Notice of Pre-AIA or AIA Status
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
Claim Objections
Claim 7 is objected to because of the following informalities: “...of an intensity the light…” should be “…of an intensity of the light…” Appropriate correction is required.
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) 1-4, 6, 8-10, and 12-20 is/are rejected under 35 U.S.C. 103 as being unpatentable over Dvoranova (Radical Intermediates in Photoinduced Reactions on TiO2 (An EPR Spin Trapping Study), 2014) in view of Nosaka (Electron Spin Resonance Studies on the Oxidation Mechanism of Sterically Hindered Cyclic Amines in TiO2 Photocatalytic Systems, 2016), Bonke (In situ electron paramagnetic resonance spectroscopy for catalysis, 2021), and Guo (The design of X-band EPR cavity with narrow detection aperture for in vivo fingernail dosimetry after accidental exposure to ionizing radiation, 2021), as evidenced by Dewar (EPR Cells, 2010).
Regarding claim 1, Dvoranova discloses a method for monitoring and evaluating the photocatalytic activity of a photocatalytic substance (Abstract), comprising:
mixing and dissolving 4-oxo-2,2,6,6-tetramethylpiperidine (TMPO) in a liquid to form a TMPO solution (3. Experimental Section, para. 1-2; The TiO2 P25 suspensions containing the spin trapping agent or the TMPO was mixed, 3. Experimental Section, para. 2);
dispersing particles of the photocatalytic substance (TiO2 P25 suspension) in the TMPO solution to form a photocatalytic suspension The TiO2 P25 suspensions containing the spin trapping agent or the TMPO was mixed, 3. Experimental Section, para. 2);
purging the photocatalytic suspension by introducing a gas composition to a reactor containing the photocatalytic suspension in the dark to form a purged photocatalytic suspension (…carefully saturated with air or oxygen using a slight gas stream immediately before the EPR measurement. 3. Experimental Section, para. 2);
illuminating the purged photocatalytic suspension in the reactor with a light to initiate a photocatalytic reaction and generate a reactive oxygen species (ROS) that is detectable by an electron paramagnetic resonance (EPR) spectrometer (During the EPR photochemical experiments the samples were irradiated at 295 K directly in the EPR resonator; 3. Experimental Section, para. 2);
wherein the EPR spectrometer comprises an EPR cell (small quartz flat cell (WG 808-Q, optical cell length 0.04 cm; Wilmad-LabGlass, Vineland, NJ, USA; 3. Experimental Section, para. 2; See WG 808-Q cells from Dewar, page 1) having a sample inlet and a sample outlet (See Figure of Dewar below, the cell contains both an inlet and outlet), a cavity for holding the EPR cell (…optimized for the TE102 cavity (Bruker, Rheinstetten, Germany) 3. Experimental Section, para. 2), at least one magnet component that are adjacent to the cavity to generate a magnetic field around the cavity (…spectrometer X-band EPR spectrometer (EMXplus, Bruker), 3. Experimental Section, para. 2);
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introducing a portion of the purged photocatalytic suspension via the sample inlet to the EPR cell in the cavity of the EPR spectrometer to generate an EPR signal by detecting the reactive oxygen species (So prepared samples were transferred to a small quartz flat cell, 3. Experimental Section, para. 2);
reacting TMPO with the reactive oxygen species (The concentration of molecular oxygen in aqueous TiO2 suspensions play an important role during the oxidation of 4-oxo-2,2,6,6-tetramethylpiperidine (TMPO) to the radical product 2,2,6,6-tetramethylpiperidine N-oxyl (Tempone; aN = 1.617 mT, a13C(413C) = 0.610 mT; g = 2.0054).) to form a EPR silent compound (2,2,6,6-tetramethylpiperidine N-oxyl; 2.3. Oxidation of Sterically Hindered Amine in TiO2 suspensions, para. 2) thereby reducing the intensity of the EPR signal generated by the reactive oxygen species; and
continuously recording the EPR signal (EPR spectra were recorded in situ during a continuous photoexcitation or after a defined exposure; 3. Experimental Section, para. 2);
wherein the EPR signal is numerically digitally displayed and visually displayed to monitor and evaluate the photocatalytic activity of the photocatalytic substance suspended in the liquid (Figure 9).
