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and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114.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 12/22/2025 has been entered.
Response to Remarks
Applicant’s arguments filed on 12/01/2025 have been fully considered but were not found persuasive over the prior art rejection of record for the reasons set forth below. See claims 1–2 and 4–7 rejections below.
Applicant argues that “claim 1 has been amended to recite that “the sulfide solid electrolyte has a D50 of 0.1 µm or more and 50 µm or less in a volume-weighted particle size distribution as determined by a laser diffraction scattering particle size distribution analysis,” and that neither Utsuno nor Wang teaches or suggests the claimed particle size” (see e.g. pages 4-5 of applicant’s argument).
Examiner respectfully disagrees. Newly applied reference, Utsuno I explicitly discloses sulfide solid electrolyte particles having a volume-based average particle size (D50) of 0.1 µm or more and 10 µm or less as measured by laser diffraction particle size distribution measurements (see e.g. paragraph [0034] of Utsuno I). The particle size range disclosed by Utsuno I therefore falls entirely within the broader claimed range of 0.1 µm to 50 µm recited in amended claim 1. When the prior art discloses a value or range that falls within the claimed range, a prima facie case of obviousness exists. See e.g. MPEP 2144.05(I). Accordingly, the limitation regarding the particle size distribution is explicitly taught by Utsuno I and does not distinguish the claimed invention from the prior art. For the above reason, applicant’s argument is not persuasive.
Applicant argues that “Utsuno II produces sulfide solid electrolytes by sintering and does not perform a pulverizing process after sintering, and therefore the sulfide solid electrolyte disclosed by Utsuno II would undergo grain growth and would not have the small particle size recited in claim 1” (see e.g. pages 5-6 of applicant’s argument).
Examiner respectfully disagrees. As discussed above, Utsuno I explicitly discloses sulfide solid electrolyte particles having a D50 particle size of 0.1 µm to 10 µm as measured by laser diffraction particle size distribution measurements (see e.g. paragraph [0034] of Utsuno I). Because the reference expressly teaches particles within the claimed particle size range, applicant’s assertions regarding the processing steps allegedly leading to larger particles are inconsistent with the explicit disclosure of Utsuno I. A reference must be considered for all that it teaches to one of ordinary skill in the art, including its explicit disclosures, and the particle size range disclosed in Utsuno I anticipates or renders obvious the broader particle size range recited in the claim. For the above reason, applicant’s argument is not persuasive.
Applicant argues that :one skilled in the art would not modify Utsuno II to obtain smaller particle sizes because smaller particles would increase grain boundary resistance and reduce ionic conductivity, whereas Utsuno II seeks to improve ionic conductivity” (see e.g. pages 6-7 of applicant’s argument).
Examiner respectfully disagrees. First, as discussed above, Utsuno I already teaches sulfide solid electrolyte particles having a D50 particle size of 0.1 µm to 10 µm, which lies within the claimed range. Therefore, no modification of Utsuno I is required to arrive at the claimed particle size limitation. Second, the rejection relies on Utsuno I for the particle size limitation and relies on Utsuno II only for the sulfur-to-phosphorus molar ratio (S/P). Utsuno II teaches that a sulfide solid electrolyte having an S/P ratio of 3.9 provides high ionic conductivity in argyrodite-type sulfide solid electrolytes (see e.g. Table 1 and paragraph [0019] of Utsuno II). Because Utsuno I and Utsuno II are directed to the same field of halogenated sulfide solid electrolytes and describe closely related compositions and structures, it would have been obvious for a person of ordinary skill in the art to adjust the S/P ratio of the composition of Utsuno I in view of the teachings of Utsuno II in order to obtain a sulfide solid electrolyte having high ionic conductivity. A reference need not recognize the same advantage as the applicant for the combination to be proper, and the motivation to combine arises from the teachings of Utsuno II regarding favorable compositional ratios for improving conductivity in argyrodite-type sulfide electrolytes. For the above reason, applicant’s argument is not persuasive.
Applicant argues that “because the prior art allegedly fails to teach or suggest all elements of claim 1, the combination of the references cannot render the claim obvious” (see e.g. page 6 of applicant’s argument).
