CN1843574A - Liquid phase flue gas desulfurizing and denitrifying purification method and apparatus - Google Patents
Liquid phase flue gas desulfurizing and denitrifying purification method and apparatus Download PDFInfo
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Abstract
The invention relates to a liquid-phase smoke desulfuration denitration purifying method and relative device, belonging to the smoke purifying technique. It can effectively remove sulfur dioxide and nitrogen oxide of smoke. It utilizes ejection bubbling method to adsorb the sulfur dioxide and nitrogen oxide of smoke, while the adsorption solution is the sodium chlorite solution in 0.001MOL/L-0.100MOL/ or the additive in 0.001MOL/L-0.005MOL/L, and the pH valve of adsorption solution is 3-11; the additive is one or the combination of calcium hypochlorite, baking soda, hydrogen dioxide solution, acid sodium phosphate, or calcium hydrate. The removing efficiency of sulfur dioxide in said invention is above 99%; the removing efficiency of nitrogen oxide is above 90%; and the utilization of adsorption solution is above 97%. Therefore, said invention has the advantages that high removing efficiency, lower cost, simple device, high utilization of adsorption solution and wider application for large, middle, and small boiler, etc.
Description
Technical Field
The invention relates to a flue gas purification method and a flue gas purification device, in particular to a method and a device for purifying flue gas by using a jet bubbler, and belongs to the technical field of flue gas purification.
Background
In recent years, with the rapid development of industry, the problem of environmental pollution is more and more prominent, for example, harmful gases such as sulfur dioxide and nitrogen oxides in combustion waste gases such as petroleum and coal are discharged into the atmosphere, which causes serious pollution to the atmospheric environment. According to the relevant information, the economic loss caused by the acid rain pollution caused by sulfur dioxide, nitrogen oxide and the like in China each year to the damage of the ecological environment and the influence of human health is about one hundred billion yuan RMB. Therefore, the national control and treatment of the pollution of harmful gases such as sulfur dioxide, nitrogen oxide and the like is more and more intensive. Domestic and foreign technologies for simultaneously desulfurizing and denitrating flue gas are reported, and various countries develop extensive research on the aspects of removing modes, improving removing efficiency and the like. At present, wet desulphurization accounts for about 82% of the world market in the flue gas desulphurization technology, and the calcium method is mainly used in the wet desulphurization. The calcium method for desulfurization has the advantages of high removal efficiency and high utilization rate of the desulfurizer, but also has the problems that equipment is easy to scale and block, so that a system cannot run and the like. The denitration technology is most researched by a catalytic reduction method in a dry method, but NO is removed by adopting the reduction methodXNot only can the nitrogen resource not be recovered, but also a large amount of reducing agent is consumed, which causes resource waste. With SO2The coexistence of (a) tends to poison the NO catalyst, which has not been a problem solved internationally for many years. The existing denitration by oxidation method generally has the problems that the price of the used oxidant is high, and even some adopted gas oxidants have potential safety hazards in equipment operation and the like. In addition, the existing flue gas desulfurization and denitration technologies are all in a grading treatment mode, and the grading treatment not only occupies a large area and is complex in system, but also is high in equipment investment and operation and maintenance cost.
Disclosure of Invention
The invention aims to provide a method and a device for simultaneously desulfurizing, denitrating and purifying flue gas, which have high removal efficiency and low investment and operation cost.
The problems stated by the invention are solved by the following technical scheme:
a liquid phase flue gas desulfurization and denitration purification method utilizes an absorbent to absorb sulfur dioxide and nitrogen oxide in flue gas in a jet bubbling reactor to complete a purification process, and is characterized in that: the absorbent consists of absorptionliquid and additive, wherein the absorption liquid is 0.001-0.100 mol/L sodium chlorite NaCLO2The absorption liquid comprises a solution and 0.001-0.008 mol/L of additive, wherein the pH value of the absorption liquid is 3-11, and the additive is calcium hypochlorite Ca (ClO)2Sodium bicarbonate NaHCO3Two, twoOxygen water H2O2Disodium hydrogen phosphate Na2HPO4Or calcium hydroxide Ca (OH)2One or a combination thereof.
The method for desulfurizing, denitrating and purifying the liquid-phase flue gas comprises the following steps: adding the sodium chlorite and the additive in the absorption liquid preparation reactor according to the proportion, calculating the concentration of the absorption liquid, adding water, uniformly mixing, adjusting the pH value to 3-11 by using sodium hydroxide or hydrochloric acid, and activating for 5-120 minutes in a dark place at the temperature of 25-80 ℃.
