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CN111974342A - Combined adsorbent for flue gas desulfurization and denitration and flue gas desulfurization and denitration method - Google Patents

Combined adsorbent for flue gas desulfurization and denitration and flue gas desulfurization and denitration method Download PDF

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CN111974342A
CN111974342A CN201910438907.9A CN201910438907A CN111974342A CN 111974342 A CN111974342 A CN 111974342A CN 201910438907 A CN201910438907 A CN 201910438907A CN 111974342 A CN111974342 A CN 111974342A
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adsorbent
temperature
flue gas
desulfurization
low
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陈航
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Shanghai Zhisheng Industrial Development Co ltd
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Shanghai Zhisheng Industrial Development Co ltd
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Abstract

The invention relates to the technical field of desulfurization and denitrification processes, in particular to a combined adsorbent for desulfurization and denitrification of flue gas and a desulfurization and denitrification method of flue gas. The flue gas desulfurization and denitrification method comprises the following steps: dedusting flue gas; performing combined adsorption, desulfurization and denitrification; adsorbent regeneration and sulfur dioxide solidification. The invention solves the problems of high desulfurization and denitrification cost, no reutilization of desulfurizer and secondary pollution in the prior art, has the characteristics of no water consumption, no low-quality byproducts, no consumption of lime and synthetic ammonia with large environmental protection pressure, small investment and occupied area, low adsorbent loss, long service life, high pollutant removal rate, no secondary pollution, realization of resource utilization of sulfur-containing flue gas, good industrial application prospect and can be used for flue gas treatment of power plants, steel plants and petrochemical plants.

Description

Combined adsorbent for flue gas desulfurization and denitration and flue gas desulfurization and denitration method
Technical Field
The invention relates to the technical field of desulfurization and denitrification processes, in particular to a combined adsorbent for flue gas desulfurization and denitrification and a flue gas desulfurization and denitrification method.
Background
There are about ten kinds of flue gas desulfurization technologies which are currently industrialized and researched at home and abroad, and the methods can be divided into a dry method and a wet method in terms of process, and can be divided into a abandoning method and a recycling method in terms of recycling of a desulfurizing agent. Among the main methods that have been industrialized or tried in the middle are: 1) ammonium sulfite method; 2) citrate method; 3) wet desulfurization with activated carbon; 4) producing a phosphorus-ammonia compound fertilizer by wet desulphurization; 5) desulfurizing by an electron beam method; 6) lime-gypsum desulfurization, and the like.
Currently, the field of flue gas desulfurization is widely applied to wet desulfurization technologies and semi-dry desulfurization technologies represented by an ammonia method, a lime/limestone method, a double-alkali method, a magnesium oxide method and the like. The wet desulphurization has high absorption and utilization rate, but slurry of lime/limestone-gypsum method, double alkali method and magnesium oxide method contains tiny hydrophilic ions, is carried out by flue gas and is discharged into the atmosphere, and meanwhile, sulfur dioxide, sulfur trioxide, hydrogen chloride, hydrogen fluoride, nitrogen oxide, harmful organic matters, bacteria and the like are easily adsorbed on the surfaces of the particles, so that the content of suspended particles (generally known as PM100, PM10, PM2.5 and the like) in the atmosphere is obviously increased, and further haze and atmospheric photochemical reaction phenomena are caused, and serious environmental pollution is caused. The sodium (potassium) sulfite desulfurization process, the Welman-Lord desulfurization process and the organic acid-organic acid salt buffer solution desulfurization process have the disadvantages of large energy consumption of regenerated steam and low regeneration rate, so the industrialization difficulty is high. Ammonia in ammonia desulphurization is highly corrosive and causes equipment corrosion, and the production process of ammonia is a high-energy-consumption and high-pollution process. Compared with wet desulphurization, the semi-dry desulphurization has the advantages of less equipment corrosion, no obvious temperature drop, contribution to exhaust diffusion of a chimney, relatively low desulphurization efficiency and slow reaction speed.
Although it has already been adoptedMany effective measures are taken to prevent and treat atmospheric pollution and reduce SO2The emission of the boiler is about 4000 (or more) power plants without the desulfurization and denitrification devices, and the total emission accounts for about 96 percent of the total number of the power plants. In addition, about 10 ten thousand large-capacity industrial boilers are required to be equipped with desulfurization devices, and thus, the environmental situation is still not optimistic. To achieve SO2The requirement of reducing the total emission is that most power plants actively seek reliable technical performance, the construction cost is 200 yuan/KW and SO is removed2The operation cost is less than 300 yuan/ton, and the resources can be comprehensively utilized.
