CN115463518A - Device and method for purifying and recycling nitrogen oxides in tail gas of mobile source - Google Patents
Device and method for purifying and recycling nitrogen oxides in tail gas of mobile source Download PDFInfo
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- CN115463518A CN115463518A CN202210965117.8A CN202210965117A CN115463518A CN 115463518 A CN115463518 A CN 115463518A CN 202210965117 A CN202210965117 A CN 202210965117A CN 115463518 A CN115463518 A CN 115463518A
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- B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
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Abstract
The invention relates to a device and a method for realizing purification and recovery of nitrogen oxides in tail gas of a mobile source, belonging to the technical field of purification of atmospheric pollution and comprising the following steps: tail gas system, ozone or low temperature plasma generation supply system, absorption liquid system, control system and absorption product concentration recovery system. The invention firstly utilizes ozone or low-temperature plasma to oxidize nitrogen oxides (including nitric oxide and nitrogen dioxide) in tail gas generated by road vehicles or non-road mobile source equipment into high-valence nitrogen oxides. Then, the alkaline absorption liquid is used for absorbing the high-valence nitrogen oxides to form an absorption product containing high-concentration nitrate. And finally, separating and absorbing the product by using a high-efficiency cyclone separator to realize the high-efficiency purification of the nitrogen oxide in the tail gas. Meanwhile, tail gas is used for heating the absorption product, so that the temperature of the tail gas is reduced, and the absorption product is concentrated. The invention does not relate to the volatile ammonia component medicament such as gaseous ammonia, ammonium water or urea aqueous solution, and has no safety risk.
Description
Technical Field
The invention relates to the technical field of air pollution purification, in particular to a device and a method for purifying and recovering nitrogen oxides in tail gas of a mobile source.
Background
Mobile source equipment fueled by oil or gas includes road vehicles and non-road mobile sources. Non-road moving sources include engineering machinery, agricultural machinery, railway internal combustion engines, ships, airplanes, trains and the like. The mobile source may emit a gas containing nitrogen oxides (NOx, including NO and NO) 2 ) And the like and has high temperature. Nitric oxide entering the environment can directly harm human health, for example, the binding capacity of nitric oxide and hemoglobin in blood is far higher than that of carbon monoxide, so that people feel anoxic, damage central nerves and even die. Nitrogen dioxide can cause harm to human body vital organs such as heart, liver, kidney and the like. Meanwhile, nitrogen oxides are also important precursor substances causing photochemical smog, haze and acid rain. Therefore, the method has great significance in purifying the nitrogen oxides in the tail gas of the mobile source.
In the existing mainstream technology, ammonia or urea aqueous solution is used as a reducing agent to reduce nitric oxide into nitrogen, so that the tail gas purification system is complex and hidden danger of ammonia escape exists, and the nitric oxide recycling is not considered, so that the invention provides a device and a method for realizing the purification and recycling of the nitric oxide in the tail gas of a mobile source.
Disclosure of Invention
The invention aims to provide a device and a method for purifying and recovering nitrogen oxides in tail gas of a mobile source.
In view of the above, the first aspect of the present invention is to provide an apparatus for purifying and recovering nitrogen oxides in exhaust gas of a mobile source.
The second aspect of the invention provides a method for realizing purification and recovery of nitrogen oxides in tail gas of a mobile source.
The invention provides a device for purifying and recovering nitrogen oxides in tail gas of a mobile source, which consists of a tail gas purification system, an ozone or low-temperature plasma generation and supply system, an absorption liquid circulating system, an absorption product concentration and recovery system and a control system embedded in a mobile source control mechanism, wherein the tail gas purification system is arranged on a chassis of a road motor vehicle or non-road mobile source equipment; the inlet of the tail gas purification system is connected with the tail gas outlet of an engine of a road motor vehicle or a non-road mobile source device, and the ozone or low-temperature plasma generation and supply system, the absorption liquid circulating system and the absorption product concentration and recovery system are connected with the tail gas purification system.
Further, the exhaust gas purification system includes: the device comprises a catalytic oxidation converter, an evaporation concentrator, a mixer, an oxidation reaction pipe, a Venturi tube, an absorption reactor and a high-efficiency cyclone separator which are connected in sequence; the air inlet of the catalytic oxidation converter is connected with an engine tail gas outlet of a road motor vehicle or a non-road mobile source device and is used for oxidizing part or all of nitric oxide in the tail gas into nitrogen dioxide and oxidizing carbon monoxide and hydrocarbon in the tail gas into carbon dioxide and water;
the inlet of the evaporation concentrator is connected with the gas outlet of the catalytic oxidation converter, the evaporation concentrator also comprises an absorption product inlet and an absorption product outlet, the absorption product inlet is connected with the outlet of an absorption product conveying pump of the absorption product concentration and recovery system, the evaporation concentrator forms a heat exchange system, high-temperature tail gas entering from the catalytic oxidation converter is used for heating and evaporating part of moisture of the absorption product conveyed by the absorption product conveying pump, and the temperature of the tail gas is reduced; an outlet of an absorption product of the evaporation concentrator is connected with inlets of a nitrate concentrated solution and a crystal temporary storage tank of the absorption product concentration recovery system, the concentrated nitrate solution obtained by concentration automatically flows into the temporary storage tank, and steam generated by evaporation is automatically discharged to the atmosphere; the mixer is connected with the ozone or low-temperature plasma generation and supply system, so that the cooled tail gas is fully mixed with the ozone or low-temperature plasma provided by the ozone or low-temperature plasma generation and supply system; the oxidation reaction tube oxidizes nitrogen monoxide and nitrogen dioxide in the tail gas into high-valence nitrogen oxides, and the high-valence nitrogen oxides comprise dinitrogen pentoxide (N) 2 O 5 ) Nitrogen trioxide (NO) 3 ) And other higher nitrogen oxides; the Venturi tube is used for promoting the tail gas and the absorption liquid from the absorption liquid circulating systemThe absorption liquid fog drops are fully mixed and contacted; the absorption reactor is used for further mixing absorption liquid fog drops from the absorption liquid circulating system with tail gas and reacting to form a nitrate water solution; the high-efficiency cyclone separator is used for separating nitrate-containing fog drops in purified gas discharged from the absorption reactor.
