CN112607847A - Sewage nitrogen and phosphorus removal treatment method, device and application - Google Patents
Sewage nitrogen and phosphorus removal treatment method, device and application Download PDFInfo
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Abstract
The invention discloses a sewage denitrification and dephosphorization treatment method, a sewage denitrification and dephosphorization treatment device and application.A reaction tank comprises a cathode chamber and an anode chamber, wherein the anode is made of iron or aluminum, and two ends of the anode and the cathode are externally connected with a direct current power supply through leads; the cathode chamber and the anode chamber are separated by a proton exchange membrane; the cathode chamber is internally provided with a filter tank, sulfur particles are filled in the filter tank, the side wall of the filter tank is provided with a porous insulating material layer, and the cathode is arranged outside the filter tank. The integrated coupling sulfur autotrophic denitrification and ferric salt or aluminum salt flocculation precipitation dephosphorization tie is realized by using a bioelectrochemical system, and iron or aluminum is used as an anode of an electrolytic cell, so that the iron or aluminum can be separated out in an electrochemical reactor in an ion form in situ and further subjected to a precipitation reaction with phosphate, and the electrochemical coagulation precipitation dephosphorization has remarkable advantages in the aspects of operation cost, operation management and the like; the cathode can consume acidity generated in the process of sulfur autotrophic denitrification, and additional alkalinity is avoided. The invention integrates two functions of denitrification and dephosphorization into one system, is simpler and can realize the deep denitrification and dephosphorization of sewage.
Description
Technical Field
The invention relates to the field of sewage treatment, in particular to a method and a device for nitrogen and phosphorus removal treatment of sewage by coupling sulfur autotrophic denitrification and micro-electric field iron oxidation and application.
Background
Eutrophication of water body is a global environmental pollution problem, which causes algae outbreak and water quality deterioration, seriously damages the stability of water body ecological system and affects the safety of urban water supply and drinking water. The discharge of nitrogen and phosphorus nutrient elements is the root cause of water eutrophication. In order to improve the water environment quality of the receiving water body, advanced treatment of nitrogen and phosphorus needs to be improved in a municipal sewage treatment plant.
At present, the denitrification mainly comprises a physical treatment technology, a chemical treatment technology and a biological treatment technology. The biological treatment technology is a process of finally reducing nitrate in water into nitrogen by using microorganisms. The biological treatment technology has the characteristics of high efficiency and low energy consumption. According to the difference of electron donors, the biological treatment technology can be divided into heterotrophic denitrification and autotrophic denitrification, wherein the autotrophic denitrification mainly refers to denitrification by relying on inorganic matters (such as hydrogen and sulfur) as the electron donors and inorganic carbon compounds (such as CO2 and HCO3-) as carbon sources for microbial metabolism. In contrast, the sulfur autotrophic denitrification process is a research hotspot because of high denitrification efficiency, low sulfur price, easily available raw materials, stable working condition operation and low sludge yield, and is safer and more convenient in transportation, use and the like.
The elemental sulfur autotrophic denitrification can efficiently treat low-concentration nitrate sewage without adding an organic carbon source, not only can reduce the cost, but also can reduce the operation risk, and compared with the heterotrophic denitrification, the sulfur autotrophic denitrification sludge has less yield and reduces the subsequent sludge treatment cost. However, in the process of autotrophic denitrification of sulfur to produce acid, it is theorized that 4.57mg CaCO is consumed to remove 1mg/L nitrate nitrogen3Alkalinity, alkali is added. In contrast, the sulfur autotrophic denitrification process is safer and more convenient in transportation and use due to high denitrification efficiency, low sulfur price, easily available raw materials, stable working condition operation and low sludge yieldAnd became a hot spot of research. In addition, the sulfate removal function of the sulfur autotrophic denitrification process is not phosphate removal, and the synchronous standard of nitrogen and phosphorus can not be reached. Therefore, a synchronous phosphorus removal mode can be adopted to enhance the phosphorus removal effect of the sulfur autotrophic denitrification process.
At present, the method for removing phosphorus from sewage mainly comprises a biological method and a chemical method. Biological methods are widely used because of their advantages of being economical, effective, environmentally friendly, and the like. But also has the problems of long reaction time, large occupied area of equipment, difficult sludge treatment, complex dephosphorization process, poor effluent stability and the like. The chemical phosphorus removal method has the advantages of economy, high efficiency, simple and convenient operation, reliable effect, difficult influence of the quality of wastewater and the like, so the chemical phosphorus removal method is popularized and applied, but most of phosphorus removal materials (agents) are industrial products such as lime, aluminum salt, ferric salt, ferrous salt, magnesium salt and the like, the phosphorus removal agents have higher cost and larger sludge amount, and the bottleneck of the method in practical application is caused. To date, chemical phosphorus removal has remained the primary process for phosphorus removal. Chemical phosphorus removal is mainly realized by adding a chemical agent into wastewater to form insoluble phosphate precipitate, and then removing phosphorus from the wastewater through solid-liquid separation. Research on phosphorus removal by adopting an electrochemical method alone is mature, and good phosphorus removal effect can be achieved by taking Fe and Al as the anode of the electrolytic cell (Chemical Engineering journal.172(2011) 137-143). The use of elemental sulfur autotrophic denitrification for nitrate removal from Water is also well established (Water Research,2014,60: 210-. At present, for the sewage treatment plants in China to meet the requirement of deep removal of phosphorus, a flocculation precipitation technical means is mostly adopted, and iron salt or aluminum salt and phosphate radical are added to form insoluble precipitate so as to remove the insoluble precipitate from water. However, in practical application, the dosage of the iron salt or the aluminum salt is difficult to control accurately, and the operation cost is high.
Disclosure of Invention
In order to solve the problems in the prior art, the invention provides a sewage nitrogen and phosphorus removal treatment device, a sewage nitrogen and phosphorus removal treatment method and an application thereof.A bioelectrochemical system is used as a tie for integrating and coupling sulfur autotrophic denitrification and ferric salt or aluminum salt flocculation precipitation phosphorus removal, iron or aluminum is used as an anode of an electrolytic cell, and can be in-situ separated out into an ion form in an electrochemical reactor so as to generate a precipitation reaction with phosphate; the cathode can consume acidity generated in the process of sulfur autotrophic denitrification, and additional alkalinity is avoided. The invention integrates two functions of denitrification and dephosphorization into one system, is simpler and can realize the deep denitrification and dephosphorization of sewage.
