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
It is noted that an information disclosure statement (IDS) was not included in the electronic file wrapper of the instant application. Applicant is reminded of the duty to disclose information material to patentability as defined by 37 C.F.R. 1.56 (also see MPEP 2001).
Claim Objection
Claims 1-13 are objected to because of the following informalities:
Claim 1: please amend “at least one polymer (Pol1, Pol2),” to -- at least one polymer (Pol1, Pol2), and --; “the at least one reference parameter of a first database relative to at least said polymer” to -- the at least one reference parameter of [[a]] the first database relative to the at least [[said]] one polymer--.
Claims 2-13: please amend “A method as claimed” to – [[A]] The method as claimed--.
Claim 2: please amend “in step c)” to -- in the step c)--.
Claim 3: please amend “steps a) and b)” to – the steps a) and b)--; “during said first heating sequence and/or” (there are five places) to -- during said first heating sequence, and/or--; “during said second heating sequence and/or” to -- during said second heating sequence, and/or--; “a representative quantity of carbon dioxide released by said sample of said defined polymer type during said second heating sequence,” to -- a representative quantity of carbon dioxide released by said sample of said defined polymer type during said second heating sequence, and --.
Claim 4: please amend “step II)” to – the step II)--.
Claim 5: please amend “in claim 2 and in any one of claim 3 or 4 wherein” to – in claim 2 , wherein--; “in step c)” to -- in the step c)--.
Claim 6: please amend “in step c)” to -- in the step c)--; “steps a) and b)” to -- the steps a) and b)--; “during said first heating sequence and/or” (there are five places) to -- during said first heating sequence, and/or--; “during said second heating sequence and/or” to -- during said second heating sequence, and/or--; “a representative quantity of carbon dioxide released by said sample of said defined matrix type during said second heating sequence” to --a representative quantity of carbon dioxide released by said sample of said defined matrix type during said second heating sequence, and--; “the reference parameter(s) of the second database” to --the at least one reference parameter[[(s)]] of the second database--; “in step d)” to -- in the step d)--; “a quantity of said at least one polymer” to – [[a]] the quantity of said at least one polymer--.
Claim 7: please amend “step ii)” to – the step ii)--.
Claim 8: please amend “step c)” to – the step c)--.
Claim 9: please amend “step c)” to – the step c)--; “step d)” to – the step d)--; “one at least of these differences” to --one temperature differences--; “one concludes to the absence of this defined polymer type in said porous medium” to --one concludes to the absence of [[this]] the defined polymer type in said porous medium--.
Claim 10: please amend “step d)” to – the step d)--; “said type of said defined polymer” to -- said type--.
Claim 11: please amend “step c)” to – the step c)--; “the initial mass” to – [[the]] an initial mass --.
Claim 12: please amend “an inert atmosphere” to – [[an]] the inert atmosphere--.
Claim 13: please amend “an oxidizing atmosphere” to – [[an]] the oxidizing atmosphere--; “40 °/minute” to --40 °C/minute--.
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 1-13 are rejected under 35 U.S.C. 112(b) or 35 U.S.C. 112 (pre-AIA ), second paragraph, as failing to set forth 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.
Regarding claim 1, claim 1 recites “a porous medium such as a natural porous medium”, wherein the phrase "such as" renders the claim indefinite because it is unclear whether the limitations following the phrase are part of the claimed invention. See MPEP § 2173.05(d). Claims 2-13 are further rejected by virtue of their dependence upon and because they fail to cure the deficiencies of indefinite claim 1.
Regarding claim 3, claim 3 recites “defining several types of polymer (Pol1, Pol2), preferably at least polyethylene terephthalate, polyethylene, polyamide and/or perfluoroalkoxy”. 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 3 recites the broad recitation “several types of polymer”, and the claim also recites “preferably at least polyethylene terephthalate, polyethylene, polyamide and/or perfluoroalkoxy” 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 4 is further rejected by virtue of its dependence upon and because it fails to cure the deficiencies of indefinite claim 3.
