CN103983682A - TIMS measuring method for oxygen isotopes - Google Patents
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- CN103983682A CN103983682A CN201410137411.5A CN201410137411A CN103983682A CN 103983682 A CN103983682 A CN 103983682A CN 201410137411 A CN201410137411 A CN 201410137411A CN 103983682 A CN103983682 A CN 103983682A
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Abstract
The invention relates to a TIMS measuring method for oxygen isotopes. The method comprises the following steps: S1, treatment of a sample; S2, processing of a boat-type tape; S3, pretreatment of the boat-type tape; S4, sample preparation; S5, sample coating; S6, observation of sample coating effects; S7, cleaning of a sample room and a flight-path tube; S8, sample filling; S9, selection and arrangement of receivers; S10, adjustment of evaporation and ionization temperatures; S11, optimization of optical parameters; S12, data acquisition; and S13, correction and uncertainty calculation of a measured value obtained in the step S12. The TIMS measuring method for oxygen isotopes has the characteristics of simple sample preparation, a small usage amount of the sample, accurate measurement, high measurement precision, a fast measurement speed, etc.
Description
Technical field
The present invention relates to isotope measure technical field, relate in particular to a kind of oxygen isotope TIMS measuring method.
Background technology
Along with international prevention of nuclear proliferation, antinucleus probably and the development of nuclear safeguards situation, core security has become international concern focus.Within 2010 and 2012, hold Nuclear Security Summit, relevant international prevention of nuclear proliferation, antinucleus have mainly been discussed and the nuclear safety problem such as have been feared.As the method for nuclear material information characteristics diagnostic analysis---core method card is learned the attention that is more and more subject to national governments and public organization.The early 1990s in last century, the relevant black case of nuclear material is seen in report.Be mainly due to after the Soviet Union's dissolution, cause the confusion in nuclear material management, and then occur loss and the illegal transaction of nuclear fuel element, nuclear material or radioactive material, make nuclear non-proliferation situation become very severe.The black appearance of nuclear material, international community is except the nuclear proliferation to traditional is worried, the public also worries that terrorist may utilize core or radioactivity disperser to start to attack.Since first intercepting and capturing smuggling nuclear material case, illegally transport the extremely common people's concern of nuclear material and radioactive material, the sum that illegal nuclear material is transported goods for sale event presents the situation of rising.For black nuclear material is tracked down, review its source, to strengthen management, the core method of having arisen at the historic moment card is learned this emerging comprehensive branch of learning.
Core method card Epidemiological Analysis is from nuclear material is intercepted and captured at scene, learn the analysis of the characteristic attribute such as technology, the principal ingredient that method is carried out sample of confirming by core method card, and compare with the information of database, review suspicious specimen source, transport pathway, investigate case-involving organization and individual, for detection and the processing of case provide abundant information.Characteristic attribute, generally comprises radioactive type, radioactivity, principal ingredient, isotopic abundance, dopant species and content, macro-size, micromechanism etc.Sometimes can not accurately trace to the source by conventional characteristic attribute, need to analyze more characteristic attribute, oxygen is exactly a principal character element for geo-location.Because change according to the composition of oxygen isotope in seawater or rainwater, different regions, due to geographic position, have caused natural oxygen isotope to have small difference at occurring in nature content, and difference is approximately 1%~5%.
The measuring method of carrying out at present oxygen isotope ratio in uranium oxide is abroad mainly gas mass spectroscopy, TIMS method and SIMS method, and domestic carried out gas mass spectroscopy and measure the method for oxygen isotope in uranium oxide.Gas mass spectroscopy is conventional, classical oxygen isotope measuring method.TIMS method, compared with gas mass spectroscopy, does not need to carry out the chemical treatment of sample, can directly measure, and has the features such as analysis speed is fast, sample preparation is simple, amount of samples is little.TIMS is by receiving UO
+measure, do not need to transform CO
2gas is measured again, has reduced intermediate link, has reduced the introducing factor of end product uncertainty, can meet core method card and learn about feature quick, accurate analysis.
