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
The amendment filed on December 18th 2025 is acknowledged. Claims 1-17 & 19 remain pending in the application. Claim 20 was added by the Applicant. The previous 112(a) rejection of Claim 6 is withdrawn due to Applicant’s amendment. The arguments to the 103 rejections of the claims have been fully considered but are not persuasive, therefore the rejections are maintained.
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.
Claim 20 is 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 20, as it depends from Claim 1, includes the limitation of the thickness of the solid electrolyte layer of 0.1-30 µm. However, Claim 20 introduces the limitation of the positions of the negative electrode layer vicinity portion of the solid electrolyte layer and the positive electrode layer vicinity portion of the solid electrolyte layer, wherein the positions of each are within 1 µm of the respective interfaces with the electrode layers. Thus, the solid electrolyte layer, as limited in Claim 20, must be no less than 2 µm. Therefore, the lower limit of the thickness range of the solid electrolyte layer as stated in Claim 1 is incompatible with the requirement of the positions of each of the vicinity portions being within 1 µm. Thus the claim is indefinite. Appropriate correction is required.
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.
The factual inquiries for establishing a background for determining obviousness under 35 U.S.C. 103 are summarized as follows:
1. Determining the scope and contents of the prior art.
2. Ascertaining the differences between the prior art and the claims at issue.
3. Resolving the level of ordinary skill in the pertinent art.
4. Considering objective evidence present in the application indicating obviousness or nonobviousness.
Claims 1-11, 16-17, & 19 are rejected under 35 U.S.C. 103 as being unpatentable over Takeuchi et al. WO 2019/188840 A1 in further in view of Liao et al. “Si-Doping Mediated Phase Control from β- to γ-Form Li3VO4 Toward Smoothing Li Insertion/Extraction”. Further evidence provided by Yazdani et al. “Thermal transport in phase-stabilized lithium zirconate phosphates”.
Regarding Claim 1, Takeuchi discloses a solid state battery comprising a positive electrode layer, a negative electrode layer, and a solid electrolyte layer between the positive electrode layer and the negative electrode layer [Page 1 Lines 53-55]. Takeuchi discloses that the negative electrode layer comprises lithium vanadium phosphate [Page 1 Lines 55-56]. Takeuchi discloses that during the process of laminating the layers of the solid state battery, the battery undergoes heating such that the vanadium diffuses towards the solid electrolyte and forms “intermediate layers” at the negative electrode layer side of the solid electrolyte [Page 8 Lines 23-34]. See Takeuchi Annotated Figure 4 below.
PNG
media_image1.png
865
676
media_image1.png
Greyscale
Takeuchi Annotated Figure 4
Takeuchi discloses that the solid electrolyte contains lithium zirconium phosphate as a main component [Page 4 Lines 4-5], which is known in the art to have a lithium super ionic conductor structure (as evidenced by Yazdani [Page 3 Left Column Lines 16-17]). Takeuchi further discloses the “intermediate layers” (Figure 4 Items 7 & 8) contain lithium vanadium zirconium phosphate wherein the specific ratio of vanadium to zirconium changes in the thickness direction from the negative electrode to the rest of the solid electrolyte [Page 4 Lines 31-44], as further shown in Figure 4b above. Thus, Takeuchi discloses that the solid electrolyte contains V. More specifically, Takeuchi discloses that the part of the electrolyte layer nearer the electrode (intermediate layer 7) has lithium vanadium phosphate containing zirconium [Page 4 Lines 31-32] whereas the part of the electrolyte layer nearer the center of the electrolyte layer (intermediate layer 8) has lithium zirconium phosphate containing vanadium [Page 4 Lines 39-40]. Thus, Takeuchi discloses that the amount of V in the electrolyte layer decreases in the thickness direction from the electrode to the electrolyte layer as shown in Figure 4b. Further, as show in Takeuchi Annotated Figure 4 – Vanadium Amount below, Takeuchi discloses that the molar fraction of V in the solid electrolyte changes gradually by an amount of 0.20 or more in the thickness direction of the solid electrolyte layer (the chart shows a change amount of 100% vanadium in the electrode layer to 0% in the electrolyte layer). Additionally, as illustrated below, Takeuchi discloses that the molar fraction of V is greater in the electrolyte layer in the vicinity of the negative electrode layer as compared to the vicinity of the positive electrode layer:
PNG
media_image2.png
865
792
media_image2.png
Greyscale
Takeuchi Annotated Figure 4 – Vanadium Amount
Takeuchi discloses that the thickness of the solid electrolyte (Figure 4 Item 3) is preferably 3 µm or more [Page 6 Lines 14-17], and the intermediate layers (Figure 4 Items 7 & 8) each have a thickness of 2-5 µm [Page 5 Lines 43-45, Page 6 Lines 1-3]. Thus Takeuchi discloses that the thickness of the electrolyte layer (which includes layers 3, 7, & 8 as above in Figure 4) is at least 7 µm to 13 µm or more. In the examples (Table 2), Takeuchi further discloses that the thickness of the electrolyte layer (which includes layers 3, 7, & 8) is anywhere from 8 µm (Example 16) to 33 µm (Example 23), which overlaps with the claimed range. In regards to the thickness of the electrolyte layer, the Examiner directs Applicant to MPEP 2144.05 I. In the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art” a prima facie case of obviousness exists. Accordingly, it would have been obvious to one of ordinary skill in the art to have selected the overlapping ranged disclosed by Takeuchi because selection of the overlapping portion or ranges has been held to be a prima facie case of obviousness. See MPEP 2144.05 I.
