CN1354143A - Method for simultaneously removing nitrogen and phosphorus in wastewater - Google Patents
Method for simultaneously removing nitrogen and phosphorus in wastewater Download PDFInfo
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- CN1354143A CN1354143A CN01121824A CN01121824A CN1354143A CN 1354143 A CN1354143 A CN 1354143A CN 01121824 A CN01121824 A CN 01121824A CN 01121824 A CN01121824 A CN 01121824A CN 1354143 A CN1354143 A CN 1354143A
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- denitrification
- sulfur
- wastewater
- phosphorus
- heterotrophic
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- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 title claims abstract description 102
- 229910052757 nitrogen Inorganic materials 0.000 title claims abstract description 51
- 238000000034 method Methods 0.000 title claims abstract description 34
- 239000002351 wastewater Substances 0.000 title claims abstract description 32
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 title claims abstract description 27
- 229910052698 phosphorus Inorganic materials 0.000 title claims abstract description 27
- 239000011574 phosphorus Substances 0.000 title claims abstract description 27
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 claims abstract description 53
- 229910052717 sulfur Inorganic materials 0.000 claims abstract description 49
- 239000011593 sulfur Substances 0.000 claims abstract description 49
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 30
- 230000001651 autotrophic effect Effects 0.000 claims abstract description 30
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 30
- 229910000831 Steel Inorganic materials 0.000 claims abstract description 19
- 239000002893 slag Substances 0.000 claims abstract description 19
- 239000010959 steel Substances 0.000 claims abstract description 19
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims description 90
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 50
- 238000004065 wastewater treatment Methods 0.000 claims description 7
- 239000000203 mixture Substances 0.000 claims description 6
- QTBSBXVTEAMEQO-UHFFFAOYSA-M Acetate Chemical compound CC([O-])=O QTBSBXVTEAMEQO-UHFFFAOYSA-M 0.000 claims description 4
- 239000008187 granular material Substances 0.000 claims 1
- 244000005700 microbiome Species 0.000 abstract description 28
- 241000894006 Bacteria Species 0.000 abstract description 21
- 239000005416 organic matter Substances 0.000 abstract description 14
- 239000002245 particle Substances 0.000 abstract description 11
- 239000011575 calcium Substances 0.000 abstract description 10
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 abstract description 10
- -1 hydrogen ions Chemical class 0.000 abstract description 8
- BHPQYMZQTOCNFJ-UHFFFAOYSA-N Calcium cation Chemical compound [Ca+2] BHPQYMZQTOCNFJ-UHFFFAOYSA-N 0.000 abstract description 7
- 229910001424 calcium ion Inorganic materials 0.000 abstract description 7
- 229910052739 hydrogen Inorganic materials 0.000 abstract description 7
- 239000001257 hydrogen Substances 0.000 abstract description 7
- 239000007787 solid Substances 0.000 abstract description 7
- 238000001556 precipitation Methods 0.000 abstract description 6
- 230000000694 effects Effects 0.000 abstract description 4
- 230000001502 supplementing effect Effects 0.000 abstract description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 abstract description 2
- 229910052760 oxygen Inorganic materials 0.000 abstract description 2
- 239000001301 oxygen Substances 0.000 abstract description 2
- 229910002651 NO3 Inorganic materials 0.000 description 21
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 21
- 238000006243 chemical reaction Methods 0.000 description 20
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 17
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical compound [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 description 11
- 238000004519 manufacturing process Methods 0.000 description 8
- 229910000019 calcium carbonate Inorganic materials 0.000 description 6
- 230000000813 microbial effect Effects 0.000 description 6
- 239000000126 substance Substances 0.000 description 6
- 239000005864 Sulphur Substances 0.000 description 5
- 239000000463 material Substances 0.000 description 5
- 230000003647 oxidation Effects 0.000 description 5
- 238000007254 oxidation reaction Methods 0.000 description 5
- ODINCKMPIJJUCX-UHFFFAOYSA-N Calcium oxide Chemical compound [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 description 4
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 4
- 230000008901 benefit Effects 0.000 description 4
- 230000007423 decrease Effects 0.000 description 4
- 150000002894 organic compounds Chemical class 0.000 description 4
- 150000003464 sulfur compounds Chemical class 0.000 description 4
- 238000011144 upstream manufacturing Methods 0.000 description 4
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 3
- 235000019738 Limestone Nutrition 0.000 description 3
- IOVCWXUNBOPUCH-UHFFFAOYSA-M Nitrite anion Chemical compound [O-]N=O IOVCWXUNBOPUCH-UHFFFAOYSA-M 0.000 description 3
- 229910019142 PO4 Inorganic materials 0.000 description 3
- 230000015572 biosynthetic process Effects 0.000 description 3
- BRPQOXSCLDDYGP-UHFFFAOYSA-N calcium oxide Chemical compound [O-2].[Ca+2] BRPQOXSCLDDYGP-UHFFFAOYSA-N 0.000 description 3
- 239000000292 calcium oxide Substances 0.000 description 3
- 239000003651 drinking water Substances 0.000 description 3
- 235000020188 drinking water Nutrition 0.000 description 3
- 238000002474 experimental method Methods 0.000 description 3
- 239000006028 limestone Substances 0.000 description 3
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 2
- 230000006978 adaptation Effects 0.000 description 2