The invention is realized by the following technical scheme:
on one hand, the invention provides a sewage denitrification and dephosphorization treatment method, denitrification and dephosphorization reactions are respectively realized in a cathode chamber and an anode chamber of a double-chamber bioelectrochemical reaction tank, a proton exchange membrane is arranged between the cathode chamber and the anode chamber, an iron or aluminum material is used as an anode electrode, a carbon-based material or a metal-based material is used as a cathode electrode, and a direct current power supply is utilized to provide external voltage at the two ends of the cathode and the anode; elemental sulfur particles are used as filler and are placed in an insulating porous material filter tank of a cathode chamber, and a cathode electrode is arranged outside the filter tank; firstly, sewage containing nitrate and phosphate enters a cathode chamber through a water inlet pump, and nitrate is removed through sulfur autotrophic denitrification and cathode denitrification; pumping the effluent from the cathode chamber into the anode chamber through circulation, and removing phosphate radicals and metal ions generated by anode iron or aluminum sacrifice through precipitation reaction or adsorption by formed iron or aluminum hydroxide; and controlling the hydraulic retention time to finish the treatment of the nitrogen and the phosphorus in the sewage.
Preferably, the carbon-based material comprises carbon paper, carbon cloth, carbon felt, graphite plate and modified modification materials thereof; the metal-based material comprises stainless steel, iron, aluminum, copper, zinc, nickel or titanium metal material; the elemental sulfur particles and the biomembrane with the denitrification function are domesticated and enriched on the cathode electrode.
Furthermore, the sewage denitrification and dephosphorization treatment method specifically comprises the following steps:
step a: filling water into the cathode chamber and the anode chamber, and connecting the anode and the cathode with the anode and the cathode of an external power supply for electrifying; meanwhile, a water inlet pump and a circulating pump are started, the flow rates of the water inlet pump and the circulating pump are the same, and the liquid level of the cathode chamber is kept balanced; introducing sewage containing nitrate and phosphate into a cathode chamber, wherein sulfur autotrophic denitrifying bacteria in the biomembrane on the surface of the elemental sulfur particles use sulfur as an electron donor, active bacteria attached to the biomembrane on the surface of the cathode use the cathode as the electron donor, nitrate in the sewage is reduced into nitrogen to be removed, and the generated nitrogen is discharged from an exhaust port; the nitrogen-free wastewater after denitrification is discharged into the anode chamber by a circulating pump;
in the cathode chamber, with the increase of the operation period, the proliferation and the updating of the biological film on the cathode electrode and the elemental sulfur particles occur, and when the dropped biological film is accumulated in the filler and the blockage occurs, the filler is required to be backwashed in time; the sulfur particle filler is a consumption type carrier, and simple substance sulfur particles are timely supplemented by combining water quality and treatment load;
step b: in the anode chamber, anode loss electrons become soluble metal ions and enter the anode chamber, the soluble metal ions react with phosphate ions in phosphate-containing wastewater to generate precipitates for removal, and meanwhile, part of phosphate is removed through the adsorption of metal hydroxide; discharging the generated precipitate through a discharge port at the bottom of the anode chamber, allowing the phosphorus-free wastewater after the precipitation reaction to flow into a sedimentation tank through a discharge pipe, and performing sedimentation filtration to obtain purified water;
in the process of carrying out phosphorus removal on the anode chamber and carrying out nitrogen removal on the cathode chamber, proton exchange is carried out between the anode chamber and the cathode chamber through a proton exchange membrane, so that charge flow is formed between the anode chamber and the cathode chamber.
More preferably, the method for domesticating and enriching the denitrification biological membrane on the elemental sulfur particles and the cathode electrode comprises the following steps: inoculating activated anaerobic sludge or sulfur autotrophic denitrifying bacteria to the sulfur granules or the cathode electrode, adding nutrient solution for culturing until the microorganism enrichment and biofilm formation are finished, and domesticating the enriched denitrifying biomembranes on the surfaces of the sulfur granules and the cathode; the sulfur autotrophic denitrifying bacteria comprise: one or more of Thiobacillus (Thiobacillus), Thiobacillus (Thiomospira), Thielavia (Thiothrix), Thiobacillus (Beggiatoa), Thiobacillus (Thiobacillus), Achromobacter (Achromobacter), and Sulfolobus (Sulfolobus).
Further, the method for domesticating and enriching the denitrification and denitrification microbial membrane on the surface of the cathode electrode comprises the following steps: enriching a biological membrane on a cathode by an intermittent operation double-chamber bioelectrochemical reactor, placing inoculated anaerobic sludge in a cathode chamber, injecting a cathode reaction solution, and applying an external voltage of 0.3-0.8V;
when an easily oxidized Fe and Al metal electrode is used as an anode, the anolyte is phosphate solution with the conductivity of 0.5-1.0ms/cm or secondary effluent of an urban domestic sewage treatment plant; when the carbon material is used as an anode, the anolyte is a ferrous ion solution with the concentration of 50-200mM, and the ferrous ion solution is prepared by a phosphate buffer solution with the concentration of 50-100 mM;
replacing the reaction solution once at intervals of 24-48h, and continuously culturing for 20-30 cycles; the volume ratio of inoculated anaerobic sludge to cathode reaction liquid to anode liquid is 1-2: 5: 5; the inoculated active anaerobic sludge is an urban domestic sewage treatment plant A2The sludge of the secondary sedimentation tank of the O process;
the cathode reaction solution is secondary effluent of an urban domestic sewage treatment plant or simulated nitrogen and phosphorus-containing sewage, and the simulated nitrogen and phosphorus-containing sewage comprises the following components: NO3 --N concentration: 15-60 mg/L; PO (PO)4 3--concentration of P: 1-3 mg/L; NaHCO 23The concentration is 100-500 mg/L; wolfe vitamin solution: 0.1-0.5 mL/L; wolfe mineral solution: 0.2-1 mL/L; CH (CH)3COONa concentration is 0.2-1.5 g/L.
