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 .
Status of the Claims
Claims 2-14 are pending and rejected. Claim 7 is amended. Claim 1 is cancelled.
Continued Examination Under 37 CFR 1.114
A request for continued examination under 37 CFR 1.114, including the fee set forth in 37 CFR 1.17(e), was filed in this application after final rejection. Since this application is eligible for continued examination under 37 CFR 1.114, and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114. Applicant's submission filed on 1/29/2026 has been entered.
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(f):
(f) Element in Claim for a Combination. – An element in a claim for a combination may be expressed as a means or step for performing a specified function without the recital of structure, material, or acts in support thereof, and such claim shall be construed to cover the corresponding structure, material, or acts described in the specification and equivalents thereof.
The following is a quotation of pre-AIA 35 U.S.C. 112, sixth paragraph:
An element in a claim for a combination may be expressed as a means or step for performing a specified function without the recital of structure, material, or acts in support thereof, and such claim shall be construed to cover the corresponding structure, material, or acts described in the specification and equivalents thereof.
The claims in this application are given their broadest reasonable interpretation using the plain meaning of the claim language in light of the specification as it would be understood by one of ordinary skill in the art. The broadest reasonable interpretation of a claim element (also commonly referred to as a claim limitation) is limited by the description in the specification when 35 U.S.C. 112(f) or pre-AIA 35 U.S.C. 112, sixth paragraph, is invoked.
As explained in MPEP § 2181, subsection I, claim limitations that meet the following three-prong test will be interpreted under 35 U.S.C. 112(f) or pre-AIA 35 U.S.C. 112, sixth paragraph:
(A) the claim limitation uses the term “means” or “step” or a term used as a substitute for “means” that is a generic placeholder (also called a nonce term or a non-structural term having no specific structural meaning) for performing the claimed function;
(B) the term “means” or “step” or the generic placeholder is modified by functional language, typically, but not always linked by the transition word “for” (e.g., “means for”) or another linking word or phrase, such as “configured to” or “so that”; and
(C) the term “means” or “step” or the generic placeholder is not modified by sufficient structure, material, or acts for performing the claimed function.
Use of the word “means” (or “step”) in a claim with functional language creates a rebuttable presumption that the claim limitation is to be treated in accordance with 35 U.S.C. 112(f) or pre-AIA 35 U.S.C. 112, sixth paragraph. The presumption that the claim limitation is interpreted under 35 U.S.C. 112(f) or pre-AIA 35 U.S.C. 112, sixth paragraph, is rebutted when the claim limitation recites sufficient structure, material, or acts to entirely perform the recited function.
Absence of the word “means” (or “step”) in a claim creates a rebuttable presumption that the claim limitation is not to be treated in accordance with 35 U.S.C. 112(f) or pre-AIA 35 U.S.C. 112, sixth paragraph. The presumption that the claim limitation is not interpreted under 35 U.S.C. 112(f) or pre-AIA 35 U.S.C. 112, sixth paragraph, is rebutted when the claim limitation recites function without reciting sufficient structure, material or acts to entirely perform the recited function.
Claim limitations in this application that use the word “means” (or “step”) are being interpreted under 35 U.S.C. 112(f) or pre-AIA 35 U.S.C. 112, sixth paragraph, except as otherwise indicated in an Office action. Conversely, claim limitations in this application that do not use the word “means” (or “step”) are not being interpreted under 35 U.S.C. 112(f) or pre-AIA 35 U.S.C. 112, sixth paragraph, except as otherwise indicated in an Office action.
This application includes one or more claim limitations that do not use the word “means,” but are nonetheless being interpreted under 35 U.S.C. 112(f) or pre-AIA 35 U.S.C. 112, sixth paragraph, because the claim limitation(s) uses a generic placeholder that is coupled with functional language without reciting sufficient structure to perform the recited function and the generic placeholder is not preceded by a structural modifier. Such claim limitation(s) is/are: “energy impacting apparatus” in claim 7.
Because this/these claim limitation(s) is/are being interpreted under 35 U.S.C. 112(f) or pre-AIA 35 U.S.C. 112, sixth paragraph, it/they is/are being interpreted to cover the corresponding structure described in the specification as performing the claimed function, and equivalents thereof.
If applicant does not intend to have this/these limitation(s) interpreted under 35 U.S.C. 112(f) or pre-AIA 35 U.S.C. 112, sixth paragraph, applicant may: (1) amend the claim limitation(s) to avoid it/them being interpreted under 35 U.S.C. 112(f) or pre-AIA 35 U.S.C. 112, sixth paragraph (e.g., by reciting sufficient structure to perform the claimed function); or (2) present a sufficient showing that the claim limitation(s) recite(s) sufficient structure to perform the claimed function so as to avoid it/them being interpreted under 35 U.S.C. 112(f) or pre-AIA 35 U.S.C. 112, sixth paragraph.
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 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 set forth in Graham v. John Deere Co., 383 U.S. 1, 148 USPQ 459 (1966), that are applied 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 2-9 and 11-14 are rejected under 35 U.S.C. 103 as being unpatentable over Zhamu, US 2017/0338472 A1 in view of Jang, US 2017/0352868 A1, and Campbell, US 2019/0198862 A1.
It is noted that the second inventor is used for US 2017/0352868 A1 to differentiate between the references.
Regarding claims 4 and 7, Zhamu teaches process for producing graphene encapsulated particulates for an alkali metal battery (abstract, where the battery electrode containing the produced active material is for a lithium-ion battery, lithium metal secondary battery, sodium-ion battery, sodium metal secondary battery, etc., 0077, such that the battery includes alkali metal batteries) said process comprising:
(b) mixing multiple particles of a graphitic material, multiple particles of a solid electrode active material, and an optional ball-milling media to form a mixture in an impacting chamber 10of an energy impacting apparatus (0049-0050, and 0100);
(c) operating said energy impacting apparatus with a frequency and an intensity for a length of time sufficient for peeling off graphene sheets from said graphitic material and transferring said graphene sheets to surfaces of the solid electrode active particles to produce graphene-embraced electrode active particles inside said 15impacting chamber (0051); and
(d) recovering said graphene-embraced metal-deposited polymer particles from said impacting chamber (0052).
