CN111111414A - Denitration system for flue gas denitration by using hydrogen peroxide and cyclone disc tower - Google Patents
Denitration system for flue gas denitration by using hydrogen peroxide and cyclone disc tower Download PDFInfo
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- CN111111414A CN111111414A CN202010035563.XA CN202010035563A CN111111414A CN 111111414 A CN111111414 A CN 111111414A CN 202010035563 A CN202010035563 A CN 202010035563A CN 111111414 A CN111111414 A CN 111111414A
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- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
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- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
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Abstract
The invention discloses a denitration system for denitration of flue gas by using hydrogen peroxide and a rotational flow disc tower, which comprises the rotational flow disc tower, a hydrogen peroxide supply system and a soluble alkali liquor supply system, wherein a rotational flow disc is arranged in the rotational flow disc tower, the hydrogen peroxide and the soluble alkali liquor flow onto the rotational flow disc from an outlet and are mixed on the rotational flow disc to form a mixed liquid layer, the mixed liquid layer meets flue gas rising from a gap of the rotational flow disc to form gas-liquid rotational flow, and the flue gas, the hydrogen peroxide and the soluble alkali liquor in the rotational flow liquid react and transfer mass. The invention applies hydrogen peroxide and the cyclone disc tower to flue gas denitration, has low cost and high efficiency, and has great economic benefit and social benefit.
Description
Technical Field
The invention relates to the technical field of flue gas denitration, in particular to a flue gas denitration system by utilizing hydrogen peroxide and a cyclone disc 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. For the catalytic reduction method, the required working temperature range is 400-450 ℃, and the emission temperature of the process flue gas is lower than the temperature, for example, the temperature of the boiler flue gas of a power plant, the sintering furnace flue gas of an iron and steel plant, and the flue gas of other boilers is usually between 80-150 ℃, so that extra energy consumption is needed to increase the temperature of the flue gas. In addition, because the reducing agent adopts ammonia gas, excessive reducing agent can be released into the atmosphere, secondary pollution can be caused finally, and moreover, the catalyst adopts precious metal and is easy to age. Therefore, the denitration cost by the reduction method is high; the oxidation methods disclosed in the prior art include ozone oxidation, sodium hypochlorite oxidation, etc., and the main disadvantages of these methods are poor removal effect of nitrogen oxides, too high cost, and great difficulty in treating the oxidation products (such as sodium hypochlorite method), thus having great disadvantages. In the existing flue gas denitration process, mature technology is rarely popularized and applied. The hydrogen peroxide has certain oxidizability and low price, and is a clean oxidant, so the hydrogen peroxide is applied to flue gas denitration and has a great prospect. However, experimental results show that the simple hydrogen peroxide has poor effect of oxidizing low-concentration NO in the flue gas. In the prior art, when hydrogen peroxide is applied to flue gas denitration, the measures adopted are that hydrogen peroxide is catalyzed at high temperature to generate hydroxyl radicals, and NO in flue gas is oxidized by the hydroxyl radicals. The publication No. CN106582277A discloses a denitration system and method using catalytic hydrogen peroxide, which uses titanium-based catalyst loaded with iron element to generate hydroxyl radical to oxidize NO at the temperature of 160-240 ℃. Patent publication No. CN106861392 discloses a process for removing nitrogen oxides based on hydrogen peroxide catalytic oxidation, wherein the adopted activating catalyst is oxides such as cerium dioxide, cobaltosic oxide, nickel oxide and the like, and the carrier is titanium dioxide. Hydroxyl radicals are generated to oxidize NO at the high temperature of 100 ℃ and 300 ℃. The above-mentioned technology has the problem that the applicable temperature is higher, so as to ensure the generation of hydroxyl free radical, thus extra energy consumption is needed to raise the flue gas temperature; noble metal oxide or noble metal is used as a catalyst, so that the cost is high; in addition, most of the hydrogen peroxide in the flue gas is directly decomposed into water and oxygen at a higher temperature instead of hydroxyl radicals, so that a large amount of hydrogen peroxide is additionally consumed, and the cost is increased.
