CN106927571B - Method for enhancing denitrification of constructed wetland by using strong carbon-secreting modified biochar - Google Patents
Method for enhancing denitrification of constructed wetland by using strong carbon-secreting modified biochar Download PDFInfo
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Abstract
The invention relates to a method for strengthening constructed wetland denitrification by utilizing strong carbon-secreting modified biochar, which is characterized in that the strong carbon-secreting modified biochar is used as a treating agent to strengthen the constructed wetland for denitrification, the strong carbon-secreting modified biochar is mixed with a matrix and filled into an artificial wetland bed body, or is directly used as a filler column and embedded into the artificial wetland bed body for denitrification, and the strong carbon-secreting modified biochar is obtained by taking wetland plants as raw materials, performing low-temperature dry distillation and then loading ferrous iron; the denitrification treatment temperature is 0-40 ℃, the pH is 6-8, and the total nitrogen content of the constructed wetland sewage is 5-60 mg/L. The invention utilizes strong carbon-secreting modified biochar to strengthen the denitrification of the constructed wetland, and obtains unexpected effect, when in application, Fe (II) can be used as an electron donor to transfer electrons to high-valence nitrogen (such as NO) through simple and convenient loading of Fe (II)3 ‑，NO2 ‑) The nitrogen in high valence state can be reduced into nitrogen while being oxidized, so that the chemical denitrification process is realized, and the high-efficiency denitrification is realized.
Description
Technical Field
The invention relates to a constructed wetland denitrification method, in particular to a method for strengthening constructed wetland chemistry and microorganism denitrification by utilizing strong carbon-secreting modified biochar, belonging to the technical field of environmental engineering sewage treatment
Background
As a unique composite ecological sewage treatment technology consisting of plants, matrixes, microorganisms and the like, the artificial wetland has outstanding application advantages in the standard-reaching tail water deep treatment of sewage treatment plants in developing regions, and gradually becomes one of the new methods commonly used for deep purification of sewage. However, because the carbon-nitrogen ratio in the tail water reaching the standard is low and the nitrate nitrogen content is high, the denitrification effect of the artificial wetland is often inhibited. In addition, the biomass area of wetland plants generated in China every year reaches more than five million hectares, part of the wetland plants are ingested by wetland animals and enter a biological chain, most plants wither and die directly, if a large number of wetland plants cannot be removed in time, the plants are decomposed after being corrupted and released into a wetland water body again, and the quality of the atmospheric environment is influenced by adopting an incineration method in some places. The lack of high value resource technology results in huge resource waste and potential secondary pollution risk.
With the increasing tightening of the discharge standard of the total nitrogen in the sewage, how to organically combine the efficient denitrification and the resource utilization of the plants in the artificial wetland is a difficult problem to be solved urgently. The research on directly burying wetland plants into the wetland to provide a carbon source has the problems that the plant decay time is difficult to control, the wetland is easy to block, the effluent chromaticity is increased and the like; chinese patent document CN103936161A discloses a method and a system for enhancing nitrogen removal efficiency of low-carbon high-nitrogen sewage by using a plant carbon source in an artificial wetland, which utilizes plant hydrolysate as a wetland organic carbon source to enhance nitrogen removal efficiency of sewage, but the method is complex to operate, and hydrolysis waste exists, so that maximum utilization of plants is not realized.
Biochar (Biochar) is a lamellar porous environment functional material which is generated by carbonizing biomass in a low-oxygen environment and has extremely rich carbon content and is closely stacked. In recent years, biochar is used as greenhouse gas N2The method has great application potential in aspects of O emission reduction, soil improvement and restoration, pollutant adsorption and the like, and is widely concerned. The biochar is simple and convenient to prepare, does not need to be activated, and has the cost of about 1/6 of the activated carbon. The introduction of the biochar in the artificial wetland system can provide a potential solution for realizing the resource utilization of plants and the improvement of the wetland effect at the same time.
Chinese patent document CN 104761057a discloses a concept of adding biochar into a vertical flow artificial wetland, but the patent does not specifically suggest a method for preparing biochar, a biochar carbon source release characteristic, and a microbial-biochar denitrification mechanism. At present, biochar is mostly used as an adsorbent or a soil conditioner, the application of denitrification enhanced nitrogen removal is rarely reported, and most biochar is prepared at high temperature at present, most organic matters are gasified, and the capability of providing a carbon source is extremely limited. Therefore, the research and development of the novel high carbon secretion type wetland substrate has important significance for promoting the denitrification effect of the wetland and realizing the high-efficiency utilization of wetland plant resources.
