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 .
Election/Restrictions
Newly submitted claims 20 and 21 are directed to inventions that are independent or distinct from the invention originally claimed for the following reasons: Claim 20 is directed to Invention II (a method of preparing anode composition) and claim 21 is directed to Invention III (an anode) as set forth in the Restriction Requirement mailed on 7/27/2023. Said inventions were non-elected without traverse in Response to Restriction/Election received on 9/26/2023.
For further information regarding the restriction requirement, see the restriction requirement mailed on 7/27/2023.
Since applicant has received an action on the merits for the originally presented invention, this invention has been constructively elected by original presentation for prosecution on the merits. Accordingly, claims 20 and 21 are withdrawn from consideration as being directed to a non-elected invention. See 37 CFR 1.142(b) and MPEP § 821.03.
To preserve a right to petition, the reply to this action must distinctly and specifically point out supposed errors in the restriction requirement. Otherwise, the election shall be treated as a final election without traverse. Traversal must be timely. Failure to timely traverse the requirement will result in the loss of right to petition under 37 CFR 1.144. If claims are subsequently added, applicant must indicate which of the subsequently added claims are readable upon the elected invention.
Should applicant traverse on the ground that the inventions are not patentably distinct, applicant should submit evidence or identify such evidence now of record showing the inventions to be obvious variants or clearly admit on the record that this is the case. In either instance, if the examiner finds one of the inventions unpatentable over the prior art, the evidence or admission may be used in a rejection under 35 U.S.C. 103 or pre-AIA 35 U.S.C. 103(a) of the other invention.
Response to Arguments
Applicant’s arguments with respect to claim(s) 1 and 6-22 have been considered but are moot because the new ground of rejection does not rely on any reference applied in the prior rejection of record for any teaching or matter specifically challenged in the argument.
The applicant asserts that none of the cited references disclose or suggest an anode composition as specified in claims 1 and 14, wherein a content of the organic acid is more than 0.7 wt% and 1.5 wt% or less, and wherein the organic acid includes maleic acid. This limitation is found to be obvious in over of Choi in view of Park, and further in view of Song, as presented herein.
Additionally, the applicant discusses the attached declaration of November 11, 2025, which asserts unexpected results. Here, the evidence presented in the declaration is not found to be persuasive, as detailed in the response to amendment presented below.
Additionally, in regards to the limitation “the viscosity change rate of the anode composition being 6% or less” the applicant asserts that Jiang does not recognize or disclose suppressing the decrease in viscosity of the anode composition by applying an organic acid such as maleic acid, but instead disclosing adjusting the viscosity of the slurry through adding water, and that therefore a rejection based on a combination including Jiang is inappropriate. This argument has been fully considered is not persuasive.
The combination of Choi and Jiang is not based on an application of techniques disclosed by Jiang, but rather based on the teachings of Jiang identifying a rate of viscosity change as a result-effective-variable, and thereby making obvious the minimization of said variable in the context of the modified invention of Choi.
Jiang discloses that when the anode slurry undergoes precipitation the stability of the anode slurry decreases (Paragraph 0039, “thereby alleviating the particle connection, gelation and precipitation caused by the hydrolysis of the silicate in the material to some extent, and further significantly improving the stability of the lithiated silicon-oxygen material during aqueous processing.”) further showing that increased precipitation correlates with gas production within the anode slurry in their table (Paragraph 0119, “The following table shows the composition and stability (precipitation, gelation and gas production rate) of the anode active material according to the comparative examples of the prior art and the embodiments of the present application.”). Accordingly, the viscosity change is identified by Jiang as a result-effective variable, where it would be obvious to one ordinarily skilled in the art to optimize in the direction of reducing said viscosity change rate.
Additionally, the applicant asserts that the specific selection of maleic acid and the resulting viscosity stabilizing mechanism of the present application cannot be derived from a combination of Jiang and other cited references. This argument is not persuasive, as the claims do not claim maleic acid and a resulting viscosity stabilizing mechanism. Instead, maleic acid is claimed, and a viscosity change rate behavior is claimed. These two features are presented separately, and there is no requirement that there be a connection between the two in the claims. A combination of prior art which includes maleic acid, and includes a viscosity change rate behavior as claimed is sufficient to read upon said limitations, even if there is no connection between the two features in the combination of art.
Response to Amendment
The affidavit under 37 CFR 1.132 filed November 11, 2025 is insufficient to overcome the rejection of claims 1-14 based upon Choi in view of Park, Jiang, and Hori as set forth in the last Office action because:
The affidavit asserts that controlling organic acid content within the specified range of more than 0.7 wt% and 1.5 wt% or less is critical to achieving both chemical and electrochemical stability of the anode composition, thereby confirming the unexpected advantageous effects of the claimed invention. Here, the declarant indicates that in comparison to claim 1 which requires the claimed organic acid content, additional examples 1 and 2 present organic acid contents below the claimed range, and additional examples 3 and 4 present organic acid contents above the claimed range, and that the examples that fall within the claimed range demonstrate significantly improved stability of viscosity over time, minimized gas generation, and high initial capacity efficiency and superior capacity retention.
This evidence has been fully considered, but has not been found to be persuasive, based on the following rationale: The examples submitted as being indicative of unexpected results are not commensurate in scope with the claimed invention, as is detailed in MPEP section 716.02(d). The declarant has submitted that in their opinion, the combination of maleic acid with at least one organic acid selected from the group consisting of palmitic acid, tartaric acid, acetic acid, methacrylic acid, glycolic acid, oxalic acid, glutaric acid, and fumaric acid are expected to behave in a manner similar to the results of testing set forth in the examples in the specification conducted using maleic acid as an organic acid.