Dvoranova is silent regarding EPR utilizing two magnet components or a pump for conveying the purged solution to the EPR cell, TEMPOL, and a step of introducing a gas composition to a reactor containing the photocatalytic suspension under continuous agitation and a step of recirculating the purged suspension.
Regarding limitation of utilizing 4-hydroxy-2,2,6,6,-tetramethylpiperidine-N-oxyl (TEMPOL), analogous art Nosaka discloses a 2-step reaction mechanism of 4-hydroxy-2,2,6,6, tetramethylpiperidine (HTMP) (a homolog to the 2,2,6,6, tetramethylpiperidine of Dvoranova, MPEP 2144.09). Nosaka discloses HTMP becomes TEMPOL under photocatalytic conditions with TiO2 as the catalyst (Scheme 2(A), page 12994). Furthermore, the staple TEMPOL would react with superoxide (ROS) to form TEMPONE. Since Nosaka discloses the TMP would need to undergo photocatalytic reaction to form TEMPOL before reacting with ROS, it would have been obvious to one of ordinary skill in the art before the effective filing date to have substituted TEMPOL (along with necessary minor changes to EPR machine operating parameter) directly in place of TMP with a reasonable expectation of success, doing so streamline the process.
Regarding limitation of using a pump for conveying the purged solution to the EPR cell, a step of introducing a gas composition to the reactor under continuous agitation, and a step of recirculating the purged suspension back to the reactor via the sample outlet after passing through the EPR cell, analogous art Bonke discloses a method and apparatus for monitoring and evaluating the photocatalytic activity of a photocatalytic substance (Homogeneous gas-liquid reactions and Heterogeneous gas-liquid reactions, page 3-4; Figure 2; Here, we showcase the use of the experimental in situ EPR set- ups shown in Fig. 2 in catalytic reactions in various studies to demonstrate broad applicability, Page 8; Photocatalysis, Pages 12-13), comprising:
purging a photocatalytic suspension by introducing a gas composition (O2 dosing Figure 2C-2D) to a reactor containing the photocatalytic suspension under continuous agitation in the dark to form a purged photocatalytic suspension (…with a capillary used to bubble gases through the analyte solution…dissolved oxygen and/or ozone in water… Heterogeneous photocatalysis, page 13, left col., para. 1-2; Figure 2C-2D);
introducing a portion of the purged photocatalytic suspension via the sample inlet to the EPR cell in the cavity of the EPR spectrometer to generate an EPR signal by detecting the reactive oxygen species and recirculating the portion of the purged photocatalytic suspension back to the reactor via the sample outlet after passing through the EPR cell (For reactions at ambient pressure and temperature, a versatile solution flow approach consists of a reaction vessel outside the EPR resonator with a pump used to cycle solution through a quartz tube running through the resonator (Fig. 2c)…The only addition is a tubing connection to flow reaction solution through a quartz tube within the resonator and back into the reaction vessel. Homogeneous gas-liquid reactions, page 4);
wherein the EPR comprises a pump for conveying the purged solution to the EPR cell (Pump, Figure 2C-2D).
As the experimental setup is set at temperature 295K (Dvoranova, 3. Experimental Section, para. 2), it would have been obvious to one of ordinary skill in the art before the effective to have utilizing recirculation setup disclosed by Bonke to derive the claimed invention, Bonke discloses the set-up is ideal for reaction at ambient pressure and temperature (page 4) and allows for automated transfer of solution to EPR cell.
