DETAILED ACTION
Notice of Pre-AIA or AIA Status
1. The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
Continued Examination Under 37 CFR 1.114
2. 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and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114.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 23 July 2026 has been entered.
Response to Amendment
3. Applicant’s response 23 July 2026 is acknowledged and considered fully responsive. The applicant has cancelled Claims 2, 7-9, 11, 15-23, and 28. Claims 1 and 26 have been amended with no new material added. Currently, Claims 1, 3-6, 10, 12-14, and 24-27 are pending and under examination.
Claim Rejections - 35 USC § 103
4. 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.
5. 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.
6. Claims 1, 3, 4, 10, 12-14, and 24-27 are rejected under 35 U.S.C. 103 as being obvious over Zhou et al. with evidence of inherency provided by Lu et al.
Zhou et al. (“Exceptional Performance of Hierarchical Ni-Fe hydroxide @ NiCu Electrocatalysts for Water Splitting,” Adv. Mater. 2019, 31, article 1806769, pg. 1-8 – previously presented) is directed toward a non-noble metal electrocatalyst for water splitting (pg. 1: abstract). Lu et al. (“High performance NiFe layered double hydroxide for methyl orange dye and Cr(VI) adsorption,” Chemosphere 2016, 152, 415-422 – previously presented) provides evidentiary support of inherency for the amount of water present in the interlayer of the Ni4Fe-LDH material (pg. 417: Fig. 1a).
Regarding Claim 1, Zhou et al. discloses a water splitting catalyst (pg. 1: title and abstract; pg. 4: Fig. 3 – OER performance; pg. 6: Fig. 4 – HER performance) comprising a double layered hydroxide including at least two transition metal (e.g.: Ni and Fe on pg. 1: Abstract and Supporting Information pg. 1-2: Experimental – Synthesis of NiFe-LDH@NiCu), and a metal particle including at least one transition metal (e.g.: Ni and Cu on pg. 1: Abstract and Supporting Information pg. 1-2: Experimental – Synthesis of NiFe-LDH@NiCu), wherein the metal particle has a surface coated with the layered double hydroxide as depicted in Fig. 1 in the various micrographs and EDS mapping (pg. 1).
Claim 1 of the instant application further describes a ratio of R2 to R1, where R2 is calculated from mass ratio of the metal particle to the mass of the LDH in the catalyst and R1 is calculated from the mass ratio of the nanoparticles added to the mass ratio of the amount of LDH that can form during the preparation. Therefore, this ratio characterizes the efficiency of the catalyst preparation process (conversion of input raw materials to synthesized product.
Pertaining to the tabulation of value of R2, Zhou et al. discloses the atomic ratios as determined by ICP-AES for both the bulk NiCu material and the NiFe-LDH@NiCu composite material in Table S1 on pg. 4 of the supporting information, which can be used to derive the weight ratio of the metal particle in the catalyst to the LDH material in the catalyst.
The specification of the instant application in ¶118 and ¶132 cited from US Pub. No. 2023/0121007 A1 indicates the mass of the LDH material to be formed can be derived by tabulating the molar mass the LDH material based on forming a species that is electrically neutral. In the case of Example 1 of the instant application, the applicant has tabulated a molar mass of 337.7 g/mol for the LDH material derived from nickel(II) chloride and ferric chloride which has the molecular formula of Ni2Fe1(OH)6Cl1‧1.5 H2O. By analogy, the LDH material disclosed in Zhou et al., which is prepared from nickel(II) nitrate and ferric nitrate has the formula Ni4Fe1(OH)10(NO3)‧m H2O. The value of m can be determined from TGA and has a value of ~3.6 as evidenced by Lu et al. which shows a mass loss of ~11.2% for interlayer water leaving the LDH material synthesized from a 4:1 ratio of nickel(II) nitrate and ferric nitrate (Lu et al. on pg. 417: Fig. 1c and 3.1. Characterization of as-synthesized NiFe-LDH). The means the electrically neutral LDH material from the nitrate salts taught by Zhou et al. has the molecular formula of Ni4Fe1(OH)10(NO3)‧3.6 H2O and a corresponding molar mass of 588.6 g/mol. Therefore, the value of the theoretical amount of LDH formed can be calculated from the amount of ferric nitrate used in the composite catalyst preparation, which is pertinent to the calculation of R1.
