CN115636526A - Organic pollutant migration and conversion method based on Fe redox enhancement - Google Patents
Organic pollutant migration and conversion method based on Fe redox enhancement Download PDFInfo
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Abstract
The invention discloses a method for migration and conversion of organic pollutants based on Fe redox enhancement, and belongs to the field of environmental pollution monitoring and restoration. The method comprises the steps of adding microorganisms and a carbon source into a medium containing organic pollutants and iron, and sequentially carrying out anaerobic culture and aerobic culture; the microorganism comprises Shewanella Oneidensis MR-1 Shewanella, is purchased from China center for type culture Collection, and has a collection number of CCTCC AB 2013238; the method provided by the invention regulates and controls the Fe redox process by Fe and microorganisms and providing microorganism growth conditions, so as to strengthen the migration and transformation processes of organic pollutants, and has great application potential in the fields of regulating and controlling the migration and transformation of organic pollutants in medium environments such as field soil, water and the like and controlling the diffusion of organic pollutants.
Description
Technical Field
The invention relates to a method for migration and transformation of organic pollutants based on Fe redox enhancement, belongs to the field of migration and transformation of environmental pollution, and is mainly used for monitoring and repairing soil-water and other multi-medium environmental organic pollutants.
Background
Persistent organic pollutants such as Polycyclic Aromatic Hydrocarbons (PAHs), petroleum hydrocarbons and the like are pollutants which are widely detected in the environments such as soil, sediments, water and the like, and mainly come from human production activities, including the discharge of wastes generated in petrochemical production, incomplete combustion of fossil fuels and the like. Persistent organic pollutants in the environment have the effects of carcinogenesis, teratogenesis, mutagenesis and the like, and pose potential threats to human health. The migration and transformation of persistent organic pollutants and pollution monitoring are important environmental problems related to human health and sustainable development of an ecosystem.
The migration and conversion of persistent organic pollutants relate to physical, chemical and microbial processes, but the migration and conversion efficiency of single physical treatment is low, the chemical oxidation cost is high, the microbial conversion degradation activity is low, and the like.
The prior art with Chinese patent application publication No. CN112872012A discloses a method for removing petroleum hydrocarbon in soil by electrochemical reinforced persulfate oxidation synergy. According to the method, a surfactant is injected into contaminated soil in a cathode transmission mode under the action of an electric field, when contaminants in the soil are migrated and enriched in an advanced oxidation filling area, an inert anode is taken out and inserted into an Fe anode in situ, and meanwhile, the inert anode moves to the anode from the inert cathode according to the migration condition of the contaminants in the soil, and then the inert anode is electrified to continue oxidative degradation until the degradation of the contaminants reaches a required value. The invention has universality, is suitable for various types of organic polluted soil and fields, and is also suitable for low-permeability and barren soil. However, the method for enhancing the pollutant migration and chemical oxidation conversion degradation by adopting an electric driving mode has high cost and high energy consumption, and is difficult to be applied to the in-situ treatment of large-area polluted soil bodies.
Disclosure of Invention
1. Problems to be solved
Aiming at the defects of low organic pollutant migration and conversion efficiency, high cost, large energy consumption and the like in the prior art, the invention provides a Fe redox-enhanced organic pollutant migration and conversion method, which increases the dissolution and migration capacity of organic pollutants by regulating the redox state of Fe by using microorganisms, and further increases the dissolution and migration capacity of the organic pollutants by using active oxygen hydrogen peroxide H generated in aerobic culture of the microorganisms 2 O 2 And hydroxyl radical · OH is oxidized and degraded, so that the enhanced migration and conversion of organic pollutants are realized.
