DETAILED ACTION
In the amendment filed on October 23, 2025, claims 1 – 5, 8 – 12, 16 – 17 are pending. Claims 1, 8, 11, 12, 16 have been amended and claims 6 – 7, 13 – 15, 18 have been canceled.
The text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
Priority
Repeating from the previous Office Action, Applicant’s claim for the benefit of a prior-filed application under 35 U.S.C. 119(e) or under 35 U.S.C. 120, 121, 365(c), or 386(c) is acknowledged. Applicant has not complied with one or more conditions for receiving the benefit of an earlier filing date under 35 U.S.C. 119(e) as follows:
The later-filed application must be an application for a patent for an invention which is also disclosed in the prior application (the parent or original nonprovisional application or provisional application). The disclosure of the invention in the parent application and in the later-filed application must be sufficient to comply with the requirements of 35 U.S.C. 112(a) or the first paragraph of pre-AIA 35 U.S.C. 112, except for the best mode requirement. See Transco Products, Inc. v. Performance Contracting, Inc., 38 F.3d 551, 32 USPQ2d 1077 (Fed. Cir. 1994).
The disclosure of the prior-filed application, provisional Application No. 63/396445 (hereafter the “provisional application”), fails to provide adequate support or enablement in the manner provided by 35 U.S.C. 112(a) or pre-AIA 35 U.S.C. 112, first paragraph for one or more claims of this application.
The provisional application particularly does not provide sufficient support for claims 1 – 18 as the provisional application’s disclosure is limited to embodiments of a substrate of copper foil, operating temperatures “near the melting point” of copper and methane as a precursor gas. The broader, more generic present claims encompass such substantial variation that the provisional applicant’s disclosure is not representative of the scope of the present claims. "A patentee will not be deemed to have invented species sufficient to constitute the genus by virtue of having disclosed a single species when … the evidence indicates ordinary artisans could not predict the operability in the invention of any species other than the one disclosed." In re Curtis, 354 F.3d 1347, 1358, 69 USPQ2d 1274, 1282 (Fed. Cir. 2004).
For the purposes of art rejections, the effective filing date of the present application is August 8, 2023, the filing date of the present application.
Claim Interpretation
Repeating from the previous Office Action, the Examiner notes that claim 1 and claims dependent on claim 1 recite a list of steps with marked alphabetical ordinals. However, the mere presence of alphabetical ordinals does not require that the ordinated steps are performed in a particular order under the broadest reasonable interpretation of the claims as ordering is required either by antecedent basis or other express language establishing timing and/or order.
Claim Objections
The objections to claims 11 – 12 are withdrawn due to Applicant amendment.
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.
The rejections of the claims 3, 6 – 7, 13 – 15 under 35 USC § 112(b) in the previous Office Action are withdrawn due to Applicant amendment.
Claims 1 – 2, 4 – 5, 8 – 12, 16 – 17 remain 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.
Regarding claims 1, 8, 9:
As a first matter, the amendments to claim 1 greatly ameliorated the clarity of the present claims with respect to the deficiencies of step (c) in the previous presentation of the claims.
However, the deficiency concerning the claim limitation elevating the temperature … to a level that is about the melting point”1 (hereinafter “Limitation A”) in claim 1 remains. Limitation A is a relative term which renders the claim indefinite. Limitation A 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 Examiner recognizes the that the term “close” was replaced by “about” in the present claims to overcome the previous rejections of the claims under 35 USC 112(b). However, the same problem exists with regards to the word “about” in the context of the present application.