Regarding claim 6, claim 6 recites “defining several types of porous media matrices, preferably the matrix types comprise at least sand, marl, carbonates and clays”. 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 6 recites the broad recitation “several types of porous media matrices”, and the claim also recites “preferably the matrix types comprise at least sand, marl, carbonates and clays” 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 claim. Claim 7 is further rejected by virtue of its dependence upon and because it fails to cure the deficiencies of indefinite claim 6.
Regarding claim 6, claim 6 recites “the at least one reference parameter of the second database preferably further comprising at least:” and “and preferably, in step d), characterizing the presence or the absence of said at least one polymer in the porous medium, and/or determining a quantity of said at least one polymer in said porous medium (c_pol, q_pol) from said comparison of said at least one parameter determined from at least one of said curves of one of said measured quantities with the at least one reference parameter of the second database relative to at least one matrix representative of the porous medium”. 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). The claim(s) are considered indefinite because there is a question or doubt as to whether the feature introduced by such narrower language of preferably is (a) merely exemplary of the remainder of the claim, and therefore not required, or (b) a required feature of the claim. Claim 7 is further rejected by virtue of its dependence upon and because it fails to cure the deficiencies of indefinite claim 6.
Regarding claim 8, “said second database” lacks antecedent basis, thus the scope of claim 8 is indefinite.
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 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.
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 1-5 and 9-11 are rejected under 35 U.S.C. 103 as being unpatentable over David et al. (Introducing a soil universal model method (SUMM) and its application for qualitative and quantitative determination of poly(ethylene), poly(styrene), poly(vinyl chloride) and poly(ethylene terephthalate) microplastics in a model soil, Chemosphere, 2019, 225, 810-819), and in view of Dümichen et al. (Analysis of polyethylene microplastics in environmental samples using a thermal decomposition method, Water Research, 2015, 85, 451-457) and Lafargue et al. (US6048497A).
Regarding claim 1, David teaches a method for characterization of the presence and/or for quantification of at least one polymer (Pol1, Pol2) in a porous medium such as a natural porous medium (a soil universal model method and its application for qualitative and quantitative determination of poly(ethylene), poly(styrene), poly(vinyl chloride) and poly(ethylene terephthalate) microplastics in a model soil [title]), characterized in that at least the following steps are carried out:
b) heating a soil sample of the porous medium according to a second heating sequence in an oxidizing atmosphere, and continuously measuring total quantity of substance thermally released during the heating sequence by means of mass loss (see section 2.2 and Figs. 1-2);
c) determining at least one parameter from at least one curve of the measured quantity, and comparing said at least one parameter with at least one reference parameter of a first database relative to said at least one polymer (see Figs. 1-3 and section 3. Results and discussion; Fig.1 shows significant changes in TGA plots after addition of microplastics in the temperature area between 30 and 550 oC. These changes were polymer-type-dependent in terms of temperatures intervals and rate of degradation, which were then further used for the qualitative and quantitative determination of microplastics in soils [section 3.1]; PET records showed a sharp peak around 400 oC; PS has a broad intensive peak around 330 oC and a second less intense peak around 400-410 oC with the ratio between the intensities 330/410 varying between 1.5 and 2. Degradation of PF produces a sharp low intensity peak at 250 oC. The difference is directly indicative to the microplastics polymer. Quantitative analysis can be carried out upon the calibration, i.e., spiking of the blank soil by the determined polymer. Fig.3 shows an example of the dependence of the difference in mass loss between spiked sample and blank soil at 400 oC [section 3.2]),
d) from said comparison of said at least one parameter characterizing the presence or the absence of said at least one polymer in the porous medium, and/or determining a quantity of said at least one polymer in said porous medium (c_pol, q_pol) (The difference is directly indicative to the microplastics polymer. Quantitative analysis can be carried out upon the calibration, i.e., spiking of the blank soil by the determined polymer. Fig.3 shows an example of the dependence of the difference in mass loss between spiked sample and blank soil at 400 oC [section 3.2]; More polymers are needed to obtain a large database for microplastics identification and determination as well as analyses of soil mixtures contaminated by more than one polymer type [section of Limited number of polymers on page 817]).
