USH800H - Method for gettering organic, inorganic and elemental iodine in aqueous solutions - Google Patents
Method for gettering organic, inorganic and elemental iodine in aqueous solutions Download PDFInfo
- Publication number
- USH800H USH800H US07/341,005 US34100589A USH800H US H800 H USH800 H US H800H US 34100589 A US34100589 A US 34100589A US H800 H USH800 H US H800H
- Authority
- US
- United States
- Prior art keywords
- iodine
- organic
- gettering
- aqueous solutions
- sub
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Abandoned
Links
- ZCYVEMRRCGMTRW-UHFFFAOYSA-N 7553-56-2 Chemical compound [I] ZCYVEMRRCGMTRW-UHFFFAOYSA-N 0.000 title claims abstract description 30
- 229910052740 iodine Inorganic materials 0.000 title claims abstract description 30
- 239000011630 iodine Substances 0.000 title claims abstract description 30
- 238000000034 method Methods 0.000 title claims abstract description 16
- 239000007864 aqueous solution Substances 0.000 title claims abstract description 8
- 238000005247 gettering Methods 0.000 title claims abstract description 4
- 230000008569 process Effects 0.000 claims abstract description 8
- 239000000243 solution Substances 0.000 claims abstract description 8
- ZXSQEZNORDWBGZ-UHFFFAOYSA-N 1,3-dihydropyrrolo[2,3-b]pyridin-2-one Chemical compound C1=CN=C2NC(=O)CC2=C1 ZXSQEZNORDWBGZ-UHFFFAOYSA-N 0.000 claims abstract description 6
- 229910001958 silver carbonate Inorganic materials 0.000 claims abstract description 6
- LKZMBDSASOBTPN-UHFFFAOYSA-L silver carbonate Substances [Ag].[O-]C([O-])=O LKZMBDSASOBTPN-UHFFFAOYSA-L 0.000 claims abstract description 6
- PNDPGZBMCMUPRI-UHFFFAOYSA-N iodine Chemical compound II PNDPGZBMCMUPRI-UHFFFAOYSA-N 0.000 claims description 4
- 150000004694 iodide salts Chemical class 0.000 abstract description 12
- 230000002285 radioactive effect Effects 0.000 abstract description 6
- 150000002497 iodine compounds Chemical class 0.000 abstract description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 12
- 239000007787 solid Substances 0.000 description 4
- 239000004327 boric acid Substances 0.000 description 3
- XMBWDFGMSWQBCA-UHFFFAOYSA-N hydrogen iodide Chemical compound I XMBWDFGMSWQBCA-UHFFFAOYSA-N 0.000 description 3
- 229910001505 inorganic iodide Inorganic materials 0.000 description 3
- OAKJQQAXSVQMHS-UHFFFAOYSA-N Hydrazine Chemical compound NN OAKJQQAXSVQMHS-UHFFFAOYSA-N 0.000 description 2
- KGBXLFKZBHKPEV-UHFFFAOYSA-N boric acid Chemical compound OB(O)O KGBXLFKZBHKPEV-UHFFFAOYSA-N 0.000 description 2
- 239000003153 chemical reaction reagent Substances 0.000 description 2
- 239000003638 chemical reducing agent Substances 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 230000004992 fission Effects 0.000 description 2
- AKHNMLFCWUSKQB-UHFFFAOYSA-L sodium thiosulfate Chemical group [Na+].[Na+].[O-]S([O-])(=O)=S AKHNMLFCWUSKQB-UHFFFAOYSA-L 0.000 description 2
- 235000019345 sodium thiosulphate Nutrition 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- JKFYKCYQEWQPTM-UHFFFAOYSA-N 2-azaniumyl-2-(4-fluorophenyl)acetate Chemical compound OC(=O)C(N)C1=CC=C(F)C=C1 JKFYKCYQEWQPTM-UHFFFAOYSA-N 0.000 description 1
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 description 1
- 229910021612 Silver iodide Inorganic materials 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000000872 buffer Substances 0.000 description 1
- 229910052792 caesium Inorganic materials 0.000 description 1
- 238000005341 cation exchange Methods 0.000 description 1
- -1 cesium ions Chemical class 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 238000004140 cleaning Methods 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 150000002496 iodine Chemical class 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 230000000116 mitigating effect Effects 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 239000006174 pH buffer Substances 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 229940045105 silver iodide Drugs 0.000 description 1
- 239000002002 slurry Substances 0.000 description 1
- DHCDFWKWKRSZHF-UHFFFAOYSA-N sulfurothioic S-acid Chemical compound OS(O)(=O)=S DHCDFWKWKRSZHF-UHFFFAOYSA-N 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
Classifications
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
- G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
- G21F9/02—Treating gases
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
- G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
- G21F9/04—Treating liquids
- G21F9/06—Processing
- G21F9/12—Processing by absorption; by adsorption; by ion-exchange
Definitions
- the invention was developed pursuant to a contract with the United States Department of Energy.
