DETAILED ACTION
STATUS OF THE APPLICATION
Receipt is acknowledged of Applicants’ Amendments and Remarks, filed 15 October 2025, in the matter of Application No. 19/194,670. Said documents have been entered on the record. The Examiner further acknowledges the following:
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
Claims 1-20 are pending.
Claims 1 and 10 have been amended.
Thus, claims 1-20 represent all claims currently under consideration.
Information Disclosure Statement (IDS)
The information disclosure statement (IDS) submitted on 25 September 2025 is in compliance with the provisions of 37 CFR 1.97. Accordingly, the IDS is being considered by the Examiner.
Claim Interpretation
The term “chemical vapor deposition” as recited in claim 1 will be interpreted in a manner consistent with its prior art definition as a technique designed for carbon nanomaterial synthesis that is based on the principle of pyrolysis (Devi et al., page 2, Col. 1, paragraph 1; Oxf. Open Mater. Sci. 2021, 1, pages 1-30; PTO-892 of 07-15-2025). Furthermore, this term will be interpreted in a manner consistent with the instant specification (paragraph [0026]) as encompassing several deposition processes, including laser chemical vapor deposition, photo-initiated chemical vapor deposition, metalorganic chemical vapor deposition, hot filament chemical vapor deposition, combustion chemical vapor deposition, atomic-layer chemical vapor deposition, microwave plasma-assisted chemical vapor deposition, plasma-enhanced chemical vapor deposition, remote plasma-enhanced chemical vapor deposition, and the like.
The term “carbonaceous material” as recited in claim 1 will be interpreted in a manner consistent with the instant specification (paragraph [0027]) as substances that can include diamond, doped diamond (e.g., n-type doped diamond, p-type doped diamond, degenerately doped diamond, etc.), graphene, carbon nanotubes, whisker carbon, polymeric carbon, pyrolytic carbon, amorphous carbon, fullerenes, glassy carbon, and/or other suitable carbonaceous materials.
The term “nitrogen species” as recited in claim 1 will be interpreted in a manner consistent with the instant specification (paragraphs [0044] and [0071]) as reactive substances that includes organo-nitrogen compounds, nitrogen oxides, and cyanides but does not include molecular nitrogen.
The term “pre-reforming” as recited in claim 1 will be interpreted in a manner consistent with its prior art definition as a technology used to convert C2-C5 hydrocarbons into methane, hydrogen, water, and carbon oxides at lower temperatures according to the following general equation (Choi et al., page 16, Col. 2, equation 1; page 17, Col. 1, paragraph 3; Chem. Eng. Sci. 2017, 168, 15-22; PTO-892 of 07-15-2025):
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The term “electrified thermal reactor” as recited in claim 2 will be interpreted in a manner consistent with the instant specification (paragraph [0037] as reactors that, for example, generate heat via induction, resistance or Joule heating, and the like).
The term “sorbent” as recited in instant claim 3 will be interpreted in a manner consistent with the instant specification (paragraphs [0007] and [0057]) as a substance that cannot catalyze carbon dioxide conversion but has a high enough affinity so that the carbon dioxide remains proximate to the catalyst, and examples of sorbent materials include alkali metals, alkaline earth metals, alkali metal oxides, alkaline earth metal oxides, amine functionalized materials, metal-organic frameworks (MOFs), activated carbon, zeolites, and/or other suitable sorbents.
The term “sorbent-enhanced” as recited in claim 10 will be, absent any strict definition in the written description, interpreted as a catalyst in combination with any of the sorbent material defined in the instant specification (paragraphs [0007] and [0057]).
The phrase “sorbing contaminants” as recited in claim 15 will be interpreted as in view of the instant specification (paragraphs [0076] and [0083]) as removing carbon contaminants (e.g., carbon oxides, non-methane hydrocarbons, etc.), nitrogen contaminants, inert gases, and/or dopants. Trace contaminants that could be harmful to the catalytic process (e.g., reactive nitrogen species, organosilicon compounds, sulfur oxides, sulfur hydride, nitrogen oxides, etc.) could be removed (e.g., using scrubbers, sorbents, etc.).
Claim 1 recites the method steps “…c) prereforming the saturated non-methane hydrocarbons to carbon oxides and water or decomposing the saturated nitrogen species to the carbon oxides, water, and nitrogen…” and “…e) when nitrogen is produced in step c), producing ammonia from the nitrogen…” The method step e) is being interpreted as a contingent limitation. MPEP § 2111.04(II) states that “The broadest reasonable interpretation of a method (or process) claim having contingent limitations requires only those steps that must be performed and does not include steps that are not required to be performed because the condition(s) precedent are not met.” Therefore, since the claimed method may be practiced without nitrogen being produced in step c), then step e) is not required by the broadest reasonable interpretation of the claim.
REJECTIONS WITHDRAWN
The status for each rejection and/or objection in the previous Office Action is set out below.
Objections to Drawings
Applicant’s corrected drawing sheets filed 15 October 2025 have fully overcome the objections to the drawings.
Claim Objections
Applicant’s amendments to claim 10 have fully overcome this claim objection.
35 U.S.C.§ 112
Applicant’s amendments to claim 1 have fully overcome the rejections over instant claims 1-9.
35 U.S.C.§ 103
The rejections of claims 1-20 are hereby withdrawn in view of Applicant’s amendments to the claims.
Claim Objections
Claim 1 is objected to because of the following informalities:
In line 10, “…to the carbon oxides…” should read “…to carbon oxides…”
Claim 16 is objected to because of the following informalities:
In line 2, “…hydrocarbons, wherein…” should read “…hydrocarbons, and wherein…”
In line 4, “…into the carbon oxides…” should read “…into carbon oxides…”
Claim 19 is objected to because of the following informalities:
In line 2, “…0.0001 %and…” should read “…0.0001% and…”
Appropriate correction is required.
NEW Claim Rejections - 35 USC § 112 – Necessitated by Amendment
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 3 and 19 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 3 recites the phrase “wherein the electrified thermal reactor comprises a bifunctional catalyst comprising a catalyst and a sorbent.” However, claim 1 on which the instant claim depends recites “a set of electrified thermal reactors in fluid connection.” Therefore, it is unclear which electrified thermal reactor of the set of electrified thermal reactors the limitation of claim 3 is referring to, and this ambiguity renders the instant claim indefinite. Further clarification is required. The Examiner notes that amending the claim language to address this ambiguity would ameliorate this claim rejection.
Claim 19 recites “wherein the waste stream comprises about 75% and 99.99% hydrogen by mass, 0.01% and 25% methane by mass, 0.001% and 10% carbon monoxide by mass, and 0.0001% and 10% carbon dioxide by mass; wherein the total percentages add up to 100%.” However, claim 10 on which the instant claim depends requires the presence of acetylene in the waste stream, and this discrepancy renders the instant claim indefinite. Further clarification is required. The Examiner notes that amending the claim language to address this ambiguity would ameliorate this claim rejection.
The following is a quotation of 35 U.S.C. 112(d):
(d) REFERENCE IN DEPENDENT FORMS.—Subject to subsection (e), a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
The following is a quotation of pre-AIA 35 U.S.C. 112, fourth paragraph:
Subject to the following paragraph [i.e., the fifth paragraph of pre-AIA 35 U.S.C. 112], a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
Claims 2 is rejected under 35 U.S.C. 112(d) or pre-AIA 35 U.S.C. 112, 4th paragraph, as being of improper dependent form for failing to further limit the subject matter of the claim upon which it depends, or for failing to include all the limitations of the claim upon which it depends.
Claim 2 recites “The method of Claim 1, wherein steps b) through e) are each performed in an electrified thermal reactor.” However, amended claim 1 on which the instant claim depends recites “…wherein the method is performed as a continuous process by a set of electrified thermal reactors in fluid connection…” Therefore, amended claim 1 appears to suggest that the method steps b) through e), which represent the chemical processes of hydrogenation, prereforming, methanation, and ammonia production, respectively, are each performed by an electrified thermal reactor. Thus, instant claim 2 does not appear to further limit the subject matter of amended claim 1 on which the instant claim depends. Applicant may cancel the claim(s), amend the claim(s) to place the claim(s) in proper dependent form, rewrite the claim(s) in independent form, or present a sufficient showing that the dependent claim(s) complies with the statutory requirements.
NEW Claim Rejections - 35 USC § 103 – Necessitated by Amendment
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 text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
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.
Claims 1-9 are rejected under 35 U.S.C. 103 as being unpatentable over Shearman et al. (US 2021/0348301 A1; PTO-892 of 07-15-2025; hereinafter “Shearman”), in view of Iaccino et al. (US 2015/0267131 A1; PTO-892 of 07-15-2025; hereinafter “Iaccino”), McCune et al. (US 4,919,974; IDS of 09-25-2025; hereinafter “McCune”), W. H. Munro (US 3,694,344; PTO-892 of 07-15-2025; hereinafter “Munro”), A. Rosen (Reactor Design Guide, 2014, pages 1-27; hereinafter “Rosen”), Kokka et al. (Int. J. Hydrogen Energy 2020, 45, 14849-14866; PTO-892 of 07-15-2025; hereinafter “Kokka”), Arroyo-Caire et al. (Nanomaterials 2023, 13, 2914, pages 1-21; PTO-892 of 07-15-2025; hereinafter “Arroyo-Caire”), Fryda et al. (Diam. Relat. Mater. 1994, 3, 1040-1044; hereinafter “Fryda”), and Zheng et al. (ACS Eng. Au 2024, 4, 4-21; published 11-06-2023; PTO-892 of 07-15-2025; hereinafter “Zheng”).
Regarding claim 1, claim 2 depending from claim 1, and claim 4 depending from claim 2, Shearman teaches a system and method for generating synthetic diamonds via atmospheric carbon capture, wherein a gaseous mixture of carbon dioxide and other components found in air from an air source (e.g., outdoor air, air pollution) serves as a low-purity carbon dioxide mixture which is transformed into a high-purity hydrocarbon precursor (i.e., >95% methane) via a methanation process, and diamond crystals are generated from the high-purity carbon precursor within a diamond reactor (e.g., a chemical vapor deposition reactor) to produce ethically-sourced, lab-grown, carbon-negative, jewelry-grade diamonds (Shearman; Title; paragraph [0022]; claim 17). Furthermore, Shearman teaches that the carbon capture device can be configured to collect air samples continuously or semi-continuously (Shearman; paragraphs [0111]-[0112]. Thus, Shearman teaches a process for methanating carbon dioxide (i.e., a carbon oxide) to upcycled methane, and using the upcycled methane for further chemical vapor deposition growth of diamonds (i.e., a carbonaceous material), in a manner consistent with steps d) and f) of instant claim 1.
