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 .
Election/Restrictions
Claim 12 withdrawn from further consideration pursuant to 37 CFR 1.142(b) as being drawn to a nonelected species 2, there being no allowable generic or linking claim. Election was made without traverse in the reply filed on 06/09/2026.
Claim Status
Claim(ss 12 is withdrawn, and Claim(s) 1-11 and 13-20 stand as originally or as previously presented. claim(s) 1-11 and 13-20 are examined in this office action.
Priority
Receipt is acknowledged of certified copies of papers required by 37 CFR 1.55.
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.
Claims 11 and 16 rejected under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), second paragraph, as being indefinite for failing to particularly point out and distinctly claim the subject matter which the inventor or a joint inventor (or for applications subject to pre-AIA 35 U.S.C. 112, the applicant), regards as the invention.
This is because both claims include the limitation that the second lithium-manganese-based oxide is a particle “having a concentration gradient having a constant nickel and manganese concentrations”. It is unclear how the particle both have a concentration gradient and have constant concentrations. For the purposes of examination, a particle having constant nickel and manganese concentrations will be interpreted as fulfilling the limitation of requiring a concentration gradient.
Double Patenting
The nonstatutory double patenting rejection is based on a judicially created doctrine grounded in public policy (a policy reflected in the statute) so as to prevent the unjustified or improper timewise extension of the “right to exclude” granted by a patent and to prevent possible harassment by multiple assignees. A nonstatutory double patenting rejection is appropriate where the conflicting claims are not identical, but at least one examined application claim is not patentably distinct from the reference claim(s) because the examined application claim is either anticipated by, or would have been obvious over, the reference claim(s). See, e.g., In re Berg, 140 F.3d 1428, 46 USPQ2d 1226 (Fed. Cir. 1998); In re Goodman, 11 F.3d 1046, 29 USPQ2d 2010 (Fed. Cir. 1993); In re Longi, 759 F.2d 887, 225 USPQ 645 (Fed. Cir. 1985); In re Van Ornum, 686 F.2d 937, 214 USPQ 761 (CCPA 1982); In re Vogel, 422 F.2d 438, 164 USPQ 619 (CCPA 1970); In re Thorington, 418 F.2d 528, 163 USPQ 644 (CCPA 1969).
A timely filed terminal disclaimer in compliance with 37 CFR 1.321(c) or 1.321(d) may be used to overcome an actual or provisional rejection based on nonstatutory double patenting provided the reference application or patent either is shown to be commonly owned with the examined application, or claims an invention made as a result of activities undertaken within the scope of a joint research agreement. See MPEP § 717.02 for applications subject to examination under the first inventor to file provisions of the AIA as explained in MPEP § 2159. See MPEP § 2146 et seq. for applications not subject to examination under the first inventor to file provisions of the AIA . A terminal disclaimer must be signed in compliance with 37 CFR 1.321(b).
The filing of a terminal disclaimer by itself is not a complete reply to a nonstatutory double patenting (NSDP) rejection. A complete reply requires that the terminal disclaimer be accompanied by a reply requesting reconsideration of the prior Office action. Even where the NSDP rejection is provisional the reply must be complete. See MPEP § 804, subsection I.B.1. For a reply to a non-final Office action, see 37 CFR 1.111(a). For a reply to final Office action, see 37 CFR 1.113(c). A request for reconsideration while not provided for in 37 CFR 1.113(c) may be filed after final for consideration. See MPEP §§ 706.07(e) and 714.13.
The USPTO Internet website contains terminal disclaimer forms which may be used. Please visit www.uspto.gov/patent/patents-forms. The actual filing date of the application in which the form is filed determines what form (e.g., PTO/SB/25, PTO/SB/26, PTO/AIA /25, or PTO/AIA /26) should be used. A web-based eTerminal Disclaimer may be filled out completely online using web-screens. An eTerminal Disclaimer that meets all requirements is auto-processed and approved immediately upon submission. For more information about eTerminal Disclaimers, refer to www.uspto.gov/patents/apply/applying-online/eterminal-disclaimer.
Claim 1-6 and 13 provisionally rejected on the ground of nonstatutory double patenting as being unpatentable over claim 1, 8, 5-17, and 20 of copending Application No. 18/323,951 (reference application). Although the claims at issue are not identical, they are not patentably distinct from each other because 18/323,951 contains each and every limitation of the instant claims.
This is a provisional nonstatutory double patenting rejection because the patentably indistinct claims have not in fact been patented.
Regarding claim 1, claim 1 of 18/323,951 discloses a bimodal-type positive electrode active material comprising a first and a second lithium manganese-based oxide, which have different particle diameters (claim 1 of 18/323,951 discloses the first oxide is a small particle and the second particle is a large particle), wherein the difference in average particle diameter between the first and second lithium manganese-based oxides is 3 µm or more (claim 8 of 18/323,951 discloses that the average particle diameter of the first oxide is 2 to 5 µm, while claim 15 discloses that the second oxide has an average particle diameter of 6 to 14 µm. Depending on the values selected for each of the oxides, the claimed difference between the first and second oxide being 3 µm or more is satisfied, creating a scenario where the claimed range is overlapped by 18/323,951. Selection of overlapping portions of ranges has been held to be a prima facie case of obviousness (see MPEP 2144.05(1))), and
the first and second lithium manganese-based oxides are oxides in which a phase belonging to a C2/m space group and a phase belonging to a R3-m space group are dissolved or complexed (claim 1 of 18/323,951).
