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 Rejections - 35 USC § 103
In the event the determination of the status of the application as subject to AIA 35 U.S.C. 102 and 103 (or as subject to pre-AIA 35 U.S.C. 102 and 103) is incorrect, any correction of the statutory basis (i.e., changing from AIA to pre-AIA ) for the rejection will not be considered a new ground of rejection if the prior art relied upon, and the rationale supporting the rejection, would be the same under either status.
The following is a quotation of 35 U.S.C. 103 which forms the basis for all obviousness rejections set forth in this Office action:
A patent for a claimed invention may not be obtained, notwithstanding that the claimed invention is not identically disclosed as set forth in section 102, if the differences between the claimed invention and the prior art are such that the claimed invention as a whole would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to which the claimed invention pertains. Patentability shall not be negated by the manner in which the invention was made.
The factual inquiries for establishing a background for determining obviousness under 35 U.S.C. 103 are summarized as follows:
1. Determining the scope and contents of the prior art.
2. Ascertaining the differences between the prior art and the claims at issue.
3. Resolving the level of ordinary skill in the pertinent art.
4. Considering objective evidence present in the application indicating obviousness or nonobviousness.
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, 3-4, 6, 9-12, 14-15, and 17-18 are rejected under 35 U.S.C. 103 as being unpatentable over Oh et al. (US PGPub 2022/0255060 A1) and further in view of Deng et al. (US PGPub 2020/0280061 A1), Fukuoka et al. (US PGPub 2007/0248525 A1), and Nakanishi (US PGPub 2011/0287317 A1).
Regarding Claims 1, 3-4, 9-10, 14-15, and 17-18, Oh discloses an electronic device ([0125]), comprising an electrochemical device ([0125], [0015]-[0016]), comprising: a negative electrode ([0016]), comprising:
a current collector and a coating located on the current collector, wherein the coating comprises silicon-based particles and carbon-based particles, wherein the carbon-based particles are preferably graphite particles ([0024], [0042]-[0043]), and
a percentage of a weight of the silicon-based particles in a total weight of the silicon-based particles and the graphite particles is N, wherein N is 1 to 30 wt % in order to improve both capacity characteristics and cycle characteristics ([0045]), which overlaps with the instantly claimed range of approximately 25 wt% - 80 wt %.
It would have been obvious to one of ordinary skill in the art to form the coating to comprise a weight of the silicon-based particles such that N is in the overlapping portion of the range disclosed by Oh in order to improve both capacity characteristics and cycle characteristics.
Modified Oh further discloses wherein the silicon-containing substrate comprises SiOx, wherein 0.5 < x < 1.5 in order to ensure structural stability of the active material ([0033], [0036] of Oh), which encompasses SiO.
It would have been obvious to one of ordinary skill in the art to utilize SiO as the silicon-containing substrate of modified Oh, as disclosed by modified Oh, wherein the skilled artisan would have reasonable expectation that such would successfully ensure structural stability of the silicon-based particles of modified Oh.
Modified Oh discloses wherein the silicon-based particles may comprise a silicon-containing substrate and a carbon-based layer located on at least a part of a surface of the silicon-containing substrate ([0038]).
However, modified Oh does not disclose wherein the silicon-based particles comprise a silicon-containing substrate and a polymer layer, the polymer layer comprises a polymer and carbon nanotubes, the polymer layer is located on at least a part of a surface of the silicon-containing substrate, and wherein, based on a total weight of the silicon-based particles, a weight ratio of the polymer to the carbon nanotubes in the polymer later is greater than 3:1 and less than or equal to 10:1, and further approximately 4:1 – 10:1.
Deng teaches a negative electrode material comprising silicon-based particles that has excellent electrochemical cycle performance and expansion inhibition and allows prolonged service life of an electrochemical device ([0006]).
Specifically, Deng teaches wherein the silicon-based particles comprise a silicon-containing substrate (silicon-based active material) and a polymer layer (composite layer) located on at least a part of a surface of the silicon-containing substrate, wherein the polymer layer comprises a polymer, such as carboxymethyl cellulose, polyacrylic acid, or combinations thereof, and a conductive material, such as carbon nanotubes ([0008], [0016], [0023], e.g. [0065]).
