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 .
Summary
This is an initial Office Action in response to application 18/193,976 filed March 31, 2023. Claims 1-20 are currently pending.
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(b):
(b) CONCLUSION.—The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the inventor or a joint inventor regards as the invention.
The following is a quotation of 35 U.S.C. 112 (pre-AIA ), second paragraph:
The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the applicant regards as his invention.
Claims 7 and 20 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.
Claims 7 and 20 recite “wherein content of the cyclic ether corresponding to 1 gram of silicon in the negative active material layer is 0.003 gram to 0.3 gram.” The limitation is unclear in light of the specification with respect to defining the relationship between a content of the cyclic ether and 1 gram of silicon in the negative active material layer. If the language of the claim is such that a person of ordinary skill in the art could not interpret the metes and bounds of the claim so as to understand how to avoid infringement, a rejection of the claim under 35 U.S.C. 112(b) is appropriate. To advance prosecution, the limitation will be interpreted as “wherein there is 0.003 g to 0.3 g of cyclic ether per 1 g of silicon in the negative active material layer.”
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.
This application currently names joint inventors. In considering patentability of the claims the examiner presumes that the subject matter of the various claims was commonly owned as of the effective filing date of the claimed invention(s) absent any evidence to the contrary. Applicant is advised of the obligation under 37 CFR 1.56 to point out the inventor and effective filing dates of each claim that was not commonly owned as of the effective filing date of the later invention in order for the examiner to consider the applicability of 35 U.S.C. 102(b)(2)(C) for any potential 35 U.S.C. 102(a)(2) prior art against the later invention.
Claims 1-12, 14-20 are rejected under 35 U.S.C. 103 as being unpatentable over Yoshikawa et al (JP 2017097995 A, published 2017-06-01) in view of Jeon et al (KR 101711985 B1, published 2017-03-06).
Support is provided by evidentiary references “Ethylene carbonate” ChemSpider, 2026; and “Diethyl carbonate” ChemSpider, 2026.
Regarding claim 1, Yoshikawa teaches an electrochemical device, comprising: a positive electrode, a negative electrode, a separator, and an electrolytic solution (machine translation [0010]); wherein
The negative electrode comprises a negative active material layer ([0068] teaches the negative electrode comprises a negative electrode active material), the negative active material layer comprises a silicon material ([0069] teaches Si and alloys and oxides thereof as examples of negative electrode active material; [0079] specifically discusses SiOx as being a suitable negative electrode active material); and a unit reaction area of the negative active material layer is C m2/cm2 (the negative active material layer participates in electrochemical reactions, therefore, inherently, the negative active material layer will have a unit reaction area as designated as C m2/cm2)
The electrolytic solution comprises fluorocarbonate and cyclic ether ([0175] teaches Examples 2-13, which uses 1,3-dioxane as in Example 1 ([0167]), which is a cyclic ether, and also use of the fluorocarbonate 4-fluoro-1,3-dioxolan-2-one (FEC)).
Yoshikawa does not provide a unit reaction area for the negative active material including the negative active material and additives, as defined by the instant spec [0049]. However, Yoshikawa further teaches the amount of fluorine-substituted cyclic carbonate (A), such as fluorocarbonate 4-fluoro-1,3-dioxolan-2-one (FEC), is preferably 0.3 wt% or more and 3 wt% or less in the electrolyte ([0127]). Yoshikawa also teaches the amount of the cyclic ether 1,3-dioxane (B) in the electrolyte is preferably 0.1 wt% or more and preferably 2% or less ([0135]). Yoshikawa also teaches that the density of the negative electrode active material layer is 1.56 g/cm3 and that the thickness of the layer can be 10-100 µm per surface of the current collector ([0109]), which would be 20-200 µm cumulative thickness, and the product of the two quantities results in a calculated range of weight per unit area (g/cm2) of about 0.00312 to 0.0312 g/cm2.
In the same field of endeavor, Jeon teaches the negative electrode active material comprising of similar SiOx composite active materials may have a specific surface area of 7 to 11.5 m2/g for the advantage of excellent cycle life characteristics of the lithium secondary battery (machine translation: p5 para 1). A skilled artisan would have found it obvious to utilize a specific surface area of 7-11.5 m2/g because Jeon teaches it is a suitable option that results in advantages such as excellent cycle life characteristics of the lithium secondary battery. The unit reaction area is the product of the weight per unit area and the specific surface area; therefore, the combination of prior art teaches the unit reaction area can range between 0.022 m2/cm2 and 0.36 m2/cm2.
