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 .
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(b):
(b) CONCLUSION.—The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the inventor or a joint inventor regards as the invention.
The following is a quotation of 35 U.S.C. 112 (pre-AIA ), second paragraph:
The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the applicant regards as his invention.
Claim 4 is rejected under 35 U.S.C. 112(b) as being indefinite for failing to particularly point out and distinctly claim the subject matter which the inventor regards as the invention.
Claim 4 depends from claim 2 and recites that the lithium-transition metal composite oxide has a composition represented by formula (3): (1−x)LiM1₁₋zM2zO₂+xLi₂MnO₃. Parent claim 2 requires that the same lithium-transition metal composite oxide have a composition represented by formula (1): Li₁₊ₓM1₁₋zM2zO₂₊β. Formula (1) describes a single-phase layered lithium-transition metal oxide, whereas formula (3) describes a two-component lithium-rich composite of a LiM1₁₋zM2zO₂ component and a Li₂MnO₃ component. It is unclear whether, and how, a single composition can simultaneously satisfy both formula (1) as required by claim 2 and formula (3) as recited in claim 4; accordingly, the bounds of claim 4 cannot be determined.
Furthermore, the variables “x” and “z” appear in both formula (1) of claim 2 and formula (3) of claim 4, but formula (3) recites no numerical ranges for “x” and “z,” while claim 2 requires 0.02 < x < 0.07 and 0.0005 ≤ z < 0.1. In formula (1), “x” represents the amount of lithium in excess of the transition metal, whereas in formula (3), “x” represents the molar fraction of the Li₂MnO₃ component; likewise, “z” in formula (3) represents the substitution level within the LiM1₁₋zM2zO₂ component only, rather than relative to the entire composite. It is therefore unclear whether the ranges recited in claim 2 for “x” and “z” apply to the differently-defined “x” and “z” of formula (3) in claim 4. For at least these reasons, claim 4 is indefinite.
Claim Rejections - 35 USC § 102
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 the appropriate paragraphs of 35 U.S.C. 102 that form the basis for the rejections under this section made in this Office action:
A person shall be entitled to a patent unless –
(a)(1) the claimed invention was patented, described in a printed publication, or in public use, on sale, or otherwise available to the public before the effective filing date of the claimed invention.
(a)(2) the claimed invention was described in a patent issued under section 151, or in an application for patent published or deemed published under section 122(b), in which the patent or application, as the case may be, names another inventor and was effectively filed before the effective filing date of the claimed invention.
Claims 1, 2, 3, 6, and 7 are rejected under 35 U.S.C. 102(a)(1) as being anticipated by Baek et al. (US 11,437,609 B2).
Claim 1: Baek discloses a positive electrode active material for a secondary battery (Abstract) comprising a lithium-transition metal composite oxide. Baek forms the material by mixing a lithium compound, a transition metal precursor, and a tungsten doping source such as tungsten trioxide (WO₃), and sintering the mixture, whereby “the inside and surface of the lithium transition metal oxide may be stably doped with the tungsten doping source” (col. 4, lines 40–50). In Example 1, the transition metal precursor is Ni₀.₉₀Co₀.₀₇Mn₀.₀₃(OH)₂, the lithium compound (LiOH) and the precursor are mixed in a molar ratio of 1.03:1, WO₃ is added, and the mixture is sintered at 760°C (Col. 11-12). The tungsten-doped oxide is then washed with distilled water only — 150 g of the oxide in 300 mL of water — filtered, dried, and heat-treated (col. 12, lines 10–40, incorporating the washing of col. 11, ll. 39–56).
As to the limitation that 90 atomic % or more of the metals other than lithium is an element M1 selected from Ni, Co, Mn, and Al: the nickel, cobalt, and manganese of the Comparative Example 1 oxide are each an element M1. As to the limitation that 0.05 atomic % or more and 1 atomic % or less of the metals other than lithium is tungsten: the tungsten content of the Comparative Example 1 material is 1600 ppm by mass (Table 1), which corresponds to approximately 0.085 atomic % relative to the total metals other than lithium. The metals other than lithium therefore consist of approximately 99.9 atomic % M1 (Ni + Co + Mn) and approximately 0.085 atomic % tungsten, satisfying both the “90 at.% or more” M1 limitation and the “0.05 at.% or more and 1 at.% or less” tungsten limitation. The reference’s worked Example 2, prepared with the same Ni₀.₉₀Co₀.₀₇Mn₀.₀₃ transition-metal composition, likewise possesses a tungsten content within the claimed range (1700 ppm by mass; Table 1), confirming that the recited composition and tungsten content are disclosed by a worked, non-comparative example. Comparative Example 1 is relied upon herein specifically for its washing with water alone, which produces the surface-depleted structure addressed below.
