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/Restriction
Applicant’s election without traverse of claims 41-50; amendment of now-withdrawn claim 67; cancellation of claims 9, 21-26, 29, 58, 59, and 62; and addition of claims 70-79 in the reply filed on 9 June 2026 are acknowledged.
Claims 1-8, 10-20, 27, 28, 30-40, 51-57, 60, 61, and 63-69 are withdrawn from further consideration pursuant to 37 CFR 1.142(b) as being drawn to nonelected inventions, there being no allowable generic or linking claim. Election was made without traverse in the reply filed on 9 June 2026.
Drawings
The drawings are objected to because the labels used in Figs. 1, 3, 11, 14, 20, and 21 appear to be in German. 37 CFR 1.52(b)(1)(ii) requires the application, including drawings, to be in English or accompanied by a translation together with a statement that the translation is accurate. Corrected drawing sheets in compliance with 37 CFR 1.121(d) are required in reply to the Office action to avoid abandonment of the application. Any amended replacement drawing sheet should include all of the figures appearing on the immediate prior version of the sheet, even if only one figure is being amended. The figure or figure number of an amended drawing should not be labeled as “amended.” If a drawing figure is to be canceled, the appropriate figure must be removed from the replacement sheet, and where necessary, the remaining figures must be renumbered and appropriate changes made to the brief description of the several views of the drawings for consistency. Additional replacement sheets may be necessary to show the renumbering of the remaining figures. Each drawing sheet submitted after the filing date of an application must be labeled in the top margin as either “Replacement Sheet” or “New Sheet” pursuant to 37 CFR 1.121(d). If the changes are not accepted by the examiner, the applicant will be notified and informed of any required corrective action in the next Office action. The objection to the drawings will not be held in abeyance.
Specification
The abstract of the disclosure is objected to because it is two paragraphs and contains the implied phrases "the invention relates to..." and "the invention further relates to...". A corrected abstract of the disclosure is required and must be presented on a separate sheet, apart from any other text. See MPEP § 608.01(b).
Claim Objections
Claims 41 and 42 are objected to because of the following informalities:
Regarding claim 41, on lines 4-5, a comma is required before the phrase “…and wherein arranged between the second electrode…” Appropriate correction is required.
Claim 42 is objected to as dependent upon withdrawn claim 27. For the purpose of examination on the merits, claim 42 will be interpreted to include the text of claim 27.
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.
Claims 47-50 and 73-77 are rejected under 35 U.S.C. 112(b) as being indefinite for failing to particularly point out and distinctly claim the subject matter which the inventor or a joint inventor regards as the invention.
Regarding claims 47, 49, and 75-77, a broad range or limitation together with a narrow range or limitation that falls within the broad range or limitation (in the same claim) may be considered indefinite if the resulting claim does not clearly set forth the metes and bounds of the patent protection desired. See MPEP § 2173.05(c). In the present instance:
Claim 47 recites the broad recitation "an electrolyte with a pH value in the range from approximately 7 to approximately 13," and the claim also recites "in particular in the range from approximately 7 to approximately 11" which is the narrower statement of the range/limitation.
Claim 49: " followed by "in particular in
Claim 75: " followed by "in particular
Claim 76: “a content in a range from approximately 5 percent by weight to approximately 13 percent by weight,” followed by “in particular approximately 9 percent by weight.”
Claim 77: “a content in a range from approximately 10 percent by weight to approximately 20 percent by weight,” followed by “in particular approximately 15 percent by weight.”
These claims are considered indefinite because there is a question or doubt as to whether the feature introduced by such narrower language is (a) merely exemplary of the remainder of the claim, and therefore not required, or (b) a required feature of the claims. For examination on the merits, the claims will be understood to refer to the broader range.
Regarding claims 47, 49, and 73-77, the term “approximately” as used to refer to measures (e.g. pH, concentration, mass fraction) is a relative term which renders the claims indefinite. The term “approximately” is not defined by the claims, the specification does not provide a standard for ascertaining the requisite degree of precision, and one of ordinary skill in the art would not be reasonably apprised of the scope of the invention. The electrolyte pH ranges of claim 47, upper limit of molar fraction of salt of claim 49, maximum value of y of claim 73, maximum second metallic content of claim 74, weight fraction of HER catalyst chemical compound of claim 75, molybdenum oxide content of claim 76, and molybdenum content of claim 77 are therefore rendered indefinite. For examination on the merits, these claims will be interpreted without the term “approximately.”