Zhou et al. also discloses the process of making NiCu nanoparticles and using the material generated in-situ to form the active catalyst (i.e.: NiFe-LDH@NiCu composite in the SI on pg. 1-2: Synthesis of NiFe-LDH@NiCu) meaning Zhou et al. does not directly disclose the mass of nanoparticles used in the preparation of the catalyst. Zhou et al. indicates that the presence of the NiCu alloy in the core-shell composite reduces the electrical resistivity or enhances the electrical conductivity compared to the bulk NiFe-LDH (pg. 6: second full paragraph). The amount of NiCu nanoparticles relative to the amount of LDH coating should be selected to optimize the catalyst coverage (or catalytic activity) and the electrical conductivity of the catalyst particles. Higher amounts of NiCu nanoparticles will improve the electrical conductivity, but reduce the effective concentration of LDH catalyst particles (and reduce catalyst efficiency). Therefore, the mass of NiCu alloy nanoparticle used in the preparation of core-shell catalyst is a result-effective variable, i.e., a variable which achieves a recognized result, and the determination of the optimum or workable ranges of said variable might be characterized as routine experimentation (See MPEP 2144.0.II.B.). Accordingly, it would have been obvious to one of ordinary skill in the art before the effective filing date of the invention to have discovered the optimum or workable ranges of the NiCu alloy nanoparticle mass (and by extension the value of R1 and the ratio of R2 to R1), including values within the claimed range (i.e.: the ratio of R2 to R1), through routine experimentation. One would have been motivated to do so in order to have formed a core-shell metal particle-LDH electrocatalyst with enhanced electrical conductivity resulting in improved catalytic efficiency.
The amendment to Claim 1 further limits the LDH to include Ni and Fe (i.e.: a layered double hydroxide) and the metal particle (i.e.: the support or core) to include Ni. Zhou et al. with evidentiary support from Lu et al. discloses the layered double hydroxide comprises Ni and Fe (pg. 1: Abstract and Supporting Information pg. 1-2: Experimental – Synthesis of NiFe-LDH@NiCu) and the metal particle includes nickel as supported on pg. 1 in Abstract and Supporting Information pg. 1-2: Experimental – Synthesis of NiFe-LDH@NiCu, which indicates a NiCu nanoparticle core. The use of “including” for the Ni particle is open-ended language meaning that a NiCu nanoparticle meets the claim limitations since the alloy is at least partially made of metallic nickel.
Regarding Claim 3, Zhou et al. with evidentiary support from Lu et al. discloses the catalyst according to Claim 1, further comprising a coating layer that is provided on the surface of the metal particle and that includes the layered double hydroxide, wherein the coating layer has an average thickness of less than or equal to 100 nm as evidenced an LDH thickness of 1.6 nm (Zhou et al. on pg. 3) and micrographs of Figure 1. It has been held that a prima facie case of obviousness exists when the range disclosed by the prior art overlaps with the claimed range. See MPEP 2144.05(I) - OVERLAPPING, APPROACHING, AND SIMILAR RANGES, AMOUNTS, AND PROPORTIONS.
Regarding Claim 4, Zhou et al. with evidentiary support from Lu et al. discloses the catalyst according to Claim 1, wherein the layered double hydroxide has a crystallize size of less than 10 nm as supported by micrographs in Figure 1. It has been held that a prima facie case of obviousness exists when the range disclosed by the prior art overlaps with the claimed range. See MPEP 2144.05(I) - OVERLAPPING, APPROACHING, AND SIMILAR RANGES, AMOUNTS, AND PROPORTIONS.
Regarding Claim 10, Zhou et al. with evidentiary support from Lu et al. discloses the catalyst according to Claim 1, wherein the metal particle has an average particle diameter of less than or equal to 50 nm as supported by Fig. S1 in the Supporting Information where the synthesized NiCu nanoparticles have an average diameter of 21 ± 4 nm (SI on pg. 8). It has been held that a prima facie case of obviousness exists when the range disclosed by the prior art overlaps with the claimed range. See MPEP 2144.05(I) - OVERLAPPING, APPROACHING, AND SIMILAR RANGES, AMOUNTS, AND PROPORTIONS.
Regarding Claim 12, Zhou et al. with evidentiary support from Lu et al. discloses a water electrolysis cell comprising: a positive electrode (i.e.: the anode for water splitting forming oxygen; Fig. 3a/c/d) including the catalyst for a water electrolysis cell according to Claim 1 (i.e.: NiFe-LDH@NiCu cast onto a glassy carbon electron gauze as the working electrode in Supporting Information on pg. 2-3: Electrochemical Measurements); a negative electrode (e.g.: Pt gauze as the counter electrode in Supporting Information on pg. 2-3: Electrochemical Measurements); and an electrolyte (1 M KOH on pg. 4: Fig. 3 and SI on pg. 2-3: Electrochemical Measurements).
