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 06/06/2023 has been considered by the examiner.
Claim Objections
Claim1 objected to because of the following informalities:
line 3 recites “stirring them” where “them” is redundant and should be removed for clarity.
Line 6 recites “stirring them” where “them” is redundant and should be removed for clarity.
Line 9 recites “then at least drying it” where “then at least” and “it” should be removed for clarity.
Line 9 recites “rawSAPO-34” which appears to be a typo. A space should be added between raw and SAPO-34.
Steps (5) and (6) recite “the resultant” which should be removed for clarity.
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 1-20 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 “a period of time” in step (1), (2) and (5). It is unclear whether the period of time in each step is the same or different.
Claim 2 recites the limitation "the fresh catalyst" in line 1. There is insufficient antecedent basis for this limitation in the claim.
Claim 2 recites the limitation “a SAPO-34 molecular sieve”. It is unclear if this SAPO-34 molecular sieve is the same or different from SAPO-34 molecular sieve recited in claim 1 line 6-7.
For purposes of examination, claim 2 is interpreted as the waste MTO catalyst fine powder used in step (1) is a permanently deactivated waste MTO catalyst, having no characteristic diffraction peaks of SAPO-34 molecular sieve in its X-ray diffraction spectrum and before being deactivated was a SAPO-34 molecular sieve.
A broad range or limitation together with a narrow range or limitation that falls within the broad range or limitation (in the same claim) may be considered indefinite if the resulting claim does not clearly set forth the metes and bounds of the patent protection desired. See MPEP § 2173.05(c). In the present instance, claim 7 recites the broad recitation an aqueous phosphoric acid solution, and the claim also recites a 85% (w/w) aqueous phosphoric acid solution which is the narrower statement of the range/limitation. The claim(s) are considered indefinite because there is a question or doubt as to whether the feature introduced by such narrower language is (a) merely exemplary of the remainder of the claim, and therefore not required, or (b) a required feature of the claims.
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 1, 3-8, 10-19 are rejected under 35 U.S.C. 103 as being unpatentable over Yuan et al (CN 115140749 A, machine translation used for citations) in view of Di et al (CN 105126903 A, machine translation used for citations).
Yuan discloses a preparation method of a micro-mesoporous SAPO-34 molecular sieve, wherein the preparation method comprises: (1) Stirring and mixing carbon deposition species… and water (Pg. 3 par. 6-7), where the adopted carbon deposition species can be derived from waste catalysts (Pg. 3 par. 13). The carbon deposition catalyst is one or more of (waste) carbon deposition MTO catalyst, carbon deposition SAPO-34 molecular sieve (Pg. 4 par. 4 meeting limitation “A method for preparing a long-lifetime SAPO-34 catalyst from waste MTO catalyst as a raw material, comprising the steps of: (1) mixing the waste MTO catalyst fine powder with water”). The (waste) carbon deposit MTO catalyst after reaction deactivation is obtained by a reaction of preparing olefin by methanol conversion of a fresh MTO catalyst… and can be a carbon deposit-containing deactivation catalyst collected industrially (Pg. 4 par. 5). Deactivated catalysts are generally specifically defined as deactivated by carbon deposition, which is close to that of a carbon deposited catalyst (Pg. 4 par. 5).
Yuan further discloses Example 1 illustrates the preparation of a micro-mesoporous SAP0-34 molecular sieve using the methods of the present invention (Pg. 5 par. 6). 85g of deionized water, and adding a carbon deposition SAPO-34 molecular sieve… 25g, mixing well (Pg. 5 par. 7 meeting limitation “(1) mixing the waste MTO catalyst fine powder with water and stirring them for a period of time to obtain a first mixture”). Dropping phosphoric acid (P2O5 85 wt.%) 17.3g, stirred for 2h, triethylamine 43.5g was added, stirred for 2h… to give a gel mixture (Pg. 5 par. 7 meeting limitation “(2) adding phosphoric acid and an organic amine to the first mixture obtained in step (1) and stirring them for a period of time to obtain an initial gel mixture for SAPO-34 molecular sieve”). Transferring into stainless steel crystallization kettle… and crystallizing at 200 deg. C for 24 hr (Pg. 5 par. 8 meeting limitation “(3) crystallizing the initial gel mixture for SAPO-34 molecular sieve obtained in step (2)”). After cooling to room temperature, the gel was filtered, washed, dried overnight at 110 °C (Pg. 5 par. 8 meeting limitation “and then at least drying it to obtain rawSAPO-34 molecular sieve powder”), and finally calcined in a muffle furnace at 650 °C for 5h (Pg. 5 par. 8 meeting limitation “(4) calcining the raw SAPO-34 molecular sieve powder obtained in step (3) to obtain SAPO-34 molecular sieve powder”). The result is to obtain the micro-mesoporous SAP0-34 molecular sieve (Pg. 5 par. 9).
