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 .
Claim Rejections - 35 USC § 102
The following is a quotation of the appropriate paragraphs of 35 U.S.C. 102 that form the basis for the rejections under this section made in this Office action:
A person shall be entitled to a patent unless –
(a)(1) the claimed invention was patented, described in a printed publication, or in public use, on sale, or otherwise available to the public before the effective filing date of the claimed invention.
Claims 11-12 are rejected under 35 U.S.C. 102(a)(1) as being anticipated by Cho, et. al. (see attached EPO machine translation of KR20200136335A).
Regarding Claim 11, Cho discloses a negative electrode active material for lithium secondary battery (“[0023] A lithium secondary battery according to an embodiment of the present disclosure includes a positive electrode; cathode; And an electrolyte, and the negative electrode may include a negative active material for a lithium secondary battery manufactured by the disclosed method”), comprising: an artificial graphite (“[0049] The base material for an anode active material according to an embodiment of the present disclosure is graphitized coke . . . [0051] high-quality artificial graphite is formed after graphitization”); and a carbon coating layer formed on the surface of the artificial graphite [0042] Finally, an amorphous carbon coating layer is formed on the surface of the negative electrode material”); wherein, the carbon coating layer is a carbonized liquid coating layer (“[0054] The coated product undergoes a heat treatment step, and the coating material is carbonized”) having a viscosity of 300 to 25,000 mPa • s at 35 °C (“[0036] The coating material is graphitizable carbon and may have a softening point of 50° C. or less. In addition, the coating material may have a viscosity of 3,000 cPs or less at room temperature, specifically, 1 to 3,000 cPs, and more specifically, 1 to 2,000 cPs. That is, the coating material of one embodiment of the present disclosure may have viscoelastic properties at room temperature. Specifically, the softening point of the coating material may be greater than 0 to 50°C or less, greater than 0 to 41°C, greater than 0 to 30°C, or 20 to 30°C or less . . . [0036] the coating material must exhibit viscoelastic properties at room temperature with a softening point of 50° C. or less.” wherein cPs is convertible 1:1 to mPa • s, indicating 3,000 mpA or less at room temperature; however, because the softening point may be 0 to 50°C and “viscoelastic properties” must be exhibited within this range, this indicates an overlapping range with the claimed viscosity range”). Cho at [0036-38, 42-49, 51-54]
Claim 11 is anticipated by Cho.
Regarding Claim 12, Claim 12 relies upon Claim 11.
Cho discloses “[0008] The base material for the negative active material may be a base material obtained by graphitizing coke. [0009] The coke may include at least 70 parts by weight of green coke and the balance of calcined coke based on 100 parts by weight of the total coke. [0010] The green coke may be coal-based green coke or petroleum-based green coke, or a combination thereof.” Cho at [0008 – 10]. Because calcined coke is petroleum based, this is “the artificial graphite is an artificial graphite derived from coal-based coke, an artificial graphite derived from petroleum-based coke, or a mixture thereof.”
Claim 12 is anticipated by Cho.
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.
Claims 1 – 3, 5, 7 – 10, 14 are rejected under 35 U.S.C. 103 as being unpatentable over Cho, in view of Lee, et. al. (US2016322636A1).
Regarding Claim 1, Cho teaches a manufacturing method of negative electrode active material for lithium secondary battery, comprising: preparing an artificial graphite (“[0049] The base material for an anode active material according to an embodiment of the present disclosure is graphitized coke . . . [0051] high-quality artificial graphite is formed after graphitization”); forming a coating layer (“[0042] Finally, an amorphous carbon coating layer is formed on the surface of the negative electrode material. The amorphous carbon coating layer formed on the surface of the negative electrode material avoids direct contact between the electrochemically active graphite edge surface and the electrolyte solution, and at the same time suppresses the simultaneous insertion reaction of Li ions and solvents into the graphite layer, thereby reducing irreversible reactions.”); and carbonizing the artificial graphite on which the coating layer is formed (“[0054] Heat-treating the product coated with the coating material; finally, a negative active material for a lithium secondary battery is obtained. The coated product undergoes a heat treatment step, and the coating material is carbonized.”); wherein, the liquid coating material has a viscosity of 25,000 mPa • s at 35 °C, (“[0036] The coating material is graphitizable carbon and may have a softening point of 50° C. or less. In addition, the coating material may have a viscosity of 3,000 cPs or less at room temperature, specifically, 1 to 3,000 cPs, and more specifically, 1 to 2,000 cPs. That is, the coating material of one embodiment of the present disclosure may have viscoelastic properties at room temperature. Specifically, the softening point of the coating material may be greater than 0 to 50°C or less, greater than 0 to 41°C, greater than 0 to 30°C, or 20 to 30°C or less . . . [0036] the coating material must exhibit viscoelastic properties at room temperature with a softening point of 50° C. or less” wherein cPs is convertible 1:1 to mPa • s, indicating 3,000 mPa • s or less at room temperature; however, because the softening point may be 0 to 50°C and “viscoelastic properties” must be exhibited within this range, this indicates an overlapping range with the claimed viscosity range). Cho at [0036-38, 42-49, 51-54].
