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 .
Status of Application
Claim 1 is amended, claims 4 and 6 are canceled, and claim 13 is new, submitted on 6/6/2025. Claims 1-2, 7, and 13 are presented for examination.
Claim Rejections - 35 USC § 103
1. 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.
2. 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.
3. 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.
4. Claims 1-2, 7, and 13 are rejected under 35 U.S.C. 103 as being unpatentable over Toya (US 20170324081 A1), in view of Akagi (US 20100117031 A1, IDS of 3/18/2022), further in view of Endo (US 20200381720 A1-Priority to 12/15/2017) and Lee (US 20180212237 A1).
Regarding claim 1, Toya discloses the method for manufacturing the composite hydroxide particles by crystallization reaction comprising: a) nucleation step for performing nucleation, and b) a particle growth step that grows the nucleus that was produced in the nucleation process ([0098] and Fig. 2B) and a particle growth step after nucleation ended ([0222]). The nucleation step is for performing nucleation ([0098]). In Example 1, Toya discloses the nucleation step of adding dissolved nickel sulfate and manganese sulfate mixed solution to a reaction tank which contains sodium hydroxide aqueous solution with adjusted pH value of 13.1 ([0219]), which is substantially equivalent to the claimed “a first step of adding to a reactor, a reaction solution comprising a transition metal-containing solution containing at least one of nickel, cobalt, or manganese, a basic aqueous solution to form seeds of precursor particles;” because nucleation of Toya corresponds to forming the seeds of precursor particles in the instant claim.
While Toya does not explicitly disclose preparing carbon-induced precursor particles by adding a carbon source comprising at least one carbon compound to the reactor when the seeds of precursor particles grow to an average particle diameter (D50) of the precursor particles is 30% in size of the average particle diameter (D50) of finally prepared precursor particles, Toya discloses a second step after nucleation ended (particle growth step, [0222]) of the seeds (nuclei, [0126]) of precursor particles (the composite hydroxide particles, [0127]) grow to a desired particle size by controlling the time of the particle growth step ([0127]). Toya further discloses in the case of the secondary particles, the thickness of the outer shell section is 10 to 45% the particle size of the secondary particles, … the cathode active material that is obtained with the composite hydroxide above as the raw material has hollow structure, and the ratio of the thickness of the outer shell section with respect to the particle size is maintained at that ratio for the composite hydroxide secondary particles above ([0083]) in order to balance the strength of the lithium nickel manganese composite oxide particles and the surface area that contributes to the battery reaction, for achieving a balanced optimization of cathode resistance and output characteristics ([0164]). The thickness of the outer shell section is 10 to 45% the particle size of the secondary particles having hollow structure, translates to particle growth step from an average particle diameter (D50) of the precursor particle is 10 to 45% in size of the average particle diameter (D50) of finally prepared precursor particles, encompassing the 30% in size as claimed.
Therefore, a skilled artisan would have found it obvious before the effective filing date of the claimed invention, to arrive at the seeds of precursor particles grow to an average particle diameter (D50) of the precursor particles is 30% in size of the average particle diameter (D50) of finally prepared precursor particles, as disclosed by Toya by controlling the time of particle growth step, in order to balance the positive electrode resistance and output characteristics, without undue experimentation and with a reasonable expectation of success.
Toya further discloses in Example 6, adding the aqueous solution for nucleation after the nucleation step to a component adjustment solution that was prepared separately from the aqueous solution of nucleation to form a reaction solution and performing the particle growth step with this reaction solution as the particle growth aqueous solution ([0265]). While Toya discloses the desire of making particles that are porous, or that have a hollow particle structure to increase the surface area that contributes to the battery reaction and reduce the reaction resistance in order to make a battery with high output ([0021]); and renders it obvious as set forth above that the seeds of precursor particles grow to an average particle diameter (D50) of the precursor particles is 30% in size of the average particle diameter (D50) of finally prepared precursor particles, Toya does not explicitly disclose the component adjustment solution contains a carbon source comprising at least one carbon compound.
