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 .
Examiner’s Comments
Applicants’ response filed on 8/4/2025 has been fully considered. Claims 3-4 are cancelled, claims 20-21 are new and claims 1-2, 5-21 are pending.
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.
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.
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 1-2, 5 and 7-12 are rejected under 35 U.S.C. 103 as being unpatentable over Okai (US 2018/0159124 A1) in view of Asami et al (JP H04-363865 A1) in further view of Wang et al (US 2017/0040598 A1).
A machine translation is being used as the English translation for Asami et al (JP H04-363865 A1).
Regarding claim 1, Okai discloses a negative electrode for a battery (paragraphs [0038] and [0042]), wherein the negative electrode comprises a copper foil (negative electrode current collector; paragraph [0042]), a layer formed from a negative electrode slurry disposed on the copper foil (negative electrode mixture layer supported on the negative electrode current collector; paragraph [0042]), wherein the negative electrode slurry comprises scale-like silicon particles (negative electrode active material capable of electrochemically absorbing and releasing lithium ions and including flaky silicon particles; paragraph [0029 and 0042]), a binder (paragraph [0042]) and graphite (conductive agent; paragraph [0043]). The negative electrode being for a non-aqueous secondary battery is an intended use limitation that is met by the battery structure noted in the references.
Okai does not disclose the negative electrode comprising the binder including a silicate.
However, Asami discloses a lithium battery with a negative electrode comprising silicon as an active material [006] and a binder comprising lithium silicate (paragraphs [0015]-[0017]).
It would have been obvious to one of ordinary skill in the art to modify the negative electrode of Okai to include the binder of lithium silicate of Asami in the negative electrode slurry of Okai because having lithium silicate as a binder does not react with lithium, does not react with the electrolyte, does not deteriorate at the electrode drying temperature, holds the active material particles without losing electrical conductivity and maintains flexibility as an electrode and has the following characteristics after drying of being insoluble in water and organic solvents, being non-flammable, having heat resistance up to 1,000 °C and exhibiting strong adhesive strength (paragraphs [0015]-[0017] of Asami).
Okai does not disclose the negative electrode comprising at least part of a surface of the flaky silicon particles being covered with a silicon dioxide film.
However, Wang discloses a method comprising providing a surface coating on silicon particles used as anodes in lithium batteries (paragraphs [0007], [0043-44], [0051] and claim 8) and wherein the surface coating includes silicon dioxide (silicon dioxide film; paragraphs [0007], [0043] and [0061-66]).
It would have been obvious to one of ordinary skill in the art to modify the negative electrode of Okai to include the surface coating of silicon dioxide of Wang on the scale-like silicon particles of Okai because having the required surface coating provides an expansion buffer for silicon particles during cycling (paragraph [0043 and 0059-0069] of Wang).
Wang does not appear to explicitly disclose the negative electrode comprising the thickness of the silicon dioxide film being 8 nm or more and 50 nm or less. Wang does teach that the silicon particles can be a variety of sizes including about 100nm [0056 and 0059]. The particle has a coating that may be silicon dioxide film that may coat substantially an entire surface of a particle [0063].
However, it would have been obvious to one of ordinary skill in the art to adjust the thickness of the surface coating of silicon dioxide to be 8 nm or more and 50 nm or less on a nanometer sized particle as one of ordinary skill in the art would reason that a coating would be generally smaller than the active material used in the electrode. One would find it obvious to try a variety of coating thicknesses because doing so would provide the desired expansion buffering for the silicon particles during cycling while not using excess material as a means for reducing cost. The surface coating provides an expansion buffer for silicon particles during cycling (paragraph [0043] of Wang).
The negative electrode being for a non-aqueous secondary battery is an intended use limitation that is met by the battery structure noted in the references. Since the structure of the negative electrode of Okai, Asami and Wang, as modified, is the same as the structure of the negative electrode as claimed in claim 1, it can be used as a negative electrode in a non-aqueous secondary battery.