Yoshida provides the range of A% (fluorocarbonate FEC) as 0.3 wt% - 3 wt % ([0127]) and the range of B% (cyclic ether 1,3-dioxane) as 0.1 wt% - 2 wt% ([0135]), therefore the combination of prior art teaches the range of (A+B)/C of 0.4/0.36 and 5/0.022 or 1.1 to 227, which overlaps with the claimed range. Overlapping ranges provide a prima facie case of obviousness; see MPEP 2144.05, I.
Regarding claim 14, Yoshikawa teaches an electronic device ([0002] discloses use of electrochemical devices such as lithium-ion secondary batteries as power sources for smartphones and automotives), comprising: an electrochemical device, comprising: a positive electrode, a negative electrode, a separator, and an electrolytic solution (machine translation [0010]); wherein
The negative electrode comprises a negative active material layer ([0068] teaches the negative electrode comprises a negative electrode active material), the negative active material layer comprises a silicon material ([0069] teaches Si and alloys and oxides thereof as examples of negative electrode active material; [0079] specifically discusses SiOx as being a suitable negative electrode active material); and a unit reaction area of the negative active material layer is C m2/cm2 (the negative active material layer participates in electrochemical reactions, therefore, inherently, the negative active material layer will have a unit reaction area as designated as C m2/cm2)
The electrolytic solution comprises fluorocarbonate and cyclic ether ([0175] teaches Examples 2-13, which uses 1,3-dioxane as in Example 1 ([0167]), which is a cyclic ether, and also uses fluorocarbonate 4-fluoro-1,3-dioxolan-2-one (FEC)).
Yoshikawa does not provide a unit reaction area for the negative active material including the negative active material and additives, as defined by the instant spec [0049]. However, Yoshikawa further teaches the amount of fluorine-substituted cyclic carbonate (A), such as fluorocarbonate 4-fluoro-1,3-dioxolan-2-one (FEC), is preferably 0.3 wt% or more and 3 wt% or less in the electrolyte ([0127]). Yoshikawa also teaches the amount of the cyclic ether 1,3-dioxane (B) in the electrolyte is preferably 0.1 wt% or more and preferably 2% or less ([0135]). Yoshikawa also teaches that the density of the negative electrode active material layer is 1.56 g/cm3 and that the thickness of the layer can be 10-100 µm per surface of the current collector ([0109]), which would be 20-200 µm cumulative thickness, and the product of the two quantities results in a calculated range of weight per unit area (g/cm2) of about 0.00312 to 0.0312 g/cm2.
In the same field of endeavor, Jeon teaches the negative electrode active material comprising of similar SiOx composite active materials may have a specific surface area of 7 to 11.5 m2/g for the advantage of excellent cycle life characteristics of the lithium secondary battery (machine translation: p5 para 1). A skilled artisan would have found it obvious to utilize a specific surface area of 7-11.5 m2/g because Jeon teaches it is a suitable option that results in advantages such as excellent cycle life characteristics of the lithium secondary battery. The unit reaction area is the product of the weight per unit area and the specific surface area; therefore, the combination of prior art teaches the unit reaction area can range between 0.022 m2/cm2 and 0.36 m2/cm2.
Yoshida provides the range of A% (fluorocarbonate FEC) as 0.3 wt% - 3 wt % ([0127]) and the range of B% (cyclic ether 1,3-dioxane) as 0.1 wt% - 2 wt% ([0135]), therefore the combination of prior art teaches the range of (A+B)/C of 0.4/0.36 and 5/0.022 or 1.1 to 227, which overlaps with the claimed range. Overlapping ranges provide a prima facie case of obviousness; see MPEP 2144.05, I.
Regarding claims 2 and 15, Yoshikawa teaches the electrochemical device of claim 1 and the electronic device of claim 14. Yoshikawa further teaches the amount of fluorine-substituted cyclic carbonate (A), such as fluorocarbonate 4-fluoro-1,3-dioxolan-2-one (FEC), is preferably 0.3 wt% or more and 3 wt% or less in the electrolyte ([0127]). Yoshikawa also teaches the amount of the cyclic ether 1,3-dioxane (B) in the electrolyte is preferably 0.1 wt% or more and preferably 2% or less ([0135]). Yoshikawa also provides specific examples of mass percentages of FEC (A) and 1,3-dioxane (B) used that are within the claimed range (Example 2: (A, B): 1%, 1.4%; Example 6: (A,B ): 1%, 1.5%). Therefore, Yoshikawa teaches an overlapping range with the claimed range of A% and an overlapping range with the claimed range of B%. Overlapping ranges provide a prima facie case of obviousness; see MPEP 2144.05, I.
