CN212348292U - Denitration system for flue gas denitration by using ozone and packed tower - Google Patents
Denitration system for flue gas denitration by using ozone and packed tower Download PDFInfo
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- CN212348292U CN212348292U CN202020200394.6U CN202020200394U CN212348292U CN 212348292 U CN212348292 U CN 212348292U CN 202020200394 U CN202020200394 U CN 202020200394U CN 212348292 U CN212348292 U CN 212348292U
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Abstract
The invention discloses a denitration system for flue gas denitration by utilizing ozone and a packed tower, which comprises the packed tower, an ozone supply system and a soluble alkali liquor supply system, wherein a packing layer is arranged in the packed tower, the ozone supply system conveys ozone into the packed tower, the soluble alkali liquor supply system conveys the soluble alkali liquor into the packed tower, a flue gas inlet of the packed tower is arranged at the upper position of the packing layer, a flue gas outlet is arranged below the packing layer, the packing layer is arranged between the flue gas inlet and the flue gas outlet, an ozone inlet pipe orifice is arranged above the packing layer, a liquid inlet pipe orifice of the soluble alkali liquor is also arranged at the upper position of the packing layer, and the ozone and the soluble alkali liquor are contacted, reacted and transferred in a gap between the packing. The packed tower is applied to the field of flue gas denitration, is low in cost and high in efficiency, and has great economic and social benefits.
Description
Technical Field
The invention relates to the technical field of flue gas denitration, in particular to a system for flue gas denitration by using ozone and a packed tower.
Background
Coal-fired power generation, steel mill steelmaking and other processes taking coal and petroleum as heat sources are one of the main sources of nitrogen oxide increase in the environment. In order to reduce the influence on the environment, various manufacturers adopt various methods to reduce the emission of nitrogen oxides in the combustion tail gas (the flue gas), namely, the flue gas is subjected to denitration treatment. The existing flue gas denitration technology mainly comprises two main types, namely a catalytic reduction method and an oxidation method. Compared with a catalytic reduction method, the oxidation method theoretically has the advantages of simple process, low cost and the like, so that the method becomes the research and research direction in the field of flue gas denitration at present. Ozone is a strong oxidant, is simple to produce, is a clean oxidant, and naturally becomes the object of choice in the oxidation process. The prior art discloses a plurality of technical schemes for denitration of flue gas by ozone. Such as CN109210955A, CN 109224820A, CN109173662A, CN108404616A, CN 109675421A, CN 109621662 a, etc., all disclose the use of ozone for flue gas denitration. However, the prior art also indicates that there are technical difficulties in the denitrification with ozone, as disclosed in CN 109621662A, O3Although a common strong oxidizer, O is3The direct oxidation reaction has higher selectivity, slower reaction rate and low utilization rate. CN108905555A discloses3Is unstable, slowly decomposes at room temperature, and rapidly decomposes at 200 ℃. More importantly, the actual conditions of the flue gas, such as higher temperature (about 100-300 ℃), lower pressure (about kilopascal level, even negative pressure), low concentration of nitric oxide (about tens-500 mg/m)3) Faster flow rates (about 1-10 m/s), etc. can greatly affect the presence of ozone and its effect on the oxidation of NO. In the actual production, the ozone oxidation method cannot be widely popularized and applied becauseIts effect is not good. In order to improve the oxidation effect, the prior art adopts the increased ozone input amount, which leads to the increased cost and cannot be popularized and applied.
Disclosure of Invention
In order to solve the technical problems, the invention provides a denitration system for flue gas denitration by using ozone and a packed tower, which comprises the following contents:
the utility model provides an utilize ozone and filled tower to carry out denitration system of flue gas denitration, including filled tower, ozone supply system, soluble alkali lye supply system, filled tower is the upright tower, inside is equipped with the packing layer, ozone supply system advances the flue gas passageway with ozone transport through the intake pipe, soluble alkali lye supply system advances filled tower with soluble alkali lye transport through the feed liquor pipe, a serial communication port, filled tower's flue gas import sets up the upper portion position at the packing layer, the below at a packing layer is established to the exhanst gas outlet, the packing layer is arranged between flue gas import and exhanst gas outlet, the ozone mouth of pipe sets up the top at the packing layer that admits air, the feed liquor mouth of pipe of soluble alkali lye also sets up the upper portion position at the packing layer, ozone, soluble alkali lye contacts in the clearance.
