CN114368835A - Full autotrophic biological denitrification device and method - Google Patents
Full autotrophic biological denitrification device and method Download PDFInfo
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Abstract
The invention discloses a denitrification device and a denitrification method for total autotrophic organisms, wherein the denitrification device and the denitrification method adopt combined denitrification of denitrifying hydroxide bacteria and anaerobic ammonium oxidizing bacteria to convert ammonium radicals and nitrate radicals in wastewater into nitrogen, simultaneously deeply remove nitrate nitrogen and ammonia nitrogen in the wastewater, do not need to additionally add an organic carbon source, and are completely autotrophic, so that the energy consumption and the cost of denitrification are obviously reduced, the denitrification device can run for a long time, the total nitrogen of effluent of a bioreactor is less than or equal to 1mgN/L, and the water quality can reach the III-class standard of surface water.
Description
Technical Field
The invention relates to the technical field of biological denitrification, in particular to a full autotrophic biological denitrification device and a full autotrophic biological denitrification method.
Background
The existing biological denitrification of wastewater mainly adopts a nitrification-denitrification technology, firstly ammonium is oxidized into nitrite by aerobic ammonia oxidizing bacteria, then the nitrite is oxidized into nitrate by aerobic nitrite oxidizing bacteria, namely, the process of nitrosation and nitrification is carried out, then acetic acid, methanol and the like are introduced in a mode of additionally adding an organic carbon source, and the nitrate is reduced into nitrogen by denitrifying bacteria, namely, the process of denitrification is carried out. The nitrification process is an aerobic autotrophic process, the denitrification process is an anaerobic heterotrophic process, and the nitrification-denitrification technology generally has the problems of long process route, high energy consumption, additional organic carbon source, high cost and the like.
Anaerobic ammonia oxidation is a relatively energy-saving biological denitrification technology, and the principle is as follows: part of ammonium radicals are oxidized into nitrite by ammonia oxidizing bacteria, and then the nitrite and the rest of ammonium radicals are converted into nitrogen together under the catalysis of anaerobic ammonia oxidizing bacteria. In the actual operation process, measures such as dissolved oxygen and hydraulic retention time need to be controlled, so that the nitrification process only reaches the step of nitrite, and the nitrite is prevented from being further oxidized into nitrate. In addition, the actual wastewater usually contains a lot of nitrate nitrogen besides ammonia nitrogen, and the traditional anaerobic ammonia oxidation denitrification method cannot remove the nitrate nitrogen in the wastewater and cannot meet the denitrification requirement.
Disclosure of Invention
In order to solve the problems, the invention provides a full autotrophic biological denitrification device and a full autotrophic biological denitrification method.
The invention adopts the following technical scheme:
the utility model provides a full autotrophic biological denitrification device, includes bioreactor and gas generator, bioreactor is including intaking the end and going out the water end, bioreactor's inside packing has porous carrier, porous carrier is including the first reaction section and the second reaction section that adsorb corresponding denitrogenation microorganism respectively, gas generator is used for producing the mist and will the mist is leading-in the bioreactor.
Further, the denitrifying microorganisms comprise denitrifying hydroxide bacteria and anaerobic ammonium oxidation bacteria, the denitrifying hydroxide bacteria are adsorbed on a first reaction section of the porous carrier, and the anaerobic ammonium oxidation bacteria are adsorbed on a second reaction section of the porous carrier.
Further, a gas disperser is further arranged at the position, close to the water inlet, in the bioreactor and used for dispersing the mixed gas.
Further, the mixed gas contains hydrogen and carbon dioxide.
Further, the device also comprises a water pump, wherein the water pump is used for guiding the wastewater to be treated into the bioreactor from the water inlet end.
