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 .
Priority
Acknowledgment is made of applicant’s claim for foreign priority under 35 U.S.C. 119 (a)-(d).
Claim Objections
Claims 4, 15-16, 20 objected to because of the following informalities:
Claim 4 recites “the second solid electrolyte is included in an amount ranging from 20% by weight to 100% by weight, based on the total of the margin layers.” The Examiner believes the claims should be amended to recite “based on the total weight of the margin layers.”
Claim 15 recites “the second solid electrolyte is included in an amount ranging from 20% by weight to 100% by weight, based on the total of the margin layer.” The Examiner believes the claims should be amended to recite “based on the total weight of the margin layers.”
Claim 16 recites “the second solid electrolyte is included in an amount ranging from 20% by weight to 100% by weight, based on the total of the outer layer.” The Examiner believes the claims should be amended to recite “based on the total weight of the outer layer.”
Claim 20 recites “the negative electrode slayer.” The Examiner believes the claim should be amended to recite “the negative electrode s.”
Appropriate correction is required.
Claim Rejections - 35 USC § 112(b)
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.
Claims 5, 9, 16-17, and 20-22 are 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.
Regarding claims 5 and 17, the instant claims recite “a sintering temperature of the first solid electrolyte and the second solid electrolyte ranges from 470ºC to 550ºC.” However, it is unclear if the instant claimed limitation is directed toward a property of the first and second solid electrolytes or if the instant claimed limitation is directed toward a process in which the first solid electrolyte and second solid electrolyte are sintered at that temperature. Further, it is unclear if the sintering temperature of the first and second solid electrolytes must be the same and lie within the range or if they may be different and lie within the range. For the purposes of examination, the claim interpretation is interpreted by the Examiner as being met if the first solid electrolyte and the second solid electrolyte is capable of being sintered at a temperature lying within the instant claimed range. Appropriate correction is required.
Regarding claim 9, the instant claim recites “the ceramic includes alumina (A12O3), aluminum nitride (AlN), beryllium oxide (BeO), boron nitride (BN), silicon (Si), silicon carbide (SiC), silica (SiO2), silicon nitride (Si3N4), gallium arsenide (GaAs), gallium nitride (GaN), barium titanate (BaTiO3), zirconium dioxide (ZrO2), a mixture thereof, or oxides or nitrides of these materials.” However, it is unclear to the examiner what is meant by “oxides or nitrides of these materials” as some of the materials included in the list of exemplary ceramic materials are oxides and nitrides. Therefore, it is unclear if the scope of the limitation of “oxides or nitrides of these materials” is intended to refer to additional nitrides or oxides mixed with these materials. Appropriate correction is required.
Regarding claim 16, the instant claim recites “the second solid electrolyte is included in an amount ranging from 20% by weight to 100% by weight, based on the total of the outer layer.” As the independent claim 12 recites that the margin layer or the outer layer includes a second solid electrolyte, it is unclear if the instant claim requires the second solid electrolyte present in the outer layer or if the second solid electrolyte may be included in an amount in the margin layer which lies within the instant claimed range based on the total weight of the outer layer. For purposes of examination, the instant claim is interpreted by the Examiner to signify a proportion of second solid electrolyte present in the outer layer based on the total weight of the outer layer. Appropriate correction is required.
Regarding claim 20, the instant claim recites” “a cell laminate including a plurality of solid electrolyte layers, a plurality of positive electrode layers and negative electrode layers alternately disposed with the plurality of solid electrolyte layers interposed therebetween.” It is unclear to the Examiner the structure resulting from the instant claimed limitation. For example, if it unclear if the solid electrolyte layer between the positive electrode layer and the negative electrode layer is a multilayer structure or if the instant claim is directed toward a cell laminate comprising a single solid electrolyte layer between a positive electrode layer and a negative electrode layer, but the cell laminate comprising multiple positive and negative electrode layers and therefore multiple layers of solid electrolyte. For the purposes of Examination, the latter interpretation is understood. Appropriate correction is required.
Regarding claims 21-22, they are rejected based on their dependence on a previously rejected claim.
Claim Rejections - 35 USC § 103
In the event the determination of the status of the application as subject to AIA 35 U.S.C. 102 and 103 (or as subject to pre-AIA 35 U.S.C. 102 and 103) is incorrect, any correction of the statutory basis (i.e., changing from AIA to pre-AIA ) for the rejection will not be considered a new ground of rejection if the prior art relied upon, and the rationale supporting the rejection, would be the same under either status.
The following is a quotation of 35 U.S.C. 103 which forms the basis for all obviousness rejections set forth in this Office action:
A patent for a claimed invention may not be obtained, notwithstanding that the claimed invention is not identically disclosed as set forth in section 102, if the differences between the claimed invention and the prior art are such that the claimed invention as a whole would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to which the claimed invention pertains. Patentability shall not be negated by the manner in which the invention was made.
Claims 1-2, 5, 8 are rejected under 35 U.S.C. 103 as being unpatentable over Koga (U.S. Patent Publication No. 2023039438 A1).
Regarding claim 1, Koga teaches an all-solid-state battery, comprising: a cell laminate including a solid electrolyte layer; a positive electrode layer and a negative electrode layer disposed with the solid electrolyte layer interposed therebetween (Paragraph 0006);
Koga teaches the solid electrolyte has a first region containing a first solid electrolyte material and a second region containing a second solid electrolyte material (Paragraph 0006). Koga teaches a third embodiment of the invention disclosed which is exemplified in Figure 10(a), where the second region (Figure 10, Element 320) is disposed to be in contact with the outer rim portion on the four sides of the counter electrode layer (Paragraph 0154) and encompasses the electrode layer (Paragraph 0157).
Therefore, Koga teaches the aforementioned cell laminate comprising margin layers (second region) disposed at the edges of the positive electrode layer and the negative electrode layer, respectively, in a lateral direction, as shown in the annotated Figure below.
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Annotated Figure 10 of Koga
Koga teaches the solid electrolyte layer (Figure 10(a), Element 310) includes a first solid electrolyte and the margin layers (Figure 10(a), Element 320) include a second solid electrolyte (Paragraph 0006). Koga teaches the first solid electrolyte material and the second solid electrolyte material may be materials different from each other, for example a solid electrolyte material having a high heat dissipating property is used as the second solid electrolyte material, a solid electrolyte material having high metal ion conductivity can be used as the first solid electrolyte material (Paragraph 0080).
Koga does not explicitly teach the solid electrolyte layer includes a first solid electrolyte that is glass or glass ceramic that does not contain an element S (sulfur), and the margin layers include a second solid electrolyte that is glass or glass ceramic that contains the element S (sulfur).
However, Koga teaches that commonly known solid electrolytes for batteries can be used as the first solid electrolyte material and the second solid electrolyte material. Koga teaches exemplary examples of such materials including lithium containing sulfides (Li2S—P2S5, Li2S—SiS2, Li2S—B2S3, Li2S—GeS2, Li2S—SiS2 —LiI, Li2S—SiS2 —Li3PO4 , Li2S—Ge2S2, Li2S—GeS2—P2SF, and Li2S—GeS2 —ZnS) and lithium-containing metal oxides (Li2 —SiO2 and Li2 —SiO2 —P2O5), to name a few (Paragraph 0077).
It would have been obvious to a person having ordinary skill in the art prior to the effective filing date of the instant invention to select Li2 —SiO2 —P2O5 from the finite lists of possible combinations for lithium-containing metal oxide solid electrolyte materials to arrive at the first solid electrolyte of the instant claim since the combination of components would have yielded predictable results as a commonly used electrolyte material in the solid electrolyte layer of an all-solid-state-battery, absent a showing of unexpected results commensurate in scope with the claimed invention. See Section 2143 of the MPEP, rationales (A) and (E). It would have been further obvious to a person having ordinary skill in the art prior to the effective filing date of the instant invention to select any of the lithium containing sulfides from the finite lists of possible combinations for the solid electrolyte materials to arrive at the second solid electrolyte of the instant claim since the combination of components would have yielded predictable results as a commonly used electrolyte material in the margin layer of an all-solid-state-battery, absent a showing of unexpected results commensurate in scope with the claimed invention. See Section 2143 of the MPEP, rationales (A) and (E).
By providing the first solid electrolyte material of Koga as Li2 —SiO2 —P2O5 in accordance with the teachings of Koga, the instant claimed limitation of the solid electrolyte layer including a first solid electrolyte that is glass ceramic that does not contain an element S (sulfur) is met. By providing the second solid electrolyte material of Koga as a lithium-sulfide (any one of Li2S—P2S5, Li2S—SiS2, Li2S—B2S3, Li2S—GeS2, Li2S—SiS2 —LiI, Li2S—SiS2 —Li3PO4 , Li2S—Ge2S2, Li2S—GeS2—P2SF, and Li2S—GeS2 —ZnS) in accordance with the teachings of Koga, the instant claimed limitation of the margin layer including a second solid electrolyte that is a glass or glass ceramic that contains an element S (sulfur) is met.
Regarding claim 2, Koga teaches the all-solid-state battery of claim 1.