- 238000011001 backwashing Methods 0.000 description 2
- 239000002585 base Substances 0.000 description 2
- 238000009388 chemical precipitation Methods 0.000 description 2
- 239000003795 chemical substances by application Substances 0.000 description 2
- 230000006378 damage Effects 0.000 description 2
- 238000000354 decomposition reaction Methods 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- 244000144972 livestock Species 0.000 description 2
- 230000014759 maintenance of location Effects 0.000 description 2
- 150000002823 nitrates Chemical class 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- 239000008188 pellet Substances 0.000 description 2
- 239000012466 permeate Substances 0.000 description 2
- 239000004576 sand Substances 0.000 description 2
- 238000010998 test method Methods 0.000 description 2
- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonia chloride Chemical compound [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 description 1
- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 description 1
- JVMRPSJZNHXORP-UHFFFAOYSA-N ON=O.ON=O.ON=O.N Chemical compound ON=O.ON=O.ON=O.N JVMRPSJZNHXORP-UHFFFAOYSA-N 0.000 description 1
- ATOZNTAYMWIJTD-UHFFFAOYSA-N ON=O.ON=O.ON=O.P Chemical compound ON=O.ON=O.ON=O.P ATOZNTAYMWIJTD-UHFFFAOYSA-N 0.000 description 1
- 241001057811 Paracoccus <mealybug> Species 0.000 description 1
- 241001478304 Paracoccus versutus Species 0.000 description 1
- 241000605118 Thiobacillus Species 0.000 description 1
- 241000605261 Thiomicrospira Species 0.000 description 1
- 241000605264 Thiomicrospira thyasirae Species 0.000 description 1
- 208000034699 Vitreous floaters Diseases 0.000 description 1
- MRRWPCWICIRLDJ-UHFFFAOYSA-N [S].CCO Chemical compound [S].CCO MRRWPCWICIRLDJ-UHFFFAOYSA-N 0.000 description 1
- QFHYHYSMAHUARD-UHFFFAOYSA-N [S].CO Chemical compound [S].CO QFHYHYSMAHUARD-UHFFFAOYSA-N 0.000 description 1
- 230000002378 acidificating effect Effects 0.000 description 1
- 239000004480 active ingredient Substances 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 238000010170 biological method Methods 0.000 description 1
- 230000033228 biological regulation Effects 0.000 description 1
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- 238000004364 calculation method Methods 0.000 description 1
- 229910052681 coesite Inorganic materials 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 229910052593 corundum Inorganic materials 0.000 description 1
- 229910052906 cristobalite Inorganic materials 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 230000006735 deficit Effects 0.000 description 1
- 229910001873 dinitrogen Inorganic materials 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
- 229910052564 epsomite Inorganic materials 0.000 description 1
- 239000004744 fabric Substances 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- 239000000945 filler Substances 0.000 description 1
- 229910000037 hydrogen sulfide Inorganic materials 0.000 description 1
- 229910052588 hydroxylapatite Inorganic materials 0.000 description 1
- 239000010842 industrial wastewater Substances 0.000 description 1
- 239000002917 insecticide Substances 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 239000010985 leather Substances 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 239000008239 natural water Substances 0.000 description 1
- 230000007935 neutral effect Effects 0.000 description 1
- 238000006386 neutralization reaction Methods 0.000 description 1
- 230000003472 neutralizing effect Effects 0.000 description 1
- 238000006396 nitration reaction Methods 0.000 description 1
- 239000000618 nitrogen fertilizer Substances 0.000 description 1
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 1
- 235000015097 nutrients Nutrition 0.000 description 1
- XYJRXVWERLGGKC-UHFFFAOYSA-D pentacalcium;hydroxide;triphosphate Chemical compound [OH-].[Ca+2].[Ca+2].[Ca+2].[Ca+2].[Ca+2].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O XYJRXVWERLGGKC-UHFFFAOYSA-D 0.000 description 1
- 235000021317 phosphate Nutrition 0.000 description 1
- 239000002686 phosphate fertilizer Substances 0.000 description 1
- 150000003013 phosphoric acid derivatives Chemical class 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 239000011435 rock Substances 0.000 description 1
- 238000009287 sand filtration Methods 0.000 description 1
- 239000013535 sea water Substances 0.000 description 1
- 239000010865 sewage Substances 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 239000010802 sludge Substances 0.000 description 1
- UIIMBOGNXHQVGW-UHFFFAOYSA-M sodium bicarbonate Substances [Na+].OC([O-])=O UIIMBOGNXHQVGW-UHFFFAOYSA-M 0.000 description 1
- 229910000030 sodium bicarbonate Inorganic materials 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 241000894007 species Species 0.000 description 1
- 230000006641 stabilisation Effects 0.000 description 1
- 238000011105 stabilization Methods 0.000 description 1
- 229910052682 stishovite Inorganic materials 0.000 description 1
- 150000004763 sulfides Chemical class 0.000 description 1
- 239000013589 supplement Substances 0.000 description 1
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- 239000010409 thin film Substances 0.000 description 1
- 150000004764 thiosulfuric acid derivatives Chemical class 0.000 description 1
- 229910021654 trace metal Inorganic materials 0.000 description 1
- 229910052905 tridymite Inorganic materials 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
- 239000002023 wood Substances 0.000 description 1
- 229910001845 yogo sapphire Inorganic materials 0.000 description 1
Images
Classifications
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/02—Aerobic processes
- C02F3/12—Activated sludge processes
- C02F3/1205—Particular type of activated sludge processes