Disclosure of Invention
In order to solve the technical problems, the invention provides a denitration system for flue gas denitration by using hydrogen peroxide and a cyclone disc tower, which comprises the following contents:
a denitration system for denitration of flue gas by using hydrogen peroxide and a cyclone disc tower comprises the cyclone disc tower, a hydrogen peroxide supply system and a soluble alkali liquor supply system, wherein a cyclone disc is arranged in the cyclone disc tower, the hydrogen peroxide supply system conveys hydrogen peroxide into the cyclone disc tower through a water inlet pipe, the soluble alkali liquor supply system conveys soluble alkali liquor into the cyclone disc tower through a liquid inlet pipe, and the denitration system is characterized in that an outlet of the hydrogen peroxide water inlet pipe is positioned at the upper part of the cyclone disc, an outlet of the soluble alkali liquor liquid inlet pipe is also positioned at the upper part of the cyclone disc, the hydrogen peroxide and the soluble alkali liquor flow onto the cyclone disc from the outlet and are mixed to form a mixed liquid layer, the mixed liquid layer meets flue gas rising from gaps of blades of the cyclone disc to form gas-liquid cyclone, the flue gas, the hydrogen peroxide and the soluble alkali liquor react and transfer mass in the cyclone liquid, and then the flue gas continuously rises, the mixed liquid flows from the wider gap of the periphery of the cyclone disk to the lye tank below.
Preferably, the outlet of the hydrogen peroxide water inlet pipe and the outlet of the soluble alkali liquor are the same outlet.
Preferably, the outlet position of the soluble alkali liquor and the hydrogen peroxide is positioned above the center of the cyclone disk.
Preferably, the center of the spinning disk is a solid disk.
Preferably, a cooling device for the soluble alkali liquor is also arranged in the soluble alkali liquor supply system.
The invention content is explained in the following with the prior art:
theoretical basis of the invention
1. Oxidation of NO:
the prior art shows that hydrogen peroxide by itself is not capable of oxidizing low concentrations of NO in flue gas (see US7628967B 2). Experiments also show that when the hydrogen peroxide is neutral or acidic, the hydrogen peroxide is very stable, and the flue gas containing NO with lower concentration is contacted with the acidic or neutral hydrogen peroxide, so that the NO cannot be oxidized by the hydrogen peroxide.
However, experiments show that hydrogen peroxide can be quickly decomposed in an alkaline solution, and NO in the flue gas can be well removed when the flue gas containing low-concentration NO is contacted with a mixed solution of alkali liquor and hydrogen peroxide. The reason for this is OH in the alkaline solution-The ions catalyze the decomposition of hydrogen peroxide:
H2O2= H2O + O——
O + O = O2——
O + O2= O3——
o produced during the decomposition of hydrogen peroxide2O and O3Collectively referred to as active oxygen.
The active oxygen formed after catalysis plays a role in oxidizing NO:
O + NO → NO2——④
NO + O + NO → N2O3——⑤
O3+ NO →NO2+ O2——⑥
2NO + O2→ 2NO2(Low temperature) - ⑦
In the above reaction, oxygen atoms have a larger oxidizing property than oxygen, and thus it is easy to oxidize nitrogen monoxide into nitrogen dioxide and other nitrogen oxides; in addition, the oxygen atom may be additionally bonded to O2Generation of O3And O is3Also has large oxidizing property, and can oxidize NO into NO2(ii) a Even if it is O2Since the oxidation reaction is generated in an aqueous solution of a soluble base and the temperature is low, NO can be oxidized into NO in the solution2.
Therefore, in alkaline solutions, the active oxygen is able to oxidize NO in the flue gas.
2. Absorption of high-valence nitrogen oxides:
in the presence of OH-In the presence of an environment in which NO is oxidized to NO2After then, NO2It is immediately absorbed by soluble alkali and converted into nitrate and nitrite.
The reaction formula is as follows:
3NO2+ 2OH-→ 2NO3 -+ H2O + NO——⑧
NO2+ NO + 2OH-→ 2NO2 -+ H2O——⑨
the oxidation and absorption are transient, i.e. NO is absorbed by the soluble base immediately after oxidation. In addition, except for NO2In addition, very small amounts of N in the flue gas2O3The nitrogen oxides with high valence also react with soluble alkali to produce nitrate, etc.