Preferably, the ozone inlet pipe orifice is arranged at a position below the inlet pipe orifice of the soluble alkali liquor.
Preferably, the flow direction in which ozone is discharged from the air inlet nozzle coincides with the flow direction of the flue gas.
Preferably, the ozone inlet pipe orifice is provided with an ozone distributor.
Preferably, the soluble alkali liquor is discharged from the liquid inlet pipe orifice in a spraying mode.
Preferably, the upper part of the ozone inlet pipe orifice is also provided with a filler layer.
The invention content is explained in the following with the prior art:
theoretical basis of the invention
1. Different from the prior art, ozone does not oxidize NO in the flue gas, but directly enters the packing layer, and is firstly contacted with soluble alkali liquor and decomposed in the packing layer.
In the prior art, the methods related to ozone denitration generally comprise: firstly, introducing ozone into the flue gas, and oxidizing NO in the flue gas by the ozone to form high-valence nitrogen oxide; then the flue gas enters an absorption system again, and oxidation products are absorbed by alkali liquor. Such technical means are adopted in CN109210955A, CN 109224820A, CN109173662A, CN108404616A, CN 109675421A, CN 109621662 a, etc.
However, in the present invention, ozone is directly fed into the packed tower and contacts with the soluble alkali liquor in the gaps of the packing. Because the flow velocity of the flue gas is extremely fast (generally more than 1 m/s), the size of the packed tower is limited, and the alkali liquor and the ozone enter from the upper part of the packing layer, so that the ozone has little time to directly oxidize NO in the flue gas and directly enters the packing layer.
In a preferred embodiment, the ozone is discharged in the same direction as the flue gas, and the ozone has less time and opportunity to oxidize NO in the flue gas.
In another preferred embodiment, the outlet for ozone is required to be below the outlet for the soluble lye, i.e. the ozone is released directly into the environment of the soluble lye. This is one of the differences between the present invention and the prior art.
The reason for adopting the technical means is as follows:
(1) applicant believes that NO is in the process of NO conversion2There is an equilibrium relationship in the transformation.
At higher temperatures, lower pressures and lower concentrations of NO, NO is not readily converted to NO2Or NO after conversion2And immediately converted to NO. Thus, even if NO in the flue gas can be replaced by O3Oxidation, the proportion of NO oxidized in the final flue gas is small.
O3 + NO → NO2 + O2 ①
NO2 → O + NO ②
O + O → O 2 ③
According to the equilibrium relationship, if the concentration of NO in the flue gas is low (generally not more than 300 mg/m)3) Even if NO in the flue gas is oxidized into high-valence NO2According toThe above formulas (i) and (ii) will eventually also convert back to NO. This is also a reason why the amount of ozone input is high and the oxidation effect is not high in the conventional ozone denitration technology.
Since ozone is difficult to directly oxidize NO in the flue gas, the invention adopts the technical means that ozone enters the packing layer to contact with soluble alkali liquor, but NO is not directly oxidized in the flue gas.
(2) Ozone is decomposed when meeting soluble alkali liquor:
the data of ozone water stability research and ozone decomposition influence of different buffer solutions indicate that the alkaline solution can cause rapid decomposition of ozone; experiments have shown that the greater the pH of the solution, the faster the ozone decomposition. When the pH value reaches 9, the half-life of ozone in water is less than 1 minute, and when the pH value exceeds 12, the decomposition of ozone is almost instantaneous.
Under alkaline environment, ozone can rapidly generate catalytic decomposition, and the decomposition process is as follows:
O3 + OH-→ O2 + HO 2 - ④
HO2 -→ OH- + O ⑤
O + O → O 2 ⑥
for the present invention, ozone directly enters the packing layer and contacts with soluble alkali liquor in the gaps of the packing. Ozone is decomposed after contacting with soluble alkali liquor, but the decomposition of ozone does not reduce O3The oxidation of NO, on the contrary, also intensifies its oxidizing effect, because: the decomposed product of ozone contains free monatomic O with stronger oxidizing property (see formula (v)), and the oxidizing property of monatomic O is stronger than that of O3More readily and efficiently oxidize NO.
