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 Claims
This is a final office action for application 17/792,351 in response to the amendment(s) filed on 06/04/2026. Claims 21, 23-27, 29-38 and 43-46 are under examination. Claim 37 remains withdrawn from consideration.
Response to Arguments
Applicant’s arguments filed on 06/04/2026 have been fully considered but were not found persuasive for the reasons set forth below. See claims 21, 23-27, 29-36, 38 and 43-46 rejections below.
Applicant’s argument that Example 17 of Iwasaki does not disclose the amended particle size limitations is acknowledged. Nevertheless, the amended limitations do not overcome the prior art. Iwasaki discloses that its active material particles may comprise layered lithium nickel cobalt manganese composite oxides and generally discloses applicable D10, D50, and D90 ranges (see e.g. paragraphs [0060] – [0064] of Iwasaki). Furthermore, Example 22 discloses D10 = 5 µm, D50 = 10 µm, D90 = 30 µm, and a particle-size range of 3–40 µm, thereby providing D90/D10 = 6.0 and Dmax = 40 µm (see e.g. Example 22 in Table 2 of Iwasaki). Takahashi further teaches combining smaller single or substantially single particles with larger secondary particles to improve particle filling, electrode density, energy density, and cycle characteristics (see e.g. paragraphs [0010] and [0023]-[0026] of Takahashi). Therefore, it would have been obvious to a person of ordinary skill in the art to modify the layered lithium metal composite oxide of Iwasaki with the known particle size distribution and mixed particle morphology of Takahashi in order to obtain the improved filling and battery performance suggested by Takahashi.
Furthermore, Applicant’s discussion of paragraph [0110] of the instant specification does not demonstrate criticality of the amended boundaries. The specification does not provide controlled comparisons between otherwise identical materials immediately below and above the respective lower limits of D90/D10 = 6.0, D50 = 4.5 µm, and Dmax = 21.0 µm. Rather, the asserted particle filling effect is consistent with the teaching of Takahashi that mixtures of smaller and larger active material particles improve filling of the positive electrode layer. Accordingly, the amended numerical ranges represent no more than selection or optimization within the particle size distributions taught by the cited art.
In conclusion, the arguments and amendments filed were not found to be persuasive over the previous prior art rejection of record. The rejections of the claims have been updated to reflect the amendments where appropriate. See claims updated claims 21, 23-27, 29-36, 38 and 43-46 rejections below.
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 Rejections - 35 USC § 103
Claims 21, 23-27, 29-33, 35-36, 38 and 44 are rejected under 35 U.S.C. 103 as being unpatentable over Iwasaki et al. (US-20180083269-A1) and further in view of Takahashi et al. (US-20220285678-A1).
Regarding Claim 21, Iwasaki discloses a positive electrode active material for an all-solid-state lithium-ion battery (see e.g. “positive electrode active material” in paragraph [0023] and part number 5b in FIG. 4) composed of particles containing crystals of a lithium metal composite oxide (see e.g. “lithium nickel cobalt manganese composite oxide” in paragraph [0062] and “LiNi0.5Co0.2Mn0.3O2” in Example 17 of Table 2),
wherein the positive electrode active material for an all-solid-state lithium-ion battery is in contact with a solid electrolyte layer (see e.g. “the insulator particles may include solid electrolyte particles” in paragraph [0071] and “a solid electrolyte layer may be provided between, for example, the positive electrode active material-containing layer and negative electrode active material-containing layer” in paragraph [0180]),
wherein the lithium metal composite oxide has a layered structure and contains at least Li and a transition metal (see e.g. “LiNi0.5Co0.2Mn0.3O2” in Example 17 of Table 2; LiNi0.5Co0.2Mn0.3O2 is a layered lithium metal composite oxide containing Li, Ni, Co, and Mn).
Iwasaki further discloses that the active material particles may have a particle size within a range of 0.5 µm to 200 µm, a D50 of 1 µm to 10 µm, a D10 of 0.6 µm to 7 µm, and a D90 of 3 µm to 100 µm (see e.g. paragraph [0064] of Iwasaki).
Iwasaki discloses ranges that overlap with the ranges claimed by the instant application. In the case where the prior art discloses a range that overlaps with the claimed range, a prima facie case of obviousness exists. See MPEP 2144.05 (I).
Iwasaki additionally discloses a positive electrode active material satisfying all of the following: 6.0 ≤ D90/D10 (see e.g. Example 22 in Table 2; D90 is 30 µm and D10 is 5 µm, such that D90/D10 = 6.0), 4.5 µm ≤ D50 ≤ 15.0 µm (see e.g. Example 22 in Table 2; D50 is 10 µm), and 21.0 µm ≤ Dmax ≤ 40.0 µm (see e.g. Example 22 in Table 2; the particle size range is 3 µm to 40 µm, such that Dmax is 40 µm).