David is silent to: a) heating the sample of said porous medium, according to a first heating sequence in an inert atmosphere, and continuously measuring a representative quantity of hydrocarbon compounds released during said first heating sequence (HC), a representative quantity of carbon monoxide and/or a representative quantity of carbon dioxide released during said first heating sequence (CO_inert, CO2_inert); (b) the residue of the sample resulting from the first heating cycle is heated in the second heating sequence in the oxidizing atmosphere; and instead of measuring the mass loss, the quantity of hydrocarbon compounds, carbon monoxide, and/or carbon dioxide released during said first and/or the second heating sequences is/are measured.
Dümichen teaches analysis of polyethylene microplastics in environmental media by using a thermal decomposition method (title and abstract), and further teaches in TGA samples were heated up and mass loss measured as a function of temperature or time. For polymer characterization, the weight change of sample masses up to 100 mg can be measured under inert atmospheres (section 3.1 on page 453). In Py-GC-MS measurements the pyrograms show a number of groups with three to five peaks. In each group one peak can be contributed to saturated and one peak to di-unsaturated hydrocarbons. A third peak can be attributed to a mono-unsaturated hydrocarbon. The results of decomposition gas analysis using TED-GC-MS are presented in Fig.3 (section 3.3). Table 1 shows identified species of PE decomposition. Thus, Dümichen teaches heating a sample of said porous medium, according to a first heating sequence in an inert atmosphere (see section 3.2 and caption of Fig.1), and continuously measuring a representative quantity of hydrocarbon compounds released during said first heating sequence (HC).
Lafargue teaches a method of evaluating at least one pollution characteristic of natural soils contaminated by hydrocarbon compounds, wherein the sample is first heated in a non-oxidizing atmosphere, and measuring an amount of hydrocarbon compounds released after feeding the sample into the first heater; and then transferring the sample from the first heater into a second heater operating in an oxidizing atmosphere, a CO2 measuring device determining CO2 contained each effluent discharged from the two heaters, said CO2 measuring device measuring continuously the CO2 throughout the heating cycle of the first and the second heaters and including a device measuring CO contained in each effluent discharged from the two heaters (abstract). Thus, Lafargue teaches heating the sample in natural soil according to a first heating sequence in an inert atmosphere, and continuously measuring a representative quantity of hydrocarbon compounds released during said first heating sequence (HC), a representative quantity of carbon monoxide and/or a representative quantity of carbon dioxide released during said first heating sequence (CO_inert, CO2_inert); (b) heating the residue of the sample from the first heating cycle in the second heating sequence in the oxidizing atmosphere, and continuously measuring a representative quantity of carbon monoxide and/or a representative quantity of carbon dioxide released during said second heating sequence (CO_oxyd, CO2_oxyd).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the method in David by adding the step of heating a sample of said porous medium, according to a first heating sequence in an inert atmosphere, and continuously measuring a representative quantity of hydrocarbon compounds released during said first heating sequence (HC), a representative quantity of carbon monoxide and/or a representative quantity of carbon dioxide released during said first heating sequence (CO_inert, CO2_inert); and b) heating a residue of said sample from said first heating sequence according to a second heating sequence in an oxidizing atmosphere, and continuously measuring a representative quantity of carbon monoxide and/or a representative quantity of carbon dioxide released during said second heating sequence (CO_oxyd, CO2_oxyd), as taught by combined Dümichen and Lafargue, since it would allow to identify and even to quantify polymer particles in various matrices through the characteristic decomposition products known for every kind of polymer (abstract in Dümichen) and would deduce at least one pollution characteristic of said sample from the measured quantities representative of the nature and of the amount of hydrocarbon compounds (Col. 2 Ln 33-40 in Lafargue).
Furthermore, It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the step of determining at least one parameter to determine the at least one parameter from at least one curve of the measured hydrocarbon compounds released from the first heating sequence, carbon monoxide and/or carbon monoxide released during the first and/or the second heating sequences, and comparing said at least one parameter with at least one reference parameter of a first database relative to said at least one polymer, since it would allow to identify and even to quantify polymer particles in various matrices through the characteristic decomposition products known for every kind of polymer (abstract in Dümichen) and would deduce at least one pollution characteristic of said sample from the measured quantities representative of the nature and of the amount of hydrocarbon compounds (Col. 2 Ln 33-40 in Lafargue).