The liquid phase flue gas desulfurization and denitration purification method is characterized in that an absorption liquid regeneration process is additionally arranged after the purification process, the regeneration process is to react the absorption liquid participating in the reaction with 5% ammonia water in a neutralization and crystallization device to generate ammonium sulfate and ammonium nitrate solution, the ammonium sulfate and the ammonium nitrate solution are mechanically stirred and indirectly cooled by water to crystallize and separate out the ammonium sulfate and the ammonium nitrate to form solid products of the ammonium sulfate and the ammonium nitrate, and the generated mother liquor is returned to the absorption liquid preparation reactor by a circulating pump for recycling.
A liquid phase flue gas desulfurization denitration purifier which characterized in that: the device comprises a jet bubbling reactor 1, an air pump 11 and an absorption liquid preparation reactor 9, wherein the lower part of the reactor 1 is provided with an air inlet 5 which is connected with the air pump, the upper part of the air inlet is provided with an air distribution plate 15, air holes 15-1 are uniformly distributed on the air distribution plate, and the upper part of the reactor is provided with a flue gas inlet 2 and a flue gas outlet 3; the middle part is equipped with absorption liquid import 4, the intake pipe 16 intercommunication of flue gas import and equipartition, intake pipe export are visited the absorption liquid bottom in the reactor, are equipped with mechanical agitator 14 in the reactor, and the reactor bottom is equipped with absorption liquid export 6.
The liquid phase flue gas desulfurization and denitration purification device is additionally provided with a post-reaction absorption liquid treatment device 7, wherein the absorption liquid treatment device 7 consists of an ammonia water tank 17, a neutralization crystallization device 18, a centrifugal machine 19 and a mother liquid tank 20, wherein an absorption liquid outlet 6 and the ammonia water tank 17 are respectively communicated with the neutralization crystallization device 18 through pipelines, the bottom of the neutralization crystallization device is connected with the centrifugal machine 19, the latter sends the regenerated absorption liquid to a circulating pump 8 through the mother liquid tank 20, and the circulating pump is connected with an absorption liquid preparation reactor 9; the absorption liquid inlet 4 is connected with an absorption liquid preparation device, and the flue gas outlet 3 is connected with a chimney 13 through a heating mechanism 12; the flue gas inlet 2 is externally connected with a dust remover 10.
The invention is characterized in that a spraying bubbling reactor is filled with absorption liquid with certain thickness, and the absorption liquid absorbs sulfur dioxide SO in flue gas under the condition that the temperature of the flue gas is 50-120 DEG C2With nitrogen oxides NOxTherefore, the sulfur and the nitrogen oxides in the flue gas can be removed simultaneously. Tests show that the gas-liquid contact time of the invention is 0.5-2.0 seconds, the concentration of sulfur dioxide is 500-3000mg/L3The concentration of NOx is 100-1500mg/L3In the process, the removal efficiency of sulfur dioxide is more than 99%, the removal efficiency of nitrogen oxide is more than 90%, and the utilization rate of the absorbent is more than 97%. The invention has the characteristics of high removal efficiency, low investment and operation cost, simple equipment, stable operation, high utilization rate of the absorbent, easy treatment of products, convenient popularization and application and the like. The invention is not only suitable for large boilers, but also suitable for medium and small boilers and other equipment generating waste gas, and has good application prospect.
Drawings
FIG. 1 is a process flow diagram of the process of the present invention;
FIG. 2 is a schematic view of the apparatus of the present invention;
FIG. 3 is a schematic view showing the structure of an apparatus for treating an absorbing solution after reaction.
The reference numbers in the figures are as follows: 1. a jet bubble reactor; 2. a flue gas inlet; 3. a flue gas outlet; 4. an absorption liquid inlet; 5. an air inlet; 6. an absorption liquid outlet; 7. an absorbent treatment device; 8. a circulation pump; 9. an absorption liquid preparation reactor; 10. a dust remover; 11. an air pump; 12. a heating mechanism; 13. a chimney; 14. a stirrer; 15. air distribution plate, 15-1, air holes; 16. an air inlet pipe; 17. an ammonia tank; 18. a neutralization crystallization device; 19. a centrifuge; 20. a mother liquor tank; 21. and a cooling device.
Detailed Description
In the invention, a large amount of fine bubbles are generated in the flue gas bubbling absorption liquid in a jet bubbling reactor, and the gas-liquid mass transfer process is completed in the bubble rising process to achieve the aim of flue gas purification, and the technological process is shown in figure 1. The spraying bubbling reactor is filled with absorption liquid with a certain liquid level height, and the absorption liquid absorbs sulfur dioxide SO in the flue gas under the condition that the flue gas temperature is 50-120 DEG C2(concentration 500-3000 mg/L)3) And nitrogen oxide NOx (concentration of 100-3) (ii) a In the absorption liquid treatment device after the reaction, the absorption products of sulfur and nitrogen in the absorption liquid are converted into ammonium sulfate and ammonium nitrate by ammonia water, the ammonium sulfate and the ammonium nitrate are crystallized and separated out, and the generated mother liquid is sent back to the absorption liquid preparation device by a circulating pump for recycling.