2. Technical scheme
A method for transferring and transforming organic pollutants based on Fe redox enhancement comprises the steps of adding microorganisms and a carbon source into a medium containing the organic pollutants and iron, and sequentially carrying out anaerobic culture and aerobic culture; the microorganism comprises Shewanella Oneidensis MR-1 Shewanella, is purchased from China center for type culture Collection, and has a collection number of CCTCC AB 2013238; the medium containing organic pollutants and iron comprises a medium formed by adding iron or an iron-containing medium to a medium containing organic pollutants, or a medium formed by adding organic pollutants to an iron-containing medium, or an iron-containing medium polluted by organic pollutants. The Shewanella Oneidensis MR-1 Shewanella is a Shewanella facultative anaerobe and can anaerobically reduce Fe (III) into Fe (II).
Preferably, the iron-containing medium comprises one or more of iron-containing soil, naturally-formed or artificially-synthesized iron-containing minerals, or a mixed system formed by artificially and externally adding iron-containing compounds. Wherein the iron-containing mineral can be goethite (iron content is 30-63% in general), hematite, lepidocrocite, ferrihydrite, magnetite, etc.
Preferably, the organic contaminants include one or more of polycyclic aromatic hydrocarbons, chlorinated hydrocarbons, petroleum hydrocarbons, benzene series, and the like. Wherein the polycyclic aromatic hydrocarbon comprises phenanthrene and pyrene.
Preferably, the method comprises the following steps:
s1, culturing and expanding the Shewanella Oneidensis MR-1 Shewanella by using a sterilized nutrient broth culture medium, and then adjusting the number or density of bacteria to a specific value;
s2, adding an iron-containing compound into a medium containing organic pollutants, adding the medium into a sterilized inorganic salt medium, and then inoculating Shewanella Oneidensis MR-1 Shewanella and a carbon source in the step S1; or
Adding a sterilized inorganic salt culture medium into an iron-containing medium, then inoculating Shewanella Oneidensis MR-1 Shewanella in the step S1 and a carbon source, and then adding an organic pollutant for mixing; or
Adding a sterilized inorganic salt medium to an iron-containing medium contaminated with organic contaminants, followed by inoculation of the Shewanella Oneidensis MR-1 Shewanella and a carbon source of step S1;
s3, anaerobic culture: introducing nitrogen into the mixed system obtained in the step S2 to remove oxygen, sealing and culturing under anaerobic conditions; during the anaerobic culture, shewanella Oneidensis MR-1 Shewanella reduces iron;
s4, aerobic culture: after the anaerobic culture in the step S3 is finished, the reaction system is cultured under a shaking aerobic condition; h production by Shewanella Oneidensis MR-1 Shewanella during aerobic culture 2 O 2 Further generate · OH； · OH attacks the surface of the medium to adsorb or dissolve organic pollutants so as to strengthen the degradation and conversion of the organic pollutants;
s5, sequentially repeating the steps of anaerobic culture and aerobic culture of the S3 and the S4, and circularly culturing; until the organic pollutants in the system are completely converted and degraded;
s6, supplementing a carbon source in the anaerobic culture and aerobic culture processes. The carbon source is appropriately supplemented depending on the consumption.
The method regulates and controls the reduction and oxidation of a medium containing Fe in the anaerobic/aerobic respiration process through Shewanella Oneidensis MR-1 Shewanella to generate Fe (II) and hydrogen peroxide H 2 O 2 On one hand, the reduction and dissolution of the iron-containing medium change the state of the medium, so that the organic pollutants adsorbed and fixed on the surface or in the medium are released into the surrounding environment, and the migration activity of the organic pollutants is enhanced; on the other hand, fe (II) and hydrogen peroxide H generated in the reduction and oxidation process of the Fe-containing medium 2 O 2 Can further react to generate hydroxyl free radical · OH， · OH attacks the surface of the medium to adsorb or dissolve organic pollutants so as to strengthen the degradation and conversion of the organic pollutants.
