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 1-8, and 12-13 are rejected under 35 U.S.C. 103 as being unpatentable over Fukuoka et al. (US 2014/0302395 A1), hereinafter “Fukuoka”, in view of Ku et al. (US 2015/0243969 A1), hereinafter, “Ku”.
Regarding claim 1, Fukuoka teaches a negative electrode material (corresponding to the claimed negative electrode active material) including silicon oxide (Fukuoka, [0048]), wherein the silicon oxide is a carbon-containing silicon oxide (corresponding to the claimed carbon-silicon-oxygen particles) (Fukuoka, [0013]) and the SiO is formed from Si and SiO2 at a molar ratio between 1 and 1.1 (which one skilled in the art recognizes could form SiOy where y is from 1 – 1.1 and thus corresponds to the claimed molar ratio of oxygen, 0.8 < y < 1.2) (Fukuoka, [0052]) and the carbon-containing silicon oxide contains a carbon content of 0.5 to 30 % (Fukuoka, [0013]).
Fukuoka does not teach an aluminum oxide layer on the surface of the carbon-containing silicon oxide material, nor does Fukuoka expressly teach a molar quantity range, x.
However, the examiner converts Fukuoka’s % carbon content range to a molar quantity range based on 1 mole of material according to equation (1) below.
x
=
1
m
o
l
S
i
*
28.085
g
m
o
l
S
i
+
y
m
o
l
O
*
15.999
g
m
o
l
O
100
%
C
-
1
*
12.011
g
m
o
l
C
(1)
Based on equation (1), the carbon content range taught by Fukuoka corresponds to x in the range of ~0.0184 - ~1.630, which overlaps with the claimed x range. In the case where the claimed ranges “overlap or lie inside ranges disclosed by prior art” a prima facie case of obviousness exists. See MPEP §2144.05.
Further, Ku teaches an anode active material for lithium ion batteries (Ku, [0009]) including a core (Ku, [0012]) which may include a composite comprising silicon (Ku, [0048]), and a metal oxide-including coating layer (Ku, [0056]). The metal oxide is of the general formula MxOy wherein M may be aluminum, 0 < x < 5, and 0 < y < 20, allowing for MxOy to be Al2O3 (corresponding to the claimed aluminum oxide layer) (Ku, [0054]). The anode active material including the metal oxide-including coating layer on the surface of the core (corresponding to the claimed aluminum oxide layer located on a surface of the carbon-silicon-oxygen particles) may provide improved structural stability (Ku, [0056]). Thus, it would have been prima facie obvious to one of ordinary skill in the art before the effective filing date of the instant invention to add Ku’s metal oxide-including coating layer to the carbon-containing silicon oxide negative electrode active material of Fukuoka in order to improve its stability (Ku, [0056]).
Regarding claim 2, Fukuoka modified by Ku suggests the negative electrode active material of claim 1 having a carbon-containing silicon oxide material according to SiCxOy wherein y is between 1.0 and 1.1 inclusive, and the carbon content disclosed by Fukuoka is ~0.0184 ≤ x ≤ ~1.630 as calculated for 1 mole of SiCxOy by the examiner according to equation (1) (discussed regarding claim 1 above). Fukuoka’s y range overlaps at the endpoint with the claimed y range and Fukuoka’s x range (as calculated by the examiner) overlaps with the claimed x range. In the case where the claimed ranges “overlap or lie inside ranges disclosed by prior art” a prima facie case of obviousness exists. See MPEP §2144.05.
Regarding claim 3, Fukuoka modified by Ku suggests the negative electrode active material according to claim 1 including an aluminum oxide coating. Fukuoka does not teach a coating thickness.
However, Ku teaches a thickness of about 0.5 nm to about 8 nm (corresponding to the claimed aluminum oxide layer thickness of 0.5 nm to 10 nm) for the metal oxide-including coating layer (corresponding to the claimed aluminum oxide layer) discussed above. When the thickness of the metal oxide-including coating layer is within the range, the anode active material including the metal oxide-including coating layer may relieve a volumetric change of the core (corresponding to the claimed carbon-silicon-oxygen particles) during charge and discharge to maintain high capacity of the anode active material in the lithium battery (Ku, [0057]). Thus, it would have been prima facie obvious to one of ordinary skill in the art before the effective filing date of the instant invention to add Ku’s metal oxide-including coating layer thickness to the metal oxide-including coating layer suggested by Fukuoka modified by Ku in order to relieve volumetric changes of the core material during cycling and maintain high capacity of the battery (Ku, [0057]).
Regarding claim 4, Fukuoka nor Ku expressly teach a silicon content a.