The mainstream technology in the field of pellet sintering flue gas denitration is NH3SCR denitration, where the SCR technology uses a catalyst, the catalytic action reduces the activation energy of the reaction. In a steel plant, because the temperature of flue gas is very low (200-300 ℃), a low-temperature denitration catalyst is needed to be adopted to carry out denitration reaction in the temperature range, and ammonia gas is needed to be sprayed into the flue gas as a reducing agent.
The independent desulfurization and denitration process not only occupies a large area, but also has high investment and operation cost. Meanwhile, the desulfurization and denitrification technology has the advantages of reducing equipment configuration, saving space, wide material source, low price, regeneration and cyclic utilization and the like. Among them, the dry desulfurization and denitration integrated technology represented by the activated carbon (coke) technology is the technology that makes the most use of heat energy in flue gas.
The method has the advantages of large investment and high operating cost, or the desulfurizing agent can not be reused after desulfurization, secondary pollution is caused, and the stacking of waste residues in a large-capacity boiler of a power plant is limited by the transportation cost or the site stacking, so that the method is a key factor influencing the commercialization of the desulfurization technology. Therefore, the technologies are difficult to popularize and use in a large scale in China at present. The flue gas desulfurization technology which is applied in large-scale commercialization internationally has high technical maturity, and power plants are introduced in China, but the technology has high cost and large investment, and the byproduct gypsum is not comprehensively utilized and is not successfully used.
Disclosure of Invention
In view of the above disadvantages of the prior art, the present invention is to provide a combined adsorbent for desulfurization and denitrification of flue gas, which is used to solve the problems of high desulfurization and denitrification cost, no reutilization of desulfurizing agent, and secondary pollution in the prior art, and also to provide a method for desulfurization and denitrification of flue gas using the combined adsorbent; the invention has the advantages of no water consumption, no low-quality by-products, no consumption of lime and synthetic ammonia with large environmental protection pressure, small investment and land occupation, low adsorbent loss, long service life, high pollutant removal rate, no secondary pollution, realization of flue gas resource utilization and good industrial application prospect.
In order to attain the above and other related objects,
in a first aspect of the invention, a combined adsorbent for flue gas desulfurization and denitration is provided, wherein the combined adsorbent consists of a low-temperature adsorbent and a high-temperature adsorbent;
the high-temperature adsorbent comprises the following components in parts by weight: 10-80 parts of a porous carrier, 1-75 parts of a metal oxide and 15-90 parts of a binder;
the low-temperature adsorbent comprises the following components in parts by weight: 50-85 parts of a porous carrier, 0-40 parts of a metal oxide and 15-50 parts of a binder.
The combined adsorbent adopts the technical scheme of combining the high-temperature adsorbent and the low-temperature adsorbent to realize SO in the flue gas2And deep removal of NOx and SO by Claus process2Converting into resource utilization of sulfur. Wherein the high-temperature adsorbent can be directly used as a low-temperature adsorbent, and is more convenient in the process of preparing raw materials.
In an embodiment of the present invention, the combined adsorbent consists of a low temperature adsorbent and a high temperature adsorbent;
the high-temperature adsorbent comprises the following components in parts by weight: 40-65 parts of a porous carrier, 10-40 parts of a metal oxide and 15-25 parts of a binder;
the low-temperature adsorbent comprises the following components in parts by weight: 60-85 parts of a porous carrier, 0-15 parts of a metal oxide and 20-30 parts of a binder.
The weight ratio is controlled within the range, the adsorption effect is good, and the cost is saved.
In the embodiment of the invention, the specific surface area of the porous carrier used for the high-temperature adsorbent is more than or equal to 100m2The specific surface area of a porous carrier used by the low-temperature adsorbent is more than or equal to 200m2/g。
In the embodiment of the invention, the specific surface area of the porous carrier used for the high-temperature adsorbent is more than or equal to 200m2The specific surface area of a porous carrier used by the low-temperature adsorbent is more than or equal to 350m2(ii) in terms of/g. Under the condition of higher specific surface area, the adsorption effect is better, and the desulfurization and denitrification rate is higher.
