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 .
Status of Amendment
The amendment filed on 22 December 2025 fails to place the application in condition for allowance.
Claims 1 and 5-21 are currently pending and under examination.
Status of Rejections
The rejection of claims 1 and 5-21 under 35 U.S.C. 103(a) are herein maintained.
Claim Interpretation
As to claim 1, the recitation of “an aqueous electrolyte comprising a combination of multiple exfoliating ions of different sizes, wherein the combination of exfoliating ions are used stepwise…” is interpreted in light of the specification’s Exampled 18 and 19 as cited by Applicant for support for the stepwise limitation. Applicant further contrasts these Examples to Example 6 which uses a combination of ions. Example 18 and 19 has been offered up as supporting the use of a first and second electrolyte, each comprising a different ion to be used separately (See for example pg. 6 1st paragraph and pg. 7 2nd paragraph of the response filed 3 March 2025). The Example uses 2 ions in a stepwise fashion using the same voltage of 10V. Thus, it stands to reason that if both ions were in the same solution, they both would be simultaneously participating in the intercalation and not actually used in a stepwise fashion. The specification is silent as to any special method steps, parameters, or the like to enable a stepwise intercalation using mixture of the ions at the same applied potential. Therefore, for examination on the merits, the “stepwise” is herein interpreted to not require a mixture of the ions in the same electrolyte solution, but allow for an exchange of aqueous electrolyte solutions. Any other interpretation would rend the claims unenabled under 35 U.S.C. 112(a) due to the lack of written description as to how the enable stepwise intercalation of a mixture of ions in the same solution at the same potential, lack of any control or predictability of such a process, and lack of direction provided with respect to such an interpretation.
Claim Rejections - 35 USC § 112
The following is a quotation of the first paragraph of 35 U.S.C. 112(a):
(a) IN GENERAL.—The specification shall contain a written description of the invention, and of the manner and process of making and using it, in such full, clear, concise, and exact terms as to enable any person skilled in the art to which it pertains, or with which it is most nearly connected, to make and use the same, and shall set forth the best mode contemplated by the inventor or joint inventor of carrying out the invention.
The following is a quotation of the first paragraph of pre-AIA 35 U.S.C. 112:
The specification shall contain a written description of the invention, and of the manner and process of making and using it, in such full, clear, concise, and exact terms as to enable any person skilled in the art to which it pertains, or with which it is most nearly connected, to make and use the same, and shall set forth the best mode contemplated by the inventor of carrying out his invention.
Claims 1 and 5-21 rejected under 35 U.S.C. 112(a) or 35 U.S.C. 112 (pre-AIA ), first paragraph, as failing to comply with the enablement requirement. The claim(s) contains subject matter which was not described in the specification in such a way as to enable one skilled in the art to which it pertains, or with which it is most nearly connected, to make and/or use the invention.
Addressing now the "Wands" factors (MPEP 2164.01 (a)).
(A) The breadth of the claims:
The breadth of the claims requires a stepwise use of a first and second electrolyte solutions with particular exfoliating ions in order to perform the exfoliation. The claims generically require the formation of “high quality graphene”.
(B) The nature of the invention:
The claims are drawn towards producing graphene via an electrochemical cell.
(C) The state of the prior art:
The most relevant prior art is deemed to be previously cited Huang and Parvez.
(D) The level of one of ordinary skill:
One of ordinary skill in the art would have an understanding of electrochemical exfoliation and the associated mechanism by which exfoliation takes place to form graphene.
(E) The level of predictability in the art:
Based on previously cited Parvez, the nitrate ion would be expected to not display exfoliation of the graphite electrode when performed 10 V for 10 minutes in 0.1 M NaNO3. (See Supporting information Figure S2). Thus, one of ordinary skill in the art carrying out the instantly claimed method would predict that the sodium nitrate would not result in exfoliation of the graphene.
Parvez further discloses in Table S1 that the sodium nitrate results in “poor exfoliation” with very low product yield. Thus, the suggestion would be either that exfoliation does not take place or it takes place producing a small quantity of graphene.
(F) and (G) The amount of direction provided by the inventor and the existence of working examples:
Table 1 provides a discussion of particular combinations of exfoliation ions and the amount of product produces. Examples 5-15 use a singular electrolyte solution with only Example 15 a singular exfoliation ion from nickel nitrate. The concentration, time, or applied potential for Example 15 is not disclosed. The disclosure explicitly states that “examples 13-15 show very kinetically sluggish processes…” (pg. 17 lines 16-17 of the as filed specification).
