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and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114.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 05/26/2026 has been entered.
Priority
Receipt is acknowledged of certified copies of papers required by 37 CFR 1.55.
Information Disclosure Statement
The information disclosure statement(s) (IDS) submitted on 03/26/2026 have been considered by the examiner.
Response to Amendment
Applicant notes the following amendments made to the claims:
Claim 1 amended
Claim 5 amended to match amendment to claim 1
Claim 6 cancelled
Response to Arguments
Applicant’s arguments, filed 05/26/2026, with respect to the rejection(s) of claim(s) 1-18 under 35 USC 103 have been fully considered and are persuasive. Specifically, by further amending to specify that both the amorphous carbon black and crystalline carbon black are particles, the previously applied prior art has been overcome. Therefore, the rejection has been withdrawn. However, upon further consideration, a new ground(s) of rejection is made in view of Abdelsalam (US 20150004488 A1), which teaches a combination of amorphous and crystalline carbon particles in an anode layer, with evidentiary support from Matsumoto (US 20160329571 A1), which teaches that the ID/IG of the materials used in Abdelsalam would inherently meet the limitations of claim 1. Dependent claims are rejected in view of Abdelsalam in view of Ku (US 20200136178 A1) as well as the previously applied prior art, as applicant arguments are all related to the previous rejection failing to teach each element of claim 1. In view of the new rejection, there is currently not considered to be any allowable subject matter present in the claims.
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.
Claim 1 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.
A broad range or limitation together with a narrow range or limitation that falls within the broad range or limitation (in the same claim) may be considered indefinite if the resulting claim does not clearly set forth the metes and bounds of the patent protection desired. See MPEP § 2173.05(c). In the present instance, claim 1 recites the broad recitation “a D peak to G peak intensity ratio of the amorphous carbon black, obtained by Raman analysis, is 1.5 or more, a D peak to G peak intensity ratio of the crystalline carbon black, obtained by Raman analysis, is greater than 0.5 and less than 1.5”, and the claim also recites “the D peak/G peak intensity ratio of the amorphous carbon black is 1.6 to 4.0, and the D peak/G peak intensity ratio of the crystalline carbon black is 0.8 to 1.5.” which is the narrower statement of the range/limitation. The claim(s) are considered indefinite because there is a question or doubt as to whether the feature introduced by such narrower language is (a) merely exemplary of the remainder of the claim, and therefore not required, or (b) a required feature of the claims.
Claim Rejections - 35 USC § 102
The text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
Claim(s) 1-3, 11-12 is/are rejected under 35 U.S.C. 102(a)(1) as being anticipated by Abdelsalam (US 20150004488 A1) with evidentiary support from Matsumoto (US 20160329571 A1)
Regarding claim 1, Abdelsalam teaches all of the following elements:
A negative electrode layer for an all-solid secondary battery (“The structure of a rechargeable metal ion battery cell is shown in FIG. 1” Abdelsalam [0061], “The polymer electrolyte material can be a solid polymer electrolyte” Abdelsalam [0064], “A composite anode layer containing active silicon particles 14 overlays the current collector 10” Abdelsalam [0062]. Abdelsalam teaches an anode layer for a secondary battery which may contain a solid electrolyte and thus be an all-solid secondary battery.)
comprising a negative electrode current collector (“The battery cell comprises a current collector for the anode 10, for example copper” Abdelsalam [0062])
and a first negative electrode active material layer containing a carbon-based material, wherein: (composite anode layer 14 contains the active material composition which includes both silicon particles and carbon based materials “In a first aspect, the invention provides a composition comprising at least 50 weight % of a first particulate electroactive material and at least 3-15 weight % of carbon additives comprising elongate carbon nanostructures and carbon black” Abdelsalam [0011])
the carbon-based material includes a mixture of an amorphous carbon black particle and a crystalline carbon black particle, (“The composition may comprise carbon black, which may be characterized as a highly conducting particulate carbon, … The carbon black particles may have dimensions in the range of 10-100 nm and a surface area in excess of 50 m.sup.2/g.” Abdelsalam [0125], “The composition may comprise a single type of carbon black or a blend of one or more types of carbon black.” Abdelsalam [0125], and “Compositions of the following materials in the following weight ratios were prepared… 12 wt % made up of VGCF: multi-wall carbon nanotubes:EC600:Ketjenblack.RTM. EC600-JD:Denka black in the ratio of 4:1:1:2.” Abdelsalam [0163]. In this case, Ketjenblack EC600-JD is the amorphous carbon black, and Denka black is the crystalline carbon black. This is supported in the instant specification “Amorphous carbon such as ketjen black is used when manufacturing the negative electrode layer for an all-solid battery. Amorphous carbon helps lithium ions move smoothly and acts like a buffer, … In addition, when crystalline carbon such as Denka black is used in manufacturing a negative electrode layer, the uniformity and physical properties of an electrode plate are excellent owing to its high crystallinity” Instant spec [0020]. Abdelsalam teaches the use of a mixture of particulate carbon blacks, one of which is amorphous, one of which is crystalline, and both of which anticipate or overlap the claimed D/G ratios via the teachings of Matsumoto, as well as later published literature.)
