CN100998987A - Electric restoring method of polluted soil and underground water - Google Patents
Electric restoring method of polluted soil and underground water Download PDFInfo
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- CN100998987A CN100998987A CN 200610037747 CN200610037747A CN100998987A CN 100998987 A CN100998987 A CN 100998987A CN 200610037747 CN200610037747 CN 200610037747 CN 200610037747 A CN200610037747 A CN 200610037747A CN 100998987 A CN100998987 A CN 100998987A
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- soil
- phreatic
- electric
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Abstract
An electric repairing method for the polluted soil and underground water includes such steps as arranging the positive electrodes and negative electrodes at both ends of a polluted region, adding the electrically conductive buffering liquid in the area between said negative electrode and polluted region to form an electric conductive area for controlling pH value, and applying a voltage across said positive and negative electrodes.
Description
Technical field
The present invention relates to the soil of contaminated soil and phreatic electric repair method, especially heavy metal pollution and the new method that underground water carries out electronic reparation.
Background technology
The present invention relates to the soil of heavy metal pollution and the new method that underground water carries out electronic reparation (EK): the basic principle that the soil of heavy metal pollution and underground water carry out electronic reparation all is to apply low DC current (mA.cm between two electrodes in inserting contaminated soil and underground water
-2) or DC voltage (V.cm
-1), utilizing the underground water in the soil aperture or add electrolyte solution as conducting medium, pollutant and other charged ion are moved by soil and underground water in the mode of electromigration and EOF in solution conductivity.(1) pollutant of arrival electrode district generally removes the heavy metal and the water-soluble good organic matter of deionization attitude by electro-deposition or ion-exchange extraction; (2), study and developed multiple enhancing restorative procedure for the efficient that improves electrokinetic process and the range of application of electrokinetic technique; (3) latest developments the coupling of some electrokinetic techniques and other method, for example electrically and biologically method, EK-Fenton process.
The initiator of contaminated soil and underground water electric repairing technique is American scholar Acar, the device of initial electronic reparation experimental provision that proposes and soil and underground water dehydration is similar, plugs electrode by electric osmose and electromigration depollution thing in contaminated soil and underground water solution.This simple mechanism mainly contains two big shortcomings: can not control soil and groundwater regime pH in (1) experimentation and change, treatment effeciency is low; (2) can not handle insoluble metal form and hydrophobic organic compound.The oxidized generation of the water of anode region H
+, pH reduces to 2; The water in cathodic region is reduced and generates OH
-, pH rises to 10, passes soil and phreatic H
+OH with the negative electrode generation
-In a narrow zone and generate water, pH in this zone from 2 hops to 10.Adopt the method do not strengthen condition to carry out the amplification test that lead contamination kaolin is repaired, they find after repair time of 123 days, and only 54% lead arrives in the soil and underground water of negative electrode 10cm (electrode spacing 72.4cm), and remediation efficiency is very low.In order to improve treatment effeciency, scholars have improved initial device, have proposed multiple effective enhancing restorative procedure.
The main feature of electroosmose process electrokinetic process is to separate with amberplex respectively between two electrode districts and soil and underground water, after galvanization, since the existence of amberplex, H
+And OH
-All can not enter soil and groundwater regime, reach and kept soil and the stable purpose of underground water pH.But electrodialysis plant makes up more complicated, cost height.Cation-exchange membrane and anion-exchange membrane are respectively CationCR67HMR412 and Anion 204SXZL386 in the experiment, and conducting solution is the 0.01MNaNO that adjusts to pH=4 with nitric acid
3Handle the Danish Loamy Sand that copper pollutes with this device, after 70 days repair time in soil and the underground water copper content reduce to 40mg/kg by 1360mg/kg.
Electronic repairing method of the contaminated soil of prior art and underground water or complexity, cost height, perhaps effect is slightly poor.
Summary of the invention
The objective of the invention is to propose a kind of new contaminated soil and the electronic repairing method of underground water, its cost is low and effective.And to adopt reactive metal be anode, efficiently repairs contaminated soil and underground water.
