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 .
Status of Claims
Claims 1, 5, 15, 19 are amended.
Claims 6 and 20 are cancelled.
Claims 1-5, 7-19 are pending.
Response to Amendment
Amendments filed on 7/16/2026 have been entered.
103 rejection from previous office action have been withdrawn in view of the amendments and arguments.
Claim Rejections - 35 USC § 103
In the event the determination of the status of the application as subject to AIA 35 U.S.C. 102 and 103 (or as subject to pre-AIA 35 U.S.C. 102 and 103) is incorrect, any correction of the statutory basis (i.e., changing from AIA to pre-AIA ) for the rejection will not be considered a new ground of rejection if the prior art relied upon, and the rationale supporting the rejection, would be the same under either status.
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.
Claims 1-5, 7-19 are rejected under 35 U.S.C. 103 as being unpatentable over Li et al (WO 2022077370 A1; machine translation), in view of Yao et al (US 20220149340 A1), in view of Matsuno et al (US 20250206976 A1; effective filing date: 03/31/2022) and in view of Konishi et al (US 20130164618 A1) further in view of Adar, F. (2022). Use of Raman Spectroscopy to Qualify Carbon Materials. Spectroscopy, 37(6), 11–15. https://doi.org/10.56530/spectroscopy.wx3481u2
Regarding Claim 1, and Claim 15,
Li teaches an electrochemical apparatus (Paragraph 0006; secondary battery), comprising an electrode assembly; wherein the electrode assembly comprises a positive electrode plate (Paragraph 0042), a negative electrode plate (Paragraph 0006), and a separator disposed between the positive electrode plate and the negative electrode plate (Paragraph 0069); the negative electrode plate comprises a negative electrode current collector, a first active material layer (Paragraph 0006; second negative electrode layer) and a second active material layer (Paragraph 0006; first negative electrode layer); the first active material layer and the second active material layer being disposed on at least one surface of the negative electrode current collector, wherein the first active material layer being located between the negative electrode current collector and the second active material layer (Paragraph 0006; the second negative electrode film being located between the negative current collector and the first negative electrode film layer).
The first active material layer comprises a first active substance (Paragraph 0023), and the second active material layer comprises a second active substance (Paragraph 0006), wherein a compacted density of the first active material layer is 1.7 to 1.85 g/cm3 (Paragraph 0035), and the compacted density of the second active material layer is 1.55 to 1.7 g/cm3 (Paragraph 0018). Hence, compacted density of first layer is greater than a compacted density of the second active material layer.
Li teaches that the particle size specific surface area of the negative electrode active material is used to characterize the degree to which the morphology of the active material deviates from sphericity. Li does not explicitly teach about the sphericity of the first and second active materials, and that the sphericity of the first active substance is smaller than a sphericity of the second active substance.
However, Yao teaches an anode comprising a first active material layer and a second active material layer such that the first layer is adjacent to the current collector (Paragraph 0054), and the second layer is located adjacent to the first layer. Yao teaches that the top layer has higher sphericity (Paragraph 0061) which is the second active material layer (shown in annotated figure 3 below). Yao teaches that having high top layer sphericity provide reduced electrode impedance, reduced electrode tortuosity, improved liquid-phase mass transport, and electrode rate capability (Paragraph 0142). Li also teaches that the motivation behind the multiple electrode layers is to improve the intercalation and deintercalation ion channels, reduce the charge exchange impedance, and improve the charging performance, and cycle performance of the battery (Paragraph 0090). Hence, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the claimed invention to use the sphericity of active material layers as shown in Yao, in combination with the material layers of Li in order to improve the electrode rate capabilities.
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Li teaches the use of a separator that allows ions to pass through (Paragraph 0069), and does not impose any particular restriction on the type of separator membrane; any known porous separator membrane with good chemical and mechanical stability can be selected (Paragraph 0176). Li also teaches the use of a multi-composite film as separator (Paragraph 0176; first coating layer). Li does not specifically teach that the first coating layer is disposed on at least one surface of the porous substrate layer facing the second active material layer, and an adhesion between the separator and the negative electrode plate is greater than or equal to 2 N/m and less than or equal to 20 N/m.