With regard to utilizing two magnet components, Dvoranova in view of Bonke and Nosaka does not disclose two magnet components in the EPR cavity. In an analogous art, Guo discloses an EPR device wherein the cavity is surrounded by at least two magnet components (Figure 1). The design of Guo is based on the principle of applying uniform magnetic field (According to the principal rules of EPR spectroscopy, the magnetic field, modulation, and microwave electromagnetic field should be applied to the sample in a certain direction, amplitude, frequency, and other parameters at the same time, Results, The system design). It would have been obvious to one of ordinary skill in the art before the effective filing date to have incorporated a two-components magnet system based on Guo’s design to the device of Modified Bonke to derive the claimed invention. Doing so allows providing uniform magnetic field around the EPR cell in the cavity.
Regarding claims 2-4, Modified Dvoranova discloses claimed invention as discussed above in claim 1. Dvoranova discloses the photocatalytic substance is titanium dioxide P25 (3. Experimental Section, para. 2).
Regarding claim 6, Modified Dvoranova discloses the claimed invention as discussed above in claim 1. Dvoranova discloses the photocatlytic suspension is at a concentration of 0.167 mg/mL (Figure 9 caption).
Regarding claims 8, Modified Dvoranova discloses the claimed invention as discussed above in claim 1. Nosaka (after incorporation with Dvoranova) discloses the concentration of TEMPOL are 10-40 microM (Figure 3).
Regarding claim 9, Modified Dvoranova discloses the claimed invention as discussed above in claim 8. Neither Dvoranova nor Nosaka discloses the claimed range for concentration of TEMPOL. Nosaka discloses the stoichiometric relationship between TEMPOL and singlet oxygen (Scheme 2B). As the amount of oxygen in solution (hence the EPR silent products) are variables that can be modified, among others, by adjusting the amount of TEMPOL, with the oxygen and EPR silent products both increasing as the amount of TEMPOL is increased, the precise concentration of TEMPOL would have been considered a result effective variable by one having ordinary skill in the art before the effective filing date of the invention. As such, without showing unexpected results, the claimed concentration of TEMPOL cannot be considered critical. Accordingly, one of ordinary skill in the art before the effective filing date of the invention would have optimized, by routine experimentation, the concentration TEMPOL in the Nosaka to obtain the desired balance between the amount of oxygen and the amount of TEMPOL as taught by Nosaka (In re Boesch, 617 F.2d. 272, 205 USPQ 215 (CCPA 1980)), since it has been held that where the general conditions of the claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. (In re Aller, 105 USPQ 223). “[W]here the general conditions of a claim are disclosed in the prior art, it is not inventive to discover the optimum or workable ranges by routine experimentation.” See In re Aller, 220 F.2d 454, 456, 105 USPQ 233, 235 (CCPA 1955). The discovery of an optimum value of a known result effective variable, without producing any new or unexpected results, is within the ambit of a person of ordinary skill in the art. See In re Boesch, 205 USPQ 215 (CCPA 1980) (see MPEP § 2144.05, II.). “[W]here the general conditions of a claim are disclosed in the prior art, it is not inventive to discover the optimum or workable ranges by routine experimentation.” See In re Aller, 220 F.2d 454, 456, 105 USPQ 233, 235 (CCPA 1955). The discovery of an optimum value of a known result effective variable, without producing any new or unexpected results, is within the ambit of a person of ordinary skill in the art. See In re Boesch, 205 USPQ 215 (CCPA 1980) (see MPEP § 2144.05, II.).
Regarding claim 10, Modified Dvoranova discloses the claimed invention as discussed above in claim 1. Dvoranova discloses the photocatalytic substance does not absorb the TEMPOL under dark condition (The results obtained demonstrate that indirect EPR spectroscopy techniques represent valuable tools for the characterization of radical intermediates generated in irradiated TiO2 suspensions. 4. Conclusions, para. 2). Though Nosaka does not explicitly disclose TEMPOL does not absorb the light, the limitation is interpreted as an inherent property of TEMPOL. "Products of identical chemical composition can not have mutually exclusive properties." In re Spada, 911 F.2d 705, 709, 15 USPQ2d 1655, 1658 (Fed. Cir. 1990). A chemical composition and its properties are inseparable. Therefore, if the prior art teaches the identical chemical structure, the properties applicant discloses and/or claims are necessarily present (MPEP 2112.01, II).