- This invention relates to the removal of iodine from aqueous solutions, particularly the trapping of radioactive iodine to mitigate damage resulting from accidents or spills associated with nuclear reactors.
- the subject invention relates to methods for removing iodine, particularly molecular I 2 and organic iodide compounds, from water pools.
- iodine particularly molecular I 2 and organic iodide compounds
- a principal area of need for this technology is the nuclear reactor industry where it is important to restrict release of radioactive iodine which can occur in accident situations or from mishandling during normal operations.
- iodine-containing water pools will be present in the containment structure. Controlling the release of the iodine from the water pools will be a significant factor in the mitigation of damage.
- the most troublesome of this class of compounds are the organic iodides for which no easy method of removal is presently available.
- An additional object of this invention is to provide a process for cleaning spills in the event of a nuclear reactor accident.
- the process of this invention may comprise removing iodine and iodide compounds from aqueous solution by exposing the solution to well dispersed silver carbonate which reacts with the iodine and iodides, thereby gettering iodine and iodine compounds from solution.
- the invention is based on the discovery that silver carbonate well dispersed in water converts virtually all iodine including elemental iodine, inorganic iodides and organic iodides into a nonvolatile form. Elemental iodine and organic iodides are chemical forms of iodine that can volatilize from water pools. In severe nuclear reactor accidents, water pools would contain boric acid and would be irradiated from fission products and fuel debris. This invention has been shown to be effective in both irradiated and unirradiated water pools and also in water pools with or without boric acid.
- I 2 may be treated ar a lower concentration of 1 ⁇ 10 -4 mol/L, but conversion of organic iodide is increased when a concentration of 1 ⁇ 10 -3 mol/L is used.
- Dispersal of silver carbonate can be accomplished by placing the material in water in an ultrasonic system and then adding the resulting slurry into the water pool. This not only getters dissolved iodine and iodides by compound formation and precipitation, it also getters volatile iodine and iodides as well.
- the present invention provides the buffer for pH control, the ability to remove both I 2 l and organic iodide, effectiveness under irradiation, and removal of iodine with a solid that is unmatched by alternative methods.
- the next best technique known to the applicants is a combination of a reducing agent such as thiosulfate or hydrazine with a pH buffer such as a borate.
- a reducing agent such as thiosulfate or hydrazine
- a pH buffer such as a borate
- the process is one for removing iodine form solution, it could be used as a method of separating fission products in a waste stream while maintaining low volatility.
- the invention could be used to remove iodine leaving cesium ions which could then be treated by cation exchange. Because of the very low solubility product of silver iodide, this invention also is very effective at removing inorganic iodides from solution.
