DETAILED CORRESPONDENCE
1. The text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
Notice of Pre-AIA or AIA Status
2. 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
3. In response to the amendment received on 1/20/2026:
Claims 1-2, 4-6, and 8-17 are pending in the current application. Claims 1, 4, 6, 8, and 14 have been amended and Claims 3 and 7 are cancelled.
The previous objection to the claims has been overcome in light of the amendment.
The previous rejection under 35 USC 112 is overcome in light of the amendment.
The cores of the previous prior art-based rejections under 35 USC 102 have been overcome in light of the amendment, but the claims remain rejected under previously relied upon prior art. All changes made to the rejection are necessitated by the amendment.
Claim Interpretation
4. All “wherein” clauses are given patentable weight unless otherwise noted. Please see MPEP 2111.04 regarding optional claim language.
Claim Rejections - 35 USC § 103
5. Claims 1-2, 4-6, 8-9, and 13 are rejected under 35 U.S.C. 103 as being unpatentable over Liao CN109524643 in view of Zhu CN111668474.
Regarding Claims 1-2, 4-5, and 13, Liao discloses a silicon composite material comprising a one-dimension conductive material (carbon nanotubes/CNT, para 0022), an inner core comprising silicon-based material (formed of nanosilicon which is elemental or elementary silicon, para 0022, meeting Claim 13), and a cladding layer (amorphous carbon is coated on the nano-silicon, para 0022, meeting Claim 5) that clads on an outer surface of the inner core, the one-dimensional conductive material is arranged on an outer surface of the cladding layer (see entire disclosure and especially paras 0004-0005, 0022, 0047).
Liao discloses that CNT (carbon nanotubes, i.e. the one-dimensional conductive material) have high mechanical strength and conductivity in the axial direction to form a highly conductive network (see e.g. para 0022) and the skilled artisan would presume that because of the randomness of the mixing of the Si/C particles into a dispersion of GO/CNT (e.g. para 0027), at least some portion of the CNT would inherently extend outwardly from the outer surface of the cladding layer (meeting Claim 2). If it is not inherent that some portion of the CNT would extend outwardly from the outer surface of the cladding layer, in the same field of endeavor of composite Si-C negative electrode active material particles, Zhu teaches that designing a layered Si-based composite active material benefits from having carbon nanotubes (CNTs) grown at the surface of the carbon coating such that the CNTs extend from the surface to mutually entangle with CNTs from other negative electrode active material particles in order to form line-to-line contact, which increases electrical connection (see entire disclosure and especially e.g. para 0037 and Fig. 1). Therefore, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the instant application to design the silicon composite material of Liao such that the one-dimensional conductive material extends outward from the outer surface of the cladding layer because Zhu teaches that this allows the material to mutually entangle with CNTs from other negative electrode active material particles in order to form line-to-line contact, which increases electrical connection (again, meeting Claim 2).
Liao fails to specifically disclose wherein the outer surface of the cladding layer further has catalyst particles, the one-dimensional conductive material is arranged on surfaces of the catalyst particles, and the catalyst particles comprise transition metal nanoparticles comprising one or more of iron nanoparticles, cobalt nanoparticles, and nickel nanoparticles. However, Zhu teaches that growing the carbon nanotubes described above is best carried out by depositing e.g. transition metal nanoparticles such as nickel nanoparticle catalyst (or Fe or Co, para 0017, meeting Claim 4) on the surface of a carbon-coated silicon particle and growing the outwardly-extending CNTs from the catalyst particles such that the CNTs would be arranged on surfaces of said catalyst nanoparticles (see entire disclosure and especially paras 0067-0072). Therefore, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the instant application to design the silicon composite material of Liao modified by Zhu such the outer surface of the cladding layer further has catalyst particles, the one-dimensional conductive material is arranged on surfaces of the catalyst particles, and the catalyst particles comprise transition metal nanoparticles comprising one or more of iron nanoparticles, cobalt nanoparticles, and nickel nanoparticles because Zhu teaches that this design and method of growing the carbon nanotubes (including the claimed catalyst) provides the desired aspect ratio which allows the negative electrode material to exhibit the benefits of the CNTs (mutually entangle with CNTs from other negative electrode active material particles in order to form line-to-line contact, which increases electrical connection).
