CN112275139A - Exhaust gas treatment method and apparatus - Google Patents
Exhaust gas treatment method and apparatus Download PDFInfo
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- CN112275139A CN112275139A CN202011132219.9A CN202011132219A CN112275139A CN 112275139 A CN112275139 A CN 112275139A CN 202011132219 A CN202011132219 A CN 202011132219A CN 112275139 A CN112275139 A CN 112275139A
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- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
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- 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
- B01D53/8603—Removing sulfur compounds
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- 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
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- 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
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- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
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- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
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- B01D53/8662—Organic halogen compounds
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- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8668—Removing organic compounds not provided for in B01D53/8603 - B01D53/8665
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- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/90—Injecting reactants
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- B01D2258/00—Sources of waste gases
- B01D2258/02—Other waste gases
- B01D2258/0283—Flue gases
Abstract
The invention relates to a waste gas treatment method and a device thereof, in particular to a method for purifying gas containing pollutants and a system capable of executing the method, wherein the method comprises the following steps: a step of adsorption to contact the pollutant-containing gas with an adsorbent in a fluidized bed reactor; a separation step of introducing the adsorbent having adsorbed the contaminant into a gas-solid separation device to separate and recover the adsorbent having adsorbed the contaminant; a regeneration step of subjecting the adsorbent having adsorbed the contaminant to a heat treatment to desorb the contaminant and obtain a regenerated adsorbent, wherein in the regeneration step, at least a part of the regenerated adsorbent is introduced into the fluidized bed reactor, and the contaminant produced by the desorption is introduced into at least one condenser to be recovered.
Description
Technical Field
The invention belongs to the field of environmental protection, relates to a method and a device for treating waste gas containing pollutants, and particularly relates to a method and a device for treating and purifying industrial waste (flue gas).
Background
The porous medium adsorption method is used as an integrated removal technology for various pollutants in industrial smoke (waste gas), and can realize combined removal of SO2，NOxAnd VOCs, and has the advantages of high removal efficiency, small occupied area, capability of generating resource byproducts, no need of process water and wastewater treatment, and the like.
The technology for treating the industrial smoke (waste gas) by utilizing the porous medium adsorption method mainly realizes the purification of the industrial smoke (waste gas) through the adsorption, catalytic oxidation and catalytic reduction processes of the porous medium material on pollutant components in the smoke. For example, SO in flue gas at 100-200 deg.C2、O2And the water vapor is physically or chemically adsorbed on the porous medium material; the porous medium material which reaches the adsorption saturation can be heated to 400 ℃ in a regeneration reactor, and high-concentration SO is generated through the catalytic reduction reaction or thermal desorption of the porous medium material2The resource utilization of the sulfur is realized after collection, and the regenerated porous medium material can be recycled. In addition, in some cases, ammonia is injected into the adsorption reactor in the presence of a porous medium, and NO is generated under the catalytic action of the porous medium materialxBy reaction with ammonia to form N2And realizing the denitration process. The porous medium adsorption method also has the function of complete or certain combined removal of pollutants such as dust, partial heavy metals, hydrogen halide and the like in industrial smoke (waste gas).
From the research and literature of enterprises in the present stage, strengthening the adsorption efficiency of the porous adsorption material and improving the connection process of adsorption and desorption processes are a problem to be solved urgently in the process of purifying industrial smoke (waste gas) by a porous medium adsorption method. For the adsorption process of porous media, the prior art mostly adopts a fixed bed or moving bed reactor mode. The following problems exist in the practical application process:
(1) the problem of uneven gas phase flow field distribution is easily caused, the utilization rate of the porous adsorption material is low, the adhesion of the porous medium material is improved in the ammonia spraying process, and the flow field unevenness is aggravated;
(2) the bed layer has poor heat transfer effect and is easy to generate local hot spots;
(3) the system has poor operation continuity, and is not beneficial to the timely regeneration and cyclic utilization of the porous adsorption material;
(4) the process equipment is complex and the occupied space is large.
For example, reference 1 discloses a dry-method multi-pollutant system efficient purification reactor for low-temperature flue gas, which comprises 3-4 pretreatment beds, catalytic beds and adsorption beds connected in series, and has the advantages of compact structure and multi-pollution combined removal.
Reference 2 proposes a device and an operation method for adsorbing and regenerating VOCs, which are capable of adsorbing VOCs in a circulating fluidized bed reactor, degrading adsorbed VOCs by combining a plasma technology, and regenerating an adsorbent, and have the advantage of high purification efficiency. However, the technology of the patent is not suitable for simultaneously treating industrial flue gas containing high-concentration nitrogen oxides and sulfur dioxide.
Reference documents:
reference 1: CN 108261904A
Reference 2: CN 109173591A
Disclosure of Invention
Problems to be solved by the invention
The circulating fluidized bed as a recyclable reaction means for gas-solid reaction has a significant advantage over a conventional fixed fluidized bed (for example, reference 1). For example, the circulating fluidized bed disclosed in reference 2 can realize a rapid flow of the mixing system at a relatively high flow rate, and can allow most of the overflowed solid materials (such as solid catalyst, etc.) to be effectively recovered and returned back into the fluidized bed.
