JP2022023989A - Method of converting elements such as calcium, copper, magnesium, and cesium into more useful elements and method of detoxifying radioactive substances by applying this element conversion technology - Google Patents

Abstract

PROBLEM TO BE SOLVED: To realize conversion of elements and detoxification of radioactive substances by applying combination of nano-microbubbles and high-frequency vibration agitation.

SOLUTION: A method of the present invention comprises: providing a high-frequency vibration agitator comprising a processing tank 1, a high-frequency vibration motor 3 fixed to an upper table of the processing tank 1, two vibrating rods 4 extending downward from the processing tank 1 connected to the table, and multi-stage vibration blades 5 arranged in a lower part of the vibrating rods 4, whose surface is plated with palladium or platinum that serves as a catalyst for element conversion; and controlling the high-frequency vibration motor 3 by an inverter 6 to vibrate the multi-stage vibration blades 5 at a frequency of 100 to 170 Hz in aqueous solution 2 containing element to be converted in the treatment tank 1 so as to convert the element in the aqueous solution 2 into another element. When heavy water is added to the solution to be treated, conversion efficiency is improved. When tritiated water of an appropriate concentration is added instead of the heavy water, elemental conversion can be achieved in a short time, and at the same time, the tritiated water can be effectively used to attenuate or detoxify its radioactivity.

SELECTED DRAWING: Figure 1

COPYRIGHT: (C)2022,JPO&INPIT

Description

The present invention shares the energy of high-frequency vibration agitation and the burst energy of nano-micro bubbles generated by electrolysis of water with the vibration blades of the high-frequency vibration agitator as both poles, and further, the surface of the vibration blades is plated with palladium. The present invention relates to a treatment method for enhancing the catalytic effect to convert one element into another, and a treatment method for detoxifying radioactive substances such as radioactive cesium 137 and 134.

Rare elements such as rare earths and rare metals have become indispensable and most important elements in the advanced technology fields of the electronic industry and the automobile industry these days, but these elements are present only in a small amount in a specific place. Therefore, we are working on technological development at the national level regarding the artificial manufacturing method of these rare elements, but although it has been realized at the laboratory level, practical technology has not been realized, and it is extremely difficult. It is the actual situation.

In addition, when "salt" is collected from seawater, a huge amount of "magnesium chloride" as "waste" is produced as a by-product of several million tons per year, and its treatment measures are extremely difficult. is the current situation.

Furthermore, even in "Fukushima", which is suffering from soil pollution and contaminated water due to radioactive substances, there is only a technology to reduce the volume of radioactive substances by simply using zeolite or special furnace materials, which is a problem of Fukushima. Not only that, it is a difficult problem that is urgently required to be solved, which is related to national or human survival, but there is still no solid technology and the birth of the innovative technology is required as soon as possible.

The inventor previously electrolyzed water with special vibration stirring to generate nano-microbubbles (fine bubbles of oxygen and hydrogen gas), which burst to generate powerful energy. It has been confirmed that it is generated (see, for example, Patent Document 1-3). Patent Documents 1 and 2 describe that nano-microbubbles are generated by vibrating stirring, and Patent Document 3 applies the nano-microbubbles to generate flammable gas from carbon dioxide gas and water. The method of generating is described.

Japanese Patent No. 2852878 Japanese Patent No. 4269318 PCT / JP2014 / 066551

A patent was filed on September 11, 2013 regarding the conversion method of elements and the detoxification of radioactive substances by applying it in combination with the above nano-microbubbles and high-frequency vibration stirring, and satisfactory conversion efficiency was obtained. However, the target elements to be converted were limited to calcium and cesium. Therefore, it is an object of the present invention to further develop a method combining nano-microbubbles and high-frequency vibration stirring, and to widely apply element conversion to the above-mentioned magnesium chloride, contaminated water caused by radioactive substances, etc., and to improve the conversion efficiency. It was done.

Rare elements such as rare metals and rare earths can be extracted by converting them from common elements such as calcium, magnesium, and iron, or radioactive substances such as cesium can be converted into elements such as barium, silver, gold, and platinum. In order to reduce the radioactivity to a permissible range that is harmless to the human body, the surface of the multi-stage vibration blades of the vibration stirrer is plated with palladium or platinum to a thickness of 2-5 μm, and it is made into an aqueous solution to be converted into elements. An elemental conversion method that achieves elemental conversion within a few hours to a few days and solves the problem by vibrating and stirring at 100 Hz to 170 Hz under the condition that heavy water is added so as to have a concentration of 0.1 to 5%. Alternatively, a method of adding a certain amount of dilute tritium (0.1 to 5 μSv) instead of “heavy water” used as a catalyst for elemental conversion to achieve elemental conversion faster than heavy water.