As discussed above in the rejection of claim 1, it would have been obvious to provide the first solid electrolyte material as Li2 —SiO2 —P2O5.
Therefore, Koga teaches the first solid electrolyte material is an oxide containing lithium and further containing silicon and phosphorous, meeting the instant claimed limitations.
Regarding claim 5, Koga teaches the all-solid-state battery of claim 1.
As described above in the 35 U.S.C. 112(b) rejection of claim 5, the limitation of “a sintering temperature of the first solid electrolyte and the second solid electrolyte ranges from 470°C to 550°C” is understood to require the first and second solid electrolyte materials to be capable of being sintered at a temperature between 470°C and 550°C.
As Koga teaches the first solid electrolyte that is a glass or glass ceramic not containing sulfur and the second solid electrolyte that is a glass or glass ceramic containing sulfur as required by the instant claimed limitation, Koga teaches the materials in the all-solid-state battery which align with those disclosed by the instant application and are thus capable of being sintered at a temperature between 470°C and 550°C, meeting the instant claimed limitations.
Regarding claim 8, Koga teaches the all-solid-state battery of claim 1.
Koga teaches that in addition to the solid electrolyte material, the second region (margin layer) can contain a bonding binder such as polyethylene oxide (Paragraph 0078).
As polyethylene oxide is known in the art to be an insulating resin, Koga meets the instant claimed limitations of the margin layer further including an insulating material including resin.
Claim 3 is rejected under 35 U.S.C. 103 as being unpatentable over Koga as applied to claims 1-2, 5, and 8 above, and further in view of Ikenomoto (W.O. 2024172493 A1).
Regarding claim 3, Koga teaches the all-solid-state battery of claim 1.
As discussed above in the rejection of claim 1, the second solid electrolyte material of Koga is a lithium-sulfide material exemplified by any one of Li2S—P2S5, Li2S—SiS2, Li2S—B2S3, Li2S—GeS2, Li2S—SiS2 —LiI, Li2S—SiS2 —Li3PO4 , Li2S—Ge2S2, Li2S—GeS2—P2SF, and Li2S—GeS2 —ZnS.
Koga is silent as to the second solid electrolyte is an oxide containing lithium (Li) and sulfur (S), and further containing boron (B), silicon (Si), phosphorus (P), aluminum (Al), germanium (Ge), chlorine (Cl), or combinations thereof.
However, Ikenomoto discloses a sulfide-based solid electrolyte implemented in an all-solid-state battery (Paragraph 1). Ikenomoto teaches that the sulfide-based solid electrolyte is a glass or glass ceramic electrolyte containing sulfur (Paragraphs 43-44) that may be suitably selected from Li2S-P2S5, Li2Si-Li-P2S5, Li2Si-Li2O-P2S5, Li2S-LiBr-P2S5, Li2S-Li2O-P2S5, Li2S-Li3PO4-P2S5, Li2S-P2S5-P2O5, Li2S-P2S5-SiS2, Li2S-P2S5-SnS, Li2S-P2S5-Al2S3, Li2S-GeS2, Li2S-GeS2-ZnS.
Therefore, given the general teachings of Ikenomoto, it would have been obvious to one of ordinary skill in the pertinent art before the effective filing date of the claimed invention to substitute either Li2Si-Li2O-P2S5 or Li2S-P2S5-P2O5 of Ikenomoto for Li2S—P2S5, Li2S—GeS2, or Li2S—GeS2 —ZnS of Koga, because Ikenomoto teaches the sulfide solid electrolyte material may suitably be selected as Li2Si—Li2O—P2S5, Li2S—P2S5—P2O5, Li2S—P2S5, Li2S—GeS2, or Li2S—GeS2 —ZnS.
The substitution would have been one known element for another and one of ordinary skill in the pertinent art would reasonably expect the predictable result that the modified composition would be useful as a solid electrolyte material is an all-solid-state battery possess the benefits of improved lithium-ion conductivity taught by Ikenomoto. See MPEP § 2143.I.(B).
The result of the modification of Koga in view of Ikenomoto is the second electrolyte material of Koga being Li2Si—Li2O—P2S5 or Li2S—P2S5—P2O5, which are known glass oxysulfide solid electrolyte materials in the art. Therefore, Koga in view of Ikenomoto teaches the second solid electrolyte is an oxide containing lithium, sulfur, silicon, and phosphorous, meeting the instant claimed limitations.
Claim 4 is rejected under 35 U.S.C. 103 as being unpatentable over Koga as applied to claims 1-2, 5, and 8 above, and further in view of Sugizaki (U.S. Patent Publication No. 20190088982A1).
Regarding claim 4, Koga teaches the all-solid-state battery of claim 1.
Koga is silent as to the second solid electrolyte is included in an amount ranging from 20% by weight to 100% by weight, based on the total of the margin layers.
However, Sugizaki discloses a solid-state battery comprising a first electrode, a second electrode, and a solid electrolyte layer (Paragraph 0029). Sugizaki teaches the solid electrolyte separator includes a central region and a peripheral edge region (Paragraph 0038).
Sugizaki teaches the peripheral edge region including solid electrolyte particles in proportion of 30% by weight to 100% by weight (Paragraph 0050). Sugizaki teaches the ion conductivity in the peripheral edge region is lower than the ion conductivity in the central region (Paragraph 0042), with the ion conductivity in the peripheral edge region preferably not more than 10-10, aligning with the ion conductivity of the second solid electrolyte of the instant application.
Sugizaki teaches that the lithium-ion conductivity in the peripheral edge region (margin layer) can be adjusted by changing the ratio of the weight of the solid electrolyte particles in this region (Paragraph 0051).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the margin layers of Koga to incorporate the teachings of Sugizaki in which the second solid electrolyte is included in an amount ranging from 30% by weight to 100% by weight. Doing so would advantageously result in the appropriate lithium-ion conductivity in this region (which is within the range of conductivity of the margin layer disclosed by the instant application).
The result of the modification is the presence of the second solid electrolyte in the margin layer in an amount which overlaps that of the instant invention. Therefore, prima facie obviousness is established and the instant claimed limitations are met. See MPEP 2144.05 (I).
Claims 5-7, 9, are rejected under 35 U.S.C. 103 as being unpatentable over Koga as applied to claims 1-2, 5, and 8 above, and further in view of Suzuki (U.S. Patent Publication No. 20190393505 A1).
Regarding claim 5, Koga teaches the all-solid-state battery of claim 1.
In the case that Koga is not found to teach a sintering temperature of the first solid electrolyte and the second solid electrolyte ranges from 470°C to 550°C, an alternate rejection of claim 5 is presented below in view of Suzuki.
Suzuki discloses an all-solid-state battery (Paragraph 0009) including an anode, cathode, solid electrolyte layer provided between the cathode and the anode layer (Paragraph 0057), and an exterior member (Figure 1B, Element 14) covering the peripheral ends of the cathode and anode layers, the exterior member containing a solid electrolyte (Paragraph 0063).
Suzuki teaches the solid electrolyte (equated with the instant first solid electrolyte) contained in the solid electrolyte layer is an oxide glass material sintered between 300ºC and 550ºC (Paragraph 0073). Suzuki teaches that when the sintering temperature is within the instant claimed range, the energy density of the battery can be improved (Paragraphs 0074-0076).
Further, Suzuki teaches that the solid electrolyte in the exterior member (Element 14) may be similar to that described in the solid electrolyte layer (Element 23). The solid electrolyte in the exterior member of Suzuki is equated with the instant second solid electrolyte.
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have also sintered the solid electrolyte in the exterior member of Suzuki. Given that Suzuki teaches the solid electrolyte in this area is similar to that of the solid electrolyte layer located between the electrodes of the cell stack, the ordinary artisan would find it obvious to also sinter the second solid electrolyte (solid electrolyte in the exterior member of Suzuki) given that it comprises similar materials and increasing energy density of the battery is a desirable attribute the ordinary artisan would want to obtain by sintering in the aforementioned range.
Therefore, it would have been further obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified Koga to incorporate the teachings of Suzuki in which the sintering temperature of the first and second solid electrolytes is 300ºC and 550ºC. Doing so would advantageously result in increased battery energy density, as recognized by Suzuki.
The result of the modification is to sinter the first and second solid electrolytes at a temperature lying within 300ºC and 550ºC. This range of temperatures overlaps with that of the instant claim. Therefore, prima facie obviousness is established and the instant claimed limitations are met. See MPEP 2144.05 (I).
Regarding claim 6, Koga teaches the all-solid-state battery of claim 1.
Koga is silent as to an ionic conductivity (25ºC) of the first solid electrolyte is 1 x 10-7 S/cm or more.
However, Suzuki discloses an all-solid-state battery (Paragraph 0009) including an anode, cathode, solid electrolyte layer provided between the cathode and the anode layer (Paragraph 0057), and an exterior member (Figure 1B, Element 14) covering the peripheral ends of the cathode and anode layers, the exterior member containing a solid electrolyte (Paragraph 0063).