Further, the exhaust gas purification system further includes: the fine particle catcher is arranged behind the high-efficiency cyclone separator and connected with the air outlet of the high-efficiency cyclone separator, is used for catching the particles with extremely small particle size and extremely low content remained after the treatment of the high-efficiency cyclone separator, and is only equipped in places with extremely high requirements on particle emission control, and does not need to be equipped in other places.
Further, the ozone or low-temperature plasma generation supply system includes: a vehicle-mounted power supply, an ozone or low-temperature plasma generator and an ozone or low-temperature plasma nozzle; the vehicle-mounted power supply is used for supplying power to the ozone or low-temperature plasma generator, the ozone or low-temperature plasma generator takes air as a gas source and converts part of gas in the ozone or low-temperature plasma generator into ozone or low-temperature plasma, and the ozone or low-temperature plasma nozzle is used for spraying the air containing the ozone or low-temperature plasma into the mixer.
Further, the absorption liquid circulation system includes: the absorption agent box, the absorption liquid circulating pump, the absorption liquid nozzle and the jet hole; the absorbent box is used for storing fresh alkaline aqueous solution, and a liquid outlet of the absorbent box is connected with a liquid inlet of the absorbent box through an electromagnetic valve; the other liquid inlet of the absorption liquid box is connected with the liquid outlet of the high-efficiency cyclone separator and the liquid outlet at the bottom of the absorption reactor, and the absorption liquid box is used for temporarily storing fresh alkaline aqueous solution and absorption liquid flowing out of the absorption reactor and the high-efficiency cyclone separator; the liquid outlet of the absorption liquid box is connected with an absorption liquid nozzle and an injection hole through an absorption liquid circulating pump, the absorption liquid nozzle is positioned at the contraction section of the Venturi tube, the absorption liquid injection hole is positioned on the central tube wall of the absorption reactor, and the absorption liquid nozzle and the injection hole are used for atomizing the circulating absorption liquid.
Further, the fresh aqueous alkaline solution includes, but is not limited to, at least one of the following: an aqueous solution of sodium hydroxide, sodium carbonate, sodium bicarbonate, potassium hydroxide, potassium carbonate, potassium bicarbonate, calcium oxide, or magnesium oxide; the absorption liquid in the absorption liquid tank is a solution formed by a fresh alkaline aqueous solution and an aqueous solution containing nitrate formed in the absorption process; the nitrates include, but are not limited to, at least one of the following: sodium nitrate, potassium nitrate, calcium nitrate and magnesium nitrate, the cations of which are the same as the metal cations contained in the alkaline absorbent solution.
Further, the absorption product concentration recovery system includes: an absorption product delivery pump and a nitrate concentrated solution and crystal temporary storage tank; a liquid inlet of the absorption product conveying pump is connected with a liquid outlet of the high-efficiency cyclone separator, and a liquid outlet of the absorption product conveying pump is connected with the evaporation concentrator and used for conveying high-concentration nitrate solution, namely the absorption product to the evaporation concentrator; the evaporation concentrator is a heat exchange system, partial water of the evaporation absorption product is heated by high-temperature tail gas to be concentrated, the concentrated nitrate solution obtained by concentration automatically flows into a nitrate concentrated solution and a crystal temporary storage tank, and the nitrate concentrated solution and the crystal temporary storage tank are connected with the evaporation concentrator and are used for storing the concentrated absorption solution flowing out of the evaporation concentrator and the nitrate crystal precipitated by natural cooling.
Further, the nitrate concentrated solution and crystal temporary storage tank is used for storing the absorption product from the evaporation concentrator and the crystal formed by natural cooling, and after the temporary storage tank is taken down by an after-sale service mechanism of a gas station or a mobile source, the nitrate concentrated solution and crystal temporary storage tank can be sent to a professional mechanism to be converted into a nitrate product.
Further, the control system includes: the device comprises a signal sensor, a control unit and an execution device; the sensors comprise a temperature sensor for sensing the temperature of the oxidation reaction tube, a pH value sensor for sensing the pH value of the absorption liquid, an ozone sensor for sensing the concentration of the ozone and the nitrogen oxide in the clean tail gas and a nitrogen oxide concentration sensor; the control unit is used for receiving signals measured by the sensor, signals of atmospheric temperature and air quantity entering the engine, performing data processing so as to determine the power supply voltage of the ozone or low-temperature plasma generator, the flow of the absorption liquid circulating pump, the parameter value of the flow of the absorption product conveying pump and the start-stop state of the absorbent feeding electromagnetic valve, and then sending commands for regulating and controlling the power supply voltage of the ozone or low-temperature plasma generator, the flow of the absorption liquid circulating pump, the flow of the absorption product conveying pump and the start-stop state of the absorbent feeding electromagnetic valve; the execution equipment comprises an ozone or low-temperature plasma generator for executing regulation and control commands, an absorption liquid circulating pump, an absorption product conveying pump and an absorbent feeding electromagnetic valve.