Further, the method for domesticating and enriching the denitrification and denitrification microbial membrane on the surface of the sulfur granules comprises the following steps: placing inoculated anaerobic sludge and sulfur particles in an anaerobic culture bottle, then adding a microbial culture solution, and placing the culture bottle in a shaking table for culture, wherein the culture conditions are as follows: 50-120rpm, 25-30 ℃; replacing the reaction solution once at intervals of 24-48h, and continuously culturing for 20-30 cycles;
the volume ratio of the inoculated active anaerobic sludge to the sulfur particles to the microbial culture solution is 1-2: 5: 2; the inoculated active anaerobic sludge is an urban domestic sewage treatment plant A2The sludge of the secondary sedimentation tank of the O process;
the main components of the microbial culture solution are nitrate and sulfide, and partial nutrient elements and trace elements are added, and the microbial culture solution comprises the following specific components: NO3 --N：15-60mg/L；Na2S·9H2O：10-50mg/L；Na2S2O3·5H2O：10-50mg/L；NaHCO3：0.1-0.5g/L；NH4Cl：1-10mg/L；KCl：0.01-0.1g/L；Na2HPO4.12H2O: 10-35 mg/L; wolfe vitamin solution: 0.1-0.5 mL/L; wolfe mineral solution: 0.2-1 mL/L.
On the other hand, the invention also provides a sewage denitrification and dephosphorization treatment device, which comprises a reaction tank, wherein the reaction tank comprises an anode chamber and a cathode chamber which are connected with each other and provided with a proton exchange membrane between the anode chamber and the cathode chamber, an anode electrode made of iron or aluminum as a conductive material is arranged in the anode chamber, a cathode electrode made of a carbon-based material or a metal-based material as a conductive material is arranged in the cathode chamber, and two ends of the anode electrode and the cathode electrode are externally connected with a direct current power supply through leads; the cathode chamber is internally provided with a filter tank, sulfur particles are filled in the filter tank, the side wall of the filter tank is provided with a porous insulating material layer, and the cathode electrode is arranged outside the filter tank.
Preferably, the cathode chamber is connected with a sewage tank through a water inlet pipe, and a water inlet pump is arranged on the water inlet pipe; the anode chamber is connected with a sedimentation tank through a water outlet pipe; the bottoms of the cathode chamber and the anode chamber are connected with a circulating pump through pipelines; a double-cathode electrode is arranged in the cathode chamber; the surfaces of the sulfur particles and the double cathodes are inoculated with enrichment biofilm and are provided with denitrification microbial biofilms.
Further, the elemental sulfur particles are sulfur particles, the purity is more than 99.0%, and the particle size is 0.5-0.8 cm; the mass filling ratio of iron or aluminum to sulfur is 1: 3-6; the conductive material of the cathode electrode is one of carbon paper, carbon cloth, carbon felt, graphite plate and modified materials thereof, or a metal material of stainless steel, iron, aluminum, copper, zinc, nickel or titanium.
In a third aspect, the invention further provides application of the sewage denitrification and dephosphorization treatment device in the aspects of advanced treatment of nitrogen and phosphorus in tail water of a sewage plant, eutrophication treatment of surface water of lakes, rivers and oceans, removal of nitrate in underground water, pretreatment of industrial wastewater containing nitrogen and phosphorus and pretreatment of drinking water in the environmental field.
The principle of the sewage denitrification and dephosphorization treatment of the invention is as follows:
the principle diagram of the invention is shown in figure 2, and the invention is realized in a double-chamber bioelectrochemical reactor, wherein an iron rod is used as an anode (left), carbon cloth is used as a cathode (right, double cathodes are arranged), and the two ends of the cathode and the anode are provided with external voltage by using a direct current power supply. Elemental sulfur is used as a filler and is placed in the cathode chamber, and the elemental sulfur is separated from cathode carbon cloth by using an insulating porous material. The cathode and anode chambers are separated by a Proton Exchange Membrane (PEM). Sludge is inoculated in the cathode chamber, and microorganisms with denitrification function are domesticated and enriched on the sulfur particles and the cathode carbon cloth. The anode chamber is a chemical process and does not need to be inoculated with microorganisms. The sewage containing nitrate and phosphate firstly enters into the cathode chamber, and nitrate is removed through sulfur autotrophic denitrification and cathode denitrification. And pumping the cathode effluent into the anode chamber, and carrying out precipitation reaction on phosphate radicals and iron ions generated by anode iron sacrifice or removing the phosphate radicals by adsorption of formed iron hydroxide. Before reaction, both the cathode chamber and the anode chamber are filled with water and have the same components. Then simultaneously starting the water inlet pump and the circulating pump to continuously work all the time, keeping the liquid level in the cathode chamber balanced, and keeping the flow rate the same. Taking the effluent of the cathode chamber to test the content of nitrate, and changing the retention time of the sewage in the cathode chamber by adjusting the flow rates of the water inlet pump and the circulating pump until the nitrate is completely removed.
The electrolysis method is an efficient sewage treatment method, integrates various processes such as precipitation, flocculation, air flotation and the like, and has obvious effect on removing phosphorus. The electrolytic dephosphorization technology has the advantages of high dephosphorization rate, stable performance, stronger selectivity and convenient daily maintenance. Taking the ferroelectric as an example: fe released at the anode during electrolysis2+And Fe in solution3+Can react with phosphorus in the form of phosphate radical to generate insoluble iron salt. In addition, part of Fe2+And Fe3+At a certain pH range with OH in solution-The reaction generates indissolvable iron hydroxyl compounds, and the iron hydroxyl complexes can generate colloid flocculation, thereby achieving the effect of treating water quality.
Anode: fe-2e-＝Fe2+
Cathode: 2H++2e-＝H2
In solution：4Fe2++2H2O+O2＝4Fe3++4OH-
Fe3++PO4 3-＝FePO4↓
3Fe2++2PO4 3-＝Fe3(PO4)2↓
Fe2++2OH-＝Fe(OH)2↓
4Fe(OH)2+O2+2H2O＝4Fe(OH)3↓
The sulfur autotrophic denitrification technology refers to that certain microorganisms utilize reduced sulfur (simple substance S, H) under the anoxic or anaerobic condition2S、S2-、S2O3 2-) Provides electron for autotrophic denitrification. In the invention, under an anaerobic condition, elemental sulfur provides an electron donor, and nitrate or nitrite is used as an electron acceptor to reduce the elemental sulfur into nitrogen so as to achieve the aim of denitrification. The sulfur has wide source, low price and easy obtainment, stable properties, low operation cost and convenient operation and management as the sulfur autotrophic denitrification electron donor, the sulfur autotrophic denitrification reaction is carried out under the anoxic condition, no additional aeration is needed, the power consumption is low, no additional organic matter is needed to be added, and the process has low sludge yield and low biological yield.
