CN107344068B - Flue gas seawater desulfurization and denitrification process integrating photocatalytic oxidation and photocatalytic aeration - Google Patents

Flue gas seawater desulfurization and denitrification process integrating photocatalytic oxidation and photocatalytic aeration Download PDF

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CN107344068B
CN107344068B CN201610286160.6A CN201610286160A CN107344068B CN 107344068 B CN107344068 B CN 107344068B CN 201610286160 A CN201610286160 A CN 201610286160A CN 107344068 B CN107344068 B CN 107344068B
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seawater
flue gas
desulfurization
denitrification
photocatalytic
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李春虎
李子真
袁国锋
孙波
冯丽娟
卞俊杰
王亮
王文泰
郑昱
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Ocean University of China
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Abstract

The invention discloses a flue gas seawater desulfurization and denitrification process integrating photocatalytic oxidation and photocatalytic aeration, which comprises the following three sub-process modules: flue gas and seawater are mixed through a jet flow reactor, and the three process modules are mutually connected in series and used in a combined mode to achieve the integrated purpose of simultaneously carrying out seawater flue gas desulfurization and denitrification and treating waste seawater. The invention has the advantages that: because the flue gas is simultaneously subjected to seawater desulfurization and denitrification, the volume of the whole photocatalytic seawater desulfurization and denitrification absorption tower and the aeration tank is greatly reduced, and the equipment installation and the technical popularization and use with limited area on a ship are facilitated. Only need photocatalyst, natural sea water just can realize the while of flue gas desulfurization denitration integration and the aeration of useless sea water discharge to reach standard, has reduced the mixing volume of air aeration volume and fresh sea water to show reduction engineering cost, have wide application prospect.

Description

Flue gas seawater desulfurization and denitrification process integrating photocatalytic oxidation and photocatalytic aeration
Technical Field
The invention relates to a flue gas seawater desulfurization and denitrification technology, in particular to a novel process for simultaneously desulfurizing and denitrifying flue gas of diesel engines of coal-fired power plants, ocean vessels, warships and offshore platforms by utilizing seawater.
Background
The seawater desulfurization technology began in the last 70 th century and was rapidly popularized and applied in coastal power plants in europe, america, asia, and the like. As is well known, natural seawater contains a large amount of soluble salts, is generally alkaline, has natural alkalinity of 1.2-2.5 mmol/L, has natural acid-base buffering capacity and SO2 absorption capacity, and is a theoretical basis for directly applying seawater to flue gas desulfurization.
The core of the seawater desulfurization process is the contact mass transfer of the flue gas and the seawater, and the process is carried out in gas-liquid contact mass transfer equipment. The packed tower is mass transfer equipment taking the packing in the tower as a gas-liquid two-phase contact member, has the characteristics of high separation efficiency, small resistance, large flux, large operation elasticity and the like, and almost has no amplification effect under the condition of good gas-liquid initial distribution.
The traditional seawater desulfurization process usually adopts random polypropylene filler or ceramic filler, and relatively, the polypropylene filler is easy to age, poor in wettability, short in service life and light in single weight; the modified catalytic ceramic structured packing has the characteristics of large specific surface area, high porosity, good wettability, small pressure drop, large flux, long service life, large operating liquid-gas ratio, large temperature elasticity and the like. In addition, the ceramic filler has the advantages of easy surface modification, high temperature resistance, seawater corrosion resistance, difficult blockage, good frost resistance, stable hydrothermal aging performance, low maintenance cost and the like. Under the support of the national '863' topic, Lichunhu et al also invented various seawater desulfurization efficient packing (preparation method of ceramic regular catalytic packing for seawater desulfurization, ZL 200910308778.8; preparation method of plastic regular catalytic packing for seawater desulfurization, ZL 200910308741.5) and seawater desulfurization process (a process for removing sulfur dioxide in flue gas by using seawater, ZL 200910310771. X). The invention of the seawater desulfurization filler and the process technology greatly improves the indexes of seawater spraying amount, seawater corrosion resistance of the filler, service life, waste acidic seawater aeration amount after desulfurization and the like in seawater desulfurization, but the technology still can not realize seawater denitrification.
