CN113003717A - Device and process for enhancing denitrification anaerobic methane oxidation denitrification based on magnetite - Google Patents
Device and process for enhancing denitrification anaerobic methane oxidation denitrification based on magnetite Download PDFInfo
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Abstract
The invention discloses a device and a process for treating nitrogen-containing wastewater based on magnetite-enhanced denitrification anaerobic methane oxidation, wherein magnetite ores are processed and added into a membrane biological aeration reactor according to the iron concentration of 10g/L to be stirred to be uniformly mixed. The invention can achieve the following effects: the magnetite is thrown and to be expected to make the microorganism diversity increase in the membrane aeration bioreactor, improves its denitrogenation efficiency, and magnetite also can promote the direct electron transfer process between the microorganism kind as conductor material moreover for nitrogen gets rid of efficiency and improves. The process not only achieves the removal of nitrogen, but also can achieve the purpose of simultaneously removing methane, reduces the emission of greenhouse gases and has obvious environmental benefit. In addition, the process has the characteristics of low investment cost, high environmental benefit, economic value, stable operation and the like.
Description
Technical Field
The invention relates to a device and a process for treating nitrogen-containing wastewater.
Background
Nitrogen is an important nutrient for plants, mainly derived from human excrement and some industrial wastewater, and is one of the main pollutants causing eutrophication of some slow-flowing water bodies. Meanwhile, many algae can secrete algal toxins to produce toxic effects on aquatic organisms and human health, and digestive tract inflammation can be caused if people carelessly drink the algal toxins produced by the blue algae. Methane is an important fossil fuel, but is also a not negligible greenhouse gas, and its contribution to the greenhouse effect is second only to carbon dioxide, reaching 20%, but its effect on global warming is 25 times that of carbon dioxide. Therefore, the control of the methane concentration has important significance for controlling global warming.
The traditional biological denitrification technology cannot avoid adding an external carbon source, but the adding of organic matters not only can increase the operation cost, but also can possibly cause secondary pollution. The denitrifying anaerobic methane is a process for synchronously denitrifying and removing methane by taking methane as an independent electron donor and nitrate radical/nitrate radical as a final electron acceptor. However, because the denitrification anaerobic methane oxidation function microorganism is difficult to enrich, the multiplication time is long, and the requirement on the environmental growth condition is strict, the practical application of the technology is limited.
The methane is directly transferred from the surface of the hollow fiber membrane to the surface of the functional microorganism by constructing the membrane aeration bioreactor, so that the mass transfer rate of methane gas is accelerated. And the hollow fiber membrane has huge specific surface area, can provide a place for the growth of microorganisms, and reduces the loss of the microorganisms in the reactor. And researches show that the anaerobic methane-oxidizing archaea has the capability of directly transferring electrons between inoculations. Magnetite is a black octahedral or dodecahedral crystalline form mineral widely found in nature, and is a conductive mineral containing divalent and trivalent iron in a ratio of 1: 2. Magnetite is widely used in anaerobic reactors. The magnetite can be used as a conductor material to promote direct electron transfer among microbial species, and the magnetite is added into the membrane bioreactor to promote the generation of a direct electron transfer process among microbial species with higher electron transfer efficiency and more stability, so that the denitrification efficiency of the membrane bioreactor is improved.
