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 .
Status of the Claims
The amendment filed on 10/20/2025 has been entered. Claim 1 has been amended and thus claims 1-5, 7-8, 15 and 17-24 are currently pending; claims 7-8 have been withdrawn from further consideration; and claims 1-5, 15 and 17-24 are under current examination.
Withdrawn Rejection
Claim 1 has been amended by reciting “wherein the reactor employs steam cooling to remove heat from the reactor produced by an exothermic catalyst reaction and operates at an hourly space velocity of 1750 to 3,000 GHSV in step (b). While, the combination of Schuetzle (Schuetzle, R. et al. Patent application publication number US2014/0250770A1; cited in Office Action 09/11/2020) in view of Ayasse (Ayasse, C. Patent number US8,053,481B2; cited in IDS 04/21/2025 and 04/22/2025), Van Hardeveld (Van Hardeveld, R. M. et al. Patent number US7,846,325B2; cited in Office Action 09/29/2023), Koveal (Koveal, R. J. et al. Patent number US6,107,353; cited in Office Action 09/29/2023) and Floudas (Floudas, C. A. et al. Patent application publication number US2015/0073188A1; cited in Office Action 10/07/2020) teaches the GHSV range, it fails to teach or suggest that the reactor employs steam cooling to remove heat from the reactor produced by an exothermic catalyst reaction. Accordingly, the 103 rejection of the record has been withdrawn.
Claim Objections
Claim 1 is objected to because of the following informalities: the unit for the hourly space velocity is missing from the claim. Appropriate correction is required.
Response to Remarks
Applicant argues that the amendment includes hourly space velocity units GHSV, which is not persuasive. GHSV is just an abbreviation for gas hourly space velocity and does not represent a unit. The hourly space velocity can be measured in Nml/g.hr, m³/m³.hr, Nl/l/h, h-1, NmL·h−1·gcat−1, etc.
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 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.
Claims 1, 3-4, 15, 18-21 and 24 are newly rejected under 35 U.S.C. 103 as being unpatentable over Schuetzle (Schuetzle, R. et al. Patent application publication number US2014/0250770A1; cited in Office Action 09/11/2020) in view of Boer (Boer, A. et al. Patent application publication number US2007/0053807A1), Van Hardeveld (Van Hardeveld, R. M. et al. Patent number US7,846,325B2; cited in Office Action 09/29/2023), Koveal (Koveal, R. J. et al. Patent number US6,107,353; cited in Office Action 09/29/2023) and Floudas (Floudas, C. A. et al. Patent application publication number US2015/0073188A1; cited in Office Action 10/07/2020).
Schuetzle teaches a process for producing two or more fuel products from gas- phase hydrocarbon feedstocks which may be natural gas, natural gas liquids, or combinations thereof ([0032]).
Regarding claims 1(a) and 4, Schuetzle teaches that the process comprises producing syngas from the aforementioned gas-phase hydrocarbon feedstocks using a steam reformer ([0059]), wherein the syngas has a H2/CO ratio of about 2.05:1.0 ([0086]).
Regarding claim 1 b)-c), Schuetzle further teaches converting syngas into fuels using a catalytic reactor comprising a single pass or two or more horizontal reactors that are connected in series (Fig. 1 and [0050]), wherein the catalytic reactor comprises a catalyst for the direct conversion of the syngas into liquid fuels, wherein diesel fuels (equivalent to liquid fuel), water, wax and light hydrocarbon gases and unreacted CO and H2 (the last two also known to a skilled artisan as tail gas) are produced ([0086]-[0087]). Schuetzle teaches that the catalyst comprises support such as gamma alumina ([0034]) which is a substrate that has a surface ([0038]). Schuetzle is silent about the alumina as having a surface with a pH ranging from 6.75 to 7.25. However, the instant specification uses the same gamma alumina substrate in the catalyst (page 11, 3rd paragraph) as in Schuetzle, and thus it is anticipated for the alumina of Schuetzle to have a surface with a pH ranging from 6.75 to 7.25. The reference further teaches that syngas is subjected to cleanup to obtain syngas free of impurities such as sulfur, ammonia and any known contaminants that result from a syngas production ([0060]). Schuetzle also teaches that the catalytic reactor is operated in a pressure range of about 100 psi to about 400 psi, ideally at 150 psi in a temperature range of about 350° F. to about 600° F., preferably at 425° F ([0092]).
