CN102303039B - Method for removing 226Ra in uranium tail sand and radioactive contaminated soil by plants - Google Patents

Method for removing 226Ra in uranium tail sand and radioactive contaminated soil by plants Download PDF

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CN102303039B
CN102303039B CN 201110280664 CN201110280664A CN102303039B CN 102303039 B CN102303039 B CN 102303039B CN 201110280664 CN201110280664 CN 201110280664 CN 201110280664 A CN201110280664 A CN 201110280664A CN 102303039 B CN102303039 B CN 102303039B
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uranium
plant
uranium tailings
pollution soil
radioactive pollution
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CN102303039A (en
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丁德馨
李广悦
胡南
王永东
李海涛
殷杰
马少维
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Nanhua University
University of South China
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Abstract

The invention relates to a method for removing 226Ra in uranium tail sand and radioactive contaminated soil by plants. The method mainly uses an accumulation plant of the 226Ra, namely a Pieris multifida, to accumulate the 226Ra in the uranium tail sand and the radioactive contaminated soil and simultaneously convey the 226Ra to the overground part of the plant, thereby removing the 226Ra in the uranium tail sand and the radioactive contaminated soil. The method has the following specific steps of: (1) spore germination cultivation; (2) potting seedling; (3) planting the plant in the uranium tail sand or the radioactive contaminated soil; (4) harvesting the overground part of the plant and executing centralized treatment on the harvested plant. The method has the advantages of being convenient to obtain materials, low in cost, high in remediation efficiency, easy to management, simple and convenient in steps, less in environmental risk, and the like, thereby being suitable for removing the 226Ra in the uranium tail sand and the radioactive contaminated soil in uranium mines, uranium water treatment factories, tailings pools and the like.

Description

A kind of utilization in plant removal uranium tailings and the radioactive pollution soil 226The method of Ra
Technical field
The present invention relates to a kind of alpha-contamination phytoremediation field, a kind of specifically through plantation 226The enriching plant of Ra-curb limit grass (Pieris multifida) is removed in uranium tailings and the radioactive pollution soil 226The technology of Ra.
Background technology
According to China's nuclear industry " 30 years Radiological Environment Quality " report; The radionuclide that uranium ore smelting system produces; Collective dose to public's irradiation on every side accounts for 91.5% of total collective of nuclear fuel system dosage, and its primary pollution source is the barren rock that digging is come out in the uranium mining process, the barren rock that ore dressing is eliminated; And the waste residue of the generation in preliminary treatment and the wet metallurgy course, mine tailing, receive its contaminated soil in addition.
For dump leaching and uranium hydrometallurgy, the rate of recovery of uranium is generally 80%-95%.Therefore, initial uranium in the uranium ore ( 238The half-life of U is 4.49 * 10 9A) 5%-20% of content is most 230Th (half-life 83000a), 226Ra (half-life 1600a) still is present in the uranium tailings, accounts for the 70-80% of ore gross activity.Owing to contain in the uranium ore uranium remaining after the whole decay daughters of uranium series, the hydrometallurgy and 99% above in the uranium tailings 230Th reaches 226Radionuclides such as Ra, these nucleic will decay for a long time and discharge radon and daughter thereof, and surrounding enviroment are caused permanent potential hazard.Especially 226The neutron exposure that Ra produces can cause human body and organism white blood cell to increase, and causes canceration and other radiation induced lesion, is one of major pollution thing in the uranium tailings.
The production Technology present according to China, general every production 1t uranium metal will produce the uranium tailings about 600t.
According to statistics, the uranium tailings that accumulates has in the world at present surpassed 20,000,000,000 t, and solid waste yard such as China's uranium tailings have 200 places approximately, is distributed in more than 30 the ground county of 14 provinces and regions, the whole nation.Wherein about 80% uranium barren rock and 90% uranium tailings are distributed in the Hunan, provinces such as Jiangxi and Guangdong, and these regional rainfall are abundant, populous.China's uranium tailings has that volume of cargo in storage is big, floor space is wide, apart from characteristics such as villages and small towns are near.The uranium tailings is stacked the region vegetation and is lacked severe water and soil erosion, wherein radionuclide 226Ra possibly pollute peripheral soil with rainwater and airborne dust diffusion.Therefore in uranium tailings and the radioactive pollution soil 226Ra removes imperative.
