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 .
Response to Amendment
The amendment filed May 15, 2026 has been entered but does not place the application in condition for allowance. The addition of new claims 21-22 are respectfully acknowledged. Claims 1-6, 8-11, 13-22 are currently pending, with 14-17 withdrawn.
New rejections follow.
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 text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
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 1-6, 8-11, 13, 18-21 are rejected under 35 U.S.C. 103 as being unpatentable over Kim et al (US 20200280060 A1) in view of Ryu et al (US 20160141608 A1), Behan et al (US 20170271651 A1), and Williams et al (WO 2018165427 A1).
Regarding Claim 1, Kim teaches (Fig. 1A) a negative active material composite for a rechargeable lithium battery ([0008]-[0009]), the lithium active material composite comprising silicon nanoparticles 11 and amorphous carbon (Abstract; [0046]-[0047]). Kim also teaches that the silicon nanoparticles can have an average particle diameter of about 50 nm to 150 nm ([0012]), which overlaps with the claimed ranges. Kim does not teach compound particles represented by SiOx particles within the negative active material composite or their average particle diameter. Kim is silent regarding wherein a maximum particle diameter (Dmax) of the compound particles is about 5 µm to about 20 µm. Kim is also silent regarding wherein the composite includes the compound particles and the silicon nanoparticles in a weight ratio of about 8:2 to about 2:8.
Ryu teaches (Fig. 1) a negative active material composite with a non-carbonaceous core (100) ([0043]) wherein the non-carbonaceous core may be Si-based particle such as Si, SiOx (0<x<2) which may be used alone or at least two thereof ([0032]), thereby teaching that SiOx particles can be included with silicon within a negative active material composite, which would read on the claimed compound particles represented by SiOx with x within the claimed range. Ryu further teaches that silicon oxide may be used as a Si-based particle because of advantages of reducing expansion rates during charging and discharging ([0032]), which Ryu has noted as a problem with silicon (Si) when charging and discharging, and which can result in capacity retention rate, charge/discharge efficiency deterioration or lead to detachment of the negative electrode ([0094], [0028]). Given that primary reference Kim has also mentioned reducing expansion of the silicon nanoparticles as improving the initial efficiency and/or cycle-life characteristics of the battery (Kim: [0092]), it would have been obvious to one of ordinary skill in the art to have modified the negative active material composite of Kim to incorporate the silicon oxide particles taught by Ryu to obtain the benefits from reduced volume expansion of the negative active material and consequently improving the capacity retention rate, and charge/discharge efficiency deterioration over cycles.
In the same field of endeavor, Williams teaches the active electrode material containing (e.g., silicon-containing) particles such as silicon and/or silicon oxide wherein they have an average dimension, which can be a diameter, of about 10 nm or more and to about 5 micron ([098]). Williams also teaches the particles can have an average largest dimension of about 0.1 micron to about 10 micron [008], wherein the average largest dimension corresponds to the claimed maximum particle diameter, i.e. Dmax, and overlap with the claimed range. In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. 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). Williams further teaches particles provided have a targeted size that provides good performance characteristics (e.g., good 1st cycle coulombic efficiency and good capacity retention) [008]. A skilled artisan would have found it obvious to have modified the modified negative active material composite of Kim to have the targeted size of the compound particles, including the average particle diameter D50 and the Dmax of compound particles represented by SiOx, as taught by Williams, to derive the benefits of good performance characteristics (e.g., good 1st cycle coulombic efficiency and good capacity retention).
In the same field of endeavor, Behan teaches the ratio of silicon to SiOx within a silicon core is critical to the stability of the material when undergoing multiple volume expansions, such as when used as an anode material in a lithium battery and discloses the preferred ratio of silicon:SiOx can be from about 1:1 to about 40:1 ([0057]). Behan’s teaching is relevant to the negative active material composite taught by modified Kim, because both Behan and Kim in view of Ryu provide core-like structure formed of silicon and SiOx regions (Behan: [0049]; Kim: Fig. 1 and [0047]; Ryu: [0032]) that would be exposed to similar silicon expansion issues during operation of the battery. Additionally, considering primary reference Kim’s disclosure that reducing expansion of the silicon nanoparticles improves the initial efficiency and/or cycle-life characteristics of the battery (Kim: [0092]), it would have been obvious to a skilled artisan to modify the modified negative active material composite of Kim with the silicon:SiOx ratio taught by Behan to improve the stability of the anode material when undergoing multiple volume expansions.