As mentioned above, Takeuchi discloses that the negative electrode layer can be a lithium vanadium phosphate or the like [Page 1 Lines 55-56]. Takeuchi is silent as to the negative electrode layer comprising a specific molar ratio of Li to V of 2.0 or more.
Liao et al discloses in their journal article a method to generate an active material for an electrode of a lithium battery with better high-temperature stability and high ionic conductivity using LVO crystal structures [Abstract]. Liao discloses anodes comprised of Li3VO4 chemical compositions [Introduction, Page 1-2], which reads directly on the requirement of Claim 1 wherein “negative electrode active material with a molar ratio of Li to V is 2.0 or more”.
Liao further discloses that when the compounds mentioned in their disclosure are used for the anodes, when doped with silicon, the anodes can achieve better high temperature stability [Conclusions].
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the present invention to modify the negative electrode active material of Takeuchi to comprise the Li3VO4 chemical compositions of Liao to arrive at a ratio of Li to V of 2.0 or more for the advantages of having a solid-state battery with improved high temperature stability.
Takeuchi discloses that the positive electrode layer can also comprise the same active material as the negative electrode layer [Page 1 Lines 55-58; Page 4 Lines 9-10]. Thus, modified Takeuchi with the negative active material modified by Liao would comprise Li3VO4 as the positive electrode active material as well.
Regarding Claims 2 & 3, Takeuchi discloses as shown in Figure 4b that the electrolyte layer in the vicinity of the negative electrode layer comprises vanadium and some of the vanadium is replaced by zirconium [Page 4 Lines 31-32]. As shown in the chart, the electrolyte layer in the vicinity of the negative electrode layer (shown as intermediate layer 7) contains zirconium and vanadium (represented by the relationship Zr/(Zr+V)) in an amount of ~0.1-0.4 (see Annotated Figure 4 below):
PNG
media_image3.png
870
645
media_image3.png
Greyscale
Takeuchi Annotated Figure 4 – Vanadium Amount
For example, when Zr/(Zr+V) = 0.5, the amounts of Zr and V would both be 50%. As show in chart 4b above, the electrolyte layer in the vicinity of the negative electrode layer comprises Zr/(Zr+V) at values between 0.1-0.4, which indicates an amount of vanadium of 60-90% compared to the overall amount of zirconium and vanadium combined. As modified by Liao above, modified Takeuchi discloses a molar fraction of V in the negative electrode layer of 1.0 (Li3VO4), and Takeuchi discloses that in the thickness direction from the negative electrode layer to the electrolyte layer, some of the vanadium is replaced with zirconium, thus modified Takeuchi discloses that the electrolyte layer in the vicinity of the negative electrode layer comprises a molar fraction of vanadium of 0.4 or more (per Claim 2) and more specifically 0.4-0.95 (per Claim 3).
Regarding Claim 4, modified Takeuchi, as mentioned above with regards to Claim 1, that the molar fraction of vanadium in the negative electrode layer is 1.0 (Li3VO4, per the modification of Liao). Further, Takeuchi discloses that, in the thickness direction from the negative electrode layer to the electrolyte layer, some of the vanadium is replaced with zirconium [Page 4 Lines 31-32], represented by layers 7 & 8 in Figure 4a and as illustrated in the chart in Figure 4b. Takeuchi discloses that the layers 7 & 8 both have a thickness of 2-5 µm [Page 5 Lines 43-45, Page 6 Lines 1-3], and the rest of the electrolyte layer 3 (Figure 4) has a thickness of 3 µm or more [Page 6 Lines 14-17]. More specifically, in Example 10, Takeuchi discloses that the thickness of layer 7 is 3.0 µm, the thickness of layer 8 is 3.0 µm, and the thickness of the rest of the electrolyte layer 3 is 17.0 µm (Table 2). Thus, Takeuchi discloses that the rest of the electrolyte layer 3 comprises 74% of the overall thickness of the electrolyte (layers 7, 8, & 3 of Figure 4). Takeuchi discloses that the boundary between the layers 7 & 8 of Example 10 occurs when Zr/(Zr+V) = 0.5 (Table 3), which represents a percentage of Zr compared to a total amount of Zr + V of 50%, which indicates that the molar fraction of vanadium at this point is 0.5 based on the modification of Liao wherein the starting molar fraction of V of the negative electrode is 1.0. Takeuchi further discloses that the gradient (Chart 4b) of layer 8 is 0.13 (slope represented by Zr/(Zr+V)/µm) over the thickness 3 µm [Table 3], which indicates that the layer 3 and the layer 8 would have a boundary at [0.5+(0.13x3µm)] = 0.89, which indicates that the molar fraction of vanadium at this point is 0.11 or less in the rest of the electrolyte layer 3. Thus, Takeuchi discloses that in 10-80% of the thickness of the electrolyte layer (layer 3 that makes up 74% of the overall thickness of the electrolyte as in Example 10), the molar fraction of vanadium is 0.6 or less (0.11 as in Example 10).
Regarding Claim 5, as mentioned with regards to Claim 4, modified Takeuchi discloses that in 30-80% of the thickness of the electrolyte layer (layer 3 that makes up 74% of the overall thickness of the electrolyte as in Example 10), the molar fraction of vanadium is 0.6 or less (0.11 as in Example 10).
Regarding Claim 6, as mentioned with regards to Claim 4, modified Takeuchi discloses that in 10% or more of the thickness of the electrolyte layer (layer 3 that makes up 74% of the overall thickness of the electrolyte as in Example 10), the molar fraction of vanadium is 0.4 or less (0.11 as in Example 10).
