TWI426265B - An automatic analysis method of technetium - Google Patents

Description

An automatic analysis method of 鎝-99

The invention relates to a method for analyzing radioactive nucleus, in particular to an automatic analysis method for strontium-99.

Radioactive nucleus is one of the important products of nuclear reaction. In order to ensure the safe operation of nuclear energy facilities and protect the environment from radiation pollution, it is necessary to understand and evaluate the concentration, distribution and influence of radioactive products. Therefore, since the development and application of nuclear energy technology, related radioactivity The identification and identification of nuclear species has always been a necessary technology for the nuclear energy industry.

The artificial element 鎝 atomic sequence 43, does not exist in the natural environment, mainly enters the environment through nuclear fuel re-production, nuclear test explosion and radioactive drugs, most of which exist in the form of 鎝-99, which will release beta particle radiation and have a long half-life. Up to 21,000 years. Because 鎝-99 is easily soluble in water and is not easily adsorbed, it has high mobility in the environment and has a wide and long-lasting impact on the environment. China has listed 鎝-99 as one of the main nuclear species for radiation waste control. In nuclear power plants, nuclear waste storage sites and environmental monitoring, long-term analysis is required. Therefore, it is necessary to continuously improve the analytical methods to achieve better analytical results.

In the past few decades, it has been customary for China to use radioanalytical methods (RA) with appropriate measuring instruments, such as liquid scintillators, to perform the activity analysis of 鎝-99. Commonly used radiochemical chemistry methods include melting, ion exchange, co-precipitation, and solvent extraction. The common disadvantage of these methods is that it takes a lot of time, usually takes days to weeks to get results, in addition to affecting the timeliness of analysis, at high activity. At the time of sample analysis, the analyst will also receive a considerable amount of radiation exposure. In addition, because 鎝-99 is easily soluble in water, radiochemical analysis methods usually require several heating, dilution and container transfer, which will cause 鎝-99 to escape during operation, resulting in low analytical results, even for measuring instruments. Detected. In the past, commonly used measuring instruments include a low background proportional counter, a liquid scintillation counter, and a neutron activation method. The low background proportional counter and the liquid scintillation counter can only measure the total activity of the Aval or beta particle radiation, and cannot directly identify the 鎝-99, so the sample must be separated and purified by radiochemical analysis; the neutron activation method needs to be matched with the neutron. Source, cannot be widely used.

In view of the above, there is a need for an automatic analysis method that can greatly shorten the operation time, reduce the use of reagents, reduce the cost, and automate the process to reduce the radiation exposure dose and human error of the analyst, to solve the problem. Problems arising from technology.

The main object of the present invention is to provide an automatic analysis method for 鎝-99, which can greatly shorten the operation time, reduce the use of reagents, reduce the cost, and automate the process to reduce the radiation exposure dose and human error of the analyst. The effect.

In a preferred embodiment, the present invention provides an automatic analysis method for strontium-99, which comprises the steps of: preparing a liquid sample comprising weighing an appropriate amount of a solid sample, the solid sample and an appropriate amount Concentrated nitrate After the acid and hydrofluoric acid are put into the digestion bottle, the microwave digestion device is placed in a digestion process, and the liquid that completes the digestion process is transferred to a beaker to be evaporated to dryness, and an appropriate amount of nitric acid is added to the beaker to dissolve the contents of the beaker. In nitric acid, the solution of the beaker is controlled to a suitable concentration and volume of the liquid sample; cleaning an ion exchange resin comprising soaking an appropriate amount of the ion exchange resin in a suitable period of time using 18.2 ohms of deionized water. Putting the ion exchange resin into a packed column of an ion exchange resin system for use, immersing the ion exchange resin in a suitable concentration of nitric acid for a period of time before using the ion exchange resin; using a flow injection analysis method The calibration curve liquid is sent to an inductively coupled plasma mass spectrometer for testing; the flow injection analysis method is used to separate and purify the liquid sample through the ion exchange resin system, which comprises using a flow injection analysis instrument to a liquid sample is added to the ion exchange resin to control at least one valve of the flow injection analysis instrument and a pump, a suitable concentration of nitric acid solution is injected into the ion exchange system at an appropriate flow rate, and the flow injection analysis instrument is used to dissolve cesium-99 from the ion exchange resin system; dilution is performed using the flow injection analysis method a solution containing cerium-99; the diluted cerium-99-containing solution was introduced into the inductively coupled plasma mass spectrometer using the flow injection analysis; and 鎝-99 was measured using the inductively coupled plasma mass spectrometer.