The taught ratio of silicon: SiOx of about 1:1 to about 40:1 corresponds to a ratio of about 1:40 to about 1:1 of compound particle SiOx to silicon. This overlaps with the claimed ratio regardless of whether it directly corresponds to a weight ratio or a molar ratio. For example, in the latter case, if SiOx is SiO1.5 and given the molar masses of Si (28.09 g/mol) and of SiO1.5 (52.09 g/mol), then the weight ratio corresponding to a molar ratio of about 1:40 to about 1:1 would be about 0.05 to 1.9, which overlaps with the claimed range of about 2:8 to about 8:2. A similar calculation can be performed for x=2; that is, SiO2 (60.09 g/mol) derives a weight ratio of 0.05 to 2.1, and which also overlaps with the claimed range. It would be obvious to one of ordinary skill in the art that within the taught SiOx composition, the taught ratio of silicon: SiOx would include compositions that overlap with the claimed range. In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. 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).
Kim further teaches (Fig. 1A) the structure of the negative active material composite as a coating layer of amorphous carbon (5) surrounding a core of silicon nanoparticles (11) and amorphous carbon ([0046]-[0047]), wherein the core would provide the matrix. Within the combination, the compound particles taught by Ryu would be in the matrix, thereby teaching the claimed limitation.
Regarding Claim 2, the combination above teaches the negative active material composite of claim 1, and Kim further teaches the silicon nanoparticles can have an average particle diameter of about 50 nm to 150 nm ([0012]), which is within the claimed range.
Regarding Claim 3, the combination above teaches the negative active material composite of claim 1, and Kim further teaches the aspect ratio of the silicon nanoparticles is about 2 to 8 ([0014]), which overlaps with the claimed range.
Regarding Claim 4, the combination above teaches the negative active material composite of claim 1 and Kim further teaches a full width at half maximum of an X-ray diffraction angle using CuKα ray corresponding to a (111) plane of the silicon nanoparticles of about 0.3° to 7° ([0013], [0052]), which overlaps with the claimed range.
Regarding Claim 5, the combination above teaches the negative active material composite as claimed in claim 1, and Kim further teaches wherein an internal pore volume of the negative active material composite is less than or equal to about 3.0 x 10-2 cm3/g ([0023]).
Regarding Claim 6, the combination above teaches the negative active material composite of claim 1 and Kim further teaches the amorphous carbon may be a soft carbon, a hard carbon, a mesophase pitch carbonized product, a fired coke, or any combination thereof ([0016]).
Regarding Claim 8, the combination above teaches the negative active material composite of claim 1 but does not teach the compound particles in an amount of about 5 wt% to about 90wt%, the silicon nanoparticles in an amount of about 10 wt% to about 95 wt%, and a balance amount of the amorphous carbon wherein all wt% being based on a total weight of the negative active material composite.
Behan teaches the amount of silicon in the material composite material can be from about 20 wt % to about 97 wt %. ([0055]) of the hybrid material, and also teaches the amount of SiOx can be from about 3 wt % to about 50 wt % ([0056]) of the hybrid material, wherein the hybrid material comprises regions of silicon oxide, SiOx, where x is from 1 to 2, and regions of silicon ([0049]). Behan’s taught ranges for the compound particles and the silicon nanoparticles overlap with the claimed ranges. In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. 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). Behan further discloses in [0048] such composites are inexpensive, able to be made on commercial scales, stable over the desired cycle life, and show cycle efficiencies that are up to 250-300% higher than graphite without the stability issues of silicon, and the composite structure minimizes the volume expansion of the Si during electrochemical cycling (lithiation and de-lithiation); and it allows for control of the final specific capacity of the anode as needed by the application. One of ordinary skill in the art at the time of filing would have found it obvious to modify the negative active material composite of modified Kim to use the weight percentages of silicon and compound particles SiOx taught by Behan for the advantages of a composite structure that minimizes volume expansion of the Si during electrochemical cycling, control of the final specific capacity of the anode as required by the application, and the commercial scalability and inexpensive costs.
