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 .
Election/Restriction
2. The applicant’s selection of Group I in their response dated 08 June 2026 is acknowledged. By the election of Group I, Claims 19-22, 25, 27, and 29 are withdrawn. Claims 5-7, 13, 18, 23-24, 26, 28, and 30-89 were previously cancelled by the applicant. Claims 1-4, 8-12, and 14-17 are currently pending and under examination.
Claim Objections
3. Claim 1 is objected to because of the following informalities: “co catalyst” should read “co-catalyst”. Appropriate correction is required.
Claim Rejections - 35 USC § 112
4. 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.
5. Claims 1-4, 8-12, and 14-17 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.
The term “discontinuous layer” in Claim 1 is a relative term which renders the claim indefinite. The term “discontinuous layer” is not defined by the claim, the specification does not provide a standard for ascertaining the requisite degree, and one of ordinary skill in the art would not be reasonably apprised of the scope of the invention. The term “discontinuous layer” is referenced in ¶23 of the instant application (cited as US Pub. No. 2023/0158459 A1), but does not define what percentage of coverage of the base layer nor the porosity of the catalyst that would typically be used to define “(dis)continuous.”
The term “dense layer” in Claim 1 is a relative term which renders the claim indefinite. The term “dense layer” is not defined by the claim, the specification does not provide a standard for ascertaining the requisite degree, and one of ordinary skill in the art would not be reasonably apprised of the scope of the invention. The term “dense layer” is referenced through the instant application (e.g.: ¶14, ¶23-4, ¶27, ¶29-33, ¶103-4, ¶106, ¶114, ¶118, ¶120-122, ¶137, ¶161) of the instant application (cited as US Pub. No. 2023/0158459 A1), but does not define the porosity, the density, or the thickness that would typically be used to define “dense.”
Claim 1 lists the following Markush grouping:
the one or more co-catalysts have an area density not exceeding 20 µg per cm2; and/or
a majority of the co catalysts are in an outer portion of the rough surface, the outer portion of the rough surface being less than one half of a thickness of the rough surface defined by peaks of the rough surface;
the one or more co-catalysts are in the form of a discontinuous layer having a thickness of 50 nm or less on the rough surface.”
Based on the placement of the “and/or” conjunction (underlined and bolded above) between clause [1] and clause [2] and the lack of any conjunction between clause [2] and clause [3], it is unclear if all three clauses are considered to be in the Markush grouping. The examiner is interpreting the Markush grouping to include clause [1], clause [2], and clause [3] as every clause characterizes the catalyst loading on the rough surface. Therefore, satisfying any single clause will meet the limitation of Claim 1.
Claims 2-4, 8-12, and 14-17 are rejected under U35 USC § 112(b) as they depend from Claim 1, which currently stands rejected under the same statute.
Claim Rejections - 35 USC § 103
6. 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.
7. 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.
8. Claims 1, 2, 3, 4, 8, 9, 10, 11, 12, 15, 16, and 17 are rejected under 35 U.S.C. 103 as being unpatentable over Roark et al. in view of Badwal et al.
Roark et al. (US Pub. No. 2004/0129135 A1) is directed toward a dense, layered membrane for hydrogen separation (title). Badwal et al. (US Pub No. 2016/0193564 A1) is directed toward a process of utilizing selectively permeable membrane (title).
Regarding Claim 1, Roark et al. discloses a hydrogen permeable membrane (title and abstract). According to ¶84, Roark et al. illustrates a cross-section of a dense (non-porous) multi-layer membrane in FIG. 1A. Layer 5 in FIG. 1A is the dense layer of the hydrogen permeable membrane having a first and a second face and which can be a hydrogen permeable metal or alloy (¶86). In the prior art discussion, Roark et al. indicates that Pd and its alloys are very common metal or metallic alloys used to fabricate the dense layer of the hydrogen permeable membrane (¶28). The metal selection for the dense hydrogen permeable membrane of Roark et al. are vanadium, niobium, tantalum, zirconium, titanium and alloys thereof (¶45). The thickness of layer 5 varies from 20 microns to about 1,000 microns and needs to be sufficiently thick so it is non-porous without unnecessarily limiting hydrogen permeation (¶86). Roark et al. further indicates layer 3 is a catalyst (layer) for hydrogen dissociation and can be a metal or an alloy (¶87). The catalyst layer 3 of Roark et al. is generally thin and may be porous (i.e.: discontinuous in the instant application). Roark et al. teaches specific example of the catalysts include: Pd, alloys of Pd, including Pd/Ag and Pd/Cu alloys, Ni and Pt and alloys thereof (¶46). The other layers in FIG. 1 of Roark et al. are further defined in ¶88-94 and listed as optional with inclusion of said layer(s) depending on the end use application. Roark et al. is silent on the use of a rough surface on one of the faces of the dense hydrogen permeable membrane.
