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
Herein claims 1-22 are pending. Claim 1 is amended, claims 21 and 22 are newly added, and claims 2-20 are as originally presented.
Information Disclosure Statement
The information disclosure statement (IDS) filed on 21 September 2026 has been reviewed and considered by the examiner.
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 1-8, 15, 17-19 and 21-22 are rejected under 35 U.S.C. 103 as being unpatentable over Xue et al. (US20240076193, English equivalent of CN11473516A, published 12 July 2022) in view of Pour et al. (Journal of Inorganic and Organometallic Polymers and Materials 2021, 31, pp. 2501-2510).
With regard to claim 1, Xue et al. teaches a method of producing zeolite-Y particles by:
Mixing an aluminum source, a silicon source, and sodium hydroxide in distilled water in a molar ratio of 7-14 Na2O : 1 Al2O3 : 20-33 SiO2 : 300-650 H2O and heat treating the mixture under continuous stirring at 70-100°C for 4-12 h [0028] & [0033];
Mixing the first mixture with an aluminum source and an alkali silicon source to form a sol with a molar ratio of 17-26 Na2O : 1 Al2O3 : 13-19 SiO2 : 400-550 H2O and heat treating the second mixture at 40-70°C for 15-41 h [0029] & [0036];
Mixing the second mixture with an aluminum source and an alkali silicon source to form a sol with a molar ratio of 12-20 Na2O : 1 Al2O3 : 14-20 SiO2 : 550-1050 H2O, heat treating the mixture at 80-105°C for 6-13 h, and filtering, washing, and drying the solid product to yield zeolite-Y particles [0030] & [0041].
Xue et al. is a three-step process being applied to the instantly claimed two-step process. For clarity, step 1 of Xue et al. is being interpreted to read as the formation of an initial zeolite precursor solution comprising initial alumina and silica source materials (lines 2-6), and step 3 of Xue et al. is being interpreted to read as the limitations of adding additional alumina source material to the intermediate mixture and heating of the intermediate mixture to form zeolite-Y particles (lines 7-10). Step 2, concerning the transformation of directing agent A from step (1) into directing agent B, is interpreted as additional processing of the intermediate mixture as instantly claimed.
Xue et al. does not teach that the initial zeolite precursor solution (indicated as step 1 above) has a silica-alumina molar ratio of between 8 and 16 as instantly claimed.
However, Pour et al. teaches the use of an initial gel composition for the template free synthesis of zeolite Y with the ratios 3.2-11.0 Na2O : 1 Al2O3 : 10 SiO2 : 205 H2O, which is within the instantly claimed silica alumina ratio of 8-16. Pour et al. teaches that the initial gel composition has a strong influence on template-free synthesis of zeolite Y (pp. 2501, right col., lines 7-12). The gel compositions employed by Pour et al. achieve, at similar crystallization temperatures and times proposed by Xue et al., higher relative crystallinity (75-90% in Xue et al. [0017], 80% to >100% in Pour et al. Fig. 4, Fig. 6). While Pour et al. uses one heat treatment as opposed to Xue et al.’s two (see Comparative Examples) or three heat treatments [0028]-[0043], Pour et al. observes that crystallization happens in two distinct steps: formation of nucleation centers (same as observed in step (1) of Xue et al.) and crystal growth (seen in steps (2) and (3) of Xue et al.; pp. 2506, left col., lines 1-2). As such, Pour et al.’s findings regarding gel composition are still relevant to the synthesis of Xue et al. due to the overlapping processes occurring in both. Therefore, a person of ordinary skill in the art would have found it obvious to modify the initial gel composition of Xue et al. by instead using the gel molar ratios taught by Pour et al., which read to the instantly claimed SAR of 8-16, in order to achieve higher crystallinity in the produced zeolite Y particles.
With regard to claim 2, Xue et al. teaches that the initial alumina source material may be sodium metaaluminate (NaAlO2) as instantly claimed ([0028] & see defined aluminum sources in [0025]).