" data correcting method when a kind of Hydrogen-oxygen Isotope component of measuring water ", application number: CN201210003976.5, the invention provides a kind of data correcting method while measuring Hydrogen-oxygen Isotope component with isotope mass spectrometer, belongs to isotope assay field.Described method is using isotope mass spectrometer to measure in the process of Hydrogen-oxygen Isotope component of water sample to be measured, every standard water sample of one group of water determination to be measured, until measured the raw data that obtains Hydrogen-oxygen Isotope after all water samples to be measured; Then described raw data is sorted, find out the variation tendency of standard water sample, obtain the measurement result of standard water sample according to described variation tendency; Finally, according to the measurement result of standard water sample, the measurement result of water sample to be measured is proofreaied and correct, obtain the measurement result more accurately of the Hydrogen-oxygen Isotope component of water sample to be measured.Convenient operation of the present invention, has considered the variation of reference gas Hydrogen-oxygen Isotope component in mensuration process effectively, has reduced to the full extent its impact on measurement result, has improved the accuracy of measurement result.
But, often prior art do not have advantages of for gas mass spectroscopy measure when oxygen isotope that amount of samples is little, chemical treatment and measuring process fairly simple, and do not there is the selection by carrier band agent, the research that is coated with sample technology and research and the optimization of other measuring conditions, set up one fast, the advantage of the method for oxygen isotope in Measurement accuracy uranium oxide.
In view of above-mentioned defect, creator of the present invention has obtained this creation finally through long research and practice.
Summary of the invention
The object of the present invention is to provide a kind of oxygen isotope TIMS measuring method, in order to overcome above-mentioned technological deficiency.
For achieving the above object, the invention provides a kind of oxygen isotope TIMS measuring method, described method comprises:
Step S1: sample preparation;
Step S2: the processing of boat type band;
Step S3: complete after described step S2 the pre-treatment of described boat type band;
Step S4: the described sample preparation in described step S1 is become to a suspending liquid sample;
Step S5: the described suspending liquid sample in described step S4 is coated with on the described boat type band of sample in described step S2;
Step S6: the painting sample effect of observing described step S5;
Step S7: complete after described step S6, a sample chamber and a dirft tube are cleaned;
Step S8: complete after described step S5, will bring luggage sample into through the described boat type being coated with after sample;
Step S9: gather one receiver, in order to receive the ion of a uranium oxide ionization;
Step S10: the ion to the ionization of uranium oxide described in described step S9 evaporates, ionization temperature regulates;
Step S11: the ion to the described uranium oxide ionization in described step S10 carries out optical parametric optimization;
Step S12: after described step S11 completes, the ion of described uranium oxide ionization is carried out to data acquisition, in order to obtain measured value;
Step S13: the described measured value obtaining in described step S12 is proofreaied and correct and uncertainty calculation.
Preferably, described uranium oxide is a UO
+ion, described UO
+ion ionizes out one at applicable temperature
238u
18o
+with one
238u
16o
+two ions.
Preferably, the detailed process of described step S1 is: described uranium oxide sample is ground in a grinding alms bowl, the described uranium oxide Sample storage after grinding is full of in the exsiccator of Ar one.
Preferably, described step S2 detailed process is as follows: a groove is set on a wood chopsticks, the center section of described common sample band is placed on the described groove of described wood chopsticks, then the two ends of described common sample band are picked up, form boat type.
Preferably, the optical viewer in described step S6 is one scan electron microscope SEM, in order to observe distribution situation, volume containing the sample, painting sample effect and the reagent volatilization situation of sample on described boat type band.
Preferably, the described sample on described boat type band is measured by a TIMS mass spectrometer.
Preferably, described TIMS mass spectrometer comprises an electron-multiplier and a Faraday cup, and described Faraday cup comprises a Faraday cup AX and a H1 Faraday cup; Described in being used for respectively receiving
238u
16o
+with
238u
18o
+two kinds of ions, and by measuring
238u
18o/
238u
16the ratio of O obtains
18o/
16the ratio of O.
Preferably, described in occurring in described step S10
238u
16o
+after signal, manually adjust voltage and deflection voltage and to D direction and Z direction lens focus, in order to obtain maximum described in
238u
16o
+with described
238u
18o
+two kinds of ion signals.
Preferably, described in described step S11
238u
16o
2 +with described
238u
16o
+ion concentration, under the highest signal intensity and peak shape condition, is moved a process of measurement, and the cycle index of acquisition time, image data and collection is set, and obtains thus a measured value.
