CN102910709A - In-situ remediation method for organic contaminated underground water - Google Patents
In-situ remediation method for organic contaminated underground water Download PDFInfo
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- CN102910709A CN102910709A CN2012104303786A CN201210430378A CN102910709A CN 102910709 A CN102910709 A CN 102910709A CN 2012104303786 A CN2012104303786 A CN 2012104303786A CN 201210430378 A CN201210430378 A CN 201210430378A CN 102910709 A CN102910709 A CN 102910709A
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- 238000000034 method Methods 0.000 title claims abstract description 20
- 238000011065 in-situ storage Methods 0.000 title claims abstract description 16
- 238000005067 remediation Methods 0.000 title claims abstract description 13
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 title description 20
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims abstract description 70
- JRKICGRDRMAZLK-UHFFFAOYSA-L peroxydisulfate Chemical compound [O-]S(=O)(=O)OOS([O-])(=O)=O JRKICGRDRMAZLK-UHFFFAOYSA-L 0.000 claims abstract description 47
- 229910052742 iron Inorganic materials 0.000 claims abstract description 30
- 230000000694 effects Effects 0.000 claims abstract description 12
- 239000003673 groundwater Substances 0.000 claims abstract description 11
- CWYNVVGOOAEACU-UHFFFAOYSA-N Fe2+ Chemical compound [Fe+2] CWYNVVGOOAEACU-UHFFFAOYSA-N 0.000 claims abstract description 5
- 230000007935 neutral effect Effects 0.000 claims abstract description 5
- 230000033228 biological regulation Effects 0.000 claims abstract description 4
- 238000005868 electrolysis reaction Methods 0.000 claims abstract description 4
- 230000009257 reactivity Effects 0.000 claims abstract 2
- 230000004913 activation Effects 0.000 claims description 13
- 239000002957 persistent organic pollutant Substances 0.000 claims description 10
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 8
- 230000001105 regulatory effect Effects 0.000 claims description 7
- 230000008439 repair process Effects 0.000 claims description 7
- 239000000243 solution Substances 0.000 claims description 7
- 230000008859 change Effects 0.000 claims description 6
- 238000002347 injection Methods 0.000 claims description 6
- 239000007924 injection Substances 0.000 claims description 6
- 230000010718 Oxidation Activity Effects 0.000 claims description 5
- 239000010936 titanium Substances 0.000 claims description 5
- 229910052719 titanium Inorganic materials 0.000 claims description 5
- LCPVQAHEFVXVKT-UHFFFAOYSA-N 2-(2,4-difluorophenoxy)pyridin-3-amine Chemical compound NC1=CC=CN=C1OC1=CC=C(F)C=C1F LCPVQAHEFVXVKT-UHFFFAOYSA-N 0.000 claims description 4
- CHQMHPLRPQMAMX-UHFFFAOYSA-L sodium persulfate Substances [Na+].[Na+].[O-]S(=O)(=O)OOS([O-])(=O)=O CHQMHPLRPQMAMX-UHFFFAOYSA-L 0.000 claims description 4
- 239000003344 environmental pollutant Substances 0.000 claims description 3
- 238000010525 oxidative degradation reaction Methods 0.000 claims description 3
- 231100000719 pollutant Toxicity 0.000 claims description 3
- 229910001448 ferrous ion Inorganic materials 0.000 claims description 2
- 125000005575 polycyclic aromatic hydrocarbon group Chemical group 0.000 claims description 2
- 239000002904 solvent Substances 0.000 claims description 2
- 150000001555 benzenes Chemical class 0.000 claims 1
- 230000006872 improvement Effects 0.000 claims 1
- 230000002401 inhibitory effect Effects 0.000 claims 1
- 238000009434 installation Methods 0.000 claims 1
- 239000005416 organic matter Substances 0.000 claims 1
- 229910001385 heavy metal Inorganic materials 0.000 abstract description 10
- 230000003647 oxidation Effects 0.000 abstract description 10
- 238000007254 oxidation reaction Methods 0.000 abstract description 10
- 230000005764 inhibitory process Effects 0.000 abstract description 4
- 239000000126 substance Substances 0.000 abstract description 3
- 150000002500 ions Chemical class 0.000 abstract 1
- XSTXAVWGXDQKEL-UHFFFAOYSA-N Trichloroethylene Chemical compound ClC=C(Cl)Cl XSTXAVWGXDQKEL-UHFFFAOYSA-N 0.000 description 16
- 238000001994 activation Methods 0.000 description 14
- 238000011109 contamination Methods 0.000 description 9
- 238000000354 decomposition reaction Methods 0.000 description 5
- 239000011734 sodium Substances 0.000 description 5
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 3
- 230000005540 biological transmission Effects 0.000 description 3
- 238000003895 groundwater pollution Methods 0.000 description 3
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 2
