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 .
Priority
Receipt is acknowledged of certified copies of papers required by 37 CFR 1.55.
Information Disclosure Statement
The information disclosure statement (IDS) submitted on 09/19/2022, 12/19/2024,02/12/2025, 03/13/2025, 05/19/2025, 08/05/2025 have been considered by the examiner.
Election/Restrictions
Claims 34-40 withdrawn from further consideration pursuant to 37 CFR 1.142(b) as being drawn to a nonelected invention, there being no allowable generic or linking claim. Election was made without traverse in the reply filed on 10/15/2025.
Applicant’s election without traverse of claims 21-33 in the reply filed on 10/15/2025 is acknowledged.
Claim Interpretation
Claim 22 recites “wherein the open face area (OFA) of the opposed surfaces”. While no definition is given in the instant specification, open face area is interpreted to be a fraction of the total cross-sectional area, and can be calculated using the following equation:
A
F
A
=
(
1
-
w
s
)
2
where
A
F
A
is the ratio of the open frontal area to the total cross-sectional area w is the wall thickness and s is the cell pitch.
Claim 23 recites “wherein a ratio of macropores to mesopores”. This is interpreted to mean a pore volume ratio of macropores to mesopores.
Claim Objections
Claim 23 objected to because of the following informalities: claim 23 recites "wherein a mesopore diameter is about 10 nm 50 nm" on line 4. Interpreting this as a range of diameters, this limitation should read "10 nm to 50 nm". Appropriate correction is required.
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(d):
(d) REFERENCE IN DEPENDENT FORMS.—Subject to subsection (e), a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
The following is a quotation of pre-AIA 35 U.S.C. 112, fourth paragraph:
Subject to the following paragraph [i.e., the fifth paragraph of pre-AIA 35 U.S.C. 112], a claim in dependent form shall contain a reference to a claim previously set forth and then specify a further limitation of the subject matter claimed. A claim in dependent form shall be construed to incorporate by reference all the limitations of the claim to which it refers.
Claim 31 rejected under 35 U.S.C. 112(d) or pre-AIA 35 U.S.C. 112, 4th paragraph, as being of improper dependent form for failing to further limit the subject matter of the claim upon which it depends, or for failing to include all the limitations of the claim upon which it depends. Claim 31 is dependent upon claim 31, which is improper. Applicant may cancel the claim(s), amend the claim(s) to place the claim(s) in proper dependent form, rewrite the claim(s) in independent form, or present a sufficient showing that the dependent claim(s) complies with the statutory requirements.
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 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 21, 23, 25-30, 33 are rejected under 35 U.S.C. 103 as being unpatentable over Pang et al (US 20190291077 A1) in view of Thompson et al (US 20190224647 A1).
Regarding claim 21, Pang discloses a method of capturing CO2, including exposing a gas mixture to a porous structure ([0005] meeting limitation “a method for removing CO2 from a gas stream”). In an embodiment, the PPI sorbent can be used to adsorb CO2 ([0035]). The PPI sorbent can be physically impregnated in the internal volume pores of the porous structure and not covalently bonded to the internal surface of the pores of the porous structure ([0037]). The preferred structure can be a honeycomb structure such as a monolith honeycomb structure that includes channels ([0058] meeting limitation “a honeycomb monolith containing a CO2 sorbent” and “wherein the honeycomb monolith is comprised of longitudinal channels connecting two opposed surfaces of the monolith”). The materials in Examples 6 and 7 were pretreated by heating to 70° C at a ramp rate of 5º C/min under a flow of N2, and held for 2 h ([0090]). The samples were cooled to 35º C. and equilibrated at this analysis temperature for 1 h ([0090]). Subsequently, the gas flow was switched to a premixed gas containing 400 ppm CO2/N2 for 3 h ([0090]). The mass gain was recorded, converted to amount of CO2 adsorbed, and normalized by the dry mass of the sample ([0090] meeting limitation “the method comprising: contacting a gas stream with a honeycomb monolith containing a CO2 sorbent”).
The structure can include porous structures (e.g., macroporous, mesoporous, microporous, or mixtures thereof (e.g., where a macroporous surface can include mesopores, … within one or more of the macropores)) ([0054] meeting limitation “wherein the longitudinal channels comprise macropore and mesopore containing walls”). The PPI sorbent is within the pore volume of the pores of the porous layers and/or porous structure surface ([0036]). In an aspect, the pores (e.g., mesopores ) may not be overfilled by the PPI sorbent, so there exists suitable space for the transport of gases through the pores via diffusion, although other gas transport processes can occur (e.g., advection, convection, and the like) ([0036] meeting limitation “wherein the CO2 sorbent occupies a fraction of a mesopore volume within the macropore and mesopore containing walls”).
