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 .
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.
Information Disclosure Statements
The Information Disclosure Statement filed on 11 March 2024, with 47 references, has been received and considered by the Examiner.
The subsequent IDS submission of 18 June 2025 includes 8 additional references, bringing the total cumulative references above 50. Consequently, an IDS size fee under 37 CFR 1.17(v)(1) is required with this submission and the submission fails to comply with the provisions of 37 CFR 1.98(a)(4) because it lacks the appropriate size fee assertion. It has been placed in the application file, but the information referred to therein has not been considered as to the merits.
The additional IDS filings of 4 September 2025, 6 January 2026, and 12 March 2026 have also not been placed in the file but not yet considered as to the merits.
Preliminary Amendment
Applicant’s preliminary amendment to the claims and specification filed on 11 March 2024 have been entered and considered for this action.
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.
Claims 1-4, 6, 11-17, and 19-20 are rejected under 35 U.S.C. 103 as being unpatentable over Kauppinen et al. (US 2014/0348721 A1) in view of Chen et al. (WO 2020/253104 A1) and Guo et al. (Plasma Science and Technology, 2010, 12(2), 188-199). The provided English machine translation of Chen (WO 2020/253104 A1) is relied upon in the analysis below.
Regarding claim 1, Kauppinen teaches a method for producing carbon nanotubes, the method comprising vaporizing a catalyst raw material using a plasma (arc discharge method; [0006]), condensing a catalyst vapor in a quenching zone to prepare a particle catalyst (evaporation and subsequent vapor nucleation followed by growth of particles due to vapor condensation and cluster coagulation; [0006]), introducing a catalyst particles and a source gas into a CVD reactor (CNT reactor) and synthesizing carbon nanotubes in the CVD reactor ([0010]-[0013]). Kauppinen also teaches that catalyst particle size is important ([0132]) and that the catalyst particles used in their method are nanoparticles (nanosized catalyst iron particles; [0158] and Fig 10(c)).
Kauppinen further teaches that the nanoparticle catalyst particles can be prepared by any available method which either inherently produces particles with a narrow distribution of properties or which can be pre-classified prior to CNT synthesis ([0006]).
Kauppinen does not specifically teach a plasma torch or transferring the catalyst vapor to a quenching zone by a plasma flow.
However, Chen also describes a method of producing carbon nanotubes comprising vaporizing a catalyst raw material using a plasma torch to form a catalyst vapor (catalyst evaporation chamber adopts a high-temperature physical evaporation method; the high-temperature physical evaporation method is a high-temperature electric arc, a high-temperature radio frequency plasma, or a high-temperature microwave plasma; [0038] and Fig 1., element 3, high temperature evaporation spray gun), introducing the nanoparticle catalyst and a source gas into a CVD reactor and synthesizing carbon nanotubes in the CVD reactor (catalyst directly enters the chemical vapor deposition chamber through the connecting channel. Simultaneously, a gas path system introduces carrier gas and carbon source gas through the catalyst evaporation chamber and the chemical vapor deposition chamber, respectively, allowing the catalyst to react with the high-temperature cracked organic carbon source to generate carbon nanotubes; [0007]).
Additionally, Guo teaches that nanoparticles (ultrafine nanopowders) can be prepared by vaporizing a catalyst raw material using a plasma torch to form a vapor, transferring the vapor to a quenching zone by plasma flow, and condensing the catalyst vapor in the quenching zone to prepare nanoparticles (the material is first heated up and evaporated in the plasma, and the resultant vapors are subsequently subjected to very rapid quenching in the quench/reaction zone where homogeneous nucleation leads to the formation of a very fine aerosol in the reactor; Section 2.2, ¶ 1 and Fig. 9). Guo further teaches that this method is able to produce uniform nanopowders with control of particle size (Section 5, ¶ 1).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to produce the nanoparticle catalysts used in the method of Kauppinen by vaporizing a catalyst raw material using a plasma troch to form a catalyst vapor, as taught by Chen and Guo, and to transfer the catalyst vapor to a quenching zone by plasma flow and to condense the catalyst vapor in the quenching zone to prepare the nanoparticle catalyst, as taught by Guo. One of ordinary skill in the art would have been motivated to do so because Chen teaches that evaporation by plasma torch is able to generate catalysts for nanotube synthesis and because Guo teaches that the quenching step is able to afford control over particle size, which Kauppinen teaches is important.
