CN108254480A - A kind of oxygen and carbon isotopes detecting system and detection method for carbonate rock - Google Patents
A kind of oxygen and carbon isotopes detecting system and detection method for carbonate rock Download PDFInfo
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- CN108254480A CN108254480A CN201611241586.6A CN201611241586A CN108254480A CN 108254480 A CN108254480 A CN 108254480A CN 201611241586 A CN201611241586 A CN 201611241586A CN 108254480 A CN108254480 A CN 108254480A
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N30/00—Investigating or analysing materials by separation into components using adsorption, absorption or similar phenomena or using ion-exchange, e.g. chromatography or field flow fractionation
- G01N30/02—Column chromatography
- G01N30/88—Integrated analysis systems specially adapted therefor, not covered by a single one of the groups G01N30/04 - G01N30/86
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N30/00—Investigating or analysing materials by separation into components using adsorption, absorption or similar phenomena or using ion-exchange, e.g. chromatography or field flow fractionation
- G01N30/02—Column chromatography
- G01N30/88—Integrated analysis systems specially adapted therefor, not covered by a single one of the groups G01N30/04 - G01N30/86
- G01N2030/8809—Integrated analysis systems specially adapted therefor, not covered by a single one of the groups G01N30/04 - G01N30/86 analysis specially adapted for the sample
- G01N2030/8859—Integrated analysis systems specially adapted therefor, not covered by a single one of the groups G01N30/04 - G01N30/86 analysis specially adapted for the sample inorganic compounds
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N30/00—Investigating or analysing materials by separation into components using adsorption, absorption or similar phenomena or using ion-exchange, e.g. chromatography or field flow fractionation
- G01N30/02—Column chromatography
- G01N30/88—Integrated analysis systems specially adapted therefor, not covered by a single one of the groups G01N30/04 - G01N30/86
- G01N2030/8809—Integrated analysis systems specially adapted therefor, not covered by a single one of the groups G01N30/04 - G01N30/86 analysis specially adapted for the sample
- G01N2030/8868—Integrated analysis systems specially adapted therefor, not covered by a single one of the groups G01N30/04 - G01N30/86 analysis specially adapted for the sample elemental analysis, e.g. isotope dilution analysis
Abstract
The present invention relates to a kind of oxygen and carbon isotopes detecting system for carbonate rock, including：Infrared laser sample-melting device, purification enrichment device and separation detecting device；The infrared laser sample-melting device includes infrared laser and sample room, and the sample room both ends, which are connected with, to be connect with the pipeline of circulated gases, wherein one end with the de-watering apparatus in the purification enrichment device, other end connection carrier gas inlet；The purification enrichment device includes the de-watering apparatus, a carbon dioxide-enriched device, gas circuit conversion equipment, the secondary enriching and purifying carbon dioxide plant that pass sequentially through pipeline connection, the secondary enriching and purifying carbon dioxide plant is connect with the separator in the separation detecting device, and the separation detecting device includes the separator and detection device that pass sequentially through pipeline connection.The present invention also provides a kind of oxygen and carbon isotopes detection methods, and using detecting system accuracy of detection of the present invention height, speed is fast and is suitable for the detection of denier sample.
Description
Technical field
The invention belongs to Hydrocarbon Formation Reservoirs geological exploration fields, are related to a kind of oxygen and carbon isotopes detecting system and detection method,
Relate more specifically to a kind of oxygen and carbon isotopes detecting system and detection method for carbonate rock.
Background technology
In Hydrocarbon Formation Reservoirs research, fluid (oil gas)-rock interaction is complicated, and geologist is usually to the not same period time
The carbonatite cement (including DOLOMITE CRYSTALS, calcite crystal etc.) of formation carries out oxygen and carbon isotopes analysis, to study carbonic acid
The Pore Genesis mechanism and diagenetic environment of rock salt reservoir.However, mixed since cement is often superimposed symbiosis in diagenetic process,
And many structural constituents and mineral crystal arteries and veins, spatial resolution are usual<500 μm, phosphoric acid method is crushed using conventional total rock sample and is surveyed
It measures entire sample and is often mixed into other uncorrelated components, it is impossible to which accurate geological information is provided, it is necessary to is " micro- to " crystal " progress
It analyzes in area ".