Shearman fails to teach a method comprising: a) receiving a waste stream from chemical vapor deposition growth of a carbonaceous material, the waste stream comprising hydrogen, methane, carbon oxides, non-methane hydrocarbons, and nitrogen species, wherein the non-methane hydrocarbons comprises between 0.1 ppm and 5000 ppm acetylene; b) hydrogenating the waste stream to reduce unsaturated non-methane hydrocarbons or unsaturated nitrogen species to saturated non-methane hydrocarbons or saturated nitrogen species; c) pre-reforming the saturated non-methane hydrocarbons to carbon oxides and water or decomposing the saturated nitrogen species to the carbon oxides, water, and nitrogen; e) when nitrogen is produced in step c), producing ammonia from the nitrogen; f) using the upcycled methane for further chemical vapor deposition growth of the carbonaceous material; wherein the method is performed as a continuous process by a set of electrified thermal reactors in fluid connection, as recited in instant claim 1; wherein steps b) through e) are each performed in an electrified thermal reactor, as recited in instant claim 2; and wherein a separate electrified thermal reactor is used for each of steps b) through e), as recited in instant claim 4.
Regarding steps a) and b) of instant claim 1, Iaccino teaches a NOx removal method from mixtures comprising molecular hydrogen, methane, and other hydrocarbons produced by hydrocarbon upgrading and conversion processes such as catalytic cracking, pyrolysis, hydroprocessing, reforming, and the like; Iaccino further teaches that gums and/or salts of compounds comprising nitrogen and oxygen (“NOx”) have been observed to react in an uncontrolled manner (e.g., explosively) (Iaccino; Title; paragraphs [0003]-[0004]).
In addition, Iaccino teaches that the first stream can be a mixture (and can referred to as a “first mixture”) obtained from one or more hydrocarbon upgrading and conversion processes such as catalytic cracking, pyrolysis, hydroprocessing, reforming, etc., and that the processes of NOx and upgrading and further processing of the first stream of the process can operate continuously or semi-continuously (Iaccino; paragraphs [0037], [0087], and [0095]; Fig. 3). One of ordinary skill in the art could reasonably deduce that gaseous mixtures produced by pyrolysis can comprise a waste stream from chemical vapor deposition (i.e., a carbon deposition technique based on the principles of pyrolysis; See Claim Interpretation section above). Iaccino further teaches that the first stream of gaseous mixture comprises hydrogen, methane, ethane, butadiene, C3+ saturates, C2+ unsaturates (such as acetylene, ethylene,or propylene), NO, and one or more of water, carbon monoxide, carbon dioxide, sulfur-containing compounds mercury-containing compounds, metals, coke, particulates, or nitrogen oxides of higher order such as NO2 (Iaccino; paragraphs [0039] and [0041]).
Iaccino further teaches an upgraded outlet stream, comprising, e.g., molecular hydrogen, water, methane, ethylene, ethane, carbon monoxide, carbon dioxide, and NOx; in certain embodiments where the outlet stream contains acetylene, one or more acetylene converters can be utilized to convert at least a portion of any acetylene in the upgraded outlet stream to, e.g., ethylene (Iaccino; paragraphs [0084]-[0085], Fig. 3). Thus, Iaccino teaches a first stream that includes all of the components of step a) of instant claim 1, including unsaturated non-methane hydrocarbons and unsaturated nitrogen species, in a manner consistent with step b) of instant claim 1.
Furthermore, Iaccino teaches that the NOx removal step utilizes one or more NOx removal agent, including those capable of reducing NO to N2 and O2 or to a metal oxide (Iaccino; paragraph [0049]); these include redox materials of one or more oxides of Groups 5, 6, 7, 8, 9, and 11 metals of the Periodic Table (Iaccino; paragraph [0061]); in one example, Iaccino teaches the use of a Cu/Al2O3 activated over substantially pure molecular hydrogen that is capable of repeatedly removing substantially all of the feed stream’s NO (Iaccino; Example 3, paragraphs [0107]-[0111]). Finally, Iaccino teaches that selective hydrogenation can be utilized for converting at least a portion of any acetylene, methyl acetylene, propadiene, butadiene, etc. in the upgrade outlet stream to mono-olefins or paraffins. One of ordinary skill in the art would interpret the term “paraffins” in this context as saturated hydrocarbons.
Although Iaccino does not explicitly teach that this waste stream is a chemical vapor deposition waste stream, Iaccino does teach that the gaseous mixtures are obtained by processes including pyrolysis, and chemical vapor deposition is established in the prior art by definition as a technique designed for carbon nanomaterial synthesis that is based on the principle of pyrolysis (c.f., Claim Interpretation section; Devi et al., page 2, Col. 1, paragraph 1; Oxf. Open Mater. Sci. 2021, 1, pages 1-30; PTO-892 of 07-15-2025). Furthermore, the presence of hydrogen, methane, non-methane carbons including acetylene in chemical vapor deposition waste streams is well-established in the prior art as evidenced by McCune, who teaches the preparation of diamond composites by chemical vapor deposition, wherein hot filament chemical vapor deposition (HFCVD) is used to dissociate gas mixtures containing CH4 and H2 at 2000-2800 K, and the dissociation products at these temperatures consist mainly of radicals, for example, CH2, C2H, and CH, acetylene, and atomic hydrogen, as well as unreacted CH4 and H2 (McCune; Title; Abstract; Col. 5, lines 30-44).
Although Iaccino does not explicitly teach wherein the non-methane hydrocarbons comprises between 0.1 ppm and 5000 ppm acetylene, as recited in instant claim 1, Iaccino does teach that in certain aspects, 100 mole of the first stream comprises 0.05 mole to 35.0 mole of ethylene, and optionally, the first stream has an acetylene:ethylene molar ratio of ≤ 1.0 (Iaccino; paragraphs [0040]-[0041]). Therefore, the skilled artisan would recognize that in certain embodiments of the gas stream of Iaccino, for example when the first stream comprises 0.05 mole ethylene per 100 mole of first stream, the first stream may also comprise ≤ 0.05 mole acetylene per 100 mole of first stream, and this mole percent (i.e., ≤ 0.05%) corresponds to ≤ 500 ppm, a range that overlaps with the range recited in the instant claim. MPEP § 2144.05(I) states that “[i]n the case where the claimed ranges ‘overlap or lie inside ranges disclosed by the prior art’ a prima facie case of obviousness exists.” Thus, Iaccino and the supporting teachings of McCune teach every limitation of steps a) and b) and also suggest to the skilled artisan that these process steps can be operated continuously, as recited in instant claim 1.
Regarding steps b), c), d), and e) of instant claim 1, Munro teaches the hydroprocessing of hydrocarbons via a combination process in which a hydrocarbonaceous charge stock is reacted with steam to produce an effluent containing hydrogen and carbon oxides (as in step c) of instant claim 1), the effluent is compressed at which pressure the hydrogen concentration is increased through the removal of oxides of carbon (as in step d) of instant claim 1), and the purified hydrogen stream is then compressed to a higher pressure level and introduced into the hydroprocessing reaction zone (as in step b) of instant claim 1) (Munro; Title; Abstract). The term “hydroprocessing” is intended to be synonymous with the term “hydrogenation,” and processes intended to be encompassed by the term “hydroprocessing” include hydrocracking, aromatic hydrogenation, ring-opening, hydrorefining (for nitrogen removal and olefin saturation), desulfurization, hydrogenation, etc. (Munro; Col. 1, lines 42-45 and 48-52).
In addition, Munro teaches that as currently practiced, hydrogen production in the manner of the invention involves the major processing steps of steam reforming, water-gas shift reaction and the removal of acid gases; it is known that various hydrocarbonaceous materials may be employed as feed streams to the steam reforming reaction zone (Munro; Col. 4, lines 14-18). It is generally acknowledged that the ideal feed stream is rich in low molecular weight, normally gaseous paraffins including methane, ethane, propane, with natural gases of relatively low nitrogen content being distinctly preferred (Munro; Col. 4, lines 18-23). Munro further teaches that the feedstocks which may be satisfactorily converted in the present invention have a wide range of compositions, and may contain large concentrations of saturates and aromatic hydrocarbons (Munro; Col. 6, lines 60-63). The skilled artisan would readily ascertain that aromatic hydrocarbons are unsaturated non-methane hydrocarbons, as recited in step b) of instant claim 1.
Of particular note, Munro teaches that at least a portion of the separated light hydrocarbons, including normally gaseous hydrocarbons (i.e., methane, ethane, propane) obtained from the hydroprocessing step may be introduced as part of the feed mixture to the steam reforming zone for the production of hydrogen, and the remaining impurities, such as carbon monoxide, are converted into a more desirable hydrocarbon by reaction with hydrogen; typically, a methanator is employed to convert residual carbon monoxide and carbon dioxide to methane (Munro; Col. 4, lines 39-41; Col. 6, lines 27-30; Col. 10, lines 69-71). This sequence of hydrogenation [Wingdings font/0xE0] steam reforming (i.e., pre-reforming) [Wingdings font/0xE0] methanation is depicted in the Figure taught by Munro, wherein the reactor 22 (as in step b) of instant claim 1) can cycle light hydrocarbons produced in the hydroprocessing step to the steam reformer 6 (as in step c) of instant claim 1) via line 2, and the hydrogen produced in the reformer can be transported to methanator 19 via line 18 for the removal of carbon oxides (as in step d) of instant claim 1). Thus, the skilled artisan would readily ascertain that the combination process of Munro teaches a process consistent with steps b) [Wingdings font/0xE0] c) [Wingdings font/0xE0] d) of instant claim 1.
