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 Status
Claims 1-17 are currently pending.
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(b):
(b) CONCLUSION.—The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the inventor or a joint inventor regards as the invention.
The following is a quotation of 35 U.S.C. 112 (pre-AIA ), second paragraph:
The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the applicant regards as his invention.
Claim 1-17 are rejected under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), second paragraph, as being indefinite for failing to particularly point out and distinctly claim the subject matter which the inventor or a joint inventor (or for applications subject to pre-AIA 35 U.S.C. 112, the applicant), regards as the invention.
Claim 1 requires “A method of synthesizing an ultrafine nano-alloy” but then requires “at least one metal salt.” As the claim is drawn to forming an alloy, requiring two or more metal elements, yet may comprise a single metal salt, it is unclear if such a single metal salt is a compound or complex comprising two or more metal elements, or whether the claim intends to also encompass forming nanoparticles of a single metal element. Claims 2-10 are indefinite based on their dependency.
Claim 5 recites “wherein the high frequency is in the range of a about 1-100 nanoseconds.” The limitation is indefinite because it uses the unit of seconds to describe a frequency. It is unclear if the claim intends to recite a frequency (e.g. in Hz) or a time of a pulse (e.g. in seconds).
Claim 6 recites “wherein the powder grains comprise 1-11 different metal salts.” It is unclear how 1 metal salt may be “different.” Additionally, as detailed with respect to claim 1, it is unclear if the metal salts may comprise compounds containing more than one metal or whether the claims are drawn to forming an alloy or single metal nanoparticles.
Claim 11 requires “A method of fabricating a powder precursor for synthesizing an ultrafine nano-alloy” but then requires only “at least one metal salt.” As the claim is drawn to a powder precursor capable of forming an alloy, requiring two or more metal elements, yet may comprise a single metal salt, it is unclear if such a single metal salt is a compound or complex comprising two or more metal elements, or whether the claim intends to also encompass forming a powder precursor for forming nanoparticles of a single metal element. Claims 12-17 are indefinite based on their dependency.
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.
Claim(s) 1-10 are rejected under 35 U.S.C. 103 as being unpatentable over Han (CN 112746213A)(machine translation provided) in view of Peng et al., “Laser solid-phase synthesis of single-atom catalysts,” Light: Science & Applications (2021) 10:168, pp. 1-14.
With respect to Claim 1, Han teaches a method of making a nano-particle alloy composite powder, thus, constituting a “ultrafine nano-alloy,” the method comprising providing a powder precursor comprising powder grains comprising at least one metal salt adhered to graphene (carbonaceous support), and subjecting the powder precursor to a heating reduction treatment to reduce the metal salt particles into nano metal particles. (pgs. 1, 3-5, 7, 10-11 of translation). Specifically, Han teaches wherein a mixture/solution of one or more metal salts is formed, graphene and grinding balls are added, mixed/milled such that the metal salt is adhered to the graphene and the grinding balls, drying the mixture to obtain a precursor powder, and heating the precursor powder to a temperature of 350-900 °C in an inert atmosphere to reduce the metal salt(s) to nano metal particles, wherein the nano metal particles may comprise a high-entropy alloy comprising 4 or more main elements. (pgs. 1-2, 8, 10-11 of translation).
In short, Han teaches a meth od of synthesizing an ultrafine nano-alloy on a carbonaceous support, the method comprising providing a powder precursor formed of powder grains comprising at least one metal salt on particles of a carbonaceous support such as graphene, and heating the powder precursor to reduce the metal atoms in the powder precursor to form an ultrafine nano-alloy. Han is silent, however, as to where this reduction of the metal atoms in the metal salt results from laser irradiation.
Peng teaches a method of synthesizing single-atom metal catalysts, the method comprising preparing a solid-phase precursor comprising a metal salt dispersed on electrochemical graphene oxide (EGO), drying, and laser irradiation of the solid-phase precursor to reduce the metal atoms of the metal salt, resulting in metal atoms dispersedly attached to a carbonaceous support. (abstract, pgs. 1-3). Peng also teaches that laser irradiation is a known method of fabricating nanoparticles, including metal and metal alloy nanoparticles, for example, comprising a photochemical reduction technique of metal salts. (p. 2). Peng teaches the use of pulsed laser irradiation delivered at high frequency. (pg. 2-3, 7, 12).