More specifically, it is solved by any of the following configurations (1) to (5), (7) and (8).

(1) A processing tank, a high-frequency vibration motor fixed to the upper table of the processing tank, two vibrating rods connected to the table and extending downward to the processing tank, and attached to the lower part of the vibrating rod. A high-frequency vibration agitator including a multi-stage vibration blade whose surface is plated with palladium or platinum as a catalyst for element conversion is provided, and the high-frequency vibration motor is controlled by an inverter in the processing tank. A method characterized by vibrating the multi-stage vibration vane at a frequency of 100 Hz to 170 Hz in an aqueous solution containing an element to be converted to convert the element in the aqueous solution into another element.

(2) The method according to (1) above, wherein 0.1% to 5% of heavy water is added to the aqueous solution.

(3) It is said that the element conversion is achieved in a shorter time than when 5% to 50% of tritiated water of 0.5μ to 5μ Sv is added to the aqueous solution and heavy water is added, and at the same time, it is said to be the cause of radioactive contamination. The method according to (1) above, wherein the tritiated water is effectively used, and at the same time, the radioactivity of the tritiated water is attenuated or detoxified to a concentration of 1/16 in 25 hours.

(4) The multi-stage vibration vane has both an anode and a cathode electrodes, and a current of 0.5 to 4 A / dm2 is passed through the electrodes to generate nano / microbubbles to improve element conversion efficiency. The method according to (1) or (2) above.

(5) The method according to any one of (1) to (3) above, wherein the aqueous solution is treated at room temperature (15 to 30 ° C.).

(6) The method according to any one of (1) to (3) above, wherein the aqueous solution during the element conversion process has no harmful effect due to a temperature rise.

(7) The treatment tank is a closed type or an open type, and when treating a gas body generated during treatment, pure water or 3% water for treating the gas generated during element conversion via a pipe. The method according to (1) above, wherein a bubbling tank holding an aqueous potassium oxide solution is connected.

(8) The method according to (7) above, wherein the material of the treatment tank is made of resin or a metal containing stainless steel.

According to the present invention, it has become possible to detoxify radioactive elements at low cost by a simple technique, and it is possible to convert common elements such as calcium into precious cobalt and nickel, and copper into gold and silver. As a result, it has become possible to make a great contribution to the protection of the global environment and resources.

It is sectional drawing of the electrode combined type high frequency vibration agitator, A is a front sectional view, B is a side sectional view. Cross section of bubbling tank Enlarged view of the multi-stage vibration blade portion of the electrode-combined high-frequency vibration agitator shown in FIG. 1.

The system used for element conversion and detoxification of radioactive elements consists of an electrode-combined high-frequency vibration agitator shown in FIG. 1 and a bubbling tank (cushion tank) shown in FIG. The electrode-combined high-frequency vibration agitator is provided with a processing tank 1 and an aqueous solution 2 containing an element to be converted is charged. A high-frequency vibration motor 3 is fixed to a table on the upper side of the processing tank 1, two vibration rods 4 are connected to the table, and the vibration rods 4 extend downward into the processing tank 1. A multi-stage vibration vane 5 is attached to the lower portion of the vibration rod 4. By controlling the high-frequency vibration motor 3 by using the inverter 6, the multi-stage vibration blade 5 can be set to vibrate at a frequency of 100 to 170 Hz in the liquid of the processing tank 1.

As shown in the enlarged view of the multi-stage vibrating blade portion in FIG. 3, the multi-stage vibrating blade 5 is attached to two vibrating rods 4, but the first vibrating blade is physically and electrically with the right vibrating rod. Although physically connected to the left vibrating rod, it is electrically insulated by the insulator 7. The second vibrating vane is physically connected to the first right vibrating rod, but is electrically insulated by the insulator 7 and physically and electrically connected to the left vibrating rod. There is. In this way, the left and right vibrating rods are in an electrically insulated state by electrically connecting the vibrating blades and alternately repeating insulation on the left and right vibrating rods. Therefore, a DC voltage application circuit, that is, an electrolysis circuit can be formed by connecting a DC power supply to the left and right vibrating rods via a rectifier 8 and alternately using a plurality of vibrating blades 5 as an anode and a cathode. The size of one vibrating blade 5 is 55 mmW × 100 mL × 0.5 mmt, and 5 blades were used as shown in FIG. In order to enhance the catalytic effect during element conversion, the surface of the vibrating blade 5 was plated with palladium to a thickness of 2-5 μm. Platinum may be used instead of palladium. The catalytic effect of palladium is clear from Tables 1 and 2 that summarize the results of Examples 1 and 2 described later. A comparison of the results with and without palladium plating will be specifically described in the Examples.

