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 .
Continued Examination Under 37 CFR 1.114
A request for continued examination under 37 CFR 1.114, including the fee set forth in 37 CFR 1.17(e), was filed in this application after final rejection. Since this application is eligible for continued examination under 37 CFR 1.114, and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114. Applicant's submission filed on 11/20/25 has been entered.
Claim Status
Claims 1-2 are amended.
Claims 7-8 are new.
Response to Arguments
Applicant's arguments filed 11/20/25 have been fully considered but they are not persuasive. Applicant argues that the instant application differs from the cited references as follows:
Liu in view of Slobodyuk fails to disclose that the material represented by Li4ZrF8 satisfies the feature “the ratio of FWHM to FWHMSi is 1.25 or more”.
The claimed range of the ratio of FWHM to FWHMSi is critical.
Solid electrolyte materials obtained by mechanochemical reaction have a broadened XRD peal reflecting the lattice distortion responsible for enhanced Li-ion conductivity.
In regards to argument a, applicant’s arguments have been considered but are moot because the new ground of rejection does not rely on any reference applied in the prior rejection of record for any teaching or matter specifically challenged in the argument.
In regards to argument b, the arguments are not commensurate in scope with the claimed subject matter and the data shown in Table 1 does not support the criticality of the ratio claimed. The results shown in instant specification Table 1 indicate that increasing heat treatment temperature results in a lower ratio of FWHM/FWHMSi. This heat treatment step is not required by the Claims. Further, Comparative Example 1 is not made using a ball milling step while Examples 1-9 include a ball milling step (pp. 14-19 instant specification).
Regarding argument c, the instant claims are directed towards a solid electrolyte material with certain properties formed by a mechanochemical process and the determination of patentability is based on the product itself. “[E]ven though product-by-process claims are limited by and defined by the process, determination of patentability is based on the product itself. The patentability of a product does not depend on its method of production. If the product in the product-by-process claim is the same as or obvious from a product of the prior art, the claim is unpatentable even though the prior product was made by a different process.” In re Thorpe, 777 F.2d 695, 698, 227 USPQ 964, 966 (Fed. Cir. 1985) (MPEP 2113). Additionally, attorney arguments directed towards the method of forming the product and the specific crystal microstructure cannot take the place of evidence.
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.
Claims 1-8 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 1 contains the limitation “in an X-ray diffraction pattern obtained by an X-ray diffraction measurement of the solid electrolyte material using a Cu-Ka ray, a ratio of a value of a full width at half maximum of a peak having a highest intensity within a range of a diffraction angle 20 from 42.50 to 44.7 to a value of a full width at half maximum of a peak corresponding to a (111) plane of Si in an X-ray diffraction pattern of Si measured under a same condition as in the X-ray diffraction measurement is more than 1.25 or more”. X-ray diffraction measurements depend on the parameters of the measurement and different parameters will affect peak values. The current claim language requires a comparison of X-ray diffraction data collected under conditions that are unknown, therefore rendering the claim limitations unclear.
Claims 2-8 are rejected at least by virtue of their dependence on claim 1.
Claim 2 contains the limitation “in a conversion pattern in which a horizontal axis of the X-ray diffraction pattern is converted from the diffraction angle 20 to q, a ratio of a value of a full width at half maximum of a peak having a highest intensity within a range of q from 2.96 to 3.10 to a value of a full width at half maximum of a peak corresponding to a (111) plane of Si in a conversion pattern of Si measured under the same condition is more than 1.19 1.25 or more”. X-ray diffraction measurements depend on the parameters of the measurement and different parameters will affect peak values. The current claim language requires a comparison of converted X-ray diffraction data collected under conditions that are unknown therefore rendering the claim limitations unclear.
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.
This application currently names joint inventors. In considering patentability of the claims the examiner presumes that the subject matter of the various claims was commonly owned as of the effective filing date of the claimed invention(s) absent any evidence to the contrary. Applicant is advised of the obligation under 37 CFR 1.56 to point out the inventor and effective filing dates of each claim that was not commonly owned as of the effective filing date of the later invention in order for the examiner to consider the applicability of 35 U.S.C. 102(b)(2)(C) for any potential 35 U.S.C. 102(a)(2) prior art against the later invention.
