US2835699A - Radioactive tracers for pipe lines - Google Patents
Radioactive tracers for pipe lines Download PDFInfo
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- US2835699A US2835699A US2835699DA US2835699A US 2835699 A US2835699 A US 2835699A US 2835699D A US2835699D A US 2835699DA US 2835699 A US2835699 A US 2835699A
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- Prior art keywords
- radioactive
- cesium
- sulfonate
- tracer
- isotope
- 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.)
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- 239000000700 tracer Substances 0.000 title claims description 50
- 229910052792 caesium Inorganic materials 0.000 claims description 46
- LSNNMFCWUKXFEE-UHFFFAOYSA-L Sulphite Chemical compound [O-]S([O-])=O LSNNMFCWUKXFEE-UHFFFAOYSA-L 0.000 claims description 36
- TVFDJXOCXUVLDH-UHFFFAOYSA-N Cesium Chemical compound [Cs] TVFDJXOCXUVLDH-UHFFFAOYSA-N 0.000 claims description 32
- 239000000047 product Substances 0.000 description 18
- 239000007788 liquid Substances 0.000 description 14
- 239000000203 mixture Substances 0.000 description 12
- 230000002285 radioactive Effects 0.000 description 12
- 150000002430 hydrocarbons Chemical class 0.000 description 10
- 239000003208 petroleum Substances 0.000 description 10
- 238000002360 preparation method Methods 0.000 description 10
- 239000000243 solution Substances 0.000 description 10
- 239000004215 Carbon black (E152) Substances 0.000 description 8
- 230000000694 effects Effects 0.000 description 8
- FAPWRFPIFSIZLT-UHFFFAOYSA-M sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 8
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 8
- 230000036499 Half live Effects 0.000 description 6
- 229940098124 cesium chloride Drugs 0.000 description 6
- TVFDJXOCXUVLDH-RNFDNDRNSA-N cesium-137 Chemical compound [137Cs] TVFDJXOCXUVLDH-RNFDNDRNSA-N 0.000 description 6
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 6
- 238000000034 method Methods 0.000 description 6
- 239000002244 precipitate Substances 0.000 description 6
- KEAYESYHFKHZAL-UHFFFAOYSA-N sodium Chemical compound [Na] KEAYESYHFKHZAL-UHFFFAOYSA-N 0.000 description 6
- 229910052708 sodium Inorganic materials 0.000 description 6
- 239000011734 sodium Substances 0.000 description 6
- HEMHJVSKTPXQMS-UHFFFAOYSA-M sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 6
- 239000002904 solvent Substances 0.000 description 6
- AIYUHDOJVYHVIT-UHFFFAOYSA-M Caesium chloride Chemical compound [Cl-].[Cs+] AIYUHDOJVYHVIT-UHFFFAOYSA-M 0.000 description 4
- WATWJIUSRGPENY-UHFFFAOYSA-N antimony Chemical compound [Sb] WATWJIUSRGPENY-UHFFFAOYSA-N 0.000 description 4
- 229910052787 antimony Inorganic materials 0.000 description 4
- 230000005251 gamma ray Effects 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxyl anion Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 4
- 238000002347 injection Methods 0.000 description 4
- 239000007924 injection Substances 0.000 description 4
- 238000000926 separation method Methods 0.000 description 4
- 239000011780 sodium chloride Substances 0.000 description 4
- 150000003871 sulfonates Chemical class 0.000 description 4
- LSNNMFCWUKXFEE-UHFFFAOYSA-N sulfonic acid Chemical compound OS(O)=O LSNNMFCWUKXFEE-UHFFFAOYSA-N 0.000 description 4
- 101710038810 CS2 Proteins 0.000 description 2
- 101710002404 FGG Proteins 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-N HCl Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 2
- 229940057007 Petroleum distillate Drugs 0.000 description 2
- 229910000831 Steel Inorganic materials 0.000 description 2
- 238000009835 boiling Methods 0.000 description 2
- UXVMQQNJUSDDNG-UHFFFAOYSA-L cacl2 Chemical compound [Cl-].[Cl-].[Ca+2] UXVMQQNJUSDDNG-UHFFFAOYSA-L 0.000 description 2