They teach that the solid electrode active particles can be pre-coated with a carbon precursor material such as a polymer where the coated electrode active material is heated to convert the precursor material to a carbon material and pores, wherein the pores for empty spaces between surfaces of the solid electrode active material particles and the graphene sheets, and the carbon material is coated on the surface of the solid electrode active material particles and/or chemically bonds the graphene sheets together (0057). They teach that the electrode active material for an anode may be nickel, cobalt, titanium, zinc, aluminum, and tin among others (0060). They teach that the battery electrode contains the graphene-embraced electrode active material produced by the described method (0077), indicating that it is desirable to use graphene embraced electrode active material particles in a battery electrode.
They do not teach forming a graphene-embraced particle formed by coating a polymer particle with a lithium-attracting or a sodium-attracting metal or pyrolyzing the resulting particle.
Jang teaches a process for producing graphene/carbon particulates for an alkali metal battery (where a graphene-carbon hybrid foam is provided for a lithium or sodium metal battery, i.e., an alkali metal battery, abstract, where the process provides graphene-coated or graphene-embraced polymer particles that are consolidated and pyrolyzed, 0049-0055) said process comprising:
(a) Depositing particles or coating of a lithium-attracting metal or sodium-attracting metal 5onto surfaces of polymer particles to obtain metal-deposited polymer carrier particles, wherein said lithium-attracting or sodium-attracting metal is selected from Au, Ag, Mg, Zn, Ti, Li, Na, K, Al, Fe, Mn, Co, Ni, Sn, V, Cr, or an alloy thereof (where a controlled amount of a higher melting point metal such as Au, Ag, Ni, Co, Mn, Fe, and Ti is deposited on the surfaces of carrier polymer particles, 0159, indicating a lithium-attracting or sodium-attracting metal is applied to the polymer particle surface);
(b) mixing multiple particles of a graphitic material, said metal-deposited polymer carrier particles, and an optional ball-milling media to form a mixture in an impacting chamber 10of an energy impacting apparatus (0049-0051, 0056, and 0159);
(c) operating said energy impacting apparatus with a frequency and an intensity for a length of time sufficient for peeling off graphene sheets from said graphitic material and transferring said graphene sheets to surfaces of said metal-deposited polymer carrier particles to produce graphene-embraced metal-deposited polymer particles inside said 15impacting chamber (0051 and 0159);
(d) recovering said graphene-embraced metal-deposited polymer particles from said impacting chamber (0052 and 0159); and
(e) pyrolyzing said graphene-embraced metal-deposited polymer particles to thermally convert said polymer into pores and carbon or graphite that bonds said graphene sheets (0055), wherein at least a porous graphene/carbon structure comprises a graphene/carbon shell encapsulating a porous core, wherein said porous core comprises one or a plurality of pores and pore walls and said lithium- attracting metal or sodium-attracting metal resides in said pores or is deposited on said pore walls (where during pyrolysis the carbon atoms are able to permeate around the metal coating layer to bond together graphene sheets, 0159 and after pyrolysis the foam has a cell configuration where each cell contains an integral graphene carbon-metal foam where the metal is deposited on the pore walls or lodged inside of the pores, which is depicted as having a porous core, and the cells can have macroscopic or mesoscopic pores, and the metal is located in the pores, 0099 and Fig. 2b-c). It is noted that since they indicate when coating the polymer with metal that the carbon atoms are able to permeate around the metal carbon and they indicate that the polymer becomes porous upon pyrolysis (0099), the metal would also be expected to be in the pores of the carbon material because the carbon is around the metal. Jang further teaches that the carbon material serves to bridge the gaps between graphene sheets to form an interconnected electron-conducting pathway (0062 and 0112). They teach that having the lithium or sodium-attracting metal residing in pores of a graphene foam provides a safe and reliable site to receive and accommodate lithium/sodium during the battery charging step (0103). They teach that since the graphene sheets are bonded by a carbon phase to from the network, there is no possibility for otherwise isolated/separated graphene sheets to get re-stacked together thereby reducing the specific surface area (0129). The cells of the carbon-metal foam is depicted as being individual particles connected together to form the foam (0099 and Fig. 2b-c). Therefore, Jang provides a method of forming a foam for an alkali battery where they coat polymer particles with metal, impact the particles with a graphite material so as to peel graphene sheets from the graphite material, recover the graphene-embraced particles, consolidate the particles, and pyrolyzed the polymer to form a carbon phase that bonds the graphene sheets to prevent them from re-stacking while also providing an electrical pathway where the metal is deposited in the pores of the carbon, providing a safe and reliable site for receiving and accommodating Li/Na.
From the teachings of Jang, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have modified the process of Zhamu to have coated polymer particles with a metal such as nickel, cobalt, and titanium, to have used the particles in place of the electrode active particles, and then to have pyrolyzed the resulting graphene-embraced metal/polymer particles to convert the polymer to carbon to provide an active material for the alkali battery because Zhamu indicates that it is desirable to have particulate active material in the battery and Jang indicates that pyrolyzing a graphene-embraced polymer particle having a metal coating results in forming a conductive pathway that bonds the graphene while also providing a safe and reliable site for the metal such that it will be expected to provide a desirable active material particle in the process of Zhamu while also containing the materials indicated by Zhamu, i.e. active electrode material (metal), graphene, and carbon. Further, while Zhamu provides a carbon coating on the solid active material particle, since Jang indicates that a polymer particle can be coated with metal, embraced by graphene and then pyrolyzed to convert the polymer to carbon to provide a desirable material for an alkali battery it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention that such a configuration will also provide a desirable active material particle for the battery of Zhamu.
