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and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114.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 February 20th, 2026 has been entered.
Claim Status
Applicant’s arguments and claim amendments submitted on February 20th, 2026 have been entered into the file. Currently claims 1, 9, 13-14 are amended and claim 15 is new, resulting in claims 1-15 pending for examination.
Response to Amendment
Applicant’s arguments and claim amendments submitted on February 20th, 2026 have been entered into the file.
Applicant’s amendment of claim 9 has overcome the 35 USC § 112(d) rejection previously set forth in the Final Office Action mailed October 21st, 2025.
Applicant’s amendment of claim 14 has overcome the 35 USC § 112(a) and USC § 112(b) rejection previously set forth in the Final Office Action mailed October 21st, 2025.
Applicant’s amendment of claim 1 has overcome the 35 USC § 103 rejection as being unpatentable over Toma in view of Takahashi previously set forth in the Final Office Action mailed October 21st, 2025. However, new grounds of rejection are presented in this Office Action.
Claim Rejections - 35 USC § 103
In the event the determination of the status of the application as subject to AIA 35 U.S.C. 102 and 103 (or as subject to pre-AIA 35 U.S.C. 102 and 103) is incorrect, any correction of the statutory basis (i.e., changing from AIA to pre-AIA ) for the rejection will not be considered a new ground of rejection if the prior art relied upon, and the rationale supporting the rejection, would be the same under either status.
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.
Claims 1-8, 10, 12-15 are rejected under 35 U.S.C. 103 as being unpatentable over Toma (U.S. Patent Publication No. 20210363027 A1) in view of Takahashi (U.S. Patent Publication No. 20230135908 A1) and Murakami (Japanese Patent Publication No. 2020021741 A).
Regarding claim 1, Toma teaches a positive electrode active material for a non-aqueous electrolyte secondary battery (Paragraph 0001), including a lithium-transition metal composite oxide (Paragraph 0014).
In the third embodiment of the invention, Toma teaches the Formula (4) for the lithium-metal composite oxide represented by Li1+aNi1-x-yCoxMnyMzO2+β where
-0.05 ≤ a ≤ 0.50
0.02 ≤ x ≤ 0.30
0.02 ≤ y ≤ 0.30
0 ≤ z ≤ 0.05
-0.5 ≤ β ≤ 0.5
and M is at least one element selected from the group consisting of Mg, Ca, Al, Si, Fe, Cr,
V, Mo, W, Nb, Ti, and Zr) (Paragraph 0020).
To determine the mole percentage of nickel based on the total number of moles of metal elements excluding Li according to the instant claimed limitations, when each element is set to the lower limit of the ranges taught by Toma, the general formula is as follows: Li0.95Ni0.96Co0.02Mn0.02M0O1.5. Accordingly, the mole percentage of nickel with respect to total number of moles of metal elements excluding Li is:
m
o
l
%
N
i
=
0.96
0.96
+
0.02
+
0.02
=
96
%
When each element is set to the upper limit of the ranges taught by Toma, the general formula is as follows: Li1.5Ni0.40Co0.30Mn0.30M0.05O2.5. Accordingly, the mole percentage of nickel with respect to total number of moles of metal elements excluding Li is:
m
o
l
%
N
i
=
0.40
0.4
+
0.30
+
0.30
+
0.05
=
38
%
Thus, the range of mole percentage of Nickel in the lithium-transition metal composite oxide with respect to the total number of moles of metal elements excluding Li is represented by 38-96% as calculated above. The range of mole percentage of Ni of Toma substantially overlaps the claimed range of 80% or more in the instant claim. It has been held that obviousness exists where the claimed ranges overlap or lie inside ranges disclosed by the prior art. See MPEP 2144.05 (I). Therefore, it would have been obvious to one of ordinary skill in the art at the time of the invention to have selected from the overlapping portion of the range taught by Toma because overlapping ranges have been held to establish prima facie obviousness.
Toma teaches that the lithium-transition metal composite oxide according to the third embodiment may contain Co and Mn, and that M may be substituted with at least one selected from Al, Ti, Nb, Fe. Therefore, the Formula (4) of Toma will have at least one selected from the group consisting of Co, Mn, Al, Ti, Nb, and Fe, as limited by the instant claim.
Using the Formula (4) defined above at the maximum and minimum quantities of the variables, the Co content in the lithium-transition metal oxide based on the total number of moles of metal elements excluding Li is determined to be:
Li0.95Ni0.96Co0.02Mn0.02M0O1.5 :
m
o
l
%
C
o
=
0.02
0.96
+
0.02
+
0.02
=
2
%
Li1.5Ni0.40Co0.30Mn0.30M0.05O2.5:
m
o
l
%
C
o
=
0.30
0.40
+
0.30
+
0.30
+
0.05
=
29
%
The range of mole percentage of cobalt of Toma substantially overlaps the claimed ranges of the mole percentage of cobalt of 5 mol% or less in the instant claim. It has been held that obviousness exists where the claimed ranges overlap or lie inside ranges disclosed by the prior art. See MPEP 2144.05 (I). Therefore, it would have been obvious to one of ordinary skill in the art at the time of the invention to have selected from the overlapping portion of the range taught by Toma because overlapping ranges have been held to establish prima facie obviousness.
Toma teaches the lithium-transition metal composite oxide includes secondary particles each formed by aggregation of primary particles (Paragraph 0035).
Toma teaches in the third embodiment a particle having a core portion inside the particle and a shell portion formed around the core (Paragraph 0020).
Toma teaches the composition of the shell portion in the third particle is represented by general formula (6): Li1+a2Ni1-x2-y2Cox2Mny2Mz2O2+β2 where
-0.05 ≤ a2 ≤ 0.50
0 < 1-x2-y2 ≤ 0.6
0 ≤ z2 ≤ 0.05
-0.5 ≤ β2 ≤ 0.5
(Paragraph 00020) and M is at least one element selected from the group consisting of Mg, Ca, Al, Si, Fe, Cr, V, Mo, W, Nb, Ti, and Zr) as M is represented by the same element as the general formula (3) (Paragraph 0156) which is similar to M of general formula 1 (Paragraph 0067).
It would have been obvious to a person having ordinary skill in the art prior to the effective filing date of the instant invention to select Ca from the finite lists of possible combinations for M to arrive at the lithium-transition metal oxide of the instant claim since the combination of components would have yielded predictable results as a surface coating for primary particles, absent a showing of unexpected results commensurate in scope with the claimed invention. See Section 2143 of the MPEP, rationales (A) and (E).
When each element is set to the lower limit of the ranges taught by Toma, z2=0 and the presence of A (Ca) on the surface of the primary particles is 0%.
When each element is set to the upper limit of the ranges taught by Toma, the general formula is as follows: Li1.5Ni0.5999Co0.2Mn0.2M0.05O2.5. The upper limit of 1-x2-y2 must be less than 0.6, and is estimated to be 0.5999. Further, x2 + y2 must = 0.4 at the upper limit. x2 and y2 are variables which represent quantities of non-lithium metals. Thus, x2 + y2 appears in the denominator in the calculations below. Accordingly, the mole percentage of element A on the surface of the primary particles with respect to total number of moles of metal elements excluding Li is:
m
o
l
%
A
=
0.05
0.5999
+
0.2
+
0.2
+
0.05
=
4.8
%
The range of the mole percentage of element A on the surface of the primary particles with respect to total number of moles of metal elements excluding Li of Toma (0 to 4.8%) overlaps the claimed ranges of the percentage of element A on the surface of the primary particles with respect to total number of moles of metal elements excluding Li in the instant claim (0.01 to 1 mol %). It has been held that obviousness exists where the claimed ranges overlap or lie inside ranges disclosed by the prior art. See MPEP 2144.05 (I). Therefore, it would have been obvious to one of ordinary skill in the art at the time of the invention to have selected from the overlapping portion of the range taught by Toma because overlapping ranges have been held to establish prima facie obviousness.
Toma does not teach an element B selected from the group consisting of B, Zr, Al, Nb, Mo, and Ti is present on surfaces of the secondary particles.
Takahashi teaches a metal composite hydroxide for use as a positive electrode active material of a secondary battery, comprising nickel, manganese, and tungsten and optionally cobalt and an element M selected from Mg, Ca, Al, Ti, V, Cr, Zr, Nb, Mo, Hf, and Ta (Paragraphs 0031-0032) where the secondary particles of the metal composite hydroxide are formed by aggregation of primary particles (Paragraph 0054). Further, Takahashi teaches the secondary particles (Figure 1B, Element 2) comprises tungsten concentrations on their surface layer (Figure 1B, Element 3) (Paragraph 0055).
Takahashi teaches that the ratio of metal elements Ni:Mn:Co:W:M is represented by x:y:z:a:b, where 0.3 ≤ x ≤ 0.95 and 0 < a ≤ 0.1. Thus, the mole percentage of the element B (W) present on the surface of the secondary particles with respect to the total number of moles of Ni is represented by:
0
0.3
≤
m
o
l
%
W
≤
0.1
0.95
=
0
%
≤
m
o
l
%
W
≤
10
%
The range of mole percentage of tungsten present on the surface of the secondary particles with respect to the total number of moles of Ni of Takahashi substantially overlaps the claimed ranges of the element B present on the surface of the secondary particles with respect to the total number of moles of Ni in the instant claim. It has been held that obviousness exists where the claimed ranges overlap or lie inside ranges disclosed by the prior art. See MPEP 2144.05 (I).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the secondary particles of the lithium-transition metal composite oxide of Toma to incorporate the teachings of Takahashi in which a layer of tungsten is present on the surface of the secondary particles at the above-calculated concentration. Doing so would result in decreased reaction resistance and enhanced crystallinity of the lithium-metal composite oxide, as recognized by Takahashi (Paragraph 0050).