On the other hand, the seawater desulfurization technology is gradually transplanted to the flue gas desulfurization of diesel engines of ships and offshore platforms, and the ship flue gas contains a large amount of atmospheric pollutants, wherein most of the atmospheric pollutants are SO2NOx and particulate matter. Wherein SO2The hazards of NOx to human health, animals and plants, crops, the ecological environment and the national economy are also increasingly well known. Data display, river vessel nationwide 2010Nitrogen oxides (NOx) in pollutants discharged by ship gases are as high as 81 million tons, and in coastal port areas where ships gather, the pollutants discharged by various ship gases are considerable and become the main source of port atmospheric pollution and haze. . The emission standard of the ship smoke is increasingly strict at home and abroad in the face of increasingly severe conditions. SO in the most strict ship tail gas according to the modification of the international Marpol convention for preventing pollution caused by ships (MARPOL) VI technical rule2NOx emission requirements have been in continuous effect in recent years. Therefore, relevant departments in China are always seeking effective solutions in recent years to meet international requirements as soon as possible.
At present, there are many international companies and technical varieties for the research of flue gas desulfurization of ships, including, for example, ten more of European, American, Marine Exhaust Solutions, Hamworthy Krystalllon, Ecospec, Advanced CleanupTectechnologies, DuPont, Wartsila, Green technology Marine, Alfa Laval Aalborg, Rolls-Roycecarine, MAN Diesel & Turbo, and Wartsila; at home, there are the Chinese ocean university, the university of continental maritime, the Shanghai ocean university, and the like. But the technology development and research for simultaneously desulfurizing and denitrating the flue gas of the ship are less.
Meanwhile, most of the ship companies simply move the developed and mature seawater desulfurization technology (alkaline or magnesium desulfurization) and the SCR denitration on land to the ship for desulfurization and denitration treatment of the ship exhaust. Although the method can achieve the purpose of purifying the flue gas, the method has the problems of large floor area, carrying of dangerous chemicals for ships, difficult supply of overseas ports, secondary pollution and the like, and the application of the method is limited to a certain extent. Therefore, the development of a flue gas purification technology more suitable for ships is gradually increasing.
Seawater desulfurization is an important research topic and a technical development direction in the field of direct utilization of seawater, and has extremely important scientific research and economic values. The subject group of the professor Lichun tiger of China ocean university invents a plurality of photocatalysts on the basis of a plurality of existing seawater desulfurization patents and research results, and makes the traditional seawater desulfurization technology change into simultaneous desulfurization and denitrification. The flue gas photocatalysis seawater purification technology has a reaction stripMild condition, low energy consumption, less secondary pollution and the like. The technique mainly utilizes semiconductor TiO2、BiVO4And g-C3N4When the materials are exposed to light with the band gap energy being more than the band gap energy, electrons on the valence band are excited to exceed the forbidden band and enter the conduction band, and corresponding holes are generated on the valence band, have strong electron gaining capability and can change water in the smoke into hydroxyl radicals, photogenerated electrons can change adsorbed oxygen into superoxide radicals, and the hydroxyl radicals and the superoxide radicals have strong oxidizing property and can capture SO2NOx system to be activated and oxidized into oxide SO in high valence state3And NO2. And high valence SO3And NO2Is easily absorbed and removed by alkaline seawater and is discharged into the sea.
Disclosure of Invention
The invention aims to provide a safe and efficient seawater desulfurization and denitrification process which is small in occupied area, low in engineering cost and suitable for integrating photocatalytic oxidation and photocatalytic aeration of ships.
The invention utilizes a photocatalytic ceramic filler catalyst to make SO in flue gas2And NOxIs catalytically oxidized into SO3And NO2The content of sulfite and nitrite entering the aeration tank is reduced from the source, meanwhile, the photocatalytic ceramic catalyst is also placed in the aeration tank, and COD and polycyclic aromatic hydrocarbon in the desulfurized wastewater seawater are further degraded, so that the area and the volume of the aeration tank can be obviously reduced, the mixing amount of air aeration and fresh seawater is reduced, and the construction cost is obviously reduced.
