CN102603079A - Method for recycling treatment of industrial uranium-containing wastes - Google Patents
Method for recycling treatment of industrial uranium-containing wastes Download PDFInfo
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- CN102603079A CN102603079A CN2012100733910A CN201210073391A CN102603079A CN 102603079 A CN102603079 A CN 102603079A CN 2012100733910 A CN2012100733910 A CN 2012100733910A CN 201210073391 A CN201210073391 A CN 201210073391A CN 102603079 A CN102603079 A CN 102603079A
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Abstract
The invention discloses a method for the recycling treatment of industrial uranium-containing wastes. By a hydrothermal reaction in which biological substances and soluble U (VI) coexist, the soluble U (VI) can be reduced into asphalt uranium of which the particle diameter is 5 to 20nm; and the asphalt uranium with larger size is beneficial to precipitating and recycling. According to the method, uranium resources can be effectively extracted and recycled from uranium-containing wastes.
Description
Technical field
The present invention relates to the leach liquor or the industrial uranium-containing waste water of industrial uranium-bearing waste; With biomass (Biomass) is reductive agent; Generate nano asphalt uranium solids precipitation through hydrothermal method reduction hexavalent uranium, thus such uranium-bearing waste of purifying treatment and make the method at its resource utilization place.
Background technology
Along with the high speed development of nuclear power cause in recent years, human demand to uranium sharply increases.According to international nuclear power structured data, by the end of in January, 2011, the whole world has 442 nuclear power plants of 30 countries to move, and 65 nuclear power plants of 16 countries build.Nuclear power plant in operation will consume uranium metal fuel 66000-69000 ton every year.20 tons of uranium metal fuel of every production (
22.7 ton UO
2) need 17000 tons of the uranium ores of exploitation 1%.Smelt from the exploitation of uranium ore and to have produced a large amount of uranium-bearing waste and waste water the spissated process.Only be the U.S., be distributed with the radionuclide contamination thing, 3,000,000 m of surpassing are arranged in 120 places, 36 areas
3Buried waste, estimated at 4,750 hundred million gallons of affected underground water and 7,500 ten thousand m
3Contaminated settling.In the world, have above 2 * 10
9The mine tailing that t uranium pollutes is threatening human health just for a long time.At numerous local uranium polluted underground water and surface water found, comprise agriculture evaporation tank, Nuclear weapons manufactured place, mill tailings site.The open-air long-term stacking of these uranium-bearing wastes and the random discharging of uranium-containing waste water cause serious pollution to surrounding environment, and human health and natural ecological environment are produced great effect.Therefore, human improvement to the uranium-bearing waste has proposed urgent demand.
Current, being used to administer the main method that nucleic pollutes has physical method and chemical process.Like solid landfill, vitrification, zeolite adsorption, IX, SX etc.But these method costs are higher, and are difficult to use in improvement by the soil of radionuclide pollution in wide area and water body.Because the function of the low cost of mikrobe, lasting self-replacation changes transportable U (VI) into insoluble uranium deposition if can realize bacterium, is expected in the reparation of big area soil and the pollution of water body uranium, to play a significant role.Research shows that several kinds of modes below mikrobe mainly passes through change transportable U (VI) into insoluble uranium deposition: 1) be reduced into pitch uranium (UO to U (VI) through the special bacterium of minority
2) (D.R.LOVLEY, 1991, Letters to nature); 2) through the PO in the water body
4 2-Or bacterium produces phosphoesterase reduction triphosphoric acid glyceryl ester (G3P) generation PO
4 2-Combine to form HUO with uranium
2PO
4Or Ca (UO
2)
2(PO
4)
2(L.E.Macaskie, 2000, Science); 3) the Polysaccharides, peptide complexes coordination of uranium and cell walls forms R-COO-UO
2+Mixture and sedimentation (A.Barkleit, 2009, Dalton transactions).Yet investigators also notice, after biological prosthetic, and formed HUO
2PO
4Be deposited in CO
2Can form soluble UO gradually again in the high water body of content
2CO
3In water body, continue migration and diffusion.Along with the decomposition of organic matter, R-COO-UO
2+UO in the mixture
2+Can be discharged into water body again again; All less than 3nm, this undersized nano asphalt uranium not only is prone to migration by the size of the formed pitch uranium of micro-reduction, and self is also unstable, and it can be oxidized to soluble U (VI) again again in well-oxygenated environment.
