CN116931117A - Method for dividing oil field water/gas field water source by sulfur isotopes - Google Patents
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- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 title claims abstract description 146
- 229910052717 sulfur Inorganic materials 0.000 title claims abstract description 144
- 239000011593 sulfur Substances 0.000 title claims abstract description 144
- 239000002332 oil field water Substances 0.000 title claims abstract description 126
- 238000000034 method Methods 0.000 title claims abstract description 25
- 239000003672 gas field water Substances 0.000 title claims description 37
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 78
- 239000013535 sea water Substances 0.000 claims description 40
- 229910052602 gypsum Inorganic materials 0.000 claims description 36
- 239000010440 gypsum Substances 0.000 claims description 36
- 230000015572 biosynthetic process Effects 0.000 claims description 30
- 238000005755 formation reaction Methods 0.000 claims description 30
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 claims description 26
- TZCXTZWJZNENPQ-UHFFFAOYSA-L barium sulfate Chemical compound [Ba+2].[O-]S([O-])(=O)=O TZCXTZWJZNENPQ-UHFFFAOYSA-L 0.000 claims description 21
- 230000008021 deposition Effects 0.000 claims description 15
- 229910052925 anhydrite Inorganic materials 0.000 claims description 14
- OSGAYBCDTDRGGQ-UHFFFAOYSA-L calcium sulfate Chemical compound [Ca+2].[O-]S([O-])(=O)=O OSGAYBCDTDRGGQ-UHFFFAOYSA-L 0.000 claims description 14
- 239000013505 freshwater Substances 0.000 claims description 10
- 239000002244 precipitate Substances 0.000 claims description 10
- 229910052601 baryte Inorganic materials 0.000 claims description 7
- 239000010428 baryte Substances 0.000 claims description 7
- 238000005520 cutting process Methods 0.000 claims description 6
- 229910021653 sulphate ion Inorganic materials 0.000 claims description 5
- 238000000638 solvent extraction Methods 0.000 claims description 4
- 239000005864 Sulphur Substances 0.000 claims description 3
- -1 sulphate ions Chemical class 0.000 claims description 3
- 238000011160 research Methods 0.000 abstract description 9
- 239000007789 gas Substances 0.000 description 38
- 238000000151 deposition Methods 0.000 description 13
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 12
- 239000000243 solution Substances 0.000 description 11
- 238000005070 sampling Methods 0.000 description 10
- 238000004458 analytical method Methods 0.000 description 9
- 239000011435 rock Substances 0.000 description 7
- 239000000203 mixture Substances 0.000 description 6
- 239000012267 brine Substances 0.000 description 5
- 150000003839 salts Chemical class 0.000 description 5
- HPALAKNZSZLMCH-UHFFFAOYSA-M sodium;chloride;hydrate Chemical compound O.[Na+].[Cl-] HPALAKNZSZLMCH-UHFFFAOYSA-M 0.000 description 5
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 4
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 4
- 238000011161 development Methods 0.000 description 4
- 238000005194 fractionation Methods 0.000 description 4
- 229910052744 lithium Inorganic materials 0.000 description 4
- 229910052700 potassium Inorganic materials 0.000 description 4
- 239000004575 stone Substances 0.000 description 4
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 3
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 3
- WTDHULULXKLSOZ-UHFFFAOYSA-N Hydroxylamine hydrochloride Chemical compound Cl.ON WTDHULULXKLSOZ-UHFFFAOYSA-N 0.000 description 3
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 description 3
- 235000011114 ammonium hydroxide Nutrition 0.000 description 3
- WDIHJSXYQDMJHN-UHFFFAOYSA-L barium chloride Chemical compound [Cl-].[Cl-].[Ba+2] WDIHJSXYQDMJHN-UHFFFAOYSA-L 0.000 description 3
- 229910001626 barium chloride Inorganic materials 0.000 description 3
- 238000009835 boiling Methods 0.000 description 3
- 238000005553 drilling Methods 0.000 description 3
- 239000010410 layer Substances 0.000 description 3
- STZCRXQWRGQSJD-GEEYTBSJSA-M methyl orange Chemical compound [Na+].C1=CC(N(C)C)=CC=C1\N=N\C1=CC=C(S([O-])(=O)=O)C=C1 STZCRXQWRGQSJD-GEEYTBSJSA-M 0.000 description 3
- 229940012189 methyl orange Drugs 0.000 description 3
- 239000011591 potassium Substances 0.000 description 3
- 239000000047 product Substances 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 241000283073 Equus caballus Species 0.000 description 2
- 238000009933 burial Methods 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 238000005119 centrifugation Methods 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 238000004140 cleaning Methods 0.000 description 2
- 239000008367 deionised water Substances 0.000 description 2
- 229910021641 deionized water Inorganic materials 0.000 description 2
- 239000012153 distilled water Substances 0.000 description 2
- 238000009826 distribution Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 238000011156 evaluation Methods 0.000 description 2
- 238000001704 evaporation Methods 0.000 description 2
- 230000008020 evaporation Effects 0.000 description 2
