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 .
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 (i.e., changing from AIA to pre-AIA ) 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.
Status of Claims
Claims 1, 3-7, 9-15, 17, 21-22, and 29-30 are currently under examination. Claims 23-24 and 27 are withdrawn from consideration. Claims 2, 8, 16, 18-20, 25-26 and 28 have been cancelled. Claim 1 is amended.
Continued Examination Under 37 CFR 1.114
A request for continued examination under 37 CFR 1.114, including the fee set forth in 37 CFR 1.17(e), was filed in this application after final rejection. Since this application is eligible for continued examination under 37 CFR 1.114, and the fee set forth in 37 CFR 1.17(e) has been timely paid, the finality of the previous Office action has been withdrawn pursuant to 37 CFR 1.114. Applicant's submission filed on 10/02/2025 has been entered.
Previous Grounds of Rejection
In the light of the amendments, the rejection under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), second paragraph, with respect to claims 1, 3-7, 9-15, 17, 21-22 and 29-30 is withdrawn.
Regarding claims 1, 5, 6, 7, 10 and 13, in the light of the amendments, the rejection under 35 U.S.C. 103 as being unpatentable over Henry, et.al. ( WO 2017/106916 A1; hereinafter Henry) in view of Kiemel, et.al. (US2018/0016142 A1) is amended as set forth below.
New grounds of rejections are set forth below.
Amended & New Grounds of Rejections
Claim Rejections - 35 USC § 112
The following is a quotation of the first paragraph of 35 U.S.C. 112(a):
(a) IN GENERAL.—The specification shall contain a written description of the invention, and of the manner and process of making and using it, in such full, clear, concise, and exact terms as to enable any person skilled in the art to which it pertains, or with which it is most nearly connected, to make and use the same, and shall set forth the best mode contemplated by the inventor or joint inventor of carrying out the invention.
The following is a quotation of the first paragraph of pre-AIA 35 U.S.C. 112:
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 of carrying out his invention.
Claims 1, 3-7, 9-15,17,21-24, 27 and 29-30 are rejected under 35 U.S.C. 112(a) or 35 U.S.C. 112 (pre-AIA ), first paragraph, as failing to comply with the written description requirement. The claim(s) contains subject matter which was not described in the specification in such a way as to reasonably convey to one skilled in the relevant art that the inventor or a joint inventor, or for applications subject to pre-AIA 35 U.S.C. 112, the inventor(s), at the time the application was filed, had possession of the claimed invention.
In this case, claim 1 contains subject matter of “the reactants defining a main flow along a longitudinal axis of the coated scaffold, and wherein the scaffold is configured to by redistribute the fluid in directions transverse to the main flow by changing the localized flow direction or to by splitting the flow by more than 200 m-1, …, and wherein the ex-situ catalyst particles are catalytically active in their final form prior to deposition and remain catalytically active after deposition without requiring in-situ activation” which was not described in the specification in such a way as to reasonably convey to one skilled in the relevant art that the inventor or a joint inventor, or for applications subject to pre-AIA 35 U.S.C. 112, the inventor(s), at the time the application was filed, had possession of the claimed invention.
All other claims depend directly or indirectly from the rejected claims and are, therefore, also rejected under 35 USC § 112(a) for the reasons set forth above.
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 (i.e., changing from AIA to pre-AIA ) 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.
Claims 1, 5-6, 8-9 and 11 are rejected under 35 U.S.C. 103 as being unpatentable over Henry et.al. ( WO 2017/106916 A1; hereinafter Henry) in view of Kiemel, et.al. (US2018/0016142 A1).
Regarding claim 1, Henry et al. "process for preparing a catalytically coated scaffold, comprising the steps of:
applying a catalytic liquid suspension to a surface of a scaffold to provide a coating containing catalytically reactive sites on the surface of the coated scaffold, wherein the catalytic liquid suspension comprises a liquid carrier containing a plurality of ex-situ catalyst particles, and wherein the coated scaffold has a non-line-of-sight configuration comprising a plurality of passages configured for dispersing and mixing one or more fluidic reactants during flow and reaction thereof, the reactants defining a main flow along a longitudinal axis of the coated scaffold, and wherein the scaffold is configured to by redistribute the fluid in directions transverse to the main flow by changing the localized flow direction or to by splitting the flow by more than 200 m-1, corresponding to a number of times within a given length along a longitudinal axis of the coated scaffold, and
drying the coated scaffold to remove the liquid carrier to provide a coated scaffold comprising ex-situ catalyst particles, wherein the step of applying the catalytic liquid suspension to the surface of the scaffold in step (i) is by wash-coating or dip-coating;
and wherein the aspect ratio (L/d) of the scaffold is at least 75.
Henry et al. teach “…undertaken significant research and development into alternative continuous flow chemical reactors and have identified that static mixers can be provided with a catalytic surface such that the resulting static mixer is capable of being used with a continuous flow chemical reactor. It was surprisingly found that incorporating catalytic material on the surface of additive manufactured static mixers can provide catalytic static mixers that can be configured to be readily removable and easily replaced, allow for further re-design enhancement, and provide for efficient mixing, heat transfer and catalytic reaction of reactants in continuous flow chemical reactors. The static mixers may be provided for use with in-line continuous flow reactors as inserts or as modular packages with the static mixer as an integral part of a section of the reactor tube itself.”