A denitrification method for total autotrophs comprises the following steps:
s1, filling a porous carrier in the bioreactor;
s2, respectively inoculating denitrifying hydroxide bacteria and anaerobic ammonium oxidation bacteria to a first reaction section and a second reaction section on the porous carrier;
s3, introducing mixed gas of hydrogen and carbon dioxide into the water inlet end of the bioreactor;
s4, introducing wastewater to be treated into the water inlet end of the bioreactor, circulating the wastewater, and changing the wastewater into continuous flow operation when the denitrifying bacteria hydroxide and the anaerobic ammonium oxidation bacteria in the porous carrier reach the biomass maximization;
and S5, gradually adjusting the flow of the wastewater according to the denitrification condition to control the retention time of the wastewater in the bioreactor until the denitrification efficiency is maximized.
Further, the porous carrier adopts any one or two of ceramics, diatomite, zeolite and fiber.
Further, the denitrifying hydroxide bacteria are pure denitrifying hydroxide bacteria or enrichment of the denitrifying hydroxide bacteria.
Furthermore, the anaerobic ammonia oxidizing bacteria adopt pure anaerobic ammonia oxidizing bacteria or enrichment of anaerobic ammonia oxidizing bacteria.
Further, the mixed gas of hydrogen and carbon dioxide is generated by any one of methanol pyrolysis, natural gas pyrolysis, biomass pyrolysis or mixing pure oxygen and pure carbon dioxide.
After adopting the technical scheme, compared with the background technology, the invention has the following advantages:
1. the invention provides a combined denitrification method by using denitrifying hydroxide bacteria and anaerobic ammonium oxidation bacteria aiming at the problem that wastewater simultaneously contains ammonia nitrogen and nitrate nitrogen, wherein the denitrifying hydroxide bacteria are used for converting the nitrate nitrogen into nitrite nitrogen, and then the anaerobic ammonium oxidation bacteria are used for converting the nitrite nitrogen and the ammonia nitrogen into nitrogen, so that the ammonia nitrogen and the nitrate nitrogen in the wastewater can be simultaneously and deeply removed to meet the denitrification requirement;
2. the mixed gas of hydrogen and carbon dioxide introduced into the bioreactor plays a role in removing oxygen in the bioreactor to provide an anaerobic environment, the carbon dioxide also serves as an inorganic carbon source of denitrifying hydroxide bacteria and anaerobic ammonium oxidation bacteria to provide energy, in addition, the denitrifying hydroxide bacteria contain catalase to oxidize hydrogen, and can oxidize the hydrogen to obtain energy for the growth of bacteria and reduce nitrate into nitrite, and the anaerobic ammonium oxidation bacteria further convert the nitrite generated in the last step and ammonia in wastewater into nitrogen, so that the denitrification method does not need to additionally add an organic carbon source and completely autotrophy, and the energy consumption and the cost of denitrification are obviously reduced;
3. the denitrifying bacteria hydroxide and the anaerobic ammonium oxidation bacteria are loaded on the porous material by adopting pure or high-purity enrichment, so that the effective interception of functional bacteria is realized, high denitrification rate can be realized when high-concentration and low-concentration nitrogen-containing wastewater is treated, the problem of poor denitrification effect due to low microorganism content in low-ammonia nitrogen wastewater is especially solved, the deep denitrification in a water body is realized, and the effluent quality through a bioreactor can reach the III-class standard of surface water;
4. the invention also provides a corresponding denitrification device which is simple in structure and easy to control, wherein two types of bacteria are simultaneously fixed in a bioreactor containing a porous carrier, and mixed gas of hydrogen and carbon dioxide is introduced into the bioreactor through a gas generator, so that the deep removal of nitrate nitrogen and ammonia nitrogen is simultaneously completed in one bioreactor, the device can run for a long time under the condition of not adding an organic carbon source, and the total nitrogen of effluent of the reactor is less than or equal to 1mg N/L.