Regarding Claim 7, as mentioned with regards to Claim 4, Takeuchi discloses in Example 10 that the slope of layer 8 of the electrolyte layer (Figure 4a) is 0.13 [Table 3] which is represented by Zr/(Zr+V)/µm, and indicates that the amount (molar fraction) of zirconium is increasing by 0.13 per micron in the thickness direction from the negative electrode layer to the electrolyte layer (Figure 4). Takeuchi discloses that, in the thickness direction from the negative electrode layer to the electrolyte layer, some of the vanadium is replaced with zirconium [Page 4 Lines 31-32], thus Takeuchi discloses that the amount of vanadium is decreasing by the same amount (i.e. 0.13 per micron in Example 10) in the thickness direction. Thus, Takeuchi discloses that the rate of change in the molar fraction of vanadium is 0.13 in the thickness direction of electrolyte layer, which falls within the claimed range.
Regarding Claim 8, similarly to Claim 7, Takeuchi discloses in Example 10 that the slope of layer 8 of the electrolyte layer (Figure 4a) is 0.13 [Table 3] which is represented by Zr/(Zr+V)/µm, and indicates that the amount (molar fraction) of zirconium is increasing by 0.13 per micron in the thickness direction from the negative electrode layer to the electrolyte layer (Figure 4). Takeuchi discloses that, in the thickness direction from the negative electrode layer to the electrolyte layer, some of the vanadium is replaced with zirconium [Page 4 Lines 31-32], thus Takeuchi discloses that the amount of vanadium is decreasing by the same amount (i.e. 0.13 per micron in Example 10) in the thickness direction. Thus, Takeuchi discloses that the rate of change in the molar fraction of vanadium is 0.13 in the thickness direction of electrolyte layer, which falls within the claimed range.
Regarding Claim 9, the present disclosure claims the formula of the negative electrode active material to be (Li3-ax+(5-b)(1-y)Ax) (VyB1-y)O4, where
A is Na, K, Mg, Ca, Al, Ga, Zn, Fe, Cr, and Co
B is Zn, Al, Ga, Si, Ge, Sn, P, As, Ti, Mo,W, Fe. Cr. and Co
0≤x≤1.0
0.5≤y≤1.0
a is an average valence of A
b is an average valence of B
Modified Takeuchi discloses, with the modification of Liao as mentioned with regards to Claim 1, a negative electrode comprised of Li3VO4 chemical compositions [Liao Introduction, Page 1-2] and doped with silicon for better high temperature stability of the anodes [Liao Conclusions]. The Si-doped Li3VO4 anodes of Liao’s disclosure satisfy the present disclosures requirements outlined previously where,
B is Si
x = 0
y = 0.85
b = 4 (average valence of Silicon)
and the remaining requirements (1 and 5) are 0 due to x = 0, thus the resulting chemical formula is Li3.15V0.85Si0.15O4 as disclosed by Liao [Conclusions].
Liao further discloses that when the above chemical composition is used as an anode, the lithium ion conductivity is enhanced and the stability of the battery cycle enhanced the performance and capacity retention of the battery [Conclusions].
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the present invention to modify the negative electrode of Takeuchi to comprise the chemical formula Li3.15V0.85Si0.15O4 as described by Liao to improve the stability, cell capacity, and performance of a solid-state lithium battery.
Regarding Claim 10, the present disclosure claims the formula of the negative electrode active material as stated in Claim 9 with the further limitations of:
A is Al or Zn
B is Si or P
0≤x≤0.06, and
0.55≤y≤1.0
As mentioned with regards to Claim 9, Liao discloses anodes comprised of Li3VO4 chemical compositions [Introduction, Page 1-2] and doped with silicon for better high temperature stability of the anodes. The Si-doped Li3VO4 anodes of Liao’s disclosure further satisfy the present disclosure’s limited requirements of claim 10, where,
B is Si
x = 0
y = 0.85
and the remaining requirement (1) is 0 due to x = 0, thus the resulting chemical formula is Li3.15V0.85Si0.15O4 as disclosed by Liao [Conclusions].
Regarding Claim 11, modified Takeuchi discloses a negative electrode active material as modified by Liao with regards to Claim 1 above. Liao discloses that the negative electrode active material has a βII-Li3VO4-type structure or a γII-Li3VO4-type structure [Abstract], and further discloses that the γ-type is more favorable due to its capacity retention during charge cycling while remaining stable [Conclusions]. Thus, modified Takeuchi discloses, with the negative electrode active material of Liao, that the negative electrode active material has γII-Li3VO4-type structure.
Regarding Claim 16, Takeuchi discloses that in the positive electrode active material and the negative electrode active material, lithium ions are inserted or desorbed during charge and discharge [Page 3 Line 59-Page 4 Line 2], thus Takeuchi discloses that the positive or negative electrode are capable of occluding and releasing lithium ions.
Regarding Claim 17, Takeuchi discloses that the battery laminate is made by producing green sheets of the layers (negative electrode, positive electrode, and electrolyte) and subjecting the laminated green sheets to thermocompression bonding by applying temperature and pressure and sintering (firing) the laminated body [Page 7 Lines 6-13]. Further, Takeuchi discloses that the temperature of the sintering step (firing) is 600-900°C [Page 8 Lines 18-21]. Thus, Takeuchi discloses that the laminated battery is an integrally sintered body.
Regarding Claim 19, as mentioned with regards to Claim 4, modified Takeuchi discloses that in 50-80% of the thickness of the electrolyte layer (layer 3 that makes up 74% of the overall thickness of the electrolyte as in Example 10), the molar fraction of vanadium is 0.6 or less (0.11 as in Example 10).