Preferably, the Shewanella Oneidensis MR-1 Shewanella propagation conditions include: aerobic culture, inoculating proper amount of bacteria liquid into a sterilized nutrient broth culture medium, and culturing overnight at 30 ℃ and 160rpm in a dark place; washing twice with sterilized phosphate buffer solution (pH7.0.1M) to adjust bacterial density to OD 600 ＝1.20。
Preferably, the solid-liquid mass ratio of the iron-containing medium or the iron-containing medium polluted by organic pollutants to the inorganic salt medium in the reaction systems of the steps S2 to S4 is 1 (20 to 100), and OD is obtained after Shewanella Oneidensis MR-1 Shewanella inoculation dilution 600 Not less than 0.05.
Preferably, the nitrogen is introduced for not less than 15min in the anaerobic culture in the step S3, so that the aim of completely removing oxygen in the system is fulfilled; the anaerobic culture time is not less than 24h to fully reduce and generate Fe (II).
Preferably, the aerobic culture time in the step S4 is 3-8 h. Aerobic culture for generating active oxygen hydrogen peroxide H 2 O 2 And hydroxyl radical · OH。
Preferably, the total number of times of the cyclic cultivation in the step S5 is not less than 3 times.
Preferably, the carbon source in step S2 is selected from one or more of lactate, citrate, pyruvate and the like; the concentration is 10-500 mM.
3. Advantageous effects
Compared with the prior art, the invention has the beneficial effects that:
(1) According to the invention, aiming at organic pollutants, especially polycyclic aromatic hydrocarbons, the steps of anaerobic culture (reduction process) and aerobic culture (oxidation process) of Shewanella Oneidensis MR-1 Shewanella and iron are cooperated to be sequentially circulated for multiple times are adopted, fe (III)/Fe (II) can be circularly generated under the condition of iron oxidation reduction, and meanwhile, shewanella Oneidensis MR-1 Shewanella generates H under the condition of aerobic 2 O 2 The above anaerobic and aerobic processes have a great influence on the migration and transformation of organic pollutants; fe (II) and H 2 O 2 Can produce an interaction between · Active oxygen such as OH enables organic pollutants to be efficiently oxidized; fe is the fourth major element in the earth crust, the content of Fe is rich in soil and water media, the redox cycle of Fe is related to various biogeochemical processes, and the Fe plays an important role in the process of pollutant migration and conversion; in a soil-groundwater redox wave environment, the interaction of microorganisms with iron-containing minerals has a significant effect on the generation of active oxygen.
(2) Aiming at iron-containing media such as iron-containing minerals polluted by organic pollutants, the method utilizes Shewanella Oneidensis MR-1 Shewanella to regulate and control the reduction and oxidation of iron in the iron-containing minerals, changes the state of the minerals, releases the organic pollutants along with the reduction and dissolution of the media such as the iron-containing minerals and the like, is further oxidized, degraded and converted by active oxygen, and achieves the purpose of strengthening the migration and conversion of the organic pollutants; the iron-containing mineral has a prominent effect on the migration and transformation of organic pollutants, probably because the iron-containing mineral is an adsorption and fixation medium of the organic pollutants, and the adsorption and dissolution states of the organic pollutants are regulated and controlled through the change of the valence state of the iron-containing mineral, so that the migration activity of the organic pollutants is influenced and changed; the iron-containing mineral can stimulate and promote microorganism growth and metabolism, and promote migration and transformation of organic pollutants.
Drawings
FIG. 1 shows the migration and transformation characteristics of Fe-containing minerals redox-enhanced polycyclic aromatic hydrocarbons phenanthrene and pyrene regulated by Shewanella Oneidensis MR-1 Shewanella under anaerobic/aerobic circulation in example 1 of the present invention: a, c: the Fe-containing goethite system phenanthrene and pyrene are converted; b, d: conversion of phenanthrene and pyrene in a kaolinite control system without Fe;
FIG. 2 is a graph showing the concentration of Fe (II) produced by the Fe-containing goethite system at the end of the anaerobic/aerobic cyclic anaerobic culture in example 2 of the present invention;
FIG. 3 is a diagram showing the end of anaerobic/aerobic circulating aerobic culture H in example 2 of the present invention 2 O 2 The concentration variation characteristic of (a): a: an Fe-containing goethite system; b: no Fe kaolinite control system;
FIG. 4 shows the formation of the 4 th anaerobic/aerobic cycle at the end of the aerobic culture in example 2 of the present invention · Concentration profile of OH, a: an Fe-containing goethite system; b: no Fe kaolinite control system.
