DETAILED ACTION
Claim 1 is amended.
Claim 3 is cancelled.
Claims 1-2 and 4-12 are pending, with claims 2 and 4 being withdrawn.
Claims 1 and 5-12 are rejected.
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 .
Election/Restrictions
Applicant’s election without traverse of Species (a-ii), claim 3, the limitation of which is cancelled and incorporated in claim 1, in the reply filed on 07/09/2025 is acknowledged.
Claims 2 and 4 are withdrawn from further consideration pursuant to 37 CFR 1.142(b) as being drawn to nonelected species, there being no allowable generic or linking claim. Election was made without traverse in the reply filed on 07/09/2025.
Claim Objections
Claims 1 and 5-12 are objected to because of the following informalities:
Claim 1,
Each of lines 6 and 28, 32-33, 42, it is suggested to amend “the reformer tubes” to “the multitude of reformer tubes”.
Each of lines 11, 13, 17 and 20, it is suggested to amend “the shell tube” to “the outer, pressure-rated shell tube”.
Each of lines 14-15, 18 and 22, it is suggested to amend “the structured catalyst” to “the at least one structured catalyst”.
Each of lines 21 and 23, it is suggested to amend “the gas stream” to “the feed gas stream”.
Line 24, it is suggested to amend “the process comprising” to “the process further comprising”
Line 27, it is suggested to amend “the feed gas” to “the hydrocarbonaceous feed gas”.
Lines 27-28, it is suggested to amend “steam reforming conditions” to “the steam reforming conditions”.
Each of lines 34-35, it is suggested to amend “the reforming flue gas” to “the steam reforming flue gas”.
Line 34, it is suggested to amend “the reformer furnace” to “the burner-heated reformer furnace”.
Line 40, it is suggested to amend “a reforming temperature” to “the reforming temperature”.
Line 41, it is suggested to amend “a steam/carbon ratio” to “the steam/carbon ratio”.
Lines 41-42, it is suggested to amend “a normalized space velocity” to “the normalized space velocity”.
Claim 5,
Each of lines 1-3 and 6, it is suggested to amend “the shell tube” to “the outer, pressure-rated shell tube”.
Lines 2-5, it is suggested to amend “the structured catalyst” to “the at least one structured catalyst”.
Claim 6,
Each of lines 2-3, it is suggested to amend “the shell tubes” to “the outer, pressure-rated shell tube”.
Claim 7,
Line 3, it is suggested to amend “the shell tube” to “the outer, pressure-rated shell tube”.
Claim 8,
Lines 1-2, it is suggested to amend “the reformer tubes” to “the multitude of reformer tubes”.
Each of lines 2-4 and 6-7, it is suggested to amend “the reformer furnace” to “the burner-heated reformer furnace”.
Each of lines 4 and 6, it is suggested to amend “the shell tube” to “the outer, pressure-rated shell tube”.
Claim 9,
Lines 1-2, it is suggested to amend “a multitude of reformer tubes” to “the multitude of reformer tubes”.
Line 2, it is suggested to amend “burners” to “the burners”.
Each of lines 2-3 and 5-6, it is suggested to amend “the reformer furnace” to “the burner-heated reformer furnace”.
Line 4, it is suggested to amend “the reformer tubes” to “the multitude of reformer tubes”.
Claim 10,
Line 3, it is suggested to amend “the reformer tubes” to “the multitude of reformer tubes”.
Claim 11,
Line 2, it is suggested to amend “the reformer tubes” to “the multitude of reformer tubes”.
Line 3, it is suggested to amend “the type of structured catalyst” to “the kind of structured catalyst”.
Claim 12,
Lines 1-2, it is suggested to amend “the structured catalyst(s)” to “the at least one structured catalyst”.
Line 4, it is suggested to amend “the elements” to “the at least one element”.
Appropriate correction is required.
Claim Rejections - 35 USC § 112
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.
Claim 1 and 5-12 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 1 recites the limitation "the burners" in line 7. There is insufficient antecedent basis for this limitation in the claim.
Claims 5-12, which depend on claim 1, are rejected for the same reason.
Claim 5 recites, “essentially” in claim 5. It is unclear if the arrangement is limited to gastight seal. The examiner interprets the arrangement is limited to gastight seal. Clarification is requested.
Claim 10 recites the limitation "the feedstock" in line 2. There is insufficient antecedent basis for this limitation in the claim.