At present, to the uranium tailings with 226The Ra treatment method of soil contaminated has cladding process, method is buried in the strange land that scoops away and the lining method.These methods often can only be slowed down 226Ra is to the radiation of surrounding enviroment, and can not be fundamentally 226Ra removes from uranium tailings and soil.And in uranium tailings and the radioactive pollution soil 226What the removal method of Ra mainly adopted at present is physical partition method and soil washing method.Physical partition method is to separate with high strength magnetic through flotation, utilizes gravity and density contrast to remove in uranium tailings and the radioactive pollution soil 226Ra.The soil washing method is to utilize harmless leaching liquor, in lixiviate uranium tailings and the radioactive pollution soil 226Ra.Adopt these conventional methods in uranium tailings and the radioactive pollution soil 226Ra removes, and in actual moving process, has many weak points, and its drawback is exactly that energy consumption height, reagent consumption are big, expensive, technological process is tediously long, subsequent treatment is loaded down with trivial details, often easily environment is caused secondary pollution.Thereby, in reality, be difficult to carry out.
Phytoremediation is to adopt hyperaccumulative plant, and with certain crosses secondary element or compound is transferred to (particularly aerial part) in the plant body in large quantities in the soil, thereby the original position of rehabilitating soil is administered technology.Compare with traditional recovery technique, phytoremediation has investment and maintenance cost is low, easy and simple to handle, do not cause advantage such as secondary pollution, and might obtain economic benefit through recycling, has broad application prospects.Adopt plant that the uranium in the uranium tailings is repaired existing successful story; Domestic now " application number/200810030860.4/ denomination of invention/based on the plant restoration method of soil polluted by uranium mine tailings " and " patent No./ZL 200910044229.4/ denomination of invention/a kind of method of utilizing phytoremediation uranium tailings " have disclosed respectively utilizes dyers' grapes and macleaya cordata to repair uranium-bearing tailings (sand); But the object of its reparation only is to uranium in the uranium tailings (sand), and to uranium tailings (sand) 226The reparation of Ra does not appear in the newspapers.These successful cases to uranium reparation in the uranium tailings show in uranium tailings itself and the radioactive pollution soil 226Ra carries out phytoremediation, will 226The Ra absorption and accumulation is at the aerial part of plant, thereby reduces in uranium tailings and the radioactive pollution soil thereof 226The content of Ra, the resistance control 226The diffusion mobility of Ra reduces 226Ra is feasible to the public's irradiation.Yet most of plant is right 226Ra does not have enrichment, though existing bibliographical information the only a few plant right 226Ra has enrichment, but these plants can only be only with 226Ra hoards at its root, and can not be transported to its aerial part.This just requires to screen new 226The Ra enriching plant, this kind of plant can not only enrichment 226Ra, and can it be transported to its aerial part, be beneficial to gather in and focus on, thereby in removing uranium tailings and radioactive pollution soil to a greater extent 226Ra removes.
Summary of the invention
To above-mentioned situation, the object of the invention provides a kind of and utilizes plant to remove in uranium tailings and the radioactive pollution soil 226The method of Ra.The present invention directly will 226Its seedling of the enriching plant of Ra----curb limit grass (Pieris multifida) is planted in uranium tailings and radioactive pollution soil, makes it become to live, grow, and in enriched uranium tailings and the radioactive pollution soil 226Ra is simultaneously with institute's enrichment 226Ra is transported to its aerial part, and the regular period to be grown into, the harvesting aerial part focuses on, thereby removes in uranium tailings and the radioactive pollution soil 226Ra.This method both had draw materials conveniently, with low cost, remediation efficiency is high, has multiple advantages such as manageability, simple processing step, environmental risk are little again.
Its concrete measure is:
(1) spore germination is cultivated: with the ripe spore of curb limit grass, evenly be sowed on the spore culture medium or leaf mould that autoclaving is crossed on, be positioned in the constant incubator, be 20 ℃ in temperature, humidity is under 85% the condition, to cultivate 7-9d to spore germination.
(2) potted plant processing: after treating spore germination 5-7d, seedling being cultivated in the flowerpot, is 18-20 ℃ in temperature, and humidity is to cultivate under the condition of 70%-85%.