Preferably, the formula of the described measured value correction in described step 13 and described uncertainty calculation is as follows respectively:
The computing formula that described measured value is proofreaied and correct is:
Wherein k is correction coefficient;
(
18o/
16o)
correct samplefor sample oxygen isotope
18o/
16the corrected value of O;
(
18o/
16o)
mea samplefor sample oxygen isotope
18o/
16the measured value of O;
The computing formula of described uncertainty is:
The synthetic standards deviation that wherein σ is measured value.
Beneficial effect of the present invention is compared with prior art: the sample band in the present invention is boat type band, therefore described boat type band has the effect of a parcel to described sample, and make described sample difficult drop-off, thereby increase the sample size on described boat type sample band; And by the research such as solution, the optimization of measuring condition to oxygen in environment, set up oxygen isotope TIMS measuring method.The method has that sample preparation is simple, amount of samples is few, measurement is accurate, measuring accuracy is high and the feature such as measuring speed is fast.The method can be applicable to core method card learn in for to the analysis of intercepting and capturing sample oxygen isotope, also can be applicable to verify, surveying work to oxygen isotope in uranium oxide in nuclear safeguards association area simultaneously.
Brief description of the drawings
Fig. 1 is the measurement procedure frame diagram of a kind of oxygen isotope TIMS measuring method of the present invention;
Fig. 2 is a kind of oxygen isotope TIMS measuring method of the present invention
238u
16o
2 +,
238u
16o
+with
238u
+signal intensity and strength of current be related to sketch.
Embodiment
Below in conjunction with accompanying drawing, technical characterictic and the advantage with other above-mentioned to the present invention are described in more detail.
Collect sample, measure the sample on a common sample band by a TIMS mass spectrometer, the described sample on described common sample band is evaporated, due to UO
+the ionization temperature of ion is lower than O
-ionization temperature, therefore select described UO
+as receiving, measuring ion, and make described UO in suitable temperature
+ionize out one
238u
18o
+with one
238u
16o
+two ions, described in use one receiver receives
238u
18o
+ion and described in
238u
16o
+ion, and it is carried out to data acquisition, finally obtain
18o/
16o ratio, thus oxygen isotope ratio in uranium oxide analyzed.
Refer to shown in Fig. 1, its measurement procedure frame diagram that is a kind of oxygen isotope TIMS measuring method of the present invention, described method comprises the steps:
Step S1: sample preparation: after described uranium oxide sample reception, appropriate described uranium oxide sample is ground in a grinding alms bowl, object both can have been removed the oxide layer of described sample surfaces, can make again described uranium oxide sample evenly, particle diameter diminishes, be conducive to the later stage to be coated with sample.Described Sample storage after grinding is full of in the exsiccator of Ar one, stand-by.
Step S2: the processing of boat type band: process a groove being of moderate size on a wood chopsticks, be that 8mm, the wide described common sample band for 0.86mm, the thick 0.026mm of being are placed on the described groove of described wood chopsticks by a length, the centre position of described common sample band is pressed on the described groove that sulculus is placed on described wood chopsticks with a screwdriver, then with one tweezers the common two ends of stating sample band pick up, form thus a boat type.In the time that the hanging drop that contains described sample arrives the described centre position of described boat type band, when described boat type band shifts and is installed on a specimen holder again, described boat type band plays the effect of parcel to described sample, therefore described sample difficult drop-off, thus the described sample size on described sample band increased.
Step S3: boat type band pre-treatment: after described boat type band processing, before being coated with sample, described sample band need to carry out degasification in a getter, and described getter in the degasification condition that described boat type band is carried out in degassing procedure is: 1 × 10
-7in Pa vacuum bakeout system, carry out degasification.Described degassing procedure both can have been removed the moisture on described boat type band, removed oxygen, also can remove the easily pollution element such as organism, Na, K and Zn simultaneously.Described boat type band after degasification is kept in the described exsiccator that is full of Ar; Thus described boat type band and described common sample band, aspect the collimation between continuation and the parallel sample of signal intensity, signal, are listed in to table 1, described boat type band is all better than described common sample band far away aspect above-mentioned three, please refer to shown in table 1:
Table 1
Step S4: sample preparation: get sample after the described grinding of about Microgram, sample after described grinding is put into a polyethylene bottle, add a cyclohexane reagent of approximately 20 μ l, therefore make suspending liquid, described cyclohexane reagent is anaerobic reagent, mainly that powdered samples is worked to make suspending liquid, transferred particle, simultaneously described cyclohexane reagent not can with described sample in oxygen exchange, the composition itself containing also can not have impact to measurement result.