Additionally, Murakami discloses a positive electrode active material for a lithium secondary battery including a lithium composite metal compound composed of secondary particles formed from aggregating primary particles and a coating layer containing a metal composite oxide formed thereon. Murakami discloses three different embodiments which differ by the metal composite oxide of the coating layer, including embodiments in which the coating includes aluminum, another containing zirconium, and another contain tungsten (Paragraph 0007). Murakami explicitly teaches the coating material may be an oxide, hydroxide, carbonate, nitrate, sulfate, halide, oxalate or alkoxide of any one of aluminum, titanium, zirconium, and tungsten (Paragraph 0088). Murakami teaches that the coating layer composed of the lithium composite metal compound can be formed on the surface of the secondary particles (Paragraph 0087).
Therefore, given the general teachings of Murakami, it would have been obvious to one of ordinary skill in the pertinent art before the effective filing date of the claimed invention to substitute aluminum, titanium, and or zirconium secondary particle coating of Murakami for the tungsten secondary particle coating of Takahashi because Murakami teaches the coating applied to the surface of secondary particles formed by the agglomeration of primary particles may suitably be selected as tungsten, aluminum, titanium, and or zirconium. The substitution would have been one known element for another and one of ordinary skill in the pertinent art would reasonably expect the predictable result that the lithium composite metal compound would be useful as a coating applied to the surface of the secondary particles of the negative electrode active material of Murakami and possess the benefits of decreased reaction resistance and enhanced crystallinity taught by Takahashi and the benefits of reduced gas production and battery swelling taught by Murakami. See MPEP § 2143.I.(B).
Thus, when substituting the tungsten in the coating of the secondary particles present from 0 to 10% with respect to the total number of moles of Ni of Takahashi for the aluminum, zirconium, or titanium-containing coatings of Murakami, the instant claimed limitations are met.
Regarding claim 2, modified Toma teaches a positive electrode active material for a non-aqueous electrolyte secondary battery as discussed above with respect to claim 1, wherein the element B is present outside the element A on the surfaces of the secondary particles.
As seen in Figure 1(A) and 1(B) of Takahashi, the secondary particles (Element 2) are formed by the aggregation of primary particles (Element 1) and the layer of tungsten is formed on the outside of the secondary particles (Element 3). According to the modification of Toma by Takahashi, the primary particles including the core and the shell of Toma would be inside the coating of tungsten on the secondary particles, as illustrated below.
PNG
media_image1.png
868
518
media_image1.png
Greyscale
Annotated Figures 1(A) and 1(B) of Takahashi
Thus, when substituting the tungsten in the coating of the secondary particles Takahashi for the aluminum, zirconium, or titanium-containing coatings of Murakami, the ordinary artisan would expect the element B (aluminum, zirconium, or titanium) to be present outside the element A on the surfaces of the secondary particles.
Regarding claim 3, modified Toma teaches a positive electrode active material for a non-aqueous electrolyte secondary battery as discussed above with respect to claim 2.
Takahashi teaches tungsten is absent (not contained) inside the secondary particles and present only on the surfaces of the secondary particles (Paragraph 0071).
Thus, when substituting the tungsten in the coating of the secondary particles Takahashi for the aluminum, zirconium, or titanium-containing coatings of Murakami, the ordinary artisan would expect the element B (aluminum, zirconium, or titanium) to be absent inside the secondary particles and present only on the surfaces of the secondary particles.
Regarding claim 4, modified Toma teaches a positive electrode active material for a non-aqueous electrolyte secondary battery as discussed above with respect to claim 1.
As calculated above, Takahashi teaches the mole percentage of the element B (W) present on the surface of the secondary particles with respect to the total number of moles of Ni is between 0% to 10 mol%.
The range of mole percentage of tungsten present on the surface of the secondary particles with respect to the total number of moles of Ni of Takahashi (0 to 10 mol%) overlaps the claimed ranges of the element B present on the surface of the secondary particles with respect to the total number of moles of Ni in the instant claim. It has been held that obviousness exists where the claimed ranges overlap or lie inside ranges disclosed by the prior art. See MPEP 2144.05 (I).
Thus, when substituting the tungsten in the coating of the secondary particles Takahashi for the aluminum, zirconium, or titanium-containing coatings of Murakami, the ordinary artisan would expect the element B (aluminum, zirconium, or titanium) to be present in a quantity with respect to the total number of moles of Ni which overlaps the instant claimed range.
Regarding claim 5, modified Toma teaches a positive electrode active material for a non-aqueous electrolyte secondary battery as discussed above with respect to claim 1, wherein a ratio of a content of the element B to a content of the element A is 0.05 or more and 200 or less.
In the instant claim, A may be Ca or Sr. Takahashi also discloses a lithium transition metal oxide comprising an element M, which may be Ca (Paragraph 0032).
Further, Takahashi discloses that the ratio of metal elements Ni:Mn:Co:W:M is represented by x:y:z:a:b (Paragraph 0032). Therefore, the ratio of the content of element B to the content of element A may be represented by W:M (W:Ca), or a:b. At their minimum and maximum values, a:b will be between 0 and 1.
Therefore, the range of W to M of Takahashi substantially overlaps the claimed ranges of B:A in the instant claim. It has been held that obviousness exists where the claimed ranges overlap or lie inside ranges disclosed by the prior art. See MPEP 2144.05 (I).
Thus, when substituting the tungsten in the coating of the secondary particles Takahashi for the aluminum, zirconium, or titanium-containing coatings of Murakami, the ordinary artisan would expect the element B (aluminum, zirconium, or titanium) to be present in a quantity such that the ratio of the content of the element B to the content of the element A overlaps the instant claimed range.
Regarding claim 6, modified Toma teaches a positive electrode active material for a non-aqueous electrolyte secondary battery as discussed above with respect to claim 1.
Toma does not explicitly teach that the full width at half maximum n of a diffraction peak of a (208) plane in an X-ray diffraction pattern of the lithium-transition metal composite oxide is 0.30º< n < 0.55º.
It is reasonable to presume that the n of the diffraction peak of a (208) plane is inherent to Toma. Support for said presumption is found in that the lithium-transition metal composite oxide of Toma, as discussed above with respect to claim 1, comprises 80 mol% or more of Ni based on a total number of moles of metal elements excluding Li, a Co content of less than 5 mol% based on a total number of moles of metal elements excluding Li, and an element Ca present on the surfaces of the primary particles in an amount of 0.01 mol% or more and 1 mol% or less based on the total number of moles of the metal elements excluding Li. Further, Toma teaches the lithium composite oxide secondary particles formed by the aggregation of primary particles. The modification of Toma by Soon resulted in a coated layer of tungsten on the exterior of the secondary particles.
Further, Toma teaches in the process of forming the lithium transition metal composite oxide a mixing step wherein proportion of the precursor and the lithium compound is adjusted so that the ratio (Li/Me) of the sum (Me) of the metal atoms other than lithium to the number of atoms of lithium (Li) in the lithium mixture is 0.95 or more and 1.5 or less, preferably 1.0 or more and 1.2 or less, more preferably 1.0 or more and 1.1 or less. (Paragraph 0179). The instant application discloses the mixing ratio of the composite oxide obtained in the first step and the Li compound to be preferably within the range of 1:0.98 to 1:1.1 (Paragraph 0048). The mixing ratios of Toma overlap those of the instant application, suggesting inherent similarities in the process of forming the lithium metal composite oxide.
Toma teaches a calcination process which may be performed after the mixing process, which occurs between 1 and 10 hours in an oxidizing atmosphere (Paragraph 0202) at a temperature between 350 oC and 800oC in order to diffuse lithium into the precursor material and obtain uniform particles (Paragraph 0201). The instant application discloses the calcination of the mixture obtained in the second step which occurs in an oxygen atmosphere for 1 to 10 hours at a temperature of 450 oC and 850oC. The time, temperature, and oxygen presence in the calcination process of Toma overlap those of the instant application, suggesting inherent similarities in the process of forming the lithium metal composite oxide.
Toma modified by Takahashi and Murakami teaches a lithium transition metal composite oxide having a layered structure and formed by the aggregation of primary particles to form secondary particles, and a coating on the surface of the secondary particles including aluminum, zirconium, and or titanium, which are the materials suitable for the coating B of the instant application. Further, in the method of manufacturing the coating of Murakami, the coating raw material is preferably an oxide of aluminum, titanium, zirconium, or tungsten (Paragraph 0088), which overlaps with the instant element-B containing raw material of the fourth step of the instant disclosure (Paragraph 0051).
