Notice of Pre-AIA or AIA Status
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
DETAILED ACTION
This Office action is based on the 19/057228 application originally filed February 19, 2025.
Amended claims 11-20, filed February 19, 2025, are pending and have been fully considered.
Double Patenting
The nonstatutory double patenting rejection is based on a judicially created doctrine grounded in public policy (a policy reflected in the statute) so as to prevent the unjustified or improper timewise extension of the “right to exclude” granted by a patent and to prevent possible harassment by multiple assignees. A nonstatutory double patenting rejection is appropriate where the conflicting claims are not identical, but at least one examined application claim is not patentably distinct from the reference claim(s) because the examined application claim is either anticipated by, or would have been obvious over, the reference claim(s). See, e.g., In re Berg, 140 F.3d 1428, 46 USPQ2d 1226 (Fed. Cir. 1998); In re Goodman, 11 F.3d 1046, 29 USPQ2d 2010 (Fed. Cir. 1993); In re Longi, 759 F.2d 887, 225 USPQ 645 (Fed. Cir. 1985); In re Van Ornum, 686 F.2d 937, 214 USPQ 761 (CCPA 1982); In re Vogel, 422 F.2d 438, 164 USPQ 619 (CCPA 1970); In re Thorington, 418 F.2d 528, 163 USPQ 644 (CCPA 1969).
A timely filed terminal disclaimer in compliance with 37 CFR 1.321(c) or 1.321(d) may be used to overcome an actual or provisional rejection based on nonstatutory double patenting provided the reference application or patent either is shown to be commonly owned with the examined application, or claims an invention made as a result of activities undertaken within the scope of a joint research agreement. See MPEP § 717.02 for applications subject to examination under the first inventor to file provisions of the AIA as explained in MPEP § 2159. See MPEP § 2146 et seq. for applications not subject to examination under the first inventor to file provisions of the AIA . A terminal disclaimer must be signed in compliance with 37 CFR 1.321(b).
The filing of a terminal disclaimer by itself is not a complete reply to a nonstatutory double patenting (NSDP) rejection. A complete reply requires that the terminal disclaimer be accompanied by a reply requesting reconsideration of the prior Office action. Even where the NSDP rejection is provisional the reply must be complete. See MPEP § 804, subsection I.B.1. For a reply to a non-final Office action, see 37 CFR 1.111(a). For a reply to final Office action, see 37 CFR 1.113(c). A request for reconsideration while not provided for in 37 CFR 1.113(c) may be filed after final for consideration. See MPEP §§ 706.07(e) and 714.13.
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Claims 11, 15 and 20 are rejected on the ground of nonstatutory double patenting as being unpatentable over claims 1, 3 and 5-9 of U.S. Patent No. 10,525,407 in view of Ogawa et al. (US 2011/0288355) hereinafter “Ogawa”. Although the claims at issue are not identical, they are not patentably distinct from each other because the current application and US Patent ‘407 disclose the method for converting methane in a gas flow stream of C2 hydrocarbons, H2 and aromatics, separating the aromatics and recycling the gas flow stream. Although, US Patent ‘407 fails to disclose an aromatic separation device, it would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to add the aromatic separation device of Oagawa to the methane conversion system of US Patent ‘407. The motivation to do so is to add an aromatic separation device to a lower hydrocarbon conversion system in order to effectively separate aromatic compounds, including benzene or the like.
Claim Rejections - 35 USC § 103
In the event the determination of the status of the application as subject to AIA 35 U.S.C. 102 and 103 (or as subject to pre-AIA 35 U.S.C. 102 and 103) is incorrect, any correction of the statutory basis (i.e., changing from AIA to pre-AIA ) for the rejection will not be considered a new ground of rejection if the prior art relied upon, and the rationale supporting the rejection, would be the same under either status.
The following is a quotation of 35 U.S.C. 103 which forms the basis for all obviousness rejections set forth in this Office action:
A patent for a claimed invention may not be obtained, notwithstanding that the claimed invention is not identically disclosed as set forth in section 102, if the differences between the claimed invention and the prior art are such that the claimed invention as a whole would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to which the claimed invention pertains. Patentability shall not be negated by the manner in which the invention was made.
