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 .
Response to Amendment
This is a final Office action in response to Applicant’s remarks and amendments filed on 04/17/2026. Claims 1 – 9 are amended. Claims 1 – 9 are pending in the current Office action.
The objection to claim 2 set forth in the previous Office action is withdrawn in light of applicant’s amendment.
Applicant’s amendment changes the scope of the claimed invention by requiring the composite particles to be of a crushed sintered material and further defining the structure of the lithium zirconate phase and silicon phase. As a result of applicant’s amendment: (1) The 35 U.S.C. 102 and 103 rejections made in view of Tahara are withdrawn; (2) the 35 U.S.C 102 and 103 rejections of claims 1 – 2 and 4 – 9 made in view of Watanabe are withdrawn, and a new grounds of rejection necessitated by applicant’s amendment, specifically a 35 U.S.C. 103 rejection utilizing Watanabe as the primary reference, is established below ; and (3) the 35 U.S.C 103 rejections of claims 1 – 9 made in view of Tahara and Watanabe are withdrawn, and a new grounds of rejection necessitated by applicant’s amendment, specifically rejection utilizing the combination of Tahara and Watanabe and citing new teaching to support structural obviousness, is established below.
Response to Arguments
Applicant’s arguments, see pgs. 14 – 16, file 04/17/2026, with respect to the 102 and 103 rejections made in view of Tahara, have been fully considered and are persuasive. Accordingly, the of 35 U.S.C. 102 and 103 rejections made in view of Tahara have been withdrawn.
Applicant's arguments filed 04/17/2026 regarding Watanabe failing to teach/render obvious the claimed composite particle structure as amended, see pgs. 7 – 12, have been fully considered but they are not persuasive in light of the following:
The examiner acknowledges that Watanabe does not explicitly disclose the feature of “the composite particles are a crushed sintered material obtained by crushing a sintered body, the sintered body is obtained by sintering a composite intermediate containing the lithium zirconate phase and the silicon phase and the lithium zirconate phase has a continuous phase derived from the sintered body, within the composite particles, and a sea-island structure in which the silicon phase is dispersed like islands in a continuous phase”; however, as established in the rejections below, by reciting “obtained by crushing a sintered body” and “is obtained by sintering a composite intermediate containing the lithium zirconate phase and the silicon phase” the claim recites a product-by-process limitation requiring a sintering and crushing step. The examiner further notes that, the structure implied by the claimed sintering and crushing process step is broad enough to include a composite particle structure formed by crushing and then sintering since the conditions/degree of sintering and crushing are not specified in the claim {i.e. under broadest reasonable interpretation, the scope of a process of sintering for a period of time and then crushing would necessarily embrace the scope of a composite particle structure equivalent to a process where crushing is performed prior to the sintering step}. Therefore, a composite particle formed form the mechanochemical process taught by Watanabe which is a process involving crushing {i.e. grinding, [0070 – 0071]} followed by sintering {i.e. heat treatment at a temperature of preferably 120°C to 1400°C, [0076 – 0078]} corresponds to the crushed sintered material as claimed.
Drawings
The corrected drawings filed 04/17/2026 are acknowledged and accepted. Furthermore, in light of filed drawings, the objection to the drawings established in the previous Office action is withdrawn.
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.
Claim(s) 1 – 3 and 8 – 9 are rejected under 35 U.S.C. 103 as being unpatentable over Watanabe (JP2013239267A, cited in previous O.A. mailed 02/27/2026)
Regarding Claim 1, Watanabe discloses composite particles for a non-aqueous electrolyte secondary battery (Fig. 1, [0031 – 0032];[0041]).
In example 4, Watanabe explicitly discloses an embodiment of the composite particle in which the amorphous/low crystalline solid electrolyte matrix of the particle 2 is specifically Li7La3Zr2O12 (Refer to Example 4 in Table 1 and [0116]), which one with ordinary skill in the art would recognize to be a type of lithium zirconate.
In the instant specification, the lithium zirconate phase is described as a lithium zirconate containing Li, Zr, and O where the atomic ratio of O to Zr is, for example, 2.0 or greater and 6.0 or less ([0025]) . Additionally, the applicant teaches that the lithium zirconate phase can also include at least one selected from the group consisting of: Na, K, Ca, Mg, B, P, and La ([0027]).