Regarding claim 2, claim 8 of 18/323,951 discloses the positive electrode active material of claim 1, wherein the first lithium manganese-based oxide has an average particle diameter of 2 to 5 µm.
Regarding claim 3, claim 15 of 18/323,951 discloses the positive electrode active material of claim 1, wherein the first lithium manganese-based oxide has an average particle diameter of 7-14 µm (claim 15 of 18/323,951 discloses a diameter of 6-14, overlapping the claimed range. Selection of overlapping portions of ranges has been held to be a prima facie case of obviousness (see MPEP 2144.05(1))).
Regarding claim 4, 18/323,951 discloses the positive electrode active material of claim 1, wherein the main peak of a particle size distribution graph (X axis: particle size, Y axis: Vol%) of the first lithium manganese-based oxide based on a volume is present between 1 to 8 µm (claim 8 of 18/323,951 discloses that the average particle diameter of the fist oxide is 2 to 5 µm. Based on this, a person of ordinary skill in the art before the effective filing date of the claimed invention would understand that a main peak of a particle size distribution graph would be between 1 to 8 µm), and
the main peak of a particle size distribution graph of the second lithium manganese-based oxide based on a volume is present between 6 to 24 µm (claim 15 of 18/323,951 discloses that the average particle diameter of the second oxide is between 6 and 14 µm. Based on this, a person of ordinary skill in the art before the effective filing date of the claimed invention would understand that it would be obvious that a main peak of a particle size distribution graph would be between 6 and 24 µm).
Regarding claim 5, 18/323,951 discloses the positive electrode active material of claim 1, wherein the first oxide and the second oxide in the positive electrode active material are included in a weight ratio of 10:90 to 80:20 (claim 16 of 18/323,951).
Regarding claim 6, 18/323,951 discloses the positive electrode active material of claim 1, wherein the first and second oxide each independently comprise at least one selected from nickel, cobalt, and manganese (claim 17 of 18/323,951)
Regarding claim 13, 18/323,951 discloses the positive electrode active material of claim 1, wherein the first and second oxide are each independently represented by formula 1-1 (Claim 20 of 18/323,951 discloses formula 1, which is identical to formula 1-1 save the inclusion of a variable M3. M3 is allowed to be zero, therefore in cases where M3 is zero, the two formulas are the same).
Claim 7-8 and 19-20 provisionally rejected on the ground of nonstatutory double patenting as being unpatentable over claim 1 of copending Application No. 18/323,951 in view of Nakabayashi (JP 2016051504 A, a machine translation from Espacenet is used as an English equivalent).
Regarding claim 7, the claims of 18/323,951 does not disclose the limitations claimed in claim 7, however these limitations are known in the art. For example, Nakabayashi discloses a similar first and second lithium manganese-based oxide, wherein the first and second oxides are each independently lithium manganese-based oxides comprising nickel and manganese [0011], and
the content (mol%) of manganese with respect to all transition metals of the first lithium manganese-based oxide is smaller than that of the second lithium manganese-based oxide ([0019] and [0027] discloses that one of the distinguishing features of Nakabayashi is that the ratio of nickel atomic concentration to manganese atomic concentration in the lithium manganese-based oxides differs among the oxides. Particularly, [0029] discloses that when the nickel atomic concentration of the oxide with the higher nickel concentration is Nir, the manganese atomic concentration is Mnr, and the nickel atomic concentration of the compound with the lower nickel atomic concentration is nip, then (Nir/Mnr)/(Nip/Mnp) is 1.1 or greater. Nakabayashi does not explicitly teach whether the first (small sized) or second (large sized) oxide should have the smaller mol% manganese with respect to transition metals, however table 1 shows an example (see [0091] of original document) wherein the content of manganese with respect to transition metals (in this case Ni) of the first oxide is smaller than that of the second oxide, satisfying the claimed limitation). [0023] discloses that the active material of Nakabayashi can offer improved capacity and volume characteristics [0030], and as a result it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to implement the teachings of Nakabayashi regarding manganese concentrations in each of the oxides in the oxides of 18/323,951 for at least these reasons.
Regarding claim 8, the claims of 18/323,951 does not disclose the limitations claimed in claim 8, however these limitations are known in the art. For example, Nakabayashi discloses a similar first and second lithium manganese-based oxide, wherein the first and second oxides are each independently lithium manganese-based oxides comprising nickel and manganese [0011], and
the content (mol%) of manganese with respect to all transition metals present in the surface portion of the first lithium manganese-based oxide is smaller than that of the second lithium manganese-based oxide ([0019] and [0027] discloses that one of the distinguishing features of Nakabayashi is that the ratio of nickel atomic concentration to manganese atomic concentration in the lithium manganese-based oxides differs among the oxides. Particularly, [0029] discloses that when the nickel atomic concentration of the oxide with the higher nickel concentration is Nir, the manganese atomic concentration is Mnr, and the nickel atomic concentration of the compound with the lower nickel atomic concentration is nip, then (Nir/Mnr)/(Nip/Mnp) is 1.1 or greater. Nakabayashi does not explicitly teach whether the first (small sized) or second (large sized) oxide should have the smaller mol% manganese with respect to transition metals, however table 1 shows an example (see [0091] of original document) wherein the content of manganese with respect to transition metals (in this case Ni) of the first oxide is smaller than that of the second oxide, satisfying the claimed limitation.
