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US2909482A - Determination of asphaltic components of petroleum - Google Patents

Determination of asphaltic components of petroleum Download PDF

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US2909482A
US2909482A US696362A US69636257A US2909482A US 2909482 A US2909482 A US 2909482A US 696362 A US696362 A US 696362A US 69636257 A US69636257 A US 69636257A US 2909482 A US2909482 A US 2909482A
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sample
asphaltic
treating
hydrocarbon
asphaltenes
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Rollie B Williams
Rhoderick K Saunders
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ExxonMobil Technology and Engineering Co
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Exxon Research and Engineering Co
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    • GPHYSICS
    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N24/00Investigating or analyzing materials by the use of nuclear magnetic resonance, electron paramagnetic resonance or other spin effects
    • G01N24/10Investigating or analyzing materials by the use of nuclear magnetic resonance, electron paramagnetic resonance or other spin effects by using electron paramagnetic resonance
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10STECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10S208/00Mineral oils: processes and products
    • Y10S208/01Automatic control

Definitions

  • This invention relates to" a method for determining the quantity oflasphaltene type hydrocarbons contained in a sira ble feed components for many hydrocarbon treating processes; such asfhydrocarbon cracking processes, and therefore are desirably excluded from the feed stock by suitable means such as fractional distillation, deasphalting, etc.
  • Asphaltic hydrocarbon components tend to be insoluble in light hydrocarbon fractions such as paraflinic naphtha fractions and therefore as'phaltene hydrocarbon determinations are normally made on the basis of time-consuming solubility tests.
  • a continuous processjfor the treatmentof-an as: phaltenes-containing petroleum hydrocarbonfraction is regulated by periodically or continuouslys'ampling a treat ing process hydrocarbon stream 'by determining the as phaltenes content of such samples and by continuously regulating a treating process: variable in response to such determination.
  • the present invention -Will.be' further illustrated by the following specific examples and by the. accompanying drawings which are given by yvay of illustration and which are not intended as limitations on the scope of the invention.
  • FIG. 1 is a graph showing the interrelationship of electron paramagnetic resonance signal intensity, with respect to asphaltenes content, as. demonstrated by the data of Example I; and p j Fig. 2 is a schematic diagram indicating onemanner in which a process for treating an asphaltic hydrocarbon may be regulated in accordance withthegpresentyinven tion 7 V f EXAMPLE I
  • a plurality of deasphalted oil samples and residuum petroleumsamples were subjected to electron paramagnetic resonance spectroscopic analysis on a spectrometer operated at a frequency of about 9200, megacycles at a magnetic field strength of about 3.000 gauss.
  • the samples were contained in thin cylindrical glass tubes of about 5 mm. outside diameter.,
  • the samples tested and the re; sults obtained are set forth in Table I. Theresults are further graphically presentedin Fig. 1;.
  • Treating zone 10 may be, for example, a solvent deasphalting zone for deasphalting an asphaltic hydro,- carbonfeed stock with a solvent such as a liquefied normally gaseous hydrocarbon, liquefied sulfur dioxide, etc.
  • a deasphalted oil suitable for catalytic cracking a distillation zone for separating an asphaltenes-free distillate fraction from an asphaltic feed stock, a blending zone wherein an asphaltic hydrocarbon fraction derived from a petroleum refining process (e.g., catalytic cracking, distillation, etc.) is blended with a non-asphaltic fuel oil fraction to provide a furnace fuel, etc.
  • a petroleum refining process e.g., catalytic cracking, distillation, etc.