The invention provides a method for purifying and recovering nitrogen oxides in tail gas of a mobile source, which comprises the following steps of after the tail gas is discharged from a tail gas outlet of an engine of the mobile source: 1) In the catalytic oxidation converter, carbon monoxide and hydrocarbons in the tail gas are oxidized into carbon dioxide and water, and simultaneously, part or all of the nitrogen monoxide is oxidized into nitrogen dioxide; 2) In an evaporation concentrator, tail gas and an absorption product conveyed by an absorption product conveying pump are in indirect contact heat exchange, so that the temperature of the tail gas is reduced to below 150 ℃; 3) In the mixer, the tail gas is uniformly mixed with the additional ozone or low-temperature plasma; 4) In the oxidation reaction tube, the nitrogen monoxide and the nitrogen dioxide in the tail gas are oxidized into nitrogen pentoxide, nitrogen trioxide and other high-valence nitrogen oxides by the additional ozone or low-temperature plasma; 5) In the Venturi tube, the oxidized tail gas is fully contacted with an additional absorption liquid; 6) In the absorption reactor, the high-valence nitrogen oxides are absorbed by an alkaline aqueous solution to form a nitrate aqueous solution; 7) In the high-efficiency cyclone separator, fog drops in the tail gas are separated from the gas; 8) In an alternative fine particle catcher, fine particles with the particle size of less than 1 mu m are separated, the equipment is only arranged at a place with extremely high requirements on particle emission control, and the equipment is not required to be arranged at other places; 9) The absorption reactor and the high-efficiency cyclone separator collect most of absorption liquid and return to the absorption liquid box, and a small part of absorption liquid is conveyed to the evaporation concentrator by the absorption product conveying pump to evaporate water and concentrate the absorption liquid; 10 In the temporary storage tank for nitrate solution and crystal, the nitrate solution is cooled to reduce the solubility and gradually crystallized and separated out; 11 Nitrate mainly in a crystalline state in the temporary storage tank can be recovered by gas stations and automobile maintenance enterprises and sent to specialized institutions for resource utilization.
Compared with the prior art, the invention can realize at least one of the following beneficial effects:
1) Realize the high-efficient purification of the tail gas nitrogen oxides of fuel and gas mobile sources
The method firstly utilizes ozone or low-temperature plasma to oxidize the nitrogen oxides (including nitric oxide and nitrogen dioxide) in the tail gas of the mobile source which is or is not subjected to catalytic oxidation treatment into high-valence nitrogen oxides. Then, the alkaline absorption liquid is used for absorbing the high-valence nitrogen oxides with good water solubility to form nitrate aqueous solution, namely an absorption product. And finally, separating the nitrate aqueous solution by using a high-efficiency cyclone separator, realizing high-efficiency purification of tail gas nitrogen oxides, and recovering the absorption liquid.
2) Can prevent secondary pollution caused by ozone leakage
To achieve the goal of efficient oxidation of nitrogen oxides to higher nitrogen oxides, it is generally necessary to add a slight excess of ozone. Ozone has the characteristics of good water solubility and reaction activity, and by utilizing the characteristics, slightly excessive ozone can be dissolved into the absorption liquid and reacts with the reducing components of the absorption liquid to consume the ozone, so that the leakage of the ozone and the secondary pollution are prevented.
Compared with the traditional tail gas nitrogen oxide treatment technology, the method also has the following advantages:
1) The effective utilization of the waste heat of the tail gas is realized, and the energy required by the recovery and utilization of nitrate is saved
According to the invention, an external heat source is not needed, the absorption product is evaporated by using the waste heat of the tail gas, the evaporation and concentration of the absorption liquid are realized, the nitrate concentrated solution is obtained, and the nitrate crystal can be separated out by naturally cooling the nitrate concentrated solution, so that the nitrate crystal is convenient to recycle.
2) Nitrate capable of being obtained by purifying nitrogen oxide in recycling mode
The prior art is limited to reducing nitrogen oxides into nitrogen, and does not consider the problems of nitrogen oxide recovery and resource utilization. The method fully utilizes the advantages of simple components of the tail gas of the mobile source and low impurity content of the obtained nitrate, and is convenient for realizing resource utilization of the nitrate obtained by purifying the nitric oxide.
3) No safety risk and secondary pollution
The invention does not relate to agents with volatile ammonia components such as gaseous ammonia, aqueous ammonium or urea solutions, and therefore there is no safety risk. Meanwhile, the hidden trouble of excessive ammonia escape does not exist. Although slightly excessive ozone needs to be added, the ozone can be ensured to be efficiently dissolved into the absorption liquid and react with the absorption liquid by utilizing the good water solubility and the reaction activity of the ozone, so that the problem of secondary pollution caused by ozone leakage can be avoided.
Drawings
The drawings are only for purposes of illustrating particular embodiments and are not to be construed as limiting the invention.
FIG. 1 is a schematic structural diagram of the present invention.
