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 .
Drawings
The drawings are objected to because:
At least one drawing submitted in file is in color without granted petition to accept color drawings.
In FIG. 12, the X-axis and Y-axis lack descriptive labels and units of measurement. Without these labels, the technical significance of the data points and the relationship between the variables cannot be understood, failing to provide a clear understanding of the claimed invention.
Appropriate correction is required.
Corrected drawing sheets in compliance with 37 CFR 1.121(d) are required in reply to the Office action to avoid abandonment of the application. Any amended replacement drawing sheet should include all of the figures appearing on the immediate prior version of the sheet, even if only one figure is being amended. The figure or figure number of an amended drawing should not be labeled as “amended.” If a drawing figure is to be canceled, the appropriate figure must be removed from the replacement sheet, and where necessary, the remaining figures must be renumbered and appropriate changes made to the brief description of the several views of the drawings for consistency. Additional replacement sheets may be necessary to show the renumbering of the remaining figures. Each drawing sheet submitted after the filing date of an application must be labeled in the top margin as either “Replacement Sheet” or “New Sheet” pursuant to 37 CFR 1.121(d). If the changes are not accepted by the examiner, the applicant will be notified and informed of any required corrective action in the next Office action. The objection to the drawings will not be held in abeyance.
Color photographs and color drawings are not accepted in utility applications unless a petition filed under 37 CFR 1.84(a)(2) is granted. Any such petition must be accompanied by the appropriate fee set forth in 37 CFR 1.17(h), one set of color drawings or color photographs, as appropriate, if submitted via the USPTO patent electronic filing system or three sets of color drawings or color photographs, as appropriate, if not submitted via the via USPTO patent electronic filing system, and, unless already present, an amendment to include the following language as the first paragraph of the brief description of the drawings section of the specification:
The patent or application file contains at least one drawing executed in color. Copies of this patent or patent application publication with color drawing(s) will be provided by the Office upon request and payment of the necessary fee.
Color photographs will be accepted if the conditions for accepting color drawings and black and white photographs have been satisfied. See 37 CFR 1.84(b)(2).
Specification
The disclosure is objected to because of the following informalities:
The use of the terms BODIPY®, LUDOX®, HP-INNOWax®, PoraPak®, QuantiNova® SYBR GREEN®, TWEEN® 20, Molecular Imager®, Gel Doc™, Triton™ X-100, ProLong Diamond®, SlowFade Diamond®, LSM 780®, ELYRA PS.1®, Axio Observer®, ZEN®, IVIS™, Rigaku®, JASCO®, and ShinCarbon ST®, which are a trade name or a mark used in commerce, has been noted in this application. The term should be accompanied by the generic terminology; furthermore the term should be capitalized wherever it appears or, where appropriate, include a proper symbol indicating use in commerce such as ™, SM , or ® following the term.
Although the use of trade names and marks used in commerce (i.e., trademarks, service marks, certification marks, and collective marks) are permissible in patent applications, the proprietary nature of the marks should be respected and every effort made to prevent their use in any manner which might adversely affect their validity as commercial marks.
Appropriate correction is required.
Claim Rejections - 35 USC § 112(d) or 35 U.S.C. 112 (pre-AIA ), fourth paragraph
The following is a quotation of 35 U.S.C. 112(d):
(d) REFERENCE IN DEPENDENT FORMS.—Subject to subsection (e), a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
The following is a quotation of pre-AIA 35 U.S.C. 112, fourth paragraph:
Subject to the following paragraph [i.e., the fifth paragraph of pre-AIA 35 U.S.C. 112], a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
Claims 2 and 3 are rejected under 35 U.S.C. 112(d) or pre-AIA 35 U.S.C. 112, 4th paragraph, as being of improper dependent form for not referencing to a claim previously set forth.
Claims 2 and 3 improperly depend from claim 20, which is a subsequently numbered claim. A dependent claim must refer to an earlier numbered claim. See 37 CFR 1.75(c) and MPEP § 608.01(n).
Correction is required to place the claims in proper dependent form. Appropriate correction may include renumbering the claims and/or amending the dependency so that each dependent claim refers only to a preceding claim.
Applicant may cancel the claim(s), amend the claim(s) to place the claim(s) in proper dependent form, rewrite the claim(s) in independent form, or present a sufficient showing that the dependent claim(s) complies with the statutory requirements.
Claim Rejections - 35 USC § 103
The following is a quotation of 35 U.S.C. 103 which forms the basis for all obviousness rejections set forth in this Office action:
A patent for a claimed invention may not be obtained, notwithstanding that the claimed invention is not identically disclosed as set forth in section 102, if the differences between the claimed invention and the prior art are such that the claimed invention as a whole would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to which the claimed invention pertains. Patentability shall not be negated by the manner in which the invention was made.
