RADIOACTIVE IODINE ADSORBENT, AND METHOD FOR TREATING RADIOACTIVE IODINE
20210304912 · 2021-09-30
Assignee
Inventors
Cpc classification
G21C9/00
PHYSICS
B01D53/685
PERFORMING OPERATIONS; TRANSPORTING
B01J20/28004
PERFORMING OPERATIONS; TRANSPORTING
Y02E30/30
GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
Y02E30/00
GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
B01J20/28011
PERFORMING OPERATIONS; TRANSPORTING
International classification
B01J20/18
PERFORMING OPERATIONS; TRANSPORTING
B01J20/28
PERFORMING OPERATIONS; TRANSPORTING
G21C9/00
PHYSICS
Abstract
Provided is a method for treating radioactive iodine contained in steam discharged from a nuclear power facility, including a filling step of filling an air-permeable container with a granulated radioactive iodine adsorbent of zeolite X, wherein ion exchange sites of the zeolite X are substituted with silver so that a size of minute pores of the zeolite X is suited to a size of a hydrogen molecule, and the radioactive iodine adsorbent has a silver content of 36 wt % or more when dried, a particle size of 10×20 mesh, a hardness of 94% or more, and a water content of 12 wt % or less when dried at 150° C. for 3 h and thereby reduced in weight; and a flow passing step of passing a flow of the steam discharged from the nuclear power facility, through the container filled with the radioactive iodine adsorbent.
Claims
1. A system for preventing leakage of radioactive iodine to an environment external to a nuclear reactor and for reducing an amount of hydrogen generated in a nuclear reactor to prevent nuclear reactor accidents, the system comprising: a nuclear reactor pressure vessel; a turbine in fluid communication with the nuclear reactor pressure vessel; a generator operatively coupled to the turbine; and a radioactive iodine treatment unit in fluid communication with the nuclear reactor pressure vessel and the turbine, the radioactive iodine treatment unit comprising a container having a radioactive iodine adsorbent stored therein, wherein steam from the nuclear reactor pressure vessel is received by the radioactive iodine treatment unit, and the radioactive iodine adsorbent removes radioactive iodine and hydrogen from the steam.
2. The system of claim 1, further comprising: a filter vent located external to the nuclear reactor pressure vessel, wherein the steam from the nuclear reactor pressure vessel is sent to the filter vent, and radioactive iodine in the steam is collected by the filter vent prior to being discharged.
3. The system of claim 2, wherein the filter vent and the radioactive iodine treatment unit are in fluid communication.
4. The system of claim 3, wherein steam treated by the filter vent is sent to the radioactive iodine treatment unit, and a flow of the steam passes through the radioactive iodine adsorbent included in the radioactive iodine treatment unit.
5. The system of claim 3, wherein the radioactive iodine treatment unit is disposed between the nuclear reactor pressure vessel and filter vent, and wherein steam discharged from the nuclear reactor pressure vessel is sent to the radioactive iodine treatment unit prior to being treated by the filter vent.
6. The system of claim 1, wherein a container of the radioactive iodine treatment unit is formed of a heat-resistant and corrosion-resistant material, and the container is provided with a plurality of minute pores.
7. The system of claim 1, wherein the radioactive iodine treatment unit is disposed between the nuclear reactor pressure vessel and the turbine, and radioactive iodine and hydrogen are absorbed by the radioactive iodine adsorbent prior to the steam being sent to the turbine.
8. The system of claim 1, wherein the nuclear reactor pressure vessel is a part of a pressurized water reactor, the pressurized water reactor comprising a steam generator, the radioactive iodine treatment unit is disposed along a pathway of the steam such that steam is sent from the steam generator to the radioactive iodine treatment unit and, after treatment by the radioactive treatment unit, is provided to the turbine.
9. The system of claim 1, wherein the radioactive iodine adsorbent comprises zeolite X, wherein Sodium at ion exchange sites of zeolite X are substituted with Silver, and wherein the substitution of Silver at the ion exchange sites causes minute pores of zeolite X to reduce in size to a size of a Hydrogen molecule.
