CN115872516A - Wastewater treatment method of Fenton system under bicarbonate coexistence condition - Google Patents
Wastewater treatment method of Fenton system under bicarbonate coexistence condition Download PDFInfo
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- CN115872516A CN115872516A CN202211643594.9A CN202211643594A CN115872516A CN 115872516 A CN115872516 A CN 115872516A CN 202211643594 A CN202211643594 A CN 202211643594A CN 115872516 A CN115872516 A CN 115872516A
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- BVKZGUZCCUSVTD-UHFFFAOYSA-M Bicarbonate Chemical compound OC([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-M 0.000 title claims abstract description 14
- 238000004065 wastewater treatment Methods 0.000 title claims abstract description 9
- CWYNVVGOOAEACU-UHFFFAOYSA-N Fe2+ Chemical compound [Fe+2] CWYNVVGOOAEACU-UHFFFAOYSA-N 0.000 claims abstract description 25
- 238000000034 method Methods 0.000 claims abstract description 22
- BAUYGSIQEAFULO-UHFFFAOYSA-L iron(2+) sulfate (anhydrous) Chemical compound [Fe+2].[O-]S([O-])(=O)=O BAUYGSIQEAFULO-UHFFFAOYSA-L 0.000 claims abstract description 18
- 238000006243 chemical reaction Methods 0.000 claims abstract description 13
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 claims abstract description 12
- 239000003638 chemical reducing agent Substances 0.000 claims abstract description 12
- 239000002351 wastewater Substances 0.000 claims abstract description 12
- 239000002738 chelating agent Substances 0.000 claims abstract description 11
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 20
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 claims description 2
- 229910002651 NO3 Inorganic materials 0.000 claims description 2
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 claims description 2
- NHNBFGGVMKEFGY-UHFFFAOYSA-N nitrate group Chemical group [N+](=O)([O-])[O-] NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 claims description 2
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 claims 3
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 claims 3
- CIWBSHSKHKDKBQ-JLAZNSOCSA-N Ascorbic acid Chemical compound OC[C@H](O)[C@H]1OC(=O)C(O)=C1O CIWBSHSKHKDKBQ-JLAZNSOCSA-N 0.000 claims 2
- KCXVZYZYPLLWCC-UHFFFAOYSA-N EDTA Chemical group OC(=O)CN(CC(O)=O)CCN(CC(O)=O)CC(O)=O KCXVZYZYPLLWCC-UHFFFAOYSA-N 0.000 claims 1
- AVXURJPOCDRRFD-UHFFFAOYSA-N Hydroxylamine Chemical compound ON AVXURJPOCDRRFD-UHFFFAOYSA-N 0.000 claims 1
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 claims 1
- 229960005070 ascorbic acid Drugs 0.000 claims 1
- 235000010323 ascorbic acid Nutrition 0.000 claims 1
- 239000011668 ascorbic acid Substances 0.000 claims 1
- 229940071106 ethylenediaminetetraacetate Drugs 0.000 claims 1
- 235000006408 oxalic acid Nutrition 0.000 claims 1
- 230000003197 catalytic effect Effects 0.000 abstract description 6
- 230000008569 process Effects 0.000 abstract description 5
- 238000001556 precipitation Methods 0.000 abstract description 4
- 239000002994 raw material Substances 0.000 abstract description 3
- 230000002779 inactivation Effects 0.000 abstract 1
- 239000002244 precipitate Substances 0.000 abstract 1
- HFZWRUODUSTPEG-UHFFFAOYSA-N 2,4-dichlorophenol Chemical compound OC1=CC=C(Cl)C=C1Cl HFZWRUODUSTPEG-UHFFFAOYSA-N 0.000 description 16
- WTDHULULXKLSOZ-UHFFFAOYSA-N Hydroxylamine hydrochloride Chemical group Cl.ON WTDHULULXKLSOZ-UHFFFAOYSA-N 0.000 description 16
- 238000006731 degradation reaction Methods 0.000 description 15
- 230000015556 catabolic process Effects 0.000 description 11
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 9
- 229910052742 iron Inorganic materials 0.000 description 7
- ZGTMUACCHSMWAC-UHFFFAOYSA-L EDTA disodium salt (anhydrous) Chemical compound [Na+].[Na+].OC(=O)CN(CC([O-])=O)CCN(CC(O)=O)CC([O-])=O ZGTMUACCHSMWAC-UHFFFAOYSA-L 0.000 description 6
- 230000000694 effects Effects 0.000 description 6
- 239000003109 Disodium ethylene diamine tetraacetate Substances 0.000 description 5
- 239000013522 chelant Substances 0.000 description 5
- 235000019301 disodium ethylene diamine tetraacetate Nutrition 0.000 description 5
- 239000003344 environmental pollutant Substances 0.000 description 5
- 230000003647 oxidation Effects 0.000 description 5
- 238000007254 oxidation reaction Methods 0.000 description 5
- 231100000719 pollutant Toxicity 0.000 description 5
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 4
- 239000001301 oxygen Substances 0.000 description 4
- 229910052760 oxygen Inorganic materials 0.000 description 4
- 239000003054 catalyst Substances 0.000 description 3
