Patent Application 17774485 - COMPOSITIONS COMPRISING A MECHANOCHEMICALLY

Title: COMPOSITIONS COMPRISING A MECHANOCHEMICALLY CARBOXYLATED MINERAL FILLER AND A CEMENT AND/OR ASPHALT BINDER

Application Information

Invention Title: COMPOSITIONS COMPRISING A MECHANOCHEMICALLY CARBOXYLATED MINERAL FILLER AND A CEMENT AND/OR ASPHALT BINDER
Application Number: 17774485
Submission Date: 2025-04-07T00:00:00.000Z
Effective Filing Date: 2022-05-05T00:00:00.000Z
Filing Date: 2022-05-05T00:00:00.000Z
National Class: 106
National Sub-Class: 405000
Examiner Employee Number: 99460
Art Unit: 1731
Tech Center: 1700

Rejection Summary

102 Rejections: 0
103 Rejections: 2

Cited Patents

No patents were cited in this rejection.

Office Action Text

DETAILED ACTION

Response to Amendment
In response to the amendment received on 01/07/2025:
claims 1-6, 8-11 and 16-24 are currently pending
claim 7 is canceled
claims 1-6, 8-11 are amended
claims 16-24 are added
the objections of the claims have been withdrawn in light of the amendments to the claims
the 112(b) rejections have been withdrawn in light of the amendment to the claims
new 112(b) rejection addressing amended claim 6 is presented herein
new grounds of rejection presented herein

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.

Claim 6 is 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 6, the phrase "preferably" renders the claim indefinite because it is unclear whether the limitation(s) following the phrase are part of the claimed invention. See MPEP § 2173.05(d).
For the purpose of claim interpretation, it is noted that claim 6 will be treated as limited by the limitation prior to phrase “preferably”.

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.
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 1-6, 9-11 and 16-24 are rejected under 35 U.S.C. 103 as being unpatentable over Monkman et al. (WO 2017/000075 A1), hereinafter referred to as MONKMAN, in view of Ji et al. (Insights into carbonation kinetics of fly ash from Victorian lignite for CO2 sequestration, Energy Fuels, 2018, 32, pages 4569-4578), hereinafter referred to as JI.