“Accordingly, in a first aspect there is provided a static mixer element configured as a module for a continuous flow chemical reactor chamber, wherein the static mixer element comprises a catalytically active scaffold defining a plurality of passages configured for mixing one or more fluidic reactants during flow and reaction thereof through the mixer, and wherein at least a portion of a surface of the scaffold comprises a catalytic material for providing the surface with catalytically reactive sites.”(page 2),
“there is provided a process for preparing a static mixer element for a continuous flow chemical reactor chamber, comprising the steps of: providing a static mixer element comprising a scaffold defining a plurality of passages configured for mixing one or more fluidic reactants during flow and reaction thereof through the mixer; and
applying a catalytic coating to at least a portion of the surface of the scaffold.
The step of applying the catalytic coating to at least a portion of the surface of the scaffold may comprise or consist of electrodeposition or cold spray. The catalytic coating may comprise a catalytic material selected from at least one of a metal, metal alloy, cermet and metal oxide, for providing the surface with a plurality of catalytically reactive sites. The process may comprise a step of preparing the scaffold of the static mixer by additive manufacture. The material of the scaffold may be selected from at least one of a metal, metal alloy, cermet and metal oxide.” (p-3),
“The static mixer element may be configured for enhancing mixing and heat transfer characteristics for redistributing fluid in directions transverse to the main flow, for example in radial and tangential or azimuthal directions relative to a central longitudinal axis of the static mixer element. The static mixer element may be configured for at least one of (i) to ensure as much catalytic surface area as possible is presented to the flow so as to activate close to a maximum number of reaction sites and (ii) to improve flow mixing so that (a) the reactant molecules contact surfaces of the static mixer element more frequently and (b) heat is transferred away from or to the fluid efficiently. The static mixer element may be provided with various geometric configurations or aspect ratios for correlation with particular applications. The static mixer elements enable fluidic reactants to be mixed and brought into close proximity with the catalytic material for activation. The static mixer element may be configured for use with turbulent flow rates, for example enhancing turbulence and mixing, even at or near the internal surface of the reactor chamber housing. It will also be appreciated that the static mixer element can be configured to enhance the heat and mass transfer characteristics for both laminar and turbulent flows.”
And “the geometry of the scaffold may be configured to change the localized flow direction or to split the flow more than a certain number of times within a given length along a longitudinal axis of the static mixer element, such as more than 200m.sup.-1 , optionally more than 400 m.sup.-1, optionally more than 800 m.sup.-1 , optionally more than 1500m.sup.-1 , optionally more than 2000m.sup.-1 , optionally more than 2500m.sup.-1 , optionally more than 3000m.sup.-1 , optionally more than 5000m.sup.-1 . The geometry or configuration of the scaffold may comprise more than a certain number of flow splitting structures within a given volume of the static mixer, such as more than 100 m- .sup.3, optionally more than 1000 m.sup.-3, optionally more than 1x10.sup.4 m.sup.-3, optionally more than lxlO.sup.6 m.sup.-3, optionally more than lxlO.sup.9 m.sup.-3, optionally more than lxlO.sup.10 m.sup.-3. The geometry or configuration of the scaffold may be substantially tubular or rectilinear. The scaffold may be formed from or comprise a plurality of segments. Some or all of the segments may be straight segments. Some or all of the segments may comprise polygonal prisms such as rectangular prisms, for example. The scaffold may comprise a plurality of planar surfaces. The straight segments may be angled relative to each other. Straight segments may be arranged at a number of different angles relative to a longitudinal axis of the scaffold, such as two, three, four, five or six different angles, for example. The scaffold may comprise a repeated structure. The scaffold may comprise a plurality of similar structures repeated periodically along the longitudinal axis of the scaffold. The geometry or configuration of the scaffold may be consistent along the length of the scaffold. The geometry of the scaffold may vary along the length of the scaffold. The straight segments may be connected by one or more curved segments.” (pages 10-13).
The examiner notes that the static mixers shown in Figs. 1 and 2 show the non-line of site geometry of the mixers. And, “The aspect ratios (L/d) of the static mixer elements, or reactor chambers comprising the static mixer elements, may be provided in a range suitable for industrial scale flow rates for a particular reaction. The aspect ratios may, for example, be in the range of about 1 to 1000, 2 to 750, 3 to 500, 4 to 250, 5 to 100, or 10 to 50. The aspect ratios may, for example, be less than about 1000, 750, 500, 250, 200, 150, 100, 75, 50, 25, 20, 15, 10, 9, 8, 7, 6, 5, 4, 3, or 2 (i.e., the newly claimed limitation of “at least 15” is taught). The aspect ratios may, for example, be greater than about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 15, 20, 25, 50, 75, or 100.” [pages 10-15].
The slurry catalytic material (the instant claimed suspension) may be provided in a composition with one or more additives such as binders, to facilitate coating of the catalyst to the scaffold (page 29).
The catalyst particles taught by Henry et al comprises metal (pages 1 and 23). They are deposited (coated) on the scaffold, and used for reaction (i.e., hydrogenation) without requiring any step to activation the catalyst (page 20). The catalyst particles are not a catalyst precursor, without requiring in-situ activation. So, the catalyst particles are ex-situ catalyst particles. They are remains their catalytically active after deposition as the instant claim.
Henry et al. teach coating a scaffold with a catalytic material to form a catalytic static mixer. The method of forming a catalytic static mixer may comprise forming the scaffold using an additive manufacturing process such as 3D printing (page 20).