  • An asphaltenes-containing hydrocarbon feed stock is charged to the treating zone 10 by way of a charge line 12 regulated by suitable means such as an electrically or pneumatically actuatable valve 14.
  • suitable means such as an electrically or pneumatically actuatable valve 14.
  • a treating proc ess product stream is discharged from the zone 10 by way of a line 16.” It will be understood that in many processes a plurality of discharge streams (not shown) may be discharged from the treating zone 10.
  • the product stream 16 is sequentially sampled (on an intermittent or continuous basis) by way of a sample line 18 controlled by a valve 20 leading to an analysis zone 22.
  • a suitable solvent may be blended with the sample in the line 18, the solvent being charged by way of a line 24 controlled by a valve 26.
  • the sample material after analysis, may be discharged from the analysis zone by way of the discharge line 30 controlled by a valve 32 for discharge from the system or alternately, for example, may be returned to the'discharge line 16 by way of a line 34 controlled by a valve 36.
  • the electron paramagnetic resonance absorptivity of the samples is measured in the zone 22 and a signal constituting a measurement of asphaltenes content is obtained which is transmitted by way of a lead 28 to a suitable process variable control means such as the actuating means for the value 14. If the intensity of the signal. transmitted through'the lead 26 falls outside of a predetermined signal intensity range, the setting of the valve 14 will be changed by actuating of thecontrol means to thereby provide for the desired treating conditions in the zone 10.
  • the treating zone 10 may be a deasphalting zone wherein a hydrocarbon residuum fraction is treated with a liquefied normally gaseous hydrocarbon solvent under conditions of temperature, contact time, and solvent-to-oil ratio sufiicien-t to provide for the obtaining of a deasphalted oil fraction suitable for catalytic cracking and an asphalt fraction.
  • a typical solvent deasphalting operation it may be desirable to regulate deasphalting operations in a manner to provide for the presence of from about 0.1 to 1 weight percent of asphaltenes in the deasphalted oil, this being done in order to insure the recovery of a maximized amount of useful non-asphaltic components or to exclude a maximized amount of asphaltic components.
  • the asphaltenes content of the discharge stream 16 is sequentially determined (ona continuous or intermittent basis) and if the asphaltenes content falls either above or below the predetermined range, a deasphalting process variable may be altered in response to determination to provide for the desired asphaltenes content.
  • the deasphalting process variables that may be regulated are solvent-to-feed stock ratio, temperature, solvent composition, etc.
  • a method for determining the asphaltenes content of an asphaltic petroleum hydrocarbon sample which comprises measuring the electron paramagnetic resonance absorptivity of said sample to thereby obtain a measurement of the asphaltenes content of said sample.
  • a method 'for determining the asphaltenes content of an asphaltic hydrocarbon sample which comprises dissolving said sample in a non-ionic organic solvent and then measuring the electron paramagnetic resonance absorptivity of said sample to thereby obtain a measurement of the asphaltenes content of said sample.
  • the improved method for regulating said treating process which comprises the steps of sequentially sampling a treating process stream, sequentially measuring the electron paramagnetic resonance absorptivity of the thus-obtained samples under predetermined analysis conditions and controlling a hydrocarbon treating process variable in response to said measurement.
  • the improved method for regulating said deasphalting operation which comprises the steps of sequentially sampling said deasphalted oil fraction, sequentially subjecting said samples to electron paramagnetic resonance spectroscopic analysis to obtain an electrical signal constituting a measurement of the asphaltenes con tent of said samples and electrically regulating a deasphalting process variable in response to said signal.