However, although a circulating reaction fluidized bed has been produced and practiced, in long-term industrial practice, the inventors of the present invention have also observed that:
on the one hand, for example, in reference 2, the solid adsorbent is first physically adsorbed with VOCs and the like in the fluidized bed, and then the organic VOCs are degraded into smaller (harmless) molecules by plasma bombardment to be discharged out of the fluidized bed reactor while rising to the plasma reaction zone, and in practice, such a treatment method depends on a single degradation treatment method, and as mentioned above, it is hard to say that it can cope with treatment of mixed industrial waste flue gas containing sulfur and nitrogen harmful substances.
On the other hand, as described above, the solid adsorbent used in reference 2 performs adsorption in the adsorption zone, and performs degradation of VOCs and desorption and regeneration of the solid adsorbent in the plasma reaction zone, and therefore, in practice, it is most desirable to perform only regeneration of the complete adsorption-degradation-adsorbent inside the fluidized bed. However, in view of the fact that, especially in large flow processes, partially desorbed or non-desorbed solid adsorbent may overflow with the high velocity gas stream. Therefore, in fact, the cyclone separator (22) of reference 2 is only for separating and recovering a part of the overflowing solid adsorbent, i.e., it only functions to avoid overflow and loss of the solid adsorbent in the high-speed gas stream treatment, but is not efficient in terms of recycling of the solid adsorbent, and regeneration of the solid adsorbent still requires a separate replacement operation, and therefore, there is still room for further improvement in terms of the efficiency of the overall recycling treatment.
Furthermore, more importantly, the inventor of the present invention also found in practice that reference 2 has a certain difficulty in controlling the overall reaction during the large-flow treatment process, and during the cyclic treatment process, not only a part of the desorbed solid adsorbent may overflow, but also a part of the desorbed solid adsorbent may overflow with the gas flow, and the desorbed solid adsorbent is separated by the cyclone separator (22) and then directly returned to the adsorption zone inside the fluidized bed through the return pipe. This situation actually causes an ineffective circulation of the solid adsorbent, and there are the following conditions: although the solid catalyst reduces the loss due to the overflow, there is no problem of increasing the cyclic utilization of the solid adsorbent.
In addition, in reference 2, the decomposed products of VOCs generated by plasma bombardment are also directly discharged in the form of small molecules, and there is practically no provision for the possibility of recovering and reusing some valuable organic or inorganic gases.
Therefore, in view of the technical problems in the prior art, the present invention is to provide an improved method and apparatus for treating waste gas, which can not only remove and purify industrial (flue) gas containing multiple pollutants, but also continuously and efficiently recycle materials, and can recover valuable chemical substances and realize resource utilization while removing and purifying, and also has the advantages of high heat and mass transfer efficiency and stable system operation.
Means for solving the problems
According to the intensive studies of the inventors, it was found that the above technical problems can be solved by the following embodiments:
[1] the present invention first provides a method for purifying a gas containing contaminants, comprising:
a step of adsorption to contact the pollutant-containing gas with an adsorbent in a fluidized bed reactor;
a separation step of introducing the adsorbent having adsorbed the contaminant into a gas-solid separation device to separate and recover the adsorbent having adsorbed the contaminant;
a regeneration step of subjecting the adsorbent having adsorbed the contaminant to a heating treatment to desorb the contaminant and obtain a regenerated adsorbent;
wherein, in the regenerating step, at least a portion of the regenerated sorbent is introduced (directed back) into the fluidized bed reactor and contaminants resulting from the desorption are introduced into at least one condenser for recovery.
[2] The method of [1], wherein the step of adsorbing, the adsorbent comprises porous particles.
[3] The method according to [1] or [2], wherein in the step of adsorbing, the gas containing the contaminant is subjected to dust removal treatment before entering the fluidized-bed reactor; the contaminants include one or more of sulfur-containing gases, nitrogen-containing gases, chlorine-containing gases, heavy metal-containing gases, and other VOCs gases.
[4] The method according to any one of [1] to [3], wherein in the step of separating, the adsorbent having adsorbed the contaminant is introduced into one or more gas-solid separation devices; the gas-solid separation device comprises a cyclone separator.
[5] The method according to any one of [1] to [4], wherein in the regenerating step, at least a part of the regenerated adsorbent is led out of the purification system.
[6] The method according to any one of [1] to [5], wherein in the regeneration step, the pollutant generated by desorption is introduced into at least two condensers connected in series to condense and recover at least part of the pollutant.
[7] Further, the present invention also provides a purification system for treating a gas containing contaminants, comprising:
a fluidized bed reactor having at least a gas feed port and a solids feed port;
the gas-solid separation device is connected with the fluidized bed reactor;
the regeneration reactor is connected with the gas-solid separation device;
at least one condenser connected to the regeneration reactor,
wherein the regeneration reactor has one or more regeneration reactor outlets, at least one of which allows for returning at least a portion of the regenerated solid matter to the sulfidation bed reactor.
[8] The system according to [7], further comprising a pre-dust collector to dust-remove the gas to be treated before it enters the fluidized-bed reactor.
[9] The system according to [7] or [8], wherein the gas feed port and the solid feed port are disposed at a lower portion or a bottom portion of the fluidized bed reactor; the fluidized bed reactor is connected with the gas-solid separation device through a discharge hole at the upper part or the top part.
[10] The system according to any one of [7] to [9], having one or more gas-solid separation devices, at least one of which is connected to the regeneration reactor.