However, the negative electrode material suggested by Fukuoka modified by Ku having Fukuoka’s carbon-containing silicon oxide and Ku’s metal oxide-including coating layer has a silicon content of a weight % based on a whole mass of the negative electrode material overlapping with the claimed range of 45 ≤ a ≤ 70. Fukuoka teaches SiO formed in the gas phase from a Si:SiO2 ratio of 1:1 – 1:1.1 (resulting in a silicon oxide range of SiO1 – SiO1.1) (Fukuoka, [0052]) and further having a carbon content between 0.5 % - 30 % (Fukuoka, [0036]). Ku teaches a metal oxide-including coating layer which may be Al2O3 (as discussed with regard to claim 1 above) and which may be in the range of ~0.5 - ~2 parts by weight based on 100 parts by weight of the total weight of the anode active material (corresponding to a range of ~0.5 % - ~2 %) (Ku, [0056]). Thus, the carbon-containing silicon oxide with an Al2O3 coating layer suggested by Fukuoka modified by Ku would have a maximum Si weight percent when y = 1.0 in SiOy, the carbon content is 0.5 %, and the Al2O3 layer is 0.5 %, or a minimum Si weight percent when y = 1.1 in SiOy, the carbon content is 30 % and the Al2O3 layer is 2 %, wherein the carbon content % is carbon % based on the whole mass of the carbon-containing silicon oxide alone and the Al-2O3 content % is Al2O3 % based on the carbon-containing silicon oxide and Al2O3 coating layer. The examiner calculates the maximum Si weight % and the minimum Si weight % both based on a whole mass of the carbon-containing silicon oxide and the Al2O3 layer, using equations (3), (4), and (5) below and for 1 mole of material.
M
c
o
r
e
=
x
m
o
l
C
*
12.011
g
m
o
l
C
+
y
m
o
l
O
*
15.999
g
m
o
l
O
+
1
m
o
l
S
i
*
28.085
g
m
o
l
S
i
(3)
M
c
o
a
t
i
n
g
=
M
c
o
r
e
100
w
e
i
g
h
t
%
A
l
2
O
3
-
1
(4)
w
e
i
g
h
t
%
S
i
=
1
m
o
l
S
i
*
28.085
g
m
o
l
S
i
M
c
o
r
e
+
M
c
o
t
a
i
n
g
*
100
(5)
Where Mcore is the whole mass of the carbon-containing silicon oxide material, x = 0.0184 for 0.5 % or x = 1.630 for 30 % carbon, y = 1.0 or y = 1.1 (as discussed with regard to claim 1 above), and Mcoating is the whole mass of the Al2O3 coating with weight % Al2O3 being 0.5 or 2. According to the above calculation, the % Si is ~63.07 % to ~42.17 %, which overlaps with the claimed a range. In the case where the claimed ranges “overlap or lie inside ranges disclosed by prior art” a prima facie case of obviousness exists. See MPEP §2144.05.
Regarding claim 5, Fukuoka nor Ku expressly teach a carbon content b.
However, in the negative electrode material suggested by Fukuoka modified by Ku including Fukuoka’s carbon-containing silicon oxide and Ku’s Al2O3 layer, a maximum carbon content would correspond to the material having y = 1.0 for SiOy, Al2O3 at 0.5 % of the whole negative electrode material, and the carbon content of the SiO material at 30 % of the carbon-containing silicon oxide; a minimum carbon content would correspond to y = 1.1 for SiOy, Al2O3 at 2 % of the whole negative electrode material, and a carbon content of 0.5 % of the carbon-containing silicon oxide. The percentage carbon values are calculated by the examiner according to equations (3) and (4) above as well as equation (6) below.
w
e
i
g
h
t
%
C
=
x
m
o
l
C
*
12.011
g
m
o
l
C
M
c
o
r
e
+
M
c
o
t
a
i
n
g
*
100
(6)
Where x is 0.0184 or 1.630 for 0.5 % carbon or 30 % carbon respectively (discussed above regarding claim 1), y is 1.0 or 1.1 for a maximum and minimum carbon content respectively, and % Al2O3 is 0.5 or 2 for a maximum and minimum carbon content respectively. Thus, the examiner calculates the maximum carbon content to be 29.85 % and the minimum carbon content to be ~0.490 %, which overlaps with the claimed b range of 0.9 – 11 % carbon inclusive. In the case where the claimed ranges “overlap or lie inside ranges disclosed by prior art” a prima facie case of obviousness exists. See MPEP §2144.05.
Regarding claim 6, Fukuoka nor Ku expressly teach an aluminum content c.
However, the negative electrode material of Fukuoka modified by Ku includes the carbon-containing silicon oxide material taught by Fukuoka and the Al2O3 coating layer suggested by Ku. Ku suggests an Al2O3 content range of ~0.5 – ~2 % of the entire anode active material, which converts to a % Al content based on a whole mass of the negative electrode material as calculated by the examiner according to equation (7) below.
%
a
l
u
m
i
n
u
m
=
2
*
26.982
g
m
o
l
A
l
101.961
g
m
o
l
A
l
2
O
3
*
z
%
A
l
2
O
3
Thus the % Al content is ~0.265 - ~1.059 % which overlaps with the claimed c % aluminum content of 0.04 ≤ c ≤ 1.0. In the case where the claimed ranges “overlap or lie inside ranges disclosed by prior art” a prima facie case of obviousness exists. See MPEP §2144.05.
Regarding claim 7, Fukuoka and Ku do not expressly teach a c/a ratio in the range 0.001 ≤ c/a ≤ 0.015 as claimed.