The absorption liquid is 0.001 MOL/L-0.100 MOL/L sodium chlorite NaCLO2The pH value of the absorption liquid is 3-11, and the additive is 0.001-0.008 mol L/L, wherein the additive is calcium hypochlorite Ca (ClO)2Sodium bicarbonate NaHCO3Hydrogen peroxide H2O2Disodium hydrogen phosphate Na2HPO4Or calcium hydroxide Ca (OH)2One or a combination thereof. Absorbent and sulfur dioxide SO in flue gas2Reaction to produce sodium sulfate Na2SO4And sodium sulfite Na2SO3React with nitrogen oxides NOx in the flue gas to generate sodium nitrate NaNO3And sodium nitrite NaNO2Thereby removing sulfur and nitrogen in the flue gas, and the main chemical reaction is as follows:
in the invention, the sodium chlorite can absorb the oxides of sulfur and nitrogen more thoroughly under the condition of a certain PH value and the catalysis of the additive, and the utilization rate of the chlorite is high. Under the condition of certain pH value, the activation efficiency of chlorite is increased, and a certain amount of chlorine dioxide CLO is generated in the activation process2Chlorine gas CL2And chlorate CLO3 -And the like. Under the catalysis of the additive, the oxidability of the chlorite and a series of intermediate products is greatly improved, and SO is promoted2And NO oxidation, thereby greatly improving the absorption of the absorption liquid to nitrogen and sulfur oxides.
The preparation method of the absorption liquid comprises the following steps: and adding the sodium chlorite and the additive in the absorption liquid preparation reactor according to the proportion, calculating the water addition amount according to the concentration of the absorption liquid, uniformly mixing, adjusting the pH value to 3-11 by using sodium hydroxide or hydrochloric acid, and activating for 5-120 minutes in a dark place at the temperature of 25-80 ℃.
Still referring to fig. 1, the apparatus used for carrying out the method of the present invention comprises a jet bubbling reactor 1, an air pump 11, an absorption liquid preparation apparatus 9, a dust remover 10, a post-reaction absorption liquid treatment apparatus 7, a circulating pump 8, and a heating mechanism 12, wherein the bottom of the reactor is provided with an absorption liquid outlet 6, the absorption liquid outlet is connected with the absorption liquid treatment apparatus, the absorption liquid is treated to crystallize and separate out ammonium sulfate and ammonium nitrate generated by the reaction, and a part of the absorption liquid which does not participate in the reaction enters the absorption liquid preparation reactor through the circulating pump 8 for recycling, so that the utilization rate of the absorption liquid is further improved. The lower part of the jet bubbling reactor is provided with an air inlet 5 which is connected with an air pump; the middle part is provided with an absorption liquid inlet 4 which is connected with a reaction liquid preparation device; the upper part is provided with a flue gas inlet 2 and a flue gas outlet 3, the flue gas inlet is connected with a dust remover 10, the flue gas outlet is connected with a heating mechanism 12, and the heating mechanism is connected with a chimney 13. If the temperature of the purified flue gas does not meet the temperature requirement of the chimney emission, the purified flue gas is heated by a heating mechanism and then enters the chimney for emission; if the temperature of the purified flue gas meets the emission requirement, the purified flue gas directly enters a chimney to be emitted.
Referring to fig. 2, an air distribution plate 15 is arranged at the upper part of an air inlet in the jet bubbling reactor, air holes 15-1 are uniformly distributed on the air distribution plate, the flue gas inlet is connected with a plurality of air inlet pipes 16 uniformly distributed in the reactor, the outlet of each air inlet pipe extends into the bottom of the absorption liquid in the reactor, the flue gas outlet is positioned above the liquid level of the absorption liquid, and a mechanical stirrer 14is arranged in the reactor.
Referring to fig. 3, the neutralization crystallization device 18 is connected to the absorption liquid outlet 6 and the ammonia tank 17. The neutralization crystallization apparatus is provided with a mechanical stirrer 14 and a cooling apparatus 21, and the cooling apparatus is cooled by cooling water. The bottom of the neutralization crystallization device is provided with a centrifuge 19 which separates solid from liquid and conveys the liquid to a mother liquid tank 20 connected with the centrifuge, and the mother liquid tank is connected with the circulating pump 8.
