CN108421413B - Flue gas denitration device and flue gas denitration method - Google Patents

Flue gas denitration device and flue gas denitration method Download PDF

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CN108421413B
CN108421413B CN201810169237.0A CN201810169237A CN108421413B CN 108421413 B CN108421413 B CN 108421413B CN 201810169237 A CN201810169237 A CN 201810169237A CN 108421413 B CN108421413 B CN 108421413B
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flue gas
catalyst
inlet
wall
adsorption
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CN108421413A (en
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杨春振
吴华
赵剑
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China Energy Conservation And Emission Reduction Co ltd
China Energy Investment Corp Ltd
Shandong Shenhua Shanda Energy and Environment Co Ltd
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China Energy Conservation And Emission Reduction Co ltd
China Energy Investment Corp Ltd
Shandong Shenhua Shanda Energy and Environment 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
    • B01D53/86—Catalytic processes
    • B01D53/90—Injecting reactants
    • 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
    • B01D53/8631—Processes characterised by a specific device
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    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01D2251/204—Carbon monoxide
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
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    • B01D2255/20738—Iron
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    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/70—Non-metallic catalysts, additives or dopants
    • B01D2255/702—Carbon
    • 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
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
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    • Y02C20/10—Capture or disposal of greenhouse gases of nitrous oxide (N2O)

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Abstract

The invention provides a flue gas denitration device and a flue gas denitration method. This flue gas denitrification facility includes: the flue gas adsorption unit comprises a flue gas adsorption chamber, the flue gas adsorption chamber is provided with a nitrogen oxide-containing flue gas inlet, a catalyst inlet and an adsorbed catalyst outlet, the nitrogen oxide-containing flue gas inlet is positioned on the side wall of the flue gas adsorption chamber, the catalyst inlet is positioned on the top wall of the flue gas adsorption chamber, and the adsorbed catalyst outlet is positioned on the bottom wall of the flue gas adsorption chamber; the flue gas reduction unit is provided with a flue gas reduction chamber, the flue gas reduction chamber is provided with a reducing gas inlet, an adsorbed catalyst inlet, a catalyst outlet and a nitrogen outlet, the reducing gas inlet and the nitrogen outlet are arranged on the side wall of the flue gas reduction chamber, the adsorbed catalyst inlet is arranged on the top wall of the flue gas reduction chamber, the catalyst outlet is arranged on the bottom wall of the flue gas reduction chamber, and the adsorbed catalyst inlet is connected with the adsorbed catalyst outlet. The denitration device can remove NOxReduction to N2Realizing industrialization.

Description

Flue gas denitration device and flue gas denitration method
Technical Field
The invention relates to the field of flue gas treatment, in particular to a flue gas denitration device and a flue gas denitration method.
Background
SCR (selective catalytic reduction) and SNCR (selective non-catalytic reduction) are currently the main techniques for industrial denitration. In the SCR, a vanadium-based catalyst is used to control the reaction temperature to be 300-400 DEG C(ii) a The SNCR is not added with a catalyst, and the reaction temperature is generally 950-1050 ℃. Because the reducing agent is urea or NH in two methods3Causing a certain escape of ammonia and secondary pollution to the environment.
Other alternatives gradually appear for the problems of high denitration reaction temperature, ammonia escape and the like: (1) first, NO is oxidized with a strong oxidant (e.g., ozone, sodium hypochlorite, etc.)xOxidation to NO2Reuse of existing absorbents (e.g. calcium based absorbents, etc.) with NO2The reaction generates available resources, and the scheme has certain application in industry; (2) using other reducing agents (e.g. CO, H)2、CH4Isoreductive gas) + corresponding catalyst, reacting NOxReduction to N2Most of the solutions focus on laboratory scale, not forming a scale industrial plant.
Disclosure of Invention
The invention mainly aims to provide a flue gas denitration device and a flue gas denitration method, so as to solve the problem that NO is converted into NO in the prior artxReduction to N2The denitration method is difficult to realize industrialization.
In order to achieve the above object, according to one aspect of the present invention, there is provided a flue gas denitration apparatus including: the flue gas adsorption unit comprises a flue gas adsorption chamber, the flue gas adsorption chamber is provided with a nitrogen oxide-containing flue gas inlet, a catalyst inlet and an adsorbed catalyst outlet, the nitrogen oxide-containing flue gas inlet is positioned on the side wall of the flue gas adsorption chamber, the catalyst inlet is positioned on the top wall of the flue gas adsorption chamber, and the adsorbed catalyst outlet is positioned on the bottom wall of the flue gas adsorption chamber; the flue gas reduction unit is provided with a flue gas reduction chamber, the flue gas reduction chamber is provided with a reducing gas inlet, an adsorbed catalyst inlet, a catalyst outlet and a nitrogen outlet, the reducing gas inlet and the nitrogen outlet are arranged on the side wall of the flue gas reduction chamber, the adsorbed catalyst inlet is arranged on the top wall of the flue gas reduction chamber, the catalyst outlet is arranged on the bottom wall of the flue gas reduction chamber, and the adsorbed catalyst inlet is connected with the adsorbed catalyst outlet.
Further, the side wall of the flue gas adsorption chamber comprises: the nitrogen oxide-containing flue gas inlet is arranged at the initial end of the first gradually-expanding wall; a first gradually-decreasing wall disposed opposite to the first gradually-increasing wall; and a first major sidewall connected between the first gradually expanding wall and the first gradually reducing wall.
Further, be provided with in the above-mentioned flue gas adsorption chamber: the first gas distributor is fixedly arranged at the joint of the first gradually-expanding wall and the first main side wall; the second gas distributor is fixedly arranged at the joint of the first tapered wall and the first main side wall; an adsorption zone disposed between the first gas distributor and the second gas distributor; and an optional first baffle disposed at the nitrous oxide containing flue gas inlet.
