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 .
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and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114.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 02/19/26 has been entered.
Status of Claims
Applicant’s amendment and arguments, filed 02/19/26, have been fully considered. Claim(s) 1 is/are amended; claim(s) 2, 5, and 8–10 stand(s) as originally or previously presented; and claim(s) 3 and 4 is/are canceled; no new matter has been added. Examiner affirms that the original disclosure provides adequate support for the amendment.
Upon considering said amendment and arguments, the previous 35 U.S.C. 103 rejection has been maintained and altered as necessitated by Applicant’s amendment.
Specification
The specification is objected to because of the following informalities: because it has been established that the specification provides sufficient antecedent basis for “{(a1+a2)/2}/b1” as instant Eq. 1, Table 2’s headers of “a1+a2” and “(a1+a2)/b1” should be replaced by “(a1+a2)/2” and “{(a1+a2)/2}/b1”, respectively.
Claim Interpretation
Claim 1 recites “1.4≤{(a1+a2)/2}/b1≤2.502 … a1 is the average content … in the region of 0 to 0.05r … [and] a2 is the average content … in the region of 0.95r to r”. Examiner notes that because claim 1’s r is a primary particle’s short-axis diameter, the region of 0–0.05r would reasonably constitute the same distance as and correspond to the region of 0.95r to r. Thus, Examiner understands the above relation to be a ratio of the average molar content of Ti in the particle “shell”—i.e., average of 0–0.05r and 0.95r to r ({a1+a2}/2)—to an average molar content of Ti in the particle “core”—i.e., b1 of 0.05–0.95r.
Claim Rejections - 35 USC § 103
The text forming the basis for the rejection under 35 U.S.C. 103 may be found in a prior Office Action.
Claim(s) 1, 2, 5, and 6 is/are rejected under 35 U.S.C. 103 as being unpatentable over Toyama et al. (WO 2020195790 A1; citations to English equivalent US 20220115656 A1) (Toyama).
Regarding claim 1, Toyama discloses a positive electrode active material comprising a lithium composite oxide containing at least nickel and titanium (e.g., Abstract and Ex. 5 in Table 1), wherein the lithium composite oxide is secondary particles in which a plurality of primary particles are agglomerated (Abstract).
Toyama further discloses a Ti-based surface layer atop each primary particle (see D1, which represents the surface vicinity of each primary particle, in FIGS. 3–6; see also ¶ 0043, where X element is preferably Ti). As D1 is 1 nm from the surface and the primary particles’ average diameter is at least 50 nm (¶ 0048), such would correlate with the instant a1 and a2 as the “shell” (as 1 nm/50 nm = 0.02r). Similarly, the Ti is also inside the primary particle’s central part as D2 (e.g., ¶ 0052), which is ≥ 0.2r from the surface (¶ 0163) and, thus, correlates with the instant b1 as the “core”. Toyama discloses that D1 and D2 are average values calculated via EDX line analysis (¶ 0162, 0164, FIGS. 3–6) in a manner appearing substantially similar to the instant disclosure’s EDX analysis (e.g., FIGS. 1–9), where D1 is, e.g., 1.87x D2 (based on D1 of 2.8 and D2 of 1.5 in Ex. 5, ¶ 0165 and FIG. 5).
Although Toyama fails to explicitly disclose the 1.87x Ti relation as an average Ti value based on the instant (a1+a2)/2—as well as the explicit 0–0.05r (a1), 0.05–0.95r (b1), and 0.95r to r (a2) regions based on the primary particle’s short-axis diameter from the TEM/EDX—and, thus, a value explicitly falling within the recited 1.4≤{(a1+a2)/2}/b1≤2.502, Toyama’s 1.87x, in being measured with a technique and at distances substantially similar to the instant disclosure, appears to correlate with, encompass, or at least approach the instant range, absent evidence otherwise. Considering that Toyama is analogous prior art to the claimed invention because they pertain to the same field of endeavor, namely Ti-doped lithium nickel oxide positive electrode material, it would have been obvious to one ordinarily skilled in the art, before the claimed invention’s effective filing date, to routinely select within the apparent overlap/encompassing range with a reasonable expectation of employing a successful, Ti-coated lithium complex oxide (MPEP 2144.05 (I)).