Nakabayashi does not teach the surface of either oxide having different concentrations of Mn or transition metals than core portions of the oxide, therefore if the first oxide has a lower ratio of Mn to transition metal overall, it would also have a lower ratio of Mn to transition metal on the surface portion, satisfying the claimed limitation). [0023] discloses that the active material of Nakabayashi can offer improved capacity and volume characteristics [0030], and as a result it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to implement the teachings of Nakabayashi regarding manganese concentrations in each of the oxides in the oxides of 18/323,951 for at least these reasons.
Regarding claim 19 and 20, 18/323,951 discloses bimodal-type positive electrode active material of claim 1, but does not explicitly disclose in the claims using it in a positive electrode or a battery. However, use of a positive electrode active material in a positive electrode and a lithium secondary battery is well known in the art and would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention. For example, Nakabayashi discloses a very similar active material as 18/323,951 (see [0011], [0026], and table 1 in the original document ([0091]), and further discloses using use of such in a positive electrode [0013] and lithium secondary battery [0019], rendering claims 19 and 20 obvious.
This is a provisional nonstatutory double patenting rejection.
Claim 9-10, 14-15, and 17-18 provisionally rejected on the ground of nonstatutory double patenting as being unpatentable over claim 1 of copending Application No. 18/323,951 in view of Wu (“Full concentration Gradient-Tailored Li-Rich Layered Oxides for High-Energy Lithium-Ion Batteries”, included with IDS of 04/01/2024).
Regarding claim 9, modified 18/323,951 discloses the positive electrode active material of claim 1, but does not disclose that at least one of the oxides is a core-shell particle having a concentration gradient of at least one selected from nickel and manganese from the central portion to the surface portion. However, inclusion of such core-shell structures having concentration gradients in lithium manganese oxides and the benefits associated with doing so is known in the art and would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include in the invention of 18/323,951.
For example, Wu discloses lithium and manganese oxides (abstract) having both Li2MnO3 and LiMO2 phases similar to 18/323,951 (fig. 1 and pg. 4, paragraph 1 of Wu), having a concentration gradient of at least one selected from nickel and manganese from the central to the surface portion (abstract discloses linearly decreasing Mn and increasing Ni from the particle center to the surface, reading on the claimed limitation). Wu discloses that the gradient-tailored oxides exhibit notably reduced voltage decay, enhanced rate performance, improved cycle stability, and thermal stability. As a result, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include concentration gradients as described in Wu in the oxide materials of 18/323,951 for at least these reasons.
Wu further discloses coating layers to improve performance of lithium oxides, as pg. 1, paragraph 1 discloses surface coating layers on the lithium oxide particles, reasonably reading as a core-shell structure, to improve cycling performance and lessen voltage decay, with paragraphs 1 and 2 of pg. 2 discussing use of coating layers in gradient oxides. As a result, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include a coating layer in the oxides of 18/323,951 to obtain the above mentioned benefits, and doing so would result in a positive electrode active material according to the instant claim 9.
Regarding claim 10, modified 18/323,951 discloses the positive electrode active material of claim 9, wherein the core-shell particle has a gradient in which the nickel concentration increases and the manganese concentration decreases from the central portion to the surface portion (abstract of Wu).
Regarding claim 14, modified 18/323,951 discloses the positive electrode active material of claim 1, but does not disclose a barrier layer present on at least part of the surface of at least one of the oxides. However, inclusion of a barrier layer on similar lithium manganese-based oxides and the benefits of doing so are known in the art and would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention.
For example Wu discloses lithium and manganese oxides (abstract) having both Li2MnO3 and LiMO2 phases similar to 18/323,951 (fig. 1 and pg. 4, paragraph 1 of Wu). Wu further discloses coating layers to improve performance of lithium oxides, as pg. 1, paragraph 1 discloses surface coating layers on the lithium oxide particles to improve cycling performance and lessen voltage decay. As a result, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include a coating layer in the oxides of modified 18/323,951 to obtain the above mentioned benefits, and doing so would result in a positive electrode active material according to the instant claim 14.
Regarding claim 15, modified 18/323,951 discloses the positive electrode active material of claim 14, wherein the first lithium manganese-based oxide has a barrier layer present on at least a part of the surface (see claim 14 above), but 18/323,951 does not disclose that the oxide is a core shell particle having a concentration gradient of at least one selected from nickel and manganese from the core to the shell. However, such an oxide structure and the benefits thereof are known in the art and would have been obvious to implement in the oxide of modified 18/323,951.
For example, Wu discloses lithium and manganese oxides (abstract) having both Li2MnO3 and LiMO2 phases similar to 18/323,951 (fig. 1 and pg. 4, paragraph 1 of Wu), having a concentration gradient of at least one selected from nickel and manganese from the central to the surface portion (abstract discloses linearly decreasing Mn and increasing Ni from the particle center to the surface, reading on the claimed limitation). Wu discloses that the gradient-tailored oxides exhibit notably reduced voltage decay, enhanced rate performance, improved cycle stability, and thermal stability. As a result, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include concentration gradients as described in Wu in the oxide materials of modified 18/323,951 for at least these reasons. This is also reasonably interpreted as a core-shell structure, as the gradient results in an outer layer (shell) with different composition than the inner portion (core). Making this modification to the oxide of 18/323,951 would result in an oxide wherein the barrier layer is present on the surface of the shell, satisfying the limitations of claim 15.