With regard to claim 3, Xue et al. teaches that the additional alumina source material (e.g. those
used in steps 2 & 3) may be sodium metaaluminate (NaAlO2) as instantly claimed ([0029], [0030], & see
defined aluminum sources in [0025]).
With regard to claim 4, Xue et al. teaches that the additional alumina source material may have the same composition as the initial alumina source (see that steps (1), (2), & (3) use sodium aluminate as an example alumina source; [0028]-[0030]).
With regard to claim 5, Xue et al. teaches that the alumina source used in the method may be
multiple distinct materials [0025] and may be different between steps (pp. 8, claim 37).
With regard to claim 6, the method taught by Xue et al. does not utilize an organic structure-
directing agent [0028]-[0030].
With regard to claim 7, Xue et al. teaches that the thermal treatment in step (1), which reads to the heating of the initial zeolite precursor solution, is carried out at 70-100°C for 4-12 h [0033]. The endpoints of both the taught range of temperature and time overlap the instantly claimed ranges of 50-70°C and 12-24 h. It would have been obvious to one of ordinary skill in the art at the time invention was made to have selected the overlapping portions of the ranges of treatment temperature and time disclosed by the reference because overlapping ranges have been held to be a prima facie case of obviousness. In re Malagari, 182 USPQ. See also MPEP 2144.05.I.
With regard to claim 8, Xue et al. teaches that the thermal treatment in step (3), which reads to
the heating of the intermediate mixture, is caried out at temperatures between 80-105°C and a time of
6-13 h. The taught range of temperature overlaps the instantly claimed range of 80-120°C and the
endpoint of the range for time overlaps the instantly claimed range of 12-24 hours. It would have been
obvious to one of ordinary skill in the art at the time invention was made to have selected the
overlapping portions of the ranges of treatment temperature and time disclosed by the reference
because overlapping ranges have been held to be a prima facie case of obviousness. In re Malagari, 182
USPQ. See also MPEP 21244.05.I. Furthermore, Pour et al. teaches that the optimal crystallization time for achieving high purity and highly crystalline zeolite Y particles is around 90°C, which is within both the range taught by Xue et al. and instantly claimed temperature range. Therefore, it would have been additionally obvious to a person of ordinary skill in the art, in view of Pour et al., to select a crystallization temperature for the final heat treatment of Xue et al.’s process, wherein the bulk of crystallinity is formed, of 90-95°C as taught by Pour et al. to achieve high crystallinity and sample purity (see Pour et al. pp. 2503-2504, Section 3.2).
With regard to claim 15, Xue et al. teaches in Comparative Example 1 a method of forming zeolite-Y particles comprising preparing a solution of sodium aluminate, silica, and sodium hydroxide in water; a first hydrothermal treatment for 5 h at 80°C; adding alkali/silica and sodium aluminate solutions; a second hydrothermal treatment for 13 h at 90°C, and filtering and drying the zeolite-Y particles which reads to the process steps recited in claim 1 ([0085], see referenced steps (2) and (3) of [0082]-[0084]).
The zeolite-Y particles of Comparative example 1 are reported to have a grain distribution (i.e. particle diameter/size) of 180-350 nm. While the average grain size is not reported, the average grain size must be between 180-350 nm. It would have been obvious to one of ordinary skill within the art at the time to optimize the conditions (time, temperature, or alkalinity) taught in order to form a product with an average particle/grain size between 150-280 nm, especially within the overlapping portion of the taught and claimed ranges (180-280 nm). It would have been obvious to one having ordinary skill in the art at the time the invention was made to arrive at the reaction conditions which result in the instantly claimed average particle size of the produced zeolite-Y particles 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 to reach a desired outcome involves only routine skill
in the art. See In re Boesch, 205 USPQ 215.