A D peak to G peak intensity ratio of the amorphous carbon black, obtained by Raman analysis, is 1.5 or more, (Abdelsalam teaches the use of EC600-JD as an amorphous carbon material. Matsumoto table 2 comparative example 31 teaches the use of EC600-JD as having an ID/IG ratio of 1.56, which anticipates the claimed range. “In Comparative Examples 28 to 34, a commercially available product of a carbon support material (made by Lion Corporation, product name EC600JD) was used and treated by third heat treatment at the treatment temperatures shown in Table 2 to obtain the carbon support materials of Comparative Examples 28 to 34.” Matsumoto [0066]. This would be an inherent property of the material, and thus would not require an obviousness combination/rejection)
a D peak to G peak intensity ratio of the crystalline carbon black, obtained by Raman analysis, is greater than 0.5 and less than 1.5, (Matsumoto table 2 comparative example 35 teaches Denka black as having an ID/IG ratio of 1.11, which anticipates the claimed range. “In the case of Comparative Example 35 where the commercially available product of Denka Black FX-35 was used” Matsumoto [0073]. This would be an inherent property of the material and thus would not require an obviousness combination/rejection.)
the D peak/G peak intensity ratio of the amorphous carbon black is 1.6 to 4.0, (Abdelsalam teaches the use of EC600-JD as an amorphous carbon material. Matsumoto table 2 comparative example 28 teaches the use of EC600-JD as having an ID/IG ratio of 1.68, which anticipates the claimed range. “In Comparative Examples 28 to 34, a commercially available product of a carbon support material (made by Lion Corporation, product name EC600JD) was used and treated by third heat treatment at the treatment temperatures shown in Table 2 to obtain the carbon support materials of Comparative Examples 28 to 34.” Matsumoto [0066]. This would be an inherent property of the material and thus would not require an obviousness combination/rejection.)
and the D peak/G peak intensity ratio of the crystalline carbon black is 0.8 to 1.5. (Matsumoto table 2 comparative example 35 teaches Denka black as having an ID/IG ratio of 1.11, which anticipates the claimed range. “In the case of Comparative Example 35 where the commercially available product of Denka Black FX-35 was used” Matsumoto [0073]. This would be an inherent property of the material and thus would not require an obviousness combination/rejection.)
Regarding claim 2, Abdelsalam teaches all of the following elements:
The negative electrode layer of claim 1, wherein a mixed weight ratio of the amorphous carbon black and the crystalline carbon black is 1:0.05 to 1:2.5. (“Compositions of the following materials in the following weight ratios were prepared… 12 wt % made up of VGCF: multi-wall carbon nanotubes:EC600: Ketjenblack.RTM. EC600-JD: Denka black in the ratio of 4:1:1:2.” Abdelsalam [0163].” In this example, there is a 1:2 ratio of amorphous carbon black [ketjen black] to crystalline carbon black [Denka black], which anticipates the claimed range.)
Regarding claim 3, Abdelsalam teaches all of the following elements:
The negative electrode layer of claim 1, wherein the first negative electrode active material layer further includes a metal, a metalloid, or a combination thereof, and the metal, metalloid, or combination thereof includes silver, platinum, zinc, silicon, tin, iron, copper, aluminum, indium, bismuth, or a combination thereof. (“Compositions of the following materials in the following weight ratios were prepared… 12 wt % made up of VGCF: multi-wall carbon nanotubes:EC600: Ketjenblack.RTM. EC600-JD: Denka black in the ratio of 4:1:1:2.” Abdelsalam [0163].” The anode layer of Abdelsalam further includes silicon, meeting the limitations of claim 3.)