Therefore, by disclosing an embodiment of the composite particle where the matrix is a lithium zirconate which appears to be within the scope of zirconates taught in the instant specification, Watanabe further discloses the claimed structure of wherein each composite particle include a lithium zirconate phase {i.e. Li7La3Zr2O12 matrix which would be 2 in Fig. 1}, and a silicon phase dispersed in the lithium zirconate phase, that is Watanabe explicitly discloses dispersing Si nanoparticles 1 in the solid electrolyte matrix of the composite particles (Fig. 1, [0038 – 0041];[0116]), and one with ordinary skill in the art would reasonably expect the nanoparticles to provide the claimed phase, because in the instant specification, the silicon phase is taught to be particulate/formed from silicon raw materials such as silicon nanoparticles ([0045 – 0048];[0059 – 0060]).
Watanabe does not explicitly disclose the composite particles being a crushed sintered material obtained by crushing a sintered body, the sintered body obtained by sintering a composite intermediate containing the lithium zirconate phase and the silicon phase; however, by reciting “obtained by crushing a sintered body” and “obtained by sintering a composite intermediate containing the lithium zirconate phase and the silicon phase” the claim recites a product-by-process limitation requiring a sintering and crushing step. The examiner further notes that, the structure implied by the claimed sintering and crushing process step is broad enough to include to include a composite particle structure formed by crushing and then sintering since the conditions/degree of sintering and crushing are not specified in the claim {i.e. under broadest reasonable interpretation, the scope of a process of sintering for a period of time and then crushing would necessarily embrace the scope of a composite particle structure equivalent to a process where crushing is performed prior to the sintering step}.
Watanabe, as an alternative to a sol-gel process, teaches forming the composite particles using a mechanochemical process where the raw materials are first grinded {i.e. equivalent to crushing} and then heat treated at a temperature of preferably 120°C to 1400°C {i.e. equivalent to sintering} ([0069 – 0071];[0076 – 0078]). As such, Watanabe also teaches, composite particles that are a crushed and sintered material, and further of a structure that could result from the claimed sintering and crushing steps and thus correspond to composite particle structure as claimed.
Although Watanabe does not disclose an example of the LLZO matrix-including composite particle formed from the mechanochemical method, It would have been obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, to form the particle of Example 4 using the mechanochemical method, as taught by Watanabe, with a reasonable expectation of success in forming the desired composite particle, because, Watanabe presents the mechanochemical method as an obvious variant to the sol gel method utilized in Example 4 ([0044 – 0045];[0069]) [See MPEP 2144.06(II)]).
Furthermore, by forming the composite particle by the taught mechanochemical method, the composite particle as established above, corresponds to the composite material structure as claimed.
Additionally, in the modified example above, the LLZO matrix {i.e. corresponds to claimed lithium zirconate phase}, reads on being a continuous phase inherently formed in the sintered body within the composite particles because it is a portion of the composite particle formed by a process including a sintering step and has a structure that surrounds and isolates the silicon nanoparticles of the composite particle (Refer to 2 in Fig. 1, [0039 – 0041]); and the silicon nanoparticles {i.e. corresponds to claimed silicon phase} read on being a sea-island structure in which the silicon phase is dispersed like islands in the continuous phase, because the silicon nanoparticles of the composite particles are dispersed within the matrix such that they are in a non-contact state (Refer to 1 in Fig. 1, [0040]).
Regarding Claim 2, modified Watanabe discloses all limitations as set forth above. For example 4, Watanabe teaches preparing the Li7La3Zr2O12 solid electrolyte raw material so as to have a molar ratio of Li:La:Zr = 7.7:3:2 and further teaches forming the composite from a mass ratio of nanosilicon: oxide solid electrolyte of 1:1 ([0115 – 0116]).
