CN114308036A - Method for oxidizing and repairing polluted soil by activated carbon-based monatomic iron catalyst - Google Patents
Method for oxidizing and repairing polluted soil by activated carbon-based monatomic iron catalyst Download PDFInfo
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 123
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 title claims abstract description 110
- 229910052742 iron Inorganic materials 0.000 title claims abstract description 55
- 239000003054 catalyst Substances 0.000 title claims abstract description 54
- 238000000034 method Methods 0.000 title claims abstract description 48
- 239000002689 soil Substances 0.000 title abstract description 78
- 230000001590 oxidative effect Effects 0.000 title abstract description 15
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims abstract description 36
- 238000010438 heat treatment Methods 0.000 claims abstract description 34
- 238000003756 stirring Methods 0.000 claims abstract description 25
- 230000008569 process Effects 0.000 claims abstract description 24
- 239000000463 material Substances 0.000 claims abstract description 13
- DGEZNRSVGBDHLK-UHFFFAOYSA-N [1,10]phenanthroline Chemical compound C1=CN=C2C3=NC=CC=C3C=CC2=C1 DGEZNRSVGBDHLK-UHFFFAOYSA-N 0.000 claims abstract description 12
- PVFSDGKDKFSOTB-UHFFFAOYSA-K iron(3+);triacetate Chemical compound [Fe+3].CC([O-])=O.CC([O-])=O.CC([O-])=O PVFSDGKDKFSOTB-UHFFFAOYSA-K 0.000 claims abstract description 12
- 239000002253 acid Substances 0.000 claims abstract description 10
- 238000001354 calcination Methods 0.000 claims abstract description 9
- 238000001035 drying Methods 0.000 claims abstract description 9
- 238000001704 evaporation Methods 0.000 claims abstract description 9
- 238000002156 mixing Methods 0.000 claims abstract description 9
- 238000002360 preparation method Methods 0.000 claims abstract description 9
- 238000005406 washing Methods 0.000 claims abstract description 9
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 22
- 238000003837 high-temperature calcination Methods 0.000 claims description 16
- 229910052757 nitrogen Inorganic materials 0.000 claims description 11
- 238000007254 oxidation reaction Methods 0.000 abstract description 34
- 230000003647 oxidation Effects 0.000 abstract description 33
- 125000005575 polycyclic aromatic hydrocarbon group Chemical group 0.000 abstract description 29
- JRKICGRDRMAZLK-UHFFFAOYSA-L peroxydisulfate Chemical compound [O-]S(=O)(=O)OOS([O-])(=O)=O JRKICGRDRMAZLK-UHFFFAOYSA-L 0.000 abstract description 19
- 230000003197 catalytic effect Effects 0.000 abstract description 8
- 238000005067 remediation Methods 0.000 abstract description 7
- 229910052799 carbon Inorganic materials 0.000 abstract 2
- 230000010355 oscillation Effects 0.000 description 24
- FMMWHPNWAFZXNH-UHFFFAOYSA-N Benz[a]pyrene Chemical compound C1=C2C3=CC=CC=C3C=C(C=C3)C2=C2C3=CC=CC2=C1 FMMWHPNWAFZXNH-UHFFFAOYSA-N 0.000 description 20
- UFWIBTONFRDIAS-UHFFFAOYSA-N Naphthalene Chemical compound C1=CC=CC2=CC=CC=C21 UFWIBTONFRDIAS-UHFFFAOYSA-N 0.000 description 20
- YNPNZTXNASCQKK-UHFFFAOYSA-N phenanthrene Chemical compound C1=CC=C2C3=CC=CC=C3C=CC2=C1 YNPNZTXNASCQKK-UHFFFAOYSA-N 0.000 description 20
- 239000000203 mixture Substances 0.000 description 13
- TXVHTIQJNYSSKO-UHFFFAOYSA-N BeP Natural products C1=CC=C2C3=CC=CC=C3C3=CC=CC4=CC=C1C2=C34 TXVHTIQJNYSSKO-UHFFFAOYSA-N 0.000 description 10
- CWRYPZZKDGJXCA-UHFFFAOYSA-N acenaphthene Chemical compound C1=CC(CC2)=C3C2=CC=CC3=C1 CWRYPZZKDGJXCA-UHFFFAOYSA-N 0.000 description 10
- RMBPEFMHABBEKP-UHFFFAOYSA-N fluorene Chemical compound C1=CC=C2C3=C[CH]C=CC3=CC2=C1 RMBPEFMHABBEKP-UHFFFAOYSA-N 0.000 description 10
- NIHNNTQXNPWCJQ-UHFFFAOYSA-N o-biphenylenemethane Natural products C1=CC=C2CC3=CC=CC=C3C2=C1 NIHNNTQXNPWCJQ-UHFFFAOYSA-N 0.000 description 10
- 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 description 9
- CHQMHPLRPQMAMX-UHFFFAOYSA-L sodium persulfate Substances [Na+].[Na+].[O-]S(=O)(=O)OOS([O-])(=O)=O CHQMHPLRPQMAMX-UHFFFAOYSA-L 0.000 description 9
- 239000007800 oxidant agent Substances 0.000 description 8
- 150000003254 radicals Chemical class 0.000 description 8
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 7
- 238000006243 chemical reaction Methods 0.000 description 6