Regarding Claim 6, Liao fails to specifically disclose wherein mass percentage of the catalyst particles is 0.001% to 0.3% based on mass of the silicon-based material. Zhu teaches that the mass ratio of carbon-coated silicon/graphite composite material to the catalyst (upon which the CNTs grow) is controlled at 1000: (1 to 10) (para 0071), for example, which is 0.1% to 1%. Zhu does not specifically disclose a mass percent based on the silicon-based material (rather, Zhu teaches that this ratio is based on the carbon-coated Si/graphite composite material, para 0071. However, the skilled artisan would understand that the amount of silicon in the core of the negative electrode active material of Zhu has a small percent of Si versus graphite and carbon coating (the core can be 10% Si and the graphite layer can be only 1 nm thick, paras 0075-0076), and so the mass % of catalyst based on the Si-based content is 0.01% to 0.1%. Therefore, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the instant application to design the silicon composite material of Liao modified by Zhu such that mass percentage of the catalyst particles is 0.01% to 0.1% (which falls in the claimed range of 0.001% to 0.3%) based on mass of the silicon-based material because Zhu teaches that this ratio is used to grow the desired nanotubes. “[W]here the general conditions of a claim are disclosed in the prior art, it is not inventive to discover the optimum or workable ranges by routine experimentation.” See In re Aller, 220 F.2d 454, 456, 105 USPQ 233, 235 (CCPA 1955). The discovery of an optimum value of a known result effective variable, without producing any new or unexpected results, is within the ambit of a person of ordinary skill in the art. See In re Boesch, 205 USPQ 215 (CCPA 1980) (see MPEP § 2144.05, II.).
Regarding Claims 8 and 9, Liao further discloses wherein the carbon nanotubes have average tube length of 7 to 20 µm and an average tube diameter of 7 nm to 15 nm (para 0011), both ranges which either fall within and, therefore, anticipate the claimed range (re: diameter) or are very close to, and therefore render obvious, the claimed range (length) of: length of 0.5 µm to 50 µm and/or a diameter of 1 nm to 50 nm (Claim 8) and length of from 1 µm to 10 µm and/or a diameter of 20 nm to 30 nm. 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) (The prior art taught carbon monoxide concentrations of "about 1-5%" while the claim was limited to "more than 5%." The court held that "about 1-5%" allowed for concentrations slightly above 5% thus the ranges overlapped.); In re Geisler, 116 F.3d 1465, 1469-71, 43 USPQ2d 1362, 1365-66 (Fed. Cir. 1997) (Claim reciting thickness of a protective layer as falling within a range of "50 to 100 Angstroms" considered prima facie obvious in view of prior art reference teaching that "for suitable protection, the thickness of the protective layer should be not less than about 10 nm [i.e., 100 Angstroms]." The court stated that "by stating that 'suitable protection' is provided if the protective layer is 'about' 100 Angstroms thick, [the prior art reference] directly teaches the use of a thickness within [applicant's] claimed range."). Similarly, a prima facie case of obviousness exists where the claimed ranges and prior art ranges do not overlap but are close enough that one skilled in the art would have expected them to have the same properties. Titanium Metals Corp. of America v. Banner, 778 F.2d 775, 227 USPQ 773 (Fed. Cir. 1985) (Court held as proper a rejection of a claim directed to an alloy of "having 0.8% nickel, 0.3% molybdenum, up to 0.1% iron, balance titanium" as obvious over a reference disclosing alloys of 0.75% nickel, 0.25% molybdenum, balance titanium and 0.94% nickel, 0.31% molybdenum, balance titanium.).
The nanotube length and diameter disclosed by Liao are understood to be given as averages. The skilled artisan would understand that stating anything but an average for a group of nanotubes grown on particles without describing which nanotubes the dimensions apply to would be non-sensical.
6. Claims 10-12, 14, and 16-17 are rejected under U.S.C. 103 as being unpatentable over Liao CN109524643 in view of Zhu CN111668474, as applied to Claim 1, and further in view of Choi US PG Publication 2023/0058028.
Regarding Claims 10-11, Liao modified by Zhu discloses the Si@C/rGO/CNT composite particles having the specified mass proportions (para 0043 of Liao):
Si@C is mixed at a glucose:Si at a 1:1 weight ratio, so the ratio of C:Si would be about 0.4:1 (since glucose is about 40% C)
GO:CNT is mixed at an 8:1 weight ratio
Si@C/ is mixed with GO:CNT at a 20:6 weight ratio
If Si@C is 40% Si, then based on the proportions listed above (resulting in 4/10 x 1/8 x 6/20 = 0.015), the weight ratios of components would result in a weight relationship between Si and CNT (the one-dimensional conductive material) of 1.5%. Even if there are slight differences in resulting masses (e.g. after the composition is heated), the skilled artisan would expect the values to be close to the claimed mass percentage. Further, Liao teaches multiple embodiments having varied proportions which also result in CNT:Si in the claimed range.