Furthermore, the process of Munro defines the feed in units of liquid hourly space velocity (Munro; claim 5, Col. 6, lines 7-8 and 41-42; Col. 9, line 7), a unit specifically used for continuous processes, as further evidenced by Rosen (Rosen; page 7, section 2.5: Space Time and Space Velocity); thus, the skilled artisan would recognize from the teachings of Munro (Figure; claim 5, Col. 6, lines 7-8 and 41-42; Col. 9, line 7) and the supporting teachings of Rosen that the process of Munro is performed in a continuous manner via a set of reactors in fluid connection, in a manner consistent with instant claim 1 (Munro; Figure).
Finally, Munro teaches that as an alternative to the methanation step, a nitrogen washing column may be employed to remove methane and carbon monoxide, thereby producing a gas suitable for the synthesis of ammonia (Munro; Col. 4, lines 48-50). The skilled artisan could reasonably ascertain based on the teachings of Munro alone that this ammonia synthesis step would, as in steps b)-d), occur in a separate reactor, especially since Munro teaches a nitrogen separation step after steam reformation and prior to methanation. Thus, the teachings of Munro further suggest to the skilled artisan that this continuous combination process can further be coupled to producing ammonia from the nitrogen involved in the process, (i.e., steps b) [Wingdings font/0xE0] e) of instant claim 1, such that these method steps could be performed in a continuous fashion and in separate continuous reactors, in a manner consistent with instant claims 1-2 and 4.
Regarding steps c) and d) of instant claim 1, Kokka teaches hydrogen production via steam reforming of propane over supported metal catalysts (Kokka; Title). Kokka further teaches that the utilization of alternative energy sources has become attractive during the last decades as a result of depletion of fossil fuel reserves and the environmental concerns induced by their use, such as air pollution and major climate changes, and the reaction of steam reforming of light alkanes (methane, propane, butane) has been proposed as a promising process for the production of high H2 yields at high temperatures:
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and depending on the reaction conditions and catalyst employed, steam reforming may run in parallel with the Water-Gas Shift (WGS) reaction, producing CO2 and improving H2 yield:
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and in addition to H2 and carbon oxides (CO and CO2), propane can be converted to methane (CH4) via the reactions of CO or CO2 methanation and decomposition of C3H8 (Kokka; page 14850, Col. 1, paragraphs 1-4 and equations 1-6):
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Thus, in a manner consistent with step c) of instant claim 1, the teachings of Kokka demonstrate that the pre-reforming of a saturated non-methane hydrocarbon (i.e., propane) is an effective way to generate H2 as an alternative energy source, and this process also generates carbon oxides (i.e., CO and CO2), H2O, and CH4 via reaction equilibria (i.e., equations 1-6 above) that are dictated by the particular reaction conditions (e.g., temperature, catalyst employed). Furthermore, the skilled artisan would realize from the teachings of Kokka that this process can be utilize for the effective production of methane via carbon oxide methanation, and is therefore intrinsically coupled to step d) of instant claim 1.
Regarding step e) of instant claim 1, Arroyo-Caire reviews the design of new catalysts for ammonia synthesis and teaches that there is a growing interest in green ammonia production that has spurred the development of new catalysts with the potential to carry out the Haber-Bosch process under mild pressure and conditions (Arroyo-Caire; Title; Abstract). Arroyo-Caire further teaches that the hydrogen used for ammonia synthesis is mainly obtained from non-renewable sources (e.g., natural gas reforming):
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and this process is normally carried out in large central facilities which contain two large industrial plants in one (a steam methane reforming plant and an ammonia synthesis plant) (Arroyo-Caire; page 1, paragraphs 1-2 and equation 1). Thus, the teachings of Arroyo-Caire would inform the skilled artisan that the production of ammonia from nitrogen (i.e., the Haber-Bosch process), as recited in step e) of instant claim 1, is well-established in the art and is in practice normally coupled with hydrocarbon reforming processes, for example as recited in step c) of instant claim 1 (i.e., steps c) [Wingdings font/0xE0] e) of instant claim 1 are known to be coupled industrial processes).
Regarding the recycling of chemical vapor deposition waste gases (as in step f) [Wingdings font/0xE0] a) of instant claim 1), Fryda teaches a method of diamond CVD with a closed gas circuit which is able to remove undesired products of the CVD process and replenish the necessary gaseous components, particularly methane and carbon monoxide (Fryda; Title; Abstract). Fryda further teaches that the gas costs, particularly for hydrogen, are significant in industrial diamond deposition processes, and a recirculation of the exhaust gas, combined with some kind of purification and reprocessing, is therefore expected to become important for industrial deposition of CVD diamond (Fryda; page 1040, Col. 1, paragraph 1). In addition, Fryda teaches a gas composition in equilibrium with graphite at temperatures between 800 and 1000 ºC and pressures between 1 and 1000 mbar suggests that an equilibration of any C,H,O-containing gas with solid carbon under appropriate conditions should yield a gas phase well suited to the growth of diamond in any of the CVD processes currently used; under the conditions quoted, methane is the dominant species in equilibrium, while the concentrations of acetylene and other species are orders of magnitude smaller (Fryda; page 1040, Col. 2, paragraph 2 and page 1041, Col. 1, paragraph 1). Furthermore, Fryda teaches the use of various feed gas compositions, including 1% ethyne in hydrogen, pure hydrogen, 5% methane in hydrogen, hydrogen containing 10% carbon monoxide; in a process run to generate a diamond film performed in a HFCVD reactor using a conventional gas supply (0.5% methane in hydrogen), the process gas was completely recovered after deposition, and therefore film growth took place without consumption of hydrogen (Fryda; page 1041, Col. 2, paragraph 2; page 1042, Col. 2, paragraph 3, Table 1; page 1043, Col. 1, paragraph 1 and Col. 2, paragraph 1; page 1044, Col. 1, paragraph 1). To replenish the carbon source of the exhaust gas prior to its reuse during the CVD process, Fryda teaches that the exhaust gas can be reprocessed through a carbon reactor to replenish the methane concentration (Fryda; page 1041, Fig. 3; page 1042, Fig. 5). In summary, Fryda teaches the feasibility of a closed gas circuit for diamond CVD, based on a chemical reprocessing of the exhaust gas from any CVD reactor (Fryda; page 1044, Col. 1, paragraph 2). Overall, Fryda demonstrates that CVD exhaust gases comprising hydrogen, methane, and small amounts of acetylene and other species can be effectively recycled and are amenable to chemical reprocessing, including the production of methane for further use in CVD processes, in a manner consistent with steps f) [Wingdings font/0xE0] a) of instant claim 1.
Finally, regarding the claim limitations wherein the method is performed by a set of electrified thermal reactors and wherein steps b) through e) are each performed in an electrified thermal reactor, as recited in instant claims 1-2; and wherein a separate electrified thermal reactor is used for each of steps b) through 3), as recited in instant claim 4, Zheng teaches Joule-heated catalytic reactors toward decarbonization and process intensification, wherein Zheng assesses that Joule heating (also known as resistive or ohmic heating) can be regarded as the most promising method for process electrification, and its application to methane reforming, cracking reactions, CO2 valorization, and transient process operation are reviewed (Zheng; Title; Abstract; page 6, Col. 2, Section 2.1. Joule Heating Fundamentals). Of particular note, Zheng summarizes recent developments and advantages for direct Joule heating in fast heating applications, including methane pyrolysis (avoids coke formation), ammonia synthesis (avoids catalyst sintering), methane steam reforming (fast start-up and shutdown to address the intermittent nature of renewable energy), and CO2 methanation (to address the intermittent nature of renewable energy); since fast heating with joule-heated reactors can be driven by renewable energy, the direct electrification of catalytic processes through the Joule effect not only eliminates CO2 emissions from fuel combustion but also provides the required heat for highly endothermic processes such as methane steam reforming (Zheng; page 14, Table 5, entries 1-2, 4, and 6; Col. 2, paragraph 3). In addition, Zheng teaches that among the three electrification approaches studied (i.e., Joule or resistance heating, induction, and microwave heating), resistance heating represents the most promising method for industrialization because its approach is more straightforward compared to the other two methods in terms of materials, reactor design, and temperature flexibility; moreover the existing knowledge and experience from the direct heating of furnaces can be transferred directly to the development of Joule heated catalytic reactors (Zheng; Abstract; page 16, Col. 1, paragraph 2).
The prior art as taught by Shearman, Iaccino, McCune, Munro, Kokka, Arroya-Caire, Fryda, and Zheng reside in the overlapping technical areas of methane and hydrogen utilization via interrelated chemical processes that are generally well-established in industrial practice, and Shearman, McCune, and Fryda explicitly teach diamond CVD processes, and are therefore deemed analogous art, as described in MPEP § 2141.01(a).
The method of Shearman is related to the chemical vapor deposition of carbonaceous materials and involves CO2 methanation, a chemical process that overlaps with saturated hydrocarbon pre-reforming, as taught by Kokka with waste streams that also include pyrolytic processes (such as chemical vapor deposition), and the hydrogen gas produced through the method of Kokka is known to be coupled to the Haber-Bosch process for producing ammonia from the reduction of nitrogen, as taught by Arroyo-Caire. Furthermore, Iaccino teaches the removal of nitrogen species (i.e., NOx) via hydrogenation from waste gas streams, and Iaccino in view of the supporting teaching of McCune inform the skilled artisan that pyrolysis and CVD exhaust gases would comprise hydrogen, methane, carbon oxides, non-methane hydrocarbons, nitrogen species and acetylene. Munro teaches a combination process involving the hydrogenation of feedstocks that include unsaturated non-methane hydrocarbons that is also useful for denitrification, and the light components of the hydrogenation process are cycled through a steam reformer and methanator to obtain hydrogen gas of high purity; Munro further teaches the possibility of coupling the steam reformer with a nitrogen washing column to produce a gas suitable for ammonia synthesis, and Munro in view of the supporting teachings of Rosen indicate that the process of Munro comprises continuous reactors in fluid connection. In addition, the teachings of Fryda demonstrate that CVD waste gases can be effectively recycled and are amenable to chemical reprocessing, including for the production of methane for further use in CVD processes. Finally, Zheng teaches direct application of Joule heated reactors to methane pyrolysis (as is known in the art to be involved with chemical vapor deposition, consistent with steps a) and f) of the method of claim 1), ammonia synthesis (consistent with step e) of the method of claim 1), methane steam reforming (consistent with step c) of the method of claim 1), and CO2 methanation (consistent with step d) of the method of claim 1). Thus, the skilled artisan would be sufficiently motivated to implement the teachings of Zheng to realize the benefits of Joule heated (i.e., electrified) thermal reactors.