Assuming, arguendo, that such failed to render obvious instant Eq. 1 by Toyama’s not disclosing D1 as an average content, Examiner provides linear-interpolation calculations below (assuming linear decrease) from Toyama’s D0, D1, and D2 from Ex. 5 (Table 1), which appear to account for the “average” content—and, thus, correlate to a1 or a2—in Toyama’s concentrated region within 3 nm from surface (where D2 is then taken as ~ b1 as being in the core, and at% would necessarily yield the same ratio as mol% because mol% is merely scaled by Avogadro’s number):
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Accordingly, even if this ~ 2.6 narrowly fails to encompass or overlap the recited 1.4–2.502, a prima facie case of obviousness exists where the claimed ranges and prior art ranges fail to overlap but are close enough that one skilled in the art would have expected them to have the same properties (see MPEP 2144.05 (I)). Because Toyama discloses the recited material, whose Ti concentration is measured substantially similarly to the instant disclosure, along with a substantially similar preparation method and mixing ratios (mixing lithium precursor, Ni/Co/Mn precursors, and TiO2, followed by multiple heating and calcination treatments) as the instant specification (e.g., p. 25, lines 14–25), the skilled artisan would have reasonably expected the disclosed and recited materials to exhibit the same properties (MPEP 2112.01 (I)).
More specifically, Toyama only includes comparative examples with, at most, D1 and D2 and, thus, appears to omit a “true” comparative example demonstrating poorer performance from a set of values (i.e., D0, D1, and D2) allowing the instant Eq. 1 to be approximated. Further, it is unclear that Eq. 1 is critical based on instant Table 2 based on below factors. Thus, absent demonstrated criticality, the recited 1.4–2.502 appears obvious over Toyama.
More importantly, however, Toyama generally discloses that D0 > D1 but preferably < 10x D1 (¶ 0058), and D1 is preferably 1.5–20x D2 (¶ 0056). When D0 > D1, the primary particle’s surface is physically protected to prevent crystal-structure deterioration from electrolyte permeation, yielding favorable (dis)charge characteristics, and when D0 < 10x D1, there is no increased resistance due to a layer containing the X element at the primary-particle interface, making it possible to obtain favorable rate characteristics (¶ 0058). Further, when D1 is 1.5x or more, the X element such as Ti is sufficiently concentrated in the vicinity of the surface to stabilize the material’s crystal structure, which improves cycle characteristics (¶ 0056). When the ratio is too large, large concentration differences exist between the vicinity of the surface and the central part of the primary particle, yielding uneven Li+ (de)intercalation and a concern that discharge capacity may diminish or that rate characteristics may deteriorate (¶ 0056). To balance all these effects, then, the skilled artisan would have readily envisaged controlling the Ti contents throughout the gradient, so it would have been obvious to arrive at the recited range by routinely optimizing the Ti content within each of D0, D1, and D2 (i.e., at surface and within core) and, thus, necessarily controlling each of a1, a2, and b1’s average values and, by extension, the ratio {(a1+a2)/2}/b1 (MPEP 2144.05 (II)).
Regarding the limitations the 1) “average of the average content (mol%) of titanium measured based on all metal elements excluding lithium in the region of 0 to 0.05r from the start point of the line sum spectrum and the average content (mol%) of titanium measured based on all metal elements excluding lithium in the region of 0.95r to r is more than 0.227 mol% and less than 2.699 mol%”, and 2) “wherein the average content (mol%) of titanium measured based on all metal elements excluding lithium in the region of 0.05r to 0.95r from the start point of the line sum spectrum is greater than 0.083 mol% and less than 0.832 mol%”, such represent (a1+a2)/2 and b1, respectively (per claim 1’s definitions of a1, a2, and b1). According to the above rationale, then, based on Toyama’s broader disclosure of D0 > D1 > D2—and the notion that the skilled artisan would have readily understood to control the Ti content at each portion of the gradient—it would have been obvious to arrive at the respectively recited ranges of (a1+a2)/2 and b1 by routinely optimizing the surface and core Ti contents (MPEP 2144.05 (II)).
Regarding claim 2, Toyama discloses the positive electrode active material of claim 1, wherein titanium in the lithium composite oxide is present in an amount in an amount of 2 mol% based on all metal elements excluding lithium (Ex. 5, Table 1), falling within greater than 0.2 mol% and less than 3.3 mol%.
Regarding claim 5, Toyama discloses the positive electrode active material of claim 1, wherein the lithium composite oxide further comprises Co and Mn (Ex. 5, Table 1).
Regarding claim 6, Toyama discloses the positive electrode active material of claim 1.
Toyama further exemplarily discloses a Li:Ni:Co:Mn:Ti ratio of 1.02:0.90:0.03:0.05:0.02 (Ex. 5, Table 1) but, in failing to explicitly articulate the O content, fails to explicitly disclose the recited
Chemical Formula 1.
