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 § 112
The following is a quotation of the first paragraph of 35 U.S.C. 112(a):
(a) IN GENERAL.—The specification shall contain a written description of the invention, and of the manner and process of making and using it, in such full, clear, concise, and exact terms as to enable any person skilled in the art to which it pertains, or with which it is most nearly connected, to make and use the same, and shall set forth the best mode contemplated by the inventor or joint inventor of carrying out the invention.
The following is a quotation of the first paragraph of pre-AIA 35 U.S.C. 112:
The specification shall contain a written description of the invention, and of the manner and process of making and using it, in such full, clear, concise, and exact terms as to enable any person skilled in the art to which it pertains, or with which it is most nearly connected, to make and use the same, and shall set forth the best mode contemplated by the inventor of carrying out his invention.
Claims 1-3, 5, 7, 9-19 rejected under 35 U.S.C. 112(a) or 35 U.S.C. 112 (pre-AIA ), first paragraph, as failing to comply with the written description requirement. The claim(s) contains subject matter which was not described in the specification in such a way as to reasonably convey to one skilled in the relevant art that the inventor or a joint inventor, or for applications subject to pre-AIA 35 U.S.C. 112, the inventor(s), at the time the application was filed, had possession of the claimed invention.
In the instant case, the specification does not appear to reasonably support the limitation of Claim 1 requiring “…the reforming step is a single-step catalytic steam reforming step”. Namely, while the specification supports a catalytic steam reforming step, it recites (at [0030] of the publication) that “[t]he reforming section 2 comprises at least a steam reforming reactor, provided with a catalyst for reforming reactions” – i.e., the specification discloses one or more steam reforming reactors provided with a catalyst, and does not provide the reforming to be “single step” as claimed. Further, the as-filed claims do not recite such a limitation. Accordingly, the limitation is not reasonably supported by the originally filed application.
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.
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.
Claim(s) 1-3, 5, 7, 17-18 is/are rejected under 35 U.S.C. 103 as being unpatentable over Dahl et al (US20060057058A1), referred to herein as ‘Dahl’, in view of Liguras et al. (Production of hydrogen for fuel cells by steam reforming of ethanol over supported noble metal catalysts, Applied Catalysis B: Environmental, 2003), hereinafter ‘Liguras’.
Regarding Claim 1, Dahl discloses a process for the production of hydrogen (Abstract), comprising
a step of reforming a carbon-containing feedstock to obtain a raw hydrogen reformed stream ([0018]: ethanol, a carbon-containing feedstock, is reformed to obtain a hydrogen, and said hydrogen is considered a raw hydrogen reformed stream);
a step of separating the raw hydrogen reformed stream to increment the concentration of hydrogen and separate a high concentration hydrogen from a recovered gas stream ([0043]: the product from step four is separated into hydrogen, considered a high concentration hydrogen, and steam, considered a recovered gas stream, which would increment the concentration of hydrogen and separate a high concentration hydrogen from a recovered gas stream);
a step of recirculating a portion of the high concentration hydrogen produced in the separating step to the reforming step together with a steam flow ([0045], FIG. 2: produced and separated hydrogen is recycled to the reforming step; [0057]: hydrogen is recirculated by the use of steam pressurized and pumped by an ejector, which recirculates the separated hydrogen to the reforming step together with a steam flow); wherein
a high concentration hydrogen stream produced in the separating step is recirculated to the reforming step such that the hydrogen entering into the reforming step is greater than or equal to 50 mol% with respect to the carbon-containing feedstock to be reformed ([0052]: The molar ratio between ethanol and hydrogen (ethanol:hydrogen) in the dehydration/hydrogenation step, which is considered the beginning of the reforming step, as the process of Dahl from dehydrogenation/hydrogenation, prereforming, and primary reforming is considered by the invention as a reforming process, is preferably between 0.2-1, corresponding to a mol% of hydrogen with respect to ethanol, or the feedstock to be reformed, of 50% to 83.3% - this ratio is maintained by the addition of hydrogen recycled from the separation step indicated above ([0051])).
Further regarding Claim 1, Dahl discloses the reforming step is a catalytic steam reforming step, in which the feedstock is contacted with a catalyst in the presence of steam and is subjected to reforming reactions resulting in formation of hydrogen (Claim 1 of Dahl: steam reforming of ethanol in the presence of a catalyst is disclosed, and said reforming results in reforming reactions that produce hydrogen).
