CN104445570A - Method for removing polycyclic aromatic hydrocarbon methylnaphthalene substance by adopting double oxidants including persulfate and calcium peroxide - Google Patents
Method for removing polycyclic aromatic hydrocarbon methylnaphthalene substance by adopting double oxidants including persulfate and calcium peroxide Download PDFInfo
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- CN104445570A CN104445570A CN201410561933.8A CN201410561933A CN104445570A CN 104445570 A CN104445570 A CN 104445570A CN 201410561933 A CN201410561933 A CN 201410561933A CN 104445570 A CN104445570 A CN 104445570A
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- methylnaphthalene
- calcium peroxide
- persulphate
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
- C02F1/722—Oxidation by peroxides
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/32—Hydrocarbons, e.g. oil
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
- C02F2103/06—Contaminated groundwater or leachate
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2209/00—Controlling or monitoring parameters in water treatment
- C02F2209/06—Controlling or monitoring parameters in water treatment pH
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/02—Specific form of oxidant
- C02F2305/023—Reactive oxygen species, singlet oxygen, OH radical
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- Hydrology & Water Resources (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
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Abstract
The invention relates to a method for removing a polycyclic aromatic hydrocarbon methylnaphthalene substance by adopting double oxidants including persulfate and calcium peroxide. The method comprises the steps of adding persulfate and calcium peroxide into a water body containing methylnaphthalene, stirring uniformly, and reacting for 4-5 days under the condition that the pH of the system is neutral and weakly acidic, thus removing the pollutant by oxidization. The double oxidants are added into the water, and free hydroxy and sulfate radicals are generated to attack the pollutant, so that the pollutant is effectively degraded. The double oxidants including persulfate and calcium peroxide can simultaneously generate free hydroxy and sulfate radicals with extremely strong oxidation, so that the acting pollutant range is wider than that of a traditional method, and the pollutant sensitive to the free hydroxy and sulfate radicals can be simultaneously removed. The acting time is long, the applicable pH range is wide, a promotion effect on microbes in the environment is achieved, the bioremediation efficiency of microbes in environmental media can be improved, and then the repair efficiency of a polluted area is improved. The method is applicable in the field of polluted underground water repair.
Description
Technical field
The present invention relates to a kind of method removing Organic Pollutants In Water, especially relate to a kind of groundwater remediation field and utilize persulphate-calcium peroxide dual oxidants to remove the method for multiring aromatic hydrocarbon substance methylnaphthalene.
Background technology
Polycyclic aromatic hydrocarbons (PAHs) typically refers to the general name of the various organic compound derived by two or more phenyl ring and they
[1].The PAHs of usual visible high density in petroleum-polluted region.Due to carcinogenic, teratogenesis, mutagenesis " three cause " toxicity that it is potential, and by biological accumulation and food chain transmission, threaten human health, all bring great harm to natural biology and ecotope.The restorative procedure of common PAHs mainly contains biological restoration, phytoremediation, chemical redemption etc., other several repair modes relatively, chemical oxidation is shorter on treatment cycle, cost is lower, little to the destruction of environment, and processing for being generally difficult to the treatment effect that organic chemical contaminant oxidation has more efficient stable.Based on the limitation of traditional ground water chemistry recovery technique, in situ chemical oxidation (in situ chemical oxidation, ISCO) technology is being subjected to increasing concern by the groundwater remediation of PAHs class Substances Pollution.
In situ chemical oxidation is a kind of organic pollutant utilizing strong oxidizer to degrade in underground water or soil, and the compound recovery technique of environmental sound.ISCO is subject to extensive concern with its high efficiency to Pollutant Treatment and the promoter action to biological restoration.It can effectively be repaired by petroleum hydrocarbon, polycyclic aromatic hydrocarbons organic pollutant contaminated soil and underground water.Oxygenant conventional in existing ISCO comprises permanganate (MnO
4 -), hydrogen peroxide (H
2o
2), persulphate (S
2o
8 2-) and calcium peroxide (CaO
2).Permanganate has the longer transformation period in neutral conditions, and it can keep longer action time in soil and underground are repaired.But for permanganate, the Optimal pH condition that its oxidisability plays is below 3 or more than 10
[2], the pH condition of the neutral meta-alkalescence of soil and underground water is also unfavorable for giving full play to of its oxidisability.Hydrogen peroxide has in ISCO to be applied comparatively widely, and hydrogen peroxide can activate and produce oxidisability extremely strong hydroxyl radical free radical (OH, E
0=1.8 ~ 2.7V), and then oxidation removal organic pollutant effectively.But hydrogen peroxide is also unstable in surrounding medium, is easy in neutral conditions disproportionation reaction occurs, generates O
2.This part invalid O
2generation, reduce H
2o
2produce the efficiency of OH, and then affect the remediation efficiency in practical application.Research in recent years shows that persulphate and calcium peroxide are the effective oxygenants of two classes in ISCO.Persulphate can effectively be degraded methyl tertiary butyl ether, petroleum hydrocarbon class pollutant matter, calcium peroxide also show great validity on removal trotyl, multiring aromatic hydrocarbon substance, and this two classes oxygenant has broad application prospects in groundwater remediation field.