[11] The system according to any one of [7] to [10], wherein the gas-solid reaction device comprises a cyclone separator; the upper part or the top of the gas-solid reaction device is provided with a purified gas exhaust port.
[12] The system according to any one of [7] to [11], wherein at least one of the regeneration reactor discharge ports of the regeneration reactor allows at least a part of the regenerated solid matter to be led out of the system.
[13] The system according to any one of [7] to [11], wherein two or more of the condensers are connected in series to the regeneration reactor.
ADVANTAGEOUS EFFECTS OF INVENTION
Through the implementation of the technical scheme, the invention can obtain the following technical effects:
the invention can provide a waste gas treatment method and a waste gas treatment system which are improved relative to the existing waste (smoke) gas treatment process containing harmful pollutants, not only can simultaneously remove and purify industrial (smoke) gas containing various pollutants, but also can continuously and efficiently utilize materials in a circulating way.
In addition, according to the treatment process disclosed by the invention, after harmful pollutants are removed and purified, valuable chemical substances can be recycled and resource utilization can be realized. Furthermore, the method and the device also have the advantages of high heat and mass transfer efficiency and stable system operation.
Drawings
FIG. 1: one specific schematic of the purification system of the present invention
Description of the reference numerals
1: a flue (exhaust) gas inlet; 2: a pre-deduster; 3: a gas inlet of the circulating fluidized bed reactor; 4: a wind distribution plate; 5: an adsorbent feeding port; 6: an ammonia spraying inlet; 7: a circulating fluidized bed reactor; 8: a cyclone separator; 9: a purified gas outlet; 10: a saturated porous media particle outlet; 11: a regeneration reactor; 12: a first-stage condenser; 13: a secondary condenser; 14: a first-stage condensation discharge port; 15: a secondary condensation discharge port; 16: a noncondensable gas outlet; 17: a discharge outlet; 18: and (6) returning the material port.
Detailed Description
The following describes embodiments of the present invention, but the present invention is not limited to these embodiments. The present invention is not limited to the configurations described below, and various modifications are possible within the scope of the claims, and embodiments and examples obtained by appropriately combining the technical means disclosed in the respective embodiments and examples are also included in the technical scope of the present invention. All documents described in this specification are incorporated herein by reference.
Unless defined otherwise, technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs.
The use of the terms "a" and "an" and "the" and similar referents in the context of describing the invention (especially in the context of the following claims) are to be construed to cover both the singular and the plural, unless otherwise indicated herein or clearly contradicted by context.
In the present specification, a numerical range represented by "a value to B value" or "a value to B value" means a range including the end point value A, B.
In this specification, the "upper portion", "lower portion", and "middle portion" are the results of description with respect to the relative position or space in which the object is described equally.
In the present specification, the meaning of "may" includes both the meaning of performing a certain process and the meaning of not performing a certain process. In this specification, "optional" or "optionally" means that the subsequently described event or circumstance may or may not occur, and that the description includes instances where the event occurs and instances where it does not.
Reference throughout this specification to "some particular/preferred embodiments," "other particular/preferred embodiments," "some particular/preferred aspects," "other particular/preferred aspects," or the like, means that a particular element (e.g., feature, structure, property, and/or characteristic) described in connection with the embodiment is included in at least one embodiment described herein, and may or may not be present in other embodiments. In addition, it is to be understood that the described elements may be combined in any suitable manner in the various embodiments.
The terms "comprises" and "comprising," and any variations thereof, in the description and claims of this invention and the above-described drawings are intended to cover non-exclusive inclusions. For example, a process, method, or system, article, or apparatus that comprises a list of steps or elements is not limited to only those steps or elements listed, but may alternatively include other steps or elements not listed, or inherent to such process, method, article, or apparatus.
< first aspect >
In a first aspect of the invention, a method for purifying a gas containing a plurality of harmful contaminants is provided.
In the method, one or more harmful pollutants are adsorbed on an adsorbent by using a fluidized bed reactor, and the adsorbent adsorbed with the harmful pollutants is led out of the fluidized bed reactor, and desorption and regeneration of the adsorbent are carried out. Further, at least a part of the regenerated adsorbent is returned to the fluidized bed for cyclic reaction, and at the same time, the chemical substances with utilization value desorbed from the adsorbent in the desorption process are enriched and recovered.
Harmful contaminants
The harmful contaminants of the present invention refer to substances having a negative influence on the environment, human body or specific production processes. These substances include solid contaminants as well as gaseous contaminants. In some specific embodiments of the present invention, the pollutants are mainly from waste gas and waste smoke discharged from industrial production, and the pollutants also include pollutants generated from human daily life without limitation.
The solid contaminants are not particularly limited, and may be one or more of dust, soot, particles, lumps, flakes, fibers, and flocs, or a mixture thereof. In some particular embodiments of the invention, the solid contaminants may be: one or more of metal or semimetal oxides, metal-containing solid complexes, metal salts, and the like; inorganic carbides, for example, solid carbides after combustion of organic substances, fossil fuels, and the like. In some specific embodiments of the present invention, the solid contaminants have a particle size of 10 μm or more, and the upper limit of the particle size of the solid contaminants is not particularly limited, and may be, for example, 100 μm to 1 cm.