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  • Physics & Mathematics (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Health & Medical Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Chemical & Material Sciences (AREA)
  • Analytical Chemistry (AREA)
  • Biochemistry (AREA)
  • General Health & Medical Sciences (AREA)
  • General Physics & Mathematics (AREA)
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  • Pathology (AREA)
  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)

Description

Oct. 20, 1959 R. B. WILLIAMS ETAL 2,909,432
DETERMINATION OF ASPHALTIC COMPONENTS OF PETROLEUM Filed Nov. 14. 1957 CORRELATION BETWEEN ASPHALTENES- CONTENT AND PARA MAGNETIC RESONANCE I' ABSORPTIVITY OF RESIDUA FRACTIONS. I 50 I E Z n I; J g
(I) El Ill 2 50 2 O In Ill 1 2 2o 0 U 2 0 2 Io 0 I0 20 3o 40 so so ASPHALTENES CONTENT,WEIGHT PERCENT.
FIG. I.
I I4 L TREATING '7 i ZONE I I 20 v V 1 l H 36 7+ I I I 22 I 2 I ANALYSIS ZONE SOLVENT i FOR DETERMINING Z ASPHALTENES 32 3o CONTENT I l i A I z I g INVENTORS. 4 FIG 2 ROLLIE B. WILLIAMS,
RHODERICK K. SAUNDERS,
ATTORNEY.
United States Patent" 071cc DETERMINATION or ASPHALTIC COMPONENTS p PETROLEUM Rollie B. Williams and Rhoderi ck K. Saunders, Baytown,
Tex'., assignors, by mesne assignments, to Esso Research and Engineering Company, Elizabeth, N.J.,'a corporation of Delaware p ApplicationNovemberM, 1957, Serial No. 696,362
6 Claims. l. 208-309) This invention relates to" a method for determining the quantity oflasphaltene type hydrocarbons contained in a sira ble feed components for many hydrocarbon treating processes; such asfhydrocarbon cracking processes, and therefore are desirably excluded from the feed stock by suitable means such as fractional distillation, deasphalting, etc.
' Asphaltic hydrocarbon components tend to be insoluble in light hydrocarbon fractions such as paraflinic naphtha fractions and therefore as'phaltene hydrocarbon determinations are normally made on the basis of time-consuming solubility tests. j p
It has been discovered in accordance with the present invention that when an asphaltenes-containin'g petroleum hydrocarbon sample is subjected to electron paramagnetic resonance spectroscopic analysis, there is obtained a sig nal having an intensity responsive to the quantity of asphal-tene components in the sample. The electron paramagnetic resonance spectroscopic determination of the present invention iseasily conducted with electron paramagnetic resonance spectrometers of conventional con- 2,909,482 I Pate e 9 tion is made under standardized predetermined operating conditions with a spectrometer of predetermined standardized construction whereby the intensity of the signalthat is obtained provides a direct quantitative determination of the asphaltenes content of the. samples The determinaa tion may be made while the sampleis in a solid, semi-solid, or liquid condition. It is preferable to dilute the. asphaltenes-containing sample with an amount ,of a. low boiling solvent suflicient to provide a solution containing. a predetermined amount of sample, such amount preferably being less than about 10% by volume. 1 I
In accordance with a preferred form of the present in.- vention, a continuous processjfor the treatmentof-an as: phaltenes-containing petroleum hydrocarbonfraction is regulated by periodically or continuouslys'ampling a treat ing process hydrocarbon stream 'by determining the as phaltenes content of such samples and by continuously regulating a treating process: variable in response to such determination. 1 The present invention -Will.be' further illustrated by the following specific examples and by the. accompanying drawings which are given by yvay of illustration and which are not intended as limitations on the scope of the invention.
In the drawingsy e 7 ;-j Fig. 1 is a graph showing the interrelationship of electron paramagnetic resonance signal intensity, with respect to asphaltenes content, as. demonstrated by the data of Example I; and p j Fig. 2 is a schematic diagram indicating onemanner in which a process for treating an asphaltic hydrocarbon may be regulated in accordance withthegpresentyinven tion 7 V f EXAMPLE I A plurality of deasphalted oil samples and residuum petroleumsamples were subjected to electron paramagnetic resonance spectroscopic analysis on a spectrometer operated at a frequency of about 9200, megacycles at a magnetic field strength of about 3.000 gauss. The samples were contained in thin cylindrical glass tubes of about 5 mm. outside diameter., The samples tested and the re; sults obtained are set forth in Table I. Theresults are further graphically presentedin Fig. 1;. I
. p Table I ELECTRON PARAMAGNETIC RESONANCE "DETERMINATIONS OF ASPHALTENES I CONTENT H Ooncentra- Aspha1- tion of Peak Height Adjusted 2 Sample tenes Sample 111 Prior to Relative Peak 'Absorp No. Nature of Sample Content, Sample Adjustment Attend Height ..tivity Tube, (Chart Div.) 48171011 (Chart Percent 1 GmsJom Div.) Length West Texas Re- 6. 87 0. 1109 16. 0 3. 8 60. 8 548 sidiuum.
Deasphalted 0il.-.- 0.08 0. 1132 1. 3 1.0 1. 3 11 -do 0.00 0.1179 2.1 1.0 2.1 18 Asphalt... 20. 6 0. 0717 36. 3 3. 8 137. 9 1, 923 Deasphalt 2. 9 0. 1156 39. 5 1. 0 39. 5 342 Asphalt 59. 8 0. 0801 27. 7 17. 483. 4 6, 035
1 By standard solubility test.
2 Adjusted peak height= original peak heightxattenuation.
5 Absorptivity= Adjusted peak height Concentration From Table I and Fig. 1, it is seen that there is a correlation between electron paramagnetic resonance signal intensity and asphaltenes content whereby a direct quantitative measurement of asphaltenes content may be made.
The manner in which a petroleum hydrocarbon treating process may be regulated in accordance with the present invention is illustrated with reference to Fig. 2.