Watanabe does not explicitly disclose the content proportion zirconium {i.e. MZr} and the content proportion of lithium {i.e. MLi} with respect to all elements other than oxygen; however, one with ordinary skill in the art would recognize that such proportions could be determined based on the mass and molar ratios taught by Watanabe as well as the atomic weights of Li, La, and Zr. Specifically, based on the molar ratio of Li:La:Zr:O and the atomic weights of Li, {i.e. 6.94 g/mol}, La {138.91 g/mol}, Zr {i.e. 91.22 g/mol}, and O {i.e. 16 g/mol}, Watanabe suggests a solid electrolyte raw material having the following: a total weight excluding oxygen of 652.61 g; a total weight including oxygen of 844.61 g; and, excluding the weight of oxygen, a mass percent of Li and a mass percent of Zr of 8.19% and 27.96%, respectively. Assuming 1g of Si and 1 g of solid electrolyte {i.e. 1:1 mass ratio} and considering the fraction of the solid electrolyte raw material excluding oxygen {i.e. 652.61 g / 844.61 g}, the mass of non-oxygen elements making up the solid electrolyte raw material is 0.7728 g and the total mass of non-oxygen elements making up the composite is 1.7728 g. Therefore, based on the total mass of non-oxygen elements making up the composite and the mass fractions of Zr and Li in the solid electrolyte raw material excluding oxygen, in example 4 of Watanabe, a content proportion of zirconium {i.e. MZr} is ≈ 15.8 mass%, which is within the claimed 14.6 mass% or more and 54.6 mass% or less, and a content proportion of lithium {i.e. MLi} is 4.62 mass% (Claim 2).
Regarding Claims 3, modified Watanabe discloses all limitations as set forth above. As established above, based on the total mass of non-oxygen elements making up the composite and the mass fractions of Zr and Li in the solid electrolyte raw material excluding oxygen, in example 4 of Watanabe, the content proportion of zirconium {i.e. MZr} is ≈ 15.8 mass% and the content proportion of lithium {i.e. MLi} is 4.62 mass%. As such, Watanabe exemplifies a ratio of the content proportion of MLi to the content proportion of MZr, calculated with the content proportion MZr taken as 100, of 29.
Therefore, Watanabe does not explicitly disclose an embodiment in which the ratio is 4.7 or greater and 23.2 or less.
However, generally, when utilizing a lithium lanthanum zirconate solid electrolyte, Watanabe teaches having the solid electrolyte represented by: Li7+xLa3Zr2O12+(x/2) where -5 ≤ x ≤ 3 ([0036]); thus, Watanabe suggests using lithium zirconates in which the molar proportion of the Li is smaller than what is exemplified in example 4. Furthermore, Watanabe teaches generally having the content of Si nanoparticles in the composite be preferably 5 mass% or more and 90 mass% or less for the purpose of achieving sufficient battery capacity {i.e. is increased by increasing the amount of Si nanoparticles} and effective suppression of the expansion/contraction of the Si nanoparticles {i.e. is decreased by increasing the amount of Si nanoparticles}. Watanabe further teaches that the ratio of oxide solid electrolyte matrix to Si is important for improving the initial capacity and cycle characteristics ([0142]).
One with ordinary skill in the art would appreciate/recognize that, in the composite of Watanabe, the content of Si and molar ratio of Li, would affect the ratio of the content proportion of MLi to the content proportion of MZr, and that because Watanabe teaches molar ratios which reduce the content Li in the lithium lanthanum zirconate, Watanabe necessarily also teaches/suggests compositions of composite particles that would provide MLi to MZr ratios overlapping/at least encompassing claimed range.
Selection of content proportion ratio within the overlapping portion of the ranges would have been prima facie obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, because such a selection would have a reasonable expectation of success in arriving at a lithium lanthanum zirconate solid electrolyte matrix with the conductivity and electrochemical durability desired by Watanabe ([0036]) [See MPEP 2144.05(I)].
Furthermore, selection of a ratio within the overlapping portion would have been further obvious to optimize the proportion of Si nanoparticles and solid electrolyte material in the composite {i.e. increasing battery capacity vs. achieving suppression of expansion/contraction of nanoparticles} while also ensuring that the lithium zirconate solid electrolyte is of a composition that provides the durability and conductivity desired by Watanabe, with a reasonable expectation of success and without undue experimentation [MPEP 2144.05(II)].
