Notice of Pre-AIA or AIA Status
The present application, filed on or after March 16, 2013, is being examined under the first inventor to file provisions of the AIA .
DETAILED ACTION
Claims 1, 4-12 of D. Asari, et al, US 17/610,160 (11/10/2021) are pending. Claims 4-5 and 9-12 are withdrawn as directed to nonelected Groups. Claims 1 and 6-8 are under examination on merits and are rejected.
Election/Restrictions
Pursuant to the restriction requirement, Applicant elected Group V ( now claims 1 and 6-8) with claims amendment by combination of the original claim into claim 1, with traverse, in the reply filed on 03/03/2025. Claims 4-5 and 10-12 drawn to non-elected Groups (I)-(II) are maintained withdrawn from consideration pursuant to 37 CFR 1.142(b). The Restriction requirement is maintained as FINAL.
Claim Interpretation
Examination requires claim terms first be construed in terms in the broadest reasonable manner during prosecution as is reasonably allowed in an effort to establish a clear record of what applicant intends to claim See MPEP § 2111. Under a broadest reasonable interpretation, words of the claim must be given their plain meaning, unless such meaning is inconsistent with the specification. See MPEP § 2111.01. It is also appropriate to look to how the claim term is used in the prior art, which includes prior art patents, published applications, trade publications, and dictionaries. MPEP § 2111.01 (III).
Interpretation of the Claim Term “Poor Solvent”
The specification defines the term of “poor solvent” as:
Here, the term "poor solvent" for an object means that the solubility in a solvent of the object is 1g/50mL (=20g/L) or less at 25°C and at atmospheric pressure.
Specification at page 5, line 3-4. Therefore, the term of “poor solvent” is interpreted as defined by the specification.
Interpretation of the Claim Term “a Centrifugal Force and a Shear Force”
The specification does not provide specific definition for the terms “centrifugal force” or “shear force”. The specification discusses these terms as follows:
[0012] Some aspects of the present invention are as described below.
[1] A method for producing a Metal-Organic Framework, comprising: simultaneously and continuously applying a centrifugal force and a shear force to a formulation containing a metal ion donor, a multidentate ligand, and a solvent.
. . . .
[6] The method according to any one of [1] to [5], wherein the centrifugal force is generated by stirring the formulation by rotating a rotary blade within a reaction vessel, and the shear force is generated by contact between the formulation and an inner wall of the reaction vessel due to the stirring, or by contact between particles constituting the formulation due to the stirring.
Specification at page 6, line 12-30. Thus, the specification recognizes that “centrifugal force” and “shear force” can be generated by simple agitation of a reaction mixture, such that there is some degree of rotation of the reaction mixture.
The prior art teaches that centrifugal force is an outward force on a mass when it is rotated. See V. Wowk, Sound & Vibration 13 (2015) (“Wowk”).
Therefore, the term of “a centrifugal force” is broadly and reasonably interpreted and consistent with the specification as any outward force formed when a mass is rotated in any manner .
The prior art teaches that shear force is a force determined from a free-body diagram, which acts tangentially to a surface which may be a real external surface or a defined surface within a material. See Oxford Dictionary of Mechanical Engineering(1 ed) (2013).
Therefore, the term of “shear force” is broadly and reasonably interpreted and consistent with the specification as any force caused by one object contact another object in any manner.
Interpretation of the Claim Term “thin film swirl mixing method”
Claim recites the claim term of “thin film swirl mixing method” as follows:
7. The method according to claim 1, wherein the centrifugal force and the shear force are applied to the formulation by a thin film swirl mixing method.
The specification does not provide specific definition for the term of “thin film swirl mixing method”. The closest information disclosed by the specification as:
[0033] One example of such a method is the thin film swirl mixing method developed by Primix Corporation. In this method, by using a thin film swirling high-speed mixer, centrifugal force and shear force can be simultaneously and continuously applied to the introduced substance. As a result, in the conventional use example, particles and droplets are dispersed and/or atomized. Specific device configurations are disclosed, for example, in JPA2007-125454.
Specification at page 6, [0033], emphasis added.