Specifically, examples 1, 3, 4, 5, and 6’s production are detailed in specification pages 21-23. Here, it indicates that these examples comprise 1 wt% of CNT as a flake-type conductive material, 2 wt% of SBR and 1.5 wt% of CMC as a thickener are used in addition to the mixture of organic acid and metal-doped silicon dioxide to form the anode composition, with the substrate for the anode being a copper material. Claims 1 and 14 do not specify the specific contents or use of CNT, SBR, and CMC, nor do they identify the substrate used for the anode. Where the declarant’s assertion of unexpected results is directed towards chemical and electrochemical stability, as well as viscosity change rate, the presence of materials which are introduced as being thickeners is likely to have an effect on the final result of a viscosity change rate, and the use of a conductive material and a specific anode substrate are likely to have effects on the chemical and electrochemical stability of the anode composition. For these reasons, the evidence presented as demonstrating unexpected results are not commensurate in scope with the claims.
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.
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.
This application currently names joint inventors. In considering patentability of the claims the examiner presumes that the subject matter of the various claims was commonly owned as of the effective filing date of the claimed invention(s) absent any evidence to the contrary. Applicant is advised of the obligation under 37 CFR 1.56 to point out the inventor and effective filing dates of each claim that was not commonly owned as of the effective filing date of the later invention in order for the examiner to consider the applicability of 35 U.S.C. 102(b)(2)(C) for any potential 35 U.S.C. 102(a)(2) prior art against the later invention.
Claim(s) 1 and 7-9 and 22 is/are rejected under 35 U.S.C. 103 as being unpatentable over Choi (US 20200168890 A1), in further view of Park (US 20170222221 A1) and Jiang (US 20200266428 A1) and further in view of Song (US 20160276672 A1).
Regarding Claim 1, Choi is an analogous art to the instant application, disclosing structure of an anode composition (Abstract, “A negative electrode active material”) for a lithium (Paragraph 0027, “intercalation of lithium ions may be smoothly performed”) secondary battery (Paragraph 0027, “Accordingly, the initial efficiency of the secondary battery may be improved.”). Additionally, Choi discloses structure which comprises a metal-doped silicon oxide (Paragraph 0049, “That is, the metal compound-doped primary particle further comprises a metal compound in the primary particle, wherein it denotes a particle in which the metal compound is doped into the primary particle which comprises the core comprising SiOx (0≤x<2);”) with the formula SiOx 0<x<2.
Additionally, Choi discloses structure wherein the anode composition includes a metal silicate area on a surface portion thereof. Here, Choi’s structure comprises a core comprising silicon dioxide (Paragraph 0023, “The core comprises SiOx (0≤x<2). The SiOx (0≤x<2) may be in the form in which silicon (Si) and SiO2 are included.”), and a metal doped silicon oxide (Paragraph 0053, “In an embodiment of the present invention, the metal compound may be included in the core of the primary particle. The metal compound may be formed by oxidation of a metal which may reduce the SiOx (0≤x<2), specifically, a metal having a reducing power capable of reducing silicon dioxide (SiO2 ) in the SiOx (0≤x<2) to silicon. The metal compound may comprise at least one of metal oxide and metal silicate.”; Paragraph 0049, “That is, the metal compound-doped primary particle further comprises a metal compound in the primary particle, wherein it denotes a particle in which the metal compound is doped into the primary particle which comprises the core comprising SiOx (0≤x<2)”; Paragraph 0055, “The metal silicate may comprise a silicate of at least one selected from the group consisting of Li, Mg, Al, Ca, and Ti. Specifically, the metal silicate may be at least one of MgSiO3, Mg2SiO4, Li2SiO3, Li4SiO4, Li2Si2O5, Al6SiO13, and Al4SiO8.”). Additionally, Choi discloses structure which comprises an intermediate layer covering the core (Paragraph 0050, “the intermediate layer which covers at least a portion of the surface of the core”), which means that the core has an outer surface. Therefore, where the core is the metal doped silicon dioxide, and the core comprises a surface, and where surface areas of the surface are areas on surface portions of the core, the core therefore comprises a metal silicate area on a surface portion of the core.
Additionally, Choi discloses structure wherein a metal doped to the metal-doped silicon oxide (Abstract, “wherein the first primary particle includes a core including SiOx, wherein 0≤x<2,”; Paragraph 0047, “The primary particle included in the secondary particle may be a metal compound-doped primary particle in which at least one of the core, the intermediate layer, and the carbon coating layer comprises a metal compound.”) includes at least one selected from the group consisting of lithium magnesium, calcium, and aluminum (Paragraph 0055, “The metal silicate may comprise a silicate of at least one selected from the group consisting of Li, Mg, Al, Ca, and Ti.”).
Additionally, in regards to the limitation which requires structure wherein the anode material comprises an organic acid including maleic acid, Choi is silent in regards to the inclusion of an acid component in their anode composition. Therefore, we look to Park, which is an analogous art to the instant application, disclosing an electrode composition for a lithium secondary battery which comprises lithium oxide (Abstract, “The present invention relates to a positive electrode active material for a lithium secondary battery,”). Here, Park discloses structure which includes a mixture of acids which act as a moisture scavenger, comprising a mixture of citric acid, tartaric acid, glycolic acid, and maleic acid (Paragraph 0148, “Specifically, the moisture scavenger may include citric acid, tartaric acid, glycolic acid, maleic acid or the like, and any one, or a mixture of two or more of these may be used.”). Additionally, Park discloses that the moisture scavenger acid is implemented in response to electrolyte decomposition and active material deterioration due to moisture inside the battery (Paragraph 0004, “This is due to a phenomenon occurring when an electrolyte is decomposed or an active material is deteriorated due to moisture inside the battery or other influences, or inner resistance of the battery increases.”).