Suzuki teaches that the ion conductivity of the solid electrolyte layer (the first solid electrolyte of Koga and the instant invention) is preferably 10-7 S/cm or more in order to improve battery performance (Paragraph 0072).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the first solid electrolyte of Koga to incorporate the teachings of Suzuki in which the ion conductivity of the layer is 10-7 S/cm or more, corresponding to the range of the instant claimed limitation. Doing so would advantageously result in improved battery performance, as recognized by Suzuki.
Regarding claim 7, Koga teaches the all-solid-state battery of claim 1.
Koga is silent as to an ionic conductivity (25ºC) of the second solid electrolyte is 5.0 x 10-9 S/cm or less.
However, as discussed above, Suzuki discloses an all-solid-state battery (Paragraph 0009) including an anode, cathode, solid electrolyte layer provided between the cathode and the anode layer (Paragraph 0057), and an exterior member (Figure 1B, Element 14) covering the peripheral ends of the cathode and anode layers, the exterior member containing a solid electrolyte (Paragraph 0063).
Suzuki teaches that the ion conductivity of the exterior member (the second solid electrolyte of Koga and the instant invention) is preferably 10-8 S/cm or less in order to suppress a self-discharge of the all-solid-state battery (Paragraph 0066).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the second solid electrolyte of Koga to incorporate the teachings of Suzuki in which the ion conductivity of the layer is 10-8 S/cm or less, which overlaps with the range of the instant claimed limitation. Doing so would advantageously result in suppressed self-discharge of the all-solid-state battery, as recognized by Suzuki
Regarding claim 9, Koga teaches the all-solid-state battery of claim 8.
Koga is silent as to the ceramic includes alumina (A12O3), aluminum nitride (AlN), beryllium oxide (BeO), boron nitride (BN), silicon (Si), silicon carbide (SiC), silica (SiO2), silicon nitride (Si3N4), gallium arsenide (GaAs), gallium nitride (GaN), barium titanate (BaTiO3), zirconium dioxide (ZrO2), a mixture thereof, or oxides or nitrides of these materials.
However, as discussed above, Suzuki discloses an all-solid-state battery (Paragraph 0009) including an anode, cathode, solid electrolyte layer provided between the cathode and the anode layer (Paragraph 0057), and an exterior member (Figure 1B, Element 14) covering the peripheral ends of the cathode and anode layers, the exterior member containing a solid electrolyte (Paragraph 0063).
Suzuki teaches that the exterior member (margin layer) may further contain crystal grains (Paragraph 0061) containing at least one of aluminum oxide : alumina (Al2O3), silicon oxide : quartz (SiO2), silicon nitride (SiN), aluminum nitride (AlN), and silicon carbide (SiC) (Paragraph 0064). Suzuki teaches that when the exterior member further contains crystal grains, a contraction of the exterior member is suppressed, resulting in reduced distortion (Paragraph 0061).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the margin layer of Koga to incorporate the teachings of Suzuki in which crystal grains containing at least one of aluminum oxide : alumina (Al2O3), silicon oxide: quartz (SiO2), silicon nitride (SiN), aluminum nitride (AlN), and silicon carbide (SiC) is contained. Doing so would advantageously result in reduced contraction and distortion of the margin layer, as recognized by Suzuki.
Therefore, Koga in view of Suzuki teaches the margin layer comprising at least one of alumina (A12O3), aluminum nitride (AlN), silicon carbide (SiC), silica (SiO2), or silicon nitride (Si3N4), meeting the instant claimed limitations.
Claim 10 is rejected under 35 U.S.C. 103 as being unpatentable over Koga as applied to claims 1-2, 5, and 8 above, and further in view of Inda (U.S. Patent Publication No. 20070259270 A1).
Regarding claim 10, Koga teaches the all-solid-state battery of claim 8.
Koga teaches the solid electrolyte in the margin layer, in addition to the solid electrolyte material, can comprise a bonding binder such as polyethylene oxide (Paragraph 0078).
Koga is silent as to the resin includes polyethylene, polypropylene, polyethylene terephthalate (PET), polyurethane, polyimide, or combinations thereof.
However, Indo discloses a solid electrolyte comprising a glass-ceramic material and a polymer (Paragraph 0023). Indo teaches that the polymer material in the solid electrolyte may be polyethylene oxide, polyethylene, polypropylene, polyolefin, fluorine-containing resin such as polytetrafluoroethylene, polychlorotrifluoroethylene and polyvinylidene fluoride, polyamides, polyesters and polyacrylates (Paragraph 0024).
Therefore, given the general teachings of Indo, it would have been obvious to one of ordinary skill in the pertinent art before the effective filing date of the claimed invention to substitute the polypropylene or polyethylene of Indo for the polyethylene oxide polymer material in the margin layer of Koga because Indo teaches the polymer material included in a solid electrolyte composition may suitably be selected as polyethylene oxide, polyethylene, or polypropylene. The substitution would have been one known element for another and one of ordinary skill in the pertinent art would reasonably expect the predictable result that the modified composition would be useful as a polymeric binding material in the margin layer of the all-solid battery and possess the benefits of increasing conductivity as taught by Indo. See MPEP § 2143.I.(B).
Claim 11, 12-13, 17-19 are rejected under 35 U.S.C. 103 as being unpatentable over Koga as applied to claims 1-2, 5, and 8 above, and further in view of Suzuki (cited above) and Ito (Japanese Patent Publication No. 2019087347 A).
Regarding claim 11, Koga teaches the all-solid-state battery of claim 1.
Koga is silent as to an outer layer disposed on one or both surfaces of the cell laminate in a stacking direction.
However, as discussed above, Suzuki discloses an all-solid-state battery (Paragraph 0009). Suzuki teaches an exterior member (also described above) including a portion which covers a surface of the battery element so that the peripheral portion of the solid electrolyte layer is not exposed from the entire end face of the exterior battery element (Paragraph 0059). Suzuki teaches the exterior member containing oxide glass or oxide glass ceramics in order to suppress moisture from permeating into the battery element by covering its surface (Element 20) with the exterior member (Paragraph 0060).
Therefore, as illustrated below, Suzuki teaches an all-solid-state battery including an outer layer disposed on one or both surfaces of the cell laminate in a stacking direction.
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Annotated Figure of Suzuki
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the all-solid-state battery of Koga to incorporate the teachings of Suzuki in which an outer layer is disposed on both surfaces of the cell laminate in a stacking direction. Doing so would advantageously prevent the exposure of the solid electrolyte layer from the end face of the exterior battery element and suppress moisture from permeating into the battery element, as recognized by Suzuki.
Koga is silent as to the outer layer includes the second solid electrolyte that is glass or glass ceramic that contains the element S (sulfur).
However, Suzuki teaches the exterior member may contain a solid electrolyte (equated with the instant second solid electrolyte) which is different in composition from that of the solid electrolyte layer (equated with the instant first solid electrolyte) (Paragraph 0063). As is seen in the annotated Figure below, Suzuki teaches the exterior member including the outer layer (exterior member on the outer surfaces of the cell laminate) and the margin layer (exterior member on the peripheral portion of the electrodes) which are indicated by Element 14.
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Therefore, it is clear that the exterior member of Suzuki refers to a composition of solid electrolyte which is positioned as the outer layer and the margin layer of the cell laminate. As described above in the rejection of claim 1, the second solid electrolyte in the margin layer of Koga was taught to be a glass or glass ceramic containing sulfur (Li2S—P2S5, Li2S—SiS2, Li2S—B2S3, Li2S—GeS2, Li2S—SiS2 —LiI, Li2S—SiS2 —Li3PO4 , Li2S—Ge2S2, Li2S—GeS2—P2SF, and Li2S—GeS2 —ZnS). Therefore, the ordinary artisan would recognize that in modifying Koga to incorporate the teachings of Suzuki pertaining to the outer layer, that the composition of the outer layer would be the same as that of the margin layer, namely including the second solid electrolyte that is glass or glass ceramic that contains the element S (sulfur), meeting the instant claimed limitations.
In the alternative, Ito discloses an all-solid battery including a solid electrolyte layer, a positive electrode layer, and a negative electrode layer (Paragraph 0006). Ito teaches a first margin layer (Element 60) and a second margin layer containing solid electrolyte (Paragraph 0033) as well as a first cover layer (Element 10) provided on the first outermost layer in the stacking direction and a second cover layer (Element 50) provided on the second outermost layer in the stacking direction (Paragraph 0010), the first and second cover layers comprising solid electrolyte (Paragraph 0040).
Ito teaches that it is preferable for the first and second cover layers to have the same composition as the first and second margin layer in order to prevent a reaction between the positive electrode and negative electrode with the cover layer interposed therebetween (Paragraph 0040).
Therefore, it would have been further obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the outer layer of Koga in view of Suzuki to incorporate the teachings of Ito in which the outer layer (cover layer of Ito) comprises the same composition as the margin layer (namely, the second solid electrolyte of Koga as described in the rejection of claim 1 above). Doing so would advantageously result in the suppression of the reaction between the electrodes and the cover layer when assembled into a battery module, as recognized by Ito.