O + NO → NO2 ⑦
Moreover, because gaps among the fillers are filled with soluble alkali liquor, the liquid isolation effect exists, and monoatomic O generated by the decomposition of ozone is difficult to combine with O2The probability of occurrence of the formula is reduced, so that a large number of monoatomic atoms O released according to the formulaNO in the flue gas entering the filler gap at the same time is oxidized, and nitrogen oxide in the flue gas can be converted from low-valence NO to high-valence NO2And (4) transformation. Therefore, the ozone is decomposed by the soluble alkali liquor in the filler gap and is used for oxidizing NO in the smoke passing through the filler gap simultaneously, which is completely different from the technical idea in the prior art.
In a preferred scheme, the spraying direction of the ozone is consistent with the direction of the flue gas, so that the ozone can be ensured to rapidly enter the packing layer, and the resistance of the flue gas can be reduced, thereby reducing the energy consumption. In the prior art, ozone is usually reversely sprayed to the smoke.
Of course, some of the undecomposed ozone is also present in the interstices of the packing and is in contact with the flue gas. The presence of this portion of ozone may directly oxidize NO:
O3 + NO → NO2 + O 2 ⑧
but, in comparison, O3The oxidation property to NO is weaker than that to O, therefore, ozone is decomposed in the gaps of the filler by soluble alkali liquor to oxidize NO, and a better oxidation effect can be obtained.
2. In the packing layer, NO is immediately absorbed by soluble alkali liquor after being oxidized.
The inventive step is also that NO is absorbed in the packing layer immediately after oxidation, compared to the prior art.
As mentioned above, O atom and O3Can oxidize NO, the oxidizing environment being in the interstices of the filler. Since the gaps between the packing are filled with soluble lye and oxidation products (high-valence nitrogen oxides, e.g. NO)2) Can be immediately absorbed by soluble alkali liquor to form nitrate, nitrite or nitrite and can be retained in the alkali liquor, and the reaction of formula (II), namely NO can not be produced2The conversion to NO, and in addition, the lye facilitates the absorption of NO, see equation r. So that the main nitrogen oxides in the flue gas can be removed in the packing layer.
3NO2 +2 OH- → NO3 - + NO + H2O ⑨
NO2 + NO + 2OH- → 2NO2 - + H2O ⑩
In the prior art, the final removal effect of NO is poor due to the separation of oxidation and absorption. The technical means that NO is absorbed after being oxidized forms the difference point between the invention and the prior art.
(II) interpretation of related nouns
1. Packed tower
The packed tower in the prior art is one of important devices for gas-liquid mass transfer in chemical production. The tower body is often a vertical cylinder, a packing support plate is arranged at the lower part in the tower, packing is used as a contact component between gas and liquid, or is placed on the support plate in a random or whole-building mode, a packing press plate is arranged above the packing to press the packing, and then a liquid distributor is arranged above the packing. The working principle of the packed tower is as follows: the liquid is sprayed onto the filler from the upper part through the liquid distributor and flows down along the surface of each filler; the gas is fed from the bottom of the tower, is in a countercurrent state with the liquid, contacts with the liquid in the gap of the packing and has mass transfer.
The packed tower of the invention has basically the same structure as the packed tower and also comprises a tower shell, a packing support plate, packing, a liquid distributor and the like, but the working principle of the packed tower of the invention is different from the prior art, in the invention, smoke and soluble alkali liquor pass through the packing in a gas-liquid cocurrent flow mode, and in a preferable scheme, ozone also flows along with the soluble alkali liquor. The working principle of the packed tower of the invention is as follows: the flue gas enters from the upper part of the packed tower, passes through gaps among the packing and exits from the packed tower from a flue gas outlet; ozone enters the packing layer from the upper part of the packing layer; soluble alkali liquor enters the packing layer from the upper part of the packing layer, passes through gaps among the packing, finally flows to the bottom of the packed tower, and the bottom of the packed tower is used as an alkali liquor tank for collecting and storing the soluble alkali liquor. The flue gas, the ozone and the soluble alkali liquor contact and collide in the irregular gap channel of the filler to complete the reaction and absorption.
