DETAILED ACTION
Notice of Pre-AIA or AIA Status
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
Applicant's election with traverse of Group I, claims 1-2, 4-14,16-17 and 19-21 in the reply filed on April 21, 2026 is acknowledged. The traversal is on the ground(s) that the claimed solid oxide electrolysis unit and the claimed molar ratio CO/CO2 are not disclosed in the cited references . This is not found persuasive because the following disclosure cited in the office action cure the deficiency of the cited reference.
The requirement is still deemed proper and is therefore made FINAL.
Claims 15 and 18-19 drawn to non-elected claims are withdrawn from consideration.
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.
Claims 1-2, 4-14,16-17 and 20-21 are rejected under 35 U.S.C. 103 as being unpatentable over Reytier et al (US 2015/0329979 A1) in view of Makoto et al (JP 6603607 machine translation).
Applicants’ claimed invention is directed to a method for producing methanol, comprising the steps of: providing a carbon dioxide-rich stream and passing it through an electrolysis unit for producing a feed stream comprising CO and CO2; providing a water feedstock and passing it through an electrolysis unit for producing a feed stream comprising H2; combining said feed stream comprising CO and CO2 and said feed stream comprising H2 into a synthesis gas ;converting said synthesis gas into said methanol, wherein the step of providing the carbon dioxide-rich stream and passing it through the electrolysis unit for producing the feed stream comprising CO and CO2, is conducted as a once-through operation in a solid oxide electrolysis cell unit, wherein the molar ratio CO/CO2 in the feed stream comprising CO and CO2, or the synthesis gas, is in the range 0.2-0.6, and wherein the step of providing the carbon dioxide-rich stream and passing it through the electrolysis unit for producing the feed stream comprising CO and CO2, and the step of providing the water feedstock and passing it through the electrolysis unit for producing the feed stream comprising H2, are conducted separately.
Reytier teaches a method for high-temperature electrolysis of steam H2O and of another gas to be electrolyzed selected from carbon dioxide CO2 or nitrogen dioxide NO2, carried out in an electrolysis reactor comprising a stack of elementary electrolysis cells of the SOEC type each formed from a cathode, an anode and an electrolyte interposed between the cathode and the anode, and a plurality of electrical and fluidic interconnectors each arranged between two adjacent elementary cells with one of its faces in electrical contact with the anode of one of the two elementary cells and the other of its faces in electrical contact with the cathode of the other of the two elementary cells, comprising the following steps: supplying and distributing steam to the cathode of one of the two adjacent elementary cells and, supplying and distributing either carbon dioxide or nitrogen to the cathode of the other of the two elementary cells. See claim 1
Reytier teaches The second route consists of producing synthesis gas by electrolysis of carbon dioxide CO2 (III) and by introducing electrolysis of water H2O (I) separately according to the following equations and then mixing the products obtained:
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See paragraph 0013.
Reytier teaches independent electrolysis of the two gases according to the second route offers the major advantage of great flexibility in management of the H2/CO mixture. However, the major drawbacks of this second route are the need for capital investment in two separate electrolyzers (electrolysis reactors) and the lack of significant thermal coupling between the two reactions (I) and (III) [0017].
Reytier discloses another aim of the process is to propose a process and a reactor for production of a synthesis gas, to achieve the aforementioned aim and obtain a variable H2/CO ratio [0032].
Reytier discloses an advantageous embodiment, the hydrogen produced and recovered in the third or alternatively the fourth openings is mixed at the outlet of the electrolysis reactor with the carbon monoxide produced and recovered in the fourth or alternatively the third openings, to produce a synthesis gas with a view to performing either a synthesis according to the Fischer-Tropsch process followed by hydrocracking to produce liquid fuel of the diesel or kerosene type, or synthesis of methane, or synthesis of methanol, or synthesis of dimethyl ether (DME) [0066].
Reytier in FIGS. 10A and 10B show curves representing the polarization (voltage change as a function of applied current) of a known cathode-supported electrolysis cell (CSC), at a temperature of 800° C., under carbon dioxide CO2 at inlet and under steam H2O at inlet, respectively [0100].
Reytier teaches that all the electrolyzers described are of the type with solid oxides (SOEC, acronym of “Solid Oxide Electrolyte Cell”) operating at high temperature. Thus, all the constituents (anode/electrolyte/cathode) of an electrolysis cell are ceramics. The high operating temperature of an electrolyzer (electrolysis reactor) is typically between 600° C. and 1000° C [0106].
FIG. 3 of Reytier shows schematically a high-temperature solid oxide electrolyzer (SOEC) according to the invention, allowing within it simultaneous electrolysis of steam and carbon dioxide, each electrolysis taking place separately in one of the elementary electrolysis cells [0133].
FIGS. 10A and 10B of Reytier illustrate the polarization curves obtained in electrolysis of carbon dioxide and of water, respectively. It is to be noted that the cathode-supported electrolysis cell on which the simulations were performed is at a temperature of 800° C. It is also to be noted that the CO2/CO ratio at cell inlet was 90/10 (FIG. 10A), just like the H2O/H2 ratio at cell inlet (FIG. 10B) [0202].
The claimed invention differs from Reytier because the present claims require a CO/CO2 molar ratio in the feed stream strictly within the range of 0.2-0.6, whereas Reytier explicitly discloses the CO2/CO ratio at the inlet cell is maintained at 90/10.