Regarding claim 12, the instant claim shares the following limitations with claim 1 which are taught by Koga as discussed above in the rejection of claim 1:
an all-solid-state battery, comprising:
a cell laminate including
a solid electrolyte layer;
a positive electrode layer
and a negative electrode layer disposed with the solid electrolyte layer interposed therebetween;
and margin layers disposed at edges of the positive electrode layer and the negative electrode layer, respectively, in a lateral direction,
wherein the solid electrolyte layer includes a first solid electrolyte that is glass or glass ceramic that does not contain an element S (sulfur), and the margin layers or the outer layer includes a second solid electrolyte that is glass or glass ceramic that contains the element S (sulfur).
Koga is silent as to an outer layer disposed on one or both surfaces of the cell laminate in a stacking direction.
However, as discussed above in the rejection of claim 11, Suzuki discloses an all-solid-state battery (Paragraph 0009). Suzuki teaches an exterior member (also described above) including a portion which covers a surface of the battery element so that the peripheral portion of the solid electrolyte layer is not exposed from the entire end face of the exterior battery element (Paragraph 0059). Suzuki teaches the exterior member containing oxide glass or oxide glass ceramics in order to suppress moisture from permeating into the battery element by covering its surface (Element 20) with the exterior member (Paragraph 0060).
Therefore, as illustrated below, Suzuki teaches an all-solid-state battery including an outer layer disposed on one or both surfaces of the cell laminate in a stacking direction.
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Annotated Figure of Suzuki
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the all-solid-state battery of Koga to incorporate the teachings of Suzuki in which an outer layer is disposed on both surfaces of the cell laminate in a stacking direction. Doing so would advantageously prevent the exposure of the solid electrolyte layer from the end face of the exterior battery element and suppress moisture from permeating into the battery element, as recognized by Suzuki.
Although not required by the instant claim (the margin layer or the outer layer included a second solid electrolyte…), Koga is silent as to the outer layer includes the second solid electrolyte that is glass or glass ceramic that contains the element S (sulfur).
However, Suzuki teaches the exterior member may contain a solid electrolyte (equated with the instant second solid electrolyte) which is different in composition from that of the solid electrolyte layer (equated with the instant first solid electrolyte) (Paragraph 0063). As is seen in the annotated Figure below, Suzuki teaches the exterior member including the outer layer (exterior member on the outer surfaces of the cell laminate) and the margin layer (exterior member on the peripheral portion of the electrodes) which are indicated by Element 14.
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Therefore, it is clear that the exterior member of Suzuki refers to a composition of solid electrolyte which is positioned as the outer layer and the margin layer of the cell laminate. As described above in the rejection of claim 1, the second solid electrolyte in the margin layer of Koga was taught to be a glass or glass ceramic containing sulfur (Li2S—P2S5, Li2S—SiS2, Li2S—B2S3, Li2S—GeS2, Li2S—SiS2 —LiI, Li2S—SiS2 —Li3PO4 , Li2S—Ge2S2, Li2S—GeS2—P2SF, and Li2S—GeS2 —ZnS). Therefore, the ordinary artisan would recognize that in modifying Koga to incorporate the teachings of Suzuki pertaining to the outer layer, that the composition of the outer layer would be the same as that of the margin layer, namely including the second solid electrolyte that is glass or glass ceramic that contains the element S (sulfur), meeting the instant claimed limitations.
In the alternative, Ito discloses an all-solid battery including a solid electrolyte layer, a positive electrode layer, and a negative electrode layer (Paragraph 0006). Ito teaches a first margin layer (Element 60) and a second margin layer containing solid electrolyte (Paragraph 0033) as well as a first cover layer (Element 10) provided on the first outermost layer in the stacking direction and a second cover layer (Element 50) provided on the second outermost layer in the stacking direction (Paragraph 0010), the first and second cover layers comprising solid electrolyte (Paragraph 0040).
Ito teaches that it is preferable for the first and second cover layers to have the same composition as the first and second margin layer in order to prevent a reaction between the positive electrode and negative electrode with the cover layer interposed therebetween (Paragraph 0040).
Therefore, it would have been further obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the outer layer of Koga in view of Suzuki to incorporate the teachings of Ito in which the outer layer (cover layer of Ito) comprises the same composition as the margin layer (namely, the second solid electrolyte of Koga as described in the rejection of claim 1 above). Doing so would advantageously result in the suppression of the reaction between the electrodes and the cover layer when assembled into a battery module, as recognized by Ito.
Regarding claim 13, the instant claim shares the following limitations with claim 2 which are taught by Koga as discussed above in the rejection of claim 2:
the first solid electrolyte is an oxide containing lithium (Li), and further containing boron (B), silicon (Si), aluminum (Al), phosphorus (P), germanium (Ge), chlorine (Cl), or combinations thereof.
Regarding claim 17, the instant claim shares the following limitations with claim 5 which are taught by Koga as discussed above in the rejection of claim 5:
a sintering temperature of the first solid electrolyte and the second solid electrolyte ranges from 470°C to 550°C.
In the case that Koga is not found to teach a sintering temperature of the first solid electrolyte and the second solid electrolyte ranges from 470°C to 550°C, an alternate rejection of claim 5 is presented below in view of Suzuki.
Suzuki discloses an all-solid-state battery (Paragraph 0009) including an anode, cathode, solid electrolyte layer provided between the cathode and the anode layer (Paragraph 0057), and an exterior member (Figure 1B, Element 14) covering the peripheral ends of the cathode and anode layers, the exterior member containing a solid electrolyte (Paragraph 0063).
Suzuki teaches the solid electrolyte (equated with the instant first solid electrolyte) contained in the solid electrolyte layer is an oxide glass material sintered between 300ºC and 550ºC (Paragraph 0073). Suzuki teaches that when the sintering temperature is within the instant claimed range, the energy density of the battery can be improved (Paragraphs 0074-0076).
Further, Suzuki teaches that the solid electrolyte in the exterior member (Element 14) may be similar to that described in the solid electrolyte layer (Element 23). The solid electrolyte in the exterior member of Suzuki is equated with the instant second solid electrolyte.
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have also sintered the solid electrolyte in the exterior member of Suzuki. Given that Suzuki teaches the solid electrolyte in this area is similar to that of the solid electrolyte layer located between the electrodes of the cell stack, the ordinary artisan would find it obvious to also sinter the second solid electrolyte (solid electrolyte in the exterior member of Suzuki) given that it comprises similar materials and increasing energy density of the battery is a desirable attribute the ordinary artisan would want to obtain by sintering in the aforementioned range.
Therefore, it would have been further obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified Koga to incorporate the teachings of Suzuki in which the sintering temperature of the first and second solid electrolytes is 300ºC and 550ºC. Doing so would advantageously result in increased battery energy density, as recognized by Suzuki.
The result of the modification is to sinter the first and second solid electrolytes at a temperature lying within 300ºC and 550ºC. This range of temperatures overlaps with that of the instant claim. Therefore, prima facie obviousness is established and the instant claimed limitations are met. See MPEP 2144.05 (I).
Regarding claim 18, Koga teaches the all-solid-state battery of claim 12.
Modified Koga is silent as to an ionic conductivity (25ºC) of the first solid electrolyte is 1 x 10-7 S/cm or more.
However, as discussed above, Suzuki discloses an all-solid-state battery (Paragraph 0009) including an anode, cathode, solid electrolyte layer provided between the cathode and the anode layer (Paragraph 0057), and an exterior member (Figure 1B, Element 14) covering the peripheral ends of the cathode and anode layers, the exterior member containing a solid electrolyte (Paragraph 0063).
Suzuki teaches that the ion conductivity of the solid electrolyte layer (the first solid electrolyte of Koga and the instant invention) is preferably 10-7 S/cm or more in order to improve battery performance (Paragraph 0072).
Therefore, it would have been further obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the first solid electrolyte of Koga to incorporate the additional teachings of Suzuki in which the ion conductivity of the layer is 10-7 S/cm or more, corresponding to the range of the instant claimed limitation. Doing so would advantageously result in improved battery performance, as recognized by Suzuki.
Regarding claim 19, Koga teaches the all-solid-state battery of claim 12.
Modified Koga is silent as to wherein an ionic conductivity (25ºC) of the second solid electrolyte is 5.0 x 10-9 S/cm or less.
However, as discussed above, Suzuki discloses an all-solid-state battery (Paragraph 0009) including an anode, cathode, solid electrolyte layer provided between the cathode and the anode layer (Paragraph 0057), and an exterior member (Figure 1B, Element 14) covering the peripheral ends of the cathode and anode layers, the exterior member containing a solid electrolyte (Paragraph 0063).
Suzuki teaches that the ion conductivity of the exterior member (the second solid electrolyte of Koga and the instant invention) is preferably 10-8 S/cm or less in order to suppress a self-discharge of the all-solid-state battery (Paragraph 0066).
Therefore, it would have been further obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the second solid electrolyte of Koga to incorporate the additional teachings of Suzuki in which the ion conductivity of the layer is 10-8 S/cm or less, which overlaps with the range of the instant claimed limitation. Doing so would advantageously result in suppressed self-discharge of the all-solid-state battery, as recognized by Suzuki.
