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 .
Priority
Receipt is acknowledged of certified copies of papers required by 37 CFR 1.55.
Information Disclosure Statement
The information disclosure statements (IDS) submitted on September 30, 2024 and June 12, 2026 have been considered by the examiner.
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.
Claim 1, and by dependency claims 2-11 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.
Regarding claim 1, the limitation in lines 7-8 reciting “a part of at least an outermost layer of the negative electrode active material particles is coated with a layer of a plasticizer” is indefinite as it is unclear if the plasticizer is intended to be a part of the negative electrode active material particles or a separate component. The use of “outermost” when referring to the particles implies that the carbon layer is the outermost layer of the particles, and the plasticizer is therefore not a component of the particles, however, paragraph [0114] of the instant invention details the coating process such that the outermost surface of the particles appears to be the plasticizer layer. For the purposes of examination, the claim is interpreted as requiring at least a part of the carbon layer of the negative electrode active material particle coated with a layer of plasticizer.
Regarding claim 1, the use of “wherein” in line 2 makes the claim limitation in lines 7-8 regarding the plasticizer indefinite. As the claim does not positively recite that the negative electrode active material particles comprise a layer of a plasticizer, the limitation “wherein… a part of at least an outermost layer of the negative electrode active material particles is coated with a layer of a plasticizer” may be considered intended use of the of the negative electrode active material particles. Additionally, as stated above, the use of “outermost” makes it unclear if the carbon layer is the outermost layer or if the particles are intended to include a plasticizer layer as the outermost layer. The use of wherein raises a question as to the limiting effect of the language in a claim (MPEP 2111.04(I)). For the purposes of examination, the claim is interpreted as requiring at least a part of the carbon layer of the negative electrode active material particle coated with a layer of plasticizer.
Regarding claims 2-11, these claims are rejected based on their dependency on claim 1.
Claim Rejections - 35 USC § 102
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 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.
(a)(2) the claimed invention was described in a patent issued under section 151, or in an application for patent published or deemed published under section 122(b), in which the patent or application, as the case may be, names another inventor and was effectively filed before the effective filing date of the claimed invention.
Claims 1-4 and 11 are rejected under 35 U.S.C. 102(a)(1) and 102(a)(2) as being anticipated by Qu, et al. (WO 2022/001880 A1), cited on IDS.
Regarding claim 1, Qu teaches a silicon-oxygen composite anode material including composite particles (negative electrode active material particles) which include lithium silicate represented by Li4SiO4 and silicon-containing material (¶ [0007], Ln. 1-4). The silicon-containing material includes nano-silicon and silicon oxide (¶ [0015], Ln. 1-2). A carbon layer is formed on the surface of the composite particles (¶ [0009], Ln. 1-2). Qu further teaches that a hydrophobic layer is formed on the surface of the carbon layer (outermost layer of the negative electrode active material particles) (¶ [0011], Ln. 1-2). Qu teaches that the hydrophobic layer is made of at least one of lauric acid, stearic acid, leucine, methionine, and phenylalanine (¶ [0014], Ln. 1-2), teaching the use of lauric acid in Example 1 (plasticizer)(¶ [0165], Ln. 7-8).
Regarding claim 2, Qu teaches all of the limitations of claim 1 above and further teaches that the thickness of the hydrophobic layer is 2-500 nm (¶ [0082], Ln. 4-5). In Example 1, the hydrophobic layer is 2 nm thick, within the claimed range of 0.1-10 nm (¶ [0165], Ln. 9).
Regarding claim 3, Qu teaches all of the limitations of claim 1 above and further teaches that the carbon layer is formed by reacting the silicon source with an organic carbon source gas under a protective gas atmosphere such as hydrogen, nitrogen, helium, neon, argon, krypton, and xenon (¶ [0126]-[0127]). In Example 1, the carbon source gas is introduced in a nitrogen atmosphere, such that a part of the carbon layer contains a nitrogen atom (¶ [0163], Ln. 1-3).
Regarding claim 4, Qu teaches all of the limitations of claim 3 above and further teaches that the organic carbon source is a hydrocarbon (¶ [0041], Ln. 1). Claim 4 is considered a product by process wherein the process does not impart distinctive structural characteristics to the final product. The process of using a hydrocarbon derived from petroleum asphalt as a starting material does not impart distinct structural characteristics compared to the carbon layer of Qu, which is formed from a hydrocarbon and contains a nitrogen atom. Thus, the carbon layer of Qu anticipates product by process claim.
