DETAILED ACTION
Notice of Pre-AIA or AIA Status
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
Status of Claims
Applicant’s amendment and arguments, filed 05/07/26, have been fully considered. Claim(s) 9 is/are amended; claim(s) 10, 11, 13, 15, and 17 stand(s) as originally or previously presented; claim(s) 1–8, 18, and 19 remain(s) withdrawn; and claim(s) 12, 14, and 16 is/are canceled. 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 set forth in the Office Action mailed 01/15/26 has/have been maintained and altered as necessitated by Applicant’s amendment, as set forth below.
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) 9–11 and 17 is/are rejected under 35 U.S.C. 103 as being unpatentable over Wu et al. (CN 109802123 A, with mach. translation) (Wu) in view of Liu et al. (JP 2016139583 A, from 06/27/23 IDS, with mach. translation) (Liu), Toyama et al. (WO 2021045025 A1, with EFD 09/06/2019; citations to English equivalent US 20220166019 A1) (Toyama), and Yonemoto et al. (WO 2019015533 A1) (Yonemoto).
Regarding claims 9–11, Wu discloses a method for preparing a cathode material (e.g., ¶ 0036), comprising 1) carrying out first mixing and first calcination in sequence on a lithium salt, a precursor and a first additive to obtain a first material (obtaining substrate A by mixing and calcining Ni-containing hydroxide precursor, lithium compound, and dopant, ¶ 0037);
(2) carrying out second mixing and second calcination in sequence on the first material and a second additive to obtain a second material (mixing mixture B (containing substrate A) with coating element, followed by calcining, ¶ 0039);
(3) crushing and sieving the second material to obtain the cathode material (e.g., ¶ 0039, 0047).
Wu discloses that the precursor is represented by Ni1–x–yM1xM2y(OH)2, where M1 is Co or Mn, M2 is one of Mn, Al, Mg, Zr, and Ba, 0 ≤ x ≤ 0.20, and 0 ≤ y ≤ 0.20 (¶ 0016); such x and y ranges overlap or encompass the recited formula (e.g., if x = 0 such that Co as M1 were absent, M2 = Mn, and y = 0.20). Although failing to explicitly disclose the recited formula, it would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to routinely incorporate the instant hydroxide by selecting metals and molar ratios from the overlapping/encompassing ranges with a reasonable expectation of achieving a successful precursor (MPEP 2144.05 (I), 2144.07). In omitting Co, moreover, such would create a cobalt-free material.
Additionally, because Wu discloses or renders obvious all of claim 9’s process steps, the skilled artisan would have reasonably expected Wu’s material to be gradient-doped, per MPEP 2112.01 (I) (as the instant gradient forms from the dopant’s gradually permeating into a bulk phase of the electrode material during sintering, per spec.’s p. 8, lines 15 and 16).
Wu further discloses that each additive may be Ti (dopant and coating element, respectively, in ¶ 0018 and 0039, respectively), which, as seen in ¶ 0075, may be in the form of TiO2. Similarly, although not explicitly embodying TiO2 as each additive, it would have been obvious to routinely select TiO2 as each additive with the reasonable expectation of achieving successful doping and coating.
Wu further discloses a general formula of substrate A (which is further coated with the coating element as well as mixed a second time with the lithium salt, ¶ 0039) of Li1+aNi1–x–yM1xM2yM3zO2, where 0 ≤ a ≤ 0.3, 0 ≤ x ≤ 0.2, 0 ≤ y ≤ 0.2, 0 ≤ z ≤ 0.1, M1 is one of Co and Mn, M2 is one of Mn, Al, Mg, Zr, and Ba, and M3 is Al, B, Ba, Mg, Ce, Cr, F, Mo, Ti, Sr, P, and/or Zr (¶ 0019). Such appears to encompass the instant general formula (e.g., if Wu’s a = x = 0, y = 0.2, M1 is absent because x = 0, M2 is Mn, z = 0.02, and M3 is Ti, such would yield LiNi0.8Mn0.2Ti0.02O2).
As in the precursor formula, then, it would have been obvious to routinely incorporate the instant oxide by selecting metals and molar ratios from the overlapping/encompassing ranges with a reasonable expectation of achieving a successful lithium metal oxide (MPEP 2144.05 (I), 2144.07).
