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 .
Drawings
The drawings are objected to as failing to comply with 37 CFR 1.84(p)(4) because reference character “20” has been used to designate both parts 11-12 and 21-22 in Figure 5 and parts 11-12 and 21-23 in Figure 6. Corrected drawing sheets in compliance with 37 CFR 1.121(d) are required in reply to the Office action to avoid abandonment of the application. Any amended replacement drawing sheet should include all of the figures appearing on the immediate prior version of the sheet, even if only one figure is being amended. Each drawing sheet submitted after the filing date of an application must be labeled in the top margin as either “Replacement Sheet” or “New Sheet” pursuant to 37 CFR 1.121(d). If the changes are not accepted by the examiner, the applicant will be notified and informed of any required corrective action in the next Office action. The objection to the drawings will not be held in abeyance.
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.
The factual inquiries for establishing a background for determining obviousness under 35 U.S.C. 103 are summarized as follows:
1. Determining the scope and contents of the prior art.
2. Ascertaining the differences between the prior art and the claims at issue.
3. Resolving the level of ordinary skill in the pertinent art.
4. Considering objective evidence present in the application indicating obviousness or non-obviousness.
Claim 1-4, 6, 7, 9, 11, 12, 14-17 and 20 are rejected under 35 U.S.C. 103 as being unpatentable over Wang et al. (CN 112599846 A, see machine translation for citation).
Regarding claim 1, Wang teaches a method for preparing a composite electrolyte membrane for an all-solid-state lithium metal negative electrode battery [0019]. The composite electrolyte membrane is made by stacking and compounding a polymer solid-state electrolyte membrane and a sulfide solid-state electrolyte membrane [0019]. The sulfide solid electrolyte membrane may comprise one or more of Li10GeP2S12,Li6PS5Cl,Li10SnP2S12,Li2S-P2S5,Li2S-SiS2,Li2S-B2S3 as sulfide electrolyte materials [0026 and 0027]. Also the sulfide solid electrolyte membrane comprises a binder which may be selected from one or more of polyvinylidene fluoride (PVDF), nitrile rubber (NBR), hydrogenated nitrile rubber (HNBR), styrene butadiene rubber, styrene-butadiene-styrene block copolymer (SBS), styrene-butene copolymer (SEBS) and polyethylene oxide (PEO) [0028].
Wang is analogous art to the current invention because it is concerned with the same field of endeavor, namely a solid electrolyte, comprising: a sulfide solid electrolyte and may comprise a first binder and a second binder.
From the previous teachings of Wang, it would have been prima facie obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to prepare a solid sulfide electrolyte membrane having one or more sulfide solid electrolytes and one or more binders, which may be selected as the first and second binder respectively. Since the taught binders are chemically different from each other, it would have been obvious that the energy of adhesion values for the “first and second” binders with respect to the selected sulfide electrolyte would be different.
The Office realizes that all of the claimed effects or physical properties are not positively stated by Wang. However, Wang teaches all of the components of the claimed solid electrolyte, i.e. a sulfide solid electrolyte membrane comprising Li6PS5Cl and hydrogenated nitrile rubber (HNBR) and styrene butadiene rubber as binders (first and second). According to the original specification, the compounds adhesion energies shown in Table 1, are presented with respect to a sulfide-based solid electrolyte [0050]. It is taught that the sulfide-based solid electrolyte may be for example, Li6PS5Cl [0049], description from which other of the taught electrolytes may be used as the referred sulfide-based solid electrolyte. From the above discussion and Table 1, hydrogenated nitrile rubber (HNBR) and styrene butadiene rubber (SBR) are reported to have an energy of adhesion of -444,076.6 kcal/mol (less than -300,000 kilocalorie per mole) and -204,937.4 kcal/mol (more than -300,000 kilocalorie per mole), respectively.