As to the energy impacting apparatus interpreted under 112(f), Zhamu further teaches that the energy impacting apparatus may be a vibratory ball mill, planetary ball mill, high energy mill, basket mill, agitator ball mill, cryogenic ball mill, micro ball mill, tumbler ball mill, stirred ball mill, pressurized ball mill, plasma-assisted ball mill, freezer mill, vibratory sieve, bead mill, nano bead mill, ultrasonic homogenizer mill, centrifugal planetary mixer, vacuum ball mill, or a resonant acoustic mixer, where the procedure can be done in a continuous manner (0070). Jang also teaches that the energy impacting apparatus may be a vibratory ball mill, planetary ball mill, high energy mill, basket mill, agitator ball mill, cryo ball mill, micro ball mill, tumbler ball mill, continuous ball mill, stirred ball mill, pressurized ball mill, freezer mill, vibratory sieve, bead mill, nano bead mill, ultrasonic homogenizer mill, centrifugal planetary mixer, vacuum ball mill, or a resonant acoustic mixer (0059). Therefore, the energy impacting devices suggested by Zhamu and Jang are understood to meet the requirements of an energy impacting apparatus as such apparatus are described by the instant specification at page 14, lines 18-23, at page 21, lines 13-18, and as required by claim 4.
As to the material of the polymer particles or the optional ball-milling media, Jang further teaches that the polymer particles can be formed from phenolic resin, polyimide, polyoxadiazole, polyvinyl alcohol, polyvinyl chloride, polymethylmethacrylate, etc. (0060-0061). Further, Jang teaches that the step of pyrolyzing includes carbonizing the polymer at a temperature ranging from 200-2500°C where the material can be optionally graphitized at a temperature from 2500-3200°C (0063). Jang teaches that when using the metal-coated polymer particles having graphene sheets on the surfaces, carbon atoms were able to permeate around the metal coating layer to bond together graphene sheets (0159).
They do not teach selecting one of the listed polymer particles.
Campbell teaches pyrolysis (carbonization) of various plastics, including recycled plastic to generate carbonaceous materials cheaply and in bulk, which can then be converted into energy storage device materials, e.g., carbon anode active material for Li-ion batteries (abstract). They teach that plastics that may be converted to high purity carbon materials after thermal pyrolysis (carbonization) and can be utilized as high-performance active material for energy storage devices, e.g., Li-ion batteries (0005). They teach that suitable thermoplastics and other types of plastics include PET, phenolics, polyvinyl chlorides, polyvinylidene chlorides, polymethyl methacrylates, polyamides, polycarbonates, polyesters, polyethylenes, etc., melamine formaldehydes, maleimides, plastarches, etc. (0005). They teach that plastic-derived carbon can be produced to provide improved graphite and activated carbons for use as active material in lithium-ion batteries with higher performance in terms of specific capacity, energy density, power density, and capacitance (0005). They teach that the porosity of the carbonized plastic material is mainly a function of the plastic precursor type and carbonization conditions (0010). They teach that the carbonized plastic may include a plurality of bubble-induced voids (0013). They teach that pyrolysis treatments typically happen under inert atmosphere in a heating chamber or furnace using temperatures between 200°C to 3500°C, with the temperatures depending on the material precursor (0095). They teach that the plastics after pyrolysis tend to form pores of multiple size regimes depending on the plastic precursor type (0095).
From the teachings of Campbell, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have modified the process of Zhamu in view of Jang to have used melamine formaldehyde, maleimide, or plastarch particles as the polymer particles because Campbell indicates that such materials are capable of carbonizing by heating in a range overlapping that of Jang as an alternative polymer material to those taught by Jang, where the carbonized forms are porous and desirable for use in lithium-ion batteries such that the polymer particles will be expected to provide a suitable substitution of one known material for another that is capable of carbonizing overlapping the temperature range of Jang as a carbon material for use in a battery. Therefore, in the process of Zhamu in view of Jang and Campbell the polymer particles are selected from melamine formaldehyde, maleimide, or plastarch.
Regarding claim 2, Zhamu in view of Jang and Campbell suggest the limitations of instant claim 7. Zhamu further teaches that the graphitic material may be selected from natural graphite (considered to be pristine), chemically modified graphite, i.e., chemically functionalized graphite, or a combination thereof (0069). Jang also teaches that the graphitic material is selected from natural graphite, graphite fluoride, chemically modified graphite, or a combination thereof (0058).
Regarding claim 3, Zhamu in view of Jang and Campbell suggest the limitations of instant claim 7. Zhamu further teaches that the particles of solid electrode active material contain pre-lithiated or pre-sodiated particles by intercalating with Li or Na ions by electrochemical charging before being wrapped by graphene sheets (0055). They teach that by pre-lithiating or pre-sodiating the particles, the electrode would no longer have any issues of electrode expansion and expansion-induced failure during subsequent charge-discharge cycles (0055).
Jang further teaches that the integral graphene-carbon-metal foam can be lithiated or sodiated before or after the cell is made (0100). They teach that a lithium or sodium metal foil or particles may be implemented at the anode and during the first battery discharge cycle lithium or sodium ions migrate to the cathode and that during the subsequent re-charge cycle lithium or sodium ions are released by the cathode active material and migrate back to the anode (0100-0102). They teach that the lithium or sodium ions naturally diffuse through the pore walls to reach that lithium- or sodium-attracting metal lodged inside the pores or on the inner pore walls of the foam so that the foam can be lithiated or sodiated (0102). They teach that alternatively the foam can be pre-lithiated or pre-sodiated electrochemically prior to being incorporated as an anode layer (0102).
