CN113877391A - Composite additive for selective non-catalytic reduction denitration of flue gas and preparation method and application thereof - Google Patents

Composite additive for selective non-catalytic reduction denitration of flue gas and preparation method and application thereof Download PDF

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CN113877391A
CN113877391A CN202010624969.1A CN202010624969A CN113877391A CN 113877391 A CN113877391 A CN 113877391A CN 202010624969 A CN202010624969 A CN 202010624969A CN 113877391 A CN113877391 A CN 113877391A
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percent
equal
flue gas
urea
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CN113877391B (en
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胡兵
师本敬
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Zhongye Changtian International Engineering Co Ltd
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • 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
    • B01D53/77—Liquid phase processes
    • B01D53/78—Liquid phase processes with gas-liquid contact
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • 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
    • B01D53/46—Removing components of defined structure
    • B01D53/54—Nitrogen compounds
    • B01D53/56—Nitrogen oxides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • 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
    • B01D53/86—Catalytic processes
    • B01D53/8621—Removing nitrogen compounds
    • B01D53/8625—Nitrogen oxides
    • B01D53/8628—Processes characterised by a specific catalyst
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2251/00—Reactants
    • B01D2251/20—Reductants
    • B01D2251/206—Ammonium compounds
    • B01D2251/2062—Ammonia
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2251/00—Reactants
    • B01D2251/20—Reductants
    • B01D2251/206—Ammonium compounds
    • B01D2251/2067—Urea
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/20—Metals or compounds thereof
    • B01D2255/207—Transition metals
    • B01D2255/20707—Titanium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/20—Metals or compounds thereof
    • B01D2255/207—Transition metals
    • B01D2255/20723—Vanadium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2258/00—Sources of waste gases
    • B01D2258/02—Other waste gases
    • B01D2258/0283—Flue gases

Abstract

The invention discloses a composite additive for selective non-catalytic reduction denitration of flue gas, which is prepared by compounding urea, NaCl, ethanol, a vanadium-titanium catalyst and an SBA-15 material. When the composite additive is used, 0.1-2.0 wt% of composite additive is added into a pellet flue gas denitration reducing agent. Then spraying the mixture on a transition section between the chain grate machine and the rotary kiln and/or a preheating two-section of the chain grate machine to carry out high-temperature flue gas denitration treatment. The composite additive greatly improves the high-temperature denitration efficiency of the grate-rotary kiln oxidized pellet flue gas through specific proportion and dosage. The raw materials of the composite additive are from the market, and the composite additive has the advantages of wide raw material source, low cost, simple preparation process and the like, and is easy to realize large-scale production.

Description

Composite additive for selective non-catalytic reduction denitration of flue gas and preparation method and application thereof
Technical Field
The invention relates to a denitration additive, in particular to a composite additive for selective non-catalytic reduction denitration of flue gas, a preparation method and application thereof, and belongs to the technical field of flue gas purification.
Background
The production of oxidized pellets for blast furnace iron making in China is mainly based on a grate-rotary kiln process, and the yield of the oxidized pellets accounts for more than 60% of the total pellet yield. In recent years, as iron ore raw materials and fuels become more complex,the proportion of hematite is increased (the roasting temperature is increased), the scale utilization of low-quality fuel, the application of nitrogen-containing coke oven gas and the like, so that the NOx emission concentration in the pellet production process of many enterprises is in an increasing trend; in addition, the increasingly severe environmental protection requirements of China are met, the emission of NOx is brought into an emission assessment system, and NOx (produced by NO) is produced by pellets from 20152Meter) emission limit 300mg/m3Therefore, the part of enterprises can meet the national emission standard by adding the denitration facility. The national environmental protection agency of 6 months in 2017 issues a revised notice of 'emission standards of atmospheric pollutants for the iron and steel sintering and pelletizing industry', and NOx (in NO form)2Meter) emission limits from 300mg/Nm3Down-regulated to 100mg/Nm3. By 2025, ultra-low emission control was carried out to control NOx (as NO)2Meter) emission limits were adjusted down to 50mg/Nm3And the reference oxygen content is 18%, and the actually measured emission concentration of the atmospheric pollutants in the roasting flue gas is converted into the emission concentration under the condition of the reference oxygen content and is used as a basis for judging whether the emission reaches the standard or not. Although pelletizing enterprises do a lot of work in the aspect of environmental protection, dust removal and desulfurization are effectively controlled, and emission requirements can be met, NOx is high in removal cost and complex in process at present, and under the environment with a low steel form, new challenges are brought to the pelletizing industry, and a part of enterprises have to reduce production greatly due to the fact that NOx exceeds the standard, and even face shutdown. From the current most oxidized pellet production conditions, the NOx emission concentration is generally 200-400 mg/Nm3And the requirement of ultra-low emission cannot be met. The method has limited effect of reducing the NOx generation amount in the production process of the grate-rotary kiln pellets by measures of reducing the injection amount of coal gas or coal powder, reducing the temperature of the rotary kiln, adopting lower NOx raw materials and fuels and the like, and can not completely meet the purification requirement of flue gas nitrogen oxides.