- 238000001816 cooling Methods 0.000 description 5
- 239000003344 environmental pollutant Substances 0.000 description 5
- 231100000719 pollutant Toxicity 0.000 description 5
- 230000008439 repair process Effects 0.000 description 5
- 239000006228 supernatant Substances 0.000 description 5
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 3
- 238000011160 research Methods 0.000 description 3
- 238000006555 catalytic reaction Methods 0.000 description 2
- 230000000593 degrading effect Effects 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 230000002195 synergetic effect Effects 0.000 description 2
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 238000001878 scanning electron micrograph Methods 0.000 description 1
- 238000003900 soil pollution Methods 0.000 description 1
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Abstract
The invention discloses a method for oxidizing and repairing polluted soil by an activated carbon-based monatomic iron catalyst. The preparation method of the activated carbon-based monatomic iron catalyst comprises the following steps: (1) dissolving ferric acetate and 1, 10-phenanthroline in an ethanol solution, uniformly mixing, adding activated carbon powder, heating and stirring, and evaporating ethanol to dryness in the heating and stirring process to obtain a dried sample; (2) and (3) calcining the dried sample at high temperature, and then carrying out acid washing and drying to obtain the activated carbon-based monatomic iron material. Compared with the prior art, the active carbon-based monatomic iron catalyst prepared by the invention is used for constructing a new system for catalytic oxidation of the soil polycyclic aromatic hydrocarbon by using the active carbon-based monatomic iron material/persulfate solution based on the catalyst, realizing efficient oxidation remediation of polycyclic aromatic hydrocarbon-polluted sites, and avoiding and overcoming some limitations of the existing advanced oxidation system.
Description
Technical Field
The invention relates to the technical field of soil pollution remediation, in particular to a method for oxidizing and remedying polluted soil by using an activated carbon-based monatomic iron catalyst, and particularly relates to a method for oxidizing the polluted soil of polycyclic aromatic hydrocarbons in an industrial field by using the activated carbon-based monatomic iron catalyst and persulfate.
Background
The organic pollution site environmental problem becomes an obstacle in the land redevelopment process of China, seriously restricts the regional economic development and influences the health of surrounding residents, and is a major social, economic and ecological environmental problem which must be faced by cities of China at the present stage. The persulfate oxidation technology is increasingly becoming a popular option for repairing domestic organic pollution sites due to the characteristics of high stability, high water solubility and no peculiar smell of persulfate. In conventional persulfate oxidation techniques, Fe2+Is the most commonly used activated persulfate material, but is limited by the distribution form of polycyclic aromatic hydrocarbons in the soil and the oxidation mechanism of free radicals, Fe2+The activation still has the problems of large oxidant consumption, tailing and the like. The introduction of the catalyst can effectively improve the problem of insufficient polycyclic aromatic hydrocarbon of persulfate oxidized soil, but the existing catalysts such as metal oxides, metal simple substances and the like have the problem of insufficient capability. In recent years, a great deal of research focuses on non-radical oxidation which is twice as high as the utilization rate of an oxidant compared with radical oxidation, while a persulfate system activated by a metal-based carbon material catalyst can generate the non-radical oxidation, but the research of applying the activated persulfate non-radical oxidation system to the remediation of the organic contaminated soil is still clear. Therefore, in view of some disadvantages of the existing non-radical oxidation, a novel activated persulfate having high efficiency has been soughtAn acid salt oxidation system.