Additionally, because Behan teaches the ratio of silicon to SiOx is critical to the stability of the material when undergoing multiple volume expansions, such as when used as an anode material in a lithium battery and discloses the preferred ratio of silicon:SiOx can be from about 1:1 to about 40:1 ([0057]), a skilled artisan would have recognized the ratio of silicon to SiOx as a result-effective variable and would have found it obvious to alternatively use routine experimentation within the taught range of ratio to arrive at a ratio of silicon to SiOx that optimizes stability of the material under repeated cycling, and consequently, arrived at the claimed range of silicon by calculating the product of the taught range of SiOx with the ratio of silicon to SiOx.
Accounting for the compound particles SiOx and the silicon nanoparticles within the combination of the negative active material composite as a coating layer of amorphous carbon surrounding a core of silicon nanoparticles and compound particles SiOx (Kim teaches in Fig. 1A and paragraphs [0046]-[0047], Ryu teaches in [0032] the compound particles SiOx can be included in the silicon-based core), the amorphous carbon forms the balance amount of the composite as claimed.
Regarding Claim 9, the combination above teaches the negative active material composite of claim 1, and Kim further teaches an average diameter of the negative active material composite is about 2 µm to about 15 µm ([0020]), which corresponds to the claimed range.
Regarding Claim 10, the combination above teaches the negative active material composite of claim 1, and Kim further teaches the internal pore diameter of the negative active material composite is less than or equal to about 200 nm ([0022]), which is within the claimed range.
Regarding Claim 11, the combination above teaches the negative active material composite of claim 1, and Kim further teaches the BET specific surface area of the negative active material composite may be less than or equal to about 10 m2/g ([0024]).
Regarding Claim 13, the combination above teaches the negative active material composite of Claim 1. Kim discloses that the adjacent distance between silicon nanoparticles 11, which refers to a distance between centers of adjacent silicon nanoparticles, may be less than or equal to about 50 nm ([0048]). An adjacent distance of 50 nm or less would result in overlap of particles with diameters of 50 nm or greater. Because Kim teaches silicon nanoparticles of an average particle diameter of 50 nm to 150 nm ([0012]), at least some of the silicon nanoparticles would be expected to overlap and touch other silicon nanoparticles and therefore be aggregated. Kim also discloses a coating layer (5) surrounding the outer surface of the secondary particles and including the amorphous carbon ([0046]-[0047]), thereby reading on the limitations as claimed.
Regarding Claim 18, the combination above teaches the negative active material composite of claim 1 and Kim further teaches it is used in a negative active material layer on a current collector within a negative electrode for a rechargeable lithium battery ([0009], [0078]).
Regarding Claim 19, the combination above teaches the negative electrode of claim 18, and Kim further teaches the negative active material layer further includes a conductive material and a binder ([0080]), which reads on the claimed limitation.
Regarding Claim 20, the combination above teaches the negative electrode of claim 18, and Kim further teaches a rechargeable lithium battery comprises a positive electrode and an electrolyte ([0031]).
Regarding Claim 21, the combination above teaches the negative active material composite of Claim 1.
As pointed out previously, Williams teaches the active electrode material containing (e.g., silicon-containing) particles such as silicon and/or silicon oxide can have an average largest dimension, which can correspond to a diameter [098], of about 0.1 micron to about 10 micron [008], wherein the particles provided have a targeted size that provides good performance characteristics (e.g., good 1st cycle coulombic efficiency and good capacity retention) [008]. A skilled artisan would have found it obvious to have also modified the modified negative active material composite of Kim such that a maximum particle diameter (Dmax) of the silicon nanoparticles is greater than or equal to about 0.1 micron to about 10 micron as taught by Williams, to derive the benefits of good performance characteristics (e.g., good 1st cycle coulombic efficiency and good capacity retention). Consequently, the Dmax of the silicon nanoparticles of the combined prior art would overlap with the claimed range. In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. 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).