Akagi teaches a method for producing a positive electrode active material for a battery having excellent discharge characteristics ([0001]) and the easy regulation of pores size can be realized by removing carbon particles mixed in a raw material for a positive electrode active material in firing, and a positive electrode active material for a battery having excellent high-rate discharge characteristics can be obtained ([0019]). Akagi further teaches adding Ketjenblack EC carbon particles to lithium manganate dispersion liquid followed by firing the mixture at 800° C, and in this process, most of the carbon particles were oxidized and evaporated, and only the sintered lithium manganate particles were left on the positive electrode active material fired body ([0087-0088]), which corresponds to the claimed “a second step of preparing carbon-introduced precursor particles by adding a carbon source comprising at least one carbon compound to the reactor; and a third step of mixing the carbon-introduced precursor particles and a lithium raw material to obtain a mixture and sintering the mixture at a temperature of 750 0C to 950 0C to prepare positive electrode active material particles, wherein the carbon source introduced to the seeds of precursor particles is volatilized by the sintering in the third step to form cavities in the positive electrode active material particles.”
It would have been further obvious for a skilled artisan before the effective filing date of the claimed invention, to modify the component adjustment solution of Toya with a carbon source comprising at least one carbon compound followed by firing the mixture at 800° C, as taught by Akagi, to realize easy regulation of pore size and obtain a positive electrode active material for a battery having excellent high-rate discharge characteristics, in order to make a battery with high-output as desired by Toya, and thus arrive at the claimed “a second step of preparing carbon-introduced precursor particles by adding a carbon source comprising at least one carbon compound to the reactor; and a third step of mixing the carbon-introduced precursor particles and a lithium raw material to obtain a mixture and sintering the mixture at a temperature of 750 0C to 950 0C to prepare positive electrode active material particles, wherein the carbon source introduced to the seeds of precursor particles is volatilized by the sintering in the third step to form cavities in the positive electrode active material particles”.
Modified Toya further discloses the cathode active material was spherical, had mostly a uniform particle size and had hollow structure ([0263]), in Table 2, the ratio of the outer shell thickness section with respect to the particle size was 14.1% (Example 2, [0248] and Table 2); and Akagi further teaches easy regulation of pore size in porosity formation of a positive electrode active material and is less likely to undergo hindrance of ion conduction caused by residues and, thus can realize excellent high-rate discharge characteristics ([0014]); the average diameter of the carbon particles can be adjusted ([0040]) and the content of the carbon particles in the mixture is preferably 0.1 to 30% by weight in view of appropriately securing the pore diameter and of securing the sufficient sintering of the positive electrode active material particles ([0041]) and the average particle diameter of the raw material for the positive electrode active material and the average particle diameter of the carbon particles or the like are desirably adjusted ([0056]); in view of the balance between porosity required for the movement of the Li ions and energy density, the total pore volume of the positive electrode active material measured by the mercury porosimeter is preferably 0.1 to 1 cc/g, and more preferably 0.35 to 0.7 cc/g ([0065]). In Table 1-1 on P11, Akagi teaches the content of carbon particles in mixture is 3.8 wt% for Examples 1-3.
However, modified Toya does not explicitly disclose the porosity of the positive electrode active material is 5-20%, and the carbon source is added so that the carbon compound is 20 vol% or less with respect to 100 vol% of total precursor particles. (Examiner notes: cavity ratio in the instant claim is interpreted as substantially equivalent to porosity in the battery art as evidenced by Lee (Lee [0036]).
Endo teaches when a lithium transition metal composite oxide with controlled porosity is in a specific range, a lithium excess type positive active material exhibits excellent energy efficiency can be obtained ([0046]) due to an achieved balance between the number of reaction points and oxidation decomposition of an electrolyte solution on an active material surface during charging ([0047]). Endo further teaches a lithium transition metal composite oxide has a porosity of 5 to 15% ([0060]), which falls within the claimed range of “a cavity ratio of the positive electrode active material is 5-20%”.
A skilled artisan would have found it obvious before the effective filing date of the claimed invention to control and prepare the positive electrode active material of modified Toya with a porosity that falls within the range of 5-15%, as taught by Endo, in order to balance between the number of reaction points and oxidation decomposition of an electrolyte solution on an active material surface during charging, and achieve a lithium excess type positive active material exhibiting excellent energy efficiency.
Further, since modified Toya has rendered obvious as set forth above that a carbon source being introduced to the precursor particles to form cavities in the positive electrode active material particles after being volatilized by the sintering in the third step, and porosity in calculated by volume, it would have been further obvious for a skilled artisan before the effective filing date of the claimed invention to control the carbon source, at least one carbon compound, which is added to form the at least a part of the porosity to have volume being 5-15 vol% with respect to 100 vol% of total precursor particles, therefore arrive at the claimed “the carbon source is added so that the carbon compound is 20 vol% or less with respect to 100 vol% of total precursor particles.”