The whole denitration technology comprises the following steps:
in aqueous solution of soluble base, due to OH-The hydrogen peroxide decomposes active oxygen under the catalytic action of ions; the active oxygen oxidizes NO into high-valence nitrogen oxide which can be absorbed by alkali liquor or water; meanwhile, in the aqueous solution, the soluble alkali reacts with the high-valence nitrogen oxide immediately to generate nitrate or nitrous acid. Thereby completing the removal of the nitrogen oxides in the flue gas. That is, there are two types of reactions: catalytic decomposition of hydrogen peroxide and absorption of nitrogen oxides, and both reactions occur in aqueous solution. Moreover, the soluble lye serves two functions: catalysis and absorption.
The technical idea is obviously different from the technical idea of the prior art.
(II) cyclone disc tower
The cyclone disc tower is a place for realizing the technical idea in the denitration system. The cyclone disc tower is composed of a cyclone disc and a tower shell, wherein the cyclone disc is arranged in the tower shell and is positioned above the flue gas inlet and below the soluble alkali liquor inlet. The whirl dish can adopt to be applied to among the prior art to the whirl dish of gaseous whirl, and its concrete structure is: a circular tower tray is composed of several cyclone blades uniformly arranged in radial shape from center to periphery of tray, and the blades are made of thin plate and have an angle with tower axis, and the gap between two blades is a flue gas channel, and the gap is correspondent to the blade and also has an inclination angle with tower axis. The cavity of the slit gradually increases from the center to the periphery. In order to be convenient to manufacture and install, the periphery of the blade is a circular ring, and the periphery of the blade is welded on the circular ring. Or the blades can be sequentially and directly welded on the inner wall of the tower shell at a certain position of the inner wall of the tower shell to form a spiral-flow disk.
In a preferred scheme, the central point of whirl dish puts and sets solid construction into, and the purpose is in better accepting liquid to make both better homogeneous mixing, also can not lead to liquid too early through the gap between the blade, influence flue gas denitration effect.
FIGS. 2-5 also show the construction of the spinning disk
In the prior art, the cyclone disc is usually applied to gas cyclone, but in the invention, the cyclone disc tower is used for flue gas denitration, which can achieve unexpected technical effects. The reason is that the cyclone disk not only has the effect of gas cyclone, but also can swirl the liquid at the upper part, and can better stir and mix the gas and the liquid, thereby enhancing the gas-liquid contact, reaction and mass transfer effects.
(III) Hydrogen peroxide solution supply System
The system comprises a hydrogen peroxide tank, a pressure pump, a valve, a water inlet pipe and the like. The device has the function of supplying hydrogen peroxide to the cyclone disc tower, and delivering the hydrogen peroxide to the upper position of the cyclone disc through the water inlet pipe. The supply amount of the hydrogen peroxide is specifically set according to the content of NO in the flue gas and the concentration of the hydrogen peroxide. According to the formula
④ and ⑧ and H2O2In a molar ratio of 1: relation of 1, i.e. an H2O2Can absorb 1 NO, but according to
④, ⑤ and ⑨ and H2O2Is less than 1:1, which can use a smaller amount of hydrogen peroxide. Considering the consumption of hydrogen peroxide and the formula
And ⑦, in the process, the amount is generally 1:1, but in any case, hydrogen peroxide has great cost and environmental advantages compared with other oxides to oxidize NO.
The hydrogen peroxide solution is called as hydrogen peroxide aqueous solution in the invention. Commercial products are available in the market, mainly 35wt% and 27.5 wt%. During denitration, industrial products can be directly used, and hydrogen peroxide can be diluted by water for use, such as to 20wt%, 15wt%, and even less than 10 wt%.
(IV) 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.
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 upper position of the cyclone disk.
Considering that the alkali liquor reacts on the spiral-flow disk, the outlet position of the soluble alkali liquor and the outlet position of the hydrogen peroxide solution are not suitable to be separated by a long distance, in a preferred scheme, after the soluble alkali liquor inlet pipe and the hydrogen peroxide solution inlet pipe are connected in parallel, a common outlet is used for conveying the mixed liquor of the hydrogen peroxide solution and the soluble alkali liquor to the spiral-flow disk. However, according to the above reaction mechanism, it is not desirable to combine the hydrogen peroxide and the soluble alkali solution prematurely, for example, the combining pipe is located outside the tower and far from the outlet, which causes the hydrogen peroxide to decompose before contacting the flue gas, and therefore, the combining pipe is generally preferably located inside the tower.
