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 .
Response to Arguments
Applicant's arguments filed 05/29/2026 have been fully considered but they are not persuasive.
Applicant argues that Qu provides a molar ratio of silicon source to lithium-containing source of 1:1.2-1:3 (see e.g., Qu; [0028], [0057]), which does not correspond with the claimed molar ratio m of element silicon to element lithium of 1≤m≤5 because Qu provides this molar ratio as the starting materials and phases and not as the final silicon-based material. However, the molar ratio of the silicon to the lithium as provided by Qu remain the same from the precursor materials to the final silicon-based material. Qu discloses that the materials with the predetermined molar ratios or calcined, cooled, and immersed in hydrophobic solution (see e.g., Qu; [0057], [0072]). However, none of the method steps of calcining, cooling, or immersing in a solution would change the molar ratio of the silicon to the lithium. Therefore, the molar ratio of silicon to lithium as provided the Qu does overlap with the claimed ratio of the final silicon-based material as claimed.
Applicant submits that Akira does not disclose that the final material provides the claimed molar ratio, and further argues that Akira provides contradictory teaches with Qu. These arguments are moot because Akira is no longer used in the rejection below. Qu is newly combined with Morigaki (US-20040234856-A1), Yan (WO-2020151093-A1) (see equivalent US-20220048774-A1 for translation), and as before, Liu (US-20200161635-A1).
Claim Rejections - 35 USC § 103
In the event the determination of the status of the application as subject to AIA 35 U.S.C. 102 and 103 (or as subject to pre-AIA 35 U.S.C. 102 and 103) is incorrect, any correction of the statutory basis (i.e., changing from AIA to pre-AIA ) for the rejection will not be considered a new ground of rejection if the prior art relied upon, and the rationale supporting the rejection, would be the same under either status.
The following is a quotation of 35 U.S.C. 103 which forms the basis for all obviousness rejections set forth in this Office action:
A patent for a claimed invention may not be obtained, notwithstanding that the claimed invention is not identically disclosed as set forth in section 102, if the differences between the claimed invention and the prior art are such that the claimed invention as a whole would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to which the claimed invention pertains. Patentability shall not be negated by the manner in which the invention was made.
The factual inquiries for establishing a background for determining obviousness under 35 U.S.C. 103 are summarized as follows:
1. Determining the scope and contents of the prior art.
2. Ascertaining the differences between the prior art and the claims at issue.
3. Resolving the level of ordinary skill in the pertinent art.
4. Considering objective evidence present in the application indicating obviousness or nonobviousness.
This application currently names joint inventors. In considering patentability of the claims the examiner presumes that the subject matter of the various claims was commonly owned as of the effective filing date of the claimed invention(s) absent any evidence to the contrary. Applicant is advised of the obligation under 37 CFR 1.56 to point out the inventor and effective filing dates of each claim that was not commonly owned as of the effective filing date of the later invention in order for the examiner to consider the applicability of 35 U.S.C. 102(b)(2)(C) for any potential 35 U.S.C. 102(a)(2) prior art against the later invention.
Claim(s) 1-2, 5-7, 9, 22-24 is/are rejected under 35 U.S.C. 103 as being unpatentable over Qu (CN-111710845-A) (see translation), and in further view of Morigaki (US-20040234856-A1), Yan (WO-2020151093-A1) (see equivalent US-20220048774-A1 for translation), and
Liu (US-20200161635-A1).