However, Matsuno teaches a separator for a secondary battery that has a functional layer (Paragraph 0027; akin to a first coating layer). Matsuno also teaches about measuring peel strength which is a measure of the adhesiveness between a separator and a negative electrode (Paragraph 0158). A peel strength of 6 N/m or more, and of not less than 2 N/m and less than 6 N/m are classified (Paragraph 0158). Table 1 in Matsuno shows that the separators with the functional layer provide adhesion/peel strength in the above defined categories of N/m. Hence, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the claimed invention to use the separator and functional layer from Matsuno in the electrode assembly of Li in order to improve adhesiveness between battery members, and reduce internal resistance of the secondary battery (Paragraph 0022).
Li teaches that the first active substance and the second active substance which are contained within the first and second active material layers are carbon based materials such as soft carbon, hard carbon (Paragraph 0041).
Li teaches the use of carbon based materials in both the first active substance and the second active substance (Paragraph 0041); but does not specifically teach that the first active substance has a peak intensity ratio of peak d to peak g in the Raman test is Id1/Ig1, wherein 0 < Id1/Ig1< 0.2; and the second active substance has a peak intensity ratio of peak d to peak g in the Raman test is Id2/Ig2, wherein 0.2 < Id2/Ig2≤ 1; wherein peak d has a wavelength range of 1270 cm-1 to 1330 cm-1 in the Raman spectrum, and peak G has a wavelength range of 1550 cm-1 to 1610 cm-1 in the Raman spectrum. The instant specification states that values of Id1/Ig1 and Id2/Ig2 can be controlled by selecting different types of negative electrode active materials. Li teaches the use of an amorphous carbon coating layer on the graphite particles in the second active material as defined in Claim 1 (Paragraph 0021). The instant specification also states that the peak intensity ratio is related to the coating degree of the active substance (based on mass of amorphous carbon coating). Li teaches in Paragraph 0022 that the second active material layer (defined in Claim 1) has more graphite than the first active material layer (defined in Claim 1) in order to effectively improve the battery’s fast charging capability. Based on the above, Li teaches controlling or adjusting the types of negative electrode active materials used in the first and second layer, but Li does not explicitly specify the relationship between the materials and the Raman test peak intensity ratio.
However, Konishi teaches different negative electrode active material classified as first active material and second active material (Paragraph 0028). The first active material is a carbon material having a D/G ratio of 0.15 or less, where G represents the peak intensity observed in a Raman spectrum from 1578 to 1592 cm-1 and D represents the peak intensity observed in a Raman spectrum from 1349 to 1353 cm-1 of Raman spectroscopy, and corresponds to a high crystalline graphite material. Examples of the high crystalline graphite material include natural graphite such as scale-shaped or spherical graphite; artificial graphite (Paragraph 0030). The lower limit of the D/G ratio in Konishi is not particularly limited, and is generally about 0.05 (Paragraph 0029).
The D band wavenumber in Konishi is different than the claimed 1270-1330 cm-1, however, Adar teaches that in the field of using Raman spectroscopy to qualify carbon materials the wavenumber (wavelength) of the D band is highly dependent on the excitation energy. Adar states that by exciting graphite with varying laser wavelengths the D band was observed to occur near 1390 cm-1 when excited with UV, and 1270 cm-1 when excited with NIR (Page 11). The instant specification and Konishi are silent with respect to the excitation energy used for Raman spectroscopy. Adar states that the origins of the Raman spectra such as excitation energy impact the empirically derived physical and chemical information of manufactured materials. For empirical correlations to be effective, measurements must be made in a consistent manner (as stated in Adar Page 12). Hence, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the claimed invention that the wavenumber of Konishi and the instant specification are within the possibility of variance based on the teaching in Adar. The D/G ratio of the first active material in Konishi overlaps with the claimed range of 0-0.2. Per MPEP 2144.05, where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists.
