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 .
DETAILED ACTION
Claims 2, 5-15, 23-25, 27-29, and 31-36 of R. Parsapur et al., US 18/151,782 (Jul. 5, 2022) are pending and under examination on the merits. Claims 2, 5-15, 24, 25, 27-29, and 33-36 are rejected. Claims 23, 31, and 32 are objectionable.
Claim Interpretation
Examination requires claim terms first be construed in terms in the broadest reasonable manner during prosecution as is reasonably allowed in an effort to establish a clear record of what applicant intends to claim See MPEP § 2111. Claim interpretation is modified in this Office action over the previous in view of Applicant’s amendments.
Summary of the Claimed Invention
Independent claim 2 recites as follows:
2. A method for synthesis of hierarchically ordered crystalline microporous material having mesoporous ordering, the method comprising:
forming an aqueous suspension of an effective amount of a parent crystalline microporous material having an underlying microporous structure,
an effective amount of an alkaline reagent and
an effective amount of a supramolecular template,
wherein the underlying microporous structure of the parent crystalline microporous material is characterized by pore-channels, cavities or window openings having a pore dimension,
further wherein if the crystalline microporous material is characterized by pore-channels, cavities or window openings of various dimensions, the pore dimension is the largest of the pore-channels, cavities or window openings of various dimensions;
wherein the supramolecular template is a bulky surfactant that possesses a dimension that constrains diffusion into the parent crystalline microporous material pore-channels, cavities or window openings having the pore dimension, and comprises one or more of:
a quaternary ammonium moiety and a constituent group selected from the group consisting of organosilanes, hydroxysilyls, alkoxysilyls, aromatics, branched alkyls, sulfonates, carboxylates, phosphates and combinations comprising one of the foregoing constituent groups;
a quaternary phosphonium moiety and a constituent group selected from the group consisting of organosilanes, hydroxysilyls, alkoxysilyls, aromatics, branched alkyls, sulfonates, carboxylates, phosphates and combinations comprising one of the foregoing constituent groups; or
two quaternary ammonium groups with an alkyl group bridging the quaternary ammonium groups containing 1-10 carbon atoms; and
hydrothermally treating the aqueous suspension under conditions effective for mesophase transition to dissolve/incise parent crystalline microporous material into oligomeric units of the parent crystalline microporous material, and then form a solid hierarchically ordered mesostructured having mesoporous order.
The specification teaches that the well-defined microporous structure of zeolites, where the molecular sized pore channels geometrically discriminate guest molecules, provides important, industrially desirable physicochemical functionalities. Specification at page 4, [0008]. The specification teaches, however, that the narrowness of micropores (micropores < 2 nm)1 can result in poor mass-transfer properties. Id. In this regard, the specification teaches that hierarchically ordered zeolites (HOZs) possessing an ordered mesoporous structure and zeolitized mesopore walls are advantageous over traditional microporous zeolites, for example in overcoming steric limitations. Id. Specification at page 4, [0009].
With reference to specification Figs. 1 and 2, the specification teaches that (per claim 2) hydrothermally treating an aqueous suspension of a parent crystalline microporous material (CMM) (10), an alkaline reagent and a supramolecular template (14) first causes the parent CMM to break into oligomeric CMM units (12) and the supramolecular template (14) forms into shaped micelles (16). Specification at pages 28-29, [0067]. The formed oligomeric CMM units can then hierarchically reassemble and crystallize around the shaped micelles to form an ordered mesostructure, HOCMM (18), having mesopores (20) of defined symmetry and mesopore walls formed of the oligomeric CMM units thereby retaining micropores (22) of the parent CMM. Specification at pages 28-29, [0067].
With reference to specification Fig. 1, claim 2 is schematically summarized by the Examiner as follows:
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Specification Working Examples
The specification discloses working examples at pages 44-63. Specification working Example 1A (alternate procedure) is summarized below. Specification at page 46, [0094].
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Specification at page 46, [0094]. With regard to Example 1A, the specification teaches that:
The AH-CT synthesized in accordance this procedure exhibits disordered mesoporosity, and is characterized in FIGs. 3A-4B, with an SEM image presented in FIG. 6 and structural and textural properties provided in Table 3.
Specification at page 46, [0094] (emphasis added). The specification further states the following regarding Example 1A:
For instance, in the examples herein, FAU zeolite is used; when the supramolecular template material was [cetyltrimethylammonium bromide (CTAB)] (~0.25 nm), [hierarchically ordered crystalline microporous materials] HOCMMs were not realized;
however, when the supramolecular template was an organosilane ( ~0.7 nm), HOCMMs were realized, as these are closer in dimension to the pore dimensions for FAU zeolite and therefore are constrained from entering such pores.
Specification at page 27, [0064] (emphasis added).
Specification working Example 1B (clearly an embodiment of the instant claims) is summarized below.
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Specification at pages 46-47, [0095]. Specification working Example 1B employs dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium chloride (DOAC) as the supramolecular template rather than the cetyltrimethylammonium bromide of Example 1A.
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All of the subsequent specification working Examples (i.e., Examples 1C-3B) are performed in a similar manner with zeolite H-Y as the parent crystalline microporous material and dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium chloride as the supramolecular template with variation of the base (either ammonium hydroxide or urea) and/or other parameters.
In sum, the working Examples are limited to only one or two species supramolecular template (i.e., dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium chloride and cetyltrimethyl ammonium bromide (CTAB)) and one species of “a parent crystalline microporous material having an underlying microporous structure”. i.e., zeolite Y.
Interpretation of “hierarchically ordered crystalline microporous material”
The claim 2 preamble recites the following bolded structural element:
2. A method for synthesis of hierarchically ordered crystalline microporous material having mesoporous ordering, the method comprising . . .
The specification does not give a closed-ended definition of “hierarchically ordered crystalline microporous material having mesoporous ordering”. See e.g., specification at page 4, [0008] et seq; Specification at page 12, [0042]. The specification does not provide a specific size definition for “mesopores” or “micropore”.
The art teaches that hierarchical porosity materials comprise interconnecting pores of more than one size regime. H. Zhang et al., 16 Chem. Mater., 4245-4256 (2004) (page 4245, col. 2); W. Cho et al., 18 Journal of Materials Chemistry, 4971-4976 (2008).
Qu teaches that according to the definition of the International Union of Pure and Applied Chemistry (IUPAC), porous materials can be classified into three categories according to their pore size: micropores (< 2 nm), mesopores (2–50 nm), and macropores (> 50 nm). H. Que et al., 3 Emergent Materials, 381-405 (2020) (page 381, col. 1). Qu teaches that in the process of synthesizing hierarchical zeolites, many surfactant molecules and polymers are used as mesoporous templating agents for the construction of mesoporous structures. Qu at page 226, col. 1. Qu states, however, in these hierarchical zeolites, mesopores are randomly distributed throughout the zeolite crystals and not ordered. Qu at page 226, col. 1. Qu teaches that the preparation of ordered mesoporous zeolites is of great significance in guiding the construction of pore structures in zeolite materials. Qu at page 226, col. 1. Qu recognizes the need in the art for mesoporous ordering in zeolites. Fig. 1 of K. Egeblad et al., 20 Chemistry of Materials, 946-960 (2008) aides in understanding zeolite hierarchical structures with respect to mesopores and micropores. Egeblad at page 948, Fig. 1.
In view of the foregoing, the claim term “hierarchically ordered crystalline microporous material having mesoporous ordering” is broadly and reasonably interpreted, consistently with the specification, as porous materials that comprise both micropores (< 2 nm) and mesopores (2–50 nm), where crystals comprise mesoporous ordering (i.e., section(s) of the material have mesopore periodicity repeating over one or more dimensions of the material).
Interpretation of the Claim 2 Preamble and ‘to Clause’
Claim 2 recites the following preamble and the result of practice of the claimed method; that is the below bolded text “to”, as follows:
2. A method for synthesis of hierarchically ordered crystalline microporous material having mesoporous ordering . . .
to
to dissolve/incise parent crystalline microporous material into oligomeric units of the parent crystalline microporous material, and then form a solid hierarchically ordered mesostructured having mesoporous order.
The plain meaning of the bolded “to” is “for the purpose of”, which is equivalent to a ‘wherein’, ‘whereby’ or ‘adapted to’ clause. MPEP § 2111.04(I). The language after “to” does not change the way the three claim 2 method steps are practiced (i.e., does not change the structure of claim 2). In this regard, claim scope is not limited by claim language that does not limit a claim to a particular structure. MPEP § 2111.04 (citing In Hoffer v. Microsoft Corp., 405 F.3d 1326, 1329, 74 USPQ2d 1481, 1483 (Fed. Cir. 2005) (the court noted that a "‘whereby clause in a method claim is not given weight when it simply expresses the intended result of a process step positively recited”).
The claim 2 preamble2 and above-identified ‘to clause’ are given effect as a claim limitation to the extent that the preamble term “hierarchically ordered mesostructures” is subsequently recited in the claim 2 ‘to clause’. The claim 2 preamble and ‘to clause’ are thus interpreted to require that the following claim 2 method steps of: (1) “forming an aqueous suspension”; and (2) “hydrothermally treating the aqueous suspension:
Claim 2 . . . forming an aqueous suspension of an effective amount of a parent crystalline microporous material having an underlying microporous structure, an effective amount of an alkaline reagent and an effective amount of a supramolecular template . . . and . . .
hydrothermally treating the aqueous suspension under conditions effective for mesophase transition. . .
result in the formation “hierarchically ordered mesostructures”.
Interpretation of “zeolite having FAU framework”
Instant claim 29 recites, and the specification working examples employ, a zeolite having and FAU framework, as the only exemplified “parent crystalline microporous material having an underlying microporous structure”.
Zeolites are inorganic crystalline aluminosilicates with a network of pores classified as microporous materials (pore size< 2 nm). G. Garcia et al., 489 Journal of Crystal Growth, 36-41 (2018). The general composition of the five zeolites can be approximated by the formula NaxAlxSiyO2(x+y) zH2O, where the SiO2/Al2O3 ratio is given by 2y/x. Garcia at page 36, col. 1. These zeolites possess different porous frameworks, except the zeolites X and Y that exhibit the FAU structure, which is related to the natural mineral faujasite. Garcia at page 36, col. 1. The FAU structure/framework is defined in the art. See e.g., Baerlocher et al., in Atlas of Zeolite Framework Types, 140-141 (6th Ed., 2007); specification at page 2, [0003]. Zeolite X and zeolite Y appear to be the only two zeolites known in the art to have the FAU framework. See e.g., T. Frising et al., 114 Microporous and Mesoporous Materials, 27-63 (2008). This is consistent with the specification, which does not teach any other zeolites (other than zeolite X and zeolite Y that have the FAU framework). Specification at page 2, [0004].