Wherein, the corresponding relation between the reference numbers and the part names in fig. 1 is:
1-catalytic oxidation converter, 2-evaporative concentrator, 3-mixer, 4-oxidation reaction tube, 5-venturi tube, 6-absorption reactor, 7-high efficiency cyclone separator, 8-fine particulate trap, 9-vehicle power supply, 10-ozone or low-temperature plasma generator, 11-ozone or low-temperature plasma nozzle, 12-absorbent box, 13-absorption liquid box, 14-absorption liquid circulating pump, 15-absorption liquid nozzle spray hole, 16-temperature sensor, 17-pH value sensor, 18-nitrogen oxide concentration sensor, 19-ozone sensor, 20-control unit, 21-absorption product delivery pump, 22-nitrate concentrated liquid and crystal temporary storage tank.
Detailed Description
The preferred embodiments of the present invention will now be described in detail with reference to the accompanying drawings, which form a part hereof, and which together with the embodiments of the invention serve to explain the principles of the invention and not to limit its scope.
One embodiment of the invention, as shown in fig. 1, discloses a device for purifying and recovering nitrogen oxide in tail gas of a mobile source, which consists of a tail gas purification system arranged on a chassis of a road motor vehicle or non-road mobile source equipment, an ozone or low-temperature plasma generation and supply system, an absorption liquid circulating system, an absorption product concentration and recovery system, and a control system embedded in a mobile source control mechanism; the inlet of the tail gas purification system is connected with the tail gas outlet of an engine of a road motor vehicle or a non-road mobile source device, the ozone or low-temperature plasma generation and supply system, the absorption liquid circulating system and the absorption product concentration and recovery system are connected with the tail gas purification system, and the ozone or low-temperature plasma is firstly utilized to oxidize the mobile source tail gas nitrogen oxides (including nitric oxide and nitrogen dioxide) which are or are not subjected to catalytic oxidation treatment into high-valence nitrogen oxides. Then, absorbing high-valence nitrogen oxides with good water solubility by using alkaline absorption liquid to form nitrate aqueous solution; and the characteristics of good water solubility and reactivity of the ozone are utilized, so that the slightly excessive ozone is dissolved into the absorption liquid and reacts with the reducing components of the absorption liquid to consume the slightly excessive ozone, thereby preventing the ozone from leaking; the invention can realize the effective utilization of the waste heat of the tail gas, saves the energy required by the recovery and utilization of nitrate, and does not relate to the medicaments of volatile ammonia components such as gaseous ammonia, ammonium water or urea aqueous solution, thereby having no safety risk.
Further, the exhaust gas purification system includes: the device comprises a catalytic oxidation converter 1, an evaporation concentrator 2, a mixer 3, an oxidation reaction pipe 4, a venturi pipe 5, an absorption reactor 6 and a high-efficiency cyclone separator 7 which are connected in sequence; the air inlet of the catalytic oxidation converter 1 is connected with an engine exhaust outlet of a road motor vehicle or a non-road mobile source device, and is used for partially or completely oxidizing nitrogen monoxide in the exhaust into nitrogen dioxide and oxidizing carbon monoxide and hydrocarbon in the exhaust into carbon dioxide and water; the inlet of the evaporation concentrator 2 is connected with the gas outlet of the catalytic oxidation converter 1, the evaporation concentrator 2 further comprises an absorption product inlet and an absorption product outlet, wherein the absorption product inlet is connected with the outlet of an absorption product conveying pump 21 of an absorption product concentration and recovery system, the evaporation concentrator 2 forms a heat exchange system, and the absorption product conveyed by the absorption product conveying pump 21, namely part of moisture of the absorption product, is heated and evaporated by using high-temperature tail gas entering from the catalytic oxidation converter 1, and the temperature of the tail gas is reduced; an outlet of an absorption product of the evaporation concentrator 2 is connected with an inlet of a temporary storage tank for nitrate concentrated solution and crystal of an absorption product concentration and recovery system, the concentrated solution of nitrate obtained by concentration automatically flows into the temporary storage tank, and steam generated by evaporation is automatically discharged to the atmosphere; the mixer 3 is connected with an ozone or low-temperature plasma generation and supply system, so that the cooled tail gas is fully mixed with the ozone or low-temperature plasma provided by the ozone or low-temperature plasma generation and supply system; the oxidation reaction tube oxidizes the nitrogen monoxide and the nitrogen dioxide in the tail gas into high-valence nitrogen oxides, and the high-valence nitrogen oxides comprise dinitrogen pentoxide, nitrogen trioxide and other high-valence nitrogen oxides; the venturi tube 5 is used for promoting the tail gas to be fully mixed and contacted with the absorption liquid fog drops from the absorption liquid circulating system; the absorption reactor 6 is used for further mixing and reacting absorption liquid fog drops and tail gas of the self-absorption liquid circulating system to form nitrate absorption liquid; the high-efficiency cyclone separator 7 is used for separating nitrate-containing fog drops in the purified gas discharged from the absorption reactor 6;
carbon monoxide and hydrocarbon in the tail gas can be oxidized into carbon dioxide and water through the catalytic oxidation converter 1, and part or all of nitric oxide in the tail gas is oxidized into nitrogen dioxide, so that the nitrogen dioxide exists in the form of nitrogen dioxide as far as possible before the nitrogen dioxide is converted into high-valence nitrogen oxide, and the dosage of ozone or low-temperature plasma which needs to be added is reduced; the mixer 3 is used for simultaneously introducing and contacting the tail gas and the ozone or the low-temperature plasma to generate primary mixing, and is internally provided with a helical blade to increase mixing force; an oxidation reaction tube is additionally arranged, so that the mixing and oxidation reaction time can be prolonged, the nitrogen oxide is oxidized by fully utilizing ozone or low-temperature plasma, and the residual ozone amount is reduced; the mixing of the absorption liquid and the tail gas is promoted by the Venturi tube 5; an absorption reactor 6 is additionally arranged, so that liquid absorption liquid can be more fully mixed and reacted with tail gas to generate nitrate; the liquid drops and the gas can be separated by adopting the high-efficiency cyclone separator 7; the ozone or low-temperature plasma generator 10 is a high-voltage discharge device which takes air as an air source and is powered by a vehicle-mounted power supply 9, and has the function of converting part of air into ozone or low-temperature plasma, and the vehicle-mounted power supply 9 can be better matched with the internal structure of the existing vehicle, so that the laying space of the device is reduced, and the portability is improved.
