CN114367193A - Efficient low-temperature combined desulfurization and denitrification system and method based on active coke function partition - Google Patents
Efficient low-temperature combined desulfurization and denitrification system and method based on active coke function partition Download PDFInfo
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Abstract
An efficient low-temperature combined desulfurization and denitrification system and method based on active coke function partitioning belongs to the field of industrial flue gas treatment. The system is respectively based on the matching relationship of desulfurization, denitrification and active coke physicochemical function requirements, wherein the desulfurization process adopts hierarchical porous active coke doped with an oxygen functional group; the saturated active coke is removed by adsorption and is regenerated by a regeneration system to obtain high-concentration SO2/H2SO4Resource product ofThen mixing with part of fresh coke and entering a desulfurization reactor for circulation; the flue gas after desulfurization and dehydration enters a denitration link, microporous active coke with nitrogen doping is adopted as a catalyst, and NH is sprayed into the flue gas3Under the action of (2) removing NO in the smokexReduction to N2And H2O, to realize NOxThe removal is efficient. The process simultaneously realizes high desulfurization rate and high denitration rate of combined desulfurization and denitration by differentiating the structure-activity relationship between the desulfurization and denitration processes and the physical and chemical functional structure of the active coke, is simple and feasible, does not increase the complexity of equipment and a system, and does not increase excessive investment and operation cost.
Description
Technical Field
The invention belongs to the field of industrial flue gas treatment, and particularly relates to an efficient low-temperature combined desulfurization and denitrification system and method based on active coke function partitioning.
Background
The traditional single flue gas desulfurization and denitration technology has high investment and operation cost, complex system and single pollutant removal technology, and the development of the combined removal technology of sulfur oxides and nitrogen oxides is urgently needed. The active coke taking coal as the raw material has the advantages of wide source, low cost, adjustable physicochemical functions and capability of removing various pollutants simultaneously, and is one of the best choices of the combined desulfurization and denitrification catalyst. Based on the characteristic that coal is both fuel and catalyst raw material, the activated coke combined desulfurization and denitrification process is developed, and the synergistic integration of the power production process and the flue gas purification process can be realized.
The active coke combined desulfurization and denitrification is an important choice for removing industrial nitrogen oxides and sulfur oxides, and can realize the cooperative integration of the power production process and the flue gas purification process. The principle of the active coke combined desulfurization and denitrification comprises the following steps: adsorption of SO in flue gas by active coke2And catalyze O in flue gas2With which reaction takes place to form SO3Then generating sulfuric acid by hydration under the action of water to realize SO2And H2Removing O; in addition, activated coke may be injected over the injected NH3Under the action of (2) removing NO in the smokexReduction to harmless N2And H2O to achieve NOxAnd (4) removing. Thus, it can be seen that the removal of active cokeThe sulfur and denitration processes have different reaction mechanisms and reaction conditions, respectively. Compared with the desulfurization process, the reaction environment of the denitration process is more severe, and SO in the flue gas2Substances such as fly ash and the like easily cause rapid poisoning of the active coke and loss of denitration activity. Therefore, the segmented continuous process of firstly desulfurizing and then denitrating is more suitable for an active coke combined desulfurization and denitration system and has been widely applied to industry. For example, patent CN205019964U discloses a flue gas low-temperature combined desulfurization and denitrification device system comprising a desulfurization regeneration system and a denitrification system. Patent CN107321135A discloses a low-temperature carbon-based combined desulfurization and denitrification flue gas system and a use method, wherein the fine desulfurization and denitrification processes are connected in series and are connected in parallel with the regeneration process, and the fine desulfurization and denitrification processes can be carried out simultaneously, so that in-situ regeneration is really realized. Patent CN108097043A provides a system and a method for powdery active coke fluidized bed tail ammonia spraying combined denitration, which realize the combined removal of nitrogen oxides by utilizing the catalytic action of fresh active coke through effectively controlling and distributing the flow of the active coke and reasonable ammonia spraying positions on the basis of the fluidized desulfurization process of the powdery active coke. However, in the combined desulfurization and denitrification system which is industrially applied at present, a high desulfurization rate and a high denitrification rate cannot be simultaneously realized.