Iwasaki therefore discloses a positive electrode active material having a particle size distribution that falls within each of the amended ranges. Although Example 22 uses LiMn2O4, Iwasaki expressly identifies lithium manganese composite oxides and layered lithium nickel cobalt manganese composite oxides as alternative positive electrode active materials and generally applies its particle size teachings to the active material particles (see e.g. paragraphs [0059]-[0064] of Iwasaki).
Iwasaki does not explicitly disclose in the same embodiment a layered lithium nickel cobalt manganese composite oxide having the particle size distribution of Example 22 and particles 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, wherein the primary particles have no grain boundaries and have a particle diameter of less than 0.5 µm, wherein the secondary particles have grain boundaries, wherein the single particles have no grain boundaries and have a particle diameter of 0.5 µm or more, and wherein an amount of the single particles is 20% or more.
Takahashi, however, in the same field of endeavor, positive electrode active materials for lithium secondary batteries, discloses a lithium transition metal composite oxide positive electrode active material containing a mixture of lithium transition metal composite oxides (A) and (B) having different particle sizes and particle morphologies (see e.g. paragraphs [0006], [0023], and [0051] of Takahashi).
Takahashi discloses that the particles are composed of primary particles (see e.g. “primary particles” in paragraph [0025] of Takahashi), secondary particles which are aggregates of the primary particles (see e.g. “a secondary particle formed by aggregation of primary particles” in paragraph [0025] of Takahashi), and single particles that exist independently of the primary particles and the secondary particles (see e.g. “being composed of substantially single particles” in paragraph [0025] of Takahashi),
wherein the primary particles have no internal grain boundaries and have a particle diameter of less than 0.5 µm (see e.g. “primary particles having a small average particle diameter of, for example, 0.3 µm or smaller” in paragraph [0025] and an average primary particle diameter of 0.13 µm in paragraph [0072] of Takahashi),
wherein the secondary particles have grain boundaries in appearance (see e.g. “a particle boundary of the primary particles is observed on the particle cross section observed with a SEM” in paragraph [0026] of Takahashi),
wherein the single particles have no grain boundaries in appearance (see e.g. “particles in which no particle boundary of the primary particles is observed by using a scanning electron microscope (SEM)” in paragraph [0025] of Takahashi) and have a particle diameter of 0.5 µm or more (see e.g. “primary particles having a large average particle diameter of 0.5 µm or larger or being composed of substantially single particles” in paragraph [0025] of Takahashi),
and wherein an amount of the single particles is 20% or more (see e.g. “approximately 95% or more of all the particles had a single particle structure” in paragraph [0063] and the composite oxide (A) being present in an amount of 50 mass% of the positive electrode active material in paragraph [0073] of Takahashi). Takahashi further teaches that the amount of composite oxide (A) containing the single particles may be adjusted within a range of 5 mass% to 65 mass% of the positive electrode active material (see e.g. paragraph [0051] of Takahashi).
Takahashi also teaches that combining the smaller single or substantially single particles of composite oxide (A) with the larger secondary particles of composite oxide (B) allows the positive electrode mixture layer to be efficiently filled, relaxes pressure during rolling and stress during charging and discharging, inhibits particle cracking, increases the density of the positive electrode mixture layer, and provides high energy density and excellent charge discharge cycle characteristics (see e.g. paragraphs [0010] and [0052] of Takahashi). Therefore, it would have been obvious to a person of ordinary skill in the art, before the effective filing date of the claimed invention, to modify the layered lithium nickel cobalt manganese composite oxide positive electrode active material of Iwasaki et al. such that it has the particle size distribution demonstrated in Example 22 of Iwasaki and is composed of the mixture of primary particles, secondary particles, and single particles taught by Takahashi et al., including an amount of single particles of 20% or more, in order to improve particle filling, increase the density of the positive electrode active material layer, inhibit particle cracking, and obtain high energy density and excellent charge discharge cycle characteristics as suggested by Takahashi.
Iwasaki in view of Takahashi discloses a layered lithium metal composite oxide positive electrode active material having primary particles, secondary particles, and single particles and having particle size parameters falling within the claimed ranges of D90/D10, D50, and Dmax. The claimed methods of measurement, including determining particle diameters from a volume based cumulative particle diameter distribution curve using laser diffraction, observing particle morphology using SEM at 20,000× magnification, and calculating the number percentage of single particles as N1/(N1+N2), merely provide particular methods of quantifying the particle size distribution and particle morphology taught by the prior art. Takahashi determines particle size and particle size distribution on a volumetric basis using a laser diffraction type particle size distribution measuring device and observes particle morphology using SEM (see e.g. paragraphs [0024]-[0026] of Takahashi). It would have been routine for a person of ordinary skill in the art to use an appropriate SEM magnification and count the disclosed single and secondary particles to verify their respective proportions. Accordingly, the recited measurement procedures do not distinguish the claimed positive electrode active material from the particle distribution and morphology taught by Iwasaki in view of Takahashi.