A person having ordinary skill in the art, prior to the effective filing date of the claimed invention looking to build an integrated system would easily bridge the gap and arrive at the claimed invention by combining the teachings of Reytier and Makoto’s specific emphasis on producing liquid methanol through combining , compressing and cooling the synthesis gas and synthesizing methanol at 2500C [0047], The PHOSITA would naturally look to optimize the upstream gas feed composition to maximize chemical reaction efficiency. To achieve the required carbon stoichiometric for optimal 250 0C methanol conversion, the PHOSITA turn to Reytier, who explicitly teaches the performing separate electrolysis provides great flexibility in the management of the H2/CO mixture. Guided by Reytier’s teaching of total operation flexibility, the PHOSITA would view Reytier’s baseline 90/10 ratio merely as a starting point. Adjusting this result-effective variable upward into the claimed 0.2-0.6 CO/CO2 range would represent routine optimization and standard engineering practice to fulfill the precise downstream feed requirements outlined by Makoto.
Reytier is silent with respect to removing the impurities from the feed gas, electrolysis unit for producing H2 is alkaline/polymer electrolyte membrane and electric power required in electrolysis is provided by renewable sources. However, Makoto teaches it is necessary to purify the raw materials by removing sulfur, for example, by supplying them to a desulfurizer, or by removing other impurities using other separation means [0004].
Makoto teaches a methanol synthesis system comprising: a power generation device that generates electricity using renewable energy; a steam electrolysis device to which electricity generated by the power generation device and thermal energy derived from renewable energy are supplied, and which electrolyzes steam at high temperature to produce hydrogen; a carbon dioxide electrolysis device to which electricity generated by the power generation device and thermal energy derived from renewable energy are supplied, and which electrolyzes carbon dioxide at high temperature to produce carbon monoxide; and a methanol synthesis device to which hydrogen produced in the steam electrolysis device and carbon monoxide produced in the carbon dioxide electrolysis device are supplied, and which performs methanol synthesis [0010].
Makoto teaches In addition, other renewable energy sources that can supply electricity through power generation, such as wind power, hydropower, tidal power, wave power, and ocean currents, may also be used [0026].
Makoto teaches the separation membrane 4 is a type of separation means, and is a membrane used to separate carbon dioxide contained in exhaust gas discharged from a factory. The separation membrane 4 is not particularly limited as long as it is a membrane capable of separating carbon dioxide, and examples include organic polymer membranes, inorganic material membranes, organic polymer-inorganic material composite membranes, and liquid membranes [0038].
Makoto teaches the steam electrolysis apparatus 2 is an electrolysis apparatus that includes a solid oxide type electrolytic cell (SOEC) which contains a cathode and an anode arranged on both sides with a solid oxide electrolyte as an intermediate layer [0030].
Furthermore, impurities such as water and higher alcohols are removed from methanol by distillation to obtain high-purity methanol of a certain concentration or higher [0006].
Reytier lacks teaching for feed gas impurity removal, the use of alkaline or PEM electrrolyzer for water electrolysis, and the application of renewable energy for CO2 reduction, which are all disclosed by Makoto. A person having ordinary skill in the art, prior to the effective filing date of the claimed invention would modify Reytier aby adopting Makoto’s purification, selecting high-efficiency PEM/alkaline technologies, and integrating renewable power to optimize performance and meet sustainability standard.
The claimed process differs from the prior art because it requires a feed stream with a high CO/CO2 molar ratio of 0.8 or higher to produce a hydrocarbon product. Reytier explicitly teaches a baseline feed mixture with a low CO/CO2 ratio of 90/10 (0.11 CO/CO2), but notes in paragraph 0066 that this syngas can be utilized via F-T hydrocarbon process to generate hydrocarbon products. However, while a low ratio suffices for the methanol synthesis focused on by Makoto, A F-T hydrocarbon process generates a massive volume of byproduct water that triggers the reverse water-gas shift side reaction, which aggressively consumes CO and floods the system unwanted CO2. Therefore, to synthesize hydrocarbons via Reytier’s F-T process rather than Makoto methanol pathway, the initial CO/CO2 ratio must be drastically increased to 0.8 or higher to counteract this thermodynamic shift and ensure enough carbon monoxide remains available to drive hydrocarbon chain growth.
A person having ordinary skill in the art, before the effective filing date of the claimed invention, looking to optimize Reytier’s F-T process would turn to Makoto’s method of combining and compressing the gases into downstream reactor. However, for producing hydrocarbon via F-T process requires low hydrogen to carbon monoxide (2/1 or lower) for hydrocarbon chain growth. In contrast, the methanol synthesis requires higher hydrogen to carbon monoxide (3/1). Therefore, it is well within the purview of one ordinary skill in the art to leverage the flexibility taught by Reytier in the managing the H2/CO mixture via a separate electrolysis, routinely optimizing the gas feed ratios to obtain a composition suitable for downstream hydrocarbon production.
Any inquiry concerning this communication or earlier communications from the examiner should be directed to JAFAR F PARSA whose telephone number is (571)272-0643. The examiner can normally be reached M-F 10:00 AM-6:30PM.
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/JAFAR F PARSA/Primary Examiner, Art Unit 1692
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