Step S5: be coated with sample: the described suspending liquid sample of vibration preparation, leave standstill 1 minute, use a pipettor to get supernatant liquor, drip in the middle part of described boat type band, after described supernatant liquor evaporation, then get described hanging drop in described boat type band middle part, repeat several times.Be coated with after sample, described sample is placed one day under room temperature environment, after organic reagent volatilization, then carries out SEM observation and TIMS measurement, and described SEM is one scan electron microscope.
Step S6: be coated with sample effect observation: use described SEM to observe the described sample on described boat type band, be mainly used in observing the distribution situation of the described powdered sample on described boat type band and volume containing the sample, painting sample effect, reagent whether to be evaporated completely congruence, to check the described painting sample effect in described step S5.
Step S7: the cleaning of sample chamber and dirft tube: carrying out before described TIMS measurement, use high-purity N
2gas rinses 2-3 time described sample chamber and described dirft tube, and detailed process is: be filled with described high-purity N
2gas, pumping high vacuum, then be filled with described high-purity N
2gas, pumping high vacuum, repeats successively.
Step S8: dress sample: after completing described step S5, described sample is installed on described specimen holder, and is fixed by a screw, then described specimen holder is installed in the sample chamber of described TIMS, and described sample is fixed.
Step S9: the gather of receiver: described TIMS comprises an electron-multiplier and two kinds of data sinks of a Faraday cup, does not have cup poor between described Faraday cup, and stable, due to described
238u
18o
+with described
238u
16o
+counting can reach the reception requirement of described Faraday cup, therefore select described in described Faraday cup AX receives
238u
16o
+, described in described H1 Faraday cup receives
238u
18o
+, by measuring
238u
18o/
238u
16the ratio of O, obtains
18o/
16the ratio of O.
Step S10: evaporation, ionization temperature regulate: refer to shown in Fig. 2, it is a kind of oxygen isotope TIMS measuring method of the present invention
238u
16o
2 +,
238u
16o
+with
238u
+signal intensity and strength of current be related to sketch,
This method sample band structure adopts single band mensuration, and when described TIMS measures, evaporation, the ionization temperature of described boat type band are embodied by the strength of current being carried on described boat type band.
In uranium oxide ionization process, described in generating respectively
238u
16o
2 +, described in
238u
16o
+with one
238u
+three kinds of ions, this method adopts to be measured
238u
18o/
238u
16o obtains
18o/
16the ratio of O, therefore, in the situation that described sample size is certain, wishes to obtain described UO
+at most, signal is the strongest.But, due to described
238u
16o
2 +, described in
238u
16o
+with described
238u
+ionization energy difference, ionization temperature difference, studies the formation ratio of described three kinds of ions under different temperatures, is chosen in described UO
+when formation ratio is the highest, carry out the measurement of oxygen isotope.In the time evaporating and ionization temperature is approximately 1000 DEG C, start described in record
238u
16o
2 +, described in
238u
16o
+with described
238u
+signal intensity, extremely described sample runs out of, by measuring described in described uranium oxide
238u
16o
2 +, described in
238u
16o
+with described
238u
+signal, can obtain the suitable ionization temperature of described three kinds of ions, the three that also can calculate described uranium oxide simultaneously forms ratio.
In the time of 1300 DEG C, described in
238u
16o
2 +there is signal in ion, along with the rising of ionization temperature, signal starts to increase at first, in the time of 1673 DEG C, described in
238u
16o
2 +the signal intensity of ion approaches 10V, and while lasting till 1740 DEG C, along with the increase of ionization temperature, signal starts to decline, and illustrates that now ionization temperature is higher than described
238u
16o
2 +the ionization temperature of ion.Described
238u
16o
+the signal occurrence law of ion with described in
238u
16o
2 +the rule of ion is basic identical, the translation backward of signal entirety.In the time that temperature reaches 1400 DEG C, described in starting to occur
238u
16o
+ion signal, in the time that strength of current is 1740 DEG C, signal intensity is greater than 10V, lasts till 1853 DEG C, after this, and along with the rising of signal ionization temperature, described UO
+ion signal declines and is unstable, illustrates that now ionization temperature is higher than described
238u
16o
+the ionization temperature of ion.In the time that strength of current is 1713 DEG C, described in
238u
+ion signal intensity is 29mV, and along with the increase of strength of current, signal starts to increase later, and in the time that strength of current is 1933 DEG C, signal intensity is 4V, and because sample size consumption in early stage is a lot, along with the increase of strength of current, signal declines also very fast.
