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 .
Priority
Acknowledgment is made of applicant’s claim for foreign priority under 35 U.S.C. 119 (a)-(d). The certified copy has been filed in parent Application No. JP2021-127586, filed on 08/03/2021 and PCT/JP2022/028918, filed on 07/27/2022.
Claim Objections
Claim 9 is objected to because of the following informalities: “A lithium secondary battery comprising: The positive electrode for the lithium secondary battery according to Claim 8” should be “A lithium secondary battery comprising: the positive electrode for the lithium secondary battery according to Claim 8”.
Appropriate correction is required.
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(d):
(d) REFERENCE IN DEPENDENT FORMS.—Subject to subsection (e), a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
The following is a quotation of pre-AIA 35 U.S.C. 112, fourth paragraph:
Subject to the following paragraph [i.e., the fifth paragraph of pre-AIA 35 U.S.C. 112], a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
Claim 4 and 11 are rejected under 35 U.S.C. 112(d) or pre-AIA 35 U.S.C. 112, 4th paragraph, as being of improper dependent form for failing to further limit the subject matter of the claim upon which it depends, or for failing to include all the limitations of the claim upon which it depends.
Claim 4 depends on claim 3, and claim 4 recites element M, which is not previously recited in claim 3. Therefore, the recitation of element M in claim 4 does not further limit the subject matter of claim 3.
Claim 11 depends on claim 10, and claim 11 recites element M, which is not previously recited in claim 10. Therefore, the recitation of element M in claim 11 does not further limit the subject matter of claim 10.
Applicant may cancel the claim(s), amend the claim(s) to place the claim(s) in proper dependent form, rewrite the claim(s) in independent form, or present a sufficient showing that the dependent claim(s) complies with the statutory requirements.
Claim Rejections - 35 USC § 103
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.
The factual inquiries 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.
Claims 1-14 are rejected under 35 U.S.C. 103 as being unpatentable over Arimura et al. (US PG Pub. 2018/0316008 A1) in view of Watanabe et al. (US PG Pub. 2017/0207455 A1).
Regarding claims 1, 5, 8 and 9, Arimura discloses a lithium secondary battery having a layered structure (para. [0139]) containing a positive electrode comprising a positive electrode active material (title).
The positive electrode active material is a particle comprising Li, Ni, X/M element and a sulfur element (para. [0014]-[0016]). The positive electrode active material is represented by the formula Li(Lix(NiaCobMncMd)1-x]O2 (para. [0014] and [0053]), where Cob, Mnc or Md represents the X/M element. Element X/M is selected from the group consisting of Co, Mn, Fe, Cu, Ti, Mg, Al, W, Mo, Nb, Zn, Sn, Zr, and Ga (para. [0014]-[0015]).
The concentration of the sulfur element (atom %) of sulfur atoms being present in the surface of the positive electrode active material is preferably between 0.01-2.5 (para. [0016]).
Arimura fails to specifically disclose that the positive electrode active material comprises a carbon element with abundance ratio and that formula (1) is satisfied.
Watanabe discloses a lithium secondary battery comprising a positive electrode active material (title) having extremely low contents of lithium carbonate (para. [0016]). Watanabe further discloses the contents of the lithium carbonate therein are reduced, gelation of an electrode slurry upon preparation thereof can be inhibited, and generation of gases upon storage under high-temperature conditions can be suppressed (para. [0031]).
The positive electrode active material comprises a lithium nickelate composite oxide particle containing Li, Ni and X/M element (para. [0019]). The positive electrode active material is represented by the formula Li1+aNi1-b-cCobMcO2 (para. [0019]), where Cob or Mc represents the X/M element. Element X/M is selected from the group consisting of Co, Mn, Ti, Mg, Al, Zn, Sn, Zr and B (para. [0019]).
The lithium nickelate composite oxide particles are coated with a lithium carbonate (para. [0021]-[0022]). The coating may be present in the form of an island-shaped coat covering a part of the surface of the core particle (para. [0045]). When the content of lithium carbonate in the positive electrode active substance particles is more than 0.65% by weight, the resulting secondary battery tends to be deteriorated in charge/discharge cycle characteristics (para. [0042]). In addition, when the content of lithium carbonate in the positive electrode active substance particles is lower than the content of lithium hydroxide therein, it may be difficult to suppress generation of gassed from the resulting secondary battery (para. [0042]-[0043]).
The carbon element is deemed to have a peak top at 289.5 ±2.0 eV when measured by X-ray photoelectron spectroscopy, since Watanabe discloses the same carbon element, carbonate, as the instant specification (para. [0018] of instant spec.).
It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to add the lithium carbonate coating of Watanabe to the positive electrode active material particle of Arimura so that gelation of an electrode slurry upon preparation thereof can be inhibited, and generation of gases upon storage under high-temperature conditions can be suppressed, thus improving the charge/discharge cycle characteristics.