Disclosure of Invention
Aiming at the defects of the prior art, the invention provides a method for enhancing the denitrification of the constructed wetland by using strong carbon-secreting modified biochar, which has high treatment efficiency.
The invention is realized by the following technical scheme:
a method for strengthening denitrification of an artificial wetland by using strong carbon-secreting modified biochar comprises the steps of using the strong carbon-secreting modified biochar as a treating agent to strengthen the artificial wetland for denitrification, mixing the strong carbon-secreting modified biochar with a matrix and filling the mixture into an artificial wetland bed body, or directly using the mixture as a filler column to be embedded into the artificial wetland bed body for carrying out denitrification, wherein the strong carbon-secreting modified biochar is obtained by using wetland plants as raw materials, carrying ferrous iron after low-temperature dry distillation; the denitrification treatment temperature is 0-40 ℃, the pH is 6-8, and the total nitrogen content of the constructed wetland sewage is 5-60 mg/L.
Preferably, the denitrification treatment temperature is 10-30 ℃, the pH value is 6-7, and the total nitrogen content of the constructed wetland sewage is 20-40 mg/L.
According to the invention, the volume ratio of the strong carbon-secreting type modified biochar to the matrix is preferably 1: 20-1: 2, the volume ratio of the strong carbon-secreting type modified biochar to the matrix is further preferably 1: 10-1: 3, and the most preferably volume ratio of the strong carbon-secreting type modified biochar to the matrix is 1: 3.
In the invention, the substrate is preferably one or a mixture of more than two of gravel, construction waste bricks or quartz sand.
Preferably, the total coverage area of the strong carbon-secreting modified biochar mixed with the matrix accounts for 1/3-2/3 of the total area of the wetland, and the porosity of the strong carbon-secreting modified biochar mixed and filled with the matrix is 20-50%; preferably, the porosity of the strong carbon-secreting modified biochar after being mixed and filled with the matrix is 30-40%.
According to the invention, the preferred method directly used as the filler column is to fill the biochar into the filler column, then vertically embed the filler column into the artificial wetland bed body, and the ratio of the total volume of the biochar to the volume of the wetland is 1: 20-1: 4; the packed column is a perforated column, the aperture is 0.5-1 cm, and the aperture ratio is 40-80%.
More preferably, the covering area of the filler columns accounts for 1/20-2/3 of the surface area of the wetland.
Preferably, the strong carbon-secreting modified biochar is prepared by the following method:
(1) cleaning wetland plants serving as raw materials, crushing the wetland plants into blocks with the diameter of 1-3 cm, and air-drying the blocks to constant weight;
(2) carrying out rapid carbonization treatment on the wetland plants treated in the step (1) at a low temperature in a dry distillation mode under the protection of inert gas to obtain biochar; the dry distillation temperature is 250-400 ℃, the heating rate is 5-10 ℃/min, and the dry distillation time is 30-60 min;
(3) and load modification treatment: and (3) mixing the biochar prepared in the step (2) with 0.5-3 mol/L ferrous chloride solution, standing for 12-16 h for carrying ferrous, washing the carried biochar with deionized water to be neutral, and drying in an anaerobic environment at 100-120 ℃ for 6-12 h to obtain the strong carbon-secreting modified biochar.
In the invention, the root or stem of the wetland plant is preferably selected as the raw material in the step (1).
Preferably, the wetland plants in the step (1) are one or more than two of wetland common plants of giant reed, brocade, salix integra and the like.
Preferably, the inert gas in step (2) is nitrogen.
Preferably, the dry distillation temperature in the step (2) is 250-300 ℃, the heating rate is 5-8 ℃/min, and the dry distillation time is 40-60 min.
Most preferably, the dry distillation temperature in the step (2) is 300 ℃, the heating rate is 5-8 ℃/min, and the dry distillation time is 60 min.
According to the invention, the concentration of the ferrous chloride solution in the step (3) is preferably 1-3 mol/L, and the most preferably, the concentration of the ferrous chloride solution is 3 mol/L.
According to the invention, the loading time of the step (3) is 12 h.
According to the invention, the anaerobic drying temperature in the step (3) is preferably 100-110 ℃, the drying time is 8-12 h, and most preferably, the anaerobic drying temperature in the step (3) is 105 ℃, and the drying time is 12 h.
The method for enhancing the denitrification of the artificial wetland by using the strong carbon-secreting modified biochar obtains unexpected effects.
