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 .
Information Disclosure Statement
The information disclosure statement (IDS) submitted on 11 September 2023 was filed prior to the mailing date of this office correspondence. The submission is in compliance with the provisions of 37 CFR 1.97. Accordingly, the information disclosure statement is being considered by the examiner.
Drawings
The drawings are objected to under 37 CFR 1.83(a). The drawings must show every feature of the invention specified in the claims. Therefore, the claimed graphene electrode socket as claimed in claim 7 must be shown or the feature(s) canceled from the claim(s). See, Fig. 5 and the specification para. [0067] (of the PG PUB) describes a rectangular graphene electrode slot (32). A graphene electrode socket is shown in the drawings. No new matter should be entered.
Corrected drawing sheets in compliance with 37 CFR 1.121(d) are required in reply to the Office action to avoid abandonment of the application. Any amended replacement drawing sheet should include all of the figures appearing on the immediate prior version of the sheet, even if only one figure is being amended. The figure or figure number of an amended drawing should not be labeled as “amended.” If a drawing figure is to be canceled, the appropriate figure must be removed from the replacement sheet, and where necessary, the remaining figures must be renumbered and appropriate changes made to the brief description of the several views of the drawings for consistency. Additional replacement sheets may be necessary to show the renumbering of the remaining figures. Each drawing sheet submitted after the filing date of an application must be labeled in the top margin as either “Replacement Sheet” or “New Sheet” pursuant to 37 CFR 1.121(d). If the changes are not accepted by the examiner, the applicant will be notified and informed of any required corrective action in the next Office action. The objection to the drawings will not be held in abeyance.
Claim Objections
Claims 1-5 are objected to because of the following informalities:
In claim 1, lines 3-7:
“producing a graphene oxide coated nanofiber surface with graphene oxide solution in a graphene oxide solution feeding syringe, on a PVDF nanofiber mat formed on a rotating drum by electrospray method, with the help of a high voltage source in the voltage range of 10- 40 kV; and
soaking the graphene oxide coated nanofiber surface in hydrazine hydrate solution for the conversion of the graphene oxide coated nanofiber surface to the reduced graphene oxide coated nanofiber surface after the graphene oxide coating process.” should read:
-- producing a graphene oxide coated nanofiber surface by feeding a graphene oxide solution from a graphene oxide solution feeding syringe, onto a PVDF nanofiber mat formed on a rotating drum by electrospray method, using a high voltage source between 10 kV and 40 kV; and
after coating the graphene oxide solution, soaking the graphene oxide coated nanofiber surface in a hydrazine hydrate solution for the conversion of the graphene oxide coated nanofiber surface to a reduced graphene oxide coated nanofiber surface. --
In claims 2-5, line 1: “An electrode production method” should read:
-- The electrode production method --
In claim 4, line 8: “adding 1 ml of” should read: -- adding 1 mL of --
Appropriate correction is required.
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 6-7 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.
In claim 6, the limitation “An electrode, which increases the mechanical stress resistance of the reduced graphene oxide-coated nanofibrous structure as a result of the reduced graphene oxide-coated nanofibrous structure tightly wrapping the PVDF nanofiber mat of the reduced graphene oxide coating and increases the output voltage and output current obtained from nanogenerators by the same tightly wrapping structure is used to increase the interface area of the PVDF nanofiber mat with reduced graphene oxide coating” is confusing. As best understood, it appears that the limitation actually intends that, an electrode, having increased mechanical stress resistance, output voltage and output current obtained as a result of tightly wrapping the reduced graphene oxide onto the PVDF nanofiber mat, and increasing an interface area of the PVDF nanofiber mat and the reduced graphene oxide fiber, or the like.
