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and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114.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 May 20, 2025 has been entered.
Response to Amendment
Applicant’s amendments filed on April 25, 2025 have been entered. Claims 1, 5, and 13 have been amended; support for the amendments can be found at least in Figure 7. Claim 8 has been cancelled. Claims 1-7 and 9-17 remain pending and have been examined on their merits in this office action.
Response to Arguments
Applicant’s arguments filed on April 25, 2025 have been fully considered. Applicant’s arguments with respect to independent claims 1 and 13 have been considered but are moot because of a new ground of rejection presented in view of the amendments.
Claim Rejections - 35 USC § 112
The previous 112(b) rejections in the Final Rejection dated March 10, 2025 are withdrawn in view of Applicant’s amendments.
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.
Claims 1-7, 11-14, and 16-17 are rejected under 35 U.S.C. 103 as being unpatentable over Lee et al. (Published U.S. Patent Application US 20100273058 A1) in view of Ma et al. (CN 103824999 A), hereinafter referred to as Lee and Ma.
Regarding claim 1, Lee teaches a negative active material for a rechargeable lithium battery (see e.g., Abstract). Lee teaches the negative active material includes a first particle precursor, a flake-shaped graphite piece (“a carbon material”), and a second particle comprising Si (“silicon particles”) dispersed between the flake-shaped graphite pieces inside the sphere-shaped first graphite particle (“wherein the carbon material encompasses the silicon particles in a bulk particle”) (see e.g., Figure 1 and paragraphs [0025]-[0026]).
Lee does not explicitly teach wherein the silicon particles from the surface of the anode active material to a point of 50% of the radius toward the center from the surface of the anode active material are included in an amount of 45 mass% to 55 mass% with respect to the anode active material in the volume of anode active material from the surface of the anode active material to a point of 50% of the radius toward the center from the surface of the anode active material, and wherein the silicon particles from the center of the anode active material to a point of 50% of the radius toward the surface from the center of the anode active material are included in an amount greater than zero and less than 45 mass% with respect to the anode active material in the volume of the anode active material from the center of the anode active material to a point of 50% of the radius toward the surface from the center of the anode active material.
However, Ma teaches a negative electrode active material with a two-layer composite structure, wherein a first layer near the current collector side is composed of a carbon material and a first material and a second layer away from the current collector side (see e.g., paragraph [0017]). Ma teaches the first material is selected from at least one of elemental silicon and silicon-containing compounds (see e.g., paragraph [0022]). Ma teaches the content of carbon material and first material (silicon) in the first layer is distributed in a gradient along the thickness direction of the lithium battery negative electrode, and the content of carbon material is higher closer to the current collector and the content of first material is lower closer to the current collector (see e.g., paragraph [0025]). Ma teaches the content of the first material in the first layer gradually increases from 0.1-2 wt% near the current collector side (“wherein the silicon particles from the surface of the anode active material to a point of 50% of the radius toward the center from the surface of the anode active material are included in an amount of 45 mass% to 55 mass% with respect to the anode active material in the volume of anode active material from the surface of the anode active material to a point of 50% of the radius toward the center from the surface of the anode active material”) to 20-60 wt% near the second layer side (“wherein the silicon particles from the center of the anode active material to a point of 50% of the radius toward the surface from the center of the anode active material are included in an amount greater than zero and less than 45 mass% with respect to the anode active material in the volume of the anode active material from the center of the anode active material to a point of 50% of the radius toward the surface from the center of the anode active material”) (see e.g., paragraph [0025]). Ma teaches the gradient of the silicon content and its inverse for the carbon material content effectively alleviate the problem of decreased cycle performance (see e.g., paragraph [0022]) by accommodating large volume changes due to the volume expansion and contraction of silicon during cycling (see e.g., paragraph [0020]).
