CN101607173A - The sulfur removal technology of using external regenerative cycle magnesium sulfate method flue gas or waste gas - Google Patents
The sulfur removal technology of using external regenerative cycle magnesium sulfate method flue gas or waste gas Download PDFInfo
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Abstract
The sulfur removal technology of a kind of using external regenerative cycle magnesium sulfate method flue gas or waste gas, it is that the flue gas or the waste gas that contain sulfur dioxide are introduced the absorption tower continuously, with the sulfur dioxide in magnesium sulfite absorption liquid circulated sprinkling absorption flue gas or the waste gas, make the magnesium sulfite in the absorption liquid change into magnesium bisulfite, remove the sulfur dioxide in flue gas or the waste gas, absorption liquid at the bottom of the absorption tower distributed partly or entirely enter the outer regenerative system of tower, regenerate with the magnesia slurry reaction, the regenerated liquid of gained is filtered, reclaim the magnesium sulfite solid, filtrate turns back to the absorption tower absorption that circulates, constantly with the sulfur dioxide removal in flue gas or the waste gas.The outer regeneration technology of absorption liquid tower, the pH of regenerative response terminal point and the conversion ratio of medicament have been improved, reduce the temperature of absorption liquid, made absorption liquid possess the characteristics of high pH (7.2-8.5), low temperature (38-48 ℃), high absorptive capacity, effectively improved the absorption activity of absorption liquid.
Description
Technical field
The present invention relates to flue gas desulfurization technique, especially relate to the magnesium sulfite wet fuel gas desulfurizing technology.
Background technology
Flue gas desulfurization by magnesia wet method technology is succeeded in developing Philadelphia Electric after the seventies (PECO) and United the sixties in last century by U.S. Kai Mike basis company the earliest; Constructor joint study magnesia method of reproduction sulfur removal technology, through after several thousand hours the trial run, (wherein two are respectively 150MW and 320MW) dropped into FGD system and two magnesia regenerative systems of full scale on three generating sets, said system was built up and is put into operation in nineteen eighty-two, later stoppage in transit sulfuric acid manufactory in 1992 directly sells product magnesium sulfate.Binzhou, domestic Shandong 2 * 240t/hr boiler flue gas desulfurization has adopted the magnesium oxide method sulfur removal technology.
The principle of flue gas desulfurization by magnesia wet method is magnesia to be carried out digestion reaction generate magnesium hydroxide, make certain density magnesium hydroxide and absorb slurries, the reaction of magnesium hydroxide and sulfur in smoke generates magnesium sulfite and magnesium bisulfite in the absorption tower, the part magnesium bisulfite that generates continues to generate magnesium sulfite with the magnesium hydroxide reaction in the absorption tower, and the mix slurry that reaction generates is proceeded circulation and absorbed.Final disposal approach by its desulfurization product magnesium sulfite is divided into magnesium sulfate method and magnesia method of reproduction, its difference is that the former carries out oxidation with the magnesium sulfite bubbling air in tower that generates, and discharges in the tower after the circulating absorption solution magnesium sulfate concentration reaches 7-8% and carries out subsequent treatment; The magnesium sulfite solid slurry that contains that the latter will generate is discharged in the absorption tower, control circulation fluid solid content 7-10%, and the magnesium sulfite solid of discharge carries out high-temperature roasting after drying and other treatment, reclaim magnesia and sulfur dioxide.Owing to of the restriction of conditions such as the regenerative response mixability that is subjected to regenerative response system in the tower, the time of staying to the regenerative response degree, for guaranteeing the conversion ratio of magnesium hydroxide, its regenerative response carries out under the excessive condition of magnesium bisulfite, and the condition of its regenerative response PH control is PH:5.8-6.5.In above-mentioned PH interval, structure and sulfur dioxide inlet concentration according to the absorption tower, the liquid-gas ratio of control absorption process is 3-5 liter (absorption liquid)/mark cubic meter (gas), 50 ℃-55 ℃ of absorption liquid temperature, desulphurization system flue gas crushing 1200-2000Pa, magnesium sulphur is than 1.1-1.2: 1, and desulfuration efficiency is greater than 90%.
