CN112023661B - Synchronous flue gas desulfurization and denitrification and sulfur and nitrogen co-recycling process combining chemical absorption with biotransformation - Google Patents
Synchronous flue gas desulfurization and denitrification and sulfur and nitrogen co-recycling process combining chemical absorption with biotransformation Download PDFInfo
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Abstract
The invention discloses a synchronous flue gas desulfurization and denitrification and sulfur and nitrogen co-recycling process combining chemical absorption with biotransformation, which is characterized in that an alkaline absorption liquid containing an oxidant is utilized in a desulfurization and denitrification absorption tower to absorb SO in flue gas2And NOxConverted into sulfate, sulfite, nitrate and nitrite. Then pumping the absorption liquid into a microbial oxygen bioreactor, and reducing sulfate and sulfite into sulfide (S) by using microorganisms (sulfate reducing bacteria)2‑) Further converted into elemental sulfur and will absorb NOxThe solution producing nitrate, nitrite is converted to ammonia. The mixed solution containing elemental sulfur and ammonia generated by the micro-aerobic bioreactor is treated by an ammonia and sulfur recovery system to obtain sulfur and ammonia with higher content for recycling, and the alkaline solution obtained by the ammonia and sulfur recovery system returns to the desulfurization and denitrification absorption tower for recycling. The method has reasonable process, low energy consumption, low investment and operation cost and small secondary pollution, can achieve the aims of simultaneously desulfurizing and denitrating the flue gas and recovering elemental sulfur and ammonia, and is an ideal process for desulfurizing and denitrating the flue gas and recycling the sulfur and the nitrogen together.
Description
Technical Field
The invention belongs to the technical field of waste gas purification of environmental protection engineering, and relates to a synchronous flue gas desulfurization and denitrification and sulfur and nitrogen co-recycling process combining chemical absorption with biotransformation.
Background
Sulfur dioxide (SO)2) And Nitrogen Oxides (NO)x) Mainly from natural sources such as volcanic eruption, thunder and lightning and microbial activity and artificial sources of artificial activities such as industry, transportation, agriculture and forestry soil destruction and fossil fuel combustion, and NOxCan form photochemical smog with hydrocarbon, generate acid rain and acid mist, damage vegetation, harm human health, destroy ozone layer, and simultaneously SO2Is also the main material for the formation of acid rain. SO discharged from industrial sources2And nitrogen NOxOccupy a major portion of the man-made resources and it is therefore important to take certain effective measures to reduce or eliminate the emissions of sulphur dioxide and nitrogen oxides from industrial sources.
The flue gas desulfurization and denitration technology which is applied more in industry is a limestone-gypsum wet desulfurization and Selective Catalytic Reduction (SCR) denitration combined process, but the combined process has the problems of large equipment investment, higher operation cost, secondary pollution and the like, so that the difficulty of application of the combined process in flue gas desulfurization and denitration is increased. Therefore, researchers are constantly working on developing more economical and efficient flue gas desulfurization and denitrification technologies. The method has the advantages of high efficiency, low cost, no secondary pollution and the like, and is widely concerned by researchers.
In the early 90 s of the 20 th century, the agriculture university of Wageningen, the Netherlands, conducted a great deal of research in the field of treating sulfate-containing wastewater, and developed a biological desulfurization process for recovering elemental sulfur. Biological desulfurization technology of HTSE & E and PAQUES company in the Netherlands, namely flue gas alkali liquor absorption/anaerobic-aerobic biotransformation desulfurization technology, is developed on the basis of biological desulfurization of HTSE & E and PAQUES companies in the Netherlands, and the new technology is applied to flue gas desulfurization engineering.
A clean biological desulfurization and denitration method for flue gas is invented by the Prochen Miner of the institute of Process engineering of Chinese academy of sciences and the device patent (CN 105561755A). Sulfur dioxide and nitrogen oxides are absorbed and converted into acidic absorption pregnant solution, organic substances are added into the acidic absorption pregnant solution, sulfide is blown off and converted into hydrogen sulfide by acidification of the acidic mixed solution, the generated hydrogen sulfide is blown off and absorbed and converted into elemental sulfur by biological sulfur oxidation reaction, and the generated denitration absorption solution is converted into nitrogen by denitrification combined with sulfate reduction. However, in an anaerobic environment, denitrifying bacteria and sulfate reducing bacteria compete for a common electron donor, and simultaneously the extracted hydrogen sulfide needs to be further absorbed and converted, thereby causing the overall operation efficiency of the denitrifying desulfurization technology to be reduced; it is difficult to ensure the high-load and high-efficiency operation of the denitrification desulfurization process.