(3) be transplanted in uranium tailings and the radioactive pollution soil: when potted plant seedling age reaches 20-25d, seedling replanting in uranium tailings and radioactive pollution soil, gathered in aerial part behind 80-150d by to be let its growth, and concentrates and handle.The aerial stem of plant that keeps 3-5cm during harvesting makes the base stubble.Treat that new talent on the base stubble is long during to 50-70cm, once gather in again that the aerial stem of plant that keeps 3-5cm makes the base stubble.
(4) focus on: the aerial part of harvesting is transferred to concentrated drying, pulverizing, burning, the landfill of carrying out of place of safety, realize effectively resistance control 226The DIFFUSION TREATMENT of Ra.
The present invention with 226Ra enriching plant-curb limit grass (Pieris multifida) is a material, has solved in uranium tailings and the radioactive pollution soil 226Ra removes a difficult problem, has the important value of environmental protection.
A kind of utilization in plant removal uranium tailings and the radioactive pollution soil that this patent is invented 226The method of Ra is compared with existing technical method, has following technical advantage;
(1) the curb limit of being selected for use perennial, that growth is fast, biomass is big is careless, and the ability enrichment is a large amount of 226Ra is to its aerial part, and its aerial part through manual work or mechanized harvest after, can concentrate and transfer to place of safety and handle, operational administrative is easy.
(2) the curb limit grass of the present invention's use, well developed root system, it is vigorous to grow, and breeding is applied in uranium tailings and the radioactive pollution soil easily 226The removal of Ra has the advantage that cost is low, removal efficient is high, potential economic benefit is considerable.
(3) curb limit grass can not searched for food by cattle and sheep, therefore 226Ra can not increase environmental risk through the food chain transmission.
(4) adopt cultivation curb limit grass to remove in uranium tailings and the radioactive pollution soil 226Ra can significantly reduce 226Ra gets into underground water and farmland, cultivated plant on the uranium tailings in addition, and fixedly the uranium tailings reduces airborne dust, drag reduction 226The diffusion of pollutants such as Ra.
(5) in the uranium tailings and radioactive pollution soil that the present invention set up 226The removal pattern of Ra is green original position reparation, and the aerial part of being gathered in the crops can be concentrated and carry out security landfill, can not cause secondary pollution, repair process simultaneously and can not destroy original ecological environment, and help to quicken the uranium tailings weathering, help to improve soil because of 226Ra pollutes and the soil property that causes is degenerated and productivity descends, and recovers and the bio-diversity of raising uranium tailings and radioactive pollution soil, and can beautify the environment.
The present invention is applicable in the uranium tailings and peripheral radioactive pollution soil in uranium mine, uranium mill and uranium mine tailing storehouse etc. 226The removal of Ra.
The specific embodiment
The I material is formed
Curb limit grass (Pieris multifida), uranium tailings, radioactive pollution soil.
II material configuration and application process
Spore germination is cultivated, and is the ripe spore with curb limit grass, evenly be sowed on the spore culture medium or leaf mould that autoclaving is crossed on, be positioned in the constant incubator, be that 20 ℃, humidity are under 85% the condition in temperature, cultivate 7-9d until spore germination.Potted plant processing is after treating spore germination 5-7d, seedling to be cultivated in the flowerpot, is 18-20 ℃ in temperature, and humidity is to cultivate under the condition of 70%-85%.When seedling age reaches 20-25d, seedling replanting in uranium tailings and radioactive pollution soil, gathered in aerial part behind 80-150d by to be let its growth, and concentrates and handle.The aerial stem of plant that keeps 3-5cm during harvesting makes the base stubble.Treat that the new talent on the base stubble grows when arriving 50-70cm, once gathers in again.At last the aerial part of harvesting is transferred to concentrated drying, pulverizing, burning, the landfill of carrying out of place of safety.
