CN1219580C - Coal-fired mercury discharge control method based on semi-dry process - Google Patents
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Abstract
The present invention discloses coal-fired mercury discharge control method on the basis of a semi-dry method. Additives are ejected in boiler flue gas, and partial elementary substance mercury in flue gas is oxidized oxidation state mercury which can be eliminated easily; solution containing oxidizing agents is sprayed to flue gas by a spraying device, elementary substance mercury is oxidized further, the temperature of flue gas is lowered simultaneously, and low temperature for adsorbing agents to perform higher adsorption efficiency is formed; adsorbing agents are ejected in the cooled flue gas, and oxidation state mercury and unconverted zero-valent mercury are basically; solid granular substances after mercury is adsorbed are collected by an electric cleaner or a bag dust collecting device; partial collected granular substances are returned, and residual partial granular substances are exhausted. The present invention has the advantages that the control of mercury pollution in coal-fired flue gas of no secondary pollution can be realized, gaseous zero-valent mercury, gaseous divalent mercury and granular mercury in flue gas of coal fired power plants are completely controlled, and the harmful substances are converted into inert compounds; mercury discharge is controlled by combining existing pollutant control devices of coal fired power plants, initial stage investments are reduced, and operation cost is saved.
Description
Technical Field
The invention relates to a coal-fired mercury emission control method based on a semi-dry method.
Background
Mercury is a well-known environmental pollutant, and various forms of mercury can be converted into inorganic divalent mercury after entering the atmosphere and water from a pollution source and then converted into methyl mercury under the biological action. Methyl mercury is enriched in aquatic organisms such as algae and fish, and is directly dangerous through food chainIs harmful to human health. The invasion of methyl mercury in the environment into various animals and plants increases the opportunity, range and way of methyl mercury invasion into human bodies, and causes more lasting harm to human bodies. The main source of mercury pollution is artificial mercury pollution. Statistically, the total amount of emissions into the atmosphere worldwide is about 5000 tons per year, of which 4000 tons is an artificial result. The anthropogenic source of mercury is related to: the smelting of mercury ores and other metals, the use in the chlor-alkali and electrical industries and the combustion of fossil fuels. Mercury evolution from coal combustion worldwide annually due to the massive combustion of coal accounts for a large portion of the mercury released by human activity, with approximately 35% of the mercury in the atmospheric environment resulting from coal combustion in 1983. Mercury is one of trace heavy metal elements in coal, and the average mercury content in the coal is in the range of 0.12-0.28 mk/kg according to statistics of the environmental protection organization of New Jersey (NJ DEPE) (1993). China is a country with large energy consumption, and the yield of 1989 raw coal exceeds 10 multiplied by 108Theton, in the total energy consumption of our country, coal accounts for over 75%, and over 80% of the coal is used for direct combustion, especially in power stations, industrial boilers and civil boilers. According to statistics, the accumulated emission of mercury to the atmosphere in the coal burning industry of China reaches 2493.8 tons since 1978 to 1995. The annual average rate of increase in mercury emissions was 4.8%. This figure will also grow as the economy develops. At present, coal-fired mercury pollution, particularly mercury discharge in coal-fired power plant boilers and environmental harmfulness have attracted attention from countries all over the world. However, with the further research, the pollution problem is solved.
With SO2、NOxCompared with the control research of pollutants, the research of the mercury precipitation and mercury control method of the fire coal is carried out at home and abroad at present. Until the 90 s of the twentieth century, many scholars began to attach attention and research. In 1990, the American Congress passed a revised air purification code. According to this amendment, the united states Environmental Protection Agency (EPA) has evaluated the emissions of hazardous pollutants (HAP) from fossil-fueled power plants, and has written a report on the sources of mercury emissions, methods of controlling emissions, and health effects to congress. Since then, the relevant scholars and research institutes in the united states have begun to do so with first and second chanceThe research on the mercury substance emission of the coal-fired power plant shows that heat waves for researching the mercury emission appear.