Regarding claim 2, modified Kauppinen teaches the method of claim 1, where Kauppinen teaches the catalyst being “nanosized” ([0158]), which may be interpreted as having an average size of 100 nm or less.
Kauppinen also teaches that the diameter and chirality of the CNTs produced via catalysts are largely determined by the properties of the catalyst particles, in particular the catalyst size ([0005]). And, Guo teaches that their method of generating nanoparticles produces metal nanoparticles of averages sizes between 20-200 nm in size (Table 3), which overlaps with the particle sizes instantly claimed.
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to optimize the average size of the nanoparticles produced by the method of Guo, including into the instantly claimed range of 100 nm or less. One of ordinary skill in the art would have been motivated to do so in order to tune the diameter of the nanotubes produced, as taught by Kauppinen.
Regarding claim 3, modified Kauppinen teaches the method of claim 1, where Guo (Fig. 13) and Chen (high temperature radio frequency plasma; [0011] and [0054]) each teach the plasma torch being an inductively coupled RF plasma torch.
Regarding claim 4, modified Kauppinen teaches the method of claim 1, where Kauppinen ([0056] and Example 1) and Guo ([0054]) each teach the catalyst raw material comprising iron (Fe).
Regarding claim 6, modified Kauppinen teaches the method of claim 1, where Kauppinen ([0056] and Example 1) and Guo ([0046] and [0054]) each teach the catalyst raw material is iron metal, a solid.
Regarding claim 11, modified Kauppinen teaches the method of claim 1, where Kauppinen teaches the source gas (carbon source) is carbon monoxide (CO; Example 1, [0148]).
Regarding claim 12, modified Kauppinen teaches the method of claim 1, where Kauppinen teaches that the nanoparticle catalyst is in an aerosol state ( first step of the method is to obtain aerosolized pre-made catalyst particles; [0051]).
Regarding claim 13, modified Kauppinen teaches the method of claim 1, where Kauppinen further teaches introducing a sulfur-containing compound (thiophene) as a cocatalyst into the CVD reactor (In the CNT reactor, the flow carrying the catalyst particles was mixed with the CO flow containing vapors of thiophene; [0185]).
Regarding claim 14, modified Kauppinen teaches the method of claim 1, where Kauppinen teaches that the nanoparticle catalyst and source gas are introduced to the CVD reactor (step S4) along with a carrier gas of nitrogen/hydrogen (metal particles produced … were carried into the CNT reactor with nitrogen/hydrogen; [0155]).
Regarding claim 15, modified Kauppinen teaches the method of claim 1, where Kauppinen teaches the CVD reactor has a maximum wall temperature of most preferable approximately 1200 °C ([0102]).
Regarding claim 16, modified Kauppinen teaches the method of claim 1, where Kauppinen teaches the nanotubes may be single walled or multi-walled ([0002]).
Regarding claim 17, modified Kauppinen teaches the method of claim 1, where Kauppinen teaches that the method may be performed continuously (The present invention includes one or more CNT reactors, which can allow continuous…production of CNTs; [0018]).
It is additionally noted that the courts have held that continuous operations are obvious in light of a batch process in the prior art. In re Dilnot, 319 F.2d 188, 138 USPQ 248 (CCPA 1963). MPEP 2144.04(V)(E).
Regarding claim 19, modified Kauppinen teaches the method of claim 13, where Kauppinen teaches that a role of the cocatalyst is to supply sulfur to the catalyst particles and to lower the melting temperature of the catalyst particles ([0185]).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to optimize the weight ratio of catalyst to cocatalyst by routine experimentation, including into the claimed range of 1:1 to 100:1. One of ordinary skill in the art would have been motivated to do so in order to achieve the desired degree of melting temperature reduction in the catalyst particles.
It is also noted that the courts have found that “where 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.” In re Aller, 220 F.2d 454, 456, 105 USPQ 233, 235 (CCPA 1955). See MPEP 2144.05 II. Therefore, the claimed ranges merely represent an obvious variant and/or routine optimization of the teachings in the cited prior art.
Regarding claim 20, modified Kauppinen teaches the method of claim 13, where the sulfur-containing compound is thiophene ([0064] and [0185]).
Claim 5 is rejected under 35 U.S.C. 103 as being unpatentable over Kauppinen et al. (US 2014/0348721 A1) in view of Chen et al. (WO 2020/253104 A1) and Guo et al. (Plasma Science and Technology, 2010, 12(2), 188-199), as applied to claim 1 above, and further in view of Moravsky et al. (US 2012/0107610 A1). The provided English machine translation of Chen (WO 2020/253104 A1) is relied upon in the analysis below.