Claim 14 is rejected under 35 U.S.C. 103 as being unpatentable over Koga in view of Suzuki and Ito as applied to claims 11, 12-13, 17-19 above, and further in view of Ikenomoto (cited above, W.O. 2024172493 A1).
Regarding claim 14, Koga teaches the all-solid-state battery of claim 12.
As discussed above in the rejection of claims 1 and 12, the second solid electrolyte material of Koga is a lithium-sulfide material exemplified by any one of Li2S—P2S5, Li2S—SiS2, Li2S—B2S3, Li2S—GeS2, Li2S—SiS2 —LiI, Li2S—SiS2 —Li3PO4 , Li2S—Ge2S2, Li2S—GeS2—P2SF, and Li2S—GeS2 —ZnS.
Koga is silent as to the second solid electrolyte is an oxide containing lithium (Li) and sulfur (S), and further containing boron (B), silicon (Si), phosphorus (P), aluminum (Al), germanium (Ge), chlorine (Cl), or combinations thereof.
However, Ikenomoto discloses a sulfide-based solid electrolyte implemented in an all-solid-state battery (Paragraph 1). Ikenomoto teaches that the sulfide-based solid electrolyte is a glass or glass ceramic electrolyte containing sulfur (Paragraphs 43-44) that may be suitably selected from Li2S-P2S5, Li2Si-Li-P2S5, Li2Si-Li2O-P2S5, Li2S-LiBr-P2S5, Li2S-Li2O-P2S5, Li2S-Li3PO4-P2S5, Li2S-P2S5-P2O5, Li2S-P2S5-SiS2, Li2S-P2S5-SnS, Li2S-P2S5-Al2S3, Li2S-GeS2, Li2S-GeS2-ZnS.
Therefore, given the general teachings of Ikenomoto, it would have been obvious to one of ordinary skill in the pertinent art before the effective filing date of the claimed invention to substitute either Li2Si—Li2O—P2S5 or Li2S—P2S5—P2O5 of Ikenomoto for Li2S—P2S5, Li2S—GeS2, or Li2S—GeS2 —ZnS of Koga, because Ikenomoto teaches the sulfide solid electrolyte material may suitably be selected as Li2Si—Li2O—P2S5, Li2S—P2S5—P2O5, Li2S—P2S5, Li2S—GeS2, or Li2S—GeS2 —ZnS.
The substitution would have been one known element for another and one of ordinary skill in the pertinent art would reasonably expect the predictable result that the modified composition would be useful as a solid electrolyte material is an all-solid-state battery possess the benefits of improved lithium-ion conductivity taught by Ikenomoto. See MPEP § 2143.I.(B).
The result of the modification of Koga in view of Ikenomoto is the second electrolyte material of Koga being Li2Si-Li2O-P2S5 or Li2S-P2S5-P2O5, which are known glass oxysulfide solid electrolyte materials in the art. Therefore, Koga in view of Ikenomoto teaches the second solid electrolyte is an oxide containing lithium, sulfur, silicon, and phosphorous, meeting the instant claimed limitations.
Claims 15-16 are rejected under 35 U.S.C. 103 as being unpatentable over Koga in view of Suzuki and Ito as applied to 11, 12-13, 17-19 above, and further in view of Sugizaki (cited above, U.S. Patent Publication No. 20190088982A1).
Regarding claim 15, Koga teaches the all-solid-state battery of claim 12.
Koga is silent as to the second solid electrolyte is included in an amount ranging from 20% by weight to 100% by weight, based on the total of the margin layers.
However, Sugizaki discloses a solid-state battery comprising a first electrode, a second electrode, and a solid electrolyte layer (Paragraph 0029). Sugizaki teaches the solid electrolyte separator includes a central region and a peripheral edge region (Paragraph 0038).
Sugizaki teaches the peripheral edge region including solid electrolyte particles in proportion of 30% by weight to 100% by weight (Paragraph 0050). Sugizaki teaches the ion conductivity in the peripheral edge region is lower than the ion conductivity in the central region (Paragraph 0042), with the ion conductivity in the peripheral edge region preferably not more than 10-10, aligning with the ion conductivity of the second solid electrolyte of the instant application.
Sugizaki teaches that the lithium ion conductivity in the peripheral edge region (margin layer) can be adjusted by changing the ratio of the weight of the solid electrolyte particles in this region (Paragraph 0051).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the margin layers of Koga to incorporate the teachings of Sugizaki in which the second solid electrolyte is included in an amount ranging from 30% by weight to 100% by weight of the margin layer. Doing so would advantageously result in the appropriate lithium-ion conductivity in this region (which is within the range of conductivity of the margin layer disclosed by the instant application).
The result of the modification is the presence of the second solid electrolyte in the margin layer in an amount which overlaps that of the instant invention. Therefore, prima facie obviousness is established and the instant claimed limitations are met. See MPEP 2144.05 (I).
Regarding claim 16, Koga teaches the all-solid-state battery of claim 12.
Koga is silent as to the second solid electrolyte is included in an amount ranging from 20% by weight to 100% by weight, based on the total of the outer layer.
As discussed above in the rejection of claim 12, the modification of Koga by Suzuki resulted in an outer layer. As discussed above in the rejection of claim 12, the modification of Koga by Suzuki and Ito resulted in the second electrolyte particles in the outer layer.
Additionally discussed above, Sugizaki discloses a solid-state battery comprising a first electrode, a second electrode, and a solid electrolyte layer (Paragraph 0029). Sugizaki teaches the solid electrolyte separator includes a central region and a peripheral edge region (Paragraph 0038).
Sugizaki teaches the peripheral edge region including solid electrolyte particles in proportion of 30% by weight to 100% by weight (Paragraph 0050). Sugizaki teaches the ion conductivity in the peripheral edge region is lower than the ion conductivity in the central region (Paragraph 0042), with the ion conductivity in the peripheral edge region preferably not more than 10-10, aligning with the ion conductivity of the second solid electrolyte of the instant application.
Sugizaki teaches that the lithium-ion conductivity in the peripheral edge region (margin layer) can be adjusted by changing the ratio of the weight of the solid electrolyte particles in this region (Paragraph 0051).
Therefore, the ordinary artisan would recognize that by tuning the composition of solid electrolyte particles in the outer layer, the lithium-ion conductivity in the outer layer can be adjusted.
Absent unexpected results, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the outer layers of Koga in view of Suzuki and Ito to incorporate the teachings of Sugizaki to optimize the amount of solid electrolyte particles since it has been held that where general conditions of a claim are disclosed in the prior art, discovering the optimum or workable ranges involved only routine skill in the art. See MPEP 2144.05.
In the present invention, one would have been motivated to optimize the amount of solid electrolyte particles to be within the claimed ranges in order to achieve desired lithium-ion conductivity.
Alternatively, in the case in which the margin layers of Koga are modified to incorporate the teachings of Sugizaki in which the second solid electrolyte is included in an amount ranging from 30% by weight to 100% by weight of the margin layer as described above in the rejection of claim 15, it would have been further obvious to also provide the second solid electrolyte of the outer layer in an amount ranging from 30% by weight to 100% by weight of the margin layer. Such a modification is supported by Ito, who discloses that it is desirable for the outer layer (first and second cover layers) to have the same composition as the margin layers in order to prevent undesirable reactions. Thus, in modifying the margin layers of Koga to incorporate a specific amount of solid electrolyte particles, the ordinary artisan considering the teachings of Ito would also include the amount of solid electrolyte particles of Sugizaki in the same range, which as described above, overlaps the instant claimed range and establishes prima facie obviousness.
Regarding claim 20, Koga teaches an stacked all-solid-state battery, comprising: a cell laminate including a plurality of solid electrolyte layers, a plurality of positive electrode layers and negative electrode layers alternately disposed with the plurality of solid electrolyte layers interposed therebetween; and margin layers disposed at edges of the positive electrode layers and the negative electrode layer, respectively, in a lateral direction, wherein the solid electrolyte layers include a first solid electrolyte that is glass or glass ceramic that does not contain an element S (sulfur), and the margin layers include a second solid electrolyte that is glass or glass ceramic that contains the element S (sulfur).
Regarding claim 20, as discussed above in the rejection of claims 1 and 12, modified Koga teaches a cell laminate including a solid electrolyte layer, a positive electrode layer, and a negative electrode layer disposed with the solid electrolyte interposed therebetween; and margin layers disposed at edges of the positive electrode layer and the negative electrode layer, respectively, in a lateral direction, wherein the solid electrolyte layer includes a first solid electrolyte that is glass or glass ceramic that does not contain an element S (sulfur) and the margin layers include a second solid electrolyte that is glass or glass ceramic that contains the element S (sulfur).
Koga does not explicitly teach the all-solid-state battery is stacked with a plurality of solid electrolyte layers, a plurality of positive electrode layers and negative electrode layers alternately disposed with the plurality of solid electrolyte layers interposed therebetween.