In the process of flue gas denitration by an oxidant wet method, nitrogen oxides are absorbed and oxidized into nitrates through the absorption liquid containing the oxidant, and the denitration wastewater containing the nitrates is directly discharged outside and can bring about the problem of water pollution.
The DNRA process converts nitrate to ammonia nitrogen, a process that is one of the microbial-mediated pathways, but is distinct from the assimilation of the process of converting N to cellular components. NH in contrast to nitrate4 +Is more readily bioavailable and is a less stable form of inorganic nitrogen. Woods have been observed as early as 1938 under pure culture conditionsClosrridiumThe nitrate reduction process of welehii has the phenomenon of dissimilatory reduction of nitrate to ammonium (DNRA). Some studies after the 70 s have shown that the DNRA process can be carried out in soil, sediment and digested sludge. The Gruca-Rokosz study showed that the accumulation of nitrite in rivers is mainly caused by anaerobic DNRA bacteria in the bottom sediments of rivers. Liujia, etc. and separating a bacterial strain (Q1-3) which can be dissimilatorily reduced into ammonium under aerobic conditions from the biological membrane, thereby proving that the DNRA process can occur in an aerobic environment. Brunet et al have discovered that a number of microorganisms can perform the fermentative DNRA process, including Clostridium, Vibrio desulforicus, and Pseudomonas (R) ((R))Clostridia, Desulfovibrio, Vibrio, and Pseudomonas). Another more specific form of DNRA is nitrate removal by oxidative degradation of inorganic chemoautotrophic sulfur bacteria, the oxidatively degraded sulfur species comprising free form sulfur (H)2S、S2-) And elemental S, with simultaneous conversion of nitrate to amino salt and N2And O. Weber et al also demonstrated that in freshwater and marine system studies, it was known that certain sulfur oxidizing bacteria could utilize nitrate to convert H2Oxidation of S and elemental S to SO4 2-And nitrate is finally converted into NH by oxidation of sulfur bacteria4 +And N2. The DNRA bacteria that have been found to date are divided into four groups according to the respiratory type, obligate anaerobes (A), (B), (CClosridium sps, Desulfovibriogigas, Desulfovibrio sp, Veillonellaalcalescens, Wolinellesuccimogenes, Selenomonasruminantium, etc.), facultative anaerobes (a)Citrobacter sp, Escherichia coli, Photobacteriumfischeri et al), Microoxophilum (A), (B), (C), (Campylobacter sputoum et al) and aerobic bacteria (Pseudomonas sps, Neisseria subflava, Bacillussps, etc.). Meanwhile, Wang Aijie et al convert sulfate into elemental sulfur in the same bioreactor in the presence of oxygen, thus realizing the micro-aerobic conversion of SRB and SOB. So that the nitrate can be directly converted into ammonia,this also makes it possible to simultaneously complete the conversion of the sulphide into elemental sulphur and the nitrate into ammonia in the same reactor.
The integrated device for desulfurization and denitrification of flue gas by seawater and biological methods (patent application number: CN 201310610594.3) such as Liudingping, etc. provides that sulfur dioxide and nitrogen oxide in flue gas are respectively removed by biological methods; in addition, Chinese patents with application numbers CN201410016624.2, CN104607029A, CN200810064858.9, CN105032152A and CN201320758902.2 all mention the desulfurization and denitration of flue gas by biological method.