Regarding Claim 8, modified Watanabe discloses all limitations as set forth above. By disclosing an embodiment in which the solid electrolyte matrix is Li7.7La3Zr2O12 ([0116]), Watanabe further discloses wherein the lithium zirconate phase contains lanthanum, which is within the claimed scope of at least one element selected from the group consisting of sodium, potassium, calcium, magnesium, boron, phosphorous, and lanthanum.
Regarding Claim 9, modified Watanabe discloses a non-aqueous electrolyte secondary battery ([0079];[0088]), comprising a positive electrode ([0089 – 0091]), a negative electrode ([0079 – 0083]), wherein the negative electrode includes the composite particles (Refer to rejection of claim 1 above and [0029]).
Claim(s) 4 – 7 are rejected under 35 U.S.C. 103 as being unpatentable over Watanabe, as applied to claim 1, and further as evidenced by Tahara (WO 2017199606A1, cited in previous O.A. mailed 02/27/2026) and Il’ina ("Morphology and transport properties of the solid electrolyte Li7La3Zr2O12 prepared by the solid-state and citrate–nitrate methods." Journal of Power Sources 201 (2012), pp. 169-173, cited in previous O.A. mailed 02/27/2026).
Regarding Claims 4 –7, modified Watanabe discloses all limitations as set forth above. In modified Watanabe, the matrix is taught to be formed around the Si nanoparticles by mechanochemical method where the heat treatment step is carried out at preferably 120°C to 1400°C ([0069 – 0078]). The composite of example 4, which includes the Li7.7La3Zr2O12 matrix, was formed from being heat treated 800°C ([0115 – 0116]).
Modified Watanabe does not explicitly disclose wherein the lithium zirconate phase contains at least one selected from the group consisting of Li6Zr2O7, Li2ZrO3, and Li5.52Zr2.62O8 (Claim 4) and, in an X-ray diffraction pattern of the composite particles obtained by X-ray diffraction measurement, a peak attributed to the lithium zirconate phase appears around 2θ = x°, and the x° is at least one selected from 18.6°, 26.5°, and 36.5° (Claim 5); however one with ordinary skill in the art would reasonably expect the composite of example 4 in Watanabe when measured by X-ray diffraction to provide at least one lithium zirconate within the claimed list and further at an angle within the claimed selection for the following reasons:
Tahara, directed toward composite particles including Si particles covered by conductive coating and a Li-containing oxide, teaches that crystal phases of Li-containing oxides are affected by heat treatment temperature, and that Li-containing oxides including metal oxides such as ZrO2, prepared from sol gel or mechano-chemical means, at heat treatment temperatures at 600°C or higher, provide mixed phase or single phases of amorphous or crystalline phase ZrO2 (monoclinic crystal, tetragonal), Li2ZrO3, Li6Zr2O7, Li8ZrO6 ([14];[16];[18]).
Il’ina, which is particularly directed to LLZO solid electrolytes, shows that Li7La3Zr2O12 synthesized at temperatures lower than 1200°C {i.e. particularly 900°C} and prior to sintering, possess a plurality of peaks corresponding to ZrO2 at 2θ including ≈ 31° (Refer to peaks labeled with +) and Li2ZrO3 at 2θ including ≈ 19° (Refer to peaks labeled with *) present within their XRD patterns (See Fig. 1(a) and first paragraph of 3.Results and Discussion section on pg. 170).
Therefore, because Watanabe teaches forming a Li7.7La3Zr2O12 matrix around the Si particles at a heat treatment temperature of 800°C ([0115 – 0116]), which is within the range of temperatures taught to be capable of providing the lithium-containing, zirconium oxide phases in Tahara, and further is a temperature relatively close to the synthesis temperature {i.e. 900°C} shown by Il’ina to result in impurity peaks including Li2ZrO3 at 2θ such as ≈ 19°, one with ordinary skill in the art would reasonably expect the example composite particle of modified Watanabe to provide, when measure by X-ray diffraction, at least a phase peak corresponding to Li2ZrO3 at around 2θ = 18.6, and thus within the claimed scope.