Accordingly, though Park discloses their composition as being used in a positive electrode, a formulation that minimizes deterioration would be equally valuable in the negative electrode, as both the positive and negative electrode engage in ion intercalation and deintercalation, as disclosed by Park (Paragraph 0078, “lithium complex metal oxide as a compound capable of reversible intercalation and deintercalation of lithium (lithiated intercalation compound).”; Paragraph 0176, “The negative electrode active material may use a compound capable of reversible intercalation and deintercalation of lithium.”). Additionally, Park discloses similar structure in the positive and negative electrodes, where the negative electrode active material includes metal oxides capable of doping and dedoping lithium (Paragraph 0176, “Specific examples thereof may [include] metal oxides capable of doping and dedoping lithium such as SiOx (0<x<2), SnO2 , vanadium oxides and lithium vanadium oxides”), and the positive electrode active material includes a complex lithium metal oxide (Paragraph 0067, “A positive electrode active material for a lithium secondary battery according to an embodiment of the present invention includes a core including a first lithium complex metal oxide”) capable of ion transfer (Paragraph 0055, “and by the particles that form the shell having a crystal structure with orientation facilitating lithium ion intercalation and deintercalation”). Therefore, it would be obvious to one ordinarily skilled in the art to make use of the moisture scavenger of Park, employing it in the anode of Choi, thereby making obvious the limitation of the instant claim which requires that the anode composition comprise an organic acid including maleic acid.
Additionally, Park discloses a moisture scavenging acid mixture comprising a mixture of citric acid, tartaric acid, glycolic acid, and maleic acid (Paragraph 0148, “Specifically, the moisture scavenger may include citric acid, tartaric acid, glycolic acid, maleic acid or the like, and any one, or a mixture of two or more of these may be used.”), thereby reading upon the limitation of the instant Claim which requires structure wherein the organic acid further includes at least one selected from a group which includes citric acid, tartaric acid, and glycolic acid.
However, Choi is silent in regards to explicit structure such that the metal-doped silicon oxide particle satisfies the equation A/B ≤ 16.0.
Though Choi is silent in regards to the measurement of peak area of the metal silicate and silicon dioxide via a deconvolution of the Si2p XPS spectrum of the active material where A corresponds to metal silicate peak area and B corresponds to silicon dioxide peak area such that A/B ≤ 16.0, where XPS analysis depicts the presence of specific electrons in the examined specimen, and where the Si2p examines both metal silicate and silicon dioxide silicon particles, Choi discloses the that their structure comprises a metal silicate (Paragraph 0055, “The metal silicate may comprise a silicate of at least one selected from the group consisting of Li, Mg, Al, Ca, and Ti. Specifically, the metal silicate may be at least one of MgSiO3, Mg2SiO4, Li2SiO3, Li4SiO4, Li2Si2O5, Al6SiO13, and Al4SiO8.”), which is a metal doped silicon oxide present alongside silicon dioxide that is not doped (Paragraph 0138, “which included both of the primary particle not doped with metal and the primary particle having a metal compound doped into at least one of the core…”).
Here, where Choi discloses metal silicates (Paragraph 0055, “The metal silicate may comprise a silicate of at least one selected from the group consisting of Li, Mg, Al, Ca, and Ti. Specifically, the metal silicate may be at least one of MgSiO3, Mg2SiO4, Li2SiO3, Li4SiO4, Li2Si2O5, Al6SiO13, and Al4SiO8.”) which comprises the same number of electrons in the 2p subshell as silicon dioxide, the formula of the instant limitation therefore represents a molar ratio of metal silicate to silicon dioxide, where the moles of metal silicate divided by the moles of silicon dioxide is less than or equal to 16.
Here, Choi discloses structure where the metal silicate is present within the core, where the core comprises doped and undoped silicon dioxide, at a weight ratio of undoped to doped particle ranges from 20:80 to 80:20 (Paragraph 0051, “In a case in which the secondary particle further comprises the metal compound-doped primary particle in addition to the primary particle, a weight ratio of the primary particle to the metal compound-doped primary particle may be in a range of 10:90 to 90:10, for example, 20:80 to 80:20”), and where the atomic weight of lithium is low, the weight ratio between silicon dioxide and lithium doped silicon dioxide is comparable to a molar ratio. Therefore, where the molar ratio that ranges from 80:20 to 20:80, the molar ratio of doped to undoped silicon dioxide ranges from 0.25 to 4 where the whole range falls within the scope of the limitation of the instant claim, thereby reading upon the limitation of the instant claim where A/B ≤ 16.0.
Assuming arguendo, that Choi does not disclose the claimed peak ratio, Choi discloses a structure which comprises a mixing ratio of lithium silicate powder to silicon dioxide powder which falls between 80:20 and 20:80, as discussed above, as well as further disclosing that the benefit of this ratio to be that it improves initial efficiency, capacity retention, and reduces an electrode thickness change rate (Paragraph 0051, “In a case in which the secondary particle comprises the primary particle and the metal compound-doped primary particle at the above weight ratio, advantages of each of the primary particle and the metal compound-doped primary particle may be appropriately harmonized to improve the initial efficiency while increasing the capacity retention and reduce an electrode thickness change rate.”), it would therefore be obvious to one ordinarily skilled in the art to select a molar mixing ratio which would produce an embodiment that possesses the peak ratio required by the instant claim, thereby making obvious a composition which reads upon the scope of the instant limitation, where A/B ≤ 16.0.
Here, where the instant claim requires that the ratio be 0.5 to 16, Choi further presents motivation to minimize the content of the silicon dioxide in the active material particle (Paragraph 0056, “SiO2 matrix may be reduced and the metal compound may be formed. Accordingly, since an amount of SiO2 , which acts as an initial irreversible phase, may be reduced, the initial efficiency of the battery may be improved”), so as to minimize the presence of an initial irreversible phase. Accordingly, this therefore makes obvious maximizing the content of the metal silicate component, where a metal silicate/silicon dioxide particle of Choi would have a molar ratio of 80:20, or an A/B value of 4, which thereby reads upon and makes obvious the limitation of the instant claim which requires structure where A/B is from 0.5 to 16.
