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 .
Election/Restrictions
Applicant’s election without traverse of Group I, Claims 1-11 in the reply filed on November 13, 2025 is acknowledged. Group II, Claims 12-13 have been withdrawn as being directed to a non-elected invention.
Claim Objections
Claim 1 is objected to because of the following informalities: typo.
Claim 1 recites: “…comprising, a rector containing a catalyst…”. The correct word appears to be “reactor”.
For purposes of examination, examiner will interpret claim 1 as reciting: “…comprising, a reactor containing a catalyst…”
Appropriate correction is required.
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, 3, 6-9 and 11 are rejected under 35 U.S.C. 103 as being unpatentable over Katsumi et al. (JP2013/095616A-relied on machine translation, hereinafter Katsumi).
In regards to Claim 1, Katsumi discloses a direct decomposition device for hydrocarbons for directly decomposing hydrocarbons into carbon and hydrogen (see paragraphs [0001], [0010], [0018] and [0024]), comprising
a reactor (#3) containing a catalyst (#) including a plurality of metal particles with an iron purity of 86% or more (see figure 1 and paragraphs [0062], [0089] and [0091]; Katsumi discloses that powdered catalyst is supplied airtightly into reaction tube #3, i.e. reactor. Iron metal catalysts are desirable because of their versatility. Further, Katsumi discloses in the working example, the metal powder catalyst is an iron catalyst which produced hydrogen in 99% or more in purity and ultrafine carbon powder was nanocarbon that grew from entanglement with the iron catalyst. Although Katsumi is silent in regards to wherein the plurality of metal particles has an iron purity of 86% or more, Katsumi clearly discloses that the decomposition device produces hydrogen in 99% purity or more. Therefore, it is considered reasonably obvious by one skilled in the art before the effective filing date of the applicant’s invention, absent evidence to the contrary, that the iron catalyst reasonably contains an iron purity of 86% or more, as claimed by the applicant, in order to obtain a highly pure hydrogen product and nanocarbons because of the entanglement with the iron catalyst.),
wherein the reactor (#3) is configured to be supplied with a raw material gas containing hydrocarbons (#13A raw city gas containing methane supplied through main raw material supply pipe #5) (see figure 1 and paragraphs [0021], [0027], [0034] and [0089]).
In regards to Claim 3, Katsumi discloses the direct decomposition device as recited in claim 1. Although Katsumi is silent in regards to wherein a specific surface area of the plurality of particles by BET method is 0.1 m2/g or more and 10 m2/g or less, or a pore specific surface area of the plurality of particles by mercury injection method is 0.01 m2/g or more and 1 m2/g or less, adjusting the specific surface area of the plurality of particles to an optimum value, such as 0.1m2/g or more and 10m2/g or less as claimed by the applicant, is obtainable by one skilled in the art through routine experimentation, in order to obtain a desired end-results, such as for improved decomposition efficiency of methane to hydrogen and carbon. See MPEP 2144.05.
In regards to Claim 6, Katsumi discloses wherein a reaction of direct decomposition of hydrocarbons into carbon and hydrogen is performed in a temperature range between 600ºC and 900ºC (see paragraph [0063]; Katsumi discloses the temperature inside the reaction tube for the direct decomposition of hydrocarbons into carbon and hydrogen is 800ºC to 900ºC, which falls inside the claimed range of between 600ºC and 900ºC, as claimed by the applicant, thereby making the claimed range prima facie obvious. See MPEP 2144.05.).
In regards to Claim 7, Katsumi discloses the direct decomposition device as recited in claim 1. Although Katsumi does not explicitly disclose wherein a partial pressure of hydrocarbons in the raw material gas is between 0.025MPa and 0.1MPa, Katsumi discloses substantially the same device and raw material gas comprising hydrocarbons, as claimed by the applicant. Therefore, it is reasonably expected, absent evidence to the contrary, that Katsumi’s raw material gas will reasonably have a partial pressure of hydrocarbons in a range of between 0.025MPa and 0.1MPa, as claimed by the applicant, as it has been held that chemical compositions and their properties as inseparable. See MPEP 2112.01.
In regards to Claim 8, Katsumi discloses further comprising a carbon removal device for removing carbon adhering to the catalyst from the catalyst (see paragraph [0068]).
In regards to Claim 9, Katsumi discloses wherein the carbon removal device is a fluidized bed forming device for forming a fluidized bed of catalyst contained in the reactor (see paragraph [0068; Katsumi discloses wherein the powder catalyst can be removed from the recovered ultra-fine carbon by oxidation methods, i.e. fluidized bed of catalysts.).
In regards to Claim 11, Katsumi discloses further comprising a reactant gas flow line (#29) through which a reactant gas containing hydrogen flows after flowing out of the reactor (#3), and a solid-gas separation device (#30) disposed in the reactant gas flow line (#29) to separate carbon from the reactant gas (see figure 1 and paragraph [0071]).
Claim 2 is rejected under 35 U.S.C. 103 as being unpatentable over Katsumi in view of Kambe et al. (US Pat. No. 6,045,769, hereinafter Kambe).