Claim(s) 1-2, 7-8 are rejected under 35 U.S.C. 103 as being unpatentable over Liu et al. (High-Throughput Computation Screening of Li-Containing Fluorides for Battery Cathode Coatings) hereinafter "Liu", cited on the IDS filed on 7/14/2023, in view of Feinaeur et. al. (Unlocking the Potential of Fluoride-Based Solid Electrolytes for Solid-State Lithium Batteries, 2019) hereinafter "Feinauer".
Regarding claim 1, Liu teaches a cathode coating material comprising: Li;Zr; and F, wherein a ratio of an amount of substance of Li to an amount of substance of Zr is 3.5 or more (pg. 950 Results, “Li4ZrF8”; pg. 952 Table 1; pg. 952-954 Discussion). Liu teaches that cathode surface coatings can diminish side reactions during cycling and that surface coating materials should have good lithium-ion conductivity, a large electrochemical stability window, and good chemical stability with respect to a cathode and/or an electrolyte (pg. 948 Introduction). Liu teaches that Li-containing fluorides has low migration barriers indicating fairly good ionic conductivity can be expected in materials including Li4ZrF8 (pg. 952 Results and Table 1). Liu teaches that lithium metal fluorides generally exhibit poor Li-ion conductivity and it is desirable to have a metal fluoride compound with high ionic conductivity, phase stability, electrochemical stability, and chemical stability (abstract; p. 948-949 – Introduction).
Liu is silent as to the method of making Li4ZrF8.
However, Feinauer teaches that Li metal fluorides exhibit minimal interfacial mixing of metal fluoride-based electrolytes with oxide-based electrodes, improving the interfacial compatibility and further, metal fluorides are electrical insulators, a highly desirable property for electrolyte applications (p. 7197; abstract). Li-containing metal fluorides possess high chemical and electrochemical stability and excellent mechanical properties and can be manufactured by mechanical milling as well as chemical methods (p. 7197). Feinauer teaches that the ionic conductivity of a metal fluoride, for example β-Li3AlF6, could be increased by reducing the particle size via mechanical milling; specifically, β-Li3AlF6 can be synthesized via mechanical milling of LiF and AlF3 for 20 h at 600 rpm (abstract; p. 7198; p. 7202 – Methods; Mechanical milling to react two substrates meets the limitation of mechanochemical reaction).
Li4ZrF8 is a known lithium metal fluoride. Mechanical milling of precursor compounds is a known method for manufacturing lithium metal fluorides. Liu and Feinauer both teach the desirability of high ionic conductivity, phase stability, electrochemical stability, and chemical stability.
Therefore it would have been obvious to one of ordinary skill in the art, prior to the effective filing date of the claimed invention, to manufacture the Li; Zr; and F containing material (Li4ZrF8) taught by Liu using a mechanochemical process (such as mechanically milling substrates), as taught by Feinauer.
One of ordinary skill in the art would be motivated to manufacture the Li; Zr; and F containing material (Li4ZrF8) taught by Liu using a mechanochemical process (such as mechanically milling substrates), as taught by Feinauer to increase the Li-ion conductivity (abstract; p. 7198; p. 7202 – Methods). Further, one of ordinary skill in the art manufacture the Li; Zr; and F containing material (Li4ZrF8) taught by Liu using a mechanochemical process (such as mechanically milling substrates), as taught by Feinauer with a reasonable expectation of success because mechanical milling is a known method of producing lithium metal fluorides.
Liu and does not explicitly teach where a Li; Zr; and F containing material is used as a solid electrolyte.
However, it would have been obvious to one of ordinary skill in the art, prior to the effective filing date of the claimed invention, to have used the material comprising: Li; Zr; and F, taught by Liu as a lithium metal fluoride solid electrolyte material.