Therefore, where the invention of Choi comprises silicon dioxide and metal silicates as discussed above, it would produce a peak area at 102 eV corresponding to the peak area of the metal silicate and a peak area at 104 eV corresponding to the peak area of silicon dioxide if exhibited to XPS analysis on the metal-doped silicon oxide particle.
Additionally, Choi discloses structure wherein their anode composition does not include a metal salt containing magnesium or aluminum (Paragraph 0013, “there is provided a negative electrode active material which is a secondary particle comprising primary particles, wherein the primary particle comprises a core comprising SiOx (0≤x<2); an intermediate layer which covers at least a portion of a surface of the core and comprises silicon nitride, silicon oxynitride, or a mixture thereof; and a carbon coating layer which covers at least a portion of the intermediate layer and comprises nitrogen-doped carbon.”).
Additionally, in regards to the limitation of the instant claim which requires structure wherein a viscosity change rate of the anode composition is 6% or less, where the viscosity change rate is determined by measuring the initial viscosity of the anode composition, measuring the viscosity of the anode composition after 7 days, and subtracting the anode composition after 7 days from the initial viscosity and dividing the result by the initial viscosity, modified Choi fails to disclose or make obvious said structure. Therefore, we look to Jiang, which discloses an anode active material which comprises a metal doped silicon oxide material (Abstract, “The present application relates to an anode active material and an anode, an electrochemical device and an electronic device using the same. Specifically, the present application provides an anode active material, including a lithiated silicon-oxygen material”). Here, Jiang discloses that their anode slurry is analyzed by a method in which their slurry is stored for 48 hours, with a final viscosity being measured and compared to an initial viscosity, with the difference in viscosity being used to determine the degree of precipitation within the anode slurry (Paragraph 0113, “The anode active material slurry was stored for 48 hours, and the final viscosity of the anode slurry was measured. The final viscosity was compared with the initial viscosity, and when the viscosity reduction was less than 1000 Pa*s, it was recorded as no precipitation; when the viscosity reduction was 1000-2000 Pa*s, it was recorded as slight precipitation; and when the viscosity reduction was greater than 2000 Pa*s, it was recorded as severe precipitation.”). Here, Jiang further discloses that when the anode slurry undergoes precipitation the stability of the anode slurry decreases (Paragraph 0039, “thereby alleviating the particle connection, gelation and precipitation caused by the hydrolysis of the silicate in the material to some extent, and further significantly improving the stability of the lithiated silicon-oxygen material during aqueous processing.”) further showing that increased precipitation correlates with gas production within the anode slurry in their table (Paragraph 0119, “The following table shows the composition and stability (precipitation, gelation and gas production rate) of the anode active material according to the comparative examples of the prior art and the embodiments of the present application.”). Accordingly, the viscosity change is identified by Jiang as a result-effective variable, where it would be obvious to one ordinarily skilled in the art to optimize in the direction of reducing said viscosity change rate.
Accordingly, where Jiang discloses that a change of viscosity results in precipitation, and that precipitation results in a decrease in stability and an increase in gas generation in the anode slurry, it would therefore be obvious to one ordinarily skilled in the art to minimize to minimize the change in viscosity. Accordingly, where the effect of viscosity change on stability would continue to apply at beyond the 48 hour standing period of Jiang, it would further be obvious to one ordinarily skilled in the art to minimize the viscosity change up to and beyond the 7 day period of the instant claim. Accordingly, though Jiang does not explicitly disclose the structure of the limitation of the instant claim, they do make obvious optimizing the viscosity change rate of a metal-doped silicon oxide slurry such that it would satisfy the limitation of the instant claim, where Jiang makes obvious optimizing the viscosity change rate to be as close to 0 percent as possible, to improve the stability of the anode slurry.
Additionally, in regards to the limitation of the instant claim which requires that the content of the organic acid is more than 0.7 wt% and is 1.5 wt% or less based on a total weight of the anode composition though as discussed above Park makes obvious the inclusion of organic maleic acid as a moisture scavenger, Park fails to disclose a specific acid content within the range of the instant claim, disclosing that their moisture scavenger is based on the weight of the precursor rather than the full anode composition weight.
Therefore we look to Song, who discloses an anode active material (Abstract, “A negative active material for rechargeable lithium secondary batteries”). Here, Song discloses structure which comprises an organic acid which is included in an amount of 0.5 to 3% by weight (Paragraph 0023, “Additionally, the organic acid may be included in an amount of 0.5 to 3% by weight, based on the total weight of the solution including the organic acid.”), where the organic acid may include acids which include maleic acid, oxalic acid, glutaric acid, and acetic acid (Paragraph 0022, “In addition, the organic acid may include at least one selected from the group consisting of acetic acid, propionic acid, stearic acid, pyruvic acid, acetoacetic acid, glyoxylic acid, oxalic acid, malonic acid, maleic acid, glutaric acid, adipic acid, phthalic acid, trimellitic acid, and a mixture thereof.”). Here, Song discloses that when the acid content fails within this range, it is capable of effective coating, as well as avoiding performance degradation (Paragraph 0049, “When the content of the coating layer is less than 0.5 parts by weight, it is difficult to coat the core completely, and thus the lithium titanium oxide constituting the core may be exposed to the outside, resulting in side reactions caused by generated moisture and thus gas generation. On the other hand, when the content of the coating layer is greater than 3 parts by weight, reduction in initial battery efficiency and performance degradation may be caused due to an increase in thickness of the coating layer.”). Accordingly, it would be obvious to one ordinarily skilled in the art to make use of the 0.5 to 3.0 percent by weight range for the organic acid content of Choi. Additionally, this constitutes a prima facie case of obvious based on an encompassing range, where the range of 0.5 to 3.0 percent by weight encompassed the weight range of 0.7 to 1.5 percent by weight, as per MPEP section 2144.05(I): “In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990) (The prior art taught carbon monoxide concentrations of "about 1-5%" while the claim was limited to "more than 5%." The court held that "about 1-5%" allowed for concentrations slightly above 5% thus the ranges overlapped.)”.