Regarding claim 5, modified Kauppinen teaches the method of claim 1, but none of Kauppinen, Chen, or Guo teach the catalyst raw material further comprising sulfur or a sulfide of any metals.
However, Moravsky also teaches the production of carbon nanotubes using a plasma-assisted CVD method ([0079]) and Moravsky further teaches that it is advantageous to include sulfur along with the iron powder when preparing the catalysts used in their system in order to increase the yield of carbon nanotubes ([0062] and [0085]).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to use in the method of modified Kauppinen a catalyst raw material comprising sulfur or a sulfide of iron, cobalt, or nickel, as taught by Moravsky. One of ordinary skill in the art would have been motivated to do so because Moravsky teaches that the combination of sulfur with the metals iron, cobalt, and nickel leads to increase yield of nanotubes.
Claim 7 is rejected under 35 U.S.C. 103 as being unpatentable over Kauppinen et al. (US 2014/0348721 A1) in view of Chen et al. (WO 2020/253104 A1) and Guo et al. (Plasma Science and Technology, 2010, 12(2), 188-199), as applied to claim 1 above, and further in view of Boulos et al. (US 2007/0029291 A1; hereinafter “Boulos ‘291’). The provided English machine translation of Chen (WO 2020/253104 A1) is relied upon in the analysis below.
Regarding claim 7, modified Kauppinen teaches the method of claim 1, where Guo teaches that raw material being vaporized are supplied as powder that must be well dispersed during injection to ensure production of uniform nanoparticles (powders were introduced into plasma using different injection probes; Section 4.3 and 5). Guo further teaches examples where the powders being injected are of 10-400 μm size (for Mo, Table 4), or are less than 150 μm (-100 mesh for Ti, Table 4). Guo does not specifically recite an average particle size of the catalyst raw material.
However, Boulos ‘291 describes the same general plasma synthesis of nanopowders (abstract) as Guo (they are each inventors/authors on both disclosures) and Boulos ‘291 further teaches that the particle raw materials from which the nanoparticles are synthesized are micron-sized metallic powders ([0046]), which are interpreted as having average sizes from ~1 μm to ~100 μm, which overlaps with the instantly claimed range of 5 μm to 100 μm.
Additionally, based upon Guo’s teaching on the importance of well dispersed raw materials and these materials being completely evaporated (Section 4.3), it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to optimize by routine experimentation the average particle size of the micron-sized metallic powder taught by Boulos ‘291, including into the instantly claimed range of 5 μm to 100 μm. One of ordinary skill in the art would have been motivated to do so in order to ensure that the powders become well dispersed and completely evaporated, as taught by Guo.
It is noted that the courts have stated where the claimed ranges “overlap or lie inside the ranges disclosed by the prior art” a prima facie case of obviousness exists (see 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); Titanium Metals Corp. of America v. Banner, 778 F2d 775. 227 USPQ 773 (Fed. Cir. 1985) (see MPEP 2144.05.01). Therefore, the claimed range of average particle size in the raw material powder merely represents an obvious variant and/or routine optimization of the micron-sized powders taught by the cited prior art.
Claims 8-10 and 18 are rejected under 35 U.S.C. 103 as being unpatentable over Kauppinen et al. (US 2014/0348721 A1) in view of Chen et al. (WO 2020/253104 A1) and Guo et al. (Plasma Science and Technology, 2010, 12(2), 188-199), as applied to claim 1 above, and further in view of Boulos et al. (US 2007/0221635 A1; hereinafter “Boulos ‘635”). The provided English machine translation of Chen (WO 2020/253104 A1) is relied upon in the analysis below.
Regarding claim 8, modified Kauppinen teaches the method of claim 1, where Guo teaches the use of a quenching zone, but neither Guo nor Kauppinen teach the quenching zone comprising a first quenching zone and a second quenching zone.