The III principle
Perennial curb limit grass (Pieris multifida) is Pteridaceae Pteris plant.Root-like stock is short and upright, thick 1-1.5cm.The high 30-70cm of plant, the close shape pitchy scale that bored.Leaf two types are grown thickly, and do not have hair; The long 5-25cm of petiole, taupe brown or straw look; Give birth to sporangial fertile frond sheet and be avette, a pinniform, above green, below light green; Long 20-45cm, wide 15-25cm, accessory pinna normal 2-3 fork in bottom has the petiole except that base portion is a pair of; All the other each to the base portion decurrence, form the narrow wing in the rachis both sides, accessory pinna is linear, 3-7 is right; To life or closely to life, wide 3-7mm, full edge living sporangiorus along the accessory pinna lower edge.Sporangiorus is linear, and indusium exceeds leaf margin slightly, and is membranous; How the top accessory pinna does not divide, and tip is point gradually, and sterile, there is serration at the edge; Do not give birth to the accessory pinna or the equal broad of pinnule of sporangiorus, linear or oval, edge have irregular sharp sawtooth.Happiness warm and moist and half cloudy environment often are born on dark and damp foundation, well limit and the limestone.Be distributed widely in provinces and regions such as Hebei, Henan, Shandong, Anhui, Jiangsu, Zhejiang, Hunan, Hubei, Jiangxi, Fujian, Taiwan, Guangdong, Guangxi, Guizhou and Sichuan.
Through outdoor investigation, we find growing in uranium tailings and the radioactive pollution soil, and the curb limits are careless in a large number, and it is right to show 226Ra has extremely strong tolerance.Through indoor culture experiment and analyzing and testing, find that curb limit grass is can enrichment a large amount of 226Ra, and can 226The Ra enrichment is to its aerial part.
In the uranium tailings 226The content of Ra is 8350Bq/kg, and when the seedling age of curb limit grass reached 3 months, its average height reached 55cm.When line-spacing is 12cm, when spacing in the rows is 10cm, 1m then 2It is heavy that the biomass of interior its aerial part of planting site on average can reach the 1050g dry ash, and its middle period is 900g, and stem is 150g.In the leaf 226The average content of Ra is 150.6Bq/g, in the stem 226The average content of Ra is 0.12Bq/g, in the root 226The Ra average content is 1.78Bq/g.Thus it is clear that, in the uranium tailings, cultivate curb limit grass after 3 months, 1m 2Curb limit grass can get rid of about 135558Bq's 226Ra.
In radioactive pollution soil 226The content of Ra is 360Bq/kg, and when the seedling age of curb limit grass reached 5 months, its average height reached 65cm.When line-spacing is 12cm, when spacing in the rows is 10cm, 1m 2The biomass average out to 1350g dry ash of aerial part is heavy in the planting site, and its middle period is 1100g, and stem is 250g.In the leaf 226The average content of Ra is 26.6Bq/g, in the stem 226The average content of Ra is 0.01Bq/g, in the root 226The average content of Ra is 0.08Bq/g.Thus it is clear that, in radioactive pollution soil, cultivate curb limit grass after 5 months, 1m 2Curb limit grass in the planting site can be removed about 29262.5Bq's 226Ra.
The IV specific embodiment
A kind of utilization in plant removal uranium tailings and the radioactive pollution soil 226The method of Ra, it will 226The enriching plant of Ra--grass (Pieris multifida) seedling in-curb limit is planted in uranium tailings and radioactive pollution soil, makes it become to live, grow, to the step of gathering in and focusing on be:
(1) spore germination is cultivated: with the ripe spore of curb limit grass, evenly be sowed on the spore culture medium or leaf mould that autoclaving is crossed on, be positioned in the constant incubator, be 20 ℃ in temperature, humidity is under 85% the condition, to cultivate 7-9d until spore germination.
(2) potted plant processing: after treating spore germination 5-7d, seedling being cultivated in the flowerpot, is 18-20 ℃ in temperature, and humidity is to cultivate under the condition of 70%-85%.
(3) be transplanted in uranium tailings and the radioactive pollution soil: when potted plant seedling age reaches 20-25d, seedling replanting in uranium tailings and radioactive pollution soil, gathered in aerial part behind 80-150d by to be let its growth, and concentrates and handle.The aerial stem of plant that keeps 3-5cm during harvesting makes the base stubble.Treat that new talent on the base stubble is long during to 50-70cm, once gather in again that the aerial stem of plant that keeps 3-5cm makes the base stubble.
(4) focus on: the aerial part of harvesting is transferred to concentrated drying, pulverizing, burning, the landfill of carrying out of place of safety, realize effectively resistance control 226The DIFFUSION TREATMENT of Ra.
