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 .
Information Disclosure Statement
The information disclosure statements filed June 13, 2023; August 9, 2024 (two filings) and November 25, 2024 have been placed in the application file and the information referred to therein has been considered as to the merits.
With respect to foreign language references with no translation of the document: “If no translation is submitted, the examiner will consider the information in view of the concise explanation and insofar as it is understood on its face, e.g., drawings, chemical formulas, English language abstracts, in the same manner that non-English language information in Office search files is considered by examiner in conducting searches.” See MPEP §609.04(a)(II) (D) and 37 CFR 1.98(a)(3)(ii).
Drawings
The drawings received June 13, 2023 are acceptable for examination purposes.
Specification
The specification received June 13, 2023 has been reviewed for examination purposes.
Claim Rejections - 35 USC § 102
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 the appropriate paragraphs of 35 U.S.C. 102 that form the basis for the rejections under this section made in this Office action:
A person shall be entitled to a patent unless –
(a)(1) the claimed invention was patented, described in a printed publication, or in public use, on sale, or otherwise available to the public before the effective filing date of the claimed invention.
Claims 1, 3-7, 9-10, 14 and 19 are rejected under 35 U.S.C. 102(a)(1) as being anticipated by Chiga et al. (U.S. Patent Application Publication No. 2007/0287071).
As to claim 1, Chiga discloses an electrolyte solution, containing a solvent, an additive and a lithium salt, 1 wherein the solvent (such AS A3 in Table 5) comprises
a first solvent and a second solvent,
the first solvent being a cyclic ester solvent (EC, ethylene carbonate, in A3, Table 5),
the second solvent being a linear carboxylic ester solvent (MA, methyl acetate, in A3, Table 5),
the additive comprises a film forming additive (FEC, fluoroethylene carbonate in A3, Table 5), and
based on the total mass of the electrolyte solution, the lithium salt has a mass fraction of W1, the film forming additive has a mass fraction of W2, and the second solvent has a mass fraction of W3, which satisfy the following relationship: 0.2 ≤ (W1 + W2)/W3 ≤ 0.4.
Notably, the electrolyte of Chiga is 1M LiPF₆, 10/80/10 EC/MA/FEC. The amounts are calculated based on 1.0 mole of LiPF₆ dissolved in 1000 mL of solvent mixture (10/80/10 EC/MA/FEC).
A 1M solution of LiPF₆ means 1 mole of LiPF₆ (151.9g/mol). Therefore W1 is 151.9g.
The density of EC is 1.321g/mL. The density of MA is 0.934g/mL. The density of vinylene carbonate is 1.485g/mL.
To determine the overall density, the mass of 1 liter (1000m) of the solvent mixture first.
Volume of EC: VEC=0.10×1000mL=100mL
Volume of MA: VMA=0.80×1000mL=800mL
Volume of FEC: VFEC=0.10×1000mL=100mL
Mass of each component:
m=ρ×V
Mass of EC: mEC=1.321g/mL×100mL=132.1g
Mass of MA: mMA=0.934g/mL×800mL=747.2g
Mass of FEC: mVC=1.485g/mL×100mL=148.5g
Total mass of 1 L solvent mixture:
msolvent=132.1g+747.2g+148.5g=1027.8g
In a 1L of 1M LiPF₆ in EC/MA/FEC (10/80/10 vol% ratio), the mass of each above is:
W1 - LiPF6 (151.9g)
W2 – FEC additive (148.5g)
W3 – MA solvent (747.2g)
(W1+W2)/W3 is (151.9g+148.5g)/747.2g = 300.4/747.2 = 0.4
Therefore, the mass fraction of lithium salt, film forming additive and second solvent (linear carboxylic ester solvent) is 0.4 which falls within the range of claim 1.
As to claim 3, the cyclic ester solvent is ethylene carbonate in example A3, Table 5.
As to claim 4, the linear carboxylic ester solvent is methyl acrylate in example A3, Table 5.
As to claim 5, the film forming additive is fluoroethylene carbonate in example A3, Table 5.
As to claim 6, the lithium salt is LiPF6 in example A3, Table 5.