Turning next to Fig. 2, there is shown a treating zone for treating an asphaltic petroleum hydrocarbon fraction. Treating zone 10 may be, for example, a solvent deasphalting zone for deasphalting an asphaltic hydro,- carbonfeed stock with a solvent such as a liquefied normally gaseous hydrocarbon, liquefied sulfur dioxide, etc. to obtain a deasphalted oil suitable for catalytic cracking, a distillation zone for separating an asphaltenes-free distillate fraction from an asphaltic feed stock, a blending zone wherein an asphaltic hydrocarbon fraction derived from a petroleum refining process (e.g., catalytic cracking, distillation, etc.) is blended with a non-asphaltic fuel oil fraction to provide a furnace fuel, etc.
An asphaltenes-containing hydrocarbon feed stock is charged to the treating zone 10 by way of a charge line 12 regulated by suitable means such as an electrically or pneumatically actuatable valve 14. Although only a single charge line for the treating zone 10 is shown in Fig. 2, it will be understood that in practice one or a plurality of charge streams may be charged to the treating zone 10, depending upon the particular treating process to be conducted therein. A treating proc ess product stream is discharged from the zone 10 by way of a line 16." It will be understood that in many processes a plurality of discharge streams (not shown) may be discharged from the treating zone 10.
In accordance with the present invention, the product stream 16 is sequentially sampled (on an intermittent or continuous basis) by way of a sample line 18 controlled by a valve 20 leading to an analysis zone 22. If desired, a suitable solvent may be blended with the sample in the line 18, the solvent being charged by way of a line 24 controlled by a valve 26.
The sample material, after analysis, may be discharged from the analysis zone by way of the discharge line 30 controlled by a valve 32 for discharge from the system or alternately, for example, may be returned to the'discharge line 16 by way of a line 34 controlled by a valve 36.
The electron paramagnetic resonance absorptivity of the samples is measured in the zone 22 and a signal constituting a measurement of asphaltenes content is obtained which is transmitted by way of a lead 28 to a suitable process variable control means such as the actuating means for the value 14. If the intensity of the signal. transmitted through'the lead 26 falls outside of a predetermined signal intensity range, the setting of the valve 14 will be changed by actuating of thecontrol means to thereby provide for the desired treating conditions in the zone 10.
As a specific example, the treating zone 10 may be a deasphalting zone wherein a hydrocarbon residuum fraction is treated with a liquefied normally gaseous hydrocarbon solvent under conditions of temperature, contact time, and solvent-to-oil ratio sufiicien-t to provide for the obtaining of a deasphalted oil fraction suitable for catalytic cracking and an asphalt fraction.
In a typical solvent deasphalting operation it may be desirable to regulate deasphalting operations in a manner to provide for the presence of from about 0.1 to 1 weight percent of asphaltenes in the deasphalted oil, this being done in order to insure the recovery of a maximized amount of useful non-asphaltic components or to exclude a maximized amount of asphaltic components. In this situation, the asphaltenes content of the discharge stream 16 is sequentially determined (ona continuous or intermittent basis) and if the asphaltenes content falls either above or below the predetermined range, a deasphalting process variable may be altered in response to determination to provide for the desired asphaltenes content. Among the deasphalting process variables that may be regulated are solvent-to-feed stock ratio, temperature, solvent composition, etc.
Having described our invention, what is claimed is:
1. A method for determining the asphaltenes content of an asphaltic petroleum hydrocarbon sample which comprises measuring the electron paramagnetic resonance absorptivity of said sample to thereby obtain a measurement of the asphaltenes content of said sample.
2. A method 'for determining the asphaltenes content of an asphaltic hydrocarbon sample which comprises dissolving said sample in a non-ionic organic solvent and then measuring the electron paramagnetic resonance absorptivity of said sample to thereby obtain a measurement of the asphaltenes content of said sample.
3. In a process for continuously treating an asphaltic hydrocarbon feed stock, the improved method for regulating said treating process which comprises the steps of sequentially sampling a treating process stream, sequentially measuring the electron paramagnetic resonance absorptivity of the thus-obtained samples under predetermined analysis conditions and controlling a hydrocarbon treating process variable in response to said measurement.
4. A process as in claim 3 wherein the treating process is a solvent deasphalting process. v
5. In a process wherein an asphaltic petroleum hydrocarbon feed stock is deasphalted by contact with a liquefied normally gaseous hydrocarbon to separate said feed stock into an asphaltic fraction and a deasphalted oil fraction, the improved method for regulating said deasphalting operation which comprises the steps of sequentially sampling said deasphalted oil fraction, sequentially subjecting said samples to electron paramagnetic resonance spectroscopic analysis to obtain an electrical signal constituting a measurement of the asphaltenes con tent of said samples and electrically regulating a deasphalting process variable in response to said signal.
6. A process as in claim 5 wherein the ratio of liquefied normally gaseous hydrocarbon to asphaltic feed stock is regulated in response to the signal.
Alway et al. Oct. 26, 1954 Kirshenbaum Oct. 2, 1956