The principle of biological electrode denitrification is that denitrifying bacteria attached to the surface of a cathode take the electrode as an electron donor or hydrogen generated by cathode electrolysis as the electron donor to remove NO3 -Reduction of-N to N2Thereby achieving the purpose of removing nitrate nitrogen. The biological cathode provides electrons, so that the problem of insufficient carbon source in the sewage denitrification process can be effectively solved, and secondary pollution caused by adding the carbon source is avoided. The biological electrode has high denitrification efficiency, simple operation and strong controllability.
2NO3 -+10e-+12H+→N2+6H2O
2NO3 -+5H2+4H+→N2+6H2O
Compared with the prior art, the invention has the following beneficial technical effects:
1) the invention integrates two functions of nitrogen removal and phosphorus removal in a bioelectrochemical system in a coupling way, thereby realizing deep nitrogen and phosphorus removal of sewage more simply and controllably; the oxidation of anode iron or aluminum is used for replacing the adding of the traditional phosphorus removing agent, and meanwhile, elemental sulfur is used for replacing an organic carbon source as an electron donor for denitrification, so that the operation cost is obviously reduced; compared with the combination of the prior deep denitrification process by adding the organic carbon source and the flocculation precipitation process by adding the ferric salt, the method has the advantages of no medicament secondary pollution risk and low sludge yield in the denitrification and dephosphorization process.
2) The sewage nitrogen and phosphorus removal method by coupling the sulfur autotrophic denitrification and the micro-electric field iron oxidation utilizes iron-aluminum simple substance to coordinate the sulfur autotrophic denitrification for nitrogen and phosphorus removal under the condition that no chemical phosphorus removal agent and organic carbon source are added, and in addition, a cathode can consume hydrogen ions generated in the sulfur autotrophic denitrification process, so that the buffer capacity of the system on pH is enhanced. The sulfur and the iron-aluminum simple substance used in the process are low in price, the raw materials are easy to obtain, the working condition operation is stable, and the sludge yield is low. The advanced nitrogen and phosphorus removal is carried out on the secondary effluent of the sewage, the nitrate removal rate can be more than 95%, and the phosphate removal rate can reach more than 90%, so that the final effluent can completely reach the first-level A standard in pollutant discharge standards of urban sewage treatment plants (GB18918-2002), the total phosphorus of the effluent is stably lower than 0.3mg/L, the nitrate nitrogen is stably lower than 3mg/L, and the sludge reduction is more than 10%.
Drawings
The invention will be further described with reference to the accompanying drawings;
FIG. 1 is a schematic configuration diagram of a sewage treatment apparatus according to embodiment 1 of the present invention; in the figure, 1-a sedimentation tank, 2-a water inlet pump, 3-a water inlet pipe, 4-a cathode electrode, 5-a porous insulating material, 6-elemental sulfur particles, 7-a cathode chamber, 8-a circulating pump, 9-a proton exchange membrane, 10-a direct current power supply, 11-an anode electrode, 12-an anode chamber, 13-a water outlet pipe, 14-a sewage tank and 15-a filter tank.
Fig. 2 is a schematic diagram of the structure of the present invention.
Detailed Description
In order that the above objects, features and advantages of the present invention can be more clearly understood, a detailed description of the present invention will be given below with reference to the accompanying drawings and specific embodiments. It should be noted that the embodiments and features of the embodiments of the present application may be combined with each other without conflict.
Example 1:
the sewage denitrification and dephosphorization treatment device comprises a reaction tank, as shown in fig. 1, the reaction tank comprises an anode chamber 12 and a cathode chamber 7 which are connected with each other and provided with a proton exchange membrane 9 therebetween, an anode electrode 11 made of iron as a conductive material is arranged in the anode chamber 12, a double-cathode electrode is arranged in the cathode chamber 7, and the cathode electrode 4 is a carbon cloth electrode. Two ends of the anode electrode 4 and the cathode electrode 11 are externally connected with a direct current power supply 10 through leads; a filter 15 is arranged in the cathode chamber 7, elemental sulfur particles 6 are filled in the filter 15, a porous insulating material layer 5 is arranged on the side wall of the filter 15, and the cathode electrode 11 is arranged outside the filter 15; the surfaces of the elemental sulfur particles 6 and the cathode electrode 4 are inoculated with enrichment biofilm and provided with denitrification microbial biofilms. The cathode chamber 7 is connected with a sewage tank 14 through a water inlet pipe 3, and a water inlet pump 2 is arranged on the water inlet pipe 3; the anode chamber 12 is connected with the sedimentation tank 1 through a water outlet pipe 13; the bottom parts of the cathode chamber 7 and the anode chamber 12 are connected with a circulating pump 8 through a pipeline. The mass filling ratio of iron to sulfur is 1: 3; the cathode is arranged as a double electrode, so that the reaction area can be increased, the effect is improved, and the reaction area can be increased and the treatment effect can be promoted by additionally arranging one cathode.
And (3) cathode film formation:
the method for domesticating and enriching the denitrification microbial membrane on the surface of the cathode electrode comprises the following steps: enriching a biological membrane on a cathode by an intermittent operation double-chamber bioelectrochemical reactor, placing inoculated anaerobic sludge in a cathode chamber, injecting a cathode reaction solution, and applying an external voltage of 0.3V;
using a carbon material as an anode, wherein the anolyte is a ferrous ion solution (potassium ferrocyanide) with the concentration of 200mM, and the ferrous ion solution is prepared by Phosphate Buffer Solution (PBS) with the concentration of 50 mM; replacing the reaction solution (50mL) once at intervals of 48h, and continuously culturing for 20 cycles; body inoculated with anaerobic sludge, cathode reaction liquid and anode liquidThe product ratio is 2: 5: 5; the inoculated active anaerobic sludge is an urban domestic sewage treatment plant A2The sludge of the secondary sedimentation tank of the O process;
the cathode reaction solution is secondary effluent of an urban domestic sewage treatment plant or simulated nitrogen and phosphorus-containing sewage, and the simulated nitrogen and phosphorus-containing sewage comprises the following components: NO3 --N concentration: 60mg/L, adding KNO3 432mg/L；PO4 3--concentration of P: 3mg/L of Na is added2HPO4.12H2O 35mg/L；NaHCO3The concentration is 500 mg/L; wolfe vitamin solution: 0.5 mL/L; wolfe mineral solution: 1 mL/L; CH (CH)3COONa concentration is 1.5 g/L.