- C02F3/1215—Combinations of activated sludge treatment with precipitation, flocculation, coagulation and separation of phosphates
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/30—Aerobic and anaerobic processes
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/02—Aerobic processes
- C02F3/10—Packings; Fillings; Grids
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/30—Aerobic and anaerobic processes
- C02F3/302—Nitrification and denitrification treatment
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/34—Biological treatment of water, waste water, or sewage characterised by the microorganisms used
- C02F3/345—Biological treatment of water, waste water, or sewage characterised by the microorganisms used for biological oxidation or reduction of sulfur compounds
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/66—Treatment of water, waste water, or sewage by neutralisation; pH adjustment
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W10/00—Technologies for wastewater treatment
- Y02W10/10—Biological treatment of water, waste water, or sewage
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- Life Sciences & Earth Sciences (AREA)
- Chemical & Material Sciences (AREA)
- Microbiology (AREA)
- Water Supply & Treatment (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Hydrology & Water Resources (AREA)
- Biodiversity & Conservation Biology (AREA)
- Organic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- Molecular Biology (AREA)
- Analytical Chemistry (AREA)
- Purification Treatments By Anaerobic Or Anaerobic And Aerobic Bacteria Or Animals (AREA)
- Biological Treatment Of Waste Water (AREA)
Abstract
The present invention relates to a method for simultaneously removing nitrogen and phosphorus from wastewater, which comprises 1) completely utilizing facultative photoautotrophic bacteria fully grown in organic matter in chemotrophic inorganic autotrophic anammox microorganisms while simultaneously performing facultative chemotrophic, heterotrophic and obligatory inorganic autotrophic anammox by supplying a small amount (required amount for heterotrophic denitrification 1/3-1/2) of external carbon source, 2) using shells or steel slag together with sulfur particles, wherein (1) the sulfur particles are used as a solid medium on which electron donors and denitrification sulfur bacteria can grow, and (2) the shells serve as a solid medium for maintaining pH at 7-8 by supplementing alkalinity when pH is further lowered by hydrogen ions generated by denitrification of sulfur, while maintaining activity of the anammox microorganisms and providing the chemotrophic inorganic autotrophic bacteria with inorganic ionsCarbon source (CO)2) And 3) calcium ion (Ca) in water generated from shell or steel slag2+) Phosphorus is simultaneously removed by precipitation in the presence of oxygen.
Description
Background
Technical Field
The invention relates to a method for removing nitrogen and phosphorus in wastewater simultaneously, which comprises the following steps:
1) the facultative aerobionts fully growing in organic matters in the chemolithoautotrophic denitrification microorganisms are completely utilized to supply a small amount (1/3-1/2 of the required amount of heterotrophic denitrification) of external carbon sources to simultaneously carry out facultative aerobiont, heterotrophic and obligate aerobiont denitrification;
2) shells or steel slag are used together with sulfur particles, wherein (1) the sulfur particles are used as an electron donor and a solid medium on which a sulfur denitrifying agent can grow, and (2) as a solid medium, the shells play a role of maintaining the pH at 7-8 by supplementing alkalinity when the pH is further lowered by hydrogen ions generated by sulfur denitrification, while maintaining the activity of denitrifying microorganisms and providing an inorganic carbon source (CO) for chemolithoautotrophic organisms2) (ii) a And
3) calcium ion (Ca) in water generated from shell or steel slag2+) Phosphorus is simultaneously removed by precipitation in the presence of oxygen.
Biological denitrification has been successfully used to remove nitrogen from wastewater. Typically, an autotrophic or heterotrophic denitrification system is used. By providing a sufficient amount of organic carbon, heterotrophic denitrification can be very effective in removing nitrate, which can be divided into two processes depending on the location of the anoxic tank: denitrogenation and post-denitrogenation. Denitrification is a cost-effective method of utilizing organic matter in wastewater without adding an external carbon source when organic carbon in wastewater is sufficient relative to nitrogen, and has a structure consisting of an anaerobic tank, an anoxic tank after an oxidation tank (aerobic tank), and a precipitation tank in this order. The denitrification reaction and the organic decomposition are mainly carried by the anaerobic tank, and the organic decomposition and the nitration are also carried out in the oxidation tank. And the nitrified wastewater in the oxidation tank is returned to the anoxic tank for denitrification.
According to the post-heterotrophic denitrification process, it is difficult to accurately control the addition of the expensive external carbon source sufficient to completely remove the nitrate (electron acceptor) and the external carbon source (electron donor); in addition, there is a need to establish a means to monitor nitrogen and another automated system to accurately add an external carbon source sufficient to remove nitrate and external organic carbon. If the external carbon source added exceeds the required amount for the heterotrophic process, the external carbon source present in the effluent is treated again.