At present, NOx is removed mainly by means of a Selective Catalytic Reduction (SCR) technology and a selective non-catalytic reduction (SNCR) technology, NOx is removed at the tail end and in the process respectively, and the SNCR technology in series connection with the SCR technology is an effective means for realizing ultralow emission of pellet smoke. For SNCR denitration techniques, a temperature range of 800 ℃ to 1100 ℃ is generally considered to be suitable. Production of pellet by chain grate-rotary kilnThe SNCR denitration technology is applied in the process, and usually, a reducing agent (ammonia water or urea) is sprayed into the flue gas at the preheating second stage (the temperature is 850-1100 ℃) to carry out flue gas denitration, but the best emission reduction effect can be achieved only by optimizing control. However, the application effect of the SNCR technique is sensitive to factors such as temperature and the amount of reducing agent. NH when fluctuations occur in the production process, e.g. excessive temperatures3Oxidation to NO may result in an increase in the concentration of NO, resulting in a decrease in the NOx removal rate. At too low a temperature, NH3The reaction rate of (2) is decreased, the NOx removal rate is also decreased, and NH is added3The amount of escape of (a) will also increase.
In order to improve the denitration efficiency of the SNCR technology, researchers have proposed many technical solutions. For example, Wu faithful Bian invented "additive for SNCR denitration of flue gas and its application (No. CN 103252159B)" discloses an additive for SNCR denitration of flue gas, which is composed of cellulose ether and inorganic sodium salt, and is mixed with denitration reducing agent and sprayed into flue gas at 760-850 ℃ for denitration, and can adapt to different oxygen concentration changes, reduce byproduct N2And O is generated, the denitration efficiency is between 40 and 70 percent, the effective denitration temperature area is expanded, the range of the allowed oxygen is expanded, and the escape of ammonia is reduced. But at present, the research on the additives of the SNCR technology applied to the denitration of the oxidized pellet flue gas of the chain grate-rotary kiln (the flue gas temperature range is 850-1100 ℃) is less.
Disclosure of Invention
Aiming at the defects of the prior art, the invention provides a composite additive added into a flue gas denitration reducing agent (generally ammonia water) so as to improve the stability and the denitration rate when an SNCR technology is applied in the production process of a chain grate machine-rotary kiln pellet, improve the utilization efficiency of the flue gas denitration reducing agent and reduce NH3The escaping amount.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
according to a first embodiment of the invention, a composite additive for selective non-catalytic reduction denitration of flue gas is provided, which comprises the following components:
40-70 parts of urea, preferably 45-65 parts of urea, and more preferably 50-60 parts of urea.
10 to 30 parts by weight of NaCl, preferably 12 to 25 parts by weight, more preferably 15 to 20 parts by weight.
8-28 parts of ethanol, preferably 10-25 parts of ethanol, and more preferably 12-22 parts of ethanol.
1-12 parts by weight of vanadium-titanium catalyst, preferably 2-10 parts by weight, more preferably 3-8 parts by weight.
Preferably, the compound ammonia agent also comprises:
SBA-150.1-5 parts by weight, preferably 0.3-4 parts by weight, more preferably 0.5-3 parts by weight.
Preferably, the urea is urea with a purity of 99% or more, and preferably urea with a purity of 99.5% or more.
Preferably, the NaCl is NaCl with a purity of 99% or more, preferably NaCl with a purity of 99.5% or more.
Preferably, the ethanol is absolute ethanol with the purity of more than or equal to 99%, and preferably absolute ethanol with the purity of more than or equal to 99.7%.
Preferably, the particle size of the urea is-0.074 mm ≥ 90%, preferably-0.074 mm ≥ 95%.
Preferably, the particle size of the NaCl is more than or equal to 90 percent when the particle size is-0.074 mm, and more preferably more than or equal to 95 percent when the particle size is-0.074 mm.
Preferably, the particle size of the vanadium-titanium catalyst is-0.074 mm ≥ 80%, preferably-0.074 mm ≥ 90%.
According to a second embodiment of the present invention, there is provided a method of preparing the additive package of the first embodiment, comprising the steps of:
1) firstly, grinding urea, NaCl and a vanadium-titanium catalyst into powder. And then uniformly stirring and mixing the powdered urea, NaCl and the vanadium-titanium catalyst according to the proportion to obtain a powder mixture. Finally, the ethanol is independently measured in proportion to obtain wet materials. And uniformly mixing the wet material and the powder mixture to obtain the composite additive.
Preferably, the SBA-15 material is also included in the step 1). Grinding urea, NaCl, a vanadium-titanium catalyst and an SBA-15 material into powder; and then uniformly stirring and mixing the powdered urea, NaCl, the vanadium-titanium catalyst and the SBA-15 material according to the proportion to obtain a powder mixture.
Preferably, in step 1), the urea has a purity of 99% or more, preferably a purity of 99.5% or more. The particle size of the urea is-0.074 mm or more and 90 percent, preferably-0.074 mm or more and 95 percent.
Preferably, in step 1), the NaCl has a purity of 99% or more, preferably a purity of 99.5% or more. The granularity of the NaCl is more than or equal to 90 percent when the granularity is-0.074 mm, and preferably more than or equal to 95 percent when the granularity is-0.074 mm. And/or
Preferably, in step 1), the vanadium-titanium catalyst is selected from any V-TiO2Is a catalyst. The particle size of the vanadium-titanium catalyst is-0.074 mm or more and 80%, preferably-0.074 mm or more and 90%. And/or
Preferably, in step 1), the ethanol is anhydrous ethanol. The purity of the absolute ethyl alcohol is more than or equal to 99 percent, and the preferred purity is more than or equal to 99.7 percent.