Interpretation of “hydrothermally treating”
Claim 2 recites the step of “hydrothermally treating”. The specification teaches that:
[0057] . . . Hydrothermal treatment is conducted: for a period of about 4-168, 12-168, 24-168, 4-96, 12-96 or 24-96 hours; at a temperature of about 70-250, 70-210, 70-180, 70-150, 90-250, 90-210, 90-180, 90-150, 110-250, 110-210, 110-180 or 110-150 °C; and at a pressure of about atmospheric to autogenous pressure.
Specification at page 28, [0057] (emphasis added). The term “autogenous pressure” is generally used in the art to mean the pressure attained upon heating a mixture in a sealed container. See, for example, specification at page 32, [0072]. The claim term “hydrothermal treatment” is therefore broadly and reasonably interpreted as simply a heating step to above ambient/room temperature at any pressure.
Withdrawal Claim Rejections 35 U.S.C. 112(b)
Previous claim rejections under § 112(b) that are not addressed below are withdrawn.
Claim Objections
Claims 23, 31 and 32 are objected to as being dependent upon a rejected base claim, but would be allowable if rewritten in independent form including all of the limitations of the base claim and any intervening claims.
Rejections 35 U.S.C. 112(b)
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.
Pursuant to 35 U.S.C. 112(b), the claim must apprise one of ordinary skill in the art of its scope so as to provide clear warning to others as to what constitutes infringement. MPEP 2173.02(II); Solomon v. Kimberly-Clark Corp., 216 F.3d 1372, 1379, 55 USPQ2d 1279, 1283 (Fed. Cir. 2000).
§ 112(b) Rejection – Unclear Claim Step of “is controlled by”
Claims 5-15 are rejected pursuant to 35 U.S.C. 112, as indefinite because the meaning of “is controlled by” is not clear to one of skill. For example, claim 5 recites “is controlled by” in the following context.
5. (Currently Amended) The method as in claim 2, wherein the aqueous suspension further comprises an ionic co-solute that is separate from an anion associated with the supramolecular template wherein shaped micelles are formed and the shape of the micelles is controlled by selection of the ionic co-solute, and wherein the ionic co-solute is selected from the group consisting of CO32-, SO42-, S2O32-, H2PO4-, F-, Cl-, Br-, NO3-, I-, ClO4-, SCN- and C6H5O8-3.
Claim 5 is indefinite because it is not clear to one of skill how to meet the limitation of “the shape of the micelles is controlled by selection of the ionic co-solute”. Dependent claims 6-15 do not cure or have this same issue. The specification teaches that different ionic co-solutes may give different the micelle curvature/shape. Specification at page 24, [0060]. Thus, one of ordinary skill can certainly control micelle curvature/shape depending upon which ionic co-solute is selected; but two different experiments (i.e., with a first and second ‘selected’ ionic co-solute) and a comparison would be required to demonstrated “controlled by selection”, which limitations are not recited in the claims at issue. This issue here is that it is not clear whether: (1) claim 5 requires a fist experiment with a first selected ionic solute and a second experiment with another (a reference ionic co-solute) and then determining whether a different micelle shape is obtained and thereby the required “control” has been achieved; or (2) the claim 5 language “the shape of the micelles is controlled by selection of the ionic co-solute” is merely an intended result; i.e., merely non-limiting mental process language.3 This limitation is further unclear because no reference ionic co-solute is given to compare whether the required “control” has been achieved. Dependent claims 6-15 do not cure or have this same issue. This rejection can be overcome simply by deleting the language at issue.
§ 112(b) Rejection – Lack of Antecedent Basis in New Claims 35 and 36
Claims 35 and 36 are rejected pursuant to 35 U.S.C. 112, as indefinite because antecedent basis for “the constituent” is unclear. MPEP § 2173.05(e).
35. The method as in claim 33, wherein the constituent is a head group moiety and is selected from the group consisting of organosilanes, hydroxysilyls and alkoxysilyls, and wherein the quaternary ammonium moiety comprises a terminal C6-C24 alkyl group.
36. The method as in claim 33, wherein the constituent group is selected from the group consisting of aromatic groups containing 6-50 carbon atoms, aryl groups containing 1-50 carbon atoms, and a combination of aromatic and alkyl groups having up to 50 carbon atoms.
Base claim 33 (dependent upon claim 2) recites the following structural elements for the supramolecular template:
Base claim 33 (imported from claim 2) . . . wherein the supramolecular template is a bulky surfactant that possesses a dimension that constrains diffusion into the parent crystalline microporous material pore-channels, cavities or window openings having the pore dimension, and comprises one or more of:
a quaternary ammonium moiety and a constituent group selected from the group consisting of organosilanes, hydroxysilyls, alkoxysilyls, aromatics, branched alkyls, sulfonates, carboxylates, phosphates and combinations comprising one of the foregoing constituent groups;
a quaternary phosphonium moiety and a constituent group selected from the group consisting of organosilanes, hydroxysilyls, alkoxysilyls, aromatics, branched alkyls, sulfonates, carboxylates, phosphates and combinations comprising one of the foregoing constituent groups; or
two quaternary ammonium groups with an alkyl group bridging the quaternary ammonium groups containing 1-10 carbon atoms; and
Because claim 33 recites two different occurrences of “constituent group”, it is not clear which of these claims 35 and 36 references. MPEP § 2173.05(e).4
Maintained Claim Rejections - 35 USC § 112(a) (Scope of Enablement)
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 2, 5-15, 24, 25, 27-29, and 33-36 are rejected under 35 U.S.C. 112(a) because the specification, while enabling one of skill in the art to make and use the following subject matter (where amendments to claim 2 are indicted by underlined and strikeout text):5
2. A method for synthesis of hierarchically ordered crystalline zeolite having FAU framework microporous material having mesoporous ordering, the method comprising:
forming an aqueous suspension of an effective amount of a parent zeolite having FAU framework crystalline microporous material having an underlying microporous structure,
an effective amount of an alkaline reagent and
an effective amount of a supramolecular template,
wherein the supramolecular template is a quaternary ammonium moiety comprising a terminal C6-C24 alkyl group and a head group comprising a moiety selected from the group consisting of organosilanes, hydroxysilyls, and alkoxysilyls
hydrothermally treating the aqueous suspension under conditions effective for mesophase transition to dissolve/incise the parent zeolite having FAU framework crystalline microporous material into oligomeric units , and then form a solid hierarchically ordered mesostructure having mesoporous order.
does not reasonably enable one of skill in the art to make and use the full scope of the claimed method directed to.
(1) per claim 2, any “parent crystalline microporous material having an underlying microporous structure”; or
(2) the full scope of supramolecular templates recited in claim 2:
Claim 2 . . . wherein the supramolecular template is a bulky surfactant that possesses a dimension that constrains diffusion into the parent crystalline microporous material pore-channels, cavities or window openings having the pore dimension, and comprises one or more of:
a quaternary ammonium moiety and a constituent group selected from the group consisting of organosilanes, hydroxysilyls, alkoxysilyls, aromatics, branched alkyls, sulfonates, carboxylates, phosphates and combinations comprising one of the foregoing constituent groups;
a quaternary phosphonium moiety and a constituent group selected from the group consisting of organosilanes, hydroxysilyls, alkoxysilyls, aromatics, branched alkyls, sulfonates, carboxylates, phosphates and combinations comprising one of the foregoing constituent groups; or
two quaternary ammonium groups with an alkyl group bridging the quaternary ammonium groups containing 1-10 carbon atoms . . .
Factors to be considered when determining whether there is sufficient evidence to support a determination that a disclosure does not satisfy the enablement requirement and whether any necessary experimentation is “undue” include, but are not limited to:
(A) The breadth of the claims;
(B) The nature of the invention;
(C) The state of the prior art;
(D) The level of one of ordinary skill;
(E) The level of predictability in the art;
(F) The amount of direction provided by the inventor;
(G) The existence of working examples; and
(H) The quantity of experimentation needed to make or use the invention based on the content of the disclosure.
MPEP. § 2164.01(a); In re Wands, 858 F.2d 731, 737, 8 USPQ2d 1400, 1404 (Fed. Cir. 1988); In re Wright, 999 F.2d 1557, 27 USPQ2d 1510 (Fed. Cir. 1993). The burden is on the examiner to show that the specification as filed and what was well known to one of skill in the art at the time of filing does not reasonably enable the full scope of the claimed invention. MPEP § 2164.05 (citing Pac. Biosciences of Cal., Inc. v. Oxford Nanopore Techs., Inc., 996 F.3d 1342, 1352, 2021 USPQ2d 519 (Fed. Cir. 2021).
Breadth of the Claims
The claim breadth is vast in view of the generic nature of the claimed method. The claim 2 term “a parent crystalline microporous material having an underlying microporous structure” is extremely broad. Not only does this term compass zeolites6 (to which the specification embodiments are primarily directed), but to any crystalline microporous material, for example, metal organic frameworks. As discussed in Z. Bao et al., 9 Energy and Environmental Science, 3612-3641 (2016) (see Bao at page 3634, col. 2) (“MOFs possess a higher degree of tailorability because of the almost infinite number of possible metal–ligand combinations”); See also J. Liu et al., 46 Chem. Soc. Rev., 5730-5770 (2017) (page 5752, col. 1, “the number of possible MOFs is virtually infinite”); see also, D. Bradshaw et al., 43 Chem. Soc. Rev. 5431-5444 (2014).
The claim 2 term genus of “supramolecular template” is extremely broad and defined by minimal structure.
