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 .
Continued Examination Under 37 CFR 1.114
A request for continued examination under 37 CFR 1.114, including the fee set forth in 37 CFR 1.17(e), was filed in this application after final rejection. Since this application is eligible for continued examination under 37 CFR 1.114, and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114. Applicant's submission filed on 1/29/2026 has been entered.
Response to Arguments
With respect to the rejection of Claims 17-19, 25-26 and 36 are rejected under 35 U.S.C. 103 as being unpatentable over US 9637381 B2 Bittencourt et al. in view of Choudhary et al., as understood the traversal relies on amendments. It is noted that Claims 19 and 26 were canceled; the rejections of those claims are withdrawn. Applicant argues “the independent claims have been amended to recite a steam pre- reforming catalyst that includes "platinum in a concentration of 0.05% w/w." In the Action, the Examiner admits that "Bittencourt et al. does not teach platinum as part of the nickel-based catalyst." (Action, p. 3.) As such, the Examiner relies on Choudhary for such teachings. However, Choudhary teaches a catalyst with a platinum concentration of 0.1 wt.%, 0.5 wt.%, and 2.5 wt.%. (Choudhary, p. 753, Table 1.) Thus, Choudhary does not disclose or suggest "platinum in a concentration of 0.05% w/w," as now claimed.” [Remarks, Page 7, Paragraph 5]. In response it is acknowledged that Choudhary et al. does not explicitly disclose a Pt concentration of 0.05% in the final catalyst, however, “A reference may be relied upon for all that it would have reasonably suggested to one having ordinary skill in the art” (MPEP 2123.I) and is not necessarily limited to the embodiments presented. In the present example Choudhary has identified the Pt concentration as a results-effective variable. It has been held that routine optimization of a results-effective variable, such as Pt concentration, that finds the optimal range would be obvious to try, see MPEP 2144.05.II. In this case the Pt concentration has been shown by Choudhary to impact the reaction temperature and methane conversion. It would have been obvious to try an intermediate concentration between 0% and 0.1%, such as 0.05%, to see if the benefits of lower reaction temperature and higher methane conversion could be achieved with a lower loading of Pt. As Pt is the most expensive component of the catalyst using less Pt would have cost benefits.
Applicant further argues that Choudhary teaches away from Pt loadings lower than 0.1 wt.% “In addition, Choudhary explicitly teaches that reaction start temperature "Ts decreases with increasing noble metal concentration" (p. 752) and that CH4 conversion increases with increasing platinum concentration (p. 753, Table 1). Thus, if anything, a person of ordinary skill in the art reading Choudhary would include more than 0.1 wt.% platinum in their catalysts to increase methane conversion and decrease reaction start temperature.” [Remarks, Page 8, Paragraph 1]. This is unpersuasive. Although the increased conversion and decreased temperature provide a motivation to increase Pt loading, Applicant fails to consider that the cost savings of using a lower Pt concentration provide a motivation for a lower Pt loading; Examiner’s rationale for combining or modifying references to support an obviousness conclusion need not mirror applicants (MPEP 2144 IV). With competing benefits it is obvious that one of ordinary skill in the art would weight the costs and benefits of Pt loading for their particular situation; a lower Pt loading reduces the upfront capital cost required to see the first profits.
Applicant further argues for process limitations “Applicant has amended the independent claims to state that the claimed steam pre-reforming catalyst "converts hydrocarbons to hydrogen and/or syngas in a steam pre-reforming process ... at a space velocity between 1,200 to 2,000 h-1." Bittencourt discloses 18,000 h-1 GHSV which is significantly higher than the claimed space velocity. Second, Applicant has amended the independent claims to recite that the claimed steam pre-reforming catalyst "converts hydrocarbons to hydrogen and/or syngas in a steam pre- reforming process ...after 48 hours of exposing the steam pre-reforming catalyst to steam at 450°C at a pressure of 20 atm." As explained in the specification, Applicant discovered that "it is possible to obtain a high resistance to deactivation by the passage of steam in the absence of a reducing agents for catalysts prepared in accordance with the present invention." (Publication, [0044].) Specifically, "the nickel catalysts with low platinum content ...present for the steam pre-reforming of hydrocarbons high resistance to deactivation by the passage of steam." (Id. at [0045].) None of the references cited by the Examiner disclose or suggest the claimed steam pre-reforming catalyst "converts hydrocarbons to hydrogen and/or syngas in a steam pre- reforming process .. after 48 hours of exposing the steam pre-reforming catalyst to steam at 450°C at a pressure of 20 atm."” [Remarks, Page 8 Paragraph 3-4]. This is unpersuasive. It is understood that if the physical composition is the same the properties must be the same (see MPEP 2112.01.II). In other words absent any physical difference between the claimed invention and what is suggested by the prior art it is understood that the functionality of the claimed invention and what is suggested by the prior art must be the same. To suggest otherwise would be to assert that two identical compositions could have mutually exclusive properties. The rejections have been MAINTAINED.