Preferably, in step 1), the amounts of the components added are as follows:
40-70 parts of urea, preferably 45-65 parts of urea, and more preferably 50-60 parts of urea.
10 to 30 parts by weight of NaCl, preferably 12 to 25 parts by weight, more preferably 15 to 20 parts by weight.
8-28 parts of ethanol, preferably 10-25 parts of ethanol, and more preferably 12-22 parts of ethanol.
1-12 parts by weight of vanadium-titanium catalyst, preferably 2-10 parts by weight, more preferably 3-8 parts by weight.
Preferably, the components of the step 1) are also added with:
SBA-150.1-5 parts by weight, preferably 0.3-4 parts by weight, more preferably 0.5-3 parts by weight.
According to a third embodiment of the present invention, there is provided a use of the additive package according to the first embodiment or the additive package prepared by the method according to the second embodiment for selective non-catalytic reduction denitration of flue gas.
Preferably, the composite additive is used for selective non-catalytic reduction denitration of oxidized pellet flue gas of a chain grate-rotary kiln.
Preferably, the specific uses of the composite additive are as follows: adding 0.1-2.0 wt% (preferably 0.3-1.2 wt%, more preferably 0.5-1.0 wt%) of composite additive (based on the total addition amount of the reducing agent) into the pellet flue gas denitration reducing agent (such as ammonia water with the concentration of 20-25%), and stirring and mixing uniformly. And then spraying the uniformly mixed denitration reducing agent containing the composite additive to high-temperature flue gas from a transition section between the chain grate machine and the rotary kiln and/or a preheating two-section of the chain grate machine for denitration treatment.
Generally, the SNCR denitration technique is considered to be preferably carried out at a temperature in the range of 800 ℃ to 1100 ℃. In the production process of the grate-rotary kiln pellets, an SNCR denitration technology is applied, and usually a reducing agent (ammonia water or urea) is sprayed into flue gas at a preheating section (the temperature is 850-1100 ℃) to carry out flue gas denitration, but the optimal emission reduction effect can be achieved only by optimizing control. However, the application effect of the SNCR technique is sensitive to factors such as temperature and the amount of reducing agent. NH when the production process fluctuates, e.g. the temperature is too high3The oxidation to NO may cause the concentration of NO to increase, the removal rate of NOx is reduced, and when the temperature is too low, NH is generated3The reaction rate of (2) is decreased, the NOx removal rate is also decreased, and the slip amount of NH3 is also increased.
According to the invention, urea, NaCl and a vanadium-titanium catalyst are weighed according to a specific mass ratio, stirred and uniformly mixed to obtain a powder mixture, then ethanol is independently weighed and placed to obtain a wet material, and the powder mixture and the wet material jointly form the composite additive.
Further, the main component of the SBA-15 mesoporous material is SiO2Has a two-dimensional straight-channel hexagonal crystal structure, the thickness of the hole wall can reach 6.4nm, the thermal stability can reach 900 ℃, the specific surface area can reach 700-2Per g, pore volume 0.6-1.3cm2(ii) in terms of/g. Has good dispersibility in water and ethanol. In the invention, the addition of the SBA-15 mesoporous material can improve the contact area of the composite ammonia agent and NOx and provide a better reaction site for the ammonia agent and the NOx, thereby accelerating the occurrence of catalytic reduction reaction.
Furthermore, the purity of the urea is more than or equal to 99 percent, and preferably the purity is more than or equal to 99.5 percent. The particle size of the urea is-0.074 mm or more and 90 percent, preferably-0.074 mm or more and 95 percent. The purity of the NaCl is more than or equal to 99 percent, and the preferred purity of the NaCl is more than or equal to 99.5 percent. The granularity of the NaCl is more than or equal to 90 percent when the granularity is-0.074 mm, and preferably more than or equal to 95 percent when the granularity is-0.074 mm. The vanadium-titanium catalyst is selected from any V-TiO2Is a catalyst. The particle size of the vanadium-titanium catalyst is-0.074 mm or more and 80%, preferably-0.074 mm or more and 90%. The ethanol is absolute ethanol. The purity of the absolute ethyl alcohol is more than or equal to 99 percent, and the preferred purity is more than or equal to 99.7 percent.
In the invention, the specific uses of the composite additive are as follows: adding 0.1-2.0 wt% (preferably 0.3-1.2 wt%, more preferably 0.5-1.0 wt%) of composite additive (based on the total addition amount of the reducing agent) into the pellet flue gas denitration reducing agent (such as ammonia water with the concentration of 20-25%), and stirring and mixing uniformly. And then spraying the uniformly mixed denitration reducing agent containing the composite additive to high-temperature flue gas from a transition section between the chain grate machine and the rotary kiln and/or a preheating two-section of the chain grate machine for denitration treatment.