Examiner respectfully disagrees. As set forth in the rejection below, Utsuno I discloses a sulfide solid electrolyte comprising Li, P, S, and halogen elements including Cl and Br, having the claimed halogen ratios and a D50 particle size within the claimed range, and including an argyrodite-type crystal structure. Utsuno II discloses a sulfide solid electrolyte composition having an S/P ratio of 3.9, which falls within the claimed range of 3.5 < S/P < 4.1. Because each limitation of claim 1 is taught or suggested by the combination of Utsuno I and Utsuno II, and because the references are directed to the same field of sulfide solid electrolytes for batteries and provide express teachings regarding compositions that achieve high ionic conductivity, the combination renders the subject matter of claim 1 obvious to one of ordinary skill in the art. For the above reason, applicant’s argument is not persuasive.
In conclusion, the arguments and amendments filed were not found to be persuasive over the prior art rejection of record. The rejections of the claims have been updated to reflect the amendments where appropriate. See claims 1–2 and 4–7 rejections below.
Summary
This is a continued examination non-final office action for application 17/792,839 in response to the amendments filed on 12/01/2025. Claims 1-2 and 4-7 are under examination.
The text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
Priority
Acknowledgment is made of applicant’s claim for foreign priority under 35 U.S.C. 119 (a)-(d). The certified copies have been filed in parent Application Nos. JP2020-051637 filed on 03/23/2020 and PCT/JP2021/010345 filed on 03/15/2021.
Information Disclosure Statement
The information disclosure statements (IDS)s submitted on 07/14/2022, 04/18/2024 and 01/03/2025 are being considered by the examiner.
Claim Rejections - 35 USC § 103
Claims 1-2 and 5-7 are rejected under 35 U.S.C. 103 as being unpatentable over Utsuno et al. (US-20200006808-A1), hereinafter, referred to as Utsuno I and further in view of Utsuno et al. (US-20190221884-A1), hereinafter, referred to as Utsuno II.
Regarding Claim 1, Utsuno I discloses a sulfide solid electrolyte (see e.g. "sulfide solid electrolyte" in paragraph [0034]) comprising elemental lithium (Li), elemental phosphorus (P), elemental sulfur (S), and an elemental halogen (X) (see e.g. "the ratio of each element (Li:P:S:Cl:Br) was 5.4:1.0:4.4:1.0:0.6" in paragraph [0244]),
a mole ratio of the elemental halogen (X) to the elemental phosphorus (P), X/P, satisfies X/P = 1.6 (see e.g. "the ratio of each element (Li:P:S:Cl:Br) was 5.4:1.0:4.4:1.0:0.6"; total molar amount of elemental halogen Cl and Br is 1.6 total molar amount of P is 1.0, 1.6/1.0 = 1.6) and
the elemental halogen (X) comprises elemental bromine (Br) and chloride (Cl) (see e.g. "the ratio of each element (Li:P:S:Cl:Br) was 5.4:1.0:4.4:1.0:0.6" in paragraph [0244]),
a ratio of a number of moles of elemental bromine (Br) to a sum of a number of moles of elemental bromine (Br) and a number of moles of elemental chloride (Cl) is 0.375 (see e.g. "the ratio of each element (Li:P:S:Cl:Br) was 5.4:1.0:4.4:1.0:0.6" in paragraph [0244]; the total molar amount of Cl and Br is 1.6 the ratio of Br to the sum of Br and Cl is 0.6/1.6 = 0.375),
the sulfide solid electrolyte has a D50 of 0.1 µm or more and 10 µm or less (see e.g. "The sulfide solid electrolyte particles of one embodiment of the invention contain lithium, phosphorus, and sulfur, and have a volume-based average particle size (D50) of 0.1 μm or more and 10 μm or less as measured by laser diffraction particle size distribution measurements." in paragraph [0034]) in a volume-weighted particle size distribution as determined by a laser diffraction scattering particle size distribution analysis (see e.g. "solid electrolyte sulfide particles containing lithium, phosphorus, and sulfur, having a volume-based average particle size measured by laser diffraction particle size distribution measurement" in paragraph [0016]), and
the sulfide solid electrolyte includes a crystalline phase having an argyrodite-type crystal structure (see e.g. "The crystal structure of the stable phase includes, for example, an argyrodite-type crystal structure" in paragraph [0044]).