With regard to claim 17, Xue et al. teaches that the formed zeolite-Y particles may have a pore volume greater than 0.36 mL/g, and preferably between 0.38 and 0.56 mL/g [0015]. The taught range overlaps the instantly claimed pore volume range of 0.45-0.7 mL/g. 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.
With regard to claim 18, Xue et al. teaches that the zeolite-Y particles formed have a specific surface area of 800-950 m2/g, which is at least 600 m2/g as instantly claimed [0012].
With regard to claim 19, Xue et al. teaches that the zeolite-Y particles preferably have a crystallinity of 83-88% after ammonium ion exchange, which is greater than 75% as instantly claimed [0017].
With regard to claim 21, Xue et al. does not teach a molar ratio of the components in the initial zeolite precursor is 8-12 Na2O : 1 Al2O3 : 8-16 SiO2 : 200-400 H2O. However, Pour et al. teaches the use of an initial gel composition for the template free synthesis of zeolite Y with the ratios 3.2-11.0 Na2O : 1 Al2O3 : 10 SiO2 : 205 H2O (pp. 2502, left col., lines 16-19), and teaches that the overall optimal ratio of Na2O to Al2O3 is 8.8 with respect to crystallization time, which is within the instantly claimed range of 8-12 Na2O : Al2O3. The value 8.8 was selected for further optimization by Pour et al. because, while a ratio of 7 resulted in the highest purity amongst the range of ratios (see Fig. 4, Na2O =7 yielded 100% zeolite Y while Na2O = 8.8 yielded ~80%), increased Na2O in the initial gel composition enhanced the rate of crystallization during the induction time, which is the formation of nucleation centers (pp. 2507, left col., lines 14-23). Therefore, in the initial gel composition of Xue et al. (step (1), which is then subjected to a hydrothermal treatment to form nucleation centers), the modification in gel composition suggested by Pour et al. would have the positive effect of decreasing the required treatment time. Therefore, a person of ordinary skill in the art would have found it obvious to modify the process taught by Xue et al. by using the gel molar ratio taught by Pour et al. in order to conduct step (1) faster in addition to the reasons cited in the rejection of claim 1.
With regard to claim 22, Xue et al. does not teach a molar ratio of the components in the intermediate zeolite precursor is 8-12 Na2O : 1 Al2O3 : 8-16 SiO2 : 200-400 H2O. However, Pour et al. teaches the use of an gel composition for the template free synthesis of zeolite Y with the ratios 3.2-11.0 Na2O : 1 Al2O3 : 10 SiO2 : 205 H2O (pp. 2502, left col., lines 16-19), and teaches that the overall optimal ratio of Na2O to Al2O3 is 8.8 with respect to crystallization time, which is within the instantly claimed range of 8-12 Na2O : Al2O3. Pour et al. teaches that increasing the ratio of Na2O : Al2O3 from 7 to 8.8 increased the rate of the transition step and crystal growth (pp. 2507, left col., lines 14-23), the two processes in which the final zeolite Y framework is formed. Furthermore, Pour et al. teaches that increased Na2O in the gel composition resulted in higher surface areas and pore volume of the prepared zeolite Y particles (pp. 2507, right col., lines 19-23). The observations regarding gel composition and characteristics of the crystallization process and final physical properties are relevant to the intermediate mixture of Xue et al., step (3), because the subsequent hydrothermal treatment is the point at which the majority of the precursor reagents are converted from amorphous gel to crystallized zeolite Y (see crystallinity measurements of steps (1)-(3) in [0028], [0029], [0030]). Therefore, it would have been obvious to one of ordinary skill in the art, to modify the teachings of Xue et al. to utilize a gel composition of 8.8 Na2O : 1 Al2O3 : 10 SiO2 : 205 H2O, as suggested by Pour et al., in the intermediate mixture of step (3) to increase the rate of crystallization (phase transition/crystal growth) and improve the observed surface area/ pore volume of the final zeolite Y particles.