Henry does not teach the following limitations in “drying the coated scaffold to remove the liquid carrier to provide a coated scaffold comprising ex-situ catalyst particles, wherein the step of applying the catalytic liquid suspension to the surface of the scaffold in step (i) is by wash-coating or dip-coating;” as per applicant claim 1, Kiemel et al. teach “In the case of metal honeycomb or metal mesh catalysts, the metal surface generally is coated with a wash-coat, whereby the wash coat layer contains porous catalyst supports in the form of porous particles. The at least one catalytically active platinum species usually is situated on the pore surface of the porous particles in the wash coat layer” [0024] and “A wash coat slurry is a liquid coating composition, usually in the form of an aqueous suspension that contains, aside from water, porous catalyst support particles with particle sizes in the range of, for example, 2-100 µm.” [0025] and “In this context, the noble metal precursor can be contacted to the porous catalyst support particles forming the ingredients of the wash coat by means of one of the impregnating methods mentioned below. In this context, the impregnated porous catalyst support particles can have been produced separately, i.e. can have been impregnated, dried, and calcined, and thus can be incorporated into the wash coat slurry while equipped with catalytically active noble metal species. As such, it is the interpretation of the office that Kiemel et al. teach the claimed limitation wherein “ex-situ particles are in their final form prior to deposition to a surface of a scaffold.
Alternatively, another interpretation is possible to meet this limitation as it is feasible to implement the impregnating step as a process step of the wash coat slurry, whereby the drying and calcination take place only after application of the wash coat [0028].
The examiner notes that the drying step is similarly performed on the wash coat where the catalytically active noble metal species had been incorporated into the wash coat slurry.
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 apply a wash coat that contains catalytically active metal species as taught by Kiemel et al. to a scaffold as taught by Henry et al. The teaching or suggested motivation for doing so being to utilize an operationally simple and inexpensive approach to impregnate the scaffold with catalytically active metal species (i.e., ex-situ catalyst particles) for use in subsequent chemical transformation reactions. As such, the ex-situ catalyst particles are catalytic active as the instant claim.
Regarding claim 5, Henry in view of Kiemel teaches all the limitations of claim 1 and further requires “wherein the process further comprises a pre-treatment step prior to applying the catalytic liquid suspension to the surface of the scaffold in step(i), and wherein the pre-treatment step comprises at least one surface treatment step to the surface of the scaffold selected from chemical treatment, anodic oxidation, hot dipping, vacuum plating, painting, thermal spraying, and acid etching”. Henry further teaches “The surface of the scaffold may be modified to provide or enhance catalytic reactivity, such as by roughening, and/or depositing a metal or alloy on at least a part of the surface of the scaffold, such as a further deposited (sputtered) layer. Surface roughening may be achieved by any process of acid treatment, heat treatment in controlled gas atmospheres, physical vapor deposition, cold spray, plasma spray, ion implantation flame spray pyrolysis electrodeposition, chemical vapor deposition, glow discharge, sputtering, and plating or by any mechanical means. The surface modification may provide one or more outer layers, example one or more metal deposited (e.g. sputtered) layers.” [p. 29, 1st paragraph]. The examiner notes that acid treatment is both an acid etching and a chemical treatment step. 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 advantageously utilize the process of Henry and Kiemel to utilize a pre-treatment step to improve the surface rugosity (such as by increasing the surface roughness) to enhance adhesion of any subsequent coatings to the substrate, leading to enhanced performance of the coated substrate, such as when applied to a scaffold.
Regarding claim 6, Henry and Kiemel teach all the limitations of claim 1 and further requires “wherein the catalyst particles are formed from a catalyst material or a catalyst supported material comprising the catalyst material on a support material”. Henry teaches application of catalyst particles to the scaffold by cold spraying or electroplating the catalyst particles [p. 28, bottom of page]. Henry does not teach applying a catalytic liquid suspension comprised of a liquid carrier containing a plurality of ex-situ catalyst particles by wash-coating or dip-coating to provide a coating containing catalytically reactive sites on the surface of the coated scaffold. Kiemel teaches “In this context, the noble metal precursor can be contacted to the porous catalyst support particles forming the ingredients of the wash coat by means of one of the impregnating methods mentioned below. In this context, the impregnated porous catalyst support particles can have been produced separately, i.e. can have been impregnated, dried, and calcined, and thus can be incorporated into the wash coat slurry while equipped with catalytically active noble metal species. Alternatively, it is feasible to implement the impregnating step as a process step of the wash coat slurry, whereby the drying and calcination take place only after application of the wash coat ” [0028] and “In one embodiment, aside from the at least one exothermic-decomposing platinum precursor, precursors of other metals or noble metals, in particular precursors of palladium, ruthenium and/or rhodium, can also be used’ [0047] and “In particular, the material of the porous catalyst supports can comprise or consist of refractory materials, for example of ceramic materials. Suitable refractory materials can be selected, for example, from the group consisting of aluminum oxides, titanium dioxide, zirconium oxides, cerium/zirconium mixed oxides, aluminum silicates ( e.g. cordierite, mullite), silicon carbides, and silicon nitrides” [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 advantageously utilize the static mixers taught by Henry coated with the catalyst or a supported catalyst materials taught by Kiemel. The teaching or suggested motivation for doing so being to utilize the advantages of a scaffold, such as effective mixing, while performing a chemical reaction for which the catalyst or supported catalyst particles are known to catalyze as the feed material flows through the scaffold.