In order to enable the reviewing committee to have a further understanding and understanding of the features, objects and functions of the present invention, the relevant detailed structure of the system of the present invention and the concept of the design are explained below so that the reviewing committee The features of the present invention can be understood. The detailed description is as follows: The present invention provides an automatic analysis method for 鎝-99, which comprises the step 1 using a flow injection analysis (FIA) to pass a liquid sample through an ion exchange. The resin system is separated and purified; in step 2, the solution containing cesium-99 is diluted by flow injection analysis; and in step 3, the diluted cesium-99-containing solution is introduced into the inductively coupled plasma mass spectrometer by flow injection analysis. Mass spectrometry, ICP-MS); Step 4 uses the inductively coupled plasma mass spectrometer to measure 鎝-99.

The flow injection analysis method is simply to transport a carrier fluid of a certain flow rate in a narrow pipe and to inject a precise and trace amount of liquid sample into the carrier fluid. The injected liquid sample is passed through a length of thin tube. After the reagent solution is reacted, the signal is continuously recorded by a continuously detectable detector, and the relative concentration of the sample can be measured compared with the signal of the standard solution, and the time based on the arrival of the sample strip to the detector can be accurately controlled. There is no need to waste a longer signal when the reaction is completely balanced. The flow injection analysis method of the present invention uses a flow injection analysis instrument comprising a plurality of valves and pumps, and the flow injection analysis instrument is used to carry the carrier fluid and liquid sample and to dilute.

Step 1 is carried out by flow injection analysis (FIA) to pass the liquid sample through an ion exchange resin system, and before the separation and purification, the visible sample type is solid or liquid to determine whether step 0 preparation is required. For liquid samples, if the original sample is a liquid sample, step 1 can be directly performed. However, if the original sample is a solid sample, it needs to be processed into a liquid sample through step 0.鎝-99 related to the present invention For the automatic analysis method, please refer to FIG. 1A to B, which is a schematic diagram of the automatic analysis method of the 鎝-99 of the present invention, which comprises the step 0 of preparing a liquid sample, comprising the step 01, and taking an appropriate amount of one solid sample, in the embodiment. The weight of the solid sample is 0.25 g; in step 02, the solid sample is placed in a digesting bottle with an appropriate amount of concentrated nitric acid and hydrofluoric acid, and then placed in a microwave digestion device for a digestion process. In this embodiment, 0.25 g of solid sample, 9 ml of concentrated nitric acid and 4 ml of hydrofluoric acid are added to the digestion bottle and placed in a microwave digestion unit for digestion; step 03 is to transfer the liquid that completes the digestion process to a beaker to evaporate. In the example, the beaker is made of Teflon; in step 04, an appropriate amount of nitric acid is added to the beaker, the contents of the beaker are dissolved in nitric acid, and the solution in the beaker is controlled to a suitable concentration and volume of the liquid sample. In the present embodiment, the solution has a concentration of 0.01 mol, and the solution has a volume of 50 ml.

Since the liquid sample contains impurities, dissolved matrix and a plurality of nucleus species, it is necessary to carry out step 1 using a flow injection analysis method to separate and purify the liquid sample through an ion exchange resin system, and separate the ruthenium through the ion exchange resin system. However, before proceeding to step 1, it is judged whether or not step 00 is performed by cleaning the ion exchange resin in the ion exchange resin system, which is to clean the ion exchange resin. Step 00 cleaning the ion exchange resin comprises the step 001: using a 18.2 Ω resistance deionized water to soak an appropriate amount of the ion exchange resin for a suitable period of time, in this embodiment, immersing 0.35 g of Eichrom in deionized water. The TEVA resin is 20 hours; in step 002, the ion exchange resin is placed in the packed column of the ion exchange resin system for use; in step 003, the ion exchange resin is immersed in a suitable concentration of nitric acid before using the ion exchange resin. Time, in this example, the TEVA resin was immersed in a 0.01 molar concentration of nitric acid for 1 hour.