The first reason that the flue gas and the soluble alkali liquor flow downstream is adopted in the invention is that the media involved in the packed tower are as follows: flue gas, ozone and soluble alkali liquor are different from the traditional packed tower which only relates to two media of a gas and a liquid, and the reaction related to the packing is more complicated than the simple absorption reaction between the traditional packing. Firstly, the ozone and the soluble alkali liquor need to complete contact catalytic reaction, then oxidation reaction (between the ozone, active oxygen atoms and nitric oxide) needs to be carried out, and finally absorption reaction and mass transfer (between an oxidation product and the alkali liquor) need to be completed between gas and liquid, and the traditional countercurrent mode is difficult to well ensure the smooth operation of the reaction. When ozone, soluble alkali liquor and flue gas downstream pass through the filler gap, the route in this clearance is complicated various, can guarantee that flue gas, ozone and soluble alkali liquor have contact and reaction for a long time, accomplishes catalysis, oxidation reaction better in three's removal in-process.
The second reason for adopting gas-liquid cocurrent flow is that the actual conditions of tail gas of chemical plants, power plants, steel plants and the like are that the flue gas volume is large, the components are complex, and equipment with high mass transfer effect is difficult to adapt to the situation, for example, the existing wet desulphurization process usually adopts a spray tower instead of a packed tower and a plate tower. However, the flue gas and the liquid adopt a downstream route, so that the process requirements can be met, the air resistance can be reduced, the cost is saved, and the traditional packed tower can be applied to flue gas treatment occasions.
The filler in the invention can adopt the fillers related in the prior art, such as Raschig ring filler, pall ring filler, stepped ring filler, saddle-shaped filler, rectangular saddle-shaped filler and the like in bulk filler, and even can adopt spherical filler; grid packing, corrugated packing and the like in the regular packing. Considering the process environment, the material of the filler is preferably oxidation-resistant, acid-base-resistant, such as ceramic, stainless steel, PE, PP, PVC and other plastics, stainless steel and the like.
The liquid distributor of the present invention functions as in a conventional packed column. The distributor can be in the form of tube, double-layer calandria, slot, disk, impact, nozzle, tower, shower nozzle, etc. The soluble alkali liquor in the invention can be used in the above type according to the diameter of the packed tower; considering that the gas and the liquid are in a downstream state, the component can be omitted, and the liquid is directly injected into the packing layer through the liquid inlet pipe.
In a preferred scheme, the outlet of the ozone inlet pipe is arranged in the packing layer, namely, a layer of packing is arranged above the outlet of the ozone inlet pipe, so that the ozone is not contacted with the flue gas before contacting with the soluble alkali liquor, the ozone is not wasted, and the oxidation products in the flue gas can be completely absorbed.
2. Ozone and ozone generator
Ozone is generated by an ozone generator. The ozone generator can be a high-voltage discharge type ozone generator which is purchased or customized in the market. The oxygen source can be pure oxygen, and air can be directly used as the oxygen source for saving cost. It should be noted that, in the actual process, no matter ozone is generated by a pure oxygen source or an air source, pure ozone only occupies a certain proportion of gas, the proportion of the pure oxygen source is high, and the proportion of the air source is low. Thus, the present invention relates to processes using ozone, and the concept of ozone also includes ozone-containing gases.
3. Ozone supply system
The ozone supply system comprises an ozone generator, a gas booster pump, a valve, an air inlet pipe, an ozone distributor and the like. Which functions to supply ozone to the packed tower.
The ozone distributor is a device for distributing ozone generated by an ozone generator into flue gas of a packed tower. Ozone distributors as disclosed in the prior art, e.g. CN108905555A, CN 109173662A; conventional means such as conical, fan nozzles; or a simple taking pipe, such as a section of coil pipe, seals one end head, and then a plurality of small holes for spraying ozone are formed in the pipe body; or directly introducing ozone into the packing layer through the air inlet pipe orifice; and other devices that can perform the ozone disposing function.