Claims 1-2 and 8-11, 13, and 21 are rejected under 35 U.S.C. 103 as being unpatentable over Behan et al (US 20170271651 A1) in view of Ryu et al (US 20160141608 A1) and Williams et al (WO 2018165427 A1).
Evidentiary support is provided by “Matrix,” Definition 3b, Merriam-Webster.
Regarding Claim 1, Behan teaches a negative active material composite for a rechargeable lithium battery (Abstract), the negative active material composite comprising a stable porous silicon (SPS) core with a coating layer, wherein the SPS comprises a silicon-silica hybrid material which comprises a combination of silicon and SiOx, wherein x is from 1-2 ([0048]-[0049]). Behan further teaches the coating layer can be made of carbon and any of the carbon precursors known in the art, including in the form of amorphous carbon ([0062]).
Behan also teaches in [0057] the ratio of silicon to SiOx is critical to the stability of the material when undergoing multiple volume expansions, such as when used as an anode material in a lithium battery and that the ratio can be from about 1:1 to about 40:1, which corresponds to 1:1 to 1:40 ratio of the compound particles SiOx to silicon. This overlaps with the claimed ratio regardless of whether it directly corresponds to a weight ratio or a molar ratio. For example, in the latter case, if SiOx is SiO1.5 and given the molar masses of Si (28.09 g/mol) and of SiO1.5 (52.09 g/mol), then the weight ratio corresponding to a molar ratio of about 1:40 to about 1:1 would be about 0.05 to 1.9, which overlaps with the claimed range of about 2:8 to about 8:2. A similar calculation can be performed for the situation wherein x=2, that is, for compound particles SiO2 (60.09 g/mol), to derive a weight ratio of 0.05 to 2.1 from a molar ratio of 1:40 to about 1:1, and which also overlaps with the claimed range. It would be obvious to one of ordinary skill in the art that within the taught SiOx composition, the taught ratio of silicon: SiOx would include compositions that overlap with the claimed range. In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. 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).
Although Behan teaches in paragraph [0011] the core material is in the form of sintered porous particles comprising subparticles comprising SiOx and crystalline silicon, Behan does not provide sufficient characterization for one of ordinary skill in the art to identify whether the subparticles are in the form of distinct compound particles of SiOx and distinct silicon nanoparticles, or if each subparticle has a hybrid composition of SiOx and silicon.
However, in the same field of endeavor, Ryu teaches (Fig. 1) a negative active material composite with a non-carbonaceous core (100) ([0043]) wherein the non-carbonaceous core may be Si-based particle such as Si, SiOx (0<x<2) which may be used alone or at least two thereof ([0032]), thereby teaching that SiOx particles can be included with silicon within a negative active material composite, which would read on distinct compound particles represented by SiOx with x within the claimed range. Ryu further teaches that silicon oxide may be used as a Si-based particle because of advantages of reducing expansion rates during charging and discharging ([0032]), which Ryu has noted as a problem with silicon (Si) when charging and discharging, and which can result in capacity retention rate, charge/discharge efficiency deterioration or lead to detachment of the negative electrode ([0094], [0028]). Seeing as primary reference Behan is also concerned with structural stabilization of silicon against multiple volume expansions ([0008]), and that Behan also provides an open-ended teaching as to how the silica-silicon core can be formed from precursors, as they disclose “The possible precursors for both the SPS and coating are numerous and inexpensive” ([0048]), it would have been obvious to one of ordinary skill in the art to have modified the negative active material composite of Behan to incorporate distinct silicon and silicon oxide particles (i.e., compound particles) as taught by Ryu given that it is a suitable configuration for obtaining the benefits from reduced volume expansion of the negative active material and consequently improving the capacity retention rate, and charge/discharge efficiency deterioration over cycles.