10. The system of claim 9, wherein, when dried, a content of Silver in zeolite X is 36 wt % or more, a particle size of zeolite X is 10×20 mesh, a hardness of zeolite X is 94% or more, and a water content of zeolite X is 12 wt % or less.
11. The system of claim 9, wherein 97% or more of the ion exchange sites of zeolite X are substituted with Silver.
Description
BRIEF DESCRIPTION OF DRAWINGS
[0033]
[0034]
[0035]
[0036]
[0037]
[0038]
[0039]
DESCRIPTION OF EMBODIMENTS
[0040] Embodiments of a radioactive iodine adsorbent according to the present invention and embodiments of a method for treating radioactive iodine according to the present invention will now be described with reference to
[0041] <Radioactive Iodine Adsorbent>
[0042] Firstly, zeolite X that is used in a radioactive iodine adsorbent according to the present invention will be described.
[0043] As shown in
[0044] The radioactive iodine adsorbent of the present invention includes zeolite 13X, which is a type of zeolite X. Zeolite 13X is widely industrially used. The composition of zeolite 13X is Na.sub.86[(AlO.sub.2).sub.86(SiO.sub.2).sub.106].276H.sub.2O. As shown in
[0045] Incidentally, when sodium sites in zeolite 13X are ion-exchanged with silver, the resultant zeolite 13X has a smaller pore diameter size than that of the original zeolite 13X. The present inventors have extensively studied to find that zeolite 13X that is adapted to have a smaller pore diameter size is effective in adsorbing hydrogen, and have conceived of using such zeolite 13X as a radioactive iodine adsorbent. Specifically, as shown in
[0046] The radioactive iodine adsorbent of the present invention is preferably formulated so that, in addition to the feature that the above ion exchange ratio is achieved, the proportion of the silver component (silver content) in the adsorbent when dried is 36 wt % or more, the particle size is 10×20 mesh (JIS K 1474-4-6), the hardness is 94% or more (JIS K 1474-4-7), and the water content of the adsorbent when dried at 150° C. for 3 h and thereby reduced in weight is 12 wt % or less. As used herein, the term “10×20 mesh” with respect to the size of a particle means that the particle can pass through a 10-mesh sieve, but not through a 20-mesh sieve, i.e., that the particle size is 10-20 mesh. If a radioactive iodine adsorbent is formulated to have such properties, the radioactive iodine adsorbent can more effectively exhibit the above high hydrogen molecule adsorptivity. Radioactive iodine adsorbents are exposed to a severe environment (high temperature, high pressure, high humidity), and therefore, are required to have a certain high particle strength. With this in mind, the radioactive iodine adsorbent of the present invention is preferably adapted to have a loss on attrition of 3% or less (ASTM D-4058). As a result, even if the radioactive iodine adsorbent is placed under severe conditions such as filter venting or the like, the radioactive iodine adsorbent can maintain its particle shape, and therefore, continue to exhibit high hydrogen molecule adsorptivity.
[0047] <Method for Treating Radioactive Iodine>
[0048] Before describing a method for treating radioactive iodine using the radioactive iodine adsorbent formulated as described above, the structure of a typical nuclear power plant will be described with reference to
First Embodiment
[0049] (Filling Step)
[0050]
[0051] (Flow Passing Step)
[0052] While, as described above, the filter vent 15 can be used to reduce the amount of radioactive iodine, it is necessary to substantially completely remove radioactive iodine before discharging the steam or gas from the nuclear reactor building 10 because radioactive iodine has serious deleterious effects on human bodies and environments. Therefore, the radioactive iodine adsorbent K of the present invention is used to substantially completely remove radioactive iodine. As shown in
Second Embodiment
[0053] In the first embodiment, the boiling water reactor 100 is provided with the radioactive iodine treatment unit 1 that is not disposed directly adjacent to the nuclear reactor containment building 11. In contrast to this, in the second embodiment, as shown in
Third Embodiment
[0054] In the first and second embodiments, it is assumed that an emergency situation occurs due to an accident or the like in a nuclear reactor facility (the boiling water reactor 100). The radioactive iodine adsorbent K and the method for treating radioactive iodine according to the present invention can be used in not only emergency situations but also other situations. In particular, in the boiling water reactor 100, steam is sent directly from the nuclear reactor pressure vessel 12 to the turbine 13 as described above, and therefore, it is necessary to strictly manage the amounts of radioactive iodine and hydrogen in order to ensure the safety. To this end, as shown in
Fourth Embodiment
[0055] The first to third embodiments are all directed to boiling water reactors. The radioactive iodine adsorbent K and the method for treating radioactive iodine according to the present invention are also applicable to pressurized water reactors (PWR). As shown in
EXAMPLES
Example 1
[0056] In Example 1, a test for adsorption of radioactive iodine using the method for treating radioactive iodine according to the present invention was conducted.