After the ion exchange resin has been cleaned, the automatic analysis method of the present invention can be started. First, the valve of the flow injection analysis instrument 010 in the embodiment is introduced. The valve of the flow injection analysis instrument 010 is a ten-phase valve 110. The first valve 1100 of the ten-phase valve is connected to a 0.05 molar concentration of the nitric acid solution 111 through a pipeline; the second valve 1101 of the phase valve is connected to the TEVA resin system 112 through a pipeline; the first of the ten-phase valves The three valve 1102 is connected to a 5 molar concentration nitric acid solution 113 through a first creeping pump 1111. The first creeping pump 1111 can pass the 5 molar concentration nitric acid solution 113 through the third valve 1102. The flow injection analysis instrument 010; the fourth valve 1103 of the ten-phase valve is connected to the 5 molar concentration nitric acid solution 113 through a pipeline, and the 5 molar concentration nitric acid solution 113 can exit the flow injection through the fourth valve 1103. The analytical instrument 010; the fifth valve 1104 of the ten-phase valve is connected through a pipeline to a liquid 114 to be formed into a calibration curve, and the middle end of the pipeline is connected to the first creeping pump 1111; the sixth valve of the ten-phase valve 1105 connects the feeling a coupled plasma mass spectrometer 115; a reactor tube 116 having a three-terminal end, the seventh valve 1106 of the ten-phase valve is connected to a first end 1160 of a reaction vessel, the first of the reaction tubes The second end 1161 is connected to the TEVA resin system 112, and the second end 1161 of the reaction tube and the middle section of the TEVA resin system 112 are connected to the first peristaltic pump 1111, and the third end of the reaction tube is connected to the 1162-deionized The first end 1170 of the water valve 117, the second end 1171 of the deionized water valve 117 is connected to a deionization water tank 1172, and the second detonation water valve 117 and the deionization water tank 1172 are supported by a second creeping gang. Connected to the pipeline of Pu 1173; the eighth valve 1107 of the ten-phase valve is connected to a waste liquid tank 118; the ninth valve 1108 of the ten-phase valve is connected to a 0.75 molar concentration nitric acid solution 119 through the pipeline; The tenth valve 1109 in the valve is connected to the 0.75 molar concentration nitric acid solution 119 through a pipeline, and the 0.75 molar concentration nitric acid solution 119 acts to use the 0.75 molar concentration nitric acid solution at the end of the flow injection analysis. 119 to clean the flow injection analysis instrument 010.

Before starting step 1, step 000 may be performed by using a flow injection analysis method to send a liquid to be prepared into a calibration curve into the inductively coupled plasma mass spectrometer for testing, as shown in FIG. In order to use the flow injection analysis method, the liquid to be prepared into a calibration curve is sent to the schematic diagram of the inductively coupled plasma mass spectrometer. In this embodiment, only the fifth valve 1104 and the sixth valve 1105 of the ten-phase valve 110 are opened. At this time, the nitric acid liquid 114 to be prepared into a calibration curve can be sent to the inductively coupled plasma mass spectrometer 115 for testing.

Step 1 includes step 10 in which a liquid sample is added to the ion exchange resin. In step 11, the valve and the peristaltic pump of the flow injection analysis instrument are controlled, and an appropriate concentration of the nitric acid solution is injected into the ion exchange system at an appropriate flow rate. Referring to FIG. 3, the flow injection analysis instrument is controlled to make the nitric acid. A schematic of a solution injected into an ion exchange system. By opening the first valve 1100 and the second valve 1101 of the flow injection analysis instrument, the 0.05 molar concentration of the nitric acid solution 111 is injected into the TEVA resin system 112 by the first peristaltic pump 1111 of the flow injection analysis instrument 010. At this time, the third valve 1102 and the fourth valve 1103 are both closed, so the 5 molar concentration of the nitric acid solution 113 does not enter the flow injection analysis instrument 010, and the seventh valve 1106 and the eighth valve 1107 are opened. The waste liquid passing through the TEVA resin system 112 is discharged to the waste liquid tank 118, so that the flow injection analysis instrument 010 is not contaminated, and the ninth valve 1108 and the tenth valve 1109 of the ten-phase valve are closed for The cleaned 0.75 molar concentration of nitric acid solution 119 is not injected into the flow injection analysis instrument 010 at step 11. In this embodiment, the time for performing step 11 is 1000 seconds, and the rotational speed of the first creeping pump is 80%. Step 12 is to dissolve 鎝-99 from the ion exchange resin system using the flow injection analysis instrument. Referring to FIG. 4, the 鎝-99 is dissolved from the ion exchange resin system using the flow injection analysis instrument. schematic diagram. In the present embodiment, the first valve 1100 is closed, so that the 0.05 molar concentration of the nitric acid solution 111 is no longer injected into the TEVA resin system 112, and the third valve 1102 is opened to make the 5 molar concentration of the nitric acid solution 113 by the first The operation of the peristaltic pump 1111 can be injected into the TEVA resin system 112 through the second valve 1101 of the flow injection analysis instrument to dissolve the cesium-99 from the ion exchange resin system. In this embodiment, the time for performing step 12 is 1100 seconds.