However, the negative electrode material suggested by Fukuoka modified by Ku includes silicon and aluminum wherein the examiner calculates the silicon content to be ~42.17 – ~63.07 % and the aluminum content range to be ~0.265 - ~1.059 % as discussed regarding claims 4 and 6 above. Thus, the c/a range suggested by Fukuoka and Ku is in the range of ~0.0042 - ~0.025 as calculated by the examiner, which overlaps with the claimed c/a range of 0.001 – 0.015 inclusive. In the case where the claimed ranges “overlap or lie inside ranges disclosed by prior art” a prima facie case of obviousness exists. See MPEP §2144.05.
Regarding claim 8, Fukuoka and Ku do not explicitly teach a c/b ratio as instantly claimed.
However, Fukuoka modified by Ku suggest a negative electrode material including aluminum in a range of ~0.265 – ~1.059 % and carbon in a range of ~0.490 – 29.85 % (discussion regarding claims 5 and 6 above). Thus, the c/b ratio suggested by Fukuoka modified by Ku would be ~0.0089 - ~2.16, as calculated by the examiner, which overlaps with the claimed range of 0.008 – 0.30 inclusive. In the case where the claimed ranges “overlap or lie inside ranges disclosed by prior art” a prima facie case of obviousness exists. See MPEP §2144.05.
Regarding claim 12, Fukuoka further teaches a BET specific surface area of the carbon-containing silicon oxide of 1 to 20 m2/g (corresponding to the claimed specific surface area of the carbon-silicon-oxygen particles of 1 m2/g to 50 m2/g).
Regarding claim 13, Fukuoka does not teach a conductivity of the carbon-containing silicon oxide.
However, Fukuoka teaches a carbon-containing silicon oxide material of overlapping composition with the instantly claimed carbon-silicon-oxygen particles (as described regarding claim 1 above) and made by a substantially similar process as that disclosed by the instant specification.
Instant specification
Fukuoka
heating a raw material generating SiO gas [0048]
Heating a raw material generating a SiO gas [0019]
feeding in a carbon source, for example, acetylene, at 600 °C to 1100 °C [0048]
Supplying the generated SiO gas with a carbon-containing gas at a temperature of 500 to 1,100° C [0019]
Thus, a conductivity range of Fukuoka’s carbon-containing silicon oxide overlapping with the instantly claimed conductivity range would have naturally flowed from the teachings of Fukuoka. See MPEP 2112(IV).
Claim 9 is rejected under 35 U.S.C. 103 as being unpatentable over Fukuoka in view of Ku as applied to claim 1 above, and further in view of Wang et al. (CN 109449373 A), hereinafter “Wang”, wherein an English machine translation of Wang is used and cited herein.
Regarding claims 9, Fukuoka teaches an average particle diameter range of 0.2 – 20 µm (Fukuoka, [0041]) where the average particle diameter is represented by the weight average particle diameter obtained in a particle size distribution measurement (Fukuoka, [0043]) but does not expressly teach a Dv50 range.
However, Wang teaches a negative electrode tab with an anode active material (corresponding to the claimed negative electrode active material) which may include a silicon-based material which may be a silicon oxide compound (corresponding to the claimed carbon-silicon-oxygen particles) (Wang, [0026]), and wherein the Dv50 of the anode active material is from 4 to 16 µm, which overlaps with the claimed range. In the case where the claimed ranges “overlap or lie inside ranges disclosed by prior art” a prima facie case of obviousness exists. See MPEP §2144.05. When the Dv50 is in this range, the uniformity of the negative electrode tab may be higher, electrolyte side reactions are prevented, solid phase diffusion and accumulation of ions in the anode active material are not hindered, and the battery performance is improved (Wang, [0023]). Thus, it would have been prima facie obvious to one of ordinary skill in the art before the effective filing date of the instant invention to substitute Wang’s Dv50 range for Fukuoka’s average particle range in order to provide better negative electrode uniformity, prevent electrolyte side reactions, allow for good ionic diffusion, and improve battery performance (Wang, [0023]).
Claims 10-11 are rejected under 35 U.S.C. 103 as being unpatentable over Fukuoka in view of Ku as applied to claim 1 above, and further in view of Liao et al. (CN 111146414 A), hereinafter “Liao”, wherein an English language machine translation of Kim is used and cited herein.
Regarding claim 10, Fukuoka does not teach a Dn10/Dv50 range.
However, Liao teaches a negative electrode material including silicon-based particles which include a silicon composite matrix (corresponding to the claimed carbon-silicon-oxygen particles) and an oxide layer (corresponding to the claimed aluminum oxide layer) (Liao, [0032], [0042]; the lithium ion battery cycle performance, deformation resistance, and rate performance is better for silicon oxide prepared by satisfying ~0.3 ≤ Dn10/Dv50 ≤ ~0.6 (corresponding to the claimed 0.3 ≤ Dn10/Dv50 ≤ 0.6) than for a lithium ion battery with silicon oxide having a Dn10/Dv50 outside of the range (Liao, [0218]). Thus, it would have been prima facie obvious to one of ordinary skill in the art before the effective filing date of the instant invention to add Liao’s Dn10/Dv50 range to the carbon-based silicon oxide of Fukuoka in order to allow for a lithium ion battery with better cycle performance, deformation resistance, and rate performance (Liao, [0218]).
