CN112978925A - Sulfur-iron synergistic polyculture denitrification enhanced low C/N sewage denitrification method and reactor - Google Patents
Sulfur-iron synergistic polyculture denitrification enhanced low C/N sewage denitrification method and reactor Download PDFInfo
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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
- C02F3/30—Aerobic and anaerobic processes
- C02F3/302—Nitrification and denitrification treatment
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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
- C02F3/345—Biological treatment of water, waste water, or sewage characterised by the microorganisms used for biological oxidation or reduction of sulfur compounds
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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
- C02F3/346—Iron bacteria
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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
- C02F2101/00—Nature of the contaminant
- C02F2101/10—Inorganic compounds
- C02F2101/16—Nitrogen compounds, e.g. ammonia
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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
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/38—Organic compounds containing nitrogen
Abstract
The invention discloses a method and a reactor for enhancing denitrification of low C/N sewage and wastewater by sulfur-iron synergistic polyculture denitrification. The method of the invention comprises the following steps: the low C/N sewage and the return nitrifying liquid of the aerobic pool are treated in an anoxic pool filled with iron shaving-magnetite composite filler and activated sludge floc to generate S under the action of denitrifying bacteria2O3 2‑、Fe0、Fe2+Autotrophic denitrification and heterotrophic denitrification processes; then the sewage enters an aerobic tank filled with activated sludge flocs to carry out a nitrification process, residual organic matters in the sewage are further decomposed, and part of nitrified liquid flows back to an anoxic tank; finally enters a central pipe of a vertical sedimentation tank, is discharged after sedimentationPart of the precipitated sludge flows back to the anoxic tank, and part of the precipitated sludge is discharged as residual sludge. The invention can reduce the requirement of AO technology on the carbon-nitrogen ratio of the influent water, does not need additional organic carbon source, has low operation cost and high denitrification efficiency, and can effectively reduce the sludge yield and the risk of secondary pollution of effluent water.
Description
Technical Field
The invention relates to a sulfur-iron synergistic polyculture denitrification enhanced low C/N sewage denitrification method and a reactor, belonging to the technical field of sewage treatment.
Background
Biological denitrification is an important measure for reducing the nitrogen discharge of sewage and wastewater and eliminating the eutrophication of a receiving water body, the traditional anoxic and aerobic combined (AO) process for denitrification by utilizing the biological action of nitrification and denitrification is a commonly adopted denitrification process of a sewage and wastewater treatment plant, and sufficient carbon sources are the precondition for ensuring the denitrification by the AO process. For sewage with low C/N, the AO process cannot reach higher denitrification efficiency of heterotrophic denitrification due to the shortage of organic carbon source, and carbon source (such asGlucose, methanol, sodium acetate, etc.) can increase the cost of sewage treatment, and improper dosage control can also cause secondary pollution risk of higher organic matters in the effluent. In contrast to heterotrophic denitrification, sulfur and iron autotrophic bacteria-mediated autotrophic denitrification may utilize lower-valent sulfur (S)0、S2-、S2O3 2-Etc.) and low valence iron (Fe)0、Fe2+) Etc. inorganic substances as electron donors, with NO3 -Reduction of-N to N2When the method is used for denitrification of low C/N sewage, no additional organic carbon source is needed, and the method has the advantages of low operation cost, high denitrification efficiency and low sludge yield, and becomes the mainstream research direction for efficient denitrification of low C/N sewage. The efficiency of the single sulfur autotrophic denitrification is higher, and the method is based on S2O3 2-The autotrophic denitrification not only can realize the liquid addition of the sulfur electron donor, but also can avoid solid S0Inconvenience of use of (hazardous articles) and S2-Is liable to generate H2S, but acid generated in the reaction process easily causes the pH of the effluent to be acidic. Based on Fe0/Fe2+The iron autotrophic denitrification can also realize higher denitrification efficiency, but alkali is generated in the treatment process, and ferric iron compounds are easily formed and attached to and coated on the sludge, so that the reaction efficiency is reduced. By combining the characteristics of the sulfur and iron autotrophic denitrification reaction, the defect of single use can be avoided by the combined mixed culture denitrification of sulfur and iron, acid and alkali neutralization in the reaction process is realized, and the reaction efficiency is promoted to be improved.
