CN113003735A - Intermittent aeration type remediation method for ammonia nitrogen and organic pollution organisms in underground water - Google Patents
Intermittent aeration type remediation method for ammonia nitrogen and organic pollution organisms in underground water Download PDFInfo
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Images
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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
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/34—Biological treatment of water, waste water, or sewage characterised by the microorganisms used
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/30—Aerobic and anaerobic processes
- C02F3/302—Nitrification and denitrification treatment
- C02F3/305—Nitrification and denitrification treatment characterised by the denitrification
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/30—Aerobic and anaerobic processes
- C02F3/302—Nitrification and denitrification treatment
- C02F3/307—Nitrification and denitrification treatment characterised by direct conversion of nitrite to molecular nitrogen, e.g. by using the Anammox process
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/34—Biological treatment of water, waste water, or sewage characterised by the microorganisms used
- C02F3/346—Iron bacteria
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F2003/001—Biological treatment of water, waste water, or sewage using granular carriers or supports for the microorganisms
-
- 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
- C02F2101/10—Inorganic compounds
- C02F2101/16—Nitrogen compounds, e.g. ammonia
-
- 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
- C02F2101/10—Inorganic compounds
- C02F2101/16—Nitrogen compounds, e.g. ammonia
- C02F2101/163—Nitrates
-
- 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
- C02F2101/10—Inorganic compounds
- C02F2101/16—Nitrogen compounds, e.g. ammonia
- C02F2101/166—Nitrites
-
- 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
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/06—Nutrients for stimulating the growth of microorganisms
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- Life Sciences & Earth Sciences (AREA)
- Microbiology (AREA)
- Biodiversity & Conservation Biology (AREA)
- Hydrology & Water Resources (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Purification Treatments By Anaerobic Or Anaerobic And Aerobic Bacteria Or Animals (AREA)
Abstract
The invention discloses an intermittent aeration type remediation method for ammonia nitrogen and organic pollutants in underground water, which comprises the following steps: carrying out indoor domestication, screening and culture on native indigenous microorganisms derived from flooded paddy field soil to obtain a bacterial liquid of a composite strain, wherein the bacterial liquid contains the domesticated and cultured composite strain which is Fe (III) reducing bacteria, denitrifying bacteria and iron ammonia oxidizing bacteria, and loading the composite strain subjected to domestication culture in the bacterial liquid to the surface of Fe (III) iron oxide minerals with particle size of 2-4mm in a biofilm formation mode to form a biological membrane to obtain a repairing functional material, and adding the repairing functional material into polluted underground water; and regulating and controlling dissolved oxygen through intermittent aeration to construct an intermittent anaerobic/aerobic environment, thereby realizing synchronous bioremediation of ammonia nitrogen and organic pollution of underground water. The method has the advantages of saving energy, improving the denitrification effect and being beneficial to the short-cut nitrification process under the condition of low carbon source.
Description
Technical Field
The invention relates to a remediation method, in particular to an intermittent aeration type remediation method for underground water ammonia nitrogen and organic pollution organisms.
Background
In 2019, the 'Chinese ecological environment condition bulletin' shows that the quality condition of Chinese underground water is not optimistic overall, and in more than 1 million national-level underground water quality monitoring points in the country, the proportion of the inferior five types of water bodies rises to 18.8%, and pollution standard exceeding factors comprise fluoride, ammonia nitrogen, organic matters and the like. A large number of researches show that ammonia nitrogen and organic matters in underground water of typical polluted sites, such as refuse landfills and industrial and mining enterprises, become common characteristic pollutants. When underground water polluted by ammonia nitrogen and organic matters is used as a drinking water source, a water treatment system can generate harmful disinfection byproducts and bad smell, and a water distribution system is easy to generate the problem of nitrobacteria regeneration; ammonia nitrogen in the underground water can be converted into nitrate after passing through an aquifer oxidation reaction zone, and can cause methemoglobinemia, namely the blue infant syndrome, after being ingested by infants; organic pollution is more likely to cause canceration of the digestive system of the human body.
In recent years, anaerobic microorganisms play an important role in the natural attenuation process of ammonia nitrogen and organic pollutants in underground environment, and attract extensive attention of researchers. In some redox reaction zones of the aquifer, microorganisms are able to utilize nitrate, sulfate, or Fe (iii) (Mn) oxide as electron acceptors and organic species as electron donors for autometabolism under anaerobic or anoxic conditions. In anaerobic areas of contaminated aquifers, the natural degradation capacity of Fe (III) reducing bacteria to benzene and other aromatic compounds is very remarkable, and the Bacillus plays a very important role in the process. Anaerobic iron ammoxidation means that under anaerobic conditions, an ammoxidation process is coupled with an Fe (III) biological reduction process, and the process can convert ammonia nitrogen into nitrogen, nitrite or nitrate. The anaerobic iron ammoxidation can occur in different environments and NH under different conditions4 +Can be anaerobically oxidized to NO3 -、NO2 -、N2And the product difference can be related to the reaction environment and the control condition. The anaerobic iron ammoxidation reaction is easier to generate N according to the judgment of the reaction kinetic energy2Instead of NO2 -And NO3 -[41]。
Because the reaction conditions such as dissolved oxygen are harsher to control by one-step denitrification, no proper reaction condition for realizing NH is available at present4 +Is directly oxidized into N2The problem of nitrite generated by anaerobic iron ammoxidation is solved, and the current technical development of ammonia nitrogen organic pollution remediation by anaerobic iron ammoxidation is limited.