Disclosure of Invention
In order to solve the problems of low denitrification efficiency of anaerobic methane oxidation and denitrification, difficult growth of functional microorganisms in the process, long multiplication time and the like, the invention provides the following technical scheme: the utility model provides a device based on denitrification anaerobism methane oxidation denitrogenation is reinforceed to magnetite, includes the membrane bioreactor barrel that is equipped with constant temperature heat preservation, and this membrane bioreactor barrel distributes from bottom to top in proper order has membrane bioreactor base, membrane bioreactor water inlet, membrane bioreactor air inlet, membrane bioreactor granule mud district, hollow fiber membrane module, membrane bioreactor suspension mud district, membrane bioreactor upper cover and reactor three-phase separator. One end of the pipe iii is connected with an exhaust pipeline fixed at the top end of the membrane bioreactor, and the other end is connected with a gas collecting device. The gas cylinder filled with high-purity methane is connected with a gas flow meter through a pipe iv, and then enters the hollow fiber membrane component through a valve ii and a gas inlet of the membrane bioreactor. One end of the membrane bioreactor water inlet pump is connected with the valve i through the pipe ii, water enters through the water inlet of the membrane bioreactor, and the other end of the membrane bioreactor water inlet pump is connected with the pipe i through the water inlet tank. The water outlet of the membrane bioreactor is connected with a valve iii and enters a water outlet tank through a pipe vi; the method is characterized in that: the process for treating the nitrogen-containing wastewater by using the device to perform denitrification anaerobic methane oxidation comprises the following procedures:
1) the used membrane bioreactor cylinder is an up-flow anaerobic sludge bed reactor.
2) The membrane bioreactor uses digested sludge from an anaerobic sludge fermentor as a seed sludge with a sludge concentration (MLSS) of 15-20 g/L.
3) 27-33 hollow fiber membranes with the length of 24-28cm are folded in half to form a hollow fiber membrane component, and the port of the membrane component is connected with the air inlet of the membrane bioreactor.
4) The processing mode of the added magnetite is as follows; firstly, mechanically crushing and grinding magnetite ore into magnetite powder particles, and then screening to obtain magnetite small particles with the particle size of 1-2 mm; washing with dilute hydrochloric acid once to remove impurities on the surface of the particles, washing with ultrapure water for 3 times, and drying in a vacuum drying oven for 10 h.
5) Opening the upper cover of the membrane bioreactor, adding magnetite with the iron concentration of 10g/L, and stirring with a glass rod for 10-20 minutes to ensure that one part of the magnetite is attached to the hollow fiber membrane component and the rest part is mixed with the granular sludge area of the membrane bioreactor.
6) And opening a water inlet pump of the membrane bioreactor, and enabling the wastewater containing nitrate and ammonia nitrogen to sequentially enter a granular sludge area, a suspended sludge area and a three-phase separator of the membrane bioreactor from a water inlet tank through a pipe i, the water inlet pump, a pipe ii, a valve i, a base of the membrane bioreactor and a water inlet of the membrane bioreactor, and finally flow into a water outlet tank through a water outlet valve iii and a pipe vi.
7) The temperature in the cylinder body of the membrane bioreactor is controlled at 28-30 ℃, the pH in the cylinder body of the membrane bioreactor is controlled at 7.0-7.2, and the hydraulic retention time of the membrane bioreactor is controlled at 21-23 hours.
8) Methane enters the hollow fiber membrane module through pipe iv, flow meter, valve ii and membrane bioreactor inlet. The flow rate of the methane gas is controlled to be 10-15 mL/min.
9) Excess methane which is emitted by the hollow fiber membrane component and is not dissolved in the water body enters the gas collecting device through the three-phase separator fixed on the upper cover of the membrane bioreactor, the exhaust pipeline of the membrane bioreactor and the pipe iii.
The device and the process for treating the nitrogen-containing wastewater based on magnetite enhanced denitrification anaerobic methane oxidation are characterized in that; the magnetite can be used as a conductor material to promote the direct intermediate electron transfer of microorganisms, and can also supplement cytochrome C to promote the inter-microbial-species electron transfer, and functional microorganisms on the surface in the denitrification anaerobic methane oxidation process have the direct inter-microbial-species electron transfer capacity, and the membrane bioreactor can be used for successfully enriching the denitrification anaerobic methane oxidation functional microorganisms on the surface of membrane filaments to form an agglomeration state, so that the inter-microbial-species electron transfer is facilitated. In addition, the process adds ammonium chloride into the water inlet tank, and the ammonium chloride reacts with nitrite generated in the oxidation process of the denitrifying anaerobic methane in the membrane bioreactor, so that not only can the toxic action of nitrate on microorganisms be realized, but also nitrate, nitrite and ammonia nitrogen can be removed simultaneously. The process has the characteristics of low investment cost, high environmental benefit, economic value, stable operation and the like.