The supply amount of ozone is specifically determined according to the content of NO in the flue gas and the ratio of ozone to NO.
Theoretically, 1 mole of ozone could oxidize and absorb more than 1 mole of NO according to the aforementioned reaction formula. However, considering the actual working condition, the molar ratio of the ozone to the NO is taken as follows: 1-5:1. The ozone generators are then purchased, or customized accordingly.
4. Soluble alkali liquor supply system
The soluble alkali in the present invention refers to a substance capable of ionizing hydroxide ions in water, and specifically includes substances capable of dissolving in water and ionizing hydroxide ions in water, such as sodium hydroxide, potassium hydroxide, calcium hydroxide, ammonia, alcohol amine, sodium carbonate, potassium carbonate, sodium bicarbonate, potassium bicarbonate, and urea.
Soluble lye refers to an aqueous solution of soluble alkali or a mixture of an aqueous solution and a part of soluble alkali.
The system comprises a lye tank, a pressure pump, a valve, a liquid inlet pipe and the like. The function is to convey the soluble alkali liquor to the liquid distributor through the liquid inlet pipe and then flow to the filler. And in consideration of the fact that the alkali liquor flowing through the filler has a larger pH value, the alkali liquor can be recycled, and the alkali liquor flowing under the filler laminar flow is collected into the alkali liquor tank and then is conveyed to the nozzle by the pressure pump for catalysis and absorption again. If the pH of the solution is lowered, it can be adjusted by adding a soluble base. The reaction product may be periodically withdrawn from the lye tank. A better definition of this system is: a soluble alkali liquor supply and circulation system.
OH of soluble base-The ion concentration is measured as pH. Experiments show that when the pH value reaches 9, the alkali liquor can catalyze and decompose ozone to oxidize NO in the flue gas, and under the condition of NO change under other conditions, the larger the pH value is, the quicker the NO can be removed, and the better the removal effect is. When the pH value is 14, the ozone can be quickly decomposed when contacting with soluble alkali liquor. The pH value is preferably in the range of 12 to 14 from the viewpoint of cost.
The soluble alkali liquor only plays a role of a catalyst in catalyzing the reaction of ozone, and has NO consumption, so that theoretically, the consumption of the soluble alkali liquor can be determined according to high-valence nitrogen oxides, and the high-valence nitrogen oxides are mainly converted from NO, so the consumption of the soluble alkali liquor is finally determined by the amount of NO in the flue gas. In practical application, the input amount of the alkali liquor in unit time can be 5-20 times of the input amount of the ozone in order to fully ensure the catalysis and absorption effects.
The invention has the beneficial effects that:
1. ozone is used for flue gas denitration, so that the cost is low and the efficiency is high;
2. the packed tower is applied to a flue gas denitration process, so that the technical bias is overcome;
3. the NO is oxidized by catalyzing ozone with lye, and oxidation products are absorbed by lye, which has unexpected technical effects.
4. The range of applicable flue gas temperature is large, such as being applicable to low-temperature flue gas; compared with the existing SCR denitration technology, the flue gas does not need to be heated, and the method has the advantage of huge cost.
Drawings
FIG. 1: a schematic diagram of a denitration system of a best mode.
FIG. 2: a structural form of an ozone distributor.