Claims 12-15 are rejected under 35 U.S.C. 103 as being unpatentable over Takeuchi and Liao as applied to Claim 1 above, and in further in view of Satou US 2017/0263981 A1.
Regarding Claim 12, the present disclosure claims the formula of the solid-state electrolyte to be (Li3-ax-(5-b)(1-y)Ax) (VyB1-y)O4, where
A is Na, K, Mg, or Ca
B is Zn, Al, Ga, Si, Ge, Sn, P, As, Ti, Mo,W, Fe, Cr. and Co
a is an average valence of A
b is an average valence of B
0≤x≤1.0 and 0<y<1.0
Satou discloses a laminated solid state lithium battery. Satou discloses that the solid electrolyte material is Li3.4Si0.4V0.6O4 [0094]. The chemical formula disclosed in Satou satisfies requirement 2 where B=Si, 4 where b=4 (average valence of Si), 5 where y=0.4, and requirement 1 and 3 when x=0.
Satou discloses that this solid electrolyte material has high ionic conductivity and good heat resistance [0094].
Therefore, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the present invention to use the solid electrolyte material of Satou in the battery of Takeuchi to achieve a solid electrolyte comprising a formula that meets the limitations set forth by Claim 12 with high ionic conductivity and good heat resistance.
Regarding Claim 13, modified Takeuchi discloses that the solid electrolyte layer can contain a Garnet-type solid electrolyte [Satou 0094].
Regarding Claim 14, Takeuchi is relied upon for the reasons given above in addressing Claim 1, however fails to disclose that the negative electrode layer further comprises a conductive additive.
Satou discloses a laminated solid state lithium battery, similar to that of Takeuchi and Liao, as mentioned above with regards to Claims 12 & 13. Satou discloses a conductive additive included in the negative electrode layer [0079, 0082].
Satou discloses that including a conductive additive in the negative electrode layer improved the electrical conductivity of the negative electrode active material [0079].
Therefore, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the present invention to include the conductive additive as suggested by Satou in the negative electrode layer of modified Takeuchi to provide improved electrical conductivity of the negative electrode active material.
Regarding Claim 15, Takeuchi discloses that the one or both of the negative electrode layer or the electrolyte layer can comprises a sintering aid [Page 9 Lines 35-42], and that the sintering aid is H3BO3 [Page 9 Line 42]. Takeuchi fails to disclose that the sintering aid has a chemical composition comprising Li, in which the molar ratio of Li to B is 2.0 or more.
Satou discloses that the negative electrode layer can further comprises a sintering aid [0079], as well as a solid state electrolyte layer that can further comprise a sintering aid [0093]. Satou further discloses that the sintering additive can be Li3BO3 [0095]. Satou discloses that the sintering additive that can be Li3BO3 [0081, 0095], which has a molar ratio of Li to B of 3.0.
Satou discloses that including a sintering additive improve sinterability among the negative electrode active material particles [0079] or among the electrolyte particles [0093].
Therefore, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the present invention to replace the sintering additive of Takeuchi with the sintering additive of Satou (Li3BO3), to provide an electrolyte layer or negative electrode layer with a sintering additive having a Li to B ratio of 2.0 or more, to achieve better sintering among the particles of the layers.
Claims 1-3 & 7-17 are rejected under 35 U.S.C. 103 as being unpatentable over Ouchi et al. US 2012/0115039 A1 in further in view of Liao et al. “Si-Doping Mediated Phase Control from β- to γ-Form Li3VO4 Toward Smoothing Li Insertion/Extraction” and Satou US 2017/0263981 A1.
Regarding Claim 1, Ouchi discloses a solid state laminated secondary battery [0012] comprising:
A positive electrode layer (Figure 1 Item 11 [0030])
A negative electrode layer (Figure 1 Item 12 [0030])
and a solid electrolyte layer interposed between the positive electrode layer and the negative electrode layer (Figure 1 Item 13 [0030]).
Ouchi discloses that the solid electrolyte layer has a thickness of 10 µm [0066]. In regards to the thickness of the electrolyte layer, the Examiner directs Applicant to MPEP 2131.03 I. In the case where the prior art “discloses a point within the claimed range, the prior art anticipates the claim”. UCB, Inc. v. Actavis Labs. UT, Inc., 65 F.4th 679, 687, 2023 USPQ2d 448 (Fed. Cir. 2023). Accordingly, the thickness disclosed in Ouchi anticipates the claimed range set forth in Claim 1. See MPEP 2131.03 I.
Ouchi discloses that the negative electrode layer contains a negative electrode active material containing Li (electrode active material is a lithium containing phosphate compound [0034]) and can further include V (Li-----3V2(PO4)2 was used in Examples [0054]), however fails to specifically discloses that the molar ratio of Li to V is 2 or more.
Regarding the negative electrode active material, Liao et al discloses in their journal article a method to generate an anode for the lithium battery with better high-temperature stability and high ionic conductivity using LVO crystal structures. Liao discloses anodes comprised of Li3VO4 chemical compositions [Introduction, Page 1-2], which reads directly on the requirement of Claim 1 wherein “negative electrode active material with a molar ratio of Li to V is 2.0 or more”.
Liao further discloses that when the compounds mentioned in their disclosure are used for the anodes, when doped with silicon, the anodes can achieve better high temperature stability [Conclusions].
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the present invention to modify the negative electrode active material of Ouchi to comprise the Li3VO4 chemical compositions of Liao to arrive at a ratio of Li to V of 2.0 or more for the advantages of having a solid-state battery with improved high temperature stability.
Ouchi fails to specifically disclose that the solid electrolyte layer contains a solid electrolyte that has a lithium super ionic conductor structure and contains V.
