DETAILED ACTION
This Office Action is responsive to the June 18th, 2026 arguments and remarks (“Remarks”).
The text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office 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and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114.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 10/20/2025 has been entered.
Response to Amendment
In response to the amendments received on June 18th, 2026:
Claims 1, 5-10, 12, 14, 17-19, and 21-24 are pending in the present application. Claims 1 and 12 are amended. Claims 2, 4, 13, and 15-16 are cancelled. Claims 22-24 are newly added.
Claim 1 is amended to:
incorporate the features recited in original Claim 2 reciting a particle size of the fine particles of 10 nm or more and 350 nm or less; and
incorporate the features of original Claim 4 reciting an average particle size of the fine particles of 30 nm or more and 100 nm or less.
Claim 12 is amended to incorporate the features of previously presented Claims 13, 15, and 16 describing a water spray mixing process, heat treatment process, and a drying process.
No new matter has been introduced. Support for the amended limitations is found in the applicant’s disclosure including the originally filed claims and specification.
Status of Claims
Claims 1-2, 4-10, 12-19, and 21 stand rejected under 35 U.S.C. 103 as described below:
Claims 1-2, 5, and 7-9 are rejected under 35 U.S.C. 103 as being unpatentable over Otsuka et al. (W.O. Pat. No. 2018043515 A1) in view of Kondo et al. (U.S. Pat. No. 20170352885 A1) (Cited in the IDS), Matsumoto et al. (U.S. Pat. No. 20140087263 A1), Uekusa et al. (W.O. Pat. No. 2017119451 A1) (US equivalent U.S. Pat. No. 20190006671 A1 is used for citation purposes) and Saka et al. (U.S. Pat. No. 20160006030 A1), and further evidenced by Koji et al. (J.P. Pat. No. 2018060759). The rejections are withdrawn.
Claim 4 is rejected under 35 U.S.C. 103 as being unpatentable over Otsuka et al. (W.O. Pat. No. 2018043515 A1) in view of Kondo et al. (U.S. Pat. No. 20170352885 A1) (Cited in the IDS), Matsumoto et al. (U.S. Pat. No. 20140087263 A1), Uekusa et al. (W.O. Pat. No. 2017119451 A1) (US equivalent U.S. Pat. No. 20190006671 A1 is used for citation purposes), and Saka et al. (U.S. Pat. No. 20160006030 A1) as applied to Claim 1, and in further view of Norio et al. (J.P. Pat. No. 2011178601 A). The rejection is withdrawn.
Claim 6 is rejected under 35 U.S.C. 103 as being unpatentable over Otsuka et al. (W.O. Pat. No. 2018043515 A1) in view of Kondo et al. (U.S. Pat. No. 20170352885 A1) (Cited in the IDS), Matsumoto et al. (U.S. Pat. No. 20140087263 A1), Uekusa et al. (W.O. Pat. No. 2017119451 A1) (US equivalent U.S. Pat. No. 20190006671 A1 is used for citation purposes), and Saka et al. (U.S. Pat. No. 20160006030 A1) as applied to Claim 5, and in further view of Kurihara et al. (J.P. Pat. No. 2017063015 A). The rejection is withdrawn.
Claim 10 is rejected under 35 U.S.C. 103 as being unpatentable over Otsuka et al. (W.O. Pat. No. 2018043515 A1) in view of Kondo et al. (U.S. Pat. No. 20170352885 A1) (Cited in the IDS), Matsumoto et al. (U.S. Pat. No. 20140087263 A1), Uekusa et al. (W.O. Pat. No. 2017119451 A1) (US equivalent U.S. Pat. No. 20190006671 A1 is used for citation purposes) and Saka et al. (U.S. Pat. No. 20160006030 A1) as further evidenced by Hayashi et al. (J.P. Pat. No. 2013125732). The rejection is withdrawn.
Claims 12 and 15-16 are rejected under 35 U.S.C. 103 as being unpatentable over Otsuka et al. (W.O. Pat. No. 2018043515 A1) in view of Uekusa et al. (W.O. Pat. No. 2017119451 A1) (US equivalent U.S. Pat. No. 20190006671 A1 is used for citation purposes), Park et al. (K.R. Pat. No. 20160050835 A), Kondo et al. (U.S. Pat. No. 20170352885 A1), Jiro et al. (J.P. Pat. No. 2017228516 A), and Shoji et al. (J.P. Pat. No. 2017131836 A) as further evidenced by Koji et al. (J.P. Pat. No. 2018060759). The rejections are withdrawn.
Claim 13 is rejected under 35 U.S.C. 103 as being unpatentable over Otsuka et al. (W.O. Pat. No. 2018043515 A1) in view of Uekusa et al. (W.O. Pat. No. 2017119451 A1) (US equivalent U.S. Pat. No. 20190006671 A1 is used for citation purposes), Park et al. (K.R. Pat. No. 20160050835 A), Kondo et al. (U.S. Pat. No. 20170352885 A1), Jiro et al. (J.P. Pat. No. 2017228516 A), and Shoji et al. (J.P. Pat. No. 2017131836 A) as applied to Claim 12 above and described below, and further in view of Nariaki et al. (K.R. Pat. No. 20160127639 A). The rejection is withdrawn.
Claim 14 is rejected under 35 U.S.C. 103 as being unpatentable over Otsuka et al. (W.O. Pat. No. 2018043515 A1) in view of Uekusa et al. (W.O. Pat. No. 2017119451 A1) (US equivalent U.S. Pat. No. 20190006671 A1 is used for citation purposes), Park et al. (K.R. Pat. No. 20160050835 A), Kondo et al. (U.S. Pat. No. 20170352885 A1), Jiro et al. (J.P. Pat. No. 2017228516 A), Shoji et al. (J.P. Pat. No. 2017131836 A), and Nariaki et al. (K.R. Pat. No. 20160127639 A) as applied to Claim 13 above, and further in view of Takeshi et al. (J.P. Pat. No. 2014194863 A). The rejection is withdrawn.
Claim 17 is rejected under 35 U.S.C. 103 as being unpatentable over Otsuka et al. (W.O. Pat. No. 2018043515 A1) in view of Uekusa et al. (W.O. Pat. No. 2017119451 A1) (US equivalent U.S. Pat. No. 20190006671 A1 is used for citation purposes), Park et al. (K.R. Pat. No. 20160050835 A), Kondo et al. (U.S. Pat. No. 20170352885 A1), Jiro et al. (J.P. Pat. No. 2017228516 A), and Shoji et al. (J.P. Pat. No. 2017131836 A) as applied to Claim 12 above, and further in view of Son et al. (U.S. Pat. No. 20140255781 A1). The rejection is withdrawn.
Claims 18 and 19 are rejected under 35 U.S.C. 103 as being unpatentable over Otsuka et al. (W.O. Pat. No. 2018043515 A1) in view of Uekusa et al. (W.O. Pat. No. 2017119451 A1) (US equivalent U.S. Pat. No. 20190006671 A1 is used for citation purposes), Park et al. (K.R. Pat. No. 20160050835 A), Kondo et al. (U.S. Pat. No. 20170352885 A1), Jiro et al. (J.P. Pat. No. 2017228516 A), and Shoji et al. (J.P. Pat. No. 2017131836 A) as applied to Claim 12 above, and further in view of Ohie et al. (J.P. Pat. No. 2011519132 A). The rejections are withdrawn.
Claim 21 is rejected under 35 U.S.C. 103 as being unpatentable over Otsuka et al. (W.O. Pat. No. 2018043515 A1) in view of Kondo et al. (U.S. Pat. No. 20170352885 A1) (Cited in the IDS), Matsumoto et al. (U.S. Pat. No. 20140087263 A1), Uekusa et al. (W.O. Pat. No. 2017119451 A1) (US equivalent U.S. Pat. No. 20190006671 A1 is used for citation purposes) and Saka et al. (U.S. Pat. No. 20160006030 A1) as applied to Claim 1 above, and further in view of Tomura (U.S. Pat. No. 20130309580 A1). The rejection is withdrawn.
