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and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114.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 June 16, 2025 has been entered.
Status of Application
Claims 1, 5, 8-9 and 27 are amended, claims 6, 7, 26, and 28 are canceled, submitted on 5/16/2025 and entered on 6/16/2025 . Claims 21-25 remain withdrawn. Claims 1-2, 5, 8-20, and 27 are presented for examination.
Claim Rejections - 35 USC § 103
1. 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.
2. 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.
3. 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.
4. Claim 1-2, 5, 8, 10-14, 16-20, and 27 are rejected under 35 U.S.C. 103 as being unpatentable over Suzuki (US 20190157723 A1, IDS of 1/20/2022) in view of Kim (US 20140087255 A1).
Regarding claim 1, Suzuki discloses an all-solid secondary battery (Title) comprising: a positive electrode comprising a positive electrode active material layer (cathode, Abstract); a negative electrode (anode, Abstract) comprising a negative electrode current collector (anode current collector, Abstract), and a negative electrode active material layer on the negative electrode current collector (Abstract); and a solid electrolyte layer between the positive electrode active material layer and the negative electrode active material layer (Abstract).
Suzuki discloses the anode material may include at least one of amorphous carbon, gold (Au), platinum (Pt), palladium (Pd), silicon (Si), silver (Ag), aluminum (Al), bismuth (Bi), tin (Sn), or zinc (Zn) ([0015]), the amorphous carbon may be in a form of a particle ([0029]), the anode active material may further include a second particle ([0030]) and the second particle may include silicon, silver, tin, zinc, platinum, or a combination thereof ([0032]). Suzuki further discloses the anode active material in Example 11F to 11L using silver (Ag) particles and furnace black (FB-B) particles ([0184]), which reads on the claimed “wherein the negative electrode active material layer comprises first particles comprising a carbon material, and second particles comprising a metallic material”, because FB-B powder corresponds to the first particle comprising carbon material; and Ag particles corresponds to the second particle comprising a metallic material.
However, while Suzuki discloses the problems of when lithium is used as an anode active material in an all-solid-state battery a lithium dendrite may form, which may cause reduce in capacity, or a short circuit ([0004]) and that as the thickness of the film increases, the anode has an increased resistance, resulting in deterioration of output characteristics ([0161]), and Ag as the second particle as set forth above, Suzuki does not explicitly disclose the metallic material of second particles comprising at least one of copper, titanium, nickel, cobalt, boron, tungsten, iron, or an alloy thereof.
Kim teaches a demand for a composite anode active material having an electrical capacity as high as those metals alloyable with lithium and which is capable of absorbing stress resulting from the volumetric expansion of metal to prevent the deterioration of the composite anode active material ([0007]), and a composite anode material with improved capacity and improved lifetime characteristics ([0008]). Kim teaches a composite anode active material 10 that includes a shell 11 of a hollow carbon fiber, and a core 15 disposed in a hollow of the shell, the core 15 includes a first metal nanostructure 12 and a conducting agent 13 ([0031] and FIG. 1) and the conducting agent in the composite anode active material may be at least one selected from the group consisting of carbon nanostructure and a second metal nanostructure ([0042]). The second metal takes on a role of a conducting agent. In general, the second metal is not alloyable with lithium, may include at least metal selected from the group consisting of silver (Ag), gold (Au), copper (Cu), aluminum (Al), calcium (Ca), tungsten (W), zinc (Zn), nickel (Ni), lithium (Li), iron (Fe), platinum (Pt), and titanium (Ti), but is not limited thereto. Any of a variety of metals that are not alloyable with lithium and available as a conducting agent may be used as the second metal ([0044]). Since Kim listed copper, titanium, nickel, tungsten, or iron as alternative choices of silver (Ag ) without any drastic effect, a skilled artisan would have found it obvious to replace silver particles of Suzuki with at least one of copper, titanium, nickel, tungsten, or iron because those metals are more cost effective.