Disclosure of Invention
The invention aims to solve the technical problem of overcoming the technical defects and provides a novel, green and efficient method for oxidizing and repairing the polluted soil by using the activated carbon-based monatomic iron catalyst.
In order to solve the problems, the technical scheme of the invention is as follows: a preparation method of an activated carbon-based monatomic iron catalyst comprises the following steps:
(1) dissolving ferric acetate and 1, 10-phenanthroline in an ethanol solution, uniformly mixing, adding activated carbon powder, heating and stirring, and evaporating ethanol to dryness in the heating and stirring process to obtain a dried sample;
(2) and (3) calcining the dried sample at high temperature, and then carrying out acid washing and drying to obtain the activated carbon-based monatomic iron material.
Further, the mass ratio of the addition amounts of the iron acetate, the 1, 10-phenanthroline and the activated carbon is 1: (3-4): (25-50).
Further, in the heating and stirring process, the heating temperature is 60-80 ℃, and the stirring time is 4-12 hours.
Further, in the high-temperature calcination process, nitrogen is introduced for protection, and the introduction flow rate of the nitrogen is 30-60 mL/min.
Further, in the high-temperature calcination process: firstly, the temperature is raised to 500-800 ℃ at a rate of 5-15 ℃/min and calcined for 1.5-2.5 h.
Compared with the prior art, the invention has the advantages that: (1) aiming at the problems of low oxidation efficiency, high consumption of an oxidant and the like of soil remediation of polycyclic aromatic hydrocarbons by a chemical oxidation method, the invention prepares the activated carbon-based monatomic iron catalyst, and constructs a new activated carbon-based monatomic iron catalyst/persulfate soil polycyclic aromatic hydrocarbon catalytic oxidation system based on the catalyst, namely, the activated carbon-based monatomic iron catalyst is firstly prepared, and then the activated carbon-based monatomic iron catalyst and persulfate are sequentially added into the polycyclic aromatic hydrocarbon contaminated soil for catalytic oxidation reaction, so that the efficient oxidation remediation of polycyclic aromatic hydrocarbon contaminated sites is realized, and some limitations of the existing advanced oxidation system can be avoided and overcome.
(2) Activated carbon based monatomic iron material is used as a catalyst, the monatomic iron and the activated carbon are coupled to easily catalyze and excite persulfate to generate strong oxidants such as hydroxyl free radicals and sulfate free radicals, and meanwhile, singlet oxygen active species can be generated to react; the biochar is used as a carrier, so that the catalyst has excellent electron storage and transfer capacity, and the purpose of degrading the soil polycyclic aromatic hydrocarbon by oxidizing persulfate in a synergistic catalysis manner is achieved.
Drawings
Fig. 1 is an SEM image of the activated carbon-based monatomic iron catalyst prepared in example 1.
Fig. 2 is an EDS diagram of the activated carbon-based monatomic iron catalyst prepared in example 1.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments; all other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
As shown in fig. 1 to 2, a method for preparing an activated carbon-based monatomic iron catalyst, the method comprising the steps of:
step one, dissolving ferric acetate and 1, 10-phenanthroline in an ethanol solution, uniformly mixing, adding activated carbon powder, heating and stirring, and evaporating ethanol to dryness in the heating and stirring process to obtain a dried sample;
and step two, calcining the dried sample at high temperature, and then carrying out acid washing and drying to obtain the activated carbon-based monatomic iron material.
The mass ratio of the addition amounts of the iron acetate, the 1, 10-phenanthroline and the activated carbon is 1: (3-4): (25-50).
In the heating and stirring process, the heating temperature is 60-80 ℃, and the stirring time is 4-12 h.
And in the high-temperature calcination process, introducing nitrogen for protection, wherein the introduction flow of the nitrogen is 30-60 mL/min.
