Radioactive decontamination and translocation method

Cleaning and liquid contact with solids – Processes – Including regeneration – purification – recovery or separation...

Reexamination Certificate

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C134S002000, C134S003000, C134S026000, C134S028000, C134S036000, C134S041000, C134S042000, C134S022190, C510S110000, C376S308000, C376S309000, C376S310000, C423S002000, C423S003000, C423S020000, C588S001000, C588S020000, C210S682000, C210S688000, C976SDIG003, C976SDIG003

Reexamination Certificate

active

06605158

ABSTRACT:

BACKGROUND OF THE INVENTION
The present invention relates generally to a method for decontamination of surfaces. More particularly, the present invention relates to using an aqueous solution having particular compositions to remove radioactive contaminants from a given area, location or surface.
Contamination of various areas or surfaces from radioactive or other unwanted materials is a common problem. The contamination of an area or surface may occur as a result of contact with a radioactive isotope during transport, storage, use in a nuclear reactor, mining operations, or a variety of other industrial or military processes. In recent years, methods have been explored to reduce or remove such contaminants from various areas or surfaces and equipment so that such items or areas may be put back into use and the contaminants be disposed of safely. These methods have met with varying success and often present trade-offs between decontamination of the surface or area and the toxicity of the waste product containing the radioactive contaminant.
One method of removing radioactive materials is to physically wash the contaminated area or surface with water and an optional surface-active agent. However, such methods are generally limited to physical separation of contaminants that are not physically or chemically adhered to surfaces or areas. Thus, this method does not work well where the contaminants are chemically bound or physically adhered to a solid surface or structure.
For example, a number of methods have been developed to remove radioactive contaminated scale or rust deposits from metal surfaces. The radioactive substances are removed in a solution that is transported at safe levels for disposal. However the concentrated radioactivity found in scale or rust adhering to surfaces presents increased danger and cost in removal and disposal. Depending on the type of scale or rust deposit either acidic or basic removal treatments may be appropriate. U.S. Pat. No. 5,200,117, 5,049,297 and 5,824,159 illustrate typical approaches to removing radioactive substances in these situations.
Another method for removing contaminants from surfaces or areas, which are not necessarily limited to deposited scales, is known generally as acid leaching. In acid leaching methods, a strong acid is used to dissolve radioactive contaminants from the surface into solution. The resulting solution is removed and disposed of leaving a clean, or at least a reduced amount of radioactive contaminants, on the surface. Such acid leaching processes may or may not use chelating agents.
Chelating agents have been the subject of much research in this area and include ligand or binding agents such as oxalate, citrate, gluconate, picolinate, EDTA, hydrazines with carboxylic acids, and hydroxamic acids. Acidic and basic solutions containing a chelating agent are used to dissolve and bind contaminants depending on the characteristics of the surface and the contaminants. When used to remove radioactive substances from contaminated areas, the chelating agent is thought to have the effect of stabilizing certain dissolved radioactive contaminants to keep them in solution. Several of these methods use concentrated carbonate solutions to recover uranium, thorium, radium, technetium, and other actinides.
With several of these methods, a separate ion-exchange process is used to purify the resulting solution to make disposal of the radioactive contaminants easier.
In addition to these challenges, other considerations include providing a decontaminating agent and method which is not excessively corrosive and is easy to prepare and use. Further, the solution containing removed contaminants should preferably be easily disposed of in compliance with state and federal regulations. It would therefore be a significant advancement and contribution to the art to provide a method which is a simple, economic, and an effective way of removing substantially all of the radioactive contaminants from various surfaces or areas.
SUMMARY OF THE INVENTION
While many methods for removing radioactive or other unwanted contaminants have been developed there remains the need for improved decontamination methods which speed up the decontamination process and remove substantially all of the radioactive contaminants. The present invention relates to the removal of radioactive contaminants from a surface or area using an aqueous solution which includes a wetting agent and an active agent. The active agent may be a complex substituted keto-amine, linear alcohol alkoxylate, ethoxylated alkyl amine, or mixtures of these. The aqueous solution is applied to a radioactively contaminated surface and retained on the surface for a period of time sufficient to allow at least a portion of the radioactive contaminants to migrate into the aqueous solution. The contaminant rich aqueous solution is then removed from the surface for further treatment or disposal.
In one aspect of the present invention the active agent is a complex substituted keto-amine having the molecular formula C
33
H
45
NO
2
.ClH.
In a more detailed aspect of the present invention the wetting agent is a lower alcohol such as methanol, ethanol, propanol, isopropanol, butanol, propargyl alcohol, tertiary butyl alcohol, pentanol, and mixtures of these alcohols.
In another aspect of the present invention, the aqueous solution includes a concentrated acid such as hydrochloric acid, hydrofluoric acid, sulfuric acid, phosphoric acid, sulfurous acid, bromic acid, iodic acid, nitric acid, perchloric acid, oxalic acid, aqua regia, citric acid, sulfamic acid, glycolic acid, ascorbic acid, and mixtures thereof. In a more detailed aspect, the resulting acidic solution using one or more of the above acids has a pH of less than 1.5.
In accordance with yet another more detailed aspect of the present invention, the method is used to remove radioactive contaminants, and particularly those found in the actinide and lanthanide series such as thorium, uranium, and plutonium. Exemplary of radioactive contaminants, some of which are in the actinide and lanthanide series, are Actinium-227, Americium-241, Americium-243, Antimony-124, Antimony-125, Barium-133, Beryllium-7, Bismuth-207, Cadmium-109, Calcium-45, Carbon-14, Cerium-139, Cerium-141, Cerium-144, Cesium-134, Cesium-135, Cesium-137, Chromium-51, Cobalt-56, Cobalt-57, Cobalt-58, Cobalt-60, Copper-67, Curium-242, Curium-243, Curium-244, Curium-247, Europium-152, Europium-154, Europium-155, Gadolinium-153, Germanium-68, Gold-195, Hafnium-181, Hydrogen-3(Tritium), Iodine-125, Iodine-126, Iodine-129, Iodine-131, Iodine-133, Iridium-192, Iron-55, Iron-59, Lead-210, Manganese-54, Mercury-203, Neptunium-237, Nickel-59, Nickel-63, Niobium-94, Plutonium-236, Plutonium-238, Plutonium-239, Plutonium-240, Plutonium-241, Plutonium-242, Plutonium-243, Plutonium-244, Polonium-210, Potassium-40, Promethium-147, Protactinium-231, Radium-223, Radium-224, Radium-226, Radium-228, Ruthenium-106, Samarium-151, Scandium-46, Selenium-75, Silver-108m, Silver-110m, Sodium-22, Strontium-85, Strontium-89, Strontium-90, Sulfur-35, Tantalum-182, Technetium-99, Thallium-204, Thorium-natural, Thorium-228, Thorium-230, Thorium-232, Tin-113, Uranium-232, Uranium-233, Uranium-234, Uranium-235, Uranium-236, Uranium-238, Uranium-natural, Uranium-depleted, Yttrium-88, Yttrium-91, Zinc-65, Zirconium-95 and associated decay products of these contaminants.
In accordance with another aspect of the present invention, the method is applied to a solid surface or area as defined above which comprises metal, plastic, glass, concrete, wood, fiberglass, soil, natural or synthetic fabrics, or any other material.
In general, the method comprises applying the aqueous solution, as hereinafter defined, in such a manner as to contact the radioactive contaminant and remove it from the surface or area to which it is associated into the solution. Such application techniques may be by spraying, wiping, soaking, immersing and the like. Once applied to a surface it is important that the solution be removed before the solution d

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