Claims (1)

1. A METHOD FOR DETERMINING THE ASPHALTENES CONTENT OF AN ASPHALTIC PETROLEUM HYDROCARBON SAMPLE WHICH COMPRISES MEASURING THE ELECTRON PARAMAGNETIC RESONANCE ABSORPTIVITY OF SAID SAMPLE TO THEREBY OBTAIN A MEASUREMENT OF THE ASPHALTENES CONTENT OF SAID SAMPLE.
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Cited By (21)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3087888A (en) * 1960-06-15 1963-04-30 Gulf Research Development Co Determination of vanadium content of hydrocarbon oils by electron paramagnetic resonance spectrometry
US4440633A (en) * 1981-04-30 1984-04-03 Institut Francais Du Petrole Process for solvent deasphalting heavy hydrocarbon fractions
US4777140A (en) * 1987-05-26 1988-10-11 Mobil Oil Corporation Measurement of vanadium content in a refinery stream by electron spin resonance spectroscopy
US11702600B2 (en) 2021-02-25 2023-07-18 Marathon Petroleum Company Lp Assemblies and methods for enhancing fluid catalytic cracking (FCC) processes during the FCC process using spectroscopic analyzers
US11802257B2 (en) 2022-01-31 2023-10-31 Marathon Petroleum Company Lp Systems and methods for reducing rendered fats pour point
US11835450B2 (en) 2021-02-25 2023-12-05 Marathon Petroleum Company Lp Methods and assemblies for determining and using standardized spectral responses for calibration of spectroscopic analyzers
US11891581B2 (en) 2017-09-29 2024-02-06 Marathon Petroleum Company Lp Tower bottoms coke catching device
US11898109B2 (en) 2021-02-25 2024-02-13 Marathon Petroleum Company Lp Assemblies and methods for enhancing control of hydrotreating and fluid catalytic cracking (FCC) processes using spectroscopic analyzers
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US11905479B2 (en) 2020-02-19 2024-02-20 Marathon Petroleum Company Lp Low sulfur fuel oil blends for stability enhancement and associated methods
US11970664B2 (en) 2021-10-10 2024-04-30 Marathon Petroleum Company Lp Methods and systems for enhancing processing of hydrocarbons in a fluid catalytic cracking unit using a renewable additive
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US12306076B2 (en) 2023-05-12 2025-05-20 Marathon Petroleum Company Lp Systems, apparatuses, and methods for sample cylinder inspection, pressurization, and sample disposal
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US12473500B2 (en) 2021-02-25 2025-11-18 Marathon Petroleum Company Lp Assemblies and methods for enhancing control of fluid catalytic cracking (FCC) processes using spectroscopic analyzers
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Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2692820A (en) * 1950-10-28 1954-10-26 Upjohn Co Method and means for effecting automatic fractionation
US2765330A (en) * 1952-07-30 1956-10-02 Exxon Research Engineering Co Magnetic control of chemical reactions

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2692820A (en) * 1950-10-28 1954-10-26 Upjohn Co Method and means for effecting automatic fractionation
US2765330A (en) * 1952-07-30 1956-10-02 Exxon Research Engineering Co Magnetic control of chemical reactions

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US3087888A (en) * 1960-06-15 1963-04-30 Gulf Research Development Co Determination of vanadium content of hydrocarbon oils by electron paramagnetic resonance spectrometry
US4440633A (en) * 1981-04-30 1984-04-03 Institut Francais Du Petrole Process for solvent deasphalting heavy hydrocarbon fractions
US4777140A (en) * 1987-05-26 1988-10-11 Mobil Oil Corporation Measurement of vanadium content in a refinery stream by electron spin resonance spectroscopy
US11891581B2 (en) 2017-09-29 2024-02-06 Marathon Petroleum Company Lp Tower bottoms coke catching device
US12000720B2 (en) 2018-09-10 2024-06-04 Marathon Petroleum Company Lp Product inventory monitoring
US12031676B2 (en) 2019-03-25 2024-07-09 Marathon Petroleum Company Lp Insulation securement system and associated methods
US11975316B2 (en) 2019-05-09 2024-05-07 Marathon Petroleum Company Lp Methods and reforming systems for re-dispersing platinum on reforming catalyst
US12345416B2 (en) 2019-05-30 2025-07-01 Marathon Petroleum Company Lp Methods and systems for minimizing NOx and CO emissions in natural draft heaters
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