DETAILED ACTION
Application 17/023655, “NEGATIVE ELECTRODE MATERIAL FOR NONAQUEOUS SECONDARY BATTERIES, NEGATIVE ELECTRODE FOR NONAQUEOUS SECONDARY BATTERIES, AND NONAQUEOUS SECONDARY BATTERY”, is a continuation of a PCT application filed on 3/29/19 and claims priority from a foreign application filed on 3/29/18.
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
This Office Action on the merits is in response to communication filed on 1/14/26.
Response to Arguments
Applicant’s arguments filed on 1/14/26 have been fully considered, but are not persuasive. Applicant presents the following arguments.
The negative electrode material disclosed by Akasaka is present includes two sets of particle distributions, each having a different d50 value, whereas, applicant’s invention is described as containing a monomodal distribution with only a single size peak. Therefore, Akasaka fails to teach or suggest “the negative electrode material consists of a distribution of particles having a single volume average particle size of from 3 µm to 50 µm”, as presently claimed. In response, applicant’s arguments point out how Akasaka’s particles are present in a bimodal distribution, rather than a monomodal distribution; however, claim 1 as worded does not actually require a monomodal distribution of particles. Instead, the claim merely requires that collection of particles have “a single volume average particle size of from 3 µm to 50 µm”, a recitation which does not suggest or require a monomodal distribution. A bimodal distribution does have a single average particle size, which is determinable by taking a number weighted average of the separate D50 values of the two peaks. Thus, applicant’s argument is not found persuasive because it is not commensurate in scope with the claimed invention which does not require a monomodal distribution of particle sizes for the negative electrode material.
Regarding claim 12, applicant achieves a d90/d10 ratio of particle sizes above 2.5 by utilizing a broadly distributed monomodal peak, whereas Akasaka achieves the high d90/d10 value by using a bimodal distribution of particle size. In response, neither of claims 1 and 12 require a monomodal distribution of particle size; therefore, the argument is unpersuasive for failing to be commensurate in scope with the presently claimed invention.
Akasaka does not disclose or suggest a negative electrode material in which a large d90/d10 ratio and a low specific surface area are achieved in combination. In response, the argument is not found persuasive since both the surface area analysis presented in the rejection of claim 1 and the d90/d10 analysis presented in the rejection of claim 12 are based on the consideration of the bimodal distribution of particles. As previously described, applicant’s argument that this distribution is distinguished from the presently claimed invention was not found persuasive.
The combination of specific surface area, d90 and d10 values are only discussed in Akasaka as independent properties. Akasaka does not teach these properties as result-effective to produce particular advantage and does not disclose how the properties could be achieved in combination, as presently claimed. In response, the argument is not found persuasive at least because it does not seem to point out the unexpected advantage associated with the combination, or compare the achievement of that advantage to the achievements of the prior art. See MPEP 716 for more detail on the requirements of evidence for demonstrating that a prima facie case of is overcome by a showing of unexpected results. Additionally, the argument may be intended to suggest that, notwithstanding the suggestion of the claimed properties individually in Akasaka, the properties could not be achieved in a practical embodiment as is achieved in applicant’s invention. This argument is also not found persuasive at least because the argument lacks the evidence and technical reasoning to persuasively demonstrate that the claimed characteristics could not be achieved in the prior art, notwithstanding the general suggestion thereof. As described in MPEP 716, inoperability of the prior art is exemplary of an argument that requires supporting evidence.
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 of this title, 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.
Claims 1-10 and 12 is/are rejected under 35 U.S.C. 103 as being unpatentable over Akasaka (JP 2014-186956).
Alternatively, claims 1-10 and 12 is/are rejected under 35 U.S.C. 103 as being unpatentable over the combination of Akasaka (JP 2014-186956) and Kim (US 2020/0127289) or Tsujiko (US 2019/0115585).
Regarding claim 1-4 and 6-9, Akasaka teaches a negative electrode material for nonaqueous secondary batteries (abstract, paragraphs [0001, 0005]), the negative electrode material comprising graphite having amorphous carbon, such as carbon black, deposited on at least a part of a surface of the graphite (specifically, Akasaka’s claim 2 and paragraph [0010] teaches the negative electrode active material including particles “B” which are comprised of spherical graphite particles “C” with carbonaceous material such as carbon black particles “D” deposited on the surface).
Akasaka further teaches that the graphite particles are spherical particles having a circularity of 0.90 or more [as required by claim 2] (paragraph [0021] generally teaches circularity of 0.92 or more, while paragraph [0169] and Table 1] teach exemplary values with circularity between 0.91 and 0.93).
Akasaka further teaches that the circularity may be measured by flow system particle analysis (paragraph [0161]).