Regarding Claim 23, Regarding Claim 23, Iwasaki in view of Takahashi discloses the positive electrode active material for an all-solid-state lithium-ion battery according to claim 21 (see claim 21 rejection above).
Iwasaki further discloses that the positive electrode active material satisfies the following Formula (1)-1: 6.0 ≤ (D90/D10) ≤ 14.0 (see e.g. Example 22 in Table 2; D90 is 30 µm and D10 is 5 µm, such that D90/D10 = 6.0).
Iwasaki discloses a point that lies within the range claimed by the instant application. In the case where the prior art discloses a point within the claimed range, a prima facie case of obviousness exists. See MPEP 2144.05(I).
Regarding Claim 24, Iwasaki in view of Takahashi discloses the positive electrode active material for an all-solid-state lithium-ion battery according to claim 21 (see claim 21 rejection above).
Iwasaki further discloses that the positive electrode active material satisfies the following 8.0 ≤ Dmax/Dmin ≤ 40.0 µm in Formula (4), Dmin is the minimum particle diameter (µm) in the cumulative particle diameter distribution curve (see e.g. Example 22 in Table 1; Range of particle size is 3 - 40 µm, therefore Dmax = 40 µm and Dmin = 3 µm; Dmax/Dmin = 13.3).
Iwasaki discloses a point that lies within the range claimed by the instant application. In the case where the prior art discloses a point within the claimed range, a prima facie case of obviousness exists. See MPEP 2144.05 (I).
Regarding Claim 25, Iwasaki in view of Takahashi discloses the positive electrode active material for an all-solid-sate lithium-ion battery according to claim 21 (see claim 21 rejection above).
Iwasaki further discloses that the transition metal is one element selected from the group consisting of Ni, Co, Mn, Fe and V (see e.g. "Examples of the active material useful as a positive electrode active material include... LisMnO2 (0 ≤ s ≤ 1)...LisNiO2 (0 ≤ s ≤ 1)... LisCoO2 (0 ≤ s ≤ 1)... LisFePO4 (0 ≤ s ≤ 1)... LisV2O5 (0 ≤ s ≤ 1)" in paragraph [0060]).
Regarding Claim 26, Iwasaki in view of Takahashi discloses the positive electrode active material for an all-solid-sate lithium-ion battery according to claim 25 (see claim 25 rejection above).
Iwasaki further discloses that the lithium metal composite oxide is represented by LiNi0.5Co0.2Mn0.3O2 (see e.g. " LiNi0.5Co0.2Mn0.3O2 " in Example 17 of Table 1). This directly corresponds with the claimed species of the instant application, which claims that the lithium metal composite oxide is Li[Lix(Ni1-y-z-w)CoyMnzMw)1-x]O2 (A) (where, 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, and -0.10 ≤ x ≤ 0.30,0 ≤ y ≤ 0.40,0 ≤ z ≤ 0.40, 0 ≤ w ≤ 0.10, and 0 < y + z + w are satisfied). If x = 0, y = 0.2, z = 0.3 and w = 0 this simplifies to LiNi0.5Co0.2Mn0.3O2 which is the same species disclosed by the prior art.
Iwasaki discloses a point that lies within the range claimed by the instant application. In the case where the prior art discloses a point within the claimed range, a prima facie case of obviousness exists. See MPEP 2144.05 (I).
Regarding Claim 27, Iwasaki in view of Takahashi discloses the positive electrode active material for an all-solid-sate lithium-ion battery according to claim 26 (see claim 26 rejection above).
Iwasaki further discloses that the lithium metal composite oxide is represented by LiNi0.5Co0.2Mn0.3O2 (see e.g. " LiNi0.5Co0.2Mn0.3O2 " in Example 17 of Table 1). This directly corresponds with the claimed species of the instant application, which claims that the lithium metal composite oxide is Li[Lix(Ni1-y-z-w)CoyMnzMw)1-x]O2 (A) (where, 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, and -0.10 ≤ x ≤ 0.30,0 ≤ y ≤ 0.40,0 ≤ z ≤ 0.40, 0 ≤ w ≤ 0.10, and 0 < y + z + w are satisfied). If x = 0, y = 0.2, z = 0.3 and w = 0 this simplifies to LiNi0.5Co0.2Mn0.3O2 which is the same species disclosed by the prior art. In this case y ≤ 0.3 and 1 - y - z - w = 1 - 0.2 - 0.3 - 0 = 0.5.
