CN111422990B - Biogenic manganese oxide substrate and application thereof in construction of constructed wetland electrode - Google Patents
Biogenic manganese oxide substrate and application thereof in construction of constructed wetland electrode Download PDFInfo
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- CN111422990B CN111422990B CN202010231813.7A CN202010231813A CN111422990B CN 111422990 B CN111422990 B CN 111422990B CN 202010231813 A CN202010231813 A CN 202010231813A CN 111422990 B CN111422990 B CN 111422990B
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- 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
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
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- C02F3/005—Combined electrochemical biological processes
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- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/32—Biological treatment of water, waste water, or sewage characterised by the animals or plants used, e.g. algae
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Abstract
The invention discloses a biogenic manganese oxide matrix and application thereof in construction of constructed wetland electrodes. The preparation method of the biogenic manganese oxide matrix comprises the following steps: s10, mixing the manganese-based material and the carbon-based material in proportion, continuously stirring and uniformly mixing, and homogenizing; s20, adding a microbial agent into the mixed material homogenized in the step S10 for composting to obtain a composted manganese-carbon-based material; s30, mixing the manganese-carbon-based material subjected to composting in the step S20 with a binder, and performing screw extrusion molding to prepare a rod-shaped manganese-carbon-based material; and S40, heating and drying the rod-shaped manganese-carbon matrix base material, and naturally cooling to obtain the biological manganese oxide matrix.
Description
Technical Field
The invention relates to a biogenic manganese oxide substrate and application thereof in construction of a coupling type microbial fuel cell constructed wetland electrode.
Background
The constructed wetland coupling microbial fuel cell (CW-MFC) has become a novel mixed technology of sewage treatment and biological power generation. Such sewage treatment systems are essentially two conventional technologies: combination of optimized features of artificial wetland (CW) and Microbial Fuel Cell (MFC). The MFC consists of an aerobic cathode compartment and an anaerobic anode compartment separated by a proton exchange membrane and connected by an external circuit. In MFC, waste water is treated and electric energy can be generated. To date, most research on MFC has been limited to laboratory scale. The constructed wetland sewage treatment has relatively low energy consumption during operation and is easy to operate and maintain. The upper part of the aerobic zone is in close contact with the atmosphere and is an aerobic zone; while the lower anaerobic conditions slow the rate of organic matter decomposition, resulting in insufficient electron acceptors available. The anode in MFC technology acts as a temporary electron acceptor and therefore helps to improve the effect of wastewater treatment in the anaerobic zone in CW. CW and MFC have similar aerobic and anaerobic areas, and the sewage treatment capacity can be effectively improved by integrating the MFC technology into CW, but the structure and the property of the electrode material of the MFC directly influence the transfer efficiency of electrons in a medium.
Oxides of manganese are active mineral phases that play an important role in the biogenic cycle and are capable of undergoing redox reactions with organic and inorganic chemicals and their compounds. Many dissimilatory metal-reducing bacteria (electrogenic bacteria) can utilize oxides of manganese as the final electron acceptor to oxidize organic matter. Meanwhile, the manganese oxide also has high adsorption capacity, so that various ions can be adsorbed, and the distribution and bioavailability of a plurality of toxic and essential elements are controlled. Besides the characteristics of high stability, low resistance, corrosion resistance, large specific surface area and the like of the electrode material, the biological source manganese oxidation has high biocompatibility and provides a good attachment position for electrogenic bacteria near the electrode, and in addition, researches show that the biological source manganese oxidation can adjust the pH value of constructed wetland sewage and wastewater and provides an attachment growth environment for electrogenic active microorganisms.
However, the substrates of oxides of manganese prepared using the prior art preparation methods are directed to CODCr、BOD5、NH3The removal rate of N, TP and SS is poor, which results in poor purification effect of the constructed wetland.
Disclosure of Invention
Aiming at the technical problems in the prior art, the embodiment of the invention provides a preparation method of a biogenic manganese oxide substrate and application of the biogenic manganese oxide substrate in construction of an artificial wetland electrode.
