A target sample based on an extraterrestrial sample combined process and a preparation method thereof

Abstract

The application belongs to the technical field of extraterrestrial sample testing, and discloses a target sample based on an extraterrestrial sample combined process and a preparation method thereof, wherein the preparation method comprises obtaining mixed eluent containing Be, Al, Na and Ca, eluent containing Mn and eluent containing Fe through an anion resin exchange method, obtaining eluent containing Na, eluent containing Be and mixed eluent containing Al and Ca based on the mixed eluent containing Be, Al, Na and Ca through a cation resin exchange method, and preparing Al2O3 target sample, CaF2 target sample, BeO target sample, Fe2O3 target sample, sodium salt target sample and MnO2 target sample based on the mixed eluent containing Al and Ca, the eluent containing Be, the eluent containing Fe, the eluent containing Na and the eluent containing Mn; the application can realize efficient separation and extraction of multiple nuclides in the same process, and can reduce the amount of extraterrestrial sample to less than 50 mg.

Description

Technical Field

[0001] This invention relates to the field of extraterrestrial sample testing technology, specifically to a target sample and its preparation method based on an extraterrestrial sample combined process. Background Technology

[0002] Extraterrestrial samples refer to materials originating from celestial bodies outside Earth. They carry original information about the formation and evolution of the solar system, like time capsules of the universe. Studying extraterrestrial samples not only deepens human understanding of the universe but also provides crucial comparative evidence for the origin and evolution of Earth, serving as an important cornerstone of planetary science.

[0003] Cosmogenic nuclides (such as) 10 Be、 22 Na、 26 Al、 41 Ca, 53 Mn and 60 The analysis and determination of cosmogenic nuclides (such as Fe) are important quantitative techniques for planetary science research. For meteorite samples, by measuring the concentration of cosmogenic nuclides in the meteorite samples, we can understand important information such as the space irradiation history of the meteorite samples in the solar system and the age of the meteorite samples after landing on the Earth's surface. For lunar samples (lunar soil), cosmogenic nuclides can provide important evidence for lunar surface exposure dating, cosmic ray energy spectrum analysis in the Milky Way, and research on novae and supernova explosions near the Earth and Moon.

[0004] Current methods for measuring cosmogenic nuclides rely on accelerator mass spectrometry (AMS), requiring the separation and purification of nuclides from extraterrestrial samples using chemical pretreatment techniques to prepare appropriate measurement targets before testing. Among these methods, the greatest interference in accelerator mass spectrometry measurements originates from isotopes. Therefore, ensuring the effective separation of the analyte and isotopes (e.g.,...) is crucial. 10 Be and 10 B. 53 Mn and 53 Cr 60 Fe and 60 Ni (etc.) is key to improving measurement sensitivity.

[0005] However, for extraterrestrial samples (silicate samples), the existing chemical pretreatment process involves: completely dissolving the sample in acid, then separating and purifying the analyte using ion exchange, liquid-liquid extraction, and precipitation to remove interference from isotopes. The resulting solid powder target is then prepared by precipitation, mixed with an auxiliary medium, and pressed into a target cone for subsequent AMS analysis. This process is relatively complex and can only extract one or two nuclides, resulting in low utilization of extraterrestrial samples.

[0006] Therefore, there is an urgent need for a new technology that can solve the problem of not being able to achieve efficient separation and extraction in the same process. Summary of the Invention

[0007] The purpose of this invention is to provide a target sample and its preparation method based on a combined extraterrestrial sample process, in order to overcome the problems existing in the prior art. This invention can achieve... 10 Be、 22 Na、 26 Al、 41 Ca, 53 Mn and 60 Highly efficient separation and extraction of Fe polynucleotides using the same process.

[0008] To achieve the above objectives, the technical solution adopted by the present invention is as follows:

[0009] In a first aspect, the present invention provides a target sample preparation method based on a combined extraterrestrial sample process, comprising the following steps:

[0010] Step 1: Take an extraterrestrial sample for digestion, and then remove fluoride from the digested extraterrestrial sample to obtain the first product;

[0011] Step 2: Based on the first product, an anion exchange resin method is used to obtain a mixed eluent containing Be, Al, Na and Ca, an eluent containing Mn and an eluent containing Fe.

[0012] Step 3: Based on the mixed eluent containing Be, Al, Na and Ca, the following eluents are obtained by cation exchange resin method: Na-containing eluent, Be-containing eluent and Al and Ca-containing mixed eluent.

[0013] Step 4: Based on the mixed eluent containing Al and Ca, a supernatant containing Ca and Al(OH)3 precipitate are obtained; based on the eluent containing Be and the eluent containing Fe, Be(OH)2 precipitate and Fe(OH)3 precipitate are obtained, respectively.

[0014] Step 5: Prepare BeO target sample, Fe2O3 target sample and Al2O3 target sample based on Be(OH)2 precipitate, Fe(OH)3 precipitate and Al(OH)3 precipitate respectively; prepare sodium salt target sample based on Na eluent; prepare CaF2 target sample based on Ca-containing supernatant; prepare MnO2 target sample based on Mn-containing eluent.

[0015] In some embodiments, the digestion of the off-site samples and the removal of fluoride from the digested off-site samples specifically include:

[0016] The extraterrestrial sample, carrier, first HNO3 and first HF are mixed to obtain a mixed solution. The mixed solution is subjected to a first heating reaction and a first evaporation treatment in sequence. Then, second HF is added and the second heating reaction and second evaporation treatment are carried out in sequence to obtain the digested extraterrestrial sample.

[0017] After adding HNO3, ultrapure water and HClO4 to the digested extraterrestrial sample, a third evaporation process was performed. The product from the third evaporation process was then dissolved in a first solution, and the first dissolved product was centrifuged in a first process to obtain the first product.

[0018] In some embodiments, the carrier includes 9 Be carrier, 23 Na carrier, 55 Mn carrier, 27 Al carrier, 56 Fe carrier, 40 Three or more Ca carriers;

[0019] The concentration of the first HNO3 is 16.5 mol / L; the concentration of the first HF is 22.5 mol / L; the concentration of the second HF is 22.5 mol / L;

[0020] The ratio of the amount of extraterrestrial sample, the first HNO3, the first HF, and the second HF added is (10-50) mg : (0.1-0.3) mL : (0.9-1.1) mL : (0.9-1.1) mL;

[0021] The temperature of both the first and second heating reactions is 140-160 ℃, and the time of both the first and second heating reactions is 4-6 h.

[0022] The temperature of the first, second, and third evaporation treatments is 200-220 ℃, and the time of the first, second, and third evaporation treatments is 1-1.5 h.

[0023] The concentration of the second HNO3 is 16.5 mol / L; the volume ratio of the second HNO3, ultrapure water, and HClO4 is (0.15-0.35) mL : (0.15-0.35) mL : (0.4-0.6) mL;

[0024] The first dissolution uses a first HCl solution with a concentration of 10 mol / L;

[0025] The first centrifugation process is carried out at a speed of 2500-3500 rpm for 4-6 minutes.

[0026] In some embodiments, the 27 Al carrier, 56 Fe carrier and 40Whether to add a Ca carrier depends on the actual content of Al, Ca, and Fe in the extraterrestrial sample. The content of each element in the lunar sample comes from relevant literature. For example, the content of Al2O3 in the lunar sample is 11.4%, FeO is 22.7%, CaO is 11.5%, Na2O is 0.42%, and MnO is 0.28%. To ensure that the amount of each element injected into the target sample is 1-3 mg, no carrier is added when taking 50 mg of lunar sample. 27 Al carrier, 56 Fe carrier and 40 Ca carrier; when taking 30 mg or 10 mg lunar samples, add 27 Al support; for example, in a chondrite sample, the contents of Al2O3 are 2.08%, FeO is 7.84%, CaO is 1.89%, Na2O is 0.85%, and MnO is 0.29%. To ensure that the amount of each element pressed into the target sample is 1-3 mg, when taking 40 mg of chondrite sample, Al support is added. 40 Ca carrier and 27 Al-carrier.

[0027] In some embodiments, the process of obtaining a mixed eluent containing Be, Al, Na, and Ca, an eluent containing Mn, and an eluent containing Fe based on the first product via anion exchange resin specifically includes:

[0028] The anion exchange column is equilibrated, and the first product is added to the equilibrated anion exchange column to obtain the anion exchange column after the addition of the first product. The anion exchange column after the addition of the first product is subjected to a first elution to obtain a mixed eluent containing Be, Al, Na and Ca.

[0029] The anion exchange column after the first elution was subjected to a second elution to obtain an eluent containing Mn.

[0030] The anion exchange column after the second elution was subjected to a third elution to obtain an eluent containing Fe.

[0031] In some embodiments, the balanced anion exchange column uses a second HCl solution with a concentration of 10 mol / L and a column volume of 1 column volume.

[0032] The first elution uses a third HCl solution with a concentration of 10 mol / L, and the sum of the volumes of the third HCl solution and the first product is 1.5 column volumes.

[0033] The second elution uses a fourth HCl solution with a concentration of 7 mol / L; the third elution uses a fifth HCl solution with a concentration of 0.1 mol / L; the column volume ratio of the fourth HCl solution to the fifth HCl solution is 2:4.

[0034] The column volume ratio of the mixed eluent containing Be, Al, Na and Ca, the eluent containing Mn, and the eluent containing Fe is 1.5:2:4.

[0035] In some embodiments, the process of obtaining Na-containing eluent, Be-containing eluent, and Al and Ca-containing mixed eluent via cation exchange using a mixed eluent containing Be, Al, Na, and Ca specifically includes:

[0036] The mixed eluent containing Be, Al, Na and Ca was subjected to a fourth evaporation to dryness, the product of the fourth evaporation to dryness was subjected to a second dissolution, and the product of the second dissolution to be subjected to a second centrifugation to obtain the second product.

[0037] Equilibrate the cation exchange column, add the second product to the equilibrated cation exchange column, and obtain the cation exchange column after adding the second product. Perform a fourth elution on the cation exchange column after adding the second product to obtain the eluent containing Na.

[0038] The cation exchange column after the fourth elution was subjected to a fifth elution to obtain a Be-containing eluent;

[0039] The cation exchange column after the fifth elution was subjected to a sixth and seventh elution in sequence to obtain a mixed eluent containing Al and Ca.

[0040] In some embodiments, the temperature of the fourth evaporation treatment is 140-160 °C, and the time of the fourth evaporation treatment is 4-6 h;

[0041] The second dissolution uses a sixth HCl solution and a first hydrogen peroxide solution, the concentration of the sixth HCl solution being 6 mol / L; the volume ratio of the sixth HCl solution to the first hydrogen peroxide solution is 1 mL: 0.05 mL;

[0042] The second centrifugation process is carried out at a speed of 2500-3500 rpm for 4-6 minutes.

[0043] The balanced cation exchange column uses one column volume of the seventh HCl solution, with a concentration of 1 mol / L.

[0044] The fourth elution uses the eighth HCl solution, which has a concentration of 1 mol / L, and the sum of the volumes of the eighth HCl solution and the second product is 4 column volumes.

[0045] The fifth elution uses the ninth HCl solution with a concentration of 1 mol / L; the sixth elution uses the tenth HCl solution with a concentration of 1 mol / L; the seventh eleventh HCl solution uses the eleventh HCl solution with a concentration of 2.5 mol / L; the column volume ratio of the ninth, tenth, and eleventh HCl solutions is 5:5:4.

[0046] The column volume ratio of the Na-containing eluent, the Be-containing eluent, and the mixed Al and Ca eluent is 4:5:4.

[0047] In some embodiments, the process of obtaining a Ca-containing supernatant and Al(OH)3 precipitate based on a mixed eluent containing Al and Ca, and obtaining Be(OH)2 precipitate and Fe(OH)3 precipitate based on a Be-containing eluent and a Fe-containing eluent, respectively, specifically includes:

[0048] The mixed eluent containing Al and Ca was subjected to a fifth evaporation treatment. The product from the fifth evaporation treatment was then dissolved in a third solution. The pH of the third dissolved product was adjusted to 8-9 and then subjected to a first vortex treatment and a third centrifugation treatment in sequence to obtain a Ca-containing supernatant and an Al(OH)3 precipitate.