It should be noted that “a thin film swirl mixing method” is not an art recognized term. Therefore, according to its plain meaning and consistent with the specification of the instant application, the claim term of “thin film swirl mixing method” is broadly and reasonably interpreted as a method of mixing wherein the material being mixed forms a thin-film by way of a centrifugal force or swirling.
Withdrawal Claim Rejections - 35 U.S.C. 112(a)(Written Description)
Rejection of claims 1, 6-8 are rejected under 35 U.S.C. 112(a)(Written Description) is withdrawn in view of the instant claim 1 has the follows new limitations on the claimed metal ion donor and on the claimed multidentate ligand:
The metal element of the metal ion donor is selected from the group consisting of magnesium, calcium, iron, aluminum, zinc, copper, nickel, cobalt, zirconium, and chromium, and the metal ion donor is selected from the group consisting of hydroxides, carbonates, chlorides, and oxides, and wherein the multidentate ligand is selected from the group of carboxylic acid anions, amine compounds, sulfonic acid anions, phosphate anions, and heterocyclic compounds.
Withdrawal Claim Rejections - 35 USC § 102 (AIA )
Rejection of claim Claims 1, and 6-8 under 35 U.S.C. 102(a)(1) as being anticipated by J. Kim, et al. 161 Microporous and mesoporous materials 48-55 (2012) (“Kim”) is withdrawn in view of in view of the instant claim 1 has the follows new limitation on the recited the metal ion donor:
The metal element of the metal ion donor is selected from the group consisting of magnesium, calcium, iron, aluminum, zinc, copper, nickel, cobalt, zirconium, and chromium, and the metal ion donor is selected from the group consisting of hydroxides, carbonates, chlorides, and oxides
which cannot be met by Kim’s metal donor that is copper (II) nitrate hydrate.
Further, Applicant submits the Declaration of inventor Daisuke ASARI filed the Declaration under 37 CFR § 1.132 (02/27/2026). The Declaration states that:
7. I submit this declaration under 37 C.F.R. 1.132 to clarify that Example 13 is not a working example within the scope of the currently pending Claim 1. Rather, Example 13 is a working example only with respect to originally filed Claim 1. The scope of the currently pending Claim 1 is narrowed to require that . . . .. In view of these narrowing limitations, Example 13 no longer falls within the scope of the currently pending Claim 1 and is therefore excluded as a working example of that claim.
The Declaration at 7.
Given the Declaration states that Example 13 is a working example only with respect to originally filed Claim 11 (which does not limit the solvent is a poor solvent for at least one of the metal ion donor and the multidentate ligand) rather than the instant claim 1, therefore, the 102 rejection based on Example 13 is an working example made in the previous Office action is withdrawn.
Withdrawal Claim Rejections - 35 USC § 103
Rejection of claims 7 under 35 U.S.C. 103 over J. Kim, et al. 161 Microporous and mesoporous materials 48-55 (2012)(“Kim”) as applied for the rejection of claim 1 further in view of H. Shibuya, et JP2007125454A (2005)(“Shibuya”) is withdrawn for the same reason as given above.
Maintained Claim Rejections - 35 USC § 103
The following is a quotation of 35 U.S.C. 103 which forms the basis for all obviousness rejections set forth in this Office action:
A patent for a claimed invention may not be obtained, notwithstanding that the claimed invention is not identically disclosed as set forth in section 102, if the differences between the claimed invention and the prior art are such that the claimed invention as a whole would have been obvious before the effective filing date of the claimed invention to a person having ordinary skill in the art to which the claimed invention pertains. Patentability shall not be negated by the manner in which the invention was made.
The factual inquiries 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.
Rejection of claims 1, 6-8 under 35 U.S.C. 103 over J. Kim, et al. 161 Microporous and mesoporous materials 48-55 (2012)(“Kim”) in view of G. Majano, et al, 25(7) Advanced Materials 1052-1057 (2013) (Majano) is maintained.
J. Kim, et al. 161 Microporous and mesoporous materials 48-55 (2012)(“Kim”)
Kim teaches that metal organic framework, Cu3(BTC)2 was prepared by ethanol reflux method comprising H3BTC (1,3,5-benzenetricarboxylic acid) as the ligand with a concentration of 1.01 M, and Cu salt/H3BTC mole ratio of 9:5 has excellent textural properties (>1700 m2/g) in yield in the range of 40–76% − depending on the stirring rate − after 24 h synthesis. Kim at Abstract, emphasis added; and page 51, left col. paragraph 1, id.
