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 .
Specification
The use of the term Tween (for example, “Tween 80 and tween 60” in [0020]), which is a trade name or a mark used in commerce, has been noted in this application. The term should be accompanied by the generic terminology; furthermore, the term should be capitalized wherever it appears or, where appropriate, include a proper symbol indicating use in commerce such as ™, SM , or ® following the term.
Although the use of trade names and marks used in commerce (i.e., trademarks, service marks, certification marks, and collective marks) are permissible in patent applications, the proprietary nature of the marks should be respected and every effort made to prevent their use in any manner which might adversely affect their validity as commercial marks.
The disclosure is objected to because of the following informalities:
In [0028], the acronym TEM should be defined.
In [0030] or [0097], the acronym CLSM should be defined.
In [0097], the acronyms PBS and FITC should be defined.
In [0098], it appears that the cell line name “BxPC-3yixianai” may have been translated incorrectly because this does not appear to be an established cell line name. The examiner suggests correcting the cell line name to BxPC-3, if that is the intended cell line, or describing the “BxPC-3yixianai” cell line.
Appropriate correction is required.
Claim Interpretation
In claims 1-3, the phrase “ultra-small metal-organic framework material” (line 1 of claims 1-3) is interpreted as being a metal-organic framework material with a particle size of 2-10 nm (last line of claim 1).
Claim Objections
Claims 1-3, 9 and 10 are objected to because of the following informalities:
In claim 1, the examiner suggests inserting the word “and” after the semi colon at the end of line 9.
In claims 1, 3, 9, and 10, the examiner suggests inserting a space between numerical values and units. For example, in the last line of claim 1, “10nm” should read “10 nm.”
In claim 2, the examiner suggests that the readability of the listed limitations could be improved by either inserting “and” at the end of line 2 or by changing the first comma in line 4 to a semi colon.
In claim 3, line 1, “ultra-small nano-metal organic framework” should read “an ultra-small nano metal-organic framework” to match the punctuation used in claim 1.
In claim 3, steps 1 through 4 should begin with lowercase letters instead of capital letters.
Claim 3, step 3 should read “Placing the mother liquor in a reaction kettle, and carrying out a solvothermal reaction under the protection of a reducing atmosphere…”
In the last line of claim 3, “frame material” should read “framework material.”
In claim 9, line 2, “; The” should read “; and the.”
Appropriate correction is required.
Claim Rejections - 35 USC § 112
The following is a quotation of 35 U.S.C. 112(b):
(b) CONCLUSION.—The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the inventor or a joint inventor regards as the invention.
The following is a quotation of 35 U.S.C. 112 (pre-AIA ), second paragraph:
The specification shall conclude with one or more claims particularly pointing out and distinctly claiming the subject matter which the applicant regards as his invention.
Claims 1-10 are rejected under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), second paragraph, as being indefinite for failing to particularly point out and distinctly claim the subject matter which the inventor or a joint inventor (or for applications subject to pre-AIA 35 U.S.C. 112, the applicant), regards as the invention.
Claim 1 recites the limitation "the solvent" in line 7. There is insufficient antecedent basis for this limitation in the claim because a solvent is not previously mentioned in the claim. One way to correct this issue is to include a solvent in the description in lines 3-4.
Claim 2 is rejected by virtue of dependency on claim 1.
Claim 3 recites the limitation "The preparation method… according to claim 1" in claim 3. There is insufficient antecedent basis for this limitation in the claim because claim 1 does not include a method. This can be corrected by replacing “The preparation method” with “A preparation method.”
Claim 3 contains the limitation “mixing a metal source and an organic ligand in proportion” in line 4. Claim 3 is a method of making the metal organic framework of claim 1. Claim 1 specifies a molar ratio of the metal source and the ligand, but claim 3 does not specify a molar ratio, making it unclear what is meant by the “proportion” of claim 3. The examiner recommends amending claim 3 to specify the proportion between the metal source and the ligand.
Claim 3 further contains the limitation “adding a solvent to prepare a mixed solution.” Claim 3 is a method of making the metal organic framework of claim 1. Claim 1 specifies that the solvent is prepared by mixing ethanol and o-dichlorobenzene according to a volume ratio of 1-3:1. Claim 3 does not specify the solvent, so it is unclear if the solvent of claim 3 is meant to be the same solvent as claim 1 or a different solvent. Solvent choice is known to influence the resulting metal organic framework structure, as evidenced by Schubert & Hüsing (Synthesis of Inorganic Materials (4th Edition), Chapter 6. Self-Assembly, John Wiley & Sons, 2019, 267-285). Schubert & Hüsing teach that metal organic framework syntheses are very sensitive to small variations of synthetic parameters, such as temperature, pressure, reaction time, solvent, kinds of precursors, pH or concentration of reactants (Schubert & Hüsing, page 276, paragraph 4). Schubert & Hüsing further teach that these parameters not only determine the obtained structure buy also affect crystal size and phase purity (Schubert & Hüsing, page 276, paragraph 4). For the purposes of examination, the solvent of claim 3 has been interpreted to be the 1-3:1 (v/v) mixture of ethanol and o-dichlorobenzene required by claim 1 because solvent choice is known to impact metal-organic framework structure and claim 3 is a method of making the metal organic framework of claim 1.