Heterotrophic denitrification is a reaction performed by heterotrophic microorganisms that use organic matter as an electron donor to reduce nitrogen, in the form of nitrate or nitrite, to nitrogen gas under anaerobic conditions. However, since various industrial wastewaters generated from nitrogen/phosphate fertilizer production, multi-layer wood production, insecticide production and leather production and seepage water in land fills have low organic carbon concentrations as compared with nitrogen, denitrification after heterotrophic culture requires the use of some very expensive organic matter such as methanol or acetic acid to reduce nitrates. In the case of treating a large amount of wastewater, the required organic matter treatment cost is high.
For this reason, many studies have been made on the inorganic autotrophic nitrogen removal method using the chemo-energy of sulfur. Although there is a remarkable denitrification efficiency in terms of economy and stabilization of the treatment process, it has been recognized that the disadvantage of this method is that hydrogen ions generated during denitrification destroy alkalinity to cause a decrease in pH. Reduction of 1mg of nitrogen to 5mg of calcium carbonate (CaCO) during denitrification of chemolithoautotrophic organisms3). The optimum pH for most denitrifiers is reported to be between 7 and 8. In this regard, it is important to provide alkalinity to maintain the pH in the neutral range (7-8). Conventional methods have disclosed that limestone can be used in the tank to provide alkalinity along with the sulfur. However, in the case of wastewater having a high nitrogen concentration such as permeate water, plant wastewater and livestock wastewater, since CaCO3The dissolution rate is limited and limestone alone does not provide sufficient alkalinity.
The use of sulfur autotrophic treatment of high concentrations of nitrates results in the production of high concentrations of sulfate by-products. The official regulations on discharged water in korea so far have not controlled sulfate ions, but they are defined as an examination substance in a drinking water test method. The korean drinking water quality test method stipulates that the sulfate ion content does not exceed 200ppm, and WHO has defined it as 400 ppm. High concentrations of sulfate ions in drinking water are reported to produce sweetness, but very high concentrations are likely to corrode pipes.
Since a sufficient amount of sulfate ions (on average 2700mg/L) is present in natural water such as seawater, the amount of sulfate ions in the effluent waste produced by the system can be disregarded unless wastewater with an extremely high nitrate concentration is treated. If a high concentration of sulfate ions is discharged into the polluted river water during the treatment of a high concentration of nitrate type nitrogen, hydrogen sulfide (H) may be caused2S) to generate odor. Therefore, formation of sulfate ions is preferably prevented. In addition, the microorganisms are inorganically autotrophic denitrogenated due to chemical energyThe growth rate (Y) is small, and it is difficult to start adapting to the environment, and the time required is long. In addition, since the surface of the sulfur particles is composed of hard, non-porous spheres, the small binding sites for the microorganisms may cause a decrease in the initial denitrification efficiency unless a large amount of autotrophic microorganisms is added to the reactor.
At present, the content of nitrogen and phosphorus is strictly regulated by the wastewater discharge quality standard. Since the Korean government planned to set the T-N and T-P contents in the wastewater treatment facilities to 20mg/L and 2mg/L, respectively, from 2002, it was said that proper treatment of nitrogen and phosphorus was inevitable.
In general, useful biological methods for the simultaneous removal of nitrogen and phosphorus include A2The modified Bardenpho method, the UCT (university of Cape Town) method and the VIP (Virginia Initiative plant) method. However, since the above method relies entirely on heterotrophic denitrifying microorganisms, its practical application has not been widely used for wastewater having a low C/N ratio. In the conventional wastewater treatment method only for dephosphorization, chemical precipitation is mainly used, but the chemical cost is high and a lot of dirt is generated.
Summary of The Invention
To overcome the above-mentioned disadvantages such as destruction of alkalinity, sulfate radicals (SO)4 2-) The formation and operation of (A) is started with difficulty in adaptation of the microorganism to the environment, and the present inventors have conducted intensive studies. KR2000-60398, which was filed by the present inventors, discloses an inorganic autotrophic nitrogen removal method using energy of sulfur, which is superior to the heterotrophic nitrogen removal method, and which can achieve a more stable treatment efficiency against temporary impact load with economic advantage without the need for an external carbon source.
The invention relates to an improved method for KR2000-60398, which aims to change the traditional sulfur-containing denitrification tank. More specifically, the object of the present invention is to simultaneously conduct facultative photoautotrophic, heterotrophic and obligatory photoautotrophic denitrification by supplying a small amount (required amount for heterotrophic denitrification 1/3-1/2) of an external carbon source while supplementing some alkalinity with seashells or steel slag and generating calcium ions (Ca) in the water produced by the seashells or steel slag2+) Dephosphorization is carried out simultaneously by chemical precipitation in the presence of phosphorus. Thus, the present invention has been completed.
Accordingly, it is an object of the present invention to provide a denitrification method for simultaneously performing facultative photoautotrophic, heterotrophic, and obligatory photoautotrophic denitrification by supplying a small amount (required amount for heterotrophic denitrification 1/3-1/2) of an external carbon source.
Another object of the present invention is to provide a method for supplementing insufficient alkalinity in the denitrification process of sulfur by adding shells or steel slag and simultaneously dephosphorizing.
Brief Description of Drawings
FIG. 1a is a cross-sectional view of an upstream tank for use in the simultaneous removal of nitrogen nitrite and phosphorus in accordance with the present invention.