Claim 2 . . . wherein the supramolecular template is a bulky surfactant that possesses a dimension that constrains diffusion into the parent crystalline microporous material pore-channels, cavities or window openings having the pore dimension, and comprises one or more of:
a quaternary ammonium moiety and a constituent group selected from the group consisting of organosilanes, hydroxysilyls, alkoxysilyls, aromatics, branched alkyls, sulfonates, carboxylates, phosphates and combinations comprising one of the foregoing constituent groups;
a quaternary phosphonium moiety and a constituent group selected from the group consisting of organosilanes, hydroxysilyls, alkoxysilyls, aromatics, branched alkyls, sulfonates, carboxylates, phosphates and combinations comprising one of the foregoing constituent groups; or
two quaternary ammonium groups with an alkyl group bridging the quaternary ammonium groups containing 1-10 carbon atoms; and
The supramolecular chemical structure is undefined in claim 2. The specification teaches that suitable surfactants for use as supramolecular templates are provided to assist the reassembly and recrystallization of dissolved components (oligomers) by covalent and/or electrovalent interactions. Specification at page 18, [0052]. The specification goes on to provide a number of chemical structural units that can be mixed and matched to achieve a supramolecular template. Specification at pages 18-23. However, the specification provides no limiting core structure for “supramolecular template”.
Generally, in the art of zeolites, the supramolecular templating method is understood to mean a supramolecular assembly of surfactants is used as the mesopore template. K. Egeblad et al., 20 Chemistry of Materials, 946-960 (2008) (see page 949, col. 1) (“[i]n the supramolecular templating method, a supramolecular assembly of surfactants is used as the mesopore template”).
State and Predictability in the Art
The claims and specification are directed to zeolite preparation by supramolecular templating. The specification teaches that hierarchically ordered crystalline microporous materials (HOCMMs) produced according to the present disclosure are effective as catalysts, or components of catalysts, in hydrocracking of hydrocarbon oil. Specification at page 42, [0086].
This art of supramolecular templating in mesoporous zeolite synthesis is nascent, unpredictable and challenging. For example, Egeblad teaches that it can be quite difficult to firmly establish to what extent the solid or the supramolecular assembly of surfactants actually acts as template and thereby directly controls the size and shape of the meso-/macropores in the resulting hierarchical zeolite material. K. Egeblad et al., 20 Chemistry of Materials, 946-960 (2008) (page 958, col. 1). This challenge is even more pronounced for the indirect templating method, because here the original template is no longer present when the hierarchical zeolite material is formed. Id.
Li teaches that the synthesis mechanisms of zeolites by nucleation and crystallization involve many time-dependent chemical processes that take place in multiple phases and, consequently, the targeted crystallization of a specific zeolite structure cannot be achieved. C. Li et al., 57 Angew. Chem. Int. Ed., 15330-15353 (2018) (“Li”) (see Li at 15331, col. 1). Li teaches that the preparation of hierarchical zeolites containing well-defined mesoporosity is an outstanding challenge in catalysis. Li at page 15349, col. 2.
In another example, Sachse teaches that surfactant-templating (also referred as supramolecular templating) emerged as general term to describe the chimie douce approaches for conceiving solids with tunable porosity. A. Sachse et al., 29 Chemistry of Materials, 3827-3853 (2017) (“Sachse”). Sachse teaches that the development of mesoporous zeolites using surfactants is still at an early stage. Sachse at page 3849, col. 1. Sachse teaches that although, surfactant-oriented strategies allow for the preparation of hierarchical zeolites with interconnected porosity at different length scales, the control over their porous architecture is much poorer than in the case of amorphous solids and the quest remains opened for the synthesis of hierarchical zeolites featuring mesopores arranged in different geometries. Id. Sachse further teaches that a better understanding on both how surfactants produce mesoporosity in zeolites and the role of this in the diffusion properties of hierarchical zeolites is essential for the rational design of new materials with improved properties. Sachse at page 3849, col. 1.
These challenges have not been resolved as the instant filing date. For example, Luan teaches that though zeolites have been successfully synthesized for several decades, the roles of templates for zeolite synthesis are still not fully understood yet. H. Luan et al., 43 Chinese Journal of Structural Chemistry, 1-11 (2024) (Abstract).7 Luan further teaches that currently, zeolite synthesis was mainly performed by trial-and-error route, and the design of zeolite synthesis was needed in the future. Luan at page 8, col. 2. Luan further teaches that the mechanisms for the zeolite nucleation and crystallization growth are still unclear, which would be the great challenges for theoretical calculations and simulations of designing zeolites. Luan at page 8, col. 2.
In another Example, R. Parsapur et al., 63 Angew. Chem. Int. Ed., 1-10 (e202314217) (2024) (“Parsapur”) states that
However, despite the notable advances in synthesizing zeolites and ordered mesoporous silicates separately, fabricating [hierarchically ordered zeolites] HOZs by integrating molecular templating and supramolecular templating mechanisms has remained a challenging task.
Consequently, the [hierarchically ordered zeolites] HOZs of FAU-type zeolites have not been reported so far despite their major applications in fluid catalytic cracking (FCC) and hydrocracking.
Parsapur at pages 1-2. See footnote 7. In sum, the art of supramolecular templating in mesoporous zeolite synthesis is nascent, unpredictable and challenging.
Guidance in the Art and the Specification
The bulk of the specification provides only general guidance, particularly with respect to the claimed “supramolecular template”. Specification at pages 1-43. The specification provides a number of chemical structural units that can be mixed and matched to achieve a supramolecular template. Specification at pages 18-23. However, the specification provides no limiting core structure for “supramolecular template”.
The most specific specification disclosure are the working examples at pages 44 et seq. It is first noted (as taught in the specification) that specification working Example 1A (employing cetyltrimethylammonium bromide as the supramolecular template) may not be an embodiment of the claimed invention, in the case where the parent zeolite is limited to the “FAU framework”. See specification Example 1A at page 46, [0093]-[0094].
Regarding Example 1A, the specification teaches:
For instance, in the examples herein, FAU zeolite is used; when the supramolecular template material was [cetyltrimethylammonium bromide (CTAB)] (~0.25 nm), [hierarchically ordered crystalline microporous materials (HOCMMs)] were not realized; however, when the supramolecular template was an organosilane ( ~0.7 nm), HOCMMs were realized, as these are closer in dimension to the pore dimensions for FAU zeolite and therefore are constrained from entering such pores.
Specification at page 27, [0064] (emphasis added). Specification working Example 1B (alternative procedure of [0096]) is summarized below. Specification at pages 47, [0096].
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Working Example 1B employs dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium chloride (referred to in the specification either as TPOAC or DOAC) as the supramolecular template rather than the cetyltrimethylammonium bromide of Example 1A.
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All of the subsequent specification working Examples (i.e., Examples 1C-3B) are performed in a similar manner with zeolite H-Y as the parent crystalline microporous material and dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium chloride as the supramolecular template with variation of the base and/or other parameters. In sum, the working Examples are limited to only one species of zeolite (i.e., zeolite Y) and one species of supramolecular template (i.e., dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium chloride).
Outside of the working examples, the only supramolecular template species disclosed in the specification body are the following:
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Specification at page 21, [0055]. These all have the same silyl-ammonium core structure.
As discussed above, the art of supramolecular templating in mesoporous zeolite synthesis is nascent. MPEP § 2164.03 (citing Chiron Corp. v. Genentech Inc., 363 F.3d 1247, 1254, 70 USPQ2d 1321, 1326 (Fed. Cir. 2004) “[n]ascent technology, however, must be enabled with a ‘specific and useful teaching.’ The law requires an enabling disclosure for nascent technology because a person of ordinary skill in the art has little or no knowledge independent from the patentee’s instruction”). Based on searches conducted, the art does not provide supplementary guidance in addition to Applicant’s specification to practice the full claim scope.
The Quantity of Experimentation Needed Is Undue
In the current case, a prima facie case of non-enablement under 35 U.S.C. § 112(a) of claims 2, 5-15, 24, 25, 27-29, and 33-36 is established because upon balancing the above-discussed wands factors, the specification at the time the application was filed, would not have taught one skilled in the art how to make and/or use the full claim scope of:
(1) per claim 2, any “parent crystalline microporous material having an underlying microporous structure”; or
(2) the full scope of supramolecular templates recited in claim 2,
without undue experimentation. The primary Wands factors considered are the claim breadth, unpredictability, and lack of guidance in the specification and art of record. A further significant factor is that (as discussed in detail above) the claims are directed a nascent technology. MPEP § 2164.03 (citing Chiron Corp. v. Genentech Inc., 363 F.3d 1247, 1254, 70 USPQ2d 1321, 1326 (Fed. Cir. 2004) “[n]ascent technology, however, must be enabled with a ‘specific and useful teaching.’ The law requires an enabling disclosure for nascent technology because a person of ordinary skill in the art has little or no knowledge independent from the patentee’s instruction”).
The primary issue with respect to the § 112 rejection is as follows. As discussed above, the specification provides specific guidance only one species of zeolite (i.e., zeolite Y) and one species of supramolecular template (i.e., dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium chloride) as disclosed in the working examples.
But neither the art of record nor the specification provides guidance with respect to how to how to extend the single species of the working example to the claim scope of:
((1) per claim 2, any “parent crystalline microporous material having an underlying microporous structure”; or
(2) the full scope of supramolecular templates recited in claim 2.
This lack of guidance is balanced with the art’s nascent nature and unpredictability. For example, as discussed above, Egeblad teaches that it can be quite difficult to firmly establish to what extent the solid or the supramolecular assembly of surfactants actually acts as template and thereby directly controls the size and shape of the meso-/macropores in the resulting hierarchical zeolite material. K. Egeblad et al., 20 Chemistry of Materials, 946-960 (2008) (page 958, col. 1). This challenge is even more pronounced for the indirect templating method, because here the original template is no longer present when the hierarchical zeolite material is formed. Id. In view of balancing the above-discussed factors, a prima facie case of undue experimentation is established.
Applicant’s Argument
Applicant argues that claim 2 is amended to recite particular combinations of moieties, with particular dimensional definitions relative to the dimensions of pores of the parent crystalline microporous material having an underlying microporous structure. Reply (3/18/2026) at page 15. Applicant further argues that based on the amount of direction provided by the inventors in the specification, a person of ordinary skill in the art is reasonably enabled to carry out controlled dissolution when diffusion into micropores is constrained due to formation of oligomers that recrystallize around the micelles formed by the supramolecular template. Reply (3/18/2026) at page 15.
Applicant further argues that the art cited to show the state-of-the-art lacks of predictability is for bottom-up zeolite synthesis. In contrast, the present claims start with a parent crystalline microporous material (already synthesized with known properties, for example, as ascertainable by the International Zeolite Association as explained in the specification), and the claims are directed to acting on that parent crystalline microporous material. Reply (3/18/2026) at page 15.