[AltContent: textbox ([img-media_image1.png]
FIG.1A from Roark et al.)]
Badwal et al. discloses a hydrogen permeable membrane (title and abstract) having a dense layer of a hydrogen permeable metal (layer 3 and layer 9) with first and second faces having a catalyst (layer 11) on at least one face as per FIG. 2 and FIG. 3. Thus, Roark et al. and Badwal et al. have a similar structure and fall into the same field of art. Badwal et al. further describes a surface modification to the dense hydrogen permeable membrane (¶9) and said modification is depicted in FIG. 1a (in-situ casting of the H2 permeable membrane) and FIG. 1b (mechanical or chemical roughening of the H2 permeable membrane). The surface modification according to ¶9 and FIG. 1c further includes a coating comprising a catalyst onto the irregular or roughened surfaces depicted in FIG. 1a or FIG 1b. The depiction of the catalyst layer clearly represents a discontinuous catalyst layer. Badwal et al. discloses the thickness of the catalyst layer or the roughened surface) ranges from 10 nm to 5000 nm (¶28 and ¶96). The surface modification provides a three dimension surface on which the co-catalyst is deposited resulting in significant surface area that is available (to enhance) catalytic activity (¶74, 89, and 90). It has been held that a prima facie case of obviousness exists when the prior art and the claimed range overlap. See MPEP 2144.05(I) - OVERLAPPING, APPROACHING, AND SIMILAR RANGES, AMOUNTS, AND PROPORTIONS.
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 hydrogen permeable membrane of Roark et al. by including a roughened face (on which the catalyst) is applied as taught by Badwal et al. with the reasonable expectation of forming a three dimensional surface having a large surface area to improve catalytic activity as suggested by Badwal et al.
The Claim 1 limitations: “the one or more co-catalysts have an area density not exceeding 20 µg per cm2” and “a majority of the co catalysts are in an outer portion of the rough surface, the outer portion of the rough surface being less than one half of a thickness of the rough surface defined by peaks of the rough surface” are being treated as optional as explained in the 112b rejection for Claim 1 above.
Regarding Claim 2, Roark et al. in view of Badwal et al. disclose the membrane according to Claim 1. As part of the roughened surface step of Badwal et al. referenced in ¶9, the co-catalyst layer/composition may be intercalated, interspersed or embedded with the hydrogen species selectively permeable solid membranes. This description indicates that the exact location of the co-catalyst composition within or on top of the dense layer is part of routine optimization depending upon the end use of the co-catalyst deposited on the dense layer. The optimization of the co-catalyst placement (for the example of ammonia synthesis) is further detailed in ¶98-101 of Badwal et al. Therefore, the location of the co-catalyst within the hydrogen permeable membrane 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 placement of the co-catalyst on the dense layer, including values within the claimed range, through routine experimentation. One would have been motivated to do so in order to ensure efficient hydrogenation of a reactant (e.g.: nitrogen as exemplified in Badwal et al.) to produce a chemical product (e.g.: ammonia as exemplified in Badwal et al.).
Regarding Claim 3, Roark et al. in view of Badwal et al. discloses the membrane according to Claim 1 wherein the one or more co-catalysts comprise one or more transition metals as supported by Roark et al. which teaches specific example of the catalysts include: Pd, alloys of Pd, including Pd/Ag and Pd/Cu alloys, Ni and Pt and alloys thereof (¶46), all of which are transition metals.