In the embodiment of the invention, the porous carrier used by the high-temperature adsorbent is at least one of a molecular sieve, silica and/or activated carbon alumina; the porous carrier used by the low-temperature adsorbent is at least one of a molecular sieve, silicon oxide and/or activated carbon; the molecular sieve used by the high-temperature adsorbent is an X molecular sieve, a Y molecular sieve, a mercerized molecular sieve, a ZSM-5 molecular sieve, a beta molecular sieve or an MCM-41 molecular sieve; the molecular sieve used by the low-temperature adsorbent is selected from an A molecular sieve, an X molecular sieve, a Y molecular sieve, a mercerized molecular sieve or a ZSM-5 molecular sieve. .
The molecular sieve is an aluminosilicate compound with cubic lattice, has a developed microporous structure, has a large specific surface area which can reach 300-1000 m 2(ii) in terms of/g. The molecular sieve has uniform hole diameter and highly polarized crystal surface, can adsorb molecules smaller than the diameter into the hole cavity, and has preferential adsorption capacity for polar molecules and unsaturated molecules, so that the molecular sieve can separate the molecules with different polarity degrees, saturation degrees, molecular sizes and boiling points, i.e. has the function of sieving the molecules, and is called as the molecular sieve. The molecular sieve has the advantages of high adsorption capacity, strong thermal stability and the like which are not possessed by other adsorbents, so that the molecular sieve can be widely applied.
The porous silicon oxide is white, loose, amorphous, nontoxic, tasteless, odorless and pollution-free nonmetal oxide, the primary particle size of the porous silicon oxide is between 7 and 80nm, and the specific surface area is generally more than 300-2/g. Due to the nanometer effect, the material shows excellent reinforcement, thickening, thixotropy and insulationThe product has the properties of edge, extinction, sagging prevention and the like, so the product is widely applied to the polymer industrial fields of rubber, plastics, paint, adhesive, sealant and the like.
The active carbon is a black porous solid carbon, and is produced by crushing and molding coal or carbonizing and activating uniform coal particles. The main component is carbon and contains a small amount of elements such as oxygen, hydrogen, sulfur, nitrogen, chlorine and the like. The specific surface area of the common activated carbon is 500-1700 m 2Between/g. Has strong adsorption performance and is an industrial adsorbent with wide application.
In an embodiment of the present invention, the metal oxide is at least one of oxides of alkali metals, alkaline earth metals, rare earths, and transition metals.
In an embodiment of the present invention, the binder is at least one of alumina, kaolin, bentonite, montmorillonite, attapulgite and/or diatomaceous earth.
In a second aspect of the present invention, there is provided a flue gas desulfurization and denitrification method using the combined adsorbent, comprising the following steps:
step one, flue gas dust removal: conveying the flue gas to be treated into an electric dust removal device for dust removal pretreatment;
step two, adsorption desulfurization and denitration: conveying the dedusted flue gas into a reactor loaded with a high-temperature adsorbent, performing desulfurization and denitrification at the temperature of 300-650 ℃, recovering heat of the desulfurized and denitrified high-temperature flue gas, conveying the desulfurized and denitrified high-temperature flue gas into the reactor loaded with the low-temperature adsorbent, and performing desulfurization and denitrification at the temperature of 20-120 ℃ to obtain gas subjected to desulfurization and denitrification;
step three, adsorbent regeneration: introducing a high-temperature regenerant into a high-temperature adsorbent reactor, separating sulfur dioxide adsorbed in the high-temperature adsorbent at the temperature of more than 300 ℃, introducing the regenerated tail gas rich in sulfur dioxide into a Claus unit to produce sulfur, and putting the regenerated high-temperature adsorbent into use again; introducing the low-temperature regenerant into a low-temperature adsorbent reactor, separating sulfur dioxide adsorbed in the low-temperature adsorbent at the temperature of more than 200 ℃, and feeding the regeneration tail gas rich in sulfur dioxide into a Claus unit to produce the regenerated sulfur, so as to reuse the regenerated low-temperature adsorbent.
The combined adsorbent adopts the technical scheme of combining the high-temperature adsorbent and the low-temperature adsorbent to realize SO in the flue gas2And deep removal of NOx and SO by Claus process2The sulfur is converted into the sulfur for resource utilization, and the method has the characteristics of no water consumption, no low-quality byproducts, no consumption of lime and synthetic ammonia with large environmental protection pressure, small investment and occupied area, low loss of the adsorbent, long service life, high pollutant removal rate, no secondary pollution and good industrial application prospect.
