CN107308949B - Preparation method of magnetic biological iron-manganese oxide capable of degrading single benzene ring pollutant - Google Patents
Preparation method of magnetic biological iron-manganese oxide capable of degrading single benzene ring pollutant Download PDFInfo
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- 238000002360 preparation method Methods 0.000 title claims abstract description 13
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- 239000001110 calcium chloride Substances 0.000 claims description 2
- 229910001628 calcium chloride Inorganic materials 0.000 claims description 2
- 150000001875 compounds Chemical class 0.000 claims description 2
- ZPWVASYFFYYZEW-UHFFFAOYSA-L dipotassium hydrogen phosphate Chemical compound [K+].[K+].OP([O-])([O-])=O ZPWVASYFFYYZEW-UHFFFAOYSA-L 0.000 claims description 2
- 229960004642 ferric ammonium citrate Drugs 0.000 claims description 2
- 239000004313 iron ammonium citrate Substances 0.000 claims description 2
- 235000000011 iron ammonium citrate Nutrition 0.000 claims description 2
- 229910052943 magnesium sulfate Inorganic materials 0.000 claims description 2
- 235000019341 magnesium sulphate Nutrition 0.000 claims description 2
- 239000011656 manganese carbonate Substances 0.000 claims description 2
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- 229910000016 manganese(II) carbonate Inorganic materials 0.000 claims description 2
- SQQMAOCOWKFBNP-UHFFFAOYSA-L manganese(II) sulfate Chemical compound [Mn+2].[O-]S([O-])(=O)=O SQQMAOCOWKFBNP-UHFFFAOYSA-L 0.000 claims description 2
- XMWCXZJXESXBBY-UHFFFAOYSA-L manganese(ii) carbonate Chemical group [Mn+2].[O-]C([O-])=O XMWCXZJXESXBBY-UHFFFAOYSA-L 0.000 claims description 2
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- 230000007935 neutral effect Effects 0.000 claims description 2
- 229910052755 nonmetal Inorganic materials 0.000 claims description 2
- 235000019319 peptone Nutrition 0.000 claims description 2
- 235000010344 sodium nitrate Nutrition 0.000 claims description 2
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- 238000012258 culturing Methods 0.000 claims 1
- 229910000396 dipotassium phosphate Inorganic materials 0.000 claims 1
- 235000019797 dipotassium phosphate Nutrition 0.000 claims 1
- 239000002054 inoculum Substances 0.000 claims 1
- 230000001590 oxidative effect Effects 0.000 claims 1
- LWIHDJKSTIGBAC-UHFFFAOYSA-K potassium phosphate Substances [K+].[K+].[K+].[O-]P([O-])([O-])=O LWIHDJKSTIGBAC-UHFFFAOYSA-K 0.000 claims 1
- 230000000694 effects Effects 0.000 abstract description 9
- 239000002351 wastewater Substances 0.000 abstract description 4
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- 108030000088 Manganese oxidases Proteins 0.000 abstract description 2
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- 230000004913 activation Effects 0.000 abstract 1
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- RZVAJINKPMORJF-UHFFFAOYSA-N Acetaminophen Chemical compound CC(=O)NC1=CC=C(O)C=C1 RZVAJINKPMORJF-UHFFFAOYSA-N 0.000 description 13
- KJCVRFUGPWSIIH-UHFFFAOYSA-N 1-naphthol Chemical compound C1=CC=C2C(O)=CC=CC2=C1 KJCVRFUGPWSIIH-UHFFFAOYSA-N 0.000 description 10
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- 239000000243 solution Substances 0.000 description 7
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- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 1
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/84—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/889—Manganese, technetium or rhenium
- B01J23/8892—Manganese
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
- B01J35/33—Electric or magnetic properties
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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
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- C—CHEMISTRY; METALLURGY
- C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
- C12P—FERMENTATION OR ENZYME-USING PROCESSES TO SYNTHESISE A DESIRED CHEMICAL COMPOUND OR COMPOSITION OR TO SEPARATE OPTICAL ISOMERS FROM A RACEMIC MIXTURE
- C12P3/00—Preparation of elements or inorganic compounds except carbon dioxide
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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
- C02F2101/34—Organic compounds containing oxygen
- C02F2101/345—Phenols
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Abstract
The invention provides a preparation method of a magnetic biological iron-manganese oxide capable of degrading single benzene ring pollutants. The method comprises the steps of providing a specific culture environment for Pseudomonas putida, inducing Pseudomonas putida manganese oxidase to oxidize Mn2+ to prepare a manganese oxide material, and interacting with a nano magnetic core to form a wrapped mosaic structure in the formation process of the manganese oxide to generate the biological iron manganese oxide with superparamagnetism. The invention has obvious effect on degrading the single benzene ring organic wastewater. The single benzene ring pollutant can be efficiently and biologically degraded under the condition of no exogenous chemical substance, the good magnetic stability is favorable for recycling, the activation effect is still good after the pollutant is repeatedly degraded for many times, and the material is a green and environment-friendly material and has wide application prospect in the aspect of degrading organic pollutants in water.