[0049] The Be-containing eluent and the Fe-containing eluent were subjected to a sixth evaporation treatment. The products from the two sixth evaporation treatments were then dissolved in the fourth solution. The pH of the two fourth solution products was adjusted to 8-9, and then they were subjected to a second vortex treatment and a fourth centrifugation treatment in sequence. The products from the two fourth centrifugation treatments were then washed in the second wash to obtain Be(OH)2 precipitate and Fe(OH)3 precipitate, respectively.

[0050] In some embodiments, the temperature of the fifth drying treatment is 140-160 °C, and the time of the fifth drying treatment is 4-6 h;

[0051] The third dissolution uses a twelfth HCl solution and a second hydrogen peroxide solution, the concentration of the twelfth HCl solution being 6 mol / L; the volume ratio of the twelfth HCl solution to the second hydrogen peroxide solution is 1 mL: 0.05 mL;

[0052] The temperature of the sixth drying treatment is 140-160 ℃, and the time of the sixth drying treatment is 4-6 h;

[0053] The fourth dissolution uses a thirteenth HCl solution and a third hydrogen peroxide solution, with the concentration of the thirteenth HCl solution being 6 mol / L; the volume ratio of the thirteenth HCl solution to the third hydrogen peroxide solution is 1 mL: 0.05 mL.

[0054] The rotational speed of both the first and second vortex processes is 1500 rpm, and the time of both the first and second vortex processes is 10-15 s.

[0055] The rotation speed of the third and fourth centrifugation processes is 2500-3500 rpm, and the time for both processes is 4-6 min.

[0056] In some embodiments, the preparation of BeO target samples, Fe2O3 target samples, and Al2O3 target samples based on Be(OH)2 precipitation, Fe(OH)3 precipitation, and Al(OH)3 precipitation, respectively; the preparation of sodium salt target samples based on Na eluent; the preparation of CaF2 target samples based on Ca-containing supernatant; and the preparation of MnO2 target samples based on Mn-containing eluent specifically include:

[0057] After dissolving Be(OH)2 precipitate, Fe(OH)3 precipitate and Al(OH)3 precipitate with HNO3, respectively, they were subjected to a seventh evaporation and a first calcination to obtain BeO, Fe2O3 and Al2O3, respectively. BeO, Fe2O3 and Al2O3 were then mixed with equal volumes of niobium powder, silver powder and copper powder to obtain BeO target sample, Fe2O3 target sample and Al2O3 target sample, respectively.

[0058] The Na-containing eluent was subjected to an eighth evaporation process, and the product from the eighth evaporation process was dissolved in a fifth process to obtain a third product. The third product was evaporated until all sodium salt crystals precipitated. The sodium salt crystals were mixed with an equal volume of silver powder to obtain a sodium salt target sample.

[0059] Acidification reaction was carried out by adding HNO3 to the Ca-containing supernatant. After the gas bubbles in the acidification reaction stopped being generated, HF was added to obtain the fourth product. The fourth product was subjected to the third vortex treatment and then subjected to the first settling and fifth centrifugation treatments to obtain CaF2. CaF2 was mixed with an equal volume of silver powder to obtain the CaF2 target sample.

[0060] The Mn-containing eluent was subjected to a ninth evaporation treatment, and the product from the ninth evaporation treatment was dissolved in a sixth process. Sodium hydroxide was added to the product from the sixth dissolution treatment, and the product was subjected to a fourth vortex treatment, a second settling treatment, a sixth centrifugation treatment, and a second calcination treatment in sequence to obtain MnO2. The MnO2 was then mixed with an equal volume of silver powder to obtain the MnO2 target sample.

[0061] In some embodiments, the concentration of the third HNO3 is 16.5 mol / L;

[0062] The temperature of the seventh evaporation treatment is 140-160 ℃, and the time of the seventh evaporation treatment is 0.5-1 h; the temperature of the first calcination is 800-1000 ℃, and the time of the first calcination is 1.5-2.5 h;

[0063] The fifth dissolution uses pure water; the evaporation temperature is 90-110 ℃, and the evaporation time is 20-40 min;

[0064] The concentration of the fourth HNO3 is 16.5 mol / L; the acidification reaction time is 30-60 min;

[0065] The concentration of the third HF is 22.5 mol / L; the volume ratio of the Ca-containing supernatant, the fourth HNO3, and the third HF is 3:2:1;

[0066] The first settling time is 12 h; the temperature of the eighth and ninth evaporation treatments is 140-160 ℃, and the time of the eighth and ninth evaporation treatments is 2-4 h.

[0067] The sixth dissolution uses the fourteenth HCl solution, the concentration of which is 12 mol / L; the ratio of the fourteenth HCl solution to sodium hydroxide is 1 mL: (0.5-1) g.

[0068] The rotational speed of the third and fourth vortex processes is 1500 rpm, and the time of the third and fourth vortex processes is 10-15 s.

[0069] The second settling time is 30 min; the speed of the fifth and sixth centrifugation treatments is 2500-3500 rpm, and the time of the fifth and sixth centrifugation treatments is 4-6 min; the temperature of the second ignition is 800-1000 ℃, and the time of the second ignition is 1.5-2.5 h.

[0070] Secondly, the present invention provides a target sample based on an extraterrestrial sample joint process, which is obtained based on the target sample preparation method based on the aforementioned extraterrestrial sample joint process.

[0071] The above technical solution has the following advantages or beneficial effects:

[0072] In a first aspect, this invention provides a target preparation method based on a combined extraterrestrial sample process. Through anion exchange and cation exchange methods, mixed eluents containing Be, Al, Na, and Ca, Mn-containing eluents, Fe-containing eluents, Na-containing eluents, Be-containing eluents, and mixed eluents containing Al and Ca are obtained, respectively. The mixed eluents containing Al and Ca are then converted into Ca-containing supernatant and Al(OH)3 precipitate, and the Be-containing and Fe-containing eluents are converted into Be(OH)2 precipitate and Fe(OH)3 precipitate, respectively. Finally, BeO target samples, Fe2O3 target samples, Al2O3 target samples, sodium salt target samples, CaF2 target samples, and MnO2 target samples are prepared, achieving… 10 Be、 22 Na、 26 Al、 41 Ca, 53 Mn and 60 Highly efficient separation and extraction of Fe nuclides using the same process.

[0073] In some embodiments, extraterrestrial samples are mixed with several carriers and acid solutions (first HNO3, first HF, second HF, second HNO3 and HClO4), subjected to several heating reactions and several evaporation treatments, and finally combined with first dissolution and first centrifugation, effectively completing the digestion and fluoride removal process of extraterrestrial samples, providing a first product for the subsequent preparation of various radionuclide target samples.

[0074] In some embodiments, by precisely defining the carrier type, the reaction conditions for the first heating reaction, the second heating reaction, the first evaporation treatment, the second evaporation treatment, the third evaporation treatment, the first dissolution, and the first centrifugation treatment, as well as the concentration and addition ratio of several acid solutions (first HNO3, first HF, second HF, second HNO3, and HClO4), the extraterrestrial sample is ensured to be fully and stably digested and defluorinated, providing a key guarantee for the efficient and reliable acquisition of the first product. At the same time, the present invention successfully reduces the amount of extraterrestrial sample used to below 50 mg, enabling multi-nucleoside integrated analysis of 10-50 mg extraterrestrial samples in the same process, significantly improving sample utilization and analytical efficiency, and providing important technical support for planetary science research.

[0075] In some embodiments, by sequentially performing three specific elutions (first elution, second elution, and third elution) on an anion exchange column containing the first product, a mixed eluent containing Be, Al, Na, and Ca, an eluent containing Mn, and an eluent containing Fe are obtained efficiently and sequentially, laying the foundation for the precise separation of each target nuclide in subsequent steps.

[0076] In some embodiments, by precisely controlling the concentrations and column volume ratios of the second, third, fourth, and fifth HCl solutions, the anion exchange process ensures efficient and orderly separation of Be, Al, Na, Ca, Mn, and Fe elements in the first product, thereby obtaining a mixed eluent containing Be, Al, Na, and Ca, an eluent containing Mn, and an eluent containing Fe, respectively.

[0077] In some embodiments, a second product is obtained by subjecting a mixed eluent containing Be, Al, Na, and Ca to a fourth evaporation, a second dissolution, and a second centrifugation. The second product is then used in conjunction with a balanced cation exchange column for four elutions (fourth elution, fifth elution, sixth elution, and seventh elution) to efficiently and continuously separate the Na-containing eluent, the Be-containing eluent, and the mixed eluent containing Al and Ca. This provides precise raw materials for the subsequent preparation of various radionuclide target samples by precipitation.

[0078] In some embodiments, by setting the reaction conditions for the fourth evaporation, the second dissolution, the second centrifugation, the fourth rinsing, the fifth rinsing, the sixth rinsing, and the seventh rinsing, the cation exchange process can efficiently and sequentially separate the Na-containing eluent, the Be-containing eluent, and the mixed Al and Ca-containing eluent from the second product, achieving effective separation of elements with similar chemical properties and providing a key guarantee for the subsequent independent preparation of high-purity target samples.

[0079] In some embodiments, through a fifth evaporation process, a third dissolution process, a first vortex process, a third centrifugation process, a sixth evaporation process, a fourth dissolution process, a second vortex process, a fourth centrifugation process, and a second washing process, the supernatant containing Ca and the precipitate containing Al and Ca are efficiently separated from the mixed eluent containing Al and Ca. Be(OH)2 precipitate and Fe(OH)3 precipitate are also obtained from the eluent containing Be and the eluent containing Fe, respectively, providing key precursors for the final preparation of each target sample.

[0080] In some embodiments, by precisely controlling the reaction conditions of the fifth evaporation treatment, the third dissolution treatment, the first vortex treatment, the third centrifugation treatment, the sixth evaporation treatment, the fourth dissolution treatment, the second vortex treatment, the fourth centrifugation treatment, and the second washing treatment, the chemical recovery rate and separation selectivity are significantly improved, providing a key guarantee for the final preparation of each target sample.

[0081] In some embodiments, the corresponding target samples are prepared by converting Be(OH)2 precipitate, Fe(OH)3 precipitate, and Al(OH)3 precipitate into BeO, Fe2O3, and Al2O3, respectively, and mixing them with the corresponding metal powders; the Na-containing eluent is made into sodium salt crystals and mixed with silver powder; a fourth HNO3 is added to the Ca-containing supernatant for acidification, and after the acidification reaction is completed, a third HF is added to obtain CaF2 precipitate, which is then mixed with silver powder; the Mn-containing eluent is converted into MnO2 and mixed with silver powder, thus achieving efficient and complete joint preparation of all target nuclide samples.

[0082] In some embodiments, by precisely defining the reaction conditions for the seventh evaporation, the first calcination, evaporation, acidification reaction, the fifth dissolution, the first settling, the eighth evaporation, the ninth evaporation, the sixth dissolution, the third vortex treatment, the fourth vortex treatment, the second settling, the fifth centrifugation, the sixth centrifugation, and the second calcination, as well as the concentrations of the fourth HNO3 and the third HF, stable and efficient preparation of BeO target samples, Fe2O3 target samples, Al2O3 target samples, sodium salt target samples, CaF2 target samples, and MnO2 target samples with the required composition and morphology is ensured, and the combined process preparation of multiple target samples is finally realized.

[0083] Secondly, the present invention provides a target sample based on an extraterrestrial sample combined process, which has the characteristics of chemical stability, high purity, and uniform mixing with metal powder, and can meet the strict requirements of accelerator mass spectrometers for high-precision measurement of multiple nuclides. Attached Figure Description

[0084] Figure 1 This is a schematic diagram of a target preparation method based on an extraterrestrial sample combined process, as shown in some embodiments of this specification.

