CN109702008A - The method that reducing agent/chelating agent strengthens electro reclamation arsenic chromium combined contamination soil - Google Patents
The method that reducing agent/chelating agent strengthens electro reclamation arsenic chromium combined contamination soil Download PDFInfo
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- CN109702008A CN109702008A CN201811640548.7A CN201811640548A CN109702008A CN 109702008 A CN109702008 A CN 109702008A CN 201811640548 A CN201811640548 A CN 201811640548A CN 109702008 A CN109702008 A CN 109702008A
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Abstract
The invention discloses the methods that a kind of reducing agent/chelating agent strengthens electro reclamation arsenic chromium combined contamination soil, and step: arsenic chromium combined contamination soil is air-dried, pulverized by a., obtains arsenic chromium combined contamination soil powder；B. calcium chloride and Aluminium chloride hexahydrate are stirred evenly, obtains mixed solution；Sodium hydroxide solution is poured into above-mentioned mixed solution while stirring under inflated with nitrogen, layered double-hydroxide solution is made；Then it washs, dries under inflated with nitrogen, grinding obtains layered double-hydroxide powder；C. above-mentioned arsenic chromium combined contamination soil powder and above-mentioned layered double-hydroxide powder are filled between two permeable reactive barriers of electronic-permeable reactive barrier (EK-PRB) prosthetic device, the reducing agents such as ascorbic acid, sodium citrate or complex reagent are added in contaminated soil again, it is powered after standing, reparation terminates.This method can efficiently remove arsenic and chromium in soil, and easy to operate, and at low cost, the period is short, the recyclable regeneration of layered double-hydroxide CaAl-LDH.
Description
Technical field
The present invention relates to a kind of reducing agent/chelating agent reinforcing electronic-permeable reactive barrier (EK-PRB) reparation arsenic-chromium is compound
The method of contaminated soil, belongs to technical field of soil remediation.
Background technique
In recent years, soil pollution situation in China's is increasingly severe." the national Soil Pollution Investigation public affairs of publication in 2014
Report " in point out, heavy metal pollution is extremely serious.Wherein, arsenic pollution point exceeding standard rate is 2.7%, and pollution of chromium point exceeding standard rate is
1.1%.Caused by arsenic chromium combined pollution mainly largely uses the preservative of the chromium containing arsenic as wood preservation industry in soil, often
The reagent of wood preservation and prolonging wood service life is mainly inorganic corrosion inhibitor such as copper chromium arsenic (CCA-C), this kind of anti-corrosion
The use of agent has resulted in the arsenic, chromium, Cu-W ore deposit of some Soils In The Regions and water body.Therefore, repair increasingly diversification, complicate
Heavy metal pollution of soil is extremely urgent.
Currently, electronic joint permeable reactive barrier technology (EK-PRB) can effectively from soil remove chromium, copper, mercury, zinc,
The organic matters such as the heavy metals such as cadmium and lead and phenol, chlorohydrocarbon, petroleum hydrocarbon and acetic acid, joint technology combine the advantage of the two,
PRB active material selectivity is more, can it is more effective, more quickly remove pollutant, save the consumption of the energy, alleviation is increasingly
Serious energy crisis.
Identical as many recovery techniques, electro reclamation can only also remove moveable pollutant in soil.The compound dirt of arsenic chromium
The most of presence in the form of reference state of arsenic in soil is contaminated, dissolution migration is not easy；Chromium exists mostly in the form of soluble state, migration compared with
It is good.Secondly, this substance of iron and manganese oxides/mineral facies is the important component being widely present in upper soll layer, in soil
The presence of the metals such as iron, aluminium, calcium and manganese, be also easy to produce under certain condition it is non-it is obligate absorption and obligate absorption, cause arsenic in soil,
The repairing effect of chromium is poor.Soil is pre-processed therefore, it is necessary to seek a kind of method, make pollutant fixed in soil to
Soluble state pollutant conversion, so that its migration under the conditions of electro reclamation be promoted to remove.Patent document is consulted, with phase of the present invention
What is closed has: entitled " restorative procedure and electronic-microbial association permeable reactive barrier prosthetic device of cadmium, lead-contaminated soil "
(application No. is CN201610474065.9), the device include reactive tank, electrode, power supply and permeable reactive barrier, can at two
Cadmium to be processed, the lead-contaminated soil of filling addition microorganism between permeable reactive wall, to the pollution of electrode transfer from soil
Object is adsorbed by permeable reactive barrier, so that cadmium, lead heavy metal are removed from soil to be processed.It can be seen by the device
Out, PRB can adsorb the fixed pollutant for moving to the two poles of the earth, so that heavy metal is removed from soil, wherein permeable reactive barrier
Electronic pollutant extraction system, more closing to reality are saved with both electric driving method combinations, optimizes electrokinetic system repairing performance.