Therefore, the claimed effects and physical properties, i.e. the claimed first and second binder energy of adhesion with respect to the sulfide solid electrolyte and its respective absolute values comparison, would expectedly be achieved by a composition with all the components of the claimed solid electrolyte. See MPEP § 2112.01. If it is the applicant' s position that this would not be the case: (1) evidence would need to be provided to support the applicant' s position; and (2) it would be the Office' s position that the application contains inadequate disclosure that there is no teaching as to how to obtain the claimed properties with only the claimed ingredients, claimed amounts, and substantially similar process of making.
Regarding claim 2, Wang teaches all the elements of the current invention in claim 1. From claim 1 discussion and selecting SBR as the second binder the claimed limitation is met.
Regarding claim 3, Wang teaches all the elements of the current invention in claim 1. From claim 1 discussion, if HNBR and SBR are selected as the first and second binder respectively the absolute value of a difference between their energy of adhesion is 239, 139.2 kcal/mol, from which the claimed limitation is met.
Regarding claim 4, Wang teaches all the elements of the current invention in claim 1. From claim 1 discussion, if HNBR and SBR are selected as the first and second binder respectively, the limitations “wherein the first binder comprises a repeating unit comprising a nitrile group” and wherein “and the second binder comprises a repeating unit comprising one or more nonpolar functional groups selected from butadiene and styrene” are met.
Regarding claims 6 and 9, Wang teaches all the elements of the current invention in claim 1. From claim 1 discussion, if HNBR is selected as the first binder, the limitations “a nitrile copolymer comprising an α, β-unsaturated nitrile first repeating unit and a conjugated diene second repeating unit” (claim 6) and wherein the nitrile copolymer “is a hydrogenated acrylonitrile-butadiene rubber comprising a nitrile repeating unit, a butadiene repeating unit, and a hydrogenated butadiene repeating unit” (claim 9) are met.
Regarding claim 7, Wang teaches one of the possible the elements of the current invention in claim 6. Since the compound taught by Wang, which can be selected as the first binder, is “a nitrile copolymer comprising an α, β-unsaturated nitrile first repeating unit and a conjugated diene second repeating unit”, the limitations recited on claim 7 are not applicable to it.
Regarding claim 11, Wang teaches all the elements of the current invention in claim 1. From claim 1 discussion, HNBR can be selected as the “first binder” from which the limitation “wherein the first binder is a hydrogenated acrylonitrile-butadiene rubber” is met.
Regarding claim 12, Wang teaches all the elements of the current invention in claim 1. From claim 1 discussion, styrene-butadiene-styrene block copolymer (SBS) can be selected as the “second binder” from which the limitation “wherein the second binder is a styrene butadiene styrene copolymer” is met.
Regarding claim 14, Wang teaches all the elements of the current invention in claim 1. From claim 1 discussion, Li6PS5Cl is presented as part of the possible sulfide electrolyte employable materials and it is an argyrodite type compound.
Regarding claim 15, Wang teaches all the elements of the current invention in claim 1. From claim 1 discussion, Li6PS5Cl,Li2S-P2S5 and Li2S-SiS2 are presented as sulfide electrolyte employable materials, from which the claimed limitation is met.
Regarding claim 16, Wang teaches all the elements of the current invention in claim 1, except the claimed properties as recited on claim 16.
The Office realizes that all of the claimed effects or physical properties are not positively stated by Wang. However, Wang teaches all of the claimed ingredients, i.e. a sulfide solid electrolyte membrane comprising Li6PS5Cl and hydrogenated nitrile rubber (HNBR) and styrene butadiene rubber as binders (first and second). According to the original specification, a solid electrolyte according to an embodiment, including a sulfide-based solid electrolyte, a first binder and a second binder, may have a Vickers hardness of 75 HV or more, a toughness of about 0.3 MPa to about 3 MPa, a Young's modulus of about 70 MPa to about 25 GPa, a tensile strength of about 2 MPa to about 50 MPa, and an elongation at break of about 0.1% to about 30% [0090 and 0091]. The solid electrolyte may have an ionic conductivity at 25 °C of about 0.1 mS/cm to about 5 mS/cm [0089]. The first binder and the second binder may be, respectively, hydrogenated nitrile butadiene rubber (HNBR) and styrene butadiene rubber (SBR) and the sulfide solid electrolyte may be at least one of Li2S-P2S5, Li2S-SiS2 and Li7-xPS6-xClx (0<x<2), among other materials [0075 and 0088].