[0085] Figure 2 This is a schematic diagram of the filtration curve of a 20 mL anion exchange column according to Example 1 of this specification;

[0086] Figure 3 This is a schematic diagram of the filtration curve of the 8 mL anion exchange column according to Example 1 of this specification;

[0087] Figure 4 This is a schematic diagram of the filtration curve of the 2 mL anion exchange column according to Example 1 of this specification;

[0088] Figure 5 This is a schematic diagram of the filtration curve of a 20 mL cation exchange column according to Example 1 of this specification;

[0089] Figure 6 This is a schematic diagram of the filtration curve of the 8 mL cation exchange column according to Example 1 of this specification;

[0090] Figure 7 This is a schematic diagram of the filtration curve of a 2 mL cation exchange column according to Example 1 of this specification. Detailed Implementation

[0091] In the following description, only certain exemplary embodiments are briefly described. As those skilled in the art will recognize, the described embodiments can be modified in various ways without departing from the spirit or scope of the invention. Therefore, the drawings and description are considered to be exemplary in nature and not restrictive.

[0092] Furthermore, the terms "first" and "second" are used for descriptive purposes only and should not be construed as indicating or implying relative importance or implicitly specifying the number of indicated technical features. Thus, a feature defined as "first" or "second" may explicitly or implicitly include one or more of that feature. In the description of this invention, "a plurality of" means two or more, unless otherwise explicitly specified.

[0093] The technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention.

[0094] Current methods for measuring cosmogenic nuclides rely on accelerator mass spectrometry (AMS), which requires chemical pretreatment techniques to separate and purify nuclides from extraterrestrial samples and prepare corresponding measurement targets before testing. However, for extraterrestrial samples (silicate samples), the existing chemical pretreatment process involves: completely dissolving the extraterrestrial sample in acid, then separating and purifying the nuclides to be tested using ion exchange, liquid-liquid extraction, and precipitation methods to remove interference from isotopes, followed by precipitation to prepare the corresponding solid powder target, which is then mixed with an auxiliary medium and pressed into a target cone for subsequent AMS testing.

[0095] In deep space exploration, the Moon, as Earth's closest natural satellite, is an inevitable choice for humankind's exploration of the universe. The development and utilization of lunar resources is currently the primary goal of lunar exploration. Lunar regolith is the main target of lunar scientific exploration and sample return, and also the best information carrier for humankind to understand the Moon. Studying the space weathering characteristics and space exposure history of lunar regolith is key to understanding the evolution of lunar surface materials and the changes in the lunar space environment. This can provide scientific data for further assessment of the lunar space environment impacts of future international lunar research station construction and manned lunar landings, thus laying the foundation for strategic planning for lunar resource development.

[0096] Cosmogenic nuclides can form a continuous range of apparent exposure ages from centuries to nearly ten million years, thus improving the lunar surface exposure dating methodology, assessing the most recent exposure age of lunar regolith, and providing crucial time constraints for studying space weathering processes on the lunar surface during that period. Furthermore, 10 Be combination 26 Al can establish the energy spectrum characteristics of the Milky Way cosmic rays (GCR) with an average annual value of millions of years, and estimate the extent of the impact of Milky Way cosmic rays on lunar surface weathering; 26 Al can reveal the depth of micrometeorite disturbances; 41 Ca can be used to explore the relationship between the yield and depth of cosmogenic nuclides produced by thermal neutron capture; 22 Na and 60 Fe can serve as a sensitive probe for identifying novae and supernova explosions near the Earth and Moon. This demonstrates that lunar soil holds many mysteries of the solar system and the universe. 10 Be、 22 Na、 26 Al、 41 Ca, 53 Mn and 60 Fe and other substances are key elements that can unlock mysteries.

[0097] Using loess samples from Earth 10 Be and 26 Taking Al extraction experiments as an example, the current demand for loess samples from Earth is about 1 g. In contrast, the Moon, lacking a magnetic field and atmosphere for shielding, exhibits a significantly higher yield of cosmogenic nuclides in its samples, allowing us to focus on a wider range of nuclides, such as… 22 Na、 41 Ca, 53 Mn and 60 Fe, and due to the increased yield, we expect to reduce the required amount of lunar samples to 10-50 mg, but currently there is no mature system for the fine separation and purification of Fe in samples. 10 Be、 22 Na、 26 Al、41 Ca, 53 Mn and 60 The combined process for Fe; although there are existing extraction processes for long-lived nuclides in meteorite samples, the required sample volume is as high as several hundred milligrams, and the process is relatively complex, involving one extraction, one anion exchange, two cation exchanges, and one hydroxide precipitation, which is not conducive to effective background value control; in addition, the biggest interference in accelerator mass spectrometry measurements comes from isotopes, therefore, ensuring the effective separation of the analyte and isotopes (e.g. 10 Be and 10 B. 53 Mn and 53 Cr 60 Fe and 60 Ni (etc.) is key to improving measurement sensitivity.

[0098] Furthermore, lunar samples are extremely difficult and costly to obtain, and the samples are very precious. If various nuclides are extracted separately through different processes, the sample utilization rate is extremely low, making it impossible to conduct comprehensive and efficient research on the same lunar sample. Therefore, if a joint process can be established to simultaneously extract valuable nuclides from lunar samples and perform high-precision quantitative analysis, it can greatly improve the utilization efficiency of lunar samples while meeting the needs of comprehensive multi-nucleoside research.

[0099] In summary, to meet the research needs of comprehensive multi-nucleoside analysis of extraterrestrial samples, this invention first utilizes anion and cation exchange resins, selecting suitable ion exchange resins and eluents, and achieving the desired results in the analysis of extraterrestrial samples through only one anion exchange resin exchange, one cation exchange resin exchange, and one hydroxide precipitation. 10 Be、 22 Na、 26 Al、 41 Ca, 53 Mn and 60 The process involves the separation and purification of Fe nuclides. Secondly, based on the different chemical properties of each element, CaF2 precipitate, BeO, Al2O3, MnO2, and Fe2O3 are prepared using a precipitation method, while mixed sodium salt crystals are prepared using an evaporation crystallization method. The obtained CaF2 precipitate, BeO, Al2O3, MnO2, Fe2O3, and mixed sodium salt crystals are then mixed uniformly with their respective conductive media and pressed into target cones to prepare target samples that meet the requirements of AMS measurements. This enables a combined (or co-process) multi-nucleoside comprehensive analysis of the same extraterrestrial sample.

[0100] Example 1:

[0101] This embodiment provides a target preparation method based on a combined extraterrestrial sample process. See [link to documentation]. Figure 1 This includes the following steps:

[0102] Step 1: Digest the lunar sample, then remove fluorine from the digested lunar sample to obtain the first product:

[0103] Step 1.1, Digesting the lunar sample: Weigh 50 mg of the lunar sample into a digestion vessel and add 0.6 mg of... 9 Be carrier, 1mg 23 Na carrier and 1 mg 55 Mn carrier was used, and 0.2 mL of 16.5 mol / L HNO3 and 1 mL of 22.5 mol / L HF were added to the digestion vessel to obtain a mixed solution. The digestion vessel containing the mixed solution was covered and placed on a heating plate at 150°C for a first heating reaction of 5 h. After the first heating reaction was carried out, the lid was removed, and the vessel was subjected to a first evaporation treatment at 210°C for 1 h. Then, 1 mL of 22.5 mol / L HF was added, the vessel was covered, and the vessel was subjected to a second heating reaction at 150°C for 5 h. After the second heating reaction was carried out, the lid was removed, and the vessel was subjected to a second evaporation treatment at 210°C for 1 h to obtain the digested lunar sample.

[0104] Step 1.2, Fluorine Removal: Add 0.25 mL of 16.5 mol / L HNO3, 0.25 mL of ultrapure water, and 0.5 mL of HClO4 to the digested lunar sample. Remove the cap and perform a third evaporation treatment at 210 °C for 1 h. Then, dissolve the third evaporation product with 10 mol / L HCl solution. Clean the digestion vessel again with 10 mol / L HCl solution. Transfer the first dissolved product to a centrifuge tube and centrifuge at 3000 rpm for 5 min to obtain the first product. After adjusting the volume of the first product, determine the elemental content using ICP-AES (Inductively Coupled Plasma - Atomic Emission Spectroscopy).

[0105] Step 2: Based on the first product, the following eluents are obtained by separation and purification using anion exchange resin method: a mixed eluent containing Be, Al, Na and Ca, an eluent containing Mn, and an eluent containing Fe.

[0106] Equilibrate the anion exchange resin (Dowex 1-X8, Cl) with one column volume of 10 mol / L second HCl solution. -After passing through a Dow 1-X8 anion exchange resin column (chlorinated form), the first product is added to the equilibrated anion exchange resin column. After complete passage, a 10 mol / L third HCl solution is added for the first elution. A clean PFA digestion vessel (PerfluoroalkoxyAlkane Digestion Vessel) is used to collect 1.5 column volumes of mixed eluent containing Be, Al, Na, and Ca, wherein the sum of the volumes of the third HCl solution and the first product is 1.5 column volumes.

[0107] The anion exchange column after the first elution was eluted a second time by adding two column volumes of 7 mol / L fourth HCl solution, and two column volumes of Mn-containing eluent were collected in a clean PFA digestion vessel.

[0108] The anion exchange column after the second elution was eluted a third time by adding four column volumes of 0.1 mol / L HCl solution. Four column volumes of Fe-containing eluent were collected in a clean PFA digestion vessel.

[0109] In some embodiments, the sum of the volumes of the third HCl solution and the first product is 1.5 column volumes, which can be understood as follows: when using a 20 mL anion exchange column, the sum of the column volumes of the third HCl solution and the first product is 30 mL; when using an 8 mL anion exchange column, the sum of the column volumes of the third HCl solution and the first product is 12 mL; and when using a 2 mL anion exchange column, the sum of the column volumes of the third HCl solution and the first product is 3 mL.

[0110] Step 3: Based on the mixed eluent containing Be, Al, Na and Ca, the following eluents are obtained by separation and purification using cation exchange resin method: Na-containing eluent, Be-containing eluent, and mixed eluent containing Al and Ca.

[0111] After the mixed eluent containing Be, Al, Na and Ca was placed on a heating plate at 150 °C for a fourth evaporation treatment for 5 h, the product from the fourth evaporation treatment was dissolved in 1 mL of 6 mol / L HCl solution and 0.05 mL of hydrogen peroxide solution. The dissolved product was transferred to a centrifuge tube and centrifuged at 3000 rpm for 5 min to obtain the second product. The beaker was washed with 5 mL of ultrapure water, and the second product was transferred to the centrifuge tube through the washed beaker.

[0112] Equilibrate the cation exchange resin (Dowex 50W-X8, H) with one column volume of 1 mol / L HCl solution. +After passing through a hydrogen-form Dow 50W-X8 cation exchange resin column, 6 mL of the second product is added to the equilibrated cation exchange resin column. After complete passage, 1 mol / L eighth HCl solution is added for the fourth elution. Four column volumes of Na-containing eluent are collected using a clean PFA digestion vessel, wherein the sum of the volumes of the eighth HCl solution and the second product is four column volumes.

[0113] The cation exchange column after the fourth elution was eluted a fifth time by adding 5 column volumes of 1 mol / L HCl solution. 5 column volumes of Be-containing eluent were collected in a clean PFA digestion vessel.

[0114] The cation exchange column after the fifth elution was eluted by adding 5 column volumes of 1 mol / L HCl solution for the sixth elution, and the eluent was discarded. Then, 4 column volumes of 2.5 mol / L HCl solution were added for the seventh eleventh elution. 4 column volumes of mixed eluent containing Al and Ca were collected in a clean PFA digestion vessel.

[0115] In some embodiments, the sum of the volumes of the eighth HCl solution and the second product is four column volumes, which can be understood as follows: when using a 20 mL cation exchange column, the sum of the column volumes of the eighth HCl solution and the second product is 80 mL; when using an 8 mL cation exchange column, the sum of the column volumes of the eighth HCl solution and the second product is 32 mL; and when using a 2 mL cation exchange column, the sum of the column volumes of the eighth HCl solution and the second product is 8 mL.