As to claim 6 and 7, Akasaka further teaches a nonaqueous secondary battery comprising positive and negative electrodes and an electrolyte (paragraph [0013, 0140]), the negative electrode comprising a current collector and an active material layer disposed on the current collector (paragraph [0128, 0140]), the active material layer including the negative electrode material according being the above-described negative electrode material (paragraph [0013, 0128, 0140]).
Claim 1 further requires that the tap density is 1.091 g/cm3 or more, while claim 4 further requires that a tap density of the negative electrode material is from 1.091 to 1.65 g/cm3.
Akasaka further teaches that the tap density of the carbon material may preferably between 0.9 and 1.5 g/cm3 (paragraph [0063, 0030]), a range which overlaps the range of claim 1.
To clarify, paragraph [0030] gives a preferable tap density for the particles A of most broadly 0.5 to 1.5 g/cm3 and most narrowly 0.7 to 1.1 g/cm3, while paragraph [0063] gives a tap density for the particles B of most broadly 0.8 to 1.8 g/cm3 and most narrowly 0.95 to 1.3 g/cm3, with the negative electrode material formed as a mixture of the particles A and the particles B (see abstract and Akasaka claim 1). The paragraphs teach this range being “preferably” used for the benefit of balancing charging/discharging characteristics, cycle path characteristics and/or lithium ion mobility. To further clarify, although the teachings of paragraphs [0030] and [0063] are specific to the constituent particles A and B of the mixed carbon electrode material, the mixture of the particles A and B would possess the same or similar tap density since the disclosed range for the two constituents substantially overlap. Of note, paragraph [0120] expressly teaches that “[t]he non-aqueous secondary battery negative electrode carbon material of the present invention has a tap density of…” most preferably 0.7 to 1.3 g/cm3, for substantially the same benefits, confirming the agreement in terms of tap density range and associated function between the constituents A and B and the mixture thereof.
Therefore, the requirements that “the tap density is 1.091 g/cm3 or more” of claim 1, and the requirement that “a tap density of the negative electrode material is from 1.091 to 1.65 g/cm3” of claim 4, are found to be obvious over Akasaka as the range disclosed as preferable in the prior art range overlaps the claimed range.
Further regarding claim 1, it is noted that claim 1 does not specify whether “the tap density” determined by tapping the sample referred to in claim 1 is the tap density of the negative electrode active material (as in present claim 4), or is the tap density of the carbon material (as in originally filed claim 4); therefore, the broadest reasonable interpretation of claim 1 includes both possibilities.
Claim 1 further requires that a surface area of the negative electrode material is 6.7 m2/g or less. Akasaka does not appear to teach a preferred range for the negative electrode active material as a whole, and therefore does not expressly teach that a surface area of the negative electrode material is 6.7 m2/g or less.
However, Akasaka does teach a negative electrode material comprised of a mixture of particles A and B (see abstract), wherein the particles A most preferably have a specific surface area of 1 to 8 m2/g (paragraph [0028]) and the particles B most preferably have a specific surface area of 3 to 6 m2/g (paragraph [0062]).
The mixture of the particles A and B would have an average specific surface area governed by these two ranges, such as to yield a suggested range which overlaps the claimed range. For example, the midpoint of the suggested specific surface area range of the particles A is 4.5 m2/g, while the midpoint of the suggested specific surface area range of the particles B is also 4.5 m2/g. Therefore, the average specific surface area range suggested by mixing the particles A and B includes at least a value of 4.5 m2/g, which lies within the claimed range demonstrating the overlap. Since the suggestion of Akasaka overlaps the claimed range of 6.7 m2/g or less, the claimed range is found to be obvious.
Akasaka is silent as to the negative electrode active material possessing the following properties:
a density index (Dr-t) of 0.080 g/cm3 or less as in claim 1, 0.073 g/cm3 or less as in claim 8, or 0.066 g/cm3 or less as in claim 9, [wherein the density index (Dr-t) is represented by Formula 1 of claim 1];
a volume resistivity of the negative electrode material which is measured when a powder density is equal to a tap density is 0.150 Ω▪cm or less [as required by claim 3];
However, it has been held that a rejection under 35 USC 102 or 103 can be made when the prior seems to be identical, but is silent as to an unreported or unrecognized but present property (MPEP 2112 III). Moreover, it has been held that the prior art need not recognize intrinsic properties of a material (MPEP 2112 II) as in the recited properties.
In this case, Akasaka doesn’t test and report density index and volume resistivity when the powder density is equal to a tap density as does applicant, but similar to applicant, does teach that the negative electrode material comprises a graphite core with carbonaceous coating and does teach a circularity of 0.90 or more (paragraph [0169-0170]), thus teaching a negative electrode material which is structurally similar to that claimed.
