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 .
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and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114.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 June 5, 2025 has been entered.
Status of Application
Claim 1 is amended, claim 10 is cancelled, claim 12 is withdrawn and claim 13 is new, submitted on June 5, 2025. Claims 6-8 remain withdrawn and claims 1-5, 9, 11, and 13 are presented for examination.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, 4-5, 9, 11, and 13 are rejected under 35 U.S.C. 103 as being unpatentable over Gunji (US 20170358799 A1, IDS of 10/27/2021) in view of Oh (US 20200335782 A1 - Priority to 10/30/2017), further in view of Xiong (Journal of Power Sources 222 (2013) 318-325).
Regarding claim 1, Gunji discloses a positive electrode active material for a lithium ion secondary battery (Li1+aNibMncCodTieMfO2+α, Abstract), comprising a lithium-nickel-manganese composite oxide (Li1.02Ni0.79Mn0.05Co0.15Ti0.01O2+α, Example 7 in TABLE 1A on P12) configured by secondary particles with a plurality of aggregated primary particles ([0052]),
wherein the lithium-nickel-manganese composite oxide has a hexagonal layered structure (R-3m layered structure, [0058]) and contains lithium (Li), nickel (Ni), manganese (Mn), an element M(M) that is at least one element selected from the group consisting of Co, V, Mg, Mo, Nb, Ca, Cr, Zr, Ta, and Al, and titanium (Ti) as metal elements (Li1.02Ni0.79Mn0.05Co0.15Ti0.01O2+α, Example 7 in TABLE 1A on P12),
a mole number ratio of the metal elements Li : Ni : Mn : M: Ti is represented as a : (1 - x - y-z) : x: y: z, respectively, provided that 0.97≤a≤1.25, 0.05≤x≤0.15, 0≤y≤0.15, and 0.01≤z≤0.05 (Li1.02Ni0.79Mn0.05Co0.15Ti0.01O2+α, Example 7 in TABLE 1A on P12).
Gunji further discloses that as shown in FIG. 5, a covering layer (different phase) like LiTiO2 was not seen ([0144]); and when a, which indicates the amount of excess or deficiency of Li in the composition formular, in the range of 0 to 0.06 and e, which indicates the Ti content in the range of 0.005 to 0.15, and a ratio of a/e of less than or equal to 5, it is considered that a different phase like a Li-Ti-O compound was not generated ([0144]), which means Example 7 with a formula of Li1.02Ni0.79Mn0.05Co0.15Ti0.01O2+α (TABLE 1A on P12) does not have a separate phase of LiTiO2.
While Gunji does not explicitly disclose the titanium oxide used for preparation of Example 7 being completely reacted to form the titanium doped lithium-nickel-manganese composite oxide (Li1.02Ni0.79Mn0.05Co0.15Ti0.01O2+α), Gunji discloses an object to provide a positive-electrode material for a lithium ion secondary battery that has a higher charge-discharge capacity than those of the conventional lithium ion secondary batteries and also has a suppressed resistance increase rate and excellent cycle characteristics ([0011]); a desire to control an unreacted Li raw material; and a third heat treatment step S23 at temperature equal to 900° C. for a period of greater than or equal to 0.5 hour and less than or equal to 50 hours for a lithium complex compound ([0082]).
Oh teaches a similar desire of having a cathode active material with increased c-axis lattice constant and powder resistivity of the lithium metal oxide thereby having the effect of improving the power characteristics at low temperature ([0020]) by doping the lithium metal oxide with a dopant (M) ([0019]); and in an embodiment using TiO2 for doping Ti ([0054]), dopant (M) is Ti (claim 3). Oh further teaches it is preferable to choose the sintering conditions with the sintering holding temperature of 900 to 1000° C., and the sintering holding time of 10 to 20 hours that may form a layered crystal structure without impurities ([0054]).
Since Gunji discloses the heat treatment condition falls within the range of the sintering conditions taught by Oh, a skilled artisan would reasonably expect that the Example 7 of Gunji with a formula of Li1.02Ni0.79Mn0.05Co0.15Ti0.01O2+α (TABLE 1A on P12) would have no impurities (TiO2) remaining in the layered crystal structure of the titanium doped lithium-nickel-manganese composite oxide with a modified heat treatment temperature equal to 900° C. for a period of greater than or equal to 0.5 hour and less than or equal to 50 hours, thus arriving at the claimed feature “a ratio of a total amount of peak intensities of most intense lines of a titanium compound to a (003) diffraction peak intensity that is the most intense line of a hexagonal layered structure in XRD measurement of the positive electrode active material is 0”, because there is no different phase like a Li-Ti-O compound generated and there is no unreacted TiO2 as impurities either.