However, one of ordinary skill in the art would have been motivated to provide additional solid electrolyte, positive electrode, and negative electrode layers in the all-solid-state battery, in order to provide higher energy capacity and power output of the battery. The mere duplication of parts, without any new or unexpected results, is within the ambit of one of ordinary skill in the art. See MPEP 2144.04.
Further, Suzuki provides evidence that it is known in the art to provide a plurality of cathode (Figure 4; Element 21), anode (Figure 4; Element 22), and solid electrolyte layers (Figure 4; Element 23), with the cathode and anode layers being alternately stacked with solid electrolyte layers interposed therebetween (Paragraph 0141) in a battery cell stack.
Therefore, it would have been further obvious to modify Koga to incorporate the teachings of Suzuki in which the cell laminate including a plurality of solid electrolyte layers, a plurality of positive electrode layers, and negative electrode layers alternately disposed with the plurality of solid electrolyte layers interposed therebetween (see 112b interpretation above), and margin layers (Element 14) disposed at edges of the positive electrode layers and negative electrode layers, meeting the instant claimed limitations.
Regarding claim 21, Koga teaches the stacked all-solid-state battery of claim 20.
The instant claim shares the following limitations with claim 11 and 12 which are taught by modified Koga as discussed above in the rejection of claims 11 and 12:
an outer layer disposed on one or both surfaces of the cell laminate in a stacking direction.
Regarding claim 22, Koga teaches the stacked all-solid-state battery of claim 21.
The instant claim shares the following limitations with claim 11 and 12 which are taught by modified Koga as discussed above in the rejection of claims 11 and 12:
the outer layer includes a second solid electrolyte that is glass or glass ceramic that contains the element S (sulfur).
Claims 1-3, 5-9 are rejected under 35 U.S.C. 103 as being unpatentable over Suzuki (cited above, U.S. Patent Publication No. 20190393505 A1).
Regarding claim 1, Suzuki teaches an all-solid-state battery, comprising: a cell laminate including a solid electrolyte layer; a positive electrode layer and a negative electrode layer disposed with the solid electrolyte layer interposed therebetween (Paragraph 0010).
Suzuki teaches an exterior member (Figure 1B, Element 14) covering the peripheral ends of the cathode and anode layers (Paragraph 0059). Therefore, Suzuki teaches margin layers disposed at edges of the positive electrode layer and the negative electrode layer, respectively, in a lateral direction, as shown in the annotated Figure below.
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Suzuki teaches the solid electrolyte (equated with the instant first solid electrolyte) contained in the solid electrolyte layer is an oxide glass material containing lithium (Paragraph 0077) and at least one of germanium, silicon, boron, and phosphorous (Paragraph 0078). Thus, Suzuki is considered to teach the solid electrolyte layer including a first solid electrolyte that is a glass or glass ceramic that does not contain an element S (sulfur).
Suzuki teaches the margin layer (exterior member) containing a solid electrolyte which may be the same or different from the electrolyte in the solid electrolyte layer (Paragraph 0063). Suzuki also teaches the margin layer containing oxide glass or oxide glass ceramics (Paragraph 0060). As discussed above, Suzuki teaches the solid electrolyte is at least one of an oxide glass and oxide glass ceramic. However, further, Suzuki teaches the solid electrolyte may further contain an additive element such as sodium (Na), magnesium (Mg), aluminum (Al), potassium (K), calcium (Ca), titanium (Ti), vanadium (V), chromium (Cr), manganese (Mn), iron (Fe), cobalt (Co), nickel (Ni), copper (Cu), zinc (Zn), gallium (Ga), selenium (Se), rubidium (Rb), sulfur (S), yttrium (Y), zirconium (Zr), niobium (Nb), molybdenum (Mo), silver (Ag), indium (In), tin (Sn), antimony (Sb), cesium (Cs), barium (Ba), hafnium (Hf), tantalum (Ta), tungsten (W), lead (Pb), bismuth (Bi), gold (Au), lanthanum (La), neodymium (Nd), and europium (Eu) (Paragraph 0082).
It would have been obvious to a person having ordinary skill in the art prior to the effective filing date of the instant invention to select sulfur from the finite lists of possible combinations for electrolyte additives to arrive at the second solid electrolyte of the instant claim since the combination of components would have yielded predictable results as an electrolyte in the margin layer of a cell laminate, absent a showing of unexpected results commensurate in scope with the claimed invention. See Section 2143 of the MPEP, rationales (A) and (E).
Therefore, Suzuki is considered by the Examiner to teach the margin layers include a second solid electrolyte that is glass or glass ceramic that contains the element S (sulfur).
Regarding claim 2, Suzuki teaches the all-solid-state battery of claim 1.
As discussed above in the rejection of claim 1, Suzuki teaches the first solid electrolyte is an oxide glass material or oxide glass ceramic containing lithium (Paragraph 0077) and at least one of germanium, silicon, boron, and phosphorous (Paragraph 0078). Thus, Suzuki is considered to teach the first solid electrolyte is an oxide containing lithium and further containing boron, silicon, germanium, and phosphorous, meeting the instant claimed limitations.
Regarding claim 3, Suzuki teaches the all-solid-state battery of claim 1.
As discussed above in the rejection of claim 1, Suzuki teaches the second solid electrolyte may be similar to the first solid electrolyte (Paragraph 0063). Therefore, Suzuki teaches the second solid electrolyte may be an oxide glass material or oxide glass ceramic containing lithium (Paragraph 0077) and at least one of germanium, silicon, boron, and phosphorous (Paragraph 0078). Thus, Suzuki is considered to teach the second solid electrolyte is an oxide containing lithium and further containing boron, silicon, germanium, and phosphorous, meeting the instant claimed limitations.
As described above, Suzuki teaches the electrolyte may comprise additives and it was found obvious to include sulfur in the second solid electrolyte composition, meeting the instant claimed limitations of the second solid electrolyte containing sulfur.
Regarding claim 5, Suzuki teaches the all-solid-state battery of claim 1.
As described above in the 35 U.S.C. 112(b) rejection of claim 5, the limitation of “a sintering temperature of the first solid electrolyte and the second solid electrolyte ranges from 470°C to 550°C” is understood to require the first and second solid electrolyte materials to be capable of being sintered at a temperature between 470°C and 550°C.
As Suzuki teaches the first solid electrolyte that is a glass or glass ceramic not containing sulfur and the second solid electrolyte that is a glass or glass ceramic containing sulfur as required by the instant claimed limitation, Suzuki teaches the materials in the all-solid-state battery which align with those disclosed by the instant application and are thus capable of being sintered at a temperature between 470°C and 550°C, meeting the instant claimed limitations.
In the alternative, Suzuki teaches the solid electrolyte (equated with the instant first solid electrolyte) contained in the solid electrolyte layer is an oxide glass material sintered between 300ºC and 550ºC (Paragraph 0073). Suzuki teaches that when the sintering temperature is within the instant claimed range, the energy density of the battery can be improved (Paragraphs 0074-0076).
Further, Suzuki teaches that the solid electrolyte in the exterior member (Element 14) may be similar to that described in the solid electrolyte layer (Element 23). The solid electrolyte in the exterior member of Suzuki is equated with the instant second solid electrolyte.
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have also sintered the solid electrolyte in the exterior member of Suzuki. Given that Suzuki teaches the solid electrolyte in this area is similar to that of the solid electrolyte layer located between the electrodes of the cell stack, the ordinary artisan would find it obvious to also sinter the second solid electrolyte (solid electrolyte in the exterior member of Suzuki) given that it comprises similar materials and increasing energy density of the battery is a desirable attribute the ordinary artisan would want to obtain by sintering in the aforementioned range.
The result of the modification is to sinter the first and second solid electrolytes at a temperature lying within 300ºC and 550ºC. This range of temperatures overlaps with that of the instant claim. Therefore, prima facie obviousness is established and the instant claimed limitations are met. See MPEP 2144.05 (I).
Regarding claim 6, Suzuki teaches the all-solid-state battery of claim 1.
Suzuki teaches that the ion conductivity of the solid electrolyte layer (the first solid electrolyte) is preferably 10-7 S/cm or more in order to improve battery performance (Paragraph 0072), which corresponds to the range of the instant claim, meeting the instant limitations.
Regarding claim 7, Suzuki teaches the all-solid-state battery of claim 1.
Suzuki teaches that the ion conductivity of the exterior member (the second solid electrolyte) is preferably 10-8 S/cm or less in order to suppress a self-discharge of the all-solid-state battery (Paragraph 0066). Therefore, Suzuki teaches a range of the ionic conductivity of the second solid electrolyte which overlaps the instant claimed range, establishing prima facie obviousness. See MPEP 2144.05 (I).
Regarding claim 8, Suzuki teaches the all-solid-state battery of claim 1.
Suzuki teaches that the exterior member (margin layer) may further contain crystal grains (Paragraph 0061) containing at least one of aluminum oxide : alumina (Al2O3), silicon oxide : quartz (SiO2), silicon nitride (SiN), aluminum nitride (AlN), and silicon carbide (SiC) (Paragraph 0064). Suzuki teaches that when the exterior member further contains crystal grains, a contraction of the exterior member is suppressed, resulting in reduced distortion (Paragraph 0061).