Further, the exhaust gas purification system further includes: the fine particle trap 8 that sets up behind high-efficient cyclone 7 and link to each other with its gas outlet, fine particle trap 8 is used for the entrapment 7 to handle the remaining particle size of back minimum, the particulate matter that the content is extremely low, only has the place of high requirement just to be equipped with to particulate matter emission control, other occasions need not be equipped with, can filter the particulate matter in the tail gas through setting up fine particle trap 8, so that the tail gas of emission can accord with the exhaust emission requirement of higher specification.
Further, the ozone or low-temperature plasma generation supply system includes: a vehicle-mounted power supply 9, an ozone or low-temperature plasma generator 10 and an ozone or low-temperature plasma nozzle 11; the vehicle-mounted power supply 9 is used for supplying power to the ozone or low-temperature plasma generator 10, the ozone or low-temperature plasma generator 10 takes air as a gas source to convert part of gas in the generator into ozone or low-temperature plasma, and the ozone or low-temperature plasma nozzle 11 is used for spraying air containing ozone or low-temperature plasma into the mixer 3.
Further, the absorption liquid circulation system includes: an absorbent tank 12, an absorption liquid tank 13, an absorption liquid circulation pump 14, an absorption liquid suction nozzle, and an injection hole 15; the absorbent box 12 is used for storing fresh alkaline aqueous solution, and a liquid outlet of the absorbent box 12 is connected with a liquid inlet of the absorbent box 13 through an electromagnetic valve; the other liquid inlet of the absorption liquid box 13 is connected with the liquid outlet of the high-efficiency cyclone separator 7 and the liquid outlet at the bottom of the absorption reactor 6, and the absorption liquid box 13 is used for temporarily storing fresh alkaline aqueous solution and absorption liquid flowing out of the absorption reactor 6 and the high-efficiency cyclone separator 7; a liquid outlet of the absorption liquid box 13 is connected with an absorption liquid nozzle and an injection hole 15 through an absorption liquid circulating pump 14, the absorption liquid nozzle 15 is positioned at the contraction section of the Venturi tube 5, the absorption liquid injection hole 15 is positioned on the central tube wall of the absorption reactor 6, and the absorption liquid nozzle and the injection hole 15 are used for injecting and atomizing circulating absorption liquid; the temporary storage of the absorbent can be carried out through the absorbent box 12, and the absorbent can be supplemented to the absorption liquid box by starting and stopping the electromagnetic valve; the absorption liquid box 13 is provided with two absorption liquid nozzles and two injection holes 15, the liquid outlet ends of which can be respectively communicated with the contraction section of the Venturi tube and the central tube of the absorption reactor, so that the absorption liquid can be ensured to be fully contacted with the tail gas, and the tail gas and the absorption liquid can be mixed at a more comprehensive angle in the process of going by means of different mixing modes of the Venturi tube 5 and the absorption reactor 6; the absorption product conveying pump 21 can convey the absorption product containing high-concentration nitrate after reaction to an evaporation concentrator so as to be evaporated, concentrated and utilized subsequently;
specifically, the absorber nozzle 15 located at the venturi tube 5 and the absorber spray hole 15 located at the absorption reactor 6 are arranged perpendicular to each other.
Further, the fresh aqueous alkaline solution includes, but is not limited to, at least one of the following: an aqueous solution of sodium hydroxide, sodium carbonate, sodium bicarbonate, potassium hydroxide, potassium carbonate, potassium bicarbonate, calcium oxide, or magnesium oxide; the absorption liquid in the absorption liquid box 13 is a solution formed by fresh alkaline aqueous solution and aqueous solution containing nitrate formed in the absorption process; nitrates include, but are not limited to, at least one of the following: sodium nitrate, potassium nitrate, calcium nitrate and magnesium nitrate.