Response to Arguments
Applicant’s arguments filed June 18th, 2026 have been fully considered as further described below:
Applicant’s arguments are based on the claims as amended. Regarding Claim 4 (limitations were moved to Claim 1), applicant argues against the reliance of reference Norio et al. for the claim limitations reciting an average particle size or diameter of the fine particles of 30 nm or more and 100 nm or less (see pgs. 11-14 of the “Remarks”). Applicant’s arguments with respect to Claim 1 (as related to reference Norio et al.) have been considered but are moot because the new grounds of rejection does not rely on any reference applied in the prior rejection of record for any teaching or matter specifically challenged in the argument.
Further, applicant argues that reference Matsumoto discloses fine particles preferably having a particle diameter of not more than 20 nm ([0088]) (see pg. 13 of the “Remarks”), while Claim 4 requires an average particle size of the fine particles of 30 nm or more and 100 nm or less. Therefore, applicant suggests that Matsumoto teaches away from a particle diameter within the claimed range.
1 “Obviousness can be established by combining or modifying the teachings of the prior art to produce the claimed invention where there is some teaching, suggestion, or motivation to do so. In re Kahn, 441 F.3d 977, 986, 78 USPQ2d 1329, 1335 (Fed. Cir. 2006)” (see MPEP 2143.01).
"The test for obviousness is what the combined teachings of the references would have suggested to one of ordinary skill in the art, and all teachings in the prior art must be considered to the extent that they are in analogous arts. Where the teachings of two or more prior art references conflict, the examiner must weigh the power of each reference to suggest solutions to one of ordinary skill in the art, considering the degree to which one reference might accurately discredit another. In re Young, 927 F.2d 588, 18 USPQ2d 1089 (Fed. Cir. 1991)" (see MPEP 2143.01.II).
Matsumoto et al. is not relied upon to teach said average particle size. The new grounds of rejection relies upon Cho et al. to teach an average particle diameter (size) between 50 to 1000 nm (para. 53), within and overlapping the claimed range of 30 nm or more and 100 nm or less (see MPEP § 2144.05, I). Cho et al. teaches that when the coated tungsten oxide has an average particle diameter within the recited range, the tungsten oxide particles may be uniformly adsorbed on the surface of the lithium metal oxide without agglomeration and thus, improve anti-corrosion characteristics of a positive current collector (para. 53). Therefore, a skilled artisan may consider the benefits of a larger average particle diameter of Cho et al. to outweigh the benefits of a smaller average particle diameter as disclosed by Matsumoto et al.
Further, Otsuka et al. is initially modified by Kondo et al. to include a thickness of the coating films of 1 to 200 nm as claimed. However, Kondo falls short in teaching an “average” film thickness. As the average film thickness cannot exceed the maximum or minimum thickness of the coating films, one of ordinary skill in the art would expect an average film thickness to fall within the range of 1 to 200 nm. However, Matsumoto is relied upon solely as additional support to show that said “average” film thickness is commonly observed in the field of endeavor; and that the prior art teaches an average film thickness falling within the claimed range.
Further, applicant argues that the claimed average particle size and average film thickness of the fine particles are separate limitations in which the layer thickness of Matsumoto cannot be relied upon for the claimed average particle size of the fine particles of the claimed invention (see pgs. 13-14 of the “Remarks”).
1 However, the rejection addresses the average particle size of the fine particles and the average film thickness of the coating films as distinct parameters. The secondary particles of Otsuka are modified by Kondo to include distinct fine particles and coating films of the W- and Li- containing compound, with a motivation to provide a positive electrode active material in which reduces the positive electrode resistance of the battery and improves output characteristics. The secondary particles of Otsuka et al. are further modified by Matsumoto et al. to include an “average” film thickness of 20 nm or less, within and overlapping the claimed range of 1 to 200 nm (see MPEP § 2144.05, I), with a motivation to perform the described modification to reduce the reaction resistance of the lithium metal composite oxide particles as describe above. As described above, Cho et al. is relied upon in the new grounds of rejection for a teaching of an average particle size of the fine particles. Therefore, applicant’s arguments are deemed unpersuasive as Matsumoto et al. is not relied upon to teach said average particle size.
Further, applicant presents arguments to Claim 12 as amended. Applicant individually attacks references Kondo, Jiro, Otsuka, Park, Shoji, and Nariaki and argues that said references do not teach a step of adding water by a water spray mixing process during dry mixing of the base material and the W compound; and applicant further argues a lack of an articulated reason for the proposed combination (see pgs. 16-22 of the “Remarks”).
In response to applicant's arguments against the references individually, one cannot show nonobviousness by attacking references individually where the rejections are based on combinations of references. See In re Keller, 642 F.2d 413, 208 USPQ 871 (CCPA 1981); In re Merck & Co., 800 F.2d 1091, 231 USPQ 375 (Fed. Cir. 1986).
A rationale to support a conclusion that a claim would have been obvious is that all the claimed elements were known in the prior art and one skilled in the art could have combined the elements as claimed by known methods with no change in their respective functions, and the combination would have yielded nothing more than predictable results to one of ordinary skill in the art. See KSR International Co. v. Teleflex Inc., 550 U.S., , 82 USPQ2d 1385, 1395 (2007) (see MPEP §§ 2143 and 2143.02).
"A person of ordinary skill in the art is also a person of ordinary creativity, not an automaton." KSR Int'l Co. v. Teleflex Inc., 550 U.S. 398, 421, 82 USPQ2d 1385, 1397 (2007). "[I]n many cases a person of ordinary skill will be able to fit the teachings of multiple patents together like pieces of a puzzle." Id. at 420, 82 USPQ2d 1397. Office personnel may also take into account "the inferences and creative steps that a person of ordinary skill in the art would employ" Id. at 418, 82 USPQ2d at 1396. (see MPEP 2141.03.I).
The steps of performing the dry mixing process, a water spray mixing process, and a heat treatment process are deemed obvious in view of the prior art. Reasonable motivation is provided in performing the described combination in which arrives at the claimed invention. The rejection is summarized below to show that the proposed combination teaches or suggests each and every claim limitation including the order of steps:
Primary reference Otsuka et al. teaches a dry mixing process of mixing a tungsten compound with the lithium-nickel-manganese-cobalt-containing composite oxide in an amount of 0.01 to 1.0 mass % with respect to the total mass of the composite oxide obtaining a mixture (para. 81-82), within the claimed range.
The method of Otsuka et al. is modified by Park et al. to include a mixture comprising the tungsten compound, water, and the lithium nickel manganese cobalt containing composite oxide and a heat treatment process of subjecting the mixture obtained after the water containing mixing process to a heat treatment in an atmospheric air pressure (air atmosphere) at a temperature of 250 to 500 deg. C ([0045]), lying inside the claimed range. The motivation includes to provide a method that effectively removes the solvent present in the positive electrode active material core and tungsten oxide while preventing deterioration of the core and providing an electrode structure for a secondary battery with excellent output characteristics as described above.
The method of Otsuka et al. is modified to include a step of introducing water to the mixture as taught by Park et al. by using the water spray mixing process (in an amount of 3% by mass with respect to the mass of the mixture, within the claimed range) as taught by Jiro et al.; the motivation includes to provide an alternative method of adding water/solvent uniformly to a composite oxide mixture (Jiro et al., para. 61) and to provide improved output characteristics (Jiro et al., “Evaluation Results”).
The method of Otsuka et al. is modified to include a drying process (temperature of 100 deg. C to 200 deg. C, lying inside the claimed range) following the heat treatment process as taught by Kondo et al. in which the drying process can be performed using a vacuum dry mixing apparatus as taught by Shoji et al. The motivation includes to allow for sufficient evaporation of the water to form the lithium tungstate compound and reduce degradation of battery characteristics (Kondo et al., para. 122); and to determine an apparatus and method for treating the surface of particles of a positive electrode active material for a lithium secondary battery (Shoji et al., para. 1 and 3).
As Park et al. teaches a step of removing the water solvent prior to heating and Kondo et al. teaches a washing step prior to heating/drying, it would have been obvious to perform the process steps in the order of dry mixing as taught by Otsuka et al. followed by the water spray mixing step of Jiro et al., the heat treatment step of Park et al., and the drying process of Kondo et al. to effectively incorporate the teachings and benefits of all references (see MPEP § 2144.05, I).