As the amount, i.e. abundance ratio, of lithium carbonate on the surface of the particle is a variable that can be modified, among others, the precise amount would have been considered a result effective variable by one having ordinary skill in the art at the time the invention was made. Accordingly, one of ordinary skill in the art at the time the invention was made would have optimized, by routine experimentation, the amount of lithium carbonate on the surface of the positive electrode active material particle to obtain the desired abundance ratio to satisfy formula (1) (In re Boesch, 617 F.2d. 272, 205 USPQ 215 (CCPA 1980)), since it has been held that where the general conditions of the claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. (In re Aller, 105 USPQ 233).
Regarding claim 2, as discussed above in claim 1, Arimura discloses the concentration of the sulfur element (atom %) of sulfur atoms being present in the surface of the positive electrode active material is preferably between 0.01-2.5 (para. [0016]).
Arimura fails to specifically disclose that the positive electrode active material satisfied formula (2).
Watanabe discloses a lithium secondary battery comprising a positive electrode active material (title) having lithium carbonate and lithium hydroxide in varying amounts (Table 1). Watanabe further shows that XPS(Li) in atom% on the surface of cathode active material (Fig. 6) in varying amounts due to the presence of LiOH and Li2CO3 on the surface which affect the battery performance characteristics (para. [0097] – [0098] and [0101] – [0102]).
It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to adjust the amount of lithium carbonate and lithium hydroxide present on the surface of the positive electrode active material as taught by Watanabe to the positive electrode active material particle of Arimura so that gelation of an electrode slurry upon preparation thereof can be inhibited, and generation of gases upon storage under high-temperature conditions can be suppressed, thus improving the charge/discharge cycle characteristics.
As the amount, i.e. abundance ratio, of lithium carbonate and lithium hydroxide on the surface of the particle is a variable that can be modified, among others, the precise amount would have been considered a result effective variable by one having ordinary skill in the art at the time the invention was made. Accordingly, one of ordinary skill in the art at the time the invention was made would have optimized, by routine experimentation, the amount of lithium carbonate and lithium hydroxide on the surface of the positive electrode active material particle to obtain the desired abundance ratio to satisfy formula (2) (In re Boesch, 617 F.2d. 272, 205 USPQ 215 (CCPA 1980)), since it has been held that where the general conditions of the claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. (In re Aller, 105 USPQ 233).
Regarding claim 3 and 10, the combination of Arimura and Watanabe teaches the positive electrode active material for the lithium secondary battery (Arimura claim 3), further comprising Ni (Arimura, Li[Lix(NiaCobMncMd)1-x]O2) and at least one element X (Arimura, element M) selected from the group consisting of Fe, Cu, Ti, Mg, Al, W, Mo, Nb, Zn, Sn, Zr, and Ga (Arimura claim 3).
Arimura discloses that, in accordance with Compositional Formula (I) Li[Lix(NiaCobMncMd)1-x]O2 (Arimura claim 3), x=0.01, a=0.902, b=0.067, c=0.019, d=0.012, and M=Al and a concentration Q of sulfuric acid radicals being present in the whole positive electrode active material was 0.23 mass % (Example 7, para. [0285]). A concentration Q (mass %) of sulfuric acid radicals being present in the whole positive electrode active material is obtained by dissolving powders of the positive electrode active material in a hydrochloric acid, performing an inductively coupled plasma emission analysis method (ICP), measuring sulfur elements, and converting the amount of the measured sulfur elements into sulfuric acid radicals (para. [0045]).
For Arimura’s Example 7, Compositional Formula (I) becomes Li1.01(Ni0.902Co0.067Mn0.019 Al0.012)0.99 O2 equals Li1.01Ni0.893Co0.066Mn0.019Al0.012O2 with formula weight about 96.68 g/mol, calculated below:
6.94*1.01 + (58.69*0.902 + 58.93*0.067 + 54.94*0.019 + 26.98*0.012) * 0.99 + 2*(16.00) = 96.68 g/mol
Assume the basis of 100g of the positive electrode active material. At 0.23 mass% sulfuric acid radicals, the positive electrode active material contains 0.23g sulfuric acid radicals SO4 and 99.77 g Compositional Formula (I) oxide.
Sulfuric acid radicals mol: 0.23g / [(32.065 + 4*16.00) (g/mol)] = 0.0024 mol
Oxide mol: 99.77g / [96.68 (g/mol)] = 1.032 mol
Each SO4 contains one S atom, so S atom mol: 0.0024 mol
In Formula (3): Li : Ni : X : S = a : (1-b) : b : c also as a result of ICP elemental analysis (Applicant’s instant Specifications, para [0153]).