Regarding claim 2, Okai discloses the negative electrode comprising the scale-like silicon particles having a thickness of 10 to 50 nm (paragraph [0025]) and a longest axis of 100 nm to 1 µm (major axis diameter; paragraph [0025]). The thickness and longest axis of the scale-like silicon particles overlaps the claimed range for the thickness and major axis diameter of the flaky silicon particles.
It would have been obvious to one of ordinary skill in the art to select any portion of the disclosed ranges including the instantly claimed ranges from the ranges disclosed in the prior art reference in order to provide sufficient mechanical strength, prevent destruction during high-speed charging and discharging and to provide the desired scale shape (paragraph [0025] of Okai). It has been held that “[i]n the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art” a prima facie case of obviousness exists.” Please see MPEP 2144.05, In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); and In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990).
Regarding claim 5, since the thickness and the longest axis of the scale-like silicon particles of Okai overlaps the claimed ranges for the thickness and major axis diameter, the scale-like silicon particles of Okai would inherently have a ratio of an area of white portions indicating crystals to an area of the silicon particles being 20% or less in a dark-field image of a silicon particle taken using a transmission electron microscope.
Regarding claim 7, Okai does not appear to explicitly disclose the negative electrode comprising the silicate including a lithium silicate.
However, Asami discloses a negative electrode comprising the binder comprising lithium silicate (paragraphs [0015]-[0017]) as previously noted.
It would have been obvious to one of ordinary skill in the art to modify the negative electrode of Okai to include the binder of lithium silicate of Asami in the negative electrode slurry of Okai because having lithium silicate as a binder does not react with lithium, does not react with the electrolyte, does not deteriorate at the electrode drying temperature, holds the active material particles without losing electrical conductivity and maintains flexibility as an electrode and has the following characteristics after drying of being insoluble in water and organic solvents, being non-flammable, having heat resistance up to 1,000 °C and exhibiting strong adhesive strength (paragraphs [0015]-[0017] of Asami).
Regarding claim 8, Okai discloses the negative electrode comprising graphite (conductive agent; paragraph [0043]).
Regarding claim 9, Okai discloses the negative electrode comprising 95% by weight of scale-like silicon particles (paragraph [0042]).
Okai does not teach a content of the flaky silicon particles in the negative electrode mixture layer is 20 mass% or more 94 mass% or less with respect to a total mass of the negative electrode mixture layer. The endpoint of 95% is sufficiently close to the endpoint of 94 mass% that it would render the limitation obvious. It is apparent that the instantly claimed amount of 94 mass% and that taught by Okai are so close to each other that the fact pattern is similar to the one in In re Woodruff , 919 F.2d 1575, USPQ2d 1934 (Fed. Cir. 1990) or Titanium Metals Corp. of America v. Banner, 778 F.2d 775, 227 USPQ 773 (Fed.Cir. 1985) where despite a “slight” difference in the ranges the court held that such a difference did not “render the claims patentable” or, alternatively, that “a prima facie case of obviousness exists where the claimed ranges and prior art ranges do not overlap but are close enough so that one skilled in the art would have expected them to have the same properties”.
In light of the case law cited above and given that there is only a “slight” difference between the amount of 95% by weight disclosed by Okai and the amount disclosed in the present claims and further given the fact that no criticality is disclosed in the present invention with respect to the amount of 94 mass%, it therefore would have been obvious to one of ordinary skill in the art that the amount of 94 mass% disclosed in the present claims is but an obvious variant of the amounts disclosed in Okai, and thereby one of ordinary skill in the art would have found the claimed invention obvious over the prior art.
Regarding claim 10, Okai does not disclose the negative electrode comprising a content of the silicate in the negative electrode mixture layer being 3 mass% or more and 20 mass% or less with respect to a total mass of the negative electrode mixture layer.
