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/Restrictions
Applicant’s election without traverse of Group I and Species A in the reply filed on 08/17/2026 is acknowledged.
Claims 5 and 16-27 are withdrawn from further consideration pursuant to 37 CFR 1.142(b) as being drawn to a nonelected invention, there being no allowable generic or linking claim. Claims 8 and 11-15 are withdrawn from further consideration pursuant to 37 CFR 1.142(b) as being drawn to a nonelected species, there being no allowable generic or linking claim. Election was made without traverse in the reply filed on 08/17/2026. Claims 1-4, 6-7, and 9-10 are examined in this Office action.
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.
Claims 1-4, 6-7, and 9-10 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 “a catalyst slurry” and later recites the limitation “the printed slurry.” The latter limitation lacks proper antecedent basis in the claims. The former limitation is further indefinite since it is unclear to one of ordinary skill in the art if the term “catalyst” is used to identify the presence of a catalyst in the slurry, or if the slurry serves as a catalyst for the subsequent CVD step. Claim 1 further recites the limitation “(b) depositing the printed slurry using chemical vapor deposition,” which is indefinite since CVD it is unclear how one skilled in the art would be able to successfully deposit a slurry using a vapor process, and the specification at [0061] instead suggests that the printed slurry is used as a catalyst for a CVD growth process. Claims 2-4, 6-7, and 9-10 depend upon claim 1 and do not rectify the issue, so are similarly rejected for indefiniteness.
Claim 9 recites the limitation “the sample infill” which lacks antecedent basis in the claims.
Claim Rejections - 35 USC § 103
In the event the determination of the status of the application as subject to AIA 35 U.S.C. 102 and 103 (or as subject to pre-AIA 35 U.S.C. 102 and 103) is incorrect, any correction of the statutory basis (i.e., changing from AIA to pre-AIA ) for the rejection will not be considered a new ground of rejection if the prior art relied upon, and the rationale supporting the rejection, would be the same under either status.
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 1 is rejected under 35 U.S.C. 103 as being unpatentable over Tour et al. 2019 (US20190308880A1) in view of Zhou et al. “Three-dimensional Printing for Catalytic Applications: Current Status and Perspectives,” Adv. Funct. Mater. 2017, 27, 1701134, provided on the IDS filed on 2/13/2024 and 7/23/2026, respectively.
Regarding claim 1, Tour discloses a method of making a 3d-shaped 3d graphene (3D graphene object, 0242) comprising (a) 3d printing a catalyst slurry (nickel/binder mixture, 0245) via “direct in situ 3D printing of graphene foams” (0212); (b) depositing the printed slurry using CVD to produce a graphene-nickel composite (0246, “graphene sheets that cover the Ni powders,” 0250); and etching the nickel-graphene composite (0247), wherein the resulting composite is a porous (0276), binder-free structure of 3D2G (“the polymer-based binder is converted into graphene sheets that cover the Ni powders,” 0250). Tour does not explicitly teach that the direct in situ 3D printing is a direct ink writing process. However, Zhou teaches analogous processes for the printing of catalyst materials (p. 3 ‘3. 3D Printing of Catalytic Materials’) which is pertinent to the field of endeavor of Tour because Zhou teaches the printing of metal structures to disperse a catalyst on the surface (p. 7 col. 2 pp. 1) as Tour teaches the use of Ni as a similar template to disperse catalyst for graphene growth in a CVD process (0202-0205). Zhou discloses direct ink writing as a popular 3D printing technique (p. 2 col. 2). It would be obvious to one skilled in the art to combine the teachings of Tour and Zhou by using DIW taught by Zhou to implement the direct in situ printing taught by Tour; one would be motivated to do so because Zhou teaches that DIW is advantageous for its easy operation and low cost (p. 2 col. 2). Therefore one skilled in the art would arrive at the claimed invention prior to the effective filing date.
Claims 2-3 are rejected under 35 U.S.C. 103 as being unpatentable over Tour and Zhou as applied to claim 1 above, and further in view of Jakus et al. 2015, “Metallic Architectures from 3D-Printed Powder-Based Liquid Inks,” Adv. Funct. Mater. 2015, 25, 6985–6995, cited on the IDS filed on 2/13/2024.