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.
Claims 17-18, 25 and 36 are rejected under 35 U.S.C. 103 as being unpatentable over US 9637381 B2 Bittencourt et al. in view of NPL - "Beneficial effects of Noble Metal Addition to Ni/Al-2-O3 Catalyst Oxidative Methane-to-Syngas Conversion " Choudhary et al. Claim 17 requires ” A steam pre-reforming catalyst, comprising: a) an inorganic oxide support selected from alumina, magnesium aluminate, or mixture thereof”. Bittencourt et al. is directed at a nickel catalyst for steam pre-reforming hydrocarbons [Abstract]. Bittencourt et al. discloses “an inorganic oxide support, preferably comprised of alumina, magnesium aluminate, calcium aluminate, or a mixture thereof” [Column 5, lines 24-26].
Claim 17 further requires “b) a mixture of nickel, lanthanum, and cerium oxides, with the total content of nickel expressed as nickel oxide (NiO), from 6 to 15:1 (w/w) between NiO and La2O3, and 2 to 4:1 (w/w) between Ce2O3 and La2O3, and a total NiO content within the catalyst is between 5 to 50% w/w”. Bittencourt et al. discloses “oxides of Ni, La, and Ce in a proportion of 6:1 (w/w) to 15:1 (w/w) of NiO:La2O3 and Ce2O3:La2O3 in proportion of 2:1 (w/w) to 4:1 (w/w) and a total content of NiO between 4% w/w and 50% w/w”. [Column 5, lines 27-30].
Claim 17 further requires “and c) platinum in a concentration of 0.05% w/w, calculated as a metallic element in a final catalyst”. Bittencourt et al. does not teach platinum as part of the nickel-based catalyst.
Claim 17 further requires “the steam pre-reforming catalyst converts hydrocarbons to hydrogen and/or syngas in a steam reforming process with a steam/carbon ratio between 0.8 to 3.0 mol/mol”. Bittencourt et al. discloses “The steam/carbon ratio at the entrance to the reactor containing the catalyst is between 0.1 mol/mol and 5 mol/mol” [Col. 6, Lines 50-52] which has significant overlap with the claimed range.
Claim 17 further requires “wherein the steam pre-reforming catalyst converts hydrocarbons to hydrogen and/or syngas … at temperatures of 330-500°C”. Bittencourt et al. discloses “Catalysts prepared in this way may be used to produce a gas rich in methane and hydrogen, free of other hydrocarbons, at pressures between 1 kgf/cm and 50 kgf/cm and temperatures between 300 °C. and 650 °C”. [Column 6, Lines 64-67].
Claim 17 further requires “wherein the steam pre-reforming catalyst converts hydrocarbons to hydrogen and/or syngas … at a H2/load ratio between 0.1 to 0.3 Nm3 of H2/kg of load”. The term “load” is interpreted to mean the hydrocarbon to be reformed. Bittencourt et al. discloses “H2/hydrocarbon content being 0.05 mol/mol to 0.4 mol/mol.” [Col. 11, Line 26] in the claims. It is understood that the hydrocarbons in Bittencourt et al. are mostly methane (CH4) with small amounts of olefins such as ethylene (see Example 4-7). For the following calculation it is assumed that the average molar mass of hydrocarbons is the same as the molar mass of methane for simplicity, therefore it should be understood that the following calculation is an approximation. Converting the endpoints of the range of Bittencourt et al. from H2/hydrocarbon in mol/mol to H2/load in Nm3/kg yields the following: 0.05 mol H2 at STP occupies a volume of 1.12 L (0.05 mol * 22.4 L/mol) which is equivalent to 0.00112 m3. 1 mol of methane weighs 16 grams, or 0.016 kg, so the lower end of the range is 0.07 Nm3/kg (0.00112/0.016). The upper end of the range is given by 0.4 mol of H2 at STP occupies a volume of 8.96 L (0.4 mol * 22.4 L/mol) which is equivalent to 0.00896 m3, the methane is the same 0.016 kg. The upper end of the range is therefore 0.56 Nm3/kg (0.00896/0.016). Therefore it is understood that Bittencourt et al. discloses a H2/load ratio between about 0.07 to about 0.56 Nm3 of H2/kg of load which significantly overlaps with the range claimed.
