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 .
Election/Restrictions
Claims 6-10 withdrawn from further consideration pursuant to 37 CFR 1.142(b), as being drawn to a nonelected inventions, there being no allowable generic or linking claim. Applicant timely traversed the restriction (election) requirement in the reply filed on 8/14/2026.
Applicant's election with traverse of Group I in the reply filed on 8/14/2026 is acknowledged. The traversal is on the ground(s) that the apparatus of Group II is specially designed, structuralized, and integrated specifically to carry out the multi-stage chemical pre-lithiation, homogenization and passivation process of claim 1. This is not found persuasive since without the process limitations, the apparatus describes a stirred reaction chamber, an inert gas supply, a solvent supply source containing a solvent selected from THF, dimethoxyethane, N-methyl-2-pyrrolidone, and mixtures therebetween, a passivation source supply consisting of hexane mixed with perfluorotripentylamine or a second tetrahydrofuran mixed with hydrofluoric acid, first and second recycling apparatus. Applicant is further reminded that an apparatus claim is limited to the structure of the apparatus (i.e., what a device is, and not what a device does) and is only limited by process limitations insofar as they define structural or functional limitations of the apparatus. See MPEP 2114. Here, the apparatus as claimed can be used for electrophllic fluorination as a process requiring THF and HF as reagents. See for example, Wang et al (Electrophilic fluorination using PhIO/HF-THF reagent”, J Fluorine Chemistry, 240 (2020), 109670, pp. 1-5) which uses a reaction chamber to which HF-THF solution is added and where the mixture is stirred and heated.
Furthermore, the Office notes that the method according to claim 1 could be performed with a materially different apparatus including one without the first and second recycling apparatus required in claim 6.
Applicant also argues that there would be no serious search burden. This is not found persuasive because searching for the process requires the search of specific process steps and conditions and searching for the apparatus of Group II requires searching of the apparatus structural elements and there is a significant divergence requiring different search terms and strategies. Therefore, the Office maintains that there is a significant search burden. Again, Applicant is reminded that an apparatus claim is limited to the structure of the apparatus (i.e., what a device is, and not what a device does) and is only limited by process limitations insofar as they define structural or functional limitations of the apparatus. See MPEP 2114.
The requirement is still deemed proper and is therefore made FINAL.
In response to Applicant’s remarks regarding rejoinder on Page 4-5 of the Office Action, Applicant is reminded that the paragraph reflects an election of the product/apparatus claims (here Group II) and rejoinder of process claims including all limitations of the allowable product/apparatus claims. Applicant has elected the process claims Group I in the reply filed 8/14/2026.
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(d):
(d) REFERENCE IN DEPENDENT FORMS.—Subject to subsection (e), a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
The following is a quotation of pre-AIA 35 U.S.C. 112, fourth paragraph:
Subject to the following paragraph [i.e., the fifth paragraph of pre-AIA 35 U.S.C. 112], a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
Claim 5 is rejected under 35 U.S.C. 112(d) or pre-AIA 35 U.S.C. 112, 4th paragraph, as being of improper dependent form for failing to further limit the subject matter of the claim upon which it depends, or for failing to include all the limitations of the claim upon which it depends. Claim 5 limits the invention to adding a phosphorus or boron in the step of homogenizing the plurality of lithium-containing silicon-based particles. However, Claim 5 depends on claim 1 which limits the step of homogenizing the plurality of lithium-containing silicon-based particles in an inert furnace atmosphere. Therefore, Claim 5 contradicts claim 1 and does not contain all of the limitations of claim 1. Applicant may cancel the claim(s), amend the claim(s) to place the claim(s) in proper dependent form, rewrite the claim(s) in independent form, or present a sufficient showing that the dependent claim(s) complies with the statutory requirements.
Claim Rejections - 35 USC § 103
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) 1-4 is/are rejected under 35 U.S.C. 103 as being unpatentable over Li et al (CN-113437280) in further view of Wang et al (CN112234160) in further view of Zhao et al (“Surface Fluorination of Reactive Battery Anode Materials for Enhanced Stability”, J American Chem. Soc. (2017) 139 (33): 11550-11558) in further view of Yun et al (CN 109155400) and in further view of Li et al (CN 113270587 hereafter cited as Li-2) where citations in this Office Action are from the Machine Translations provided by the Examiner.
Li teaches a preparation method of slurry stable lithiated silicon-based composite material, comprising the following steps:
(1) carbon coating the silicon-based material to obtain the carbon-coated silicon-based material;
(2) mixing the complexing agent, metal lithium and organic solvent uniformly, stirring and dipping under the inert atmosphere to obtain the homogeneous aryl lithium complex solution;
(3) soaking the material obtained in the step (1) in the homogeneous solution obtained in step (2); after finishing dipping, separating to obtain the carbon-coated silicon-based material particles uniformly immersed in lithium;
(4) the particles obtained in the step (3) under the inert atmosphere, low temperature pre-sintering, the temperature is 80-100 ℃, the time is 3-10h;
(5) adding metal precursor or metal compound;
(6) the product obtained in the step (5) under the inert atmosphere, high temperature calcining, the temperature is 500-850 ℃, the time is 1-24h, cooling, grinding;
(7) the grinding product obtained in the step (6) by alcohol treatment, vacuum drying to obtain the coated metal coated silicon-based composite material, namely obtaining the negative electrode material for lithium ion battery stable aqueous slurry (see Contents of Invention, Page 5).