Further, Toma teaches a process of forming the layered primary particles including the mixing ratios and calcination step conditions which align with those of the instant application. It is therefore reasonable to presume that the crystallinity of the lithium metal composite oxide taught by Toma in view of Soon would result in an X-ray diffraction pattern where the full width at half max of the (208) plane is as claimed. Support for said presumption is also found in that Toma uses the same material for element A (calcium sulfate) (Paragraph 0110) to form an equivalent lithium metal composite oxide as the claimed invention.
Regarding claim 7, modified Toma teaches a nonaqueous electrolyte secondary battery comprising a positive electrode including the positive electrode active material according to claim 1, a negative electrode, and a non-aqueous electrolyte (Paragraph 0024).
Regarding claim 8, modified Toma teaches the positive electrode active material for a non-aqueous electrolyte secondary battery according to claim 1,
As discussed above in the rejection of claim 1, Toma teaches the composition of the shell portion of particle is represented by general formula (6): Li1+a2Ni1-x2-y2Cox2Mny2Mz2O2+β2 where -0.05 ≤ a2 ≤ 0.50, 0 < 1-x2-y2 ≤ 0.6, 0 ≤ z2 ≤ 0.05, and -0.5 ≤ β2 ≤ 0.5, (Paragraph 0020) where M was obviously selected as Ca from the from the finite lists of possible combinations for M to arrive at the lithium-transition metal oxide of the instant claim since the combination of components would have yielded predictable results as a surface coating for primary particles.
Further, when each element is set to the lower limit of the ranges taught by Toma, z2=0 and the presence of A (Ca) on the surface of the primary particles is 0%.
When each element is set to the upper limit of the ranges taught by Toma, the general formula is as follows: Li1.5Ni0.5999Co0.2Mn0.2M0.05O2.5and the mole percentage of element A on the surface of the primary particles with respect to total number of moles of metal elements excluding Li was calculated to be:
m
o
l
%
A
=
0.05
0.5999
+
0.2
+
0.2
+
0.05
=
4.8
%
The range of the mole percentage of element A on the surface of the primary particles with respect to total number of moles of metal elements excluding Li of Toma (0 to 4.8%) overlaps the claimed ranges of the percentage of element A on the surface of the primary particles with respect to total number of moles of metal elements excluding Li in the instant claim (0.1 to 0.8 mol %). Therefore, prima facie obviousness is established. See MPEP 2144.05 (I).
Regarding claim 10, modified Toma teaches the positive electrode active material for a non-aqueous electrolyte secondary battery according to claim 1.
As discussed above in the rejection of claim 1, Toma in view of Takashi teaches a layer of tungsten is present on the surface of the secondary particles in order to decrease reaction resistance and enhance crystallinity of the lithium-metal composite oxide, where the tungsten present on the surface of the secondary particles is 0 mol% to 10 mol% with respect to the total number of moles of Ni in the instant claim.
Thus, when substituting the tungsten in the coating of the secondary particles Takahashi for the aluminum, zirconium, or titanium-containing coatings of Murakami, the ordinary artisan would expect the element B (aluminum, zirconium, or titanium) to be present in a quantity that overlaps the instant claimed range according to the teachings of Takahashi.
Regarding claim 12, modified Toma teaches the positive electrode active material for a non-aqueous electrolyte secondary battery according to claim 11.
As discussed above in the rejection of claim 1, Toma teaches the Formula (4) for the lithium-metal composite oxide represented by Li1+aNi1-x-yCoxMnyMzO2+β where -0.05 ≤ a ≤ 0.50, 0.02 ≤ x ≤ 0.30, 0.02 ≤ y ≤ 0.30, 0 ≤ z ≤ 0.05, and -0.5 ≤ β ≤ 0.5, where M is at least one element selected from the group consisting of Mg, Ca, Al, Si, Fe, Cr, V, Mo, W, Nb, Ti, and Zr (Paragraph 0020).
Further calculated in the rejection of claim 1 was the mole percentage of nickel based on the total number of moles of metal elements excluding Li. When each element in the formula of Toma was set to the lower limit of the ranges taught by Toma, the general formula is as follows: Li0.95Ni0.96Co0.02Mn0.02M0O1.5. Accordingly, the mole percentage of nickel with respect to total number of moles of metal elements excluding Li is:
m
o
l
%
N
i
=
0.96
0.96
+
0.02
+
0.02
=
96
%
When each element is set to the upper limit of the ranges taught by Toma, the general formula is as follows: Li1.5Ni0.40Co0.30Mn0.30M0.05O2.5. Accordingly, the mole percentage of nickel with respect to total number of moles of metal elements excluding Li is:
m
o
l
%
N
i
=
0.40
0.40
+
0.30
+
0.30
+
0.05
=
38
%
Thus, the range of mole percentage of Nickel in the lithium-transition metal composite oxide with respect to the total number of moles of metal elements excluding Li is represented by 38-96% as calculated above. The range of mole percentage of Ni of Toma substantially overlaps the claimed range of 90% or more in the instant claim. Therefore, prima facie obviousness is established. See MPEP 2144.05 (I).
The Formula (4) of Toma teaches Mn present in the lithium-metal composite oxide with subscript y, 0.02 ≤ y ≤ 0.30 and M with subscript z, 0 ≤ z ≤ 0.05. Further, it would have been obvious to a person having ordinary skill in the art prior to the effective filing date of the instant invention to select Al from the finite lists of possible combinations for M in the Formula for the metal oxide of Takahashi to arrive at the positive electrode active material of the instant claim since the combination of components would have yielded predictable results in a non-aqueous electrolyte secondary battery, absent a showing of unexpected results commensurate in scope with the claimed invention. See Section 2143 of the MPEP, rationales (A) and (E).
When each element in the formula of Toma was set to the lower limit of the ranges taught by Toma, the general formula is as follows: Li0.95Ni0.96Co0.02Mn0.02Al0O1.5. Accordingly, the mole percentage of Mn and Al with respect to total number of moles of metal elements excluding Li is:
m
o
l
%
M
n
+
A
l
=
0.02
+
0
0.96
+
0.02
+
0.02
=
2
%
When each element is set to the upper limit of the ranges taught by Toma, the general formula is as follows: Li1.5Ni0.40Co0.30Mn0.30Al0.05O2.5. Accordingly, the mole percentage of Mn and Al with respect to total number of moles of metal elements excluding Li is:
m
o
l
%
M
n
+
A
l
=
0.30
+
0.05
0.4
+
0.30
+
0.30
+
0.05
=
33
%
Thus, the range of mole percentage of Mn and Al in the lithium-transition metal composite oxide with respect to the total number of moles of metal elements excluding Li is represented by 2-33% as calculated above. The range of mole percentage of Mn and Al of Toma substantially overlaps the claimed range of 1 mol% to 5 mol% in the instant claim. Therefore, prima facie obviousness is established. See MPEP 2144.05 (I).
Regarding claim 13, modified Toma teaches the positive electrode active material for a non-aqueous electrolyte secondary battery according to claim 1. As discussed above, the substitution of tungsten of Takahashi for the suitable coating materials of Murakami resulted in the element B is at least one selected from the group consisting of Zr and Al.
Regarding claim 14, modified Toma teaches the positive electrode active material for a non-aqueous electrolyte secondary battery according to claim 1.
As discussed above, Toma teaches the composition of the shell portion of the particle including the element A, Ca. Because the element A is formed as a coating layer on the surface of the primary particles, it is considered to not form a solid solution with Ni, meeting the instant claimed limitations.
Regarding claim 15, Toma teaches the positive electrode active material for a non-aqueous electrolyte secondary battery according to claim 2.
As discussed above in the rejection of claim 1, Toma teaches the composition of the shell portion of the primary particle include Ca as the element A.
Further, Toma teaches the range of the mole percentage of element A on the surface of the primary particles with respect to total number of moles of metal elements excluding Li is 0 to 4.8%, which overlaps the claimed ranges of the percentage of element A on the surface of the primary particles with respect to total number of moles of metal elements excluding Li in the instant claim (0.1 to 0.8 mol %). Therefore, prima facie obviousness is established. See MPEP 2144.05 (I).
As discussed above in the rejection of claim 1, Toma in view of Takashi teaches a layer of tungsten is present on the surface of the secondary particles in order to decrease reaction resistance and enhance crystallinity of the lithium-metal composite oxide, where the tungsten present on the surface of the secondary particles is 0 mol% to 10 mol% with respect to the total number of moles of Ni in the instant claim.
Thus, when substituting the tungsten in the coating of the secondary particles Takahashi for the aluminum, zirconium, or titanium-containing coatings of Murakami, the ordinary artisan would expect the element B (aluminum, zirconium, or titanium) to be present in a quantity that overlaps the instant claimed range according to the teachings of Takahashi.
Further, as discussed above, Takahashi discloses that the ratio of metal elements Ni:Mn:Co:W:M is represented by x:y:z:a:b (Paragraph 0032). Therefore, the ratio of the content of element B to the content of element A may be represented by W:M (W:Ca), or a:b. At their minimum and maximum values, a:b will be between 0 and 1.
Therefore, the range of W to M of Takahashi substantially overlaps the claimed ranges of B:A in the instant claim. It has been held that obviousness exists where the claimed ranges overlap or lie inside ranges disclosed by the prior art. See MPEP 2144.05 (I).