Regarding claim 2, modified David teaches the method as claimed in claim 1 wherein, in step c), at least one temperature corresponding to a peak of said curve of said measured representative quantity of hydrocarbon compounds released during the first heating sequence (HC) is determined (at least four quantities Q0, Q1, Q2, Q3 representative of the nature and of the amount of hydrocarbon compounds contained in said sample are determined from the previous four stages [Col. 2 Ln1 -40 in Lafargue ; Fig. 3 in Lafargue shows the temperature profile, and Fig.4 in Lafargue shows the corresponding peaks Q0-Q4 at the respective temperatures).
Regarding claim 3, modified David teaches the method as claimed in claim 1, wherein the first database is built as follows:
I) defining several types of polymer (Pol1, Pol2) (David teaches identifying PE, PET, PVC and PS [title, Figs. 1-3]), preferably at least polyethylene terephthalate and/or polyethylene (see title in David),
II) for each defined polymer type, applying steps a) and b) to a sample of each defined polymer type in place of said sample of said porous medium, and determining for each defined polymer type the at least one reference parameter of the first database (see section 2.1 and Figs. 1-3 in David), the at least one reference parameter of the first database comprising at least one temperature to which the following correspond:
a peak of said curve of said measured representative quantity of hydrocarbon compounds released by said sample of said defined polymer type during said first heating sequence (as outlined in the rejection of claim 1 above, hydrocarbon compounds released from the first heating sequence is measured and Figs. 3-4 in Lafargue show at least one temperature corresponding to a peak of the measured hydrocarbon compounds [Col. 2 Ln 1-40]),
and the at least one reference parameter of the first database further preferably comprising at least: a representative quantity of hydrocarbon compounds released by said sample of said defined polymer type during said first heating sequence and/or
a representative quantity of carbon monoxide and/or a representative quantity of carbon dioxide released by said sample of said defined polymer type during said first heating sequence and/or a representative quantity of carbon monoxide and/or a representative quantity of carbon dioxide released by said sample of said defined polymer type during said second heating sequence (this limitation is not required due to the phrase “preferably”; Furthermore, as outlined in the rejection of claim 1 above, Lafargue teaches measuring hydrocarbon compounds, CO, and/CO2 during the first heating sequence, and CO and/CO2 during the second heating sequence [abstract]),
III) adding to the first database, for each defined polymer type, the at least one reference parameter of the first database (David teaches adding the at least one reference parameter of the first database for each defined polymer type [section 3.2 and Fig.3]; Lafargue teaches measuring hydrocarbon compounds, CO, and/CO2 during the first heating sequence, and CO and/CO2 during the second heating sequence to determine the pollution characteristic [abstract]. Thus, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to add to the first database, for each defined polymer type, the at least one reference parameter of the first database for identifying and quantifying polymer particles in various matrices).
Regarding claim 4, modified David teaches the method as claimed in claim 3, wherein step II) is repeated with several samples of each defined polymer type (David teaches the soils were analyzed in duplicate and results were averaged [section 2.2]).
Regarding claim 5, modified David teaches the method as claimed in claim 2, wherein, in step c), at least one of the temperatures determined in step c) (Tpeak2) for the porous medium sample is compared with at least one corresponding temperature of the at least one reference parameter of said first database (Tpeak1) (David teaches PET records showed a sharp peak around 400 oC; Thermal degradation of PS resulted in a broad intensive peak around 330 oC and a second less intense peak around 400-410 oC; Degradation of PE produced a sharp low intensity peak at 250 oC; and PVC produced a sharp peak at 270 oC. The difference is directly indicative to the microplastics polymer. Quantitative analysis can be carried out upon the calibration, i.e., spiking of the blank soil by the determined polymer [section 3.2]; Thus, in the step c Tpeak2 for the porous medium sample is compared with Tpeak1 of the at least one reference parameter of said first database to determine each type of polymer).