This argument is not persuasive because it does not discuss what errors the Examiner made in the analysis of the Wands factors, which form the basis of the instant § 112 rejection. MPEP. § 2164.01(a); In re Wands, 858 F.2d 731, 737, 8 USPQ2d 1400, 1404 (Fed. Cir. 1988); In re Wright, 999 F.2d 1557, 27 USPQ2d 1510 (Fed. Cir. 1993). Regarding, Applicant’s argument regarding predictability, other than C. Garcia-Martinez et al., 2 Catalyst & Scientific Technology, 987-994 (2012) (“Garcia-Martinez”), which is limited to CTAB as the supramolecular template, there is no art of record (nor has Applicant’s Reply cited such) regarding the claimed process that starts with a parent crystalline microporous material (already synthesized with known properties) that can supplement Applicant’s specification. Rather, the art of record demonstrates that supramolecular templating in mesoporous zeolite synthesis is nascent, unpredictable and challenging. For example, Li teaches that the synthesis mechanisms of zeolites by nucleation and crystallization involve many time-dependent chemical processes that take place in multiple phases and, consequently, the targeted crystallization of a specific zeolite structure cannot be achieved. C. Li et al., 57 Angew. Chem. Int. Ed., 15330-15353 (2018) (“Li”) (see Li at 15331, col. 1). Li teaches that the preparation of hierarchical zeolites containing well-defined mesoporosity is an outstanding challenge in catalysis. Li at page 15349, col. 2.
Maintained Claim Rejections 35 U.S.C. 112(a) – Written Description
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.
For an originally filed claim, 35 U.S.C. 112(a) requires that the specification shall contain a written description of the invention demonstrate that the inventor was in possession of the invention that is claimed.8 MPEP § 2163(I); MPEP § 2163(II)(A)(3)(a). Possession may be shown by disclosure of drawings or structural chemical formulas that show that the invention was complete. MPEP § 2163(I).
The written description requirement for a claimed genus may be satisfied through sufficient description of a representative number of species by actual reduction to practice, reduction to drawings, or by disclosure of relevant, identifying characteristics, i.e., structure or other physical and/or chemical properties, by functional characteristics coupled with a known or disclosed correlation between function and structure, or by a combination of such identifying characteristics, sufficient to show the inventor was in possession of the claimed genus. MPEP § 2163(II)(A)(3)(a)(ii). A "representative number of species" means that the species which are adequately described are representative of the entire genus. MPEP § 2163(II)(A)(3)(a)(ii). Thus, when there is substantial variation within the genus, one must describe a sufficient variety of species to reflect the variation within the genus. MPEP § 2163(II)(A)(3)(a)(ii) (citing AbbVie Deutschland GmbH & Co., KG v. Janssen Biotech, Inc., 759 F.3d 1285, 1300, 111 USPQ2d 1780, 1790 (Fed. Cir. 2014).
The § 112(a) rejection
Claims 2, 5-15, 24, 25, 27-29, and 33-36 are rejected under 35 U.S.C. 112(a) as failing to comply with the written description requirement because the application as filed does not disclose either sufficient species, of the claim 2 genera of:
(1) per claim 2, any “parent crystalline microporous material having an underlying microporous structure”; or
(2) the full scope of supramolecular templates recited in claim 2:
Claim 2 . . . wherein the supramolecular template is a bulky surfactant that possesses a dimension that constrains diffusion into the parent crystalline microporous material pore-channels, cavities or window openings having the pore dimension, and comprises one or more of:
a quaternary ammonium moiety and a constituent group selected from the group consisting of organosilanes, hydroxysilyls, alkoxysilyls, aromatics, branched alkyls, sulfonates, carboxylates, phosphates and combinations comprising one of the foregoing constituent groups;
a quaternary phosphonium moiety and a constituent group selected from the group consisting of organosilanes, hydroxysilyls, alkoxysilyls, aromatics, branched alkyls, sulfonates, carboxylates, phosphates and combinations comprising one of the foregoing constituent groups; or
two quaternary ammonium groups with an alkyl group bridging the quaternary ammonium groups containing 1-10 carbon atoms . . .
or a structure-function correlation, such that one of skill can recognize which combinations of these species function such that upon hydrothermally treating in an aqueous suspension with an alkaline reagent, can perform the claim 2 function of:
2 . . . synthesis of hierarchically ordered crystalline microporous material having mesoporous ordering . . .
form a solid hierarchically ordered mesostructure having mesoporous order.
or that can perform the further functions recited in dependent claims 8, 9, and 11-15:
8 and 11 . . . wherein the hierarchically ordered mesostructures possess a cubic mesophase symmetry and the mesophase transition is characterized by a surfactant packing parameter g in the range of about 0.4-0.8 or about 0.9-1.1. . .
9 and 12-15. . . wherein the hierarchically ordered mesostructures possess a cubic mesophase symmetry or a hexagonal mesophase symmetry or a lamellar mesophase symmetry . . .
Claim Breadth
Claim breath is relevant to the instant § 112(a) written description rejection. The written description must lead a person of ordinary skill in the art to understand that the inventor possessed the entire scope of the claimed invention. MPEP § 2163(II)(A)(3)(a)(ii) (citing Juno Therapeutics, Inc. v. Kite Pharma, Inc., 10 F.4th 1330, 1337, 2021 USPQ2d 893 (Fed. Cir. 2021)). The vast claim breadth of
(1) per claim 2, any “parent crystalline microporous material having an underlying microporous structure”; or
(2) the full scope of supramolecular templates recited in claim 2,
was discussed in detail above in the § 112(a) enablement rejection.
Guidance in the Art and Specification
It is first noted that what is conventional or well known to one of ordinary skill in the art need not be disclosed in detail. MPEP § (II)(A)(3)(a). Thus, the state of and predictability in the art is a relevant consideration in determining compliance with § 112(a), written description. MPEP § (II)(A)(3)(a) (citing Capon v. Eshhar, 418 F.3d 1349, 1357, 76 USPQ2d 1078, 1085 (Fed. Cir. 2005) ("The ‘written description’ requirement must be applied in the context of the particular invention and the state of the knowledge…. As each field evolves, the balance also evolves between what is known and what is added by each inventive contribution”).
Guidance in the specification and art was discussed in detail above. As discussed above, the only supramolecular template species disclosed in the specification body are the following:
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which all have a similar core structure. Specification at page 21, [0055]. The only “parent crystalline microporous material having an underlying microporous structure” demonstrated as effective in the claimed method is zeolite Y, which has an FAU framework. See Claim Interpretation above. That is all the specification working Examples (i.e., Examples 1B-3B) are performed in a similar manner with zeolite H-Y as the parent crystalline microporous material and dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium chloride as the supramolecular template with variation of the base and/or other parameters. Specification at pages 44-58.
Neither the art nor the specification teaches a structure-functional relationship between the claimed “parent crystalline microporous material having an underlying microporous structure” and the vast claim 2 genus of supramolecular template such that one of skill can recognize which combinations can perform the above-cited claimed functions.
Originally Supported Claims 2, 5-15, 24, 25, 27-29, and 33-36 Lack Adequate Written Description Support
Neither the art nor specification disclose either sufficient species of, per claim 2:
(1) any “parent crystalline microporous material having an underlying microporous structure”; or
(2) the full scope of supramolecular templates recited in claim 2:
Claim 2 . . . wherein the supramolecular template is a bulky surfactant that possesses a dimension that constrains diffusion into the parent crystalline microporous material pore-channels, cavities or window openings having the pore dimension, and comprises one or more of:
a quaternary ammonium moiety and a constituent group selected from the group consisting of organosilanes, hydroxysilyls, alkoxysilyls, aromatics, branched alkyls, sulfonates, carboxylates, phosphates and combinations comprising one of the foregoing constituent groups;
a quaternary phosphonium moiety and a constituent group selected from the group consisting of organosilanes, hydroxysilyls, alkoxysilyls, aromatics, branched alkyls, sulfonates, carboxylates, phosphates and combinations comprising one of the foregoing constituent groups; or
two quaternary ammonium groups with an alkyl group bridging the quaternary ammonium groups containing 1-10 carbon atoms . . .
or a structure-function correlation, such that one of skill can recognize which species of “parent crystalline microporous material having an underlying microporous structure” that upon hydrothermally treating in an aqueous suspension with an alkaline reagent, can perform the functions of:
2 . . . synthesis of hierarchically ordered crystalline microporous material having mesoporous ordering . . .
form a solid hierarchically ordered mesostructure having mesoporous order.
or that can perform the further functions recited in dependent claims 8, 9, and 11-15:
8 and 11 . . . wherein the hierarchically ordered mesostructures possess a cubic mesophase symmetry and the mesophase transition is characterized by a surfactant packing parameter g in the range of about 0.4-0.8 or about 0.9-1.1. . .
9 and 12-15. . . wherein the hierarchically ordered mesostructures possess a cubic mesophase symmetry or a hexagonal mesophase symmetry or a lamellar mesophase symmetry . . .
In sum, the claims recite very minimal structure (with respect the both the parent crystalline material and the supramolecular template and co-template) and neither the art nor the specification shows a well-established correlation between the structure of these and the claimed functions, such that one of skill can recognize which species to select to practice the claimed methods. As stated above, the written description requirement may also be satisfied through disclosure of function and minimal structure when there is a well-established correlation between structure and function. MPEP § 2163(II)(A)(3)(a)(i). In contrast, without such a correlation, the capability to recognize or understand the structure from the mere recitation of function and minimal structure is highly unlikely. MPEP § 2163(II)(A)(3)(a)(i) (citing Eli Lilly, 119 F.3d at 1568, 43 USPQ2d at 1406).
Further, the specification does not disclose a representative number of species because, as discussed above, only three supramolecular templates are disclosed that performs the claimed function, all of which have the same core structure. A "representative number of species" means that the species which are adequately described are representative of the entire genus. MPEP § 2163(II)(A)(3)(a)(ii); see also, Idenix Pharms. LLC v. Gilead Scis. Inc., 941 F.3d 1149, 1164 (Fed. Cir. 2019) (“[a]s a result, a POSA is deprived of any meaningful guidance into what compounds beyond the examples and formulas, if any, would provide the same result”).