By on can know, solve the pollution problem of uranium, must develop relevant method and carry out the recovery of uranium resources, it is removed from environment effectively.Based on this thinking, we select the representational biomass of multiclass (bacterium, yeast and algae) for use, carry out the uranyl ion of fast enriching solubility through biomass; And then through hydrothermal method under the condition of biomass as reductive agent, change into the pitch uranium particle of large-size to hexavalent uranium, recycle.
Summary of the invention
The method that the object of the present invention is to provide a kind of industrial uranium-bearing changing rejected material to useful resource to handle effectively solves the method for the pollution problem of uranium.
The present invention adopts following technical scheme:
With biomass (Biomass) is reductive agent, adopts hydrothermal method to reduce the hexavalent uranium in industrial uranium-bearing waste leach liquor or the uranium-containing waste water, generates nano asphalt uranium particle, and then reclaims uranium resources.
Described industrial uranium-bearing waste is that uranium mine tailing or uranium are smelted leach liquor or the uranium-containing waste water that produces waste residue.The U of solubility (VI) concentration use range is 42 μ mol/L-4.2mmol/L.
These biomass (Biomass) comprise bacterium, a kind of or wherein any several kinds combination in yeast and the algae.Biomass join in corresponding uranium-bearing leach liquor and the uranium-bearing trade effluent by the amount of dry weight 10-1000mg/L.
Said hydrothermal method reductive temperature is 150-300 ℃, and the hydrothermal method reductive time is 12-72 hour.
Said hydrothermal method reductive optimum temperuture is 240 ℃, and the reduction Best Times is 48 hours.
Described nano asphalt uranium particle grain size is 5-20nm.The pitch uranium of this large-size helps recycling.The precipitate recovery rate of uranium is greater than 97%.
Embodiment
Instance 1. Gram-negative bacterias are to the conversion of uranyl acetate
Human pallid bacillus, enterobacter cloacae and intestinal bacteria preservation or buy in Chinese common micro-organisms preservation administrative center (CGMCC).Preserving number or purchase numbering are respectively: CGMCC1715,1.1015 and 1.1100.The gained bacterial classification inserts and to be equipped with in the 100ml triangular flask of 30ml LB liquid nutrient medium, under aerobic, normal pressure, 30 ℃ of conditions, is placed in 200 rev/mins of shaking tables shaking culture and spends the night and make the bacterial classification recovery.Gram prolapse of uterus after above-mentioned three kinds of recoveries is transferred four according to bacterium liquid and 1: 100 ratio of substratum and to be equipped with respectively in the triangular flask of 250ml LB substratum.After cultivating 24 hours under 37 ℃ the condition, got into and carried out microorganism collection.The gained thalline is called biomass.Three kinds of biomass join by the amount of dry weight 500mg/L in the solubility uranyl acetate of U (VI) of 210 μ mol/L.After acting on 20-30 minute, there are a large amount of depositions to produce, through centrifugal collecting precipitate; U (VI) residual in the supernatant is with induction coupled plasma radiating light spectrometer (ICP-OES; Model: Ultima2, producer: Britain Jobin Yvon, down with) measure (as shown in table 1).Through three kinds of sedimentary uranium of biomass, joining the liner volume by the amount of every milliliter of 0.1g weight in wet base respectively is 20 milliliters water heating kettle, adds 15 milliliters of people in every still.Build after the baking oven of putting into 240 ℃ after the kettle cover hatched 48 hours.X-ray diffraction (XRD, model: X ' Pert PRO, producer: Dutch PANalytical, down with) result shows that soluble U (VI) is reduced into pitch uranium, this reduzate--the particle diameter of pitch uranium is respectively 10.9,12.4 and 11.6nm.The precipitate recovery rate such as the table 1 of uranium.
Table 1 Gram-negative bacteria is to the conversion of uranyl acetate
Instance 2. gram-positive microorganisms are to the conversion of uranyl acetate
Subtilis and bacillus cereus are bought in CGMCC, buy numbering and are respectively: 1.1630 and 1.1626.The gained bacterial classification is pressed the method for instance 1 and is cultivated the corresponding biomass of acquisition.These biomass join in the solubility uranyl acetate of 84 μ mol/L by the amount of dry weight 200mg/L.After acting on 20-30 minute, through centrifugal collecting precipitate, U (VI) residual in the supernatant measures (result such as table 2) with ICP-AAS.Through two kinds of sedimentary uranium of gram-positive microorganism, joining the liner volume by the amount of every milliliter of 0.1g weight in wet base respectively is 20 milliliters water heating kettle, adds 15 milliliters of people in every still.Build after the baking oven of putting into 240 ℃ after the kettle cover hatched 48 hours.XRD result shows that soluble U (VI) is reduced into pitch uranium, this reduzate--the particle diameter of pitch uranium is respectively 9.6. and 8.4nm.The precipitate recovery rate such as the table 2 of uranium.