The second active material includes at least one of the first carbon material having the D/G ratio of 0.2 to 2.0 and the second carbon material having the D/G ratio of 1.0 to 2.0 (Paragraph 0032). The first carbon material may be, e.g., a carbon material obtained by coating the natural graphite or the artificial graphite with an amorphous layer of petroleum pitch, coal pitch, or the like (i.e., pitch-coated graphite) or a carbon material. The thickness of the coating layer is not particularly limited, and may be appropriately adjusted so that the D/G ratio falls in the range of 0.2 to 2.0 (paragraph 0033). Konishi teaches choosing negative electrode active material that matches the D/G ratio for peak intensity in a Raman spectrum in order to ensure conductivity of the electrode, improve charge-discharge load characteristics (Paragraph 0018, 0019). Hence, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the claimed invention that the materials selected in Li would be capable of meeting the peak intensity ratio as shown in Konishi to improve battery characteristics. Also, based on the teaching of Adar the D band wavenumber as claimed and in Konishi are within the possibility of variance based on measurement technique utilized.
Li also teaches the use of the secondary battery/electrochemical apparatus in a device containing the secondary battery such as electronic devices and electric vehicles (Paragraph 0002). These electronic devices are akin to the electronic apparatus of Claim 15.
Regarding Claim 2, Claim 3, Claim 16, Claim 17,
Li does not explicitly teach the mass % of first active material layer is 10% to 90%, or 20% to 80% based on a total mass of the first active material layer and the second active material layer.
However, Li does teach that the thickness ratio of the first active layer to the second active layer as defined in rejection of Claim 1 is 0.7:1 to 2.3:1 (Paragraph 0040). Li also teaches the density of the first and second active layers (Paragraph 0017, 0034). Upon using the relationship between the thickness, and the densities as taught in Li, the mass ratio between the two layers is determined. Based on that mass ratio it is found that the mass percentage of the first active material layer is between 10 to 90%, and between 20 to 80%. Hence, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the claimed invention to use a suitable thickness value as shown in Li along with a suitable density in Li in order to improve the fast charging capability or energy density of the battery (Paragraph 0040).
Regarding Claim 4, and Claim 18,
Li teaches first active material layer and second active material layer as defined in rejection of Claim 1. Li also teaches that the second active material has a powder compaction density of 1.55 to 1.7 g/cm3 (Paragraph 0018). This range lies within the claimed range of compacted density D2 of the second active material layer, wherein 1.5 g/cm3≤ D2 ≤ 1.7 g/cm3 . Li also teaches that the first active material has a powder compacted density of 1.7 to 1.85 g/cm3. This range lies within the claimed range of compacted density D1 of the first active material layer, wherein 1.7 g/cm3< D1 ≤ 1.9 g/cm3.
Li teaches that the particle size specific surface area of the negative electrode active material is used to characterize the degree to which the morphology of the active material deviates from sphericity. The instant specification also states that sphericity is a parameter that characterizes the morphology of the particles. Hence, sphericity is a result effective variable of the specific surface area (SSA) of the active material, and sphericity has an inverse relationship with SSA. Li shows that the SSA of the first active material is 1 to 2 m2/g, and the second active material is 0.8 to 1.3 m2/g. This means that the sphericity of the second active material is less than the first active material. Li does not teach that the sphericity of the first active substance is S1, wherein 0.7 ≤ S1 ≤ 0.8; and the sphericity of the second active substance is S2, wherein 0.8 < S2 ≤ 0.9.
However, Yao teaches that the second active layer (top layer as taught in Yao) has a sphericity of greater than 0.8 (Paragraph 0063), and the first active layer (bottom layer as taught in Yao) has a sphericity less than the top layer (Paragraph 0065). Sphericity less than top layer includes a value within the claimed range of 0.7 ≤ S1 ≤ 0.8. Hence, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the claimed invention to use materials with sphericity as shown in Yao in order to improve the intercalation and deintercalation ion channels, reduce the charge exchange impedance, and improve the charging performance, and cycle performance of the battery (Paragraph 0090).
Regarding Claim 5, and Claim 19,
Li teaches that the first active substance and the second active substance which are contained within the first and second active material layers are one or more of silicon-based materials, tin-based materials; soft carbon, hard carbon (Paragraph 0041).