Iwasaki discloses a point that lies within the range claimed by the instant application. In the case where the prior art discloses a point within the claimed range, a prima facie case of obviousness exists. See MPEP 2144.05 (I).
Regarding Claim 29, Iwasaki in view of Takahashi discloses an electrode (see e.g. "The nonaqueous electrolyte battery includes a positive electrode" in paragraph [0018]) comprising the positive electrode active material (see e.g. "the positive electrode of this aspect may include a current collector, and a positive electrode active material-containing layer provided on one or both surfaces of the current collector " in paragraph [0152] part number 5 in FIG. 4) for an all- solid-state lithium-ion battery according to claim 21 (see claim 21 rejection above).
Regarding Claim 30, Iwasaki in view of Takahashi discloses the electrode according to claim 29 (see claim 29 rejection above).
Iwasaki further discloses that the electrode further comprises a solid electrolyte (see e.g. "the insulator particles may include solid electrolyte particles" in paragraph [0071] and FIG.1; FIG. 1 is schematic of an electrode including the current collector, the positive active material, and the insulator particles (solid electrolyte particles).
Regarding Claim 31, Iwasaki in view of Takahashi discloses an all-solid-state lithium-ion battery (see e.g. "a nonaqueous electrolyte battery" in paragraph [0018] and FIG. 3) comprising a positive electrode (see e.g. "positive electrode" in paragraph [0018]), a negative electrode (see e.g. "a negative electrode" in paragraph [0018]), and a solid electrolyte layer (see e.g. "nonaqueous electrolyte" in paragraph [0137]) and interposed between the positive electrode and the negative electrode (see e.g. "The solid electrolyte particles as an example of the insulator particles, which may be included in the electrode according to the first embodiment as positive electrode and/or negative electrode, may constitute at least a part of the nonaqueous electrolyte... The nonaqueous electrolyte may be hold by the electrode group." in paragraph [0137] and "a solid electrolyte layer may be provided between, for example, the positive electrode active material-containing layer and negative electrode active material-containing layer." in paragraph [0180] and FIGs. 1, 4 and 5),
wherein the solid electrolyte layer contains a first solid electrolyte (see e.g. " The nonaqueous electrolyte battery of the present example may further include a liquid nonaqueous electrolyte other than solid electrolyte particles as a nonaqueous electrolyte." in paragraph [0137]),
wherein the positive electrode has a positive electrode active material layer in contact with the solid electrolyte layer and a current collector on which the positive electrode active material layer is laminated (see e.g. part numbers 1a, 11, and 12 in FIG. 1), and
wherein the positive electrode active material layer contains the positive electrode active material (see e.g. part number 11 in FIG.1) for an all-solid-state lithium-ion battery according to claim 21 (see claim 21 rejection above).
Regarding Claim 32, Iwasaki in view of Takahashi discloses the all-solid-state lithium-ion battery according to claim 31 (see claim 31 rejection above).
Iwasaki further discloses that the positive electrode active material layer contains the positive electrode active material for an all-solid-state lithium-ion battery (see e.g. part number 11 in FIG. 1) and a second solid electrolyte (see e.g. part number 12 in FIG.1 and "The solid electrolyte particles as an example of the insulator particles, which may be included in the electrode according to the first embodiment as positive electrode and/or negative electrode, may constitute at least a part of the nonaqueous electrolyte. The nonaqueous electrolyte battery of the present example may further include a liquid nonaqueous electrolyte other than solid electrolyte particles as a nonaqueous electrolyte." in paragraph [0137]).
Regarding Claim 33, Iwasaki in view of Takahashi discloses the all-solid-state lithium-ion battery according to claim 32 (see claim 32 rejection above).
Iwasaki further discloses that the first solid electrolyte and the second solid electrolyte are the same substance (see e.g. "the insulator particles may include solid electrolyte particles." in paragraph [0071];the first solid electrolyte is the solid electrolyte particles and the second solid electrolyte is the insulator particles).
Regarding Claim 35, Iwasaki in view of Takahashi discloses the all-solid-state lithium-ion battery according to claim 31 (see claim 31 rejection above).
Iwasaki further discloses that the first solid electrolyte is an oxide-based solid electrolyte (see e.g. "The inorganic solid particles having Li ion conductivity are preferably inorganic solid particles having a garnet structure... The inorganic solid particles having a garnet structure include... Li7La3Zr2O12" in paragraph [0073] and "Li7La3Zr2O12" Example 17 in Table 1; Li7La3Zr2O12 is an oxide-based solid electrolyte).