Therefore, it would have been obvious before the effective filing date of the claimed invention that one of ordinary skill would modify the negative active material comprising carbon and silicon of Lee to distribute the silicon material along a gradient with 0.1-2 wt% at the center to 20-60 wt% along the outside, as taught by Ma, in order to effectively alleviate the problem of decreased cycle performance (see e.g., paragraph [0022]) by accommodating large volume changes due to the volume expansion and contraction of silicon during cycling (see e.g., paragraph [0020]).
It has been held in the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art,” and because the 0.1-2wt % overlaps with the recited range of 0-45 mass % and the 20-60 wt% overlaps with the recited range of 45-55 mass %, a “prima facie” case of obviousness exists (see MPEP 2144.05(l)).
Regarding claim 2, Lee, as modified by Ma, teaches the instantly claimed invention of claim 1, as previously described.
Lee teaches the first particle precursor is a flake-shaped graphite (“natural graphite”) (see e.g., paragraph [0043]) and can also include expanded graphite (“expanded graphite”) (see e.g., paragraph [0061]).
Regarding claim 3, Lee, as modified by Ma, teaches the instantly claimed invention of claim 1, as previously described.
Lee teaches the negative active material may include the second particle (“silicon particles”) in a range of 1 to 70 wt % based on the entire weight of the sphere-shaped first graphite particle. For example, Lee teaches the first particle precursor (“carbon material” and Si particles were mixed in a weight ratio of 70:30 (“wherein a weight ratio of the silicon particles to the carbon material ranges from 2:8 to 4:6) (see e.g., Example 3).
Regarding claim 4, Lee, as modified by Ma, teaches the instantly claimed invention of claim 1, as previously described.
Lee teaches the negative active material may include the second particle (“silicon particles”) in a range of 1 to 70 wt % based on the entire weight of the sphere-shaped first graphite particle (“wherein a mass ratio of the carbon material to the silicon particles is 45 to 55: 55 to 45”).
It has been held in the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art,” and because the second particle in a range of 1 to 70 wt % based on the entire weight of the sphere-shaped first graphite particle overlap with the recited range, a “prima facie” case of obviousness exists (see MPEP 2144.05(l)).
Regarding claim 5, Lee, as modified by Ma, teaches the instantly claimed invention of claim 1, as previously described.
Lee teaches the negative active material may include the second particle (“silicon particles”) in a range of 1 to 70 wt % based on the entire weight of the sphere-shaped first graphite particle (“the silicon particles are in an amount of 55 by mass or less of the anode active material”).
It has been held in the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art,” and because the second particle in a range of 1 to 70 wt % based on the entire weight of the sphere-shaped first graphite particle overlap with the recited range, a “prima facie” case of obviousness exists (see MPEP 2144.05(l)).
Regarding claim 6, Lee, as modified by Ma, teaches the instantly claimed invention of claim 1, as previously described.
Lee teaches the negative active material has an average particle diameter of 20 µm (an average particle radius of 10 µm) (“the anode active material has a radius of 12 µm or lower”) (see e.g., Comparative Example 2). Lee teaches the negative active material may include the second particle (“silicon particles”) in a range of 1 to 70 wt % based on the entire weight of the sphere-shaped first graphite particle (“the silicon particles are in an amount of 45 mass% to 55 mass%”).
It has been held in the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art,” and because the second particle in a range of 1 to 70 wt % based on the entire weight of the sphere-shaped first graphite particle overlap with the recited range, a “prima facie” case of obviousness exists (see MPEP 2144.05(l)).
Regarding claim 7, Lee, as modified by Ma, teaches the instantly claimed invention of claim 1, as previously described.
Lee teaches the negative active material has an average particle diameter of 25 µm (an average particle radius of 12.5) (“the anode active material has a radius of 12 µm to 18 µm”) (see e.g., Example 1).