Drawings
FIG. 1 is a schematic view of a denitrification apparatus according to the present invention;
FIG. 2 is a graph showing the trinitrogen concentration of the combined denitrification inlet and outlet water as a function of time in the fourth example;
FIG. 3 is a graph showing the time-dependent changes in the ammonia nitrogen and nitric acid nitrogen concentrations of inlet and outlet water of the nitration reaction in the fifth example;
FIG. 4 is a graph showing the time-dependent changes of the ammonia nitrogen and nitric acid nitrogen concentrations of the combined denitrification inlet and outlet water in the fifth embodiment.
Description of reference numerals:
1. a bioreactor; 11. a water inlet end; 111. a water inlet; 112. an air inlet; 12. a water outlet end; 121. a water outlet; 122. an air outlet; 13. a first sampling port; 14. a second sampling port;
2. a gas generator; 21. a gas flow meter; 22. a gas circulation pump;
3. a porous support; 31. a first reaction section; 32. a second reaction section;
4. a gas disperser;
5. a water pump;
6. and (5) collecting the gas.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is described in further detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
Example one
As shown in fig. 1, the fully autotrophic biological nitrogen removal device comprises a bioreactor 1 and a gas generator 2, wherein the bioreactor 1 comprises a water inlet end 11 and a water outlet end 12, the bioreactor 1 is filled with a porous carrier 3, the porous carrier 3 comprises a first reaction section 31 and a second reaction section 32, which are respectively adsorbed with corresponding nitrogen removal microorganisms, and the gas generator 2 is used for generating mixed gas and guiding the mixed gas into the bioreactor 1.
And a gas disperser 4 is also arranged at the position, close to the water inlet end 11, in the bioreactor 1, and the gas disperser 4 is used for dispersing the mixed gas. The side wall of the bioreactor 1 is provided with a first sampling port 13 and a second sampling port 14 at the first reaction section 31 and the second reaction section 32 respectively, and the first sampling port 13 and the second sampling port 14 are used for sampling and observing the water in the bioreactor 1 in real time. The water inlet end 11 of the bioreactor 1 is provided with a water inlet 111 and a gas inlet 112, and the water outlet end 12 is provided with a water outlet 121 and a gas outlet 122. The bioreactor 1 of this example was 10cm in diameter and 1m high.
The denitrifying microorganisms comprise denitrifying hydroxide bacteria and anaerobic ammonium oxidation bacteria, the denitrifying hydroxide bacteria are adsorbed on a first reaction section 31 on the porous carrier 3, and the anaerobic ammonium oxidation bacteria are adsorbed on a second reaction section 32 on the porous carrier 3.
The gas generator 2 of the present embodiment employs a hydrogen and carbon dioxide mixed generator, and the generated mixed gas contains hydrogen and carbon dioxide. A gas collection chamber 6 communicated with the gas outlet 122 is arranged at the water outlet end 12 of the bioreactor 1, and the gas collection chamber 6 is used for collecting excessive mixed gas in the bioreactor 1; a gas circulation pump 22 is provided between the gas generator 2 and the gas inlet 112, and the inlet of the gas circulation pump 22 is connected to both the gas generator 2 and the gas outlet 122 of the bioreactor 1 for circulating the excess mixed gas in the bioreactor 1. A gas flow meter 21 is further arranged between the gas circulation pump 22 and the gas inlet 112, and the flow rate of the mixed gas can be controlled by adjusting the switch of the gas flow meter 21.
The device also comprises a water pump 5, wherein the water pump 5 is used for guiding the wastewater to be treated into the bioreactor 1 from the water inlet end 11.