As to the ratio W2/W1 = α of the surface tungsten content to the whole tungsten content being 0 < α < 0.1: Baek teaches that upon washing the tungsten-doped oxide with the washing liquid, “tungstate anions (e.g., WO₄²⁻) are lost from the tungsten-doped lithium transition metal oxide while being ionized by the washing liquid” (col. 4, line 65 – col. 5, line 2), i.e., the washing removes tungsten from the surface of the oxide while the tungsten doped into the interior remains (col. 4, lines 40–50). The Comparative Example 1 material is thus prepared by a process — bulk mixing of a tungsten source with the transition metal precursor and the lithium compound, sintering, and washing with water — that is substantially identical to the process disclosed by this application for producing a material having 0 < α < 0.1 (specification, [0049]). Moreover, the washing of Comparative Example 1 employs 150 g of oxide in 300 mL of water, i.e., 500 g/L, which is a greater quantity of water per unit mass of oxide than the washed examples of the present application (750 g/L to 1750 g/L; Table 1), which examples yield α of 0.025 to 0.039. Because a greater quantity of wash water per unit mass removes more surface tungsten, the Comparative Example 1 material necessarily possesses α below the values of the applicant’s washed examples and thus within the claimed range of 0 < α < 0.1.
Where the prior art product is made by a process substantially identical to that used by applicant, and where the reference expressly teaches that the washing removes tungsten from the surface, the claimed ratio 0 < α < 0.1 is necessarily present in the prior art product (MPEP 2112.01).
Claim 2: Baek discloses the lithium-transition metal composite oxide of claim 1 having a composition within formula (1), Li₁₊ₓM1₁₋zM2zO₂₊β, wherein M2 includes at least tungsten. In Comparative Example 1, the lithium compound and the transition metal precursor are combined in a molar ratio of 1.03:1 (Example 1), such that the excess-lithium parameter x is approximately 0.03, satisfying 0.02 < x < 0.07. The tungsten (M2) content of approximately 0.085 at.% relative to the metals other than lithium corresponds to a subscript z of approximately 0.00085, satisfying 0.0005 ≤ z < 0.1. The oxide is a layered lithium-nickel composite oxide of substantially stoichiometric oxygen content, such that β is within −0.02 ≤ β ≤ 0.04.
Claim 3: Baek discloses the composition of claim 2 within formula (2), Li₁₊ₓNiᵧM3₁₋ᵧ₋zM2zO₂₊β, wherein M3 is selected from Co, Mn, and Al. In Comparative Example 1, the transition metal precursor is Ni₀.₉₀Co₀.₀₇Mn₀.₀₃(OH)₂ (col. 11, lines 28–56), such that the nickel fraction y is 0.90 and M3 is cobalt and manganese, satisfying 0.7 < y < 0.95.
Claim 6: Baek discloses a secondary battery comprising the positive electrode active material of claim 1. In the Preparation Example (col. 12, line 47 – col. 13, line 8), the positive electrode active material of Comparative Example 1 is formed into a positive electrode on an aluminum current collector, lithium metal is used as a negative electrode facing the positive electrode, a porous polyethylene separator is interposed between the positive electrode and the negative electrode, and a nonaqueous electrolyte of 1.0M LiPF₆ in ethylene carbonate/dimethyl carbonate/ethylmethyl carbonate is provided (col. 12, line 55 - col. 13, line 8).
Claim 7: Baek discloses the secondary battery of claim 6 as set forth above. In the Preparation Example, lithium metal is used as the negative electrode (col. 12, lines 55–65). Lithium metal contains no tungsten; accordingly, the amount Wn of tungsten in the negative electrode is zero, and the ratio Wn/Wp of the amount of tungsten in the negative electrode to the amount of tungsten in the positive electrode per unit facing area is zero, which is within the recited range of 0 ≤ Wn/Wp < 0.07.
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.
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.
This application currently names joint inventors. In considering patentability of the claims the examiner presumes that the subject matter of the various claims was commonly owned as of the effective filing date of the claimed invention(s) absent any evidence to the contrary. Applicant is advised of the obligation under 37 CFR 1.56 to point out the inventor and effective filing dates of each claim that was not commonly owned as of the effective filing date of the later invention in order for the examiner to consider the applicability of 35 U.S.C. 102(b)(2)(C) for any potential 35 U.S.C. 102(a)(2) prior art against the later invention.