- 238000000605 extraction Methods 0.000 description 2
- 239000008398 formation water Substances 0.000 description 2
- 229910052742 iron Inorganic materials 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 230000001376 precipitating effect Effects 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- 238000004321 preservation Methods 0.000 description 2
- 230000008569 process Effects 0.000 description 2
- 230000001105 regulatory effect Effects 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- 241000894006 Bacteria Species 0.000 description 1
- 240000008574 Capsicum frutescens Species 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- 241001233242 Lontra Species 0.000 description 1
- 241000282320 Panthera leo Species 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000005137 deposition process Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000012530 fluid Substances 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 239000003673 groundwater Substances 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 229910052500 inorganic mineral Inorganic materials 0.000 description 1
- 239000011229 interlayer Substances 0.000 description 1
- 238000011835 investigation Methods 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 238000013508 migration Methods 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
- 239000011707 mineral Substances 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 238000004806 packaging method and process Methods 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 238000007789 sealing Methods 0.000 description 1
- 239000013049 sediment Substances 0.000 description 1
- 238000007873 sieving Methods 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- YALHCTUQSQRCSX-UHFFFAOYSA-N sulfane sulfuric acid Chemical compound S.OS(O)(=O)=O YALHCTUQSQRCSX-UHFFFAOYSA-N 0.000 description 1
- 150000003463 sulfur Chemical class 0.000 description 1
- 150000003467 sulfuric acid derivatives Chemical class 0.000 description 1
- 230000001360 synchronised effect Effects 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- 238000012795 verification Methods 0.000 description 1
- 238000005406 washing Methods 0.000 description 1
- 238000005303 weighing Methods 0.000 description 1
Classifications
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01V—GEOPHYSICS; GRAVITATIONAL MEASUREMENTS; DETECTING MASSES OR OBJECTS; TAGS
- G01V15/00—Tags attached to, or associated with, an object, in order to enable detection of the object
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
- G01N27/62—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating the ionisation of gases, e.g. aerosols; by investigating electric discharges, e.g. emission of cathode
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- General Life Sciences & Earth Sciences (AREA)
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- Health & Medical Sciences (AREA)
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Abstract
The invention discloses a method for dividing oil field water/gas-containing field water sources by sulfur isotopes. The method can determine different sources of the oil field water/gas-containing field water, is simple and feasible, has strong operability and lays a foundation for the research of the oil field water/gas-containing field water.
Description
Technical Field
The invention belongs to the field of oil and gas technology research, and particularly relates to a method for dividing oil field water/gas field water sources by sulfur isotopes.
Background
The world big oil-gas fields are often accompanied with oil-field water (or gas-containing water) output in the oil-gas exploitation process, and because the oil-field water is closely related to hydrocarbon migration, the study knowledge of the oil-field water is widely applied to understanding the formation history of oil-gas reservoirs and serving oil-gas perspective evaluation and oil-gas exploration development decision. In addition, oilfield water is often enriched in a variety of elements, such as: br, I, K, li, B, etc. Along with the fluctuation of potassium resource price and the rapid development of lithium battery technology in the new energy field in recent years, the lithium consumption is driven to climb, the resource evaluation quality and extraction test work for various useful elements in the oilfield water are greatly developed, and investigation shows that the useful components of the oilfield water in part of areas reach industrial grade, and the oilfield water is gradually becoming a development target of potential potassium resources and liquid new energy mineral resources. It has been reported that U.S. and canada are conducting oil field water lithium extraction projects and generating revenue. The German oilfield water is also very rich in lithium and potassium. However, the specific causes of various useful elements are controversial, and the cause mechanism difference and the process for enriching various useful elements in oilfield water have not been discussed deeply.
