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 .
Claim Rejections - 35 USC § 102
The following is a quotation of the appropriate paragraphs of 35 U.S.C. 102 that form the basis for the rejections under this section made in this Office action:
A person shall be entitled to a patent unless –
(a)(1) the claimed invention was patented, described in a printed publication, or in public use, on sale, or otherwise available to the public before the effective filing date of the claimed invention.
(a)(2) the claimed invention was described in a patent issued under section 151, or in an application for patent published or deemed published under section 122(b), in which the patent or application, as the case may be, names another inventor and was effectively filed before the effective filing date of the claimed invention.
Claims 1, 6, 12, 16-18, 21 and 25 are rejected under 35 U.S.C. 102(a)(1) as being anticipated by Cao (CN106379913A). In regards to claim 1, Cao teaches a production method of a porous material including Si and Al [0025] By producing a first Si source composition from a plant-derived raw material by recovering the Si source from a treatment of the plant-derived raw material after a carbonization treatment with an alkali extraction [0025] And using at least the Si source and an Al source as a raw material to produce a porous material [0002], [0025], where the porous material is the P-type zeolite molecular sieve.
In regards to the mole ratio of the alkali extraction being carried out on a carbonized plant-derived raw material in a mole ratio of at least 0.5:1, Cao teaches that the carbonized material, a rice husk ash, is in a weight ratio with sodium hydroxide of 1:1.7-2.8 [0017]. Converting to the molar ratio for NaOH (39.997g) and rice husk ash being 99% purity of silicon dioxide [0006] with Si being 28.0855g of it, the following was converted using the weight ratio to the molar weight ratio:
1g Si / 28.0855 g/mole = 0.03560 mole SiO2
-1.7g NaOH / 39.997g = 0.0425 mole NaOH | 2.8g NaOH / 39.997g = 0.07 mole NaOH
0.0425-0.07 mole NaOH : 0.03560 mole SiO2 [Wingdings font/0xE0] 1:19:1 – 1.96:1 mole ratio NaOH:Si
As such, Cao teaches that the NaOH and Si mole ratio is at least 0.5:1 during the alkali extraction.
In regards to the extraction efficiency of 80%, as the claim states that the extraction is carried out at a mole ratio of at least 0.5:1 to produce a Si extraction efficiency of 80% or greater, as Cao teaches the necessary mole ratio recited by the claim, the alkali extraction would be done at an efficiency of 80% or greater as recited. MPEP 2112 (implicit disclosure).
In regards to claim 6, Cao teaches a Si/Al composition ratio where the Si source composition to the Al source composition is 1:1 to 300:1 [0013]. Cao teaches that the molar ratio for Al in regards to Si is 1:2.6, which is also a molar ratio of 2.6:1.
In regards to claim 12, Cao teaches a heating treatment of a mixture of a first Si source and an Al source [0036].
In regards to claim 16-18, Cao teaches that the first Si source composition is an aqueous solution removing silica from a plant-derived raw material [0028], [0030],
Where the porous material produced is a zeolite [0002],
And the plant-derived raw material is a gramineous plant, such as rice husk [0002].
In regards to claims 21 and 25, the mole ratio of the alkali extraction being carried out on a carbonized plant-derived raw material in a mole ratio of at least 0.5:1, Cao teaches that the carbonized material, a rice husk ash, is in a weight ratio with sodium hydroxide of 1:1.7-2.8 [0017]. Converting to the molar ratio for NaOH (39.997g) and rice husk ash being 99% purity of silicon dioxide [0006] with Si being 28.0855g of it, the following was converted using the weight ratio to the molar weight ratio:
1g Si / 28.0855 g/mole = 0.03560 mole SiO2
-1.7g NaOH / 39.997g = 0.0425 mole NaOH | 2.8g NaOH / 39.997g = 0.07 mole NaOH
0.0425-0.07 mole NaOH : 0.03560 mole SiO2 [Wingdings font/0xE0] 1:19:1 – 1.96:1 mole ratio NaOH:Si
As such, Cao teaches that the NaOH and Si mole ratio is at least 0.5:1 during the alkali extraction.