FIG. 1b is a cross-sectional view of a downstream tank for use in the simultaneous removal of nitrogen and phosphorus nitrite of the present invention.
FIG. 2 shows the heterotrophic and chemolithoautotrophic denitrification efficiency as a function of methanol addition.
FIG. 3 shows the heterotrophic and chemolithoautotrophic denitrification efficiency as a function of ethanol addition.
FIG. 4 shows the formation of sulfate ions as a function of methanol and ethanol addition.
Figure 5 shows the pH of the fired and dried shells as a function of time.
Explanation of main numbering in the drawings
1: sulfur and shell (or steel slag)
2: backwashing
3: sulfur-containing denitrification tank
4: sand filter tank
5: external carbon source (methanol, ethanol, acetate, etc.)
6: pump and method of operating the same
10: upstream tank
20: downstream trough
Detailed Description
The invention features a method for the simultaneous removal of nitrogen and phosphorus from wastewater, wherein the wastewater treatment is such that: sulfur particles and a small amount (required amount for heterotrophic denitrification, 1/3-1/2) of an external carbon source are added to a sulfur-containing denitrification tank to simultaneously perform obligatory inorganic autotrophic denitrification, facultative inorganic autotrophic denitrification and heterotrophic denitrification, and the loss of alkalinity and dephosphorization are supplemented by simultaneously adding shells or steel slag.
The present invention is explained in more detail below.
The invention relates to a post-denitrification process, wherein an anoxic tank is positioned behind a nitrification tank. Sulfur can be used as an electron donor and carrier in sulfur-containing denitrification tanks. And adding a certain proportion of shells or steel slag as an alkali source into the tank. In addition, facultative photoautotrophic, heterotrophic, and obligatory photoautotrophic denitrification is performed simultaneously by supplying a small amount (required for heterotrophic denitrification 1/3-1/2) of an external carbon source to the inlet stream.
With regard to microbiology, bacteria capable of oxidizing and reducing sulfur compounds such as sulfides, sulfur or thiosulfates can be physiologically classified into four groups: obligate inorganic autotrophic bacteria, facultative inorganic autotrophic bacteria, chemoenergetic inorganic heterotrophic bacteria, and heterotrophic bacteria. Obligate inorganic autotrophic bacteria capable of denitrification, such as Thiobacillus densificans and Thiomicrospira densificans, are practically limited to autotrophic growth modes, since they do not obtain energy from the oxidation of organic compounds and only have limited use of organic compounds. In contrast, facultative aerobically autotrophic anammox bacteria such as Thiobacillus versutus, Thiobacillus thyasiris, Thiosphaerapantopha and Paracoccus denitificans can grow heterotrophically, not only using reduced sulfur compounds as an energy source, but also. Thus, it is clear that these bacteria can adapt to different environments (i.e., autotrophic, heterotrophic, or mixotrophic conditions). Table 1: physiological type definition of bacteria capable of oxidizing reduced sulfur compounds
| Type (B) | Carbon (C)Source | Energy source | ||
| Inorganic substance | Organic compounds | Inorganic substance | Organic compounds | |
| Specific inorganic self Culture of bacteriaA | + | - | + | - |
| Facultative inorganic self Culture of bacteriaB | + | + | + | |
| Energy-conversion inorganic heterotrophic bacteria | - | + | + | |
| Heterotrophic bacteria | - | + | + | |
| Synonyms:Aobligate autotrophic bacteria;Bfacultative autotrophic bacteria and mixed-culture bacteria | ||||
As shown in the following reaction formula 1, various sulfur compounds (S) are produced by using sulfur-producing inorganic autotrophic microorganisms2-、S、S2O3 2-、S4O6 2-、SO3 2-) By oxidation toSulphate (SO)4 2-) While converting nitrogen in the form of nitrate to nitrogen. Reaction scheme 1
Thus, sulfur can be used as an electron donor and carrier in a sulfur-containing denitrification tank.
In addition, heterotrophic denitrification microorganisms, and facultative inorganic autotrophic microorganisms, may undergo some partial denitrification in the reactor due to the addition of small amounts of external organic matter to the inlet stream.
As shown in equation 1, sulfur is oxidized to sulfate by the reaction between sulfur and nitrogen in the inlet stream while nitrogen is reduced to nitrogen for discharge. However, in the case where the above reaction generates hydrogen ions, the supplementation of alkalinity is very important for the pH condition (pH7-8) to provide denitrification.
For this, shells are added to the tank to neutralize hydrogen ions as shown in the following reaction formula 2.
Calcium ion (Ca) produced as in equation 22+) Reacts with the phosphorus in the inlet stream to produce a water insoluble productHydroxyapatite (Ca)5(OH)(PO4)3) Phosphorus is removed as shown in the following reaction formula 3.
Typical materials used for phosphorus removal include rock phosphates, bone char, artificial dephosphorizing materials derived from limestone, calcines, and the like. Important selection criteria for dephosphorizing materials include appearance, removal efficiency, and economic benefit of the solid form used.
Since the precipitation reaction of equation 3 has a large pKso value, the reaction easily occurs. Factors affecting precipitation include pH, calcium ion (Ca)2+) Concentration and concentration of coexisting ions (including dephosphorizing materials).
