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
This is a final Office action in response to Applicant’s remarks and amendments filed on 01/09/2026. Claims 13 and 24 are amended. Claim 16 is canceled. Claims 13 – 15 and 17 – 24 are pending in the current Office action.
With respect to claim 13, a new grounds of rejection necessitated by applicant’s amendment {i.e. range for x in amended claim 1 is narrower than the range previously considered} that utilizes the previously cited prior art is presented below. With respect to claim 24, the 35 U.S.C. 103 rejection set forth in the previous Office action is maintained.
The terminal disclaimer filed 01/09/2026 is acknowledged. In light of the filed terminal disclaimer, the nonstatutory double patenting over U.S. Patent No. 12401030 B2 established in the previous Office action is withdrawn.
Response to Arguments
Applicant's arguments with respect to claim 13 and the teachings of Hodge, filed 01/09/2026, have been fully considered but they are not persuasive. Specifically, applicant argues that since amended claim 13 specifies a Ge concentration that falls squarely within the range defined to be problematic by Hodge {i.e. Hodge suggests that Ge incorporation can improve conductivity up to an optimal level but introduces mechanical problems in the ~35 – 65 mol% Ge range}, a person of ordinary skill in the art would not reasonably choose/be motivated to choose such a Ge content based on what is presented in Hodge.
In response to applicant's arguments against the references individually, one cannot show nonobviousness by attacking references individually where the rejections are based on combinations of references. See In re Keller, 642 F.2d 413, 208 USPQ 871 (CCPA 1981); In re Merck & Co., 800 F.2d 1091, 231 USPQ 375 (Fed. Cir. 1986).
Therefore, while examiner acknowledges that Hodge teaches pellets of a composition having ~35 – 65 mol% Ge having little mechanical strength/crumbling when cooled, when considering the application of the LSPO material in Miki {i.e. particles mixed with cathode active material to form electrode material}, since a crumbled pellet of a solid electrolyte material would still provide particles of solid electrolyte capable of being mixed in cathode active material, it would be in the purview of one with ordinary skill in the art to include an amount of Ge within the higher range taught by Hodge in the interest of obtaining a solid electrolyte material of higher conductivity. Furthermore, the solid electrolyte of modified Miki as established in the rejection below and previously does not only include Li, Si, Ge, and O like the solid electrolyte taught in Hodge, rather the solid electrolyte further includes P, as such it is indeterminate that the primary reference would experience the crumbling suggested in Hodge.
Additionally, the test for obviousness is not whether the features of a secondary reference may be bodily incorporated into the structure of the primary reference; nor is it that the claimed invention must be expressly suggested in any one or all of the references. Rather, the test is what the combined teachings of the references would have suggested to those of ordinary skill in the art. See In re Keller, 642 F.2d 413, 208 USPQ 871 (CCPA 1981). Therefore, in light of the above discussion and the additional prior art reference Zhang, applicant’s arguments regarding the teachings of Hodge are unpersuasive.
Applicant's arguments with respect to claim 24, filed 01/09/2026, have been fully considered but they are not persuasive. Specifically applicant argues that since Miki provides no teaching/ suggestion of co-sintering the cathode active material and bulk solid electrolyte into a fused “catholyte” and since Miki does not teach/suggest/contemplate co-sintering to form a catholyte, nor does it recognize the processing and performance benefits associated with such an approach, a person of ordinary skill in the art starting from Miki would not be motivated/have reasonable expectation of success in arriving at the claimed catholyte.
In response to applicant's argument that the references fail to show certain features of the invention, it is noted that the features upon which applicant relies (i.e., co-sintering to form a fused catholyte ) are not recited in the rejected claim(s). Although the claims are interpreted in light of the specification, limitations from the specification are not read into the claims. See In re Van Geuns, 988 F.2d 1181, 26 USPQ2d 1057 (Fed. Cir. 1993). The examiner respectfully notes that claim 24, as written, requires a catholyte comprising a solid solution electrolyte with the claimed formula and a cathode active material with the claimed general formula not the fused catholyte formed by co-sintering. As such applicant’s argument regarding the catholyte in Miki failing to be formed in the same manner as the catholyte of the claimed invention is narrower in scope that the claimed invention. That is, the scope of the claim as currently written does not particularly require a “fused catholyte” as seemingly argued by the applicant, and by teaching a positive electrode mixture comprising a solid electrolyte within the scope of the claimed general formula and positive electrode active material within the scope of the claimed general formula, modified Miki, as established below, still appears to render obvious the claimed catholyte.