At present, from the general view of the developed countries on the control of the emission of pollutants in flue gas, the environmental protection requirement is higher and higher, and the control content is finer and finer. To meet these stringent regulations, a batch of new coal-fired flue gas demercuration methods and new devices should be developed successively. The current research aiming at the method for treating mercury by coal-fired flue gas is approximately as follows by combining domestic and foreign documents:
and removing mercury in the flue gas by using activated carbon adsorption. The garbage incinerator adopts the activated carbon adsorption and cloth bag dust removal technology for controlling the emission of heavy metal mercury, and the mercury removal efficiency of more than 90 percent can be obtained by selecting a proper carbon-mercury (C/Hg) ratio due to higher mercury concentration. For the mercury removal of flue gas of a coal-fired power plant boiler, the mercury concentration is low, the mercury removal efficiency is poor, the carbon mercury (C/Hg) ratio is properly increased, the mercury removal efficiency can reach more than 30%, but the method has high cost and is difficult to bear by a coal-fired power plant.
With calcium-based adsorbents (CaO, Ca (OH)2、CaCO3、CaSO4·2H2O) to remove mercury. In experiments carried out in simulation of coal-fired flue gas, it was found that Ca (OH)2For HgCl2The adsorption efficiency of the mercury can reach 85 percent, but the mercury can not adsorb the mercury (Hg) in the mercury0) Only at SO2In the presence of 18% Hg0Can be removed. Alkaline adsorbents like CaO also adsorb HgCl very well2，SO2When present, to Hg0The removal rate of (D) was 35%. At present, the calcium-based adsorbent is still in a laboratory research stage and is not used in industrial practice, and the method only treats Hg in flue gas of a coal power station boiler2+Has higher removal rate to Hg in the flue gas of the coal-fired power station boiler0The removal effect is not significant.
Zeolite materials are used as adsorbents for industrial boilers to control mercury emissions. One has added a known amount of elemental mercury (Hg) to the coal combustion flue gas0) The experiment shows that the zeolite can adsorb Hg at high temperature and low temperature0And Hg2+. The new adsorbent of zeolite material is still under study and should be engineeredThe use is not mature, and the efficiency of removing mercury from the flue gas of the coal-fired power station boiler is still to be improved.
Mercury is removed by a desulfurizer (FGD). Due to Hg in the flue gas2+Compounds such as HgCl2Is water soluble, the desulfurization system can capture the divalent mercury in the flue gas by dissolving it, and part of the elemental mercury and part of the divalent mercury in the flue gas are removed when passing through a dust collector (FF or ESP). The Wet desulphurization device (Wet FGD) can remove 80-95% of Hg in the flue gas2+And (4) removing. But for Hg which is insoluble in water0The catching effect was not significant. According to statistics, the removal rate of the total mercury in the flue gas by the WFGD is within the range of 45-55%. However, the WFGD treatment was only for Hg2+Effective when Hg is contained in smoke2+When most of mercury exists in the form, the mercury removal efficiency of WFGD is greatly improved, and the method can only be used as an auxiliary method for removing mercury from flue gas.
The mercury in the flue gas is removed by utilizing the adsorption effect of the fly ash. The fly ash generated by the fire coal can absorb mercury in flue gas, the fly ash with high carbon content is very beneficial to mercury adsorption, but scientists think that the carbon content of the fly ash is greatly increased, and the mercury adsorption capacity of the fly ash cannot be correspondingly improved. Furthermore, fly ash with high carbon content has low resistivity, which reduces the dust removal efficiency of the ESP. The use of Circulating Fluidized Bed (CFB) for mercury adsorption and particulate emission control has been studied abroad. The CFB increases the residence time of the particles (large amounts of fly ash stay in the CFB for 4s), making full use of the adsorption capacity of small particles for Hg. Meanwhile, the agglomeration of small particles is enhanced, the discharge of the small particles is reduced, and in addition, iodine-containing activated carbon (IAC) can be sprayed into the fluidized bed, so that the capture efficiency of Hg can be further improved. However, in general, the removal rate of the total mercury in the flue gas of the coal-fired power plant boiler is too low, and the method is difficult to popularize and apply.
At present, the mercury pollution control technology is applied to the industry of garbage incinerators abroad, and China does not have an industrial device special for removing mercury in flue gas. In view of the low mercury concentration and the high removal difficulty in the coal-fired flue gas, the technology in the field is in the industrial test and the pilot plant stage abroad, and is not popularized on a large scale. With increasingly stringent environmental requirements, the pollution control of heavy metals, especially mercury, from coal combustion is a matter of course. The method can be directly applied to occasions for controlling mercury emission in flue gas, such as coal-fired boilers, garbage incineration boilers and chemical manufacturers needing tail gas treatment, can be applied in a large scale after the coal-fired boilers come out of the country and come out of the emission control standard of mercury pollution of coal-fired, the United states can control mercury emission of coal-fired power station boilers in 2004, and China will come out of the corresponding environmental protection standard in the near future.
