CN112090270B - Method for inhibiting generation of flue gas sulfur trioxide and cooperatively removing mercury - Google Patents
Method for inhibiting generation of flue gas sulfur trioxide and cooperatively removing mercury Download PDFInfo
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- CN112090270B CN112090270B CN202010892970.2A CN202010892970A CN112090270B CN 112090270 B CN112090270 B CN 112090270B CN 202010892970 A CN202010892970 A CN 202010892970A CN 112090270 B CN112090270 B CN 112090270B
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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
- 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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- A62—LIFE-SAVING; FIRE-FIGHTING
- A62D—CHEMICAL MEANS FOR EXTINGUISHING FIRES OR FOR COMBATING OR PROTECTING AGAINST HARMFUL CHEMICAL AGENTS; CHEMICAL MATERIALS FOR USE IN BREATHING APPARATUS
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- B01D53/34—Chemical or biological purification of waste gases
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- B01D53/64—Heavy metals or compounds thereof, e.g. mercury
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- A—HUMAN NECESSITIES
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- B—PERFORMING OPERATIONS; TRANSPORTING
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Abstract
The invention relates to a method for inhibiting generation of sulfur trioxide in flue gas and cooperatively removing mercury, which is characterized in that in a process section at a temperature higher than the dew point temperature of the sulfur trioxide, a sulfur-based compound agent is added to carry out surface vulcanization on fly ash and dust particles in the flue gas, and the vulcanized fly ash and dust enter low-temperature flue gas at downstream to cooperatively adsorb zero-valent mercury in the flue gas and are finally removed by a dust removal device. Compared with the prior art, the method can inhibit the generation of sulfur trioxide from the source, and the conversion rate of sulfur dioxide can be reduced to about 2 percent, so that the corrosion to equipment is reduced.
Description
Technical Field
The invention belongs to the field of environmental protection, mainly aims at the treatment of flue gas sulfur trioxide, and relates to a technical method for inhibiting the generation of the flue gas sulfur trioxide and cooperatively removing mercury.
Background
In the production process of the fields of coal burning, metallurgy, chemical industry and the like, sulfur dioxide (SO) is accompanied2) And the generation of acid gases, especially in the non-ferrous metal smelting industry, generally uses sulfide ores as raw materials, resulting in the generation of high sulfur dioxide flue gas in smelting flue gas. The metal oxides in the smoke dust such as fly ash generated in the burning process of the ore, such as ferric oxide, aluminum oxide and the like, have certain catalytic action on sulfur dioxide under the high-temperature condition, SO that the metal oxides are converted into sulfur trioxide (SO)3). When the temperature is lower than the dew point temperature of sulfur trioxide, the condensed sulfur trioxide is easy to cause the corrosion of smelting equipment and equipmentSuch as high-temperature corrosion of a water-cooled wall, low-temperature corrosion of a heating surface at the tail part of a flue, blockage of an SCR catalyst, blockage of an air preheater and the like, and the mercury removal efficiency in flue gas is reduced and the opacity of the flue gas is increased.
Meanwhile, the raw ore material is associated with mercury element, usually as granular mercury (Hg) in the production processp) Mercury (Hg) in its oxidized state2+) And zero-valent mercury (Hg)0) Three forms enter the flue gas, of which Hg ispAnd Hg2+Is easy to be removed by the existing dust removing device and the existing desulphurization or washing device, and Hg is easily removed0It is difficult to capture the conversion by existing devices. Because of Hg0The high-volatility high-toxicity methyl mercury has the characteristics of high volatility, high toxicity, easy migration and the like, once the high-toxicity methyl mercury enters the atmosphere, the high-toxicity methyl mercury is easy to enrich in organisms once the high-volatility high-toxicity methyl mercury easily migrates in the global range and enters water environments in the processes of dry sedimentation, wet sedimentation and the like, and the high-toxicity methyl mercury is formed through biotransformation and seriously harms human health, so that the mercury is listed as a global pollutant. The united nations formally issued international "water guarantee on mercury" in 2013, aiming at enhancing the control strength on mercury (especially atmospheric mercury) emission. China has formally become the contracting country of the convention in 2016 and bears huge mercury emission reduction pressure.