Additionally, the examiner respectfully notes that the claim 24 is directed to a product and not a method of making, as such applicant’s arguments regarding the method of making the catholyte of the claimed invention are not fully commensurate with the scope of the claim, and applicant’s arguments regarding claim 24 are further rendered unpersuasive.
In response to applicant's argument that Miki does not recognize the processing and performance benefits associated with co-sintering to form a catholyte, the fact that the inventor has recognized another advantage which would flow naturally from following the suggestion of the prior art cannot be the basis for patentability when the differences would otherwise be obvious. See Ex parte Obiaya, 227 USPQ 58, 60 (Bd. Pat. App. & Inter. 1985).
Therefore, in light of the above discussion the rejection of claim 24 established in the previous Office action is maintained.
Claim Rejections - 35 USC § 103
Claim(s) 13 – 15 and 21 are rejected under 35 U.S.C. 103 as being unpatentable over Miki (US PG Pub. 2013/0295451 A1) in view of Hodge ("Ionic conductivity of Li4SiO4, Li4GeO4, and their solid solutions." Journal of the American Ceramic Society 59, no. 7‐8, pp. 360-366), Ivanov-Shitz ("Growth and ionic conductivity of Li3+ xP1− xGexO4 (x= 0.34) single crystals." Crystallography Reports 48, pp.112-115), and Deng ("Structural and mechanistic insights into fast lithium-ion conduction in Li4SiO4–Li3PO4 solid electrolytes." Journal of the American Chemical Society 137, no. 28, pp. 9136-9145). {Examiner notes: All prior art was cited in previous Office action mailed 11/15/2025}
Regarding Claims 13 – 14 , Miki discloses a solid electrolyte suitable for a solid state-rechargeable lithium ion battery, that is Miki teaches a solid electrolyte used in an electrode for a solid state battery ([0023];[0031]).
Miki teaches using oxide-type non-crystalline solid electrolytes, sulfide-type non-crystalline solid electrolytes and crystalline oxides and oxynitrides for the solid electrolyte, and, as one example of a crystalline oxide teaches Li3.6Si0.6P0.4O4 {i.e. LSPO} ([0031]). Li3.6Si0.6P0.4O4 is partially within the scope of the claimed general formula Li(3.5+L+x)Si(0.5+s-x)P(0.5+p-x)Ge2xO4 , specifically in Li3.6Si0.6P0.4O4, L = 0.10 which is within the claimed range of -0.1 0≤ L ≤ 0.10; s = 0 which is within the claimed range of -0.10 ≤ s ≤ 0.10; p = 0.10 which is within the claimed range -0.10 ≤ p ≤ 0.10; a = 0 which is within the claimed range of -0.40 ≤ a ≤ 0.40; and x = 0, which is outside the claimed range of 0.0 < x ≤ 0.30.
Since Miki teaches a finite list of example solid electrolytes, it would have been obvious to one with ordinary skill in the art, before the effective filings date of the claimed invention, to select Li3.6Si0.6P0.4O4 as the solid electrolyte material of Miki, and thus obtain solid electrolyte consisting of a compound with a composition significantly similar to the claimed general formula, with a reasonable expectation of success that such a selection would be suitable for the solid electrolyte-including electrode of Miki.
Miki as established above; however, does not disclose an LSPO compound including germanium {i.e. LSPGO}; and therefore, does not specifically disclose a compound with the general formula of Li(3.5+L+x)Si(0.5+s-x)P(0.5+p-x)Ge2xO4 wherein 0.20 < x ≤ 0.30 or more particularly the general formula of Li(3.5+x)Si(0.5-x)P(0.5-x)Ge2xO4 (Claim 14),
Hodge teaches solid solutions comprising Li4GeO4 and Li4SiO4 that increase in conductivity with increases in Li4GeO4 content (Table 1; Fig. 8; Section (2) Variation of Conductivity with Composition and Temperature, first paragraph pg. 363). Hodge further teaches that the increases in conductivity are a result of the Si in Li4SiO4 being replaced by Ge (Section (2) Variation of Conductivity with Composition and Temperature, second paragraph pg. 363). The molar ratios amounts of Ge taught by Hoge include 0.17, 0.25, and 0.33 and the particular formulas are Li4Si0.83Ge0.17O4, Li4Si0.75Ge0.25O4 , and Li4Si0.67Ge0.33O4, respectively (Table 1). Hodge further teaches Li-Si-Ge-O electrolyte compositions including ~35 – 65 mol% Ge, and based on the line data in Fig. 7, at least for compositions between 0.35 and 0.50 %mol an increase in conductivity can be obtained as the mol% of Ge increases (Section (2) Variation of Conductivity with Composition and Temperature, first paragraph pg. 36).