Coating sulfur particles:
the method for domesticating, enriching and denitrifying microorganism films on the surfaces of sulfur granules comprises the following steps: taking municipal domestic sewage treatment plant (A)2O process) secondary sedimentation tank sludge (100mL) and sulphur granules (filling volume 200 mL; purity of>99.0% and 0.5-0.8cm in particle size) in an anaerobic flask, then 200mL of microbial broth was added, the flask was placed in a shaker for cultivation, the culture conditions: 120rpm, 25 ℃; replacing the reaction solution once at intervals of 48h, and continuously culturing for 20 cycles; the sulfur particles with obvious biofilm attachment are filled into the filter in the cathode chamber on the surface.
The volume ratio of the inoculated active anaerobic sludge to the sulfur particles to the microbial culture solution is 1-2: 5: 2; the inoculated active anaerobic sludge is an urban domestic sewage treatment plant A2The sludge of the secondary sedimentation tank of the O process;
the main components of the microbial culture solution are nitrate and sulfide, and partial nutrient elements and trace elements are added, and the microbial culture solution comprises the following specific components: NO3 --N：60mg/L；Na2S·9H2O：50mg/L；Na2S2O3·5H2O：50mg/L；NaHCO3：0.5g/L；NH4Cl：10mg/L；KCl：0.1g/L；Na2HPO4.12H2O: 35 mg/L; wolfe vitamin solution: 0.5 mL/L; wolfe mineral solution: 1 mL/L.
The sewage denitrification and dephosphorization treatment method comprises the following steps:
step a, filling water into a cathode chamber and an anode chamber, and connecting and electrifying an anode and a cathode with the anode and the cathode of an external power supply; meanwhile, a water inlet pump and a circulating pump are started, the flow rates of the water inlet pump and the circulating pump are the same, and the liquid level of the cathode chamber is kept balanced; introducing sewage containing nitrate and phosphate into a cathode chamber, wherein sulfur autotrophic denitrifying bacteria in the biomembrane on the surface of the elemental sulfur particles use sulfur as an electron donor, active bacteria attached to the biomembrane on the surface of the cathode use the cathode as the electron donor, nitrate in the sewage is reduced into nitrogen to be removed, and the generated nitrogen is discharged from an exhaust port; the nitrogen-free wastewater after denitrification is discharged into the anode chamber by a circulating pump;
b, in the anode chamber, anode loss electrons become soluble metal ions and enter the anode chamber, the soluble metal ions react with phosphate ions in phosphate-containing wastewater to generate precipitates to be removed, and meanwhile, part of phosphate is removed through the adsorption of metal hydroxide; and discharging the generated precipitate through a discharge port at the bottom of the anode chamber, allowing the phosphorus-free wastewater after the precipitation reaction to flow into a sedimentation tank through a discharge pipe, and performing sedimentation filtration to obtain purified water.
As a result: and (5) verifying the removal effect of nitrate and phosphate by using simulated water quality. The simulated water quality is as follows: KNO3(216mg/L)，Na2HPO4.12H2O(35mg/L)NaHCO3(1g/L) KCl (0.13g/L), wolfe vitamin solution (0.2mL/L) and wolfe mineral element solution (1 mL/L). The applied voltage is 0.3V, the reactor residence time is 4h, the nitrate removal rate can be more than 98.7 percent, and the phosphate removal rate reaches 95.3 percent.
Example 2:
the sewage denitrification and dephosphorization treatment device comprises a reaction tank, wherein the reaction tank comprises an anode chamber 12 and a cathode chamber 7 which are connected with each other and provided with a proton exchange membrane 9 therebetween, an anode electrode 11 made of iron as a conductive material is arranged in the anode chamber 12, a double-cathode electrode is arranged in the cathode chamber 7, and the cathode electrode 4 is a carbon cloth electrode. Two ends of the anode electrode 4 and the cathode electrode 11 are externally connected with a direct current power supply 10 through leads; a filter 15 is arranged in the cathode chamber 7, elemental sulfur particles 6 are filled in the filter 15, a porous insulating material layer 5 is arranged on the side wall of the filter 15, and the cathode electrode 11 is arranged outside the filter 15; the surfaces of the elemental sulfur particles 6 and the cathode electrode 4 are inoculated with enrichment biofilm and provided with denitrification microbial biofilms. The cathode chamber 7 is connected with a sewage tank 14 through a water inlet pipe 3, and a water inlet pump 2 is arranged on the water inlet pipe 3; the anode chamber 12 is connected with the sedimentation tank 1 through a water outlet pipe 13; the bottom parts of the cathode chamber 7 and the anode chamber 12 are connected with a circulating pump 8 through a pipeline. The mass filling ratio of iron to sulfur is 1: 3. the surfaces of the sulfur particles and the cathode are not inoculated with enrichment biofilm and are provided with denitrification denitrogenation microbial membranes.