As alumina (A12O3), aluminum nitride (AlN), silicon carbide (SiC), silica (SiO2), silicon nitride (Si3N4) are exemplary insulating ceramic materials in the instant disclosure, Suzuki teaches the margin layers including an insulating material including ceramic.
Regarding claim 9, Suzuki teaches the all-solid-state battery of claim 8, wherein the ceramic includes alumina (A12O3), aluminum nitride (AlN), silicon carbide (SiC), silica (SiO2), silicon nitride (Si3N4).
Claims 11-14, 17-22 are rejected under 35 U.S.C. 103 as being unpatentable over Suzuki as applied to claims 1-3, 5-9 above, and further in view of Ito (cited above).
Regarding claim 11, Suzuki teaches the all-solid-state battery of claim 1.
as discussed above, Suzuki discloses an all-solid-state battery (Paragraph 0009). Suzuki teaches an exterior member (also described above) including a portion which covers a surface of the battery element so that the peripheral portion of the solid electrolyte layer is not exposed from the entire end face of the exterior battery element (Paragraph 0059). Suzuki teaches the exterior member containing oxide glass or oxide glass ceramics in order to suppress moisture from permeating into the battery element by covering its surface (Element 20) with the exterior member (Paragraph 0060).
Therefore, as illustrated below, Suzuki teaches an all-solid-state battery including an outer layer disposed on one or both surfaces of the cell laminate in a stacking direction.
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Suzuki teaches the exterior member may contain a solid electrolyte (equated with the instant second solid electrolyte) which is different in composition from that of the solid electrolyte layer (equated with the instant first solid electrolyte) (Paragraph 0063). As is seen in the annotated Figure below, Suzuki teaches the exterior member including the outer layer (exterior member on the outer surfaces of the cell laminate) and the margin layer (exterior member on the peripheral portion of the electrodes) which are indicated by Element 14.
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Therefore, it is clear that the exterior member of Suzuki refers to a composition of solid electrolyte which is positioned as the outer layer and the margin layer of the cell laminate. As described above in the rejection of claim 1, the second solid electrolyte in the margin layer of Suzuki was taught to be a glass oxide or glass ceramic oxide containing sulfur. Therefore, the ordinary artisan would recognize that in the teachings of Suzuki pertaining to the outer layer, that the composition of the outer layer would be the same as that of the margin layer, namely including the second solid electrolyte that is glass or glass ceramic that contains the element S (sulfur), meeting the instant claimed limitations.
In the alternative, Ito discloses an all-solid battery including a solid electrolyte layer, a positive electrode layer, and a negative electrode layer (Paragraph 0006). Ito teaches a first margin layer (Element 60) and a second margin layer containing solid electrolyte (Paragraph 0033) as well as a first cover layer (Element 10) provided on the first outermost layer in the stacking direction and a second cover layer (Element 50) provided on the second outermost layer in the stacking direction (Paragraph 0010), the first and second cover layers comprising solid electrolyte (Paragraph 0040).
Ito teaches that it is preferable for the first and second cover layers to have the same composition as the first and second margin layer in order to prevent a reaction between the positive electrode and negative electrode with the cover layer interposed therebetween (Paragraph 0040).
Therefore, it would have been further obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the outer layer of Suzuki to incorporate the teachings of Ito in which the outer layer (cover layer of Ito) comprises the same composition as the margin layer (namely, the second solid electrolyte as described in the rejection of claim 1 above). Doing so would advantageously result in the suppression of the reaction between the electrodes and the cover layer when assembled into a battery module, as recognized by Ito.
Regarding claim 12, the instant claim shares the following limitations with claim 1 which are taught by Suzuki as discussed above in the rejection of claim 1:
an all-solid-state battery, comprising:
a cell laminate including
a solid electrolyte layer;
a positive electrode layer
and a negative electrode layer disposed with the solid electrolyte layer interposed therebetween;
and margin layers disposed at edges of the positive electrode layer and the negative electrode layer, respectively, in a lateral direction,
wherein the solid electrolyte layer includes a first solid electrolyte that is glass or glass ceramic that does not contain an element S (sulfur), and the margin layers or the outer layer includes a second solid electrolyte that is glass or glass ceramic that contains the element S (sulfur).
As discussed above in the rejection of claim 11, Suzuki discloses an all-solid-state battery (Paragraph 0009). Suzuki teaches an exterior member (also described above) including a portion which covers a surface of the battery element so that the peripheral portion of the solid electrolyte layer is not exposed from the entire end face of the exterior battery element (Paragraph 0059). Suzuki teaches the exterior member containing oxide glass or oxide glass ceramics in order to suppress moisture from permeating into the battery element by covering its surface (Element 20) with the exterior member (Paragraph 0060).
Therefore, as illustrated below, Suzuki teaches an all-solid-state battery including an outer layer disposed on one or both surfaces of the cell laminate in a stacking direction.
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Although not required by the instant claim (the margin layer or the outer layer included a second solid electrolyte…), Suzuki teaches the outer layer includes the second solid electrolyte that is glass or glass ceramic that contains the element S (sulfur).
Suzuki teaches the exterior member may contain a solid electrolyte (equated with the instant second solid electrolyte) which is different in composition from that of the solid electrolyte layer (equated with the instant first solid electrolyte) (Paragraph 0063). As is seen in the annotated Figure below, Suzuki teaches the exterior member including the outer layer (exterior member on the outer surfaces of the cell laminate) and the margin layer (exterior member on the peripheral portion of the electrodes) which are indicated by Element 14.
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Therefore, it is clear that the exterior member of Suzuki refers to a composition of solid electrolyte which is positioned as the outer layer and the margin layer of the cell laminate. As described above in the rejection of claim 1, the second solid electrolyte in the margin layer of Suzuki was taught to be a glass oxide or glass oxide ceramic containing sulfur. Therefore, the ordinary artisan would recognize that the composition of the outer layer would be the same as that of the margin layer, namely including the second solid electrolyte that is glass or glass ceramic that contains the element S (sulfur), meeting the instant claimed limitations.
In the alternative, Ito discloses an all-solid battery including a solid electrolyte layer, a positive electrode layer, and a negative electrode layer (Paragraph 0006). Ito teaches a first margin layer (Element 60) and a second margin layer containing solid electrolyte (Paragraph 0033) as well as a first cover layer (Element 10) provided on the first outermost layer in the stacking direction and a second cover layer (Element 50) provided on the second outermost layer in the stacking direction (Paragraph 0010), the first and second cover layers comprising solid electrolyte (Paragraph 0040).
Ito teaches that it is preferable for the first and second cover layers to have the same composition as the first and second margin layer in order to prevent a reaction between the positive electrode and negative electrode with the cover layer interposed therebetween (Paragraph 0040).
Therefore, it would have been further obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the outer layer of Suzuki to incorporate the teachings of Ito in which the outer layer (cover layer of Ito) comprises the same composition as the margin layer (namely, the second solid electrolyte). Doing so would advantageously result in the suppression of the reaction between the electrodes and the cover layer when assembled into a battery module, as recognized by Ito.
Regarding claim 13, the instant claim shares the following limitations with claim 2 which are taught by Suzuki as discussed above in the rejection of claim 2:
the first solid electrolyte is an oxide containing lithium (Li), and further containing boron (B), silicon (Si), aluminum (Al), phosphorus (P), germanium (Ge), chlorine (Cl), or combinations thereof.
Regarding claim 14, the instant claim shares the following limitations with claim 3 which are taught by Suzuki as discussed above in the rejection of claim 3:
the second solid electrolyte is an oxide containing lithium (Li) and sulfur (S), and further containing boron (B), silicon (Si), aluminum (Al), phosphorus (P), germanium (Ge), chlorine (Cl), or combinations thereof.
Regarding claim 17, the instant claim shares the following limitations with claim 5 which are taught by Suzuki as discussed above in the rejection of claim 5:
a sintering temperature of the first solid electrolyte and the second solid electrolyte ranges from 470°C to 550°C.
Regarding claim 18, the instant claim shares the following limitations with claim 6 which are taught by Suzuki as discussed above in the rejection of claim 6:
an ionic conductivity (25ºC) of the first solid electrolyte is 1 x 10-7 S/cm or more.
Regarding claim 19, the instant claim shares the following limitations with claim 7 which are taught by Suzuki as discussed above in the rejection of claim 7:
an ionic conductivity (25ºC) of the second solid electrolyte is 5.0 x 10-9 S/cm or less.
Regarding claim 19, the instant claim shares the following limitations with claim 7 which are taught by Suzuki as discussed above in the rejection of claim 7:
an ionic conductivity (25ºC) of the second solid electrolyte is 5.0 x 10-9 S/cm or less.
Regarding claim 20, as discussed above in the rejection of claims 1 and 12, Suzuki teaches a cell laminate including a solid electrolyte layer, a positive electrode layer, and a negative electrode layer disposed with the solid electrolyte interposed therebetween; and margin layers disposed at edges of the positive electrode layer and the negative electrode layer, respectively, in a lateral direction, wherein the solid electrolyte layer includes a first solid electrolyte that is glass or glass ceramic that does not contain an element S (sulfur) and the margin layers include a second solid electrolyte that is glass or glass ceramic that contains the element S (sulfur).