[0116] Step 4: Based on the mixed eluent containing Al and Ca, a Ca-containing supernatant and Al(OH)3 precipitate are obtained; based on the eluent containing Be and the eluent containing Fe, Be(OH)2 precipitate and Fe(OH)3 precipitate are obtained, respectively.

[0117] Step 4.1, Separation of Al and Ca elements by precipitation: The mixed eluent containing Al and Ca was placed on a heating plate at 150 ℃ for a fifth evaporation treatment for 5 h. The product from the fifth evaporation treatment was dissolved in 1 mL of 6 mol / L 12th HCl solution and 0.05 mL of second hydrogen peroxide for a third dissolution. The third dissolution product was then transferred to a centrifuge tube, and the pH was adjusted to 8.5 with ammonia. The centrifuge tube was placed on a vortex mixer and vortexed at 1500 rpm for 12 s. After standing for 30 min, it was centrifuged at 3000 rpm for 5 min to obtain a Ca-containing supernatant and Al(OH)3 precipitate. The Ca-containing supernatant was poured into a centrifuge tube, and the Al(OH)3 precipitate was washed 3 times with ultrapure water. The washed Al(OH)3 precipitate was kept for later use.

[0118] Step 4.2, Separation of Be and Fe elements by precipitation: The Be-containing eluent and the Fe-containing eluent were placed on a heating plate at 150 ℃ for a sixth evaporation treatment for 5 h. The two products from the sixth evaporation treatment were dissolved in 1 mL of 6 mol / L 13th HCl solution and 0.05 mL of 3rd hydrogen peroxide solution for a fourth dissolution. The two fourth dissolution products were then transferred to centrifuge tubes, and the pH was adjusted to 8.5 with ammonia. The two centrifuge tubes were then vortexed at 1500 rpm for 12 s and allowed to stand for 30 min. They were then centrifuged at 3000 rpm for 5 min. The supernatant was discarded, and the precipitates were washed three times with ultrapure water to obtain Be(OH)2 precipitate and Fe(OH)3 precipitate, respectively.

[0119] Step 5: Prepare BeO, Fe2O3, and Al2O3 target samples based on Be(OH)2, Fe(OH)3, and Al(OH)3 precipitates, respectively; prepare sodium salt target samples based on Na eluent; prepare CaF2 target samples based on Ca-containing supernatant; and prepare MnO2 target samples based on Mn-containing eluent.

[0120] Step 5.1, Preparation of BeO target sample, Fe2O3 target sample, and Al2O3 target sample: Dissolve 2.87 mg Be(OH)2 precipitate, 16.85 mg Fe(OH)3 precipitate, and 8.72 mg Al(OH)3 precipitate respectively in 0.25 mL of 16.5 mol / L HNO3. Transfer the Be(OH)2, Fe(OH)3, and Al(OH)3 precipitate dissolution products to quartz crucibles, place them on a 150 ℃ heating plate for a seventh evaporation treatment for 0.5 h, and then perform a first calcination at 900 ℃ in a muffle furnace for 2 hours. h, BeO, Fe2O3 and Al2O3 were obtained respectively. BeO, Fe2O3 and Al2O3 were mixed with equal volumes of niobium powder (Nb), silver powder (Ag) and copper powder (Cu) respectively to obtain uniformly mixed BeO-Nb powder, Fe2O3-Ag powder and Al2O3-Cu powder respectively. BeO-Nb powder, Fe2O3-Ag powder and Al2O3-Cu powder were loaded into targets respectively to obtain BeO target sample, Fe2O3 target sample and Al2O3 target sample required for AMS measurement;

[0121] Step 5.2, Preparation of sodium salt mixed solid (sodium salt target sample): The Na-containing eluent was placed on a heating plate at 150 °C for the eighth evaporation treatment for 3 h. The product of the eighth evaporation treatment was dissolved in 1 mL of pure water to obtain the third product. The third product was transferred to a quartz crucible and evaporated at 100 °C for 30 min on a heating plate to allow all sodium salt crystals to precipitate. The sodium salt crystals were mixed with an equal volume of silver powder (Ag) to obtain a uniformly mixed sodium salt crystal-Ag powder. The sodium salt crystal-Ag powder was loaded into the target to obtain the sodium salt target sample required for AMS measurement.

[0122] Step 5.3, Preparation of CaF2 target sample: Add 2 mL of 16.5 mol / L HNO3 to 3 mL of Ca-containing supernatant and perform acidification reaction for 45 min. After the generation of bubbles in the acidification reaction stops, add 1 mL of 22.5 mol / L HF to obtain the fourth product. Vortex the fourth product at 1500 rpm for 12 s and let it stand for 12 h. Then, centrifuge it at 3000 rpm for 5 min to obtain the first supernatant and the first bottom precipitate. Discard the first supernatant and wash the first bottom precipitate with ultrapure water 3 times to obtain CaF2. Mix CaF2 with an equal volume of silver powder (Ag) to obtain a uniformly mixed CaF2-Ag powder. Load the CaF2-Ag powder into the target to obtain the CaF2 target sample required for AMS measurement.

[0123] Step 5.4, Preparation of MnO2 target sample: The Mn-containing eluent was subjected to the ninth evaporation treatment at 150 °C for 3 h, and then transferred to a centrifuge tube. The sixth dissolution was performed with 1 mL of 12 mol / L HCl solution. 0.8 g of sodium hydroxide was added to the sixth dissolution product. The centrifuge tube was placed on a vortex mixer and subjected to the fourth vortex treatment at 1500 rpm for 13 s. After standing for 30 min, it was placed in a centrifuge and subjected to the sixth centrifugation treatment at 3000 rpm for 5 min to obtain the second supernatant and the second bottom precipitate. The second supernatant was discarded, and the second bottom precipitate was washed three times with ultrapure water. The washed second bottom precipitate was transferred to a quartz crucible and subjected to the second calcination at 900 °C for 2 h in a muffle furnace to obtain MnO2. The MnO2 was mixed with an equal volume of silver powder (Ag) to obtain MnO2-Ag powder. The MnO2-Ag powder was loaded into the target to obtain the MnO2 target sample required for AMS measurement.

[0124] Example 1 describes the separation and extraction of six elements (Be, Na, Al, Ca, Mn, and Fe) from a lunar sample using a combined process, and the resulting samples were prepared as AMS measurement targets to meet the requirements of AMS for... 10 Be、 22 Na、 26 Al、41 Ca, 53 Mn and 60 Analysis requirements for six Fe nuclides.

[0125] Example 2:

[0126] This embodiment provides a target preparation method based on a combined extraterrestrial sample process. See [link to documentation]. Figure 1 This includes the following steps:

[0127] Step 1: Digest the lunar sample, then remove fluorine from the digested lunar sample to obtain the first product:

[0128] Step 1.1, Digesting the lunar sample: Weigh 10 mg of the lunar sample into a digestion vessel and add 0.6 mg of... 9 Be carrier, 1mg 23 Na-carrier, 1 mg 55 Mn carrier and 2.5 mg 27 Al support was used, and 0.2 mL of 16.5 mol / L HNO3 and 1 mL of 22.5 mol / L HF were added to the digestion vessel to obtain a mixed solution. The digestion vessel containing the mixed solution was covered and placed on a heating plate at 150 °C for a first heating reaction of 5 h. After the first heating reaction was carried out, the cover was removed, and the vessel was subjected to a first evaporation treatment at 210 °C for 1 h. Then, 1 mL of 22.5 mol / L HF was added, the vessel was covered, and the vessel was subjected to a second heating reaction at 150 °C for 5 h. After the second heating reaction was carried out, the cover was removed, and the vessel was subjected to a second evaporation treatment at 210 °C for 1 h to obtain the digested lunar sample.

[0129] Step 1.2, Fluorine Removal: Add 0.25 mL of 16.5 mol / L HNO3, 0.25 mL of ultrapure water, and 0.5 mL of HClO4 to the digested lunar sample. Remove the cap and perform a third evaporation treatment at 210 °C for 1 h. Then, dissolve the third evaporation product with 10 mol / L HCl solution. Clean the digestion vessel again with 10 mol / L HCl solution. Transfer the first dissolved product to a centrifuge tube and centrifuge at 3000 rpm for 5 min to obtain the first product. After adjusting the volume of the first product, determine the elemental content using ICP-AES (Inductively Coupled Plasma - Atomic Emission Spectroscopy).

[0130] Step 2: Based on the first product, the following eluents are obtained by separation and purification using anion exchange resin method: a mixed eluent containing Be, Al, Na and Ca, an eluent containing Mn, and an eluent containing Fe.

[0131] Equilibrate the anion exchange resin (Dowex 1-X8, Cl) with one column volume of 10 mol / L second HCl solution. - After passing through a Dow 1-X8 anion exchange resin column (chlorinated form), the first product is added to the equilibrated anion exchange resin column. After complete passage, a 10 mol / L third HCl solution is added for the first elution. A clean PFA digestion vessel (PerfluoroalkoxyAlkane Digestion Vessel) is used to collect 1.5 column volumes of mixed eluent containing Be, Al, Na, and Ca, wherein the sum of the volumes of the third HCl solution and the first product is 1.5 column volumes.

[0132] The anion exchange column after the first elution was eluted a second time by adding two column volumes of 7 mol / L fourth HCl solution, and two column volumes of Mn-containing eluent were collected in a clean PFA digestion vessel.

[0133] The anion exchange column after the second elution was eluted a third time by adding four column volumes of 0.1 mol / L HCl solution. Four column volumes of Fe-containing eluent were collected in a clean PFA digestion vessel.

[0134] In some embodiments, the sum of the volumes of the third HCl solution and the first product is 1.5 column volumes, which can be understood as follows: when using a 20 mL anion exchange column, the sum of the column volumes of the third HCl solution and the first product is 30 mL; when using an 8 mL anion exchange column, the sum of the column volumes of the third HCl solution and the first product is 12 mL; and when using a 2 mL anion exchange column, the sum of the column volumes of the third HCl solution and the first product is 3 mL.

[0135] Step 3: Based on the mixed eluent containing Be, Al, Na and Ca, the following eluents are obtained by separation and purification using cation exchange resin method: Na-containing eluent, Be-containing eluent, and mixed eluent containing Al and Ca.

[0136] After the mixed eluent containing Be, Al, Na and Ca was placed on a heating plate at 150 °C for a fourth evaporation treatment for 5 h, the product from the fourth evaporation treatment was dissolved in 1 mL of 6 mol / L HCl solution and 0.05 mL of hydrogen peroxide solution. The dissolved product was transferred to a centrifuge tube and centrifuged at 3000 rpm for 5 min to obtain the second product. The beaker was washed with 5 mL of ultrapure water, and the second product was transferred to the centrifuge tube through the washed beaker.

[0137] Equilibrate the cation exchange resin (Dowex 50W-X8, H) with one column volume of 1 mol / L HCl solution. + After passing through a hydrogen-form Dow 50W-X8 cation exchange resin column, 6 mL of the second product is added to the equilibrated cation exchange resin column. After complete passage, 1 mol / L eighth HCl solution is added for the fourth elution. Four column volumes of Na-containing eluent are collected using a clean PFA digestion vessel, wherein the sum of the volumes of the eighth HCl solution and the second product is four column volumes.

[0138] The cation exchange column after the fourth elution was eluted a fifth time by adding 5 column volumes of 1 mol / L HCl solution. 5 column volumes of Be-containing eluent were collected in a clean PFA digestion vessel.

[0139] The cation exchange column after the fifth elution was eluted by adding 5 column volumes of 1 mol / L HCl solution for the sixth elution, and the eluent was discarded. Then, 4 column volumes of 2.5 mol / L HCl solution were added for the seventh eleventh elution. 4 column volumes of mixed eluent containing Al and Ca were collected in a clean PFA digestion vessel.

[0140] In some embodiments, the sum of the volumes of the eighth HCl solution and the second product is four column volumes, which can be understood as follows: when using a 20 mL cation exchange column, the sum of the column volumes of the eighth HCl solution and the second product is 80 mL; when using an 8 mL cation exchange column, the sum of the column volumes of the eighth HCl solution and the second product is 32 mL; and when using a 2 mL cation exchange column, the sum of the column volumes of the eighth HCl solution and the second product is 8 mL.