Regarding the solid electrolyte containing V, Satou discloses a laminated solid state lithium battery. Satou discloses that the solid electrolyte material is Li3.4Si0.4V0.6O4 [0094], thus Satou discloses a solid electrolyte material having a super ionic conductor structure and containing V.
Satou discloses that this solid electrolyte material has high ionic conductivity and good heat resistance [0094].
Therefore, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the present invention to use the solid electrolyte material of Satou in the battery of Ouchi to achieve a solid electrolyte material containing V with high ionic conductivity and good heat resistance.
Ouchi further fails to disclose a ratio of V in the solid electrolyte changes gradually by an amount of 0.20 or more in a thickness direction of the solid electrolyte layer as stated in Claim 1 of the present disclosure.
Regarding a ratio of V in the solid electrolyte changes gradually by an amount of 0.20 or more in a thickness direction of the solid electrolyte layer, in the specification of the present disclosure, the applicant discloses that the gradient of the electrolyte is created due to element diffusion during sintering [0189]. More specifically, the applicant discloses that a process of sintering the laminated battery body at a temperature of 750°C for 1 hour causes the element diffusion from the anode to the electrolyte, increasing the amount of V in the electrolyte immediately adjacent to the anode [0189]. Applicant further discloses that the ratio of V can be controlled by either laminating green sheets of the positive electrode, solid electrolyte, and negative electrode, each containing a known amount of V and a specific thickness, such that the desired change in the ratio of V across the layers is achieved [0222-0223], or by sintering the laminated layers for a certain amount of time (30 minutes or more) to allow element diffusion [0224-0226]. Specifically in Example 7, Applicant discloses a laminated battery including an anode comprising Li3.2Si0.2V0.8O4, an electrolyte comprising Li3.2Si0.2V0.8O4 (ratio of V = 0.8), and a positive electrode not containing V, that is made via sintering at 750°C for 1 hour, and Example 7 as shown in Table 5 has a ratio of V that changes by an amount of 0.77 across the electrolyte thickness [0341], also see Figure 11 of the instant application.
Modified Ouchi discloses similar materials and a similar method of making to that of the Applicant's Example 7:
Temperature & Time: Ouchi discloses a laminated solid state lithium battery and method of producing the battery through the process of sintering at high temperatures [0020]. More specifically, in the preparation steps of the examples [0080], Ouchi further discloses that the sintering process includes the firing step at 750°C for 1 hour, which are the same processing parameters as Applicant's Example 7. Additionally, Satou discloses sintering the laminated battery at 800°C for 2 hours [0140], which would further increase diffusion at the higher temperature and longer time.
Materials: Modified Ouchi discloses that the solid electrolyte material is Li3.4Si0.4V0.6O4 (as modified by Satou [Satou 0094]), which has a similar ratio of V (0.6) to that of Example 7. Modified Ouchi discloses that the negative electrode active material is a lithium vanadium oxide comprising Li3VO4 (as modified by Liao [Liao Introduction, Page 1-2].
Therefore, modified Ouchi teaches a laminated lithium battery produced under the same sintering conditions at 750°C for 1 hour as Example 7 in the instant disclosure, and with similar materials comprising a lithium vanadium anode, a vanadium-containing electrolyte with a similar ratio of V, and a vanadium-free positive electrode as in Example 7 (modified with Satou and Liao). Examiner notes that while Ouchi lacks the additional electrolyte layer that is free of vanadium immediately adjacent to the vanadium rich electrolyte layer that Applicant discloses in Example 7, modified Ouchi does disclose a vanadium rich layer (electrolyte of Satou) immediately adjacent to a vanadium free layer (the positive electrode), and in that manner when the laminated structure is sintered at 750°C for 1 hour, one would expect diffusion to occur across the electrolyte layer in the same way as disclosed by Applicant. Therefore, one would reasonably expect the laminated battery of modified Ouchi to display the recited properties, namely allowing for “a ratio of V in the solid electrolyte changes gradually by an amount of 0.20 or more in a thickness direction of the solid electrolyte layer” by diffusion of the negative electrode active material through the electrolyte due to sintering. See MPEP 2112.01 I.
Regarding the ratio of V in a negative electrode layer vicinity portion of the solid electrolyte is greater than that of the positive electrode vicinity portion, modified Ouchi teaches a laminated lithium battery produced under the same sintering conditions at 750°C for 1 hour as Example 7 in the instant disclosure, and with similar materials comprising a lithium vanadium anode, a vanadium-containing electrolyte with a similar ratio of V, and a vanadium-free positive electrode as in Example 7 (modified with Satou and Liao). Examiner notes that while Ouchi lacks the additional electrolyte layer that is free of vanadium immediately adjacent to the vanadium rich electrolyte layer that Applicant discloses in Example 7, modified Ouchi does disclose a vanadium rich layer (electrolyte of Satou) immediately adjacent to a vanadium free layer (the positive electrode), and in that manner when the laminated structure is sintered at 750°C for 1 hour, one would expect diffusion to occur across the electrolyte layer in the same way as disclosed by Applicant. Example 7, as shown in Figure 11 of the instant application, results in a higher ratio of V in the negative electrode vicinity than the positive electrode vicinity.
Therefore, one would reasonably expect the laminated battery of modified Ouchi to display the recited properties, namely allowing for “the ratio of V in a negative electrode layer vicinity portion of the solid electrolyte is greater than that of the positive electrode vicinity portion” by diffusion of the negative electrode active material through the electrolyte due to sintering. See MPEP 2112.01 I.