Moreover, the oilfield water is closely related to the oil reservoir, and the movable oilfield water can damage the oil and gas reservoir to cause oil and gas damage; and the closed oilfield water and the impermeable stratum are jointly closed to form the hydrodynamic oil and gas reservoir.
Research on the source of oilfield water is of great importance in solving the above problems.
Disclosure of Invention
The object of the present invention is to provide a method for dividing sources of oilfield water/gas field water by sulfur isotopes of the oilfield water/gas field water. The method can determine different sources of the oil field water/gas-containing field water, is simple and feasible, has strong operability and lays a foundation for the research of the oil field water/gas-containing field water.
The oilfield water/gas field water originates from among the various pores and fissures in the oilfield/gas field formation. The original oil/gas field water comes from the closed formation water (in fact, the original seawater/lake water at the time was captured) and then undergoes a long-term geological evolution. Thus, the sulfur isotopes of sulfate in formation water represent the sulfur isotopes of the body of water at the time of the sedimentary burial, i.e., the sulfur isotopes of sulfate of sea/lake water during the sedimentary period. The main ion components of the original oil field water/gas field water inherit the components in the original sea water/lake water, so the sulfate ion components are inherited, and the sulfur isotopes of the original water body at the time can be directly recorded under the condition of not being influenced by external fluid.
Sulfate deposition such as gypsum, anhydrite and the like does not generate obvious sulfur isotope fractionation in the deposition process, thus being capable of directly representing delta of the original water body 34 S sulfur isotope data. For example, delta of early-stage gypsum in the early-stage of the british section 34 The S sulfur isotope is about +35 mill, the sulfur isotope of the contemporaneous sea stratum water is about +35 mill unless the stratum water of other geological times and sources is mixed; whereas if the salt lake is a land-phase closed salt lake sediment, gypsum delta 34 The S sulfur isotope is about +15 mill, and the sulfur isotope of the contemporaneous terrestrial stratum water is about +15 mill; if the gypsum is deposited in a land open salt lake, the sulfur isotope of gypsum is about +25 mill or even higher, and the sulfur isotope of the land stratum water in the same period is about +25 mill; on the other hand, groundwater also dissolves the evaporite, but dissolution of sulfate deposits such as gypsum and anhydrite does not result in fractionation of sulfur isotopes. The sulfur isotope data in sea water/salt lake water can be directly recorded by sulfate deposition of gypsum, anhydrite and the like without fractionation, the sulfate deposition of gypsum, anhydrite and the like can record the original sulfur isotope components of ancient sea water/salt lake water sulfate radical, and even if the deposition is dissolved and reprecipitated, no obvious change is found in the data. The original oilfield/field water typically inherits the sulfur identity of the sulfate salt of the brine during the original seawater/lake water deposition periodTherefore, the sulfur isotope content of the original oilfield water can be estimated from the sulfur isotope data of gypsum, anhydrite, and the like in the formation.
In a closed oilfield water environment, oilfield water has similar sulfur isotope components with original seawater and lake water in the stratum at the time, for example, the sulfur isotope data of the oilfield water from sea phase is very similar to that of the gypsum sulfur isotope data at the time; and the freshwater deposition, the open salt lake deposition and the closed salt lake deposition in the land-phase stratum have different sulfur isotopes, and the oilfield water and the lake water in the land-phase stratum in different environments have similar sulfur isotope components. After being influenced by external water bodies, the sulfur isotopes of the original seawater and lake water can be obviously changed, and particularly, the sulfur isotopes are used for sea stratum and sedimentary basins for sealing the salt lake environment.
Based on the above principles, a first aspect of the present invention provides a method for sulfur isotope partitioning an oilfield water/gas field water source comprising the steps of:
1) Measuring sulfur isotope data of oil field water/gas field water to be measured;
2) Obtaining sulfur isotope data of an original source of the oilfield water/gas field water to be tested, comprising:
-collecting a sample of sulfate deposits in the formation in which the oilfield water/gas field water to be tested is located and determining its sulfur isotope data; and/or the number of the groups of groups,
obtaining raw deposited sulfur isotope data of the stratum where the oil field water/gas field water to be measured is located according to sea water sulfur isotope curves of different geological histories,
namely, the sulfur isotope data of the original source of the oilfield water/gas-containing field water to be detected;
3) Comparing the measured sulfur isotope data of the oil field water/gas-containing field water to be measured with the sulfur isotope data of the original source of the oil field water/gas-containing field water to be measured, and determining the source of the oil field water/gas-containing field water.
