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 .
Continued Examination Under 37 CFR 1.114
A request for continued examination under 37 CFR 1.114, including the fee set forth in 37 CFR 1.17(e), was filed in this application after final rejection. Since this application is eligible for continued examination under 37 CFR 1.114, and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114. Applicant's submission filed on 05/06/2026 has been entered.
Priority
Receipt is acknowledged of certified copies of papers required by 37 CFR 1.55.
Information Disclosure Statement
The information disclosure statement(s) (IDS) submitted on 04/21/2026 have been considered by the examiner.
Response to Amendment
Examiner notes the following amendments made to the claims:
Claim 1 amended to further include a carbonaceous material and a specific weight ratio between the Mg-containing silicon oxide and the carbonaceous material
Claim 8 cancelled
Response to Arguments
Applicant’s arguments, filed 05/26/2026, with respect to the rejection(s) of claim(s) 1-3, 5, 7, 9-11 under 35 USC 103 have been fully considered and are persuasive. Specifically, by further amending the ratio of Mg-containing silicon oxide negative electrode active material to carbonaceous negative electrode active material, the previously applied prior art is overcome. Therefore, the rejection has been withdrawn. However, upon further consideration, a new ground(s) of rejection is made in view of Iwaya (US 20210083275 A1), which teaches a negative electrode containing a silicon oxide negative active material and a carbonaceous negative active material, in a weight ratio which encompasses the claimed range. Since no arguments are made regarding the dependent claims, the rejections remain in place and unchanged other than now being further in view of Iwaya.
Claim Rejections - 35 USC § 103
The text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
Claim(s) 1-3, 5, 7, 9-11 is/are rejected under 35 U.S.C. 103 as being unpatentable over Lee (US 20230238514 A1) in view of Jo (US 20130248772 A1), further in view of Son (US 20150380728 A1) further in view of Lee (US 20190334161 A1), hereinafter referred to as Lee ‘161, and further in view of Iwaya (US 20210083275 A1).
Regarding claim 1, Lee teaches the following elements:
A negative electrode, comprising: a current collector; and a negative electrode active material layer on at least one surface of the current collector, wherein the negative electrode active material layer comprises: (“The negative electrode may be composed of a negative electrode composition only or may be composed of a negative electrode current collector and a negative electrode composition layer (negative electrode active material layer) supported thereon.” Lee [0235])
1) a negative electrode active material comprising a Mg- containing silicon oxide, a carbon coating layer surrounding the surface of the Mg- containing silicon oxide and a graphene coating layer surrounding the surface of the carbon coating layer, (“an embodiment of the present invention provides a silicon-based-carbon composite having a core-shell structure, wherein the core comprises silicon, a silicon oxide compound, and magnesium silicate, and the shell comprises at least two carbon layers comprising a first carbon layer and a second carbon layer, wherein the second carbon layer is reduced graphene oxide.” Lee [0014])
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3) a binder, (“In addition, the negative electrode composition and the positive electrode composition may each further comprise a conductive agent and a binder.” Lee [0235])
wherein an amount of the graphene coating layer is 0.5 wt% to 10 wt % based on a total weight of the negative electrode active material. (“The content of carbon (C) in the second carbon layer may preferably be 3% by weight to 20% by weight, more preferably, 3% by weight to 15% by weight, even more preferably, 3% by weight to 10% by weight, based on the total weight of the silicon-based-carbon composite.” Lee [0097] and “The second carbon layer according to an embodiment of the present invention may be reduced graphene oxide having particularly high electrical conductivity.” Lee [0116] and “A negative electrode and a battery (coin cell) comprising the silicon-based-carbon composite (composite E1) of a core-shell structure as a negative electrode active material were fabricated.” Lee [0259])
The examiner takes note of the fact that the prior art range of 3-20 wt % for the amount of graphene based on the total weight of the negative electrode active material layer overlaps the claimed range of 0.5-10 wt % for the same parameter. Absent any additional and more specific information in the prior art, a prima facie case of obviousness exists. In re Peterson, 315 F.3d 1325, 1330, 65 USPQ2d 1379 (Fed. Cir. 2003). MPEP 2144.05.
wherein the negative electrode active material layer further comprises a carbonaceous active material, (“In addition, the negative electrode active material may further comprise a carbon-based negative electrode material.” Lee [0229])
Lee is silent on the following elements of claim 1:
wherein the graphene present in the graphene coating layer has a D/G band intensity ratio of 0.8 to 1.5, and the D/G band intensity ratio of the graphene is defined as an average value of a ratio of a maximum peak intensity of D band at 1360 ± 50 cm' based on a maximum peak intensity of G band at 1580 ± 50 cm1, as determined by Raman spectroscopy of graphene.
