DETAILED ACTION
Introductory Notes
Any paragraph citation of the instant is in reference to the U.S. published patent application.
Claim Interpretation
Claims 1, 10, and 19 recite the limitation “an average particle size of the first active material is greater than an average particle size of the second active material”. Notably paragraph [0037] of the instant specification states “In this application, when the difference between the average particle size of the second active material and the average particle size of the first active material is not more than 10%, it is believed that the average particle size of the second active material and the average particle size of the first active material are identical”. Therefore, the limitation is being interpreted such that the first active material is greater than an average particle size of the second active material by more than 10%.
Claim Rejections - 35 USC § 103
The text of those sections of Title 35, U.S. Code not included in this action can be found in a prior Office action.
Claims 1-2, 4-6, 8, 10-11, 13-15, 17, and 19-22 are rejected under 35 U.S.C. 103 as being unpatentable over Subbaraman (US 20180358659 A1) in view of Lee (US 20160329567 A1, hereinafter Lee) in view of Lee (KR 20140080837 A, hereinafter KR’837, supplied with an IDS, English translation used for citations) in view of Kang (US 20200185768 A1).
Regarding claims 10 and 19, Subbaraman teaches an electronic device (see “electronic devices and electric and hybrid-electric vehicles” in [0003]) comprising an electrochemical device (see 100, fig. 1, and [0013]) comprising a positive electrode (see 140, fig. 1, and [0013]); and a separator located between the positive electrode and the negative electrode (see 130, fig. 1, and [0016]).
Regarding claims 1, 10, and 19, Subbaraman teaches a negative electrode (see 128, fig. 1 and [0015]), comprising: a negative electrode current collector (see 110, fig. 1 and [0013]), a first active material layer (see “second ad-layer”, 125, fig. 1 and [0015]), and a second active material layer (see “first ad-layer”, 120, fig. 1 and [0015]); wherein the second active material layer (see “first ad-layer”, 120, fig. 1 and [0015]) is located between the negative electrode current collector (see 110, fig. 1 and [0013]) and the first active material layer (see 125, fig. 1); the first active material layer (see “second ad-layer”, 125, fig. 1 and [0015]) comprises a first active material (see "the second ad-layer 125 includes materials which are ionically conductive to Li ions" in [0015]) and a target compound (see “Li3N” in [0015]), the target compound (see “Li3N” in [0015]) comprising AxBy (see “Li3N” in [0015]), wherein 0 < x < 4, 0 < y < 8 (see “Li3N” in [0015], where x = 3, and y = 1); A comprises a metal element (see “Li3N” in [0015], where A = Li which, is a metal) comprising at least one selected from the group consisting of Li, Na, Mg, Ca, Zn, and Cs (see “Li3N” in [0015], where A = Li); and B comprises a non-metallic element (see “Li3N” in [0015], where B = N, which is a non-metal) comprising at least one selected from the group consisting of N, S, and Si (see “Li3N” in [0015]), wherein the first active material is graphene oxide ([0014] discloses graphene oxide while [0015] discloses a mixed first ad-layer); the second active material layer comprises a second active material [0015]; but does not disclose wherein the first active material is one selected from the group consisting of artificial graphite, natural graphite, coke, silicon-oxygen compound, and silicon-containing metal.
Lee discloses a protective layer for an anode which describes graphene oxide or particles of metal silicate [0088].
Since the prior art of Lee recognizes the equivalency of graphene oxide and particles of metal silicate in the field of anode protective layers, it would have been obvious to one of ordinary skill in the art at the time of filing to replace the graphene oxide of Subbaraman with the particles of metal silicate of Lee as it is merely the selection of functionally equivalent inorganic materials protection materials recognized in the art and one of ordinary skill in the art would have a reasonable expectation of success in doing so.
Modified Subbaraman does not expressly teach an average particle size of the first active material is greater than an average particle size of the second active material.
KR’837 is directed to electrode structure having multiple layers like Subbaraman. KR’837 discloses “size of the first [note: furthest from current collector] negative electrode active material particles is larger than the size of the second [note: closest to the current collector] negative electrode active material particles” (page 6, line 3 of the translation). Regarding the naming and ordering of layers in KR’837 see Fig. 2 (provided below) as well as the final paragraph of page 5 of the translation bridging to page 6. KR’837 provides example with a top layer of “graphite with a particle size of 25 µm” [0041] and a bottom layer of “graphite with a particle size of 10 μm” [0043], fully reading on the limitation.
