DETAILED ACTION
Terminal Disclaimer
The terminal disclaimer filed on 5/28/26 disclaiming the terminal portion of any patent granted on this application which would extend beyond the expiration date of 18/457,216 has been reviewed and is accepted. The terminal disclaimer has been recorded.
Second Non-Final
An updated search revealed new prior art pertinent to the instant claims. Therefore, the indication of allowable subject matter in the last office action dated 3/10/26 is withdrawn and a second non-final follows.
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 3 and 4 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 3 recites the limitation “from each of said three radial flow reactors” in lines 1 and 2. There is insufficient antecedent basis for this limitation in the claim. It appears claim 3 should depend on claim 2, where ‘three radial reactors’ were first recited, instead of claim 1.
Claim 4 recites “said three radial flow reactors” lacking antecedent basis. Claim 4 should also depend on claim 2 instead of claim 1.
Claims 5-9 are rejected under 112 2nd paragraph by virtue of their dependency on claim 4.
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.
Claims 1 are rejected under 35 U.S.C. 102(a)(1) as being anticipated by Coupard US Patent 9,085,502.
Regarding claim 1, Coupard teaches a dehydration process of ethanol to ethylene comprising feeding the ethanol to a radial reactor under dehydration to produce ethylene (column 9 lines 4-5 and line 12). The feed stream in line 6 contains ethanol and vaporized water (steam)(column 11 lines 14-16 and line 34) and is in a gas phase when it enters the reactor (column 11 lines 35-40).
Claim Rejections - 35 USC § 103
In the event the determination of the status of the application as subject to AIA 35 U.S.C. 102 and 103 (or as subject to pre-AIA 35 U.S.C. 102 and 103) is incorrect, any correction of the statutory basis (i.e., changing from AIA to pre-AIA ) for the rejection will not be considered a new ground of rejection if the prior art relied upon, and the rationale supporting the rejection, would be the same under either status.
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 2 and 3 are rejected under 35 U.S.C. 103 as being unpatentable over Coupard US Patent 9,085,502 in view of Schulz et al. US Patent 6,224,838.
Regarding claims 2 and 3, Coupard teaches two serial radial reactors R1 and R2 with a heater H1 and H2 are placed upstream of each of the reactors (column 11 line 47 and line 53).
Coupard does not teach three serial reactors and a third heater upstream of the third reactor.
However, Schulz teaches an arrangement of at least three serial reactors in Figure 4 with a heater upstream of each reactor. The serial arrangement of three reactors with intermittent heating allows more reaction conditions control for high temperature conversion reactions. The arrangement also allows intermittent withdrawal of spent catalyst and reintroduction of fresh/regenerated catalyst, thereby reducing unwanted byproducts and increasing ethylene selectivity (column 8 lines 40-48). The heater upstream allows extra temperature control for the reaction.
Thus, in light of Schulz, one having ordinary skill in the art at the time of filing would find it obvious to add a third reactor and third heater in the process of Coupard to allow the benefits of reducing byproducts, increasing selectivity, and better reaction conditions control.
Claims 4-15 are rejected under 35 U.S.C. 103 as being unpatentable over Coupard US Patent 9,085,502 in view of Schulz et al. US Patent 6,224,838 and in further view of Taheri et. al. US2013/0178674.
Regarding claims 4 and 5, Coupard and Schulz in combination do not explicitly teach wherein a mixture comprising said ethanol feed stream and said steam is divided into two portions of said mixture, wherein a first portion of said mixture is sent to a first of said three radial flow reactors and a second portion of said mixture is sent to a second of said three radial flow reactors an effluent from said second of said three radial flow reactors is sent to a third of said three radial flow reactors.
However, Taheri teaches a reactor process train for the dehydration of ethanol to ethylene where the feed stream 1 is split into three portions 3, 8, and 13 which are each sent to the first reaction stage, the second reaction stage, and the third reaction stage (Figure 1) thus supplying fresh ethanol feed to each reactor. Ethanol is highly endothermic and feeding all the ethanol together can expose it to excessive heated surfaces and cause decomposition, coke and unwanted byproducts. Staged ethanol feeding allows the ethanol and heat-carrying steam to be independently controlled for each reactor stage. Dividing the feed optimizes the residence time and temperature profile of each catalyst bed. Thus, these advantages promote complete conversion of ethanol to ethylene while reducing dimethyl ether, aldehydes, and higher hydrocarbons ([0037], [0038], and [0039]).