Early stage P.Dennis (1979) develops micro- drilling tool to drill through these micro-examples, enters oxygen and carbon isotopes point
" microcell " epoch of analysis, but still it is difficult to ensure that the sample source relatively deposited, and complicated for operation time-consuming.The mid-80 Jones
(1986) laser beam of proposition high-energy replaces micro- drilling tool, it has the characteristics that " high spatial resolution, micro-zone in situ ",
Hereafter foreign scholar has carried out a large amount of laser microprobe isotopic compositions analysis method research and transformation, achieves one
Serial achievement, it is believed that there are certain inhomogeneities, carbon under laser sampling scale not to be fractionated significantly, be obtained for standard substance
Data and total rock phosphoric acid method substantially close to, and fractionation can occur for oxygen isotope, during due to laser heat action,3 O atoms only have 2 to be converted into CO2, remaining O remained in CaO.It therefore must be right
Measured O data does a correction.
Although laser capture microdissection isotope analysis technology comes out for many years, its reproducibility (accuracy) of the data of lab analysis
All be significantly less than the analysis of total rock phosphoric acid method as a result, especially oxygen isotope value.
There is patent to disclose a kind of measuring device and measuring method of the oxygen and carbon isotopes of carbonate rock in recent years
(CN201410854514.3), inventor measures oxygen and carbon isotopes using ultraviolet laser.Device includes：Ultraviolet laser degrades device
With oxygen and carbon isotopes measuring appliance；Ultraviolet laser degrades device and includes ultraviolet laser and carbonate samples pond；Ultraviolet laser is set
Above carbonate samples pond, carbonate samples pond is provided with helium import and helium outlet, and ball is provided on helium outlet
Shape frosted connector, quartz filter are arranged among spherical frosted connector；Oxygen and carbon isotopes measuring appliance includes sequentially connected：Automatically
Injector removes water trap A, eight ways valve, chromatographic column, removes water trap B, open split and mass spectrograph.Method includes：It is shelled through ultraviolet laser
Carbonate samples after erosion are sent into oxygen and carbon isotopes measuring appliance, and oxygen and carbon isotopes are measured using phosphoric acid acid hydrolyzation.The invention overcomes
Asking for the isotope fractionation of precise calibration is difficult in infrared laser probe carbonate micro-zone in situ C-O isotopes analysis method
Topic, improves precision and the accuracy of analysis result.But for our geological samples and actual conditions, there are following for the invention
Problem：1st, using high-end UP213 ultraviolet lasers, acquisition cost is far longer than infrared laser, furthermore laser ablation generates
Be aerosol particle, generate definitely memory effect in pipeline, next isotope analysis result may be influenced.2nd, it finally adopts
Traditional acidolysis is taken to chemically react, chemical reaction and equilibrium process consume the longer ground time.3rd, reservoir denier cannot be met
The detection demand of sample mineral.
Invention content
In view of the deficiencies of the prior art, it is an object of the present invention to provide a kind of oxygen and carbon isotopes inspections for carbonate rock
Examining system, the detecting system is simple and efficient, improve detection oxygen and carbon isotopes accuracy and precision and the degree of automation more
It is high.
According to an aspect of the invention, there is provided a kind of oxygen and carbon isotopes detecting system for carbonate rock, including：
Laser sample-melting device, purification enrichment device and separation detecting device, wherein the laser sample-melting device is infrared
Laser capture microdissection sample-melting device.
According to some embodiments of the present invention, the infrared laser sample-melting device includes infrared laser and sample room；Institute
State the top that infrared laser is located at the sample room, the sample room both ends be connected with can with the pipeline of circulated gases, wherein
One end is connect with the de-watering apparatus in the purification enrichment device, other end connection carrier gas inlet.The laser is located at described
The top of sample room so that the laser that laser is sent out can be irradiated on the region to be measured of the sample in sample room.