Further, the absorption product concentration recovery system comprises: an absorption product delivery pump 21 and a nitrate concentrated solution and crystal temporary storage tank 22; a liquid inlet of the absorption product conveying pump 21 is connected with a liquid outlet of the high-efficiency cyclone separator 7, and a liquid outlet of the absorption product conveying pump is connected with the evaporation concentrator 2 and used for conveying the high-concentration nitrate solution to the evaporation concentrator 2; the evaporation concentrator 2 is a heat exchange system, high-temperature tail gas heats part of water of evaporation absorption products to concentrate the water, the concentrated nitrate solution obtained by concentration automatically flows into a nitrate concentrated solution and crystal temporary storage tank 22, and the nitrate concentrated solution and crystal temporary storage tank 22 is connected with the evaporation concentrator 2 and is used for storing the concentrated absorption solution flowing out of the evaporation concentrator 2 and nitrate crystals separated out due to natural cooling; the absorption liquid circulating pump 14 is additionally arranged, so that the absorption liquid can be caused to flow back, the effective components of the absorption liquid can be utilized to the maximum extent, and the absorption liquid circulating pump is matched with the absorbent box 12 and the electromagnetic valve to ensure that the absorption liquid can be stably and sufficiently supplied; the cooled nitrate solution and crystals can be collected in a centralized way by arranging the nitrate concentrated solution and crystal temporary storage tank 22 so as to be unloaded and reused regularly.
Further, the nitrate concentrate and crystal holding tank 22 is used for storing the absorption product from the evaporation concentrator 2 and the crystal formed by natural cooling, and the nitrate concentrate and crystal holding tank 22 can be taken out by a service station or a mobile source after the after-sales service organization and can be sent to a professional organization to be converted into the nitrate product.
Further, the control system includes: signal sensors, control unit 20 and actuators; the sensors comprise a temperature sensor 16 for sensing the temperature of the oxidation reaction tube, a pH value sensor 17 for sensing the pH value of the absorption liquid, an ozone sensor 19 for sensing the concentration of ozone and nitrogen oxides in the clean tail gas and a nitrogen oxide concentration sensor 18; the control unit 20 is configured to receive signals detected by the sensors, signals of the atmospheric temperature and signals of the amount of air entering the engine, perform data processing to determine parameter values such as the power supply voltage of the ozone or low-temperature plasma generator 10, the flow rate of the absorption liquid circulating pump 14, the flow rate of the absorption product delivery pump 21, and start and stop of the absorbent adding solenoid valve, and then issue commands for regulating and controlling the power supply voltage of the ozone or low-temperature plasma generator 10, the flow rate of the absorption liquid circulating pump 14, the flow rate of the absorption product delivery pump 21, and start and stop of the absorbent adding solenoid valve; the execution equipment comprises an ozone or low-temperature plasma generator 10 for executing regulation and control commands, an absorption liquid circulating pump 14, an absorption product delivery pump 21 and an absorbent feeding electromagnetic valve; the addition of the control unit 20 can detect various signals of the device during operation, and perform adaptive adjustment and response according to preset settings, such as heat release in oxidation reaction, detection of pH value of output absorption liquid, detection of ozone concentration and nitrogen oxide concentration in exhaust gas, so as to ensure stable internal reaction, stable supply of absorption liquid and continuous compliance of exhaust gas emission in continuous operation of the device.
The invention provides a method for purifying and recovering nitrogen oxides in tail gas of a mobile source, which comprises the following steps of after the tail gas is discharged from a tail gas outlet of an engine of the mobile source: 1) In the catalytic oxidation converter 1, carbon monoxide and hydrocarbons in the exhaust gas are oxidized into carbon dioxide and water, and at the same time, part or all of the nitrogen monoxide is oxidized into nitrogen dioxide; 2) In the evaporation concentrator 2, the tail gas and the absorption products conveyed by the absorption product conveying pump 21 are indirectly contacted for heat exchange, so that the temperature of the tail gas is reduced to below 150 ℃; 3) In the mixer 3, the tail gas is uniformly mixed with the additional ozone or low-temperature plasma; 4) In an oxidation reaction tube, nitrogen monoxide and nitrogen dioxide in tail gas are oxidized into dinitrogen pentoxide, nitrogen trioxide and other high-valence nitrogen oxides by additional ozone or low-temperature plasma; 5) In the Venturi tube 5, the oxidized tail gas is fully contacted with an externally added absorption liquid; 6) In the absorption reactor 6, the high-valence nitrogen oxides are absorbed by the alkaline aqueous solution to form a nitrate aqueous solution; 7) In the high-efficiency cyclone separator 7, fog drops in the tail gas are separated from the gas; 8) In the alternative fine particle catcher 8, fine particles with the particle size of less than 1 μm are separated, and the equipment is only equipped in places with extremely high requirements on particle emission control, and is not required to be equipped in other places; 9) The absorption reactor 6 and the high-efficiency cyclone separator 7 collect most of absorption liquid and return to the absorption liquid box 13, and a small part of absorption liquid is conveyed to the evaporation concentrator 2 by an absorption product conveying pump 21 to evaporate water and concentrate the absorption liquid; 10 In the temporary storage tank for the nitrate concentrated solution and the crystallisate, the nitrate solution is reduced in solubility due to cooling and gradually crystallized and separated out; 11 Nitrate mainly in a crystalline state in the temporary storage tank can be recovered by gas stations and automobile maintenance enterprises and sent to specialized institutions for resource utilization.
The above description is only for the preferred embodiment of the present invention, but the scope of the present invention is not limited thereto, and any changes or substitutions that can be easily conceived by those skilled in the art within the technical scope of the present invention are included in the scope of the present invention.