Disclosure of Invention
The embodiment of the invention aims to overcome the defects of the prior art and provide an intermittent aeration type remediation method for underground water ammonia nitrogen and organic pollutants, which can solve the problem of nitrite generated by anaerobic iron ammoxidation and realize efficient and synergistic removal of ammonia nitrogen and organic matters in underground water.
In order to achieve the aim, the invention adopts the technical scheme that:
an intermittent aeration type groundwater ammonia nitrogen and organic pollution organism remediation method comprises the following steps:
carrying out indoor domestication, screening and culture on native indigenous microorganisms derived from flooded paddy field soil to obtain a bacterial liquid of a composite strain, wherein the bacterial liquid contains the domesticated and cultured composite strain which is Fe (III) reducing bacteria, denitrifying bacteria and iron ammonia oxidizing bacteria, and loading the composite strain subjected to domestication culture in the bacterial liquid to the surface of Fe (III) iron oxide minerals with particle size of 2-4mm in a biofilm formation mode to form a biological membrane to obtain a repairing functional material, and adding the repairing functional material into polluted underground water;
under the action of domesticated and cultured Fe (III) reducing bacteria and iron ammonia oxidizing bacteria, Fe (III) on the surface of iron-oxidized mineral in underground water is converted into Fe (II), NH4 +Conversion of NO2 -Conversion of organic matter into middle molecular organic matter, HCO3 -、CO2；
The Fe (II) is aerated and oxidized into Fe (III), NO by intermittent aerobic aeration2 -Oxidation by aeration to NO3 -(ii) a Middle molecular organic matter, HCO3 -、CO2Oxidizing into small molecular organic matters;
in an anaerobic environment, Fe (III) is converted into Fe (II) and NO under the action of domesticated and cultured denitrifying bacteria and iron reducing bacteria3 -Conversion to N2Anaerobic oxidation of small molecule organic matter to HCO3 -、CO2。
The weight ratio of the bacterial liquid volume of the compound bacterial strain to Fe (III) iron oxide minerals is 8-12mL:1 g.
The steps of domesticating, screening and culturing the bacterial liquid of the composite bacterial strain are as follows:
anaerobic treatment of deionized water: putting deionized water into an anaerobic reaction bottle, introducing nitrogen, and performing anaerobic treatment;
adding rice field soil and then vibrating at constant temperature: weighing fresh paddy field soil, adding the fresh paddy field soil into the deionized water after anaerobic treatment, introducing nitrogen, covering a bottle stopper tightly, and oscillating at the constant temperature of 20-25 ℃ for 1.5-2.5h at the rotating speed of 100-150 rpm;
the dosage ratio of the deionized water to the paddy field soil is 40-60 mL: 2-4 g;
bottling: transferring the upper layer bacterium liquid after shaking to an anaerobic reaction bottle filled with a culture medium and Fe (III) iron oxide mineral particles;
the volume-mass ratio of the upper layer bacteria liquid, the culture medium and the Fe (III) iron oxide mineral particles is as follows: 2mL, 15-25mL, 8-12 g;
culturing: introducing N into the anaerobic reaction bottle for 3-6min2And CO2Mixed gas of (2), said N2：CO2The mixing volume ratio is 70-90: 20, culturing for 1 month at room temperature and 25 ℃ in a dark place to obtain a culture bacterial liquid;
subculturing: adding a culture medium into the culture bacterial liquid for 1 time per month to obtain a second-generation culture bacterial liquid, wherein the volume ratio of the culture bacterial liquid to the culture medium is as follows: and (2) 90-110, inoculating 10% volume (v/v) of the second-generation culture bacterial liquid into a freshly prepared culture medium, wherein the volume of the freshly prepared culture medium is 9-11 times of that of the second-generation culture bacterial liquid, and carrying out passage for 3-5 times to obtain the bacterial liquid of the domesticated and cultured composite bacterial strain.
The culture medium is a mixed solution of a trace element mixed solution, Wolfe's vitamin solution and bicarbonate buffer solution; the dosage ratio of the trace element mixed solution mL, the Wolfe's vitamin solution mL and the bicarbonate buffer solution mmol in each liter of culture medium is 8-12: 25-35;
the 1 liter microelement mixed solution comprises the following components in percentage by weight: 0.05-0.1g CoCl2·6H2O，0.21-0.425g MnCl2·4H2O，0.02-0.05g ZnCl2，0.01-0.02g NiCl2·6H2O，0.015-0.03g CuSO4·5H2O，0.01-0.02g Na2MoO4·2H2O，0.01-0.02g Na2SeO4·2H2O。
Further, the culture medium filled in the bottle is a culture medium sterilized by introducing nitrogen gas and high pressure steam for 4-6 min.
The high-pressure steam sterilization treatment is 100-130 ℃ sterilization treatment for 15-25 min.
The Fe (III) iron oxide mineral is hematite, limonite or goethite.
The intermittent aerobic aeration mode comprises the adoption of a ground aeration fan, and the aeration fan is connected with an aeration pipe; or a buried aeration fan is adopted, and the aeration frequency and the aeration flow are changed through automatic control, so that the variable regulation and control of the dissolved oxygen environment in the underground water are realized.
