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and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114.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 10 June 2026 has been entered.
Response to Amendment
Applicant amended claim 1, and cancelled claim 11. The rejection of claim 11 is withdrawn because it was cancelled. Claims 1, 3-4, 9-10, and 12-15 are pending and considered in the present Office action.
The rejections of claims 1, 3-4, 9-10, and 12-15 are maintained with the art of record, and a new ground of rejection is presented in view of new art.
Response to Arguments
Applicant’s main argument is that Kim suggests a secondary particle (aggregation of primary particles), hence does not suggest the “single particle” recitation of the claim. Applicant’s argument is not persuasive and Kim’s primary particles read on the “single particle” feature of claim 1.
The secondary particles of Kim are indeed the aggregation of primary particles; however, the fact that the primary particles are aggregated into secondary particles is moot since the claims are not limited to exclude secondary particles. The primary particle read on the claimed “single particle”.
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The particle morphology depicted in Fig. 2b shows the aggregation of primary particles forming the secondary particle. Specifically, the primary particles are needle shaped, having a length and width and an aspect ratio greater than 1 (e.g., elongated shape), thereby extending from the center of the secondary particle to the surface thereof. Kim suggests the Co gradient is present at the surface of the secondary particle (concentration gradient layer), hence at the surface of each primary particle (see e.g., Fig. 1). Further, the average particle diameter is suggested as 10-11 µm (Table); since the primary particles extend from the center to the surface of the secondary particle, the particle diameter of each primary particle (hence each single particle) is about 5µm (i.e., particle diameter of each primary particle is the radius of the secondary particle), which overlaps with that claimed.
Applicant also argues that cobalt is present in the central portion. Kim suggests the core layer has the formula (1); formula (1) suggests the amount of cobalt (Coa) is zero, see claim 9 of Kim; thus, Kim reads on the absence of Co in the core layer (first portion/inner portion).
Applicant argues the claimed objective is that the active material itself is in the form of a primary particle, while Kim’s objective (i.e., “improve battery capacity, output characteristics, and lifespan by arranging primary particles …to have a particular orientation…”) differs from that claimed; these arguments are not persuasive. Regardless of Kim’s objective, since the claim is not limited to exclude secondary particles, Kim’s disclosure of the primary particle reads on the claimed “single particle”.
Applicant argues Kim does not suggest either the composition or internal structure of the primary particles themselves, and mentions the inclusion of Na, W, Mg and Ti was not disclosed for the purpose of maintaining crystal stability. These arguments are not persuasive.
The primary particles of Kim aggregate into secondary particles, see e.g., Fig. 2b. Since the claims are not limited to exclude secondary particles, the primary particle read on the claimed “single particle”. The particle morphology depicted in Fig. 2b shows the aggregation of primary particles forming the secondary particle. Specifically, the primary particles are needle shaped, having a length and width and an aspect ratio greater than 1 (e.g., elongated shape), thereby extending from the center of the secondary particle to the surface thereof. The core of the secondary particle is limited by formula 1, where the amount of cobalt (Coa) is zero, and includes Mg and Ti elements, see claim 9 of Kim; thus, Kim suggests the absence of Co in a first region of the primary particle, as well as Mg and Ti elements. Further, Kim suggests a concentration gradient layer is formed on the periphery of the core layer ([0027], Fig. 1). Provided the primary particles each extend as a needle shape from the center of the core to the surface of the secondary particle (Fig.2b), each of the primary particles includes a concentration gradient at the outer portion of each primary particle (i.e., second region) to achieve the concentration gradient layer on the core layer of the secondary particle (Fig.1). Kim suggests the second region (concentration gradient layer) follows formula 2, hence includes Mg and Ti, and has a concentration gradient due to a continuous change in concentration of one or more transition metals; examples ([0038-0047]) show Co increase from core to shell. The elements which are not suggested by Kim (i.e., Na, W) where addressed in view of secondary references as set forth in the rejection (e.g., Choi addressed the Na element, Choi II addressed the S element, Hirai (and Shin) addressed the inclusion of W in combination with Kim’s Mg and Ti elements). The fact that the secondary references might suggest a different reason to include the elements does not make the claimed composition(s) nonobvious. The reason or motivation to modify the reference may often suggest what the inventor has done, but for a different purpose or to solve a different problem. It is not necessary that the prior art suggest the combination to achieve the same advantage or result discovered by applicant. MPEP 2144 IV.