Pang discloses a method of capturing CO2, comprising: exposing a gas mixture to a porous structure having supported thereon at least one of: a poly(propylenimine) (PPI) sorbent… capturing the CO2 in the structure; capturing in the porous structure the CO2 from the gas mixture (claim 17 meeting limitation “removing CO2 from the gas stream by sorbing CO2 using the CO2 sorbent as the gas stream flows through the longitudinal channels”). Heating the porous structure to release the CO2 (claim 22). The method of claim 22, wherein heating includes exposing the porous structure to steam, wherein the temperature of the steam is about 60° C. to 150° C. (claim 23 meeting limitation “removing the sorbed CO2 from the CO2 sorbent by heating the honeycomb monolith”).
As set forth in MPEP 2144.05, in the case where the claimed range “overlap or lie inside ranges disclosed by the prior art”, a prima facie case of obviousness exists, In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990). In the instant case, the range taught by Pang (60° C. to 150° C.) overlaps with the claimed range (60 °C to 130 °C). Therefore, the range in Pang renders obvious the claimed range.
Pang does not disclose “wherein an amount of time taken for removing the CO-2 from the gas stream is about 3 to 10 times an amount of time taken for removing the sorbed CO2”.
Thompson discloses solid sorbents for gas capture and separation… based on the solidification of polyethyleneimine (PEI), as well as other amines, with polyaldehyde containing phosphorous dendrimers ([0059]). The solid sorbent can be coated onto a support or structural surfaces to afford additional pathways for gas capture ([0059]). In a typical experiment: a solid sorbent (5-30 mg) is placed on a pre-weighed platinum pan which is lowered into the TGA reactor ([0108]). Under a helium atmosphere with a flow rate of 60 mL/min, the sample was heated to 120° C. for 10 minutes, at which point no more weight loss was observed ([0108]). The reactor temperature was adjusted to 65° C. and then pure CO2 was introduced at a flow rate of 60 mL/min for 50 minutes ([0108]). For multiple cycles, the sample would be reheated to 120° C. for 10 minutes to desorb CO2 , and the remaining procedure would be followed as described for as many cycles as was desired ([0108]). Thompson discloses a time taken for removing the CO2 from the gas stream is 50 minutes, and a time taken for removing the sorbed CO2 as 10 minutes. The amount of time taken for removing the CO2 from the gas stream is about 5 times an amount of time taken for removing the sorbed CO2 which is within the claimed range of about 3 to 10. Thompson further discloses regeneration of sorbent proceed smoothly, with complete removal of CO2, realized within the first 5 minutes of heating at 120° C ([0118]).
Thus, prior to the effective filing date of the claimed invention it would have been obvious to one of ordinary skill in the art for an amount of time taken for removing the CO-2 from the gas stream to be about 3 to 10 times an amount of time taken for removing the sorbed CO2 in the method of Pang since this allows complete removal of CO2 as taught by Thompson.
Regarding claim 23, Pang discloses the macropores of the porous structure can have pores having a diameter of about 100 nm to 10,000 nm ([0054] which is equivalent to 0.1 microns to 10 microns.
As set forth in MPEP 2144.05, in the case where the claimed range “overlap or lie inside ranges disclosed by the prior art”, a prima facie case of obviousness exists, In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990). In the instant case, the range taught by Pang (0.1 microns to 10 microns) overlaps with the claimed range (10 nm 50 nm). Therefore, the range in Pang renders obvious the claimed range.
Pang discloses the mesopores of the porous structure can have pores having a diameter of about 5 nm to 100 nm… and a volume of 0.5 – 2 cc/g ([0054]).
As set forth in MPEP 2144.05, in the case where the claimed range “overlap or lie inside ranges disclosed by the prior art”, a prima facie case of obviousness exists, In re Wertheim, 541 F.2d 257, 191 USPQ 90 (CCPA 1976); In re Woodruff, 919 F.2d 1575, 16 USPQ2d 1934 (Fed. Cir. 1990). In the instant case, the range taught by Pang (5 nm to 100 nm) overlaps with the claimed range (10 nm to 50 nm). Therefore, the range in Pang renders obvious the claimed range. In the instant case, the range taught by Pang (0.5 – 2 cc/g) overlaps with the claimed range (0.4 cc/g to 1.5 cc/g). Therefore, the range in Pang renders obvious the claimed range.