According to some embodiments of the invention, the sulfur isotope data is δ 34 S sulfur isotope value.
According to some embodiments of the present invention, when the oil/gas field water to be measured is sea stratum oil/gas field water, if the measured sulfur isotope data in the oil/gas field water to be measured and the measured sulfur isotope data of the original source of the oil/gas field water to be measured are similar, it is indicated that the oil/gas field water to be measured is derived from contemporaneous sea water, wherein the similarity means that the measured sulfur isotope data in the oil/gas field water to be measured is within ±2 mill of the original source sulfur isotope data;
when the oil field water/gas-containing field water to be detected is land stratum oil field water/gas-containing field water, if the measured sulfur isotope data in the oil field water/gas-containing field water to be detected is +7%o to +9%o, the oil field water/gas-containing field water to be detected is from fresh water input, and if the measured sulfur isotope data in the oil field water/gas-containing field water to be detected is +10%o to +15%o, the oil field water/gas-containing field water to be detected is from open salt lake of fresh water input; and if the measured sulfur isotope data in the oil field water/gas-containing field water to be measured is +25.0%o to +50.0%o, indicating that the oil field water/gas-containing field water to be measured is derived from a closed salt lake.
According to some embodiments of the invention, the sulphur isotope data in step 1) is determined by converting sulphate ions in the oilfield/gas field water into sulphate precipitates.
According to some preferred embodiments of the invention, the determination of the sulphur isotope data of the oil/gas field water in step 1) is performed by precipitating sulphate ions as barium sulphate, for example by a method comprising the steps of:
a) Adding hydroxylammonium hydrochloride and methyl orange indicator into the oil field water/gas field water sample to be detected, adjusting the pH value to be red by ammonia water and hydrochloric acid, adding excessive concentrated hydrochloric acid, boiling, adding barium chloride solution, and reacting to obtain solution containing white precipitate;
b) Separating white precipitate from the solution, washing, drying and weighing to obtain a sample to be detected;
c) Sulfur isotope data of a sample to be measured is determined, for example, by EA-MS (elemental analyzer-gas isotope mass spectrometer) in-line analysis.
In some embodiments, step 1) determines the sulfur isotope data for the oilfield water by: and 5g of hydroxylammonium hydrochloride and 2 drops of methyl orange indicator are added into the oilfield water sample to be measured, and the pH value of the solution is regulated by ammonia water and hydrochloric acid until the solution is red. Then, 3mL of excess concentrated hydrochloric acid (12 mol/L) was added, boiling was performed, and then 20mL of 100g/L barium chloride solution was added, followed by heat preservation for 30 minutes. After 12 hours of standing, the white precipitate was separated from the solution by centrifugation, while the precipitate was washed 3 times with deionized water. The resulting white precipitate BaSO4 was dried in an oven and weighed for preparation of sulfur isotope samples. The extracted BaSO4 sulfur isotope sample is analyzed by EA-MS connection line, and an Element Analyzer (EA) and a gas isotope Mass Spectrometer (MS) are connected by a continuous flow interface to realize isotope analysis.
According to some embodiments of the present invention, in the case that the formation where the oilfield water/gas-containing field water to be measured is an evaporite-containing formation, a sulfate deposition sample may be collected on the evaporite-containing formation and sulfur isotope data therein may be measured, that is, sulfur isotope data of an original source of the oilfield water/gas-containing field water to be measured. The stratum where the oil field water/gas-containing field water to be measured is not strictly limited to be the stratum where the oil field water/gas-containing field water to be measured is on the same plane, and the skilled person knows that the thickness of the oil field water layer varies greatly from a few meters to tens of meters, and the thickness is determined according to the burial depths of the upper bottom plate and the lower bottom plate of the oil field water reservoir; the oilfield water layer may exhibit a lenticular distribution at high salinity.
According to some embodiments of the invention, the sulfate deposit sample is selected from at least one of gypsum, anhydrite, and barite.
According to some embodiments of the invention, the sulfate deposit sample is obtained from a core and/or cuttings of evaporite from an evaporite-bearing formation, preferably a core, and the cuttings sample may be systematically collected in wells where no core is taken. In some embodiments, a sample of gypsum, anhydrite, and/or barite is collected from a core of evaporite in an evaporite-containing formation. In other embodiments, the collection of cuttings of gypsum, anhydrite, and barite is performed on the evaporite in the evaporite-containing formation.