From the teachings of Zhamu and Jang, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have pre-lithiated or pre-sodiated the particles before incorporation into the battery because Zhamu indicates that pre-lithiating or pre-sodiating the active particles prevents expansion related issues and Jang indicates that the graphene/carbon foam can be pre-lithiated or pre-sodiated prior to incorporation into a battery where lithium or sodium ions naturally diffuse through the pore walls to reach that lithium- or sodium-attracting metal lodged inside the pores or on the inner pore walls of the foam such that the ions are also expected to be capable of diffusing through the particles in the process of Zhamu in view of Jang and Campbell so as to at least partially fill the pores of the particles and be in contact with the lithium or sodium-attracting metal so as to provide pre-lithiated or pre-sodiated active particles that avoid expansion related problems.
Regarding claim 5, Zhamu in view of Jang and Campbell suggest the limitations of instant claim 7. Zhamu further teaches that the energy impacting apparatus may be conducted in a continuous manner (0070). Jang also teaches using a continuous ball mill (0059), suggesting that the process is continuous by using a continuous impacting apparatus.
Regarding claim 6, Zhamu in view of Jang and Campbell suggests the limitations of instant claim 7. Zhamu further teaches that impacting balls may be added into the impacting chambers, where examples of the ball include stainless steel or zirconia beads (0100), such that the milling media is a metal alloy or a ceramic. Jang further teaches that impacting balls such as zirconium dioxide or steel balls can be used (0115), such that the balls include a metal alloy and ceramic.
Regarding claim 8, Zhamu in view of Jang and Campbell suggest the limitations of instant claim 7. Zhamu further teaches using the active material in a battery such as a lithium-ion battery, lithium metal secondary battery, lithium-sulfur battery, lithium-selenium battery, lithium-air battery, sodium-ion battery, sodium metal secondary battery, or sodium-air battery (0077). Jang further teaches using the graphene-carbon-metal foam in a lithium metal or sodium metal battery (0208). From this, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have used the active material in the batteries suggested by Zhamu and Jang because both Zhamu and Jang provide active material for batteries having similar materials, i.e. (graphene, active material, and carbon) such that the resulting graphene-porous carbon-metal particles are expected to be suitable active materials for the range of batteries indicated by Zhamu.
Regarding claim 9, Zhamu in view of Jang and Campbell suggest the limitations of instant claim 3. As discussed above for claim 8, Zhamu in view of Jang and Campbell suggest using the particles in a lithium-ion battery, lithium metal secondary battery, lithium-sulfur battery, lithium-selenium battery, lithium-air battery, sodium-ion battery, sodium metal secondary battery, or sodium-air battery. Zhamu further teaches using the graphene-embraced particles as an anode material (0048 and Fig. 2). Jang further teaches using the graphene-carbon hybrid foam for the anode (abstract). From this, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have used the pre-lithiated or pre-sodiated graphene/carbon particulates of Zhamu in view of Jang and Campbell in an anode electrode of a lithium-ion battery, lithium metal secondary battery, lithium-sulfur battery, lithium-selenium battery, lithium-air battery, sodium-ion battery, sodium metal secondary battery, or sodium-air battery because both Zhamu and Jang suggest using particles having similar materials (graphene, carbon, and lithium or sodium attracting metal that is pre-lithiated or pre-sodiated as discussed above for claim 3) as anode materials in batteries such that they will be expected to be suitable anode materials for the batteries described by Zhamu. Therefore, since Zhamu in view of Jang and Campbell suggests using the pre-lithiated or pre-sodiated particles in the anode electrode they are also expected to act as a pre-lithiating or pre-sodiating agent of the battery.
Regarding claims 11 and 12, Zhamu in view of Jang and Campbell suggest the limitations of instant claim 7. Jang further teaches pyrolyzing the polymer at a temperature from 200°C to 2500°C to obtain carbon-bonded graphene sheets, where the carbon-bonded graphene sheets can be optionally substantially graphitized at a temperature from 2500-3200°C to obtain graphite-bonded graphene sheets (0063). Jang further teaches mixing the graphene-coated or graphene embraced polymer particles with the lithium-attracting metal or a precursor of the metal followed by pyrolyzing the polymer, where in the pyrolysis step the precursor is thermally converted or reduced to a metal phase residing in the pores of the foam or adhering to pore walls (0053-0055 and 0108). Jang teaches using metals such as sodium and tin (0040). Therefore, Jang teaches mixing the metals with the graphene-embraced polymer particles prior to pyrolyzing and graphitizing, suggesting that tin and sodium can acceptably undergo the pyrolyzing and graphitizing steps since they are mixed prior to graphitizing.
Campbell teaches performing pyrolysis at temperatures between 200°C to 3500°C, where the temperatures depend on the material precursor (0095).
From this, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have provided the step of pyrolyzing at a temperature ranging from 200-3500°C to carbonize the polymer particles to become a carbon material, such that the temperature range overlaps the claimed range, because Campbell teaches that such a range is suitable for carbonizing the material, where Jang indicates that sodium and tin can be added to the material prior to pyrolyzation such that it will be expected to provide the desirable material for the battery. Therefore, in the process of Zhamu in view of Jang and Campbell, the step of pyrolyzing will comprise carbonizing the polymer to become a carbon using a temperature overlapping the claimed range. According to 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.”
Regarding claim 13, Zhamu in view of Jang and Campbell suggest the limitations of instant claim 7. Jang further teaches mixing the graphene-coated or graphene embraced polymer particles with the lithium-attracting metal or a precursor of the metal followed by pyrolyzing the polymer, where in the pyrolysis step the precursor is thermally converted or reduced to a metal phase residing in the pores of the foam or adhering to pore walls (0053-0055 and 0108). As discussed above for claim 7, Jang also teaches depositing metal on the surface of the carrier polymer particles prior to impacting with graphene (0159). From this, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have deposited a metal precursor on the polymer particles and then converted the precursor to metal in the pyrolyzing stage because Jang indicates that a metal precursor can be converted to metal in the pyrolyzing step, where metal can be applied directly onto the polymer particle such that by applying a precursor to the polymer particle it will also be expected to be converted to metal in the pyrolyzing step to provide the desired graphene-embraced porous carbon particle having the metal in the pores.