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.
Claims 1, 5, 6, 12, 14, 16-18, 21, 24, and 26-27 are rejected under 35 U.S.C. 103 as being unpatentable over Okuya (JP2010208872A) in view of Cao (CN106379913A). In regards to claim 1, Okuya (JP2010208872A) teaches a production method for a porous material including Si and Al, where the first Si source composition is a plant-derived source and an Al source [0016]. The rice husk is carbonized and then used as a raw material to produce the porous material [0028], [0032].
Okuya does not teach that the plant derived material is subjected to alkali extraction before contact with the aluminum source. However, Cao teaches a method of producing zeolites using rice husks as raw material [0008]. Cao also teaches that the NaOH/Si ratio within the reaction is 1.19:1-1.96:1 as calculated above. Cao teaches that by using an alkaline solution in a mixture, the final product zeolite produced has high crystallinity and high whiteness [0025]. Cao’s method of reacting an alkaline solution with the rice husks is considered to read on the alkali extraction in the claimed method, since it is the same as that disclosed in the instant spec in terms of contacting NaOH with the Si source. It is known in the art to separate the steps of adding an alkaline and Al product to a biogenic silica source as shown by Cao [0012-0013]. It is also known in the art as taught by Cao that NaOH can be added prior to the addition of an Al source [0030]. While Okuya teaches the addition of both NaOH and an Al source with the rice husk ash [0036-0037], it would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to substitute Cao’s order of process steps for adding an alkali product prior to the Al source [0012-0013] into the process taught by Okuya to predictably produce a porous material, such as a zeolite, from rice husk ash. See MPEP 2413.02.I. Cao also teaches that the extraction efficiency of Si is 80% or greater [0006].
In regards to claim 5, Okuya defines that the first Si source composition has a silicon content of 10 g/L or more in regards to the mass of the husk [0025].
In regards to claim 6, Okuya teaches that the Si/Al composition ratio can be from 1:1 to 300:1 [0014].
In regards to claim 12, Okuya teaches a heating treatment of the first Si source composition that is plant-derived and the Al source [0014].
In regards to claim 14, Okuya teaches a production method for a porous material, where the heating treatment of the mixture is hydrothermal synthesis [0014].
In regards to claim 16, Okuya teaches that the first Si source composition is an aqueous solution removing silica from a plant-derived raw material containing the silica [0030].
In regards to claim 17, Okuya teaches porous material is a zeolite [0017].
In regards to claim 18, Okuya teaches that the plant in the production of a porous material is a gramineous plant, as rice would be considered a gramineous plant [0024].
In regards to claim 21, Okuya does not explicitly teach a production method where the NaOH/Si mole ratio is 0.5:1 to 2:1.
Cao teaches a production method where the NaOH/Si mole ratio is 0.5:1 to 2:1 [0017]. See also the discussion vis-à-vis claim 1, above.
In regards to claim 24, Okuya teaches a Si/Al composition ratio from 5:1 to 20:1 [0031], where a 1:0.1-0.2 ratio for Si:Al is a 5:1 ratio. This presents an overlapping range with the instant claim and overlapping ranges are prima facie obviousness. See MPEP 2144.05.
In regards to claims 26 and 27, Okuya teaches that the porous material produced is a zeolite that has the structure of an LTA zeolite [0044].
Claims 2, 7, 10, and 13 are rejected under 35 U.S.C. 103 as being unpatentable over Okuya (JP2010208872A) in view of Cao (CN106379913A) and further in view of Wang (US20120093715A1). In regards to claim 2, Okuya and Cao does not teach a second Si source composition that is further used as a raw material.
Wang teaches that a second silicon source can be used to form a zeolite [0017]. It would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to use a second Si source as taught by Wang in the method taught by Okuya to adjust the Si/Al molar ratio to create the specific type of zeolite needed, as is discussed by Okuya [0031].