Drawings
FIG. 1 is a schematic diagram of a device and a process based on magnetite enhanced denitrification anaerobic methane oxidation denitrification.
FIG. 2 is a schematic diagram of ammonia nitrogen removal effect of a device and a process based on ore enhanced denitrification anaerobic methane oxidation denitrification.
In fig. 1: 1. the system comprises a water inlet tank, 2, pipes i and 3, a membrane bioreactor water inlet pump, 4, pipes ii and 5, valves i and 6, a membrane bioreactor base, 7, a membrane bioreactor water inlet, 8, a membrane bioreactor air inlet, 9, a membrane bioreactor heat-insulating layer, 10, a hollow fiber membrane component, 11, a membrane bioreactor cylinder, 12, a membrane bioreactor three-phase separator, 13, a membrane bioreactor exhaust pipeline, 14 pipes iii and 15, a gas collecting device, 16, valves iii and 17, a water outlet pipe, 18, a water outlet tank, 19, a membrane bioreactor granular sludge area, 20, a membrane bioreactor suspended sludge area, 21, a methane gas cylinder, 22, pipes iv and 23, a flow meter, 24, valves ii and 25 and a membrane bioreactor upper cover.
Detailed Description
The device and the process for treating the nitrogen-containing wastewater by using the magnetite-enhanced denitrification anaerobic methane oxidation have the application mechanism that:
1. magnetite is a conductor material consisting of ferrous iron and ferric iron in a ratio of 1: 2. The magnetite provides growth support for the dissimilatory iron reducing bacteria. The addition of the magnetite changes the microbial community structure in the membrane bioreactor, so that the abundance of microorganisms with denitrification capability is increased.
2. The direct electron transfer between microbe species is a high-efficiency electron transfer process which can directly transfer electrons between microbes without passing through intermediates such as hydrogen, formic acid and the like. Magnetite, as a conductive material, acts as cytochrome c and thus facilitates the direct electron transfer process between microbial species.
3. Based on two functions of magnetite, the magnetite is added into the membrane bioreactor, and the addition of the magnetite can lead various microorganisms in the membrane bioreactor to play a synergistic role in the processes of direct electronic transmission among species of microorganism populations and the like, thereby accelerating the reduction process of nitrogen.
The invention is further illustrated with reference to the following figures and examples:
as shown in figure 1, the magnetite-based enhanced denitrification anaerobic methane oxidation denitrification device has the following technical characteristics: the membrane bioreactor comprises a membrane bioreactor cylinder 11 provided with a constant temperature insulation layer 9, wherein a membrane bioreactor base 6, a membrane bioreactor water inlet 7, a membrane bioreactor air inlet 8, a membrane bioreactor granular sludge area 19, a hollow fiber membrane component 10, a membrane bioreactor suspended sludge area 20, a membrane bioreactor upper cover 25 and a reactor three-phase separator 12 are sequentially distributed on the membrane bioreactor cylinder 11 from bottom to top, one end of a pipe iii-14 is connected with an exhaust pipeline 13 fixed at the top end of the membrane bioreactor, and the other end of the pipe iii-14 is connected with a gas collecting device 15. A gas cylinder 21 filled with high-purity methane is connected with a gas flow meter 23 through a pipe iv-22 and then enters the hollow fiber membrane module 10 through a valve ii-24 and a membrane bioreactor gas inlet 8. One end of the membrane bioreactor water inlet pump 3 is connected with the valve i-5 through the pipe ii-4 and the water inlet 7 of the membrane bioreactor, and the other end is connected with the pipe i-2 through the water inlet tank 1. The water outlet of the membrane bioreactor is connected with a valve iii-16 and enters a water outlet tank 18 through a pipe vi-17.