Regarding claim 7, Henry and Kiemel teach all the limitations of claim 6 and further requires “wherein the catalyst material is selected from a metal, metal oxide, aluminum silicate, activated carbon, mesoporous carbon, graphene, graphitic material, metal-organic framework, zeolite, or any combination thereof, wherein the metal is selected from at least one of aluminum, iron, cerium, calcium, cobalt, copper, magnesium, zinc, nickel, palladium, platinum, gold, silicon, silver, ruthenium, iridium, rhodium, titanium, vanadium, zirconium, niobium, tantalum, and chromium, or a metal oxide thereof”. Henry teaches “In an embodiment, the scaffold or catalytic material comprises at least one of a metal, semi-- metal and metal oxide. For example, the scaffold or catalytic material may comprise one or more of the following: a metal selected from iron, cobalt, chromium, aluminum, vanadium, copper, zinc, nickel, palladium, platinum, gold, silver, ruthenium, iridium, and rhodium, or alloys or mixtures thereof; a semimetal selected from Bi, CdTe, HgCdTe, GaAs, or mixtures thereof; and a metal oxide selected from PbO, PbO2, ZnO, TiO2, CoO, Al2O3, or mixtures thereof.” [p. 28, bottom of page]. Henry does not specifically teach catalyst materials applied in a wash coat or dipcoat. Kiemel teaches use of a platinum catalyst added by an incipient wetness approach or as a pre-formed catalyst supported on a support when noting “In this context, the noble metal precursor can be contacted to the porous catalyst support particles forming the ingredients of the wash coat by means of one of the impregnating methods mentioned below. In this context, the impregnated porous catalyst support particles can have been produced separately, i.e. can have been impregnated, dried, and calcined, and thus can be incorporated into the wash coat slurry while equipped with catalytically active noble metal species. Alternatively, it is feasible to implement the impregnating step as a process step of the wash coat slurry, whereby the drying and calcination take place only after application of the wash coat ” [0028] and “In one embodiment, aside from the at least one exothermic-decomposing platinum precursor, precursors of other metals or noble metals, in particular precursors of palladium, ruthenium and/or rhodium, can also be used’ [0047] and “In particular, the material of the porous catalyst supports can comprise or consist of refractory materials, for example of ceramic materials. Suitable refractory materials can be selected, for example, from the group consisting of aluminum oxides, titanium dioxide, zirconium oxides, cerium/zirconium mixed oxides, aluminum silicates ( e.g. cordierite, mullite), silicon carbides, and silicon nitrides” [0034].
The examiner notes that the additional metals taught by Kiemel (palladium, ruthenium and/or rhodium) can also be utilized in the “impregnated porous catalyst support particles can have been produced separately” also taught by Kiemel [0028,0047]. 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 advantageously utilize the process of Henry and Kiemel to utilize a catalyst material. The teaching or suggested motivation for doing so being to utilize the advantages of dispersed catalyst particles incorporated in the wash coat surface known to be effective for bringing about the desired chemical reactions being performed with the scaffold.
Regarding claim 10, Henry and Kiemel teach all the limitations of claim 6 and further requires “wherein the catalyst supported material is selected from at least one of ruthenium on aluminum oxide, palladium on aluminum oxide, lead-poisoned palladium on calcium carbonate, iron on aluminum oxide, silver on aluminum oxide, silica diphenyl phosphine palladium, palladium on titanium silicate, palladium on carbon, nickel modified aluminum oxide silicon oxide, or zeolite”, to which Henry is silent. Kiemel teaches “In this context, the noble metal precursor can be contacted to the porous catalyst support particles forming the ingredients of the wash coat by means of one of the impregnating methods mentioned below. In this context, the impregnated porous catalyst support particles can have been produced separately, i.e. can have been impregnated, dried, and calcined, and thus can be incorporated into the wash coat slurry while equipped with catalytically active noble metal species. Alternatively, it is feasible to implement the impregnating step as a process step of the wash coat slurry, whereby the drying and calcination take place only after application of the wash coat ” [0028] and “In one embodiment, aside from the at least one exothermic-decomposing platinum precursor, precursors of other metals or noble metals, in particular precursors of palladium, ruthenium and/or rhodium, can also be used’ [0047] and “In particular, the material of the porous catalyst supports can comprise or consist of refractory materials, for example of ceramic materials. Suitable refractory materials can be selected, for example, from the group consisting of aluminum oxides, titanium dioxide, zirconium oxides, cerium/zirconium mixed oxides, aluminum silicates ( e.g. cordierite, mullite), silicon carbides, and silicon nitrides” [0034].
The examiner notes that from the metals and support materials taught by Kiemel, at least the catalyst supported materials Ru on aluminum oxide and Pd of aluminum oxide could be prepared. 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 advantageously utilize the process of Henry and Kiemel to utilize a catalyst supported catalyst material as specifically taught by Kiemel. The teaching or suggested motivation for doing so being to utilize an effectively chosen metal and support to bring about the subsequent desired chemical reaction as the feed material flows through the wash-coat coated scaffold.
Regarding claim 13 Henry and Kiemel teach all the limitations of claim 1 and further requires “wherein the liquid carrier is selected from the group comprising water, ethanol, isopropanol, butanol, ethyl acetate, acetone or a combination thereof”, to which Henry is silent. Kiemel teaches “A wash coat slurry is a liquid coating composition, usually in the form of an aqueous suspension that contains, aside from water, porous catalyst support particles with particle sizes in the range of, for example, 2-100 µm” [0025]. 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 advantageously utilize a solvent from the listing of this claim limitation, as taught by Kiemel. The teaching or suggested motivation for doing so being to utilize solvents that are inexpensive and readily available and effective for use in wash coat formulations.