More importantly, however, Wu discloses that high-Ni materials exhibit high energy density but poor structural and high-temperature stability (¶ 0006), so doping and coating—via, e.g., Ti—remedy these deficiencies (¶ 0006). Moreover, Wu discloses that reducing the Co content significantly reduces cost (¶ 0005), further motivating omitting Co. One skilled in the art, meanwhile, would reasonably understand that enough Li must be present for proper Li+ (de)intercalation without detracting from the transition metals’ effects. To balance all these considerations, it would have been obvious to arrive at the recited formula by routinely optimizing the lithium metal oxide’s molar ratios and, thus, formula, including within the apparent overlapping/encompassing ranges (MPEP 2144.05 (II)).
Although Wu appears to disclose or render obvious a gradient-doped material (per above), Wu fails to explicitly disclose that, in the gradient, the content of element A in the cathode material decreases in a direction from a skin layer to a center of the cathode material, wherein with reference to the total weight of the cathode material, the content of the element A in the skin layer of the cathode material is 0.2–1% by weight and the content of the element A in the center of the cathode material is 0.05–0.1% by weight.
Liu, in teaching an analogous, metal-gradient-doped positive electrode material (Title), teaches a dopant such as Ti whose concentration continuously decreases toward the active-particle core (¶ 0012). Liu teaches that the relatively high surface concentration effectively reduces the material’s reactivity with the electrolyte to improve safety and operational stability (¶ 0012), while the concentration gradually decreases toward the core to reduce the total dopant content to maintain high capacitance and service life (¶ 0012).
It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to incorporate Wu’s dopant in a concentration gradient decreasing toward the center with the reasonable expectation of improving safety and operational stability without significantly reducing capacitance, as taught by Liu.
Regarding the concentrations in the core and skin, then, Wu discloses that doping—corresponding to the center’s concentration—improves the material’s lattice and high-temperature stability (¶ 0006, 0023), while coating—corresponding to the skin’s concentration—isolates the electrolytic damage to the electrode to improve long-cycle performance (¶ 0006, 0025). The skilled artisan would recognize that each of the dopant and coating element must necessarily be distributed at some concentration within the cathode material while conforming to Liu’s decreasing concentration gradient. The artisan would understand, therefore, that a compromise must necessarily exist between the maintained capacity and service life due to the reduced dopant content toward the center and the improved safety from surface-concentrating the dopant (similar to the compromise that must necessarily exist between the dopant/central concentration for lattice stability and the coating element/skin concentration to protect against electrolytic damage). To balance these effects, then, it would have been obvious to arrive at the respectively recited ranges by routinely optimizing the A concentrations in the center and skin (MPEP 2144.05 (II)).
Wu further discloses exemplary and substantially similar weight ratios of the starting materials (e.g., ¶ 0013, 0015) but appears to fail to explicitly disclose the recited ratios of the lithium salt, precursor, and additives of claims 9–11.
However, Wu discloses, as noted above, that the dopant improves the cathode material’s lattice stability, while the coating element protects from electrolytic damage. Meanwhile, the skilled artisan would generally realize that enough of the precursor must be present to form the final Ni-metal oxide for Li+ (de)intercalation and, thus, capacity, while enough of the lithium salt must be present to transform the precursor into the final lithiated oxide for proper (de)intercalation, further recognizing that adding too much of any material would necessarily reduce the relative content and, thus, effects of the other materials. To balance all these effects, then, it would have been obvious to arrive at the respectively recited ratios by routinely optimizing the mass ratios of the lithium salt, precursor, and additives (MPEP 2144.05 (II)).
Wu further exemplarily discloses first calcining at 650–900°C (¶ 0037) at, e.g., 13 h (Ex. 3, ¶ 0073) yet, while not appearing necessarily limited to these values to achieve the desired calcination (note no technical significance to either value), modified Wu fails to explicitly disclose that conditions of the first calcining comprise 1) a temperature of 500–600°C and 2) a duration of 4–6 h.
Regarding 1), Toyama, in teaching an analogous positive active material mixed with an additive such as TiO2 (Abstract and, e.g., Ex. 2, ¶ 0123), teaches multi-stage calcining involving first and second heating treatments (fig. 1B, ¶ 0058). Toyama teaches that the first heating is 600–750°C because ≥ 600°C advances crystal generation to reduce residual surface lithium carbonate—as Wu desires (¶ 0014)—to obtain excellent output (¶ 0072), while ≤ 750°C prevents excessive crystal-grain growth and sufficiently oxidizes the metal oxide layer such as Mn oxide (MeO2, Abstract and ¶ 0069 and 0072).