However, Boulos ‘635 describes the same general plasma synthesis of nanopowders as Guo (they are each inventors/authors on both disclosures) and Boulos ‘635 further teaches that the quenching chamber may comprise a first quenching zone (hot quench section) and a second quenching zone (cold quench section), where the catalyst vapor flows from the first quenching zone to the second quenching zone (the quenching chamber comprising an upstream hot quench section and a downstream cold quench section; [0012]). Boulos ‘635 also teaches that by independently controlling the temperature and chemical composition of the renewable gaseous condensation front [generated in the hot quench zone], excellent control of the chemistry, morphology, uniformity and particle size distribution of the resulting nanopowder could be achieved ([0013]).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to use in the method of modified Kauppinen a quenching zone comprised of a first quenching zone and a second quenching zone, as taught by Boulos ‘635. One of ordinary skill in the art would have been motivated to do so because Boulos ‘635 teaches that independent control of the temperature in the two quenching zones allows for excellent control over uniformity and particle size, two features identified as important by Kauppinen for their nanoparticle catalysts ([0006] and [0132]).
Regarding claim 9, modified Kauppinen teaches the method of claim 8, where Boulos also teaches injecting an inert gas (argon) into the first quenching zone and the second quenching zone ([0048]).
Regarding claim 10, modified Kauppinen teaches the method of claim 8, where Kauppinen teaches hydrogen in the carrier gas, which will be injected into the second quenching zone along with the catalyst nanoparticles.
Regarding claim 18, modified Kauppinen teaches the method of claim 1, where Kauppinen teaches that the size and distribution of the nanoparticle catalyst are important parameters of the method ([0006] and [0132]). None of Kauppinen, Chen, or Guo teach the time over which the catalyst is transferred prior to being introduced into the quenching zone.
However, Boulos ‘635 teaches that the residence time has an effect on particle nucleation and growth and that control of this variable may afford control over the nanopowder particle size distribution ([0006]).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to optimize by routine experimentation the time between when the catalyst raw material is vaporized and when it quenched, corresponding to the time of transferring, in the method of Kauppinen. One of ordinary skill in the art would have been motivated to do so in order to control the size distribution of the nanoparticle catalyst, as taught by Boulos ‘635, because Kauppinen teaches that size and size distribution are important parameters in their method.
Claim 19 is rejected under 35 U.S.C. 103 as being unpatentable over Kauppinen et al. (US 2014/0348721 A1) in view of Chen et al. (WO 2020/253104 A1) and Guo et al. (Plasma Science and Technology, 2010, 12(2), 188-199), as applied to claim 1 above, and further in view of Lee et al. (KR 2003 0080521A). The provided English machine translations of Chen (WO 2020/253104 A1) and Lee (KR 2003 0080521A) are relied upon in the analysis below.
Regarding claim 19, modified Kauppinen teaches the method of claim 13, where Kauppinen teaches that a role of the cocatalyst (thiophene) is to supply sulfur to the catalyst particles and to lower the melting temperature of the catalyst particles ([0185]). Kauppinen does not teach a specific ratio of the nanoparticle catalyst to the cocatalyst.
However, Lee also teaches a method for synthesizing carbon nanotubes using plasma (title and [13]) where an iron catalyst is used in combination with a thiophene cocatalyst ([28]). Lee further teaches that the amount of catalyst is preferably 2 to 8 weight% relative to the hydrocarbon being used while the amount of thiophene is preferably 0.1 to 3 % relative to the hydrocarbon ([27]-[28]). This corresponds to a ratio of catalyst to cocatalyst of 80:1 to 0.7:1, a range which overlaps significantly with the instantly claimed range.
Furthermore, Lee also teaches an example where the amount of iron pentacarbonyl catalyst precursor is 25 mg/min and the amount of thiophene cocatalyst is 2.5 mg/min ([47]), for a ratio of 10:1. If only the iron mass in iron pentacarbonyl is considered, then the ratio is 2.8:1. Each of these ratios fall in the claimed range of 1:1 to 100:1.
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to use in the method of modified Kauppinen a weight ratio of iron catalyst to thiophene cocatalyst of 2.8:1, as taught by Lee. One of ordinary skill in the art would have been motivated to do so in order because Lee teaches that such a ratio is appropriate effective for promoting nanotube growth without becoming an impurity in the nanotubes produced ([28]).