The water inlet constant flow of the underground water is 0.15-0.35 mL/min-1The hydraulic retention time is set to be 3.5-4.5 hours, when aeration is carried out, an aeration valve is opened, the aeration flow is set to be 0.01-0.02L/min, so that the reaction system is in an aerobic state, and the aeration frequency is 10-13 h/d.
The technical scheme provided by the embodiment of the invention has the following beneficial effects:
(1) aiming at the characteristic that the ammonia nitrogen and the organic matters are not completely removed through biological reduction and anaerobic oxidation based on Fe (III), the dissolved oxygen environment is regulated and controlled through intermittent aeration, so that complete denitrification and full-scale oxidation of the organic matters can be realized, the cyclic conversion of Fe (III) and Fe (II) is promoted, the complete oxidation of the ammonia nitrogen to nitrogen is realized, the problem that nitrate nitrogen and nitrite nitrogen generated by anaerobic iron ammoxidation are not completely removed is solved, and the ammonia nitrogen and the organic matters in underground water are synergistically and efficiently removed.
(2) Can realize the further oxidation of the organic matter and can realize the purpose of continuously converting and oxidizing macromolecular and medium molecular organic matter into micromolecular organic matter.
Drawings
FIG. 1 is a schematic flow chart of a repair method provided in embodiment 1 of the present invention;
FIG. 2 is a schematic view of a testing apparatus provided in an embodiment of the present invention;
FIG. 3 is a variation curve of ammonia nitrogen concentration provided by the embodiment of the present invention;
FIG. 4 is a graph illustrating the variation of organic concentration according to an embodiment of the present invention;
FIG. 5 is a graph of the permeability of the reaction medium provided by an example of the present invention.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, embodiments of the present invention will be described in detail with reference to the accompanying drawings.
Example 1
Referring to fig. 1, an intermittent aeration type remediation method for ammonia nitrogen and organic pollutants in underground water comprises the following steps:
carrying out indoor domestication, screening and culture on native indigenous microorganisms derived from flooded paddy field soil to obtain a bacterial liquid of a composite strain, wherein the bacterial liquid contains the domesticated and cultured composite strain which is Fe (III) reducing bacteria, denitrifying bacteria and iron ammonia oxidizing bacteria, loading the domesticated and cultured composite strain in the bacterial liquid to the surface of hematite with particle size of 2-4mm in a membrane hanging manner to form a biological membrane to obtain a repairing functional material, and adding the repairing functional material into polluted underground water; the weight ratio of the bacteria liquid volume of the domesticated and cultured Fe (III) reducing bacteria, denitrifying bacteria and iron ammonia oxidizing bacteria to the hematite is 10mL:1 g;
under the action of domesticated and cultured Fe (III) reducing bacteria and iron ammonia oxidizing bacteria, Fe (III) on the surface of iron-oxidized mineral in underground water is converted into Fe (II), NH4 +Conversion of NO2 -Conversion of organic matter into middle molecular organic matter, HCO3 -、CO2；
The constant inflow rate of the underground water is 0.25 mL/min-1Setting the hydraulic retention time to be 4 hours, opening an aeration valve during aeration, and setting the aeration flow to be 0.01L/min so as to enable the reaction system to be in an aerobic state, wherein the aeration frequency is 12 h/d; the aeration fan is connected with the aeration pipe and adopts a ground type aeration fan; the Fe (II) is aerated and oxidized into Fe (III), NO by intermittent aerobic aeration2 -Oxidation by aeration to NO3 -(ii) a Middle molecular organic matter, HCO3 -、CO2Oxidizing into small molecular organic matters;
in an anaerobic environment, Fe (III) is converted into Fe (II) and NO under the action of domesticated and cultured denitrifying bacteria and iron reducing bacteria3 -Conversion to N2Anaerobic oxidation of small molecule organic matter to HCO3 -、CO2。
The invention relates to an Fe (III) biological reduction anaerobic process, which is a biological process that Fe (III) is used as an electron acceptor, characteristic pollutants such as ammonia nitrogen and organic matters in underground water are used as electron donors, Fe (III) is reduced into Fe (II), the organic matters are oxidized, and the ammonia nitrogen is converted into nitrate nitrogen and nitrite nitrogen by anaerobic oxides under the action of typical domesticated and cultured Fe (III) reducing bacteria. Fe (III) as electron acceptor, soluble Fe (III), i.e. amorphous Fe (III) oxide, may be used; non-soluble fe (iii) oxides, i.e., weakly crystalline fe (iii) oxides or strongly crystalline fe (iii) oxides, may also be employed.
The invention regulates and controls the dissolved oxygen environment through intermittent aeration, further controls the anaerobic iron ammoxidation reaction process, and repairs the ammonia nitrogen and organic pollution of underground water. The problem of nitrite generated by anaerobic iron ammoxidation is solved, complete and thorough denitrification is realized, and the high-efficiency synergistic removal of ammonia nitrogen and organic matters in the underground water is realized.
Further, the general process of acclimatizing and culturing the composite strain comprises the following steps: the indigenous microorganisms in the flooded paddy field, namely dissimilatory Fe (III) reducing bacteria, denitrifying bacteria and iron ammonia oxidizing bacteria, are enriched and cultured as functional microorganisms, and the functional microorganisms are further screened in a laboratory to obtain a mixed strain with optimal growth activity.