Pang discloses the macropores of the porous structure can have… a volume of 0.2-1 cc/g ([0054]). The mesopores of the porous structure can have … a volume of 0.5-2 cc/g ([0054]). In the case where the macropore volume is 1 cc/g and the mesopore volume is 0.5 cc/g, the ratio of macropores to mesopores is 2:1, which is within the claimed range.
Regarding claim 25, Pang in view of Thompsons discloses all the limitations in the claims as set forth above and Pang further discloses the substrate can include a porous coating (also referred to as a "washcoat ”) on the surface of the substrate ([0057]). The porous coating can be about 100 µm to 1500 µm thick and the pores can be of the dimension described above and herein, i.e. macropores and mesopores, ([0057]).
Regarding claim 26, Pang in view of Thompson discloses all the limitations in the claims as set forth above and Pang further discloses the PPI sorbent can be coated or otherwise immobilized on the inside of the pores of the ceramic honeycomb structure and/or within a porous layer on the surface of the ceramic honeycomb structure ([0060]).
Regarding claim 27, Pang in view of Thompson discloses all the limitations in the claims as set forth above and Pang further discloses the PPI sorbent can be physically impregnated in the internal volume pores of the porous structure ([0037]). Aspects of the present disclosure provide a supported amine material, incorporating a physically impregnated poly(propylenimine) (PPI) as the amine, that can be used as a CO2 sorbent in a variety of CO2 capture applications ([0068]).
Regarding claim 28, Pang in view of Thompson discloses all the limitations in the claims as set forth above and Pang further discloses aspect of the disclosure can have a polymer architecture that may be linear or dendritic, as well as branched or hyperbranched ([0070]).
Regarding claim 29, Pang in view of Thompson discloses all the limitations in the claims as set forth above and further discloses the pores (e.g., mesopores ) can be substantially filled by the PPI sorbent and still function to adsorb CO2 ([0036]). While Pang does not explicitly disclose the fraction is about 40% to 100%, this limitation would be obvious to one having ordinary skill in the art given Pang’s disclosure of the pores being substantially filled.
Regarding claim 30, Pang in view of Thompson discloses all the limitations in the claims as set forth above including Pang discloses heating includes exposing the porous structure to steam (claim 23).
Regarding claim 33, Pang in view of Thompson discloses all the limitations in the claims as set forth above including Thompson discloses a time taken for removing the CO2 from the gas stream is 50 minutes, and a time taken for removing the sorbed CO2 as 10 minutes ([0108]).
Thompson further discloses the sorbent reached higher capacities with increasing adsorption temperatures ([0140]). At 25° C. and 45° C., the sorbent obtained capacities of 4.1 wt.% and 9.3 wt.% respectively ([0140]). At 85° C. the adsorption is dominated by the exothermic binding and decreases the capacity to 11.3 wt.% ([0140]). Exposing 1-GO./600PEI to 1 atm of CO2 at 65° C. adsorbed 13.1 wt.% capacity over 50 minutes ([0139]). Therefore, Thompson discloses sorbent capacity is temperature dependent, and therefore time for removing the CO2 from the gas stream is temperature dependent.
Thompson further discloses the reactor temperature was adjusted to 65° C. and then pure CO2 was introduced at a flow rate of 60 mL/min for 50 minutes ([0108]). For multiple cycles, the sample would be reheated to 120° C. for 10 minutes to desorb CO2, and the remaining procedure would be followed as described for as many cycles as was desired ([0108]). Therefore, Thompson discloses the amount of time taken for removing the CO2 from the gas stream is about 5 times an amount of time taken for removing the sorbed CO2 when the gas stream is pure CO2.
Thompsons further discloses adsorption from 15 Vol % CO2, from simulated Flue Gas ([0109]) where the end of the adsorption stage may also be determined by the minimum and maximum adsorption times, which was defined as 30 and 35 min ([0111]). The regeneration end point was determined by the minimum or maximum desorption times of 20 and 25 min, respectively ([0111]).