The raw materials and equipment used in the invention are all the prior art.
Compared with the prior art, the invention has the following advantages:
(1) the invention utilizes strong carbon-secreting modified biochar to strengthen the denitrification of the constructed wetland, and obtains unexpected effect, when in application, Fe (II) can be used as an electron donor to transfer electrons to high-valence nitrogen (such as NO)3 -，NO2 -) The nitrogen with high valence can be reduced into nitrogen while being oxidized, and the chemical denitrification process is realized. Meanwhile, the microorganism can also take ferrous iron and nitrate as an electron donor and an electron acceptor respectively to oxidize the ferrous iron into ferric iron and reduce the nitrate simultaneously so as to remove NO3 -Conversion to N2. In addition, when NO is present in the reaction system3 -When the consumption is finished, the microorganisms can also utilize organic matters released by the biochar to reduce Fe (III) into Fe (II), thereby realizing the redox cycle of iron-nitrogen.
(2) The strong carbon secretion type modified biochar used by the invention is prepared by dry distillation at low temperature, and the dissolution capacity of organic carbon is greatly higher than that of biochar prepared at high temperature (400 ℃). FIG. 1 is an organic carbon dissolution curve of Arundo donax biochar prepared by dry distillation at different temperatures, and it can be seen from the graph that organic carbon dissolution determination of the Arundo donax biochar prepared at a low temperature of 300 ℃ is carried out by deionized water according to a ratio of 1:20, the organic carbon concentration is as high as 135mg/L (2700mg/kg) which is nearly 3 times of the effluent concentration (50mg/L) of the first-class A standard COD of a sewage treatment plant, and therefore, the organic carbon plays an important role in enhanced denitrification of wastewater with a low carbon-nitrogen ratio. As the temperature rises, the dissolution amount of organic carbon in the biochar is greatly reduced, so that the high-temperature biochar has a very limited effect on releasing a carbon source and promoting denitrification.
(3) A great number of reports show that the biochar is in the soilCan relieve greenhouse gas N2O release, in the invention, the strong carbon-secreting type modified biochar is applied to the deep denitrification treatment of the sewage of the artificial wetland, not only plays a role in carbon fixation and emission reduction, but also can relieve the N content of the artificial wetland by promoting the denitrification process2And releasing the O.
The method provided by the invention has the advantages that the denitrification efficiency of the sewage with the low carbon-nitrogen ratio is improved by a simple method, meanwhile, a reference is provided for solving the problem of plant resource utilization in situ, the method is simple to operate and high in practicability, and the method has important significance for comprehensively realizing the quality improvement of total nitrogen in sewage discharge to reach the standard and relieving the global greenhouse effect.
Drawings
FIG. 1 is a graph of the concentration of biochar-dissolved organic carbon at different temperatures;
fig. 2 is a schematic structural view of a strong carbon-secreting modified biochar used in the present invention.
Fig. 3 is a schematic structural diagram of a horizontal subsurface wetland in the method for enhancing denitrification of the artificial wetland.
In the figure: 1. the wetland comprises a water inlet, 2 parts of a packed column, 3 parts of a strong carbon secretion type modified biochar substrate, 4 parts of a wetland main body substrate, 5 parts of a water outlet, 6 parts of wetland plants, 7 parts of a wetland bed body.
FIG. 4 is a bar chart of the effect of the addition of different strong carbon-secreting modified biochar on total nitrogen removal.
Detailed Description
The present invention is further illustrated by, but is not limited to, the following specific examples.
Example 1
A method for strengthening denitrification of an artificial wetland by using strong carbon-secreting modified biochar, which is used as a treating agent to strengthen denitrification of the artificial wetland, comprises the following steps:
filling the biochar into a filler column, and vertically embedding the filler column into an artificial wetland bed body, wherein the ratio of the total volume of the biochar to the volume of the wetland is 1: 6; the packed column is a perforated column, the aperture is 0.5-1 cm, and the aperture ratio is 40-80%. The filler column is round or square, the width of the filler column is the same as that of the wetland when the filler column is square, and the top of the filler column is provided with a detachable sealing plug for sealing the filler column or replacing the biochar filler in the invention. The covering area of the filler columns accounts for 1/20-2/3 of the surface area of the wetland. The horizontal subsurface flow wetland comprises a pool body 7, wetland plants 6, a wetland main body matrix 4, filler columns 2 and wetland strongly carbon-secreting modified biochar 3, which is specifically shown in figure 3. The wetland main body matrix filler is one or the combination of any more of gravel, building waste bricks and fly ash, and coarse sand or quartz sand of 15cm is paved on the top.