In this embodiment, the flow rate of the TEVA resin injected is 3.5 ml/min, and the flow rate of the TEVA resin flowing out is 3.4 ml/min, except that the line connecting the first, second, third, and fourth peristaltic pumps is the inner diameter. For the 1.02 mm space tube (Tygon), the others used a Teflon tube with an inner diameter of 0.76 mm and a length of 30 cm. The first peristaltic pump had a rotational speed of 80%.

Step 2: The solution containing cerium-99 is diluted by flow injection analysis. In this embodiment, in order to dilute the nitric acid solution containing strontium-99, please refer to FIG. 5, which is to dilute cerium by using the flow injection analysis instrument. -99 Schematic diagram of a nitric acid solution. Opening the deionized water valve 117 connected to the third end 1162 of the reaction tube, so that deionized water can enter the deionized water valve 117 connected to the third end 1162 of the reaction tube from the deionized water tank 1172. The reaction tube 116, during which the second peristaltic pump 1173 is four times faster than the flow injection analysis instrument, introduces deionized water into the reaction tube 116, and the deionized water utilizes the entangled Teflon tube and contains cesium. Mixing -99 nitric acid solution, this process can dilute 5 molar concentration of nitric acid to 4% concentration, which avoids inductive coupling due to excessive acidity when introducing nitric acid solution containing yttrium-99 into inductively coupled plasma mass spectrometer The plasma mass spectrometer is damaged.

Step 3 uses a flow injection analysis method to introduce the diluted yttrium-99-containing solution into an inductively coupled plasma mass spectrometer. See Figure 6 for introducing the diluted yttrium-99-containing solution into the induction using flow injection analysis. Schematic diagram of a coupled plasma mass spectrometer. In this embodiment, by closing the eighth valve 1107 and opening the sixth valve 1105, the diluted niobium-containing nitric acid solution can be introduced into the inductively coupled plasma mass spectrometer 115, and the flow rate introduced into the inductively coupled plasma mass spectrometer 115 is 3.4 ml / min.

Step 4 is to measure 鎝-99 using the inductively coupled plasma mass spectrometer. Table 1 shows the results of detecting the 鎝-99 content by inductively coupled plasma mass spectrometer and liquid scintillation counter (known technique). As shown in Table 1, the 鎝-99 content detected by inductively coupled plasma mass spectrometer is used. The signal-to-noise ratio is much higher than that of the liquid scintillation counter; Table 2 is the system recovery rate measured by the analytical method of the present invention. As shown in Table 2, the average system recovery rate is 96.35% in ten experiments. It can be seen that the present invention can accurately measure the content of strontium-99.

Table 1 shows the results of detecting the 鎝-99 content by an inductively coupled plasma mass spectrometer and a liquid scintillation counter (known technique).

Table 2 System recovery table tested by the analytical method of the present invention

The automatic analysis method of 鎝-99 provided by the invention can automate all processes by flow injection analysis without manual replacement by personnel. Moreover, the flow injection analysis method can obtain high reproducibility and high analysis speed by precisely controlling experimental parameters such as reaction rate, reaction time and reaction diffusion degree before the chemical reaction has reached a steady state. In addition, the flow injection analysis method can be freely combined with various types of measuring instruments and analysis techniques, so it is suitable as an automatic control device for the ion exchange process.

In the present invention, the inductively coupled plasma mass spectrometer for analyzing the strontium-99 content can simultaneously quantify a plurality of analytes, and when analyzing samples of a plurality of radioactive nucleus samples, it can be identified for a specific atomic amount, thereby greatly reducing the chance of interference occurrence. . It has the advantages of fast analysis, large linear range, easy automation and system integration, and is an ideal radioactive nuclear measurement instrument. At present, the application range of nuclear analysis of inductively coupled plasma mass spectrometers has included the characteristics of nuclear materials, nuclear recycling and by-products, radioactive waste, environmental monitoring, biomedical analysis, health monitoring, geochemistry, geological age and other fields. Identification.