Regarding claim 17, modified 18/323,951 discloses the positive electrode active material of claim 14, wherein the barrier layer comprises an oxide comprising at least one selected from a metal element (Wu discloses a metal oxide for the coating layer, see pg. 1, paragraph 1, or pg. 2, paragraphs 1-2).
Regarding claim 18, modified 18/323,951 discloses the positive electrode active material of claim 14, wherein the barrier layer comprises at least one selected from a second oxide represented by formula 3 (pg. 1, paragraph 1 of Wu discloses, for example, a surface coating layer of Li-4Mn5O12, which matched the claimed formula 3 when g is 4, h is 5, i is 12, and M4 is Mn).
Claim 11 and 16 provisionally rejected on the ground of nonstatutory double patenting as being unpatentable over claim 1 of copending Application No. 18/323,951 in view of Wu (“Full concentration Gradient-Tailored Li-Rich Layered Oxides for High-Energy Lithium-Ion Batteries”, included with IDS of 04/01/2024), and further in view of Kim (KR 20190093454 A, a machine translation from Espacenet is used as an English equivalent).
Regarding claim 11, as best understood based on the 35 USC 112 rejection mentioned above, 18/323,951 discloses the positive electrode active material of claim 1, but does not disclose that the first lithium manganese-based oxide is a core-shell particle having a concentration gradient of at least one selected from nickel and manganese from the central to the surface portion. However, inclusion of such core-shell structures having concentration gradients in lithium manganese oxides and the benefits associated with doing so is known in the art and would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include in the invention of 18/323,951.
For example, Wu discloses lithium and manganese oxides (abstract) having both Li2MnO3 and LiMO2 phases similar to 18/323,951 (fig. 1 and pg. 4, paragraph 1 of Wu), having a concentration gradient of at least one selected from nickel and manganese from the central to the surface portion (abstract discloses linearly decreasing Mn and increasing Ni from the particle center to the surface, reading on the claimed limitation). Wu discloses that the gradient-tailored oxides exhibit notably reduced voltage decay, enhanced rate performance, improved cycle stability, and thermal stability. As a result, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include concentration gradients as described in Wu in the oxide materials of modified 18/323,951 for at least these reasons.
Wu further discloses coating layers to improve performance of lithium oxides, as pg. 1, paragraph 1 discloses surface coating layers on the lithium oxide particles, reasonably reading as a core-shell structure, to improve cycling performance and lessen voltage decay, with paragraphs 1 and 2 discussing use of coating layers in gradient oxides. As a result, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include a coating layer in the oxides of 18/323,951 to obtain the above mentioned benefits.
Wu does not discuss bimodal positive electrode active material, and therefore does not disclose a first oxide having a concentration gradient, and a second oxide having constant nickel and manganese concentrations or a lower slope than the concentration gradient of the first oxide. However, use of bimodal positive electrode active material oxides, wherein a first oxide has a concentration gradient of Nickel and/or manganese, a second oxide has a lower slope than the concentration gradient of the first oxide or a constant nickel and manganese concentration, was known in the art before the effective filing date of the claimed invention and would have been obvious to a person of ordinary skill in the art.
For example, Kim discloses a bimodal positive electrode active material highly similar to modified 18/323,951 wherein two lithium composite oxides, one having smaller particle sizes and one having larger particle sizes, are used [0006]. Kim further discloses that one of the oxides is a lithium complex transition metal oxide having a concentration gradient ([0014] discloses a lithium transition metal oxide having a concentration gradient with respect to nickel and manganese), and the other is a lithium complex transition metal oxide not having a concentration gradient [0034]. Kim discloses that by using a mixture of differently sized particles having a concentration gradient and not having a concentration gradient, it is possible to secure a higher capacity while ensuring thermal stability, and improve high-temperature life characteristics and high temperature storage stability. As a result, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to use a first oxide having a concentration gradient of at least one selected from nickel and manganese from the central portion to the surface, and a second oxide having a constant nickel and manganese concentration, in the invention of 18/323,951, as taught by Kim. A person of ordinary skill would have been motivated to do this to obtain the benefits disclosed by Kim, and doing so would result in a positive electrode active material according to the instant claim.
Regarding claim 16, as best understood based on the 35 USC 112 rejection mentioned above, 18/323,951 discloses the positive electrode active material of claim 14, wherein a barrier layer is present on at least part of the surface of the second oxide (see claim 14 rejection above).
18/323,951 does not disclose that either oxide has a concentration gradient or a constant concentration with respect to nickel or manganese concentrations. However, inclusion of such a second oxide having a concentration gradient having constant concentrations or a lower slope than that of a first oxide, and the benefits associated with doing so, is known in the art and would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include in the invention of modified 18/323,951.