The specific working process of the vertical flow wetland comprises the following steps:
the continuous water inlet and water outlet mode is adopted for operation. After high nitrate nitrogen sewage uniformly enters a wetland bed body 7 through a water distribution pipeline, nitrate nitrogen in inlet water is contacted with a biochar packed column in the invention, on one hand, strong carbon-secreting biochar in the invention directly promotes denitrification of denitrifying microorganisms in the sewage by releasing an organic carbon source; on the other hand, the modified biochar in the invention transfers electrons to high-valence nitrogen (such as NO) by taking surface Fe (II) as an electron donor3 -，NO2 -) The nitrogen with high valence can be reduced into nitrogen while being oxidized, so that the chemical denitrification process is realized; meanwhile, denitrifying microorganisms respectively take ferrous iron and nitrate as electron donors and acceptors to oxidize the ferrous iron into ferric iron and reduce the nitrate simultaneously to remove NO3 -Conversion to N2. The treated water is discharged out of the wetland through a water outlet.
The strong carbon-secreting modified charcoal is prepared by the following method:
(1) cleaning and cutting the wet plant rhizoma arundinaceae of the wet plant into blocks with the diameter of 1-3 cm, and air-drying the blocks until the weight is constant.
(2) Carrying out rapid carbonization treatment on the wetland plants treated in the step (1) at low temperature in a dry distillation mode under the protection of nitrogen to obtain biochar; the dry distillation temperature is 300 ℃, the heating rate is 8 ℃/min, and the dry distillation time is 60 min;
(3) and load modification treatment: mixing the biochar prepared in the step (2) with 3mol/L ferrous chloride solution, standing for 12h for carrying ferrous, washing the carried biochar with deionized water to be neutral, and drying for 12h in an anaerobic environment at 105 ℃ to obtain the strong carbon-secreting type modified biochar, as shown in figure 2.
Example 2
The method for enhancing the denitrification of the constructed wetland by using the strong carbon-secreting modified biochar is the same as that in the embodiment 1, and is characterized in that:
the strong carbon-secreting type modified biochar and the matrix are mixed and filled into the artificial wetland bed body for enhanced denitrification, the volume ratio of the strong carbon-secreting type modified biochar to the matrix is 1:3, and the coverage area of the mixed filler accounts for 1/3-2/3 of the total area of the wetland. The other structures are the same as the embodiment 2, and the sewage flows out of the pool body from the water outlet after being subjected to deep denitrification and denitrification purification by the wetland.
Application Experimental example
Firstly, the application experiments of the method for enhancing the denitrification of the artificial wetland by using the strong carbon-secreting modified biochar in the embodiment 1 and the embodiment 2 are respectively carried out, the high-nitrate-nitrogen sewage simulation wastewater enters the vertical-flow wetland in the embodiment 1 and the embodiment 2 through a water distribution pipeline, the total nitrogen content of inlet water is 25mg/L, the pH value of inlet water is 7, the inlet water load is 10L/h, denitrification treatment is carried out at the ambient temperature of 8-10 ℃, each treatment is carried out in parallel, and compared with the treatment without biochar, under the condition of HRT (hydraulic retention time) 5 days, the total nitrogen removal rate can reach 88%, the total nitrogen content of outlet water is less than 8mg/L, and the influence of the addition amount of different strong carbon-secreting modified biochar on the total nitrogen removal effect is shown in figure 4. As can be seen from FIG. 4, the addition amount of the strong carbon-secreting modified biochar is about 30% and the treatment effect is the strongest.
Claims (10)
1. A method for strengthening constructed wetland denitrification by using strong carbon-secreting modified biochar comprises the steps of using the strong carbon-secreting modified biochar as a treating agent to strengthen the constructed wetland for denitrification, mixing the strong carbon-secreting modified biochar with a matrix and filling the mixture into a constructed wetland bed body, or directly using the mixture as a filler column to be embedded into the constructed wetland bed body for denitrification, wherein the denitrification treatment temperature is 0-40 ℃, the pH value is 6-8, and the total nitrogen content of constructed wetland sewage is 5-60 mg/L;
the strong carbon-secreting modified charcoal is prepared by the following method:
(1) cleaning wetland plants serving as raw materials, crushing the wetland plants into blocks with the diameter of 1-3 cm, and air-drying the blocks to constant weight;
(2) carrying out rapid carbonization treatment on the wetland plants treated in the step (1) at a low temperature in a dry distillation mode under the protection of inert gas to obtain biochar; the dry distillation temperature is 250-400 ℃, the heating rate is 5-10 ℃/min, and the dry distillation time is 30-60 min;
(3) and load modification treatment: and (3) mixing the biochar prepared in the step (2) with 0.5-3 mol/L ferrous chloride solution, standing for 12-16 h for carrying ferrous, washing the carried biochar with deionized water to be neutral, and drying in an anaerobic environment at 100-120 ℃ for 6-12 h to obtain the strong carbon-secreting modified biochar.