Schuetzle is silent about the catalyst producing levels of carboxylic acids in the fuels and catalyst reaction water below 25 ppm. However, since Schuetzle teaches the same claimed process steps of (a)-(b), there is a prima facie case of either anticipation or obviousness in the reference for the catalyst in producing levels of carboxylic acids in the fuels and catalyst reaction water below 25 ppm. In fact, the instant specification describes that the direct fuel production catalyst produces reaction water that contains undetectable or barely detectable deleterious carboxylic acids (page 9), and thus, Schuetzle’s catalyst, which is as instantly claimed, would also produces fuels directly from syngas. As such, the product fuels of the reference would contain the same or carboxylic acid as claimed.
Furthermore, Schuetzle teaches that wax and water are separated in a single knock out vessel from the diesel fuel and light hydrocarbon gases and unreacted CO and H2 (0087). It is noted that a skilled artisan would not have a reasonable expectation for such separation to obstruct the syngas flow. Furthermore, Schuetzle teaches that a fraction water comprising wax ([0062]) after separation is recycled directly to the syngas generation unit ([0064]) (see also Fig. 1). Schuetzle also teaches in [0022]-[0024] that a variety of catalyst parameters allow for efficient operation, such as support material and size, shape, pore diameter, surface area, crush strength and pellet radius of the support material and a unique combination of the parameters produces the unique product. Schuetzle further teaches in [0025] that variations of these parameters have dramatic effect on product distribution, i.e. by finding the optimal support, metals loading, crystalline size, pore diameter, surface area, crush strength, and effective pellet radius of a supported catalyst can change the product distribution. Hence, since the ultimate goal in Schuetzle is to obtain diesel fuel comprising a majority of hydrocarbons in the C8-C24 range ([0020]) and since the Fischer-Tropsch process produces light gases and wax in addition to diesel fuel ([0061]), a skilled artisan would have been motivated to control the operating conditions and catalytic parameters taught by the reference, with a reasonable expectation of success in efficiently obtaining diesel fuel. Furthermore, Schuetzle teaches in [0077] the operating Fischer-Tropsch conditions that are selected to achieve the desired selectivity of diesel fuel, i.e. keeping the reactor at a pressure between 150 psi and 450 psi, and at a temperature between about 350 F and 460 F. Hence a skilled artisan would have been motivated to vary the operating Fischer-Tropsch conditions to the temperature range and pressure range of Schuetzle to produce diesel fuel.
Regarding claim 3, it is known to a skilled artisan that the feedstock of Schuetzle comprising natural gas or natural gas liquids necessarily comprises the claimed normal alkanes, is-alkanes, olefins, alcohols, ketones, aldehydes and aromatic hydrocarbons.
Regarding claim 15, Schuetzle is silent about the claimed conversion of the CO in the syngas into hydrocarbons. However, Schuetzle teaches the same process steps as instantly claimed to obtain diesel fuel from syngas and thus, there is a prima facie case of obviousness or anticipation in the reference for more than about 85 volume % of the CO is converted into hydrocarbons.
Regarding Claims 18, 20 and 21, since Schuetzle teaches the same reaction steps as claim 1, there is a prima facie case of obviousness or anticipation for the liquid fuels in Schuetzle to demonstrate the claimed ASTM D130 copper strip corrosion ratings and for the catalyst reaction water to contain the claimed composition.