Modified Gunji further discloses the average particle size of the primary particles of the positive-electrode material is preferably greater than or equal to 0.1 µm and less than or equal to 2 µm, for example ([0053]). FIG. 9A shows a photograph of a cross-section of the positive-electrode material of Example 2 after 0 cycle ([0027]) and a primary particle size of about 200 nm, which inherently discloses a crystallite diameter range from equal to or smaller than 100 nm to about 200 nm, overlapping the diameter range of a crystallite diameter as claimed “a crystallite diameter at (003) plane as determined by the XRD measurement is 177.8 nm or more and 234.7 nm or less”. A skilled artisan would have found it obvious before the effective filing date of the claimed invention to arrive at a crystallite diameter value that falls within the overlapping portion (from 177.8 nm to 200 nm) of the taught range and the claimed range without undue experimentation.
While Gunji discloses the concern that if the amount of unreacted Li raw material is large, dissolution of the Li raw material will occur, and the particles will be likely to grow due to liquid-phase sintering. Excessive growth of the particles will lead to a decrease in the charge-discharge capacity ([0081]) and through heat treatment, the amount of an unreacted Li raw material can be controlled ([0081]), and the amount of excess or deficiency of Li in the composition of formula, in the range of 0 to 0.06 ([0144] and Table 1), Gunji does not explicitly disclose water-washing the positive electrode active material.
Xiong teaches the effect of water washing on electrochemical performance and storage characteristics of LiNi0.8Co0.1Mn0.1O2 as cathode material for lithium-ion batteries (Title) and water washing can improve the cycling performance and structure stability of LiNi0.8Co0.1Mn0.1O2 material in electrolyte (Abstract).
It would have been obvious before the effective filing date of the claimed invention, for one having ordinary skill in the art to water wash the positive electrode active material of Gunji, as taught by Xiong, in order to improve the cycling performance and structure stability of the positive active materials in electrolyte. And it would have been further obvious before the effective filing date of the claimed invention, for one having ordinary skill in the art to recognize an amount of lithium to be eluted in water would necessarily be less than 0.07% by mass with respect to the entire positive electrode active material because Li is the lightest element in the formula, and the amount of excess or deficiency of Li in the composition of formula, in the range of 0 to 0.06, thus arriving at the claimed “an amount of lithium to be eluted in water when the positive electrode active material is immersed in water is 0.07% by mass or less with respect to the entire positive electrode active material”.
Regarding claim 2, modified Gunji discloses all of the limitations as set forth above. While modified Gunji does not explicitly disclose 0.03≤z≤0.05, modified Gunji further discloses the range of e, which indicates the Ti content in Formula (1) Li1+aNibMncCodTieMfO2+α ([0040-0041]), from perspectives of obtaining the advantageous effect of adding Ti and suppressing an increase in the material cost and improving the sintering property of the positive-electrode material, e is further preferably greater than or equal to 0.005 and less than or equal to 0.05 ([0063]), which encompasses the claimed range of Ti content as 0.03≤z≤0.05 with the same higher end value of 0.05. It would have been obvious for an ordinary skilled artisan before the effective filing date of the claimed invention, to arrive at a z value for Ti content that falls within the overlapping portion (0.03≤z≤0.05) between the range taught by Gunji and as claimed, in order to achieve an optimized balance between having the advantageous effects of adding Ti and suppressing an increase in the material cost and improving the sintering property of the positive-electrode material.
Regarding claim 4, modified Gunji discloses all of the limitations as set forth above. While modified Gunji further discloses the average particle size of the secondary particles of the positive-electrode material is preferably greater than or equal to 3 µm and less than or equal to 50 µm ([0053]), which encompasses the range as claimed “a volume average particle diameter Mv is 8 µm or more and 20 µm or less”, modified Gunji does not specifically mention the particle size of Example 7.
However, modified Gunji further discloses Example 1 which has a similar composition as that of Example 7, the Example 1 positive-electrode material particles with secondary particle sizes of 5 to 10 µm were selected ([0118]), which falls within the range as claimed “a volume average particle diameter Mv is 8 µm or more and 20 µm or less”. It would have been obvious for an ordinary skilled artisan before the effective filing date of the claimed invention, to have adjusted the volume average particle diameter of Example 7 as taught by Example 1 of modified Gunji, with a reasonable expectation that this selected average particle size of the secondary particles would make a successful positive-electrode material.