Further regarding Claim 1, while Dahl is silent regarding the reforming step being performed under thermodynamic conditions selected so as to operate, in a C-O- H ternary plot expressed in molar percentages, in a zone having H between 70 and 90%, carbon between 5 and 35%, oxygen between 10 and 40%, this would be inherent to the method of Dahl. Since the process of Dahl uses the same reactants as the instant invention (both the instant invention and Dahl use ethanol feedstock and hydrogen gas) in the same proportions as shown above, including operating using a ratio of hydrogen to reforming feedstock within the range claimed, the resulting operating ternary mixture of carbon, oxygen, and hydrogen in the reforming step must necessarily be the same in both the instant invention and that of Dahl, absent evidence of the contrary. Further, at Page 8 of the instant specification, it is disclosed that, as a result of the high concentration of hydrogen which is extracted from the separating step and recirculated to the reforming step, the disclosed process is distinguished from the prior art process – this is further evidence that the amount of hydrogen, which is identical in both the instant claims and in Dahl, is critical to achieving the aspects of the claimed invention, including achieving the thermodynamic conditions claimed. Products produced by the same or nearly the same process cannot have mutually exclusive properties – see MPEP 2112.01 (I).
Further, Dahl discloses the recirculation step is performed by means of an ejector using a flow of steam as a driving fluid for recirculating hydrogen ([0057]: water derived from the inlet streams is heated and evaporated to form steam that acts as a driving fluid driving the recycle).
Further regarding Claim 1, Dahl does not disclose the use of steam coming from the reforming step to drive the recycle stream; however, Dahl does disclose that, after reforming, the resulting product stream is separated into hydrogen and water (steam; [0043]). Therefore, Dahl discloses the isolation of steam from the reforming step that would be useful for driving the recycle, as disclosed, and does not disclose any particular use or destination for said steam.
Given this, one of ordinary skill in the art before the effective filing date of the claimed invention would have found it obvious to use a flow of steam coming from the reforming step as a driving fluid for recirculating hydrogen, as Dahl discloses the production of steam coming from such a reforming step that would be useful for such a purpose, and the use of such separated steam would reduce the heat duty of the process such that less energy would be required for the production of steam to drive the recycle stream, thereby making the process more economical and less wasteful.
Further regarding Claim 1, Dahl does not disclose that the reforming step is a single-step catalytic steam reforming step.
However, such single-step catalytic processes of reforming hydrocarbons with steam are known and utilized in the prior art. In particular, Liguras discloses an apparatus for catalytic steam reforming of ethanol that only utilizes one reforming step (i.e., a single-step reforming as claimed), and shows high output of hydrogen in the use of such a single-step reforming process (2.2. Apparatus and procedures; 3. Results and discussion; 4. Conclusions: “Long-term tests conducted under severe conditions showed that the catalyst is acceptably stable and could be used for the production of hydrogen for fuel cell applications.”). Furthermore, it is apparent that utilizing such a single-step reforming process as compared to a multi-reforming step would simplify the process of steam reforming, thereby reducing process costs and complexity, and improving the economics of the process.
Therefore, one of ordinary skill in the art before the effective filing date of the claimed invention would have found it obvious to utilize a single-step reforming process as disclosed by Liguras within the process of Dahl – such a process would simplify the process of steam reforming, thereby reducing process costs and complexity, and improving the economics of the process, while simultaneously providing a process considered suitable for the production of hydrogen for use in fuel cells.
Regarding Claim 2, the prior art meets the limitations of Claim 1 as shown above. Further, Dahl discloses the feedstock is a feedstock from renewable sources selected in the group consisting of: alcohols, vegetable oils, bio-oils or pyrolysis oils (the carbon-containing feedstock to be ethanol, which is considered a feedstock from renewable sources as claimed, as discussed above).
Regarding Claim 3, the prior art meets the limitations of Claim 1 as shown above. Further, Dahl discloses the feedstock is ethanol produced from biomass ([0002]: use of ethanol obtained from biomass is disclosed).
Regarding Claim 5, the prior art meets the limitations of Claim 1 as shown above. Further, Dahl discloses the separating step is performed by pressure swing adsorption on a selective adsorption porous material ([0036]: the use of pressure swing adsorption for the purification of the produced hydrogen, which would inherently utilize a selective adsorption porous material, as the use of a selective adsorption porous material is fundamental to pressure swing adsorption processes).
Regarding Claim 9, the prior art meets the limitations of Claim 1 as shown above. Further, Dahl discloses the molar ratio between ethanol and hydrogen (ethanol:hydrogen) in the dehydration/hydrogenation step is preferably between 0.2-1, corresponding to a mol% of hydrogen with respect to ethanol, or the feedstock to be reformed, of 50% to 83.3%, as discussed above – further, this hydrogen is considered to be dry, in that water is not included in this calculation).