In order to solve the technical problem, the embodiment of the invention adopts the following technical scheme:
a method for preparing biogenic manganese oxide matrix comprises the following steps:
s10, mixing the manganese-based material and the carbon-based material in proportion, continuously stirring and uniformly mixing, and homogenizing;
s20, adding a microbial agent into the mixed material homogenized in the step S10 for composting to obtain a composted manganese-carbon-based material;
s30, mixing the manganese-carbon-based material subjected to composting in the step S20 with a binder, and performing screw extrusion molding to prepare a rod-shaped manganese-carbon-based material;
and S40, heating and drying the rod-shaped manganese-carbon matrix base material, and naturally cooling to obtain the biological source manganese oxide matrix.
Preferably, the mixing ratio of the manganese-based material to the carbon-based material is 1: 1-1: 25 by mass, and the binder accounts for 5% -30% of the total mass of the manganese-carbon-based material and the binder after composting.
Preferably, the manganese-based material is a manganese-based raw material with the total manganese content of more than 2.5-5% by mass, and the particle size is 0.5-1.0 mm; the carbon-based material is granular agricultural waste material and is sieved by a sieve with 20-100 meshes; the binder is a plastic inorganic mineral material.
Preferably, the manganese-based material is manganese slag; the carbon-based material is one or a mixture of more than two of crop straws, sawdust, rice hulls, bagasse, beet pulp and coffee grounds; the binder is one or more of clay, bentonite and kaolin.
Preferably, the microbial agent comprises a composite microbial agent of two or more of bacillus, actinomycetes, yeast, trichoderma, white rot fungi and photosynthetic bacteria.
Preferably, the composting treatment is to mix the microbial agent and the manganese-carbon-based material obtained in step S10 according to a ratio of 1: 1000-3: 1000, and the composting time is 4-8 days.
Preferably, the rod-shaped manganese carbon-based substrate in step S30 has a particle size of 1 to 10 mm.
Preferably, the temperature for heating and drying the rod-shaped manganese carbon matrix base material in the step 40 is 40-80 ℃, and the rod-shaped manganese carbon matrix base material is naturally cooled for 4-8 hours.
The invention also discloses application of the biogenic manganese oxide matrix prepared by the preparation method in construction of artificial wetland electrodes.
Compared with the prior art, the preparation method of the biogenic manganese oxide matrix has the beneficial effects that:
the artificial wetland adopting the manganese oxide substrate prepared by the preparation process of the invention can improve CODCr、BOD5、NH3Compared with the constructed wetland in the prior art, the removal rate of-N, TP and SS has obvious advantages.
The summary of various implementations or examples of the technology described in this disclosure is not a comprehensive disclosure of the full scope or all features of the disclosed technology.
Detailed Description
Example 1
A method for preparing biogenic manganese oxide matrix comprises the following steps: s10: mixing manganese slag with the manganese content of 3 percent and the average grain diameter of 1mm serving as a manganese-based material with a carbon-based material of rice hull powder sieved by a 40-mesh sieve according to the proportion of 1: 2, continuously stirring and uniformly mixing, and performing homogenization treatment; s20: adding a microbial agent into the mixed material homogenized in the step S10 in a ratio of 1000: 1 for 6 days of composting treatment to obtain a manganese-carbon-based material subjected to composting treatment; s30: mixing the composted manganese-carbon base material in the step S20 with a binder in a ratio of 10: 1, and performing screw extrusion molding to prepare a rod-shaped manganese-carbon base material with a particle size of 3 mm; s40: and (3) drying the rod-shaped manganese carbon matrix base material at 60 ℃, and naturally cooling for 4 hours to obtain the biological source manganese oxide matrix.
Example 2
A method for preparing biogenic manganese oxide matrix comprises the following steps: s10: mixing manganese slag with manganese content of 4.5% and average particle size of 0.8mm as manganese-based material with carbon-based material of 60 mesh rice hull powder at a ratio of 1: 3, stirring and homogenizing; s20: adding a microbial agent into the mixed material homogenized in the step S10 in a ratio of 1000: 2 for 8 days of composting treatment to obtain a manganese-carbon-based material subjected to composting treatment; s30: mixing the composted manganese-carbon base material in the step S20 with a binder in a ratio of 15: 1, and performing screw extrusion molding to prepare a rod-shaped manganese-carbon base material with the particle size of 4 mm; s40, drying the rod-shaped manganese carbon matrix base material at 60 ℃, and naturally cooling for 4 hours to obtain the biogenic manganese oxide matrix.
