CN102126789B - Method and device for removing nitrates from drinking water - Google Patents
Method and device for removing nitrates from drinking water Download PDFInfo
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- CN102126789B CN102126789B CN2010100101269A CN201010010126A CN102126789B CN 102126789 B CN102126789 B CN 102126789B CN 2010100101269 A CN2010100101269 A CN 2010100101269A CN 201010010126 A CN201010010126 A CN 201010010126A CN 102126789 B CN102126789 B CN 102126789B
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Abstract
The invention relates to environmental protection, in particular to a method and a device for removing nitrates from drinking water. The method comprises the following steps that: organic micromolecules generated by the anaerobic digestion of strains in an anaerobic fermentation unit permeate through a separating diffusion layer and are diffused to enter a denitrification unit to serve as a reducing agent for strains subjected to habituated culture in the denitrification unit, namely an electron donor source, wherein for 30 to 50 mg/L of NO3<->-N nitrates at the temperature of between 20 and 25 DEG C, water is cut for 24 to 36 hours; and voltage difference between the denitrification unit and the anaerobic fermentation unit forms microbial current through activated carbon fibers, and the microbial current is transmitted to the denitrification unit from the anaerobic fermentation unit to promote bio-electrochemical denitrification, so that heterotrophic denitrification and bio-electrochemical denitrification are synchronously and synergetically to remove the nitrates from the drinking water. By the method and the device, an electron dornor is prevented from being excessive, and the problem that the nitrates in the drinking water exceed the standard is solved economically and reliably. The method is suitable for removing the nitrates in the drinking water in large scale and is also suitable for the in-situ treatment of the nitrate pollution in a drinking water source.
Description
Technical field
The present invention relates to environment protection, specifically a kind of method and device thereof of removing Nitrate In Drinking Water.
Background technology
Excessive nitrogen and the Pollution from livestock and poultries etc. executed of agriculture production cause a lot of local tap water nitrate of China to exceed standard seriously.Drink the water that nitrate exceeds standard and directly endanger the healthy of baby and pregnant woman; Concerning general grownup, the water that long-term drinking nitrate exceeds standard can cause the generation of the various diseases such as cancer of the stomach.Therefore, it is great to solve the tap water nitrate question meaning that exceeds standard.
The method of removing Nitrate In Drinking Water mainly contains ion exchange method, reverse osmosis method, chemical method, biological denitrification method etc.Wherein ion-exchange, reverse osmosis method, cost is expensive, and the waste water that forms after processing can cause secondary pollution, is not suitable for removing on a large scale tap water nitrate.Chemical method, such as the iron powder reducing method, speed of reaction is wayward, and nitrate reduction is that nitrogen can produce ammonia simultaneously.
The biological denitrification method is considered to promise to be most the method for mass-producing processing drinking water azotate pollution.Tap water generally lacks nutrition source, and the biological denitrification method is removed nitrate need add an amount of reducing substances as electron donor.According to the difference of used reducing substances, biological denitrification is divided into heterotrophic denitrification and autotrophic denitrification.Heterotrophic denitrification is generally used methyl alcohol, and the small molecules such as acetic acid are as electron donor, and also available biodegradable macromole is such as cotton and wood fragments bits etc.Wherein, as electron donor, additive capacity and microorganism growth are wayward with small molecules such as methyl alcohol, need subsequent disposal, and running cost is high; The biodegradable macromole is generally made permeability anti-nitration reaction wall, and the original position that is used for groundwater azotate is removed.
The autotrophic denitrification method mainly adopts sulphur or hydrogen as electron donor.Remove nitrate with sulphur as the autotrophy source, cost is lower, but after sulphur is oxidized to sulfate radical, causes the water outlet sulphate content to increase, and pH descends.During as the autotrophy source, the security control of external source hydrogen supply requires high, generally adopts the electrolysis process hydrogen supply with hydrogen.But, hydrogen solubleness in water is little, and hydrogen utilization ratio is low.In order to overcome this problem, by regulating external source voltage, electronics is delivered on the electrode, allow be grown in electro-chemical activity denitrifying bacteria on the electrode and directly utilize hydrogen ion reduction nitrate (such as patent publication No. CN101381128A) in electronics and the water.In order to remedy the deficiency of single method, also available compounding method, such as autotrophic denitrification and electrochemical denitrifying compounding method (such as Granted publication CN 1162356C), heterotrophic denitrification and electrochemical denitrifying compounding method (such as Granted publication CN 1170780C).
