DETAILED ACTION
Application 18/576,351, “LITHIUM SECONDARY BATTERY AND MANUFACTURING METHOD THEREOF”, was filed with the USPTO on 1/3/2024 and has a foreign priority document of KR10-2022-0075481 filed on 6/21/2022.
This office action is in response to communication filed on 1/3/2024.
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 .
Priority
Acknowledgment is made of applicant’s claim for foreign priority under 35 U.S.C. 119 (a)-(d). The certified copy has been filed in parent Application No. 18/576,351, filed on 1/3/2024.
Information Disclosure Statement
The information disclosure statement (IDS) submitted on 1/3/2024 and 6/26/2025 are in compliance with the provisions of 37 CFR 1.97. Accordingly, the information disclosure statement is being considered by the examiner.
Claim Objections
Claim 3 objected to because the recitation “a polymeric compound” in claim 3 is inconsistent with the specification “a polymerizable compound” (see PGpub [0060] and [0061]). The aforementioned recitation should read “a polymerizable compound”. Appropriate correction is required.
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(b):
(b) CONCLUSION.—The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the inventor or a joint inventor regards as the invention.
The following is a quotation of 35 U.S.C. 112 (pre-AIA ), second paragraph:
The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the applicant regards as his invention.
Claims 1-10 are rejected under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), second paragraph, as being indefinite for failing to particularly point out and distinctly claim the subject matter which the inventor or a joint inventor (or for applications subject to pre-AIA 35 U.S.C. 112, the applicant), regards as the invention.
Claim 1 is indefinite because the recitation “wherein the positive electrode comprises a positive electrode active layer including a positive electrode active material and a polymer film stacked on a positive electrode current collector” is unclear whether the polymer film is part of the positive electrode active layer or is a separate layer stacked with the positive electrode active layer on the current collector.
For examination purposes, the aforementioned recitation has been interpreted as “wherein the positive electrode comprises a positive electrode current collector, a positive electrode active layer including a positive electrode active material disposed on the positive electrode current collector, and a polymer film also disposed on the positive electrode current collector.”
Claims 2-10 are rejected as they depend from, and therefore incorporate the claimed subject matter from claims rejected under this statute.
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, 3-9 and 11-12 are rejected under 35 U.S.C. 103 as being unpatentable over Kang et al. (US 20150104716 A1) in view of Ophir et al. (US 20180166680 A1, provided on IDS filed on 6/26/2025).
Regarding claim 1, Kang et al. teaches a lithium secondary battery (Example 7, [0121]; also see 100, Fig. 2), the lithium secondary battery comprising:
an electrode assembly comprising a positive electrode (positive electrode, [0122]; also see 114, Fig. 2), a negative electrode (graphite negative electrode, [0122]; also see 112, Fig. 2), and a separator (polyethylene separator, [0122]; also see 113, Fig. 2) between the positive electrode and the negative electrode (see Fig. 2); and
an electrolyte composition (electrolyte prepared in Example 1, [0122]) comprising a non-aqueous organic solvent (organic solvent mixture including ethylene carbonate (“EC”), ethylmethyl carbonate (“EMC”), and dimethyl carbonate (“DMC”), [0114]), a lithium salt (LiPF6, [0114]), and an electrolyte additive (1-(2-hydroxyethyl)pyrrolidone (“HEP”), [0114]),
wherein the positive electrode (positive electrode, [0121] and [0122]; also see 114, Fig. 2) comprises a positive electrode active layer (formed by coating and drying of the positive electrode slurry on aluminum foil, see [0121]) including a positive electrode active material (Li1+x(NiaCobMnc)1-xO2 (0.05≦x≦0.2), [0121]; also see 22, Fig. 1) and a film (formed by pyrrolidine compound (HEP), see [0082], [0083] and [0131]; also see 26, Fig. 1) stacked (26 is on 22 and 20, see Fig. 1) on a positive electrode current collector (aluminum foil, [0121]; also see 20, Fig. 1) (interpretation see 112b rejection above),
wherein the negative electrode (graphite negative electrode, [0122]; also see 112, Fig. 2) comprises a negative electrode current collector (112 includes a negative electrode current collector, see [0088]), and a negative electrode active layer (negative electrode active material layer, [0088]) comprises a carbon material (graphite, [0122]) as a negative electrode active material (ICG1OH graphite, a product of Mitsubishi, [0122]) on the negative electrode current collector.