It would have been obvious for an ordinary skilled artisan before the effective filing date of the claimed invention, to have selected at least one of copper, titanium, nickel, tungsten, or iron by replacing the Ag powder of Suzuki, as taught by Kim, as the conductive metallic powder because those metals are more cost effective, and thus arrive at the claimed “second particles comprising a metallic material comprising at least one of copper, titanium, nickel, tungsten, or iron”.
Modified Suzuki further discloses FB-B particles having an average primary particle diameter D50 of about 38 nm ([0133]), which falls within the range as claimed “wherein an average particle diameter of the first particles is about 10 nanometers to about 1 micrometer”; and silver (Ag) particles having an average particle diameter D50 of 60 nm ([0184]), which falls within the range about 5 nanometers to about 100 nanometers as claimed. A skilled artisan would have found it obvious to control the average particle diameter of the second particle of modified Suzuki, as taught by Suzuki arriving at the claimed “an average particle diameter of the second particles is about 5 nanometers to about 100 nanometers” with a reasonable expectation of success.
Modified Suzuki further discloses that the weight ratio of Ag /FB-B in Example 11I is 1:3 ([0184] and Table 5), which falls within the range of about 1:1 to about 1:20 as claimed.
Modified Suzuki further discloses the solid electrolyte may include, for example, a sulfide-based solid electrolyte material (Suzuki [0107]), which reads on “the solid electrolyte layer comprises a sulfide solid electrolyte.”
As established above, modified Suzuki’s all-solid secondary battery includes the negative electrode active material layer comprises second particles comprising a metallic material comprising at least one of copper, titanium, nickel, tungsten, or iron; and a sulfide solid electrolyte. Further, modified Suzuki discloses manufacturing of all-solid-state secondary battery involves stacking the solid electrolyte layer between the cathode and the anode, followed by pressing with applied pressing pressure may be about 0.5 Mpa to about 10 Mpa ([0119-0120]). This is substantially the same process of manufacturing the all-solid secondary battery with contacting and pressing the negative electrode active material layer and the solid electrolyte layer, the second particles of metallic material and the sulfur of the solid electrolyte layer which may react to generate the third particle as provided in the instant disclosure in Paragraph [0090].
Therefore, a skilled artisan would reasonably expect that with substantially the same composition of metallic second particles and sulfide solid electrolyte, and under substantially the same contacting and pressing manufacturing process, modified Suzuki necessarily and inherently possesses the same feature as claimed “the negative active material layer further comprises third particles comprising a metal sulfide comprising the metallic material of the second particles and the sulfur of the sulfide solid electrolyte”, absent evidence to the contrary for secondary consideration.
Regarding claim 2, modified Suzuki discloses all of the limitations as set forth above. Modified Suzuki further discloses wherein a ratio of an initial charge capacity (b) of the anode active material layer to an initial charge capacity (a) of the cathode active material layer satisfies a condition of Equation 1: 0.01<(b/a)<0.5, wherein a is the initial charge capacity of the cathode active material layer determined from a first open circuit voltage to a maximum charging voltage, and b is the initial charge capacity of the anode active material layer determined from a second open circuit voltage to 0.01 volts vs. Li/Li+ (Abstract), which falls within the claimed limitation.
Regarding claim 5, modified Suzuki discloses all of the limitations as set forth above. Modified Suzuki further discloses that the weight ratio of Ag /FB-B in Example 11I is 1:3 ([0184] and Table 5), which falls with the range of a weight ratio of the metallic material to the carbon material is about 1:1 to about 1:5; an average particle diameter D50 of FB-B is about 38 nm which is considered to meet the claim limitation “an average particle diameter of the first particle is about 40 nanometers to about 100 nanometers” (Examiner-added emphasis), absent a special definition in the instant specification of the term “about” which has been broadly and reasonably interpreted to encompass the scope of how the term is commonly used in the field of endeavor (e.g. 10% tolerance).
Modified Suzuki has rendered obvious using copper in the place of Ag as the second particle metallic material, as set forth above. Modified Suzuki further discloses the average particle diameter of the second particle is about 60 nm (Suzuki [0184]), which falls within the range as claimed “an average particle diameter of the second particle is about 30 nanometers to about 100 nanometers”.