Detailed Description
The invention is described with reference to figures 1 and 2:
the packed column was a cylinder of diameter 0.8m, height 5m, wall thickness 8mm, and made of 304L stainless steel. The flue gas inlet 1 is arranged at the top of the packed tower, a 90-degree conical solid nozzle 2 is arranged at the upper part in the tower, the function of the nozzle 2 is equal to that of a liquid distributor, and the nozzle 2 is connected with a liquid inlet pipe 3 of soluble alkali liquor; the ozone distributor 3 is arranged below the nozzle 2, the ozone distributor 3 is positioned at the position of 0.5m below the nozzle 2, the ozone distributor 4 is a plane spiral pipe, and a plurality of small holes with the diameter of 1mm are uniformly formed in the lower part of the pipe and right opposite to the direction of the packing layer 6. The ozone distributor 4 is connected with an ozone inlet pipe 5, the ozone inlet pipe 5 is connected with an ozone generator 10, and a gas booster pump 11 and a flow regulating valve 12 are further arranged on the pipeline. The lower part of the ozone distributor 4 is provided with a packing layer 6, the packing is a ceramic raschig ring, the layer height of the packing layer 6 is 2m, and the packing is supported by a packing support plate 7. The flue gas outlet 8 is arranged at the position 0.8m below the packing support plate 7 and 0.6m away from the bottom of the tower, and the bottom of the packing tower is used as a lye tank 9. The pipeline of the liquid inlet pipe 3 of the soluble alkali liquor is provided with a booster pump 13 and a flow regulating valve 14, and the other end of the pipeline is connected to an alkali liquor tank 9 at the bottom of the packing tower.
The flue gas is the sintering flue gas of a sintering workshop of a certain steel mill. The initial flue gas parameters are:the smoke temperature is 133-135 ℃, the humidity of the smoke is 0.01-0.03 percent, and the NO content is 154-176mg/m3Oxygen content is 14-16%, and flue gas flow is 1800m3/h。
The ozone generator 10 is OZ type air source ozone generator produced by ozone purification equipment of Clarithroma of Islands, with ozone production of 500g/h and ozone concentration of 18-30g/m3. The soluble alkali solution is 0.5M sodium hydroxide solution.
The flue gas enters the packed tower through a flue gas inlet 1 and flows downwards from the top of the tower; starting the ozone generator 10, opening the flow regulating valve 11 and the booster pump 12, and conveying the ozone generated by the ozone generator 10 to the ozone distributor 4 through the air inlet pipe 5. The flow of the ozone is adjusted by the adjusting valve 11, so that the input quantity is not less than 400 g/h; meanwhile, an adjusting valve 14 and a booster pump 13 of the soluble alkali liquor input and circulation system are also opened, the alkali liquor in the alkali liquor tank 9 is conveyed to the nozzle 2 through the liquor inlet pipe 3, and the flow of the alkali liquor is adjusted through the adjusting valve 14, so that the input quantity per hour is not less than 5 kg.
Measured at the flue gas outlet 8 of the packed tower, the NO content is 24-32mg/m3。
Claims (6)
1. The utility model provides an utilize ozone and filled tower to carry out denitration system of flue gas denitration, including filled tower, ozone supply system, soluble alkali lye supply system, the inside packing layer that is equipped with of filled tower, ozone supply system carries ozone into filled tower through the intake pipe, soluble alkali lye supply system passes through the feed liquor pipe and carries soluble alkali lye into filled tower, a serial communication port, filled tower's flue gas import sets up the upper portion position at the packing layer, the exhanst gas outlet is established in the below of packing layer, the packing layer is arranged between exhanst gas inlet and exhanst gas outlet, the ozone mouth of pipe sets up the top at a packing layer that admits air, the feed liquor mouth of pipe of soluble alkali lye also sets up the upper portion position at the packing layer, ozone, soluble alkali lye contacts in the.
2. The denitration system for flue gas denitration using ozone and a packed tower as claimed in claim 1, wherein the ozone inlet pipe is located at a position below the inlet pipe of the soluble alkali solution.
3. The denitration system of flue gas using ozone and packed tower as claimed in claim 1, wherein the flow direction of ozone discharged from the inlet pipe orifice is the same as the flow direction of flue gas.
4. The denitration system for flue gas denitration using ozone and a packed tower according to claim 1, 2 or 3, wherein an ozone distributor is installed at an ozone inlet pipe.
5. The denitration system for flue gas denitration using ozone and a packed tower as claimed in claim 1, wherein the soluble alkali solution is discharged from the inlet pipe orifice in a spraying manner.
6. The denitration system for denitration of flue gas by using ozone and packed tower as claimed in claim 1, wherein a packing layer is further provided on the upper part of the ozone inlet pipe.
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