The process for treating the nitrogen-containing wastewater by using the device to perform denitrification anaerobic methane oxidation comprises the following specific operation procedures:
the used membrane bioreactor cylinder 11 is an up-flow anaerobic sludge bed reactor.
The membrane bioreactor barrel 11 uses digested sludge from an anaerobic sludge fermentor as a seed sludge with a sludge concentration (MLSS) of 15-20 g/L.
27-33 hollow fiber membranes with the length of 24-28cm are folded in half to form a hollow fiber membrane component 10, and the port of the membrane component is connected with the air inlet 8 of the membrane bioreactor. The optimal length of the hollow fiber membrane is 30cm, and the optimal number of the hollow fiber membranes is 26.
The processing mode of the added magnetite is as follows; firstly, mechanically crushing and grinding magnetite ore into magnetite powder particles, and then screening to obtain magnetite small particles with the particle size of 1-2 mm; washing with dilute hydrochloric acid once to remove impurities on the surface of the particles, washing with ultrapure water for 3 times, and drying in a vacuum drying oven for 10 h.
Opening the upper cover 25 of the membrane bioreactor, adding magnetite with the iron concentration of 10g/L, and stirring for 10-20 minutes by using a glass rod, wherein the optimal time is 15 minutes, so that a part of the magnetite is attached to the hollow fiber membrane component 10, and the rest part of the magnetite is mixed with the granular sludge zone 19 of the membrane bioreactor.
And opening a water inlet pump 3 of the membrane bioreactor, and allowing the wastewater containing nitrate and ammonia nitrogen to sequentially enter a granular sludge zone 19 of the membrane bioreactor, a suspended sludge zone 20 of the membrane bioreactor and a three-phase separator 12 of the membrane bioreactor from a water inlet tank through a pipe i-2, the water inlet pump 3, a pipe ii-4, a valve i-5, a base 6 of the membrane bioreactor and a water inlet 7 of the membrane bioreactor, and finally to flow into a water outlet tank 18 through a water outlet valve iii-16 and a pipe vi-17.
The temperature of the barrel body 11 of the membrane bioreactor is controlled at 28-30 ℃, and the optimal temperature is 30 ℃; the pH value of the barrel body 11 of the membrane bioreactor is controlled between 7.0 and 7.2, and the optimal pH value is 7.2; the hydraulic retention time of the cylinder 11 of the membrane bioreactor is controlled to be 21-23 hours, and the optimal hydraulic retention time is 22 hours.
Methane enters the hollow fiber membrane module 10 through pipe iv-22, flow meter 23, valves ii-24 and membrane bioreactor inlet 8. Controlling the flow rate of methane gas at 10-15 mL/min; the optimum flow rate is 10 mL/min.
Excess methane which is emitted by the hollow fiber membrane component 10 and is not dissolved in the water body enters the gas collecting device 15 through the three-phase separator 12 fixed on the upper cover 25 of the membrane bioreactor, the exhaust pipeline 13 of the membrane bioreactor and the pipes iii-14.
Example 1:
an up-flow anaerobic sludge bed reactor with the effective volume of 1L is used as a membrane bioreactor cylinder body, and sludge in an anaerobic fermentation tank is inoculated, so that the concentration of the sludge in the reactor is 16 g/L. The inlet water is artificial simulated nitrogen-containing wastewater, wherein NO is3N concentration of 50mg/L, NH4 +The concentration of N-N was 50 mg/L. The pH was 7.0 and the gas flow rate was 10 mL/min. The temperature of the heat-insulating layer of the membrane bioreactor is 30 ℃, and the hydraulic retention time is 23 hours. As shown in figure 2, the removal efficiency of ammonia nitrogen after adding magnetite is 30%, which is 25% higher than that of a blank reactor.