Detailed Description
Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs; as used herein, the term "and/or" includes any and all combinations of one or more of the associated listed items.
The examples, in which specific conditions are not specified, were conducted under conventional conditions or conditions recommended by the manufacturer. The reagents or instruments used are conventional products which are not indicated by manufacturers and are commercially available.
Concentrations, amounts, and other numerical data may be presented herein in a range format. It is to be understood that such a range format is used merely for convenience and brevity and should be interpreted flexibly to include not only the numerical values explicitly recited as the limits of the range, but also to include all the individual numerical values or sub-ranges encompassed within that range as if each numerical value and sub-range is explicitly recited. For example, a numerical range of about 1 to about 4.5 should be interpreted to include not only the explicitly recited limit values of 1 to about 4.5, but also include individual numbers (such as 2, 3, 4) and sub-ranges (such as 1 to 3, 2 to 4, etc.). The same principle applies to ranges reciting only one numerical value, such as "less than about 4.5," which should be construed to include all of the aforementioned values and ranges. Moreover, such an interpretation should apply regardless of the breadth of the range or feature being described.
The following description of the embodiments of the present invention is provided in connection with the accompanying drawings and examples, but the invention is not limited thereto. It is noted that the processes described below, if not specifically described in detail, are all realizable or understandable by those skilled in the art with reference to the prior art. The reagents or apparatus used are not indicated to the manufacturer, and are considered to be conventional products available by commercial purchase.
By way of example, experiments were conducted in the following examples using goethite as the Fe-containing mineral medium, kaolinite as the Fe-free mineral medium, phenanthrene and pyrene in polycyclic aromatic hydrocarbons as representative organic contaminants, and Shewanella Oneidensis MR-1 Shewanella. The strain is Fe reducing bacteria, is purchased from China center for type culture Collection, has a collection number of CCTCC AB2013238, and is gram-negative bacteria.
Example 1
1. Preparation of polycyclic aromatic hydrocarbon polluted mineral medium
Mixing the polycyclic aromatic hydrocarbon with the mineral, comprising the following steps:
respectively weighing 10g of minerals (goethite, the iron content is about 60 percent; kaolinite, and no iron) in a 100mL glass beaker, adding 10mL of phenanthrene and pyrene mixed solution prepared by acetone, shaking up gently, standing in a fume hood, and preparing the minerals polluted by phenanthrene and pyrene after the acetone is completely volatilized. The content of phenanthrene and pyrene in the polluted minerals are respectively as follows:
goethite: phenanthrene, 346. + -. 25. Mu.g -1 (ii) a Pyrene 328. + -. 11. Mu.g -1 ；∑PAHs，674±27μg g -1 。
Kaolinite: phenanthrene, 258. + -. 31. Mu.g -1 (ii) a Pyrene, 238. + -. 17. Mu.g -1 ；∑PAHs，495±36μg g -1 。
The minerals were ground and sieved through a 60 mesh sieve and stored in brown glass reagent bottles.