According to a preferred embodiment of the present invention, the infrared laser is infrared laser commonly used in the art, excellent
Selecting laser output power, the sample room is the sample room of good seal, and preferably vacuum degree is 10 for 30w-4Below Pa's
Sample room, the laser video window of the sample room can specifically select the fluorination barium glass of infrared light, and (light transmittance reaches
92%), and by O shape fluorine rubber sealings.Being connected at sample room both ends can be with the pipeline of circulated gases, specially in sample room two
It holds and is equipped with 1/8 inch of stainless steel threaded sleeve hole, 1/32 inch of stainless steel tubing leakproofness is connected by Vespel gaskets in hole
Good sample room, one end connection carrier gas inlet, the other end connect the de-watering apparatus, the preferred He of carrier gas.Have two-way into
Carrier gas He, is connected to sample room input end all the way, is connected to six-way valve port all the way.
According to certain embodiments of the present invention, the purification enrichment device is included through the sequentially connected water removal dress of pipeline
It puts, a carbon dioxide-enriched device, gas circuit conversion equipment and secondary enriching and purifying carbon dioxide plant.
Never start once to be enriched to before primary enrichment terminates, a carbon dioxide-enriched device passes through the gas circuit
Conversion equipment is connected to the ambient atmosphere other than the oxygen and carbon isotopes detecting system, described primary after primary enrichment
Carbon dioxide-enriched device is connected to the secondary enriching and purifying carbon dioxide plant by the gas circuit conversion equipment, and described two
Secondary enriching and purifying carbon dioxide plant is connect with the separation impurity device in the separation detecting device.
According to a preferred embodiment of the present invention, its role is to remove after molten sample in product for the de-watering apparatus
Water, in some specific embodiments, the de-watering apparatus is semipermeable membrane, it is preferable to use Nafion is managed.
According to certain embodiments of the present invention, the gas that remaining is not enriched with when carrying out a carbon dioxide-enriched is by carrier gas
It is discharged to outside oxygen and carbon isotopes detection device, so that revert to gaseous carbon dioxide is sent to institute by carrier gas after enrichment
State secondary enriching and purifying carbon dioxide plant.
According to a preferred embodiment of the present invention, a carbon dioxide-enriched device is by reducing in the device
Temperature gaseous carbon dioxide is caused to become the carbon dioxide of solid-state or liquid, so as to be enriched with to obtain solid-state or liquid carbon dioxide
Device, cold-trap can be selected in some specific embodiments, more specifically for be a kind of U-shaped stainless steel tubing.
According to certain embodiments of the present invention, the gas circuit conversion equipment is manually or automatically changes gas circuit flow direction
Device so that sample introduction without shunt it is lossless, in some specific embodiments, the gas circuit conversion equipment be six-way valve.
According to a preferred embodiment of the present invention, the secondary enriching and purifying carbon dioxide plant is in enrichment titanium dioxide
The device of purification of carbon dioxide again while carbon, more specifically the inner sleeve capillary chromatograph specially in cold-trap, inner sleeve hairiness
The U-shaped stainless steel tubing of thin chromatographic column.A specific embodiment in the present invention, the capillary chromatograph are PLOT-Q types
Capillary chromatograph.
According to certain embodiments of the present invention, the separation detecting device includes separator and detection device, described
Separator is connect by pipeline with the secondary enriching and purifying carbon dioxide plant of the device for enriching and purifying.
According to a preferred embodiment of the present invention, gaseous carbon dioxide is can be mixed by the separator with other
Foreign gas separation device, the specific foreign gas is air；In some specific embodiments, the separation impurity
Device is specially gas chromatographic column, in the present invention a specific embodiment, and the chromatographic column is HP-PLOT-Q type gas phases
Chromatographic column.
According to certain embodiments of the present invention, the detection device is isotope mass spectrometer, for the isotope matter
There is no particular limitation for spectrometer, is the common gas isotope detection device of those skilled in the art, in a specific embodiment,
For oxygen and carbon isotopes mass spectrograph.
According to certain embodiments of the present invention, to the type of the carbonate rock, there is no particular restriction, preferably calcite
And dolomite, for sample size and weight, also there is no particular restriction, it is particularly suited for reservoir denier sample, specific sample
Spatial resolution be less than 500 μm.
According to another aspect of the present invention, a kind of oxygen and carbon isotopes detection method for carbonate rock is additionally provided,
It is detected using above-mentioned for the oxygen and carbon isotopes detecting system of carbonate rock, including：
Before sample is melted to carbonate samples, carrier gas is passed through so that sample room air is discharged to other than detecting system,
After molten sample, carrier gas is passed through so that the gas generated after molten sample passes through purification enrichment and separation detection.