2) a conductive material comprising single-walled carbon nanotubes (SWCNTs),
The negative electrode according to claim 1, wherein an amount of the single-walled carbon nanotubes is 0.01 wt % to 0.06 wt% based on a total weight of the negative electrode active material layer.
and a weight ratio of the negative electrode active material comprising the Mg-containing silicon oxide, the carbon coating layer surrounding the surface of the Mg-containing silicon oxide and the graphene coating layer surrounding the surface of the carbon coating layer to the carbonaceous active material is in a range of 1:5.7 to 1:33
Jo teaches the following elements of claim 1 that are not explicitly taught by Lee:
2) a conductive material comprising single-walled carbon nanotubes (SWCNTs), electrode (“The first and second carbon nano conductive agents may include single-walled carbon nanotubes (SWNTs), multi-walled carbon nanotubes (MTWNTs), cup-stack type MTWNTs or mixtures thereof. “ Jo [0016])
Jo and Lee are considered to be analogous because they are both within the same field of electrode materials containing carbonaceous materials. Therefore, it would have been obvious to one of ordinary skill before the effective filing date of the claimed invention to modify the carbon nanotubes taught by Lee (“The carbon-based negative electrode material may comprise, for example, at least one selected from the group consisting of natural graphite, synthetic graphite, soft carbon, hard carbon, mesocarbon, carbon fibers, carbon nanotubes,” Lee [0230]) to be specifically SWCNTs, as taught by Jo. This would be obvious as it would only require a simple substitution of one known material with another, and the simple substitution of one known element for another is likely to be obvious when predictable results are achieved. (see MPEP § 2143, B.).
Lee and Jo are both silent on the following elements of claim 1:
wherein the graphene present in the graphene coating layer has a D/G band intensity ratio of 0.8 to 1.5, and the D/G band intensity ratio of the graphene is defined as an average value of a ratio of a maximum peak intensity of D band at 1360 ± 50 cm' based on a maximum peak intensity of G band at 1580 ± 50 cm1, as determined by Raman spectroscopy of graphene.
The negative electrode according to claim 1, wherein an amount of the single-walled carbon nanotubes is 0.01 wt % to 0.06 wt% based on a total weight of the negative electrode active material layer.
and a weight ratio of the negative electrode active material comprising the Mg-containing silicon oxide, the carbon coating layer surrounding the surface of the Mg-containing silicon oxide and the graphene coating layer surrounding the surface of the carbon coating layer to the carbonaceous active material is in a range of 1:5.7 to 1:33
Son teaches the following elements of claim 1 that are not found in Lee or Jo:
wherein the graphene contained in the graphene coating layer has a D/G band intensity ratio of 0.8-1.5, and the D/G band intensity ratio of the graphene is defined as an average value of the ratio of the maximum peak intensity of D band at 1360 ± 50 cm' based on the maximum peak intensity of G band at 1580 ± 50 cm1, as determined by Raman spectroscopy of graphene. (“The coating of graphene on the silicon oxide (SiOx) by vapor deposition may form a coating layer having high crystallinity on the composite.” Son [0148]) and “The graphene may have a degree of crystallinity of about 0.5 to about 1.5, for example, about 1.055 to about 1.146, or about 1.06 to about 1.14. The degree of crystallinity (or degree of disordering of graphene crystals) of the graphene may be obtained by measuring an intensity ratio of D peak to G peak (D/G) in a Raman spectra of the composite.” Son [0086-0087])
The examiner takes note of the fact that the prior art range of ------0.5-1.5 for the D/G ratio in the graphene coating encompasses the claimed range of 0.8-1.5 for the same parameter. Absent any additional and more specific information in the prior art, a prima facie case of obviousness exists. In re Peterson, 315 F.3d 1325, 1330, 65 USPQ2d 1379 (Fed. Cir. 2003). MPEP 2144.05.