Disclosure of Invention
The invention aims to provide a coal-fired mercury emission control method based on a semi-dry method.
The method comprises the following steps:
1) spraying an additive at the flue gas temperature of 500-900 ℃, wherein the additive/mercury is approximately 600-1600 ℃;
2) when the temperature of the boiler flue gas is 150-160 ℃, spraying a solution to the flue gas through a spraying device, wherein the flow is less than or equal to 0.12% multiplied by the mass flow of the flue gas, so that the amount of the mercury in a catalytic oxidation elementary substance state is more than or equal to 80%;
3) spraying an adsorbent into the flue gas subjected to spray cooling, wherein the amount of the sprayed adsorbent is about 2000-30000 adsorbent/mercury;
4) collecting all the mercury-adsorbed particulate matters by an electric dust collector or a cloth bag dust collector;
5) the collected particulate matter is partially returned to discharge the remaining particulate matter.
The invention has the advantages that:
1) the method can realize the control of mercury pollution in coal-fired flue gas without secondary pollution, comprehensively control three forms of mercury (gaseous zero-valent mercury, gaseous divalent mercury and granular mercury) in the coal-fired power plant flue gas, and convert the forms into inert compounds.
2) The combined operation of spraying additive, spraying oxidant-containing solution (or oxidant-free water) and spraying adsorbent is adopted, and the adsorbent is chemically pretreated, so that the condition of forming stable compound between mercury and adsorbent is created, the content of oxidized mercury is increased, and the adsorption efficiency of the adsorbent and fly ash on mercury is improved.
3) After gaseous mercury is converted into solid stable inert compounds, the solid stable inert compounds can be removed by utilizing high-efficiency dust removal equipment (such as an electrostatic precipitator (ESP) or a bag-type dust remover and the like) commonly adopted by a coal-fired power plant without adding additional dust removal equipment.
4) The mercury emission control device can be combined with the existing pollutant control devices (such as a wet desulphurization device (WFGD), a dry desulphurization device (DFGD) and a semi-dry desulphurization device (SDFGD)) of the coal-fired power plant to control the mercury emission, so that the initial investment is reduced, and the operation cost is also saved.
5) The oxidized mercury is generated by spraying the additive and the solution containing the oxidant in the cooling process of the flue gas, and the newly generated oxidized mercury has high reaction activity, is easy to be adsorbed and has high removal efficiency.
6) And one part of the collected particulate matter is returned, so that the utilization rate of the adsorbent is improved.
Drawings
FIG. 1 is a diagram of a semi-dry based coal mercury emission control process (additive injection, flue gas spray and sorbent injection, considering particle fraction return);
FIG. 2 is a diagram of a semi-dry based coal mercury emission control scheme (simplified scheme A, only flue gas is sprayed and sorbent is injected, particle fraction return is considered);
FIG. 3 is a semi-dry based flow diagram for coal-fired mercury emission control (simplified scheme B, spraying and injection of sorbent only on flue gas, without regard to particle return).
Detailed Description
The method for controlling mercury in coal-fired flue gas based on the semidry method comprises the following steps:
1) when the temperature of the flue gas is 500-900 ℃, a proper amount of additive (additive/mercury is approximately 600-1600) is sprayed, the additive is one or more oxides and chlorides of transition metals and rare earth metals or a precursor and a precursor mixture thereof, the effective additive is a precursor compound of Fe, Cu, Zn and Mn metals and HCl, and after the additive is sprayed, the elemental mercury in the flue gas is converted into oxidized mercury which is easy to absorb and remove in the cooling process of the flue gas (the conversion rate is more than or equal to 30%).
2) When the temperature of the boiler flue gas is 150-160 ℃, a solution containing an oxidant (or water without the oxidant, which only plays a role of temperature reduction) is sprayed to the flue gas through a spraying device, the flow is less than or equal to 0.12% multiplied by the mass flow of the flue gas, elemental mercury (more than or equal to 80%) is further oxidized, part of bivalent mercury in the flue gas is dissolved, the elemental mercury is adhered to fly ash or an adsorbent through liquid particles, and meanwhile, the temperature of the flue gas is reduced to 90-100 ℃ after the solution is sprayed, so that the adsorption efficiency of the adsorbent is improved. The effective oxidant is hydrogen peroxide, chlorine water, chloric acid and sodium hypochlorite.