In the high-temperature calcination process: firstly, the temperature is raised to 500-800 ℃ at a rate of 5-15 ℃/min and calcined for 1.5-2.5 h.
The activated carbon-based monatomic iron catalyst is prepared by adopting the method.
The application of the activated carbon-based monatomic iron catalyst is used for oxidizing and repairing polycyclic aromatic hydrocarbon polluted soil.
An oxidation remediation method of contaminated soil by using an activated carbon-based monatomic iron catalyst, which comprises the following steps: the method comprises the steps of taking an activated carbon-based monoatomic iron material as a catalyst, taking sodium persulfate as an oxidant, and carrying out oxidation remediation on the polycyclic aromatic hydrocarbon polluted soil at normal temperature and normal pressure.
The oxidation repairing method comprises the following steps:
under the oscillation condition, sequentially adding an activated carbon-based monoatomic iron catalyst and a sodium persulfate solution into polycyclic aromatic hydrocarbon polluted soil, wherein the adding amount of the catalyst is 0.5-2%;
and step two, stirring and reacting for 1-2 hours at 20-30 ℃, and separating to obtain the repaired soil.
The oxidation repairing method specifically comprises the following steps:
step one, sequentially adding an activated carbon-based monatomic iron catalyst into polycyclic aromatic hydrocarbon polluted soil under an oscillation condition, wherein the mass ratio of the catalyst to the soil is 1: (100-200); under the oscillation condition, adding a sodium persulfate solution into the catalyst and soil mixture, wherein the mass-volume ratio of the catalyst to the soil mixture to the solution is (1-2): 1g/mL, and the mass ratio of the sodium persulfate to the soil is 0.5-5%.
And step two, carrying out oscillation reaction on the soil mixture at the temperature of 20-30 ℃ for 1-2 h, separating to obtain the repaired soil, and analyzing the content of the polycyclic aromatic hydrocarbon in the soil.
Persulfate is a strong oxidant, and has been widely used as an oxidant for organically-polluted soil due to its characteristics of high stability, high water solubility and no peculiar smell. However, in an actual polluted site, polycyclic aromatic hydrocarbons are mostly distributed in soil organic matters, so that the effective contact rate of persulfate and the polycyclic aromatic hydrocarbons in the soil is low, and the problems of low oxidation efficiency, high oxidant consumption, tailing and the like are caused. The introduction of the activated carbon-based monatomic iron catalyst can effectively solve the problem of shortage of persulfate oxidized soil polycyclic aromatic hydrocarbon. Researches show that the activated carbon-based monatomic iron catalyst can react with persulfate adsorbed on the surface of the activated carbon-based monatomic iron catalyst to generate singlet oxygen, and the soil polycyclic aromatic hydrocarbon is oxidized and decomposed under the action of the singlet oxygen, so that the aim of degrading the soil polycyclic aromatic hydrocarbon by the oxidation of the persulfate under the synergetic catalysis of the activated carbon-based monatomic iron catalyst is fulfilled.
Specific examples are as follows.
Example 1:
1. soil source and pollutant content
The soil is original soil of a site polluted by certain polycyclic aromatic hydrocarbon, wherein the contents of naphthalene, acenaphthene, fluorene, phenanthrene and benzo (a) pyrene are respectively 105mg/kg, 44.2mg/kg, 41.0mg/kg, 42.3mg/kg and 10.8 mg/kg.
2. Preparation of activated carbon based monatomic iron catalyst
(1) Dissolving ferric acetate (0.0435g) and 1, 10-phenanthroline (0.1485g) in an ethanol solution (100mL), uniformly mixing, adding activated carbon powder (2.0g), heating at 60 ℃, stirring, and evaporating ethanol to dryness (4h) in the heating and stirring process to obtain a dried sample;
(2) and (2) carrying out high-temperature calcination on the dried sample, wherein the introduction flow of nitrogen is 30mL/min, heating to 800 ℃ at the heating rate of 10 ℃/min in the high-temperature calcination process, calcining for 2.0h, then naturally cooling, and then carrying out acid washing and drying on the calcined sample to obtain the activated carbon-based monatomic iron material, wherein SEM and EDS diagrams of the activated carbon-based monatomic iron catalyst are respectively shown in figures 1 and 2.
