DETAILED ACTION
Citation to the Specification will be in the following format: (S. # : ¶/L) where # denotes the page number and ¶/L denotes the paragraph number or line number. Citation to patent literature will be in the form (Inventor # : LL) where # is the column number and LL is the line number. Citation to the pre-grant publication literature will be in the following format (Inventor # : ¶) where # denotes the page number and ¶ denotes the paragraph number.
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 Application
The response dated 12/19/2025 has been received and will be entered.
Claim(s) 1-22 is/are pending.
Claim(s) 1, 4, 6, 12, 16, 19, and 21 is/are currently amended.
The action is FINAL.
Response to Arguments
Claim Rejections – 35 U.S.C. §112
I. With respect to the rejection of Claims 1-22 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 rejection was not addressed. Instead, the Remarks rely on amendments alone. (Remarks of 12/19/2025 at 6).
The amendment requiring graphene to actually be present in “a graphene/plastic mixture” eliminates the mathematical impossibility that was previously present in Claim 1, Claim 21, and all dependent claims identified in the Non-Final Office Action. That issue is obviated by amendment.
The amendment to Claim 6 corrects the antecedent basis issue.
The amendment to Claim 12 corrects the antecedent basis issue.
The amendment to Claim 16 corrects the antecedent basis issue.
The amendment to Claim 19 corrects the antecedent basis issue.
The rejection is WITHDRAWN.
Claim Rejections – 35 U.S.C. §§ 102-103
I. With respect to the rejection of Claim(s) 1-2, 8-10, 16-17, and 19-22 under 35 U.S.C. 102(a)(1) as being anticipated by Ko, et al., Preparation of synthetic graphite from waste PET plastic, Journal of Industrial and Engineering Chemistry 2020; 83: 449-458 (hereinafter “Ko at __”), the Remarks rely on the amendment narrowing Claim 1 and Claim 21 to require graphene. This is persuasive. The rejection is WITHDRAWN.
II. With respect to the rejection of Claim(s) 1-2, 3, 8-10, 16-17, and 19-22 under 35 U.S.C. 103 as being unpatentable over Ko, et al., Preparation of synthetic graphite from waste PET plastic, Journal of Industrial and Engineering Chemistry 2020; 83: 449-458 (hereinafter “Ko at __”) in view of: (i) Agnoli, et al., Doping graphene with boron: a review of synthesis methods, physiochemical characterization, and emerging applications, J. Mater. Chem. A 2016; 4: 5002-5025 (hereinafter “Agnoli at __”), the Remarks state: “Official notice of doping graphene with small amounds of dopands (boron) does not in any way suggest that the doped graphene could or should be substituted for boron. This makes no sense.” (Remarks of 12/19/2025 at 7).
In response: why not? Why does this not make sense? Why wouldn’t adding boron doped graphene to a composition that is to be graphitized (i.e. turned to graphene) not catalyze the graphitization of that which is to be turned into graphite/graphene? Boron is a graphitization catalyst. Ko teaches that it is a graphitization catalyst. (Ko at 450, col. 2 – Experimental). Applicants do not dispute this teaching from Ko. Graphitization catalysts are well described in the literature. In addition to the teachings of Ko, Applicants state elsewhere that Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Zr, Nb, Mo, Ru, Pd, Ag, Cd, Pt, Au, and combinations thereof are known graphitization catalysts. US 2019/0077668 to Zhamu, et al. was not provided on any IDS, but is made of record here. See (Zhamu ‘668 5: [0046]).
The rejection is obviated by the amendment narrowing Claim 1 and Claim 21 to require graphene. The rejection is WITHDRAWN.
