DETAILED ACTION
Claims 1-18 are presented for examination, wherein claims 1and 15 are currently amended.
The objection to claim 15 is withdrawn, as a result of the amendment to said claim.
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(d):
(d) REFERENCE IN DEPENDENT FORMS.—Subject to subsection (e), a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
The following is a quotation of pre-AIA 35 U.S.C. 112, fourth paragraph:
Subject to the following paragraph [i.e., the fifth paragraph of pre-AIA 35 U.S.C. 112], a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
Claim 18 is rejected under 35 U.S.C. 112(d) or pre-AIA 35 U.S.C. 112, 4th paragraph, as being of improper dependent form for failing to further limit the subject matter of the claim upon which it depends, or for failing to include all the limitations of the claim upon which it depends.
Regarding claim 18, which depend from newly amended independent claim 1, the limitation “at least one of (1) the positive electrode layer and the solid-state electrolyte layer and (2) the negative electrode layer and the solid-state electrolyte layer are an integrally sintered body” does not further distinguish the solid-state battery from the newly amended claim 1, which includes the newly added limitation “the solid-state battery is an integrally sintered body” (emphasis added), see further instant specification, at e.g. ¶0019.
Applicant may cancel the claim(s), amend the claim(s) to place the claim(s) in proper dependent form, rewrite the claim(s) in independent form, or present a sufficient showing that the dependent claim(s) complies with the statutory requirements.
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 text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
Claims 1-7, 9-14, and 16-18 are rejected under 35 U.S.C. 103 as being unpatentable over Kinkata et al (US 2014/0186720) in view of Ichikawa (JP 2017/135041).
Regarding newly amended independent claim 1, Kinkata teaches an entire-solid lithium ion battery comprising a solid electrolyte composition, said battery comprising:
(i) a cathode layer comprising a cathode active material, such as LiCoO2, Li(Ni,Mn,Co)O2, LiFePO4, and Li4Ti5O12; and, said solid electrolyte composition,
(ii) a solid electrolyte layer comprising said solid electrolyte composition, and
(iii) an anode layer comprising an anode active material, such as graphite, metal oxides, and materials capable of reversibly storing or releasing lithium ions, but not limited thereto; and, said solid electrolyte composition,
wherein said cathode layer, said solid electrolyte layer, and said anode layer are integrated by firing a laminate comprising—in sequence—a layer formed of a green sheet for said cathode layer , a layer containing said solid electrolyte, and a layer formed of a green sheet for said anode layer; then said firing said laminate to form a sintered body,
wherein said solid electrolyte is a cubic system garnet type composition that is preferably
Li7(La1-xBix)3Zr2O12, wherein x satisfies 0.01 ≤ x ≤ 0.2
(e.g. ¶¶ 0001, 08-21, 61-63, 76-78), reading on “solid-state battery,” said battery comprising:
(1) said cathode layer comprising said cathode active material, such as LiCoO2, Li(Ni,Mn,Co)O2, LiFePO4, and Li4Ti5O12; and, said solid electrolyte composition (e.g. supra), reading on “a positive electrode layer;”
(2) said anode layer comprising said anode active material, such as graphite, metal oxides, and materials capable of reversibly storing or releasing lithium ions, but not limited thereto (e.g. supra), reading on “a negative electrode layer;” and,
(3) said solid electrolyte layer formed between said cathode layer and said anode layer (e.g. supra), reading on “a solid-state electrolyte layer between the positive electrode layer and the negative electrode layer,”
wherein said solid electrolyte is a cubic system garnet type composition that is preferably
Li7(La1-xBix)3Zr2O12,
wherein x satisfies 0.01 ≤ x ≤ 0.2 (e.g. supra), reading on “the negative electrode layer includes…a garnet-type solid-state electrolyte.”
Kinkata teaches said anode layer comprising said anode active material, such as graphite, metal oxides, and materials capable of reversibly storing or releasing lithium ions, but not limited thereto; and, said solid electrolyte composition (e.g. supra), but does not expressly teach the limitation “the negative electrode layer includes: a negative electrode active material containing Li, M, and O, wherein M is one or more elements selected from the group consisting of W, Mo, Ta, and Zr, and a molar ratio (Li/M) of a Li content to a M content is more than 2.0.”