For example, Kim discloses a bimodal positive electrode active material highly similar to 18/323,951 wherein two lithium composite oxides, one having smaller particle sizes and one having larger particle sizes, are used [0006]. Kim further discloses that one of the oxides is a lithium complex transition metal oxide having a concentration gradient ([0014] discloses a lithium transition metal oxide having a concentration gradient with respect to nickel and manganese), and the other is a lithium complex transition metal oxide not having a concentration gradient [0034]. Kim discloses that by using a mixture of differently sized particles having a concentration gradient and not having a concentration gradient, it is possible to secure a higher capacity while ensuring thermal stability, and improve high-temperature life characteristics and high temperature storage stability. As a result, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to use a first oxide having a concentration gradient of at least one selected from nickel and manganese from the central portion to the surface, and a second oxide having a constant nickel and manganese concentration, in the invention of 18/323,951, as taught by Kim. A person of ordinary skill would have been motivated to do this to obtain the benefits disclosed by Kim, and doing so would result in a positive electrode active material according to the instant claim.
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.
Claim(s) 1-3, 5-8, 13, and 19-20 is/are rejected under 35 U.S.C. 103 as being unpatentable over Nakabayashi (JP 2016051504 A, a machine translation from Espacenet is used as an English equivalent) in view of Choi (US 20180145322 A1).
Regarding claim 1, Nakabayashi discloses a bimodal-type positive electrode active material comprising a first lithium manganese-based oxide and a second lithium manganese-based oxide, which have different average particle diameters ([0026] discloses lithium transition metal composite oxides including Mn, reading on lithium manganese-based oxides, [0011] discloses a first and second solution containing both nickel and manganese, wherein there are at least two types of particles with different average particle diameters),
wherein the difference in average particle diameter between the first oxide and the second oxide is 3 µm or more ([0011] discloses that D1 is the larger particle and D2 is the smaller particle, and D1/D2 ≥ 2, therefore D1 is at least twice the size of D2. As a result, the difference between the first lithium-manganese-based oxide and the second will be 3 µm or more in cases where the smaller oxide D2 is at least is 3 µm or greater in size. Table 2 ([0091], see original document) discloses an example where the smaller oxide is 4µm, which would necessitate a large oxide particle size of at least 8µm, falling within the clamed range).
Nakabayashi does not explicitly teach that the first and second oxides are oxides in which a C2/m and R3-m space group are dissolved or completed. However, [0026] discloses that the lithium metal composite oxides are represented by a formula Li2MnO3-LiMO2, wherein M represents elements such as Co, Ni and Mn ([0011] discloses that the oxides include at least Ni and Mn).
Choi, in the same field of endeavor, discloses a similar bimodal positive electrode active material [0054] of a similar formula Li-2MnO3-LiMnO2 [0045], additionally disclosing that the dissolved or completed C2/m phase is associated with the Li-2MnO3- portion, and the dissolved or completed R3-m phase is associated with the LiMnO2- portion. Abstract of Choi discloses including the R3-m space group, with [0044] disclosing the inclusion of both space groups at the same time. [0092] discloses that the inclusion of the C2/m space group improves charge/discharge capacity. As a result of this, and the fact that both Choi and Nakabayashi disclose using the same or a highly similar material, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention, to include the structure as taught by Choi in the active material of Nakabayashi, to predictably yield a positive electrode active material with improved charge/discharge capacity, and doing so would result in a positive electrode active material meeting the limitations of claim 1.
Regarding claim 2, modified Nakabayashi discloses the positive electrode active material of claim 1, wherein the first lithium manganese-based oxide has an average particle diameter of 2 to 6 µm (Table 2 ([0091], see original document) discloses an example where the smaller oxide (corresponding to the claimed first oxide) is 4 µm.
Regarding claim 3, modified Nakabayashi discloses the positive electrode active material of claim 1, wherein the second lithium manganese-based oxide has an average particle diameter of 7 to 14 µm ([0036 discloses that the average particle size of each of the secondary particles is 1 µm or more and 60 µm or less, with [0037[ disclosing D1/D2 ≥ 2, when the larger particle size and smaller particle size of the two types of primary particles are denoted as D1 and D2, respectively. Table 2 ([0091], see original document) discloses an example where the smaller oxide (corresponding to the claimed first oxide) is 4 µm, therefore a person of ordinary skill in the art before the effective filing date of the claimed invention would find it obvious to routinely select an average particle size of, for example, 8 µm or greater, as the size of the second lithium manganese-based oxide, overlapping the claimed range and satisfying D1/D2 ≥ 2. Selection of overlapping portions of ranges has been held to be a prima facie case of obviousness (see MPEP 2144.05(1))).
Regarding claim 5, modified Nakabayashi discloses the positive electrode active material of claim 1, wherein the first and second lithium manganese-based oxides in the positive electrode active material are included in a weight ratio of 10:90 to 80:20 ([0011] discloses that when the mass of the large-sized oxide (corresponding to the claimed second oxide) W1 and the mass of the small-sized oxide (corresponding to the claimed first oxide) is W2, the following formula 0.2 ≤ W1/(W1 + W2) ≤ 0.9 is satisfied, overlapping the claimed mass ratio range. Selection of overlapping portions of ranges has been held to be a prima facie case of obviousness (see MPEP 2144.05(1))).
Regarding claim 6, modified Nakabayashi discloses the positive electrode active material of claim 1, wherein the first and second oxides each independently comprise at least one selected from nickel, cobalt, and manganese (see [0026], claim 1 rejection above).
