CN109859874A - A method of uranium-containing waste water is handled using alloy material - Google Patents
A method of uranium-containing waste water is handled using alloy material Download PDFInfo
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- CN109859874A CN109859874A CN201711232395.8A CN201711232395A CN109859874A CN 109859874 A CN109859874 A CN 109859874A CN 201711232395 A CN201711232395 A CN 201711232395A CN 109859874 A CN109859874 A CN 109859874A
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Abstract
The present invention provides a kind of method of reduction adsorption performance processing uranium-containing waste water using two kinds of activity metals.This method is the ability for providing electronics using the reproducibility of iron, aluminium using iron and aluminium as material and the adsorptivity processing uranium-containing waste water of ferriferous oxide.Comprise the concrete steps that: (1) under conditions of sodium borohydride solution is added dropwise, by iron: aluminium molal weight is than synthesizing ferrum-aluminium alloy material in the way of for 1:10；(2) uranium concentration is in 1-200 mg/L in adjusting uranium-containing waste water, and pH is between 4-6；(3) the ratio of 0.1-0.4 g alloy material to be added in every liter of waste water, it is sufficiently mixed uranium-containing waste water and alloy material, is stirred evenly；(4) it after acting on 5 min-2 h, is separated by solid-liquid separation in the way of film pressure filtration or standing.The present invention can make in the uranium-containing waste water of 1-200 mg/L uranium removal rate up to 96%.This method is simple and efficient, and the removal efficiency of uranium is high, has good environmental benefit and social benefit.
Description
Technical field
The present invention relates to uranium-bearing Spent Radioactive water treatment fields, more particularly, are related to a kind of by synthesis metal material
Quickly remove the method for sexavalence uranyl ion in uranium-containing waste water.
Background technique
Uranium is most important nuclear fuel in current nuclear energy uses, with the continuous development of global atomic energy cause, in uranium ore
Exploitation, smelt and the elimination of nuclear facilities during caused by uranium-containing waste water type and quantity it is more and more, to human health and
The potential threat of natural ecological environment is on the rise, and also just more stringent requirements are proposed for processing of the people to uranium-containing waste water.Containing
In terms of the processing of uranium waste water, current main processing method has: chemical precipitation, ion exchange, evaporation and concentration, absorption method, cohesion
The methods of method, UF membrane.In place of these conventional methods more or less come with some shortcomings in actual application, week is such as handled
The problems such as phase is long, and process flow is many and diverse, and purification efficiency is low.
Uranium usually exists in water body with sexavalence uranyl ionic forms, when sexavalence uranyl ion is reduced to uranous,
It is capable of forming and precipitates and by standing or filtering removal.Zero-valent Iron has very high reduction activation, can be used in quickly restoring
Sexavalence uranyl, and the iron ion after oxidation can form complex with sexavalence uranyl and uranous, enhance uranous goes
Except stability, improve the adsorption efficiency of sexavalence uranyl, but since Zero-valent Iron is too active, preparation process be easy in air and environment
Oxygen react and be oxidized, thus application when unit mass removal efficiency it is not high.At the same time, aluminium also has higher
Reduction activation, and when zeroth order aluminium of unit mass is converted into trivalent, is capable of providing more electronics for restoring, but zeroth order aluminium
When simple substance and the ionization of sexavalence uranyl, zeroth order aluminium can form fine and close oxidation film after being oxidized on surface, prevent further
Reaction, so that the removal efficiency of unit mass is relatively low.So if Zero-valent Iron and zeroth order aluminium are used in combination, it can not only
Enough prevent the formation of aluminium surface oxidation film, additionally it is possible to extend the action time of iron to improve the reduction removal efficiency of uranium.
Summary of the invention
For above situation, sexavalence uranyl is efficiently restored and removed using ferroaluminium the object of the present invention is to provide a kind of
The method of ion, this method is using ferroaluminium, the reduction of material collection and adsorption function integration is chemically synthesized, in waste water
Sexavalence uranyl ion remaval it is high-efficient.