Modified Watanabe further does not explicitly disclose wherein a ZrO2 phase is dispersed in the lithium zirconate phase (Claim 6) and, in an X-ray diffraction pattern of the composite particles obtained by X-ray diffraction measurement, a peak attributed ZrO2 phase appears around 2θ = 30.7° (Claim 7); however, one with ordinary skill in the art would reasonably expect the Li7.7La3Zr2O12 matrix in modified Watanabe to include a ZrO2 phase and further provide a peak attributed ZrO2 phase around 2θ = 30.7°, because, as established above, Watanabe teaches forming a Li7.7La3Zr2O12 matrix around the Si particles at a heat treatment temperature of 800°C ([0115 – 0116]), which is within the range of temperatures taught to be capable of providing the lithium-containing, zirconium oxide phases in Tahara, and further is a temperature relatively close to the synthesis temperature {i.e. 900°C} shown by Il’ina to result in phase peaks including ZrO2 at 2θ such as ≈ 31°.
Claim(s) 1 – 3 and 8 – 9 are alternately rejected under 35 U.S.C. 103 as being unpatentable over Tahara (WO 2017199606A1) in view of Watanabe (JP2013239267A).
Regarding Claim 1, Tahara discloses composite particles, that is Tahara teaches aggregate particles formed from a plurality of a Si particles that are covered by a Li-containing oxide and bonded by a conductive substance, which one with ordinary skill in the art would recognize to be a type of composite particle (Fig. 1; [08 – 11]), for a non-aqueous electrolyte secondary battery (Fig. 2; [09 – 11]).
Tahara teaches the composite particles being aggregate particles formed by aggregation of Li-containing oxide and Si particles having a conductive binder substance ([09]). As show in Fig. 1, the Li-containing oxide 30 covers the Si particles 20 of the composite particles. Tahara further teaches the Li-containing oxide being a matrix material containing Li and a metal oxide selected from SiO2, Al2O3, TiO2, and ZrO2 ([13]). In example 3, Tahara provides an embodiment of the composite particle using a Li-containing oxide that includes Zr as the metal of the metal oxide and further teaches that when the Li-containing oxide contains Zr, a Li-containing oxide coating of the mixed phase or single phase of
amorphous or crystalline phase ZrO2 (monoclinic crystal, tetragonal), Li2ZrO3, Li6Zr2O7, Li8ZrO6 is obtained (Table 1; [14];[44];[46]).
By teaching an embodiment of aggregate particles including Si particles coated by a lithium-containing oxide consisting of Zr, Tahara further discloses a composite particle comprising a lithium zirconate phase (Fig. 1, 30; [14];[44];[46];[59]) and a silicon phase (Fig. 1, 20; [21];[59]).
Tahara does not particularly disclose the silicon phase dispersed in the lithium zirconate phase.
Watanabe teaches composite particles for the negative electrode active material of a battery comprising Si nanoparticles 1 dispersed in a solid electrolyte matrix 2 (Fig. 1, [0038 – 0041];[0116]). The solid electrolyte that forms the matrix is taught to be Li ion conductive, oxide solid electrolytes that are amorphous/have low crystallinity and high ionic conductivity ([0032 – 0035]). Lithium zirconates are included among Watanabe’s taught solid electrolyte and the matrix suppresses the expansion and contraction of the individual Si nanoparticles, and therefore, the expansion and contraction of the entire negative electrode active material can be suppressed compared to when the Si nanoparticles are in contact with each other and form clumps ([0036];[0040]).
Therefore, it would have been obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, to form the composite particles of Tahara by dispersing the solid silicon particles in the Li-containing zirconate, and thus obtain the claimed composite particle structure, because, as shown by Watanabe, it is already known in the art to form composite negative electrode active material particles by dispersing Si particles in amorphous/low crystalline, conductive lithium zirconates, and such a modification would have a reasonable expectation of success, to provide the Li ion conductivity and particle stability {i.e. suppression of expansion/contraction of Si particles} effects desired by Tahara (Tahara: [08])
Modified Tahara, as established above, does not explicitly disclose the composite particles being a crushed sintered material obtained by crushing a sintered body, the sintered body obtained by sintering a composite intermediate containing the lithium zirconate phase and the silicon phase; however, by reciting “obtained by crushing a sintered body” and “obtained by sintering a composite intermediate containing the lithium zirconate phase and the silicon phase” the claim recites a product-by-process limitation requiring a sintering and crushing step. The examiner further notes that, the structure implied by the claimed sintering and crushing process step is broad enough to include to include a composite particle structure formed by crushing and then sintering since the conditions/degree of sintering and crushing are not specified in the claim {i.e. under broadest reasonable interpretation, the scope of a process of sintering for a period of time and then crushing would necessarily embrace the scope of a composite particle structure equivalent to a process where crushing is performed prior to the sintering step}.