Claim Rejections - 35 USC § 103
The text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
I. Claim(s) 1, 2, 4, 8, 9, 10, 11, 12, 14, 16, 17, 18, 19, 20, 21, and 22 - or as stated below - is/are rejected under 35 U.S.C. 103 as being unpatentable over Ko, et al., Preparation of synthetic graphite from waste PET plastic, Journal of Industrial and Engineering Chemistry 2020; 83: 449-458 (hereinafter “Ko at __”) in view of:
(i) Cunning, et al., Structure-directing effect of single crystal graphene film on polymer carbonization and graphitization, Mater. Horiz. 2019; 6: 796-801 (with Supporting Information, hereinafter “Cunning at ___”).
With respect to Claim 1, this claim requires “A) providing a graphene/plastic mixture of multiple plastic particles, having a plastic particle size from 10 nm to 10 cm, and a first amount of multiple sheets of a first graphene material, wherein the first graphene-to-plastic weight ratio is from 0.001 to 1.0, wherein the first graphene is selected from pristine graphene, having a carbon content greater than 99%, graphene oxide, reduced graphene oxide, halogenated graphene, nitrogenated graphene, hydrogenated graphene, doped graphene, chemically functionalized graphene, or a combination thereof.” Ko teaches 10 mm x 10 mm PET (plastic) particles. (Ko at 450, col. 2 – Experimental). Ko would not appear to recite any of the various graphene as claimed. Note however that Ko is generally directed to graphitizing plastic. (Ko, entire reference). Cunning teaches adding graphene to polymers prior to carbonization and graphitization. See (Cunning at 797, col. 1 et seq.: “we created thin polymer films with and without continuous layers of single crystal (or near single crystal) graphene embedded within the film to observe the effect graphene has when the polymer is subsequently carbonized and graphitized.”). Cunning provides other relevant teachings. For example, Cunning states:
“Adding crystalline carbon nanomaterials to carbonaceous precursors prior to heat treatment has been shown to influence the structure and texture of the heat-treated carbon adjacent to the crystalline region.” (Cunning at 797, col. 1).
“Thus, after heating to 1000 °C the presence of graphene promotes the ordering of carbon in the vicinity of the graphene.” (Cunning at 797, col. 2).
“The effect of graphene had a minor improvement in the crystallite parameters; from powder XRD measurements, the d-spacing of the (002) peak of SU-8_G_3000 is marginally smaller (3.360 Å versus 3.361 Å) and has a narrower peak width (0.181° versus 0.189° full-width at half maximum (FWHM)) than that of SU-8_3000 (Fig. 3b). The most significant difference between the two samples is in the distribution of grain orientations. By analyzing the angular broadening of reflections in the 2D GIWAXS pattern (Fig. 3e–h and Table S1, ESI†), we can see the presence of the graphene caused the intensity distribution to be spread over a smaller range of angles, with the fitted profiles displaying a smaller FWHM in all observable graphitic planes indicating the grains in SU-8_G_3000 to have an improved preferential orientation. From high resolution TEM images of the cross-section for both samples (Fig. 3i and k), highly aligned (002) lattice fringes are observed, but the FFT image of SU-8_G_3000 with sharper spots suggests it is more ordered than SU-8_3000 which is consistent with the GIWAXS analysis. By heating to 3000 °C, the structural directing effect of graphene was also observed during the graphitization process, and resulted in a higher degree of graphitization.” (Cunning at 798, col. 2 – 799, col. 1) (emphasis added).
“a structural directing effect of CVD-grown single crystal graphene film on the carbonization and graphitization of SU-8 thin films was observed. By embedding single layer graphene sheets in layered SU-8 films and with subsequent heat treatment, we observed improved graphitization, and more significantly, a preferred orientation of the graphite grains when compared to the graphene-free polymer film. Discovery of this structure-directing effect provides a new approach which may lead to high-quality graphite films without the need for stress recrystallization, or may provide a starting material which in combination with stress recrystallization results in a more perfect graphite material.” (Cunning at 799, col. 2) (emphasis added).