The sewage denitrification and dephosphorization treatment method comprises the following steps:
step a, filling water into a cathode chamber and an anode chamber, and connecting and electrifying an anode and a cathode with the anode and the cathode of an external power supply; meanwhile, a water inlet pump and a circulating pump are started, the flow rates of the water inlet pump and the circulating pump are the same, and the liquid level of the cathode chamber is kept balanced; introducing sewage containing nitrate and phosphate into a cathode chamber, wherein sulfur autotrophic denitrifying bacteria in the biomembrane on the surface of the elemental sulfur particles use sulfur as an electron donor, active bacteria attached to the biomembrane on the surface of the cathode use the cathode as the electron donor, nitrate in the sewage is reduced into nitrogen to be removed, and the generated nitrogen is discharged from an exhaust port; the nitrogen-free wastewater after denitrification is discharged into the anode chamber by a circulating pump;
b, in the anode chamber, anode loss electrons become soluble metal ions and enter the anode chamber, the soluble metal ions react with phosphate ions in phosphate-containing wastewater to generate precipitates to be removed, and meanwhile, part of phosphate is removed through the adsorption of metal hydroxide; and discharging the generated precipitate through a discharge port at the bottom of the anode chamber, allowing the phosphorus-free wastewater after the precipitation reaction to flow into a sedimentation tank through a discharge pipe, and performing sedimentation filtration to obtain purified water.
As a result: under the condition that the cathode electrode and the sulfur particles are not subjected to biofilm formation treatment, the method realizes the high-efficiency removal of phosphate by using simulated water quality, and verifies the feasibility of the method for removing phosphorus. The simulated water quality is as follows: KNO3(216mg/L)，Na2HPO4.12H2O(35mg/L)NaHCO3(1g/L) KCl (0.13g/L), wolfe vitamin solution (0.2mL/L) and wolfe mineral element solution (1 mL/L). At an applied voltage of 0.3V, reverseThe reactor residence time is 4 hours, the phosphate removal rate reaches 80.7 percent, and the nitrate removal rate is lower than 10 percent. In the invention, phosphate radical and iron ions generated by anode iron sacrifice are subjected to precipitation reaction or are absorbed and removed by formed iron hydroxide, and the process is a non-biological reaction. Electrochemical reduction of nitrate is difficult to occur under a set potential, and elemental sulfur can stably coexist with nitrate, so that the nitrate removal efficiency is low under the condition that a cathode electrode and sulfur particles are not subjected to film forming treatment. Although theoretically at a greater applied voltage (C:)>1V), nitrates are removed by an electrochemical reduction process, but too high a voltage results in excessive precipitation of anode metal and high energy consumption. Thus, this example illustrates that the coating of the cathode electrode and the surface of the sulphur particles is essential for the efficient and economical removal of nitrate in the present invention.
Example 3:
the sewage denitrification and dephosphorization treatment device comprises a reaction tank, wherein the reaction tank comprises an anode chamber 12 and a cathode chamber 7 which are connected with each other and provided with a proton exchange membrane 9 therebetween, an anode electrode 11 made of aluminum serving as a conductive material is arranged in the anode chamber 12, and a double-cathode electrode which is a carbon brush electrode is arranged in the cathode chamber 7. Two ends of the anode electrode 4 and the cathode electrode 11 are externally connected with a direct current power supply 10 through leads; a filter 15 is arranged in the cathode chamber 7, elemental sulfur particles 6 are filled in the filter 15, a porous insulating material layer 5 is arranged on the side wall of the filter 15, and the cathode electrode 11 is arranged outside the filter 15; the surfaces of the elemental sulfur particles 6 and the cathode electrode 4 are inoculated with enrichment biofilm and provided with denitrification microbial biofilms. The cathode chamber 7 is connected with a sewage tank 14 through a water inlet pipe 3, and a water inlet pump 2 is arranged on the water inlet pipe 3; the anode chamber 12 is connected with the sedimentation tank 1 through a water outlet pipe 13; the bottom parts of the cathode chamber 7 and the anode chamber 12 are connected with a circulating pump 8 through a pipeline. The mass filling ratio of iron to sulfur is 1: 6.
and (3) cathode film formation:
the method for domesticating and enriching the denitrification microbial membrane on the surface of the cathode electrode comprises the following steps: enriching a biological membrane on a cathode by an intermittent operation double-chamber bioelectrochemical reactor, placing inoculated anaerobic sludge in a cathode chamber, injecting a cathode reaction solution, and applying an external voltage of 0.3V;
an easily oxidized Fe metal electrode is used as an anode, and anolyte is phosphate solution with the conductivity of 0.5-1.0ms/cm or secondary effluent of an urban domestic sewage treatment plant; replacing the reaction solution once at intervals of 48h, and continuously culturing for 20 cycles; the volume ratio of inoculated anaerobic sludge to cathode reaction liquid to anode liquid is 1: 5: 5; the inoculated active anaerobic sludge is an urban domestic sewage treatment plant A2The sludge of the secondary sedimentation tank of the O process;
the cathode reaction solution is secondary effluent of an urban domestic sewage treatment plant or simulated nitrogen and phosphorus-containing sewage, and the simulated nitrogen and phosphorus-containing sewage comprises the following components: NO3 --N concentration: 15 mg/L; PO (PO)4 3--concentration of P: 1 mg/L; NaHCO 23The concentration is 100 mg/L; wolfe vitamin solution: 0.1 mL/L; wolfe mineral solution: 0.2 mL/L; CH (CH)3COONa concentration is 0.2 g/L.
Coating sulfur particles:
the method for domesticating, enriching and denitrifying microorganism films on the surfaces of sulfur granules comprises the following steps: taking municipal domestic sewage treatment plant (A)2O process) secondary sedimentation tank sludge (200mL) and sulphur granules (filling volume 500 mL; purity of>99.0% and 0.5-0.8cm in particle size) in an anaerobic flask, then 200mL of microbial broth was added, the flask was placed in a shaker for cultivation, the culture conditions: 50rpm, 30 ℃; replacing the reaction solution once at intervals of 24h, and continuously culturing for 30 cycles; the sulfur particles with obvious biofilm attachment are filled into the filter in the cathode chamber on the surface. The inoculated active anaerobic sludge is an urban domestic sewage treatment plant A2The sludge of the secondary sedimentation tank of the O process;
the main components of the microbial culture solution are nitrate and sulfide, and partial nutrient elements and trace elements are added, and the microbial culture solution comprises the following specific components: NO3 --N：15mg/L；Na2S·9H2O：10mg/L；Na2S2O3·5H2O：10mg/L；NaHCO3：0.1g/L；NH4Cl：10mg/L；KCl：0.01g/L；Na2HPO4.12H2O: 10 mg/L; wolfe vitamin solution: 0.1 mL/L; wolfe mineral solution: 0.2 mL/L.