Claims (1)
1. A denitrification anaerobic methane oxidation denitrification device and a process based on magnetite strengthening comprises a membrane bioreactor barrel (11) provided with a constant temperature insulation layer (9), wherein a membrane bioreactor base (6), a membrane bioreactor water inlet (7), a membrane bioreactor air inlet (8), a membrane bioreactor granular sludge area (19), a hollow fiber membrane component (10), a membrane bioreactor suspended sludge area (20), a membrane bioreactor upper cover (25) and a reactor three-phase separator (12) are sequentially distributed on the membrane bioreactor barrel (11) from bottom to top, one end of a pipe iii (14) is connected with an exhaust pipeline (13) fixed at the top end of the membrane bioreactor, and the other end of the pipe iii (14) is connected with a gas collecting device (15); a gas cylinder (21) filled with high-purity methane is connected with a gas flow meter (23) through a pipe iv (22), and then enters the hollow fiber membrane component (10) through a valve ii (24) through a gas inlet (8) of the membrane bioreactor; one end of a membrane bioreactor water inlet pump (3) is connected with a valve i (5) through a pipe ii (4) and is used for water inlet through a membrane bioreactor water inlet (7), and the other end of the membrane bioreactor water inlet pump is connected with a pipe i (2) through a water inlet tank (1); the water outlet of the membrane bioreactor is connected with a valve iii (16) and enters a water outlet tank (18) through a pipe vi (17); the method is characterized in that the anaerobic biological process for treating the nitrogen-containing wastewater by using the device comprises the following specific operation processes:
1) the used membrane bioreactor cylinder (11) is an up-flow anaerobic sludge bed reactor;
2) the membrane bioreactor cylinder (11) uses the digested sludge from the anaerobic sludge fermentation tank as the seed sludge, and the sludge concentration (MLSS) is 15-20 g/L;
3) 27-33 hollow fiber membranes with the length of 24-28cm are folded in half to form a hollow fiber membrane component (10), and the port of the membrane component is connected with the air inlet (8) of the membrane bioreactor;
4) the processing mode of the added magnetite is as follows; firstly, mechanically crushing and grinding magnetite ore into magnetite powder particles, and then screening to obtain magnetite small particles with the particle size of 1-2 mm; washing with dilute hydrochloric acid once to remove impurities on the surface of the particles, washing with ultrapure water for 3 times, and drying in a vacuum drying oven for 10 h;
5) opening an upper cover (25) of the membrane bioreactor, adding magnetite with the iron concentration of 10g/L, and stirring for 10-20 minutes by using a glass rod to ensure that one part of the magnetite is attached to the hollow fiber membrane component (10) and the rest part of the magnetite is mixed with a granular sludge area (19) of the membrane bioreactor;
6) opening a water inlet pump (3) of the membrane bioreactor, and enabling the wastewater containing nitrate and ammonia nitrogen to sequentially enter a granular sludge zone (19), a suspended sludge zone (20) and a three-phase separator (12) of the membrane bioreactor from a water inlet tank through a pipe i (2), the water inlet pump (3), a pipe ii (4), a valve i (5), a base (6) of the membrane bioreactor and a water inlet (7) of the membrane bioreactor, and finally flow into a water outlet tank (18) through a water outlet valve iii (16) and a pipe vi (17);
7) the temperature of the cylinder body (11) of the membrane bioreactor is controlled to be 28-30 ℃, the pH of the cylinder body (11) of the membrane bioreactor is controlled to be 7.0-7.2, and the hydraulic retention time of the cylinder body (11) of the membrane bioreactor is controlled to be 21-23 hours;
8) methane enters the hollow fiber membrane module (10) through a pipe iv (22), a flow meter (23), a valve ii (24) and a membrane bioreactor air inlet (8); controlling the flow rate of methane gas at 10-15 mL/min;
9) excess methane which is scattered by the hollow fiber membrane component (10) and not dissolved in water enters a gas collecting device (15) through a three-phase separator (12) fixed on an upper cover (25) of the membrane bioreactor, an exhaust pipeline (13) of the membrane bioreactor and a pipe iii (14).
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| CN112093994A (en) * | 2020-09-23 | 2020-12-18 | 四川农业大学 | CW-MFC device and method for reducing methane and ammonia nitrogen pollution |
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Application publication date: 20210622 |