The invention comprises the following three sub-process modules: flue gas and seawater are mixed through a jet flow reactor, and the three process modules are mutually connected in series and used in a combined mode to achieve the integrated purpose of simultaneously carrying out seawater flue gas desulfurization and denitrification and treating waste seawater.
The specific process flow of the invention is as follows:
(1) the flue gas discharged by the ship diesel engine and fresh seawater are subjected to jet flow reactionAfter the reactor is mixed, the temperature of the flue gas is reduced from 380-450 ℃ to 70-90 ℃, and solid particles and partial SO in the flue gas are removed simultaneously2(first process module);
(2) the flue gas washed and cooled by the jet reactor is sent into a photocatalytic oxidation seawater desulfurization and denitrification absorption tower with a photocatalyst from the bottom, and fresh seawater is sprayed and washed from the top of the tower to remove SO in the flue gas2And NO2(ii) a At the same time, most of the SO is photocatalytically converted2By oxidation to SO3Oxidation of NO to NO2(ii) a The clean flue gas after the integrated treatment of desulfurization and denitrification is completed by the photocatalytic oxidation seawater desulfurization and denitrification absorption tower is discharged through a chimney (a second process module);
(3) the waste seawater washed by the jet reactor and discharged from the bottom of the absorption tower are simultaneously converged into an aeration tank, solid particles in the intercepted water are filtered by a ceramic plate, the filtered waste seawater is subjected to photocatalytic oxidation degradation of COD and part of polycyclic aromatic hydrocarbon by a photocatalyst under the aeration condition to reach the discharge standard, and the filtered waste seawater is directly discharged into the sea or is mixed with fresh seawater to ensure that the pH value of the mixed seawater is more than or equal to 6.8 and then is discharged into the sea; the solid particles trapped by the ceramic plate are compressed into a filter cake for storage (third process module).
The photocatalytic oxidation seawater desulfurization and denitrification absorption tower is a circular or square tower internally provided with a sieve plate, a photocatalyst and a light source.
The photocatalyst and the light source lamp in the photocatalytic oxidation seawater desulfurization and denitrification absorption tower are alternately placed through the sieve plate.
The light source is an ultraviolet lamp, a fluorescent lamp, a mercury lamp, an electrodeless lamp or an LED light source.
The photocatalyst is prepared from carbon nitride (g-C) as carrier3N4) Photoactive catalyst TiO2And graphene oxide; wherein the carbon nitride (g-C)3N4) Is a synthetic visible light catalyst; the optically active catalyst TiO2Is TiO as a nano agent2(ii) a The graphene oxide is prepared by oxidizing graphene which is prepared by taking graphite as a raw material through various methods.
The technological parameters of the photocatalytic oxidation seawater desulfurization and denitrification in the photocatalytic oxidation seawater desulfurization and denitrification absorption tower are that the temperature is 50-140 ℃, and the pressure is normal pressure.
The technological parameters of the photocatalytic degradation of the desulfurized acidic wastewater seawater COD and the polycyclic aromatic hydrocarbon in the aeration tank are that the temperature is normal temperature to 40 ℃, the air aeration is carried out, and the pH value is 1.0 to 7.0.
The invention has the advantages that: because the flue gas is simultaneously subjected to seawater desulfurization and denitrification, the volume of the whole photocatalytic seawater desulfurization and denitrification absorption tower and the aeration tank is greatly reduced, and the equipment installation and the technical popularization and use with limited area on a ship are facilitated. Only need photocatalyst, natural sea water just can realize the while of flue gas desulfurization denitration integration and the aeration of useless sea water discharge to reach standard, has reduced the mixing volume of air aeration volume and fresh sea water to show reduction engineering cost, have wide application prospect.
Drawings
FIG. 1 is a process flow diagram of the present invention.
1. Marine diesel engines; 2. a seawater-flue gas jet reactor; 3. a seawater pump for jet flow; 4. a photocatalytic oxidation seawater desulfurization and denitrification absorption tower; 5. a filler type photocatalyst; 6. an ultraviolet lamp; 7. a chimney; 8. a first-stage tower desulfurization and denitrification seawater pump; 9. a two-section tower desulfurization and denitrification seawater pump; 10. an aeration tank; 11. a mixing tank; 12. daylight lamp 13. photocatalyst filling; 14. an aeration tank seawater dilution pump; 15. an aeration blower.