Wherein the dust removal step is a necessary procedure in all flue gas treatment processes; performing high-temperature adsorption at the temperature of 300-650 ℃, introducing the dedusted flue gas into a high-temperature adsorbent, and performing SO adsorption2While being adsorbed, NOXIs reduced to N2The high-temperature flue gas removes most of SO2And NOXThen, the high-temperature flue gas can be used for generating steam or other purposes, such as heating boiler air supply to recover heat, and the treated flue gas can be disregarded for dew point corrosion, so that the temperature of the flue gas can be reduced to normal temperature, the heat recovery rate is greatly improved, and the economic benefit is remarkable; carrying out low-temperature adsorption at the temperature of 20-120 ℃ to deeply remove SO in the flue gas2Can remove SO in the flue gas2The content is reduced to ppm level, which is obviously lower than the current control index. When the catalyst is put into use for the first time, the high-temperature adsorbent can be activated by adopting a regenerant, and the process conditions are the same as or close to those of the regeneration process.
The Claus process comprises a primary Claus reactor, a secondary Claus reactor, a primary sulfur condenser, a secondary sulfur condenser and a secondary reheater; the first-stage and second-stage Claus reactors are filled with high-efficiency active catalysts, the flue gas after catalytic reduction firstly enters the first-stage Claus reactor for catalytic reaction, then enters a first-stage sulfur condenser connected with a pipeline of the first-stage Claus reactor, the separated liquid sulfur enters a liquid sulfur pool, the flue gas enters the second-stage Claus reactor for continuous catalytic reaction, the flue gas after secondary catalytic reaction enters a second-stage reheater connected with a pipeline and then enters a second-stage sulfur condenser, the liquid sulfur separated by condensation treatment enters the liquid sulfur pool, and the sulfur-containing tail gas of the Claus process enters a high-temperature adsorbent bed for recovery.
In the embodiment of the present invention, the reactor in the second step is a fixed bed reactor or a fluidized bed reactor.
In embodiments of the invention, the reactor employs a three-or four-vessel flow scheme. In the two flow modes, four flows are adopted, namely, two high-temperature adsorbents are regenerated by one, and two low-temperature adsorbents are regenerated by one; the three-device flow path shares one regenerator, in this case, two agents are actually one agent to respectively utilize the functions of chemical adsorption and physical adsorption. If the four-device mode is adopted, namely the high-temperature and low-temperature adsorbents are different, the low-temperature adsorbent can be regenerated by using tail gas at the outlet of the high-temperature adsorbent, and the regenerated tail gas returns to the high-temperature adsorbent, so that the four-device mode is very convenient.
For a fixed bed reactor and a fluidized bed reactor, when a high-temperature adsorbent can not be used as a low-temperature adsorbent, four-device flow can be adopted for respective regeneration; when the high-temperature adsorbent can be used as the low-temperature adsorbent, a three-device flow can be adopted, and three devices are switched to regenerate.
In the embodiment of the invention, the high-temperature regenerant is carbon monoxide, C1-C12 hydrocarbon, hydrogen or carbon powder; the low-temperature regenerant is nitrogen, carbon dioxide, carbon monoxide, C1-C12 hydrocarbon, hydrogen or carbon powder. When a high temperature adsorbent is used as the low temperature adsorbent, both can be regenerated under the same regeneration conditions.
As described above, the combined adsorbent for flue gas desulfurization and denitration and the flue gas desulfurization and denitration method provided by the invention have the following beneficial effects: the combined adsorbent adopts the technical scheme of combining the high-temperature adsorbent and the low-temperature adsorbent to realize SO in the flue gas2And the deep removal of NOx can reduce the content of SO2 in the flue gas to 30ppm, the removal rate is more than or equal to 95 percent and is obviously lower than the current control index, and the realization of SO removal by using the Claus process2The sulfur is converted into the sulfur for resource utilization, and the method has the characteristics of no water consumption, no low-quality byproducts, no consumption of lime and synthetic ammonia with large environmental protection pressure, small investment and occupied area, low loss of the adsorbent, long service life, high pollutant removal rate, no secondary pollution and good industrial application prospect.
Drawings
FIG. 1 is a flow chart of the four-device process of desulfurization and denitrification of flue gas.
FIG. 2 is a flow chart of the process of the three devices for desulfurization and denitrification of flue gas.
Detailed Description
The following description of the embodiments of the present invention is provided for illustrative purposes, and other advantages and effects of the present invention will become apparent to those skilled in the art from the present disclosure.