Regarding claim 9, modified David teaches the method as claimed in claim 5, and David teaches wherein, in step c), the comparison is made by calculating at least a difference between at least one temperature corresponding to said peak of one of said curves of the quantities measured on said sample of said porous medium (Tpeak2) and the corresponding temperature of the at least one reference parameter for each defined polymer type of the first database (Tpeak1), and in step d), if, for at least one of the defined polymer types, one at least of these differences is below a predetermined threshold, one concludes to the presence of this defined polymer type in said porous medium and, in the opposite case, one concludes to the absence of this defined polymer type in said porous medium (Fig.1 shows significant changes in TGA plots after addition of microplastics in the temperature area between 30 and 550 oC. These changes were polymer-type-dependent in terms of temperatures intervals and rate of degradation, which were then further used for the qualitative and quantitative determination of microplastics in soils [section 3.1]; PET records showed a sharp peak around 400 oC; PS has a broad intensive peak around 330 oC and a second less intense peak around 400-410 oC with the ratio between the intensities 330/410 varying between 1.5 and 2. Degradation of PF produces a sharp low intensity peak at 250 oC. The difference is directly indicative to the microplastics polymer. Quantitative analysis can be carried out upon the calibration, i.e., spiking of the blank soil by the determined polymer. Fig.3 shows an example of the dependence of the difference in mass loss between spiked sample and blank soil at 400 oC [section 3.2]. Thus the presence/absence of peak(s) at respective temperature(s) is/are used to determine the presence/absence of the corresponding polymer in the soil sample, and the temperature difference of the peaks is directly indicative to the microplastics polymer).
Regarding claim 10, modified David teaches the method as claimed in claim 9, and David teaches wherein, in step d), if one has concluded to the presence of said defined polymer type in said porous medium, said type of said defined polymer in said porous medium is quantified by determining a percentage of said defined polymer type in said porous medium from a ratio between the measured representative quantity of thermal mass loss from the sample and the measured mass loss of said defined polymer type (see normalized thermal mass loss in y-axis of Fig.2 and caption of Fig.2), and if one has concluded to the absence of said defined polymer type in said porous medium, a zero quantity is assigned to said defined polymer type (the normalized thermal mass loss is zero in the absence of the defined polymer type in the porous medium, as shown in Fig.2).
David is silent to wherein the ratio is between the measured representative quantity of hydrocarbon compounds released during the first heating sequence in the porous medium sample and the measured representative quantity of hydrocarbon compounds released by said defined polymer type during the first heating sequence.
As outlined in the rejection of claim 1 above, Lafargue teaches measuring hydrocarbon compounds released during the first heating sequence in the porous medium sample (abstract). Dümichen teaches measuring a representative quantity of hydrocarbon compounds released during said first heating sequence (HC).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to use the ratio between the measured representative quantity of hydrocarbon compounds released during the first heating sequence in the porous medium sample and the measured representative quantity of hydrocarbon compounds released by said defined polymer type during the first heating sequence, since it would allow to identity and quantify polymer particles in various matrices (abstract in Dümichen).
Regarding claim 11, modified David teaches the method as claimed in claim 1, and David teaches wherein, in step c), the measured representative quantities of thermal mass loss are normalized by the initial mass of the sample (see Normalized thermal mass loss in y-axis of Fig.2).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to normalize the measured representative quantities of hydrocarbon compounds, carbon monoxide and carbon dioxide by the initial mass of the sample to show the amount of hydrocarbon compounds, carbon monoxide and carbon dioxide released from the initial mass of the sample in the same way as normalizing the measured thermal mass loss as that in Fig.2 of David.
Claims 6-8 are rejected under 35 U.S.C. 103 as being unpatentable over David, Dümichen and Lafargue, as applied to claim 1 above, and further in view of Banerjee et al. (Analysis of hydrocarbon-contaminated soil by thermal extraction-gas chromatography, Environ. Sci. Technol., 1997, 31, 646-650).