Further, above-mentioned flue gas denitrification facility still includes catalyst supply unit, and catalyst supply unit links to each other with the catalyst entry, still is provided with first catalyst distributor in the flue gas adsorption chamber, and first catalyst distributor links to each other and sets up in the below of catalyst entry with the catalyst entry.
Further, the side wall of the flue gas reduction chamber comprises: the reducing gas inlet is arranged at the initial end of the second gradually-expanding wall; the second gradually-reducing wall is arranged opposite to the second gradually-expanding wall, and the nitrogen outlet is arranged at the tail end of the second gradually-reducing wall; and a second major sidewall connected between the second tapered wall and the second diverging wall.
Further, the flue gas reduction chamber is internally provided with: the third gas distributor is fixedly arranged at the joint of the second gradually-expanding wall and the second main side wall; the fourth gas distributor is fixedly arranged at the joint of the second tapered wall and the second main side wall; a reaction zone disposed between the third gas distributor and the fourth gas distributor; and an optional second baffle disposed at the reducing gas inlet.
Furthermore, a second catalyst distributor is arranged in the flue gas reduction chamber, and the second catalyst distributor is connected with the adsorbed catalyst inlet and is arranged below the adsorbed catalyst inlet.
Further, above-mentioned flue gas denitrification facility still includes catalyst purification unit, and catalyst purification unit connects the setting between catalyst export after the absorption and catalyst entry after the absorption.
Further, the above catalyst purification unit includes: and the vibration separator is connected and arranged between the adsorbed catalyst outlet and the adsorbed catalyst inlet and is provided with a nitrogen sealing valve.
Further, the nitrogen oxide-containing flue gas inlet, the catalyst inlet, the post-adsorption catalyst outlet, the reducing gas inlet, the post-adsorption catalyst inlet, and the catalyst outlet are each independently provided with a flow rate regulating valve.
According to another aspect of the present invention, there is provided a flue gas denitration method, wherein flue gas is sequentially adsorbed and reduced by using a catalyst by using any one of the above-mentioned flue gas denitration devices to realize denitration.
Further, the catalyst is a low-temperature denitration catalyst, the low-temperature denitration catalyst is activated carbon, an iron-based catalyst or a molecular sieve catalyst, the catalyst is preferably a granular catalyst with the particle size of 500-10 mm, and the moving speed of the catalyst in the flue gas adsorption chamber and the moving speed of the catalyst in the flue gas reduction chamber are respectively and independently 0.05-0.6 m/s.
Further, in the flue gas adsorption chamber, the temperature of the catalyst for adsorbing the flue gas is 150-350 ℃, the thickness of the catalyst along the flow direction of the flue gas is preferably 1-4 m, and the time for the flue gas to pass through the adsorption area of the flue gas adsorption chamber is 0.5-3 s; in the flue gas reduction chamber, the temperature of the catalyst for reducing the flue gas is 150-350 ℃, the thickness of the catalyst in the flowing direction of the reducing gas is preferably 1-4 m, and the time for the flue gas to pass through the reaction zone of the flue gas reduction chamber is 0.5-3 s.
Further, the reducing gas is H2、CH4Or CO, preferably the flow resistance of the reducing gas is 200-1000 Pa, and the flow resistance of the flue gas is 200-1000 Pa.
By applying the technical scheme of the invention, firstly, the nitrogen oxide in the flue gas is adsorbed in the catalyst by using the flue gas adsorption unit and is separated from other oxygen and the like, and then the nitrogen oxide is reduced to form nitrogen under the action of the catalyst and in an environment isolated from the oxygen by using the flue gas reduction unit, so that the large consumption of the reducing agent and the generation of reaction heat caused by the fact that the reducing agent is firstly oxidized due to the fact that the oxygen in the flue gas enters the reduction process are avoided; meanwhile, the catalyst inlet is arranged on the top wall of the flue gas adsorption chamber, so that the catalyst falls under the action of gravity; meanwhile, the flue gas inlet containing the nitrogen oxides is arranged on the side wall of the flue gas adsorption chamber, so that airflow flows in the horizontal direction, thereby realizing cross flow contact between the catalyst and the flue gas containing the nitrogen oxides, reducing airflow resistance of the flue gas, and ensuring sufficient contact time between the catalyst and the nitrogen oxides to realize adsorption; and the adsorbed catalyst is enabled to fall under the action of gravity by arranging the adsorbed catalyst inlet on the top wall of the flue gas reduction chamber, and reducing gas enters the side wall through the reducing gas inlet and contacts with the adsorbed catalyst in a cross flow manner, so that the airflow resistance of the reducing gas is reduced, the contact time of the reducing gas, the catalyst and nitrogen oxides adsorbed by the catalyst is ensured, and further, the possibility is provided for fully reducing the nitrogen oxides into nitrogen at relatively low temperature. Meanwhile, in the reduction process, the nitrogen oxides adsorbed by the catalyst are analyzed from the catalyst and participate in reduction, and the nitrogen generated by the reduction reaction can be timely separated from the catalyst, so that the aim of continuously and simultaneously carrying out adsorption, reduction and separation is fulfilled, the reaction heat can be timely emitted, and the safety of industrial implementation is ensured. And the separated catalyst can be returned to the flue gas adsorption unit for recycling or returned to the flue gas adsorption unit for recycling after regeneration.
Drawings
The accompanying drawings, which are incorporated in and constitute a part of this application, illustrate embodiments of the invention and, together with the description, serve to explain the invention and not to limit the invention. In the drawings:
fig. 1 shows a schematic structural diagram of a flue gas denitration device provided according to an embodiment of the invention.
