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 without traverse of Group I, claims 1-13 in the reply filed on 6/22/2026 is acknowledged. Applicant elected Chemical formula 3, and the species gold (Au). Claim 4 is withdrawn from consideration as being drawn to a non-elected invention.
Full consideration was given to claims 1-3, 5-13.
Claims 4, 14-18 are hereby withdrawn.
Priority
Acknowledgement has been made of applicant’s claim for priority under 35 USC 119 (a-d). The certified copy has been filed on 1/9/2025.
Information Disclosure Statement
The Information Disclosure Statement (IDS) filed 11/26/2024, 4/6/2026 has been placed in the application file and the information referred to therein has been considered.
Drawings
The drawings received 11/26/2024 are acceptable for examination purposes.
Claim Rejections - 35 USC § 103
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.
Claims 1, 10-13 are rejected under 35 U.S.C. 103 as being unpatentable over Kim (US 2019/0044186) in view of Zan (CN 117317157).
Regarding claim 1, Kim discloses a solid electrolyte for a lithium secondary battery, comprising: lithium oxide comprising at least one substitution element selected from the group consisting of gallium (Ga), aluminum (Al), tantalum (Ta), and combinations thereof and having a predetermined shape [0078, 0079];
a coating layer comprising a noble metal and located on a surface of the lithium oxide [0118].
Regarding claim 10, the noble metal comprises at least one selected from the group consisting of silver (Ag), gold (Au), platinum (Pt), and combinations thereof [0118].
Regarding claim 1, Kim does not disclose an intermediate layer comprising an alloy of the substitution element and the noble metal and located between the lithium oxide and the coating layer. Zan teaches a positive active material particle comprising a core made of lithium cobaltate and a shell made of a manganese-rich material. There is a transition interface layer between the lithium cobaltate core and the manganese-rich material shell that contains a co-lattice structure formed by co-melting with lithium cobaltate on one side in contact with the lithium cobaltate matrix (page 4 of translation). Because under high temperature calcining, the manganese-rich material shell will generate fusion reaction and element mutual diffusion at the place where it contacts with the lithium cobaltate substrate, so the newly generated transition interface layer is actually the interface layer after the lithium cobaltate substrate and the multi-crystal manganese-rich shell are doped with each other, The chemical formula similar to the matrix and the shell is still maintained. the transition interface layer is provided with a co-lattice structure formed with the lithium cobaltate at one side contacted with the lithium cobaltate, wherein the co-lattice is a continuous space lattice structure kept with the lithium cobaltate. It will be understood that regions of the transition interface layer that are not in direct contact with the lithium cobaltate may also have portions of the non-eutectic lattice. The transition interface layer can eliminate the interface impedance effect between the multi-crystal manganese-rich material shell and the single crystal inner core, which is covered on the surface of the lithium cobaltate inner core as a solid solution layer, and forms a co-crystal lattice structure with the inner core, at the same time, it is firmly connected with the multi-crystal shell layer in the form of chemical bond. The transition interface layer can be formed by independently adding manganese-rich component in the synthesis process, and also can be directly formed in the process of sintering the polycrystalline manganese-rich shell and the lithium cobaltate core at high temperature. The interface layer can ease the bad contact between the compact polycrystalline shell layer and the single crystal lithium cobaltate core and promote the conduction of the lithium ion and the electron (page 9 of translation).
An ordinary artisan would glean from the teaching of Zan that an interface layer is desired when a particle core has a shell with a different composition, for the benefit of easing the stress at the joining interface and hence, promote lithium-ion conduction.
It would have been obvious to one of ordinary skilled in the art at the time the invention was made to form an interface layer between the solid electrolyte and the gold interlayer of Kim, as taught by Zan, for the benefit of forming a strong bond between the solid electrolyte and the gold interlayer.
Regarding claim 11, it is noted that the lithium oxide of Kim is blocked from outside by the intermediate layer, as modified by Zan.
Regarding claim 12, the intermediate layer comprises an alloy of gallium (Ga) and gold (Au), it is noted that the intermediate layer of Kim modified by Zan would include any of the metal ions contained in the core, including gallium.
Regarding claim 13, the intermediate layer has a thickness of 1 nm to 10 nm. Considering that Zan identifies the intermediate layer as a result-effective variable, it would have been obvious to one of ordinary skilled in the art at the time the invention was made to adjust the amount of the intermediate layer, or the thickness, of Kim modified by Zan for the benefit of determining the thickness required for forming a strong bond between the solid electrolyte layer and the interlayer of Kim.
The Examiner notes that forming the intermediate layer too thin would not provide enough to provide a strong bond between the solid electrolyte layer and the interlayer. Forming the intermediate layer too thick would reduce the ion conductivity of the solid electrolyte.
Claims 2, 6-9 are rejected under 35 U.S.C. 103 as being unpatentable over Kim (US 2019/0044186) in view of Zan (CN 117317157) as applied to claim 1, further in view of Huang (Liquid metallic Ga as sintering aid to promote the densification of garnet electrolytes for all-solid-state Li-ion batteries, Journal of Power Sources, 556 (2023) 232527).
Kim modified by Zan does not teach the elements of claims 2, 6-9. Huang teaches a garnet-type LiLaZrTaO (LLZTO) ceramic electrolyte containing gallium (Ga) in between grain boundary by adding gallium in liquid metallic form. See Abstract and Figure 2b. The liquid form gallium filled the gaps between LLZTO particles and densified the structure, which increased its density, for example up to 100%. Page 3. Densified LLZTO electrolytes can provide continuous pathways for ion transportation and smooth surfaces for adequate contact with electrodes (page 6).