2. Culture and propagation of bacterial strain
Activating and propagating the strain, wherein the strain is Shewanella Oneidensis MR-1 Shewanella, is purchased from China center for type culture Collection, and has a collection number of CCTCC AB 2013238. The bacterium is a typical metal-reducing bacterium, and can reduce Fe (III) to generate Fe (II). The activation and propagation comprises the following steps:
thawing degrading bacteria (Shewanella Oneidensis MR-1 Shewanella) preserved in glycerol at-80 deg.C, inoculating into sterilized nutrient broth culture medium at an inoculation ratio of 0.2mL per 100mL culture medium, performing aerobic light-shielding culture at 30 deg.C and 160rpm overnight, taking out when the strain grows to logarithmic phase, centrifuging at 5000rpm in a sterilized centrifuge tube to collect lower layer thallus, adopting sterilized phosphate buffer solution (pH7.0) to obtain supernatant for 2 times, resuspending, and adjusting bacterial density to OD 600 ＝1.20。
3. Microorganism regulation and control Fe-containing medium reduction oxidation enhanced polycyclic aromatic hydrocarbon phenanthrene and pyrene migration transformation
The microorganism-regulated reduction and oxidation strengthening polycyclic aromatic hydrocarbon phenanthrene and pyrene migration transformation of a Fe-containing medium comprises the following steps:
MR-1+ carbon source group: 0.6g of each of the two contaminated minerals was weighed into a 50mL glass centrifuge tube, and 28mL of sterilized inorganic salt medium was added, followed by inoculation of 2mL of prepared Shewanella Oneidensis MR-1 Shewanella bacterial suspension (OD) 600 = 1.20) add 0.12ml 60% lactate as carbon source (final concentration 20 mM). In this experiment, the solid-to-liquid ratio was 1 (1 600 Not less than 0.05.
MR-1 group: treatment with the inoculum strain but without a lactate carbon source (control 1, MR-1) was also set to determine whether Shewanella Oneidensis MR-1 Shewanella can grow and metabolize with PAHs as the sole carbon source.
And (5) CK group: the experiment also set up a treatment without inoculation of Shewanella Oneidensis MR-1 Shewanella (control 2, CK) to exclude the non-bioregulated degradation of mineral system PAHs.
The experimental system is firstly introduced with N 2 Removing oxygen in the solution for 15min, standing at 28 deg.C for anaerobic culture for 40 hr, and performing aerobic culture under shaking for 8 hr, thereby performing anaerobic/aerobic culture cycle.
The anaerobic/aerobic culture cycle was 4 times in this experimental procedure.
And (3) absorbing the sample liquid at the end of each anaerobic/aerobic culture stage to determine the concentrations of phenanthrene and pyrene, and analyzing the migration and transformation characteristics of the phenanthrene and pyrene. Extracting the sample solution with organic solvent, determining the content of the residual phenanthrene and pyrene in the extracting solution by High Performance Liquid Chromatography (HPLC), drawing a conversion kinetic curve (figure 1) of the phenanthrene and pyrene, and calculating the conversion rate of the phenanthrene and pyrene. The results showed that 60% phenanthrene and 48.6% pyrene were degraded and converted after 4 anaerobic/aerobic cycles of culture (192 h) by treatment with MR-1+ carbon source in goethite system (FIG. 1a, c). Although the phenanthrene and pyrene treated by the control are also degraded to some extent, the conversion rate of the phenanthrene and pyrene treated by the MR-1+ carbon source is remarkably improved, but the degradation conversion of the phenanthrene and pyrene treated by inoculating the MR-1 is not different from that of the control. In the kaolinite system, 38.1% phenanthrene and 37.2% pyrene are degraded and converted by the MR-1+ carbon source treatment (figure 1b, d), and compared with the control treatment, the PAHs conversion is not obviously different in the MR-1+ carbon source treatment and the MR-1 treatment, and is even lower than that in the control group 2 treatment (figure 1 b). The results show that the strain MR-1 can not convert PAHs by using PAHs as a sole carbon source and can not convert PAHs by co-metabolism with lactate. Only in the coexistence of Fe and a carbon source, the strain MR-1 can regulate and control the enhanced migration and transformation of PAHs under the aerobic/anaerobic circulating condition of the Fe-containing mineral medium.