Regarding claim 19, Schuetzle teaches that wax is formed in the liquid fuels product ([0017]) and because Schuetzle teaches the same reaction steps as instantly claimed, the wax product in Schuetzle would necessarily form at an amount of less than 5 weight percent of the combination of liquid fuels and wax
Regarding Claim 24, Schuetzle teaches that the produced liquid fuels are suitable for sale into the market ([0018]).
Regarding claim 1 b), Schuetzle fails to teach that the reactor employs steam cooling to remove heat from the reactor produced by an exothermic catalyst reaction and operates at an hourly space velocity of 1750 to 3,000 GHSV. Furthermore, while Schuetzle teaches that the synthesis gas is subjected to purification process to obtain syngas free of impurities, the reference fails to teach subjecting syngas to a purification process, wherein the purification process is solid-phase process, and wherein the process reduces sulfur compounds and hydrogen cyanide in the syngas to less than 20 ppb and reduces ammonia in the syngas to less than 5 ppm. However, the deficiencies are cured by Boer, Van Hardeveld and Koveal.
Boer teaches the conversion of syngas to fuels in which alumina support is used in the catalyst ([0001] and [0086]). The reference further teaches that the reactor comprises a cooling module comprising coolant to be used in the exothermic reaction reactor ([0001], [0009]-[0011]), wherein suitable coolants include water/steam or oil based coolants ([0061]). The reference teaches that heat control enhances the reactor performance with respect to CO conversion and product selectivity ([0006]). Thus, a skilled artisan would have been motivated to use steam cooling in the reactor of Schuetzle with a reasonable expectation of success in cooling the exothermic reaction and in improving CO conversion and product selectivity.
The reference further teaches that the gaseous hourly space velocity may vary within wide ranges and is typically in the range from 1500 to 10000 Nl/l/h ([0093]). Accordingly, using the GHSV of Boer in the process of Schuetzle would still have a reasonable expectation of success in converting syngas to fuels.
Van Hardeveld teaches a method for removing sulfur containing compounds by the use of solid adsorbent to obtain syngas having sulfur compounds at a concentration of below 5 ppbv (col. 2, ll. 35-58).
Furthermore, Koveal also teaches method of purifying syngas by the use of solid adsorbent to reduce the combined total of HCN and ammonia to less than 50 vppb (col. 2, ll. 1-67).
Accordingly, a skilled artisan would have been motivated to use the methods of Van Hardeveld and Koveal in Schuetzle with a reasonable expectation of success of purifying the synthesis gas from sulfur compounds, HCN and ammonia.
Regarding claim 1 step (d), while Schuetzle teaches the separation of water from the diesel fuels, Schuetzle fails to teach distilling the diesel fuels. The deficiency is cured by Floudas.
Floudas teaches the production of synthetic hydrocarbons from natural gas by first steam reforming natural gas followed by Fischer-Tropsch process. Furthermore, Floudas teaches that the synthetic hydrocarbons are further converted to the desired fuel composition via distillation followed by additional upgrading ([0095]). Accordingly, a skilled artisan would have been motivated to use the distillation and upgrading process of Floudas in the process of Schuetzle with a reasonable expectation of success in obtaining the desired fuel composition from the hydrocarbons of Schuetzle.
It would thus have been prima facie obvious to a skilled artisan before the effective filing date of the instantly claimed invention to conduct the claimed process for producing two or more fuel products from gas-phase hydrocarbon feedstock using the claimed steps (a)-(d) in view of the combination of Schuetzle, Boer, Van Hardeveld, Koveal and Floudas.
Response to Arguments
Applicant amends claim 1 and argues that the cited references do not discuss/report the element of the amended claims. The argument is mute in view of the new ground of rejection that addresses amended claim 1.
