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 .
Response to Amendment
Examiner notes the following amendments made to the claims:
Claim 1 and 7 amended
Claims 3-6 cancelled
New claim 10 added
Response to Arguments
Applicant’s arguments, filed 3/12/2026, with respect to the rejection(s) of claim(s) 1-2, 7-9 under 35 USC 103 have been fully considered and are persuasive. Specifically, the amendment made to specify the dispersion state of the positive electrode active mixture overcomes the previously applied prior art. Therefore, the rejection has been withdrawn. However, upon further consideration, a new ground(s) of rejection is made in view of Ota (US 20130059209 A1), which teaches a positive electrode mixture layer that meets the amended limitations, and Hasegawa (US 20190319252 A1), which teaches a confining member and pressure, which needed to be included in addition to Ota due to the amendments of the claims. New claim 10 is rejected further in view of Takeuchi et al. Therefore, there is currently not considered to be any allowable subject matter present in the claims.
Claim Rejections - 35 USC § 103
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(s) 1,2, and 7-9 is/are rejected under 35 U.S.C. 103 as being unpatentable over Ota (US 20130059209 A1) in view of Minami (US 20200136193 A1), further in view of Takahashi (US 20130309575 A1), and further in view of Hasegawa (US 20190319252 A1), with evidentiary support from Chen et al (Chen, Y., Schneider, P. and Erbe, A. (2012), Investigation of native oxide growth on zinc in different atmospheres by spectroscopic ellipsometry. Phys. Status Solidi A, 209: 846-853.).
Regarding claim 1, Ota teaches the following limitations:
A battery comprising: a stack including a positive electrode; a negative electrode (“As exemplified in FIG. 2, a nonaqueous-electrolyte battery 100 according to the present invention includes a positive-electrode body 1 for a nonaqueous-electrolyte battery (positive-electrode body 1); a negative-electrode body 2; a solid-electrolyte layer 3 disposed between the electrode bodies;” Ota [0027] Ota figure 2 clearly depicts the two electrodes and solid electrolyte layer being stacked together.)
the positive electrode comprises: a positive electrode mixture layer including a positive electrode active material and a positive solid electrolyte; (“A positive-electrode body for a nonaqueous-electrolyte battery according to the present invention includes a mixture of covered positive-electrode active-material particles and sulfide-solid-electrolyte particles.” Ota [0014])
and a positive electrode current collector in contact with the positive electrode mixture layer, (“The positive-electrode collector 4 is configured to collect current for the positive-electrode body.” Ota [0038])
the negative electrode comprises: a negative electrode current collector in contact with the negative electrode mixture layer (“The negative-electrode collector 5 is configured to collect current for the negative-electrode body.” Ota [0040])
each of the positive electrode active material and the positive solid electrolyte has a particulate shape, the positive electrode mixture layer is a single layer in which positive electrode active material particles of the positive electrode active material and positive electrode solid electrolyte particles of the positive solid electrolyte are dispersed, (“As a result of appropriately mixing the covered positive-electrode active-material particles and the solid-electrolyte particles, Li ions and electrons can be stably exchanged through the cover layers in the positive-electrode body.” Ota [0018])
Ota is silent on the following elements of claim 1:
a negative electrode including graphite and zinc;
and a confining member confining the stack,
a negative electrode mixture layer including graphite and zinc;
an oxide film is formed on the zinc,
a ratio of a mass of zinc to a sum of a mass of graphite and the mass of zinc in the negative electrode is 10 mass% or more and 60 mass% or less,
a filling density of the negative electrode mixture layer is 2.0 g/cm3 or more and 2.8 g/cm3 or less,
and a confining pressure applied to the stack by the confining member is 30 MPa or more and 50 MPa or less.