Claims 3 and 9 are rejected under 35 U.S.C. 103 as being unpatentable over Henry and Kiemel, as applied to claim 1, in view of Peela, et.al. (“Wash coating of γ-alumina on stainless steel microchannels”, Catalysis Today 147S (2009) S17–S23; hereinafter Peela).
Regarding claim 3, Henry and Kiemel teach all the limitations of claim 1 as noted above. Henry and Kiemel do not teach “wherein the surface of the static mixer is pre-coated before step (i) with a support material and optionally a binder”. Peela teaches “Wash coating was done following a two-step procedure: primer coating followed by slurry coating. Wash coat was characterized by SEM, adherence test and BET surface area measurement. For coating of the primer, Disperal with or without polyvinyl alcohol (PVA) was used.” [Abstract] and “Even though the advantages of using microreactors have been reported for several reactions, the effect of slurry properties on the adherence, uniformity and loading of the wash coat layer has not been reported. These features depend on the slurry properties and more importantly on primer coating. The primer coating, consisting of a sol and/or viscosity modifier, is necessary to enhance the adherence of the alumina coating. Moreover, binders, viscosity modifiers and dispersants added in the slurry, can have a significant effect on the wash coat properties.” [p. S17, Introduction section, left column, 1st paragraph] and “Primer deposition was done by using a mixture of boehmite sol and/or a binder in water.
The boehmite sol was prepared by adding aluminum hydroxide powder (Disperal P2, average particle size = 45 µm Sasol, Germany) to a 0.4 wt.% HNO3 aqueous solution” [p. S18, section 2.2]. 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 advantageously modify the process of Henry and Kiemel in view of Peela to utilize a pre-coat (a primer in the language of Peela). The teaching or suggested motivation for doing so being to enhance adhesion of the wash coat to the scaffold substrate.
Regarding claim 9, Henry and Kiemel in view of Peela teach all the limitations of claim 3 as noted above. Henry and Kiemel do not teach “wherein the support material is selected from at least one of activated carbon, mesoporous carbon, graphene, graphitic material, metal-organic framework, zeolite, aluminum oxide, silicon dioxide, ceramic, magnesium chloride, calcium carbonate or dipotassium oxide”.
Peela teaches “Primer deposition was done by using a mixture of boehmite sol and/or a binder in water. The boehmite sol was prepared by adding aluminum hydroxide powder (Disperal P2, average particle size = 45 µm Sasol, Germany) to a 0.4 wt.% HNO3 aqueous solution” [p. S18, section 2.2].
The examiner notes that boehmite is a form of aluminum oxide. 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 advantageously modify the process of Henry and Kiemel in view of Peela to utilize a support material chosen from the listing in this claim limitation. The teaching or suggested motivation for doing so being to enhance adhesion of the wash coat to the scaffold substrate as taught by Peela when noting “a primer coating can be used to form a thin layer of alumina which can enhance the adherence of the subsequent wash coat” [p. S17, top right column].
Claims 4, 14, 21 and 29-30 are rejected under 35 U.S.C. 103 as being unpatentable over Henry and Kiemel, as applied to claim 1, in view of Mitra, et.al. (“Wash coating of Different Zeolites on Cordierite Monoliths”, J. Am. Ceram. Soc., 91 [1] 64–70 (2008); hereinafter Mitra).
Regarding claim 4, Henry and Kiemel teach all the limitations of claim 1 as noted above. Henry and Kiemel do not teach “wherein the catalytic liquid suspension further comprises a binder”. Mitra teaches “To study the effect of binder addition, in some cases, 3 wt% colloidal silica (Ludox-AS 40, Grace Davison, Columbia, MD, particle diameter 20–24 nm) was added to the suspension before wash coating” [p. 65, upper left column] and “The suspensions were prepared by mixing the zeolite powders with demineralized water in a ball mill till a stable uniform slurry was formed. Suspensions having solid concentrations of 20%, 30%, and 40% were prepared for mordenite, ZSM5, and Zeolite Y.” [p. 64, bottom right – p. 65, top right] and “Addition of a binder (colloidal silica) helps to improve the intraparticle cohesion and enhances the loading as well as adhesion of the washcoat layer.” [p. 70, left column]. 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 advantageously modify the process of Henry and Kiemel in view of Mitra to utilize a binder. The teaching or suggested motivation being to enhance adhesion of the washcoat to the substrate, leading to enhanced durability of the coated substrate, such as when applied to a scaffold.
Regarding claim 14, Henry and Kiemel teach all the limitations of claim 1 as noted above. Henry and Kiemel do not teach “wherein the catalytic liquid suspension has a solids content of between about 3 wt.% to about 28 wt.%”. Mitra teaches “To study the effect of binder addition, in some cases, 3 wt% colloidal silica (Ludox-AS 40, Grace Davison, Columbia, MD, particle diameter 20–24 nm) was added to the suspension before wash coating” [p. 65, upper left column] and “The suspensions were prepared by mixing the zeolite powders with demineralized water in a ball mill till a stable uniform slurry was formed. Suspensions having solid concentrations of 20%, 30%, and 40% were prepared for mordenite, ZSM5, and Zeolite Y.” [p. 64, bottom right – p. 65, top right]. 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 advantageously utilize a catalytic liquid suspension % solids content as taught by Mitra to the scaffold of Henry and the washcoat technology of Kiemel. The teaching or suggested motivation for doing so being to utilize a suspension that provides good rheological and handling properties while obtaining the desired coating weight or thickness of the scaffold coating.