Example two
1. Screening of denitrifying bacteria
The source of the screened strain is sludge in a denitrification pool of a certain sewage treatment plant, and a proper amount of the strain to be screened is added into the prepared autotrophic denitrification culture medium. The autotrophic denitrification culture medium comprises the following components: KNO31g/L，NaHCO31.2g/L，KH2PO40.2 g/L. The culture was carried out in a closed manner using a 150mL anaerobic flask filled with 50mL of liquid and filled with excess hydrogen. Sampling daily to measure the change of nitrate concentration until the nitrate concentration is reduced to 0.5mgAnd (3) supplementing nitrate and hydrogen below N/L, transferring the bacterial liquid after supplementing nitrate twice, wherein the transfer amount is 20% (10mL), and the components of the culture medium are the same as those of the above. Repeating the steps for three times after the nitrate is completely reduced to nitrogen, and then obtaining pure species of the hydroxyl denitrifying bacteria by adopting an anaerobic agar plate coating method. The agar plate composition was as follows: KNO31g/L，NaHCO31.2g/L，KH2PO40.2g/L, peptone 0.1g/L, agar concentration 2%. The slab headspace was filled with hydrogen and sealed with a seal. After about three days, a single colony grew on the solid medium, and then spread on a new agar plate, and this was repeated three times. And selecting a single colony to a culture medium with peptone 1g/L, yeast powder 0.5g/L and NaCl 2 g/L. Shaking-culturing at 200rpm until OD600 is about 1.0, centrifuging the bacterial liquid at 2000g for 3min, washing with water, and centrifuging to obtain bacterial sludge. And (3) fixing the volume of the bacterial sludge in an autotrophic denitrification culture medium, performing sealed culture, and filling hydrogen in a bottle. The denitrification capacity was measured. 16S rDNA sequencing is carried out on the separated and purified bacteria, and the denitrifying bacteria belong to Thauera mechernichensis and have the purity of 99.95 percent.
2. Domestication and enrichment of anammox bacteria
The source of the screened strain is anaerobic sludge in an anaerobic pool of a certain sewage treatment plant. Adding a proper amount of anaerobic sludge into the prepared anaerobic ammonia oxidation culture medium. The anaerobic ammonia oxidation culture medium comprises the following components: NH (NH)4Cl 0.21g/L，NaNO20.36g/L，NaHCO31.2g/L，KH2PO40.2 g/L. The culture was carried out in a closed 150mL anaerobic flask filled with 120mL of liquid and filled with excess argon for removing oxygen from the water. Sampling every day to measure the concentration change of the ammonium radical and the nitrite radical, and measuring that the molar ratio of the removal amount of the ammonium radical to the nitrite radical is close to 1: 1.32, the acclimation of the anaerobic ammonium oxidation bacteria in the anaerobic sludge is successful. And when the content of ammonium radicals and nitrite radicals measured in the anaerobic bottle is lower than 0.5mg N/L, continuously supplementing the ammonium radicals, nitrite radicals and sodium bicarbonate into the bottle so as to supplement enough carbon sources and nitrogen sources for growth and reproduction of the anaerobic ammonium oxidation bacteria. After long-term culture, the high-purity enrichment anaerobic ammonium oxidation bacteria are obtained. 16S rDNA sequencing is carried out on the enriched bacteria, and the strain is detectedAnammox bacteria belong to the classification Candidatus Kuenenia, and the purity is 51.95%.
EXAMPLE III
Immobilizing biological carriers of denitrifying hydroxide bacteria and anaerobic ammonium oxidation bacteria:
the bioreactor of this example has a diameter of 10cm and a height of 100cm, and is filled with a ceramic porous material having a diameter of about 5mm, and the gap of the ceramic material is 60%.
The simulated wastewater contains ammonia nitrogen, nitrite nitrogen and nitrate nitrogen, and comprises the following specific components: NH (NH)4Cl 0.31g/L，NaNO20.35g/L，KNO30.5g/L，NaHCO31.2g/L，KH2PO40.2g/L。
The bottom of the bioreactor is provided with a gas disperser, and mixed gas of hydrogen and carbon dioxide generated by methanol cracking is introduced. The gas produced by methanol cracking comprises 70% of hydrogen and about 25% of carbon dioxide.