In claim 7, the limitation “a graphene electrode socket” renders claim indefinite because it is unclear what does the claimed socket mean. Both specification and the drawings fail to define the claimed socket. As best understood, it appears that the limitation “A piezoelectric nanogenerator with a graphene electrode comprising a graphene electrode socket in the middle of spacer paper positioned between two aluminum electrodes and an electrode according to claim 6 placed in the said graphene electrode socket.” actually intends that, “A piezoelectric nanogenerator structure comprising the electrode according to claim 6 stacked with a graphene electrode, wherein the piezoelectric nanogenerator structure is positioned between two aluminum electrodes, and wherein the graphene electrode is positioned in the middle of a spacer paper”, or the like.
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.
Claim(s) 1-6 are rejected under 35 U.S.C. 103 as being unpatentable over Unsal (Unsal et.al., “Poly(vinylidene fluoride) nanofiber-based piezoelectric nanogenerators using reduced graphene oxide/polyaniline”, J of Applied Polymer Science, 2019, pp 48517, one of the prior arts listed in 09/11/2023 IDS) in view of Yang (Yang et.al., “Piezoelectric Nanogenerators based on Graphene Oxide/PVDF Electrospun Nanofiber with Enhanced Performances by In-Situ Reduction”, Materials Today Communications, 26, 2021, 101629).
Regarding claim 1, Unsal teaches, a production method of an electrode containing reduced graphene oxide for use in piezoelectric generators (electrospun poly (vinylidene fluoride) (PVDF) nanofiber-based piezoelectric nanogenerators with reduced graphene oxide (rGO), Abstract) comprising the following steps:
producing a graphene oxide coated nanofiber surface (nanofiber-based piezoelectric nanogenerators with reduced graphene oxide (rGO), Abstract) with graphene oxide solution in a graphene oxide solution feeding syringe (needle collector, page 4, col. 2), on a PVDF nanofiber mat (PVDF nanofiber mats, page 5, col. 2) formed on a rotating drum by electrospray method (preparation of spray-coated nanofiber mats with PANI, rGO, and rGOPANI…nanoparticle solution…were sprayed onto each side of PVDF nanofiber mats, page 4 col. 2 to page 5, col. 1), with the help of a high voltage source in the voltage range of 10- 40 kV (electrospinning of neat PVDF nanofibers was fabricated at 4 mL h−1 of feeding rate, 20 cm of needle-collector distance, 30 kV of voltage, page 4, col. 1); and
soaking the graphene oxide coated nanofiber surface in hydrazine hydrate solution for the conversion of the graphene oxide coated nanofiber surface to the reduced graphene oxide coated nanofiber surface after the graphene oxide coating process (500 mg of GO was homogenized in 500 mL of water, and 8.55 mL and 55% hydrazine monohydrate was added into the dispersion. The reaction begun at 950C and continued for 12 h, page 3, col.1, a reduction process with hydrazine was performed, page 3, col. 2).
[AltContent: arrow][AltContent: textbox (PVDF nanofiber mat)]
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Annotated Fig. 1, Yang.
Unsal does not explicitly teach, preparing an electrode. However, Yang teaches, a production method of an electrode (polymer-based piezoelectric nanogenerator electrode, Fig. 1) containing reduced graphene oxide for use in piezoelectric generators (graphene oxide (GO) was added into polyvinylidene fluoride (PVDF) to prepare nanofiber mats by electrospinning, Abstract, page 2, col. 1) comprising: producing a graphene oxide coated nanofiber surface with graphene oxide solution in a graphene oxide solution feeding syringe (see annotated Fig. 1), on a PVDF nanofiber mat (PVDF film and GO/ PVDF nanofiber mat, page 2, col. 1) formed on a rotating drum by electrospray method (PVDF and filler were mixed together and then the spinning solution spurted out and was collected to form a nanofiber mat, page 2, col. 2), with the help of a high voltage source in the voltage range of 10- 40 kV (electrospun via a high voltage electrospinning apparatus, voltage =14 kV, page 2, col. 2); reduced graphene oxide coated nanofiber surface after the graphene oxide coating process (reduced GO (rGO)/PVDF composite nano nanofiber mats, page 2, col. 1).