Regarding Claim 7, modified Choi makes obvious the invention of Claim 1. Additionally, Choi discloses structure which comprises a binder (Paragraph 0058, “Furthermore, the negative electrode active material layer may further comprise a binder”), as well as disclosing that the binder acts to provide adhesion between primary particles (Paragraph 0043, “The adhesive binder may be disposed between the primary particles to provide adhesion between the primary particles, and thus, the adhesive binder may allow the primary particles to be aggregated, bonded, or assembled to form the secondary particle”), thereby thickening the overall structure. Accordingly, where Choi further discloses that their structure comprises a plurality of binders (Paragraph 0060, “The binder may comprise at least one selected from the group consisting of”), and where the binders act to both bind and thicken, Choi inherently discloses structure which comprises both a binder and a thickener.
Regarding Claim 8, modified Choi makes obvious the invention of Claim 7. Additionally, Choi discloses structure wherein the anode composition comprises a styrene-butadiene rubber (Paragraph 0060, “a styrene-butadiene rubber (SBR),”), thereby reading upon the limitation of the instant claim which requires structure wherein the binder comprises at least one of an acrylic binder and styrene-butadiene rubber.
Regarding Claim 9, modified Choi makes obvious the invention of Claim 7. Additionally, Choi discloses structure which comprises carboxymethylcellulose (Paragraph 0060, “carboxymethylcellulose (CMC),”). Accordingly, Choi reads upon the limitation of the instant Claim which requires structure wherein the thickener includes carboxymethylcellulose.
Regarding Claim 22, modified Choi makes obvious the invention of Claim 1. Additionally, in regards to the limitation of the instant claim which requires structure wherein the organic acid does not include polyacrylic acid, Choi discloses structure which comprises a binder that does not include polyacrylic acid (Paragraph 0060, “The binder may comprise at least one selected from the group consisting of a polyvinylidene fluoride-hexafluoropropylene copolymer (PVDF-co-HFP), polyvinylidene fluoride (PVDF), polyacrylonitrile, polymethylmethacrylate, polyvinyl alcohol, carboxymethylcellulose (CMC), starch, hydroxypropyl cellulose, regenerated cellulose, polyvinylpyrrolidone, tetrafluoroethylene, polyethylene, polypropylene, polyacrylate, an ethylene-propylene-diene monomer (EPDM), a sulfonated EPDM, a styrene-butadiene rubber (SBR), a fluorine rubber, polyacrylic acid, and polymers in which hydrogen thereof is substituted with Li, sodium (Na), or Ca, and may also comprise various copolymers thereof.”).
Claim(s) 6 is/are rejected under 35 U.S.C. 103 as being unpatentable over Choi (US 20200168890 A1), Park (US 20170222221 A1) and Jiang (US 20200266428 A1), and Song (US 20160276672 A1) as applied to claim 1 above, and further in view of Oshawa (US PGPUB 20190260030 A1).
Regarding Claim 6, modified Choi makes obvious the invention of Claim 1. However, Choi is silent in regards to the pH of the negative electrode composition, and we therefore look to Oshawa, which is an analogous art to the instant application. Here, Oshawa discloses a lithium secondary battery which includes a negative electrode active material (Abstract, “A lithium-ion secondary battery includes at least a negative electrode, a positive electrode, and an electrolyte. The negative electrode includes at least a negative electrode active material and a polymer binder.”). Additionally, Oshawa discloses structure where the pH of the negative electrode material may be adjusted to not be lower than 7 and not higher than 9 (Paragraph 0109, “The pH of the negative-electrode-forming coating material may be adjusted to not lower than 7 and not higher than 9, for example.”), disclosing that when the quantity of acidic groups that facilitates said pH range is lower than such required for said range, bond strength and capacity retention is (Paragraph 0178, “In Comparative Examples 1 to 3, cycle capacity retention was low. It is considered that because the amount of acidic functional groups per unit surface area of graphitic material 21 was lower than 0.017 mmol/m2, the bond strength between graphitic material 21 and polymer binder 23 was low.”), and when the quantity is higher than such required for said pH range, side reactions occur readily, reducing cycle capacity retention (Paragraph 0179, “In Comparative Example 4, cycle capacity retention was low. It is considered that because the amount of acidic functional groups per unit surface area of graphitic material 21 was greater than 0.086 mmol/m2, phenomena such as side reactions of the electrolyte solution and variations in reactions readily occurred.”). Additionally, Oshawa discloses the benefit of capacity retention improvement when the quantity of acidic groups is such that said pH is achieved (Paragraph 0050, “When the amount of acidic functional groups per unit surface area is within such a range, cycle capacity retention is expected to be improved.”). Accordingly, where Oshawa discloses this as being necessary for the effective function of the negative electrode active material, as well as providing the benefit of improved cycle capacity retention, and Choi is silent in regards to the pH of the material, one ordinarily skilled in the art would find it obvious to apply the teaching of the pH range of Oshawa’s invention to the invention of Choi.
Claim(s) 14 and 16-19 is/are rejected under 35 U.S.C. 103 as being unpatentable over Choi (US 20200168890 A1), in further view of Park (US 20170222221 A1) and Hosaka (US 20150125744 A1), and Song (US 20160276672 A1).
Regarding Claim 14, Choi is an analogous art to the instant application, disclosing structure of an anode composition (Abstract, “A negative electrode active material”) for a lithium (Paragraph 0027, “intercalation of lithium ions may be smoothly performed”) secondary battery (Paragraph 0027, “Accordingly, the initial efficiency of the secondary battery may be improved.”). Additionally, Choi discloses structure which comprises a metal-doped silicon oxide (Paragraph 0049, “That is, the metal compound-doped primary particle further comprises a metal compound in the primary particle, wherein it denotes a particle in which the metal compound is doped into the primary particle which comprises the core comprising SiOx (0≤x<2);”) with the formula SiOx 0<x<2.