It would have been obvious to one of ordinary skill in the art to form the silicon-based particles of modified Oh to comprise a polymer layer, wherein the polymer layer comprises a polymer comprising carboxymethyl cellulose, polyacrylic acid, or combinations thereof and carbon nanotubes and is located on at least a part of a surface of the silicon-containing substrate of modified Oh, as taught by Deng, in order to form a negative electrode having excellent electrochemical cycle performance and expansion inhibition that allows for prolonged service life of the electrochemical device of modified Oh.
Modified Oh further discloses:
wherein, based on a total weight of the silicon-based particles, a content of the polymer layer is greater than 0 to 35 wt%, e.g. 0.5 to 35 wt% ([0024]-[0026] of Deng), which encompasses the instantly claimed range of 12 – 15 wt%; and
wherein, based on the total weight of the silicon-based particles, a content of the carbon nanotubes is greater than 0 to 5 wt%, e.g. 0.5 to 5 wt% ([0026] of Deng), which falls within and therefore reads on the instantly claimed range of approximately 0.01 – 10 wt%; and
wherein, based on the total weight of the silicon-based particles, a weight ratio of the polymer to the carbon nanotubes is 0.1:1 to 20:1 ([0024], [0026] of Deng), which encompasses the instantly claimed range of greater than 3:1 and less than or equal to 10:1 and further approximately 4:1 – 10:1.
It would have been obvious to one of ordinary skill in the art to form the silicon-based particles of modified Oh to have a content of the polymer layer in the encompassing portion of the range disclosed by modified Oh, wherein the skilled artisan would have a reasonable expectation that such would successfully form negative electrode that has excellent electrochemical cycle performance and expansion inhibition and allows prolonged service life of the electrochemical device of modified Oh, as desired by modified Oh.
Furthermore, it would have been obvious to one of ordinary skill in the art to form the silicon-based particles of modified Oh to have a weight ratio of the polymer to the carbon nanotubes in the encompassing portion of the range disclosed by modified Oh, wherein the skilled artisan would have a reasonable expectation that such would successfully form negative electrode that has excellent electrochemical cycle performance and expansion inhibition and allows prolonged service life of the electrochemical device of modified Oh, as desired by modified Oh.
Modified Oh remains silent regarding a minimum value and a maximum value of film resistances at different positions on a surface of the coating and consequently does not disclose wherein a minimum value of film resistances at different positions on a surface of the coating is R1, a maximum value of film resistances at different positions on a surface of the coating is R2, an R1/R2 ratio is M, wherein M > 0.65.
The Examiner notes that the instant specification discloses exemplary embodiments of a negative electrode having an R1/R2 ratio is M, wherein M > 0.65 (Tables 1-3).
For example, the Examiner notes that the instant specification discloses a method forming a negative electrode having an M that falls within the instantly claimed range, wherein the method comprises:
(1) mixing silicon dioxide and metal silicon powder at a molar ratio of 1:1 by mechanical dry mixing and ball milling to obtain a mixed material;
(2) heating the mixed material in an Ar2 atmosphere in a temperature range of 1,100~1,550°C and a pressure range of approximately 10-3~10-1 kPa for 0.5~24 hr to obtain a gas;
(3) condensing the obtained gas to obtain a solid, and pulverizing and sifting the solid; and
(4) thermally treating the solid in a nitrogen atmosphere in temperature range of 400~1200°C for 1~24 hr and cooling to obtain a silicon-containing substrate material;
(5) dispersing carbon nanotubes and a polymer in water at a high speed for 12 hours to obtain a homogenously mixed slurry;
(6) adding the silicon-containing substrate into the slurry and stirring for 4 hr to obtain a homogeneously mixed dispersed solution;
(7) spray-drying at an inlet temperature of 200°C and an outlet temperature of 110°C to obtain a powder; and
(8) cooling and pulverizing the powder
(9) mixing the silicon-based particles (the powder) with graphite at a rotation speed of 20 r/min for 1 hr to obtain a mixed negative active material;
(10) adding a binder, deionized water, and a conductive agent to the mixed negative active material, stirring at a rotation speed of 15 r/min for 2 hr, and dispersing the mixture at a rotation speed of 1,500 r/min for 1 hr to obtain a negative electrode slurry; and
(11) coating the negative electrode slurry onto a copper foil and performing drying and cold calendering to obtain the negative electrode (Table 1, [00140]-[00148], [00152]-[00154]).