The invention combines the advantages of both, can shorten the analysis time from several days and weeks to 24 hours, greatly shorten the analysis time, reduce the use of reagents, effectively reduce the cost, and the flow injection analysis method and the inductively coupled plasma mass spectrometer Both operate automatically through a computer program, which reduces operator error and reduces the amount of radiation exposure that analysts are exposed to. In addition, the present invention is a closed system, and the 鎝-99 is not easy to escape during the analysis, and the original 鎝-99 is preserved in the past method to ensure the correctness of the analysis result. Based on the above advantages, the present invention is well suited for use in nuclear power plants, nuclear waste storage sites, and environmental monitoring and utilization.

The above is only the preferred embodiment of the present invention, and the scope of the present invention is not limited thereto. That is, the equivalent changes and modifications made by the present invention in the scope of the present invention will remain as the further embodiment of the present invention.

0. . . Preparation of liquid samples

01~04. . . step

00. . . Clean ion exchange resin

001~003. . . step

000. . . The liquid to be prepared into a calibration curve is sent to the inductively coupled plasma mass spectrometer for testing using a flow injection analysis method.

010. . . Flow injection analysis instrument

110. . . Ten phase valve

1100. . . The first valve in the ten-phase valve

1101. . . The second valve in the ten-phase valve

1102. . . The third valve in the ten-phase valve

1103. . . The fourth valve in the ten-phase valve

1104. . . The fifth valve in the ten-phase valve

1105. . . The sixth valve in the ten-phase valve

1106. . . The seventh valve in the ten-phase valve

1107. . . The eighth valve in the ten-phase valve

1108. . . The ninth valve in the ten-phase valve

1109. . . The tenth valve in the ten-phase valve

111. . . 0.05 molar concentration of nitric acid solution

1111. . . First peristal pump

112. . . TEVA resin system

113. . . 5 molar concentration of nitric acid solution

114. . . a liquid to be made into a calibration curve

115. . . Inductively coupled plasma mass spectrometer

116. . . Reaction tube

1160. . . First end of the reaction tube

1161. . . Second end of the reaction tube

1162. . . Third end of the reaction tube

117. . . Deionized water valve

1170. . . First end of deionized water valve

1171. . . Second end of deionized water valve

1172. . . Deionized sink

1173. . . Second peristal pump

118. . . Waste tank

119. . . 0.75 molar concentration of nitric acid solution

1. . . The flow injection analysis method is used to separate and purify the liquid sample through the ion exchange resin system.

10~12. . . step

2. . . Use this flow injection assay to dilute a solution containing strontium-99

3. . . Using the flow injection analysis method to introduce the diluted yttrium-99-containing solution into an inductively coupled plasma mass spectrometer

4. . . Measurement using the inductively coupled plasma mass spectrometer 鎝-99

Figure 1A to B are schematic diagrams of the automatic analysis method of the 鎝-99 of the present invention.

Figure 2 is a schematic diagram showing the flow of a liquid to be prepared into a calibration curve into the inductively coupled plasma mass spectrometer using flow injection analysis.

Figure 3 is a schematic diagram of controlling the flow injection analysis instrument to inject a nitric acid solution into the ion exchange system.

Figure 4 is a schematic diagram of the dissolution of yttrium-99 from an ion exchange resin system using the flow injection analysis instrument.

Figure 5 is a schematic diagram of diluting a solution containing cerium-99 nitric acid using the flow injection analysis instrument.

Figure 6 is a schematic diagram showing the introduction of a diluted solution containing cerium-99 into an inductively coupled plasma mass spectrometer using flow injection analysis.

0. . . Preparation of liquid samples

01~04. . . step

00. . . Clean ion exchange resin

001~003. . . step

000. . . The liquid to be prepared into a calibration curve is sent to the inductively coupled plasma mass spectrometer for testing using a flow injection analysis method.

1. . . The flow injection analysis method is used to separate and purify the liquid sample through the ion exchange resin system.