Table 2 gram-positive microorganism is to the conversion of uranyl acetate
Instance 3. yeast and yeast extract thereof are to the conversion of uranyl acetate
Yeast is bought in Chinese common micro-organisms preservation administrative center (CGMCC), is numbered: 2.2081; Yeast extract is bought in Angel Yeast Co.,Ltd.The gained barms inserts 30ml yeast perfect medium (yeast perfect medium: yeast extract 10g is housed; Peptone 20g; Glucose 20g; Be settled to 1L) triangular flask in, under aerobic, normal pressure, 28 ℃ of conditions, be placed in 200 rev/mins of shaking tables shaking culture and spend the night and make the barms recovery.The yeast of recovery is transferred according to bacterium liquid and 1: 100 ratio of substratum and is equipped with in the triangular flask of 250ml yeast perfect medium.After cultivating 24 hours under 28 ℃ the condition, got into and collected.This yeast gleanings joins in the solubility uranyl acetate of 252 μ mol/L with the amount of the commercial yeast extract of buying by dry weight 600mg/L.After acting on 20-30 minute, through the throw out of centrifugal collection uranium, U (VI) residual in the supernatant measures result such as table 3 with ICP-AAS.The sedimentary uranium of yeast and yeast extract, joining the liner volume by the amount of every milliliter of 0.1g weight in wet base respectively is 20 milliliters water heating kettle, adds 15 milliliters of people in every still.Build after the baking oven of putting into 240 ℃ after the kettle cover hatched 48 hours.XRD result shows that soluble U (VI) also is reduced into pitch uranium, this reduzate--the particle diameter of pitch uranium is respectively 14.2 and 12.8nm.The precipitate recovery rate such as the table 3 of uranium.
Table 3 yeast and yeast extract thereof are to the conversion of uranyl acetate
Instance 4. various biomass are to the conversion of uranyl nitrate
The various biomass that instance 1-3 cultivates join in the solubility uranyl nitrate of 316 μ mol/L by the amount of dry weight 800mg/L.After acting on 20-30 minute, through the throw out of centrifugal collection uranium, U (VI) residual in the supernatant measures result such as table 4 with ICP-AAS.The sedimentary uranium of various biomass, joining the liner volume by the amount of every milliliter of 0.1g weight in wet base respectively is 20 milliliters water heating kettle, adds 15 milliliters of people in every still.Build after the baking oven of putting into 240 ℃ after the kettle cover hatched 48 hours.XRD result shows that soluble uranyl nitrate also is reduced into pitch uranium, and this reduzate--the particle diameter of pitch uranium and the precipitate recovery rate of uranium are as shown in table 4.
The various biomass of table 4 are to the conversion of uranyl nitrate
Instance 5. biomass are to uranium mine tailing leach liquor and uranium-bearing trade effluent
Human pallid bacillus and yeast extract join uranium mine tailing leach liquor and uranium-bearing trade effluent respectively by the amount of dry weight 1000mg/L, and wherein uranium concentration is respectively 4.2 and 1.2mmol/L.The uranium mine tailing is taken from uranium mine tailing storehouse, Pucheng, Fujian, and the uranium trade effluent is taken from Xinjiang Hong Shitan uranium ore factory.After acting on 20-30 minute, through the throw out of centrifugal collection uranium.Two kinds of sedimentary uranium of biomass, joining the liner volume by the amount of every milliliter of 0.1g weight in wet base respectively is 20 milliliters water heating kettle, adds 15 milliliters of people in every still.Build after the baking oven of putting into 240 ℃ after the kettle cover hatched 48 hours.XRD result shows that the hexavalent uranium in uranium mine tailing leach liquor and the uranium-bearing trade effluent is reduced into pitch uranium, and the median size of pitch uranium is respectively 10.6nm and 14.5nm (table 5).The precipitate recovery rate of uranium is respectively 98.9% and 98.3% (table 5) in uranium mine tailing leach liquor and the uranium-bearing trade effluent.