The factual inquiries for establishing a background for determining obviousness under 35 U.S.C. 103 are summarized as follows:
1. Determining the scope and contents of the prior art.
2. Ascertaining the differences between the prior art and the claims at issue.
3. Resolving the level of ordinary skill in the pertinent art.
4. Considering objective evidence present in the application indicating obviousness or nonobviousness.
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 20 is rejected under 35 U.S.C. 103 as being unpatentable over Garcia-Martinez (US 2012 0024776; cited on IDS filed August 2, 2023) in view of Zhang et al. (Catalysts, 2018; cited on PTO-892), Majeed and Saleh (Iraqi Journal of Chemical and Petroleum Engineering, 2016; cited on PTO-892), Miyazawa and Inagaki (Chemical Communications, 2000; cited on PTO-892), Gao et al. (The Journal of Physical Chemistry B, 2009; cited on PTO-892), Heracleous and Lemonidou (Journal of Catalysis, 2010; cited on PTO-892), and Varisli et al. (Industrial and Engineering Chemistry Research, 2008; cited on PTO-892).
Garcia-Martinez discloses a silica composite comprising an inorganic material such as ZSM-5 (a specific form of MFI) (claim 7) and a mesostructure such as MCM-41 (claim 14) for use as catalysts (abstract). Garcia-Martinez discloses that the mesopores can have an ordered arrangement (stereoregular) (¶ 129) and a narrow pore size distribution (uniformly-sized) (claim 10; ¶ 200), with diameters in a range of 2-60 nm (¶ 82) and with a pore wall thickness in a range of 1-5 nm (claim 9).
Garcia-Martinez does not disclosethe MFI silicalite with diameters of less than 2 nm located within the mesopore walls.
Zhang discloses that silicalite-1 is an all-silica zeolite with an MFI topology structure, having a pore diameter of about 5-6 Å (0.5-0.6 nm) and a three-dimensional channel structure (page 2, ¶ 3). Zhang discloses that silicalite-1 can be used as an effective catalyst due to its high-temperature resistance, strong hydrophobicity and oleophilicity, and the relative ease of synthesizing high-quality crystals (page 2, ¶ 3).
Majeed discloses a micro-mesoporous composite (abstract). Majeed discloses that the zeolite micropores can be less than 2 nm and mesopores can be 2-50 nm (page 71, column 2, ¶ 3). Majeed discloses that the composite can be multiporous (hierarchical) (page 73, column 1, ¶ 2) and can have ordered structure (stereoregular) (page 76, column 2, ¶ 2).
Miyazawa discloses that micropores can exist within the walls of mesopores such as MCM-41 (page 2121, column 1, ¶ 2). Miyazawa discloses that this bimodal pore system is an ideal porous material for catalysts (page 2121, column 1, ¶ 2).
It would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to use the MFI silicalite of Zhang having a pore diameter of less than 2 nm located within the mesopore walls for the silica composite of Garcia-Martinez for catalytic applications as taught by Majeed and Miyazawa. A person of ordinary skill in the art would have been motivated to make these modifications and reasonably would have expected success because Zhang teaches MFI silicalite such as silicalite-1 can be used as micropores for catalyst, Majeed teaches the silica composite can be hierarchical and stereoregular, and Miyazawa teaches that the micropores can be located within the mesopore walls for catalytic applications. Further, a person of ordinary skill in the art would have been motivated to use uniformly-sized microspores in order to achieve precise selectivity and homogeneous active sites of the catalysts.
None of Garcia-Martinez, Zhang, Majeed, and Miyazawa discloses the spherical silica.
Gao discloses that monodispersed spherical silica nanoparticles with controlled diameter (70-300 nm) and with uniform pores of 20 nm can be prepared (abstract; page 1798, Figure 2). Gao discloses that silica materials with controlled particle size, morphology, and porosity are highly attractive for a wide variety of nanotechnological applications such as catalysis (page 1796, column 1, ¶ 1).
It would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to add the spherical silica of Gao to the silica composite of Garcia-Martinez, Zhang, Majeed, and Miyazawa. A person of ordinary skill in the art would have been motivated to make these modifications and reasonably would have expected success because Gao teaches that monodispersed spherical silica nanoparticles can be used for applications in catalysis. “It is prima facie obvious to combine two compositions each of which is taught by the prior art to be useful for the same purpose, in order to form a third composition to be used for the very same purpose. [T]he idea of combining them flows logically from their having been individually taught in the prior art.” In re Kerkhoven, 626 F.2d 846, 850, 205 USPQ 1069, 1072 (CCPA 1980) see MPEP § 2144.06. A person of ordinary skill in the art would have been motivated to combine the spherical silica of Gao for use as catalysts and the silica composite of Garcia-Martinez, Zhang, Majeed, and Miyazawa for use as catalysts in order to form a third silica composite to be used as catalysts with increased catalytic performance provided by more active sites and improved stability. The pore size and particle size of spherical silica of the prior art overlap with those instantly claimed. In the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art” a prima facie case of obviousness exists. The pore size and particle size of spherical silica are clearly result effective parameters that a person of ordinary skill in the art would routinely optimize. Optimization of parameters is a routine practice that would be obvious for a person of ordinary skill in the art to employ and reasonably would expect success. It would have been customary for an artisan of ordinary skill to determine the pore size and particle size in order to best achieve the desired catalytic activity as these sizes critically determine catalytic activity by controlling reactant access to active sites, mass transfer, and stability of the catalysts. “[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 MPEP § 2144.05.
