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 .
Claims 9-27 are pending in the application.
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 9-27 are 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.
Claim 9 recites “doped with lithium”, it is unclear if silicon monoxide particles coated with a carbon coating is doped with lithium or uncoated silicon monoxide is doped with lithium or the carbon coating is doped with lithium rendering the claim vague and indefinite.
Claim 9 and 10 recites “an integrated value of a relative amount of particles”. It is unclear what is the reference basis for relative amount rendering the claim vague and indefinite. Additionally, it is unclear whether it is relative to weight, volume, or particle count etc. rendering the claim vague and indefinite.
Claim 17 – 24 recites “ before the negative electrode … charged and discharged” rendering the claim vague and indefinite. It is unclear if applicant is claiming a negative electrode active material that presently exists or if the applicant is claiming a negative electrode active material having properties that existed at an earlier stage before charging and discharging. If the claim is directed towards latter, it would be an intermediate state of the electrode active material rather than its current form. If so, the applicant would be claiming a material property of an intermediate product using a product by process claim and does not have patentable weight.
Claims 10 - 27 are similarly rejected as they are dependent on claim 9.
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.
Claims 9, 10, 11, 12, 13, 14, 15, 16, 26, and 27 are rejected under 35 U.S.C. 103 as being unpatentable over Takumi (JP 2017-199657, for prior art discussion please see attached machine translation) in view of Fukui (US 20090305129 A1).
As set forth in MPEP 2144.05, in the case where the claimed range “overlap or lie inside ranges disclosed by the prior art”, a prima facie case of obviousness exists, 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).
Regarding claim 9, Takumi discloses a negative electrode active material, comprising silicon monoxide particles (SiOx: 0.5≤ x≤1.6) coated with a carbon coating and doped with lithium (para. 0013, 0029). Takumi further discloses silicon monoxide particles satisfy D50 1.0 μm or more and 15 μm or less (para. 0065) and the proportion of the particles having a particle diameter 1.0 μ m or less is preferably 1% or less (para. 0044).
Takumi fails to disclose integrated value of a relative amount of particles having a particles size of 5.0 μ m or less is 20% or less.
The claim limitation “integrated value of a relative amount of particles having a particles size of 5 μm or less is 20% or less” is being interpreted as referring to the cumulative volume percentage of particles smaller than 5 μm, which is equivalent to 20% or less of particles are smaller than 5 μm.
Fukui discloses a negative electrode comprising of silicon particles and/or silicon alloy particles (abstract, para. 0014) having a particle size distribution in which D10 of 3 μm or greater and D90 is 30 μm or less. Fukui further discloses in an embodiment silicon particles having an average particle size of 15 μm, and the particle size distribution of D10 was 8 μm, and D50 was 15 μm (para. 0084). Therefore, the D10 of 8 μm meets the claim limitation of integrated value of a relative amount of particles having a particles size of 5 μm or less is 20% or less since a D10 refers to 10% of the particles have a diameter of 8 μm or less. The content of particles of 5 μm or less would then be less than 10%, overlapping with the presently claimed range.
Fukui further discloses when the particle size distribution of the silicon/silicon alloy particles is controlled to be narrow in this way so that the particle sizes of the silicon/silicon alloy particles are uniform, the local degradation (expansion) of the silicon/silicon alloy particles can be prevented. (para. 0026). Therefore, the effect of improving the charge-discharge cycle performance and the effect of preventing the expansion of the silicon/silicon alloy particles can be exerted more effectively (para. 0026).
It would have been obvious to one of ordinary skill in the art before effective filling date of the claimed invention to modify the silicon monoxide particles of Takumi to have particles size distribution as taught by Fukui. One of ordinary skill in the art would have been motivated to modify the silicon monoxide of Takumi as taught by Fukui to improving the charge-discharge cycle performance and preventing the particle expansion.
Regarding claim 10, Takumi fails to discloses silicon monoxide particles satisfy that the integrated value of the relative amount of particles having a particles size of 5 μ m or less is 10% or less.
The claim limitation “integrated value of a relative amount of particles having a particles size of 5 μm or less is 10% or less” is being interpreted as referring to the cumulative volume percentage of particles smaller than 5 μm, which is equivalent to 10% or less of its particles are smaller than 5 μm.
