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 .
Information Disclosure Statement
The information disclosure statement (IDS) submitted on 04/18/2023 has been considered by the Examiner.
Status of Claims
Claims 22-41, filed on 04/18/2023, are under consideration.
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.
Claim 41 is 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.
The term “gentle depolymerization” in claim 41 is a relative term which renders the claim indefinite. The term “gentle depolymerization” is not defined by the claim, the specification does not provide a standard for ascertaining the requisite degree, and one of ordinary skill in the art would not be reasonably apprised of the scope of the invention. Here, there is no discussion of what the conditions for gentle polystyrene depolymerization are and thus; the term is interpreted broadly to refer to any pyrolysis method that breaks down polystyrene into its monomers.
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 22-23, 25-31 and 36-31 are rejected under 35 U.S.C. 103 as being unpatentable over Ikematsu et al. (JP 2000 119440 A, translation attached, cited by Applicants), as evidenced by Jung et al. (“Fast pyrolysis of a waste fraction of high impact polystyrene (HIPS) containing brominated flame retardants in a fluidized bed reactor: The effects of various Ca-based additives (CaO, Ca(OH)2 and oyster shells) on the removal of bromine”, Fuel 95 (2012) 514–520; cited by Applicants).
Regarding claim 22, Ikematsu (Abstract) teaches a method to “reduce contaminating halogens, to form a decomposition product desirably usable as a fuel or a chemical material without being subjected to any halogen removal step, which process comprises heat-decomposing plastic wastes containing a halogen-containing flame retardant in the presence of an inorganic neutralizing agent”. In terms of the polymer being introduced, it is disclosed “The halogen-containing flame retardant is exemplified by a bromine-containing one such as tetrabromobisphenol A or a chlorine-containing one such as a chlorinated paraffin. The plastic is not particularly limited so far as it is heat-decomposable. The inorganic neutralizing agent is desirably an oxide, a hydroxide, or a carbonate of a group IA, IIA, or IIIB metal and is exemplified by calcium oxide. The necessary amount is 0.5-10 times as high as the number of chemical equivalents necessary to neutralize the halogens contained in the wastes… The heat decomposition temperature is in the range of 300-600 deg.C when the contained polymer is polyethylene, polypropylene, or polystyrene”. More specifically, Ikematsu teaches when the plastic waste to be treated is polystyrene, the cracked oil contains a large amount of styrene monomer, which can be recycled as a monomer. In this case, it is necessary to separate and purify the styrene monomer from the cracked oil (pg. 3 of translation, 6th paragraph).
Ikematsu is reasonably interpreted as a pyrolysis process for depolymerizing polystyrene (claimed compound A1) into styrene monomers. The polystyrene comprises flame retardant having halogen functionality such as bromine and chlorine: these compounds are similar to claimed compound A3). Compounds A1) and A3) are the only required compounds for polymer composition (A) of pending step a) I). The disclosed inorganic neutralizing agent being an oxide or hydroxide of Group IA or IIA metals such as calcium oxide are similar to the claimed inorganic basic compound (B) in pending step a) II).
Moreover, heat decomposition of polystyrene compound is exemplified by Ikematsu using a feed modeled in composition after High Impact Polystyrene (HIPS) as described in the examples (pg. 3 of translation, paragraphs 8-9): “The mixed plastic waste was processed into pellets having a diameter of about 3 mm and then used in a pyrolysis experiment. Next, a thermal decomposition experiment was performed. A 100 ml quartz flask equipped with a polymer inlet, a stirrer, and a vaporized gas outlet is prepared. Further, a cooling pipe and a receiver are prepared so as to be connected thereto. Plastic waste in flask 30 g, the inside of the apparatus is replaced with nitrogen, and then the nitrogen line is closed. Thereafter, it is gradually heated to 350 °C by an electric heater, and then kept at a constant temperature. As the temperature rises, the polymer softens, and then a decomposition gas is gradually generated. This gas is condensed and liquefied in a cooling pipe through which water flows, and is stored in a receiver. The non-condensable gas generated partially flows further and accumulates in the Teflon bag”.