Regarding Claims 2 & 3, modified Ouchi discloses an electrolyte layer comprising Li3.4Si0.4V0.6O4 (Satou 0094), thus comprising a ratio of V of 0.6. Thus modified Ouchi discloses that the ratio of V is 0.6 in the negative electrode layer vicinity portion of the solid electrolyte layer, which reads on the limitations set forth in Claims 2 & 3.
Regarding Claims 7 & 8, as mentioned with regards to claim 1, modified Ouchi teaches a laminated lithium battery produced under the same sintering conditions at 750°C for 1 hour as Example 7 in the instant disclosure, and with similar materials comprising a lithium vanadium anode, a vanadium-containing electrolyte with a similar ratio of V, and a vanadium-free positive electrode as in Example 7 (modified with Satou and Liao). Examiner notes that while Ouchi lacks the additional electrolyte layer that is free of vanadium immediately adjacent to the vanadium rich electrolyte layer that Applicant discloses in Example 7, modified Ouchi does disclose a vanadium rich layer (electrolyte of Satou) immediately adjacent to a vanadium free layer (the positive electrode), and in that manner when the laminated structure is sintered at 750°C for 1 hour, one would expect diffusion to occur across the electrolyte layer in the same way as disclosed by Applicant. Example 7 of the instant disclosure results in a maximum value [dy/dL]MAX of a rate of change in the ratio y of V of 0.20 (Table 5).
Therefore, one would reasonably expect the laminated battery of modified Ouchi to display the recited properties, namely allowing for “a maximum value [dy/dL]MAX of a rate of change in the ratio y of V is 0.55 or less (Claim 7) and further 0.05-0.55 (Claim 8) in the thickness direction of the solid electrolyte layer” by diffusion of the negative electrode active material through the electrolyte due to sintering. See MPEP 2112.01 I.
Regarding Claim 9, the present disclosure claims the formula of the negative electrode active material to be (Li3-ax+(5-b)(1-y)Ax) (VyB1-y)O4, where
A is Na, K, Mg, Ca, Al, Ga, Zn, Fe, Cr, and Co
B is Zn, Al, Ga, Si, Ge, Sn, P, As, Ti, Mo,W, Fe. Cr. and Co
0≤x≤1.0
0.5≤y≤1.0
a is an average valence of A
b is an average valence of B
Modified Ouchi discloses, with the modification of Liao as mentioned with regards to Claim 1, anodes comprised of Li3VO4 chemical compositions [Liao Introduction, Page 1-2] and doped with silicon for better high temperature stability of the anodes [Liao Conclusions]. The Si-doped Li3VO4 anodes of Liao’s disclosure satisfy the present disclosures requirements outlined previously where,
B is Si
x = 0
y = 0.85
b = 4 (average valence of Silicon)
and the remaining requirements (1 and 5) are 0 due to x = 0, thus the resulting chemical formula is Li3.15V0.85Si0.15O4 as disclosed by Liao [Conclusions].
Liao further discloses that when the above chemical composition is used as an anode, the lithium ion conductivity is enhanced and the stability of the battery cycle enhanced the performance and capacity retention of the battery [Conclusions].
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the present invention to modify the anode of Ouchi to comprise the chemical formula Li3.15V0.85Si0.15O4 as described by Liao to improve the stability, cell capacity, and performance of a solid-state lithium battery.
Regarding Claim 10, the present disclosure claims the formula of the negative electrode active material as stated in Claim 9 with the further limitations of:
A is Al or Zn
B is Si or P
0≤x≤0.06, and
0.55≤y≤1.0
As mentioned with regards to Claim 9, Liao discloses anodes comprised of Li3VO4 chemical compositions [Introduction, Page 1-2] and doped with silicon for better high temperature stability of the anodes. The Si-doped Li3VO4 anodes of Liao’s disclosure further satisfy the present disclosure’s limited requirements of claim 10, where,
B is Si
x = 0
y = 0.85
and the remaining requirement (1) is 0 due to x = 0, thus the resulting chemical formula is Li3.15V0.85Si0.15O4 as disclosed by Liao [Conclusions].
Regarding Claim 11, modified Ouchi discloses a negative electrode active material as modified by Liao with regards to Claim 1 above. Liao discloses that the negative electrode active material has a βII-Li3VO4-type structure or a γII-Li3VO4-type structure [Abstract], and further discloses that the γ-type is more favorable due to its capacity retention during charge cycling while remaining stable [Conclusions]. Thus, modified Ouchi discloses, with the negative electrode active material of Liao, that the negative electrode active material has γII-Li3VO4-type structure.
Regarding Claim 12, the present disclosure claims the formula of the solid-state electrolyte to be (Li3-ax-(5-b)(1-y)Ax) (VyB1-y)O4, where
A is Na, K, Mg, or Ca
B is Zn, Al, Ga, Si, Ge, Sn, P, As, Ti, Mo,W, Fe, Cr. and Co
a is an average valence of A
b is an average valence of B
0≤x≤1.0 and 0<y<1.0
Satou discloses suggested materials for the solid-state electrolyte such as lithium transitional metal composite oxides, more specifically Li3.4Si0.4V0.6O4 [0094]. The chemical formula disclosed in Satou satisfies requirement 2 where B=Si, 4 where b=4 (average valence of Si), 5 where y=0.4, and requirement 1 and 3 when x=0.
Thus, modified Ouchi discloses, with the modification of Satou as mentioned with regards to Claim 1 above, that the solid electrolyte comprises a formula that meets the limitations set forth by Claim 12.
Regarding Claim 13, modified Ouchi discloses that the solid electrolyte layer can contain a Garnet-type solid electrolyte [Satou 0094].
Regarding Claim 14, Ouchi discloses that the negative electrode layer can further comprise a conductive additive [0021].