The method comprises the following specific steps of domesticating, screening and culturing bacterial liquid of the compound bacterial strain (mainly comprising Fe (III) reducing bacteria, denitrifying bacteria and iron ammonia oxidizing bacteria):
anaerobic treatment of deionized water: 50mL of deionized water is placed in a 100mL anaerobic reaction bottle, and nitrogen is introduced for 5min for anaerobic treatment;
adding fresh rice field soil and then vibrating at constant temperature: weighing 3g of fresh paddy field soil, adding the soil into 50mL of anaerobic treated deionized water, introducing nitrogen for 5 minutes, covering a bottle stopper tightly, and oscillating at a constant temperature of 25 ℃ for 2 hours at a rotating speed of 120 rpm;
bottling: transferring 2mL of the vibrated upper layer bacterial liquid into an anaerobic reaction bottle with the specification of 50mL, wherein 20mL of a culture medium which is subjected to anaerobic treatment by introducing 5min of nitrogen and is subjected to high-pressure steam sterilization treatment at 120 ℃ for 20min and 10g of Fe (III) iron oxide mineral particles after being cleaned and removed of impurities are filled in the anaerobic reaction bottle;
culturing: introducing N into the anaerobic reaction bottle for 5min2And CO2Mixed gas of (2), said N2：CO2The mixing volume ratio is 80: 20, culturing for 1 month at room temperature and 25 ℃ in a dark place to obtain a culture bacterial liquid;
subculturing: adding a culture medium into the culture bacterial liquid for 1 time per month to obtain second-generation culture bacterial liquid, wherein the volume ratio of the culture bacterial liquid to the culture medium is as follows: and (3) taking 10% volume (v/v) of the second-generation culture bacterial liquid, inoculating the second-generation culture bacterial liquid into a freshly prepared culture medium, wherein the volume of the freshly prepared culture medium is 10 times of the volume of the second-generation culture bacterial liquid, and carrying out passage for 4 times to obtain a bacterial liquid of the domesticated and cultured composite bacterial strain.
The culture medium is a mixed solution of 10mL/L, Wolfe's mixed solution of trace elements, 10mL/L vitamin solution and 30mmol L-1 bicarbonate buffer solution;
the 1 liter microelement mixed solution comprises the following components in percentage by weight: 0.1g CoCl2·6H2O，0.425g MnCl2·4H2O，0.05g ZnCl2，0.01g NiCl2·6H2O，0.015g CuSO4·5H2O，0.01g Na2MoO4·2H2O，0.01g Na2SeO4·2H2O。
Example 2
The repairing method of this embodiment is basically the same as that of embodiment 1, except that:
the constant inflow rate of the underground water is 0.15 mL/min-1The hydraulic retention time is set to 4.5 hours, and when aeration is carried out, an aeration valve is opened, the aeration flow is set to 0.02L/min, so that the reaction system is in an aerobic state, and the aeration frequency is 13 h/d.
Fe (III) the iron-oxidizing mineral is goethite;
the weight ratio of the bacterial liquid volume of the domesticated and cultured Fe (III) reducing bacteria, denitrifying bacteria and iron ammonia oxidizing bacteria to the goethite is 8mL:1 g;
the intermittent aerobic aeration of the embodiment adopts a buried aeration fan, and the aeration frequency and the aeration flow are changed through automatic control, so that the variable regulation and control of the dissolved oxygen environment in the underground water are realized.
The method specifically comprises the following steps of domesticating, screening and culturing bacterial liquid of the composite bacterial strain (Fe (III)) reducing bacteria, denitrifying bacteria and iron ammonia oxidizing bacteria:
anaerobic treatment of deionized water: 50mL of deionized water is placed in a 100mL anaerobic reaction bottle, and nitrogen is introduced for 5min for anaerobic treatment;
adding fresh rice field soil and then vibrating at constant temperature: weighing 4g of fresh paddy field soil, adding the soil into 60mL of deionized water subjected to anaerobic treatment, introducing nitrogen for 5 minutes, covering a bottle stopper tightly, and oscillating at a rotation speed of 150rpm and a constant temperature of 20 ℃ for 1.5 hours;
bottling: transferring 2mL of the vibrated upper layer bacterial liquid into an anaerobic reaction bottle with the specification of 50mL, wherein 25mL of a culture medium which is subjected to 6min nitrogen anaerobic treatment and is subjected to 100 ℃ sterilization for 25min high-pressure steam sterilization and 12g of Fe (III) iron oxide mineral particles after being cleaned and removed of impurities are filled in the anaerobic reaction bottle;
the volume-mass ratio of the upper layer bacteria liquid, the culture medium and the Fe (III) iron oxide mineral particles is as follows: 2mL, 15-25mL, 8-12 g;
culturing: introducing 6min N into the anaerobic reaction bottle2And CO2Mixed gas of (2), said N2：CO2The mixing volume ratio is 70: 20, culturing for 1 month at room temperature and 25 ℃ in a dark place to obtain a culture bacterial liquid;
subculturing: adding a culture medium into the culture bacterial liquid for 1 time per month to obtain a second-generation culture bacterial liquid, wherein the volume ratio of the culture bacterial liquid to the culture medium is as follows: and (3) 10:90, inoculating the second-generation culture bacterial liquid with the volume of 10% (v/v) into a freshly prepared culture medium, wherein the volume of the freshly prepared culture medium is 11 times of the volume of the second-generation culture bacterial liquid, and carrying out passage for 3 times to obtain the bacterial liquid of the domesticated and cultured composite bacterial strain.