According to a particular embodiment of the invention, the detection method is specially and includes the following steps：
1. air in discharge sample room, carries out molten sample later before molten sample；
2. it is enriched with carbon dioxide gas therein and when being enriched with by the gas generated after molten sample water removal, by cold-trap
Foreign gas is removed, the gas after enrichment is passed through to the cold-trap enriching and purifying for being cased with capillary chromatograph again later；
3. carbon dioxide gas after purification is detached with mixed air, gas progress carbon oxygen is same after being finally based on separation
Position element detection.
Detection method according to the present invention, for the enrichment time in step 2, there is no particular limitation, people in the art
Member can adjust enrichment time according to the amount of sample to be tested；For the enriching and purifying time, also there is no particular limitation, this field
Technical staff can adjust the enriching and purifying time according to the gas flow that cold-trap discharges.
According to the present invention, the detecting system composition is easy, and accuracy of detection is high, and detection time used is few and suitable for atomic
Measure the detection of sample.
Description of the drawings
Fig. 1 is the structure diagram of the oxygen and carbon isotopes detecting system.
Fig. 2 is the gas circuit status diagram represented after be once enriched with.
Fig. 3 is to represent never to start once to be enriched to the gas circuit status diagram before primary enrichment terminates.
Reference sign：
101：Sample room；102：Infrared laser；103：Sample sheet；104、105：1/8 inch of stainless steel threaded sleeve
Hole；106：Nafion is managed；107：Stainless steel cold-trap；108：Capillary column cold-trap；109：Six-way valve；110：Chromatographic column；111：Same position
Plain mass spectrograph.
Specific embodiment
Technical scheme of the present invention is described further with reference to embodiment, but is not formed to any of the present invention
Limitation.
As shown in Figure 1, oxygen and carbon isotopes detecting system of the present invention includes laser sample-melting device, purification enrichment device and divides
From detection device.
Wherein, the laser sample-melting device is the micro- sample-melting device of infrared laser, including sample room 101 and infrared laser
102, sample sheet 103 is sealed in sample room 101, and infrared laser 102 is suspended on the top of sample room 101, infrared laser
The laser that device 102 is sent out can be irradiated on the region to be measured of sample sheet 103, it is made to be generated carbon dioxide gas by thermal decomposition
Body.In a specific embodiment of the present invention, the vacuum degree of sample room 101 is up to 10-4Pa is provided with laser form on sample room
Piece, for the barium fluoride sheet glass (light transmittance up to 92%) of infrared optical fiber can be penetrated, and by O shape fluorine rubber sealings；In sample room
Both ends, which are connected with, to be specially equipped with 1/8 inch of stainless steel threaded sleeve hole at sample room both ends with the pipeline of circulated gases
104th, 105,1/32 inch of good sample room of stainless steel tubing leakproofness is connected by Vespel gaskets in hole, one end connection carries
Gas import, other end connection de-watering apparatus.The output power of infrared laser 102 is 30w.
The purification enrichment device include successively via the sequentially connected Nafion pipes 106 of pipeline, stainless steel cold-trap 107,
Six-way valve 109 and capillary column cold-trap 108, in a specific embodiment of the present invention, the effect of Nafion pipes 106 are after removing molten sample
Water in product；The temperature of stainless steel cold-trap 107 is very low, and gaseous carbon dioxide becomes the two of solid-state or liquid to gas after entering
Carbonoxide, so as to be enriched with to obtain solid-state or liquid carbon dioxide；Six-way valve 109 can manually or automatically change gas circuit flow direction；
Capillary column cold-trap 108 is to carry out secondary enrichment to carbon dioxide to be carried out at the same time purifying.
The separation detecting device includes chromatographic column 110 and isotope mass spectrometer 111, and chromatographic column 110 is HP-PLOT-Q types
Gas chromatographic column, one end connection capillary column cold-trap 108, receives enriched carbon dioxide after purification, is further separated off
Other mixed gaseous impurities in carbon dioxide, other end connection isotope mass spectrometer 111, the carbon dioxide after separation is sent into
Isotope mass spectrometer 111 carries out isotope detection.