As previously described in claim 1, Ma teaches the content of carbon material and first material (silicon) in the first layer is distributed in a gradient along the thickness direction of the lithium battery negative electrode, and the content of carbon material is higher closer to the current collector and the content of first material is lower closer to the current collector (see e.g., paragraph [0025]). Ma teaches the content of the first material in the first layer gradually increases from 0.1-2 wt% near the current collector side (“wherein the silicon particles from the surface of the anode active material to a point of 70% of the radius toward the center from the surface of the anode active material are included in an amount of 45 mass% to 55 mass% with respect to the anode active material in the volume of anode active material from the surface of the anode active material to a point of 70% of the radius toward the center from the surface of the anode active material”) to 20-60 wt% near the second layer side (“wherein the silicon particles from the center of the anode active material to a point of 30% of the radius toward the surface from the center of the anode active material are included in an amount greater than zero and less than 45 mass% with respect to the anode active material in the volume of the anode active material from the center of the anode active material to a point of 30% of the radius toward the surface from the center of the anode active material”) (see e.g., paragraph [0025]). Ma teaches the gradient of the silicon content and its inverse for the carbon material content effectively alleviate the problem of decreased cycle performance (see e.g., paragraph [0022]) by accommodating large volume changes due to the volume expansion and contraction of silicon during cycling (see e.g., paragraph [0020]).
Therefore, it would have been obvious before the effective filing date of the claimed invention that one of ordinary skill would modify the negative active material comprising carbon and silicon of Lee to distribute the silicon material along a gradient with 0.1-2 wt% at the center to 20-60 wt% along the outside, as taught by Ma, in order to effectively alleviate the problem of decreased cycle performance (see e.g., paragraph [0022]) by accommodating large volume changes due to the volume expansion and contraction of silicon during cycling (see e.g., paragraph [0020]).
It has been held in the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art,” and because the 0.1-2wt % overlaps with the recited range of 0-45 mass % and the 20-60 wt% overlaps with the recited range of 45-55 mass %, a “prima facie” case of obviousness exists (see MPEP 2144.05(l)).
Regarding claim 11, Lee, as modified by Ma, teaches the instantly claimed invention of claim 1, as previously described.
Lee teaches the Si particles have a particle diameter of about 70 nm (“wherein the silicon particles have an average diameter of 50 nm to 120 nm”) (see e.g., Example 1).
Regarding claim 12, Lee, as modified by Ma, teaches the instantly claimed invention of claim 1, as previously described.
Lee teaches the negative active material further comprises a coating membrane 13 formed by coating the surface of a sphere-shaped first graphite particle with an amorphous carbon or a soft carbon material (“an outer coating layer outside the anode active material”) (see e.g., paragraph [0053]).
Regarding claim 13, Lee teaches a negative active material for a rechargeable lithium battery (see e.g., Abstract). Lee teaches the negative active material includes a first particle precursor, a flake-shaped graphite piece (“a carbon material”), and a second particle comprising Si (“silicon particles”) dispersed between the flake-shaped graphite pieces inside the sphere-shaped first graphite particle (“wherein the carbon material encompasses the silicon particles in a bulk particle”) (see e.g., Figure 1 and paragraphs [0025]-[0026]). Lee teaches the negative active material is prepared by preparing a first particle precursor, a flake-shaped graphite piece, by exfoliating a flake-shaped graphite, preparing a mixture by mixing the first particle precursor with the second particle, and assembling the mixture (“preparing a mixture powder by mixing a carbon material and silicon particles and mechanically over-mixing the mixture powder”) (see e.g., paragraph [0056]).
Lee does not explicitly teach wherein the silicon particles from the surface of the anode active material to a point of 50% of the radius toward the center from the surface of the anode active material are included in an amount of 45 mass% to 55 mass% with respect to the anode active material in the volume of anode active material from the surface of the anode active material to a point of 50% of the radius toward the center from the surface of the anode active material, and wherein the silicon particles from the center of the anode active material to a point of 50% of the radius toward the surface from the center of the anode active material are included in an amount less than 45 mass% with respect to the anode active material in the volume of the anode active material from the center of the anode active material to a point of 50% of the radius toward the surface from the center of the anode active material.