Claims 9-14 and 20 are rejected under 35 U.S.C. 103 as being unpatentable over Xue et al. and Pour et al. as applied to claim 1 above, and further in view of Zhu et al. (Adv. Mater. 2020, 32, 2000272).
With regard to claim 9, Xue et al. teaches that the initial zeolite precursor solution is formed by dissolving an aluminum source, a silicon source, and a basic compound (i.e. sodium hydroxide) into a solvent (distilled water) as instantly claimed [0028]. Xue et al. does not teach that the mixture is aged by stirring for at least 10 hours prior to a heat treatment (i.e. constant temperature crystallization, [0028]).
However, Pour et al. teaches aging the initial solution of an aluminum source, a silicon source, and a basic compound for 24 h prior to crystallization (pp. 2502, left col., lines 18-20). Pour et al. teaches that aging prior to hydrothermal treatment can help to orient the crystallization towards the desired structure and morphology (pp. 2503, right col., lines 4-6). In turn, an aging period before hydrothermal treatment/crystallization can improve sample purity and reduce crystallinity defects in the form of zeolite P impurities (pp. 2503, right col., lines 2-4). Therefore, it would have been obvious to a person of ordinary skill in the art to modify the synthesis process of Xue et al. to include an aging period of 24 h as taught by Pour et al., which is within the instantly claimed range of >10 h, in order to improve early structural arrangement of the zeolite Y framework and increase sample purity/crystallinity in the final zeolite Y particles.
Neither Xue et al. nor Pour et al. teach that the mixture, during aging, is stirred. However, stirring the mixture of reagents during the aging process is also routine in the art. Zhu et al. in
their procedures for producing zeolite-Y particles, age a reaction mixture of sodium aluminate, silica gel,
NaOH, TBAOH, and zeolite nuclei for 2 h with stirring (e.g. strong agitation) at 25°C (Supporting
Information, first paragraph, pp. 3). Stirring or agitation of the reaction solution allows the reaction
mixture to remain homogenous, which is advantageous for providing energy to the reaction and
supporting mass transport. Therefore, it would have been obvious to one of ordinary skill in the art to
adopt an aging step involving stirring the mixture for at least 10 h, based on the combined teachings
of Pour et al. and Zhu et al., as the conditions for preparing zeolite-Y particles as the general
conditions were known in the prior art, common practice, and improved the quality of the reaction.
With regard to claim 10, Xue et al. teaches that water is used as the solvent for the initial zeolite
precursor solution [0028].
With regard to claim 11, Xue et al. does not teach that an aging period of 10 or more hours was conducted at 20-40°C. However, Pour et al. teaches an aging period after mixing the gel composition and before hydrothermal treatment as noted above (pp. 2502, left col., lines 14-25). Pour et al. teaches that the optimal aging temperature for the formation of pure-phase zeolite-Y particles is 27°C (pp. 2509, left col., lines 19-22). At lower the lower temperatures tested, 15°C and 4°C, the competing phase of zeolite P was formed, which reduced purity and overall crystallinity due to defects in the framework (complete formation of zeolite P at 4°C, mixed phase Y/P at 5°C, pp. 2503, left col., line 22 – right col., line 5). Therefore, in applying the aging period taught by Pour et al. to the process of Xue et al. for the reasons noted above with respect to claim 9, it would have been obvious to a person of ordinary skill in the art to select 27°C, which is within the instantly claimed temperature range of 20-40°C, as the aging temperature in order to form a pure zeolite Y phase in the final particles.
With regard to claim 12, Xue et al. does not teach that an aging period was conducted for 10-30 hours. However, Pour et al. teaches an aging period of 24 h after mixing the gel composition and before hydrothermal treatment as noted above (pp. 2502, left col., lines 14-25). In applying the aging period of Pour et al. for the reasons noted above with respect to claim 9, it would have been obvious to a person of ordinary skill in the art to, in the absence of any contrary teachings, to adopt the same aging period of 24 hours.
