DETAILED ACTION
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
Specification has been amended. Claims 1, and 9-10 have been amended. Claims 1-18 are pending in the instant application. Claims 5-15 remain withdrawn. Claims 1-4, and 16-18 are under examination on the merits.
Response to Amendment
The Amendment by Applicants’ representative Dr. Randolph E. Treece on 05/08/2026 has been entered.
Response to Arguments/Amendments
Claim rejection under 35 U.S.C.§112(a)
Applicant’s argument over rejection of claims 17-18 of the phrases “a crystallinity of greater than or equal to 120%” and “a crystallinity of greater than or equal to 140%” is on the ground that the crystallinity referred to in Claims 17 and 18 and in the specification of the present application is relative crystallinity. Paragraph [0037] of the specification of the present
application states that the crystallinity of the ZSM-35 molecular sieve is obtained by a common calculation method using the intensities of characteristic peaks at 23.3 24.5°, and 25.3° measured by an X-ray diffractometer. However, the specific measurement method discloses at pages 11-12 of the Remark including using the reference sample of a ZSM-35 molecular sieve reagent commercially available from Aladdin Industrial Corporation is not disclosed in the original disclosure (e.g., paragraph 37 of the present Specification). In addition, Applicant fails to explain how to calculate the crystallinity from the intensities of characteristic peaks at 23.3 24.5°, and 25.3° measured by an X-ray diffractometer, using an average intensity of all the peaks (23.3 24.5°, and 25.3°) or from a single peak thereof in order to achieve a crystallinity of greater than or equal to 120% or 140%. The statement and Appendix A should be filed in 132 Declaration because they were not described in the original disclosure, nor well-known to one ordinary skilled in the art. Therefore, the rejection is maintained.
Claim rejection under 35 U.S.C.§112(b)
For the same reason as articulated above under 112(a) rejection, the 112(b) rejection is also maintained. In addition, it seems that the term “crystallinity” actually should be “relative crystallinity” in light of Applicant’s response. However, the term “relative crystallinity” is not clearly defined in terms of how to measure it because Applicant fails to explain how to calculate the relative crystallinity from the intensities of characteristic peaks at 23.3 24.5°, and 25.3° measured by an X-ray diffractometer, using an average intensity of all the peaks (23.3 24.5°, and 25.3°) or from a single peak thereof? The rejection is maintained.
Claim rejection under 35 U.S.C.§103(a)
In terms of the distinguishing technical feature 1 (i.e., adding polyacrylamide to the mixed solution), Applicant argued the secondary reference Han et al. does not teach polyacrylamide(PAM) has an effect on the crystal size of ZSM-35 molecular sieve; and polyacrylamide in Claim 1 of the present application has the effect of improving the crystallinity of ZSM-35 molecular sieve, while Han et al. teaches that adding polyacrylamide will reduce the crystallinity of SAPO-34 molecular sieve.
Applicant’s argument is not persuasive. Han et al. teaches at appropriate low concentrations, PAM forms network nodes through the interaction of long-chain entanglement and hydrogen bonding, and its solution can be considered as a network structure. The surface (of the network structure) is rich in amide groups and has good combability with molecular sieve synthetic gels. Thus, the combination of space constraints and molecular interactions created by the polymer networks provides greater freedom in controlling zeolite formation and assembly. Accordingly, the synthesis of hollow ZSM-5 (Jiang et al., Microporous Mesoporous Mater., (2012), v.163, p11-20), zeolite A spheres and nanosized SAPO-34 using a cross-linked PAM hydrogel has been reported. See 2nd paragraph, left column at p.110676. It can be seen that Han’s teaching of using PAM in synthesis of zeolite does not limit to SAPO-34 molecular sieve, but also applies to synthesis of ZSM-5 and other zeolites because the combination of space constraints and molecular interactions created by the polymer networks provides greater freedom in controlling zeolite formation and assembly. In terms of motivation to combine the references of the `245 patent and Han et al., the Fed. Cir Court have repeatedly held that the motivation to modify a prior art reference to arrive at the claimed invention need not be the same motivation that the patentee had. The obviousness analysis cannot be confined by a formalistic conception of the words teaching, suggestion, and motivation, or by overemphasis on the importance of published articles and the explicit content of issued patents. Any motivation to combine references, whether articulated in the references themselves or supported by evidence of the knowledge of a skilled artisan, is sufficient to combine those references to arrive at the claimed process. Outdry Techs Corp. v. Geox S.P.A. 859 F.3d 1364, Fed. Cir. (2017) (123 USPQ2d starting 1141 at 1143-1144).