In the same field of endeavor, Williams teaches the active electrode material containing (e.g., silicon-containing) particles such as silicon and/or silicon oxide wherein they have an average dimension, which can be a diameter, of about 10 nm or more and to about 5 micron ([098]). Williams also teaches the particles can have an average largest dimension of about 0.1 micron to about 10 micron [008], wherein the average largest dimension corresponds to the claimed maximum particle diameter, i.e. Dmax, and overlap with the claimed range. In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. 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). Williams further teaches the particles provided have a targeted size that provides good performance characteristics (e.g., good 1st cycle coulombic efficiency and good capacity retention) [008]. A skilled artisan would have found it obvious to have modified the modified negative active material composite of Kim to have the targeted size of the compound particles, including the average particle diameter D50 and the Dmax of compound particles represented by SiOx, as taught by Williams, to derive the benefits of good performance characteristics (e.g., good 1st cycle coulombic efficiency and good capacity retention).
The term “matrix” as defined by Merriam-Webster is “a material in which something is enclosed or embedded” (Merriam-Webster: “matrix” definition 3b). As previously pointed out in addressing the limitations of claim 1, modified Behan teaches the negative active material composite as comprising a silicon-SiOx core material ([0048]-[0049]), with a coating layer adhered to at least part of the surface of the core and which can be formed of amorphous carbon ([0062]), wherein Ryu of the combination teaches the silicon and SiOx can be distinct particles (Ryu: [0032]). The silicon nanoparticles and the amorphous carbon coating correspond to the matrix, and Behan’s teaching implies the SiOx compound particles is integrally embedded in the core material and enclosed by the amorphous carbon coating. Therefore, Behan also teaches the limitation of a matrix including the silicon nanoparticles and the amorphous carbon; and the compound particles are in the matrix.
Regarding Claim 2, the combination above teaches the negative active material composite of claim 1, and as previously pointed out in addressing the limitations of claim 1, Ryu of the combination teaches that an average particle diameter of the non-carbonaceous core, which may comprise SiOx and/or Si, as in the range of about 1 nm to about 50 µm ([0015], [0032]), which overlaps with the claimed range for the silicon nanoparticles. In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. 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).
Regarding Claim 8, the combination above teaches the negative active material composite of claim 1. Behan further teaches the amount of silicon in the material composite material can be from about 20 wt % to about 97 wt %. ([0055]) of the composite material, and also teaches the amount of SiOx can be from about 3 wt % to about 50 wt % ([0056]) of the composite material. Behan’s taught ranges for the compound particles and the silicon nanoparticles overlap with the claimed ranges.
Given that Behan teaches a composite material comprising a stable porous silicon (SPS) core with a coating layer that can be amorphous carbon ([0048]-[0049], [0062]), the amorphous carbon in the coating layer would accordingly form the balance amount of the total negative active material composite as claimed.
Regarding Claim 9, the combination above teaches the negative active material composite of claim 1. Behan further teaches that of their composite material comprising a core material and a coating material coating at least part of the outer surface of the core material, the core material of the composite is in the form of particles with an average diameter along the longest axis of from about 1 μm to about 10 μm ([0011]), and further teaches the coating material has a thickness from about 1 nm to about 5 μm. The diameter of the composite material particle would be the sum of the diameter of the core material and that of a coating material on the outer surface of the core material, and would result in an average total diameter of composite material particles, i.e. average particle diameter of the negative active material composite, that would be greater than about 1 μm to no more than about 15 μm ([0014]). The range overlaps with the claimed range and therefore provides a prima facie case of obviousness; see MPEP 2144.05, I.
Regarding Claim 10, the combination above teaches the negative active material composite of claim 1. Behan further teaches the silicon-silica hybrid material can have an average pore size of about 50 Å to about 1350 Å ([0052]), which would correspond to about 5 nm to 135 nm and which would overlap the claimed range.
Regarding Claim 11, the combination above teaches the negative active material composite of claim 1. Behan further teaches the surface area of from about 10 m2/g to about 250 m2/g ([0010]) and discloses “Porosity may be measured using techniques such as the Barrett, Joyner and Halenda method (BJH) and the Brunauer, Emmer and Teller method (BET) and Mercury Porosimetry, which are standard methods to determine the surface area, pore size and pore size distribution and bulk density in materials” ([0041]); therefore, Behan teaches a range for the claimed BET specific surface area of the negative active material composite that overlaps the claimed range.
