DETAILED ACTION
Notice of Pre-AIA or AIA Status
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
Claim Rejections - 35 USC § 103
The following is a quotation of 35 U.S.C. 103 which forms the basis for all obviousness rejections set forth in this Office action:
A patent for a claimed invention may not be obtained, notwithstanding that the claimed invention is not identically disclosed as set forth in section 102, if the differences between the claimed invention and the prior art are such that the claimed invention as a whole would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to which the claimed invention pertains. Patentability shall not be negated by the manner in which the invention was made.
The factual inquiries for establishing a background for determining obviousness under 35 U.S.C. 103 are summarized as follows:
1. Determining the scope and contents of the prior art.
2. Ascertaining the differences between the prior art and the claims at issue.
3. Resolving the level of ordinary skill in the pertinent art.
4. Considering objective evidence present in the application indicating obviousness or nonobviousness.
Claims 1-7 and 14 are rejected under 35 U.S.C. 103 as being unpatentable over Tsuchiya et al. (WO 2019220576 A1) in view of Kawase et al. (US 20070105017 A1). It is noted that the disclosures of Tsuchiya et al. are based on a machine translation of the reference included with this action.
Regarding claims 1-7:
Tsuchiya et al. teaches a positive electrode, negative electrode, and a negative electrode material for lithium-ion secondary batteries comprising a silicon-containing particles A and particles B and C containing carbonaceous material (0006). The silicon particle A corresponds to the claimed second silicon and particle C corresponds to the claimed carbon material. The silicon particle A has average circularity (Zs2) of 0.8 to 1.0 (0064) and average particle diameter of 1-25 microns (0059). Carbon particle C includes graphite (0079) and has average circularity (Zc) of 0.85 to 1.0 (0093) and average particle diameter of 1-40 microns (0092). The ratio of the average circularity of carbon particle C to silicon particle A is 1/(0.89 to 1.06) (0011) or 0.95 to 1.12 which includes where Zs2 < Zc.
However, Tsuchiya et al. does not teach a first silicon-containing material, an average particle diameter of the first silicon-containing material, an average circularity Zs1 of the first silicon-containing material, wherein the average circularity Zs1 is 0.6 or less, the average particle diameter of the first silicon-containing material is in a range of 1 to 15 µm, and wherein a ratio Zs1/Zs2 of the average circularity Zsl to the average circularity Zs2 is in a range of 0.4 to 0.9.
Kawase et al. teaches an anode material for a secondary battery (0021) that includes silicone-containing material (0014), corresponding to claimed first silicon material, having average circularity (Zs1) of 0.75 or less to reduce the number of cracks (0016). The silicone-containing material has an average particle diameter of 0.3-20 microns to prevent cracks and reduce decomposition of the particles (0019).
In light of the motivation for using the silicone-containing material disclosed by Kawase et al. as set forth above, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to use the silicone-containing material in the negative electrode material of Tsuchiya et al. in order to prevent cracks and reduce decomposition of the particles.
Given that Tsuchiya et al. disclose the second silicon material has an average particle diameter of 1-25 microns and the carbon material has average particle size of 1-40 microns and given that Kawase et al. disclose the first silicon material has an average particle size of 0.3-20 microns, it is clear that the average particle diameter of each of the first silicon material and second silicon material is less than the average particle diameter of the carbon material. Further, given that Tsuchiya et al. discloses that the average circularity of the second silicon material (Zs2) is 0.8 to 1.0 and the average circularity of the carbon material (Zc) is 0.85 to 1.0 and Kawase et al. disclose the average circularity of the first silicon material (Zs1) is 0.75 or less, Zs1<Zc, Zs1<Zs2 and it is calculated that the ratio of Zs1/Zs2 is less than 0.75 (0.75/1.0) while the ratio of Zs1/Zc is less than 0.75 (0.75/1).
Claims 8-11 are rejected under 35 U.S.C. 103 as being unpatentable over Tsuchiya et al. (WO 2019220576 A1) in view of Kawase et al. (US 20070105017 A1) and further in view of Pang et al. (US 20200058924 A1).
Regarding claims 8-11:
Tsuchiya et al. in view of Kawase et al. teaches a negative electrode material as set forth above.
However, Tsuchiya et al. in view of Kawase et al. does not teach the silicon-containing material is composite particles that include an ion-conducting phase and silicon phases dispersed in the ion-conducting phase, wherein the ion-conducting phase is at least one selected from the group consisting of a silicate phase, a carbon phase, and a silicon oxide phase, wherein the first silicon-containing material and the second silicon-containing material are each independently a first composite material that includes a silicate phase and first silicon phases dispersed in the silicate phase, or a second composite material that includes a carbon phase and second silicon phases dispersed in the carbon phase, and wherein the silicate phase contains at least one selected from the group consisting of alkali metal elements and Group 2 elements.
