DETAILED ACTION
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
This is a final office action in response to Applicant’s remarks and amendments filed on April 24, 2026. Claim 1 is currently amended. Claim 21 is canceled. Claims 1-12 are pending review in this action.
New grounds of rejection necessitated by Applicant’s amendments are presented below.
Information Disclosure Statement
The information disclosure statement submitted on April 24, 2026 has been considered by the examiner.
Claim Rejections - 35 USC § 102
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 and 6 are rejected under 35 U.S.C. 102(a)(2) as being anticipated by U.S. Pre-Grant Publication No. 2018/0294517, hereinafter Yersak.
Regarding claim 1, Yersak teaches a method for forming an electrolyte (abstract). The method comprises a step of ball-milling starting materials comprising Na2S (sodium sulfide) and P2O5 (an oxide material) (paragraphs [0043, 0046, 0033, 0006, 0010]). The method further includes a step of pressing the resulting material to form a solid-state electrolyte (paragraphs [0034, 0035, 0042]). The electrolyte is a fully amorphous sodium oxy-sulfide glass (paragraph [0036]) – therefore it is “in the form of a continuous glass”. Yersak teaches that the entire solid-state electrolyte is in the form of a continuous glass (paragraph [0036]).
Regarding claim 6, Yersak teaches that the ball-milling is performed at room temperature (paragraph [0046]).
Claim Rejections - 35 USC § 103
The text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
Claims 2-5, 7 and 10 are rejected under 35 U.S.C. 103 as being unpatentable over U.S. Pre-Grant Publication No. 2018/0294517, hereinafter Yersak.
Regarding claim 2, Yersak teaches that the starting materials are Na2S, P2S5 and P2O5 mixed at a molar ratio of x Na2S · (100-x-y) P2S5 · y P2O5, where x is in the range 50 to 90 and y is up to 20 (paragraphs [0006, 0010, 0035]).
Yersak’s optimum range of 50 to 90 overlaps the instant application's optimum value of 75 for the molar fraction of Na2S in the claimed composition. It has been held that in the case where claimed ranges “overlap or lie inside ranges disclosed by the prior art” a prima facie case of obviousness exists. See MPEP 2144.05.
Regarding claim 3, Yersak teaches that y is up to 20 (paragraph [0035]).
Regarding claim 4, the values x = 75 and y = 20 are within the optimal ranges taught by Yersak. Selecting x = 75 and y = 20 results in the sodium oxy-sulfide glass Na3PS2O2, which satisfies the instantly claimed formula.
Yersak’s optimum ranges for the content of Na2S and P2O5 result in overlapping ranges for the molar content of the constitutive elements (Na, P, S and O) in the instant application. It has been held that in the case where claimed ranges “overlap or lie inside ranges disclosed by the prior art” a prima facie case of obviousness exists. See MPEP 2144.05.
Regarding claim 5, the values x = 75 and y = 6 are within the optimal ranges taught by Yersak. Selecting x = 75 and y = 6 results in the sodium oxy-sulfide glass Na3PS3.4O0.6, which satisfies the instantly claimed formula.
Yersak’s optimum ranges for the content of Na2S and P2O5 result in overlapping ranges for the molar content of the constitutive elements (Na, P, S and O) in the instant application. It has been held that in the case where claimed ranges “overlap or lie inside ranges disclosed by the prior art” a prima facie case of obviousness exists. See MPEP 2144.05.
Regarding claim 7, Yersak teaches that the pressing step is performed at a pressure in the range 0.1 MPa to 360 MPa (paragraph [0035]).
Yersak’s optimum range for the pressure of the pressing step overlaps the instant application's optimum range of 100 MPa to 450 MPa. It has been held that in the case where claimed ranges “overlap or lie inside ranges disclosed by the prior art” a prima facie case of obviousness exists. See MPEP 2144.05.
Regarding claim 10, Yersak teaches a pressing step to form a fully dense electrolyte layer. Yersak defines a “fully dense” material as one having a residual porosity of up to 15%, which corresponds to a relative density of 85% or greater (paragraph [0034]).
