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 .
Election/Restrictions
Applicant’s election of Group I, claims 1-10, drawn to a solid electrolyte in the reply filed on 04/21/2026 is acknowledged. Because applicant did not distinctly and specifically point out the supposed errors in the restriction requirement, the election has been treated as an election without traverse (MPEP § 818.01(a)).
Claims 11-20 are withdrawn from further consideration pursuant to 37 CFR 1.142(b) as being drawn to a nonelected Group II, there being no allowable generic or linking claim. Election was made without traverse in the reply filed on 04/21/2026.
Priority
Receipt is acknowledged of certified copies of papers required by 37 CFR 1.55.
Information Disclosure Statement
The information disclosure statement (IDS) submitted on 06/29/2023, and 03/05/2024 are in compliance with the provisions of 37 CFR 1.97. Accordingly, the information disclosure statement is being considered by the examiner.
Specification
Applicant is reminded of the proper language and format for an abstract of the disclosure.
The abstract should be in narrative form and generally limited to a single paragraph on a separate sheet within the range of 50 to 150 words in length. The abstract should describe the disclosure sufficiently to assist readers in deciding whether there is a need for consulting the full patent text for details.
The language should be clear and concise and should not repeat information given in the title. It should avoid using phrases which can be implied, such as, “The disclosure concerns,” “The disclosure defined by this invention,” “The disclosure describes,” etc. In addition, the form and legal phraseology often used in patent claims, such as “means” and “said,” should be avoided.
The abstract of the disclosure is objected to because it contains three paragraphs and includes the divisions/headings "[Chemical Formula 1]", and "[ Chemical Formula 2]". A corrected abstract of the disclosure is required and must be presented on a separate sheet, apart from any other text. See MPEP § 608.01(b) for abstract formatting requirements.
Claim Rejections - 35 USC § 103
In the event the determination of the status of the application as subject to AIA 35 U.S.C. 102 and 103 (or as subject to pre-AIA 35 U.S.C. 102 and 103) is incorrect, any correction of the statutory basis (i.e., changing from AIA to pre-AIA ) for the rejection will not be considered a new ground of rejection if the prior art relied upon, and the rationale supporting the rejection, would be the same under either status.
The 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.
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.
Claims 1-2, 4, and 9-10 are rejected under 35 U.S.C. 103 as being unpatentable over Li et al. (US 20260038873 A1, published U.S. patent application with provisional application filed on Oct. 30, 2020).
Regarding claim 1, Li teaches a solid electrolyte ([0004-0005]: multilayers of solid state electrolytes) comprising:
a core comprising a first electrolyte represented by Chemical Formula 1 ([0011, 0084, 0087]: the first solid-state electrolyte may be selected from Table 1, specifically, solid electrolyte number 5 and 6, and the solid-state electrolyte may adopt a core-shell structure);
and a shell comprising a second electrolyte represented by Chemical Formula 2 ([0012,0084, 0087]: the second solid-state electrolyte may also be selected from Table 1 and the solid-state electrolyte may adopt a core-shell structure shell electrolyte from table 1, specifically, solid electrolyte number 1 and 5 ) and disposed on a surface of the core ([0084, 0087]: the solid state electrolyte may adopt a core-shell structure),
[Chemical Formula 1] LiaPSbX1c, wherein 4≤a≤7, 3≤b≤7, 0≤c≤2, and X1 comprises Br or I; and
[Chemical Formula 2] LidPSeX2f, wherein 4≤d≤7, 3≤e≤7, 0≤f≤2, and X2 comprises Cl or Br; and
an ionic radius of X1 is greater than an ionic radius of X2.
Specifically, Li teaches a rechargeable solid-state battery including multilayers of solid-state electrolytes ([0004-0005, 0076]), wherein a first and second solid-state electrolyte may be selected from Table 1 ([0011, 0012, 0078, 0087]). Li further teaches that the solid-state electrolytes may adopt a core-shell structure ([0016, 0084, 0087]).
Li specifically teaches halide-containing sulfide solid-state electrolytes including Li₆PS₅Cl, Li₆PS₅Br, and Li₆PS₅I in Table 1. Li further teaches that different electrolyte compositions provide different properties, including conductivity, and electrochemical stability, and that different core and shell compositions may be selected to achieve desired performance characteristics ([0016, 0081]).