The present invention forms ferroaluminium, using in alloy by the way that a small amount of iron ion is restored to zeroth order aluminium simple substance surface
Simple substance and low price iron reproducibility, the sub- ability of pure aluminum continued power and high price iron flocculation adsorption performance, with efficiently quickly
Reduce the ratio of sexavalence uranyl ion in solution.Concrete measure is: it is equal that mixing is added into uranium-containing waste water in ferroaluminium solution
It is even, redox reaction is brought it about, sexavalence uranyl in waste water is quickly reduced to uranous and forms flocculent deposit, separation is received
Collect the precipitating of uranium.It comprises the concrete steps that:
(1) according to iron: aluminium molal weight weighs a certain amount of ferrous salt and zeroth order aluminium simple substance particle than the ratio for 1:10, point
It is not placed in the solution of certain volume and is heated to 80 DEG C (ferrous salt solution can dissolve, and zeroth order alumina particles will not dissolve)；
(2) sodium borohydride solution of 7.5mg/mL is configured；
(3) ferrous solution and aluminum solutions in (1) are quickly mixed and stirred for uniformly, the sodium borohydride solution being then added dropwise in (2) is straight
Into solution, iron ion is reduced to alumina particles surface (alloy of configuration 0.15g about needs 10mL sodium borohydride solution) entirely, and 4000
Rpm is centrifuged 10min, and separation of solid and liquid obtains ferroaluminium material；
(4) alloy material 0.1-0.4 g, stirring are added in the uranium-containing waste water that every liter of uranium concentration is 1-200 mg/L, pH=4-6
Uniformly；
(5) it after reacting 5min-2h, is separated by solid-liquid separation in the way of film pressure filtration or standing.
In order to reach better removal effect, following measures can be taken:
(1) micro sodium borohydride solution can be added dropwise into pure aluminum particle solution first to remove aluminium when synthesizing metal material
The oxidation film on grain surface；
(2) reaction temperature control is advisable at 30 DEG C -50 DEG C, and increase temperature appropriate can promote the ferric ion after oxidation
Ferric hydroxide colloid is formed, to reach the flocculation sedimentation effect of enhancing uranium；
(3) dosage for suitably increasing alloy material can be improved the removal rate of sexavalence uranyl ion in waste water, but dosage with
Every liter is advisable no more than 0.4g；
(4) material is preferably ready-to-use, can also be saved under conditions of low temperature oxygen-free, and the uranium-containing waste water after processing should be as early as possible
It is separated by solid-liquid separation, to prevent uranous sediment to be oxidized to sexavalence uranyl ion again in aerobic environment.
The present invention is that a kind of a kind of alloy material synthesized using Zero-valent Iron and a variety of advantages of zeroth order aluminium is contained for removing
Sexavalence uranyl ion in uranium waste water, compared to present technology have it is following the utility model has the advantages that
(1) easy to operate, it can be saved in a certain way after materials synthesis, it is used as needed when can accomplish to need；
(2) reduction and adsorption efficiency are high, and total removal ability of sexavalence uranyl ion reaches as high as 578mg/g；
(3) action time is short, allow in 5 minutes reduction reaction carry out it is more complete, effectively reduce processing the time, mention
High technology treatment effeciency；
(4) source of drawing material is wide and safe, environmentally friendly, without secondary pollution, and uranium-bearing radiates during being suitable for nuclear fuel cycle
The efficient process and recycling of property waste water.
The invention patent relates to main function mechanism see attached drawing 1, be described as follows:
(1) sexavalence uranyl ion reduction at uranous and is formed precipitating by Zero-valent Iron first, and Zero-valent Iron is oxidized to ferric iron
Ion；
(2) then the zeroth order aluminium in conjunction with Zero-valent Iron provides enough electronics to ferric ion, and ferric ion is restored again
For Zero-valent Iron, recycled with this；
(3) part ferric ion can act on forming stable complex precipitating or forming hydroxide with uranous or hexavalent uranium
Iron colloid, and product has certain suction-operated to the uranium in waste water；
(4) solution can be entered otherwise by providing the aluminium after electronics, and non-formation oxidation film.