Example 2
Microorganism regulation of Fe reduction activity of Fe-containing mineral medium
The research of the microorganism regulation and control of Fe reduction activity of the Fe-containing mineral medium comprises the following steps:
in an anaerobic/aerobic culture system for transferring and converting microorganism-mineral (Shewanella Oneidensis MR-1+ carbon source-mineral) into polycyclic aromatic hydrocarbon by adopting the method of example 1, a sample liquid is sucked at the end of each anaerobic culture stage to measure the content of Fe (II), and the reduction activity of Fe is analyzed. And measuring the generation concentration of Fe (II) in the system at the end of anaerobic culture by adopting phenanthroline. Fe (II) forms a red complex with phenanthroline, with an absorption maximum at 562 nm. Sucking 0.5mL of sample liquid into a 2mL centrifuge tube, adding 0.5mL of 2mM phenanthroline solution, reacting for 5min, fixing the volume to 1.5mL, then centrifuging at 6000r/min for 5min, determining the color of Fe (II) in the supernatant by using an ultraviolet visible spectrophotometer at 562nm wavelength in a colorimetric way, wherein the molar absorption coefficient is 27900M -1 cm -1 . The results show (FIG. 2) that essentially no Fe (II) was detected in the goethite system without Shewanella Oneidensis MR-1 and carbon source addition (control 2); in the treatments (MR-1 and MR-1+ carbon source) inoculated with MR-1, the formation of Fe (II) was observed, and the concentration of Fe (II) was 0.6 to 9.0. Mu.M. It was demonstrated that goethite can be reduced and dissolved by the strain MR-1 to produce Fe (II) under anaerobic culture conditions.
(II) microorganism regulation and control of generation of Fe-containing mineral medium oxidation active substance
The research of the microorganism regulation and control of the generation of the Fe-containing mineral medium oxidation active substance comprises the following steps:
in the anaerobic/aerobic culture system for transferring and converting the polycyclic aromatic hydrocarbon by the microorganism-mineral (Shewanella Oneidensis MR-1+ carbon source-mineral) constructed by the method of the embodiment 1, the hydrogen peroxide H is measured by absorbing the sample liquid at the end of each aerobic culture stage 2 O 2 Content, extracting sample at the end of the last aerobic culture stage to analyze hydroxyl radical · OH content. The specific method comprises the following steps:
(1) Hydrogen peroxide H 2 O 2 Content determination: the specific process is as follows: determination of H generated in system by horseradish peroxidase method 2 O 2 . 0.5mL of the aspirated sample is added to a 2mL centrifuge tube and 0.1mL of 1mg/mL is addedAfter adding 0.5mL of 10mM ABTS solution, the reaction was carried out for 5min, then the volume was adjusted to 1.5mL, and the mixture was centrifuged at 6000r/min for 5min. H 2 O 2 ABTS is oxidized to generate green ABTS under the catalysis of horseradish peroxidase ·+ . ABTS in supernatant after centrifugation of samples ·+ The molar absorbance is 34000M measured at 415nm by colorimetry -1 cm -1 。H 2 O 2 And ABTS ·+ ABTS in stoichiometric ratio of 2 ·+ The concentration is divided by the coefficient 2 to obtain H generated in the solution 2 O 2 The concentration of (c). The results show (fig. 3): in the aerobic culture stage, H can be detected by the goethite and kaolinite system 2 O 2 And (4) generating. In the CK processing and MR-1 processing, only a very small amount of H is detected 2 O 2 Generate (a)<0.3. Mu.M), revealing H in the absence of added carbon source, either sterile or inoculated 2 O 2 The accumulative generation amount of active oxygen is extremely low, and the activity of the reaction microorganism is very low. In the treatment of MR-1+ carbon sources, both mineral systems produce higher concentrations of H 2 O 2 And the cumulative concentration reaches the highest (-40 mu M) after the 2 nd aerobic stage culture, and the phases H in 3 rd and 4 th 2 O 2 The formation concentration decreased sharply (. About.0.64. Mu.M), which is presumably due to the fact that the added lactate concentration of the carbon source was low (20 mM), and the carbon source was consumed after two anaerobic/aerobic cycles of cultivation (96H), resulting in a decrease in aerobic respiration activity and further H in the subsequent cultivation 2 O 2 The yield decreases.