Claim 3 contains the limitation “the filter cake” in line 11 and “the dried product” in lines 11-12. There is insufficient antecedent basis for these limitations in the claim.
Claims 4-10 are rejected by virtue of dependency on claim 3.
Claim 6 contains the trademark/trade name “Tween 80 or tween 60.” Where a trademark or trade name is used in a claim as a limitation to identify or describe a particular material or product, the claim does not comply with the requirements of 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), second paragraph. See Ex parte Simpson, 218 USPQ 1020 (Bd. App. 1982). The claim scope is uncertain since the trademark or trade name cannot be used properly to identify any particular material or product. A trademark or trade name is used to identify a source of goods, and not the goods themselves. Thus, a trademark or trade name does not identify or describe the goods associated with the trademark or trade name. In the present case, the trademark/trade name is used to identify/describe a polysorbate non-ionic surfactant and, accordingly, the identification/description is indefinite.
Claim 10 recites the limitation "the pulverizer" in 10. There is insufficient antecedent basis for this limitation in the claim. Claim 10 depends from claim 3, but claim 3 does not claim a pulverizer. For the purposes of examination, the pulverizer is interpreted as the device that carries out ultrasonic crushing in claim 3 of step 3 (see specification [0036] where ultrasonic pulverization is carried out with a pulverizer).
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 8 is 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 8 states “the preparation method according to claim 3 is characterized in that step 4 is to dissolve the dried product in dimethyl sulfoxide or o-dichlorobenzene.” Claim 8 depends from claim 3 where step 4 comprises actions that are not included in the step 4 of claim 8. This can be corrected by amending claim 8 to clarify that the dried product of step 4 is dissolved in dimethyl sulfoxide or o-dichlorobenzene. For the purposes of examination, claim 8 is interpreted as limiting the solvent used for dissolving the dried product in step 4 of claim 3 rather than replacing all of the actions of claim 3 step 4.
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.
Allowable Subject Matter
Claims 1-10 are free of prior art.
The closest prior art is Liang (US 2017/0166661 A1) in view of Schubert & Hüsing (Synthesis of Inorganic Materials (4th Edition), Chapter 6. Self-Assembly, John Wiley & Sons, 2019, 267-285) and Huang (CN 110124034 A, English machine translation provided) and Seyedpour (US 2020/0079796 A1, Cite No. 1 on 9/29/2022 IDS) in view of Schubert & Hüsing (Synthesis of Inorganic Materials (4th Edition), Chapter 6. Self-Assembly, John Wiley & Sons, 2019, 267-285).
Liang teaches a metal-organic framework (Liang, abstract) where the metal ions are selected from a list including Fe3+ (reading on ferric ions), Cu2+ (reading on divalent copper ions), Zn2+ (reading on divalent zinc ions), and combinations thereof (Liang, [0055]) and the organic ligands are selected from a list including terephthalic acid, 2-amino-1,4-benzenedicarboxylic acid (reading on 2-aminoterephthalic acid), and 5, 10, 15, 20-tetrakis(4-carboxyphenyl)porphyrin (reading on meso-tetra(4-carboxyphenyl) porphine), and mixtures thereof (Liang, [0090]). The organic ligand to metal salt molar ratio of Liang is 5:1 to 1:5 (Liang, [0099]). The solvents that can be used to prepare the solution in which metal organic framework precursors are combined may include ethanol (Liang, [0094-0095]) and the formation temperature is lower than 100 °C (Liang, [0106]). Theses conditions read on a solvothermal reaction. Liang teaches that the largest dimension of the particles ranges from about 10 nm up to 500 µm (Liang, [0080]).
To arrive at the instant invention, one would have to select a combination of at least two of ferric ions, divalent copper ions or divalent zinc ions from all of the metal ions taught by Liang. Furthermore, one would need to select any two or three of terephthalic acid, 2-aminoterephthalic acid, and meso-tetra(4-carboxyphenyl) porphine from all of the ligands taught by Liang. One would further need to select an organic ligand to metal salt molar ratio of 1:1-5 from the range of 5:1-1:5 taught by Liang. Liang teaches a broad particle size range of 10 nm up to 500 µm. The range is very wide and only slightly overlaps claimed range of 2-10 nm.