In regards to claim 7, Okuya and Cao do not teach that the second Si source is mineral or plant derived.
Wang teaches that the second Si source can be plant or mineral derived [0017]. It would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to use the plant or mineral derived second Si source as taught by Wang in the method taught by Okuya to adjust the Si/Al molar ratio to create the specific type of zeolite needed, as is discussed by Okuya [0031].
In regards to claim 10, Okuya and Cao do not teach that the second Si source is a Si source recovered from a carbonized plant-derived raw material.
Wang teaches that a second silicon source can be used to form a zeolite, where the source can be plant-derived [0017]. It would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to use a well-known carbonized Si source (rice husk carbide) as taught by Okuya as the second Si source taught by Wang in the method taught by Okuya to adjust the Si/Al molar ratio to create the specific type of zeolite needed, as is discussed by Okuya [0031].
In regards to claim 13, Okuya and Cao do not teach that a second Si source composition is in the mixture.
Wang teaches that a second silicon source can be used to form a zeolite, where the silicon source can be solid or liquid [0017]. It would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to use a second Si source in the mixture as taught by Wang in the method taught by Okuya to adjust the Si/Al molar ratio to create the specific type of zeolite needed, as is discussed by Okuya [0031].
Claim 11 is rejected under 35 U.S.C. 103 as being unpatentable over Okuya (JP2010208872A) in view of Cao (CN106379913A) and further in view of Bonilla (“Zeolite (MFI) Crystal Morphology Control Using Organic Structure-Directing Agents”, Chem. Mater., 2004, Volume 16, Pages 5697-5705). Regarding claim 11, Okuya and Cao do not teach or suggest using an organic structure directing agent in the formation of a porous material.
Bonilla (“Zeolite (MFI) Crystal Morphology Control Using Organic Structure-Directing Agents”, Chem. Mater., 2004, Volume 16, Pages 5697-5705) teaches using an organic structure directing agent to manipulate the crystal structure of a microporous aluminosilicate zeolite (Introduction, “Here, we focus on the use of structure-directing agents (SDAs), not to guide the formation of a certain zeolite crystal structure,13-15 but to systematically manipulate the zeolite crystal shape”). It would have been obvious to a person of ordinary skill in the art before the effective filing date of the claimed invention to use an organic structure directing agent with the method taught by Okuya in order to control particle size and shape for catalysis, adsorption, growth of zeolite membranes, synthesis of polymer-zeolite composites, or building blocks for hierarchal porous crystalline structures (Introduction, “The ability to control the particle size and shape of a given zeolite structure is desirable not only for applications in catalysis and adsorption,1,2 but also for a variety of uses of these zeolite particles as seeds for the growth of zeolite membranes,3-6 for synthesis of polymer-zeolite composites,7,8 or as building blocks for the construction of hierarchical porous crystalline structures”).
Claim 15 is rejected under 35 U.S.C. 103 as being unpatentable over Okuya (JP2010208872A) in view of Cao (CN106379913A) and further in view of Liu (“Aluminosilicate mesostructures with improved acidity and hydrothermal stability” J. Mater. Chem., 2002, Volume 12, pages 3179-3190) in view of Guth (“Synthesis of Aluminosilicate Zeolites and Related Silica-Based Materials”, Catalysis and Zeolites, Spring, 1999, Edition 1, Page 26). In regards to claim 15, Okuya and Cao do not teach or suggest that ageing is done before the hydrothermal step in the production method of a porous material.