Ivanov-Shitz teaches a solid solution Li(3.5+x)P(1-x)GexO4 where x = 0.34 and the solid solution was prepared from equimolar amounts of Li3PO4 and Li4GeO4 (Abstract and Experimental section pg. 112). Ivanov-Shitz further teaches that an increase in conductivity was observed for the doped lithium phosphate solid solution in comparison to pure lithium phosphate solid solution (Results and Discussion section, second paragraph in right column pg. 113 and continuing in left column on pg. 114).
Deng teaches Li4SiO4-Li3PO4 solid electrolytes with varying compositions represented by (1-z)Li4SiO4-(z)Li3PO4 where z = 0 – 1 (Abstract). Deng further teaches that the intermediate compositions, z = 0.25, 0.50, and 0.75, provide ionic conductivities 3 – 4 orders of magnitude higher than when z = 0 and when z = 1, and further, based on Fig. 8, it appears that equal amounts of Si and P {i.e. x = 0.5}
provided the highest conductivity (3.2 Li-ion Conductivity and Dynamics section, pg. 9141).
Since Miki teaches an LSPO material with a composition that falls within Deng’s compositional scope, and Hodge and Ivanov-Shitz teach that solid solutions comprising Li4SiO4 or Li3PO4 achieve higher conductivities when doped with Ge, it would have been obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, to dope Miki’s LSPO material with Ge, and obtain a solid solution with the claimed elements of Li, S, P, Ge, and O, with a reasonable expectation of success in obtaining a solid electrolyte with increased conductivity.
Furthermore, since Hodge teaches LSO solid electrolyte compositions with mol% of Ge encompassing the claimed range and Deng teaches LSPO materials with molar ratios of Li, Si, P, and O that are within/overlap the claimed range, it would have been further obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, to prepare the LSPGO compound of modified Miki, with Li4SiO4, Li4GeO4 , and Li3PO4 in amounts that would provide Li, Si, P, Ge, and O within the claimed molar ranges, to optimize the lithium ion conductivity of the material, with a reasonable expectation of success and without undue experimentation [MPEP 2144.05(II)].
The solid electrolyte of modified Miki is not particularly disclosed to be a solid solution electrolyte; however, since Deng teaches that LSPO-type electrolytes are of a solid solution system (last paragraph in 1. Introduction section, pg. 9136), one with ordinary skill in the art would reasonably expect the LSPGO electrolyte material of modified Miki to necessarily and inherently be a solid solution electrolyte.
Regarding Claim 15, modified Miki discloses all limitations as set forth above. The solid electrolyte of modified Miki is an LSPO material doped with Ge.
Deng teaches that LSPO materials have ion conductivities within the range of 10-3 S/cm or higher (Deng: 3.2 Li-ion Conductivity and Dynamics section, pg. 9141) and, as established above, Hodge and Ivanov-Shitz teach that doping with Ge provides increases in conductivity for Li4SiO4 and Li3PO4 materials.
Therefore, since modified Miki’s solid electrolyte compound is an LSPO compound including Ge, with a composition within the claimed scope, one with ordinary skill in the art would expect the solid solution of modified Miki to have a lithium ion conductivity of at least 10-5 S/cm at room temperature.
Regarding Claim 21, modified Miki discloses all limitations as set forth above. Miki further discloses a solid-state rechargeable lithium ion battery ([0031];[0034]).