Summary of the invention
The object of the invention is to provide a kind of method and device thereof of removing Nitrate In Drinking Water.
For achieving the above object, the technical solution used in the present invention is:
A kind of method of removing Nitrate In Drinking Water: the organic molecule that produces by bacterial classification anaerobic digestion in the anaerobically fermenting unit sees through the separation diffusion layer, diffuse into the denitrification unit, reductive agent as bacterial classification after domestication is cultivated in the denitrification unit is the electron donor source, at 20-25 ℃, to 30-50mg/LNO
3 --N nitrate, water stopping time 24-36 hour, the voltage difference between denitrification unit and the anaerobically fermenting unit then, form the microorganism electric current by active carbon fiber electrode, be passed to the denitrification unit from the anaerobically fermenting unit, promote biological electrochemical denitrification, and then make heterotrophic denitrification and biological electrochemical denitrification synchronous synergetic, remove the nitrate in the tap water.
The volume ratio 10 of described denitrification unit and anaerobically fermenting unit: 1-1: 1; It is the 2-5mm active carbon granule that particle diameter is filled in the denitrification unit, accounts for denitrification unit volume 25-75%; Particle diameter 2-5mm active carbon granule is filled in the anaerobically fermenting unit, accounts for anaerobically fermenting unit volume 30-90%; Separate diffusion bed thickness 1-10cm, be comprised of less than the artificial cotton of 0.1mm or quartz sand and nylon cloth quartz sand and penetrating grain diameter, porosity is at 20-80%.Tamed strain in the described anaerobically fermenting unit is inoculated in the anaerobically fermenting unit with active sludge, and adds the biodegradable macromole mixed solution of anaerobically fermenting unit volume 0.25-2.5%, is aided with simultaneously the acetic acid of 1-5mM; And the every 6-7 days fresh biodegradable macromole mixed solutions of ratio displacement with anaerobically fermenting unit volume 10-90% continue 18-21 days altogether, and are stand-by.Tamed strain in the described denitrification unit, the NO of interpolation 40-80mg/L in the denitrification unit
3 -N and/or NO
2 -N, 0.5-1mM acetic acid, and then cultivated bacterial classification 5-7 days; Then in the denitrification unit, add 40-80mg/L NO again
3 --N or NO
2 -N and then cultivating bacterial classification 10-14 days, stand-by.
Remove the device of Nitrate In Drinking Water method: comprise reactor body 13, separate diffusion layer 3, positive electrode 10 and negative potential 11, wherein separating diffusion layer 3 is installed in the reactor body 13, reactor body 13 is separated into denitrification unit 1 and anaerobic unit two portions about in the of 2, in denitrification unit 1 and interior being filled with respectively of anaerobic unit 2 fill grain, described positive electrode 10 and negative potential 11 lay respectively on the filling grain in denitrification unit 1 and the anaerobic unit 2; Be respectively equipped with the first water-in 4, the first water outlet 5, thief hatch 6 and venting port 7 on the described denitrification unit 1; Be respectively equipped with the second water-in 8 and the second water outlet 9 on the described anaerobic unit 2.
The first water-in 4 on the described denitrification unit 1 is positioned at the below of the first water outlet 5, and venting port is positioned at the top of denitrification unit 1; The second water-in 8 on the described anaerobically fermenting unit 2 is positioned at the below of the second water outlet 9.The volume ratio 10 of described denitrification unit 1 and anaerobically fermenting unit 2: 1-1: 1; Filling grain in the denitrification unit 1 is the active carbon granule of particle diameter 2-5mm, accounts for denitrification unit volume 25-75%; It is particle diameter 2-5mm active carbon granule that grain is filled in anaerobically fermenting unit 2, accounts for anaerobically fermenting unit volume 30-90%.Described separation diffusion bed thickness 1-10cm is comprised of less than the artificial cotton of 0.1mm or quartz sand and the nylon cloth of granularity 1.0-3.0mm quartz sand and the penetrating grain diameter of granularity 1.0-3.0mm, and porosity is at 20-80%.Be connected with varistor 12 between the described positive and negative electrode 10,11, variation range is at 5-500 ohm; The ratio of the surface-area of positive and negative electrode is 1: 5-5: 1.
The advantage that the present invention has:
1, the present invention is heterotrophic denitrification and the integrative coordinated operation of biological electrochemical denitrification, and then removes Nitrate In Drinking Water.
2, the inventive method is by anaerobic fermentation and acid production, and the basicity that denitrification produces does not generally need pH regulator can guarantee that denitrification carries out smoothly yet.