In the traditional smelting process flow, the flue gas is conveyed to the downstream after passing through a waste heat boiler and undergoes the processes of dust removal, dynamic wave washing, two-conversion and two-absorption acid making and the like in sequence. Large amount of oxidation state Hg in dynamic wave washing process2+And SO3Is washed off to form "dirty acid", however, SO3In the process of conveying from a high-temperature flue gas section of the waste heat boiler to a low-temperature flue gas section of dynamic wave washing, the temperature is lower than the dew point of the high-temperature flue gas section, and the high-temperature flue gas section is inevitably condensed into acid mist, so that equipment is corroded and damaged, and the operation cost is greatly increased.
Therefore, the temperature of the molten metal is controlled,
disclosure of Invention
The invention aims to overcome the defects in the prior art and provide a method for inhibiting the generation of flue gas sulfur trioxide and cooperatively removing mercury, aiming at the problem of corrosivity of nonferrous smelting flue gas sulfur trioxide, the method for directly inhibiting the conversion of sulfur dioxide in a high-temperature flue gas section is developed, the generation of sulfur trioxide can be effectively reduced from the source, and simultaneously, the zero-valent mercury in the flue gas is collected.
The purpose of the invention can be realized by the following technical scheme: a method for inhibiting generation of sulfur trioxide in flue gas and cooperatively removing mercury is characterized in that in a process section with the temperature higher than the dew point temperature (generally greater than 180 ℃) of the sulfur trioxide, a sulfur-based compound agent is added to carry out surface vulcanization on fly ash and dust particles in the flue gas, so that catalytic conversion of components such as iron oxide, aluminum oxide and the like in the flue gas on sulfur dioxide is inhibited, generation of the sulfur trioxide is inhibited, and the vulcanized fly ash and dust enter low-temperature flue gas to cooperatively adsorb zero-valent mercury in the flue gas and are finally removed through a dust removal device.
The sulfur-based compound agent reacts with metal oxides in the fly ash at high temperature to generate metal sulfides such as iron oxide and the like, and then iron sulfide and the like are generated.
Further, the sulfur-based compound agent comprises one or more of a solid compound agent, a liquid compound agent or a gas compound agent.
Furthermore, the solid compound agent comprises one or more of elemental sulfur, ammonium sulfide, sodium peroxide, thiourea, thioacetamide and the like, the liquid compound agent comprises carbon disulfide, the gas compound agent comprises hydrogen sulfide, and the vulcanization effect can be enhanced by adopting a gas-solid combination, a gas-liquid combination or a solid-liquid combination.
The process section higher than the dew point temperature of sulfur trioxide is a waste heat boiler process section, the flue gas temperature is 400-500 ℃, and the temperature is higher than the dew point temperature of sulfur trioxide.
The sulfur-based compound agent enters a waste heat boiler in a spraying mode.
The dosage of the sulfur-based compound agent is related to the concentration of sulfur dioxide in flue gas and the content of smoke dust, and the addition amount of the compound agent is 5-20 wt% of the concentration of sulfur dioxide in the flue gas.
Active sulfur sites (S) are generated on the surfaces of the vulcanized fly ash and the vulcanized dust, have high affinity to mercury, and synergistically adsorb zero-valent mercury in flue gas to form stable HgS on the surfaces of particles, so that the stable HgS is removed by a dust removal device.
Specifically, the method provided by the invention is used for inhibiting the generation of sulfur trioxide by adding a sulfur-based compound agent in a process section of a waste heat boiler, and mainly comprises the following steps:
the first step is as follows: selecting a sulfur-based compound agent and selecting a proper dosage;
the second step is that: selecting a proper smoke opening in a high-temperature smoke section, namely a waste heat boiler, and spraying the selected compound agent;
the third step: the compound agent and fly ash, dust and the like in the flue gas generate a vulcanization reaction, so that components such as ferric oxide, aluminum oxide and the like in the flue gas, which have a catalytic conversion effect on sulfur dioxide, lose activity, and the generation of sulfur trioxide is inhibited;
the fourth step: meanwhile, active sulfur sites generated on the surfaces of fly ash and dust particles in the flue gas adsorb zero-valent mercury in the flue gas, and the active sulfur sites are converted into HgS attached to the surfaces of the particles;
the fifth step: fly ash and dust are finally removed by a dust removal device.