Overall, one of ordinary skill would be sufficiently motivated to incorporate the teachings of Iaccino, McCune, Munro, Rosen, Kokka, Arroya-Caire, Fryda, and Zheng into the method of Shearman to arrive at the process of the claimed invention with a reasonable expectation of success. Such an endeavor would result in combining prior art elements according to known methods to yield predictable results, as described in MPEP § 2143(I)(A). Therefore, 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 have modified Shearman to incorporate the teachings of Iaccino, McCune, Munro, Rosen, Kokka, Arroya-Caire, Fryda, and Zheng to develop the claimed process. The motivation to do so would permit the skilled artisan to pursue, with a reasonable expectation of success, an improved CVD method that minimizes waste and energy consumption in the precursor supply chain, recycles CVD exhaust gas, and utilizes reactors that can be driven by renewable energy, that eliminate CO2 emissions from fuel combustion, provide the required heat for highly endothermic processes such as methane steam reforming, and is more friendly towards industrialization by virtue of its more straightforward approach in terms of materials, reactor design, temperature flexibility, and the ability to transfer existing knowledge from the direct heating of furnaces, as described above.
Regarding claim 3 depending from claim 2, Munro teaches a combination process that comprises steps b) [Wingdings font/0xE0] c) [Wingdings font/0xE0] d) of the method of claim 1, as detailed above, wherein suitable catalytic composites comprise at least one metallic component of Groups VI-B and VIII of the Periodic Table combined with a suitable refractory inorganic oxide such as alumina, silica, and mixtures thereof; a preferred carrier material constitutes faujasite, a form of crystalline aluminosilicate, which carrier material is at least about 90.0% by weight zeolitic (Munro; Col. 7, lines 23-27 and lines 52-55) and which qualifies as the claimed sorbent. In addition, Arroyo-Caire teaches K-Fe/Al2O3-CaO and (Ba-Cs)-Ru/MgO catalyst examples for ammonia synthesis, as in step e) of the method of claim 1 (Arroyo-Caire; page 15; Table 1). These catalyst compositions comprising an alkaline earth metal sorbent (i.e., CaO and MgO) read directly on the bifunctional catalyst limitation of the instant claim. Therefore, as with claim 2, it would have been prima facie obvious to combine Shearman, Iaccino, McCune, Munro, Rosen, Kokka, Arroya-Caire, Fryda, and Zheng to arrive at the claimed invention.
Regarding claims 5 and 8 depending from claim 4 and claim 6 depending from claim 5, Munro teaches a combination process that comprises steps b) [Wingdings font/0xE0] c) [Wingdings font/0xE0] d) of the method of claim 1, as detailed above, wherein suitable catalytic composites comprise at least one metallic component of Groups VI-B and VIII of the Periodic Table combined with a suitable refractory inorganic oxide such as alumina, silica, and mixtures thereof (Munro; Col. 7, lines 23-27). Of particular note, Munro teaches that a preferred catalytic composite comprises nickel in an amount of 0.5% to about 10.0% by weight, composited with an alumina-silica carrier material, thus reading directly on instant claims 5 and 8 (Munro; Col. 7, lines 49-52). In addition, Munro teaches that the Group VI-B metal, such as chromium, molybdenum, or tungsten, is usually present in an amount of from about 0.5% to about 10.0% by weight (Munro; Col. 7, lines 38-40). Based on these teachings, the skilled artisan could readily arrive at a catalyst comprising Ni/Mo on a alumina-silica support, in a manner consistent with instant claim 6.
Regarding claim 7 depending from claim 4, Kokka teaches hydrogen production via steam reforming, in a manner consistent with step c) of the instantly claimed invention, as detailed above, wherein Rh/SiO2, Rh/TiO2, Rh/CeO2, and Rh/Al2O3 are disclosed (Kokka; page 14853; Table 1).
Regarding claim 9 depending from claim 4, Arroyo-Caire reviews the design of new catalysts for ammonia synthesis, as detailed above, wherein Arroyo-Caire teaches that a sole Ru over carbon catalyst commonly exhibits poor ammonia synthesis activity and ruthenium-based materials are thus commonly promoted by the addition of some extra compounds: alkali and alkaline earth metal promoters have been demonstrated to be very effective at achieving high activities towards ammonia production; among them, cesium and barium are the most widely used (Arroyo-Caire; page 4, paragraph 1). Of particular note, Arroyo-Caire teaches that the addition of different amounts of cesium to a ruthenium over ceria (Ru/CeO2) catalyst, as well as the impact of the synthesis route, were recently explored; it was concluded that both the concentration of the cesium promoter and the procedure followed for the preparation of the catalyst could influence the performance of the material for the ammonia synthesis reaction, and from these results it was observed that optimal behavior in terms of ammonia production and Turnover Frequencies (TOF) was obtained by adding the cesium to the support before ruthenium impregnation, with an optimal load of Ru of 2% wt. and a Cs/Ce ratio of 0.35 (Arroyo-Caire; page 4, paragraph 1).
Claims 10-16 and 18-20 are rejected under 35 U.S.C. 103 as being unpatentable over Shearman et al. (US 2021/0348301 A1; PTO-892 of 07-15-2025; hereinafter “Shearman”), in view of Iaccino et al. (US 2015/0267131 A1; PTO-892 of 07-15-2025; hereinafter “Iaccino”), McCune et al. (US 4,919,974; IDS of 09-25-2025; hereinafter “McCune”), Jeong-Potter et al. (US 2024/0115987 A1; IDS of 06-03-2025; published 04-11-2024; hereinafter “Jeong-Potter”), and Fryda et al. (Diam. Relat. Mater. 1994, 3, 1040-1044; hereinafter “Fryda”).
Regarding claim 10, Shearman teaches a system and method for generating synthetic diamonds via atmospheric carbon capture, wherein a gaseous mixture of carbon dioxide and other components found in air from an air source (e.g., outdoor air, air pollution) serves as a low-purity carbon dioxide mixture which is transformed into a high-purity hydrocarbon precursor (i.e., >95% methane) via a methanation process, and diamond crystals are generated from the high-purity carbon precursor within a diamond reactor (e.g., a chemical vapor deposition reactor) to produce ethically-sourced, lab-grown, carbon-negative, jewelry-grade diamonds (Shearman; Title; paragraph [0022]; claim 17). Thus, Shearman teaches a process for methanating carbon dioxide (i.e., a carbon oxide) to upcycled methane, and using the upcycled methane for further chemical vapor deposition growth of diamonds (i.e., a carbonaceous material), in a manner consistent with instant claim 10.
Shearman fails to teach the claim limitation of receiving a waste stream from chemical vapor deposition growth of a carbonaceous material, the waste stream comprising hydrogen, methane, acetylene, and carbon oxide. In addition, although Shearman does teach converting of carbon oxide into upcycled methane from a waste stream, Shearman fails to teach the claim limitation of treating the waste stream using a thermal reactor comprising sorbent-enhanced catalysts.
Regarding the claim limitation of receiving a waste stream from chemical vapor deposition growth of a carbonaceous material, the waste stream comprising hydrogen, methane, acetylene, and carbon oxide, Iaccino teaches a NOx removal method from mixtures comprising molecular hydrogen, methane, and other hydrocarbons produced by hydrocarbon upgrading and conversion processes such as catalytic cracking, pyrolysis, hydroprocessing, reforming, and the like; Iaccino further teaches that gums and/or salts of compounds comprising nitrogen and oxygen (“NOx”) have been observed to react in an uncontrolled manner (e.g., explosively) (Iaccino; Title; paragraphs [0003]-[0004]). In addition, teaches that the first stream can be a mixture (and can referred to as a “first mixture”) obtained from one or more hydrocarbon upgrading and conversion processes such as catalytic cracking, pyrolysis, hydroprocessing, reforming, etc., and that the processes of NOx and upgrading and further processing of the first stream of the process can operate continuously or semi-continuously (Iaccino; paragraphs [0037], [0087], and [0095]; Fig. 3). One of ordinary skill in the art could reasonably deduce that gaseous mixtures produced by pyrolysis can comprise a waste stream from chemical vapor deposition (i.e., a carbon deposition technique based on the principles of pyrolysis; See Claim Interpretation section above).
Iaccino further teaches that the first stream of gaseous mixture comprises hydrogen, methane, ethane, butadiene, C3+ saturates, C2+ unsaturates (such as acetylene, ethylene,or propylene), NO, and one or more of water, carbon monoxide, carbon dioxide, sulfur-containing compounds mercury-containing compounds, metals, coke, particulates, or nitrogen oxides of higher order such as NO2 (Iaccino; paragraphs [0039] and [0041]); in one embodiment, Iaccino teaches an upgraded outlet stream, comprising, e.g., molecular hydrogen, water, methane, ethylene, ethane, carbon monoxide, carbon dioxide, and NOx; in certain embodiments where the outlet stream contains acetylene, one or more acetylene converters can be utilized to convert at least a portion of any acetylene in the upgraded outlet stream to, e.g., ethylene (Iaccino; paragraphs [0084]-[0085], Fig. 3). Thus, Iaccino teaches a first stream that includes all of the components of instant claim 10. .
Although Iaccino does not explicitly teach that this waste stream is a chemical vapor deposition waste stream, Iaccino does teach that the gaseous mixtures are obtained by processes including pyrolysis, and chemical vapor deposition is established in the prior art by definition as a technique designed for carbon nanomaterial synthesis that is based on the principle of pyrolysis (c.f., Claim Interpretation section; Devi et al., page 2, Col. 1, paragraph 1; Oxf. Open Mater. Sci. 2021, 1, pages 1-30; PTO-892 of 07-15-2025). Furthermore, the presence of hydrogen, methane, non-methane carbons including acetylene in chemical vapor deposition waste streams is well-established in the prior art as evidenced by McCune, who teaches the preparation of diamond composites by chemical vapor deposition, wherein hot filament chemical vapor deposition (HFCVD) is used to dissociate gas mixtures containing CH4 and H2 at 2000-2800 K, and the dissociation products at these temperatures consist mainly of radicals, for example, CH2, C2H, and CH, acetylene, and atomic hydrogen, as well as unreacted CH4 and H2 (McCune; Title; Abstract; Col. 5, lines 30-44).