Regarding Claim 15, modified Ouchi is relied upon for the reasons stated above in addressing Claim 1, however fails to discloses a sintering additive in the solid electrolyte layer or the negative electrode layer.
Satou discloses a solid state electrolyte layer comprising an electrolyte material, a binder, and a sintering additive [0093]. Satou further discloses that the sintering additive can be Li3BO3 [0095]. Satou also discloses that the negative electrode may also contain a sintering additive that can be Li3BO3 [0079, 0081].
Satou discloses that including a sintering additive improve sinterability among the negative electrode active material particles [0079] or among the electrolyte particles [0093].
Therefore, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the present invention to incorporate the sintering additive as suggested by Satou in the electrolyte or negative electrode of modified Ouchi to achieve better sintering among the particles of the layers.
Regarding Claim 16, Ouchi discloses a battery with a positive electrode layer that is capable of occluding and releasing lithium ions (contains a NASICON structure that conducts lithium ions at high speeds [0006]). Modified Ouchi, with the modification of Liao’s negative electrode material, discloses a negative electrode layer that is capable of occluding and releasing lithium ions (Liao a lithium vanadium oxide anode with high ionic conductivity [Abstract]).
Regarding Claim 17, Ouchi discloses a laminated solid-state lithium battery wherein the solid electrolyte layer, the positive electrode layer, and the negative electrode layer are joined by sintering [0012], thus forming an integrally sintered body.
Claims 4-6 & 19 are rejected under 35 U.S.C. 103 as being unpatentable over Ouchi, Liao, and Satou as applied to Claim 1 above, and in further in view of Takeuchi et al. WO 2019/188840 A1.
Regarding Claim 4, Ouchi, Liao, and Satou are relied upon for the reasons given above in addressing Claim 1, however fail to disclose that 10% to 80% of the thickness of the solid electrolyte layer contains a molar fraction of vanadium of 0.6 or less in the thickness direction.
Takeuchi discloses a battery comprising a positive electrode layer, a negative electrode layer, and a solid electrolyte layer between the positive and negative electrode [Page 1 Lines 53-55]. Takeuchi discloses that the negative electrode layer comprises vanadium (lithium vanadium phosphate [Page 1 Lines 55-56]). Takeuchi discloses that during the process of laminating the layers of the solid state battery, the battery undergoes heating such that the vanadium diffuses towards the solid electrolyte and forms “intermediate layers” at the negative electrode layer side of the solid electrolyte [Page 8 Lines 23-34] (See Figure 4).
Further, Takeuchi discloses that, in the thickness direction from the negative electrode layer to the electrolyte layer (Item 3 Figure 4), some of the vanadium is replaced with zirconium [Page 4 Lines 31-32], represented by layers 7 & 8 in Figure 4a and as illustrated in the chart in Figure 4b. In Example 10, Takeuchi discloses that the thickness of layer 7 is 3.0 µm, the thickness of layer 8 is 3.0 µm, and the thickness of the rest of the electrolyte layer 3 is 17.0 µm (Table 2). Thus, Takeuchi discloses that the rest of the electrolyte layer 3 comprises 74% of the overall thickness of the electrolyte (layers 7, 8, & 3 of Figure 4). Takeuchi discloses that the boundary between the layers 7 & 8 of Example 10 occurs when Zr/(Zr+V) = 0.5 (Table 3), which represents a percentage of Zr compared to a total amount of Zr + V of 50%, which indicates that the molar fraction of vanadium at this point is 0.5 based on the modification of Liao wherein the starting molar fraction of V of the negative electrode is 1.0. Takeuchi further discloses that the gradient (Chart 4b) of layer 8 is 0.13 (slope represented by Zr/(Zr+V)/µm) [Table 3], which indicates that the layer 3 and the layer 8 would have a boundary at [0.5+(0.13x3µm)] = 0.89, which indicates that the molar fraction of vanadium at this point is 0.11 or less in the rest of the electrolyte layer 3. Thus, Takeuchi discloses that in 10-80% of the thickness of the electrolyte layer (layer 3 that makes up 74% of the overall thickness of the electrolyte as in Example 10), the molar fraction of vanadium is 0.6 or less (0.37 as in Example 10).
Takeuchi discloses that an battery with this gradient of vanadium amount reduces the risk of the electrolyte peeling off of the electrode and enables strong bonding between the layers [Page 4 Lines 31-44]. Takeuchi further discloses that the concentration gradient reduces the contraction and expansion effect during battery operation [Page 4 Lines 21-29], which further reduces the risk of separation of the layers and improves battery characteristics [Page 4 Lines 27-29].
Therefore, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the present invention to incorporate the concentration gradient of Takeuchi in the battery of modified Ouchi to provide an electrolyte layer with 10-80% of the thickness comprising a molar fraction of vanadium of 0.6 or less (as mentioned above), to achieve a battery with reducing peeling between layers, stronger bonding between layers, and reduced contraction and expansion during battery operation.
Regarding Claim 5, similarly to Claim 4 above, modified Ouchi, with the modification of Takeuchi, discloses that in 30-80% of the thickness of the electrolyte layer (layer 3 that makes up 74% of the overall thickness of the electrolyte as in Example 10 of Takeuchi), the molar fraction of vanadium is 0.6 or less (0.11 as in Example 10 of Takeuchi).
Regarding Claim 6, as mentioned with regards to Claim 4, modified Ouchi discloses that in 10% or more of the thickness of the electrolyte layer (layer 3 that makes up 74% of the overall thickness of the electrolyte as in Example 10 of Takeuchi), the molar fraction of vanadium is 0.4 or less (0.11 as in Example 10 of Takeuchi).