To balance proper crystal generation and reduced residual lithium carbonate to obtain excellent output with preventing excessive crystal-grain growth while sufficiently oxidizing the metal oxide layer such as Mn oxide, it would have been obvious to arrive at the recited range by routinely optimizing the first calcination temperature, including within the overlap, as taught by Toyama (MPEP 2144.05 (II)).
Regarding 2), Toyama further teaches performing the first heat treatment at preferably 4–15 h because this range sufficiently promotes the lithium-carbonate reaction (to remove residual lithium, as discussed above) while being short enough to improve productivity (¶ 0075).
To balance sufficiently promoting the lithium-carbonate reaction to remove residual lithium with enhancing the method’s productivity, it would have been obvious to arrive at the recited range by routinely optimizing the first heating time, including within 4–6 h, as taught by Toyama (MPEP 2144.05 (II)).
However, despite disclosing or rendering obvious these conditions, in being unconcerned with further heating details, modified Wu fails to explicitly articulate the temperature ramp rate and, thus, 1–5°/min.
Yonemoto, in teaching an analogous method for producing cathode particles (Title), teaches that multiple holding temperatures and ramp rates are usable during calcination (bottom of p. 7), teaching a ramp rate of preferably 2–5°C/min (top of p. 8).
It would have been obvious to one of ordinary skill in the art, before the claimed invention's effective filing date, that Wu’s first calcination temperature must necessarily be scaled at some rate to arrive at the proper temperature, and, as demonstrated by Yonemoto, the skilled artisan would find it obvious to employ a ramp rate of 2–5°C/min, falling within 1–5°C/min.
Wu discloses that the second calcining occurs at 650–900°C (¶ 0039) but fails to explicitly embody 900–1000°C.
It would have been obvious to routinely select within Wu and the instant range’s overlap with the reasonable expectation of selecting a successful calcination temperature (MPEP 2144.05 (I)).
Regarding the calcination duration, Wu exemplifies 10 h in Ex. 3 (¶ 0076) but fails to explicitly embody such in combination with the general disclosure cited above.
It would have been obvious to one of ordinary skill in the art, before the claimed invention's effective filing date, that Wu's second calcination must necessarily occur for some duration, and, as demonstrated by Wu’s Ex. 3, the skilled artisan would find it obvious to select 10 h as an appropriate time.
However, despite disclosing these conditions, in being unconcerned with further heating details, modified Wu fails to explicitly articulate the temperature ramp rate and, thus, 1–5°/min.
Yonemoto further teaches that multiple holding temperatures and ramp rates are usable during calcination (bottom of p. 7), teaching a ramp rate of preferably 2–5°C/min (top of p. 8).
It would have been obvious to one of ordinary skill in the art, before the claimed invention's effective filing date, that Wu’s first calcination temperature must necessarily be scaled at some rate to arrive at the proper temperature, and, as demonstrated by Yonemoto, the skilled artisan would find it obvious to employ a ramp rate of 2–5°C/min, falling within 1–5°C.
Regarding claim 17, modified Wu discloses a cobalt-free cathode material prepared by the method according to claim 9 (Wu, e.g., ¶ 0039).
Claim(s) 13 and 15 is/are rejected under 35 U.S.C. 103 as being unpatentable over over Wu et al. (CN 109802123 A) (Wu) in view of Liu et al. (JP 2016139583 A, from 06/27/23 IDS) (Liu, Toyama et al. (WO 2021045025 A1, with EFD 09/06/2019; citations to English equivalent US 20220166019 A1) (Toyama), and Yonemoto et al. (WO 2019015533 A1) (Yonemoto), as applied to claim 9, further in view of Mizuno (WO 2019163476 A1; citations to English equivalent US 20210057716 A1) and Dai et al. (CN 104425814 A, with mach. translation) (Dai).
Regarding claims 13 and 15, modified Wu discloses the method according to claim 9 but, in being unconcerned with the conditions under which such steps occur, fails to explicitly disclose that conditions of the first mixing comprise stirring for 10–20 min with a 100L device at a rotational speed of 800–900 rpm, and conditions of the second mixing comprise stirring for 5–15 min with a 100L device at a rotational speed of 900–1000 rpm.
Mizuno, in teaching an analogous positive active material (Title), teaches mechanochemically treating a lithium compound, a transition metal such as Ni and Mn, and an additive element via, e.g., ball mill (¶ 0071–0074, 0076, 0077). Mizuno teaches that when using ball milling, the speed should be 100–1000 rpm, while the time should be 0.1–10 hr, i.e., 6 min to 10 hr (¶ 0078).