[0141] Step 4: Based on the mixed eluent containing Al and Ca, a Ca-containing supernatant and Al(OH)3 precipitate are obtained; based on the eluent containing Be and the eluent containing Fe, Be(OH)2 precipitate and Fe(OH)3 precipitate are obtained, respectively.

[0142] Step 4.1, Separation of Al and Ca elements by precipitation: The mixed eluent containing Al and Ca was placed on a heating plate at 150 °C for a fifth evaporation treatment for 5 h. The product from the fifth evaporation treatment was dissolved in 1 mL of 6 mol / L 12th HCl solution and 0.05 mL of second hydrogen peroxide for a third dissolution. The third dissolution product was then transferred to a centrifuge tube, and the pH was adjusted to 8.5 with ammonia. The centrifuge tube was placed on a vortex mixer and vortexed at 1500 rpm for 12 s. After standing for 30 min, it was centrifuged at 3000 rpm for 5 min to obtain a Ca-containing supernatant and Al(OH)3 precipitate. The Ca-containing supernatant was poured into a centrifuge tube, and the Al(OH)3 precipitate was reserved for later use.

[0143] Step 4.2, Separation of Be and Fe elements by precipitation: The Be-containing eluent and the Fe-containing eluent were placed on a heating plate at 150 ℃ for a sixth evaporation treatment for 5 h. The two products from the sixth evaporation treatment were dissolved in 1 mL of 6 mol / L 13th HCl solution and 0.05 mL of 3rd hydrogen peroxide solution for a fourth dissolution. The two fourth dissolution products were then transferred to centrifuge tubes, and the pH was adjusted to 8.5 with ammonia. The two centrifuge tubes were then vortexed at 1500 rpm for 12 s and allowed to stand for 30 min. They were then centrifuged at 3000 rpm for 5 min. The supernatant was discarded, and the precipitates were washed three times with ultrapure water to obtain Be(OH)2 precipitate and Fe(OH)3 precipitate, respectively.

[0144] Step 5: Prepare BeO, Fe2O3, and Al2O3 target samples based on Be(OH)2, Fe(OH)3, and Al(OH)3 precipitates, respectively; prepare sodium salt target samples based on Na eluent; prepare CaF2 target samples based on Ca-containing supernatant; and prepare MnO2 target samples based on Mn-containing eluent.

[0145] Step 5.1, Preparation of BeO, Fe2O3, and Al2O3 target samples: Dissolve 2.87 mg Be(OH)2 precipitate, 3.36 mg Fe(OH)3 precipitate, and 8.96 mg Al(OH)3 precipitate respectively in 0.25 mL of 16.5 mol / L HNO3. Transfer the Be(OH)2, Fe(OH)3, and Al(OH)3 precipitate dissolution products to quartz crucibles, place them on a 150 ℃ heating plate for a seventh evaporation treatment for 0.5 h, and then perform a first calcination at 900 ℃ in a muffle furnace for 2 hours. h, BeO, Fe2O3 and Al2O3 were obtained respectively. BeO, Fe2O3 and Al2O3 were mixed with equal volumes of niobium powder (Nb), silver powder (Ag) and copper powder (Cu) respectively to obtain uniformly mixed BeO-Nb powder, Fe2O3-Ag powder and Al2O3-Cu powder respectively. BeO-Nb powder, Fe2O3-Ag powder and Al2O3-Cu powder were loaded into targets respectively to obtain BeO target sample, Fe2O3 target sample and Al2O3 target sample required for AMS measurement;

[0146] Step 5.2, Preparation of sodium salt mixed solid (sodium salt target sample): The Na-containing eluent was placed on a heating plate at 150 °C for the eighth evaporation treatment for 3 h. The product of the eighth evaporation treatment was dissolved in 1 mL of pure water to obtain the third product. The third product was transferred to a quartz crucible and evaporated at 100 °C for 30 min on a heating plate to allow all sodium salt crystals to precipitate. The sodium salt crystals were mixed with an equal volume of silver powder (Ag) to obtain a uniformly mixed sodium salt crystal-Ag powder. The sodium salt crystal-Ag powder was loaded into the target to obtain the sodium salt target sample required for AMS measurement.

[0147] Step 5.3, Preparation of CaF2 target sample: Add 2 mL of 16.5 mol / L HNO3 to 3 mL of Ca-containing supernatant and perform acidification reaction for 45 min. After the generation of bubbles in the acidification reaction stops, add 1 mL of 22.5 mol / L HF to obtain the fourth product. Vortex the fourth product at 1500 rpm for 12 s and let it stand for 12 h. Then, centrifuge it at 3000 rpm for 5 min to obtain the first supernatant and the first bottom precipitate. Discard the first supernatant and wash the first bottom precipitate with ultrapure water 3 times to obtain CaF2. Mix CaF2 with an equal volume of silver powder (Ag) to obtain a uniformly mixed CaF2-Ag powder. Load the CaF2-Ag powder into the target to obtain the CaF2 target sample required for AMS measurement.

[0148] Step 5.4, Preparation of MnO2 target sample: The Mn-containing eluent was subjected to the ninth evaporation treatment at 150 °C for 3 h, and then transferred to a centrifuge tube. The sixth dissolution was performed with 1 mL of 12 mol / L HCl solution. 0.8 g of sodium hydroxide was added to the sixth dissolution product. The centrifuge tube was placed on a vortex mixer and subjected to the fourth vortex treatment at 1500 rpm for 13 s. After standing for 30 min, it was placed in a centrifuge and subjected to the sixth centrifugation treatment at 3000 rpm for 5 min to obtain the second supernatant and the second bottom precipitate. The second supernatant was discarded, and the second bottom precipitate was washed three times with ultrapure water. The washed second bottom precipitate was transferred to a quartz crucible and subjected to the second calcination at 900 °C for 2 h in a muffle furnace to obtain MnO2. The MnO2 was mixed with an equal volume of silver powder (Ag) to obtain MnO2-Ag powder. The MnO2-Ag powder was loaded into the target to obtain the MnO2 target sample required for AMS measurement.

[0149] To demonstrate the beneficial effects of Example 2, recovery rate experiments were conducted on anion exchange resins with specifications of 20 mL, 8 mL, and 2 mL, and cation exchange resins with specifications of 20 mL, 8 mL, and 2 mL, respectively. The specific experimental data are shown in Table 1.

[0150] Table 1. Schematic diagram of the recovery rates of various elements by anion exchange resins and cation exchange resins.

[0151]

[0152] See Table 1. Figures 2-7 While the separation effects of 20 mL, 8 mL, and 2 mL anion exchange resin columns were similar for Be, Fe, Al, Na, and Ca, the 20 mL anion exchange resin column showed better separation performance than the 8 mL and 2 mL columns for Mn. When using a 20 mL anion exchange resin column, the recoveries of Be, Na, Al, Ca, Mn, and Fe were all greater than 90%. For cation exchange resins, the 20 mL column showed better separation performance for Na than the 8 mL and 2 mL columns, and the recoveries of Al, Be, Ca, and Na were all greater than 80%.

[0153] The results show that the target sample preparation method based on the extraterrestrial sample joint process described in Example 2 of this invention can achieve a concentration of 10 mg lunar sample. 10 Be、 22 Na、 26 Al、 41 Ca, 53 Mn and 60Combined extraction and AMS analysis of six Fe nuclides.

[0154] Example 3:

[0155] This embodiment provides a target preparation method based on a combined extraterrestrial sample process. See [link to documentation]. Figure 1 This includes the following steps:

[0156] Step 1: Digest the lunar sample, then remove fluorine from the digested lunar sample to obtain the first product:

[0157] Step 1.1, Digesting the lunar sample: Weigh 30 mg of the lunar sample into a digestion vessel and add 0.6 mg of... 9 Be carrier, 1mg 23 Na-carrier, 1 mg 55 Mn carrier and 1.2 mg 27 Al support was used, and 0.1 mL of 16.5 mol / L HNO3 and 0.9 mL of 22.5 mol / L HF were added to the digestion vessel to obtain a mixed solution. The digestion vessel containing the mixed solution was covered and placed on a heating plate at 140 °C for a first heating reaction of 6 h. After the first heating reaction was carried out, the lid was removed, and the vessel was subjected to a first evaporation treatment at 200 °C for 1.5 h. Then, 0.9 mL of 22.5 mol / L HF was added, the vessel was covered, and the vessel was subjected to a second heating reaction at 140 °C for 4 h. After the second heating reaction was carried out, the lid was removed, and the vessel was subjected to a second evaporation treatment at 200 °C for 1.5 h to obtain the digested lunar sample.

[0158] Step 1.2, Fluorine Removal: Add 0.15 mL of 16.5 mol / L HNO3, 0.15 mL of ultrapure water, and 0.4 mL of HClO4 to the digested lunar sample. Remove the cap and perform a third evaporation treatment at 200 °C for 1.5 h. Then, dissolve the third evaporation product with 10 mol / L HCl solution. Clean the digestion vessel again with 10 mol / L HCl solution. Transfer the first dissolved product to a centrifuge tube and centrifuge at 2500 rpm for 6 min to obtain the first product. After adjusting the volume of the first product, determine the elemental content using ICP-AES (Inductively Coupled Plasma - Atomic Emission Spectroscopy).

[0159] Step 2: Based on the first product, the following eluents are obtained by separation and purification using anion exchange resin method: a mixed eluent containing Be, Al, Na and Ca, an eluent containing Mn, and an eluent containing Fe.

[0160] Equilibrate the anion exchange resin (Dowex 1-X8, Cl) with one column volume of 10 mol / L second HCl solution. - After passing through a Dow 1-X8 anion exchange resin column (chlorinated form), the first product is added to the equilibrated anion exchange resin column. After complete passage, a 10 mol / L third HCl solution is added for the first elution. A clean PFA digestion vessel (PerfluoroalkoxyAlkane Digestion Vessel) is used to collect 1.5 column volumes of mixed eluent containing Be, Al, Na, and Ca, wherein the sum of the volumes of the third HCl solution and the first product is 1.5 column volumes.

[0161] The anion exchange column after the first elution was eluted a second time by adding two column volumes of 7 mol / L fourth HCl solution, and two column volumes of Mn-containing eluent were collected in a clean PFA digestion vessel.

[0162] The anion exchange column after the second elution was eluted a third time by adding four column volumes of 0.1 mol / L HCl solution. Four column volumes of Fe-containing eluent were collected in a clean PFA digestion vessel.

[0163] In some embodiments, the sum of the volumes of the third HCl solution and the first product is 1.5 column volumes, which can be understood as follows: when using a 20 mL anion exchange column, the sum of the column volumes of the third HCl solution and the first product is 30 mL; when using an 8 mL anion exchange column, the sum of the column volumes of the third HCl solution and the first product is 12 mL; and when using a 2 mL anion exchange column, the sum of the column volumes of the third HCl solution and the first product is 3 mL.

[0164] Step 3: Based on the mixed eluent containing Be, Al, Na and Ca, the following eluents are obtained by separation and purification using cation exchange resin method: Na-containing eluent, Be-containing eluent, and mixed eluent containing Al and Ca.

[0165] After the mixed eluent containing Be, Al, Na and Ca was placed on a heating plate at 140 °C for a fourth evaporation treatment for 6 h, the product from the fourth evaporation treatment was dissolved in 1 mL of 6 mol / L HCl solution and 0.05 mL of hydrogen peroxide solution. The dissolved product was transferred to a centrifuge tube and centrifuged at 2500 rpm for 6 min to obtain the second product. The beaker was washed with 5 mL of ultrapure water, and the second product was transferred to the centrifuge tube through the washed beaker.

[0166] Equilibrate the cation exchange resin (Dowex 50W-X8, H) with one column volume of 1 mol / L HCl solution.+ After passing through a hydrogen-form Dow 50W-X8 cation exchange resin column, 6 mL of the second product is added to the equilibrated cation exchange resin column. After complete passage, 1 mol / L eighth HCl solution is added for the fourth elution. Four column volumes of Na-containing eluent are collected using a clean PFA digestion vessel, wherein the sum of the volumes of the eighth HCl solution and the second product is four column volumes.

