isotherm is 1.05 or less”, which is a method of measuring a property/structure of the claimed metal-supported catalyst. A nitrogen absorption isotherm describes (i.e., by plotting on a graph) the relationship between the amount of nitrogen gas adsorbed on a solid surface and the relative pressure at a constant temperature, typically 77 K. The present specification discloses “in the nitrogen adsorption isotherm obtained by the nitrogen adsorption method (more specifically, BET method)” [0085]. Claim 7 recites a BET specific surface area of the carbon carrier. Thus, a carbon carrier having the BET specific surface area of claim 7 would read upon the BET method of measuring using a nitrogen adsorption isotherm plot of claim 1. See also claim 8 that describes methods of measuring adsorption.
Claim 1 has been amended to recite “the average pore diameter being calculated by the following equation: average pore diameter (nm)=4x{total pore volume of the metal-supported catalyst (cm³/g-metal-supported catalyst)x10²¹}/BET specific surface area of the metal-supported catalyst (m²/g-metal-supported catalyst)x10¹⁸, the total pore volume and the BET specific surface area being obtained from the nitrogen adsorption isotherm at a temperature of 77 K obtained by a nitrogen adsorption method of the metal-supported catalyst”, which does not appear to limit the metal-supported catalyst of claim 1 as the recitation is directed to a method of measuring/calculated. The method of calculating the average pore diameter does not impart structure to the claimed metal-supported catalyst. Similarly, the method of obtaining the total pore volume and the BET specific surface area by a nitrogen adsorption method is not given patentable weight. No structure is imparted by the claimed calculating, obtaining or nitrogen adsorption method.
Claim 1 has been amended to recite “the volumes V3 and V4 being obtained from a nitrogen adsorption isotherm at a temperature of 77 K obtained by a nitrogen adsorption method of the metal-supported catalyst, and the weight ratio of the carbon carrier being calculated by the following equation: weight ratio of carbon carrier=1-(metal content (wt%) of the metal-supported catalyst obtained by inductively coupled plasma mass spectrometry)/100”, which has not been given patentable weight and does not appear to impart any structure to the claimed metal-supported catalyst. No structure is imparted by the claimed calculating, obtaining or nitrogen adsorption method.
Claim Rejections - 35 USC § 112
The following is a quotation of the first paragraph of 35 U.S.C. 112(a):
(a) IN GENERAL.—The specification shall contain a written description of the invention, and of the manner and process of making and using it, in such full, clear, concise, and exact terms as to enable any person skilled in the art to which it pertains, or with which it is most nearly connected, to make and use the same, and shall set forth the best mode contemplated by the inventor or joint inventor of carrying out the invention.
The following is a quotation of the first paragraph of pre-AIA 35 U.S.C. 112:
The specification shall contain a written description of the invention, and of the manner and process of making and using it, in such full, clear, concise, and exact terms as to enable any person skilled in the art to which it pertains, or with which it is most nearly connected, to make and use the same, and shall set forth the best mode contemplated by the inventor of carrying out his invention.
Claims 1, 5-10 and 12-15 are rejected under 35 U.S.C. 112(a) or 35 U.S.C. 112 (pre-AIA ), first paragraph, as failing to comply with the written description requirement. The claim(s) contains subject matter which was not described in the specification in such a way as to reasonably convey to one skilled in the relevant art that the inventor or a joint inventor, or for applications subject to pre-AIA 35 U.S.C. 112, the inventor(s), at the time the application was filed, had possession of the claimed invention.
Claim 1 recites ““the volumes V1 and V2 being obtained by dividing a volume V3 (cm³/g-metal-supported catalyst) of pores having a pore diameter of less than 5 nm and a volume V4 (cm³/g-metal-supported catalyst) of pores having a pore diameter of 5 nm or more, respectively, by a weight ratio of the carbon carrier included in the metal- supported catalyst, the volumes V3 and V4 being obtained from a nitrogen adsorption isotherm at a temperature of 77 K obtained by a nitrogen adsorption method of the metal- supported catalyst, and the weight ratio of the carbon carrier being calculated by the following equation: weight ratio of carbon carrier=1-(metal content (wt%) of the metal- supported catalyst obtained by inductively coupled plasma mass spectrometry)/100”, which does not appear to be supported by the specification as filed. The present specification discloses [0100] the ratio of the less than 5 nm pore volume of the catalyst of the present invention to the 5 nm or more pore volume of the catalyst of the present invention (hereinafter referred to as “less than 5 nm pore/5 nm or more pore volume ratio”) may be, for example, 1.80 or more, and is preferably 1.90 or more, particularly preferably 2.00 or more. The upper limit value of the less than 5 nm pore/5 nm or more pore volume ratio of the catalyst of the present invention is not particularly limited, but the pore volume ratio may be, for example, 15.00 or less”, which does not entirely support the amendment to claim 1.