- 239000012190 activator Substances 0.000 description 2
- 239000003513 alkali Substances 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 230000006378 damage Effects 0.000 description 2
- 238000006731 degradation reaction Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 229910052500 inorganic mineral Inorganic materials 0.000 description 2
- 239000011707 mineral Substances 0.000 description 2
- 238000012544 monitoring process Methods 0.000 description 2
- 150000002894 organic compounds Chemical class 0.000 description 2
- 230000037452 priming Effects 0.000 description 2
- 230000008569 process Effects 0.000 description 2
- 238000011084 recovery Methods 0.000 description 2
- 238000007789 sealing Methods 0.000 description 2
- 238000007725 thermal activation Methods 0.000 description 2
- 231100000331 toxic Toxicity 0.000 description 2
- 230000002588 toxic effect Effects 0.000 description 2
- 229910001018 Cast iron Inorganic materials 0.000 description 1
- JPVYNHNXODAKFH-UHFFFAOYSA-N Cu2+ Chemical compound [Cu+2] JPVYNHNXODAKFH-UHFFFAOYSA-N 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 230000003213 activating effect Effects 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- HRYZWHHZPQKTII-UHFFFAOYSA-N chloroethane Chemical compound CCCl HRYZWHHZPQKTII-UHFFFAOYSA-N 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- 229910001431 copper ion Inorganic materials 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 239000003651 drinking water Substances 0.000 description 1
- 235000020188 drinking water Nutrition 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000006053 organic reaction Methods 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 230000000750 progressive effect Effects 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 238000007086 side reaction Methods 0.000 description 1
- 238000004088 simulation Methods 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 238000005728 strengthening Methods 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- 239000003643 water by type Substances 0.000 description 1
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Abstract
本发明涉及一种对有机污染地下水的原位修复方法，具体步骤是向地下水的有机污染区域注入S2O8 2-，将通电的铁电极插入该污染区域中，通过调节铁电极上的电流大小提供二价铁离子Fe(II)，铁电极通正电流时铁电极部分溶解和产生Fe(II)从而活化S2O8 2-；铁电极通负电流时使铁电极处于钝化状态从而抑制甚至终止S2O8 2-的反应活性；当S2O8 2-消耗完毕后，将铁电极作为阳极继续电解提供Fe2/3+和OH-从而提高体系的pH至中性。该方法解决了过硫酸根原位化学氧化修复中过硫酸根活性的原位调控（增强和抑制）和重金属释放难题。
The invention relates to an in-situ restoration method for organically polluted groundwater. The specific steps are: injecting S 2 O 8 2- into the organically polluted area of the groundwater, inserting an energized iron electrode into the polluted area, and adjusting the current on the iron electrode The size provides divalent iron ions Fe(II). When the iron electrode is passed a positive current, the iron electrode is partially dissolved and Fe(II) is generated to activate S 2 O 8 2- ; when the iron electrode is passed a negative current, the iron electrode is in a passivated state so that Inhibit or even terminate the reactivity of S 2 O 8 2- ; when S 2 O 8 2- is consumed, use the iron electrode as the anode to continue electrolysis to provide Fe 2/3+ and OH - to increase the pH of the system to neutral. This method solves the problem of in situ regulation (enhancement and inhibition) of persulfate activity and heavy metal release in persulfate in situ chemical oxidation remediation.
Description
Technical field
The present invention relates to a kind of in-situ remediation method to organic contamination underground water, especially regulate and control persulfate (S by regulating the ferroelectric polarity that extremely goes up and size of current
2O
8 2-) to the oxidation activity of organic pollutant to realize the in-situ remediation method to organic contamination underground water, belong to underground water recovery technique field.
Background technology
Underground water is the drinking water source that is widely adopted, but a lot of urban groundwater polluted in various degree, and wherein the pollution that causes of toxic organic compound such as hydrochloric ether is particularly serious, and total body pollution situation is very severe.In groundwater pollution, the small area contaminated sites underground water take the source pollution as feature is because pollution level is high and harm seriously has been subject to showing great attention to.Therefore repair significant to the contaminated site underground water that caused by toxic organic compound.