Son and Lee are considered to be analogous because they are both within the same field of graphene-coated silicon oxide materials to be used in anodes of secondary batteries. Therefore, it would have been obvious to one of ordinary skill before the effective filing date of the claimed invention to modify the graphene coating of Lee to have the specific D/G ratio of Son in order to improve conductivity without requiring structural change (“The coating of graphene on the silicon oxide (SiOx) by vapor deposition may form a coating layer having high crystallinity on the composite. When the composite having such a highly-crystalline coating layer is used as an anode active material, the anode active material may have improved conductivity without structural change.” Son [0148]). Additionally, both inventions use a graphene coating, and therefore it would only require a simple substitution to replace that of Lee with that of Son, and the simple substitution of one known element for another is likely to be obvious when predictable results are achieved. (see MPEP § 2143, B.).
By using the graphene coating layer of Son in place of that of Lee, the additional limitations of claims 2-3, 5, 8-10 would all be met without requiring any further modification or motivation.
Lee, Son, and Jo are silent on the following elements of claim 1:
The negative electrode according to claim 1, wherein an amount of the single-walled carbon nanotubes is 0.01 wt % to 0.06 wt% based on a total weight of the negative electrode active material layer.
and a weight ratio of the negative electrode active material comprising the Mg-containing silicon oxide, the carbon coating layer surrounding the surface of the Mg-containing silicon oxide and the graphene coating layer surrounding the surface of the carbon coating layer to the carbonaceous active material is in a range of 1:5.7 to 1:33
However, Lee ‘161 teaches the following elements of claim 1 that are not found in modified Lee:
The negative electrode according to claim 1, wherein an amount of the single-walled carbon nanotubes is 0.01 wt % to 0.06 wt% based on a total weight of the negative electrode active material layer. (“97.45 wt % of artificial graphite, 1.5 wt % of styrene butadiene rubber, 0.05 wt % of an SWCNT conductive agent of Table 1, and 1 wt % of carboxymethyl cellulose were mixed in water to prepare negative active material slurry.” Lee [0115])
Lee ‘161 is considered to be analogous to Lee because they are both within the same field of negative electrode active materials. Therefore, it would have been obvious to one of ordinary skill before the effective filing date of the claimed invention to modify the conductive agent of Lee to be the specific ratio of Lee ‘161 (0.05 wt % of the total) as this proportion is known in the art and was shown in Lee ‘161 to have a higher capacity retention and lower are specific resistance than comparative examples (Lee ‘161 figures 6 and 7).
Lee, Son, Jo, and Lee ‘161 are silent on the following elements of claim 1:
and a weight ratio of the negative electrode active material comprising the Mg-containing silicon oxide, the carbon coating layer surrounding the surface of the Mg-containing silicon oxide and the graphene coating layer surrounding the surface of the carbon coating layer to the carbonaceous active material is in a range of 1:5.7 to 1:33
However, Iwaya teaches all of the elements of claim 1 that are not found in the aforementioned references:
and a weight ratio of the negative electrode active material comprising the Mg-containing silicon oxide, the carbon coating layer surrounding the surface of the Mg-containing silicon oxide and the graphene coating layer surrounding the surface of the carbon coating layer to the carbonaceous active material is in a range of 1:5.7 to 1:33 (“In the present invention, the electrode active material contains a silicon particle having a high energy density. Examples of the silicon particle may include … a silicon oxide” Iwaya [0061], “The electrode active material contains at least the silicon particle (a first active material) or may contain the first active material and a second active material in combination. Such a second active material may include, for example, a carbonaceous or carbon material (carbon)” Iwaya [0067] and “The ratio of the second active material particle (e.g., the carbonaceous particle) relative to the silicon particle is not particularly limited to a specific one, and the former/the latter (weight ratio) may be selected from a wide range of about 99/1 to 0/100” Iwaya [0071]. Iwaya teaches a combination of silicon oxide and a carbonaceous material as negative electrode active materials in a weight ratio which would render obvious the above limitation.)