While Thompson does not explicitly disclose the amount of time taken for removing the C02 from the gas stream is about 3 times the amount of time taken for removing the sorbed CO2, about 9 times the amount of time taken for removing the sorbed CO2, or about 10 times the amount of time taken for removing the sorbed CO2, the ratio of sorption time and desorption time is not considered to confer patentability to the claims. Thompson teaches that it was known in the art at the time of the invention that sorption and desorption time is dependent on temperature and CO2 concentration in the gas stream. Therefore, the time taken for removing the C02 from the gas stream and the amount of time taken for removing the sorbed CO2 are variables that can be modified, among others, by varying the temperature and CO2 concentration. For that reason, the time taken for removing the C02 from the gas stream and the amount of time taken for removing the sorbed CO2 would have been considered a result effective variable by one having ordinary skill in the art at the time the invention was made. As such, without showing unexpected results, the time taken for removing the C02 from the gas stream and the amount of time taken for removing the sorbed CO2. Accordingly, one of ordinary skill in the art at the time the invention was made would have optimized, by routine experimentation, the time taken for removing the C02 from the gas stream and the amount of time taken for removing the sorbed CO2 in the method of Pang in view of Thompson to obtain the desired number of sorption/desorption cycles (In re Boesch, 617 F.2d. 272, 205 USPQ 215 (CCPA 1980)), since it has been held that where the general conditions of the claim are disclosed in the prior art, discovering the optimum or workable ranges involves only routine skill in the art. (In re Aller, 105 USPQ 223).
Claim 22 is rejected under 35 U.S.C. 103 as being unpatentable over Pang et al (US 20190291077 A1) in view of Thompson et al (US 20190224647 A1), and in further view of Addiego (US 20130207034 A1).
Regarding claim 22, Pang in view of Thompson discloses all the limitations in the claims as set forth above but does not disclose “wherein the honeycomb monolith has a channel opening density of about 50 channels per square inch to 400 channels per square inch; wherein the open face area (OFA) of the opposed surfaces is about 0.5 to 0.9; and wherein a length of the honeycomb monolith is about 3 inches to 24 inches”.
Addiego discloses an absorbent structure for CO2, capture includes a honey comb substrate having a plurality of partition walls extending in an axial direction from an inlet end to an outlet end thereby forming a plurality of flow channels (abstract). The absorbent structure also includes a functional mer group dispersed throughout the powder component of the partition walls of the honeycomb substrate (abstract). The functional mer group is positioned in and on the partition walls such that, when a gas stream containing CO2 flows in the flow channels from the inlet end to the outlet end, the functional mer group absorbs the CO2 (abstract). Examples of functional mer groups that absorb CO2 include, but are not limited to, amine polymers ([0036]). The second configuration consisted of a consolidated monolith having about 150-200 flow channels per square inch of the inlet end ([0059]) which is within the claimed range of 50 to 400 channels per square inch. Th flow channels were defined by walls having a minimum thickness from about 0.006 to about 0.009 inches ([0059]). Fig. 3 shows honeycomb substrates with circular cells in a square packing pattern. Cell pitch can be calculated by:
P
i
t
c
h
=
√
1
N
where N is cells per square inch.
150 cells per square inch
200 cells per square inch
Pitch = 0.0817 inches
Pitch = 0.0707 inches
Wall thickness 0.006 inches
Wall thickness 0.009 inches
Open face area = 0.859
Open face area = 0.762
Therefore, Addiego discloses an open face area from 0.762 to 0.859 which is within the claimed range of about 0.5 to 0.9.
Addiego further discloses the monolith is 4 inches in diameter and 6 inches in length ([0014]), where 6 inches in length is within the claimed range of about 3 inches to 24 inches. A particular advantage of this work is that it provides high absorption capacity versus thermal mass of the substrates ([0091]).
Thus, prior to the effective filing date of the claimed invention it would have been obvious to one of ordinary skill in the art for the honeycomb monolith to have a channel opening density of about 50 channels per square inch to 400 channels per square inch; wherein the open face area (OFA) of the opposed surfaces is about 0.5 to 0.9; and wherein a length of the honeycomb monolith is about 3 inches to 24 inches in the method of Pang in view of Thompson in order for the honeycomb monolith to have high absorption capacity versus thermal mass of the substrates as taught by Addiego.
Claim 24 is rejected under 35 U.S.C. 103 as being unpatentable over Pang et al (US 20190291077 A1) in view of Thompson et al (US 20190224647 A1), and in further view of Colombo et al (“Fabrication of ceramic components with hierarchical porosity”).
Pang in view of Thompson discloses all the limitations in the claims as set forth above including Pang discloses a linear PPI is defined as containing only primary amines, secondary amines, or both primary and secondary amines ([0045]). Since Pang discloses PPI is the sorbent ([0036]), the claim limitation “wherein the sorbent comprises an amine” is met.