- 230000005591 charge neutralization Effects 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 239000007795 chemical reaction product Substances 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-M chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 101710041798 cys-12 Proteins 0.000 description 2
- 238000007865 diluting Methods 0.000 description 2
- 239000003085 diluting agent Substances 0.000 description 2
- 238000001704 evaporation Methods 0.000 description 2
- 239000012467 final product Substances 0.000 description 2
- 229910000041 hydrogen chloride Inorganic materials 0.000 description 2
- 238000005342 ion exchange Methods 0.000 description 2
- PMZURENOXWZQFD-UHFFFAOYSA-L na2so4 Chemical compound [Na+].[Na+].[O-]S([O-])(=O)=O PMZURENOXWZQFD-UHFFFAOYSA-L 0.000 description 2
- 230000001264 neutralization Effects 0.000 description 2
- 238000006386 neutralization reaction Methods 0.000 description 2
- CTQNGGLPUBDAKN-UHFFFAOYSA-N o-xylene Chemical compound CC1=CC=CC=C1C CTQNGGLPUBDAKN-UHFFFAOYSA-N 0.000 description 2
- 239000003209 petroleum derivative Substances 0.000 description 2
- 229910052938 sodium sulfate Inorganic materials 0.000 description 2
- 235000011152 sodium sulphate Nutrition 0.000 description 2
- 239000010959 steel Substances 0.000 description 2
- 238000003756 stirring Methods 0.000 description 2
- QAOWNCQODCNURD-UHFFFAOYSA-L sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 2
- 238000006277 sulfonation reaction Methods 0.000 description 2
- 239000008399 tap water Substances 0.000 description 2
- 235000020679 tap water Nutrition 0.000 description 2
- 238000003809 water extraction Methods 0.000 description 2
- 239000008096 xylene Substances 0.000 description 2
Classifications
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C309/00—Sulfonic acids; Halides, esters, or anhydrides thereof
- C07C309/01—Sulfonic acids
- C07C309/62—Sulfonated fats, oils or waxes of undetermined constitution
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
- A61K51/00—Preparations containing radioactive substances for use in therapy or testing in vivo
- A61K51/02—Preparations containing radioactive substances for use in therapy or testing in vivo characterised by the carrier, i.e. characterised by the agent or material covalently linked or complexing the radioactive nucleus
- A61K51/04—Organic compounds
Definitions
- This invention relates to liquid radioactive tracers and methods for their preparation, and particularly refers to those prepared from isotopes of cesium that are of specific utility in tracing the flow of liquid hydrocarbons through pipe lines.
- a suitable method that has been developed consists in the introduction into the interface between successive different products of a small quantity of an oil-soluble liquid carrying a radioisotope that can be detected outside of the pipe line at any point along the length.
- the isotope is chosen to be a gamma-emitter, and compounds of radioactive antimony and the like have been employed, as described in the Patent No. 2,706,254 of R. C. Mithoff and D. E. Hull.
- This invention is particularly directed to improve longlived liquid radioactive tracers, particularly but not necessarily exclusively suited for such pipe line operations, and employing radioisotopes of cesium, namely, Cs having a 2.3 year half-life and emitting gamma radiation in the 0.57-0.79 m. e. v. range, and Cs having a 37 year half-life which does not emit gamma radiation but is in equilibrium with a 2.6 minute Ba daughter emitting 0.66 m. e. v. gamma radiation.
- a given number of millicuries of the Cs isotope is about twice as specifically effective as the Cs
- the radioactive tracer composition containing either isotope may be prepared by the procedures which will be described below.
- the C8137 isotope has the advantage of a longer effective life, which can be of substantial importance in certain tracer applications.