One of ordinary skill in the art could have used the material comprising: Li; Zr; and F, taught by Liu as a solid electrolyte material with a reasonable expectation of producing a functioning solid electrolyte layer because lithium metal fluoride compounds with good ionic conductivity are known in the art for use as solid electrolyte materials. Further, the selection of a known material, which is based upon its suitability for the intended use, is within the ambit of one of ordinary skill in the art. See In re Leshin, 125 USPQ 416 (CCPA 1960) (see MPEP §2144.07).
Modified Liu does not teach where, in an X-ray diffraction pattern obtained by an X-ray diffraction measurement of the solid electrolyte material using a Cu-Ka ray, a ratio of a value of a full width at half maximum of a peak having a highest intensity within a range of a diffraction angle 2θ from 42.5 to 44.7° to a value of a full width at half maximum of a peak corresponding to a (111) plane of Si in an X-ray diffraction pattern of Si measured under a same condition as in the X-ray diffraction measurement is more than 1.19.
However, modified Liu teaches a material comprising: Li;Zr; and F, wherein a ratio of an amount of substance of Li to an amount of substance of Zr is 3.5 or more and the material is made by a mechanochemical process (Liu pg. 950 Results, “Li4ZrF8”; Feinauer abstract; p. 7198; p. 7202 – Methods). Therefore, one of ordinary skill in the art would expect that should the material taught by modified Liu be subject to testing, such as X-ray diffraction measurement using a Cu-Ka ray and subsequent comparison to an X-ray diffraction measurement using a Cu-Ka ray of Si, the material would exhibit the claimed attributes. Absent specific claimed features that create the X-ray diffraction pattern ratio, one of ordinary skill in the art would reasonably expect the x-ray diffraction pattern of the material taught by modified Liu, when compared to an x-ray diffraction pattern of Si, to have the claimed ratio of a value of a full width at half maximum of a peak having a highest intensity within a range of a diffraction angle 2θ from 42.50 to 44.7 to a value of a full width at half maximum of a peak corresponding to a (111) plane of Si in an X-ray diffraction pattern of Si measured under a same condition as in the X-ray diffraction measurement.
Regarding claim 2, modified Liu teaches the solid electrolyte material according to claim 1.
Modified Liu does not teach wherein in a conversion pattern in which a horizontal axis of the X-ray diffraction pattern is converted from the diffraction angle 2θ to q, a ratio of a value of a full width at half maximum of a peak having a highest intensity within a range of q from 2.96 to 3.10 to a value of a full width at half maximum of a peak corresponding to a (111) plane of Si in a conversion pattern of Si measured under the same condition is more than 1.25, where q = 4πsinθ/λ and A represents a wavelength of an X-ray used for the X-ray diffraction measurement.
However, modified Liu teaches a material comprising: Li;Zr; and F, wherein a ratio of an amount of substance of Li to an amount of substance of Zr is 3.5 or more and the material is made by a mechanochemical process (Liu pg. 950 Results, “Li4ZrF8”; Feinauer abstract; p. 7198; p. 7202 – Methods). Therefore, one of ordinary skill in the art would expect that should the material taught by modified Liu be subject to testing, such as X-ray diffraction measurement using a Cu-Ka ray and subsequent comparison to an X-ray diffraction measurement using a Cu-Ka ray of Si, the material would exhibit the claimed attributes. Absent specific claimed features that create the X-ray diffraction pattern ratio, one of ordinary skill in the art would reasonably expect the x-ray diffraction pattern of the material taught by modified Liu, when compared to an x-ray diffraction pattern of Si, to have the claimed ratio of a ratio of a value of a full width at half maximum of a peak having a highest intensity within a range of q from 2.96 to 3.10 to a value of a full width at half maximum of a peak corresponding to a (111) plane of Si in a conversion pattern of Si measured under the same condition is more than 1.25.
Regarding claim 7, modified Liu teaches the solid electrolyte material according to claim 2.
Modified Liu does not teach wherein the ratio is 3.88.