Watanabe further teaches forming the matrix of solid electrolyte material around the Si nanoparticles by a sol-gel method or a mechanochemical method ([0044 – 0045]). In the mechanochemical method, the raw materials of the composite particle are first grinded {i.e. equivalent to crushing} and then heat treated at a temperature of preferably 120°C to 1400°C {i.e. equivalent to sintering} ([0069 – 0071];[0076 – 0078]). As such, Watanabe also teaches forming composite particles that are a crushed sintered material, and further of a structure that could result from the claimed sintering and crushing steps and thus correspond to composite particle structure as claimed.
It would have been further obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, when modifying the composite particles of Tahra to have the structure taught by Watanabe, to form the particles by the mechanochemical method as taught by Watanabe, with a reasonable expectation of success in achieving the desired particle structure that allows for enhanced ion conductivity and particle stability.
Furthermore, by forming the composite particle by the mechanochemical method taught by Watanabe, the composite particle of modified Tahara, as established above, correspond to the composite particle structure as claimed.
Additionally, in the modified example particle established above, the Li-Zr containing oxide matrix of modified Tahara {i.e. corresponds to claimed lithium zirconate phase}, reads on being a continuous phase inherently formed in the sintered body within the composite particles because it is a portion of the composite particle formed by a process including a sintering step and has a structure that surrounds and isolates the silicon nanoparticles of the composite particle (Watanabe: Refer to 2 in Fig. 1, [0039 – 0041]); and the silicon particles {i.e. corresponds to claimed silicon phase} read on being a sea-island structure in which the silicon phase is dispersed like islands in the continuous phase, because the silicon nanoparticles of the composite particles are dispersed within the matrix such that they are in a non-contact state (Watanabe: Refer to 1 in Fig. 1, [0040]).
Regarding Claims 2 – 3, modified Tahara discloses all limitations as set forth above. In example 3, the Li-containing oxide has a composition in which the molar ratio of Li and the metal element Zr, Zr/Li = 10 (Refer to Example 3 in Table 1). In modified Tahara, as established above, it is the Li-containing oxide in which the Si particles are dispersed in (Watanabe: (Fig. 1, [0038 – 0041];[0116]).
Modified Tahara does not explicitly disclose the composite particles having a content proportion MZr of zirconium relative to non-oxygen elements of 14.6 mass% or more and 54.6 mass% or less and a content proportion MLi of lithium relative to non-oxygen elements of 0.9 mass% or more and 10.4 mass% or less (Claim 2) or further wherein a ratio of MLi to MZr, calculated with MZr taken as 100, is 4.7 or greater and 23.3 or less (Claim 3).
Generally Tahara teaches controlling the molar ratio of the metal M to Li to be preferably 0.2 to 10 to prevent Li2O precipitates from causing defects, sufficiently ensure that contact between the active material and electrolytic solution is restricted and prevent increases in Li ion conduction resistance ([13]). When the metal Zr, the taught molar ratio provides a general mass ratio of Li/Zr of 6.94/912.2 ≈ 0.007 to 6.94/18.244 ≈ 38. As such, Tahara suggests Li-containing oxides with proportions of Zr as high as 99 wt% and as low as 73 wt%. The Li-containing oxide is further taught to be included in the composite in an amount of 0.5 – 10 mass% for the purpose of sufficiently preventing contact between the active material and electrolyte while also preventing increases in Li ion conduction resistance/deterioration in responsiveness of the electrode reaction ([12]).