Additionally, in consideration of applicant’s remarks on the record suggesting that the inclusion of a microparticulate carbon material such as carbon black is critical to achievement of the recited properties (e.g. applicant’s arguments filed on 9/14/23), Akasaka further teaches that the active material may include carbon black as a conductive aid (paragraph [0134]) and/or as a subcomponent of the deposited layer (carbonaceous particle D of abstract is deposited on the surface of spherical graphite particle B; carbonaceous particle D may be microparticles such as carbon black and the like as described in paragraph [0108]).
Moreover, Akasaka teaches that the negative electrode material may be made by a process including coating a graphite precursor with heavy oil, heat treating the coated composite at 1100 C in inert gas, and calcining and crushing the formed product (paragraph [0168]; see also paragraph [0006]). This is similar to the technique taught by applicant as effective to produce the claimed invention (e.g. applicant’s published paragraphs [0061]; see also [0041, 0127]).
Finally, in terms of performance, applicant teaches that the claimed density index property is associated with excellence in terms of low-temperature output characteristic, fast charge-discharge characteristic, and cycle characteristic for the negative electrode material (applicant’s published paragraph [0026]). Akasaka further teaches that his inventive negative electrode has desirable low temperature characteristics, input/output characteristics, and cycle characteristics (abstract, paragraph [0009, 0011]).
Since the prior art teaches a negative electrode material which is substantially the same in terms of disclosed structure and method of manufacture and provides the same performance improvements [excellence in terms of low-temperature output characteristic, fast charge-discharge characteristic, and cycle characteristic], the same or substantially the same properties [the same density index and volume resistivity property] would be expected of the prior art product, if measured as described by applicant. Accordingly, the claimed invention is unpatentable over Akasaka with the claimed density index and volume resistivity properties being implicitly present.
Alternatively, it has been held that a prima facie case of obviousness exists when a product suggested by the prior art has a property which does not lie within the claimed range, but is close that a skilled artisan would have expected the claimed product and the prior art product to perform in the same manner due to substantially the same properties. (MPEP 2144.05) Here, the claims are alternatively obvious over Akasaka because even if the Akasaka negative electrode material possessed density index and volume resistivity values lying outside the claimed range, the difference is not so great as to suggest a product which behaves in a significantly different manner. The characteristics disclosed by Akasaka are similar to that of applicant’s invention as discussed above in detail.
Regarding the 1/14/26 amendment to claim 1, Akasaka further teaches the negative electrode material consists of a distribution of particles having a single volume average particle size from 3 µm to 50 µm (Akasaka describes a bimodal distribution of particles A, which have a d50 value of most preferably 7 to 12 µm (paragraph [0018]), and particle B which have a d50 value of most preferably 10 to 20 µm (paragraphs [0018, 0057]); a bimodal distribution of particles still possesses a single volume average particle value obtainable by number-averaging the average size value of each of the two peaks. In this case, the single volume average particle size would have a value lying between 3 µm and 20 µm, i.e. above the lower limit of the smaller particles and below the upper limit of the larger particles).
It is noted that either the mixture of particles A and particles B, or just the particle B, could be read on the “a negative electrode material” of claim 1. If only the particle B are read on the “a negative electrode material”, the volume average particle size lies in the range of 10 to 20 µm. But if the composite include both particles A and particles B are read on the “a negative electrode material”, then the volume average would be reduced from that of the particles B alone to a value still lying within the claimed range, as described above.
Additionally, it is noted that Akasaka teaches the particles “B” as actually comprised of spherical graphite particles “C” with carbonaceous material such as carbon black particles “D” deposited on the surface (claim 2, paragraph [0010]). The particles D are nanoparticles (paragraph [0110]) deposited on the surface of graphite particles C for the benefit of improving low temperature properties (paragraph [0054]). In this rejection as previously set forth, the particles D are interpreted to be a subcomponent of the particles B; therefore, the presence of the nanoparticles D is not interpreted to change the “volume average particle size”, which is determined by the mixture of the particles A and B.
Alternatively, in the battery art, Kim teaches that graphite particles of a negative electrode material may be coated with amorphous carbon for the same benefit of improving low temperature properties and/or protecting the graphite particle from unwanted exfoliation caused by the electrolyte (paragraph [0023]).
Moreover, in the battery art, Tsujiko teaches that graphite particles may be coated with an amorphous carbon material made by heating a precursor material such as phenol resin (paragraph [0047]) for the benefit of improving low temperature properties and/or improving compression breaking strength of the graphite particle (paragraph [0015]).
Therefore, it would have been obvious to a person having ordinary skill in the art at the time of invention to substitute the carbon nanoparticle layer D of Akasaka with an amorphous carbon layer, since both graphite particle coatings provide the same or similar benefit of improving low temperature properties, as taught by Kim or Tsujiko, and the amorphous layer further includes a benefit of protecting the graphite from undesired exfoliation as taught by Kim and compression strength as taught by Tsujiko.