However, joined microorganism in this method --- Acidithiobacillus thiooxidans realize the activation and extraction of metal ion in soil,
Thallus needs 7 day time to realize the activation of heavy metal after adding, reduce reparation rate, extend repairing efficiency.
Summary of the invention
In view of the deficienciess of the prior art, the purpose of the present invention is to propose to a kind of reducing agent/chelating agents to strengthen electronic repair
The method of multiple arsenic chromium combined contamination soil, this method can promote arsenic chromium electronic by ascorbic acid/sodium citrate/EDTA-2Na
It is dissolved out under the conditions of permeable reactive barrier (EK-PRB) and migrates removal, and is easy to operate, at low cost, the period is short.
To achieve the above object of the invention, the present invention adopts the following technical solutions: a kind of reducing agent/chelating agent strengthens electronic repair
The method of multiple arsenic chromium combined contamination soil, it is characterised in that have process and step below:
A. 500~600g arsenic chromium combined contamination soil is carried out air-dried, pulverized, remove grit and plant residue, cross 20 mesh
Sieve, obtains arsenic chromium combined contamination soil powder, stores for future use；
B. by 4.25~6.00g (50mmol) calcium chloride (CaCl2) and 5.35~6.50g (25mmol) Aluminium chloride hexahydrate
(AlCl3·6H2O it) stirs evenly, obtains mixed solution；Under conditions of inflated with nitrogen, while stirring by the hydroxide of 45~60ml
Sodium (NaOH) solution is poured slowly into above-mentioned mixed solution, stirs 50~75min, is configured to layered double-hydroxide (CaCl2With
AlCl3·6H2O) solution；Then be stirred at room temperature 18~for 24 hours after, then filter, be put into 105 DEG C of baking ovens drying, take out solid-like
Product, then under conditions of inflated with nitrogen, after being washed repeatedly with distilled water, then 105 DEG C of baking oven drying are put into, grinding sieves with 100 mesh sieve,
Obtain layered double-hydroxide (CaCl2And AlCl3·6H2O) powder stores for future use；
C. by the arsenic chromium combined contamination soil powder that above-mentioned steps a is obtained and the double hydroxides of the stratiform that above-mentioned steps b is obtained
Object (CaCl2And AlCl3·6H2O) be filled into electronic-permeable reactive barrier (EK-PRB) prosthetic device two of powder can seep
Between saturating reaction wall, two electrodes are inserted into above-mentioned contaminated soil both ends, then by 500~800ml concentration are 0.01~0.05M
Reducing agent be added in above-mentioned contaminated soil, stand 18~for 24 hours；Direct current is then passed to, voltage of electric field is 20~60V, is protected
24~96h of energization is held, reparation terminates.
Sodium hydroxide solution described in above-mentioned steps b are as follows: (150mmol) sodium hydroxide of 6.4g is dissolved in the steaming of 100ml
The solution of distilled water.
Reducing agent described in above-mentioned steps c is ascorbic acid, sodium citrate and disodium ethylene diamine tetraacetate (EDTA-
One or more of 2Na).
The present invention has the advantages that
The method of the present invention can accelerate the release and migration of arsenic chromium in the soil by the pretreatment of reducing agent and chelating agent,
And arsenic and chromium in soil can efficiently be removed by electronic-permeable reactive barrier (EK-PRB)；Easy to operate, at low cost, the period is short,
The recyclable regeneration of layered double-hydroxide CaAl-LDH.