In the invention, the composite additive is compounded by urea, NaCl, ethanol and a vanadium-titanium catalyst. Wherein the urea decomposes at high temperature to release ammonia in NH3When the nitrogen oxide is reduced, the reducing agent can be slowly released and provided within a certain period of time, so that the denitration reduction reaction is continuously carried out, and the conversion rate of the nitrogen oxide is improved. NaCl and ethanol can react or decompose after entering high-temperature flue gas to generate a large amount of active groups such as H, CH and OH, and a denitration reaction chain is activated at a lower temperature, so that the sensitivity of SNCR denitration to reaction temperature is obviously reduced, the optimal reaction temperature zone of the SNCR is moved downwards, a denitration reaction temperature window is expanded, and the flue gas denitration rate is improved. In addition, the vanadium-titanium catalyst in the composite additive has the function of promoting the flue gas denitration reaction, and can obviously promote the SNCR denitration reaction. Therefore, the composite additive greatly improves the high-temperature denitration efficiency of the grate-rotary kiln oxidized pellet flue gas under the synergistic effect of several components.
Compared with the prior art, the invention has the following beneficial effects:
1. the composite additive provided by the invention takes urea, NaCl and ethanol as main raw materials, and is formed by matching a small amount of vanadium-titanium catalyst and SBA-15 material when in use, so that the high-temperature denitration efficiency of the oxidized pellet flue gas of the grate-rotary kiln can be effectively improved, the denitration rate of the flue gas can reach 80%, and the difficulty and the cost of subsequent flue gas treatment are greatly reduced.
2. The raw materials added into the composite additive have the functions of ammonia component slow release, catalytic reduction and the like, can realize the denitration effect under the condition of higher ammonia-nitrogen ratio under the condition of lower ammonia-nitrogen ratio, improve the use efficiency of ammonia water during flue gas denitration, reduce the ammonia-nitrogen ratio and ammonia escape, and reduce the ammonia escape concentration to be less than 2mg/m3Greatly reducing the secondary pollution.
3. The raw materials of the composite additive are from the market, and the composite additive has the advantages of wide raw material source, low cost, simple preparation process and the like, and is easy to realize large-scale production.
Detailed Description
The technical solution of the present invention is illustrated below, and the claimed scope of the present invention includes, but is not limited to, the following examples. The invention is also suitable for denitration treatment of the production process of the pellets of the belt type roasting machine.
According to a first embodiment of the invention, a composite additive for selective non-catalytic reduction denitration of flue gas is provided, which comprises the following components:
40-70 parts of urea, preferably 45-65 parts of urea, and more preferably 50-60 parts of urea.
10 to 30 parts by weight of NaCl, preferably 12 to 25 parts by weight, more preferably 15 to 20 parts by weight.
8-28 parts of ethanol, preferably 10-25 parts of ethanol, and more preferably 12-22 parts of ethanol.
1-12 parts by weight of vanadium-titanium catalyst, preferably 2-10 parts by weight, more preferably 3-8 parts by weight.
Preferably, the compound ammonia agent also comprises:
SBA-150.1-5 parts by weight, preferably 0.3-4 parts by weight, more preferably 0.5-3 parts by weight.
Preferably, the urea is urea with a purity of 99% or more, and preferably urea with a purity of 99.5% or more.
Preferably, the NaCl is NaCl with a purity of 99% or more, preferably NaCl with a purity of 99.5% or more.
Preferably, the ethanol is absolute ethanol with the purity of more than or equal to 99%, and preferably absolute ethanol with the purity of more than or equal to 99.7%.
Preferably, the particle size of the urea is-0.074 mm ≥ 90%, preferably-0.074 mm ≥ 95%.
Preferably, the particle size of the NaCl is more than or equal to 90 percent when the particle size is-0.074 mm, and more preferably more than or equal to 95 percent when the particle size is-0.074 mm.
Preferably, the particle size of the vanadium-titanium catalyst is-0.074 mm ≥ 80%, preferably-0.074 mm ≥ 90%.
According to a second embodiment of the present invention, there is provided a method of preparing the additive package of the first embodiment, comprising the steps of:
1) firstly, grinding urea, NaCl and a vanadium-titanium catalyst into powder. And then uniformly stirring and mixing the powdered urea, NaCl and the vanadium-titanium catalyst according to the proportion to obtain a powder mixture. Finally, the ethanol is independently measured in proportion to obtain wet materials. And uniformly mixing the wet material and the powder mixture to obtain the composite additive.
Preferably, the SBA-15 material is also included in the step 1). Grinding urea, NaCl, a vanadium-titanium catalyst and an SBA-15 material into powder; and then uniformly stirring and mixing the powdered urea, NaCl, the vanadium-titanium catalyst and the SBA-15 material according to the proportion to obtain a powder mixture.
Preferably, in step 1), the urea has a purity of 99% or more, preferably a purity of 99.5% or more. The particle size of the urea is-0.074 mm or more and 90 percent, preferably-0.074 mm or more and 95 percent.
Preferably, in step 1), the NaCl has a purity of 99% or more, preferably a purity of 99.5% or more. The granularity of the NaCl is more than or equal to 90 percent when the granularity is-0.074 mm, and preferably more than or equal to 95 percent when the granularity is-0.074 mm. And/or
As a preferenceIn step 1), the vanadium-titanium catalyst is selected from any V-TiO2Is a catalyst. The particle size of the vanadium-titanium catalyst is-0.074 mm or more and 80%, preferably-0.074 mm or more and 90%. And/or
Preferably, in step 1), the ethanol is anhydrous ethanol. The purity of the absolute ethyl alcohol is more than or equal to 99 percent, and the preferred purity is more than or equal to 99.7 percent.
