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 .
Status of Claims
Claims 1-7 and 10 are currently pending, claims 1-7 have been amended and claim 10 is as originally presented.
Claims 8-9 and 11-12 have been canceled.
Claim Rejections - 35 USC § 103
The following is a quotation of the appropriate paragraphs of 35 U.S.C. 102 that form the basis for the rejections under this section made in this Office action:
A person shall be entitled to a patent unless –
(a)(1) the claimed invention was patented, described in a printed publication, or in public use, on sale, or otherwise available to the public before the effective filing date of the claimed 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.
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.
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, 7, and 10 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 (a type of adsorbent clay) 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 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).
Response to Arguments
Applicant's arguments filed 08 May 2026 have been fully considered but they are not persuasive.
Applicant traverses the rejection of claim 1 over McDaniel et al. in view of CN ‘284A. Applicant argues that McDaniel does not teach or suggest the features of amended claim 1.
Applicant argues that McDaniel et al. does not teach the composition of claim 1. McDaniel et al. teaches a composition of 14±2 SiO2 : 1 Al2O3 : 15±2 Na2O : 350±50 H2O, prepared at or below 35°C, aged at or below 25°C for at least 2 hours which applicant argues is different from the instantly claimed seed material with a composition of 10-20 SiO2 : 1 Al2O3 : 10-20 Na2O : 200-300 H2O prepared by stirring for 1-1.5 hours, aged at 30-45°C for 18-26 hours. The ratios of SiO2, Al2O3, Na2O, and H2O in both McDaniel et al. and the instant application overlap, creating a case of prima facie obviousness. Specifically, the ranges of water added in the prior art and instant application both include an Al2O3 : H2O ratio of 1 : 300. McDaniel et al. does not teach that the seed mixture is prepared by aging at 30-45°C, however as discussed in the above rejection of amended claim 1 a person of ordinary skill in the art at the relevant time would have been motivated to optimize the aging temperature for improved crystallinity based on the teachings of McDaniel et al. cited above.
Applicant further argues that McDaniel does not discuss a process to produce a 13X zeolite cake as instantly claimed. The examiner acknowledges this argument. However, one cannot show nonobviousness by attacking references individually where the rejections are based on combinations of references. See In re Keller, 642 F.2d 413, 208 USPQ 871 (CCPA 1981); In re Merck & Co., 800 F.2d 1091, 231 USPQ 375 (Fed. Cir. 1986).
Applicant further argues that the 13X zeolite formed from the process as instantly claimed has unexpectedly superior properties to those taught by McDaniel, including 110-120% relative crystallinity, 750-810 m2/g surface area, enhanced nitrogen adsorption capacity, and improved crushing strength. However, the observed properties of the instantly claimed 13X zeolite are not unexpectedly superior to other reported 13X zeolites. For example, McDaniel et al. teaches 13X zeolites synthesized using seeds which have surface areas between 700 and 843 m2/g (Table III, pp. 4). McDaniel et al. and CN ‘284A do not contemplate the nitrogen adsorption and crush strength of the produced 13X zeolites, however recognition of features of a product formed via a process suggested by McDaniel et al. and CN ‘284A does not render the process as instantly claimed nonobvious over the references. A person of ordinary skill in the art at the relevant time would have readily envisioned the properties observed in the instant application as being present in products formed by the combination of the procedures of McDaniel et al. and CN ‘248A.