The method of Otsuka et al. is modified to include stirring at a peripheral speed of 21 m/s (within the claimed range of 4m/sec to 30 m/sec) for 60 minutes (within the claimed time range) as taught by Shoji et al. when water spraying (Jiro et al.) and to use the spray velocity of 0.014 ml/min per g of the mixture (equivalent to a water spray rate of 14.4 g/min per 1 kg, within the claimed range) of Nariaki et al. as the water spray velocity during the water spray mixing process (as modified by Jiro et al.). Shoji et al. teaches damage to the surface of the particles when stirred at higher speeds (para. 54). One of ordinary skill in the would find the teachings useful when determining a specific spray rate for application of a solution to a positive electrode active material comprising a lithium nickel manganese cobalt oxide (Nariaki et al., Example 1).
The process of Otsuka et al. is modified to further include performing the heat treatment step for 30 to 120 minutes (within the claimed range) as taught by Kondo et al. while stirring at 21 m/s (within the claimed range of 4 m/sec to 30 m/sec) as taught by Shoji et al. (See MPEP § 2144.05, I). The heating time of Kondo et al. allows the lithium compound to react with the tungsten compound for sufficient penetration (para. 120). One of ordinary skill in the art would find the teachings of Shoji et al. useful to provide a particle treatment process capable of coating a particle and providing mass productivity (Shoji et al., para. 13). Utilizing the conditions described above when coating particles reduces particle damage and improves overall yield (Shoji et al., para. 66).
The process of Otsuka et al. is modified to further include performing the drying process for 60 to 720 minutes (overlapping the claim range) as taught by Kondo et al. while stirring at the speed of 21 m/s (within the claimed range) as taught by Shoji et al. (See MPEP § 2144.05, I). The drying time of Kondo et al. allows for sufficiently evaporating the water to form the lithium tungstate compound (para. 123). One of ordinary skill in the art would find the teachings of Shoji et al. useful to provide a particle treatment process capable of coating a particle and providing mass productivity (Shoji et al., para. 13). Utilizing the conditions described above when coating particles reduces particle damage and improves overall yield (Shoji et al., para. 66).
Therefore, each and every element of the claimed invention is taught by the prior art and can be pieced together by a skilled artisan to arrive at the claimed invention; and a reasonable motivation is provided. As applicant fails to address deficiencies or nonobviousness of the references as combined, the provided arguments are deemed unpersuasive.
Further, applicant argues that the peripheral speed or water spray velocity in the water spray mixing process are not arbitrary optimizations; and have an unexpected beneficial effect (e.g., uniform dispersion of the tungsten compound, prevent crushing of the positive electrode active material) (see pgs. 20-21 of the “Remarks”).
"The fact that appellant has recognized another advantage which would flow naturally from following the suggestion of the prior art cannot be the basis for patentability when the differences would otherwise be obvious." Ex parte Obiaya, 227 USPQ 58, 60 (Bd. Pat. App. & Inter. 1985) (see MPEP 2145 (II)).
Rebuttal evidence and arguments can be presented in the specification, In re Soni, 54 F.3d 746, 750, 34 USPQ2d 1684, 1687 (Fed. Cir. 1995), by way of an affidavit or declaration under 37 CFR 1.132, e.g., Soni, 54 F.3d at 750, 34 USPQ2d at 1687; In re Piasecki, 745 F.2d 1468, 1474, 223 USPQ 785, 789-90 (Fed. Cir. 1984), or otherwise presented during prosecution. See, e.g., MPEP §§ 714 to 716 et seq. However, arguments presented by applicant cannot take the place of factually supported objective evidence. See, e.g., In re Schulze, 346 F.2d 600, 602, 145 USPQ 716, 718 (CCPA 1965); In re De Blauwe, 736 F.2d 699, 705, 222 USPQ 191, 196 (Fed. Cir. 1984) (see MPEP 2145 (II)).
As the claimed peripheral speed and water spray velocity are taught or suggested by the prior art (Kondo et al., Shoji et al., Jiro et al. as described above), the recognition of another advantage cannot be the basis for patentability. Applicant has the opportunity to provide objective evidence in the form of an affidavit or declaration; applicant must ensure that the evidence is commensurate with the scope of the claims.
Cited Prior Art
Previously Cited Otsuka et al. (W.O. Pat. No. 2018043515 A1) (“Otsuka et al.”).
Previously Cited Kondo et al. (U.S. Pat. No. 20170352885 A1) (Cited in the IDS) (“Kondo et al.”).
Previously Cited Uekusa et al. (W.O. Pat. No. 2017119451 A1) (“Uekusa et al.”)
US equivalent U.S. Pat. No. 20190006671 A1 is used for citation purposes.
Previously Cited Saka et al. (U.S. Pat. No. 20160006030 A1) (“Saka et al.”).
Previously Cited Norio et al. (J.P. Pat. No. 2011178601 A) (“Norio et al.”).
Previously Cited Kurihara et al. (J.P. Pat. No. 2017063015 A) (“Kurihara et al.”).
Previously Cited Koji et al. (J.P. Pat. No. 2018060759) (“Koji et al.”).
Previously Cited Jiro et al. (J.P. Pat. No. 2017228516 A) (“Jiro et al.”).
Previously Cited Shoji et al. (J.P. Pat. No. 2017131836 A) (“Shoji et al.”).
Previously Cited Nariaki et al. (K.R. Pat. No. 20160127639 A) (“Nariaki et al.”).
Previously Cited Takeshi et al. (J.P. Pat. No. 2014194863 A) (“Takeshi et al.”).
Previously Cited Son et al. (U.S. Pat. No. 20140255781 A1) (“Son et al.”).
Previously Cited Ohie et al. (J.P. Pat. No. 2011519132 A) (“Ohie et al.”).
Previously Cited Matsumoto et al. (U.S. Pat. No. 20140087263 A1) (“Matsumoto et al.”)
Previously Cited Park et al. (K.R. Pat. No. 20160050835 A) (“Park et al.”)
Okada et al. (U.S. Pat. No. 20190051929 A1 equivalent to JP. Pat. No. 2017228516 A) (“Okada et al.”)
Cho et al. (U.S. Pat. No. 20140099545 A1) (“Cho et al.”)
Miyazaki et al. (WO. Pat. No. 2018190374 A1) (“Miyazaki et al.”)
Claim Objections
Claim 14 is objected to because of the following informalities: Claim 14 is objected to as being dependent upon a cancelled claim (i.e., Claim 13). Appropriate correction is required.
Claim Interpretation
As the limitations from cancelled Claim 13 were incorporated into Claim 12, Claim 14 is interpreted as being dependent upon Claim 12 in view of the objection above.
Claim Rejections - 35 USC § 103
The following is a quotation of 35 U.S.C. 103 which forms the basis for all obviousness rejections set forth in this Office action:
A patent for a claimed invention may not be obtained, notwithstanding that the claimed invention is not identically disclosed as set forth in section 102, if the differences between the claimed invention and the prior art are such that the claimed invention as a whole would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to which the claimed invention pertains. Patentability shall not be negated by the manner in which the invention was made.
Claims 1, 5, 7-8, 10, and 21-23 are rejected under 35 U.S.C. 103 as being unpatentable over Otsuka et al. (W.O. Pat. No. 2018043515 A1) in view of Kondo et al. (U.S. Pat. No. 20170352885 A1) (Cited in the IDS), Matsumoto et al. (U.S. Pat. No. 20140087263 A1), Saka et al. (U.S. Pat. No. 20160006030 A1), Okada et al. (U.S. Pat. No. 20190051929 A1 equivalent to JP. Pat. No. 2017228516 A) (“Okada et al.”), and further view of Cho et al. (U.S. Pat. No. 20140099545 A1) (“Cho et al.”) and further evidenced by Koji et al. (J.P. Pat. No. 2018060759).