3, the inventive method has been avoided electron donor surplus and microorganism hypertrophy, reduces the subsequent disposal difficulty.
4, the inventive method adopts biological electrochemical denitrification to need not outer source current, removes Nitrate In Drinking Water.Adopt method of the present invention and treatment unit can avoid electron donor superfluous, economic and reliable ground solves the tap water nitrate problem that exceeds standard.The method is fit to mass-producing and removes tap water nitrate, also is fit to the in-situ treatment of drinking water resource azotate pollution.
Description of drawings
Fig. 1 is the treatment unit that the present invention removes the Nitrate In Drinking Water method.
Embodiment
Comprise as shown in Figure 1 reactor body 13 internal diameter 12.5cm, high 14cm, separation diffusion layer 3, positive electrode 10 and negative potential 11, wherein separating diffusion layer 3 is installed in the reactor body 13, reactor body 13 is separated into denitrification unit 1 and anaerobic unit two portions about in the of 2, in denitrification unit 1 and interior being filled with respectively of anaerobic unit 2 fill grain, described positive electrode 10 and negative potential 11 lay respectively on the filling grain in denitrification unit 1 and the anaerobic unit 2; Be respectively equipped with the first water-in 4, the first water outlet 5, thief hatch 6 and venting port 7 on the described denitrification unit 1; Be respectively equipped with the second water-in 8 and the second water outlet 9 on the described anaerobic unit 2.Intake-outlet lays respectively at the both sides of reactor body 13 axial cross sections; The first water-in 4 on the described denitrification unit 1 is positioned at the below of the first water outlet 5, and venting port is positioned at the top of denitrification unit 1; The second water-in 8 on the described anaerobically fermenting unit 2 is positioned at the below of the second water outlet 9.Be connected with varistor 12 between the described positive and negative electrode 10,11, variation range is at 0-500 ohm.
The volume ratio of described denitrification unit and anaerobically fermenting unit 1: 1; It is the 2-5mm active carbon granule that particle diameter is filled in the denitrification unit, accounts for denitrification unit volume 30%; Particle diameter 2-5mm active carbon granule is filled in the anaerobically fermenting unit, accounts for anaerobically fermenting unit volume 80%; Separate diffusion bed thickness 2cm, be made of quartz sand and the nylon cloth of granularity 1.0-3.0mm, porosity is 60%; The ratio of the surface-area of positive and negative electrode is 1: 1, and positive and negative electrode is activated carbon fiber, counterpoise 15g.Positive and negative electrode is connected with outer meeting resistance by the titanium silk.Interpolation concentration in anaerobically fermenting unit is 0.5% powdered rice hulls.
Treatment process: the tap water that contains nitrate flows to into the denitrification unit by denitrification unit water-in 4 upstream side.25 ℃, water inlet 0.61L, pH 7.0, dissolved oxygen 0.6mg/L, SODIUMNITRATE 30mg N/L cut off the water 24 hours, 20 ohm of outer meeting resistances.The organic molecule that the bacterial classification anaerobic digestion produces in the anaerobically fermenting unit sees through separates diffusion layer, diffuse into the denitrification unit, reductive agent as bacterial classification after domestication is cultivated in the denitrification unit is the electron donor source, the voltage difference between denitrification unit and the anaerobically fermenting unit then, form the microorganism electric current by active carbon fiber electrode, be passed to the denitrification unit from the anaerobically fermenting unit, promote biological electrochemical denitrification, and then make heterotrophic denitrification and biological electrochemical denitrification synchronous synergetic.The methane of the nitrogen that denitrification produces and the diffusion of anaerobically fermenting unit etc. is discharged by venting port 7.Containing the macromolecular mixed solution upstream side of biodegradable flows to into the anaerobically fermenting unit.Determine the mouth of a river and get water outlet, pH 7.2, NO
3 --N content 6.4mg N/L, NO
2 --N content＜0.01mg N/L, nitrate removal rate 79%.
Tamed strain in the described anaerobically fermenting unit is inoculated in the anaerobically fermenting unit with active sludge, and adds the biodegradable macromole mixed solution of 0.25-2.5%, is aided with simultaneously acetic acid and the trace element of 1-5mM; And the every 6-7 days fresh biodegradable macromole mixed solutions of ratio displacement with anaerobically fermenting unit volume 10-90% continue three Sunday altogether, and are stand-by.Tamed strain in the described denitrification unit, the NO of interpolation 40-80mg/L in the denitrification unit
3 -N and/or NO
2 -N, 0.5-1mM acetic acid and a small amount of trace element, and then cultivate one Sunday of bacterial classification; Then in the denitrification unit, add 40-80mg/L NO again
3 --N or NO
2 -N and then cultivating the bacterial classification fortnight, stand-by.Described biodegradable macromole is rice husk.When anaerobically fermenting unit and denitrification unit domesticated strain, can add in addition the conventional trace element that is applicable on a small quantity the anaerobic species growth.