The invention provides a method for absorbing SO in flue gas by adding alkaline absorption liquid containing oxidant in a desulfurization and denitrification absorption tower on the basis of biological desulfurization of flue gas and then absorbing SO in the flue gas by using the alkaline absorption liquid containing oxidant2And NOxConverting into sulfate, sulfite, nitrate and nitrite, pumping the absorption liquid into a microbial oxygen bioreactor, and reducing the sulfate and sulfite into sulfide (S) by using sulfate reducing bacteria in the bioreactor2-) Meanwhile, the generated sulfide, nitrate and nitrite are converted into ammonia by using the functional bacteria for reducing nitrate into ammonia through dissimilation. More and more strains are found to be capable of effectively converting nitrogen-containing compounds into ammonia under the micro-aerobic and oxygen conditions, so that the microbial sulfur and nitrogen resource utilization and the wet flue gas desulfurization and denitration by an oxidant can be combined, sulfides generated by sulfate reduction are converted into elemental sulfur under the micro-aerobic condition, nitrate is reduced into ammonia, and the elemental sulfur and ammonia resource utilization is realized.
The combined process is based on a microbial flue gas desulfurization process, sulfur dioxide and nitrogen oxides can be simultaneously removed from flue gas only by adding a certain amount of oxidant in a spray tower, elemental sulfur and ammonia can be recovered, and a certain amount of dissolved oxygen is added into a reactor, so that the toxicity of sulfide to organisms in the reactor is solved, the reactor stably runs, the process of reducing nitrate into ammonia through dissimilation is promoted, and the pollution problem caused by wet desulfurization and denitration is eliminated.
Disclosure of Invention
The invention aims to provide a synchronous flue gas desulfurization and denitrification and sulfur and nitrogen co-recycling process combining chemical absorption with biological conversion.
The technical scheme of the invention is as follows:
a synchronous flue gas desulfurization and denitrification and sulfur and nitrogen co-recycling process combining chemical absorption and biotransformation is characterized in that:
(1) sulfur dioxide (SO) in the flue gas2) And Nitrogen Oxides (NO)x) Absorbing with an absorption tower, and absorbing SO in the flue gas with an absorption liquid containing an oxidant in the absorption tower2And NOxProducing sulfate, sulfite, nitrate, nitrite;
(2) containing absorbed SO2And NOxThe solution which generates sulfate, sulfite, nitrate and nitrite enters a micro-aerobic bioreactor, and sulfate and sulfite are reduced into sulfide (S) by sulfate reducing bacteria2-) Meanwhile, the generated sulfide, nitrate and nitrite are converted into ammonia by using the functional bacteria for reducing nitrate into ammonia;
(3) and (2) respectively treating the mixed solution containing elemental sulfur and ammonia generated by the bioreactor by a sulfur recovery system and an ammonia recovery system to obtain sulfur and ammonia with higher content for recycling, and returning the alkaline solution generated after the sulfur and the ammonia are separated to the desulfurization and denitrification absorption tower for recycling.
The absorption tower is a packed tower or a spray tower, the micro-aerobic bioreactor adopts an activated sludge reactor, the ammonia recovery system comprises a distillation tower, and the sulfur recovery system comprises a sedimentation tank and a solid-liquid separation device.
The absorption liquid in the desulfurization and denitrification absorption process is NaOH and NaHCO3、Na2CO3One or more than two of (A) and H2O2Or a combination of NaClO.
The pH value in the micro-aerobic bioreactor is controlled to be 7.5 +/-0.2, and the temperature is controlled to be 25-45oC, controlling the retention time at2-45 h，CODcrN: S = (2-20):1:1, and the dissolved oxygen is controlled to be 0-0.2 mg/L.
The carbon source used by the microorganism in the micro-aerobic reactor is lactic acid, sludge breaking liquid and high-concentration easily degradable organic wastewater, and the phosphorus source is dihydric phosphate or dibasic phosphate.
The invention has the advantages that:
the utility model provides a flue gas desulfurization denitration technology when chemical absorption combines anaerobic-aerobic conversion is on the desulfurization of biological method's basis, only needs to increase some oxidants in the spray column and both can realize flue gas desorption sulfur dioxide and nitrogen oxide simultaneously, recoverable simple substance sulphur and ammonia again, realizes simultaneously flue gas desulfurization denitration in-process, retrieves simple substance sulphur and ammonia to sulfur dioxide and nitrogen oxide resource recovery. The method has reasonable process, low energy consumption, low investment and operation cost, and no secondary pollution.