Li further teaches that in a preferred embodiment of the present invention, the specific implementation of the present invention is as follows:
The silicon-based material may be represented by SiOx, wherein 0 <x < 2, preferably 0.8 < x < 1.0;
The complexing agent is polycyclic aromatic compound, specifically selected from the group consisting of biphenyl, 4, 4'-dimethyl-biphenyl, terphenyl, naphthalene, anthracene, phenanthrene, and at least one of tetracene and pentacene, preferably biphenyl, naphthalene;
the organic solvent is ether solvent, the ether solvent is selected from 1, 3-pentane, tetrahydrofuran, diethylene glycol dimethyl ether, ethylene glycol dimethyl ether, methyl tert-butyl ether, butyl methyl ether in the one kind of or combination of several; preferably is 1, 3-pentane, tetrahydrofuran, ethylene glycol dimethyl ether single or multiple mixed ether solvent; most preferably is 1, 3-pentane, tetrahydrofuran;
The concentration of the aromatic lithium in the homogeneous solution is 0.1-3 mol/L, preferably 0.5-2 mol/L. the dipping time is 30-60min
the adding amount of the metal lithium accounts for 5-15wt% carbon-coated silicon-based material obtained in the step (1), in this case, it can improve the lithium ion immersion rate and embedding degree
the metal coating precursor or metal compound in step (5) is selected from metal salt, metal alkoxide, metal oxide and metal hydroxide in the one kind of or more. In the alkaline environment of the lithiated silicon-based negative electrode material, the metal is covered by the film precursor or the metal compound through the alkaline environment, or the compound can be replaced, neutralized, hydrolyzed, dehydrated or complexed and so on, generating uniform and dense metal coated film. the metal element comprises one or more of aluminium, magnesium, zirconium and titanium. The pre-lithiation material caused by the introduction of a large amount of lithium on the surface of the material of the material causes flocculation and gas production of the aqueous slurry, forming a metal coating film in situ, can stabilize the slurry so as to improve the cycle stability (see Contents of the Invention, Page 5-6).
Therefore, Li teaches the preparing step for a plurality of silicon-based anode comprising the same chemical formula (step 1), an immersion step for preparing a plurality of lithium-containing silicon-based particles with the claimed carrier solution and solvent and the first heating step in an inert furnace atmosphere comprising the claimed first temperature and period of time (steps 3-4), a second heating step with overlapping second temperature and period of time (step 6).
Further regarding the second temperature, as cited above, Li teaches a second temperature range of 500 to 850°C. As set forth in MPEP 2144.05, in the case where the claimed range “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). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the method as taught by Li where the second temperature is any workable or optimum range overlapping with 500 to 850°C as taught by Li including the claimed range.
Further regarding the second period of time, as cited above, Li teaches a second period of time from 1 to 24 hours. It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the method as taught by Li where the second period of time is any workable or optimum range overlapping with 1 to 24 hours as taught by Li including the claimed range.
Li does not teach that the mole ratio of lithium source to polycyclic aromatic hydrocarbon is equal or greater than 5, a volume ratio of the solvent to the silicon-based particles is equal or greater than 1.
Li does not teach a method comprising passivation by immersing the homogenized lithium-containing silicon-based particles where the passivation solution consists of a hexane mixed with a perfluorotripentylamine or a second tetrahydrofuran mixed with a hydrofluoric acid, a first weight percentage of the perfluorotripentylamine is equal to or less than 5 wt%, a second weight percentage of the hydrofluoric acid is equal to or less than 10 wt%, the passivation gas is a nitrogen trifluoride or a chlorofluorocarbon(Freon), the third temperature ranges from 30°C to 250°C and the third period of time ranges from 10 minutes to 24 hours.
Regarding the mole ratio of lithium source to polycyclic aromatic hydrocarbon, Wang teaches a method for supplementing lithium to negative electrode active material comprising dispersing lithium metal into a solution comprising polycyclic aromatic organic compound in a solvent then dispersing a silicon-based negative electrode active material in the organic lithium solution (see Contents of the Invention, Page 3). Wang further teaches where the ratio of the amount of substance of lithium metal and polycyclic aromatic organic compound is 0.1-50:1 (see Contents of the Invention, Page 3). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform a method for preparing a lithiated silicon-based composite material that is used in a negative electrode comprising immersing in a lithium-polycyclic aromatic hydrocarbon complex solution as taught by Li where the molar ratio of the lithium metal to the polycyclic aromatic organic compound is in any workable or optimum range overlapping with 0.1-50:1 as taught by Wang including the claimed range since Wang suggests that the ratio is suitable for lithiating electrode material.