Regarding Claim 19, as mentioned with regards to Claim 4, modified Ouchi discloses that in 50-80% of the thickness of the electrolyte layer (layer 3 that makes up 74% of the overall thickness of the electrolyte as in Example 10 of Takeuchi), the molar fraction of vanadium is 0.6 or less (0.11 as in Example 10 of Takeuchi).
Allowable Subject Matter
Claim 20 would be allowable if rewritten to overcome the rejection(s) under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), 2nd paragraph, set forth in this Office action and to include all of the limitations of the base claim and any intervening claims.
The following is a statement of reasons for the indication of allowable subject matter: Claim 20 is allowable because the closest prior art of record (Takeuchi) fails to disclose that the molar ratio of vanadium is greater in a negative electrode layer vicinity portion of the solid electrolyte layer than the molar ratio of vanadium in a positive electrode layer vicinity portion of the solid electrolyte layer, wherein the negative electrode layer vicinity portion of the solid electrolyte layer is within a distance of 1 µm from an interface with the negative electrode layer, and the positive electrode layer vicinity portion of the solid electrolyte layer is within a distance of 1 µm from an interface with the positive electrode layer. Similarly, Ouchi in view of Satou and Liao fails to disclose the limitations of Claim 20 because while modified Ouchi teaches that there would be a gradient of the molar ratio of vanadium present in the solid electrolyte layer, there is no basis that modified Ouchi discloses a greater molar ratio of vanadium in the solid electrolyte layer within 1 µm of the interface with the negative electrode than the molar ratio of vanadium in the solid electrolyte layer within 1 µm of the interface with the positive electrode. The dimensions of the vicinity portions, as claimed in Claim 20, draw distinction from the prior art of record.
Response to Arguments
Applicant argues that lithium zirconium phosphate (LZP), as taught by Takeuchi, does not have a LISICON structure and has instead a NASICON structure. Examiner respectfully points out that as evidenced by Yazdani, as stated in the rejection above, LZP can have a LISICON structure. Examiner notes that while LZP is disclosed in the art as having a NASICON structure, it is also disclosed in the art as having an LISICON structure as evidenced by Yazdani and as further supported by Gorodylova et al. “DTA–TGA and XRD study of the formation of LISICON-type Li1+xCrxZr2-x(PO4)3 ceramic using ZrOCl2-8H2O as precursor”, see Gorodylova Page 1 Right Column Lines 7-19, Page 1 Left Column Lines 18-23, and therefore Claim 1 as presently written is taught by Takeuchi as further evidenced by Yazdani. Accordingly, for the reasons stated above, this argument is unpersuasive.
Applicant argues that Takeuchi does not teach that the molar fraction of V in the negative electrode layer vicinity portion of the solid electrolyte layer is greater than that in the positive electrode layer vicinity portion of the solid electrolyte layer. Examiner respectfully points out that as stated in the rejection above, and as shown in Takeuchi Annotated Figure 4 above, Takeuchi illustrates that the molar fraction of V in the negative electrode layer vicinity portion of the solid electrolyte layer (left side) is greater than that in the positive electrode layer vicinity portion of the solid electrolyte layer (right side), as noted in the annotated figure above. The claim as presently written is not specific as to the exact location of the “negative electrode layer vicinity portion” or the “positive electrode layer vicinity portion” of the solid electrolyte layer, and as such the claim as presently written is taught by Takeuchi. Accordingly, for the reasons stated above, this argument is unpersuasive.
Applicant argues that one of skill in the art would not combine the conditions disclosed in Ouchi with the materials of Satou. As stated previously in the prior Office Action mailed on September 19th, 2025, Examiner respectfully points out that the conditions of Ouchi are considered to be similar to that of Satou and one of skill in the art would find them to be analogous and combinable. Ouchi discloses sintering the laminated body of green sheets at a temperature of 750°C for 1 hour [Ouchi 0080], whereas Satou discloses sinter bonding green sheets to produce an integrally sintered body by subjecting them to sintering at 800°C for two hours [Satou 0140]. Further, Ouchi discloses heating the laminated body prior to sintering at a lower temperature (500°C) to remove the resin [Ouchi 0080], and Satou discloses a similar step of heating the laminated body to a lower temperature (600°C) to remove the resin prior to sintering [Satou 0140]. Examiner additionally points out that Ouchi discloses using negative electrode active material containing a lithium phosphate that can have a NASICON structure, as well as an olivine structure, layered structure, or a spinel compound including a transition metal [Ouchi 0034], and using an electrolyte material containing a lithium phosphate that can have a NASICON structure, an oxide with a perovskite structure, an oxide with a garnet structure, or similar [Ouchi 0034]. Similarly, Satou discloses that the negative electrode active material can be a lithium transition metal oxide having a crystal structure [Satou 0080], and that the solid electrolyte can be a lithium composite oxide such as a garnet type, perovskite type, NASICON type, or glass type [Satou 0094]. Ouchi and Satou share overlapping materials for both the negative electrode active material and the solid electrolyte, as well as used similar conditions for sintering the laminated bodies, and thus Ouchi and Satou would be considered analogous to one of skill in the art. Accordingly, for the reasons stated above, this argument is unpersuasive.
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to ANNA E GOULD whose telephone number is (571)270-1088. The examiner can normally be reached Monday-Friday 9:00am-5:00pm.
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, Jeffrey T. Barton can be reached at (571) 272-1307. 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.
/A.E.G./Examiner, Art Unit 1726
/JEFFREY T BARTON/Supervisory Patent Examiner, Art Unit 1726 27 March 2026
Prosecution Insights