The examiner takes note of the fact that the prior art range of 100:0 to 1:99 for the weight ratio of silicon oxide active material to carbonaceous active material encompasses the claimed range of 1:5.7 to 1:33 for the same parameter. Absent any additional and more specific information in the prior art, a prima facie case of obviousness exists. In re Peterson, 315 F.3d 1325, 1330, 65 USPQ2d 1379 (Fed. Cir. 2003). MPEP 2144.05.
Iwaya and Lee are considered to be analogous because they are both within the same field of negative electrodes containing a combination of a silicon-oxide based particle and a carbonaceous material as the negative electrode active material. Therefore, it would have been obvious to one of ordinary skill before the effective filing date of the claimed invention to modify the active material mixture of Lee to have the weight ratio of Iwaya in order to optimize the benefits of both materials. Iwaya states that (“A higher ratio of the silicon particle allows a higher discharge capacity.” Iwaya [0071]) and (“In particular, among the second electrode active materials, the carbonaceous (or carbon) material is preferred for improving the adhesion to the current collector without lowering of the charge-discharge efficiency of the silicon particle.” Iwaya [0070].) Therefore, one of ordinary skill in the art would be capable of adjusting the ratio in order to optimize the benefits of both materials through routine experimentation, and using the range provided by Iwaya prior to the effective filing date of the invention to do so.
Regarding claim 2, modified Lee teaches all of the elements of claim 1, as shown above. Lee is silent on the following elements of claim 2:
The negative electrode according to claim 1, wherein the D/G band intensity ratio of the graphene present in the graphene coating layer ranges from 0.8 to 1.4.
However, Son teaches all of the elements of claim 2 that are not found in Lee:
The negative electrode according to claim 1, wherein the D/G band intensity ratio of the graphene present in the graphene coating layer ranges from 0.8 to 1.4. (“The coating of graphene on the silicon oxide (SiOx) by vapor deposition may form a coating layer having high crystallinity on the composite.” Son [0148]) and “The graphene may have a degree of crystallinity of about 0.5 to about 1.5, for example, about 1.055 to about 1.146, or about 1.06 to about 1.14. The degree of crystallinity (or degree of disordering of graphene crystals) of the graphene may be obtained by measuring an intensity ratio of D peak to G peak (D/G) in a Raman spectra of the composite.” Son [0086-0087])
The examiner takes note of the fact that the prior art range of ------0.5-1.5 for the D/G ratio in the graphene coating encompasses the claimed range of 0.8-1.4 for the same parameter. Absent any additional and more specific information in the prior art, a prima facie case of obviousness exists. In re Peterson, 315 F.3d 1325, 1330, 65 USPQ2d 1379 (Fed. Cir. 2003). MPEP 2144.05.
Regarding claim 3, modified Lee teaches all of the elements of claim 1, as shown above. Lee teaches all of the additional elements of claim 3:
The negative electrode according to claim 1, wherein the Mg-containing silicon oxide comprises 4 wt % to 15 wt % of Mg. (“Meanwhile, the content of magnesium (Mg) in the silicon-based-carbon composite may be 0.2% by weight to 15% by weight, 0.2% by weight to 10% by weight, or 0.2% by weight to 8% by weight, based on the total weight of the silicon-based-carbon composite.” Lee [0034])
The examiner takes note of the fact that the prior art range of 0.2-15 wt% for Mg present in the silicon oxide containing composite material encompasses the claimed range of 4-15 wt% for the same parameter. Absent any additional and more specific information in the prior art, a prima facie case of obviousness exists. In re Peterson, 315 F.3d 1325, 1330, 65 USPQ2d 1379 (Fed. Cir. 2003). MPEP 2144.05.
Regarding claim 5, modified Lee teaches all of the elements of claim 1, as shown above. Lee teaches all of the additional elements of claim 5:
The negative electrode according to claim 1, wherein an amount of the carbon coating layer is 0.5 wt % to 10 wt % based on a total weight of the negative electrode active material. (“Meanwhile, the total content of carbon (C) in the first carbon layer and the second carbon layer may be 5% by weight to 50% by weight based on the total weight of the silicon-based-carbon composite.” Lee [0095])
The examiner takes note of the fact that the prior art range of 5-50 wt % for the amount of carbon based on the total weight of the negative electrode active material layer overlaps the claimed range of 0.5-10 wt % for the same parameter. Absent any additional and more specific information in the prior art, a prima facie case of obviousness exists. In re Peterson, 315 F.3d 1325, 1330, 65 USPQ2d 1379 (Fed. Cir. 2003). MPEP 2144.05.