Watanabe further teaches generally having the content of Si nanoparticles in the composite be preferably 5 mass% or more and 90 mass% or less for the purpose of achieving sufficient battery capacity {i.e. is increased by increasing the amount of Si nanoparticles} and effective suppression of the expansion/contraction of the Si nanoparticles {i.e. is decreased by increasing the amount of Si nanoparticles}. Watanabe further teaches that the ratio of oxide solid electrolyte matrix to Si is important for improving the initial capacity and cycle characteristics ([0142]).
Since the composite particles of modified Tahara have a composition/structure like the particles in Watanabe {i.e. compose of lithium zirconate and Si particles dispersed in the lithium zirconate} and thus contain an amount of Si particles that overlaps the amount the amount taught to be included in the applicant’s composite particles (Watanabe: [0042]; Instant Specification: [0049]), and since Tahara teaches lithium zirconate compositions in which have mass ratio of Li/Zr that encompasses the claimed ratio, one with ordinary skill in the art would reasonably expect modified Tahara content proportions of MLi, content proportions of MZr, and MLi / MZr ratios to overlap/at least encompass the claimed content proportion ranges and ratio range.
Selection of content proportions ratio within the overlapping portion of ranges and further content proportions that provide a ratio within the claimed range, would have been prima facie obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, because such a selection would have a reasonable expectation of success in arriving at a lithium coating capable of achieving the Li ion conductivity and stability desired by Tahara ([08]) [See MPEP 2144.05(I)].
One with ordinary skill in the art would also appreciate/recognize that, in the composite of modified Tahara, the amount of Si particles, the amount of Li-containing oxide and molar ratio of Li and Zr in the Li-containing oxide, would affect the content proportion of MLi, the content proportion of MZr, and the ratio of the content proportion of MLi to MZr.
Therefore, selection of content proportions within the overlapping portion of the ranges and further content proportions that provide a ratio within the claimed range would have further been obvious, before the effective filing date of the claimed invention, to optimize the molar ratios {i.e. Li/Zr} of the Li-containing oxide compositions {i.e. balance increases in resistances vs. formation of free Li2O precipitates}, the amount of lithium containing oxide in the composite {i.e. balance increases in resistance vs. sufficient particle coverage}, and the amount of conductive binder {i.e. balance increases in resistance vs. achieving sufficient expansion/contraction effect}, with a reasonable expectation of success and without undue experimentation [MPEP 2144.05(II)].
Regarding Claim 8, modified Tahara discloses all limitations as set forth above. For the Li-containing oxide of composite particles, Tahara generally teaches using Li-containing oxides having stable and high Li-ion conductivity ([13]). Furthermore, Tahara teaches and exemplifies using Lithium zirconates (Refer to Table 1, Example 3 and [13 – 14]).
Modified Tahara does not explicitly disclose wherein the lithium zirconate phase contains at least one element selected from the group consisting of sodium, potassium, calcium, magnesium, boron, phosphorus, and lanthanum.
As established above, Lithium zirconates are included among Watanabe’s taught solid electrolyte ([0035 – 0036]). Watanabe further teaches a preference for using Li7+xLa3Zr2O12+(x/2) where -5 ≤ x ≤ 3 because of its high electrochemical durability ([0036]). The solid electrolytes in Watanabe are also taught to have high ionic conductivity ([0034]).
It would have been obvious to one with ordinary skill in the art, before the effective filing date of the claimed invention, to have modified the lithium zirconate material of Tahara to include La, as taught by Watanabe, and thus obtain a lithium zirconate containing an element within the claimed list, with a reasonable expectation of success in obtaining a Li-containing oxide with the desired characteristic of high conductivity and further high electrochemical durability in the composite particles of Tahara.
Regarding Claim 9, Tahara discloses a non-aqueous electrolyte secondary battery (Fig. 2; [32]) comprising a positive electrode ([33 – 34]), a negative electrode ([29]), wherein the negative electrode includes the composite particles (Refer to rejection of claim 1 above and [27];[29]).
Claim(s) 4 – 5 and 6 – 7 are rejected under 35 U.S.C. 103 as being unpatentable over Tahara (WO 2017199606A1) and Watanabe (JP2013239267A), as applied to claim 1 above, and further as evidenced by Pfeiffer ("Reaction mechanisms and kinetics of the synthesis and decomposition of lithium metazirconate through solid-state reaction." Journal of the European Ceramic Society 24, no. 8, pp. 2433-2443, cited in previous O.A. mailed 02/27/2026).