The factual inquiries for establishing a background for determining obviousness under 35 U.S.C. 103 are summarized as follows:
1. Determining the scope and contents of the prior art.
2. Ascertaining the differences between the prior art and the claims at issue.
3. Resolving the level of ordinary skill in the pertinent art.
4. Considering objective evidence present in the application indicating obviousness or nonobviousness.
This application currently names joint inventors. In considering patentability of the claims the examiner presumes that the subject matter of the various claims was commonly owned as of the effective filing date of the claimed invention(s) absent any evidence to the contrary. Applicant is advised of the obligation under 37 CFR 1.56 to point out the inventor and effective filing dates of each claim that was not commonly owned as of the effective filing date of the later invention in order for the examiner to consider the applicability of 35 U.S.C. 102(b)(2)(C) for any potential 35 U.S.C. 102(a)(2) prior art against the later invention.
Claim(s) 11-20 is/are rejected under 35 U.S.C. 103 as being unpatentable over Wachsman et al. (US 2018/0296974) hereinafter “Wachsman” in view of Ogawa et al. (US 2011/0288355) hereinafter “Ogawa”.
Regarding Claims 11-13 and 17-19
Wachsman discloses in paragraph 0007, the reactor can have a first volume, where a feed gas including methane is provided, separated from a second volume, where a sweep gas is provided, by an H2-permeable wall. The H2-permeable wall includes a dense mixed ionic-electronic permeable thin film membrane supported on a porous wall and transports H2 generated in the first volume by the conversion reaction to the second volume for removal by (or reaction with) the sweep gas. The removal of H2 from the first volume can lead to significant increase in the amount of methane converted (up to 40%), while maintaining product selectivity for C2 hydrocarbons and aromatics.
Wachsman discloses in paragraph 0008, a method of converting methane comprises flowing methane in a first volume so as to contact a catalyst in a reactor while heating the reactor to an elevated temperature. The method can further include transporting hydrogen (H2) from the first volume to a second volume in the reactor via a membrane supported within the reactor, and removing products from the first volume. The products can comprise C2+ hydrocarbons and/or aromatics.
Wachsman discloses in paragraph 0009, a methane conversion device comprises a reactor, a membrane, and a catalyst. The reactor can have first and second gas volumes separated by the membrane. The catalyst can be disposed to interact with gas of the first gas volume. The membrane can be constructed to transport H2 between the first and second gas volumes.
Wachsman discloses in paragraph 0059, methane can be provided from a primary feed gas source 206 to the reactor 202 via a respective inlet line that passes through a wall of the furnace 204, e.g., via respective heat seal 214 b. In certain embodiments, the gas provided to the first gas volume of the reactor consists essentially of methane, i.e., minor concentrations (e.g., <20%) of other gases (such as, but not limited to, a tracer or inert gas) may be included but do not otherwise affect the reaction. In other embodiments, a secondary feed gas from one or more secondary feed gas sources 216 can be provided to the first gas volume to tune the conversion efficiency and/or selection of products, as described in further detail below. The resulting products and/or any remaining unconverted methane can be removed from the first volume of the reactor 202 via a respective outlet line that passes through a wall of the furnace 204, e.g., via respective heat seal 214 d. The products can be separated from the methane for subsequent use or storage, while the unconverted methane may be recirculated back to source 206 or the first gas volume of the reactor 202 for conversion.
Wachsman discloses in paragraph 0064, the reactor 202 can be configured as a tubular reactor, with an inner tube defining the first gas volume and an annular space between the inner tube and an outer tube serving as the second gas volume. A wall of the inner tube can be formed with the permeable membrane thereon, such that the reactor can be considered a tubular membrane reactor. In addition, a catalyst can be provided in or adjacent to the first gas volume so as to catalyze the desired methane conversion, such that the reactor can be considered a packed-bed tubular membrane reactor.
Wachsman further discloses in paragraph 0065, an exemplary configuration of such a packed-bed tubular membrane reactor 300 is illustrated schematically in FIG. 3A. The reactor 300 can have a first gas volume 302 formed by the interior volume of a porous support tube 304. A permeable membrane 306 can be provided on a surface of the support tube 304, for example, on the radially outer surfaces of the support tube 304. Feed gas can be provided to the first gas volume 302 via gas inlet 312, where an inlet tube 320 disposed within the porous support tube 304 conveys the feed gas down to the first gas volume 302 into contact with a catalyst 324.