Regarding claim 7, modified Lee teaches all of the elements of claim 1, as shown above. Lee and Son are silent on the following elements of claim 7:
The negative electrode according to claim 1, wherein the conductive material further comprises at least one of carbon black, acetylene black, ketjen black, carbon nanofibers, channel black, furnace black, lamp black, thermal black, carbon fibers, metal fibers, fluorocarbon, metal powder, conductive whisker, conductive metal oxide, or polyphenylene derivative.
However, Jo teaches all of the elements of claim 7 that are not found in Lee:
The negative electrode according to claim 1, wherein the conductive material further comprises at least one of carbon black, acetylene black, ketjen black, carbon nanofibers, channel black, furnace black, lamp black, thermal black, carbon fibers, metal fibers, fluorocarbon, metal powder, conductive whisker, conductive metal oxide, or polyphenylene derivative. (“The first and second carbon nano conductive agents may include single -walled carbon nanotubes (SWNTs), multi-walled carbon nanotubes (MTWNTs), cup-stack type MTWNTs or mixtures thereof. The secondary battery may further include an additional conductive agent selected from the group consisting of natural graphite, artificial graphite, carbon black, acetylene black, ketjen black, carbon fiber, copper, nickel, aluminum, silver, polyphenylene derivatives and combinations thereof, and a mixing ratio of the first and second carbon nano conductive agents and the additional conductive agent may range from 1:1 to 1:10” Jo [0016-0017])
Jo is analogous to Lee because they are both within the same field of negative electrode active materials, as shown above for claim 1. Therefore, it would have been obvious to one of ordinary skill before the effective filing date of the claimed invention to modify the conductive material of Lee to comprise both SWCNTs and a second conductive agent, as taught in Jo, in order to reduce the electrical resistance and improve the binding strength of the active material (“the conductive agent for an electrode of a secondary battery may include a first carbon nano conductive agent which has a first diameter and is dispersed on a surface of an active material and a second carbon nano conductive agent which has a second diameter and is positioned between molecules of active material and forms a micro network of electrical conduction. Such conductive agent reduces the electrical resistance of the active material and improves the binding strength of the active material.” Jo [0027]). Additionally, the combination of conductive agents taught by Jo can improve discharge characteristics (“In addition, the conductive agent for the electrode of a secondary battery constructed with an embodiment of the present invention serves to perform a conducting function like the contemporary conductive agent and improves the binding strength between active materials and between an active material and a current collector, thereby improving the high-rate discharge characteristic and the cycle life characteristics.” Jo [0028]).
Regarding claim 9, modified Lee teaches all of the elements of claim 1, as shown above. Lee teaches all of the additional elements of claim 9:
The negative electrode according to claim 8, wherein the carbonaceous active material comprises at least one of artificial graphite, natural graphite, graphitizable carbon fibers, graphitizable mesocarbon microbeads, petroleum cokes, baked resin, carbon fibers, or pyrolyzed carbon. (“The negative electrode active material may be used as a mixture of the silicon-based-carbon composite and the carbon-based negative electrode material. In such an event, the electrical resistance of the negative electrode active material can be reduced, while the expansion stress involved in charging can be relieved at the same time. The carbon-based negative electrode material may comprise, for example, at least one selected from the group consisting of natural graphite, synthetic graphite, soft carbon, hard carbon, mesocarbon, carbon fibers, carbon nanotubes, pyrolytic carbon, coke, glass carbon fibers, sintered organic high molecular compounds, and carbon black.” Lee [0230])
Regarding claim 10, modified Lee teaches all of the elements of claim 1, as shown above. Lee teaches all of the additional elements of claim 10:
A lithium secondary battery comprising the negative electrode as defined in claim 1. (“The present invention may provide a negative electrode comprising the negative electrode active material and a secondary battery comprising the same.” Lee [0233])
Regarding claim 11, modified Lee teaches all of the elements of claim 1, as shown above. Lee teaches the following elements of claim 11:
an amount of the graphene coating layer is 1.0 wt% to 9.7 wt% based on a total weight of the negative electrode active material, (“The content of carbon (C) in the second carbon layer may preferably be 3% by weight to 20% by weight, more preferably, 3% by weight to 15% by weight, even more preferably, 3% by weight to 10% by weight, based on the total weight of the silicon-based-carbon composite.” Lee [0097] and “The second carbon layer according to an embodiment of the present invention may be reduced graphene oxide having particularly high electrical conductivity.” Lee [0116] and “A negative electrode and a battery (coin cell) comprising the silicon-based-carbon composite (composite E1) of a core-shell structure as a negative electrode active material were fabricated.” Lee [0259])
The examiner takes note of the fact that the prior art range of 3-20 wt % for the amount of graphene based on the total weight of the negative electrode active material layer overlaps the claimed range of 1-9.7 wt % for the same parameter. Absent any additional and more specific information in the prior art, a prima facie case of obviousness exists. In re Peterson, 315 F.3d 1325, 1330, 65 USPQ2d 1379 (Fed. Cir. 2003). MPEP 2144.05.