In regards to Claim 2, Katsumi discloses the direct decomposition device as recited in claim 1, but fails to disclose wherein a crystallite size of iron constituting the plurality of particles is 2nm or more and less than 60nm.
However, Kambe teaches improved catalyst particles for elemental carbon formation. The improved catalyst particles have a high degree of uniformity and have small average particles for the production of desirable small diameter carbon particles and fibers. The improved catalyst particles are contacted with a molecular stream including carbon precursors to generate an improved elemental carbon product (see column 1, lines 35-48). Nanoscale iron and iron compound particles useful as catalysts for carbon formation have a very high level of uniformity with respect to composition, crystallinity and crystal morphology. The catalyst particles include elemental iron, iron carbide or iron sulfides (see column 2, lines 43-52). The catalyst particles have an average diameter of about 5nm to about 50nm, and upon closer examination, the particles have facets corresponding to the underlying crystal lattice, and for crystalline particles, the particle size corresponds to the crystal size (see column 9, lines 9-31). The catalyst particles having an average diameter of about 5nm to about 50nm, falls inside the claimed range of from 2nm or more and less than 60nm, as claimed by the applicant, thereby making the claimed range prima facie obvious. See MPEP 2144.05.
It would have been obvious by one of ordinary skill in the art before the effective filing date of the applicant’s invention to modify the direct decomposition device as disclosed by Katsumi by substituting a known iron catalyst for another known iron catalyst having a crystallite size of iron constituting the plurality of particles of 2nm or more and less than 60nm, as claimed by the applicant, with a reasonable expectation of success, as Kambe teaches improved catalyst particles for elemental carbon formation, wherein the improved catalyst particles have a high degree of uniformity and have small average particles for the production of desirable small diameter carbon particles and fibers, whereby the improved catalyst particles are contacted with a molecular stream including carbon precursors to generate an improved elemental carbon product, wherein nanoscale iron and iron compound particles useful as catalysts for carbon formation have a very high level of uniformity with respect to composition, crystallinity and crystal morphology and have an average diameter of about 5nm to about 50nm, thereby obtaining a catalyst having small average diameters for the production of desirable small diameter carbon particles and fibers (see column 1, lines 35-48 and column 9, lines 9-31).
Claim 10 is rejected under 35 U.S.C. 103 as being unpatentable over Katsumi in view of Chen et al. (CN104998654A, relied on machine translation, hereinafter Chen).
In regards to Claim 10, Katsumi discloses the direct decomposition device as recited in claim 8, but fails to disclose wherein the carbon removal device includes: a catalyst regeneration device for regenerating part of the catalyst in the reactor; a catalyst supply line for supplying the catalyst from the reactor to the catalyst regeneration device; and a catalyst return line for returning the catalyst from the catalyst regeneration device to the reactor.
However, Chen teaches a methane catalytic cracking device for producing hydrogen and carbon. The catalyst comprises a nickel-based catalyst for catalytic methane cracking, and the nickel-based catalyst may also comprise an auxiliary metal component such as iron (see paragraphs [0022]-[0025] and [0040]). The apparatus used in a method for producing hydrogen through catalytic cracking or methane includes a high-density circulating fluidizing bed reactor, a settling tank, a regenerator, a regeneration inclined tube and a waiting inclined tube. The regenerator (#2) comprises a catalyst outlet pipe which connects to a feed pipe of the high-density circulating fluidized bed reactor (#3) through a regeneration inclined pipe (#4), and the catalyst inlet of the regenerator is connected to the catalyst outlet of the settling tank through the regeneration inclined pipe (#5) (see figure 1 and paragraph [0041]). The methane feed gas is introduced into the reactor through the feed pipe at the bottom of the high-density circulating fluidized bed reactor, and comes into contact with the catalyst in the reactor for catalytic cracking of methane to produce hydrogen and undergoes catalytic cracking reaction to obtain the generated gas including hydrogen and the deactivated catalyst. The deactivated catalyst is introduced into the regenerator through the regenerated inclined tube and an oxygen source is introduced into the regenerator for obtaining a regenerated catalyst and regenerated flue gas. The regenerated flue gas exits through the regenerated flue gas outlet at the top of the regenerator and the regenerated catalyst is fed into the high-density circulating fluidized bed reactor through the regeneration inclined tube (see paragraphs [0043]-[0046]).