Fukui discloses in an embodiment silicon particles having an average particle size of 15 μm, and the particle size distribution of D10 was 8 μm (para. 0084). Therefore, the D10 of 8 μm meets the claim limitation of integrated value of a relative amount of particles having a particles size of 5 μm or less is 20% or less since a D10 refers to 10% of the particles have a diameter of 8 μm or less. The content of particles of 5 μm or less would then be less than 10%, overlapping with the presently claimed range.( see MPEP 2144.05 (I))
One of ordinary skill in the art would have been motivated to modify the silicon monoxide particles of Takumi as taught by Fukui to improving the charge-discharge cycle performance and preventing the particle expansion.
Regarding claim 11, Takumi discloses the silicon monoxide particles at accumulative 99.9% particle size distribution defined by D99.9 is 20 μ m or less (para. 0067), thereby overlapping with the claimed range of 18.0 μ m≤D99.9≤50.0 μ m. (MPEP 2144. 05 (I)).
Regarding claim 12, As discussed above with respect to claim 10, Fukui discloses in a silicon particles having an average particle size of 15 μm, and the particle size distribution of D10 was 8 μm (para. 0084)thereby overlapping with the claimed range (MPEP 2144. 05 (I)) and Takumi discloses the silicon monoxide particles at accumulative 99.9% particle size distribution defined by D99.9 is 20 μ m or less (para. 0067), thereby overlapping with the claimed range of 18.0 μ m≤D99.9≤50.0 μ m. (MPEP 2144. 05 (I)).
Regarding claim 13, 14, 15 and 16, as discussed above the combination of Takumi and Fukui discloses a negative electrode active material comprising of silicon monoxide particles coated with carbon coating and doped with Li and satisfies the particle size distribution with respect to claims 9, 10, 11, and 12.
Takumi discloses a part of lithium present is Li2SiO3 (para. 57, 0013, 0061). Takumi further discloses when Li2SiO3 is present inside the bulk of the particles of the organosilicon compound, the battery characteristics are improved (para. 0058).
Regarding claim 26, Takumi discloses a negative electrode comprising the negative elect rode active material (para. 0048, 0104).
Regarding claim 27, Takumi discloses a lithium-ion secondary battery comprising of a negative electrode, a positive electrode, a separator and an electrolyte (para. 0004, 0095, 0104-0109).
Claims 17-24 are rejected under 35 U.S.C. 103 as being unpatentable over Takumi (JP 2017-199657, for prior art discussion please see attached machine translation) in view of Fukui (US 20090305129 A1) as applied to claim 9-16 above, and further in view of Kizaki (US PG Pub. 2018/0309160 A).
Takumi and Fukui are relied upon as discussed above.
Regarding claim 17, Takumi discloses the negative electrode active material comprising of the silicon monoxide particles coated with the carbon coating and doped with lithium has a peak derived from a Si (111) crystal plane obtained by X-ray diffraction using Cu-Ka radiation, a crystallite size corresponding to the crystal plane is 7.5 nm or less there by encompassing the claimed range of 5.0 nm or less (para. 0021, 0161).
Takumi fails to disclose a ratio A/B of an intensity A of the peak derived from the Si (111) crystal plane relative to an intensity B of a peak derived from a Li2SiO3 (111) crystal plane satisfies 0.5≤ A/B≤ 1.0.
Kizaki discloses a powder that comprises of silicon oxide containing Li2SiO3 with a volume median diameter of the powder for the negative electrode is within a range of 0.5 to 30 μm (para. 0014-0016) and having a carbon film on at least a portion of the surface of the particles (para. 0043). Kizaki discloses x-ray diffraction measurement disclosing a peak attributed to the Si(111) crystal plane (2θ of about 28.4o) and discloses a ratio of an intensity A of the peak derived from the Si (111) crystal plane relative to an intensity B of a peak derived from a Li2SiO3 (110 plane, 2θ of about 19.0o ) crystal plane satisfies P2/P1≤1.0. (para. 0038-0039). Additionally, Kizaki implicitly discloses the x-ray diffraction measurement is performed before the negative electrode active material is charged and discharged by disclosing “when an x-ray diffraction measurement using the Cu Kα ray is performed with respect to the powder”. (para. 0033)
Kizaki further discloses that the crystalline Si expands and contracts intensely during charging of the relevant lithium-ion secondary battery and the working electrode is liable to detach from the working electrode current collector and therefore electrical conduction is liable to be lost between particles constituting the working electrode. (para. 0010).Consequently, the capacity retention rate over a long-term cycle of the lithium-ion secondary battery decreases (para. 0010). Kizaki discloses when the powder having the content ratio of crystalline Si small is used for a negative electrode of a lithium-ion secondary battery, the capacity retention rate over a long-term cycle of the lithium-ion secondary battery is high (para. 0022).