Regarding claim 11, Abdelsalam teaches all of the following elements:
The negative electrode layer of claim 1, wherein: the first negative electrode active material layer includes a binder, (“The binder may be provided to provide cohesion of the particles and, in the case of use in a metal ion battery, for adhesion of the composition to an anode current collector.” Abdelsalam [0137])
and the binder is styrene butadiene rubber, polytetrafluoroethylene, polyvinylidene fluoride, polyethylene, carboxymethylcellulose, or a combination thereof. (“The binder material may be a polymeric material, for example polyimide, polyacrylic acid (PAA) and alkali metal salts thereof, polyvinylalchol (PVA), polyvinylidene fluoride (PVDF) and sodium carboxymethylcellulose (Na-CMC) or rubber-based binders such as SBR. Mixtures of different binder materials may be used.” Abdelsalam [0138])
Regarding claim 12, Abdelsalam teaches all of the following elements:
An all-solid secondary battery comprising: a positive electrode layer; a negative electrode layer; and a solid electrolyte layer disposed between the positive electrode layer and the negative electrode layer, (A liquid electrolyte may be provided between the anode and the cathode. In the example of FIG. 1, a porous plastic spacer or separator 20 is provided between the anode layer 14 and the lithium containing cathode layer 16, … The porous plastic spacer or separator 20 may be replaced by a polymer electrolyte material and in such cases the polymer electrolyte material is present within both the composite anode layer 14 and the composite cathode layer 16. The polymer electrolyte material can be a solid polymer electrolyte” Abdelsalam [0064]. In this case, if the liquid electrolyte is substituted with a solid polymer electrolyte, there would be a solid electrolyte layer disposed between an anode and a cathode.)
wherein the negative electrode layer is the negative electrode layer as claimed in claim 1. (See above for how all of the limitations of claim 1 are met.)
Claim Rejections - 35 USC § 103
The text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
Claim(s) 4, 7-10, 13-18 is/are rejected under 35 U.S.C. 103 as being unpatentable over Abdelsalam (US 20150004488 A1) with evidentiary support from Teixeira et al (2026) and Ishida et al (2020) in view of Ku (US 20200136178 A1).
Regarding claim 4, Abdelsalam is silent on the following elements. Specifically, Abdelsalam teaches a negative electrode layer which includes 50% silicon and 45% carbon-based material. (“In a first aspect, the invention provides a composition comprising at least 50 weight % of a first particulate electroactive material” Abdelsalam [0011] “Optionally, the at least first and second elongate carbon nanostructure materials are provided in a total amount in the range of 0.1-15 weight % of the composition.” Abdelsalam [0024], “Optionally, the graphite is provided in the composition in an amount of 1-30 wt %,” Abdelsalam [0027] and “Optionally, the carbon black is provided in an amount of at least 0.5 weight % of the composition, and optionally less than 10 wt % of the composition” Abdelsalam [0030])
The negative electrode layer of claim 3, wherein the content of the metal, metalloid, or combination thereof is, based on 100 parts by weight of the total weight of the first negative electrode active material layer, 1 to 40 wt % and the content of the carbon-based material is 60 wt% to 99 wt %.
However, Ku teaches all of the elements of claim 4 not found in Abdelsalam:
The negative electrode layer of claim 3, wherein the content of the metal, metalloid, or combination thereof is, based on 100 parts by weight of the total weight of the first negative electrode active material layer, 1 to 40 wt % and the content of the carbon-based material is 60 wt% to 99 wt %. (“The anode active material included in the first anode active material layer 22 includes, for example, a mixture of first particles including amorphous carbons and second particles including metals or metalloids. The metal or metalloid includes, for example, … silicon (Si), … The amount of the second particles is about 8 weight percent (wt %) to about 60 wt %, about 10 wt % to about 50 wt %, about 15 wt % to about 40 wt %, or about 20 wt % to about 30 wt % with respect to the total weight of the mixture.” Ku [0044] and “Mixed powder obtained by mixing the furnace black (FB-C) and the silver particles at a weight ratio of 3:1 was used in an anode. 4 grams (g) of the mixed powder was put in a container and 4 g of an NMP solution containing 5 wt % of a PVDF binder” Ku [0083]. Assuming the NMP solution dissolves, the final active material would include .2g binder, 3g furnace black, and 1g of metal material., this would be 71% carbon material, 23.8% metal, and 4.7% binder, which would anticipate the claimed ranges.)
Ku and Abdelsalam are considered to be analogous because they are both within the same field of lithium secondary batteries that teach a mixture of a carbon black material and a silicon material for use in an anode layer. Therefore, it would have been obvious to one of ordinary skill before the effective filing date of the claimed invention to modify the teachings of Abdelsalam to include a higher weight ratio of the carbon-based material in order to improve cycle characteristics of the battery (“The metalloid is alternatively a semiconductor. The amount of the second particles is about 8 weight percent (wt %) to about 60 wt %, about 10 wt % to about 50 wt %, about 15 wt % to about 40 wt %, or about 20 wt % to about 30 wt % with respect to the total weight of the mixture. The amount of the second particles is in such a range, and as a result, the cycle characteristics of the all-solid secondary battery 1 are further improved.” Ku [0044])
It would additionally be obvious to modify the teachings of Abdelsalam with those of Ku that teach the inclusion of a second anode active material layer, specifically, a metal layer that is placed in between the current collector and the first anode active material layer, which is used as a lithium reservoir. This would have been obvious because the usage of a lithium reservoir improves characteristics in solid-electrolyte lithium-ion secondary batteries and this was known in the art prior to the effective filing date of the instant invention (“When the second anode active material layer 23 is placed between the anode current collector 21 and the first anode active material layer 22 before assembling the all-solid secondary battery 1, the second anode active material layer 23 is a metal layer including lithium to serve as a lithium reservoir. The cycle characteristics of the all-solid secondary battery 1 including the second anode active material layer 23 are further improved.” Ku [0054]).