Claim Rejections - 35 USC § 103
The text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
Claim(s) 1, 3-4, 9-10, and 13 is/are rejected under 35 U.S.C. 103 as being unpatentable over Kim US 2016/0359165, in view of Choi et al. (US 2016/0211518), Choi (WO 2017204428), Hirai et al. (US 2016/0013486), and Shin et al. (US 20180287135), hereinafter Kim, Choi, Choi II, Hirai, and Shin (all of record).
Regarding Claims 1, 9, 10, and 13, Kim suggests a cathode active material (see e.g., claims 1, and 9, Fig. 1, and Examples) comprising a lithium transition metal oxide particle. The primary particles of Kim aggregate into secondary particles; the particle morphology depicted in Fig. 2b which shows the aggregation of primary particles forming the secondary particle. Specifically, the primary particles are needle shaped, having a length and width and an aspect ratio greater than 1 (e.g., elongated shape), such that each extends from the center of the secondary particle to the surface thereof. Each of these primary particles reads on the claimed “single particle”. Each of the primary particles includes a first region/inner portion (e.g., region of the core layer of the secondary particle) and a second region/outer portion (e.g., region of the concentration gradient layer of the secondar particle) to achieve the secondary particle comprising the core layer and concentration gradient layer on the core layer (Fig.1); the first region forms an inner portion of the lithium transition metal oxide particle, and the second region forms an outer portion of the lithium transition metal oxide particle (see Fig. 1, 2b). Kim suggests the first region of the primary particle (i.e., core layer portion of the secondary particle) comprises an element other than a Co element and does not contain cobalt (e.g., core layer follows Formula (1): LiNiCoMnMeO2X, thereby includes an element other than Co (i.e., Ni, Mn); further, a in Coa is zero, see e.g., [0027-0028] and claims 1, and 9), and the second region of the primary particle (e.g., concentration gradient layer of the secondary particle) comprises the Co element and a concentration gradient region in which a concentration of Co atoms changes (e.g., concentration gradient layer has a concentration gradient due to a continuous change in concentration of one or more transition metals; examples ([0038-0047]) show Co increase from core to shell); the concentration gradient region (i.e., concentration gradient layer) has a thickness of 500 nm or less (e.g., 10-500 nm, see e.g., claim 1).
Kim suggests the lithium transition metal oxide secondary particle has an average particle diameter (D50) in a range of about 10-11 µm, see e.g., Table 1); since each of the primary particles extend from the center of the secondary particle to the surface of the secondary particle (Fig.2), the particle diameter of each primary particle (hence, diameter each single particle) is equal to the radius of the secondary particle. In view of the foregoing, Kim suggests the single particle (primary particle) has an average particle diameter of about 5-5.5µm (i.e., radius = diameter/2, e.g., 10µm/2 = 5µm), which overlaps with that claimed (i.e., 5 µm to 20 µm).
Kim does not disclose part of Li is substituted with Na. However, Choi discloses a lithium transition metal oxide in which a part of the lithium is substituted by sodium. Specifically, Li1-aAa is suggested where A is sodium (Na) and 0.0025 ≤ a ≤ 0.02; improved structural stability and improved cycle characteristics are expected by partial substitution of lithium sites with Na. It would be obvious to one having ordinary skill in the art the lithium is substituted by small amounts of sodium since there is an expectation of improved structural stability.
Kim does not disclose sulfur substituted in the oxygen sites. However, Choi II discloses a lithium transition metal oxide (i.e., LixM1-m-zAmDzO2-tXt, where M is Ni, Co, Mn, etc., A is Mg, etc, D is Ti, etc., and X is S and t is between 0 and 0.2) and suggests sulfur in the oxygen sites strengthens the bond with the transition metal, thereby contributing to the improvement of cycling characteristics by suppressing transition metal elution, page 5/36. It would be obvious to one having ordinary skill in the art to include sulfur in the amount of greater than 0 and less than 0.01 with the expectation of strengthening the bond with the transition metals, thereby improving cycling characteristics by suppressing transition metal elution, as suggested by Choi II.