With the above configuration, the processing tank 1 can be operated to perform electrolysis only with high-frequency vibration or with high-frequency vibration flow at the same time. The material of the treatment tank may be made of resin or a metal such as stainless steel, and may be arbitrarily selected according to the conditions of use.

When performing electrolysis, a direct current voltage (DC12V) is applied to the two vibrating rods 4 via the rectifier 8. The current density at that time is set to 0.5 to 4 A / dm2.

FIG. 2 is a cross-sectional view showing a bubbling tank. The bubbling tank is provided so that oxyhydrogen gas (OHMASA-GAS) generated by electrolysis in the vibration stirrer is not released into the atmosphere with radioactive elements, etc., and is pure water or pure water from the top of the bubbling tank. It is connected to the top of the processing tank 1 by a pipe so that the gas generated in the processing tank 1 of the high-frequency vibration stirring device is blown into the 3% potassium hydroxide aqueous solution.

Using this system, expecting the effect of the powerful burst energy of nano-microbubbles generated during the electrolysis of water, the procedure for performing element conversion using high-frequency stirring and electrolysis together is as follows. It's a street.
1) The aqueous solution 2 containing the element to be treated is charged into the treatment tank 1 of the electrode-combined high-frequency agitator. In addition, in order to efficiently achieve elemental conversion in a short time, it is preferable to add 0.1 to 5% heavy water to the aqueous solution 2. In addition, when 5 to 50% of tritiated water of 0.5 to 5 μSv is added instead of heavy water, elemental conversion can be achieved in a shorter time, and at the same time, tritiated water, which is said to be one of the main causes of radioactive contamination. Can be used effectively. The effect of tritiated water will be described later in Examples.
2) The frequency of the high frequency vibration motor 3 is set by the inverter 6 and energized.
3) The electrolytic voltage and current value are set by the electrolytic rectifier 8 (this starts the element conversion process).
4) Perform elemental conversion processing for a predetermined time.
5) Turn off the power of the electrolytic rectifier 8.
6) Turn off the power of the high frequency vibration motor 3.
7) After stirring the aqueous solution 2 in the treatment tank 1 for 3 minutes to homogenize, the treatment liquid is collected and the elemental amount is measured. For the element measurement, copper, nickel, cobalt, titanium, silver and gold were quantified by an ICP mass analyzer (HP-4500) manufactured by Yokogawa Analytical Systems Co., Ltd. In addition, calcium, magnesium, iron, and zinc were quantified by an ICP emission spectrometer (iCAP6300) manufactured by Thermo Fisher Scientific Co., Ltd.

An embodiment in which the conditions are changed using the above system will be described.

The result of putting a 0.5% aqueous solution of calcium chloride in the treatment tank 1, adding 5 g / L (about 0.5%) of heavy water, and vibrating the vibrating blade 5 at 170 Hz with a high-frequency stirrer for 3 hours. Is shown in Table 1. In addition, in order to confirm the catalytic effect of palladium, a conversion treatment was also performed using a stirring blade plated with palladium on the surface and a stirring blade not plated. The temperature of the aqueous solution was 18.6 ° C. before the treatment and 18.5 ° C. after the treatment regardless of the presence or absence of palladium plating, and there was no significant change.

As a result, calcium with a concentration of 1400 mg / L is a more beneficial element when there is no palladium plating on the surface of the stirring blade, iron (0.5 mg / L), copper (11 mg / L), nickel (9 mg). It can be seen that it is converted to / L), cobalt (7 mg / L), and titanium (12 mg / L), and the concentration is reduced to 1050 mg / L. When the surface of the stirring blade is plated with palladium, it is converted into iron (2 mg / L), copper (31 mg / L), nickel (26 mg / L), cobalt (14 mg / L), and titanium (23 mg / L). It can be seen that the concentration has decreased to 890 mg / L. From this result, it can be seen that the catalytic effect of palladium is clear, and although it depends on the element, the conversion efficiency of the element is increased by about 2 to 3 times depending on the element.