Lee is silent on the following elements of claim 11:
The negative electrode according to claim 1, wherein the graphene present in the graphene coating layer has a D/G band intensity ratio of 0.8 to 1.32,
and an amount of the single-walled carbon nanotubes is 0.04 wt% to 0.06 wt% based on a total weight of the negative electrode active material layer.
Son teaches the following elements of claim 11:
The negative electrode according to claim 1, wherein the graphene present in the graphene coating layer has a D/G band intensity ratio of 0.8 to 1.32, (“The coating of graphene on the silicon oxide (SiOx) by vapor deposition may form a coating layer having high crystallinity on the composite.” Son [0148]) and “The graphene may have a degree of crystallinity of about 0.5 to about 1.5, for example, about 1.055 to about 1.146, or about 1.06 to about 1.14. The degree of crystallinity (or degree of disordering of graphene crystals) of the graphene may be obtained by measuring an intensity ratio of D peak to G peak (D/G) in a Raman spectra of the composite.” Son [0086-0087])
The examiner takes note of the fact that the prior art range of ------0.5-1.5 for the D/G ratio in the graphene coating encompasses the claimed range of 0.8-1.32 for the same parameter. Absent any additional and more specific information in the prior art, a prima facie case of obviousness exists. In re Peterson, 315 F.3d 1325, 1330, 65 USPQ2d 1379 (Fed. Cir. 2003). MPEP 2144.05.
Lee and Son are silent on the following elements of claim 11:
and an amount of the single-walled carbon nanotubes is 0.04 wt% to 0.06 wt% based on a total weight of the negative electrode active material layer.
However, Lee II teaches all of the elements of claim 11 not found in Lee or Son:
and an amount of the single-walled carbon nanotubes is 0.04 wt% to 0.06 wt% based on a total weight of the negative electrode active material layer. (“97.45 wt % of artificial graphite, 1.5 wt % of styrene butadiene rubber, 0.05 wt % of an SWCNT conductive agent of Table 1, and 1 wt % of carboxymethyl cellulose were mixed in water to prepare negative active material slurry.” Lee [0115]. The 0.05% by weight of SWCNT anticipates the claimed range, see above arguments for why the composition of the slurry is considered analogous to the composition of the negative electrode active material.)
Conclusion
The following references were discovered in an updated search and were considered to be relevant but were not used in rejection:
Shin (US 20200235383 A1)—teaches a negative electrode which includes an Mg-containing silicon oxide and a carbonaceous material in a weight ratio which encompasses the claimed range.
Any inquiry concerning this communication or earlier communications from the examiner should be directed to BENJAMIN ELI KASS-MULLET whose telephone number is (571)272-0156. The examiner can normally be reached Monday-Friday 8:30am-6pm except for the first Friday of bi-week.
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/BENJAMIN ELI KASS-MULLET/Examiner, Art Unit 1752
/NICHOLAS A SMITH/Supervisory Primary Examiner, Art Unit 1752
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