Accordingly, it would have been obvious to a person of ordinary skill in the art to select Li₆PS₅I or Li₆PS₅Br as the first electrolyte and Li₆PS₅Cl or Li₆PS₅Br as the second electrolyte based on their recognized suitability for use in solid-state electrolyte systems and their known properties. The selection of known materials, according to suitability or intended use, is within the ambit of one of ordinary skill in the art. See MPEP 2144.07; See In re Leshin.
It also would have been obvious to configure the selected electrolytes in a core-shell structure because Li expressly teaches that core-shell structures provide advantageous electrolyte properties ([0016, 0087]). A person of ordinary skill in the art would have been motivated to combine different electrolyte materials in such a structure to obtain the predictable benefits taught by Li, including improved stability and electrochemical performance ([0016, 0081]).
Further, when Li₆PS₅I or Li₆PS₅Br is selected for the first electrolyte and Li₆PS₅Cl or Li₆PS₅Br is selected for the second electrolyte, the ionic radius of X1 would be greater than the ionic radius of X2. In one embodiment, Li₆PS₅Br is the first electrolyte and Li₆PS₅Cl is the second electrolyte, accordingly, Br for X1 and Cl for X2 results in the ionic radius of X1 being greater than the ionic radius of X2.
In another embodiment, Li₆PS₅I is the first electrolyte and Li₆PS₅Cl or Li₆PS₅Br are the second electrolyte. Accordingly, I for X1 and Cl or Br for X2 results in the ionic radius of X1 being greater than the ionic radius of X2 because iodide ions have larger ionic radii than bromide and chloride ions.
Regarding claim 2, Li teaches all limitations of claim 1, as stated above. Li further teaches a limitation wherein the first electrolyte comprises Li6PS5Br ([0011], Table 1: electrolyte number 5, y = 0); and the second electrolyte comprises Li6PS5Cl ([0011, 0012], Table 1: electrolyte number 1).
Li specifically teaches Li₆PS₅Br and Li₆PS₅Cl as sulfide solid-state electrolytes in Table 1, and further teaches that different solid-state electrolytes may be used in a core-shell particle structure ([0087]: the solid state electrolyte may adopt a core-shell structure).
Further, Li teaches that the first solid-state electrolyte and the second solid-state electrolyte may differ in composition ([0016]). The selection of known materials, according to suitability or intended use, is within the ambit of one of ordinary skill in the art. See MPEP 2144.07. Thereby rendering obvious selecting Li₆PS₅Br as the first electrolyte and Li₆PS₅Cl as the second electrolyte.
Regarding claim 4, Li teaches all limitations of claim 1, as stated above. Li further teaches a limitation wherein a particle size D50 of the second electrolyte is about 0.5 μm to 20 μm (Table 15, particle size of Li₆PS₅Cl (LPSCl)).
Li specifically teaches that Li₆PS₅Cl particles have a particle size of about 1-3 µm (Table 15), which overlaps the claimed range of about 0.5 µm to 20 µm. 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(I).
Regarding claim 9, Li teaches all limitations of claim 1, as stated above. Li further teaches a skin layer disposed on a surface of the shell and comprising a third electrolyte represented by Chemical Formula 3,
[Chemical Formula 3] LigPShX3i, wherein 4≤g≤7, 3≤h≤7, O≤i≤2, and X3 comprises Cl; and the ionic radius of X2 is greater than an ionic radius of X3 ([0004-0005, 0016, 0087], Table 1).
Specifically, Li teaches a multilayer solid-state electrolyte including at least two layers and, in some embodiments, at least three layers ([0004-0005, 0078]). Li further teaches that the first and/or second solid-state electrolytes may adopt a core-shell structure and that different core and shell compositions may provide different electrochemical properties ([0016]).
Therefore, it would have been obvious to include an additional skin layer disposed on the surface of the shell because Li expressly teaches multilayer solid-state electrolyte structures including multiple electrolyte layers and teaches that different electrolyte compositions may be combined to provide advantageous electrochemical properties, including improved conductivity, stability, and electrolyte performance ([0004-0005, 0016, 0076, 0084, 0087). A person of ordinary skill in the art would have been motivated to provide the additional skin layer using a known halide-containing sulfide electrolyte in order to obtain the predictable benefits taught by Li.
Li specifically teaches halide-containing sulfide electrolytes including Li₆PS₅Cl (electrolyte 1), Li₆PS₅Br (electrolyte 5), and Li₆PS₅I (electrolyte 6) in Table 1. The selection of known materials, according to suitability or intended use, is within the ambit of one of ordinary skill in the art. See MPEP 2144.07; See In re Leshin.