Disclosure of Invention
The technical problem to be solved by the invention is as follows: the problem of how to realize low-cost and high-efficiency denitrification on the sewage and the wastewater with low C/N.
In order to solve the technical problem, the invention provides a sulfur-iron synergetic polyculture denitrification enhanced low C/N sewage denitrification method, which comprises the following steps:
step 1): continuously adding a sulfur source electron donor into the low C/N sewage as inlet water, feeding the inlet water and a nitrifying liquid returned from an aerobic tank into an anoxic tank with an iron shaving-magnetite composite filler for treatment, performing a sulfur and iron synergetic autotrophic denitrification process under the action of autotrophic denitrifying bacteria, and simultaneously performing a heterotrophic denitrification process by using organic matters contained in the low C/N sewage as a heterotrophic denitrification carbon source;
the autotrophic denitrification process comprises the following steps:
S2O3 2-autotrophic denitrification: s2O3 2-+1.24NO3-+0.45HCO3 -+0.09NH4 ++0.11H2O→0.09C5H7O2N+0.4H++0.62N2+2SO4 2-；
Fe0Autotrophic denitrification: fe0+0.4NO3 -+1.2H2O→Fe2++0.2N2+2.4OH-；
Fe2+Autotrophic denitrification: fe2++0.2NO3 -+2.4H2O→Fe(OH)3+0.1N2+1.8H+；；
The heterotrophic denitrification process has the following chemical reactions:
CH3COO-+1.18NO3 -+2.18H+→0.12C5H7O2N+1.4CO2+2.5H2O+0.53N2。
step 2): treating the effluent treated in the step 1) in an aerobic tank, and performing a nitrification process under the action of aerobic bacteria in the activated sludge floc to further decompose residual organic matters in the sewage;
the nitration process takes place by the following chemical reactions:
NH4 ++2O2→NO3 -+2H++H2O；
step 3): returning a part of the nitrifying liquid obtained after the treatment in the step 2) to the anoxic tank, allowing the other part of the nitrifying liquid to enter a vertical sedimentation tank for sedimentation, and discharging waste water obtained after sedimentation through a water outlet pipe; and returning one part of the sludge obtained after precipitation to the anoxic tank, and discharging the other part of the sludge as residual sludge.
Preferably, the COD/TN in the low C/N sewage and wastewater in the step 1) is 2-2.5; the iron shaving-magnetThe mineral composite filler includes providing Fe0Iron shaving of iron source electron donor and provision of Fe2+Fe of iron source electron donor3O4Magnetite; said Fe0And Fe3O4The mass ratio of (A) to (B) is 4: 1.
preferably, the sulfur source electron donor in the step 1) is sodium thiosulfate; the S/N molar ratio in the inlet water is 0.8-1.0.
Preferably, the dissolved oxygen of the anoxic tank in the step 1) is controlled to be below 0.5mg/L, and the hydraulic retention time is controlled to be 1.5-2.5 h; in the step 2), the dissolved oxygen of the aerobic pool is controlled to be 2.0-4.0 mg/L, and the hydraulic retention time is controlled to be 5.0-10.0 h.
Preferably, the reflux ratio of the nitrifying liquid in the step 3) is controlled to be 150-250%; the reflux ratio of the sludge is controlled to be 50-100%.