Claim 10 recites, “an extent of at least 50% under steam reforming conditions in the reformer tubes to give the crude synthesis gas product, based on the hydrocarbons present in the feedstock” in lines 2-4. It is unclear what type of ratio the “extent of at least 50%” refers to, e.g., weight ratio, volume ratio, molar ratio, etc. There is no definition of the “ratio” in Specification. The examiner interprets the “extent of at least 50%” being any type of ratio e.g., weight ratio, volume ratio, molar ratio, etc based on the hydrocarbons present in the feedstock . Clarification is requested.
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, 5 and 7-12 are rejected under 35 U.S.C. 103 as being unpatentable over Ulber et al. (US 2019/0275494 A1) (Ulber), as provided in the IDS filed 03/21/2023, in view of Ahmed et al. “Catalytic steam reforming of biogas - Effects of feed composition and operating conditions” (Ahmed), Idaho National Laboratory “Sensitivity of Hydrogen Production via Steam Methane Reforming to High Temperature Gas-Cooled Reactor Outlet Temperature Process Analysis” (INL) and De Vreede (US 2008/0276633 A1) (De Vreede).
Regarding claim 1, Ulber discloses reformer tubes having a structured catalyst (Ulber, Title and Abstract).
Ulber further discloses a process for producing synthesis gas by catalytic steam reforming of hydrocarbon-containing feed under steam reforming conditions using the reformer tubes and a reformer furnace equipped with a plurality of (i.e. in a multitude of) the reformer tubes, where the synthesis gas contains carbon oxides and hydrogen, where the reformer tubes and at least one burner for heating the reformer tube are arranged in an interior space of the reformer furnace (i.e., a burner-heated reformer furnace) in fluid communication with the interior space in respect of the burner flue gases (i.e., a steam reforming flue gas) (Ulber, [0002]-[0003]; [0019]; [0038]).
Ulber further discloses the reformer tubes comprising a reaction chamber A comprising an outer, pressure-bearing (i.e., pressure-rated) casing tube (i.e., shell tube) which is heated from the outside by means of burners, where the feed gas stream, e.g., natural gas, together with reforming steam enter the reaction chamber in the casing tube via an inlet conduit (i.e., an inlet), go through a structured catalyst (i.e., an inlet end) which is catalytically active for steam reforming, and then leave the structured catalyst (i.e., an outlet end), where the partially reacted feed gas (i.e., a crude synthesis gas product stream) stream enters a free space arranged at the closed tube end (i.e., an outlet) of the casing tube (Ulber, [0018]; Fig. 1; [0055]-[0058]).
Ulber further discloses the reformer tubes comprising a heat exchanger tube arranged within the catalyst bed, where the partially reacted feed gas stream that leaves the structured catalyst (i.e., the outlet end) subsequently goes into the inlet end of the heat exchanger tube which is in fluid communication (i.e., in fluid connection) with the gas outlet from the structured packing (i.e., the outlet end of the structured catalyst), and flow through the heat exchanger tube, where the gas stream flowing through the heat exchanger tube releases part of its sensible heat (i.e., in a heat-exchanging relationship) in countercurrent to the catalyst bed and the feed gas stream flowing through it. After flowing through the heat exchanger tube, the synthesis gas product stream enters a collection conduit (i.e., discharged from the shell tube) from the outlet end of the heat exchanger tube, which is in fluid communication (i.e., in fluid connection) with the outlet chamber and an inner tube that represents the connection between the heat exchanger tubes and the collection conduit (Ulber, [0018]; Fig. 1, [0058]; [0061]).
Ulber further discloses the process comprising (a) provision of a feed gas stream containing hydrocarbon-containing feeds (i.e., hydrocarbonaceous feed gas) and addition of reforming steam, (b) catalytic conversion of the feed under steam reforming conditions into a synthesis gas product containing carbon oxides and hydrogen, (c) discharge of the synthesis gas product, characterized in that the catalytic conversion in step (b) is carried out in the reformer tubes (Ulber, [0046]).
Ulber further discloses the reforming steam reforming conditions are the process conditions, in particular temperature, pressure and residence time, which are known per se to a person skilled in the art (Ulber, [0022]).