However, Ichikawa teaches a lithium tungsten composite oxide anode active material, wherein the theoretical capacity density of lithium tungsten composite oxide (e.g. 1500 mAh/cc) is higher than that of graphite (820 mAh/cc) and further said lithium tungsten composite oxide anode active material has excellent discharge capacity density, wherein said lithium tungsten composite oxide may be Li4WyM1−yO5, wherein 0.05 ≤ y ≤ 0.75 and M may be Mn, Zn, and Sn (e.g. ¶¶ 0009-14, 25, and 51-57).
As a result, it would have been obvious to substitute the anode active material, such as graphite, in the anode layer of Kinkata with the lithium tungsten composite oxide anode active material of Ichikawa, which may be Li4WyM1−yO5, wherein 0.05 ≤ y ≤ 0.75 and M may be Mn, Zn, and Sn, since Ichikawa teaches its lithium tungsten composite oxide anode active material has excellent discharge capacity density; and/or, since Ichikawa teaches its lithium tungsten composite oxide anode active material has a theoretical capacity density than that of graphite.
Ichikawa as modified reading on “the negative electrode layer includes: a negative electrode active material containing Li, M, and O;” wherein “M is one or more elements selected from the group consisting of W, Mo, Ta, and Zr;” and, establishing a prima facie case of obviousness of the claimed range, see also e.g. MPEP § 2144.05(I), reading on “a molar ratio (Li/M) of a Li content to a M content is more than 2.0.”
Regarding the newly added limitation “the solid-state battery is an integrally sintered body,” Kinkata teaches said cathode layer, said solid electrolyte layer, and said anode layer are integrated by firing a laminate comprising—in sequence—a layer formed of a green sheet for said cathode layer , a layer containing said solid electrolyte, and a layer formed of a green sheet for said anode layer; then said firing said laminate to form a sintered body (e.g. supra); and/or, the process order of sintering steps or sintering a laminated green body as a step does not patentably distinguish the instant invention form the art, see e.g. MPEP § 2113, see also instant specification, at e.g. ¶0019, reading on said newly added limitation.
Regarding claims 2-4, Kinkata as modified teaches the battery of claim 1, wherein said anode active material of Ichikawa is said lithium tungsten composite oxide, which may be Li4WyM1−yO5, wherein 0.05 ≤ y ≤ 0.75 and M may be Mn, Zn, and Sn (e.g. supra), reading on “the M includes W” (claim 2), and severably establishing a prima facie case of obviousness of the claimed ranges, see also e.g. MPEP § 2144.05(I), reading on “the negative electrode active material has a chemical composition represented by:
Liα1Mβ1M’γ1Oω1
wherein M’ is one or more elements selected from the group consisting of Na, K, Ca, Ti, V, Sn, Nb, Zn, Mn, Mg, Al, and Ga, 2 < α1 < 10, 0 < β1 < 1.5, α1/β1 > 2, 0 ≤ γ1 < 3, and 4 < ω1 < 9” (claim 3); and, “3 ≤ α1 ≤ 8, 0.4 ≤ β1 ≤ 1.2, 2 < α1/β1 ≤ 7, 0 ≤ γ1 ≤ 2, and 4 < ω1 ≤ 7” (claim 4).
Regarding claims 5-6 and 13, Kinkata as modified teaches the battery of claims 1 and 11, wherein said anode active material is said lithium tungsten composite oxide anode active material of Ichikawa, which may be Li4WyM1−yO5, wherein 0.05 ≤ y ≤ 0.75 and M may be Mn, Zn, and Sn (e.g. supra), but does not expressly teach the limitations “the negative electrode active material has one or more crystal structures selected from the group consisting of a low-temperature phase Li4WO5 crystal structure, a high-temperature phase Li4WO5 crystal structure, and a Li6WO6 crystal structure” (claim 5); “the negative electrode active material has a low-temperature phase Li4WO5 crystal structure or a high-temperature phase Li4WO5 crystal structure” (claim6); or “the negative electrode active material has a single-phase structure of a high-temperature phase Li4WO5 crystal structure” (claim 13).