As illustrated in Figure 4 of Suzuki, the battery element may comprise a plurality of cathode (Element 21), anode (Element 22), and solid electrolyte layers (Element 23), with the cathode and anode layers being alternately stacked with solid electrolyte layers interposed therebetween (Paragraph 0141).
Therefore, Suzuki teaches the cell laminate including a plurality of solid electrolyte layers, a plurality of positive electrode layers, and negative electrode layers alternately disposed with the plurality of solid electrolyte layers interposed therebetween (see 112b interpretation above), and margin layers (Element 14) disposed at edges of the positive electrode layers and negative electrode layers, meeting the instant claimed limitations.
Regarding claim 21, the instant claim shares the following limitations with claim 11 and 12 which are taught by Suzuki as discussed above in the rejection of claims 11 and 12:
an outer layer disposed on one or both surfaces of the cell laminate in a stacking direction.
Regarding claim 22, the instant claim shares the following limitations with claim 11 and 12 which are taught by Suzuki as discussed above in the rejection of claims 11 and 12:
the outer layer includes a second solid electrolyte that is glass or glass ceramic that contains the element S (sulfur).
Claim 4 is rejected under 35 U.S.C. 103 as being unpatentable over Suzuki as applied to claims 1-3, 5-9 above, and further in view of Sugizaki (cited above).
Regarding claim 4, Suzuki teaches the all-solid-state battery of claim 1.
Suzuki is silent as to the second solid electrolyte is included in an amount ranging from 20% by weight to 100% by weight, based on the total of the margin layers.
However, Sugizaki discloses a solid-state battery comprising a first electrode, a second electrode, and a solid electrolyte layer (Paragraph 0029). Sugizaki teaches the solid electrolyte separator includes a central region and a peripheral edge region (Paragraph 0038).
Sugizaki teaches the peripheral edge region including solid electrolyte particles in proportion of 30% by weight to 100% by weight (Paragraph 0050). Sugizaki teaches the ion conductivity in the peripheral edge region is lower than the ion conductivity in the central region (Paragraph 0042), with the ion conductivity in the peripheral edge region preferably not more than 10-10, aligning with the ion conductivity of the second solid electrolyte of the instant application and Suzuki.
Sugizaki teaches that the lithium ion conductivity in the peripheral edge region (margin layer) can be adjusted by changing the ratio of the weight of the solid electrolyte particles in this region (Paragraph 0051).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the margin layers of Suzuki to incorporate the teachings of Sugizaki in which the second solid electrolyte is included in an amount ranging from 30% by weight to 100% by weight. Doing so would advantageously result in the appropriate lithium-ion conductivity in this region (which is within the range of conductivity of the margin layer disclosed by the instant application).
The result of the modification is the presence of the second solid electrolyte in the margin layer in an amount which overlaps that of the instant invention. Therefore, prima facie obviousness is established and the instant claimed limitations are met. See MPEP 2144.05 (I).
Claims 15-16 are rejected under 35 U.S.C. 103 as being unpatentable over Suzuki in view of Ito as applied to claims 11-14, 17-22 above, and further in view of Sugizaki (cited above).
Regarding claim 15, Suzuki teaches the all-solid-state battery of claim 12.
Suzuki is silent as to the second solid electrolyte is included in an amount ranging from 20% by weight to 100% by weight, based on the total of the margin layers.
However, as discussed above, Sugizaki discloses a solid-state battery comprising a first electrode, a second electrode, and a solid electrolyte layer (Paragraph 0029). Sugizaki teaches the solid electrolyte separator includes a central region and a peripheral edge region (Paragraph 0038).
Sugizaki teaches the peripheral edge region including solid electrolyte particles in proportion of 30% by weight to 100% by weight (Paragraph 0050). Sugizaki teaches the ion conductivity in the peripheral edge region is lower than the ion conductivity in the central region (Paragraph 0042), with the ion conductivity in the peripheral edge region preferably not more than 10-10, aligning with the ion conductivity of the second solid electrolyte of the instant application.
Sugizaki teaches that the lithium-ion conductivity in the peripheral edge region (margin layer) can be adjusted by changing the ratio of the weight of the solid electrolyte particles in this region (Paragraph 0051).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the margin layers of Suzuki to incorporate the teachings of Sugizaki in which the second solid electrolyte is included in an amount ranging from 30% by weight to 100% by weight of the margin layer. Doing so would advantageously result in the appropriate lithium-ion conductivity in this region (which is within the range of conductivity of the margin layer disclosed by the instant application).
The result of the modification is the presence of the second solid electrolyte in the margin layer in an amount which overlaps that of the instant invention. Therefore, prima facie obviousness is established and the instant claimed limitations are met. See MPEP 2144.05 (I).
Regarding claim 16, Suzuki teaches the all-solid-state battery of claim 12.
Suzuki is silent as to the second solid electrolyte is included in an amount ranging from 20% by weight to 100% by weight, based on the total of the outer layer.
As discussed above in the rejection of claim 12, Suzuki teaches an outer layer. As discussed above in the rejection of claim 12, Suzuki as well as the modification of Suzuki by Ito taught the second electrolyte particles in the outer layer.
Additionally discussed above, Sugizaki discloses a solid-state battery comprising a first electrode, a second electrode, and a solid electrolyte layer (Paragraph 0029). Sugizaki teaches the solid electrolyte separator includes a central region and a peripheral edge region (Paragraph 0038).
Sugizaki teaches the peripheral edge region including solid electrolyte particles in proportion of 30% by weight to 100% by weight (Paragraph 0050). Sugizaki teaches the ion conductivity in the peripheral edge region is lower than the ion conductivity in the central region (Paragraph 0042), with the ion conductivity in the peripheral edge region preferably not more than 10-10, aligning with the ion conductivity of the second solid electrolyte of the instant application.
Sugizaki teaches that the lithium-ion conductivity in the peripheral edge region (margin layer) can be adjusted by changing the ratio of the weight of the solid electrolyte particles in this region (Paragraph 0051).
Therefore, the ordinary artisan would recognize that by tuning the composition of solid electrolyte particles in the outer layer, the lithium-ion conductivity in the outer layer can be adjusted.
Absent unexpected results, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the outer layers of Suzuki in view of Ito to incorporate the teachings of Sugizaki to optimize the amount of solid electrolyte particles since it has been held that where general conditions of a claim are disclosed in the prior art, discovering the optimum or workable ranges involved only routine skill in the art. See MPEP 2144.05. In the present invention, one would have been motivated to optimize the amount of solid electrolyte particles to be within the claimed ranges in order to achieve desired lithium-ion conductivity.
Alternatively, in the case in which the margin layers of Suzuki are modified to incorporate the teachings of Sugizaki in which the second solid electrolyte is included in an amount ranging from 30% by weight to 100% by weight of the margin layer as described above in the rejection of claim 15, it would have been further obvious to also provide the second solid electrolyte of the outer layer in an amount ranging from 30% by weight to 100% by weight of the margin layer.
Such a modification is supported by Ito, who discloses that it is desirable for the outer layer (first and second cover layers) to have the same composition as the margin layers in order to prevent undesirable reactions. Thus, in modifying the margin layers of Suzuki to incorporate a specific amount of solid electrolyte particles, the ordinary artisan considering the teachings of Ito would also include the amount of solid electrolyte particles of Sugizaki in the same range, which as described above, overlaps the instant claimed range and establishes prima facie obviousness.
Claim 10 is rejected under 35 U.S.C. 103 as being unpatentable over Suzuki as applied to claims 1-3, 5-9 above, and further in view of Inda (U.S. Patent Publication No. 20070259270 A1).
Regarding claim 10, Suzuki teaches the all-solid-state battery of claim 8.
In the method of forming the exterior member, Suzuki teaches an organic-based binder can be included in the paste (Paragraph 0121).
Suzuki is silent as to the margin layer including an insulating resin that is polyethylene, polypropylene, polyethylene terephthalate (PET), polyurethane, polyimide, or combinations thereof.
However, Inda discloses a solid electrolyte comprising a glass-ceramic material and a polymer. Inda teaches that the polymer constituting the composite electrolyte can increase cell capacity per unit volume and has flexibility that enables the cell to be formed in various shapes (Paragraph 0023). Inda teaches that the polymer material in the solid electrolyte may be polyethylene oxide, polyethylene, polypropylene, polyolefin, fluorine-containing resin such as polytetrafluoroethylene, polychlorotrifluoroethylene and polyvinylidene fluoride, polyamides, polyesters, and polyacrylates (Paragraph 0024).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the margin layer of Suzuki to incorporate the teachings of Inda in which a polymer such as polyethylene or polypropylene. Doing so would advantageously result in increased cell capacity and flexibility, as recognized by Indo.
Conclusion
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/O.A.J./Examiner, Art Unit 1789
/JENNIFER A BOYD/Supervisory Patent Examiner, Art Unit 1786
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