[0057] Initially, 97% of the sodium sites of zeolite 13X were ion-exchanged with silver, followed by granulation, so that the silver component was 36 wt %, the particle size was 10×20 mesh (JIS K 1474-4-6), and the water content when dried at 150° C. for 3 h was 12 wt %. An air-permeable container was filled with the resultant zeolite 13X, where the filling density was 1.0 g/ml. Thus, a radioactive iodine adsorbent was formulated. The radioactive iodine adsorbent thus formulated had a hardness of 94% (JIS K 1474-4-7). Next, various radioactive iodine adsorbents having different thicknesses were measured in terms of the steam retaining time in the container and the methyl iodide adsorption effect, with respect to steam, where the steam had a humidity of 95%, a temperature of 130° C., and a pressure of 399 kPa, and contained 1.75 mg/m.sup.3 of methyl iodide (CH.sub.3.sup.131I), and had a linear speed of 20 cm/sec and 41 cm/sec. The result of the measurement is shown in Table 1.
TABLE-US-00001 TABLE 1 20 cm/sec 41 cm/sec Thickness Retaining time Adsorption rate Thickness Retaining time Adsorption rate (cm) (sec) (%) (cm) (sec) (%) 2.5 0.123 99.032 2.5 0.061 97.989 5.0 0.246 99.967 5.0 0.123 99.673 7.5 0.369 >99.999 7.5 0.184 99.843 10.0 0.492 >99.999 10.0 0.246 99.974
[0058] As can be seen from the result of Table 1, even when the linear speed was set to 41 cm/sec, the methyl iodide adsorption rate was high. In particular, even when the retaining time was as short as 0.061 sec, the methyl iodide adsorption rate was 97.989%, which is a good result.
Example 2
[0059] In Example 2, the radioactive iodine adsorbent formulated in Example 1, that had a thickness of 5.0 cm, was measured in terms of the methyl iodide adsorption effect at various temperatures, with respect to steam, where the steam had a pressure of 101 kPa and contained 17 mg/m.sup.3 of methyl iodide (CH.sub.3I), and had a linear speed of 46 cm/sec. The result of the measurement is shown in Table 2.
TABLE-US-00002 TABLE 2 Temperature (° C.) 110 125 150 Adsorption rate (%) 99.90 99.95 99.95
[0060] As can be seen from the result of Table 2, even when the steam had a temperature of as high as 100° C. or more, the methyl iodide adsorption rate was as high as 99% or more.
Example 3
[0061] In Example 3, a filter (100 cm×83 cm) formed of the radioactive iodine adsorbent formulated in Example 1, that had a radioactive iodine adsorbent thickness of 26 mm and a mass of 26 kg, was measured in terms of the methyl iodide adsorption effect at various temperatures, with respect to steam, where the steam had a pressure of 101 kPa and contained 0.608 mg/m.sup.3 of methyl iodide (CH3I), and had a linear speed of 20 cm/sec. The result of the measurement is shown in Table 3.
