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 .
Claim Rejections - 35 USC § 102
The following is a quotation of the appropriate paragraphs of 35 U.S.C. 102 that form the basis for the rejections under this section made in this Office action:
A person shall be entitled to a patent unless –
(a)(1) the claimed invention was patented, described in a printed publication, or in public use, on sale, or otherwise available to the public before the effective filing date of the claimed invention.
Claim(s) 1-4, 7-9, 11 and 13 is/are rejected under 35 U.S.C. 102(a)(1) as being anticipated by WO’2022/073071.
Regarding claims 1 and 2, WO’3071 teaches N2 oxidation in plasma and then converting the NOx from the oxidation step to ammonia in another electrocatalytic unit (Pg. 3, lines 5-8). The reference teaches using water to oxidize N2 into NOx before electrocatalytically reducing said NOx to provide ammonia (Pg. 4, lines 35-40). This water would be expected to be vapor or steam in the plasma environment.
Regarding claims 3 and 4, WO’3071 teaches that the oxidation is performed by contact with oxygen or air (Pg. 5, line 5). Air would be expected to have some carbon dioxide. Air is well known to have a non-zero amount of CO2.
Regarding claim 7, the reference specifies a dielectric barrier discharge reactor (Pg. 21, line 5).
Regarding claims 8 and 9, the WO’3071 reference highlights the superior performance of Cu nanowires (Pg. 25, line 25-27).
Regarding claim 11, the WO’3071 teaches using a packed bed with monoliths (Pg. 3, line 33).
Regarding claim 13, WO’3071 teaches using atmospheric pressure (Pg. 9, line 37).
Regarding claim 15, the WO’3071 teaches a step where the formed ammonia is desorbed from the catalyst after the adsorbed NOx is converted on the catalyst (Pg. 24, lines 11). This indicates that a part of the catalyst has an ammonia adsorbent.
Claim(s) 1, 3, 4, 7 and 13 is/are rejected under 35 U.S.C. 102(a)(1) as being anticipated by Hollevoet et al. “Towards Green Ammonia Synthesis through Plasma-Driven Nitrogen Oxidation and Catalytic Reduction”.
Regarding claims 1 and 7, Hollevoet et al. teaches oxidation of N2 in a plasma reactor where it is converted to NO and then to NO2 (Pg. #23826, right hand column, last para). The NOx mixture is then fed with H2 to perform reduction of NOx to NH3 on Pt/BaO based catalyst (Pg. #23826, right hand column, last para). This reduction of NOx in the presence of hydrogen to ammonia is considered to read on the hydrogenating step. An arc discharge reactor is taught (Pg. 23826, left hand column, 3rd para).
Regarding claims 3 and 4, Hollevoet et al. teaches that the oxidation is performed by contact with oxygen or air (Pg. #23826, right hand column, last para). Air would be expected to have some carbon dioxide. Air is well known to have a non-zero amount of CO2.
Regarding claim 13, Hollevoet et al. teaches using a gliding arc plasma reactor operated at atmospheric pressure (Pg. 23826 , right hand column, first para).
Claim Rejections - 35 USC § 103
The following is a quotation of 35 U.S.C. 103 which forms the basis for all obviousness rejections set forth in this Office action:
A patent for a claimed invention may not be obtained, notwithstanding that the claimed invention is not identically disclosed as set forth in section 102, if the differences between the claimed invention and the prior art are such that the claimed invention as a whole would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to which the claimed invention pertains. Patentability shall not be negated by the manner in which the invention was made.
Claim(s) 2 and 5 is/are rejected under 35 U.S.C. 103 as being unpatentable over Hollevoet et al. “Towards Green Ammonia Synthesis…”, in view of Caldwell US 20230142620.
Regarding claim 2, the Hollevoet et al. reference does not teach using steam for the N2 oxidation step in the plasma discharge reactor.
Caldwell teaches ammonia production in a microjet plasma unit (Abstract). The reference identifies a detrimental issue emanating from too much oxygen in the air creating disproportionate amounts of NOx species in the plasma jet (Para [0166]). The reference teaches that adding water vapor to the nitrogen plasma will increase the production rate of NH3 and also produces NOx species (Para [0173]).
Before the effective filing date of the claimed invention, it would have been obvious for a person of ordinary level of skill in the art to use water vapor or steam in the process of Hollevoet. The selection of a known material based on its suitability for its intended use supported a prima facie obviousness determination (MPEP §2144.07).
Regarding claim 5, the reference of Hollevoet et al. does not teach using argon in the N2 oxidation step in the plasma discharge reactor.
Caldwell teaches that introduction of inert diluent gasses, such as argon, that can modulate plasma discharge efficiency (Para [00232]).
Before the effective filing date of the claimed invention, it would have been obvious for a person of ordinary level of skill in the art to use argon in the plasma reactor of Hollevoet in the N2 oxidation step. One would be motivated to do so to modulate plasma discharge efficiency, as taught by Caldwell.
Claim(s) 14 and 16 is/are rejected under 35 U.S.C. 103 as being unpatentable over Hollevoet et al. “Towards Green Ammonia Synthesis…”,
Regarding claim 14, Before the effective filing date of the claimed invention it would have been within the skill of a person of ordinary level of skill in the art to determine a suitable or optimal flow rate within the reactor. The flow rate of nitrogen or air would directly corelate to the conversion rate or ammonia formation rate. Thus, this is an effective variable which can be optimized without undue experimentation.