Utsuno I discloses points that lie within the ranges claimed by the instant application. In the case where the prior art discloses a point within the claimed range, a prima facie case of obviousness exists. See MPEP 2144.05 (I).
Utsuno I does not disclose that a mole ratio of the elemental sulfur (S) to the elemental phosphorus (P), S/P, satisfies 3.5 < S/P < 4.1.
Utsuno II, however, in the same field of endeavor halogenated sulfide solid electrolytes, discloses a sulfide solid electrolyte comprising elemental lithium (Li), elemental phosphorus (P), elemental sulfur (S), and an elemental halogen (X) see e.g. "A sulfide solid electrolyte containing lithium, phosphorus, sulfur; and one or more of elements X selected from the group consisting of halogen elements" in Abstract of Utsuno II), wherein a mole ratio of the elemental sulfur (S) to the elemental phosphorus (P), S/P, satisfies S/P = 3.9 (see e.g. (S/P) is 3.90 in Example 11 in Molar ratio of each element to phosphorus in Table 1 of Utsuno II).
Utsuno II discloses a point that lies within the range claimed by the instant application. In the case where the prior art discloses a point within the claimed range, a prima facie case of obviousness exists. See MPEP 2144.05 (I).
Utsuno II also teaches that utilizing a sulfide solid electrolyte of this type leads to an argyrodite-type crystal structure in which a high ion conductivity is achieved (see e.g. paragraph [0019] of Utsuno II). Therefore, it would have been obvious to a person of ordinary skill in the art, before the effective filing date of the claimed invention, to modify the sulfide solid electrolyte of Utsuno I et al. such that is has a mole ratio of elemental sulfur (S) to elemental phosphorus (P), S/P, that satisfies S/P = 3.90 as taught by Utsuno II et al. in order to have a sulfide solid electrolyte with high ion conductivity as suggested by Utsuno II.
Regarding Claim 2, Utsuno I in view of Utsuno II disclose the sulfide solid electrolyte according to claim 1 (see e.g. claim 1 rejection above).
Utsuno I in view of Utsuno II does not explicitly disclose that in an X-ray diffraction pattern determined using an X-ray diffractometer (XRD) with CuK-α radiation, a ratio of la to lo, la/lo, is 2.3 or less, where la is a maximum intensity of a diffraction peak A observed at a position of 2θ = 21.3°±0.30, and Io is a background in the X-ray diffraction pattern. However, Utsuno I in view of Utsuno II does disclose a sulfide solid electrolyte composition that has no compositional or structural distinction to the sulfide solid electrolyte composition claimed in the instant application. Because both the prior art and instant application have no compositional or structural difference, the property of having a 2θ peak observed at 21.3°±0.30 is inherent and thus a prima facie case of obviousness exists. See MPEP 2112 (III) and MPEP 2112.01 (I). Regarding Claim 5, Utsuno I in view of Utsuno II discloses an electrode material mixture (see e.g. "electrode mix" in paragraph [0112] of Utsuno I) comprising the sulfide solid electrolyte (see e.g. "includes the sulfide solid electrolyte particles" in paragraph [0112] of Utsuno I) according to claim 1 (see e.g. claim 1 above) and an active material (see e.g. "A negative electrode mix is obtained by incorporating a negative electrode active material to the sulfide solid electrolyte particles" in paragraph [0114] of Utsuno I).
Regarding Claim 6, Utsuno I in view of Utsuno II discloses a solid electrolyte layer comprising the sulfide solid electrolyte (see e.g. "The sulfide solid electrolyte particles of the invention can be used in a solid electrolyte layer" in paragraph [0111] of Utsuno I) according to claim 1 (see e.g. claim 1 rejection above).
