DETAILED ACTION
Introductory Notes
Any paragraph citation of the instant is in reference to the U.S. published patent application.
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and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114.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 3/30/2026 has been entered.
Claim Objections
Claim 7 is objected to because of the following informalities: cobalt (Co) is incorrectly capitalized and written as “CO” in claim 7. Notably the initially filed claims of 7/12/2022 as well as all previous claim sets and the specification [0019] make it clear Co is intended as opposed to Carbon and Oxygen. Appropriate correction is required.
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.
Claims 1, 3-4, 6-10 and 23 are rejected under 35 U.S.C. 103 as being unpatentable over TAKAMORI (JP 6600734 B1 with US 20220029158 A1 used as an English translation for citations, both supplied with the IDS of 7/12/2022) in view of KAWASATO (US 20150380737 A1).
Regarding claim 1, TAKAMORI discloses a positive electrode active material for an all-solid-state lithium-ion battery (“solid electrolyte” [0188] as well as “lithium secondary battery” per claim 16) composed of particles containing crystals of a lithium metal composite oxide (claim 1),
wherein the positive electrode active material for an all-solid-state lithium-ion battery is in contact with a solid electrolyte layer (“in those cases where a solid electrolyte is used, the solid electrolyte can sometimes also function as a separator,” [0189]) ,
wherein the particles have a hexagonal layered crystal structure belonging to the space group R-3m (“preferable that the crystal structure is a hexagonal crystal structure belonging to the space group R-3m” [0086]) and contain at least Li and a transition metal (claim 1),
wherein the BET specific surface area is 0.2 m2/g or more and 2.0 m2/g or less (“BET specific surface area that is less than 2 m2/g, preferably at least 0.2 m2/g” [0050]),
wherein the particles are composed of primary particles, secondary particles which are aggregates of the primary particles, and single particles that exist independently of the primary particles and the secondary particles (“composed of secondary particles that are aggregates of primary particles, and single particles that exist independently from the secondary particles” [0025]),
wherein the primary particles are particles having no grain boundaries in an appearance observed using a scanning electron microscope in a field of view of 20,000x, and having a particle diameter of less than 0.5 µm (“20,000× using a scanning electron microscope … an average particle size of less than 0.5 μm” [0021]),
wherein the secondary particles are particles having grain boundaries in the appearance (“the term “secondary particle” means a particle composed of aggregated primary particles” [0022] and as such have grain boundaries, which is in contrast to TAKAMORI’s definition of primary and single particles having no grain boundaries per [0021] and [0023] respectively),
wherein the single particles are particles having no grain boundaries in the appearance (“no grain boundaries exist in the external appearance” [0023]), and having a particle diameter of 0.5 µm or more (“an average particle size of at least 0.5 μm” [0023]),
wherein an amount of the single particles in the particles is 20% or more (“the abundance ratio of single particles: secondary particles is preferably within a range from 1/99 to 60/40” [0072] and that this represents the mass ratio per [0072] wherein the count ratio would be even higher due to lower mass of single particles compared to secondary particles; along with TAKAMORI’s use of “Circularity Distribution” [0052] to determine “the number of particles along the vertical axis” [0054] where the results reported in Table 2 for Examples 1-3 each lead to the single particles being approximately 40% to 45% of the particles, with illustrative math for Example 1 being 0.61/(0.61+0.84) = 42%).
Regarding the “wherein the amount of the single particles in the particles is determined by counting the single particles and the secondary particles in the field of view of 20,000x, and calculating a number percentage of the single particles by N1/(N1+N2) (%), in which N1 is the number of the single particles and N2 is the number of the secondary particles”:
TAKAMORI discloses the use of 20,000x field of view in [0021] and [0023].
TAKAMORI discloses the preferrable mass ratio in [0072].
TAKAMORI discloses examples of circularity distribution in Table 2 which lead N1/(N1+N2) values.
Regarding the claimed method of counting, this is being given limited patentable weight as it is a description of measurement protocol and lacks a patentable distinction from other measurement methods such as laser diffraction or TAKAMORI’s circularity distribution. Each method of counting may arrive at a percent of single particles reading on the claimed range.
As discussed above, TAKAMORI discloses the same single to secondary particle relationship as the instant and further discloses the same formula for the NCM active material (see claim 1 of TAKAMORI and claim 7 of the instant). Furthermore, TAKAMORI describes the example preparation steps mirroring those of the instant (see TAKAMORI [0224-227] and instant [0442-0449]). However, TAKAMORI is silent regarding x-ray diffraction measurements of the NCM active material. Given the overlap in particles, formula, and preparation the x-ray diffraction can be expected to read on the wide ranges claimed, as shown by KAWASATO.
KAWASATO like TAKAMORI discloses a lithium-ion battery with a solid electrolyte [0114]; as well as a formula for the lithium composite oxide like TAKAMORI (see claim 2 of KAWASOTA in comparison to claim 1 of TAKAMORI); as well as the same crystal structure of TAKAMORI ([0023]); as well as similar surface areas (Table 3 wherein each sample is between 0.2 and 2 m2/g as disclosed by TAKAMORI). As shown in Table 3 of KAWASOTA, the ratio of L003/L110 is in all cases well within the range of 0.65 to 3, which notably allows for L003 to be three times L110 as well as the opposite of L110 being three times L003.