Additionally, Choi discloses structure wherein the anode composition includes a metal silicate area on a surface portion thereof. Here, Choi’s structure comprises a core comprising silicon dioxide (Paragraph 0023, “The core comprises SiOx (0≤x<2). The SiOx (0≤x<2) may be in the form in which silicon (Si) and SiO2 are included.”), and a metal doped silicon oxide (Paragraph 0053, “In an embodiment of the present invention, the metal compound may be included in the core of the primary particle. The metal compound may be formed by oxidation of a metal which may reduce the SiOx (0≤x<2), specifically, a metal having a reducing power capable of reducing silicon dioxide (SiO2 ) in the SiOx (0≤x<2) to silicon. The metal compound may comprise at least one of metal oxide and metal silicate.”; Paragraph 0049, “That is, the metal compound-doped primary particle further comprises a metal compound in the primary particle, wherein it denotes a particle in which the metal compound is doped into the primary particle which comprises the core comprising SiOx (0≤x<2)”; Paragraph 0055, “The metal silicate may comprise a silicate of at least one selected from the group consisting of Li, Mg, Al, Ca, and Ti. Specifically, the metal silicate may be at least one of MgSiO3, Mg2SiO4, Li2SiO3, Li4SiO4, Li2Si2O5, Al6SiO13, and Al4SiO8.”). Additionally, Choi discloses structure which comprises an intermediate layer covering the core (Paragraph 0050, “the intermediate layer which covers at least a portion of the surface of the core”), which means that the core has an outer surface. Therefore, where the core is the metal doped silicon dioxide, and the core comprises a surface, and where surface areas of the surface are areas on surface portions of the core, the core therefore comprises a metal silicate area on a surface portion of the core.
Additionally, Choi discloses structure wherein a metal doped to the metal-doped silicon oxide (Abstract, “wherein the first primary particle includes a core including SiOx, wherein 0≤x<2,”; Paragraph 0047, “The primary particle included in the secondary particle may be a metal compound-doped primary particle in which at least one of the core, the intermediate layer, and the carbon coating layer comprises a metal compound.”) includes at least one selected from the group consisting of lithium magnesium, calcium, and aluminum (Paragraph 0055, “The metal silicate may comprise a silicate of at least one selected from the group consisting of Li, Mg, Al, Ca, and Ti.”).
Additionally, in regards to the limitation which requires structure wherein the anode material comprises an organic acid including maleic acid, Choi is silent in regards to the inclusion of an acid component in their anode composition. Therefore, we look to Park, which is an analogous art to the instant application, disclosing an electrode composition for a lithium secondary battery which comprises lithium oxide (Abstract, “The present invention relates to a positive electrode active material for a lithium secondary battery,”). Here, Park discloses structure which includes a mixture of acids which act as a moisture scavenger, comprising a mixture of citric acid, tartaric acid, glycolic acid, and maleic acid (Paragraph 0148, “Specifically, the moisture scavenger may include citric acid, tartaric acid, glycolic acid, maleic acid or the like, and any one, or a mixture of two or more of these may be used.”). Additionally, Park discloses that the moisture scavenger acid is implemented in response to electrolyte decomposition and active material deterioration due to moisture inside the battery (Paragraph 0004, “This is due to a phenomenon occurring when an electrolyte is decomposed or an active material is deteriorated due to moisture inside the battery or other influences, or inner resistance of the battery increases.”).
Accordingly, though Park discloses their composition as being used in a positive electrode, a formulation that minimizes deterioration would be equally valuable in the negative electrode, as both the positive and negative electrode engage in ion intercalation and deintercalation, as disclosed by Park (Paragraph 0078, “lithium complex metal oxide as a compound capable of reversible intercalation and deintercalation of lithium (lithiated intercalation compound).”; Paragraph 0176, “The negative electrode active material may use a compound capable of reversible intercalation and deintercalation of lithium.”). Additionally, Park discloses similar structure in the positive and negative electrodes, where the negative electrode active material includes metal oxides capable of doping and dedoping lithium (Paragraph 0176, “Specific examples thereof may [include] metal oxides capable of doping and dedoping lithium such as SiOx (0<x<2), SnO2 , vanadium oxides and lithium vanadium oxides”), and the positive electrode active material includes a complex lithium metal oxide (Paragraph 0067, “A positive electrode active material for a lithium secondary battery according to an embodiment of the present invention includes a core including a first lithium complex metal oxide”) capable of ion transfer (Paragraph 0055, “and by the particles that form the shell having a crystal structure with orientation facilitating lithium ion intercalation and deintercalation”). Therefore, it would be obvious to one ordinarily skilled in the art to make use of the moisture scavenger of Park, employing it in the anode of Choi, thereby making obvious the limitation of the instant claim which requires that the anode composition comprise an organic acid including maleic acid.
Additionally, as discussed above Park discloses a moisture scavenging acid mixture comprising a mixture of citric acid, tartaric acid, glycolic acid, and maleic acid (Paragraph 0148, “Specifically, the moisture scavenger may include citric acid, tartaric acid, glycolic acid, maleic acid or the like, and any one, or a mixture of two or more of these may be used.”), thereby reading upon the limitation of the instant Claim which requires structure wherein the organic acid further includes at least one selected from a group which includes citric acid, tartaric acid, and glycolic acid.
However, Choi is silent in regards to explicit structure such that the metal-doped silicon oxide particle satisfies the equation A/B ≤ 16.0.
Though Choi is silent in regards to the measurement of peak area of the metal silicate and silicon dioxide via a deconvolution of the Si2p XPS spectrum of the active material where A corresponds to metal silicate peak area and B corresponds to silicon dioxide peak area such that A/B ≤ 16.0, where XPS analysis depicts the presence of specific electrons in the examined specimen, and where the Si2p examines both metal silicate and silicon dioxide silicon particles, Choi discloses the that their structure comprises a metal silicate (Paragraph 0055, “The metal silicate may comprise a silicate of at least one selected from the group consisting of Li, Mg, Al, Ca, and Ti. Specifically, the metal silicate may be at least one of MgSiO3, Mg2SiO4, Li2SiO3, Li4SiO4, Li2Si2O5, Al6SiO13, and Al4SiO8.”), which is a metal doped silicon oxide present alongside silicon dioxide that is not doped (Paragraph 0138, “which included both of the primary particle not doped with metal and the primary particle having a metal compound doped into at least one of the core…”).