Regarding claim 8, modified Suzuki discloses all of the limitations as set forth above. Since as established above, modified Suzuki includes metal sulfide comprising the metallic material of the secondary particles and the sulfur of the sulfide solid electrolyte, as well as second particles comprising a metallic material comprising at least one of copper, titanium, nickel, tungsten, or iron, a skilled artisan would reasonably expect to have the metal sulfide comprises at least one of copper sulfide, titanium sulfide, cobalt sulfide or nickel sulfide, without undue experimentation and with a reasonable expectation of success.
Regarding claim 10, modified Suzuki discloses all of the limitations as set forth above. Modified Suzuki further discloses the solid electrolyte layer 130 may further include a binder ([0109]).
Regarding claim 11, modified Suzuki discloses all of the limitations as set forth above. Modified Suzuki further discloses wherein the negative active material layer further comprises a lithium-alloying metal (Sn, [0086]) or a lithium-alloying semiconductor material (Si, [0086]).
Regarding claim 12, modified Suzuki discloses all of the limitations as set forth above. Modified Suzuki further discloses the negative electrode active material layer may further include a binder ([0101]).
Regarding claim 13, modified Suzuki discloses all of the limitations as set forth above. Modified Suzuki further discloses the amount of the binder may range from about 0.3 wt% to about 15 wt%, based on a total weight of the anode active material ([0103]).
Regarding claim 14, modified Suzuki discloses all of the limitations as set forth above. Modified Suzuki further discloses the thickness of the anode active material layer may range from about 1 µm to about 20 µm ([0104]).
Regarding claim 16, modified Suzuki discloses all of the limitations as set forth above. Modified Suzuki discloses FB-B powder is carbon black ([0190]).
Regarding claim 17, modified Suzuki discloses all of the limitations as set forth above. Modified Suzuki further discloses at the initial stage or after discharging, lithium may be not present or substantially not present between the anode current collector 310 and the anode active material layer 320 ([0190]), which inherently teaches the claimed “prior to a first charge or when the all-solid secondary battery is in a discharged state, the negative electrode current collector, the negative electrode active material layer, and an area between the negative electrode current collector and the negative electrode active material layer do not comprise lithium metal”, because Li metal is not formed yet and there is no lithium metal in an area between the negative electrode current collector and the negative electrode active material layer during the assembly of the all-solid-state secondary battery. It would have been obvious for an ordinary skilled artisan before the effective filing date of the claimed invention, to arrive at the claim limitation as taught by another embodiment of modified Suzuki.
Regarding claim 18, modified Suzuki discloses all of the limitations as set forth above. Modified Suzuki further discloses during charging, lithium is deposited between the anode current collector 310 and the anode active material layer 320 and a metal layer 330 may be formed by such lithium ([0190]), which reads on the claimed “further comprising, when the all-solid secondary battery is in a charged state, a metal layer comprising lithium metal between the negative electrode current collector and the negative electrode active material layer.” It would have been obvious for an ordinary skilled artisan before the effective filing date of the claimed invention, to arrive at the claim limitation as taught by another embodiment of Suzuki.
Regarding claim 19, modified Suzuki discloses all of the limitations as set forth above. Modified Suzuki further discloses a ratio of initial charge capacity (b) of the anode active material layer 320 to initial charge capacity (a) of the cathode active material layer 520 may satisfy the following condition: 0.01<(b/a)<0.5 ([0190]), which reads on the claimed “wherein the ratio of the initial charge capacity of the negative electrode active material layer to the initial charge capacity of the positive electrode active material layer satisfies Equation 1A:
Equation 1A 0.01<(b/a)<0.5”.
It would have been obvious for an ordinary skilled artisan before the effective filing date of the claimed invention, to arrive at the claim limitation as taught by another embodiment of Suzuki.