Persulphate is the oxygenant that a class oxidisability is stronger, and its standard oxidationreduction potential is 2.01V.Persulphate ionizes and produces S in water
2o
8 2-, under certain activation ,-O-O-the bond rupture in persulphate, can produce the potentiometric titrations (SO that oxidisability is stronger
4 -, E
0=2.5 ~ 3.1V).Although OH is oxygenant that a class oxidisability is very strong but lifetime is short in aqueous for it, be less than 1 μ s
[3], the pollutent OH special to some structure then loses effective degradation capability (as: perfluorocarboxylic acid).SO
4 -have stronger selectivity to pollutent, the pH that its oxidation activity adapts to is wider general, SO
4 -good stability in the environment, its transformation period at about 4s, much larger than OH.The water-soluble height of persulfuric acid salts substances, as Sodium Persulfate solubleness in water can reach 73g/100g(25 DEG C), and commercially available low price, relative hydrogen peroxide, the persulphate of solid is more convenient for transporting in practical engineering application.Persulphate and product S O thereof
4 2-affect little on indigenous microorganism group in surrounding medium, thus also comparatively faint on the biological restoration impact dominated by these microorganisms
[4].Persulphate is good stability in underground environment, and Absorbable organic halogens exists several weeks
[3], its stability is much larger than H
2o
2, be conducive to the mass transfer process in actual repair application.Usually, persulphate activates generation potentiometric titrations by heating, UV illumination or this several mode of transition metal ion.
Calcium peroxide has the environmental friendliness shaped material of oxygen release and oxidisability concurrently as a class, is not only widely used in agricultural planting, aquaculture, food and medical industry, is also used to soil and groundwater remediation field in recent years.Calcium peroxide is water-soluble can generate H
2o
2, its H
2o
2output reach 0.47g H according to Theoretical Calculation is maximum
2o
2/ CaO
2 [5], so calcium peroxide is also referred to as " solid H
2o
2".Compare H
2o
2, calcium peroxide character is more stable, and it generates H
2o
2amount by regulation system pH, control CaO
2dissolution rate controls, and can be utilized more fully so hydrogen peroxide compared by calcium peroxide in actual repair.As the environmentally friendly oxygenant of one, calcium peroxide not only can not bring detrimentally affect to surrounding medium while oxidize contaminants, and on the contrary, it more can produce oxygen and promote the growth of indigenous microorganism, and then improves biological restoration efficiency.
[1] Li Zhu. polycyclic aromatic hydrocarbons is in the distribution characteristics of Huangpu River and adsorption mechanism research. Tongji University, 2007.
[2] R.J. Watts, A.L. Teel, Treatment of contaminated soils and groundwater using ISCO, Practice Periodical of Hazardous, Toxic, Radioact. Waste Manage. 10 (2006) 2-9.
[3] Yan Jingchun. iron containing compounds activation persulphate and the application in organic pollutant is repaired thereof. the Central China University of Science and Technology, 2012.
[4] A. Tsitonaki, B.F. Smets, P.L. Bjerg, Effects of heat-activated persulfate oxidation on soil microorganisms, Water Res. 42 (2008) 1013-1022.
[5] A. Northup, D. Cassidy, Calcium peroxide (CaO
2) for use in modified Fenton chemistry, J. Hazard. Mater. 152 (2008) 1164-1170。
Summary of the invention
The present invention be directed to conventional in situ chemical oxidation agent at present short for effective acting time, unstable under the pH condition of actual underground water or soil, technical barrier large to microbiological effect in surrounding medium in engineer applied, thus provide a kind of method utilizing persulphate and calcium peroxide dual oxidants to remove Organic Pollutants In Water.This dual oxidants is long for the effective acting time to pollutent, the pH scope of its neutral slant acidity is conducive to playing good oxygenizement in the surrounding medium such as underground water or soil, calcium peroxide can promote the biological growth of indigenous microorganism in surrounding medium, improves biological restoration efficiency.Dual oxidants can produce sulfate radical, hydroxyl radical free radical simultaneously, and wide to pollutent sphere of action, validity is strong.