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KR’837 teaches the “advantage of being able to improve the slow electrode reaction speed of the second coating layer” (page 6 line 8 of the translation) and as such “the output characteristics can be improved” (page 6 final paragraph of the translation).
Before the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to utilize the particle sizes of KR’837 for the layers of modified Subbaraman to improve output characteristics by improving the reaction speed of the second coating layer.
Therefore, modified Subbaraman discloses an average particle size of the first active material is greater than an average particle size of the second active material (as taught by KR’837).
Modified Subbaraman does not expressly teach the mass percentage of AxBy.
Kang is directed to an anode for a secondary battery like Subbaraman. Kang discloses that the “first anode active material layer 22 [note furthest layer from current collector] may include an anode active material and an ionic compound” [0035] and that the “ionic compound included in the first anode active material layer 22 may be, for example, a metal salt compound including a metal cation” [0038] where “the metal salt compound may include, for example, an alkali metal element such as Li, Na” [0038] and the specific lithium salts may include “Li2S … Li3N” [0040].
Kang discloses the ionic compound in the first anode active material layer 22 may be "3 wt % to less than about 50 wt %, about 3 wt % to about 30 wt %, or about 7 wt % to about 13 wt %" [0042]. Kang further discloses Examples 1-12 where the % of added ionic compound ranges from 3% to 80% with the highest efficiency coming from those examples with 10-20% ionic compound (see Table 2 and Examples [0097-0116]. While these values are reported in relation to the first anode active material layer, one of ordinary skill in the art would readily be able to apply the disclosure and teachings to the total mass of two layers.
Kang teaches “by the inclusion of the ionic compound in the first anode active material layer, the first anode active material layer may serve as a kind of an artificial solid electrolyte interface film” [0033] and that when the ionic compound is within the taught range “improved cycle characteristics” [0042] as well: “When the amount of the ionic compound is excessively small, a cycle characteristics improvement effect may be negligible. When the amount of the ionic compound is excessive, the amount of the anode active material may become relatively small, so that the first anode active material layer may not function properly” [0042].
Before the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to utilize the ionic compound percentages taught my Kang in the anode of modified Subbaraman. The motivation to do so being to serve to as an artificial SEI film and improve cycle characteristics.
Therefore, modified Subbaraman discloses AxBy has a mass percentage of 0.1% to 20%, based on a total mass of the first active material layer and the second active material layer (as taught by Kang).
Regarding claims 2 and 11, modified Subbaraman discloses all the limitations as set forth above and Subbaraman further teaches wherein AxBy is at least one selected from the group consisting of Li3N, Li2S, Na3N, Na2S, Ca3N2, CaS, Mg3N2, and MgS (see “Li3N” in [0015]).
Regarding claims 4 and 13, modified Subbaraman discloses all the limitations as set forth above and Subbaraman further teaches wherein the first active material layer (see “second ad-layer”, 125, fig. 1 and [0015]) has a thickness of h1 (see “thickness of the second ad-layer 125” in [0015]), and the second active material layer (see “first ad-layer”, 120, fig. 1 and [0015]) has a thickness of h2 (see “thickness of the first ad-layer 120” in [0014]). Subbaraman does not specifically teach wherein 10% < h1/(h1+h2) < 90%. However, the thicknesses for h1 and h2 can both be less than 1 micrometer (µm) and greater than 3 nanometers (nm) (see [0014]-[0015]). It would be obvious to a person having ordinary skill in the art before the effective filing date of the invention to modify the thickness of h1 to 0.9 µm, and h2 to 0.9 µm because Subbaraman teaches that these values can be used for the thickness of each layer, and it would yield the same result of conducting lithium ions and preventing dendrite formation in the battery (see [0014]-[0015]). 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. The examiner would like to note with the modification above that 10% < 0.9 µm /(0.9 µm + 0.9 µm) < 90%.
Regarding claims 5 and 14, modified Subbaraman does not specifically teach wherein 10% < h1/(h1+h2) < 50%. However, the thicknesses for h1 and h2 can both be less than 1 micrometer (µm) and greater than 3 nanometers (see [0014]-[0015]). It would be obvious to a person having ordinary skill in the art before the effective filing date of the invention to modify the thickness of h1 to 0.9 µm, and h2 to 0.9 µm because Subbaraman teaches that these values can be used for the thickness of each layer, and it would yield the same result of conducting lithium ions and preventing dendrite formation in the battery (see [0014]-[0015]). 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. The examiner would like to note with the modification above that 10% < 0.9 µm /(0.9 µm + 0.9 µm) < 50%.