Unsal teaches spray-coating method for industrial production of nanogenerators. Yang teaches producing an electrode comprising graphene oxide coated nanofiber surface by electrospinning graphene oxide solution in a graphene oxide solution through a feeding syringe. Therefore, in view of the teachings of Yang, it would have been prima facie obvious to one of ordinary skill in the art before the effective filing date of the claimed invention, to modify the production method of an electrode containing reduced graphene oxide of Unsal and to include preparing an electrode as Yang taught in Figs. 1 and 4 so that it enables manufacturing an electrode having improved power generation performance. Moreover, there is no indication in the instant invention that any surprising results were derived, or that any special steps were devised in forming the electrode, or feeding or spraying the graphene oxide solution. Such a combination would have been done by one of ordinary skill in the art without any need for experimentation and with reasonable expectations of success.
Regarding claim 2, Unsal in view of Yang teaches the recited limitations with respect to claim 1. Unsal further teaches, an electrode production method according to claim 1,comprising; exposing the PVDF nanofiber mat formed on the rotating drum to the solution from a distance of 8 cm with a solution feed rate of 30 mL/h in the potential difference provided by the high voltage source in the step of producing the graphene oxide coated nanofiber surface by electrospray method (electrospinning of neat PVDF nanofibers was fabricated at 4 mL/h of feeding rate, 20 cm of needle-collector distance, 30 kV of voltage, and 300 rpm of collector spin rate, page 4, col. 1).
Regarding claim 3, Unsal in view of Yang teaches the recited limitations with respect to claim 1. Unsal further teaches, an electrode production method according to claim 1, wherein in the graphene oxide coating step with the electrospray method on the PVDF nanofiber mat, the graphene oxide solution in the graphene oxide solution feeding syringe contains the graphene oxide solution that is mixed with 0.5 mg/mL of graphene oxide produced by Hummers’ method in a solvent containing deionized water and 2-propanol by volume (production of rGO was carried out according to improved Hummers’ method, page 3, col. 1).
Regarding claim 4, Unsal in view of Yang teaches the recited limitations with respect to claim 3. Unsal further teaches, an electrode production method according to claim 3, wherein the Hummer's method comprises the steps of:
dispersing 1 gram of graphite powder into 120 mL of concentrated sulfuric acid and 13.3 mL of concentrated phosphoric acid mixture, adding 6 grams of potassium permanganate into graphite-acid mixture and maintaining of the reaction for 12 hours at 50 °C, pouring 120 mL of ice on the mixture obtained after 12 hours, adding 1 ml of hydrogen peroxide in order to eliminate the excess amount of potassium permanganate, separating solid graphene oxide and supernatant by centrifugation, repeating the centrifugation process at least once, by washing the solid material separately with ethyl alcohol and HCI between the centrifugation processes (production of rGO was carried out according to improved Hummers’ method. Two grams of graphite powder, 240 mL sulfuric acid, and 26.6 mL phosphoric acid were mixed in a reaction flask for 30 min. Then, 12 g of potassium permanganate was added into the mixture. The reaction mixture was taken in an oil bath at 50 0C, and the reaction was continued for 12h …mixture was poured onto 300 mL deionized water ice, and 2 mL 30% hydrogen peroxide was added. Stirring was continued for 30 min. Finally, GO and liquid phase were separated with centrifugation,… resulting solid was washed with ethanol, HCl, and water, respectively, page 3, col 1).
Regarding claim 5, Unsal in view of Yang teaches the recited limitations with respect to claim 3. Unsal further teaches, an electrode production method according to claim 1, wherein said hydrazine hydrate solution, which enables the conversion of the graphene oxide coated nanofiber surface to the reduced graphene oxide coated nanofiber surface after the graphene oxide coating process, is 0.3 molar (8.55 mL and 55% hydrazine monohydrate was added into the dispersion, page 3, col. 1).