Claim 17 further requires “wherein the steam pre-reforming catalyst converts hydrocarbons to hydrogen and/or syngas … at a space velocity between 1,200 to 2,000 h-1 based on hydrocarbon flow.”. Bittencourt et al. discloses 18,000 h-1 GHSV [Col. 10, Table 1] which is higher than the range claimed. However, it is noted that Claim 17 does not require a space velocity between 1,200 to 2,000 h-1, only a catalyst that can convert some amount of hydrocarbon at those space velocities. Nothing in the disclosure of Bittencourt et al. teaches or suggests that high space velocities are required, or that low space velocities are wholly ineffective. It is therefore understood that the catalyst suggested by the combination of Bittencourt et al. and Choudhary et al., having the same physical composition as what is claimed would have the same physical properties, including an effective range of space velocities, see MPEP 2112.01.II.
Regarding the limitation not taught by Bittencourt, namely the platinum concentration, Choudhary et al. discloses a steam reforming catalyst, Pt-Ni/Al2O3, with 0, 0.1, and 0.5 wt.% platinum [Page 753, Table 1]. Choudhary teaches “The as-prepared/calcined form of the catalyst contains a catalytically inactive NiAl2O4 phase, which is difficult to reduce … However, the reaction on calcined Ni/MgO, Ni/CaO, and Ni/rare earth oxide [La2O3 and Ce2O3] catalysts is found to start at much lower temperatures because of their ease of reduction during the initial reaction period” [page 752, Column 1, Paragraph 1]. Choudhary concludes “the addition of noble metal (Pt, Pd, or Ru) to Ni/Al2O3 catalyst results in a large decrease in the reaction start temperature in the oxidative conversion of methane to syngas over the unreduced catalyst and also causes an improvement in the catalytic activity/selectivity” [Page 754, last paragraph of column 1 through the top of column 2].
It is noted that the limitation of 0.05% Pt (w/w) is not explicitly disclosed by Choudhary et al., however Choudhary et al. clearly identified Pt concentration as a results effective variable (see MPEP 2144.05.II), that is by varying the amount of Pt on the catalyst a predictable trend of lower activation temperature and higher methane conversion was observed. This makes the selection of an intermediate value between 0% and 0.1% Pt, such as 0.05% Pt, obvious to try to see if the disclosed benefits could be realized with a lower Pt loading, thus saving start-up cost of an operation.
It would have been obvious for one of ordinary skill in the art to have combined the catalyst of Bittencourt et al. with the teaching to use platinum of Choudhary et al. because these catalysts have the same active species (Ni0) and perform the same reaction (conversion of hydrocarbons and steam into syngas mixtures). Furthermore, although Choudhary et al. does not specifically study nickel catalyst supported on rare earth oxides they do teach that such catalysts are useful because they are more easily reduced than the nickel catalysts supported on Al2O3 alone. The motivation to combine these catalysts is given in Choudhary et al. when they teach that the addition of platinum results in a decrease in the reaction start temperature and an improvement in the catalytic activity/selectivity. Having a lower start temperature in the first stage is useful because that means less energy cost has to be spent to start the reaction. An improvement in catalytic activity/selectivity is obviously beneficial. Therefore it would have been obvious to one of ordinary skill in the art to combine the support of Bittencourt et al. with the platinum doping of Choudhary et al. to have arrived at the invention as claimed. Furthermore Choudhary et al. teaches that platinum concentration and reaction temperature have a result effective variable relationship [Page 753, Table 1] and therefore it would have been obvious to try to optimize the concentration of platinum in order to balance the initial upfront cost savings of using less platinum with the running costs savings expected from a catalyst with more platinum that lowered reaction temperatures.