Thus, when substituting the tungsten in the coating of the secondary particles Takahashi for the aluminum, zirconium, or titanium-containing coatings of Murakami, the ordinary artisan would expect the element B (aluminum, zirconium, or titanium) to be present in a quantity such that the ratio of the content of the element B to the content of the element A overlaps the instant claimed range.
Claim 6 is additionally rejected under 35 U.S.C. 103 as being unpatentable over Toma in view of Takahashi and Murakami as applied to claims 1-8, 10, 12-15 above, further in view of Aoki (W.O. 2019131234 A1) (machine translation relied upon).
Further regarding claim 6, modified Toma teaches a positive electrode active material for a non-aqueous electrolyte secondary battery as discussed above with respect to claim 1.
Toma does not explicitly teach that the full width at half maximum n of a diffraction peak of a (208) plane in an X-ray diffraction pattern of the lithium-transition metal composite oxide is 0.30º< n < 0.55º.
Aoki discloses a lithium transition metal oxide for use in a positive electrode active material for a non-aqueous electrolyte secondary battery (Paragraph 0008). Aoki teaches the lithium transition metal oxide has a layered structure, wherein the ratio of Ni in the lithium transition metal oxide is 91 mol % to 99 mol % with respect to the total number of moles of metal elements excluding Li, a transition metal present in the layered structure from 1 mol % to 2.5 mol % relative to the total molar amount of the transition metal in the Ni-containing lithium transition metal oxide. Further, Aoki teaches that the X-ray diffraction pattern of this compound is characterized by a half-value width n of the diffraction peak of (208) plane to be 0.30° ≤ n ≤ 0.50° (Paragraph 0009). At these quantities, Aoki teaches the high capacity of the non-aqueous electrolyte secondary battery can be achieved as well as increase of the charge/discharge cycle characteristics (Paragraph 0011).
As discussed above with respect to claim 1, the lithium composite oxide of modified Toma contains a range of nickel with respect to the total number of moles of metal elements excluding Li calculated to be 38 to 96 mol%, which overlaps the range of Ni in the lithium transition metal oxide of Aoki. Further discussed in claim 1 is the presence of a transition metal (cobalt) present in the range of 2 to 29 mol% with respect to the total moles of metal elements excluding Li in the lithium metal composite oxide, which overlaps the molar percentage range of the transition metal of Aoki. Toma also teaches the core and shell portion of the primary particles which make up a layered structure of the lithium metal composite oxide. Thus, these similarities suggest that the lithium composite oxide of modified Toma is open to modification of Aoki.
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the X-ray diffraction pattern of the lithium metal composite oxide of Toma modified by Takahashi to incorporate the teachings of Aoki in which the half-value width n of the diffraction peak of (208) plane to be 0.30° ≤ n ≤ 0.50°. Doing so would result in the suppression of the decrease of the charge/discharge cycle characteristics, as recognized by Aoki.
Claim 9 is rejected under 35 U.S.C. 103 as being unpatentable over Toma in view of Takahashi and Murakami as applied to claims 1-8, 10, 12-15 above, further of Kim (U.S. Patent Publication No. 20170358796 A1).
Regarding claim 9, Toma teaches the positive electrode active material for a non-aqueous electrolyte secondary battery according to claim 1.
As discussed above in the rejection of claim 1, Toma teaches the composition of the shell portion of the positive electrode material particles includes calcium (when M=Ca, as set forth in the obviousness rejection above).
Toma is silent as to the element A present on the surface of the primary particles is present as Sr.
However, Kim discloses a positive active material for a lithium ion secondary battery (Paragraph 0001). Kim teaches the positive electrode active material particles made of a lithium metal oxide composition (Formula 1) including metals such as nickel and cobalt in addition to lithium and oxygen (Paragraphs 00038-0039). Kim teaches the lithium metal oxide represented by Formula 1 may be in the form of secondary particles resulting from the agglomeration of primary particles (Paragraph 0042). Thus, Kim teaches a positive electrode active material which shares a similar structure and composition as that of the instant disclosure.
Further, Kim teaches a lithium-containing compound of Formula 2 in the form of a layer which may be disposed on the surface of the primary particles (Paragraph 0042). Kim teaches Formula 2 of the form Li2-xM’O3-y, where M’ is at least one element selected from Mg, Al, Ca, Ti, V, Cr, Fe, Cu, Zn, Ga, Sr, Y, Zr, Nb, Mo, Ru, and F; 0≦x≦1; and 0≦y≦3. As discussed above, Toma teaches the general formula 6 to represent the shell portion of the positive electrode material, comprising lithium, nickel, cobalt, manganese, oxygen, and at least one element selected from Mg, Ca, Al, Si, Fe, Cr, V, Mo, W, Nb, Ti, and Zr. Thus, Kim teaches a coating for the secondary particles of positive electrode active material which shares a similar structure and composition as that of the instant disclosure.
Therefore, given the general teachings of Kim it would have been obvious to one of ordinary skill in the pertinent art before the effective filing date of the claimed invention to substitute strontium in the primary particle coating of Kim for calcium in the shell portion of Toma, because Kim teaches the coating for the primary particles may suitably be selected as strontium or calcium. The substitution would have been one known element for another and one of ordinary skill in the pertinent art would reasonably expect the predictable result that the modified composition would be useful as a coating/shell for the primary particles of Toma and possess the benefits of improved battery performance, initial efficiency, and rate and lifetime characteristics taught by Kim (Paragraph 0014). See MPEP § 2143.I.(B).
Claim 11 is rejected under 35 U.S.C. 103 as being unpatentable over Toma in view of Takahashi and Murakami as applied to claims 1-8, 10, 12-15 above, further in view of Li (Non-Patent Literature, “Is Cobalt Needed in Ni-Rich Positive Electrode Materials for Lithium Ion Batteries?”).
Regarding claim 11, modified Toma teaches the positive electrode active material for a non-aqueous electrolyte secondary battery according to claim 1.
Modified Toma does not teach the lithium-transition metal composite oxide is free of Co and contains Mn and Al.
However, Li discloses that NCA materials with formula LiNi1-x-yCoxAlyO2 widely used in the electric vehicle industry are traditionally believed to have enhanced properties due to cobalt and aluminum in these materials. Li studies the roles of different cation substituents in materials represented by LiNi1-nMnO2, where M=Al, Mn, Mg, or Co. Li teaches that cobalt brings little or no value at all to NCA-type materials with high nickel content (> 90% Ni), with materials such as LiNi0.95M0.05O2 (M= Al, Mn, or Mg) performing superior to NCA materials with 5% cobalt content (Abstract). Li also teaches the high price of cobalt as motivation for finding alternative NCA materials with minimal cobalt (Page A429, Column 1, Paragraph 1).
In particular, Li finds that Co content up to 5% does not effectively suppress phase transitions during charge and discharge, while 5% Mn, 5% Mg, and 5% Al materials represented by LiNi1-nMnO2, where M=Al, Mn, or Mg showed an effective suppression of phase transitions (Page A431, Column 2, Paragraph 3). Further, Li teaches that Co included in electrode active materials does not contribute to structural stabilization (Page A435, Column 2, Paragraph 2) or thermal stability (Page A436, Column 2, Paragraph 2) while cation substitution with Mn, Al, or Mg were able to lower the reactivity of the positive electrode material with the electrolyte (Page A436, Column 2, Paragraph 2).
As discussed above, Toma teaches the Formula (4) for the lithium-metal composite oxide represented by Li1+aNi1-x-yCoxMnyMzO2+β. The material for the positive electrode active material of Toma may be considered high nickel content according to Li, as the mole percentage of nickel in the lithium-transition metal composite oxide was calculated to be 38-96%, overlapping the > 90% nickel content set forth by Li.
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the lithium-metal composite oxide of Toma to incorporate the teachings of Li in which the cobalt is removed and replaced with substituted cations Al or Mn. As seen in the Formula 4 of Toma, the addition of Mn cations to replace Co in the formula would increase the subscript of Mn, (y), while the addition of Al cations would necessitate the ordinary artisan selecting Al from the finite list of possible combinations for the placeholder element M in the formula (4) of Toma and increasing the subscript of M, (z). Doing so would advantageously remove the expensive cobalt in the positive electrode active material without negatively impacting and even providing superior suppression of phase transitions, structural and thermal stability, and lower reactivity of the positive electrode material with the electrolyte, as recognized by Li.
Claims 1-8, 10, 12-15 are alternately rejected under 35 U.S.C. 103 as being unpatentable over Toma in view of Soon (Korean Patent Publication No. 20150013077 A).
Regarding claim 1, Toma teaches a positive electrode active material for a non-aqueous electrolyte secondary battery (Paragraph 0001), including a lithium-transition metal composite oxide (Paragraph 0014).
In the third embodiment of the invention, Toma teaches the Formula (4) for the lithium-metal composite oxide represented by Li1+aNi1-x-yCoxMnyMzO2+β where
-0.05 ≤ a ≤ 0.50
0.02 ≤ x ≤ 0.30
0.02 ≤ y ≤ 0.30
0 ≤ z ≤ 0.05
-0.5 ≤ β ≤ 0.5
and M is at least one element selected from the group consisting of Mg, Ca, Al, Si, Fe, Cr,
V, Mo, W, Nb, Ti, and Zr) (Paragraph 0020).