The invention also provides a sulfur-iron synergetic polyculture denitrification enhanced low C/N sewage denitrification reactor, which comprises:
the anaerobic tank (4) is provided with an iron shaving-magnetite composite filler (25) and an activated sludge floc I (5), one side of the anaerobic tank (4) is provided with a sewage and wastewater inlet pipe (1), the other side is provided with an anaerobic tank outlet pipe (7), and the sewage and wastewater inlet pipe (1) is connected with a sulfur source feeding pipe (23);
the aerobic tank (9) is provided with an activated sludge floc II (10), one side of the aerobic tank (9) is connected with the anoxic tank water outlet pipe (7), the other side of the aerobic tank is provided with a nitrifying liquid water outlet pipe (12), the nitrifying liquid water outlet pipe (12) is connected with a nitrifying liquid return pipe (20), and the nitrifying liquid return pipe (20) is communicated with the sewage and wastewater water inlet pipe (1);
the device comprises a vertical flow type sedimentation tank (13) provided with a central pipe (16), wherein one side of the vertical flow type sedimentation tank (13) is communicated with a nitrifying liquid outlet pipe (12) and the central pipe (16) respectively, the other side of the vertical flow type sedimentation tank is provided with a sedimentation tank outlet pipe (15), a sludge discharge pipe (17) is arranged at the bottom of the vertical flow type sedimentation tank (13), the sludge discharge pipe (17) is connected with a sludge discharge pipe (18) and a sludge return pipe (21) respectively, and the sludge return pipe (21) is communicated with a sewage and wastewater inlet pipe (1).
Preferably, the gouge-magnetite composite filler (25) is made of polyethyleneThe weight of each bag is 5-7.5 kg, and the filling density is 20-30 kg/m3(ii) a One or more stainless steel filler frames (3) are arranged in the anoxic tank (4), and stainless steel partition plates (24) used for placing iron shavings-magnetite composite fillers (25) are arranged in the filler frames (3).
Preferably, the bottom in oxygen deficiency pond (4) is equipped with electric agitator (22), dirty waste water inlet tube (1) one side in oxygen deficiency pond (4) is equipped with water distribution channel (2), oxygen deficiency pond outlet pipe (7) one side in oxygen deficiency pond (4) is equipped with water collection channel (6).
Preferably, the bottom of the aerobic tank (9) is provided with a microporous aeration disc (19); one side of the aerobic tank (9) connected with the water outlet pipe (7) of the anoxic tank is provided with a water distribution channel II (8), and one side of the nitrifying liquid water outlet pipe (12) of the aerobic tank (9) is provided with a water collecting channel II (11).
Preferably, one side of a sedimentation tank water outlet pipe (15) of the vertical flow type sedimentation tank (13) is provided with a third water collecting channel (14).
The principle of the invention is as follows: in a reactor for enhancing the denitrification of the low C/N sewage and wastewater by the synergistic mixed culture of sulfur and iron and denitrification, microorganisms in an aerobic tank are utilized to nitrify and Fe in an anoxic tank0、Fe2+And S2O3 2-The autotrophic denitrification and the heterotrophic denitrification cooperate to achieve the aim of denitrification without an additional carbon source.
Compared with the prior art, the invention has the beneficial effects that:
1. the application range of the denitrification method is low C/N sewage denitrification, and the effluent TN can stably reach the discharge standard of pollutants (first grade A) of urban sewage treatment plants (TN is less than or equal to 15.0mg/L) by the sulfur-iron synergistic polyculture denitrification enhanced low C/N sewage denitrification method and the reactor;
2. compared with the traditional AO process, the sulfur-iron synergetic polyculture denitrification enhanced low C/N sewage denitrification reactor provided by the invention can reduce the requirement on the carbon-nitrogen ratio of inlet water, realize denitrification without an external carbon source, has simple operation, low operation cost and easy engineering realization, can realize acid-base complementation in an anoxic tank, and effectively reduce the sludge yield and the risk of secondary effluent pollution while enhancing the denitrification efficiency of the system.