The patent of at present domestic and international magnesium oxide method and the significant improvement that document does not relate to reaction mechanism and technology, domestic patent " a kind of magnesia flue gas desulfurization and the oxidation of product thick slurry process reclaim technology " (CN1762550A) and " a kind of flue gas desulfurization by magnesia wet method and product reclaim new technology " (CN1481926A) proposed to adopt flue gas recirculation to carry dense reclaim sulfuric acid magnesium and adopt in the absorption tower respectively to propose the technology that the underflow oxidation generates magnesium sulfate, do not relate to improvement to flue gas desulfurization absorption and regeneration of absorption solution technology from the angle of reclaim sulfuric acid magnesium." the continuous reclaiming method of a kind of exhuast gas desulfurization, defluorinating absorbent liquid " of inventor's invention though (CN200610098180.7) sulfur method is improved to some extent, also needs NaOH, sodium carbonate, sodium acid carbonate or sodium sulfite.
China's magnesite reserves the first in the world, purity height, desulfurization material light-burning magnesium powder are the product after the simple calcining of magnesite, relative low price, and the magnesium oxide method desulfurization has huge resources advantage in China for this reason; In flue gas desulfurization course, because the solubility of the neutralization reaction speed of magnesia and acid solution and formation sulphite is all greater than the calcium method, all show bigger advantage aspect the preventing of fouling in the comprehensive utilization of absorption reaction speed, absorptivity, liquid-gas ratio, power consumption, waste residue and tower, this method has become the optimised process of present replace lime-gypsum method.But this method is owing to prolong the method for having used regeneration in the lime-gypsum method circulating absorption solution tower, though at project occupation of land, the compatible aspect of process equipment and lime stone-gypsum method possesses certain advantage, but because regenerative response is subjected to solid-liquid to mix degree in the tower, the restriction of conditions such as reaction time, for keeping its higher regenerative response and oxidizing reaction rate and raising raw material availability, can only implement the regenerative response under low pH (5.8-6.5) condition, the high regenerative response speed of magnesium method desulfurization, the absorption activity of high PH reaction solution, advantages such as reaction generation sediment free settling separation are not embodied fully, mainly show:
Absorption system still is low pH slurries circulating system, equipment anticorrosion, wear-resisting and anti-blocking requirement height, and key equipments such as stirring in circulating pump, the tower, shower nozzle still need import, and the engineering equipment investment is big;
Be subjected to the restriction of low pH absorption liquid absorption reaction activity and absorptive capacity, for reaching higher desulfuration efficiency, still need bigger liquid-gas ratio, flue gas is bigger in the pressure loss of absorption system, and power consumption and operating cost are bigger;
Regenerative response is high to the equipment requirement in the tower, power consumption is big, efficient is low.
The desulfurization product oxidation generates only 5-10% of magnesium sulfate concentration, and comprehensive utilization value is low, consumes a large amount of supplementing water simultaneously; Desulfurization product adopts the recovery system of roasting recovery magnesia technology huge, and investment and energy consumption are big;
Regenerative response is incomplete, and the magnesian utilization rate of medicament is low, has increased operating cost, has increased the difficulty of Treatment of Sludge;
Be to improve the reaction rate of regenerative response in the tower, need magnesia unslacked is digested to magnesium hydroxide, increased the investment of equipment and power, consumption of heat energy.
Summary of the invention
The sulfur removal technology of a kind of using external regenerative cycle magnesium sulfate method flue gas or waste gas, it comprises the following steps:
Flue gas or waste gas that step 1. will contain sulfur dioxide are introduced the absorption tower continuously, with the sulfur dioxide in magnesium sulfite absorption liquid circulation absorption flue gas or the waste gas, make the magnesium sulfite in the absorption liquid change into magnesium bisulfite, remove the sulfur dioxide in flue gas or the waste gas, its reaction is:
MgSO
3+SO
2+H
2O→Mg(HSO
3)
2 (1)
Reaction (1) is a fast response, has possessed high absorption reaction activity under low liquid-gas ratio.Absorption reaction is controlled by air film, reduces the absorption liquid temperature, and the pH value that improves absorption liquid helps reducing SO
2Equilibrium partial pressure, improve absorption efficiency.