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Regarding Claim 1, Otsuka et al. teaches a positive electrode active material for a lithium-ion secondary battery (para. 1,4). The positive electrode active material is formed of a lithium metal composite oxide comprising nickel, manganese, and cobalt, formed of primary particles coated with a second compound containing lithium and tungsten (para. 18), analogous to a W- and Li-containing compound-coated lithium nickel manganese cobalt-containing composite oxide as claimed. The lithium nickel manganese cobalt-containing composite oxide is configured by secondary particles (2) formed with a plurality of aggregated primary particles (1). The W- and Li- containing compound may cover the entire surface or may cover at least part of the surface of the primary particles constituting the secondary particles (para. 54). The secondary particles have a visibly porous structure (Fig. 1A, para. 45). As shown in annotated Figure 1A, the secondary particle includes a visibly distinct outer layer (equivalent to an outer shell section) formed with aggregated primary particles, aggregated sections exist inside the outer shell section (formed of aggregated primary particles), and electrically connected to the outer shell section by the electrolytic solution and structural connection between the particles (Fig. 1A, para. 33, 45). Further, gaps or voids (forming a space section) exist in a dispersed manner in between the aggregated sections and around the aggregated sections inside the outer shell section as shown in annotated Figure 1A; the outer shell section is separated from the aggregated sections by the space sections (para. 33, annotated Fig. 1A).
Otsuka et al. teaches a composite oxide of a positive electrode active material having the general formula Lis1 Ni1 – x1 – y1 – z1 Cox1 Mny1 Mz1 02 + alpha (where 0 ≤ x1 ≤ 0.35, 0 ≤ y1 ≤ 0.35, 0 ≤ z1 ≤ 0.10, 0.95 < s1 < 1.30, 0 ≤ alpha ≤ 0.2, with M as element tungsten (W) and alpha = 0). It is obvious to one of ordinary skill in the art that the sum of the number of atoms of Ni, Co, Mn, and M total to 1 which is confirmed by provided Example 1 where the number of atoms of all elements of the composite oxide powder excluding Li and O2 total to 1 (para. 81). Therefore, the formula is equivalent to the claimed general formula (A): Li1+uNixMnyCozWsMtO2 (where -0.05 ≤ u ≤ 0.30, 0.2 ≤ x ≤ 1, 0 ≤ y ≤ 0.35, 0 ≤ z ≤ 0.35, M is additive element W, t = 0, and x + y + z + s + t = 1). Regarding the subscripts (u, x, y, z, s, t), (see MPEP § 2144.05, I). Otsuka et al. further teaches the composite oxide having a crystal layered structure (para. 69) in which can be a hexagonal layered rock salt structure as evident by Koji et al. (para. 13) as Koji et al. also teaches a lithium-nickel-manganese-cobalt composite oxide of similar structure (Koji et al., para. 13).
Otsuka et al. does not teach the W- and Li-containing compounds existing in a form of both fine particles and coating films with the fine particles not being containing in the coating films; a particle size of the fine particles of the W- and Li-containing compound existing on the surface of the secondary particle as determined from surface observation of the secondary particle using a scanning electron microscope is 10 nm or more and 350 nm or less.
Kondo et al. teaches a positive electrode active material for lithium-ion secondary batteries (para. 1-3). The positive electrode active material is equivalent to a W- and Li-containing compound-coated lithium nickel manganese cobalt-containing composite oxide as further described below (para. 25). A lithium tungstate compound (W- and Li-containing compound) is coated on the surface of the primary particles (para. 25). The W- and Li-containing compound exists on at least part of the surface of the primary particles constituting the secondary particles in the form of fine particles and coating films in which the fine particles are not contained in the coating films (para. 38). The fine particles of the W- and Li- containing compound existing on the surface of the secondary particle have a particle size of 1 to 500 nm. The coating films of the W- and Li- containing compound existing on the surface of the secondary particle have a film thickness of 1 to 200 nm (para. 38). The properties of the surface of the composite oxide can be determined by observation (or cross-sectional observation) using a scanning electron microscope or a transmission electron microscope (para. 67).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the secondary particles of Otsuka et al. by Kondo et al. to include the W- and Li- containing compound existing on at least part of the surface of the primary particles constituting the secondary particles in the form of fine particles and coating films in which the fine particles are not contained in the coating films; the fine particles of the W- and Li- containing compound existing on the surface of the secondary particle having a particle size of 1 to 500 nm, overlapping the claimed range of 10 nm or more and 350 nm or less, determined by observation (or cross-sectional observation) using a scanning electron microscope or a transmission electron microscope (para. 38). In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. See In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990) (see MPEP § 2144.05, I). One of ordinary skill in the art would have been motivated to perform the described modification as taught by Kondo et al. to provide a positive electrode active material in which reduces the positive electrode resistance of the battery and improves output characteristics (Kondo et al., para. 23).
Otsuka et al. does not teach an average film thickness of the coating films of the W- and Li-containing compound existing on the surface of the secondary particle as determined from cross-sectional observation of the secondary particle using a transmission electron microscope is 1 nm or more and 200 nm or less.
Matsumoto et al. teaches a positive electrode active material comprising a lithium metal composite oxide formed of primary particles and secondary particles composed of aggregated primary particles (para. 84-85). A W- and Li- containing compound layer (coating layer or film ) with an average layer thickness of not more than 20nm (20nm or less) observed using a transmission electron microscope, can be formed on the whole surface of the primary particles constituting the secondary particles in which the reaction resistance of the lithium metal composite oxide particles can be further reduced (para. 35, 92, 218, 364).
Further, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to further modify the secondary particles of Otsuka et al. by Matsumoto et al. to include an average film thickness of 20 nm or less, within and overlapping the claimed range of 1 to 200 nm (see MPEP § 2144.05, I). One of ordinary skill in the art would have been motivated to perform the described modification to reduce the reaction resistance of the lithium metal composite oxide particles as describe above.
Otsuka et al. does not explicitly teach the thickness of the outer shell section of the secondary particle being 0.1 µm or more and 1.5 µm or less.
Saka et al. teaches the thickness of a shell section (115) (outer shell section) of the positive electrode active material based on an electron microscope observation of 0.1 µm or greater and 2 µm or smaller (Fig. 4, para. 22).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the secondary particles of Otsuka et al. to include a thickness of the outer shell section between 0.1 and 2 µm as specified by Saka et al. (overlapping the claimed range of 0.1 µm or more and 1.5 µm or less) (see MPEP § 2144.05, I). One of ordinary skill in the art would have been motivated to perform the described modification to provide a specific thickness of the outer shell section as unspecified by Otsuka et al. in which provides improved input-output characteristics and durability against stress during battery usage (Saka et al., para. 22).
Otsuka et al. does not explicitly teach a porosity of the secondary particles being 10% or more and 50% or less.
Okada et al. teaches a lithium nickel manganese cobalt composite oxide for a positive electrode active material ([0059]) comprising secondary particles with a porosity measured by cross-sectional observation of preferably 4.5% to 60% ([0063]). Okada et al. teaches that when the porosity is in the above-mentioned range, the reduction effect of the positive electrode resistance can be enhanced while suppressing gelation of the paste; further, when the porosity is higher than 60%, the filling density decreases so that sometimes a sufficient battery capacity per battery's volume cannot be obtained ([0063]).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the secondary particles of Otsuka et al. to include a porosity of 4.5% to 60% as specified by Okada et al., overlapping the claimed range of 10% or more and 50% or less (see MPEP § 2144.05, I). One of ordinary skill in the art would have been motivated to perform the described modification to enhance the reduction effect of the positive electrode resistance as described above.
Otsuka et al. does not teach an average particle size or diameter of the fine particles of a W- and Li- containing compound of 30 nm or more and 100 nm or less.
Cho et al. teaches a lithium nickel cobalt manganese oxide cathode material comprising fine particles of a W- containing compound coated on a surface thereon having an average particle size of about 50 nm to 1000 nm; Cho et al. teaches that when the coated tungsten oxide has an average particle diameter within the range, the tungsten oxide particles may be uniformly adsorbed on the surface of the lithium metal oxide without agglomeration and thus, improve anti-corrosion characteristics of a positive current collector (para. 53).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to further modify the coating of Otsuka et al. to include an average particle diameter between 50 to 1000 nm as taught by Cho et al., within and overlapping the claimed range of 30 nm or more and 100 nm or less (see MPEP § 2144.05, I). One of ordinary skill in the art would have been motivated to perform the described modification to allow uniform adsorption of the W- containing compound on the surface of the lithium nickel cobalt manganese oxide cathode material, improving the anti-corrosion characteristics of a positive current collector as described above.
