CN106319019B - Nano manganese dioxide for removing heavy metal pollution of underground water and preparation method thereof - Google Patents

Nano manganese dioxide for removing heavy metal pollution of underground water and preparation method thereof Download PDF

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CN106319019B
CN106319019B CN201610831824.2A CN201610831824A CN106319019B CN 106319019 B CN106319019 B CN 106319019B CN 201610831824 A CN201610831824 A CN 201610831824A CN 106319019 B CN106319019 B CN 106319019B
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姜永海
席北斗
杨昱
廉新颖
梁冠男
徐祥健
董子萱
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Chinese Research Academy of Environmental Sciences
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Abstract

Nanometer manganese dioxide for removing heavy metal pollution of underground water is obtained by the following method: 1) inoculating one or more of Leptothrix discophora (SS-1), Pseudomonas putida (Pseudomonas putida) MnB1 and Bacillus (Bacillus sp) SG-1 to a microorganism growth culture medium, and culturing at 25-30 ℃; 2) centrifuging the mixture obtained in the step 1 to obtain thalli, and cleaning the precipitated thalli; 3) inoculating the thalli obtained in the step 2 into a manganese oxide culture medium, and culturing at 25-30 ℃; 4) adding MnCl in the step 32And Na3VO4And culturing at 28-30 ℃ to obtain black precipitate, namely the nano manganese dioxide material. The invention also discloses a preparation method of the nano manganese dioxide.