Regarding Claim 13, Zhou et al. with evidentiary support from Lu et al. discloses a water electrolysis cell comprising: a positive electrode (e.g.: Pt gauze counter electrode in Supporting Information on pg. 2-3: Electrochemical Measurements); a negative electrode (i.e.: the cathode for water splitting forming hydrogen; Fig. 4a/b) including the catalyst for a water electrolysis cell according to Claim 1 (i.e.: NiFe-LDH@NiCu cast onto a glassy carbon electron gauze as the working electrode in Supporting Information on pg. 2-3: Electrochemical Measurements) and an electrolyte (1 M KOH on pg. 4: Fig. 3 and SI on pg. 2-3: Electrochemical Measurements).
Regarding Claim 14, Zhou et al. with evidentiary support from Lu et al. discloses the
water electrolysis cell according to Claim 12, and a voltage applicator that applies a voltage between the positive and negative electrode, the voltage applicator being connected to the positive electrode and the negative electrode as described in Supporting Information on pg. 2-3 in the Electrochemical Measurements Section using linear sweep voltammetry to power the water splitting reaction.
Regarding Claim 24, Zhou et al. with evidentiary support from Lu et al. discloses the catalyst according to Claim 1. As discussed in Claim 1 above, the molecular formula for the NiFe-LDH derived from nickel nitrate and ferric nitrate is Ni4Fe1(OH)10(NO3)‧3.6 H2O. When this formula is rewritten in the form listed in Claim 24 of the instant application, the result is:
N
i
0.8
F
e
0.2
O
H
2
0.2
(
N
O
3
∙
0.72
H
2
O
]
where M12+ = Ni; M23+ = Fe; An- is NO31-; x = 0.2 which falls between 0 and 1; y = 0.2; n = -1; and m = 0.72. The aforementioned values for each variable and chemical elements meet the limitations of Claim 24.
Regarding Claim 25, Zhou et al. with evidentiary support from Lu et al. discloses the catalyst according to Claim 24, wherein the interlayer ion is nitrate (i.e.: NO31-) as supported by the chemical formula
Regarding Claim 26, Zhou et al. with evidentiary support from Lu et al. discloses the catalyst according to Claim 1, wherein a ratio of an amount of Fe to a total amount of Ni and Fe present in the layered double hydroxide is greater than or equal to 0.25 and less than or equal to 0.5. The ratio of Ni to Fe disclosed by Zhou et al. has a ratio of 4 mol nickel to 1 mol of iron, which is a ratio of 0.2 mol iron to 1.0 mol of Fe+Ni (Synthesis of NiFe-LDH@NiCu section on pg. 1-2 of the supporting info of Zhou et al.), which is similar to the range disclosed in Claim 26. It has been held that a prima facie case of obviousness exists when the range disclosed by the prior art is similar to the claimed range. See MPEP 2144.05(I) - OVERLAPPING, APPROACHING, AND SIMILAR RANGES, AMOUNTS, AND PROPORTIONS.
Regarding Claim 27, Zhou et al. with evidentiary support from Lu et al. discloses the catalyst according to Claim 1, wherein the layered double hydroxide includes primary particles and secondary particles, and the secondary particles are aggregates of the primary particles as supported by Figure 1d and Figure 1e (TEM micrographs on pg. 2 of Zhou et al.).
7. Claims 5 and 6 are rejected under 35 U.S.C. 103 as being unpatentable over Zhou et al. with evidence of inherency provided by Lu et al. as applied to Claim 1 above, and further in view of Zhang et al.
Zhou et al. (“Exceptional Performance of Hierarchical Ni-Fe hydroxide @ NiCu Electrocatalysts for Water Splitting,” Adv. Mater. 2019, 31, article 1806769, pg. 1-8 – previously presented) is directed toward a non-noble metal electrocatalyst for water splitting (pg. 1: abstract). Lu et al. (“High performance NiFe layered double hydroxide for methyl orange dye and Cr(VI) adsorption,” Chemosphere 2016, 152, 415-422 – previously presented) provided evidentiary support of inherency for the amount of water present in the interlayer of the Ni4Fe-LDH material (pg. 417: Fig. 1a). Zhang et al. (CN104857960A – previously presented) is directed toward a multi-level composite oxide catalyst and preparation thereof (title).
Regarding Claim 5, Zhou et al. with evidentiary support from Lu et al. discloses the catalyst according to Claim 1, but does not include the use of a multidentate ligand. Like Zhou et al., Zhang et al. discloses a layered double hydroxide catalyst, “LDH,” (Ex. 5: ¶58-61) comprising at least two transition metals (Ex. 5: Ni and Fe) with an electrically conductive graphene core (analogous to the particle of the instant application). The LDH layer of Zhang et al. in Ex. 5 is prepared by a mixture of nickel(II) nitrate, iron(III) nitrate, and citric acid (¶58). The use of citric acid functions as both a complexing agent and a dispersing agent as per ¶9 and ¶11by facilitating the uniform distribution of the metal ions on the nanoparticle surface. Higher catalytic activity results from the small size and high dispersion of the LDH catalyst on the surface of the graphene (¶25).
