US5596196A
Expired / Lapsed
US
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Oxygenate analysis and control by Raman spectroscopy
Assignee: Marathon Petroleum Co LP
•
Filing: 1995-05-24
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Granted: 1997-01-21
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Expires: 2015-05-24
Abstract
Abstract Oxygenated hydrocarbons can be predicted within ±0.2% wt or better, using Raman NIR spectroscopy and multivariate analysis, with optional fiberoptics multistreaming. The resulting signal can be used to control concentration of such compounds in product to desired levels.
Inventors
- 👤 John B. Cooper
- 👤 Kent L. Wise
- 👤 William T. Welch
- 👤 Michael B. Sumner
Bibliographic Details
Application Number
—
Jurisdiction
US
Data Source
google_patents
Last Synchronized
2026-10-27 08:48
CPC Classifications
G; G01; G01N; G01N21/00; G01N21/62; G01N21/63; G01N21/65; G01N21/17; G01N21/25; G01N21/31; G01N21/35; G01N21/3577; G01N21/359; G01N2021/651; G01N2021/653; G01N2021/656; G01N21/658; G01N2201/00; G01N2201/12; G01N2201/129; G01N2201/1293
Claims Analysis
Total Claims: 44
Claim 1
Independent Claim
127 words
A process comprising: a) irradiating a sample of a liquid mixture consisting essentially of liquid hydrocarbons and comprising one or more oxygenated component to produce Raman scattered radiation emitted from the sample; b) collecting Raman scattered radiation emitted from the sample; c) dispersing or transforming the collected Raman scattered radiation from the sample into spectra with intensities corresponding to the concentration of components of the mixture; d) processing said spectra according to a regression model derived by multivariate analysis of Raman spectra, or a mathematical function of Raman spectra, of liquid mixtures containing known concentrations of one or more oxygenated hydrocarbons, to produce a control signal representative of the concentration of an oxygenated component in said mixture; e) controlling a process in response to said control signal.
Claim 2
Dependent Claim
127 words
A process comprising: a) irradiating a sample of a liquid mixture consisting essentially of liquid hydrocarbons and comprising one or more oxygenated component to produce Raman scattered radiation emitted from the sample; b) collecting Raman scattered radiation emitted from the sample; c) dispersing or transforming the collected Raman scattered radiation from the sample into spectra with intensities corresponding to the concentration of components of the mixture; d) processing said spectra according to a regression model derived by multivariate analysis of Raman spectra, or a mathematical function of Raman spectra, of liquid mixtures containing known concentrations of one or more oxygenated hydrocarbons, to produce a control signal representative of the concentration of an oxygenated component in said mixture; e) controlling a process in response to said control signal.
Claim 3
Dependent Claim
34 words
A process according to claim 1 wherein said oxygenated hydrocarbon comprises methanol and wherein said collected Raman scattered radiation from the sample is measured in the range of frown about 2964-2814 and/or 1477-1014 nm.
Claim 4
Dependent Claim
34 words
A process according to claim 1 wherein said oxygenated hydrocarbon comprises 1-propanol and wherein said collected Raman scattered radiation from the sample is measured in the range of from about 2958-2858 and/or 1477-446 nm.
Claim 5
Dependent Claim
34 words
A process according to claim 1 whereto said oxygenated hydrocarbon comprises 2-propanol and whereto said collected Raman scattered radiation from the sample is measured in the range of from about 2995-2860 and/or 1473-800 nm.
Claim 6
Dependent Claim
34 words
A process according to claim 1 wherein said oxygenated hydrocarbon comprises 1-butanol and wherein said collected Raman scattered radiation from the sample is measured in the range of from about 2961-2859 and/or 1475-382 nm.
Claim 7
Dependent Claim
34 words
A process according to claim 1 whereto said oxygenated hydrocarbon comprises 2-butanol and wherein said collected Raman scattered radiation from the sample is measured in the range of from about 2990-2861 and/or 1477-481 nm.
Claim 8
Dependent Claim
34 words
A process according to claim 1 wherein said oxygenated hydrocarbon comprises isobutanol and wherein said collected Raman scattered radiation from the sample is measured in the range of from about 2995-2860 and/or 1473-800 nm.