Respectively putting a proper amount of ceramic porous materials into the pure cultured Thauera mechernichensis denitrifying bacteria and the enriched and purified bacterial liquid of the anaerobic ammonium oxidation bacteria. Standing for five days to make the filler fully adsorb bacteria liquid, allowing the strains to enter the micron holes, and respectively adding inorganic carbon source and nitrogen source into the two culture bottles to make the strains continuously grow and enrich in the biological filler. Then respectively placing the ceramic porous materials with adsorbed strains in a reactor, and respectively placing the ceramic porous materials with adsorbed denitrifying bacteria hydroxide and the ceramic porous materials with adsorbed anaerobic ammonium oxidation bacteria in the first reaction section and the second reaction section. The bioreactor is filled with culture medium reactor bottom aeration hydrogen, which is circulated to maximize biomass in the porous carrier, and then continuous flow operation is changed, and the hydraulic retention time is gradually adjusted from large to small according to denitrification condition until the denitrification efficiency is maximized.
Example four
The embodiment utilizes the denitrifying bacteria hydroxide and the anaerobic ammonium oxidation bacteria to jointly treat the high ammonia nitrogen wastewater, and the high ammonia nitrogen wastewater is specifically aquaculture wastewater. The concentrations of ammonia nitrogen, nitrite nitrogen and nitrate nitrogen in the wastewater are respectively 50mg N/L, 5mg N/L,50mg N/L, COD concentration 100mg O2And L, storing the wastewater in a reservoir, and pumping the wastewater into a bioreactor through a water pump, wherein the diameter of the bioreactor is 10cm, the height of the bioreactor is 1m, and porous carriers are respectively arranged inside the bioreactor. Pure cultured Thauera mechernichensis hydroxide denitrifying bacteria, enriched high-purity anaerobic ammonium oxidation bacteria are respectively adsorbed on a first reaction section and a second reaction section on a porous carrier, a gas disperser is arranged at the bottom of a bioreactor, a gas generator is a hydrogen and carbon dioxide mixed generating device, and the flow of mixed gas is controlled to be about 20mL/min by a switch of a gas flowmeter. Maintaining dissolved oxygen < 2mg O in the bioreactor2And L. The water quality of the inlet water and the outlet water of the bioreactor changing along with time is shown in figure 2, after 30 days of operation, the ammonia nitrogen in the outlet water is 0.3mg N/L, the nitrite nitrogen is 0.1mg N/L, the nitrate nitrogen is 0.5mg N/L, the total nitrogen is less than or equal to 1mg N/L, and the three-nitrogen index reaches the standard of surface water III class.
EXAMPLE five
The embodiment utilizes the denitrifying bacteria hydroxide and the anaerobic ammonium oxidation bacteria to jointly treat the low ammonia nitrogen wastewater, and the low ammonia nitrogen wastewater is specifically similar to municipal sewage first-level B effluent, wherein the ammonia nitrogen concentration is 15mg N/L, and the nitrate concentration is 3mg N/L. If the conventional anaerobic ammonia oxidation denitrification technology is adopted, part of ammonia nitrogen needs to be oxidized into nitrite nitrogen by using aerobic Ammonia Oxidation Bacteria (AOB), but the AOB and Nitrite Oxidizing Bacteria (NOB) belong to aerobic bacteria, so that nitrite is further oxidized into nitrate. In the embodiment, part of ammonia nitrogen wastewater is oxidized into nitrate without limiting aeration, then the nitrate wastewater and the rest raw water are fed into a bioreactor together, dissolved oxygen is rapidly removed by an aeration gas mixture method, and the speed of reducing the nitrate into nitrite is controlled by a hydrogen gas control method. Because only ammonia nitrogen exists, part of the wastewater can be nitrified to generate the nitric acid nitrogen required by the invention. And (3) carrying out traditional nitrification treatment on part of wastewater to generate wastewater containing 15mg of N/L nitric acid nitrogen, mixing the nitrified wastewater and the original ammonia nitrogen wastewater to form ammonia nitrogen and nitric acid nitrogen wastewater, and enabling the ammonia nitrogen and nitric acid nitrogen wastewater to enter the denitrification device of the embodiment, wherein the other parts are the same as those in the fourth embodiment. The water quality of the water inlet and outlet of the traditional nitration reactor changing along with time is shown in figure 3, the water quality of the water inlet and outlet of the oxidation-denitrification and anaerobic ammonia oxidation reactor changing along with time is shown in figure 4, after 30 days of operation, the ammonia nitrogen in the water outlet is less than or equal to 0.3mg N/L, the nitrite nitrogen is less than or equal to 0.2mg N/L, the nitrate nitrogen is less than or equal to 0.5mg N/L, the total nitrogen is less than or equal to 1mg N/L, and the three-nitrogen index reaches the standard of surface water III.