Regarding claim 1, MONKMAN teaches composition comprising a mechanochemically carboxylated mineral filler and a binder (see MONKMAN at Abstract: combining the carbonated fly ash with a cement binder); wherein the binder is selected from the group consisting of cement (see MONKMAN at Abstract), asphalt and combination thereof; and wherein the mechanochemically carboxylated mineral filler is obtainable by a method comprising the following steps:
providing a solid feedstock comprising a silicate mineral (see MONKMAN at paragraph [0030]: Class C fly ash);
providing an oxidizing gas comprising CO2 (see MONKMAN at paragraph [0030]: fly ash is treated with carbon dioxide);
introducing said solid feedstock and said oxidizing gas into a mechanical agitation unit (see MONKMAN at paragraph [0044]: fly ash may be carbonated by the use of mixing silo); and
subjecting the material of said solid feedstock to a mechanical agitation operation in the presence of said oxidizing gas at an oxidizing gas pressure of more than 1 atm to obtain the mechanochemically carboxylated mineral filler (see MONKMAN at paragraphs [0053]- [0054]: mixture (fly ash, water and sand) was subjected to carbonation in a sealed vessel under the following conditions: 25 psi/1.7 atm, 6 RPS mixing);
wherein the CO2 content of the mechanochemically carboxylated mineral filler is more than 1 wt.% (by total weight of the mechanochemically carboxylated mineral filler) (see MONKMAN at paragraph [0034]: the mass of carbon dioxide converted to stable form per mass of fly ash is at least 1%); MONKMAN teaches range of at least 1%, which overlaps with the claimed range;
wherein step (d) comprises grinding or milling (see MONKMAN at paragraph [0025]: grinding or blending of fly ash in presence of moisture and CO2);
It is noted that the statement “wherein the CO2 content is determined as the mass loss above 120°C measured by TGA-MS employing a temperature trajectory wherein the temperature was increased from room temperature to 800°C at a rate of 10°C/min and then decreased to room temperature at a rate of 15°C/min” is not considered as further limiting structurally a mechanochemically carboxylated fly ash.
While MONKMAN fails to explicitly teach the solid feedstock is a particulate material which has a BET surface area of more than 0.01 m2/g and a D50 within the range of 0.1-5000 µm, MONKMAN discloses fly ash composition with a Blaine fitness of minimum 100 m2/kg (0.1 m2/g) (see MONKMAN at paragraph [0038]). MONKMANN also fails to explicitly teach the mechanochemically carboxylated mineral filler having a D90 within the range of 20-100 µm and/or D50 within the range of 0.5-50 µm.
However, JI teaches carbonation reactions of fly ash carried out in an autoclave reactor comprising the following steps: (1) water and fly ash were added to autoclave and heated to desired temperature, (2) high-purity CO2 gas (99.99%) was injected into the vessel to a given pressure, (3) magnetic stirring was initiated and fly ash particles were dispersed (see JI at 2.2. Aqueous carbonation experiments in a vessel reactor, p. 4570). JI also teaches particle size and surface area of fly ash samples, e.g., D50=8.40 µm and BET surface area of 30.29 m2/g (see JI at Table 1). JI also discloses the morphology characterization of carbonated fly ash (see JI at Fig. 4: sample C-1: D90 = 20.53 µm and D50 = 7.33 µm). JI teaches ranges which are within the claimed ranges. Additionally, JI discloses that the particle size and surface area significantly affect both carbonation rate and efficiency, and that the physical properties of the fly ash suggest that pretreatment grinding is not required prior to mineral carbonation (see JI at 3.1. Physical and chemical properties, p. 4571).
One of ordinary skill in the art would have recognized the potential benefit of utilizing the fly ash with a BET surface area and D50 as disclosed by JI in the method of MONKMAN since JI explicitly teaches that the particle size and surface area significantly affect both carbonation rate and efficiency, and that the physical properties of the fly ash suggest that pretreatment grinding is not required prior to mineral carbonation (see JI at 3.1. Physical and chemical properties, p. 4571). Moreover, one of ordinary skill in the art would have recognized that utilization of fly ash disclosed by JI would result in obtaining carboxylated product with D90 and D50 within the claimed range.
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have utilized fly ash with D50 of 8.40 µm and BET surface area of 30.29 m2/g as disclosed by JI to obtain the mechanochemically carboxylated mineral filler of MONKMAN in order to avoid pretreatment grinding prior to mineral carbonation.
Regarding claim 2, MONKMAN as modified by JI teaches the composition according to claim 1, wherein the solid feedstock comprises of a material selected from the group consisting of pyroxenes, hydrous magnesium silicates, talc, serpentines, olivine, fly ash (see MONKMAN at paragraph [0030]), bottom ash and combination thereof.
Regarding claim 3, MONKMAN as modified by JI teaches the composition of claim 2, wherein the solid feedstock comprises fly ash (see MONKMAN at paragraph [0030]) which meets ASTM C618 (2019) requirements (see MONKMAN at Abstract and paragraph [0024]).
Regarding claim 4, MONKMAN as modified by JI teaches the composition according to claim 1, wherein the mechanochemically carboxylated mineral filler has a D50 within the range of 0.5-50 µm (see rejection of claim 1 above, and JI at Fig. 4: sample C-1: D50 = 7.33 µm). JI teaches 7.33 µm, which is within the claimed range of 0.5-50 µm.
Regarding claim 5, MONKMAN as modified by JI teaches the composition according to claim 1, wherein the oxidizing gas comprises more than 90 mol% CO2 (see MONKMAN at paragraph [0032]: the carbon dioxide is more than 99% pure). MONKMAN teaches range, which is within the claimed range.
Regarding claim 6, MONKMAN as modified by JI teaches the composition according to claim 1, but MONKMAN fails to explicitly teach wherein step (d) is performed