Kang et al. does not teach
a negative electrode active layer comprises a silicon material;
the film is a polymer film;
wherein a ratio (DC/CC) of an initial discharge capacity (DC) and an initial charge capacity (CC) of the lithium secondary battery is 0.7 to 1.2.
Different embodiment of Kang et al. teaches a negative electrode active layer (negative electrode active material layer, [0090]) comprises a silicon material (silicon (Si), [0092]).
It would have been obvious to one of ordinary skill in the art before the effective filling date of the claimed invention to modify the graphite negative electrode taught by Example 7 of Kang et al. by adding the silicon Si taught by Kang et al. to incorporate and deincorporate (e.g., intercalate and deintercalate) lithium (see Kang et al. [0091]). Further, it has been held that combining two embodiments disclosed adjacent to each other in a prior art patent does not require a leap of inventiveness and involves only routine skill in the art.
However, Kang et al. does not teach the film is a polymer film;
wherein a ratio (DC/CC) of an initial discharge capacity (DC) and an initial charge capacity (CC) of the lithium secondary battery is 0.7 to 1.2.
Ophir et al. teaches the film is a polymer film (polypyrrole (PPy) or polyaniline (PAni), the conductive polymer on 115, electro-polymerized from 95 (pyrrole, aniline), see Fig. 1 and [0030] and [0026]; polypyrrole and polyaniline see [0045]);
wherein a ratio (DC/CC) of an initial discharge capacity (DC) (~125 mAh/g, see disclosed cathode-discharging, cycle number 1, Fig. 3) and an initial charge capacity (CC) (~135 mAh/g, see disclosed cathode-charging, cycle number 1, Fig. 3) of the lithium secondary battery is 0.7 to 1.2 (DC/CC = 125/135 = 0.93).
It would have been obvious to one of ordinary skill in the art before the effective filling date of the claimed invention to modify the positive electrode taught by Kang et al. by adding pyrrole or aniline to form the polypyrrole or polyaniline layer prepared by the electro-polymerization during charging cycles having the initial discharging capacity to the initial charging capacity ratio as 0.93 taught by Ophir et al. because introduction of electrochemically-active conducting polymers such as polypyrrole (PPy) and polyaniline (PAni) into cathodes is known to enhance both the capacity and rate capability (see Ophir et al. [0045]).
Regarding claim 3, Kang et al. in view of Ophir et al. does not teach wherein the electrolyte additive is a polymeric compound containing nitrogen (N) and carbon (C).
Ophir et al. teaches wherein the electrolyte additive (pyrrole, see monomer of polypyrrole (PPy), [0045]; note: prior art method (iv): in the presence of a monomer pyrrole dissolved in an electrolyte; embodiments of Fig. 1 has monomer pyrrole in cathode formulation while in prior art method (iv) has pyrrole in the electrolyte) is a polymeric compound containing nitrogen (N) and carbon (C) (pyrrole with the chemical formula C₄H₅N, has N and C).
It would have been obvious to one of ordinary skill in the art before the effective filling date of the claimed invention to modify the electrolyte taught by Kang et al. in view of Ophir et al. by adding the monomer pyrrole taught by Ophir et al. to make polypyrrole film by the well-known electro-polymerization in the presence of the monomer pyrrole dissolved in an electrolyte (see Ophir et al. [0045]) therefore to host for Li+ insertion/extraction and to enhance the cathode capacity and rate capability (see Ophir et al. [0045]).
Regarding claim 4, Kang et al. in view of Ophir et al. does not teach wherein the electrolyte additive is a compound containing at least one of a pyrrole group or an aniline group, or combinations thereof.
Ophir et al. teaches wherein the electrolyte additive (pyrrole, see monomer of polypyrrole (PPy), [0045]; note: prior art method (iv): in the presence of a monomer pyrrole dissolved in an electrolyte; embodiments of Fig. 1 has monomer pyrrole in cathode formulation while in prior art method (iv) has pyrrole in the electrolyte) is a compound containing at least one of a pyrrole group (pyrrole, see monomer of polypyrrole (PPy), [0045]) or an aniline group, or combinations thereof.