The present invention seeks to realize like this: contaminated soil and phreatic electric repair method, (1) is provided with positive and negative electrode at contaminated soil and phreatic regional two ends, the formation conductive region that between negative electrode and soil and underground water, keeps the adding conductie buffer solution of a segment distance, the length 10-30cm of conductive region, the zone that is used for the pH in control electrode district hinders the OH that negative electrode produces
-Soil and groundwater province be can not enter, soil and phreatic low pH condition kept.Electric-force gradient is 1-5V/cm, and especially 1-1.5V/cm is good; (2) selected silver electrode, the ferroelectric utmost point and aluminium electrode as anode, especially the aluminium sheet electrode has been obtained good effect; (3) area of electrode is also very important: under identical electrolytic condition, the current density of broad-area electrode system is less than the small size electrode system, and along with the rising of decomposition voltage, this trend gets over obviously.So when actual electrical is repaired, should select big surface electrode for use as far as possible, plate electrode preferably, the life-span of working electrode can be enhanced like this.
The present invention especially anode electrode uses silver electrode, aluminium sheet electrode or iron staff electrode.Cathode electrode material is selected graphite cake.
Mechanism of the present invention is: when direct current is applied on saturated soil and the underground water, cause water in anode generation oxidation reaction, generate sour face; And, generate alkali face (2H in negative electrode generation reduction reaction
2O-4e
-=O
2↑+4H
+(anode), 2H
2O+2e
-=H
2↑+2OH
-(negative electrode)).The acid that anode generates advances towards negative electrode, and the alkali face of negative electrode generation simultaneously also anode advances.Because hydrionic mobility has surpassed the mobility of hydroxide ion, and the direction of EOF is to negative electrode, so the speed that acid advances towards negative electrode will be far away faster than the alkali face, but the OH that cation selective membrane stops cathode reaction to generate
-In soil and underground water, move the pH condition that maintenance system is appropriate.And use active metal to do anode such as iron, hydrogen ion and iron reaction have been consumed, and are not very greatly so the pH of solution changes.
For some weakly alkaline metals, different pH conditions have different forms.Some amphoteric metals exist with cation or anion form, for example pb according to condition of different pH
2+/ [PbO
2H]
-, Cr
3+/ [Cr (OH)
4]
-, Zn
2+/ ZnO
2 2-, under acid condition, have (Zn with the metal cation form
2+), but under alkali condition, there is (ZnO with the metallate ion
2 2-), in the solubility minimum of pH step place metal ion, they are with the form precipitation of hydroxide.
Characteristics of the present invention are: by selecting appropriate electrode material, shape and area size, control the current potential of electric field, the employing reactive metal is an anode, efficiently repairs contaminated soil and underground water.The pH scope in control electrode district hinders the OH that negative electrode produces
-Soil and groundwater province be can not enter, soil and phreatic low pH condition kept.Cost is low and effective.
Description of drawings
Fig. 1 is broad-area electrode of the present invention and small size electrode voltage current curve schematic diagram
Fig. 2 is a silver electrode electrode voltage current curve schematic diagram of the present invention
Fig. 3,4 is respectively graphite electrode material decomposition voltage of the present invention and electrode potential and decomposition voltage and current curve
The specific embodiment
The current density of different electrode areas is relatively: when the current density of electrode surface was big, a large amount of bubbles that form on electrode surface often were suspended in the electrolyte and the solution resistance between the cathode and anode are enlarged markedly.So be necessary research under identical electrolysis and electrode material condition, the relation of electrode area and current density.
Contrast the K of large and small electrolysis 40mmol/L
2SO
4Solution:
The small size electrode is (less than 20cm
2, down together): solution parameter is initial conductivity=8450 μ S/cm, initial pH=5.61; Final electrical conductivity=8360 μ S/cm, final pH=4.65;
Broad-area electrode is (greater than 100cm
2, down together): solution parameter is initial conductivity=8450 μ S/cm, initial pH=5.61; Final electrical conductivity=8360 μ S/cm, final pH=4.54.
Current density is power taking stream and electrode area ratio (mA/cm
2).Observing the negative electrode bubble will be far away more than anode, and the about 0.1mm of negative electrode bubble diameter, and anode is thinner.From the result, under identical electrolytic condition, the current density of broad-area electrode system is less than the small size electrode system, and along with the rising of decomposition voltage, this trend gets over obviously.So when actual electrical is repaired, should select the large electrode surface electrode for use as far as possible, plate electrode preferably, the life-span of working electrode can be enhanced like this.It is shown in Figure 1.
Anode material is selected
1. silver is as anode, and electrolysis 50mmol/LNaCl solution, electrode material are silver rod (anode) and tungsten bars (negative electrode), electrode shape: φ 1.6 * 9cm, electrode spacing 7cm.