Regarding Claim 36, Iwasaki discloses a positive electrode that is in contact with a solid electrolyte layer (see e.g. “a solid electrolyte layer may be provided between, for example, the positive electrode active material-containing layer and negative electrode active material-containing layer” in paragraph [0180]),
wherein the positive electrode has a positive electrode active material layer in contact with the solid electrolyte layer (see e.g. “a solid electrolyte layer may be provided between, for example, the positive electrode active material-containing layer and negative electrode active material-containing layer” in paragraph [0180] and part number 5b in FIG. 4) and a current collector on which the positive electrode active material layer is laminated (see e.g. “a current collector, and a positive electrode active material-containing layer provided on one or both surfaces of the current collector” in paragraph [0152] and part numbers 5a and 5b in FIG. 4),
wherein the positive electrode active material layer contains a positive electrode active material composed of particles containing crystals of a lithium metal composite oxide (see e.g. “lithium nickel cobalt manganese composite oxide” in paragraph [0062] and “LiNi0.5Co0.2Mn0.3O2” in Example 17 of Table 2),
wherein the lithium metal composite oxide has a layered structure and contains at least Li and a transition metal (see e.g. “LiNi0.5Co0.2Mn0.3O2” in Example 17 of Table 2; LiNi0.5Co0.2Mn0.3O2is a layered lithium metal composite oxide containing Li, Ni, Co, and Mn).
Iwasaki further discloses that the active material particles may have a particle size within a range of 0.5 µm to 200 µm, a D50 of 1 µm to 10 µm, a D10 of 0.6 µm to 7 µm, and a D90 of 3 µm to 100 µm (see e.g. paragraph [0064] of Iwasaki).
Iwasaki discloses ranges that overlap with the ranges claimed by the instant application. In the case where the prior art discloses a range that overlaps with the claimed range, a prima facie case of obviousness exists. See MPEP 2144.05 (I).
Iwasaki additionally discloses a positive electrode active material satisfying all of the following: 6.0 ≤ D90/D10 (see e.g. Example 22 in Table 2; D90 is 30 µm and D10 is 5 µm, such that D90/D10 = 6.0), 4.5 µm ≤ D50 ≤ 15.0 µm (see e.g. Example 22 in Table 2; D50 is 10 µm), and 21.0 µm ≤ Dmax ≤ 40.0 µm (see e.g. Example 22 in Table 2; the particle size range is 3 µm to 40 µm, such that Dmax is 40 µm).
Iwasaki therefore discloses a positive electrode active material having a particle size distribution that falls within each of the amended ranges. Although Example 22 uses LiMn2O4, Iwasaki expressly identifies lithium manganese composite oxides and layered lithium nickel cobalt manganese composite oxides as alternative positive electrode active materials and generally applies its particle size teachings to the active material particles (see e.g. paragraphs [0059]-[0064] of Iwasaki).
Iwasaki does not explicitly disclose in the same embodiment a positive electrode containing a layered lithium nickel cobalt manganese composite oxide having the particle size distribution of Example 22 and particles 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, wherein the primary particles have no grain boundaries and have a particle diameter of less than 0.5 µm, wherein the secondary particles have grain boundaries, wherein the single particles have no grain boundaries and have a particle diameter of 0.5 µm or more, and wherein an amount of the single particles is 20% or more.
Takahashi, however, in the same field of endeavor, positive electrode active materials for lithium secondary batteries, discloses a lithium transition metal composite oxide positive electrode active material containing a mixture of lithium transition metal composite oxides (A) and (B) having different particle sizes and particle morphologies (see e.g. paragraphs [0006], [0023], and [0051] of Takahashi).
Takahashi discloses that the particles are composed of primary particles (see e.g. “primary particles” in paragraph [0025] of Takahashi), secondary particles which are aggregates of the primary particles (see e.g. “a secondary particle formed by aggregation of primary particles” in paragraph [0025] of Takahashi), and single particles that exist independently of the primary particles and the secondary particles (see e.g. “being composed of substantially single particles” in paragraph [0025] of Takahashi),
wherein the primary particles have no internal grain boundaries and have a particle diameter of less than 0.5 µm (see e.g. “primary particles having a small average particle diameter of, for example, 0.3 µm or smaller” in paragraph [0025] and an average primary particle diameter of 0.13 µm in paragraph [0072] of Takahashi),
wherein the secondary particles have grain boundaries in appearance (see e.g. “a particle boundary of the primary particles is observed on the particle cross section observed with a SEM” in paragraph [0026] of Takahashi),
wherein the single particles have no grain boundaries in appearance (see e.g. “particles in which no particle boundary of the primary particles is observed by using a scanning electron microscope (SEM)” in paragraph [0025] of Takahashi) and have a particle diameter of 0.5 µm or more (see e.g. “primary particles having a large average particle diameter of 0.5 µm or larger or being composed of substantially single particles” in paragraph [0025] of Takahashi),
and wherein an amount of the single particles is 20% or more (see e.g. “approximately 95% or more of all the particles had a single particle structure” in paragraph [0063] and the composite oxide (A) being present in an amount of 50 mass% of the positive electrode active material in paragraph [0073] of Takahashi). Takahashi further teaches that the amount of composite oxide (A) containing the single particles may be adjusted within a range of 5 mass% to 65 mass% of the positive electrode active material (see e.g. paragraph [0051] of Takahashi).