Yuan does not disclose “(5) mixing the SAPO-34 molecular sieve powder obtained in step (4) with a binder and a matrix carrier in water with stirring, and then aging the resultant by standing it for a period of time to obtain a second mixture;
and (6) molding the second mixture obtained in step (5) and then calcining the resultant to obtain the long-lifetime SAPO-34 catalyst”.
Di discloses a method for reusing fine powder from spent methanol-to-olefins (MTO) catalyst ([0002]). The method of the present invention includes the following steps ([0012]): The waste methanol-to-olefins catalyst fine powder… was calcined ([0013]). Place the calcined catalyst powder in the upper part of the crystallization kettle, and put deionized water and organic amine template agent in the lower part of the reaction kettle ([0014]). Crystallize ([0014]). (3) The crystallized fine powder is mixed with deionized water, SAPO-34 molecular sieve powder, binder and matrix to obtain a slurry ([0015] meeting limitation “(5) mixing the SAPO-34 molecular sieve powder obtained in step (4) with a binder and a matrix carrier in water”). After stirring and grinding, the slurry is aged for 6 to 36 hours, preferably 8 to 20 hours ([0015] meeting limitation “with stirring, and then aging the resultant by standing it for a period of time to obtain a second mixture”). Then, it is spray-formed and calcined at 580 to 700°C for 2 to 8 hours to prepare methanol-to-olefins catalyst microspheres ([0015] meeting limitation “and (6) molding the second mixture obtained in step (5) and then calcining the resultant to obtain the long-lifetime SAPO-34 catalyst”).
Di further discloses that mixing binder, support, and molecular sieve into a slurry and then aging it under mild conditions for a certain period of time can effectively improve the wear resistance of the molded catalyst ([0006]).
Thus, prior to the effective filing date of the claimed invention it would have been obvious to one of ordinary skill in the art to mix the SAPO-34 molecular sieve powder obtained in step (4) with a binder and a matrix carrier in water with stirring, and then aging the resultant by standing it for a period of time to obtain a second mixture; and molding the second mixture obtained in step (5) and then calcining the resultant to obtain the long-lifetime SAPO-34 catalyst in the method of Yuan in order to improve the wear resistance of the molded catalyst as taught by Di.
Regarding claim 3, Yuan in view of Di discloses all the limitations in the claims as set forth above including Yuan discloses 85g of deionized water, and adding a carbon deposition SAPO-34 molecular sieve… 25g, mixing well (Pg. 5 par. 7). Dropping phosphoric acid (P2O5 85 wt.%) 17.3g, stirred for 2h, triethylamine 43.5g was added, stirred for 2h… to give a gel mixture (Pg. 5 par. 7). While Yuan does not explicitly disclose stirring the waste MTO catalyst and water for 2 to 6 hours, it is well known in the art to conduct stirring until the mixture is properly mixed and that duration of stirring affects the uniformity of the mixture. Since Yuan discloses stirring the phosphoric acid and triethylamine for 2 hours, it would be obvious to one having ordinary skill in the art to stir the deionized water and carbon deposition SAPO-34 molecular sieve for 2 hours in order to insure proper mixing and uniformity of the mixture.
Regarding claim 4, Yuan in view of Di discloses all the limitations in the claims as set forth above and further discloses in Example 2 deionized water 69g, and adding a carbon deposition MTO catalyst … 8g, mixing (Pg. 5 par. 10). The disclosed masses are equivalent to a mass ratio of 1: 8.6 which is within the claimed range of 1:(5-50).