Pang et al. teaches an anode material for secondary batteries (0001) that includes a Si—O—C—Li composite, wherein the composite comprises nano-silicon, a silicon oxide, a lithium-containing compound including lithium silicate (0024), i.e. silicate phase, and a carbon coating. The composite has such a structure that nano-silicon is dispersed in the lithium-containing compound to form fusion particles, and the fusion particles are dispersed in a silicon oxide served as a matrix in a sea-island form to form composite particles, with the carbon coating coated on the surface of the composite particles (0073).
Pang et al. also teaches the composite has a stable structure, which can avoid the failure of active ingredients due to the infiltration of components such as air into the interior of the particles, and the structure and properties of the composite will not deteriorate during long-term storage (0074).
In light of the motivation for using the Si—O—C—Li composite disclosed by Pang et al. as set forth above, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to use the Si—O—C—Li composite in the negative electrode material of Tsuchiya et al. in order to avoid the failure of active ingredients and deterioration during long-term storage.
Claims 12-13 are rejected under 35 U.S.C. 103 as being unpatentable over Tsuchiya et al. (WO 2019220576 A1) in view of Kawase et al. (US 20070105017 A1) and further in view of Uchiyama et al. (WO 2019130787 A1). It is noted that the disclosures of Uchiyama et al. are based on a machine translation of the reference included with this action.
Regarding claims 12-13:
Tsuchiya et al. in view of Kawase et al. teaches a negative electrode material as set forth above.
However, Tsuchiya et al. in view of Kawase et al. does not teach the silicate phase contains at least one selected from the group consisting of B, Al, Zr, Nb, Ta, V, lanthanoids, Y, Ti, P, and W, wherein the first composite material contains composite particles that include the silicate phase and the first silicon phases, and a coating layer covering at least a portion of surfaces of the composite particles.
Uchiyama et al. teaches a negative electrode active material including a lithium silicate phase and silicon particles dispersed within the lithium silicate phase, wherein the silicate phase contains at least one selected from the group consisting of B, Al, Zr, Nb, Ta, La, V, Y, Ti, P, and W can be used. Specifically, for example, material B has a low melting point, which increases its fluidity during sintering, improves its sinterability, and increases its hardness. Al, Zr, Nb, Ta, and La have the effect of increasing hardness while maintaining ionic conductivity (0010, 0012).
In light of the motivation for using at least one of B, Al, Zr, Nb, Ta, La, V, Y, Ti, P, and W in the lithium silicate phase disclosed by Uchiyama et al. as set forth above, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to use at least one of Al, Zr, Nb, Ta, La, V, Y, Ti, P, and W in the lithium silicate phase in the negative electrode material of Tsuchiya et al. in order to increase fluidity during sintering, improve sinterability, and increase hardness while maintaining ionic conductivity.
Claims 14-15 are rejected under 35 U.S.C. 103 as being unpatentable over Tsuchiya et al. (WO 2019220576 A1) in view of Kawase et al. (US 20070105017 A1) and further in view of Xing et al. (JP 2012124114 A).
Tsuchiya et al. in view of Kawase et al. teaches a negative electrode material as set forth above.
Further, Tsuchiya et al. teaches the proportion of particle C in the negative electrode material for lithium-ion secondary batteries is preferably 1% to 99% by mass, i.e. “c” in the equations below. The mass-based content ratio of particle A, i.e. second silicon-containing, to particle B, is preferably 0.05 to 20 ([0098]). It is therefore calculated that the mass percent of the second silicon-containing particle ranges from 0.048% to 94.286% as shown by the mathematical steps below, where “a” is the mass percent of particle A, i.e. second silicon material, “b” is the mass percent of particle B, “c” is the mass percent of particle C, and Rab is the mass-based content ratio of particle A to particle B.
100
%
=
a
+
b
+
c
R
a
b
=
a
b
b
=
a
R
a
b
a
+
b
=
100
%
-
c
a
+
a
R
a
b
=
100
%
-
c
a
1
+
1
R
a
b
=
100
%
-
c
a
R
a
b
+
1
R
a
b
=
100
%
-
c
a
=
100
%
-
c
R
a
b
+
1
R
a
b
a
min
100
%
-
99
%
0.05
0.05
+
1
=
0.048
%
a
m
ax
100
%
-
1
%
20
20
+
1
=
94.286
%
However, Tsuchiya et al. in view of Kawase et al. does not teach in the negative electrode, the amount of first silicon material and therefore does not teach the amount of silicon-containing material.