Example 1
A combined adsorbent for desulfurization and denitrification of flue gas consists of a low-temperature adsorbent and a high-temperature adsorbent;
the high-temperature adsorbent comprises the following components in parts by weight: 35 parts of mercerized molecular sieve, 15 parts of ferric oxide and 15 parts of binder;
the low-temperature adsorbent comprises the following components in parts by weight: 50 parts of MCM-41 molecular sieve, 5 parts of magnesium oxide and 15 parts of binder;
wherein the specific surface area of the mercerized molecular sieve is 280m2Per g, the specific surface area of the MCM-41 molecular sieve is 1156m2/g。
The binder is alumina and kaolin according to the mass ratio of 1: 6, mixing to obtain the product.
A flue gas desulfurization and denitrification method using the combined adsorbent comprises the following steps:
step one, flue gas dust removal: conveying the flue gas to be treated into an electric dust removal device for dust removal pretreatment;
Step two, adsorption desulfurization and denitration: conveying the dedusted flue gas into a four-flow fixed bed reactor loaded with a high-temperature adsorbent, desulfurizing and denitrating at the temperature of 300 ℃, recovering heat of the desulfurized and denitrated high-temperature flue gas, conveying the desulfurized and denitrated high-temperature flue gas into a reactor loaded with a low-temperature adsorbent, and desulfurizing and denitrating at the temperature of 120 ℃ to obtain gas subjected to desulfurization and denitrating;
step three, adsorbent regeneration: introducing carbon monoxide into a high-temperature adsorbent reactor, separating sulfur dioxide adsorbed in the high-temperature adsorbent at the temperature of 350 ℃, introducing the regenerated tail gas rich in sulfur dioxide into a Claus unit to produce sulfur, and putting the regenerated high-temperature adsorbent into use again; introducing the high-temperature adsorbent tail gas into a low-temperature adsorbent reactor, separating sulfur dioxide adsorbed in the low-temperature adsorbent at the temperature of 250 ℃, returning the regenerated tail gas to the inlet of the high-temperature adsorbent reactor, and putting the regenerated low-temperature adsorbent into use again.
SO in unadsorbed flue gas in the above examples2The content of SO in the gas is 1023ppm after the adsorption is finished235ppm of SO2The removal rate is 96.6 percent; the activity of the regenerated high-temperature adsorbent is 96% of that of the previously unreduced high-temperature adsorbent, and the activity of the regenerated low-temperature adsorbent is 97% of that of the previously unreduced low-temperature adsorbent.
Example 2
A combined adsorbent for desulfurization and denitrification of flue gas consists of a low-temperature adsorbent and a high-temperature adsorbent;
the high-temperature adsorbent comprises the following components in parts by weight: 40 parts of ZSM-5 molecular sieve, 20 parts of calcium oxide and 15 parts of bentonite; the low-temperature adsorbent comprises the following components in parts by weight: 50 parts of silicon oxide, 20 parts of bentonite;
wherein the specific surface area of the ZSM-5 molecular sieve is 350m2(ii)/g, silica specific surface area is 600m2/g。
A flue gas desulfurization and denitrification method using the combined adsorbent comprises the following steps:
step one, flue gas dust removal: conveying the flue gas to be treated into an electric dust removal device for dust removal pretreatment;
step two, adsorption desulfurization and denitration: conveying the dedusted flue gas into a four-flow fluidized bed reactor loaded with a high-temperature adsorbent, desulfurizing and denitrating at the temperature of 450 ℃, recovering heat of the desulfurized and denitrated high-temperature flue gas, conveying the desulfurized and denitrated high-temperature flue gas into a reactor loaded with a low-temperature adsorbent, and desulfurizing and denitrating at the temperature of 100 ℃ to obtain gas subjected to desulfurization and denitrating;
step three, adsorbent regeneration: introducing hydrogen into a high-temperature adsorbent reactor, separating sulfur dioxide adsorbed in the high-temperature adsorbent at the temperature of 400 ℃, allowing the regenerated tail gas rich in sulfur dioxide to enter a Claus unit to produce sulfur, and putting the regenerated high-temperature adsorbent into use again; introducing carbon monoxide into a low-temperature adsorption reactor, separating sulfur dioxide adsorbed in the low-temperature adsorbent at the temperature of 200 ℃, returning the regenerated tail gas to the inlet of the high-temperature adsorbent reactor, and putting the regenerated low-temperature adsorbent into use again.
SO in unadsorbed flue gas in the above examples2The content of SO in the gas after adsorption is 950ppm2Content of 30ppm, SO2The removal rate is 96.8 percent; the activity of the regenerated high-temperature adsorbent was 97% of that of the previously unreregenerated adsorbent, and the activity of the regenerated low-temperature adsorbent was 97% of that of the previously unreregenerated adsorbent.