Regarding Claim 10, the prior art meets the limitations of Claim 1 as shown above. Further, Dahl discloses the process is in steady operation, the steam reforming is performed only with the steam already present and used in the process without supplying steam from the outside, and without necessarily producing steam to be exported to the outside (Fig. 2: depicted is a process flow diagram for the process – while it is not explicitly disclosed, one of ordinary skill in the art would understand, based on the figure and context of the invention, and based on the use of a “recycle” stream (the term “recycle” inherently means to use a stream in a new “cycle” of a continuous process), that the process of Dahl is considered a continuous and steady operation process for continuously producing hydrogen; further, Dahl does not disclose the addition of steam to the inventive process after the process reaches a steady operation, and does not disclose producing steam to be exported to the outside).
Regarding Claim 11, the prior art meets the limitations of Claim 1 as shown above. Further, Dahl discloses the process is in steady operation after transitory steps of initiating and triggering the reforming reactions (while Dahl is silent regarding transitory steps of initiating and triggering the reforming reactions, transient operation of any chemical process is required before a process may reach a continuous, steady state – this transient operation is typically referred to as “start-up” operation, in which the initial reactants are fed to the reactor, and the process proceeds dynamically until a steady state, i.e., a state in which process variables no longer change, is reached. Every chemical process operating at steady state must first perform transitory steps of initiating reactions, as it is impossible for a process to begin at steady state, and therefore this transient operation is considered implicit to and necessarily present in the process of Dahl).
Regarding Claims 12 and 13, the prior art meets the limitations of Claim 1 as shown above. Further, Dahl discloses the use of ethanol as a feedstock as discussed above, which is considered a renewable source comprising at least one alcohol.
Regarding Claim 19, Dahl discloses a process for the production of hydrogen (Abstract), comprising
reforming a carbon-containing feedstock to obtain a raw hydrogen reformed stream ([0018]: ethanol, a carbon-containing feedstock, is reformed to obtain a hydrogen, and said hydrogen is considered a raw hydrogen reformed stream);
separating the raw hydrogen reformed stream to create a supply of high concentration hydrogen ([0043]: the produced hydrogen is separated from the produced hydrogen-rich product stream, which would increment the concentration of hydrogen and separate a high concentration hydrogen from a recovered gas stream);
recirculating a portion of the high concentration hydrogen produced in the separating step to the reforming step together with a steam flow ([0051]: produced and separated hydrogen is recycled to the reforming step; [0057]: hydrogen is recirculated by the use of steam pressurized and pumped by an ejector, which would thereby recycle the separated hydrogen to the reforming step together with a steam flow), such that
a high concentration hydrogen stream produced in the separating step is recirculated to the reforming step such that the hydrogen entering into the reforming step is greater of or equal to 50 mol% with respect to the carbon-containing feedstock to be reformed ([0052]: The molar ratio between ethanol and hydrogen (ethanol:hydrogen) in the dehydration/hydrogenation step, which is considered the beginning of the reforming step, as the process of Dahl from dehydrogenation/hydrogenation, prereforming, and primary reforming is considered by the invention as a reforming process, is preferably between 0.2-1, corresponding to a mol% of hydrogen with respect to ethanol, or the feedstock to be reformed, of 50% to 83.3% - this ratio is maintained by the addition of hydrogen recycled from the separation step indicated above ([0051])).
Further regarding Claim 19, while Dahl is silent regarding the reforming step being performed under thermodynamic conditions selected so as to operate, in a C-O- H ternary plot expressed in molar percentages, in a zone having H between 70 and 90%, carbon between 5 and 35%, oxygen between 10 and 40%, this would be inherent to the method of Dahl. Since the process of Dahl uses the same reactants as the instant invention (both the instant invention and Dahl use ethanol feedstock and hydrogen gas) in the same proportions as shown above, including operating using a ratio of hydrogen to reforming feedstock within the range claimed, the resulting operating ternary mixture of carbon, oxygen, and hydrogen in the reforming step must necessarily be the same in both the instant invention and that of Dahl, absent evidence of the contrary. Further, at Page 8 of the instant specification, it is disclosed that, as a result of the high concentration of hydrogen which is extracted from the separating step and recirculated to the reforming step, the disclosed process is distinguished from the prior art process – this is further evidence that the amount of hydrogen, which is identical in both the instant claims and in Dahl, is critical to achieving the aspects of the claimed invention, including achieving the thermodynamic conditions claimed. Products produced by the same or nearly the same process cannot have mutually exclusive properties – see MPEP 2112.01 (I).