By modifying Abdelsalam to include the second anode active layer of Ku, which comprises a metal layer, and a thin film layer, which includes a lithium-alloyable metal, the additional limitations of claims 7-10, 13, 15 would all be met without requiring further modification or motivation.
It would additionally have been obvious prior to the filing date of the instant invention to modify the teachings of Abdelsalam with those of Ku to teach the inclusion of a lithium-free region in order to suppress the short circuit and capacity decrease of the all-solid secondary battery (“Accordingly, it is possible to suppress the short circuit and the capacity decrease of the all-solid secondary battery 1, thereby improving the cycle characteristics of the all-solid secondary battery 1. Further, when the second anode active material layer 23 is placed by charging after assembling the all-solid secondary battery 1, the anode current collector 21, the first anode active material layer 22, and an area therebetween are, for example, Li-free areas not including lithium (Li) in an initial state or a state after discharging of the all-solid secondary battery.” Ku [0055])
By modifying Abdelsalam to include the Li-free region as taught by Ku, the additional limitations of claim 14 would be met without requiring any further modification or motivation.
It would additionally be obvious to modify the teachings of Abdelsalam to substitute the solid polymer electrolyte of Abdelsalam with the sulfide-based solid electrolyte of Ku, as this would only require the simple substitution of one solid electrolyte material for a lithium-ion secondary battery for another, and the simple substitution of one known element for another is likely to be obvious when predictable results are achieved. (see MPEP § 2143, B.).
By modifying the teachings of Abdelsalam with those of Ku teaching the usage of a sulfide solid electrolyte, the additional limitations of claims 16-18 would all be met without requiring any further modification or motivation.
Regarding claim 7, Abdelsalam teaches all of the elements of claim 1, as shown above. Abdelsalam is silent on the following elements of claim 7:
The negative electrode layer of claim 1, further comprising a lithium metal or lithium alloy thin film between the negative electrode current collector and the first negative electrode active material layer.
However, Ku teaches all of the elements of claim 7 that are not found in Abdelsalam:
The negative electrode layer of claim 1, further comprising a lithium metal or lithium alloy thin film between the negative electrode current collector and the first negative electrode active material layer. (“the all-solid secondary battery 1 further includes, for example, a second anode active material layer 23 between the anode current collector 21 and the first anode active material layer 22 … The second anode active material layer 23 is a metal layer including lithium or a lithium alloy.” Ku [0051]. The lithium metal or lithium alloy layer is considered to be a thin film, in addition to the thin film layer of Ku which includes a lithium alloyable metal, used in claims 8 and 9.)
Regarding claim 8, Abdelsalam teaches all of the elements of claim 1, as shown above. Abdelsalam is silent on the following elements of claim 8:
The negative electrode layer of claim 1, further comprising a metal or metalloid thin film between the negative electrode current collector and the first negative electrode active material layer.
However, Ku teaches all of the elements of claim 8 that are not found in Abdelsalam:
The negative electrode layer of claim 1, further comprising a metal or metalloid thin film between the negative electrode current collector and the first negative electrode active material layer. (“the all-solid secondary battery 1 further includes, for example, a thin film 24 including elements capable of forming an alloy with lithium on the anode current collector 21. The thin film 24 is placed between the anode current collector 21 and the first anode active material layer 22. The thin film 24 includes, for example, an element capable of forming an alloy with lithium.” Ku [0049])
Regarding claim 9, Abdelsalam teaches all of the elements of claim 8, as shown above. Abdelsalam is silent on the following elements of claim 9:
The negative electrode layer of claim 8, wherein the metal or metalloid thin film includes gold (Au), silver (Ag), magnesium (Mg), zinc (Zn), silicon (Si), tin (Sn), platinum (Pt), palladium (Pd), aluminum (Al), bismuth (Bi), or a combination thereof, and the metal or metalloid thin film has a thickness of 1 nm to 800 nm.