Regarding claims 6 and 15, modified Subbaraman discloses all the limitations as set forth above and Subbaraman further teaches wherein, the first active material (see "the second ad-layer 125 includes materials which are ionically conductive to Li ions" in [0015]) has a capacity per gram of c1 (Li3N has a capacity of 1761 mAh/g, according to “Sun et al.,”); the second active material (see “the first ad-layer 120 includes materials that are ionically conductive” in [0014]) has a capacity per gram of c2 (see “Mesocarbon microbeads data”, where the capacity is 327 mAh/g). As discussed in the rejection of claim 1, KR’837 teaches “size of the first negative electrode active material particles is larger than the size of the second”; therefore, given that c1 is larger than c2 for modified Subbaraman it holds that c1 x d1 > c2 x d2 (1761 mAh/g > 327 mAh/g; wherein the difference only gets larger as d1 increases relative to d2).
Regarding claims 8 and 17, modified Subbaraman discloses all the limitations as set forth above and Subbaraman further teaches wherein the second active material layer (see “first ad-layer”, 120, fig. 1 and [0015]) comprises a second active material (see “the first ad-layer 120 includes materials that are ionically conductive” in [0014]), and a capacity per gram of the first active material (see "the second ad-layer 125 includes materials which are ionically conductive to Li ions" in [0015]) is greater than or equal to a capacity per gram of the second active material (the capacity of the first active material, Li3N is 1761 mAh/g, according to “Sun et al.,”, and the capacity of the second active material is 327 mAh/g according to “Mesocarbon microbeads data”).
Regarding claims 20, 21, and 22, modified Subbaraman discloses all the limitations as set forth above and Kang discloses that the “ionic compound included in the first anode active material layer 22 may be, for example, a metal salt compound including a metal cation” [0038] where “the metal salt compound may include, for example, an alkali metal element such as Li, Na” [0038]. Given Kang’s teaching of Na and the relationship of Li and Na per the periodic table, it would have been obvious to one of ordinary skill in the art at the time of filing that both Li and Na may be used as the metal for the ionic compound. Therefore, modified Subbaraman discloses A comprises the metal element comprising at least one selected from the group consisting of Na, Mg, Ca, Zn, and Cs (as taught by Kang).
Claims 7 and 16 are rejected under 35 U.S.C. 103 as being unpatentable over Subbaraman in view of Lee in view of KR’837 in view of Kang and in further view of Ise (US 20190296327 A1).
Regarding claims 7 and 16, modified Subbaraman discloses all the limitations as set forth above and modified Subbaraman does not teach wherein the first active material has an average particle size of 6µm < d1 < 20 µm.
However, Ise teaches wherein active material has an average particle size of 6µm < d1 < 20 µm (see “the average secondary particle size of the active material preferably ranges from 1 μm to 50 μm” in Ise [0063]).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the invention to modify the size of the first active material of modified Subbaraman to be within the range of 6µm < d1 < 20 µm as taught by Ise to improve battery productivity at the time of manufacture, and battery performance (see Ise [0063]). Further, Subbaraman teaches that various changes may be made to the device without departing from the disclosed subject matter (see Subbaraman [0026]).
Response to Arguments
Regarding art-based rejections, applicant’s arguments with respect to the amendment regarding to what extent Li (US 20 180301745 A1) taught a mass percentage of 0.1-20% (previous claim 3) have been considered and are persuasive. Notably the rejections of currently amended claims 1 and 10 are not in view of Li. It is also noted that in the previous claim set of 11/13/2025, claim 3 and twin claim 12 were to the mass percentage of the target compound where the target compound comprised AxBy, but did not consist of only AxBy. In currently amended claims 1 and 10, the mass percentage is in relation to AxBy alone. As such the currently amendments are narrower in scope than previous claims 3 and 12.
Conclusion
The prior art made of record and not relied upon considered pertinent to applicant's disclosure (previously cited):
He (US 20190386342 A1) directed to improving anode stability by implementing two anode-protecting layers wherein graphite may be present in two protective layers [0031] and the top protective layer (relative to the current collector being bottom) may include Li2S or Na2S.
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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/T.L.M./Examiner, Art Unit 1721
/ALLISON BOURKE/Supervisory Patent Examiner, Art Unit 1721
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