Double Patenting
The nonstatutory double patenting rejection is based on a judicially created doctrine grounded in public policy (a policy reflected in the statute) so as to prevent the unjustified or improper timewise extension of the “right to exclude” granted by a patent and to prevent possible harassment by multiple assignees. A nonstatutory double patenting rejection is appropriate where the conflicting claims are not identical, but at least one examined application claim is not patentably distinct from the reference claim(s) because the examined application claim is either anticipated by, or would have been obvious over, the reference claim(s). See, e.g., In re Berg, 140 F.3d 1428, 46 USPQ2d 1226 (Fed. Cir. 1998); In re Goodman, 11 F.3d 1046, 29 USPQ2d 2010 (Fed. Cir. 1993); In re Longi, 759 F.2d 887, 225 USPQ 645 (Fed. Cir. 1985); In re Van Ornum, 686 F.2d 937, 214 USPQ 761 (CCPA 1982); In re Vogel, 422 F.2d 438, 164 USPQ 619 (CCPA 1970); In re Thorington, 418 F.2d 528, 163 USPQ 644 (CCPA 1969).
A timely filed terminal disclaimer in compliance with 37 CFR 1.321(c) or 1.321(d) may be used to overcome an actual or provisional rejection based on nonstatutory double patenting provided the reference application or patent either is shown to be commonly owned with the examined application, or claims an invention made as a result of activities undertaken within the scope of a joint research agreement. See MPEP § 717.02 for applications subject to examination under the first inventor to file provisions of the AIA as explained in MPEP § 2159. See MPEP § 2146 et seq. for applications not subject to examination under the first inventor to file provisions of the AIA . A terminal disclaimer must be signed in compliance with 37 CFR 1.321(b).
The filing of a terminal disclaimer by itself is not a complete reply to a nonstatutory double patenting (NSDP) rejection. A complete reply requires that the terminal disclaimer be accompanied by a reply requesting reconsideration of the prior Office action. Even where the NSDP rejection is provisional the reply must be complete. See MPEP § 804, subsection I.B.1. For a reply to a non-final Office action, see 37 CFR 1.111(a). For a reply to final Office action, see 37 CFR 1.113(c). A request for reconsideration while not provided for in 37 CFR 1.113(c) may be filed after final for consideration. See MPEP §§ 706.07(e) and 714.13.
The USPTO Internet website contains terminal disclaimer forms which may be used. Please visit www.uspto.gov/patent/patents-forms. The actual filing date of the application in which the form is filed determines what form (e.g., PTO/SB/25, PTO/SB/26, PTO/AIA /25, or PTO/AIA /26) should be used. A web-based eTerminal Disclaimer may be filled out completely online using web-screens. An eTerminal Disclaimer that meets all requirements is auto-processed and approved immediately upon submission. For more information about eTerminal Disclaimers, refer to www.uspto.gov/patents/apply/applying-online/eterminal-disclaimer.
Claims 1, 8-10, and 16-17 are provisionally rejected on the ground of nonstatutory double patenting as being unpatentable over claims 1-12 of copending Application No. 18/688,960. Although the claims at issue are not identical, they are not patentably distinct from each other because claim 1 of the ‘960 application recites an apparatus configured for producing carbon nanotubes having elements configured to perform all the steps of the instant claim 1. Therefore, it would have been obvious to perform the method of the instant claim 1 using the apparatus of the ‘960 patent.
Additionally, claims 2-5 of the ‘960 application recite elements of the apparatus that render instant claims 8-10 obvious. Furthermore, claims 10 and 11 recite the further limitations of instant claims 16 and 17.
This is a provisional nonstatutory double patenting rejection because the patentably indistinct claims have not in fact been patented.
Claims 2, 4, 6, 11-15, and 19-20 are provisionally rejected on the ground of nonstatutory double patenting as being unpatentable over claims 1-12 of copending Application No. 18/688,960, as applied to claim 1 above, and further in view of Kauppinen et al. (US 2014/0348721 A1).
Regarding instant claim 2, the method of claim 1 is obvious over the claims of the ‘960 application, and Kauppinen teaches the catalyst being “nanosized” ([0158]), which may be interpreted as having an average size of 100 nm or less.
Kauppinen also teaches that the diameter and chirality of the CNTs produced via catalysts are largely determined by the properties of the catalyst particles, in particular the catalyst size ([0005]). And, Guo teaches that their method of generating nanoparticles produces metal nanoparticles of averages sizes between 20-200 nm in size (Table 3), which overlaps with the particle sizes instantly claimed.
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to optimize the average size of the nanoparticles produced using the apparatus of the ‘960 application including into the instantly claimed range of 100 nm or less. One of ordinary skill in the art would have been motivated to do so in order to tune the diameter of the nanotubes produced, as taught by Kauppinen.