However, Cho is silent as to forming a coating layer covering the artificial graphite by mixing the artificial graphite and a liquid coating material, because the coating layer of Cho is formed by “[0040] Methods of coating the negative active material include wet coating and dry coating. Wet coating is a method of coating by immersing the base material for negative active material to be coated in a solution containing the coating material, and in the dry coating, mixing the base material and the coating material without adding a separate solvent (including a mixer with shearing force), etc.” In this case, the base material is an artificial graphite precursor (coke), and the heat treatment forms the carbonizing and the graphitization step. In other words, Cho fails to teach the requisite order, while the underlying material is identical.
Lee discloses a method of making a negative electrode active material: “[0054] Meanwhile, according to another aspect of the present invention, there is provided a method of manufacturing a negative electrode active material, which includes sintering soft carbon at a temperature range of approximately 2,000° C. or higher to less than 2,800° C., preferably 2,000° C. or higher to 2,500° C. to obtain low crystalline artificial graphite; and [0055] forming an amorphous carbon coating layer on the low crystalline artificial graphite.” Lee at [0054-55]. Further, “[0061] In the method of manufacturing a negative electrode active material according to one exemplary embodiment of the present invention, the amorphous carbon coating layer may be formed by mixing low crystalline carbon particles with an amorphous carbon precursor, and thermally treating the resulting mixture,” wherein low crystalline carbon is the same artificial graphite. Id. at [0061]. Finally, Lee teaches “Unlike conventional graphite-based negative electrode active materials or hard carbon-based negative electrode active materials, the soft carbon has high power and a short period of time required for charging. However, when the soft carbon is used in lithium secondary batteries, an increase in irreversible capacity may be caused, resulting in poor initial efficiency and low reversible capacity. . . . [0008] The present invention is designed to solve the problems of prior art, and therefore it is an object of the present invention to provide a negative electrode active material capable of forming a stable SEI layer to improve initial efficiency and reversible capacity, and a method of manufacturing the same.” In other words, coating the high power soft carbon (artificial graphite) with the hard carbon (non-graphitizable amorphous carbon) in this order serves to produce a protective coating around the artificial graphite more effectively.
One of ordinary skill in the art before the effective filing date of the claimed invention would find it obvious to modify the method of Cho, such that the mixing step of Lee occurs, wherein artificial graphite is formed first, and a coating layer is formed covering the artificial graphite (however, with the proviso that the liquid precursor of the wet mixing step of Cho is utilized), such that the method comprises “preparing an artificial graphite; forming a coating layer covering the artificial graphite by mixing the artificial graphite and a liquid coating material,” because Lee teaches its method allows the amorphous carbon layer to protect graphitizable carbon and form a stable SEI layer.
Claim 1 is obvious over Cho, in view of Lee.
Regarding Claim 2, Claim 2 relies upon Claim 1. Claim 1 is obvious over modified Cho.
Cho discloses “[0047] In addition, the coating material may be included in 2.5 parts by weight to 50 parts by weight per 100 parts by weight of the base material.” Cho at [0047]. Modified Cho, because it modifies the base material to be artificial graphite within the mixing step, thus teaches “in the step of forming a coating layer, the liquid coating material content for 100 parts by weight of artificial graphite is 5 to 30 parts by weight.”
Claim 2 is obvious over Cho, in view of Lee.
Regarding Claim 3, Claim 3 relies upon Claim 1. Claim 1 is obvious over modified Cho.
Cho teaches “[0037] Specifically, the coating material may be one or more selected from the group consisting of coal-based coal tar,” and “[0068] The coal tar used in this experiment has a residual carbon ratio of 20 parts by weight per 100 parts by weight of coal tar, a softening point of 25 to 30°C, a fixed carbon 21.94% by weight, and a phenolic resin has a residual carbon ratio of 40 parts by weight per 100 parts by weight of the phenol resin. It is a part, and the softening point is 37-50°C, and one containing 40.05% by weight of fixed carbon was used.” Cho at [0037, 68]. This reads upon “wherein: in the step of forming the coating layer, the fixed carbon content at 25 0C of the liquid coating material is 15 to 60 wt%.”