Even further, in the same field of endeavor of silicon-based composite negative electrode active material design, Choi discloses that silicon composite material having a silicon-based core coated in a carbon layer and having enhanced conductivity due to use of carbon nanotubes uses the nanotubes in a weight ratio with silicon-based active material that is designed to optimize the security of the conductive path of the silicon-based active material, e.g. from 0.2% to 1.0% (99:1 to 99.8:0.2) or 0.01% to 8.6% (92:8 to 99.99:0.01) (see e.g. para 0085). Therefore, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the instant application to design the material of Liao modified by Zhu such that mass percentage of the one-dimensional conductive material of modified Liao is 0.01% to 5% or 0.4% to 5% based on the mass of the silicon-based material because Choi teaches values in this range and teaches that this value should be optimized to ensure the security of the conductive path of the silicon-based active material. “[W]here the general conditions of a claim are disclosed in the prior art, it is not inventive to discover the optimum or workable ranges by routine experimentation.” See In re Aller, 220 F.2d 454, 456, 105 USPQ 233, 235 (CCPA 1955). The discovery of an optimum value of a known result effective variable, without producing any new or unexpected results, is within the ambit of a person of ordinary skill in the art. See In re Boesch, 205 USPQ 215 (CCPA 1980) (see MPEP § 2144.05, II.).
Regarding Claim 12, Liao modified by Zhu fails to specifically disclose the Dv50 of the silicon composite material is 1 µm to 30 µm. However, Choi teaches that the silicon composite active material particles preferably have a volume average particle size (D50) 4 µm to 11 µm, optimized for preventing side reactions with electrolyte and swelling effects disrupting the conductive path (see e.g. para 0159). Therefore, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the instant application to design the silicon composite material of Liao and Zhu to have a Dv50 of 4 µm to 10 µm (which falls within and therefore anticipates the claimed range of 1 µm to 30 µm) because Choi teaches that these values provide particles that are sized to be optimized for preventing side reactions with electrolyte and swelling effects disrupting the conductive path. “[W]here the general conditions of a claim are disclosed in the prior art, it is not inventive to discover the optimum or workable ranges by routine experimentation.” See In re Aller, 220 F.2d 454, 456, 105 USPQ 233, 235 (CCPA 1955). The discovery of an optimum value of a known result effective variable, without producing any new or unexpected results, is within the ambit of a person of ordinary skill in the art. See In re Boesch, 205 USPQ 215 (CCPA 1980) (see MPEP § 2144.05, II.).
Regarding Claims 14 and 16-17, Liao discusses the silicon composite negative electrode active material as an improvement upon previous materials based on issues involving e.g. loss of contact between active material and the electrode current collector (para 0005) but Liao modified by Zhu does not specifically disclose a negative electrode plate comprising a negative electrode current collector, and a negative electrode active material layer arranged on at least one surface of the negative electrode current collector, wherein the negative electrode active material layer comprises the silicon composite of Claim 1 or a secondary battery comprising said negative electrode plate or an electrical apparatus comprising said negative electrode plate. However, Choi discloses that silicon composite material having a silicon-based core coated in a carbon layer and having enhanced conductivity due to use of carbon nanotubes is useful in a negative electrode active material layer in a negative electrode plate in a secondary battery used in an electrical apparatus (see entire disclosure and especially e.g. paras 0004-0006, 0010-0011, 0109). Therefore, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the instant application to use the silicon composite material of Liao in a negative electrode active material layer arranged on at least one surface of a negative electrode current collector of a negative electrode plate, wherein the negative electrode active material layer comprises the silicon composite of Claim 1 and to use said negative electrode plate in a secondary battery comprising and an electrical apparatus because Choi teaches that this type of material is useful for the same technology and the selection of a known material, which is based upon its suitability for the intended use, is within the ambit of one of ordinary skill in the art. See In re Leshin, 125 USPQ 416 (CCPA 1960) (see MPEP § 2144.07). The combination of familiar elements is likely to be obvious when it does no more than yield predictable results. See KSR International Co. v. Teleflex Inc., 550 U.S. __,__, 82 USPQ2d 1385, 1395 – 97 (2007) (see MPEP § 2143, A.).
7. Claim 15 is rejected under U.S.C. 103 as being unpatentable over Liao CN109524643 in view of Zhu CN111668474 and Choi US PG Publication 2023/0058028, as applied to Claim 14, and further in view of Salem US PG Publication 2019/0214640.