However, Kinkata teaches a substantially identical lithium tungsten composite oxide anode active material (e.g. supra, compared with instant specification, at e.g. ¶¶ 0038, 40-41, 88-89, and 98), severably establishing a prima facie case of obviousness of the claimed limitations, see also e.g. MPEP § 2112.01.
Regarding claims 7 and 9-11, Kinkata as modified teaches the battery of claims 1 and 3, wherein said solid electrolyte is said cubic system garnet type composition that is preferably
Li7(La1-xBix)3Zr2O12,
wherein x satisfies 0.01 ≤ x ≤ 0.2 (e.g. supra), reading on “the garnet-type solid-state electrolyte contains Li, La, Zr, and O” (claim 7) and severably establishing a prima facie case of obviousness of the claimed ranges, see also e.g. MPEP § 2144.05(I), reading on “garnet-type solid-state electrolyte has a chemical composition represented by:
LiαAxBIβ-yBIIyDIγ-zDIIzOω
wherein, A is one or more elements in a solid solution in an Li site of the oxide having the garnet-type crystal structure, BI is one or more elements selected from the group consisting of elements having tervalent valency among elements belonging to Groups 1 to 3 having eight-coordination with oxygen, BII is one or more elements selected from the group consisting of elements having valences other than tervalent valency among the elements belonging to Groups 1 to 3 having eight-coordination with oxygen, DI is one or more elements selected from the group consisting of elements having tetravalent valency among transition elements and elements belonging to Groups 12 to 15 having six-coordination with oxygen, DII is one or more elements selected from the group consisting of elements having valences other than tetravalent valency among the transition elements and the elements belonging to Groups 12 to 15 having six-coordination with oxygen, coordination with oxygen, 3.0 ≤ α ≤ 8.0, 2.5 ≤ β ≤ 3.5, 1.5 ≤ γ ≤ 2.5, 11 ≤ ω ≤ 13, 0 ≤ x ≤ 1.0, 0 ≤ y ≤ 1.0, and 0 ≤ z ≤ 2.2” (claim 9); 5.5 ≤ α ≤ 7.0, 2.6 ≤ β ≤ 3.4, 1.6 ≤ γ ≤ 2.4, 11 ≤ ω ≤ 12.5, 0 ≤ x ≤ 0.8, 0 ≤ y ≤ 0.8, and 0 ≤ z ≤ 2.0” (claim 10); and, “garnet-type solid-state electrolyte has a chemical composition represented by:
Liα2AxBIβ2-yBIIyDIγ2-zDIIzOω2
wherein, A is one or more elements in a solid solution in an Li site of the oxide having the garnet-type crystal structure, BI is one or more elements selected from the group consisting of elements having tervalent valency among elements belonging to Groups 1 to 3 having eight-coordination with oxygen, BII is one or more elements selected from the group consisting of elements having valences other than tervalent valency among the elements belonging to Groups 1 to 3 having eight-coordination with oxygen, DI is one or more elements selected from the group consisting of elements having tetravalent valency among transition elements and elements belonging to Groups 12 to 15 having six-coordination with oxygen, DII is one or more elements selected from the group consisting of elements having valences other than tetravalent valency among the transition elements and the elements belonging to Groups 12 to 15 having six-coordination with oxygen, 3.0 ≤ α2 ≤ 8.0, 2.5 ≤ β2 ≤ 3.5, 1.5 ≤ γ2 ≤ 2.5, 11 ≤ ω2 ≤ 13, 0 ≤ x ≤ 1.0, 0 ≤ y ≤ 1.0, and 0 ≤ z ≤ 2.2 “ (claim 11).