KAWASATO discloses “(003) crystallite size in the XRD pattern of the present composite oxide is preferably from 700 to 1,200 Å” [0045] and “(110) crystallite size in the XRD pattern of the present composite oxide is preferably from 400 to 760 Å” [0046]. Notably comparing minimums and maximums gives a range of 003/110 of 0.9 to 3. KAWASATO teaches when the (110) crystallite size is in the proper range “the capacity can be increased since there is a sufficient amount of Li which contributes to charge and discharge, and the cycle durability can be improved since the amount of elution of the transition metals can be reduced. Further, when the crystallite size is at most 760 Å, the diffusion distance of Li in the crystal structure tends to be short, whereby excellent rate retention will be achieved” [0046]. KAWASATO teaches when the (003) crystallite size is in the proper range “the aspect ratio of the crystallite size in the c-axis direction to in the a-axis direction can be increased. As a result, the amount of lithium ions present between layers can be increased, whereby a high capacity will be achieved, the proportion of (110) exposed to the particle surface can be reduced, the amount of elution of the transition metals can be reduced, and the cycle durability can be improved. Further, when the crystallite size is at most 1,200 Å, the volume expansion and contraction in the c-axis direction at the time of charge and discharge can be made small” [0047]. As such, KAWASATO teaches the ranges and ratios of 003 and 110 that are preferential for high capacity and cycle durability.
Before the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art that the desirable ranges and ratios of x-ray diffraction measurements for TAKAMORI’s active material would be expected to be within the teachings of KAWASATO because measured values within these ranges would indicate increased capacity and cycle durability.
Therefore, modified TAKAMORI discloses in powder x-ray diffraction measurement using CuKa rays, the crystallite size L003 of a diffraction peak in a range of 2θ=18.7±10 is 1,300 Å or less (overlap in particles, formula, and preparation of TAKAMORI as well as KAWASATO “the (003) crystallite size in an XRD pattern is from 700 to 1,200 Å” [0015]),
wherein, in the particles, in the powder x-ray diffraction measurement, a ratio L003/L110 of L003 to a crystallite size L110 of a diffraction peak in a range of 2θ=64.5±1 is 0.65 or more and 3.00 or less (overlap in particles, formula, and preparation of TAKAMORI with the instant as well as Table 3 of KAWASATO and the previously referenced paragraphs [0045-0046] of KAWASATO which give ranges for 003 and 110 and therefore ratios; furthermore the instant lacks a comparative example outside the claimed range wherein the particle distribution, formula, and structure reads on the claim; notably the lone comparative example outside the range is comparative example 3 which is LiCoO2, not prepared in the same manner per [0496] and only has single particles per [0497], and has a L003/L110 of 0.62 just outside the claimed range; furthermore the remaining examples of the instant, including comparative examples, were all within 0.9 to 1.27 for L003/L110; and the claimed range broadly includes both L003 being three times L110 and the reverse of L110 being three times L003).
Regarding claim 3, modified TAKAMORI discloses all the claim limitations as set forth above and TAKAMORI further discloses a sum of mass fractions of K atoms, Fe atoms, Cr atoms, Cu atoms, Ca atoms, Mg atoms, and Na atoms with respect to a total mass of the positive electrode active material for an all-solid-state lithium-ion battery is 0.03% or more and 1.0% or less (formula of claim 1 including “M is at least one element selected from the group consisting of Fe, Cu, … Mg” as well the amount of M, which is given as w, as being “preferably that 0.001≤w≤0.07” [0042] along with Example 1 where the amount of M is 1% per [0225]). Furthermore, TAKAMORI teaches proper selection of M and w yields “high cycle characteristics” [0045] as well as “low battery internal resistance” [0041]. Given the overlapping ranges and an example within the claimed range, it would have been obvious to one of ordinary skill in the art to select an element reading on the claim from the finite list provided by TAKAMORI as well as an amount for the element within the claimed range for the benefit of high cycle characteristics and low battery internal resistance.
Regarding claim 4, modified TAKAMORI discloses all the claim limitations as set forth above and KAWASATO further discloses in the particles, in the powder x-ray diffraction measurement, a ratio L003/L104 of L003 to a crystallite size L104 of a diffraction peak in a range of 2Ɵ=44.6±1° is 0.70 or more and 3.00 or less (Table 2 of KAWASATO for examples as well KAWASATO disclosing “(I003/I104) of the (003) peak to the (104) peak in an XRD pattern is from 1.21 to 1.39” [0014] and that “I003/I104 is an index how the cation mixing of the lithium-containing composite oxide is suppressed” [0030]; furthermore the overlap in particles, formula, and preparation between TAKAMORI and the instant with the expected similarity in measurements, especially given the breadth of the claimed range, is again noted).