Regarding Claim 18, Bittencourt et al. and Choudhary et al. together teach all of the limitations of Claim 17. Claim 18 further requires “a total content of NiO within the catalyst is between 7 and 30% w/w”. Bittencourt et al. discloses “a total content of NiO between 4% w/w and 50% w/w, preferably between 7% w/w and 30% w/w” [Column 5, lines 30-31].
Claim 25 requires “A steam pre-reforming catalyst, comprising: a) nickel oxide (NiO)”. Bittencourt et al. discloses “oxides of Ni, La, and Ce in a proportion of 6:1 (w/w) to 15:1 (w/w) of NiO:La2O3 and Ce2O3:La2O3 in proportion of 2:1 (w/w) to 4:1 (w/w) and a total content of NiO between 4% w/w and 50% w/w” [Column 6, lines 34-37].
Claim 25 further requires “and b) platinum in a concentration of 0.05% w/w, calculated as a metallic element in the final catalyst.”. Bittencourt et al. does not disclose the final catalyst comprises platinum.
Choudhary et al. discloses platinum containing catalysts with 0, 0.1, and 0.5 wt.% platinum [Table 1, Page 753] and identifies Pt loading as a results-effective variable (see Claim 17). This renders a Pt loading of 0.05% obvious to try to one of ordinary skill in the art.
Claim 25 further requires “the steam pre-reforming catalyst converts hydrocarbons to hydrogen and/or syngas with a steam/carbon ratio between 0.8 to 3.0 mol/mol, at temperatures of 330-500 °C, at a H2/load ratio between 0.1 to 0.3 Nm3 of H2/kg of load, and at a space velocity between 1,200 to 2,000 h-1 based on hydrocarbon flow”. These limitations are identical to those found in Claim 17 and therefore support for them can be found above. It would have been obvious for one of ordinary skill in the art to have combined the catalyst of Bittencourt et al. with the teaching to use platinum of Choudhary et al. because these catalysts have the same active species (Ni0) and perform the same reaction (conversion of hydrocarbons and steam into syngas mixtures). Furthermore, although Choudhary et al. does not specifically study nickel catalyst supported on rare earth oxides they do teach that such catalysts are useful because they are more easily reduced than the nickel catalysts supported on Al2O3 alone. The motivation to combine these catalysts is given in Choudhary et al. when they teach that the addition of platinum results in a decrease in the reaction start temperature and an improvement in the catalytic activity/selectivity. Having a lower start temperature in the first stage is useful because that means less energy cost has to be given to start the reaction. An improvement in catalytic activity/selectivity is obviously beneficial. Therefore it would have been obvious to one of ordinary skill in the art to combine the support of Bittencourt et al. with the platinum doping of Choudhary et al. to have arrived at the invention as claimed. Furthermore Choudhary et al. teaches that platinum concentration and reaction temperature have a result effective variable relationship [Page 753, Table 1] and therefore it would have been obvious to try and optimize the concentration of platinum in order to balance the initial upfront cost savings by using less platinum with the running costs savings expected from a catalyst with more platinum that required lower temperatures to be effective.
Regarding Claim 36, Bittencourt et al. and Choudhary et al. together teach all of the limitations of Claim 17. Claim 36 further requires “the steam pre-reforming catalyst is effective for a steam pre-reforming process of converting hydrocarbons to hydrogen and/or syngas at a pressure between 2 to 40 kgf/cm2.”. Bittencourt et al. discloses “Catalysts prepared in this way may be used to produce a gas rich in methane and hydrogen, free of other hydrocarbons, at pressures between 1 kgf/cm and 50 kgf/cm” [Column 6, Lines 64-66]. Although the units of the present invention and Bittencourt et al. differ (kgf/cm2 vs. kgf/cm) this is understood to be due to an obvious typo, as kgf/cm is not a unit of pressure (Force/Area) and one of ordinary skill in the art would recognize that the intended pressure of Bittencourt et al. was between 1 kgf/cm2 and 50 kgf/cm2.
Conclusion
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/JOSHUA MAXWELL SPEER/
Examiner
Art Unit 1736
/DANIEL BERNS/Primary Examiner, Art Unit 1736