The reparation of contaminated site underground water came into one's own in developed country from the eighties in last century, and China still is in the starting stage at present.Because high density feature and the repairing efficiency requirement of contaminated site, in situ chemical oxidation (ISCO) owing to an important recovery technique of repairing fast and implementing conveniently to become in recent years, are thought to repair innovating technologies of " brown ground " by U.S. EPA.Traditional oxygenant mainly comprises H
2O
2, O
3With MnO4 etc., although repairing effect is good, because the loss that the active high side reaction of these oxygenants causes is larger, so that effective rate of utilization is lower.Persulfate (S
2O
8 2-) be a kind of emerging site remediation oxygenant, because its unique oxidation susceptibility is paid attention to rapidly and is used.S
2O
8 2-Although have higher oxidizing potential, itself and organic reaction kinetics process are extremely slow, thereby have preferably stability, and the loss in course of conveying is minimum.S
2O
8 2-Behind overactivation, can produce SO
4 -, have the oxidation capacity suitable with OH.Thereby, S
2O
8 2-The key of oxidation reparation is S
2O
8 2-Activation.
In the site remediation to S
2O
8 2-Activation method commonly used comprise the activation of thermal activation, alkali and Fe (II) activation.Thermal activation needs water temp. heating is arrived comparatively high temps (such as 50
oMore than the C), the alkali activation needs more than the pH regulator to 12, and these two kinds of activation methods have increased rehabilitation cost and difficulty, S
2O
8 2-Also can inevitably occur to decompose before the arrival zone of pollution and cause losing.Comparatively speaking, Fe (II) (containing the chelating attitude) priming reaction condition is more gentle, but the absorption of Fe (II) in transmission course, oxidation, precipitation etc. also can cause damage, greatly reduce effective propagation path, and the Fe (II) of initial injection stage high density also can consume oxygenant.In addition, S
2O
8 2-After priming reaction was complete, the pH of system can be reduced to 2 – 3, caused the release risk of heavy metal in the underground environment.
In present persulfate oxidation is repaired, have following problem: 1. present activation method can only improve the oxidation activity of persulfate, in case just can't regulate active size after persulfate is activated, more can't suppress or eliminate activity, this certainly will cause a large amount of persulfate can't be utilized and be wasted when Pollutant levels are low.2. it is underground that activator mixes rear injection with persulfate solution, can't realize the in-situ activation after persulfate is transferred to Polluted area.The decomposition of persulfate with activator mix after begin immediately, thereby injecting underground and all can causing the decomposition loss of persulfate in the transmission course of underground environment, reduced the utilization ratio of persulfate.3. self decompose the sulfuric acid that produces after the persulfate oxidation and the pH of restoring area underground water can be reduced to 2 – 3, thereby cause that the total heavy metal desorb of underground environment Minerals surface adsorption attitude heavy metal and minerals discharges, and causes the quadratic risk function of underground water acidifying and heavy metal contamination.
Summary of the invention
For overcoming the deficiency of above-mentioned prior art, the invention provides a kind of in-situ remediation method to organic contamination underground water, original position regulation and control (strengthening and inhibition) and heavy metal that the method has solved persulfate activity in the reparation of persulfate in situ chemical oxidation discharge a difficult problem.
Realize that the technical scheme that the object of the invention adopts is to regulate and control persulfate S by regulating the ferroelectric polarity that extremely goes up and size of current
2O
8 2-To realize the original position reparation to organic contamination underground water, concrete grammar is as follows to the oxidation activity of organic pollutant: S is injected in the organic contamination zone to underground water
2O
8 2-, the ferroelectric utmost point of energising is inserted in this Polluted area, provide ferrous ion Fe (II) by regulating the ferroelectric size of current that extremely goes up, the ferroelectric utmost point is partly dissolved and produces Fe (II) thereby activation S during ferroelectric extremely logical positive current
2O
8 2-Thereby make the ferroelectric utmost point be in passive state inhibition even termination S during ferroelectric extremely logical negative current
2O
8 2-Reactive behavior; Work as S
2O
8 2-After being exhausted, the ferroelectric utmost point is continued electrolysis as anode provides Fe
2/3+And OH
-Thereby improve the pH of system to neutral.