Claims (10)
1. A device for realizing the purification and recovery of nitrogen oxides in tail gas of mobile sources is characterized in that,
the device consists of a tail gas purification system, an ozone or low-temperature plasma generation and supply system, an absorption liquid circulating system, an absorption product concentration and recovery system and a control system embedded in a mobile source control mechanism, wherein the tail gas purification system is arranged on a chassis of a road motor vehicle or non-road mobile source equipment;
the inlet of the tail gas purification system is connected with the tail gas outlet of an engine of a road motor vehicle or a non-road mobile source device, and the ozone or low-temperature plasma generation and supply system, the absorption liquid circulating system and the absorption product concentration and recovery system are connected with the tail gas purification system.
2. The apparatus for implementing mobile source exhaust nitrogen oxide purification and recovery of claim 1, wherein the exhaust gas purification system comprises: the device comprises a catalytic oxidation converter, an evaporation concentrator, a mixer, an oxidation reaction pipe, a Venturi tube, an absorption reactor and a high-efficiency cyclone separator which are connected in sequence;
the air inlet of the catalytic oxidation converter is connected with an engine tail gas outlet of a road motor vehicle or a non-road mobile source device and is used for oxidizing part or all of nitric oxide in the tail gas into nitrogen dioxide and oxidizing carbon monoxide and hydrocarbon in the tail gas into carbon dioxide and water;
the inlet of the evaporation concentrator is connected with the gas outlet of the catalytic oxidation converter, the evaporation concentrator also comprises an absorption product inlet and an absorption product outlet, wherein the absorption product inlet is connected with the outlet of an absorption product conveying pump of the absorption product concentration and recovery system, the evaporation concentrator forms a heat exchange system, and part of moisture of the absorption product conveyed by the absorption product conveying pump is heated and evaporated by using high-temperature tail gas entering from the catalytic oxidation converter, and the temperature of the tail gas is reduced; an outlet of an absorption product of the evaporation concentrator is connected with inlets of a nitrate concentrated solution and a crystal temporary storage tank of the absorption product concentration recovery system, the concentrated nitrate solution obtained by concentration automatically flows into the temporary storage tank, and steam generated by evaporation is automatically discharged to the atmosphere;
the mixer is connected with the ozone or low-temperature plasma generation and supply system, so that the cooled tail gas is fully mixed with the ozone or low-temperature plasma provided by the ozone or low-temperature plasma generation and supply system;
the oxidation reaction pipe oxidizes nitrogen monoxide and nitrogen dioxide in tail gas into high-valence nitrogen oxides, and the high-valence nitrogen oxides comprise dinitrogen pentoxide, nitrogen trioxide and other high-valence nitrogen oxides;
the venturi tube is used for promoting the tail gas to be fully mixed and contacted with the absorption liquid fog drops from the absorption liquid circulating system;
the absorption reactor is used for further mixing absorption liquid fog drops of the self-absorption liquid circulating system with tail gas and reacting to form absorption liquid containing nitrate;
the high-efficiency cyclone separator is used for separating nitrate-containing mist droplets in the purified gas discharged from the absorption reactor.
3. The apparatus for implementing mobile source exhaust nitrogen oxide purification and recovery of claim 1, wherein the exhaust purification system further comprises: the fine particle catcher is arranged behind the high-efficiency cyclone separator and connected with the air outlet of the high-efficiency cyclone separator, is used for catching the particles with extremely small particle size and extremely low content remained after the treatment of the high-efficiency cyclone separator, and is only equipped in places with extremely high requirements on particle emission control, and does not need to be equipped in other places.
4. The apparatus for purifying and recovering nitrogen oxides in tail gas of mobile source according to claim 1, wherein the ozone or low-temperature plasma generation supply system comprises: a vehicle-mounted power supply, an ozone or low-temperature plasma generator and an ozone or low-temperature plasma nozzle;
the vehicle-mounted power supply is used for supplying power to the ozone or low-temperature plasma generator, the ozone or low-temperature plasma generator takes air as a gas source and converts part of gas in the ozone or low-temperature plasma generator into ozone or low-temperature plasma, and the ozone or low-temperature plasma nozzle is used for spraying the air containing the ozone or low-temperature plasma into the mixer.
5. The device for realizing purification and recovery of nitrogen oxides in tail gas of mobile source according to claim 1, wherein the absorption liquid circulating system comprises: the absorption agent box, the absorption liquid circulating pump, the absorption liquid nozzle and the jet hole;
the absorbent box is used for storing fresh alkaline aqueous solution, and a liquid outlet of the absorbent box is connected with a liquid inlet of the absorbent box through an electromagnetic valve;
the other liquid inlet of the absorption liquid box is connected with the liquid outlet of the high-efficiency cyclone separator and the liquid outlet at the bottom of the absorption reactor, and the absorption liquid box is used for temporarily storing fresh alkaline aqueous solution and absorption liquid flowing out of the absorption reactor and the high-efficiency cyclone separator;
the liquid outlet of the absorption liquid box is connected with an absorption liquid nozzle and a jet hole through an absorption liquid circulating pump, the absorption liquid nozzle is positioned on the contraction section of the Venturi tube, the absorption liquid jet hole is positioned on the central tube wall of the absorption reactor, and the absorption liquid nozzle and the jet hole are used for atomizing the circulating absorption liquid.