According to some embodiments of the invention, the cuttings sample is used after being soaked, screened, washed and selected, for example, by a 40 mesh screen. In some examples, samples were individually poured into one-to-one and numbered open cylindrical plastic boxes of 1 liter capacity, and then poured into a barrel of distilled water to soak for about 5-15 minutes, and the cuttings material in the plastic boxes was slowly and uniformly stirred with a glass rod. And then cleaning and sieving the samples one by using a 40-mesh stainless steel mesh screen and using barreled distilled water. And after the cleaning is finished, carrying out preliminary sample picking, and picking out gypsum in the rock debris sample one by one.
According to the present invention, the determination of sulfur isotope data in sulfate deposits such as gypsum, anhydrite, and barite can be performed using methods commonly used in the art such as EA-MS in-line analysis.
According to some preferred embodiments of the present invention, existing wells may be used for sampling to conduct studies of oil/gas field water sources, such as by determining the location and depth of gypsum-containing wells for various geological histories through geologic maps and logging data, sampling to conduct studies of different formation oil/gas field water based on records of geologic samples. In some embodiments, sampling of sulfate deposit samples in the evaporite basin is accomplished by comprehensive analysis of the geologic map and stratigraphic columns, log data, and the like of the evaporite basin in combination with research project sampling requirements.
According to some embodiments of the present invention, for the oil field water/gas-containing field water of the sea-phase stratum without the evaporite, the originally deposited sulfur isotope data of the stratum where the oil field water/gas-containing field water to be measured is located, that is, the originally sourced sulfur isotope data of the oil field water/gas-containing field water to be measured, may be obtained according to the sea water sulfur isotope curves of different geological histories. According to some embodiments of the invention, global isotope averages of the seawater sulfur isotope curves of the different geological histories are taken for comparison.
According to some embodiments of the invention, the brine sulfur isotopes deposited in the sea-phase formation at different geological historic times correspond to the sulfur isotopes of the then-current sea water, i.e., the sulfur isotopes of sea-phase gypsum.
Delta of seawater throughout geological historic period 34 The S sulfur isotope composition is obviously changed, and the sulfate sulfur isotope composition in the sea water can be faithfully recorded by sulfate deposition. According to the present invention, the sulfur isotope curves of seawater for different geological histories can be derived from research results known in the art, and prior related studies are incorporated herein by reference. For example, delta of seawater throughout the geological history 34 S sulfur isotope composition is obviously changed, delta of sea water 34 The S sulfur isotope reaches the highest value of the whole universe of development in the period of the chilly, and can reach +35 permillage or even higher; in the middle of the Ornithogali, the sulfur isotope drops rapidly to 27 per mill and continues to drop; thereafter a high value occurs during the transition from the di-to tri-stitch; and has a minimum value of 10 per mill in the two-fold, wherein, the research on gypsum sulfur isotopes in Sichuan basin finds that in the Jiang river group, delta in the early three-fold of Sichuan basin in China 34 The S sulfur isotope data can reach +34.5%o, see Table 1 and FIG. 1. Sea phase formation evaporite studies have found that sea phase gypsum can directly record ancient sea water sulfur isotopes without fractionation and establish a pattern of sea water sulfur isotope changes throughout the geological history, as shown in fig. 1. The sulfate deposits of original gypsum, anhydrite and the like in the synchronous each sea phase evaporation rock basin record the sulfur isotope of the seawater at the time of the basin, and the sulfur isotope composition of the seawater is basically consistent with that of the closed original oilfield water.
TABLE 1 Sulfur isotopes of gypsum and brine from different stages of formation
According to some embodiments of the present invention, for a sea-phase formation without evaporite, it is possible to take fossil therein (sea-phase formation lacking evaporite is rich in various fossil) and then determine the geologic time based on biological geology, thereby obtaining raw deposited sulfur isotope data of the formation where the oilfield water/gas field water to be measured is located from sea water sulfur isotope curves of different geologic history periods.