Claim 9
Dependent Claim
36 words
A process according to claim 1 wherein said oxygenated hydrocarbon comprises tertiary butyl alcohol and wherein said collected Raman scattered radiation from the sample is measured in the range of from about 3000-2898 and/or 1470-320 nm.
Claim 10
Dependent Claim
35 words
A process according to 1 wherein said oxygenated hydrocarbon comprises tertiary amyl alcohol and wherein said collected Raman scattered radiation from the sample is measured in the range of from about 3000-2690 and/or 1470-320 nm.
Claim 11
Dependent Claim
35 words
A process according to 1 wherein said oxygenated hydrocarbon comprises tertiary amyl alcohol and wherein said collected Raman scattered radiation from the sample is measured in the range of from about 3000-2690 and/or 1470-320 nm.
Claim 12
Dependent Claim
38 words
A process according to claim 1 wherein said oxygenated hydrocarbon comprises methyl tertiary butyl ether (MTBE) and wherein said collected Raman scattered radiation from the sample is measured in the range of from about 3011-2791 and/or 892-466 nm.
Claim 13
Dependent Claim
38 words
A process according to claim 1 wherein said oxygenated hydrocarbon comprises ethyl tertiary butyl ether (ETBE) and wherein said collected Raman scattered radiation from the sample is measured in the range of from about 3011-2791 and/or 892-466 nm.
Claim 14
Dependent Claim
38 words
A process according to claim 1 wherein said oxygenated hydrocarbon comprises tertiary amyl methyl ether (TAME) and wherein said collected Raman scattered radiation from the sample is measured in the range of from about 3011-2791 and/or 892-466 nm.
Claim 15
Dependent Claim
36 words
A process according to claim 1 wherein said oxygenated hydrocarbon comprises diisopropyl ether (DIPE) and wherein said collected Raman scattered radiation from the sample is measured in the range of frown about 2995-2860 and/or 1473-800 nm.
Claim 16
Dependent Claim
146 words
A process comprising: a) irradiating a sample of a liquid mixture comprising as oxygenated component methanol, 1-propanol, 2-propanol, 1-butanol, 2-butanol, isobutanol, tertiary butanol, tertiary amyl alcohol, methyl tertiary butyl ether (MTBE), ethyl tertiary butyl ether (ETBE), tertiary amyl methyl ether (TAME), and/or diisopropyl ether (DIPE) to produce Raman scattered radiation emitted from the sample; b) collecting Raman scattered radiation emitted from the sample; c) dispersing or transforming the collected Raman scattered radiation from the sample into spectra with intensities corresponding to the concentration of said components; d) processing said spectra according to a regression model derived by multivariate analysis of Raman spectra, or derived from a mathematical function of Raman spectra, of liquid mixtures containing known concentrations of oxygenated hydrocarbons, to produce a control signal representative of the concentration of the oxygenated component in said mixture; e) controlling a process in response to said control signal.
Claim 17
Dependent Claim
146 words
A process comprising: a) irradiating a sample of a liquid mixture comprising as oxygenated component methanol, 1-propanol, 2-propanol, 1-butanol, 2-butanol, isobutanol, tertiary butanol, tertiary amyl alcohol, methyl tertiary butyl ether (MTBE), ethyl tertiary butyl ether (ETBE), tertiary amyl methyl ether (TAME), and/or diisopropyl ether (DIPE) to produce Raman scattered radiation emitted from the sample; b) collecting Raman scattered radiation emitted from the sample; c) dispersing or transforming the collected Raman scattered radiation from the sample into spectra with intensities corresponding to the concentration of said components; d) processing said spectra according to a regression model derived by multivariate analysis of Raman spectra, or derived from a mathematical function of Raman spectra, of liquid mixtures containing known concentrations of oxygenated hydrocarbons, to produce a control signal representative of the concentration of the oxygenated component in said mixture; e) controlling a process in response to said control signal.
Claim 18
Dependent Claim
13 words
The process of claim 14 wherein the liquid mixture is a hydrocarbon mixture.
Claim 19
Dependent Claim
14 words
The process of claim 14 wherein the sample is irradiated with near infrared radiation.
Claim 20
Dependent Claim
10 words
The process of claim 14 wherein the sample comprises methanol.