Claim 3 is obvious over Cho, in view of Lee.
Regarding Claim 5, Claim 5 relies upon Claim 1. Claim 1 is obvious over modified Cho.
Lee teaches “[0078] A coal tar pitch obtained from coal by fractional distillation was coked, thermally treated at 550° C., and then sintered at 1,400° C. to obtain pitch coke (i.e., soft carbon) having a major axis length of 11.5 μm, a specific surface area of 6 m2 /g to 8 m2 /g, and a tap density of 1.3 g/cc. [0079] The resulting pitch coke was sintered at approximately 2,000° C. for 10 hours to prepare low crystalline artificial graphite. The low crystalline artificial graphite had an interplanar spacing of (002) plane of 0.3396 nm, as measured by XRD.” Lee at [0078 – 79]. This reads upon “wherein: in the step of preparing artificial graphite, the artificial graphite is coal- based coke-derived artificial graphite, petroleum-based coke-derived artificial graphite, or a mixture thereof.”
Claim 5 is obvious over Cho, in view of Lee.
Regarding Claim 6, Claim 6 relies upon Claim 5. Claim 5 is obvious over modified Cho.
Cho teaches “[0008] The base material for the negative active material may be a base material obtained by graphitizing coke. [0009] The coke may include at least 70 parts by weight of green coke and the balance of calcined coke based on 100 parts by weight of the total coke. [0010] The green coke may be coal-based green coke or petroleum-based green coke, or a combination thereof.” This presents an overlapping range with “[t]he method of claim 5, wherein: the artificial graphite is a mixture of the artificial graphite derived from coal-based coke and the artificial graphite derived from petroleum-based coke, and more than 50 parts by weight of petroleum-based coke-derived artificial graphite is mixed with respect to 100 parts by weight of the mixture.” MPEP 2144.05 (I).
Claim 6 is obvious over Cho, in view of Lee.
Regarding Claim 7, Claim 7 relies upon Claim 1. Claim 1 is obvious over modified Cho.
Cho teaches at Table III a span for the coal tar 2 coating of the base material of 0.98, and “[0075] -Particle size: Laser diffraction method, particle size span = (D90-D10)/D50)”. While this is presented at [0081] of the attached machine translation, a formatting error places the span in the wrong column. A screenshot of the attached original foreign document shows the relevant Table 3, with the relevant span appearing in the 11th row of results. This reads upon “in the step of preparing artificial graphite, a particle size SPAN ((D90- D10)/D50) of the artificial graphite is 0.7 to 2.5.”
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618
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Table 3 of Cho. While row 11 is the cited result, the Office notes all values fall within the claimed SPAN range.
Claim 7 is obvious over Cho, in view of Lee.
Regarding Claim 8, Claim 8 relies upon Claim 1. Claim 1 is obvious over modified Cho.
Cho teaches “[0061] In the method of manufacturing a negative electrode active material according to one exemplary embodiment of the present invention, the amorphous carbon coating layer may be formed by mixing low crystalline carbon particles with an amorphous carbon precursor, and thermally treating the resulting mixture.” This amorphous carbon precursor is in the context of “ [0003] A carbonaceous material has been used [in the art] as a negative electrode material for lithium secondary batteries. The carbonaceous material includes crystalline carbon and amorphous carbon. The crystalline carbon representatively includes graphite carbon such as natural graphite, and artificial graphite, and the amorphous carbon includes hard carbon (i.e., non-graphitizable carbon) obtained by carbonizing a polymeric resin, soft carbon (i.e., graphitizable carbon) obtained by thermally treating pitch, etc.” This indicates the amorphous carbon precursor of modified Cho reads upon “in the step of forming a coating layer, the liquid coating material is a soft- graphitized carbon precursor or a hard-graphitized carbon precursor.”
Claim 8 is obvious over Cho, in view of Lee.
Regarding Claim 9, Claim 9 relies upon Claim 1. Claim 1 is obvious over modified Cho.
Cho teaches “[0055] The temperature range of the heat treatment step may be 1000 to 1400°C, specifically 1100 to 1300°C, and more specifically 1200 to 1300°C. The time range of the heat treatment step may be 1 hour to 4 hours, specifically 1 hour to 3 hours, preferably about 2 hours.” This presents an overlapping range with “the carbonization temperature is 800 to 2,000 °C.” MPEP 2144.05 (I).