In determining the range encompassed by the term “about” (and relatedly the previous presentation of “close to”), one must consider the context of the term as it is used in the specification and claims of the application. Ortho-McNeil Pharm., Inc. v. Caraco Pharm. Labs., Ltd., 476 F.3d 1321, 1326, 81 USPQ2d 1427, 1432 (Fed. Cir. 2007). The term “about” is entitled to latitude in characterizing features which are not critical, to distinction over prior art. General Foods Corp. v. Perk Foods Co. 283 F. Supp. 100,157 USPQ 14. In determining the range encompassed by the term "about," one must consider the context of the term as it is used in the specification and claims of the application. Ortho-McNeil Pharm., Inc. v. Caraco Pharm. Labs., Ltd., 476 F.3d 1321, 1326, 81 USPQ2d 1427, 1432 (Fed. Cir. 2007). Where there is nothing in the specification, prosecution history, or the prior art to provide any indication as to what range of specific activity is covered by the term "about.", the claims may be held indefinite. See Amgen, Inc. v. Chugai Pharmaceutical Co., 927 F.2d 1200, 18 USPQ2d 1016 (Fed. Cir. 1991).
The specification appears to place great emphasis (i.e. criticality) on what the temperature of the substrate is after heating in combination with the cooling rate from the final temperature to room temperature, stating “once the temperature of the substrate has reached the level that is close to its melting point (e.g. about 1000 °C to about 1100° in this invention)” in paragraph [0025] of the instant specification.
Furthermore, while the instant specification provides an example of heating copper to a temperature that is within the range of 1000°C to about 1100°C (1080°C, 1085°C in paragraph [0024]), the particular example is in relation to a copper substrate (see also [0031] of the instant specification which indicates heating to 1080°C). Under the broadest reasonable interpretation, the same limitations would be required by any other material, such as nickel (bulk melting point of about 1453°C). Examples are not sufficient to provide definition to the scope of a claim limitation, especially when the range of what is considered “about” is critical in view of the prior art.
Finally, the scope of the term “substrate” under the broadest reasonable interpretation does not require a monolithic substrate. Multiple materials with different melting points in a composite construction (or alloys thereof or both) can fall under the meaning of a substrate, for example. It then becomes unclear which potential material melting point within such a substrate is the substrate to be heated. The Examiner also notes that present claim 2 and 3 appears to restrict the material of the substrate to only copper, only nickel, only platinum or only an alloy of any of copper, nickel or platinum.
Dependent claims 8 and 9 as presented aggravate the issue as it requires heating to e.g. “about 1080°C” without identifying the melting point of the substrate from which the recited limitation of “about 1000°C to 1100°C” (for claim 8)/ “about 1080°C”.
Applicant’s response filed on October 23, 2025 does not address the particular deficiency discussed above.
Thus it becomes unclear by what standard would be considered “about”, rendering the relative term indefinite. See e.g. in Ex parte Oetiker, 23 USPQ2d 1641 (Bd. Pat. App. & Inter. 1992), Ortho-McNeil Pharm., Inc. v. Caraco Pharm. Labs., Ltd., 476 F.3d 1321, 1326, 81 USPQ2d 1427, 1432 (Fed. Cir. 2007).
Claim 3 is not rejected under 35 USC 112(b) because the substrate is limited to copper, which has a clear bulk melting point and fair direction for one of ordinary skill in the art to ascertain the range of values that may be considered “about” in view of the prior art. The Examiner does note that in vacuum, claim 1 as originally presented and claim 1 as currently presented allows for the heating temperature to be above the melting point of the substrate.
Claim Rejections - 35 USC § 102
The following is a quotation of the appropriate paragraphs of 35 U.S.C. 102 that form the basis for the rejections under this section made in this Office action:
A person shall be entitled to a patent unless –
(a)(1) the claimed invention was patented, described in a printed publication, or in public use, on sale, or otherwise available to the public before the effective filing date of the claimed invention.
(a)(2) the claimed invention was described in a patent issued under section 151, or in an application for patent published or deemed published under section 122(b), in which the patent or application, as the case may be, names another inventor and was effectively filed before the effective filing date of the claimed invention.
The rejections of the claims under 35 USC § 102 in the previous Office Action are withdrawn due to Applicant amendment.
Claim Rejections - 35 USC § 103
The rejections of the claims under 35 USC § 103 in the previous Office Action are withdrawn due to Applicant amendment.