Regarding Claim 7,
Li teaches the use of a separator and does not impose any particular restriction on the type of separator membrane; any known porous separator membrane with good chemical and mechanical stability can be selected (Paragraph 0176). Li also teaches the use of a multi-composite film as separator (Paragraph 0176; first coating layer). Li does not specifically teach a second coating layer disposed between the porous substrate layer and the first coating layer, wherein the second coating layer comprises heat-resistant particles, and the heat-resistant particles comprise at least one selected from the group consisting of alumina, boehmite, barium sulfate, titanium dioxide, and magnesium hydroxide.
However, Matsuno teaches the use of heat resistant particles in a functional layer applied on the separator (Paragraph 0101). Some of the heat resistant particles used are aluminum oxide, boehmite (Paragraph 0103). Hence, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the claimed invention to have a coating layer on the separator comprising heat resistant material as shown in Matsuno in order to increase the heat resistance of a battery separator (Paragraph 0019).
Regarding Claim 8,
Li does not teach that a ratio of an area of the first coating layer to an area of the porous substrate layer is 0.10 to 0.85.
However, Matsuno teaches in an example that the coating area density of the functional layer (akin to the coating layer) is 0.2 g/m2 (Paragraph 0155). Matsuno also teaches that the functional layer is coated as stripes, dots or lattice shape (Paragraph 0127). This means that only a partial area of the porous substrate layer is coated with the functional layer and would fall within the claimed range of 0.1 to 0.85. Hence, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the claimed invention to have a ratio of an area of the first coating layer to an area of the porous substrate layer within 0.10 to 0.85 in order to reduce secondary battery resistance (Paragraph 0127).
Regarding Claim 9, and Claim 14,
Li does not teach that the first coating layer comprises polymer particles, wherein the polymer particles comprise polymers polymerized from at least one selected from the group consisting of the following monomers: vinylidene chloride, vinylidene fluoride, hexafluoropropylene, styrene, butadiene, acrylonitrile, acrylic acid, methyl acrylate, and butyl acrylate.
However, Matsuno teaches the formation of a functional layer, and the slurry used to make the same comprising polymers such as polyvinylidene fluoride, polymethyl methacrylate. Hence, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the claimed invention to use the polymer particles in Matsuno in order to increase the adhesiveness of the functional layer after immersion in electrolyte solution (Paragraph 0033).
Regarding Claim 10,
Li does not teach that a median particle size D50 of the polymer particles is 0.2 μm to 2 μm. However, Matsuno teaches particle diameter of the particulate polymer is preferably 0.25 μm or more, more preferably 0.30 μm or more, and even more preferably 0.40 μm or more, and is preferably 5.0 μm or less, more preferably 4.0 μm or less, even more preferably 3.0 μm or less. This overlaps with the claimed range. Hence, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the claimed invention to use the particle size in Matsuno in order to ensure that fine gaps are present in the functional layer, and adhesiveness of the functional layer can be improved (Paragraph 0035).
Regarding Claim 11,
Li does not teach that a swelling degree of the polymer particles is 20% to 100%.
However, Matsuno teaches that the proportional increase of thickness of the battery after cycling relative to before cycling is evaluated as a swelling property of the battery (Paragraph 0172). A smaller proportional increase of the thickness of the battery after cycling relative to before cycling indicates a better swelling property. The instant specification also states that when the swelling degree of the polymer particles is small, the electrochemical apparatus is less likely to swell in the charge and discharge cycles which is more conducive to improving the overall performance of the electrochemical apparatus. In Matsuno it is possible to adjust the increase in thickness of the battery by adjusting the functional layer composition as shown in Table 1. Hence, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the claimed invention to optimize the functional layer/coating slurry composition to reduce the change in thickness of the battery, and in turn lower the swelling degree such that it is within the claimed range of 20 to 100 %. One of ordinary skill in the art would be motivated to do so in order to improve the high temperature cycle characteristics of the battery (Paragraph 0172).
Regarding Claim 12,
Li does not teach that the polymer particles are core-shell structured microspheres, and each polymer particle comprises a shell and a core, wherein the shell comprises polymers polymerized from at least one selected from the group consisting of the following monomers: polyvinyl chloride, polyvinyl fluoride, hexafluoropropylene, polystyrene, polybutadiene, acrylonitrile, acrylic acid, methyl acrylate, and butyl acrylate; and the core comprises at least one selected from the group consisting of acrylate and acrylate polymer.