Regarding claim 5, modified Gunji discloses all of the limitations as set forth above. Modified Gunji further discloses in order to balance between the filling property of the positive-electrode material and thus high energy density, and the area in contact with an electrolyte solution and thus suppress an increase in the resistance ([0056]), the BET specific surface area of the positive-electrode material is preferably about greater than or equal to 0.2 m2/g and less than or equal to 2.0 m2/g ([0056]), which encompasses the range of 0.4 m2/g or more and 1.5 m2/g or less as claimed “wherein the specific surface area measured by a BET method is 0.4 m2/g or more and 1.5 m2/g or less”. It would have been obvious for an ordinary skilled artisan before the effective filing date of the claimed invention, to have adjusted the BET specific surface area of the positive-electrode material and arrive at the claimed specific surface area measured by a BET method being 0.4 m2/g or more and 1.5 m2/g or less, with a reasonable expectation of success, in order to balance between the filling property of the positive-electrode material and thus high energy density, and the area in contact with an electrolyte solution and thus suppress an increase in the resistance.
Regarding claim 9, modified Gunji discloses all of the limitations as set forth above. Modified Gunji further discloses a lithium ion secondary battery ([0098]) comprising: a positive electrode ([0098]); a negative electrode ([0100]); and a non-aqueous electrolyte ([0098]), the positive electrode containing the positive electrode active material according to claim 1 ([0098]).
Regarding claim 11, modified Gunji discloses all of the limitations as set forth above. As established above in claim 1, Example 7 of modified Gunji with a formula of Li1.02Ni0.79Mn0.05Co0.15Ti0.01O2+α (TABLE 1A on P12) has no different phase like a Li-Ti-O compound generated, and no impurities of TiO2, the titanium is necessarily and inherently uniformly solid-solved in the primary particles because otherwise, there would present a different Ti containing phase.
Regarding claim 13, modified Gunji discloses all of the limitations as set forth above. As established above in claim 1, modified Gunji inherently discloses a crystallite diameter ranging from equal to or smaller than 100 nm to about 200 nm, overlapping the diameter range of a crystallite diameter as claimed “a crystallite diameter at (003) plane as determined by the XRD measurement is 180 nm or more and 234.7 nm or less”. A skilled artisan would have found it obvious before the effective filing date of the claimed invention to arrive at a crystallite diameter value that falls within the overlapping portion (from 180 nm to 200 nm) of the taught range and the claimed range without undue experimentation.
5. Claim 3 is rejected under 35 U.S.C. 103 as being unpatentable over Gunji (US 20170358799 A1, IDS of 10/27/2021) in view of Oh (US 20200335782 A1 - Priority to 10/30/2017) and Xiong (Journal of Power Sources 222 (2013) 318-325), as applied to claim 1, further in view of Kaneda (US 20190252681 A1 - Priority to 7/29/2016).
Regarding claim 3, modified Gunji discloses all of the limitations as set forth above. While modified Gunji further discloses the object to provide a positive-electrode material for a lithium ion secondary battery that has a higher charge-discharge capacity than those of the conventional lithium ion secondary batteries and also has a suppressed resistance increase rate and excellent cycle characteristics ([0011]) and the average particle size of the secondary particles of the positive-electrode material is preferably greater than or equal to 3 µm and less than or equal to 50 µm ([0053]), modified Gunji does not explicitly disclose wherein [(D90 - D10)/Mv] calculated by D90 and D10 based on a volume standard in a particle size distribution by a laser diffraction scattering method and a volume average particle diameter (Mv) and indicating a variation index of particle size is 0.80 or more and 1.20 or less.
Kaneda teaches a method for producing a positive electrode active material for a nonaqueous electrolyte secondary battery (Formula (2),[0085]), having extremely high output characteristics and having sufficient energy density ([0016]). Kaneda further teaches the composite hydroxide 1 preferably has [(D90 - D10)/an average particle diameter] as an indicator indicating a spread of particle size distribution of at least 0.7. This can improve particle fillability and further increase the volume energy density. The upper limit of [(D90 - D10)/an average particle diameter], is preferably up to 1.2, in view of inhibiting excessive mixing of fine particles or coarse particles into the positive electrode active material ([0046]). Kaneda further teaches in Example 1, the volume-average particle diameter MV was 10.1 µm, and [(D90 - D10)/an average particle diameter] was 0.91, which falls within the range of 0.8 or more and 1.20 or less as claimed “wherein [(D90 - D10)/Mv] calculated by D90 and D10 based on a volume standard in a particle size distribution by a laser diffraction scattering method and a volume average particle diameter (Mv) and indicating a variation index of particle size is 0.80 or more and 1.20 or less.”