Regarding the claim limitation of treating the waste stream using a thermal reactor comprising sorbent-enhanced catalysts, Jeong-Potter teaches a dual functional material that captures carbon dioxide from ambient air, i.e., direct air capture, and converts the CO2 to a desired product such as methane; the material includes a high surface area carrier such as Al2O3 upon which catalysts and alkaline adsorbents are positioned proximate each other; the materials can be employed in isothermal, cyclic reactor systems where target species are bound and then desorbed to reactivate the material, e.g., bind more target species for desorption and/or conversion to additional product (Jeong-Potter; Abstract; claim 1). Jeong-Potter further teaches that the reaction system 300 includes a heat source 310 for controlling the temperature of the interior of reactor 302, dual functional material (DFM) 304, or combinations thereof (Jeong-Potter; paragraph [0052] and Fig. 3). Thus, Jeong-Potter teaches treating the waste stream using a thermal reactor comprising sorbent-enhanced catalysts, in a manner consistent with instant claim 10.
Finally, regarding receiving a waste stream from chemical vapor deposition growth of a carbonaceous material, Fryda teaches a method of diamond CVD with a closed gas circuit which is able to remove undesired products of the CVD process and replenish the necessary gaseous components, particularly methane and carbon monoxide (Fryda; Title; Abstract). Fryda further teaches that the gas costs, particularly for hydrogen, are significant in industrial diamond deposition processes, and a recirculation of the exhaust gas, combined with some kind of purification and reprocessing, is therefore expected to become important for industrial deposition of CVD diamond (Fryda; page 1040, Col. 1, paragraph 1). In addition, Fryda teaches a gas composition in equilibrium with graphite at temperatures between 800 and 1000 ºC and pressures between 1 and 1000 mbar suggests that an equilibration of any C,H,O-containing gas with solid carbon under appropriate conditions should yield a gas phase well suited to the growth of diamond in any of the CVD processes currently used; under the conditions quoted, methane is the dominant species in equilibrium, while the concentrations of acetylene and other species are orders of magnitude smaller (Fryda; page 1040, Col. 2, paragraph 2 and page 1041, Col. 1, paragraph 1). Furthermore, Fryda teaches the use of various feed gas compositions, including 1% ethyne in hydrogen, pure hydrogen, 5% methane in hydrogen, hydrogen containing 10% carbon monoxide; in a process run to generate a diamond film performed in a HFCVD reactor using a conventional gas supply (0.5% methane in hydrogen), the process gas was completely recovered after deposition, and therefore film growth took place without consumption of hydrogen (Fryda; page 1041, Col. 2, paragraph 2; page 1042, Col. 2, paragraph 3, Table 1; page 1043, Col. 1, paragraph 1 and Col. 2, paragraph 1; page 1044, Col. 1, paragraph 1). To replenish the carbon source of the exhaust gas prior to its reuse during the CVD process, Fryda teaches that the exhaust gas can be reprocessed through a carbon reactor to replenish the methane concentration (Fryda; page 1041, Fig. 3; page 1042, Fig. 5). In summary, Fryda teaches the feasibility of a closed gas circuit for diamond CVD, based on a chemical reprocessing of the exhaust gas from any CVD reactor (Fryda; page 1044, Col. 1, paragraph 2). Overall, Fryda demonstrates that CVD exhaust gases comprising hydrogen, methane, and small amounts of acetylene and other species can be effectively recycled and are amenable to chemical reprocessing, including the production of methane for further use in CVD processes, in a manner consistent with instant claim 10.
The prior art as taught by Shearman, Iaccino, McCune, Jeong-Potter, and Fryda reside in the overlapping technical areas of methane and hydrogen utilization via interrelated chemical processes that are generally well-established in industrial practice, and Shearman, McCune, Jeong-Potter, and Fryda teach CVD diamond processes and are therefore deemed analogous art, as described in MPEP § 2141.01(a). The method of Shearman is related to the chemical vapor deposition of carbonaceous materials and involves CO2 methanation, and the composition of methane pyrolysis (e.g., as in a chemical vapor deposition process) waste streams is taught by Iaccino in view of the supporting teachings of McCune. Furthermore, Jeong-Potter also teaches an air capture/CO2 methanation process analogous to the method of Shearman, with the added features of treating the waste stream using a thermal reactor comprising sorbent-enhanced catalysts. Finally, the teachings of Fryda demonstrate that CVD waste gases can be effectively recycled and are amenable to chemical reprocessing, including for the production of methane for further use in CVD processes. Thus, one of ordinary skill would be sufficiently motivated to incorporate the teachings of Iaccino, McCune, Jeong-Potter, and Fryda into the method of Shearman to arrive at the process of the claimed invention with a reasonable expectation of success. Such an endeavor would result in combining prior art elements according to known methods to yield predictable results, as described in MPEP § 2143(I)(A).
Therefore, 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 have modified Shearman to incorporate the teachings of Iaccino, McCune, Jeong-Potter, and Fryda to develop a method comprising: receiving a waste stream from chemical vapor deposition growth of a carbonaceous material, the waste stream comprising hydrogen, methane, acetylene, and carbon oxide; treating the waste stream using a thermal reactor comprising sorbent-enhanced catalysts to convert the carbon oxide into upcycled methane; wherein the upcycled methane is used for further chemical vapor deposition growth of the carbonaceous material. The motivation to do so permit the skilled artisan to pursue, with a reasonable expectation of success, an improved CVD method that minimizes waste and energy consumption by recycling CVD exhaust gas, as described above.
Regarding claim 11 depending on claim 10, Jeong-Potter teaches that the reactor for CO2 methanation can be heated to 300-350 ºC (Jeong-Potter; paragraph [0007]). This temperature range overlaps with the range recited in the instant claim. MPEP § 2144.05(I) states that “[i]n the case where the claimed ranges ‘overlap or lie inside ranges disclosed by the prior art’ a prima facie case of obviousness exists.”
Regarding claim 12 depending from claim 11, Jeong-Potter teaches a reaction example wherein the following steps were taken for subsequent adsorption/methanation cycles: CO2 capture step at 25 °C with simulated ambient air (400 ppm CO2/air) overnight to ensure saturation of material; heat to 300 °C in 30 minutes (9-10 °C./min) in 15% H2/N2; hold at 300° C for 2 hours in 15% H2/N2. All steps were performed at 1 atm with a total flow rate of 100 ml/min (GHSV: 12 L(STP)/h/g, 6950 h−1) (Jeong-Potter; paragraph [0072]). Although Jeong-Potter does not explicitly teach that the thermal reactor is operated intermittently to prevent a temperature from exceeding about 300 °C as recited in the instant claim, one of ordinary skill would ascertain from the teachings of Jeong-Potter alone that the reactor is expected to remain at 300 °C and that the flow rate and inert gas composition (85% N2) could reasonably absorb excess heat generated by the CO2 methanation process, such that intermittent operation of the thermal reactor is not necessary to maintain a reaction temperature that does not exceed 300 °C. Furthermore, if the skilled artisan is unable to effectively prevent a temperature from exceeding about 300 °C based on the method of Jeong-Potter alone, the skilled artisan could reasonably arrive at a method that employs intermittent operation as a consequence of routine experimentation. MPEP § 2144.05(II) states that “[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.”
Regarding claims 13 and 15 depending from claim 10, Shearman teaches that the hydrocarbon precursor can be passed through a set of filters (e.g., a filter membrane) at an outlet of the methanation reactor; the set of filters can be configured to collect impurities-such as compounds containing nitrogen (e.g., nitric oxide, nitrogen dioxide), hydrogen, carbon dioxide, argon, or other gases (e.g., other than methane)-present in the hydrocarbon mixture (Shearman; paragraph [0057]). In the context of hydrogen separation, one of ordinary skill would realize from the teachings of Sherman alone that the use of a filter membrane to separate hydrogen from methane intrinsically teaches a hydrogen selective membrane, in a manner consistent with instant claim 13, wherein the filter membranes taught by Shearman would be expected to sorb the desired gaseous contaminants from the upcycled methane gaseous mixture. Therefore, as with claim 10, it would have been prima facie obvious to combine Shearman, Iaccino, McCune, Jeong-Potter, and Fryda to arrive at the claimed invention.
Regarding claim 14 depending from claim 10, Shearman teaches that a stream of inert gas (e.g., argon) is cycled through the methanation reactor to purge the methanation reactor of impurities; for example, a stream of argon can be cycled through the methanation reaction prior to introduction of the high-purity gaseous carbon dioxide mixture into the methanation reactor; further, in the example, the stream of argon can be cycled through the methanation reactor both during methanation of the high-purity carbon dioxide mixture (e.g., while the high-purity gaseous carbon dioxide is present in the methanation reactor) and after the high-purity gaseous carbon dioxide mixture exits the methanation reactor to purge impurities from within the methanation reactor and to maintain an operational pressure within the methanation reactor (Shearman; paragraph [0049]). Furthermore, Shearman teaches that the hydrocarbon precursor can be purified in the buffer vessel, such that the hydrocarbon precursor can be recovered. For example, the hydrocarbon precursor (i.e., methane) can be transferred from an outlet of the methanation reactor into the accumulator. The accumulator can include an inline nitrogen reader configured to estimate a concentration of nitrogen present in the hydrocarbon precursor. Then, in response to the concentration of nitrogen exceeding a threshold concentration (e.g., greater than 400 parts-per-million, greater than 10 parts-per-million, greater than 1.2 parts-per-billion), the hydrocarbon precursor can be diverted (e.g., via a purge line) into a buffer vessel. In this example, the hydrocarbon precursor can be conveyed through a secondary separation unit (e.g., a set of filters) configured to remove nitrogen from the hydrocarbon precursor (Shearman; paragraph [0053]). Thus, the method of Shearman comprises purging of upcycled methane to remove inert contaminants (i.e., nitrogen), in a manner consistent with the instant claim and as with claim 10, it would have been prima facie obvious to combine Shearman, Iaccino, McCune, Jeong-Potter, and Fryda to arrive at the claimed invention.