However, Asami discloses a negative electrode comprising a binder comprising lithium silicate (paragraphs [0015]-[0017]) and wherein the amount of binder is about 1 to 10% by weight (content of the silicate in the negative electrode mixture layer; paragraph [0018]).
It would have been obvious to one of ordinary skill in the art to modify the negative electrode of Okai to include the binder of lithium silicate of Asami in the negative electrode slurry of Okai because having lithium silicate as a binder does not react with lithium, does not react with the electrolyte, does not deteriorate at the electrode drying temperature, holds the active material particles without losing electrical conductivity and maintains flexibility as an electrode and has the following characteristics after drying of being insoluble in water and organic solvents, being non-flammable, having heat resistance up to 1,000 °C and exhibiting strong adhesive strength (paragraphs [0015]-[0017] of Asami).
Regarding claim 11, Okai discloses the negative electrode comprising graphite (conductive agent; paragraph [0043]).
Okai does not appear to explicitly disclose the content of the conductive agent in the negative electrode mixture layer being 3 mass% or more and 60 mass% or less with respect to a total mass of the negative electrode mixture layer.
However, it would have been obvious to one of ordinary skill in the art to adjust the amount of graphite in the negative mixture slurry of Okai to 3 mass% or more and 60 mass% or less as graphite is an known conductive material and because doing so would provide the desired conductivity of the negative electrode active material layer while not using excess material as a means for reducing cost.
Regarding claim 12, Okai discloses the negative electrode comprising a layer formed from a negative electrode slurry disposed on the copper foil (negative electrode mixture layer having a first material mixture layer disposed on a surface of the negative electrode current collector; paragraph [0042]) and wherein the negative electrode slurry comprises scale-like silicon particles (flaky silicon particles; paragraph [0042]), a binder (paragraph [0042]) and graphite (conductive agent; paragraph [0043]).
Okai does not appear to explicitly disclose the negative electrode comprising the binder including a silicate.
However, Asami discloses a negative electrode comprising a binder comprising lithium silicate (paragraphs [0015]-[0017]).
It would have been obvious to one of ordinary skill in the art to modify the negative electrode of Okai to include the binder of lithium silicate of Asami in the negative electrode slurry of Okai because having lithium silicate as a binder does not react with lithium, does not react with the electrolyte, does not deteriorate at the electrode drying temperature, holds the active material particles without losing electrical conductivity and maintains flexibility as an electrode and has the following characteristics after drying of being insoluble in water and organic solvents, being non-flammable, having heat resistance up to 1,000 °C and exhibiting strong adhesive strength (paragraphs [0015]-[0017] of Asami).
Okai and Asami does not appear to explicitly disclose the negative electrode comprising a second material mixture layer covering a surface of the first material mixture layer and wherein the second material mixture layer includes the silicate and the conductive agent.
However, it would have been obvious to one of ordinary skill in the art to duplicate the layer formed from a negative electrode slurry of Okai and Asami in order to provide an additional active material layer.
It has been held that "mere duplication of parts has no patentable significance unless a new and unexpected result is produced". Please see MPEP 2144.04 and In re Harza, 274 F.2d 669, 124 USPQ 378 (CCPA 1960). It would be obvious to duplicate the layer formed from a negative electrode slurry since the mere duplication of the layer formed from a negative electrode slurry would produce a known and unexpected result which would be higher capacity and longer life for the negative electrode active material.
Paragraph [0010] of Okai discloses that the conductive material layer with the scale-like silicon particles provides high capacity and long life for the negative electrode active material. Including a layer of binder and conductive material on the surface of the active material will provide the known properties of conducting electrons through the electrode during charge/discharge while the lithium silicate will not react with the electrolyte and will exhibit strong adhesive strength (paragraphs [0015]-[0017] of Asami).
Claim 6 is rejected under 35 U.S.C. 103 as being unpatentable over Okai (US 2018/0159124 A1) in view of Asami et al (JP H04-363865 A1) in further view of Wang et al (US 2017/0040598 A1) in further view of Araki et al (JP 2019-067579 A1).
