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 1-5, 7, & 9-18 are currently pending and have been amended.
Claims 6 and 8 have been cancelled.
Claim Objections
Claim 14 is objected to because of the following informalities:
In claim 14, line 2, “duratoin,” appears to contain a typographical error and is intended to read as, “duration.”
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 10 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.
Claim 10 recites the limitation "the remaining part of the solution" in line 2. There is insufficient antecedent basis for this limitation in the claim.
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 1-4 are rejected under 35 U.S.C. 103 as being unpatentable over Chen et. al. (Microporous and Mesoporous Materials, 252, 2017 pp. 146-153).
In regard to claim 1, Chen et al. teaches a ZSM-23 zeolite (sample SNNa) with a total acid amount of 0.105 mmol/g and a strong acid content of >33% of the total acid amount when strong acids are characterized as having a desorption temperature above 350°C (SNNa in Table 3, pp. 150-151). Chen et al. does not teach that the strong acid content of the ZSM-23 zeolite is 10-28%. However, Chen et al. teaches that the acidity of ZSM-23 zeolites has a profound effect on its catalyst activity and lifetime (pp. 149, right column, 2nd paragraph – pp. 150, left column). Furthermore, of the catalysts tested, Pt/H-SNNa had the highest catalytic performance and best selectivity, which was attributed to the sample having the highest amount of weak and medium acid sites (i.e. the least strong acid sites) which favor production of a specific product (pp. 152, right column, 1st paragraph). Therefore, a person of ordinary skill in the art at the relevant time would have been motivated to further decrease the amount of strong acid sites characterized as having a desorption temperature above 350°C, and to optimize such composition, in order to improve selectivity of a ZSM-23 zeolite based catalyst based on the trends observed in the study by Chen et al. Therefore, it would have been obvious to one of ordinary skill in the art at the relevant time to select the range of strong acid content instantly claimed through process optimization as the strong acid content has been demonstrated to be a results-effective variable with regard to catalyst activity and selectivity and furthermore because 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 claims 2-3, Chen et. al. further teaches that the zeolite forms as needle-like crystals with dimensions of 500-1100 nm in length and 50-200 nm in diameter (left column, pp. 148), a SiO2:Al2O3 ratio of 80, 100, 120, 140 or 200 (Fig. 3b, pp. 149 and paragraph 3, right column, pp. 148), a specific surface area of 281 m2/g, and a pore volume of 0.35 cm3/g (SNNa in Table 2, pp. 150).
In regard to claim 4, Chen et. al. teaches ZSM-23 zeolite samples with 100% crystallinity relative to a reference sample (Fig. 4. & pp. 148, right column, paragraph 3). The process limitations in claim 4 are noted. However, when the examiner has found the same or substantially similar product as in the applied prior art, the burden of proof is shifted to applicant to establish that their product is patentably distinct and not the examiner to show the same process of making. In re Brown, 173 USPQ 685 and In re Fessmann, 180 USPQ 324.
Claims 5, 7, 9-18 are rejected under 35 U.S.C. 103 as being unpatentable over Chen et. al. as applied above for claim 1 and further in view of Wang et al. (Microporous and Mesoporous Materials, 134(1–3), 2010, pp. 203-209) and Chinese Patent Pub. CN104591213A (2015-05-06, machine translation provided and cited herein).
In regard to claim 5, Chen et al. does not teach the order of mixing reagents as claimed. Wang et al. teaches a method for preparing a ZSM-23 zeolite comprising forming a mixed solution containing a template agent, DMF (N,N-dimethylformamide, as claimed), and an aluminum source, aluminum sulfate; adding to the mixed solution a second solution of an alkali source, sodium hydroxide, and silicon source, silica sol to form a gel material; and crystallizing, filtering, washing, and drying the material (pp. 204, Section 2.2). Wang et al. discloses a clear benefit of DMF as a template agent as it both acts as a template agent and promotes nucleation and crystallization (pp. 206, right column, Section 3.3). Crystallization was conducted in 65 hours in Wang et al.’s method, versus 132 hours in Chen et al. This significant reduction in crystallization time provides ample justification to modify Chen et al.’s synthesis with the teachings of Wang et al. to hastened synthesis without compromising physical properties.