The gaseous pollutants are also not particularly limited and may be one or more of sulfur-containing gases, nitrogen-containing gases, chlorine-containing gases, heavy metal-containing gases, and other gases of VOCs. For sulfur-containing gases, various oxides of sulfur, hydrogen sulfide, gaseous acids containing sulfur, and the like are mainly included, such as sulfur dioxide, sulfur trioxide, sulfuric acid vapor, and the like; for nitrogen-containing gases, predominantly NaObIn the form ofNitrogen-containing gases and ammonia, e.g., one or more of nitric oxide, nitrogen dioxide, nitrous oxide, and the like; by chlorine-containing gas, primarily gaseous hydrogen chloride is meant; as the heavy metal-containing gas, mercury vapor, sublimated or evaporated heavy metal-containing gas, and the like can be included; other VOCs may include: hydrocarbons (including alkanes, aromatics, olefins), halogenated hydrocarbons, esters, aldehydes, ketones, ethers, and acids, and in some embodiments, these other VOCs may be one or more of the benzene series, organic chlorides, freon series, and petroleum hydrocarbon compounds, among others.
Step of pretreatment
In the present invention, before the step of adsorption of contaminants by the fluidized bed reactor, various pretreatment steps may optionally be used.
In some preferred embodiments of the present invention, a pre-separation device is used in the pre-treatment step to separate solid contaminants from the gas containing a plurality of harmful contaminants, in view of improving the adsorption efficiency of the subsequent fluidized bed reactor and improving the stability of the operation of the purification system.
Such a preseparating device is not particularly limited, and various preseparators generally used in the art can be used. In some preferred embodiments of the present invention, the pre-dust collector may be used in combination with one or more selected from the group consisting of a cyclone separator, a bag-type dust collector, a screen dust collector, and an electrostatic adsorption dust collector.
For the pretreatment step, 70% or more of solid contaminants in the gas containing the plurality of harmful contaminants may be removed, preferably 80% or more, more preferably 90% or more, further preferably 95% or more, and most preferably 98% or more of solid contaminants may be removed. The pretreated gas is then introduced into the fluidized-bed reactor.
Step of adsorption
The present invention utilizes an adsorption step to contact the gas containing the plurality of hazardous contaminants with an adsorbent in a fluidized bed reactor. The contaminants herein are primarily meant to be gaseous contaminants and in some cases may also be permitted to contain small amounts of solid contaminants, preferably where the contaminants are substantially or essentially all gaseous contaminants.
The fluidized bed reactor of the invention is a circulating fluidized bed reactor. The adsorbent is brought into intimate mixing contact with the gas within the adsorbent so that the adsorbent is able to adsorb contaminants in the gas in a saturated state. The height and the internal average internal diameter of the fluidized bed reactor are not particularly limited, and can be designed according to the actual gas flow to be treated, and the residence time of the flue gas in the reactor is 1 to 10s, preferably 3 to 6s from the aspects of production and stability of system operation; the superficial gas flow rate is 1 to 5m/s, preferably 2 to 4.5 m/s.
As the adsorbent, there is no particular limitation, and a solid particulate adsorbent can be used. In some embodiments of the invention, the solid adsorbent particles may be selected from porous media particulate materials having adsorbent properties. Preferably, these porous materials include activated coke/carbon, modified activated coke/carbon, molecular sieves, modified molecular sieves, and oxides or hydroxides of alkali metals or alkaline earth metals (e.g., calcium oxide or calcium hydroxide having a porous structure), and the like. The solid particulate adsorbent of the present invention preferably has good abrasion resistance from the viewpoint of recycling, and from this viewpoint, the solid particles have a substantially spherical shape.
In some specific embodiments of the present invention, the average particle diameter (D) of the solid particulate adsorbent is50) The particle size of the adsorbent may be 100 to 600 μm, preferably 150 to 500 μm, from the viewpoint of improving the operation stability and adsorption efficiency of the purification system. If the average particle diameter of the solid particles is too small, undesirable agglomeration and clogging of the inside of the fluidized bed reactor may occur; if the average particle size of the solid particles is too large, there is a possibility that significant sedimentation occurs inside the fluidized bed and it is difficult to lead out of the fluidized bed reactor in the case of low-flow treatment, and the adsorption efficiency may be lowered due to the reduction in specific surface area.
Further, in some preferred embodiments of the present invention, the solid particulate adsorbent has a particle size of 10m2A specific surface area of not less than 15m, preferably2A surface area of not less than 20 m/g, more preferably2Specific surface area of/g or more. The upper limit of the specific surface area is not particularly limited, and may be, for example, 100m2A ratio of 80m or less per gram2A total of 50m or less in terms of/g2Specific surface area of/g or less. If the specific surface area is too small, there is a concern that the adsorption efficiency is affected, and if the specific surface area is too large, in addition to the increase in the use cost of raw materials, too high specific surface energy may cause agglomeration and adversely affect the adsorption efficiency, and at the same time, there is a concern that the adsorption of the present invention may cause clogging of piping and decrease of the smoothness of the operation of the system in the step of "separation" described later. In the present invention, the measurement of the specific surface area can be obtained based on the BET adsorption method.