[0167] The cation exchange column after the fourth elution was eluted a fifth time by adding 5 column volumes of 1 mol / L HCl solution. 5 column volumes of Be-containing eluent were collected in a clean PFA digestion vessel.

[0168] The cation exchange column after the fifth elution was eluted by adding 5 column volumes of 1 mol / L HCl solution for the sixth elution, and the eluent was discarded. Then, 4 column volumes of 2.5 mol / L HCl solution were added for the seventh eleventh elution. 4 column volumes of mixed eluent containing Al and Ca were collected in a clean PFA digestion vessel.

[0169] In some embodiments, the sum of the volumes of the eighth HCl solution and the second product is four column volumes, which can be understood as follows: when using a 20 mL cation exchange column, the sum of the column volumes of the eighth HCl solution and the second product is 80 mL; when using an 8 mL cation exchange column, the sum of the column volumes of the eighth HCl solution and the second product is 32 mL; and when using a 2 mL cation exchange column, the sum of the column volumes of the eighth HCl solution and the second product is 8 mL.

[0170] Step 4: Based on the mixed eluent containing Al and Ca, a Ca-containing supernatant and Al(OH)3 precipitate are obtained; based on the eluent containing Be and the eluent containing Fe, Be(OH)2 precipitate and Fe(OH)3 precipitate are obtained, respectively.

[0171] Step 4.1, Separation of Al and Ca elements by precipitation: The mixed eluent containing Al and Ca was placed on a heating plate at 140 ℃ for a fifth evaporation treatment for 6 h. The product from the fifth evaporation treatment was dissolved in 1 mL of 6 mol / L 12th HCl solution and 0.05 mL of second hydrogen peroxide for a third dissolution. The third dissolution product was then transferred to a centrifuge tube, and the pH was adjusted to 8 with ammonia. The centrifuge tube was placed on a vortex mixer and vortexed at 1500 rpm for 10 s. After standing for 30 min, it was centrifuged at 2500 rpm for a third centrifugation treatment for 6 min to obtain a supernatant containing Ca and Al(OH)3 precipitate. The supernatant containing Ca was poured into a centrifuge tube, and the Al(OH)3 precipitate was reserved for later use.

[0172] Step 4.2, Separation of Be and Fe elements by precipitation: The Be-containing eluent and the Fe-containing eluent were placed on a heating plate at 140 ℃ for a sixth evaporation treatment for 6 h. The two products from the sixth evaporation treatment were dissolved in 1 mL of 6 mol / L 13th HCl solution and 0.05 mL of 3rd hydrogen peroxide solution for a fourth dissolution. The two fourth dissolution products were then transferred to centrifuge tubes, and the pH was adjusted to 8 with ammonia. The two centrifuge tubes were then vortexed at 1500 rpm for a second vortex treatment for 10 s and allowed to stand for 30 min. They were then centrifuged at 2500 rpm for a fourth centrifuge treatment for 6 min. The supernatant was discarded, and the precipitates were washed three times with ultrapure water to obtain Be(OH)2 precipitate and Fe(OH)3 precipitate, respectively.

[0173] Step 5: Prepare BeO, Fe2O3, and Al2O3 target samples based on Be(OH)2, Fe(OH)3, and Al(OH)3 precipitates, respectively; prepare sodium salt target samples based on Na eluent; prepare CaF2 target samples based on Ca-containing supernatant; and prepare MnO2 target samples based on Mn-containing eluent.

[0174] Step 5.1: Preparation of BeO, Fe2O3, and Al2O3 target samples: Dissolve 2.87 mg Be(OH)2 precipitate, 10.11 mg Fe(OH)3 precipitate, and 8.67 mg Al(OH)3 precipitate respectively in 0.25 mL of 16.5 mol / L HNO3. Transfer the Be(OH)2, Fe(OH)3, and Al(OH)3 precipitate dissolution products to quartz crucibles, place them on a 140 ℃ heating plate for a seventh evaporation treatment for 1 h, and then perform a first calcination at 800 ℃ for 1.5 h in a muffle furnace. h, BeO, Fe2O3 and Al2O3 were obtained respectively. BeO, Fe2O3 and Al2O3 were mixed with equal volumes of niobium powder (Nb), silver powder (Ag) and copper powder (Cu) respectively to obtain uniformly mixed BeO-Nb powder, Fe2O3-Ag powder and Al2O3-Cu powder respectively. BeO-Nb powder, Fe2O3-Ag powder and Al2O3-Cu powder were loaded into targets respectively to obtain BeO target sample, Fe2O3 target sample and Al2O3 target sample required for AMS measurement;

[0175] Step 5.2, Preparation of sodium salt mixed solid (sodium salt target sample): The Na-containing eluent was placed on a heating plate at 140 ℃ for the eighth evaporation treatment for 4 h. The product of the eighth evaporation treatment was dissolved in 1 mL of pure water to obtain the third product. The third product was transferred to a quartz crucible and evaporated at 90 ℃ for 40 min on a heating plate to allow all sodium salt crystals to precipitate. The sodium salt crystals were mixed with an equal volume of silver powder (Ag) to obtain a uniformly mixed sodium salt crystal-Ag powder. The sodium salt crystal-Ag powder was loaded into the target to obtain the sodium salt target sample required for AMS measurement.

[0176] Step 5.3, Preparation of CaF2 target sample: Add 2 mL of 16.5 mol / L HNO3 to 3 mL of Ca-containing supernatant and perform acidification reaction for 30 min. After the generation of bubbles in the acidification reaction stops, add 1 mL of 22.5 mol / L HF to obtain the fourth product. Vortex the fourth product at 1500 rpm for 10 s and let it stand for 12 h. Then, centrifuge it at 2500 rpm for 6 min to obtain the first supernatant and the first bottom precipitate. Discard the first supernatant and wash the first bottom precipitate with ultrapure water 3 times to obtain CaF2. Mix CaF2 with an equal volume of silver powder (Ag) to obtain a uniformly mixed CaF2-Ag powder. Load the CaF2-Ag powder into the target to obtain the CaF2 target sample required for AMS measurement.

[0177] Step 5.4, Preparation of MnO2 target sample: The Mn-containing eluent was subjected to the ninth evaporation treatment at 140 °C for 4 h, and then transferred to a centrifuge tube. The sample was dissolved in 1 mL of 12 mol / L HCl solution for the sixth dissolution. 0.5 g of sodium hydroxide was added to the sixth dissolution product. The centrifuge tube was then vortexed at 1500 rpm for 10 s, allowed to stand for 30 min, and then centrifuged at 2500 rpm for 6 min to obtain the second supernatant and the second bottom precipitate. The second supernatant was discarded, and the second bottom precipitate was washed three times with ultrapure water. The washed second bottom precipitate was transferred to a quartz crucible and calcined in a muffle furnace at 800 °C for 2.5 seconds. h, obtain MnO2, mix MnO2 with an equal volume of silver powder (Ag) to obtain MnO2-Ag powder, load the MnO2-Ag powder into the target to obtain the MnO2 target sample required for AMS measurement.

[0178] Example 4:

[0179] This embodiment provides a target preparation method based on a combined extraterrestrial sample process. See [link to documentation]. Figure 1 This includes the following steps:

[0180] Step 1: Take a chondrite sample and digest it. Then, remove fluorine from the digested chondrite sample to obtain the first product:

[0181] Step 1.1, digestion of chondrite sample: Weigh 40 mg of chondrite sample into a digestion vessel, add 0.6 mg of... 9 Be carrier, 1 mg 23 Na-carrier, 1 mg 40 Ca carrier, 1 mg 55 Mn carrier and 2.5 mg 27 Al support was used, and 0.3 mL of 16.5 mol / L HNO3 and 1.1 mL of 22.5 mol / L HF were added to the digestion vessel to obtain a mixed solution. The digestion vessel containing the mixed solution was covered and placed on a heating plate at 160 ℃ for a first heating reaction of 4 h. After the first heating reaction was carried out, the cover was removed, and the vessel was subjected to a first evaporation treatment at 220 ℃ for 1 h. Then, 1.1 mL of 22.5 mol / L HF was added, the vessel was covered, and the vessel was subjected to a second heating reaction at 160 ℃ for 6 h. After the second heating reaction was carried out, the cover was removed, and the vessel was subjected to a second evaporation treatment at 220 ℃ for 1 h to obtain the digested chondrite sample.

[0182] Step 1.2, Fluorine Removal: Add 0.35 mL of 16.5 mol / L HNO3, 0.35 mL of ultrapure water, and 0.6 mL of HClO4 to the digested chondrite sample. Remove the cap and perform a third evaporation treatment at 220 °C for 1 h. Then, dissolve the third evaporation product with 10 mol / L HCl solution. Clean the digestion vessel again with 10 mol / L HCl solution. Transfer the first dissolved product to a centrifuge tube and centrifuge at 3500 rpm for 4 min to obtain the first product. After adjusting the volume of the first product, determine the elemental content using ICP-AES (Inductively Coupled Plasma - Atomic Emission Spectroscopy).

[0183] Step 2: Based on the first product, the following eluents are obtained by separation and purification using anion exchange resin method: a mixed eluent containing Be, Al, Na and Ca, an eluent containing Mn, and an eluent containing Fe.

[0184] Equilibrate the anion exchange resin (Dowex 1-X8, Cl) with one column volume of 10 mol / L second HCl solution. -After passing through a Dow 1-X8 anion exchange resin column (chlorinated form), the first product is added to the equilibrated anion exchange resin column. After complete passage, a 10 mol / L third HCl solution is added for the first elution. A clean PFA digestion vessel (PerfluoroalkoxyAlkane Digestion Vessel) is used to collect 1.5 column volumes of mixed eluent containing Be, Al, Na, and Ca, wherein the sum of the volumes of the third HCl solution and the first product is 1.5 column volumes.

[0185] The anion exchange column after the first elution was eluted a second time by adding two column volumes of 7 mol / L fourth HCl solution, and two column volumes of Mn-containing eluent were collected in a clean PFA digestion vessel.

[0186] The anion exchange column after the second elution was eluted a third time by adding four column volumes of 0.1 mol / L HCl solution. Four column volumes of Fe-containing eluent were collected in a clean PFA digestion vessel.

[0187] In some embodiments, the sum of the volumes of the third HCl solution and the first product is 1.5 column volumes, which can be understood as follows: when using a 20 mL anion exchange column, the sum of the column volumes of the third HCl solution and the first product is 30 mL; when using an 8 mL anion exchange column, the sum of the column volumes of the third HCl solution and the first product is 12 mL; and when using a 2 mL anion exchange column, the sum of the column volumes of the third HCl solution and the first product is 3 mL.

[0188] Step 3: Based on the mixed eluent containing Be, Al, Na and Ca, the following eluents are obtained by separation and purification using cation exchange resin method: Na-containing eluent, Be-containing eluent, and mixed eluent containing Al and Ca.

[0189] After the mixed eluent containing Be, Al, Na and Ca was placed on a heating plate at 160 °C for a fourth evaporation treatment for 4 h, the product from the fourth evaporation treatment was dissolved in 1 mL of 6 mol / L HCl solution and 0.05 mL of hydrogen peroxide solution. The dissolved product was transferred to a centrifuge tube and centrifuged at 3500 rpm for 4 min to obtain the second product. The beaker was washed with 5 mL of ultrapure water, and the second product was transferred to the centrifuge tube through the washed beaker.

[0190] Equilibrate the cation exchange resin (Dowex 50W-X8, H) with one column volume of 1 mol / L HCl solution. +After passing through a hydrogen-form Dow 50W-X8 cation exchange resin column, 6 mL of the second product is added to the equilibrated cation exchange resin column. After complete passage, 1 mol / L eighth HCl solution is added for the fourth elution. Four column volumes of Na-containing eluent are collected using a clean PFA digestion vessel, wherein the sum of the volumes of the eighth HCl solution and the second product is four column volumes.