In terms of the distinguishing technical feature 2 (i.e., subjecting the feedstock solution to a two-stage crystallization at 140-160°C for 12-24 h and then a second stage crystallization at 120- 140°C for 48-72 h), Applicant argued the examiner’s statement (the `245 patent teaches the crystallization of zeolite molecular sieves at various temperatures and times, and the adjustment of particular conventional working conditions, such as reaction temperature, reaction time and use of solvents, rearranging steps in a reaction sequence, are deemed merely a matter of judicious selection and routine optimization which is well within the purview of the skilled artisan) is not supported by evidence.
Applicant’s argument is found not persuasive. The `245 patent teaches crystallizing the zeolite molecular sieves at various temperatures (from about 150 °F to about 400 °F) under various durations (from about 6 hours to about 100 days), see col. 4, lns. 60-66. Han et al. teaches crystallizing the zeolite molecular sieves at 200 °C for 24 h. In addition, Jiang et al. teaches preparation of hollow ZSM-5 crystals in the presence of polyacrylamide (PAM) by recrystallization at 120-180 °C for 144h, see “2.1. Synthesis”, left column at p.12). It is well known that the adjustment of particular conventional working conditions, such as reaction temperature, reaction time and use of solvents, rearranging steps in a reaction sequence, are deemed merely a matter of judicious selection and routine optimization which is well within the purview of the skilled artisan. See In re Mostovych, Weber, Mitchell and Aulbach, 144 USPQ 38. It would have been obvious for one ordinary skilled in the art to try different recrystallization temperature and duration with a predictable result. It is "Obvious to try" - choosing from a finite number of identified, predictable solutions, with a reasonable expectation of success.
Therefore, Applicant’s amendment and argument are not sufficient to overcome the rejection. The rejection is maintained.
The following rejection is necessitated by the amendment filed 05/08/2026.
Claim Rejections - 35 USC § 112
The following is a quotation of the first paragraph of 35 U.S.C. 112(a):
(a) IN GENERAL.—The specification shall contain a written description of the invention, and of the manner and process of making and using it, in such full, clear, concise, and exact terms as to enable any person skilled in the art to which it pertains, or with which it is most nearly connected, to make and use the same, and shall set forth the best mode contemplated by the inventor or joint inventor of carrying out the invention.
Claims 17 and 18 are rejected under 35 U.S.C. 112, first paragraph, as failing to comply with the written description requirement. The claim(s) contains subject matter which was not described in the specification in such a way as to reasonably convey to one skilled in the relevant art that the inventor(s), at the time the application was filed, had possession of the claimed invention.
Claims 17 and 18 are drawn to a method for producing a ZSM-35 molecular sieve wherein the ZSM-35 molecular sieve has a crystallinity of greater than or equal to 120% according to claim 17, and a crystallinity of greater than or equal to 140%. By definition, “crystallinity” of a molecular sieve refers to the degree of structural order, periodicity, and packing density of atoms or molecules within a solid material. It measures the fraction of a material structured in a highly ordered, repeating crystal lattice versus disordered amorphous regions. According to Google search, a value of crystallinity exceeding 100% (e.g., 140%) is not physically possible in terms of total material composition, unless a “relative crystallinity”. This conclusion is further supported by Yuan et al., “1.3 Crystallinity”, Comprehensive Analytical Chemistry, (2023), V.100, Ch. 6, p.120-121, which states commercial plastics almost do not reach 100% crystallinity.
In addition, Applicant’s specification does not define the phrases “a crystallinity of greater than or equal to 120%” and “a crystallinity of greater than or equal to 140%”. Instead, specification [0037] describes “The crystallinity was obtained using the measurements of intensities of characteristic peaks (9.4°, 22.4°, 22.7°, 23.3°, 23.7°, 24.5°, 25.3°) by a common calculation method”. However, said “common calculation method” is not described in the specification. Therefore, the specification fails to comply with the written description requirement.
As stated in the Fed. Cir. Court decision regarding written description requirement, the hallmark of written description is disclosure. Thus, “possession as shown in the disclosure” is a more complete formulation. Yet whatever the specific articulation, the test requires an objective inquiry into the four corners of the specification from the perspective of a person of ordinary skill in the art. Based on that inquiry, the specification must describe an invention understandable to that skilled artisan and show that the inventor actually invented the invention claimed.” Ariad Pharmaceuticals Inc. v. Eli Lilly &Co. (C.A.F.C.), 1172, 94 USPQ2d 1161, 598 F3d 1336 (2010).
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.
Claims 17 and 18 are 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 pre-AIA the applicant regards as the invention.
Specifically, the phrases “a crystallinity of greater than or equal to 120%” and “a crystallinity of greater than or equal to 140%” are not defined nor clearly described in the specification, because the common calculation method cited in paragraph [0037] of the specification is not specified. Therefore, claims 17 and 18 are indefinite.