All of Cunning is relied upon. One of skill in the art would be motivated to add graphene to the plastic in the plastic graphitization process of Ko, as Cunning teaches it results in a “a more perfect graphite material.” (Cunning at 799, col. 2). The graphene-to-plastic ratio is now claimed in a range: 0.001 to 1.0. Another way of thinking of this is 1000 parts of plastic to 1 part graphene to equal parts graphene and plastic. Cunning does not teach the graphene and plastic in amounts by which a ratio can be calculated. (Cunning at 800, col. 1). However, to the extent Cunning may not inherently teach the claimed ratio, it compares samples graphitized with and without graphene. (Cunning at 797, col. 1 et seq.). The amount of graphene is a result effective variable, optimization of which does not impart patentability. MPEP 2144.05.
Claim 1 further requires “B) heat-treating said graphene/plastic mixture at a first temperature selected from 250°C to 1,500°C for a first period of time to carbonize the graphene/plastic mixture into a graphene/carbon mixture.” Carbonization is taught. (Ko at 450, col. 2 – Experimental).
Claim 1 further requires “C) heat-treating said graphene/carbon mixture, after step (B), at a second temperature, higher than the first temperature, for a second period of time to produce a crystalline graphite, wherein the second temperature is selected from 900°C to 3,500°C. Graphitization at 2400°C is taught. (Ko at 450, col. 2 – Experimental).
As to Claim 2, polyethylene terephthalate is taught. (Ko at 450, col. 2 – Experimental).
As to Claim 4, adding more graphene is an obvious expedient for the reasons noted in connection with the rejection of Claim 1 above related to increased graphitization, etc. The optimization rationale above applies, etc.
As to Claim 8, the temperatures are taught. (Ko at 450, col. 2 – Experimental).
As to Claim 9, “upcycling,” taught by Ko, is interpreted as recycling. (Ko at 450, col. 2 – Experimental).
As to Claim 10, polyethylene terephthalate is taught. (Ko at 450, col. 2 – Experimental).
As to Claim 11, dispersing graphene in the plastic is an obvious expedient to facilitate graphitization. The teachings, suggestions, and motivations addressed in the rejection of Claim 1 are relied upon. Note the folding of graphene into the polymer.
As to Claim 12, the optimization rationale accompanying Claim 1 is relied upon.
As to Claim 14, as discussed above, Cunning teaches “a more perfect graphite material.” (Cunning at 799, col. 2). Perfect graphite would be understood to have the claimed inter-planar spacing. See Id. (“the d-spacing of the (002) peak of SU-8_G_3000 is marginally smaller (3.360 Å versus 3.361 Å)”).
As to Claim 16, two different furnaces are taught. (Ko at 450, col. 2 – Experimental).
As to Claim 17, a continuous manner appears taught. (Ko at 450, col. 2 – Experimental).
As to Claim 18, the inter-plane spacing has been discussed above. Cunning teaches treatment at 3000 C. (Cunning at 798, col. 2). The density is reasonably suggested by virtue of Cunning teaching “more perfect graphite material.” (Cunning at 799, col. 2). Graphite has a density of approx. 2.26 g/cm3. Official notice is taken. Evidence will be supplied if requested.
As to Claim 19, a level of graphitization of 80.6% is taught. (Ko at 453, col. 2).
As to Claim 20, exfoliation is taught. (Ko at 450, col. 2 – Preparation of graphene from PET-derived graphite).
With respect to Claim 21, this claim requires “A) providing a graphene/plastic mixture of multiple plastic particles, having a plastic particle size from 10 nm to 10 cm, and a first amount of multiple sheets of a first graphene material, wherein the first graphene-to-plastic weight ratio is from 0.001 to 1.0” Ko teaches 10 mm x 10 mm PET (plastic) particles. (Ko at 450, col. 2 – Experimental). Ko would not appear to recite any of the various graphene as claimed. Note however that Ko is generally directed to graphitizing plastic. (Ko, entire reference). Cunning teaches adding graphene to polymers prior to carbonization and graphitization. See (Cunning at 797, col. 1 et seq.: “we created thin polymer films with and without continuous layers of single crystal (or near single crystal) graphene embedded within the film to observe the effect graphene has when the polymer is subsequently carbonized and graphitized.”). Cunning provides other relevant teachings. For example, Cunning states:
“Adding crystalline carbon nanomaterials to carbonaceous precursors prior to heat treatment has been shown to influence the structure and texture of the heat-treated carbon adjacent to the crystalline region.” (Cunning at 797, col. 1).