Regarding Claim 13, the combination above teaches the negative active material composite of claim 1. Behan teaches generally that the silicon-silica hybrid materials, or SPS core ([0083]), can be formed from an agglomerate structure comprising subparticles of silicon and SiOx ([0054]), and the agglomerate structure thus corresponds to the claimed secondary particles in which the silicon particles are agglomerated, or aggregated. Behan further discloses the coating layer coats at least part of the SPS material, which is formed from the agglomerate structure (Fig. 8 and [0059]). Therefore, Behan’s teaching also reads on the limitation of a coating layer surrounding the outer layer of the secondary particles and the outer surface of the silicon nanoparticles (which are within the secondary particles) and including the amorphous carbon, given that the coating layer can be formed of amorphous carbon ([0062]).
Regarding Claim 21, the combination above teaches the negative active material composite of Claim 1. As pointed out previously, Williams teaches the active electrode material containing (e.g., silicon-containing) particles such as silicon and/or silicon oxide can have an average largest dimension, which can correspond to a diameter [098], of about 0.1 micron to about 5 micron [008], wherein the particles provided have a targeted size that provides good performance characteristics (e.g., good 1st cycle coulombic efficiency and good capacity retention) [008]. A skilled artisan would have found it obvious to have also modified the modified negative active material composite of Behan such that a maximum particle diameter (Dmax) of the silicon nanoparticles is greater than or equal to about 0.1 micron to about 5 micron as taught by Williams, to derive the benefits of good performance characteristics (e.g., good 1st cycle coulombic efficiency and good capacity retention). Consequently, the Dmax of the silicon nanoparticles of the combined prior art would overlap with the claimed range. In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. 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).
Claims 1-6, 8-11, 13, 18-22 are rejected under 35 U.S.C. 103 as being unpatentable over Shin et al (US 20200280062 A1, published 2020-09-03) in view of Tabuchi et al (US 20060166098 A1, published 2006-07-27), and Williams et al (WO 2018165427 A1).
Regarding claim 1, Shin teaches (Fig. 1A) a negative active material composite for a rechargeable lithium battery ([0002]), the lithium active material composite comprising silicon nanoparticles 11 and amorphous carbon (Abstract; [0043]-[0044]). Shin also teaches that the silicon nanoparticles can have an average particle diameter of about 50 nm to 150 nm ([0011]), which overlaps with the claimed ranges. Shin does not teach compound particles represented by SiOx particles within the negative active material composite or their average particle diameter, nor wherein a maximum particle diameter (Dmax) of the compound particles is about 5 µm to about 20 µm, nor does Shin teach the compound particles and the silicon nanoparticles in a weight ratio of about 8:2 to about 2:8.
In the same field of endeavor, Tabuchi teaches a composite particle 10 (also called composite particle (C)) (Figs. 4-5; [0120]) which can be used in a negative active material for a rechargeable lithium battery (Abstract, [0007]), wherein the composite particle 10 has particle 11 consisting of Si and particle 12 consisting of SiOx (where 0 <x ≤ 2) and carbon material A13 ([0120]). Tabuchi further teaches that including silicon oxide in the composite particle improves the cycle life ([0017]) and that preferably the proportion of the weight of Si to the total weight of Si and SiOx falls within the range of 20 wt. % to 80 wt. % for the reason that since Si exhibits a larger discharge capacity than SiOx, if the proportion of the weight of Si is less than 20 wt. %, the discharge capacity decreases; and that, on the other hand, since SiOx exhibits smaller volume expansion during charge/discharge and more excellent cycle performance than Si, if the proportion of the weight of Si is greater than 80 wt%, the cycle performance deteriorates ([0052]). One of ordinary skill in the art would have found it obvious to have modified Shin’s negative active material composite for a rechargeable lithium battery to further include SiOx particles, given that Tabuchi teaches it is a known configuration that improves cycle life of the battery, and they would have further included the SiOx such that the proportion of the weight of Si to the total weight of Si and SiOx fell within the range of 20 wt. % to 80 wt. % to optimize the discharge capacity, volume expansion during charge/discharge, and cycle performance of the battery as taught by Tabuchi. Accordingly, the proportion of the weight of SiOx to the total weight of Si and SiOx would be in the range of 20 wt. % to 80 wt.%, and the weight ratio of the compound particles (SiOx) and the silicon nanoparticles (Si) would be 80:20 to 20:80, or about 8:2 to about 2:8 as claimed. In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. 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).