Regarding claim 16 depending from claim 10, Iaccino teaches a methane pyrolysis (i.e., as for example in chemical vapor deposition) waste stream that comprises hydrogen, methane, ethylene, ethane, propylene, butadiene, C3+ saturates, NO, and one or more of water, carbon monoxide, carbon dioxide, sulfur-containing compounds mercury-containing compounds, metals, coke, particulates, or nitrogen oxides of higher order such as NO2 (Iaccino; paragraph [0041]). The skilled artisan would recognize that ethylene, ethane, propylene, butadiene, and C3+ saturates represent non-methane hydrocarbons, in a manner consistent with the instant claim. In addition, Jeong-Potter teaches that in some embodiments, the reactive gas includes hydrogen, a hydrocarbyl compound, e.g., C2H4, or combinations thereof (Jeong-Potter; paragraph [0051]). Furthermore, both Shearman and Jeong-Potter teach the methanation of carbon dioxide, as detailed above (Shearman; Title; paragraph [0022]; claim 17; Jeong-Potter; Abstract; claim 1).
Regarding claim 18 depending from claim 16, Jeong-Potter teaches that in some embodiments, the reaction system 300 includes a plurality of reactors 302 connected in series, connected in parallel, or combinations thereof (Jeong-Potter; paragraph [0050]; Fig. 3). Furthermore, Jeong-Potter teaches that in some embodiments of system 300 that include a plurality of reactors 302, continuous adsorption and desorption of target species and thus generation of desired product is enabled as first stream 306 can be fed to a first reactor (resulting in adsorption of target species in that reactor) while second stream 308/third stream 309/vacuum is applied to a second reactor (simultaneously resulting in desorption of target species in that reactor and, in some embodiments, catalytic generation of desired product) (Jeong-Potter; paragraph [0053]; Fig. 3). One of ordinary skill in the art would recognize that actively feeding a first stream into a first reactor while vacuum is applied to a second reactor comprises thermal reaction modules that operate at different temperatures. Therefore, as with claim 10, it would have been prima facie obvious to combine Shearman, Iaccino, McCune, Jeong-Potter, and Fryda to arrive at the claimed invention.
Regarding claim 19 depending from claim 10 and claim 20 depending from claim 18, Iaccino teaches a NOx removal method from mixtures comprising molecular hydrogen, methane, and other hydrocarbons produced by hydrocarbon upgrading and conversion processes such as catalytic cracking, pyrolysis, hydroprocessing, reforming, and the like, as detailed above (Iaccino; Title; paragraph [0003]). One of ordinary skill in the art could reasonably deduce that gaseous mixtures produced by pyrolysis can comprise a waste stream from chemical vapor deposition (i.e., a carbon deposition technique based on the principles of pyrolysis). Of particular note, Iaccino teaches a first stream of hydrocarbon gas, comprising ≥ 1.0 wt.% methane, ≥ 1.0 wt.% molecular hydrogen, and ≥ 2.0 ppbw of NOx (Iaccino; claim 1). The ranges of methane and hydrogen overlap with the ranges recited in instant claim 19, and the range of NOx overlaps with the range recited in instant claim 20. MPEP § 2144.05(I) states that “[i]n the case where the claimed ranges ‘overlap or lie inside ranges disclosed by the prior art’ a prima facie case of obviousness exists.” In addition, Iaccino teaches that in certain aspects, the first stream has a molecular weight in the range of 16.0 to 27.0, wherein 100 mole of the first stream comprises 10.0 mole to 50.0 mole of molecular hydrogen, 5.0 mole to 30.0 mole of methane, 0.05 mole to 35.0 mol of ethylene, 5.0 mole to 20.0 mole of ethane, 0.1 mole to 15.0 mole of propylene, 4×10−4 mole to 3.0 mole of butadiene, 0.1 mole to 25 mole of C3+ saturates, and ≧3.0 ppbm NO, with the balance being, e.g., one or more of water, carbon monoxide, carbon dioxide, sulfur-containing compounds, mercury and/or mercury-containing compounds, metals, coke, particulates, or nitrogen oxides of higher order, such as ≧1.0 ppbm of NO2 (Iaccino; paragraph [0041]). Although Iaccino does not explicitly teach that the waste stream comprises about 0.0001% and 10% carbon monoxide by mass and about 0.0001% and 10% carbon dioxide by mass, as recited in instant claim 19, the skilled artisan would recognize that certain embodiments of the gas stream of Iaccino exist that would render amounts of carbon monoxide and carbon dioxide that read on these ranges. For example, when 99.8/100 mole of the first stream is accounted for as detailed above, and the remaining balance is 0.1 mole of carbon monoxide (2.8 grams) and 0.1 mole of carbon dioxide (4.4 grams), this would correspond to (based on the first stream molecular weight range of 16.0 to 27.0 grams per mole) 0.001-0.002% carbon monoxide by mass and 0.002-0.003% carbon dioxide by mass, respectively, and these ranges read directly on the ranges recited in instant claim 19. MPEP § 2144.05(I) states that “[i]n the case where the claimed ranges ‘overlap or lie inside ranges disclosed by the prior art’ a prima facie case of obviousness exists.”
Although Iaccino does not explicitly teach that the waste stream further comprises or wherein the waste stream further comprises between 0.1 ppm and 5000 ppm non-methane hydrocarbons and 0.01 ppm and 5000 ppm inert gases, as recited in instant claim 20, the teachings of Iaacino do indicate that trace amounts of carbon monoxide and carbon dioxide are present in the gaseous mixture, and that the quantity of non-methane hydrocarbons in the gaseous mixture is variable. Furthermore, Fryda teaches CVD embodiments with up to 50% argon in the gas phase and successful closed gas diamond CVD circuits with methane-argon-hydrogen gas flows (Fryda; page 1042, Col. 2, paragraph 3; page 1044, Col. 1, paragraph 2).
In spite of the deficiencies in the prior art cited above, in particular with the claim limitations wherein the waste stream further comprises between 0.1 ppm and 5000 ppm non-methane hydrocarbons and 0.01 ppm and 5000 ppm inert gases, as recited in instant claim 20, the teachings of Iaccino as a whole would inform the skilled artisan that the waste gas composition of methane pyrolysis can vary substantially. Furthermore, the skilled artisan would recognize that the waste gas streams from CVD processes are directly correlated with the input gas streams, and the inert gas content such as argon can vary, as taught by Fryda. Therefore, these prior art teachings as a whole would inform the skilled artisan that the waste stream compositions can be adjusted and controlled by virtue of the selected CVD gas input stream composition and the CVD parameters employed, such that the waste stream composition as recited in instant claims 19-20 could be arrived at through means of routine optimization, and is thus not inventive in nature. MPEP § 2144.05(II) states that “[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.” Therefore, as with claim 10, it would have been prima facie obvious to combine Shearman, Iaccino, McCune, Jeong-Potter, and Fryda to arrive at the claimed invention.
Claim 17 is rejected under 35 U.S.C. 103 as being unpatentable over Shearman et al. (US 2021/0348301 A1; PTO-892 of 07-15-2025; hereinafter “Shearman”), in view of Iaccino et al. (US 2015/0267131 A1; PTO-892 of 07-15-2025; hereinafter “Iaccino”), McCune et al. (US 4,919,974; IDS of 09-25-2025; hereinafter “McCune”), Jeong-Potter et al. (US 2024/0115987 A1; IDS of 06-03-2025; published 04-11-2024; hereinafter “Jeong-Potter”), and Fryda et al. (Diam. Relat. Mater. 1994, 3, 1040-1044; hereinafter “Fryda”) as applied to claims 10-16 and 18-20 above, and further in view of Arroyo-Caire et al. (Nanomaterials 2023, 13, 2914, pages 1-21; PTO-892 of 07-15-2025; hereinafter “Arroyo-Caire”).
Regarding claim 17, claim 16 is rendered obvious over Shearman in view of Iaccino, McCune, Jeong-Potter, and Fryda, as detailed above.
Although Iaccino teaches a waste stream comprising, e.g., molecular hydrogen, water, methane, ethylene, ethane, carbon monoxide, carbon dioxide, and NOx, wherein the NOx removal step utilizes one or more NOx removal agent, including those capable of reducing NO to N2 and O2 or to a metal oxide, as detailed above (Iaccino; paragraphs [0049] and [0084], Fig. 3), and Shearman teaches a first mixture from a first air sample comprising nitrogen (Shearman; claim 1), Shearman, Iaccino, McCune, Jeong-Potter, and Fryda fail to explicitly teach wherein treating the waste stream further comprises producing ammonia from the nitrogen or reactive nitrogen species, as recited in instant claim 17. However, Arroyo-Caire reviews the design of new catalysts for ammonia synthesis and teaches that there is a growing interest in green ammonia production that has spurred the development of new catalysts with the potential to carry out the Haber-Bosch process under mild pressure and conditions, and there is a pressing need to increase the sustainability of the process (Arroyo-Caire; Title; Abstract; page 1, paragraph 3). Arroyo-Caire further teaches that the hydrogen used for ammonia synthesis is mainly obtained from non-renewable sources (e.g., natural gas reforming):
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and this process is normally carried out in large central facilities which contain two large industrial plants in one (a steam methane reforming plant and an ammonia synthesis plant) (Arroyo-Caire; page 1, paragraphs 1-2 and equation 1). Thus, the teachings of Arroyo-Caire would inform the skilled artisan that the production of ammonia from nitrogen (i.e., the Haber-Bosch process), as recited in the instant claim, is well-established in the art and is in practice normally coupled with hydrocarbon reforming processes and industrial processes involving the processing of methane and the utilization of hydrogen gas, and therefore resides in the overlapping technical fields taught by Shearman, Iaccino, and Jeong-Potter, and is thus deemed analogous art, as described in MPEP § 2141.01(a). Furthermore, both Arroyo-Caire and Fryda emphasize the need for sustainable practices for chemical processes. Thus, the skilled artisan would be sufficiently motivated to incorporate the teachings of Arroyo-Caire with Shearman, Iaccino, McCune, Jeong-Potter, and Fryda to realize an improved method wherein nitrogen in the waste steam is further utilized for the sustainable production of ammonia. Such an endeavor would result in combining prior art elements according to known methods to yield predictable results, as described in MPEP § 2143(I)(A). Therefore, 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 have modified Shearman, Iaccino, McCune, Jeong-Potter, and Fryda to incorporate the teachings of Arroyo-Caire to implement wherein treating the waste stream further comprises producing ammonia from the nitrogen. The motivation to do so would permit the skilled artisan to pursue, with a reasonable expectation of success, an efficient ammonia production from waste streams comprising nitrogen that minimize waste and energy consumption and increase the sustainability of the process, as described above.