Regarding claim 12, Kinkata as modified teaches the battery of claim 11, wherein said anode active material is said lithium tungsten composite oxide anode active material of Ichikawa, which may be Li4WyM1−yO5, wherein 0.05 ≤ y ≤ 0.75 and M may be Mn, Zn, and Sn (e.g. supra), severably establishing a prima facie case of obviousness of the claimed ranges, see also e.g. MPEP 2144.05(I), reading on “3 ≤ α1 ≤ 8, 0.4 ≤ β1 ≤ 1.2, 2 < α1/β1 ≤ 7, 0 ≤ γ1 ≤ 2, and 4 < ω1 ≤ 7;” and,
wherein said solid electrolyte is said cubic system garnet type composition that is preferably Li7(La1-xBix)3Zr2O12, wherein x satisfies 0.01 ≤ x ≤ 0.2 (e.g. supra), severably establishing a prima facie case of obviousness of the claimed ranges, see also e.g. MPEP 2144.05(I), reading on “5.5 ≤ α2 ≤ 7.0, 2.6 ≤ β2 ≤ 3.4, 1.6 ≤ γ2 ≤ 2.4, 11 ≤ ω2 ≤ 12.5, 0 ≤ x ≤ 0.8, 0 ≤ y ≤ 0.8, and 0 ≤ z ≤ 2.0.”
Regarding claim 14, Kinkata as modified teaches the battery of claim 13, wherein said anode active material is said lithium tungsten composite oxide anode active material of Ichikawa, which may be Li4WyM1−yO5, wherein 0.05 ≤ y ≤ 0.75 and M may be Mn, Zn, and Sn (e.g. supra), reading on “in the negative electrode active material…M is W,” and establishing a prima facie case of obviousness of the claimed range, see also e.g. MPEP 2144.05(I), reading on “in the negative electrode active material: 3.8≤α1/β1≤6.5;” and,
wherein said solid electrolyte is said cubic system garnet type composition that is preferably Li7(La1-xBix)3Zr2O12, wherein x satisfies 0.01 ≤ x ≤ 0.2 (e.g. supra), reading on “in the garnet-type solid-state electrolyte: x=0, or the A contains Ga and 0 < x ≤ 1.0.”
Regarding claim 16, Kinkata as modified teaches the battery of claim 1, wherein solid electrolyte layer comprises said solid electrolyte composition, wherein said solid electrolyte is said cubic system garnet type composition (e.g. supra), reading on “the solid-state electrolyte layer contains a garnet-type solid-state electrolyte.”
Regarding claim 17, Kinkata as modified teaches the battery of claim 1, wherein said cathode layer comprises said cathode active material, such as LiCoO2, Li(Ni,Mn,Co)O2, LiFePO4, and Li4Ti5O12 (e.g. supra); and, said anode layer comprises said anode active material is said lithium tungsten composite oxide anode active material of Ichikawa, which may be Li4WyM1−yO5, wherein 0.05 ≤ y ≤ 0.75 and M may be Mn, Zn, and Sn (e.g. supra), but does not expressly teach said cathode active materials within said cathode layer and said anode active material within said anode layer being “capable of occluding and releasing lithium ions” in the limitation “the positive electrode layer and the negative electrode layer are layers capable of occluding and releasing lithium ions.”
However, Kinkata teaches at least one substantially identical cathode active material (e.g. supra, compared with instant specification, at e.g. ¶0117) and at least one substantially identical anode active material (e.g. supra, compared with instant specification, at e.g. ¶¶ 0020-41), establishing a prima facie case of obviousness of the claimed limitation, see further e.g. MPEP § 2112.01.
Regarding claim 18, Kinkata as modified teaches the battery of claim 1, wherein said cathode layer, said solid electrolyte layer, and said anode layer are integrated to form said sintered body (e.g. supra), reading on “at least one of (1) the positive electrode layer and the solid-state electrolyte layer and (2) the negative electrode layer and the solid-state electrolyte layer are an integrally sintered body.”
Claims 8 and 15 are rejected under 35 U.S.C. 103 as being unpatentable over Kinkata et al (US 2014/0186720) in view of Ichikawa (JP 2017/135041), as provided supra, and further in view of Yan e al (WO 2020/199755, citations to US 2022/0131153).