However, Ku teaches all of the elements of claim 9 that are not found in Abdelsalam:
The negative electrode layer of claim 8, wherein the metal or metalloid thin film includes gold (Au), silver (Ag), magnesium (Mg), zinc (Zn), silicon (Si), tin (Sn), platinum (Pt), palladium (Pd), aluminum (Al), bismuth (Bi), or a combination thereof, and the metal or metalloid thin film has a thickness of 1 nm to 800 nm. (“the all-solid secondary battery 1 further includes, for example, a thin film 24 including elements capable of forming an alloy with lithium on the anode current collector 21. The thin film 24 is placed between the anode current collector 21 and the first anode active material layer 22. The thin film 24 includes, for example, an element capable of forming an alloy with lithium.” Ku [0049] and “Examples of the element capable of forming the alloy with lithium include gold, silver, zinc, tin, indium, silicon, aluminum, bismuth and the like,” Ku [0049] and “A thickness d24 of the thin film is, for example, about 1 nm to about 800 nm, about 10 nm to about 700 nm, about 50 nm to about 600 nm, or about 100 nm to about 500 nm.” Ku [0050]. This anticipates the claimed range for the thickness of the metal or metalloid thin film.)
Regarding claim 10, Abdelsalam teaches all of the elements of claim 1, as shown above. Abdelsalam is silent on the following elements of claim 10:
The negative electrode layer of claim 1, further comprising a second negative electrode active material layer, wherein the second negative electrode active material layer includes a metal, a metalloid element, or a combination thereof capable of forming an alloy with lithium, and is a metal layer including lithium or a lithium alloy.
However, Ku teaches all of the elements of claim 10 that are not found in Abdelsalam:
The negative electrode layer of claim 1, further comprising a second negative electrode active material layer, wherein the second negative electrode active material layer includes a metal, a metalloid element, or a combination thereof capable of forming an alloy with lithium, and is a metal layer including lithium or a lithium alloy. (“the all-solid secondary battery 1 further includes, for example, a second anode active material layer 23 between the anode current collector 21 and the first anode active material layer 22 … The second anode active material layer 23 is a metal layer including lithium or a lithium alloy.” Ku [0051])
Regarding claim 13, Abdelsalam teaches all of the elements of claim 12, as shown above. Abdelsalam teaches the following elements of claim 13:
The all-solid secondary battery of claim 12, wherein the negative electrode layer includes a negative electrode current collector and a first negative electrode active material layer, (“The battery cell comprises a current collector for the anode 10, for example copper” Abdelsalam [0062] and “A composite anode layer containing active silicon particles 14 overlays the current collector 10” Abdelsalam [0062].)
Abdelsalam is silent on the following elements of claim 13:
The all-solid secondary battery of claim 12, wherein the negative electrode layer includes a negative electrode current collector and a first negative electrode active material layer, a second negative electrode active material is disposed on at least one of the first negative electrode active material layer and between the negative electrode current collector and the first negative electrode active material layer, and the second negative electrode active material layer includes lithium or a lithium alloy.
However, Ku teaches all of the elements of claim 10 that are not found in Abdelsalam:
The all-solid secondary battery of claim 12, wherein the negative electrode layer includes a negative electrode current collector and a first negative electrode active material layer, a second negative electrode active material is disposed on at least one of the first negative electrode active material layer and between the negative electrode current collector and the first negative electrode active material layer, and the second negative electrode active material layer includes lithium or a lithium alloy. (“the all-solid secondary battery 1 further includes, for example, a second anode active material layer 23 between the anode current collector 21 and the first anode active material layer 22 … The second anode active material layer 23 is a metal layer including lithium or a lithium alloy.” Ku [0051])
Regarding claim 14, Abdelsalam teaches all of the elements of claim 12, as shown above. Abdelsalam teaches the following elements of claim 14:
The all-solid secondary battery of claim 12, wherein the negative electrode layer includes a negative electrode current collector and a first negative electrode active material layer, (“The battery cell comprises a current collector for the anode 10, for example copper” Abdelsalam [0062] and “A composite anode layer containing active silicon particles 14 overlays the current collector 10” Abdelsalam [0062].)
Abdelsalam is silent on the following elements of claim 14:
and the negative electrode current collector, the first negative electrode active material layer, and a region therebetween are lithium (Li)-free regions that do not include Li at an initial state or post-discharge state of the all-solid secondary battery.
However, Ku teaches all of the elements of claim 14 not found in Abdelsalam:
and the negative electrode current collector, the first negative electrode active material layer, and a region therebetween are lithium (Li)-free regions that do not include Li at an initial state or post-discharge state of the all-solid secondary battery. (“Accordingly, it is possible to suppress the short circuit and the capacity decrease of the all-solid secondary battery 1, thereby improving the cycle characteristics of the all-solid secondary battery 1. Further, when the second anode active material layer 23 is placed by charging after assembling the all-solid secondary battery 1, the anode current collector 21, the first anode active material layer 22, and an area therebetween are, for example, Li-free areas not including lithium (Li) in an initial state or a state after discharging of the all-solid secondary battery.” Ku [0055])
Regarding claim 15, Abdelsalam teaches all of the elements of claim 12, as shown above. Abdelsalam is silent on the following elements of claim 15:
The all-solid secondary battery of claim 12, wherein a lithium precipitation layer is included between the negative electrode current collector and the negative electrode active material during charging or after charging.