Preferably, in step 1), the amounts of the components added are as follows:
40-70 parts of urea, preferably 45-65 parts of urea, and more preferably 50-60 parts of urea.
10 to 30 parts by weight of NaCl, preferably 12 to 25 parts by weight, more preferably 15 to 20 parts by weight.
8-28 parts of ethanol, preferably 10-25 parts of ethanol, and more preferably 12-22 parts of ethanol.
1-12 parts by weight of vanadium-titanium catalyst, preferably 2-10 parts by weight, more preferably 3-8 parts by weight.
Preferably, the components of the step 1) are also added with:
SBA-150.1-5 parts by weight, preferably 0.3-4 parts by weight, more preferably 0.5-3 parts by weight.
According to a third embodiment of the present invention, there is provided a use of the additive package according to the first embodiment or the additive package prepared by the method according to the second embodiment for selective non-catalytic reduction denitration of flue gas.
Preferably, the composite additive is used for selective non-catalytic reduction denitration of oxidized pellet flue gas of a chain grate-rotary kiln.
Preferably, the specific uses of the composite additive are as follows: adding 0.1-2.0 wt% (preferably 0.3-1.2 wt%, more preferably 0.5-1.0 wt%) of composite additive (based on the total addition amount of the reducing agent) into the pellet flue gas denitration reducing agent (such as ammonia water with the concentration of 20-25%), and stirring and mixing uniformly. And then spraying the uniformly mixed denitration reducing agent containing the composite additive to high-temperature flue gas from a transition section between the chain grate machine and the rotary kiln and/or a preheating two-section of the chain grate machine for denitration treatment.
Example 1
A flue gas denitration system of a grate-rotary kiln oxidized pellet process is selected, wherein ammonia water is sprayed at a preheating section of a grate to serve as a reducing agent, a composite additive with the total addition of 0.4% of the reducing agent is added (wherein the components comprise 55% of urea, 20% of NaCl, 20% of ethanol and 5% of vanadium-titanium catalyst, and the total amount is 100%), the ammonia nitrogen molar ratio of the sprayed ammonia water is 1.1:1, and high-temperature denitration is carried out on the grate-rotary kiln oxidized pellet flue gas. The concentration of nitrogen oxide in flue gas at the inlet of the ammonia water spraying position is 680ppm, the concentration of nitrogen oxide in flue gas at the outlet of the preheating section is 193ppm, the denitration rate is 71.6%, and the escape concentration of ammonia is about 4mg/m3。
Example 2
A flue gas denitration system of a grate-rotary kiln oxidized pellet process is selected, wherein ammonia water is sprayed at a preheating section of a grate to serve as a reducing agent, a composite additive with the total addition of 0.7% of the reducing agent is added (wherein the components comprise 55% of urea, 20% of NaCl, 20% of ethanol and 5% of vanadium-titanium catalyst, and the total amount is 100%), the ammonia nitrogen molar ratio of the sprayed ammonia water is 1.1:1, and high-temperature denitration is carried out on the grate-rotary kiln oxidized pellet flue gas. The concentration of nitrogen oxide in flue gas at the inlet of the ammonia water spraying position is 680ppm, the concentration of nitrogen oxide in flue gas at the outlet of the preheating section is 146ppm, the denitration rate is 78.5%, and the escape concentration of ammonia is about 3mg/m3。
Example 3
A flue gas denitration system of a grate-rotary kiln oxidized pellet process is selected, wherein ammonia water is sprayed at a preheating section of a grate to serve as a reducing agent, a composite additive with the total addition of 1.0% of the reducing agent is added (wherein the components comprise 55% of urea, 20% of NaCl, 20% of ethanol and 5% of vanadium-titanium catalyst, and the total amount is 100%), the ammonia nitrogen molar ratio of the sprayed ammonia water is 1.1:1, and high-temperature denitration is carried out on the grate-rotary kiln oxidized pellet flue gas. The concentration of nitrogen oxide in flue gas at the inlet of the ammonia water spraying position is 680ppm, the concentration of nitrogen oxide in flue gas at the outlet of the preheating section is 113ppm, the denitration rate is 83.4%, and the escape concentration of ammonia is about 2mg/m3。
Example 4
Selective grate-rotaryIn the denitration system for the flue gas produced by the kiln oxidation pelletizing process, ammonia water is sprayed at the preheating section of a chain grate machine to serve as a reducing agent, a composite additive with the total addition of the reducing agent being 0.7% (wherein the components comprise 65% of urea, 15% of NaCl, 15% of ethanol and 5% of vanadium-titanium catalyst, and the total amount is 100%) is added, the ammonia nitrogen molar ratio of the sprayed ammonia water is 1.1:1, and high-temperature denitration is carried out on the oxidized pellet flue gas produced by the chain grate machine and the rotary kiln. The concentration of nitrogen oxide in flue gas at the inlet of the ammonia water spraying position is 680ppm, the concentration of nitrogen oxide in flue gas at the outlet of the preheating section is 180ppm, the denitration rate is 73.6%, and the escape concentration of ammonia is about 5mg/m3。
Example 5