Regarding claim 21, Henry and Kiemel teach all the limitations of claim 1 as noted above. Henry does not teach “wherein the ex-situ catalyst particles are less than about 5µm”. Kiemel teaches “A washcoat slurry is a liquid coating composition, usually in the form of an aqueous suspension that contains, aside from water, porous catalyst support particles with particle sizes in the range of, for example, 2-100 µm” [0025]. The examiner notes that the catalytically active noble metal particles are disposed on the 2-100 µm support particles, thus the expectation that the catalytically active noble metal particles are no larger than the support particles upon which they have been deposited. Henry and Kiemel do not teach wherein the ex-situ catalyst particles are less than about 5 µm.
Mitra teaches “The stability of the suspension used for wash coating and the adhesion of the wash coat to the cordierite substrate is strongly influenced by the size of the suspended particles in the slurry. The macropores in the bare cordierite are in the range of 3–5 µm and, consequently, it is necessary that the particle size of the zeolite powders be reduced to values smaller than 5 µm in order to have a stable wash coat”. [p. 65, Results and Discussions, section (1)]. The examiner notes that using the process of Kiemel to prepare a catalytically active noble metal catalyst using the support particle sizes taught by Mitra would provide catalytically active noble metal catalyst particles smaller than the support particles, which Mitra notes should be smaller than 5 µm for a stable wash coat. Therefore, one of ordinary skill in the art would utilize the particle sizes taught by Mitra when preparing the supported ex-situ catalyst particles taught by Kiemel for use on the scaffold taught by Henry. The teaching or suggested motivation being to utilize effective catalyst particles for the subsequent desired chemical reactions to occur as the feed material is passed through the scaffold.
Regarding claim 29, Henry and Kiemel in view Mitra teach all the limitations of claim 4 as noted above. Henry and Kiemel do not teach “wherein the binder for the catalytic liquid suspension is selected from the group comprising hydroxypropyl cellulose, methyl cellulose, polyester, polyurethane, acrylic resins, condensation resins, polyvinyl acetate, poly (acrylic acid) sodium salt, polyvinylidene fluoride, polyethylene oxide, polyethylene glycol, dextrin, sodium silicate, colloidal silica, polydimethyl siloxane, boehmite, colloidal aluminum oxide, or polyisobutylene”. Mitra teaches “To study the effect of binder addition, in some cases, 3 wt% colloidal silica (Ludox-AS 40, Grace Davison, Columbia, MD, particle diameter 20–24 nm) was added to the suspension before wash coating” [p. 65, upper left column] and “The suspensions were prepared by mixing the zeolite powders with demineralized water in a ball mill till a stable uniform slurry was formed. Suspensions having solid concentrations of 20%, 30%, and 40% were prepared for mordenite, ZSM5, and Zeolite Y.” [p. 64, bottom right – p. 65, top right] and “Addition of a binder (colloidal silica) helps to improve the intraparticle cohesion and enhances the loading as well as adhesion of the washcoat layer.” [p. 70, left column]. 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 advantageously utilize a binder chosen from the group listed in the limitation for this claim. The teaching or suggested motivation for doing so being to utilize a cost-effective and readily available binder that can enhance adhesion of the washcoat to the substrate, leading to enhanced durability of the coated substrate, such as when applied to a scaffold.
Regarding claim 30, Henry and Kiemel in view Mitra teach all the limitations of claim 29 as noted above. Henry and Kiemel do not teach “wherein the binder is added at a concentration of between about 0.3 wt.% to about 5 wt.% based on the total weight of the catalytic liquid suspension”. Mitra teaches “To study the effect of binder addition, in some cases, 3 wt% colloidal silica (Ludox-AS 40, Grace Davison, Columbia, MD, particle diameter 20–24 nm) was added to the suspension before wash coating” [p. 65, upper left column] and “The suspensions were prepared by mixing the zeolite powders with demineralized water in a ball mill till a stable uniform slurry was formed. Suspensions having solid concentrations of 20%, 30%, and 40% were prepared for mordenite, ZSM5, and Zeolite Y.” [p. 64, bottom right – p. 65, top right] and “Addition of a binder (colloidal silica) helps to improve the intraparticle cohesion and enhances the loading as well as adhesion of the washcoat layer.” [p. 70, left column]. 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 prepare a catalytically coated scaffold as taught by Henry and Kiemel using the binder concentration taught by Mitra. The teaching or suggested motivation for doing so being it would lead to the enhanced adhesion of the washcoat and durability of the coated substrate.
Claims 11 and 12 are rejected under 35 U.S.C. 103 as being unpatentable over Henry and Kiemel in view of Peela, as applied to claim 3, further in view of Mitra.
