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 .
Priority
Acknowledgment is made of applicant’s claim for foreign priority under 35 U.S.C. 119 (a)-(d). The certified copy has been filed in parent Application No. IN202141059895, filed on 21 December 2021.
Information Disclosure Statement
The information disclosure statement (IDS) submitted on 07/25/2023 has been considered by the examiner. The non-patent literature citations of Anbia et. al. and Koohsaryan et. al. were struck from the IDS as full copies of the literature were not provided.
Claim Objections
Claim 8 is objected to because of the following informalities:
The limitation, “wherein the binder is selected from a clay, an organic polymer,” should instead read “wherein the binder is selected from a clay or an organic polymer,” to clarify that the limitation is intended as two options for the binder. In light of the examples given in the specification, the claim is interpreted for examination purposes to mean the binder may be either a clay or organic polymer. If applicant instead intended to draw the claim to an organic polymer originating from a clay, the claim language should be amended to reflect such.
Appropriate correction is required.
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(b):
(b) CONCLUSION.—The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the inventor or a joint inventor regards as the invention.
The following is a quotation of 35 U.S.C. 112 (pre-AIA ), second paragraph:
The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the applicant regards as his invention.
Claim 11 is rejected under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), second paragraph, as being indefinite for failing to particularly point out and distinctly claim the subject matter which the inventor or a joint inventor (or for applications subject to pre-AIA 35 U.S.C. 112, the applicant), regards as the invention.
The claim limitation, “said 13X zeolite adsorbent has crystallinity in the range of 110 - 120%,” is considered indefinite for failing to adequately state how a relative crystallinity is being measured and/or calculated. In light of the specification, examiner assumes that crystallinity refers to a relative crystallinity with respect to a 13X zeolite-based adsorbent standard. In amending the claim, applicant is reminded that materials must be defined in universal terms, and that commercial or trade names do not have a precise meaning.
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.
Claims 1-5 are rejected under 35 U.S.C. 103 as being unpatentable over McDaniel et. al. (US Patent 4,166,099; 1979) in view of Chinese Patent Publication No. CN110790284A (published 14 February 2020, provided English translation cited herein).
In regard to claim 1, McDaniel teaches a synthetic methodology for seed-assisted growth of Type X and Type Y faujasite zeolites (Col. 2, lines 49-53 & 60-64). The 13X zeolite as instantly claimed is understood to have a cubic faujasite-type framework in space group Fd-3m with ring sizes of 12,6, and 4T-atoms (see Results and reaction mechanism, pp. 1399; Guo et. al., Ads. Sci. & Tech., 36(7-8), 2018, 1389-1404). Structurally, this characterizes the 13X zeolite as a synthetic faujasite zeolite (Framework type FAU, Database of Zeolite Structures, 2007) and could reasonable be synthesized by the methods disclosed by McDaniel et. al.
McDaniel et. al. teaches a method of preparing a type X faujasite zeolite seed material (e.g. nucleation centers) by mixing sodium aluminate, sodium silicate, sodium hydroxide, and water in a ratio of 15±2 Na2O:1 Al2O3:14±2 SiO2:350±50 H2O, stirring for 1 hour (Col. 4, lines 25-26, pp. 3), aging the zeolite seeds for 22 hours (Col. 4, lines 26-29, pp. 3), filtering, and washing (Col. 2, line 15-22, pp. 1 & Example 1, pp. 3). The ratio of reagents for preparing the seed material is encompassed by the claimed ratio in the instant application, and the time of stirring and aging are within the instantly claimed ranges.
McDaniel et. al. teaches a method of preparing a type X faujasite zeolite by mixing sodium aluminate, sodium silicate, sodium hydroxide, and the seed material with ratios 3.6-7.5 Na2O:1 Al2O3:3-5 SiO2:75-300 H2O (ratios converted from Col. 2, lines 50-60, pp. 1) and 0.1-10% of seed material (Col. 3, lines 27-32, pp. 3). The reagents are combined by rapid mixing (Col. 3, lines 12-15 and lines 23-27, pp. 3) and heated at 60-110°C to form crystalline zeolites (Col. 3 line 51 – Col. 4. line 4, pp. 3). The zeolite product is preferably recovered by filtration and washed (Col 4, lines 5-10, pp. 3). It would have been obvious to one having ordinary skill in the art at the time the invention was made to choose the instantly claimed reaction temperatures and durations through process optimization, since it has been held that there the general conditions of a claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. See In re Boesch, 205 USPQ 215.