Modified Oh discloses dispersing the carbon nanotubes and the polymer in a solvent, such as water, to obtain a slurry, adding the silicon-containing substrate into the slurry and stirring to obtain a homogeneously mixed dispersed solution, drying the solution to obtain a powder, to obtain the silicon-based particles ([0027]-[0033], [0036], e.g. [0062] of Deng) and then mixing the silicon-based particles with the graphite particles, adding a binder, a solvent, and a conductive agent (e.g. SWCNT aggregates) to the mixed negative active material to obtain a negative electrode slurry; and coating the negative electrode slurry onto a negative electrode current collector, such as copper foil, and performing drying to obtain the negative electrode ([0071], [0096], [0027], [0029] of Oh).
However, modified Oh remains silent regarding the method of forming the silicon oxide in the silicon-containing substrate and consequently does not disclose
(1) mixing silicon dioxide and metal silicon powder at a molar ratio of 1:1 by mechanical dry mixing and ball milling to obtain a mixed material;
(2) heating the mixed material in an Ar2 atmosphere in a temperature range of 1,100~1,550°C and a pressure range of approximately 10-3~10-1 kPa for 0.5~24 hr to obtain a gas;
(3) condensing the obtained gas to obtain a solid, and pulverizing and sifting the solid; and
(4) thermally treating the solid in a nitrogen atmosphere in temperature range of 400~1200°C for 1~24 hr and cooling to obtain a silicon-containing substrate material.
Fukuoka teaches a method of producing silicon oxide powder at a high efficiency and low cost ([0006]).
Specifically, Fukaoka teaches wherein the method comprises:
mixing silicon dioxide and metal silicon powder at a molar ratio of 1:1 by mechanical dry mixing and ball milling to obtain a mixed material ([0016]-[0017], wherein a molar ratio in the range of 1:1.01 to 1:1.08 reads on the molar ratio of 1:1 when rounded to the nearest significant figure recited in the instant specification);
heating the mixed material in an inert gas atmosphere in a temperature range of 1,100 to 1,450°C , which falls within the range of 1,100~1,550°C, and a pressure range of approximately 10-3~10-1 kPa for 5 hr, which falls within the range of 0.5 to 24h, to obtain a gas ([0018]-[0019], [0024]);
condensing the obtained gas to obtain a solid ([0020], [0024]).
It would have been obvious to one of ordinary skill in the art to mix silicon dioxide and metal silicon powder at a molar ratio of 1:1 by mechanical dry mixing and ball milling to obtain a mixed material, heat the mixed material in an inert gas atmosphere in a temperature range of 1,100 to 1,450°C and a pressure range of approximately 10-3~10-1 kPa for 5 hr to obtain a gas and condense the obtained gas to obtain a solid, as taught by Fukaoka, in order to obtain a silicon oxide powder, as desired by modified Oh, at a high efficiency and low cost.
Furthermore, Nakanishi teaches a method for forming a silicon-containing substrate that comprises obtaining a solid by heating a silicon material to form a gas, and then condensing the gas ([0028]).
Specifically, Nakanishi teaches pulverizing and sifting the solid and then thermally treating the solid in an inert atmosphere in temperature range of 600 to 1,100°C , which falls within the range of 400~1200°C, for approximately 1 to 5 hr, which falls within the range of 1~24 hr in order to decrease a specific surface area of the obtained silicon-containing substrate in order to suppress acceleration of the decomposition reaction of an electrolyte ([0028], [0031], [0036], [0101]-[0104]).
It would have been obvious to one of ordinary skill in the art to pulverize and sift the obtained solid of modified Oh and then thermally treating the solid in an inert atmosphere in temperature range of 600 to 1,100°C for approximately 1 to 5 hr, as taught by Nakanishi, in order to decrease a specific surface area of the obtained silicon-containing substrate, thereby suppressing acceleration of the decomposition reaction of an electrolyte in the electrochemical device of modified Oh.
The Examiner notes that modified Oh does not disclose some of the mixing speeds and times recited by the method disclosed in the instant specification. However, such do not appear to be critical in achieving the claimed effects in light of Tables 1-3 of the instant specification.
Thus, the Examiner notes that the negative electrode comprising the coating comprises the silicon-based particles comprising the silicon-containing substrate, the polymer, and the carbon nanotubes and the graphite particles in suitable amounts as disclosed Tables 2-3 of the instant specification and further notes that the method of forming the negative electrode of modified Oh is substantially similar as that disclosed in Table 1 and [00140]-[00148], [00152]-[00154] of the instant specification and therefore modified Oh discloses a coating that necessarily and inherently comprises a minimum value of film resistances at different positions on a surface of the coating is R1, a maximum value of film resistances at different positions on a surface of the coating is R2, an R1/R2 ratio is M, wherein M > 0.65, as evidenced by Tables 1-3 and [00140]-[00148] of the instant specification.