Regarding claim 1, Qu discloses a secondary battery comprising a positive-electrode plate, a negative-electrode plate, a separator disposed between the positive-electrode plate and the negative-electrode plate, and an electrolyte (see e.g., Qu; [0111]-[0116], wherein the examples provide a test battery provides the lithium metal counter electrode corresponding to the positive-electrode plate, the negative electrode and active material, a PP/PE separator, and EC, DEC, DMC electrolyte mixture), wherein the negative-electrode plate comprises a negative-electrode current collector and a negative-electrode film layer provided on at least one surface of the negative-electrode current collector (see e.g., Qu; [0111], regarding the example in which the negative electrode active material is coated on a copper foil), the negative-electrode film layer comprises a silicon-based material, the silicon-based material comprising a core structure and a coating layer provided on at least partial surface of the core structure (see e.g., Qu; [0015], regarding the silicon-oxygen composite corresponding to the core structure and a carbon layer formed on the surface corresponding to a coating layer), wherein the core structure comprises both a silicon phase and a lithium metasilicate phase (see e.g., Qu; [0009] [0010], regarding lithium composite particle comprising of lithium silicate and a non-metallic silicon-containing material such as nano-silicon, [0081], regarding example 1 in which nano-silicon and silicon oxide is included), the lithium metasilicate phase comprises at least Li4SiO4 (see e.g., Qu; [0011]-[0012] regarding the lithium silicate as Li4SiO4 so that the electrode material can still have a high capacity after pre-lithiation, [0070]-[0072], regarding the example with Li4SiO4), in the silicon-based material, a molar ratio m of element silicon to element lithium is 1:1.2-1.3 (see e.g., Qu; [0028], [0057], [0072], [0080], [0086], [0092]), which falls within the claimed range of 1≤m≤5, and the coating layer is made of carbon (see e.g., Qu; [0044]-[0045], [0056]-[0057], [0073]) which corresponds with the claimed at least one of carbon-based material, organic polymer, metal, and metal oxide.
Qu discloses a crystal grain size of the Li4SiO4 may be below 60 nm (see e.g., Qu; [0015]), and provides examples with the grain size of the Li4SiO4 to be 500 nm (see e.g., Qu; [0073]), 80 nm (see e.g., Qu; [0081]), 20 nm (see e.g., Qu; [0087]), and 210 nm (see e.g., Qu; [0093]). Qu does not explicitly disclose a particle size P of the lithium metasilicate phase is 40nm < P ≤ 500nm. However, Morigaki discloses a lithium ion battery wherein the negative electrode may comprise of lithium-containing oxide selected from a group of materials including Li4SiO4 (see e.g., Morigaki; [0016]), wherein the particle size of the lithium oxide is 0.01 to 0.5 μm (see e.g., Morigaki; [0013], [0024], [0039]), and provides examples wherein the particle size of Li4SiO4 of 0.01 μm to 0.8 μm, including 0.04 μm, 0.2 μm, and 0.5 μm (see e.g., Morigaki; [0103], table 9), which overlaps with the claimed particle size P of the lithium metasilicate phase is 40nm < P ≤ 500nm. Therefore, it would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the Li4SiO4 particles as disclosed by Qu to have a particle size of 0.01 to 0.5 μm as disclosed by Morigaki in order to uniformly disperse particles, prevent the reduction of the transport of lithium ions, and provide high utilization rate (see e.g., Morigaki; [0039], [0103], table 9).
Qu discloses a grain size of the nano-silicon is below 10nm (see e.g., Qu; [0024]), an example in which the grain size of the nano-silicon is 8.8 nm (see e.g., Qu; [0073]), 5 nm (see e.g., Qu; [0081]), 3 nm (see e.g., Qu [0087]), and 7 nm (see e.g., Qu; [0093]). Qu does not explicitly disclose, a particle size Q of the silicon phase is 50nm ≤ Q ≤ 300nm. However, Yan discloses wherein the particle size of nano-silicon may be 5-300 nm and most preferably 10-100 nm (see e.g., Yan; [0009]), and further provides an examples wherein the nano-silicon is 50 nm (see e.g., Yan; [0035]) and 100 nm (see e.g., Yan; [0038], [0038], [0040]), which overlaps with the claimed range of the particle size Q of the silicon phase is 50nm ≤ Q ≤ 300nm. Yan is further analogous art because Yan provides that the anode material is a silicon-carbon composite comprising a carbon coating layer (see e.g., Yan; [0007]). It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have had the silicon phase material of Qu to be 5-300 nm as disclosed by Yan in order to provide high first-cycle efficiency, low expansion, long cycle life, improved cycle, conductivity and rate performance (see e.g., Yan; [0005]).