Detailed description of the invention
Fig. 1 is a kind of method mechanism schematic diagram that uranium-containing waste water is handled using alloy material of the present invention.
The removal efficiency of the position Fig. 2 fe, pure aluminum and ferroaluminium to Uranium in Waste Water.
Fig. 3 is the influence that pH removes Uranium in Waste Water to ferroaluminium.
Fig. 4 is the influence that ionic strength removes waste water uranium to ferroaluminium.
Fig. 5 is the influence that temperature removes waste water uranium to ferroaluminium.
Fig. 6 is uranium and (c) electron-microscope scanning figure after (b), alloy effect before pure aluminum (a), alloy effect.
Fig. 7 is the infared spectrum of aluminium and ferroaluminium and uranium effect front and back.
Fig. 8 is the X-ray diffractogram of iron, aluminium, ferroaluminium and uranium effect front and back.
X-ray photoelectron spectroscopy figure after the position Fig. 9 alloy and uranium effect.
Specific embodiment
Invention is further described in detail With reference to embodiment.
Embodiment 1: 0.06g Zero-valent Iron is put into respectively into the uranium-containing waste water of three groups of 1L, 100mg/L, pH=5 at room temperature
Grain, 0.30g zeroth order alumina particles and 0.36g ferroaluminium, the removal efficiency relationship of changing with time of uranium are shown in attached drawing 2.5min
Reaction levels off to balance afterwards, reacts after 1h and reaches complete equipilibrium, the results showed that, ferroaluminium is to the removal effect of uranium than iron, aluminium
The sum of the effect of simple substance removal uranium will be got well.
Embodiment 2: adjust at room temperature eight groups of 100mL 100mg/L, pH be respectively 3,4,5,6,7,8,9,10 uranium-bearing it is useless
Water is separately added into 0.036g ferroaluminium, and the removal efficiency of uranium is as shown in Figure 3 with pH variation relation after reaction 1h.The result shows that
Uranium has good removal efficiency when between pH=4-6, maximum in the uranium removal efficiency of pH 5.
Embodiment 3: a certain amount of sodium chloride is added into the uranium-containing waste water of three groups of 1L, 100mg/L, pH=5 at room temperature
Grain, making its concentration is respectively 0.01mol/L, 0.05mol/L, 0.10mol/L, adds 0.36g ferroaluminium respectively, and uranium is gone
Except the efficiency relationship of changing with time is shown in attached drawing 4.As a result illustrate that the ionic strength big solution removal time is shorter.
Embodiment 4: under the conditions of different temperatures (30 DEG C, 40 DEG C, 50 DEG C), respectively to the different uranium concentrations of 100mL, pH=5
(50,75,100,125,150,175,200mg/L), uranium-containing waste water in add 0.025g ferroaluminium, after effect 1 hour, uranium
Removal rate it is as shown in Figure 5 with the variation relation of uranium concentration.The removal ability of alloy material with uranium concentration increase and temperature
Increase and increase, highest removal ability reaches 578mg/g.
Embodiment 5: take alumina particles (a), alloy material (b), reacted with 100mg/L uranium-containing waste water after sediment (c)
Make electron-microscope scanning and energy spectrum analysis (Fig. 6), the results showed that, in alloy material, iron particle burden is on alumina particles surface.Alloy with contain
After uranium waste water reaction, uranium is deposited on alloy surface.
Embodiment 6: take alumina particles, alloy material, reacted with 100mg/L uranium-containing waste water after sediment make Fourier's change
Change infrared spectrum analysis (Fig. 7), the results showed that, there is the absorption peak of uranium in the alloy after reaction.
Embodiment 7: take iron particle, alumina particles, alloy material, reacted with 100md/L uranium-containing waste water after sediment make X
X ray diffraction analysis x (Fig. 8), the results showed that, there are the crystal diffractions of uranous and sexavalence uranyl for the alloy material after reacting
Peak, while also occurring the hydroxide characteristic peak of iron in sediment, it was confirmed that the reduction of alloy and the hydroxide of iron
The formation and its adsorption effect of colloid.