It would have been obvious to one of ordinary skill in the art before the effective filling date of the claimed invention to modify the electrolyte taught by Kang et al. in view of Ophir et al. by adding the monomer pyrrole taught by Ophir et al. to make polypyrrole film by the well-known electro-polymerization in the presence of the monomer pyrrole dissolved in an electrolyte (see Ophir et al. [0045]) therefore to host for Li+ insertion/extraction and to enhance the cathode capacity and rate capability (see Ophir et al. [0045]).
Regarding claim 5, Kang et al. in view of Ophir et al. teaches wherein an amount of the electrolyte additive (1-(2-hydroxyethyl)pyrrolidone (“HEP”), Kang [0114]) is 0.01 to 5 wt % (0.1 wt %, Kang [0114]) based on a total weight of the electrolyte composition.
Regarding claim 6, Kang et al. in view of Ophir et al. does not teach wherein the polymer film has an average thickness of 5 nm to 500 μm.
Kang et al. teaches wherein the film (26, Fig. 1) has an average thickness of 5 nm to 500 μm (0.05 nm to about 100 nm, see [0054]).
It would have been obvious to one of ordinary skill in the art before the effective filling date of the claimed invention to modify the thickness of the polypyrrole or polyaniline layer taught by Kang et al. in view of Ophir et al. to be 5 nm to about 100 nm taught by Kang et al. because having such thickness, the transfer of lithium ions is not negatively affected, and oxidation of the electrolyte on the positive electrode surface is effectively prevented (see Kang et al. [0054]).
Regarding claim 7, Kang et al. in view of Ophir et al. does not teach wherein the positive electrode active material comprises an iron phosphate compound represented by Formula 1 below:
LiFeaM1 1-aXO4, [Formula 1]
wherein, in Formula 1,
M1 is one or more elements selected from the group consisting of W, Cu, Fe, V, Cr, Co, Ni, Mn, Ti, Zr, Zn, Al, In, Ta, Y, La, Sr, Ga, Sc, Gd, Sm, Ca, Ce, Nb, Mg, B, and Mo,
X is one or more selected from the group consisting of P, Si, S, As, and Sb, and
a is 0≤a≤0.5.
Different embodiment of Kang et al. teaches wherein the positive electrode active material comprises an iron phosphate compound represented by Formula 1 below:
LiFeaM1 1-aXO4, [Formula 1] (LiFePO4, [0104])
wherein, in Formula 1,
M1 is one or more elements selected from the group consisting of W, Cu, Fe, V, Cr, Co, Ni, Mn, Ti, Zr, Zn, Al, In, Ta, Y, La, Sr, Ga, Sc, Gd, Sm, Ca, Ce, Nb, Mg, B, and Mo (M1 = Fe, see LiFePO4, [0104]),
X is one or more selected from the group consisting of P, Si, S, As, and Sb (X = P, see LiFePO4, [0104]), and
a is 0≤a≤0.5 (a = 0, see LiFePO4, [0104]).
It would have been obvious to one of ordinary skill in the art before the effective filling date of the claimed invention to modify the Li1+x(NiaCobMnc)1-xO2 (0.05≦x≦0.2) taught by Kang et al. in view of Ophir et al. by adding the LiFePO4 by Kang et al. because it’s well known in the art that LiFePO4 is a representative example of the positive electrode active material (see Kang et al. [0104]). Further, it has been held that combining two embodiments disclosed adjacent to each other in a prior art patent does not require a leap of inventiveness and involves only routine skill in the art.
Regarding claim 8, Kang et al. in view of Ophir et al. teaches wherein the carbon material (graphite, Kang [0122]) comprises at least one of natural graphite, artificial graphite (ICG1OH graphite, a product of Mitsubishi, [0122]; note: product ICG stands for artificial graphite-based materials*), expanded graphite, non-graphitizable carbon, carbon black, acetylene black, or ketjen black, or combinations thereof. (*see: <https://www.m-chemical.co.jp/en/products/departments/mcc/anode/product/1201073_7544.html>)
Regarding claim 9, Kang et al. in view of Ophir et al. teaches wherein the silicon material comprises at least one of silicon (Si) (silicon (Si), Kang [0092]), silicon carbide (SiC), or silicon oxide (SiOq, where 0.8≤q≤2.5), or combinations thereof.