Generally, the gas containing the hazardous contaminants (after being treated by the pretreatment step) may be introduced into the fluidized bed reactor through an inlet provided at the lower part or bottom of the fluidized bed reactor. The adsorbent may be introduced from a gas inlet (feed) provided at the lower part or bottom part of the fluidized bed reactor. In some preferred embodiments of the present invention, the gas feed port containing the hazardous contaminant is located at the bottom of the fluidized bed reactor, while the sorbent feed port is located at the lower portion of the fluidized bed reactor.
In addition, the gas containing the hazardous contaminants and the adsorbent may be alternately introduced into the fluidized bed reactor at arbitrary intervals or both simultaneously during operation of the overall purification system.
In some preferred embodiments of the present invention, the gas introduced from the gas inlet of the fluidized bed reactor has a flow rate and a pressure, and after such gas enters the fluidized bed reactor, the flow rate, the flow direction and the pressure of the gas can be adjusted by using the air distribution plate, so as to ensure uniformity of the flow rate, the pressure distribution and the like of the gas in the internal space of the fluidized bed reactor. The type of the air distribution plate is not particularly limited, and an air distribution plate of a type common in the art or commercially available may be used.
In the case of using the air distribution plate, the position of the adsorbent feeding port can be set in the range of 0.2-1m, preferably 0.3-0.5m above the air distribution plate, so that the solid granular adsorbent can better contact with the gas and adsorb the harmful pollutants therein.
In the case of using the grid, the fluidized-bed reactor may be divided into two sections, i.e., an air inlet zone below the grid and a mixing reaction zone above the grid, with the grid as a boundary. In some preferred embodiments, the average diameter of the interior of the mixing reaction zone is greater than the average diameter of the interior of the air intake zone.
The gas containing the hazardous contaminant is mixed with the solid particulate adsorbent at a gas flow rate and the temperature at which mixing occurs may, in some embodiments of the invention, be no more than 200 c, preferably 160 c or less. In addition, for the purpose of promoting mixing and adsorption, a mechanical auxiliary unit, such as a stirring unit or the like, may be disposed in the region where the solid particulate adsorbent is in mixing contact with the gas to promote contact between the gas and the solid.
In addition, without limitation, for the fluidized bed reactor of the present invention, besides the above-mentioned harmful pollutant-containing gas inlet and adsorbent inlet, other material inlets may be added as required, for example, these inlets may be reducing gas inlets. In some specific embodiments of the present invention, especially considering when nitrogen oxides are contained in a gas containing harmful pollutants, ammonia gas may be additionally supplied to the fluidized bed reactor to reduce the nitrogen oxides to nitrogen and water, typically, for example:
NOx+NH3→N2+H2O
the feed port for these other substances is not particularly limited and may be provided in the fluidized bed reactor as desired, in some specific embodiments such feed port is provided in the middle or upper portion of the fluidized bed reactor, and in other embodiments such feed port is provided at a position higher than the sorbent feed port.
Through the arrangement or the mode, under certain physical and chemical reaction conditions, the adsorbent is subjected to saturated adsorption on harmful pollutants, and is led out from an outlet arranged at the upper part or the top of the fluidized bed reactor and further led into a subsequent gas-solid separation device.
In addition, in order to improve the operation stability of the entire purification system, the pressure of the gas at the outlet disposed at the upper portion or the top of the fluidized bed reactor may be made lower than the pressure at the gas inlet disposed at the lower portion or the bottom of the fluidized bed.
Step of separation
In the present invention, the adsorbent having adsorbed the harmful contaminant is separated by a gas-solid separation device, and in some preferred embodiments, some of the purified gas or harmless gas, such as a part of oxygen, nitrogen, etc., is also discharged out of the purification system. For such a vent, it is advantageously arranged at the top of the gas-solid separation device.
In some preferred embodiments of the present invention, a cyclone is used as the gas-solid separation means in view of improving the gas-solid separation efficiency. In some particular embodiments of the invention, one or more gas-solid separation devices may be used, wherein at least one gas-solid separation device is the cyclone. In some preferred embodiments, these cyclones can be operated simultaneously in parallel to efficiently separate the solid adsorbent.
The number of revolutions and the treatment time of the cyclone are not particularly limited, and may be adjusted as needed or according to the specific operation state of the apparatus.
With respect to the cyclone, in some embodiments of the present invention, the classification of the solid particulate adsorbent may also be achieved by adjusting the number of revolutions, and when a plurality of cyclones are used, the cyclones may also be adjusted to different numbers of revolutions in series to classify the adsorbent particles, and the adsorbents having average particle sizes suitable or not suitable for recycling may be separately collected and separately introduced into different regeneration reactors in the regeneration step.
Step of regeneration
In the regeneration step of the present invention, the adsorbent having adsorbed the contaminant is subjected to a heating treatment to desorb the contaminant and obtain a regenerated adsorbent. It should be noted that "desorption" in the present invention includes not only physical desorption but also possible desorption of chemical reaction products from the adsorbent due to the catalytic properties of the adsorbent.
In the present invention, the regeneration treatment of the adsorbent having adsorbed the contaminants is performed using a regeneration reactor connected to the gas-solid separation device. The treatment conditions for the regeneration treatment may be carried out by heating in some specific embodiments of the present invention, and the heating method is not particularly limited, and may be carried out by a direct heat transfer method or a microwave heating method. Further, the temperature for the heat treatment may be generally 350-450 ℃. The regeneration treatment time is not particularly limited, and may be adjusted depending on the type of the adsorbent, the kind of the harmful substance to be adsorbed, and the heating temperature.