However, Minami teaches the following elements that are not found in Ota:
a negative electrode (negative electrode 1, Minami paragraph 0034, figure 1) including graphite (“The second negative electrode material is, for example, a carbon material. Examples of the carbon material include graphite and amorphous carbon.” Minami paragraph 0059) and zinc (“Examples of the negative electrode material (first negative electrode material) that absorbs lithium to form a lithium alloy include silicon, silicon compounds (e.g., oxides), tin, tin compounds (e.g., oxides), aluminum, zinc, and magnesium.” Minami paragraph 0058);
a negative electrode mixture layer including graphite and zinc; (Minami paragraphs 0058 and 0059, as shown above);
an oxide film is formed on the zinc, (This limitation would be inherently met by the zinc particles used by Minami, as oxide films are formed naturally on zinc in standard atmospheric conditions “Zn is widely used for corrosion protection under outdoor conditions. Protection is achieved by coating Zn on the surface of a reactive metal, mostly steel [1, 2]. Films of oxide are naturally formed on the surface of Zn metal under atmospheric conditions.” Chen et al page 1 paragraph 1 lines 1-5.)
a ratio of a mass of zinc to a sum of a mass of graphite and the mass of zinc in the negative electrode is 10 mass% or more and 60 mass% or less, (Minami paragraph 0059 states that the ratio of graphite to the total amount [in which the other material is Zinc] can be between 20 and 95%, which would be overlapping much of the range given in the limitation—for example, if there was 50% graphite by weight then there would be 50% zinc by weight, which is within the range given in the claim.)
The examiner takes note of the fact that the prior art ranges of 20-95% graphite (which would conversely be 5-80% zinc) encompasses the claimed range of 10% mass or more and 60% mass or less of a ratio of a mass of zinc to a sum of a mass of graphite and the mass of zinc in the negative electrode. Absent any additional and more specific information in the prior art, a prima facie case of obviousness exists. In re Peterson, 315 F.3d 1325, 1330, 65 USPQ2d 1379 (Fed. Cir. 2003). MPEP 2144.05.
Ota and Minami are considered to be analogous because they are both within the same field of secondary batteries containing non-aqueous electrolytes and including zinc in their negative electrode active materials. Therefore, it would have been obvious to one of ordinary skill before the effective filing date of the claimed invention to modify the nonaqueous secondary battery containing a positive electrode, negative electrode, and a solid electrolyte layer in between of Ota with the negative electrode material containing zinc and graphite as taught by Minami, in order to improve the overall cycle characteristics of the battery. It would be desirable to incorporate the teachings of Minami as adding graphite into a zinc-containing active material would provide increased conductivity, and the provided ratio would do so while making sure the amount of metal is not too high, as there is a large volume change upon absorbing and desorbing lithium in a metal, which can lead to electrical junction being lost if the ratio is skewed too high in regards to the proportion of metal present.
Minami and Ota are silent on the following elements of claim 1:
a filling density of the negative electrode mixture layer is 2.0 g/cm3 or more and 2.8 g/cm3 or less,
and a confining pressure applied to the stack by the confining member is 30 MPa or more and 50 MPa or less.
and a confining member confining the stack,
Takahashi teaches the following elements of claim 1 that are not found in Ota and Minami. Specifically, Takahashi teaches the desired filling density in a negative electrode containing graphite and zinc:
and a filling density of the negative electrode mixture layer is 2.0 g/cm3 or more and 2.8 g/cm3 or less. (“The packing density of the negative electrode is preferably 1.7 g/cm3 or more, more preferably 1.7 g/cm3 or more and 3.0 g/cm3 or less” Takahashi [0024] and “ Spherical zinc (produced by Kishida Chemical Co., Ltd., special grade, product number 000-87575) having an average particle diameter of 4.5 µm and prepared by an atomizing method was used as the first negative electrode active material. Artificial graphite having an average particle diameter of 23 µm and a crystal lattice constant of 0.3362 nm was used as the second negative electrode active material.” Takahashi [0062])
The examiner takes note of the fact that the prior art range of 1.7-3.0 cm3 for the packing (filling) density of the negative electrode mixture layer encompasses the claimed range of 2.0-2.8cm3 for the same parameter . Absent any additional and more specific information in the prior art, a prima facie case of obviousness exists. In re Peterson, 315 F.3d 1325, 1330, 65 USPQ2d 1379 (Fed. Cir. 2003). MPEP 2144.05.