Regarding claim 20, modified Suzuki discloses all of the limitations as set forth above. Modified Suzuki further discloses the all-solid-state secondary battery of claim 19, wherein the ratio of the initial charge capacity of the anode active material layer to the initial charge capacity of the cathode active material layer satisfies a condition of Equation 1C:
0.01<(b/a)<0.1 Equation 1C
wherein a and b are as defined in claim 19 (claim 30), which reads on the claimed “the all-solid secondary battery of claim 19, wherein the ratio of the initial charge capacity of the negative electrode active material layer to the initial charge capacity of the positive electrode active material layer satisfies Equation 1B: 0.01<(b/a)<0.1”.
Regarding claim 27, modified Suzuki discloses all of the limitations as set forth above. Since as established above, modified Suzuki has rendered obvious that the metallic material comprises copper among other choices, thus rendering obvious the specific choice of copper for the metallic material as claimed.
5. Claim 9 is rejected under 35 U.S.C. 103 as being unpatentable over Suzuki (US 20190157723 A1, IDS of 1/20/2022) in view of Kim (US 20140087255 A1); as applied to claim 1, further in view of Furukawa (US 20230216043 A1-priority to 5/28/2020).
Regarding claim 9, modified Suzuki discloses all of the limitations as set forth above. While modified Suzuki discloses the problem that as the thickness of the film increases, the anode has an increased resistance, resulting in deterioration of output characteristics ([0161]) and an ion conductive agent as one choice of the additive for the anode active material layer ([0105]), and also rendered obvious of metal sulfide as set forth above in the rejection to claim 1, modified Suzuki does not explicitly disclose a content of the metal sulfide based on a total weight of the negative electrode active material layer.
Furukawa teaches a similar desire to provide a negative electrode for an all-solid-state secondary battery having a low resistance value ([0015]) and the negative-electrode material contains a carbon material as the negative-electrode active material, …, and the negative electrode contains a sulfide-based solid electrolyte as the solid electrolyte ([0016]). Furukawa further teaches it is preferable that the content of the solid electrolyte in the negative-electrode mixture is 4 to 70 mass % ([0043]).
It would have been obvious for a skilled artisan to have controlled the sulfide-based solid electrolyte content being pressed in the negative electrode active material layer of Suzuki to be 4 to 70 mass %, as taught by Furukawa, in order to obtain a negative electrode for an all-solid-state secondary battery having a low resistance value.
Therefore, it would have been further obvious for a skilled artisan to arrive at the claimed “a content of the metal sulfide is about 4 weight percent to about 50 weight percent, based on a total weight of the negative electrode active material layer”, because take for an example, CuS is the metal sulfide formed, and Li2S-P2S5-Li2O-LiI is the sulfide based solid electrolyte chosen from the list of Suzuki (Suzuki [0107]), atomic weight of Cu (63.5 g/mol) is very close to one-sixth of the total weight of the other elements (Li5, P2, O, and I) combined except S (about 53.3 g/mol), which means the weight gain after being converted to CuS won’t be too high; further, in consideration of the fact that only the portion of the sulfide-based solid electrolyte in direct contact with the negative electrode active material under pressing would have a chance to react with Cu, not all of the sulfide-based solid electrolyte (4 to 70 mass %). The foregoing affect the weight change in two directions offsetting the weight percent value change, the former increasing the weight percentage, the latter reducing the weight percentage based on the total weight of the negative electrode active material layer, therefore, a skilled artisan would expect to arrive at a weight percent value of the formed metal sulfide that falls within the claimed range of about 4 weight percent to about 50 weight percent based on a total weight of the negative electrode active material layer, without undue experimentation and with a reasonable expectation of success, in light of various choices regarding the metallic material and sulfide-based solid electrolyte.
6. Claim 15 is rejected under 35 U.S.C. 103 as being unpatentable over Suzuki (US 20190157723 A1, IDS of 1/20/2022) in view of Kim (US 20140087255 A1), as applied to claim 1, further in view of Ose (US 20180301747 A1).