Claim(s) 17 and 22 – 23 are rejected under 35 U.S.C. 103 as being unpatentable over Miki (US PG Pub. 2013/0295451 A1) in view of Hodge ("Ionic conductivity of Li4SiO4, Li4GeO4, and their solid solutions." Journal of the American Ceramic Society 59, no. 7‐8, pp. 360-366), Ivanov-Shitz ("Growth and ionic conductivity of Li3+ xP1− xGexO4 (x= 0.34) single crystals." Crystallography Reports 48, pp.112-115), and Deng ("Structural and mechanistic insights into fast lithium-ion conduction in Li4SiO4–Li3PO4 solid electrolytes." Journal of the American Chemical Society 137, no. 28, pp. 9136-9145), as applied to claim 13 above, and further in view of Albano (WO2018089430A1, cited in previous Office action mailed 10/15/2025).
Regarding Claim 17, modified Miki discloses all limitations as set forth above. The solid electrolyte of modified Miki is an LSPO material doped with Ge.
Modified Miki does not explicitly disclose the solution electrolyte having a lithium ion conductivity at room temperature superior or equal to 2.0 x 10-5 S/cm and inferior or equal to 3.0 10-5 S/cm.
Albano teaches solid electrolyte conductivities, including LSPO, at working temperatures within the range of 10-6 and 10-1 S/cm ([00055];[0057]). Albano’s further teaches that such a conductivity range allows for safe operation of the solid-state battery at high temperatures with faster charge/discharge rates ([00055];[00092-00093];[00096];[000104]).
Deng also teaches LSPO materials that have ion conductivities within the range of 10-3 S/cm or higher (Deng: 3.2 Li-ion Conductivity and Dynamics section, pg. 9141) and, as established above, both Hodge and Ivanov-Shitz teach that doping with Ge provides increases in conductivity for Li4SiO4 and Li3PO4 materials.
Therefore, Since modified Miki’s solid electrolyte compound is an LSPO compound including Ge, with a composition within the claimed scope, one with ordinary skill in the art would reasonably expect the solid solution of modified Miki to have a lithium ion conductivity at room temperature that encompasses or at least overlaps the claimed range of superior or equal to 2.0 x 10-5 S/cm and inferior or equal to 3.0 10-5 S/cm.
Selection of an ionic conductivity at room temperature within the claimed range would have been obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, to optimize the safety and discharge/charge rates for modified Miki’s battery with a reasonable expectation of success and without undue experimentation [MPEP 2144.05(II)].
Regarding Claim 22, modified Miki discloses all limitations as set forth above. Miki further discloses a solid-state rechargeable lithium ion battery comprising a negative electrode contacting the solid solution electrolyte ([0030 – 0031];[0034];[0037]).
While modified Miki generally teaches using lithium metal as an electrode material ([0030]), modified Miki does not particularly disclose a solid-state battery embodiment comprising a negative electrode having a Li metal-based anode.
Albano teaches using a metal anode within a similar system {i.e. solid-state battery including solid electrolyte/active material cathode} ([0007 – 0008];[00095];[00098 – 00099]). The Li-metal anode is taught to provide batteries with higher volumetric-gravimetric energy density ([0007];[000104]).
Therefore, it would have been obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, to modify the battery if Miki to include a Li-metal anode as the negative electrode, with a reasonable expectation of success in obtaining a battery with a higher volumetric-gravimetric energy density.
Regarding Claim 23, modified Miki discloses all limitations as set forth above. Miki teaches applying the electrode including the solid electrolyte in a solid-state battery, and further teaches obtaining a high-output solid state battery ([0034];[0041])
Albano teaches applying solid-state batteries with a similar system {i.e. solid-state battery including solid electrolyte/active material cathode} in vehicular applications ([0003 – 0008]; [00095];[00098 – 00099]).
Since Albano teaches that solid-state with similar systems to Miki are applicable in vehicles, and the battery of modified Miki utilizes the claimed LSGPO as a solid electrolyte, one with ordinary sill in the art would reasonably expect the battery of modified Miki to be capable of having an operating voltage superior or equal to 200 V and inferior or equal to 500 V such that the battery is suitable for use in an electric car.