A flue gas denitration system of a grate-rotary kiln oxidized pellet process is selected, wherein ammonia water is sprayed at a preheating section of a grate to serve as a reducing agent, a composite additive with the total addition of 0.7% of the reducing agent is added (wherein the components comprise 48% of urea, 23% of NaCl, 23% of ethanol and 6% of vanadium-titanium catalyst, and the total amount is 100%), the ammonia nitrogen molar ratio of the sprayed ammonia water is 1.1:1, and high-temperature denitration is carried out on the grate-rotary kiln oxidized pellet flue gas. The concentration of nitrogen oxide in flue gas at the inlet of the ammonia water spraying position is 680ppm, the concentration of nitrogen oxide in flue gas at the outlet of the preheating section is 141ppm, the denitration rate is 79.2%, and the escape concentration of ammonia is about 3mg/m3。
Example 6
A flue gas denitration system of a grate-rotary kiln oxidized pellet process is selected, wherein ammonia water is sprayed at a preheating section of a grate to serve as a reducing agent, a composite additive with the total addition of 0.7% of the reducing agent is added (wherein the components comprise 52% of urea, 20% of NaCl, 20% of ethanol and 8% of vanadium-titanium catalyst, and the total amount is 100%), the ammonia nitrogen molar ratio of the sprayed ammonia water is 1.1:1, and high-temperature denitration is carried out on the grate-rotary kiln oxidized pellet flue gas. The concentration of nitrogen oxide in flue gas at the inlet of the ammonia water spraying position is 680ppm, the concentration of nitrogen oxide in flue gas at the outlet of the preheating section is 121ppm, the denitration rate is 82.2%, and the escape concentration of ammonia is about 2mg/m3。
Example 7
Flue gas denitration system for selective grate-rotary kiln pellet oxidation process, wherein a preheating section of the grate is sprayed with flue gasSpraying ammonia water as a reducing agent, adding a composite additive with the total addition of the reducing agent being 0.7% (wherein the components comprise 45% of urea, 25% of NaCl, 25% of ethanol and 5% of vanadium-titanium catalyst, and the total amount is 100%), spraying ammonia water with the ammonia nitrogen molar ratio of 1.1:1, and carrying out high-temperature denitration on the oxidized pellet flue gas of the chain grate-rotary kiln. The concentration of nitrogen oxide in flue gas at the inlet of the ammonia water spraying position is 680ppm, the concentration of nitrogen oxide in flue gas at the outlet of the preheating section is 145ppm, the denitration rate is 78.6%, and the escape concentration of ammonia is about 2mg/m3。
Example 8
A flue gas denitration system of a grate-rotary kiln oxidized pellet process is selected, wherein ammonia water is sprayed at a preheating section of a grate to serve as a reducing agent, a composite additive with the total addition of 0.7% of the reducing agent is added (wherein the components comprise 30% of urea, 35% of NaCl, 20% of ethanol and 15% of vanadium-titanium catalyst, and the total amount is 100%), the ammonia nitrogen molar ratio of the sprayed ammonia water is 1.1:1, and high-temperature denitration is carried out on the grate-rotary kiln oxidized pellet flue gas. The concentration of nitrogen oxide in flue gas at the inlet of the ammonia water spraying position is 680ppm, the concentration of nitrogen oxide in flue gas at the outlet of the preheating section is 246ppm, the denitration rate is 63.8%, and the escape concentration of ammonia is about 6mg/m3。
Example 9
A flue gas denitration system of a grate-rotary kiln oxidized pellet process is selected, wherein ammonia water is sprayed at a preheating section of a grate to serve as a reducing agent, a composite additive with the total addition of 0.7% of the reducing agent is added (wherein the components comprise 75% of urea, 5% of NaCl, 5% of ethanol and 15% of vanadium-titanium catalyst, and the total amount is 100%), the ammonia nitrogen molar ratio of the sprayed ammonia water is 1.1:1, and high-temperature denitration is carried out on the grate-rotary kiln oxidized pellet flue gas. The concentration of nitrogen oxide in flue gas at the inlet of the ammonia water spraying position is 680ppm, the concentration of nitrogen oxide in flue gas at the outlet of the preheating section is 303ppm, the denitration rate is 55.4%, and the escape concentration of ammonia is about 11mg/m3。
Example 10
Selecting a flue gas denitration system of a grate-rotary kiln pellet oxidation process, wherein ammonia water is sprayed at a preheating section of the grate to serve as a reducing agent, and a composite addition with the total addition amount of 0.7 percent of the reducing agent is addedThe agent (wherein the components are 44% of urea, 25% of NaCl, 25% of ethanol, 5% of vanadium-titanium catalyst, 1% of SBA-15 and 100% in total), ammonia nitrogen molar ratio of ammonia water spraying is 1.1:1, and high-temperature denitration of the oxidized pellet flue gas of the chain grate-rotary kiln is carried out. The concentration of nitrogen oxides in flue gas at the inlet of the ammonia water spraying position is 680ppm, the concentration of nitrogen oxides in flue gas at the outlet of the preheating section is 120ppm, the denitration rate is 82.3%, and the escape concentration of ammonia is less than 2mg/m3。
Comparative example 1