Regarding claim 11, Que teaches a negative electrode active material meeting the limitations of claim 1 above, and further teaches that the negative electrode active material is used in a negative electrode including binder, conductive material, and the active material (¶ [0214], Ln. 1-9).
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 5-6 are rejected under 35 U.S.C. 103 as being unpatentable over Qu, et al. (WO 2022/001880 A1) as applied to claim 1 above, and further in view of Vieira, M. G. A. Natural-based plasticizers and biopolymer films: A review, European Polymer Journal, Vol. 47 (2011), pp. 254-263, cited on IDS.
Regarding claims 5-6, Qu teaches all of the limitations of claim 1 above. Qu does not expressly teach that the hydrophobic layer contains at least one of a phthalate ester plasticizer, an adipate ester plasticizer, a phosphate ester plasticizer, and a sulfonamide plasticizer.
Vieira teaches a review of plasticizers and their use as additives in polymers (pp. 254, Col. 1, Ln. 1-5). Vieira teaches that hydrophobic plasticizers, which are water insoluble, lead to a decrease in water uptake (pp. 256, Col. 1, Ln. 35-44). Vieira teaches that phthalic acid esters continue to the be largest class of plasticizers in the 21st century, citing dioctyl phthalate as the most widely used plasticizer since the 1930s (pp. 254, Col. 2, Ln. 15-20). As an alternative natural plasticizer, Vieira teaches the use of lauric acid (Table 1).
It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to modify the lauric acid in the hydrophobic layer of Qu to use a widely known hydrophobic plasticizer such as dioctyl phthalate. As taught by Vieira, the use of dioctyl phthalate is very well known. Further, as Vieira teaches natural plasticizers including lauric acid, one of ordinary skill in the art would find it obvious that dioctyl phthalate could be used in place of the lauric acid in the hydrophobic layer of Qu. As both are capable of imparting hydrophobicity to the coating, one of ordinary skill in the art would find it obvious to make the substitution. One would be motivated to use dioctyl phthalate based on its wide commercial use and cost.
Claims 7-8 are rejected under 35 U.S.C. 103 as being unpatentable over Qu, et al. (WO 2022/001880 A1) as applied to claim 1 above, and further in view of Horie, et al. (US 2023/0317953 A1).
Regarding claims 7-8, Qu teaches all of the limitations of claim 1 above. Qu does not expressly teach that the composite particle further comprises a solid electrolyte.
Horie teaches a coated negative electrode active material for a lithium ion battery (¶ [0013], Ln. 1-5). Horie teaches that the negative electrode active material particle may include silicon materials such as silicon oxide (¶ [0019], Ln. 1-8). Horie teaches that the coating layer includes a polymer compound, a compound A which functions as a plasticizer, a conductive assistant, and ceramic particles (¶ [0023], Ln. 1-3, ¶ [0077], Ln. 1-2). Horie teaches that the ceramic particles inhibit side reactions that occur between the electrolytic solution and the negative electrode active material particles, preventing the internal resistance value of the lithium ion battery from increasing (¶ [0078], Ln. 1-6). Specifically, Horie teaches the use of aluminum oxide in order to suitably inhibit the side reaction (¶ [0082], Ln. 1-6).
It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to modify the hydrophobic layer of Qu to include aluminum oxide (solid electrolyte) based on the teachings of Horie. One of ordinary skill in the art would find it obvious to apply the teachings of Horie to the composite particle of Qu, as both teach a coated silicon oxide negative electrode active material particle. One of ordinary skill in the art would be motivated to include aluminum oxide in the hydrophobic coating in order to inhibit side reactions between the composite particle and the electrolyte solution. As the hydrophobic layer is the outer layer of the particle, one of ordinary skill in the art would find it obvious to include the aluminum oxide in this layer.
Claims 9-10 are rejected under 35 U.S.C. 103 as being unpatentable over Qu, et al. (WO 2022/001880 A1) as applied to claim 1 above, and further in view of Hirose, et al. (US 2019/0131618 A1).
Regarding claim 9, Qu teaches all of the limitations of claim 1 above. Qu does not expressly teach that the crystallite size corresponding to an Si (111) crystal face is 5.0 nm or less and that a ratio of an intensity A of the peak derived from the Si (111) face relative to an intensity B of a peak derived from a Li2SiO3 (111) crystal face satisfies the formula 0.4≤A/B≤1.0.