To determine the mole percentage of nickel based on the total number of moles of metal elements excluding Li according to the instant claimed limitations, when each element is set to the lower limit of the ranges taught by Toma, the general formula is as follows: Li0.95Ni0.96Co0.02Mn0.02M0O1.5. Accordingly, the mole percentage of nickel with respect to total number of moles of metal elements excluding Li is:
m
o
l
%
N
i
=
0.96
0.96
+
0.02
+
0.02
=
96
%
When each element is set to the upper limit of the ranges taught by Toma, the general formula is as follows: Li1.5Ni0.40Co0.30Mn0.30M0.05O2.5. Accordingly, the mole percentage of nickel with respect to total number of moles of metal elements excluding Li is:
m
o
l
%
N
i
=
0.40
0.4
+
0.30
+
0.30
+
0.05
=
38
%
Thus, the range of mole percentage of Nickel in the lithium-transition metal composite oxide with respect to the total number of moles of metal elements excluding Li is represented by 38-96% as calculated above. The range of mole percentage of Ni of Toma substantially overlaps the claimed range of 80% or more in the instant claim. It has been held that obviousness exists where the claimed ranges overlap or lie inside ranges disclosed by the prior art. See MPEP 2144.05 (I). Therefore, it would have been obvious to one of ordinary skill in the art at the time of the invention to have selected from the overlapping portion of the range taught by Toma because overlapping ranges have been held to establish prima facie obviousness.
Toma teaches that the lithium-transition metal composite oxide according to the third embodiment may contain Co and Mn, and that M may be substituted with at least one selected from Al, Ti, Nb, Fe. Therefore, the Formula (4) of Toma will have at least one selected from the group consisting of Co, Mn, Al, Ti, Nb, and Fe, as limited by the instant claim.
Using the Formula (4) defined above at the maximum and minimum quantities of the variables, the Co content in the lithium-transition metal oxide based on the total number of moles of metal elements excluding Li is determined to be:
Li0.95Ni0.96Co0.02Mn0.02M0O1.5 :
m
o
l
%
C
o
=
0.02
0.96
+
0.02
+
0.02
=
2
%
Li1.5Ni0.40Co0.30Mn0.30M0.05O2.5:
m
o
l
%
C
o
=
0.30
0.40
+
0.30
+
0.30
+
0.05
=
29
%
The range of mole percentage of cobalt of Toma substantially overlaps the claimed ranges of the mole percentage of cobalt of 5 mol% or less in the instant claim. It has been held that obviousness exists where the claimed ranges overlap or lie inside ranges disclosed by the prior art. See MPEP 2144.05 (I). Therefore, it would have been obvious to one of ordinary skill in the art at the time of the invention to have selected from the overlapping portion of the range taught by Toma because overlapping ranges have been held to establish prima facie obviousness.
Toma teaches the lithium-transition metal composite oxide includes secondary particles each formed by aggregation of primary particles (Paragraph 0035).
Toma teaches in the third embodiment a particle having a core portion inside the particle and a shell portion formed around the core (Paragraph 0020).
Toma teaches the composition of the shell portion in the third particle is represented by general formula (6): Li1+a2Ni1-x2-y2Cox2Mny2Mz2O2+β2 where
-0.05 ≤ a2 ≤ 0.50
0 < 1-x2-y2 ≤ 0.6
0 ≤ z2 ≤ 0.05
-0.5 ≤ β2 ≤ 0.5
(Paragraph 00020) and M is at least one element selected from the group consisting of Mg, Ca, Al, Si, Fe, Cr, V, Mo, W, Nb, Ti, and Zr) as M is represented by the same element as the general formula (3) (Paragraph 0156) which is similar to M of general formula 1 (Paragraph 0067).
It would have been obvious to a person having ordinary skill in the art prior to the effective filing date of the instant invention to select Ca from the finite lists of possible combinations for M to arrive at the lithium-transition metal oxide of the instant claim since the combination of components would have yielded predictable results as a surface coating for primary particles, absent a showing of unexpected results commensurate in scope with the claimed invention. See Section 2143 of the MPEP, rationales (A) and (E).
When each element is set to the lower limit of the ranges taught by Toma, z2=0 and the presence of A (Ca) on the surface of the primary particles is 0%.
When each element is set to the upper limit of the ranges taught by Toma, the general formula is as follows: Li1.5Ni0.5999Co0.2Mn0.2M0.05O2.5. The upper limit of 1-x2-y2 must be less than 0.6, and is estimated to be 0.5999. Further, x2 + y2 must = 0.4 at the upper limit. x2 and y2 are variables which represent quantities of non-lithium metals. Thus, x2 + y2 appears in the denominator in the calculations below. Accordingly, the mole percentage of element A on the surface of the primary particles with respect to total number of moles of metal elements excluding Li is:
m
o
l
%
A
=
0.05
0.5999
+
0.2
+
0.2
+
0.05
=
4.8
%
The range of the mole percentage of element A on the surface of the primary particles with respect to total number of moles of metal elements excluding Li of Toma (0 to 4.8%) overlaps the claimed ranges of the percentage of element A on the surface of the primary particles with respect to total number of moles of metal elements excluding Li in the instant claim (0.01 to 1 mol %). It has been held that obviousness exists where the claimed ranges overlap or lie inside ranges disclosed by the prior art. See MPEP 2144.05 (I). Therefore, it would have been obvious to one of ordinary skill in the art at the time of the invention to have selected from the overlapping portion of the range taught by Toma because overlapping ranges have been held to establish prima facie obviousness.
Toma does not teach an element B selected from the group consisting of B, Zr, W, Al, Nb, Mo, and Ti is present on surfaces of the secondary particles.
Soon discloses a positive electrode active material containing a boron-containing coating, and an embodiment as illustrated in Figure 1 in which the boron-containing coating layer is included on the surface of polycrystalline lithium manganese oxide particles (Paragraphs 0001, 0025) (Figure 1).
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Figure 1 of Soon
Soon teaches the positive electrode active material comprising manganese and aluminum in additional to lithium and oxygen (Paragraphs 0032-0036), which overlaps the materials comprising the composition of the positive electrode active material of the instant claim. Soon teaches the polycrystal having a structure that is a secondary particle formed by a plurality of aggregated primary particles (Paragraph 0037), which overlaps the structure of the positive electrode active material of the instant claim. Soon teaches the advantage of the boron-containing coating to prevent direct contact between the lithium metal oxide and the electrolyte, in order to suppress side reactions between the positive electrode active material and the electrolyte (Paragraph 0020).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the secondary particles of the lithium-transition metal composite oxide of Toma to incorporate the teachings of Soon in which a boron-containing layer is present on the surface of the secondary particles. Doing so would result in the prevention of contact between the electrolyte and the positive electrode material, as recognized by Soon.
Toma does not teach the element B present on surfaces of the secondary particles in an amount of 0.05 mol% or more and 2 mol% or less based on a total number of moles of Ni in the composite oxide.
Soon, as discussed above, discloses a positive electrode active material containing a boron-containing coating on the surface of polycrystalline lithium manganese oxide particles. Soon teaches the thickness of the coating layer formed on the surface of the secondary particles may be in the range of 1 nm to 500 nm (Paragraph 0043). Soon teaches that when the thickness of the coating layer is less than 1 nm, the coating layer formed on the surface of the polycrystalline lithium manganese oxide is too thin so that the effect of suppressing side reactions between the positive electrode active material and the electrolyte during charging and discharging may be insignificant,. Soon teaches when the thickness of the coating layer exceeds 500 nm, it is too thick and can cause electrochemical degradation due to increased resistance (Paragraph 0044).
Thus, Soon teaches the thickness of the coating layer as able to be tuned in order to achieve a balance between maximizing the ability to suppress side reactions between the positive electrode active material while also keeping resistance low. The ordinary artisan would recognize that by adjusting the thickness of the boron-containing coating layer on the polycrystalline secondary particles, the amount of boron present on the surface of the secondary particles based on the total number of moles of nickel present in the composite oxide would also be adjusted.
Therefore, absent unexpected results, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to optimize the coating thickness of boron on the secondary particles of positive electrode active material (and therefore the quantity of boron present on the surfaces of the secondary particles based on the total number of moles of Ni in the composite oxide) since it has been held that where general conditions of a claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. See MPEP 2144.05. In the present invention one would have been motivated to optimize the thickness of the boron coating layer on the secondary polycrystalline particles to obtain a quantity of boron present on the surfaces of the secondary particles based on the total number of moles of Ni in the composite oxide within the claimed ranges in order to achieve a favorable balance between suppressing side reactions between positive electrode material and electrolyte while also minimizing electrochemical degradation and resistance, as recognized Soon.
Regarding claim 2, modified Toma teaches a positive electrode active material for a non-aqueous electrolyte secondary battery as discussed above with respect to claim 1, wherein the element B is present outside the element A on the surfaces of the secondary particles.
As seen in the embodiment exemplified by Figure 1 of Soon, the secondary particles (polycrystalline lithium manganese oxide) are formed by the aggregation of primary particles (Paragraph 0037) and the coating layer comprising boron is formed on the outside of the secondary particles. According to the modification of Toma by Soon, the primary particles including the core and the shell of Toma would be inside the coating comprising boron on the secondary particles, as illustrated below.