- BDOYKFSQFYNPKF-UHFFFAOYSA-N 2-[2-[bis(carboxymethyl)amino]ethyl-(carboxymethyl)amino]acetic acid;sodium Chemical group [Na].[Na].OC(=O)CN(CC(O)=O)CCN(CC(O)=O)CC(O)=O BDOYKFSQFYNPKF-UHFFFAOYSA-N 0.000 description 2
- 239000004677 Nylon Substances 0.000 description 2
- 239000012190 activator Substances 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 235000003891 ferrous sulphate Nutrition 0.000 description 2
- 239000011790 ferrous sulphate Substances 0.000 description 2
- 238000004128 high performance liquid chromatography Methods 0.000 description 2
- 229910000359 iron(II) sulfate Inorganic materials 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 229910052757 nitrogen Inorganic materials 0.000 description 2
- 229920001778 nylon Polymers 0.000 description 2
- 238000010525 oxidative degradation reaction Methods 0.000 description 2
- 239000002957 persistent organic pollutant Substances 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- 230000035484 reaction time Effects 0.000 description 2
- 229910021642 ultra pure water Inorganic materials 0.000 description 2
- 239000012498 ultrapure water Substances 0.000 description 2
- BEQKKZICTDFVMG-UHFFFAOYSA-N 1,2,3,4,6-pentaoxepane-5,7-dione Chemical compound O=C1OOOOC(=O)O1 BEQKKZICTDFVMG-UHFFFAOYSA-N 0.000 description 1
- 230000003213 activating effect Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000000593 degrading effect Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 description 1
- 239000007800 oxidant agent Substances 0.000 description 1
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W10/00—Technologies for wastewater treatment
- Y02W10/30—Wastewater or sewage treatment systems using renewable energies
- Y02W10/37—Wastewater or sewage treatment systems using renewable energies using solar energy
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- Treatment Of Water By Oxidation Or Reduction (AREA)
Abstract
The invention discloses a wastewater treatment method of a Fenton system under the condition of bicarbonate coexistence, which mainly solves the problems of narrow pH application range and low utilization efficiency of ferrous salt of the traditional Fenton system; firstly, mixing a ferrous salt and a chelating agent to prepare a solution A with a certain concentration, simultaneously preparing hydrogen peroxide and bicarbonate to prepare a solution B with a certain concentration, adding wastewater to be treated into the solution B, and finally adding the solution A or simultaneously adding the ferrous salt and a reducing agent until the reaction is finished. The method has the advantages of simple process, easily obtained raw materials, simple process and strong controllability of reaction conditions, and can effectively solve the problem of low utilization efficiency caused by easy precipitation of ferrous salt under alkaline conditions. The method has high treatment efficiency on the alkaline wastewater, and simultaneously the problem of low catalytic utilization efficiency caused by inactivation of ferrous iron precipitate can be effectively solved by adding the reducing agent or the chelating agent, and the addition amount of ferrous iron can be effectively reduced under the condition of the same treatment efficiency.
Description
Technical Field
The invention belongs to the technical field of water treatment, and particularly relates to a wastewater treatment method of a Fenton system under the condition of bicarbonate coexistence.
Background
The fenton technology is a typical advanced oxidation treatment technology and is widely applied to the removal of organic pollutants which are difficult to degrade in water. Compared with other advanced oxidation technologies, hydroxyl radicals generated by the Fenton system have stronger oxidation capacity than other oxidants, and can realize non-selective oxidation on pollutants in wastewater. But the Fenton technology has the outstanding problems of narrow pH application range, large iron mud generation amount and the like in the application process. The intermediate peroxybicarbonate is generated by activating hydrogen peroxide with bicarbonate (based on an advanced oxidation method of peroxybicarbonate), and can realize efficient degradation of pollutants under the alkaline condition under the catalytic action of catalysts such as cobalt, manganese, iron and the like, thereby effectively solving the bottleneck problem that the traditional Fenton system can not be applied to the alkaline environment. The method has the advantages of high treatment efficiency, thorough removal, low cost, convenience in operation and high pH tolerance, but ferrous iron is easy to precipitate when used as a catalyst, so that the dosage of the ferrous iron is large, and the utilization efficiency is not high finally.
