DETAILED ACTION
Notice of Pre-AIA or AIA Status
The present application, filed on or after March 16, 2013, is being examined under the first
inventor to file provisions of the AIA .
Election/Restrictions
Applicant’s election without traverse of Group I, claims 1-12, in the reply filed on 03/26/2026 is acknowledged.
Claim Objections
Claims 1-12 are objected to because of the following informalities:
Regarding claim 1, the term “smaller than” is likely intended to be “less than”.
Claims 2-12 depend on claim 1 and thus are also objected to.
Appropriate correction is required.
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(b):
(b) CONCLUSION.—The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the inventor or a joint inventor regards as the invention.
The following is a quotation of 35 U.S.C. 112 (pre-AIA ), second paragraph:
The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the applicant regards as his invention.
Claims 1-12 are rejected under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), second paragraph, as being indefinite for failing to particularly point out and distinctly claim the subject matter which the inventor or a joint inventor (or for applications subject to pre-AIA 35 U.S.C. 112, the applicant), regards as the invention.
Regarding claim 1, the phrase “Me/A1” is unclear and the term “A1” has insufficient antecedent basis for this limitation in the claim. The lack of clarity is due the term “A1” possibly referring to either the alkali metal “AOH” or the aluminum component, where aluminum is possibly being referred to as its molecular symbol “Al” with a typo for the “l”. Additionally it is unclear from the claim if the Me/A1 ratio is referring to the ratio in the reaction mixture or the ratio of the two in the final CHA zeolite product. In the interest of compact prosecution and in view of the instant specification, the term Me/A1 is interpreted to be referring to the molar ratio of the first metal cation to aluminum in the final dried product, where the “1” in A1 is intended to be “Al” in the claims. This interpretation is supported by the instant specification on Pg. 19, line 20, that refers to a “Me/Al” ratio in addition to at least Example 1 on Pg. 42, line 14 that describes the produced zeolite having a Cu/Al ratio of 0.33.
Regarding claim 11, line 2, the term “the part of the transition metal” has insufficient antecedent basis. In particular, while a transition metal is included in independent claim 1, from which claim 11 depends, it is unclear what “part” of the transition metal is being referred to in claim 11. In the interest of compact prosecution, removing any transition metal is interpreted as equivalent to removing “the part of the transition metal.”
Claims 2-12 all depend from claim 1 and thus, are also rendered indefinite.
Claim Rejections - 35 USC § 103
In the event the determination of the status of the application as subject to AIA 35 U.S.C.
102 and 103 (or as subject to pre-AIA 35 U.S.C. 102 and 103) is incorrect, any correction of the
statutory basis for the rejection will not be considered a new ground of rejection if the prior art
relied upon, and the rationale supporting the rejection, would be the same under either status.
The following is a quotation of 35 U.S.C. 103 which forms the basis for all obviousness
rejections set forth in this Office action:
A patent for a claimed invention may not be obtained, notwithstanding that the
claimed invention is not identically disclosed as set forth in section 102, if the
differences between the claimed invention and the prior art are such that the claimed invention as a whole would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to which the claimed invention pertains. Patentability shall not be negated by the manner in which the invention was made.
The factual inquiries for establishing a background for determining obviousness under 35 U.S.C.
103 are summarized as follows:
1. Determining the scope and contents of the prior art.
2. Ascertaining the differences between the prior art and the claims at issue.
3. Resolving the level of ordinary skill in the pertinent art.
4. Considering objective evidence present in the application indicating obviousness or
nonobviousness.
This application currently names joint inventors. In considering patentability of the claims the examiner presumes that the subject matter of the various claims was commonly owned as of the effective filing date of the claimed invention(s) absent any evidence to the contrary. Applicant is advised of the obligation under 37 CFR 1.56 to point out the inventor and effective filing dates of each claim that was not commonly owned as of the effective filing date of the later invention in order for the examiner to consider the applicability of 35 U.S.C. 102(b)(2)(C) for any potential 35 U.S.C. 102(a)(2) prior art against the later invention.