The sewage denitrification and dephosphorization treatment method comprises the following steps:
step a, filling water into a cathode chamber and an anode chamber, and connecting and electrifying an anode and a cathode with the anode and the cathode of an external power supply; meanwhile, a water inlet pump and a circulating pump are started, the flow rates of the water inlet pump and the circulating pump are the same, and the liquid level of the cathode chamber is kept balanced; introducing sewage containing nitrate and phosphate into a cathode chamber, wherein sulfur autotrophic denitrifying bacteria in the biomembrane on the surface of the elemental sulfur particles use sulfur as an electron donor, active bacteria attached to the biomembrane on the surface of the cathode use the cathode as the electron donor, nitrate in the sewage is reduced into nitrogen to be removed, and the generated nitrogen is discharged from an exhaust port; the nitrogen-free wastewater after denitrification is discharged into the anode chamber by a circulating pump;
b, in the anode chamber, anode loss electrons become soluble metal ions and enter the anode chamber, the soluble metal ions react with phosphate ions in phosphate-containing wastewater to generate precipitates to be removed, and meanwhile, part of phosphate is removed through the adsorption of metal hydroxide; and discharging the generated precipitate through a discharge port at the bottom of the anode chamber, allowing the phosphorus-free wastewater after the precipitation reaction to flow into a sedimentation tank through a discharge pipe, and performing sedimentation filtration to obtain purified water.
The high-efficiency removal of nitrate and phosphate is realized by using simulated water quality, and the feasibility of the method is verified. The simulated water quality is as follows: KNO3(216mg/L)，Na2HPO4.12H2O(35mg/L)NaHCO3(1g/L) KCl (0.13g/L), wolfe vitamin solution (0.2mL/L) and wolfe mineral element solution (1 mL/L). The applied voltage is 0.3V, the reactor residence time is 4h, the nitrate removal rate can be more than 96.2 percent, and the phosphate removal rate reaches 92.5 percent.
Verification example:
taking a certain urban sewage treatment plant as an example, and taking the actual quality of secondary treated effluent in the plant in Table 1, after advanced treatment is carried out by adopting the biological sewage treatment nitrogen and phosphorus removal method, the total phosphorus concentration of the effluent is 0.1-0.3 mg/L, the total nitrogen concentration of the effluent is 1.0-2.8mg/L, and the effluent completely reaches the first-grade A standard in pollutant discharge Standard of urban sewage treatment plant (GB18918-2002) under the condition of no addition of chemical agents.
TABLE 1 quality of secondary treated effluent from municipal sewage treatment plant
The foregoing is merely exemplary of embodiments of the present invention and is not intended to limit the invention in any manner. The scope of the present invention is defined by the claims and is not limited by the embodiments described above, and any simple modifications or equivalent changes and modifications made to the above embodiments according to the technical spirit of the present invention are included in the scope of the present invention.
Claims (10)
1. A sewage denitrification and dephosphorization treatment method is characterized by comprising the following steps: the denitrification and dephosphorization reactions are respectively realized in a cathode chamber and an anode chamber of the double-chamber bioelectrochemical reaction tank, a proton exchange membrane is arranged between the cathode chamber and the anode chamber, an iron or aluminum material is used as an anode electrode, a carbon-based material or a metal-based material is used as a cathode electrode, and a direct-current power supply is utilized to provide external voltage at the two ends of the cathode and the anode; elemental sulfur particles are used as filler and are placed in an insulating porous material filter tank of a cathode chamber, and a cathode electrode is arranged outside the filter tank; firstly, sewage containing nitrate and phosphate enters a cathode chamber through a water inlet pump, and nitrate is removed through sulfur autotrophic denitrification and cathode denitrification; pumping the effluent from the cathode chamber into the anode chamber through circulation, and removing phosphate radicals and metal ions generated by anode iron or aluminum sacrifice through precipitation reaction or adsorption by formed iron or aluminum hydroxide; and controlling the hydraulic retention time to finish the treatment of the nitrogen and the phosphorus in the sewage.
2. The sewage denitrification and dephosphorization treatment method according to claim 1, wherein: the carbon-based material comprises carbon paper, carbon cloth, carbon felt, graphite plate and modified modification materials thereof; the metal-based material comprises stainless steel, iron, aluminum, copper, zinc, nickel and titanium electrode base materials; the elemental sulfur particles and the biomembrane with the denitrification function are domesticated and enriched on the cathode electrode.
3. The sewage denitrification and dephosphorization treatment method according to claim 1 or 2, which comprises the following steps:
step a, filling water into a cathode chamber and an anode chamber, and connecting and electrifying an anode and a cathode with the anode and the cathode of an external power supply; meanwhile, a water inlet pump and a circulating pump are started, the flow rates of the water inlet pump and the circulating pump are the same, and the liquid level of the cathode chamber is kept balanced; introducing sewage containing nitrate and phosphate into a cathode chamber, wherein sulfur autotrophic denitrifying bacteria in the biomembrane on the surface of the elemental sulfur particles use sulfur as an electron donor, active bacteria attached to the biomembrane on the surface of the cathode use the cathode as the electron donor, nitrate in the sewage is reduced into nitrogen to be removed, and the generated nitrogen is discharged from an exhaust port; the nitrogen-free wastewater after denitrification is discharged into the anode chamber by a circulating pump; in the cathode chamber, with the increase of the operation period, the proliferation and the updating of the biological film on the cathode electrode and the elemental sulfur particles occur, and when the dropped biological film is accumulated in the filler and the blockage occurs, the filler is required to be backwashed in time; the elemental sulfur particle filler is a consumption type carrier and is combined with water quality and treatment load to supplement elemental sulfur particles in time;
b, in the anode chamber, anode loss electrons become soluble metal ions and enter the anode chamber, the soluble metal ions react with phosphate ions in phosphate-containing wastewater to generate precipitates to be removed, and meanwhile, part of phosphate is removed through the adsorption of metal hydroxide; discharging the generated precipitate through a discharge port at the bottom of the anode chamber, allowing the phosphorus-free wastewater after the precipitation reaction to flow into a sedimentation tank through a discharge pipe, and performing sedimentation filtration to obtain purified water;
in the process of carrying out phosphorus removal on the anode chamber and carrying out nitrogen removal on the cathode chamber, proton exchange is carried out between the anode chamber and the cathode chamber through a proton exchange membrane, so that charge flow is formed between the anode chamber and the cathode chamber.