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, 5-10 and 12-15 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.
Claim 1 recites the limitation "the catalyst metal particles" in lines 9-10. There is insufficient antecedent basis for this limitation in the claim. The claim previously recites “catalyst metal particles” and “at least some of the catalyst metal particles”. It is unclear if the number-average particle diameter in line 9 is related to all the catalyst metal particles or the at least some of the catalyst metal particles that are partially buried in inner surfaces of pores of the carbon carrier.
Claim 1 recites the limitation "the nitrogen adsorption isotherm" in line 15. There is insufficient antecedent basis for this limitation in the claim.
Claim 1 recites the limitation "a nitrogen adsorption isotherm" in line 18. There is insufficient antecedent basis for this limitation in the claim.
Claim 1 recites “wherein a proportion of the number of catalyst metal particles supported on the outer surface of the carbon carrier to the total number of the catalyst metal particles supported on the carbon carrier is 33% or less”, which contains multiple limitations having insufficient antecedent basis. Furthermore, it is unclear what “a proportion” encompasses. Furthermore, it is unclear what encompasses “the outer surface”.
Claim 1 recites “the volumes V1 and V2 being obtained by dividing a volume V3 (cm³/g-metal-supported catalyst) of pores having a pore diameter of less than 5 nm and a volume V4 (cm³/g-metal-supported catalyst) of pores having a pore diameter of 5 nm or more, respectively, by a weight ratio of the carbon carrier included in the metal- supported catalyst, the volumes V3 and V4 being obtained from a nitrogen adsorption isotherm at a temperature of 77 K obtained by a nitrogen adsorption method of the metal- supported catalyst, and the weight ratio of the carbon carrier being calculated by the following equation: weight ratio of carbon carrier=1-(metal content (wt%) of the metal- supported catalyst obtained by inductively coupled plasma mass spectrometry)/100”, which is indefinite. It is unclear what Applicant is intending to claim. It is unclear what encompasses V1 and/or V2 and/or V3 and/or V4. Furthermore, it is unclear if the volume of pores of the carbon carrier is before or after the catalyst metal particles are supported on the carbon carrier. The volume of pores would be different as the catalyst metal particles would occupy the pores of the metal-supported catalyst.
Claim 7 recites “the metal-supported catalyst has a BET specific surface area, measured by a nitrogen adsorption method of the metal-supported catalyst, of 200 m2/g-carbon carrier)”, which is indefinite. It is unclear how a BET specific surface area of the carbon carrier is measured by a nitrogen adsorption method of the metal-supported catalyst. The metal-supported catalyst includes both a carbon carrier and catalyst metal particles supported on the carbon carrier.
Claim 7 recites the limitation "a nitrogen adsorption isotherm". There is insufficient antecedent basis for this limitation in the claim.
Claim 7 recites “the weight ratio of the carbon carrier being calculated by the following equation: weight ratio of carbon carrier=1-(metal content (wt%) of the metal-supported catalyst obtained by ICP-MS)/100”, which is indefinite. It is unclear what the “weight ratio of the carbon carrier” encompasses. It is unclear what “metal content” encompasses and how “metal content” is determined.
Claim 8 recites “the metal-supported catalyst has a ratio of a vapor-BET specific surface area (m2/g-carbon carrier)…measured by a water vapor adsorption method of the metal-supported catalyst”, which is indefinite. It is unclear how a vapor-BET specific surface area of the carbon carrier is measured by a water vapor adsorption method of the metal-supported catalyst. The metal-supported catalyst includes both a carbon carrier and catalyst metal particles supported on the carbon carrier.
Claim 8 recites the limitation "a nitrogen adsorption isotherm". There is insufficient antecedent basis for this limitation in the claim. It is unclear what encompasses “a N2-BET specific area (m2/g-carbon carrier) and how the N2-BET is determined. Page 33 of the present specification discloses BET specific surface area is referred to as N2-BET specific surface area, thus, it appears the term lacks proper antecedent basis in the claims.