Additionally, Takahashi is considered to be analogous to both Ota and Minami because it is also within the same field of non-aqueous electrolyte secondary batteries, and like Minami, it contains both graphite and zinc in the negative electrode. Therefore, it would have been obvious to one of ordinary skill before the effective filing date of the claimed invention to modify the zinc and graphite mixture of Minami to have the specific filling density of Takahashi in order to improve charge/discharge characteristics without sacrificing cycle properties (“A negative electrode that yields high capacity and high energy density can be prepared by increasing the packing density of the negative electrode. According to the present invention, good high-rate charge/discharge characteristic and good charge/discharge cycle property can be obtained even when the packing density of the negative electrode is increased. Takahashi [0050]). A negative electrode that yields high capacity and high energy density can be prepared by increasing the packing density of the negative electrode. According to the present invention, good high-rate charge/discharge characteristic and good charge/discharge cycle property can be obtained even when the packing density of the negative electrode is increased. This would be desirable in a secondary battery as it would improve on certain battery characteristics without sacrificing others.
Takahashi, Ota, and Minami are silent on the following elements of claim 1:
and a confining pressure applied to the stack by the confining member is 30 MPa or more and 50 MPa or less.
and a confining member confining the stack,
However, Hasegawa teaches all of the remaining elements of claim 1 that are not found in Ota, Minami, or Takahashi:
and a confining pressure applied to the stack by the confining member is 30 MPa or more and 50 MPa or less. (“a constraint pressure by the constraining member 40 is preferably no less than 0.5 MPa, more preferably no less than 1.5 MPa, and further preferably no less than 7.5 MPa. The upper limit of a constraint pressure is not specifically limited, and for example, is preferably no more than 50 MPa,” Hasegawa [0086])
and a confining member confining the stack, (constraining member 40)
Hasegawa is considered to be analogous to Ota because they are both within the same field of stacked batteries. Therefore, it would have been obvious to one of ordinary skill before the effective filing date of the claimed invention to modify the stacked battery of Ota to include the constraining member and constraining pressure of Hasegawa in order to reduce the risk of short circuit (“When heat is generated in the battery due to internal short circuits etc. and the temperature of the battery reaches the melting point of the insulating layer, the insulating layer melts, and changes its shape due to a constraint pressure, a first current collector and a second current collector are in contact with each other to short-circuit the short-circuit current shunt part, and current flows from electric elements into the short-circuit current shunt part.” Hasegawa [0016])
The additional limitations of claims 2, 7-8 would all be met without requiring any further modification or motivation:
Regarding claim 2, modified Ota teaches all of the elements of claim 1, as shown above. Ota is silent on the following elements of claim 2:
The battery according to claim 1, wherein the ratio is 20 mass% or more and 40 mass% or less.
However, Minami teaches all of the elements of claim 2 that are not found in Ota:
The battery according to claim 1, wherein the ratio is 20 mass% or more and 40 mass% or less. (Minami paragraph 0059 states that the ratio of graphite to the total amount [in which the other material is Zinc] can be between 20 and 95%, which would be overlapping much of the range given in the limitation—for example, if there was 50% graphite by weight then there would be 50% zinc by weight, which is within the range given in the claim.)
The examiner takes note of the fact that the prior art ranges of 20-95% graphite (which would conversely be 5-80% zinc) encompasses the claimed range of 20% mass or more and 40% mass or less of a ratio of a mass of zinc to a sum of a mass of graphite and the mass of zinc in the negative electrode. Absent any additional and more specific information in the prior art, a prima facie case of obviousness exists. In re Peterson, 315 F.3d 1325, 1330, 65 USPQ2d 1379 (Fed. Cir. 2003). MPEP 2144.05. Additionally, the rationale for using the provided ratio, as taught by the prior art, is shown above.