Regarding claim 49, it is unclear from the claim alone if, when taking (b) into consideration, the neutral to alkaline salt is limited to either comprising or consisting of the recited salts. For examination on the merits, the claim will be interpreted as consistent with the specification at [0110], where the neutral to alkaline salt is described with the phrase “is or contains” followed by the claimed members of the group.
Claims 48 and 50 are also rejected because they inherit all limitations of claim 47 from which they depend.
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.
This application currently names joint inventors. In considering patentability of the claims the examiner presumes that the subject matter of the various claims was commonly owned as of the effective filing date of the claimed invention(s) absent any evidence to the contrary. Applicant is advised of the obligation under 37 CFR 1.56 to point out the inventor and effective filing dates of each claim that was not commonly owned as of the effective filing date of the later invention in order for the examiner to consider the applicability of 35 U.S.C. 102(b)(2)(C) for any potential 35 U.S.C. 102(a)(2) prior art against the later invention.
Claims 41-46, 70, 75, 77, and 79 are rejected under 35 U.S.C. 103 as being unpatentable over Masel et al. (US 10,724,142 B2) in view of Ma et al. (CN 110681404 A, using attached machine translation).
Regarding claims 41-43, 45, 46, and 70, Masel teaches a water electrolyzer with an anode and a cathode, and an ion exchange membrane between the anode and cathode; with catalytically active catalyst layers present on/applied to both the anode and cathode, facing and in contact with the ion exchange membrane (Col. 5-6, lines 67-8: as “membrane electrode assembly,” interface with membrane indicates direct contact; Col. 6, lines 17-18: water electrolyzer; Fig. 1). The ion exchange membrane between the anode and cathode is an anion exchange membrane (Col. 10, lines 18-25).
Masel does not specifically teach that one or both electrocatalysts of the anode and/or cathode is a HER catalyst containing a chemical compound formed of a transition metal and C, O, or S wherein the transition metal is Mo or W as required by claim 41; only that the catalyst is substantially free of precious metals (Col. 5, lines 59-62). However, Ma teaches a molybdenum carbide hydrogen evolution catalyst for the cathode of a water electrolyzer ([0009]). The molybdenum carbide catalyst is highly efficient in electrolytic production of hydrogen, allowing it to replace the more expensive conventional platinum or palladium catalysts ([0005]).
It would have been obvious to one of ordinary skill in the art as of the effective filing date to use the molybdenum carbide HER catalyst of Ma in the water electrolyzer of Masel. One would have been motivated to make this substitution in order to reduce the cost of a water electrolyzer compared to a PEM electrolyzers (Masel Col. 2, lines 12-21), as further supported by the teachings of Ma ([0005]).
Regarding claim 44, Masel in view of Ma further teaches that the electrocatalyst of the anode is suitable for oxygen evolution reaction (Masel Col. 8, lines 16-25). The electrocatalyst of the cathode, i.e. second electrode, is the molybdenum carbide of Ma as previously applied to claim 41.
Regarding claims 75 and 77, Masel and Ma teach all inherited limitations from claim 41 on which it depends. Masel as modified by Ma further teaches that the HER catalyst does not exclude components besides the chemical compound of claim 41 (Masel Col. 10, line 20-21: “comprising”) but does not disclose any weight percentage of the claimed chemical compound. Likewise, the weight percentage of molybdenum in the final catalyst is not disclosed by either Masel or Ma. However, the ideal weight percentages of the claimed chemical compound and molybdenum in the catalyst are obvious to one skilled in the art through routine experimentation to find the most effective weight percentages for the water electrolyzer of claim 41. It is not inventive to discover the optimum or workable ranges by routine experimentation. See MPEP §2144.05(II). The ranges of 67 to 85 percent by weight of chemical compound and 10 to 20 percent by weight of molybdenum as claimed would have been obvious through such routine experimentation.