Here, where Choi discloses metal silicates (Paragraph 0055, “The metal silicate may comprise a silicate of at least one selected from the group consisting of Li, Mg, Al, Ca, and Ti. Specifically, the metal silicate may be at least one of MgSiO3, Mg2SiO4, Li2SiO3, Li4SiO4, Li2Si2O5, Al6SiO13, and Al4SiO8.”) which comprises the same number of electrons in the 2p subshell as silicon dioxide, the formula of the instant limitation therefore represents a molar ratio of metal silicate to silicon dioxide, where the moles of metal silicate divided by the moles of silicon dioxide is less than or equal to 16.
Here, Choi discloses structure where the metal silicate is present within the core, where the core comprises doped and undoped silicon dioxide, at a weight ratio of undoped to doped particle ranges from 20:80 to 80:20 (Paragraph 0051, “In a case in which the secondary particle further comprises the metal compound-doped primary particle in addition to the primary particle, a weight ratio of the primary particle to the metal compound-doped primary particle may be in a range of 10:90 to 90:10, for example, 20:80 to 80:20”), and where the atomic weight of lithium is low, the weight ratio between silicon dioxide and lithium doped silicon dioxide is comparable to a molar ratio. Therefore, where the molar ratio that ranges from 80:20 to 20:80, the molar ratio of doped to undoped silicon dioxide ranges from 0.25 to 4 where the whole range falls within the scope of the limitation of the instant claim, thereby reading upon the limitation of the instant claim where A/B ≤ 16.0.
Assuming arguendo, that Choi does not disclose the claimed peak ratio, Choi discloses a structure which comprises a mixing ratio of lithium silicate powder to silicon dioxide powder which falls between 80:20 and 20:80, as discussed above, as well as further disclosing that the benefit of this ratio to be that it improves initial efficiency, capacity retention, and reduces an electrode thickness change rate (Paragraph 0051, “In a case in which the secondary particle comprises the primary particle and the metal compound-doped primary particle at the above weight ratio, advantages of each of the primary particle and the metal compound-doped primary particle may be appropriately harmonized to improve the initial efficiency while increasing the capacity retention and reduce an electrode thickness change rate.”), it would therefore be obvious to one ordinarily skilled in the art to select a molar mixing ratio which would produce an embodiment that possesses the peak ratio required by the instant claim, thereby making obvious a composition which reads upon the scope of the instant limitation, where A/B ≤ 16.0.
Here, where the instant claim requires that the ratio be 0.5 to 16, Choi further presents motivation to minimize the content of the silicon dioxide in the active material particle (Paragraph 0056, “SiO2 matrix may be reduced and the metal compound may be formed. Accordingly, since an amount of SiO2 , which acts as an initial irreversible phase, may be reduced, the initial efficiency of the battery may be improved”), so as to minimize the presence of an initial irreversible phase. Accordingly, this therefore makes obvious maximizing the content of the metal silicate component, where a metal silicate/silicon dioxide particle of Choi would have a molar ratio of 80:20, or an A/B value of 4, which thereby reads upon and makes obvious the limitation of the instant claim which requires structure where A/B is from 0.5 to 16.
Therefore, where the invention of Choi comprises silicon dioxide and metal silicates as discussed above, it would produce a peak area at 102 eV corresponding to the peak area of the metal silicate and a peak area at 104 eV corresponding to the peak area of silicon dioxide if exhibited to XPS analysis on the metal-doped silicon oxide particle.
Additionally, Choi discloses structure wherein their anode composition does not include a metal salt containing magnesium or aluminum (Paragraph 0013, “there is provided a negative electrode active material which is a secondary particle comprising primary particles, wherein the primary particle comprises a core comprising SiOx (0≤x<2); an intermediate layer which covers at least a portion of a surface of the core and comprises silicon nitride, silicon oxynitride, or a mixture thereof; and a carbon coating layer which covers at least a portion of the intermediate layer and comprises nitrogen-doped carbon.”).
Additionally, in regards to the limitation of the instant claim which requires that the content of the organic acid is more than 0.7 wt% and is 1.5 wt% or less based on a total weight of the anode composition though as discussed above Park makes obvious the inclusion of organic maleic acid as a moisture scavenger, Park fails to disclose a specific acid content within the range of the instant claim, disclosing that their moisture scavenger is based on the weight of the precursor rather than the full anode composition weight.
Therefore we look to Song, who discloses an anode active material (Abstract, “A negative active material for rechargeable lithium secondary batteries”). Here, Song discloses structure which comprises an organic acid which is included in an amount of 0.5 to 3% by weight (Paragraph 0023, “Additionally, the organic acid may be included in an amount of 0.5 to 3% by weight, based on the total weight of the solution including the organic acid.”), where the organic acid may include acids which include maleic acid, oxalic acid, glutaric acid, and acetic acid (Paragraph 0022, “In addition, the organic acid may include at least one selected from the group consisting of acetic acid, propionic acid, stearic acid, pyruvic acid, acetoacetic acid, glyoxylic acid, oxalic acid, malonic acid, maleic acid, glutaric acid, adipic acid, phthalic acid, trimellitic acid, and a mixture thereof.”). Here, Song discloses that when the acid content fails within this range, it is capable of effective coating, as well as avoiding performance degradation (Paragraph 0049, “When the content of the coating layer is less than 0.5 parts by weight, it is difficult to coat the core completely, and thus the lithium titanium oxide constituting the core may be exposed to the outside, resulting in side reactions caused by generated moisture and thus gas generation. On the other hand, when the content of the coating layer is greater than 3 parts by weight, reduction in initial battery efficiency and performance degradation may be caused due to an increase in thickness of the coating layer.”). Accordingly, it would be obvious to one ordinarily skilled in the art to make use of the 0.5 to 3.0 percent by weight range for the organic acid content of Choi. Additionally, this constitutes a prima facie case of obvious based on an encompassing range, where the range of 0.5 to 3.0 percent by weight encompassed the weight range of 0.7 to 1.5 percent by weight, as per MPEP section 2144.05(I): “In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990) (The prior art taught carbon monoxide concentrations of "about 1-5%" while the claim was limited to "more than 5%." The court held that "about 1-5%" allowed for concentrations slightly above 5% thus the ranges overlapped.)”.