Regarding claim 16, the Hollevoet et al. reference is silent on whether the process is adiabatic. No external heating is taught to be supplied to the catalyst.
Before the effective filing date of the claimed invention, it would have been obvious for a person or ordinary level of skill in the art to us an adiabatic process for the conversion in the process of Hollevoet. One would be motivated to do so to make the process more energy efficient. The reference highlights concerns regarding conversing energy and monitoring consumption in the plasma reactor (Pg. 23828, left hand column, 2nd para). The reference aims to be more efficient by using heat exchangers to recover waste heat (Pg. 23828).
Claim(s) 5 is/are rejected under 35 U.S.C. 103 as being unpatentable over WO 2022/073071, in view of Caldwell US 20230142620.
Regarding claim 5, the reference of WO’3071 does not teach using argon in the N2 oxidation step in the plasma discharge reactor.
Caldwell teaches that introduction of inert diluent gasses, such as argon, that can modulate plasma discharge efficiency (Para [00232]).
Before the effective filing date of the claimed inventiinvention,ld have been obvious for a person of ordinary level of skill in the art to use argon in the plasma reactor of WO’2620 in the N2 oxidation step. One would be motivated to do so to modulate plasma discharge efficiency, as taught by Caldwell.
Claim(s) 10, 14 and 16 is/are rejected under 35 U.S.C. 103 as being unpatentable over WO 2022/073071.
Regarding claim 10 the reference broadly teaches using a transitional metal catalyst such as copper, nickel , iron, cobalt or titanium (See WO’3071 claim 30) and using a nanostructured or nanoparticulate catalyst (See WO’3071 claim 31). Among other metals, copper and nickel are preferred (Pg. 13, line 17).
Before the effective filing date, it would have been obvious for a person of ordinary level of skill in the art to use iron nanowires or nickel nanoparticulate. One would be selecting from a closed group of well-defined options (MPEP §2141 III E).
Regarding claim 14, Before the effective filing date of the claimed invention it would have been within the skill of a person of ordinary level of skill in the art to determine a suitable or optimal flow rate within the reactor. The flow rate of nitrogen would directly corelate to the conversion rate or ammonia formation rate. Thus this is a result effective variable which can be optimized without undue experimentation.
Regarding claim 16, the WO’3071 reference is silent on whether the process is adiabatic. No external heating is taught to be supplied to the catalyst.
Before the effective filing date of the claimed invention it would have been obvious for a person or ordinary level of skill in the art to us an adiabatic process for the conversion in the process of WO’3071. One would be motivated to do so to make the process more energy efficient. The reference focuses on improving thermal efficiency and uses room temperature cold plasma (Pg. 12, lines 6-9). Combining two forms of discharges within a single unit made efficient utilization of power minimizing energy losses (Pg. 12, lines 28-29).
Claim(s) 12 is/are rejected under 35 U.S.C. 103 as being unpatentable over WO 2022/073071, in view of Goldberger US3404078.
Regarding claim 12, the WO’3071 reference does not teach using a fluidized catalytic bed with the catalyst being of a size of 10mm to 10mm.
Goldberger teaches a plasma arc unit with a fluidized bed for performing heating processes (Col. 1, lines 13-23). The reference teaches a bed of electrically conductive fluidized particles as an integral electrical part of the plasma generator. This permits direct contact of the plasma with the fluidized particles. As a result, the plasma is not subject to energy losses which might otherwise occur (Col. 5, lines 42-48). The reference uses a particles size of 65 mesh (or 0.23 mm) (See Col. 7, line 7).
Before the effective filing date of the claimed invention it would have been obvious for a person of ordinary level of skill in the art to use a fluidized bed as taught by Goldberger, for the plasma reactor of WO’3071. One would be motivated to do so to take advantage of the high surface area of contact between solid particles and gases.
Allowable Subject Matter
Claim 17 is allowed.
Claim 6 is objected to as being dependent upon a rejected base claim, but would be allowable if rewritten in independent form including all of the limitations of the base claim and any intervening claims.
The following is a statement of reasons for the indication of allowable subject matter for claim 6 and reasons for allowance for claim 17:
Claim 6 requires “The method of claim 1, wherein the hydrogenating step is performed by introducing H2 at a position above a plasma flame in the plasma discharge reactor.”
Claim 17 requires “A method for producing ammonia, comprising: providing a plasma discharge reactor with a fixed or fluidized catalyst bed; introducing N2 gas and an oxidizing agent into a plasma flame of the plasma discharge reactor; introducing hydrogen at a position above the plasma flame over catalyst to produce ammonia; and collecting the ammonia produced.”
There is no teaching or suggestion from the Hollevoet reference or the WO’3071 reference regarding “…introducing hydrogen at a position above a plasma flame…”.
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to SYED TAHA IQBAL whose telephone number is (571)270-5857. The examiner can normally be reached M-F; 7-5.
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/SYED T IQBAL/ Examiner, Art Unit 1736
/ANTHONY J ZIMMER/Supervisory Patent Examiner, Art Unit 1736