Drawings
The attached drawing is a process flow chart of synchronous flue gas desulfurization and denitrification and sulfur and nitrogen co-recycling by combining chemical absorption with biotransformation.
In the figure: 1. a flue gas inlet; 2. a booster fan; 3. a desulfurization and denitrification absorption tower; 4. a desulfurization and denitrification absorption liquid circulating pump, wherein a circulating liquid outlet flows back to 3; 5. a micro-aerobic bioreactor; 6. a stirring system; 7. a gas outlet; 8. a sulfur/ammonia recovery system; 9. recovering sulfur sludge; 10. a flue gas outlet; 11. adding alkali liquor and oxidant solution to prepare a system; 12. adding an alkali liquor pump.
Detailed Description
The following detailed description of the present invention will be made in conjunction with the accompanying drawings and the technical solutions, but the present invention is not limited to the following examples.
The flue gas is sent to the lower part of a desulfurization and denitrification absorption tower 3 by a booster fan 2 arranged in the process, sodium hydroxide absorption liquid containing oxidant in the absorption tower is in countercurrent contact with the absorption liquid flowing from the upper part of the tower, and SO in the flue gas2And NOxAbsorbed by sodium hydroxide containing an oxidant and oxidized into sulfate, sulfite, nitrate or nitrite, and the absorption liquid is pumped into a micro-aerobic tank; sulfate and nitrate in micro-aerobic biological tankThe sulfate reducing bacteria and the nitrate dissimilatory reducing bacteria are utilized to oxidize the sulfide into elemental sulfur, the nitrate is converted into ammonia, the aim of simultaneously desulfurizing and denitrating can be achieved, the elemental sulfur and the ammonia can be recycled, and the aim of simultaneously achieving environmental protection and waste recycling is achieved.
The treated liquid after the microbial conversion treatment enters a sulfur recovery system 11 and an ammonia recovery system 12, and the alkaline solution is returned to the absorption tower circulation system by a circulation liquid conveying pump and is recycled as the desulfurization and denitrification absorption liquid.
Example 1
The flue gas flow of the coal-fired thermoelectric boiler is 10 ten thousand Nm3/h，SO2The content is 1000 mg/Nm3NO content of 500 mg/Nm3Flue gas temperature of 130oC, SO when leaving the absorption column according to the process of the invention2The content is 35 mg/Nm3NO content of 50 mg/Nm3(ii) a The desulfurization efficiency is more than 95%, the denitration efficiency is more than 90%, the elemental sulfur is recycled at 1158 kg/d, and the ammonia is recycled at 505 kg/d.
SO2The absorption tower is a spray tower with a diameter of 3.5 m and a height of 22 m, and the liquid-gas ratio is 15L/Nm3The denitration absorption liquid in the absorption process is NaOH and NaHCO3、Na2CO3One or more than two of (A) and H2O2Or a combination of NaClO.
The micro-aerobic bioreactor adopts an activated sludge method, the pH value is controlled to be 7.5 +/-0.2, and the temperature is controlled to be 25-45oC, the retention time is controlled to be 2-45h, CODcrN: S = (2-20):1:1, and the dissolved oxygen is controlled to be 0-0.2 mg/L.
The sulfur recovery system consists of a coagulating sedimentation system, a sulfur sludge drying system and a sulfur sludge purification system.
The ammonia recovery system consists of an ammonia distillation system and a condensation system.
Example 2
The flue gas flow of a 200 t/h coal-fired thermoelectric boiler is 25 ten thousand Nm3/h，SO2The content is 900 mg/Nm3NO content of 400 mg/Nm3Flue gas temperature of 150oC, SO when leaving the absorption column according to the process of the invention2The content is 35 mg/Nm3NO content of 50 mg/Nm3(ii) a The desulfurization efficiency is more than 95 percent, the denitration efficiency is more than 85 percent, the elemental sulfur is recovered by 2595 kg/d, and the ammonia is recovered by 1190 kg/d.
SO2The absorption tower is a spray tower with diameter of 6 m and height of 25 m, and liquid-gas ratio of 15L/Nm3The denitration absorption liquid in the absorption process is NaOH and NaHCO3、Na2CO3One or more than two of (A) and H2O2Or a combination of NaClO.