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Figure 1 of Soon
Regarding claim 3, modified Toma teaches a positive electrode active material for a non-aqueous electrolyte secondary battery as discussed above with respect to claim 2.
As discussed above, Soon teaches the embodiment as illustrated in Figure 1 in which the boron-containing compound is included in the coating layer on the surface of the secondary particles. Also discussed above, Soon teaches the coating layer on the surface of the secondary particles in order to reduce contact between the lithium manganese oxide positive electrode material and the electrolyte to mitigate side reactions.
Soon is silent as to the element B is absent inside the secondary particles and present only on the surfaces of the secondary particles. However, it is reasonable to presume that this feature is inherent to Soon. Support for said presumption is found in that the coating of the element B on the lithium metal oxide secondary particles taught by Soon is similar to that of the instant disclosure (fourth step). The instant disclosure provides that the composite oxide in the fourth step is mixed with a compound including the element B is added in powder or aqueous state and the mixture is heat treated in order to include the element B on the surface of the secondary particles (Paragraph 0050). The instant disclosure provides examples of the compound including the element B such as B2O3 and a temperature of the heat treatment is between 150ºC and 300ºC (Paragraph 0051).
In the method of forming the boron-containing coating layer on the secondary particles of Soon, the surface of the secondary (polycrystalline) particle precursor in step (i) is coated with a boron-containing compound by mixing and heat treat the polycrystalline manganese precursor and the boron precursor (Paragraph 0064). Soon teaches the polycrystalline material being comprised of two or more primary particles which agglomerate to form a secondary particle (Paragraphs 0074-0075). Soon teaches the boron compound such as B2O3 added by dissolving it in polar solvent (Paragraph 0068-0070). Soon teaches that when the boron-containing compound is uniformly coated on the surface of the secondary particle (polycrystalline material), it is possible to minimize friction between particles and provide good crystallinity (Paragraphs 0071-0072). Soon further teaches that the boron-containing compound is formed on the surface of the secondary particles by heat treatment at a temperature range of 120ºC and 300ºC Paragraph 0070).
Thus, Soon teaches in the method of coating the polycrystalline material with boron which the boron-containing compound is the same material (B2O3) applied in the same form (dissolved in polar solvent) and at an overlapping temperature range as the instant disclosure. Further, Soon teaches the coating applied to the secondary particles in the method which are formed by the agglomeration of a plurality of primary particles, in order to achieve the desired crystallinity and reduce friction between particles. Additionally, Soon teaches the coating layer as the exterior layer on the polycrystalline particles so as to reduce the side reactions between the positive electrode active material and the electrolyte. Therefore, the ordinary artisan would expect the coating layer of the polycrystalline material of Soon which modified Toma above to remain on the surface of the secondary particles, as the boron coating layer taught by Soon is applied to the aggregated secondary structure in a similar manner as the instant disclosure.
Regarding claim 4, modified Toma teaches a positive electrode active material for a non-aqueous electrolyte secondary battery as discussed above with respect to claim 1.
Toma does not explicitly teach the content of the element B is 1.2 mol% or less based on the total number of moles of Ni in the composite oxide.
As discussed above, absent unexpected results, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to optimize the coating thickness of boron on the secondary particles of positive electrode active material (and therefore the quantity of boron present on the surfaces of the secondary particles based on the total number of moles of Ni in the composite oxide) since it has been held that where general conditions of a claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. See MPEP 2144.05.
In the present invention one would have been motivated to optimize the thickness of the boron coating layer on the secondary polycrystalline particles to obtain a quantity of boron present on the surfaces of the secondary particles based on the total number of moles of Ni in the composite oxide to be within the claimed ranges in order to achieve a favorable balance between suppressing side reactions between positive electrode material and electrolyte while also minimizing electrochemical degradation and resistance, as recognized by Soon.
Regarding claim 5, modified Toma teaches a positive electrode active material for a non-aqueous electrolyte secondary battery as discussed above with respect to claim 1.
Toma does not explicitly teach a ratio of a content of the element B to a content of the element A is 0.05 or more and 200 or less.
However, as discussed above, As discussed above, absent unexpected results, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to optimize the coating thickness of boron on the secondary particles of positive electrode active material (and therefore the quantity of boron present on the surfaces of the secondary particles based on the total number of moles of Ni in the composite oxide) since it has been held that where general conditions of a claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. See MPEP 2144.05.
The ordinary artisan would recognize that by adjusting the thickness of the boron-containing coating layer on the polycrystalline secondary particles, the ratio of a content of the element B to the content of the element A would also be adjusted. In the present invention one would have been motivated to optimize the thickness of the boron coating layer on the secondary polycrystalline particles to obtain a ratio of a content of the element B to the content of the element A within the claimed ranges in order to achieve a favorable balance between suppressing side reactions between positive electrode material and electrolyte while also minimizing electrochemical degradation and resistance, as recognized by Soon.
Regarding claim 6, modified Toma teaches a positive electrode active material for a non-aqueous electrolyte secondary battery as discussed above with respect to claim 1.
Toma does not explicitly teach that the full width at half maximum n of a diffraction peak of a (208) plane in an X-ray diffraction pattern of the lithium-transition metal composite oxide is 0.30º< n < 0.55º.
It is reasonable to presume that the n of the diffraction peak of a (208) plane is inherent to Toma. Support for said presumption is found in that the lithium-transition metal composite oxide of Toma, as discussed above with respect to claim 1, comprises 80 mol% or more of Ni based on a total number of moles of metal elements excluding Li, a Co content of less than 5 mol% based on a total number of moles of metal elements excluding Li, and an element Ca present on the surfaces of the primary particles in an amount of 0.01 mol% or more and 1 mol% or less based on the total number of moles of the metal elements excluding Li. Further, Toma teaches the lithium composite oxide secondary particles formed by the aggregation of primary particles. The modification of Toma by Soon resulted in a coated layer of tungsten on the exterior of the secondary particles.
Further, Toma teaches in the process of forming the lithium transition metal composite oxide a mixing step wherein proportion of the precursor and the lithium compound is adjusted so that the ratio (Li/Me) of the sum (Me) of the metal atoms other than lithium to the number of atoms of lithium (Li) in the lithium mixture is 0.95 or more and 1.5 or less, preferably 1.0 or more and 1.2 or less, more preferably 1.0 or more and 1.1 or less. (Paragraph 0179). The instant application discloses the mixing ratio of the composite oxide obtained in the first step and the Li compound to be preferably within the range of 1:0.98 to 1:1.1 (Paragraph 0048). The mixing ratios of Toma overlap those of the instant application, suggesting inherent similarities in the process of forming the lithium metal composite oxide.
Toma teaches a calcination process which may be performed after the mixing process, which occurs between 1 and 10 hours in an oxidizing atmosphere (Paragraph 0202) at a temperature between 350 oC and 800oC in order to diffuse lithium into the precursor material and obtain uniform particles (Paragraph 0201). The instant application discloses the calcination of the mixture obtained in the second step which occurs in an oxygen atmosphere for 1 to 10 hours at a temperature of 450 oC and 850oC. The time, temperature, and oxygen presence in the calcination process of Toma overlap those of the instant application, suggesting inherent similarities in the process of forming the lithium metal composite oxide.
Toma modified by Soon teaches a lithium transition metal composite oxide having a layered structure and formed by the aggregation of primary particles to form secondary particles, and a coating on the surface of the secondary particles including boron
Further, Toma teaches a process of forming the layered primary particles including the mixing ratios and calcination step conditions which align with those of the instant application. It is therefore reasonable to presume that the crystallinity of the lithium metal composite oxide taught by Toma in view of Soon would result in an X-ray diffraction pattern where the full width at half max of the (208) plane is as claimed. Support for said presumption is also found in that Toma uses the same material for element A (calcium sulfate) (Paragraph 0110) to form an equivalent lithium metal composite oxide as the claimed invention.
Regarding claim 7, modified Toma teaches a nonaqueous electrolyte secondary battery comprising a positive electrode including the positive electrode active material according to claim 1, a negative electrode, and a non-aqueous electrolyte (Paragraph 0024).
Regarding claim 8, modified Toma teaches the positive electrode active material for a non-aqueous electrolyte secondary battery according to claim 1,
As discussed above in the rejection of claim 1, Toma teaches the composition of the shell portion of particle is represented by general formula (6): Li1+a2Ni1-x2-y2Cox2Mny2Mz2O2+β2 where -0.05 ≤ a2 ≤ 0.50, 0 < 1-x2-y2 ≤ 0.6, 0 ≤ z2 ≤ 0.05, and -0.5 ≤ β2 ≤ 0.5, (Paragraph 0020) where M was obviously selected as Ca from the from the finite lists of possible combinations for M to arrive at the lithium-transition metal oxide of the instant claim since the combination of components would have yielded predictable results as a surface coating for primary particles.
Further, when each element is set to the lower limit of the ranges taught by Toma, z2=0 and the presence of A (Ca) on the surface of the primary particles is 0%.