Disclosure of Invention
The invention aims to solve the problem that the existing desulfurization and denitrification system cannot realize high desulfurization rate and high denitrification rate, and provides an efficient low-temperature combined desulfurization and denitrification system and method based on active coke function partition. Oxygen-doped hierarchical pore active coke is adopted in the desulfurization process, and oxygen functional groups are utilized to react with O2The catalytic activation of the catalyst and the functions of micropores and mesopores in adsorption reaction and product transportation and migration to catalyze SO2Oxidation to SO3And combined with H in the flue gas2Conversion of O to H2SO4Realizing SO in the flue gas2And H2The negative effects of sulfur and water poisoning of the denitration catalyst are reduced while the O is efficiently removed; the denitration process adopts nitrogen-doped microporous active coke, and is realized by utilizing the catalytic oxidation capacity of nitrogen-containing functional groups and a microporous structure on NOAnd (4) high-efficiency denitration. Meanwhile, the high-efficiency operation of the whole desulfurization and denitrification process is realized through the coupling of the regeneration process of the active coke. So far, the combined desulfurization and denitrification process considering the active coke functional partition has not been disclosed in a patent.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
an efficient low-temperature combined desulfurization and denitrification system based on active coke function partition comprises an oxygen-doped graded-hole active coke storage bin, a desulfurization reactor, a regeneration system, an ammonia spraying system, a nitrogen-doped microporous active coke storage bin and a denitrification reactor;
the oxygen-doped graded hole active coke storage bin is communicated with the desulfurization reactor, the nitrogen-doped microporous active coke storage bin is communicated with the denitrification reactor, the bottom of the desulfurization reactor is communicated with the regeneration system, and the ammonia spraying system is arranged at or in front of an inlet of the denitrification reactor;
the desulfurization reactor and the denitration reactor are in a double-reactor parallel mode or a single-reactor up-down series mode; the arrangement mode of the active coke catalyst in the desulfurization reactor and the denitration reactor is one of a fixed bed, a moving bed and a fluidized bed.
A method for combined desulfurization and denitrification by using the system comprises the following steps:
the method comprises the following steps: the flue gas after dust removal enters a desulfurization reactor, active coke with oxygen-doped hierarchical pores is used as a catalyst, and oxygen functional groups are used for reacting with O2The catalytic activation of the catalyst and the functions of micropores and mesopores in adsorption reaction and product transportation and migration are realized to realize SO2Catalytic oxidation to SO3And combined with H in the flue gas2Conversion of O to H2SO4Completion of SO2And H2The negative effects of sulfur and water poisoning of the denitration catalyst are reduced while the O is efficiently removed;
step two: the saturated active coke is removed by adsorption and is regenerated by a regeneration system to obtain high-concentration SO2/H2SO4The resource products are mixed with part of fresh coke and enter a desulfurization reactor for circulation, so that the efficient operation of the whole desulfurization and denitrification process is ensured;
step three: the flue gas after desulfurization and dehydration enters a denitration reactor, nitrogen-doped microporous active coke is used as a catalyst, and the catalytic oxidation capacity of nitrogen-containing functional groups and a microporous structure on NO is utilized to spray NH3Under the action of (2) removing NO in the smokexReduction to N2And H2O, to realize NOxThe removal is efficient. The saturated sulfur capacity of the active coke combined desulfurization and denitrification is more than 100mg/g, the desulfurization rate is up to more than 95%, and the denitrification rate is up to more than 90%.
Further, in the second step, the regeneration is thermal regeneration or water washing regeneration, and the obtained resource product is high-concentration SO2Or sulfuric acid; the inlet of the regeneration system is connected with the active coke outlet of the desulfurization reactor.
Further, in the third step, the ammonia gas sprayed by the ammonia spraying system and the desulfurized flue gas are uniformly mixed in front of the denitration reactor, and pure NH is added3NH being 5% of the total flow of the flue gas3With NO in the flue gasxThe molar ratio of (A) to (B) is controlled to be 1-1.2: 1, to ensure that NOx is sufficiently oxidized while preventing excessive ammonia slip.