Regarding Claim 7, the prior art meets the limitations of Claim 1 as shown above. Further, Dahl makes obvious a gas recirculating step, in which the recovered gas stream separated in the separating step is recirculated to the reforming step (as discussed above, it would be obvious to utilize the steam separated from the hydrogen from the reforming product stream, said steam being considered “the recovered gas stream”, to drive the recycle stream, thereby reintroducing this recovered gas stream into the reforming step).
Regarding Claims 17 and 18, the prior art meets the limitations of Claim 1 as shown above. Further, Dahl makes obvious a high concentration hydrogen stream produced in the separating step is recirculated to the reforming step such that the hydrogen entering into the reforming step is greater of or equal to 60 mol% and 70 mol% with respect to the carbon-containing feedstock to be reformed ([0052]: The molar ratio between ethanol and hydrogen (ethanol:hydrogen) in the dehydration/hydrogenation step, otherwise known as the reforming step, is preferably between 0.2-1, corresponding to a mol% of hydrogen with respect to ethanol, or the feedstock to be reformed, of 50% to 83.3%, which overlaps with the instantly claimed ranges - this ratio is maintained by the addition of hydrogen recycled from the separation step indicated above ([0051]). As set forth in MPEP 2144.05, in the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art,” a prima facie case of obviousness exists, In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990) – as such, the instant claimed range is obvious over the prior art range).
Claim(s) 14 is/are rejected under 35 U.S.C. 103 as being unpatentable over Dahl et al (US20060057058A1), referred to herein as ‘Dahl’, in view of Liguras et al. (Production of hydrogen for fuel cells by steam reforming of ethanol over supported noble metal catalysts, Applied Catalysis B: Environmental, 2003), hereinafter ‘Liguras’, and further in view of Marquevich et al. (Hydrogen Production by Steam Reforming of Vegetable Oils Using Nickel-Based Catalysts, Industrial and Engineering Chemistry Research, 2001), hereinafter ‘Marquevich’.
Regarding Claim 14, while Dahl discloses a method of reforming ethanol using steam reforming in the presence of a catalyst (Claim 1), and further discloses the use of biomass materials as a source of reactants in the present invention ([0002]), Dahl does not disclose that the carbon-containing feedstock is a feedstock from a renewable source comprising at least one vegetable oil.
Marquevich discloses a process for the production of hydrogen using a feedstock comprising vegetable oils, including sunflower, rapeseed, soybean, and corn oils (Introduction). A person of ordinary skill in the art would have recognized Marquevich as analogous to Dahl, as both references are drawn to the same field of endeavor as the claimed invention, steam reforming of biomass-based feedstocks in the presence of a catalyst to produce hydrogen - a reference is analogous art to the claimed invention if the reference is from the same field of endeavor as the claimed invention, In re Bigio, 381 F.3d at 1325, 72 USPQ2d at 1212.
Further, Marquevich discloses the composition of each oil (Table 1) – with the exception of the presence of some organic acids, the composition of the oils mainly comprises oxygen, hydrogen, and carbon. These elements are also the primary elements found in the feedstock of Dahl (ethanol has a molecular formula of C2H5OH), and as such the feedstocks of both Marquevich and Dahl have substantially similar compositions, and would be expected to act in a similar way when subjected to steam reforming. Further, Marquevich discloses that hydrogen can be produced from vegetable oils by catalytic steam reforming using nickel-based catalysts and at process conditions very similar to those used industrially for the steam reforming of hydrocarbons, and that these oils can be used as feedstocks for the process with equivalent yields and rates of hydrogen formation (Conclusions).
Accordingly, the prior art has recognized that both ethanol and vegetable oils are suitable feedstocks that, when subjected to steam reforming as disclosed by Dahl, result in the production of hydrogen gas. Accordingly, one of ordinary skill in the art before the effective filing date of the claimed invention would have found it obvious to combine ethanol as disclosed by Dahl with vegetable oils as disclosed by Marquevich in order to form a third composition to be used for the very same purpose, as ethanol and vegetable oils are both known in the art to be useful for such a purpose – it is prima facie obvious to combine two compositions, each of which is taught by the prior art to be useful for the same purpose, in order to form a third composition to be used for the very same purpose…[T]he idea of combining them flows logically from their having been individually taught in the prior art." In re Kerkhoven, 626 F.2d 846, 850, 205 USPQ 1069, 1072 (CCPA 1980). Such a combination would result in a feedstock as claimed.
Claim(s) 15-16 is/are rejected under 35 U.S.C. 103 as being unpatentable over Dahl et al (US20060057058A1), referred to herein as ‘Dahl’, in view of Liguras et al. (Production of hydrogen for fuel cells by steam reforming of ethanol over supported noble metal catalysts, Applied Catalysis B: Environmental, 2003), hereinafter ‘Liguras’, and further in view of Wang et al. (Biomass to Hydrogen via Fast Pyrolysis and Catalytic Steam Reforming of the Pyrolysis Oil or Its Fractions, Industrial and Engineering Chemistry Research, 1997), hereinafter ‘Wang.