(2) Hydroxyl radical · And (3) OH content determination: the specific process is as follows: using coumarin as probe for determining formation of coumarin at the end of aerobic culture in system · The concentration of OH. Mixing 0.5mL of sample solution with 0.5mL of 2mM coumarin, aerobic culturing for 2h, and adding 0.5mL of methanol to terminate the reaction when the culture is finished. And then centrifuging the mixed solution at 6000r/min for 5min, and measuring an oxidation product 7-hydroxycoumarin by adopting an HPLC-fluorescence detection system after the supernate passes through a 0.22 mu m filter membrane. The concentration of 7-hydroxycoumarin is calculated by a standard curve of 0.005-1 mu M, and the detection limit of the method is 0.0032 mu M. Generated by · OH concentration was calculated by dividing 7-hydroxycoumarin concentration by a factor of 14.5%And obtaining the product. The results show (fig. 4): detected in all processes · OH, the content of which is between 0.008 MuM and 0.54 MuM. In control treatment · The formation of OH reveals the possible presence of non-biological transformations of contaminants of the mineral system. In the research result, the reduction of the concentrations of phenanthrene and pyrene in CK treatment proves the non-biotransformation degradation of the mineral system PAHs. In the microbial treatment, only the treatment of inoculating MR-1 · The production of OH was minimal and even less than the control treatment. This is because the aerobic respiration activity of the microorganism of the strain MR-1 is very low without an additional carbon source, as compared with Fe (II) and H in the above 2 O 2 The result is consistent with low activity, resulting in the failure of MR-1 to regulate · OH is produced and affects abiotic factors · And (4) generation of OH. MR-1 regulated production of large quantities in the presence of carbon sources · OH, which is reduced by anaerobic respiration to form Fe (II) and aerobic respiration to form H 2 O 2 In connection with the reaction of the two to form · OH, thereby converting organic pollutants such as phenanthrene and pyrene in mineral systems.
The results show that the microbial regulation of the reduction and oxidation processes of Fe (III)/Fe (II) can cause the reduction dissolution of Fe-containing mineral medium and release of organic pollutants, and the Fe-containing mineral medium is subjected to active oxygen H in the subsequent aerobic culture process 2 O 2 And · OH attacks and converts and degrades, thereby realizing the enhanced migration and conversion of organic pollutants. Experiments show that the Fe-based oxidation-reduction process has important influence on the migration and transformation process and pollution distribution of organic pollutants in environmental media such as soil-water and the like, and has better application potential in the aspect of field organic pollution control.
The above examples are only preferred embodiments of the present invention, which are intended to be illustrative and not limiting, and those skilled in the art should understand that they can make various changes, substitutions and alterations without departing from the spirit and scope of the invention.
Claims (10)
1. A method for transferring and transforming organic pollutants based on Fe redox enhancement is characterized in that microorganisms and a carbon source are added into a medium containing the organic pollutants and iron, and the steps of anaerobic culture and aerobic culture are sequentially carried out; the microorganism comprises Shewanella Oneidensis MR-1 Shewanella, is purchased from China center for type culture Collection, and has a collection number of CCTCC AB 2013238; the medium containing organic pollutants and iron comprises a medium formed by adding iron or an iron-containing medium to a medium containing organic pollutants, or a medium formed by adding a medium containing organic pollutants to an iron-containing medium, or an iron-containing medium polluted by organic pollutants.