Regarding Claim 4, Roark et al. in view of Badwal et al. discloses the membrane according to Claim 1, wherein the one or more co-catalysts comprise: Pd/Ag alloys, Pd/Cu alloys, Ni, Ni alloys, Pt, or Pt alloys (Roark et al. in ¶46).
Regarding Claim 8, Roark et al. in view of Badwal et al. discloses the membrane according to Claim 1, wherein the one or more co-catalysts have a thickness of 10 nm to 5000 nm as evidenced by ¶96 in Badwal et al. It has been held that a prima facie case of obviousness exists when the prior art and the claimed range overlap. See MPEP 2144.05(I) - OVERLAPPING, APPROACHING, AND SIMILAR RANGES, AMOUNTS, AND PROPORTIONS.
Regarding Claim 9, Roark et al. in view of Badwal et al. discloses the membrane according to Claim 8, wherein the one or more co-catalysts have a thickness of 10 nm to 5000 nm as evidenced by ¶96 in Badwal et al. It has been held that a prima facie case of obviousness exists when the prior art and the claimed range overlap. See MPEP 2144.05(I) - OVERLAPPING, APPROACHING, AND SIMILAR RANGES, AMOUNTS, AND PROPORTIONS.
Regarding Claim 10, Roark et al. in view of Badwal et al. discloses the membrane according to Claim 1, wherein the rough surface comprises a layer of palladium black deposited on the dense layer as evidenced by Ex. 10 of Roark et al. In ¶269, Roark et al. indicates that Pd (black) was vapor deposited onto a vanadium-palladium based dense layer.
Regarding Claim 11, Roark et al. in view of Badwal et al. disclose the membrane according to Claim 1. The surface modification of Badwal et al. according to ¶9 and FIG. 1c further includes a coating comprising a co-catalyst deposited onto the irregular or roughened surfaces depicted in FIG. 1a or FIG 1b. The depiction of the co-catalyst layer clearly represents a discontinuous co-catalyst layer. The surface modification provides a three dimension surface on which the co-catalyst is deposited resulting in significant surface area that is available (to enhance) catalytic activity (¶74, 89, and 90). Given these two facets, the geometric area and the actual area of the first face are not expected to be similar. The surface area should be set to ensure maximum catalytic activity (as per ¶84-¶98 of Badwal et al). Therefore, surface area of the surface of the hydrogen permeable membrane 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 ratio of the actual area to the geometric area of the dense layer, including values within the claimed range, through routine experimentation. One would have been motivated to do so in order to improve the catalytic activity of the hydrogen permeable membrane.
Regarding Claim 12, Roark et al. in view of Badwal et al. discloses the membrane according to Claim 1, wherein the dense layer comprises palladium having a purity of at least 95% as supported by ¶103 of Badwal which teaches the hydrogen species permeable metal may be selected from palladium (i.e.: greater than 95% purity) or Pd alloyed with silver, copper, chromium, iron, nickel or cobalt. It has been held that a prima facie case of obviousness exists when the prior art and the claimed range overlap. See MPEP 2144.05(I) - OVERLAPPING, APPROACHING, AND SIMILAR RANGES, AMOUNTS, AND PROPORTIONS.
Regarding Claim 15, Roark et al. in view of Badwal et al. discloses the membrane according to Claim 1, wherein the dense layer comprises a foil as per ¶86 of Roark et al. The thickness of the foil is capable of having a thickness of 100 µm as Roark et al. indicates the thickness of layer 5 (i.e.: the dense layer or the foil) varies from 20 microns to about 1,000 microns allowing for sufficient thickness to lack porosity, but without unnecessarily limiting hydrogen permeation (Roark et al. in ¶86). It has been held that a prima facie case of obviousness exists when the prior art and the claimed range overlap. See MPEP 2144.05(I) - OVERLAPPING, APPROACHING, AND SIMILAR RANGES, AMOUNTS, AND PROPORTIONS.
Regarding Claim 16, Roark et al. in view of Badwal et al. discloses the membrane according to Claim 1, wherein the dense layer has a thickness in the range of 15 µm to 40 µm as supported by ¶86 of Roark et al. which indicates the thickness of layer 5 (i.e.: the dense layer) varies from 20 microns to about 1,000 microns. This thickness needs to be sufficiently thick so it is non-porous without unnecessarily limiting hydrogen permeation (Roark et al. ¶86). It has been held that a prima facie case of obviousness exists when the prior art and the claimed range overlap. See MPEP 2144.05(I) - OVERLAPPING, APPROACHING, AND SIMILAR RANGES, AMOUNTS, AND PROPORTIONS.