Detailed Description
The present invention will be described in detail below with reference to the accompanying drawings by way of specific embodiments.
Example 1:
as shown in fig. 1, the main apparatus used in the present invention comprises: the device comprises a jet flow reactor 2, a photocatalytic oxidation seawater desulfurization and denitrification absorption tower 4 and an aeration tank 10, wherein the jet flow reactor 2 is a venturi tube made of stainless steel. The photocatalytic oxidation seawater desulfurization and denitrification absorption tower 4 consists of a square tower with the inner diameter of 1996 x 1996mm and the height of 98400mm (2 x 492 mm). A sieve plate is arranged in the device, a ceramic structured packing photocatalyst is arranged on the sieve plate, and an ultraviolet lamp is arranged on the photocatalyst to form the photocatalystThe seawater absorption tower plate unit is used for repeating the unit formed by combining the regular packing type photocatalyst and the ultraviolet lamp until the top of the tower, or the photocatalytic seawater absorption tower plate unit is formed by the ultraviolet lamp, the sieve plate and the ceramic regular packing type photocatalytic desulfurization and denitrification agent from bottom to top in the tower, and the unit is repeated to the top of the tower or mixed and assembled. Built-in 9.0m3Coating TiO2The regular ceramic packing photocatalyst. In order to facilitate observation of the flowing state of the fluid in the tower and the filling state of the filler, the tower body is provided with a pressure and temperature measuring port. The seawater is sprayed onto a regular ceramic filler type photocatalyst from the upper part of an absorption tower through a spray head, an H-shaped 350W ultraviolet lamp or a visible light source or an LED lamp is arranged in the absorption tower, an aeration tank is made of polytetrafluoroethylene with the length, the width and the height of 3000 x 3000 x 1200mm respectively, the H-shaped 350W ultraviolet lamp and the ceramic photocatalyst are arranged in the aeration tank, a miniature air compressor is used for aeration, and the air aeration amount is about 250m 3/H; SULZER S20 ship diesel engine produced by SULZER company of 2x1270KW Netherlands, and the generated tower inlet flue gas flow rate is 16000m3/h，SO2The inlet pressure is 0.12MPa, and the simulated flue gas SO2The content is about 1800mg/m3NO content of about 800mg/m3And also 12% of O2And 8% water vapor. The seawater spray flow is changed under the condition that the operating temperature of the seawater photocatalytic desulfurization and denitrification tower is 60 ℃, and the photocatalytic desulfurization rate and the denitrification rate of the flue gas at the outlet of the photocatalytic desulfurization and denitrification tower under four different seawater flows are measured. Wherein, the alkalinity of the desulfurized seawater is 2.28. The measured photocatalytic seawater desulfurization and denitrification rates are shown in table 1 below.
Table 160 ℃ and 350W ultraviolet lamp photocatalytic oxidation seawater desulfurization and denitrification rate
Serial number Jet sea water volume/m 3/h Spraying amount of seawater/m 3/h SO2Removal rate/% Denitration rate/%)
1 15 150 99.0 85
2 15 120 98.1 82
3 15 100 97.8 78
4 15 90 94.5 74
As can be seen from Table 1, the desulfurization rate and the denitrification rate were both decreased as the amount of sprayed seawater was decreased.
Example 2:
the device and the process flow are the same as those of the example 1, and the photocatalyst is changed into the modified TiO2Coating a ceramic filler photocatalyst which is coating g-C3N49m with graphene3Regular ceramic packing type photocatalyst and 400 is installedW H-type ultraviolet lamp, the simulated flue gas introduced into the photocatalytic seawater absorption tower is 1000mg/m3SO of (A)2、800mg/m3NO, 12% of O2And 8% of water vapor, the balance being N2The experimental temperature of the balanced mixed gas is 60-90 ℃. Jet sea water volume of 13m3Per hour, the spraying amount of seawater is 120m3And h, the waste seawater flowing out of the spray tower enters an aeration tank, the pH value in the aeration tank is measured to be about 1.0-1.5, and the COD is about 500-1000 mg/L. After the COD is degraded by photocatalysis and the seawater is diluted, the final experimental result is shown in the table 2.