Thus, Han and Peng are both drawn to the formation of nanoscale metal atoms/particles attached to graphene/carbonaceous support material, the metal particles formed by reduction of metal salt precursor particles. It would have been obvious to one of ordinary skill in the art to modify the method of Han to substitute a heating reduction technique for reducing the metal salt precursor for a laser irradiation technique of reducing the metal salt precursor comprising pulsed laser at high frequency, as taught by Peng, in order to enable fine control of the reduction of the metal salt precursor powder particles enabling enhanced control over nanoparticle size/growth. Furthermore, the substitution of one process of heating and reducing a metal salt to a metal, for another, known to be useful in the same art/problem, would have been prima facie obvious to one of ordinary skill in the art. See MPEP 2144.
With respect to Claim 2, Peng teaches laser irradiation and is silent as to requiring a specialized environment (e.g. inert atmosphere). It would have been obvious to one of ordinary skill in the art to perform the method of Han in view of Peng in air at atmospheric pressure in order to reduce the costs and time associated with carrying out laser irradiation in a controlled atmosphere.
With respect to Claims 3-4, the claims are to drawn to removing residual metal salts, however, the claims do not require the presence of residual metal salts. “Claim scope is not limited by claim language that suggests or makes optional but does not require steps to be performed, or by claim language that does not limit a claim to a particular structure.” MPEP 2111.04
With respect to Claims 3-4, the claims recite “removing residual metal salts from the ultrafine nano-alloy,” but does not require that the method result in residual metal salts. Therefore, the limitations of claims 3 and 4 are interpreted as conditional/contingent limitations. “Claim scope is not limited by claim language that suggests or makes optional but does not require steps to be performed, or by claim language that does not limit a claim to a particular structure.” MPEP 2111.04. As Han in view of Peng teach the method of claim 1, and are drawn to fully reducing the metal salts to metal, the combined method is deemed to meet claims 3 and 4. Alternatively, Han and Peng both recognize that metal salts may be dissolved in a liquid solvent (see, e.g., Han, p. 10-11; Peng, p. 12). It would have been obvious to one of ordinary skill in the art to dissolve residual metal salts from the nano alloy with a liquid solvent, in order to obtain a purified nano alloy, with a predictable result of success.
With respect to Claim 5, Peng teaches wherein the laser pulse may be, for example 5 nanoseconds at a frequency of 30 kHz, deemed to fall within the claimed range. (p. 12).
With respect to Claim 6, Han teaches providing 4 or more metal salts supported on the particles of the carbonaceous support in order to form a high entropy alloy. (see rejection of claim 1 above). It would have been obvious to one of ordinary skill in the art to select from the portion of the overlapping ranges. Overlapping ranges, in particular, where the ranges of a claimed composition overlap with the ranges disclosed in the prior art, have been held sufficient to establish a prima facie case of obviousness. MPEP § 2144.05.
With respect to Claim 7, Han teaches wherein the carbonaceous support is graphene. (see rejection of claim 1 above).
With respect to Claim 8, Han teaches naturally cooling the nano alloy after performing a reduction step. (pgs. 10, 12 of translation). Peng recognize that after the laser pulse ends, the nano alloy immediately beings cooling. (p. 7). Accordingly, it would have been obvious to one of ordinary skill in the art to allow the nano-alloy formed by the method of Han in view of Peng to immediately begin natural cooling as a result of no longer being irradiated by a laser, in order to obtain a product useful for further processing or desired applications.
With respect to Claim 9, Peng teaches that the laser parameters may be varied, wherein each parameter may be balanced in order to achieve the desired outcome of reducing metal salt to metal. (see, e.g., pgs. 7-12). In view of the teachings of Peng and the knowledge of one of ordinary skill in the art, one of ordinary skill would recognize that the number of pulses may be varied depending on the length and power supplied in such pulses and therefore, the number of pulses needed to heat a given mass of powder to a desired temperature is a result effective variable. It would have been obvious to one of ordinary skill in the art to select an optimum or workable number of laser pulses per mg of powder precursor, including that claimed, in order to reduce the metal salts to a nano alloy, with a predictable result of success. MPEP 2144.05.