In regard to claim 13, Xue et al. teaches that the basic compound used to produce the zeolite
precursor solution is sodium hydroxide/NaOH [0028].
In regard to claim 14, Xue et al. teaches that a certain amount of additional alumina (e.g. an
aluminum source) is added to the initial reaction mixture (e.g. directing agent A obtained in step (1)) in
order to meet a specific ratio of silica:alumina:water. Therefore, the amount of additional alumina
added may be the same or different from the amount of alumina source material used to form the initial
precursor mixture.
In regard to claim 20, Xue et al. teaches that the method of making zeolite-Y particles includes
washing and drying the particles [0030]. Xue et al. does not teach that the method to form
zeolite-Y particles comprising the step of calcining the particles.
However, calcination of zeolite-Y particles is a routine procedure in the art and is often utilized to remove template agents or extraneous reagents or affect a structural change to a zeolite framework. Zhu et al. teaches that zeolite-Y samples were calcined at 500°C as a final step in the synthetic process (Supporting Information, pp. 3, first paragraph). In the case of Zhu et al., a calcination step is included to remove an organic template agent. A person of ordinary skill in the art at the relevant time would be capable of implementing a calcination step in the method as instantly claimed in order to enact a structural change or remove an organic material added to the zeolite mixture during the synthesis process.
Claim 16 is rejected under 35 U.S.C. 103 as being unpatentable over Xue et. al. and Pour et al. as applied to claim 1 above, and further in view of Ding et al. (US20180334390A1, published 22 November 2018).
With regard to claim 16, Xue et al. is silent on the average pore size of the zeolite-Y particles produced by the taught method. However, Ding et al. teaches that a mesoporous zeolite Y have an average pore size of 2-50 nm and specifically cites 2-5 nm as a favorable range ([0027], see Table 4B for an example with an average pore size of 4.6 nm). Ding et al. further teaches that for Y-type zeolites used as hydrocracking catalysts, the pore size of the particles impacts the efficacy of the reaction due to the inability of large reactants to travel through micropores to catalytic active sites [0007], [0031]. The inclusion of mesopores (d > 2 nm) has been utilized to solve this issue [0008]. However, if pores are too large, the crystal lattice of the zeolite structure may be compromised or less resilient under high temperatures. Therefore, it would have been obvious to one of ordinary skill in the art at the relevant time to select a method which results in zeolite-Y particles with an average pore size of 2-5 nm, as taught by Ding et al., to improve the catalytic properties of the zeolite-Y particles produced without introducing major structural flaws.
Response to Arguments
Applicant’s arguments, see pp. 6, filed 08/04/2026, with respect to the rejection(s) of claim(s) 1-6 and 18-19 under 35 USC § 102(a)(1) have been fully considered and are persuasive. The examiner agrees with the assertion that the primary reference, Xue et al., does not teach the amended claim limitation of, “a molar ratio of Al2O3 to SiO2 in the initial zeolite precursor is of from 1:16 to 1:8,” and the previously cited secondary references do not render said limitation obvious. Therefore, the rejection under 35 USC § 102(a)(1) has been withdrawn. However, upon further consideration, a new ground(s) of rejection is made in view of Xue et al. and Pour et al., see above.
In addition, applicant’s arguments, see pp. 7, filed 08/04/2026, with respect to newly added claims 21 and 22 have been fully considered. As noted above, a new ground(s) of rejection with respect to claims 1, 21, and 22 is made in view of Xue et al. and Pour et al.
Conclusion
The prior art made of record and not relied upon is considered pertinent to applicant's disclosure:
Chinese Patent Application No. CN107089668A, for teaching a 3-type addition and crystallization method of synthesizing zeolite-Y particles without an organic structure-directing agent with gel compositions that encompass the instantly claimed ratios.
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