Claim(s) 1 – 2, 4 – 5, 8 – 12, 16 – 17 is/are rejected under 35 U.S.C. 103 as being unpatentable over Gao et al. US 2022/0081300 A1 (hereafter “Gao”) in view of Lin et al. Synthesis of Graphene by CVD and its Nitrogen-plasma Treatment for Electrodes in Electrochemical Capacitor: Significance of Cooling and Plasma Conditions. Electrochemistry, 84(7), 506–510 (2016) (hereafter “Lin”) and optionally in view of Lai GB 2530974A (hereafter “Lai”).
Regarding claims 1, 2, 4, 5, 8, 9, 10, 11, 16, 17:
Gao is directed to a method for forming graphene films without wrinkles from graphene films containing wrinkles (Abstract; [0001], [0006]). As part of their overall method, Gao discloses a method of forming a wrinkled [3D origami2] graphene ([0011], [0050], [0053], [0056]). In a specific embodiment, Gao discloses that their method for growing the wrinkled graphene comprises (all steps disclosed in [0050]):
placing a copper substrate [meeting claim 2] in a tubular furnace [reaction chamber];
introducing argon [carry gas, meeting claims 4, 5] and hydrogen into the tubular furnace at a respective ratio of 10:1 and holding the flow for 40 minutes, thus purging the tubular furnace and introducing hydrogen;
heating the tubular furnace and its contents to 1000°C [close to melting point of copper at 1084°C and about 1080°C in light of the indefiniteness of claims, meeting claims 8 and 9];
introducing a 1% diluted methane gas flow [precursor flow, meeting claim 10] for 600 to 3600 seconds [10 to 60 minutes, meeting claim 11], thus depositing a flat graphene layer onto the substrate ([0050], [0005] with regards to wrinkling occurring during cooling);
naturally cooling the deposited graphene and substrate to form a wrinkled graphene; and
treating the deposited graphene to, among other embodiments, reduce the height of the wrinkles ([0019]; claim 8).
In Fig. 2 a-d, Gao discloses an embodiment of “wrinkle-free” graphene that was grown on a copper surface ([0030], [0064]). As evident in Fig. 2b, atomic force microscopy reveals that the deposited graphene takes on a periodic structure that can be characterized as triangular or rhomboidal [rectangular]; Furthermore, Fig. 2c indicates that while minimized the deposited graphene sheet still contained peaks and valleys that peak at 3 micrometers, thus indicating that both the deposited graphene before the treatment and after the treatment are origami 3-dimensional graphene films. Finally, Gao discloses that the heating time for the deposition of the graphene film, the heating temperature and subsequent treatment parameters affect the height and distribution of graphene wrinkles ([0019], [0024]).
Gao does not expressly teach that the cooling rate of the substrate is at a rate of about 2 – 6 °C per minute; and that the provided flow of carry gas, hydrogen and precursor into the reaction chamber is at a volume ratio of about 1000:5:1 to 1000:5:3.
With regards to the cooling rate of the substrate:
Lin is directed to the synthesis of graphene by chemical vapor deposition (CVD) having wrinkles (Abstract; page 508). Lin discloses that their CVD method comprises:
providing a nickel foam [substrate, meeting claim 2] and pre-heating the nickel foam substrate to 1000°C (page 507 Experiment);
growing a flat graphene layer onto the surfaces of the nickel foam substrate by introducing methane gas [meeting claim 10] alongside the hydrogen gas and argon at specific flow rates for 10 minutes [meeting claim 11]; and
cooling the coated nickel foam substrate at specified cooling rates in an atmosphere of H2 and Ar without methane gas [purging the reaction chamber, introducing a flow of hydrogen, meeting claims 4 and 5] to form graphene films with wrinkles (page 508).