As shown in table 2 below, the steel slag contains calcium oxide (CaO) as an active ingredient. Calcium oxide has been used as a neutralizing agent for acidic wastewater in general wastewater treatment processes. Table 2: chemical composition of steel slag
| Composition (I) | Percentage of |
| CaO | 40-52 |
| SiO2 | 10-19 |
| FeO | 10-40 |
| MnO | 5-8 |
| MgO | 5-10 |
| Al2O3 | 1-3 |
| P2O5 | 0.5-1 |
| S | ＜0.1 |
| Metallic Fe | 0.5-10 |
As shown in table 1, the object of the present invention can be achieved by: the facultative aerobiont denitrification microorganism is utilized to supply a small amount of external carbon source and simultaneously carry out facultative aerobiont, heterotrophic and obligate aerobiont denitrification.
The present invention is explained in detail below based on the drawings.
FIGS. 1a and 1b are schematic views of a denitrification tank [ upstream 10, downstream 20], an external carbon source (methanol, ethanol, acetate, etc.), and a sand filtration apparatus for removing organisms, which contain sulfur and shells, for treating nitrate type nitrogen-containing wastewater (wastewater with a low C/N ratio).
The inlet liquid stream suitable for denitrification includes wastewater containing nitrate type nitrogen having a low C/N ratio, wastewater containing nitrate type nitrogen after nitrification, or wastewater containing high-concentration nitrogen (permeate water, livestock wastewater, factory wastewater, etc.).
Sulfur particles and shells were added to the upstream and downstream tanks. These sulfur particles can be used as a solid medium on which autotrophic bacteria grow in the form of a thin film and as an electron donor.
Because the obligate and facultative anotrophic denitrification microorganisms have small growth rate (Y) values in the absence of a carbon source in the inlet stream, they take longer to begin acclimatizing. In order to overcome the defect, the invention has been completed, and has the following advantages:
1) the use of a small amount of an external carbon source (1/3-1/2 for methanol used in general post-denitrification) ensures easy adaptation to the environment of the sulfur-containing denitrification tank because the facultative aerobically-competent inorganic autotrophic microorganisms rapidly grow in a short time by utilizing organic matter. Adding 3mg of methanol to remove 1mg of nitrogen according to a general heterotrophic denitrification method;
2) the tank retains a large number of microorganisms and performs partial heterotrophic denitrification; the use of a small amount of external carbon source is effective in preventing the discharge of organic matter because the organic matter is completely reacted in the tank;
3) in order to prevent the alkalinity loss in the process of chemo-energy inorganic autotrophic nitrogen removal by sulfur, part of hydrogen ions formed by chemo-energy inorganic autotrophic nitrogen removal in the tank are neutralized by hydroxyl ions generated in the heterotrophic reaction, so thatthe damage of the alkalinity is minimized;
4) in order to prevent the reduction of pH by hydrogen ions generated during the reduction of nitrite type nitrogen by sulfur microorganisms, the pH is maintained at a level of 6 to 8 by shells or steel slag so that denitrification microorganisms can exert their denitrification activity. Preferably, sulfur and shell are mixed at a ratio of 4: 1 to 2: 1, and the amount of sulfur and shell is determined in consideration of inflow concentration of nitrite type nitrogen and supply period of shell;
5) calcium ion (Ca) generated by shell or steel slag ionization2-) Reacting with phosphorus in the inlet stream to form water-insoluble hydroxyapatite (Ca)5(OH)(PO4)3) Thereby removing the phosphorus. Long-term operation may cause tank blockage due to microbial floaters, requiring frequent backwashing (2); and
6) the microorganisms are removed in the sand filter tank (4) because of the low growth rate (Y) of the denitrogenating microorganisms and the very low concentration of microorganisms in the inlet liquid stream passing through the denitrogenating tank (3) containing sulphur.
The following specific examples are intended to illustrate the invention and should not be construed as limiting the scope of the invention, which is defined by the claims.
Example 1
1.1) Experimental set-Up and analytical overview
Columns containing sulfur particles were operated with varying organic concentrations at alkalinity below the theoretical amount of heterotrophic denitrification to study the distribution of organic denitrogenated from sulfur microorganisms in the presence of high concentrations of nitrate-type nitrogen. Table 3: experimental conditions for column experiments
| Column number | Filler material | Organic matter | Electron donor | Condition | |
| E1 | Control | Sulfur (253g) | - | Sulfur |
NO3-N：600mg/L
Low alkalinity
Room temperature (24-25 deg.C)
Sulfur particle size: 2-4mm
HRT: 14 |
| E2 | Column | ||||
| 1 | Methanol | Sulphur and | |||
| Column | |||||
| 2 | Ethanol | Sulphur and ethanol |
The reactor was inoculated with aerobic return sludge from a municipal sewage treatment plant. After 24 hours of contact, the column was operated continuously in upflow mode for 20 days (table 1) at a hydraulic retention time of 20h to form microorganisms on the solid medium.