Kim suggests the first region of the primary particle (i.e., core region portion of the secondary particles) excludes Co (i.e., Coa in Formula (1) is 0≤a≤0.10, thereby suggesting Co is excluded, see e.g., claim 9) and includes one or more of Mg and Ti (see e.g., Mec in Formula (1) is between 0-0.2). Kim does not disclose the element W in the first region of the lithium metal oxide formula. However, Hirai suggests replacing the transition metals (i.e., Ni, Mn, etc.) with Ti, W, and Mg (i.e., Mx in General Formula (1) includes Ti, W, and Mg, 0 ≤ x ≤ 0.3); using Ti, W, and Mg is desirable from the viewpoint to the cycle characteristics because the elements stabilize the crystal structure so that a decrease in capacity is prevented with repeated charge/discharge, thereby achieving excellent cycle characteristics, [0028-0029]. It would be obvious to one having ordinary skill in the art to include, W, along with Ti and Mg, in the first region of Kim with the expectation of preventing a decrease in capacity with repeated cycling, thereby achieving excellent cycle characteristics, as suggested by Hirai. Kim was modified with Hirai to suggest Ti, W, and Mg; the amount thereof is more than 0 to 0.3 from the standpoint of stabilizing crystal structure to prevent capacity decreases, thereby achieving excellent cycle characteristics, [0028-0029]. Further, Shin suggests the value of W is between 0.002 to 0.03 from the standpoint of output characteristics and obtaining significant battery characteristics, [0045-0046], while Ti and Mg substituted for Ni, and Mn are kept from 0 to 0.2 because they do not degrade characteristics of the active material, [0052-0053]. It would be obvious to one having ordinary skill in the art for Kim to select the claimed values of Ti (above 0 to 0.005, or above 0 to 0.003), W (above 0 to 0.005), and Mg (above 0 to 0.005, or above 0 to 0.003) to stabilize the crystal structure, thereby achieving excellent battery characteristics, without degrading the active material characteristics, as suggested by Hirai and Shin.
The values of Na, S, Mg, Ti and W suggested in the prior art overlap with those claimed or are close. In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. Similarly, a prima facie case of obviousness exists where the claimed ranges or amounts do not overlap with the prior art but are merely close. See MPEP 2144.05, I., and MPEP 2144.05, II.
Routine Optimization: Generally, differences in concentration or temperature will not support the patentability of subject matter encompassed by the prior art unless there is evidence indicating such concentration or temperature is critical. "[W]here the general conditions of a claim are disclosed in the prior art, it is not inventive to discover the optimum or workable ranges by routine experimentation." In re Aller, 220 F.2d 454, 456, 105 USPQ 233, 235 (CCPA 1955); "The normal desire of scientists or artisans to improve upon what is already generally known provides the motivation to determine where in a disclosed set of percentage ranges is the optimum combination of percentages", Peterson, 315 F.3d at 1330, 65 USPQ2d at 1382.
Regarding Claim 3, Kim suggests the concentration of cobalt atoms in the concentration gradient region increases toward the outside, see e.g., Example 1 has Co increasing from about 0 to 0.2, see also the other examples in [0043-0047].
Regarding Claim 4, Kim suggests the concentration gradient region includes Ni atoms which decrease toward the outside, see e.g., Example 1 where Ni decreases from 0.97 to 0.6, see also the other examples in [0043-0047].
Claim(s) 1, 3-4, 9-10, and 12-13 is/are rejected under 35 U.S.C. 103 as being unpatentable over Kim, Choi, Choi II, Hirai, and Shin, in view of Gan (WO 2020043140), hereinafter Gan.
Regarding Claims 1, 3-4, 9-10, and 12-13, in contrast to the rejection of claims 1, 3-4, 9-10, and 13 over Kim, Choi, Choi II, Hirai, and Shin, this rejection interprets the whole secondary particle as the lithium transition metal oxide particle; the core portion of the secondary particle is interpreted as the first region/inner portion and the concentration gradient layer of the secondary particle is interpreted as the second region/outer portion. The remaining limitations of claims 1, 3-4, 9-10, and 13 are treated the same as set forth under the rejection of claims 1, 3-4, 9-10, and 13 over Kim, Choi, Choi II, Hirai, and Shin (thus not repeated here for brevity),
Kim’s disclosure of a secondary particle formed from the aggregation of primary particles (e.g., Fig. 2) does not suggest the lithium transition metal oxide particle is a single particle or a single crystal. However, Gan suggests a single crystal particle structure having an average particle diameter between 2-15 microns is advantageous because without the gaps between primary particles thermal stability is higher and the phase transition (oxygen evolution) in the high lithium delithiation state of the cathode materials is suppressed. Additionally, the single crystal particle structure has good crystallinity, smooth crystal surface, few lattice defects, high lithium ion conductivity, and improved rate performance. See e.g., [0027-0030]. It would be obvious to one having ordinary skill in the art the lithium transition metal oxide particle of Kim is a single particle and single crystal without the gaps between primary particles (as shown by Kim) because one of ordinary skill in the art would expect higher thermal stability, and the suppression of phase transition (oxygen evolution) in the high lithium delithiation state of the cathode; additionally, the single crystal particle structure offers good crystallinity, a smooth crystal surface, few lattice defects, and improved rate performance, as suggested by Gan.