Landscapes
- Physics & Mathematics (AREA)
- Engineering & Computer Science (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
Abstract
A process for the removal of iodine from aqueous solutions, particularly the trapping of radioactive iodine to mitigate damage resulting from accidents or spills associated with nuclear reactors, by exposing the solution to well dispersed silver carbonate which reacts with the iodine and iodides, thereby gettering iodine and iodine compounds from solution. The iodine is not only removed from solution but also from the contiguous vapor.
Description
The invention was developed pursuant to a contract with the United States Department of Energy.
This invention relates to the removal of iodine from aqueous solutions, particularly the trapping of radioactive iodine to mitigate damage resulting from accidents or spills associated with nuclear reactors.
The subject invention relates to methods for removing iodine, particularly molecular I2 and organic iodide compounds, from water pools. A principal area of need for this technology is the nuclear reactor industry where it is important to restrict release of radioactive iodine which can occur in accident situations or from mishandling during normal operations. In severe nuclear reactor accidents, iodine-containing water pools will be present in the containment structure. Controlling the release of the iodine from the water pools will be a significant factor in the mitigation of damage. The most troublesome of this class of compounds are the organic iodides for which no easy method of removal is presently available.
A wide range of chemicals has been studied at Oak Ridge National Laboratory for effective removal of organic iodides from aqueous solution. One of the best reagents for this purpose is sodium thiosulfate which reacts with organic iodides as well as I2 and I-. Unfortunately sodium thiosulfate is not stable in radioactive environments. Therefore, there is a need for a reagent that can remove the radioactive species of organic iodides as well as I2 and I- from aqueous solution.
In view of the above needs, it is an object of this invention to provide a process for removing iodine from aqueous streams.
It is another object of this invention to provide a process for removing organic and inorganic iodides from radioactive aqueous streams.
An additional object of this invention is to provide a process for cleaning spills in the event of a nuclear reactor accident.
Additional objects, advantages and novel features of the invention will be set forth in part in the description which follows, and in part will become apparent to those skilled in the art upon examination of the following or may be learned by practice of the invention. The objects and advantages of the invention may be realized and attained by means of the instrumentalities an combinations particularly pointed out in the appended claims.
To achieve the foregoing and other objects and in accordance with the purpose of the present invention, as embodied and broadly described herein, the process of this invention may comprise removing iodine and iodide compounds from aqueous solution by exposing the solution to well dispersed silver carbonate which reacts with the iodine and iodides, thereby gettering iodine and iodine compounds from solution. This is an improvement over prior methods that were inappropriate for use in radiation environments.
The invention is based on the discovery that silver carbonate well dispersed in water converts virtually all iodine including elemental iodine, inorganic iodides and organic iodides into a nonvolatile form. Elemental iodine and organic iodides are chemical forms of iodine that can volatilize from water pools. In severe nuclear reactor accidents, water pools would contain boric acid and would be irradiated from fission products and fuel debris. This invention has been shown to be effective in both irradiated and unirradiated water pools and also in water pools with or without boric acid.
In order to practice the invention, it is only necessary to introduce well dispersed silver carbonate into the iodine containing water so that the overall amount, both dissolved and undissolved, is 1×10-3 mol/L. I2 may be treated ar a lower concentration of 1×10-4 mol/L, but conversion of organic iodide is increased when a concentration of 1×10-3 mol/L is used.
Dispersal of silver carbonate can be accomplished by placing the material in water in an ultrasonic system and then adding the resulting slurry into the water pool. This not only getters dissolved iodine and iodides by compound formation and precipitation, it also getters volatile iodine and iodides as well.
The effectiveness of this iodine retaining process has been demonstrated in tests in an open system of aqueous solution and air where air was removed and stripped of iodine at a rate that resulted in replacement of the air volume in one hour. Results of these tests are given in the Table.