[0191] The cation exchange column after the fourth elution was eluted a fifth time by adding 5 column volumes of 1 mol / L HCl solution. 5 column volumes of Be-containing eluent were collected in a clean PFA digestion vessel.

[0192] The cation exchange column after the fifth elution was eluted by adding 5 column volumes of 1 mol / L HCl solution for the sixth elution, and the eluent was discarded. Then, 4 column volumes of 2.5 mol / L HCl solution were added for the seventh eleventh elution. 4 column volumes of mixed eluent containing Al and Ca were collected in a clean PFA digestion vessel.

[0193] In some embodiments, the sum of the volumes of the eighth HCl solution and the second product is four column volumes, which can be understood as follows: when using a 20 mL cation exchange column, the sum of the column volumes of the eighth HCl solution and the second product is 80 mL; when using an 8 mL cation exchange column, the sum of the column volumes of the eighth HCl solution and the second product is 32 mL; and when using a 2 mL cation exchange column, the sum of the column volumes of the eighth HCl solution and the second product is 8 mL.

[0194] Step 4: Based on the mixed eluent containing Al and Ca, a Ca-containing supernatant and Al(OH)3 precipitate are obtained; based on the eluent containing Be and the eluent containing Fe, Be(OH)2 precipitate and Fe(OH)3 precipitate are obtained, respectively.

[0195] Step 4.1, Separation of Al and Ca elements by precipitation: The mixed eluent containing Al and Ca was placed on a heating plate at 160 ℃ for a fifth evaporation treatment for 4 h. The product from the fifth evaporation treatment was dissolved in 1 mL of 6 mol / L 12th HCl solution and 0.05 mL of second hydrogen peroxide for a third dissolution. The third dissolution product was then transferred to a centrifuge tube, and the pH was adjusted to 9 with ammonia. The centrifuge tube was placed on a vortex mixer and vortexed at 1500 rpm for 15 s. After standing for 30 min, it was centrifuged at 3500 rpm for a third centrifugation treatment for 4 min to obtain a supernatant containing Ca and an Al(OH)3 precipitate. The supernatant containing Ca was poured into a centrifuge tube, and the Al(OH)3 precipitate was kept for later use.

[0196] Step 4.2, Separation of Be and Fe elements by precipitation: The Be-containing eluent and the Fe-containing eluent were placed on a 160 ℃ heating plate for a sixth evaporation treatment for 4 h. The two products from the sixth evaporation treatment were dissolved in 1 mL of 6 mol / L 13th HCl solution and 0.05 mL of 3rd hydrogen peroxide solution for a fourth dissolution. The two fourth dissolution products were then transferred to centrifuge tubes, and the pH was adjusted to 9 with ammonia. The two centrifuge tubes were then vortexed at 1500 rpm for a second vortex treatment for 15 s and allowed to stand for 30 min. They were then centrifuged at 3500 rpm for a fourth centrifuge treatment for 4 min. The supernatant was discarded, and the precipitates were washed three times with ultrapure water to obtain Be(OH)2 precipitate and Fe(OH)3 precipitate, respectively.

[0197] Step 5: Prepare BeO, Fe2O3, and Al2O3 target samples based on Be(OH)2, Fe(OH)3, and Al(OH)3 precipitates, respectively; prepare sodium salt target samples based on Na eluent; prepare CaF2 target samples based on Ca-containing supernatant; and prepare MnO2 target samples based on Mn-containing eluent.

[0198] Step 5.1: Preparation of BeO, Fe2O3, and Al2O3 target samples: Dissolve 2.87 mg Be(OH)2 precipitate, 14.12 mg Fe(OH)3 precipitate, and 8.67 mg Al(OH)3 precipitate respectively in 0.25 mL of 16.5 mol / L HNO3. Transfer the Be(OH)2, Fe(OH)3, and Al(OH)3 precipitate dissolution products to quartz crucibles, place them on a 160 ℃ heating plate for a seventh evaporation treatment for 1 h, and then perform a first calcination at 1000 ℃ for 2.5 h in a muffle furnace. h, BeO, Fe2O3 and Al2O3 were obtained respectively. BeO, Fe2O3 and Al2O3 were mixed with equal volumes of niobium powder (Nb), silver powder (Ag) and copper powder (Cu) respectively to obtain uniformly mixed BeO-Nb powder, Fe2O3-Ag powder and Al2O3-Cu powder respectively. BeO-Nb powder, Fe2O3-Ag powder and Al2O3-Cu powder were loaded into targets respectively to obtain BeO target sample, Fe2O3 target sample and Al2O3 target sample required for AMS measurement;

[0199] Step 5.2, Preparation of sodium salt mixed solid (sodium salt target sample): The Na-containing eluent was placed on a heating plate at 160 ℃ for the eighth evaporation treatment for 2 h. The product of the eighth evaporation treatment was dissolved in 1 mL of pure water to obtain the third product. The third product was transferred to a quartz crucible and evaporated at 110 ℃ for 20 min on a heating plate to allow all sodium salt crystals to precipitate. The sodium salt crystals were mixed with an equal volume of silver powder (Ag) to obtain a uniformly mixed sodium salt crystal-Ag powder. The sodium salt crystal-Ag powder was loaded into the target to obtain the sodium salt target sample required for AMS measurement.

[0200] Step 5.3, Preparation of CaF2 target sample: Add 2 mL of 16.5 mol / L HNO3 to 3 mL of Ca-containing supernatant and perform acidification reaction for 60 min. After the generation of bubbles in the acidification reaction stops, add 1 mL of 22.5 mol / L HF to obtain the fourth product. Vortex the fourth product at 1500 rpm for 15 s and let it stand for 12 h. Then, centrifuge it at 3500 rpm for 4 min to obtain the first supernatant and the first bottom precipitate. Discard the first supernatant and wash the first bottom precipitate with ultrapure water 3 times to obtain CaF2. Mix CaF2 with an equal volume of silver powder (Ag) to obtain a uniformly mixed CaF2-Ag powder. Load the CaF2-Ag powder into the target to obtain the CaF2 target sample required for AMS measurement.

[0201] Step 5.4, Preparation of MnO2 target sample: The Mn-containing eluent was subjected to the ninth evaporation treatment at 160 °C for 2 h, and then transferred to a centrifuge tube. The sixth dissolution was performed with 1 mL of 12 mol / L HCl solution. 1 g of sodium hydroxide was added to the sixth dissolution product. The centrifuge tube was placed on a vortex mixer and subjected to the fourth vortex treatment at 1500 rpm for 15 s. After standing for 30 min, it was placed in a centrifuge and subjected to the sixth centrifugation treatment at 3500 rpm for 4 min to obtain the second supernatant and the second bottom precipitate. The second supernatant was discarded, and the second bottom precipitate was washed three times with ultrapure water. The washed second bottom precipitate was transferred to a quartz crucible and subjected to the second calcination at 1000 °C for 1.5 h in a muffle furnace to obtain MnO2. The MnO2 was mixed with an equal volume of silver powder (Ag) to obtain MnO2-Ag powder. The MnO2-Ag powder was loaded into the target to obtain the MnO2 target sample required for AMS measurement.

[0202] Examples 1-4 of this specification use a mixed acid solution of HNO3 and HF to dissolve the samples from the ground. Using an anion exchange column, Mn and Fe are purified from the solution using hydrochloric acid of different concentrations. Simultaneously, Mn and Fe are separated from interfering elements Cr and Ni; Cr and Ni are present in the third HCl solution, while Mn and Fe are present in the fourth and fifth HCl solutions, respectively. Then, using a cation exchange column with the eighth HCl solution, Na and Be are sequentially separated and purified from the solution by controlling the volume of the eluent. Be is also separated from interfering element B; B and Na are present in 1-4 column volumes of eluent, while Be is present in 5-9 column volumes. Next, Al and Ca are purified from the solution using the eleventh HCl solution. Finally, by precipitation separation, the pH of the third dissolved product (a mixed solution of Ca and Al) is adjusted to 8-9 using ammonia, separating the two and obtaining a Ca-containing supernatant and Al(OH)3 precipitate.

[0203] Based on the properties of each element, the isolated and purified nuclides were prepared into testable target samples using different methods: (1) Ammonia was added to the Be-containing eluent and the Fe-containing eluent to a pH of 8-9 to generate Be(OH)2 precipitate and Fe(OH)3 precipitate. The Be(OH)2 precipitate, Fe(OH)3 precipitate and Al(OH)3 precipitate were subjected to a first calcination to obtain BeO, Fe2O3 and Al2O3 respectively. BeO was mixed with niobium powder (Nb), Fe2O3 was mixed with silver powder (Ag), and Al2O3 was mixed with copper powder (C). (1) Mix to obtain the test target sample; (2) Obtain sodium salt crystals by evaporation crystallization, and mix the sodium salt crystals with silver powder (Ag) to obtain the test target sample; (3) Acidify the Ca-containing supernatant with nitric acid, and after the gas bubbles of the acidification reaction stop being generated, obtain Ca(NO3)2 solution, and then add the third HF to the Ca(NO3)2 solution to prepare CaF2 precipitate, and mix CaF2 with silver powder (Ag) to obtain the test target sample; (4) Obtain MnO2 by treating the Mn-containing eluent, and mix MnO2 with silver powder (Ag) to obtain the test target sample.

[0204] This invention enables the efficient extraction of substances from extraterrestrial samples (extraterrestrial celestial body samples) at the tens of milligram level via a combined process. 10 Be、 22 Na、 26 Al、 41 Ca, 53 Mn and 60 Six Fe nuclides can be converted using an anion exchange column. 53 Mn and 60Fe was separated and purified from the solution, with recoveries of all elements exceeding 90%; cation exchange column chromatography can be used to further purify Fe. 22 Na and 10 Be was separated and purified from the solution, with the recovery rate of each element being greater than 80%.

[0205] Furthermore, current chemical separation procedures for all samples (including Earth samples and extraterrestrial samples) are mostly designed for the extraction of one or two nuclides (such as...). 10 Be and 26 Al), and the dosage must be significantly increased to meet the measurement requirements of AMS.

[0206] This invention establishes a method capable of extracting from extraterrestrial samples. 10 Be、 22 Na、 26 Al、 41 Ca, 53 Mn and 60 The combined process of Fe enables the extraction of multiple nuclides from the same extraterrestrial sample in a single process; at the same time, the amount of extraterrestrial sample used is controlled to be less than 50 mg, and further, based on the chemical properties of different nuclides, different chemical methods are used to prepare test targets that can be used for high-precision quantitative analysis, thereby meeting the needs of multi-nucleoside comprehensive analysis of the same extraterrestrial sample.

[0207] The foregoing has shown and described the basic principles, main features, and advantages of the present invention. It will be apparent to those skilled in the art that the present invention is not limited to the details of the exemplary embodiments described above, and that the invention can be implemented in other specific forms without departing from its spirit or basic characteristics. Therefore, the embodiments should be considered exemplary and non-limiting in all respects.

[0208] Furthermore, it should be understood that although this specification describes embodiments, not every embodiment contains only one independent technical solution. This narrative style is merely for clarity. Those skilled in the art should consider the specification as a whole, and the technical solutions in each embodiment can be appropriately combined to form other embodiments that can be understood by those skilled in the art. The above content is only for illustrating the technical concept of the present invention and should not be used to limit the scope of protection of the present invention. Any modifications made to the technical solutions based on the technical concept proposed in this invention fall within the scope of protection of this invention.