Description

Nano manganese dioxide for removing heavy metal pollution of underground water and preparation method thereof
Technical Field
The invention belongs to the technical field of groundwater pollution remediation, and particularly relates to nano manganese dioxide for removing heavy metal pollution of groundwater.
The invention also relates to a preparation method of the nano manganese dioxide.
Background
Groundwater is a natural resource on which human beings live, however, with the rapid development of modern industry and agriculture, heavy metal pollution of groundwater by heavy metal containing pesticides and fertilizers is becoming serious due to the large amount of application. Heavy metals cannot be biodegraded and are easily accumulated in the living body and finally enter the human body through the food chain, causing various diseases and body abnormalities. In order to prevent the heavy metals from entering the environment and food chain fundamentally, heavy metal contamination in groundwater must be remediated.
The groundwater heavy metal pollution remediation method comprises a chemical method, a physical method and the like, wherein the physical method comprises a membrane separation method, an electrolytic reduction method, an ion exchange method, an adsorption method and the like. Traditional treatment methods such as a chemical precipitation method and an electrolysis method are difficult to economically and effectively reduce the concentration of heavy metal ions in the wastewater to the discharge standard, and generate sludge which is difficult to treat, so that the traditional treatment methods are not suitable for treating the low-concentration heavy metal ion wastewater; although the ion exchange method, the membrane separation technique and the activated carbon adsorption method have good treatment effects, the treatment method is greatly influenced by impurities in water and treatment conditions, has high treatment cost and is difficult to apply on a large scale. Therefore, adsorption methods using inexpensive adsorbents as active materials have been the focus of recent years, particularly for lower concentrations of heavy metals in underground water.
Manganese dioxide, as a functional material, has shown many special physical and chemical properties in oxidation, catalysis, electrochemistry, adsorption, magnetism, etc. due to its advantages of abundant sources, low price, environmental friendliness, etc. To make better use of manganese dioxide, nano manganese dioxide with specific properties can be used, nanoparticles having many unique properties, such as small size, large surface area, and many surface active sites. The main current production methods of nano manganese dioxide comprise: mechanical crushing, electrochemical precipitation, coprecipitation, redox deposition, self-assembly, etc., but these methods have high requirements for equipment, complex process and are liable to cause pollution. Therefore, the expectation of the field for a nano manganese dioxide material which is economically feasible, simple in process, remarkable in effect and environment-friendly is very high.
Disclosure of Invention
The invention aims to provide the nano manganese dioxide material which is economical, feasible, simple in process and obvious in effect and can remove heavy metal pollution of underground water.
The invention also aims to provide a preparation method of the nano manganese dioxide material.
In order to achieve the purpose, the nano manganese dioxide for removing heavy metal pollution of underground water provided by the invention is obtained by the following method:
1) inoculating one or more of Leptothrix discophora (SS-1), Pseudomonas putida (MnB 1) and Bacillus (Bacillus sp) SG-1 to a microorganism growth culture medium, and culturing at 25-30 ℃;
2) centrifuging the mixture obtained in the step 1 to obtain thalli, and cleaning the precipitated thalli;
3) inoculating the thalli obtained in the step 2 into a manganese oxide culture medium, and culturing at 25-30 ℃;
4) adding MnCl in the step 32And Na3VO4And culturing at 28-30 ℃ to obtain black precipitate, namely the nano manganese dioxide.
The preparation method of the nano manganese dioxide comprises the following steps:
1) inoculating one or more of Leptothrix discophora (SS-1), Pseudomonas putida (MnB 1) and Bacillus (Bacillus sp) SG-1 to a microorganism growth culture medium, and culturing at 25-30 ℃;
2) centrifuging the mixture obtained in the step 1 to obtain thalli, and cleaning the precipitated thalli;
3) inoculating the thalli obtained in the step 2 into a manganese oxide culture medium, and culturing at 25-30 ℃;
4) adding MnCl in the step 32And Na3VO4And culturing at 28-30 ℃ to obtain black precipitate, namely the nano manganese dioxide.
Wherein the microbial growth medium: 1L deionized water containing yeast extract 2g, beef extract 1g, peptone 5g, NaCl5g, KH2PO40.45g、Na2HPO42.39g, and controlling the pH value to be 6.8-7.0.
Wherein, manganese oxide culture medium: 1L deionized water contains yeast extract 0.5g, acid hydrolyzed casein 0.5g, glucose 1g, HEPES 2.38g, CaCl20.053g、MgSO4·7H2O 0.2042g、FeCl3·6H20.001g of O and 1mL of trace element liquid.
Wherein 1L of microelement liquid contains CuSO4·5H2O 10mg、ZnSO4·7H2O 44mg、CoCl2·6H2O20mg、NaMoO4·2H2O 13mg。
Wherein, acid hydrolyzed casein in manganese oxide culture medium is sterilized at low temperature, and glucose and HEPES are sterilized by 0.22 μm filter membrane; added MnCl2And Na3VO4Pass through a 0.22 μm filter.
The invention has the following advantages:
1. the method is simple and easy to implement, low in cost, high in generation efficiency, stable in performance, green and energy-saving;
2. the material is generated by microbial metabolism, is nanoscale, has an irregular spatial structure and a larger specific surface area, and is favorable for carrying out oxidation adsorption on heavy metal pollutants;
3. the nano manganese dioxide material is a mixture of microorganism and manganese dioxide. The manganese dioxide is converted into bivalent or trivalent manganese after oxidizing pollutants, and the bivalent or trivalent manganese is converted into the manganese dioxide again under the synergistic action of microorganisms. The regeneration of the material is realized, the service life of the material is prolonged, and the concept of circular economy is met;