In addition, the sprayed alkali liquor has a larger pH value, so that the alkali liquor can be recycled. And collecting the alkali liquor flowing down from the gaps of the rotational flow blades to an alkali liquor tank, conveying the alkali liquor to a nozzle by a pressure pump, and catalyzing and absorbing the alkali liquor again. If the pH is lowered, a soluble base may be added for adjustment. 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, NO in the flue gas can be oxidized, and under the condition of NO change under other conditions, the larger the pH value is, the better the NO removal effect is. When the pH value is 11, the denitration rate of NO can exceed 70%, and when the pH value reaches 12, the denitration rate of NO exceeds 83%. 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 the reaction of catalyzing hydrogen peroxide, 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 that the consumption of the soluble alkali liquor is finally determined by the amount of NO in the flue gas. In practical application, in order to fully ensure the catalysis and absorption effects, the unit spraying amount of the alkali liquor can be 2-20 times of the input amount of the hydrogen peroxide.
In addition, the hydrogen peroxide can be decomposed (water and oxygen are generated) at a high temperature (about 60 ℃ at normal pressure), and if the temperature of the alkali liquor in the mixer is too high, the hydrogen peroxide can be additionally consumed before being sprayed out of the nozzle. The soluble alkali liquor is contacted with the flue gas in circulation, and a large amount of heat can be absorbed from the flue gas, so that the temperature is increased. In order to solve the technical problem, in a preferred scheme, the adopted measures are that the soluble alkali liquor is cooled by adopting a cooling method, the cooling method is a conventional method, and a condensing pipe can be arranged in an alkali liquor tank; a jacket can be arranged outside the lye tank; a heat exchanger and the like can be arranged on the alkali liquor circulation path; the cooling medium may be cold water, cold air, etc., and is preferably at a temperature of less than 60 deg.C, 50 deg.C, or even lower in the mixer. This is obviously different from the technical idea of patent publication No. CN106582277A and publication No. CN 106861392.
At this time, the soluble alkali liquor plays a third role: namely, the temperature of the flue gas is reduced, which is beneficial to the subsequent processes of the flue gas, such as the capture of carbon dioxide, the dust removal of the flue gas and the like.
The invention has the beneficial effects that:
1. the hydrogen peroxide is used for flue gas denitration, and the method is low in cost and high in efficiency.
2. The cyclone disc tower is used for flue gas denitration, and the contact, reaction and mass transfer effects between gas and liquid are enhanced.
3. The NO is oxidized by catalyzing hydrogen peroxide with alkali liquor, and the oxidation product is absorbed by the alkali liquor, so that NO additional catalyst is needed, the cost is low, and unexpected technical effects are achieved.
4. The range of applicable flue gas temperature is large, the flue gas is particularly suitable for low-temperature flue gas, and the lower the flue gas temperature is, the better the denitration effect is; compared with the prior art, the flue gas does not need to be heated, and has huge cost advantage.
Drawings
FIG. 1: the denitration system of the embodiment is schematically shown.
FIG. 2: top view of the spinning disk in the examples.
FIG. 3: right side view of the swirl disk in the examples
FIG. 4: top view of the blade in the example.
FIG. 5: left side view of the blade in the example.
FIG. 6: the connection relationship of the blades and the solid disc is shown in the drawing (A).
FIG. 7: and (B) a schematic diagram of the connection position relation of the outer ring.
Best mode for carrying out the invention
The invention is described with reference to the accompanying figure 1:
the cyclone disk tower is a cylinder with the diameter of 0.8m, the height of the tower is 5m, the wall thickness is 8mm, and the tower is made of 304L stainless steel. The cyclone disk 1 is arranged at a position 2.5 meters away from the bottom of the tower shell. The diameter of the outer ring 2 of the cyclone disk 1 is 790mm, and the cyclone disk is connected with the tower shell by spot welding. The center of the cyclone disk 1 is a solid disk 3 with a diameter of 150 mm. The thickness of the blades 4 is 6mm, the total number of the blades is 36, the blades are uniformly arranged between the solid disc 3 and the outer ring 2, and the included angle between the blades 4 and the horizontal direction is 36 degrees.