Per the experimental section, Kim teaches that the Cu salt used by Kim is copper (II) nitrate hydrate. Kim at page 49, 2.1, 2.1. Synthesis of Cu3(BTC)2 by ethanol reflux.
Thus, Kim teaches a method preparation of metal organic framework Cu3(BTC)2 from a mixture of 1,3,5-benzenetricarboxylic acid, copper (II) nitrate hydrate and ethanol; wherein the concentration of 1,3,5-benzenetricarboxylic acid, copper (II) nitrate hydrate is 1.01 M, 1.82 M respectively. Therefore, the weight ratio between ethanol (1 ml × 0.789 g/ml = 0.789 g) which is a solvent and the total amount of copper (II) nitrate hydrate ( 1 ml ×1.82 mmol/ml x 187 mg/mmol=340 mg) which is a metal ion donor and 1,3,5-benzenetricarboxylic acid (1 ml ×1.01 mmol/ml x 210 mg/mmol=212 mg) which is a multidentate ligand is 143% [789÷(212+340=1.43]; which anticipated the claim 1 limitation of:
an amount of the solvent is in a range of 100% to 1000% by weight based on a total amount of the metal ion donor and the multidentate ligand
Per table 1, Kim teaches that the synthesis of MOF Cu3(BTC)2 is conducted at a condition of stirring with a rpm 150-300.
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Kim at page 50, right col. Table 1.
Thus, the Kim method also meets the claim 1 limitation of:
reacting a metal ion donor and a multidentate ligand in a solvent to obtain the Metal-Organic Framework by simultaneously and continuously applying a centrifugal force and a shear force to a formulation containing the metal ion donor, the multidentate ligand, and the solvent
because stirring with a stirring bar provides a simultaneously and continuously applying a centrifugal force and a shear force to the retraction mixture per claim interpretation above.
Difference between Kim and Claims 1, 6-8
The Kim method differs from the instant claim 1 in that ethanol is not a poor solvent for at least one of 1,3,5-benzenetricarboxylic acid and copper (II) nitrate hydrate.
G. Majano, et al, 25(7) Advanced Materials 1052-1057 (2013) (Majano)
Majano teaches a method for scalable conversion of copper (II) hydroxide into MOF Cu3(BTC)2 which also named as HKUST-1. Majano at title, emphasis added.
Majano teaches that:
Excluding the last example, the rest of the work on Cu-based (and several other) MOFs has been carried out using soluble metal salts such as nitrates. The latter are oxidizers and may constitute a safety hazard in industrial use. Other soluble precursors such as acetates are cost-wise prohibitive. An appealing alternative, from safety and economic standpoints, is copper(II) hydroxide. The conversion of Cu(OH)2 into HKUST-1 would be desirable, as the resulting process expressed as a simple acid-base reaction: 3 Cu(OH)2 + 2 H3btc → Cu3btc2 + 6 H2O, is waste-free and sets aside issues concerning by-product anions such as Cl− and NO3−. Chlorides tend to increase corrosion levels in the mixture while nitrates require special attention in high volumes due to the exothermic nature of MOF synthesis. Additionally, one should bear in mind that salt removal in waste water is costly. Despite all these considerations, in laboratory practice the insoluble nature of Cu(OH)2 has kept it far from its utilization as a precursor for the MOF synthesis. Upon closer examination, despite its insoluble character, its structure is relatively flexible as put in evidence by intercalation of organics akin to clay-based chemistry, which can be also applied to other layered metal hydroxides. [ 21 ] As described by Jaggi and Oswald,[22] Cu(OH)2 consists of chains of distorted octahedra organized as corrugated layers. The Cu-Cu distance between layers lies in the range of 2.95–3.34 Å, which would be ideal for diffusion of linker molecules and subsequent rearrangement into HKUST-1 with Cu-Cu distances of 2.63 Å.
Majano at page 1052, left col. paragraph 3, line 1 to right col. paragraph 3, emphasis added.