Claims 2 and 22 are newly rejected under 35 U.S.C. 103 as being unpatentable over Schuetzle (Schuetzle, R. et al. Patent application publication number US2014/0250770A1; cited in Office Action 09/11/2020) in view of Boer (Boer, A. et al. Patent application publication number US2007/0053807A1), Van Hardeveld (Van Hardeveld, R. M. et al. Patent number US7,846,325B2), Koveal (Koveal, R. J. et al. Patent number US6,107,353) and Floudas (Floudas, C. A. et al. Patent application publication number US2015/0073188A1; cited in Office Action 10/07/2020) as applied to claims 1, 3-4, 15, 18-21 and 24 above, and further in view of Chlapik (Chlapik, K. et al. Patent application publication number US2016/0347613A1; Effectively filed on Mar. 4, 2014; cited in Office Action 09/11/2020).
The teachings of Schuetzle, Boer, Van Hardeveld, Koveal and Floudas have been set forth above.
Regarding claim 2, the combination of Schuetzle, Boer, Van Hardeveld, Koveal and Floudas fails to teach or suggest that the that the steam reformer is a catalytic steam-reforming process, and wherein the syngas has a H2/CO ratio in the range of about 2.0-3.3, and wherein the process for producing syngas has a conversion efficiency of better than about 90% at temperatures below about 1700° F., and wherein the catalyst is a steam reforming, structured catalyst. However, Chlapik teaches that the steam reformer of natural gas is a catalytic steam reformer with structured catalyst ([0007]-[0010] and [0027]). Furthermore, Chlapik teaches that the maximum reaction temperature is 917 ºC (Table in [0041]), which is equivalent to 1682.6 F. Thus, the claimed H2/CO and better than about 90% conversion efficiency are necessarily produced in Chlapik because the reference teaches the same claimed catalytic steam reformer, reforming temperature and structured catalyst.
Chlapik teaches that the structured catalyst results in maximum performance and increases catalyst lifetime at high temperatures ([0006]). Thus, a skilled artisan would have been motivated to use the catalyst of Chlapik in the steam reforming process of Schuetzle and Floudas with a reasonable expectation of success in increasing the steam reforming performance and catalyst lifetime.
Regarding claim 22, Chlapik teaches that a steam ratio over the natural gas of 3.0 has been used in the steam reforming process ([0040]). Thus, a skilled artisan would have been motivated to adjust the amount of the recycled catalyst reactor water of Schuetzle and Floudas to obtain a steam to carbon ratio in the steam reformer to 3.0.
It would thus have been prima facie obvious to a skilled artisan before the effective filing date of the instantly claimed invention to conduct the claimed process for producing two or more fuel products from gas-phase hydrocarbon feedstock using the claimed steps (a)-(d), wherein the process for producing syngas from gas-phase hydrocarbon feedstocks is a catalytic steam-reforming process, and wherein the syngas has a H2/CO ratio in the range of about 2.0-3.3, and wherein the process for producing syngas has a conversion efficiency of better than about 90% at temperatures below about 1700° F., wherein the catalyst is a steam reforming, structured catalyst, and wherein the recycled catalyst reaction water is used to adjust the water to carbon mass ratio in the syngas generator to between about 1.5/1.0 and 3.0/1.0 in view of the combination of Schuetzle, Boer, Van Hardeveld, Koveal, Floudas and Chlapik.
Claims 5 is newly rejected under 35 U.S.C. 103 as being unpatentable over Schuetzle (Schuetzle, R. et al. Patent application publication number US2014/0250770A1; cited in Office Action 09/11/2020) in view of Boer (Boer, A. et al. Patent application publication number US2007/0053807A1), Van Hardeveld (Van Hardeveld, R. M. et al. Patent number US7,846,325B2; cited in Office Action 09/29/2023), Koveal (Koveal, R. J. et al. Patent number US6,107,353; cited in Office Action 09/29/2023) and Floudas (Floudas, C. A. et al. Patent application publication number US2015/0073188A1; cited in Office Action 10/07/2020) as applied to Claims 1, 3-4, 15, 18-21 and 24 above, and further in view of Silvey (Silvey, L. G. “Hydrogen and Syngas Production from Biodiesel Derived Crude Glycerol”, 2011, pp. 1-127; cited in Office Action 09/11/2020).