Regarding claim 7, modified Nakabayashi discloses the positive electrode active material of claim 1, wherein the first and second oxides are each independently lithium manganese-based oxides comprising nickel and manganese [0011], and
the content (mol%) of manganese with respect to all transition metals of the first lithium manganese-based oxide is smaller than that of the second lithium manganese-based oxide ([0019] and [0027] discloses that one of the distinguishing features of Nakabayashi is that the ratio of nickel atomic concentration to manganese atomic concentration in the lithium manganese-based oxides differs among the oxides. Particularly, [0029] discloses that when the nickel atomic concentration of the oxide with the higher nickel concentration is Nir, the manganese atomic concentration is Mnr, and the nickel atomic concentration of the compound with the lower nickel atomic concentration is nip, then (Nir/Mnr)/(Nip/Mnp) is 1.1 or greater. Nakabayashi does not explicitly teach whether the first (small sized) or second (large sized) oxide should have the smaller mol% manganese with respect to transition metals, however table 1 shows an example (see [0091] of original document) wherein the content of manganese with respect to transition metals (in this case Ni) of the first oxide is smaller than that of the second oxide, satisfying the claimed limitation).
Regarding claim 8, modified Nakabayashi discloses the positive electrode active material of claim 1, wherein the first and second oxides are each independently lithium manganese-based oxides comprising nickel and manganese [0011], and
the content (mol%) of manganese with respect to all transition metals present in the surface portion of the first lithium manganese-based oxide is smaller than that of the second lithium manganese-based oxide ([0019] and [0027] discloses that one of the distinguishing features of Nakabayashi is that the ratio of nickel atomic concentration to manganese atomic concentration in the lithium manganese-based oxides differs among the oxides. Particularly, [0029] discloses that when the nickel atomic concentration of the oxide with the higher nickel concentration is Nir, the manganese atomic concentration is Mnr, and the nickel atomic concentration of the compound with the lower nickel atomic concentration is nip, then (Nir/Mnr)/(Nip/Mnp) is 1.1 or greater. Nakabayashi does not explicitly teach whether the first (small sized) or second (large sized) oxide should have the smaller mol% manganese with respect to transition metals, however table 1 shows an example (see [0091] of original document) wherein the content of manganese with respect to transition metals (in this case Ni) of the first oxide is smaller than that of the second oxide, satisfying the claimed limitation.
Nakabayashi does not teach the surface of either oxide having different concentrations of Mn or transition metals than core portions of the oxide, therefore if the first oxide has a lower ratio of Mn to transition metal overall, it would also have a lower ratio of Mn to transition metal on the surface portion, satisfying the claimed limitation).
Regarding claim 13, modified Nakabayashi discloses the positive electrode active material of claim 1, wherein the first and second oxides are each independently represented by formula 1-1 below:
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([0026] of Nakabayashi discloses that the lithium metal composite oxides are represented by a formula Li2MnO3-LiMO2, wherein M represents elements such as Co, Ni and Mn ([0011] discloses that the oxides include at least Ni and Mn, which matches the claimed formula 1-1 when, for example, b”, b’, and y’ are zero, r is 0.5, M1 is Ni and Mn). Table 1 for example discloses Li1.16Ni0.2Mn0.6O2, falling within the claimed formula).
Regarding claim 19, modified Nakabayashi discloses a positive electrode comprising the positive electrode active material of claim 1 ([0013] of Nakabayashi).
Regarding claim 20, modified Nakabayashi discloses a lithium secondary battery using the positive electrode of claim 19 ([0019] of Nakabayashi)
Claim(s) 4 is/are rejected under 35 U.S.C. 103 as being unpatentable over Nakabayashi (JP 2016051504 A, a machine translation from Espacenet is used as an English equivalent) in view of Choi (US 20180145322 A1), and further in view of Ogawa (US 20190319257 A1).
Regarding claim 4, modified Nakabayashi discloses the positive electrode active material of claim 1, but does not explicitly disclose a particle size distribution graph for the particle sizes of the two oxides. However, it is generally known in the art that more uniform particle size distributions lead to more preferable results concerning active materials. For example, Ogawa discloses that a more narrow or uniform particle size distribution for composite oxide active materials lead to high durability and output characteristics [0049]. As a result, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to use oxides with uniform particle size distributions in the invention of Nakabayashi to obtain these benefits.
Nakabayashi discloses an example wherein the average particle size of the first oxide is 4 µm (Table 2, see [0091] of original document), and a person of ordinary skill in the art before the effective filing date of the claimed invention would understand that a uniform distribution would result in a particle size distribution graph wherein the main peak of a particle having an average diameter of 4 µm was between 1 and 8 µm.
Regarding the second oxide, [0036 discloses that the average particle size of each of the secondary particles is 1 µm or more and 60 µm or less, with [0037[ disclosing D1/D2 ≥ 2, when the larger particle size and smaller particle size of the two types of primary particles are denoted as D1 and D2, respectively. Table 2 above discloses an example where the smaller oxide (corresponding to the claimed first oxide) is 4 µm, therefore a person of ordinary skill in the art before the effective filing date of the claimed invention would find it obvious to routinely select an average particle size of, for example, 8 µm or greater, as the size of the second lithium manganese-based oxide, satisfying D1/D2 ≥ 2. A person of ordinary skill in the art would understand that a uniform distribution for a material having an average particle size of 8µm or greater would result in a particle size distribution graph wherein the main peak overlapping the space between 6 and 24 µm. Selection of overlapping portions of ranges has been held to be a prima facie case of obviousness (see MPEP 2144.05(1))).