Claim(s) 18 – 20 are rejected under 35 U.S.C. 103 as being unpatentable over Miki (US PG Pub. 2013/0295451 A1), Hodge ("Ionic conductivity of Li4SiO4, Li4GeO4, and their solid solutions." Journal of the American Ceramic Society 59, no. 7‐8, pp. 360-366, NPL provided), Ivanov-Shitz ("Growth and ionic conductivity of Li3+ xP1− xGexO4 (x= 0.34) single crystals." Crystallography Reports 48, pp.112-115) and Deng ("Structural and mechanistic insights into fast lithium-ion conduction in Li4SiO4–Li3PO4 solid electrolytes." Journal of the American Chemical Society 137, no. 28, pp. 9136-9145), as applied to claim 13 above, and further as evidenced by Koseva ("Thermal behavior of germanates with olivine structure." Thermochimica Acta 646, pp. 1-7, cited in previous Office action mailed 10/15/2025).
Regarding Claim 18, modified Miki discloses all limitations as set forth above. Modified Miki’s solid solution electrolyte, as established above, is an LSPGO material comprising Li, Si, P, Ge, and O in molar ratios within the claimed scope.
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Annotated Fig. 2(a) from Deng showing first and second peaks
Deng shows the XRD patterns of Li4SiO4-Li3PO4 systems with varying compositions represented by (1-z)Li4SiO4-(z)Li3PO4 where z = 0 – 1 (Refer to Fig. 2(a)). In the diffraction pattern, in a range of 2θ superior or equal to 27.5 and inferior or equal to 30.0±0.5°, a first and a second peak having a first and second intensity (Refer to annotated Fig.2(a) from Deng) are shown. Furthermore, in a range of 37.0±0.50° ≤ 2θ ≤ 47.0±0.50°, the peaks shown do not appear to have an intensity greater than the first and second intensities of the first and second peaks (Refer to annotated Fig.2(a) from Deng).
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Annotated Fig.3 from Koseva showing first and second peaks
Koseva shows an XRD patten for different germinates, including, Li4GeO4 (Fig. 3). In the diffraction pattern, in a range of 2θ superior or equal to 27.5 and inferior or equal to 30.0±0.5°, a first and a second peak having a first and second intensity (Refer to annotated Fig.3 from Koseva) are shown. Furthermore, in a range 37.0±0.50° ≤ 2θ ≤ 47.0±0.50°, the peaks shown do not appear to have an intensity greater than the first peak (Refer to annotated Fig.2(a) from Deng).
Since the LSGPO material of modified Miki is within the claimed range, and further would be prepared from solutions of Li4SiO4-Li4GeO4 -Li3PO4, as evidenced by the preparation methods taught by Hodge (Refer to 1st paragraph in Experimental Procedure section, pg. 361), Ivanov-Shitz (Refer to Experimental section, pg. 112), and Deng (Refer to 2.1 Synthesis section pg. 9137), one with ordinary skill in the art would reasonably expect, based on XRD patterns taught by Deng and Koseva, modified Miki’s solid solution electrolyte to comprise a crystal structure having the claimed XRD pattern when measured at a wavelength of 1.5418Å.
Regarding Claim 19, modified Miki discloses all limitations as set forth above. Modified Miki’s solid solution electrolyte, as established above, is an LSPGO material comprising Li, Si, P, Ge, and O in molar ratios within the claimed scope.
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Annotated Fig. 2(a) from Deng showing first and second peaks
In a second range of 2θ superior or equal to 21.0 and inferior or equal to 25.0±0.5°, the diffraction patterns in Deng further show three peaks with an intensity superior to the intensities of the first or second peak, which is within the claimed range of no more three peaks having an intensity superior to said first or second intensity (Refer to annotated Fig. 2(a)).
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Annotated Fig.3 from Koseva showing first and second peaks
In a second range of 2θ superior or equal to 21.0 and inferior or equal to 25.0±0.5°, the diffraction pattern in Koseva includes three peaks with two of the three peaks having an intensity superior to the first or second peak intensities (Refer to annotated Fig. 2(a)).
Since the LSGPO material of modified Miki is within the claimed range, and further would be prepared from solutions of Li4SiO4-Li4GeO4 -Li3PO4, as evidenced by the preparation methods taught by Hodge (Refer to 1st paragraph in Experimental Procedure section, pg. 361), Ivanov-Shitz (Refer to Experimental section, pg. 112), and Deng (Refer to 2.1 Synthesis section pg. 9137), one with ordinary skill in the art would reasonably expect, based on XRD patterns taught by Deng and Koseva, modified Miki’s solid solution electrolyte to comprise a crystal structure having the claimed XRD pattern when measured at a wavelength of 1.5418Å.