Regarding claim 11, Henry and Kiemel in view of Peela teach all the limitations of claim 3 as noted above. Henry and Kiemel in view of Peela do not teach “wherein the binder for the catalytic liquid suspension is selected from the group comprising hydroxypropyl cellulose, methyl cellulose, polyester, polyurethane, acrylic resins, condensation resins, polyvinyl acetate, poly(acrylic acid) sodium salt, polyvinylidene fluoride, polyethylene oxide, polyethylene glycol, dextrin, sodium silicate, colloidal silica, polydimethyl siloxane, boehmite, colloidal aluminum oxide, or polyisobutylene”. Mitra teaches “To study the effect of binder addition, in some cases, 3 wt% colloidal silica (Ludox-AS 40, Grace Davison, Columbia, MD, particle diameter 20–24 nm) was added to the suspension before wash coating” [p. 65, upper left column] and “The suspensions were prepared by mixing the zeolite powders with demineralized water in a ball mill till a stable uniform slurry was formed. Suspensions having solid concentrations of 20%, 30%, and 40% were prepared for mordenite, ZSM5, and Zeolite Y.” [p. 64, bottom right – p. 65, top right] and “Primer deposition was done by using a mixture of boehmite sol and/or a binder in water. The boehmite sol was prepared by adding aluminum hydroxide powder (Disperal P2, average particle size = 45 µm Sasol, Germany) to a 0.4 wt.% HNO3 aqueous solution” [p. S18, section 2.2]. 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 advantageously incorporate a binder chosen from the grouping of this claim limitation as taught by Mitra with the catalytic liquid suspension taught by Kiemel for coating of the scaffold taught by Henry. The teaching or suggested motivation for doing so being to utilize an effectively chosen binder to provide a durable and robust coating on the scaffold.
Regarding claim 12, Henry and Kiemel in view of Peela teach all the limitations of claim 11 as noted above. Henry and Kiemel in view of Peela do not teach “wherein the binder is added at a concentration of between about 0.3 wt.% to about 5 wt.% based on the total weight of the catalytic liquid suspension”. Mitra further teaches “To study the effect of binder addition, in some cases, 3 wt% colloidal silica (Ludox-AS 40, Grace Davison, Columbia, MD, particle diameter 20–24 nm) was added to the suspension before wash coating” [p. 65, upper left column] and “Addition of a binder (colloidal silica) helps to improve the intraparticle cohesion and enhances the loading as well as adhesion of the washcoat layer.” [p. 70, left column]. 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 advantageously utilize a binder concentration taught by Mitra with the catalytic liquid suspension taught Kiemel for coating the scaffold taught by Henry. The teaching or suggested motivation for doing so being to utilize an effectively chosen binder concentration to provide a durable and robust coating in order to obtain good washcoat properties on the scaffold.
Claims 15 and 17 are rejected under 35 U.S.C. 103 as being unpatentable over Henry and Kiemel, as applied to claim 1, in view of Yuan, et.al. (“One-step dip-coating of uniform γ-Al2O3 layers on cordierite honeycombs and its environmental applications”, Ceramics International 42 (2016) 14384–14390; hereinafter Yuan).
Regarding claim 15, Henry and Kiemel teach all the limitations of claim 1 as noted above. Henry and Kiemel do not teach “wherein the thickness of the coating is between about 1 µm to about 50 µm”. Yuan teaches “On the top view, much coarser appearance (Fig. 4d) of the coated channel wall could be observed, in contrast to the typical structure of the bare walls (Fig. 4b). It indicated a complete coverage of the monolith. The coating thickness was ca. 30 µm.” [p.14388, Section 3.2.3] and “Given that Sc was approximately equal to Scoat, the calculated result of Ttheoretical was 30.0 µm, corresponding very well to the measured thickness. It indicated a complete and homogeneous coating of γ-Al2O3” [p. 14389, upper left column]. 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 advantageously utilize a coating thickness as taught by Yuan for the washcoat-coated scaffold as taught by Henry and Kiemel. The teaching or suggested motivation for doing so being to optimize the coating thickness for durability and efficient operation.
Regarding claim 17, Henry and Kiemel teach all the limitations of claim 1 as noted above. Henry and Kiemel do not teach “wherein the adhesion of the coating provides a total mass loss of the coating of less than about 0.5 wt.% when measured by sonication testing”. Yuan teaches Fig. 3 [p. 14386; see below] showing weight loss curves of wash coats upon ultrasonic treatment, where the 10 % , 12.5 % and 15 % pseudo-boehmite binder samples exhibited wt loss % of 0.5 % or less.
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And “It was revealed that under the acidic conditions, the pseudo-boehmite was partially dissolved, generating better binders [section 3.1, p.14386] and “Furthermore, the sample from 12.5 wt% content of pseudo-boehmite in slurry gave the smallest weight loss (< 1%) after 3 h ultrasonic treatment” [section 3.2.1, p. 14387] and “The formed “nail-like” structure enhances the interaction between the coating and the support, resulting in a firm adhesion after drying and calcinating” [p. 14387, Section 3.1, upper right column]. The examiner notes that the present claim recites “less than about 0.5 wt %” wherein “about” includes values slightly above and slightly below those claimed, therefore, it is clear that Yuan meets the claim limitation. 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 incorporate a coating with good adhesion properties as taught by Yuan for the washcoat-coated scaffold as taught by Henry and Kiemel. The teaching or suggested motivation for doing so being to prepare durable coatings, leading to a coated scaffold with enhanced service life properties.
Claim 22 is rejected under 35 U.S.C. 103 as being unpatentable over Henry and Kiemel, as applied in claim 1, in view of Peela in further in view of Montebelli, et. al. (“Wash coating and chemical testing of a commercial Cu/ZnO/Al2O3 catalyst for the methanol synthesis over copper open-cell foams”, Applied Catalysis A: General 481 (2014) 96–103; hereinafter Montebelli).