Wherein the figures include the following reference numerals:
10. a flue gas adsorption unit; 11. a first tapered wall; 12. a first tapered wall; 13. a first major side wall; 14. a first gas distributor; 15. a second gas distributor; 16. an adsorption zone; 17. a first baffle; 18. a first catalyst distributor;
21. vibrating the separator;
30. a flue gas reduction unit; 31. a second tapered wall; 32. a second tapered wall; 33. a second major side wall; 34. a third gas distributor; 35. a fourth gas distributor; 36. a reaction zone; 37. a second baffle; 38. a second catalyst distributor;
01. a flue gas inlet containing nitrogen oxides; 02. a catalyst inlet; 03. a post-adsorption catalyst outlet; 04. a reducing gas inlet; 05. a post-adsorption catalyst inlet; 06. a catalyst outlet; 07. and (4) a nitrogen outlet.
Detailed Description
It should be noted that the embodiments and features of the embodiments in the present application may be combined with each other without conflict. The present invention will be described in detail below with reference to the embodiments with reference to the attached drawings.
As analyzed in the background of the present application, the prior art utilizes CO, H2、CH4As a reducing agent to reduce NO in the flue gas under the action of corresponding catalystsxAdsorption reanalysis and reduction to N2The technology of (2) is concentrated on a laboratory scale and is difficult to expand to industrial application, because the prior device cannot realize complete stripping of NOx adsorption and desorption processes, and flue gas is easy to exchange (cross gas) in an adsorption zone and a desorption zone, so that CO and H are easy to generate2、CH4When the reducing agent reacts with oxygen in the flue gas, a large amount of reducing agent is consumed, a large amount of heat energy is generated, the cost, the energy consumption and the safety are difficult to control, and further the industrial application is difficult to realize. In order to solve the problem, the application provides a flue gas denitration device and a flue gas denitration method.
In an exemplary embodiment of the present application, a flue gas denitration device is provided, as shown in fig. 1, the flue gas denitration device includes a flue gas adsorption unit 10 and a flue gas reduction unit 30, the flue gas adsorption unit 10 includes a flue gas adsorption chamber, the flue gas adsorption chamber has a flue gas inlet 01 containing oxynitride, a catalyst inlet 02 and a catalyst outlet 03 after adsorption, the flue gas inlet 01 containing oxynitride is located on a side wall of the flue gas adsorption chamber, the catalyst inlet 02 is located on a top wall of the flue gas adsorption chamber, and the catalyst outlet 03 after adsorption is located on a bottom wall of the flue gas adsorption chamber; the flue gas reduction unit 30, the flue gas reduction unit 30 has the flue gas reduction room, the flue gas reduction room has reduction gas entry 04, adsorbed catalyst entry 05, catalyst export 06 and nitrogen outlet 07, reduction gas entry 04 and nitrogen outlet 07 set up on the lateral wall of flue gas reduction room, adsorbed catalyst entry 05 sets up on the roof of flue gas reduction room, catalyst export 06 sets up on the diapire of flue gas reduction room, adsorbed catalyst entry 05 and adsorbed catalyst export 03 link to each other.
The flue gas denitration device firstly utilizes the flue gas adsorption unit 10 to adsorb nitrogen oxides in flue gas into a catalyst, and the nitrogen oxides are separated from other oxygen and the like, and then the flue gas reduction unit 30 is utilized to reduce the nitrogen oxides under the action of the catalyst and in an environment isolated from the oxygen to form nitrogen, so that the phenomenon that the oxygen in the flue gas enters a reduction process to cause that the reducing agent is firstly oxidized to cause large consumption of the reducing agent and the generation of reaction heat is avoided; meanwhile, the catalyst inlet 02 is arranged on the top wall of the flue gas adsorption chamber, so that the catalyst falls under the action of gravity; meanwhile, the flue gas inlet 01 containing the nitrogen oxides is arranged on the side wall of the flue gas adsorption chamber, so that airflow flows in the horizontal direction, thereby realizing cross flow contact between the catalyst and the flue gas containing the nitrogen oxides, reducing airflow resistance of the flue gas, and ensuring sufficient contact time between the catalyst and the nitrogen oxides to realize adsorption; and the adsorbed catalyst inlet 05 is arranged on the top wall of the flue gas reduction chamber, so that the adsorbed catalyst falls under the action of gravity, the reducing gas enters the side wall of the flue gas reduction chamber through the reducing gas inlet 04 and contacts with the adsorbed catalyst in a cross flow manner, the airflow resistance of the reducing gas is reduced, the contact time of the reducing gas and the catalyst and the nitrogen oxides adsorbed by the catalyst is ensured, and the possibility is provided for fully reducing the nitrogen oxides into nitrogen at a relatively low temperature. Meanwhile, in the reduction process, the nitrogen oxides adsorbed by the catalyst are analyzed from the catalyst and participate in reduction, and the nitrogen generated by the reduction reaction can be timely separated from the catalyst, so that the aim of continuously and simultaneously carrying out adsorption, reduction and separation is fulfilled, the reaction heat can be timely emitted, and the safety of industrial implementation is ensured. And the separated catalyst can be returned to the flue gas adsorption unit for recycling or returned to the flue gas adsorption unit for recycling after regeneration.
In order to increase the contact area between the flue gas and the catalyst, preferably, as shown in fig. 1, the side walls of the flue gas adsorption chamber include a first gradually expanding wall 11, a first gradually reducing wall 12 and a first main side wall 13, and the nitrogen oxide-containing flue gas inlet 01 of the first gradually expanding wall 11 is arranged at the beginning of the first gradually expanding wall 11; the first tapered wall 12 is arranged opposite to the first gradually-expanding wall 11; the first main side wall 13 is connected between the first gradually expanding wall 11 and the first gradually tapering wall 12. The flue gas containing the nitrogen oxides enters the flue gas adsorption chamber through a gradually expanding channel formed by the first gradually expanding wall 11, so that the airflow resistance is reduced, and the airflow area is increased, thereby increasing the contact area with the catalyst and ensuring the full contact with the catalyst; the residual gas after adsorption flows out of the smoke adsorption chamber through the tapered channel formed by the first tapered wall 12, so that the airflow resistance is increased, the airflow area is reduced, and the smoke can be allowed to have enough retention time to participate in adsorption.