6. The apparatus for implementing mobile source tail gas nitrogen oxide clean-up and recovery of claim 5, wherein the fresh alkaline aqueous solution includes but is not limited to at least one of: an aqueous solution of sodium hydroxide, sodium carbonate, sodium bicarbonate, potassium hydroxide, potassium carbonate, potassium bicarbonate, calcium oxide, or magnesium oxide;
the absorption liquid in the absorption liquid tank is a solution formed by a fresh alkaline aqueous solution and an aqueous solution containing nitrate formed in the absorption process;
the nitrates include, but are not limited to, at least one of the following: sodium nitrate, potassium nitrate, calcium nitrate and magnesium nitrate, the cations of which are the same as the metal cations contained in the alkaline absorbent solution.
7. The apparatus for purifying and recovering nitrogen oxides in tail gas of mobile source according to claim 1, wherein the absorption product concentration and recovery system comprises: an absorption product delivery pump, a nitrate concentrated solution and a crystal temporary storage tank;
a liquid inlet of the concentrated absorption product delivery pump is connected with a liquid outlet of the high-efficiency cyclone separator, and a liquid outlet of the concentrated absorption product delivery pump is connected with the evaporation concentrator, so that high-concentration nitrate solution, namely an absorption product, is delivered to the evaporation concentrator;
the evaporation concentrator is a heat exchange system, partial water of the evaporation absorption product is heated by high-temperature tail gas to be concentrated, the concentrated nitrate solution obtained through concentration automatically flows into a nitrate concentrated solution and crystal temporary storage tank, the nitrate concentrated solution and crystal temporary storage tank is connected with the evaporation concentrator and is used for storing the concentrated absorption solution flowing out of the evaporation concentrator and the nitrate crystal separated out due to natural cooling.
8. The device for purifying and recovering nitrogen oxides in tail gas of mobile source according to claim 1, wherein the nitrate concentrated solution and crystal temporary storage tank is used for storing absorption products from the evaporation concentrator and crystals formed by natural cooling, and after the temporary storage tank is removed by an after-sales service mechanism of a gas station or a mobile source device, the nitrate concentrated solution and crystals can be sent to a professional mechanism to be converted into nitrate products.
9. The apparatus for purifying and recovering nitrogen oxides in tail gas of mobile source according to claim 1, wherein the control system comprises: the system comprises a signal sensor, a control unit and an execution device;
the sensors comprise a temperature sensor for sensing the temperature of the oxidation reaction tube, a pH value sensor for sensing the pH value of the absorption liquid, an ozone sensor for sensing the concentration of the clean tail gas ozone and the concentration of the nitric oxide and a nitric oxide concentration sensor;
the control unit is used for receiving signals measured by the sensors, signals of atmospheric temperature and air quantity entering the engine, performing data processing so as to determine parameter values or start-stop states of the ozone or low-temperature plasma generator power supply voltage, absorption liquid circulating pump flow, absorption product conveying pump flow, absorbent feeding solenoid valve start-stop and the like, and then sending commands for regulating and controlling the ozone or low-temperature plasma generator power supply voltage, the absorption liquid circulating pump flow, the absorption product conveying pump flow and the absorbent feeding solenoid valve start-stop;
the execution equipment comprises an ozone or low-temperature plasma generator for executing regulation and control commands, an absorption liquid circulating pump, an absorption product conveying pump and an absorbent feeding electromagnetic valve.
10. The method for purifying and recovering the nitrogen oxides in the tail gas of the mobile source by adopting the device as claimed in any one of claims 1 to 9, which is characterized in that after the tail gas is discharged from a tail gas outlet of an engine of the mobile source, the following steps are carried out in sequence to purify and recover the nitrogen oxides in the tail gas:
1) In the catalytic oxidation converter, carbon monoxide and hydrocarbons in the tail gas are oxidized into carbon dioxide and water, and simultaneously, part or all of the nitrogen monoxide is oxidized into nitrogen dioxide;
2) In the evaporation concentrator, the tail gas and the absorption product conveyed by the absorption product pump are indirectly contacted for heat exchange, so that the temperature of the tail gas is reduced to below 150 ℃;
3) In the mixer, the tail gas is uniformly mixed with the additional ozone or low-temperature plasma;
4) In an oxidation reaction tube, nitrogen monoxide and nitrogen dioxide in tail gas are oxidized into dinitrogen pentoxide, nitrogen trioxide and other high-valence nitrogen oxides by additional ozone or low-temperature plasma;
5) In the Venturi tube, the oxidized tail gas is fully contacted with an externally added absorption liquid;
6) In the absorption reactor, the high-valence nitrogen oxides are absorbed by an alkaline aqueous solution to form a nitrate aqueous solution;
7) In the high-efficiency cyclone separator, fog drops in the tail gas are separated from the gas;
8) In an alternative fine particle catcher, fine particles with the particle size of less than 1 mu m are separated, the equipment is only arranged at a place with extremely high requirements on particle emission control, and the equipment is not required to be arranged at other places;
9) The absorption reactor and the high-efficiency cyclone separator collect most of absorption liquid and return to the absorption liquid box, and a small part of absorption liquid is conveyed to the evaporation concentrator by the absorption product conveying pump to evaporate water and concentrate the absorption liquid;
10 In the temporary storage tank for nitrate solution and crystal, the nitrate solution is cooled to reduce the solubility and gradually crystallized and separated out;
11 Nitrate mainly in a crystalline state in the temporary storage tank can be recovered by gas stations and automobile maintenance enterprises and sent to specialized institutions for resource utilization.
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