Description
Technical Field
The invention belongs to the field of biomass processing, and particularly relates to a preparation method and application of a magnetic biological iron-manganese oxide capable of degrading single benzene ring pollutants.
Background
In recent years, some emerging pollutants, namely single benzene ring pollutants, appear in water environments, the compounds and the metabolites thereof are continuously discharged into various environment media such as surface water, underground water and soil, and the continuous existing state can cause potential harm to aquatic ecosystems and human bodies through complex interaction among various species. These single benzene ring contaminants are frequently detected in the environment, are difficult to biodegrade, and remain in the environment at concentrations that are highly acute toxic to organisms in water. Some single benzene ring pollutants can generate drug-resistant pathogens in the environment, which can not only cause harm to the health safety of human bodies, but also cause adverse effects on the growth of vertebrates and fishes on land. The method for removing the single benzene ring pollutants comprises the following steps: the method comprises the following steps of a traditional treatment method, an oxidation method, an adsorption method, an electrochemical treatment method, a thin film method, an ultrasonic method, a microbial degradation method and the like, wherein the microbial degradation method is economical and safe, the threshold value of pollutants to be treated is low, the residues are few, secondary pollution to the environment cannot be caused, and the application prospect is good.
Magnetic nanomaterials are a new class of functional materials with properties that differ from conventional magnetic materials in that, in relation to the fact that the characteristic physical length associated with magnetism is well on the order of nanometers, magnetic nanomaterials, due to their small size, often exhibit superparamagnetism: i.e. no magnetism when no external magnetic field is acting; when an external magnetic field acts, the magnetic field is easy to be magnetized; after the external magnetic field is removed, the external magnetic field can be demagnetized in a short time, hysteresis is avoided, and the coercive force is zero. The magnetic nano material is added into the solution, and under the action of an external magnetic field, the magnetic nano material is easy to separate from the aqueous solution, and can be recycled for repeated use. Some nanomaterials also exhibit better contaminant degradation characteristics, e.g., nanoscale zero-valent iron can adsorb some organic contaminants (chloride solvents, etc.) to the surface or reduce them to products with relatively lower toxicity. The magnetic material has the characteristics of easy recovery and recycling, so that the magnetic material has better application prospect in the field of organic wastewater purification.
Disclosure of Invention
The invention aims to provide a specific culture environment for Pseudomonas putida, induce Pseudomonas putida manganese oxidase to oxidize Mn2+ to prepare a manganese oxide material, form a wrapped mosaic structure with a nano magnetic core in the process of manganese oxide formation, generate a biological iron manganese oxide with superparamagnetism, degrade and remove residual single benzene ring non-steroid medicines in a water environment, and further achieve the purpose of purifying a water body, so that the water quality can reach the national relevant specified discharge standard, and reduce pollution to the ecological environment and harm to human.
In order to achieve the purpose, the invention adopts the following technical scheme.
A preparation method of a magnetic biological iron-manganese oxide capable of degrading single benzene ring pollutants comprises the following steps:
(1) preparation of biological manganese oxide: inoculating dry powder of a strain Psuedonomas putida (strain accession number) into a PYCM culture medium sterilized by a high-pressure steam sterilizer at 121 ℃ for 20min at an inoculation amount of 1% (m/v), and performing shake culture in a constant-temperature gas bath shaker at 25 ℃ for 24h at a rotating speed of 125r/min until black granular precipitates are generated; inoculating the activated culture into a fermentation tank with sterile aeration and stirring functions in an inoculation amount of 1%, wherein the volume of a PYCM culture medium in the tank is 2/3 of the volume of the fermentation tank, and sterilizing at 121 ℃ for 20min and then pouring;
(2) preparing magnetic biological manganese oxide: when the activated culture is inoculated into a fermentation tank, magnetic nano Fe subjected to high-temperature sterilization is added at the same time3O4The adding amount is 0.5g/L, and the nano Fe is quickly added in a uniform aeration mode3O4The particles are uniformly dispersed. Under the conditions of continuous stirring and aeration at the temperature of 25 ℃, black particles with the particle size of 70.72um are formed after 24 hours under the oxidation action of Psuedonomas putida, namely the magnetic biological manganese oxide material.