Detailed description of the invention
Fig. 1 be the embodiment of the present invention one it is electronic-structural schematic diagram of permeable reactive barrier (EK-PRB) prosthetic device；
Fig. 2 is point of the remaining arsenic in the embodiment of the present invention 1 (a) and embodiment 2 (b) after the reparation of arsenic chromium combined contamination soil
Butut；
Fig. 3 is point of the residual chromium in the embodiment of the present invention 1 (a) and embodiment 2 (b) after the reparation of arsenic chromium combined contamination soil
Butut.
Specific embodiment
The present invention is described in further details below with reference to embodiment and attached drawing.
Referring to Fig. 1, electronic-permeable reactive barrier (EK- of a kind of cadmium, As polluted soil that use in the present embodiment
PRB) prosthetic device, the device include DC power supply 1, anode chamber 2, cathode chamber 3, earth pillar room 4, graphite electrode anode 5, graphite electricity
Pole cathode 6 and permeable reaction wall body 7, arsenic chromium combined contamination soil is loaded in earth pillar room 4, and anode chamber 2 and cathode chamber 3 load
Clean soil；Anode chamber 2 and cathode chamber 3 are inserted directly into soil mode using electrode without cathode and anode electrolyte；Earth pillar room 4 is close
Permeable reaction wall body 7 is set at anode chamber 2；7 filler of permeable reaction wall body is layered double-hydroxide；Reduction
Agent is added in the contaminated soil of earth pillar room 4, and standing 18~for 24 hours；The direct current power source voltage of application is 20~60V；The device can
S0 sampling area, 7 right side contaminated soil region of permeable reaction wall body is arranged in 7 left side clean soil region of permeability response wall
The sample region spaced set S1~S6 from left to right.
Embodiment 1
A kind of method that reducing agent/chelating agent strengthens electro reclamation arsenic chromium combined contamination soil, the specific steps of which are as follows:
A. 600g arsenic chromium combined contamination soil is carried out air-dried, pulverized, remove grit and plant residue, crossed 20 meshes, obtain
To arsenic chromium combined contamination soil powder, store for future use；
B. by 5.55g (50mmol) calcium chloride (CaCl2) and 6.04g (25mmol) Aluminium chloride hexahydrate (AlCl3·6H2O)
It stirs evenly, obtains mixed solution；It is while stirring that the sodium hydroxide of 50ml (NaOH) solution is slow under conditions of inflated with nitrogen
Above-mentioned mixed solution is poured into, 60min is stirred, is configured to layered double-hydroxide (CaCl2And AlCl3·6H2O) solution；Then exist
It after stirring 23h at room temperature, then filters, is put into 105 DEG C of baking oven drying, solid sample is taken out, then under conditions of inflated with nitrogen, with steaming
After distilled water is washed repeatedly, then 105 DEG C of baking oven drying are put into, grinding sieves with 100 mesh sieve, obtains 8.1g layered double-hydroxide
(CaCl2And AlCl3·6H2O) powder stores for future use；
C. by the arsenic chromium combined contamination soil powder that above-mentioned steps a is obtained and the double hydroxides of the stratiform that above-mentioned steps b is obtained
Object (CaCl2And AlCl3·6H2O) be filled into electronic-permeable reactive barrier (EK-PRB) prosthetic device two of powder can seep
Between saturating reaction wall, two electrodes are inserted into above-mentioned contaminated soil both ends, then the sodium citrate of 0.05M is configured to 800ml
Reducing agent is added in above-mentioned contaminated soil, is stood for 24 hours；Direct current is then passed to, voltage of electric field 60V remains powered on 96h,
Reparation terminates.
After reaction, two permeable reactive barriers in electronic-permeable reactive barrier (EK-PRB) prosthetic device it
Between Polluted area be divided into the six sampling regions S1~S6, by each region rehabilitating soil take out, be placed in 105 DEG C of drying, grinding.