Ulber does not explicitly disclose the steam reforming conditions comprise a reforming temperature Tref of at least 900°C, a steam/carbon ratio S/C of not more than 2.8 mol/mol and a normalized space velocity of the feed gas stream at the inlet into the reformer tubes between 2 and 5 mN3/(s*mcat3), wherein the specific amount of export steam is between 0 and 0.8 kg of steam per mN3 of hydrogen generated, wherein the steam reforming conditions comprise a reforming temperature Tref of at least 930°C, a steam/carbon ratio S/C of not more than 2.7 mol/mol and a normalized space velocity of the feed gas stream at the inlet into the reformer tubes between 3.5 and 4.0 mN3/(s*mcat3), in that the specific amount of export steam is between 0 and 0.3 kg of steam per mN3 of hydrogen generated, as presently claimed.
With respect to the difference, Ahmed teaches catalytic steam reforming of biogas under effects of feed composition and operating conditions (Ahmed, Title and Abstract).
Ahmed further specifically teaches using the operating conditions for the steam reforming process including steam to carbon (S/C) ratio from 1.28-3.86, which overlaps the claimed range (Ahmed, Abstract).
As Ahmed expressly teaches, the methane conversion increases with the S/C molar ratio (Ahmed, page 1014, Summary and conclusions).
Ahmed and Ulber are analogous art as they are both drawn to steam reforming process.
In light of the motivation of the effect of operating conditions (e.g., S/C ratio) disclosed by Ahmed as described above, it would therefore have been obvious to one of ordinary skill in the art to incorporate appropriate operation conditions, e.g., the S/C ratio of Ahmed, in order to optimize methane conversion and performance of the steam reforming process of Ulber, and thereby arrive at the claimed invention.
Ahmed further teaches the effect of gas hourly space velocity (GHSV) on the methane conversion and product yields, which showed that methane conversion decreased with increasing space velocities (Ahmed, Abstract; page 1007, Table 2; page 1009, “Effect of GHSV”).
Although there are no disclosures on the amounts of a normalized space velocity of the feed gas stream at the inlet into the reformer tubes as presently claimed, it has long been an axiom of United States patent law that it is not inventive to discover the optimum or workable ranges of result-effective variables by routine experimentation. In re Peterson, 315 F.3d 1325, 1330 (Fed. Cir. 2003) ("The normal desire of scientists or artisans to improve upon what is already generally known provides the motivation to determine where in a disclosed set of percentage ranges is the optimum combination of percentages."); In re Boesch, 617 F.2d 272, 276 (CCPA 1980) ("[D]iscovery of an optimum value of a result effective variable in a known process is ordinarily within the skill of the art."); In re Aller, 220 F.2d 454, 456 (CCPA 1955) ("[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."). "Only if the 'results of optimizing a variable' are 'unexpectedly good' can a patent be obtained for the claimed critical range." In re Geisler, 116 F.3d 1465, 1470 (Fed. Cir. 1997) (quoting In re Antonie, 559 F.2d 618, 620 (CCPA 1977)).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the invention to vary the space velocity of the feed gas stream at the inlet into the reformer tubes within an appropriate range, including over the amounts presently claimed, in order to optimize methane conversion and performance of the steam reforming process, and thereby arrive at the claimed invention.
Ahmed does not explicitly teach the reforming temperature Tref of at least 900°C and at least 930°C, as presently claimed.
With respect to the difference, INL teaches the impact of increasing gas-cooled reactor reactor outlet temperature on hydrogen production via steam methane reforming of natural gas (INL, Title and page 4, EXECUTIVE SUMMARY, first paragraph).
INL further teaches a high temperature gas-cooled reactor (HTGR) that supplies required heat for reforming with an outlet temperature (ROT) (i.e., a steam reforming temperature) of e.g., 900 °C and as high as 950 °C, which falls within the claimed range (INL, page 4, fourth full paragraph; page 5, first paragraph).
INL further teaches a decrease in fuel gas combustion leads to a corresponding decrease in the amount of steam generated and exported (i.e., reduced steam export) (INL, page 5).
As INL expressly teaches, increasing the ROT (i.e., the steam reforming temperature) significantly reduces natural gas consumption. As the ROT is increased, the CO2 emissions are also reduced (INL, page 5).
INL is analogous art as it is drawn to steam reforming process.
In light of the motivation of the reforming temperature disclosed by INL as described above, it would therefore have been obvious to one of ordinary skill in the art to apply the reforming temperature of INL, in order to reduce natural gas consumption and reduce CO2 emission in Ulber for environmental sustainability, and thereby arrive at the claimed invention.
Ulber in view of Ahmed and INL does not explicitly disclose discharging the reforming flue gas from the reformer furnace, cooling at least a portion of the reforming flue gas and/or of the crude synthesis gas product by indirect heat exchange with cooling water to generate steam which can be discharged at least partly from the process as export steam, as presently claimed.