Table 5 biomass are to the conversion of uranium mine tailing leach liquor and uranium-bearing trade effluent
Claims (8)
1. method that industrial uranium-bearing changing rejected material to useful resource is handled is characterized in that: as reductive agent, adopt hydrothermal method to reduce hexavalent uranium in the industrial uranium-bearing waste with biomass, generate recyclable nano asphalt uranium particle, carry out uranium resources and recycle.
2. the method that industrial uranium-bearing changing rejected material to useful resource as claimed in claim 1 is handled, it is characterized in that: described industrial uranium-bearing waste is a uranium mine tailing leach liquor.
3. the method that industrial uranium-bearing changing rejected material to useful resource as claimed in claim 1 is handled is characterized in that: the leach liquor that described industrial uranium-bearing waste is the uranium ore melting waste slag.
4. the method that industrial uranium-bearing changing rejected material to useful resource as claimed in claim 1 is handled, it is characterized in that: described industrial uranium-bearing waste is a uranium ore smeltery uranium-bearing trade effluent.
5. the method that industrial uranium-bearing changing rejected material to useful resource as claimed in claim 1 is handled, it is characterized in that: described biomass comprise bacterium, a kind of or wherein any several kinds combination in yeast and the algae.
6. the method that industrial uranium-bearing changing rejected material to useful resource as claimed in claim 1 is handled, it is characterized in that: described nano asphalt uranium particle grain size is 5-20nm.
7. the method that industrial uranium-bearing changing rejected material to useful resource as claimed in claim 1 is handled, it is characterized in that: said hydrothermal method reductive temperature is 150-300 ℃, and the reductive time is 12-72 hour.
8. the method that industrial uranium-bearing changing rejected material to useful resource as claimed in claim 1 is handled, it is characterized in that: said hydrothermal method reductive temperature is 240 ℃, and the reductive time is 48 hours.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103881929A (en) * | 2014-03-13 | 2014-06-25 | 湛江德玥生物工程有限公司 | Purification compound bacterium and purification compound probiotic preparation as well as preparation method of compound probiotic preparation |
| CN104485148A (en) * | 2014-11-18 | 2015-04-01 | 中国科学院福建物质结构研究所 | High-efficient method of extracting uranyl ions from water |
| CN110441384A (en) * | 2019-07-12 | 2019-11-12 | 核工业北京地质研究院 | A kind of determining pitch sinks the experimental method of poly- action intensity to uranium |
Citations (1)
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|---|---|---|---|---|
| CN1948527A (en) * | 2006-10-30 | 2007-04-18 | 北京斯帕顿矿产资源投资咨询有限公司 | Method of extracting radioactive uranium in fly ash |
-
2012
- 2012-03-19 CN CN2012100733910A patent/CN102603079A/en active Pending
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1948527A (en) * | 2006-10-30 | 2007-04-18 | 北京斯帕顿矿产资源投资咨询有限公司 | Method of extracting radioactive uranium in fly ash |
Non-Patent Citations (2)
| Title |
|---|
| LAURENT RICHARD ET AL.: "A thermodynamic model of uranium reduction by organic matter in the Proterozoic hydrothermal systems of Oklo (Gabon)", 《GEOCHIMICA ET COSMOCHIMICA ACTA》, vol. 71, no. 15, 31 August 2007 (2007-08-31), pages 837 * |
| 闵茂中等: "厌氧菌Shewcenella putrefaciens 还原U(VI)的实验研究：应用于中国层间氧化带砂岩型铀矿", 《中国科学D辑 地球科学》, vol. 34, no. 2, 31 December 2004 (2004-12-31), pages 125 - 129 * |
Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103881929A (en) * | 2014-03-13 | 2014-06-25 | 湛江德玥生物工程有限公司 | Purification compound bacterium and purification compound probiotic preparation as well as preparation method of compound probiotic preparation |
| CN103881929B (en) * | 2014-03-13 | 2017-03-01 | 湛江德玥生物工程有限公司 | Purification compound bacteria and purification composite probiotics preparations and preparation method |
| CN104485148A (en) * | 2014-11-18 | 2015-04-01 | 中国科学院福建物质结构研究所 | High-efficient method of extracting uranyl ions from water |
| CN110441384A (en) * | 2019-07-12 | 2019-11-12 | 核工业北京地质研究院 | A kind of determining pitch sinks the experimental method of poly- action intensity to uranium |
| CN110441384B (en) * | 2019-07-12 | 2021-11-09 | 核工业北京地质研究院 | Experimental method for determining uranium precipitation action strength of asphalt |
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Application publication date: 20120725 |