In the embodiment of the present invention, infrared laser used is the U.S. Electro Scientific Industries, Inc.
The MIR10 lasers of production；Nafion pipes are produced for E.I.Du Pont Company；Capillary column cold-trap is the PLOT-Q that inner sleeve aperture is 0.32mm
The U-shaped stainless steel tubing of capillary chromatograph；Chromatographic column is the HPPLOT-Q type gas chromatographic columns of Agilent company of the U.S. production；Carbon
Oxygen isotope mass spectrograph is the Mat253 isotope mass spectrometers of Thermo Fisher companies of U.S. production.Sample to be tested is derived from
GBW04417, NBS-18 (American National Standard).
According to certain embodiments of the present invention, the course of work of the detecting system is as follows：
(1) rotation six-way valve becomes gas circuit state not start the state being once enriched with, as shown in figure 3, stainless steel cold-trap
107 and capillary column cold-trap 108 be in room temperature state, by pre-fabricated 103 fixing seal of sample sheet in sample room 101.
Helium is continually fed by carrier gas inlet first, the indoor air of sample is taken away and the drain 6 through six-way valve 109 is discharged；Again
Cold-trap device 107 is immersed in liquid nitrogen container, region to be analyzed, microcell are determined by the microscopic system of computer control software
After positioning, infrared laser 102 inspires the laser beam of high-energy, and being irradiated on sample sheet 103 makes it be generated by thermal decomposition
CO2Gas, this process may generate a small amount of CO gases since incomplete reaction occurs.
(2) CO that laser melting generates at this time2, CO and there may be foreign gas H2O、O2Deng with helium stream
It is managed into Nafion, impurity H2O is removed, and enrichment under test gas CO is freezed subsequently into stainless steel cold-trap 1072, CO2It is left on
In stainless steel cold-trap 107, foreign gas follows helium to be discharged through drain 6.Cold-trap 108 is immersed in liquid nitrogen container at this time, then
Gas circuit state is become the state after being once enriched with by rotation six-way valve, as shown in Fig. 2, being then placed in cold-trap 107
Room temperature state, CO therein2It is released and freezes purifying again through capillary column cold-trap 108.It freezes after purification, by cold-trap 108
It is placed in room temperature state, the CO after enriching and purifying2All released into gas chromatographic column 110.
(3) gas chromatographic column 110 is to CO after purification2It is kept completely separate with possible mixed air, obtains CO to be measured2,
It finally enters isotope mass spectrometer 111 and detects oxygen and carbon isotopes composition.
Embodiment 1
First, cold-trap 107 and 108 is placed in room temperature, gas circuit state is become not start the state being once enriched with, is passed through load
Gas discharges air in sample room before molten sample, at this point, cold-trap 107 is immersed in liquid nitrogen container, 107 temperature of cold-trap is made to be reduced to and can make
The cured degree of carbon dioxide gas later carries out sample 103 using infrared laser 102 molten sample, the work of the laser
Make mode as continuous agitation mode, laser power 30w, used sample is derived from GBW04417, and the sample is less than sample room
The thin slice of the 1mm thickness of size is passed through carrier gas so that the gas generated after molten sample is by Nafion pipes 106, in cold-trap 107 after melting sample
Middle freezing enrichment 3 minutes, becomes state after being once enriched with, while cold-trap 107 is restored by gas circuit state later
To room temperature, cold-trap 108 is immersed in liquid nitrogen container, and the gas after enrichment is sent into cold-trap 108 later, freezing enriching and purifying 3 minutes,
Cold-trap 108 is restored to room temperature later, gas after purification is sent in chromatographic column 110 and is detached, finally by the gas after separation
Body is sent into oxygen and carbon isotopes mass spectrograph 111 and is measured.
It repeats above step 3 times, carbon isotope is calculated and oxygen isotope standard deviation is as shown in table 2.
Embodiment 2
It is identical with 1 implementation steps of embodiment, it is derived from NBS-18 the difference lies in sample is used.
It repeats above step 3 times, carbon isotope is calculated and oxygen isotope standard deviation is as shown in table 2.