Compared with the prior art, the invention has the following advantages:
1. prior art SO scrubbing by dynamic wave3Leaching into polluted acid, inevitably washing with SO3The invention is directly carried out in SO to corrode equipment by condensation in the flue gas conveying process3The sulfur-based compound agent is added in the generation stage, SO that SO is fundamentally inhibited3Generation of (1);
2. the method does not need to be provided with a separate device for removing SO3The injection port is only needed to be arranged at the process section of the waste heat boiler, the temperature of the waste heat boiler is generally 400-plus-500 ℃ and is higher than the dew point temperature of sulfur trioxide, the added sulfur-based compound agents in the waste heat boiler are all reductive sulfides which are higher than sulfur dioxide and are easier to react with metal oxides in flue gas, and the oxidation activity of the metal oxides can be fully exerted at high temperature to carry out morphological conversion on sulfur.
3. The sulfur-based compound agent adopted by the method directly reacts with particulate matters in the flue gas, does not generate secondary pollutants, has the advantage of environmental friendliness, and has no problems of secondary pollution and the like;
4. the sulfuration fly ash and the dust generated by the method can cooperatively remove zero-valent mercury in the flue gas, and are finally removed by a dust removal device.
Drawings
FIG. 1 is a flow chart of the method of the present invention.
Detailed Description
The invention is described in detail below with reference to the figures and specific embodiments.
As shown in FIG. 1, the method of the present invention for inhibiting the generation of sulfur trioxide by adding a sulfur-based compound agent in the process stage of a waste heat boiler mainly comprises the following steps:
the first step is as follows: the non-ferrous smelting flue gas flows out from the fluidized bed furnace 1 and enters a spraying temperature section 2 of the compound agent, the main equipment of the adjusting stage is a waste heat boiler, the temperature of the non-ferrous smelting flue gas is 400-2，Hg0Fly ash and other particles, in the high temperature section, SO is easily generated in the prior art2+O2→SO3The waste heat boiler is provided with a flue gas opening, and the sulfur-based compound agent is sprayed in through the flue gas opening;
the second step is that: selecting a proper smoke opening in a waste heat boiler, and spraying the selected sulfur-based compound agent;
the third step: the sulfur-based compound agent and fly ash, dust and the like in the flue gas generate a vulcanization reaction, so that components such as ferric oxide, aluminum oxide and the like in the flue gas, which have a catalytic conversion effect on sulfur dioxide, lose activity, and the generation of sulfur trioxide is inhibited;
the fourth step: meanwhile, active sulfur sites (S) are generated on the surfaces of fly ash and dust particles in the flue gas, zero-valent mercury in the flue gas is adsorbed and converted into HgS which is attached to the surfaces of the particles;
the fifth step: fly ash and dust are finally removed by a dust removal device 3;
and a sixth step: the flue gas after dust removal contains SO2And a small amount of SO3A small amount of SO is input into the dynamic wave washing tower 43Is leached to form 'dirty acid', and the rest contains SO2The mixed flue gas enters a flue gas acid making section 5 for post-treatment。
Example 1:
(1) the impregnation method is adopted to prepare 10 percent Fe2O3Loading a ZSM-5 molecular sieve to simulate a flue gas fly ash component;
(2) the fixed bed is adopted to simulate the actual flue gas condition, the mass of the catalyst is 5g, and the SO is imported2The concentration is 1000ppm, the oxygen concentration is 10 percent, the flow rate is 500mL/min, and the reaction temperature is 500 ℃. The preheating boiler is not sprayed with sulfur-based compound (the rest is the same as the invention) and SO3The stable yield was about 7% (yield was determined to be 7.18, 7.02, 6.51, 7.29% per 10 h).
(3) Selection of H2S is used as gas sulfur-based compound agent and treated by the method of the invention, and when an inlet H is adopted2When the concentration of S is 50, 100 and 200ppm, the outlet SO3The yields were reduced to 5.3, 3.9, 2.1% (three average yields), respectively.
It can be seen that the addition of the sulfur-based combination agent can greatly reduce SO3Yield.