TABLE-US-00003 TABLE 3 Temperature (° C.) 30 40 70 150 Adsorption rate (%) 99.77 99.85 99.91 99.98
[0062] In Example 3, unlike Examples 1 and 2, the radioactive iodine adsorbent was measured in terms of the adsorption rate, where the radioactive iodine adsorbent had a size and a mass similar to those in actual use. As can be seen from the result of Table 3, in such a case, even when the temperature of the steam increased to as high as 150° C., the methyl iodide adsorption rate was still high. Therefore, it was demonstrated that the radioactive iodine adsorbent of the present invention has practical utility.
Example 4
[0063] In Example 4, the radioactive iodine adsorbent formulated in Example 1 was measured in terms of the methyl iodide adsorption effect for various radioactive iodine adsorbent thicknesses, with respect to steam, where the steam had a pressure of 103 kPa, a temperature of 66° C., and a linear speed of 20.3 cm/sec, and contained 1.75 mg/m.sup.3 of methyl iodide (CH.sub.3.sup.131I), and the humidity was 70%. The result of the measurement is shown in Table 4.
TABLE-US-00004 TABLE 4 Thickness (mm) Retaining time (sec) Adsorption rate ( % ) 50.8 0.250 >99.999 76.2 0.375 >99.999 101.6 0.500 >99.999
Example 5
[0064] In Example 5, the radioactive iodine adsorbent formulated in Example 1 was measured in terms of the methyl iodide adsorption effect related to the thickness and temperature of the radioactive iodine adsorbent, with respect to steam, where the steam had a pressure of 103 kPa and a linear speed of 20.3 cm/sec, and contained 1.75 mg/m.sup.3 of methyl iodide (CH3131I), and the humidity was 95%. The result of the measurement is shown in Table 5.
TABLE-US-00005 TABLE 5 Thickness Retaining Adsorption rate (%) (mm) time (sec) 30° C. 60° C. 90° C. 50.8 0.250 98.738 99.685 99.970 76.2 0.375 99.850 99.950 99.983 101.6 0.500 99.960 99.987 99.995
[0065] As can be seen from the result of Table 4, when the humidity was 70%, the methyl iodide adsorption rate was as high as 99.999% or more in all the cases. Meanwhile, the result of Table 5 shows that even when the humidity was as high as 95%, the methyl iodide adsorption rate was still high. Therefore, it is demonstrated that the radioactive iodine adsorbent of the present invention has a high adsorption effect even at high humidity.
Example 6
[0066] In Example 6, the radioactive iodine adsorbent formulated in Example 1 was measured in terms of the methyl iodide adsorption effect at various temperatures in a dried state, with respect to steam, where the steam had a pressure of 101 kPa and a linear speed of 20 cm/sec, the radioactive iodine adsorbent had a thickness of 5.0 cm, the retaining time was 0.25 sec, and the steam contained 1.75 mg/m.sup.3 of methyl iodide (CH313II). The result of the measurement is shown in Table 6.
TABLE-US-00006 TABLE 6 Temperature (° C.) 30 80 150 Adsorption rate (%) 99.9 99.9 99.9
[0067] As can be seen from the result of Table 6, even when the temperature was as high as 150° C., the methyl iodide adsorption rate was high.
Example 7
[0068] In Example 7, the radioactive iodine adsorbent formulated in Example 1 was measured in terms of the methyl iodide adsorption effect at various humidity at a temperature of 80° C., with respect to steam, where the steam had a pressure of 101 kPa and a linear speed of 20 cm/sec, the radioactive iodine adsorbent had a thickness of 5.0 cm, the retaining time was 0.25 sec, and the steam contained 1.75 mg/m.sup.3 of methyl iodide (CH.sub.3.sup.131I). The result of the measurement is shown in Table 7.
TABLE-US-00007 TABLE 7 Humidity (%) 0 70 90 Adsorption rate (%) 99.9 99.9 99.9
[0069] As can be seen from the result of Table 7, even when the humidity was as high as 90% at a temperature of 80° C., the methyl iodide adsorption rate was high.