Mg(HSO
3)
2+MgO→MgSO
3↓+H
2O (2)
Because the reaction product magnesium sulfite is the slightly soluble material, its solubility is much larger than the solubility of calcium method calcium sulfite, the magnesium sulfite that regenerative response produces enters liquid phase rapidly and combines generation three water magnesium sulfite crystallizations with crystal seed, avoided magnesium sulfite to influence further carrying out of regenerative response in the deposition of mgo surface, the reproduction speed of reaction (2) is far above the calcium method for this reason.
Step 3. is filtered the regenerated liquid of step 2 gained, reclaims the magnesium sulfite solid, and filtrate turns back to the absorption tower absorption that circulates, constantly with the sulfur dioxide removal in flue gas or the waste gas.
The above-mentioned using external regenerative cycle magnesium sulfate method flue gas or the sulfur removal technology of waste gas, the magnesium sulfite absorption liquid is solution or the suspension that comprises magnesium sulfite or magnesium sulfite and magnesium bisulfite in the described step 1.
The above-mentioned using external regenerative cycle magnesium sulfate method flue gas or the sulfur removal technology of waste gas, the pH=6-6.8 of absorption liquid at the bottom of the described absorption tower of step 2.
The above-mentioned using external regenerative cycle magnesium sulfate method flue gas or the sulfur removal technology of waste gas, the spray flux of the described absorption liquid of step 1 are 1-4 liter/mark cubic meter flue gas.In this liquid-gas ratio scope, the clearance of sulfur dioxide is 85-99.5%.
The above-mentioned using external regenerative cycle magnesium sulfate method flue gas or the sulfur removal technology of waste gas, the described magnesia slurries of step 2 are to contain magnesia or/and the slurries of magnesium hydroxide also can be directly to use magnesia solid regenerated.
The above-mentioned using external regenerative cycle magnesium sulfate method flue gas or the sulfur removal technology of waste gas, to distribute and partly or entirely enter the outer regenerative system of tower be to distribute absorption liquid at the bottom of the tower of 25-100% to absorption liquid at the bottom of the described tower of step 2.
The above-mentioned using external regenerative cycle magnesium sulfate method flue gas or the sulfur removal technology of waste gas, the regenerative response time of the described regenerative process of step 2 needs 12-36 minute.
The above-mentioned using external regenerative cycle magnesium sulfate method flue gas or the sulfur removal technology of waste gas, the described regenerative process of step 2, its startup stage, control the crystallization water content and the particle diameter of its crystal by adding crystal seed, the composition of crystal seed is three water magnesium sulfites.
The above-mentioned using external regenerative cycle magnesium sulfate method flue gas or the sulfur removal technology of waste gas, the pH of the filtrate after the described regeneration of step 3 is 7.2-8.5.
The above-mentioned using external regenerative cycle magnesium sulfate method flue gas or the sulfur removal technology of waste gas, the temperature of the described regeneration rear filtrate of step 3 is 38-48 ℃.
The above-mentioned using external regenerative cycle magnesium sulfate method flue gas or the sulfur removal technology of waste gas, the filtrate after the described regeneration of step 3 are clear liquid or solid-liquid mixing suspension, and the mass ratio of its solid content is 0-1.5%.Its liquid phase main component is the aqueous solution of magnesium sulfite and magnesium sulfate, and solid phase composition main component is magnesium sulfite, magnesia and/or magnesium hydroxide.Magnesium sulfate in the liquid phase be owing to the dioxygen oxidation that contains some in the flue gas magnesium sulfite form, be the side reaction in the course of reaction:
2MgSO
3+O
2→2MgSO
4 (3)
The MgSO that reaction (3) generates
4Influence the absorption activity of absorption liquid, control its concentration in circulating system by draining.
The above-mentioned using external regenerative cycle magnesium sulfate method flue gas or the sulfur removal technology of waste gas, described absorption tower comprises the upper and lower two-layer spraying layer that is positioned at the absorption tower, absorption liquid after the regeneration preferentially enters the upper strata spray, and the pH value of upper strata spray absorption liquid is more than or equal to the pH value of lower floor's spray absorption liquid.