Regarding claim 79, Ma further teaches that the molybdenum carbide HER catalyst is made from a solution of ammonium molybdate tetrahydrate, 4-chloro-o-phenylenediamine, water, and hydrochloric acid ([0010]; [0013]: solvent is deionized water; [0015]: ammonium molybdate tetrahydrate; [0018]: hydrochloric acid). Ammonium molybdate tetrahydrate is a molybdenum salt, and 4-chloro-o-phenylenediamine is an aromatic amine. It would have therefore been obvious to one of ordinary skill in the art to prepare the HER catalyst of claim 41 in this way. One would be motivated to do so in order to control the nanostructure of the resulting molybdenum carbide ([0033]: the use of 4-chloro-o-phenylenediamine results in formation of sheets after the carbonization step).
Claims 47-50 are rejected under 35 U.S.C. 103 as being unpatentable over Masel et al. (US 10,724,142 B2) in view of Ma et al. (CN 110681404 A) as applied to claim 41 above, and further in view of Bonduelle-Skrzypczak et al. (WO 2020/109064, using attached machine translation).
Regarding claims 47-50, Masel in view of Ma does not teach an electrolyte with a pH in the range of 7 to 13. Several embodiments of the Ma catalyst as used in hydrogen evolution reaction are taught with a 1 M KOH solution, which corresponds to a pH of 14 ([0042]).
However, Bonduelle-Skrzypczak teaches an electrode for water splitting suitable for use in an alkaline liquid electrolyte ([0141]-[0142]). The pH of the electrolytic medium is greater than 7 ([0127]). The electrolyte may be an aqueous solution of KOH ([0143]); indicating water is the solvent. The limitation of the solution molarity is given in the alternative alongside the limitation of its actual composition.
It would have therefore been obvious to one of ordinary skill in the art to use a more neutral pH solution in the water electrolysis cell, because Masel teaches that operating alkaline water electrolyzers at high pH leads to excessive corrosion of components when the temperature is increased in order to improve current density (Col. 2, lines 22-37). The claimed range of 7 to 13 is not disclosed by Masel, Ma, or Bonduelle-Skrzypczak. However, it is not inventive to discover the optimum or workable pH range through routine experimentation for what is most suitable for the claimed electrolyzer, especially because any pH below 7 would be acidic and the claimed range is broad. See MPEP §2144.05(II). The range of electrolyte pH of approximately 7 to approximately 13 as claimed would have been obvious through such routine experimentation.
Claims 71-74 are rejected under 35 U.S.C. 103 as being unpatentable over Masel et al. (US 10,724,142 B2) in view of Ma et al. (CN 110681404 A) as applied to claim 41 above, and further in view of Sasaki et al. (US 2015/0083585 A1).
Regarding claims 71-72, Masel as modified by Ma teaches all inherited limitations from claim 41, but not a HER catalyst chemical compound further containing at least one second transition metal.
However, Sasaki teaches that suitable compounds for HER catalytic materials for electrodes in water splitting include molybdenum carbide nanoparticles with secondary transition metals ([0016]: MaMobCx). The metal M is selected from a group which includes the claimed Ni, Co, Cu, Fe, and Ti ([0016]; claim 8). The molybdenum metallic content, or “first metallic content” as claimed, is greater than the “second metallic content” in most embodiments except when the ratio is 1:1 ([0035]: “about 1:1 to 1:20…” “…or about 1:1 to 1:5”).
It would have been obvious to one of ordinary skill in the art to use the molybdenum carbide taught by Sasaki which incorporates a second transition metal. One would be motivated to do so because “it is proposed that [by] combining or alloying a metal that binds hydrogen weakly with a metal that binds it strongly, a functional but relatively inexpensive HER catalyst could be developed” ([0008]). The range of all ratios of a “first metallic content greater than the second metallic content” is obvious to one skilled in the art, because the claimed range is so broad as to encompass all ratios less than 1:1 as described by Sasaki, and only excluding 1:1. No special effect is noted at the ratio of 1:1 in the art of record.