“Thus, after heating to 1000 °C the presence of graphene promotes the ordering of carbon in the vicinity of the graphene.” (Cunning at 797, col. 2).
“The effect of graphene had a minor improvement in the crystallite parameters; from powder XRD measurements, the d-spacing of the (002) peak of SU-8_G_3000 is marginally smaller (3.360 Å versus 3.361 Å) and has a narrower peak width (0.181° versus 0.189° full-width at half maximum (FWHM)) than that of SU-8_3000 (Fig. 3b). The most significant difference between the two samples is in the distribution of grain orientations. By analyzing the angular broadening of reflections in the 2D GIWAXS pattern (Fig. 3e–h and Table S1, ESI†), we can see the presence of the graphene caused the intensity distribution to be spread over a smaller range of angles, with the fitted profiles displaying a smaller FWHM in all observable graphitic planes indicating the grains in SU-8_G_3000 to have an improved preferential orientation. From high resolution TEM images of the cross-section for both samples (Fig. 3i and k), highly aligned (002) lattice fringes are observed, but the FFT image of SU-8_G_3000 with sharper spots suggests it is more ordered than SU-8_3000 which is consistent with the GIWAXS analysis. By heating to 3000 °C, the structural directing effect of graphene was also observed during the graphitization process, and resulted in a higher degree of graphitization.” (Cunning at 798, col. 2 – 799, col. 1) (emphasis added).
“a structural directing effect of CVD-grown single crystal graphene film on the carbonization and graphitization of SU-8 thin films was observed. By embedding single layer graphene sheets in layered SU-8 films and with subsequent heat treatment, we observed improved graphitization, and more significantly, a preferred orientation of the graphite grains when compared to the graphene-free polymer film. Discovery of this structure-directing effect provides a new approach which may lead to high-quality graphite films without the need for stress recrystallization, or may provide a starting material which in combination with stress recrystallization results in a more perfect graphite material.” (Cunning at 799, col. 2) (emphasis added).
All of Cunning is relied upon. One of skill in the art would be motivated to add graphene to the plastic in the plastic graphitization process of Ko, as Cunning teaches it results in a “a more perfect graphite material.” (Cunning at 799, col. 2). The graphene-to-plastic ratio is now claimed in a range: 0.001 to 1.0. Another way of thinking of this is 1000 parts of plastic to 1 part graphene to equal parts graphene and plastic. Cunning does not teach the graphene and plastic in amounts by which a ratio can be calculated. (Cunning at 800, col. 1). However, to the extent Cunning may not inherently teach the claimed ratio, it compares samples graphitized with and without graphene. (Cunning at 797, col. 1 et seq.). The amount of graphene is a result effective variable, optimization of which does not impart patentability. MPEP 2144.05.
Claim 21 further requires “B) heat-treating said graphene/plastic mixture at a first temperature selected from 250"C to 1,500"C for a first period of time to carbonize the graphene/plastic mixture into a 24 graphene/carbon mixture.” Carbonization is taught. (Ko at 450, col. 2 – Experimental).
Claim 21 further requires “C) adding a second amount of multiple sheets of a second graphene material into the graphene/carbon mixture, wherein the second graphene-to-plastic weight ratio, based on the original non-carbonized plastic weight, is from 0.001 to 1.0 and the total graphene-to- plastic weight ratio is no less than 0.001, where the total graphene weight = first graphene weight + second graphene weight, and wherein the first graphene or the second graphene is selected from pristine graphene, having a carbon content greater than 99%, graphene oxide, reduced graphene oxide, halogenated graphene, nitrogenated graphene, hydrogenated graphene, doped graphene, chemically functionalized graphene, or a combination thereof.” For purposes of this rejection, the claim is interpreted as not requiring any graphene, by virtue of the “0” (zero) weight ratio. See discussion above. Ko would not appear to add graphene.