However, modified Liu teaches a material comprising: Li;Zr; and F, wherein a ratio of an amount of substance of Li to an amount of substance of Zr is 3.5 or more and the material is made by a mechanochemical process (Liu pg. 950 Results, “Li4ZrF8”; Feinauer abstract; p. 7198; p. 7202 – Methods). Therefore, one of ordinary skill in the art would expect that should the material taught by modified Liu be subject to testing, such as X-ray diffraction measurement using a Cu-Ka ray and subsequent comparison to an X-ray diffraction measurement using a Cu-Ka ray of Si, the material would exhibit the claimed attributes. Absent specific claimed features that create the X-ray diffraction pattern ratio, one of ordinary skill in the art would reasonably expect the x-ray diffraction pattern of the material taught by modified Liu, when compared to an x-ray diffraction pattern of Si, to have the claimed ratio of a value of a full width at half maximum of a peak having a highest intensity within a range of a diffraction angle 2θ from 42.50 to 44.7 to a value of a full width at half maximum of a peak corresponding to a (111) plane of Si in an X-ray diffraction pattern of Si measured under a same condition as in the X-ray diffraction measurement.
Regarding claim 8, modified Liu teaches the solid electrolyte material according to claim 2.
Modified Liu does not teach wherein the ratio in the conversion pattern is 3.88 or less.
However, modified Liu teaches a material comprising: Li;Zr; and F, wherein a ratio of an amount of substance of Li to an amount of substance of Zr is 3.5 or more and the material is made by a mechanochemical process (Liu pg. 950 Results, “Li4ZrF8”; Feinauer abstract; p. 7198; p. 7202 – Methods). Therefore, one of ordinary skill in the art would expect that should the material taught by modified Liu be subject to testing, such as X-ray diffraction measurement using a Cu-Ka ray and subsequent comparison to an X-ray diffraction measurement using a Cu-Ka ray of Si, the material would exhibit the claimed attributes. Absent specific claimed features that create the X-ray diffraction pattern ratio, one of ordinary skill in the art would reasonably expect the x-ray diffraction pattern of the material taught by modified Liu, when compared to an x-ray diffraction pattern of Si, to have the claimed ratio of a ratio of a value of a full width at half maximum of a peak having a highest intensity within a range of q from 2.96 to 3.10 to a value of a full width at half maximum of a peak corresponding to a (111) plane of Si in a conversion pattern of Si measured under the same condition is more than 1.25.
Claim(s) 3-4 is rejected under 35 U.S.C. 103 as being unpatentable over Liu (High-Throughput Computation Screening of Li-Containing Fluorides for Battery Cathode Coatings) in view of Feinaeur (Unlocking the Potential of Fluoride-Based Solid Electrolytes for Solid-State Lithium Batteries, 2019), as applied above, in further view of Dugat et al. (Crystal Structures of Li4ZrF8 and Li3Zr4F19 and Reinvestigation of the LiF-ZrF4 Phase Diagram, 1995).
Regarding claim 3, modified Liu teaches the solid electrolyte material according to claim 1. Liu further teaches a material represented by the following composition formula (1), LiXZrF4+X ... (1) where a mathematical relation 3.5 ≤ x is satisfied (Liu pg. 950 Results, “Li4ZrF8”; pg. 952 Table 1; pg. 952-954 Discussion). Liu teaches additional cathode coating materials with crystalline phases such as LixMF6 materials (pg. 952 Results) including crystalline Li2ZrF6, Li3AlF6 (pg. 954 Discussion).
Modified Liu is silent as to a crystalline phase of the material represented by formula (1), LiXZrF4+X ... (1) where a mathematical relation 3.5 ≤ x is satisfied.
However, Dugat teaches that Li4ZrF8 made by reacting LiF and ZrF4 comprises a crystalline phase of Li4ZrF8 (Experimental p. 187-188), meeting the claimed composition formula (1), LiXZrF4+X ... (1) where a mathematical relation 3.5 ≤ x is satisfied (Experimental p. 187-188).
Li4ZrF8 containing a crystalline phase is known in the prior art; therefore absent evidence to the contrary, one of ordinary skill in the art would expect the Li4ZrF8 taught by modified Liu to have a crystalline phase.