Table 2 shows the results of treatment by putting a 1% aqueous solution of copper chloride in the treatment tank 1, adding 5 g / L (about 0.5%) of heavy water, and vibrating the vibrating blade 5 at 170 Hz with a high-frequency stirrer for 3 hours. Shown in. Similar to Example 1, in order to confirm the catalytic effect of palladium, a conversion treatment using a stirring blade plated with palladium on the surface and a stirring blade not plated was also performed. The temperature of the aqueous solution was 18.2 ° C. before the treatment and 18.4 ° C. after the treatment, and there was no significant change.

As a result, copper at a concentration of 4200 mg / L is the more beneficial elements silver (11 mg / L), gold (8 mg / L) and nickel (12 mg / L) when the surface of the stirring blade is not plated with palladium. ), It can be seen that the concentration of copper is reduced to 2800 mg / L after being converted to zinc (16 mg / L).

When the surface of the stirring blade is plated with palladium, it is converted into silver (34 mg / L), gold (26 mg / L), nickel (27 mg / L), and zinc (31 mg / L), and the concentration of copper is 1900 mg / L. It can be seen that it has decreased to. From this result, it can be seen that the catalytic effect of palladium is clear, and although it depends on the element, the conversion efficiency of the element is increased by about 2 to 3 times depending on the element.

A 0.5% magnesium chloride aqueous solution was placed in the treatment tank 1, heavy water was added at 5 g / L (about 0.5%), and a vibration blade 5 having a palladium-plated surface was provided at 170 Hz by a high-frequency stirrer. Table 3 shows the results of vibrating and processing for 3 hours. The temperature of the aqueous solution was 18.4 ° C before the treatment and 18.5 ° C after the treatment, showing no significant change.

As a result, magnesium having a concentration of 1760 mg / L was converted to gold (14 mg / L), silver (32 mg / L), and copper (48 mg / L), and the magnesium concentration was reduced to 1020 mg / L. Recognize.

Table 4 shows the results of treatment by putting a 1% aqueous solution of cesium chloride in the treatment tank 1, adding 5 g / L (about 0.5%) of heavy water, and vibrating the vibration blade 5 at 170 Hz with a high-frequency stirrer for 3 hours. Shown in. Table 4 also shows the results of adding 5 g / L of tritiated water of 0.5 μSv instead of heavy water. The temperature of the aqueous solution was 19.8 ° C. before the treatment, 20.0 ° C. for heavy water and 20.2 ° C. for tritiated water after the treatment, showing no significant change.

As a result, when heavy water was added, cesium having a concentration of 6700 mg / L was barium (48 mg / L), tungsten (22 mg / L), platinum (24 mg / L), gold (18 mg / L), and silver (8 mg). It can be seen that the concentration of cesium is reduced to 4800 mg / L by being converted to / L), copper (4 mg / L) zinc (16 mg / L), nickel (5 mg / L), and iron (18 mg / L). ..

When tritiated water was added, cesium having a concentration of 6700 mg / L was barium (58 mg / L), tungsten (40 mg / L), platinum (51 mg / L), gold (42 mg / L), and silver (19 mg). / L), copper (10 mg / L), zinc (25 mg / L), nickel (22 mg / L), iron (33 mg / L), and the concentration of cesium was reduced to 3880 mg / L. Recognize. Compared with radioactive and heavy water, tritiated water has a higher concentration in all elements, indicating that the elements are converted efficiently.

In addition, the radioactivity of tritium, which was 0.5 μsievert before treatment, becomes 0.05 μsievert or less after treatment for 3 hours, and the vibration and flow of the solution according to the present invention significantly attenuates the radioactivity of tritium. It turns out that it is extremely effective in detoxifying.

Tritiated water was placed in the treatment tank 1 and the multi-stage vibrating blade 5 having a surface plated with palladium of 3 to 5 μm was vibrated at 170 Hz with a high-frequency stirrer to vibrate the tritiated water treated for up to 25 hours every 5 hours. The measurement results of are shown in Table 5. The radiation concentration was measured using a survey meter [SM5D] manufactured by Sensor Technique & Electronic Bokaw (Germany).

As is clear from the results shown in Table 5, the tritium concentration before treatment was 0.8 μsv, but after 10 hours of treatment, the concentration was reduced to 0.35 μsv, which was less than half, and after 20 hours of treatment, it was 0.084 μsv, which was almost the same. The concentration decreased to 1/10, and the concentration decreased to 1/16 at 0.051 μsv in 25 hours.

During the treatment of tritiated water, the treatment tank 1 was filled with a "gas body" considered to be "helium", and the entire liquid was in a cloudy state with "bubbles". This cloudiness is considered to be due to the fact that tritium comes into contact with the palladium-catalyzed vibrating blade 10,000 times or more per minute and is given "vibration energy" 10,000 times or more per minute.