Embodiment 8: using x-ray photoelectron spectroscopy to alloy material (on), reacted with 100mg/L uranium-containing waste water after
Sediment (under) iron (a), aluminium (b), oxygen (c), the discovery of uranium (d) element valence in (Fig. 9), the content of the Zero-valent Iron after reacting
It being reduced, uranium exists jointly with tetravalence and sexavalence, and it is consistent with X-ray diffraction analysis result, further demonstrate machine before this
It is reasonable that reason, which speculates,.
Claims (9)
1. a kind of method using alloy material processing uranium-containing waste water, it is characterised in that: the processing method packet of the uranium-containing waste water
Include following steps: (1) pH of adjusting uranium-containing waste water to acidity；(2) homemade conjunction is added into the uranium-containing waste water for being adjusted to acidity
Golden material reacts certain time；(3) it is separated by solid-liquid separation, obtains supernatant and uranium-bearing solids.
2. the processing method of uranium-containing waste water according to claim 1, which is characterized in that uranium concentration is in the uranium-containing waste water
1-200 mg/L。
3. the processing method of uranium-containing waste water according to claim 1, which is characterized in that the pH value for adjusting uranium-containing waste water
To 4-6.
4. the processing method of uranium-containing waste water according to claim 1, which is characterized in that the homemade alloy material is iron
With the alloy material of aluminium, specific preparation process is as follows: (1), according to iron: aluminium molal weight ratio is 1:10, weighs a certain amount of Asia
Molysite and zeroth order aluminium simple substance particle are respectively placed in the deionized water of certain volume and are heated to 80 DEG C (ferrous salt can dissolve, zeroth order
Alumina particles will not dissolve)；(2), the sodium borohydride solution of 7.5mg/mL is configured；(3), two solution in (1) are quickly mixed, is passed through
It stirs (250 rpm) to be uniformly mixed, the sodium borohydride solution (alloy of 0.15 g of configuration about needs 10mL) being then added dropwise in (2) is straight
Into solution, ferrous ion is reduced to alumina particles surface completely, and 4000 rpm are centrifuged 10 min, is separated by solid-liquid separation, obtains iron aluminium
Alloy material.
5. the processing method of uranium-containing waste water according to claim 1, which is characterized in that every liter of uranium-containing waste water, which is added, to be closed
Golden amount 0.1-0.4 g, reaction time are 5 min-2 h, and reaction temperature is 30-50 DEG C.
6. the temperature appropriate that increases can promote the iron ion after oxidation to form ferric hydroxide colloid to reach flocculation sedimentation
Effect.
7. the processing method of uranium-containing waste water according to claim 1, which is characterized in that the mode of the separation of solid and liquid is film
Pressure filtration stands 1-2 h.
8. a kind of method using alloy material processing uranium-containing waste water according to claim 1, which is characterized in that in order to more preferable
Ground prepares ferroaluminium, micro sodium borohydride solution can first be added dropwise into pure aluminum particle solution before the mixing of iron aluminium, to go
Except the oxidation film on alumina particles surface.
9. a kind of method of the processing uranium-containing waste water using metal material according to claim 1, which is characterized in that alloy material
Material is preferably ready-to-use, can also be saved under conditions of low temperature oxygen-free, and the uranium-containing waste water after restoring should separate as early as possible, to prevent
Only uranous precipitating is oxidized to sexavalence uranyl ion again.
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Cited By (2)
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| CN110550695A (en) * | 2019-09-29 | 2019-12-10 | 核工业北京地质研究院 | Method for selecting material for treating radioactive uranium-containing wastewater from sandstone-type uranium ores |
| CN117438124A (en) * | 2023-12-22 | 2024-01-23 | 中核第四研究设计工程有限公司 | Method for long-term stable treatment of uranium-containing waste residues |
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Application publication date: 20190607 |