Regarding Claim 17, Roark et al. in view of Badwal et al. discloses the membrane according to Claim 1, wherein the dense layer comprises a fluid permeable substrate and a layer of hydrogen permeable metal on the substrate as evidenced by FIG. 2 of Badwal et al. FIG. 2 of Badwal depicts a reaction apparatus for the formation of ammonia from nitrogen and hydrogen and is further described in ¶166-169. Badwal et al. indicates that the fluid permeable substrate is membrane 3 (e.g.: 100-micron thick Pd membrane) and the layer of hydrogen permeable membrane is 9 (e.g.: Pd sputtered surface) as per ¶167.
9. Claim 14 is rejected under 35 U.S.C. 103 as being unpatentable over Roark et al. in view of Badwal et al. with evidentiary support from Paolone et al.
Roark et al. (US Pub. No. 2004/0129135 A1) is directed toward a dense, layered membrane for hydrogen separation (title). Badwal et al. (US Pub No. 2016/0193564 A1) is directed toward a process of utilizing selectively permeable membrane (title). Paolone et al. (“Hydrogen and Deuterium Solubility in Commercial Pd-Ag Alloys for Hydrogen Purification,” ChemEngineering 2017, 1, article 14, pg. 1-9) is directed toward the characterization Pd-Ag alloys (pg. 1: title)
Regarding Claim 14, Roark et al. in view of Badwal et al. discloses the membrane according to Claim 1.
In order for a dense material to be characterized as hydrogen storage material, it must be able to either adsorb hydrogen or activate hydrogen via a metal-hydrogen complex or metal-hydride/proton complex reversibly. One well known material that forms hydrides is palladium as per Paolone et al (pg. 3: 1. Introduction), where it says Pd is capable of repeated hydrogenation/dehydrogenation cycles under specific operative conditions. This repeated stress means that the Pd material can suffer from embrittlement due to the mismatches in various lattice parameters, but this issue can be obviated by alloying with other like Ag (pg. 3: Introduction of Paolone et al.). Among Pd-Ag alloys, the best compromise between the mitigation of lattice mismatch, the hydrogen-diffusion coefficient, and permeability is obtained around the composition Pd77Ag23 or Pd75Ag25 with alloying also increasing the mechanical strength and reliability Pd-Ag alloyed membrane modules (pg. 3: Introduction of Paolone et al.). In Figure 7, Paolone et al. depicts a comparison of H2 and D2 binding on Pd77Ag23 at different pressures finding that low pressures favor D2 absorption over H2 absorption (pg. 7) indicating that Pd77Ag23 is a deuterium-selective material.
Since Roark et al. in view of Badwal et al. disclose the dense layer may comprise a Pd-Cu alloy and/or a Pd-Ag alloy (¶82 of Badwal) and Roark et al. discloses specific Pd-Ag alloys with 20% to 50% Ag, the combination of references meets the limitation of Claim 14 (i.e.: wherein the dense layer comprises a hydrogen storage material, and wherein the dense layer comprises a deuterium selective material”) with evidentiary support from Paolone et al. as explained in detail above.
Conclusion
10. The prior art made of record and not relied upon is considered pertinent to applicant's disclosure. Pisarev et al. (“Hydrogen Permeation Through Membranes With Rough Surface,” AIP Conf. Proc. 2006, 837, 238-249) is directed toward hydrogen permeation through membranes with a rough surface (pg. 238: abstract). Al-Mufachi et al. (“Hydrogen selective membranes: A review of palladium-based dense metal membranes,” Renewable Sustainable Energy Rev. 2015, 47, 540–551) is a review of palladium-based dense metal membranes (pg. 540: title). Li et al. (US Pub. No. 2009/0277331 A1) is directed toward hydrogen separation composite membrane module and the method of production thereof (title).
11. 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
/BRIAN W COHEN/Primary Examiner, Art Unit 1759
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