In this case, the contribution of the nanoparticles D to the volume average particle size can be omitted as they would not be present, leaving the volume average particle size within the claimed range as described above.
Regarding claim 5, Akasaka remains as applied to claim 1. Akasaka further teaches that the Raman value of the carbon material may preferably between 0.2 and 1.5 (paragraph [0065, 0104]), a range which falls within the claimed range.
Regarding claim 10, Akasaka remains as applied to claim 1. Akasaka does not expressly teach wherein the negative electrode active material has a circularity of 0.94 or more.
However, Akasaka paragraph [0021] generally teaches circularity of 0.92 or more, while paragraph [0169] and Table 1 teach exemplary values with circularity as 0.93.
Claim 10 is therefore found to be obvious over Akasaka as the prior art discloses a preferred range substantially overlapping the claimed range (MPEP 2144.05), and gives examples which are close enough to the claimed range (0.93 vs 0.94) that a skilled artisan would have expected substantially the same consequential results.
Regarding claim 12, Akasaka remains as applied to claim 1. Claim 12 further requires that a ratio d90/d10 of the negative electrode material is 2.5 or more. Akasaka does not appear to teach a preferred d90/d10 range for the negative electrode active material as a whole, and therefore does not expressly teach that a ratio d90/d10 of the negative electrode material is 2.5 or more.
However, Akasaka does teach a negative electrode material comprised of a mixture of particles A and B (see abstract), wherein: i) the particles A have a d10 value most preferably in the range of 2 to 9 microns (paragraph [0024]) and a d90 value most preferably in the range of 12 to 15 microns (paragraph [0026]); ii) the particles B have a d10 value most preferably in the range of 5 to 20 microns (paragraph [0060]) and a d90 value most preferably in the range of 15 to 40 microns (paragraph [0061]); and iii) the mixture of A and B type particles may preferably include 3 to 6 mass % of type A, implying 94 to 97% B particles (paragraph [0117]).
Since the B particles are thus the primary component, the d90/d10 distribution of the composition of the negative electrode active material as a whole, should be similar to that of the B particles, but broadened by the presence of the added A particles. The midpoint of the paragraph [0060] B particle d10 range is 12.5, while the midpoint of the d90 range is 27.5, suggesting a midpoint d10/d90 ratio of 2.5. Although the midpoint values have been used in this simple calculation, the disclosure of Akasaka is broader than only the midpoint values, suggesting a broader range than this. Further including a small amount of the A type particles would be expected to broaden this distribution range, so as to suggest a total d90/10 value of a value which is greater than 2.5, as claimed. Therefore, the requirement that a ratio d90/d10 of the negative electrode material is 2.5 or more is found to be obvious over the disclosure of Akasaka, which suggests a range overlapping the claimed range.
Alternatively, it is noted that applicant’s remarks suggest that Akasaka teaches a d90/d10 value of 2.4 (5/23/25 remarks at page 7; see also the Examiner’s Response to Arguments section above which identifies an apparent source for the 2.4 value). The value 2.4 is very close to the claimed range of 2.5 or greater. As described in MPEP 2144.05, a prima facie case of obviousness exists which the range/value suggestion by the prior art does not overlap the claimed range, but is close enough that substantially the same properties are expected. Here, applicant’s originally filed disclosure does not explain why a d90/d10 value of 2.4 is substantially different from the claimed range of 2.5 or greater; therefore, a prima facie case of obviousness exists, even without overlap.
Relevant or Related Art
The prior art made of record and not relied upon is considered pertinent to applicant's disclosure, though not necessarily pertinent to applicant’s invention as claimed.
Choi (USP 6391495): negative electrode material comprising graphite core and amorphous carbon coating.
Nanba (US 2006/0133980): negative electrode material comprising graphite core and amorphous carbon coating.
Ikado (US 2019/0334173): negative electrode material comprising graphite core and amorphous carbon coating.
Conclusion
Applicant's amendment necessitated the new ground(s) of rejection presented in this Office action. Accordingly, THIS ACTION IS MADE FINAL. See MPEP § 706.07(a). Applicant is reminded of the extension of time policy as set forth in 37 CFR 1.136(a).
A shortened statutory period for reply to this final action is set to expire THREE MONTHS from the mailing date of this action. In the event a first reply is filed within TWO MONTHS of the mailing date of this final action and the advisory action is not mailed until after the end of the THREE-MONTH shortened statutory period, then the shortened statutory period will expire on the date the advisory action is mailed, and any nonprovisional extension fee (37 CFR 1.17(a)) pursuant to 37 CFR 1.136(a) will be calculated from the mailing date of the advisory action. In no event, however, will the statutory period for reply expire later than SIX MONTHS from the mailing date of this final action.
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/JEREMIAH R SMITH/Primary Examiner, Art Unit 1723