Regarding claim 14, Zhamu in view of Jang and Campbell suggest the limitations of instant claim 7. Jang further teaches mixing the graphene-coated or graphene embraced polymer particles with the lithium-attracting metal or a precursor of the metal followed by pyrolyzing the polymer (0053-0055 and 0108). As discussed above for claim 7, Jang also teaches depositing metal on the surface of the carrier polymer particles prior to impacting with graphene (0159). Jang also teaches that the metal precursors can be converted to a metal by chemical or thermal conversion, where an example of conversion is electrolysis (0196-0197). They also indicate that nickel can be provided by hydrogenolysis of nickelocene at a low temperature of less than 70°C (0200). From this, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have deposited a metal precursor on the polymer particles and then convert the precursor to metal by chemical means such as electrolysis or hydrogenolysis because Jang indicates that a metal precursor can be converted to metal using such chemical means, where metal can be applied directly onto the polymer particle such that by applying a precursor to polymer particle it will also be expected to be converted to metal using chemical means to provide a metal coated polymer particle for use in the subsequent impacting process.
Claim 10 is rejected under 35 U.S.C. 103 as being unpatentable over Zhamu in view of Jang and Campbell as applied to claim 7 above, and further in view of Toulis, US 2016/0204420 A1.
Regarding claim 10, Zhamu in view of Jang and Campbell suggests the limitations of instant claim 7. Campbell teaches performing pyrolysis under an inert atmosphere such as argon, nitrogen, or helium gas (0095).
They do not teach pyrolyzing in a flowing gaseous environment or a fluidized bed.
Toulis teaches a process of producing active material for an electrode of an electrochemical step in which a pulverulent composite composed of lithium-intercalating carbon particles (component 1), silicon particles (component 2), and a polymer that can be pyrolyzed to form amorphous carbon (component 3) is formed followed by pyrolyzing the composite to form amorphous carbon as component 3 (abstract). They teach that the particles in step A do not tend to form agglomerates even when the contact one another during the pyrolysis step B where step B preferably results in a powder (0053). They teach that the powder to be pyrolyzed in a fluidized-bed pyrolysis reactor can be brought by an upward-flowing carrier gas into a fluidized state and subjected to temperatures at which component 3 decomposes into amorphous carbon (0053). They teach that the carrier gas can be nitrogen (0035 and 0054). Therefore, they teach loading particles containing a polymer to be pyrolyzed in a fluidized bed reactor for pyrolysis so as to provide a powder material.
From the teachings of Toulis, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have modified the process of Zhamu in view of Jang and Campbell to have pyrolyzed the particles in a fluidized bed reactor containing a nitrogen atmosphere because Toulis indicates that such a process successfully pyrolyzes a polymer in a particle to provide a powder material and Campbell teaches pyrolyzing under nitrogen such that it will be expected to also pyrolyzed the polymer particle in the particulates of Zhamu in view of Jang and Campbell while also preventing agglomeration due to the particles being separated from one another in the fluidized bed so as to maintain the particulate form. Therefore, in the process of Zhamu in view of Jang, Campbell, and Toulis, the step of pyrolyzing is conducted in a fluidized bed which will keep the graphene-embraced metal-deposited polymer particles separated.
Claims 2-9 and 11-14 are rejected under 35 U.S.C. 103 as being unpatentable over Jang, US 2017/0352868 A1 in view of Zhamu, US 2017/0338472 A1 and Campbell, US 2019/0198862 A1.
It is noted that the second inventor is used for US 2017/0352868 A1 to differentiate between the references.
Regarding claims 4 and 7, Jang teaches process for producing graphene/polymer particulates for an alkali metal battery (where a graphene-carbon hybrid foam is provided for a lithium or sodium metal battery, i.e., and alkali metal battery, abstract, where the process provides graphene-coated or graphene-embraced polymer particles that are consolidated and pyrolyzed, 0049-0055) said process comprising:
(a) Depositing particles or coating of a lithium-attracting metal or sodium-attracting metal 5onto surfaces of polymer particles to obtain metal-deposited polymer carrier particles, wherein said lithium-attracting or sodium-attracting metal is selected from Au, Ag, Ti, Fe, Mn, Co, or Ni (where a controlled amount of a higher melting point metal such as Au, Ag, Ni, Co, Mn, Fe, and Ti is deposited on the surfaces of carrier polymer particles, 0159, indicating a lithium-attracting or sodium-attracting metal is applied to the polymer particle surface);
(b) mixing multiple particles of a graphitic material, said metal-deposited polymer carrier particles, and an optional ball-milling media to form a mixture in an impacting chamber 10of an energy impacting apparatus (0049-0051, 0056, and 0159);
(c) operating said energy impacting apparatus with a frequency and an intensity for a length of time sufficient for peeling off graphene sheets from said graphitic material and transferring said graphene sheets to surfaces of said metal-deposited polymer carrier particles to produce graphene-embraced metal-deposited polymer particles inside said 15impacting chamber (0051 and 0159);
(d) recovering said graphene-embraced metal-deposited polymer particles from said impacting chamber (0052 and 0159); and
(e) pyrolyzing said graphene-embraced metal-deposited polymer particles to thermally convert said polymer into pores and carbon or graphite that bonds said graphene sheets (0055), wherein at least a porous graphene/carbon structure comprises a graphene/carbon shell encapsulating a porous core, wherein said porous core comprises one or a plurality of pores and pore walls and said lithium- attracting metal or sodium-attracting metal resides in said pores or is deposited on said pore walls (where during pyrolysis the carbon atoms are able to permeate around the metal coating layer to bond together graphene sheets, 0159 and after pyrolysis the foam has a cell configuration where each cell contains an integral graphene carbon-metal foam where the metal is deposited on the pore walls or lodged inside of the pores, which is depicted as having a porous core, and the cells can have macroscopic or mesoscopic pores, and the metal is located in the pores, 0099 and Fig. 2b-c). It is noted that since they indicate when coating the polymer with metal that the carbon atoms are able to permeate around the metal carbon and they indicate that the polymer becomes porous upon pyrolysis (0099), the metal would also be expected to be in the pores of the carbon material because the carbon is around the metal. They teach that having the lithium or sodium-attracting metal residing in pores of a graphene foam provides a safe and reliable site to receive and accommodate lithium/sodium during the battery charging step (0103). The cells of the carbon-metal foam is depicted as being individual particles connected together to form the foam (0099 and Fig. 2b-c). Therefore, Jang provides a method of forming a foam for an alkali battery where they coat polymer particles with metal, impact the particles with a graphite material so as to peel graphene sheets from the graphite material, recover the graphene-embraced particles, consolidate the particles, and pyrolyzed the polymer to form a carbon phase that bonds the graphene sheets to prevent them from re-stacking while also providing an electrical pathway where the metal is deposited in the pores of the carbon, providing a safe and reliable site for receiving and accommodating Li/Na.