Regarding Claims 4 – 7, modified Tahara discloses all limitations as set forth above. In example 3, Tahara provides an embodiment of the composite particle using a Li-containing oxide that includes Zr as the metal of the metal oxide and further teaches that when the Li-containing oxide contains Zr, a Li-containing oxide coating of the mixed phase or single phase of amorphous or crystalline phase ZrO2 (monoclinic crystal, tetragonal), Li2ZrO3, Li6Zr2O7, Li8ZrO6 is obtained (Table 1; [14];[44];[46]). The particle of modified Tahara is formed by a mechanochemical method including a heat treatment step performed at a temperature of 1000°C (Tahara: [44];[46] and Watanabe ([0069];[0077 – 0078]).
Modified Tahara does not particularly disclose, for the Zr-including embodiment of the composite particles, the lithium zirconate phase containing at least one selected from the group consisting of Li6Zr2O7, Li2ZrO3, and Li5.52Zr2.62O8 (Claim 4) and, in an X-ray diffraction pattern of the composite particles obtained by X-ray diffraction measurement, a peak attributed to the lithium zirconate phase appearing around 2θ = x°, and the x° being at least one selected from 18.6°, 26.5°, and 36.5° (Claim 5); however one with ordinary skill in the art would reasonably expect the modified composite of Tahara when measured by X-ray diffraction to provide at least one lithium zirconate within the claimed list and further at an angle within the claimed selection, because Pfeiffer, directed toward lithium zirconates consisting of Li, Zr, and O, shows an XRD pattern for lithium zirconate formed by heat treating at 1000°C, and in the XRD pattern peaks corresponding to phases Li2Zr2O3 at 2θ ≈ 36° (Refer to peaks labeled with + in Fig. 2) and ZrO2 at 2θ ≈ 31° (Refer to peaks labeled with diamond in Fig. 2) are shown (Fig. 2; First paragraph in 1. Introduction section, pg. 2433; (Refer to first and second paragraph of 3. Results and Discussion section, pg. 2434 – 2435).
As such, since modified Tahara teaches forming a Li-containing Zr oxide matrix at a heat treatment temperature of 1000°C (Tahara: [44];[46] and Watanabe ([0069];[0077 – 0078]), and already suggests obtaining phases such as ZrO2 (monoclinic crystal, tetragonal), Li2ZrO3, Li6Zr2O7, and/or Li8ZrO6 (Tahara: [14]), one with ordinary skill in the art would reasonably expect the example composite particle of modified Tahara to provide, when measured by X-ray diffraction, at least a peak corresponding to Li2ZrO3 at around 2θ = 36.5, and thus within the claimed scope since, as shown by Pfeiffer, heat treatment temperatures of 1000°C for lithium zirconates provide Li2ZrO3 as a phase and a peak corresponding to said phase at a 2θ of ≈ 36.
Modified Tahara further does not explicitly disclose a ZrO2 phase dispersed in the lithium zirconate phase (Claim 6) and, in an X-ray diffraction pattern of the composite particles obtained by X-ray diffraction measurement, a peak attributed ZrO2 phase appearing around 2θ = 30.7° (Claim 7); however, one with ordinary skill in the art would reasonably expect the Li-containing Zr oxide coating of modified Tahara to include a ZrO2 phase and further provide a peak attributed ZrO2 phase around 2θ = 30.7°, because, as established above, Tahara already suggests obtaining phases such as ZrO2 (monoclinic crystal, tetragonal), Li2ZrO3, Li6Zr2O7, and/or Li8ZrO6 (Tahara: [14]) and teaches forming the Li-containing Zr oxide matrix at a heat treatment temperature of 1000°C (Tahara: [44];[46] and Watanabe ([0069];[0077 – 0078]), which, as shown by Pfeiffer, is a synthesis temperature that provides a ZrO2 phase and a peak corresponding to said phase at a 2θ ≈ 31°.
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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/A.Y.O./Examiner, Art Unit 1751
/JONATHAN G LEONG/Supervisory Patent Examiner, Art Unit 1751 7/1/2026
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