Regarding claim 8, all claim limitations require proper antecedent basis. Appropriate correction is required. It is unclear what “the water vapor adsorption method of the metal-supported catalyst” encompasses. It is unclear what the “weight ratio of the carbon carrier” encompasses. It is unclear what “metal content” encompasses and how “metal content” is determined. It is unclear what “the nitrogen adsorption method of the metal-supported catalyst” encompasses.
Claim 10 recites the limitation "a volume of pores of the carbon carrier having a pore diameter of less than 5 nm” in lines 2-3. There is insufficient antecedent basis for this limitation in the claim. See “V1” of claim 1.
Claim 10 recites “a volume of pores of the carbon carrier having a pore diameter of less than 5 nm of 0.50 (cm³/g-carbon carrier) or more, the volume (cm³/g-carbon carrier) being obtained by dividing a volume (cm³/g-metal-supported catalyst) of pores having a pore diameter of less than 5 nm by a weight ratio of the carbon carrier included in the metal-supported catalyst, the volume (cm³/g-metal-supported catalyst) being obtained from a nitrogen adsorption isotherm at a temperature of 77 K obtained by a nitrogen adsorption method of the metal-supported catalyst, the weight ratio of the carbon carrier being calculated by the following equation: weight ratio of carbon carrier=1-(metal content (wt%) of the metal-supported catalyst obtained by ICP-MS)/100”, which is indefinite. It is unclear what Applicant is attempting to claim. Claim 10 recites the limitation "a nitrogen adsorption isotherm". There is insufficient antecedent basis for this limitation in the claim. Regarding claim 10, all claim limitations require proper antecedent basis. Appropriate correction is required. It is unclear what “a nitrogen adsorption method of the metal-supported catalyst” encompasses. It is unclear what the “weight ratio of the carbon carrier” encompasses. It is unclear what “metal content” encompasses and how “metal content” is determined. It is unclear what “the nitrogen adsorption method of the metal-supported catalyst” encompasses.
It is unclear how a pore volume of the carbon carrier is measured by a nitrogen adsorption method of the metal-supported catalyst. The metal-supported catalyst includes both a carbon carrier and catalyst metal particles supported on the carbon carrier.
Claim 12 recites “wherein a proportion of the number of catalyst metal particles supported in pores at a position having a depth of 20 nm or more from the outer surface of the carbon carrier to the total number of the catalyst metal particles supported on the carbon carrier is 11% or more”, which contains multiple limitations having insufficient antecedent basis. Furthermore, it is unclear what “a proportion” encompasses. Furthermore, it is unclear what encompasses “the outer surface”. Furthermore, if 33% or less of the catalyst metal particles are supported on an outer surface of the carbon carrier, it is unclear how 11% or more are supported at a position having a depth of 20 nm or more from the outer surface of the carbon carrier.
To the extent the claims are interpreted in view of the claims analysis section above and understood in view of the 35 USC 112 rejections above, note the following prior art rejections.
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.
Claim(s) 1, 5-10 and 12-15 is/are rejected under 35 U.S.C. 103 as being unpatentable over, Suzue et al., US 2014/0287344 A1.
Suzue teaches an electrode catalyst layer for a fuel cell comprising a catalyst, a porous carrier for supporting the catalyst, and a polymer electrolyte, in which a mode diameter of the pore distribution of the porous carrier is 4 to 20 nm, and the catalyst is supported in a pore with a pore diameter of 4 to 20 nm of the porous carrier (abstract). A mode diameter of the pore distribution of the primary pores of the porous carrier is controlled to 4 to 20 nm. That is to say, the primary pores 32b of the porous carrier 32 are formed more widely and shallowly than a conventional porous carrier [0049]. The material for the porous carrier is not particularly limited as long as the primary pores with the above-mentioned mode diameter can be formed in the carrier and the material has sufficient specific surface area and sufficient electron conductivity for supporting the catalyst component in a desired distributed state. The main component is preferably carbon. More specifically, examples thereof include carbon particles made of carbon black (such as Ketjen black, oil furnace black, channel black, lamp black, thermal black and acetylene black), and activated carbon [0053]. The catalyst may be catalyst metal particles such as catalyst platinum particles having an average particle diameter of 1-10 nm [0064-0066]. See at least Figure 4 of Suzue.