Claim 4 is rejected under 35 U.S.C. 103 as being unpatentable over Baek in view of Kang et al. (US 2005/0058588 A1). This rejection is made to the extent claim 4 can be understood in light of the indefiniteness set forth above.
Claim 4: Baek discloses the positive electrode active material of claims 1 and 2 as set forth above, including the tungsten-doped, water-washed lithium-transition metal composite oxide in which 0 < α < 0.1, the tungsten content is 0.05 at.% or more and 1 at.% or less, x is approximately 0.03, and z is approximately 0.00085. Baek does not disclose that the composite oxide has a composition represented by formula (3), (1−x)LiM11-zM2zO2+xLi₂MnO₃, i.e., a lithium-rich composite containing a Li₂MnO₃ component.
Kang, directed to layered lithium nickel-manganese oxide cathode materials for lithium secondary batteries, discloses lithium-excess compositions such as Li[Li₀.₂Ni₀.₁₅Co₀.₁Mn₀.₅₅]O₂ ([0046]; FIG. 4), in which the lithium in excess of the transition metals occupies transition-metal sites in the form of a Li₂MnO₃ component. Kang teaches that such lithium-excess compositions exhibit X-ray diffraction peaks at 2θ of 20–25° attributable to cation ordering in the transition-metal layer ([0046]; FIG. 4), and that increasing the lithium content in this manner increases the discharge capacity by more than 10% while improving cycling performance ([0047]). A lithium-excess layered oxide of this type, in which excess lithium and manganese occupy the transition-metal layer in the ordered arrangement giving rise to the 20–25° superlattice reflections, is compositionally equivalent to, and is conventionally represented as, a two-component composite (1−x)LiM1₁₋zM2zO₂+xLi₂MnO₃, the ordered lithium-and-manganese domains constituting the Li₂MnO₃ component of that representation. Such a lithium-excess composition of nickel, cobalt, and manganese corresponds to the composite (1−x)LiM11-zM2zO2+xLi₂MnO₃ of formula (3), wherein M1 is Ni, Co, and Mn.
Baek teaches that the transition metal of the lithium transition metal oxide may include manganese (col. 3, ll. 57–66), and Kang teaches that forming the layered lithium nickel-manganese oxide as a lithium-excess composition containing a Li₂MnO₃ component increases the discharge capacity by more than 10% and improves cycling performance ([0047]). Accordingly, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to form the tungsten-doped, water-washed lithium-transition metal composite oxide as a lithium-rich composite comprising a Li₂MnO₃ component, in order to increase the discharge capacity and improve the cycling performance. The resulting composite oxide has a composition represented by formula (3).
Claim 5 is rejected under 35 U.S.C. 103 as being unpatentable over Baek in view of Kondo et al. (US 10,784,500 B2).
Claim 5: Baek discloses the positive electrode active material of claim 1 as set forth above. The Comparative Example 1 material of Baek contains cobalt in an amount of about 7 at.% of the metals other than lithium (Ni₀.₉₀Co₀.₀₇Mn₀.₀₃; Example 1) and thus does not contain substantially no cobalt. Baek does not disclose a material containing substantially no cobalt.
Kondo, directed to the same field of tungsten-bearing, water-washed lithium-nickel composite oxides for nonaqueous electrolyte secondary batteries, discloses a base material represented by Liz₃Ni₁₋ₓ₃₋ᵧ₃Coₓ₃M1ᵧ₃O₂, wherein 0.00 ≤ x3 ≤ 0.35 and M1 is at least one of Mn, V, Mg, Mo, Nb, Ti, and Al (col. 13, lines 32–40;), such that cobalt (x3) may be entirely absent and the composite oxide may be cobalt-free. Baek further teaches that lithium-cobalt oxide is expensive and cost-limited owing to the resource limitations of cobalt, and that nickel is cheaper than cobalt (col. 1, lines 40-54).
Accordingly, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the claimed invention to form the tungsten-doped, water-washed high-nickel composite oxide with a cobalt-free composition, in order to reduce the raw-material cost. The resulting positive electrode active material contains substantially no cobalt.
Conclusion
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/ATEF A SHAT/Examiner, Art Unit 1712
/MICHAEL B CLEVELAND/Supervisory Patent Examiner, Art Unit 1712
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