Claim 21 further requires “D) heat-treating said graphene/carbon mixture, after step (B) or step (C), at a second temperature, higher than the first temperature, for a second period of time to produce a crystalline graphite, wherein the second temperature is selected from 900°C to 3,500°C.” Graphitization at 2400°C is taught. (Ko at 450, col. 2 – Experimental).
As to Claim 22, a continuous manner appears taught. (Ko at 450, col. 2 – Experimental).
II. Claim(s) 1, 2, 3, 4, 8, 9, 10, 11, 12, 14, 16, 17, 18, 19, 20, 21, and 22– or as stated below - is/are rejected under 35 U.S.C. 103 as being unpatentable over Ko, et al., Preparation of synthetic graphite from waste PET plastic, Journal of Industrial and Engineering Chemistry 2020; 83: 449-458 (hereinafter “Ko at __”) in view of:
(i) Cunning, et al., Structure-directing effect of single crystal graphene film on polymer carbonization and graphitization, Mater. Horiz. 2019; 6: 796-801 (with Supporting Information, hereinafter “Cunning at ___”), and further in view of:
(ii) Agnoli, et al., Doping graphene with boron: a review of synthesis methods, physiochemical characterization, and emerging applications, J. Mater. Chem. A 2016; 4: 5002-5025 (hereinafter “Agnoli at __”).
The discussion accompanying “Rejection I” above is incorporated by reference.
As to Claim 3, note that Ko teaches adding a boron catalyst to facilitate graphitization. (Ko at 450, col. 2 – Experimental). Boron doped graphene is old, known, and well studied. Official notice is taken. Agnoli is offered as evidence. Substituting the boron of Ko for boron doped graphene reflects substitution of known components for another to achieve predictable results. This does not impart patentability. MPEP 2143; KSR.
III. Claim(s) 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 14, 16, 17, 18, 19, 20, 21, and 22– or as stated below - is/are rejected under 35 U.S.C. 103 as being unpatentable over Ko, et al., Preparation of synthetic graphite from waste PET plastic, Journal of Industrial and Engineering Chemistry 2020; 83: 449-458 (hereinafter “Ko at __”) in view of:
Cunning, et al., Structure-directing effect of single crystal graphene film on polymer carbonization and graphitization, Mater. Horiz. 2019; 6: 796-801 (with Supporting Information, hereinafter “Cunning at ___”), and further in view of:
US 2019/0077668 to Zhamu, et al.
The discussion accompanying “Rejection I” above is incorporated by reference.
As to Claim 5, as noted elsewhere, Ko teaches a boron graphitization catalyst. (Ko at 450, col. 2). To the extent Ko may not teach the claimed catalysts, Zhamu does. (Zhamu 6: [0058]). Use of known components (graphitization catalysts) to achieve predictable results (graphitization) does not impart patentability. MPEP 2143; KSR.
As to Claim 6, to the extent Ko in view of Cunning may not teach adding polynuclear hydrocarbons, Zhamu dues. (Zhamu 2: [0022] et seq.; passim). Combining equivalents known for the same purpose (making graphene/graphite) is an obvious expedient. MPEP 2144.06.
As to Claim 7, the polynuclear hydrocarbons are taught. (Zhamu 3: [0025]).
Allowable Subject Matter
Claims 13 and 15 are objected to as being dependent upon a rejected base claim, but would be allowable if rewritten in independent form including all of the limitations of the base claim and any intervening claims.
Conclusion
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 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.
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/DANIEL C. MCCRACKEN/Primary Examiner, Art Unit 1736