Its more specifically step that adopts is:
1., electrode is selected and is installed: use iron staff or iron plate and titanium rod or titanium sheet or titanium net as two electrodes, directly insert the organic contamination zone in the waterbearing stratum, distance between two electrodes is 2 – 30cm, uses wire electrode to be connected to two output terminals of constant voltage dc source;
2., persulfate injection of solution: directly inject Sodium Persulfate solution to Polluted area, make Sodium Persulfate concentration in this Polluted area be 15 times of 3 – of organic contamination substrate concentration in this Polluted area;
3., the persulfate activity regulation with repair to implement: after persulfate is transferred to Polluted area, take iron as anodal and apply the positive current of 10 – 500mA, persulfate is activated, thereby realizes organic oxidative degradation; By regulating the size of positive current, regulate the activation degree of persulfate; When the organic pollutant reparation reaches mass percent 95% when above, changing iron is negative pole and the negative current that applies 50 – 200mA, suppresses even to eliminate persulfate active;
4., the raising of underground water pH value and reparation: after the pollutent decomposition is complete, continuation applies positive current to the ferroelectric utmost point, and raising is applied to ferroelectric current value to the 0.1 – 1A that extremely goes up, the pH variation of monitoring underground water, namely stop energising more than 6.0 when pH brings up to, finish repair process.
The present invention directly inserts the ferroelectric utmost point to the groundwater pollution zone as shown from the above technical solution, and the realization in-situ activation has been avoided the decomposition loss in persulfate injection and the course of conveying; By polarity and the size of current that changes the ferroelectric utmost point, can reach the oxidation activity that strengthens or suppress persulfate, so can regulate targetedly according to Pollutant levels the activity of persulfate, improve the utilization ratio of persulfate; By using iron anode and improving electric current and the prolongation electrolysis time, the pH after the raising reparation is complete avoids the quadratic risk function of underground water acidifying and heavy metal release to neutral.
Compare with existing persulfate activation method, progressive meaning of the present invention is: 1. the activated positions with persulfate changes to the groundwater pollution zone, has reduced the loss in persulfate injection and the transmission course; 2. can regulate flexibly the activity of persulfate, except activating, in repair process, can also suppress even eliminate the activity of persulfate.3. alleviate even avoided the acidifying of underground water after the persulfate oxidation and heavy metal to discharge quadratic risk function.
Description of drawings
Fig. 1 is for applying under the different electric currents influence curve figure to persulfate degraded TCE to the ferroelectric utmost point.
Heavy metal concentration change curve when Fig. 2 is ferroelectric utmost point activation persulfate degraded TCE.
PH value of solution and ORP change curve when Fig. 3 is ferroelectric utmost point activation persulfate degraded TCE.
Embodiment
Embodiment 1:
Simulated groundwater Organic pollutants zone in sealed reactor, trieline (TCE) and the Na of the 52mg/L of adding 410mL in reactor
2S
2O
8, Na
2S
2O
8Concentration is 12.5 times of TCE concentration, (long * wide * high=76 * 9.5 * 3.2mm) and titanium net (length * wide * height=85 * 15 * 1.8 mm) serve as two electrodes to insert iron plate, distance between two electrodes is 2 – 30cm, use wire electrode to be connected to two output terminals of constant voltage dc source, after the sealing take iron plate as anodal and apply the positive current of 50mA, persulfate is activated, thereby realize organic oxidative degradation, current value can be regulated between 10 – 500mA in the degradation process, when the organic pollutant reparation reaches 95% mass percent, changing iron is negative pole and the negative current that applies 50mA, suppress persulfate active, current value can be regulated between 50 – 200mA in the process of inhibition, after the pollutent decomposition is complete, continue to apply the 100mA positive current to the ferroelectric utmost point, the pH of monitoring underground water changes, namely stop energising more than 6.0 when pH brings up to, finish repair process.
Comparison embodiment 1:
In sealed reactor simulation Organic pollutants waters, in container, add trieline (TCE) and the Na of the 52mg/L of 410mL
2S
2O
8, Na
2S
2O
8Concentration is 12.5 times of TCE concentration, (long * wide * high=76 * 9.5 * 3.2mm) and titanium net (length * wide * height=85 * 15 * 1.8 mm) serve as two electrodes to insert the cast iron sheet, change is applied to the ferroelectric polarity of electrode of extremely going up and size of current after the sealing, and the removal effect of TCE as shown in Figure 1.Clearly, the degradation effect of TCE accelerates with the increase of positive current, is suppressed more significantly with the increase of negative current, reach when applying negative current-degraded of TCE is almost suppressed fully during 50mA.