Regarding claim 11, Kang et al. teaches a method of manufacturing (manufacture a battery, see [0122]) a lithium secondary battery (Example 7, [0121]; also see 100, Fig. 2), the manufacturing method comprising:
assembling the lithium secondary battery (Example 7, [0121]; also see 100, Fig. 2) by injecting (the electrolyte prepared in Example 1 were used to manufacture a battery, see [0122]) an electrolyte composition (electrolyte prepared in Example 1, [0122]) in a battery case (case of a 2032 standard coin cell, [0122]; also see 120, Fig. 2) into which an electrode assembly comprising a positive electrode (positive electrode, [0122]; also see 114, Fig. 2), a negative electrode (graphite negative electrode, [0122]; also see 112, Fig. 2), and a separator (polyethylene separator, [0122]; also see 113, Fig. 2) between the positive electrode and the negative electrode is inserted (see Fig. 2); and
forming a film (formation of the pyrrolidine film on the positive electrode surface, [0081] and [0131]; also see 26, Fig. 1) on a positive electrode active layer (formed by coating and drying of the positive electrode slurry on aluminum foil, see [0121]) comprising a positive electrode active material (Li1+x(NiaCobMnc)1-xO2 (0.05≦x≦0.2), [0121]; also see 22, Fig. 1) by charging (formation charge at room temperature, [0133]) the lithium secondary battery (the lithium secondary batteries manufactured in Examples 7, [0133]) to a state-of-charge (SOC) of 10% or more (140%; note: formation charge is a type of over-charge, reached 4.65 V [0134] and a fully charged 2032 standard coin cell is well known to be 3.3 V),
wherein the electrolyte composition (electrolyte prepared in Example 1, [0122]) comprises a non-aqueous organic solvent (organic solvent mixture including ethylene carbonate (“EC”), ethylmethyl carbonate (“EMC”), and dimethyl carbonate (“DMC”), [0114]), a lithium salt (LiPF6, [0114]), and an electrolyte additive (1-(2-hydroxyethyl)pyrrolidone (“HEP”), [0114]),
wherein the negative electrode (graphite negative electrode, [0122]; also see 112, Fig. 2) comprises a negative electrode current collector (112 includes a negative electrode current collector, see [0088]), and a negative electrode active layer (negative electrode active material layer, [0088]) comprising a carbon material (graphite, [0122]) as a negative electrode active material (ICG1OH graphite, a product of Mitsubishi, [0122]) on the negative electrode current collector.
Kang et al. does not teach
a negative electrode active layer comprises a silicon material;
the film is a polymer film;
wherein a ratio (DC/CC) of an initial discharge capacity (DC) and an initial charge capacity (CC) of the lithium secondary battery is 0.7 to 1.2.
Different embodiment of Kang et al. teaches a negative electrode active layer (negative electrode active material layer, [0090]) comprises a silicon material (silicon (Si), [0092]).
It would have been obvious to one of ordinary skill in the art before the effective filling date of the claimed invention to modify the graphite negative electrode taught by Example 7 of Kang et al. by adding the silicon Si taught by Kang et al. to incorporate and deincorporate (e.g., intercalate and deintercalate) lithium (see Kang et al. [0091]). Further, it has been held that combining two embodiments disclosed adjacent to each other in a prior art patent does not require a leap of inventiveness and involves only routine skill in the art.
However, Kang et al. does not teach the film is a polymer film;
wherein a ratio (DC/CC) of an initial discharge capacity (DC) and an initial charge capacity (CC) of the lithium secondary battery is 0.7 to 1.2.
Ophir et al. teaches the film is a polymer film (polypyrrole (PPy) or polyaniline (PAni), the conductive polymer on 115, electro-polymerized from 95 (pyrrole, aniline), see Fig. 1 and [0030] and [0026]; polypyrrole and polyaniline see [0045]);
wherein a ratio (DC/CC) of an initial discharge capacity (DC) (~125 mAh/g, see disclosed cathode-discharging, cycle number 1, Fig. 3) and an initial charge capacity (CC) (~135 mAh/g, see disclosed cathode-charging, cycle number 1, Fig. 3) of the lithium secondary battery is 0.7 to 1.2 (DC/CC = 125/135 = 0.93).