They do not teach producing graphene/carbon particulates because the resulting particles are compacted into a foam.
Zhamu teaches process for producing graphene encapsulated particulates for an alkali metal battery (abstract, where the battery electrode containing the produced active material is for a lithium-ion battery, lithium metal secondary battery, sodium-ion battery, sodium metal secondary battery, etc., 0077, such that the battery includes alkali metal batteries) said process comprising:
(b) mixing multiple particles of a graphitic material, multiple particles of a solid electrode active material, and an optional ball-milling media to form a mixture in an impacting chamber 10of an energy impacting apparatus (0049-0050, and 0100);
(c) operating said energy impacting apparatus with a frequency and an intensity for a length of time sufficient for peeling off graphene sheets from said graphitic material and transferring said graphene sheets to surfaces of the solid electrode active particles to produce graphene-embraced electrode active particles inside said 15impacting chamber (0051); and
(d) recovering said graphene-embraced metal-deposited polymer particles from said impacting chamber (0052).
They teach that the solid electrode active particles can be pre-coated with a carbon precursor material such as a polymer where the coated electrode active material is heated to convert the precursor material to a carbon material and pores, wherein the pores for empty spaces between surfaces of the solid electrode active material particles and the graphene sheets, and the carbon material is coated on the surface of the solid electrode active material particles and/or chemically bonds the graphene sheets together (0057). They teach that the electrode active material for an anode may be nickel, cobalt, and titanium among others (0060). They teach that the battery electrode contains the graphene-embraced electrode active material produced by the described method (0077), indicating that it is desirable to use graphene embraced electrode active material particles in a battery electrode. They teach preparing lithium-ion cells or lithium metal cells using the conventional slurry coating method in which graphene-encapsulated Si or Co3O4 particles, acetylene black, and PVDF binder dissolved in NMP are combined and then coated onto a Cu foil (0166).
From the teachings of Zhamu, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have modified the process of Jang to have also provided graphene/carbon particles (i.e. non-consolidated particles) because Zhamu indicates that it is desirable and conventional to use particulate active material in forming batteries where particles comprising graphene-embraced active material are desirable for such as use such that it will be expected to provide a desirable active material that can be used in conventional processes for forming batteries.
As to the energy impacting apparatus interpreted under 112(f), Jang further teaches that the energy impacting apparatus may be a vibratory ball mill, planetary ball mill, high energy mill, basket mill, agitator ball mill, cryo ball mill, micro ball mill, tumbler ball mill, continuous ball mill, stirred ball mill, pressurized ball mill, freezer mill, vibratory sieve, bead mill, nano bead mill, ultrasonic homogenizer mill, centrifugal planetary mixer, vacuum ball mill, or a resonant acoustic mixer (0059). Zhamu further teaches that the energy impacting apparatus may be a vibratory ball mill, planetary ball mill, high energy mill, basket mill, agitator ball mill, cryogenic ball mill, micro ball mill, tumbler ball mill, stirred ball mill, pressurized ball mill, plasma-assisted ball mill, freezer mill, vibratory sieve, bead mill, nano bead mill, ultrasonic homogenizer mill, centrifugal planetary mixer, vacuum ball mill, or a resonant acoustic mixer, where the procedure can be done in a continuous manner (0070). Therefore, the energy impacting devices suggested by Jang and Zhamu are understood to meet the requirements of an energy impacting apparatus as such apparatus are described by the instant specification at page 14, lines 18-23, at page 21, lines 13-18, and as required by claim 4.
As to the material of the polymer particles or the optional ball-milling media, Jang further teaches that the polymer particles can be formed from phenolic resin, polyimide, polyamide, polybenzimidazole, polyvinyl alcohol, polymethylmethacrylate, etc. (0061). Further, Jang teaches that the step of pyrolyzing includes carbonizing the polymer at a temperature ranging from 200-2500°C where the material can be optionally graphitized at a temperature from 2500-3200°C (0063). Jang teaches that when using the metal-coated polymer particles having graphene sheets on the surfaces, carbon atoms were able to permeate around the metal coating layer to bond together graphene sheets (0159).
They do not teach selecting one of the listed polymer particles.
As discussed above for the rejection of claim 7 over Zhamu in view of Jang and Campbell, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have used melamine formaldehyde, maleimide, or plastarch particles as the polymer particles because Campbell indicates that such materials are capable of carbonizing by heating in a range overlapping that of Jang as an alternative polymer material to those taught by Jang, where the carbonized forms are porous and desirable for use in lithium-ion batteries such that the polymer particles will be expected to provide a suitable substitution of one known material for another that is capable of carbonizing overlapping the temperature range of Jang as a carbon material for use in a battery. Therefore, in the process of Jang in view of Zhamu and Campbell, the polymer particles are selected from melamine formaldehyde, maleimide, or plastarch.