Silver electrode surface is oxidized in the experiment, the coarse injustice that original smooth surface becomes.Experimental result as shown in Figure 2, the trend of this curve is different with the front graphite electrode, it is in disorder that electric current changes, and infers that silver electrode is the oxidized (Ag-e of beginning below 2.5V
-→ Ag
+, E
0=-0.7991V) increased the ionic strength of solution, makes that electrical conductivity of solution continues to rise.When applied voltage 10V, electric current increases sharply, estimation be silver electrode under this electrolytic potential by complete oxidation.
2. (area of selecting for use in the practicality is at 10-50cm for the aluminium sheet electrode
2, also can be chosen in 100-1000cm by aluminium sheet electrode area electrode
2) as anode, graphite electrode is as negative electrode, electrolysis 80mmol/L NaNO
3The black flocculent deposit appears in solution in the solution.This mainly is because graphite rod flakes off into fine particle in the solution, the dissolved aluminium ion (Al-3e that goes out
-→ Al
3+, E
0The flocculating setting of=-1.662V).Al (OH)
3Colloidal sol is positive electrosol, and soil and underground water surface are electronegative.So can use active metal aluminium as anode, make Nano sol and be coated on soil and underground water particle surface, make cationic soil and underground water particle, resolve the metal ion on soil and underground water surface, improve electronic remediation efficiency.
3. 8mm iron staff electrode is as anode, and observing solution in the experiment does not have obvious change color, but yellow spotting has appearred in electrode surface, illustrates that electrode surface is oxidized.Under acid condition, Fe (II) is by reaction Cr
2O
7 2-+ 14H
++ Fe
2+→ 2Cr
3++ Fe
3++ 7H
2O reduces Cr (VI).
Cathode material is selected
Negative electrode generation reduction reaction, the reduction reaction of water are (2H
2O+2e
-→ H
2↑+2OH
-, E
0=-0.83V).If the same with anode, suppress the reaction of water with the reaction of other ion, the reaction potential that just requires other ion can use the graphite cathode material than-0.828V height, also can adopt carbon-point or tungsten bar.
Handle the result of several typical pollutants:
The electronic reparation of the present invention mainly is at heavy-metal contaminated soil and underground water, needs therefore to consider whether heavy metal can bring new pollution to environment after electrode reaction.Choose Cu (II), Pb (II) and Cr several typical heavy metals such as (III) as the simulating pollution thing,
Handle electrolysis CuSO
4Solution parameter: initial pH=4.78, initial conductivity=2750 μ S/cm.
Electrode parameter: electrode material: graphite; Shape: 6 * 57mm; Electrode spacing: 17cm.
Mainly investigate the electrolysis under the appropriate voltage condition, therefore directly voltage is set to 8.3V, and being converted to electric-force gradient is 1.2V/cm.
Generate the black floccule in the solution and be suspended in electrode surface, shape is as coral reef, drive away the suspension of electrode surface behind the experiment 1h with glass bar, find that electrode surface has covered one deck light, dark red copper (this phenomenon be in the document not report), this moment, cathode surface had intensive bubble, finished experiment behind the 3h.
Location parameter is as follows: E
Decompose=8.3V, electric current=102mA, current density=10.40mA/cm
2, anode pH=3.03, negative electrode pH=2.26-2.43.Cathode reaction mechanism to Cu (II) is inferred as follows: Cu
2++ e
-→ Cu
+, E
0=+0.153V (1); Cu
++ e
-→ Cu, E
0=+0.512V (2).The reason that pH descends in the solution mainly is that cathode reaction is separated out based on Cu, and anode has OH
-Oxidized, OH
-Concentration reduces, so pH reduces.Calculate 20mmol/LCuSO
4Cathode reaction and reaction potential during electrolysis:
The possible reaction of negative electrode water and Cu (II) is: 2H
2O+2e
-→ H
2↑+2OH
-
0=-0.828V
Cu
2++2e
-→Cu↓
0＝0.337V
Determining of the various ion electrode reaction potentials of negative electrode:
H
2Separating out overpotential on graphite electrode is 1.1V
Cu (S) separates out overpotential 0.23V on graphite electrode
The theoretical deposition potential of Cu:
Elutriation goes out H
2The time reduction potential:
Cu＞
H2So Cu has precedence over H
2Separate out
Electrolysis Pb (NO
3)
2Solution
Solution parameter: initial pH=4.70, initial conductivity=4050 μ S/cm; Final pH=1.66, final electrical conductivity=9720 μ S/cm.Electrode parameter: electrode material, graphite, shape: 6 * 60mm, electrode distance: 27cm.