However, Ku teaches all of the elements of claim 15 not found in Abdelsalam. Specifically, by including the thin film layer and second anode active layer of Ku, there is inherently a lithium precipitation layer present:
The all-solid secondary battery of claim 12, wherein a lithium precipitation layer is included between the negative electrode current collector and the negative electrode active material during charging or after charging. (“The thin film 24 is placed on the anode current collector 21 to further planarize a precipitation form of, for example, a second anode active material layer (not shown) precipitated between the thin film 24 and the first anode active material layer 22 and further improve the cycle characteristics of the all-solid secondary battery 1.” Ku [0049] and “In the all-solid secondary battery 1, the second anode active material layer 23 may be placed between the anode current collector 21 and the first anode active material layer 22 before assembling the all-solid secondary battery 1 or precipitated between the anode current collector 21 and the first anode active material layer 22 by charging after assembling the all-solid secondary battery 1.” Ku [0053] Ku teaches that the second anode layer may be formed via the precipitation of lithium, thus making it a lithium precipitation layer.)
Regarding claim 16, Abdelsalam teaches all of the elements of claim 12, as shown above. Abdelsalam is silent on the following elements of claim 16:
The all-solid secondary battery of claim 12, wherein the solid electrolyte layer includes a sulfide-based solid electrolyte.
However, Ku teaches all of the elements of claim 16 not found in Abdelsalam:
The all-solid secondary battery of claim 12, wherein the solid electrolyte layer includes a sulfide-based solid electrolyte. (“The solid electrolyte layer may include, for example, a sulfide-based solid electrolyte.” Ku [0057])
Regarding claim 17, modified Abdelsalam teaches all of the elements of claim 16, as shown above. Abdelsalam is silent on the following elements of claim 17:
The all-solid secondary battery of claim 16, wherein the sulfide-based solid electrolyte is one or more selected from Li2S-P2S5, Li2S-P2S5-LiX (where X is a halogen element), Li2S-P2S5-Li2O, Li2S-P2S5-Li2O-LiI, Li2S-SiS2, Li2S-SiS2-LiI, Li2S-SiS2-LiBr, Li2S-SiS2-LiCl, Li2S-SiS2-B2S3-LiI, Li2S-SiS2-P2S5-LiI, Li2S-B2S3, Li2S- P2S5-ZmSn (where m and n are positive numbers, and Z is one of Ge, Zn and Ga), Li2S-GeS2, Li2S-SiS2-Li3PO4, Li2S-SiS2-LipMOq (where p and q are positive numbers, and M is one of P, Si, Ge, B, Al, Ga, and In), Li7-xPS6-xClx (where Ox<2), Li7-xPS6-xBrx (where Ox<2), and Li7-xPS6-xIx (where Ox<2).
However, Ku teaches all of the elements of claim 17 not found in Abdelsalam:
The all-solid secondary battery of claim 16, wherein the sulfide-based solid electrolyte is one or more selected from Li2S-P2S5, Li2S-P2S5-LiX (where X is a halogen element), Li2S-P2S5-Li2O, Li2S-P2S5-Li2O-LiI, Li2S-SiS2, Li2S-SiS2-LiI, Li2S-SiS2-LiBr, Li2S-SiS2-LiCl, Li2S-SiS2-B2S3-LiI, Li2S-SiS2-P2S5-LiI, Li2S-B2S3, Li2S- P2S5-ZmSn (where m and n are positive numbers, and Z is one of Ge, Zn and Ga), Li2S-GeS2, Li2S-SiS2-Li3PO4, Li2S-SiS2-LipMOq (where p and q are positive numbers, and M is one of P, Si, Ge, B, Al, Ga, and In), Li7-xPS6-xClx (where Ox<2), Li7-xPS6-xBrx (where Ox<2), and Li7-xPS6-xIx (where Ox<2). (“The sulfide-based solid electrolyte is at least one of, for example, Li.sub.2S—P.sub.2S.sub.5, Li.sub.2S—P.sub.2S.sub.5—LiX wherein X is a halogen element, Li.sub.2S—P.sub.2S.sub.5—Li.sub.2O, Li.sub.2S—P.sub.2S.sub.5—Li.sub.2O—LiI, Li.sub.2S—SiS.sub.2, Li.sub.2S—SiS.sub.2—LiI, Li.sub.2S—SiS.sub.2—LiBr, Li.sub.2S—SiS.sub.2—LiCl, Li.sub.2S—SiS.sub.2—B.sub.2S.sub.3—LiI, Li.sub.2S—SiS.sub.2—P.sub.2S.sub.5—LiI, Li.sub.2S—B.sub.2S.sub.3, Li.sub.2S—P.sub.2S.sub.5-ZmSn wherein m and n are positive numbers, Z is one of Ge, Zn or Ga, Li.sub.2S—GeS.sub.2, Li.sub.2S—SiS.sub.2—Li.sub.3PO.sub.4, Li.sub.2S—SiS.sub.2-Li.sub.pMO.sub.q wherein p and q are positive numbers, M is one of P, Si, Ge, B, Al, Ga In, Li.sub.7-xPS.sub.6-xCl.sub.x wherein 0≤x≤2, Li.sub.7-xPS.sub.6-xBr.sub.x wherein 0≤x≤2, and Li.sub.7-xPS.sub.6-xI.sub.x wherein 0≤x≤2.” Ku [0057])
Regarding claim 18, modified Abdelsalam teaches all of the elements of claim 16, as shown above. Abdelsalam is silent on the following elements of claim 18:
The all-solid secondary battery of claim 12, wherein the sulfide-based solid electrolyte is an argyrodite-type solid electrolyte including Li6PS5Cl,Li6PS5Br, or Li6PS5I.