This disclosure reads on pending step b) claiming thermal cleaving polystyrene in a reaction zone of pyrolysis reactor (e.g. the quartz reactor) to obtain a product mixture containing styrene monomers. It also reads on step c) of withdrawing the product mixture from the reactor, and step d) of cooling the mixture to obtain a condensed product containing styrene and further components.
For claimed step e), Ikematsu teaches when the plastic waste to be treated is polystyrene, the cracked oil contains a large amount of styrene monomer, which can be recycled as a monomer. In this case, it is necessary to separate and purify the styrene monomer from the cracked oil (pg. 3 of translation, 6th paragraph): here the cracked oil being separated from styrene is considered the claimed “further components”.
For the recited limitation “wherein no antimony oxide (Sb2O3) is present in the polymer composition (A) or in the at least one inorganic basic compound (B)”, it is noted the Ikematsu does not require the presence of antimony in the flame retardant or the neutralizing agent.
Ikematsu suggests using 0.5-10 equivalents of neutralizing agent to halogens, but the reference does not provide amounts of halogen present in the plastic. The provided tables in the translation document are not illegible. However, Jung discloses the composition of high impact polystyrene plastic (section 2.1 on pg. 515) which is similar to the plastic model of Ikematsu; HIPS contains about 5.6 wt% bromine based on the weight of the polystyrene plastic (or about 5.7 wt% if we exclude Sb from the table).
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Therefore, it can be reasonably expected that HIPS contains about 5.6 wt% halogen/bromine. Using this amount in calculating the amount of inorganic neutralizing agent which is 0.5-10 times the amount of bromine, it equals 2.8-56 wt%.
The disclosed amount of inorganic neutralizing agent being 2.8-56 wt% overlaps the claimed amounts of 0.05-75 wt% of inorganic basic compound (B) in step a) II). Furthermore, the disclosed amount of polystyrene being introduced can be 94.4 wt% of the polymer sample being pyrolyzed (minus the weight of the bromine) which overlaps:
1) the claimed amount of 25-99.95 wt% of polymer composition (A) in step a) I);
2) the claimed amount of 30-99.9999 wt% styrene-containing polymer in step a) I) A1); and
3) the claimed amount of 10-100% polymer with repeating styrene monomers in step a) I) A1) Ia).
Also, the disclosed amount of bromine being 5.6 wt% overlaps the claimed amount of 0.0001-50 wt% halogen containing compound (A3) in step a) I) A3). These range overlaps establish prima facie case of obviousness—see MPEP 2144.05.I.
Regarding claim 23, Ikematsu teaches pyrolysis temperature of 300-600°C such as 350-500 °C (pg. 3, 3rd paragraph) which overlaps the claimed range of 250-1000 °C.
Regarding claim 25, Ikematsu teaches regarding the reaction pressure: “It is easiest for equipment to set the pressure of the pyrolysis tank to normal pressure. However, suppressing the vaporization of the decomposition gas by increasing the pressure in the pyrolysis tank increases the liquid retention in the tank and lowers the viscosity of the pyrolysis tank contents. As a result, stirring and heat transfer are facilitated, which is preferable in some cases. Conversely, reducing the pressure in the tank in order to reduce the stagnation of the liquid and the decomposition gas in the tank, the side reaction of the thermal decomposition is suppressed. It may be preferable in some cases” (pg. 3, paragraph 4). Here, it can be reasonably assumed that Ikematsu reasonably suggests using normal pressure (e.g. 1 atm or 1013 milibar); lower pressures are also suggested (less than 1013 mbar) to reduce side reaction of liquid pyrolysis products. The disclosed values of 1013 mbar or less overlaps the claimed value of less than 1200 mbar.
Regarding claim 26, Ikematsu teaches “Further, depending on the conditions, the crude cracked oil may contain a component having a relatively high molecular weight or an extremely high boiling point. In such a case, if necessary, fractionation can be performed at a boiling point or the like through a fractionation tower, or high-boiling components can be cut off by a distillation operation. Such fractionation or distillation may be preferred for use of the cracked oil for fuel or other purposes. Further, when the plastic waste to be treated is polystyrene, the cracked oil contains a large amount of styrene monomer, which can be recycled as a monomer. In this case, it is necessary to separate and purify the styrene monomer from the cracked oil. In this case as well, known purification operations and techniques such as fractionation and adsorption can be used” (pg. 3, 6th paragraph).