Regarding claim 5, Yuan in view of Di discloses all the limitations in the claims as set forth above and further discloses dropping phosphoric acid (P2O5 85 wt.%) 17.3g, stirred for 2h, triethylamine 43.5g was added, stirred for 2h… to give a gel mixture (Pg. 5 par. 7). The disclosed 2h is within the claimed range of 2 to 4 hours.
Regarding claim 6, Yuan in view of Di discloses all the limitations in the claims as set forth above and further discloses dropping phosphoric acid (P2O5 85 wt.%) 17.3g, stirred for 2h, triethylamine 43.5g was added, stirred for 2h… to give a gel mixture (Pg. 5 par. 7 meeting limitation “the organic amine comprises one or more of … triethylamine”).
Regarding claim 7, Yuan in view of Di discloses all the limitations in the claims as set forth above and further discloses dropping phosphoric acid (P2O5 85 wt.%) 17.3g, stirred for 2h, triethylamine 43.5g was added, stirred for 2h… to give a gel mixture (Pg. 5 par. 7 meeting limitation “the phosphoric acid is in a form of an 85% (w/w) aqueous phosphoric acid solution”).
Regarding claim 8, Yuan in view of Di discloses all the limitations in the claims as set forth above including 85g of deionized water, and adding a carbon deposition SAPO-34 molecular sieve… 25g, mixing well (Pg. 5 par. 7 meeting limitation “(1) mixing the waste MTO catalyst fine powder with water and stirring them for a period of time to obtain a first mixture”). Dropping phosphoric acid (P2O5 85 wt.%) 17.3g, stirred for 2h, triethylamine 43.5g was added, stirred for 2h… to give a gel mixture (Pg. 5 par. 7). The disclosure of 25g of carbon deposition SAPO-34 molecular sieve, 17.3g phosphoric acid and 43.5g triethylamine is equivalent to a ratio of 1: 0.7:1.74 which is within the claimed range of 1:(0.2-1.5):(0.3-2.2).
Regarding claim 10, Yuan in view of Di discloses all the limitations in the claims as set forth above including transferring into stainless steel crystallization kettle… and crystallizing at 200 deg. C for 24 hr (Pg. 5 par. 8). 200 °C is within the claimed range of 160 to 220 °C and 24 hr is within the claimed range of 5 to 48 hours.
Regarding claim 11, Yuan in view of Di discloses all the limitations in the claims as set forth above including after cooling to room temperature, the gel was filtered, washed, dried overnight at 110 °C (Pg. 5 par. 8). 110 °C is within the claimed range of 100 to 120°C. The disclosure of dried overnight is reasonably interpreted as within the claimed time period of 4 to 12 hours.
Regarding claim 12, Yuan in view of Di discloses all the limitations in the claims as set forth above and further discloses the temperature of the calcination is 550 to 700 °C (claim 8). Calcined in a muffle furnace…for 5h (Pg. 5 par. 8). The disclosed 5h is within the claimed range of a time period of 4 to 10 hours.
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 Yuan (550 to 700 °C) overlaps with the claimed range (500 to 600°C). Therefore, the range in Yuan renders obvious the claimed range.
Regarding claim 13, Yuan in view of Di discloses all the limitations in the claims as set forth above and Di further discloses the slurry is aged for… preferably 8 to 20 hours ([0015].
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 Di (8 to 20 hours) overlaps with the claimed range (4 to 12 hours). Therefore, the range in Di renders obvious the claimed range.
Regarding claim 14, Yuan in view of Di discloses all the limitations in the claims as set forth above and Di further discloses the binder mentioned in step (3) above is aluminum sol or silica sol ([0019]).
Regarding claim 15, Yuan in view of Di discloses all the limitations in the claims as set forth above and Di further discloses the matrix mentioned in step (3) above is… preferably kaolin ([0020]).