It is not clear from Examples 18 and 19 the amount of graphene produced using each electrolytic solution. In other words, the amount of graphene produced in the two methods is a result of the combined process and not directly from either the first or second electrolyte solution.
Example 19 first performs exfoliation sodium nitrate followed by a second solution using ammonium sulfate and results in about 0.6 g graphene produced. Example 15 does not provide any actual process conditions which would result in the formation graphene using only a nickel nitrate solution. Example 15 provides an expected amount of 0.4 g of graphene produces where Example 5 using only ammonium sulfate at the same exfoliation time of 2:30 hours results in a formation of 0.8 g of graphene produced. Thus, one of ordinary skill in the art would expect an enhanced yield using two exfoliation steps instead of just a singular exfoliation step. In other words, using only ammonium sulfate without a preceding step using sodium nitrate results in more graphene produced. While Example 18 shows a greater yield than Example 19, it is still lower (1.1 grams) than would be expected performing a combined process using Example 15 and Example 5 (0.4+0.8 = 1.2 g).
(H) The quantity of experimentation needed to make or use the invention based on the content of the disclosure:
The Examiner has no comment on the quantity of experimentation.
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.
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.
Claims 1-2, 5-8, and 11-18 are rejected under 35 U.S.C. 103(a) as being unpatentable over Huang et al (Nanotechnology, vol. 26, pg. 1-6, 2015 as provided with the IDS dated 15 May 2024) in view of Parvez (J. Am. Chem. Soc., vol. 136, pp. 6083-6091, 2014 as provided with the IDS dated 15 May 2024).
As to claim 1, Huang discloses a method of making a high quality graphene (Title) comprising:
Providing an electrochemical cell (Fig. 1A) wherein the electrochemical cell comprises:
One or more working electrodes (Fig. 1A graphite foil electrode)
One or more counter electrodes (Fig. 1A Pt flake electrode)
An aqueous electrolyte (electrolyte Fig. 1A]) comprising a combination of multiple exfoliating ions of different sizes (NaOH and H2SO4)
Exfoliating the working electrode to produce high quality graphene
wherein the combination of exfoliating ions are used stepwise (first with NaOH and subsequently with sulfuric acid – see Section 2.1),
wherein one exfoliating ion is used in a first electrolyte solution, followed by a second exfoliating ion in an second electrolyte solution, wherein the first electrolyte solution is different from the second electrolyte solution; (Section 2.1 methods “. The processes by the two-step electrochemical exfoliation method mentioned above were described as following. In the first step, the electrodes were placed into 1 M NaOH solution with a positive potential of +10 V for 10 min, and during this process, the graphite foil just expanded without obvious peeling. Then, the electrodes were transferred into 0.5 M H2SO4 electrolyte for further exfoliation.”)
wherein the exfoliating ions are generated through use of salts in aqueous media (via use of NaOH); and
wherein the high quality graphene has characteristics that are engineered for targeted applications (this limitation does not add anything specifically limiting as it can apply to literally any formation of the graphene in accordance with the electrochemical exfoliation, such as “thin FLG sheets with high quality…” pg. 105602 col. 1 1st half paragraph).
Huang discloses explicitly that the intercalation of hydroxide is used to expand the graphite without peeling then using the sulfate ion to perform the actual exfoliation due to the rapid generation of gas (Section 2.1 and Section 4 pg. 5). Huang states that the mechanism relied up in introduction of hydroxyl ions into the interlayer spacing of the foil which because of the size of the hydroxyl ion being smaller than the interlayer spacing, graphene is not exfoliated. Upon the addition of the sulfuric acid, two steps are involved 1) liberated hydrogen of dissociated sulfuric acid results in the formation of water which “may contribute to enlarging the interlayer spacing of the graphite” and 2) the intercalation of the sulfate ions where the generation of SO2 and the sulfate ion has a size larger than the interlayer distance, graphene is exfoliated (Section 4).
Huang fails to explicitly disclose the combination of ions are nitrate and the sulfate used stepwise, first exfoliating the nitrate and the secondly with the sulfate ion.