Further, the flow velocity of flue gas in the desulfurization reactor and the denitration reactor is 1-5 m/s, the operation temperature in the desulfurization reactor is 50-120 ℃, and the relative humidity is 6-12%; the operation temperature in the denitration reactor is 80-200 ℃. Provides proper environmental conditions for the activated coke to exert high desulfurization and denitration activity.
Furthermore, the active coke catalyst is sourced from a corresponding active coke storage bin, is in the form of one of powder, granules or column, and has the size of 1 mu m-10 mm. Can be flexibly adapted to different reactor forms, different gas-solid contact forms and different catalyst arrangement modes.
Further, the specific surface area of the oxygen-doped hierarchical pore active coke is 300-1500 m2The grading degree is 10% -60%; the oxygen doping amount is 4 to 20 at-%.
Further, the specific surface area of the nitrogen-doped microporous active coke is 500-2000 m2The nitrogen doping amount is 1 to 15 at-%.
Compared with the prior art, the invention has the beneficial effects that:
(1) the invention realizes SO in the flue gas by the functional partition of the active coke2、H2O and NOxIn a synergistic manner, high efficiency removal while obtaining high concentrations of SO2Sulfuric acid resource products: based on different requirements of efficient desulfurization and efficient denitration on the physical and chemical structure of the active coke, the invention provides that the oxygen-doped hierarchical pore active coke is adopted as a catalyst in a desulfurization section to realize SO2Catalytic oxidation to SO3And combined with H in the flue gas2Conversion of O to H2SO4To ensure SO in the flue gas2And H2O is removed efficiently, and the negative effects of sulfur and water poisoning of the denitration catalyst are reduced; the denitration section takes nitrogen-doped microporous active coke as a catalyst and sprays NH3Under the action of (2) removing NO in the smokexReduction to N2And H2And O, realizing efficient denitration. In addition, the regeneration process of the coupling desulfurization active coke obtains high-concentration SO2Sulfuric acid recycling products, so that the high-efficiency operation of the whole desulfurization and denitrification process is realized.
(2) The process of the invention is flexibly suitable for the existing mature combined desulfurization and denitrification system, does not increase the complexity of equipment and the system, and does not increase too much investment and operation cost: the process only carries out functional partition on the active coke, does not need to change the prior combined desulfurization and denitrification equipment system, and does not increase the complexity of the equipment and the system; the shape and the size of the active coke can be flexibly adjusted according to different reactor forms, different gas-solid contact forms and different catalyst arrangement forms, the method is simple and easy to implement, and excessive investment and operation cost are not increased.
Drawings
FIG. 1 is a flow chart of a dual reactor mode of the active coke function-based zone low-temperature combined desulfurization and denitrification system.
FIG. 2 is a flow chart of a single reactor mode of the activated coke function-based zone low-temperature combined desulfurization and denitrification system.
Wherein, 1-oxygen doping hierarchical hole active coke storage bin; 2-a desulfurization reactor; 3-a regeneration system; 4-ammonia injection system; 5-nitrogen-doped micropore active coke storage bin; 6-a denitration reactor; 7-separating the sand cores.
Detailed Description
The invention is explained in more detail below with reference to exemplary embodiments and the accompanying drawings. The following examples are not intended to limit the present invention in any way, and all technical solutions obtained by means of equivalent substitution or equivalent transformation are within the scope of the present invention.
The invention is respectively based on the matching relationship of the physical and chemical functional requirements of desulfurization, denitrification and active coke, wherein the desulfurization process adopts the graded-pore active coke doped with oxygen functional groups, and the oxygen functional groups are utilized to carry out O treatment2The catalytic activation of the catalyst and the functions of micropores and mesopores in adsorption reaction and product transportation and migration to catalyze SO2Oxidation to SO3And combined with H in the flue gas2Conversion of O to H2SO4Realizing SO in the flue gas2And H2The negative effects of sulfur and water poisoning of the denitration catalyst are reduced while the O is efficiently removed; the saturated active coke is removed by adsorption and is regenerated by a regeneration system to obtain high-concentration SO2/H2SO4Recycling the product, mixing with part of fresh coke, and circulating in a desulfurization reactor; the flue gas after desulfurization and dehydration enters a denitration link, nitrogen-doped microporous active coke is used as a catalyst, and the catalytic oxidation capacity of nitrogen-containing functional groups and a microporous structure on NO is utilized to spray NH3Under the action of (2) removing NO in the smokexReduction to N2And H2O, to realize NOxThe removal is efficient.