However, when the vibration stirring was stopped, the "gas body" that had made the entire liquid cloudy emerged, and the liquid became "transparent" after a few minutes. Immediately after resuming the stirring vibration, it became cloudy due to the "gas body".

As is clear from the above examples, by applying the element conversion technique according to the present invention to an aqueous solution of calcium, an aqueous solution of copper or an aqueous solution of magnesium, a considerably large amount of precious rare metals and precious metals such as gold and silver can be produced. Demonstrated.

What is noteworthy here is the fact that even if the processing time is extremely short (3 hours), a large amount of new elements are produced from the original common elements by the element conversion technology.

By plating the surface of the vibrating blade with palladium, which plays an important role as a catalyst for element conversion, the vibration and flow (170 Hz) of the vibrating blade causes the palladium catalyst to come into contact with the element about 10,000 times per minute. I think it is due to the fact that it is done in an unimaginable number of times.

Of course, it is also an important factor that heavy water, which is another catalyst important for element conversion, fully fulfills its function by vigorous vibration and flow of about 10,000 times per minute, similar to the catalytic reaction of palladium. Is.

However, if the vibration blades plated with palladium are subjected to vibration of about 10,000 times per minute, the effect is very small, but the "fluid flow at the same time as the vibration" that the inventor has already invented is generated. Of course, that is the most important factor.

It is an epoch-making invention that elemental conversion can be performed by simply agitating the inside of a tank containing an aqueous solution containing an element to be converted into elements at a high frequency and giving vibrational flow to the aqueous solution. It opens the way for easy elemental conversion of one type of element into another.

Achieving the desired elemental conversion at room temperature, safely and easily simply by installing and operating a high-frequency agitator corresponding to the capacity of the processing tank will be necessary in order to create the required amount of elements by elemental conversion in the future. , Can make a big contribution.

In addition, as shown in the examples, the fact that cesium was converted to another element such as barium and platinum in a short time has made it possible to realize an urgently safe society in today's difficult situation in the treatment of radioactive contaminants. It will be a great technological innovation that will be possible.

As can be understood from the treatment results of tritium water, a "high frequency vibration stirrer" with vibration blades plated with a palladium catalyst for "tritium", which is extremely difficult all over the world, is vibrated and stirred at 170 Hz for about 25 hours. We believe that the fact that we obtained epoch-making data to reduce the tritium concentration to about 1/16 is a technical achievement that can immediately dispel the "tritium fear" from the world including Fukushima.

1 Treatment tank 2 Aqueous solution (containing elements) 3 High frequency vibration motor 4 Vibration rod 5 Multi-stage vibration blade 6 Inverter 7 Insulator 8 Rectifier

Claims (7)

Processing tank,
A high-frequency vibration motor fixed to the upper platform of the processing tank,
Two vibrating rods connected to the table and extending downward from the processing tank, and a multi-stage vibrating blade whose surface is plated with palladium or platinum as a catalyst for element conversion attached to the lower part of the vibrating rod. Equipped with a high frequency vibration stirrer configured to include
The high-frequency vibration motor is controlled by an inverter, and in an aqueous solution containing an element to be converted in the processing tank, the multi-stage vibration blade is vibrated at a frequency of 100 Hz to 170 Hz to separate the element in the aqueous solution. A method characterized by converting to an element. The method according to claim 1, wherein 0.1% to 5% of heavy water is added to the aqueous solution. Tritiated water, which is said to be the cause of radioactive contamination at the same time as achieving element conversion in a shorter time than when adding 5% to 50% of tritiated water of 0.5μ to 5μ Sv to the aqueous solution and adding heavy water. The method according to claim 1, wherein the tritiated water is attenuated or detoxified to a concentration of 1/16 in 25 hours at the same time as effectively utilizing the above. The claim is characterized in that the multi-stage vibration vane has both an anode and a cathode electrodes, and a current of 0.5 to 4 A / dm2 is passed through the electrodes to generate nano-microbubbles to improve element conversion efficiency. 1 or the method according to claim 2. The method according to any one of claims 1 to 3, wherein the aqueous solution is treated at room temperature (15 to 30 ° C.). The treatment tank is a closed type or an open type, and when treating a gas body generated during the treatment, pure water or a 3% potassium hydroxide aqueous solution for treating the gas generated during element conversion via a pipe is used. The method according to claim 1, wherein the bubbling tanks holding the above-mentioned gas are connected to each other. The method according to claim 6, wherein the material of the treatment tank is made of resin or a metal containing stainless steel.

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