Example 3
A combined adsorbent for desulfurization and denitrification of flue gas consists of a low-temperature adsorbent and a high-temperature adsorbent;
the high-temperature adsorbent comprises the following components in parts by weight: 60 parts of Y-type molecular sieve, 40 parts of nickel oxide and 25 parts of binder;
the low-temperature adsorbent comprises the following components in parts by weight: 60 parts of activated carbon and 25 parts of binder;
wherein the specific surface area of the Y-type molecular sieve is 742m2Per g, the surface area of the activated carbon is 890m2/g；
The binder is alumina and attapulgite according to a mass ratio of 1: 5 mixing to obtain the final product.
A flue gas desulfurization and denitrification method using the combined adsorbent comprises the following steps:
step one, flue gas dust removal: conveying the flue gas to be treated into an electric dust removal device for dust removal pretreatment;
step two, adsorption desulfurization and denitration: conveying the dedusted flue gas into a three-flow fluidized bed reactor loaded with a high-temperature adsorbent, desulfurizing and denitrating at the temperature of 500 ℃, recovering heat of the desulfurized and denitrated high-temperature flue gas, conveying the desulfurized and denitrated high-temperature flue gas into a reactor loaded with a low-temperature adsorbent, and desulfurizing and denitrating at the temperature of 120 ℃ to obtain gas subjected to desulfurization and denitrating;
Step three, adsorbent regeneration: introducing carbon powder gas into a high-temperature adsorbent and a high-temperature regenerant, adding the carbon powder gas and the high-temperature regenerant into a regeneration reactor together, separating sulfur dioxide adsorbed in the high-temperature adsorbent out at the temperature of 500 ℃, introducing the regeneration tail gas rich in the sulfur dioxide into a Claus unit to produce sulfur, and putting the regenerated high-temperature adsorbent into use again; introducing carbon monoxide into a regeneration reactor, separating sulfur dioxide adsorbed in the low-temperature adsorbent at the temperature of 300 ℃, returning the regeneration tail gas to the inlet of the high-temperature adsorbent reactor, and putting the regenerated low-temperature adsorbent into use again.
SO in unadsorbed flue gas in the above examples2The content of SO in the gas after adsorption is 1020ppm2Content of 30ppm, SO2The removal rate is 97.0 percent; the activity of the regenerated high-temperature adsorbent is 96% of that of the previously unreregenerated high-temperature adsorbent, and the activity of the regenerated low-temperature adsorbent is 95% of that of the previously unreregenerated low-temperature adsorbent.
Example 4
A combined adsorbent for desulfurization and denitrification of flue gas consists of a low-temperature adsorbent and a high-temperature adsorbent;
the high-temperature adsorbent comprises the following components in parts by weight: 60 parts of a Y-type molecular sieve, 10 parts of copper oxide and 20 parts of a binder;
The high-temperature adsorbent comprises the following components in parts by weight: 60 parts of a Y-type molecular sieve, 10 parts of copper oxide and 20 parts of a binder;
wherein the specific surface area of the Y-type molecular sieve is 734m2(ii)/g; the binder is alumina and attapulgite according to a mass ratio of 1: 4, mixing the components.
A flue gas desulfurization and denitrification method using the combined adsorbent comprises the following steps:
step one, flue gas dust removal: conveying the flue gas to be treated into an electric dust removal device for dust removal pretreatment;
step two, adsorption desulfurization and denitration: conveying the dedusted flue gas into a three-flow fluidized bed reactor loaded with a high-temperature adsorbent, desulfurizing and denitrating at the temperature of 500 ℃, recovering heat of the desulfurized and denitrated high-temperature flue gas, conveying the desulfurized and denitrated high-temperature flue gas into a reactor loaded with a low-temperature adsorbent, and desulfurizing and denitrating at the temperature of 100 ℃ to obtain gas subjected to desulfurization and denitrating;
step three, adsorbent regeneration: introducing carbon monoxide into a regeneration reactor with a high-temperature adsorbent and a low-temperature adsorbent, separating sulfur dioxide adsorbed in the high-temperature adsorbent out at the temperature of 500 ℃, introducing the regeneration tail gas rich in sulfur dioxide into a Claus unit to produce sulfur, and putting the regenerated high-temperature adsorbent and the regenerated low-temperature adsorbent into use again.
