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 .
Response to Arguments
Applicant’s remarks regarding the interpretation of the claim term “carbon black” are acknowledged. The Office herein cites additional evidence, Carbon Black edited by Donnet et al, to help further explain the term as it would have been understood by one of ordinary skill in the art. The term is not any carbon formed under the conditions set forth in the claims, instead it is interpreted as requiring near spherical particles of carbon of colloidal size. See e.g. Carbon Black at Introduction, p. xvii and SEM images in Chapter 5, p. 224.
In view of both Applicant’s amendment to claim 1 and the new interpretation of the claim language, all prior grounds of rejection are withdrawn since none of the references applied in the prior rejections taught both using a current density of 1-10 A/cm2 AND forming carbon black (near spherical carbon particles).
In view of both Applicant’s amendment to claim 1 and the new interpretation of the claim language, the Office conducted further search. New rejection grounds are presented below in view of Li et al (“A novel route to synthesize carbon spheres and carbon nanotubes from carbon dioxide in a molten carbonate electrolyzer”) and Licht (“Co-production of cement and carbon nanotubes with a carbon negative footprint”).
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 1-4, 9, 11-16, 19, and 20 are rejected under 35 U.S.C. 103 as being unpatentable over Li et al (“A novel route to synthesize carbon spheres and carbon nanotubes from carbon dioxide in a molten carbonate electrolyzer”) in view of Licht (“Co-production of cement and carbon nanotubes with a carbon negative footprint”) with evidence from Carbon Black (ed. by Donnet et al).
Li et al teach (see abstract, sections 2, 3.1 and 3.2, fig. 2(c) and fig. 3) a method for the production of carbon spheres comprising immersing an anode and a cathode in a molten carbonate electrolyte that included dissolved CO2, applying an electric current to the cathode and the anode and forming the carbon spheres on the cathode.
The SEM images of the carbon product show clusters of carbon spheres, where the individual sphere particles having diameters of less than 1 μm.
Carbon Black shows SEM images of carbon black having a very similar shape, size and clusters of spheres that constitute carbon black.
Therefore, one of ordinary skill in the art at the time of filing would have classified the carbon sphere product of Li et al as being carbon black due to the nearly identical nature of the particulate carbon.
Li et al fail to teach that the applied current density was in the range of 1-10 A/cm2.
In the same field of forming particulate carbon by electrolysis of carbon dioxide in a molten carbonate electrolyte, Licht teaches (see fig. 3) that selection of the particular conditions of the electrolysis could result in different allotropes of carbon, including ~1μm spherical carbon on a galvanized steel cathode without the presence of nickel, copper, cobalt or iron. Licht also teaches (see paragraph spanning pages 387 and 388 and fig. 12) that high current densities in excess of 1 A/cm2 resulted in fast elemental carbon formation.
Therefore, given the known formation of carbon black using the conditions set forth by Li et al and the demonstration from Licht that higher current density were possible for forming elemental carbon in a molten carbonate electrolysis suggested to one of ordinary skill in the art to conduct the process of Li et al at higher current densities to increase the rate of reaction as suggested by Licht. Absent a showing of unexpected results, conducting routine experimentation on the process taught by Li et al by using larger current densities as suggested by Licht would have been well within the ordinary level of skill in the art.
Regarding claim 2, Licht teaches using current densities in excess of 1 A/cm2. Absent a showing of unexpected results, it would have been obvious to one of ordinary skill in the art to have applied as high a current density as possible since the current was directly proportional to the rate of reaction.
Regarding claim 3, 4, 11 and 12, Li et al teach using a galvanized iron cathode (conductive metal substrate with zinc (i.e. passivating) layer).
Regarding claim 9, Li et al teach using a metal (nickel) anode.
Regarding claim 13, Li et al teach (see section 2) conducting the electrolysis at 750°C.
Regarding claims 14 and 15, Li et al teach conducting the electrolysis using a molten carbonate electrolyte that was a mixture one or more of lithium carbonate, calcium carbonate, sodium carbonate, potassium carbonate and barium carbonate.
Regarding claim 16, Li et al teach (see paragraph spanning pages 211 and 212) using a eutectic mixture of lithium carbonate with either sodium carbonate or potassium carbonate.
Regarding claim 19, Li et al show (see SEM images in fig. 3) that the carbon particles had an average particles size of ~800nm (estimated from fig. 3(d)).
Regarding claim 20, Li et al teach (see caption of fig. 7) that the carbon product may be collected from the cathode.