In the same field of endeavor, Williams teaches the active electrode material containing (e.g., silicon-containing) particles such as silicon and/or silicon oxide wherein they have an average dimension, which can be a diameter, of about 10 nm or more and to about 5 micron ([098]). Williams also teaches the particles can have an average largest dimension of about 0.1 micron to about 10 micron [008], wherein the average largest dimension corresponds to the claimed maximum particle diameter, i.e. Dmax, and overlap with the claimed range. In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. 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). Williams further teaches the particles provided have a targeted size that provides good performance characteristics (e.g., good 1st cycle coulombic efficiency and good capacity retention) [008]. A skilled artisan would have found it obvious to have modified the modified negative active material composite of Shin to have the targeted size of the compound particles, including the average particle diameter D50 and the Dmax of compound particles represented by SiOx, as taught by Williams, to derive the benefits of good performance characteristics (e.g., good 1st cycle coulombic efficiency and good capacity retention).
Within the combination of prior art, the negative active material composite would thus have a matrix including the silicon nanoparticles and the amorphous carbon as taught by Shin and the compound particles taught by Tabuchi, wherein Tabuchi teaches the compound particles are in the matrix.
Regarding claim 2, the combination above teaches the negative active material composite of claim 1, and Shin further teaches the silicon nanoparticles can have an average particle diameter of about 50 nm to 150 nm ([0011]), which is within the claimed range.
Regarding claim 3, the combination above teaches the negative active material composite of claim 1, and Shin further teaches the aspect ratio of the silicon nanoparticles is about 2 to 8 ([0013]), which overlaps with the claimed range.
Regarding claim 4, the combination above teaches the negative active material composite of claim 1 and Shin further teaches a full width at half maximum of an X-ray diffraction angle using CuKα ray corresponding to a (111) plane of the silicon nanoparticles of about 0.3° to 7° ([0012], [0049]), which overlaps with the claimed range.
Regarding claim 5, the combination above teaches the negative active material composite as claimed in claim 1, and Shin further teaches wherein an internal pore volume of the negative active material composite is less than or equal to about 3.0 x 10-2 cm3/g ([0020]).
Regarding claim 6, the combination above teaches the negative active material composite of claim 1 and Shin further teaches the amorphous carbon may be a soft carbon, a hard carbon, a mesophase pitch carbonized product, a fired coke, or any combination thereof ([0015]).
Regarding claim 8, the combination above teaches the negative active material composite of claim 1. Shin teaches the silicon nanoparticles may be included in an amount of about 20 wt % to about 80 wt % based on a total weight of the negative active material composite ([0014]).
Tabuchi teaches the weight ratio of the compound particles (SiOx) and the silicon nanoparticles (Si) would be 80:20 to 20:80, or about 8:2 to about 2:8 as claimed, as previously pointed out in addressing the limitations of claim 2. Accordingly, an amount of compound particles which may be included can be calculated based on the product of the weight ratio of the compound particles and the silicon nanoparticles with the weight percentage range of silicon nanoparticles, resulting in a range of compound particles in an amount of about 5% to about 100% of the negative active material composite, which overlaps with the claimed range. In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. 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).
Given that amorphous carbon is present as a remaining component in the negative active material composite, its amount in the negative active material composite would be considered a balance amount or amorphous carbon.
Regarding claim 9, the combination above teaches the negative active material composite of claim 1, and Shin further teaches an average diameter of the negative active material composite is about 2 µm to about 15 µm ([0018]), which corresponds to the claimed range.
Regarding claim 10, the combination above teaches the negative active material composite of claim 1, and Shin further teaches the internal pore diameter of the negative active material composite is less than or equal to about 200 nm ([0019]), which is within the claimed range.
Regarding claim 11, the combination above teaches the negative active material composite of claim 1, and Shin further teaches the BET specific surface area of the negative active material composite may be less than or equal to about 10 m2/g ([0021]).