Any influence of phototrophic microorganisms utilizing sulphur is prevented with a black fabric. The inflow artificial wastewater is prepared by 600mgN/l KNO3、1g/l NH4Cl、2g/l KH2PO4、0.8g/l MgSO4·7H2O、2g/l NaHCO3And trace metal solutions plus methanol and ethanol. About 930mg/l CaCO for the wastewater treatment process3The inlet stream is subjected to a base concentration in the form of a concentration insufficient to remove all NO3 --N (theoretical alkalinity required 3200mg/L CaCO)3). The column test was also performed at room temperature.
In test 1, which was designed to induce microbial nitrogen removal of sulfur, the base nutrient, the buffer solution and nitrate-type nitrogen (600mg NO) to be treated were mixed3 --N/L) is added to the column in the absence of organic matter at insufficient alkalinity.
In contrast, to investigate the correlation between the organic matter, the sulfur particles contained in the column, and the microbial treatment efficiency, test 2 was performed as follows: a theoretical amount of methanol ranging from 1/4 to 1/2 (T-1140 mg CH)3OH/L) and ethanol (T822 mg C)2H5OH/L) was added to the inlet stream (600mg NO) in the column3 -N/L) as the theoretical amount of methanol/ethanol required for heterotrophic denitrificationThe basis of (1). T means the stoichiometry of heterotrophic denitrification, corresponding to the removal of 1mg of nitrate-type nitrogen, requiring 1.9 and 1.37mg of methanol and ethanol, respectively. Equations 4 and 5 are not considered to be growth of the bacteria in an amount of about 30% higher than the stoichiometry given in the following equation.
Reaction formula 4
Reaction formula 5
The Hydraulic Retention Time (HRT) was fixed at 14 hours during wastewater treatment. This corresponds to NO3 -The load factor of-N was 1.2kg NO3 --N/m3D, sufficient to remove more than 95% of NO at sufficient alkalinity according to previous studies3 --N。
When the treatment results were within 5% of the analytical values, analysis was performed by collecting the inlet stream and the final effluent. The actual wastewater was used for tests for removing phosphorus. The experiment was carried out in a similar manner to that described above using a 3: 1 mixture of sulphur pellets and shells.
2.1) changes in pH and alkalinity
In the control experiment without organic alkalinity deficit, the inlet stream ph7.3-7.5 was lowered to the effluent ph5.9-6.0, while 40% of the nitrate in the inlet stream was removed. Calculating the Δ SO produced4 2-Reduced Delta NO3 -The ratio of-N is 5.5.
When 1/4T methanol (C1) and ethanol (C2) were added to simultaneously heterotrophically and chemolithoautotrophic denitrogenation, the pH of the effluent was increased to 6.6 and 6.7, respectively. This increase is believed to be the alkalinity provided by heterotrophic denitrification.
Initial alkalinity (920mg/L CaCO) in a control run without any organics in the stream3) More than 90% was consumed and the pH was below 6.0. Therefore, since the activity of sulfur microorganisms is significantly reduced, denitrification reaction hardly occurs.
The alkalinity of the effluent increased more than the control when methanol and ethanol were supplied to each inlet stream. The alkalinity of methanol and ethanol was maintained at 50% and 60%, respectively, with the theoretical amount of 1/4 supplied into the inlet stream. This is presumably because ethanol is more suitable for heterotrophic denitrification than methanol.
2.2) removal efficiency of nitrate type Nitrogen and production of sulfate ion
FIGS. 2 and 3 show the heterotrophic and chemolithoautotrophic denitrification efficiency as a function of methanol and ethanol addition.
NO of the inlet stream in the absence of organics during sulfur denitrogenation3 -The N concentration was 40% removed. 1/4T methanol (C1) and ethanol (C2) supplied, NO3 -The removal efficiency of N increased by 64.2% and 50.8%, respectively; with 1/2T methanol and ethanol supplies in columns 1 and 2, NO3 -The removal efficiency of-N increased to 93.1% and 73.5%, respectively. The fractions of heterotrophic denitrification and thiodenitrification are based on the Δ SO obtained in test 14 2-/ΔNO3 --N (5.5) calculation. The fraction of chemolithoautotrophic nitrogen removal in methanol increases with increasing amount of methanol, but in the case of ethanol, the fraction decreases. This is because, in the case of methanol, CO produced by the heterotrophic denitrification reaction increases with the methanol concentration2And OH-Increased, resulting in enhanced autotrophic nitrogen removal in the OT-1/2T methanol range.
In the case of ethanol, the decreased fraction of chemo-autotrophic nitrogen removal indicates that ethanol is more conducive to the high-rate growth of heterotrophic microorganisms.
Fig. 4 shows the sulfate ion generation amounts of columns 1 and 2.
As can be seen from the figure, the amount of sulfate ion production increases parallel to the supply of methanol, while the amount of sulfate ion production decreases parallel to the supply of ethanol.
Further, when 93% of nitrate type nitrogen was removed, 2800mg/L of sulfate ion was generated. Although the addition of 1/2 in the theoretically required amount in column 1 improved the treatment efficiency of nitrate type nitrogen, approximately 1,900mg/L of sulfate ion was produced. Therefore, the simultaneous autotrophic and heterotrophic denitrification reduces the amount of sulfate ion produced.