Machine translations are being used as the English translation for Asami et al (JP H04-363865 A1) and Araki et al (JP 2019-067579 A1). The teachings of Okai, Asami and Wang have been made of record.
Regarding claim 6, modified Okai discloses a negative electrode comprising a carbon layer coated on the scale-like silicon particle (paragraph [0025]) and wherein the carbon layer comprises nanographene (paragraph [0030]). Wang teaches using various carbon phases, including amorphous carbon, in addition to the silicon particles [0053-0055 and 0062].
Okai, Asami and Wang may not explicitly disclose the negative electrode comprising the flaky silicon particles including at least one component selected from amorphous carbon, diamond, a zirconium oxide, an aluminum oxide, and an yttrium oxide..
However, Araki discloses a negative electrode comprising a negative electrode material (paragraph [0015]), wherein the negative electrode material comprises scaly silicon particles dispersed in a carbon material (paragraph [0016] and wherein the carbon material is nanographene or amorphous carbon (paragraph [0027]).
It would have been obvious to one of ordinary skill in the art to modify the negative electrode of Okai, Asami and Wang to include the carbon layer of amorphous carbon of Araki for the carbon layer of nanographene of Okai because having the required carbon material, such as amorphous carbon, on silicon particles reduces the exposed surface area, suppresses reaction with the electrolyte and suppresses deterioration of the active material (paragraph [0027] of Araki).
Claim 13 is rejected under 35 U.S.C. 103 as being unpatentable over Okai (US 2018/0159124 A1) in view of Asami et al (JP H04-363865 A1) in further view of Wang et al (US 2017/0040598 A1) in further view of Hirose et al (US 2008/0113270 A1).
A machine translation is being used as the English translation for Asami et al (JP H04-363865 A1). The teachings of Okai, Asami and Wang have been made of record.
Regarding claim 13, Okai discloses the negative electrode comprising a copper foil (negative electrode current collector including a metal foil; paragraph [0042]).
Okai, Asami and Wang do not appear to explicitly disclose the negative electrode comprising the metal foil having a surface roughness Ra of 0.5 µm or more and 5 µm or less.
However, Hirose discloses an anode comprising an anode current collector made of a metal material comprising copper (paragraph [0025]) and wherein the anode current collector has a surface roughness Ra of 0.1 µm or more and 3.5 µm or less (paragraph [0028]). The surface roughness Ra of the anode current collector overlaps the claimed range for the surface roughness Ra of the metal foil.
It would have been obvious to one of ordinary skill in the art to select any portion of the disclosed ranges including the instantly claimed ranges from the ranges disclosed in the prior art reference in order to improve the contact characteristics between the anode active material layer and the anode current collector and to prevent cracking of the anode current collector due to expansion of the anode active material layer (paragraph [0028] of Hirose). It has been held that “[i]n the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art” a prima facie case of obviousness exists.” Please see MPEP 2144.05, In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); and In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990).
It would have been obvious to one of ordinary skill in the art to modify the negative electrode of Okai, Asami and Wang to include the surface roughness Ra of the anode current collector of Hirose for the copper foil of Okai because doing so improves the contact characteristics between the anode active material layer and the anode current collector and to prevent cracking of the anode current collector due to expansion of the anode active material layer (paragraph [0028] of Hirose).
Claim 20 is rejected under 35 U.S.C. 103 as being unpatentable over Okai (US 2018/0159124 A1) in view of Asami et al (JP H04-363865 A1).
The teachings of Okai have been made of record.