Regarding claim 2, Tour and Zhou teach the invention as applied to claim 1. Tour further teaches that the catalyst slurry comprises nickel particles mixed with an organic solvent and a polymer (0050). Tour does not teach that the slurry further comprises a plasticizer. However, Zhou teaches the mixture of nickel powder with polylactic-co-glycolic acid and dibutyl phthalate, plasticizer, with dichloromethane solvent (p. 7 col. 2 pp. 3) for use in a printing of a catalyst which is then subjected to sintering. It would be obvious to one skilled in the art to combine the teachings of Tour and Zhou and arrive at the claimed mixture in view of Jakus, since Jakus motivates the selection of a polymer for the robust polymer-like mechanical properties of the resulting object (p. 6988 col. 2 pp. 2), Jakus motivates the selection of dibutyl phthalate for allowing rapid fabrication by fusion of parts (p. 6988 col. 2 pp. 2), and Jakus motivates the selection of DCM as solvent for its evaporative properties which allow the remaining materials to maintain increased viscosity and form a self-supporting structure (p. 6988 col. 2 pp. 2). Further Jakus teaches the importance of these materials since they are selected such that there are only physical interactions between the metal powders and solvents and polymer, which allows the scalability of the resultant ink process (p. 6988 col. 1-2). One skilled in the art would find these properties of the mixture advantageous for the invention of Tour since Tour discloses that the invention uses inexpensive carbon sources through sintering to arrive at graphene (0008) since the current state of the technology is limited to microscale 3D printed graphene objects (0007), and Zhou teaches that the taught mixture is subjected to sintering and obtains macroscopic structures (p. 7 col. 2 pp. 3, Figure 11).Therefore one skilled in the art would arrive at the claimed composition of catalyst slurry, such that it contains nickel particles mixed with an organic solvent, a polymer, and a plasticizer, prior to the effective filing date.
Regarding claim 3, Tour, Zhou, and Jakus teach the invention as applied to claim 2, wherein the solvent is dichloromethane, the polymer is poly lactic-co-glycolic acid, and the plasticizer is dibutyl phthalate.
Claim 4 is rejected under 35 U.S.C. 103 as being unpatentable over Tour and Zhou as applied to claim 1 above, and further in view of Al-Hilfi et al. 2021, “Chemical Vapor Deposition of Graphene on Cu-Ni Alloys: The Impact of Carbon Solubility,” Coatings 2021, 11, 892, referred to herein as Al-Hilfi.
Regarding claim 4, Tour and Zhou teach the invention as applied to claim 1. Tour additionally teaches that a hydrocarbon gas can be used as the atmosphere for the heating process (methane, 0252). It is prima facie obvious to combine two compositions known for the same purpose each of which is taught by the prior art to be useful for the same purpose to form a third composition to be used for the very same purpose. See MPEP 2144.06.I. Tour therefore discloses that CH4 gas and the H2/Ar gases are known equivalents useful for reacting in the CVD process to produce the nickel-graphene composite. It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the method for preparing a 3D2G by using an H2/Ar gas further comprising CH4 as disclosed by Tour as the mere combination of equivalents known for the same purpose. Furthermore, one would be motivated to make this modification to achieve the additional purpose of the CH4 gas acting as a carbon source for the growth of graphene during the CVD, as Tour teaches (0252).
Tour and Zhou do not teach a rate of cooling falling within the claimed range of 10 to 60 C. Tour discloses heating the printed slurry in a gas mixture of hydrogen and argon (0251) to a temperature of around 1000 Celsius (0250), followed by reducing the temperature at a rate of about 97 °C/min until room temperature (over 10 minutes, 0255). However, Al-Hilfi teaches a method of growing graphene on nickel (abstract) which is pertinent to the field of endeavor of Tour since Al-Hilfi teaches growth with chemical vapor deposition at a temperature of 1000 C and cooling to room temperature (p. 6) as Tour does. Al-Hilfi teaches a rate of cooling to room temperature at 27 C per minute (Figure 5). It would be obvious to combine the teachings of Tour, Zhou, and Al-Hilfi to modify the cooling rate taught by Tour to be the cooling rate taught by Al-Hilfi; one would be motivated to do so because Al-Hilfi teaches that a slower cooling rate sees more graphene growth on nickel as nickel content increases (Figure 5, p. 10), which is advantageous to the invention of Tour since Tour teaches that the nickel is used as a template to grow graphene (0211). Therefore one skilled in the art would arrive at the claimed invention.
Claims 6-7 and 9-10 are rejected under 35 U.S.C. 103 as being unpatentable over Tour and Zhou as applied to claim 1 above, and further in view of Arapov et al. 2016 “Conductivity Enhancement of Binder-Based Graphene Inks by Photonic Annealing and Subsequent Compression Rolling,” Conductivity Enhancement of Binder-Based Graphene Inks by Photonic Annealing and Subsequent Compression Rolling† . Adv. Eng. Mater., 18: 1234-1239, provided with this Office action.