More generally, though, Toyama discloses a formula of Li1+aNibCocMdXeO2+α, where, based on Ex. 5, M is Mn, and X is Ti (¶ 0027). Further, a is preferably -0.02–0.02 because this range suppresses cation mixing to obtain high discharge capacity (¶ 0033, 0034); b is 0.85–0.95 because this range increases discharge capacity while reducing crystal-structure distortion (¶ 0037); c is 0–0.2 because this range stabilizes the crystal structure without reducing costs (¶ 0038); d is 0–0.2 because this range provides favorable rate characteristics without decreasing discharge capacity (¶ 0041); e is 0–0.08 because this range stabilizes the crystal structure in the surface’s vicinity without reducing discharge capacity (¶ 0044); and α is greater than -0.2 and less than 0.2 because this range provides high discharge capacity alongside an appropriate crystal structure (¶ 0046). To balance all these effects, then, it would have been obvious to arrive at the recited formula by routinely optimizing the molar ratios in the lithium composite oxide’s composition (MPEP 2144.05 (II)).
Claim(s) 7–10 is/are rejected under 35 U.S.C. 103 as being unpatentable over Toyama et al. (WO 2020195790 A1; citations to English equivalent US 20220115656 A1) (Toyama), as applied to claim 1, in view of Nakamura et al. (EP 3690999 A1) (Nakamura).
Regarding claims 7 and 8, Toyama discloses the positive electrode active material of claim 1, wherein the primary particle is a core-shell particle comprising a core and a shell present on at least a portion of a surface of the core (central part plus surface layer, FIG. 3b and, e.g., ¶ 0043).
Toyama further discloses that the X element, i.e., Ti, reacts with Li to form the concentrated surface layer (¶ 0043) but fails to explicitly disclose the surface layer’s composition and, thus, a metal oxide of Chemical Formula 2 in the shell.
Nakamura, in teaching a lithium metal oxide coated and solid-solved with Ti (Abstract), teaches a lithium titanium compound of, e.g., LiTiO3 for improved electron conductivity (¶ 0013, 0054).
Nakamura is analogous prior art to the claimed invention because they pertain to the same field of endeavor, namely Ti-coated positive electrode active material.
It would have been obvious to one of ordinary skill in the art, before the claimed invention's effective filing date, that Toyama's Li- and Ti-based surface layer must necessarily be incorporated as some compound, and, as demonstrated by Nakamura, the skilled artisan would find it obvious to employ LiTiO3 for improved electron conductivity.
Thus, modified Toyama would disclose a metal oxide of Chemical Formula 2 in the shell, where a = b = 1, c = 0, d = 3, and M3 is absent because c = 0 (Nakamura’s LiTiO3), which further reads on claim 8’s lithium titanium oxide’s being present in the shell.
Regarding claims 9 and 10, modified Toyama discloses a lithium secondary battery using a positive electrode comprising the positive electrode active material according to claim 8 (Toyama, e.g., Abstract, ¶ 0118 and Ex. 5).
Response to Arguments
Applicant’s arguments with respect to claim 1 have been fully considered but are unpersuasive.
Applicant argues that Toyama’s examples fail to satisfy Eq. 1. Examiner notes that, using Applicant’s linear interpolation method, Toyama’s Ex. 5 appears to yield a value of Eq. 1 of ~ 2.6 (see claim 1’s calculations), which is very close to 2.502. Absent demonstrated criticality, then, to 2.502, the skilled artisan would have expected substantially similar performance from Toyama’s material, as corroborated at least by Toyama’s Ex. 5’s capacity-retention rate of 94% (Table 1) compared to Applicant’s rate of 92~93.5% (Table 3; see MPEP 2144.05 (I) and further explanation of Toyama’s comp. exs. above).
Applicant further argues that Toyama’s examples fail to simultaneously satisfy Eq. 1 alongside “the average of the average content (mol%) of titanium measured based on all metal elements excluding lithium in the region of 0 to 0.05r from the start point of the line sum spectrum and the average content (mol%) of titanium measured based on all metal elements excluding lithium in the region of 0.95r to r is more than 0.227 mol% and less than 2.699 mol%”, and 2) “wherein the average content (mol%) of titanium measured based on all metal elements excluding lithium in the region of 0.05r to 0.95r from the start point of the line sum spectrum is greater than 0.083 mol% and less than 0.832 mol%”, asserting that Toyama’s broader D0 > D1 > D2, with their respective ratios, are only relative and, thus, cannot disclose (absolute) values outside Toyama’s exs.
Examiner respectfully disagrees because Toyama’s exs. are preferred embodiments, whereas Toyama more broadly allows D0 > D1 but preferably < 10x D1 (¶ 0058), and D1 is preferably 1.5–20x D2 (¶ 0056). As Toyama’s examples do not discredit/discourage the broader values, the skilled artisan reasonably would have considered Toyama’s more general D0 > D1 > D2 when determining the suitable surface and core Ti contents when balancing the considerations discussed above (see MPEP 2123). Further, as explained above, the skilled artisan would have readily envisaged controlling the Ti content throughout the gradient to account for the above factors and, thus, would have routinely arrived at the instant ranges.