Then in the treatment unit running, according to water stopping time and anaerobically fermenting unit biomacromolecule addition and the frequency of Nitrate In Drinking Water concentration to be removed and working temperature decision denitrification unit.At 20-25 ℃, to 30-50mg NO
3 --N/L nitrate, water stopping time 24-36 hour, the water outlet nitrate concentration was at 10mg NO
3 -Under-the N/L, clearance is between 65-85%.The anaerobically fermenting unit is according to working temperature, and the nitrate concentration of processing contained the biomacromolecule mixed solution of 0.25-2.5% in 15-60 days with the displacement of 10-90% ratio.Under the same nitrate concentration, temperature is high, and the adding proportion of anaerobically fermenting unit biomacromolecule suitably reduces, and time swap shortens.During the operation certain hour has been found denitrification unit enrichment other pollutent, can wash it, and imitative the unloading phase, add 0.2-1.0mM acetic acid in the former water and enter denitrification unit 1-3 time, the recovery of promotion denitrifying capacity.
Difference from Example 1 is: the volume ratio of described denitrification unit and anaerobically fermenting unit 2: 1; It is the 2-5mm active carbon granule that particle diameter is filled in the denitrification unit, accounts for denitrification unit volume 40%; Particle diameter 2-5mm active carbon granule is filled in the anaerobically fermenting unit, accounts for anaerobically fermenting unit volume 60%; Separate diffusion bed thickness 2cm, form porosity 60% by the quartz sand of granularity 1.0-3.0mm and penetrating grain diameter less than the artificial cotton of 0.1mm; The ratio of the surface-area of positive and negative electrode is 2: 1, and positive and negative electrode is activated carbon fiber, weighs respectively 20 and 10g.Positive and negative electrode is connected with outer meeting resistance by the titanium silk.It is 0.75% that anaerobically fermenting unit powdered rice hulls adds concentration.Pending tap water 0.61L, pH 7.0, dissolved oxygen 0.6mg/L, SODIUMNITRATE 40mg N/L, cut off the water 5 ohm of outer meeting resistances 24 hours by 25 ℃.Record water outlet pH 7.3, NO
3 --N content 7.9mg N/L, NO
2 --N content＜0.01mg N/L.Nitrate removal rate 80%.
Difference from Example 1 is: the volume ratio of described denitrification unit and anaerobically fermenting unit 3: 1; It is the 2-5mm active carbon granule that particle diameter is filled in the denitrification unit, accounts for denitrification unit volume 50%; Particle diameter 2-5mm active carbon granule is filled in the anaerobically fermenting unit, accounts for anaerobically fermenting unit volume 60%; Separate diffusion bed thickness 3cm, consist of porosity 70% by the quartz sand of granularity 1.0-3.0mm and penetrating grain diameter less than the artificial cotton of 0.1mm; The ratio of the surface-area of positive and negative electrode is that 2: 1 positive and negative electrodes are activated carbon fiber, weighs respectively 20 and 10g.Positive and negative electrode is connected with outer meeting resistance by the titanium silk.It is 1.0% that anaerobically fermenting unit powdered rice hulls adds concentration.Pending tap water 0.61L, pH 7.0, dissolved oxygen 0.6mg/L, SODIUMNITRATE 50mg N/L, cut off the water 10 ohm of outer meeting resistances 36 hours by 25 ℃.Record water outlet pH 7.4, NO
3 --N content 7.3mg N/L, NO
2 --N content＜0.01mg N/L.Nitrate removal rate 85%.
Claims (9)
1. method of removing Nitrate In Drinking Water, it is characterized in that: the organic molecule that produces by bacterial classification anaerobic digestion in the anaerobically fermenting unit sees through the separation diffusion layer, diffuse into the denitrification unit, reductive agent as bacterial classification after domestication is cultivated in the denitrification unit is the electron donor source, at 20-25 ℃, to 30-50mg/L NO
3 --N nitrate, water stopping time 24-36 hour, the voltage difference between denitrification unit and the anaerobically fermenting unit then, form the microorganism electric current by active carbon fiber electrode, be passed to the denitrification unit from the anaerobically fermenting unit, promote biological electrochemical denitrification, and then make heterotrophic denitrification and biological electrochemical denitrification synchronous synergetic, remove the nitrate in the tap water.