A kind of persulphate that the present invention proposes-calcium peroxide dual oxidants removes the method for multiring aromatic hydrocarbon substance methylnaphthalene, and concrete steps are as follows:
To in the water body containing pollution substance methylnaphthalene, add a certain amount of persulphate and calcium peroxide, stir, maintain system pH and react 4 ~ 5 days under neutral slant acidity condition, oxidation removal pollution substance; Wherein: in dual oxidants, the mass concentration ratio of persulphate and calcium peroxide is 1:0.5 ~ 5, in pollutent methylnaphthalene and dual oxidants, the mass concentration ratio of persulphate is 1:13 ~ 30, and in pollutent methylnaphthalene and dual oxidants, the mass concentration ratio of calcium peroxide is 1:13 ~ 200.
In the present invention, described persulphate is any one in Sodium Persulfate, Potassium Persulphate, ammonium persulphate, persulfuric acid calcium, persulfuric acid magnesium.
In the present invention, the Optimal pH condition that dual oxidants plays a role is neutral or slant acidity.
In the present invention, regulation system pH acid used is nitric acid.
The present invention for renovation agent with persulphate-calcium peroxide dual oxidants, degrades to PAHs class representative methylnaphthalene, can obtain good removal effect.
The present invention includes following beneficial effect:
1, persulphate in the present invention, calcium peroxide cost are low, and the hydrogen peroxide of phase liquid towards, persulphate, calcium peroxide are solid particulate, are convenient to transport, thus workable in practical engineering application.
2, dual oxidants of the present invention is long for the effective acting time to pollutent, and character is more stable, and calcium peroxide generates H
2o
2amount by regulation system pH, control CaO
2dissolution rate controls, and can be utilized more fully so hydrogen peroxide compared by calcium peroxide in actual repair, the utilization ratio of other oxygenant dual oxidants is higher relatively.The pH scope of the neutral slant acidity of dual oxidants is conducive to playing good oxygenizement in the surrounding medium such as underground water or soil.
3, dual oxidants of the present invention mutually activates and can produce sulfate radical, hydroxyl two type free base simultaneously, compares other single-oxidizers and expands degraded scope to pollutent, can remove the pollutent to sulfate radical or this two type frees base sensitivity of hydroxyl simultaneously.Calcium peroxide has promoter action to microorganism growth in surrounding medium, can improve biological restoration efficiency.So dual oxidants effectively can improve the remediation efficiency of Polluted Groundwater or soil.
Accompanying drawing explanation
Fig. 1 is the clearance graphic representation of methylnaphthalene under the condition of 1g/L calcium peroxide and different concns Sodium Persulfate.
Fig. 2 is the clearance graphic representation of methylnaphthalene under the condition of 1g/L Sodium Persulfate and different concns calcium peroxide.
Fig. 3 is the clearance graphic representation of methylnaphthalene under 1g/L Sodium Persulfate and 1g/L calcium peroxide condition of different pH.
Fig. 4 be 1g/L Sodium Persulfate and 1g/L calcium peroxide in ultrapure water and actual underground water to the clearance graphic representation of methylnaphthalene.
Embodiment
Below in conjunction with specific embodiment, set forth the present invention further.Should be understood that these embodiments are only not used in for illustration of the present invention to limit the scope of the invention.In addition should be understood that those skilled in the art can make various changes or modifications the present invention, and these equivalent form of values fall within the application's appended claims limited range equally after the content of having read the present invention's instruction.
Embodiment 1
Be dissolved in a certain amount of ultrapure water by 0.1g calcium peroxide, be placed on agitator and stir, add dilute nitric acid solution regulation system pH to 7, add methylnaphthalene, adding ultrapure water to the last volume of system is 100mL.At room temperature uniform stirring reaction 96h, namely completes the removal utilizing separately calcium peroxide to multiring aromatic hydrocarbon substance methylnaphthalene.In the present embodiment, the clearance of methylnaphthalene 96h reaches 34%.
Embodiment 2
0.1g calcium peroxide and 0.01g, 0.05g, 0.1g, 0.2g and 0.4g Sodium Persulfate are dissolved in a certain amount of ultrapure water respectively, be placed on agitator and stir, add dilute nitric acid solution regulation system pH to 7 respectively, add methylnaphthalene, adding ultrapure water to the last volume of system is 100mL.At room temperature uniform stirring reaction 96h, namely completes the method utilizing persulphate-calcium peroxide dual oxidants to remove multiring aromatic hydrocarbon substance methylnaphthalene.In the present embodiment, the clearance of methylnaphthalene is respectively 77%(96h), 100%(96h), 100%(72h), 100%(72h) and 100%(48h).
Embodiment 3
Be dissolved in a certain amount of ultrapure water by 0.1g Sodium Persulfate, be placed on agitator and stir, add dilute NaOH solution regulation system pH to 7, add methylnaphthalene, adding ultrapure water to the last volume of system is 100mL.At room temperature uniform stirring reaction 96h, namely completes the removal utilizing separately persulphate to multiring aromatic hydrocarbon substance methylnaphthalene.In the present embodiment, the clearance of methylnaphthalene 96h reaches 95%.