3. Oxidation repair method
(1) Under the oscillation condition that the oscillation speed is 250 revolutions per minute, 0.1g of activated carbon-based monatomic iron catalyst, 5mL of water and 1% of sodium persulfate are respectively and sequentially added into 10g of polycyclic aromatic hydrocarbon-polluted soil.
(2) The soil mixture is controlled at the temperature of 25 ℃ and subjected to oscillation reaction for 2 hours at the oscillation speed of 250 revolutions per minute.
(3) And placing the reacted soil mixture in a centrifuge, centrifuging for 10min at the rotation speed of 4000 revolutions per minute, and removing the supernatant to obtain the repaired soil.
(4) The contents of naphthalene, acenaphthene, fluorene, phenanthrene and benzo (a) pyrene in the treated soil are respectively measured to be 13.2mg/kg, 21.8mg/kg, 10.5mg/kg, 10.4mg/kg and 5.3mg/kg, and the removal rate of polycyclic aromatic hydrocarbon in the soil by the catalytic oxidation system is 74.8%.
Example 2:
1. soil source and pollutant content
The soil is original soil of a site polluted by certain polycyclic aromatic hydrocarbon, wherein the contents of naphthalene, acenaphthene, fluorene, phenanthrene and benzo (a) pyrene are respectively 105mg/kg, 44.2mg/kg, 41.0mg/kg, 42.3mg/kg and 10.8 mg/kg.
2. Preparation of activated carbon based monatomic iron catalyst
(1) Dissolving ferric acetate (0.0435g) and 1, 10-phenanthroline (0.1485g) in an ethanol solution (100mL), uniformly mixing, adding activated carbon powder (1.5g), heating at 60 ℃, stirring, and evaporating ethanol to dryness (4h) in the heating and stirring process to obtain a dried sample;
(2) and (3) carrying out high-temperature calcination on the dried sample, wherein the introduction flow of nitrogen is 30mL/min, heating to 800 ℃ at the heating rate of 10 ℃/min in the high-temperature calcination process, calcining for 2.0h, naturally cooling, and then carrying out acid washing and drying on the calcined sample to obtain the activated carbon-based monatomic iron material.
3. Oxidation repair method
(1) Under the oscillation condition that the oscillation speed is 250 revolutions per minute, 0.1g of activated carbon-based monatomic iron catalyst, 5mL of water and 1% of sodium persulfate are respectively and sequentially added into 10g of polycyclic aromatic hydrocarbon-polluted soil.
(2) The soil mixture is controlled at the temperature of 25 ℃ and subjected to oscillation reaction for 2 hours at the oscillation speed of 250 revolutions per minute.
(3) And placing the reacted soil mixture in a centrifuge, centrifuging for 10min at the rotation speed of 4000 revolutions per minute, and removing the supernatant to obtain the repaired soil.
(4) The contents of naphthalene, acenaphthene, fluorene, phenanthrene and benzo (a) pyrene in the treated soil are respectively 10.3mg/kg, 18.5mg/kg, 10.4mg/kg, 7.2mg/kg and 4.2mg/kg, and the removal rate of polycyclic aromatic hydrocarbon in the soil by the catalytic oxidation system is 79.8%.
Example 3:
1. soil source and pollutant content
The soil is original soil of a site polluted by certain polycyclic aromatic hydrocarbon, wherein the contents of naphthalene, acenaphthene, fluorene, phenanthrene and benzo (a) pyrene are respectively 105mg/kg, 44.2mg/kg, 41.0mg/kg, 42.3mg/kg and 10.8 mg/kg.
2. Preparation of activated carbon based monatomic iron catalyst
(1) Dissolving ferric acetate (0.0435g) and 1, 10-phenanthroline (0.1485g) in an ethanol solution (100mL), uniformly mixing, adding activated carbon powder (2.0g), heating at 60 ℃, stirring, and evaporating ethanol to dryness (4h) in the heating and stirring process to obtain a dried sample;
(2) and (3) carrying out high-temperature calcination on the dried sample, wherein the introduction flow of nitrogen is 30mL/min, heating to 900 ℃ at the heating rate of 10 ℃/min in the high-temperature calcination process, calcining for 2.0h, naturally cooling, and then carrying out acid washing and drying on the calcined sample to obtain the activated carbon-based monatomic iron material.