Thus, one having ordinary skill in the art at the time of filing would be motivated to modify Coupard and Schulz by dividing the feed into three portions and sending each portion to each of the three reactors in order to benefit from complete conversion of ethanol to ethylene while reducing dimethyl ether, aldehydes, and higher hydrocarbons.
Regarding claim 6, the temperature of the first stage reaction in Coupard is from 350 ⁰C to 500 ⁰C (column 2 line 55).
Regarding claim 7, Coupard teaches the ratio of diluent (steam) to feedstock ratio is 2.5 (column 12 lines 36-40). The feedstock contains about 91.9 wt% ethanol (Table 1), so the ratio of steam to ethanol in the feed is within the range of 1:1 to 2.5:1.
Regarding claim 8, Taheri teaches a first stage inlet at 400-500 ⁰C and an outlet at 300-480 ⁰C ([0025]), thus teaches an endotherm (difference of the inlet and outlet temperatures) of about 150 ⁰C. The second stage inlet is at 380-530 ⁰C and outlet at 300-460 ⁰C ([0026]), thus comprises an endotherm of about 120 ⁰C. The third stage reactor comprise an inlet temperature of 370-520 ⁰C and an outlet temperature of 290-420 ⁰C (0027]), thus comprises an endotherm of about 25 ⁰C.
Taheri teaches that temperature decreases through each catalyst bed and the temperature profile is critical to conversion and ethylene selectivity ([0032], [0036], [0038]). It would have been obvious to optimize the inlet and outlet temperatures within Taheri’s disclosed ranges, thereby producing the claimed temperature drops across the three reactors.
Regarding claim 9, Taheri teaches the pressure across the reactor beds is 2 barg to 50 barg ([0024]) which is equivalent to 200 to 5000 kpa(g). In Table 1, the first stage is at 6.45 barg and second stage is at 5.95 barg, thus teaches a decreasing pressure across the reactors.
It would have been obvious to one having ordinary skill in the art to use Taheri’s decreasing pressures in the radial reactor system of Coupard, because the reactor configuration would not substantially change the pressure requirements of an ethanol dehydration reaction. One having ordinary skill in the art would expect that pressure would naturally decrease as the stream passes through successive catalyst beds and equipment resulting in the first reactor having a higher pressure than the third.
Regarding claims 10, 11, 12, and 13, Schulz teaches that the gas flows from the outer scallops radially across the catalyst beds and into the central conduit. The central conduit 70 is a closed bottom and transports the effluent upward and out through nozzle 72 (Figure 5, column 9 lines 11-25). In Figure 4 depicting the serial arrangement, the effluent of each reaction stage is taken from the top, thus one having ordinary skill in the art would find it obvious that effluent is a the top of each reactor. With regards to claims 11 and 12, an outlet 28 is at the bottom of the reactor (column 8 line 45).
Regarding claim 14, Coupard teaches the reactors are side by side (not stacked) in Figure 1. The combination of Coupard and Schulz above teach one having ordinary skill in the art that it would be obvious to duplicate the reactors to have three. Thus, Coupard in light of Schulz suggests three reactors side by side.
Regarding claim 15, Schulz teaches in Figure 4 and Taheri in Figure 1 teach that the reactors are stacked, thus positioned in a single vertical axis.
Claims 14, 16, and 17 are rejected under 35 U.S.C. 103 as being unpatentable over Coupard US Patent 9,085,502 in view of Celik US Patent 8,313,561.
Regarding claim 14, Coupard teaches two radial reactors arranged side by side in Figure 1. Celik teaches more than 3 in Figure 2, thus teaching that it would be obvious to one having ordinary skill in the art to modify Coupard by including 3 radial reactors side by side.
Regarding claims 16 and 17, one having ordinary skill in the art would expect a natural pressure drop across the reactors in Coupard. However, Coupard does not explicitly teach a pressure drop of less than 69 kPa or less than 35 kPa.
Celik teaches a serial arrangement of radial reactors with a very pressure drop of about 138-207 Pa across the beds (column 17 line 48).
Thus, it would have been obvious to one having ordinary skill in the art to expect a low pressure drop from serially connected radial flow reactors as shown in Celik. One having ordinary skill in the art would further be motivated to have this arrangement because it would reduce a natural pressure drop in other types of reactors.
Conclusion
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/SHARON PREGLER/Primary Examiner, Art Unit 1772
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