Claims 1-3, 6, 10, and 12 are rejected under 35 U.S.C. 103 as being unpatentable over Xiao et al. (CN101973562A English; cited in IDS dated 09/27/2023) in view of Bull et al. (US20160101411A1).
Regarding claim 1, Xiao teaches the preparation of a CHA molecular sieve containing copper and an amine as a templating agent where the reaction is carried out in a single reaction kettle (Abstract; Claim 1; Pg. 3, Summary of Invention). Xiao teaches the reaction mixture produced prior to the final crystallization has a molar ratio of Na20: Al2O3: SiO2: H2O: Cu-R, where Cu = R, is 3-60: 1: 8- 500: 20-1000: 2-300 (Claim 1). Xiao teaching the reaction occurring in a single vessel with targeted range of copper and alkali metal (i.e. Na2O) meets the limitation “targeted contents of copper, iron, zinc, and mixtures thereof as well as targeted contents of alkali metals.” The term “targeted” was interpreted in view of the instant specification that describes the synthesis providing molecular sieves of the CHA-type with targeted contents of copper oxide and alkali metals (see Pg. 8, lines 22-29 in the instant specification).
Xiao teaches the synthesis includes a copper source, a silicon source, an aluminum source, water, sodium hydroxide, and an organic amine template comprising tetraethylenepentamine (Pg. 3, Summary of Invention). Xiao teaches the silicon source includes silica sol (i.e. contains SiO2) and the aluminum source includes sodium aluminate (Pg. 3, Summary of Invention; Pg. 4, Embodiment 1). These are consistent with non-molecular sieve sources of silicon and aluminum listed in claims 2 and 3 and meet the limitation required by claim 1.
Xiao teaches sodium aluminate is dissolved in water, followed by addition of cupric salt and organic amine with stirring prior to adding sodium hydroxide and silica sol with stirring, after which the reaction mixture is crystallized and collected (Claim 1; Pg. 3, Summary of Invention; Pg. 4, Embodiment 1). Xiao teaching the contents are stirred between and during the addition of reagents is equivalent to the term “crystallization” in steps ac), ae), and bb) where the instant specification describes crystallization as occurring at 20 to 110 °C with stirring (se Pg. 17, lines 7-16).
Xiao teaches the final reaction mixture obtained contains Na2O: Al2O3: SiO2: H2O: Cu-R, where Cu = R, is 3-60: 1: 8- 500: 20-1000: 2-300, wherein R is an organic amine template (Claim 1).
Converting the ranges of Xiao to the ranges required by the claims provides the following:
Ratio
Xiao et al.
Claims
SiO2/Al2O3
8 to 500
about 10 to about 35
SiO2/AOH
0.65 to 292
about 1 to about 2
SiO2/H2O
0.008 to 25
about 0.03 to about 0.2
OSDA1/SiO2
0.002 to 18.75
about 0.01 to about 0.1
Me/OSDA1
1
equal to or smaller than 1.0
In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. MPEP 2144.05 (I). In the instant case, the ranges taught by Xiao (SiO2/Al2O3 = 8 to 500; SiO2/AOH = 0.65 to 292; SiO2/H2O = 0.008 to 25; OSDA1/SiO2 = 0.002 to 18.75; and Me/OSDA1 1) overlaps with the claimed ranges (SiO2/Al2O3 = about 10 to 35; SiO2/AOH = about 1 to about 2; SiO2/H2O = about 0.03 to 0.2; OSDA1/SiO2 = about 0.01 to 0.1; and Me/OSDA1 equal to or smaller than 1.0). Therefore, the ranges in Xiao renders obvious the claimed range.
Regarding the limitation “aa) mixing first portions of the components a), b) and c) according to step (I); ab) optionally adding component g) according to step (I) ac) crystallization of the mixture in a reactor; ad) adding second portions of the components a), b) and c) and components d),” the disclosure of Xiao differs from the instant claims in that Xiao mixes the aluminum source, metal, organic templating agent, and water prior to adding a mixed solution of silica source and alkali metal source where the claims mix the silicon, aluminum, alkali metal hydroxide, and water prior to adding the remaining amounts of those reagents in addition to adding the first organic structure directing agent and cations of the first metal.