Regarding claim 13, the combination above teaches the negative active material composite of claim 12. Shin discloses that the adjacent distance between silicon nanoparticles 11, which refers to a distance between centers of adjacent silicon nanoparticles, may be less than or equal to about 50 nm ([0045]). An adjacent distance of 50 nm or less would result in overlap of particles with diameters of 50 nm or greater. Because Shin teaches silicon nanoparticles of an average particle diameter of 50 nm to 150 nm ([0011]), at least some of the silicon nanoparticles would be expected to overlap and touch other silicon nanoparticles and therefore be aggregated. Shin also discloses a coating layer (5) surrounding the outer surface of the secondary particles and including the amorphous carbon ([0043], [0055]), thereby reading on the limitations as claimed.
Regarding claim 18, the combination above teaches the negative active material composite of claim 1 and Shin further teaches it is used in a negative active material layer on a current collector within a negative electrode for a rechargeable lithium battery ([0002], [0074]).
Regarding claim 19, the combination above teaches the negative electrode of claim 18, and Shin further teaches the negative active material layer further includes a conductive material and a binder ([0076]), which reads on the claimed limitation.
Regarding claim 20, the combination above teaches the negative electrode of claim 18, and Shin further teaches a rechargeable lithium battery comprises a positive electrode and an electrolyte ([0027]).
Regarding claim 21, the combination above teaches the negative active material composite of Claim 1. As pointed out previously, Williams teaches the active electrode material containing (e.g., silicon-containing) particles such as silicon and/or silicon oxide can have an average largest dimension, which can correspond to a diameter [098], of about 0.1 micron to about 5 micron [008], wherein the particles provided have a targeted size that provides good performance characteristics (e.g., good 1st cycle coulombic efficiency and good capacity retention) [008]. A skilled artisan would have found it obvious to have also modified the modified negative active material composite of Shin such that a maximum particle diameter (Dmax) of the silicon nanoparticles is greater than or equal to about 0.1 micron to about 5 micron as taught by Williams, to derive the benefits of good performance characteristics (e.g., good 1st cycle coulombic efficiency and good capacity retention). Consequently, the Dmax of the silicon nanoparticles of the combined prior art would overlap with the claimed range. In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. 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).
Regarding claim 22, the combination above teaches the negative active material composite of claim 1. As previously pointed out in addressing the limitations of claim 1, Tabuchi teaches the proportion of the weight of Si to the total weight of Si and SiOx falls within the range of 20 wt. % to 80 wt. % [0052]. Accordingly, the proportion of the weight of SiOx to the total weight of Si and SiOx would be in the range of 20 wt. % to 80 wt.%, and the weight ratio of the compound particles (SiOx) and the silicon nanoparticles (Si) would be 80:20 to 20:80, or about 8:2 to about 2:8, which overlaps with the claimed range of 8:2 to 6:4. In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. 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).
Response to Arguments
Applicant’s arguments with respect to the prior art rejections have been considered but are moot because the new ground of rejection does not rely on any reference applied in the prior rejection of record for any teaching or matter specifically challenged in the argument.
Conclusion
Applicant's amendment necessitated the new ground(s) of rejection presented in this Office action. Accordingly, THIS ACTION IS MADE FINAL. See MPEP § 706.07(a). Applicant is reminded of the extension of time policy as set forth in 37 CFR 1.136(a).
A shortened statutory period for reply to this final action is set to expire THREE MONTHS from the mailing date of this action. In the event a first reply is filed within TWO MONTHS of the mailing date of this final action and the advisory action is not mailed until after the end of the THREE-MONTH shortened statutory period, then the shortened statutory period will expire on the date the advisory action is mailed, and any nonprovisional extension fee (37 CFR 1.17(a)) pursuant to 37 CFR 1.136(a) will be calculated from the mailing date of the advisory action. In no event, however, will the statutory period for reply expire later than SIX MONTHS from the mailing date of this final action.
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/G.L.L./ Examiner, Art Unit 1726
/BACH T DINH/ Primary Examiner, Art Unit 1726
09/29/2026