It would have been obvious for an ordinary skilled artisan before the effective filing date of the claimed invention, to have further modifying the value of [(D90 - D10)/Mv] calculated by D90 and D10 based on a volume standard in a particle size distribution by a laser diffraction scattering method and a volume average particle diameter (Mv) and indicating a variation index of particle size of Gunji, arriving at a value that falls within the overlapping portion (from 0.8 to 1.2) of the Kaneda taught range and the claimed range, with a reasonable expectation of success achieving extremely high output characteristics and having sufficient energy density without undue experimentation. [MPEP 2144.05(II)].
Response to Arguments
6. Applicant’s arguments filed on 6/5/2025 have been fully considered but they are not found fully persuasive and moot in view of the new ground(s) of rejection.
First, regarding the amended claim 1 the Applicant argues about expected results by stating a primary particle size measured under SEM can be different from a crystallite size measure by XRD for the same material thus, it is not inherent that Gunji has the crystallite size smaller than 200 nm, citing WO2017/221554 (US20190207215 for citation purpose) as supporting material. (Remarks P9-10).
The Examiner respectfully acknowledges the fact that primary particles are not necessarily formed of a single crystallite, may contains plural crystallites. However, Examiner fails to find this argument persuasive for the following reasons: Gunji discloses the average particle size of the primary particles of the positive-electrode material is preferably greater than or equal to 0.1 µm ([0053]), which means the size of a crystallite of the positive-electrode material of Gunji should be about or smaller than 100 nm in light of the lower end of primary particle size being greater than or equal to 0.1 µm. Gunji further discloses the primary particle size of about 200 nm (FIG. 9A), which at least means the crystallite size should be smaller than 200 nm. Therefore, Gunji at least inherently discloses the crystallite size range can be from about or smaller than 100 nm to 200 nm, which overlaps the claimed range of crystallite diameter being 177.8 nm or more and 234.7 nm or less. A skilled artisan would have found it obvious to arrive at a crystallite diameter value that falls within the overlapping portion of Gunji’s taught range and the claimed range (177.8 nm to 200 nm) without undue experimentation. Thus this argument is not persuasive.
Further, the instant disclosure provides evidence that support the Office’s standing, quote “preferably 160 nm or more and 300 nm or less, and may be 170 nm or more and 280 nm or less or may be 180 nm or more and 250 nm or less” and “by setting the crystallite diameter at (003) plane in the above range, both battery characteristics and thermal stability can be achieved at a high level” ([0066]). Since the crystallite size of Gunji falls within the range as the instant disclosure provides, the battery characteristics and thermal stability achieved at a high level are expected properties from Gunji, contrary to the Applicant’s unexpected results argument.
The supporting material WO2017/221554 (US20190207215 for citation purpose) cited by the Applicant has been considered and the Examiner has not found it persuasive since all the working Examples in Table 4 do not have Ti constituent (see Table 1), which is different from the composition of the instant claim 1. The Examiner further notes that Kaneda (US 20190252681 A1) cited in rejection to claim 3 does not have Comparative Example 4 in Table 1, nor showing the maximum crystallite diameter was 144 nm, contrary to the Applicant’s mentioning on P11, thus this portion of argument is unpersuasive.
Second, the Applicant argues against the rejection to claim 11 in that the claimed material has unexpected result by referring to FIG. 4B of Gunji’s Example 4 that Ti is concentrated at the top surface of the primary particles that are located on the surface of the secondary particles and at 5 nm depth from the surface of those secondary particles. (Remarks P11-12).
The Examiner respectfully submits that Example 4 of Gunji and its associated FIG. 4B were not cited in the rejection of claim 1, because Example 4 has a formula outside of the claimed range with respect to the constituent of Mn (0.04) while the claim requires Mn constituent with subscript of x, and 0.05≤x≤0.15. The rejection to claim 1 is based on Example 7 which has a different composition from Example 4, thus this argument is not responsive to the previous rejection and is moot. Further, there is no evidence supporting that the Ti detected at 5 nm depth from the surface shown in FIG. 4B (Example 4) represents a titanium compound as claim 1 requires, rather than Ti metal, thus this argument is not found persuasive either.
Further, regarding claim 11, the Examiner notes since Gunji’s Example 7 has rendered obvious that it has no different phase like a Li-Ti-O compound generated, and no impurities of TiO2, as set forth in rejection to claim 1, the titanium is necessarily and inherently uniformly solid-solved in the primary particles.
Conclusion
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 9/29/2025
/JONATHAN G LEONG/Supervisory Patent Examiner, Art Unit 1751 9/30/2025