Record electrode potential and electric current such as Fig. 3,4.After decomposition voltage surpassed 5V, negative electrode became coralliform, the about 1cm of its cotton-shaped diameter, and the sediment of electrolytic cell bottom adularescent light has graphite to peel off near the anode.Report is handled Pb contaminated soil and underground water with graphite electrode in forefathers' the document, and this experimental phenomena is not all had report.Document says that the Pb of anode region forms anion, and the Pb in cathodic region forms cation, and anionic complex compound is PbSO
4
Electrolysis CrCl
3Solution
Solution parameter: initial pH=2.9, initial conductivity=5890 μ S/cm
Electrode parameter: material: graphite; Electrode shape: 6 * 60mm; Electrode spacing: 32cm
Decomposition voltage and current data see Table 2.
Table 2 electrolysis CrCl
3Experimental record
| Decomposition voltage (V) | 1.02 | 1.96 | 3.02 | 4.01 | 5.01 | 6.04 | 7.08 | 8.07 |
| Electric current (mA) | 0.3 | 5.3 | 18.65 | 42.28 | 67.45 | 21.34 | 23.5 | 29.2 |
This group experiment is different with preceding two groups of experimental phenomenas, mainly shows:
(1). do not produce any attachment at negative electrode, can't see precipitation in the solution, but anode adheres to the yellowish-brown precipitation, this layer attachment is very fine and close.
(2). solution is by the yellowish-brown of testing after preceding navy blue changes experiment into, and upward lower leaf, and the upper strata is based on navy blue, and lower floor is based on yellowish-brown.
(3). from the data of table 2, electric current changes from small to big (during E=6V), after diminish again, electrical conductivity, the pH of solution do not have significant change.
From three groups of top experiments, we can draw to draw a conclusion: (1). and most metal ions can both be reduced at negative electrode, are plated in electrode surface; (2). some heavy metal is not suitable for using electric repair method, and for example Cr (III) can be changed into the Cr (VI) of severe toxicity in anodic oxygen.
By above experiment and calculating, the present invention has studied the electrode reaction of representative heavy metal pollutant can be used for improving one's methods of electronic reparation, and to heavy-metal contaminated soil and phreatic reparation, by electrode reaction deposition and separating beavy metal.
In the electronic repair process, electrode also is to consume electromotive force, and is a fixed value for the process of concrete work.Electrode spacing can not be too short, because electrode spacing has been lacked, the proportion of the total decomposition voltage of electrode potential consumption will increase, but can not be oversize, repair time can be prolonged like this, soil of the present invention and underground water spacing 30-60cm (distance between electrodes) are proper, and this moment, electrode potential accounted for total electric field about 20%.When reality is used, should select the big electrode of electrode area for use as far as possible, preferably plate electrode can reduce electrode current density like this, increases the service life.Electronic reparation will avoid electrode reaction to bring secondary pollution as far as possible.
Carbon electrode also is the desirable scheme of cathode electrode, mainly is because the relative precious metal electrode of graphite is very cheap and chemical property is also more stable; Use the active metal electrode instead at anode, with the way inhibition H of sacrificial anode
+Generation, pH that like this can the hierarchy of control.What anode took place is oxidation reaction, most metals all can be oxidized, we have selected silver electrode, the ferroelectric utmost point and aluminium as anode, especially the aluminium sheet electrode is as the advantage and the condition of anode: as area big or small the electrolysis process condition, use active metal aluminium as anode, make Nano sol and be coated on soil and underground water particle surface, improve electronic remediation efficiency.Infer Al (OH)
3Application in soil and the electronic reparation of underground water can become the focus that electricity is repaired research. 8mm iron staff electrode is as anode, and observing solution does not have obvious change color, but yellow spot has appearred in electrode surface, illustrates that electrode surface is oxidized.Under acid condition, Fe (II) is by reaction Cr
2O
7 2-+ 14H
++ Fe
2+→ 2Cr
3++ Fe
3++ 7H
2O reduces Cr (VI).