The culture medium is a mixed solution of 8mL/L, Wolfe's mixed solution of trace elements, 12mL/L vitamin solution and 25mmol L-1 bicarbonate buffer solution;
the 1 liter microelement mixed solution comprises the following components in percentage by weight: 0.05g CoCl2·6H2O，0.3g MnCl2·4H2O，0.02g ZnCl2，0.015g NiCl2·6H2O，0.03g CuSO4·5H2O，0.015g Na2MoO4·2H2O，0.01g Na2SeO4·2H2O。
Example 3
The repairing method of this embodiment is basically the same as that of embodiment 1, except that:
the constant inflow rate of the underground water is 0.35 mL/min-1The hydraulic retention time is set to be 3.5 hours, when aeration is carried out, an aeration valve is opened, the aeration flow is set to be 0.02L/min, so that the reaction system is in an aerobic state, and the aeration frequency is 10 h/d.
Fe (iii) iron oxide minerals are limonites.
The weight ratio of the bacterial liquid volume of the domesticated and cultured Fe (III) reducing bacteria, denitrifying bacteria or iron ammonia oxidizing bacteria to the limonite is 12mL:1 g;
the method specifically comprises the following steps of domesticating, screening and culturing bacterial liquid of the composite bacterial strain (Fe (III)) reducing bacteria, denitrifying bacteria and iron ammonia oxidizing bacteria:
anaerobic treatment of deionized water: 50mL of deionized water is placed in a 100mL anaerobic reaction bottle, and nitrogen is introduced for 5min for anaerobic treatment;
adding fresh rice field soil and then vibrating at constant temperature: weighing 2g of fresh paddy field soil, adding the soil into 40mL of deionized water subjected to anaerobic treatment, introducing nitrogen for 5 minutes, covering a bottle stopper tightly, and oscillating at a constant temperature of 23 ℃ for 2.5 hours at a rotating speed of 100 rpm;
bottling: transferring 2mL of the vibrated upper layer bacterial liquid into an anaerobic reaction bottle with the specification of 50mL, wherein 15mL of a culture medium which is subjected to 6min nitrogen anaerobic treatment and is subjected to 130 ℃ sterilization for 15min high-pressure steam sterilization treatment and 8g of Fe (III) iron oxide mineral particles after being cleaned and removed of impurities are filled in the anaerobic reaction bottle;
the volume-mass ratio of the upper layer bacteria liquid, the culture medium and the Fe (III) iron oxide mineral particles is as follows: 2mL, 15-25mL, 8-12 g;
culturing: introducing 3min N into an anaerobic reaction bottle2And CO2Mixed gas of (2), said N2：CO2The mixing volume ratio is 90: 20, culturing for 1 month at room temperature and 25 ℃ in a dark place to obtain a culture bacterial liquid;
subculturing: adding a culture medium into the culture bacterial liquid for 1 time per month to obtain a second-generation culture bacterial liquid, wherein the volume ratio of the culture bacterial liquid to the culture medium is as follows: and (2) 10:110, inoculating the second-generation culture bacterial liquid with the volume of 10% (v/v) into a freshly prepared culture medium, wherein the volume of the freshly prepared culture medium is 9 times of the volume of the second-generation culture bacterial liquid, and carrying out passage for 5 times to obtain the bacterial liquid of the domesticated and cultured composite bacterial strain.
The culture medium is a mixed solution of 12mL/L, Wolfe's mixed solution of trace elements, 5mL/L vitamin solution and 35mmol L-1 bicarbonate buffer solution.
The 1 liter microelement mixed solution comprises the following components in percentage by weight: 0.07g CoCl2·6H2O，0.21g MnCl2·4H2O，0.03g ZnCl2，0.02g NiCl2·6H2O，0.02g CuSO4·5H2O，0.02g Na2MoO4·2H2O，0.02g Na2SeO4·2H2O。
The principle of the intermittent aeration type groundwater ammonia nitrogen and organic pollution bioremediation method adopted by the invention is as follows: aiming at nitrate nitrogen and nitrite nitrogen (non-complete denitrification) generated by anaerobic iron ammoxidation, an anaerobic and aerobic environment is constructed through intermittent aeration, and the synchronous bioremediation of ammonia nitrogen and organic pollution of underground water is realized. Firstly, an aerobic condition is created by aeration, the aeration flow can be set to be 0.01L/min during aeration, an aeration valve is opened to enable a reaction system to be in an aerobic state, and the conversion of nitrite nitrogen to nitrate nitrogen and Fe are realized2+To Fe3+The cyclic conversion of (2); after 12h of aeration, the aeration valve is closed, and the reaction system enters an anaerobic state. Under the action of denitrifying bacteria and iron reducing bacteria (Fe (III)) reducing bacteria, on one hand, the oxidizing efficiency of organic matters can be enhanced, and the gradual degradation of macromolecular organic matters is promoted; on the other hand, Fe can be realized2+To Fe3+To promote further reduction; finally, the problem of nitrite generated by anaerobic iron ammoxidation can be solved, and the complete and thorough effects are achievedAnd denitrification is performed, so that the ammonia nitrogen and organic matters in the underground water are removed synergistically. The intermittent regulation and control of the dissolved oxygen environment are realized by the circulation. By making an anoxic or aerobic alternate environment, the oxygen supply mode has the advantages of saving energy under the condition of low carbon source, improving the denitrification effect and being beneficial to the short-cut nitrification process.