Modified Toya further discloses adding the aqueous solution for nucleation after the nucleation step to a component adjustment solution that was prepared separately from the aqueous solution of nucleation to form a reaction solution and performing the particle growth step with this reaction solution as the particle growth aqueous solution ([0265]), the average particle size of the composite hydroxide particles was 4.1 µm ([0265]) and the secondary particles were spherical with a center section having primary particles with a particle size of 0.04 µm and an outer shell section having plate shape or needle shaped primary particles with a particle size of 0.9 µm; the thickness of the outer shell section being 1.1 µm and the ratio of the thickness of the outer shell section with respect to the particle size being 26.8% ([0267]), which translates to the component adjustment solution was added when the average particle diameter (D50) of the seeds of the precursor particles was grown to 4.1-1.1=3 µm, falling within the range of claimed “wherein when the average particle diameter (D50) of the seeds of the precursor particles is grown to 1 µm to 7 µm in the second step.”
However, modified Toya does not explicitly disclose that the cavity ratio is determined by: cutting positive electrode active material particles using a focused ion-beam, taking a cross-sectional image of the positive electrode active material particles, and calculating a ratio of a total area of the cavity with respect to a cross-sectional area of the positive electrode active material particles based on the cross-sectional image.
Lee teaches a secondary battery positive electrode active material which includes a core; a shell located to around the core; and a buffer layer located between the core and the shell (Abstract and FIG. 1) with a porosity of 5 vol% to 25 vol% with respect to a total volume of the positive electrode active material, measured by cross-section analysis of particles using a focused ion beam (FIB) or mercury intrusion ([0036]) and the precursor manufactured was observed by field emission scanning electron microscopy (FE-SEM) to calculate diameters and volumes of the core and the shell ([0195]). Therefore, a skilled artisan would have found it obvious before the effective filing date of the claimed invention to choose FIB-FE-SEM method taught by Lee for measuring the cavity ratio of modified Toya, and thus arrive at the claimed “the cavity ratio is determined by: cutting positive electrode active material particles using a focused ion-beam, taking a cross-sectional image of the positive electrode active material particles, and calculating a ratio of a total area of the cavity with respect to a cross-sectional area of the positive electrode active material particles based on the cross-sectional image”, without undue experimentation and with a reasonable expectation of success.
Toya does not explicitly disclose the at least one carbon compound is selected from the group consisting of carbon black, acetylene black, Ketjen black, channel black, furnace black, lamp black, thermal black, carbon fibers, and carbon nanotubes.
Akagi teaches the carbon particles easily employing a structure are preferable in view of securing the pore diameter and the pore volume. For example, a carbon fiber…, active carbon, and carbon black are preferable ([0037]). Akagi further teaches Ketjenblack EC ([0087]), carbon black ([0090]) being used as carbon compound, which reads on that the at least one carbon compound is selected from the group consisting of carbon black, Ketjen black and carbon fibers.
It would have been obvious for a skilled artisan before the effective filing date of the claimed invention, to choose the carbon source of modified Toya from the carbon source comprising at least one carbon compound selected from the group consisting of carbon black, Ketjen black and carbon fibers, as taught by Akagi, to realize easy regulation of pore size and obtain a positive electrode active material for a battery having excellent high-rate discharge characteristics, in order to make a battery with high-output as desired by Toya.
While modified Toya does not explicitly disclose an average particle diameter (D50) of the carbon compound being from 10 nm to 1 µm, modified Toya discloses the thickness of the outer shell section was 1.1 µm ([0267]) and the pores formed in the outer shell appear to be between 10 nm to 1 µm (FIG. 6). Based on these information, a skilled artisan would reasonably choose the carbon compound with an average particle diameter (D50) to be between 10 nm to 1 µm, in view of securing the pore diameter and the pore volume taught by Akagi (Akagi [0040-0041]), in order to obtain the pore size of the shell portion as shown in FIG. 6 of Toya, which renders obvious the claimed “the carbon compound has an average particle diameter (D50) of 10 nm to 1 µm”.
Akagi teaches the average particle diameter of the raw material for the positive electrode active material and the average particle diameter of the carbon particles or the like are desirably adjusted ([0056]) between 0.1 to 10 µm ([0061]), overlapping the claimed range of 10 nm to 1 µm. A skilled artisan would reasonably choose a carbon particle with an average particle size that falls within the overlapping portion (0.1 to 1 µm) between the Akagi taught range and the claimed range without undue experimentation and with a reasonable expectation of success.
Regarding claim 2, modified Toya discloses all of the limitation as set forth above. Toya further discloses the finally prepared precursor particles (composite hydroxide particles, [0266]) have an average particle diameter (D50) ([0094]) of 4.1 µm, which falls within the claimed range of “2 µm to 20 µm”.