Claims (6)
1, contaminated soil and phreatic electric repair method are provided with positive and negative electrode at contaminated soil and phreatic regional two ends, it is characterized in that electrode spacing 30-60cm in contaminated soil and underground water; And the zone that the formation of the adding conductie buffer solution of maintenance one segment distance is conducted electricity between negative electrode and soil and underground water, the length 10-30cm of conductive region, soil and phreatic low pH condition are kept in the zone that is used for the pH in control electrode district, and electric-force gradient is 1-5V/cm.
2,, it is characterized in that anode electrode uses silver electrode, aluminium sheet electrode or iron staff electrode by described contaminated soil of claim 1 and phreatic electric repair method.
3,, it is characterized in that cathode electrode material selection graphite cake by claim 1 or 2 described contaminated soils and phreatic electric repair method.
4,, it is characterized in that aluminium sheet electrode area electrode 100-1000cm by claim 1 or 2 described contaminated soils and phreatic electric repair method
2
5,, it is characterized in that electric-force gradient is 1-1.5V/cm by claim 1 or 2 described contaminated soils and phreatic electric repair method.
6, by claim 1 or 2 described contaminated soils and phreatic electric repair method, it is characterized in that adopting plate electrode.
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|---|---|---|---|
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|---|---|---|---|
| CNB200610037747XA CN100464878C (en) | 2006-01-13 | 2006-01-13 | Electric restoring method of polluted soil and underground water |
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| Publication Number | Publication Date |
|---|---|
| CN100998987A true CN100998987A (en) | 2007-07-18 |
| CN100464878C CN100464878C (en) | 2009-03-04 |
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102259111A (en) * | 2011-04-01 | 2011-11-30 | 重庆大学 | Method for protecting soil and underground water from electromotive repairing focusing |
| CN102527707A (en) * | 2012-02-24 | 2012-07-04 | 上海市环境科学研究院 | Enhanced electrokinetic remediation method of heavy metal contaminated soil |
| CN103232096A (en) * | 2013-04-26 | 2013-08-07 | 清华大学 | In-situ repairing system and repairing method capable of continuously removing Cr in underground water |
| CN103341485A (en) * | 2013-06-04 | 2013-10-09 | 孔亦周 | Electrodynamic force method electrodes for adsorption of soil pollutants by pitch-based spherical activated carbon |
| CN106269840A (en) * | 2016-08-29 | 2017-01-04 | 付融冰 | A kind of electrode restorative procedure of contaminated soil or subsoil water |
| CN108435781A (en) * | 2018-03-23 | 2018-08-24 | 李延顺 | A kind of automatic detection process equipment of heavy metal for soil remediation |
Family Cites Families (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1695834A (en) * | 2005-06-09 | 2005-11-16 | 上海交通大学 | Method of electrodynamics for restoring soil polluted by heavy metal |
| CN1325179C (en) * | 2005-06-09 | 2007-07-11 | 上海交通大学 | Method of electrodynamics for quick restoring soil polluted by heavy metal in situ |
-
2006
- 2006-01-13 CN CNB200610037747XA patent/CN100464878C/en not_active Expired - Fee Related
Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102259111A (en) * | 2011-04-01 | 2011-11-30 | 重庆大学 | Method for protecting soil and underground water from electromotive repairing focusing |
| CN102527707A (en) * | 2012-02-24 | 2012-07-04 | 上海市环境科学研究院 | Enhanced electrokinetic remediation method of heavy metal contaminated soil |
| CN103232096A (en) * | 2013-04-26 | 2013-08-07 | 清华大学 | In-situ repairing system and repairing method capable of continuously removing Cr in underground water |
| CN103232096B (en) * | 2013-04-26 | 2014-07-23 | 清华大学 | In-situ repairing system and repairing method capable of continuously removing Cr in underground water |
| CN103341485A (en) * | 2013-06-04 | 2013-10-09 | 孔亦周 | Electrodynamic force method electrodes for adsorption of soil pollutants by pitch-based spherical activated carbon |
| CN106269840A (en) * | 2016-08-29 | 2017-01-04 | 付融冰 | A kind of electrode restorative procedure of contaminated soil or subsoil water |
| CN108435781A (en) * | 2018-03-23 | 2018-08-24 | 李延顺 | A kind of automatic detection process equipment of heavy metal for soil remediation |
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|---|---|
| CN100464878C (en) | 2009-03-04 |
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