Example 8
[0070] In Example 8, the radioactive iodine adsorbent formulated in Example 1 was measured in terms of the methyl iodide adsorption effect related to the thickness and temperature of the radioactive iodine adsorbent in a dried state under atmospheric pressure, with respect to steam, where the steam had a pressure of 104 kPa and a linear speed of 20 cm/sec, and contained 75 mg/m.sup.3 of iodine (.sup.131I). The result of the measurement is shown in Table 8.
TABLE-US-00008 TABLE 8 Thickness (cm) Retaining time (sec) Adsorption rate (%) 2.5 0.123 100 5.0 0.246 100 10.0 0.492 100
[0071] As can be seen from the result of Table 8, the iodine adsorption rate was 100% in a dried state under atmospheric pressure in all the cases. It was demonstrated that the radioactive iodine adsorbent has considerably high performance.
Example 9
[0072] In Example 9, the radioactive iodine adsorbent formulated in Example 1 was measured in terms of the hydrogen adsorption effect, where the radioactive iodine adsorbent had a thickness of 5 cm. The result of the measurement is shown in Table 9.
TABLE-US-00009 TABLE 9 Hydrogen Flow Hydrogen content rate of Flow contentbefore after humidified rate of Retaining passage Increase in passage air hydrogen time of flow Temperature temperature of flow (ml/min) (ml/min) (sec) (%) (° C.) (° C.) (%) 2200 45 2.62 2.0 54 — 1.2 62 — 0.8 79 — 0.5 2200 68 2.60 3.0 77 — 1.0 117 2 <0.5 137 15 <0.5 6600 205 0.87 3.0 75 1 >1.5 120 15 <0.5 136 17 <0.5
[0073] As can be seen from the result of Table 9, when the temperature is as high as 100° C. or more, the hydrogen content after a flow of the steam was passed through the radioactive iodine adsorbent was 0.5% or less, i.e., about 83% or more of hydrogen were adsorbed. It was also observed that when the temperature was 137° C. or 136° C., the temperature increased by 15° C. and 17° C., respectively. Even in this case, the hydrogen content after a flow of the steam was passed through the radioactive iodine adsorbent was 0.5% or less. This demonstrates that the radioactive iodine adsorbent of the present invention is a high-performance adsorbent that can adsorb hydrogen in a stable manner even at high temperature.
Example 10
[0074] In Example 10, the radioactive iodine adsorbent formulated in Example 1 was measured in terms of an increase in temperature, with respect to steam having a hydrogen content of 3%, where a flow of the steam was passed through the radioactive iodine adsorbent having a temperature of 136° C., and the hydrogen content after a flow of the steam was passed through the radioactive iodine adsorbent was 0.5% or less. The result of the measurement is indicated by a graph shown in
[0075] As can be seen from the graph of
[0076] The results of Examples 1-8 demonstrate that the radioactive iodine adsorbent of the present invention and the method for treating radioactive iodine using the same have a considerably excellent adsorption effect on steam having high temperature, high pressure and high humidity, and in addition, a quick and efficient adsorption effect. Moreover, the results of Examples 9 and 10 demonstrate that the radioactive iodine adsorbent of the present invention effectively adsorbs hydrogen as well as radioactive iodine with high efficiency.
INDUSTRIAL APPLICABILITY
[0077] The radioactive iodine adsorbent and the method for treating radioactive iodine according to the present invention are effective in avoiding or controlling the risks of leakage and release of radioactive iodine, nuclear reactor accidents, and the like in a nuclear reactor facility.
REFERENCE SIGNS LIST
[0078] 1 RADIOACTIVE IODINE TREATMENT UNIT [0079] 2 CONTAINER [0080] 10 NUCLEAR REACTOR BUILDING [0081] 11, 20 NUCLEAR REACTOR CONTAINMENT BUILDING [0082] 12, 21 NUCLEAR REACTOR PRESSURE VESSEL [0083] 100 BOILING WATER REACTOR [0084] 200 PRESSURIZED WATER REACTOR [0085] K RADIOACTIVE IODINE ADSORBENT