Disclosure of Invention
Aiming at the defects of the prior art, the invention provides a wastewater treatment method of a Fenton system under the condition of bicarbonate coexistence, and the addition of a reducing agent or a chelating agent can effectively reduce the precipitation rate of ferrous iron in an alkaline environment, simultaneously can ensure the catalytic efficiency of the ferrous iron on peroxybicarbonate, generates different active components under the catalytic action, and realizes the oxidative degradation of wastewater pollutants in the alkaline environment. The method can effectively solve the problem that ferrous iron is precipitated as a catalyst in an alkaline environment to cause low catalytic efficiency and utilization efficiency, and can effectively reduce the dosage of ferrous iron salt on the premise of ensuring the pollutant degradation efficiency.
The specific technical scheme is as follows:
the invention provides a wastewater treatment method of a Fenton system under the condition of bicarbonate coexistence, which mainly comprises the following steps:
mixing a ferrous salt and a reducing agent or a chelating agent to prepare a solution A with a certain concentration, simultaneously preparing hydrogen peroxide and bicarbonate into a solution B with a certain concentration, then adding the solution B into the wastewater to be treated, and finally adding the solution A or adding the solution A and adding the ferrous salt and the reducing agent simultaneously until the reaction is finished.
Furthermore, the reducing agent is hydroxylamine hydrochloride, and the chelating agent is ethylene diamine tetraacetic acid disodium.
Further, the ferrous salt is nitrate, sulfate or chloride.
Further, the molar ratio of the ferrous salt to the reducing agent or the chelating agent is (2).
Further, the molar ratio of ferrous iron to bicarbonate is 1.
Furthermore, the dosage of the ferrous salt is 2-20 mmol/L, and the molar ratio of the ferrous salt to the hydrogen peroxide is 1.
The improved Fenton system is used for degrading organic pollutants in alkaline wastewater.
The invention provides a wastewater treatment method of a Fenton system under the condition of bicarbonate coexistence, which only needs to add a reducing agent or a chelating agent into the system, has easily obtained raw materials, is simple to operate, and is safe and environment-friendly.
Compared with the prior art, the invention has the following characteristics and advantages:
1) The raw materials used in the invention are common chemical reagents, and have wide sources, low price and easy obtainment;
2) The method has the advantages of simple process, low requirement on equipment, simple process and strong controllability of reaction conditions;
3) According to the invention, the effect of the reducing agent and the chelating agent is utilized, the precipitation rate of ferrous iron in an alkaline environment can be effectively reduced, the efficiency of catalyzing peroxydicarbonate by ferrous iron is improved, the dosage of ferrous iron is reduced by 2-5 times under the condition of the same pollutant degradation efficiency, and the efficient oxidative degradation of organic matters in alkaline wastewater is realized.
Drawings
FIG. 1 is a graph showing the degradation effect of divalent iron activated peroxybicarbonate on 2, 4-dichlorophenol with hydroxylamine hydrochloride addition in the examples;
FIG. 2 is a graph showing the degradation effect of divalent iron activated peroxybicarbonate on 2, 4-dichlorophenol by disodium EDTA in the example.
Detailed Description
In order to enhance the understanding of the present invention, the present invention will be described in more detail and fully with reference to the following examples.
Example 1
A method for removing 2, 4-dichlorophenol in a water body by using ferrous iron activated peroxybicarbonate radical added by hydroxylamine hydrochloride specifically comprises the following steps:
the experimental water is ultrapure water, nitrogen is introduced for 1 hour before the reaction starts, and the dissolved oxygen concentration is measured by using a dissolved oxygen meter and used for subsequent solution preparation after the use standard is reached. According to the addition of 2mM of ferrous iron and 2mM of hydroxylamine hydrochloride 3 The concentration was 25mM 2 O 2 At a concentration of 50mM, a pre-weighed amount of NaHCO was added to each reaction flask 3 And H 2 O 2 After 5-10 minutes of reaction, adding 2,4-DCP solution, then immediately adding the prepared ferrous sulfate solution and hydroxylamine hydrochloride at the same time, putting the conical flask into a constant-temperature water bath kettle for degradation reaction, wherein the rotating speed is 200rpm, the temperature is set to be 25 ℃, and the reaction time is 60min.
The control group in this example was degradation reactions with ferrous concentrations of 2mM and 4mM, respectively, under otherwise identical conditions.
In this example, samples were periodically taken in a constant temperature water bath, and the samples were filtered through a 0.22 μm nylon filter and the concentration of the remaining 2,4-DCP in the solution was measured by high performance liquid chromatography. According to the change of the concentration of the 2,4-DCP in the solution before and after the reaction, the removal rate of the 2,4-DCP is calculated.