Xing et al. disclose negative electrode for lithium-ion secondary battery comprising negative electrode material comprising carbonaceous particles A, carbonaceous particles B, and second particles comprising silicone atoms (0010, 0052). The second particles are present in an amount of 0.5-20 wt% to improve the battery capacity and cycle characteristics (0056).
In light of the motivation for using the second particles present in an amount of 0.5-20 wt% disclosed by Xing et al. as set forth above, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to use first silicon material present in an amount of 0.5-20 wt% in the negative electrode material of Tsuchiya et al. in order to improve the battery capacity and cycle characteristics.
Given that Tsuchiya et al. disclose using 0.048-94.286% second silicon material and Xing et al. disclose using 0.5-20 wt.% first silicone material, it is clear that the amount of silicon-containing material (first silicon and second silicon) in Tsuchiya et al. in view of Kawase et al. and further in view of Xing et al. would overlap that presently claimed.
Claim 15 is rejected under 35 U.S.C. 103 as being unpatentable over Tsuchiya et al. (WO 2019220576 A1) in view of Kawase et al. (US 20070105017 A1) and further in view of Fukuoka et al. (JP 5500047 B2). It is noted that the disclosures of Fukuoka et al. are based on a machine translation of the reference included with this action.
Regarding claim 15:
Tsuchiya et al. in view of Kawase et al. teaches a negative electrode material as set forth above.
Further, Tsuchiya et al. teaches the proportion of particle C in the negative electrode material for lithium-ion secondary batteries is preferably 1% to 99% by mass, i.e. “c” in the equations below. The mass-based content ratio of particle A, i.e. second silicon-containing, to particle B, is preferably 0.05 to 20 ([0098]). It is therefore calculated that the mass percent of the second silicon-containing particle ranges from 0.048% to 94.286% as shown by the mathematical steps below, where “a” is the mass percent of particle A, i.e. second silicon material, “b” is the mass percent of particle B, “c” is the mass percent of particle C, and Rab is the mass-based content ratio of particle A to particle B.
100
%
=
a
+
b
+
c
R
a
b
=
a
b
b
=
a
R
a
b
a
+
b
=
100
%
-
c
a
+
a
R
a
b
=
100
%
-
c
a
1
+
1
R
a
b
=
100
%
-
c
a
R
a
b
+
1
R
a
b
=
100
%
-
c
a
=
100
%
-
c
R
a
b
+
1
R
a
b
a
min
100
%
-
99
%
0.05
0.05
+
1
=
0.048
%
a
m
ax
100
%
-
1
%
20
20
+
1
=
94.286
%
However, Tsuchiya et al. in view of Kawase et al. does not teach in the negative electrode, the mass of the first silicon-containing material is in a range of 0.2 to 5 times the mass of the second silicon-containing material.
Fukuoka et al. teaches a negative electrode material for a non-aqueous electrolyte secondary battery, comprising a mixture of silicon oxide particles (0011). In the particles, the ratio of carbon nanotubes, carbon nanofibers or carbon fibers to Si particles, i.e. first silicon-containing material, (100% by mass) is preferably 3 to 50% by mass, i.e. the mass percent of Si particles is 50 to 97%. When this ratio is less than 3% by mass, the force of entanglement of fibers is reduced, and when the negative electrode material is obtained, the cycle performance may be lowered. On the other hand, when the ratio exceeds 50% by mass, the bulk density is reduced, and there is a concern that the charge-discharge capacity per unit volume may be reduced when used as a negative electrode material (0021).
In light of the motivation for using the mass percent of Si particles is 50 to 97% disclosed by Fukuoka et al. as set forth above, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to use the mass percent of Si particles is 50 to 97% in the lithium silicate phase in the negative electrode material of Tsuchiya et al. in order to avoid lowered cycle performance and reduced charge-discharge capacity per unit volume.
It is therefore calculated that the mass percent of particle A taught by Tsuchiya et al. is 0.000491 to 1.886 times the mass percent of Si particles taught by Fukuoka et al. as shown below, meeting the claimed relational expression.
0.0476
%
=
97
%
x
m
i
n
x
m
i
n
=
0.000491
94.2857
%
=
50
%
x
m
a
x
x
m
a
x
=
1.886
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to MADISON E. BROWN whose telephone number is (571)775-5984. The examiner can normally be reached M-Th 8am-6pm.
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If attempts to reach the examiner by telephone are unsuccessful, the examiner’s supervisor, Callie Shosho can be reached at 5712721123. The fax phone number for the organization where this application or proceeding is assigned is 571-273-8300.
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/MADISON ELIZABETH BROWN/Examiner, Art Unit 1787
/CALLIE E SHOSHO/Supervisory Patent Examiner, Art Unit 1787
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