Modified Qu above with Morigaki and Yan therefore also teaches that the silicon-based material satisfies 1.2 ≤ Q/P ≤ 3.3.
Qu does not explicitly disclose a thickness of the coating layer is ≤ 30nm. However, Liu discloses a coating layer having a thickness of 2 nm to 5 nm, and particularly 2 nm to 3nm (see e.g., Liu; [0017], [0045]), which overlaps with the claimed range of ≤30nm. Liu is further analogous art because Liu discloses the coating layer is also carbon material (see e.g., Liu; [0045]), the particle being coated is also a silicon-based material (see e.g., Liu; [0007]), and the particle is used in lithium-ion batteries (see e.g., Liu; [0003]). Therefore, it would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the thickness of the carbon coating layer disclosed by Qu to be 2nm to 5nm as disclosed by Liu. One of ordinary skill in the art would have been motivated to make this modification in order to seal the surface of the particle (see e.g., Liu; [0045]), increase the overall conductivity, improve mechanical strength, and makes high pressure electrode calendaring viable (see e.g., Liu; [0038]).
Regarding claim 2, modified Qu teaches the secondary battery according to claim 1. As above in claim 1, Qu modified with Morigaki provides a particle size which overlaps with the claimed particle size P of the lithium metasilicate phase is 40nm < P ≤ 100nm.
Regarding claim 5, modified Qu teaches the secondary battery according to claim 1. As above in claim 1, Qu provides a molar ratio of silicon to lithium that falls within the claimed range of 1≤m≤3.
Regarding claim 6, modified Qu teaches the secondary battery according to claim 1. Qu does not explicitly disclose a median particle size by volume Dv50 of the silicon-based material is ≤10 μm. However, Yan discloses a particle size of the silicon composite material is 2-20 μm, and more preferably 2-10 μm (see e.g., Yan; [0008]). It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have had the silicon-based material of Qu have a particle size D50 of 2-10 μm as disclosed by Yan in order to provide high first-cycle efficiency, low expansion, long cycle life, improved cycle, conductivity and rate performance (see e.g., Yan; [0005]).
Regarding claim 7, modified Qu teaches the secondary battery according to claim 1. Qu does not explicitly disclose a specific surface area of the silicon-based material is 0.5 m2/g-3m2/g. However, Yan discloses that the specific surface area of a silicon-carbon composite material is 1-30 m2/g, and more preferably 2-8 m2/g (see e.g., Yan; [0008]), which overlaps with the claimed ranged of 0.5-3 m2/g. It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have had the particle of Qu to have a specific surface area of 0.5-3 m2/g as disclosed by Yan in order to provide high first-cycle efficiency, low expansion, long cycle life, improved cycle, conductivity and rate performance (see e.g., Yan; [0005]).
Regarding claim 9, modified Qu teaches the secondary battery according to claim 1, wherein the lithium metasilicate phase comprises Li4SiO4 (see e.g., Qu; [0009]), which overlaps with the claimed lithium silicate options.
Regarding claim 22, modified Qu teaches the silicon-based material according to claim 9, wherein the lithium metasilicate phase comprises Li4SiO4 (see e.g., Qu; [0009]).
Regarding claim 23, modified Qu teaches the secondary battery according to claim 1, wherein the coating layer comprises the carbon-based material (see e.g., Qu; [0044], [0081], [0087]). Qu discloses that the carbon layer is formed by cracking carbon (see e.g., Qu; [0017]), which can make the claimed carbon nanotube, carbon fiber, or graphene materials. Qu does not explicitly disclose that cracking carbon does form these materials. However, Yan discloses wherein the carbon coating of a particle may be carbon nanotubes or graphene (see e.g., Yan; [0009]). It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have modified had the carbon layer disclosed by Qu form a carbon nanotube or graphene carbon layer as disclosed by Yan in order to provide high first-cycle efficiency, low expansion, long cycle life, improved cycle, conductivity and rate performance (see e.g., Yan; [0005]).