Example 3
A method for preparing biogenic manganese oxide matrix comprises the following steps: s10: mixing manganese slag with 5% of manganese content and an average particle size of 1.5mm serving as a manganese-based material with a carbon-based material of rice hull powder sieved by a 60-mesh sieve according to a ratio of 1: 1, continuously stirring and uniformly mixing, and performing homogenization treatment; s20: adding a microbial agent into the mixed material homogenized in the step S10 in a ratio of 1000: 2 for 6 days of composting treatment to obtain a manganese-carbon-based material subjected to composting treatment; s30: mixing the manganese-carbon-based material subjected to composting in the step S20 with a binder in a ratio of 15: 1, and performing screw extrusion molding to prepare a rod-shaped manganese-carbon-based material with the particle size of 1 mm; s40: and (3) drying the rod-shaped manganese carbon matrix base material at 50 ℃, and naturally cooling for 6 hours to obtain the biological source manganese oxide matrix.
Application examples
The quality of sewage inlet water is slightly polluted by organic matters, in examples 1-3 (microbial fuel cell coupled horizontal subsurface flow constructed wetland) and a comparative example (horizontal subsurface flow constructed wetland adopting a traditional substrate), a substrate layer 320mm position in the constructed wetland is constructed according to the thickness of 100mm and is used as an anode, a lead is embedded in the anode and led out to the surface layer of the wetland, a load is connected, and a data recorder is connected to the load and is used for recording the electricity generation amount. The manual construction is completely adopted, and the compaction is not required; after 3 days, COD was measuredCr、BOD5、NH3-variation of N, TP, SS, calculating removal rate, formula: the removal rate is (the index concentration of the water quality of the inlet water is-3 days later, the index concentration of the water quality of the wetland)/the index concentration of the water quality of the inlet water is multiplied by 100 percent.
| Example 1 | Example 2 | Example 3 | Comparative example | |
| CODCrRemoval rate | 94.24％ | 94.15％ | 94.52％ | 77.50％ |
| BOD5Removal rate | 93.33％ | 97.47％ | 98.67％ | 86.67％ |
| NH3-N removal rate | 83.66％ | 76.49％ | 73.50％ | 61.25％ |
| TP removal Rate | 95.34％ | 96.38％ | 95.54％ | 75.81％ |
| Removal rate of SS | 92.54％ | 95.50％ | 96.47％ | 76.23％ |
| Electricity production amount kWh/m3 | 1.04×10-2 | 1.26×10-2 | 1.33×10-2 | - |
As can be seen from the above table, the constructed wetland adopting the manganese oxide substrate prepared by the preparation process of the invention can improve CODCr、BOD5、NH3Compared with the constructed wetland in the prior art, the method has obvious advantages in the removal rate of-N, TP and SS.
In addition, the invention also has the following advantages:
manganese slag and cellulose carbon-based materials are used as original production matrixes and are used as fillers of artificial wetlands and electrodes of microbial fuels. The manganese slag is an industrial waste, the cellulose carbon-based material is an agricultural waste, and the biogenic manganese oxide prepared by the preparation method can realize the resource utilization of the waste and improve the microbial diversity in the artificial wetland and the electricity generation efficiency of the microbial fuel cell. In addition, by using the technical scheme of the invention, the construction cost of the artificial wetland can be saved, and an ideal colonization site can be provided for the electrogenesis microorganisms. Firstly, biogenic manganese oxide can enable electrogenic bacteria in the constructed wetland to be more active, so that the electrogenic capability of the microbial fuel cell is improved; in the aspect of sewage purification, when the constructed wetland is used for treating acidic sewage and wastewater, the biogenic manganese oxide is used as constructed wetland filler, the pH of the sewage is properly increased, the species abundance in the constructed wetland is correspondingly increased, the degradation capability of microorganisms on organic matters in the sewage is also improved, and the improvement is beneficial to the activity of electrogenesis organisms, so that the bioelectricity output of the air cathode microbial fuel cell is enhanced.