Yersak’s optimum range for the relative density overlaps the instant application's optimum range of greater than 95%. It has been held that in the case where claimed ranges “overlap or lie inside ranges disclosed by the prior art” a prima facie case of obviousness exists. See MPEP 2144.05.
Claims 8, 9 and 11 are rejected under 35 U.S.C. 103 as being unpatentable over U.S. Pre-Grant Publication No. 2018/0294517, hereinafter Yersak as applied to claim 1 and further in view of “Development of glass solid electrolytes for all-solid-state sodium batteries”, hereinafter Hayashi and Japanese Patent Publication No. 2012-121789, hereinafter Hayashi ‘789. (A machine of Hayashi ‘789 was provided with a prior office action).
Regarding claims 8, 9 and 11, Yersak teaches a fully amorphous sodium oxy-sulfide glass (paragraph [0036]).
The sodium oxy-sulfide glass is produced from the starting materials Na2S, P2S5 and P2O5 mixed at a molar ratio of x Na2S · (100-x-y) P2S5 · y P2O5, where x is in the range 50 to 90 and y is up to 20 (paragraphs [0006, 0010, 0035]).
The sodium oxy-sulfide glass is formed in a method comprising a ball-milling step, followed by a pressing step at a pressure in the range 0.1 MPa to 360 MPa to achieve full density (paragraphs [0034, 0035, 0046]).
Yersak does not report on the instantly claimed properties of the material.
Hayashi teaches the sodium oxy-sulfide solid electrolyte Na3PS2O2 (p.4, Section 3. Method of Research). This material is formed from the same starting materials as taught by Yarsek ball-milled at a molar ratio of 75 Na2S, 5 P2S5 and 20 P2O5.
Hayashi ‘789 teaches an analogous material ball-milled at room temperature and a speed of 510 rpm and pressed at 370 MPa (Hayashi‘789’s paragraphs [0024, 0025]).
It would have been obvious to the ordinarily skilled artist before the effective filing date of the claimed invention to select the molar ratio taught by Hayashi and the ball-milling speed and pressure taught by Hayashi ‘789 for the purpose of forming the material without undue experimentation and with a reasonable expectation of success.
Given that the material in the combination of Yersak, Hayashi and Hayashi ‘789 has the instantly disclosed and claimed structure and is formed by the instantly disclosed and claimed method, it is expected to have the instantly claimed properties.
Claim 12 is rejected under 35 U.S.C. 103 as being unpatentable over U.S. Pre-Grant Publication No. 2018/0294517, hereinafter Yersak as applied to claim 1 above, and further in view of Japanese Patent Publication No. 2012-121789, hereinafter Hayashi ‘789.
Regarding claim 12, Yersak teaches a ball milling step (paragraph [0046]).
Yersak fails to report the speed of the ball milling step.
The Hayashi ‘789 reference is directed to forming a solid electrolyte from ball-milled sodium sulfide. Hayashi ‘789 teaches a rotation speed in the range 50 to 600 rpm and explains that the higher the rotation speed, the more uniformly the raw materials may be mixed and reacted (paragraph [0017]). In Hayashi ‘789’s own method, the rotation speed is 510 rpm (paragraph [0024]).
Therefore it would have been obvious to the ordinarily skilled artist before the effective filing date of the claimed invention to set the rotation speed higher that 500 rpm, e.g. at 510 rpm, for the purpose of ensuring a complete and uniform reaction between the raw materials in Yersak’s mixture.
Claims 1-4, 6-9, 11 and 12 are rejected under 35 U.S.C. 103 as being unpatentable over “Development of glass solid electrolytes for all-solid-state sodium batteries”, hereinafter Hayashi in view of Japanese Patent Publication No. 2012-121789, hereinafter Hayashi ‘789.
Regarding claim 1, Hayashi teaches a method for forming an electrolyte. The method comprises a step of ball-milling starting materials comprising Na2S (sodium sulfide) and P2O5 (an oxide material) (p.4, Section 3. Method of Research). The method further includes a step of pressing the resulting material to form a dense, solid-state electrolyte body, (p.2, Section 1. Background). The electrolyte is a sodium oxy-sulfide glass, with the chemical formula Na3PS4-yOy (p. 7).