Applicant further argues that CN ‘284A teaches generalized synthesis parameters for forming a 13X zeolite using a seeded approach, and does not teach or suggest the criticality of the instantly application’s parameters towards yielding the aforementioned superior adsorbent properties of the 13X zeolite produced. CN ‘248A teaches a generalized approach to seed-assisted production of 13X zeolites. However, CN ‘284A explicitly teaches the criticality o the molar ratio of SiO2 and Al2O3 on the adsorbent efficiency of the resulting 13X zeolite. Furthermore, CN ‘284A explicitly teaches that 13X zeolites produced via the method disclosed do have a gas absorbency that is superior to commercial adsorbents [0006] and a significantly narrower range of the molar ratio of silica to alumina, which would contribute to the overall crystallinity of the 13X zeolites [0027]. With regard to the criticality of the reaction parameters time, CN ‘284A in Example 1 discloses mixing 2.2 SiO2 : 1 Al2O3 : 2.6 Na2O : 100 H2O with 6 wt% seeds, stirring for 60 minutes, and crystallizing at 95°C for 5 hours, followed by separation, washing, and drying to yield a 13X zeolite with superior CO2 adsorption and a small particle size. It is well known in the zeolite art that crystallization time (5 hours vs. claimed 8 hour minimum) and reagent concentration (1:100 vs. claimed 1:200-300) impacts particle size, and a person of ordinary skill would have been capable of optimizing the crystallization time and H2O : Al2O3 ratio to yield a different crystallite size. Therefore, applicant’s argument, that McDaniel et al. and CN ‘284A do not sufficiently disclose the criticality of the reaction parameters to achieving high adsorption, high specific area, and other physical parameters, is considered unpersuasive.
Applicant further argues that a person of ordinary skill in the art would not arrive at the process parameters of the amended claim 1 through the combination of McDaniel et al. and CN ‘284A with a reasonable expectation of success. Both McDaniel et al. and CN ‘284A are directed to the synthesis of faujasite or 13X-type zeolites via a seed-assisted approach, and primarily differ only in the times and temperatures used for mixing, aging (if employed), and crystallization. A person of ordinary skill in the art at the relevant time would determine that the synthesis conditions presented in both references were compatible and would readily envision that the combination of the two references would lead to a desirable 13X zeolite product. With respect to the specific process parameters of amended claim 1, McDaniel et al. and CN ‘284A suggest the importance of developing highly crystalline seeds for use in creating a 13X zeolite product (as per the parameters of step a) and the success of a crystallization conducted at the temperatures and times instantly claimed. Therefore, there is no reason why a person of ordinary skill in the art at the relevant time would be incapable of optimizing the process parameters disclosed by McDaniel et al. and CN ‘284A to yield the instantly claimed parameters with a reasonable expectation of successfully synthesizing a 13X zeolite with excellent physical properties relevant for gas adsorption.
Applicant further argues that the proposed combination of McDaniel et al. and CN ‘284A to yield the synthesis parameters instantly claimed could only be derived using impermissible hindsight reconstruction. In response to applicant's argument that the examiner's conclusion of obviousness is based upon improper hindsight reasoning, it must be recognized that any judgment on obviousness is in a sense necessarily a reconstruction based upon hindsight reasoning. But so long as it takes into account only knowledge which was within the level of ordinary skill at the time the claimed invention was made, and does not include knowledge gleaned only from the applicant's disclosure, such a reconstruction is proper. See In re McLaughlin, 443 F.2d 1392, 170 USPQ 209 (CCPA 1971).
Applicant traverses the rejection of claims 2-7 and 10 by virtue of their dependency on amended claim 1, which they argue as being allowable, and on account of the additionally recited features. As stated previously, the arguments presented in regards to amended claim 1 are considered unpersuasive. As such, the argument that claims 2-7 and 10 are allowable by virtue of their dependency on claim 1 are also unpersuasive. As applicant has not clearly pointed out or stated the patentable novelty which makes claims 2-7 and 10 allowable in view of the presented prior art and the rejections made, these arguments are also considered not persuasive.
Conclusion
The prior art made of record and not relied upon is considered pertinent to applicant's disclosure:
Pourazar et al. (2020 Mater. Res. Express 7 035004) for providing a systematic study of the effect of reagent molar ratios (and effective solution concentration), gel alkalinity, crystallization time and crystallization temperature on the adsorbent properties of 13X zeolites synthesized via seeded supports.
THIS ACTION IS MADE FINAL. 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 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.
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/MORDECAI M LEAVITT/Examiner, Art Unit 1742 /CHRISTINA A JOHNSON/Supervisory Patent Examiner, Art Unit 1742
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