Regarding claim 6, modified David teaches the method as claimed in claim 1, and David is silent to in step c), said at least one parameter is compared with at least one reference parameter of a second database relative to at least one matrix representative of said porous medium, the second database being built as follows:
i) defining several types of porous media matrices, preferably the matrix types comprise at least sand, marl, carbonates and clays,
ii) for each defined matrix type, carrying out steps a) and b) with a sample of each defined matrix type in place of said sample of said porous medium, and determining for each defined matrix type the at least one reference parameter of the second database, the at least one reference parameter of the second database comprising at least one temperature to which the following correspond:
a peak of said curve of said measured representative quantity of hydrocarbon compounds released by said sample of said defined matrix type during said first heating sequence and/or
a peak of said curve of said measured representative quantity of carbon monoxide released by said sample of said defined matrix type during said first heating sequence and/or
a peak of said curve of said measured representative quantity of carbon dioxide released by said sample of said defined matrix type during said first heating sequence and/or
a peak of said curve of said measured representative quantity of carbon monoxide released by said sample of said defined matrix type during said second heating sequence and/or
a peak of said curve of said measured representative quantity of carbon dioxide released by said sample of said defined matrix type during said second heating sequence,
and the at least one reference parameter of the second database preferably further comprising at least:
a representative quantity of hydrocarbon compounds released by said sample of said defined matrix type during said first heating sequence and/or
a representative quantity of carbon monoxide and/or a representative quantity of carbon dioxide released by said sample of said defined matrix type during said first heating sequence and/or
a representative quantity of carbon monoxide and/or a representative quantity of carbon dioxide released by said sample of said defined matrix type during said second heating sequence
iii) adding to the second database, for each defined matrix type, the reference parameter(s) of the second database,
and preferably, in step d), characterizing the presence or the absence of said at least one polymer in the porous medium, and/or determining a quantity of said at least one polymer in said porous medium (c_pol, q_pol) from said comparison of said at least one parameter determined from at least one of said curves of one of said measured quantities with the at least one reference parameter of the second database relative to at least one matrix representative of the porous medium.
Dümichen does teach through the characteristic decomposition products known for every kind of polymer it is possible to identify and even to quantify polymer particles in various matrices (abstract). Dümichen further teaches as environmental matrices, soil, suspended solids and mussels were used (the 2nd paragraph in Col. 2 on page 452).
Banerjee teaches a method of analyze hydrocarbons in cresosote- and petroleum-contaminated soil (abstract). Both soils have significant clay content (Table 1) and a higher content of nonvolatile compounds; therefore, the matrix factors must be attributed to cracking of nonvolatile hydrocarbons in the solid matrix during the thermal desorption at 325 oC (the 3rd paragraph in Col. 1 on page 650).
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the method of modified David to take into account the effects of different matrices in the step c) such that said at least one parameter is compared with at least one reference parameter of a second database relative to at least one matrix representative of said porous medium, the second database being built as follows:
i) defining several types of porous media matrices, preferably the matrix types comprise at least sand, marl, carbonates and clays (various environmental matrices [the 2nd paragraph in Col. 2 on page 452 in Dümichen]; soils having significantly different clay contents [Table 1 in Banerjee]),
ii) for each defined matrix type, carrying out steps a) and b) with a sample of each defined matrix type in place of said sample of said porous medium, and determining for each defined matrix type the at least one reference parameter of the second database (carrying out the steps a and b in claim 1 by using a sample of each defined matrix type in place of said sample of said porous medium), the at least one reference parameter of the second database comprising at least one temperature to which the following correspond a peak of said curve of said measured representative quantity of hydrocarbon compounds released by said sample of said defined matrix type during said first heating sequence (as outlined in the rejection of claim 1 above, hydrocarbon compounds released from the first heating sequence is measured for each sample and Figs. 3-4 in Lafargue show at least one temperature corresponding to a peak of the measured hydrocarbon compounds [Col. 2 Ln 1-40]),
and the at least one reference parameter of the second database preferably further comprising at least: a representative quantity of hydrocarbon compounds released by said sample of said defined matrix type during said first heating sequence (this limitation is not required due to the phrase “preferably”; furthermore, Lafargue teaches the at least one reference parameter comprising at least a representative quantity of hydrocarbon compounds released by said sample during said first heating sequence [abstract]),
iii) adding to the second database, for each defined matrix type, the reference parameter(s) of the second database (since the matrix factors must be attributed to cracking of nonvolatile hydrocarbons in the solid matrix during the thermal desorption at 325 oC [the 3rd paragraph in Col. 1 on page 650 in Banerjee], it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to add to the second database, for each defined matrix type, the reference parameter(s) of the second database in order to take into account the effects of the different matrices),
and preferably, in step d), characterizing the presence or the absence of said at least one polymer in the porous medium, and/or determining a quantity of said at least one polymer in said porous medium (c_pol, q_pol) from said comparison of said at least one parameter determined from at least one of said curves of one of said measured quantities with the at least one reference parameter of the second database relative to at least one matrix representative of the porous medium (first, this limitation is not required due to the phrase “preferably”; Furthermore, It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the step d for characterizing the presence or the absence of said at least one polymer in the porous medium, and/or determining a quantity of said at least one polymer in said porous medium (c_pol, q_pol) from said comparison of said at least one parameter determined from at least one of said curves of one of said measured quantities with the at least one reference parameter of the second database relative to at least one matrix representative of the porous medium since it would take into account the effects of the different matrices).