Regarding claim 24, modified Qu teaches the secondary battery according to claim 1. Qu discloses that the coating layer comprises a hydrophobic layer (see e.g., Qu; [0019]-[0022]). Qu does not explicitly disclose wherein the coating layer comprises the organic polymer, the organic polymer comprises polyacrylonitrile. However, Yan discloses wherein the coating layer comprises an organic carbon which may include polyacrylonitrile (see e.g., Yan; [0019]). It would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the coating layer of Qu by providing an organic polymer comprising polyacrylonitrile in order to provide high first-cycle efficiency, low expansion, long cycle life, improved cycle, conductivity and rate performance (see e.g., Yan; [0005]).
Claim(s) 8 is/are rejected under 35 U.S.C. 103 as being unpatentable over Qu (CN-111710845-A) (see translation), Morigaki (US-20040234856-A1), Yan (WO-2020151093-A1) (see equivalent US-20220048774-A1 for translation), and Liu (US-20200161635-A1), and in further view of Behan (US-20170033353-A1).
Regarding claim 8, modified Qu teaches the secondary battery according to claim 1. Qu does not explicitly disclose a powder tap density of the silicon-based material is 0.6g/cm3- 1.2g/cm3, or, a powder press density of the silicon-based material is 1.0g/cm3-1.5g/cm3. However, Behan discloses a tap density of a silicon-based material of greater than 0.07 g/mL, which may be about 0.07 g/mL to 1.0 g/mL (see e.g., claim 11, [0053]) which overlaps with the claimed range of 0.6g/cm3-1.2g/cm3. Behan is equivalent analogous art because Behan similarly teaches the hybrid material comprises a crystalline silicon with the formula MxSiO2+x wherein M is a metal (see e.g., Behan; [0008], claim 11) with an overlapping particle size of less than 45 um, or 1 um to 10 um, or a bimodal distribution with particles of size 10nm to 500 nm (see e.g., Behan; [0008]), and to be provided in a lithium ion secondary battery. Therefore, it would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the silicon-based material disclosed by Qu by providing a powder tap density of greater than 0.07 g/mL, which may be about 0.07 g/mL to 1.0 g/mL, as disclosed by Behan. One of ordinary skill in the art would have been motivated to make this modification in order to structurally stabilize silicon against multiple volume expansions (see e.g., Behan; [0006]), and to achieve the desired packing of the particles during coating and handling (see e.g., Behan; [0053]).
Claim(s) 20-21 is/are rejected under 35 U.S.C. 103 as being unpatentable over Qu (CN-111710845-A) (see translation), Morigaki (US-20040234856-A1), Yan (WO-2020151093-A1) (see equivalent US-20220048774-A1 for translation), and Liu (US-20200161635-A1), and in further view of Koh (US-20190058218-A1).
Regarding claim 20, modified Qu teaches the elements of claim 19 as described above. Qu does not explicitly disclose a battery module. However, Koh discloses a battery module (see e.g., Koh; [0133]). Koh is equivalent analogous art because Koh similarly teaches a lithium ion secondary battery in which the negative active material may include silicon, such as silicon particles and silicon oxide or a combination thereof (see e.g., Koh; [0107]). Therefore, it would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the secondary battery disclosed by Qu by providing them within a battery module disclosed by Koh. One of ordinary skill in the art would have been motivated to make this modification in order to provide a battery module to be included into a battery pack for applications such as a power tool or an electric vehicle (see e.g., Koh; [0134]).
Regarding claim 21, modified Qu teaches the elements of claim 20 as described above. Qu does not explicitly disclose a battery pack. However, Koh discloses a battery pack (see e.g., Koh; [0133]-[0144]). Therefore, it would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the secondary battery module disclosed by modified Qu by further providing them within a battery pack disclosed by Koh. One of ordinary skill in the art would have been motivated to make this modification in order to provide a battery pack for applications such as a power tool or an electric vehicle (see e.g., Koh; [0134]).