In other specific embodiments of the present invention, a mechanical stirring unit or a mechanical vibration unit may be further included in the regeneration reactor to perform contaminant desorption on the adsorbent under a dynamic state, thereby improving desorption efficiency.
In the present invention, the regeneration reactor used in the regeneration step may have one or more, and when there are a plurality of regeneration reactors, at least one regeneration reactor has a return port to allow at least a part of the regenerated solid matter (adsorbent) to be led back to the inside of the fluidized bed reactor; in addition, there is also at least one regeneration reactor with a discharge opening to allow at least a part of the regenerated solid matter (sorbent) to be conducted out of the purification system, which normally is not suitable for recycling again. In some embodiments of the invention, the flow rate and/or amount of solids introduced back into the fluidized bed reactor and out of the purification system can be controlled to ensure smooth operation of the purification system.
Step of condensing and recovering
In the invention, when the adsorbent is subjected to regeneration treatment, various pollutants adsorbed by the adsorbent are desorbed from the surface of the adsorbent under the heating condition, and the desorbed gas is introduced into at least one condenser and is recovered and enriched through condensation, so that the resource utilization of the available pollutants is realized.
Such a condenser is not particularly limited, and a condensing device generally used in the art, such as a condensing tube, a condensing tower, or a condensing tray, may be used. In some preferred embodiments of the invention, a plurality of identical or different condensers may be used, which may be used in series. And, control different condensing temperature in these condensers, can carry out (gradient) condensation recovery to different harmful pollutant. Preferably, at least two such condensers may be used in series.
After the condensation recovery process, the gases that cannot be condensed are discharged from the purification system and can continue to be subjected to further processing by other available devices as desired.
Circulating operation
Through the explanation of the steps, the invention can realize continuous treatment of the gas containing harmful pollutants, especially the industrial waste flue gas, can circularly utilize the solid adsorbent to carry out purification treatment, and can enrich and recycle at least a part of the available pollutants.
In addition, in some preferred embodiments of the present invention, in addition to recycling, the solid adsorbent may be supplemented with new solid adsorbent (catalyst) as the reaction proceeds, so as to achieve smooth operation of the purification system and ensure purification effect.
In addition, in some embodiments of the present invention, if the temperature of the to-be-treated gas containing the harmful material, which is introduced into the fluidized-bed reactor, is excessively high, such gas may be arranged to exchange heat with the regeneration reactor to effectively utilize the heat of the to-be-treated gas.
< second aspect >
In a second aspect of the invention, the invention also provides a purification system for a gas containing contaminants, comprising: a fluidized bed reactor having at least a gas feed port and a solids feed port; the gas-solid separation device is connected with the fluidized bed reactor; the regeneration reactor is connected with the gas-solid separation device; at least one condenser connected to the regeneration reactor. Wherein the regeneration reactor has one or more regeneration reactor outlets, at least one of the regeneration reactor outlets to allow at least a portion of the regenerated solid matter to be returned to the sulfidation bed reactor.
A specific embodiment of the present invention will be further described with reference to the accompanying drawings.
As shown in fig. 1, the industrial smoke (waste gas) to be purified passes through the pre-dust collector 2 and then enters the circulating fluidized bed reactor 7, the gas passes through the air distribution plate 4 to realize the flow equalization effect, and forms gas-solid fluidization with the porous medium particles (solid adsorbent particles) above the air distribution plate 4. SO in industrial flue gas (waste gas) during fluidized state motion2、NOxAnd pollutants such as VOCs, heavy metals, hydrogen halide and the like are adsorbed by the porous medium particles. The porous medium particle adsorption is prepared from substances with adsorption property such as active coke/carbon, molecular sieve, active coke/carbon or molecular sieve modified material, and has particle diameter (D)50) 100 to 600 μm.
An ammonia spraying inlet 6 is arranged on the side surface of a sparse phase region of the circulating fluidized bed reactor 7, and NO is catalyzed by porous medium particlesxAnd NH3Form N2And H2And O, realizing the denitration process. SO (SO)2With H in industrial flue gas (waste gas)2O、O2Adsorption occurs on the porous media particles. VOCs, partial heavy metals, hydrogen halide and ammonia in industrial smoke (waste gas)After the porous medium particles with adsorption capacity are fully contacted, the porous medium particles are adsorbed and purified.
The adsorbed saturated porous medium particles and the purified gas are introduced into a cyclone separator 8 to realize gas-solid separation, the purified industrial smoke (waste gas) is discharged through a purified gas outlet 9, and the saturated porous medium particles enter a regeneration reactor 11 from a saturated porous medium particle outlet 10 of the cyclone separator 8.
In the regeneration reactor 11, the adsorbed pollutants or (chemical) reaction byproducts are desorbed from the saturated porous medium particles under the heating condition, so that the regeneration of the porous medium particles is realized.
Part of the regenerated porous medium particles enter the circulating fluidized bed reactor 7 again through the material returning port 18 to participate in the circulating purification of the industrial smoke (waste gas); and the other part, is collected from the discharge opening 18. Meanwhile, the adsorbent feeding port 5 of the circulating fluidized bed reactor 7 also maintains a certain feeding rate, so as to ensure the balance of materials in the circulating fluidized bed reactor 7 and the balance of pollutant purification capacity.