Regarding claim 20, Okai discloses a negative electrode for a battery (paragraphs [0038] and [0042]), wherein the negative electrode comprises a copper foil (negative electrode current collector; paragraph [0042]), a layer formed from a negative electrode slurry disposed on the copper foil (negative electrode mixture layer supported on the negative electrode current collector; paragraph [0042]), wherein the negative electrode slurry comprises scale-like silicon particles (negative electrode active material capable of electrochemically absorbing and releasing lithium ions and including flaky silicon particles; paragraph [0042]), a binder (paragraph [0042]) and graphite (conductive agent; paragraph [0043]).
Okai does not disclose the negative electrode comprising the binder including a silicate.
However, Asami discloses a lithium battery with a negative electrode comprising silicon as an active material [006] and a binder comprising lithium silicate (paragraphs [0015]-[0017]).
It would have been obvious to one of ordinary skill in the art to modify the negative electrode of Okai to include the binder of lithium silicate of Asami in the negative electrode slurry of Okai because having lithium silicate as a binder does not react with lithium, does not react with the electrolyte, does not deteriorate at the electrode drying temperature, holds the active material particles without losing electrical conductivity and maintains flexibility as an electrode and has the following characteristics after drying of being insoluble in water and organic solvents, being non-flammable, having heat resistance up to 1,000 °C and exhibiting strong adhesive strength (paragraphs [0015]-[0017] of Asami).
Okai and Asami do not disclose the negative electrode comprising the silicate including potassium silicate.
However, it would have been obvious to one of ordinary skill in the art to modify the negative electrode of Okai and Asami to substitute the binder of lithium silicate of Asami in the negative electrode slurry for potassium silicate as both lithium and potassium are in the same column in the Periodic Table and have a +1 charge.
Claim 21 is rejected under 35 U.S.C. 103 as being unpatentable over Okai (US 2018/0159124 A1) in view of Asami et al (JP H04-363865 A1) in further view of Nanba et al (US 2013/0164611 A1).
Regarding claim 21, Okai discloses a negative electrode for a battery (paragraphs [0038] and [0042]), wherein the negative electrode comprises a copper foil (negative electrode current collector; paragraph [0042]), a layer formed from a negative electrode slurry disposed on the copper foil (negative electrode mixture layer supported on the negative electrode current collector; paragraph [0042]), wherein the negative electrode slurry comprises scale-like silicon particles (negative electrode active material capable of electrochemically absorbing and releasing lithium ions and including flaky silicon particles; paragraph [0042]), a binder (paragraph [0042]) and graphite (conductive agent; paragraph [0043]).Okai does not appear to explicitly disclose the negative electrode comprising the binder including a silicate.
However, Asami discloses a negative electrode comprising a binder comprising lithium silicate (paragraphs [0015]-[0017]).
It would have been obvious to one of ordinary skill in the art to modify the negative electrode of Okai to include the binder of lithium silicate of Asami in the negative electrode slurry of Okai because having lithium silicate as a binder does not react with lithium, does not react with the electrolyte, does not deteriorate at the electrode drying temperature, holds the active material particles without losing electrical conductivity and maintains flexibility as an electrode and has the following characteristics after drying of being insoluble in water and organic solvents, being non-flammable, having heat resistance up to 1,000 °C and exhibiting strong adhesive strength (paragraphs [0015]-[0017] of Asami).
Okai and Asami does not appear to explicitly disclose the negative electrode comprising a second material mixture layer covering a surface of the first material mixture layer and wherein the second material mixture layer includes the silicate and the conductive agent, but not the flaky silicon particles.
However, it would have been obvious to one of ordinary skill in the art to duplicate the layer formed from a negative electrode slurry of Okai and Asami in order to provide an additional active material layer that conducts electrons and will not react with the electrolyte.
Paragraph [0010] of Okai discloses that the conductive material layer with the scale-like silicon particles provides high capacity and long life for the negative electrode active material. Including a layer of binder and conductive material on the surface of the active material will provide the known properties of conducting electrons through the electrode during charge/discharge while the lithium silicate will not react with the electrolyte and will exhibit strong adhesive strength (paragraphs [0015]-[0017] of Asami).