The content for measuring remaining arsenic and chromium in soil, measures the arsenic in rehabilitating soil, the average removal rate of chromium is respectively 50.5% and
44.0%.From Fig. 2 (a) and Fig. 3 (a) as can be seen that in six sample points of S1~S6, in soil remaining arsenic, chromium account for former arsenic,
Ratio (the C/C of chromium total amount0) it is both less than 1, illustrate to repair above-mentioned arsenic chromium combined contamination soil.
Embodiment 2
The method that the present embodiment 2 repairs arsenic chromium combined contamination soil is same as Example 1, wherein the difference is that: this
Reducing agent described in step c is the combined citric acid 0.05M EDTA-2Na of 0.05M in embodiment 2.After reaction, measurement is repaired
The average removal rate of arsenic, chromium in earth backing earth is respectively 41.2% and 46.8%.From Fig. 2 (b) and Fig. 3 (b) as can be seen that in S1
In six sample points of~S6, remaining arsenic, chromium account for the ratio (C/C of former arsenic, chromium total amount in soil0) it is both less than 1, illustrate to above-mentioned
Arsenic chromium combined contamination soil is repaired.
Claims (3)
1. the method that a kind of reducing agent/chelating agent strengthens electro reclamation arsenic chromium combined contamination soil, which is characterized in that this method tool
Steps are as follows for body:
A. 500~600g arsenic chromium combined contamination soil is carried out air-dried, pulverized, remove grit and plant residue, crossed 20 meshes, obtain
To arsenic chromium combined contamination soil powder, store for future use；
B. by 4.25~6.00g calcium chloride (CaCl2) and 5.35~6.50g Aluminium chloride hexahydrate (AlCl3·6H2O) stirring is equal
It is even, obtain mixed solution；Under conditions of inflated with nitrogen, the sodium hydroxide of 45~60ml (NaOH) solution is slowly fallen while stirring
Enter above-mentioned mixed solution, stirs 50~75min, be configured to layered double-hydroxide (CaCl2And AlCl3·6H2O) solution；Then
Be stirred at room temperature 18~for 24 hours after, then filter, be put into 105 DEG C of baking ovens drying, take out solid sample, then the condition in inflated with nitrogen
Under, after being washed repeatedly with distilled water, then 105 DEG C of baking oven drying are put into, grinding sieves with 100 mesh sieve, obtains layered double-hydroxide
(CaCl2And AlCl3·6H2O) powder stores for future use；
C. by the arsenic chromium combined contamination soil powder that above-mentioned steps a is obtained and the layered double-hydroxide that above-mentioned steps b is obtained
(CaCl2And AlCl3·6H2O) be filled into electronic-permeable reactive barrier (EK-PRB) prosthetic device two of powder are permeable
Between reaction wall, two electrodes are inserted into above-mentioned contaminated soil both ends, then by 500~800ml concentration are 0.01~0.05M's
Reducing agent is added in above-mentioned contaminated soil, and standing 18~for 24 hours；Direct current is then passed to, voltage of electric field is 20~60V, is kept
Be powered 24~96h, and reparation terminates.
2. the method that reducing agent according to claim 1/chelating agent strengthens electro reclamation arsenic chromium combined contamination soil, special
Sign is, sodium hydroxide solution described in above-mentioned steps b are as follows: the sodium hydroxide of 6.4g is dissolved in the solution of the distilled water of 100ml.
3. the method that reducing agent according to claim 1/chelating agent strengthens electro reclamation arsenic chromium combined contamination soil, special
Sign is that reducing agent described in above-mentioned steps c is ascorbic acid, sodium citrate and disodium ethylene diamine tetraacetate (EDTA-2Na)
One of or it is a variety of.