According to some embodiments of the present invention, for the case where the formation in which the oilfield water/gas field water to be measured is located is a land-phase formation where evaporite is deposited, the correspondence relationship between oilfield water in the evaporite deposit basin and the evaporite sulfur isotope is: river input salt lake (freshwater input open salt lake), δ 34 The S value is approximately +10%o to +15%o; while inland closed salt lake (closed salt lake), delta 34 The S value is +25.0- +50.0-%. For example delta in our country terrestrial basin 34 The S value has a clear interval range (+21%o-25%o) and can be divided into A, B areas. Delta in zone A basin 34 S values are all lower than +21%o, and in the fourth century, the drilling gypsum delta of the Gellera lake is obtained 34 The S value is 11.3-13.4%, the salt lake in the sea is 10.9-20.0%, the sweat-taking Sila diagram is 9.6%, the concave place in the North of China is 7.4-11.5%, and the average delta of the sea water is obviously lower than that of the modern sea water 34 S (20.5%o), which is a typical terrestrial cause and is supplied by the surrounding fresh water, has lighter delta 34 S value. While in zone B, basin delta 34 S values are higher than 25 per mill, and the ancient near-line sulfate delta in the depression of the submerged river 34 The S value is 31-40.43%, the east Pu pit palace is 28-33%, the Jiangling pit palace is 25.2-32.6%, and the Qing sea lion subslot palace is drilled at 26.5-32.3%. These values are all higher than 25 per mill, compared with the average delta of modern seawater 34 The S value is high and is far higher than the possible water source delta at the time 34 S value, this extremely high delta 34 The S value is a closed inland salt lake, sulfate bacteria continuously reduce sulfate radical, and delta in residual brine is caused 34 The S value increases.
According to some embodiments of the invention, the oilfield water in the different environmental land formations is similar in sulfur isotope composition to the lake water at the time. Wherein the sulfur isotopes input into the river are approximately between +7 permillage and +9 permillage, such as about +8 permillage; inland salt lakes are divided into open salt lakes and closed salt lakes, the open salt lakes with fresh water input being between +10 permillage and +15 permillage, and the closed salt lakes being above +25.0 permillage, in particular +25.0 permillage to +50.0 permillage.
According to some embodiments of the present invention, for the case that the stratum where the oil field water/gas field water to be measured is an evaporite-containing stratum, particularly a sea-phase evaporite stratum, the original deposited sulfur isotope data of the stratum where the oil field water/gas field water to be measured is located may be obtained according to sea water sulfur isotope curves of different geological histories, for example, carbon and oxygen isotopes in upper and lower carbonate strata and an interlayer of the evaporite stratum may be measured, the exact age of the evaporite and the geological period may be determined through carbon isotope stratigraphy study, and then corresponding sulfur isotope data may be obtained according to sea water sulfur isotope curves of different geological histories. In particular, sulfur isotope data determined by carbonate depositions can also be compared to sulfur isotope data obtained by seawater sulfur isotope curves of different geological historic periods for verification. It should be noted that there is some small difference between the sulfur isotopes of the respective sea basin due to the regional variation, so that the analysis of the sulfur isotopes is preferably performed by selecting sulfate rock (gypsum, anhydrite, etc.) among the evaporite in the region where the evaporite exists.
According to the method disclosed by the invention, a large number of rock core and rock debris samples of gypsum, anhydrite or barite in drilling evaporite strata with different depths or horizons in the same evaporite basin can be treated, and sulfur isotope data of water bodies (seawater/lake water) in various geological periods in the evaporite basin can be obtained.
The second aspect of the invention also provides the use of a method according to the first aspect of the invention for partitioning an oilfield water and/or a source of a gas-containing field water.
In the present invention, the sulfur isotope data includes delta 34 S sulfur isotope number of 32 S and 34 the relative ratio of the two stable isotopes of S is normalized to the iron merle in the Dibulogel iron merle (CDT).
In the invention, the sulfate deposition sample refers to delta which can faithfully record seawater in each geological history period 34 Sulfate deposits of the S sulfur isotope composition information, such as gypsum, anhydrite, barite, etc., are not found to significantly change the sulfur isotope data even if these deposits are dissolved and reprecipitated.
The invention has the following beneficial effects:
the method can obviously determine different sources of the oil field water/gas-containing field water, is simple and feasible, has strong operability and lays a foundation for the research of the oil field water/gas-containing field water.
Drawings
FIG. 1 is a graph of the sulfur isotope curves of seawater and the gypsum sulfur isotope distribution of the three-fold of the Sichuan basin for different geological histories.
Detailed Description
In order that the invention may be more readily understood, a detailed description of the invention will be presented below in conjunction with examples, it being emphasized that the following description is exemplary only and should not be taken as limiting the scope of the invention.