Regarding claim 11, Modified Dvoranova discloses the claimed invention as discussed above in claim 1. Dvoranova discloses the TEMPOL has at least one peak in the range of 320 to 350 mT (Figure 9) on an EPR spectrum with a g-value of 1.97-2.03 (g = 2.0054; 2.3. Oxidation of Sterically Hindered Amine in TiO2 suspensions).
Regarding claim 13, Modified Dvoranova discloses the claimed invention as discussed above in claim 1. Dvoranova discloses the gas composition comprises air or oxygen (…carefully saturated with air or oxygen using a slight gas stream immediately before the EPR measurement. 3. Experimental Section, para. 2).
Regarding claim 14, Modified Dvoranova discloses the claimed invention as discussed above in claim 1. Nosaka (after modification with Dvoranova) discloses the EPR signal is collected at modulation frequency at a 100 kHz (Figure 1 caption).
Regarding claim 15, Modified Dvoranova discloses the claimed invention as discussed above in claim 1. Dvoranova discloses the sweep time is 20 s (scan, 20 s; 3. Experimental Section, para. 3) and width of 8-16 mT (sweep width, 8–16 mT, Experimental Section, para. 3).
Regarding claim 16, Modified Dvoranova discloses the claimed invention as discussed above in claim 1. Dvoranova discloses the EPR is collected at an amplitude attenuation of 10.53 mW (microwave power, 10.53 mW), and an amplitude modulation of 5-100 microTesla (modulation amplitude, 0.05–0.1 mT; 3. Experimental Section, para. 3).
Regarding the overlapping amplitude modulation, it would have been obvious to one of ordinary skill in the art before the effective filing date of the invention to have selected the overlapping portion of the ranges disclosed by the reference because selection of overlapping portion of ranges has been held to be a prima facie case of obviousness. See MPEP § 2144.05.I.
Regarding close amplitude attenuation 10.52 mW to the claimed range of 5 mW, it is the Examiner’s position that the disclosed values are close enough that one of ordinary skill in the art before the effective filing date of the invention would have expected the same properties. Case law holds that a prima facie case of obviousness exists where the claimed ranges and prior art ranges do not overlap but are close enough that one skilled in the art would have expected them to have the same properties. Titanium Metals Corp. of America v. Banner, 778 F.2d 775, 227 USPQ 773 (Fed. Cir. 1985).
Regarding claim 17, Modified Dvoranova discloses the claimed invention as discussed above in claim 1. Dvoranova discloses the reactive oxygen species presents is in the form of singlet oxygen (2.3. Oxidation of Sterically Hindered Amine in TiO2 suspension).
Regarding claim 18, Modified Dvoranova discloses the claimed invention as discussed above in claim 1. Nosaka (after modification with Dvoranova) discloses the EPR silent compound is 4-hydroxyl-tetramethypiperidine (Scheme 2B product).
Regarding claim 19, Modified Dvoranova discloses the claimed invention as discussed above in claim 1. Bonke (after modification with Dvoranova) discloses the set-up in Figure 2C-2D has no filtration required to separate photocatalytic substance from the photocatalytic suspension as the process is a recirculating and continuous flow reactor (Figure 2C-2D).