Regarding claim 27, Ikematsu teaches halogen containing compound (A3) is the organic flame retardant and is exemplified by a bromine-containing such as tetra-bromo-bisphenol A or a chlorine-containing such as a chlorinated paraffin (Abstract).
Regarding claim 28, Ikematsu teaches the polymer composition comprises about 5.6 wt% halogen which is within the claimed amount of at least 10 ppm.
Regarding claim 29, it should be noted that “main group metals” is interpreted as elements of Groups 1-2 and 13-15 of the periodic tables including calcium (Group 2 metal). Here, Ikematsu teaches the inorganic neutralizing agent (inorganic basic compound B) is an oxide, a hydroxide, or a carbonate of a group IA, IIA, or IIIB metal and is exemplified by calcium oxide (Abstract). Also, CaO reads on the alkaline earth metal oxide of pending claim 30.
Regarding claim 31, it should be noted that the recited “and any further polymers (A2) present are polymethyl methacrylate” is considered optional since the word “any” does not positively recite the presence of polymethyl methacrylate. As discussed above, Ikematsu teaches the styrene-containing polymer (A1) is polystyrene.
Regarding claim 36, Ikematsu does not require the presence of antimony in the process.
Regarding claim 37, Ikematsu does not specifically suggest that the condensed product mixture (G') contains more than 40% by weight of styrene, based on the total weight of the repeating units (la) derived from styrene in the at least one styrene-containing polymer (Al). However, the reference does recognize when the plastic waste to be treated is polystyrene, the cracked oil contains a large amount of styrene monomer, which can be recycled as a monomer (pg. 3 paragraph 6). Considering that the reference discloses similar process feed, neutralizing agents, and overlapping temperatures to the instant claims, it is expected that the reference process provides similar products to G’: "The fact that appellant has recognized another advantage which would flow naturally from following the suggestion of the prior art cannot be the basis for patentability when the differences would otherwise be obvious."—see MPEP 2145 II.
Regarding claim 38, Ikematsu teaches a condensed product mixture containing styrene monomers and further components obtained from step d) of the process of claim 22, as discussed above.
Regarding claim 39, Ikematsu teaches the styrene monomer-containing liquid obtained by the process of claim 22, as discussed above.
Regarding claim 40, Ikematsu teaches the styrene monomer-containing liquid as discussed above however, the reference does not disclose the claimed amount halogenated compounds being less than 1000 ppm, based on the total weight of the styrene monomer-containing liquid. Here, the amount of halogen in the product of the prior art process is viewed as implicit, and in the absence of criticality or evidence to the contrary, it is assumed that the prior art styrene meets the claimed amount halogenated compounds being less than 1000 ppm because both the instant claims and the prior art teach similar pyrolysis feeds (HIP), similar basic neutralizer (CaO), and similar pyrolysis temperatures (around 300-500 °C).
Regarding claim 41, Ikematsu teaches the apparatus for performing the process of claim 22, comprising a pyrolysis reactor (P) having a reaction zone (R) (the discussed quartz flow cell of Examples on pg. 3 of translation), wherein the apparatus is configured such that gentle depolymerization of styrene of the polymer composition (A) is carried out (the product contains styrene monomer as discussed above).
Claims 24 and 32-34 are rejected under 35 U.S.C. 103 as being unpatentable over Ikematsu as applied to claim 22 above, and further in view of Sasaki et al. (US 2010/0121097).
It is noted that Ikematsu mixes the basic neutralizer with the HIP plastic as pellets for the experiments (pg. 3 of translation).Ikematsu is silent about the claimed wherein the at least one inorganic basic compound (B) is introduced into the reaction zone (R) of the pyrolysis reactor (P) independently of the polymer composition (A) and in the course of the process is wholly or partially, continuously or discontinuously withdrawn from the reaction zone (R) and wholly or partially replaced by at least one unused inorganic basic compound (B) recited in pending claim 32. Ikematsu is also silent about pending claim 33 reciting wherein the pyrolysis reactor (P) is a fluidized bed reactor and a fluidized bed of the fluidized bed reactor wholly or partially consists of the at least one inorganic basic compound (B), and pending claim 34 reciting wherein the pyrolysis reactor (P) is a twin-screw extruder, a continuous stirred tank reactor, or a vortex reactor. Furthermore, Ikematsu is silent about pending claim 24 reciting wherein an average residence time (Z) of the polymer composition (A) in the reaction zone (R) of the pyrolysis reactor (P) in step b) is from 0.01 seconds to 21,600 seconds.