Regarding claim 6, Tour and Zhou teach the invention as applied to claim 1. Tour and Zhou do not teach a method of making a compressed 3D2G, by compressing 3D2G wherein the compression is accomplished with rolling compression (as elected in the response filed on 8/17/2026). However, Arapov teaches a method of compressing a graphene ink (abstract) which is pertinent to the field of endeavor of Tour since Tour teaches the conductivity of the printed graphene materials and that conductivity can be improved (0286) and teaches that 3D graphene with good conductivity has utility (0291), and Arapov teaches that the compression results in improved structural integrity of graphene yielding high conductivity (p. 1237 col. 1 pp. 2). Arapov teaches a method of photonic annealing followed by rolling compression (p. 1235 col. 1 pp. 4) of a 3D graphene structure (Fig. 5). It would be obvious to combine the teachings of Tour, Zhou, and Arapov by using the rolling compression taught by Arapov on the obtained graphene product to arrive at the claimed invention; one would be motivated to do so in order to improve the conductivity of the graphene product, in order to facilitate printed graphene conductors as Arapov teaches (p. 1238 col. 1 pp. 1).
Regarding claim 7, Tour, Zhou, and Arapov teach the invention as applied to claim 6. Arapov further teaches that the samples are held at room temperature unless being subjected to heat from the annealing process (“after the end of each pulse, the sample cools down to room temperature,” p. 1235 col. 2) and the rolling compression is conducted after the annealing; therefore Arapov teaches that the rolling compression is conducted at room temperature, as claimed. Alternatively, it would be obvious to one skilled in the art, absent the explicit mention of a temperature to conduct the rolling compression by Arapov, to conduct the rolling compression at ambient conditions, in a range of temperatures overlapping with the claimed range. As set forth in MPEP 2144.05, in the case where the claimed range "overlap or lie inside ranges disclosed by the prior art," a prima facie case of obviousness exists, In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. 1990). Therefore one skilled in the art would arrive at the claimed invention prior to the effective filing date.
Regarding claim 9, Tour, Zhou, and Arapov teach the invention as applied to claim 6. Zhou further teaches that graphene and metallic oxide architectures are printed with infill (Figures 7-9, 11-12), wherein at least an infill of 57% is taught in Figure 12 (Fig. 12e). It would be obvious to one skilled in the art to combine the teachings of Tour, Arapov, and Zhou to arrive at the claimed range of infill; one would be motivated to do so because Tour teaches the use of the 3D product as a catalyst (0291), and Zhou teaches that the printing improves the heat and mass transfer properties of catalysts compared to monolithic catalysts (p. 10 col. 2 pp. 2). One skilled in the art would therefore arrive at the claimed invention prior to the effective filing date.
Regarding claim 10, Tour, Zhou, and Arapov teach the invention as applied to claim 6. Arapov further teaches that the samples are held at room temperature unless being subjected to heat from the annealing process (“after the end of each pulse, the sample cools down to room temperature,” p. 1235 col. 2) and the rolling compression is conducted after the annealing; therefore Arapov teaches that the rolling compression is conducted at room temperature, as claimed. Alternatively, it would be obvious to one skilled in the art, absent the explicit mention of a temperature to conduct the rolling compression by Arapov, to conduct the rolling compression at ambient conditions, in a range of temperatures overlapping with the claimed range. As set forth in MPEP 2144.05, in the case where the claimed range "overlap or lie inside ranges disclosed by the prior art," a prima facie case of obviousness exists, In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. 1990).
Tour, Zhou, and Arapov do not explicitly teach that the compression is conducted in air or in an inert environment. However, absent the express teaching of an environment to conduct the taught step, one skilled in the art would find it necessary and obvious to use at least the disclosed conditions taught by the prior art and maintain these conditions, without any teaching to motivate the altering of conditions. Accordingly, one would look to the prior art to find teachings of an atmosphere, where Tour teaches that the step of obtaining graphene can be performed in air (0044) or in an atmosphere including argon which is inert (0045). Therefore one skilled in the art would arrive at the claimed invention prior to the effective filing date.
Conclusion
The prior art made of record and not relied upon is considered pertinent to applicant's disclosure. Huang et al. “Binder-free highly conductive graphene laminate for low cost printed radio frequency applications,” Appl. Phys. Lett. 106, 203105 (2015) teaches a process of compressing graphene ink via rolling compression to improve the conductivity of graphene.
Any inquiry concerning this communication or earlier communications from the examiner should be directed to Eileen Moudou whose telephone number is (571)272-1768. The examiner can normally be reached M-Th 8 AM - 4 PM EST.
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/Eileen Moudou/ Examiner, Art Unit 1738
/SALLY A MERKLING/SPE, Art Unit 1738