3) Spraying an adsorbent into the flue gas after being sprayed and cooled, wherein the amount of the adsorbent is about 2000-30000 per the type of the adsorbent, the adsorbent is generally activated carbon or modified activated carbon adsorbent, ore or modified ore adsorbent, biomass or modified biomass adsorbent or a mixture thereof, the effective adsorbent is activated carbon modified by activated carbon, modified montmorillonite, modified vermiculite, modified zeolite, modified activated clay, seaweed powder, biomass derived carbon and the like, the adopted adsorbent modification method is an impregnation method or a fumigation method, the adopted modified substance is generally a substance which can chemically react with mercury to generate a stable compound, and the effective modified substance is a compound of sulfur, polysulfide, sulfide, iodine, iodide, high-valence iron salt and manganese, the bivalent mercury and the elementary mercury in the adsorbed flue gas are converted into inert substances so as to eliminate the secondary pollution of the mercury.
4) All the mercury-adsorbed particulate matters are collected by an electric dust collector or a cloth bag dust collector (the total mercury removal efficiency is more than or equal to 85 percent).
5) The collected particulate matter is partially returned and the excess solid particulate matter is discharged.
The technical scheme of the invention can be improved into a simpler or more reasonable scheme according with the actual conditions, such as a simplified scheme A (shown in figure 2), aiming at the actual conditions of different furnace types, coal types, the existing desulfurization and dust removal pollution control equipment, combustion working conditions and the like in the implementation process: before the dust removing equipment, only spraying and spraying the adsorbent to the flue gas, and considering the particle return; simplified scheme B (as in fig. 3): before the dust removing equipment,only the flue gas is sprayed and sprayed with the adsorbent, and the particle return is not considered.
Example 1
As shown in figure 1, the flue gas flow of a certain coal-fired utility boiler is 8.31 multiplied by 105Nm3The mercury content in the generated flue gas is 6.8 mu g/Nm3. The additive is selected to be HCl (excessive HCl can be removed in a desulfurization device, secondary pollution cannot be caused), the injection amount of HCl/Hg is 600, the additive is injected at the temperature of 900 ℃, a part of elemental mercury is oxidized into mercury in an oxidation state under the condition that oxygen exists in flue gas, morphological analysis is carried out by an Ontario-Hydro method, and the result shows that the ratio of elemental mercury to mercury in the oxidation state is 80%; the reaction chemical equation is as follows:
when the temperature of the flue gas is 150 ℃, spraying a solution containing 0.5% of hydrogen peroxide into the flue gas through a spraying device, wherein the liquid flow is 600Kg/h, the hydrogen peroxide is decomposed by heat to generate active oxygen atoms, under the condition that hydrogen chloride exists in the flue gas, the elemental mercury is oxidized into mercury chloride or mercury oxide, morphological analysis is carried out by an Ontario-Hydro method, the result shows that the ratio of the elemental mercury converted into the oxidized mercury is increased to 90%, and the reaction chemical equation is as follows:
simultaneously, the temperature of the flue gas is reducedto 90 ℃; and then spraying the sulfur steam fumigation modified activated carbon adsorbent into the flue gas, wherein the spraying amount of C/Hg is 8000, so that the elemental mercury is converted into an inert substance HgS, secondary pollution of the mercury is prevented, and the reaction chemical equation is as follows (ad in the following formula represents an adsorption state):
so that bivalent mercury in the flue gas is converted into chemical adsorption state mercury to be solidified:
then collecting all the particulate matters by cloth bag dust removing equipment, and returning 8% of the total collected matters to a material storage tankThe mercury content in the flue gas after the dust remover is about 0.56-0.64 mug/Nm by repeated monitoring3The mercury removal efficiency is higher than 90%.
Example 2
As shown in FIG. 1, the flue gas flow and the mercury content in the flue gas were the same as in example one, and the additive was selected to be FeCl3FeCl of injected amount3The Hg is 1600, the mercury is sprayed at the smoke temperature of 800 ℃, a part of elementary mercury is oxidized into oxidized mercury, morphological analysis is carried out by an Ontario-Hydro method, and the result shows that the ratio of the elementary mercury converted into the oxidized mercury is 50 percent; the reaction chemical equation is as follows:
when the temperature of the flue gas is 160 ℃, spraying a solution containing 0.4 percent of sodium hypochlorite into the flue gas through a spraying device, wherein the liquid flow rate isThe ratio of the single mercury to the mercuric chloride or the mercuric oxide is increased to 80 percent at 600Kg/h, and the temperature of the flue gas is reduced to 100 ℃; then FeCl is sprayed into the flue gas3Dipping the modified vermiculite adsorbent, wherein the sprayed amount of vermiculite/Hg is 30000, collecting all the particulate matters by cloth bag dust removal equipment, returning 6% of the total collected amount to a flue through a material returning device, and repeatedly monitoring to obtain a flue gas with the total mercury content of about 0.95 mu g/Nm3Mercury removal efficiency reaches about 86%.
