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 .
Response to Amendment
The examiner acknowledges Applicant’s response filed on 05/31/2025 containing remarks and amendments to the claims.
The rejection of claims 1-10 under 35 USC 112(b) is withdrawn in view of the amendment.
Response to Arguments
Applicant's arguments (see Remarks) with respect to the rejection of claims 1-10 under 35 U.S.C. 103 as being unpatentable over Claus (WO 2011/107565), in view of Asplund ("Catalyst deactivation in liquid-and gas-phase hydrogenation of acetylene using a monolithic catalyst reactor" Catalysis Today24 (1995) 181-187), have been fully considered but they are not persuasive.
On pages 6-7, Applicant argues that the disclosure of Asplund et al., which is focused on the deactivation behavior associated with using the catalyst in gaseous-phase versus liquid-phase selective hydrogenation of acetylene, provides no motivation or suggestion to modify the catalyst of Claus et al. so as to use a catalyst having a monolithic support with a CPSI of between 400 and 700, and in which the active phase is provided in the form of a layer with a thickness of between 60-90 µm on walls of the support.
In response, Claus teaches using a palladium catalyst supported in the form of a ceramic or metal monolith with an active phase (referred to as “outer shell region” characterized by the presence of at least 90 of the total amount of palladium) being provided in the form of a layer and having a maximum depth of 100 µm (pg. 9, lines 5-11 and 26-32), which renders the claimed range of “60-90 µm.” Since Claus is silent on the channel density (CPSI) of the monolith, one skilled in the art operating Claus would have been motivated to look in the prior art for a similar process that teaches an effective CPSI for carrying out the reaction. As noted in the rejection, Asplund teaches a process of selective hydrogenation of acetylene in the gas phase using a monolithic Pd/α-alumina catalyst having a cell density of about 710 CPSI (Abstract; pg. 182-183, “2. Experimental methods”; Table 1). Therefore, it would have been obvious for one skilled in the art to apply a CPSI of about 710 in the Claus process to yield predictable results. It is acknowledged that a CPSI of 710 is greater than the upper limit of the claimed range of “between 400 and 700.” However, a CPSI of 710 in Asplund is considered so close to a CPSI value of 700 (i.e., a difference of 1.4%) that one skilled in the art would have expected these CPSI values to have the same effect in the reaction. A prima facie case of obviousness exists where the claimed ranges or amounts do not overlap with the prior art but are merely close. MPEP 2144.05.
Claim Objections
Claim 19 is objected to because of the following informalities.
Claim 19 is a duplicate of claim 8. Applicant is suggested to amend or cancel claim 19.
Appropriate correction is required.
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 1-4 and 6-19 are rejected under 35 U.S.C. 103 as being unpatentable over Claus et al. (WO 2011/107565 A1, cited IDS dated 06/08/2023), in view of Asplund et al. (“Catalyst deactivation in liquid- and gas-phase hydrogenation of acetylene using a monolithic catalyst reactor” Catalysis Today 24 (1995) 181-187; cited in IDS dated 06/08/2023).
Regarding claim 1, Claus discloses a process for selective hydrogenation of a stream comprising acetylene, the process comprising performing selective hydrogenation of the stream comprising acetylene in gaseous phase under reaction conditions in the presence of a hydrogenation catalyst comprising an active phase (referred to as “outer shell region” in Claus) comprising at least one group VIII metal (palladium and platinum) and a support provided in the form of a ceramic or metal monolith (line pg. 9, lines 5-11; pg. 12, lines 6-8; pg. 25, lines 7-31).
The reaction conditions include a temperature of 10 to 250°C, a GHSV of 1000 to 15000 h-1, and a molar ratio of hydrogen/acetylene of from 0.8 to 1.8 (pg. 25, lines 26-30; pg. 26, lines 3-6 and 15-17), which fall within the claimed ranges of “between 0°C and 300°C,” “100 h-1 and 60,000 h-1,” and “between 0.5 and 1000,” respectively. The reaction conditions further include a pressure of 0.5 to 90 bars, i.e., 0.05-9 MPa (pg. 25, line 33 – pg. 26, line 1), which overlaps and renders obvious the claimed range of “between 0.1 MPa and 6.0 MPa.” In the case where the claimed ranges “overlap or lie inside ranges disclosed by the prior art” a prima facie case of obviousness exists. MPEP 2144.05. I.
Claus further teaches that the active phase (“the outer shell region”) is provided in the form of a layer which may have a maximum thickness of 100 µm, wherein an active metal, e.g., palladium, is distributed in said support layer (pg. 9, lines 16-32). The claimed range of “60 µm and 90 µm” overlaps the active phase layer range taught by Claus and is considered prima facie obvious.