Regarding the volume ratio of silicon-based particles and solvent, Wang teaches an example comprising adding 200 g of silicon oxide into 1000 mL of organic lithium solution (see Embodiment 1). Depending on whether the silicon oxide is amorphous or crystalline 200 g of silicon oxide is about 75.5 ml or 91.07 ml and Wang therefore teaches an embodiment where the volume ratio of solvent to the negative electrode material is greater than 1. It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the method as taught by Li comprising immersing in the organic lithium solution in a volume ratio of greater than 1 as taught by Wang since Wang suggests that the volume ratio is suitable for lithiating the electrode material.
Regarding the passivating step, Zhao teaches a process for surface fluorination of a lithium metal or a lithiated silicon for enhanced stability (see Abstract). Zhao teaches a method comprising a fluoropolymer and does not teach immersing in a passivating solution or passivating gas as claimed.
Yun teaches a process for forming a protective film on the lithium metal surface of an electrode layer, the method comprising:
soaking the lithium metal in an acid solution containing HF in an organic solvent;
where the concentration is 3,000 to 10,000 ppm HF (i.e., 0.3 to 1% HF);
the organic solvent may be a carbonate solvent, and the specific examples include selected from the group consisting of propylene carbonate (PC), ethylene carbonate (EC), butylene carbonate (BC), diethyl carbonate (DEC), dimethyl carbonate (DMC); dipropyl carbonate (DPC), methyl propionate (MP), dimethyl sulfoxide, acetonitrile, dimethoxyethane, diethoxyethane, tetrahydrofuran, N-methyl - -2 - pyrrolidone (NMP), methyl carbonate (EMC), gamma-butyrolactone (GBL), fluoro-ethylene carbonate (FEC); methyl formate, ethyl formate, propyl formate, methyl acetate, ethyl acetate, propyl acetate, amyl acetate, methyl propionate, ethyl propionate, propyl propionate, butyl propionate or a combination thereof, halogen derivative, linear ester, linear ether, cyclic ether and so on at least one (see Manufacturing method of cathode, Page 6).
It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the method as taught Li where the lithiated silicon particles are surface fluorinated as taught by Zhao to make the anode material more stable. It also would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the method as taught by Li and Zhao where the surface fluorination uses a passivation solution comprising HF and THF as taught by Yun as a known equivalent for fluorinating Li for passivating electrodes.
Further regarding the third heating step, Li-2 teaches a method of in-situ fluorination constructing a high-stability silicon-based composite material comprising an immersion in a fluorinating agent including HF where after the fluorination step, the silicon-based material is vacuum dried at a temperature of 60-150°C for 8 to 16 hours (see Content of the Invention, Page 4). It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the method of Li as modified by Zhao and Yun where after immersion the silicon-based material is dried at 60-150°C for 8 to 16 hours since Zhao and Yun both teach immersion processes.
Regarding claim 2, as applied above Li teaches where the concentration of the aromatic lithium in the solution is 0.1 to 3 mol/L. It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform the method as taught by modified Li where the concentration of the carrier solution is in any workable or optimum range overlapping with 0.1 to 3 mol/L as taught by Li including the claimed range.
Regarding claim 3, It would have been obvious to one of ordinary skill in the art at the time of filing of the invention to perform a method for preparing a lithiated silicon-based composite material that is used in a negative electrode comprising immersing in a lithium-polycyclic aromatic hydrocarbon complex solution as taught by Li where the molar ratio of the lithium metal to the polycyclic aromatic organic compound is in any workable or optimum range overlapping with 0.1-50:1 as taught by Wang including the claimed range since Wang suggests that the ratio is suitable for lithiating electrode material.
Regarding claim 4, since the surface composition of the anode material as suggested by modified Li would be the same (namely LiF and SiOx@C), one of ordinary skill in the art would reasonably expect that the pH of the particles would be identical.
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to MICHAEL FORREST whose telephone number is (571)270-5833. The examiner can normally be reached Monday-Friday (10AM-6PM).
Examiner interviews are available via telephone, in-person, and video conferencing using a USPTO supplied web-based collaboration tool. To schedule an interview, applicant is encouraged to use the USPTO Automated Interview Request (AIR) at http://www.uspto.gov/interviewpractice.
If attempts to reach the examiner by telephone are unsuccessful, the examiner’s supervisor, Sally A Merkling can be reached at (571)272-6297. The fax phone number for the organization where this application or proceeding is assigned is 571-273-8300.
Information regarding the status of published or unpublished applications may be obtained from Patent Center. Unpublished application information in Patent Center is available to registered users. To file and manage patent submissions in Patent Center, visit: https://patentcenter.uspto.gov. Visit https://www.uspto.gov/patents/apply/patent-center for more information about Patent Center and https://www.uspto.gov/patents/docx for information about filing in DOCX format. For additional questions, contact the Electronic Business Center (EBC) at 866-217-9197 (toll-free). If you would like assistance from a USPTO Customer Service Representative, call 800-786-9199 (IN USA OR CANADA) or 571-272-1000.
/MICHAEL FORREST/Primary Examiner, Art Unit 1738
Prosecution Insights