Example 3
As shown in fig. 2, no additive was sprayed compared to fig. 1. Flue gas production of about 6X 10 for a coal-fired boiler5Nm3H, the total mercury content in the flue gas produced is about 3.8 mug/Nm3. When the temperature of the flue gas is 150 ℃, spraying a solution containing 0.2 percent of chlorine water into the flue gas through a spraying device, wherein the liquid flow is 400Kg/h, the rate of oxidizing single mercury into mercuric chloride or mercuric oxide is increased to 86 percent, and the temperature of the flue gas is reduced to 100 ℃; then spraying MnO into the flue gas2Impregnating the modified activated carbon adsorbent, wherein the spraying amount is C/Hg 12000, so that the elemental mercury is converted into Hg2MnO2So as to be solidified, the adsorption process is a stronger chemical adsorption process, and new compound Hg is generated after the adsorption2MnO2：
The mercury is in a low-price state in the compound, and electrons are transferred from the mercury to manganese in the compound, so that the mercury and the manganese are strongly combined. Then collecting all the particulate matters by cloth bag dust removal equipment, returning 30% of the total collected amount to the flue through a material returning device, and reducing the content of total mercury in the flue gas after the dust remover to 0.36-0.38 mu g/Nm3The total mercury removal efficiency was 90%.
Example 4
As shown in FIG. 3, compared with FIG. 2, the method is further simplified, no additive is injected, the collected particles are not returned, the flue gas yield and the total mercury content in the flue gas are the same as those of the embodiment, and the flue gas temperature is about 150 DEG CWhen in use, a solution containing 0.1% chloric acid is sprayed into the flue gas through a spraying device, the flow rate is 400Kg/h, the ratio of the single mercury to the mercuric chloride or the mercuric oxide is improved to 83%, and the temperature of the flue gas is reduced to 100 ℃; then toSpraying activated MnO into flue gas2Soaking modified activated clay, spraying activated clay/mercury 20000, collecting all particulate matters by cloth bag dust removing equipment, returning 10% of the total collected amount to flue via material returning device, and measuring to reduce total mercury content in flue gas to 0.57 μ g/Nm3And the total removal efficiency of mercury in the flue gas after the dust remover reaches 85 percent.
Claims (5)
1. A coal-fired mercury emission control method based on a semidry method is characterized by comprising the following steps:
1) when the temperature of the flue gas of the boiler is 500-900 ℃, the additive is sprayed, and the additive/mercury is approximately 600-1600 ℃;
2) when the temperature of the boiler flue gas is 150-160 ℃, spraying a solution to the flue gas through a spraying device, wherein the flow is less than or equal to 0.12% multiplied by the mass flow of the flue gas, so that the amount of the mercury in a catalytic oxidation elementary substance state is more than or equal to 80%;
3) spraying an adsorbent into the flue gas subjected to spray cooling, wherein the amount of the sprayed adsorbent is about 2000-30000 adsorbent/mercury;
4) collecting all the mercury-adsorbed particulate matters by an electric dust collector or a cloth bag dust collector;
5) the collected particulate matter is partially returned to discharge the remaining particulate matter.
2. The semi-dry based coal-fired mercury emissions control method of claim 1 wherein said additive is selected from the group consisting of oxides, chlorides of Fe, Cu, Zn, Mn metals.
3. The semi-dry based coal-fired mercury emissions control method of claim 1 wherein the spray solution is an aqueous solution containing an oxidant or water without an oxidant.
4. The semi-dry based coal-fired mercury emissions control method of claim 3, wherein said oxidant is selected from the group consisting of hydrogen peroxide, chlorine water, chloric acid, sodium hypochlorite.
5. The semi-dry based coal-fired mercury emissions control method of claim 1 wherein the sorbent is selected from the group consisting of activated carbon, modified activated carbon, montmorillonite, modified montmorillonite, vermiculite, modified vermiculite, zeolite, modified zeolite, activated clay, modified activated clay, seaweed meal, biomass-derived carbon.
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