2.3) DOC and turbidity Change
In all cases of columns 1 and 2, it was shown that more than 95% DOC was removed in both species. This is because the organic matter is used for heterotrophic denitrification and microbial growth. It is noted that ethanol is more favorable than methanol in terms of overall microbial growth, but the former is inferior to the latter in terms of denitrification. For this reason, more ethanol is required to maintain the same treatment efficiency as methanol.
The amount of cells in the effluent is measured indirectly as turbidity. The turbidity of the effluent from column 1 (greater than 2.5NUT) was higher than that of column 2(6.5 NTU).
2.4) removal of phosphorus
For the dephosphorization test, the actual wastewater containing 250mg/L of nitrate type nitrogen and 20.1mg/L of phosphorus was used. A3: 1 mixture of sulphur pellets and shell was added to the sulphur containing tank and the test was carried out in a similar manner to that described above. The results showed removal of more than 98% of nitrate-type nitrogen at 8 Hours (HRT) with removal of about 10mg/L phosphorus, showing removal rates of 40-50%.
Example 2: pH of fired and dried shells over time
FIG. 5 shows the change over time of the pH of a mixture containing 1g of shells (1 hour shell fired at 550 ℃ C. and shell dried at 105 ℃ C.) and 50ml of 0.1N sulfuric acid.
The neutralization rate of the burnt shells is greater than that of the dried shells. When the tank is fully neutralized, the shell will maintain a pH (about 8) suitable for microbial growth. At CaO and Ca (OH)2In the case of (2), the reaction takes place very rapidly, and after the reaction, pH (12) conditions are established which are unsuitable for the growth of microorganisms.
Thus, it is noted that seashells can be effectively used to provide a carbon source CO for chemolithoautotrophic denitrification of microorganisms2Maintaining the pH and dephosphorizing. In addition, organic matter adhering to the dried shells should be removed to a desired level.
As described above, the present invention has the following advantages: (1) removal of sulfur-utilizing organismsIn addition to denitrification process, small amount (required amount of heterotrophic denitrification 1/3-1/2) of external carbon source (methanol, ethanol, acetate, etc.) is added to perform facultative, heterotrophic and obligatory inorganic autotrophic denitrification simultaneously to improve denitrification efficiency, (2) shell or steel slag can be used to supplement alkalinity deficiency during denitrification of sulfur, and calcium ion (Ca) in water generated by shell or steel slag can be used2+) Dephosphorizing by precipitation in the presence of phosphorus, and (3) reusing a large amount of the discarded source of conches and steel slag.
Claims (5)
1. A method for simultaneous removal of nitrogen and phosphorus from wastewater, wherein said wastewater treatment is carried out by: sulfur granules and a small amount (required amount of heterotrophic denitrification 1/3-1/2) of an external carbon source are fed into a sulfur-containing denitrification tank to simultaneously perform obligatory inorganic autotrophic, facultative inorganic autotrophic and heterotrophic denitrification, and the consumption of alkalinity and phosphorus removal are supplemented by simultaneously adding shells or steel slag.
2. The method for simultaneous removal of nitrogen and phosphorus from wastewater as claimed in claim 1, wherein said external carbon source is selected from the group consisting of methanol, ethanol and acetate.
3. The method for simultaneous nitrate-type nitrogen and phosphorus removal from wastewater as claimed in claim 1, wherein said shell or steel slag is added to said reactor in the form of a mixture of sulfur and shell in a ratio of 4: 1 to 2: 1.
4. The method for simultaneous nitrate-type nitrogen and phosphorus removal from wastewater according to claim 1, wherein said shells are selected from the group consisting of burnt or dried shells.
5. The method for simultaneous nitrate-type nitrogen and phosphorus removal from wastewater according to claim 4, wherein said shells are burnt shells.
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| KR68483/2000 | 2000-11-17 | ||
| KR1020000068483A KR20020038322A (en) | 2000-11-17 | 2000-11-17 | Simultaneous removal process of N, P for the wastewater |
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| JP (1) | JP2002166293A (en) |
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| JPS60206494A (en) * | 1984-03-30 | 1985-10-18 | Susumu Hashimoto | Simultaneous removal of nitrogen and phosphorus in waste water by sulfur replenishing aerobic-anaerobic activated sludge method |
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| JP3958900B2 (en) * | 1999-09-14 | 2007-08-15 | 新日本製鐵株式会社 | How to remove nitrogen from wastewater |
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| KR100346910B1 (en) * | 2000-03-10 | 2002-08-03 | 학교법인 인하학원 | Autotrophic denitrification using sulfur and sea shell |
| KR100503960B1 (en) * | 2000-06-29 | 2005-07-26 | 현대중공업 주식회사 | Sewage, wastewater treatment apparatus using sulfur-based denitrification process with packed bed of alkali material |
-
2000
- 2000-11-17 KR KR1020000068483A patent/KR20020038322A/en not_active Application Discontinuation
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2001
- 2001-05-11 JP JP2001141132A patent/JP2002166293A/en active Pending
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Also Published As
| Publication number | Publication date |
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| KR20020038322A (en) | 2002-05-23 |
| GB2369115A (en) | 2002-05-22 |
| GB0111584D0 (en) | 2001-07-04 |
| GB2369115B (en) | 2003-01-08 |
| JP2002166293A (en) | 2002-06-11 |
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