Regarding claim 11, Fukuoka does not teach the claimed range of I2/I1.
However, Liao teaches a negative electrode material including silicon-based particles which include a silicon composite matrix (corresponding to the claimed carbon-silicon-oxygen particles) (Liao, [0032], [0042]), wherein the negative electrode active material has a range of ~0 < I2/I1 ≤ ~1 (corresponding to the claimed 0 < I2/I1 ≤ 1) wherein for an X-ray diffraction pattern I2 is the highest intensity value from 2Θ ~28.0° to ~29.0° and I1 is the highest intensity value from 2Θ ~20.5° to ~21.5°. When I2/I1 is within the given range, the negative electrode active material has good cycle performance and a lithium ion battery prepared from it has good anti-swelling performance (Liao, [0107]). Thus, it would have been prima facie obvious to one of ordinary skill in the art before the effective filing date of the instant invention to add the I2/I1 range taught by Liao to Fukuoka’s carbon-containing silicon oxide to provide a negative electrode active material with good cycle performance and capable of providing a lithium ion battery it is used in with good anti-swelling performance (Liao, [0107]).
Claim 14 is rejected under 35 U.S.C. 103 as being unpatentable over Liao in view of Fukuoka.
Regarding claim 14, Liao teaches a negative electrode material including silicon-based particles (corresponding to the claimed negative electrode active material) (Liao, [0032]) including a silicon composite matrix (corresponding to the claimed carbon-silicon-oxygen particles) and an oxide layer which may be Al2O3 (corresponding to the claimed aluminum oxide layer) covering at least a portion of the silicon composite matrix (corresponding to the claimed aluminum oxide layer located on a surface of the carbon-silicon-oxygen particles) (Liao, [0042]-[0043]). Liao also discloses a method for preparing the silicon-based particles having an oxide coating on the surface (Liao, [0078]) including forming a mixed solution including the solid silicon oxide compound and an oxide precursor which may be aluminum isopropoxide (corresponding to the claimed aluminum source) then drying the mixed solution to obtain a powder (corresponding to the claimed deposition reaction to obtain a reaction product as one skilled in the art would recognize that drying a mixture of solid silicon oxide particles suspended in a solution containing aluminum isopropoxide would deposit the aluminum isopropoxide on the surface of the particles as the solvent was removed) (Liao, [0079]-[0080], [0087]). Next, the obtained powder is sintered (corresponding to the claimed roasting) to obtain silicon-based particles with an oxide layer on the surface (Liao, [0081]) wherein the sintering temperature may be 350 – 700 °C (corresponding to the claimed 300 to 800 °C roasting temperature) and the sintering time may be 1- 5 hours (corresponding to the claimed roasting time is 1 to 5 h) (Liao, [0089] – [0090]).
Liao does not teach the exact y range as claimed or carbon included in the silicon composite matrix.
However, Fukuoka teaches a carbon-containing silicon oxide (corresponding to the claimed carbon-silicon-oxygen particles) for a non-aqueous electrolyte secondary battery negative electrode material (corresponding to the claimed negative electrode active material) having a carbon content of 0.5 to 30 % (which overlaps with the claimed x range as discussed with regard to claim 1 above) (Fukuoka, [0014]) and which is formed from a precursor mixture of 1:1 to 1:1.1 Si:SiO2 (corresponding to the claimed y value between 0.8 – 1.2 as one skilled in the art would recognize that the precursor mixture stoichiometry could result in a silicon oxide material having the same stoichiometry) (Fukuoka, [0052]). In the case where the claimed ranges “overlap or lie inside ranges disclosed by prior art” a prima facie case of obviousness exists. See MPEP §2144.05. When such a carbon-containing silicon oxide is used, a battery having a high capacity and excellent cycle characteristics can be manufactured (Fukuoka, [0014]). Thus, it would have been prima facie obvious to one of ordinary skill in the art before the effective filing date of the instant invention to substitute the silicon composite matrix of Liao with the carbon-containing silicon oxide of Fukuoka in order to manufacture a battery having a high capacity and excellent cycle characteristics (Fukuoka, [0014]).
Claims 15-18 are rejected under 35 U.S.C. 103 as being unpatentable over Kim et al. (US 2022/0006121 A1), hereinafter “Kim”, in view of Fukuoka and Ku.
Regarding claim 15, Kim teaches a lithium secondary battery (corresponding to the claimed electrochemical apparatus) (Kim, [0013]) including a silicon-based negative electrode active material (Kim, [0018]) which may be SiOx (corresponding to the claimed carbon-silicon-oxygen particles) where x is 2 or less which overlaps with the claimed y range.
Kim does not teach the exact claimed y range or a carbon content having the claimed x range or an aluminum oxide coating.