Example 1:
an efficient low-temperature combined desulfurization and denitrification system and method based on active coke function zoning are shown as a working mode 1 in figure 1. The system consists of an oxygen-doped graded-hole active coke storage bin 1, a nitrogen-doped microporous active coke storage bin 5, a moving bed type desulfurization reactor 2, an ammonia spraying system 4, a moving bed type denitration reactor 6 and a regeneration system 3. The working temperature in the desulfurization reactor 2 and the denitration reactor 6 is 90 ℃, and the flue gas flow is 2 m/s; NH in denitration reactor 63With NO in the flue gasxIn a molar ratio of 1: 1. the active coke catalyst in the reactor is granular, the grain size is 3-5 mm, and oxygen is used for desulfurizationThe specific surface area of the active coke with the mixed hierarchical pores is 900m2The grading degree is 50%, and the oxygen doping amount is 11.26 at-%; the specific surface area of the nitrogen-doped microporous active coke for denitration is 1200m2(ii)/g; the nitrogen doping amount is 4 at-%.
The process method comprises the following steps: containing SO2、NOx、O2、H2The flue gas after dust removal of O enters a desulfurization reactor 2 to catalyze SO under the action of graded-hole active coke doped with oxygen functional groups2Oxidation to SO3And combined with H in the flue gas2Conversion of O to H2SO4The saturated sulfur capacity reaches 100mg/g, and the desulfurization rate reaches 95 percent; the saturated active coke is removed by adsorption and is thermally regenerated by a regeneration system 3 to obtain high-concentration SO2Then mixed with part of fresh coke and enters a desulfurization reactor 2 for circulation; the desulfurized and dehydrated flue gas enters a denitration reactor 6, nitrogen-doped microporous active coke is used as a catalyst, and NH is sprayed into the flue gas3Under the action of (2) removing NO in the smokexReduction to N2And H2O, the denitration rate is as high as 90%.
Example 2:
an efficient low-temperature combined desulfurization and denitrification system and method based on active coke function zoning is shown as a working mode 2 in figure 2. The system consists of an oxygen-doped hierarchical pore active coke storage bin 1, a nitrogen-doped micropore active coke storage bin 5, a desulfurization and denitrification single fluidized bed reactor, an ammonia spraying system 4 and a regeneration system 3. The working temperature in the desulfurization and denitrification reactor is 80 ℃, and the flue gas flow is 3 m/s; denitrated part NH3With NO in the flue gasxIn a molar ratio of 1: 1.1. the active coke catalyst in the reactor is powdery and has the size of 100-200 mm, wherein the specific surface area of the oxygen-doped hierarchical pore active coke for desulfurization is 1000m2The grading degree is 60 percent, and the oxygen doping amount is 10at percent; the specific surface area of the nitrogen-doped microporous active coke for denitration is 1300m2(ii)/g; the nitrogen doping amount is 5 at-%.
The process method comprises the following steps: containing SO2、NOx、O2、H2The flue gas after dust removal of O enters a desulfurization area at the lower part of the single fluidized bed reactor to catalyze SO under the action of the oxygen functional group-doped hierarchical porous active coke2Oxidation toSO3And combined with H in the flue gas2Conversion of O to H2SO4The saturated sulfur capacity reaches 120mg/g, and the desulfurization rate reaches 98 percent; the saturated active coke is adsorbed and removed, and is washed and regenerated by a regeneration system to obtain high-concentration H2SO4Then mixing with part of fresh coke and entering a desulfurization reactor for circulation; the desulfurized and dehydrated flue gas enters a denitration reactor 6, nitrogen-doped microporous active coke is used as a catalyst, and NH is sprayed into the flue gas3Under the action of (2) removing NO in the smokexReduction to N2And H2O, the denitration rate is as high as 95 percent.