Therefore, the claimed effects and physical properties, i.e. the claimed properties, would expectedly be achieved by a composition with all the claimed ingredients, claimed amounts, and substantially similar process of making. See MPEP § 2112.01. If it is the applicant' s position that this would not be the case: (1) evidence would need to be provided to support the applicant' s position; and (2) it would be the Office' s position that the application contains inadequate disclosure that there is no teaching as to how to obtain the claimed properties with only the claimed ingredients, claimed amounts, and substantially similar process of making.
Regarding claim 17, Wang teaches all the elements of the current invention in claim 1. Wang further teaches an all solid-state sulfide lithium-ion battery comprising a positive electrode, a negative electrode and the composite electrolyte (as taught for claim 1) between them [0038 and claim 14]. Since the battery is prepared as a soft package battery which can be cycled, it is a secondary battery [0038].
Regarding claim 20, Wang teaches all the elements of the current invention in claim 1. Wang further teaches that in a preferred embodiment the sulfide solid electrolyte membrane is prepared by dissolving the binder in a second solvent to prepare a glue solution, mixing the glue solution with a sulfide electrolyte to form a second mixed solution; coating a second mixed solution on the surface of the second substrate, and drying to obtain the sulfide solid electrolyte membrane attached to the surface of the second substrate [0026]. Because I was previously taught for claim 1 that the binder may be selected from group of materials, from which a first and second binder can be selected, the claimed limitations are met.
Claim 5 is rejected under 35 U.S.C. 103 as being unpatentable over Wang et al. (CN 112599846 A, see machine translation for citation) as applied to claim 1 above, further in view of Kim et al. (US 20210202949 A1).
Regarding claim 5, Wang teaches all the elements of the current invention in claim 1, except “wherein a weight ratio of the first binder to the second binder is about 1:9 to about 9:1”.
Kim teaches a solid electrolyte layer (10), employable on an all solid-state battery, which is preferred to include a sulfide solid electrolyte having high lithium ion conductivity [0044 and 0081]. The solid electrolyte layer (10) may comprise a binder solution, which have a first and a second binder [0046 and 0079]. The binder solution may include 10 wt. % or less, but exceeding 0 wt. %, of the first binder and the second binder [0062]. From the previous taught ranges the “weight ratio of the first binder to the second binder being about 1:9 to about 9:1” is overlapped. It is taught that when the sum of the amount of the first binder and the amount of the second binder falls in the above range, the binding force and lithium ion conductivity of the binder solution may be obtained at desired levels in a balanced manner [0062].
Kim is analogous art to the current invention because it is concerned with the same field of endeavor, namely a solid electrolyte , comprising: a sulfide solid electrolyte, a first binder and a second binder.
It would have been obvious to one of ordinary skill in the art before the effective filing date of the invention to have selected the overlapping portion of the first and second binder content disclosed by Kim, from which the claimed weight ratio would be overlapped, because overlapping ranges have been held to be a prima facie case of obvious. In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990). See MPEP § 2144.05.
Claim 8 is rejected under 35 U.S.C. 103 as being unpatentable over Wang et al. (CN 112599846 A, see machine translation for citation) as applied to claim 7 above, further in view of Maeda (US 20180254520 A1).
Regarding claim 8, Wang teaches one of the possible the elements of the current invention in claim 7, except “wherein the first binder is an (meth)acrylate copolymer, and a content of the (meth)acrylate repeating unit in the acrylate copolymer is about 50 wt.% to less than 100 wt.%, and a content of the non-(meth)acrylate repeating unit in the (meth)acrylate copolymer is greater than 0 wt.% to about 50 wt.%”.