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112170474A (en) * | 2020-09-06 | 2021-01-05 | 桂林理工大学 | Method for repairing arsenic-polluted soil by electrically-driven reinforced permeable reactive barrier |
| CN113182349A (en) * | 2021-06-08 | 2021-07-30 | 福州大学 | Method for restoring chromium-polluted soil by utilizing electro-dynamic coupling permeation reaction wall |
| CN113695380A (en) * | 2021-09-07 | 2021-11-26 | 天津大学 | Electrode system device for repairing soil heavy metal pollutants |
| CN114472495A (en) * | 2022-01-21 | 2022-05-13 | 西安建筑科技大学 | Device and method for electrokinetic remediation of polluted soil by combining chelating agent and permeable reactive barrier |
| CN114534682A (en) * | 2022-03-23 | 2022-05-27 | 福建农林大学 | Composition and method for removing adsorbable organic halides in industrial sludge |
Citations (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104174648A (en) * | 2014-08-21 | 2014-12-03 | 中国科学院生态环境研究中心 | Method for repairing heavy metal polluted soil and special equipment thereof |
| KR101619944B1 (en) * | 2014-02-25 | 2016-05-12 | 한국토양복원기술(주) | Method for remediating contaminated soils by electrokinetic technology |
| CN105880276A (en) * | 2016-06-27 | 2016-08-24 | 上海大学 | Repair method of cadmium and lead polluted soil and electric-microorganism united permeable reaction wall repair device |
| CN106881345A (en) * | 2017-03-14 | 2017-06-23 | 上海大学 | The EK PRB combined remediation methods and its device of heavy metal Cr (VI) contaminated soil |
| CN107012473A (en) * | 2017-04-24 | 2017-08-04 | 北京化工大学 | A kind of double metallic composite material and its preparation method and application |
| CN107030101A (en) * | 2017-03-28 | 2017-08-11 | 上海大学 | A kind of method of utilization microbial association EK PRB restoration of soil polluted by heavy metal |
| CN108326030A (en) * | 2018-01-11 | 2018-07-27 | 上海理工大学 | The heavy metal-polluted soil prosthetic device of convertible array-type electrode |
-
2018
- 2018-12-29 CN CN201811640548.7A patent/CN109702008A/en active Pending
Patent Citations (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| KR101619944B1 (en) * | 2014-02-25 | 2016-05-12 | 한국토양복원기술(주) | Method for remediating contaminated soils by electrokinetic technology |
| CN104174648A (en) * | 2014-08-21 | 2014-12-03 | 中国科学院生态环境研究中心 | Method for repairing heavy metal polluted soil and special equipment thereof |
| CN105880276A (en) * | 2016-06-27 | 2016-08-24 | 上海大学 | Repair method of cadmium and lead polluted soil and electric-microorganism united permeable reaction wall repair device |
| CN106881345A (en) * | 2017-03-14 | 2017-06-23 | 上海大学 | The EK PRB combined remediation methods and its device of heavy metal Cr (VI) contaminated soil |
| CN107030101A (en) * | 2017-03-28 | 2017-08-11 | 上海大学 | A kind of method of utilization microbial association EK PRB restoration of soil polluted by heavy metal |
| CN107012473A (en) * | 2017-04-24 | 2017-08-04 | 北京化工大学 | A kind of double metallic composite material and its preparation method and application |
| CN108326030A (en) * | 2018-01-11 | 2018-07-27 | 上海理工大学 | The heavy metal-polluted soil prosthetic device of convertible array-type electrode |
Non-Patent Citations (1)
| Title |
|---|
| 郭书海，黄殿男等著: "《污染土壤电动修复原理与技术》", 31 December 2017, 中国环境出版社 * |
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112170474A (en) * | 2020-09-06 | 2021-01-05 | 桂林理工大学 | Method for repairing arsenic-polluted soil by electrically-driven reinforced permeable reactive barrier |
| CN113182349A (en) * | 2021-06-08 | 2021-07-30 | 福州大学 | Method for restoring chromium-polluted soil by utilizing electro-dynamic coupling permeation reaction wall |
| CN113695380A (en) * | 2021-09-07 | 2021-11-26 | 天津大学 | Electrode system device for repairing soil heavy metal pollutants |
| CN114472495A (en) * | 2022-01-21 | 2022-05-13 | 西安建筑科技大学 | Device and method for electrokinetic remediation of polluted soil by combining chelating agent and permeable reactive barrier |
| CN114534682A (en) * | 2022-03-23 | 2022-05-27 | 福建农林大学 | Composition and method for removing adsorbable organic halides in industrial sludge |
| CN114534682B (en) * | 2022-03-23 | 2024-04-19 | 福建农林大学 | Composition for removing adsorbable organic halide in industrial sludge and method thereof |
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