Regarding claim 7, modified Ota teaches all of the limitations of claim 1, as shown above. Ota also teaches that its negative active material is in the form of particles (“The negative-electrode body 2 contains negative-electrode active-material particles.” Ota [0039]). Therefore, by simply substituting the negative electrode active material of Ota with that of Minami, the zinc and graphite materials of Minami would be included as particles:
The battery according to claim 1, wherein the negative electrode includes a graphite particle and a zinc particle. (“The negative-electrode body 2 contains negative-electrode active-material particles.” Ota [0039]. Therefore, if the negative electrode active material containing zinc and graphite taught by Minami was used in Ota, as described above, it is disclosed that it is in particulate form, which would inherently contain particles of both graphite and zinc.)
Regarding claim 8, modified Ota teaches all of the elements of claim 1, as shown above. Ota is silent on the following elements of claim 8:
The battery according to claim 1, wherein a ratio of a mass of zinc to a sum of a mass of graphite and the mass of zinc in the negative electrode mixture layer is 10 mass% or more and 60 mass% or less.
However, Minami meets all of the elements of claim 8 that are not found in Ota:
The battery according to claim 1, wherein a ratio of a mass of zinc to a sum of a mass of graphite and the mass of zinc in the negative electrode mixture layer is 10 mass% or more and 60 mass% or less. (Minami paragraph 0059 states that the ratio of graphite to the total amount [in which the other material is Zinc] can be between 20 and 95%, which would be overlapping much of the range given in the limitation—for example, if there was 50% graphite by weight then there would be 50% zinc by weight, which is within the range given in the claim.)
The examiner takes note of the fact that the prior art ranges of 20-95% graphite (which would conversely be 5-80% zinc) encompasses the claimed range of 10% mass or more and 60% mass or less of a ratio of a mass of zinc to a sum of a mass of graphite and the mass of zinc in the negative electrode. Absent any additional and more specific information in the prior art, a prima facie case of obviousness exists. In re Peterson, 315 F.3d 1325, 1330, 65 USPQ2d 1379 (Fed. Cir. 2003). MPEP 2144.05.
Regarding claim 9, modified Ota teaches all of the elements of claim 1, as shown above. Ota is silent on the following elements of claim 9. Specifically, Ota teaches a solid electrolyte layer in between the positive and negative electrodes, but not explicitly as part of the negative electrode:
The battery according to claim 1, wherein the negative electrode further includes a solid electrolyte having lithium-ion conductivity
However, Minami teaches all of the elements of claim 9 that are not found in Ota. Specifically, Minami teaches a protective layer on the negative electrode that may comprise a solid electrolyte having lithium ion conductivity:
The battery according to claim 1, wherein the negative electrode further includes a solid electrolyte having lithium-ion conductivity (“a protective layer may be formed on a surface of the negative electrode current collector. The protective layer preferably contains a solid electrolyte, an organic substance, and/or an inorganic substance.” Minami [0064] and “The solid electrolyte preferably has lithium ion conductivity.” Minami [0065])
It would have been obvious to one of ordinary skill before the effective filing date of the claimed invention to further modify Ota to include the protective layer of Minami in order to separate the negative electrode active layer from the negative current collector, and improve the overall safety of the battery.
Claim(s) 10 is/are rejected under 35 U.S.C. 103 as being unpatentable over Ota (US 20130059209 A1) in view of Minami (US 20200136193 A1), further in view of Takahashi (US 20130309575 A1), further in view of Hasegawa (US 20190319252 A1), and further in view of Takeuchi et al (Tomonari Takeuchi et Al, Application of graphite–solid electrolyte composite anode in all-solid-state lithium secondary battery with Li2S positive electrode, Solid State Ionics, Volume 262, 2014, Pages 138-142)
Regarding claim 10, modified Ota teaches all of the elements of claim 1, as shown above. Ota is silent on the following elements of claim 10:
The battery according to claim 1, wherein the negative electrode mixture layer further includes a negative solid electrolyte,
each of the graphite, the zinc and the negative solid electrolyte has a particulate shape,
and a median diameter of negative solid electrolyte particles of the negative solid electrolyte is smaller than a median diameter of graphite particles and a median diameter of zinc particles in the negative electrode mixture layer.