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The crystallinity of the carbon carrier is preferably controlled for the purpose of improving corrosion resistance of the catalyst layer. C band peak intensity and D band peak intensity calculated by Raman scattering spectral analysis may be used for the crystallinity and the crystalline composition of the carbon material [0055]. When the carbon material is analyzed by Raman spectroscopy, a peak ordinarily occurs in the vicinity of 1340 cm-1 and in the vicinity of 1580 cm-1. These peaks are ordinarily called "D band" and "G band" respectively. Incidentally, the peak of diamond is strictly 1333 cm-1 and is distinguished from the above-mentioned D band [0056]. The porous carrier may be carbon black such that the half-value width of D band, which appears at 1340 cm-1 in Raman spectrum, is 100 cm-1 or less. The porous carrier may be such that the half-value width of G band, which appears at 1580 cm-1 in Raman spectrum, is 60 cm-1 or less. In these cases, corrosion resistance of the catalyst layer is improved by the graphitization of the carbon carrier; thus, the catalyst layer, in which the initial performance is high and the performance may be maintained over a long term, may be provided [0057]. The lower limit values of the half-value width of D band and the half-value width of G band are not particularly limited. However, the primary pores are closed simultaneously with the progress of the graphitization of the carrier, so that it is preferable that the half-value width of D band is 50 cm-1 or more and the half-value width of G band is 40 cm-1 or more from the viewpoint of making the graphitization of the carrier compatible with the securing of the desired primary pore region [0058]. See also [0059-0063] of Suzue.
FIG. 5 of Suzue is a graph showing a result of measuring pore distribution of a porous carrier used in examples and comparative examples by a nitrogen adsorption method. See [0051-0052]. The support amount of the catalyst in the porous carrier is preferably 10 to 80% by mass, more preferably 30 to 70% by mass with respect to the whole amount of the catalyst carrier. The support amount is preferable by reason of allowing sufficient dispersity of the catalyst components on the carrier, the improvement of power generation performance, the economic advantages, and the catalyst activity per unit mass [0070]. See also Figure 4. The BET specific surface area of the porous carrier may be a specific surface area sufficient to support the catalyst component in a highly distributed state, but is preferably within the range of 20 to 1600 m2/g, or more preferably 80 to 1200 m2/g. When the specific surface area of the catalyst carrier is a value within such a range, the balance between the dispersibility of the catalyst component on the catalyst carrier and the effective utilization rate of the catalyst component may be appropriately controlled [0062]. The average particle diameter of the porous carrier is preferably 20 to 100 nm [0063].
Suzue does not explicitly teach the V1/V2 ratio recited by at least claim 1. However, FIG. 5 of Suzue is a graph showing a result of measuring pore distribution of a porous carrier used in examples and comparative examples by a nitrogen adsorption method. Suzue teaches a mode diameter of the pore distribution of pores (primary pores) in a porous carrier is controlled to a predetermined range and the catalyst is supported in the primary pores [0012]. Suzue further teaches the pore capacity with a pore diameter of 4 to 20 nm of the porous carrier is determined at 0.23 to 0.78 cm3/g, so that the electrolyte coverage factor is decreased to allow proton transport resistance to be inhibited from increasing and allow activity per the same catalyst weight to be improved [0050]. Figure 5 at least suggests the ratio of V1/V2 recited by claim 1.
Also, the pore capacity with a pore diameter of 4 to 20 nm of the porous carrier is preferably 0.23 to 0.78 cm3/g. A pore capacity of 0.23 cm3/g or more allows the amount of the catalyst not coated with the electrolyte to be sufficiently secured, allows the effective surface area of the catalyst to be sufficiently secured, and allows proton transport resistance to be inhibited from increasing. On the other hand, a pore capacity of 0.78 cm3/g or less allows the catalyst layer to be prevented from thickening by reason of a decrease in bulk density of the porous carrier, and allows proton transport resistance and diffused resistor to be inhibited from increasing. The pore capacity with a pore diameter of 4 to 20 nm of the porous carrier is determined at 0.23 to 0.78 cm3/g, so that the electrolyte coverage factor is decreased to allow proton transport resistance to be inhibited from increasing and allow activity per the same catalyst weight to be improved. Accordingly, the catalyst layer for a high durable fuel cell, which exhibits excellent power generation performance, may be provided even in the case of reducing the catalyst amount [0050]. "The pore capacity with a pore diameter of 4 to 20 nm of the porous carrier" signifies the total capacity of pores with a pore diameter of 4 to 20 nm existing in the porous carrier, and is calculated as an area (an integrated value) under a differential pore distribution curve obtained by a nitrogen adsorption method. The differential pore distribution is a distribution curve obtained by plotting a pore diameter on the horizontal axis and a pore capacity corresponding to the pore diameter in a sample on the vertical axis. That is to say, in the case of regarding the pore capacity of the porous carrier obtained by a nitrogen adsorption method as V and the pore diameter as D, a value (dV/d(log D)) such that differential pore capacity dV is divided by logarithmic difference of the pore diameter d(log D) is calculated. Then, the differential pore distribution curve is obtained by plotting this dV/d(log D) on the average pore diameter of each section. The differential pore capacity dV signifies the increment of the pore capacity between measuring points [0051].