- the earlier-used antimony isotopes having a 60-day half-life, required frequent preparation in small quantities, due to their rapid decay, and were accordingly more expensive to prepare and to store.
- Another object is to provide an improved method of preparing a radioactive tracer composition that may be carried out conveniently and with safety to the operator.
- Another object is to provide an improved method of purifying a sulfonate component of a radioactive liquid tracer to produce a product having desirable characteristics.
- the cesium isotopes Cs and Cs are available to qualified users from Oak Ridge National Laboratory 2,835,699 Patented May 20, 1958 ice of the United States Atomic Energy Commission as a chloride solution having a very high specific radioactivity, requiring shielded handling, as is well known in this art.
- the final product also requires suitable equipment for safe storage and utilization.
- This mixture was heated to 150 C. with stirring to remove water and alcohol.
- the cooled mixture was then dissolved in a low boiling hydrocarbon diluent, in this case xylene, and made up to ml. volume.
- the yield of activity was greater than 99%, resulting in 100 ml. having 9 me. activity or about 0.1 mc./ml. of product.
- the specific activity of the sulfonate-cesium mixture and the final diluted tracer may be chosen to suit the particular use to which the product may be put. In the usual pipe line operation, about 3 to 12 millicuries of the cesium isotope may be used for each injection, diluted to a convenient quantity to suit the injection equipment.
- Certain commercial sulfonates contain a trace of sodium sulfate, Na SO which precipitates when the product is dissolved in very large quantities of certain hydrocarbon thinners and solvents.
- cesium sulfonate preparations made from these commercial sulfonates no radioactivity was carried down in the precipitate, although it may be deemed advisable to remove the sulfate from the sulfonate before the cesium salt is added. This may be done conveniently by water extraction or by first diluting the sodium sulfonate with a petroleum thinner, followed by separation of the precipitate and evaporation of the excess solvent.
- cesium sulfonate solutions which have been prepared according to this invention may be highly diluted with petroleum or other hydrocarbon solvents without separation of radioactivity. Also, it is substantially unaffected by water, as was evidenced by making up 400 ml. of petroleum thinner containing 1,25 ml. of tracer solution and shaking it successively with 25 ml. of tap water, 25 ml. of NaCl solution containing 0.7 mg./ml. NaCl, and with 25 ml. of CaCl containing 3 mg./ml. of CaCl- No radioactivity was found in any extract.
- the tracer is quite stable for use in pipe lines carrying oil, but in which small amounts of water may unavoidably be present.
- the Cs isotope emits several gamma rays that are of suitable magnitude to penetrate the steel wall of a pipe line and be detected outside of the pipe by suitable single or multiple units of gamma ray detectors.
- Each disintegration yields one 0.60 m. e. v. and one 079 'm; e. v. gamma 'ray, and, in addition, 25% of the disintegrations yield a'f0.57 m. e. v. gamma ray.
- radioactive tracers compared with radioactive tracers .from SblZt, .with 2.7 n1.v ,e, -v. .gamma, '".a somewhat greater quantity. of
- a radioactive tracer consisting essentially of an oil soluble sulfonate of an isotope of cesium selectedfrom the group consisting of Cs" and CS 2.
- A-radioactive tracer consisting essentially of anionsoluble sulfonate ,o'f Csm. i
- Aradioactiv'e tracer consisting essentiallyof .an' oil soluble sulfonateof Cs 4.
- a radioactive tracer consisting essentially of a sulfonate obtained by, reactingran oil soluble sulfonate and an inorganic cesium salt, wherein thecesium is selected prising the steps of reacting an oil soluble sulfonate a radioactive cesium isotope selected fromthegrouprcon- 4 from the group consisting of radioactive isotopes Cs and Cs 5.
- a radioactive tracer consisting essentially of the reaction product of a petroleum sulfonate and an inorganic cesium salt, wherein the cesium is a radioactive isotope selected fromthe-group consisting of Cs and Cs v V V V 6.