3. Oxidation repair method
(1) Under the oscillation condition that the oscillation speed is 250 revolutions per minute, 0.1g of activated carbon-based monatomic iron catalyst, 5mL of water and 1% of sodium persulfate are respectively and sequentially added into 10g of polycyclic aromatic hydrocarbon-polluted soil.
(2) The soil mixture is controlled at the temperature of 25 ℃ and subjected to oscillation reaction for 2 hours at the oscillation speed of 250 revolutions per minute.
(3) And placing the reacted soil mixture in a centrifuge, centrifuging for 10min at the rotation speed of 4000 revolutions per minute, and removing the supernatant to obtain the repaired soil.
(4) The contents of naphthalene, acenaphthene, fluorene, phenanthrene and benzo (a) pyrene in the treated soil are respectively 27.4mg/kg, 20.9mg/kg, 12.7mg/kg, 12.8mg/kg and 8.9mg/kg, and the removal rate of polycyclic aromatic hydrocarbon in the soil by the catalytic oxidation system is 66.0%.
Example 4:
1. soil source and pollutant content
The soil is original soil of a site polluted by certain polycyclic aromatic hydrocarbon, wherein the contents of naphthalene, acenaphthene, fluorene, phenanthrene and benzo (a) pyrene are respectively 105mg/kg, 44.2mg/kg, 41.0mg/kg, 42.3mg/kg and 10.8 mg/kg.
2. Preparation of activated carbon based monatomic iron catalyst
(1) Dissolving ferric acetate (0.0435g) and 1, 10-phenanthroline (0.1485g) in an ethanol solution (100mL), uniformly mixing, adding activated carbon powder (1.0g), heating at 60 ℃, stirring, and evaporating ethanol to dryness (4h) in the heating and stirring process to obtain a dried sample;
(2) and (3) carrying out high-temperature calcination on the dried sample, wherein the introduction flow of nitrogen is 30mL/min, heating to 600 ℃ at the heating rate of 10 ℃/min in the high-temperature calcination process, calcining for 2.0h, naturally cooling, and then carrying out acid washing and drying on the calcined sample to obtain the activated carbon-based monatomic iron material.
3. Oxidation repair method
(1) Under the oscillation condition that the oscillation speed is 250 revolutions per minute, 0.1g of activated carbon-based monatomic iron catalyst, 5mL of water and 1% of sodium persulfate are respectively and sequentially added into 10g of polycyclic aromatic hydrocarbon-polluted soil.
(2) The soil mixture is controlled at the temperature of 25 ℃ and subjected to oscillation reaction for 2 hours at the oscillation speed of 250 revolutions per minute.
(3) And placing the reacted soil mixture in a centrifuge, centrifuging for 10min at the rotation speed of 4000 revolutions per minute, and removing the supernatant to obtain the repaired soil.
(4) The contents of naphthalene, acenaphthene, fluorene, phenanthrene and benzo (a) pyrene in the treated soil are respectively measured to be 44.8mg/kg, 35.8mg/kg, 25.4mg/kg, 20.7mg/kg and 7.1mg/kg, and the removal rate of polycyclic aromatic hydrocarbon in the soil by the catalytic oxidation system is 45.0%.
Example 5:
1. soil source and pollutant content
The soil is original soil of a site polluted by certain polycyclic aromatic hydrocarbon, wherein the contents of naphthalene, acenaphthene, fluorene, phenanthrene and benzo (a) pyrene are respectively 105mg/kg, 44.2mg/kg, 41.0mg/kg, 42.3mg/kg and 10.8 mg/kg.
2. Preparation of activated carbon based monatomic iron catalyst
(1) Dissolving ferric acetate (0.0435g) and 1, 10-phenanthroline (0.1485g) in an ethanol solution (100mL), uniformly mixing, adding activated carbon powder (3.0g), heating at 60 ℃, stirring, and evaporating ethanol to dryness (12h) in the heating and stirring process to obtain a dried sample;
(2) and (3) carrying out high-temperature calcination on the dried sample, wherein the introduction flow of nitrogen is 60mL/min, heating to 500 ℃ at the heating rate of 10 ℃/min in the high-temperature calcination process, calcining for 2.5h, naturally cooling, and then carrying out acid washing and drying on the calcined sample to obtain the activated carbon-based monatomic iron material.