Regarding claim 4, Liu further teaches wherein a mathematical relation 3.5 ≤x ≤ 4.5 is satisfied (Liu pg. 950 Results, “Li4ZrF8”; pg. 952 Table 1; pg. 952-954 Discussion).
Claim(s) 5-6 are rejected under 35 U.S.C. 103 as being unpatentable over Liu (High-Throughput Computation Screening of Li-Containing Fluorides for Battery Cathode Coatings) in view of Feinaeur (Unlocking the Potential of Fluoride-Based Solid Electrolytes for Solid-State Lithium Batteries, 2019) in further view of Dugat (Crystal Structures of Li4ZrF8 and Li3Zr4F19 and Reinvestigation of the LiF-ZrF4 Phase Diagram, 1995), as applied above, in further view of Iwamoto (Pat. App. Pub. No. US20170309964A1).
Regarding claim 5, modified Liu teaches the solid electrolyte material according to claim 1. Liu teaches where a material comprising: Li;Zr; and F is used in a cathode (pg. 950 Results, “Li4ZrF8”; pg. 952 Table 1; pg. 952-954 Discussion).
Modified Liu does not teach a battery comprising: a positive electrode; a negative electrode; and an electrolyte layer provided between the positive electrode and the negative electrode, wherein at least one selected from the group consisting of the positive electrode, the negative electrode, and the electrolyte layer includes the solid electrolyte material.
However, Iwamoto teaches a battery comprising: a positive electrode; a negative electrode; and an electrolyte layer provided between the positive electrode and the negative electrode, wherein at least one selected from the group consisting of the positive electrode, the negative electrode (par. [0005]; par. [0045]).
It would have been obvious to one of ordinary skill in the art to use the solid electrolyte material taught by modified Liu in a battery as taught by Iwamoto.
One of ordinary skill in the art could have used the solid electrolyte material as taught by modified Liu in the battery taught by Iwamoto with a reasonable expectation of producing a solid electrolyte battery. The selection of a known material, which is based upon its suitability for the intended use, is within the ambit of one of ordinary skill in the art. See In re Leshin, 125 USPQ 416 (CCPA 1960) (see MPEP §2144.07).
In regard to claim 6, modified Liu in view of Iwamoto teaches battery according to claim 5.
Iwamoto further teaches wherein the electrolyte layer includes a first electrolyte layer and a second electrolyte layer, the first electrolyte layer is disposed between the positive electrode and the negative electrode, the second electrolyte layer is disposed between the first electrolyte layer and the negative electrode (par. [0045]). Iwamoto teaches that a first electrolyte layer and a second layer electrolyte reduce the probability of a short circuit occurring due to pinholes generated in a solid electrolyte layer (par. [0063]). Iwamoto further teaches where a first solid electrolyte and second solid electrolyte can be chosen from known solid electrolyte materials (par. [0079]).
It would have been obvious to one of ordinary skill in the art to include a first electrolyte layer and a second electrolyte layer as taught by Iwamoto.
One of ordinary skill in the art would have been motivated to include a first electrolyte layer and a second electrolyte layer as taught by Iwamoto to reduce the probability of a short circuit occurring due to pinholes generated in a solid electrolyte layer (par. [0063]).
Further it would have been obvious to one of ordinary skill in the art to include the solid electrolyte material taught by modified Liu in the first electrolyte layer taught by Iwamoto.
One of ordinary skill in the art could have selected the solid electrolyte material taught by modified Liu as the solid electrolyte material for the first electrolyte layer taught by Iwamoto to achieve the predictable result of a solid-state battery. The selection of a known material, which is based upon its suitability for the intended use, is within the ambit of one of ordinary skill in the art. See In re Leshin, 125 USPQ 416 (CCPA 1960) (see MPEP §2144.07).
Conclusion
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/F.B.A./Examiner, Art Unit 1728
/MATTHEW T MARTIN/Supervisory Patent Examiner, Art Unit 1728