It would have been obvious to one of ordinary skill in the art, before the claimed invention's effective filing date, that Wu’s mixing must necessarily be performed in a certain manner for a certain length of time and at a certain speed, and, as demonstrated by Mizuno, the skilled artisan would find it obvious to employ ball milling at a mixing/stirring speed of 100–1000 rpm and a time of 6 min to 10 hr. This speed overlaps each of the first mixing’s 800–900 rpm and the second mixing’s 900–1000 rpm, and this time overlaps each of the first mixing’s 10–20 min and the second mixing’s 5–15 min such that the skilled artisan could have routinely selected within each overlap with a reasonable expectation of selecting conditions suitable for producing a successful cathode material (MPEP 2144.05 (I)).
Moreover, the artisan would reasonably recognize that each mixing must occur long enough for the reaction to occur, whereas mixing for too long would necessarily delay manufacturing. To balance these effects, then, it would have been obvious to arrive at the recited time by routinely optimizing at least the stirring time, including within 6–15 min and 6–20 min, respectively (MPEP 2144.05 (II)).
Though modified Wu discloses or renders obvious the first and second mixings’ speed and time, modified Wu fails to explicitly articulate the volume of the mill and, thus, fails to explicitly disclose that each mixing occurs in a 100 L device.
Dai, in teaching an analogous, metal-doped lithium manganate cathode material (Abstract), teaches stirring a lithium compound, a manganese compound, and a dopant compound in a 100 L ball mill (e.g., Ex. 1, ¶ 0060).
It would have been obvious to one of ordinary skill in the art, before the claimed invention's effective filing date, that Wu’s ball mill must necessarily be incorporated with some volume, and, as demonstrated by Dai, the skilled artisan would find it obvious to employ a 100 L device in each mixing step as an appropriate volume.
Response to Arguments
Applicant’s arguments with respect to claim(s) 9 have been fully considered but are unpersuasive.
Applicant argues that Wu fails to disclose or suggest that the dopant and coating element must be the same and merely discloses an overlap of possible dopants and coating elements, including Ti, implying that one skilled in the art could arbitrarily combine the dopant and coating element. Examiner agrees that Wu’s disclosure is broad enough to arbitrarily select the same element as the dopant and coating element and respectfully submits that such was precisely the rationale in the rejection, as in selecting a known material based on suitability for its intended use in MPEP 2144.07. There need be no specific direction to select the same species from each genus, absent unexpected results.
Applicant then argues that the first and second additive’s being the same possesses technical significance for a) doping consistency and lattice-distortion prevention, b) simplicity, and c) uniformity. Examiner respectfully submits, however, that 1) such language is not in the specification and, thus, appears speculative (MPEP 2145 (I)) and, therefore, unpersuasive. 2) At least a) and b) would seem expected from Wu in tandem with the general knowledge of one of ordinary skill because Wu mentions that doping and surface coating are known to improve lattice stability (¶ 0006), and the skilled artisan would realize that choosing the same element for doping and coating would necessarily simplify production by being able to use the same raw-material source. 3) There appear to be no unexpected results based on selecting the same versus different elements as dopant and coating agent in the evidence of record given all comparative examples (pp. 16–18) choose the same element for each step. Thus, absent additional evidence, this argument is unpersuasive, and the case of obviousness based on routinely selecting the same element for doping and coating appears to remain proper.
Applicant next argues that the weight ratio of the first:second additives ensures gradient doping such that the content of element A decreases from skin to center. Applicant specifically alleges that Wu does not mention controlling this relation and could, e.g., instead disclose uniform doping or reverse gradient doping. Examiner respectfully disagrees because, as mentioned above, the recited gradient trend forms from the instant process, where the sintering/calcination makes element A gradually diffuse into the bulk/interior and, thus, exhibit a concentration decreasing toward the center. Because Wu discloses the process steps, including the first and second calcining at substantially similar temperatures, Wu’s process would reasonably achieve the instant gradient, absent evidence otherwise. Moreover, Liu was used to further render obvious this feature.
Applicant argues that the first:second weight ratio achieves unexpected results based on Comp. Ex. 3, which is outside this ratio, meaning the skilled artisan would be unmotivated to control the additives’ ratio based on Wu. Examiner respectfully disagrees because Comp. Ex. 3 only tests below the instant range, but it is unclear what occurs above the range and, thus, indeterminable whether exceeding the range would yield deleterious results. As criticality demonstrations require comparing a sufficient number of tests both inside and outside—and, thus, above and below the range—this argument is unpersuasive. Rather, as discussed above, the skilled artisan would have routinely optimized this ratio to balance the effects of doping and coating, absent additional evidence.