However, Ku teaches all of the elements of claim 18 not found in Abdelsalam:
The all-solid secondary battery of claim 12, wherein the sulfide-based solid electrolyte is an argyrodite-type solid electrolyte including Li6PS5Cl,Li6PS5Br, or Li6PS5I. (“The sulfide-based solid electrolyte included in the solid electrolyte layer may be an argyrodite-type compound including at least one of Li.sub.7-xPS.sub.6-xCl.sub.x wherein 0≤x≤2, Li.sub.7-xPS.sub.6-xBr.sub.x wherein 0≤x≤2, and Li.sub.7-xPS.sub.6-xI.sub.x wherein 0≤x≤2.” Ku [0059])
Claim(s) 5 is/are rejected under 35 U.S.C. 103 as being unpatentable over Abdelsalam (US 20150004488 A1) with evidentiary support from Teixeira et al (2026) and Ishida et al (2020) in view of Ku (US 20200136178 A1), and further in view of Masakazu (JP 2007227368A) and Spahr (US 20180155552 A1).
Regarding claim 5, Abdelsalam teaches the following elements:
The negative electrode layer of claim 1, wherein:
the amorphous carbon black particle has a primary particle size of 15 nm to 60 nm, (“The carbon black particles may have dimensions in the range of 10-100 nm and a surface area in excess of 50 m.sup.2/g.” Abdelsalam [0125])
a specific surface area of 15 m2/g to 1500 m2/g, (“The carbon black particles may have dimensions in the range of 10-100 nm and a surface area in excess of 50 m.sup.2/g.” Abdelsalam [0125])
and the crystalline carbon black particle has a primary particle size of 15 nm to 60 nm, (“The carbon black particles may have dimensions in the range of 10-100 nm and a surface area in excess of 50 m.sup.2/g.” Abdelsalam [0125])
a specific surface area of 15 m2/g to 500 m2/g, (“The carbon black particles may have dimensions in the range of 10-100 nm and a surface area in excess of 50 m.sup.2/g.” Abdelsalam [0125])
The examiner takes note of the fact that the prior art ranges of ------10-100nm and 50m2/g or more for the particle size and surface area of the carbon black(s), both crystalline and amorphous, of Abdelsalam overlap the claimed ranges of 15-60nm and 15-1500 m2/g (or 15-500 m2/g in the case of crystalline) for the same parameters. Absent any additional and more specific information in the prior art, a prima facie case of obviousness exists. In re Peterson, 315 F.3d 1325, 1330, 65 USPQ2d 1379 (Fed. Cir. 2003). MPEP 2144.05.
Abdelsalam is silent on the following elements:
The amorphous carbon black particle has a crystallite size Lc in the c-axis direction of 3.0 nm or less, and a carbon interlayer spacing (d002) of 0.350 nm to 0.370 nm,
and the crystalline carbon black particle has a crystallite size Lc in the c-axis direction of 2.0 nm to 10.0 nm, and a carbon interlayer spacing (d002) of 0.335 nm to 0.357 nm.
Spahr teaches the following elements of claim 5 not found in Abdelsalam:
wherein the amorphous carbon black has a crystallite size Lc in the c-axis direction of 3.0 nm or less, (Spahr Table 2 shows that each of the carbon blacks used have a crystalline size of 2nm, which anticipates the claimed range)
and a carbon interlayer spacing (d002) of 0.350 nm to 0.370 nm, (“Alternatively or in addition, the carbon black material may be characterized by an interlayer spacing c/2 of between about 0.3580 and about 0.3640 nm. In certain embodiments, the interlayer spacing c/2 will be between about 0.3590 and about 0.3630 nm, or between about 0.3600 and about 0.36200 nm, or between about 0.3600 and about 0.3615 nm.” Spahr [0040] This anticipates the claimed range.)