Obvious Rationale of Claims 1, 6-8
It would have been prima facie obvious for one skilled artisan to arrive at the instantly claimed invention based on the teachings from Kim and Majano with a reasonable expectation of success before the effective filing date of the claimed invention.
Claim 1, 6-8 are obvious because one ordinary skilled artisan seeking Cu3(BTC)2 is motivated to modify the Kim method by replacing copper (II) nitrate hydrate with Cu(OH)2 that is insoluble as taught by Majano, thus arrive at a method meeting each and every limitation of claims 1, 6-8 for the same reason given in the 102 rejection above.
One ordinary skilled artisan has a motivation to do so with a reasonable expectation of success because Majano teaches that:
(i). copper (II) nitrate may constitute a safety hazard in industrial use;
(ii). The conversion of Cu(OH)2 into Cu3(BTC)2 would be desirable, as the resulting process expressed as a simple acid-base reaction: 3 Cu(OH)2 + 2 H3btc → Cu3btc2 + 6 H2O, is waste-free and sets aside issues concerning by-product anions;
(iii). The structure of Cu(OH)2 is ideal for diffusion of linker molecules and subsequent rearrangement into Cu3(BTC)2
The Rationale supporting the modification is simple substitution of one known element for another to obtain predictable results. MPEP 2143. I (B).
Applicant’s Argument
Applicant first argument on the ground that:
Kim discloses a conventional solvothermal synthesis of Cu3(BTC)2 conducted under ethanol reflux. A person of ordinary skill in the art would not have been motivated to substitute copper nitrate with an insoluble metal source such as Cu(OH)2 in such a reflux-based synthetic system. The insolubility of Cu(OH)2 in ethanol is incompatible with a homogeneous reflux process and would be expected to hinder dissolution, coordination, and ultimately the formation of a high-quality MOF under Kim's liquid-phase conditions.
Remarks filed on 02/27/2026 at page 9, V. Claim Rejections under 35 U.S.C. Q103, to page 10, line 2.
This argument has been fully considered but not persuasive. As mentioned in the previous Office action that Majano teaches that while despite its insoluble character, Cu(OH)2 consists of chains of distorted octahedra organized as corrugated layers. The Cu-Cu distance between layers lies in the range of 2.95–3.34 Å, which would be ideal for diffusion of linker molecules and subsequent rearrangement into HKUST-1. (See Majano at page 1052, left col. paragraph 3, line 1 to right col. paragraph 3). Given Majano teaches Cu(OH)2 is a waste-free metal donor and is ideal for diffusion of linker molecules and subsequent rearrangement into Cu3(BTC)2, one ordinary skill seeking Cu3(BTC)2 is motivated to modify the Kim method by replacing copper nitrate with Cu(OH)2 .
Applicant also argues on the ground that the viscosity and physical state of Majano's mixture would not permit the simultaneous and continuous application of centrifugal and shear forces to a semi-solid formulation. Remarks filed at 02/27/2026 at page 10, paragraph 2. This argument is not persuasive because the proposed method is to modify the Kim’s reaction mixture (wherein the concentration of Cu2+ is 1.82 M) rather the Majano's mixture.
Applicant further argues on the ground that Kim does not teach to apply a thin film swirl mixing method. Remarks filed at 02/27/2026 at page 10, paragraph 3. This argument is not persuasive because as discussed in the Claim Interpretation above that “thin film swirl mixing method” is broadly and reasonably interpreted as a method of mixing wherein the material being mixed forms a thin-film by way of a centrifugal force or swirling. Given Kim teaches that the reaction mixture is stirred with a rpm 150-300, a thin film of the reaction mixture is formed on the wall of the reaction flask by a centrifugal force during the stirring.
Conclusion
THIS ACTION IS MADE FINAL. 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 FRANK S. HOU whose telephone number is (571)272-1802. The examiner can normally be reached Friday.
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/FRANK S. HOU/Examiner, Art Unit 1692
/ALEXANDER R PAGANO/Primary Examiner, Art Unit 1692
1 The original claim 1 filed on 11/10/2021 as:
1. A method for producing a Metal-Organic Framework, comprising: simultaneously and continuously applying a centrifugal force and a shear force to a formulation containing a metal ion donor, a multidentate ligand, and a solvent.