Regarding claim 2, Jang in view of Zhamu and Campbell suggest the limitations of instant claim 7. Jang further teaches that the graphitic material is selected from natural graphite, graphite fluoride, chemically modified graphite, or a combination thereof (0058). Zhamu also teaches that the graphitic material may be selected from natural graphite (considered to be pristine), chemically modified graphite, i.e., chemically functionalized graphite, or a combination thereof (0069).
Regarding claim 3, Jang in view of Zhamu and Campbell suggest the limitations of instant claim 7. Jang further teaches that the integral graphene-carbon-metal foam can be lithiated or sodiated before or after the cell is made (0100). They teach that a lithium or sodium metal foil or particles may be implemented at the anode and during the first battery discharge cycle lithium or sodium ions migrate to the cathode and that during the subsequent re-charge cycle lithium or sodium ions are released by the cathode active material and migrate back to the anode (0100-0102). They teach that the lithium or sodium ions naturally diffuse through the pore walls to reach that lithium- or sodium-attracting metal lodged inside the pores or on the inner pore walls of the foam so that the foam can be lithiated or sodiated (0102). They teach that alternatively the foam can be pre-lithiated or pre-sodiated electrochemically prior to being incorporated as an anode layer (0102).
Zhamu further teaches that the particles of solid electrode active material contain pre-lithiated or pre-sodiated particles by intercalating with Li or Na ions by electrochemical charging before being wrapped by graphene sheets (0055). They teach that by pre-lithiating or pre-sodiating the particles, the electrode would no longer have any issues of electrode expansion and expansion-induced failure during subsequent charge-discharge cycles (0055).
From the teachings of Jang and Zhamu, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have pre-lithiated or pre-sodiated the particles before incorporation into the battery because Zhamu indicates that pre-lithiating or pre-sodiating the active particles prevents expansion related issues and Jang indicates that the graphene/carbon foam can be pre-lithiated or pre-sodiated prior to incorporation into a battery where lithium or sodium ions naturally diffuse through the pore walls to reach that lithium- or sodium-attracting metal lodged inside the pores or on the inner pore walls of the foam such that the ions are also expected to be capable of diffusing through the particles in the process of Jang in view of Zhamu and Campbell so as to at least partially fill the pores of the particles and be in contact with the lithium or sodium-attracting metal so as to provide pre-lithiated or pre-sodiated active particles that avoid expansion related problems.
Regarding claim 5, Jang in view of Zhamu and Campbell suggest the limitations of instant claim 7. Jang further teaches using a continuous ball mill (0059), suggesting that the process is continuous by using a continuous impacting apparatus. Zhamu also teaches that the energy impacting apparatus may be conducted in a continuous manner (0070).
Regarding claim 6, Jang in view of Zhamu and Campbell suggests the limitations of instant claim 7. Jang further teaches that impacting balls such as zirconium dioxide or steel balls can be used (0115), such that the balls include a metal alloy and ceramic. Zhamu further teaches that impacting balls may be added into the impacting chambers, where examples of the ball include stainless steel or zirconia beads (0100), such that the milling media is a metal alloy or a ceramic.
Regarding claim 8, Jang in view of Zhamu and Campbell suggest the limitations of instant claim 7. Jang further teaches using the graphene-carbon-metal foam in a lithium metal or sodium metal battery (0208). Zhamu further teaches using the active material in a battery such as a lithium-ion battery, lithium metal secondary battery, lithium-sulfur battery, lithium-selenium battery, lithium-air battery, sodium-ion battery, sodium metal secondary battery, or sodium-air battery (0077). From this, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have used the active material in the batteries suggested by Jang and Zhamu because both Jang and Zhamu provide active material for batteries having similar materials, i.e. (graphene, active material, and carbon) such that the resulting graphene-porous carbon-metal particles are expected to be suitable active materials for the range of batteries indicated by Zhamu.
Regarding claim 9, Jang in view of Zhamu and Campbell suggest the limitations of instant claim 3. As discussed above for claim 8, Jang in view of Zhamu and Campbell suggest using the particles in a lithium-ion battery, lithium metal secondary battery, lithium-sulfur battery, lithium-selenium battery, lithium-air battery, sodium-ion battery, sodium metal secondary battery, or sodium-air battery. Jang further teaches using the graphene-carbon hybrid foam for the anode (abstract). Zhamu further teaches using the graphene-embraced particles as an anode material (0048 and Fig. 2). From this, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have used the pre-lithiated or pre-sodiated graphene/carbon particulates of Jang in view of Zhamu and Campbell in an anode electrode of a lithium-ion battery, lithium metal secondary battery, lithium-sulfur battery, lithium-selenium battery, lithium-air battery, sodium-ion battery, sodium metal secondary battery, or sodium-air battery because both Jang and Zhamu suggest using particles having similar materials (graphene, carbon, and lithium or sodium attracting metal that is pre-lithiated or pre-sodiated as discussed above for claim 3) as anode materials in batteries such that they will be expected to be suitable anode materials for the batteries described by Zhamu. Therefore, since Jang in view of Zhamu and Campbell suggests using the pre-lithiated or pre-sodiated particles in the anode electrode they are also expected to act as a pre-lithiating or pre-sodiating agent of the battery.