When each element is set to the upper limit of the ranges taught by Toma, the general formula is as follows: Li1.5Ni0.5999Co0.2Mn0.2M0.05O2.5and the mole percentage of element A on the surface of the primary particles with respect to total number of moles of metal elements excluding Li was calculated to be:
m
o
l
%
A
=
0.05
0.5999
+
0.2
+
0.2
+
0.05
=
4.8
%
The range of the mole percentage of element A on the surface of the primary particles with respect to total number of moles of metal elements excluding Li of Toma (0 to 4.8%) overlaps the claimed ranges of the percentage of element A on the surface of the primary particles with respect to total number of moles of metal elements excluding Li in the instant claim (0.1 to 0.8 mol %). Therefore, prima facie obviousness is established. See MPEP 2144.05 (I).
Regarding claim 10, modified Toma teaches the positive electrode active material for a non-aqueous electrolyte secondary battery according to claim 1.
Toma does not explicitly teach the content of the element B is 0.1 mol% or more and 1 mol% or less based on the total number of moles of Ni in the composite oxide.
As discussed above, absent unexpected results, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to optimize the coating thickness of boron on the secondary particles of positive electrode active material (and therefore the quantity of boron present on the surfaces of the secondary particles based on the total number of moles of Ni in the composite oxide) since it has been held that where general conditions of a claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. See MPEP 2144.05.
In the present invention one would have been motivated to optimize the thickness of the boron coating layer on the secondary polycrystalline particles to obtain a quantity of boron present on the surfaces of the secondary particles based on the total number of moles of Ni in the composite oxide to be within the claimed ranges in order to achieve a favorable balance between suppressing side reactions between positive electrode material and electrolyte while also minimizing electrochemical degradation and resistance, as recognized by Soon.
Regarding claim 12, modified Toma teaches the positive electrode active material for a non-aqueous electrolyte secondary battery according to claim 11.
As discussed above in the rejection of claim 1, Toma teaches the Formula (4) for the lithium-metal composite oxide represented by Li1+aNi1-x-yCoxMnyMzO2+β where -0.05 ≤ a ≤ 0.50, 0.02 ≤ x ≤ 0.30, 0.02 ≤ y ≤ 0.30, 0 ≤ z ≤ 0.05, and -0.5 ≤ β ≤ 0.5, where M is at least one element selected from the group consisting of Mg, Ca, Al, Si, Fe, Cr, V, Mo, W, Nb, Ti, and Zr (Paragraph 0020).
Further calculated in the rejection of claim 1 was the mole percentage of nickel based on the total number of moles of metal elements excluding Li. When each element in the formula of Toma was set to the lower limit of the ranges taught by Toma, the general formula is as follows: Li0.95Ni0.96Co0.02Mn0.02M0O1.5. Accordingly, the mole percentage of nickel with respect to total number of moles of metal elements excluding Li is:
m
o
l
%
N
i
=
0.96
0.96
+
0.02
+
0.02
=
96
%
When each element is set to the upper limit of the ranges taught by Toma, the general formula is as follows: Li1.5Ni0.40Co0.30Mn0.30M0.05O2.5. Accordingly, the mole percentage of nickel with respect to total number of moles of metal elements excluding Li is:
m
o
l
%
N
i
=
0.40
0.40
+
0.30
+
0.30
+
0.05
=
38
%
Thus, the range of mole percentage of Nickel in the lithium-transition metal composite oxide with respect to the total number of moles of metal elements excluding Li is represented by 38-96% as calculated above. The range of mole percentage of Ni of Toma substantially overlaps the claimed range of 90% or more in the instant claim. Therefore, prima facie obviousness is established. See MPEP 2144.05 (I).
The Formula (4) of Toma teaches Mn present in the lithium-metal composite oxide with subscript y, 0.02 ≤ y ≤ 0.30 and M with subscript z, 0 ≤ z ≤ 0.05. Further, it would have been obvious to a person having ordinary skill in the art prior to the effective filing date of the instant invention to select Al from the finite lists of possible combinations for M in the Formula for the metal oxide of Takahashi to arrive at the positive electrode active material of the instant claim since the combination of components would have yielded predictable results in a non-aqueous electrolyte secondary battery, absent a showing of unexpected results commensurate in scope with the claimed invention. See Section 2143 of the MPEP, rationales (A) and (E).
When each element in the formula of Toma was set to the lower limit of the ranges taught by Toma, the general formula is as follows: Li0.95Ni0.96Co0.02Mn0.02Al0O1.5. Accordingly, the mole percentage of Mn and Al with respect to total number of moles of metal elements excluding Li is:
m
o
l
%
M
n
+
A
l
=
0.02
+
0
0.96
+
0.02
+
0.02
=
2
%
When each element is set to the upper limit of the ranges taught by Toma, the general formula is as follows: Li1.5Ni0.40Co0.30Mn0.30Al0.05O2.5. Accordingly, the mole percentage of Mn and Al with respect to total number of moles of metal elements excluding Li is:
m
o
l
%
M
n
+
A
l
=
0.30
+
0.05
0.4
+
0.30
+
0.30
+
0.05
=
33
%
Thus, the range of mole percentage of Mn and Al in the lithium-transition metal composite oxide with respect to the total number of moles of metal elements excluding Li is represented by 2-33% as calculated above. The range of mole percentage of Mn and Al of Toma substantially overlaps the claimed range of 1 mol% to 5 mol% in the instant claim. Therefore, prima facie obviousness is established. See MPEP 2144.05 (I).
Regarding claim 13, modified Toma teaches the positive electrode active material for a non-aqueous electrolyte secondary battery according to claim 1, wherein the element B is B.
As discussed above in the rejection of claim 1, Toma in view of Soon teaches a coating layer comprising boron present on the surface of the secondary particles, meeting the instant claimed limitations.
Regarding claim 14, modified Toma teaches the positive electrode active material for a non-aqueous electrolyte secondary battery according to claim 1.
As discussed above, Toma teaches the composition of the shell portion of the particle including the element A, Ca. Because the element A is formed as a coating layer on the surface of the primary particles, it is considered to not form a solid solution with Ni, meeting the instant claimed limitations.
Regarding claim 15, Toma teaches the positive electrode active material for a non-aqueous electrolyte secondary battery according to claim 2.
As discussed above in the rejection of claim 1, Toma teaches the composition of the shell portion of particle is represented by general formula (6): Li1+a2Ni1-x2-y2Cox2Mny2Mz2O2+β2 where -0.05 ≤ a2 ≤ 0.50, 0 < 1-x2-y2 ≤ 0.6, 0 ≤ z2 ≤ 0.05, and -0.5 ≤ β2 ≤ 0.5, (Paragraph 0020) where M was obviously selected as Ca from the from the finite lists of possible combinations for M to arrive at the lithium-transition metal oxide of the instant claim since the combination of components would have yielded predictable results as a surface coating for primary particles.
Further, when each element is set to the lower limit of the ranges taught by Toma, z2=0 and the presence of A (Ca) on the surface of the primary particles is 0%.
When each element is set to the upper limit of the ranges taught by Toma, the general formula is as follows: Li1.5Ni0.5999Co0.2Mn0.2M0.05O2.5and the mole percentage of element A on the surface of the primary particles with respect to total number of moles of metal elements excluding Li was calculated to be:
m
o
l
%
A
=
0.05
0.5999
+
0.2
+
0.2
+
0.05
=
4.8
%
The range of the mole percentage of element A on the surface of the primary particles with respect to total number of moles of metal elements excluding Li of Toma (0 to 4.8%) overlaps the claimed ranges of the percentage of element A on the surface of the primary particles with respect to total number of moles of metal elements excluding Li in the instant claim (0.1 to 0.8 mol %). Therefore, prima facie obviousness is established. See MPEP 2144.05 (I).
Toma does not explicitly teach the content of the element B is 0.05 mol% or more and 1.2 mol% of less based on the total number of moles of Ni in the composite oxide, and wherein the ratio of the content of the element B to the content of the element A is 0.05 or more and 200 or less.
Toma does not explicitly teach the content of the element B is 0.1 mol% or more and 1 mol% or less based on the total number of moles of Ni in the composite oxide.
However, as discussed above, absent unexpected results, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to optimize the coating thickness of boron on the secondary particles of positive electrode active material (and therefore the quantity of boron present on the surfaces of the secondary particles based on the total number of moles of Ni in the composite oxide and the ratio of the element B to the element A) since it has been held that where general conditions of a claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. See MPEP 2144.05.
In the present invention one would have been motivated to optimize the thickness of the boron coating layer on the secondary polycrystalline particles to obtain a quantity of boron present on the surfaces of the secondary particles based on the total number of moles of Ni in the composite oxide as well as the ratio of the content of the element B to the content of the element A to be within the claimed ranges in order to achieve a favorable balance between suppressing side reactions between positive electrode material and electrolyte while also minimizing electrochemical degradation and resistance, as recognized by Soon.
Claim 6 is additionally rejected under 35 U.S.C. 103 as being unpatentable over Toma in view of Soon as applied to claims 1-8, 10, 12-15 above, further in view of Aoki (W.O. 2019131234 A1) (machine translation relied upon).
Further regarding claim 6, modified Toma teaches a positive electrode active material for a non-aqueous electrolyte secondary battery as discussed above with respect to claim 1.