Huang fails to explicitly disclose wherein the sulfate ion is generated through use of a salt in an aqueous media.
Parvez discloses the use of the nitrate ion leads to an expansion of the graphite electrode and the sulfate ion exhibits pronounced exfoliation efficiency (p. 6084 col. 2 1st full paragraph). Parvez discloses the use of ammonium sulfate as a source of the needs sulfate ion (Title). Parvez discloses that upon application of a bias voltage, hydroxyl ions also attack the graphite electrode allowing the sulfate ions and water molecules to co-intercalate and cause subsequent exfoliation.
Thus, it would have been obvious to one of ordinary skill in the art at the time the invention was filed to have used sodium nitrate and ammonium sulfate as taught by Parvez in place of the sodium hydroxide and sulfuric acid for exfoliation in the method of Huang because the modification amounts to an obvious exchange of ions recognized to perform exfoliation of a graphite electrode with both processes of Huang and Parvez are used with water intercalation as well and provide an expected result of allowing expansion and exfoliation with nitrate and a sulfate ion from sodium nitrate and ammonium sulfate, respectively, which is efficient under neutral pH conditions (Parvez p. 6083 col. 2 last paragraph) which avoids a significant amount of oxygen containing functional groups brought about by overoxidation in an acid (Parvez p. 6083 col. 2 partial paragraph) which effectively reduces the oxidation degree and thereby significantly improves the chemical and electronic properties of graphene (Parvez conclusions). See MPEP 2144.07 and 2143 B.
As to the recitation of “wherein the NaNO3 exfoliates the graphene”, while Parvez discloses that the sodium nitrate is a poor exfoliator, Parvez does discloses that some exfoliation takes place (as opposed to none – see Supplementary Information Table S1). Thus, since Parvez carries out the process at the same voltage and same time, it would have been expected that some exfoliation of the graphene would have taken place in the combined process of Parvez and Huang. See MPEP 2112 II and 2112.02.
As to claims 5-7, Huang discloses performing the method at room temperature (pg. 2 section 2.1).
As to claim 8, Huang discloses using a graphite foil which may be considered synthetic or natural graphite as those are the only two options for a type of graphite.
As to claims 11-12, Huang discloses using platinum metal (Fig. 1A Pt flake electrode).
As to claims 13-15, Huang and Parvez both disclose using a voltage of 10 V (Huang section 2.1 Parvez p. 6084 col. 1 last pargraph).
As to claim 16, Huang, as modified by Parvez, disclose the use of neutral electrolytes when used with ammonium sulfate ( Parvez “under neutral pH onditions” pg. 6083 col. 2 last 3 lines) as well as the explicit use of 1M NaOH explicitly cited in Huang.
As to claim 17, Huang discloses wherein the engineered characteristic is inherently the size and number of layers (See Fig. 3) and surface functionalization via controlling the amount of oxygen bound to the surface via use of the ammonium sulfate as cited above.
As to claims 18, the recitation of “wherein the graphene is continuously removed from the electrolytic cell and continuously manufactured.” Would have been obvious to one of ordinary skill in the art to repeat the procedure to continuously form graphene and subsequently use it for further applications in Huang. See MPEP 2144.04 V E and 2144.04 VI B.
Claims 9, 19, and 20 are rejected under 35 U.S.C. 103 as being unpatentable over Huang, as modified by Parvez, as applied to claim 1 above, and further in view of Kurkina (EP 2878709 A1).
As to claim 9, Huang, as modified by Parvez, fails to explicitly disclose wherein the working electrode is produced from carbon powder or flakes compressed together to form sheets, rods, pellets, or combinations thereof.
Kurkina discloses wherein the working electrode may be preseed together powder or flakes in a rod ([0017]).
It would have been obvious to one of ordinary skill in the art at the time the invention was filed to have used a working electrode formed from pressed powder or flakes as taught by Kurkina in the method of Huang, as modified by Parvez, in the routine selection of providing an appropriate working electrode suitable for forming graphene in an electrochemical exfoliation process. See MPEP 2143 B and 2144.07.
As to claims 19 and 20, Huang, as modified by Parvez, fails to explicitly disclose wherein the voltage applies is of alternating polarity specified by duty cycled or is ramped.