However, Fukuoka teaches a carbon-containing silicon oxide (corresponding to the claimed carbon-silicon-oxygen particles) for a non-aqueous electrolyte secondary battery (corresponding to the claimed electrochemical device) having a carbon content of 0.5 to 30 % (which overlaps with the claimed x range as discussed with regard to claim 1) (Fukuoka, [0013]) and which is formed from codeposition of an SiO gas generated from a 1-1 to 1-1.1 stoichiometric mixture of Si-SiO2 solids (corresponding to the claimed y range as one skilled in the art would recognize that a precursor mixture of the given stoichiometry could result in a silicon oxide having the same stoichiometry) (Fukuoka, [0052]). In the case where the claimed ranges “overlap or lie inside ranges disclosed by prior art” a prima facie case of obviousness exists. See MPEP §2144.05. When Fukuoka’s carbon-containing silicon oxide is used as a negative electrode material, a battery having a high capacity and excellent cycle characteristics can be manufactured (Fukuoka, [0014]). Ku teaches an anode active material including a core which may include silicon and a metal oxide-including coating layer (corresponding to the claimed aluminum oxide layer) which may be Al2O3 (as discussed regarding claim 1 above) on the surface of the core (corresponding to the claimed aluminum oxide layer located on a surface of the carbon-silicon-oxygen particles) may provide improved structural stability (Ku, [0012], [0048], [0056]). Thus, it would have been prima facie obvious to one of ordinary skill in the art before the effective filing date of the instant invention to substitute Kim’s SiOx with Fukuoka’s carbon-containing silicon oxide in order to manufacture a high capacity battery having excellent cycle characteristics (Fukuoka, [0014]) and to add the Al2O3 coating layer suggested by Ku to the surface of the carbon-containing silicon oxide in order to provide improved structural stability.
Regarding claim 16, Kim does not teach a sheet resistance of the negative electrode.
However, Kim modified by Fukuoka and Ku suggests the electrochemical device according to claim 15 and Kim further teaches a negative electrode formed in a manner substantially the same as the instant disclosure.
Instant specification, [0078]
Kim, [0134]
The SiCxOy@Al2O3 material and graphite were mixed at a specified ratio to obtain mixed powder with a gram capacity of 850 mAh/g
negative electrode active material of composition SiO:graphite=30:70 weight ratio
The mixed powder, a conductive agent acetylene black, and PAA at a mass ratio of 95:1.2:3.8 were fully stirred and mixed to uniformity in solvent system of deionized water
A negative electrode active material, poly(acrylic acid sodium)-polyvinyl alcohol (PAA-PVA) as a binder, and carbon black, as a conductive agent were added in a weight ratio of 95:3.5:1.5 to water to prepare a negative electrode mixture slurry
the resulting mixture was applied on a Cu foil, followed by drying and cold pressing to obtain a negative electrode plate
A copper thin film, as a negative electrode collector, was coated with the negative electrode mixture slurry, dried, and then roll pressed
Kim also generally teaches that the silicon-based negative electrode active material and the carbon-based negative electrode active material may be included in a weight ratio of 5:95 to 50:50 wherein a negative electrode active material in the given range may secure room-temperature life characteristics and high-temperature life characteristics as well as excellent capacity characteristics. Thus, it would have been obvious to substitute the specific SiO:graphite ratio of 30:70 with any ratio between 5:95 and 50:50, providing a negative electrode with a sheet resistance range wherein said sheet resistance range overlapping with that of the instant invention would have naturally flowed from the teachings of Kim, Fukuoka, and Ku. In the case where the claimed ranges “overlap or lie inside ranges disclosed by prior art” a prima facie case of obviousness exists. See MPEP §2144.05.
Regarding claim 17, Kim does not teach the claimed c/b ratio.
However, the lithium secondary battery suggested by Kim modified by Fukuoka and Ku includes Fukuoka’s carbon-containing silicon oxide having a carbon content of 0.5 to 30 % (based on the whole mass of the carbon-containing silicon oxide) and Ku’s suggested Al2O3 coating layer at 0.5 to 2 % by mass of the entire negative electrode active material. Taken together, the carbon and metal oxide contents correspond to a c/b ratio range of ~0.0042 - ~0.025, which overlaps with the claimed c/b range. In the case where the claimed ranges “overlap or lie inside ranges disclosed by prior art” a prima facie case of obviousness exists. See MPEP §2144.05.
Regarding claim 18, Kim does not teach an aluminum oxide coating layer thickness.
However, Kim modified by Fukuoka and Ku suggests an Al2O3 coating layer and Ku further teaches a thickness of about 0.5 nm to about 8 nm (corresponding to the claimed aluminum oxide layer thickness of 0.5 nm to 10 nm) for the metal oxide-including coating layer (corresponding to the claimed aluminum oxide layer as discussed regarding claim 1 above). When the thickness of the metal oxide-including coating layer is within the range, the anode active material including the metal oxide-including coating layer may relieve a volumetric change of the core (corresponding to the claimed carbon-silicon-oxygen particles) during charge and discharge to maintain high capacity of the anode active material in the lithium battery (Ku, [0057]). Thus, it would have been prima facie obvious to one of ordinary skill in the art before the effective filing date of the instant invention to add the thickness range taught by Ku to the Al2O3 coating layer of the lithium secondary battery suggested by Kim modified by Fukuoka and Ku to help relieve volumetric changes of Fukuoka’s carbon-containing silicon oxide during battery cycling and to help maintain the high capacity of the anode material (Ku, [0057]).