Wachsman discloses in paragraph 0068, a catalyst 324 can be provided in or adjacent to the first volume 302 for catalyzing the conversion of methane to the valued-added products. For example, the catalyst can be an Fe(c)SiO2 or Mo/ZSM5 material, preferably Fe(c)SiO2, where (c) denotes confinement and represents a catalyst characterized by the lattice-confined single iron sites embedded within a silica matrix. Although shown as extending to within inlet tube 320 and the first gas volume 302, it is also possible that the catalyst 324 can be disposed in other locations according to one or more contemplated embodiments. For example, the catalyst 324 can be disposed outside the inlet tube 320, for example, between the end cap 322 and an outlet end of the inlet tube 320 and/or in the annular space between the inlet tube 320 and the radially inner wall of the porous support 304.
Wachsman discloses in paragraph 0073, the feed gas entering the first gas volume 356 interacts with catalyst 354 and undergoes a reaction at elevated temperatures that results in the production of C2 hydrocarbons and aromatics, which are conveyed from the first gas volume via outlet 348, and H2, which is transported via porous support 334 and permeable membrane 336 to the second gas volume 332. In the second gas volume 332, the H2 potentially reacts with the sweep gas and is subsequently removed via outlet 344.
Wachsman discloses in paragraph 0080, the primary feed gas consists essentially of methane, i.e., it can have minor concentrations of tracer or inert gases that do not otherwise affect the conversion reactions. The secondary feed gas can include, for example, H2, C2H2, C2H4, C2H6, or any other hydrocarbon gas, such as, but not limited to, propane, butane, heptane, benzene, toluene, xylene, or an impurity hydrocarbon from shale gas. The secondary feed gas can be used to tune the methane conversion efficiency and/or selection of products, as described in further detail herein. Otherwise the process proceeds from 502 to 504, where only the primary feed gas is supplied to the first volume.
Wachsman discloses in paragraph 0083, the removed gases can be analyzed, separated, and/or processed for subsequent use. For example, unreacted feed gas or sweep gases can be resupplied to their respective inlets of the reactor for reprocessing. Desired products, such as C2 hydrocarbons, aromatics, H2 gas, ammonia, and/or syngas, can be separated and stored. Wachsman discloses in paragraph 0103, optimal flow rate for methane conversion may be dependent on temperature. Note, the selectivity to aromatics (e.g., benzene of about 15% and naphthalene of about 50%) is about the same for each temperature.
Wachsman discloses in paragraph 0084, although illustrated as separate steps, it is contemplated that various steps may occur simultaneously or iteratively. For example, the determinations regarding secondary feed gas 502 and secondary sweep gas 512 can repetitively occur at the same time as the other steps to allow the conversion efficiency and/or product selection to be altered based on feedback of removed products or other analyses. Moreover, the product reactions 508, H2 transport 510, sweep gas flows, and product removal 518 occur simultaneously despite being illustrated as sequential steps. Furthermore, certain steps illustrated as occurring after others may indeed occur before. For example, a sweep gas flow 514, 516 may be initiated before any feed gas flow 504, 506 begins.
It is to be noted Wachsman discloses separating the aromatics but fails to specifically teach an aromatic separation device.
However, it is known to apply an aromatic separation device after methane conversion, as taught by Oagawa.
Oagawa discloses in the abstract, a method of producing aromatic hydrocarbon and an apparatus for producing aromatic hydrocarbon by repeating a reaction step for obtaining aromatic hydrocarbon upon making a contact reaction between lower hydrocarbon and a catalyst and a regeneration step for regenerating the catalyst used in the reaction step. Off-gas which is gas obtained by removing aromatic hydrocarbon produced in the reaction step from discharge gas passing through the reaction step is used as a regeneration gas in the regeneration step.
Oagawa discloses in paragraph 0040, the aromatic hydrocarbon producing apparatus 10 is constituted of a first reactor 1, an aromatic hydrocarbon separation apparatus 3, a hydrogen monitor 4, an off-gas tank 6, a raw material gas tank 5, and a valve 7. Oagawa further discloses in paragraph 0041, the first reactor 1 is charged with a catalyst for aromatizing lower hydrocarbon. A raw material gas (for example, methane) is supplied from the raw material gas tank 5 and makes a contact reaction with the catalyst, thereby producing aromatic hydrocarbon (for example, benzene) and hydrogen. Oagawa discloses in paragraph 0042, gas obtained after a catalytic reaction and discharged from the first reactor 1 is supplied to the aromatic hydrocarbon separation apparatus 3 which separates aromatic hydrocarbon produced in the first reactor 1, from the supplied gas. Oagawa discloses in paragraph 0048, thus produced benzene and hydrogen (containing unreacted methane and argon and the like in a reaction gas) are supplied to the aromatic hydrocarbon separation apparatus 3 in which aromatic hydrocarbon is separated and removed. Gas (off-gas) obtained upon removing aromatic hydrocarbon from discharge gas obtained after the reaction is stored in the off-gas tank 6. Oagawa discloses in paragraph 0049, at this time, a hydrogen concentration of the off-gas is measured by the hydrogen monitor 4 provided to the aromatic hydrocarbon separation apparatus 3. The hydrogen concentration is a standard for making a changeover between the catalytic reaction and the regeneration reaction in the first reactor 1.