In addition, in order to further enhance the uniformity of the gas participating in the reaction, it is preferable that as shown in fig. 1, a first gas distributor 14, a second gas distributor 15, an adsorption zone 16 and an optional first guide plate 17 are arranged in the flue gas adsorption chamber, and the first gas distributor 14 is fixedly arranged at the connection position of the first gradually expanding wall 11 and the first main side wall 13; the second gas distributor 15 is fixedly arranged at the joint of the first tapered wall 12 and the first main side wall 13; the adsorption zone 16 is arranged between the first gas distributor 14 and the second gas distributor 15; the first baffle 17 is arranged at the flue gas inlet 01 containing nitrogen oxides. The first gas distributor 14 is utilized to uniformly distribute the gas to be adsorbed to the flue gas containing the nitrogen oxides, so that the contact uniformity of the flue gas and the catalyst is improved; the gas after adsorption is subjected to gas distribution by the second gas distributor 15, so that the gas after adsorption can be uniformly and intensively discharged, the turbulence degree of the gas flow is weakened, and the gas flow resistance of the system is reduced. The first guide plate 17 is utilized to improve the flowing stability of the flue gas containing the nitrogen oxides.
In order to control the moving speed of the catalyst, it is preferable that the flue gas denitration apparatus further includes a catalyst supply unit connected to the catalyst inlet 02, and a first catalyst distributor 18 is further provided in the flue gas adsorption chamber, and the first catalyst distributor 18 is connected to the catalyst inlet 02 and is provided below the catalyst inlet 02, as shown in fig. 1. Set up first catalyst distributor 18 in catalyst entry 02 below, on the one hand to the whereabouts of catalyst play certain buffering and then adjusted the moving speed of catalyst, on the other hand makes the catalyst contact with the flue gas with great area and comparatively even density distribution when the whereabouts, and then optimizes the adsorption effect.
In a preferred embodiment of the present application, as shown in fig. 1, the side walls of the flue gas reduction chamber include a second gradually expanding wall 31, a second gradually contracting wall 32 and a second main side wall 33, and the reducing gas inlet 04 is arranged at the beginning of the second gradually expanding wall 31; the second tapered wall 32 is arranged opposite to the second tapered wall 31, and the nitrogen outlet 07 is arranged at the tail end of the second tapered wall 32; the second main side wall 33 is connected between the second tapered wall 31 and the second tapered wall 32. Reducing gas enters the flue gas reduction chamber through a divergent channel formed by the second divergent wall 31, so that the resistance of the gas flow is reduced and the area of the gas flow is increased, the contact area of the reducing gas and the catalyst after adsorbing the flue gas is increased, and the full contact of the reducing gas and the catalyst is ensured; the gas generated after the reduction reaction flows out of the flue gas adsorption chamber through a reducing channel formed by the second reducing wall 32, so that the airflow resistance is increased, the airflow area is reduced, and the reducing gas can be retained for enough time to participate in adsorption.
In addition, in order to further enhance the uniformity of the gas participating in the reaction, it is preferable that as shown in fig. 1, a third gas distributor 34, a fourth gas distributor 35, a reaction zone 36 and an optional second baffle 37 are disposed in the flue gas reduction chamber, and the third gas distributor 34 is fixedly disposed at the connection position of the second gradually expanding wall 31 and the second main side wall 33; a fourth gas distributor 35 is fixedly arranged at the junction of the second tapered wall 32 and the second main side wall 33; a reaction zone 36 is arranged between the third gas distributor 34 and the fourth gas distributor 35; the second baffle 37 is disposed at the reducing gas inlet 04. The third gas distributor 34 is used for uniformly distributing the reducing gas, so that the contact uniformity of the reducing gas and the catalyst adsorbed with the flue gas is improved; the third gas distributor 34 is used for carrying out gas distribution on the adsorbed gas, so that the gas after the reduction reaction can be uniformly and intensively discharged, the turbulence degree of the gas flow is weakened, and the gas flow resistance of the system is reduced. The stability of the flow of the reducing gas is improved by the second baffle 37.
Preferably, as shown in fig. 1, a second catalyst distributor 38 is further disposed in the flue gas reduction chamber, and the second catalyst distributor 38 is connected to the post-adsorption catalyst inlet 05 and disposed below the post-adsorption catalyst inlet 05. The second catalyst distributor 38 is arranged below the adsorbed catalyst inlet 05, so that on one hand, certain buffering is performed on the falling of the adsorbed catalyst to further adjust the moving speed of the adsorbed catalyst, and on the other hand, the adsorbed catalyst is in contact with the reducing gas in a larger area and more uniform density distribution when falling, and further the reduction effect is optimized.
Because when adsorbing the flue gas in flue gas adsorption unit 10, can lead to the dust in the flue gas and the dust that flue gas and catalyst wearing and tearing produced to lose on the catalyst, in order to avoid the dust to cover nitrogen oxide and lead to the reduction effect variation, preferably above-mentioned flue gas denitrification facility still includes catalyst purification unit, catalyst purification unit connects and sets up between catalyst outlet 03 after adsorbing and catalyst inlet 05 after adsorbing. And purifying the adsorbed catalyst to remove dust in the catalyst.
Preferably, as shown in fig. 1, the catalyst purification unit comprises a shaking separator 21, the shaking separator 21 is connected and arranged between the adsorbed catalyst outlet 03 and the adsorbed catalyst inlet 05, and the shaking separator 21 is provided with a nitrogen sealing valve. By utilizing the catalyst purification unit, the adsorbed catalyst is purified under the condition of nitrogen sealing, so that dust in the catalyst is effectively removed, oxygen-containing gas such as air and the like is prevented from being introduced in the process, and the reduction reaction efficiency of the reducing gas in the flue gas reduction chamber is ensured.