Claim(s) 25-26 is/are rejected under 35 U.S.C. 103 as being unpatentable over Qu (CN-111710845-A) (see translation), Morigaki (US-20040234856-A1), Yan (WO-2020151093-A1) (see equivalent US-20220048774-A1 for translation), and Liu (US-20200161635-A1), and in further view of Cho (US-20140234714-A1).
Regarding claim 25, modified Qu teaches the secondary battery according to claim 1. Qu does not explicitly disclose wherein the coating layer comprises a metal, the metal comprising at least one of Cu and Ni. However, Cho discloses a coating layer wherein the coating layer may comprise of a metal oxide (see e.g., Cho; [0030]-[0031]), the metal oxide may be a copper or nickel oxide (see e.g., Cho; [0032]-[0035]). Cho is further analogous art because Cho discloses that the coating layer also includes a carbon material (see e.g., Cho; [0029]), and wherein the particle core may include silicon-based materials (see e.g., Cho; [0056]). Therefore, it would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the coating layer of Qu to include a metal oxide such as copper or nickel oxide as disclosed by Cho in order to improve capacity characteristics and cycle lifetime (see e.g., Cho; [0010]).
Regarding claim 26, modified Qu teaches the secondary battery according to claim 1. Qu does not explicitly disclose wherein the coating layer comprises the metal oxide, the metal oxide comprises at least one of TiO2 and Al2O3. However, Cho discloses a coating layer wherein the coating layer may comprise of a metal oxide (see e.g., Cho; [0030]-[0031]), the metal oxide may be an aluminum oxide (Al2O3) or a titanium oxide (TiO2) (see e.g., Cho; [0032]-[0035]). Cho is further analogous art because Cho discloses that the coating layer also includes a carbon material (see e.g., Cho; [0029]), and wherein the particle core may include silicon-based materials (see e.g., Cho; [0056]). Therefore, it would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the coating layer of Qu to include a metal oxide such as aluminum oxide or titanium oxide as disclosed by Cho in order to improve capacity characteristics and cycle lifetime (see e.g., Cho; [0010]).
Claim(s) 27 is/are rejected under 35 U.S.C. 103 as being unpatentable over Qu (CN-111710845-A) (see translation), Morigaki (US-20040234856-A1), Yan (WO-2020151093-A1) (see equivalent US-20220048774-A1 for translation), and Liu (US-20200161635-A1), and in further view of Cui (US-20150099187-A1).
Regarding claim 27, modified Qu teaches the secondary battery according to claim 1. Qu does not explicitly disclose wherein the coating layer comprises resorcinol. However, Cui discloses wherein the coating layer is formed using resorcinol (see e.g., Cui; [0015], [0047], [0053], [0074], [0094], [0102], [0121]-[0123]). Cui is further analogous art because Cui discloses that the core of the particle may comprise of silicon (see e.g., Cui; [0007], [0010], [0094]). Therefore, it would have been obvious for one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the coating layer disclosed by Qu to comprise of resorcinol as disclosed by Cui in order to diffuse into inner space to provide a thicker coating which results in thick carbon at the surface to fill the packing gap and block the electrolyte, while the interior includes thin carbon to conduct Li and e− while keeping the Si content in the composite as high as possible (see e.g., Cui; [0053]).
Conclusion
THIS ACTION IS MADE FINAL. 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.
Any inquiry concerning this communication or earlier communications from the examiner should be directed to KEVIN SONG whose telephone number is (571)270-7337. The examiner can normally be reached Monday - Friday 9:00 am - 5:00 pm EST.
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/KEVIN SONG/Examiner, Art Unit 1728
/MATTHEW T MARTIN/Supervisory Patent Examiner, Art Unit 1728
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