Claim 19 is rejected under 35 U.S.C. 103 as being unpatentable over Kim, Fukuoka, and Ku as applied to claim 15 above, and further in view of Liao.
Rgearding claim 19, Kim does not teach an X-ray diffraction pattern having the claimed I2/I1 ratio.
However, Liao teaches a negative electrode material including silicon-based particles which include a silicon composite matrix (corresponding to the claimed carbon-silicon-oxygen particles) (Liao, [0032], [0042]), and the negative electrode active material has an X-ray diffraction pattern I2 is the highest intensity value from 2Θ ~28.0° to ~29.0° and I1 is the highest intensity value from 2Θ ~20.5° to ~21.5°. When ~0 < I2/I1 ≤ ~1 (corresponding to the claimed 0 < I2/I1 ≤ 1), the negative electrode active material has good cycle performance and a lithium ion battery prepared from it has good anti-swelling performance (Liao, [0107]). Thus, it would have been prima facie obvious to one of ordinary skill in the art before the effective filing date of the instant invention to add the I2/I1 range taught by Liao to the carbon-containing silicon oxide of the lithium secondary battery suggested by Kim modified by Fukuoka, and Ku, to provide a negative electrode active material with good cycle performance and capable of providing a lithium ion battery it is used in with good anti-swelling performance (Liao, [0107]).
Claim 20 is rejected under 35 U.S.C. 103 as being unpatentable over Liao in view of Fukuoka.
Regarding claim 20, Liao teaches an electronic device including an electrochemical device including a negative electrode which includes a negative electrode material (corresponding to the claimed negative electrode active material) (Liao, [0009] – [0011]). The negative electrode material includes silicon-based particles (Liao, [0032]) which include a silicon composite matrix (corresponding to the claimed carbon-silicon-oxygen particles) and an oxide layer (corresponding to the claimed aluminum oxide layer) which may include Al2O3 and which covers at least a portion of the silicon composite matrix (corresponding to the claimed aluminum oxide layer located on a surface of the carbon-silicon-oxygen particles) (Liao, [0041] – [0042]).
Liao does not teach the exact x range instantly claimed or a claimed carbon content in the SiOx particles.
However, Liao teaches the silicon composite matrix includes SiOx where ~0.6 ≤ x ≤ ~1.5, which overlaps with the claimed y range (Liao, [0048]). Furthermore, Fukuoka teaches a carbon-containing silicon oxide (corresponding to the claimed carbon-silicon-oxygen particles) for a negative electrode material (corresponding to the claimed negative electrode active material) and having a carbon content of 0.5 to 30 % (Fukuoka, [0013]), which overlaps with the claimed x range (see discussion regarding claim 1 above). In the case where the claimed ranges “overlap or lie inside ranges disclosed by prior art” a prima facie case of obviousness exists. See MPEP §2144.05. The carbon-containing silicon oxide is prepared by generating SiO gas from a precursor mixture of 1:1 to 1:1.1 mole ratio of Si:SiO2 which one skilled in the art would recognize could form SiOy with y from 1 to 1.1 (corresponding to the claimed y range). When such a carbon-containing silicon oxide is used for a negative electrode material, a non-aqueous electrolyte secondary battery of high capacity and with excellent cycle characteristics can be manufactured (Fukuoka, [0014]). Thus, it would have been prima facie obvious to one of ordinary skill in the art before the effective filing date of the instant invention to substitute Fukuoka’s carbon-containing silicon oxide for Liao’s SiOx to allow for the manufacturing of a high capacity battery with excellent cycling characteristics (Fukuoka, [0014]).
Double Patenting
The nonstatutory double patenting rejection is based on a judicially created doctrine grounded in public policy (a policy reflected in the statute) so as to prevent the unjustified or improper timewise extension of the “right to exclude” granted by a patent and to prevent possible harassment by multiple assignees. A nonstatutory double patenting rejection is appropriate where the conflicting claims are not identical, but at least one examined application claim is not patentably distinct from the reference claim(s) because the examined application claim is either anticipated by, or would have been obvious over, the reference claim(s). See, e.g., In re Berg, 140 F.3d 1428, 46 USPQ2d 1226 (Fed. Cir. 1998); In re Goodman, 11 F.3d 1046, 29 USPQ2d 2010 (Fed. Cir. 1993); In re Longi, 759 F.2d 887, 225 USPQ 645 (Fed. Cir. 1985); In re Van Ornum, 686 F.2d 937, 214 USPQ 761 (CCPA 1982); In re Vogel, 422 F.2d 438, 164 USPQ 619 (CCPA 1970); In re Thorington, 418 F.2d 528, 163 USPQ 644 (CCPA 1969).