Claims

1. A target sample preparation method based on a combined extraterrestrial sample process, characterized in that, Includes the following steps: An extraterrestrial sample is digested, and the digested extraterrestrial sample is subjected to fluoride removal to obtain a first product. Specifically, the process includes: mixing the extraterrestrial sample, a carrier, a first HNO3, and a first HF to obtain a mixed solution; subjecting the mixed solution to a first heating reaction and a first evaporation treatment in sequence; adding a second HF; and subjecting the mixture to a second heating reaction and a second evaporation treatment in sequence to obtain a digested extraterrestrial sample; adding a second HNO3, ultrapure water, and HClO4 to the digested extraterrestrial sample; subjecting the mixture to a third evaporation treatment; subjecting the product of the third evaporation treatment to a first dissolution; and subjecting the product of the first dissolution to a first centrifugation treatment to obtain the first product; the ratio of the amount of extraterrestrial sample, the first HNO3, the first HF, and the second HF added is (10-50) mg : (0.1-0.3) mL : (0.9-1.1) mL : (0.9-1.1) mL. Based on the first product, a mixed eluent containing Be, Al, Na and Ca, an eluent containing Mn, and an eluent containing Fe were obtained by anion exchange resin method; the column volume ratio of the mixed eluent containing Be, Al, Na and Ca, the eluent containing Mn, and the eluent containing Fe was 1.5:2:

4. Based on a mixed eluent containing Be, Al, Na and Ca, a Na-containing eluent, a Be-containing eluent, and a mixed eluent containing Al and Ca were obtained by cation exchange resin method; the column volume ratio of the Na-containing eluent, the Be-containing eluent, and the mixed eluent containing Al and Ca was 4:5:

4. Based on the mixed eluent containing Al and Ca, a Ca-containing supernatant and Al(OH)3 precipitate were obtained; based on the eluent containing Be and the eluent containing Fe, Be(OH)2 precipitate and Fe(OH)3 precipitate were obtained, respectively. BeO, Fe2O3, and Al2O3 targets were prepared based on Be(OH)2, Fe(OH)3, and Al(OH)3 precipitation, respectively. Sodium salt targets were prepared based on Na eluent, CaF2 targets were prepared based on Ca-containing supernatant, and MnO2 targets were prepared based on Mn-containing eluent.

2. The target preparation method based on a combined extraterrestrial sample process according to claim 1, characterized in that, The carrier includes 9 Be carrier, 23 Na carrier, 55 Mn carrier, 27 Al carrier, 56 Fe carrier, 40 Three or more Ca carriers; The concentration of the first HNO3 is 16.5 mol / L; the concentration of the first HF is 22.5 mol / L; the concentration of the second HF is 22.5 mol / L; The temperature of both the first and second heating reactions is 140-160 ℃, and the time of both the first and second heating reactions is 4-6 h. The temperature of the first, second, and third evaporation treatments is 200-220 ℃, and the time of the first, second, and third evaporation treatments is 1-1.5 h. The concentration of the second HNO3 is 16.5 mol / L; the volume ratio of the second HNO3, ultrapure water, and HClO4 is (0.15-0.35) mL : (0.15-0.35) mL : (0.4-0.6) mL; The first dissolution uses a first HCl solution with a concentration of 10 mol / L; The first centrifugation process is carried out at a speed of 2500-3500 rpm for 4-6 minutes.

3. The target preparation method based on a combined extraterrestrial sample process according to claim 1, characterized in that, The process of obtaining a mixed eluent containing Be, Al, Na, and Ca, an eluent containing Mn, and an eluent containing Fe from the first product via anion exchange resin specifically includes: The anion exchange column is equilibrated, and the first product is added to the equilibrated anion exchange column to obtain the anion exchange column after the addition of the first product. The anion exchange column after the addition of the first product is subjected to a first elution to obtain a mixed eluent containing Be, Al, Na and Ca. The anion exchange column after the first elution was subjected to a second elution to obtain an eluent containing Mn. The anion exchange column after the second elution was subjected to a third elution to obtain an eluent containing Fe.

4. A target preparation method based on a combined extraterrestrial sample process according to claim 3, characterized in that, The balanced anion exchange column uses a second HCl solution with a concentration of 10 mol / L and a column volume of 1 column. The first elution uses a third HCl solution with a concentration of 10 mol / L, and the sum of the volumes of the third HCl solution and the first product is 1.5 column volumes. The second elution uses a fourth HCl solution with a concentration of 7 mol / L; the third elution uses a fifth HCl solution with a concentration of 0.1 mol / L; the column volume ratio of the fourth HCl solution to the fifth HCl solution is 2:

4.

5. The target preparation method based on a combined extraterrestrial sample process according to claim 1, characterized in that, The method for obtaining Na-containing eluent, Be-containing eluent, and Al and Ca-containing mixed eluent via cation exchange resin based on a mixed eluent containing Be, Al, Na, and Ca specifically includes: The mixed eluent containing Be, Al, Na and Ca was subjected to a fourth evaporation to dryness, the product of the fourth evaporation to dryness was subjected to a second dissolution, and the product of the second dissolution to be subjected to a second centrifugation to obtain the second product. Equilibrate the cation exchange column, add the second product to the equilibrated cation exchange column, and obtain the cation exchange column after adding the second product. Perform a fourth elution on the cation exchange column after adding the second product to obtain the eluent containing Na. The cation exchange column after the fourth elution was subjected to a fifth elution to obtain a Be-containing eluent; The cation exchange column after the fifth elution was subjected to a sixth and seventh elution in sequence to obtain a mixed eluent containing Al and Ca.

6. A target preparation method based on a combined extraterrestrial sample process according to claim 5, characterized in that, The temperature of the fourth evaporation treatment is 140-160 ℃, and the time of the fourth evaporation treatment is 4-6 h; The second dissolution uses a sixth HCl solution and a first hydrogen peroxide solution, the concentration of the sixth HCl solution being 6 mol / L; the volume ratio of the sixth HCl solution to the first hydrogen peroxide solution is 1 mL: 0.05 mL; The second centrifugation process is carried out at a speed of 2500-3500 rpm for 4-6 minutes. The balanced cation exchange column uses one column volume of the seventh HCl solution, and the concentration of the seventh HCl solution is 1 mol / L. The fourth elution uses the eighth HCl solution, which has a concentration of 1 mol / L, and the sum of the volumes of the eighth HCl solution and the second product is 4 column volumes. The fifth elution uses the ninth HCl solution with a concentration of 1 mol / L; the sixth elution uses the tenth HCl solution with a concentration of 1 mol / L; the seventh eleventh HCl solution uses the eleventh HCl solution with a concentration of 2.5 mol / L; the column volume ratio of the ninth, tenth, and eleventh HCl solutions is 5:5:

4.

7. The target preparation method based on a combined extraterrestrial sample process according to claim 1, characterized in that, The process of obtaining a Ca-containing supernatant and Al(OH)3 precipitate based on a mixed eluent containing Al and Ca, and obtaining Be(OH)2 precipitate and Fe(OH)3 precipitate based on a Be-containing eluent and a Fe-containing eluent, respectively, specifically includes: The mixed eluent containing Al and Ca was subjected to a fifth evaporation treatment. The product from the fifth evaporation treatment was then dissolved in a third solution. The pH of the product from the third solution was adjusted to 8-9 and then subjected to a first vortex treatment and a third centrifugation treatment in sequence to obtain a Ca-containing supernatant and an Al(OH)3 precipitate. The Be-containing eluent and the Fe-containing eluent were subjected to a sixth evaporation treatment. The products from the two sixth evaporation treatments were then dissolved in the fourth solution. The pH of the two fourth solution products was adjusted to 8-9, and then they were subjected to a second vortex treatment and a fourth centrifugation treatment in sequence. The products from the two fourth centrifugation treatments were then washed in the second wash to obtain Be(OH)2 precipitate and Fe(OH)3 precipitate, respectively.

8. A target preparation method based on a combined extraterrestrial sample process according to claim 7, characterized in that, The temperature of the fifth drying treatment is 140-160 ℃, and the time of the fifth drying treatment is 4-6 h; The third dissolution uses a twelfth HCl solution and a second hydrogen peroxide solution, wherein the concentration of the twelfth HCl solution is 6 mol / L; and the volume ratio of the twelfth HCl solution to the second hydrogen peroxide solution is 1 mL: 0.05 mL. The temperature of the sixth drying treatment is 140-160 ℃, and the time of the sixth drying treatment is 4-6 h; The fourth dissolution uses a thirteenth HCl solution and a third hydrogen peroxide solution, with the concentration of the thirteenth HCl solution being 6 mol / L; the volume ratio of the thirteenth HCl solution to the third hydrogen peroxide solution is 1 mL: 0.05 mL. The rotational speed of both the first and second vortex processes is 1500 rpm, and the time of both the first and second vortex processes is 10-15 s. The rotation speed of the third and fourth centrifugation processes is 2500-3500 rpm, and the time for both processes is 4-6 min.

9. The target preparation method based on a combined extraterrestrial sample process according to claim 1, characterized in that, The preparation of BeO, Fe2O3, and Al2O3 target samples based on Be(OH)2, Fe(OH)3, and Al(OH)3 precipitation, respectively; the preparation of sodium salt target samples based on Na eluent; the preparation of CaF2 target samples based on Ca-containing supernatant; and the preparation of MnO2 target samples based on Mn-containing eluent, specifically includes: After dissolving Be(OH)2 precipitate, Fe(OH)3 precipitate and Al(OH)3 precipitate with HNO3, respectively, they were subjected to a seventh evaporation and a first calcination to obtain BeO, Fe2O3 and Al2O3, respectively. BeO, Fe2O3 and Al2O3 were then mixed with equal volumes of niobium powder, silver powder and copper powder to obtain BeO target sample, Fe2O3 target sample and Al2O3 target sample, respectively. The Na-containing eluent was subjected to an eighth evaporation process, and the product from the eighth evaporation process was dissolved in a fifth process to obtain a third product. The third product was evaporated until all sodium salt crystals precipitated. The sodium salt crystals were mixed with an equal volume of silver powder to obtain a sodium salt target sample. Acidification reaction was carried out by adding HNO3 to the supernatant containing Ca. After the bubbles in the acidification reaction stopped being generated, HF was added to obtain the fourth product. The fourth product was subjected to the third vortex treatment and then subjected to the first settling and the fifth centrifugation treatment to obtain CaF2. CaF2 was mixed with an equal volume of silver powder to obtain the CaF2 target sample. The Mn-containing eluent was subjected to a ninth evaporation treatment, and the product from the ninth evaporation treatment was dissolved in a sixth process. Sodium hydroxide was added to the product from the sixth dissolution treatment, and the product was subjected to a fourth vortex treatment, a second settling treatment, a sixth centrifugation treatment, and a second calcination treatment in sequence to obtain MnO2. The MnO2 was then mixed with an equal volume of silver powder to obtain the MnO2 target sample.

10. A target preparation method based on a combined extraterrestrial sample process according to claim 9, characterized in that, The concentration of the third HNO3 was 16.5 mol / L; The temperature of the seventh evaporation treatment is 140-160 ℃, and the time of the seventh evaporation treatment is 0.5-1 h; the temperature of the first calcination is 800-1000 ℃, and the time of the first calcination is 1.5-2.5 h; The fifth dissolution uses pure water; the evaporation temperature is 90-110 ℃, and the evaporation time is 20-40 min; The concentration of the fourth HNO3 is 16.5 mol / L; the acidification reaction time is 30-60 min; The concentration of the third HF is 22.5 mol / L; the volume ratio of the Ca-containing supernatant, the fourth HNO3, and the third HF is 3:2:1; The first settling time is 12 h; the temperature of the eighth and ninth evaporation treatments is 140-160℃, and the time of the eighth and ninth evaporation treatments is 2-4 h. The sixth dissolution uses the fourteenth HCl solution, the concentration of which is 12 mol / L; the ratio of the fourteenth HCl solution to sodium hydroxide is 1 mL: (0.5-1) g. The rotational speed of the third and fourth vortex processes is 1500 rpm, and the time of the third and fourth vortex processes is 10-15 s. The second settling time is 30 min; the speed of the fifth and sixth centrifugation treatments is 2500-3500 rpm, and the time of the fifth and sixth centrifugation treatments is 4-6 min; the temperature of the second ignition is 800-1000 ℃, and the time of the second ignition is 1.5-2.5 h.

11. A target sample based on a combined extraterrestrial sample process, characterized in that, The target sample preparation method based on the extraterrestrial sample joint process described in any one of claims 1-10 is obtained.

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