2. The method for enhancing denitrification of the artificial wetland by using the strong carbon-secreting modified biochar as claimed in claim 1, wherein the denitrification treatment temperature is 10-30 ℃, the pH value is 6-7, and the total nitrogen content of the sewage of the artificial wetland is 20-40 mg/L.
3. The method for enhancing denitrification of the constructed wetland by using strong carbon-secreting modified biochar according to claim 1, wherein the volume ratio of the mixture of the strong carbon-secreting modified biochar and the matrix is 1: 10-1: 3.
4. The method for enhancing denitrification of the constructed wetland by using the strong carbon-secreting modified biochar as claimed in claim 1, wherein the matrix is one or a mixture of more than two of gravel, building waste bricks or quartz sand.
5. The method for enhancing denitrification of the artificial wetland by using the strong carbon-secreting modified biochar as claimed in claim 1, wherein the total coverage area of the strong carbon-secreting modified biochar mixed with the substrate accounts for 1/3-2/3 of the total area of the wetland, and the porosity of the strong carbon-secreting modified biochar mixed with the substrate is 20-50%.
6. The method for enhancing denitrification of the artificial wetland by using the strong carbon-secreting modified biochar as claimed in claim 1, wherein the biochar is directly used as a filler column, the biochar is filled into the filler column, then the filler column is vertically embedded into an artificial wetland bed body, and the ratio of the total volume of the biochar to the volume of the wetland is 1: 20-1: 4; the filler column is a perforated column, the aperture is 0.5-1 cm, and the aperture ratio is 40% -80%.
7. The method for enhancing denitrification of the artificial wetland by using the strong carbon-secreting modified biochar as claimed in claim 1, wherein the covering area of the filler columns accounts for 1/20-2/3 of the surface area of the wetland.
8. The method for enhancing the denitrification of the artificial wetland by using the strong carbon-secreting modified biochar as claimed in claim 1, wherein the root or stem of the wetland plant is selected as the raw material in the step (1).
9. The method for enhancing the denitrification of the artificial wetland by using the strong carbon-secreting modified biochar as claimed in claim 1, wherein the inert gas in the step (2) is nitrogen; the dry distillation temperature is 250-300 ℃, the heating rate is 5-8 ℃/min, and the dry distillation time is 40-60 min.
10. The method for enhancing denitrification of the constructed wetland by using the strong carbon-secreting modified biochar as claimed in claim 1, wherein the concentration of the ferrous chloride solution in the step (3) is 1-3 mol/L, the load time of the step (3) is 12 hours, the anaerobic drying temperature of the step (3) is 100-110 ℃, and the drying time is 8-12 hours.
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| CN107824612B (en) * | 2017-11-04 | 2018-09-28 | 江西夏氏春秋环境股份有限公司 | A kind of Fe3O4The preparation method of base charcoal soil passivator |
| CN108101222B (en) * | 2017-12-29 | 2020-07-31 | 华南农业大学 | Artificial wetland for deep nitrogen and phosphorus removal of tail water and tail water treatment method thereof |
| CN111943359B (en) * | 2020-07-24 | 2022-06-03 | 山东大学 | Artificial wetland coupled with iron ore enhanced denitrification, operation method and application |
| CN114409089A (en) * | 2022-01-21 | 2022-04-29 | 北京林业大学 | Subsurface flow constructed wetland river water treatment method based on carbon-supplementing columns |
| CN114940564B (en) * | 2022-05-31 | 2023-12-22 | 太原理工大学 | Method for controlling release of nitrogen in bottom mud of landscape water body by coupling iron-type autotrophic denitrification with biochar |
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| US6569321B2 (en) * | 1999-04-16 | 2003-05-27 | Larry Steven Coffman | Method and apparatus for treating stormwater runoff |
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