Comparative examples
(1) Selecting typical Fe (III) iron oxide minerals as natural hematite (alpha-Fe)2O3) For example, the percentage content of Fe element is 55-70%, the semi-metal is to the metallic luster, the Moss hardness is 5.5-6.5, the specific gravity is 4.9-5.3, the granular hematite is sieved into the grain size of 2-4mm, and the grain needs to be washed for 2-3 times by using clean water before the test to remove surface impurities. 200kg of the obtained granular hematite was used as a reaction medium for standby.
(2) Two sets of cylindrical test devices made of organic glass are constructed, as shown in fig. 2, a peristaltic pump 1 is connected with a water inlet pipe 2 through a pipeline, and then is connected with a biological reaction column 4 and a comparison test column 5 through a water inlet pipe 3, the biological reaction column 4 and the comparison test column 5 are respectively connected with a corresponding water outlet barrel 7 through respective water outlet pipes 6, aeration ports 8 are arranged on the biological reaction column 4 and the comparison test column 5, and the two aeration ports 8 are connected with an aeration pump 9 through aeration pipelines. The test device uses 1 multichannel peristaltic pump 1(Longer pump, BT100-2J/YZ1515x) as two sets of test devices for supplying water from bottom to top, one set is a biological reaction device, the hematite in the biological reaction column 3 is loaded with a compound strain for inoculation and domestication culture, and the other set is a non-biological reaction device, and is not loaded with Fe (III) reducing bacteria, denitrifying bacteria and iron ammonia oxidizing bacteria for inoculation and domestication culture. The two sets of test devices are respectively filled with 100kg of filler medium hematite, the filler media are completely the same and are both the granular hematite, and the difference is that the composite strains are inoculated in the load of the filler medium in the biological reaction device, but the composite strains are inoculated in the non-load of the filler medium in the biological reaction device.
(3) Indigenous microorganisms in the flooded paddy field, namely dissimilatory Fe (III) reducing bacteria, denitrifying bacteria and iron ammonia oxidizing bacteria, were cultured by enrichment as functional microorganisms, and further screened in the laboratory according to the method of example 1 to obtain probiotic microorganismsGrowing the mixed strain with the optimal activity to obtain 100L of the bacteria liquid of the domesticated and cultured composite strain for carrying out subsequent tests. The selected flooded paddy field soil is obtained from the middle part of Jiangxi province (N28 degrees 10 ' -28 degrees 45 ', E116 degrees 1 ' -116 degrees 34 '), and the culture medium is 10mL/L, Wolfe's mixed solution of trace elements, 10mL/L vitamin solution and 30mmol L bicarbonate buffer solution-1The mixed solution of (1); the formula of the mixed solution of the trace elements is CoCl2·6H2O(0.1g/L)，MnCl2·4H2O(0.425g/L)，ZnCl2(0.05g/L)，NiCl2·6H2O(0.01g/L)，CuSO4·5H2O(0.015g/L)，Na2MoO4·2H2O(0.01g/L)，Na2SeO4·2H2O(0.01g/L)。
(4) According to the following method, the domesticated and cultured composite strain is loaded and filmed to the surface of hematite: the test apparatus was filled with the filling medium uniformly, 100L of the liquid solution of the acclimatized and cultured complex strain of fe (iii) reducing bacteria, denitrifying bacteria and iron ammonia oxidizing bacteria prepared in example 1 was introduced into the glass test apparatus using 1 multichannel peristaltic pump, the liquid surface was filled, and then the water inlet and the water outlet of the test apparatus were closed to carry out static biofilm formation of the microorganisms for 1 week. And after the film is fully coated for 1 week, opening a water outlet of the glass test device, discharging residual bacteria liquid in the glass test device, circularly injecting normal saline (0.90% sodium chloride solution) into the glass test device by using a peristaltic pump, and flushing interfering eutrophic ions in the culture medium, so that the Fe (III) reducing bacteria, the denitrifying bacteria and the iron ammonia oxidizing bacteria which are subjected to acclimation culture are loaded on the surface of the hematite chelate.
(5) The two sets of test devices use the same water and are taken from underground water polluted by percolate in a certain irregular domestic garbage landfill, and are mainly characterized in that pollutants comprise ammonia nitrogen (heavily polluted) and organic matters (lightly polluted), and the concentration range of the ammonia nitrogen is 16-18mg N/L (the background value is 0.5mg N/L). The COD concentration is 100-120mg/L (the background value is 50mg/L), the carbon-nitrogen ratio of the underground water is disordered, and the pollution belongs to typical low-carbon high-nitrogen type pollution. The concentration of nitrate nitrogen in the system is 1.50mg N/L, and the nitrite nitrogen is lower than the detection limit.
(6) Two sets of test clothesSetting the constant flow of water inlet at 0.25 mL/min-1The hydraulic retention time was set to 4 hours. The aeration pump is manually started at regular time every day, intermittent aeration oxygen supply is respectively carried out on the two sets of test devices at the frequency of 12h/d, the aeration flow is set to be 0.01L/min during aeration, and the aeration valve is opened to enable the test devices to be in an aerobic state. After 12h of aeration, the aeration valve is closed, and the test device is in an anaerobic state. The intermittent regulation and control of the dissolved oxygen environment are realized by the circulation.