Further, regarding the limitation “wherein in step (II)(aa) 30 to 75 mol-% of the non-molecular sieve source of silicon, 80 to 100 mol-% of the non-molecular sieve source of aluminum, 40 to 100 mol-% of the alkali metal hydroxide AOH and 30 to 90 mol-% of water are added, and wherein in step (II)(ad) 70 to 25 mol-% of the non-molecular sieve source of silicon, 20 to 0 mol-% of the non-molecular sieve source of aluminum, 60 to 0 mol-% of the alkali metal hydroxide AOH and 70 to 10 mol-% of water are added, so that the mixture obtained after the completion of step (II)(ad) contains 100 mol- % each of the non-molecular sieve source of silicon and aluminum, the alkali metal hydroxide AOH and water, and the molar ratios of the components a), b) c), d), e) and optionally g), h) and/or i) of step (I) obtained after the completion of step (II)(ad) are the ones given above,” Xiao differs from the instant claims in that Xiao adds all the reagents at once rather than adding a percentage of the reagents at differ times prior to obtaining the final reaction composition as claimed.
However, it has been established that selection of any order of performing process steps is prima facie obvious in the absence of new or unexpected results. See MPEP. 2144.04.C. Xiao teaches providing a reaction mixture comprising all of the components as claimed in the amounts required by the claim. Accordingly, in the absence of new or unexpected results, despite the instant invention adding reagents at different proportions to arrive at a reaction mixture, the reaction mixture obtained is the same as the reaction mixture taught by Xiao and describes overlapping contents of all the required components taught by Xiao. Therefore, despite the difference in the order of performing process steps between the prior art Xiao and the instant invention, the selection of any order of performing process steps is considered to be prima facie obvious in the absence of new or unexpected results and the method of Xiao renders obvious the instantly claimed method.
The claim further requires the “Me/A1 ratio is smaller than 0.5”. As noted above in the 112(b) section, this limitation is interpreted as referring to the molar ratio of the first metal cation to aluminum in the final dried product. Xiao does not explicitly teach this ratio.
Bull teaches a Cu-CHA catalyst that is effective at removing nitrogen oxides from gaseous streams over broad temperature ranges with hydrothermal stability at high reaction temperatures that comprises a Cu to Al ratio of about 0.25:1 to about 1:1 (Abstract; [0035]). In the case where the claimed ranges "overlap or lie inside ranges disclosed by the prior art" a prima facie case of obviousness exists. MPEP 2144.05 (I). In the instant case, the range taught by Bull (Cu:Al = 0.25 to 1) overlaps with the claimed ranges (Me:Al smaller than 0.5). Therefore, the ranges in Bull renders obvious the claimed range.
Advantageously, providing a Cu-CHA zeolite with the Cu loading and Al ratio taught by Bull prevents thermal degradation up to about 800 °C while also providing improved water resistance up to about 10% or more ([0034]).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to provide a Cu-CHA zeolite with a Cu:Al ratio between 0.25 to 1 in the product produced by the process of Xiao in order to provide a catalyst with improved thermal and water resistance as taught by Bull.
It is noted the claims describe the optional steps (I)(f)-(I)(i) and (II)(ab), with the optional addition of components (I)(f)-(I)(i) in step (II). While not indefinite, use of the word “optionally” does not constitute necessary aspects required by the claim and are not considered as required in the above rejection over Xiao in view of Bull.
Regarding claim 2, Xiao in view of Bull teach the method of claim 1.
Xiao further teaches the silicon source includes silica sol (i.e. contains SiO2) (Pg. 3, Summary of Invention; Pg. 4, Embodiment 1).
Regarding claim 3, Xiao in view of Bull teach the method of claim 1.