Regarding Claim 5, Otsuka et al. is modified by Kondo et al., Matsumoto et al., Saka et al., Okada et al., and Cho et al. teaching all limitations as applied to Claim 1 above. Otsuka et al. teaches the W- and Li- containing compound can include lithium tungstate (para. 51). Therefore, all claim limitations are met.
Regarding Claim 7, Otsuka et al. is modified by Kondo et al., Matsumoto et al., Saka et al., Okada et al., and Cho et al. teaching all limitations as applied to Claim 1 above. Otsuka et al. teaches a volume-based average particle diameter of 5 μm or more and 20 μm or less (para. 63), overlapping and within the claimed range of 3 µm or more and 10 µm or less (see MPEP § 2144.05, I). Otsuka et al. teaches an index [(d90 – d10)/average particle size] indicating the spread of particle size distribution of 0.7 or more (para. 63), touching the claimed range of 0.7 or less (see MPEP § 2144.05, I). One of ordinary skill in the art would consider the average particle size to be equivalent to the claimed “average particle size MV.”
Otsuka et al. does not clearly specify whether the average particle diameter and index is of the primary or secondary particles.
Saka et al. teaches an average particle size of the secondary particles of the positive electrode active material of 3 µm or greater and 10 µm or smaller, equivalent to the claimed range (para. 43). Saka et al. further teaches an index ((D90 – D10)/D50) that denotes the spread of the particle size distribution with D50 being the average particle size of 0.7 or less, equivalent to the claimed range (para. 44). One of ordinary skill in the art would consider the average particle size D50 to be equivalent to the claimed “average particle size MV.”
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the secondary particles of Otsuka et al. to include an average particle size of 3 µm or greater and 10 µm or smaller and an index of particle size distribution ((D90 – D10)/D50) of 0.7 or less as claimed and taught by Saka et al. One of ordinary skill in the art would have found the teachings useful to provide improved battery characteristics as Saka et al. teaches setting a small particle size distribution of 0.7 or less provides a uniform granularity of the positive electrode active material, allowing more homogeneous voltage to be applied and suppressing local degradation (para. 44). Further, the average particle size of the secondary particles of 3 µm to 10 µm provides good battery performance and greater stability (Saka et al., para. 43).
Regarding Claim 8, Otsuka et al. is modified by Kondo et al., Matsumoto et al., Saka et al., Okada et al., and Cho et al. teaching all limitations as applied to Claim 1 above.
Otsuka et al. does not teach the thickness of the outer shell section of the secondary particle being 0.1 µm or more and 1.0 µm or less.
Saka et al. teaches the thickness of a shell section (115) or outer shell section of the positive electrode active material based on an electron microscope observation of 2 µm or smaller and 0.1 µm or greater (Fig. 4, para. 22), which overlaps the claimed range of 0.1 µm or more and 1.0 µm or less.
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the secondary particles of Otsuka et al. to include a thickness of the outer shell section between 0.1 and 2 µm as specified by Saka et al., overlapping the claimed range of 0.1 µm or more and 1.0 µm or less (see MPEP § 2144.05, I). One of ordinary skill in the art would find the teachings useful in determining a specific thickness of the outer shell section which provides higher input-output characteristics and higher durability against stress during battery usage (Saka et al., para. 22).
Regarding Claim 10, Otsuka et al. is modified by Kondo et al., Matsumoto et al., Saka et al., Okada et al., and Cho et al. teaching all limitations as applied to Claim 1 above.
Otsuka et al. does not teach a BET specific surface area of 2.0 m2/g or more and 5.0 m2/g or less.
Okada et al. teaches a preferable range for the BET specific surface area of a positive electrode active material of 1 m2/g to 50 m2/g ([0065]), and provides a specific Example of a Lithium-nickel-manganese-cobalt-tungsten containing compound with specific surface area of 2.48 m2/g (Table 1). A BET specific surface area within said ranges provides sufficient contact with the electrolyte solution to obtain high output characteristics and to provide sufficient suppression of gelation ([0065]).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to further modify the positive electrode active material of Otsuka et al. to include a BET specific surface area between 1 m2/g to 50 m2/g, such as approximately 2.48 m2/g, as taught by Okada et al in which is within the claimed range of 2 m2/g or more and 5 m2/g or less. One of ordinary skill in the art would have been motivated to perform the described modification to provide sufficient contact with the electrolyte solution to obtain high output characteristics and to provide sufficient suppression of gelation as described above.
Regarding Claim 21, Otsuka et al. is modified by Kondo et al., Matsumoto et al., Saka et al., Okada et al., and Cho et al. teaching all limitations as applied to Claim 1 above. Otsuka et al. teaches a lithium-ion secondary battery comprising a positive electrode, a negative electrode, a separator, and a nonaqueous electrolyte wherein the positive electrode active material as applied to Claim 1 is used as the positive electrode active material in the positive electrode (para. 97). Therefore, all claim limitations are met.
Regarding Claim 22, Otsuka et al. is modified by Kondo et al., Matsumoto et al., Saka et al., Okada et al., and Cho et al. teaching all limitations as applied to Claim 1 above. As applied to Claim 1, the secondary particles of Otsuka et al. are modified by Matsumoto et al. to include an average film thickness of 20 nm or less, within and overlapping the claimed range of 1 to 3 nm (see MPEP § 2144.05, I). One of ordinary skill in the art would have been motivated to perform the described modification to reduce the reaction resistance of the lithium metal composite oxide particles as taught by Matsumoto et al. (para. 35, 92, 218, 364).
Regarding Claim 23, Otsuka et al. is modified by Kondo et al., Matsumoto et al., Saka et al., Okada et al., and Cho et al. teaching all limitations as applied to Claim 1 above. As applied to Claim 1, the secondary particles of Otsuka et al. are modified by Okada et al. to include a porosity of 4.5% to 60%, overlapping the claimed range of 32% or more and 50% or less (see MPEP § 2144.05, I). One of ordinary skill in the art would have been motivated to perform the described modification to enhance the reduction effect of the positive electrode resistance as described above.
Claim 6 is rejected under 35 U.S.C. 103 as being unpatentable over Otsuka et al. (W.O. Pat. No. 2018043515 A1) in view of Kondo et al. (U.S. Pat. No. 20170352885 A1) (Cited in the IDS), Matsumoto et al. (U.S. Pat. No. 20140087263 A1), Saka et al. (U.S. Pat. No. 20160006030 A1), Okada et al. (U.S. Pat. No. 20190051929 A1 equivalent to JP. Pat. No. 2017228516 A) (“Okada et al.”), and Cho et al. (U.S. Pat. No. 20140099545 A1) (“Cho et al.”) as applied to Claim 5 above, and further view of Kurihara et al. (J.P. Pat. No. 2017063015 A).
Regarding Claim 6, Otsuka et al. is modified by Kondo et al., Matsumoto et al., Saka et al., Okada et al., and Cho et al. teaching all limitations as applied to Claim 5 above.
Otsuka et al. does not teach the lithium tungstate compound having the formula 7Li2WO44H2O.
Kurihara et al. teaches a coating later such as lithium tungsten oxide with a preferred composition of lithium tungstate with the formula of 7Li2WO44H2O (para. 13).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the lithium tungstate compound of Otsuka et al. to have the formula of 7Li2WO44H2O as specified by Kurihara et al. One of ordinary skill in the art would have found the teachings useful when determining a preferred composition of lithium tungstate in a coating layer for a positive electrode active material of a nonaqueous electrolyte secondary battery (Kurihara et al., para. 13). The selection of a known material, which is based upon its suitability for the intended use, is within the ambit of one of ordinary skill in the art. See In re Leshin, 125 USPQ 416 (CCPA 1960) (see MPEP § 2144.07). Kurihara et al. further teaches that by selecting a lithium tungstate compound with the formula above, the stability of the coating layer can be increased with adverse effects of the battery eliminated (para. 14), providing reasonable motivation in performing the described modification.