Hence, Ni + X = (1 - b) + b = 1 as the normalization denominator for Formula (3)
For Arimura’s Example 7: element X is element Al
a
=
L
i
N
i
+
A
l
=
1.01
0.893
+
0.012
=
1.116
b
=
A
l
N
i
+
A
l
=
0.012
0.893
+
0.012
=
0.013
c
=
S
n
o
r
m
a
l
i
z
e
d
m
o
l
o
x
i
d
e
(
N
i
+
A
l
)
=
0.0024
99.77
g
o
x
i
d
e
96.68
g
m
o
l
o
x
i
d
e
(
0.893
+
0.012
)
=
0.00256
The calculated results a, b and c satisfy 0.90 ≤ a ≤ 1.2, 0 < b ≤ 0.3, and 0.001 ≤ c ≤ 0.05, respectively.
Regarding claim 4 and 11, as discussed above in claim 1, Arimura discloses the concentration of the sulfur element (atom %) of sulfur atoms being present in the surface of the positive electrode active material is preferably between 0.01-2.5 (para. [0016]).
Arimura fails to specifically disclose that the positive electrode active material satisfied formula (4).
Watanabe discloses a lithium secondary battery comprising a positive electrode active material (title) having Li2CO3, LiOH, and Al2O3 in varying amounts (Table 1). Specifically, the positive electrode active material has coating compound Y comprising at least one element selected from the group consisting of Al, Mg, Zr, Ti and Si; and a coating compound Z comprising Li2CO3 and LiOH (abstract). The coating compound Y and Z may be present in the form of an island-shaped coat covering a part of the surface of the core particle (para. [0045]). The weight ratio of the coating compound Z to the coating compound Y, is usually 1 to 100, preferably 2 to 50 and more preferably 3 to 40 so that the resulting positive electrode active substance particles can exhibit excellent repeated charge/discharge cycle characteristics when being highly charged, and generation of gases therefrom upon storage under high-temperature conditions can be suppressed (para. [0066]).
Watanabe’s element Al in coating compound Y corresponds to Applicant’s element M, so Watanabe’s XPS (Al) corresponds to Applicant’s XPS(M). Watanabe further shows varying surface atom% of C, Li, Ni, and Al, as measured by XPS (Fig. 6), for the respective examples in Table 1 of the surface of the positive electrode active material which affect the battery performance characteristics (para. [0097] – [0098] and [0101] – [0102]).
It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to adjust the amount of Li2CO3, LiOH, and Al2O3 present on the surface of the positive electrode active material particle as taught by Watanabe to the positive electrode active material particle of Arimura so that the resulting positive electrode active material particles can exhibit excellent repeated charge/discharge cycle characteristics when being highly charged, and generation of gases therefrom upon storage under high-temperature conditions can be suppressed.
As the amount, i.e. abundance ratio, of Li2CO3, LiOH, and Al2O3 on the surface of the particle is a variable that can be modified, among others, the precise amount would have been considered a result effective variable by one having ordinary skill in the art at the time the invention was made. Accordingly, one of ordinary skill in the art at the time the invention was made would have optimized, by routine experimentation, the amount of Li2CO3, LiOH, and Al2O3 on the surface of the positive electrode active material particle to obtain the desired abundance ratio to satisfy formula (4) (In re Boesch, 617 F.2d. 272, 205 USPQ 215 (CCPA 1980)), since it has been held that where the general conditions of the claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. (In re Aller, 105 USPQ 233).
Regarding claim 6 and 13, the combination of Arimura and Watanabe teaches the positive electrode active material for the lithium secondary battery wherein a BET specific surface area is 0.1 m2/g or more and 3.5 m2/g or less (Arimura, para. [0091]), which overlaps with the claimed range of 0.1 m2/g or more and 3 m2/g or less. Per MPEP 2144.05, in the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art” a prima facie case of obviousness exists.
Regarding claim 7 and 14, the combination of Arimura and Watanabe teaches the positive electrode active material for the lithium secondary battery wherein a 50% cumulative volume particle size D50 (μm) is 3 μm or more and 20 μm or less (Arimura, para. [0086]), which overlaps with the claimed range of 5 μm or more and 30 μm or less. Per MPEP 2144.05, in the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art” a prima facie case of obviousness exists.
Regarding claim 12, the combination of Arimura and Watanabe teaches the positive electrode active material for the lithium secondary battery wherein XPS(S), which is the abundance ratio [at %] of the sulfur element, is from 0.01 to 2.5 (Arimura, para. [0070]). The disclosed range overlaps with the claimed range of 1 to 5 in formula (5). Per MPEP 2144.05, in the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art” a prima facie case of obviousness exists.
Conclusion
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/T.T.T./
THU T TRANExaminer, Art Unit 1788
10/07/2026
/Alicia Chevalier/Supervisory Patent Examiner, Art Unit 1788
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