Regarding Claim 7, Utsuno I in view of Utsuno II discloses a battery comprising a positive electrode layer (see e.g. "a positive electrode layer" in paragraph [0142] of Utsuno I), a negative electrode layer (see e.g. "a negative electrode layer" in paragraph [0142] of Utsuno I), and a solid electrolyte layer between the positive electrode layer and the negative electrode layer (see e.g. " negative electrode layer, an electrolyte layer, and a positive electrode layer are stacked in this order." in paragraph [0142] and "The electrolyte layer is a layer containing a solid electrolyte or a layer made from a solid electrolyte. The solid electrolyte is not particularly limited, but is preferably a sulfide solid electrolyte particle of the present invention." in paragraph [0147] of Utsuno I), wherein the battery contains the sulfide solid electrolyte according to claim 1 (see e.g. claim 1 rejection above).
Claim 4 is rejected under 35 U.S.C. 103 as being unpatentable over Utsuno et al. (US-20200006808-A1), hereinafter, referred to as Utsuno I, in view of Utsuno et al. (US-20190221884-A1), hereinafter, referred to as Utsuno II, as applied to claim 1 above, and further in view of Wang et al. (A lithium argyrodite Li6PS5Cl0.5Br0.5 electrolyte with improved bulk and interfacial conductivity, 1 February 2019, Journal of Power Sources, Volume 412).
Regarding Claim 4, Utsuno I in view of Utsuno II disclose the sulfide solid electrolyte according to claim 1 (see e.g. claim 1 rejection above).
Utsuno I in view of Utsuno II are both silent as to the crystallite size of the argyrodite-type crystal and thus do not disclose that the argyrodite-type crystal structure has a crystallite size of 60 nm or less.
Wang, however, in the same field of endeavor, sulfide solid electrolytes with an argyrodite crystal structure for use in all-solid-state batteries, discloses a sulfide solid electrolyte with an argyrodite crystal structure that is Li6PS5Cl0.5Br0.5 (see e.g. " Li6PS5Cl0.5Br0.5" in Abstract of Wang). Wang further discloses that the Li6PS5Cl0.5Br0.5 material has a particle size of 20 nm (see e.g. "The particle sizes of Li2S and Li6PS5Cl0.5Br0.5 in the cathode mixture were estimated to be 32 and 20 nm, respectively" in Section 2.3 Electrochemical performance evaluation on page 31 paragraph starting with "Laboratory-scale" of Wang).
Wang discloses a point that lies within the range claimed by the instant application. In the case where the prior art discloses a point within the claimed range, a prima facie case of obviousness exists. See MPEP 2144.05 (I).
Wang discloses an analogous example in the art to the instant application. It would have been obvious to a person of ordinary skill in the art, before the effective filing date of the invention, to apply the teachings of Wang to the sulfide solid electrolyte of Utsuno, as both references are in the same field of endeavor and address similar compositions of sulfide solid electrolytes. Given that Wang explicitly discloses particle sizes as small as 20 nm, which falls within the claimed crystallite size range of 60 nm or less, a person of ordinary skill in the art would have found it obvious to achieve the claimed crystallite size through routine optimization or known processing techniques. Furthermore, when the prior art discloses a range that overlaps with the claimed range, there is a presumption of obviousness unless the applicant can demonstrate that the claimed range yields unexpected results. See MPEP 2144.05(II).
Wang further teaches that this material possesses a higher bulk ionic conductivity and reduced activation energy when compared to single halogen doped argyrodites and hat batteries fabricated with this material show high reversible capacity (see e.g. Abstract of Wang). Therefore, it would have been obvious to a person of ordinary skill in the art, before the effective filing date of the claimed invention, to modify the crystalline phase of the argyrodite-type crystal of Utsuno I et al. in view of Utsuno II et al. such that it has a crystallite size of 20 nm as taught by Wang et al. in order to have a material that possesses a higher bulk ionic conductivity and reduced activation energy as suggested by Wang.
Conclusion
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/J.J.E./Examiner, Art Unit 1723
/TONG GUO/Supervisory Patent Examiner, Art Unit 1723