It would have been obvious to one of ordinary skill in the art to optimize the relative peaks of Si in the (111) plane and Li2SiO3 in the (110) plane in Takumi to lie within the range disclosed in Kazaki et al.
While Kizaki doesn’t disclose peak derived from a Li2SiO3 (111) crystal plane, given the broad disclosure of in Kizaki of a ratio of P2/P1≤1.0, it would be expected that the ratio would be substantially identical when measured using the (111) plane rather than the (110) plane for Li2SiO3 given that both values measure the proportion of crystalline Si in the Li2SiO3.
Furthermore, Kizaki establishes the amount of crystalline Si as result-effective variable for improving the capacity retention rate over a long-term cycle of the lithium-ion secondary battery. One of ordinary skill in the art would have found it obvious to optimize the content of Li2SiO3 as measured in the (111) plane to obtain an overlapping amount of A/B ratio as claimed. One of ordinary skill in the art would have found it obvious to obtain an overlapping amount of A/B as claimed in order to keep the content ratio of crystalline Si small in the powder in order to improve the capacity retention rate over a long-term cycle of the lithium-ion secondary battery. (para. 0022, 0041-0042). Therefore, it would have been obvious to one of the ordinary skill in the art before effective filing date of the invention, to have arrived at the claimed ratio of relative intensity of peak derived from Si (111) crystal plane relative to an intensity of a peak derived from a Li2SiO3 (111) to achieve an active material with suitable characteristics. (MPEP 2144.05 II).
Regarding claim 18, 19, and 20, as discussed above the combination of Takumi and Fukui discloses a negative electrode active material comprising of silicon monoxide particles coated with carbon and doped with Li and satisfies the particle size distribution with respect to claims 9, 10, 11, and 12.
The combination of Takumi, Fukui and Kizaki with respect to claim 17 applies here and for reasons as set above.
Regarding claims 21, 22, 23 and 24, as discussed above the combination of Takumi and Fukui discloses a negative electrode active material comprising of silicon monoxide particles coated with carbon and doped with Li and satisfies the particle size distribution with respect to claims 13, 14, 15, and 16.
The combination of Takumi, Fukui and Kizaki with respect to claim 17 applies here and for reasons as set above.
Claim 25 is rejected under 35 U.S.C. 103 as being unpatentable over Takumi (JP 2017-199657, for prior art discussion please see attached machine translation) in view of Fukui (US 20090305129 A1) as applied to claim 9 above, and further in view of Awano (JP 2017-188319 for prior art discussion please see attached machine translation).
Takumi and Fukui are relied upon as discussed above.
Takumi fails to disclose the silicon monoxide particles coated with the carbon coating and doped with lithium have a true density of more than 2.3g/cc and less than 2.4g/cc.
Awano discloses a negative electrode active material (para. 0013), wherein the material comprises silicon compound - silicon oxide and the silicon compound includes Li2SiO3 (para. 57, 0013), and the particles are covered with a carbon layer (para. 0032). Awano discloses that it is preferable that the negative electrode active material have a true density of 2.20 g/cc or more and 2.50 g/cc or less (para. 0021), there by encompassing the claimed range. MPEP 2144.05 (I). Awano further discloses when the true density is within the above range, the reaction rate of the silicon compound particles and Li is within a desired range, and Li is properly inserted into the silicon compound particles. Therefore, the cycle characteristics are further improved. (para. 0022, 0075)
It would have been obvious to one of ordinary skill in the art before effective filling date of the claimed invention to modify silicon monoxide of Takumi as taught by Awano. One of ordinary skill in the art would have been motivated to modify Takumi’s negative electrode active material such that the true density of the negative electrode active material is 2.2 g/cc or more and 2.5 g/cc or less to improve the cycle characteristics.
Conclusion
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/I.M./
Iswarya Mathew Examiner, Art Unit 1788
06/17/2026
/ALEXANDRE F FERRE/ Primary Examiner, Art Unit 1788
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