Regarding Claim 6, modified Oh discloses all of the limitations as set forth above. Modified Oh remains silent regarding an X-ray diffraction pattern of the silicon-based particles and consequently does not disclose wherein a highest intensity value of 2θ attributed to a range of approximately 28.0° - 29.0° is I2, and a highest intensity value attributed to a range of approximately 20.5° - 21.5° is I1, and approximately 0 < I2/I1 < approximately 1.
However, the Examiner notes that the negative electrode comprising the coating comprises the silicon-based particles comprising the silicon-containing substrate, the polymer, and the carbon nanotubes and the graphite particles in suitable amounts as disclosed Tables 2-3 of the instant specification and further notes that the method of forming the negative electrode of modified Oh is substantially similar as that disclosed in Table 1 and [00140]-[00148], [00152]-[00154] of the instant specification and therefore the silicon-based particles of modified Oh necessarily and inherently have a highest intensity value of 2θ attributed to a range of approximately 28.0° - 29.0° is I2, and a highest intensity value attributed to a range of approximately 20.5° - 21.5° is I1, and approximately 0 < I2/I1 < approximately 1, as evidenced by Tables 1-3 and [00140]-[00148], [00152]-[00154] of the instant specification.
Regarding Claim 11, modified Oh discloses all of the limitations as set forth above and further discloses wherein a thickness of the polymer layer is 10 – 100 nm ([0012] of Deng), which falls within and therefore reads on the instantly claimed range of approximately 5 – 200 nm.
Regarding Claim 12, modified Oh discloses all of the limitations as set forth above and further discloses wherein an average particle size of the silicon-based particles is 1 µm to 15 µm in order to ensure the structural stability of the silicon-based particles during charging and discharging while preventing a problem of increasing a level of volume expansion/contraction and a problem of degrading initial efficiency ([0041] of Oh), which falls within and therefore reads on the instantly claimed range of approximately 500 nm - 30 µm.
Claim 5 is rejected under 35 U.S.C. 103 as being unpatentable over Oh et al. (US PGPub 2022/0255060 A1) in view Deng et al. (US PGPub 2020/0280061 A1), Fukuoka et al. (US PGPub 2007/0248525 A1), and Nakanishi (US PGPub 2011/0287317 A1), as applied to Claim 4 above, and further in view of Chae et al. (US PGPub 2021/0024358 A1).
Regarding Claim 5, modified Oh discloses all of the limitations as set forth above and further discloses wherein the silicon-containing substrate comprises Si ([0033], [0036] of Oh).
However, modified Oh remains silent regarding a particle size of Si in the silicon-based particles and consequently does not disclose wherein such is less than approximately 100 nm.
Chae teaches a negative electrode comprising a coating comprising silicon-based particles, wherein the silicon-based particles comprise a silicon-containing substrate and a layer, wherein the layer comprises carbon ([0017]).
Chae further teaches wherein a particle size of Si in the silicon-based particles is most preferably from 30 nm to 100 nm in order to prevent a problem of decreasing first cycle Coulombic efficiency as specific surface area increases ([0053]), which falls within and therefore reads on the instantly claimed range of less than approximately 100 nm.
It would have been obvious to one of ordinary skill in the art to form the Si in the silicon-based particles of modified Oh to have a particle size in the range taught by Chae in order to prevent a problem of decreasing first cycle Coulombic efficiency as specific surface area increases.
Claims 7 and 13 are rejected under 35 U.S.C. 103 as being unpatentable over Oh et al. (US PGPub 2022/0255060 A1) in view of Deng et al. (US PGPub 2020/0280061 A1), Fukuoka et al. (US PGPub 2007/0248525 A1), and Nakanishi (US PGPub 2011/0287317 A1), as applied to Claim 1 above, and further in view of Yasuda et al. (CN 103229336 A, see also the provided EPO machine generated English translation).
Regarding Claim 7, modified Oh discloses all of the limitations as set forth above and further discloses wherein an average particle size of the silicon-based particles is 1 µm to 15 µm in order to ensure the structural stability of the silicon-based particles during charging and discharging while preventing a problem of increasing a level of volume expansion/contraction and a problem of degrading initial efficiency ([0041] of Oh),
However, modified Oh does not disclose wherein a particle size distribution of the silicon-based particles satisfies: approximately 0.3 < Dn10/Dv50 < approximately 0.6.