In order to control the flow rates of the flue gas, the catalyst, the reducing gas, and the like, it is preferable that the flue gas containing nitrogen oxides inlet 01, the catalyst inlet 02, the post-adsorption catalyst outlet 03, the reducing gas inlet 04, the post-adsorption catalyst inlet 05, and the catalyst outlet 06 be each independently provided with a flow rate control valve.
In another exemplary embodiment of the present application, a flue gas denitration method is provided, in which flue gas is sequentially adsorbed and reduced by using a catalyst in a flue gas denitration apparatus using any one of the above methods to realize denitration.
The flue gas denitration device firstly utilizes the flue gas adsorption unit 10 to adsorb nitrogen oxides in flue gas into a catalyst, and the nitrogen oxides are separated from other oxygen and the like, and then the flue gas reduction unit 30 is utilized to reduce the nitrogen oxides under the action of the catalyst and in an environment isolated from the oxygen to form nitrogen, so that the phenomenon that the oxygen in the flue gas enters a reduction process to cause that the reducing agent is firstly oxidized to cause large consumption of the reducing agent and the generation of reaction heat is avoided; meanwhile, the catalyst inlet 02 is arranged on the top wall of the flue gas adsorption chamber, so that the catalyst falls under the action of gravity; meanwhile, the flue gas inlet 01 containing the nitrogen oxides is arranged on the side wall of the flue gas adsorption chamber, so that airflow flows in the horizontal direction, thereby realizing cross flow contact between the catalyst and the flue gas containing the nitrogen oxides, reducing airflow resistance of the flue gas, and ensuring sufficient contact time between the catalyst and the nitrogen oxides to realize adsorption; and the adsorbed catalyst inlet 05 is arranged on the top wall of the flue gas reduction chamber, so that the adsorbed catalyst falls under the action of gravity, the reducing gas enters the side wall of the flue gas reduction chamber through the reducing gas inlet 04 and contacts with the adsorbed catalyst in a cross flow manner, the airflow resistance of the reducing gas is reduced, the contact time of the reducing gas and the catalyst and the nitrogen oxides adsorbed by the catalyst is ensured, and the nitrogen oxides can be fully reduced into nitrogen at a relatively low temperature. Meanwhile, in the reduction process, the nitrogen oxides adsorbed by the catalyst are analyzed from the catalyst and participate in reduction, and the nitrogen generated by the reduction reaction can be timely separated from the catalyst, so that the aim of continuously and simultaneously carrying out adsorption, reduction and separation is fulfilled, the reaction heat can be timely emitted, and the safety of industrial implementation is ensured.
The catalyst used in the present application may refer to a catalyst used in laboratory research in the prior art, and in order to reduce energy consumption, the catalyst is preferably a low temperature denitration catalyst to achieve low temperature catalysis, and more preferably activated carbon, an iron-based catalyst or a molecular sieve catalyst. The iron-based catalyst is an iron-based catalyst with a carrier, and the carrier can be activated carbon or a molecular sieve. Further, in order to improve the contact effect between the catalyst and the flue gas, the catalyst is preferably a granular catalyst having a particle size of 500 μm to 10 mm. In order to optimize the adsorption effect and the catalytic effect of the catalyst, the moving speed of the catalyst in the flue gas adsorption chamber and the moving speed of the catalyst in the flue gas reduction chamber are further preferably between 0.05m/h and 0.6m/s respectively and independently.
In a preferred embodiment of the application, in the flue gas adsorption chamber, the temperature of the catalyst for adsorbing the flue gas is 150-350 ℃, and the temperature of the catalyst for adsorbing the flue gas is controlled, so that the adsorption effect is optimized, and the flue gas is preheated. Experiments prove that the flue gas absorption effect is more ideal when the thickness of the catalyst in the flue gas flowing direction is 1-4 m and the time of the flue gas passing through the absorption area of the flue gas absorption chamber is 0.5-3 s.
In another preferred embodiment of the application, in the flue gas reduction chamber, the temperature of the catalyst for reducing the flue gas is 150-350 ℃, the thickness of the catalyst along the flowing direction of the reducing gas is preferably 1-4 m, and the time for the flue gas to pass through the reaction zone of the flue gas reduction chamber is 0.5-3 s. The reduction is carried out under the conditions, so that the heat energy consumption is low, and a more ideal reduction effect can be realized.
Preferably, the reducing gas is H2、CH4Or CO. And the flow resistance of the reducing gas is preferably 200-1000 Pa, and the flow resistance of the flue gas is preferably 200-1000 Pa.
The advantageous effects of the present application will be further described below with reference to examples and comparative examples.
Example 1
The flue gas denitration device shown in figure 1 is adopted to sequentially adsorb and reduce the flue gas containing the nitrogen oxides so as to realize denitration, and a chain furnace with the capacity of 0.7 steam ton/hour is adopted to generate the flue gas to be processed.
The main composition of the flue gas containing nitrogen oxides is shown in Table 1.
TABLE 1
Composition (I) CO NOx O2 CO2
Content (wt.) 0.084wt％ 50ppm 16.83wt％ 1.99wt％
Wherein the catalyst is granular activated carbon with the grain diameter of 500 mu m-4 mm, and the moving speed of the catalyst in the flue gas adsorption chamber and the moving speed of the catalyst in the flue gas reduction chamber are respectively and independently 0.03 m/s.
In the flue gas adsorption chamber, the temperature of the catalyst for adsorbing flue gas is 250 ℃, the thickness of the catalyst in the flow direction of the flue gas is 1.5m, and the time for the flue gas to pass through the adsorption area of the flue gas adsorption chamber is 1 s.
In the flue gas reduction chamber, the temperature of the catalyst for reducing the flue gas is 250 ℃, the thickness of the catalyst in the flow direction of the reducing gas is 1.5m, and the time for the flue gas to pass through the reaction zone of the flue gas reduction chamber is 1 s.