Further in regard to claim 5, neither Chen et al. or Wang et al. teaches the use of an aluminum-silica precursor as an aluminum source or reactant. However, CN ‘213A teaches a preparation of NaY zeolites (e.g. NaY-type molecular sieves) by mixing water, a silicon source, a directing/template agent, an alkali source, and a prepared amorphous silica-alumina precursor at 0-40°C and 9.5-12 pH to obtain a gel [0020], followed by crystallization, filtering, and drying [0021]. CN ‘213A teaches that the method improves other synthesis methods by preventing agglomeration of silica particles which commonly occurs when adding a large amount of the silicon source at once [0029]. Additionally, CN ‘213A teaches that zeolites prepared via the method had a large specific surface area, external surface area, and increased exposed pores [0028]. One of ordinary skill in the art would note the improved physical characteristics of the NaY-type zeolites would impart desirable adsorption properties as taught by CN ‘213A.
As typical synthesis preparations between the ZSM-23 and NaY-type zeolites differ primarily in the ratio of reagents used, one of ordinary skill in the art would assume the application of improvements synthesis of one zeolite composition to yield similar improvements in another. Therefore, it would have been obvious to one of ordinary skill in the art at the relevant time to modify the teachings of Chen et al. and Wang et al. to prepare and use an amorphous silica-alumina precursor in place of aluminum sulfate to yield a ZSM-23 zeolite with improved physical characteristics.
In regard to claim 7, Chen et al. teaches a ratio of SiO2:Al2O3 of 1:0.1 which is within the claimed molar ratio of silicon (as silica) : aluminum (as alumina) of 1:(0.10-0.85) and a ratio of 1:45 Al2O3:pyrrolidine which is within the claimed molar ratio of aluminum (as alumina) : template agent of 1:(10-100) (pp. 147, left column, Section 2.1.2).
In regard to claim 9, Chen et al. does not teach the instantly claimed preparation steps. However, CN ‘213A teaches a preparation of an amorphous silica-alumina precursor comprising the preparation of an aluminum source solution and a silicon source solution (not explicit in broad disclosure, but stated in Example 1, step (2)); acid-base neutralization to form a gel via introducing part of the silicon-containing material before and/or during the gelation process of the aluminum-containing material, and the remaining silicon-containing material is introduced after the aluminum-containing material is neutralized to form a gel; and aging the gel [0018]. The alkali aluminum source used is precipitated via the addition of CO2 during the gel forming process [0024]. As CN ‘213A discloses that a portion of the silicon-containing solution may be added at the beginning and during the gel forming reaction [0018], and that continuous neutralization titration is used to gel the aluminum source [0024], it teaches the instantly claimed gelation steps as CO2 would be continuously added and by necessity a portion of the total CO2 would be added to solution after the first addition of silicon-containing solution and after a second addition during the gelation process.
The method of CN ‘213A differs from the instant claim in that it does not teach that the first addition of CO2 accounts for 70-90% of the total volume of CO2 added. However, from the disclosure, a person of ordinary skill in the art would have arrived at such a range after routine experimentation. As noted above, the addition of CO2 is responsible for the precipitation of aluminum out of solution [0024]. The inventive concept of the process of CN ‘213A is that the silicon source is added in multiple parts to keep the concentration in the reaction solution low, thereby preventing agglomeration of silicon particles which disrupt the properties of the final product [0013], [0029]-[0030]. Therefore, it would have been obvious to add a majority of the required CO2, precipitating the majority of the added silicon source out of solution, before making a second addition. Determining the exact optimal ratio of CO2 added to solution between additions would have within the capabilities of one of ordinary skill in the art, 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. As noted above, the process of CN ‘213A solves a longtime problem in the art of silica agglomeration and poor distribution in zeolite products. Therefore, it would have been obvious to one of ordinary skill in the art to apply the teachings of CN ‘213A to the processes taught by Chen et al. and Wang et al. to impart improved characteristics onto the ZSM-23 products as noted in above rejections.
In regard to claim 10, CN ‘213A does not explicitly disclose that the second addition of a silicon-containing material accounts for 5-85 wt% the total silicon-containing material added. However, CN ‘213A teaches the addition of the silicon-containing material as a first aliquot of 0.17 L at the beginning of the gelation reaction, and a second aliquot of 0.33 L after the gelation reaction is completed [0041]. Since the working solution is homogenous, the first aliquot is 33 wt% and the second aliquot is 66 wt% the total material. If the silicon-containing material added during the gelation reaction (first aliquot), is split into two as suggested by CN ‘213A [0018], the second addition during gelation would necessarily be between 0 and 33 wt%, which overlaps the instantly claimed range of 5-85 wt%. 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. It would have been obvious to one of ordinary skill in the art to modify the teachings of Chen et al. and Wang et al. with the gelation process taught by CN ‘213A for reasons noted above with regard to claim 9, and to further optimize the combined teachings as noted here to achieve the optimal reaction parameters for the synthesis of ZSM-23 zeolites.