Moreover, although exemplary embodiments have been described herein, the scope of the present invention includes any and all embodiments based on the present invention with equivalent elements, modifications, omissions, combinations (e.g., of various embodiments across), adaptations or alterations. The elements of the claims are to be interpreted broadly based on the language employed in the claims and not limited to examples described in the present specification or during the prosecution of the application, which examples are to be construed as non-exclusive. It is intended, therefore, that the specification and examples be considered as exemplary only, with a true scope and spirit being indicated by the following claims and their full scope of equivalents.
The above description is intended to be illustrative, and not restrictive. For example, the above-described examples (or one or more versions thereof) may be used in combination with each other. For example, other embodiments may be used by those of ordinary skill in the art upon reading the above description. In addition, in the foregoing detailed description, various features may be grouped together to streamline the disclosure. This should not be interpreted as an intention that a non-claimed disclosed feature is essential to any claim. Rather, inventive subject matter may lie in less than all features of a particular disclosed embodiment. Thus, the following claims are hereby incorporated into the detailed description as examples or embodiments, with each claim standing on its own as a separate embodiment, and it is contemplated that the embodiments can be combined with each other in various combinations or permutations. The scope of the invention should be determined with reference to the appended claims, along with the full scope of equivalents to which such claims are entitled.
The above embodiments are only exemplary embodiments of the present invention, and are not intended to limit the present invention, and the scope of the present invention is defined by the claims. Various modifications and equivalents may be made by those skilled in the art within the spirit and scope of the present invention, and such modifications and equivalents should also be considered as falling within the scope of the present invention.
Claims (4)
1. The application of the biogenic manganese oxide matrix in construction of artificial wetland electrodes is characterized in that the preparation method of the biogenic manganese oxide matrix comprises the following steps:
s10, mixing the manganese-based material and the carbon-based material in proportion, continuously stirring and uniformly mixing, and carrying out homogenization treatment;
s20, adding a microbial agent into the mixed material homogenized in the step S10 for composting to obtain a composted manganese-carbon-based material;
s30, mixing the manganese-carbon-based material subjected to composting in the step S20 with a binder, and performing screw extrusion molding to prepare a rod-shaped manganese-carbon-based material;
s40, heating and drying the rod-shaped manganese-carbon matrix base material, and naturally cooling to obtain a biological source manganese oxide matrix;
the manganese-based material is a manganese-based raw material with the total manganese content of more than 2.5-5%, and the manganese-based raw material is manganese slag with the particle size of 0.5-1.0 mm; the carbon-based material is granular agricultural waste material which is a mixture of one or more than two of crop straws, sawdust, rice hulls, bagasse, beet pulp and coffee grounds and is sieved by a sieve with 20-100 meshes; the adhesive is a plastic inorganic mineral material, and the plastic inorganic mineral material is bentonite or kaolin;
the microbial agent is a composite microbial agent of two or more of bacillus, actinomycetes, microzyme, trichoderma, white-rot fungi and photosynthetic bacteria;
the composting treatment is to mix the microbial inoculum and the manganese-carbon-based material obtained in the step S10 according to the proportion of 1: 1000-3: 1000 for composting for 4-8 days.
2. The application of the biogenic manganese oxide matrix in construction of artificial wetland electrodes as claimed in claim 1, wherein the mixing ratio of the manganese-based material to the carbon-based material is 1: 1-1: 25 by mass, and the binder accounts for 5% -30% of the total mass of the manganese-carbon-based material and the binder after composting.
3. The use of biogenic manganese oxide matrix in construction of constructed wetland electrode according to claim 1, wherein the rod-shaped manganese carbon matrix substrate in step S30 has a particle size of 1-10 mm.
4. The application of biogenic manganese oxide matrix in construction of artificial wetland electrode according to claim 1, wherein the temperature for heating and drying the rod-shaped manganese carbon matrix substrate in step S40 is 40-80 ℃, and the rod-shaped manganese carbon matrix substrate is naturally cooled for 4-8 hours.
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| WO2014150415A1 (en) * | 2013-03-15 | 2014-09-25 | Solina Brent A | Electroactive cultures and apparatuses therefor |
| CN105347481B (en) * | 2015-11-26 | 2017-11-03 | 山东大学 | The method that biofermentation coupling artificial wet land system purifies low ratio of carbon to ammonium sanitary sewage |
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