Regarding claims 11 and 12, Jang in view of Zhamu and Campbell suggest the limitations of instant claim 7. Jang further teaches pyrolyzing the polymer at a temperature from 200°C to 2500°C to obtain carbon-bonded graphene sheets, where the carbon-bonded graphene sheets can be substantially graphitized at a temperature from 2500-3200°C to obtain graphite-bonded graphene sheets (0063). Jang further teaches mixing the graphene-coated or graphene embraced polymer particles with the lithium-attracting metal or a precursor of the metal followed by pyrolyzing the polymer, where in the pyrolysis step the precursor is thermally converted or reduced to a metal phase residing in the pores of the foam or adhering to pore walls (0053-0055 and 0108). Jang teaches using metals such as sodium and tin (0040). Therefore, Jang teaches mixing the metals with the graphene-embraced polymer particles prior to pyrolyzing and graphitizing, suggesting that tin and sodium can acceptably undergo the pyrolyzing and graphitizing steps since they are mixed prior to graphitizing.
Campbell teaches performing pyrolysis at temperatures between 200°C to 3500°C, where the temperatures depend on the material precursor (0095).
From this, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have provided the step of pyrolyzing at a temperature ranging from 200-3500°C to carbonize the polymer particles to become a carbon material, such that the temperature range overlaps the claimed range, because Campbell teaches that such a range is suitable for carbonizing the material, where Jang indicates that sodium and tin can be added to the material prior to pyrolyzation such that it will be expected to provide the desirable material for the battery. Therefore, in the process of Jang in view of Zhamu and Campbell, the step of pyrolyzing will comprise carbonizing the polymer to become a carbon using a temperature overlapping the claimed range. According to 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.”
Regarding claim 13, Jang in view of Zhamu and Campbell suggest the limitations of instant claim 7. Jang further teaches mixing the graphene-coated or graphene embraced polymer particles with the lithium-attracting metal or a precursor of the metal followed by pyrolyzing the polymer, where in the pyrolysis step the precursor is thermally converted or reduced to a metal phase residing in the pores of the foam or adhering to pore walls (0053-0055 and 0108). As discussed above for claim 7, Jang also teaches depositing metal on the surface of the carrier polymer particles prior to impacting with graphene (0159). From this, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have deposited a metal precursor on the polymer particles and then converted the precursor to metal in the pyrolyzing stage because Jang indicates that a metal precursor can be converted to metal in the pyrolyzing step, where metal can be applied directly onto the polymer particle such that by applying a precursor to the polymer particle it will also be expected to be converted to metal in the pyrolyzing step to provide the desired graphene-embraced porous carbon particle having the metal in the pores.
Regarding claim 14, Jang in view of Zhamu and Campbell suggest the limitations of instant claim 7. Jang further teaches mixing the graphene-coated or graphene embraced polymer particles with the lithium-attracting metal or a precursor of the metal followed by pyrolyzing the polymer (0053-0055 and 0108). As discussed above for claim 7, Jang also teaches depositing metal on the surface of the carrier polymer particles prior to impacting with graphene (0159). Jang also teaches that the metal precursors can be converted to a metal by chemical or thermal conversion, where an example of conversion is electrolysis (0196-0197). They also indicate that nickel can be provided by hydrogenolysis of nickelocene at a low temperature of less than 70°C (0200). From this, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have deposited a metal precursor on the polymer particles and then convert the precursor to metal by chemical means such as electrolysis or hydrogenolysis because Jang indicates that a metal precursor can be converted to metal using such chemical means, where metal can be applied directly onto the polymer particle such that by applying a precursor to polymer particle it will also be expected to be converted to metal using chemical means to provide a metal coated polymer particle for use in the subsequent impacting process.
Claim 10 is rejected under 35 U.S.C. 103 as being unpatentable over Jang in view of Zhamu and Campbell as applied to claim 7 above, and further in view of Toulis, US 2016/0204420 A1.
Regarding claim 10, Jang in view of Zhamu and Campbell suggests the limitations of instant claim 7. Campbell further teaches pyrolyzing under an inert atmosphere such as argon, nitrogen, or helium gas (0095).
They do not teach pyrolyzing in a flowing gaseous environment or a fluidized bed.
Toulis teaches a process of producing active material for an electrode of an electrochemical step in which a pulverulent composite composed of lithium-intercalating carbon particles (component 1), silicon particles (component 2), and a polymer that can be pyrolyzed to form amorphous carbon (component 3) is formed followed by pyrolyzing the composite to form amorphous carbon as component 3 (abstract). They teach that the particles in step A do not tend to form agglomerates even when the contact one another during the pyrolysis step B where step B preferably results in a powder (0053). They teach that the powder to be pyrolyzed in a fluidized-bed pyrolysis reactor can be brought by an upward-flowing carrier gas into a fluidized state and subjected to temperatures at which component 3 decomposes into amorphous carbon (0053). They teach that the carrier gas can be nitrogen (0035 and 0054). Therefore, they teach loading particles containing a polymer to be pyrolyzed in a fluidized bed reactor for pyrolysis so as to provide a powder material.
From the teachings of Toulis, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to have modified the process of Jang in view of Zhamu and Campbell to have pyrolyzed the particles in a fluidized bed reactor using a nitrogen atmosphere because Toulis indicates that such a process successfully pyrolyzes a polymer in a particle to provide a powder material and Campbell teaches pyrolyzing under a nitrogen atmosphere such that it will be expected to also pyrolyzed the polymer particle in the particulates of Jang in view of Zhamu and Campbell while also preventing agglomeration due to the particles being separated from one another in the fluidized bed so as to maintain the particulate form. Therefore, in the process of Jang in view of Zhamu, Campbell, and Toulis, the step of pyrolyzing is conducted in a fluidized bed which will keep the graphene-embraced metal-deposited polymer particles separated.
Response to Arguments
Applicant's arguments filed 1/29/2026 have been fully considered.
In light of the amendments to the claims, Applicant’s arguments are considered persuasive. Therefore, the rejections have been amended to include the new reference of Campbell.
Conclusion
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/CHRISTINA D MCCLURE/ Examiner, Art Unit 1718