Liu teaches an ageing step prior to a hydrothermal treatment to form steam-stable hexagonal mesoporous aluminosilicates (4.1 “The first steam-stable hexagonal mesoporous aluminosilicates were successfully assembled from faujasitic-type Y zeolite seeds. Nanoclustered zeolite Y seeds were prepared by reacting sodium hydroxide, sodium aluminate, and sodium silicate under vigorous stirring at 100 °C overnight”; “The steam-stable mesoporous aluminosilicate (denoted MSU-S) was obtained by exchanging the as-synthesized structure with NH4aNQ3 and then calcining at 540 °C for 7 h. Fig. 11 shows the XRD patterns of calcined 10%AI-MSU-S before and after exposure to 20% (v/v) water vapor in N> at 800 °C for 5 h”). It would have been obvious to a person of ordinary skill in the art prior to the effective filing date of the claimed date of the invention to have an ageing step prior to the hydrothermal synthesis taught by Okuya in order to produce a more metastable zeolite Y when the mixture is heated, as evidenced by Guth (1.4.1.4, “It is sometimes necessary to ‘age’ the reaction mixture during a given time at a temperature below the crystallization temperature and generally near room temperature. During this period a chemical and structural reorganization occurs which affects both the solid and the liquid phases. For instance, with the same reaction mixture, depending on whether an aging period is applied or not, zeolite Y or zeolite P will be produced. It can be assumed that during the aging, the supersaturation in the solution rises enough to allow the crystallization of the more metastable zeolite Y when the mixture is heated”).
Claim Objection/Potentially Allowable Subject Matter
Claim 28 is objected to as being dependent upon a rejected base claim, but would be allowable if rewritten in independent form including all of the limitations of the base claim and any intervening claims. Cao (CN106379913A) and Okuya (JP2010208872A) are considered to be the closest prior art to the claimed invention. Neither Cao or Okuya teach that the alkali extraction is carried out at 60°C to 110°C for 18 to 30 hours. Instead, Cao teaches an alkali extraction that is performed at 180-230°C for 2-4 hours.
Response to Arguments
Applicant’s 6/18/26 arguments, see page 6 of Remarks, as to the rejection of claim 1 under 35 USC 112(b) have been fully considered and are persuasive due to amendments. The rejection of claims 1-2, 5-7, 10-18, and 21-24 under 35 USC 112(b) has been withdrawn.
Applicant's 6/18/26 arguments have been fully considered but they are not persuasive. On pages 6-7, applicant states that the alkali extraction is carried out at a NaOH/Si mole ratio of at least 0.5:1. Converting the weight ratio taught by Cao as shown above, a molar ratio of 1:19:1 – 1.96:1 NaOH:Si is taught. As the molar ratio taught by Cao is within the range as recited in claim 1 of the instant application, the extraction efficiency of 80% or greater is also implicitly achieved. In the 3/27/26 Non-Final Rejection, the molar ratio was inadvertently expressed is different units as the weight ratio. However, as calculated above, the molar ratio range recited from claim 1 is still fulfilled by the same disclosures of Cao and is not a new ground of rejection.
Conclusion
Any inquiry concerning this communication or earlier communications from the examiner should be directed to JAANZEB RAJA whose telephone number is (703)756-4531. The examiner can normally be reached M - F 8:30-6. Examiner interviews are available via telephone, in-person, and video conferencing using a USPTO supplied web-based collaboration tool. To schedule an interview, applicant is encouraged to use the USPTO Automated Interview Request (AIR) at http://www.uspto.gov/interviewpractice. If attempts to reach the examiner by telephone are unsuccessful, the examiner’s supervisor, Anthony Zimmer can be reached at 571-270-3591. The fax phone number for the organization where this application or proceeding is assigned is 571-273-8300. Information regarding the status of published or unpublished applications may be obtained from Patent Center. Unpublished application information in Patent Center is available to registered users. To file and manage patent submissions in Patent Center, see https://patentcenter.uspto.gov. See https://www.uspto.gov/patents/apply/patent-center for more information about Patent Center and https://www.uspto.gov/patents/docx for information about filing in DOCX format. For additional questions, contact the Electronic Business Center (EBC) at 866-217-9197 (toll-free). If you would like assistance from a USPTO Customer Service Representative, call 800-786-9199 (IN USA OR CANADA) or 571-272-1000.
/JAANZEB C RAJA/ Examiner, Art Unit 1736 /DANIEL BERNS/Primary Examiner, Art Unit 1736
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