The flue gas is the sintering flue gas of a sintering workshop of a certain steel mill. The initial flue gas parameters are: the temperature of the smoke is 125-3Total nitrogen oxide content 239-276mg/m3Oxygen content is 14-16%, and flue gas flow is 1800m3/h。
The concentration of the hydrogen peroxide is 35 wt%. The soluble alkali is NaOH, and is adjusted to be an aqueous solution with pH value of 14 and then injected into the lye tank 7.
The flue gas enters the cyclone disc tower through the flue gas inlet 5, rises in the tower, passes through the gaps of the blades 4 of the cyclone disc to form cyclone, then rises again, and exits the tower from the flue gas outlet 6. The flow regulating valve 11-a of the hydrogen peroxide pipeline is opened, the booster pump 10-a is started, and the hydrogen peroxide in the hydrogen peroxide tank 9 is conveyed to the solid disc 3 through the water inlet pipe 8. The flow of the hydrogen peroxide is adjusted by the adjusting valve 11-a, so that the hydrogen peroxide is uniformly input, and the input quantity per hour is not lower than 3 kg; meanwhile, an adjusting valve 11-b and a booster pump 10-b of the soluble alkali liquor input and circulation system are also opened, the alkali liquor in the alkali liquor tank 7 is also conveyed to the solid disc 3 of the spiral-flow disc 1 through a liquor inlet pipe 12, and the flow of the alkali liquor is adjusted through the adjusting valve 11-b, so that the input quantity per hour is ensured to be 30 kg.
The hydrogen peroxide and the soluble alkali liquor on the solid disc 3 are mixed and transversely diffused to the periphery. The cyclone is formed under the effect of the lifting force of the flue gas in the gaps of the blades 4, and the flue gas continuously diffuses to the periphery, and flows downwards under the action of gravity and finally converges to the bottom of the tower due to the increase of the gap when the flue gas flows to the gaps of the blades 4 close to the wall of the tower shell.
On the cyclone disk 1, the flue gas and the liquid are mixed to form a gas-liquid mixed cyclone layer, and in the cyclone layer, the contact, reaction and mass transfer among the flue gas, the hydrogen peroxide and the alkali liquor are completed.
Measured at the flue gas outlet 6 of the cyclone disc tower, the NO content is 13-27mg/m3The total content of nitrogen oxides is 19-41mg/m3。
Claims (5)
1. A denitration system for denitration of flue gas by using hydrogen peroxide and a cyclone disc tower comprises the cyclone disc tower, a hydrogen peroxide supply system and a soluble alkali liquor supply system, wherein a cyclone disc is arranged in the cyclone disc tower, the hydrogen peroxide supply system conveys hydrogen peroxide into the cyclone disc tower through a water inlet pipe, the soluble alkali liquor supply system conveys soluble alkali liquor into the cyclone disc tower through a liquid inlet pipe, and the denitration system is characterized in that an outlet of the hydrogen peroxide water inlet pipe is positioned at the upper part of the cyclone disc, an outlet of the soluble alkali liquor liquid inlet pipe is also positioned at the upper part of the cyclone disc, the hydrogen peroxide and the soluble alkali liquor flow onto the cyclone disc from the outlet and are mixed to form a mixed liquid layer, the mixed liquid layer meets flue gas rising from gaps of blades of the cyclone disc to form gas-liquid cyclone, the flue gas, the hydrogen peroxide and the soluble alkali liquor react and transfer mass in the cyclone liquid, and then the flue gas continuously rises, the mixed liquid flows from the wider gap of the periphery of the cyclone disk to the lye tank below.
2. The denitration system for flue gas denitration by using hydrogen peroxide and the cyclone tray tower as claimed in claim 1, wherein the outlet of the hydrogen peroxide inlet pipe and the outlet of the soluble alkali liquor are the same outlet.
3. The denitration system for flue gas denitration by using hydrogen peroxide and the cyclone disk tower as claimed in claim 1, wherein the outlet positions of the soluble alkali solution and the hydrogen peroxide are positioned above the center of the cyclone disk.
4. The denitration system for flue gas denitration by using hydrogen peroxide and a cyclone disk tower according to claim 3, wherein the center of the cyclone disk is a solid disk.
5. The denitration system for denitration of flue gas by using hydrogen peroxide and a spray tower as claimed in claim 1, wherein a cooling device for the soluble alkali solution is further provided in the soluble alkali solution supply system.
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