Liang teaches a variety of solvents, including ethanol, but does not a combination of ethanol and o-dichlorobenzene with a volume ratio of 1-3:1.
Metal organic frameworks are sensitive to solvent choice, as evidenced by Schubert & Hüsing. Schubert & Hüsing teach that metal organic framework syntheses are very sensitive to small variations of synthetic parameters, such as temperature, pressure, reaction time, solvent, kinds of precursors (counter-ion of the employed metal salt, for example), pH or concentration of reactants (Schubert & Hüsing, page 276, paragraph 4). Schubert & Hüsing further teach that these parameters not only determine the obtained structure buy also affect crystal size and phase purity (Schubert & Hüsing, page 276, paragraph 4).
Based on the disclosure of Schubert & Hüsing, it is reasonable to expect that the choice of a 1-3:1 (v/v) mixture of ethanol and o-dichlorobenzene impacts the structure of the resulting metal organic framework.
Huang teaches a method of synthesizing a metal organic framework material (Huang, page 1, claim 1). Huang teaches that the ligand can be selected from terephthalic acid, 2-aminoterephthalic acid, and tetrakis (4-carboxyphenyl) porphin and that the metal ion is selected from tetravalent cerium ions, tetravalent zirconium ions, ferric ions, divalent copper ions, and divalent zinc ions (Huang, page 1, claim 3). Huang further teaches that the solvent is one or more of a list including ethanol and o-dichlorobenzene (Huang, page 1, claim 4). Based on the disclosure of Huang, it is clear that both ethanol and o-dichlorobenzene were known in the art as appropriate solvents for the preparation of metal-organic frameworks derived from the metal sources and ligands of Liang. However, because Huang does not suggest any motivation to utilize a mixture of ethanol and o-dichlorobenzene rather than the solvents taught by Liang and further does not teach a ratio between the solvents, one of ordinary skill would not have been motivated to use a 1-3:1 (v/v) mixture of ethanol and o-dichlorobenzene based on the disclosure of Liang in view of Huang.
Because one would need to select a specific combination of at least two metal ions and at least two ligands from those taught by Liang along with a ligand to metal ion ratio within the claimed range and further select the end point of particle size all while utilizing a different solvent that the claimed solvent mixture, it is unlikely that one would arrive at the metal organic framework of claim 1 based on the disclosure of Liang.
Seyedpour teaches a metal-organic framework (Seyedpour, title) prepared by the reaction of a metal source and a ligand (contacting a homogenized ligand solution with a homogenized aqueous metal salt solution… agitating the mixture for an amount of time to thereby form the nanostructured metal organic framework, Seyedpour, [0005]). Seyedpour teaches that the metal salt can comprise mixtures of iron, copper, and/or zinc (Seyedpour, [0008]). Seyedpour exemplifies zinc acetate dihydrate and copper (II) acetate hydrate as metal salts (Seyedpour, [0008]). Zinc acetate dihydrate comprises divalent zinc ions and copper (II) acetate comprises divalent copper ions. Seyedpour further teaches that the ligand can be mixtures of 2-aminoterephthalic acid and terephthalic acid (Seyedpour, [0006]). With respect to particle size, Seyedpour teaches an average particle size from 1 nanometer to 1 micrometer (Seyedpour, [0013]), overlapping with the claimed range of 2-10 nm. It would have been obvious to one of ordinary skill in the art before the effective filing date of the invention to have selected the overlapping portion of the ranges disclosed by the reference because selection of overlapping portion of ranges has been held to be a prima facie case of obviousness. See MPEP § 2144.05.I. As a solvent, Seyedpour teaches that the metal salt is dispersed in an aqueous solvent and the ligand is dispersed in a solvent that can be ethanol (Seyedpour, [0006]).
Seyedpour differs from claim 1 in that Seyedpour does not teach a metal source to ligand molar ratio of 1: 1-5 or that the solvent is a combination of ethanol and o-dichlorobenzene with a volume ratio of 1-3:1. Because Seyedpour requires the use of an aqueous solvent for dispersing the metal salt (Seyedpour, [0005]), it would not have been obvious for one to have utilized a solvent that is a combination of ethanol and o-dichlorobenzene with a volume ratio of 1-3:1.