Regarding claims 8 and 15, Kinkata as modified teaches the battery of claims 7 and 13, as provided supra, wherein said anode active material is said lithium tungsten composite oxide anode active material of Ichikawa, which may be Li4WyM1−yO5, wherein 0.05 ≤ y ≤ 0.75 and M may be Mn, Zn, and Sn (e.g. supra), reading on “in the negative electrode active material…M is W,” and establishing a prima facie case of obviousness of the claimed range, see also e.g. MPEP 2144.05(I), reading on “in the negative electrode active material: 3.8≤α1/β1≤6.5” (claim 15); and,
wherein said solid electrolyte is said cubic system garnet type composition that is preferably Li7(La1-xBix)3Zr2O12, wherein x satisfies 0.01 ≤ x ≤ 0.2 (e.g. supra), reading on “in the garnet-type solid-state electrolyte: x=0 or the A contains Ga and 0 < x ≤ 1.0 (claim 15), but does not expressly teach the limitations “the garnet-type solid-state electrolyte further contains W” (claim 8) or “…in the garnet-type solid-state electrolyte…the DII includes Ta and W” (claim 15).
However, Yan teaches a liquid lithium-ion battery, semi-solid-state battery, or an all-solid-state battery that may include a garnet-type solid electrolyte that may be used as a diaphragm coating material, an anode-material cladding material, a cathode-material cladding material, an anode-material additive, a cathode-material additive, an additive to polymer solid electrolyte, or a solid-liquid hybrid solid electrolyte,
wherein said garnet-type solid electrolyte is
Li7+m−n−3zAlzLa3−mA4mZr2−nB4nO12,
wherein m, n and z are all in a range of [0-1], A4 is one or more of La, Ca, Sr, Ba, or K, and B4 is at least one of Ta and W (e.g. ¶¶ 0009-11, 26, 36, 63, and 85).
However, it would have been obvious to substitute some of the Zr in the garnet solid electrolyte of Kinkata with some of at least one of Ta and W, since Yan teaches Ta and W may substitute for Zr in a garnet solid electrolyte, see also e.g. MPEP § 2144.06, reading on said limitations.
Response to Arguments
Applicant’s arguments filed June 18, 2026 have been fully considered but they are not persuasive.
First, the applicant alleges the following.
A. A POSA would have had no reasonable expectation of success, nor a motivation to try to manufacture a solid-state battery having a sintered body and the structure recited by claim 1, based on the teachings of Kintaka and Ichikawa.
In particular, the present disclosure illustrates that by setting the Li/M molar ratio of the negative electrode active material to greater than 2.0, reactions between the W-based negative electrode active material and the garnet-type solid electrolyte during sintering can be suppressed. As shown in Table 1 of the present application: when Li/M is 2.0 or less, the garnet-type solid electrolyte decomposes during sintering, whereas when Li/M is greater than 2.0, decomposition of the garnet-type solid electrolyte is suppressed. Table 2 provides additional relevant experimental data. In particular, Comparative Examples 5-7 demonstrate negative electrode utilization rates of 5% or less because side reactions occur between the negative electrode active material and the garnet-type solid electrolyte during sintering. In contrast, Examples 4, 6, and 7 – in accordance with the present claims – achieve practical utilization rates because such side reactions are suppressed. Applicant’s experimental data thus demonstrates the technical significance of having an Li/M molar ratio greater than 2; this parameter is not merely a compositional limitation, rather it is a critical condition for suppressing reactions between the negative electrode active material and the garnet-type solid electrolyte.
Prior to Applicant’s disclosure of this finding, a POSA would have expected that Li-W-based negative electrode materials would react with garnet-type solid electrolytes (such as LLZO). Accordingly, a POSA would have had reasonably expected that such combinations were unsuitable for co-firing. The Comparative Examples in the present application support this understanding. In particular: Comparative Examples 1-3 show that WO3, Li2WO4, and Li2W2O7 all react completely with LLZ and become deactivated. Furthermore, Comparative Example 4 shows that even Li4WO5 becomes deactivated when combined with NASICON, which is another solid electrolyte. These results illustrate that W-based materials generally exhibit high reactivity with garnet-type and other solid electrolytes.