Regarding claim 20, Modified Dvoranova discloses the claimed invention as discussed above in claim 1. Dvoranova discloses the light intensity is 15 mW∙cm−2 (3. Experimental Section, para. 2) but does not disclose the signal intensity result. In method claims, it is the overall method steps that are given patentable weight not the intended result thereof because the intended result does not materially alter the overall method. In method claims, the intended result is not given patentable weight when it simply expresses the intended result of a process step positively recited (MPEP § 2111.04)
Claim(s) 5 is/are rejected under 35 U.S.C. 103 as being unpatentable over Dvoranova in view of Nosaka, Bonke, and Guo as discussed above in claim 1, and further in view of Evonic (AEROXIDE, AERODISP AND AEROPERL Titanium Dioxide as Photocatalyst, Technical Information 1243, 2018).
Regarding claim 5, Modified Dvoranova discloses the claimed invention as discussed above in claim 1. Dvoranova discloses commercial titanium dioxide Aeroxide® P25 (Evonic Degussa, Essen, Germany) was used for preparing the stock suspension (3. Experimental Section, para. 1). Evonic discloses the P25 consists of aggregated primary particles. The aggregates are several hundred nm in size and the primary particles have a mean diameter of approx. 21 nm (2.3. Properties of Aeroxide TiO2 P25, Page 4). Furthermore, Evonic discloses once the particle sizes reach above 200 nm, the particles lose their transparency (Figure 1, 2.2 Fundamental Properties, Page 4). Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date to have keep the average particle size of the particles to the range as claimed. Doing so allows for the particle solution to retain transparency (As can be seen from Figure 1 the pigmentary properties (white pigments have primary particle sizes around 200 – 500 nm) are no longer relevant for nanostructured particles. 2.2 Fundamental Properties, Page 4).
Claim(s) 7 is/are rejected under 35 U.S.C. 103 as being unpatentable over Dvoranova in view of Nosaka, Bonke, and Guo, as evidenced by Prozzi (Assessing a Photocatalytic Activity Index for TiO2 Colloids by Controlled Periodic Illumination, 2020).
Regarding claim 7, Modified Dvoranova discloses the claimed invention as discussed above in claim 1. Neither Dvoranova, Nosaka, nor Guo discloses the photonic efficiency of the photocatalytic suspension has a linear dependence on the square root of an intensity the light during the illuminating. Evidential reference Prozzi discloses that photonic efficiency of a TiO2 suspension/colloids has a linear dependence on square root of an intensity of the light during the illuminating (Intrinsic degradation rate (kDeg) as a function of the square root of the photonic flux incident on the reaction cell (I0). As required by the recombination regime hypothesis, kDeg shows a linear dependence on the square root of I0 with R2 = 0.991. Figure 5 Caption; A direct implication of the recombination regime is the dependence of the intrinsic degradation rate (kDeg) on the square root of the incident photonic flux (I0) (eq 2). Because, as illustrated in Section 2.2, this aspect is of fundamental importance for kinetic modeling under CPI conditions, this relationship was verified by performing a series of experiments at different incident photonic fluxes. 3. Results and Discussion, para. 1).
Claim(s) 12 is/are rejected under 35 U.S.C. 103 as being unpatentable over Dvoranova in view of Nosaka, Bonke, and Guo, as evidenced by Honle (Bluepoint LED, April, 2013).
Regarding claim 12, Modified Dvoranova discloses the claimed invention as discussed above in claim 1. Dvoranova discloses the light has an intensity in 15 mW∙cm−2 (3. Experimental Section, para. 2). Dvoranova discloses the light source is a UV LED monochromatic radiator (λmax = 365 nm; Bluepoint LED, Hönle UV Technology, Gräfelfing/München, Germany) (3. Experimental Section, para. 2). As disclosed by Honle, the Bluepoint LED is configured to display by UV light (365 nm, 385 nm; Spectral distribution, Page 3) and visible light (405 nm; Spectral distribution, Page 3).
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to MICKEY HUANG whose telephone number is (571)272-7690. The examiner can normally be reached M-F 9:30-5:30 PM ET.
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/M.H./Examiner, Art Unit 1758
/MARIS R KESSEL/Supervisory Patent Examiner, Art Unit 1758