at a pressure of more than 3 atm,
at a temperature less than 100°C,
for at least 1 hour.
However, JI teaches the carbonation efficiency of fly ash in the carbonation reaction as a function of time at different temperatures (40, 50, 60 and 70°C) and CO2 pressures (3, 4, 5 6 and 7 bar or 2.9, 3.9, 4.9, 5.9 and 6.9 atm) (see JI at 3.3.1. Effects of operational parameters on the carbonation reaction, p. 4572). JI also teaches that the carbonation efficiency increased rapidly in the first 2 h and reached a maximum value after 8 h reaction (see JI at Figure 2 (a and c), and 3.3.1. Effects of operational parameters on the carbonation reaction, p. 4572). JI also discloses that due to rapid carbonation reaction at elevated temperatures, the fly ash particles were quickly converted by the rapidly formed product layer, which resulted in a low maximum carbonation efficiency at elevated temperatures (see JI at Figure 2a and 3.3.1. Effects of operational parameters on the carbonation reaction, sentence spanning pages 4572-4573). Additionally, JI discloses that as the initial CO2 pressure increased from 3 to 7 bar, the carbonation rate and the maximum carbonation efficiency increased, indicating the significant impact of CO2 pressure on the carbonation reaction; increasing CO2 pressure also increases the CO2 solubility in the solution and thus increases the carbonate ions available for the carbonation reaction (see JI at Figure 2c and 3.3.1. Effects of operational parameters on the carbonation reaction, p. 4573).
One of ordinary skill in the art would have recognized the potential need to improve the method of MONKMAN by utilizing the operational parameters of JI. Moreover, one of ordinary skill in the art would have been motivated to perform fly ash carbonation of MONKMAN at a pressure of 7 bar, temperature of 40°C for at least 2 h as disclosed by JI, since JI explicitly teaches the highest carbonation efficiency (see JI at Figure 2 (a and c)).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective foiling date of the claimed invention to have modified the method of fly ash carbonation of MONKMAN by adjusting the operational parameters to reap the benefits disclosed by JI such as to achieve high carbonation efficiency.
Regarding claim 9, MONKMAN as modified by JI teaches the composition according to claim 1, wherein the binder is a cement (see MONKMAN at paragraph [0030]).
Regarding claim 10, MONKMAN as modified by JI teaches the composition according to claim 1, comprising more than 1 wt.% by the total weight of the composition of the mechanochemically carboxylated mineral filler and more than 20 wt.% by the total weight of the composition of the binder (see MONKMAN at paragraph [0030]: the carbonated fly ash displaces at least 2% of the cement binder). MONKMAN teaches 2% of the carboxylated fly ash and 98% of the binder, which are within the claimed ranges.
Regarding claim 11, MONKMAN as modified by JI teaches the composition according to claim 1, comprising 5-70 wt.% by the total weight of the composition of the mechanochemically carboxylated mineral filler and 30-95 wt.% by the total weight of the composition of the binder (see MONKMAN at paragraph [0030]: the carbonated fly ash displaces at least 30% of the cement binder). MONKMAN teaches 30% of the carboxylated fly ash and 70% of the binder, which are within the claimed ranges.
Regarding claim 16, MONKMAN as modified by JI teaches the composition according to claim 1, wherein the feedstock comprises fly ash (see MONKMAN at paragraph [0030]).
Regarding claim 17, MONKMAN as modified by JI teaches the composition according to claim 16, wherein the feedstock consists of fly ash (see MONKMAN at Abstract: carbonating the fly ash).
Regarding claim 18, MONKMAN as modified by JI teaches the composition according to claim 4, wherein the mechanochemically carboxylated mineral filler has a D50 within the range of 1-25 µm (see rejection of claim 1 above, and JI at Fig. 4: sample C-1: D50 = 7.33 µm).
Regarding claim 19, MONKMAN as modified by JI teaches the composition according to claim 6, wherein step (d) is performed for at least 1 hour (see rejection of claim 6 above and JI at Figure 2 (a and c): carbonation up to 8 h). JI teaches carbonation time range which overlaps with the claimed range.
Regarding claim 20, MONKMAN as modified by JI teaches the composition according to claim 6, wherein step (d) is performed for at least 4 hours (see rejection of claim 6 above and JI at Figure 2 (a and c): carbonation up to 8 h). JI teaches carbonation time range which overlaps with the claimed range.
Regarding claim 21, MONKMAN as modified by JI teaches the composition according to claim 19, wherein step (d) is performed at a temperature of less than 100°C (see rejection of claim 6 above and JI at Figure 2: temperature of 40, 50, 60 and 70°C). JI teaches temperatures which are within the claimed range.
Regarding claim 22, MONKMAN as modified by JI teaches the composition according to claim 9, wherein the binder is Portland cement (see MONKMAN at Abstract: cement binder such as Portland cement).
Regarding claim 23, MONKMAN as modified by JI teaches the composition according to claim 10, comprising more than 5 wt.% by the total weight of the composition, of the mechanochemically carboxylated mineral filler and more than 20 wt.% by the total weight of the composition of the binder (see MONKMAN at paragraph [0030]: the carbonated fly ash displaces at least 10% of the cement binder). MONKMAN teaches 10% of the carboxylated fly ash and 90% of the binder, which are within the claimed ranges.
Regarding claim 24, MONKMAN as modified by JI teaches the composition according to claim 1, wherein the CO2 content of the mechanochemically carboxylated mineral filler is more than 5 wt.% (see MONKMAN at paragraph [0034]: the mass of carbon dioxide converted to stable form per mass of fly ash is at least 1%); MONKMAN teaches range of at least 1%, which overlaps with the claimed range.