Claims 5-8 and 10 are rejected under 35 U.S.C. 103 as being unpatentable over Li et al (“A novel route to synthesize carbon spheres and carbon nanotubes from carbon dioxide in a molten carbonate electrolyzer”) in view of Licht (“Co-production of cement and carbon nanotubes with a carbon negative footprint”) as applied to claim 3 or 9 above, and further in view of Douglas et al (WO 2018/075123).
Regarding claims 5-8, Li et al teach using a zinc metal passivation layer on the cathode.
Douglas et al teach (see abstract, page 10, line 32 to page 11, line 17, page 12, lines 22- 28, page 14, lines 4-6 and Example 1 spanning pages 19-27) that electrodes, including both anode and cathode, in a molten carbonate electrolysis process for formation of elemental carbon may be coated with a passivation layer such as Al2O3, TiO2, MgO, TiN, or VN deposited by ALD may substantially prevent the migration of small amounts of metals from the electrode which would alter the nucleation characteristics of the carbon on the cathode surface.
Therefore, it would have been obvious to one of ordinary skill in the art at the time of filing to have utilized a passivated cathode according to the suggestion of Douglas et al for the cathode of Li et al for the purpose of preventing migration of unwanted metals from the interior of the cathode which would have altered the nucleation characteristics of the carbon on the cathode surface.
Regarding claim 10, note that Li et al teach (see left hand column on page 210) that the anode reaction was formation of oxygen gas.
Douglas et al teach (see page 11, lines 25-28) utilizing a passivated steel anode.
Therefore, absent a showing of unexpected results, it would have been obvious to one of ordinary skill in the art to have substituted other known materials for the construction of the oxygen evolving anode of Li et al as taught by Douglas et al. Steel was recognized as suitable for this purpose by Douglas et al.
Claims 17, 18, 21 and 22 are rejected under 35 U.S.C. 103 as being unpatentable over Li et al (“A novel route to synthesize carbon spheres and carbon nanotubes from carbon dioxide in a molten carbonate electrolyzer”) in view of Licht (“Co-production of cement and carbon nanotubes with a carbon negative footprint”) as applied to claims 1 or 20 above, and further in view of Elgammal et al (US 2014/0202874 A1).
Regarding claim 17, Li et al teach providing an atmosphere of carbon dioxide into a sealed reactor, and thus failed to teach providing a flow of carbon dioxide into the reactor.
In the same field of forming particulate carbon by electrolysis of carbon dioxide in a molten carbonate electrolyte, Elgammal et al teach (see fig. 2A, paragraph [0082]) that the carbon dioxide to be electrolyzed into carbon may be injected into the molten carbonate electrolyte.
Therefore, it would have been obvious to one of ordinary skill in the art at the time of filing to have provided a continuous flow of carbon dioxide injected into the molten carbonate as suggested by Elgammal et al to convert the batch process of Li et al into a continuous process allowing for greater formation of carbon from the carbon dioxide.
Regarding claim 18, Li et al fail to teach the origin of the carbon dioxide.
In the same field of forming particulate carbon by electrolysis of carbon dioxide in a molten carbonate electrolyte, Elgammal et al teach (see paragraph [0054]) obtaining the carbon dioxide as an exhaust from an industrial process, e.g. petroleum recovery.
Therefore, it would have been obvious to one of ordinary skill in the art at the time of filing to have utilized carbon dioxide exhausted from an industrial process in the process of Li et al to prevent the release of the carbon dioxide into the atmosphere.
Regarding claims 21 and 22, Li et al fail to describe the details of the carbon collection process.
In the same field of forming particulate carbon by electrolysis of carbon dioxide in a molten carbonate electrolyte, Elgammal et al teach (see fig. 2A, paragraphs [0065] and [0082]) collecting the carbon from the cathode by (1) immersing the cathode in the molten electrolyte (i.e. “a fluid”), removing the carbon from the surface of the cathode by a method including dislodging by turbulent electrolyte flow (i.e. “slough”, claim 21) or scraping or sonicating the surface of the cathode (claim 22), and collecting the fluid and the carbon from the bottom of the reactor and/or disperse the carbon in the fluid, and filtering the fluid to separate the carbon from the fluid.
Therefore, it would have been obvious to one of ordinary skill in the art at the time of filing to have utilized the collection process taught by Elgammal et al for recovering the carbon product of Li et al because Elgammal et al show that the claimed steps resulted in recovery of the carbon product formed on the cathode.
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.
Any inquiry concerning this communication or earlier communications from the examiner should be directed to HARRY D WILKINS III whose telephone number is (571)272-1251. The examiner can normally be reached M-F 9:30am -6:00pm.
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/HARRY D WILKINS III/Primary Examiner, Art Unit 1794