TABLE 2 desulfurization, denitrification and COD degradation by photocatalytic oxidation of seawater at different temperatures and under 400W UV lamp
Temperature in the column/. degree.C SO2Removal rate/% NO removal Rate/% COD removal Rate/% pH value before treatment in aeration tank pH value of the diluted seawater in the aeration tank
60 99.0 88.2 80.1 1.1 6.8
70 98.4 87.9 82.2 1.0 6.9
80 98.0 85.8 82.4 1.3 6.9
90 97.1 85.6 82.1 1.4 6.9
As can be seen from Table 2, the flow of the jet flow seawater and the spray seawater is improved, the novel process not only realizes the simultaneous desulfurization and denitrification of the seawater, but also can treat the desulfurized acidic waste seawater up to the standard after the seawater is diluted.

Claims (6)

1. A flue gas seawater desulfurization and denitrification process integrating photocatalytic oxidation and photocatalytic aeration is characterized by comprising the following steps:
(1) mixing the flue gas discharged by the marine diesel engine and fresh seawater in a jet reactor, reducing the temperature of the flue gas from 380-450 ℃ to 70-90 ℃, and simultaneously removing solid particles and partial SO in the flue gas2；
(2) The flue gas washed and cooled by the jet reactor is sent into a photocatalytic oxidation seawater desulfurization and denitrification absorption tower with a photocatalyst from the bottom, and fresh seawater is sprayed and washed from the top of the tower to remove SO in the flue gas2And NO2(ii) a The photocatalyst is a quartz glassThe whole ceramic is used as carrier and consists of carbon nitride and optical active catalyst TiO2And graphene oxide; at the same time, most of the SO is photocatalytically converted2By oxidation to SO3Oxidation of NO to NO2(ii) a Discharging the clean flue gas subjected to the integrated desulfurization and denitrification treatment by the photocatalytic oxidation seawater desulfurization and denitrification absorption tower through a chimney;
(3) the waste seawater washed by the jet reactor and discharged from the bottom of the absorption tower are simultaneously converged into an aeration tank, solid particles in the intercepted water are filtered by a ceramic plate, the filtered waste seawater is subjected to photocatalytic oxidation degradation of COD and part of polycyclic aromatic hydrocarbon by a photocatalyst under the aeration condition to reach the discharge standard, and the filtered waste seawater is directly discharged into the sea or is mixed with fresh seawater to ensure that the pH value of the mixed seawater is more than or equal to 6.8 and then is discharged into the sea; and solid particles trapped by the ceramic plate are compressed into a filter cake for storage.
2. The seawater desulfurization and denitrification process for flue gas according to claim 1, wherein the photocatalytic oxidation seawater desulfurization and denitrification absorption tower is a circular or square tower with a built-in sieve plate, a photocatalyst and a light source.
3. The seawater desulfurization and denitrification process for flue gas as claimed in claim 2, wherein the photocatalyst and the light source lamp in the photocatalytic oxidation seawater desulfurization and denitrification absorption tower are alternately arranged through a sieve plate.
4. The process for seawater desulfurization and denitration of flue gas according to claim 2, wherein the light source is an ultraviolet lamp, a fluorescent lamp, a mercury lamp, an electrodeless lamp or an LED light source.
5. The seawater desulfurization and denitrification process for flue gas according to claim 1, wherein the photocatalytic oxidation seawater desulfurization and denitrification process parameter in the photocatalytic oxidation seawater desulfurization and denitrification absorption tower is 50-140 ℃, and the pressure is normal pressure.
6. The seawater desulfurization and denitrification process for flue gas according to claim 1, wherein the technological parameters for photocatalytic degradation of desulfurized acidic wastewater COD and polycyclic aromatic hydrocarbons in the aeration tank are temperature of normal temperature to 40 ℃, air aeration, and pH of 1.0 to 7.0.
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