It would be obvious to one of ordinary skill in the art prior to the effective filing date of the claimed invention to modify the LDH/Ni-Cu core shell catalyst of Zhou et al. by including a multidentate ligand such as citrate as taught by Zhang et al. with the reasonable expectation of improving the catalytic activity of the LDH/NiCu catalyst owing to the small size and uniform dispersion of said catalyst.
Regarding Claim 6, Zhou et al. with evidentiary support from Lu in view of Zhang et al. discloses the catalyst according to Claim 5, wherein the multidentate ligand includes a citric acid salt as evidenced by Ex. 5 of Zhang et al. which is a mixture of nickel(II) nitrate, iron(III) nitrate, and citric acid (¶58). The aforementioned species in solution will form complexes of nickel citrate and iron citrate, i.e., salts of citric acid as required by Claim 6 of the instant application.
Response to Arguments
8. Applicant's arguments filed 23 July 2026 have been fully considered but they are not persuasive. Therefore, the rejection of Claims 1, 3-6, 10, 12-14, and 24-27 as being obvious in view of Zhou et al. with evidence from Lu et al. is maintained.
9. The applicant has amended Claim 1 to be limited to explicitly the ratios of R2/R1 and the compositions (i.e.: Ni and Fe LDH and metallic Ni core) disclosed in inventive examples 1-3.
The applicant has further argued in their response that the ratio of R-values in Claim 1 is important since specific ratios of those values result in excellent durability, thus the applicant is claiming unexpected results. In TABLE I of the instant application (cited from US Pub. No. 2023/0121007 A1), the ratios of R2/R1 for the inventive examples are 0.87, 0.92, and 1.11. While the inventive examples do have better current retention than the comparative examples (with R2/R1 ratios of 1.73, and 9.0), the comparative examples have been prepared by a different method (¶146-147 of the instant application cited from US Pub. No. 2023/0121007 A1). Rather than growing the LDH directly onto the nanoparticulate supports and controlling the reaction using propylene oxide to adjust the pH (¶142 of the instant application cited from US Pub. No. 2023/0121007 A1), the preformed and isolated NiFe-LDH is added to the nanoparticulate support making a two-component mixture. The SEM images depicted in FIG. 11 and FIG. 12 of the instant application show no or very poor coverage of the metallic Ni nanoparticle with the NiFe-LDH material rather than complete coverage (i.e.: a clear core-shell structure) as for the inventive examples depicted in FIG. 8, FIG. 9, and FIG. 10. The applicant has not demonstrated the criticality of the R2/R1 ratio despite claiming the exact values in the inventive examples since no data with a R2/R1 value less than 0.87 nor greater than 1.11 made by the same method as the inventive examples is presented.
10. The applicant has argued that ICP-AES cannot be used to determine the values for R1 and R2 relevant for the limitations of Claim 1 in their response; however, the examiner does not agree with this assertion. Since both the elemental composition of the uncoated NiCu nanoparticle (i.e.: the bare particle) and the elemental composition of the LDH-coated onto the NiCu nanoparticle are both characterized, the values of R1 and R2 can be derived from the data provided by Zhou et al.
11. The applicant has argued that the examiner has not explained how Zhou et al. can be used to derive the R2/R1 ratio as required by Claim 1. The examiner finds this assertion without merit as explained in detail above for Claim 1. The applicant is further reminded that the rationale for citing/combining references supplied by the examiner does not have to be the same as the rationale disclosed by the applicant. The applicant has argued the R2/R1 ratio results in enhanced catalyst durability. However, examiner has argued that the R-value ratio can be derived from Zhou et al. by balancing the weight of nanoparticle with the amount of LDH coating since a very large excess amount of NiCu will give higher conductivity, but will lower the catalyst surface area (i.e.: catalyst activity). Therefore, optimization of the R-value ratio is directed toward balancing electrical conductivity of the LDH-nanoparticle catalyst and the catalytic activity.
Conclusion
12. Any inquiry concerning this communication or earlier communications from the examiner should be directed to KEVIN SYLVESTER whose telephone number is 703-756-5536. The examiner can normally be reached Mon - Fri 8:15 AM to 4:30 PM EST.
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/KEVIN SYLVESTER/Examiner, Art Unit 1794
/CIEL P CONTRERAS/Primary Examiner, Art Unit 1794
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