Applicant’s Argument
Applicant argues that regarding the written description requirement, "possession" is shown by representative species and/or structural features common to the genus. (Ariad v. Lilly, 598 F.3d 1336 (Fed. Cir. 2010); MPEP §2163, as cited by the Examiner). Reply (3/18/2026) at page 16. Applicant argues that the Office Action contends the specification fails to show possession of the entire scope of the genus because it does not disclose a representative number of species or a structure-function correlation for "any parent crystalline microporous material". Reply (3/18/2026) at page 16. Applicant argues that the disclosure very clearly identifies how the function is performed and the result is achieved: by constraining diffusion into micropores of a parent CMM, oligomers are formed as very clearly explained in the specification and figures, and as summarized above by the Examiner. Reply (3/18/2026) at page 16. In addition, the genus claim is presented AND the disclosure describes many different species, and based on the explanation of the supramolecular template dimensions, the pore dimensions of certain zeolites are given, and pore dimensions of the other zeolites and CMMs are available from the IZA and other sources.
This argument is not persuasive because, while the specification does disclose how the function and result is achieved with only one species of supramolecular template and one species of zeolite, it does not disclose a structure function relationship permitting one of skill to recognize what other species within the large claimed genera of “supramolecular template” and “parent crystalline microporous material having an underlying microporous structure” can be chosen, in combination, to achieve the claimed function; particularly, in view of the art’s unpredictability. Applicant argues that disclosure describes many different species. However, only one species combination that actually achieves the claimed function is disclosed (i.e., zeolite Y and dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium). As discussed above, the specification body discloses two additional species of structurally similar dimethyl[3-(trimethoxysilyl)propyl]ammonium salts a supramolecular templates (see specification at page 21, [0055]) and a number of zeolite species (see specification at pages 25-26, [0062]). But outside the limited number of three disclosed supramolecular template and zeolite species, neither the art nor specification teaches which supramolecular templates are suitable in combination with the specifically disclosed zeolite species, let alone in combination with the full scope of any “parent crystalline microporous material having an underlying microporous structure”.
Maintained Claim Rejections - 35 USC § 103
The following is a quotation of 35 U.S.C. 103 which forms the basis for all obviousness rejections set forth in this Office action:
A patent for a claimed invention may not be obtained, notwithstanding that the claimed invention is not identically disclosed as set forth in section 102, if the differences between the claimed invention and the prior art are such that the claimed invention as a whole would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to which the claimed invention pertains. Patentability shall not be negated by the manner in which the invention was made.
The factual inquiries 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 AIA 35 U.S.C. 103(a) 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 2, 24, 27-29, and 33-36 are rejected under AIA 35 U.S.C. 103 as being unpatentable C. Garcia-Martinez et al., 2 Catalyst & Scientific Technology, 987-994 (2012) (“Garcia-Martinez”) and/or J. Ying et al., US 7,589,041 (2009) (“Ying”).
Claim 25 rejected under AIA 35 U.S.C. 103, as above, in further view of X. Zhang et al. 126 Energy, 677-688 (2017) (“Zhang”) and/or F. Tian et al., 83 Catalyst Communications, 66-69 (2016) (“Tian”).
C. Garcia-Martinez et al., 2 Catalyst & Scientific Technology, 987-994 (2012) (“Garcia-Martinez”)
Garcia-Martinez teaches a surfactant-based technique that allows precisely controlled mesoporosity to be introduced within a wide range of zeolite crystals (i.e. mesostructuring), e.g. FAU, MOR and MFI of various Si/Al ratios, while maintaining the chemical and physical properties of the zeolites (i.e. microporosity, crystallinity, acidity, etc.). Garcia-Martinez at page 987, col. 2.
Garcia-Martinez further teaches that fluid catalytic cracking catalysts made from the mesostructured Y zeolites demonstrate significant improvement in product selectivity as a result of reduced limitation in reactant and product diffusion. Garcia-Martinez at Abstract; Id. at page 933, col. 2.
Garcia-Martinez teaches a surfactant-based technique that allows precisely controlled mesoporosity to be introduced within a wide range of zeolite crystals (i.e., mesostructuring), e.g. FAU, MOR and MFI of various Si/Al ratios, while maintaining the chemical and physical properties of the zeolites (i.e. microporosity, crystallinity, acidity, etc.). Garcia-Martinez at page 987, col. 2.
Garcia-Martinez teaches synthesis of mesoporous zeolite Y crystals as follows:
Experimental
Syntheses
In a typical synthesis, 1.00 g of a Y material (Zeolyst CBV720 with Si/Al = 15) in 64 mL of a 0.37 M solution of NH4OH containing 0.70 g of cetyltrimethyl ammonium bromide (CTAB) was stirred for 20 min. The mixture was next heated at 150 °C under autogenous pressure for 10 h. The solid was filtered, washed, and dried. Close to 100% recovery was observed, and there was no significant leaching of Si or Al species into the filtrate. Alternatively, other bases such as NaOH, Na2CO3 or tetrapropylammonium hydroxide (TPAOH) could be used. The pH of the reaction mixture was maintained at [Symbol font/0x7E]9–11 to avoid desilication.
Garcia-Martinez at pages 987-988 (emphasis added). Garcia-Martinez’s above experimental can be schematically summarized as follows:
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As discussed above in Claim Interpretation, zeolite Y is, per claim 2, a “a parent crystalline microporous material having an underlying microporous structure” (and per claim 29 has a FAU framework).
The above Garcia-Martinez process meets each and every physical method-step limitation of claim 2.
Claim 2 . . . forming an aqueous suspension of an effective amount of a parent crystalline microporous material having an underlying microporous structure, an effective amount of an alkaline reagent and an effective amount of a supramolecular template . . . and . . .
hydrothermally treating the aqueous suspension under conditions effective for mesophase transition. . .
where Garcia-Martinez’s step of “[t]he mixture was next heated at 150 °C under autogenous pressure for 10 h”, clearly teaches the conditions the hydrothermal treatment of claim 2.
Garcia-Martinez’s teaches that:
The observations described above suggest that the introduction of controlled mesoporosity into crystalline zeolites proceeds possibly through a surfactant-assisted crystal rearrangement mechanism. Fig. 3 illustrates a plausible scheme of the critical steps in this process. Under the basic reaction conditions (pH E 10.5), some of the Si–O–Si bonds are broken to offer some flexibility in the crystalline structure, and yield negatively charged sites in the zeolite framework that attract cationic surfactants. Electrostatic interactions between these negatively charged sites and the positively charged surfactants, and self-assembly of surfactant cations to form micelles within the zeolite crystals (so as to minimize the interaction of hydrophobic surfactant tails with the aqueous solution) cause the crystal structure to rearrange to form mesopores around the micelles.
Garcia-Martinez at page 989, col. 2.
Garcia-Martinez clearly meets the following claim 2 recitations.
claim 2 . . . hydrothermally treating the aqueous suspension under conditions effective for mesophase transition to dissolve/incise parent crystalline microporous material into oligomeric units of the parent crystalline microporous material, and then form a solid hierarchically ordered mesostructured having mesoporous order.
See also, Garcia-Martinez at page 989, col. 2 (“The role of the cationic surfactant was therefore critical because it protected the zeolite from desilication (as confirmed by control experiments with no surfactant), and allowed us to obtain much higher ‘‘hierarchy factors’’”).
Garcia-Martinez’s Y material (Zeolyst CBV720 with Si/Al = 15) meets the claim 2 limitation of:
Claim 2 . . . wherein the underlying microporous structure of the parent crystalline microporous material is characterized by pore-channels, cavities or window openings having a pore dimension,
As discussed in Claim Interpretation above, zeolite Y is one of only two zeolites known in the art to have the FAU framework. See e.g., T. Frising et al., 114 Microporous and Mesoporous Materials, 27-63 (2008).
It is further noted that Garcia-Martinez teaches that the size of these mesopores can be nicely controlled by using surfactant molecules of different lengths confirming the surfactant-templating mechanism proposed (ESI†, Fig. S2) as well as the mesopore architecture which can be controlled by adjusting the synthesis conditions to produce hexagonal ordering (ESI†, Fig. S3) at a higher degree of mesostructuring, or non-ordered mesoporosity (ESI†, Fig. S4) at a lower degree of mesostructuring. Garcia-Martinez at pages 988-989. Garcia-Martinez provides motivation to one of ordinary skill to explore different surfactant supramolecular templates.
In this regard, Garcia-Martinez teaches that:
The severity of this pre-treatment (e.g. amount of acid, time, temperature, etc.) could be fine-tuned to control the degree of dealumination and the amount of the mesoporosity that could be introduced in the subsequent treatment by surfactants in a basic media.
Garcia-Martinez at page 990, col. 1.
Differences between Garcia-Martinez and Claim 2
Garcia-Martinez differs from claim 2 becuase Garcia-Martinez’s supramolecular template cetyltrimethylammonium bromide,
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does not meet the claim 2 recitation of:
claim 2 . . . wherein the supramolecular template is a bulky surfactant that possesses a dimension that constrains diffusion into the parent crystalline microporous material pore-channels, cavities or window openings having the pore dimension, and comprises one or more of:
a quaternary ammonium moiety and a constituent group selected from the group consisting of organosilanes, hydroxysilyls, alkoxysilyls, aromatics, branched alkyls, sulfonates, carboxylates, phosphates and combinations comprising one of the foregoing constituent groups;
a quaternary phosphonium moiety and a constituent group selected from the group consisting of organosilanes, hydroxysilyls, alkoxysilyls, aromatics, branched alkyls, sulfonates, carboxylates, phosphates and combinations comprising one of the foregoing constituent groups; or
two quaternary ammonium groups with an alkyl group bridging the quaternary ammonium groups containing 1-10 carbon atoms . . .
because it is a quaternary ammonium moiety that comprises only straight-chain alkyl groups and not a branched alkyl group as required by claim 2.
J. Ying et al., US 7,589,041 (2009) (“Ying”)
Ying is cited here to supplement Garcia-Martinez. Ying appears to be a patent based on Garcia-Martinez’s published work.
Ying teaches a method of preparing a mesostructured zeolite comprising: a) adding a zeolite to a medium comprising an acid or base, and optionally a surfactant; b) adding a surfactant to the medium from Step a) if it is not there already; c) optionally adding a swelling agent to the medium from step b); d) optionally hydrothermally treating the medium from step b) or c); and e) washing and drying the resulting material. Ying at col. 2, lines 54-61.
Ying teaches that the mesostructured zeolite is useful as a catalyst. Ying at col. 4,lines 16-20.