None of Garcia-Martinez, Zhang, Majeed, Miyazawa, and Gao discloses the active catalytic material such as nickel and cation dopant as in claim 20 impregnated on the silica composite.
Heracleous discloses the use of Ni-based mixed oxides doped metals as effective oxidative dehydrogenation catalysts (abstract). Specifically, Heracleous discloses that nickel oxide doped with metals such as Nb5+ exhibits improved catalytic performance in ethane oxidative dehydrogenation reaction (abstract).
Varisli discloses the impregnation procedures of catalysts such as silicotungstic acid into silica composite such as MCM-41 (abstract). Varisli discloses that the impregnated catalytic material shows high catalytic activity even at high temperature (page 4076, column 1, ¶ 1).
It would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to impregnate the catalyst of Heracleous into the silica composite of Garcia-Martinez, Zhang, Majeed, Miyazawa, and Gao using the impregnation method of Varisli. A person of ordinary skill in the art would have been motivated to make these modifications and reasonably would have expected success because Heracleous teaches Nb5+ doped nickel oxide can be used as an effective catalyst and Varisli teaches catalysts can be impregnated into the silica composite for improved stability. “It is prima facie obvious to combine two compositions each of which is taught by the prior art to be useful for the same purpose, in order to form a third composition to be used for the very same purpose. [T]he idea of combining them flows logically from their having been individually taught in the prior art.” In re Kerkhoven, 626 F.2d 846, 850, 205 USPQ 1069, 1072 (CCPA 1980) see MPEP § 2144.06. A person of ordinary skill in the art would have been motivated to combine the impregnation of Nb5+ doped nickel oxide of Heracleous and Varisli for use as catalysts and the silica composite of Garcia-Martinez, Zhang, Majeed, Miyazawa, and Gao for use as catalysts in order to form a third silica composite to be used as catalysts with increased catalytic performance provided by enhanced selectivity and improved stability. Accordingly, applying the teachings of Majeed, Zhang, Miyazawa, Gao, Heracleous, and Varisli to the silica composite of Garcia-Martinez to use as an oxidative dehydrogenation catalyst represents a predictable use of prior art elements according to their established functions and therefore renders claim 20 obvious.
Claim 2 is rejected under 35 U.S.C. 103 as being unpatentable over Garcia-Martinez, Zhang, Majeed, Miyazawa, Gao, Heracleous, and Varisli as applied to instant claim 20 above, and further in view of Vermeiren et al. (US 2008 0050308; cited on IDS filed August 2, 2023).
Garcia-Martinez, Zhang, Majeed, Miyazawa, Gao, Heracleous, and Varisli are discussed above.
None of Garcia-Martinez, Zhang, Majeed, Miyazawa, Gao, Heracleous, and Varisli discloses the silica composite has a silicon to aluminum molar ratio in a range of 1,000:1 to 3,000:1.
Vermeiren discloses zeolite materials such as aluminosilicate (¶ 45) having silicon/metal ratio from 22.5 to 15,000 (22.5:1 to 15,000:1) (¶ 43). Vermeiren teaches that the zeolite can be MFI (ZSM-5) (¶ 80). Vermeiren discloses that dealumination of zeolites improves process performance such as selectivity, product quality, catalyst stability, and reduced surface activity (¶ 4).
It would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to modify the silica composite of Garcia-Martinez, Zhang, Majeed, Miyazawa, Gao, Heracleous, and Varisli to have a low aluminum content as taught by Vermeiren. A person of ordinary skill in the art would have been motivated to make these modifications and reasonably would have expected success because Vermeiren teaches that silica composites can be made with low aluminum content for improving performance and reducing surface activity. Further, a person of ordinary skill in the art would have been motivated to make this modification in order to improve catalyst stability and to prevent unwanted side reactions. The silicon to aluminum ratio of the prior art overlap with that instantly claimed. In the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art” a prima facie case of obviousness exists. The silicon to aluminum ratio is clearly a result effective parameter that a person of ordinary skill in the art would routinely optimize. Optimization of parameters is a routine practice that would be obvious for a person of ordinary skill in the art to employ and reasonably would expect success. It would have been customary for an artisan of ordinary skill to determine the optimal silicon to aluminum ratio in order to best achieve the desired catalytic activity as the ratio determine catalytic activity by controlling acidity, selectivity, and stability of the catalysts . “[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 MPEP § 2144.05. Accordingly, applying the teachings of Vermeiren to the silica composite of Garcia-Martinez, Zhang, Majeed, Miyazawa, Gao, Heracleous, and Varisli to achieve low aluminum content represents a predictable use of prior art elements according to their established functions and therefore renders claim 2 obvious.