Selecting a flue gas denitration system of a grate-rotary kiln oxidized pellet process, wherein ammonia water is sprayed at a preheating section of the grate as a reducing agent, a compound additive is not added, the ammonia nitrogen molar ratio of the sprayed ammonia water is 0.7:1, and carrying out high-temperature denitration on the grate-rotary kiln oxidized pellet flue gas. The concentration of nitrogen oxide in flue gas at the inlet of the ammonia water spraying position is 680ppm, the concentration of nitrogen oxide in flue gas at the outlet of the preheating section is 630ppm, the denitration rate is 7.3%, and the escape concentration of ammonia is about 5mg/m3。
Comparative example 2
Selecting a flue gas denitration system of a grate-rotary kiln oxidized pellet process, wherein ammonia water is sprayed at a preheating section of the grate as a reducing agent, a compound additive is not added, the ammonia nitrogen molar ratio of the sprayed ammonia water is 1.1:1, and carrying out high-temperature denitration on the grate-rotary kiln oxidized pellet flue gas. The concentration of nitrogen oxide in flue gas at the inlet of the ammonia water spraying position is 680ppm, the concentration of nitrogen oxide in flue gas at the outlet of the preheating section is 359ppm, the denitration rate is 47.2%, and the escape concentration of ammonia is about 8mg/m3。
Comparative example 3
Selecting a flue gas denitration system of a grate-rotary kiln oxidized pellet process, wherein ammonia water is sprayed at a preheating section of the grate as a reducing agent, a compound additive is not added, the ammonia nitrogen molar ratio of the sprayed ammonia water is 1.7:1, and carrying out high-temperature denitration on the grate-rotary kiln oxidized pellet flue gas. The concentration of nitrogen oxide in flue gas at the inlet of the ammonia water spraying position is 680ppm, the concentration of nitrogen oxide in flue gas at the outlet of the preheating section is 182ppm, the denitration rate is 73.3%, and the escape concentration of ammonia is about 15mg/m3。
Comparative example 4
Selecting a flue gas denitration system of a grate-rotary kiln oxidized pellet process, wherein ammonia water is sprayed at a preheating section of the grate as a reducing agent, urea with the total addition of 0.7% of the reducing agent is added, and the ammonia nitrogen molar ratio of the sprayed ammonia water is 1.1:1, so that high-temperature denitration of the grate-rotary kiln oxidized pellet flue gas is carried out. The concentration of nitrogen oxide in flue gas at the inlet of the ammonia water spraying position is 680ppm, the concentration of nitrogen oxide in flue gas at the outlet of the preheating section is 322ppm, the denitration rate is 52.6%, and the escape concentration of ammonia is about 13mg/m3。
Comparative example 5
Selecting a flue gas denitration system of a grate-rotary kiln oxidized pellet process, wherein ammonia water is sprayed at a preheating section of the grate as a reducing agent, NaCl with the total addition of 0.7% of the reducing agent is added, and the ammonia nitrogen molar ratio of the sprayed ammonia water is 1.1:1, so that high-temperature denitration is carried out on the grate-rotary kiln oxidized pellet flue gas. The concentration of nitrogen oxide in flue gas at the inlet of the ammonia water spraying position is 680ppm, the concentration of nitrogen oxide in flue gas at the outlet of the preheating section is 361ppm, the denitration rate is 46.9%, and the escape concentration of ammonia is about 10mg/m3。
Comparative example 6
Selecting a flue gas denitration system of a grate-rotary kiln oxidized pellet process, wherein ammonia water is sprayed at a preheating section of the grate as a reducing agent, ethanol with the total addition of 0.7% of the reducing agent is added, and the ammonia nitrogen molar ratio of the sprayed ammonia water is 1.1:1, so that high-temperature denitration of the grate-rotary kiln oxidized pellet flue gas is carried out. The concentration of nitrogen oxide in flue gas at the inlet of the ammonia water spraying position is 680ppm, the concentration of nitrogen oxide in flue gas at the outlet of the preheating section is 378ppm, the denitration rate is 44.4%, and the escape concentration of ammonia is about 12mg/m3。
Comparative example 7
Selecting a flue gas denitration system of a grate-rotary kiln oxidized pellet process, wherein ammonia water is sprayed at a preheating section of the grate as a reducing agent, a vanadium-titanium catalyst with the total addition of 0.7% of the reducing agent is added, the ammonia nitrogen molar ratio of the sprayed ammonia water is 1.1:1, and carrying out high-temperature denitration on the grate-rotary kiln oxidized pellet flue gas. The concentration of nitrogen oxide in flue gas at the inlet of the ammonia water spraying position is 680ppm, the concentration of nitrogen oxide in flue gas at the outlet of the preheating section is 306ppm, and the denitration rate is55.0% and ammonia slip concentration of about 9mg/m3。
Effect comparison table
Figure BDA0002565821930000101
Figure BDA0002565821930000111

Claims (10)

1. The composite additive for selective non-catalytic reduction denitration of flue gas is characterized in that: the composite additive comprises the following components:
40-70 parts of urea, preferably 45-65 parts of urea, and more preferably 50-60 parts of urea;
10-30 parts of NaCl, preferably 12-25 parts, more preferably 15-20 parts;
8-28 parts of ethanol, preferably 10-25 parts of ethanol, and more preferably 12-22 parts of ethanol;
1-12 parts by weight of vanadium-titanium catalyst, preferably 2-10 parts by weight, more preferably 3-8 parts by weight;
preferably, the compound ammonia agent also comprises:
SBA-150.1-5 parts by weight, preferably 0.3-4 parts by weight, more preferably 0.5-3 parts by weight.