Maeda teaches an all solid state secondary battery comprising a solid electrolyte layer, a positive electrode and a negative electrode [0044]. The solid electrolyte layer comprises solid electrolyte particles and a binder for a solid electrolyte layer, where the electrolyte particles may be a sulfide solid electrolyte material [0046 and 0054]. The employed binder is obtained by polymerizing or copolymerizing a monomer composition containing a polyalkylene oxide-based monomer, which may be a (meth)acrylate [0019 and 0020]. The binder may contain a monomer unit derived from a (meth) acrylate copolymerized with a copolymerizable monomer such as methacrylamide, vinyl acetate, N-vinyl pyrrolidone, among others [0026 and 0027]. As examples of the employable (meth)acrylate monomers methyl methacrylate, ethyl methacrylate and n-butyl methacrylate are mentioned, among other materials [0024]. It is taught that a content ratio of a monomer unit derived from a (meth)acrylate in the binder polymer used in the present invention is usually 40% by mass or more and a content ratio of the copolymerizable monomer in the binder polymer used in the present invention is usually 50% by mass or less [0025 and 0027]. It is taught that all-solid-state secondary batteries, containing the above taught binder had excellent output and charge/discharge cycle characteristics [0122].
Maeda is analogous art to the current invention because it is concerned with the same field of endeavor, namely a solid electrolyte comprising a sulfide solid electrolyte and a binder having a (meth)acrylate and non-(meth)acrylate repeating unit.
If one of the possible Maeda’s taught copolymers is incorporated in the binder taught by Wang, this material could be selected as the “first binder” and the recited limitations would be met because the repeating units content will be overlapped.
It would have been prima facie obvious to one of ordinary skill in the art before the
effective filing date of the claimed invention to modify the binder of Wang to include the feature “wherein the first binder is an (meth)acrylate copolymer”, because Maeda teaches that that an all-solid-state secondary battery comprising this polymeric binder had excellent output and charge/discharge cycle characteristics.
It would have been obvious to one of ordinary skill in the art before the effective filing date of the invention to have selected the overlapping portion of the (meth)acrylate and non-(meth)acrylate repeating units content ranges disclosed by Maeda because overlapping ranges have been held to be a prima facie case of obvious. In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990). See MPEP § 2144.05.
Claim 10 is rejected under 35 U.S.C. 103 as being unpatentable over Wang et al. (CN 112599846 A, see machine translation for citation) as applied to claim 6 above, evidenced by GMOR (HNBR, see NPL documents for citation).
Regarding claim 10, Wang teaches all the elements of the current invention in claim 6. Regarding the “nitrile copolymer having a content of the nitrile repeating unit about 10 wt.% to about 50 wt.%”, GMOR evidence that in hydrogenated nitrile rubber (HNBR) polymers the content of acrylonitrile (ACN) (nitrile repeating unit) can be varied from 17% to 49% [p. 1; par. 2].
Claim 13 is rejected under 35 U.S.C. 103 as being unpatentable over Wang et al. (CN 112599846 A, see machine translation for citation) as applied to claim 1 above, further in view of Van Berkel et al. (US 20170005367 A1).
Regarding claim 13, Wang teaches all the elements of the current invention in claim 1. From claim 1 discussion, the first and second binder can be selected as hydrogenated nitrile butadiene rubber and styrene butadiene rubber respectively.
Wang does not teach the feature “wherein a total content of the first binder and the second binder is about 1 part by weight to about 5 parts by weight with respect to a total weight of 100 parts by weight of the solid electrolyte”.
Van Berkel teaches a variety of composite electrolytes, which in any of the examples herein may be a solid [0110 and 0126]. The described electrolyte is an inorganic material embedded in an organic material, where the organic material in is bonded to, adsorbed on, molded around, or entangled with the surface of the inorganic material, a surface attached species on the surface of the inorganic material, or an inorganic material particle [0111 and 0112]. It is taught that in some examples, the solid state electrolyte is sulfide electrolyte [0197]. The taught composite electrolyte, in certain examples, include a polymer or organic binder, as the organic material [0070].