As to claim 7, Total mass of 1 L solvent mixture:
msolvent=132.1g+747.2g+148.5g=1027.8g. The mass of LiPF₆ in 1M of this solution is 151.9. The total mass of the solution is 1179.7g and the mass% of LiPF₆ (151.9) based on the total mass of 1179.7g is 12.9%.
As to claim 9, Total mass of 1 L solvent mixture:
msolvent=132.1g+747.2g+148.5g=1027.8g. The mass of LiPF₆ in 1M of this solution is 151.9. The total mass of the solution is 1179.7g and the mass% of methyl acetate (747.2g) based on the total mass of 1179.7g is 63.3%.
As to claim 10, Total mass of 1 L solvent mixture:
msolvent=132.1g+747.2g+135.5g=1027.8g. The mass of LiPF₆ in 1M of this solution is 151.9. The total mass of the solution is 1179.5g and the mass% of ethylene carbonate (132.1g) based on the total mass of 1179.7g is 11.2%.
As to claims 14 and 19, the electrolyte above is employed in a secondary battery (title, examples) and further in a power consuming electronic device (para. [0004]).
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 nonobviousness.
Claims 2 and 8 are rejected under 35 U.S.C. 103 as being unpatentable over Chiga et al. (U.S. Patent Application Publication No. 2007/0287071) as applied to claim 1 above.
As to claim 2, the example in Chiga noted above satisfies the relationship of t0 be 0.4.
As to claim 8, Total mass of 1 L solvent mixture:
msolvent=132.1g+747.2g+148.5g=1027.8g. The mass of LiPF₆ in 1M of this solution is 151.9. The total mass of the solution is 1179.7g and the mass% of fluoroethylene carbonate (148.5g) based on the total mass of 1179.7g is 12.6%.
Chiga does not teach of a value in the range of claim 2, noting that Chiga does teach of the relationship satisfying the equation of claim 1 at 0.40 which is within the inventive range but narrower range of claim 2. Similarly Chiga discloses that the mass% of fluoroethylene carbonate is 12.6% which is slightly outside of the range of claim 8 of 1-10%.
As discussed above, Example A3 of Chiga satisfies the relationship of claim 1 (0.4; near the range of claim 2) and teaches of a mass of the film forming additive to be 12.6% (claim 8). All of these fall at or near the inventive amounts while satisfying the base relationship of claim 1. The differences in ranges are held to be minor and obvious differences further noting that there is no evidence of criticality to the particular percentages of claims 2 and 8 to the inventive range.
Furthermore as to claim 2, it is noted that Chiga teaches that the amount of FEC can be as low as 7% volume or more to obtain desirable discharge load characteristics (para. [0126]). This would lower the threshold mass for FEC to be as low as 103.95g (7% in a 1M LiPF6 electrolyte of the mixture noted above, determining ratios based on a 1L solution).
Notably, the electrolyte of Chiga is 1M LiPF₆, 10/83/7 EC/MA/FEC or 13/80/7 EC/MA/FEC (using the lowest amount of FEC taught above, 7%). The amounts are calculated based on 1.0 mole of LiPF₆ dissolved in 1000 mL of solvent mixture (10/83/7 EC/MA/FEC or 13/80/7 EC/MA/FEC).
A 1M solution of LiPF₆ means 1 mole of LiPF₆ (151.9g/mol). Therefore W1 is 151.9g.
The density of EC is 1.321g/mL. The density of MA is 0.934g/mL. The density of vinylene carbonate is 1.485g/mL.