McDaniel et. al. does not teach that the seed material is aged at 30-45°C. However, McDaniel et. al. states that it may be preferable to use seed materials which are highly crystalline (Col. 2, lines 35-38, pp. 2). McDaniel et. al. further teaches and that seed materials aged at or below 25°C do not exhibit crystalline patterns (Col. 2, lines 26-29, pp. 2) and suggests that total crystallization of the zeolite samples does not occur until a reaction temperature of 60°C (Col. 3, lines 40-42, pp. 3). One of ordinary skill in the art would find it obvious to optimize the seed material aging temperature, which is demonstrated to affect the structure of the product, to achieve a greater degree of crystallinity in the zeolite seed materials.
McDaniel et. al. does not teach that the prepared zeolite material is stirred for 50-70 minutes, that the crystallization step is carried out for 8-12 hours, or that the wash solvent is demineralized water. However, CN ‘284A teaches a method of producing a 13X zeolite with crystallite seeds, where in preparing the zeolite material solution, the reagents are stirred for 0.1 to 6 hours (paragraph [0014]). CN ‘284A further teaches that the solution is crystallized at 90-120°C for 3-12 hours (paragraph [0015]). CN ‘284A teaches that the 13X zeolites prepared by the disclosed method contain a narrower distribution range of silicon-to-aluminum over conventional methods (paragraph [0027]). Therefore, it would be obvious to one of ordinary skill in the art at the relevant time to modify the conditions of McDaniel et. al. with the reaction times and temperatures of CN ‘248A to achieve improved physical characteristics of the 13X zeolite.
Like McDaniel et. al., CN ‘284A also teaches the solid 13X zeolite is washed after crystallization (paragraph [0015]). While neither art explicitly teaches a wash solvent, when working with an aqueous reaction mixture one of ordinary skill in the art would find it obvious to use demineralized or deionized water as a wash solvent to remove side salt products.
In regard to claims 2 and 3, McDaniel et. al. teaches that the amount of seed material used to prepared 13X zeolite may be 0.5 wt% of the product which is within the claimed ranges (Example 2, Col 4, lines 46-47, pp. 3).
In regard to claim 4, McDaniel et. al. teaches the ratio of reagents 15±2 Na2O:1 Al2O3:14±2 SiO2:350±50 H2O to prepare the seed material (Col. 2, line 15-22, pp. 1), which overlaps the instantly claimed ratio of 12-15 SiO2:1 Al2O3:13-16 Na2O:250-300 H2O. The subject matter as a whole would have been obvious to one of ordinary skill in the art at the time invention was made to have selected the overlapping portion of the range disclosed by the reference because overlapping ranges have been held to be a prima facie case of obviousness. In re Malagari, 182 USPQ.
In regard to claim 5, McDaniel et. al. teaches the ratio of reagents 3.6-7.5 Na2O:1 Al2O3:3-5 SiO2:75-300 H2O to form a gel mixture (Col. 2, lines 50-60, pp. 1), which overlaps the instantly claimed ratio of 2-4 SiO2:1 Al2O3:3-5 Na2O:250-300 H2O. The subject matter as a whole would have been obvious to one of ordinary skill in the art at the time invention was made to have selected the overlapping portion of the range disclosed by the reference because overlapping ranges have been held to be a prima facie case of obviousness. In re Malagari, 182 USPQ.
Claims 6-8 and 10-12 are rejected under 35 U.S.C. 103 as being unpatentable over McDaniel et. al. and CN ‘284A as applied to claim 1 above, and further in view of Khoramzadeh et. al. (J. Chem. Eng. Data, 64, 2019, pp. 5648-5664).
In regard to claim 6, McDaniel et. al. teaches that after crystallization, the prepared 13X zeolites may be dried or used as an aqueous slurry (Col. 4, lines 7-10, pp. 3). McDaniel et. al. does not set forth specific drying temperatures or durations or suggest that the zeolite material should be ground into a powder. However, Khoramzadeh et. al. teaches that after crystallization, 13X zeolite samples were dried at 100°C until the samples reached a constant weight (left column, lines 11-13, pp. 5650). In addition, the 13x zeolite material in referred to as a powder in the following step (right column, lines 9-11, pp. 5650). It would be obvious to one of ordinary skill in the art to assume it was necessary to first grind the 13X zeolite product into a powder before mixing with a binder. It would be obvious to modify the teachings of McDaniel et. al. with the teachings of Khoramzadeh to produce a 13X zeolite product which is intended to be used as an adsorbent. Furthermore, the determination of optimal temperature and duration of drying is considered to be a part of routine experimentation. It would have been obvious to one having ordinary skill in the art at the time the invention was made to choose the instantly claimed temperature through process optimization, since it has been held that there the general conditions of a claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. See In re Boesch, 205 USPQ 215.
In regard to claim 7, the teachings of McDaniel et. al., CN ‘284A, and Khoramzadeh et. al. are applied as above.