Regarding Claim 15-16, while Dahl discloses a method of reforming ethanol using steam reforming in the presence of a catalyst ([0032]), and further discloses the use of biomass materials as a source of reactants in the present invention ([0002]), Dahl does not disclose that the carbon-containing feedstock is a feedstock from a renewable source comprising at least one pyrolysis oil or bio-oil.
Wang discloses a process for the production of hydrogen using a feedstock comprising pyrolytic oil, considered a “pyrolysis oil” and also known as “bio-oil” or “biocrude” (Introduction). A person of ordinary skill in the art would have recognized Wang as analogous to Dahl, as both references are drawn to the same field of endeavor as the claimed invention, steam reforming of biomass-based feedstocks in the presence of a catalyst to produce hydrogen - a reference is analogous art to the claimed invention if the reference is from the same field of endeavor as the claimed invention, In re Bigio, 381 F.3d at 1325, 72 USPQ2d at 1212.
Further, Wang discloses the use of these pyrolysis oils/bio-oils as feedstocks in the generation of hydrogen by traditional steam reforming, and compares the performance thereof to that of more traditional feedstocks for such a process (Table 6), including methanol, which has a chemical structure substantially similar to that of ethanol as disclosed by Dahl (CH3OH). As is apparent from the table, the pyrolysis oil/bio-oil derivatives, such as levoglucosan, cellulose, and xylan, produced a hydrogen yield higher than that of even methanol when subjected to steam reforming.
Accordingly, the prior art has recognized that both ethanol and pyrolysis oils/bio-oils derived from levoglucosan, cellulose, and xylan are suitable feedstocks that, when subjected to steam reforming as disclosed by Dahl, result in efficient production of hydrogen gas. Accordingly, one of ordinary skill in the art before the effective filing date of the claimed invention would have found it obvious to combine ethanol as disclosed by Dahl with pyrolysis oils/bio-oils derived from levoglucosan, cellulose, and xylan as disclosed by Wang in order to form a third composition to be used for the very same purpose, as ethanol and pyrolysis oils/bio-oils derived from levoglucosan, cellulose, and xylan are both known in the art to be useful for such a purpose – it is prima facie obvious to combine two compositions, each of which is taught by the prior art to be useful for the same purpose, in order to form a third composition to be used for the very same purpose…[T]he idea of combining them flows logically from their having been individually taught in the prior art." In re Kerkhoven, 626 F.2d 846, 850, 205 USPQ 1069, 1072 (CCPA 1980). Such a combination would result in a feedstock as claimed.
Response to Arguments
Applicant’s arguments, filed 08/05/2025, are acknowledged.
With respect to arguments in regard to prior art rejections under section 102, Applicant’s arguments have been fully considered and are persuasive. Therefore, the rejection has been withdrawn. However, upon further consideration, a new ground(s) of rejection is made under section 103 in view of Liguras.
Applicant argues that Dahl alone does not disclose or suggest the newly amended limitations of Claim 1; however, as shown above, these limitations are obvious in view of Liguras.
Further, Applicant argues that Dahl does not disclose any particular use or destination of the steam generated and separated by the process: “[t]he Examiner argues that for a person skilled in the art it would be obvious to use said steam to drive the recycling, however the Applicant respectfully disagrees with the Examiner. Such steam coming from the reforming step may have different applications or no application at all. There is no hint in Dahl to use it as a driving fluid for recirculating hydrogen; as a matter of fact, Dahl does not disclose or suggest any particular use of said steam.” This is not considered persuasive – while Dahl does not “hint” at utilizing said steam to drive the ejector fluid, Dahl clearly does disclose the use of steam to drive the ejector – utilization of steam generated in a process for other purposes is a routine optimization of a process to reduce operations costs, such as heat needed to generate and provide said steam; these are the same benefits disclosed as resulting from the claimed invention (Remarks, Page 9, paragraph 1). As such, it is irrelevant that Dahl does not explicitly disclose such a configuration. Absent some other evidence of unexpected results associated with such a feature, this argument is not persuasive.
Conclusion
Applicant's amendment necessitated the new ground(s) of rejection presented in this Office action. Accordingly, THIS ACTION IS MADE FINAL. See MPEP § 706.07(a). 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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/L.E.L./ Examiner, Art Unit 1738
/SALLY A MERKLING/ SPE, Art Unit 1738