Kurkina discloses wherein the polarity is alternating ([0050]-[0051]) which can inherently be specified by duty cycle and/or ramped since the recitation of “can be” does not impart further limitation as to the instant claim language, but rather an option of how the alternating polarity is applied.
It would have been obvious to one of ordinary skill in the art at the time the invention was filed to have used an alternating polarity with a duty cycle as taught by Kurkina in the method of Huang, as modified by Parvez, as the selection of the appropriate voltage is routine to one of ordinary skill in the art to provide the expected results of exfoliating the graphene. See MPEP 2144.07.
Claims 10 and 21 are rejected under 35 U.S.C. 103 as being unpatentable over Huang, as modified by Parvez, as applied to claim 1 above, and further in view of Achee et al (US 2019/0233291 A1).
As to claims 10, Huang, as modified by Parvez, fails to explicitly disclose wherein the working electrode is pretreated.
Achee discloses pretreating the working electrode via a thermal treatment ([0119]).
Thus, it would have been obvious to one of ordinary skill in the art at the time the invention was filed to have used a pretreatment as taught by Achee in the method of Huang, as modified by Parvez, in order to prepare the graphite for exfoliation.
As to claim 21, Huang, as modified by Parvez, fails to explicitly disclose the use of a membrane enclosure or bag.
Achee discloses wherein the electrodes are within a membrane (#100 in Figures 3-7).
Thus, it would have been obvious to one of ordinary skill in the art at the time the invention was filed to have used a membrane as taught by Achee in the method of Huang, as modified by Parvez, because it allows to maintain a pressure on the graphite material to maintain the condition necessary for the exfoliation (Achee [0044]).
Response to Arguments
Applicant's arguments filed 22 December 2025 have been fully considered but they are not persuasive.
In response to Applicant’s arguments on pgs. 5-6 of the response espousing technical advantages, these arguments are not persuasive because the claims are not commensurate in scope with the alleged process and specifics of the as formed graphene, and thus not in compliance with MPEP 716.02(d). Applicant notes an alleged higher thermal stability based on Figure 8. Applicant further cites that Fig. 9 shows the absence of the 2D band leads to evidence that the as formed produce possess few functional groups, and therefore defects when compared to Example 6 which uses the combination of ions just not in stepwise fashion. Interestingly, it is noted the curves of Examples 18 and 19 are very similar to curve of Example 5 of showing a reduced 2D curve using only ammonium sulfate as the electrolyte. Example 5 also shows a more stable thermal stability curve in Fig. 7 when compares to the curve of Examples 18 and 19 in Fig. 8. Based on Applicant’s own results, the combined stepwise process does not appear to produce a more stable graphene, and thus less desirable, than use of a singular ion electrolyte. Example 5 even has a higher yield than Example 19.
In response to Applicant’s arguments towards Huang and Parvez, the arguments are presented against the as amended claim limitations addressed herein and the rejections maintained for the reasons outline above. In response to applicant’s argument that there is no teaching, suggestion, or motivation to combine the references, the examiner recognizes that obviousness may be established by combining or modifying the teachings of the prior art to produce the claimed invention where there is some teaching, suggestion, or motivation to do so found either in the references themselves or in the knowledge generally available to one of ordinary skill in the art. See In re Fine, 837 F.2d 1071, 5 USPQ2d 1596 (Fed. Cir. 1988), In re Jones, 958 F.2d 347, 21 USPQ2d 1941 (Fed. Cir. 1992), and KSR International Co. v. Teleflex, Inc., 550 U.S. 398, 82 USPQ2d 1385 (2007). In this case, the result of the exfoliation when sodium nitrate is used would be at least somewhat expected due the disclosure that it leads to poor exfoliation. Thus would not dissuade one of ordinary skill in the art to use the particular ion for the reasons outlined above, where even poor exfoliation as a result of its use reads on the amended claim language of “wherein the NaNO3 exfoliates graphene”.
No further arguments are presented.
Conclusion
THIS ACTION IS MADE FINAL. 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 nonprovisional extension fee (37 CFR 1.17(a)) 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 mailing date of this final action.
Any inquiry concerning this communication or earlier communications from the examiner should be directed to LOUIS J RUFO whose telephone number is (571)270-7716. The examiner can normally be reached Monday to Friday, 9 am to 5 pm.
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/LOUIS J RUFO/ Primary Examiner, Art Unit 1795
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