Step S11: the optimization of optical parametric: described in occurring in described step S10
238u
16o
+after signal, manually adjust ion gun place voltage, extract the parameter such as focusing and deflection voltage, Z direction lens focus and deflection voltage and slit place voltage of voltage, D direction lens, obtain maximum described in
238u
16o
+with described
238u
18o
+the signal of two kinds of ions.
Step S12: data acquisition: described in described step S11
238u
16o
2 +with described
238u
16o
+ion concentration is under the highest signal intensity and perfect peak shape condition, described in described center Faraday cup AX receives
238u
16o
+ion, described in described H1 Faraday cup receives
238u
18o
+ion, operating measurement program, the acquisition time that each data are set is 1s, 5 data of each circle collection, gather 10 circulations altogether, totally 50 data, described 50 data are image data, obtain thus measured value.
Step S13: the described measured value in described step S12 is proofreaied and correct and uncertainty calculation: owing to there being the influence factor such as mass fractionation, space charge effect, make to there are differences between described measured value in described step S12 and actual value, need to proofread and correct described measured value with standard substance.Described trimming process is: first use mass spectrometer measurement standard material
18o/
16o ratio, utilizes formula (1) to calculate correction coefficient k, and recycling k value is proofreaied and correct the measurement result of oxygen isotope ratio in described sample, as formula (2).
As shown in formula (1) and formula (2)
Wherein:
(
18o/
16o)
true standardfor the oxygen isotope of oxygen isotope standard substance
18o/
16the reference value of O ratio;
(
18o/
16o)
mea standardfor the oxygen isotope of oxygen isotope standard substance
18o/
16the measured value of O;
K is correction coefficient;
(
18o/
16o)
correct samplefor sample oxygen isotope
18o/
16the corrected value of O;
(
18o/
16o)
mea samplefor sample oxygen isotope
18o/
16the measured value of O.
The uncertainty calculation of described measured value, its calculating standard is: the measurement standard deviation (σ of measured value
mea), the measurement standard deviation (σ of measurement standard material
standard) and the uncertainty (W of standard substance
true standard);
Measurement standard deviation (the σ of described measured value
mea) use following formula (3) to calculate
The synthetic standards deviation of measured value is used following formula (4) to calculate
The uncertainty of described sample is used following formula (5) to calculate
Step S14: pass through thus the calculating of described formula (1), (2), (3), (4) and (5), draw the final measurement of described sample, that is: the uncertainty of described corrected value and described measured value.
The TIMS measuring method of a kind of oxygen isotope provided by the invention, the research such as optimization by the solution to oxygen in environment, measuring condition, has set up a kind of TIMS measuring method of oxygen isotope.The method has that sample preparation is simple, amount of samples is few, measurement is accurate, measuring accuracy is high and the feature such as measuring speed is fast.The method can be applicable to core method card learn in for to the analysis of intercepting and capturing sample oxygen isotope, also can be applicable to verify, surveying work to oxygen isotope in uranium oxide in nuclear safeguards association area simultaneously.
The foregoing is only preferred embodiment of the present invention, is only illustrative for invention, and nonrestrictive.Those skilled in the art is understood, and in the spirit and scope that limit, can carry out many changes to it in invention claim, amendment, and even equivalence, but all will fall within the scope of protection of the present invention.
Claims (10)
1. an oxygen isotope TIMS measuring method, is characterized in that, described method comprises:
Step S1: sample preparation;
Step S2: the processing of boat type band;
Step S3: complete after described step S2 the pre-treatment of described boat type band;
Step S4: the described sample preparation in described step S1 is become to a suspending liquid sample;
Step S5: the described suspending liquid sample in described step S4 is coated with on the described boat type band of sample in described step S2;
Step S6: the painting sample effect of observing described step S5;
Step S7: complete after described step S6, a sample chamber and a dirft tube are cleaned;
Step S8: complete after described step S5, will bring luggage sample into through the described boat type being coated with after sample;
Step S9: gather one receiver, in order to receive the ion of a uranium oxide ionization;
Step S10: the ion to the ionization of uranium oxide described in described step S9 evaporates, ionization temperature regulates;
Step S11: the ion to the described uranium oxide ionization in described step S10 carries out optical parametric optimization;
Step S12: after described step S11 completes, the ion of described uranium oxide ionization is carried out to data acquisition, in order to obtain measured value;
Step S13: the described measured value obtaining in described step S12 is proofreaied and correct and uncertainty calculation.