With respect to Claim 10, Han teaches forming a mixture of metal salts and carbonaceous support material in a liquid solvent, wherein the metal salts are adhered to carbonaceous support material and drying the mixture to form a powder precursor. (see rejection of claim 1 above). Accordingly, Han in view of Peng, is deemed to teach a step of “wet-impregnating the at least one metal salt on the particles of the carbonaceous support to form a precursor slurry, and drying the slurry to form the powder precursor.”
Claim(s) 11-17 are rejected under 35 U.S.C. 103 as being unpatentable over Han (CN 112746213A)(machine translation provided).
With respect to Claim 11, Han teaches a method of making a nano-particle alloy composite powder, thus, constituting a “ultrafine nano-alloy,” the method comprising providing a powder precursor comprising powder grains comprising at least one metal salt adhered to graphene (carbonaceous support), and subjecting the powder precursor to a heating reduction treatment to reduce the metal salt particles into nano metal particles. (pg. 1, 3-5, 7, 10-11 of translation). Specifically, Han teaches mixing in a solvent one or more metal salts (dissolving the at least one metal salt in liquid solvent), graphene particles (carbonaceous support particles), and grinding balls wherein the order of mixture is not considered material, wherein the mixture is mixed/milled such that the metal salt is adhered to the graphene and the grinding balls, drying the mixture to obtain a precursor powder, and heating the precursor powder to a temperature of 350-900 °C in an inert atmosphere to reduce the metal salt(s) to nano metal particles, wherein the nano metal particles may comprise a high-entropy alloy comprising 4 or more main elements. (pgs. 1-2, 8, 10-11 of translation).
Thus, Han teaches a method of fabricating a powder precursor for synthesizing an ultrafine nano-alloy, the powder precursor being formed of powder grains comprising at least one metal salt on particles of a carbonaceous support, the method comprising dissolving at least one metal salt in a liquid solvent, such as ethyl alcohol, adding particles of a carbonaceous support, such as graphene, to the liquid solvent, dispersing by mixing (ultrasonic) and/or milling the particles of the carbonaceous support in the dissolved at least one metal salt and liquid solvent to form a mixture, deemed to constitute a “dispersion solution,” and drying the dispersion solution to form the powder precursor. While the reference refers to a suspension rather than a solution or dispersion solution, the method of Han is interpreted to form a solution of at least one metal salt in a solvent (the same as required by dependent claim 12), and also comprises additional material such as grinding balls and graphene support particles, and therefore, is deemed to teach forming a “dispersion solution” as instantly claimed.
Han does not specifically teach a step of “degassing the dispersion solution,” however, the reference does teach drying the dispersion solution wherein liquid solvent is removed (vaporized/evaporates; see also Han, p. 8 recognizes that ethyl alcohol as a solvent is easy to volatilize) and therefore, is deemed to comprise degassing the dispersion solution. Furthermore, as the reference teaches the same method steps, materials, and structures, including the same solvent as required by dependent claim 12, it would necessarily be expected to result in at least some “degassing.” MPEP 2112.01.
Finally, Han does not specify the order in which the metal salts are dissolved in the liquid solvent and the particles of carbonaceous support material are added. It would have been prima facie obvious to one of ordinary skill in the art to select either order of adding the metal salts and carbonaceous support particles to the liquid solvent to form a dispersion solution. Selection of any order of mixing has been held to be prima facie obvious to one of ordinary skill in the art. Ex parte Rubin, 128 USPQ 440 (Bd. App. 1959) (Prior art reference disclosing a process of making a laminated sheet wherein a base sheet is first coated with a metallic film and thereafter impregnated with a thermosetting material was held to render prima facie obvious claims directed to a process of making a laminated sheet by reversing the order of the prior art process steps.). See also In re Burhans, 154 F.2d 690, 69 USPQ 330 (CCPA 1946) (selection of any order of performing process steps is prima facie obvious in the absence of new or unexpected results); In re Gibson, 39 F.2d 975, 5 USPQ 230 (CCPA 1930) (Selection of any order of mixing ingredients is prima facie obvious.). MPEP § 2144.04.