The above-mentioned using external regenerative cycle magnesium sulfate method flue gas or the sulfur removal technology of waste gas, before step 1 setting up procedure can be arranged: the flue gas or the waste gas that will contain sulfur dioxide are introduced the absorption tower continuously, be lower than 0.5% magnesium hydroxide slurry with solid content in the absorption system absorption that circulates, remove the sulfur dioxide in flue gas or the waste gas, finish start-up course to absorption liquid pH≤6, absorption liquid enters the external regeneration system and regenerates.Following chemical absorbing reaction takes place in the absorption tower during this time:
Mg(OH)
2+SO
2→MgSO
3 (4)
MgSO
3+SO
2+H
2O→Mg(HSO
3)
2 (5)
Reaction (4) (5) are the main chemical reaction that absorbs, and the startup incipient stage is mainly reacted (4), and this reaction is long response time, and absorption process is controlled by liquid film, and absorption efficiency is extremely low; Along with the carrying out of reaction (4), liquid phase MgSO3 concentration constantly increases, and absorption process is mainly reacted (5), and this reaction is fast response, and absorption efficiency significantly improves; Along with constantly carrying out of absorption process, liquid phase Mg (HSO3) 2 content increase, and pH value of solution reduces, and behind pH≤6, absorption efficiency significantly descends, and absorption liquid at the bottom of the absorption tower is entered the outer regenerative system of tower, regeneration magnesium sulfite absorption liquid.
Advantage of the present invention is in particular in:
The outer regeneration technology of absorption liquid tower, the pH of regenerative response terminal point and the conversion ratio of medicament have been improved, reduce the temperature of absorption liquid, made absorption liquid possess the characteristics of high pH (7.2-8.5), low temperature (38-48 ℃), high absorptive capacity, effectively improved the absorption activity of absorption liquid;
Height absorbs active absorption liquid, has reduced the liquid-gas ratio of absorption system, has reduced the pressure loss of flue gas in desulphurization system simultaneously.(under the situation that reaches identical removal efficient, liquid-gas ratio of the present invention and air-channel system crushing only be conventional oxidation magnesium method 1/2 and 3/5), effectively reduce operating cost;
Because absorption system is the low-solid content absorption liquid circulating system of high pH, equipment and pipeline anticorrosion antiwear require to reduce, avoided the import of key equipments such as desulfuration recycle pump, shower nozzle, the interior stirring of tower, the high reaction activity of absorption liquid has reduced the volume on absorption tower simultaneously, and equipment investment significantly reduces;
The outer regenerative response of tower has further improved regenerative response speed and efficient; Induced crystallization technology makes regeneration product magnesium sulfite crystal formation good, has created condition for follow-up efficient Separation of Solid and Liquid, and the equipment scale of external regeneration system is little;
Power consumption significantly reduces, improve constantly under the situation in present promotion energy-saving and emission-reduction and rate for incorporation into the power network, the advantage of the present invention aspect society, economy, environmental benefit is obvious day by day, simultaneously in non-electricity or thermoelectric enterprise, because its electricity rates and rate for incorporation into the power network all are higher than electricity power enterprise, its economic advantages are obvious further;
The solidliquid mixture that Separation of Solid and Liquid produces after mud concentrates, need not to carry out press filtration and handles, and its content of magnesium has reached 5-8%, if with its oxidation, the magnesium sulfate concentration of generation approaches the saturated concentration of magnesium sulfate, produces magnesium sulfate for comprehensive utilization and has created condition;
The magnesian utilization rate of desulfurizing agent improves 5-10% than prior art.Magnesia slurries (solid) are directly participated in regenerative response, need not magnesian digestion process; Material consumption, energy consumption, the water consumption of digestion facility and digestion process have been reduced;
Employing equipment is conventional homemade common apparatus, and the present invention uses on medium and small boiler flue gas desulfurization still has good cost performance;
Increased the floor space of regenerative system than magnesium oxide method, but because the reclaim equiment scale is less, the regenerative system floor space is in the acceptable scope of electric power enterprise.Simultaneously, regenerative system can be arranged with the absorption system branch, is convenient to the horizontal layout of project and the desulfurization transformation of old facility.
Description of drawings
Fig. 1 is a process flow diagram of the present invention, and wherein: 1 is desulfuration absorbing tower, and 2 is the liquid storage section, 3 are lower floor's spray, 4 are the upper strata spray, and 5 is demister, and 6 is the absorption liquid storage tank, 7 are the regeneration liquid bath, 8 is static mixer, and 9 is magnesia slurry batch tank, and 10 is regeneration reactor, 11 is sedimentation basin, and 12 is filter press.