Claim 8 is rejected under 35 U.S.C. 103 as being unpatentable over MONKMAN in view of JI as applied to claim 1 above, and further in view of Constantz et al. (WO 2016/160612 A1), hereinafter referred to as CONSTANTZ.

Regarding claim 8, MONKMAN as modified by JI teaches the composition according to claim 1, but fails to explicitly teach wherein step (d) is performed in the presence of a transition metal oxide catalyst.
However, CONSTANTZ teaches modular units configured for use in sequestering CO2 and methods for using the unit/systems in CO2 sequestration protocol (see CONSTANTZ at Abstract). CONSTANTZ also teaches CO2 mineralization subunit (see CONSTANTZ at line 27, p. 9) and the CO2 sequestering carbonate material (see CONSTANTZ at lines 32-34, p. 9). Additionally, CONSTANTZ discloses that CO2 containing gas can be contacted with the capture liquid in the presence of a catalyst that mediates the conversion of CO2 to bicarbonate (see CONSTANTZ at lines 31-34, p. 35); and when employed, the catalyst is present to provide the rate increase of bicarbonate production (see CONSTANTZ at lines 24-26, p. 36). Finally, CONSTANTZ teaches that colloidal metal particles, e.g., transition metal nanoparticles, can be made available in the reaction using any convenient approach (see CONSTANTZ at lines 1-2, p. 38). CONSTANTZ also discloses colloidal metal particles, such as those described in Bhaduri and Siller: nickel nanoparticles, and the like, e.g., colloidal metal oxide nanoparticles (see CONSTANTZ at lines 9-13, p. 36).
The role of bicarbonate production in the process of fly ash carbonation is demonstrated by JI teaching that fly ash comprises CaO and MgO, indicating its capacity for CO2 sequestration (see JI at 3.1. Physical and chemical properties, p. 4571), and disclosing the carbonation reaction pathways (see JI at 2.3. Reaction pathways, p. 4571). The equations 5-11 demonstrate the formation of bicarbonate (equation 6), and its role in the formation of calcite (equations 7-11).

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One of ordinary skill in the art would have recognized the potential need to improve the method of MONKMAN by performing the carbonation step in the presence of a catalyst such as transition metal nanoparticles, as disclosed by CONSTANTZ since CONSTANTZ explicitly teaches that when employed, the catalyst is present to provide the rate increase of bicarbonate production (see CONSTANTZ at lines 24-26, p. 36).
Therefore, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to have modified the method of MONKMAN by performing the carbonation step in the presence of a catalyst as disclosed by CONSTANTZ in order to increase the rate of bicarbonate production.