Examiner notes the claims are indefinite and have been rejected under 35 USC 112. The claims do not clearly recite the specific elements of the claimed metal-supported catalyst.
Regarding the “nitrogen adsorption isotherm” limitation of at least claim 1, see the claims analysis section above. Suzue teaches the BET specific surface area of the porous carrier may be a specific surface area sufficient to support the catalyst component in a highly distributed state, but is preferably within the range of 20 to 1600 m2/g, or more preferably 80 to 1200 m2/g.
Suzue discloses "the catalyst is supported in the pore" signifies that the center of gravity of the catalyst particle is located inside the pore (the opposite side to the surface; the deep side in the depth direction of the pore) from a line which connects both end points of the pore opening on the catalyst layer surface in a cross section of the catalyst layer (the porous carrier) [0026].
Response to Arguments
Applicant's arguments filed 5/21/26 have been fully considered but they are not persuasive. While claims 1, 7, 8, 10 and 12 have been amended, the claims remain rejected under 35 USC 112. Furthermore, the claims amendments required new grounds of rejection under 35 USC 112.
Applicant states “reference to the specification below will be to the applicable paragraph number of the published patent application”. However, no paragraph numbers have been cited by Applicant. Further the reference figure referred to by Applicant is “a modified version of FIG. 1 of the present application”. Furthermore, the argument the “catalyst metal particles supported on the carbon carrier do not have pores and the pores of the carbon carrier in which the catalyst metal particles are supported still have some pore space and remain open”, is not commensurate in scope with the claimed invention. It is unclear if the specification supports such as argument.
Applicant argues Suzue does not teach or suggest a metal-supported catalyst according to amended claim 1. Applicant points to Figure 5 of Suzue and an inventor analysis of Figure 5 of Suzue (see the table on page 14 of the amendment). However, no explanation, calculations and/or support is given to show how the results shown in the table were determined from Figure 5 of Suzue. Furthermore, Applicant’s argument “it is highly probable” that the carbon carrier of Suzue fails to satisfy the V1/V2 ratio of claim 1 is not found persuasive and is without proper support.
Applicant present arguments regarding the Ketjen black used in Comparative example 2 of Suzue. This argument is not commensurate in scope with the claimed invention and/or representative of the entire teachings of Suzue.
Applicant further argues a person of ordinary skill in the art would not have expected that a metal-supported catalyst according to the amended claims would have superior catalytic activity and durability compared to other metal-supported catalysts known in the art. Applicant states the subject application demonstrates metal-supported catalysts according to the amended claims (Examples 1-4) have improved catalytic activity and durability compared to Examples C1-C9. Applicant notes Figure 7. However, any evidence of unexpected results must distinguish the claimed invention over the prior art of record. Examples 1-4 of the present specification are not commensurate in scope with the claimed invention. At least amended claim 1 is significantly broader than Examples 1-4 of the present specification. Furthermore, Examples C1-C9 are not representative of the teachings of Suzue. Examiner emphasizes Suzue teaches activity per catalyst weight is improved and the catalyst layer exhibits excellent power generation performance [0026]. See also [0049], [0050], [0052], [0068] and [0070] of Suzue that clearly teaches the electrode catalyst has improved catalytic activity. No evidence of unexpected results has been provided that distinguishes the claimed invention over the teachings of Suzue. Suzue further teaches a durability test was performed, the results are disclosed at Table 2, Figure 9 and [0147-0148].
Conclusion
The prior art made of record and not relied upon is considered pertinent to applicant's disclosure. Kamai (WO 2018/116586 A1) teaches a metal supported catalyst (1) includes platinum group metal atoms and carbon atoms. The metal supported catalyst can exhibit high catalytic activity even if the proportion of the platinum group element is small (abstract).
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/TRACY M DOVE/Primary Examiner, Art Unit 1725
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