Claim 9 is rejected under 35 U.S.C. 103 as being unpatentable over Otsuka et al. (W.O. Pat. No. 2018043515 A1) in view of Kondo et al. (U.S. Pat. No. 20170352885 A1) (Cited in the IDS), Matsumoto et al. (U.S. Pat. No. 20140087263 A1), Saka et al. (U.S. Pat. No. 20160006030 A1), Okada et al. (U.S. Pat. No. 20190051929 A1 equivalent to JP. Pat. No. 2017228516 A) (“Okada et al.”), and Cho et al. (U.S. Pat. No. 20140099545 A1) (“Cho et al.”) as applied to Claim 1 above, and further view of Uekusa et al. (W.O. Pat. No. 2017119451 A1) (US equivalent U.S. Pat. No. 20190006671 A1 is used for citation purposes).
Regarding Claim 9, Otsuka et al. is modified by Kondo et al., Matsumoto et al., Saka et al., Okada et al., and Cho et al. teaching all limitations as applied to Claim 1 above. As evident by Kondo et al., the tap density need only to fall within the range of commonly used positive electrode active materials (para. 86).
Otsuka et al. does not teach a tap density of 1.0 g/cm3 or more.
Uekusa et al. teaches a tap density of the positive-electrode active material of 1.7 g/cm3 or higher, lying inside the claimed range of 1.0 g/cm3 as claimed (para. 183).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the positive electrode active material taught by Otsuka et al. to include a tap density of 1.7 g/cm3 or higher as specified by Uekusa et al., within the claimed range of 1.0 g/cm3 or more (see MPEP § 2144.05, I). One of ordinary skill in the art would have been motivated to perform the described modification to provide a tap density commonly used in a positive electrode active material with a high initial discharge capacity (Uekusa et al., para. 184-185).
Claims 12 and 24 are rejected under 35 U.S.C. 103 as being unpatentable over Otsuka et al. (W.O. Pat. No. 2018043515 A1) in view of Okada et al. (U.S. Pat. No. 20190051929 A1 equivalent to JP. Pat. No. 2017228516 A) (“Okada et al.”), Park et al. (K.R. Pat. No. 20160050835 A), Kondo et al. (U.S. Pat. No. 20170352885 A1), Jiro et al. (J.P. Pat. No. 2017228516 A), and Shoji et al. (J.P. Pat. No. 2017131836 A) as further evidenced by Koji et al. (J.P. Pat. No. 2018060759, and further in view of Nariaki et al. (K.R. Pat. No. 20160127639 A).
Regarding Claim 12, Otsuka et al. teaches a method for producing (manufacturing method) a positive electrode active material for a lithium-ion secondary battery (para. 1,4). The positive electrode active material is formed of a lithium metal composite oxide comprising nickel, manganese, and cobalt, formed of primary particles coated with a second compound containing lithium and tungsten (para. 18), analogous to a W- and Li-containing compound-coated lithium nickel manganese cobalt-containing composite oxide as claimed. Otsuka et al. teaches a preparation process of preparing the lithium nickel manganese cobalt-containing composite oxide (lithium-metal composite oxides comprising nickel, manganese, and cobalt, para. 18) as a base material (para. 34). The lithium nickel manganese cobalt-containing composite oxide base material is configured by secondary particles (2) formed with a plurality of aggregated primary particles (1) (Fig. 1A, para. 45).
The secondary particles have a visibly porous structure (Fig. 1A, para. 45). As shown in annotated Figure 1A, the secondary particle includes a visibly distinct outer layer (equivalent to an outer shell section) formed with aggregated primary particles, aggregated sections exist inside the outer shell section (formed of aggregated primary particles), and electrically connected to the outer shell section by the electrolytic solution and structural connection between the particles (Fig. 1A, para. 33, 45). The electrolyte solution is in contact with the surface of the primary particles of the outer shell section and the surface of the primary particles existing inside the outer shell section, electrically connecting the primary particles inside the outer shell section to the primary particles of the outer shell section (para. 33). Further, gaps or voids (forming a space section) exist in a dispersed manner in between the aggregated sections and around the aggregated sections inside the outer shell section as shown in annotated Figure 1A; the outer shell section is separated from the aggregated sections by the space sections (para. 33, annotated Fig. 1A). A tungsten compound with a 0.01-1.0 mass % relative to the entirety of the positive electrode active substance or composite oxide can be dry mixed with the fired powder (composite oxide) forming a mixture (para. 81-82), within and overlapping the claimed range of 0.1 to 5.0 mass % (see MPEP § 2144.05, I).
Otsuka et al. teaches a composite oxide of a positive electrode active material having the general formula Lis1 Ni1 – x1 – y1 – z1 Cox1 Mny1 Mz1 02 + alpha (where 0 ≤ x1 ≤ 0.35, 0 ≤ y1 ≤ 0.35, 0 ≤ z1 ≤ 0.10, 0.95 < s1 < 1.30, 0 ≤ alpha ≤ 0.2, with M as element tungsten (W) and alpha = 0). It is obvious to one of ordinary skill in the art that the sum of the number of atoms of Ni, Co, Mn, and M total to 1 which is confirmed by provided Example 1 where the number of atoms of all elements of the composite oxide powder excluding Li and O2 total to 1 (para. 81). Therefore, the formula is equivalent to the claimed general formula (A): Li1+uNixMnyCozWsMtO2 (where -0.05 ≤ u ≤ 0.30, 0.2 ≤ x ≤ 1, 0 ≤ y ≤ 0.35, 0 ≤ z ≤ 0.35, M is additive element W, t = 0, and x + y + z + s + t = 1). Regarding the subscripts (u, x, y, z, s, t), (see MPEP § 2144.05, I). Otsuka et al. further teaches the composite oxide having a crystal layered structure (para. 69) in which can be a hexagonal layered rock salt structure as evident by Koji et al. (para. 13) as Koji et al. also teaches a lithium-nickel-manganese-cobalt composite oxide of similar structure (Koji et al., para. 13).
Otsuka et al. does not explicitly teach a porosity of the secondary particles of 10% or more and 50% or less.
Okada et al. teaches a lithium nickel manganese cobalt composite oxide for a positive electrode active material ([0059]) comprising secondary particles with a porosity measured by cross-sectional observation of preferably 4.5% to 60% ([0063]). Okada et al. teaches that when the porosity is in the above-mentioned range, the reduction effect of the positive electrode resistance can be enhanced while suppressing gelation of the paste; further, when the porosity is higher than 60%, the filling density decreases so that sometimes a sufficient battery capacity per battery's volume cannot be obtained ([0063]).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the secondary particles of Otsuka et al. to include a porosity of 4.5% to 60% as specified by Okada et al. measured by cross-sectional observation, overlapping the claimed range of 10% or more and 50% or less (see MPEP § 2144.05, I). One of ordinary skill in the art would have been motivated to perform the described modification to enhance the reduction effect of the positive electrode resistance as described above ([0063], Okada et al.).
Otsuka et al. does not teach a water spray mixing process of spraying water to the mixture in an amount of 1% by mass or more and 30% or less with respect to a total mass of the mixture while the mixture is stirred, to mix the mixture. Furthermore, Otsuka et al. does not explicitly teach a heat treatment process or a drying process meeting the claim limitations.
Park et al. teaches a method for producing a positive electrode active material ([0036]) formed of a W- and Li-containing compound coated lithium nickel manganese cobalt containing composite oxide ([0029],[0037]) comprising forming a mixture comprised of a tungsten compound, water, and a lithium nickel manganese cobalt containing composite oxide ([0045]). Park et al. further teaches a heat treatment process of subjecting the mixture obtained after the water containing mixing process to a heat treatment in an atmospheric air pressure (air atmosphere) at a temperature of 250 to 500 deg. C ([0045]). The method allows effective removal of the solvent present in the positive electrode active material core and tungsten oxide while preventing deterioration of the core; and provides an electrode structure for a secondary battery with excellent output characteristics ([0041], [0052]).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the method of Otsuka et al. to include a mixture comprising the tungsten compound, water, and the lithium nickel manganese cobalt containing composite oxide and a heat treatment process of subjecting the mixture obtained after the water containing mixing process to a heat treatment in an atmospheric air pressure (air atmosphere) at a temperature of 250 to 500 deg. C as taught by Park et al. ([0045]), lying inside the claimed range of 40 to 500 deg. C. One of ordinary skill in the art would have been motivated to perform the described modification to provide a method that effectively removes the solvent present in the positive electrode active material core and tungsten oxide while preventing deterioration of the core and providing an electrode structure for a secondary battery with excellent output characteristics as described above.