4. reasonable addition of Na3VO4·12H2O not only contributes to microbial productionManganese dioxide is produced, and the manganese dioxide has more gaps and active sites, so that the oxidation and adsorption capacity of the manganese dioxide is enhanced;
5. the nano manganese dioxide material is safe and environment-friendly in the using process, and cannot cause secondary pollution to underground water.
Detailed Description
The dielectric material provided by the invention is generated by metabolism of manganese oxidizing microorganisms, high-temperature calcination, acid-base treatment, mechanical crushing and the like in the traditional preparation process of manganese dioxide are not needed, and the material has a larger specific surface area, more void structures, stronger oxidation adsorption capacity and a longer service cycle.
The invention provides two culture media, namely a microorganism growth culture medium and a manganese oxide culture medium, wherein the microorganism growth culture medium comprises the following components in parts by weight: 1L deionized water containing yeast extract 2g, beef extract 1g, peptone 5g, NaCl5g, KH2PO40.45g、Na2HPO42.39g, and controlling the pH value to be 6.8-7.0.
Manganese oxide culture medium: 1L deionized water contains yeast extract 0.5g, acid hydrolyzed casein 0.5g, glucose 1g, HEPES 2.38g, CaCl20.053g、MgSO4·7H2O 0.2042g、FeCl3·6H20.001g of O, 1mL of trace elements, 1L of trace element liquid containing CuSO4·5H2O 10mg、ZnSO4·7H2O 44mg、CoCl2·6H2O 20mg、NaMoO4·2H2O13mg。
The manganese-oxidizing microorganism used for preparing manganese dioxide may be Leptothrix discophora SS-1, Pseudomonas putida MnB1, Bacillus (Bacillus sp) SG-1.
The invention provides a nano manganese dioxide material and a preparation method thereof, wherein the nano manganese dioxide material comprises the following steps:
1) inoculating the manganese-oxidizing microorganisms into a sterilized microorganism growth medium, wherein the microorganisms can be one or more of the manganese-oxidizing microorganisms, and culturing for 18-28 h at 25-30 ℃.
2) And (3) centrifuging the mixture obtained in the step (1) at a high speed to obtain thalli, and washing the precipitated thalli with sterile water for 2-3 times.
3) Inoculating the thallus obtained in step 2 into sterilized manganese oxide culture medium, wherein acid hydrolyzed casein is sterilized separately at low temperature, and glucose and HEPES are sterilized by passing through 0.22 μm filter membrane. Culturing for 4-8 h at 25-30 ℃, and adding MnCl filtered by a 0.22 mu m filter membrane2Making the concentration of the Na mixed solution be 10-60 mM and passing through a 0.22 mu m filter membrane3VO4The concentration of the compound is 5 to 10 mM. Culturing for 18-24 h at the temperature of 28-30 ℃ to obtain black precipitate, namely the nano manganese dioxide material.
Example 1
The strain (Leptothrix discophora) SS-1 was inoculated into a sterilized growth medium of the microorganism and cultured at 25 ℃ for 18 hours. Then, the resulting mixture was centrifuged at high speed to obtain cells, and the cells were washed with sterile water and precipitated 2 times. The obtained cells were inoculated into sterilized manganese oxide medium, in which acid-hydrolyzed casein was sterilized alone at a low temperature of 115 ℃ and glucose and HEPES were sterilized through a 0.22 μm filter. After culturing at 25 ℃ for 4h, MnCl filtered through a 0.22 mu m filter membrane is added2The concentration was adjusted to 10mM and Na was passed through a 0.22 μm filter3VO4The concentration was adjusted to 5 mM. Culturing at 28 deg.C for 18h to obtain black precipitate as nanometer manganese dioxide material.
0.2g of the prepared manganese dioxide material was used to remediate 400ml of groundwater having an As (III) concentration of 1 mg/L. By detecting and analyzing the content of arsenic in the liquid phase, all As (III) is oxidized into As (V) within 1h, and the removal rate of total arsenic after 24h is 99.4%.
Example 2
The mixed strain of Pseudomonas putida (Pseudomonas putida) MnB1 and Bacillus (Bacillus sp) SG-1 was inoculated into a sterilized microorganism growth medium and cultured at 30 ℃ for 28 hours. Then, the resulting mixture was centrifuged at high speed to obtain cells, and the cells were washed with sterile water and precipitated 3 times. The obtained cells were inoculated into sterilized manganese oxide medium, in which acid-hydrolyzed casein was sterilized alone at a low temperature of 115 ℃ and glucose and HEPES were sterilized through a 0.22 μm filter. After culturing for 8h at 30 ℃, adding MnCl filtered by a 0.22 mu m filter membrane2The concentration was adjusted to 60mM and Na was passed through a 0.22 μm filter3VO4The concentration was adjusted to 10 mM. Culturing for 24h at 30 ℃ to obtain black precipitate, namely the nano manganese dioxide material.
0.5g of the prepared manganese dioxide material was used to remediate 400ml of groundwater having a Tl (I) concentration of 20 mg/L. After 28h, the removal rate of Tl (I) by the dielectric material is 98.3 percent by detecting and analyzing the content of total thallium in the liquid phase.
Example 3
Bacillus sp SG-1 was inoculated into a sterilized microbial growth medium and cultured at 28 ℃ for 22 hours. Then, the resulting mixture was centrifuged at high speed to obtain cells, and the cells were washed with sterile water and precipitated 3 times. The obtained cells were inoculated into sterilized manganese oxide medium, in which acid-hydrolyzed casein was sterilized alone at a low temperature of 115 ℃ and glucose and HEPES were sterilized through a 0.22 μm filter. After culturing for 6h at 28 ℃, adding MnCl filtered by a 0.22 mu m filter membrane2The concentration was adjusted to 40mM and Na was passed through a 0.22 μm filter3VO4The concentration was adjusted to 8 mM. Culturing for 22h at 30 ℃ to obtain black precipitate, namely the nano manganese dioxide material.
0.3g of the prepared manganese dioxide material was used to remediate 400ml of groundwater having a Pb (II) concentration of 40 mg/L. After 20h, the content of the total lead in the analyzed liquid phase is detected, so that the removal rate of the medium material to Pb (II) is 99.1%.