Regarding Claim 15, Liao modified by Zhu and Choi discloses the claimed silicon composite material as described in the rejection of Claim 14, which is incorporated herein in its entirety. Liao fails to specifically disclose wherein the negative electrode active material layer further comprises a carbon-based material and mass ratio of the silicon composite material to the carbon-based material is (10%-90%):(90%-10%). However, Choi teaches that the carbon layer on the Si core can comprise at least one of amorphous and crystalline carbon, and that the crystalline carbon can be carbon nanotubes (see e.g. paras 0037-0040), and if both materials were used (amorphous carbon and CNTs), the structure would be similar to that of Liao. Choi further teaches the use of a conductive additive (carbon-based conductive material) in the negative electrode active material layer (see at least para 0093). Therefore, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the instant application to further use a conductive additive with the silicon composite material of the negative electrode of Liao modified by Choi because Choi teaches the use of multiple materials for enhancing conductivity in the electrode, including an additional carbon-based conductive material mixed with the silicon-based active material particle. Liao modified by Choi does not specifically disclose a mass ratio of silicon composite material to the carbon-based in the same field of endeavor of silicon-based composite negative electrode active material design, Salem teaches that silicon composite active material particles (such as silicon coated with carbon, paras 0200-0204) are enhanced by the presence of e.g. 2.5 wt% conductive additive (see paras 0239, 0242). Therefore, it would have been obvious to a person having ordinary skill in the art before the effective filing date of the instant application to design the silicon composite material of Liao and Choi to include a conductive additive of carbon-based material in addition to the carbon-and-silicon composite electrode material and to include said carbon-based material in a weight percent of e.g. 2.5 wt% because Salem teaches that this is a functional amount of conductive additive to use in a similar application and “[W]here the general conditions of a claim are disclosed in the prior art, it is not inventive to discover the optimum or workable ranges by routine experimentation.” See In re Aller, 220 F.2d 454, 456, 105 USPQ 233, 235 (CCPA 1955).
Response to Arguments
8. Applicant's arguments with respect to the claims are based on the claims as amended. The amended claims have been addressed in the new rejection above.
Further,
9. Applicant argues that Zhu is cited for teaching deposition of a nanoparticle catalyst on the surface of a carbon-coated silicon particle as opposed to the claimed invention which clads on an outer surface of the inner core and the inner core comprises the silicon-based material and that there is no suggestion in the combination of references or a reasonable expectation of success of the claimed invention in light of the cited prior art.
The Office has considered this argument and respectfully disagrees. It is submitted that arguments of counsel cannot take the place of factually supported objective evidence. See, e.g., In re Huang, 100 F.3d 135, 139-40, 40 USPQ2d 1685, 1689 (Fed. Cir. 1996); In re De Blauwe, 736 F.2d 699, 705, 222 USPQ 191, 196 (Fed. Cir. 1984). Since Zhu teaches an inner core of the active material comprising graphite coated in Si and coats that inner core with carbon, this structure is is considered to meet the open language of “inner core comprises a silicon-based material”. “(B)y in-situ growing carbon nanotubes with an aspect ratio greater than 3000 on the surface of carbon-coated silicon/graphite composite material, the conductivity of the obtained negative electrode material is significantly improved, and the shortcomings of silicon's weak conductivity are compensated. At the same time, due to the large aspect ratio of carbon nanotubes, they are prone to entanglement, which can form line-to-line contact between negative electrode material particles, increasing electrical connection. Furthermore, during the slurry mixing process, a flexible "cage" structure can be formed on the outermost layer of the negative electrode material particles, providing a buffer for the volume expansion effect of silicon. This further reduces the stress caused by the volume expansion effect of silicon powder during charging and discharging on the negative electrode material particles, thus ensuring the cycle performance of the obtained negative electrode material” (para 0037 of Zhu).
Because Zhu teaches a benefit to the formation of the CNTs on catalyst particles over a carbon-coated inner core of silicon and graphite, the benefit is based not only on the presence of silicon in the core but also on interactions between particles, and the skilled artisan would find the benefit of Zhu to be reasonably predictable.
10. Applicant argues that the rest of the claims are patentable over the prior art of record for the same reason as the independent claim 1. The Office respectfully disagrees. The rejections with respect to the independent claim have been maintained, and thus the rejections of the dependent claims are maintained as well.
Conclusion
11. 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 extension fee 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 date of this final action.
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/LISA S PARK/Primary Examiner, Art Unit 1729
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