1 standard sample deviation of table
Table 2
It can be seen that from more than experimental result using detecting system of the present invention, accuracy of detection is high, carbon isotope point
It is reliable to analyse real result, oxygen isotope analysis precision is better than the prior art, and detection speed is fast and is suitable for the inspection of denier sample
It surveys.
It should be noted that embodiment described above is only used for explaining the present invention, do not form to any of the present invention
Limitation.By referring to exemplary embodiments, invention has been described, it should be appreciated that word used in it is descriptive
With explanatory vocabulary rather than limited vocabulary.The present invention can be made within the scope of the claims by regulation
It changes and the present invention is revised in without departing substantially from scope and spirit of the present invention.Although the present invention described in it relates to
And specific method, material and embodiment, it is not intended that the present invention is limited to wherein disclosed particular case, on the contrary, this hair
It is bright to can be extended to other all methods and applications with identical function.
Claims (10)
1. a kind of oxygen and carbon isotopes detecting system for carbonate rock, including：
Laser sample-melting device, purification enrichment device and separation detecting device, wherein the laser sample-melting device is infrared laser
Micro- sample-melting device.
2. detecting system according to claim 1, which is characterized in that the infrared laser sample-melting device includes infrared laser
Device and sample room；The infrared laser is located at the top of the sample room, and the sample room both ends are connected with the gas that can circulate
The pipeline of body, wherein one end are connect with the de-watering apparatus in the purification enrichment device, other end connection carrier gas inlet.
3. detecting system according to claim 1, which is characterized in that the purification enrichment device is included through pipeline successively
The de-watering apparatus of connection, a carbon dioxide-enriched device, gas circuit conversion equipment and secondary enriching and purifying carbon dioxide plant.
4. the detecting system according to claim 1 or 3, which is characterized in that the de-watering apparatus is semipermeable membrane；And/or
The gas circuit conversion equipment is six-way valve.
5. according to claim 1 or 3 or the detecting system, which is characterized in that a carbon dioxide-enriched device is
Cold-trap.
6. according to claim 1 or 3 or the detecting system, which is characterized in that the secondary enriching and purifying carbon dioxide dress
Being set to inner sleeve has the cold-trap of capillary chromatograph.
7. detecting system according to claim 1, which is characterized in that the separation detecting device includes passing sequentially through pipeline
The separator and detection device of connection, the separator are pure by the secondary enrichment in pipeline and the purification enrichment device
Change carbon dioxide plant connection.
8. the detecting system in a kind of 1-7 using claim described in any one carries out the inspection of the oxygen and carbon isotopes of carbonate rock
Survey method, including：
Before sample is melted to sample, sample room air is discharged to other than detecting system, carries out molten sample later, to the production after molten sample
Object carries out carbon dioxide and is once enriched with, the secondary enrichment of carbon dioxide, purifies and detach, based on the carbon dioxide gas finally obtained
Carry out isotope detection.
9. according to the method described in claim 8, it is characterized in that, detect the entire institute for obtaining testing result from proceeding by
It is no more than 12 minutes with the time.
10. a kind of detecting system used according to any one in claim 1-7 is used according in claim 8-9
Application of the method on reservoir exploration described in any one.
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109100452A (en) * | 2018-09-13 | 2018-12-28 | 中国科学院地质与地球物理研究所 | A kind of carbonate coupling isotope test temperature-controlling system and prepare test integrated device |
| CN109596701A (en) * | 2019-01-17 | 2019-04-09 | 中国地质科学院矿产资源研究所 | Method and device for analyzing silicon isotope composition |
| CN114609288A (en) * | 2022-03-21 | 2022-06-10 | 中国科学院地质与地球物理研究所 | Silicate oxygen isotope testing system and method |
| CN114910593A (en) * | 2022-03-14 | 2022-08-16 | 中海油能源发展股份有限公司 | High-temperature molten carbonate enriched carbon dioxide gas purification system and use method thereof |
| CN109596701B (en) * | 2019-01-17 | 2024-05-14 | 中国地质科学院矿产资源研究所 | Method and device for analyzing silicon isotope composition |
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| CN109596701B (en) * | 2019-01-17 | 2024-05-14 | 中国地质科学院矿产资源研究所 | Method and device for analyzing silicon isotope composition |
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