In the method, in the step (1), the strain is Psuedonomas putida (strain deposit number), and the strain can oxidize Mn2+ under neutral conditions to form biological manganese oxide with the capacity of catalyzing and degrading single benzene ring pollutants.
In the above method, in step (1), the PYCM medium has a composition of (mg/L): peptone (800), yeast powder (200), dipotassium hydrogen phosphate (100), magnesium sulfate (200), sodium nitrate (200), calcium chloride (100), ammonium chloride (100), ferric ammonium citrate (1000) and manganese source (200), wherein the manganese source is manganese carbonate or manganese sulfate, the substances are dissolved in water, and after the substances are fully stirred uniformly, the pH value of the solution is adjusted to 7.1-7.2 by using a saturated sodium hydroxide solution.
In the method, in the step (1), the fermentation tank requires stirring, aeration and other parts to be nonmagnetic substances, the aeration can be performed by adopting a perforated pipe aeration or a membrane aeration mode, a microporous aeration head is not suitable, and an aeration device is made of a nonmetal material.
In the method, in the step (2), the particle size of the nano Fe3O4 particles is 5-20 nm.
When the magnetic biological manganese oxide material capable of degrading single-benzene-ring organic pollutants is applied to single-benzene-ring organic wastewater treatment, the method comprises the following steps: adding a magnetic biological manganese oxide material into the organic wastewater, and reacting in a shaker at the normal temperature and at the rotating speed of 150-180 rpm for 30-240 min.
In the application, the adding amount of the magnetic biological manganese oxide material added into the single benzene ring organic wastewater is 5-15 g/L.
Drawings
FIG. 1 is a Scanning Electron Microscope (SEM) of the prepared magnetic biological manganese oxide material;
FIG. 2 is a diagram showing the effect of the prepared magnetic biological manganese oxide material on degrading acetaminophen (APAP);
FIG. 3 is a diagram showing the effect of the prepared magnetic biological manganese oxide material on the removal of 1-naphthol.
Detailed Description
The present invention will be described in further detail with reference to specific embodiments, but the embodiments of the present invention are not limited thereto, and the process parameters specifically noted may be performed with reference to conventional techniques.
Example 1
A preparation method of a magnetic biological iron-manganese oxide material capable of degrading single benzene ring pollutants comprises the following steps:
(1) preparation of biological manganese oxide: inoculating dry powder of a strain Psuedonomas putida (strain accession number) into a PYCM culture medium sterilized by a high-pressure steam sterilizer at 121 ℃ for 20min at an inoculation amount of 1% (m/v), and performing shake culture in a constant-temperature gas bath shaker at 25 ℃ for 24h at a rotating speed of 125r/min until black granular precipitates are generated; inoculating the activated culture into a fermentation tank with sterile aeration and stirring functions in an inoculation amount of 1%, wherein the volume of a PYCM culture medium in the tank is 2/3 of the volume of the fermentation tank, and sterilizing at 121 ℃ for 20min and then pouring;
(2) preparing magnetic biological manganese oxide: when the activated culture is inoculated into a fermentation tank, magnetic nano Fe subjected to high-temperature sterilization is added at the same time3O4The adding amount is 0.5g/L, and the nano Fe is quickly added in a uniform aeration mode3O4The particles are uniformly dispersed. Under the conditions of continuous stirring and aeration at the temperature of 25 ℃, black particles with the particle size of 70.72um are formed after 24 hours under the oxidation action of Psuedonomas putida, namely the magnetic biological manganese oxide material. Scanning electron micrographs of the obtained magnetic biological manganese oxide(SEM), as shown in FIG. 1.
Example 2
Degradation effect of magnetic biological iron-manganese oxide material on acetaminophen
(1) The preparation method of the magnetic biological manganese oxide material is the same as the steps (1) and (2) in the embodiment 1;
(2) adding 5-15 g/L of magnetic biological manganese oxide into 100ml of 10mg/L paracetamol solution, placing the solution in a constant-temperature air bath shaking table to perform shaking table culture at the temperature of 25 ℃ and the rotating speed of 125r/min for 24 hours, taking 1ml of supernatant fluid in a centrifugal tube, centrifuging at 12000r/min for 10 minutes, filtering by using a 0.22-micron filter membrane to obtain samples, and measuring the content of paracetamol at different moments by using UV-HPLC. FIG. 2 is a graph showing the degradation effect of a magnetic biological iron-manganese oxide material on acetaminophen of 10 mg/L. The detection result shows that: the degradation efficiency of the magnetic biological iron-manganese oxide material can reach 75% in 2h, and the acetaminophen content in the aqueous solution is 0 in 24h, which shows that the magnetic biological iron-manganese oxide material can completely remove acetaminophen.