Claim 21
Dependent Claim
10 words
The process of claim 14 wherein the sample comprises 1-propanol.
Claim 22
Dependent Claim
10 words
The process of claim 14 wherein the sample comprises 2-propanol.
Claim 23
Dependent Claim
10 words
The process of claim 14 wherein the sample comprises 1-butanol.
Claim 24
Dependent Claim
10 words
The process of claim 14 wherein the sample comprises 2-butanol.
Claim 25
Dependent Claim
10 words
The process of claim 14 wherein the sample comprises isobutanol.
Claim 26
Dependent Claim
12 words
The process of claim 14 wherein the sample comprises tertiary butyl alcohol.
Claim 27
Dependent Claim
12 words
The process of claim 14 wherein the sample comprises tertiary amyl alcohol.
Claim 28
Dependent Claim
11 words
The process of claim 14 wherein said mixture comprises an alcohol.
Claim 29
Dependent Claim
199 words
A process according to claim 25 for determining the concentration of one or more alcohols or ethers in a liquid sample consisting essentially of hydrocarbons and said alcohols and/or said ethers, said process comprising: a) irradiating the liquid sample with radiation from a near infrared source to produce Raman scattered radiation emitted from said sample; b) collecting Raman scattered radiation emitted from the sample; c) transferring collected Raman scattered radiation and dispersing or transforming the collected Raman scattered radiation from the sample into spectra with intensities corresponding to the chemical composition of the components of said sample and concentrations of said components; d) processing said spectra according to a regression model derived by multivariate analysis of Raman spectra, or derived from a mathematical function of Raman spectra, of liquid mixtures containing known concentrations of alcohols and ethers, wherein the near infrared radiation source wavelength irradiating said sample is the same as, or correlated to, that employed in establishing said regression model; e) determining the concentration of at least one alcohol or ether present by processing the spectral intensities according to said model and producing a control signal representative of the concentration of an alcohol and/or ether in said mixture.
Claim 30
Dependent Claim
43 words
A process according to claim 26 wherein said determining of the concentration comprises emitting a signal indicative of said concentration and wherein said signal is transmitted to a means for controlling a process for producing a product comprising said alcohol or said ether.
Claim 31
Dependent Claim
28 words
A process according to claim 26 wherein the intensities corresponding to the chemical composition of components are determined at wave numbers comprising 3300-2250 and/or 1900-175 cm -1 .
Claim 32
Dependent Claim
11 words
The process of claim 14 wherein said mixture comprises an ether.
Claim 33
Dependent Claim
31 words
A process according to claim 14 wherein said multivariate analysis is accomplished by mathematical manipulation comprising neural network partial least squares (PLS), principal component regression (PCR), and/or multiple linear regression (MLR).
Claim 34
Dependent Claim
21 words
A process according to claim 14 wherein said regression model is derived by methods comprising Raman intensity differences and/or spectral subtraction.
Claim 35
Dependent Claim
14 words
A process according to claim 14 wherein said mixture comprises a synthetic fuel mixture.
Claim 36
Dependent Claim
20 words
A process according to claim 14 wherein said control signal is used in a feed-forward or a feed-back control apparatus.
Claim 37
Dependent Claim
25 words
A process according to claim 14 wherein said Raman scattered radiation is collected from regions comprising the fingerprint (FP) region or the CH stretching region.
Claim 38
Dependent Claim
17 words
A process according to claim 14 wherein transforming said collected Raman scattered radiation is by FT Raman.
Claim 39
Dependent Claim
165 words
A process comprising: a) irradiating a sample of a liquid mixture comprising hydrocarbons and further comprising as oxygenated hydrocarbon methanol, ethanol, 1-propanol, 2-propanol, 1-butanol, 2-butanol, isobutanol, tertiary butanol, tertiary amyl alcohol, methyl tertiary butyl ether (MTBE), ethyl tertiary butyl ether (ETBE), tertiary amyl methyl ether (TAME), and/or diisopropyl ether (DIPE) with near infrared radiation, producing Raman scattered radiation emitted from the sample; b) collecting Raman scattered radiation emitted from the sample; c) dispersing or transforming the collected Raman scattered radiation from the sample into spectra with intensities corresponding to the chemical composition of the components of the mixture of said sample and concentration of said components; d) processing said spectra according to a regression model derived by multivariate analysis of Raman spectra, or derived from a mathematical function of Raman spectra, of liquid mixtures containing known concentrations of oxygenated hydrocarbons, to produce a control signal representative of the concentration of oxygenated hydrocarbon in said mixture; e) controlling a process in response to said control signal.