Regarding claims 73-74, Sasaki further teaches one possible molybdenum carbide is Ni0.2--Mo-1.8-C, satisfying both the requirements of the instant application claim 73’s y < 0.25 and the relationships between a, b, and x taught by Sasaki ([0016]: a = 0.2, b = 1.8, x = 1, 1/(0.2+1.8) = 1/2). The metallic content of nickel in this nickel-molybdenum carbide, or “second metallic content” as claimed, is within the claimed 0-25 Mol%.
While not all possible values of a, b, and x disclosed by Sasaki will be within the claimed range of y < 0.25, it is obvious to one skilled in the art to find the most optimal ranges of coefficients for the chemical compound’s composition, as evidenced by the routine experimentation carried out by Sasaki ([0066]: preparation of NiMo and Mo nitrides, but specification also directed to NiMo carbides). The claimed range of y < 0.25 is therefore obvious.
Claim 76 is rejected under 35 U.S.C. 103 as being unpatentable over Masel et al. (US 10,724,142 B2) in view of Ma et al. (CN 110681404 A) as applied to claim 41 above, and further in view of Wang et al. (Electrochimica Acta, 2020, as attached).
Regarding claim 76, Masel as modified by Ma and applied to claim 41 teaches all inherited limitations. Neither Masel nor Ma specifically teaches a molybdenum oxide in the HER catalyst. Masel only teaches that the base metal catalyst is substantially free of precious metals (Col. 5, lines 59-62).
However, Wang et al. teaches a molybdenum oxide HER electrocatalyst for use in alkaline solutions (p. 1, Abstract; p. 6, Conclusion). The molybdenum oxide is present along with a nickel foam in the HER electrocatalyst (p.3, Results and Discussion, first para.). By varying the duration of a hydrazine treatment process step, different overpotentials vs RHE were observed (p. 5, Fig 4(b) and caption).
It would have been obvious to one of ordinary skill in the art to use a molybdenum oxide electrocatalyst in the water electrolyzer taught by Masel in view of Ma. One would have been motivated to make this modification because the molybdenum oxide electrocatalyst as taught by Wang is a viable electrocatalyst for HER in alkaline solution, especially due to its low cost and high stability (p. 1, Introduction, “MoO2 with a rutile structure shows competent properties as bifunctional electrocatalyst for water splitting…”).
Wang does not teach a mass ratio between the molybdenum oxide and the nickel foam. However, as demonstrated by the use of different concentrations of solution of molybdenum salt for forming the catalyst (p.3, Results and Discussion, first para.), it is within the ability of one of ordinary skill in the art to experiment to find an optimal or workable range for the claimed 5 to 13 percent weight content of the molybdenum oxide in the HER catalyst. See MPEP §2144.05(II). The 5 to 13 percent by weight range is therefore obvious.
Claim 78 is rejected under 35 U.S.C. 103 as being unpatentable over Masel et al. (US 10,724,142 B2) in view of Ma et al. (CN 110681404 A) as applied to claim 41 above, and further in view of Dong et al. (CN 111013619 A, using attached machine translation).
Regarding claim 78, Masel as modified by Ma teaches all inherited limitations from claim 41 upon which it depends, but not that the HER catalyst is needle-shaped.
However, Dong teaches molybdenum carbide nanorods for use as hydrogen evolution catalysts in alkaline media ([0020]). The nanorods as taught are substantially similar in structure as claimed ([Fig. 2]). The molybdenum carbide nanorods increase the specific surface area and facilitate electron transport, improving reaction kinetics on the catalyst surface; leading to excellent catalytic performance and low overpotential ([0023]).
It would have therefore been obvious to one of ordinary skill in the art to use a needle-shaped HER catalyst in the claimed water electrolyzer. One would be motivated to do so because the nanorods taught by Dong are shown to be more effective by their significantly lower overpotential of 129 mV at 10 mA/cm2 -in 1 M KOH solution ([0046]), compared to the various overpotentials at the same current densities and KOH solution (Ma Fig. 7 and [0042]; Dong Fig. 4, below). In the claimed electrolyzer cell, this would be expected to result in more efficient operation.
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Conclusion
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/CBF/Examiner, Art Unit 1711
/MICHAEL E BARR/Supervisory Patent Examiner, Art Unit 1711