However, by combining Ota, Minami and Takeuchi, all of the limitations of claim 10 would be met. Takeuchi et al teaches an all solid lithium secondary with an anode that comprises a mixture of graphite and solid electrolyte particles. Specifically, where the solid electrolyte particles are smaller than the graphite ones. As described in claim 8, the combination of Ota and Minami would render the use of particulate graphite and zinc obvious.
The battery according to claim 1, wherein the negative electrode mixture layer further includes a negative solid electrolyte, (“In the present work, we have tried to apply graphite anode in all solid-state cells with Li2S-C positive electrode for an attempt to improve the energy density of the cells. For improving the electrical contact inside the anode layer, the graphite–SE composites were prepared using the spark-plasma-sintering (SPS) process” Takeuchi page 1 column 2 lines 21-25)
each of the graphite, the zinc and the negative solid electrolyte has a particulate shape, (“The negative-electrode body 2 contains negative-electrode active-material particles.” Ota [0039]. Therefore, if the negative electrode active material containing zinc and graphite taught by Minami was used in Ota, as described above, it is disclosed that it is in particulate form, which would inherently contain particles of both graphite and zinc. “(“Fig 2 shows typical SEM micrographs of the graphite–SE composite and the graphite + SE blended powder. The graphite + SE blended powder consisted of relatively larger particles (ca.20–50 μm, assigned to graphite) and smaller ones (bca.5μm, assigned to SE).” Takeuchi page 2 column 2 lines 31-34)
and a median diameter of negative solid electrolyte particles of the negative solid electrolyte is smaller than a median diameter of graphite particles and a median diameter of zinc particles in the negative electrode mixture layer. (“Fig 2 shows typical SEM micrographs of the graphite–SE composite and the graphite + SE blended powder. The graphite + SE blended powder consisted of relatively larger particles (ca.20–50 μm, assigned to graphite) and smaller ones (bca.5μm, assigned to SE).” Takeuchi page 2 column 2 lines 31-34)
Takeuchi is considered to be analogous to Ota because it is with the same field of all-solid batteries that contain solid electrolyte introduced into the electrodes. Therefore, it would have been obvious to one of ordinary skill before the effective filing date of the claimed invention to modify Ota to include a solid electrolyte particle in the negative electrode in order to improve energy density of the electrochemical cell, as taught by Takeuchi. Additionally, it would have been obvious to have the SE particles be smaller than those of the zinc and graphite, as Takeuchi additionally teaches this in regards to the graphite, and a PHOSITA would be capable of altering the zinc particle size in order to achieve optimal results, as the teachings of the applied prior art already show that altering particle size is within the scope of routine experimentation.
Conclusion
Applicant's amendment necessitated the new ground(s) of rejection presented in this Office action. Accordingly, THIS ACTION IS MADE FINAL. See MPEP § 706.07(a). Applicant is reminded of the extension of time policy as set forth in 37 CFR 1.136(a).
A shortened statutory period for reply to this final action is set to expire THREE MONTHS from the mailing date of this action. In the event a first reply is filed within TWO MONTHS of the mailing date of this final action and the advisory action is not mailed until after the end of the THREE-MONTH shortened statutory period, then the shortened statutory period will expire on the date the advisory action is mailed, and any nonprovisional extension fee (37 CFR 1.17(a)) pursuant to 37 CFR 1.136(a) will be calculated from the mailing date of the advisory action. In no event, however, will the statutory period for reply expire later than SIX MONTHS from the mailing date of this final action.
Any inquiry concerning this communication or earlier communications from the examiner should be directed to BENJAMIN ELI KASS-MULLET whose telephone number is (571)272-0156. The examiner can normally be reached Monday-Friday 8:30am-6pm except for the first Friday of bi-week.
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/BENJAMIN ELI KASS-MULLET/Examiner, Art Unit 1752
/NICHOLAS A SMITH/Supervisory Primary Examiner, Art Unit 1752
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