Accordingly, it would have been obvious to one of ordinary skill in the art to configure Li’s disclosed multilayer electrolyte having at least three layers such that: (1) a core comprises a first electrolyte, (2) a shell comprises a second electrolyte disposed on a surface of the core, and (3) a third layer comprises a skin layer disposed on a surface of the shell. In one embodiment, Li₆PS₅I (electrolyte 6) may be selected as the core electrolyte, Li₆PS₅Br (electrolyte 5) may be selected as the shell electrolyte, and Li₆PS₅Cl (electrolyte 1) may be selected as the skin electrolyte. In this arrangement, the third electrolyte represented by Chemical Formula 3 comprises Cl, while the second electrolyte represented by Chemical Formula 2 comprises Br, thereby resulting in the ionic radius of X2 being greater than the ionic radius of X3 because bromide ions have a larger ionic radius than chloride ions.
Further, Li teaches that multilayer solid-state electrolytes having different electrolyte compositions may provide different properties, such as conductivity ([0016]). Therefore, it would have been obvious before the effective filing date of the claimed invention that one of ordinary skill in the art would utilize three different halide-containing sulfide electrolytes in Li’s disclosed multilayer structure in order to optimize conductivity and electrolyte performance ([0016]).
Regarding claim 10, Li teaches all limitations of claim 9, as stated above. Li further teaches a limitation wherein the first electrolyte comprises Li6PS5I; the second electrolyte comprises Li6PS5Br; and the third electrolyte comprises Li6PS5Cl ([0005, 0016, 0087], Table 1).
As discussed with respect to claim 9, Li specifically teaches halide-containing sulfide electrolytes including Li₆PS₅I (electrolyte 6), Li₆PS₅Br (electrolyte 5), and Li₆PS₅Cl (electrolyte 1) in Table 1. Li further teaches a multilayer solid-state electrolyte including at least three layers ([0005]) and teaches that the first and/or second solid-state electrolytes may adopt a core-shell particle structure with different electrolyte compositions providing different properties ([0016], [0087]). The selection of known materials, according to suitability or intended use, is within the ambit of one of ordinary skill in the art. See MPEP 2144.07.
Accordingly, it would have been obvious to one of ordinary skill in the art to configure Li’s disclosed multilayer electrolyte such that Li₆PS₅I (electrolyte 6) is selected as the core electrolyte, Li₆PS₅Br (electrolyte 5) is selected as the shell electrolyte disposed on the core, and Li₆PS₅Cl (electrolyte 1) is selected as the skin electrolyte disposed on the shell in order to optimize conductivity and electrolyte performance ([0016]).
Claims 3 and 5 are rejected under 35 U.S.C. 103 as being unpatentable over Li, as applied to claim 1 above, and further in view of Yoon et al. (US 20190198916 A1).
Regarding claim 3, Li teaches all limitations of claim 1, as stated above. Li does not teaches a limitation wherein a particle size D50 of the first electrolyte is about 1μm to 40μm.
However, Yoon teaches this limitation ([0010, 0015, 0016, 0051, 0053]). Yoon specifically teaches that the first solid electrolyte may include Li₆PS₅Br ([0010, 0053]) and may have a particle size of about 5 to 20 µm as measured by D50 ([0015-0016, 0051]), which overlaps the claimed range of about 1 µm to 40 µm. Yoon further teaches that when the particle size of the first solid electrolyte is less than about 5 µm, nano-sized fine powder may be included and slurry mixing may become problematic, whereas when the particle size is greater than about 20 µm, pinholes may form in the electrode due to the large particle size, thereby deteriorating battery performance ([0051]). Thus, Yoon teaches optimization of the particle size of the first electrolyte to improve battery performance ([0051]).
It has been held that where the claimed ranges “overlap or lie inside ranges disclosed by the prior art,” a prima facie case of obviousness exists. See MPEP 2144.05(I).
Further, Li and Yoon are considered to be analogous to the claimed invention because both references are directed to sulfide solid electrolytes for solid state batteries.
Therefore, it would have been obvious before the effective filing date of the claimed invention that one of ordinary skill in the art would modify Li to use the particle size of about 5 to 20 µm of Yoon for the first electrolyte because Yoon teaches that excessively small or excessively large particle sizes may deteriorate battery performance ([0051]).