Lin discloses that induced wrinkles of graphene formed by CVD are formed by mismatch in thermal expansion between the nickel foam substrate and the graphene; the nickel foam substrate contracts more than the graphene during postgrowth cooling (page 508). As the effects of thermal mismatch is a function of the difference of temperature from the beginning of cooling to the end of cooling alongside the cooling rate, the initial heating rate likewise affects the amount of wrinkling that occurs as it provides more time for the thermal mismatch to act upon the graphene film and the nickel foam substate. The amount of wrinkling affects the specific capacitance of the resulting graphene-nickel composite (Fig. 2; page 508).
With regards to the relationship between the specific capacitance and the cooling rate after deposition of flat graphene, Lin discloses experimental results of the specific capacitance of wrinkled graphene sheets that were produced by practice of the method of Lin at different cooling rates (Fig. 2; page 508). Higher cooling rates leads to higher specific capacitances while lower cooling rates lead to lower specific capacitances. Furthermore, the number of graphene layers that are deposited is a function of the cooling rate (page 506 1st column). Lin indicates a trendline where the lower the cooling rate, the lower the specific capacitance of the resultant graphene. Lin furthermore associates the cooling rate with wrinkling behavior; graphene that is cooled at a higher cooling rate possesses more wrinkles which in turns affects the total surface area of the graphene leading to an increase of the specific capacitance (page 508 bottom; Fig. 3). Likewise a slower cooling rate would be readily inferred to lead to lower specific capacitances because less wrinkles are formed.
Furthermore, Lin discloses that the number of graphene layers deposited also depends on the cooling rate during chemical vapor deposition (page 506).
Therefore, it would have been obvious to one of ordinary skill before the effective filing date of the claimed invention to have modified the method of Gao to obtain desired wrinkle heights, including to become “wrinkle-free” by controlling the cooling rate because Lin teaches that the amount and nature of wrinkling CVD-grown graphene affects the specific capacitance of the resultant graphene film. Optionally and additionally, both Lin and Lai also disclose that the cooling rate is controlled to determine the amount of graphene layers that are deposited.
Additionally, it would have been obvious to one of ordinary skill before the effective filing date of the claimed invention to have modified the method of Gao in view of Lin by cooling the substrate within the claimed ranges as a matter of routine experimentation in order to set a desired given specific capacitance of the graphene film and desired film morphology/ graphene layer number, including desired wrinkle heights for a given desired application of the graphene film. Discovery of optimum value of result effective variable in known process is ordinarily within skill of art. In re Boesch, CCPA 1980, 617 F.2d 272, 205 USPQ215.
With regards to the provided flow of carry gas, hydrogen and precursor into the reaction chamber is at a volume ratio of about 1000:5:1 to 1000:5:3:
Lin discloses that in their experiment the argon gas may be supplied at a volumetric flow rate of 1000 sccm and hydrogen at volumetric flow rates e.g. 100 sccm, 75 sccm or 50 sccm (Fig. 4; page 107 1st column, page 109 1st column). Lin also discloses that in their experiment a flow of precursor gas may be 50 sccm and a flow of hydrogen may be 100 sccm, 75 sccm, or 50 sccm [1:2, 1:1.5, 1:1 respectively] (page 507 1st col). Lin further discloses that their experiments concerning cooling occur with 1000 sccm of argon with a variable amount of hydrogen. Lin further discloses that the amount of hydrogen flowing concurrently with argon gas affects the specific capacitance of the resultant graphene film (Fig. 4, page 509 2nd paragraph).
Outside of a showing of unexpected results commensurate with the scope of the claims, it would have been obvious to one of ordinary skill before the effective filing date of the claimed invention to have modified the amount of hydrogen flowing in the cooling of the graphene relative to both the amount of argon flowing and precursor flowing as a matter of routine experimentation in order to obtain a desired specific capacitance. Discovery of optimum value of result effective variable in known process is ordinarily within skill of art. In re Boesch, CCPA 1980, 617 F.2d 272, 205 USPQ215. Accordingly, as the amount of hydrogen is optimized, so is the ratio of precursor to hydrogen and carry gas to hydrogen may overlap with the claimed value.