2. oxygen isotope TIMS measuring method according to claim 1, is characterized in that, described uranium oxide is a UO
+ion, described UO
+ion ionizes out one at applicable temperature
238u
18o
+with one
238u
16o
+two ions.
3. oxygen isotope TIMS measuring method according to claim 1 and 2, it is characterized in that, the detailed process of described step S1 is: described uranium oxide sample is ground in a grinding alms bowl, the described uranium oxide Sample storage after grinding is full of in the exsiccator of Ar one.
4. oxygen isotope TIMS measuring method according to claim 1, it is characterized in that, described step S2 detailed process is as follows: a groove is set on a wood chopsticks, the center section of described common sample band is placed on the described groove of described wood chopsticks, then the two ends of described common sample band are picked up, form boat type.
5. oxygen isotope TIMS measuring method according to claim 4, it is characterized in that, optical viewer in described step S6 is one scan electron microscope SEM, in order to observe distribution situation, volume containing the sample, painting sample effect and the reagent volatilization situation of sample on described boat type band.
6. according to the oxygen isotope TIMS measuring method described in claim 2 or 3, it is characterized in that, the described sample on described boat type band is measured by a TIMS mass spectrometer.
7. oxygen isotope TIMS measuring method according to claim 6, is characterized in that, described TIMS mass spectrometer comprises an electron-multiplier and a Faraday cup, and described Faraday cup comprises a Faraday cup AX and a H1 Faraday cup; Described in being used for respectively receiving
238u
16o
+with
238u
18o
+two kinds of ions, and by measuring
238u
18o/
238u
16the ratio of O obtains
18o/
16the ratio of O.
8. oxygen isotope TIMS measuring method according to claim 1, is characterized in that, described in occurring in described step S10
238u
16o
+after signal, manually adjust voltage and deflection voltage and to D direction and Z direction lens focus, in order to obtain maximum described in
238u
16o
+with described
238u
18o
+two kinds of ion signals.
9. according to the oxygen isotope TIMS measuring method described in claim 2 or 3, it is characterized in that, described in described step S11
238u
16o
2 +with described
238u
16o
+ion concentration, under the highest signal intensity and peak shape condition, is moved a process of measurement, and the cycle index of acquisition time, image data and collection is set, and obtains thus a measured value.
10. oxygen isotope TIMS measuring method according to claim 2, is characterized in that, the described measured value correction in described step 13 and the formula of described uncertainty calculation are as follows respectively:
The computing formula that described measured value is proofreaied and correct is:
Wherein, k is correction coefficient;
(
18o/
16o)
correct samplefor sample oxygen isotope
18o/
16the corrected value of O;
(
18o/
16o)
mea samplefor sample oxygen isotope
18o/
16the measured value of O;
The computing formula of described uncertainty is:
The synthetic standards deviation that wherein σ is measured value.
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CN108037172A (en) * | 2017-11-10 | 2018-05-15 | 中国科学院广州地球化学研究所 | The method that one kind carries out analysis at the same time based on large-scale Secondary Ion Mass Spectrometry to " water " content in zircon and oxygen isotope |
CN108037172B (en) * | 2017-11-10 | 2019-12-06 | 中国科学院广州地球化学研究所 | Method for simultaneously analyzing water content and oxygen isotope in zircon based on large-scale secondary ion mass spectrometry |
CN109900771A (en) * | 2017-12-08 | 2019-06-18 | 核工业北京地质研究院 | A kind of measuring method of uranium isotope ratio |
CN109900771B (en) * | 2017-12-08 | 2021-10-19 | 核工业北京地质研究院 | Method for determining uranium isotope ratio |
CN112098396A (en) * | 2020-09-16 | 2020-12-18 | 中国科学院地质与地球物理研究所 | Method for detecting zircon hafnium isotope |
CN112098396B (en) * | 2020-09-16 | 2021-08-24 | 中国科学院地质与地球物理研究所 | Method for detecting zircon hafnium isotope |
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