The reducing gas is CO. The flow resistance of the reducing gas is 800Pa, and the flow resistance of the flue gas is 800 Pa.
And (3) detecting the concentration of NOx at an inlet and an outlet of the flue gas in real time by using an online flue gas analyzer, wherein the denitration rate of the reduced flue gas is 76%.
Example 2
The catalyst was a granular activated carbon having a particle size of 2mm to 10mm, as in example 1. Real-time detection of NO at inlet and outlet of flue gas by using on-line flue gas analyzerxThe concentration and the denitration rate of the reduced flue gas are 74 percent.
Example 3
The moving speed of the catalyst in the flue gas adsorption chamber and the moving speed of the catalyst in the flue gas reduction chamber are respectively and independently 0.6 m/s. Otherwise, the same procedure as in example 1 was repeated.
And (3) detecting the concentration of NOx at an inlet and an outlet of the flue gas in real time by using an online flue gas analyzer, wherein the denitration rate of the reduced flue gas is 78%.
Example 4
The moving speed of the catalyst in the flue gas adsorption chamber and the moving speed of the catalyst in the flue gas reduction chamber are respectively and independently 0.05 m/h. Otherwise, the same procedure as in example 1 was repeated.
And (3) detecting the concentration of NOx at an inlet and an outlet of the flue gas in real time by using an online flue gas analyzer, wherein the denitration rate of the reduced flue gas is 75%.
Example 5
In the flue gas adsorption chamber, the temperature of the catalyst for adsorbing flue gas is 150 ℃, the thickness of the catalyst in the flow direction of the flue gas is 1.5m, and the time for the flue gas to pass through the adsorption area of the flue gas adsorption chamber is 1 s.
In the flue gas reduction chamber, the temperature of the catalyst for reducing the flue gas is 150 ℃, the thickness of the catalyst in the flow direction of the reducing gas is 1.5m, and the time for the flue gas to pass through the reaction zone of the flue gas reduction chamber is 1 s. Otherwise, the same procedure as in example 1 was repeated.
And (3) detecting the concentration of NOx at an inlet and an outlet of the flue gas in real time by using an online flue gas analyzer, wherein the denitration rate of the reduced flue gas is 65%.
Example 6
In the flue gas adsorption chamber, the temperature of the catalyst for adsorbing flue gas is 350 ℃, the thickness of the catalyst in the flow direction of the flue gas is 1.5m, and the time for the flue gas to pass through the adsorption area of the flue gas adsorption chamber is 1 s.
In the flue gas reduction chamber, the temperature of the catalyst for reducing the flue gas is 350 ℃, the thickness of the catalyst in the flow direction of the reducing gas is 1.5m, and the time for the flue gas to pass through the reaction zone of the flue gas reduction chamber is 1 s. Otherwise, the same procedure as in example 1 was repeated.
And (3) detecting the concentration of NOx at an inlet and an outlet of the flue gas in real time by using an online flue gas analyzer, wherein the denitration rate of the reduced flue gas is 63%.
Example 7
In the flue gas adsorption chamber, the temperature of the catalyst for adsorbing flue gas is 250 ℃, the thickness of the catalyst in the flow direction of the flue gas is 4m, and the time for the flue gas to pass through the adsorption area of the flue gas adsorption chamber is 1 s. Otherwise, the same procedure as in example 1 was repeated.
And (3) detecting the concentration of NOx at an inlet and an outlet of the flue gas in real time by adopting an online flue gas analyzer, wherein the denitration rate of the reduced flue gas is 77%.
Example 8
In the flue gas adsorption chamber, the temperature of the catalyst for adsorbing flue gas is 250 ℃, the thickness of the catalyst in the flow direction of the flue gas is 1.5m, and the time for the flue gas to pass through the adsorption area of the flue gas adsorption chamber is 0.5 s. Otherwise, the same procedure as in example 1 was repeated.
And (3) detecting the concentration of NOx at an inlet and an outlet of the flue gas in real time by using an online flue gas analyzer, wherein the denitration rate of the reduced flue gas is 73%.
Example 9
In the flue gas adsorption chamber, the temperature of the catalyst for adsorbing flue gas is 250 ℃, the thickness of the catalyst in the flow direction of the flue gas is 1.5m, and the time for the flue gas to pass through the adsorption area of the flue gas adsorption chamber is 3 s. Otherwise, the same procedure as in example 1 was repeated.
And (3) detecting the concentration of NOx at an inlet and an outlet of the flue gas in real time by using an online flue gas analyzer, wherein the denitration rate of the reduced flue gas is 79%.
Example 10
In the flue gas reduction chamber, the temperature of the catalyst for reducing the flue gas is 150 ℃, the thickness of the catalyst in the flow direction of the reducing gas is 1m, and the time for the flue gas to pass through a reaction zone of the flue gas reduction chamber is 1 s. Otherwise, the same procedure as in example 1 was repeated.
And (3) detecting the concentration of NOx at an inlet and an outlet of the flue gas in real time by using an online flue gas analyzer, wherein the denitration rate of the reduced flue gas is 68%.
Example 11
In the flue gas adsorption chamber, the temperature of the catalyst for adsorbing flue gas is 250 ℃, the thickness of the catalyst in the flow direction of the flue gas is 1.5m, and the time for the flue gas to pass through the adsorption area of the flue gas adsorption chamber is 1 s.
In the flue gas reduction chamber, the temperature of the catalyst for reducing the flue gas is 250 ℃, the thickness of the catalyst in the flow direction of the reducing gas is 4m, and the time for the flue gas to pass through the reaction zone of the flue gas reduction chamber is 1 s. Otherwise, the same procedure as in example 1 was repeated.
And (3) detecting the concentration of NOx at an inlet and an outlet of the flue gas in real time by using an online flue gas analyzer, wherein the denitration rate of the reduced flue gas is 81%.