Jiro et al. teaches a water spray mixing process in which water is sprayed on the lithium metal composite oxide mixture in an amount of 3% by mass with respect to the total mass of the mixture while the mixture is stirred (Example 8), falling within the claimed range of 1% by mass or more and 30% by mass or less.
It would have been obvious to modify the method of Otsuka et al. to include a step of introducing water to the mixture as taught by Park et al. by using a water spray mixing process (in an amount of 3% by mass with respect to the mass of the mixture, within the claimed range of 1% by mass or more and 30% by mass or less) as taught by Jiro et al. One of ordinary skill in the art would have been motivated to perform the described modification to provide an alternative method of adding water/solvent uniformly to a composite oxide mixture (Jiro et al., para. 61) and to provide improved output characteristics (Jiro et al., “Evaluation Results”).
Kondo et al. teaches a lithium nickel manganese cobalt composite oxide containing a lithium tungstate coating; the composite oxide powder is washed with water and subjected to a heat treatment step and a drying process of drying the mixture obtained after the heat treatment at a preferable temperature of 100 deg. C to 200 deg. C to obtain said composite oxide.
Further, Shoji et. al. teaches a vacuum mixing dryer equivalent to a vacuum dry mixing apparatus with vacuum, drying, and mixing capabilities (para. 133).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to further modify the method of Otsuka et al. to include a drying process (temperature of 100 deg. C to 200 deg. C, lying inside the claimed range of 70 deg. C or greater and 500 deg. C or lower) following the heat treatment process as taught by Kondo et al. in which the drying process can be performed using a vacuum dry mixing apparatus as taught by Shoji et al. (See MPEP § 2144.05, I). Further, performing the drying step at the conditions above allow for sufficient evaporation of the water to form the lithium tungstate compound and reduce degradation of battery characteristics (Kondo et al., para. 122). One of ordinary skill in the art would find the teachings of Shoji et al. useful in determining an apparatus and method for treating the surface of particles of a positive electrode active material for a lithium secondary battery (Shoji et al., para. 1 and 3).
Further, as Park et al. teaches a step of removing the water solvent prior to heating and Kondo et al. teaches a washing step prior to heating/drying, it would have been obvious to perform the process steps in the order of dry mixing as taught by Otsuka et al. followed by the water spray mixing step of Jiro et al., the heat treatment step of Park et al., and the drying process of Kondo et al. to effectively incorporate the teachings and benefits of all references (see MPEP § 2144.05, I).
Otsuka et al. does not teach stirring performed at a peripheral speed of 4 m/sec or more and 30 m/sec or less while water spraying at a velocity of 0.01 ml/min or more and 0.1 ml/min or less per 1 g of the mixture. Otsuka et al. does not teach mixing for 5 minutes or longer and 120 minutes or shorter after the water spraying while stirring at the peripheral speed of 4 m/sec to 30 m/sec.
Shoji et al. teaches stirring a solution at 200 rpms equivalent to a peripheral speed of 21 m/s, falling with the claimed range of 4m/sec to 30 m/sec. The mixture was continuously stirred at 21 m/s for 60 minutes after the water spraying began, falling within the claimed time range of 60 minutes to 120 minutes (para. 133).
Further, Nariaki et al. teaches a spray rate of a coating solution of 14.4 g/min applied to 1 kg of a positive electrode active material (Example 1: Coating and heat treatment).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to further modify the method of Otsuka et al. to include stirring at a peripheral speed of 21 m/s (within the claimed range of 4m/sec to 30 m/sec) for 60 minutes (within the claimed time range of 60 minutes to 120 minutes) as taught by Shoji et al. when water spraying (as modified by Jiro et al.) and to use the spray velocity of 0.014 ml/min per g of the mixture (equivalent to a water spray rate of 14.4 g/min per 1 kg, within the claimed range of 0.01 ml/min to 0.1 ml/min) of Nariaki et al. as the water spray velocity during the water spray mixing process as modified by Jiro et al. One of ordinary skill in the would find the teachings useful when determining a specific spray rate for application of a solution to a positive electrode active material comprising a lithium nickel manganese cobalt oxide (Nariaki et al., Example 1). Shoji et al. teaches damage to the surface of the particles when stirred at higher speeds (para. 54).
As applied above, the method of Otsuka et al. is modified to include the water spray mixing process (in an amount of 3% by mass with respect to the mass of the mixture) of Jiro et al. followed by a heat treatment process (temperature of 60 to 80 deg. C) and then a drying process (temperature of 100 deg. C to 200 deg. C) as taught by Kondo et al. in which the drying process can be performed using a vacuum dry mixing apparatus as taught by Shoji et al. As described, the heat treatment process of Kondo et al., is performed at temperature of 60 to 80 deg. C, lying inside the claimed range of 40 deg. C or higher and 200 deg. C. or lower (see MPEP § 2144.05, I).
Otsuka et al. does not teach the heat treatment process being performed in a time of 15 minutes to 120 minutes while the mixture is stirred at a speed of 4 m/sec to 30 m/sec.
Kondo et al. teaches the heat treatment process being performed in a time of 30 minutes to 120 minutes (para. 120), lying inside the claim range of 15 minutes to 120 minutes (see MPEP § 2144.05, I).
Shoji et al. further teaches warming the vacuum mixer dryer while stirring a solution at 200 rpms equivalent to a peripheral speed of 21 m/s (within the claimed range of 4 m/sec to 30 m/sec) (para. 133).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the process of Otsuka et al. to further include performing the heat treatment step for 30 to 120 minutes (within the claimed range of 15 minutes to 120 minutes) as taught by Kondo et al. while stirring at 21 m/s (within the claimed range of 4 m/sec to 30 m/sec) as taught by Shoji et al. (See MPEP § 2144.05, I). The heating time of Kondo et al. allows the lithium compound to react with the tungsten compound for sufficient penetration (para. 120). One of ordinary skill in the art would find the teachings of Shoji et al. useful to provide a particle treatment process capable of coating a particle and providing mass productivity (Shoji et al., para. 13). Utilizing the conditions described above when coating particles reduces particle damage and improves overall yield (Shoji et al., para. 66).
As applied above, the method of Otsuka et al. is modified to include the water spray mixing process (in an amount of 3% by mass with respect to the mass of the mixture) of Jiro et al. followed by a heat treatment process (temperature of 60 to 80 deg. C) and then a drying process (temperature of 100 deg. C to 200 deg. C) as taught by Kondo et al. in which the drying process can be performed using a vacuum dry mixing apparatus as taught by Shoji et al. As described, the drying process of Kondo et al., is performed at temperature of 100 to 200 deg. C, lying inside the claimed range of 70 deg. C or higher and 200 deg. C. or lower. (See MPEP § 2144.05, I).
Otsuka et al. does not teach the drying process being performed in a time of 60 minutes to 240 minutes while the mixture is stirred at a speed of 4 m/sec to 30 m/sec.
Kondo et al. teaches the drying process being performed in a time of 60 minutes to 720 minutes (para. 123), overlapping the claim range of 60 minutes to 240 minutes (see MPEP § 2144.05, I).
Shoji et al. teaches warming the vacuum mixer dryer while stirring a solution at 200 rpms equivalent to a peripheral speed of 21 m/s (within the claimed range of 4 m/sec to 30 m/sec) (para. 133).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the process of Otsuka et al. to further include performing the drying process for 60 to 720 minutes (overlapping the claim range of 60 minutes to 240 minutes) as taught by Kondo et al. while stirring at a speed of 21 m/s (within the claimed range of 4 m/sec to 30 m/sec) as taught by Shoji et al. (See MPEP § 2144.05, I). The drying time of Kondo et al. allows for sufficiently evaporating the water to form the lithium tungstate compound (para. 123). One of ordinary skill in the art would find the teachings of Shoji et al. useful to provide a particle treatment process capable of coating a particle and providing mass productivity (Shoji et al., para. 13). Utilizing the conditions described above when coating particles reduces particle damage and improves overall yield (Shoji et al., para. 66).