In regard to claim 11, CN ‘213A teaches the gelation reaction of the amorphous silica-alumina precursor is conducted between a temperature of 5-80°C and a pH of 7-10 ([0024], pp. 11), which overlap the instantly claimed ranges of 10-40°C and a pH of 9-12. With respect to the encompassing and overlapping ranges previously discussed, the subject matter as a whole would have been obvious to one of ordinary skill in the art at the time of invention to select the portion of the prior art’s range which is within the range of the applicants’ claims because it has been held prima facie case of obviousness to select a value in a known range by optimization for the results. In re Aller, 105 USPQ 233. Additionally, 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. It would have been obvious to one of ordinary skill in the art to modify the teachings of Chen et al. and Wang et al. with the gelation process taught by CN ‘213A for reasons noted above with regard to claim 9, and to further optimize the combined teachings as noted here to achieve the optimal reaction parameters for the synthesis of ZSM-23 zeolites.
In regard to claim 12, CN ‘213A teaches that the silicon-containing solution used to prepare the amorphous silica-alumina precursor is a sodium silicate solution [0041]. It would have been obvious to one of ordinary skill in the art to modify the teachings of Chen et al. and Wang et al. with the gelation process taught by CN ‘213A for reasons noted above with regard to claim 9.
In regard to claim 13, CN ‘213A teaches using a sodium aluminate solution with an 80 g/L Al2O3 concentration and a sodium silicate solution with a 150 g/L SiO2-NER58 concentration as reagents [0049]. CN ‘213A teaches the use of CO2 gas to neutralize excess aluminum salts during the formation of the amorphous silica-alumina precursor ([0024], pp. 11). CN ‘213A does not teach that the aluminum source solution has a concentration of 15-60 g/L or the concentration of CO2 gas is 30-60 v%.
With regard to the concentration of the aluminum source solution, it would have been obvious to one of ordinary skill in the art to use concentration of the aluminum source lower than what is disclosed in CN ‘213A because the ratio of alumina to silica and water is responsible for determining the formed structure of the zeolite. NaY-type zeolites, for which the process of CBN ‘213A is intended, have significantly lower silica:alumina ratios than ZSM-23 zeolites (below 10, [0012] & [0027] vs. 20+, Chen et al., Abstract). Therefore, decreasing the concentration of the aluminum source material would yield significantly higher silica:alumina ratios in the gel and be conducive to formation of ZSM-23 zeolites. 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 concentrations of the aluminum source solution 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.
With regard to the concentration of CO2, CN ‘213A further teaches that there is an optimal pH range (7-10, preferably 7.5-9) at which the reaction should be conducted, where the CO2 gas plays a key role as an acidic precipitant ([0024], pp. 11). Finding the optimal concentration of CO2 gas added to the reaction mixture to maintain a specific solution pH would be within the level of one of ordinary skill in the art. 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 CO2 gas concentration 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. It would have been obvious to one of ordinary skill in the art to modify the teachings of Chen et al. and Wang et al. with the gelation process taught by CN ‘213A for reasons noted above with regard to claim 9, and to further optimize the combined teachings as noted here to achieve the optimal reaction parameters for the synthesis of ZSM-23 zeolites.
In regard to claim 14, CN ‘213A broadly teaches that the aging of the precursor may be conducted at temperatures from room temperature (25°C) to 85°C and for a time of 0.2-8 hours ([0024], pp. 12) which overlaps the instantly claimed range of 10-40°C and encompasses the instantly claimed range of 5-60 minutes. With respect to the encompassing and overlapping ranges, the subject matter as a whole would have been obvious to one of ordinary skill in the art at the time of invention to select the portion of the prior art’s range which is within the range of the applicants’ claims because it has been held prima facie case of obviousness to select a value in a known range by optimization for the results. In re Aller, 105 USPQ 233. Additionally, 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. It would have been obvious to one of ordinary skill in the art to modify the teachings of Chen et al. and Wang et al. with the gelation process taught by CN ‘213A for reasons noted above with regard to claim 9, and to further optimize the combined teachings as noted here to achieve the optimal reaction parameters for the synthesis of ZSM-23 zeolites.