Yasuda teaches an electrochemical device comprising a negative electrode comprising a coating comprising silicon-based particles that has a large discharge capacity, good cycle characteristics, and can withstand practical use in an electrochemical device ([0023]).
Specifically, Yasuda teaches wherein the silicon-based particles comprise a silicon-containing substrate comprising silicon oxide and a layer, wherein the layer comprises a carbon material ([0023], [0028]).
Yasuda further teaches wherein the silicon-based particles have an average particle diameter (Dv50) preferably of 3 to 12 µm, in order to suppress bubbles from being generated when preparing a slurry while preventing an increase in the roughness of the surface of the coating, thereby ensuring sufficient adhesion between the coating and a current collector ([0028]), which falls within the range of 1 µm to 15 µm desired by modified Oh.
Moreover, Yasuda teaches wherein a particle size distribution of the silicon-based particles satisfies: 1.4 < Dn50/Dv10 < 2.4 in order to suppress bubbles from being generated when preparing a slurry while facilitating uniform mixing, thereby ensuring sufficient adhesion between the coating and a current collector and a large discharge capacity ([0052]-[0053], [0041]).
The Examiner notes that 1.4 < Dn50/Dv10 < 2.4 is mathematically equivalent to approximately 0.42 < Dn10/Dv50 < approximately 0.71, which overlaps with the instantly claimed range of approximately 0.3 < Dn10/Dv50 < approximately 0.6.
It would have been obvious to one of ordinary skill in the art to form the silicon-based particles of modified Oh to have a particle size distribution in the overlapping portion of the range taught by Yasuda, in order to ensuring sufficient adhesion between the coating of modified Oh and the current collector of modified Oh and to achieve a large discharge capacity, wherein the skilled artisan would have reasonable expectation that such would successfully ensure the structural stability of the silicon-based particles during charging and discharging while preventing a problem of increasing a level of volume expansion/contraction and a problem of degrading initial efficiency, as desired by modified Oh.
Regarding Claim 13, modified Oh discloses all of the limitations as set forth above and further discloses in the teachings of Nakanishi wherein the silicon-containing substrate in the silicon-based particles of modified Oh should have a specific surface area of 0.1 – 5.0 m2/g in order to suppress acceleration of the decomposition reaction of the electrolyte ([0036] of Nakanishi) and therefore modified Oh discloses a desire to minimize reactions with the electrolyte.
However, modified Oh remains silent regarding a specific surface area of the silicon-based particles and consequently does not disclose wherein such is approximately 1 – 50 m2/g.
Yasuda teaches an electrochemical device comprising a negative electrode comprising a coating comprising silicon-based particles that has a large discharge capacity, good cycle characteristics, and can withstand practical use in an electrochemical device ([0023]).
Specifically, Yasuda teaches wherein the silicon-based particles comprise a silicon-containing substrate comprising silicon oxide and a layer, wherein the layer comprises a carbon material ([0023], [0028]).
Yasuda further teaches wherein the silicon-based particles have a specific surface area in the range of 0.3 - 7 m2/g in order to prevent the formation of a thick SEI film that may cause reduced capacity while facilitating production of the silicon-based particles from an economical point of view ([0054]), which overlaps with the range desired by modified Oh and further overlaps with the instantly claimed range.
It would have been obvious to one of ordinary skill in the art to form the silicon-based particles of modified Oh to have a specific surface area in the overlapping portion of the range taught by Yasuda, in order to prevent the formation of a thick SEI film that may cause reduced capacity while facilitating production of the silicon-based particles from an economical point of view, wherein the skilled artisan would have reasonable expectation that such would successfully form the silicon-based particles desired by modified Oh.
Claims 1 and 19 are rejected under 35 U.S.C. 103 as being unpatentable over Ko et al. (US PGPub 2019/0123352 A1) and further in view of Deng et al. (US PGPub 2020/0280061 A1), Fukuoka et al. (US PGPub 2007/0248525 A1), and Nakanishi (US PGPub 2011/0287317 A1).