SO in unadsorbed flue gas in the above examples2The content of SO in the gas after adsorption is 920ppm2Content of 31ppm, SO2The removal rate is 96.6 percent; the activity of the regenerated high-temperature adsorbent was 95% of that of the previously unreregenerated adsorbent, and the activity of the regenerated low-temperature adsorbent was 95% of that of the previously unreregenerated adsorbent.
Example 5
A combined adsorbent for desulfurization and denitrification of flue gas consists of a low-temperature adsorbent and a high-temperature adsorbent;
the high-temperature adsorbent comprises the following components in parts by weight: 40 parts of silicon oxide, 10 parts of copper oxide and 20 parts of binder;
the high-temperature adsorbent comprises the following components in parts by weight: 80 parts of Y-type molecular sieve and 20 parts of binder;
wherein the specific surface area of the silicon oxide is 550m2Specific surface area of 750 m/g, Y type molecular sieve2/g；
The binder is alumina and attapulgite according to a mass ratio of 1: 4, mixing the components.
A flue gas desulfurization and denitrification method using the combined adsorbent comprises the following steps:
step one, flue gas dust removal: conveying the flue gas to be treated into an electric dust removal device for dust removal pretreatment;
step two, adsorption desulfurization and denitration: conveying the dedusted flue gas into a three-flow fluidized bed reactor loaded with a high-temperature adsorbent, desulfurizing and denitrating at the temperature of 500 ℃, recovering heat of the desulfurized and denitrated high-temperature flue gas, conveying the desulfurized and denitrated high-temperature flue gas into a reactor loaded with a low-temperature adsorbent, and desulfurizing and denitrating at the temperature of 100 ℃ to obtain gas subjected to desulfurization and denitrating;
Step three, adsorbent regeneration: introducing carbon powder gas into a high-temperature adsorbent and a high-temperature regenerant, adding the carbon powder gas and the high-temperature regenerant into a regeneration reactor together, separating sulfur dioxide adsorbed in the high-temperature adsorbent out at the temperature of 400 ℃, introducing the regeneration tail gas rich in the sulfur dioxide into a Claus unit to produce sulfur, and putting the regenerated high-temperature adsorbent into use again; introducing carbon monoxide into a regeneration reactor, separating sulfur dioxide adsorbed in the low-temperature adsorbent at the temperature of 200 ℃, returning the regeneration tail gas to the inlet of the high-temperature adsorbent reactor, and putting the regenerated low-temperature adsorbent into use again.
SO in unadsorbed flue gas in the above examples2The content is 1150ppm, SO in the gas is absorbed2A content of 40ppm, SO2The removal rate is 96.5 percent; the activity of the regenerated high-temperature adsorbent is 96% of that of the previously unreduced high-temperature adsorbent, and the activity of the regenerated low-temperature adsorbent is 97% of that of the previously unreduced low-temperature adsorbent.
In conclusion, the method has the characteristics of no water consumption, no low-quality byproducts, no consumption of lime and synthetic ammonia with large environmental protection pressure, small investment and land occupation, low adsorbent loss, long service life, high pollutant removal rate, no secondary pollution and good industrial application prospect. Therefore, the invention effectively overcomes various defects in the prior art and has high industrial utilization value.
The foregoing embodiments are merely illustrative of the principles and utilities of the present invention and are not intended to limit the invention. Any person skilled in the art can modify or change the above-mentioned embodiments without departing from the spirit and scope of the present invention. Accordingly, it is intended that all equivalent modifications or changes which can be made by those skilled in the art without departing from the spirit and technical spirit of the present invention be covered by the claims of the present invention.

Claims (10)

1. The combined adsorbent for desulfurization and denitrification of flue gas is characterized by consisting of a low-temperature adsorbent and a high-temperature adsorbent;
the high-temperature adsorbent comprises the following components in parts by weight: 10-80 parts of a porous carrier, 1-75 parts of a metal oxide and 15-90 parts of a binder;
the low-temperature adsorbent comprises the following components in parts by weight: 50-85 parts of a porous carrier, 0-40 parts of a metal oxide and 15-50 parts of a binder.
2. The combined adsorbent for desulfurization and denitrification of flue gas according to claim 1, characterized in that: the high-temperature adsorbent comprises the following components in parts by weight: 40-65 parts of a porous carrier, 10-40 parts of a metal oxide and 15-25 parts of a binder;
The low-temperature adsorbent comprises the following components in parts by weight: 60-85 parts of a porous carrier, 0-15 parts of a metal oxide and 20-30 parts of a binder.