Regarding Claim 24, Otsuka et al. is modified by Okada et al., Park et al., Kondo et al., Jiro et al., and Shoji et al. teaching all limitations as applied to Claim 12 above. As applied to Claim 12, the secondary particles of Otsuka et al. are modified by Okada et al. to include a porosity of 4.5% to 60%, overlapping the claimed range of 32% or more and 50% or less (see MPEP § 2144.05, I). One of ordinary skill in the art would have been motivated to perform the described modification to enhance the reduction effect of the positive electrode resistance as described above ([0063], Okada et al.).
Claim 14 is rejected under 35 U.S.C. 103 as being unpatentable over Otsuka et al. (W.O. Pat. No. 2018043515 A1) in view of Okada et al. (U.S. Pat. No. 20190051929 A1 equivalent to JP. Pat. No. 2017228516 A) (“Okada et al.”), Park et al. (K.R. Pat. No. 20160050835 A), Kondo et al. (U.S. Pat. No. 20170352885 A1), Jiro et al. (J.P. Pat. No. 2017228516 A), Shoji et al. (J.P. Pat. No. 2017131836 A), and Nariaki et al. (K.R. Pat. No. 20160127639 A) as applied to Claim 12 above, and further in view of Takeshi et al. (J.P. Pat. No. 2014194863 A).
Regarding Claim 14, Otsuka et al. is modified by Okada et al., Park et al., Kondo et al., Jiro et al., Shoji et al., and Nariaki et al. teaching all limitations as applied to Claim 12 above.
Otsuka et al. does not teach the water spraying being performed with a plurality of nozzles and a water spray velocity of each of the plurality of nozzles being set to 0.005 ml/min or more and 0.02 ml/min or less per 1 g of the mixture.
Takeshi et al. teaches a water spraying apparatus with plurality of nozzles and each nozzle spraying water towards the surface of an electrode material (para. 95).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to further modify the method of Otsuka et al. to include a plurality of nozzles in which water is sprayed with each nozzle having the water spray velocity taught by Nariaki et al. of 0.014 ml/min per 1 g of the mixture as applied to Claim 13 above. One of ordinary skill in the art would have found the teachings of Takeshi et al. useful in determining an optimal method of water spraying to suppress the occurrence of unevenness in the solidified state of the electrode material (Takeshi et al., para. 95); furthermore, Takeshi teaches a lithium-ion battery manufacturing apparatus and method (Takeshi et al., para. 1).
Claim 17 is rejected under 35 U.S.C. 103 as being unpatentable over Otsuka et al. (W.O. Pat. No. 2018043515 A1) in view of Okada et al. (U.S. Pat. No. 20190051929 A1 equivalent to JP. Pat. No. 2017228516 A) (“Okada et al.”), Park et al. (K.R. Pat. No. 20160050835 A), Kondo et al. (U.S. Pat. No. 20170352885 A1), Jiro et al. (J.P. Pat. No. 2017228516 A), and Shoji et al. (J.P. Pat. No. 2017131836 A) as applied to Claim 12 above, and further in view of Son et al. (U.S. Pat. No. 20140255781 A1).
Regarding Claim 17, Otsuka et al. is modified by Okada et al., Park et al., Kondo et al., Jiro et al., and Shoji et al. teaching all limitations as applied to Claim 12 above. As applied to Claim 16, the process of Otsuka et al. is modified to further include performing the drying process for 60 to 720 minutes as taught by Kondo et al. while stirring at a speed of 21 m/s as taught by Shoji et al. Regarding the claimed stir speed of 1 m/s to 20 m/s, a prima facie case of obviousness exists where the claimed ranges or amounts do not overlap with the prior art but are merely close. Titanium Metals Corp. of America v. Banner, 778 F.2d 775, 783, 227 USPQ 773, 779 (Fed. Cir. 1985) (see MPEP § 2144.05, I). As the stir speed taught by Shoji et al. is so close to the claimed range, one of ordinary skill in the art would expect the same results.
Otsuka et al. does not specifically teach a cooling process of cooling the mixture or composite oxide to 25°C in a time of 60 minutes or longer and 240 minutes or shorter while the composite oxide is stirred in a vacuum atmosphere after the drying process.
Son et al. teaches cooling a reactor comprised of a lithium composite oxide to room temperature for 4 hours equivalent to 240 minutes, within the claimed range of 60 to 240 minutes, to recover a coated lithium nickel cobalt manganese composite metal oxide after subjecting to heat or a drying process (para. 121). It is obvious to one of ordinary skill in the art that the universal room temperature is 25°C.
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the method of Otsuka et al. to further include a cooling process after the drying process to obtain the composite oxide as taught by Son et al. Specifically, the cooling process comprises cooling the mixture or composite oxide to room temperature or 25°C in a time of 240 minutes, within the claimed range of 60 to 240 minutes, as taught by Son et al. while the composite oxide is stirred at the peripheral speed of 21 m/s in the vacuum atmosphere as taught by Shoji et al as described above. One of ordinary skill in the art would find the teachings useful in determining a method of recovering a coated composite oxide (Son et al., para. 121), specifically for a positive electrode active material providing improved battery performance (para. 5).
Claims 18 and 19 are rejected under 35 U.S.C. 103 as being unpatentable over Otsuka et al. (W.O. Pat. No. 2018043515 A1) in view of Okada et al. (U.S. Pat. No. 20190051929 A1 equivalent to JP. Pat. No. 2017228516 A) (“Okada et al.”), Park et al. (K.R. Pat. No. 20160050835 A), Kondo et al. (U.S. Pat. No. 20170352885 A1), Jiro et al. (J.P. Pat. No. 2017228516 A), and Shoji et al. (J.P. Pat. No. 2017131836 A) as applied to Claim 12 above, and further in view of Ohie et al. (J.P. Pat. No. 2011519132 A).
Regarding Claim 18, Otsuka et al. is modified by Okada et al., Park et al., Kondo et al., Jiro et al., and Shoji et al. teaching all limitations as applied to Claim 12 above. As applied to Claim 12, Otsuka et al. is modified to include the vacuum dry mixing apparatus as taught by Shoji et al.
Otsuka et al. does not teach the dry mixing process being performed in a time of 5 minutes or longer and 50 minutes or shorter while the stirring is performed at a peripheral speed of 5 m/sec or more and 30 m/sec.
Ohie et al. teaches dry mixing a positive electrode active material for 30 minutes using a stirrer mixer at 200 rpms for 30 minutes equivalent to a peripheral speed of 21 m/s (Comparative Example 2).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to further modify Otsuka et al. to perform the dry mixing process in the vacuum dry mixing apparatus of Shoji et al., or stirrer mixer as taught by Ohie et al., prior to beginning the water spray mixing process. Furthermore, the teachings of Ohie et al. also specify stirring at 21 m/s (within the claimed range of 5 m/sec or more and 30 m/sec) for a time of 30 minutes (within the claimed range of 5 minutes or longer and 50 minutes or shorter) (Comparative Example 2). (See MPEP § 2144.05, I). Ohie et al. also teaches a method producing a positive electrode active material for a lithium secondary battery (para. 2). One of ordinary skill in the art would find the teachings of Ohie et al. useful in determining an optimal time and speed of a stirrer mixer to perform dry mixing of a positive electrode active material.
Regarding Claim 19, Otsuka et al. is modified by Okada et al., Park et al., Kondo et al., Jiro et al., and Shoji et al. teaching all limitations as applied to Claim 12 above. As applied to Claim 12, Otsuka et al. is modified to include the vacuum dry mixing apparatus as taught by Shoji et al. As applied to Claim 18, the dry mixing process can be performed using the vacuum dry mixing apparatus.
Conclusion
The prior art made of record and not relied upon is considered pertinent to applicant's disclosure. Miyazaki et al. (WO. Pat. No. 2018190374 A1) teaches a method of manufacturing a positive electrode active material comprising preparing a coated particle by forming a coating layer on the surface of particles comprising a lithium-containing compound in which the average thickness of the coating layer is 0.2 nm or more and 5 nm or less (para. 8).
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/C.R.D./Examiner, Art Unit 1729
/ULA C RUDDOCK/Supervisory Patent Examiner, Art Unit 1729
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