Regarding claim 5, Li teaches all limitations of claim 1, as stated above. Li does not teaches a limitation wherein a particle size D50 of the first electrolyte is 2 times to 5 times a particle size D50 of the second electrolyte.
However, the combination of Li and Yoon teaches this limitation. Specifically, Yoon teaches that the first solid electrolyte may include Li₆PS₅Br ([0010, 0053]) and may have a particle size of about 5 to 20 µm as measured by D50 ([0015-0016, 0051]). Yoon further teaches that when the particle size of the first solid electrolyte is less than about 5 µm, nano-sized fine powder may be included and slurry mixing may become problematic, whereas when the particle size is greater than about 20 µm, pinholes may form in the electrode due to the large particle size, thereby deteriorating battery performance ([0051]). Thus, Yoon teaches selecting the first electrolyte particle size within the range of about 5 to 20 µm to improve battery performance ([0051]).
Li teaches that the second electrolyte, Li₆PS₅Cl (LPSCl), may have a particle size of about 1–3 µm (Table 15).
For example, selecting a first electrolyte particle size of 5 µm and a second electrolyte particle size of 1 µm results in the first electrolyte particle size being 5 times the second electrolyte particle size. Further, selecting a first electrolyte particle size of 6 µm and a second electrolyte particle size of 3 µm results in the first electrolyte particle size being 2 times the second electrolyte particle size.
Thus, the combined teachings of Li and Yoon disclose particle size ratios overlapping the claimed range of 2 times to 5 times. It has been held that where the claimed ranges “overlap or lie inside ranges disclosed by the prior art,” a prima facie case of obviousness exists. See MPEP 2144.05(I).
Further, Li and Yoon are considered to be analogous to the claimed invention because both references are directed to sulfide solid electrolytes for solid state batteries.
Therefore, it would have been obvious before the effective filing date of the claimed invention that one of ordinary skill in the art would select particle sizes within the ranges taught by Li and Yoon such that the first electrolyte particle size is about 2 times to 5 times the second electrolyte particle size in order to optimize battery performance ([0051] of Yoon) .
Claim 6 is rejected under 35 U.S.C. 103 as being unpatentable over Li, as applied to claim 1 above, and further in view of Masuda et al. (US 20260058192 A1).
Regarding claim 6, Li teaches all limitations of claim 1, as stated above. Li does not teach a limitation wherein a pellet density of the solid electrolyte is about 1.8 g/ml to 2.0 g/ml.
However, Masuda teaches this limitation. Specifically, Masuda teaches sulfide solid electrolytes containing lithium, phosphorus, sulfur, and halogen elements including bromine, and teaches that filling rate (consolidation characteristic) and ion conductivity are affected by pellet density and softness of the electrolyte ([0002, 0008-0009]). Masuda further teaches that a higher relative density (pellet density, with respect to the true density) corresponds to a higher filling rate ([0074]-[0075]), thereby establishing pellet density as a result-effective variable affecting electrolyte consolidation and conductivity ([0002, 0008-0009]).
Masuda further discloses pellet density values within or overlapping the claimed range. For example, Table 1 discloses pellet density values including about 1.81 g/cm3, 1.85 g/cm3, and 1.99 g/cm3 , which are equivalent to claimed g/ml unit. Masuda also teaches measuring pellet density by pressurizing electrolyte powder in a cylindrical jig having a diameter of 10 mm at about 400 MPa ([0144-0146], Fig. 1). Similarly, the instant application teaches determining pellet density by pressing the solid electrolyte in a cylindrical pelletizer under about 3 metric tons (page 9, lines 21-29). Thus, Masuda teaches a comparable pellet-density measurement technique and overlapping density values.
Further, Li and Masuda are considered to be analogous to the claimed invention because both references are directed to solid electrolytes.
Therefore, it would have been obvious before the effective filing date of the claimed invention to optimize the pellet density of Li’s core-shell sulfide solid electrolyte in view of Masuda to achieve suitable filling characteristics and conductivity ([0002, 0008-0009]). Optimizing a result-effective variable to obtain workable or optimum values through routine experimentation is within the level of ordinary skill in the art. See MPEP 2144.05(II); see also In re Aller, 220 F.2d 454 (CCPA 1955).
Claim 7 is rejected under 35 U.S.C. 103 as being unpatentable over Li, as applied to claim 1 above, and further in view of Hiroshi et al. (EP 3419098 A1, citations from enclosed machine translation).