Regarding instant claims 4 and 6, the method of claim 1 is obvious over the claims of the ‘960 application, and Kauppinen teaches the catalyst for a similar method each teach the catalyst raw material comprising iron metal, a solid (Fe; [0056] and Example 1).
Therefore, it would have been obvious to use iron as the catalyst raw material in the method performed using the apparatus of the ‘960 application. One of ordinary skill in the art would have been motivated to do so because Kauppinen teaches that iron is an effective catalyst for preparing nanotubes using a similar method.
Regarding instant claim 11, the method of claim 1 is obvious over the claims of the ‘960 application, and Kauppinen teaches the source gas (carbon source) used in an analogous method is carbon monoxide (CO; Example 1, [0148]).
Therefore, it would have been obvious to use carbon monoxide as source gas in the method performed using the apparatus of the ‘960 application. One of ordinary skill in the art would have been motivated to do so because Kauppinen teaches that carbon monoxide is an effective catalyst for preparing nanotubes using a similar method.
Regarding instant claim 12, the method of claim 1 is obvious over the claims of the ‘960 application, and Kauppinen teaches that in an analogous method utilizing preformed nanoparticle catalysts that the nanoparticle catalyst is in an aerosol state (first step of the method is to obtain aerosolized pre-made catalyst particles; [0051]).
Therefore, it would have been obvious to use nanoparticle catalysts in an aerosol state in the method performed using the apparatus of the ‘960 application. One of ordinary skill in the art would have been motivated to do so because Kauppinen teaches that iron is an effective catalyst for preparing nanotubes using a similar method.
Regarding instant claims 13 and 20, the method of claim 1 is obvious over the claims of the ‘960 application, and Kauppinen teaches that in an analogous method utilizing preformed nanoparticle catalysts that a sulfur-containing compound, thiophene, can be introduced into the CVD reactor as a cocatalyst (In the CNT reactor, the flow carrying the catalyst particles was mixed with the CO flow containing vapors of thiophene; [0185]).
Therefore, it would have been obvious to introduce thiophene into the CVD reactor in the method performed using the apparatus of the ‘960 application. One of ordinary skill in the art would have been motivated to do so because Kauppinen teaches that such a compound can act as a promoter for synthesizing carbon nanotubes ([0064] and [0185]).
Regarding instant claim 14, the method of claim 1 is obvious over the claims of the ‘960 application, and Kauppinen teaches that in an analogous method utilizing preformed nanoparticle catalysts that the nanoparticle catalyst and source gas are introduced to the CVD reactor (step S4) along with a carrier gas of nitrogen/hydrogen (metal particles produced … were carried into the CNT reactor with nitrogen/hydrogen; [0155]).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to use in the method performed using the apparatus of the ‘960 application a carrier gas comprised of nitrogen and hydrogen, as taught by Kauppinen. One of ordinary skill in the art would have been motivated to do so because Kauppinen teaches that such a carrier gas is effective at transporting the catalysts and source gas.
Regarding instant claim 15, the method of claim 1 is obvious over the claims of the ‘960 application, and Kauppinen teaches an analogous method where the CVD reactor has a maximum wall temperature of most preferable approximately 1200 °C ([0102]).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to use in the method performed using the apparatus of the ‘960 application a CVD reactor with a temperature of 1200 °C, as taught by Kauppinen. One of ordinary skill in the art would have been motivated to do so because Kauppinen teaches that such a temperature is effective at producing nanotubes in an analogous method.
Regarding instant claim 19, claim 13 is obvious over the claims of the ‘960 application in view of Kauppinen, as analyzed above, where Kauppinen teaches that a role of the cocatalyst is to supply sulfur to the catalyst particles and to lower the melting temperature of the catalyst particles ([0185]).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to optimize the weight ratio of catalyst to cocatalyst by routine experimentation, including into the claimed range of 1:1 to 100:1. One of ordinary skill in the art would have been motivated to do so in order to achieve the desired degree of melting temperature reduction in the catalyst particles.
It is also noted that the courts have found that “where 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.” In re Aller, 220 F.2d 454, 456, 105 USPQ 233, 235 (CCPA 1955). See MPEP 2144.05 II. Therefore, the claimed ranges merely represent an obvious variant and/or routine optimization of the teachings method suggested by the ‘960 application.
This is a provisional nonstatutory double patenting rejection.