- a method of preparing a radioactive tracer comsisting of CS and Cs to produce anoilsoluble radioactive tracer.
- a method of preparing a ,radioactivetracer comprising the steps of reacting sodium sulfonate derived from petroleum and a radioactivecesium isotope selected from the group consisting of Cs and CS to produce an oil soluble radioactive tracer.
Description
RADIOACTIVE TRACERS FOR PIPE LINES Bernard A. Fries, Berkeley, Calif., assignor to California Research Corporation, San Francisco, Calif., a corporation of Delaware No Drawing. Application March 29, 1955 Serial No. 497,800
9 Claims. (Cl. 260-504) This invention relates to liquid radioactive tracers and methods for their preparation, and particularly refers to those prepared from isotopes of cesium that are of specific utility in tracing the flow of liquid hydrocarbons through pipe lines.
In the operation of long pipe lines through which successive batches of liquid hydrocarbon products are passed, it is essential to be able to distinguish the interfaces between ditferent products so that they may be separated at their points of take-oil? or delivery. A suitable method that has been developed consists in the introduction into the interface between successive different products of a small quantity of an oil-soluble liquid carrying a radioisotope that can be detected outside of the pipe line at any point along the length. Usually the isotope is chosen to be a gamma-emitter, and compounds of radioactive antimony and the like have been employed, as described in the Patent No. 2,706,254 of R. C. Mithoff and D. E. Hull.
This invention is particularly directed to improve longlived liquid radioactive tracers, particularly but not necessarily exclusively suited for such pipe line operations, and employing radioisotopes of cesium, namely, Cs having a 2.3 year half-life and emitting gamma radiation in the 0.57-0.79 m. e. v. range, and Cs having a 37 year half-life which does not emit gamma radiation but is in equilibrium with a 2.6 minute Ba daughter emitting 0.66 m. e. v. gamma radiation. A given number of millicuries of the Cs isotope is about twice as specifically effective as the Cs The radioactive tracer composition containing either isotope may be prepared by the procedures which will be described below. The C8137 isotope has the advantage of a longer effective life, which can be of substantial importance in certain tracer applications. The earlier-used antimony isotopes, having a 60-day half-life, required frequent preparation in small quantities, due to their rapid decay, and were accordingly more expensive to prepare and to store.
It is an object of this invention to provide an improved oil-soluble and water-insoluble radioactive liquid tracer composition which is simply prepared and conveniently used, and which has a longer effective useful life than certain of those tracers heretofore available, and which may be prepared at a much lower cost.
Another object is to provide an improved method of preparing a radioactive tracer composition that may be carried out conveniently and with safety to the operator.
Another object is to provide an improved method of purifying a sulfonate component of a radioactive liquid tracer to produce a product having desirable characteristics.
These and other objects and advantages will be further apparent from the following specification, which describes the improved product and an exemplary procedure for producing it.
The cesium isotopes Cs and Cs are available to qualified users from Oak Ridge National Laboratory 2,835,699 Patented May 20, 1958 ice of the United States Atomic Energy Commission as a chloride solution having a very high specific radioactivity, requiring shielded handling, as is well known in this art. The final product also requires suitable equipment for safe storage and utilization.
In this example, an 0.5 ml. (milliliter) aliquot of cesium chloride containing 9 me. (millicuries) of Cs activity and 0.5 mg. cesium in 0.5 N HCl was evaporated to dryness and then redissolved in 0.5 ml. of water to which 2.0 ml. of ethanol was added. To this solution wasadded 15 ml. of sodium sulfonate which had been prepared by sulfonation of a petroleum distillate stock followed by conversion to free sulfonic acid and neutralization with NaOH. It is considered that the radioactive cesium chloride reacts to form cesium sulfonate.