Regarding claim 7, Li teaches all limitations of claim 1, as stated above. Li does not teach a limitation wherein an average particle diameter of the solid electrolyte is about 100 μm to 300 μm.
However, Hiroshi teaches this limitation ([0072]). Specifically, Hiroshi teaches that the average particle diameter of the solid electrolyte preferably 100 μm or less ([0072]). Thus, Hiroshi teaches an overlapping range with the claimed range because the claimed lower limit of about 100 μm overlaps the upper limit disclosed by Hiroshi. It has been held that where the claimed ranges “overlap or lie inside ranges disclosed by the prior art,” a prima facie case of obviousness exists. See MPEP 2144.05(I).
Further, Hiroshi teaches sulfide-based inorganic solid electrolytes including halogen-containing sulfide electrolytes represented by Formula (1) and Formula (2) ([0008]-[0009]), which are analogous to the sulfide solid-state electrolytes of Li. Hiroshi further teaches that controlling particle diameter improves cycle characteristics in all-solid-state secondary batteries ([0007, 0072]).
Further, Li and Hiroshi are considered to be analogous to the claimed invention because both references are directed to sulfide solid electrolytes for all-solid-state batteries and both references teach combining different sulfide solid electrolytes to improve battery performance.
Therefore, it would have been obvious before the effective filing date of the claimed invention to one of ordinary skill in the art to optimize the average particle diameter of the solid electrolyte as taught by Hiroshi in the core-shell sulfide solid electrolyte system of Li in order to improve cycle characteristics ([0007, 0072]).
Claim 8 are rejected under 35 U.S.C. 103 as being unpatentable over Li, as applied to claim 1 above, and further in view of Choi et al. (US 20200052330 A1) and Yu et al. (US 20220131184 A1).
Regarding claim 8, Li teaches all limitations of claim 1, as stated above. Li does not teach a limitation wherein a hydrogen sulfide generation amount of the solid electrolyte is equal to or less than about 100,000 ppm/g when the solid electrolyte comes into contact with air having a moisture content of about 20 wt% at room temperature.
However, Choi teaches hydrogen sulfide generation characteristics of sulfide-based solid electrolytes exposed to atmospheric conditions ([0123, 0140], Fig.6). Specifically, Choi teaches hydrogen sulfide generation analysis for a Li6PS5Cl sulfide solid electrolyte exposed to air at about 20°C and a dew point of about −30°C for 2 hours ([0123, 0140], Comparative Example 1, “SE” in Fig. 6). Fig. 6 shows hydrogen sulfide generation values below approximately 6 ppm/g-SE during the tested exposure period, which is substantially below the claimed upper limit. Choi further teaches that hydrogen sulfide generation deteriorates ion conductivity ([0004, 0145]), thereby teaching hydrogen sulfide generation as a result-effective variable affecting sulfide electrolyte ion conductivity. Although Choi does not teach the claimed moisture percentage.
Yu teaches that atmospheric humidity affects hydrogen sulfide generation in sulfide solid electrolytes ([0019, 0021, 0064, 0067], Figs. 3A-3B and Fig. 5.). Specifically, Yu teaches H2S generation measurements under relative humidity conditions of 10% and 20% at room temperature for sulfide solid electrolytes including Li6PS5Cl and other sulfide electrolytes. Yu shows that increased humidity exposure increases hydrogen sulfide generation ([0019, 0021, 0064, 0067], Figs. 3A-3B and Fig. 5.)
Therefore, it would have been obvious before the effective filing date of claimed invention that one of ordinary skill in the art would optimize the moisture exposure conditions and sulfide electrolyte composition of Li in view of Choi and Yu to achieve a hydrogen sulfide generation amount equal to or less than about 100,000 ppm/g through routine experimentation in order to improve ion conductivity ([0004] of Choi). Optimizing a result-effective variable to obtain workable or optimum values through routine experimentation is within the level of ordinary skill in the art. See MPEP 2144.05(II); see also In re Aller, 220 F.2d 454 (CCPA 1955).
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to Lili Rassouli whose telephone number is (571)272-9760. The examiner can normally be reached Monday-Thursday 8:00 AM-4:00 PM.
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, Matthew T Martin can be reached at (571) 270-7871. 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.
/LILI RASSOULI/ Examiner, Art Unit 1728
/MATTHEW T MARTIN/ Supervisory Patent Examiner, Art Unit 1728
Prosecution Insights