Examples
A series of sulfur isotope analyses were performed on gypsum from the Ordosbasin Ortha Majia ditch group and oil field water from the top of the Majia ditch group, with the following specific steps and results:
1) According to the comprehensive analysis of the geological map, the stratum histogram and the logging data, the sampling requirement of a research project is combined, and the sampling of the core sample gypsum is completed: sampling the corresponding position of the sampling well according to the compiled sampling depth table, sequentially numbering the sampled products according to the drilling depth and registering the well depth, packaging the sampled products with a special paper bag and measuring the sulfur isotope delta of the sampled products 34 S value.
2) Sampling oilfield water at the corresponding horizon, precipitating sulfate radicals into barium sulfate, and analyzing sulfur isotopes: and 5g of hydroxylammonium hydrochloride and 2 drops of methyl orange indicator are added into the oilfield water sample to be measured, and the pH value of the solution is regulated by ammonia water and hydrochloric acid until the solution is red. Then, 3mL of excess concentrated hydrochloric acid (12 mol/L) was added, boiling was performed, and then 20mL of 100g/L barium chloride solution was added, followed by heat preservation for 30 minutes. After 12 hours of standing, the white precipitate was separated from the solution by centrifugation, while the precipitate was washed 3 times with deionized water. The resulting white precipitate BaSO4 was dried in an oven and weighed for preparation of sulfur isotope samples. The extracted BaSO4 sulfur isotope sample is analyzed by EA-MS connection, and an Elemental Analyzer (EA) and a gas isotope mass spectrometer (M S) are connected through oneContinuous flow interfaces are connected to measure sulfur isotope delta 34 S value.
3) Comparing sulfur isotope delta of sulfur isotope of oilfield water to be tested 34 S value and sulfur isotope delta of sulfur isotope of gypsum sample of stratum where oilfield water to be measured is located 34 S value, comprehensively presuming source of oilfield water to be detected, and sulfur isotope delta 34 The S-value results are shown in table 2 below:
table 2 sulfur isotopes of the Ordosbasin Ornith gypsum and brine
Sulfur isotope test data delta for gypsum samples obtained through core logs 34 S value and international contemporaneous stratum sulfur isotope data delta 34 The S values were compared and found that the gypsum of the ottoman ditch group of the erdos basin was similar to the other ottoman evaporation rock basins internationally and in line with the previously published data. These data lay the foundation for finding a comparison of the source of oilfield water at the top of the rotunda ottoman family of the erdosbasin.
The top of the Majia ditch group stratum in the middle of the Ordos basin is an unconformity weathered crust, and the sea Liu Jiaohu stratum of the carbolic-dichotomy is covered on the top. The Majia ditch group stratum is a stratum mainly containing carbonate rock, but the eastern part of the Erdos basin is a stratum containing evaporite; the sea water sulfur isotope in the period of the Ordosbasin is from the analysis of gypsum samples of the ancient world underground in the Earthur basin (as shown in Table 2), wherein the average value of the sea water gypsum sulfur isotope in the stratum of the Majia group in the middle of the Ordosis is approximately +27 per mill, so that the corresponding original oilfield water sulfur isotope in the stratum is estimated to be approximately +27 per mill. Analysis of sulfur isotopes in the top oilfield water of the equine sulcus group stratum in the middle of the Ornithogali shows that the oilfield water has a large fluctuation range from +12.7%o to +28.1%o; wherein 3 data are between +26.7 permillage and +28.1 permillage, which are consistent with the data of the otter sea phase evaporite; however, other data were between +12.7% and +19.9%, showing clearly the input of fresh water or the mixing of the formation field water for the upper stone charcoal-di-stack sea Liu Jiaohu phase. The rock-binary sea stratum lacks of evaporite deposition, and the sulfur isotope of the rock-binary sea water is estimated to be about +10 mill according to the international sulfur isotope curve; the sulfur isotope of the oil field water obtained from the upper stone charcoal-bilge Liu Jiaohu phase stratum is about +10%; the sulfur isotope of the oilfield water from the two-folded land-phase stratum stone box group is about +8 mill, and meets the input of fresh water.
According to the correlation between the sulfur isotopes of the oil field water and the sea stratum, we can speculate that the sulfur isotopes of the original oil field water from the sea water at the top of the Ordosbasin Olympic horse family ditch group is about +27 per mill. However, the top of the Ordosbasin Ortzma ditch group was a non-integral surface, and was also covered with a layer of stone charcoal-the binary sea Liu Jiaohu phase, which also matched the previous study projections.