However, Ma teaches a negative electrode active material with a two-layer composite structure, wherein a first layer near the current collector side is composed of a carbon material and a first material and a second layer away from the current collector side (see e.g., paragraph [0017]). Ma teaches the first material is selected from at least one of elemental silicon and silicon-containing compounds (see e.g., paragraph [0022]). Ma teaches the content of carbon material and first material (silicon) in the first layer is distributed in a gradient along the thickness direction of the lithium battery negative electrode, and the content of carbon material is higher closer to the current collector and the content of first material is lower closer to the current collector (see e.g., paragraph [0025]). Ma teaches the content of the first material in the first layer gradually increases from 0.1-2 wt% near the current collector side (“wherein the silicon particles from the surface of the anode active material to a point of 50% of the radius toward the center from the surface of the anode active material are included in an amount of 45 mass% to 55 mass% with respect to the anode active material in the volume of anode active material from the surface of the anode active material to a point of 50% of the radius toward the center from the surface of the anode active material”) to 20-60 wt% near the second layer side (“wherein the silicon particles from the center of the anode active material to a point of 50% of the radius toward the surface from the center of the anode active material are included in an amount greater than zero and less than 45 mass% with respect to the anode active material in the volume of the anode active material from the center of the anode active material to a point of 50% of the radius toward the surface from the center of the anode active material”) (see e.g., paragraph [0025]). Ma teaches the gradient of the silicon content and its inverse for the carbon material content effectively alleviate the problem of decreased cycle performance (see e.g., paragraph [0022]) by accommodating large volume changes due to the volume expansion and contraction of silicon during cycling (see e.g., paragraph [0020]).
Therefore, it would have been obvious before the effective filing date of the claimed invention that one of ordinary skill would modify the negative active material comprising carbon and silicon of Lee to distribute the silicon material along a gradient with 0.1-2 wt% at the center to 20-60 wt% along the outside, as taught by Ma, in order to effectively alleviate the problem of decreased cycle performance (see e.g., paragraph [0022]) by accommodating large volume changes due to the volume expansion and contraction of silicon during cycling (see e.g., paragraph [0020]).
It has been held in the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art,” and because the 0.1-2wt % overlaps with the recited range of 0-45 mass % and the 20-60 wt% overlaps with the recited range of 45-55 mass %, a “prima facie” case of obviousness exists (see MPEP 2144.05(l)).
Regarding claim 14, Lee, as modified by Ma, teaches the instantly claimed invention of claim 13, as previously described.
Lee teaches that preparing a mixture by mixing the first particle precursor with the second particle and assembling the mixture comprising a rotor mill of a blade method to prepare a sphere-shaped and assembled first graphite-silicon particle by blade-spinning power and frictional power (“wherein the over-mixing mixes by a milling process”) (see e.g., paragraph [0090]).
Regarding claim 16, Lee, as modified by Ma, teaches the instantly claimed invention of claim 1, as previously described.
Lee teaches the negative electrode includes the negative active material (“wherein an anode comprises the anode active material”) (see e.g., paragraph [0083]).
Regarding claim 17, Lee, as modified by Ma, teaches the instantly claimed invention of claim 16, as previously described.
Lee teaches the negative electrode includes the negative active material (“the anode of claim 16”) (see e.g., paragraph [0083]). Lee teaches the positive electrode includes a positive active material (“a cathode comprising a cathode active material”) (see e.g., paragraph [0084]). Lee teaches a separator is further interposed between the positive electrode and the negative electrode (“a separator interposed between the anode and the cathode”) (see e.g., paragraph [0088]).
Claims 9-10 are rejected under 35 U.S.C. 103 as being unpatentable over Lee et al. (Published U.S. Patent Application US 20100273058 A1) in view of Ma et al. (CN 103824999 A), and further in view of Misaki et al. (JP 2018170246 A), hereinafter referred to as Misaki.