A timely filed terminal disclaimer in compliance with 37 CFR 1.321(c) or 1.321(d) may be used to overcome an actual or provisional rejection based on nonstatutory double patenting provided the reference application or patent either is shown to be commonly owned with the examined application, or claims an invention made as a result of activities undertaken within the scope of a joint research agreement. See MPEP § 717.02 for applications subject to examination under the first inventor to file provisions of the AIA as explained in MPEP § 2159. See MPEP § 2146 et seq. for applications not subject to examination under the first inventor to file provisions of the AIA . A terminal disclaimer must be signed in compliance with 37 CFR 1.321(b).
The filing of a terminal disclaimer by itself is not a complete reply to a nonstatutory double patenting (NSDP) rejection. A complete reply requires that the terminal disclaimer be accompanied by a reply requesting reconsideration of the prior Office action. Even where the NSDP rejection is provisional the reply must be complete. See MPEP § 804, subsection I.B.1. For a reply to a non-final Office action, see 37 CFR 1.111(a). For a reply to final Office action, see 37 CFR 1.113(c). A request for reconsideration while not provided for in 37 CFR 1.113(c) may be filed after final for consideration. See MPEP §§ 706.07(e) and 714.13.
The USPTO Internet website contains terminal disclaimer forms which may be used. Please visit www.uspto.gov/patent/patents-forms. The actual filing date of the application in which the form is filed determines what form (e.g., PTO/SB/25, PTO/SB/26, PTO/AIA /25, or PTO/AIA /26) should be used. A web-based eTerminal Disclaimer may be filled out completely online using web-screens. An eTerminal Disclaimer that meets all requirements is auto-processed and approved immediately upon submission. For more information about eTerminal Disclaimers, refer to www.uspto.gov/patents/apply/applying-online/eterminal-disclaimer.
Claims 1-2, and 4-8 are rejected on the ground of nonstatutory double patenting as being unpatentable over claims 1 and 9 of U.S. Patent No. 12,418,029. Although the claims at issue are not identical, they are not patentably distinct from each other because claims 1 and 9 of the 029 patent each individually recite limitations overlapping with those of the instant claims 1-2, and 4-8.
Claim 3 is rejected on the ground of nonstatutory double patenting as being unpatentable over claims 1 and 9 of U.S. Patent No. 12,418,029 in view of Ku.
Regarding claim 3, claims 1 and 9 of the 029 patent each individually recite limitations overlapping in scope with those of the instant claim 3 but do not disclose a thickness range of the MeOy (which may be AlO1.5 as claimed by the 029 patent and which one skilled in the art recognizes is chemically equivalent to the claimed aluminum oxide).
However, Ku teaches a thickness range of about 0.5 nm to about 8 nm (corresponding to the claimed range of 0.5 nm to 10 nm) and that when the thickness is in this range, the anode active material (corresponding to the claimed carbon-silicon-oxygen particles) may relieve a volumetric change during charge and discharge to maintain the high capacity of the anode active material in the lithium battery (Ku, [0057]). Thus, it would have been prima facie obvious to one of ordinary skill in the art to add the thickness range of Ku to the anode material recited by claims 1 and 9 of the 029 patent to relieve volumetric changes during cycling and to preserve the capacity of the anode material (Ku, [0057]).
Claim 9 is rejected on the ground of nonstatutory double patenting as being unpatentable over claim 1 of U.S. Patent No. 12,418,029 in view of Wang.
Regarding claim 9, claim 1 of the 029 patent recites limitations overlapping in scope with those recited in the instant claim 9 but does not recite a Dv50 range.
However, Wang teaches an anode active material which may be a silicon oxide compound, having a Dv50 from 4 – 16 µm, which overlaps with the claimed Dv50 range (Wang, [0026]). In the case where the claimed ranges “overlap or lie inside ranges disclosed by prior art” a prima facie case of obviousness exists. See MPEP §2144.05. When the Dv50 is within the given range the uniformity of the negative electrode may be higher, electrolyte side reactions can be prevented, ion diffusion is not hindered and the battery performance is improved (Wang, [0023]). Thus, it would have been prima facie obvious to one of ordinary skill in the art before the effective filing date of the instant invention to add Wang’s Dv50 range to the anode material recited by claim 1 of the 029 patent to provide better negative electrode uniformity, prevent electrolyte side reactions, allow for good ion diffusion, and to allow for the construction of a battery with improved performance (Wang, [0023]).
Claim 10 is rejected on the ground of nonstatutory double patenting as being unpatentable over claim 1 of U.S. Patent No. 12,418,029 in view of Liao.
Regarding claim 10, claim 1 of the 029 patent recites limitations overlapping in scope with those recited in the instant claim 10 but does not recite the claimed Dn10/Dv50.
However, Liao teaches a negative electrode material including silicon-based particles which include a silicon composite matrix and an oxide layer (Liao, [0032], [0042]). The cycle performance, deformation resistance, and rate performance is better for a lithium ion battery having silicon oxide prepared by satisfying ~0.3 ≤ Dn10/Dv50 ≤ ~0.6 (corresponding to the claimed 0.3 ≤ Dn10/Dv50 ≤ 0.6) than prepared with a Dn10/Dv50 outside of the given range (Liao, [0218]). Thus, it would have been prima facie obvious to one of ordinary skill in the art before the effective filing date of the instant invention to add the Dn10/Dv50 range taught by Liao to Fukuoka’s carbon-based silicon oxide in order to allow for a lithium ion battery with better cycle performance, deformation resistance, and rate performance (Liao, [0218]).