Hayashi’s method includes a heat treatment step after the ball-milling which creates some crystallinity in the solid electrolyte and renders it a glass ceramic (p. 7).
Hayashi fails to teach that the whole pressed sample is a continuous glass.
The Hayashi ‘789 reference is produced by the same author as the Hayashi reference and teaches forming an analogous solid electrolyte by ball-milling sodium sulfide and a glass former at room temperature and a rotation speed of 510 rpm (paragraphs [0015, 0016, 0024]). Hayashi ‘789 teaches pressing the ball-milled sample into pellets by applying pressure of 370 MPa prior to any heat treatment step and shows that at this stage the sample is a glass (paragraphs [0024-0026] and figures 1 and 2).
Therefore it would have been obvious to the ordinarily skilled artist before the effective filing date of the claimed invention to ball-mill Hayashi’s starting materials at room temperature and a rotation speed of 510 rpm and to press the ball-milled sample by applying a pressure of 370 MPa prior to heat treatment in the manner taught by Hayashi ’789 as these are the conditions and order of steps for forming a dense electrolyte body taught by Hayashi ‘789 or alternatively, at least for the purpose of being able to compare the amorphous sample’s structure and properties to the subsequently formed heat-treated glass ceramic sample.
Thus, prior to the heating step, in the combination of Hayashi and Hayashi ‘789, there would be a pressed solid electrolyte pellet, which is a sodium oxy-sulfide glass and given that the starting materials and the conditions for the formation of the pressed pallet are the same as instantly disclosed, it is expected that the entire solid-state electrolyte is in the form of a continuous glass.
Regarding claims 2-4, Hayashi teaches the starting materials Na2S, P2S5 and P2O5 (p.4, Section 3. Method of Research).
The chemical formula for the final product is Na3PS4-yOy, which means that y was varied over a range. Hayashi further explicitly mentions y = 2, which would result in the formula Na3PS2O2 (p. 7). (Hayashi’s y corresponds to the instantly claimed x).
Hayashi does not explicitly describe the molar ratio of the mixed materials, however, in order to arrive at the final product of Na3PS2O2, the starting ratio Na2S:P2S5:P2O5 would necessarily have to be 75:5:20.
Regarding claim 6, Hayashi as modified by Hayashi ‘789 teaches that the ball milling step is performed at room temperature (Hayashi ’789’s paragraph [0024]).
Regarding claim 7, Hayashi as modified by Hayashi ‘789 teaches that the pressing step is performed at a pressure of 370 MPa (Hayashi ‘789’s paragraphs [0024, 0025]).
Regarding claim 8, Hayashi teaches a solid-state electrolyte, which is formed through ball-milling the starting materials Na2S, P2S5 and P2O5 in quantities to achieve the final chemical formula Na3PS2O2 (p.4, Section 3. Method of Research). The method includes a subsequent step of pressing the resulting material to form a solid-state electrolyte pellet (p.2, Section 1. Background).
Hayashi as modified by Hayashi ‘789 teaches that the ball-milling is performed at room temperature and 510 rpm and the pressing is performed at 370 MPa (Hayashi‘789’s paragraphs [0024, 0025]).
Thus, the material of Hayashi as modified by Hayashi ‘789 (prior to the heating step) has the instantly disclosed and claimed structure and is formed by the instantly disclosed and claimed method, therefore it is expected to have the instantly claimed properties.
Regarding claim 9, the solid-state electrolyte of Hayashi as modified by Hayashi ‘789 is a glass (prior to the heating step) – therefore it is amorphous.
Regarding claim 11, Hayashi teaches a solid-state electrolyte, which is formed through ball-milling the starting materials Na2S, P2S5 and P2O5 in quantities to achieve the final chemical formula Na3PS2O2 (p.4, Section 3. Method of Research). The method includes a subsequent step of pressing the resulting material to form a solid-state electrolyte pellet (p.2, Section 1. Background).