Ying teaches that the zeolite is selected from the group consisting of faujasite (FAU), mordenite (MOR), and ZSM-5 (MFI).
Ying teaches that the base is an alkali hydroxide, alkaline earth hydroxide, NH-OH or a tetralkylammonium hydroxide. In a further embodiment, the base is NaOH, NHOH, or tetramethylammoniumhydroxide. Ying at col. 3, lines 6-10.
Ying teaches that the surfactant is an alkylammonium halide and in a further embodiment, the surfactant is a cetyltrimethylammonium bromide (CTAB) surfactant. Ying at col. 3, lines 13-14.
Ying teaches that:
The mesopore size and architecture may also be conveniently tuned by well-known techniques, such as the use of surfactants with different aliphatic chain lengths, non-ionic surfactants, triblock copolymers, swelling agents, etc. also, post-synthesis treatments (e.g., silanation, grafting, surface functionalization, ion-exchange, immobilization of homogeneous catalysts and deposition of metal nanoclusters) could be employed to further improve the textural properties of the materials and/or modify their surface chemistry.
Ying at col. 8, line 62- col. 9, line 3 (emphasis added).
Ying teaches the following working Example 1:
Example 1
Synthesis of H-YMCM-41 - 0.79 g of H-Y (Zeolyst CBV-720 Si/Al=15) were stirred in 50 mL of a 0.37 M NHOH solution containing 0.55g of CTAB, for 20 minutes, after which time the synthesis mixture was hydrothermally treated at 150° C. for 10 hours. The solid was filtered, washed, and finally ramped in nitrogen at 5°C/min until 550°C., and then switched to air for 4 hours. Similar conditions were used to calcine all of the samples.
Alternatively, 1 g of H-Y (Zeolyst CBV-720 Si/Al=15) was stirred for in 30 mL of a 0.09 M tetramethylammonium hydroxide (TMA-OH) solution. Then 0.5 g of cetyltrimethylammonium bromide (CTAB) was added. After 30 minutes of stirring the suspension was hydrothermally treated for 20 hours at 150° C. Structural parameters are presented in Table 1.
Ying at col. 14, lines 39-52 (emphasis added).
X. Zhang et al. 126 Energy, 677-688 (2017) (“Zhang”)
Zhang teaches in aqueous solution above 120 °C, urea hydrolyzes to form ammonia, carbon dioxide, and water. Zhang at page 678.
F. Tian et al., 83 Catalyst Communications, 66-69 (2016) (“Tian”)
Tian supplements Zhang and teaches a facile and moderate method to achieve hierarchical zeolite beta, where urea solution is employed to provide a mild, stable and homogeneous alkaline media (pH = 9.25–9.58), where the alkalinity was provided by ammonia, the product of the hydrolysis reaction of urea solution under controlled conditions. Tian at page 66, col. 2. In this regard, note that Garcia-Martinez teaches that the pH of the reaction mixture was maintained at [Symbol font/0x7E]9–11 to avoid desilication. Garcia-Martinez at pages 987-988.
Obviousness Rationale
Independent claim 2 is obvious over the cited reference combination because one of ordinary skill is motivated to modify Garcia-Martinez process by replacing cetyltrimethylammonium bromide with a branched isomer of cetyltrimethylammonium bromide as the supramolecular template so as to arrive at each and every limitation of claim 2:
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One of ordinary skill is so motivated, and has a reasonable expectation of success, because Garcia-Martinez motivates one of ordinary skill to explore different supramolecular templates in teaching that the size of these mesopores can be nicely controlled by using surfactant molecules of different (alkyl) lengths. Garcia-Martinez at pages 988-989.
Ying similarly provides such motivation in teaching that
The mesopore size and architecture may also be conveniently tuned by well-known techniques, such as the use of surfactants with different aliphatic chain lengths . . .
Ying at col. 8, line 62- col. 9, line 3 (emphasis added).
The obviousness rationale is substituting equivalents known for the same purpose. MPEP § 2144.06(II) (citing Smith v. Hayashi, 209 USPQ 754 (Bd. of Pat. Inter. 1980)). The proposed modification of Garcia-Martinez represents a simple substitution of one known supramolecular template for another to obtain the predictable result of mesostructured zeolite Y. MPEP 2143(I)(B). Each and every claim 2 limitation is met by practice of Garcia-Martinez as proposed above.
Claim 24 is obvious because the concentration of ammonium hydroxide in Garcia-Martinez’s above-cited synthesis of synthesis of mesoporous zeolite Y crystals is 0.13 weight percent of Garcia-Martinez’s aqueous suspension, which falls within the claim 24 range. See Garcia-Martinez at pages 987-988 (employing 64 mL of a 0.37 M solution of NH4OH).
Claim 25 is obvious as above, in further view of X. Zhang et al. 126 Energy, 677-688 (2017) (“Zhang”), for the following reasons. Claim 25 recites:
25. The method as in claim 2, wherein the alkaline reagent is urea, wherein during hydrothermal treatment, urea reacts to form ammonium hydroxide, thereby controlling hydrothermal treatment.
Zhang teaches in aqueous solution above 120 °C, urea hydrolyzes to form ammonia, carbon dioxide, and water. Zhang at page 678. One of ordinary skill is motivated by Zhang’s teaching that “[t]he hydrolysis of urea to ammonia proceeds rapidly above a temperature of approximately 120 °C” (Zhang at page 678, col. 1) to employ urea in the above-proposed modification of Garcia-Martinez (which operates in aqueous solution at above 120 °C) as a convenient source of the required ammonia, thereby meeting the further limitations of claim 25.
Claim 27 is obvious because Garcia-Martinez teaches calcination of the mesoporous zeolite Y crystals before catalytic testing; that is Garcia-Martinez teaches the following calcination:
In order to remove the occluded templates, the dried product was heated in a nitrogen atmosphere from room temperature to 550 °C (at a ramping rate of 5 °C min-1), and kept at 550 °C for 2 hours.
Garcia-Martinez at page 988, col. 1.
Claims 28, 29, and 33 are obvious because in Garcia-Martinez’s above-cited synthesis of synthesis of mesoporous zeolite Y crystals the parent crystalline microporous material zeolite Y, which has an FAU framework. See Claim Interpretation above.
The further limitations of claim 34 are clearly met by the proposed modification of Garcia-Martinez.
The further limitations of claims 35 and 36 are met by the proposed modification of Garcia-Martinez, where the recited “constituent” in claims 35 and 36 refers to the “a quaternary phosphonium moiety and a constituent group” of base claim 2. See § 112(b) rejection of claims 35 and 36 above.
Applicant’s Argument
Applicant argues that Regarding claim 2, there is no proper motivation to substitute the surfactant used in Tempelman for those in Garcia-Martinez and Ying. Tempelman concerns a bottom-up approach where structures are formed from a mixture of zeolite precursors (NaAlO2 and sodium silicate) grown around a seed crystal in the presence of a surfactant. In contrast, Garcia-Martinez and Ying start with an already formed FAU zeolite, which is subject to a top-down mesoporous synthesis approach using an alkaline reagent. Reply (3/18/2026) at page 17. Applicant argues that there is no suggestion that the dimensions of the surfactant in Garcia-Martinez and Ying are considered to be relative to the dimensions of the pores of the parent crystalline microporous material, such that diffusion therein is constrained, which contributes to the method during hydrothermal treatment, where dissolving/incising parent crystalline microporous material into oligomeric units of the parent crystalline microporous material is followed by forming a solid hierarchically ordered mesostructure. Reply (3/18/2026) at page 17.
This argument is not persuasive because they do not address the reasoning of the above § 103 rejection, modified from the previous Office action in view of Applicant’s amendments. As stated above, one of ordinary skill is motivated to modify Garcia-Martinez process by replacing cetyltrimethylammonium bromide with a branched isomer of cetyltrimethylammonium bromide as the supramolecular template so as to arrive at each and every limitation of claim 2.
Non-Statutory Double Patenting
The nonstatutory double patenting rejection is based on a judicially created doctrine grounded in public policy (a policy reflected in the statute) so as to prevent the unjustified or improper timewise extension of the “right to exclude” granted by a patent and to prevent possible harassment by multiple assignees. A nonstatutory double patenting rejection is appropriate where the conflicting claims are not identical, but at least one examined application claim is not patentably distinct from the reference claim(s) because the examined application claim is either anticipated by, or would have been obvious over, the reference claim(s). See, e.g., In re Berg, 140 F.3d 1428, 46 USPQ2d 1226 (Fed. Cir. 1998); In re Goodman, 11 F.3d 1046, 29 USPQ2d 2010 (Fed. Cir. 1993); In re Longi, 759 F.2d 887, 225 USPQ 645 (Fed. Cir. 1985); In re Van Ornum, 686 F.2d 937, 214 USPQ 761 (CCPA 1982); In re Vogel, 422 F.2d 438, 164 USPQ 619 (CCPA 1970); In re Thorington, 418 F.2d 528, 163 USPQ 644 (CCPA 1969).
Non-Statutory Double Patenting Rejection over R. Parsapur et al., US 12,600,736 (2026) (US 17/875,671 (Jul. 5, 2022))
Claims 2, 5-15, 23-25, 27-29, and 31-36 are rejected on the ground of non-statutory double patenting as being unpatentable over respective conflicting claims 1-17 (of R. Parsapur et al., US 12,600,736 (2026), US 17/875,671 (2022).
The Conflicting method claims anticipate the instant method claims because each “hierarchically ordered zeolite having FAU framework” genus of conflicting dependent claims completely falls within the broader “hierarchically ordered crystalline microporous material” genera of the instant claims (i.e., the conflicting claim recite a method of synthesizing a subgenus of the instant claims) and the conflicting claims recite the same method steps (using the same alkaline reagent and supramolecular template) as the instant claims. Note that the same working examples are present in the instant specification and the conflicting specification.
Terminal Disclaimer
A timely filed terminal disclaimer in compliance with 37 CFR 1.321(c) or 1.321(d) may be used to overcome an actual or provisional rejection based on nonstatutory double patenting provided the reference application or patent either is shown to be commonly owned with the examined application, or claims an invention made as a result of activities undertaken within the scope of a joint research agreement. See MPEP § 717.02 for applications subject to examination under the first inventor to file provisions of the AIA as explained in MPEP § 2159. See MPEP § 2146 et seq. for applications not subject to examination under the first inventor to file provisions of the AIA . A terminal disclaimer must be signed in compliance with 37 CFR 1.321(b).