The absorption liquid after the reaction reacts with ammonia water in a neutralization crystallization device to generate ammonium sulfate and ammonium nitrate solution. In the neutralization crystallization device, a mechanical stirrer is used for stirring and water is used for indirect cooling, so that ammonium sulfate and ammonium nitrate are crystallized and separated out to form ammonium sulfate and ammonium nitrate solid products, and the generated mother liquor is returned to the absorption liquid preparation reactor by a circulating pump for recycling.
The device used by the invention is beneficial to promoting the absorption of sodium chlorite to sulfur and nitrogen oxides. When gas is sprayed into liquid at a certain speed and pressure in the spraying bubbler, the floating bubbles are rapidly dispersed to form a spraying bubbling layer, the bubbles generate vortex motion and have the liquid spraying effect of internal circulation, so that the mass transfer area is increased, and the absorption liquid is fully contacted with sulfur and nitrogen in the flue gas for absorption. The air blown into the reactor by the air pump is uniformly distributed in the reactor through the air distribution plate, generates turbulence, increases the contact area of gas and liquid, promotes the oxidation and absorption of oxides of sulfur and nitrogen, and is favorable for promoting the further oxidation of sodium sulfite and sodium nitrite.
Some specific examples of the preparation of the absorption liquid are given below:
example 1: adding an absorbent solution containing 0.001mol/L sodium chlorite and 0.001mol/L calcium chlorite into a preparation reactor, adjusting the pH value to 3, and standing and activating for 5 minutes at the temperature of 259 ℃ in a dark place to obtain the absorption liquid.
Example 2: adding an absorbent solution containing 0.002mol/L sodium chlorite and 0.001mol/L hydrogen peroxide into a preparation reactor, adjusting the pH value to 4, and activating at the temperature of 40 ℃ for 60 minutes to obtain the absorption liquid.
Example 3: adding sodium chlorite of 0.005mol/L and sodium bicarbonate of 0.001mol/L into a preparation reactor, adjusting the pH value to 5, and activating at the temperature of 40 ℃ for 10 minutes to obtain the absorption liquid.
Example 4: adding an absorbent solution containing 0.010mol/L sodium chlorite and 0.002mol/L hydrogen peroxide into a preparation device, adjusting the pH value to 6, and activating at the temperature of 40 ℃ for 60 minutes to obtain the absorption liquid.
Example 5: adding an absorbent solution containing 0.050mol/L sodium chlorite and 0.003mol/L calcium hydroxide into a preparation reactor, adjusting the pH value to 11, and activating at the temperature of 80 ℃ for 120 minutes to obtain the absorption liquid.
Example 6: adding an absorbent solution containing 0.100mol/L sodium chlorite and 0.002mol/L calcium hypochlorite into a preparation reactor, adjusting the pH value to 9, and activating at the temperature of 60 ℃ for 80 minutes to obtain the absorption liquid.
Example 7: adding an absorbent solution containing 0.003mol/L sodium chlorite and 0.005mol/L calcium hydroxide into a preparation reactor, adjusting the pH value to 8, and activating at the temperature of 50 ℃ for 10 minutes to obtain the absorption liquid.
Example 8: adding absorbent solution containing 0.007mol/L sodium chlorite, 0.003mol/L calcium hypochlorite and 0.005mol/L sodium bicarbonate into a reactor, adjusting pH to 6, and activating at 40 deg.C for 30 min to obtain the absorption solution.
Example 9: adding sodium chlorite of 0.020mol/L, hypooxydol of 0.002mol/L and disodium hydrogen phosphate of 0.001mol/L into a preparation reactor, adjusting the pH value to 4, and activating at the temperature of 30 ℃ for 90 minutes to obtain the absorption liquid.
Example 10: adding a calcium hydroxide absorbent containing 0.040mol/L sodium chlorite, 0.005mol/L sodium hypochlorite and 0.001mol/L sodium hypochlorite into a preparation reactor, adjusting the pH value to 10, and activating at the temperature of 70 ℃ for 50 minutes to obtain the absorption liquid.
Example 11: adding sodium chlorite of 0.020mol/L and disodium hydrogen phosphate of 0.001mol/L into a preparation reactor, adjusting the pH value to 5, and activating at the temperature of 70 ℃ for 20 minutes to obtain the absorption liquid.
Example 12: adding the sodium chlorite with the concentration of 0.080mol/L, the calcium chlorite with the concentration of 0.004mol/L and the calcium hydroxide with the concentration of 0.001mol/L into a preparation reactor, adjusting the pH value to 10, and activating at the temperature of 70 ℃ for 50 minutes to obtain the absorption liquid.