Claim(s) 9-10, 14-15, and 17-18 is/are rejected under 35 U.S.C. 103 as being unpatentable over Nakabayashi (JP 2016051504 A, a machine translation from Espacenet is used as an English equivalent) in view of Choi (US 20180145322 A1), and further in view of Wu (“Full concentration Gradient-Tailored Li-Rich Layered Oxides for High-Energy Lithium-Ion Batteries”, included with IDS of 04/01/2024).
Regarding claim 9, modified Nakabayashi discloses the positive electrode active material of claim 1, but does not disclose that at least one of the oxides is a core-shell particle having a concentration gradient of at least one selected from nickel and manganese from the central portion to the surface portion. However, inclusion of such core-shell structures having concentration gradients in lithium manganese oxides and the benefits associated with doing so is known in the art and would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include in the invention of modified Nakabayashi.
For example, Wu discloses lithium and manganese oxides (abstract) having both Li2MnO3 and LiMO2 phases similar to Nakabayashi (fig. 1 and pg. 4, paragraph 1 of Wu), having a concentration gradient of at least one selected from nickel and manganese from the central to the surface portion (abstract discloses linearly decreasing Mn and increasing Ni from the particle center to the surface, reading on the claimed limitation). Wu discloses that the gradient-tailored oxides exhibit notably reduced voltage decay, enhanced rate performance, improved cycle stability, and thermal stability. As a result, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include concentration gradients as described in Wu in the oxide materials of modified Nakabayashi for at least these reasons.
Wu further discloses coating layers to improve performance of lithium oxides, as pg. 1, paragraph 1 discloses surface coating layers on the lithium oxide particles, reasonably reading as a core-shell structure, to improve cycling performance and lessen voltage decay, with paragraphs 1 and 2 of pg. 2 discussing use of coating layers in gradient oxides. As a result, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include a coating layer in the oxides of modified Nakabayashi to obtain the above mentioned benefits, and doing so would result in a positive electrode active material according to the instant claim 9.
Regarding claim 10, modified Nakabayashi discloses the positive electrode active material of claim 9, wherein the core-shell particle has a gradient in which the nickel concentration increases and the manganese concentration decreases from the central portion to the surface portion (abstract of Wu).
Regarding claim 14, modified Nakabayashi discloses the positive electrode active material of claim 1, but does not disclose a barrier layer present on at least part of the surface of at least one of the oxides. However, inclusion of a barrier layer on similar lithium manganese-based oxides and the benefits of doing so are known in the art and would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention.
For example Wu discloses lithium and manganese oxides (abstract) having both Li2MnO3 and LiMO2 phases similar to Nakabayashi (fig. 1 and pg. 4, paragraph 1 of Wu). Wu further discloses coating layers to improve performance of lithium oxides, as pg. 1, paragraph 1 discloses surface coating layers on the lithium oxide particles to improve cycling performance and lessen voltage decay. As a result, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include a coating layer in the oxides of modified Nakabayashi to obtain the above mentioned benefits, and doing so would result in a positive electrode active material according to the instant claim 14.
Regarding claim 15, modified Nakabayashi discloses the positive electrode active material of claim 14, wherein the first lithium manganese-based oxide has a barrier layer present on at least a part of the surface (see claim 14 above), but Nakabayashi does not disclose that the oxide is a core shell particle having a concentration gradient of at least one selected from nickel and manganese from the core to the shell. However, such an oxide structure and the benefits thereof are known in the art and would have been obvious to implement in the oxide of modified Nakabayashi.
For example, Wu discloses lithium and manganese oxides (abstract) having both Li2MnO3 and LiMO2 phases similar to Nakabayashi (fig. 1 and pg. 4, paragraph 1 of Wu), having a concentration gradient of at least one selected from nickel and manganese from the central to the surface portion (abstract discloses linearly decreasing Mn and increasing Ni from the particle center to the surface, reading on the claimed limitation). Wu discloses that the gradient-tailored oxides exhibit notably reduced voltage decay, enhanced rate performance, improved cycle stability, and thermal stability. As a result, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include concentration gradients as described in Wu in the oxide materials of modified Nakabayashi for at least these reasons. This is also reasonably interpreted as a core-shell structure, as the gradient results in an outer layer (shell) with different composition than the inner portion (core). Making this modification to the oxide of Nakabayashi would result in an oxide wherein the barrier layer is present on the surface of the shell, satisfying the limitations of claim 15.
Regarding claim 17, modified Nakabayashi discloses the positive electrode active material of claim 14, wherein the barrier layer comprises an oxide comprising at least one selected from a metal element (Wu discloses a metal oxide for the coating layer, see pg. 1, paragraph 1, or pg. 2, paragraphs 1-2).
Regarding claim 18, modified Nakabayashi discloses the positive electrode active material of claim 14, wherein the barrier layer comprises at least one selected from a second oxide represented by formula 3 (pg. 1, paragraph 1 of Wu discloses, for example, a surface coating layer of Li-4Mn5O12, which matched the claimed formula 3 when g is 4, h is 5, i is 12, and M4 is Mn).