In addition, Nanba discloses a power storage device comprising a silicon oxide layer between a negative electrode active material layer and a graphene layer (conductive agent; paragraph [0127]) and wherein the silicon oxide layer is a mixture of silicon oxide and silicate (paragraph [0127]).
The combination of the silicon oxide layer and the graphene layer on the negative electrode active material layer would provide the second material mixture layer.
It would have been obvious to one of ordinary skill in the art to modify the negative electrode of Okai to include the silicon oxide layer and the graphene layer of Nanba on the layer of negative electrode slurry of Okai because doing so provides a path through which carrier ions are transferred, expansion of the negative electrode active material layer is suppressed and breakdown of the negative electrode active material layer is suppressed while capacity of the negative electrode active material layer is maintained (paragraphs [0015]-[0017] of Asami).
Response to Arguments
Applicant’s arguments, see page 9, filed 8/4/2025, with respect to the claim objections have been fully considered and are persuasive. The claim objections have been withdrawn.
Applicant’s arguments, see page 9, filed 8/4/2025, with respect to the 112(b) rejections have been fully considered and are persuasive. The 112(b) rejections have been withdrawn.
Applicant's arguments filed 8/4/2025 have been fully considered but they are not persuasive.
Applicants argue that Okai in view of Asami in further view of Wang do not disclose or suggest amended claim 1 and that experimental data shows excellent initial charge and capacity retention performance.
This argument is not persuasive as Okai in view of Asami in further view of Wang disclose claim 1 as noted above. One of ordinary skill in the art would incorporate the silicon dioxide film as an expansion buffer for silicon particles during cycling (paragraph [0043] of Wang). The thickness of the silicon dioxide film is an optimizable feature and can be adjusted to be 8 nm or more and 50 nm or less because doing so would provide the desired expansion buffering for the silicon particles during cycling while not using excess material as a means for reducing cost. Also, the data in Applicant’s Specification is not commensurate in scope with the claims as criticality is only shown for 8 nm or more and 10 nm or less for the thickness and the claims are broader than Examples 1-3 of Applicant’s Specification.
Applicants argue that Wang does not disclose controlling thickness of the silicon dioxide film in the range of 8 nm or more and 50 nm or less.
This argument is not persuasive as the thickness of the silicon dioxide film is an optimizable feature and can be adjusted to be 8 nm or more and 50 nm or less because doing so would provide the desired expansion buffering for the silicon particles during cycling while not using excess material as a means for reducing cost. The data in Applicant’s Specification is not commensurate in scope with the claims as criticality is only shown for 8 nm or more and 10 nm or less for the thickness and the claims are broader than Examples 1-3 of Applicant’s Specification.
Conclusion
Applicant's amendment necessitated the new ground(s) of rejection presented in this Office action. Accordingly, THIS ACTION IS MADE FINAL. See MPEP § 706.07(a). Applicant is reminded of the extension of time policy as set forth in 37 CFR 1.136(a).
A shortened statutory period for reply to this final action is set to expire THREE MONTHS from the mailing date of this action. In the event a first reply is filed within TWO MONTHS of the mailing date of this final action and the advisory action is not mailed until after the end of the THREE-MONTH shortened statutory period, then the shortened statutory period will expire on the date the advisory action is mailed, and any nonprovisional extension fee (37 CFR 1.17(a)) pursuant to 37 CFR 1.136(a) will be calculated from the mailing date of the advisory action. In no event, however, will the statutory period for reply expire later than SIX MONTHS from the mailing date of this final action.
Any inquiry concerning this or earlier communications from the examiner should be directed to SATHAVARAM I REDDY whose telephone number is (571)270-7061. The examiner can normally be reached Monday-Friday 9:00 AM-6:00 PM EST.
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/SATHAVARAM I REDDY/Examiner, Art Unit 1785
/MARK RUTHKOSKY/Supervisory Patent Examiner, Art Unit 1785
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