To determine the overall density, the mass of 1 liter (1000m) of the solvent mixture first. 10/83/7 EC/MA/FEC
Volume of EC: VEC=0.10×1000mL=100mL
Volume of MA: VMA=0.83×1000mL=830mL
Volume of FEC: VFEC=0.07×1000mL=70mL
Mass of each component:
m=ρ×V
Mass of EC: mEC=1.321g/mL×100mL=132.1g
Mass of MA: mMA=0.934g/mL×830mL=775.2g
Mass of FEC: mVC=1.485g/mL×70mL=104.0g
Total mass of 1 L solvent mixture:
msolvent=132.1g+775.2g+104.0g=1011.3g
In a 1L of 1M LiPF₆ in EC/MA/FEC (10/83/7 vol% ratio), the mass of each above is:
W1 - LiPF6 (151.9g)
W2 – FEC additive (104g)
W3 – MA solvent (775.2g)
(W1+W2)/W3 is (151.9g+104g)/775.2g = 255.9/775.2 = 0.33
To determine the overall density, the mass of 1 liter (1000m) of the solvent mixture first. 13/80/7 EC/MA/FEC
Volume of EC: VEC=0.13×1000mL=130mL
Volume of MA: VMA=0.80×1000mL=800mL
Volume of FEC: VFEC=0.07×1000mL=70mL
Mass of each component:
m=ρ×V
Mass of EC: mEC=1.321g/mL×130mL=171.7g
Mass of MA: mMA=0.934g/mL×800mL=747.2g
Mass of FEC: mVC=1.485g/mL×70mL=104.0g
Total mass of 1 L solvent mixture:
msolvent=171.7g+747.2g+104.0g=1022.9g
In a 1L of 1M LiPF₆ in EC/MA/FEC (13/80/7 vol% ratio), the mass of each above is:
W1 - LiPF6 (151.9g)
W2 – FEC additive (104.0g)
W3 – MA solvent (747.2g)
(W1+W2)/W3 is (151.9g+104g)/747.2g = 255.9/747.2 = 0.34
As to claim 8, Total mass of 1 L solvent mixture for modified amount of FEC at 7%:
For EC/MA/FEC - 10/83/7
msolvent=132.1g+775.2g+104g=1011.3g. The mass of LiPF₆ in 1M of this solution is 151.9. The total mass of the solution is 1163.2g and the mass% of fluoroethylene carbonate (104g) based on the total mass of 1163.2g is 8.9%.
For EC/MA/FEC - 13/80/7
msolvent=171.7g+747.2g+104g=1022.9g. The mass of LiPF₆ in 1M of this solution is 151.9. The total mass of the solution is 1174.8g and the mass% of fluoroethylene carbonate (104g) based on the total mass of 1174.8g is 8.8%.
Therefore, the mass fraction of lithium salt, film forming additive and second solvent (linear carboxylic ester solvent) of Example A3, Table 5, is 0.4 which falls within the range of claim 1. Given the broader teachings of Chiga, FEC can be as low as 7% effectively and applying a slightly lower amount of FEC to Example A3 would have been of routine skill in the art while still achieving the desired effects of FEC. In modifying the amount of FEC accordingly, the modified electrolyte solution would obviously satisfy the relationship of claim 2 as noted above to be as low as 0.33-0.34 and amounts of FEC as low as 8.8-8.9% mass.
Therefore it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to encompass minor differences to the relationship of claim 2 and percentage of film forming additive of claim 8 as Chiga teaches of the same or similar amounts as noted above and further obviates the use of 7% FEC as discussed above. Upon modifying any example, including example A3 used above to have 7% FEC as taught by Chiga as a sufficient amount for performance purposes, the resultant modification would have obviated satisfying the narrower range of claim 2 and % mass of claim 8, the differences in percentages are held to be minor and obvious differences, absent clear evidence to the contrary. Generally, differences in ranges will not support the patentability of subject matter encompassed by the prior art unless there is evidence indicating such ranges is critical. In re Boesch, 617 F.2d 272, 205 USPQ 215 (CCPA 1980). In re Aller, 220 F.2d 454, 456, 105 USPQ 233, 235 (CCPA 1955). In re Hoeschele, 406 F.2d 1403, 160 USPQ 809 (CCPA 1969). It has been held that when the difference between a claimed invention and the prior art is the range or value of a particular variable, then a prima facie rejection is properly established when the difference in the range or value is minor. Titanium Metals Corp. of Am. v. Banner, 778 F.2d 775, 783, 227 USPQ 773, 779 (Fed. Cir. 1985).
Claims 11-13 are rejected under 35 U.S.C. 103 as being unpatentable over Chiga et al. (U.S. Patent Application Publication No. 2007/0287071) as applied to claim 1 above and further in view of Zhang et al (CN 107749466A).
Chiga does not teach of the electrolyte further including a water removal additive as in claim 11, more particularly at least one of the specific materials recited in claim 12, in an amount of 0.5% or less as in claim 13.
Zhang teaches of adding a minor amount of hexamethyldisilazane (abstract, examples, applied to claims 11 and 12) for the benefit reducing water formation in a non-aqueous secondary battery. The amount of additive is minor amount ranging from 0.2 to 0.4% (claim 13).