Example 12
In the flue gas adsorption chamber, the temperature of the catalyst for adsorbing flue gas is 250 ℃, the thickness of the catalyst in the flow direction of the flue gas is 1.5m, and the time for the flue gas to pass through the adsorption area of the flue gas adsorption chamber is 1 s.
In the flue gas reduction chamber, the temperature of the catalyst for reducing the flue gas is 250 ℃, the thickness of the catalyst in the flow direction of the reducing gas is 1.5m, and the time for the flue gas to pass through the reaction zone of the flue gas reduction chamber is 0.5 s. Otherwise, the same procedure as in example 1 was repeated.
And (3) detecting the concentration of NOx at an inlet and an outlet of the flue gas in real time by using an online flue gas analyzer, wherein the denitration rate of the reduced flue gas is 67%.
Example 13
In the flue gas adsorption chamber, the temperature of the catalyst for adsorbing flue gas is 250 ℃, the thickness of the catalyst in the flow direction of the flue gas is 1.5m, and the time for the flue gas to pass through the adsorption area of the flue gas adsorption chamber is 1 s.
In the flue gas reduction chamber, the temperature of the catalyst for reducing the flue gas is 250 ℃, the thickness of the catalyst in the flow direction of the reducing gas is 1.5m, and the time for the flue gas to pass through the reaction zone of the flue gas reduction chamber is 3 s. Otherwise, the same procedure as in example 1 was repeated.
And (3) detecting the concentration of NOx at an inlet and an outlet of the flue gas in real time by using an online flue gas analyzer, wherein the denitration rate of the reduced flue gas is 82%.
Example 14
The flue gas denitration device shown in fig. 1 is adopted to sequentially perform adsorption and reduction treatment on the flue gas containing the nitrogen oxides so as to realize denitration.
The main composition of the flue gas containing nitrogen oxides is shown in Table 2.
TABLE 2
Composition (I) CO NOx O2 CO2
Content (wt.) 0.004wt％ 475ppm 15.91wt％ 2.81wt％
Otherwise, as in example 1, the concentration of NOx at the inlet and outlet of the flue gas was measured in real time by using an on-line flue gas analyzer, and the denitration rate of the reduced flue gas was 79%.
Example 15
The catalyst is a granular Fe-Ce-ZSM-5 molecular sieve carrier type iron-based catalyst with the grain diameter of 2 mm-10 mm, and the rest is the same as the example 1. Real-time detection of NO at inlet and outlet of flue gas by using on-line flue gas analyzerxThe concentration and the denitration rate of the reduced flue gas are 78 percent.
From the above description, it can be seen that the above-described embodiments of the present invention achieve the following technical effects:
the flue gas denitration device firstly utilizes the flue gas adsorption unit to adsorb nitrogen oxides in flue gas into a catalyst, and the nitrogen oxides are separated from other oxygen and the like, and then the flue gas reduction unit is utilized to reduce the nitrogen oxides under the action of the catalyst and in an environment isolated from the oxygen to form nitrogen, so that the phenomenon that the oxygen in the flue gas enters a reduction process to cause that a reducing agent is firstly oxidized to cause large consumption of the reducing agent and the generation of reaction heat is avoided; meanwhile, the catalyst inlet is arranged on the top wall of the flue gas adsorption chamber, so that the catalyst falls under the action of gravity; meanwhile, the flue gas inlet containing the nitrogen oxides is arranged on the side wall of the flue gas adsorption chamber, so that airflow flows in the horizontal direction, thereby realizing cross flow contact between the catalyst and the flue gas containing the nitrogen oxides, reducing airflow resistance of the flue gas, and ensuring sufficient contact time between the catalyst and the nitrogen oxides to realize adsorption; and the adsorbed catalyst is enabled to fall under the action of gravity by arranging the adsorbed catalyst inlet on the top wall of the flue gas reduction chamber, and reducing gas enters the side wall through the reducing gas inlet and contacts with the adsorbed catalyst in a cross flow manner, so that the airflow resistance of the reducing gas is reduced, the contact time of the reducing gas, the catalyst and nitrogen oxides adsorbed by the catalyst is ensured, and further, the possibility is provided for fully reducing the nitrogen oxides into nitrogen at relatively low temperature. Meanwhile, in the reduction process, the nitrogen oxides adsorbed by the catalyst are analyzed from the catalyst and participate in reduction, and the nitrogen generated by the reduction reaction can be timely separated from the catalyst, so that the aim of continuously and simultaneously carrying out adsorption, reduction and separation is fulfilled, the reaction heat can be timely emitted, and the safety of industrial implementation is ensured.
The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.