Response to Arguments
Applicant's arguments filed on 01/07/2025 have been fully considered but they are not persuasive.
Applicant argues that neither MONKMAN or JI describe a mechanochemical carbonation method such as claimed. See Remarks received on 01/07/2025 at i) on page 8.
However, the Examiner respectfully disagrees for the following reasons. While MONKMAN does not explicitly disclose mechanochemically carboxylated fly ash, MONKMAN teaches mixture (fly ash, water and sand) was subjected to carbonation in a sealed vessel under the following conditions: 25 psi/1.7 atm, 6 RPS mixing (see MONKMAN at paragraphs [0053]- [0054]); as well as grinding or blending of fly ash in presence of moisture and CO2 (see MONKMAN at paragraph [0025]). And while JI does not explicitly disclose mechanochemically carboxylated fly ash, JI teaches that carbonation reaction was performed under pressure and stirring (see JI at 2.2 Aqueous carbonation experiments in a vessel reactor, p. 4570). Additionally, according to MPEP §2111 claims should be given their broadest reasonable interpretation in light of the specification. Specification, paragraph [0050], discloses that “step (d) comprises a mechanical agitation operation… stirring (low-speed stirring or high-speed stirring)”; according to paragraphs [0046] and [0047]: “step (d) is performed at the pressure of more than 3 atm”, and “the mechanochemical carboxylation methods described herein are preferably performed without employing a strong acid, preferably without employing any further oxidizing agent”. Therefore, JI’s disclosure of performing carbonation reaction in a pressurized vessel under stirring reads on the limitations of claim 1 as set forth.
According to MPEP §2141.03(I) “the level of disclosure in the specification of the application under examination or in relevant references may also be informative of the knowledge and skills of a person of ordinary skill in the art”, therefore, the Examiner asserts what an ordinary artisan would know in light of the disclosure in the specification provided by the Applicant. Please note, that the arguments as to what an ordinary artisan would know or understand, when only argued by the Applicant is not supported by independent factual evidence to be persuasive and is mere attorney arguments, and that it’s the burden of the Applicant to offer facts to support the positions.
In response to Applicant arguments that none of MONKMAN or JI teach or suggest a method comprising grinding or milling, it is noted that the added limitation of “grinding” was addressed in rejection of claim 1 above (see MONKMAN at paragraph [0025]: grinding or blending of fly ash in presence of moisture and CO2).
Applicant argues that MONKMAN in view of JI fails to teach or suggest a mechanochemically carboxylated mineral filler has a D90 within the range of 20-100 µm and/or a D50 within the range of 0.5-50 µm. See Remarks received on 01/07/2025 at iii) on pages 9-10.
However, the Examiner respectfully disagrees for the following reasons. As was discussed in the rejection of claim 1 above, JI explicitly teaches the morphology characteristics of the carbonated fly ash. Additionally, MPEP §2112.01(I) states that “where the claimed and prior art products are identical or substantially identical in structure or composition, or are produced by identical or substantially identical processes, a prima facie case of either anticipation or obviousness has been established. In re Best, 562 F.2d 1252, 1255, 195 USPQ 430, 433 (CCPA 1977). Therefore, since MONKMAN teaches the carbonation steps as set forth in claim 1, the claimed properties such as D90 and/or D50 are presumed to be inherent.
In response to applicant’s arguments that MONKMAN in view of JI fails to teach or suggest a mechanochemically carbonated filler wherein the C02 content of the mechanochemically carboxylated mineral filler is more than 1 wt. % (by total weight of the mechanochemically carboxylated mineral filler) wherein the C02 content is determined as the mass loss above 120°C measured by TGA-MS (see Remarks received on 01/07/2025 at iv) on page 10), it is noted that the statement “wherein the CO2 content is determined as the mass loss above 120°C measured by TGA-MS employing a temperature trajectory wherein the temperature was increased from room temperature to 800°C at a rate of 10°C/min and then decreased to room temperature at a rate of 15°C/min” is not considered as further limiting structurally a mechanochemically carboxylated fly ash.
Therefore, the rejection of amended and added claims as being unpatentable over MONKMAN in view of JI and CONSTANTZ is maintained.

Conclusion
The prior art made of record and not relied upon is considered pertinent to applicant's disclosure.
Tanikella et al. Updating Physical and Chemical Characteristics of Fly Ash for Use in Concrete. Joint Transportation Research Program, Report Number: FHWA/IN/JTRP-2017/11 • DOI: 10.5703/1288284315213 (Table 4.1)
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 ANASTASIA KUVAYSKAYA whose telephone number is (703)756-5437. The examiner can normally be reached Monday-Thursday 7:30am-6:00pm.
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If attempts to reach the examiner by telephone are unsuccessful, the examiner’s supervisor, Bryan Ripa can be reached on 571-270-7875. The fax phone number for the organization where this application or proceeding is assigned is 571-273-8300.
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/A.A.K./Examiner, Art Unit 1731
/BRYAN D. RIPA/Supervisory Patent Examiner, Art Unit 1731

Patent Application 17774485 - COMPOSITIONS COMPRISING A MECHANOCHEMICALLY - Rejection

Patent Application 17774485 - COMPOSITIONS COMPRISING A MECHANOCHEMICALLY

Application Information

Rejection Summary

Cited Patents

Office Action Text

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