Claims 3 and 7 are provisionally rejected on the ground of nonstatutory double patenting as being unpatentable over claims 1-12 of copending Application No. 18/688,960, as applied to claim 1 above, and further in view of Boulos et al. Boulos et al. (US 2007/0029291 A1; hereinafter “Boulos ‘291’).
Regarding instant claim 3, the claims of the ‘970 application render the method of claim 1 obvious, but they do not specify that the plasma torch is an inductively coupled RF thermal plasma torch.
However, Boulos ‘291 teaches that raw materials can be vaporized and quenched as nanopowders with a plasma torch and the plasma torch can be an inductively coupled RF thermal plasma torch [0035]).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to use as the plasma torch in the method suggested by the ‘970 application an inductively coupled RF thermal plasma torch. One of ordinary skill in the art would have been motivated to do so because Boulos ‘291 teaches that such a troch is effective at carrying out the same operation required by the plasma torch of the ‘970 application.
Regarding instant claim 7, the claims of the ‘970 application suggest the method of instant claim 6, as analyzed above, but they do specify the size of the powders being vaporized.
However, Boulos ‘291 describes the same general plasma vaporization and quenching to form nanopowders (abstract) and Boulos ‘291 further teaches that the particle raw materials from which the nanoparticles are synthesized are micron-sized metallic powders ([0046]), which are interpreted as having average sizes from ~1 μm to ~100 μm, which overlaps with the instantly claimed range of 5 μm to 100 μm.
It is noted that the courts have stated where the claimed ranges “overlap or lie inside the ranges disclosed by the prior art” a prima facie case of obviousness exists (see 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); Titanium Metals Corp. of America v. Banner, 778 F2d 775. 227 USPQ 773 (Fed. Cir. 1985) (see MPEP 2144.05.01). Therefore, the claimed range of average particle size in the raw material powder merely represents an obvious variant and/or routine optimization of the micron-sized powders taught by the cited prior art.
This is a provisional nonstatutory double patenting rejection.
Claim 5 is provisionally rejected on the ground of nonstatutory double patenting as being unpatentable over claims 1-12 of copending Application No. 18/688,960, as applied to claim 1 above, and further in view of Moravsky et al. (US 2012/0107610 A1).
Regarding instant claim 5, the claims of the ‘970 application render the method of claim 1 obvious, but they do not suggest the catalyst raw material further comprising sulfur or a sulfide of any metals.
However, Moravsky also teaches the production of carbon nanotubes using a plasma-assisted CVD method ([0079]) and Moravsky further teaches that it is advantageous to include sulfur along with the iron powder when preparing the catalysts used in their system in order to increase the yield of carbon nanotubes ([0062] and [0085]).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to use in the method suggested by the ‘970 application a catalyst raw material comprising sulfur or a sulfide of iron, cobalt, or nickel, as taught by Moravsky. One of ordinary skill in the art would have been motivated to do so because Moravsky teaches that the combination of sulfur with the metals iron, cobalt, and nickel leads to increase yield of nanotubes.
This is a provisional nonstatutory double patenting rejection.
Claim 18 is provisionally rejected on the ground of nonstatutory double patenting as being unpatentable over claims 1-12 of copending Application No. 18/688,960, as applied to claim 1 above, and further in view of Kauppinen et al. (US 2014/0348721 A1) and Boulos et al. (US 2007/0221635 A1; hereinafter “Boulos ‘635”).
Regarding instant claim 18, the claims of the ‘970 application render the method of claim 1 obvious, but they do not suggest the time of transferring.
However, Kauppinen also teaches a method of preparing carbon nanotubes using per-formed catalysts and further teaches that the size and distribution of the nanoparticle catalyst are important parameters of the method ([0006] and [0132]).
Additionally, Boulos ‘635 teaches that the residence time has an effect on particle nucleation and growth and that control of this variable may afford control over the nanopowder particle size distribution ([0006]).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to optimize by routine experimentation the time between when the catalyst raw material is vaporized and when it quenched, corresponding to the time of transferring, in the method suggested by the ‘970 application. One of ordinary skill in the art would have been motivated to do so in order to control the size distribution of the nanoparticle catalyst, as taught by Boulos ‘635, because Kauppinen teaches that size and size distribution are important parameters in the synthesis of carbon nanotubes.
This is a provisional nonstatutory double patenting rejection.
Conclusion
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/NICHOLAS A. PIRO/Assistant Examiner, Art Unit 1738
/PAUL A WARTALOWICZ/Primary Examiner, Art Unit 1735
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