Comparison embodiment 2:
Use identical reactor, in another group test, reduce Na
2S
2O
8Concentration, for TCE concentration 4 times are continuously applied+100mA to the ferroelectric utmost point.Experimental result as shown in Figure 2, as shown in Figure 2, TCE and persulfate concentration changes with time and significantly reduce, TCE is by degradable behind the 30min, continuation applies+the 100mA electric current to the ferroelectric utmost point, and persulfate concentration concentration continues to reduce, and 50min begins free state heavy metal copper ion (Cu
2+) concentration begins remarkable reduction.PH and the redox potential (ORP) corresponding by Fig. 3 change as can be known, and the pH of the aqueous solution begins remarkable increase during 50min, and reaches neutral range when 90min.
Can use other material in chlorinated solvent, benzene homologues and the polycyclic aromatic hydrocarbons to replace the pollutent TCE in above-described embodiment, can obtain similar experimental result equally.
Claims (3)
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|---|---|---|---|
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|---|---|---|---|
| CN201210430378.6A CN102910709B (en) | 2012-11-01 | 2012-11-01 | In-situ remediation method for organic contaminated underground water |
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| CN102910709A true CN102910709A (en) | 2013-02-06 |
| CN102910709B CN102910709B (en) | 2014-06-04 |
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Cited By (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103342410A (en) * | 2013-07-25 | 2013-10-09 | 中山大学 | Water treatment method for removing arsenic by strengthening zero-valent iron |
| CN103342405A (en) * | 2013-07-23 | 2013-10-09 | 哈尔滨工业大学 | Method for degrading organic pollutants in water through electrochemical cathodic activation of persulfate |
| CN105347445A (en) * | 2015-12-10 | 2016-02-24 | 湖南大学 | Method for removing micropollutants in water by activating peroxysulphate through iron electrode |
| CN109019822A (en) * | 2018-08-07 | 2018-12-18 | 北京伦至环境科技有限公司 | A kind of Organic Chemicals In Groundwater in-situ remediation method |
| CN109110955A (en) * | 2018-08-17 | 2019-01-01 | 中国石油天然气集团有限公司 | A kind of wastewater treatment method |
| CN110918632A (en) * | 2019-09-20 | 2020-03-27 | 河北工业大学 | Method for restoring organic contaminated soil by using electrothermal activated persulfate |
| CN113683163A (en) * | 2021-09-01 | 2021-11-23 | 营口理工学院 | Treatment device for degrading dye wastewater by periodically reversing electrochemistry in cooperation with persulfate and use method thereof |
| CN114127018A (en) * | 2019-06-19 | 2022-03-01 | 懿华水处理技术有限责任公司 | Electrochemically activated persulfates for advanced oxidation processes |
| CN114314796A (en) * | 2021-12-29 | 2022-04-12 | 北京师范大学 | Material with double functions of activating persulfate and solubilizing chlorohydrocarbon |
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Cited By (10)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103342405A (en) * | 2013-07-23 | 2013-10-09 | 哈尔滨工业大学 | Method for degrading organic pollutants in water through electrochemical cathodic activation of persulfate |
| CN103342410A (en) * | 2013-07-25 | 2013-10-09 | 中山大学 | Water treatment method for removing arsenic by strengthening zero-valent iron |
| CN103342410B (en) * | 2013-07-25 | 2015-03-25 | 中山大学 | Water treatment method for removing arsenic by strengthening zero-valent iron |
| CN105347445A (en) * | 2015-12-10 | 2016-02-24 | 湖南大学 | Method for removing micropollutants in water by activating peroxysulphate through iron electrode |
| CN109019822A (en) * | 2018-08-07 | 2018-12-18 | 北京伦至环境科技有限公司 | A kind of Organic Chemicals In Groundwater in-situ remediation method |
| CN109110955A (en) * | 2018-08-17 | 2019-01-01 | 中国石油天然气集团有限公司 | A kind of wastewater treatment method |
| CN114127018A (en) * | 2019-06-19 | 2022-03-01 | 懿华水处理技术有限责任公司 | Electrochemically activated persulfates for advanced oxidation processes |
| CN110918632A (en) * | 2019-09-20 | 2020-03-27 | 河北工业大学 | Method for restoring organic contaminated soil by using electrothermal activated persulfate |
| CN113683163A (en) * | 2021-09-01 | 2021-11-23 | 营口理工学院 | Treatment device for degrading dye wastewater by periodically reversing electrochemistry in cooperation with persulfate and use method thereof |
| CN114314796A (en) * | 2021-12-29 | 2022-04-12 | 北京师范大学 | Material with double functions of activating persulfate and solubilizing chlorohydrocarbon |
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