Therefore 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 electrolyte of Chiga to further include 0.2-0.4% hexamethyldisilazane as taught by Zhang since it would have predictably provided an additive for preventing/reducing water formation in the battery.
Claims 15 and 17-18 are rejected under 35 U.S.C. 103 as being unpatentable over Chiga et al. (U.S. Patent Application Publication No. 2007/0287071) as applied to claim 1 above and further in view of Shirakata et al. (U.S. Patent Application Publication No. 2006/0216605) and Du et al (U.S. Patent Application Publication No. 2018/0315992).
As to claim 15, Chiga teaches of the positive electrode plate comprising a substrate and electrode film layer. The electrode film layer comprising an active material such as LiCoO2 (para. [0051], for example).
Chiga does not teach of the positive electrode film layer comprising a lithium containing phosphate of an olivine structure (claim 15) where the thickness of the film on one side is 80-140 microns (claim 17), where the porosity of the film is 20-50% (claim 18).
Shirakata teaches that secondary batteries employing an olivine-type lithium metal phosphate active material as a low-cost material compared to other conventional materials such as LiCoO2 (para. [0003]). Du teaches of manufacturing thicker electrodes including LiCoO2 and LiFePO4 (lithium containing phosphate of an olivine structure, claim 15). The electrode has a porosity of 20-40% and an overlapping thickness as low as 100 microns or more (para. [0019], claims 17-18). Du recognized that electrode thickness and porosity are important to battery performance and selected based on battery application (para. [0005]).
Therefore 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 material, thickness and porosity of the positive electrode active material to be an olivine-type lithium metal phosphate active material as taught by Shirakata and Du having a thickness of at least 100 microns and a porosity of 20-40% since it would have provided a conventionally recognized active material, LiFePO4, having excellent electrochemical performance at low-cost and provided electrode parameters, thickness and porosity of sufficient amounts to provide a robust mechanical and electrochemical positive electrode active material layer. The selection of a known material based on its suitability for its intended use supported a prima facie obviousness determination in Sinclair & Carroll Co. v. Interchemical Corp., 325 U.S. 327, 65 USPQ 297 (1945) See also In re Leshin, 227 F.2d 197, 125 USPQ 416 (CCPA 1960). MPEP § 2144.07. Generally, differences in ranges will not support the patentability of subject matter encompassed by the prior art unless there is evidence indicating such ranges is critical. In re Boesch, 617 F.2d 272, 205 USPQ 215 (CCPA 1980). In re Aller, 220 F.2d 454, 456, 105 USPQ 233, 235 (CCPA 1955). In re Hoeschele, 406 F.2d 1403, 160 USPQ 809 (CCPA 1969).
Allowable Subject Matter
Claim 16 is objected to as being dependent upon a rejected base claim, but would be allowable if rewritten in independent form including all of the limitations of the base claim and any intervening claims.
The following is a statement of reasons for the indication of allowable subject matter: none of the cited prior art of record, alone or in combination are held to reasonably teach, suggest or render obvious the secondary battery of claim 16, including all of the limitations of the base claim and any intervening claims, wherein the battery further satisfies the relationship of claim 16.
While Chiga satisfies the relationship of claim 1, Chiga itself does not teach or suggest satisfying this relationship in combination with the positive electrode film layer active material comprising a lithium-containing phosphate of an olivine structure which further satisfies the relationship of claim 16 which includes the second relationship and it would not appear to be obvious to one of ordinary skill in the art to satisfy this second relationship with sufficient specificity to appreciate the need to satisfy the two relationships in combination. While the secondary references above obviate certain features of an olivine-type lithium metal phosphate active material, there is no reasonably teaching or suggestion from the combination above to effectively satisfy the relationships together (relationship of claim 1 in combination with the relationship of claim 16).
Conclusion
The prior art made of record and not relied upon is considered pertinent to applicant's disclosure. U.S. Patent No. 5,744,262 discloses an electrolyte comprising EC/EA/LiClO4/1/1/1M (Table 3 for example). U.S. Patent No. 6,235,431 discloses hexamethyldisilizane water scavenger for nonaqueous electrolytes.
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/GREGG CANTELMO/Primary Examiner, Art Unit 1725