Hayashi as modified by Hayashi ‘789 teaches that the ball-milling is performed at room temperature and 510 rpm and the pressing is performed at 370 MPa (paragraphs [0024, 0025]).
Thus, the material of Hayashi as modified by Hayashi ‘789 (prior to the heating step) has the instantly disclosed and claimed structure and is formed by the instantly disclosed and claimed method, therefore it is expected to have the instantly claimed properties.
Regarding claim 12, Hayashi as modified by Hayashi ‘789 teaches that the ball-milling step is performed at a rotation sped of 510 rpm (Hayashi ‘789’s paragraph [0024]).
Claim 5 is rejected under 35 U.S.C. 103 as being unpatentable over “Development of glass solid electrolytes for all-solid-state sodium batteries”, hereinafter Hayashi and Japanese Patent Publication No. 2012-121789, hereinafter Hayashi ‘789 as applied to claim 1 above as applied to claim 4 above, and further in view of U.S. Pre-Grant Publication No. 2012/0189918, hereinafter Tatsumisago.
Regarding claim 5, Hayashi teaches the starting materials Na2S, P2S5 and P2O5 (p.4, Section 3. Method of Research). The chemical formula for the final product is Na3PS4-yOy, which means that y was varied over a range (Hayashi’s y corresponds to the instantly claimed x). In an example, the final product is Na3PS2O2, which corresponds to the starting ratio Na2S:P2S5:P2O5 of 75:5:20.
Hayashi does not specify the values of y (instantly claimed x) used.
Tatsumisago teaches a sulfide solid state electrolyte formed by ball milling the starting materials Li2S, P2S5 and P2O5 (paragraphs [0039-0046]). Tatsumisago teaches that a preferred fraction for Li2S is 75 and P2S5:P2O5 are related by (25-x):x, where x is less than 25 (paragraphs [0026, 0024]).
Therefore it would have been obvious to the ordinarily skilled artist before the effective filing date of the claimed invention to vary Hayashi’s starting materials composition according to Tatsumisago’s teaching for the purpose of finding an optimum composition.
Within the range of values taught by the combination of Hayashi and Tatsumisago is the ratio 75:22.5:2.5, which would result in the final product formula of Na3PS3.75O0.25.
The optimum range in the combination of Hayashi and Tasumisago overlaps the instant application's optimum value for the molar fraction of oxygen in the claimed compound. It has been held that in the case where claimed ranges “overlap or lie inside ranges disclosed by the prior art” a prima facie case of obviousness exists. See MPEP 2144.05.
Furthermore, Hayashi as modified by Hayashi ‘789 and Tasumisago discloses the claimed invention except for the exact optimum value for the molar fraction of oxygen in the claimed compound in the instant application. It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to determine this exact optimum range, since it has been held that where the general conditions of a claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. In re Aller, 220 F.2d 454, 456 105 USPQ 233, 235 (CCPA 1955).
Claim 10 is rejected under 35 U.S.C. 103 as being unpatentable over “Development of glass solid electrolytes for all-solid-state sodium batteries”, hereinafter Hayashi and Japanese Patent Publication No. 2012-121789, hereinafter Hayashi ‘789 as applied to claim 1 above, and further in view of U.S. Pre-Grant Publication No. 2018/0351159, hereinafter Fujiki.
Regarding claim 10, Hayashi teaches a solid-state electrolyte, which is formed through ball-milling the starting materials Na2S, P2S5 and P2O5 in quantities to achieve the final chemical formula Na3PS2O2 (p.4, Section 3. Method of Research). The method includes a subsequent step of pressing the resulting material to form a solid-state electrolyte pellet (p.2, Section 1. Background).
Hayashi as modified by Hayashi ‘789 teaches that the ball-milling is performed at room temperature and 510 rpm and the pressing is performed at 370 MPa (paragraphs [0024, 0025]).
Thus, the material of Hayashi as modified by Hayashi ‘789 (prior to the heating step) has the instantly disclosed and claimed structure and is formed by the instantly disclosed and claimed method, therefore it is expected to have the instantly claimed properties.
Hayashi fails to report the relative density of the electrolyte pellets.