Applicant then argues that Liu fails to teach the additive ratio, but, again, such remains routinely optimizable based on Wu as well as Liu’s general teachings of incorporating the decreasing gradient to balance capacity with safety.
Applicant then argues that Wu’s calcination temperatures are different than the recited ranges. Regarding the first temperature, Applicant argues that Wu’s 650–900°C is too high and would yield rapid thermal diffusion and non-gradient doping. Examiner respectfully submits that, again, such language is not in the specification and, thus, appears speculative, and Wu’s range appears exemplary and not strictly limiting, which is why Toyama was used to motivate first calcination of 600–750°C for sufficient lithium-carbonate removal while preventing excessive crystal-grain growth and sufficient oxidation.
Although Applicant cites Comp. Ex. 4, with first temp. 650°C, as evidence that Wu’s first range would yield inferior results, Examiner respectfully notes that both the first and second calcination temperatures are outside their respective ranges, making it indeterminable whether the poorer performance is due to the first temperature, second temperature, or both.
Applicant then argues that Toyama teaches away from < 600°C as being insufficient for carbonate removal, while Applicant’s 500–600°C is, again, critical for preventing rapid dopant diffusion and reverse-gradient doping. Examiner respectfully disagrees because Toyama’s 600–750°C plainly overlaps 500–600°C, and, as discussed above, there appears to be no comparative evidence of record of inferior performance isolated to the first temperature, again making the rapid-diffusion argument appear speculative.
Rather, the premise of MPEP 2144.05 is that the skilled artisan, in the absence of criticality, would have reasonably expected success from selecting any value—including within the overlap and at the endpoints—and, specifically regarding 2144.05 (II), the artisan would have been apprised of differences within the range—here the need to balance carbonate removal with preventing excess grain growth from Toyama—and would have known to account for and optimize the value to balance the effects. Thus, this argument is unpersuasive, and the same rationale of the apparent lack of criticality as well as speculation applies to the auxiliary argument that the skilled artisan would not have known to lower the temperature to Applicant’s 500–600°C because such “acts contrary to conventional teaching.”
Applicant then submits a “preemptive rebuttal” of the above argument of overlapping endpoints, alleging that a) the overlap consists of isolated endpoints versus substantive overlap; b) Comp. Ex. 4 demonstrates that operating within the overlap yields poorer results; and c) Toyama teaches away. Again, however, a) MPEP 2144.05 clearly supports obviousness of endpoint overlap without criticality; b) CE 4’s weaker performance does not appear isolatable to the first temperature; and c) Toyama plainly includes 600°C as a sufficient first temperature, and the artisan would have optimized this temperature to remove carbonate while preventing excess grain growth, making this argument unpersuasive.
Applicant finally argues that Wu’s second temperature of 650–900°C teaches away from 900–1000°C because “one should operate way from the upper limit to avoid over-sintering and structural degradation.” However, 1) Wu plainly describes 900°C, as part of the above range, as a suitable second temperature, and 2) Comp. Ex. 4’s second temperature is 50°C below 900°C (i.e., indeterminable what occurs directly below 900°), while the example also varies the first temperature outside its range, making it unclear which variable(s) is responsible for the poorer performance. Rather, as explained above, the case of obviousness appears to remain proper because the skilled artisan, absent criticality, would have reasonably expected success in choosing any value of Wu’s second temperature, including 900°, making this argument unpersuasive.
Conclusion
Applicant's amendment necessitated the new ground(s) of rejection presented in this Office action. Accordingly, THIS ACTION IS MADE FINAL. See MPEP § 706.07(a). Applicant is reminded of the extension of time policy as set forth in 37 CFR 1.136(a).
A shortened statutory period for reply to this final action is set to expire THREE MONTHS from the mailing date of this action. In the event a first reply is filed within TWO MONTHS of the mailing date of this final action and the advisory action is not mailed until after the end of the THREE-MONTH shortened statutory period, then the shortened statutory period will expire on the date the advisory action is mailed, and any nonprovisional extension fee (37 CFR 1.17(a)) pursuant to 37 CFR 1.136(a) will be calculated from the mailing date of the advisory action. In no event, however, will the statutory period for reply expire later than SIX MONTHS from the mailing date of this final action.
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/J.S.M./Examiner, Art Unit 1751
/Haroon S. Sheikh/Primary Examiner, Art Unit 1751
Prosecution Insights