Drawings
FIG. 1 is a schematic view of a reactor for enhancing denitrification of wastewater with low C/N content by sulfur and iron co-culture denitrification provided by the invention;
FIG. 2 is a schematic view of a stuffing frame of the present invention;
reference numerals: 1. a sewage and wastewater inlet pipe; 2. a first water distribution channel; 3. a packing frame; 4. an anoxic tank; 5. activated sludge floc I; 6. a first water collecting channel; 7. a water outlet pipe of the anoxic tank; 8. a water distribution channel II; 9. an aerobic tank; 10. activated sludge floc II; 11. a second water collecting channel; 12. a water outlet pipe of the aerobic tank; 13. a vertical flow sedimentation tank; 14. a third water collecting channel; 15. a water outlet pipe of the sedimentation tank; 16. a central tube; 17. a sludge discharge pipe; 18. a sludge discharge pipe; 19. a microporous aeration disc; 20. a nitrifying liquid return pipe; 21. a sludge return pipe; 22. an electric stirrer; 23. a sulfur source feeding pipe; 24. a stainless steel separator; 25. iron shaving-magnetite composite filler.
Detailed Description
In order to make the invention more comprehensible, preferred embodiments are described in detail below with reference to the accompanying drawings.
Examples
The raw water in this example was simulated low C/N wastewater with Chemical Oxygen Demand (COD), Total Nitrogen (TN), and ammonia Nitrogen (NH)4 +-N), nitrate Nitrogen (NO)3 --N), nitrite Nitrogen (NO)2 --N) are respectively 100 +/-5 mg/L, 41 +/-5 mg/L, 40 +/-5 mg/L, 1.02 +/-0.2 mg/L and 0.09 +/-0.02 mg/L, and nitrogen in the wastewater is in the form of NH4 +-N is dominant.
Mixing the low C/N sewage and nitrifying liquid returned by the aerobic tank, feeding the mixture into an anoxic tank filled with iron shaving-magnetite composite filler and activated sludge flocs, controlling the molar ratio of water inlet S/N to be 0.8-1.0 by taking sodium thiosulfate as an additional sulfur source electron donor, and simultaneously performing heterotrophic denitrification and Fe denitrification under the action of denitrifying bacteria0-Fe2+Autotrophic denitrification and S2O3 2-An autotrophic denitrification process; the effluent enters an aerobic tank filled with activated sludge flocs, an ammonia nitrogen nitration process is carried out under the action of aerobic bacteria, and furtherDecomposing the residual organic matters, and refluxing the nitrified liquid to the front-end anoxic tank; and after the reaction is finished, the sludge-water mixed liquid enters a central pipe of the vertical sedimentation tank, the wastewater is discharged after sedimentation, part of the precipitated sludge flows back to the water inlet pipe, and enters the anoxic tank after being mixed with the low C/N sewage to supplement the lost sludge, and part of the precipitated sludge is discharged as residual sludge. After treatment, COD in the wastewater is lower than 50.0mg/L, TN is lower than 10.0mg/L, and TN of the effluent reaches the pollutant discharge standard (first-class A) of urban sewage treatment plants (TN is less than or equal to 15.0 mg/L).
The denitrification method for the low C/N sewage adopts a sulfur-iron synergetic polyculture denitrification enhanced low C/N sewage denitrification reactor as shown in figure 1, which comprises an anoxic tank 4 provided with iron shaving-magnetite composite filler 25 and an activated sludge floc I5, an aerobic tank 9 provided with an activated sludge floc II 10 and a vertical sedimentation tank 13 provided with a central pipe 16, wherein a plurality of groups of stainless steel filler frames 3 are arranged in the anoxic tank 4, the specific structure of the filler frames 3 is shown in figure 2, the iron shaving-magnetite composite filler 25 wrapped by polyethylene mesh bags is stacked on a stainless steel partition plate 24 of each filler frame, a water distribution channel I2 is arranged at the water inlet side of the anoxic tank 4, a sewage inlet pipe 1 is connected with the water distribution channel I2 and a sulfur source feeding pipe 23, an electric stirrer 22 is arranged at the bottom of the anoxic tank 4, a water collection channel I6 is arranged at the water outlet side of the anoxic tank 4, the water collecting channel I6 is connected with a water outlet pipe 7 of the anoxic pond; an outlet pipe 7 of the anoxic tank is connected with an aerobic tank 9, a water distribution channel II 8 is arranged on the water inlet side of the aerobic tank 9, the outlet pipe 7 of the anoxic tank is connected with the water distribution channel II 8, a microporous aeration disc 19 is arranged at the bottom of the aerobic tank 9, a water collection channel II 11 is arranged on the water outlet side of the aerobic tank 9, the water collection channel II 11 is connected with an outlet pipe 12 of the aerobic tank, a nitrifying liquid return pipe 20 is connected with the outlet pipe 12 of the aerobic tank, and nitrifying liquid returns through the nitrifying liquid return pipe 20 to be mixed with low C/N sewage and wastewater in the sewage and wastewater; the water outlet pipe 12 of the aerobic tank is connected with the central pipe 16 of the vertical flow sedimentation tank 13, the waste water after sedimentation is discharged through the water outlet pipe 15 of the sedimentation tank, the sludge discharge pipe 17 arranged at the bottom of the sedimentation tank is connected with the sludge return pipe 21 and the sludge discharge pipe 18, the returned sludge returns through the sludge return pipe 21 and is mixed with the low C/N sewage and waste water in the water inlet pipe 1 and then enters the anoxic tank 4, the residual sludge is discharged through the sludge discharge pipe 18, the water outlet side of the vertical flow sedimentation tank 13 is provided with a water collecting channel III 14, and the water collecting channel III 14 is connected with the water outlet pipe 15 of.