The filing of a terminal disclaimer by itself is not a complete reply to a nonstatutory double patenting (NSDP) rejection. A complete reply requires that the terminal disclaimer be accompanied by a reply requesting reconsideration of the prior Office action. Even where the NSDP rejection is provisional the reply must be complete. See MPEP § 804, subsection I.B.1. For a reply to a non-final Office action, see 37 CFR 1.111(a). For a reply to final Office action, see 37 CFR 1.113(c). A request for reconsideration while not provided for in 37 CFR 1.113(c) may be filed after final for consideration. See MPEP §§ 706.07(e) and 714.13.
The USPTO Internet website contains terminal disclaimer forms which may be used. Please visit www.uspto.gov/patent/patents-forms. The actual filing date of the application in which the form is filed determines what form (e.g., PTO/SB/25, PTO/SB/26, PTO/AIA /25, or PTO/AIA /26) should be used. A web-based eTerminal Disclaimer may be filled out completely online using web-screens. An eTerminal Disclaimer that meets all requirements is auto-processed and approved immediately upon submission. For more information about eTerminal Disclaimers, refer to www.uspto.gov/patents/apply/applying-online/eterminal-disclaimer.
Applicant’s Remarks
Applicant states that upon indication of allowable subject matter, Applicant will submit a timely filed terminal disclaimer in order to overcome this ground of rejection. Reply (3/18/2026) at page 13.
Subject Matter Free of the Art of Record
Subject to the above § 112 rejections and double patenting rejection, claims 5-15, 23, 31 and 32 are free of the art of record.
Claims 5-15
Claims 5-15 are free of the art of record for the following reasons. Each of claims 5-15 requires the step of including in the aqueous suspension of at least one of:
ionic co-solute is selected from the group consisting of CO32-, SO42-, S2O32-, H2PO4-, F-, Cl-, Br-, NO3-, I-, ClO4-, SCN- and C6H5O8-3.
This limitation distinguishes over the art of record. The closest art of record is C. Garcia-Martinez et al., 2 Catalyst & Scientific Technology, 987-994 (2012) (“Garcia-Martinez”) and/or J. Ying et al., US 7,589,041 (2009) (“Ying”), as discussed in detail above. Neither Garcia-Martinez nor Ying provides any teaching regarding an ionic co-solute.
The art of record does not motivate one of ordinary skill to perform Garcia-Martinez’s synthesis of mesoporous zeolite Y and also include in the Garcia-Martinez aqueous suspension “ionic co-solute is selected from at least one of CO32-, SO42-, S2O32-, H2PO4-, F-, Cl-, Br-, NO3-, I-, ClO4-, SCN- and C6H5O8-3”.
Claims 23, 31 and 32
Claim 23, 31 and 32 are free of the art of record for the following reasons. The closest art of record to claim 23 is C. Garcia-Martinez et al., 2 Catalyst & Scientific Technology, 987-994 (2012) (“Garcia-Martinez”) and/or J. Ying et al., US 7,589,041 (2009) (“Ying”) in view of secondary reference C. Tempelman et al., 139 Fuel Processing Technology, 248-258 (2015) (“Tempelman”);.
C. Garcia-Martinez et al., 2 Catalyst & Scientific Technology, 987-994 (2012) (“Garcia-Martinez”)
Garcia-Martinez teaches a surfactant-based technique that allows precisely controlled mesoporosity to be introduced within a wide range of zeolite crystals (i.e. mesostructuring), e.g. FAU, MOR and MFI of various Si/Al ratios, while maintaining the chemical and physical properties of the zeolites (i.e. microporosity, crystallinity, acidity, etc.). Garcia-Martinez at page 987, col. 2.
Garcia-Martinez further teaches that fluid catalytic cracking catalysts made from the mesostructured Y zeolites demonstrate significant improvement in product selectivity as a result of reduced limitation in reactant and product diffusion. Garcia-Martinez at Abstract; Id. at page 933, col. 2.
Garcia-Martinez teaches a surfactant-based technique that allows precisely controlled mesoporosity to be introduced within a wide range of zeolite crystals (i.e., mesostructuring), e.g. FAU, MOR and MFI of various Si/Al ratios, while maintaining the chemical and physical properties of the zeolites (i.e. microporosity, crystallinity, acidity, etc.). Garcia-Martinez at page 987, col. 2.
Garcia-Martinez teaches synthesis of mesoporous zeolite Y crystals as follows:
Experimental
Syntheses
In a typical synthesis, 1.00 g of a Y material (Zeolyst CBV720 with Si/Al = 15) in 64 mL of a 0.37 M solution of NH4OH containing 0.70 g of cetyltrimethyl ammonium bromide (CTAB) was stirred for 20 min. The mixture was next heated at 150 °C under autogenous pressure for 10 h. The solid was filtered, washed, and dried. Close to 100% recovery was observed, and there was no significant leaching of Si or Al species into the filtrate. Alternatively, other bases such as NaOH, Na2CO3 or tetrapropylammonium hydroxide (TPAOH) could be used. The pH of the reaction mixture was maintained at [Symbol font/0x7E]9–11 to avoid desilication.
. . .
In order to remove the occluded templates, the dried product was heated in a nitrogen atmosphere from room temperature to 550 °C (at a ramping rate of 5 °C min-1), and kept at 550 °C for 2 hours. Next, the atmosphere was switched to air for 2 hours to remove any residual carbonaceous species. In order to convert the mesostructured NH4-Y (CBV300) sample to a typical USY, the rived sample (with template inside) was heated instead at 550 °C in 100% steam for 2 hours, followed by heating at 550 °C for another 2 hours in flowing air to remove any carbonaceous residue.
Garcia-Martinez at pages 987-988 (emphasis added). Garcia-Martinez’s above experimental can be schematically summarized as follows:
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As discussed above in Claim Interpretation, zeolite Y is, per claim 1, a “parent zeolite having FAU framework having micropores of 7.4 angstroms”. Garcia-Martinez teaches the mesostructured zeolite USY prepared by calcination of the above zeolite product, is “highly mesostructured” but not ordered. Garcia-Martinez at page 992, col. 1.
Garcia-Martinez’s further teaches that:
The observations described above suggest that the introduction of controlled mesoporosity into crystalline zeolites proceeds possibly through a surfactant-assisted crystal rearrangement mechanism. Fig. 3 illustrates a plausible scheme of the critical steps in this process. Under the basic reaction conditions (pH E 10.5), some of the Si–O–Si bonds are broken to offer some flexibility in the crystalline structure, and yield negatively charged sites in the zeolite framework that attract cationic surfactants. Electrostatic interactions between these negatively charged sites and the positively charged surfactants, and self-assembly of surfactant cations to form micelles within the zeolite crystals (so as to minimize the interaction of hydrophobic surfactant tails with the aqueous solution) cause the crystal structure to rearrange to form mesopores around the micelles.
Garcia-Martinez at page 989, col. 2. Garcia-Martinez’s above stated mechanism for introduction of mesoporosity into crystalline zeolites (what happens in the reaction vessel) is similar to that taught by the instant specification. Specification at pages 26-27, [0053].
J. Ying et al., US 7,589,041 (2009) (“Ying”)
Ying is cited here to supplement Garcia-Martinez. Ying appears to be a patent based on Garcia-Martinez’s published work.
Ying teaches a method of preparing a mesostructured zeolite comprising: a) adding a zeolite to a medium comprising an acid or base, and optionally a surfactant; b) adding a surfactant to the medium from Step a) if it is not there already; c) optionally adding a swelling agent to the medium from step b); d) optionally hydrothermally treating the medium from step b) or c); and e) washing and drying the resulting material. Ying at col. 2, lines 54-61.
Ying teaches that the mesostructured zeolite is useful as a catalyst. Ying at col. 4,lines 16-20.
Ying teaches that the zeolite is selected from the group consisting of faujasite (FAU), mordenite (MOR), and ZSM-5 (MFI).
Ying teaches that the base is an alkali hydroxide, alkaline earth hydroxide, NH-OH or a tetralkylammonium hydroxide. In a further embodiment, the base is NaOH, NHOH, or tetramethylammoniumhydroxide. Ying at col. 3, lines 6-10.
Ying teaches that the surfactant is an alkylammonium halide and in a further embodiment, the surfactant is a cetyltrimethylammonium bromide (CTAB) surfactant. Ying at col. 3, lines 13-14.
Ying teaches that:
The mesopore size and architecture may also be conveniently tuned by well-known techniques, such as the use of surfactants with different aliphatic chain lengths, non-ionic surfactants, triblock copolymers, swelling agents, etc. also, post-synthesis treatments (e.g., silanation, grafting, surface functionalization, ion-exchange, immobilization of homogeneous catalysts and deposition of metal nanoclusters) could be employed to further improve the textural properties of the materials and/or modify their surface chemistry.
Ying at col. 8, line 62- col. 9, line 3 (emphasis added).
Ying teaches the following working Example 1:
Example 1
Synthesis of H-YMCM-41 - 0.79 g of H-Y (Zeolyst CBV-720 Si/Al=15) were stirred in 50 mL of a 0.37 M NHOH solution containing 0.55g of CTAB, for 20 minutes, after which time the synthesis mixture was hydrothermally treated at 150° C. for 10 hours. The solid was filtered, washed, and finally ramped in nitrogen at 5°C/min until 550°C., and then switched to air for 4 hours. Similar conditions were used to calcine all of the samples.
Alternatively, 1 g of H-Y (Zeolyst CBV-720 Si/Al=15) was stirred for in 30 mL of a 0.09 M tetramethylammonium hydroxide (TMA-OH) solution. Then 0.5 g of cetyltrimethylammonium bromide (CTAB) was added. After 30 minutes of stirring the suspension was hydrothermally treated for 20 hours at 150° C. Structural parameters are presented in Table 1.
Ying at col. 14, lines 39-52 (emphasis added).
Differences between Garcia-Martinez/Ying and the Claims
Garcia-Martinez and Ying differs from the claims 23, 31, and 32 to the extent that Garcia-Martinez’s supramolecular template, cetyltrimethylammonium bromide (CTAB), does not meet the limitations of:
claim 23 . . . the supramolecular template is dimethyloctadecyl(3-trimethoxysilyl-propyl)-ammonium . . .
claim 31 . . . the supramolecular template is [2,3-bis(dodecanoyloxy)-propyl](3-(trimethoxysilyl)propyl)-dimethylammonium . . .
claim 32 . . . the supramolecular template is dimethylhexadecyl[3-(trimethoxysilyl)propyl] ammonium . . .