Claim(s) 11 and 16 is/are rejected under 35 U.S.C. 103 as being unpatentable over Nakabayashi (JP 2016051504 A, a machine translation from Espacenet is used as an English equivalent) in view of Choi (US 20180145322 A1), and Wu (“Full concentration Gradient-Tailored Li-Rich Layered Oxides for High-Energy Lithium-Ion Batteries”, included with IDS of 04/01/2024), and further in view of Kim (KR 20190093454 A, a machine translation from Espacenet is used as an English equivalent).
Regarding claim 11, as best understood based on the 35 USC 112 rejection mentioned above, modified Nakabayashi discloses the positive electrode active material of claim 1, but does not disclose that the first lithium manganese-based oxide is a core-shell particle having a concentration gradient of at least one selected from nickel and manganese from the central to the surface portion. However, inclusion of such core-shell structures having concentration gradients in lithium manganese oxides and the benefits associated with doing so is known in the art and would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include in the invention of modified Nakabayashi.
For example, Wu discloses lithium and manganese oxides (abstract) having both Li2MnO3 and LiMO2 phases similar to Nakabayashi (fig. 1 and pg. 4, paragraph 1 of Wu), having a concentration gradient of at least one selected from nickel and manganese from the central to the surface portion (abstract discloses linearly decreasing Mn and increasing Ni from the particle center to the surface, reading on the claimed limitation). Wu discloses that the gradient-tailored oxides exhibit notably reduced voltage decay, enhanced rate performance, improved cycle stability, and thermal stability. As a result, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include concentration gradients as described in Wu in the oxide materials of modified Nakabayashi for at least these reasons.
Wu further discloses coating layers to improve performance of lithium oxides, as pg. 1, paragraph 1 discloses surface coating layers on the lithium oxide particles, reasonably reading as a core-shell structure, to improve cycling performance and lessen voltage decay, with paragraphs 1 and 2 discussing use of coating layers in gradient oxides. As a result, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include a coating layer in the oxides of modified Nakabayashi to obtain the above mentioned benefits.
Wu does not discuss bimodal positive electrode active material, and therefore does not disclose a first oxide having a concentration gradient, and a second oxide having constant nickel and manganese concentrations or a lower slope than the concentration gradient of the first oxide. However, use of bimodal positive electrode active material oxides, wherein a first oxide has a concentration gradient of Nickel and/or manganese, a second oxide has a lower slope than the concentration gradient of the first oxide or a constant nickel and manganese concentration, was known in the art before the effective filing date of the claimed invention and would have been obvious to a person of ordinary skill in the art.
For example, Kim discloses a bimodal positive electrode active material highly similar to Nakabayashi wherein two lithium composite oxides, one having smaller particle sizes and one having larger particle sizes, are used [0006]. Kim further discloses that one of the oxides is a lithium complex transition metal oxide having a concentration gradient ([0014] discloses a lithium transition metal oxide having a concentration gradient with respect to nickel and manganese), and the other is a lithium complex transition metal oxide not having a concentration gradient [0034]. Kim discloses that by using a mixture of differently sized particles having a concentration gradient and not having a concentration gradient, it is possible to secure a higher capacity while ensuring thermal stability, and improve high-temperature life characteristics and high temperature storage stability. As a result, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to use a first oxide having a concentration gradient of at least one selected from nickel and manganese from the central portion to the surface, and a second oxide having a constant nickel and manganese concentration, in the invention of modified Nakabayashi, as taught by Kim. A person of ordinary skill would have been motivated to do this to obtain the benefits disclosed by Kim, and doing so would result in a positive electrode active material according to the instant claim.
Regarding claim 16, as best understood based on the 35 USC 112 rejection mentioned above, modified Nakabayashi discloses the positive electrode active material of claim 14, wherein a barrier layer is present on at least part of the surface of the second oxide (see claim 14 rejection above).
Nakabayashi does not disclose that either oxide has a concentration gradient or a constant concentration with respect to nickel or manganese concentrations. However, inclusion of such a second oxide having a concentration gradient having constant concentrations or a lower slope than that of a first oxide, and the benefits associated with doing so, is known in the art and would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to include in the invention of modified Nakabayashi.
For example, Kim discloses a bimodal positive electrode active material highly similar to Nakabayashi wherein two lithium composite oxides, one having smaller particle sizes and one having larger particle sizes, are used [0006]. Kim further discloses that one of the oxides is a lithium complex transition metal oxide having a concentration gradient ([0014] discloses a lithium transition metal oxide having a concentration gradient with respect to nickel and manganese), and the other is a lithium complex transition metal oxide not having a concentration gradient [0034]. Kim discloses that by using a mixture of differently sized particles having a concentration gradient and not having a concentration gradient, it is possible to secure a higher capacity while ensuring thermal stability, and improve high-temperature life characteristics and high temperature storage stability. As a result, it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to use a first oxide having a concentration gradient of at least one selected from nickel and manganese from the central portion to the surface, and a second oxide having a constant nickel and manganese concentration, in the invention of modified Nakabayashi, as taught by Kim. A person of ordinary skill would have been motivated to do this to obtain the benefits disclosed by Kim, and doing so would result in a positive electrode active material according to the instant claim.
Conclusion
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/ZACKARY RICHARD COCHENOUR/Examiner, Art Unit 1752
/JEFFREY T BARTON/Supervisory Patent Examiner, Art Unit 1726 10 August 2026
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