(7) The outlet pipe inserts the waste water bucket during test device operation, inserts during the sample in the dry erlenmeyer flask that seals. In order to evaluate the permeability of the packing, the calculation formula is as follows by monitoring the height of the water level in the head pipe and converting the permeability of the reaction medium according to Darcy's law: q is K A (delta h)/L, wherein Q is the seepage flow rate per unit time, K is the permeability coefficient of the reaction medium, A is the cross-sectional area of the water flow, L is the seepage path length, and delta h is the head difference of the monitoring pipe.
After running for a period of time, the water quality indexes of inlet and outlet water are detected, and the following can be found:
as can be seen from FIG. 3, no intermittent aeration was performed 10d before the reaction. When the ammonia nitrogen inflow concentration of underground water is 16-18mg N/L, the reaction is carried out until the 10 th day, the ammonia nitrogen concentration of the effluent of the biological reaction test device is reduced to 5.85mg N/L from 18.50mg N/L, and the ammonia nitrogen removal rate is 68.38%; compared with the prior art, the ammonia nitrogen concentration of the effluent of the non-biological reaction test device is reduced from 16.05mg N/L to 13.60mg N/L, and the ammonia nitrogen removal rate is only 15.26%; this shows that under the condition of no loading of functional microorganisms, hematite is used as a filling medium, and the adsorption, interception and removal effects on ammonia nitrogen are general. After the microorganism is loaded, the anaerobic biological oxidation efficiency of ammonia nitrogen is still better (68.38%) under the condition of underground water flowing. After the 10 th reaction, the oxygenation pump was periodically turned on every day to periodically adjust the dissolved oxygen conditions (12h/d) in the two sets of test units. The ammonia nitrogen concentration of the effluent of the two sets of test devices shows a descending trend when the reaction reaches the 20 th day, wherein the ammonia nitrogen concentration of the effluent of the biological test device is reduced to about 2mg N/L; the ammonia nitrogen concentration of the effluent of the non-biological reaction test device is reduced to about 6mg N/L. Then, by regulating and controlling a carbon source in the reaction system, after 55d of reaction, the concentration of the ammonia nitrogen in the effluent of the biological reaction test device is 0.42mg N/L, and the concentration of the ammonia nitrogen in the effluent of the non-biological reaction test device is 9.51mg N/L, which shows that the ammonia nitrogen in the underground water can be effectively removed by the hematite filler loaded with functional microorganisms, and the biological removal rate is 93%.
As can be seen from FIG. 4, the COD concentration of the effluent of the two groups of test devices is in a trend of rising firstly and then falling firstly before the non-aeration time of 10 days, and the difference of the two groups is small, and the COD concentration of the biological test device is reduced to 50mg/L after the reaction reaches the 10 th day, which shows that organic matters in the groundwater are gradually consumed under the metabolism activity of functional microorganisms. After the 10 th reaction, intermittent aeration is started in the reaction system, the COD concentration of the effluent of the biological reaction test device is 20mg/L and the COD concentration of the effluent of the non-biological reaction test device is 140mg/L after the reaction is carried out to the 20 th reaction, and further the organic matters in the biological reaction system are gradually consumed. As mentioned above, after 20d of reaction, the water inlet of the two sets of test devices is added with glucose, the COD of the water outlet of the non-biological reaction test device rises to a certain extent after 20d of reaction, and the COD of the water outlet of the biological reaction test device is still maintained at 40-60mg/L, which shows that when glucose is added as a carbon source, microorganisms in the reaction system can utilize glucose as the carbon source, and the phenomenon of organic carbon accumulation does not occur, and the addition of glucose well promotes the denitrification process. And in the reaction from the 38 th to the 55 th, the carbon sources in the two groups of test devices are replaced by solid-phase wood chips, so that the COD concentration of the effluent of the two test devices is increased, the COD concentration of the effluent of the non-biological reaction test device is obviously higher than that of the biological reaction test device, the solid-phase carbon source is slowly released along with the reaction, the reduced organic matters and ammonia nitrogen in the reaction system are gradually oxidized and degraded, and the COD concentration of the effluent is finally and integrally maintained at 60 mg/L.
As can be seen from fig. 5, the permeability coefficient of the hematite reaction medium was measured, i.e. calculated by the waterhead measurement device according to the darcy formula. Within the whole operation period of the two groups of test devices, the permeability coefficient K of the hematite filler is relatively stable, and the K value range is (0.11-2.85) multiplied by 103cm·d-1Within this range, this indicates better permeability of the mixed filler. In contrast, twoThe difference of the K value of the permeability coefficient of the reaction medium in the group test device is not large, which shows that the influence of the loaded microorganism on the permeability coefficient of the hematite filler is not large, the groundwater cannot be blocked in a flowing state, and the groundwater remediation application prospect is better.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents, improvements and the like that fall within the spirit and principle of the present invention are intended to be included therein.