Claim 9 is obvious over Cho, in view of Lee.
Regarding Claim 10, Claim 10 relies upon Claim 1. Claim 1 is obvious over modified Cho.
Cho teaches “[0041] Since the coating material having viscoelasticity at room temperature according to an embodiment of the present disclosure has fluidity, which is a property of a liquid, the coverage property of coating the surface of the anode material is better than that of a general solid coating material having little fluidity. That is, a coating material having viscoelastic properties at room temperature is uniformly attached to the surface of the negative electrode material and carbonized through heat treatment to form an amorphous carbon coating layer on the negative electrode material surface.” Id. at [0041]. This reads upon in the step of forming a coating layer, the mixing of the artificial graphite and the liquid coating material is performed at a temperature of 50 0C or less,” because the viscoelasticity at room temperature and the mixing strongly implies that this mixing is occurring at room temperature prior to heat treatment.
Claim 10 is obvious over Cho, in view of Lee.
Regarding Claim 13, Claim 13 relies upon Claim 12. Claim 12 is obvious over modified Cho.
Cho teaches “[0008] The base material for the negative active material may be a base material obtained by graphitizing coke. [0009] The coke may include at least 70 parts by weight of green coke and the balance of calcined coke based on 100 parts by weight of the total coke. [0010] The green coke may be coal-based green coke or petroleum-based green coke, or a combination thereof.” This presents an overlapping range with “[t]he method of claim 5, wherein: the artificial graphite is a mixture of the artificial graphite derived from coal-based coke and the artificial graphite derived from petroleum-based coke, and more than 50 parts by weight of petroleum-based coke-derived artificial graphite is mixed with respect to 100 parts by weight of the mixture.” MPEP 2144.05 (I).
Claim 13 is obvious over Cho, in view of Lee.
Regarding Claim 14, Claim 14 relies upon Claim 1.
Cho teaches “[0023] A lithium secondary battery according to an embodiment of the present disclosure includes a positive electrode; cathode; And an electrolyte, and the negative electrode may include a negative active material for a lithium secondary battery manufactured by the disclosed method.” Cho at [0023]. This indicates modified Cho teaches “a lithium secondary battery comprising: a negative electrode comprising a negative electrode active material manufactured from the negative electrode active material manufacturing method for a lithium secondary battery claim 1; a positive electrode; and an electrolyte.”
Claim 14 is obvious over Cho, in view of Lee.
Claim 4 is rejected under 35 U.S.C. 103 as being unpatentable over Cho, in view of Lee, further in view of Sotowa, et. al. (US10377634B2).
Regarding Claim 4, Claim 4 relies upon Claim 1. Claim 1 is obvious over modified Cho.
Cho and Lee are silent as to the step of preparing artificial graphite comprises: pulverizing a coke; and graphitizing the coke.
Sotowa teaches a carbon material for a battery, wherein “[0108] Next, the calcined coke is to be pulverized. [0109] There is not particular limit to the method of pulverization . . .[0111] In the pulverized calcined coke, lattice defects are generated . . . [0112] When there are many defects on the particle edge surface, the particles become highly responsive to the electrolyte composition and consume much electricity in the initial charge: i.e. at the time of the lithium ion intercalation, which results in forming an excessively thick coating. As a result, it inhibits reversible lithium intercalation and release reaction of lithium ions and may adversely effect on the battery life such as cycle characteristics. Therefore, in the graphite edge surface, the status having fewer defects is desirable. [0113] In order to reduce the influence of defects generated at the time of heat treatment of the pulverized calcined coke, the particles obtained by pulverizing a defect repairing material selected from petroleum pitch or coal-tar pitch may be mixed into the coke after graphitization, and the mixture can be subjected to heat treatment. By performing the operation, the defects on the fracture surface (particle edge surface) generated by the pulverization are repaired through the heat treatment and a material in which few defects are exposed on the particle edge surface can be obtained.” Sotowa at [00108 – 114]. In other words, the pulverization process of Sotowa improves the uniformity of the fracture surface and helps to eliminate defects.
One of ordinary skill in the art before the effective filing date would find it obvious to modify the method of modified Cho, such that the pulverization step of Sotowa is applied such that the method now comprises “the step of preparing artificial graphite comprises: pulverizing a coke; and graphitizing the coke.”
Claim 4 is obvious over Cho, in view of Lee, further in view of Sotowa.
Conclusion
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/K.R.H./Examiner , Art Unit 1725
/NICOLE M. BUIE-HATCHER/Supervisory Patent Examiner, Art Unit 1725
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