Regarding Claim 20, modified Miki discloses all limitations as set forth above. Modified Miki’s solid solution electrolyte, as established above, is an LSPGO material comprising Li, Si, P, Ge, and O in molar ratios within the claimed scope.
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Annotated Fig. 2(a) from Deng showing first and second peaks
In a second range of 2θ superior or equal to 34.0 and inferior or equal to 36.0±0.5°, the diffraction patterns in Deng further show no more than two peaks with an intensity superior to the intensities of the first or second peak, which is within the claimed range of no more three peaks having an intensity superior to said first or second intensity (Refer to annotated Fig. 2(a)).
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Annotated Fig.3 from Koseva showing first and second peaks
In a second range of 2θ superior or equal to 34.0 and inferior or equal to 36.0±0.5°, the diffraction pattern in Koseva does not appear to include peaks with an intensity superior to the intensities of the first or second peak, which is within the claimed range of no more three peaks having an intensity superior to said first or second intensity (Refer to annotated Fig. 2(a)).
Since the LSGPO material of modified Miki is within the claimed range, and further would be prepared from solutions of Li4SiO4-Li4GeO4 -Li3PO4, as evidenced by the preparation methods taught by Hodge (Refer to 1st paragraph in Experimental Procedure section, pg. 361), Ivanov-Shitz (Refer to Experimental section, pg. 112), and Deng (Refer to 2.1 Synthesis section pg. 9137), one with ordinary skill in the art would reasonably expect, based on XRD patterns taught by Deng and Koseva, modified Miki’s solid solution electrolyte to comprise a crystal structure having the claimed XRD pattern when measured at a wavelength of 1.5418Å.
Claim(s) 24 is rejected under 35 U.S.C. 103 as being unpatentable over Miki (US PG Pub. 2013/0295451 A1), Hodge ("Ionic conductivity of Li4SiO4, Li4GeO4, and their solid solutions." Journal of the American Ceramic Society 59, no. 7‐8, pp. 360-366, NPL provided), Ivanov-Shitz ("Growth and ionic conductivity of Li3+ xP1− xGexO4 (x= 0.34) single crystals." Crystallography Reports 48, pp.112-115) and Deng ("Structural and mechanistic insights into fast lithium-ion conduction in Li4SiO4–Li3PO4 solid electrolytes." Journal of the American Chemical Society 137, no. 28, pp. 9136-9145), as evidenced by Kim (US PG Pub. 2016/036557 A1), and further in view of Albano (WO 2018/089430 A1) and Snyder (US PG Pub. 2011/0300432 A1). {Examiner Note: All prior art was cited in previous Office action mailed 11/15/2025. For citations of the instant specification, the examiner utilizes the US PG Pub. version of the instant application: US 2022/0149427 A1.}
Regarding Claim 24, Miki discloses a catholyte, that is Miki teaches positive electrode material including active material particles, ion conductor particles, and solid electrolyte particles ([0023];[0029 – 0031];[0033 – 0034]) and thus teaches a composition which one with ordinary skill in the art would readily understand/recognize to be catholyte {i.e. The examiner is interpreting catholyte to mean a solid electrolyte/cathode material mixture which appears supported by [0046] of the instant specification }.
Miki further discloses a solid electrolyte suitable for a solid state-rechargeable lithium ion battery, that is Miki teaches a solid electrolyte used in an electrode for a solid state battery ([0023];[0031]).
Miki teaches using oxide-type non-crystalline solid electrolytes, sulfide-type non-crystalline solid electrolytes and crystalline oxides and oxynitrides for the solid electrolyte, and, as one example of a crystalline oxide teaches Li3.6Si0.6P0.4O4 {i.e. LSPO} ([0031]). Li3.6Si0.6P0.4O4 is partially within the scope of the claimed general formula Li(3.5+L+x)Si(0.5+s-x)P(0.5+p-x)Ge2xO4 , specifically in Li3.6Si0.6P0.4O4, L = 0.10 which is within the claimed range of -0.1 0≤ L ≤ 0.10; s = 0 which is within the claimed range of -0.10 ≤ s ≤ 0.10; p = 0.10 which is within the claimed range -0.10 ≤ p ≤ 0.10; a = 0 which is within the claimed range of -0.40 ≤ a ≤ 0.40; and x = 0, which is outside the claimed range of 0.0 < x ≤ 0.30.