The teachings of Schuetzle, Boer, Van Hardeveld, Koveal and Floudas have been set forth above.
Regarding claim 5, the combination of Schuetzle, Boer, Van Hardeveld, Koveal and Floudas fails to teach or suggest the use of vaporized liquid by-products from chemical processes. However, Silvey teaches that glycerol is a by-product for the production of biodiesel (Abstract, page iii, 1st paragraph). Silvey teaches that glycerol is converted into a syngas using steam reformer (Abstract, page iii, 2nd paragraph; Eqn. 2, page 21) by first vaporizing the liquid reactant (equivalent to glycerol; page 32, last paragraph).
Silvey teaches that increase in the production of biodiesel also produces glycerol by-products and that steam reforming crude glycerol instead of disposing it, and that the mixed gas obtained from the steam reforming can be used in the production of diesel fuel via a Fischer-Tropsch process (Abstract, page iii, 1st paragraph). Thus, a skilled artisan would have been motivated to use the feedstock of Silvey in place of the feedstock of Schuetzle and Floudas with a reasonable expectation of success in effectively using glycerol byproduct in the production of useful products such as diesel fuel.
It would thus have been prima facie obvious to a skilled artisan before the effective filing date of the instantly claimed invention to conduct the claimed process for producing two or more fuel products from gas-phase hydrocarbon feedstock using the claimed steps (a)-(d), wherein the gas-phase hydrocarbon feedstocks comprise vaporized liquid by-products from chemical processes in view of the combination of Schuetzle, Boer, Van Hardeveld, Koveal, Floudas and Silvey.
Claims 17 is newly rejected under 35 U.S.C. 103 as being unpatentable over Schuetzle (Schuetzle, R. et al. Patent application publication number US2014/0250770A1; cited in Office Action 09/11/2020) in view of Boer (Boer, A. et al. Patent application publication number US2007/0053807A1), Van Hardeveld (Van Hardeveld, R. M. et al. Patent number US7,846,325B2; cited in Office Action 09/29/2023), Koveal (Koveal, R. J. et al. Patent number US6,107,353; cited in Office Action 09/29/2023) and Floudas (Floudas, C. A. et al. Patent application publication number US2015/0073188A1; cited in Office Action 10/07/2020) as applied to Claims 1, 3-4, 15, 18-21 and 24 above, and further in view of Bracht (Bracht, M. et al. Patent application publication number US2010/0184873A1; cited in Office Action 09/11/2020).
The teachings of Schuetzle, Boer, Van Hardeveld, Koveal and Floudas have been set forth above. However, the combination of Schuetzle, Boer, Van Hardeveld, Koveal and Floudas fails to teach the limitations of claim 17.
These deficiencies are cured by Bracht. Bracht teaches the use of a first, second, third and later stage reactor for Fischer-Tropsch process ([0033]-[0034]). Bracht teaches that the first stage comprises the following conditions:
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Bracht teaches that the CO conversion in the first stage is preferably 30-50% ([0042]).
Furthermore, Bracht teaches that the second stage comprises the following conditions:
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Bracht teaches that the CO conversion in the second stage is preferably 25-70% ([0054]). Bracht further teaches that the gaseous effluent from the second stage is conveyed to the third stage and thus a skilled artisan would have a reasonable expectation to result in CO conversion higher than the second stage.
Bracht teaches that such multi stage process in the Fischer-Tropsch process results in high conversion of CO and high selectivity of C5+ ([0026]) and allows the use of syngas with a relatively low hydrogen/CO ratio ([0028]). Accordingly, a skilled artisan would have been motivated to use the multistage reactors and reaction conditions of Bracht in the process of the combination of Schuetzle and Floudas with a reasonable expectation of success of increasing CO conversion, C5+ selectivity and usage of low hydrogen/CO ratio.