Accordingly, the combination of Li4WO5 and a garnet-type solid electrolyte was not a routine or predictable choice prior to the filing of the present application. To the contrary, a POSA would have expected substantial reaction between a Li-W-based negative electrode material and a garnet-type solid electrolyte during co-firing. Thus, instead of having a reasonable expectation of success, a POSA would instead have reasonably expected failure, absent the roadmap provided by Applicant's disclosure.
The Examiner’s findings fail to rebut this conclusion. Even if Kintaka discloses a sintered solid-state battery including a garnet-type solid electrolyte, Kintaka does not teach that: 1) a Li-W-based negative electrode active material having Li/M molar ratio > 2 can be co-fired with a garnet-type solid electrolyte; 2) reactions during sintering can be suppressed; or 3) practical utilization of the negative electrode active material can be achieved after co-firing.
As demonstrated by the Comparative Examples of the present application, simply combining a Li-W-based negative electrode material with a garnet-type solid electrolyte results in decomposition of the solid electrolyte. Indeed, the Comparative Examples demonstrate that W-based materials generally exhibit high reactivity toward garnet-type and other solid electrolytes and therefore a POSA would have expected failure rather than success, when combining the teachings relied upon by the Examiner.
Thus, the asserted prior art of record fails to provide guidance that would have given a POSA any reason to select the parameters recited by claim 1, even if one accepts the proposed combination of teachings relied upon in the Office Action.
(Remarks, at e.g. 8:2-9:4, emphasis in the original.)
In response, the examiner respectfully notes that the argument is not commensurate with the scope of the art.
While Kintaka teaches difficulty in co-sintering electrolyte with active material, its inventive concept is an electrolyte composition that is capable of co-sintering electrolyte with active material. Some relevant portions of Kintaka are reproduced below for ease of reference.
[0010] In these cases, when the material for solid electrolyte is composed of a mixed phase rather than forming a single phase of an objective compound in the stage where the solid electrolyte is a powder (before becoming a sintered body) prior to the heat treatment of the mixture with the cathode active material or the anode active material, or prior to the firing of a laminate of the green sheets, various reactions with the electrode active materials can occur during the firing, and a desired solid electrolyte may not be obtained after sintering. Therefore, a single phase of cubic Li7La3Zr2O12 should be formed at least in the stage prior to sintering.
[0011] However, even if a single phase of cubic Li7La3Zr2O12 is formed in the stage prior to sintering, the severer the firing conditions for sintering as is in the existent techniques, the higher the possibility of reacting with contacting materials (cathode active material, anode active material and the like), and there is a fear that a desired material design cannot be made. Therefore, it is desired to be able to generate a sintered body of cubic system garnet type Li7La3Zr2O12 by firing at lower temperature in shorter time to suppress the reaction between these materials, however, such materials have not been developed yet.
[0012] Therefore, it is a primary object of the present invention to provide a material capable of producing a sintered body of cubic system garnet type Li7La3Zr2O12 serving as a solid electrolyte having specified ion conductivity by firing at relatively low temperature in short time.
[0013] As a result of diligent efforts in light of the aforementioned problems in the existent techniques, the inventor of the present invention found that the above object can be achieved by employing a specified composition, and accomplished the present invention.
[0014] That is, the present invention relates to the following material for solid electrolyte.
[0015] A material for solid electrolyte for use for a solid electrolyte, wherein (1) the material is an oxide containing Li, La, Zr and Bi, and (2) the oxide has a cubic system garnet crystal structure wherein La sites are partly or entirely substituted by Bi.
[0016] Preferably, a substitution amount of Bi is 1 to 20% by mol in 100% by mol of La.
[0017] In the material for a solid electrolyte, Al is preferably contained in a cubic system garnet crystal structure represented by composition formula Li7(La1-xBix)3Zr2O12 (provided that x satisfies 0.01≤x≤0.2).
…
[0020] A method for producing a solid electrolyte-containing sintered body includes firing a raw material containing the above-mentioned material for a solid electrolyte at a temperature of 900 to 1150° C. for 1 to 10 hours to obtain a sintered body.
[0021] The raw material is preferably a mixture containing the material for solid electrolyte, and a cathode active material or an anode active material.
[0022] The raw material may also be a laminate including, in sequence, a layer formed of a green sheet for cathode, a layer containing the material for solid electrolyte, and a layer formed of a green sheet for anode.