Fujiki teaches sulfide solid electrolytes formed by mechanical milling followed by pressing (paragraphs [0080, 0085]). Fujiki teaches that a relative density of 95% or greater is desirable, because at a high relative density there is a reduced number and size of gaps in the material and this allows for the prevention of a short-circuit in the battery (paragraphs [0083, 0084]).
Given that the solid electrolyte of Hayashi as modified by Hayashi ‘789 is substantially the same as instantly claimed and disclosed, it is expected that it would be capable of attaining the claimed relative density
Further, given that the solid electrolyte material in the combination of Hayashi and Hayashi ‘789 is subjected to a pressure within the instantly claimed and disclosed range, it is expected that it would attain the claimed relative density of greater than 95%. Finally, the ordinarily skilled artist before the effective filing date of the claimed invention would have been motivated to achieve a relative density greater than 95% in order to maximally reduce the size and number of gaps within the material as taught by Fujiki.
Response to Arguments
Applicant's arguments filed on April 24, 2026 have been fully considered but they are not persuasive.
Applicant argues that Yersak teaches a glass fiber composite with one or more dopants and due to its heterogenous nature cannot have an “entirely continuous glass”.
It is unclear why applicant is characterizing Yersak’s material as a “glass fiber composite”. The word “fiber” does not appear in Yersak.
Further, a review of Yersak’s disclosure indicates that the dopants referred to by applicant are not required components. Specifically, Yersak teaches that the dopants “may be used” (paragraph [0024]). Further, the glass compositions explicitly recited by Yersak make no mention of the dopants – see, e.g. paragraph [0035]. As such, the dopants are understood to be optional components.
Yersak’s glass compositions include the same starting materials as applicant’s (Na2S, P2S5 and P2O5) (paragraphs [0010, 0035]) and Yersak describes the finished glass film as fully amorphous (paragraph [0036]). When describing the effect of the pressing step on the material, Yersak says that the initial glass particles are consolidated into an amorphous body such that the boundaries of the original particles are not identifiable (paragraph [0039]). As such, the material is understood to be “in the form of a continuous glass”.
Applicant argues that the combination of Hayashi and Hayashi ‘789 does not produce continuous glass. To support this assertion, applicant points to instant figures 1a and 1b.
Instant figures 1a and 1b show the material Na3PS4. The material taught by Hayashi is Na3PS4-yOy. Applicant attributes the formation of the continuous glass under compression to the presence of oxygen which changes the viscoelastic behavior of the glass (Instant specification, paragraph [0053]). This argument is the purpose of including figures 1a and 1b in the instant specification, because they allow for a comparison of the effect of pressure on Na3PS4 and on an oxy-sulfide of the class Na3PS4-yOy.
As such, compressing Hayashi’s ball-milled Na3PS4-yOy at a pressure of 370 MPa as described by Hayashi ‘789 is expected to result in the continuous glass found by applicant when subjecting the same material to the same pressure.
Applicant argues that modifying Hayashi to form an entirely continuous glass would make the reference unusable for its intended purpose of providing an electrolyte that includes crystalline regions (a glass-ceramic).
As the prior and current office actions make clear, the modification in Hayashi is not intended to change Hayashi’s final product. The only modifications – to the extent that they are modifications – are the conditions and order (ball milling rotation speed and pressing pressure) for the steps Hayashi already teaches. Modifying Hayashi with Hayashi ‘789 does not change Hayashi’s final product – following the heating step, the final product of Hayashi as modified by Hayashi ‘789 would still be a glass-ceramic. However, the intermediate product – prior to the heating step – would have the instantly claimed structure.
It is noted that the instant claims are directed to method steps for forming an electrolyte. The ball milling and pressing steps of Hayashi as modified by Hayashi ‘789 are steps for forming an electrolyte. The instant claims as phrased do not exclude additional steps or further modifications of the electrolyte that may be taught in the prior art.
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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LILIA V. NEDIALKOVA
Examiner
Art Unit 1724
/MIRIAM STAGG/Supervisory Patent Examiner, Art Unit 1724
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