Embodiment 4
0.1g Sodium Persulfate and 0.02g, 0.1g, 0.5g and 1.5g calcium peroxide are dissolved in a certain amount of ultrapure water respectively, be placed on agitator and stir, add dilute nitric acid solution regulation system pH to 7 respectively, add methylnaphthalene, adding ultrapure water to the last volume of system is 100mL.At room temperature uniform stirring reaction 96h, namely completes the method utilizing persulphate-calcium peroxide dual oxidants to remove multiring aromatic hydrocarbon substance methylnaphthalene.In the present embodiment, the clearance of methylnaphthalene is respectively 96%(96h), 100%(72h), 100%(72h) and 100%(48h).
Embodiment 5
0.1g calcium peroxide and 0.1g Sodium Persulfate are dissolved in a certain amount of ultrapure water, are placed on agitator and stir, add dilute nitric acid solution regulation system pH to 5,7,9 respectively, add methylnaphthalene, adding ultrapure water to the last volume of system is 100mL.At room temperature uniform stirring reaction 96h, namely completes the method utilizing persulphate-calcium peroxide dual oxidants to remove multiring aromatic hydrocarbon substance methylnaphthalene.In the present embodiment, the clearance of methylnaphthalene is respectively 100%(48h), 100%(72h) and 25%(96h).
Comparative example 1
0.1g Sodium Persulfate and 0.1g calcium peroxide are dissolved in respectively in a certain amount of ultrapure water and actual sampling of ground water, be placed on agitator and stir, add dilute nitric acid solution respectively regulation system pH to 7, add methylnaphthalene, add ultrapure water or actual underground water is 100mL to the last volume of system.At room temperature uniform stirring reaction 96h, namely completes the method utilizing persulphate-calcium peroxide dual oxidants to remove multiring aromatic hydrocarbon substance methylnaphthalene.In this comparative example, the clearance of methylnaphthalene in ultrapure water is 100%(72h), the clearance in actual sampling of ground water is 84%(96h).
Claims (4)
1. the method for persulphate-calcium peroxide dual oxidants removal multiring aromatic hydrocarbon substance methylnaphthalene, it is characterized in that concrete steps are as follows: in the water body containing pollution substance methylnaphthalene, add a certain amount of persulphate and calcium peroxide, stir, maintenance system pH reacts 4 ~ 5 days under neutral slant acidity condition, oxidation removal pollution substance; In dual oxidants, the mass concentration ratio of persulphate and calcium peroxide is 1:0.5 ~ 5, in pollutent methylnaphthalene and dual oxidants, the mass concentration ratio of persulphate is 1:13 ~ 30, and in pollutent methylnaphthalene and dual oxidants, the mass concentration ratio of calcium peroxide is 1:13 ~ 200.
2. a kind of persulphate according to claim 1-calcium peroxide dual oxidants removes the method for multiring aromatic hydrocarbon substance methylnaphthalene, it is characterized in that, described persulphate is any one in Sodium Persulfate, Potassium Persulphate, ammonium persulphate, persulfuric acid calcium or persulfuric acid magnesium.
3. a kind of persulphate according to claim 1-calcium peroxide dual oxidants removes the method for multiring aromatic hydrocarbon substance methylnaphthalene, it is characterized in that, the pH condition that dual oxidants plays a role is neutral or slant acidity.
4. a kind of persulphate according to claim 1-calcium peroxide dual oxidants removes the method for multiring aromatic hydrocarbon substance methylnaphthalene, and it is characterized in that, regulation system pH acid used is nitric acid.
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| CN107474865A (en) * | 2017-08-29 | 2017-12-15 | 北京化工大学 | A kind of modification process of pitch |
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| CN107474865A (en) * | 2017-08-29 | 2017-12-15 | 北京化工大学 | A kind of modification process of pitch |
| CN107474865B (en) * | 2017-08-29 | 2020-06-26 | 北京化工大学 | Modification treatment process for asphalt |
| CN108640250A (en) * | 2018-04-19 | 2018-10-12 | 济南大学 | A kind of method that calper calcium peroxide-sodium peroxydisulfate dual oxidants remove 2,4- Dichlorophenols in water removal |
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| CN111760899A (en) * | 2020-06-22 | 2020-10-13 | 南京农业大学 | Feeding improvement method for repairing toxic organic contaminated soil through oxidant compounding oxidation |
| CN111760899B (en) * | 2020-06-22 | 2021-08-24 | 南京农业大学 | Feeding improvement method for repairing toxic organic contaminated soil through oxidant compounding oxidation |
| CN112457858A (en) * | 2020-11-05 | 2021-03-09 | 北辰(上海)环境科技有限公司 | Chemical oxidation remediation agent for organic contaminated soil and use method |
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