It should be noted that the above-described embodiments are only for explaining the present invention and do not constitute any limitation of the present invention. The invention has been described with reference to exemplary embodiments, but it is understood that the words which have been used are words of description and illustration, rather than words of limitation. Modifications may be made to the invention as defined in the appended claims, and the invention may be modified without departing from the scope and spirit of the invention. Although the invention is described herein with reference to particular means, materials and embodiments, the invention is not intended to be limited to the particulars disclosed herein, as the invention extends to all other means and applications which perform the same function.
Claims (10)
1. A method of sulfur isotope partitioning an oilfield water/gas field water source comprising the steps of:
1) Measuring sulfur isotope data of oil field water/gas field water to be measured;
2) Obtaining sulfur isotope data of an original source of the oilfield water/gas field water to be tested, comprising:
-collecting a sample of sulfate deposits in the formation in which the oilfield water/gas field water to be tested is located and determining its sulfur isotope data; and/or the number of the groups of groups,
obtaining raw deposited sulfur isotope data of the stratum where the oil field water/gas field water to be measured is located according to sea water sulfur isotope curves of different geological histories,
namely, the sulfur isotope data of the original source of the oilfield water/gas-containing field water to be detected;
3) Comparing the measured sulfur isotope data of the oil field water/gas-containing field water to be measured with the sulfur isotope data of the original source of the oil field water/gas-containing field water to be measured, and determining the source of the oil field water/gas-containing field water.
2. The method of claim 1, wherein the sulfur isotope data is δ 34 S sulfur isotope value.
3. The method according to claim 1 or 2, wherein when the oilfield water/gas-containing field water to be measured is a sea-phase formation oilfield water/gas-containing field water, if the measured sulfur isotope data in the oilfield water/gas-containing field water to be measured is similar to the original source sulfur isotope data of the oilfield water/gas-containing field water to be measured, it is indicated that the oilfield water/gas-containing field water to be measured is derived from contemporaneous seawater, wherein the similarity means that the measured sulfur isotope data in the oilfield water/gas-containing field water to be measured is within ±2%o of the original source sulfur isotope data;
when the oil field water/gas-containing field water to be detected is land stratum oil field water/gas-containing field water, if the measured sulfur isotope data in the oil field water/gas-containing field water to be detected is +7%o to +9%o, the oil field water/gas-containing field water to be detected is from fresh water input, and if the measured sulfur isotope data in the oil field water/gas-containing field water to be detected is +10%o to +15%o, the oil field water/gas-containing field water to be detected is from open salt lake of fresh water input; and if the measured sulfur isotope data in the oil field water/gas-containing field water to be measured is +25.0%o to +50.0%o, indicating that the oil field water/gas-containing field water to be measured is derived from a closed salt lake.
4. A method according to any one of claims 1-3, characterized in that in step 1) the sulphur isotope data thereof is determined by converting sulphate ions in the oilfield/gas field water to be tested into sulphate precipitates, preferably barium sulphate.
5. The method according to any one of claims 1 to 4, wherein in step 2), in case the formation in which the oilfield water/gas field water to be measured is an evaporite-containing formation, a sulfate deposition sample is collected on the evaporite-containing formation and sulfur isotope data therein is determined, i.e. the sulfur isotope data of the original source of the oilfield water/gas field water to be measured;
and obtaining the original deposited sulfur isotope data of the stratum where the oil field water/gas-containing field water to be detected is located according to the sea water sulfur isotope curves of the sea water stratum without the evaporite in different geological historic periods, namely the original source sulfur isotope data of the oil field water/gas-containing field water to be detected.
6. The method of any one of claims 1-5, wherein the sulfate deposition sample is selected from at least one of gypsum, anhydrite, and barite.
7. The method of claim 5, wherein the sulfate deposit sample is taken from a core and/or cuttings of evaporite from the evaporite-containing formation.
8. The method according to claim 5, wherein for sea-phase formations without evaporite, fossil therein is taken and geological time periods are determined based on biological geology, whereby the raw deposited sulfur isotope data of the formation in which the field water/gas-containing field water to be tested is located is obtained from sea water sulfur isotope curves of different geological historic time periods.
9. The method of any one of claims 1-8, further comprising determining the location and depth of the gypsum-containing well for each geological historic period from the geological map and logging data, and conducting studies of the source of oil and/or gas field water for different formations based on recorded samples of the geological samples.
10. Use of the method according to any one of claims 1-9 for partitioning oilfield water and/or a source of gas-containing water.
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