With respect to Claim 12, Han teaches wherein the solvent is ethyl alcohol (i.e. ethanol) meeting the instant claim. (pgs. 8, 10-11 of translation).
With respect to Claim 13, Han teaches ultrasonically dispersing (i.e. sonicating) the at least one metal salt and carbonaceous support in the liquid solvent (pg. 3, 5-6, 8 of translation) meeting the instant claim.
With respect to Claims 14-15, Han teaches wherein the step of dissolving comprises dissolving a plurality of different metal salts, in particular four or more metal salts, in the liquid solvent in order to form a precursor powder for forming a high entropy nano alloy. (see rejection of claims 1 and 11 above; pgs. 3, 10-11 of translation). It would have been obvious to one of ordinary skill in the art to select from the portion of the overlapping ranges. Overlapping ranges, in particular, where the ranges of a claimed composition overlap with the ranges disclosed in the prior art, have been held sufficient to establish a prima facie case of obviousness. MPEP § 2144.05.
With respect to Claim 16, Han teaches wherein the carbonaceous support comprises graphene particles (see rejection of claims 1 and 11 above). One of ordinary skill in the art would recognize that graphene particles, due to the nature of graphene structure, may be referred to as flakes. In the alternative, it would have been prima facie obvious to one of ordinary skill in the art to select one of the limited number of particles forms for graphene, such as flakes. See MPEP 2144.
With respect to Claim 17, Han teaches ultrasonically dispersing (i.e. sonicating) the at least one metal salt and carbonaceous support in the liquid solvent (pg. 3, 5-6, 8 of translation) meeting the instant claim.
Claim(s) 2 is rejected under 35 U.S.C. 103 as being unpatentable over Han (CN 112746213A)(machine translation provided) in view of Peng et al., “Laser solid-phase synthesis of single-atom catalysts,” Light: Science & Applications (2021) 10:168, pp. 1-14 as applied to claim 1 above, further in view of Deng (CN 110695366A)(machine translation provided).
In the alternative to the above rejection of claim 2, if Han in view of Peng are not interpreted tyo teach the limitations of claim 2, Deng teaches a method of fabricating metal nanoparticles on carbonaceous support material, the method comprising irradiation with a laser, wherein the method may be carried out in air atmosphere (interpreted as air at standard atmospheric pressure), eliminating the need for a vacuum. (pgs. 1, 4, 6, and 8 of translation). Deng also teaches that the preparation method may comprise in the alternative to an air environment, comprise a vacuum, nitrogen, argon, hydrogen, oxygen or methane environment. (pgs. 4 and 10 of translation).
It would have been obvious to one of ordinary skill in the art to modify the method of Han in view of Peng, in order to carry out the laser irradiating step in air at standard atmospheric pressure, as taught by Deng, in order to reduce costs and complexity of the method by eliminating the need for a controlled environment such as a vacuum chamber.
Claim(s) 16 is rejected under 35 U.S.C. 103 as being unpatentable over Han (CN 112746213A)(machine translation provided) in view of El-Shall (US 9768355).
In the alternative to the above rejection of claim 16, if Han is not deemed to teach graphene “flakes,” El-Shall teaches a method of forming graphene and nanoparticle catalysts using laser irradiation. (abstract, title). The reference teaches wherein the method may comprise flake graphene. (col. 6, ln. 44-49; col. 18, ln. 44-52).
Thus, both Han and El-Shall are drawn to forming metal nanoparticles on graphene. It would have been obvious to one of ordinary skill in the art to use a known form of graphene, graphene flakes, as taught by El-Shall, in order to form provide a support material suitable for metal nanoparticles.
Conclusion
The prior art made of record and not relied upon is considered pertinent to applicant's disclosure. CN 112719274, to Han, having a substantially similar disclose to the Han reference used in the rejections above.
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/JOHN A HEVEY/ Primary Examiner, Art Unit 1735
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