V embodiment
Embodiment 1, annual February the ripe spore of curb limit grass evenly is sowed on the solid agar medium, be positioned in the constant incubator, and be 20 ℃ in temperature, humidity is under 85% the condition, to cultivate 7-9d until spore germination.Behind the spore germination 5-7d, seedling being cultivated in the flowerpot, is 18-20 ℃ in temperature, and humidity is to cultivate under the condition of 70%-85%.When potted plant seedling age reaches 20-25d, seedling replanting is arrived 226Ra content is in the 8350Bq/kg uranium tailings, and the line-spacing of plantation is 12cm, and spacing in the rows is 10cm, gathers in aerial part behind the 90d, stays the aerial stem of plant of 3-5cm to make the base stubble.1m 2The biomass average out to 1050g dry ash of its aerial part is heavy in the planting site, and its middle period is 900g, and stem is 150g.In the leaf 226The average content of Ra is 150.6Bq/g, in the stem 226The average content of Ra is 0.12Bq/g, in the root 226The average content of Ra is 1.78Bq/g.When treating that the base stubble is gone up new talent length to 50-70cm, once gather in again.At this moment, 1m 2The biomass average out to 880g dry ash of aerial part is heavy in the planting site, and its middle period is 780g, and stem is 100g.In the leaf 226Ra just average content is 136.6Bq/g, stem 226The Ra average content is 0.10Bq/g, in the root 226The average content of Ra is 1.52Bq/g.At last the aerial part of harvesting is transferred to concentrated drying, pulverizing, burning, the landfill of carrying out of place of safety.Use this patent, in the uranium tailings, cultivate curb limit grass after 1 year, 1m 2Curb limit grass can get rid of about 242116Bq's 226Ra.
Embodiment 2, annual February the ripe spore of curb limit grass evenly are sowed on the leaf mould that autoclaving crosses, be positioned in the constant incubator, and be 20 ℃ in temperature, humidity is under 85% the condition, to cultivate 7-9d until spore germination.Behind the spore germination 5-7d, seedling being cultivated in the flowerpot, is 18-20 ℃ in temperature, and humidity is to cultivate under the condition of 70%-85%.When potted plant seedling age reaches 20-25d, seedling replanting is arrived 226Ra content is in the 6780Bq/kg uranium tailings, and the line-spacing of plantation is 12cm, and spacing in the rows is 10cm, gathers in aerial part behind the 90d, stays the aerial stem of plant of 3-5cm to make the base stubble.1m 2The biomass average out to 1080g dry ash of its aerial part is heavy in the planting site, and its middle period is 920g, and stem is 160g.In the leaf 226The average content of Ra is 128.5Bq/g, in the stem 226The average content of Ra is 0.08Bq/g, in the root 226The average content of Ra is 1.62Bq/g.When treating that the base stubble is gone up new talent length to 50-70cm, once gather in again.At this moment, 1m 2The biomass average out to 920g dry ash of its aerial part is heavy in the planting site, and its middle period is 790g, and stem is 130g.In the leaf 226The average content of Ra is 102.5Bq/g, in the stem 226The average content of Ra is 0.06Bq/g, in the root 226The Ra average content is 1.13Bq/g.At last the aerial part of harvesting is transferred to concentrated drying, pulverizing, burning, the landfill of carrying out of place of safety.Use this patent, in the uranium tailings, cultivate curb limit grass after 1 year, 1m 2Curb limit grass can get rid of about 199215.6Bq's 226Ra.
Embodiment 3, annual February the ripe spore of curb limit grass evenly are sowed on the solid agar medium, be positioned in the constant incubator, and be 20 ℃ in temperature, humidity is under 85% the condition, to cultivate 7-9d until spore germination.Behind the spore germination 5-7d, seedling being cultivated in the flowerpot, is 18-20 ℃ in temperature, and humidity is to cultivate under the condition of 70%-85%.When potted plant seedling age reaches 20-25d, seedling replanting is arrived 226Ra content is in the 680Bq/kg radioactive pollution soil, and the line-spacing of plantation is 12cm, and spacing in the rows is 10cm, gathers in aerial part behind the 150d, stays the aerial stem of plant of 3-5cm to make the base stubble.1m 2The biomass average out to 1260g dry ash of interior aerial part is heavy, and its middle period is 1050g, and stem is 210g.In the leaf 226The average content of Ra is 58.5Bq/g, in the stem 226The average content of Ra is 0.05Bq/g, in the root 226The average content of Ra is 1.13Bq/g.When treating that the base stubble is gone up new talent length to 50-60cm, once gather in again.At this moment, 1m 2The biomass average out to 860g dry ash of its aerial part is heavy in the planting site, and its middle period is 750g, and stem is 110g.In the leaf 226The average content of Ra is 46.0Bq/g, in the stem 226The average content of Ra is 0.04Bq/g, in the root 226The Ra average content is 0.96Bq/g.At last the aerial part of harvesting is transferred to concentrated drying, pulverizing, burning, the landfill of carrying out of place of safety.Use this patent, in radioactive pollution soil, cultivate curb limit grass after 1 year, 1m 2Curb limit grass can get rid of about 95939.9Bq's 226Ra.