This mixture was heated to 150 C. with stirring to remove water and alcohol. The cooled mixture was then dissolved in a low boiling hydrocarbon diluent, in this case xylene, and made up to ml. volume. The yield of activity was greater than 99%, resulting in 100 ml. having 9 me. activity or about 0.1 mc./ml. of product. The specific activity of the sulfonate-cesium mixture and the final diluted tracer may be chosen to suit the particular use to which the product may be put. In the usual pipe line operation, about 3 to 12 millicuries of the cesium isotope may be used for each injection, diluted to a convenient quantity to suit the injection equipment.
In large-scale preparations, where an appreciable weight of cesium is present, it has been found to be desirable to convert the cesium chloride to the hydroxide, using an appropriate ion-exchange column. The hydroxide may then be directly reacted with sulfonic acid to produce the sulfonate carrying the active isotope in oil-soluble form. The same procedures as just given apply also to preparation of the improved traced from the Cs isotope.
Certain commercial sulfonates contain a trace of sodium sulfate, Na SO which precipitates when the product is dissolved in very large quantities of certain hydrocarbon thinners and solvents. In cesium sulfonate preparations made from these commercial sulfonates, no radioactivity was carried down in the precipitate, although it may be deemed advisable to remove the sulfate from the sulfonate before the cesium salt is added. This may be done conveniently by water extraction or by first diluting the sodium sulfonate with a petroleum thinner, followed by separation of the precipitate and evaporation of the excess solvent.
The radioactive and other properties of the cesium isotope products of this invention are very desirable for certain tracer applications, such as the pipe line oil interface tracer of patent No. 2,706,254 discussed above. For example, cesium sulfonate solutions which have been prepared according to this invention may be highly diluted with petroleum or other hydrocarbon solvents without separation of radioactivity. Also, it is substantially unaffected by water, as was evidenced by making up 400 ml. of petroleum thinner containing 1,25 ml. of tracer solution and shaking it successively with 25 ml. of tap water, 25 ml. of NaCl solution containing 0.7 mg./ml. NaCl, and with 25 ml. of CaCl containing 3 mg./ml. of CaCl- No radioactivity was found in any extract. Hence, the tracer is quite stable for use in pipe lines carrying oil, but in which small amounts of water may unavoidably be present.
As stated above, the Cs isotope emits several gamma rays that are of suitable magnitude to penetrate the steel wall of a pipe line and be detected outside of the pipe by suitable single or multiple units of gamma ray detectors. Each disintegration yields one 0.60 m. e. v. and one 079 'm; e. v. gamma 'ray, and, in addition, 25% of the disintegrations yield a'f0.57 m. e. v. gamma ray. As compared with radioactive tracers .from SblZt, .with 2.7 n1.v ,e, -v. .gamma, '".a somewhat greater quantity. of
the cesiumisotope would be required, but :wouldstill,
economical as compared .to. Present practices in this :art.
I claim:
1. A radioactive tracer consisting essentially of an oil soluble sulfonate of an isotope of cesium selectedfrom the group consisting of Cs" and CS 2. A-radioactive tracer .consisting essentially of anionsoluble sulfonate ,o'f Csm. i
3. Aradioactiv'e tracer consisting essentiallyof .an' oil soluble sulfonateof Cs 4. A radioactive tracer consisting essentially of a sulfonate obtained by, reactingran oil soluble sulfonate and an inorganic cesium salt, wherein thecesium is selected prising the steps of reacting an oil soluble sulfonate a radioactive cesium isotope selected fromthegrouprcon- 4 from the group consisting of radioactive isotopes Cs and Cs 5. A radioactive tracer consisting essentially of the reaction product of a petroleum sulfonate and an inorganic cesium salt, wherein the cesium is a radioactive isotope selected fromthe-group consisting of Cs and Cs v V V V 6. A method of preparing a radioactive tracer comsisting of CS and Cs to produce anoilsoluble radioactive tracer. g,
7. A method of preparing a ,radioactivetracer comprising the steps of reacting sodium sulfonate derived from petroleum and a radioactivecesium isotope selected from the group consisting of Cs and CS to produce an oil soluble radioactive tracer.