Regarding claim 7, modified David teaches the method as claimed in claim 6, and David further teaches wherein step ii) is repeated with several samples of each soil (the soils were analyzed by TGA/SDTA 851 in duplicate and results were averaged [section 2.2]). Thus, it would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to repeat the step ii) with several samples of each defined matrix type, and average the measured results.
Regarding claim 8, modified David teaches the method as claimed in claim 6, and David is silent to in step c), at least one of the temperatures determined in step c) is compared with at least one corresponding temperature of the at least one reference parameter of said second database.
David does teach Fig.1 shows significant changes in TGA plots after addition of microplastics in the temperature area between 30 and 550 oC. These changes were polymer-type-dependent in terms of temperatures intervals and rate of degradation, which were then further used for the qualitative and quantitative determination of microplastics in soils [section 3.1]; PET records showed a sharp peak around 400 oC; PS has a broad intensive peak around 330 oC and a second less intense peak around 400-410 oC with the ratio between the intensities 330/410 varying between 1.5 and 2. Degradation of PF produces a sharp low intensity peak at 250 oC. The difference is directly indicative to the microplastics polymer. Quantitative analysis can be carried out upon the calibration, i.e., spiking of the blank soil by the determined polymer. Fig.3 shows an example of the dependence of the difference in mass loss between spiked sample and blank soil at 400 oC [section 3.2]. Thus the difference in temperature corresponding to the peak is used to determine the types of polymers.
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to modify the step c) to compare at least one of the temperatures determined in step c) with at least one corresponding temperature of the at least one reference parameter of said second database since it would allow to determine the corresponding polymer type(s) based on the occurrence of sharp peak at a specific temperature.
Note: Examiner interprets Claim 8 being dependent from claim 6 to provide the antecedent basis of the second database.
Claims 12-13 are rejected under 35 U.S.C. 103 as being unpatentable over David, Dümichen and Lafargue, as applied to claim 1 above, and further in view of Romero-Sarmiento et al. ( US20190107522A1).
Regarding claim 12, modified David teaches the method as claimed in claim 1, and is silent to wherein said first heating sequence in an inert atmosphere comprises at least the following step: from a temperature ranging between 100° C and 300° C, raising the temperature according to a temperature gradient ranging between 5 and 30° C/minute, up to a temperature ranging between 500° C and 650° C.
Romero-Sarmiento teaches a sample of sedimentary rock and a sample of total organic matter isolated from the rock are heated in a sequence under an inert atmosphere and quantities of hydrocarbon-containing compounds, CO and CO2 released by each sample are measured. The residue from each sample originating from heating under an inert atmosphere is subjected to a heating sequence under an oxidizing atmosphere, and quantities of CO and CO2 released by each residue are measured (abstract). Romero-Sarmiento further teaches the heating under an inert atmosphere comprising: a) starting heating from a first temperature between 50° C and 120° C, raising the temperature of the selected sample according to a first temperature gradient between 1 °C/min and 50 °C/min, up to a second temperature between 180 °C and 220 °C, and maintaining the selected sample at the second temperature for a first predetermined duration; b) starting heating from the second temperature, raising the temperature of the selected sample according to a second temperature gradient between 1 °C/min and 50 °C/min, up to a third temperature between 330 °C and 370 ° C, and maintaining the selected sample at the third temperature during a second predetermined duration; and c) starting heating from the third temperature by raising the temperature of the sample according to a third temperature gradient between 1 °C/min and 50 °C/min, up to a fourth temperature between 630 °C and 670 °C (claim 7). Thus, Romero-Sarmiento teaches wherein said first heating sequence in an inert atmosphere comprises at least the following step: from a temperature ranging between 50 °C and 120 °C, raising the temperature according to a temperature gradient ranging between 1 and 50 °C/minute, up to a temperature ranging between 630 °C and 670 °C.