Takahashi also teaches that combining the smaller single or substantially single particles of composite oxide (A) with the larger secondary particles of composite oxide (B) allows the positive electrode mixture layer to be efficiently filled, relaxes pressure during rolling and stress during charging and discharging, inhibits particle cracking, increases the density of the positive electrode mixture layer, and provides high energy density and excellent charge discharge cycle characteristics (see e.g. paragraphs [0010] and [0052] of Takahashi). Therefore, it would have been obvious to a person of ordinary skill in the art, before the effective filing date of the claimed invention, to modify the positive electrode of Iwasaki et al. such that the layered lithium nickel cobalt manganese composite oxide positive electrode active material has the particle size distribution demonstrated in Example 22 of Iwasaki and is composed of the mixture of primary particles, secondary particles, and single particles taught by Takahashi et al., including an amount of single particles of 20% or more, in order to improve particle filling, increase the density of the positive electrode active material layer, inhibit particle cracking, and obtain high energy density and excellent charge discharge cycle characteristics as suggested by Takahashi.
Iwasaki in view of Takahashi discloses a positive electrode containing a layered lithium metal composite oxide positive electrode active material having primary particles, secondary particles, and single particles and having particle size parameters falling within the claimed ranges of D90/D10, D50, and Dmax. The claimed methods of measurement, including determining particle diameters from a volume based cumulative particle diameter distribution curve using laser diffraction, observing particle morphology using SEM at 20,000× magnification, and calculating the number percentage of single particles as N1/(N1+N2), merely provide particular methods of quantifying the particle size distribution and particle morphology taught by the prior art. Takahashi determines particle size and particle size distribution on a volumetric basis using a laser diffraction type particle size distribution measuring device and observes particle morphology using SEM (see e.g. paragraphs [0024]-[0026] of Takahashi). It would have been routine for a person of ordinary skill in the art to use an appropriate SEM magnification and count the disclosed single and secondary particles to verify their respective proportions. Accordingly, the recited measurement procedures do not distinguish the claimed positive electrode from the particle distribution and morphology taught by Iwasaki in view of Takahashi.
Regarding Claim 38, Iwasaki in view of Takahashi discloses the positive electrode active material for an all-solid-state lithium-ion battery according to claim 21 (see claim 21 rejection above).
Iwasaki further discloses that its active material particles may have a D10 within a range of 0.6 µm to 7 µm and a D90 within a range of 3 µm to 100 µm (see e.g. paragraph [0064] of Iwasaki). Iwasaki also expressly demonstrates positive electrode active material particle distributions having a D90/D10 ratio falling within the claimed range of 7.0 to 14.0 (see e.g. Examples 15, 18, 21, and 23 in Table 2; D90 is 80 µm and D10 is 7 µm, such that D90/D10 is approximately 11.43).
Although these examples do not expressly disclose the D90/D10 ratio of approximately 11.43 in combination with the Dmax limitation of claim 21, Iwasaki separately demonstrates a positive electrode active material having D50 = 10 µm, D90 = 30 µm, and Dmax = 40 µm in Example 22 and generally teaches a D10 range of 0.6 µm to 7 µm (see e.g. paragraph [0064] and Example 22 in Table 2 of Iwasaki).
Takahashi further teaches that the positive electrode active material may contain 5 mass% to 65 mass% of smaller composite oxide (A) particles and 35 mass% to 95 mass% of larger composite oxide (B) particles and that the relative amounts of the smaller and larger particles may be selected to improve particle filling and increase the density of the positive electrode mixture layer (see e.g. paragraphs [0051]-[0052] of Takahashi). The relative amounts and sizes of the smaller and larger particles affect the resulting D10 and D90 values and, consequently, the D90/D10 ratio of the positive electrode active material.
Therefore, it would have been obvious to a person of ordinary skill in the art, before the effective filing date of the claimed invention, to adjust the relative amounts and particle sizes of the smaller and larger positive electrode active material particles taught by Iwasaki et al. and Takahashi et al. such that the D90/D10 ratio is within the range of 7.0 to 14.0 while retaining the D50 and Dmax values recited in claim 21, in order to improve particle filling and increase the density of the positive electrode active material layer as suggested by Takahashi. Determining the optimum or workable D90/D10 ratio through routine experimentation would have been within the ordinary skill in the art because the prior art recognizes that the relative particle sizes and proportions affect particle filling and electrode density.