Claus is silent on the number of channels per unit length (CPSI) and thus fails to teach the claimed CSPI range of between 400 and 700.
However, Asplund teaches a process of selective hydrogenation of acetylene in the gas phase, wherein the reaction is carried out in the presence of a monolithic Pd/α-alumina catalyst (Abstract; pg. 182-183, “2. Experimental methods”). Asplund discloses that the monolithic catalyst has a cell density of 110 cells/cm2 (Table 1), which is equivalent to about 709.7 cells/in2 or 709.7 channels/in2 (channels and cells are interchangeable terms in the art).
Therefore, before the effective filing date of the instant invention, it would have been obvious to one of ordinary skill in the art to modify Claus by use a monolithic catalyst having a CSPI of about 709.7, as taught by Asplund, because (i) Claus teaches a monolithic Pd catalyst but does not specify the CPSI, (ii) Asplund suggests that a CSPI of about 709 is effective for a monolithic Pd catalyst in an acetylene hydrogenation process, and (iii) this involves application of a known catalyst characteristic/property effective for a known process to yield predictable results.
It is noted that 710 cells/in2 lies outside the claimed range of between 400 and 700. However, a CPSI of 710 in Asplund is considered so close to a CPSI value of 700 (i.e., a difference of 1.4%) that one skilled in the art would have expected these CPSI values to have the same effect in the reaction. A prima facie case of obviousness exists where the claimed ranges or amounts do not overlap with the prior art but are merely close. MPEP 2144.05.
Regarding claims 2, 4, 15, 17, and 18 Claus does not teach the claimed geometric surface areas of 1500-5000 m2/m3 (claim 2) and 1500-4000 m2/m3 (claim 15) and the claimed degrees of porosity of between 20% and 90% (claim 4), between 15% and 90% (claim 17), and between 20% and 70% (claim 18). However, surface area and porosity are important parameters of catalyst that directly affect the catalytic activity as a surface area provides active sites for reaction and porosity allows reactants to reach the active sites. Therefore, it would have been obvious to one of ordinary skill in the art to optimize the geometric surface area and porosity of the catalyst and arrive at the claimed ranges of 1500-5000 m2/m3 (claim 2) and 1500-4000 m2/m3 (claim 15) and the degrees of porosity of between 20% and 90% (claim 4), between 15% and 90% (claim 17), and between 20% and 70% (claim 18), since it has been held that, where the general conditions of a claim are disclosed in the prior art, it is not inventive to discover the optimum or workable ranges by routine experimentation. MPEP 2144.05 II
Regarding claim 3, Claus does not explicit teach that the catalyst has a wall thickness (interpreted as the total depth from the surface to the center of the catalyst) of between 0.08 mm and 0.5 mm. However, Claus discloses that the radius of the catalyst center may be 2 times greater than the depth of the outer shell region (pg. 5, lines 28-31). Claus further discloses that the outer shell region may have a thickness of 100 µm (pg. 9, lines 16-32), which suggests that the catalyst may have a radius of the catalyst center of 200 µm or greater and, thus, a wall thickness of >300 µm, which overlaps and the renders obvious the claimed range of 0.08 mm and 0.5 mm (80-500 µm).
Regarding claim 6, Claus is silent on the material of the monolithic body, which corresponds to the claimed support.
However, Asplund teaches a process of selective hydrogenation of acetylene in the gas phase, wherein the reaction is carried out in the presence of a monolithic Pd/α-alumina catalyst (Abstract; pg. 182-183, “2. Experimental methods”). Asplund discloses that the monolithic catalyst comprises an α-Al2O3 monolith body (pg. 182, “2.2 The catalyst”).
Therefore, before the effective filing date of the instant invention, it would have been obvious to one of ordinary skill in the art to modify Claus by use a monolith body/support made of alumina, as taught by Asplund, because (i) Claus teaches a monolithic Pd catalyst but does not specify the material of the monolith boy, (ii) Asplund suggests that alumina is an effective material for monolithic catalysts in acetylene hydrogenation processes, and (iii) this involves application of a known catalyst material effective for a known process to yield predictable results.
Regarding claims 7 and 8, Claus teaches that the catalyst comprises palladium (pg. 8, lines 16-21).
Regarding claim 9, Claus discloses that the palladium concentration is from 0.01 to 5.0 wt% based on the total weight of the catalyst (pg. 15, lines 23-25). The claimed range of “between 0.005% and 2% by weight” overlaps the range taught by Claus and is considered prima facie obvious.