With respect to the difference, De Vreede teaches a process for cooling down a hot flue gas stream (Title and Abstract).
De Vreede further teaches the hot flue gas stream being any flue gas stream, e.g., a furnace flue gas, a steam methane reformer flue gas (De Vreede, [0020]), thus it would have been obvious to one of ordinary skill in the art before the effective filing date of the invention that the process would comprise discharging the reforming flue gas from the reformer furnace, in order to provide the flue gas stream for further process (e.g., cooling).
De Vreede further teaches heat exchange achieved through indirect cooling (i.e., indirect heat exchange) of the hot flue gas stream and the cooling water stream (De Vreede, [0023]-[0024]), where the cooled down gas stream (i.e., export stream) that is separated from the combined water stream is further processed (i.e., steam which can be discharged at least partly from the process) to remove and recover its carbon dioxide content, which can be sequestrated in a subsurface formation (De Vreede, [0033]-[0034]).
As De Vreede expressly teaches, the cooled down gas stream, especially the carbon dioxide recovered as a concentrated carbon dioxide stream, may be used in enhanced oil recovery to recover hydrocarbons from a subsurface reservoir. Alternatively, the carbon dioxide recovered from the cooled down gas stream may be sequestrated in a subsurface formation (De Vreede, [0035]).
De Vreede is analogous art as it is drawn to steam reforming process.
In light of the motivation of cooling the flue gases disclosed by De Vreede as described above, it would therefore have been obvious to one of ordinary skill in the art to discharge the reforming flue gas from the reformer furnace and cool at least a portion of the reforming flue gas by indirect heat exchange with cooling water in Ulber in view of Ahmed and INL, to generate steam which can be discharged at least partly from the process as export steam, in order to recover carbon dioxide for industrial uses (e.g., enhanced oil recovery) and environmental benefits (e.g., sequestration of carbon dioxide), and thereby arrive at the claimed invention.
Regarding claim 5, as applied to claim 1, Ulber further discloses that the casing tube and the heat exchanger tube each have a circular cross section, while the structured packing has an annular (i.e., circular ring-shaped) cross section. The casing tube, the structured packing and the heat exchanger tube are arranged coaxially and concentrically, with the structured packing being arranged between the inner wall of the casing tube and the outer wall of the heat exchanger tube so as to form an essentially gastight closure (i.e., gastight seal) (Ulber, [0025]).
Regarding claim 7, as applied to claim 1, Ulber further discloses both the inlet for the feed gas stream and also the collection conduit for the synthesis gas product (i.e., crude synthesis gas product stream) are located on the underside of the plant (i.e., disposed at the same end of the shell tube) that are accessible for installation and inspection work (Ulber, [0018]; [0026]).
Regarding claim 8, as applied to claim 7, Ulber further discloses the reformer tubes being arranged in a freely suspended or freestanding manner in the interior space of the reformer furnace (Ulber, [0041]).
Ulber further discloses the reformer furnace comprising a lid, a bottom and walls clad or lined with refractory material and an interior space formed thereby, where the inlet for the feed gas stream being arranged outside the interior space of the reformer furnace, thus it would have been obvious to one of ordinary skill in the art before the effective filing date of the invention that the inlet for the feed gas stream is arranged outside the reformer furnace (i.e., projects out of the reformer furnace), with the part of the reformer tube encompassing the reaction chamber (i.e., the opposite end of the shell tube) being arranged at least partly in the interior space of the reformer furnace (i.e., within the reformer furnace) (Ulber, [0038]-[0040]; Fig. 1).
Regarding claim 9, as applied to claim 1, Ulber further discloses a plurality (i.e., a multitude) of reformer tubes and burners are arranged in the interior space of the reformer furnace in such a way that the longitudinal axes of the flames produced by the burners are directed parallel to the longitudinal axes of the reformer tubes (Ulber, [0044]), where it is known in the art that the burners can be installed on the upper side (i.e., roof) or underside (i.e., at the base) of the reformer furnace (Ulber, [0005]).
Regarding claim 10, as applied to claim 1, Ahmed further teaches a methane conversion (i.e., conversion of the feedstock) of 88.4%, 99.2%, where the methane conversion increases with increased temperature, which fall within the claimed ranges (Ahmed, page 1009, right column, last two paragraphs; page 1014, Summary and conclusions).