The above description is only for the preferred embodiment of the present invention, but the scope of the present invention is not limited thereto, and any changes or substitutions that can be easily conceived by those skilled in the art within the technical scope of the present invention are included in the scope of the present invention. Therefore, the protection scope of the present invention shall be subject to the protection scope of the claims.
Claims (10)
1. A full autotrophic biological denitrification device is characterized in that: including bioreactor and gas generator, bioreactor includes into water end and play water end, bioreactor's inside is filled with porous carrier, porous carrier is including adsorbing first reaction section and the second reaction section that has corresponding denitrogenation microorganism respectively, gas generator is used for producing the mist and will the mist is leading-in the bioreactor.
2. The apparatus of claim 1, wherein: the denitrifying microorganisms comprise denitrifying hydroxide bacteria and anaerobic ammonium oxidation bacteria, the denitrifying hydroxide bacteria are adsorbed on a first reaction section on the porous carrier, and the anaerobic ammonium oxidation bacteria are adsorbed on a second reaction section on the porous carrier.
3. The completely autotrophic biological nitrogen removal device of claim 2, wherein: the bioreactor is characterized in that a gas disperser is further arranged at the position close to the water inlet end and used for dispersing the mixed gas.
4. The apparatus according to claim 3, wherein: the mixed gas contains hydrogen and carbon dioxide.
5. The apparatus according to claim 4, wherein: the bioreactor also comprises a water pump, wherein the water pump is used for guiding the wastewater to be treated into the bioreactor from the water inlet end.
6. The process according to any one of claims 1 to 5, wherein: the method comprises the following steps:
s1, filling a porous carrier in the bioreactor;
s2, respectively inoculating denitrifying hydroxide bacteria and anaerobic ammonium oxidation bacteria to a first reaction section and a second reaction section on the porous carrier;
s3, introducing mixed gas of hydrogen and carbon dioxide into the water inlet end of the bioreactor;
s4, introducing wastewater to be treated into the water inlet end of the bioreactor, circulating the wastewater, and changing the wastewater into continuous flow operation when the denitrifying bacteria hydroxide and the anaerobic ammonium oxidation bacteria in the porous carrier reach the biomass maximization;
and S5, gradually adjusting the flow of the wastewater according to the denitrification condition to control the retention time of the wastewater in the bioreactor until the denitrification efficiency is maximized.
7. The process of claim 6, wherein the total autotrophic nitrogen removal: the porous carrier adopts any one or two of ceramics, diatomite, zeolite and fiber.
8. The process of claim 7, wherein the total autotrophic nitrogen removal is: the denitrifying bacteria are pure denitrifying bacteria or the enrichment of the denitrifying bacteria.
9. The process of claim 7, wherein the total autotrophic nitrogen removal is: the anaerobic ammonium oxidation bacteria adopt pure anaerobic ammonium oxidation bacteria or enrichment of anaerobic ammonium oxidation bacteria.
10. The process of claim 6, wherein the total autotrophic nitrogen removal: the mixed gas of the hydrogen and the carbon dioxide is generated by any one of methanol pyrolysis, natural gas pyrolysis, biomass pyrolysis or mixing of pure oxygen and pure carbon dioxide.
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