Xiao further teaches the aluminum source includes sodium aluminate (Pg. 3, Summary of Invention; Pg. 4, Embodiment 1).
Regarding claim 6, Xiao in view of Bull teach the method of claim 1.
Xiao further teaches the metal cation is copper (Abstract; Claim 1; Pg. 3, Summary of Invention).
Regarding claim 10, Xiao in view of Bull teach the method of claim 1.
Xiao further teaches the templating agent is selected from diethylamine, triethylene tetramine or tetraethylene pentaamine (TEPA) while teaching examples using exclusively TEPA (Pg. 3, Summary of Invention; Pg. 4, Embodiment 1).
Regarding claim 12, Xiao in view of Bull teach the method of claim 1.
Xiao further teaches the template is removed by calcining to obtain the finished product (Pg. 2, Summary of Invention).
Claim 4, 7-9, and 11 are rejected under 35 U.S.C. 103 as being unpatentable over Xiao et al. (CN101973562A English; cited in IDS dated 09/27/2023) in view of Bull et al. (US20160101411A1) and further in view of Vennestrom et al. (WO2020039074A1).
Regarding claim 4, Xiao in view of Bull teach the method of claim 1.
The claim further requires “the non-molecular sieve source of silicon and aluminum is selected from precipitated silica-alumina, amorphous silica-alumina, kaolin, amorphous mesoporous materials, and mixtures thereof,” where Xiao teaches separate silicon and aluminum sources. Bull is silent regarding the limitation.
Vennestrom teaches the preparation of a molecular sieve of the CHA-type where suitable non-molecular sieve sources of silicon and aluminum include precipitated silica-alumina, amorphous silica-alumina, kaolin, amorphous mesoporous materials and mixtures thereof (Pg. 1, lines 14-17; Pg. 6, lines 27-35).
Advantageously, the non-molecular sieve sources of silicon and aluminum taught by Vennestrom can be used as sources of both aluminum and silicon during the synthesis (Pg. 6, lines 27-35). Vennestrom teaches these sources are inexpensive and reduce production cost (Pg. 10, lines 7-15).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to provide a non-molecular sieve source of silicon and aluminum that include precipitated silica-alumina, amorphous silica-alumina, kaolin, amorphous mesoporous materials and mixtures thereof in the process of Xiao in order to provide both silicon and aluminum sources in a single reagent and reduce product cost, as taught by Vennestrom.
Regarding claim 7, Xiao in view of Bull teach the method of claim 1.
The claim further requires “the molecular sieve source of silicon and aluminum is selected from FAU, LTL, GME, LEV, AEI, LTA, OFF, CHA, ERI, and mixtures thereof,” to which Xiao and Bull are silent.
Vennestrom teaches the preparation of a molecular sieve of the CHA-type where suitable crystalline molecular sieve sources include FAU, LTL, GME, LEV, AEI, LTA, OFF, CHA, ERI, and mixtures thereof (Pg. 1, lines 14-17; Pg. 8, lines 30-37).
Advantageously, the molecular sieve sources taught by Vennestrom are less expensive molecular sieves starting materials that contain low SAR (i.e. silicon to aluminum ratio) that reduce production cost (Pg. 10, lines 7-15).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to provide a molecular sieve source selected from FAU, LTL, GME, LEV, AEI, LTA, OFF, CHA, ERI, and mixtures thereof in the process of Xiao in order to provide a less expensive molecular sieve starting material containing low SAR that reduces production cost, as taught by Vennestrom.
Regarding claims 8-9, Xiao in view of Bull teach the method of claim 1.
The claim further requires “at least one salt of one or more second metals P is selected from salts of manganese, cesium, magnesium, calcium, strontium, barium, yttrium, titanium, zirconium, niobium, iron, zinc, silver, lanthanum, cerium, praseodymium, neodymium, promethium, samarium, europium, gadolinium, terbium, dysprosium, holmium, erbium, thulium, ytterbium, lutetium, and mixtures thereof,” to which Xiao and Bull are silent.