______________________________________
OPEN SYSTEM TESTS
Room temperature Ag.sub.2 CO.sub.3 :1 × 10.sup.-3
______________________________________
I.sub.2 control (initially 5 × 10.sup.-5 mol/L I.sub.2)
Without treatment
None 27 138
None 32 309
With Ag.sub.2 CO.sub.3 treatment
98 None detected <0.002
72
0.05 M o-boric acid with
>99 0.002 72
Ag.sub.2 CO.sub.3 treatment
γ irradiated (0.45 Mrad/h)
95 2 29
with Ag.sub.2 CO.sub.3 treatment
Organic iodide control (initially 1 × 10.sup.-4 mol/L CH.sub.3 I)
Without treatment
None 56 66
None 58 186
With Ag.sub.2 CO.sub.3 treatment
95 5 141
γ irradiated (0.45 Mrad/h)
93 7 29
with Ag.sub.2 CO.sub.3 treatment
______________________________________
In all the tests that employed Ag2 CO3, more than 90% of the initial iodine was associated with dispersed or settled solids. These solids can easily be removed by filtration. Also, there was a large reduction in the percentage of the initial iodine that volatilized. Thus, this invention provides for both control of volatility and for removal of iodine from water pools.
the present invention provides the buffer for pH control, the ability to remove both I2 l and organic iodide, effectiveness under irradiation, and removal of iodine with a solid that is unmatched by alternative methods. The next best technique known to the applicants is a combination of a reducing agent such as thiosulfate or hydrazine with a pH buffer such as a borate. However, this would not be stable under irradiation, and the reducing agents are subject to depletion by atmospheric oxidation. In addition, such a technique would not permit removal with solids.
Since the process is one for removing iodine form solution, it could be used as a method of separating fission products in a waste stream while maintaining low volatility. For example, the invention could be used to remove iodine leaving cesium ions which could then be treated by cation exchange. Because of the very low solubility product of silver iodide, this invention also is very effective at removing inorganic iodides from solution.
Claims (1)
1. A process for removing iodine, from aqueous solution and from vapor contiguous thereto comprising exposing an iodine-containing solution to well dispersed silver carbonate which reacts with said iodine, thereby gettering said iodine from solutio and contiguous vapor.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| US07/341,005 USH800H (en) | 1989-04-20 | 1989-04-20 | Method for gettering organic, inorganic and elemental iodine in aqueous solutions |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| US07/341,005 USH800H (en) | 1989-04-20 | 1989-04-20 | Method for gettering organic, inorganic and elemental iodine in aqueous solutions |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| USH800H true USH800H (en) | 1990-07-03 |
Family
ID=23335871
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| US07/341,005 Abandoned USH800H (en) | 1989-04-20 | 1989-04-20 | Method for gettering organic, inorganic and elemental iodine in aqueous solutions |
Country Status (1)
| Country | Link |
|---|---|
| US (1) | USH800H (en) |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20070223645A1 (en) * | 2004-05-19 | 2007-09-27 | Wilfried Ruehle | Bonding Radioactive Iodine in a Nuclear Reactor |
| CN102371192A (en) * | 2010-08-23 | 2012-03-14 | 中国石油化工股份有限公司 | Preparation method of deiodination agent |
Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3865688A (en) | 1970-08-05 | 1975-02-11 | Frank W Kleimola | Passive containment system |
| US3896042A (en) | 1974-02-15 | 1975-07-22 | Us Energy | Low temperature, low pressure hydrogen gettering |
| US3898125A (en) | 1971-12-08 | 1975-08-05 | Gen Electric | Nuclear fuel element containing strips of an alloyed Zr, Ti and Ni getter material |
| US3899392A (en) | 1971-12-08 | 1975-08-12 | Gen Electric | Nuclear fuel element containing particles of an alloyed Zr, Ti and Ni getter material |