Toma modified by Takahashi does not explicitly teach that the full width at half maximum n of a diffraction peak of a (208) plane in an X-ray diffraction pattern of the lithium-transition metal composite oxide is 0.30º< n < 0.55º.
Aoki discloses a lithium transition metal oxide for use in a positive electrode active material for a non-aqueous electrolyte secondary battery (Paragraph 0008). Aoki teaches the lithium transition metal oxide has a layered structure, wherein the ratio of Ni in the lithium transition metal oxide is 91 mol % to 99 mol % with respect to the total number of moles of metal elements excluding Li, a transition metal present in the layered structure from 1 mol % to 2.5 mol % relative to the total molar amount of the transition metal in the Ni-containing lithium transition metal oxide. Further, Aoki teaches that the X-ray diffraction pattern of this compound is characterized by a half-value width n of the diffraction peak of (208) plane to be 0.30° ≤ n ≤ 0.50° (Paragraph 0009). At these quantities, Aoki teaches the high capacity of the non-aqueous electrolyte secondary battery can be achieved as well as increase of the charge/discharge cycle characteristics (Paragraph 0011).
As discussed above with respect to claim 1, the lithium composite oxide of Toma modified by Takahashi contains a range of nickel with respect to the total number of moles of metal elements excluding Li calculated to be 38 to 96 mol%, which overlaps the range of Ni in the lithium transition metal oxide of Aoki. Further discussed in claim 1 is the presence of a transition metal (cobalt) present in the range of 2 to 29 mol% with respect to the total moles of metal elements excluding Li in the lithium metal composite oxide, which overlaps the molar percentage range of the transition metal of Aoki. Toma also teaches the core and shell portion of the primary particles which make up a layered structure of the lithium metal composite oxide. Thus, these similarities suggest that the lithium composite oxide of Toma modified by Takahashi is open to modification of Aoki.
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the X-ray diffraction pattern of the lithium metal composite oxide of Toma modified by Takahashi to incorporate the teachings of Aoki in which the half-value width n of the diffraction peak of (208) plane to be 0.30° ≤ n ≤ 0.50°. Doing so would result in the suppression of the decrease of the charge/discharge cycle characteristics, as recognized by Aoki.
Claim 9 is rejected under 35 U.S.C. 103 as being unpatentable over Toma in view of Soon as applied to claims 1-8, 10, 12-15 above, further of Kim (U.S. Patent Publication No. 20170358796 A1).
Regarding claim 9, Toma teaches the positive electrode active material for a non-aqueous electrolyte secondary battery according to claim 1.
As discussed above in the rejection of claim 1, Toma teaches the composition of the shell portion of the positive electrode material particles includes calcium (when M=Ca, as set forth in the obviousness rejection above).
Toma is silent as to the element A present on the surface of the primary particles is present as Sr.
However, Kim discloses a positive active material for a lithium ion secondary battery (Paragraph 0001). Kim teaches the positive electrode active material particles made of a lithium metal oxide composition (Formula 1) including metals such as nickel and cobalt in addition to lithium and oxygen (Paragraphs 00038-0039). Kim teaches the lithium metal oxide represented by Formula 1 may be in the form of secondary particles resulting from the agglomeration of primary particles (Paragraph 0042). Thus, Kim teaches a positive electrode active material which shares a similar structure and composition as that of the instant disclosure.
Further, Kim teaches a lithium-containing compound of Formula 2 in the form of a layer which may be disposed on the surface of the primary particles (Paragraph 0042). Kim teaches Formula 2 of the form Li2-xM’O3-y, where M’ is at least one element selected from Mg, Al, Ca, Ti, V, Cr, Fe, Cu, Zn, Ga, Sr, Y, Zr, Nb, Mo, Ru, and F; 0≦x≦1; and 0≦y≦3. As discussed above, Toma teaches the general formula 6 to represent the shell portion of the positive electrode material, comprising lithium, nickel, cobalt, manganese, oxygen, and at least one element selected from Mg, Ca, Al, Si, Fe, Cr, V, Mo, W, Nb, Ti, and Zr. Thus, Kim teaches a coating for the secondary particles of positive electrode active material which shares a similar structure and composition as that of the instant disclosure.
Therefore, given the general teachings of Kim it would have been obvious to one of ordinary skill in the pertinent art before the effective filing date of the claimed invention to substitute strontium in the primary particle coating of Kim for calcium in the shell portion of Toma, because Kim teaches the coating for the primary particles may suitably be selected as strontium or calcium. The substitution would have been one known element for another and one of ordinary skill in the pertinent art would reasonably expect the predictable result that the modified composition would be useful as a coating/shell for the primary particles of Toma and possess the benefits of improved battery performance, initial efficiency, and rate and lifetime characteristics taught by Kim (Paragraph 0014). See MPEP § 2143.I.(B).
Claim 11 is rejected under 35 U.S.C. 103 as being unpatentable over Toma in view of Soon as applied to claims 1-8, 10, 12-15 above, further in view of Li (Non-Patent Literature, “Is Cobalt Needed in Ni-Rich Positive Electrode Materials for Lithium Ion Batteries?”).
Regarding claim 11, modified Toma teaches the positive electrode active material for a non-aqueous electrolyte secondary battery according to claim 1.
Modified Toma does not teach the lithium-transition metal composite oxide is free of Co and contains Mn and Al.
However, Li discloses that NCA materials with formula LiNi1-x-yCoxAlyO2 widely used in the electric vehicle industry are traditionally believed to have enhanced properties due to cobalt and aluminum in these materials. Li studies the roles of different cation substituents in materials represented by LiNi1-nMnO2, where M=Al, Mn, Mg, or Co. Li teaches that cobalt brings little or no value at all to NCA-type materials with high nickel content (> 90% Ni), with materials such as LiNi0.95M0.05O2 (M= Al, Mn, or Mg) performing superior to NCA materials with 5% cobalt content (Abstract). Li also teaches the high price of cobalt as motivation for finding alternative NCA materials with minimal cobalt (Page A429, Column 1, Paragraph 1).
In particular, Li finds that Co content up to 5% does not effectively suppress phase transitions during charge and discharge, while 5% Mn, 5% Mg, and 5% Al materials represented by LiNi1-nMnO2, where M=Al, Mn, or Mg showed an effective suppression of phase transitions (Page A431, Column 2, Paragraph 3). Further, Li teaches that Co included in electrode active materials does not contribute to structural stabilization (Page A435, Column 2, Paragraph 2) or thermal stability (Page A436, Column 2, Paragraph 2) while cation substitution with Mn, Al, or Mg were able to lower the reactivity of the positive electrode material with the electrolyte (Page A436, Column 2, Paragraph 2).
As discussed above, Toma teaches the Formula (4) for the lithium-metal composite oxide represented by Li1+aNi1-x-yCoxMnyMzO2+β. The material for the positive electrode active material of Toma may be considered high nickel content according to Li, as the mole percentage of nickel in the lithium-transition metal composite oxide was calculated to be 38-96%, overlapping the > 90% nickel content set forth by Li.
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the lithium-metal composite oxide of Toma to incorporate the teachings of Li in which the cobalt is removed and replaced with substituted cations Al or Mn. As seen in the Formula 4 of Toma, the addition of Mn cations to replace Co in the formula would increase the subscript of Mn, (y), while the addition of Al cations would necessitate the ordinary artisan selecting Al from the finite list of possible combinations for the placeholder element M in the formula (4) of Toma and increasing the subscript of M, (z). Doing so would advantageously remove the expensive cobalt in the positive electrode active material without negatively impacting and even providing superior suppression of phase transitions, structural and thermal stability, and lower reactivity of the positive electrode material with the electrolyte, as recognized by Li.
Response to Arguments
Response to Arguments: 35 USC § 103
Applicant argues in the remarks filed February 20th, 2026 that Toma in view of Takahashi does not provide for all the aspects of the claims, nor is there any rationale prompting a skilled artisan to modifying the combination so as to derive the current invention. Applicant notes that the relied upon disclosure of Takahashi is directed toward a tungsten-concentration layer on the positive electrode active material. As amended, tungsten is no longer listed on the suitable candidates for the element B of the instant disclosure.
Applicant's arguments have been fully considered and are persuasive.
In response to applicant’s arguments, the Examiner presents that the amended claim limitations with a narrower scope for the element B necessitated a new grounds of rejection presents above in view of Toma and Soon.
On page 9 of the Remarks filed September 2nd, 2025, applicant argues that regarding claims 6and 11, they are dependent on claim 1 and therefore should be allowable at least for the reasons presented above regarding claim 1.
Applicant's arguments have been fully considered but they are not persuasive for at least the reasons presented above with respect to the arguments regarding claim 1.
Cited Art Not Relied Upon
Baek (W.O. 2019088806 A1) discloses a lithium transition metal composite oxide for use as a positive electrode material in a lithium secondary battery (Paragraph 4), the lithium metal composite oxide comprising a coating layer which may include elements including strontium (Paragraph 45). More specifically, Baek teaches the presence of strontium in the form of strontium oxide on the surface of the lithium metal composite oxide particles to assist in the capture and decomposition of HF formed by the reaction with the electrolyte (Paragraph 69).
Conclusion
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/O.A.J./Examiner, Art Unit 1789
/MARLA D MCCONNELL/Supervisory Patent Examiner, Art Unit 1789
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