Regarding claim 16, Yuan in view of Di discloses all the limitations in the claims as set forth above and Di further discloses 20g of SAPO-34 molecular sieve, 25g of aluminum sol (Al 2 O 3 mass fraction of 21%) and 23g of kaolin were added in sequence ([0031]). The disclosed masses are equivalent to a mass ratio of 1:1.25:1.15 which is within the claimed range of mass ratios of 1:(0.1-1.25):(0.2-10).
Regarding claim 17, Yuan in view of Di discloses all the limitations in the claims as set forth above and Di further discloses the separated solid was dispersed in 75g of deionized water, and 20g of SAPO-34 molecular sieve ([0031]). The disclosed masses are equivalent to a mass ratio of 1:3.75 which is within the claimed range of 1 :(1-10).
Regarding claim 18, Yuan in view of Di discloses all the limitations in the claims as set forth above and Di further discloses the spray drying described in step (3) above uses a centrifugal spray drying device with an inlet temperature of 350-550°C and an outlet temperature of 110-190°C ([0022]). The outlet temperature disclosed by Di is within the claimed range of outlet temperature of 80 to 200°C.
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 Di (inlet temperature of 350-550°C) overlaps with the claimed range (inlet temperature of 250 to 350°C). Therefore, the range in Di renders obvious the claimed range.
Regarding claim 18, Yuan in view of Di discloses all the limitations in the claims as set forth above and Di further discloses it is spray-formed and calcined at 580 to 700°C for 2 to 8 hours to prepare methanol-to-olefins catalyst microspheres ([0015]). The disclosed temperature of 580 to 700°C is within the claimed temperature of 500 to 700°C.
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 Di (2 to 8 hours) overlaps with the claimed range (4 to 8 hours). Therefore, the range in Di renders obvious the claimed range.
Claim 2 is rejected under 35 U.S.C. 103 as being unpatentable over Yuan et al (CN 115140749 A, machine translation used for citations) in view of Di et al (CN 105126903 A, machine translation used for citations) and in further view of Wragg et al (“SAPO-34 methanol-to-olefin catalysts under working conditions: A combined in situ powder X-ray diffraction, mass spectrometry and Raman study”).
Regarding claim 2, Yuan in view of Di discloses all the limitations in the claims as set forth above including Yuan discloses the carbon deposition catalyst is one or more of (waste) carbon deposition MTO catalyst, carbon deposition SAPO-34 molecular sieve (Pg. 4 par. 4 meeting limitation “wherein the fresh catalyst corresponding to the waste MTO catalyst fine powder used in step (1) is a SAPO-34 molecular sieve”). The (waste) carbon deposit MTO catalyst after reaction deactivation is obtained by a reaction of preparing olefin by methanol conversion of a fresh MTO catalyst… and can be a carbon deposit-containing deactivation catalyst collected industrially (Pg. 4 par. 5). Deactivated catalysts are generally specifically defined as deactivated by carbon deposition, which is close to that of a carbon deposited catalyst (Pg. 4 par. 5 meeting limitation “and the waste MTO catalyst fine powder used in step (1) is a permanently deactivated waste MTO catalyst”).
Yuan does not explicitly disclose “having no characteristic diffraction peaks of SAPO-34 molecular sieve in its X-ray diffraction spectrum”.
Wragg discloses we have studied the behavior of the zeotype silicoaluminophosphate SAPO-34 catalyst in the methanol-to-olefin (MTO) process under real working conditions using simultaneous synchrotron powder X-ray diffraction (PXRD) (abstract). When the MTO process is run at 440 °C changes in both the intensity and position of the PXRD peaks are observed (Pg. 291 Section 3.1). This suggests … that the reaction causes greater strain in the cages than adsorbed aromatics (Pg. 291 Section 3.1). The results suggest a strong link between intermediate formation within the cages and expansion of the SAPO-34 unit cell (especially in the c-axis direction) (Pg. 295 Conclusion). Both XRD and Raman show that aromatic coke appears very rapidly and has an immediate effect on the catalyst structure (Pg. 295 Conclusion). The development of the FWHM of the (101) peak indicates that the formation of coke induces strain in the lattice of SAPO-34 (Pg. 295 Conclusion).