Regarding claim 9, Lee, as modified by Ma, teaches the instantly claimed invention of claim 1, as previously described.
Lee, as modified by Ma, does not explicitly teach the anode active material has a porosity of 1% to 7%.
However, Misaki teaches a composite active material for a lithium secondary battery that include Si or Si alloy and graphite (see e.g., Abstract). Misaki teaches the composite active material has a porosity (a void formed between the Si and graphite layer) of 2 to 50% (see e.g., paragraph [0012]). Misaki teaches the porosity of the composite active material suppresses volume expansion even after repeated charging and discharging and exhibits excellent cycle characteristics (see e.g., paragraph [0013]).
Therefore, it would have been obvious before the effective filing date of the claimed invention that one of ordinary skill would modify the negative active material comprising carbon and silicon of Lee, as modified by Ma, to have a porosity of 2 to 50%, as taught by Misaki, in order to suppress volume expansion of the composite active material even after repeated charging and discharging and exhibit excellent cycle characteristics (see e.g., paragraph [0013]).
It has been held in the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art,” and because the porosity of 2 to 50% overlaps with the recited range, a “prima facie” case of obviousness exists (see MPEP 2144.05(l)).
Regarding claim 10, Lee, as modified by Ma and Misaki, teaches the instantly claimed invention of claim 9, as previously described.
As previously described in claim 9, Misaki teaches the porosity is defined as a void formed between the Si and graphite layer (see e.g., paragraph [0012]).
Claim 15 is rejected under 35 U.S.C. 103 as being unpatentable over Lee et al. (Published U.S. Patent Application US 20100273058 A1) in view of Ma et al. (CN 103824999 A), and further in view of Senna et al. (JP 2004213927 A), hereinafter referred to as Senna.
Regarding claim 15, Lee, as modified by Ma, teaches the instantly claimed invention of claim 14, as previously described.
Lee, as modified by Ma, does not explicitly teach a milling speed of the milling process ranges from 2000 to 6000 rpm, and the milling process is performed for 30 minutes to 480 minutes.
Senna teaches a negative electrode active material comprising a carbonaceous material, a graphite material, and at least one kind of fine nano-metallic particles selected from a group composed of Si (see e.g., Abstract). Senna teaches the rotation of the raw material particles is performed at a rotation speed of 100 rpm or more and 20,000 or less (“a milling speed of the milling process ranges from 2000 to 6000 rpm”) (see e.g., paragraph [0033]). Senna teaches this rotation is carried out for a period of 10 minutes or more and 5 hours or less (“the milling process is performed for 30 minutes to 480 minutes”) (see e.g., paragraph [0033]). Senna teaches the speed and duration is to break down agglomerates of primary metal particles by selectively applying a relative weak impact stress (see e.g., paragraph [0033]).
Therefore, it would have been obvious before the effective filing date of the claimed invention that one of ordinary skill would modify the assembling process of the negative active material of Lee, as modified by Ma, to be performed at a rotation speed of 100 rpm or more and 20,000 or less and carried out for a period of 10 minutes or more and 5 hours or less, as taught by Senna, in order to break down agglomerates of primary metal particles by selectively applying a relative weak impact stress (see e.g., paragraph [0033]).
It has been held in the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art,” and because the rotation speed 100 rpm or more and 20,000 or less and duration of 10 minutes or more and 5 hours or less overlap with the recited ranges, a “prima facie” case of obviousness exists (see MPEP 2144.05(l)).
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to Katherine N Higgins whose telephone number is (703)756-1196. The examiner can normally be reached Mondays - Thursdays 7:30-4:30 EST, Fridays 7:30 - 11:30 EST.
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, Matthew T Martin can be reached at (571) 270-7871. 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.
/KATHERINE N HIGGINS/Examiner, Art Unit 1728
/MATTHEW T MARTIN/Supervisory Patent Examiner, Art Unit 1728