Regarding claim 6, modified TAKAMORI discloses all the claim limitations as set forth above and TAKAMORI further discloses the transition metal is at least one element selected from the group consisting of Ni, Co, Mn, Ti, V and W (claim 1, formula 1: Li[Lix(Ni(1-y-z-w)CoyMnzMw)1-x]O2).
Regarding claims 7-9 and 23, which state:
Claim 7: Composition Formula (A): Li[Lix(Ni(1-y-z-w)CoyMnzMW)1-x]02 (where, M is at least one element selected from the group consisting of Ti, Al, W, B, Mo, Nb, Zn, Sn, Zr, Ga and V,
and -0.10≤x≤0.30, 0≤y≤0.40, 0≤z≤0.40, and 0≤w≤0.10 are satisfied).
Claim 8: y>0 and z+w>0 are satisfied.
Claims 9 and 23: 1-y-z-w≥0.50 and y≤0.30 are satisfied.
Modified TAKAMORI discloses all the claim limitations as set forth above and TAKAMORI further discloses claim 1 which reads on the limitations:
Li[Lix(Ni(1-y-z-w)CoyMnzMw)1-x]O2 (1)
(wherein M is at least one element selected from the group consisting of Fe, Cu, Ti, Mg, Al, W, B, Mo, Nb, Zn, Sn, Zr, Ga and V, −0.1≤x≤0.2, 0<y≤0.4, 0≤z≤0.4 and 0≤w≤0.1)
Furthermore, TAKAMORI discloses “y in the above compositional formula (1) preferably exceeds 0 … preferably 0.33 or less” [0035], “z in the above compositional formula (1) is preferably at least 0.01 … preferably 0.35 or less” [0039], and “w in the above compositional formula (1) preferably exceeds 0 … preferably 0.07 or less” [0041].
Regarding claim 10, modified TAKAMORI discloses all the claim limitations as set forth above and TAKAMORI further discloses the amount of the single particles in the particles is 90% or more (Comparative Example 4 with Active Material A3 [0252] where A3 contains “mainly single particles” [0242], in other words nearly 100% single particles by count. Notably preferred embodiments, such as the 60/40 ratio by mass of TAKAMORI paragraph [0072] do not constitute a teaching away from a broader disclosure or nonpreferred embodiments, see MPEP 2123(II)).
Response to Arguments
Regarding art-based rejections, applicant’s arguments with respect to the claims have been considered but are not persuasive.
Applicant concedes Takamori teaches the “primary particles, secondary particles, and single particles” (remarks, bottom of page 8) and then at the top of page 9 applicant states “Takamori teaches that, during electrode formation, mechanical interaction between particles causes fracturing of secondary particles” and that “the present application is directed to a structure that suppresses particle cracking”.
Examiner disagrees with the comparison being made. The fracturing referenced in Takamori is when “pressed and affixed to the collector” [0087], i.e. during manufacture. The benefit of the Takamori’s particle structure is “the single particles 57 move into the spaces between the broken secondary particles 56A, thereby increasing the contact surface area between the secondary particles (symbols 56A and 56) and the single particles 57, and reducing voids. It is thought that this improves the density of the electrode” [0087].
In contrast the suppression of particle cracking in the instant is during “charging” [0142], not during manufacture. Takamori does not teach cracking or decreased performance during charging, instead Takamori teaches that when “the battery is subjected repeated charging and discharging, depletion of the electrolyte solution and the like is less likely to occur … the present embodiment containing secondary particles and single particles exhibits improved volumetric capacity and volumetric capacity retention” [0088]. Notably the single and secondary particles as well as the reduction in voids taught by Takamori yields the same BET specific surface area 0.2 to 2.0 m2/g as that of the instant (instant [0103] and Takamori [0050]).
Regarding L003/L110, at the bottom of page 10 applicant states that the “cited references do not identify this parameter as a variable affecting performance, nor do they provide any teaching or motivation to control it within the claimed range”. As discussed in the rejection of claim 1 it is the examiner’s position that the prior art (now TAKAMORI in view of KAWASATO) disclose the claimed ratio beyond a preponderance of the evidence. This is due to the overlap in single and secondary particles, formula, and preparation of Takamori with the instant; and further due to the ranges provided in Kawasato which are well within the claimed range that includes both L003 being three times L110 and the reverse of L110 being three times L003. Furthermore, the instant lacks a comparative example outside the claimed range wherein the particle distribution, formula, and structure reads on the claim. Notably the lone comparative example outside the range is comparative example 3 which is LiCoO2 which is not prepared in the same manner per [0496], only has single particles per [0497], and has a L003/L110 of 0.62 just outside the claimed range. The remaining examples of the instant, including comparative examples, were all within 0.9 to 1.27 for L003/L110 per Table 1. These comparative examples do not lend credence to L003/L110 being between 3:1 and 1:3 as being a critical range.
Conclusion
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/T.L.M./Examiner, Art Unit 1721
/ALLISON BOURKE/Supervisory Patent Examiner, Art Unit 1721
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