Based on the combined teachings of the references, the Examiner submits that a person of ordinary skill in the art would have had a reasonable expectation of success of arriving at the instantly claimed method. Therefore, the invention as a whole would have been prima facie obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, and absent a clear showing of evidence to the contrary.
Response to Arguments
Claim Rejections - 35 USC § 103
Applicant's arguments filed 15 October 2025, asserting that the cited prior art teachings do not teach each and every limitation of independent claims 1 and 10, have been fully considered but they are not persuasive.
Applicant argues the following:
“"receiving a waste stream from chemical vapor deposition growth [...] the waste stream comprising [...] acetylene"
The Applicant respectfully asserts that the references, alone or in combination, do not teach “receiving a waste stream from chemical vapor deposition growth [...] the waste stream comprising [...] acetylene” as recited in Claim 1 and Claim 10.
None of the references teach a chemical vapor deposition “waste stream comprising [...] acetylene”. While Iaccino mentions acetylene, reciting “In addition to the methane and the molecular hydrogen, the first stream can further comprise water and additional hydrocarbon such as C2+ hydrocarbon, and in particular, C2+ unsaturates, such as one or more of acetylene, ethylene, or propylene” (Iaccino, [0039]), Iaccino does not teach that this stream is a chemical vapor deposition waste stream. Specifically, Iaccino recites that the first stream can be “obtained from one or more hydrocarbon upgrading and conversion processes such as catalytic cracking, pyrolysis, hydroprocessing, reforming, etc.” (Iaccino, [0037]). Therefore, Iaccino does not teach “receiving a waste stream from chemical vapor deposition growth [...] the waste stream comprising [...] acetylene” as recited in Claim 1 and Claim 10. The other references are silent of “acetylene” (and the analogous 'ethyne') and, therefore, fail to overcome this deficiency.”
This argument has been fully considered, but is not found to be persuasive. According to the new 103 rejection above (necessitated by amendment), although Iaccino does not explicitly teach that the waste stream is a chemical vapor deposition waste stream, Iaccino does teach that the gaseous mixtures are obtained by processes including pyrolysis, and chemical vapor deposition is established in the prior art by definition as a technique designed for carbon nanomaterial synthesis that is based on the principle of pyrolysis (c.f., Claim Interpretation section; Devi et al., page 2, Col. 1, paragraph 1; Oxf. Open Mater. Sci. 2021, 1, pages 1-30; PTO-892 of 07-15-2025). Furthermore, the presence of hydrogen, methane, non-methane carbons including acetylene in chemical vapor deposition waste streams is well-established in the prior art as evidenced by McCune (IDS of 09-25-2025), who teaches the preparation of diamond composites by chemical vapor deposition, wherein hot filament chemical vapor deposition (HFCVD) is used to dissociate gas mixtures containing CH4 and H2 at 2000-2800 K, and the dissociation products at these temperatures consist mainly of radicals, for example, CH2, C2H, and CH, acetylene, and atomic hydrogen, as well as unreacted CH4 and H2 (McCune; Title; Abstract; Col. 5, lines 30-44). Finally, Fryda teaches a method of diamond CVD with a closed gas circuit which is able to remove undesired products of the CVD process and replenish the necessary gaseous components, particularly methane and carbon monoxide, wherein Fryda further teaches a gas composition comprising methane as the dominant species in equilibrium, while the concentrations of acetylene and other species are orders of magnitude smaller (Fryda; Title; Abstract; page 1040, Col. 2, paragraph 2 and page 1041, Col. 1, paragraph 1). Thus, one of ordinary skill in the art would recognize based on this cited prior art that the waste gas of CVD processes commonly contain at least small amounts of acetylene. Therefore, the new claim rejections are maintained for the reasons of record and the reasons set forth above.
Applicant argues the following:
“Affidavit under 37 CFR §1.132
The Applicant additionally asserts that it would not be obvious to receive acetylene in the waste stream for processing. The Applicant has submitted a first 1.132 Affidavit requesting special consideration for the present Application in view of the unexpected absence of green oil formed via polymerization of acetylene in the waste stream.
In the affidavit submitted under 37 CFR §1.132, the Applicant respectfully asserts that the methods of the claimed invention of the present application have produced unexpected results in the field, in relation to processing waste streams containing acetylene. In particular, a person of ordinary skill in the art would have expected that acetylene present in a waste stream from CVD processes would polymerize or oligomerize when exposed to the conditions of a thermal reactor. Further, the presence of hydrogen in the waste stream can further promote partial hydrogenation, generating reactive intermediates and radicals that can initiate chain-growth polymerization. These combined effects can result in the formation of "green oil," a sticky polymeric deposit known to accumulate in thermal reactors, leading to clogging, fouling, and potential reactor failure. Such behavior of acetylene under thermal reactor conditions is well documented in the literature and is a recognized concern for reactor operation and maintenance.
Specifically, the Kuruchki reference (Appendix B1) states: "In the C2 acetylene hydrogenation reactor where acetylene is hydrogenated to ethylene and ethane, the most commonly used catalyst is palladium (Pd) on Alumina (A12O3) support. Green oil polymer is formed by side reactions of the hydrogenation reaction itself, and it cannot be totally avoided." (pg 48). Kuruchki further teaches: "The gas leaving the hydrogenation reactor is cooled, and more green oil condenses into fine droplets, which deposit on the downstream heat exchangers, dehydrator beds, and on the ethylene fractionator internals. These depositing droplets are polymeric and cause fouling of the equipment, thus potentially leading to expensive unplanned shutdowns to clean up the deposited green oil." Furthermore, the Trotuş reference (Appendix B2) teaches the reactivity of acetylene and how the polymerization of acetylene can impair reactors by "deactivating the catalyst by blocking access to the active sites" (pg. 1765). In particular, the affidavit submitted under 37 CFR §1.132 recites that well-known challenges of a thermal reactor "receiving a waste stream [...] comprising [...] acetylene", as recited in Claim 1 and Claim 10, including the polymerization of acetylene and formation of green oil which can clog a reactor and block active sites. The Applicant respectfully asserts that a person of ordinary skill in the art would not expect a thermal reactor "receiving a waste stream [...] comprising [...] acetylene" nor that the thermal reactor could operate without fouling, as presented in Appendix A.
As such, the Applicant respectfully requests secondary consideration of the claims of the present Application by the Examiner, in light of the first affidavit submitted under 37 CFR §1.132.”
This argument has been fully considered, but is not found to be persuasive. Applicant’s claims of unexpected results in the affidavit and corresponding supporting appendices filed 15 October 2025 are not persuasive, because the claimed amount of acetylene in the waste stream (i.e., “…wherein the non-methane hydrocarbons comprises between 0.1 ppm and 5000 ppm acetylene…” as recited in amended claim 1; and “…wherein the waste stream further comprises between 0.1 ppm and 5000 ppm non-methane hydrocarbons…” as recited in claim 20 which is indirectly dependent on amended claim 10) is present in such low quantities that one of ordinary skill in the art would not reasonably expect significant polymerization or green oil formation in the process. Furthermore, references of Appendix B1 and B2 are not considered germane to the instantly claimed process. For example, the teachings of Kuruchki et al. (Appendix B1) refer to an acetylene hydrogenation unit wherein the feed stream comes from petroleum steam crackers (not CVD exhaust gas), the overhead contains some 0.5%-2.5% acetylene (a range that exceeds the acetylene quantities described in Appendix A), and the hydrogenation catalyst is Pd/Al2O3 (Kuruchki; page 59, Col. 2, paragraphs 1 and 3); although Pd/Al2O3 is a catalyst encompassed by the genus of instant claim 5, the Appendix A provide in Applicant’s affidavit filed 15 October 2025 does not specify what hydrogenation catalyst is used, therefore a direct comparison (in terms of the production of green oil) of the alleged unexpected results of the presently claimed invention and the teachings of Kuruchki cannot be clearly defined. In addition, the teachings of Trotuş et al. (Appendix B2) regarding “"deactivating the catalyst by blocking access to the active sites" (pg. 1765)” as cited by Applicant is specifically referring to catalysts (Hg, Au, Cu, ZnO/SiO2) used for the electrophilic addition of Bronsted acids to the triple bond of acetylene (Trotuş; page 1765, Col. 2, paragraph 3), and is therefore associated with a class of catalysts and a reaction transformation is not commensurate in scope with the claims. See MPEP § 716. Therefore, the new claim rejections are maintained for the reasons of record and the reasons set forth above.
Applicant argues the following:
“Failure to motivate combination/impermissible hindsight
The Patent Office recites:
"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 have modified Shearman to incorporate the teachings of laccino, Munro, Kokka, Arroya-Caire, and Pedersen to develop a method comprising: a) receiving a waste stream from chemical vapor deposition growth of a carbonaceous material, the waste stream comprising hydrogen, methane, carbon oxides, non-methane hydrocarbons, and nitrogen species; b) hydrogenating the waste stream to reduce unsaturated non-methane hydrocarbons or unsaturated nitrogen species to saturated non-methane hydrocarbons or saturated nitrogen species; c) pre- reforming the saturated non- methane hydrocarbons or saturated nitrogen species to the carbon oxides, water, and nitrogen; d) methanating the carbon oxides to upcycled methane; e) producing ammonia from the nitrogen; and f) using the upcycled methane for further chemical vapor deposition growth of the carbonaceous material."