FIG. 1 is a graph showing the effect of divalent iron activated peroxybicarbonate on the degradation of 2,4-DCP with hydroxylamine hydrochloride in example 1 of the present invention. As can be seen from FIG. 1, with the addition of 2mM Fe 2+ Compared with the system, the degradation rate of 2,4-DCP is improved to 50 percent after the hydroxylamine hydrochloride is added, probably because the addition of the hydroxylamine hydrochloride inhibits Fe 3+ Promote the precipitation of Fe 2+ The existence of the Fe is beneficial to maintaining the Fe existing in a dissolved state, and the catalytic capability of the system is improved to a certain extent.
Example 2
A method for comparing degradation effects of divalent iron activated peroxybicarbonate radical on 2, 4-dichlorophenol by adding disodium ethylene diamine tetraacetate with a schematic diagram specifically comprises the following steps:
the experimental water is ultrapure water, nitrogen is introduced for 1 hour before the reaction starts, and the dissolved oxygen concentration is measured by using a dissolved oxygen meter and used for subsequent solution preparation after the use standard is reached. Before reaction, mixing a ferrous sulfate solution and ethylene diamine tetraacetic acid disodium according to a concentration ratio of 2:1 to prepare the chelate. Add pre-weighed NaHCO to the reaction flask 3 And H 2 O 2 (NaHCO 3 At a concentration of 25mM 2 O 2 Concentration is 50 mM), after reacting for 5-10 minutes, 2,4-DCP solution is added, and then the prepared chelate of ferrous iron and disodium ethylenediaminetetraacetate is added immediately to make the concentration 2mM. And (3) putting the conical flask into a constant-temperature water bath kettle for degradation reaction, wherein the rotating speed is 200rpm, the temperature is set to be 25 ℃, and the reaction time is 60min.
The control group of this example was degradation reaction of ferrous iron with 4mM and 10mM of activator added, respectively, under the same conditions.
In this example, samples were periodically taken in a constant temperature water bath, and the samples were filtered through a 0.22 μm nylon filter and the concentration of the remaining 2,4-DCP in the solution was measured by high performance liquid chromatography. And calculating the removal rate of the 2,4-DCP according to the concentration change condition of the 2,4-DCP in the solution before and after the reaction.
FIG. 2 is a graph showing the effect of divalent iron activated peroxybicarbonate on the degradation of 2,4-DCP with disodium EDTA. As can be seen from FIG. 2, the degradation rate of 2,4-DCP was improved to 100% after adding the chelate of disodium EDTA and ferrous iron, compared to the system in which the activator was added at 4mM ferrous iron, and the degradation rate of the system in which the chelate of ferrous iron was added was much higher than that of the system in which the ferrous iron was added at the same time point. The chelate system of adding disodium ethylenediamine tetraacetic acid and ferrous iron can greatly reduce the ferrous iron dosage compared with the system of adding 10mM ferrous iron.
The above description is only a preferred example of the present invention and is not intended to limit the present invention, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, improvement and the like of the present invention shall be included in the protection scope of the present invention.
Claims (6)
1. A method for treating wastewater of a Fenton system under the condition of coexistence of bicarbonate is characterized by comprising the following steps:
mixing a ferrous salt and a chelating agent to prepare a solution A, and simultaneously preparing hydrogen peroxide and bicarbonate to prepare a solution B;
then adding the wastewater to be treated into the solution B;
and finally adding the solution A, or adding the solution A and simultaneously adding the ferrous salt and the reducing agent until the reaction is finished.
2. The method for treating wastewater of Fenton's system according to claim 1, wherein said method further comprises the steps of: the reducing agent is ascorbic acid, hydroxylamine, iron powder and sulfide, and the chelating agent is ethylenediamine tetraacetate, citric acid and oxalic acid.
3. The method for treating wastewater of Fenton's system according to claim 1, wherein said method further comprises the steps of: the ferrous salt is nitrate, sulfate or chloride.
4. The method according to claim 1, wherein the wastewater treatment method comprises: the molar ratio of the ferrous salt to the reducing agent or the chelating agent is 2.
5. The method for treating wastewater of Fenton's system according to claim 1, wherein said method further comprises the steps of: the molar ratio of ferrous iron to bicarbonate is 1 to 1.
6. The method according to claim 1, wherein the wastewater treatment method comprises: the dosage of the ferrous salt is 2-20 mmol/L, and the molar ratio of the ferrous salt to the hydrogen peroxide is 1.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115745137A (en) * | 2022-12-20 | 2023-03-07 | 成都理工大学 | Method for treating alkaline wastewater by Fenton system |
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