Example 13: adding sodium chlorite of 0.008mol/L, sodium bicarbonate of 0.003mol/L and hydrogen peroxide of 0.004mol/L into a preparation reactor, adjusting the pH value to 7, and activating at the temperature of 25 ℃ for 40 minutes to obtain the absorption liquid.
Claims (5)
1. A liquid phase flue gas desulfurization and denitration purification method utilizes an absorbent to absorb sulfur dioxide and nitrogen oxide in flue gas in a jet bubbling reactor to complete a purification process, and is characterized in that: the absorbent consists of absorption liquid and additive, wherein the absorption liquid is 0.001 MOL/L-0.100 MOL/L sodium chlorite NaCLO2The absorption liquid comprises a solution and 0.001-0.008 MOL/L of additive, wherein the pH value of the absorption liquid is 3-11, and the additive is calcium hypochlorite Ca (ClO)2Sodium bicarbonate NaHCO3Hydrogen peroxide H2O2Disodium hydrogen phosphate Na2HPO4Or calcium hydroxide Ca (OH)2One or a combination thereof.
2. The liquid-phase flue gas desulfurization, denitrification and purification method according to claim 1, characterized in that: the preparation method of the absorption liquid comprises the following steps: adding the sodium chlorite and the additive in the absorption liquid preparation reactor according to the proportion, calculating the water addition amount according to the concentration of the absorption liquid, uniformly mixing, adjusting the pH value to 3-11 by using sodium hydroxide or hydrochloric acid, and activating for 5-120 minutes in a dark place at the temperature of 25-80 ℃.
3. The liquid-phase flue gas desulfurization, denitrification and purification method according to claim 1 or 2, characterized in that: and in the regeneration process, the absorption liquid participating in thereaction reacts with ammonia water in a neutralization crystallization device to generate ammonium sulfate and ammonium nitrate solution, the ammonium sulfate and the ammonium nitrate solution are stirred and indirectly cooled by water to crystallize and separate out the ammonium sulfate and the ammonium nitrate to form solid ammonium sulfate and ammonium nitrate products, and the generated mother liquor is returned to the absorption liquid preparation reactor by a circulating pump for recycling.
4. The utility model provides a liquid phase flue gas desulfurization denitration purifier which characterized in that: the device comprises a jet bubbling reactor (1), an air pump (11), an absorption liquid preparation reactor (9) and an absorption liquid treatment device (7), wherein an air inlet (5) is formed in the lower part of the reactor (1) and is connected with the air pump, an air distribution plate (15) is arranged on the upper part of the air inlet, air holes (15-1) are uniformly distributed in the air distribution plate, and a flue gas inlet (2) and a flue gas outlet (3) are formed in the upper part of the reactor; the middle part is equipped with absorption liquid import (4), the intake pipe (16) intercommunication of gas inlet and equipartition, intake pipe export probe into the absorption liquid bottom in the reactor, is equipped with mechanical agitator (14) in the reactor, and the reactor bottom is equipped with absorption liquid export (6), and the absorption liquid export is connected with absorption liquid processing apparatus (7).
5. The liquid-phase flue gas desulfurization, denitrification and purification device of claim 4, wherein: a post-reaction absorption liquid treatment device (7) is additionally arranged, wherein the absorption liquid treatment device (7) consists of an ammonia water tank (17), a neutralization crystallization device (18), a centrifugal machine (19) and a mother liquid tank (20), an absorption liquid outlet (6) and the ammonia water tank (17) are respectively communicated with the neutralization crystallization device (18) through pipelines, the bottom of the neutralization crystallization device is connected with the centrifugal machine (19), the centrifugal machine is used for conveying regenerated absorption liquid to a circulating pump (8) through the mother liquid tank (20), and the circulating pump is connected with an absorption liquid preparation reactor (9); the absorption liquid inlet (4) is connected with an absorption liquid preparation device, and the flue gas outlet (3) is connected with a chimney (13) through a heating mechanism (12); the flue gas inlet (2) is externally connected with a dust remover (10).
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| CN101574621A (en) * | 2009-06-19 | 2009-11-11 | 华北电力大学（保定） | Liquid phase method for removing dioxin-like compounds from flue gas and device thereof |
| CN102068888A (en) * | 2010-12-28 | 2011-05-25 | 北京博奇电力科技有限公司 | Method for simultaneously desulfurizing and denitrating flue gas by wet method |
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| CN104069723A (en) * | 2014-07-17 | 2014-10-01 | 南京信息工程大学 | Combined method for desulfurization, denitration and decarburization of exhaust gas |
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