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 .
Summary
Since the Office Action mailed on 14 May 2025, claim 1 has been amended, and claim 1 remains in the application and is being further examined.
New in this Office Action are 112(b) and 103 rejections necessitated by amendment.
The text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
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.
Claim 1 is rejected under 35 U.S.C. 112(b) as being indefinite for failing to particularly point out and distinctly claim the subject matter which the inventor or a joint inventor regards as the invention.
Claim 1 recites a “ton/cm” units, and it is not clear which dimension the “cm” unit corresponds to. The filed specification does not provide any further definition to the recited units. For compact prosecution purposes, this Office Action interprets “/cm” as per unit length of the disclosed first and second active materials. Appropriate correction is required for withdrawal of this rejection.
Claim Rejections - 35 USC § 103
Claim 1 is rejected under 35 U.S.C. 103 as being unpatentable over Kitaura (JP 2014127463 A) in view of Okamura et al (US 2010/0209763 A1) and Mori et al (US 2018/0226652 A1). These prior art references cited as Kitaura, Okamura and Mori, respectively, hereinafter.
Regarding claim 1, Kitaura discloses a method for producing an all solid-state battery (“a method of manufacturing a general all-solid-state battery” [0013]), the method comprising:
A first step of stacking a first active material layer (“negative electrode layer 3” [0013]) over one surface of a solid electrolyte layer (“pressing the negative electrode layer and the solid electrolyte layer in advance” [0014]) and a second active material layer over another surface of the solid electrolyte layer (“the positive electrode layer bites into the solid electrolyte layer” [0014]) to constitute a stack (“laminate, etc.” [0013]), the first active material layer having an opposing part that is opposite to the second active material layer across the solid electrolyte layer (the middle section of 3 that is overlapped by 1 and 2 in Fig. 14), and an extending part that extends beyond the opposing part in a width direction (the distal ends of 3 that is not overlapped by 1 in Fig. 14); and
a second step of pressing the stack (“The pressing pressure in the pressing step (D) can be carried out at a pressure capable of pressure-bonding the solid electrolyte layer to the electrode layer having a larger area, for example, 90 to 780 MPa or 290 to 780 MPa.” [0037]).
.
Kitaura does not disclose the first and second active material layers configured to be broken down into primary particles under a load of less than or equal to 1 ton/cm, the stack having unevenness over surfaces of the first and second active material layers, the unevenness being caused by the secondary particles; and
the second step and thereby, crushing, in the opposing part, the secondary particles being present in an interfacial portion between the first and second active material layers and the solid electrolyte, and after the first step of stacking, into the primary particles having a diameter that is at most a one fifth of a diameter of the secondary particles, wherein
after the second step, a proportion of a number of the secondary particles present in the interfacial portion within a range to which pressure is applied by the pressing is no more than 10% of a total number of the primary particles and the secondary particles,
relation of 0 < (X/Y) ≤ 0.03 is satisfied wherein X is the diameter (µm) of the primary particle, and Y is a thickness (µm) of the solid electrolyte layer,
the secondary particles present in the interfacial portion are crushed to the primary particles by the pressing to reduce the unevenness over the surfaces of the first and second active material layers in the interfacial portion, and
after the pressing, a proportion of a number of the secondary particles in a total number of particles of the active material in the extending part is larger than a proportion of a number of the secondary particles in a total number of particles of the active material in the opposing part.