In some examples, the above taught organic material is a polymer and it may be selected from a group of materials on which nitrile butadiene rubber and styrene butadiene rubber, among others, are mentioned [0199]. In some examples, the electrolyte or composite electrolyte, herein, includes an inorganic material and an organic material in a weight ratio of (inorganic material):(organic material) of at least 1:1 to 99:1 [0189]. From the above teaching, a solid electrolyte having a sulfide electrolyte and a binder comprising a nitrile butadiene rubber, family to which hydrogenated nitrile butadiene rubber belongs, and styrene butadiene rubber (first and second binder analogous). Having 100 parts of a solid sulfide electrolyte, the employable amount of the binder would be between 100 to 1.01 parts, which overlaps the claimed ratio.
Van Berkel is analogous art to the current invention because it is concerned with the same field of endeavor, namely a solid electrolyte comprising a sulfide solid electrolyte and binder materials which can be selected as the first and second binders.
It would have been obvious to one of ordinary skill in the art before the effective filing date of the invention to have selected the overlapping portion of the binder weight ratio ranges disclosed by Van Berkel because overlapping ranges have been held to be a prima facie case of obvious. In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990). See MPEP § 2144.05.
Claims 18 and 19 are rejected under 35 U.S.C. 103 as being unpatentable over Wang et al. (CN 112599846 A, see machine translation for citation) as applied to claim 17 above, further in view of Kim et al. (US 20210280853 A1).
Regarding claims 18 and 19, Wang teaches all the elements of the current invention in claim 17, except wherein the anode comprises an anode current collector and a first anode active material layer as recited on claim 18 and a second anode active material as recited on claim 19.
Kim teaches an all-solid secondary battery (1) including a cathode (10), an anode (20) and a solid electrolyte layer (30) interposed between them [0083 and Fig. 1]. The solid electrolyte layer (30) may comprise a sulfide-based solid electrolyte and a binder or a combination of binders which is not particularly limited [0103 and 0106]. From this description a solid sulfide electrolyte having a first and second binder is achievable. The anode (20) includes an anode current collector (21), a first anode active material layer (221) which may be disposed on the anode current collector (21) and a second anode active material layer (222) which may be disposed over the first anode active material layer (221) [0107, 0114 and Fig. 1]. The first anode active material layer (221) may be a first metal layer including lithium metal or a lithium alloy (analogous to the second anode active material layer of claim 19) [0111]. The second anode active material layer (222) may include an anode active material including a carbon-based active material, a metal or a metalloid anode active material, or a combination of the carbon-based active material and the metal or metalloid active material (analogous to the second anode active material layer of claim 18) [0121]. It is taught that during a charging process, the pressure applied by an anode having the above configuration on the solid electrolyte layer (30) is reduced, and thus a short-circuit of the solid electrolyte layer (30) may be delayed [0126].
Kim is analogous art to the current invention because it is concerned with the same field of endeavor, namely a solid electrolyte comprising a sulfide electrolyte which may have a first and second binder. In addition such solid electrolyte is employable on an all-solid secondary battery.
If the lithium metal negative electrode of Wang is modified to have a configuration as the anode taught by Kim, the limitations of claims 18 and 19 would be met.
It would have been prima facie obvious to one of ordinary skill in the art before the
effective filing date of the claimed invention to modify the lithium metal negative electrode of Wang to include the features wherein the anode comprises an anode current collector and a first anode active material layer as recited on claim 18 and a second anode active material as recited on claim 19, because Kim teaches that during a charging process, the pressure applied by an anode having the above configuration on the solid electrolyte layer is reduced, and thus a short-circuit of the solid electrolyte layer may be delayed.
Conclusion
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/G.R./Examiner, Art Unit 1725
/NICOLE M. BUIE-HATCHER/ Supervisory Patent Examiner, Art Unit 1725
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