Claim Rejections - 35 USC § 103(a) (revised)
In the event the determination of the status of the application as subject to AIA 35 U.S.C. 102 and 103 (or as subject to pre-AIA 35 U.S.C. 102 and 103) is incorrect, any correction of the statutory basis for the rejection will not be considered a new ground of rejection if the prior art relied upon, and the rationale supporting the rejection, would be the same under either status.
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 of this title, 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 set forth in Graham v. John Deere Co., 383 U.S. 1, 148 USPQ 459 (1966), that are applied 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.
Claims 1-4 and 16-18 are rejected under 35 U.S.C. 103 as being unpatentable over US4016245 (“the `245 patent”) to Plank et al. in view of Han et al., Microporous and Mesoporous Materials, (2021), v.311, p.110676 (Pub. 6 Oct. 2020), Jiang et al., Microporous Mesoporous Mater., (2012), v.163, p11-20, and Xu et al., Molecules, (2020), v.25, p.3722 (1-18).
Applicant’s claim 1 is drawn to a method for producing a ZSM-35 molecular sieve, comprising: mixing a silicon source, an aluminum source, an alkali, and a template agent with water to form a mixed solution, adding polyacrylamide to the mixed solution to form a feedstock solution, and subjecting the feedstock solution to a first stage crystallization at 140-160°C for 12-24 h and then subjecting the feedstock solution to a second stage crystallization at 120- 140°C for 48-72 h, wherein the temperature of the first stage crystallization is higher than that of the second stage crystallization, to obtain the ZSM-35 molecular sieve, wherein the template agent comprises pyrrolidine.
Determination of the scope and content of the prior art (MPEP §2141.01)
The `245 patent (Abstract and claim 10) discloses a method for preparing the crystalline aluminosilicate zeolite ZSM-35 molecular sieve comprises preparing a mixture containing sources of an alkali metal oxide, an organic nitrogen-containing oxide, an oxide of aluminum, an oxide of silicon and water and having a composition, in terms of mole ratios of oxides, falling within the following ranges: R+/M+= 0.2-1.0; OH-/SiO2=0.05-0.5; H2O/OH-=41-500; and SiO2/Al2O3=8.8-200, and maintaining the mixture at the temperature between about 150° F (66° C) and 400° F (204° C), wherein R is pyrrolidine, and M is an alkali metal ion. In addition, the `245 patent (EXAMPLES 1-25) discloses specific methods for preparing the crystalline aluminosilicate zeolite comprises preparing a mixture containing an aluminum source of sodium aluminate, an alkali of NaOH, a silicon source of colloidal silica, and a template agent of pyrrolidine with water to form a mixed solution. The mixed solution was heated at 276° F (131° C) for 17 days (EXAMPLE 1); 210° F (99° C) for 62 days (EXAMPLE 2); or exchanged with NH4Cl and dried at 230° F (110° C) for 16 hours and calcined at 1000° F for 10 hours (EXAMPLE 3).
Ascertainment of the difference between the prior art and the claims (MPEP §2141.02)
The difference between Applicant’s claim 1 and the `245 patent is that the prior art does not teaches adding polyacrylamide to the mixed solution to form a feedstock solution, and the two-stage of crystallizing the feedstock solution at 140-160°C for 12-24 h and then at 120-140°C for 48-72 h to obtain the ZSM-35 molecular sieve.
Finding of prima facie obviousness--rational and motivation (MPEP §2142-2413)
However, the differences are further taught and/or suggested by Han et al. and Jiang et al. Han et al. teaches using polyacrylamide in polyacrylamide-assisted synthesis of hierarchical porous zeolite, as well as synthesis of molecular sieves including hollow ZSM-5 (see left column at p.110676-2) to make better performed hierarchical porous zeolite. One ordinary skilled in the art would have been motivated to further include polyacrylamide for synthesis of the crystal molecular sieves with better performance, wherein Jiang et al. was cited, which teaches preparation of hollow ZSM-5 crystals in the presence of polyacrylamide (PAM) by recrystallization at 120-180 °C for 144h, see “2.1. Synthesis”, left column at p.12).