The desorbed pollutants or reaction byproducts enter the primary condenser 12, and part of substances with higher condensation points are condensed into liquid state and then enter a primary condensation outlet; the residual gaseous mixture enters a secondary condenser 13, and substances with lower condensation points are condensed and then discharged from a secondary condensation outlet 15; the remaining non-condensable gases are removed from the non-condensable gas outlet 16. After the gas and liquid pollutants or reaction byproducts exhausted at different stages are enriched, the gas and liquid pollutants or reaction byproducts can be further purified in a proper mode, so that the recycling is realized.
Besides, the purification system of the present invention may further include various conventional auxiliary devices or auxiliary units, in addition to the above-described parts, devices or apparatuses, according to actual needs. These additional devices or units include, but are not limited to:
a power/electricity supply unit;
a heating unit;
a control unit comprising a mechanical control unit and/or an electronic control unit;
a detection or detection unit;
a display unit;
an alarm unit;
further, the purification system of the present invention is not limited and can be used with other gas purification systems known in the art.
Examples
Hereinafter, the present invention will be described by way of specific examples.
Example 1
The smoke quantity of a coal-fired boiler of a certain 300MW power station is about 1200000m3H, the flue gas temperature is 120 ℃. The concentrations of sulfur dioxide, nitrogen oxide and Hg in the flue gas are respectively 2000mg/Nm3,400mg/Nm3,50μg/Nm3. Porous medium particles with the particle size of 0.5mm are prepared by adopting activated carbon with adsorption and catalysis functions and are used as circulating materials, and the total circulating amount is 500 tons.
The specific process is as follows:
the flue gas discharged from the tail part of the boiler firstly enters a pre-dust remover 2, the flue gas after pre-dust removal enters a circulating fluidized bed reactor 7 through an air distribution plate 4, and porous medium particles are added from an adsorbent feeding port 5 of the circulating fluidized bed reactor 7. The flue gas and the porous medium particles form gas-solid fluidization motion in the circulating fluidized bed reactor 7.
SO is essentially completed in a dense phase zone in the circulating fluidized bed reactor 72To produce SO in an adsorbed state3. At the same time, ammonia, NH is sprayed in the sparse phase region of the circulating fluidized bed reactor 73/NOxThe molar ratio can be adjusted within a dynamic range of 1.05 to 1.2. Under the catalytic action of the porous medium particles, NOxAnd NH3Form N2And H2And O, realizing the denitration process.
In addition, in the whole fluidization movement process, the adsorption and removal process of Hg in the flue gas can be realized. Adsorbing Hg and SO3The porous medium particles are subjected to gas-solid separation through the cyclone separator 8 and enter the regeneration reactor 11.
Heating at 350-450 ℃ by adopting a microwave heating regeneration method to desorb the adsorption Hg on the surface of the porous medium particles into gaseous Hg; SO in adsorbed state3Reduction of porous medium particles to SO under the catalytic action of the porous medium particles2. The regeneration of the porous medium particles is realized by a microwave heating regeneration method, one part of regenerated porous medium particles are discharged from a discharge port 17, and the other part of regenerated porous medium particles enter the circulating fluidized bed reactor 7 for cyclic utilization.
The desorbed gaseous mixture enters the primary condenser 12, the condenser temperature is controlled below the condensation point of the mercury vapor, and the liquid mercury is removed through the primary condenser outlet 14. The sulfur dioxide is discharged from the non-condensable gas outlet 16 and collected. For the present embodiment, the secondary condenser 13 is not provided.
Example 2
500m for a certain iron and steel enterprise2The discharge amount of flue gas of the sintering machine after adopting a certain flue gas circulation process is 660000m3The temperature of the flue gas is about 200 ℃; the concentrations of sulfur dioxide, nitrogen oxide and dioxin in the flue gas are respectively 900mg/Nm3,350mg/Nm3,1ng/Nm3. Porous medium particles with the particle size of 0.5mm are prepared by adopting activated carbon with adsorption and catalysis functions and are used as circulating materials, and the total circulating amount is 220 tons.
The specific process is as follows:
the discharged flue gas firstly enters a pre-dust remover 2, the flue gas after pre-dust removal enters a circulating fluidized bed reactor 7 through an air distribution plate 4, and porous medium particles are added from an adsorbent feeding port 5 of the circulating fluidized bed reactor 7. The smoke and the porous medium particles adsorb and purify pollutants in the fluidized movement process.
In flue gas H2O and O2Under the reaction conditions, SO2Chemical adsorption is carried out to form adsorption state SO3. In the presence of ammonia, NOxAnd NH3Form N2And H2And O, realizing the denitration process. Meanwhile, dioxin in the flue gas is adsorbed by the porous medium particles.
The porous medium particles with saturated adsorption enter the regeneration reactor 11 after gas-solid separation: under the temperature range of 200-250 ℃, the decomposition of dioxin is realized under the temperature of 350-450 ℃ by a microwave heating mode; simultaneous adsorption of SO3In porous media particlesIs reduced to SO under the catalysis of2. Part of the regenerated porous medium particles (which can be dynamically adjusted) enter the circulating fluidized bed reactor 7 again for flue gas purification, and the SO desorbed2And realizing resource utilization after enrichment.