However, Okamura discloses first and second active material layers (“the invention is advantageously applicable to either the positive electrode or negative electrode of a non-aqueous electrolyte secondary battery” [0066]) containing secondary particles of an active material (“The active material comprises first active material particles of Substantially spherical shape” [0036]). Okamura teaches the first and second active material layers configured to be broken down into primary particles (“second active material particles of non-spherical shape. The second active material particles are particles of the first active material particles crushed and are packed so as to close gaps between the first active material particles.” [0036]) under a load of less than or equal to 1 ton/cm (Examples 1-6 listed in Table 1 disclose a compression rupture strength range of 60 to 94 MPa. This MPa range is equivalent to a ton/cm2 range of 0.602 to 0.943 ton/cm2. The battery disclosed in Kitaura [0063] “has an arbitrary area of, for example, 1 to 300 cm 2”. The ton/cm2 range taught in Okamura is equivalent to a force applied range of 0.602 to 283 ton. Therefore, Okamura discloses a maximum range of 0.602-283 ton per at least 1 cm length of the disclosed corresponding first and second active material layers, which is a range that overlaps with the claimed load range. Additionally, Okamura discloses the positive electrode active material to comprise of “lithium cobaltate (LiCoO), modified lithium cobaltate, lithium nickelate (LiNiO), modified lithium nickelate, lithium manganate (LiMn2O), modified lithium manganate, and Such oxides in which Co, Ni or Mn is partially replaced with other transition metal element(s), typical metal (s) such as aluminum, or alkaline earth metal(s) such as magnesium.” [0073] and the negative electrode active material to comprise of “carbon materials such as various natural graphites, various artificial graphites, petroleum coke, carbon fiber, baked organic polymers, carbon nanotubes and carbon nanohorns, oxides, composite materials containing silicon or tin Such as silicides, various metals, and alloy materials” [0085] while Kitaura [0051] discloses “the active material contained in the positive electrode layer and the negative electrode layer, materials usable as electrode active materials of all solid batteries can be used. As the active material, for example, lithium cobaltate (LiCoO2), lithium nickelate (LiNiO2), lithium manganate (LiMn2O4), LiCo1 / 3Ni1 / 3Mn1 / 3O2, Li1 + xMn2-x-yMyO4 (M is Al, Mg) , Co, Fe, Ni, and Zn), different element substituted Li-Mn spinel, lithium titanate (Lix TiOy), lithium metal phosphate (LiMPO 4, M is Fe) having a composition represented by one or more metal elements selected from Transition metal oxides such as Mn, Co, or Ni), vanadium oxide (V 2 O 5) and molybdenum oxide (MoO 3), titanium sulfide (TiS 2), carbon materials such as graphite and hard carbon, lithium cobalt nitride (LiCoN), Lithium silicon oxide (LixSiyOz), lithium metal (Li), lithium alloy (LiM, M Are Sn, Si, Al, Ge, Sb, or P), lithium storage intermetallic compounds (MgxM or NySb, M is Sn, Ge or Sb, N is In, Cu or Mn)”. Therefore, based on the common active materials used as the positive electrode active material and as the negative electrode active material in both Okamura and Kitaura, Kitaura also discloses the limitation “the first and second active material layers configured to be broken down into primary particles under a load of less than or equal to 1 ton/cm”), the stack having unevenness over surfaces of the first and second active material layers, the unevenness being caused by the secondary particles (Fig. 5 showing a layer of corresponding secondary particles, versus Fig. 6 showing a layer of corresponding primary particles, shows that the particles in Fig. 5 has more unevenness over the surface); and
the second step and thereby, crushing, in the opposing part, the secondary particles being present in an interfacial portion between the first and second active material layers and the solid electrolyte, and after the first step of stacking, into the primary particles having a diameter that is at most a one fifth of a diameter of the secondary particles (Examples 1-6 in Table 1 disclose a (D0-D1)/D0 x 100% range between 20-50% in which the lower 20% datapoint overlaps with the claimed maximum of one fifth of a diameter of the secondary particles),
relation of 0 < (X/Y) ≤ 0.03 is satisfied wherein X is the diameter (µm) of the primary particle, and Y is a thickness (µm) of the solid electrolyte layer (Examples 1-6 in [0099]-[0115] disclose a second active material particle size range of 3-11 µm, and Kitaura [0059] discloses “thickness of the solid electrolyte layer before pressing is preferably 15 to 250 μm”, which combines to disclose a X/Y range of 0.01-0.73), and
the secondary particles present in the interfacial portion are crushed to the primary particles by the pressing to reduce the unevenness over the surfaces of the first and second active material layers in the interfacial portion (“the packed state A of active material, i.e., … non-spherical second active material particles were packed so as to close the gaps between the substantially spherical first active material particles, resulted in a high packing rate of the electrode mixture layer.” [0125]).