McDaniel et. al. and CN ‘284A do not teach a method for producing a 13X zeolite adsorbent. Khoramzadeh et. al. teaches a method for producing a 13X zeolite adsorbent by mixing a 13X zeolite powder with 5 wt% bentonite as a binder and water, extruding the resulting paste into pellets, and drying the extruded pellets at 100°C for 3 hours (Section 2.3, pp. 5650). It would be obvious to one of ordinary skill in the art to apply the teachings of Khoramzadeh et. al. to McDaniel et. al. to produce a 13X zeolite adsorbent from a wide range of 13X zeolite compositions. Using seeding, McDaniel et. al. achieves crystallization of a wide range of reagent ratios, many of which McDaniel et. al. teaches do not crystallize without seed material present (Example III, Col. 5, lines 9-13, pp. 4). Therefore, a person of ordinary skill would be motivated to apply the methods of Khoramzadeh et. al. to 13X zeolite materials taught by McDaniel et. al. that could not be made using the non-seeded synthesis methods discussed in the work.
Khoramzadeh does not teach the claimed extrude drying temperature of 120°C. It would have been obvious to one having ordinary skill in the art at the time the invention was made to choose the instantly claimed drying temperature through process optimization, since it has been held that there the general conditions of a claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. See In re Boesch, 205 USPQ 215.
In regard to claim 8, the method of Khoramzadeh et. al. uses bentonite as a binder, which is an absorbent clay (Section 2.3, pp. 5650).
In regard to claim 10, the method of Khoramzadeh et. al. uses a weight ratio of 5% bentonite with respect to dry zeolite powder, which is within the instantly claimed wt% range of 2-5 wt% (Section 2.3, pp. 5650).
In regard to claim 11, Khoramzadeh et. al. is silent on the relative crystallinity of the produced 13X adsorbent with respect to a standard. Khoramzadeh et. al. teaches that changing synthesis parameters such as molar ratio of the reaction mixture, reactants, pH of reaction mixture, and time and temperature of the crystallization step influence the type of zeolite created, and thus are results-effective (Section 1, left column, pp. 5648). Therefore, one of ordinary skill in the art at the relevant time would have been capable of optimizing the synthesis parameters to yield the desired degree of crystallinity of 13X zeolite material in the adsorbent, such as the 110-120% relative crystallinity instantly claimed. It would have been obvious to one of ordinary skill, in the art at the time, to modify the teachings of McDaniel et. al., CN ‘284A, and Khoramzadeh et. al. via parameter optimization to yield a 13X zeolite material and adsorbent with a crystallinity higher than 13X zeolite standards. It has been held that when the general conditions of a claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. See In re Boesch, 205 USPQ 215.
In regard to claim 12, Khoramzadeh et. al. teaches a 13X adsorbent with a BET specific surface area of 786.38 m2/g, which is within the instantly claimed range of 750-810 m2/g (13X, Table 2, pp. 5653).
Claim 9 is rejected under 35 U.S.C. 103 as being unpatentable over McDaniel et. al., CN '284A, and Khoramzadeh et. al. as applied to claim 7 above, and further in view of Anbia et. al. (Scientia Iranica, 26(3), 2019, pp. 1497-1504).
McDaniel et. al., CN ‘284A, and Khoramzadeh et. al. do not teach using polyvinyl alcohol as a binder to produce a 13X zeolite adsorbent. However, Anbia et. al. teaches a method of creating 13X zeolite granules comprising mixing a 13X zeolite powder with a binder, polyvinyl alcohol, and water, preparing beads (spherical granules) using a lab-sized disc-type granulator, and drying the beads at 70°C for 2 hours (Section 2.2, pp. 1498).
Anbia et. al. teaches that the identity of the binder has a clear effect on the final material, as clay minerals such as bentonite influence the porosity of shaped zeolites while organic binders like polyvinyl alcohol can be decomposed under oxidizing conditions, leaving micropores unblocked (left column, lines 9-17, pp. 1498). Therefore, it would have been obvious to one of ordinary skill, in the art at the time, to modify the teachings of McDaniel et. al., CN ‘284A, and Khoramzadeh et. al. to substitute polyvinyl alcohol for bentonite as the adsorbent binder in order to provide an easy method to remove binder obstructing the adsorbent’s microporous structures, such as calcination.
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to MORDECAI M LEAVITT whose telephone number is (571)272-6637. The examiner can normally be reached Monday-Friday 8AM-5PM.
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, CHRISTINA JOHNSON can be reached at (571) 272-1176. 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.
/MORDECAI M LEAVITT/Examiner, Art Unit 1742 /CHRISTINA A JOHNSON/Supervisory Patent Examiner, Art Unit 1742