The above-described embodiments are only preferred embodiments of the present invention, and are not intended to limit the present invention in any way and substantially, it should be noted that those skilled in the art may make several modifications and additions without departing from the scope of the present invention, which should also be construed as a protection scope of the present invention.
Claims (10)
1. A sulfur-iron synergetic polyculture denitrification enhanced low C/N sewage denitrification method is characterized by comprising the following steps:
step 1): continuously adding a sulfur source electron donor into the low C/N sewage as inlet water, feeding the inlet water and a nitrifying liquid returned from an aerobic tank into an anoxic tank with an iron shaving-magnetite composite filler for treatment, performing a sulfur and iron synergetic autotrophic denitrification process under the action of autotrophic denitrifying bacteria, and simultaneously performing a heterotrophic denitrification process by using organic matters contained in the low C/N sewage as a heterotrophic denitrification carbon source;
step 2): treating the effluent treated in the step 1) in an aerobic tank, and performing a nitrification process under the action of aerobic bacteria in the activated sludge floc to further decompose residual organic matters in the sewage;
step 3): returning a part of the nitrifying liquid obtained after the treatment in the step 2) to the anoxic tank, allowing the other part of the nitrifying liquid to enter a vertical sedimentation tank for sedimentation, and discharging waste water obtained after sedimentation through a water outlet pipe; and returning one part of the sludge obtained after precipitation to the anoxic tank, and discharging the other part of the sludge as residual sludge.
2. The method for enhancing denitrification of low C/N sewage and wastewater by sulfur-iron synergetic polyculture denitrification according to claim 1, wherein COD/TN in the low C/N sewage and wastewater in the step 1) is 2-2.5; the iron shaving-magnetite composite filler comprises Fe0Iron shaving of iron source electron donor and provision of Fe2+Fe of iron source electron donor3O4Magnetite; said Fe0And Fe3O4The mass ratio of (A) to (B) is 4: 1.
3. the method for enhancing the denitrification of the low C/N sewage by the sulfur-iron co-culture denitrification as claimed in claim 1, wherein the sulfur source electron donor in the step 1) is sodium thiosulfate; the S/N molar ratio in the inlet water is 0.8-1.0.
4. The method for enhancing the denitrification of the low-C/N sewage and wastewater by the sulfur-iron synergetic polyculture denitrification as claimed in claim 1, wherein the dissolved oxygen in the anoxic pond in the step 1) is controlled to be below 0.5mg/L, and the hydraulic retention time is controlled to be 1.5-2.5 h; in the step 2), the dissolved oxygen of the aerobic pool is controlled to be 2.0-4.0 mg/L, and the hydraulic retention time is controlled to be 5.0-10.0 h.
5. The method for enhancing the denitrification of the low-C/N sewage and wastewater by the sulfur-iron synergetic polyculture denitrification according to claim 1, wherein the reflux ratio of the nitrifying liquid in the step 3) is controlled to be 150-250%; the reflux ratio of the sludge is controlled to be 50-100%.