Regarding claim 12:
Gao discloses that the 1% diluted methane gas flow is introduced for 600 to 3600 seconds [10 to 60 minutes] ([0050]).
While Gao does not expressly teach that the precursor gas is provided for a period of about 30 to 45 minutes, Gao does disclose an overlapping range. In the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art”, a prima facie case of obviousness exists. In re Wertheim, 541 F.2d 257, 191USPQ 90 (CCPA 1976); In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990); In re Geisler, 116 F.3d 1465, 1469-71, 43 USPQ2d 1362, 1365-66(Fed. Cir. 1997). See MPEP 2144.05.
Claim(s) 3 is/are rejected under 35 U.S.C. 103 as being unpatentable over Gao in view of Link and optionally in view of Lai as applied to claims 1 – 2, 4 – 5, 8 – 12, 16 – 17 above, and further in view of Lai GB 2530974A (hereafter “Lai”).
Regarding claim 3:
Gao discloses that the substrate may be made of copper ([0050]).
Gao in view of Lin does not expressly teach that the thickness of the copper substrate has a thickness from about 0.025 mm to about 0.1 mm.
Lai is directed to the manufacture of graphene-copper-graphene heterogeneous films (Abstract). Lai discloses a method of depositing graphene onto two copper substrate that differ in thickness: one copper substrate has a thickness of 25 micrometers (0.025 mm) and the other has a thickness of 9 micrometers (page 6 2nd paragraph, page 7 2nd paragraph; Fig. 3). Lai discloses that after growing the graphene at e.g. 1030°C, the substrate is cooled at a controlled cooling rate to e.g. room temperature (Abstract; Fig. 1; pages 3, 5; Claim 1).
Lai additionally discloses that the grain size of the copper substrate is directly proportional to the thickness of the copper substrate (page 8 2nd paragraph) and that the grain size affects the amount of defects of copper surfaces that in turn affects the properties of graphene grown on the copper substrate (page 9 2nd full paragraph, page 2 1st paragraph).
Therefore, it would have been obvious to one of ordinary skill before the effective filing date of the claimed invention to have modified the method of Gao in view of Lin by depositing a flat graphene layer onto a copper substrate with a thickness within the claimed range of thicknesses as a matter of routine experimentation to optimize control of the grain sizes of the copper substrate that affects graphene growth and material properties of a graphene-copper heterogenous film. "[W]here the general conditions of a claim are disclosed in the prior art, it is not inventive to discover the optimum or workable ranges by routine experimentation." In re Aller, 220 F.2d 454, 456, 105 USPQ 233, 235 (CCPA 1955).
Response to Arguments
Applicant's arguments filed October 23, 2025 have been fully considered but they are not fully persuasive.
Some of the Applicant’s arguments do not directly touch on the new grounds of rejection (necessitated by amendment), but are relevant to the present rejection of the claims. Applicant’s relevant arguments are:
a.) Lin teaches away from the presently claimed method. Fig. 3 of the Lin reference indicates that graphene being cooled at a higher cooling rate possessed more wrinkles. Gao and Lai do not teach or suggest cooling the substrate having the flat graphene layer deposited thereon in step (e) to ambient temperature at a rate of about 2-6°C/min as recited in claim 1.
b.) Lai is directed to a method of forming graphene-Cu-graphene heterogenous films and not a graphene with origami structure on a substrate.
In response to the applicant's arguments, please consider the following comments.
a.) A prior art reference that "teaches away" from the claimed invention is a significant factor to be considered in determining obviousness. However, "the nature of the teaching is highly relevant and must be weighed in substance. In re Gurley, 27 F.3d 551, 553, 31 USPQ2d 1130, 1132 (Fed. Cir. 1994).
As discussed in the rejection above, while Gao professes a desire for wrinkle free graphene sheets, Gao also discloses specific embodiments where there is some wrinkling that is present (Fig. 2 (b) and (c); [0019], [0030]) in addition to the finding that following of the steps of the method within Gao that reads upon the method (outside of the difference addressed by Lin) renders a pronounced graphene film.