It would thus have been prima facie obvious to a skilled artisan before the effective filing date of the instantly claimed invention to conduct the claimed process for producing two or more fuel products from gas-phase hydrocarbon feedstock using the claimed steps (a)-(d), wherein the catalytic reactor is operated under conditions of temperature, pressure and space velocity such that greater than about 25% of the CO in the syngas is converted to fuels in a first horizontal or vertical reactor and the primary remaining CO is transferred to a second horizontal or vertical reactor, and wherein greater than about 40% of the remaining CO in the second horizontal or vertical reactor is converted to fuels and secondary remaining CO, and wherein the secondary remaining CO is transferred to a third horizontal or vertical reactor, and wherein greater than about 55% of the secondary remaining CO is converted to fuels in view of the combination of Schuetzle, Boer, Van Hardeveld, Koveal, Floudas and Bracht.
Claim 23 is newly rejected under 35 U.S.C. 103 as being unpatentable over Schuetzle (Schuetzle, R. et al. Patent application publication number US2014/0250770A1; cited in Office Action 09/11/2020) in view of Boer (Boer, A. et al. Patent application publication number US2007/0053807A1), Van Hardeveld (Van Hardeveld, R. M. et al. Patent number US7,846,325B2), Koveal (Koveal, R. J. et al. Patent number US6,107,353) and Floudas (Floudas, C. A. et al. Patent application publication number US2015/0073188A1; cited in Office Action 10/07/2020) as applied to Claims 1, 3-4, 15, 18-21 and 24 above, and further in view of Herrmann (Herrmann, R. P. et al. Patent application publication number US2014/0213669A1; cited in IDS 06/04/2019).
While Schuetzle teaches recycling of catalyst reaction water to the syngas generator (steam reformer), nowhere in Schuetzle, Boer, Van Hardeveld, Koveal or Floudas teaches or suggests injecting a part of catalyst reaction reactor into oil wells.
However, Hermann teaches in the abstract injecting catalyst reaction water of a Fischer-Tropsch process into oil wells (water flowing from the bottom into the producing well) which necessarily increases the production of additional oil. Accordingly, a skilled artisan would have been motivated to modify the methods of Schuetzle and Floudas in providing a second part of the catalyst reaction water to inject into oil wells for increasing the production of additional oil as taught by Herrmann, in order to provide synthetic hydrocarbon related products to gas lift tubing arrangement or production well.
It would thus have been prima facie obvious to a skilled artisan before the effective filing date of the instantly claimed invention to conduct the claimed process for producing two or more fuel products from gas-phase hydrocarbon feedstock using the claimed steps (a)-(d), wherein a first part of the catalyst reaction water is recycled, and wherein a second part of the catalyst reaction water is injected into an oil well for increasing the production of oil in view of the combination of Schuetzle, Boer, Van Hardeveld, Koveal, Floudas and Herrmann.
Conclusion
Claims 1-5, 15 and 17-24 are rejected and no claims are allowed.
THIS ACTION IS MADE FINAL. Applicant is reminded of the extension of time policy as set forth in 37 CFR 1.136(a).
A shortened statutory period for reply to this final action is set to expire THREE MONTHS from the mailing date of this action. In the event a first reply is filed within TWO MONTHS of the mailing date of this final action and the advisory action is not mailed until after the end of the THREE-MONTH shortened statutory period, then the shortened statutory period will expire on the date the advisory action is mailed, and any nonprovisional extension fee (37 CFR 1.17(a)) pursuant to 37 CFR 1.136(a) will be calculated from the mailing date of the advisory action. In no event, however, will the statutory period for reply expire later than SIX MONTHS from the mailing date of this final action.
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/MEDHANIT W BAHTA/Primary Examiner, Art Unit 1692