However, Matsuno teaches a particulate polymer used in the functional layer that has a core-shell structure (Paragraph 0016). Matsuno also teaches the use of polyvinyl acetate, polyvinylidene fluoride, polymethyl methacrylate, or the like without any specific limitations. Matsuno teaches the use of methyl acrylate, ethyl acrylate, n-propyl acrylate, isopropyl acrylate, n-butyl acrylate, t-butyl acrylate, isobutyl acrylate, n-pentyl acrylate etc for core material (Paragraph 0061, 0065). Matsuno teaches the use of monovinyl monomers and other types in Paragraph 0067, 0069. Hence, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the claimed invention to use the specified materials in the core-shell structure in order to improve the adhesiveness of the functional layer, and cycle characteristics of the battery (Paragraph 0016).
Regarding Claim 13,
Li does not teach that the electrochemical apparatus satisfies at least one selected from the group consisting of the following characteristics: (a) a ratio of an area of the first coating layer to an area of the porous substrate layer is 0.30 to 0.70; (b) a median particle size D50 of the polymer particles is 0.3 μm to 1 μm; (c) the shell comprises at least one selected from the group consisting of polyvinylidene fluoride, polyvinylidene chloride, styrene-butadiene copolymer, acrylonitrile, butadiene-acrylonitrile copolymer, acrylic acid, styrene-methyl methacrylate copolymer, and styrene-butyl methacrylate copolymer; and (d) the core comprises at least one selected from the group consisting of methyl acrylate and butyl acrylate.
However, Li teaches particle diameter of the particulate polymer is preferably 0.30 μm or more, and particularly preferably 1.4 μm or less. This range overlaps with the claimed range of 0.3 μm to 1 μm. Hence, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the claimed invention to use the particle diameter in the claimed range in order to ensure that fine gaps are present in the functional layer, and adhesiveness of the functional layer can be improved (Paragraph 0035).
References of Interest
Katogi et al (US 20250140786 A1)
Chen et al (US 20230307643 A1)
Response to Arguments
Applicant’s arguments, see Page 5, filed 7/16/2026, with respect to the rejection(s) of claim(s) 6 under 35USC 103 have been fully considered and are persuasive. Therefore, the rejection has been withdrawn. However, upon further consideration, a new ground(s) of rejection is made in view of previously cited prior art further in view of Adar. Examiner points to explanation in rejection above wherein Konishi and Adar provide support for the D/G ratios used in negative electrode carbon materials.
Applicant argues that Konishi does not teach or suggest the selectively positioned materials having different Raman characteristics. Examiner disagrees with this argument because the reference of Li is used in the rejection to support the position of the materials along with the type of materials utilized, and the reference of Konishi supports the characterization of that material using Raman spectroscopy. In response to applicant's arguments against the references individually, one cannot show nonobviousness by attacking references individually where the rejections are based on combinations of references. See In re Keller, 642 F.2d 413, 208 USPQ 871 (CCPA 1981); In re Merck & Co., 800 F.2d 1091, 231 USPQ 375 (Fed. Cir. 1986).
Applicant argues that there is no motivation to combine the teachings of Li, Yao, Matsuno, and Konishi. Examiner disagrees with this because the inventions of Li, Yao, Matsuno and Konishi are in the same field of art pertaining to negative electrode active material which comprise multiple active materials such that they result in a battery with higher energy density, fast charging performance and cycling performance, reduce electrode impedance, improved high temperature cycle characteristics. In response to applicant’s argument that there is no teaching, suggestion, or motivation to combine the references, the examiner recognizes that obviousness may be established by combining or modifying the teachings of the prior art to produce the claimed invention where there is some teaching, suggestion, or motivation to do so found either in the references themselves or in the knowledge generally available to one of ordinary skill in the art.
Conclusion
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/SUHANI JITENDRA PATEL/Examiner, Art Unit 1783
/MARIA V EWALD/Supervisory Patent Examiner, Art Unit 1783
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