8. Oil soluble Cs sulfonate.
9. Oil soluble C8137 sulfonate.
References Cited in the file of this patent UNITED STATES PATENTS Fischer et al Feb. 26, 1929 2,706,254 Mithoif et. a1 Apr. ,12, 19 55
Claims (1)
1. A RADIOACTIVE TRACER CONSISTING ESSENTIALLY OF AN OIL SOLUBLE SULFONATE OF AN ISOTOPE OF CESIUM SELECTED FROM THE GROUP CONSISTING OF CS134N AND CS137.
Publications (1)
| Publication Number | Publication Date |
|---|---|
| US2835699A true US2835699A (en) | 1958-05-20 |
Family
ID=3447054
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| US2835699D Expired - Lifetime US2835699A (en) | Radioactive tracers for pipe lines |
Country Status (1)
| Country | Link |
|---|---|
| US (1) | US2835699A (en) |
Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US2936371A (en) * | 1956-11-05 | 1960-05-10 | Sun Oil Co | Measuring velocity of transported material |
| US3014054A (en) * | 1959-08-19 | 1961-12-19 | California Research Corp | Radioactive tracers |
| US3130314A (en) * | 1959-11-23 | 1964-04-21 | Exxon Research Engineering Co | Method of using radioactive tracers |
| US3140262A (en) * | 1955-12-05 | 1964-07-07 | Diversey Corp | Contamination detection compositions |
| US3230261A (en) * | 1966-01-18 | Aromatic hydrogen | ||
| US3340202A (en) * | 1965-06-23 | 1967-09-05 | Commissariat Energie Atomique | Sintered pollucite radioactive source and method of production |
| US3489218A (en) * | 1966-08-22 | 1970-01-13 | Dow Chemical Co | Method of killing organisms by use of radioactive materials |
| US3766388A (en) * | 1971-06-04 | 1973-10-16 | Gen Nuclear Inc | Radioactive tracer method and apparatus for boreholes |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US1703838A (en) * | 1929-02-26 | And warren t | ||
| US2058744A (en) * | 1934-01-27 | 1936-10-27 | Migiel J Uline | Machine for squaring the ends of cakes of ice |
| US2706254A (en) * | 1951-07-12 | 1955-04-12 | California Research Corp | Operation of pipelines |
-
0
- US US2835699D patent/US2835699A/en not_active Expired - Lifetime
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US1703838A (en) * | 1929-02-26 | And warren t | ||
| US2058744A (en) * | 1934-01-27 | 1936-10-27 | Migiel J Uline | Machine for squaring the ends of cakes of ice |
| US2706254A (en) * | 1951-07-12 | 1955-04-12 | California Research Corp | Operation of pipelines |
Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3230261A (en) * | 1966-01-18 | Aromatic hydrogen | ||
| US3140262A (en) * | 1955-12-05 | 1964-07-07 | Diversey Corp | Contamination detection compositions |
| US2936371A (en) * | 1956-11-05 | 1960-05-10 | Sun Oil Co | Measuring velocity of transported material |
| US3014054A (en) * | 1959-08-19 | 1961-12-19 | California Research Corp | Radioactive tracers |
| US3130314A (en) * | 1959-11-23 | 1964-04-21 | Exxon Research Engineering Co | Method of using radioactive tracers |
| US3340202A (en) * | 1965-06-23 | 1967-09-05 | Commissariat Energie Atomique | Sintered pollucite radioactive source and method of production |
| US3489218A (en) * | 1966-08-22 | 1970-01-13 | Dow Chemical Co | Method of killing organisms by use of radioactive materials |
| US3766388A (en) * | 1971-06-04 | 1973-10-16 | Gen Nuclear Inc | Radioactive tracer method and apparatus for boreholes |
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