(Kintaka, at e.g. ¶¶ 0010-17 and 20-22, emphasis added.)
Further, there is no indication that the composition of the anode active material is limited. Rather, as noted above, the Kimtake teaches its inventive concept is to prevent unwanted reactions by using a specific electrolyte composition.
[0061] The raw material is not particularly limited as far as the present material is contained. For example, a mixture containing a cathode active material or an anode active material of lithium ion battery (collectively referred to as “electrode active material”) and the present material may be used as the raw material.
[0062] More particularly, for example, 1) mixed powder containing powder of the electrode active material and the powdery present material, 2) a laminated green sheet containing, in sequence, a layer formed of a green sheet for cathode, a layer containing the material for solid electrolyte, and a layer formed of a green sheet for anode, or the like may be used as the raw material.
[0063] In the case of the above 1), as the electrode active material, those similar to the electrode active materials employed in a known lithium ion battery may be used. As the cathode active material, for example, compounds of lithium and transition metal (Ni, Mn, Ti, Fe or the like) may be used. More specific examples thereof include lithium-containing metal oxides such as LiCoO2, LiMn2O4, LiNiO2, Li(Ni, Mn, Co)O2, LiFePO4, and Li4Ti5O12. As the anode active material, for example, in addition to 1) carbon-based materials such as graphite, amorphous carbon, and carbon black, 2) oxides of metal such as silicon, titanium, tin, niobium, or molybdenum, 3) materials capable of reversibly storing or releasing lithium ions such as metal lithium, lithium compounds or lithium alloys (including intermetallic compounds) may be used.
(Kintaka, at e.g. ¶¶ 0061-63, emphasis added.)
As a result, a proper prima facie case of obviousness has been established.
Second, the applicant alleges the following.
B. Ichikawa's disclosure of Li/M > 2 relates to liquid-electrolyte batteries and does not teach interactions with garnet-type solid electrolytes during co-firing.
Although Ichikawa discloses Li-W-based negative electrode active materials, Ichikawa is directed to liquid-electrolyte batteries, and consequently does not teach: 1) co-firing with garnet-type solid electrolytes; 2) interactions between Li-W-based active materials and garnet-type solid electrolytes during sintering; 3) whether garnet-type solid electrolytes decompose during co-firing; and 4) that such decomposition can be suppressed by setting a Li/M molar ratio > 2.
A POSA familiar with Ichikawa would have had no reason to extrapolate from the teachings in this reference relied upon by the Examiner, alone or further in view of Kintaka, given Ichikawa's focus on liquid-electrolyte batteries. The Office Action fails to provide any compelling argument to conclude otherwise.
(Remarks, at e.g. 9:5-6, emphasis in the original.)
In response, the examiner respectfully notes that the argument is not commensurate with the scope of the art or the scope of the Office action.
As noted supra, while Kintaka teaches difficulty in co-sintering electrolyte with active material, its inventive concept is an electrolyte composition that is capable of co-sintering electrolyte with active material. Some relevant portions of Kintaka are reproduced below for ease of reference.
Further, there is no indication that the composition of the anode active material is limited. Rather, as noted above, the Kimtake teaches its inventive concept is to prevent unwanted reactions by using a specific electrolyte composition.
Finally, the prior and instant Office actions provide proper motivation to combine, e.g. a relevant portion reproduced below for ease of reference.
Kinkata teaches said anode layer comprising said anode active material, such as graphite, metal oxides, and materials capable of reversibly storing or releasing lithium ions, but not limited thereto; and, said solid electrolyte composition (e.g. supra), but does not expressly teach the limitation “the negative electrode layer includes: a negative electrode active material containing Li, M, and O, wherein M is one or more elements selected from the group consisting of W, Mo, Ta, and Zr, and a molar ratio (Li/M) of a Li content to a M content is more than 2.0.”