10~12. . . step

2. . . Use this flow injection assay to dilute a solution containing strontium-99

3. . . Using the flow injection analysis method to introduce the diluted yttrium-99-containing solution into an inductively coupled plasma mass spectrometer

4. . . The 鎝-99 was measured using the inductively coupled plasma mass spectrometer.

Claims (7)

An automatic analysis method for 鎝-99, comprising the steps of: using a flow injection analysis method to feed a liquid to be prepared into a calibration curve into an inductively coupled plasma mass spectrometer for testing; using the flow injection analysis method Separating and purifying a liquid sample through an ion exchange resin system, comprising adding the liquid sample to an ion exchange resin using a flow injection analysis instrument, controlling at least one valve and the peristaltic pump of the flow injection analysis instrument to An appropriate concentration of nitric acid solution is injected into the ion exchange system at an appropriate flow rate, and 鎝-99 is eluted from the ion exchange resin system using the flow injection analysis instrument; dilution is carried out using the flow injection analysis method containing 鎝-99 a solution; the diluted cerium-99-containing solution is introduced into the inductively coupled plasma mass spectrometer using the flow injection analysis; and the 鎝-99 is measured using the inductively coupled plasma mass spectrometer. According to the automatic analysis method of 鎝-99 described in claim 1 of the patent application, the method further comprises the following steps of preparing the liquid sample, which comprises weighing an appropriate amount of a solid sample, and the solid sample and an appropriate amount of concentrated nitric acid And the hydrofluoric acid is placed in the digestion bottle and placed in a microwave digestion device for a digestion process, the liquid that completes the digestion process is transferred to a beaker and evaporated to dryness, and an appropriate amount of nitric acid is added to the beaker to dissolve the contents of the beaker into the nitric acid. And controlling the solution in the beaker to a suitable concentration and volume of the liquid sample; and cleaning the ion exchange resin comprising soaking an appropriate amount of the ion exchange resin in a suitable period of time using 18.2 ohms of deionized water Putting the ion exchange resin into the packed column of the ion exchange resin system for use, so that The ion exchange resin is immersed in a suitable concentration of nitric acid for a period of time before the ion exchange resin. The automatic analysis method of 鎝-99 according to the first aspect of the patent application, wherein the automatic analysis method of 鎝-99 is carried out in a closed system. According to the automatic analysis method of 鎝-99 described in the first application of the patent scope, the flow injection analysis method and the inductively coupled plasma mass spectrometer are automatically controlled by using a computer. An automatic analysis method for strontium-99, comprising the steps of: preparing a liquid sample comprising weighing an appropriate amount of a solid sample, and placing the solid sample with an appropriate amount of concentrated nitric acid and hydrofluoric acid into the digestion bottle Put into the microwave digestion device for a digestion process, move the liquid that completes the digestion process to a beaker, and add an appropriate amount of nitric acid to the beaker to dissolve the contents of the beaker into nitric acid, and control the beaker solution to a suitable concentration and volume of the liquid sample; cleaning an ion exchange resin comprising soaking an appropriate amount of the ion exchange resin using a 18.2 Ω resistance deionized water for a suitable period of time, placing the ion exchange resin in an ion exchange Filling the column of the resin system for use, immersing the ion exchange resin in a suitable concentration of nitric acid for a period of time before using the ion exchange resin; using a flow injection analysis method to feed the liquid to be prepared into a calibration curve into an inductively coupled electricity Testing in a plasma mass spectrometer; using the flow injection analysis to pass the liquid sample through the ion exchange resin system Purification line, which line comprises a flow injection analysis using a liquid sample into the instrument of the ion-exchange resin, to control the flow of the at least one injection valve and the analytical instrument of the peristaltic pump, an appropriate amount of the nitrate concentration An acid solution is injected into the ion exchange system at a suitable flow rate, and 鎝-99 is eluted from the ion exchange resin system using the flow injection analysis instrument; the solution containing strontium-99 is diluted using the flow injection analysis; The flow injection analysis method introduces the diluted cerium-99-containing solution into the inductively coupled plasma mass spectrometer; and the 鎝-99 is measured using the inductively coupled plasma mass spectrometer. The automatic analysis method of 鎝-99 according to item 5 of the patent application scope, wherein the automatic analysis method of 鎝-99 is carried out in a closed system. According to the automatic analysis method of 鎝-99 described in claim 5, the flow injection analysis method and the inductively coupled plasma mass spectrometer are automatically controlled by using a computer.