Applicant has not demonstrated that the lower limit of D90/D10 = 7.0 is critical or produces an unexpected result relative to the particle size distributions taught by Iwasaki and Takahashi. Accordingly, selection of a D90/D10 ratio within the claimed range would have amounted to no more than routine optimization of a result effective variable. See MPEP 2144.05(II).
Regarding Claim 44, Iwasaki in view of Takahashi discloses the all-solid-state lithium-ion battery according to claim 32 (see claim 32 rejection above).
Iwasaki further discloses that the first solid electrolyte is an oxide-based solid electrolyte (see e.g. "The inorganic solid particles having Li ion conductivity are preferably inorganic solid particles having a garnet structure... The inorganic solid particles having a garnet structure include... Li7La3Zr2O12" in paragraph [0073] and "Li7La3Zr2O12" Example 17 in Table 1; Li7La3Zr2O12 is an oxide-based solid electrolyte).
Claims 34 and 43 are rejected under 35 U.S.C. 103 as being unpatentable over Iwasaki et al. (US-20180083269-A1) in view of Takahashi et al. (US-20220285678-A1) as applied to claims 31 and 32 above, and further in view of Fukuchi et al. (US-20110020704-A1).
Regarding Claim 34, Iwasaki in view of Takahashi discloses the all-solid-state lithium-ion battery according to claim 31 (see claim 31 rejection above).
Iwasaki in view of Takahashi does not explicitly disclose that the first solid electrolyte has an amorphous structure.
Fukuchi, however, in the same field of endeavor, lithium secondary batteries and solid electrolytes, discloses an inorganic solid electrolyte having an amorphous structure (see e.g. “the inorganic solid electrolyte is an amorphous material (glass)” in paragraph [0060] of Fukuchi).
Fukuchi further teaches that when the inorganic solid electrolyte is an amorphous material, oxygen-containing or nitrogen-containing compounds may be incorporated into the inorganic solid electrolyte to increase the clearance between the amorphous skeletons, thereby reducing hindrance to the movement of lithium ions and improving ion conductivity (see e.g. paragraph [0060] of Fukuchi). Therefore, it would have been obvious to a person of ordinary skill in the art, before the effective filing date of the claimed invention, to modify the first solid electrolyte of the all-solid-state lithium-ion battery of Iwasaki et al. in view of Takahashi et al. such that the first solid electrolyte has an amorphous structure as taught by Fukuchi et al. in order to reduce hindrance to the movement of lithium ions and improve ion conductivity as suggested by Fukuchi.
Regarding Claim 43, Iwasaki in view of Takahashi discloses the all-solid-state lithium-ion battery according to claim 32 (see claim 32 rejection above).
Iwasaki in view of Takahashi does not explicitly disclose that the first solid electrolyte has an amorphous structure.
Fukuchi, however, in the same field of endeavor, lithium secondary batteries and solid electrolytes, discloses an inorganic solid electrolyte having an amorphous structure (see e.g. “the inorganic solid electrolyte is an amorphous material (glass)” in paragraph [0060] of Fukuchi).
Fukuchi further teaches that when the inorganic solid electrolyte is an amorphous material, oxygen-containing or nitrogen-containing compounds may be incorporated into the inorganic solid electrolyte to increase the clearance between the amorphous skeletons, thereby reducing hindrance to the movement of lithium ions and improving ion conductivity (see e.g. paragraph [0060] of Fukuchi). Therefore, it would have been obvious to a person of ordinary skill in the art, before the effective filing date of the claimed invention, to modify the first solid electrolyte of the all-solid-state lithium-ion battery of Iwasaki et al. in view of Takahashi et al. such that the first solid electrolyte has an amorphous structure as taught by Fukuchi et al. in order to reduce hindrance to the movement of lithium ions and improve ion conductivity as suggested by Fukuchi.
Claims 45 and 46 are rejected under 35 U.S.C. 103 as being unpatentable over Iwasaki et al. (US-20180083269-A1) in view of Takahashi et al. (US-20220285678-A1) as applied to claim 26 above, and further in view of Tani et al. (US-20170256794-A1).
Regarding Claim 45, Iwasaki in view of Takahashi discloses the positive electrode active material for an all-solid-state lithium-ion battery according to claim 26 (see claim 26 rejection above).
Iwasaki in view of Takahashi does not explicitly disclose in the same lithium metal composite oxide that 0 < w ≤ 0.10 and 0 < z ≤ 0.40.