6. A sulfur-iron synergetic polyculture denitrification enhanced low C/N sewage denitrification reactor is characterized by comprising:
the device comprises an anoxic tank (4) provided with an iron shaving-magnetite composite filler (25) and an activated sludge floc I (5), wherein one side of the anoxic tank (4) is provided with a sewage and wastewater inlet pipe (1), the other side of the anoxic tank is provided with an anoxic tank outlet pipe (7), and the sewage and wastewater inlet pipe (1) is connected with a sulfur source electron donor feeding pipe (23);
the aerobic tank (9) is provided with an activated sludge floc II (10), one side of the aerobic tank (9) is connected with the anoxic tank water outlet pipe (7), the other side of the aerobic tank is provided with a nitrifying liquid water outlet pipe (12), the nitrifying liquid water outlet pipe (12) is connected with a nitrifying liquid return pipe (20), and the nitrifying liquid return pipe (20) is communicated with the sewage and wastewater water inlet pipe (1);
the device comprises a vertical flow type sedimentation tank (13) provided with a central pipe (16), wherein one side of the vertical flow type sedimentation tank (13) is communicated with a nitrifying liquid outlet pipe (12) and the central pipe (16) respectively, the other side of the vertical flow type sedimentation tank is provided with a sedimentation tank outlet pipe (15), a sludge discharge pipe (17) is arranged at the bottom of the vertical flow type sedimentation tank (13), the sludge discharge pipe (17) is connected with a sludge discharge pipe (18) and a sludge return pipe (21) respectively, and the sludge return pipe (21) is communicated with a sewage and wastewater inlet pipe (1).
7. The reactor for denitrification of wastewater with low C/N content reinforced by synergistic mixotrophy of pyrite and pyrite as claimed in claim 6, wherein said iron shaving-magnetite composite filler (25) is wrapped by polyethylene mesh bags, each bag weighs 5-7.5 kg, and the packing density is 20-30 kg/m3(ii) a One or more stainless steel filler frames (3) are arranged in the anoxic tank (4), and stainless steel partition plates (24) used for placing iron shavings-magnetite composite fillers (25) are arranged in the filler frames (3).
8. The reactor for enhancing denitrification of sewage and wastewater with low C/N content according to claim 6, wherein the bottom of the anoxic tank (4) is provided with an electric stirrer (22), one side of the sewage and wastewater inlet pipe (1) of the anoxic tank (4) is provided with a water distribution channel I (2), and one side of the anoxic tank outlet pipe (7) of the anoxic tank (4) is provided with a water collection channel I (6).
9. The reactor for enhancing denitrification of sewage containing low C/N content according to claim 6, wherein the bottom of the aerobic tank (9) is provided with a microporous aeration disc (19); one side of the aerobic tank (9) connected with the water outlet pipe (7) of the anoxic tank is provided with a water distribution channel II (8), and one side of the nitrifying liquid water outlet pipe (12) of the aerobic tank (9) is provided with a water collecting channel II (11).
10. The reactor for enhancing denitrification of wastewater with low C/N content by sulfur and iron co-culture denitrification as claimed in claim 6, wherein a third water collecting channel (14) is arranged on one side of a water outlet pipe (15) of the sedimentation tank of the vertical sedimentation tank (13).
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| CN113716689A (en) * | 2021-08-11 | 2021-11-30 | 中国长江三峡集团有限公司 | Mixed nutrition type denitrification method based on sulfur reduction and sulfur autotrophic denitrification |
| CN113912184A (en) * | 2021-10-22 | 2022-01-11 | 广州市香港科大霍英东研究院 | Method for improving sewage treatment effect of low CN ratio |
| CN114409082A (en) * | 2022-02-08 | 2022-04-29 | 东华大学 | High-ammonia-nitrogen and low-carbon-nitrogen-ratio sewage wastewater OAO coupling zero-valent iron nitrogen and phosphorus removal method |
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