Regarding claims 3 and 16, Yoshikawa teaches the electrochemical device of claim 1 and the electronic device of claim 14. Yoshikawa further teaches the amount of fluorine-substituted cyclic carbonate (A), such as fluorocarbonate 4-fluoro-1,3-dioxolan-2-one (FEC), is preferably 0.3 wt% or more and 3 wt% or less in the electrolyte ([0127]). Yoshikawa also teaches the amount of the cyclic ether 1,3-dioxane (B) in the electrolyte is preferably 0.1 wt% or more and preferably 2% or less ([0135]). Yoshikawa also provides specific examples of mass percentages of FEC (A) and 1,3-dioxane (B) used that are within the claimed range (Example 2: (A, B): 1%, 1.4%; Example 6: (A,B): 1%, 1.5%) Accordingly, the range of B/A is 0.03 to 7, which overlaps with the claimed range. Overlapping ranges provide a prima facie case of obviousness; see MPEP 2144.05, I.
Regarding claims 4 and 17, Yoshikawa teaches the electrochemical device of claim 1 and the electronic device of claim 14. Yoshikawa further teaches the cyclic ether can be 1,3-dioxane, which is a compound represented by Formula I.
Regarding claims 5 and 18, Yoshikawa teaches the electrochemical device of claim 4 and the electronic device of claim 17. Yoshikawa further teaches the cyclic ether can be 1,3-dioxane, which corresponds to the following claimed structure:
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Regarding claims 6 and 19, Yoshikawa teaches the electrochemical device of claim 1 and the electronic device of claim 14. Yoshikawa further teaches the fluorocarbonate can be 4-fluoro-1,3-dioxolan-2-one, which is a synonym for fluoroethylene carbonate.
Regarding claims 7 and 20, Yoshikawa teaches the electrochemical device of claim 1 and the electronic device of claim 14.
Yoshikawa discloses that the 1,3-dioxane contained in the non-aqueous electrolyte forms a coating on the surface of the negative electrode ([0134]) and also discloses the dimensions of the battery case and the electrodes, and the compositions of the negative electrode active material layer. Thus, a skilled artisan would be able to assess the claimed content of the cyclic ether corresponding to 1 gram of silicon in the negative active material.
Velectrolyte = Vcase -Vanode-Vcathode-Vseparator (The volume of the liquid electrolyte fills the space of the battery case that is not occupied by the anode, cathode, and separator, based on [0168]-[0169].)
Velectrolyte = (15.7 cm3) – (6.7 cm3) – (4.7 cm3) – (0.39 cm3) = 3.9 cm3
(See Yoshikawa: [0165]-[0166], [0168], [0109]; electrode thickness includes current collector)
A mass of 1,3-dioxane added can be calculated based on Yoshikawa’s example in [0167] disclosing an electrolyte solvent ratio of 3:7 EC to DEC, and the composition of the electrolyte including 1 wt% 1,3-dioxane (cyclic ether), such that the mass of 1,3-dioxane added to the electrolyte can be calculated:
m1,3D = Velectrolyte (3.9 cm3) x (0.3 x ρEC + 0.7 x ρDEC) x 1 wt% of 1,3-dioxane) = 0.039 g
(density of ethylene carbonate ρEC is 1.321 g/ml (ChemSpider: ethylene carbonate) and the density of diethyl carbonate ρDEC is 0.975 g/ml (ChemSpider: diethyl carbonate))
A mass of silicon in the negative active material layer can be calculated based on wherein the fraction of SiO composite in the negative electrode layer is 2.35 % based on 98% active material within the negative electrode layer, 3% SiO/C within the active material, 20% C in the SiO/C (Yoshikawa: [0166], [0185]), the wt% fraction of Si in SiO (about 28/44 or 0.64%), and the dimensions of the negative electrode (Yoshikawa: [0109] discloses wherein the negative electrode can have a thickness 100 µm, and [0166] for negative electrode length and width and density))
mSi = (wt % active material in anode layer) x (wt % SiO/C in active material) x (wt% SiO in SiO/C composite) x (wt% Si in SiO) x (Vanode x ρanode)
mSi = (98% x 3% x 80%) x (28/44) x (6.53 cm3 x 1.56 g/cm3) = 0.153 g
The mass of cyclic ether added to the electrolyte relative to the mass of silicon in the negative active material layer is thus (0.039/0.153) g cyclic ether in electrolyte/g Si in the negative active material layer, or about 0.3, which is within the claimed range. Alternatively, at least some amount of cyclic ether forms a coating on the surface of the negative electrode ([0134]), therefore the mass of the cyclic ether in the negative active material layer corresponding to 1 gram of silicon in the negative active material layer will be less than or equal to 0.3, which also overlaps with the claimed range. Overlapping ranges provide a prima facie case of obviousness; see MPEP 2144.05, I.