In regard to claim 15, Chen et. al. teaches that the reaction mixture prior to crystallization is stirred for 1 hour (pp. 147, Section 2.1.2, left column). Stirring conditions beyond time are not specified, which is suggestive that stirring was completed at standard temperature and pressure, 25°C and 1 atm. Furthermore, examiner considers finding the best conditions necessary to mix a solution in step (1) to be routine optimization. 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 stirring 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 16, the claimed amount of reagents added are based on the final charging ratio of components in the zeolite. To make the ratio of reagents comparable to the prior art, which only describe initial reactant ratios, the appropriate range of added hydroxide (ROH) can be back-calculated by doubling the range of the R2O unit cell (where R = an alkali metal). The given charging ratio of 1 SiO2:0.030-0.080 R2O in the ZSM-23 zeolite is then equivalent to 1 SiO2:0.030-0.160 ROH in the reaction mixture. Chen et. al. teaches a ratio of 1 SiO2:0.083 NaOH, which is within the claimed range (pp. 147, Section 2.1.2, left column).
In regard to claim 17, Chen et. al. teaches using fumed silica as the silicon source and sodium hydroxide as an alkali source as claimed in the instant application (pp. 147, Section 2.1.2, left column).
In regard to claim 18, Chen et. al. teaches a crystallization of a formed gel conducted at 180°C for 48 hours (pp. 147, NS-2 in Section 2.1.2, right column), drying of zeolite products at 65°C for 12 hours, and calcination at 550°C for 3 hours after temperature ramping (pp. 147, Section 2.1.1, 2nd paragraph). These preparation conditions are within the instantly claimed ranges of 150-200°C for 8-72 hours, 60-130°C for 2-12 hours, and 500-600°C for 2-8 respectively.
Response to Arguments
Applicant's arguments filed 13 May 2026 have been fully considered but they are not persuasive.
With regard to claims 1-4, applicant argues that Chen et al. does not anticipate the clams because Chen et al. does not teach the limitation of amended claim 1 that the strong acid content of the ZSM-23 zeolite is 18-28% of the total acid amount wherein strong acid sites are those having a desorption temperature above 350°C in a NH3-TPD. The examiner agrees with this finding, as Chen et al. teaches a ZSM-23 zeolite with at least 33% strong acid content when strong acid sites are defined as having a desorption temperature above 350°C (pp. 151,Table 3). However, the instantly claimed strong acid content of 18-28% is still obvious over Chen et al. Based on the trends in catalytic activity/selectivity disclosed by Chen et al. (pp. 152, right column, 1st paragraph), a person of ordinary skill in the art, at the relevant time, would have been motivated to produce a ZSM-23 zeolite with lower strong acid content than the most effective catalyst disclosed (SNNa, strong acid content of >33%) in order to improve the hydroisomerization selectivity, which is dependent on having a large number of weak and medium strength acid sites. See above the rejection of claim 1 under 25 USC 103 over Chen et al. Applicant argues that sine claims 2-4 are dependent from claim 1, they are not anticipated for the same reason. The examiner agrees with this finding. However, claims 2-4 are still obvious over Chen et al. for the reasons stated herein.
With regard to claims 5-7, 10-12, and 14-18, applicant argues that Wang et al. and CN ‘213A do not cure the deficiencies of the rejection of claim 1, and therefore the claims are allowable at least by virtue of their dependence on claim 1. As stated above, while the examiner agrees that Chen et al. does not anticipate claim 1 because it does not explicitly teach a ZSM-23 zeolite with a strong acid content of 18-28%, but claim 1 is still obvious over Chen et al. Therefore, claims 5-7, 10-12, and 14-18 are unpatentable over Chen et al. in view of Wang et al. and CN ‘213A.
With regard to claim 9, applicant argues that Wang et al. and CN ‘213A do not cure the deficiencies of the rejection of claim 1, and that neither Chen et al., Wang et al., or CN ‘213A teach the four sub-steps of the gelation step as instantly claimed. However, as noted above in the rejection of claim 9, CN ‘213A teaches acid-base neutralization to form a gel via introducing part of the silicon-containing material before and/or during the gelation process of the aluminum-containing material wherein CO2 is continuously added during the gelation step [0018], [0024]. Due to the continuous neutralization/addition of CO2, the process of CN ‘213A would necessarily lead to an addition of a silicon-containing material, an addition of CO2, a second addition of a silicon-containing material, and a second addition of CO2. Applicant has not argued a reason why it would be improper to combine the teachings of CN ‘213A with Chen et al. and Wang et al. to form the instantly claimed invention. Therefore, claim 9 is still considered obvious over Chen et al. in view of Wang et al. and CN ‘213A.
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 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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