It would have been obvious to one of ordinary skill in the art before the effective filling date of the claimed invention to modify the positive electrode taught by Kang et al. by adding pyrrole or aniline to form the polypyrrole or polyaniline layer prepared by the electro-polymerization during charging cycles having the initial discharging capacity to the initial charging capacity ratio as 0.93 taught by Ophir et al. because introduction of electrochemically-active conducting polymers such as polypyrrole (PPy) and polyaniline (PAni) into cathodes is known to enhance both the capacity and rate capability (see Ophir et al. [0045]).
Regarding claim 12, Kang et al. in view of Ophir et al. teaches wherein the charging the lithium secondary battery is performed at a C-rate of 0.01 C to 3.0 C at 25 to 70° C (charged at 1C at a temperature of 25° C, see Kang [0138]).
Claim 2 is rejected under 35 U.S.C. 103 as being unpatentable over Kang et al. (US 20150104716 A1) in view of Ophir et al. (US 20180166680 A1, provided on IDS filed on 6/26/2025) in view of Kuss et al. (US 20250125362 A1).
Regarding claim 2, Kang et al. in view of Ophir et al. does not teach wherein the positive electrode satisfies the following Equation 1 upon performing an X-ray photoelectron spectroscopy (XPS) analysis:
[Equation1]
0.5 ≤ PC/PN ≤ 5,
wherein, in Equation 1,
PC represents an intensity of a peak present at 284.0±0.5 eV, and
PN represents an intensity of a peak present at 402.5±0.5 eV.
Kuss et al. teaches wherein the positive electrode (cathode comprising Polypyrrole:carboxymethyl cellulose (PPy:CMC), see Abstract and [0011]) satisfies the following Equation 1 upon performing an X-ray photoelectron spectroscopy (XPS) analysis (XPS spectra, Figs 3b and 3c, [0011]):
[Equation1]
0.5 ≤ PC/PN ≤ 5, (2.75; PC/PN = 2.2 a.u. / 0.8 a.u., see citations below for Pc and PN)
wherein, in Equation 1,
PC (2.2 a.u., see Cβ peak in Fig. 3c, intensity axis on the right) represents an intensity of a peak present at 284.0±0.5 eV (Cβ peak in Fig. 3c at 284.2 eV), and
PN (0.8 a.u., see C=N+ peak in Fig. 3b, intensity axis on the right) represents an intensity of a peak present at 402.5±0.5 eV (C=N+ peak in Fig. 3b at 402.5 eV).
It would have been obvious to one of ordinary skill in the art before the effective filling date of the claimed invention to substitute the polypyrrole layer taught by Kang et al. in view of Ophir et al. with the Polypyrrole:carboxymethyl cellulose (PPy:CMC) composite taught by Kuss et al. to be a conductor providing electrical conduction pathways between electrode active materials, allowing batteries to function at high C-rates and the same time to be a strong adhesive binder for cathode active materials (see Kuss et al. [0005]).
Claim 10 is rejected under 35 U.S.C. 103 as being unpatentable over Kang et al. (US 20150104716 A1) in view of Ophir et al. (US 20180166680 A1, provided on IDS filed on 6/26/2025) in view of Ren et al. (US 20190237753 A1)
Regarding claim 10, Kang et al. in view of Ophir et al. does not teach wherein an amount of the silicon material is 1 to 20 wt % based on a total weight of the negative electrode active material.
Ren et al. teaches wherein an amount of the silicon material (SiO particles, [0019]) is 1 to 20 wt % (mass percentages of the SiO particles: 1˜19%, see [0019]) based on a total weight of the negative electrode active material (anode active material, [0016]; note: the anode active material includes SiO particles, graphite particles, and a carbon coating layer, [0016]).
It would have been obvious to one of ordinary skill in the art before the effective filling date of the claimed invention to substitute the negative electrode active material (graphite ICG1OH) taught by Kang et al. in view of Ophir et al. with the anode active material having 1-19 % mass percentages of SiO particles taught by Ren et al. to have a very large total surface area on the anode active materials which increases the rate of charge transfer of ions and electrons (see Ren et al. [0018]).
Conclusion
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/NING CHEN/Examiner, Art Unit 1723 /TIFFANY LEGETTE/Supervisory Patent Examiner, Art Unit 1723
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