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to perform the first heating sequence in the inert atmosphere comprising at least the following step: from a temperature ranging between 50 °C and 120 °C, raising the temperature according to a temperature gradient ranging between 1 and 50 °C/minute, up to a temperature ranging between 630 °C and 670 °C, as taught by Romero-Sarmiento, since Romero-Sarmiento the suitable temperature profile for heating the sample under an inert atmosphere (claim 7).
The disclosed initial temperature ranging between 50 °C and 120 °C overlaps the claimed temperature ranging between 100 °C and 300 °C; the disclosed temperature gradient ranging between 1 and 50 °C/minute overlap with the claimed temperature gradient ranging between 5 and 30° C/minute; and the disclosed final temperature ranging between 630 °C and 670 °C overlap with the claimed final temperature ranging between 500 °C and 650 °C.
It would have been obvious to have selected and utilized an initial temperature, temperature gradient, and final temperature in the disclosed temperature profile, as taught by Romero-Sarmiento, including those amounts that overlap within the claimed ranges, since one of ordinary skill in the art would reasonably expect any value within the taught range to be suitable given that Romero-Sarmiento specifically teaches the ranges to be suitable for the initial temperature, temperature gradient, and final temperature in the disclosed temperature profile for heating the sample under an inert atmosphere. It has been held that obviousness exists where the claimed ranges overlap or lie inside ranges disclosed by the prior art. See MPEP 2144.05 (I).
Regarding claim 13, modified David teaches the method as claimed in claim 1, and is silent to wherein said second heating sequence in an oxidizing atmosphere comprises at least the following step: from a temperature ranging between 200 °C and 400 °C, raising the temperature according to a temperature gradient ranging between 10 and 40 °C/minute, up to a temperature ranging between 750 °C and 950 °C.
Romero-Sarmiento teaches a sample of sedimentary rock and a sample of total organic matter isolated from the rock are heated in a sequence under an inert atmosphere and quantities of hydrocarbon-containing compounds, CO and CO2 released by each sample are measured. The residue from each sample originating from heating under an inert atmosphere is subjected to a heating sequence under an oxidizing atmosphere, and quantities of CO and CO2 released by each residue are measured (abstract). Romero-Sarmiento further teaches B. heating a residue of the sample originating from the first heating sequence according to a second heating sequence under an oxidizing atmosphere, wherein the heating sequence in step B starts from a temperature between 200° C and 400° C, and is raised according to a temperature gradient comprised between 20 and 40° C/minute, up to a temperature between 750 and 950° C (claims 1 and 3). Thus, Romero-Sarmiento teaches
wherein said second heating sequence in an oxidizing atmosphere comprises at least the following step: from a temperature ranging between 200° C and 400° C, raising the temperature according to a temperature gradient ranging between 20 and 40 °/minute, up to a temperature ranging between 750° C and 950° C.
It would have been obvious to one of ordinary skill in the art before the effective filing date of the claimed invention to perform the second heating sequence in the oxidizing atmosphere comprising at least the following step: from a temperature ranging between 200° C and 400° C, raising the temperature according to a temperature gradient ranging between 20 and 40 °/minute, up to a temperature ranging between 750° C and 950° C, as taught by Romero-Sarmiento, since Romero-Sarmiento the suitable temperature profile for heating the residue of the sample under an oxidizing atmosphere (claims 1 and 3).
Conclusion
The prior arts made of record and not relied upon are considered pertinent to applicant's disclosure: Goedecke et al. (Evaluation of thermoanalytical methods equipped with evolved gas analysis for the detection of microplastic in environmental samples, Journal of Analytical and Applied Pyrolysis, 2020, 152, 104961) teaches analysis of polymers PE, PP, PS and PET by the three TGA methods. Espitalie et al. (US5811308A) teaches a method for determining at least one petroleum characteristic of a geologic sediment sample heated in a non-oxidizing atmosphere and an oxidizing atmosphere.
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/SHIZHI QIAN/Examiner, Art Unit 1795
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