Claims (8)
1. The utility model provides a desulfurization deNOx systems is united to high-efficient low temperature based on active burnt function subregion which characterized in that: the system comprises an oxygen-doped hierarchical pore active coke storage bin (1), a desulfurization reactor (2), a regeneration system (3), an ammonia spraying system (4), a nitrogen-doped microporous active coke storage bin (5) and a denitration reactor (6);
the oxygen-doped graded-hole active coke storage bin (1) is communicated with the desulfurization reactor (2), the nitrogen-doped microporous active coke storage bin (5) is communicated with the denitration reactor (6), the bottom of the desulfurization reactor (2) is communicated with the regeneration system (3), and the ammonia spraying system (4) is arranged at or in front of an inlet of the denitration reactor (6);
the desulfurization reactor (2) and the denitration reactor (6) are in a double-reactor parallel mode or a single-reactor up-down series mode; the arrangement mode of the active coke catalyst in the desulfurization reactor (2) and the denitration reactor (6) is one of a fixed bed, a moving bed and a fluidized bed.
2. A method for combined desulfurization and denitrification by using the system of claim 1, which is characterized in that: the method comprises the following steps:
the method comprises the following steps: the flue gas after dust removal enters a desulfurization reactor (2), active coke with oxygen-doped hierarchical pores is used as a catalyst, and oxygen functional groups are used for reacting with O2The catalytic activation of the catalyst and the functions of micropores and mesopores in adsorption reaction and product transportation and migration are realized to realize SO2Catalytic oxidation to SO3And combined with H in the flue gas2Conversion of O intoH2SO4；
Step two: the saturated active coke is removed by adsorption and regenerated by a regeneration system (3) to obtain high-concentration SO2/H2SO4Recycling the product, mixing with part of fresh coke, and entering a desulfurization reactor (2) for circulation;
step three: the flue gas after desulfurization and dehydration enters a denitration reactor (6), nitrogen-doped microporous active coke is used as a catalyst, and the catalytic oxidation capacity of nitrogen-containing functional groups and a microporous structure to NO is utilized to spray NH3Under the action of (2) removing NO in the smokexReduction to N2And H2O。
3. The efficient low-temperature combined desulfurization and denitrification method based on the active coke functional partition as claimed in claim 1, wherein the method comprises the following steps: in the second step, the regeneration is thermal regeneration or water washing regeneration; the inlet of the regeneration system is connected with the active coke outlet of the desulfurization reactor.
4. The efficient low-temperature combined desulfurization and denitrification method based on the active coke functional partition as claimed in claim 1, wherein the method comprises the following steps: in the third step, the ammonia gas sprayed by the ammonia spraying system (4) and the desulfurized flue gas are uniformly mixed in front of the denitration reactor (6), and pure NH is added3NH being 5% of the total flow of the flue gas3With NO in the flue gasxThe molar ratio of (A) to (B) is controlled to be 1-1.2: 1.
5. the efficient low-temperature combined desulfurization and denitrification method based on the active coke functional partition as claimed in claim 1, wherein the method comprises the following steps: the flow velocity of flue gas in the desulfurization reactor (2) and the denitration reactor (6) is 1-5 m/s, the operating temperature in the desulfurization reactor (2) is 50-120 ℃, and the relative humidity is 6-12%; the operation temperature in the denitration reactor (6) is 80-200 ℃.
6. The efficient low-temperature combined desulfurization and denitrification method based on the active coke functional partition as claimed in claim 1, wherein the method comprises the following steps: the active coke catalyst is from a corresponding active coke storage bin, is in the form of one of powder, granules or column, and has the size of 1 mu m-10 mm.
7. The efficient low-temperature combined desulfurization and denitrification method based on the active coke functional partition as claimed in claim 1, wherein the method comprises the following steps: the specific surface area of the oxygen-doped hierarchical pore active coke is 300-1500 m2The grading degree is 10% -60%; the oxygen doping amount is 4 to 20 at-%.
8. The efficient low-temperature combined desulfurization and denitrification method based on the active coke functional partition as claimed in claim 1, wherein the method comprises the following steps: the specific surface area of the nitrogen-doped microporous active coke is 500-2000 m2The nitrogen doping amount is 1 to 15 at-%.
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