Pang in view of Thompson does not disclose “wherein the macropore and mesopore containing walls comprises sintered mesoporous particles having macropores separating the mesoporous particles”.
Colombo discloses different methodologies for the fabrication of monolithic ceramic components possessing multiscale porosity, i.e., with pores ranging from a few nanometers to several hundred microns (abstract). A macroporous monolith can serve as a host matrix, to which micro- and/or mesopores are then added using different strategies (Pg. 5437 right col. bottom paragraph). Coating the cell wall surface of a macroporous ceramic with a high SSA layer is a well-established route, which has been widely used to fulfill the specific requirements of industrial applications (such as catalytic converters in automobile industry) for several decades (Pg. 5438 right col. bottom paragraph). Typically, this approach leads to components having bimodal porosity (micro/macro or meso/macro) (Pg. 5439 right col. top paragraph meeting limitation “the macropore and mesopore containing walls” and “having macropores separating the mesoporous particles”). γ-Al2O3 (SSA ~ 200 m2/g) is commonly used as a coating material for cellular ceramics (Pg. 5439 left col. bottom paragraph). This material, deposited on several substrates (foams, honeycombs and ceramic fibers…) using several methods, increases the SSA of the porous body and the structure remains stable up to temperatures of ~ 700-800 °C (Pg. 5439 right col. top paragraph) Typically, a dilute slurry containing the washcoat precursors (particle/colloidal suspension, i.e. mesoporous particles, … and small amounts of viscosity-modifying agents) is deposited on the substrate, which is then dried and calcined at moderate temperatures (~500 °C), i.e. sintered (Pg. 5439 right col. top paragraph through Pg. 5440 left col. top paragraph).
Thus, prior to the effective filing date of the claimed invention it would have been obvious to one of ordinary skill in the art for the macropore and mesopore containing walls to comprise sintered mesoporous particles having macropores separating the mesoporous particles in the method of Pang in view of Thompson in order to increase the SSA (geometric surface area) of the porous body as taught by Colombo.
Claims 31-32 are rejected under 35 U.S.C. 103 as being unpatentable over Pang et al (US 20190291077 A1) in view of Thompson et al (US 20190224647 A1), and in further view of Bourhis et al (WO 2019161114 A1).
Regarding claim 31, Pang in view of Thompson discloses all the limitations in the claims as set forth above but does not disclose “wherein the gas stream has an approach velocity of about 2 m/s to 10 m/s”.
Bourhis discloses a method for capturing carbon dioxide from ambient air… and comprises contacting a packed bed or fluidized bed device with a stream of ambient air, wherein the packed bed or fluidized bed device comprises a humidity-sensitive sorbent material that adsorbs carbon dioxide from the ambient air (abstract). One embodiment of the presently disclosed system 1100 comprises a first stage circulating fluidized bed (CFB) absorber 1104 to capture the C02 from ambient air (which enters the system through inlet 1102) ([0134]). The CFB adsorber 1104 is designed to have a cross-sectional area of approximately 113 m2 (12 meter diameter) and a height of 40 meters, both of which are fairly typical dimensions for industrial-scale CFB-based facilities ([0134]). The height was chosen to ensure sufficient gas-solid contact time with an air intake velocity of approximately 4 meters/sec ([0134]).
Bourhis teaches an air, i.e. gas stream, velocity of 4 meters/sec, which is within the claimed range of about 2 m/s to 10 m/s which allows sufficient gas-solid contact time between the air stream and the sorbent material which absorbs carbon dioxide.
Thus, prior to the effective filing date of the claimed invention it would have been obvious to one of ordinary skill in the art for the gas stream to have an approach velocity of about 2 m/s to 10 m/s in the method of Pang in view of Thompson in order for there to be sufficient gas-solid contact time between the gas stream and the sorbent material as taught by Bourhis.
Regarding claim 32, Pang in view of Thompson and Bourhis discloses all the limitations in the claims as set forth above and Pang further discloses the gas flow was switched to a premixed gas containing 10 % CO2/ N2 ([0111] meeting limitation “CO2 concentration of about 10% or less”). The PPI sorbent can be used to capture CO2, in gas streams including high concentrations of CO2 (e.g., 1 to 15 %, such as in flue gas) ([0033] meeting limitation “wherein the gas is selected from ambient air, flue gas, or a combination thereof”).
Conclusion
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/N.L.Q./Examiner, Art Unit 1738
/MICHAEL FORREST/Primary Examiner, Art Unit 1738