Example 3
In an electronic component manufacturing enterprise, waste gas including NO generated in the processing of electronic components2NO, nitric acid, sulfuric acid, acetic acid, hydrogen chloride, dust and other pollutants with concentrations of 400mg/Nm3，50mg/Nm3，50mg/Nm3，10mg/Nm3，200mg/Nm3，10mg/Nm3And 80mg/Nm3The smoke discharge temperature is 25 ℃, and the smoke discharge flow is 50000m3H is used as the reference value. Porous medium particles with the particle size of 0.5mm are prepared by adopting a molecular sieve with an adsorption function and used as a circulating material, and the total circulating amount is 18 tons.
The specific process is as follows:
the generated waste gas enters a circulating fluidized bed reactor 7 through an air distribution plate 4 after being subjected to pre-dedusting, and porous medium particles are added from an adsorbent feeding port 5 of the circulating fluidized bed reactor 7. In the circulating fluidized bed reactor 7, the adsorption and removal of pollutants are realized in the gas-solid fluidized movement process of the exhaust gas and the porous medium particles. The pollutant components in the waste gas, including nitrogen oxides, sulfuric acid, acetic acid, hydrogen chloride and other acidic gases, are adsorbed together. And (3) allowing the porous medium particles with saturated adsorption to enter a regeneration reactor, and desorbing various pollutants adsorbed by the porous medium particles at the temperature of 350-450 ℃.
Regenerated porous medium particles enter the circulating fluidized bed reactor 7 through the material returning port 18 for recycling; the desorbed gaseous pollutants sequentially pass through a first-stage condenser 12 and a second-stage condenser 13, and are gradually enriched and recovered according to the difference of acid dew points of different acid gases.
It should be noted that, although the technical solutions of the present invention are described by specific examples, those skilled in the art can understand that the present disclosure should not be limited thereto.
Having described embodiments of the present disclosure, the foregoing description is intended to be exemplary, not exhaustive, and not limited to the disclosed embodiments. Many modifications and variations will be apparent to those of ordinary skill in the art without departing from the scope and spirit of the described embodiments. The terminology used herein is chosen in order to best explain the principles of the embodiments, the practical application, or improvements made to the technology in the marketplace, or to enable others of ordinary skill in the art to understand the embodiments disclosed herein.
Industrial applicability
The purification method and the purification system can be industrially used for purifying waste flue gas.
Claims (13)
1. A method for purifying a gas containing contaminants, comprising:
a step of adsorption to contact the pollutant-containing gas with an adsorbent in a fluidized bed reactor;
a separation step of introducing the adsorbent having adsorbed the contaminant into a gas-solid separation device to separate and recover the adsorbent having adsorbed the contaminant;
a regeneration step of subjecting the adsorbent having adsorbed the contaminant to a heating treatment to desorb the contaminant and obtain a regenerated adsorbent;
wherein, in the regenerating step, at least a portion of the regenerated sorbent is introduced into the fluidized bed reactor and contaminants resulting from the desorption are introduced into at least one condenser for recovery.
2. The method of claim 1, wherein in the step of adsorbing, the adsorbent comprises porous particles.
3. The method according to claim 1 or 2, wherein in the step of adsorbing, the gas containing contaminants is dedusted before entering the fluidized bed reactor; the contaminants include one or more of sulfur-containing gases, nitrogen-containing gases, chlorine-containing gases, heavy metal-containing gases, and other VOCs gases.
4. A process according to any one of claims 1 to 3, wherein in the separation step the adsorbent having adsorbed the contaminants is introduced into one or more gas-solid separation devices; the gas-solid separation device comprises a cyclone separator.
5. The method of any of claims 1 to 4, wherein in the regenerating step, at least a portion of the regenerated sorbent is directed out of the purification system.
6. The method according to any one of claims 1 to 5, wherein in the regeneration step, the pollutants generated by desorption are introduced into at least two condensers connected in series to condense and recover at least part of the pollutants.
7. A purification system for treating a gas containing contaminants, comprising:
a fluidized bed reactor having at least a gas feed port and a solids feed port;
the gas-solid separation device is connected with the fluidized bed reactor;
the regeneration reactor is connected with the gas-solid separation device;
at least one condenser connected to the regeneration reactor,
wherein the regeneration reactor has one or more regeneration reactor outlets, at least one of which allows for returning at least a portion of the regenerated solid matter to the sulfidation bed reactor.
8. The system of claim 7, further comprising a pre-precipitator to remove dust from the gas to be treated prior to its entry into the fluidized bed reactor.
9. The system of claim 7 or 8, wherein the gas feed and solids feed are located at a lower portion or bottom of the fluidized bed reactor; the fluidized bed reactor is connected with the gas-solid separation device through a discharge hole at the upper part or the top part.
10. The system according to any one of claims 7 to 9, wherein the system comprises one or more gas-solid separation devices, at least one of which is connected to the regeneration reactor.
11. The system according to any one of claims 7 to 10, wherein the gas-solid reaction device comprises a cyclone separator; the upper part or the top of the gas-solid reaction device is provided with a purified gas exhaust port.
12. The system of any one of claims 7 to 11, wherein at least one of the regeneration reactor outlets of the regeneration reactor allows for at least a portion of the regenerated solid matter to be directed out of the system.
13. The system according to any one of claims 7 to 11, wherein two or more of the condensers are connected in series with the regeneration reactor.
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