Vennestrom teaches the preparation of a molecular sieve of the CHA-type where transition metals, including iron, and alkaline earth metals including rubidium, cesium, magnesium, calcium, strontium and barium (Pg. 16, lines 31-36; Pg. 15, lines 23-36). Vennestrom teaches the transition metal and/or alkaline earth metals can be introduced by liquid ion exchange, incipient wetness, or solid state exchange, which occurs after forming the CHA-zeolite by synthesis (Pg. 14, line 4-Pg. Pg. 15, line 36; Pg. 16, lines 4-29).
Advantageously, incorporating a transition metal or alkaline earth metal cations, including iron, rubidium, cesium, magnesium, calcium, strontium and barium, by one of the techniques taught by Vennestrom, can reduce the concentration of other cations in the framework and allow the skilled person the choice of which metal to incorporate based on the intended purpose (Pg. 16, lines 11-20). For example, transition metals, including iron, titanium, niobium, and cesium, can improve selective catalytic reduction (SCR) activity in nitrogen oxide reduction in metal-loaded molecular sieves (Pg. 25, lines 16-21; Pg. 19, lines 28-34).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to introduce a metal including iron, titanium, niobium, cesium, rubidium, magnesium, calcium, strontium and barium by liquid ion exchange, incipient wetness, or solid state exchange, after forming the CHA-zeolite in the process of Xiao in order to provide a flexible way to change the metal in the zeolite and improve performance in SCR of nitrogen oxides, as taught by Vennestrom.
Regarding claim 11, Xiao in view of Bull teach the method of claim 1.
The claim further requires “a part or all of the alkali ions and/or the part of the transition metal are removed from the molecular sieve after the separation of the molecular sieve of the CHA-type by ion- exchange,” to which Xiao and Bull are silent.
Vennestrom teaches the preparation of a molecular sieve of the CHA-type where the method further comprises removing the alkali or alkaline earth metals from the synthesized CHA-type molecular sieve by ion-exchange with ammonium and/or hydrogen (Pg. 34-35, Claim 14; ).
Advantageously, performing ion exchange is a well-recognized method for obtaining the NH4-form or H-form of the molecular sieve, which provides flexibility when incorporating metals or when performing heat treatment conversion (Pg. 12, lines 21-27).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to remove the alkali or alkaline earth metals from the synthesized CHA-type molecular sieve by ion exchange in the process of Xiao in order to provide a flexible way to further incorporate metals into the zeolite or enable heat treatment conversion, as taught by Vennestrom.
Claim 5 is rejected under 35 U.S.C. 103 as being unpatentable over Xiao et al. (CN101973562A English; cited in IDS dated 09/27/2023) in view of Bull et al. (US20160101411A1) and further in view of Martens et al. (US020180304242A).
Regarding claim 5, Xiao in view of Bull teach the method of claim 1.
The claim further requires “the alkali metal hydroxide cations in the alkali metal hydroxide AOH are a mixture of sodium cations with potassium and/or ammonium cations,” where Xiao teaches the alkali metal source is sodium hydroxide. Bull is silent regarding the limitation.
Martens teaches a one-pot synthesis of Cu-CHA where the process uses a metal hydroxide MOH, where M is selected from alkali metals including sodium and potassium (Abstract; [0020]). Martens teaches the nature of the obtained copper zeolite depends on the what metals are selected as the metal hydroxide ([0038]).
Advantageously, selecting sodium and/or potassium as the metal hydroxide provides CHA zeolite rather than different zeolite frameworks while the process of Martens provides improved flexibility and avoids expensive templates ([0041]).
Thus, prior to the effective filing date of the claimed invention, it would have been obvious to one of ordinary skill in the art to utilize sodium and/or potassium hydroxide in the process of Xiao in order to produce CHA-type zeolite rather than other zeolites without requiring expensive templates, as taught by Martens.
Conclusion
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/JORDAN W TAYLOR/Examiner, Art Unit 1738