The respective structure of the claim 23, 31, and 32 templates are:
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C. Tempelman et al., 139 Fuel Processing Technology, 248-258 (2015) (“Tempelman”)
Tempelman teaches investigated the feasibility of using dimethyloctadecyl-(3-trimethoxysilylpropyl)-ammonium chloride (TPOAC) in the direct synthesis of hierarchical zeolite Y for use in FCC composite catalyst. Tempelman at page 249, col. 1. Tempelman teaches that the composite catalysts show excellent catalytic performance in the fluid catalytic cracking (FCC) of a vacuum gas oil (VGO). The catalytic data indicate that the relatively weak acid sites are responsible for the FCC activity. Tempelman at page 257, col. 1.
Tempelman teaches that mesoporous zeolite Y was synthesized by using an amphiphilic organosilane dimethyloctadecyl-(3-trimethoxysilylpropyl)-ammonium chloride (TPOAC). Tempelman at Abstract.
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Tempelman discloses the following procedure to prepare mesoporous zeolite Y:
2.1. Zeolite synthesis
For the synthesis of reference bulk zeolite Y, a seed gel was prepared by dissolving 4.04 g NaOH and 2.0 g NaAlO2 in 19.97 g water. Then, 22.80 g sodium silicate solution (Prolabo, 25.5–26.5% SiO2) was added dropwise under vigorous stirring. The resulting seed gel (gel A) was aged overnight at room temperature.
In a second round bottom flask, a feedstock gel (gel B) was prepared. After dissolving 0.04 g NaOH and 3.31 g NaAlO2 in 33.19 g water, 35.56 g sodium silicate (26 wt.% in water, Prolabo) was added dropwise under vigorous stirring. The Si/Al ratio of the feedstock gel was varied between 2.5 and 5.0 by adjusting the amount of sodium aluminate.
To prepare the final synthesis gel, an amount of 4.46 g of the aged seed gel A was added to the feedstock gel B under vigorous stirring and was stirred for another hour. The resulting gel was transferred into a 125 mL Teflon-lined stainless-steel autoclave and heated in a static oven at 373 K for 24 h.
The gel for obtaining mesoporous zeolite Y was prepared in the same way as described above.
Prior to the hydrothermal step, dimethyloctadecyl-(3-trimethoxysilylpropyl)-ammonium chloride (TPOAC, ABCR, 60 wt.% in methanol) was added dropwise to the synthesis gel; this gel was further stirred for 4 h. The Si/TPOAC ratio was varied between 10 and 125. The gels were then hydrothermally treated at 373 K for 72 h.
The solid materials were recovered by filtration of the suspension, followed by washing with copious amounts of water. To remove TPOAC, the solids were calcined in artificial air (20/80 (v%/v%) O2/He). The materials are denoted by FAU(x, y) with x being the SiO2/ TPOAC ratio (∞, 125, 45, 20, 10) and y the Si/Al ratio (2.5, 3.5, 5.0) in the starting gel.
Tempelman at page 249, col. 1 (emphasis added). Per above, Tempelman therefore teaches adding seed gel A to feedstock B and to this mixture further adding dimethyloctadecyl-(3-trimethoxysilylpropyl)-ammonium chloride (TPOAC) (the instant specification working example’s supramolecular template) to form an aqueous suspension in the form of a synthesis gel. Per above, Tempelman further teaches, the synthesis gel was hydrothermally treated at 373 K (i.e., 100 ˚C) for 72 h and the solid materials were recovered by filtration of the suspension, followed by washing.
Tempelman teaches that texture analysis of FAU (45, 5.0) shows that this material contains both micropores and mesopores and the TEM images of FAU (45, 5.0) reveal that the mesopores are well integrated into the primary zeolite particles (Fig. 6c). Tempelman at page 252, col. 1.
The Claims Art not Obvious over the Cited Art
Claims 23, 31 and 32 are not obvious over the cited reference combination because one of ordinary skill, seeking catalytic cracking catalysts, does not have a reasonable expectation of success that modification of Garcia-Martinez’s process by replacing cetyltrimethylammonium bromide with the any of the claimed supramolecular templates will produce a catalytically or otherwise useful zeolite or the claimed “solid hierarchically ordered mesostructured having mesoporous order”. MPEP § 2143.02.
The lack of a reasonable expectation of success is because Tempelman’s process for forming a hierarchically ordered FAU zeolite is much different than that of Garcia-Martinez in view of the art’s unpredictability. That is, Tempelman teaches that a zeolite gel (i.e., a mixture of NaAlO2 and sodium silicate), in the presence of a seed crystal, base NaOH, and template dimethyloctadecyl(3-trimethoxysilylpropyl)-ammonium (TPOAC), condenses to form a hierarchically ordered FAU zeolite. Tempelman at page 252, col. 1. On the other hand, Garcia-Martinez mixes an already formed FAU zeolite (i.e., Y material (Zeolyst CBV720) with Si/Al = 15) in a solution of NH4OH containing the template cetyltrimethyl ammonium bromide (CTAB) to form the a hierarchically ordered FAU zeolite. The art of supramolecular templating in mesoporous zeolite synthesis is nascent, unpredictable and challenging. For example, Li teaches that the synthesis mechanisms of zeolites by nucleation and crystallization involve many time-dependent chemical processes that take place in multiple phases and, consequently, the targeted crystallization of a specific zeolite structure cannot be achieved. C. Li et al., 57 Angew. Chem. Int. Ed., 15330-15353 (2018) (“Li”) (see Li at 15331, col. 1). Li teaches that the preparation of hierarchical zeolites containing well-defined mesoporosity is an outstanding challenge in catalysis. Li at page 15349, col. 2.
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.
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ALEXANDER R. PAGANO
Examiner
Art Unit 1692
/ALEXANDER R PAGANO/Primary Examiner, Art Unit 1692
1 The specification does not define “micropores” or “mesopores”. As discussed in the previous Office action, the art teaches that according to the definition of the International Union of Pure and Applied Chemistry (IUPAC), porous materials can be classified into three categories according to their pore size: micropores (< 2 nm), mesopores (2–50 nm), and macropores (> 50 nm). H. Que et al., 3 Emergent Materials, 381-405 (2020) (page 381, col. 1).
2 As a general rule preamble language is not treated as limiting. Arctic Cat Inc. v. GEP Power Prods., Inc., 919 F.3d 1320, 1327 (Fed. Cir. 2019). Exceptions arise where, for example, the preamble (1) recites essential structure or steps; (2) provides antecedent basis for terms in the claim body; or (3) was relied on during prosecution to distinguish the claimed invention from prior art. Catalina Mktg. Int’l, Inc. v. Cool savings.com, Inc., 289 F.3d 801, 808 (Fed. Cir. 2002). If the body of a claim fully and intrinsically sets forth all of the limitations of the claimed invention, and the preamble merely states, for example, the purpose or intended use of the invention, rather than any distinct definition of any of the claimed invention’s limitations, then the preamble is not considered a limitation and is of no significance to claim construction. MPEP § 2112.02(II) (citing Rowe v. Dror, 112 F.3d 473, 478, 42 USPQ2d 1550, 1553 (Fed. Cir. 1997) ("where a patentee defines a structurally complete invention in the claim body and uses the preamble only to state a purpose or intended use for the invention, the preamble is not a claim limitation")).
3 In this regard, the mental process of “selection” of a particular ionic co-solute, itself, cannot control “the shape of the micelles”. Further, this mental step limitation cannot be given patentable weight because the mental step(s)/abstract idea of selecting is not functionally related to the claim 5 method. MPEP § 2111.05; (citing In re Ngai, 367 F.3d 1336, 1339 (Fed. Cir. 2004). That is, the practice of claim 5 remains unchanged regardless of whether or not the required “control” has been achieved.
4 As discussed in the MPEP a lack of clarity could arise where a claim refers to "said lever" or "the lever," where the claim contains no earlier recitation or limitation of a lever and where it would be unclear as to what element the limitation was making reference. MPEP § 2173.05(e). Similarly, if two different levers are recited earlier in the claim, the recitation of "said lever" in the same or subsequent claim would be unclear where it is uncertain which of the two levers was intended. MPEP § 2173.05(e). A claim which refers to "said aluminum lever," but recites only "a lever" earlier in the claim, is indefinite because it is uncertain as to the lever to which reference is made. MPEP § 2173.05(e).
5 The proposed amendment attempts to identify the broadest enabled subject taking into account supporting written description support per § 112(a). Certain language in strike-out/italic text is suggested as removed because it is superfluous in view of the proposed amendment and/or per Claim Interpretation above.
6 Zeolites are hydrated aluminosilicate that is made from tetrahedral alumina (AlO45-) and silica (SiO44-) through interlinkage of oxygen atoms. T. Derbe et al., Hindawi Advances in Materials Science and Engineering (2021).
7 Luan is a review published after the instant effective filing date. In general, the examiner should not use post-filing date references to demonstrate that a patent is not enabled. MPEP § 2164.05(a). However, exceptions to this rule could occur if a later-dated reference provides evidence of what one skilled in the art would have known on or before the effective filing date of the patent application. MPEP § 2164.05(a). If a publication demonstrates that those of ordinary skill in the art would find that a particular invention was not enabled years after the filing date, the publication would be evidence that the claimed invention was not possible at the time of filing. MPEP § 2164.05(a).
8 While there is a presumption that an adequate written description of the claimed invention is present in the specification as filed, a question as to whether a specification provides an adequate written description may arise in the context of an original claim. MPEP § 2163.03 (V) (citing In re Wertheim, 541 F.2d 257, 262, 191 USPQ 90, 96 (CCPA 1976)). An original claim may lack written description support when (1) the claim defines the invention in functional language specifying a desired result but the disclosure fails to sufficiently identify how the function is performed or the result is achieved or (2) a broad genus claim is presented but the disclosure only describes a narrow species with no evidence that the genus is contemplated. MPEP § 2163.03 (V) (citing Ariad Pharms., Inc. v. Eli Lilly & Co., 598 F.3d 1336, 1349-50 (Fed. Cir. 2010) ("[e]ven if a claim is supported by the specification, the language of the specification, to the extent possible, must describe the claimed invention so that one skilled in the art can recognize what is claimed”).
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