Claim 40
Dependent Claim
165 words
A process comprising: a) irradiating a sample of a liquid mixture comprising hydrocarbons and further comprising as oxygenated hydrocarbon methanol, ethanol, 1-propanol, 2-propanol, 1-butanol, 2-butanol, isobutanol, tertiary butanol, tertiary amyl alcohol, methyl tertiary butyl ether (MTBE), ethyl tertiary butyl ether (ETBE), tertiary amyl methyl ether (TAME), and/or diisopropyl ether (DIPE) with near infrared radiation, producing Raman scattered radiation emitted from the sample; b) collecting Raman scattered radiation emitted from the sample; c) dispersing or transforming the collected Raman scattered radiation from the sample into spectra with intensities corresponding to the chemical composition of the components of the mixture of said sample and concentration of said components; d) processing said spectra according to a regression model derived by multivariate analysis of Raman spectra, or derived from a mathematical function of Raman spectra, of liquid mixtures containing known concentrations of oxygenated hydrocarbons, to produce a control signal representative of the concentration of oxygenated hydrocarbon in said mixture; e) controlling a process in response to said control signal.
Claim 41
Dependent Claim
13 words
The process of claim 36 wherein the liquid mixture is a hydrocarbon mixture.
Claim 42
Independent Claim
147 words
An apparatus for the control of a process comprising in combination: a) irradiating means for irradiating a sample of a liquid mixture comprising at least one oxygenated hydrocarbon to produce scattered radiation emitted from the sample; b) Raman scattered radiation collecting means for collecting said Raman scattered radiation; c) mathematical manipulation means for dispersing or transforming the collected Raman scattered radiation into spectra with intensities corresponding to the concentration of components of the mixture; d) processing means liar processing said spectra according to a regression model derived by multivariate analysis of Raman spectra or mathematical function thereof, of liquid mixtures containing known concentrations of oxygenated hydrocarbons; e) control signal generation means for producing a control signal representative of the concentration in said mixture of one or more of said oxygenated hydrocarbons; f) control means responsive to said signal for controlling a process in response to said signal.
Claim 43
Independent Claim
147 words
An apparatus for the control of a process comprising in combination: a) irradiating means for irradiating a sample of a liquid mixture comprising at least one oxygenated hydrocarbon to produce scattered radiation emitted from the sample; b) Raman scattered radiation collecting means for collecting said Raman scattered radiation; c) mathematical manipulation means for dispersing or transforming the collected Raman scattered radiation into spectra with intensities corresponding to the concentration of components of the mixture; d) processing means liar processing said spectra according to a regression model derived by multivariate analysis of Raman spectra or mathematical function thereof, of liquid mixtures containing known concentrations of oxygenated hydrocarbons; e) control signal generation means for producing a control signal representative of the concentration in said mixture of one or more of said oxygenated hydrocarbons; f) control means responsive to said signal for controlling a process in response to said signal.
Claim 44
Dependent Claim
49 words
An apparatus according to claim 38 wherein said control means comprises means for controlling the quantity of at least one component being delivered to a blending zone in which fuels are blended to produce a finished fuel blend having a preset desired concentration of at least one oxygenated hydrocarbon.
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USPTO Annuity & Maintenance Windows
| Annuity Stage | Window Opens | Payment Deadline | Surcharge Period Until | Estimated Fee | Status |
|---|---|---|---|---|---|
| 3.5 Years (Year 4) | 2000-01-21 | 2000-07-22 | 2001-01-21 | $2000.00 | Window Closed / Lapsed |
| 7.5 Years (Year 8) | 2004-01-21 | 2004-07-22 | 2005-01-21 | $3760.00 | Window Closed / Lapsed |
| 11.5 Years (Year 12) | 2008-01-21 | 2008-07-22 | 2009-01-21 | $7700.00 | Window Closed / Lapsed |