Claim(s) 12 is/are rejected under 35 U.S.C. 103 as being unpatentable over Kim, Choi, Choi II, Hirai, and Shin, in view of Celasun et al. (US 2021/0119204, of record), hereinafter Celasun.
Regarding Claim 12, Kim does not disclose whether the lithium transition metal oxide is a single crystal. However, Celasun suggests a lithium transition metal oxide powder comprising a single monolithic particle, see e.g., EEX1.1-FE in Figs. 2-3 and 6.2, claim 18 [0100-0101]; the single crystal monolithic particle can endure volume changes better than polycrystalline particles, as evidenced from the lack of micro-cracks, thereby resulting in improved cycling stability, [0101]. It would be obvious to one having ordinary skill in the art the primary lithium transition metal oxide particles of Kim are a single crystal with the expectation of improved cycling stability from being able to endure volume changes without microcracking, as suggested by Celasun.
Claim(s) 14-15 is/are rejected under 35 U.S.C. 103 as being unpatentable over Kim, Choi, Choi II, Hirai, and Shin in view of Hiroka et al. (JP2015118898, of record), hereinafter Hiroka.
Regarding Claim 14, Kim suggests the second region of the primary particle (i.e., concentration gradient layer, Formula (2)) includes an element other than Co, W, Mg, and Ti (e.g., Ni, Mn) in an amount of greater than 0 and less than 1 (e.g., Ni is present based on the amount of the other elements, e.g., 0.97 to 0.6 in Example 1, 0.9 to 0.3 in Example 6, etc), Co in an amount greater than 0 and less than 1 (e.g., Coa varies from about 0 to 0.2 in Example 1, see also claim 9, and [0027-0029, 0042-0044], and rejection of claim 1), and at least one element selected from W, Mg, and Ti (e.g., Mec is Mg, Ti and present in an amount from 0 to 0.2, see [0027-0029]).
Kim does not disclose sulfur substituted in the oxygen sites. However, Choi II discloses a lithium transition metal oxide (i.e., LixM1-m-zAmDzO2-tXt, where M is Ni, Co, Mn, etc., A is Mg, etc, D is Ti, etc., and X is S and t is between 0 and 0.2) and suggests sulfur in the oxygen sites strengthens the bond with the transition metal, thereby contributing to the improvement of cycling characteristics by suppressing transition metal elution, page 5/36. It would be obvious to one having ordinary skill in the art to include sulfur in the amount of greater than 0 and less than 0.01 with the expectation of strengthening the bond with the transition metals, thereby improving cycling characteristics by suppressing transition metal elution, as suggested by Choi II.
Kim does not suggest the inclusion of sodium for lithium. However, Hiroka suggests the inclusion Na for Li sites where the amount of Na is between 0.001 and 0.03 from the standpoint of promoting grain growth without deteriorating capacity and cycle life, and has the effect of suppressing structural collapse, [0029]. It would be obvious to one having ordinary skill in the art to include Na in lithium sites were the amount of Na is above 0 to 0.01 to promote grain growth without deteriorating capacity and cycle life, and to suppress structural collapse.
Regarding Claim 15, the broader disclosure of Kim suggests the inclusion of Mec (e.g., Mg, Ti, etc., see e.g., claim 9), where the ratio of Coa/(Coa+Ni1-a-b-c+Mnb+Mec) is greater than 0 and less than or equal to 0.2 (e.g., amount of Coa = 0.2 in example 2).
Claim(s) 14-15 is/are rejected under 35 U.S.C. 103 as being unpatentable over Kim, Choi, Choi II, Hirai, Shin, and Gan in view of Hiroka et al. (JP2015118898, of record), hereinafter Hiroka.
Regarding Claims 14-15, the features of claims 14-15 have already been addressed under the rejection of claims 14-15 over Kim, Choi, Choi II, Hirai, Shin, and Hiroka. The rejection of Claims 14-15 over Choi II, Hirai, Shin, Gan in view of Hiroka are applied in the same way, hence not repeated for brevity.
Conclusion
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/ANNA KOROVINA/Examiner, Art Unit 1729
/ULA C RUDDOCK/Supervisory Patent Examiner, Art Unit 1729
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