With regards to Lin, Applicant’s argument does not appreciate the actual teachings of Lin. Lin does not expressly state that a cooling rate dropped to 10°C/min produces no wrinkles. Lin actually teaches that “The graphene being cooled to ambient temperatures at a higher cooling rate possessed more wrinkles (See Fig. 3).” Less wrinkles is not the same as no wrinkles. The Examiner also respectfully disagrees with the Applicant’s characterization of what Fig. 3 (a) teaches. While the FESEM (field emission scanning electron microscopy) images show a relatively smooth graphene film, such a film still has wrinkles as shown by the lighter areas of the image compared to the darker regions of the image.
Both Gao and Lin discuss the general methodology of forming graphene films by CVD from a catalytic metal surface by heating and cooling in specific environments having hydrogen and precursor gases. Therefore, the principle of operation between Gao and Lin are the same, differing only by parameters for the purposes of tuning specific desired properties with a reasonable expectation of success.
Based on the totality of the teachings and the context of such teachings, the Examiner maintains the position that a prima facie case of obviousness exists against the claimed subject matter.
b.) In response to applicant's argument that Lai is nonanalogous art, it has been held that a prior art reference must either be in the field of the inventor’s endeavor or, if not, then be reasonably pertinent to the particular problem with which the inventor was concerned, in order to be relied upon as a basis for rejection of the claimed invention. See In re Oetiker, 977 F.2d 1443, 24 USPQ2d 1443 (Fed. Cir. 1992). In this case, the teachings of Lai are reasonably pertinent to the particular problem with which the inventor is concerned and within the field of endeavor. Lai discloses considerations for CVD deposition of graphene and teaches CVD deposition on both sides of a Cu substrate to result in the “heterologous films” (page 5). The field of endeavor is therefore the same as that of the claimed invention. Furthermore, discussion of a method that involves the deposition of graphene onto copper naturally is reasonably pertinent to the particular problem with which the inventor is concerned because consideration of deposition conditions over similar methods and the results of such methods would have informed one of ordinary skill in the art to the state of the art concerning graphene films on substrates, and thus reasonably pertinent.
Conclusion
Applicant is invited to hold an interview with the Examiner concerning the present application to further prosecution.
Applicant's amendment necessitated the new ground(s) of rejection presented in this Office action. Accordingly, THIS ACTION IS MADE FINAL. See MPEP § 706.07(a). Applicant is reminded of the extension of time policy as set forth in 37 CFR 1.136(a).
A shortened statutory period for reply to this final action is set to expire THREE MONTHS from the mailing date of this action. In the event a first reply is filed within TWO MONTHS of the mailing date of this final action and the advisory action is not mailed until after the end of the THREE-MONTH shortened statutory period, then the shortened statutory period will expire on the date the advisory action is mailed, and any extension fee pursuant to 37 CFR 1.136(a) will be calculated from the mailing date of the advisory action. In no event, however, will the statutory period for reply expire later than SIX MONTHS from the date of this final action.
Any inquiry concerning this communication or earlier communications from the examiner should be directed to JOSE I HERNANDEZ-KENNEY whose telephone number is (571)270-5979. The examiner can normally be reached M-F 6:30-3:30.
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If attempts to reach the examiner by telephone are unsuccessful, the examiner’s supervisor, Dah-Wei Yuan can be reached on (571) 272-1295. The fax phone number for the organization where this application or proceeding is assigned is 571-273-8300.
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/JOSE I HERNANDEZ-KENNEY/
Primary Examiner
Art Unit 1717
1 In the case of alloys, which is encompassed by the scope of a substrate in the present claims, the Examiner interprets the “melting point” to refer to a given alloy’s bulk solidus temperature.
2 Under the broadest reasonable interpretation consistent to the specification, wrinkles of graphene are considered 3D origami structures in light of original claim 18, and paragraph [0016] and [0027] of the originally filed disclosure.