3. The combined adsorbent for desulfurization and denitrification of flue gas according to claim 1 or 2, characterized in that: the specific surface area of the porous carrier used by the high-temperature adsorbent is more than or equal to 100m2The specific surface area of a porous carrier used by the low-temperature adsorbent is more than or equal to 200m2/g；
The metal oxide is at least one of oxides of alkali metals, alkaline earth metals, rare earths and transition metals;
the binder is at least one of alumina, kaolin, bentonite, montmorillonite, attapulgite and/or diatomite.
4. The combined adsorbent for desulfurization and denitrification of flue gas according to any one of claims 1 to 3, wherein: the specific surface area of the porous carrier used by the high-temperature adsorbent is more than or equal to 200m2/gThe specific surface area of the porous carrier used by the low-temperature adsorbent is more than or equal to 350m2/g。
5. The combined adsorbent for desulfurization and denitrification of flue gas according to any one of claims 1 to 4, wherein: the porous carrier used by the high-temperature adsorbent is at least one of molecular sieve, silicon oxide and/or aluminum oxide; the porous carrier used by the low-temperature adsorbent is at least one of a molecular sieve, silicon oxide and/or activated carbon.
6. The combined adsorbent for desulfurization and denitrification of flue gas according to claim 5, wherein: the molecular sieve used by the high-temperature adsorbent is an X molecular sieve, a Y molecular sieve, a mercerized molecular sieve, a ZSM-5 molecular sieve, a beta molecular sieve or an MCM-41 molecular sieve; the molecular sieve used by the low-temperature adsorbent is an A molecular sieve, an X molecular sieve, a Y molecular sieve, a mercerized molecular sieve or a ZSM-5 molecular sieve.
7. A flue gas desulfurization and denitrification method using the combined adsorbent of any one of claims 1 to 6, characterized by comprising the following steps:
step one, flue gas dust removal: conveying the flue gas to be treated into an electric dust removal device for dust removal pretreatment;
step two, adsorption desulfurization and denitration: conveying the dedusted flue gas into a reactor loaded with a high-temperature adsorbent, desulfurizing and denitrating at the temperature of 300-650 ℃, recovering heat of the desulfurized and denitrated high-temperature flue gas, conveying the desulfurized and denitrated high-temperature flue gas into the reactor loaded with the low-temperature adsorbent, and desulfurizing at the temperature of 20-120 ℃ to obtain gas subjected to desulfurization and denitrating;
step three, adsorbent regeneration: introducing a high-temperature regenerant into a high-temperature adsorbent reactor, separating sulfur dioxide adsorbed in the high-temperature adsorbent at the temperature of more than 300 ℃, introducing the regenerated tail gas rich in sulfur dioxide into a Claus unit to produce sulfur, and putting the regenerated high-temperature adsorbent into use again; introducing the low-temperature regenerant into a low-temperature adsorbent reactor, separating sulfur dioxide adsorbed in the low-temperature adsorbent at the temperature of more than 200 ℃, and feeding the regeneration tail gas rich in sulfur dioxide into a Claus unit to produce the regenerated sulfur, so as to reuse the regenerated low-temperature adsorbent.
8. The method for desulfurization and denitrification of flue gas by using combined adsorbent as claimed in claim 7, wherein: and the low-temperature adsorbent in the second step is the same as the high-temperature adsorbent, and the reactor is a three-flow fixed bed reactor or a three-flow fluidized bed reactor.
9. The method for desulfurization and denitrification of flue gas by using combined adsorbent as claimed in claim 7, wherein: and the low-temperature adsorbent and the high-temperature adsorbent in the second step are different, and the reactor is a four-flow fixed bed reactor or a four-flow fluidized bed reactor.
10. The method for desulfurization and denitrification of flue gas by using combined adsorbent as claimed in claim 7, wherein: the high-temperature regenerant is at least one of carbon monoxide, C1-C12 hydrocarbon, hydrogen and/or carbon powder gas; the low-temperature regenerant is at least one of nitrogen, carbon dioxide, carbon monoxide, C1-C12 hydrocarbons, hydrogen, air and/or high-temperature adsorbent tail gas.
CN201910438907.9A 2019-05-24 2019-05-24 Combined adsorbent for flue gas desulfurization and denitration and flue gas desulfurization and denitration method Pending CN111974342A (en)

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US11602727B2 (en) * 2019-02-20 2023-03-14 Sarp Industries Method for treating flue gas from combustion units

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US11602727B2 (en) * 2019-02-20 2023-03-14 Sarp Industries Method for treating flue gas from combustion units

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