Since Miki teaches a finite list of example solid electrolytes, it would have been obvious to one with ordinary skill in the art, before the effective filings date of the claimed invention, to select Li3.6Si0.6P0.4O4 as the solid electrolyte material of Miki, and thus obtain solid electrolyte consisting of a compound with a composition significantly similar to the claimed general formula, with a reasonable expectation of success that such a selection would be suitable for the solid electrolyte-including electrode of Miki.
Miki as established above; however, does not disclose an LSPO compound including germanium {i.e. LSPGO}; and therefore, does not specifically disclose a compound with the general formula of Li(3.5+L+x)Si(0.5+s-x)P(0.5+p-x)Ge2xO4, and more particularly the general formula of Li(3.5+x)Si(0.5-x)P(0.5-x)Ge2xO4, wherein 0.0 < x ≤ 0.3.
Hodge teaches solid solutions comprising Li4GeO4 and Li4SiO4, that increase in conductivity with increases in Li4GeO4 content (Table 1; Fig. 8; Section (2) Variation of Conductivity with Composition and Temperature, first paragraph pg. 363). Hodge further teaches that the increases in conductivity are a result of the Si in Li4SiO4 being replaced by Ge (Section (2) Variation of Conductivity with Composition and Temperature, second paragraph pg. 363). The molar ratios amounts of Ge taught by Hoge include 0.17, 0.25, and 0.33 and the particular formulas are Li4Si0.83Ge0.17O4, Li4Si0.75Ge0.25O4 , and Li4Si0.67Ge0.33O4, respectively (Table 1).
Ivanov-Shitz teaches a solid solution Li(3.5+x)P(1-x)GexO4 where x = 0.34 and the solid solution was prepared from equimolar amounts of Li3PO4 and Li4GeO4 (Abstract and Experimental section pg. 112). Ivanov-Shitz further teaches that an increase in conductivity was observed for the doped lithium phosphate solid solution in comparison to pure lithium phosphate solid solution (Results and Discussion section, second paragraph in right column pg. 113 and continuing in left column on pg. 114).
Deng teaches Li4SiO4-Li3PO4 solid electrolytes with varying compositions represented by (1-z)Li4SiO4-(z)Li3PO4 where z = 0 – 1 (Abstract). Deng further teaches that the intermediate compositions, z = 0.25, 0.50, and 0.75, provide ionic conductivities 3 – 4 orders of magnitude higher than when z = 0 and when z = 1, and further, based on Fig. 8, it appears that equal amounts of Si and P {i.e. x = 0.5}
provided the highest conductivity (3.2 Li-ion Conductivity and Dynamics section, pg. 9141).
Since Miki teaches an LSPO material with a composition that falls within Deng’s compositional scope, and Hodge and Ivanov-Shitz teach that solid solutions comprising Li4SiO4 or Li3PO4 achieve higher conductivities when doped with Ge, it would have been obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, to dope Miki’s LSPO material with Ge, and obtain a solid solution with the claimed elements of Li, S, P, Ge, and O, with a reasonable expectation of success in obtaining a solid electrolyte with increased conductivity.
Furthermore, since Hodge and Ivanov-Shitz teach molar ratios of Ge that are within/overlap the claimed molar ratio ranges, and Miki and Deng teach LSPO materials with molar ratios of Li, Si, P, and O that are within/overlap the claimed range, it would have been further obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, to prepare the LSPGO compound of modified Miki, with Li4SiO4, Li4GeO4 , and Li3PO4 in amounts that would provide Li, Si, P, Ge, and O within the claimed molar ranges, to optimize the lithium ion conductivity of the material, with a reasonable expectation of success and without undue experimentation [MPEP 2144.05(II)].
The solid electrolyte of modified Miki is not particularly disclosed to be a solid solution electrolyte; however, since Deng teaches that LSPO-type electrolytes are of a solid solution system (last paragraph in 1. Introduction section, pg. 9136), one with ordinary skill in the art would reasonably expect the LSPGO electrolyte material of modified Miki to necessarily and inherently be a solid solution electrolyte.