It would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to add the aromatic separation device of Oagawa to the methane conversion system of Wachsman. The motivation to do so is to add an aromatic separation device to a lower hydrocarbon conversion system in order to effectively separate aromatic compounds, including benzene or the like.
Regarding Claim 14
Wachsman discloses in paragraph 0089, at 608, the solution can be heated to a first temperature (e.g., 393K), and maintained at that temperature in order to evaporate the water under constant stirring. Once all the water evaporates, a gel is formed. The process proceeds to 610 where the temperature is raised to a higher second temperature (e.g., 673K) in order to auto-ignite the combustion.
Regarding Claims 15 and 16
Wachsman discloses in paragraph 0060, at a same time as the feed gas flow in the first gas volume of the reactor 202, a sweep gas flow can be provided in the second gas volume of the reactor 202. A primary sweep gas is provided from one or more primary sweep gas sources 208 to the reactor 202 via a respective inlet line that passes through a wall of the furnace 204, e.g., via a respective heat seal 214 a. For example, the sweep gas is helium (He) or another noble gas, so as not to react with any transported H2 from the first volume to the second volume. In some embodiments, a secondary sweep gas of H2 can be provided from secondary sweep gas source 218 can be provided to the second gas volume to modulate the transport of H2 between the first and second volumes, thereby tuning the conversion efficiency and/or product selection.
Wachsman discloses in paragraph 0061, the primary sweep gas is specifically selected to react with the transported H2. For example, the sweep gas can be air or steam and can react with the transported H2 to form water. In another example, the sweep gas can be N2 and can react with the transported H2 to form NH3 (ammonia). In still another example, the sweep gas can be CO2 or CO and can react with the transported H2 to form syngas, methanol, di-methyl ether, higher alcohols, and/or other hydrocarbons. In such embodiments, a secondary catalyst may be provided adjacent to or within the second gas volume to catalyze the reaction between the sweep gas and the H2. For example, a nickel (Ni) catalyst or other oxidation catalyst may be used on the sweep side, such as in the annular space between the porous support and an outer housing, or on a surface of either. Alternatively or additionally, the secondary catalyst can comprise Ni, Cu, Zn, or Fe supported on a metal oxide support, such as, but not limited to, SiO2, Al2O3, ZrO2, and CeO2.
Regarding Claim 20
Wachsman discloses in paragraph 0054, the permeable gas membrane can be a ceramic or ceramic composite, such as a perovskite-type oxide conductor. The porous support may be formed of a same or different material than the permeable gas membrane. For example, the porous support can be a ceramic or ceramic composite, such as a perovskite-type material. In embodiments, the material of the permeable gas membrane and the porous support are selected so as to have substantially the same coefficients of thermal expansion. The permeable gas membrane can be formed on the porous support and have a thickness of 50 μm or less. The porous support, in contrast, could have a thickness on the order of hundreds of microns, for example, 1 mm.
Wachsman discloses in paragraph 0055, the perovskite-type oxide conductor for the membrane can have a formula of M′Ce1-x-yZrxM″yO3-δ, where M′ is Sr or Ba, M″ is at least one of Ti, V, Cr, Mn, Fe, Co Ni, Cu, Nb, Mo, W, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm and Yb, x is between 0.1 and 0.2, inclusive, y is between 0.1 and 0.3, inclusive.
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to LATOSHA D HINES whose telephone number is (571)270-5551. The examiner can normally be reached Monday thru Friday 9:00 AM - 6:00 PM.
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If attempts to reach the examiner by telephone are unsuccessful, the examiner’s supervisor, Prem Singh can be reached at 571-272-6381. The fax phone number for the organization where this application or proceeding is assigned is 571-273-8300.
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/Latosha Hines/Primary Examiner, Art Unit 1771
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