Regarding Claim 16, modified Choi makes obvious the invention of Claim 14. Additionally, Choi discloses structure which comprises a binder (Paragraph 0058, “Furthermore, the negative electrode active material layer may further comprise a binder”), as well as disclosing that the binder acts to provide adhesion between primary particles (Paragraph 0043, “The adhesive binder may be disposed between the primary particles to provide adhesion between the primary particles, and thus, the adhesive binder may allow the primary particles to be aggregated, bonded, or assembled to form the secondary particle”), thereby thickening the overall structure. Accordingly, where Choi further discloses that their structure comprises a plurality of binders (Paragraph 0060, “The binder may comprise at least one selected from the group consisting of”), and where the binders act to both bind and thicken, Choi inherently discloses structure which comprises both a binder and a thickener.
Regarding Claim 17, modified Choi makes obvious the invention of Claim 14. Additionally, Choi discloses structure wherein the anode composition comprises a styrene-butadiene rubber (Paragraph 0060, “a styrene-butadiene rubber (SBR),”), thereby reading upon the limitation of the instant claim which requires structure wherein the binder comprises at least one of an acrylic binder and styrene-butadiene rubber.
Regarding Claim 18, modified Choi makes obvious the invention of Claim 14. Additionally, Choi discloses structure which comprises carboxymethylcellulose (Paragraph 0060, “carboxymethylcellulose (CMC),”). Accordingly, Choi reads upon the limitation of the instant Claim which requires structure wherein the thickener includes carboxymethylcellulose.
Regarding Claim 19, modified Choi makes obvious the invention of Claim 14. Additionally, in regards to the limitation of the instant claim which requires structure wherein the organic acid does not include polyacrylic acid, Choi discloses structure which comprises a binder that does not include polyacrylic acid (Paragraph 0060, “The binder may comprise at least one selected from the group consisting of a polyvinylidene fluoride-hexafluoropropylene copolymer (PVDF-co-HFP), polyvinylidene fluoride (PVDF), polyacrylonitrile, polymethylmethacrylate, polyvinyl alcohol, carboxymethylcellulose (CMC), starch, hydroxypropyl cellulose, regenerated cellulose, polyvinylpyrrolidone, tetrafluoroethylene, polyethylene, polypropylene, polyacrylate, an ethylene-propylene-diene monomer (EPDM), a sulfonated EPDM, a styrene-butadiene rubber (SBR), a fluorine rubber, polyacrylic acid, and polymers in which hydrogen thereof is substituted with Li, sodium (Na), or Ca, and may also comprise various copolymers thereof.”).
Claim(s) 15 is/are rejected under 35 U.S.C. 103 as being unpatentable over Choi (US 20200168890 A1), Park (US 20170222221 A1) and Jiang (US 20200266428 A1), and Song (US 20160276672 A1) as applied to claim 14 above, and further in view of Oshawa (US PGPUB 20190260030 A1).
Regarding Claim 15, modified Choi makes obvious the invention of Claim 14. However, Choi is silent in regards to the pH of the negative electrode composition, and we therefore look to Oshawa, which is an analogous art to the instant application. Here, Oshawa discloses a lithium secondary battery which includes a negative electrode active material (Abstract, “A lithium-ion secondary battery includes at least a negative electrode, a positive electrode, and an electrolyte. The negative electrode includes at least a negative electrode active material and a polymer binder.”). Additionally, Oshawa discloses structure where the pH of the negative electrode material may be adjusted to not be lower than 7 and not higher than 9 (Paragraph 0109, “The pH of the negative-electrode-forming coating material may be adjusted to not lower than 7 and not higher than 9, for example.”), disclosing that when the quantity of acidic groups that facilitates said pH range is lower than such required for said range, bond strength and capacity retention is (Paragraph 0178, “In Comparative Examples 1 to 3, cycle capacity retention was low. It is considered that because the amount of acidic functional groups per unit surface area of graphitic material 21 was lower than 0.017 mmol/m2, the bond strength between graphitic material 21 and polymer binder 23 was low.”), and when the quantity is higher than such required for said pH range, side reactions occur readily, reducing cycle capacity retention (Paragraph 0179, “In Comparative Example 4, cycle capacity retention was low. It is considered that because the amount of acidic functional groups per unit surface area of graphitic material 21 was greater than 0.086 mmol/m2, phenomena such as side reactions of the electrolyte solution and variations in reactions readily occurred.”). Additionally, Oshawa discloses the benefit of capacity retention improvement when the quantity of acidic groups is such that said pH is achieved (Paragraph 0050, “When the amount of acidic functional groups per unit surface area is within such a range, cycle capacity retention is expected to be improved.”). Accordingly, where Oshawa discloses this as being necessary for the effective function of the negative electrode active material, as well as providing the benefit of improved cycle capacity retention, and Choi is silent in regards to the pH of the material, one ordinarily skilled in the art would find it obvious to apply the teaching of the pH range of Oshawa’s invention to the invention of Choi.
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).
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/J.W.E./Examiner, Art Unit 1725
/BASIA A RIDLEY/Supervisory Patent Examiner, Art Unit 1725