Claims 3 and 21 are rejected under 35 U.S.C. 103 as being unpatentable over Garcia-Martinez, Zhang, Majeed, Miyazawa, Gao, Heracleous, and Varisli as applied to instant claim 20 above, and further in view of Agúndez et al. (Studies in Surface Science and Catalysis, 2004; cited on IDS filed August 2, 2023).
In addition to the teachings of Garcia-Martinez, Zhang, Majeed, Miyazawa, Gao, Heracleous, and Varisli discussed above, Garcia-Martinez discloses that the silica composite have a pore volume of 0.05-2 cc/g (cm3/g) (claim 34). Garcia-Martinez discloses that the composites have a high surface area but does not specify exact numbers (¶ 194; ¶ 196). Garcia-Martinez discloses high surface areas facilitates access for bulky molecules and reduces intracrystalline diffusion barriers, thereby increase catalytic activity (¶ 208; ¶ 213; ¶ 220).
None of Garcia-Martinez, Zhang, Majeed, Miyazawa, Gao, Heracleous, and Varisli discloses the silica composite having a surface area in a range of 800-1,600 or 1,000-1,600 m2/g.
Agúndez discloses ZSM-5/MCM-41 materials having surface areas of 894-1373 m2/g and total pore volumes of 0.68-1.53 cm3/g (page 2910, Table 2). Agúndez discloses that most samples have high surface areas greater than 1,000 m2/g and exhibit enhanced catalytic activity (page 2910, ¶ 1; abstract).
It would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to modify the silica composite of Garcia-Martinez, Zhang, Majeed, Miyazawa, Gao, Heracleous, and Varisli to have high surface area as taught by Agúndez. A person of ordinary skill in the art would have been motivated to make these modifications and reasonably would have expected success because Agúndez teaches that silica composites can be made with high surface areas greater than 1,000 m2/g for improving catalytic activity. Further, a person of ordinary skill in the art would have been motivated to increase surface area in order to improve catalytic activity for bulky molecules and intracrystalline diffusivity. The pore volume and surface area of the prior art overlap with those instantly claimed. In the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art” a prima facie case of obviousness exists. The pore volume and surface area are clearly result effective parameters that a person of ordinary skill in the art would routinely optimize. Optimization of parameters is a routine practice that would be obvious for a person of ordinary skill in the art to employ and reasonably would expect success. It would have been customary for an artisan of ordinary skill to determine the optimal pore volume and surface area in order to best achieve the desired catalytic activity as the pore volume and surface area critically determine catalytic activity by controlling active site density and reactant diffusion. “[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 MPEP § 2144.05. Accordingly, applying the teachings of Agúndez to the silica composite of Garcia-Martinez, Zhang, Majeed, Miyazawa, Gao, Heracleous, and Varisli to achieve high surface area represents a predictable use of prior art elements according to their established functions and therefore renders claims 3 and 21 obvious.
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to JONG HWAN BAEK whose telephone number is (571)272-0670. The examiner can normally be reached Mon - Thu, 9 am - 3 pm ET.
Examiner interviews are available via telephone, in-person, and video conferencing using a USPTO supplied web-based collaboration tool. To schedule an interview, applicant is encouraged to use the USPTO Automated Interview Request (AIR) at http://www.uspto.gov/interviewpractice.
If attempts to reach the examiner by telephone are unsuccessful, the examiner’s supervisor, Michael G Hartley can be reached at 571-272-0616. The fax phone number for the organization where this application or proceeding is assigned is 571-273-8300.
Information regarding the status of published or unpublished applications may be obtained from Patent Center. Unpublished application information in Patent Center is available to registered users. To file and manage patent submissions in Patent Center, visit: https://patentcenter.uspto.gov. Visit https://www.uspto.gov/patents/apply/patent-center for more information about Patent Center and https://www.uspto.gov/patents/docx for information about filing in DOCX format. For additional questions, contact the Electronic Business Center (EBC) at 866-217-9197 (toll-free). If you would like assistance from a USPTO Customer Service Representative, call 800-786-9199 (IN USA OR CANADA) or 571-272-1000.
/JONG HWAN BAEK/Examiner, Art Unit 1618
/Nissa M Westerberg/ Primary Examiner, Art Unit 1618