Tani, however, in the same field of endeavor, positive electrode active materials for lithium ion batteries, discloses a nickel lithium metal composite oxide represented by LixNi1-y-zMyNzO1.7-2.2, wherein M represents one or more metal elements selected from the group consisting of Co, Mn, Fe, and Cu, N represents one or more metal elements selected from the group consisting of Al, W, Ta, and B, 0.90 < x < 1.10, 0.01 < y < 0.15, and 0.005 < z < 0.10 (see e.g. paragraphs [0015]-[0016] and [0038]-[0041] of Tani).
Tani discloses that M can contain both Co and Mn and N to be Al. For example, when x = 1, y = 0.10, z = 0.05, O is selected as O2, M contains Co and Mn in equal proportions, and N is Al, the formula corresponds to LiNi0.85Co0.05Mn0.05Al0.05O2. This species directly correlates to the claimed species Li[Lix(Ni1-y-z-w)CoyMnzMw)1-x]O2 when the claimed x = 0, y = 0.05, z = 0.05, w = 0.05, and M is Al, which likewise simplifies to LiNi0.85Co0.05Mn0.05Al0.05O2. Accordingly, both z and w are greater than zero and fall within the claimed ranges.
Tani discloses ranges that overlap with the ranges claimed by the instant application. In the case where the prior art discloses a range that overlaps with the claimed range, a prima facie case of obviousness exists. See MPEP 2144.05 (I).
Tani also teaches that when the disclosed nickel lithium metal composite oxide is used as a positive electrode active material, the active material can be disposed on an electrode at a high density and overall battery performance improves (see e.g. paragraph [0052] of Tani). Therefore, it would have been obvious to a person of ordinary skill in the art, before the effective filing date of the claimed invention, to modify the lithium metal composite oxide positive electrode active material of Iwasaki et al. in view of Takahashi et al. such that it contains both Mn and Al in amounts satisfying 0 < z ≤ 0.40 and 0 < w ≤ 0.10 as taught by Tani et al. in order to dispose the active material on an electrode at a high density and improve overall battery performance as suggested by Tani.
Regarding Claim 46, Iwasaki in view of Takahashi discloses the positive electrode active material for an all-solid-state lithium-ion battery according to claim 26 (see claim 26 rejection above).
Iwasaki in view of Takahashi does not explicitly disclose in the same lithium metal composite oxide that 0 < w ≤ 0.10 and M is at least one element selected from the group consisting of Fe, Cu, Mg, W, B, Mo, Nb, Zn, Sn, Zr, Ga, and V.
Tani, however, in the same field of endeavor, positive electrode active materials for lithium ion batteries, discloses a nickel lithium metal composite oxide represented by LixNi1-y-zMyNzO1.7-2.2, wherein M represents one or more metal elements selected from the group consisting of Co, Mn, Fe, and Cu, N represents one or more metal elements selected from the group consisting of Al, W, Ta, and B, 0.90 < x < 1.10, 0.01 < y < 0.15, and 0.005 < z < 0.10 (see e.g. paragraphs [0015]-[0016] and [0038]-[0041] of Tani).
Tani discloses W and B as alternatives that may be incorporated into the nickel lithium metal composite oxide. For example, when x = 1, y = 0.10, z = 0.05, O is selected as O2, M is Co, and N is W, the formula simplifies to LiNi0.85Co0.10W0.05O2. This species directly correlates to the claimed species Li[Lix(Ni1-y-z-w)CoyMnzMw)1-x]O2 when the claimed x = 0, y = 0.10, z = 0, w = 0.05, and M is W, which likewise simplifies to LiNi0.85Co0.10W0.05O2. Accordingly, w is greater than zero and W is an element expressly included within the group recited in claim 46.
Tani discloses ranges that overlap with the ranges claimed by the instant application. In the case where the prior art discloses a range that overlaps with the claimed range, a prima facie case of obviousness exists. See MPEP 2144.05 (I).
Tani also teaches that when the disclosed nickel lithium metal composite oxide is used as a positive electrode active material, the active material can be disposed on an electrode at a high density and overall battery performance improves (see e.g. paragraph [0052] of Tani). Therefore, it would have been obvious to a person of ordinary skill in the art, before the effective filing date of the claimed invention, to modify the lithium metal composite oxide positive electrode active material of Iwasaki et al. in view of Takahashi et al. such that it contains W in an amount satisfying 0 < w ≤ 0.10 as taught by Tani et al. in order to dispose the active material on an electrode at a high density and improve overall battery performance as suggested by Tani.
Conclusion
The prior art made of record and not relied upon is considered pertinent to applicant's
disclosure:
Kurita et al. (US-20170187031-A1)
Ho et al. (US-20190157681-A1)
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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/J.J.E./ Examiner, Art Unit 1723
/NICHOLAS P D'ANIELLO/ Primary Examiner, Art Unit 1723
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