4. The sewage nitrogen and phosphorus removal treatment method of claim 2, wherein the elemental sulfur particles and the method for domesticating the enriched denitrification biological membrane on the cathode electrode are as follows: inoculating activated anaerobic sludge or sulfur autotrophic denitrifying bacteria to the sulfur granules or the cathode electrode, adding nutrient solution for culturing until the microorganism enrichment and biofilm formation are finished, and domesticating the enriched denitrifying biomembranes on the surfaces of the sulfur granules and the cathode; the sulfur autotrophic denitrifying bacteria comprise: one or more of Thiobacillus (Thiobacillus), Thiobacillus (Thiomospira), Thielavia (Thiothrix), Thiobacillus (Beggiatoa), Thiobacillus (Thiobacillus), Achromobacter (Achromobacter), and Sulfolobus (Sulfolobus).
5. The sewage nitrogen and phosphorus removal treatment method of claim 4, wherein the method for domesticating and enriching the denitrification microbial membrane on the surface of the cathode electrode comprises the following steps: enriching a biological membrane on a cathode by an intermittent operation double-chamber bioelectrochemical reactor, placing inoculated anaerobic sludge in a cathode chamber, injecting a cathode reaction solution, and applying an external voltage of 0.3-0.8V;
when an easily oxidized Fe and Al metal electrode is used as an anode, the anolyte is phosphate solution with the conductivity of 0.5-1.0ms/cm or secondary effluent of an urban domestic sewage treatment plant; when the carbon material is used as an anode, the anolyte is a ferrous ion solution with the concentration of 50-200mM, and the ferrous ion solution is prepared by a phosphate buffer solution with the concentration of 50-100 mM;
replacing the reaction solution once at intervals of 24-48h, and continuously culturing for 20-30 cycles; the volume ratio of inoculated anaerobic sludge to cathode reaction liquid to anode liquid is 1-2: 5: 5; the inoculated active anaerobic sludge is an urban domestic sewage treatment plant A2The sludge of the secondary sedimentation tank of the O process;
the cathode reaction solution is secondary effluent of an urban domestic sewage treatment plant or simulated nitrogen and phosphorus-containing sewage, and the simulated nitrogen and phosphorus-containing sewage comprises the following components: NO3 --N concentration: 15-60 mg/L; PO (PO)4 3--concentration of P: 1-3 mg/L; NaHCO 23The concentration is 100-500 mg/L; wolfe vitamin solution: 0.1-0.5 mL/L; wolfe mineral solution: 0.2-1 mL/L; CH (CH)3COONa concentration is 0.2-1.5 g/L.
6. The sewage nitrogen and phosphorus removal treatment method of claim 4, wherein the method for domesticating and enriching the denitrification microbial film on the surface of the sulfur granules comprises the following steps: placing inoculated anaerobic sludge and sulfur particles in an anaerobic culture bottle, then adding a microbial culture solution, and placing the culture bottle in a shaking table for culture, wherein the culture conditions are as follows: 50-120rpm, 25-30 ℃; replacing the reaction solution once at intervals of 24-48h, and continuously culturing for 20-30 cycles;
the volume ratio of the inoculated active anaerobic sludge to the sulfur particles to the microbial culture solution is 1-2: 5: 2; the inoculated active anaerobic sludge is an urban domestic sewage treatment plant A2The sludge of the secondary sedimentation tank of the O process;
the main components of the microbial culture solution are nitrate and sulfide, and partial nutrient elements and trace elements are added, and the microbial culture solution comprises the following specific components: NO3 --N：15-60mg/L；Na2S·9H2O：10-50mg/L；Na2S2O3·5H2O：10-50mg/L；NaHCO3：0.1-0.5g/L；NH4Cl：1-10mg/L；KCl：0.01-0.1g/L；Na2HPO4.12H2O: 10-35 mg/L; wolfe vitamin solution: 0.1-0.5 mL/L; wolfe mineral solution: 0.2-1 mL/L.
7. The sewage denitrification and dephosphorization treatment device is characterized by comprising a reaction tank, wherein the reaction tank comprises an anode chamber and a cathode chamber which are connected with each other and provided with a proton exchange membrane between the anode chamber and the cathode chamber, an anode electrode made of iron or aluminum as a conductive material is arranged in the anode chamber, a cathode electrode made of a carbon-based material or a metal-based material as a conductive material is arranged in the cathode chamber, and two ends of the anode electrode and two ends of the cathode electrode are externally connected with a direct current power supply through leads; the cathode chamber is internally provided with a filter tank, sulfur particles are filled in the filter tank, the side wall of the filter tank is provided with a porous insulating material layer, and the cathode electrode is arranged outside the filter tank.
8. The sewage denitrification and dephosphorization treatment device according to claim 6, wherein said cathode chamber is connected to a sewage tank through a water inlet pipe, said water inlet pipe being provided with a water inlet pump; the anode chamber is connected with a sedimentation tank through a water outlet pipe; the bottoms of the cathode chamber and the anode chamber are connected with a circulating pump through pipelines; a double-cathode electrode is arranged in the cathode chamber; the surfaces of the sulfur particles and the cathode are inoculated with an enrichment biofilm, and a denitrification microbial film is arranged on the enrichment biofilm.
9. The sewage denitrification and dephosphorization treatment device according to claim 6, wherein said elemental sulfur particles are sulfur particles, with a purity of > 99.0% and a particle size of 0.5-0.8 cm; the mass filling ratio of iron or aluminum to sulfur is 1: 3-6; the conductive material of the cathode electrode is one of carbon paper, carbon cloth, carbon felt, graphite plate and modified materials thereof, or a metal material of stainless steel, iron, aluminum, copper, zinc, nickel or titanium.
10. The sewage denitrification and dephosphorization treatment device according to any one of claims 7 to 9 is applied to the environmental field for advanced treatment of nitrogen and phosphorus in tail water of sewage plants, eutrophication treatment of surface water of lakes, rivers and oceans, removal of nitrate from underground water, pretreatment of industrial wastewater containing nitrogen and phosphorus and pretreatment of drinking water.
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