Regarding claim 6, Unsal in view of Yang teaches the recited limitations with respect to claim 1. Unsal further teaches, increases the mechanical stress resistance of the reduced graphene oxide-coated nanofibrous structure as a result of the reduced graphene oxide-coated nanofibrous structure tightly wrapping the PVDF nanofiber mat of the reduced graphene oxide coating and increases the output voltage and output current obtained from nanogenerators by the same tightly wrapping structure is used to increase the interface area of the PVDF nanofiber mat with reduced graphene oxide coating, is obtained by claim 1 (mechanical sensitivity of D11 was considerably higher compared with the other doped and coated samples…small-sized rGO layers penetrated into the nanofiber mat and wrapped the individual nanofibers in the inner layers… output voltage, which was 1.92 V for neat PVDF nanofiber mat, was increased by coating and doping processes… rGOPANI coating material, PANI and rGO brought out a synergistic effect and produced a higher voltage than other materials, page 12, col. 1 to 2).
Yang teaches, an electrode comprising reduced graphene oxide. Therefore, in view of the teachings of Yang, it would have been prima facie obvious to one of ordinary skill in the art before the effective filing date of the claimed invention, to modify the production method of an electrode containing reduced graphene oxide of Unsal and to include preparing an electrode as Yang taught in Figs. 1 and 4 so that it enables manufacturing an electrode having improved mechanical stress resistance, and power generation performance.
Claim(s) 7 is rejected under 35 U.S.C. 103 as being unpatentable over Unsal in view of Yang as applied to claim 1 above, and further in view of Miwa (US 20130065120).
Regarding claim 7, Unsal in view of Yang teaches the recited limitations with respect to claim 6. Unsal further teaches, a piezoelectric nanogenerator with a graphene electrode comprising a graphene electrode socket (see Fig. 1) in the middle of two aluminum electrodes (nanofiber mats were placed between two aluminum foil-coated PDMS films, page 5, col. 2). Modified Unsal does not teach a graphene electrode. However, Miwa teaches a production method of an electrode including the graphene oxide or multilayer graphene oxide or reduced graphene oxide or reduced multilayer graphene oxide (para. [0041]), and middle spacer paper (insulating porous materials, can be used as the separator…for example, paper, para. [0075]). Therefore, in view of the teachings of Miwa, it would have been prima facie obvious to one of ordinary skill in the art before the effective filing date of the claimed invention, to modify the production method of an electrode containing reduced graphene oxide of Unsal and to prepare an electrode as Miwa taught in Fig. 2B so that it enables manufacturing an electrode having improved energy density and output performance.
Conclusion
Prior art Joo (US 20190044143) teaches production method of an electrode comprising piezoelectric nanogenerators including an electrospray process for forming graphene oxide in piezoelectric binder; and forming a reduced graphene oxide coated nanofiber surface by treating with hydrazine hydrate solution.
Prior art Ongun (Ongun et.al., Enhancement of piezoelectric energy-harvesting capacity of electrospun β-PVDF nanogenerators by adding GO and rGO, Journal of Materials Science: Materials in Electronics (2020) 31:1960–1968) teaches a production method of nanogenerators including electrospinning graphene oxide for use in piezoelectric generators including PVDF polymeric material and electrospun nanofibers, with the help of a high voltage source; and forming a reduced graphene oxide coated nanofiber surface using hydrazine hydrate solution.
Prior art Fei (Fei, L., et. al., Graphene Oxide Involved Air-Controlled Electrospray for Uniform, Fast, Instantly Dry, and Binder-Free Electrode Fabrication, Applied Materials Interfaces 2017, 9, 9738-9746) teaches a production method of piezoelectric nanogenerators including electrospray method that directly depositing binder-free active materials/graphene oxide (GO) onto current collectors.
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/JOSE K ABRAHAM/Examiner, Art Unit 3729
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