Regarding claim 11, as applied to claim 1, Ulber further discloses a structured catalyst being a structured packing which contains a catalyst applied as coating to the surface of the structured packing or being embedded in the form of small particles in the structural elements of the structured packing, where the structured packing consisting of thin, corrugated and perforated metal plates or wire meshes (i.e., more than one kind of structured catalyst, wherein the type of structured catalyst relates to the material, structural or textural characteristics thereof), as known in the art (Ulber, [0011]).
Regarding claim 12, as applied to claim 1, Ulber further discloses the structured catalyst that is active for steam reforming comprises structured packings, as known in the art (Ulber, [0011]; [0018]; [0023]).
Claim 6 is rejected under 35 U.S.C. 103 as being unpatentable over Ulber et al. (US 2019/0275494 A1) (Ulber), as provided in the IDS filed 03/21/2023, in view of Ahmed et al. “Catalytic steam reforming of biogas - Effects of feed composition and operating conditions” (Ahmed), Idaho National Laboratory “Sensitivity of Hydrogen Production via Steam Methane Reforming to High Temperature Gas-Cooled Reactor Outlet Temperature Process Analysis” (INL) and De Vreede (US 2008/0276633 A1) (De Vreede) as applied to claim 1 above, and further in view of Shannon et al. “Optimizing Reformer Tube Life by Employing a Realistic Condition-Based Methodology” (Shannon).
Regarding claim 6, as applied to claim 1, Ulber in view of Ahmed, INL and Vreede does not explicitly disclose the heat flow density between the outer wall and the inner wall of the shell tubes is between 50 and 200 kW/m2, averaged over the length of the shell tubes, as presently claimed.
With respect to the difference, Shannon teaches optimizing reformer tube life by employing a realistic condition-based methodology (Shannon, Title).
Shannon further teaches reformer tubes typically operate at metal temperatures in the range of 820 to 950 °C with internal pressures in the range of 2,000 to 3,500 kPa, where high-temperature creep damage in reformer tubes typically initiates between the inner surface and the mid-wall, which occurs because there is thermal gradient through the catalyst tube wall, with the outer surface (i.e., outer wall) being hotter than the inner surface (i.e., inner wall) (Shannon, page 1, last paragraph; page 3, last paragraph to page 4, first paragraph).
As Shannon expressly teaches, the thermal gradient induces stresses in the tube wall that relax and redistribute during operation between start-up and shut-downs or operating trips. The complex stress history must be modeled in order to properly predict the initiation and growth of creep damage and hence tube life (Shannon, page 4, first paragraph).
As Shannon further expressly teaches, creep also can cause permanent changes in tube dimensions – increased diameter and decreased wall thickness (Shannon, page 4, second paragraph).
Shannon is analogous art as it is drawn to using reformer tubes for steam reforming process.
Although there are no disclosures on the amounts the heat flow density between the outer wall and the inner wall of the shell tubes is between 50 and 200 kW/m2, averaged over the length of the shell tubes, as presently claimed, it has long been an axiom of United States patent law that it is not inventive to discover the optimum or workable ranges of result-effective variables by routine experimentation. In re Peterson, 315 F.3d 1325, 1330 (Fed. Cir. 2003) ("The normal desire of scientists or artisans to improve upon what is already generally known provides the motivation to determine where in a disclosed set of percentage ranges is the optimum combination of percentages."); In re Boesch, 617 F.2d 272, 276 (CCPA 1980) ("[D]iscovery of an optimum value of a result effective variable in a known process is ordinarily within the skill of the art."); In re Aller, 220 F.2d 454, 456 (CCPA 1955) ("[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."). "Only if the 'results of optimizing a variable' are 'unexpectedly good' can a patent be obtained for the claimed critical range." In re Geisler, 116 F.3d 1465, 1470 (Fed. Cir. 1997) (quoting In re Antonie, 559 F.2d 618, 620 (CCPA 1977)).
At the time of the invention, it would have been obvious to one of ordinary skill in the art to vary the amounts of heat flow density between the outer wall and the inner wall of the shell tubes of Ulber in view of Ahmed, INL and Vreede, including over the amounts presently claimed, in order to optimize the reformer tube life, and thereby arrive at the claimed invention.
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to JIALAN ZHANG whose telephone number is (703)756-1794. The examiner can normally be reached M-F 9-5.
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/J.Z./Examiner, Art Unit 1732
/CORIS FUNG/Supervisory Patent Examiner, Art Unit 1732