In terms of the two-stage temperature of crystallizing the feedstock solution at 140-160°C for 12-24 h and then at 120-140°C for 48- 72 h at two-stage process to obtain the ZSM-35 molecular sieve, the `245 patent teaches crystallizing the zeolite molecular sieves at various temperatures (from about 150 °F to about 400 °F) under various durations (from about 6 hours to about 100 days), see col. 4, lns. 60-66. Han et al. teaches crystallizing the zeolite molecular sieves at 200 °C for 24 h. In addition, Jiang et al. teaches preparation of hollow ZSM-5 crystals in the presence of polyacrylamide (PAM) by recrystallization at 120-180 °C for 144h, see “2.1. Synthesis”, left column at p.12). The references teach recrystallization at various temperatures under various durations related to the two-stage crystallization process. It is well known that the adjustment of particular conventional working conditions, such as reaction temperature, reaction time and use of solvents, rearranging steps in a reaction sequence, are deemed merely a matter of judicious selection and routine optimization which is well within the purview of the skilled artisan. See In re Mostovych, Weber, Mitchell and Aulbach, 144 USPQ 38. It would have been obvious for one ordinary skilled in the art to try different recrystallization temperature and duration with a predictable result. It is "Obvious to try" - choosing from a finite number of identified, predictable solutions, with a reasonable expectation of success. The rationale to support a conclusion that the claim would have been obvious is that "a person of ordinary skill has good reason to pursue the known options within his or her technical grasp. If this leads to the anticipated success, it is likely that product [was] not of innovation but of ordinary skill and common sense. In that instance the fact that a combination was obvious to try might show that it was obvious under § 103."KSR, 550 U.S. at ___, 82 USPQ2d at 1397. Therefore, in looking at the instant claimed formulation as a whole, the claimed process would have been suggested to one skilled in the art and therefore, is obvious, absent evidence to the contrary. Therefore, the `245 patent in view of Han et al. and Jiang et al. would have rendered claims 1-3 and 16 obvious.
In terms of claim 4, wherein the polyacrylamide has a weight- average molecular weight of 3 million -10 million, Han et al. teaches the molecular weights and content of PAM (polyacrylamide) were above 6 million (see “2.1. Materials” at p.2).
In terms of claim 17, wherein the ZSM-35 molecular sieve is lamellar crystal, and has a grain thickness of less than or equal to 50 nm, a grain length and/or the grain width of less than or equal to 500 nm, and a crystallinity of greater than or equal to 120%, Xu et al. discloses the synthesis of aluminosilicate FER zeolite (namely ZSM-35) through various routes using different organic templates including pyrrolidine (THP) (see Table 1 at p.3722 (2), and Table 2 at p. p.3722 (4)). Xu et al. further discloses the synthesized aluminosilicate FER zeolite is the nanosheet-like FER zeolite (i.e., lamellar crystal) with the thickness at 6-8 nm (see p.3722 (5)). Xu et al. also discloses synthesis of hierarchically porous aluminosilicate FER zeolite consisted of the agglomerated sheets (~9-15 nm thickness) (see Figure 4 at p.3722 (8)); or 6-8 nm and 6-200 nm thickness (see Figure 5 at p.3722 (9). In terms of the limitation “a crystallinity of greater than or equal to 120%”, Xu et al. discloses the hierarchically aluminosilicate FER zeolites are crystals.
In terms of claim 18, wherein the ZSM-35 molecular sieve has a grain thickness of less than 50 nm, a grain length and/or width of less than or equal to 200 nm, and a crystallinity of greater than or equal to 140%, Xu et al. discloses the synthesis of aluminosilicate FER zeolite (namely ZSM-35) through various routes using different organic templates including pyrrolidine (THP) (see Table 1 at p.3722 (2), and Table 2 at p. p.3722 (4)). Xu et al. further discloses the synthesized aluminosilicate FER zeolite is the nanosheet-like FER zeolite (i.e., lamellar crystal) with the thickness at 6-8 nm (see p.3722 (5)). Xu et al. also discloses synthesis of hierarchically porous aluminosilicate FER zeolite consisted of the agglomerated sheets (~9-15 nm thickness) (see Figure 4 at p.3722 (8)); or 6-8 nm and 6-200 nm thickness (see Figure 5 at p.3722 (9). In terms of the limitation “a crystallinity of greater than or equal to 140%”, Xu et al. discloses the hierarchically aluminosilicate FER zeolites are crystals.
Conclusions
Claims 1-4 and 16-18 are rejected.
Claims 5-15 are withdrawn.
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 extension fee 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 date of this final action.
Telephone Inquiry
Any inquiry concerning this communication or earlier communications from the examiner should be directed to Yong L. Chu, whose telephone number is (571)272-5759. The examiner can normally be reached on M-F 8:30am-5:00pm.
If attempts to reach the examiner by telephone are unsuccessful, the examiner’s supervisor, Amber R. Orlando can be reached on 571-270-3149. The fax phone number for the organization where this application or proceeding is assigned is (571) 273-8300.
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/YONG L CHU/Primary Examiner, Art Unit 1731