Claims (9)
1. An intermittent aeration type groundwater ammonia nitrogen and organic pollution organism remediation method is characterized by comprising the following steps:
carrying out indoor domestication, screening and culture on native indigenous microorganisms derived from flooded paddy field soil to obtain a bacterial liquid of a composite strain, wherein the bacterial liquid contains the domesticated and cultured composite strain which is Fe (III) reducing bacteria, denitrifying bacteria and iron ammonia oxidizing bacteria, and loading the composite strain subjected to domestication culture in the bacterial liquid to the surface of Fe (III) iron oxide minerals with particle size of 2-4mm in a biofilm formation mode to form a biological membrane to obtain a repairing functional material, and adding the repairing functional material into polluted underground water;
under the action of domesticated and cultured Fe (III) reducing bacteria and iron ammonia oxidizing bacteria, Fe (III) on the surface of iron-oxidized mineral in underground water is converted into Fe (II), NH4 +Conversion of NO2 -Conversion of organic matter into middle molecular organic matter, HCO3 -、CO2；
The Fe (II) is aerated and oxidized into Fe (III), NO by intermittent aerobic aeration2 -Oxidation by aeration to NO3 -(ii) a Middle molecular organic matter, HCO3 -、CO2Oxidizing into small molecular organic matters;
in an anaerobic environment, Fe (III) is converted into Fe (II) and NO under the action of domesticated and cultured denitrifying bacteria and iron reducing bacteria3 -Conversion to N2Anaerobic oxidation of small molecule organic matter to HCO3 -、CO2。
2. The repair method according to claim 1, characterized in that:
the weight ratio of the bacterial liquid volume of the compound bacterial strain to Fe (III) iron oxide minerals is 8-12mL:1 g.
3. The repair method according to claim 2, characterized in that:
the steps of domesticating, screening and culturing the bacterial liquid of the composite bacterial strain are as follows:
anaerobic treatment of deionized water: putting deionized water into an anaerobic reaction bottle, introducing nitrogen, and performing anaerobic treatment;
adding rice field soil and then vibrating at constant temperature: weighing fresh paddy field soil, adding the fresh paddy field soil into the deionized water after anaerobic treatment, introducing nitrogen, covering a bottle stopper tightly, and oscillating at the constant temperature of 20-25 ℃ for 1.5-2.5h at the rotating speed of 100-150 rpm;
the dosage ratio of the deionized water to the paddy field soil is 40-60 mL: 2-4 g;
bottling: transferring the upper layer bacterium liquid after shaking to an anaerobic reaction bottle filled with a culture medium and Fe (III) iron oxide mineral particles;
the volume-mass ratio of the upper layer bacteria liquid, the culture medium and the Fe (III) iron oxide mineral particles is as follows: 2mL, 15-25mL, 8-12 g;
culturing: introducing N into the anaerobic reaction bottle for 3-6min2And CO2Mixed gas of (2), said N2：CO2The mixing volume ratio is 70-90: 20, culturing for 1 month at room temperature and 25 ℃ in a dark place to obtain a culture bacterial liquid;
subculturing: adding a culture medium into the culture bacterial liquid for 1 time per month to obtain a second-generation culture bacterial liquid, wherein the volume ratio of the culture bacterial liquid to the culture medium is as follows: and (2) 90-110, inoculating 10% volume (v/v) of the second-generation culture bacterial liquid into a freshly prepared culture medium, wherein the volume of the freshly prepared culture medium is 9-11 times of that of the second-generation culture bacterial liquid, and carrying out passage for 3-5 times to obtain the bacterial liquid of the domesticated and cultured composite bacterial strain.
4. The method for repairing according to claim 3, wherein the medium is a mixed solution of trace elements, a vitamin solution of Wolfe's and a bicarbonate buffer; the dosage ratio of the trace element mixed solution mL, the Wolfe's vitamin solution mL and the bicarbonate buffer solution mmol in each liter of culture medium is 8-12: 25-35;
the 1 liter microelement mixed solution comprises the following components in percentage by weight: 0.05-0.1g CoCl2·6H2O，0.21-0.425g MnCl2·4H2O，0.02-0.05g ZnCl2，0.01-0.02g NiCl2·6H2O，0.015-0.03g CuSO4·5H2O，0.01-0.02g Na2MoO4·2H2O，0.01-0.02g Na2SeO4·2H2O。
5. The repairing method according to claim 4, wherein the medium filled in the flask is a medium sterilized by introducing nitrogen gas and high pressure steam for 4 to 6 min.
6. The repair method according to claim 5, wherein the high pressure steam sterilization treatment is 100-130 ℃ sterilization treatment for 15-25 min.
7. The repair method according to claim 6, wherein the Fe (III) iron oxide mineral is hematite, limonite or goethite.
8. The remediation method of any one of claims 1 to 7 wherein the intermittent aerobic aeration comprises a ground-based aeration blower connected to an aeration pipe; or a buried aeration fan is adopted, and the aeration frequency and the aeration flow are changed through automatic control, so that the variable regulation and control of the dissolved oxygen environment in the underground water are realized.
9. The method of remediation of claim 8 wherein the constant rate of inflow of groundwater is from 0.15 to 0.35 mL-min-1The hydraulic retention time is set to be 3.5-4.5 hours, when aeration is carried out, an aeration valve is opened, the aeration flow is set to be 0.01-0.02L/min, so that the reaction system is in an aerobic state, and the aeration frequency is 10-13 h/d.
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| CN113526669A (en) * | 2021-07-22 | 2021-10-22 | 南京佳荣再生物资回收有限公司 | Intermittent aeration type landfill leachate ammonia nitrogen and organic pollution bioremediation device and method |
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