| US3969185A (en) | 1973-05-09 | 1976-07-13 | General Electric Company | Getter for nuclear fuel elements |
-
1989
- 1989-04-20 US US07/341,005 patent/USH800H/en not_active Abandoned
Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3865688A (en) | 1970-08-05 | 1975-02-11 | Frank W Kleimola | Passive containment system |
| US3898125A (en) | 1971-12-08 | 1975-08-05 | Gen Electric | Nuclear fuel element containing strips of an alloyed Zr, Ti and Ni getter material |
| US3899392A (en) | 1971-12-08 | 1975-08-12 | Gen Electric | Nuclear fuel element containing particles of an alloyed Zr, Ti and Ni getter material |
| US3969185A (en) | 1973-05-09 | 1976-07-13 | General Electric Company | Getter for nuclear fuel elements |
| US3896042A (en) | 1974-02-15 | 1975-07-22 | Us Energy | Low temperature, low pressure hydrogen gettering |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20070223645A1 (en) * | 2004-05-19 | 2007-09-27 | Wilfried Ruehle | Bonding Radioactive Iodine in a Nuclear Reactor |
| DE102004024722B4 (en) * | 2004-05-19 | 2011-05-26 | Enbw Kraftwerke Ag Kernkraftwerk Philippsburg | Binding of radioactive iodine in a nuclear reactor |
| CN102371192A (en) * | 2010-08-23 | 2012-03-14 | 中国石油化工股份有限公司 | Preparation method of deiodination agent |
| CN102371192B (en) * | 2010-08-23 | 2013-04-03 | 中国石油化工股份有限公司 | Preparation method of deiodination agent |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| US5205999A (en) | Actinide dissolution | |
| US4284472A (en) | Method for enhanced control of radioiodine in the production of fission product molybdenum 99 | |
| US5809394A (en) | Methods of separating short half-life radionuclides from a mixture of radionuclides | |
| US4572797A (en) | Method for removing trace pollutants from aqueous solutions | |
| US5352367A (en) | Process for the separation of radioactive iodine compounds by precipitation | |
| GB1533955A (en) | Method of purifying ion exchanger resin used in nuclear reactors | |
| EP0281672B1 (en) | Minimization of radioactive material deposition in water-cooled nuclear reactors | |
| DE69105884T2 (en) | Process for removing cesium from aqueous solutions with high nitric acid concentration. | |
| USH800H (en) | Method for gettering organic, inorganic and elemental iodine in aqueous solutions | |
| EP1029328B1 (en) | Treatment of organic materials | |
| Sinha et al. | Removal of radioiodine from liquid effluents | |
| US3920577A (en) | Iodine retention during evaporative volume reduction | |
| US4839100A (en) | Decontamination of surfaces | |
| US3852407A (en) | Method for removing alkyl iodides from air by mercuric nitrate solution | |
| JPS6363271B2 (en) | ||
| JPH0727069B2 (en) | Separation method of cesium in nitric acid-containing aqueous solution | |
| US3737373A (en) | Method of decontaminating heavy water cooled and moderated reactor | |
| US4162206A (en) | Separation of iodine from mercury containing scrubbing solutions | |
| Yoshihara et al. | Chemical Effects of the 35Cl (n, ρ) 35S Reaction: I. Protection Effects against Sulfur Oxidation | |
| US4362660A (en) | Mercuric iodate precipitation from radioiodine-containing off-gas scrubber solution | |
| US5489736A (en) | Treatment of solid organic wastes | |
| JPH0149919B2 (en) | ||
| JP2002333498A (en) | Radioactive material decontamination method | |
| EP0261662A2 (en) | Method for removal of iodine in gas | |
| US3658714A (en) | Method of decontaminating radioactive wastes |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| AS | Assignment |
Owner name: UNITED STATES OF AMERICA, THE, AS REPRESENTED BY T Free format text: ASSIGNMENT OF ASSIGNORS INTEREST.;ASSIGNORS:BEAHM, EDWARD C.;SHOCKLEY, WILLIAM E.;REEL/FRAME:005125/0232 Effective date: 19890403 |
|
| STCF | Information on status: patent grant |
Free format text: PATENTED CASE |