Okamura further teaches that the claimed load achieves an active material packed state in which non-spherical primary particles were packed so as to close the gaps between the substantially spherical secondary particles, which also exhibited excellent discharge capacities because the mechanical strength of the active material particles and the compressive stress were controlled favorably ([0125]-[0126]), and that primary particles of more than one fifth of a diameter of the secondary particles result in excessive crushing that does not improve the packing rate of the first and second active material particles ([0058]).
Therefore, it would have been obvious for a person of ordinary skill in the art to add to the method for producing an all solid-state battery of Kitaura, in view of Okamura, such that the first and second active material layers are configured to be broken down into primary particles under a load of less than or equal to 1 ton/cm, the stack having unevenness over surfaces of the first and second active material layers, the unevenness being caused by the secondary particles; and
the second step and thereby, crushing, in the opposing part, the secondary particles being present in an interfacial portion between the first and second active material layers and the solid electrolyte, and after the first step of stacking, into the primary particles having a diameter that is at most a one fifth of a diameter of the secondary particles,
relation of 0 < (X/Y) ≤ 0.03 is satisfied wherein X is the diameter (µm) of the primary particle, and Y is a thickness (µm) of the solid electrolyte layer, and
the secondary particles present in the interfacial portion are crushed to the primary particles by the pressing to reduce the unevenness over the surfaces of the first and second active material layers in the interfacial portion.
The person of ordinary skill would thus achieve a solid-state battery that exhibits excellent discharge capacities because the mechanical strength of the active material particles and the compressive stress were controlled favorably where the packing of the active material layers is improved by the primary particles of the claimed limitations.
Additionally, Mori discloses an all solid-state battery (“all - solid - state battery” [0033]; 100 Fig. 1) that comprises a solid electrolyte layer (“solid electrolyte layer” [0033]; 10 Fig. 1), a first active material layer that is provided for one surface of the solid electrolyte layer (30 Fig. 1; “negative electrode layer” [0033]), wherein the first active material layer has an opposing part that is opposite to the second active material layer (the portion of 30 that 20 overlaps in the height direction of the battery shown in Fig. 1) and an extending part that extends beyond the opposing part (31 Fig. 4; “heat affected region 31 of negative electrode layer 30… formed at the end portion of each of the layers” [0039]), and when a cross section of the first active material layer is observed, it is observed that a first active material that is included in the opposing part is constituted of a primary particle (3 Fig. 1; “negative-electrode active material 3” [0038]).
Mori teaches a proportion of a number of the secondary particles present in the interfacial portion within a range to which pressure is applied by the pressing is no more than 10% of a total number of the primary particles and the secondary particles (“The ratio between solid electrolyte 1 and negative-electrode active material 3 is preferably in a range of solid electrolyte: negative-electrode active material which is equal to or greater than 5:95…” [0077]. The cited ratio is the total amount of corresponding secondary particles in the whole negative electrode layer 30. Therefore in this embodiment, an amount smaller than the cited 5 parts of the “5:95” ratio corresponding to the claimed secondary particle is present in the corresponding claimed interfacial portion, and Fig. 1 provides a representation of the relative amounts between the primary and secondary particles in the negative electrode layer 30.), and
a proportion of a number of the secondary particles in a total number of particles of the active material (“particles in each of the layers are melted and aggregated (aggregated solid electrolyte 16) by the influence of heat” [0042]) in the extending part is larger than a proportion of a number of the secondary particles in a total number of particles of the active material in the opposing part (“In each of the heat affected regions 11, 21, and 31, regarding solid electrolyte 1, positive-electrode active material 2, or negative-electrode active material 3 which is included in each of the layers, the same materials are thermally solidified, and thus a dense structure in which the particle size is increased, the size of the void in each of the layers is decreased, and particle density is high is obtained.” [0039]).