Regarding claim 2, the lithium oxide comprises a plurality of grains and a grain boundary between the grains, and a metal derived from the substitution element is precipitated along the grain boundary. See figure 2b.
Regarding claim 6, the lithium oxide is a sintered body, the liquid metal -gallium was added to LLZTO to facilitate sintering (page 3).
Regarding claim 7, the lithium oxide has a relative density of 90% or more (page 3).
Regarding claim 8, the lithium oxide has a surface roughness (Ra) of 1 μm or less, and regarding claim 9, the lithium oxide has a surface roughness (Ra) of 100 nm or less, Huang teaches that a bare LLZTO sheet features abundant pores and a rough surface. In contrast, the LLZTO sheet with 2 wt% Ga presented a smooth surface topography owing to the tightly packed grains (page 6). Figure 6c shows surface roughness of less than 0.1 um.
It would have been obvious to one of ordinary skilled in the art at the time the invention was made to add the gallium of Kim in liquid format, as taught by Huang, for the benefit of forming good contact between the electrolyte and the electrode.
Claims 3, 5 are rejected under 35 U.S.C. 103 as being unpatentable over Kim (US 2019/0044186) in view of Zan (CN 117317157) as applied to claim 1, further in view of Kim (KR 20200029227) and Lin (US 2022/0376255).
Regarding claim 3, the lithium oxide is represented by Chemical Formula 1 LiaAlbGacLa3ZrdTaeO12 and, regarding claim 5, the lithium oxide is represented by Chemical Formula 3 Li7.7-3m-0.534Al0.172GamLa3Zr1.982Ta0.018O12, Kim discloses a solid electrolyte comprising a lithium-lanthanum-zirconium oxide (LLZO-based film) [0070]. In particular, Kim discloses formula 1:
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24
396
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162
423
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Greyscale
But does not disclose the subscripts as claimed by the Applicants.
Kim ‘227 teaches a lithium lanthanum zirconium oxide (LLZO) solid electrolyte doped with aluminum (Al) and gallium (Ga) having an effect of enabling ionic conductivity of the solid electrolyte to be improved by adjusting aluminum, gallium and lithium contents of a starting material and controlling feeding speed of raw material, thereby forming a high precision cubic structure and improving sintering characteristics. See Abstract.
Kim ‘227 teaches the solid electrolyte for the all-solid-state battery has a structure Li6.25Al0.2Ga0.05La3Zr2O12 in Example 1 (see Kim [0124] of the original document), and Li6.25Al0.2Ga0.1La3Zr2O12 in Example 2 (see Kim [0130] of the original document), Li6.25Al0.05Ga0.2La3Zr2O12 in Example 3 (see Kim [0136] of the original document), and Li6.1Al0.1Ga0.2La3Zr2O12 in Example 3 (see Kim [0142] of the original document).
Regarding claim 5, the amount of lithium, gallium, and aluminum, Kim discloses that ionic conductivity is improved by controlling the lithium, gallium, and aluminum content [0010]. It would have been obvious to one of ordinary skilled in the art at the time the invention was made to adjust the amount of lithium, gallium, and aluminum for the benefit of improving ionic conductivity.
Regarding claim 5, Kim modified by Kim ‘227 discloses a solid electrolyte for an all-solid-state battery, which contains Li, La, and Zr and is doped with Al, Ga, and Ta but does not disclose a solid electrolyte for a triple-doped garnet-type battery having Zr in an amount of 1.982 and Ta in an amount of 0.018. Lin teaches a solid electrolyte having high ionic conductivity [0005]. The solid electrolyte comprises a material having the basic formula Li7La3Zr2O12 (LLZO) and derivatives thereof wherein at least one of Al, Ta, or Nb is substituted in Zr sites of the Li7La3Zr2O12 [0014]. Ceramic particles that are AlxLi7-xLa3Zr1.75Ta0.25O12 exhibits improved ionic transport [0038]. Another example is AlxLi7-xLa3Zr2-y-zTayO12, wherein x ranges from 0 to 0.85, y ranges from 0 to 0.50, and z ranges from 0 to 0.75 [0038]. It would have been obvious to one of ordinary skilled in the art at the time the invention was made to partially substitute Zr with Ta of Kim modified by Kim ‘227, as taught by Lin, for the benefit of further improving ionic conductivity of Kim’s solid electrolyte.
Regarding claim 5, Formula I that includes Ta as a dopant with an amount between 0.01 and 0.02, Lin teaches a LLZO with a partial substitution of Zr with Al, Ta, and Nb exhibits improved ionic transport [0038]. Lin clearly teaches that Ta is a result effective variable. It has been held by the courts that discovering an optimum value or workable ranges of a result-effective variable involves only routine skill in the art, and thus not novel. In re Boesch, 617 F.2d 272, 205 USPQ 215 (CCPA 1980). See MPEP 2144.05.
It would have been obvious to one of ordinary skilled in the art at the time the invention was made to add and adjust the substitution amount of Ta to the lithium lanthanum zirconium oxide doped with aluminum and gallium of Kim ‘227, as taught by Lin, for the benefit of further improving ionic conductivity. In the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art” a prima facie case of obviousness exists. In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990). See MPEP 2144.05.
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to CYNTHIA KYUNG SOO WALLS whose telephone number is (571)272-8699. The examiner can normally be reached on M-F until 5pm.
If attempts to reach the examiner by telephone are unsuccessful, the examiner’s supervisor, Jonathan Leong can be reached at 571-270-1292. The fax phone number for the organization where this application or proceeding is assigned is 571-273-8300.
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/CYNTHIA K WALLS/ Primary Examiner, Art Unit 1751
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