The specific embodiment
Embodiment
Shown in process chart: the boiler sulfur-containing smoke gas of process dust removal process, send into desulfuration absorbing tower 1 by air-introduced machine, with the absorption liquid counter current contacting absorption desulfurization of lower floor's spray 3 and 4 ejections of upper strata spray, process demister 5 demists are after the chimney emptying.Liquid storage section absorption liquid enters absorption liquid storage tank tower outside through pipeline 13 gravity flow at the bottom of the tower, partially absorbs liquid and proceeds the desulfurization absorption by circulating pump through lower floor's spray that pipeline 14 pumps in the absorption tower, partially absorbs liquid and is reproduced pump and pumps into static mixer 8 through pipeline 15.Magnesia powder as desulfurizing agent, sending into magnesia slurry batch tank 9 from the magnesia storage tank mixes with fresh water (FW) and joins slurry, the magnesia slurry of configuration pumps into static mixer 8 by mashing pump through pipeline 16 efficiently to be mixed with the absorption liquid that enters, and mixed suspension enters regeneration reactor 10 through pipeline 18 and carries out regenerative response; The absorption liquid of finishing regenerative response enters sedimentation basin 11 through pipeline 19 gravity flows and carries out the separation of solid-liquid body, and sediment is transported outward comprehensive utilization or sanitary landfills by sludge pump after pipeline 21 pumps into the filter press press filtration.The upper strata suspension of sedimentation basin or clear liquid enter regeneration liquid bath 7 through pipeline 20 gravity flows, and regeneration liquid bath 7 links to each other by subsurface pipeline 22 with absorption liquid storage tank 6, to keep the level balance of regeneration liquid bath 7 and absorption liquid storage tank 6.Absorption liquid in the regeneration liquid bath 7 carries out the desulfurization absorption by spray pump through the upper strata spray that pipeline 17 pumps in the absorption tower.According to regeneration liquid measure big I be provided with a plurality of parallel connections or series connection static mixer and regeneration reactor.
We utilize one 75 of certain thermoelectric enterprise to steam a ton/hour coal-fired fluidized bed boiler and are provided with experimental provision of the present invention by above-mentioned technological process, boiler steady-state operation parameter is: exhaust gas volumn 100,000 mark cubic meters/hour, 135 ℃ of desulfurizer gas approach temperature, SO 2 from fume concentration 1260-1450 milligram/mark cubic meter.Absorption system and regenerative system apart arrangement, 120 square metres of regenerative system floor spaces.Desulphurization system is provided with as follows:
Absorption system: absorption tower Φ 2800 * 15000, adopt spray column, two-layer spray, upper and lower layer spray provides absorption liquid respectively by two circulating pumps, the upper strata spray adopts the high pH absorption liquid in the regeneration liquid bath, lower floor's spray adopts the low pH absorption liquid in the circulation liquid bath, and pump flow passes through VFC.Two-layer corrugated plating demister, resistance 200Pa are established in the top, absorption tower; Establish the liquid storage section at the bottom of the absorption tower, 2 meters of height; Each 20 cubic metres of regeneration liquid bath, absorption liquid storage tanks, pipeline links to each other to keep level balance under the two tank liquor faces.
Regenerative system: low pH absorption liquid pumps into regenerative system by regenerative pump, by regenerative pump is implemented its regenerant flow of VFC; 10 cubic metres of magnesia slurry batch tank dischargeable capacitys, stirring is set, magnesia concentration of slurry 20%, configuration magnesia slurries do not carry out slaking, adopt measuring pump that the magnesia slush pump is gone into static blender, regenerative process added the magnesia slurry by magnesium sulphur than 1.08: 1; Regeneration reactor is made up of the stirred tank of four parallel connections, 20 cubic metres of every stirred tank dischargeable capacitys, and the cooling heat transferring face is established in the stirred tank outside, by being arranged on the use number of the valve control stirred tank before the stirred tank, thereby regulates the regenerative response time of staying; Solid-liquid separation system adopts inclined-plate clarifying basin, 50 square metres of sedimentation basin surface areas.Mud adopts the plate and frame filter press drying and other treatment.