Embodiment 4, annual February the ripe spore of curb limit grass evenly are sowed on the leaf mould that autoclaving crosses, be positioned in the constant incubator, and be 20 ℃ in temperature, humidity is under 85% the condition, to cultivate 7-9d until spore germination.Behind the spore germination 5-7d, seedling being cultivated in the flowerpot, is 18-20 ℃ in temperature, and humidity is to cultivate under the condition of 70%-85%.When potted plant seedling age reaches 20-25d, seedling replanting is arrived 226Ra content is in the 360Bq/kg radioactive pollution soil, and the line-spacing of plantation is 12cm, and spacing in the rows is 10cm, gathers in aerial part behind the 150d, stays the aerial stem of plant of 3-5cm to make the base stubble.1m 2The biomass average out to 1350g dry ash of its aerial part is heavy in the planting site, and its middle period is 1100g, and stem is 250g.In the leaf 226The average content of Ra is 26.6Bq/g, in the stem 226The average content of Ra is 0.01Bq/g, in the root 226The average content of Ra is 0.08Bq/g.When treating that the base stubble is gone up new talent length to 50-60cm, once gather in again.At this moment, 1m 2The biomass average out to 1020g dry ash of its aerial part is heavy in the planting site, and its middle period is 860g, and stem is 160g.In the leaf 226The average content of Ra is 17.2Bq/g, in the stem 226The average content of Ra is 0.01Bq/g, in the root 226The average content of Ra is 0.20Bq/g.At last the aerial part of harvesting is transferred to concentrated drying, pulverizing, burning, the landfill of carrying out of place of safety.Use this patent, in radioactive pollution soil, cultivate curb limit grass after 1 year, 1m 2Curb limit grass can get rid of about 30743.3Bq's 226Ra.
Below only be preferred embodiments of the present invention, according to above-mentioned design of the present invention, those skilled in the art can also make various modifications and conversion to this.For example, be planted in difference 226In the uranium tailings and radioactive pollution soil of Ra concentration, line-spacing, spacing in the rows and the various nutritional condition of plantation are improved, adopted different harvesting mode and period, different spore germinations, cultivation and method for culturing seedlings or the like.Yet similar this conversion all belongs to essence of the present invention with revising.

Claims (1)

1. one kind is utilized plant to remove in uranium tailings and the radioactive pollution soil 226The method of Ra is characterized in that, concrete steps are:
(1) spore germination is cultivated: with the ripe spore of curb limit grass, evenly be sowed on the spore culture medium or leaf mould that autoclaving is crossed on, be positioned in the constant incubator, be 20 ℃ in temperature, humidity is under 85% the condition, to cultivate 7-9d to spore germination;
(2) potted plant processing: after treating spore germination 5-7d, seedling being cultivated in the flowerpot, is 18-20 ℃ in temperature, and humidity is to cultivate under the condition of 70%-85%;
(3) be transplanted in uranium tailings and the radioactive pollution soil: when potted plant seedling age reaches 20-25d, seedling replanting in uranium tailings and radioactive pollution soil, gathered in aerial part behind 80-150d by to be let its growth, and concentrates and handle; The aerial stem of plant that keeps 3-5cm during harvesting makes the base stubble; Treat that new talent on the base stubble is long during to 50-70cm, once gather in again that the aerial stem of plant that keeps 3-5cm makes the base stubble;
(4) focus on: the aerial part of harvesting is transferred to concentrated drying, pulverizing, burning, the landfill of carrying out of place of safety, realize effectively resistance control 226The DIFFUSION TREATMENT of Ra.
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