Regarding claim 8, Yoshikawa teaches the electrochemical device of claim 1. Yoshikawa further teaches it is preferable that silicon material is a composite with a carbon material wherein the surface of SiOx (silicon composite substrate) is coated with a carbon material (a protection layer) ([0081]-[0082]), thereby further teaching the silicon material comprises a silicon composite substrate and a protection layer and the protection layer is disposed on at least a part of a surface of the silicon composite substrate.
Regarding claim 9, Yoshikawa teaches the electrochemical device of claim 8. Yoshikawa teaches the protection layer comprises carbon ([0081]-[0082]).
Regarding claim 10, Yoshikawa teaches the electrochemical device of claim 8. Yoshikawa further teaches wherein the silicon composite substrate comprises silicon oxide or silicon ([0080]).
Regarding claim 11, Yoshikawa teaches the electrochemical device of claim 8. Yoshikawa further teaches the silicon composite substrate comprises SiOx with x satisfying 0.5≦x≦1.5, which overlaps with the claimed range for the subscript on oxygen. Overlapping ranges provide a prima facie case of obviousness; see MPEP 2144.05, I.
Regarding claim 12, Yoshikawa teaches the electrochemical device of claim 8. Yoshikawa does not expressly claim a thickness of the protection layer is 1 nm to 900 nm. However, Yoshikawa teaches the carbon coating (i.e., protection layer) improves conductivity of the silicon material particles and contributes to a better conductive network in the negative electrode that results in a battery with higher capacity and charge-discharge cycle characteristics ([0083], [0095]). A skilled artisan would have understood that the amount of carbon coating present would impact its conductivity, and that the thickness of the carbon coating would thus be a result-effective variable. Consequently, they would have been motivated to adjust the thickness of the carbon coating to optimize its conductivity within the negative electrode and would have arrived at the claimed thickness of the protection layer.
Claim 13 is rejected under 35 U.S.C. 103 as being unpatentable over Yoshikawa et al (JP 2017097995 A) in view of Jeon et al (KR 101711985 B1) as applied to claim 1 above, and further in view of Ogata et al (US 20170077497 A1).
Regarding claim 13, Yoshikawa teaches the electrochemical device of claim 1, and Yoshikawa further teaches negative active material layer comprises carbon nanotubes ([0085]). However, Yoshikawa does not teach their diameter or length.
In the same field of endeavor, Ogata teaches particles of silicon composite active material that can have carbon nanotubes disposed on them ([0087], [0089], Fig. 2D), wherein the carbon nanotubes may have an average tube diameter of 5 nm to about 20 nm and a length of about 5 µm to about 30 µm. Ogata further teaches that within the taught diameter size range, the carbon nanotube may provide a sufficient mechanical strength, and that within the taught length size range, the carbon nanotube facilitates electron charge transfer into the particles of the silicon composite active material ([0090]). A skilled artisan would have found it obvious to modify the carbon nanotubes within Yoshikawa’s negative active material layer to utilize the dimensions taught by Ogata for sufficient mechanical strength of the material and also to facilitate electron charge transfer into the particles of the silicon material within the negative active material layer. Ogata’s taught ranges for the diameter of the carbon nanotubes and the length of the carbon nanotubes overlaps with the claimed ranges. Overlapping ranges provide a prima facie case of obviousness; see MPEP 2144.05, I.
Conclusion
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/G.L.L./Examiner, Art Unit 1726
/JEFFREY T BARTON/Supervisory Patent Examiner, Art Unit 1726 2 February 2026