Regarding claim 15, modified Suzuki discloses all of the limitations as set forth above. Modified Suzuki discloses an all-solid-state secondary battery that uses lithium as an anode active material ([0004]) with enhanced energy density, and may inhibit the deposition and growth of a dendrite, inhibit or reduce the likelihood of a short circuit and capacity reduction of the all-solid-state secondary battery and enhance the characteristics of the all-solid-state secondary battery ([0008]). However, modified Suzuki does not explicitly disclose the porosity of the anode active material layer.
Ose teaches a method for producing an all-solid-state lithium ion secondary battery including an anode that is excellent in cycle characteristics ([0006]) by using such an anode mixture that the voidage V of the anode mixture after being dried in the anode mixture forming step is in a specific range, an all-solid-state lithium ion secondary battery being excellent in cycle characteristics compared to the case of using an anode out of the range ([0012]). Ose further teaches to maintain the ion conducting path and the electron conducting path with balance, the voidage V may be 44% or more and 53% or less, or it may be 45% or more and 52% or less ([0058]), which falls within the porosity range of about 30% to about 60% as claimed “wherein porosity of the negative electrode active material layer is about 30 % to about 60 %” because voidage is considered substantially the same as porosity.
It would have been obvious for an ordinary skilled artisan before the effective filing date of the claimed invention, to adjust and control the porosity of the anode active material layer of Suzuki, as taught by Ose, to be at a value that falls within the porosity range as claimed “porosity of the negative electrode active material layer is about 30 % to about 60 %”, in order to maintain the ion conducting path and the electron conducting path with balance and thus achieve excellent cycle characteristics.
Response to Arguments
7. Applicant’s arguments regarding amended claim 1 filed on 5/16/2025 have been fully considered but are not found fully persuasive for the following reasons.
The Applicant first argues that the cited references fail to disclose, teach or suggest the negative active material layer further comprises third particles comprising a metal sulfide comprising the metallic material of the second particles and the sulfur of the sulfide solid electrolyte. (Remarks P9-10).
The Examiner respectfully submits that modified Suzuki’s all-solid secondary battery includes the negative electrode active material layer comprises second particles comprising a metallic material comprising at least one of copper, titanium, nickel, tungsten, or iron; and a sulfide solid electrolyte, which is substantially the same composition combination as provided in the instant disclosure paragraphs [0078] and [0112], and the manufacturing of all-solid-state secondary battery of modified Suzuki involves stacking the solid electrolyte layer between the cathode and the anode, followed by pressing with applied pressing pressure may be about 0.5 Mpa to about 10 Mpa (Suzuki [0119-0120]), which is also substantially the same process as provided in the instant disclosure in Paragraph [0090], quote “In the process of manufacturing the all-solid secondary battery 100, and in the process of contacting and pressing the negative electrode active material layer 122 and the solid electrolyte layer 130, the second particles 1222 of the negative electrode active material layer 122 and the sulfur of the solid electrolyte layer 130 may react to generate the third particle 1223”. A skilled artisan would reasonably expect that with substantially the same composition of metallic second particles and sulfide solid electrolyte, and under substantially the same contacting and pressing manufacturing process, modified Suzuki necessarily and inherently possesses the same feature as claimed “the negative active material layer further comprises third particles comprising a metal sulfide comprising the metallic material of the second particles and the sulfur of the sulfide solid electrolyte”, as evidenced by the instant disclosure in Paragraph [0090], absent evidence to the contrary for secondary consideration. Thus this argument is not found persuasive.
The Applicant further argues by referring to Example 6 vs. Comparative Example 2 (Table 1 and FIG.s 6-7) that using a combination of carbon and copper as a material of a negative active material layer has better average discharge capacity and average coulombic efficiency than using a combination of carbon and silver, and a capacity retention characteristic is also significantly improved. (Remarks P11-12).
The Examiner respectfully submits that Example 6 ([0162]) uses oxide based solid electrolyte (LLZO) rather than sulfide solid electrolyte, thus this argument is not commensurate in scope with the amended claim 1 which requires a sulfide solid electrolyte. This argument is moot.
Conclusion
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/K. L./Examiner, Art Unit 1751 9/29/2025
/JONATHAN G LEONG/Supervisory Patent Examiner, Art Unit 1751 9/29/2025