Regarding claim 7, modified Toya discloses all of the limitation as set forth above. While Toya discloses desire of making particles that are porous, or that have a hollow particle structure to increase the surface area that contributes to the battery reaction and reduce the reaction resistance in order to make a battery with high output ([0021]), and the cathode active material was spherical, had mostly a uniform particle size and had hollow structure ([0263]), Toya does not explicitly disclose the porosity of the positive electrode active material is 5-15%.
Endo teaches the porosity of the positive electrode active material is 5-15% ([0060]) and the claimed limitation has been rendered obvious as set forth above in rejection to claim 1.
Regarding claim 13, modified Toya discloses all of the limitation as set forth above. As set forth in claim 1, similarly, while modified Toya does not explicitly disclose an average particle diameter (D50) of the carbon compound being from 10 nm to 100 nm, modified Toya discloses the thickness of the outer shell section was 1.1 µm ([0267]) and the pores formed in the outer shell appear to be between 10 nm to 100 nm (FIG. 6), a skilled artisan would reasonably choose the carbon compound with an average particle diameter (D50) to be between 10 nm to 100 nm, in view of securing the pore diameter and the pore volume taught by Akagi (Akagi [0040-0041]), in order to obtain the pore size of the shell portion as shown in FIG. 6 of Toya, thus arrive at the claimed “the carbon compound has an average particle diameter (D50) of 10 nm to 100 nm” without undue experimentation and with a reasonable expectation of success.
Response to Arguments
5. Applicant’s arguments regarding the amended claim 1 filed on 6/6/2025 have been fully considered but are not found persuasive.
Applicant argues about criticality and excellent effect of the claimed range “the carbon compound has an average particle diameter (D50) of from 10 nm to 1 µm”, by citing instant disclosure [0050-0051]), and further referring to comparative example 4 vs. Example 1 to demonstrate the Comparative Example 4 showing a cavity ratio exceeding 20% such that the tap density was deteriorated over that of the Examples, resulting in capacity and resistance properties as well as energy density were remarkably inferior using thereof.
Examiner respectfully submits that since modified Toya discloses the thickness of the outer shell section was 1.1 µm ([0267]) and FIG. 6 appears to show the pores formed in the outer shell between 10 nm to 1 µm, a skilled artisan would reasonably choose the carbon compound with an average particle diameter (D50) to be between 10 nm to 1 µm, in order to secure the pore size of the shell portion to be between 10 nm to 1 µm as shown in FIG. 6 of Toya.
Alternatively, since Akagi teaches the average particle diameter of the carbon particles can be adjusted between 0.1 to 10 µm ([0061]) in view of securing the pore diameter and the pore volume (Akagi [0040-0041]), a skilled artisan would reasonably choose an average particle diameter (D50) value that falls within the overlapping portion between the taught range and the claimed range.
Since modified Toya would be expected to have a maximum carbon particle size of 1.1 micron, and as taught by Akagi would be reasonably having the overlapping portion (0.1 to 1 µm) of the Akagi’s taught range and the claimed range, to fit within the outer shell dimension requirement as shown in FIG. 6 of Toya, and further in view of Endo (Endo [0060]) as set forth in rejection to claim 1, modified Toya has rendered obvious a cavity ratio of the positive electrode active material is 5-20%. Therefore, modified Toya’s positive electrode active material would necessarily and inherently possess same properties as what the Applicant considered as excellent effect referring to the comparison of comparative example 4 vs. Example 1, such that the difference in results would not have been unexpected.
Moreover, regarding Applicant cited comparison (the comparative Example 4 vs Example 1) as evidence for criticality, it appears to be unpersuasive because according to Table 1 of the instant disclosure, at least the positive electrode active material particle sizes and BET data are both different for comparative Example 4 and Example 1. Therefore, it is not convincing that the achieved excellent effects regarding capacity and resistance properties as well as energy density is solely due to the claimed limitation “the carbon compound has an average particle diameter (D50) of from 10 nm to 1 µm”.
Conclusion
6. THIS ACTION IS MADE FINAL. 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 extension fee 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 date of this final action.
7. Any inquiry concerning this communication or earlier communications from the examiner should be directed to KAN LUO whose telephone number is (571)270-5753. The examiner can normally be reached 8:00AM -5:00PM ET. ET.
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/K. L./Examiner, Art Unit 1751 8/21/2025
/JONATHAN G LEONG/Supervisory Patent Examiner, Art Unit 1751 8/21/2025