Metal organic frameworks are sensitive to the concentration of reactants and solvent choice, as evidenced by Schubert & Hüsing. Schubert & Hüsing teach that metal organic framework syntheses are very sensitive to small variations of synthetic parameters, such as temperature, pressure, reaction time, solvent, kinds of precursors (counter-ion of the employed metal salt, for example), pH or concentration of reactants (Schubert & Hüsing, page 276, paragraph 4). Schubert & Hüsing further teach that these parameters not only determine the obtained structure buy also affect crystal size and phase purity (Schubert & Hüsing, page 276, paragraph 4).
Based on the disclosure of Schubert & Hüsing, it is reasonable to expect that the claimed metal ion to organic ligand ratio and solvent composition would impact the structure of the claimed metal-organic framework.
Given that Seyedpour teaches a different solvent the claimed solvent and solvent composition is known to impact the structure of metal-organic frameworks, it is unlikely that one would arrive at the metal organic framework of claim 1 based on the disclosure of Seyedpour. Similarly, Seyedpour does not teach the claimed metal source to ligand ratio and the concentration of reactants is known to impact the structure of metal-organic frameworks.
Claim 1 is free of prior art. Claim 2 depends from claim 1 and requires all of the limitations of claim 1 and is therefore free of art. Furthermore, claim 2 limits claim 1 by requiring specific metal salts and requiring that the organic ligand is a 3:1-5:8 mixture of terephthalic acid, meso-tetra(4-carboxyphenyl) porphine, and trimellitic acid. The examiner is not aware of a prior art disclosure of this combination of terephthalic acid, meso-tetra(4-carboxyphenyl) porphine, and trimellitic acid in a molar ratio of 3:1-5:8.
Claims 3-10 are drawn to a method of making the ultra-small nano metal-organic framework of claim 1 and are therefore also free of prior art.
The preparation method of Liang comprises mixing a metal source and an organic ligand with a suitable solvent (Liang, [0085-0086]). Liang further teaches a solution temperature lower than 100 °C (Liang, [0106]) and a reaction temperature of 30 minutes or 60 minutes (Liang, [0114]), reading on placing the mother liquor in a reaction kettle, and carrying out solvothermal reaction, wherein the reaction temperature is within the claimed range of 50-150°C, and the reaction time is within the claimed range of 0.5-1 hour. Compared to claim 3, Liang does not teach step 2, a reducing atmosphere during step 3, or step 4. Liang further does not teach the ethanol and o-dichloromethane solvent mixture required by claim 1 to achieve the desired structure.
The preparation method of Seyedpour comprises containing a ligand solution with an aqueous metal salt solution at room termpature to form a mixture (Seyedpour, [0074]). The metal salt is dispersed in an aqueous solvent and the ligand is dispersed in a solvent that can be ethanol (Seyedpour, [0006]). Seyedpour does not teach the ethanol and o-dichloromethane solvent mixture required by claim 1 to achieve the desired structure.
Seyedpour teaches that surfactant-assisted preparation allows a certain degree of control over crystal size and morphology and that surfactants can act as capping agents or inhibitors, slowing down the crystal growth rate and providing steric stabilization that allows the formation of nanoparticles (Seyedpour, [0128-0129]). Based on the disclosure of Seyedpour it would have been obvious to one or ordinary skill that increasing the amount of surfactant would slow the crystal growth rate. Therefore, it would have been obvious to one of ordinary skill in the art prior to the effective filing date of the claimed invention to have included a surfactant and optimized the surfactant concentration into the claimed range of 1-3% of the mass of the metal source. One would have been motivated to optimize the surfactant concentration in order to tune the crystallization rate. The discovery of an optimum value of a known result effective variable, without producing any new or unexpected results, is within the ambit of a person of ordinary skill in the art. See In re Boesch, 205 USPQ 215 (CCPA 1980) (see MPEP § 2144.05, II.).
The metal-organic framework is obtained by agitating for 30 minutes or less at room temperature (Seyedpour, [0086]), overlapping with the claimed reaction time. It would have been obvious to one of ordinary skill in the art before the effective filing date of the invention to have selected the overlapping portion of the ranges disclosed by the reference because selection of overlapping portion of ranges has been held to be a prima facie case of obviousness. See MPEP § 2144.05.I. Seyedpour does not teach a reducing atmosphere. Furthermore, Seyedpour does not teach a solvothermal reaction because the reaction is conducted at room temperature and the solvent is aqueous.
Seyepour further teaches collecting and drying the nanostructured metal-organic framework (Seyedpour, [0015]), but does not teach an ultrasonic crushing step following the reaction.
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to AUDRA DESTEFANO whose telephone number is (703)756-1404. The examiner can normally be reached Monday-Friday 9-5.
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/AUDRA J DESTEFANO/Examiner, Art Unit 1766
/RANDY P GULAKOWSKI/Supervisory Patent Examiner, Art Unit 1766