Claims (12)

1. A flue gas denitration device, which is characterized by comprising:
the flue gas adsorption unit (10) comprises a flue gas adsorption chamber, the flue gas adsorption chamber is provided with a nitrogen oxide-containing flue gas inlet (01), a catalyst inlet (02) and an adsorbed catalyst outlet (03), the nitrogen oxide-containing flue gas inlet (01) is positioned on the side wall of the flue gas adsorption chamber, the catalyst inlet (02) is positioned on the top wall of the flue gas adsorption chamber, and the adsorbed catalyst outlet (03) is positioned on the bottom wall of the flue gas adsorption chamber;
the flue gas reduction unit (30), the flue gas reduction unit (30) is provided with a flue gas reduction chamber, the flue gas reduction chamber is provided with a reducing gas inlet (04), an adsorbed catalyst inlet (05), a catalyst outlet (06) and a nitrogen outlet (07), the reducing gas inlet (04) and the nitrogen outlet (07) are arranged on the side wall of the flue gas reduction chamber, the adsorbed catalyst inlet (05) is arranged on the top wall of the flue gas reduction chamber, the catalyst outlet (06) is arranged on the bottom wall of the flue gas reduction chamber, and the adsorbed catalyst inlet (05) is connected with the adsorbed catalyst outlet (03);
the flue gas denitration device also comprises a catalyst purification unit, and the catalyst purification unit is connected and arranged between the adsorbed catalyst outlet (03) and the adsorbed catalyst inlet (05);
the catalyst purification unit includes:
a vibratory separator (21) connected between the post-adsorption catalyst outlet (03) and the post-adsorption catalyst inlet (05), the vibratory separator (21) having a nitrogen sealing valve,
the side wall of the flue gas adsorption chamber comprises:
the first gradually-expanding wall (11), the nitrogen oxide-containing flue gas inlet (01) is arranged at the beginning of the first gradually-expanding wall (11);
a first tapered wall (12) disposed opposite the first tapered wall (11); and
a first main lateral wall (13) connected between the first diverging wall (11) and the first converging wall (12);
the flue gas adsorption chamber is internally provided with:
a first gas distributor (14) fixedly arranged at the connection of the first gradually expanding wall (11) and the first main side wall (13);
a second gas distributor (15) fixedly arranged at the junction of the first tapered wall (12) and the first main side wall (13);
an adsorption zone (16) disposed between the first gas distributor (14) and the second gas distributor (15); and
an optional first baffle (17) disposed at the nitrous oxide containing flue gas inlet (01);
the flue gas denitration device further comprises a catalyst supply unit, the catalyst supply unit is connected with the catalyst inlet (02), a first catalyst distributor (18) is further arranged in the flue gas adsorption chamber, and the first catalyst distributor (18) is connected with the catalyst inlet (02) and is arranged below the catalyst inlet (02);
the side wall of the flue gas reduction chamber comprises:
a second gradually expanding wall (31), wherein the reducing gas inlet (04) is arranged at the beginning of the second gradually expanding wall (31);
a second tapered wall (32) disposed opposite to the second tapered wall (31), the nitrogen outlet (07) being disposed at a tip end of the second tapered wall (32); and
a second main lateral wall (33) connected between the second diverging wall (31) and the second converging wall (32);
the flue gas reduction chamber is internally provided with:
a third gas distributor (34) fixedly arranged at the joint of the second gradually expanding wall (31) and the second main side wall (33);
a fourth gas distributor (35) fixedly arranged at the junction of the second tapered wall (32) and the second main side wall (33);
a reaction zone (36) disposed between the third gas distributor (34) and the fourth gas distributor (35); and
an optional second baffle (37) disposed at the reducing gas inlet (04).
2. The flue gas denitration device according to claim 1, wherein a second catalyst distributor (38) is further disposed in the flue gas reduction chamber, and the second catalyst distributor (38) is connected to the post-adsorption catalyst inlet (05) and disposed below the post-adsorption catalyst inlet (05).
3. The flue gas denitration apparatus according to claim 1, wherein the flue gas inlet (01) containing nitrogen oxide, the catalyst inlet (02), the post-adsorption catalyst outlet (03), the reducing gas inlet (04), the post-adsorption catalyst inlet (05), and the catalyst outlet (06) are each independently provided with a flow rate adjustment valve.
4. A flue gas denitration method, characterized in that flue gas is adsorbed and reduced in sequence by a catalyst by using the flue gas denitration device of any one of claims 1 to 3 to realize denitration.
5. The flue gas denitration method according to claim 4, wherein the catalyst is a low-temperature denitration catalyst, and the low-temperature denitration catalyst is activated carbon, an iron-based catalyst or a molecular sieve catalyst.
6. The flue gas denitration method according to claim 5, wherein the catalyst is a granular catalyst having a particle size of 500 μm to 10 mm.
7. The flue gas denitration method according to claim 6, wherein the moving speed of the catalyst in the flue gas adsorption chamber and the moving speed of the catalyst in the flue gas reduction chamber are each independently between 0.05m/h and 0.6 m/s.
8. The flue gas denitration method according to claim 4, wherein the temperature of the catalyst adsorbing the flue gas in the flue gas adsorption chamber is 150-350 ℃.
9. The flue gas denitration method according to claim 8, wherein the thickness of the catalyst in the flow direction of the flue gas is 1-4 m, and the time for the flue gas to pass through the adsorption zone of the flue gas adsorption chamber is 0.5-3 s; in the flue gas reduction chamber, the temperature of the catalyst for reducing the flue gas is 150-350 ℃.
10. The flue gas denitration method according to claim 8, wherein the thickness of the catalyst in the flow direction of the reducing gas is 1 to 4m, and the time for the flue gas to pass through the reaction zone of the flue gas reduction chamber is 0.5 to 3 s.
11. The flue gas denitration method of claim 4, wherein the reducing gas is H2、CH4Or CO.
12. The flue gas denitration method according to claim 11, wherein the flow resistance of the reducing gas is 200 to 1000Pa, and the flow resistance of the flue gas is 200 to 1000 Pa.
CN201810169237.0A 2018-02-28 2018-02-28 Flue gas denitration device and flue gas denitration method Active CN108421413B (en)

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CN201692766U (en) * 2010-03-19 2011-01-05 东南大学 Device for removing hazardous constituents from cement kiln flue gas by utilizing cross-flow moving bed
CN105107379A (en) * 2015-08-20 2015-12-02 山东大学 All-carbon flue gas denitrification system and method
CN106731823A (en) * 2016-12-08 2017-05-31 山东大学 A kind of fan housing formula subregion Benitration reactor

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Publication number Priority date Publication date Assignee Title
CN1033508A (en) * 1987-12-15 1989-06-28 包头钢铁公司环境保护研究所 Dry cleaning contains the method and apparatus that mixes the harmful components flue gas
CN201692766U (en) * 2010-03-19 2011-01-05 东南大学 Device for removing hazardous constituents from cement kiln flue gas by utilizing cross-flow moving bed
CN105107379A (en) * 2015-08-20 2015-12-02 山东大学 All-carbon flue gas denitrification system and method
CN106731823A (en) * 2016-12-08 2017-05-31 山东大学 A kind of fan housing formula subregion Benitration reactor

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