Regarding Claims 1 and 19, Ko discloses a negative electrode ([0006], [0052]), comprising: a current collector and a coating located on the current collector ([0006], [0052]), wherein the coating comprises silicon-based particles and graphite particles ([0056], e.g. [0086], wherein graphite is a crystalline carbon), and a percentage of a weight of the silicon-based particles in a total weight of the silicon-based particles and the graphite particles is N, and N is about 1 wt% to about 50 wt% ([0057]), which overlaps with the instantly claimed range of approximately 25 wt% - 80 wt%, and further approximately 40 wt% - 80 wt%.
It would have been obvious to one of ordinary skill in the art to form the coating to comprise a weight of the silicon-based particles such that N is in the overlapping portion of the range disclosed by Ko, wherein the skilled artisan would have a reasonable expectation that such would successfully form the negative electrode desired by Ko.
However, modified Ko does not disclose wherein the silicon-based particles comprise a silicon-containing substrate, wherein the silicon-containing structure comprises SiOx wherein 0.5 < x < 1.5, and a polymer layer, the polymer layer comprises a polymer and carbon nanotubes, the polymer layer is located on at least a part of a surface of the silicon-containing substrate, and wherein, based on a total weight of the silicon-based particles, a weight ratio of the polymer to the carbon nanotubes in the polymer later is greater than 3:1 and less than or equal to 10:1, and further approximately 4:1 – 10:1.
Deng teaches a negative electrode material comprising silicon-based particles that has excellent electrochemical cycle performance and expansion inhibition and allows prolonged service life of a lithium ion battery ([0006]).
Specifically, Deng teaches wherein the silicon-based particles comprise a silicon-containing substrate (silicon-based active material), wherein the silicon-containing structure comprises SiOx wherein 0 < x < 2, which encompasses 0.5 < x < 1.5, and a polymer layer (composite layer) located on at least a part of a surface of the silicon-containing substrate, wherein the polymer layers comprises a polymer and a conductive material, such as carbon nanotubes ([0008], [0016], [0023], e.g. [0065]).
It would have been obvious to one of ordinary skill in the art to utilize the silicon-based particles taught by Deng as the silicon-based particles of modified Ko, wherein the silicon-containing structure comprises SiOx when x is in the encompassing portion of the range taught by Deng and wherein the polymer layer comprises a polymer and carbon nanotubes and is located on at least a part of a surface of the silicon-containing substrate, in order to form a negative electrode having excellent electrochemical cycle performance and expansion inhibition that allows for prolonged service life of a lithium ion battery.
Modified Ko further discloses: wherein, based on a total weight of the silicon-based particles, a content of the polymer layer is greater than 0 to 35 wt%, e.g. 0.5 to 35 wt% ([0024]-[0026] of Deng), which encompasses the instantly claimed range of 12 – 15 wt%.
It would have been obvious to one of ordinary skill in the art to form the silicon-based particles of modified Ko to have a content of the polymer layer in the encompassing portion of the range disclosed by modified Ko, wherein the skilled artisan would have a reasonable expectation that such would successfully form negative electrode that has excellent electrochemical cycle performance and expansion inhibition and allows prolonged service life of a lithium ion battery, as desired by modified Ko.
Modified Ko remains silent regarding a minimum value and a maximum value of film resistances at different positions on a surface of the coating and consequently does not disclose wherein a minimum value of film resistances at different positions on a surface of the coating is R1, a maximum value of film resistances at different positions on a surface of the coating is R2, an R1/R2 ratio is M, wherein M > approximately 0.5.
The Examiner notes that the instant specification discloses exemplary embodiments of a negative electrode having an R1/R2 ratio is M, wherein M > 0.65 (Tables 1-3).
For example, the Examiner notes that the instant specification discloses a method forming a negative electrode having an M that falls within the instantly claimed range, wherein the method comprises:
(1) mixing silicon dioxide and metal silicon powder at a molar ratio of 1:1 by mechanical dry mixing and ball milling to obtain a mixed material;
(2) heating the mixed material in an Ar2 atmosphere in a temperature range of 1,100~1,550°C and a pressure range of approximately 10-3~10-1 kPa for 0.5~24 hr to obtain a gas;
(3) condensing the obtained gas to obtain a solid, and pulverizing and sifting the solid; and
(4) thermally treating the solid in a nitrogen atmosphere in temperature range of 400~1200°C for 1~24 hr and cooling to obtain a silicon-containing substrate material;
(5) dispersing carbon nanotubes and a polymer in water at a high speed for 12 hours to obtain a homogenously mixed slurry;
(6) adding the silicon-containing substrate into the slurry and stirring for 4 hr to obtain a homogeneously mixed dispersed solution;
(7) spray-drying at an inlet temperature of 200°C and an outlet temperature of 110°C to obtain a powder; and
(8) cooling and pulverizing the powder
(9) mixing the silicon-based particles (the powder) with graphite at a rotation speed of 20 r/min for 1 hr to obtain a mixed negative active material;
(10) adding a binder, deionized water, and a conductive agent to the mixed negative active material, stirring at a rotation speed of 15 r/min for 2 hr, and dispersing the mixture at a rotation speed of 1,500 r/min for 1 hr to obtain a negative electrode slurry; and
(11) coating the negative electrode slurry onto a copper foil and performing drying and cold calendering to obtain the negative electrode (Table 1, [00140]-[00148], [00152]-[00154]).