The micro-aerobic bioreactor adopts an activated sludge method, the pH value is controlled to be 7.5 +/-0.2, and the temperature is controlled to be 25-45oC, the retention time is controlled to be 2-45h, CODcrN: S = (2-20):1:1, and the dissolved oxygen is controlled to be 0-0.2 mg/L.
The sulfur recovery system consists of a coagulating sedimentation system, a sulfur sludge drying system and a sulfur sludge purification system.
The ammonia recovery system consists of an ammonia distillation system and a condensation system.
Claims (4)
1. A synchronous flue gas desulfurization and denitrification and sulfur and nitrogen co-recycling process combining chemical absorption and biotransformation is characterized in that: the method comprises the following process steps:
(1) sulfur dioxide (SO) in the flue gas2) And Nitrogen Oxides (NO)x) Absorbing with an absorption tower, and absorbing SO in the flue gas with an absorption liquid containing an oxidant in the absorption tower2And NOxConverting into sulfate, sulfite, nitrate and nitrite;
(2) containing the above-mentioned absorbed SO2And NOxThe solution for generating sulfate, sulfite, nitrate and nitrite enters a micro-aerobic bioreactor, and sulfate and sulfite are reduced into sulfide (S) by sulfate reducing bacteria2-) Meanwhile, nitrate dissimilatory reduction ammonia-forming functional bacteria are utilized to convert the generated sulfide, the nitrate and the nitrite generated by absorption into ammonia; the pH value in the micro-aerobic bioreactor is controlled to be 7.5 +/-0.2, the temperature is controlled to be 25-45 ℃, the retention time is controlled to be 2-45h, and the CODcr:N:S＝(2-20) 1:1, wherein the dissolved oxygen is controlled to be 0-0.2 mg/L;
(3) and (2) respectively treating the mixed solution containing elemental sulfur and ammonia generated by the bioreactor by a sulfur recovery system and an ammonia recovery system to obtain sulfur and ammonia with higher content for recycling, and returning the alkaline solution generated after the sulfur and the ammonia are separated to the desulfurization and denitrification absorption tower for recycling.
2. The synchronous flue gas desulfurization and denitrification and sulfur and nitrogen co-recycling process combining chemical absorption and biological conversion as claimed in claim 1, characterized in that: the absorption tower is a packed tower or a spray tower, the micro-aerobic bioreactor adopts an activated sludge reactor, the ammonia recovery system comprises a distillation tower, and the sulfur recovery system comprises a sedimentation tank and a solid-liquid separation device.
3. The synchronous flue gas desulfurization and denitrification and sulfur and nitrogen co-recycling process combining chemical absorption and biological conversion as claimed in claim 1, characterized in that: the absorption liquid in the desulfurization and denitrification absorption process is NaOH and NaHCO3、Na2CO3One or more than two of (A) and H2O2Or a combination of NaClO.
4. The synchronous flue gas desulfurization and denitrification and sulfur and nitrogen co-recycling process combining chemical absorption and biological conversion as claimed in claim 1, characterized in that: the carbon source used by the microorganism in the micro-aerobic reactor is lactic acid, sludge breaking liquid and high-concentration easily degradable organic wastewater, and the phosphorus source is dihydric phosphate or dibasic phosphate.
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| CN101327397A (en) * | 2008-07-03 | 2008-12-24 | 大连理工大学 | Method for simultaneously removing SO2 and NO in flue gas by biological reduction and complexing absorption |
| CN101302069A (en) * | 2008-07-04 | 2008-11-12 | 哈尔滨工业大学 | Technological system and method for removing carbon, nitrogen and sulphur in waste water synchronously |
| WO2015155208A1 (en) * | 2014-04-09 | 2015-10-15 | Tischmacher Heinz | Device and method for producing fertilizer from the exhaust gases of a production system |
| CN108328730A (en) * | 2018-02-11 | 2018-07-27 | 山东大学 | A method of Anammox efficient process nitrogenous effluent is coupled for ammonium combination denitrification based on nitrate dissimilatory reduction |
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