Spahr is silent on the following elements of claim 5:
and the crystalline carbon black particle has a crystallite size Lc in the c-axis direction of 2.0 nm to 10.0 nm, and a carbon interlayer spacing (d002) of 0.335 nm to 0.357 nm.
Masakazu teaches the following elements of claim 5 that are not found in Abdelsalam or Spahr:
wherein the crystalline carbon black has a crystallite size Lc in the c-axis direction of 2.0 nm to 10.0 nm, (Further, the crystallite size (Lc) of the amorphous carbonaceous (002) plane obtained by X-ray diffraction by the Gakushin method is essential to be 80 nm or less, preferably 35 nm or less. Preferably it is 20 nm or less, more preferably, it is 10 nm or less.” Masakazu [62])
The examiner takes note of the fact that the prior art range of less than 10nm for the crystallite size of crystalline carbon black encompasses the claimed range of between 2 and 10nm for the same parameter. Absent any additional and more specific information in the prior art, a prima facie case of obviousness exists. In re Peterson, 315 F.3d 1325, 1330, 65 USPQ2d 1379 (Fed. Cir. 2003). MPEP 2144.05.
and a carbon interlayer spacing (d002) of 0.335 nm to 0.357 nm. (“The spacing (d002) of the (002) plane of the amorphous carbonaceous material used as the negative electrode active material of the lithium-ion secondary battery of the present invention by the wide-angle X-ray diffraction method is Although it is essential that it is 0.337 nm or more, it is preferably 0.34 nm or more. As an upper limit, it is 0.39 nm or less normally, “ Masakazu [60]. This anticipates the claimed range.)
The use of the specific crystallite size and interlayer spacing of the crystalline and amorphous carbon blacks as taught by Masakazu and Spahr, respectively, would be obvious for the following reasons:
Regarding the crystalline carbon black, Masakazu is considered to be analogous to Abdelsalam because it is within the same field of lithium-ion secondary batteries. Therefore, it would have been obvious to one of ordinary skill before the effective filing date of the claimed invention to modify the crystalline carbon black of Abdelsalam to have the specific crystallite size and interlayer spacing parameters of Masakazu in order to have crystalline particles with high conductivity without sacrificing current density and charge/discharge characteristics (“Although it is essential that it is 0.337 nm or more, it is preferably 0.34 nm or more. As an upper limit, it is 0.39 nm or less normally, preferably it is 0.38 nm or less, more preferably, it is 0.37 nm or less, more preferably, it is 0.36 or less, most preferably, it is 0.35 or less. If it exceeds this range, the crystallinity is remarkably lowered, the decrease in conductivity between particles cannot be ignored, and it may be difficult to obtain the effect of improving the high current density charge / discharge characteristics for a short time. On the other hand, below this range, the crystallinity becomes too high, and it may be difficult to obtain the effect of improving the high current density charge / discharge characteristics for a short time.” Masakazu [60])
Regarding the amorphous carbon black, Spahr is considered to be analogous to Abdelsalam because it is related to modifying carbon black to optimize properties in the context of lithium-ion batteries. Therefore, it would have been obvious to one of ordinary skill before the effective filing date of the claimed invention to modify the amorphous carbon black of Abdelsalam to have the specific crystalline size and interlayer spacing properties taught by Stahl in order to provide a portion of the carbonaceous material having low viscosity and low resistivity (“The materials may inter alia be characterized by a low viscosity in dispersions and by exhibiting low electrical resistivity. Such materials can be advantageously used in various applications, for example in the manufacture of electrochemical cells such as lithium-ion batteries” Stahl [0001])
Conclusion
The following references were also considered to be relevant, but were not used in the above rejection:
Teixeira et al (2026)—teaches that commercially available Ketjen black EC600-JD have as ID/IG ratio of 1.57 plus or minus 0.09, which would meet/anticipate all of the limitations regarding this in claim 1.
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Ishida et al (2020)—The teachings found in Ishida et al show that the D/G ratio of Denka black is 1.25, which would anticipate the claimed range in claim 1. (“The crystal structure of Denka Black was between those of #32b and #4040b. Carbon black #32b, Denka Black, and #4040b are therefore referred to as less-crystalline, mid-crystalline, and highly crystalline carbons, respectively … The G/D band intensity ratios in the Raman spectra in Fig. 1b also show that the crystallinity of the highly crystalline carbon was higher than those of the others; the values were 2.8, 0.8, and 1.4 for the highly, mid-, and less-crystalline carbons, respectively.” Ishida results section lines 2-10.) By inverting the G/D ratio of 0.8, it is shown that the D/G ratio of Denka black is 1.25.
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/BENJAMIN ELI KASS-MULLET/Examiner, Art Unit 1752
/OLATUNJI A GODO/Primary Examiner, Art Unit 1752
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