3. Oxidation repair method
(1) Under the oscillation condition that the oscillation speed is 250 revolutions per minute, 0.2g of activated carbon-based monatomic iron catalyst, 5mL of water and 1% of sodium persulfate are respectively and sequentially added into 10g of polycyclic aromatic hydrocarbon-polluted soil.
(2) The soil mixture is controlled at the temperature of 25 ℃ and subjected to oscillation reaction for 2 hours at the oscillation speed of 250 revolutions per minute.
(3) And placing the reacted soil mixture in a centrifuge, centrifuging for 10min at the rotation speed of 4000 revolutions per minute, and removing the supernatant to obtain the repaired soil.
(4) The contents of naphthalene, acenaphthene, fluorene, phenanthrene and benzo (a) pyrene in the treated soil are respectively 21.3mg/kg, 10.4mg/kg, 9.5mg/kg, 18.4mg/kg and 9.1mg/kg, and the removal rate of polycyclic aromatic hydrocarbon in the soil by the catalytic oxidation system is 71.8%.
The invention and its embodiments have been described above, without limitation, and the embodiments shown in the drawings are only one of the embodiments of the invention, and the actual structure is not limited thereto. In summary, those skilled in the art should appreciate that they can readily use the disclosed conception and specific embodiments as a basis for designing or modifying other structures for carrying out the same purposes of the present invention without departing from the spirit and scope of the invention as defined by the appended claims.
Claims (5)
1. A preparation method of an activated carbon-based monatomic iron catalyst is characterized by comprising the following steps: the preparation method of the activated carbon-based monatomic iron catalyst comprises the following steps;
step one, dissolving ferric acetate and 1, 10-phenanthroline in an ethanol solution, uniformly mixing, adding activated carbon powder, heating and stirring, and evaporating ethanol to dryness in the heating and stirring process to obtain a dried sample;
and step two, calcining the dried sample at high temperature, and then carrying out acid washing and drying to obtain the activated carbon-based monatomic iron material.
2. The method for preparing an activated carbon-based monatomic iron catalyst according to claim 1, wherein: the mass ratio of the addition amounts of the iron acetate, the 1, 10-phenanthroline and the activated carbon is 1: (3-4): (25-50).
3. The method for preparing an activated carbon-based monatomic iron catalyst according to claim 1, wherein: in the heating and stirring process, the heating temperature is 60-80 ℃, and the stirring time is 4-12 h.
4. The method for preparing an activated carbon-based monatomic iron catalyst according to claim 1, wherein: and in the high-temperature calcination process, introducing nitrogen for protection, wherein the introduction flow of the nitrogen is 30-60 mL/min.
5. The method for preparing an activated carbon-based monatomic iron catalyst according to claim 1, wherein: in the high-temperature calcination process: firstly, the temperature is raised to 500-800 ℃ at a rate of 5-15 ℃/min and calcined for 1.5-2.5 h.
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| CN114849708A (en) * | 2022-06-10 | 2022-08-05 | 苏州大学 | Three-dimensional macroporous carbon anchored monatomic iron catalyst, and preparation method and application thereof |
| CN116832810A (en) * | 2023-05-25 | 2023-10-03 | 广东工业大学 | Preparation method of iron single-atom catalyst for activating persulfate to generate singlet oxygen and application of iron single-atom catalyst in degrading new pollutants in water body |
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| CN114849708A (en) * | 2022-06-10 | 2022-08-05 | 苏州大学 | Three-dimensional macroporous carbon anchored monatomic iron catalyst, and preparation method and application thereof |
| CN114849708B (en) * | 2022-06-10 | 2023-11-03 | 苏州大学 | Three-dimensional macroporous carbon anchored monoatomic iron catalyst and preparation method and application thereof |
| CN116832810A (en) * | 2023-05-25 | 2023-10-03 | 广东工业大学 | Preparation method of iron single-atom catalyst for activating persulfate to generate singlet oxygen and application of iron single-atom catalyst in degrading new pollutants in water body |
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