Embodiment 3
Degradation effect of magnetic biological iron-manganese oxide material on 1-naphthol
(1) The preparation method of the magnetic biological manganese oxide material is the same as the steps (1) and (2) in the embodiment 1;
(2) adding 5-15 g/L of magnetic biological manganese oxide into 100ml of 10 mg/L1-naphthol solution, placing the solution in a constant-temperature air bath shaking table to carry out shaking table culture at the temperature of 25 ℃ and the rotating speed of 125r/min for 24h, taking 1ml of supernatant fluid in a centrifugal tube, centrifuging at 12000r/min for 10min, filtering by using a 0.22-micron filter membrane to obtain a sample, and measuring the content of 1-naphthol by using UV-HPLC (ultraviolet-high performance liquid chromatography) at different moments. FIG. 3 is a graph showing the degradation effect of a magnetic biological iron-manganese oxide material on 10 mg/L1-naphthol. The detection result shows that: the magnetic biological iron-manganese oxide material can rapidly degrade 1-naphthol, the content of the 1-naphthol in the aqueous solution is 2.608mg/L at 240min, and the degradation efficiency reaches more than 70%.
Claims (7)
1. A preparation method of a magnetic biological manganese oxide material for degrading single benzene ring organic pollutants is characterized by comprising the following steps:
(1) preparation of biological manganese oxide: inoculating strain Pseudomonas putida dry powder with an inoculum size of 1% m/v into PYCM medium sterilized by high pressure steam sterilizer at 121 deg.C for 20min, placing in constant temperature gas bath shaking table, and shake-culturing at 25 deg.C and 125r/min for 24h until black granular precipitate is generated; inoculating the activated culture into a fermentation tank with sterile aeration and stirring functions in an inoculation amount of 1%, wherein the volume of a PYCM culture medium in the tank is 2/3 of the volume of the fermentation tank, and sterilizing at 121 ℃ for 20min and then pouring;
(2) preparing magnetic biological manganese oxide: when the activated culture is inoculated into a fermentation tank, magnetic nano Fe subjected to high-temperature sterilization is added at the same time3O4The adding amount is 0.5g/L, and the nano Fe is quickly added in a uniform aeration mode3O4The particles are uniformly dispersed; under the conditions of continuous stirring and aeration at the temperature of 25 ℃, black particles with the particle size of 70.72 mu m are formed after 24 hours under the oxidation action of Pseudomonas putida, namely the magnetic biological manganese oxide material.
2. The method for preparing a magnetic biological manganese oxide material according to claim 1, wherein: in the step (1), the strain is Pseudomonas putida, and Mn is added to the strain under neutral conditions2+Oxidizing to form biological manganese oxide with the capability of catalyzing and degrading single benzene ring organic pollutants.
3. The method for preparing a magnetic biological manganese oxide material according to claim 1, wherein: in the step (1), the composition of the PYCM medium is mg/L: the compound feed is prepared from peptone 800, yeast powder 200, dipotassium phosphate 100, magnesium sulfate 200, sodium nitrate 200, calcium chloride 100, ammonium chloride 100, ferric ammonium citrate 1000 and manganese source 200, wherein the manganese source is manganese carbonate or manganese sulfate, the substances are dissolved in water, and after the substances are fully stirred uniformly, the pH value of the solution is adjusted to 7.1-7.2 by using a saturated sodium hydroxide solution.
4. The method for preparing a magnetic biological manganese oxide material according to claim 1, wherein: in the step (1), the fermentation tank requires stirring, aeration and other parts to be nonmagnetic substances, the aeration adopts a perforated pipe aeration or membrane aeration mode, a microporous aeration head is not suitable, and an aeration device is made of a nonmetal material.
5. The method for preparing a magnetic biological manganese oxide material according to claim 1, wherein: in the step (2), the nano Fe3O4The particle size of the particles is 5-20 nm.
6. The method for preparing a magnetic biological manganese oxide material according to claim 1, wherein: in the step (2), the rotation speed of the continuous stirring is 80-100 rpm, and the aeration intensity is 2.0-3.0L/min.
7. The magnetic biological manganese oxide material for degrading single benzene ring organic pollutants is prepared by the preparation method of any one of claims 1 to 6.
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| CN201710583319.5A CN107308949B (en) | 2017-07-12 | 2017-07-12 | Preparation method of magnetic biological iron-manganese oxide capable of degrading single benzene ring pollutant |
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|---|---|---|---|
| CN201710583319.5A CN107308949B (en) | 2017-07-12 | 2017-07-12 | Preparation method of magnetic biological iron-manganese oxide capable of degrading single benzene ring pollutant |
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