2. The Fe redox-enhanced organic pollutant migration and conversion method based on claim 1, characterized in that the iron-containing medium comprises one or more of iron-containing soil, naturally-formed or artificially-synthesized iron-containing minerals, or a mixed system formed by artificially and externally adding iron-containing compounds.
3. The Fe-based redox enhanced migratory conversion of organic contaminants as claimed in claim 2, wherein said organic contaminants include one or more of polycyclic aromatic hydrocarbons, chlorinated hydrocarbons, petroleum hydrocarbons, benzene series, etc.
4. The method for the Fe redox-enhanced migratory conversion of organic pollutants as claimed in claim 1, comprising the steps of:
s1, culturing and expanding the Shewanella Oneidensis MR-1 Shewanella by using a sterilized nutrient broth culture medium, and then adjusting the number or density of bacteria to a specific value;
s2, adding an iron-containing compound into a medium containing organic pollutants, adding the medium into a sterilized inorganic salt medium, and then inoculating Shewanella Oneidensis MR-1 Shewanella and a carbon source in the step S1; or
Adding a sterilized inorganic salt culture medium into an iron-containing medium, then inoculating Shewanella Oneidensis MR-1 Shewanella in the step S1 and a carbon source, and then adding an organic pollutant for mixing; or
Adding a sterilized mineral salt medium to an iron-containing medium contaminated with organic contaminants, followed by inoculation with Shewanella Oneidensis MR-1 Shewanella and a carbon source as described in step S1;
s3, anaerobic culture: introducing nitrogen into the mixed system obtained in the step S2 to remove oxygen, sealing and culturing under anaerobic conditions;
s4, aerobic culture: after the anaerobic culture in the step S3 is finished, the reaction system is changed to culture under a shaking aerobic condition;
s5, sequentially repeating the steps of anaerobic culture and aerobic culture of the S3 and the S4, and circularly culturing;
s6, supplementing a carbon source in the anaerobic culture and aerobic culture processes.
5. The method for Fe redox-enhanced organic pollutant migration and transformation based on claim 4, characterized in that the Shewanella Oneidensis MR-1 Shewanella propagation conditions comprise: aerobic culture, inoculating a proper amount of bacterial liquid in a sterilized nutrient broth culture medium, and culturing overnight at 30 ℃ and 160rpm in a dark condition; washing twice with sterilized phosphate buffer solution (pH7.0.1M) to adjust bacterial density to OD 600 ＝1.20。
6. The method for Fe redox-enhanced organic pollutant migration and conversion based on the step S2-S4 reaction system is characterized in that the solid-liquid mass ratio of the iron-containing medium or the iron-containing medium polluted by the organic pollutants to the inorganic salt medium in the step S2-S4 reaction system is 1 (20-100), OD is obtained after Shewanella Oneidensis MR-1 Shewanella inoculation dilution 600 Not less than 0.05.
7. The method for migration and transformation of organic pollutants based on Fe redox enhancement as claimed in claim 4, wherein the anaerobic cultivation in the step S3 is not less than 15min and not less than 24h.
8. The method for migration and transformation of organic pollutants based on Fe redox enhancement as claimed in claim 4, characterized in that the aerobic cultivation time in step S4 is 3-8 h.
9. The method for migration and transformation of organic pollutants based on Fe redox enhancement according to any one of claims 4 to 8, characterized in that the total number of times of cyclic culture in step S5 is not less than 3 times.
10. The Fe redox-enhanced organic pollutant migration conversion method based on the claim 4, characterized in that the carbon source in the step S2 is selected from one or more of lactate, citrate and pyruvate; the concentration is 10-500 mM.
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| CN114703104A (en) * | 2022-04-29 | 2022-07-05 | 暨南大学 | Bacterial strain with iron reduction capacity and electrochemical activity and application thereof |
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| US6627428B1 (en) * | 1999-09-24 | 2003-09-30 | Georgia Tech Research Corp. | Degradation of organic contaminants by a microbially-driven fenton reaction |
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