2. by the method for removal Nitrate In Drinking Water claimed in claim 1, it is characterized in that: the volume ratio 10 of described denitrification unit and anaerobically fermenting unit: 1-1: 1; It is the 2-5mm active carbon granule that particle diameter is filled in the denitrification unit, accounts for denitrification unit volume 25-75%; Particle diameter 2-5mm active carbon granule is filled in the anaerobically fermenting unit, accounts for anaerobically fermenting unit volume 30-90%; Separate diffusion bed thickness 1-10cm, be comprised of quartz sand and artificial cotton or quartz sand and nylon cloth, porosity is at 20-80%.
3. press the method for removal Nitrate In Drinking Water claimed in claim 1, it is characterized in that: tamed strain in the described anaerobically fermenting unit, active sludge is inoculated in the anaerobically fermenting unit, and add the biodegradable macromole mixed solution of anaerobically fermenting unit volume 0.25-2.5%, be aided with simultaneously the acetic acid of 1-5mM; And the every 6-7 days fresh biodegradable macromole mixed solutions of ratio displacement with anaerobically fermenting unit volume 10-90% continue 18-21 days altogether, and are stand-by.
4. by the method for removal Nitrate In Drinking Water claimed in claim 1, it is characterized in that: tamed strain in the described denitrification unit, the NO of interpolation 40-80mg/L in the denitrification unit
3 -N and/or NO
2 -N, 0.5-1mM acetic acid, and then cultivated bacterial classification 5-7 days; Then in the denitrification unit, add 40-80mg/L NO again
3 --N or NO
2 -N and then cultivating bacterial classification 10-14 days, stand-by.
5. device by removal Nitrate In Drinking Water method claimed in claim 1, it is characterized in that: comprise reactor body (13), separate diffusion layer (3), positive electrode (10) and negative potential (11), wherein separating diffusion layer (3) is installed in the reactor body (13), reactor body (13) is separated into up and down two portions of denitrification unit (1) and anaerobic unit (2), be filled with respectively in denitrification unit (1) and anaerobic unit (2) and fill grain, described positive electrode (10) and negative potential (11) lay respectively on the interior filling grain of denitrification unit (1) and anaerobic unit (2); Be respectively equipped with the first water-in (4), the first water outlet (5), thief hatch (6) and venting port (7) on the described denitrification unit (1); Be respectively equipped with the second water-in (8) and the second water outlet (9) on the described anaerobic unit (2).
6. by device claimed in claim 5, it is characterized in that: the first water-in (4) on the described denitrification unit (1) is positioned at the below of the first water outlet (5), and venting port is positioned at the top of denitrification unit (1); The second water-in (8) on the described anaerobically fermenting unit (2) is positioned at the below of the second water outlet (9).
7. by device claimed in claim 6, it is characterized in that: the volume ratio 10 of described denitrification unit (1) and anaerobically fermenting unit (2): 1-1: 1; Filling grain in the denitrification unit (1) is the active carbon granule of particle diameter 2-5mm, accounts for denitrification unit volume 25-75%; It is particle diameter 2-5mm active carbon granule that grain is filled in anaerobically fermenting unit (2), accounts for anaerobically fermenting unit volume 30-90%.
8. by device claimed in claim 6, it is characterized in that: described separation diffusion bed thickness 1-10cm, formed by the quartz sand of granularity 1.0-3.0mm and quartz sand and the nylon cloth of artificial cotton or granularity 1.0-3.0mm, porosity is at 20-80%.
9. by device claimed in claim 6, it is characterized in that: be connected with varistor (12) between described positive and negative electrode (10), (11), variation range is at 5-500 ohm; The ratio of the surface-area of positive and negative electrode is 1: 5-5: 1.
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| CN102515453B (en) * | 2011-11-22 | 2013-04-24 | 中国科学院沈阳应用生态研究所 | High-concentration anaerobic digestion treating device for urban sludge and use method |
| CN104556385B (en) * | 2015-01-29 | 2016-06-15 | 哈尔滨工业大学 | Integrated mobile sanitary wastewater purifies and resource recovery device and method |
| WO2023184491A1 (en) * | 2022-04-01 | 2023-10-05 | 中山大学 | Denitrification strengthening method and device |
| CN114716015B (en) * | 2022-04-01 | 2022-12-27 | 中山大学 | Method and device for enhanced denitrification |
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