Modified Oh discloses dispersing the carbon nanotubes and the polymer in a solvent, such as water, to obtain a slurry, adding the silicon-containing substrate into the slurry and stirring to obtain a homogeneously mixed dispersed solution, drying the solution to obtain a powder, to obtain the silicon-based particles ([0027]-[0033], [0036], e.g. [0062] of Deng) and then mixing the silicon-based particles with the graphite particles, adding a binder, a solvent, and a conductive agent to the mixed negative active material to obtain a negative electrode slurry; and coating the negative electrode slurry onto a negative electrode current collector, such as copper foil, and performing drying to obtain the negative electrode ([0056], [0058], e.g. [0086]-[0087]).
However, modified Ko remains silent regarding the method of forming the silicon oxide in the silicon-containing substrate and consequently does not disclose
(1) mixing silicon dioxide and metal silicon powder at a molar ratio of 1:1 by mechanical dry mixing and ball milling to obtain a mixed material;
(2) heating the mixed material in an Ar2 atmosphere in a temperature range of 1,100~1,550°C and a pressure range of approximately 10-3~10-1 kPa for 0.5~24 hr to obtain a gas;
(3) condensing the obtained gas to obtain a solid, and pulverizing and sifting the solid; and
(4) thermally treating the solid in a nitrogen atmosphere in temperature range of 400~1200°C for 1~24 hr and cooling to obtain a silicon-containing substrate material.
Fukuoka teaches a method of producing silicon oxide powder at a high efficiency and low cost ([0006]).
Specifically, Fukaoka teaches wherein the method comprises:
mixing silicon dioxide and metal silicon powder at a molar ratio of 1:1 by mechanical dry mixing and ball milling to obtain a mixed material ([0016]-[0017], wherein a molar ratio in the range of 1:1.01 to 1:1.08 reads on the molar ratio of 1:1 when rounded to the nearest significant figure recited in the instant specification);
heating the mixed material in an inert gas atmosphere in a temperature range of 1,100 to 1,450°C , which falls within the range of 1,100~1,550°C, and a pressure range of approximately 10-3~10-1 kPa for 5 hr, which falls within the range of 0.5 to 24h, to obtain a gas ([0018]-[0019], [0024]);
condensing the obtained gas to obtain a solid ([0020], [0024]).
It would have been obvious to one of ordinary skill in the art to mix silicon dioxide and metal silicon powder at a molar ratio of 1:1 by mechanical dry mixing and ball milling to obtain a mixed material, heat the mixed material in an inert gas atmosphere in a temperature range of 1,100 to 1,450°C and a pressure range of approximately 10-3~10-1 kPa for 5 hr to obtain a gas and condense the obtained gas to obtain a solid, as taught by Fukaoka, in order to obtain a silicon oxide powder, as desired by modified Ko, at a high efficiency and low cost.
Furthermore, Nakanishi teaches a method for forming a silicon-containing substrate that comprises obtaining a solid by heating a silicon material to form a gas, and then condensing the gas ([0028]).
Specifically, Nakanishi teaches pulverizing and sifting the solid and then thermally treating the solid in an inert atmosphere in temperature range of 600 to 1,100°C , which falls within the range of 400~1200°C, for approximately 1 to 5 hr, which falls within the range of 1~24 hr in order to decrease a specific surface area of the obtained silicon-containing substrate in order to suppress acceleration of the decomposition reaction of an electrolyte ([0028], [0031], [0036], [0101]-[0104]).