Claim 11 is rejected on the ground of nonstatutory double patenting as being unpatentable over claims 8 and 14 of U.S. Patent No. 12,418,029. Although the claims at issue are not identical, they are not patentably distinct from each other because claims 8 and 14 of the 029 patent recite limitations overlapping with the instant claim 11 (see also claims 1 and 9 of the 029 patent).
Claim 12 is rejected on the ground of nonstatutory double patenting as being unpatentable over claim 4 of U.S. Patent No. 12,418,029. Although the claims at issue are not identical, they are not patentably distinct from each other because claim 4 of the 029 patent recites limitations overlapping in scope with those of the instant claim 12 (see also claim 1 of the 029 patent).
Claim 13 is rejected on the ground of nonstatutory double patenting as being unpatentable over claim 1 of U.S. Patent No. 12,418,029. Although the claims at issue are not identical, they are not patentably distinct from each other because claim 1 of the 029 patent recites limitations overlapping in scope with those of the instant claim 13 but does not recite a powder conductivity.
However, the matrix material recited by the 029 patent is made by a substantially similar process as the instantly claimed carbon-silicon-oxygen particles (see col. 12 ln. 64 – col. 13 ln. 10 of the 029 patent and [0048] of the instant specification). Thus, powder conductivity overlapping with the instantly claimed powder conductivity would have naturally flowed from the recitation of the 029 patent. See MPEP 2112(IV).
Claims 15 and 17 are rejected on the ground of nonstatutory double patenting as being unpatentable over claim 9 of U.S. Patent No. 12,418,029. Although the claims at issue are not identical, they are not patentably distinct from each other because claim 9 of the 029 patent recites limitations overlapping in scope with those of the instant claims 15 and 17.
Claim 16 is rejected on the ground of nonstatutory double patenting as being unpatentable over claim 9 of U.S. Patent No. 12,418,029. Although the claims at issue are not identical, they are not patentably distinct from each other because claim 1 of the 029 patent recites limitations overlapping in scope with those of the instant claim 16 but does not recite a sheet resistance.
However, the anode recited by the 029 patent and the instantly claimed negative electrode are made by a substantially similar process (see col. 13 ln. 54 – col. 14 ln. 8 of the 029 patent and [0078] of the instant specification). Thus, a sheet resistance overlapping with the instantly claimed sheet resistance would have naturally flowed from the claims of the 029 patent.
Claim 18 rejected on the ground of nonstatutory double patenting as being unpatentable over claim 9 of U.S. Patent No. 12,418,029 in view of Ku.
Regarding claim 18, claim 9 of the 029 patent recites all the limitations of claim 18 except an aluminum oxide layer thickness.
However, Ku teaches a metal oxide-containing coating layer with a thickness range of about 0.5 nm to about 8 nm (corresponding to the claimed range of 0.5 nm to 10 nm) and when the thickness is in this range, the anode active material (corresponding to the claimed carbon-silicon-oxygen particles) may relieve a volumetric change during charge and discharge to maintain the high capacity of the anode active material in the lithium battery (Ku, [0057]). Thus, it would have been prima facie obvious to one of ordinary skill in the art to add the thickness range of Ku to the anode material recited by claim 9 of the 029 patent to relieve volumetric changes during cycling and to preserve the capacity of the anode material (Ku, [0057]).
Claim 19 is rejected on the ground of nonstatutory double patenting as being unpatentable over claim 14 of U.S. Patent No. 12,418,029. Although the claims at issue are not identical, they are not patentably distinct from each other because claim 14 of the 029 patent recites limitations overlapping in scope with those of the instant claim 19 (see also claim 9 of the 029 patent).
Claim 20 is rejected on the ground of nonstatutory double patenting as being unpatentable over claim 15 of U.S. Patent No. 12,418,029. Although the claims at issue are not identical, they are not patentably distinct from each other because claim 15 of the 029 patent recites limitations overlapping in scope with those of the instant claim 20 (see also claim 9 of the 029 patent).
Conclusion
The prior art made of record and not relied upon is considered pertinent to applicant's disclosure. Rudolfovich et al. (US 2023/0246166 A1), Kim et al. (US 2024/0030416 A1), and Watanabe (US 2010/0009261 A1) teach the particles of claim 1. Bergner et al. (US 2022/0212950 A1), Du et al. (CN 112928269 A), Luo et al. (CN 111180692 A), Wu et al. (CN 112751011 A) teach the alumina coating and/or the method of claim 14. Sheng et al. (US 2021/0313567 A1) teaches the Dv50 range of claim 9.
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/SIMRAN S. SAUND/Examiner, Art Unit 1734
/JONATHAN JOHNSON/Supervisory Patent Examiner, Art Unit 1734