It would have been obvious by one of ordinary skill in the art before the effective filing date of the applicant’s invention to modify the direct decomposition device as disclosed by Katsumi by substituting a known carbon removal device for another known carbon removal device which includes a catalyst regeneration device for regenerating part of the catalyst in the reactor, a catalyst supply line for supplying the catalyst from the reactor to the catalyst regeneration device, and a catalyst return line for returning the catalyst from the catalyst regeneration device to the reactor, as claimed by the applicant, with a reasonable expectation of success, as Chen teaches a methane catalytic cracking device for producing hydrogen and carbon, wherein the catalyst comprises a nickel-based catalyst for catalytic methane cracking, and the nickel-based catalyst may also comprise an auxiliary metal component such as iron, whereby the apparatus used in a method for producing hydrogen through catalytic cracking or methane includes a high-density circulating fluidizing bed reactor, a settling tank, a regenerator, a regeneration inclined tube and a waiting inclined tube, wherein the methane feed gas is introduced into the reactor through the feed pipe at the bottom of the high-density circulating fluidized bed reactor, and comes into contact with the catalyst in the reactor for catalytic cracking of methane to produce hydrogen and undergoes catalytic cracking reaction to obtain the generated gas including hydrogen and the deactivated catalyst, the deactivated catalyst is introduced into the regenerator through the regenerated inclined tube and an oxygen source is introduced into the regenerator for obtaining a regenerated catalyst and regenerated flue gas, and the regenerated flue gas exits through the regenerated flue gas outlet at the top of the regenerator and the regenerated catalyst is fed into the high-density circulating fluidized bed reactor through the regeneration inclined tube, thereby efficiently regenerating the catalyst for continuous hydrogen generation (see paragraphs [0043]-[0046]).
Claims 4-5 are rejected under 35 U.S.C. 103 as being unpatentable over Katsumi in view of Ibrahim et al. (“Methane Decomposition Over Iron Catalyst for Hydrogen Production” ScienceDirect, hereinafter Ibrahim).
In regards to Claim 4, Katsumi discloses the direct decomposition device as recited in claim 1, but fails to disclose wherein a pore volume of the plurality of particles is 0.01cc/g or more and 1cc/g or less.
However, Ibrahim teaches the decomposition of methane by iron catalyst to produce hydrogen and carbon. The study involved the use of different iron loadings (15-100%) supported on alumina catalysts and the yield of hydrogen production was investigated. Time on stream tests of the supported catalyst for about 4 hours at 700ºC showed the relative profiles of hydrogen production and hydrogen yield increased as the % loading of Fe was increased (see abstract). According to Table 2, the catalyst comprising 100% Fe particles has a pore volume of 0.04cm3/g (0.04cc/g) (see page 7596 and table 2), which falls inside the claimed range of between 0.01cc/g or more and 1cc/g or less, as claimed by the applicant, thereby making the claimed range prima facie obvious. See MPEP 2144.05.
It would have been obvious by one of ordinary skill in the art before the effective filing date of the applicant’s invention to modify the direct decomposition device as disclosed by Katsumi by having the plurality of iron catalyst particles to have a pore volume of 0.01cc/g or more and 1cc/g or less, as claimed by the applicant, with a reasonable expectation of success, as Ibrahim teaches the decomposition of methane by iron catalyst to produce hydrogen and carbon, wherein the study involved the use of different iron loadings (15-100%) supported on alumina catalysts and the yield of hydrogen production was investigated, wherein time on stream tests of the supported catalyst for about 4 hours at 700ºC showed the relative profiles of hydrogen production and hydrogen yield increased as the % loading of Fe was increased, whereby the catalyst comprising 100% Fe particles has a pore volume of 0.04cm3/g (0.04cc/g) (see page 7596 and table 2) and showed good yield of hydrogen production (see page 7596 and table 2 and conclusions).
In regards to Claim 5, Katsumi discloses the direct decomposition device as recited in claim 1, but fails to disclose wherein a particle size range of the plurality of particles is between 2µm and 3mm.
However, Ibrahim teaches the decomposition of methane by iron catalyst to produce hydrogen and carbon. The study involved the use of different iron loadings (15-100%) supported on alumina catalysts and the yield of hydrogen production was investigated. Time on stream tests of the supported catalyst for about 4 hours at 700ºC showed the relative profiles of hydrogen production and hydrogen yield increased as the % loading of Fe was increased (see abstract). According to Table 1, the catalyst comprising 100% Fe particles has a particle size of less than 150mesh (less than 125µm or less than 0.125mm) (see page 7595 and table 1), which falls inside the claimed range of between 2µm and 3mm, as claimed by the applicant, thereby making the claimed range prima facie obvious. See MPEP 2144.05.
It would have been obvious by one of ordinary skill in the art before the effective filing date of the applicant’s invention to modify the direct decomposition device as disclosed by Katsumi by having the plurality of iron catalyst particles to have a particle size range between 2µm to 3mm, as claimed by the applicant, with a reasonable expectation of success, as Ibrahim teaches the decomposition of methane by iron catalyst to produce hydrogen and carbon, wherein the study involved the use of different iron loadings (15-100%) supported on alumina catalysts and the yield of hydrogen production was investigated, wherein time on stream tests of the supported catalyst for about 4 hours at 700ºC showed the relative profiles of hydrogen production and hydrogen yield increased as the % loading of Fe was increased, whereby the catalyst comprising 100% Fe particles has a particle size of less than 150mesh (less than 125µm or less than 0.125mm) and showed good yield of hydrogen production (see page 7595 and table 1 and conclusions).
Conclusion
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/JELITZA M PEREZ/Primary Examiner, Art Unit 1774