Regarding claim 10, it would have been obvious for one skilled in the art to use a monolithic catalyst having a cell density of about 710 channels/in2 in view of Asplund, as discussed above (Table 1). A CPSI of 710 is considered so close to the upper limit in the claimed range of “between 450 and 700” that one skilled in the art would have expected CPSI values of 710 and 700 to have the same effect in the reaction.
Regarding claim 11, Claus teaches a reaction temperature 10 to 250°C (pg. 25, lines 27-32), which overlaps and renders obvious the claimed range of “between 15°C and 280°C."
Regarding claim 12, Claus teaches a reaction pressure of 0.5 to 90 bars, i.e., 0.05-9 MPa (pg. 25, line 33 – pg. 26, line 1), which encompasses and renders obvious the claimed range of “between 2.0 MPa and 5.0 MPa.”
Regarding claim 13, Claus teaches a molar ratio of hydrogen/acetylene of from 0.8 to 1.8 (pg. 26, lines 15-18), which falls within the claimed range of “between 0.7 and 800.”
Regarding claim 14, Claus teaches a GHSV of 1000 to 15000 h-1 (pg. 26, lines 3-8), which falls within the claimed range of “500 h-1 and 50,000 h-1.”
Regarding claim 16, Claus does not explicit teach that the catalyst has a wall thickness (interpreted as the total depth from the surface to the center of the catalyst) of between 0.1 mm and 0.4 mm. However, Claus discloses that the radius of the catalyst center may be 2 times greater than the depth of the outer shell region (pg. 5, lines 28-31). Claus further discloses that the outer shell region may have a thickness of 100 µm (pg. 9, lines 16-32), which suggests that the catalyst may have a radius of the catalyst center of 200 µm or greater and, thus, a wall thickness of >300 µm, which overlaps and the renders obvious the claimed range of 0.1 mm and 0.4 mm (100-400 µm).
Regarding claim 19, Claus discloses that the palladium concentration is from 0.01 to 5.0 wt% based on the total weight of the catalyst (pg. 15, lines 23-25). The claimed range of “between 0.005% and 2% by weight” overlaps the range taught by Claus and is considered prima facie obvious.
Claim 20 is rejected under 35 U.S.C. 103 as being unpatentable over Claus et al. (WO 2011/107565 A1, cited IDS dated 06/08/2023), in view of Asplund et al. (“Catalyst deactivation in liquid- and gas-phase hydrogenation of acetylene using a monolithic catalyst reactor” Catalysis Today 24 (1995) 181-187; cited in IDS dated 06/08/2023), as applied to 8, and further in view of Keith et al. (US 3,489,809)
Regarding claim 20, Claus, in view of Asplund, teaches the process of claim 8, as discussed above.
Claus, in view of Asplund (“Claus/Asplund”), does not teach the active phase further comprises an element from Group IB selected from silver and copper, and the content of the element from Group 1B is between 0.01 % and 0.3% by weight with respect to the total weight of the catalyst.
However, Keith discloses a selective hydrogenation process for removing acetylene in an ethylene stream using a ceramic honeycomb-type catalyst containing palladium (col. 3, lines 29-61). Keith further teaches that the catalyst may be promoted for improved selectivity with a promoter metal such as rhodium, ruthenium, gold, silver, copper or iron, the promoter metal being present in an amount from about 0.001%-5% by weight of the palladium utilized (col. 3, lies 60-64). Keith notes that the content of palladium in the catalyst is about 0.01-10 % based on the total weight of the catalyst (col. 3, lines 68-73), which suggests that the content of promoter in the catalyst is calculated to be about 0.0000001-0.5% based on the total weight of the catalyst.
Therefore, before the effective filing date of the instant invention, it would have been obvious to one of ordinary skill in the art to modify Claus/Asplund by including silver and/or copper as promoters in an amount of about 0.0000001-0.5% based on the total weight of the catalyst, as taught by Keith, because (i) both Claus/Asplund and Keith are drawn to a selective hydrogenation for removing acetylene in an ethylene stream using a palladium-monolithic catalyst, (ii) Keith teaches that silver and copper are promoters that can be added to a palladium catalyst for improved selectivity, and (iii) this involves application of a known catalyst promoter to improve a known catalytic process to yield predictable results. It is further noted that a range of about 0.0000001-0.5 wt% Ag and/or Cu encompasses and renders obvious the claimed range of “between 0.01% and 0.3% by weight with respect to the total weight of the catalyst.”
Conclusion
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 JASON Y CHONG whose telephone number is (571)431-0694. The examiner can normally be reached Monday-Friday 9:00am-5:30pm.
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/JASON Y CHONG/Examiner, Art Unit 1772
/IN SUK C BULLOCK/Supervisory Patent Examiner, Art Unit 1772