Claims (8)

1. Nanometer manganese dioxide for removing heavy metal pollution of underground water is obtained by the following method:
1) inoculating manganese-oxidizing microorganisms into a sterilized microorganism growth medium, wherein the microorganisms are one or more of strain of Tricholoma fuliginosum (Leptothrix discophora) SS-1, Pseudomonas putida (Pseudomonas putida) MnB1 and Bacillus sp (Bacillus sp.) SG-1, and culturing at 25-30 ℃ for 18-28 h;
2) centrifuging the mixture obtained in the step 1 at a high speed to obtain thalli, and cleaning the precipitated thalli with sterile water for 2-3 times;
3) inoculating the cells obtained in step 2 into sterilized manganese oxide medium, wherein acid hydrolyzed casein is sterilized at low temperature and glucose and HEPES are 0.22 μmSterilizing with a filter membrane; culturing for 4-8 h at 25-30 ℃, and adding MnCl filtered by a 0.22 mu m filter membrane2Making the concentration of the Na mixed solution be 10-60 mM and passing through a 0.22 mu m filter membrane3VO4The concentration of the solution is 5 to 10 mM; culturing for 18-24 h at the temperature of 28-30 ℃ to obtain black precipitate, namely the nano manganese dioxide material.
2. Nano manganese dioxide for groundwater heavy metal pollution removal according to claim 1, wherein the microbial growth medium: 1L deionized water containing yeast extract 2g, beef extract 1g, peptone 5g, NaCl5g, KH2PO40.45g、Na2HPO42.39g, and controlling the pH value to be 6.8-7.0.
3. Nano manganese dioxide for groundwater heavy metal pollution removal according to claim 1, wherein the manganese oxide medium: 1L deionized water contains yeast extract 0.5g, acid hydrolyzed casein 0.5g, glucose 1g, HEPES 2.38g, CaCl20.053g、MgSO4·7H2O 0.2042g、FeCl3·6H2O0.001g and 1mL of trace element liquid.
4. Nano manganese dioxide for groundwater decontamination of heavy metal pollution as claimed in claim 3, wherein 1L of trace element solution contains CuSO4·5H2O 10mg、ZnSO4·7H2O 44mg、CoCl2·6H2O 20mg、NaMoO4·2H2O 13mg。
5. The method for preparing nano manganese dioxide according to claim 1:
1) inoculating manganese-oxidizing microorganisms to a sterilized microorganism growth medium, wherein the microorganisms are one or more of strain of coiling block (Leptothrix discophora) SS-1, Pseudomonas putida (Pseudomonas putida) MnB1 and Bacillus (Bacillus sp) SG-1, and culturing for 18-28 h at 25-30 ℃;
2) centrifuging the mixture obtained in the step 1 at a high speed to obtain thalli, and cleaning the precipitated thalli with sterile water for 2-3 times;
3) inoculating the thallus obtained in the step 2 into a sterilized manganese oxide culture medium, wherein acid hydrolyzed casein is independently sterilized at low temperature, and glucose and HEPES are sterilized by a 0.22 mu m filter membrane; culturing for 4-8 h at 25-30 ℃, and adding MnCl filtered by a 0.22 mu m filter membrane2Making the concentration of the Na mixed solution be 10-60 mM and passing through a 0.22 mu m filter membrane3VO4The concentration of the solution is 5 to 10 mM; culturing for 18-24 h at the temperature of 28-30 ℃ to obtain black precipitate, namely the nano manganese dioxide material.
6. The production method according to claim 5, wherein the microorganism growth medium: 1L deionized water containing yeast extract 2g, beef extract 1g, peptone 5g, NaCl5g, KH2PO40.45g、Na2HPO42.39g, and controlling the pH value to be 6.8-7.0.
7. The production method according to claim 5, wherein the manganese oxide medium: 1L deionized water contains yeast extract 0.5g, acid hydrolyzed casein 0.5g, glucose 1g, HEPES 2.38g, CaCl20.053g、MgSO4·7H2O 0.2042g、FeCl3·6H20.001g of O and 1mL of trace element liquid.
8. The method according to claim 7, wherein 1L of the trace element liquid contains CuSO4·5H2O 10mg、ZnSO4·7H2O 44mg、CoCl2·6H2O 20mg、NaMoO4·2H2O13mg。
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CN107151678A (en) * 2017-01-26 2017-09-12 大连理工大学 The magnetic iron and manganese oxides of aerobic microbiological synthesis and its application
CN109337840B (en) * 2018-11-12 2021-08-13 中国科学院合肥物质科学研究院 Nano manganese oxide producing strain and method for preparing nano manganese oxide by using strain
CN109295109B (en) * 2018-11-12 2021-08-13 中国科学院合肥物质科学研究院 Preparation method and application of nano manganese oxide
CN114177887B (en) * 2021-12-02 2023-01-03 中国环境科学研究院 Biochar-manganese composite material wrapping biochar and preparation method and application thereof

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