It would have been obvious to one of ordinary skill in the art to pulverize and sift the obtained solid of modified Ko and then thermally treating the solid in an inert atmosphere in temperature range of 600 to 1,100°C for approximately 1 to 5 hr, as taught by Nakanishi, in order to decrease a specific surface area of the obtained silicon-containing substrate, thereby suppressing acceleration of the decomposition reaction of an electrolyte in the electrochemical device of modified Ko.
The Examiner notes that modified Ko does not disclose some of the mixing speeds and times recited by the method disclosed in the instant specification. However, such do not appear to be critical in achieving the claimed effects in light of Tables 1-3 of the instant specification.
Thus, the Examiner notes that the negative electrode comprising the coating comprises the silicon-based particles comprising the silicon-containing substrate, the polymer, and the carbon nanotubes and the graphite particles in suitable amounts as disclosed Tables 2-3 of the instant specification and further notes that the method of forming the negative electrode of modified Ko is substantially similar as that disclosed in Table 1 and [00140]-[00148], [00152]-[00154] of the instant specification and therefore modified Ko discloses a coating that necessarily and inherently comprises a minimum value of film resistances at different positions on a surface of the coating is R1, a maximum value of film resistances at different positions on a surface of the coating is R2, an R1/R2 ratio is M, wherein M > 0.65, as evidenced by Tables 1-3 and [00140]-[00148] of the instant specification.
Response to Arguments
Applicant's arguments filed January 8, 2026 have been fully considered but they are not persuasive.
Regarding amended Claim 1, Applicant’s arguments with respect to the polymer layer content have been considered but are moot because the new ground of rejection does not rely on any reference applied in the prior rejection of record for any teaching or matter specifically challenged in the argument.
The Applicant argues that the inherency position set forth by the Office is legally and factionally unsupported. Inherency requires that a claimed characteristic be necessary and inevitably present in the prior art. However, the cited prior art fails to disclose the critical preparation sets and processing conditions required to achieve the claimed film resistance uniformity. For example, the cited prior art does not disclose the dispersing step (step (5)) ([0145, e.g. dispersing for 12 hours) nor does it disclose the dispersing conditions used in preparing the negative electrode described in [0152]-[0153] of the specification.
As explained in [0086]-[0087] of the specification, the present application aims to make CNTs not prone to be entangled with other silicon-based particles and the silicon-based particles being homogeneously dispersed in the graphite. The cited prior art provides no teaching.
The Examiner respectfully disagrees and notes that, as set forth in the rejection of record, the newly cited prior art discloses a dispersing the CNTs and the polymer in a solvent, such as water ([0027]-[0033], [0036], e.g. [0062] of Deng).
The Examiner further notes that modified Oh does not disclose some of the mixing speeds and times recited by the method disclosed in the instant specification. However, such do not appear to be critical in achieving the claimed effects in light of Tables 1-3 of the instant specification.
For example, the instant specification does not set forth a required mixing speed and time nor discuss the mixing speed and time as being critical parameters for achieving the claimed invention.
Specifically, the Examiner notes that the mixing speed and time referenced by the Applicant are ones used in an exemplary embodiment. However, the instant specification explicitly recites that the embodiments of the application shall not be construed as a limitation on the application ([0017]).
Furthermore, the Applicant has not provided any evidence showing that different mixing speeds and times produce different results. For example, see Tables 1-3 of the instant specification, which demonstrate differences between exemplary embodiments and comparative embodiments when parameters are changed, such as the temperature of thermal processing after grading or the amounts of the silicon-containing substrate, CNTs, graphite, polymer, binder, and conductive agent used in the negative electrode. None of Tables 1-3 reference a stirring speed and time.
Therefore, the Applicant has not met the burden of proof that the cited prior art does not necessarily or inherently possess the claimed ratio M, see MPEP 2112(V).
Lastly, the Examiner notes that [0086]-[0087] of the instant specification discloses that when carbon nanotubes are bound by the polymer onto the surface of the silicon-containing substrate (e.g. are dispersed in the polymer layer), the CNTs are not prone to be entangled with other silicon-based particles.
In other words, [0086]-[0087] discusses the significance of the polymer layer comprising the polymer and the carbon nanotubes, not the mixing speed and time.
Thus, the arguments are not found to be persuasive.
Applicant’s arguments with respect to new Claim 19 have been considered but are moot because the new ground of rejection does not rely on any reference applied in the prior rejection of record for any teaching or matter specifically challenged in the argument.
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.
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/KIMBERLY WYLUDA/Primary Examiner, Art Unit 1725
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