Mori further teaches the active material layers with the cited features of the secondary particles improves rigidity of the layer to prevent loss of active material and secures long-term reliability of the battery with a reasonable expectation of success ([0039]), and that the cited number of the secondary particles to the total number of the secondary particles and the primary particles is sufficient to secure lithium ion conduction and electron conduction in the first active material layer ([0077]).
Therefore, it would have been obvious for a person having ordinary skill in the art before the effective filing date of the claimed invention to modify the first active material layer of the all solid-state battery of Sugiyo in view of Mori, wherein, when the cross section of the first active material layer is observed, a number of secondary particles of the first active material which are included in the extending part per unit area is larger than a number of the secondary particles of the first active material which are included in the opposing part per unit area,
wherein in an interfacial portion between the first active material layer and the solid electrolyte layer, only the primary particles are present, or the secondary particles and the primary particles are present, a number of the secondary particles being less than or equal to 10% of a total number of the secondary particles and the primary particles, and
wherein the secondary particle of the active material is present in a portion of the first active material layer, the portion being different from the interfacial portion,
in order to achieve improved rigidity of the layer that prevents loss of active material, and secures long-term reliability of the battery with a reasonable expectation of success, as well as lithium ion conduction and electron conduction in the first active material layer.
Response to Arguments
Applicant’s arguments with respect to claim 1 has been considered but are moot because the new ground 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.
Conclusion
THIS ACTION IS MADE FINAL. Applicant is reminded of the extension of time policy as set forth in 37 CFR 1.136(a).
A shortened statutory period for reply to this final action is set to expire THREE MONTHS from the mailing date of this action. In the event a first reply is filed within TWO MONTHS of the mailing date of this final action and the advisory action is not mailed until after the end of the THREE-MONTH shortened statutory period, then the shortened statutory period will expire on the date the advisory action is mailed, and any nonprovisional extension fee (37 CFR 1.17(a)) pursuant to 37 CFR 1.136(a) will be calculated from the mailing date of the advisory action. In no event, however, will the statutory period for reply expire later than SIX MONTHS from the mailing date of this final action.
Any inquiry concerning this communication or earlier communications from the examiner should be directed to CHARLENE BERMUDEZ whose telephone number is (571)272-0610. The examiner can normally be reached Mon, Thu, and Fri generally from 8 AM to 5 PM.
Examiner interviews are available via telephone, in-person, and video conferencing using a USPTO supplied web-based collaboration tool. To schedule an interview, applicant is encouraged to use the USPTO Automated Interview Request (AIR) at http://www.uspto.gov/interviewpractice.
If attempts to reach the examiner by telephone are unsuccessful, the examiner’s supervisor, Allison Bourke can be reached at (303) 297-4684. The fax phone number for the organization where this application or proceeding is assigned is 571-273-8300.
Information regarding the status of published or unpublished applications may be obtained from Patent Center. Unpublished application information in Patent Center is available to registered users. To file and manage patent submissions in Patent Center, visit: https://patentcenter.uspto.gov. Visit https://www.uspto.gov/patents/apply/patent-center for more information about Patent Center and https://www.uspto.gov/patents/docx for information about filing in DOCX format. For additional questions, contact the Electronic Business Center (EBC) at 866-217-9197 (toll-free). If you would like assistance from a USPTO Customer Service Representative, call 800-786-9199 (IN USA OR CANADA) or 571-272-1000.
/CHARLENE BERMUDEZ/Examiner, Art Unit 1721
/ALLISON BOURKE/Supervisory Patent Examiner, Art Unit 1721