Examiner also respectfully reiterates that Toyama recognizes a D1 of 1.5–20x D2 as important for balancing suitable Li+ (de)intercalation and stable crystal structures for suitable (dis)charge cycling (¶ 0056), which seems to be a similar effect as the instant disclosure (i.e., combined doping and coating for improved (dis)charge cycling and output efficiency), meaning that the improved cycling appears expected (see MPEP 716.02(c)). Specifically, instant Comp. Exs. 3, 4, 9, and 10, in exhibiting an {(a1+a2)/2}/b1 < 1.4 and displaying lower (dis)charge capacities, reasonably appear expected based on Toyama’s disclosure that D1 should be ≥ 1.5x D2 for crystal-structure stability and suitable (dis)charge cycling.
Additionally, it is unclear if (a1+a2)/2, b1, and/or {(a1+a2)/2}/b1 is/are meant to be critical. For example, the closest comp. ex. immediately outside the instant {(a1+a2)/2}/b1 range is CE 5, where (a1+a2)/2 = 0.227, b1 = 0.083, and {(a1+a2)/2}/b1 = 2.735. However, each of (a1+a2)/2, b1, and/or {(a1+a2)/2}/b1 is outside its respective range, making it unclear if the poorer performance is due to (a1+a2)/2, b1, {(a1+a2)/2}/b1, or some combination. Conversely, e.g., CE 3 includes an (a1+a2)/2 and b1 of 0.528 and 0.476, respectively, yet each of these values is within claim 1’s respective ranges.
If Applicant intends (a1+a2)/2, b1, and {(a1+a2)/2}/b1 to be synergistic, again, CE 3 (as well as CE 1, 2, 4, and 7–10), with its poorer performance, includes each of (a1+a2)/2 and b1 within each of claim 1’s respective ranges, so these three variables do not appear synergistic.
Nonetheless, arguendo, if Applicant’s results were both unexpected and superior, Examiner respectfully observes that such results appear incommensurate with claim 1 at least as follows:
Claim 1 allows a primary particle of any lithium composite oxide containing Ni and Ti, whereas the data only support high-Ni, low-Co, and low-Mn lithium oxides (Table 1); it is unclear if the results would occur over any Ni- and Ti-containing lithium composite oxide, particularly as high Ni content is known to improve capacity (per Toyama’s ¶ 0036).
Claim 1 allows a primary particle of any structure, whereas the results employ a core-shell particle including the lithium oxide core and titanium-oxide- or LTO-based shell (e.g., ¶ 0107, 0159, 0163, 0183); it is unclear if the results would occur using particles without this structure.
Claim 1 allows any b1 as long as the recited ratio as well as range of (a1+a2)/2 are fulfilled, whereas Table 2 only supports a b1 of 0.454–0.623, respectively; it is unclear if a1, a2, (a1+a2)/2, and/or b1 itself is/are critical or if only the recited ratio of Eq. 1 is intended to be critical (and the other values like (a1+a2)/2 and b1 intended to merely test within Eq. 1’s range).
Claim 1 allows any (total) average Ti content, whereas the specification appears to indicate that greater than 0.2 mol% < Ti content < 3.3 mol%, when combined with the recited 1.4–2.502 range, affords the improved efficiency characteristics (¶ 0104); it is unclear if the results occur over the entire (total) average Ti content range, e.g., at 10% Ti.
Claim 1 allows a particle of any size (either of a given secondary particle or each primary particle within); as the results center around (dis)charge capacity, which the skilled artisan would recognize directly correlates with particle size as the amount of charge able to be stored/delivered, it is unclear if substantially similar results would occur with, e.g., a secondary particle with diameter of 500 nm as with a secondary particle with diameter 10 μm.
Claim 1’s scope is to a positive active material, whereas the results stem from incorporating the active material into a positive electrode, which is incorporated as part of a lithium battery alongside a negative electrode and a separator/electrolyte (spec., e.g., pp. 26 and 27).
Similar to the preceding point, the results further center around (dis)charge efficiency and capacity retention, which the skilled artisan would recognize would directly correlate with active-material availability within each electrode; it is unclear if such capacity retention/efficiency would occur using a positive electrode including, e.g., 95% active material as with one including 70% active material.
Further similar to the preceding point, the results further center around resistance (via EIS, i.e., electrical impedance), which the skilled artisan would recognize would be affected by other factors like amount of conductive agent or amount of (insulating) binder in each electrode (see, e.g., p. 26, Prep. Ex. 2); it is unclear if the results would occur using a positive electrode including, e.g., 0.01% conductive agent and 10% binder as one using 0.01% binder and 10% conductive agent.
As MPEP 716.02(d) requires unexpected results to be commensurate with the claimed scope, this argument is further unpersuasive.
Conclusion
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/J.S.M./Examiner, Art Unit 1751
/JONATHAN G LEONG/Supervisory Patent Examiner, Art Unit 1751 5/7/2026
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