Example 2:
(1) selecting CS2As liquid sulfur-based compounding agents, CS2Can be injected directly or through N in liquid form2The carrier gas is injected in a gaseous state under the condition of a certain water bath temperature;
(2) the fixed bed is adopted to simulate the actual flue gas condition, the mass of the catalyst is 5g, and the SO is imported2The concentration is 1000ppm, the oxygen concentration is 10 percent, the flow rate is 500mL/min, and the reaction temperature is 500 ℃.
(3) When CS is used2Injecting into inlet simulation flue gas in gaseous form, inlet CS2Outlet SO at concentration of 100, 200, 300ppm3The yield was reduced to 6.0, 3.3, 1.8% (three average yields), respectively.
Example 3:
(1) selection of Na2S and simple substance S are used as solid sulfur-based compound agents, and different Na is adopted2The molar ratio of S to simple substance S (1: 0, 1: 1, 1: 2, 1: 3) is mixed with the Fe2O3The supported molecular sieve catalyst is sulfided.
(2) The mass of the catalyst is 5g, the vulcanization temperature is 100 ℃, and the vulcanization time is 1 h. And after the vulcanization is finished, obtaining the vulcanization catalyst through the steps of suction filtration, washing and drying.
(3) The fixed bed is adopted to simulate the actual flue gas condition, the mass of the sulfuration catalyst is 5g, and the SO is imported2The concentration is 1000ppm, the oxygen concentration is 10 percent, the flow rate is 500mL/min, and the reaction temperature is 500 ℃.
When Na is present2When the S/S molar ratio is (1: 0, 1: 1, 1: 2, 1: 3), the SO is discharged3The conversion decreased to 6.4, 5.5, 4.0, 2.8% (three average yields), respectively.
Claims (4)
1. A method for inhibiting the generation of sulfur trioxide in flue gas and cooperatively removing mercury is characterized in that in a process section at a temperature higher than the dew point temperature of the sulfur trioxide, a sulfur-based compound agent is added to carry out surface vulcanization on fly ash and dust particles in the flue gas, and the vulcanized fly ash and dust enter low-temperature flue gas at downstream to cooperatively adsorb zero-valent mercury in the flue gas and are finally removed by a dust removal device; the sulfur-based compound agent enters a waste heat boiler in a spraying mode; the addition amount of the sulfur-based compound agent is 5-20 wt% of the concentration of sulfur dioxide in the flue gas;
the process section higher than the dew point temperature of sulfur trioxide is a waste heat boiler process section, the flue gas temperature is 400-500 ℃, and the temperature is higher than the dew point temperature of sulfur trioxide; active sulfur sites (S) are generated on the surfaces of the vulcanized fly ash and the vulcanized dust, have high affinity to mercury, and synergistically adsorb zero-valent mercury in the flue gas to form stable HgS on the surfaces of particles, so that the stable HgS is removed by a dust removal device;
the flue gas is non-ferrous smelting flue gas, enters a waste heat boiler, and is sprayed with a sulfur-based compound agent, wherein the sulfur-based compound agent inhibits the catalytic conversion of iron oxide and aluminum oxide components in the flue gas on sulfur dioxide, so that the generation of sulfur trioxide is inhibited, and meanwhile, mercury is adsorbed on the surfaces of fly ash and dust particles in the flue gas and then removed by a dust removal device.
2. The method for inhibiting the generation of sulfur trioxide in flue gas and synergistically removing mercury according to claim 1, wherein said sulfur-based combination agent reacts with metal oxides in fly ash to form metal sulfides under high temperature conditions.
3. The method of claim 1, wherein the sulfur-based combination comprises one or more of a solid combination, a liquid combination, or a gaseous combination.
4. The method for inhibiting generation of sulfur trioxide in flue gas and synergistically removing mercury according to claim 3, wherein the solid compound comprises one or more combinations of elemental sulfur, ammonium sulfide, sodium persulfate, thiourea, thioacetamide, and the like, the liquid compound comprises carbon disulfide, the gaseous compound comprises hydrogen sulfide, and the use of the method can be in a gas-solid combination, a gas-liquid combination or a solid-liquid combination to enhance the effect of vulcanization.
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