Furthermore, while modified Miki does not explicitly disclose an embodiment of a catholyte comprising the solid solution as established above, it would have been obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, to form a positive electrode with the solid solution electrolyte established above, and thus obtain the claimed catholyte, with a reasonable expectation of success in obtaining a positive electrode that is suitable for the solid-state battery taught in Miki.
For the cathode material, Miki particularly exemplifies using LixCoO2, LixNiO2, LixMn2O4, LixNi1/2Mn1/2O2, LixNi1/3Co1/3Mn1/3O2, Lix[NiyLi1/3-2y/3]O3 (0≦x≦1, 0<y<1/2), and lithium transition metal oxides e.g., LiNiMnCoO2, as provided by replacing the lithium or transition metal in the preceding lithium transition metal oxides with another element. The cathode materials exemplified in Miki overlap in scope with the claimed cathode material having the general formula Li1+kM’1-kO2, where M’= Ni1-x’-y’-z’Mnx’Coy’Az’ with -0.05≤k≤0.05, 0≤x'≤0.40, 0.05≤y'≤0.40, and 0≤z'≤0.05, wherein A is a doping element which is different to Li, M' and O, because z = 0.
Since Miki teaches a finite list of exemplary Li(NixMyCoz)O2 cathode materials, it would have been obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, to select a cathode material within the claimed scope, with a reasonable expectation of success that such a selection would be suitable for the cathode active material of the solid-state battery.
Modified Miki does not explicitly disclose the cathode material, as set forth above, comprising particles having a layered R-3m crystal structure; however, as evidenced by Kim in [0003], LiMO2 structured materials are crystalline with an R-3m space group; therefore, one with ordinary skill in the art would reasonably expect the LiMO2-type cathode material of modified Miki to necessarily and inherently have the claimed layered R-3m crystal structure.
Modified Miki does not explicitly disclose the catholyte having a D99 ≤ 50 µm.
Albano teaches, for a similar structure {i.e. active material/electrolyte electrode}, a preference for electrolyte nanoparticle sizes of 29 – 900 nanometers {i.e. 0.020 – 0.900 µm} and active material particles sizes (D50) of 5 – 10 µm ([0060];[0074]).
Snyder teaches adding ion conductive materials in an electrode wherein a size distribution of the ion conductive material is arranged to enhance ion conductivity of the material ([0031 – 0032]). Snyder further teaches a preference for particle sizes in the range of approximately 0.1-10 μm, and most preferably 0.5-5 μm, for both the ionic conductivity enhancing material and the electrochemically active material within the cathode, and that particles larger than 10 μm can interrupt the ionic conduction path and electron conduction path in the electronic network of the electrode ([0032]).
Therefore, since both Albano and Synder teach that particle sizes significantly lower than 50 µm are suitable for catholyte, it would have been obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, to have made the catholyte of modified Miki with a D99 ≤ 50 µm to optimize the ion conductivity of the particles while ensuring particle sizes that do not interrupt the ionic conduction path/electron conduction path in the electronic network of the electrode, with a reasonable expectation of success and without undue experimentation [See MPEP 2144.05(II)].
As established above, the catholyte of modified Miki is an LSPO material doped with Ge.
Modified Miki does not explicitly disclose the catholyte having a lithium ion conductivity 1.0 x 10-6 S/cm.
Albano teaches solid electrolyte conductivities, including LSPO, at working temperatures within the range of 10-6 and 10-1 S/cm ([00055];[0057]). Albano’s further teaches that such a conductivity range allows for safe operation of the solid-state battery at high temperatures with faster charge/discharge rates ([00055];[00092-00093];[00096];[000104]).
Deng also teaches LSPO materials that have ion conductivities within the range of 10-3 S/cm or higher (3.2 Li-ion Conductivity and Dynamics section, pg. 9141) and, as established above, both Hodge and Ivanov-Shitz teach that doping with Ge provides increases in conductivity for Li4SiO4 and Li3PO4 materials.
Therefore, Since modified Miki’s solid electrolyte compound is an LSPO compound including Ge, with a composition within the claimed scope, one with ordinary skill in the art would reasonably expect the catholyte of modified Miki to have a lithium ion conductivity of at least 1.0 x 10-6 S/cm.
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.
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/A.Y.O./Examiner, Art Unit 1751
/JONATHAN G LEONG/Supervisory Patent Examiner, Art Unit 1751 4/3/2026
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