However, Ichikawa teaches a lithium tungsten composite oxide anode active material, wherein the theoretical capacity density of lithium tungsten composite oxide (e.g. 1500 mAh/cc) is higher than that of graphite (820 mAh/cc) and further said lithium tungsten composite oxide anode active material has excellent discharge capacity density, wherein said lithium tungsten composite oxide may be Li4WyM1−yO5, wherein 0.05 ≤ y ≤ 0.75 and M may be Mn, Zn, and Sn (e.g. ¶¶ 0009-14, 25, and 51-57).
As a result, it would have been obvious to substitute the anode active material, such as graphite, in the anode layer of Kinkata with the lithium tungsten composite oxide anode active material of Ichikawa, which may be Li4WyM1−yO5, wherein 0.05 ≤ y ≤ 0.75 and M may be Mn, Zn, and Sn, since Ichikawa teaches its lithium tungsten composite oxide anode active material has excellent discharge capacity density; and/or, since Ichikawa teaches its lithium tungsten composite oxide anode active material has a theoretical capacity density than that of graphite.
(March 18, 2026 non-final Office action, at pp. 4-5, bolding in the original.)
Third, the applicant alleges the following.
C. Neither Kintaka, Ichikawa, nor Yan provides a reasonable expectation that practical utilization could be achieved after co-firing.
…
Neither Kintaka, Ichikawa, nor Yan provides a reasonable basis for a POSA to expect that: 1) the garnet phase would survive co-firing, nor that 2) the Li-W phase would survive co-firing.
Kintaka fails to teach that a Li-W-based negative electrode active material having Li/M molar ratio > 2 can be co-fired with a garnet-type solid electrolyte, or that reactions during sintering can be suppressed. Moreover, Kintaka explains that active materials and solid electrolytes may be fired together, that positive electrodes, solid electrolytes, and negative electrodes may be integrally co-fired; that reactions may occur between active materials and solid electrolytes during firing; and that such reactions may prevent obtaining the desired solid electrolyte. See Kintaka at [0008]-[0011], [0025], [0074]. Furthermore, Kintata teaches that suppressing such reactions is an important consideration. Therefore, Kintaka does not suggest that any active material can simply be combined with a garnet-type solid electrolyte and co-fired. Instead, Kintaka teaches that compatibility during co-firing is a critical consideration when selecting electrode materials, in view of firing reactions being a significant technical issue. Consequently, a POSA familiar with Kintaka would not have simply incorporated Ichikawa's Li-W-based negative electrode material into Kintaka merely because of its higher capacity, as proposed by the Examiner. To the contrary, Ichikawa's Li-W-based negative electrode material would have been viewed as likely to be incompatible for the reasons discussed above, outweighing any alleged capacity gains.
When these factors are considered in totality, it is unreasonable to conclude that the combined teachings of the asserted prior art would have led a POSA to the battery of claim 1. As such, reconsideration and withdrawal of the present rejections under 35 U.S.C. 103 is respectfully requested. Dependent claims 2-18 are nonobvious based on their dependence on claim 1, in addition to the various additional elements recited by each of these claims.
(Remarks, at e.g. 10:4-11:1, emphasis in the original.)
In response, the examiner respectfully notes that the argument is not commensurate with the scope of the art or the scope of the Office action, incorporating herein the discussion supra.
Conclusion
The art made of record and not relied upon is considered pertinent to applicant's disclosure.
Wu et al (US 2024/0006586);
Badding et al (US 2023/0295049);
Paolella et al (US 2021/0147299);
Mo et al (US 2021/0083319);
Mo et al (US 2021/0083318);
Wang et al (US 2020/0227775);
Takano et al (US 2020/0106130);
Brew et al (US 2018/0006333);
Badding et al (US 2016/0308244);
Gaben (US 2016/0013513);
Tsuchida et al (US 2013/0260258); and
Miyazaki et al (US 4803137).
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 YOSHITOSHI TAKEUCHI whose telephone number is (571)270-5828. The examiner can normally be reached M-F, 8-4.
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If attempts to reach the examiner by telephone are unsuccessful, the examiner’s supervisor, TIFFANY LEGETTE-THOMPSON can be reached at (571)270-7078. The fax phone number for the organization where this application or proceeding is assigned is 571-273-8300.
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/YOSHITOSHI TAKEUCHI/Primary Examiner, Art Unit 1723
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