The Applicant respectfully disagrees. The Applicant asserts that the Patent Office's rationale relies on knowledge of the Applicant's disclosure to identify a benefit and motivation for the combination. This constitutes impermissible hindsight reconstruction. See In re Rouffet, 149 F.3d 1350, 1357 (Fed. Cir. 1998) ("hindsight bias makes it difficult to determine obviousness without relying upon the applicant's disclosure"). Absent the teachings of the present application, the cited references do not suggest or provide a reason to combine the synthetic diamond growth using upcycled methane taught by Shearman, the NOx removal method taught by Iaccino, the hydroprocessing method taught by Munro, the hydrogen production process taught by Kokka, the ammonia synthesis process taught by Arroyo-Caire, and the green chemical vapor deposition teachings taught by Pedersen. While the Patent Office states that the references "reside in the overlapping technical areas of methane and hydrogen utilization via interrelated chemical processes that are generally well-established in industrial practice", the Applicant asserts that the technical areas of the references are disparate and would not be obvious to combine. Each reference is directed towards solving a specific problem within its own technical domain. A person of ordinary skill in the art, when faced with the problem of producing synthetic diamonds from atmospheric carbon, would not be led to combine the very specific NOx removal techniques, detailed catalyst studies for propane reforming or ammonia synthesis, general hydroprocessing methods, and a sustainability philosophy for CVD with a particular reactor heating technology, especially when these combinations introduce unforeseen complexities and challenges.”
This argument has been fully considered, but is not found to be persuasive.
In response to Applicant's argument that the Examiner's conclusion of obviousness is based upon improper hindsight reasoning, it must be recognized that any judgment on obviousness is in a sense necessarily a reconstruction based upon hindsight reasoning. But so long as it takes into account only knowledge which was within the level of ordinary skill at the time the claimed invention was made, and does not include knowledge gleaned only from the applicant's disclosure, such a reconstruction is proper. See In re McLaughlin, 443 F.2d 1392, 170 USPQ 209 (CCPA 1971).
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, as detailed in the new 103 rejections above, the skilled artisan could reasonably arrive at the method steps of b) [Wingdings font/0xE0] e), wherein the processes are carried out in separate continuous reactors, based on the teachings of Munro and the supporting teachings of Rosen. Furthermore, Iaccino in view of the supporting teachings of McCune inform the skilled artisan that pyrolysis waste gas, including from diamond CVD processes, contain acetylene and the other components described in instant claims 1 and 10. In addition, Fryda teaches the feasibility of a closed gas circuit for diamond CVD, based on a chemical reprocessing of the exhaust gas from any CVD reactor (Fryda; page 1044, Col. 1, paragraph 2). Thus, Fryda demonstrates that CVD exhaust gases comprising hydrogen, methane, and small amounts of acetylene and other species can be effectively recycled and are amenable to chemical reprocessing, including the production of methane for further use in CVD processes, in a manner consistent with instant claims 1 and 10. Taken together, one of ordinary skill in the art would be sufficiently motivated to incorporate these processes into the method of Shearman (who teaches upcycling of methane as a precursor for CVD diamond synthesis) to pursue, with a reasonable expectation of success, an improved CVD method that minimizes waste and energy consumption in the precursor supply chain by recycling CVD exhaust gas, as described above. Therefore, the new claim rejections are maintained for the reasons of record and the reasons set forth above.
Applicant argues the following:
“Assuming arguendo that references teach each of the disparate limitations of Claim 1, as indicated by the Patent Office, the references do not motivate the exact combination of steps of the chemical processing pipeline recited in Claim 1 and do not suggest that the steps can be "performed as a continuous process by a set of electrified thermal reactors in fluid connection". While Pedersen mentions "recycl[ing] unconsumed CVD gases and precursors" (Pedersen, F. Summary of suggested Green CVD philosophy), Pedersen only describes recycling helium, stating:
"Helium is very abundant in the universe (approximately 24% in mass) but relatively scarce on earth since it can escape the earth's gravitational field. Helium is captured during the fractional distillation of natural gas, which makes it prone to global cyclic supply and demand issues. This provides an economic incentive for recycling He since recovering and recycling helps reduce exposure to shortages, lowering the burden on keeping a stable production and minimizing the impact of supply disruptions." (Pedersen, C. Sustainable reactor design.).
Pedersen never discloses processes involving "hydrogen, methane, carbon oxides, non- methane hydrocarbons, acetylene, and nitrogen species" as recited in Claim 1 and/or any methods for processing (e.g. "hydrogenating", "methanating", "prereforming", as recited in Claim 1), reusing, upcycling, and/or recycling the unconsumed CVD gases. Pedersen even suggests that processing unconsumed CVD gases may be harmful for the environment, teaching away from the practice, stating, "Some of these principles are seemingly contradictory [...] Recycling of unconsumed CVD gases could require increased vacuum volume and energy consumption for the CVD reactor and possibly also for compression of the gases: this increase in energy must then be compared with the energy saved by the lower molecular consumption in the CVD process." (Pedersen, F. Summary of suggested Green CVD philosophy). Therefore, the "recycling" concept taught by Pedersen is not enough to motivate the limitations as recited in Claim 1.
Furthermore, the Applicant respectfully asserts that the references do not teach or suggest "wherein the method is performed as a continuous process by a set of electrified thermal reactors in fluid connection", as recited in Claim 1. The Applicant asserts that it would not be obvious to perform the steps (steps a-f of Claim 1) "as a continuous process by a set of electrified thermal reactors in fluid connection" as recited in Claim 1. Given the highly specialized nature and distinct problems addressed by each reference, a person of ordinary skill would not have had a reasonable expectation of success in combining them to achieve the claimed invention. The synergistic combination of these disparate technologies, as defined in the claims and shown in the 1.132 Affidavit, represents a unique and non-obvious solution that is not taught or suggested by the prior art.”
This argument has been fully considered, but is not found to be persuasive. Applicant’s arguments regarding the teachings of Pedersen cited in the previous Office Action mailed 15 July 2025 are moot in view of the new 103 claim rejections detailed herein (necessitated by amendment), wherein the teachings of Pedersen are no longer relied upon. The newly cited prior art of In Fryda teaches the feasibility of a closed gas circuit for diamond CVD, based on a chemical reprocessing of the exhaust gas from any CVD reactor and thus demonstrates that CVD exhaust gases comprising hydrogen, methane, and small amounts of acetylene and other species can be effectively recycled and are amenable to chemical reprocessing, including the production of methane for further use in CVD processes, in a manner consistent with instant claims 1 and 10 (Fryda; page 1044, Col. 1, paragraph 2).
Regarding Applicant’s assertion that the references do not teach or suggest "wherein the method is performed as a continuous process by a set of electrified thermal reactors in fluid connection", as recited in amended claim 1, the limitations are adequately addressed by Munro, Rosen, and Zheng as detailed in the new 103 rejections above. The sequence of hydrogenation [Wingdings font/0xE0] steam reforming (i.e., pre-reforming) [Wingdings font/0xE0] methanation is depicted in the Figure taught by Munro, wherein the reactor 22 (as in step b) of instant claim 1) can cycle light hydrocarbons produced in the hydroprocessing step to the steam reformer 6 (as in step c) of instant claim 1) via line 2, and the hydrogen produced in the reformer can be transported to methanator 19 via line 18 for the removal of carbon oxides (as in step d) of instant claim 1). Thus, the skilled artisan would readily ascertain that the combination process of Munro teaches a process consistent with steps b) [Wingdings font/0xE0] c) [Wingdings font/0xE0] d) of instant claim 1. Furthermore, the process of Munro defines the feed in units of liquid hourly space velocity (Munro; claim 5, Col. 6, lines 7-8 and 41-42; Col. 9, line 7), a unit specifically used for continuous processes, as further evidenced by Rosen (Rosen; page 7, section 2.5: Space Time and Space Velocity); thus, the skilled artisan would recognize from the teachings of Munro (Figure; claim 5, Col. 6, lines 7-8 and 41-42; Col. 9, line 7) and the supporting teachings of Rosen that the process of Munro is performed in a continuous manner via a set of reactors in fluid connection, in a manner consistent with instant claim 1 (Munro; Figure). Finally, Munro teaches that as an alternative to the methanation step, a nitrogen washing column may be employed to remove methane and carbon monoxide, thereby producing a gas suitable for the synthesis of ammonia (Munro; Col. 4, lines 48-50). In addition, the skilled artisan could reasonably ascertain based on the teachings of Munro alone that this ammonia synthesis step would, as in steps b)-d), occur in a separate reactor, especially since Munro teaches a nitrogen separation step after steam reformation and prior to methanation. Thus, the teachings of Munro further suggest to the skilled artisan that this continuous combination process can further be coupled to producing ammonia from the nitrogen involved in the process, (i.e., steps b) [Wingdings font/0xE0] e) of instant claim 1, such that these method steps could be performed in a continuous fashion and in separate continuous reactors, in a manner consistent with instant claims 1-2 and 4. Finally, Zheng teaches direct application of Joule heated reactors to methane pyrolysis (as is known in the art to be involved with chemical vapor deposition, consistent with steps a) and f) of the method of claim 1), ammonia synthesis (consistent with step e) of the method of claim 1), methane steam reforming (consistent with step c) of the method of claim 1), and CO2 methanation (consistent with step d) of the method of claim 1). Thus, the skilled artisan would be sufficiently motivated to implement the teachings of Zheng to realize the benefits of Joule heated (i.e., electrified) thermal reactors, since fast heating with joule-heated reactors can be driven by renewable energy, the direct electrification of catalytic processes through the Joule effect not only eliminates CO2 emissions from fuel combustion but also provides the required heat for highly endothermic processes such as methane steam reforming (Zheng; page 14, Table 5, entries 1-2, 4, and 6; Col. 2, paragraph 3). Thus, the skilled artisan would be sufficiently motivated to incorporate the elements of Munro, Rosen, and Zheng to arrive at the instantly claimed process wherein each method step is performed continuously in separate electrified thermal reactors, in a manner consistent with instant claims 1-2 and 4, respectively. Therefore, the new claim rejections are maintained for the reasons of record and the reasons set forth above.
Conclusion
No claims are allowed.
Applicant’s amendment under 37 CFR 1.97(c) with the fee set forth in 37 CFR 1.17(p) on 15 October 2025 necessitated and prompted 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 mailing date of this final action.
Any inquiry concerning this communication or earlier communications from the Examiner should be directed to Derek Rhoades whose telephone number is (703)-756-5321. The Examiner can normally be reached Monday–Thursday, 7:30 am-5:00 pm EST; Friday, 7:30 am-4:00 pm EST.
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/D.R./Examiner, Art Unit 1692
/AMY C BONAPARTE/Primary Examiner, Art Unit 1692
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