Hirose teaches a negative electrode active material including a silicon compound particle which includes Li2SiO3 and Li2Si2O5 (¶ [0026]-[0027]). Hirose teaches that the silicon compound particle includes a carbon coating on the surface (¶ [0045], Ln. 1-2). Hirose teaches that the peak intensity derived from Li2SiO3 is A and the peak intensity derived from Si is B (¶ [0028], Ln. 1-3), further teaching that when the peak intensity A is the highest, water resistance is improved and the crystallinity of the Si component is suppressed, improving cycle characteristics (¶ [0030], Ln. 8-17). Hirose also teaches that Li4SiO4 is present in the bulk of the silicon compound particle, improving battery characteristics (¶ [0096], Ln. 1-3). Li4SiO4 is converted to Li2SiO3 and Li2Si2O5 during a heat treatment, such that the peak intensity of Li2SiO3 and Li2Si2O5 is higher than the peak intensities corresponding to Si or SiO2 (¶ [0128], Ln. 1-14). Hirose further teaches that the crystallite size corresponding to a Si (111) crystal plane is 7.5 nm or less, teaching that when amount of the Si crystal is small, the battery characteristics can be improved and also a stable Li compound can be produced (¶ [0101], Ln. 1-12). In Examples 1-1 – 1-4, the Si (111) crystallite sizes are under 5 nm (Table 1).
It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to modify the composite particle of Qu to include Li2SiO3 as well as Li4SiO4 and to limit the Si (111) crystallite size based on the teachings of Hirose. One of ordinary skill in the art would find it obvious to apply the teachings of Hirose to the composite particle of Qu as both teach a lithium silicate particle with a carbon coating used as a negative electrode active material and further teach improving water resistance. One of ordinary skill in the art would find it obvious to heat treat the particle such that Li2SiO3 is formed, and would be motivated to do so to improve water resistance. Further, as Hirose teaches that the peak intensity corresponding to Li2SiO3 is higher than the peak intensity corresponding to Si, one of ordinary skill in the art would find it obvious that the ratio of an intensity A of the peak derived from the Si (111) face relative to an intensity B of a peak derived from a Li2SiO3 (111) crystal face satisfies the formula 0.4≤A/B≤1.0. Finally, as Hirose teaches the benefits of keeping the amount of the Si crystal is small, one of ordinary skill in the art would find it obvious to target a crystallite size corresponding to the Si (111) crystal face of 5 nm or less, as taught in the examples of Hirose. One of ordinary skill in the art would be motivated to target this value in order to improve battery characteristics and produce a stable Li compound.
Regarding claim 10, Qu teaches all of the limitations of claim 1 above. Qu further teaches that prior to coating with carbon and the hydrophobic layer, the silicon monoxide particles have a median particle size of 6 µm (¶ [0162], Ln. 6-7). Qu does not expressly teach the median diameter of the composite particle, and therefore does not expressly teach that the median diameter is 4.5-15 µm.
Hirose teaches a negative electrode active material including a silicon compound particle which includes a silicon compound, Li2SiO3 and Li2Si2O5 (¶ [0026]-[0027]), and Li4SiO4 present in the bulk of the silicon compound particle (¶ [0096], Ln. 1-3). Hirose teaches that the silicon compound particle includes a carbon coating on the surface (¶ [0045], Ln. 1-2). Hirose further teaches that the median diameter of the negative electrode active material particle is 1.0-15 µm, teaching that when the diameter is 1.0 μm or more, increase in the irreversible capacity of the battery due to the increase in the surface area per mass can be suppressed, and when median diameter is 15 μm or less, the particles are difficult to be cracked (¶ [0044], Ln. 1-6).
It would have been obvious to one of ordinary skill in the art, before the effective filing date of the claimed invention, to modify the median diameter of the composite particles of Qu to be within 1.0-15 µm based on the teachings of Hirose. Further, as Qu teaches silicon monoxide particles having a median particle size of 6 µm prior to introducing lithium and the coating materials, one of ordinary skill in the art would find it obvious to have composite particles having a median diameter from 6-15 µm, within the claimed range of 4.5-15 µm. One of ordinary skill in the art would find it obvious to apply the particle diameter teachings of Hirose to the composite particles of Qu as both teach a silicon oxide and lithium silicate containing negative electrode active material with a carbon coating. One would be motivated to the apply the particle diameter teachings of Hirose to the composite particles of Qu in order to suppress the increase in irreversible capacity of the battery due to the increase in the surface area per mass and to suppress cracking.
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to SARAH J JACOBSON whose telephone number is (703)756-1647. The examiner can normally be reached Monday - Friday 8:00am - 5:00pm.
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/SARAH J JACOBSON/Examiner, Art Unit 1785
/MARK RUTHKOSKY/Supervisory Patent Examiner, Art Unit 1785
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