2. The additive package of claim 1 wherein: the urea is urea with the purity of more than or equal to 99 percent, and preferably urea with the purity of more than or equal to 99.5 percent; and/or
The NaCl is the NaCl with the purity of more than or equal to 99 percent, and preferably the NaCl with the purity of more than or equal to 99.5 percent; and/or
The ethanol is absolute ethanol with the purity of more than or equal to 99 percent, and preferably absolute ethanol with the purity of more than or equal to 99.7 percent.
3. The additive package according to claim 1 or 2, wherein: the granularity of the urea is-0.074 mm which is more than or equal to 90 percent, preferably-0.074 mm which is more than or equal to 95 percent; and/or
The granularity of the NaCl is more than or equal to 90 percent when the granularity is-0.074 mm, and is preferably more than or equal to 95 percent when the granularity is-0.074 mm; and/or
The particle size of the vanadium-titanium catalyst is-0.074 mm or more and 80%, preferably-0.074 mm or more and 90%.
4. A method of preparing the composite additive of any one of claims 1 to 3, wherein: the method comprises the following steps:
1) firstly, grinding urea, NaCl and a vanadium-titanium catalyst into powder; then uniformly stirring and mixing the powdered urea, NaCl and the vanadium-titanium catalyst according to the proportion to obtain a powder mixture; finally, independently measuring ethanol in proportion to obtain wet materials; uniformly mixing the wet material and the powder mixture to obtain a composite additive;
preferably, the step 1) also comprises SBA-15 material; grinding urea, NaCl, a vanadium-titanium catalyst and an SBA-15 material into powder; and then uniformly stirring and mixing the powdered urea, NaCl, the vanadium-titanium catalyst and the SBA-15 material according to the proportion to obtain a powder mixture.
5. The method of claim 4, wherein: in the step 1), the purity of the urea is more than or equal to 99 percent, and preferably the purity is more than or equal to 99.5 percent; the granularity of the urea is-0.074 mm which is more than or equal to 90 percent, preferably-0.074 mm which is more than or equal to 95 percent; and/or
The purity of the NaCl is more than or equal to 99 percent, and the preferred purity of the NaCl is more than or equal to 99.5 percent; the granularity of the NaCl is more than or equal to 90 percent when the granularity is-0.074 mm, and preferably more than or equal to 95 percent when the granularity is-0.074 mm.
6. The method of claim 5, wherein: in step 1), the vanadium-titanium catalyst is selected from any V-TiO2A catalyst; the particle size of the vanadium-titanium catalyst is-0.074 mm which is more than or equal to 80 percent, preferably-0.074 mm which is more than or equal to 90 percent; and/or
The ethanol is absolute ethanol; the purity of the absolute ethyl alcohol is more than or equal to 99 percent, and the preferred purity is more than or equal to 99.7 percent.
7. The method according to any one of claims 4-6, wherein: the addition amounts of the components are as follows:
40-70 parts of urea, preferably 45-65 parts of urea, and more preferably 50-60 parts of urea;
10-30 parts of NaCl, preferably 12-25 parts, more preferably 15-20 parts;
8-28 parts of ethanol, preferably 10-25 parts of ethanol, and more preferably 12-22 parts of ethanol;
1-12 parts by weight of vanadium-titanium catalyst, preferably 2-10 parts by weight, more preferably 3-8 parts by weight;
preferably, the method further comprises the following steps:
SBA-150.1-5 parts by weight, preferably 0.3-4 parts by weight, more preferably 0.5-3 parts by weight.
8. Use of a composite additive according to any one of claims 1 to 3 or a composite additive prepared by a process according to any one of claims 4 to 7, wherein: the composite additive is used for selective non-catalytic reduction denitration of flue gas.
9. Use of the composite additive according to claim 8, characterized in that: the composite additive is used for selective non-catalytic reduction denitration of grate-rotary kiln oxidized pellet flue gas.
10. Use of a composite additive according to claim 9, characterized in that: the specific use of the composite additive is as follows: adding 0.1-2.0 wt% (preferably 0.3-1.2 wt%, more preferably 0.5-1.0 wt%) of a composite additive to a pellet flue gas denitration reducing agent (such as ammonia water with a concentration of 20-25%), based on the total addition amount of the reducing agent; stirring and mixing uniformly; and then spraying the uniformly mixed denitration reducing agent containing the composite additive to high-temperature flue gas from a transition section between the chain grate machine and the rotary kiln and/or a preheating two-section of the chain grate machine for denitration treatment.
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US5281403B1 (en) * 1991-09-27 1996-06-11 Noell Inc Method for converting urea to ammonia
WO2000030733A1 (en) * 1998-11-23 2000-06-02 Mobil Oil Corporation Liquid urea exhaust gas treatment additive
CN101721904A (en) * 2010-01-21 2010-06-09 山东大学 Composite denitration method by biomass direct reburning and selective non-catalytic reduction
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