However, Sasaki discloses a method to pyrolyze resin, including polystyrene [0102]-[0103], to produce pyrolysis products comprising monomers such as styrene [0104]-[0106]. The pyrolysis of the resin is carried out continuously with solids such as CaO that act to provide heat to the pyrolysis reaction as well as trap halogens such as chlorine [0093]: “The solid particles are not particularly limited and examples thereof include sand, ceramic particles, metal particles, metal oxide particles, metal hydroxide particles, and metal halide particles. The solid particles may be used alone or in combination of two or more kinds. The solid particles may be inert to the pyrolysis of the resin, may be a catalyst promoting the pyrolysis of the resin, or may absorb harmful materials generated from the resin. For example, when resin including chlorine atoms in molecules, such as polyvinyl chloride resin, is heated and pyrolyzed, toxic materials such as chlorine, hydrogen chloride, and chlorine-containing materials are generated. It is preferable that the solid particles such as calcium oxide, calcium hydroxide, and calcium carbide neutralize or absorbs chlorine, hydrogen chloride, and chlorine-containing materials”.
Here, it is clear that the field of endeavor of Ikematsu is similar to Sasaki considering that they are both directed to the depolymerization of polystyrenes at 350-500 °C in the presence of basic metal oxides, that neutralize halogens, to make monomers with low halogen contents. Viewing the art from experimental scale of Ikematsu, to larger scale continuous process, it would have been obvious to one of ordinary skill in art and before the effective filing date of the instant invention to have used the fluidized bed depolymerization techniques of Sasaki in the method of Ikematsu because this involves using effective continuous fluidized bed techniques in this technical endeavor, and because this involves applying known polystyrene depolymerization /pyrolysis techniques with predictable results and a reasonable expectation of success—see MPEP 2143 I, 2143 A, 2143 D, and 2143.02.
Regarding claim 32, The basic neutralizer particles (e.g. CaO solids) are introduced separately, after being heated/regenerated, into the fluidized bed pyrolysis reactor (Fig. 7 label B and [0077] and [0084]). The independent feeding of the solid particles allows the control of heating rate to the resin being pyrolyzed and to maintain reaction temperature of about 350-500 °C [0073].
The residence time of the solids in the pyrolysis reactor, which is assumed similar to the polymer particles since they both move together in the fluidizes bed, is disclosed to be 0.5-1.5 hrs (Sasaki at [0035] and [0123]-[0126]) which reads on time recited in pending claim 24 of 0.01-21,600 seconds (up to 6 hours).
Regarding claim 33, Ikematsu in view of Sasaki disclose using metal oxides solid particles B, such as CaO, as the fluidized bed in the depolymerization of polystyrene (Sasaki at [0073] and [0093]).
Regarding claim 34, Ikematsu in view of Sasaki (at [0140]) disclose using twin screw feeders in the pyrolysis reactor (claimed label P) to feed the resin into the pyrolysis reaction zone (claimed label R).
Claim 35 is rejected under 35 U.S.C. 103 as being unpatentable over Ikematsu as applied to claim 22 above, and further in view of Wu et al. (US 2022/0402006).
Ikematsu is silent about wherein the reaction zone (R) of the pyrolysis reactor (P) is heated through microwave-assisted heating.
However, Wu teaches an efficient method for pyrolysis of plastics to produce petrochemical intermediates ([0007]-[0010] and Fig. 1) including polystyrene ([0164]-[0165]) wherein the pyrolysis reactor can be a microwave reactor [0211].
Therefore, and before the effective filing date of in the instant invention, it would have been obvious to one of ordinary skill in the art to have used microwave reactor in pyrolysis of polystyrene, as suggested by Wu, because this this involves using effective pyrolysis reactor technique with predictable results and a reasonable expectation of success—see MPEP 2143 I, 2143 A, 2143 D, and 2143.02.
Conclusion
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/ALI Z FADHEL/Primary Examiner, Art Unit 1772
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