Since Wragg discloses the formation of coke induces strain in the lattice of SAPO-34, and the MTO process changes the intensity and position of the PXRD peaks of the SAPO-34 catalyst, it is reasonable to conclude that Yuan discloses the waste MTO catalyst used in step (1) has no characteristic diffraction peaks of SAPO-34 molecular sieve in its X-ray diffraction spectrum, since Yuan discloses the (waste) carbon deposit MTO catalyst after reaction deactivation is obtained by a reaction of preparing olefin by methanol conversion of a fresh MTO catalyst… and can be a carbon deposit-containing deactivation catalyst collected industrially (Pg. 4 par. 5).
The Patent and Trademark Office can require Applicant to prove that prior art products do not necessarily or inherently possess characteristics of claimed products where claimed and prior art products are identical or substantially identical, or are produced by identical or substantially identical processes; burden of proof is on Applicants where rejection based on inherency under 35 U.S.C. § 102 or on prima facie obviousness under 35 U.S.C. § 103, jointly or alternatively, and Patent and Trademark Office’s inability to manufacture products or to obtain and compare prior art products evidences fairness of this rejection, In re Best, Bolton, and Shaw, 195 U.S.P.Q. 431 (CCPA 1977).
Claim 9 is rejected under 35 U.S.C. 103 as being unpatentable over Yuan et al (CN 115140749 A, machine translation used for citations) in view of Di et al (CN 105126903 A, machine translation used for citations) and in further view of Ding (CN 117185308 A, machine translation used for citations).
Regarding claim 9, Yuan in view of Di discloses all the limitations in the claims as set forth above but does not disclose “wherein the initial gel mixture for SAPO-34 molecular sieve obtained in step (2) has a pH of 5 to 10”.
Ding discloses a method for preparing SAPO-34 molecular sieve, comprising ([0007]): (2) Aluminum source, phosphorous source, water, and selectively added silicon source and selectively added template agent are mixed to prepare gel II ([0009]); (3) The directing agent prepared in step (1) is mixed with the gel II prepared in step (2), the pH is adjusted, and hydrothermal crystallization is carried out to prepare SAPO-34 molecular sieve ([0010]). Further, the method for preparing the directing agent in step (1) includes: preparing an initial gel I by combining the in-service MTO catalyst with … water ([0011]). Step 3 disclosed by Ding is interpreted as reading on claim 1 step 2 where the disclosed gel II contains phosphoric acid (phosphorous source) and organic amine (template agent triethylamine as disclosed in [0014]). The disclosed directing agent reads on the claimed first mixture obtained in step (1). Ding discloses adjusting the pH after the directing agent is mixed with the gel II. in step (3), the pH is adjusted to 6-11 ([0019]).
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 Ding (6-11) overlaps with the claimed range (5-10). Therefore, the range in Ding renders obvious the claimed range.
Ding further discloses the prepared molecular sieves have smaller particle size and more uniform distribution, and when applied to methanol-to-olefins reaction, they exhibit high diene yield ([0027]).
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 initial gel mixture for SAPO-34 molecular sieve obtained in step (2) to have a pH of 5 to 10 in the method of Yuan in view of Di in order for the prepared molecular sieve to have smaller particle size and more uniform distribution, and when applied to methanol-to-olefins reaction, they exhibit high diene yield as taught by Ding.
Claim 20 is rejected under 35 U.S.C. 102(a)(1) as anticipated by or, in the alternative, under 35 U.S.C. 103 as obvious over Yuan et al (CN 115140749 A, machine translation used for citations).
Regarding claim 20, Yuan discloses a preparation method of a micro-mesoporous SAPO-34 molecular sieve prepared from waste MTO catalyst as a raw material meeting the limitations of claim 1 as discussed above.
If the structure of the SAPO-34 molecular sieve of Yuan is different from the claimed long-lifetime SAPO-34 catalyst prepared from waste MTO catalyst as a raw material by the method according to claim 1, it would have been obvious to one of ordinary skill in the art that the micro-mesoporous SAPO-34 of Yuan meet the claim limitations since they are both prepared from waste MTO catalyst as a raw material.
Conclusion
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/N.L.Q./Examiner, Art Unit 1738
/MICHAEL FORREST/Primary Examiner, Art Unit 1738