Regarding claim 22, Henry and Kiemel teach all the limitations of claim 1 as noted above. Henry and Kiemel do not teach “wherein the drying step comprises the steps of:(a) applying a first temperature ranging between about 15 °C to about 30 °C to the coated surface of the scaffold for a first period of about 4 to 24 hours to volatilize at least a portion of volatile material from the catalytic liquid suspension; and (b) applying a second temperature ranging between about 100 °C to about 180 °C under controlled atmosphere for a second period of about 4 to 24 hours such that a dried coating is formed on the surface of the scaffold drying steps”, Peela teaches “(iii) drying of the substrate at room temperature for 3 h and then at 120 oC for 8 h” [p. S18, section 2.2].
The examiner notes that the primer coating dispersion of Peela is a liquid suspension. The examiner notes that Peela teaches drying for 3h at the initial temperature of “room temperature”, where the claim limitation requires a 4-24h time range for the initial drying step at about 15 °C to about 30 °C. Peela does not teach drying for 4h at the initial drying temperature. Montebelli teaches “Cleaned copper foams were then dipped in the ball-milled slurry and withdrawn at constant speed (3 cm/min). A strong N2 flow was then applied to blow the excess slurry out from the 3D network of struts”. Drying in static air at RT overnight and calcination in static air from RT to 573 K, 1 K/min as heating ramp followed” [p.98, upper right column].
The examiner notes that Montebelli teaches the use drying at room temperature for overnight for the initial drying temperature, which one could reasonably understand to be a time period of 8 hours or more. In the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art,” a prima facie case of obviousness exists. See In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990). See MPEP 2144.05. Therefore, one of ordinary skill in the art would utilize the teaching of Montebelli to inform the skilled artisan of the initial drying temperature and time period to be employed and would utilize the teaching of Peela to inform the skilled artisan of the second drying temperature and time period to be employed.
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 advantageously utilize the process of Henry and Kiemel in view of Peela further in view of Montebelli to select the optimal first and second drying times and temperatures. The teaching or suggested motivation for doing so being to prepare wash coats with “negligible cracks and pore blocking” [Montebelli, p. 102, Conclusions section, bottom left column] leading to the preparation of durable coatings, leading to a coated scaffold with enhanced service life properties.
Response to Arguments
With regards to the previous Grounds of Rejection
Applicant's arguments filed on 08/29/2025, with respect to claims 1, 3-7, 9-15, 17, 21-22, and 29-30, have been considered but are not persuasive. The examiner would like to take this opportunity to address the Applicant's arguments.
On pages 9-10 of their arguments, Applicant continues by stating what the Henry reference does not teach “non-line-of sight techniques”.
In response, Applicant is reminded that the Henry reference was not relied upon for these teachings given the rejection was a 103 and combined the teachings of Henry et al. and Kiemel et al.
While it is Applicant’s position that Henry does not have a “non-line-of-sight configuration. Henry et al. do teach the static mixers shown in Figs. 1 and 2 show the non-line of site geometry of the mixers as well as the capability to change the geometry of the mixers as was stated in the rejection above. Again Kiemel et al. was relied upon for the wash coating steps.
The catalyst particles taught by Henry et al comprises metal (pages 1 and 23). They are deposited (coated) on the scaffold, and used for reaction (i.e., hydrogenation) without requiring any step to activation the catalyst (page 20). It is not a catalyst precursor, and does not require in-situ activation. So, the catalyst particles are ex-situ catalyst particles. They are remains their catalytically active after deposition as the instant claim.
Henry et al. teach coating a scaffold with a catalytic material to form a catalytic static mixer. The method of forming a catalytic static mixer may comprise forming the scaffold using an additive manufacturing process such as 3D printing (page 20).
As such, the catalytic liquid suspension taught by the combined references of Kiemel et al and Henry et al. teach the claimed ex-situ catalyst particles which are catalytic active and remain catalytic active after deposition without requiring in-situ activation.
In response to applicant's arguments against the references individually (Peela, Mitra, Yuan or Montebelli) (pages 10-18), one cannot show nonobviousness by attacking references individually where the rejections are based on combinations of references. See In re Keller, 642 F.2d 413, 208 USPQ 871 (CCPA 1981); In re Merck & Co., 800 F.2d 1091, 231 USPQ 375 (Fed. Cir. 1986). The motivations for the combination can also be found above in the art rejections.
As such, the rejection of claim 1 as set forth in the office action above is proper and stands.
The rejection for the remaining claims were either directly or indirectly dependent thereon stands.
Conclusion
Applicant's amendment necessitated the new ground(s) of rejection presented in this Office action. Accordingly, THIS ACTION IS MADE FINAL. See MPEP § 706.07(a). Applicant is reminded of the extension of time policy as set forth in 37 CFR 1.136(a).
A shortened statutory period for reply to this final action is set to expire THREE MONTHS from the mailing date of this action. In the event a first reply is filed within TWO MONTHS of the mailing date of this final action and the advisory action is not mailed until after the end of the THREE-MONTH shortened statutory period, then the shortened statutory period will expire on the date the advisory action is mailed, and any nonprovisional extension fee (37 CFR 1.17(a)) pursuant to 37 CFR 1.136(a) will be calculated from the mailing date of the advisory action. In no event, however, will the statutory period for reply expire later than SIX MONTHS from the mailing date of this final action.
Any inquiry concerning this communication or earlier communications from the examiner should be directed to YUN QIAN whose telephone number is (571)270-5834. The examiner can normally be reached Monday-Thursday 10:00am-4:00pm.
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YUN . QIAN
Examiner
Art Unit 1732
/YUN QIAN/Primary Examiner, Art Unit 1738