Under flue gas steady-state operation parameter condition, according to the form below content adjustment liquid-gas ratio, reproduction ratio and the regeneration time of staying, after treating regenerative system stable operation, measure the temperature and the solid content of desulfuration efficiency, desulphurization system crushing, regenerative response pH variation, regenerative system water outlet, test data shows, under the condition of following examples, desulphurization system all can reach satisfactory absorption efficiency.Adopt operation and the online detection of flue gas of 7 continuous half a year of embodiment to show: system's desulfuration efficiency maintains more than 95% all the time, and stable equipment operation finds no fouling and burn into wear phenomenon.
Claims (10)
1. the sulfur removal technology of using external regenerative cycle magnesium sulfate method flue gas or waste gas is characterized in that it comprises the following steps:
Flue gas or waste gas that step 1. will contain sulfur dioxide are introduced the absorption tower continuously, with the sulfur dioxide in magnesium sulfite absorption liquid circulation absorption flue gas or the waste gas, make the magnesium sulfite in the absorption liquid change into magnesium bisulfite, remove the sulfur dioxide in flue gas or the waste gas
Step 2. with the absorption tower at the bottom of absorption liquid distribute and partly or entirely enter the outer regenerative system of tower, regenerate with the magnesia slurry reaction,
Step 3. is filtered the regenerated liquid of step 2 gained, reclaims the magnesium sulfite solid, and filtrate turns back to the absorption tower absorption that circulates, constantly with the sulfur dioxide removal in flue gas or the waste gas.
2. the sulfur removal technology of using external regenerative cycle magnesium sulfate method flue gas according to claim 1 or waste gas is characterized in that: the magnesium sulfite absorption liquid is solution or the suspension that comprises magnesium sulfite or magnesium sulfite and magnesium bisulfite in the described step 1.
3. the sulfur removal technology of using external regenerative cycle magnesium sulfate method flue gas according to claim 1 or waste gas is characterized in that: the pH=6-6.8 of absorption liquid at the bottom of the described absorption tower of step 2.
4. the sulfur removal technology of using external regenerative cycle magnesium sulfate method flue gas according to claim 1 or waste gas is characterized in that: the described magnesia slurries of step 2 are to contain magnesia or/and the slurries of magnesium hydroxide, or directly use magnesia solid regenerated.
5. the sulfur removal technology of using external regenerative cycle magnesium sulfate method flue gas according to claim 1 or waste gas is characterized in that: to distribute and partly or entirely enter the outer regenerative system of tower be to distribute absorption liquid at the bottom of the tower of 25-100% to absorption liquid at the bottom of the described tower of step 2.
6. the sulfur removal technology of using external regenerative cycle magnesium sulfate method flue gas according to claim 1 or waste gas, it is characterized in that: the described regenerative process of step 2, its the startup stage, control the crystallization water content and the particle diameter of its crystal by adding crystal seed, the composition of crystal seed is three water magnesium sulfites.
7. the sulfur removal technology of using external regenerative cycle magnesium sulfate method flue gas according to claim 1 or waste gas is characterized in that: the pH of the filtrate after the described regeneration of step 3 is 7.2-8.5.
8. the sulfur removal technology of using external regenerative cycle magnesium sulfate method flue gas according to claim 1 or waste gas, it is characterized in that: the filtrate after the described regeneration of step 3 is clear liquid or solid-liquid mixing suspension, the mass ratio of its solid content is 0-1.5%, its liquid phase main component is the aqueous solution of magnesium sulfite and magnesium sulfate, and the solid phase main component is magnesium sulfite, magnesia and/or magnesium hydroxide.
9. the sulfur removal technology of using external regenerative cycle magnesium sulfate method flue gas according to claim 1 or waste gas, it is characterized in that: described absorption tower comprises the upper and lower two-layer spraying layer that is positioned at the absorption tower, absorption liquid after the regeneration preferentially enters the upper strata spray, and the pH value of upper strata spray absorption liquid is more than or equal to the pH value of lower floor's spray absorption liquid.
10. the sulfur removal technology of using external regenerative cycle magnesium sulfate method flue gas according to claim 1 or waste gas, it is characterized in that: setting up procedure was arranged before step 1: the flue gas or the waste gas that will contain sulfur dioxide are introduced the absorption tower continuously, be lower than 0.5% magnesium hydroxide slurry with solid content in the absorption system absorption that circulates, remove the sulfur dioxide in flue gas or the waste gas, finish start-up course to absorption liquid pH≤6, absorption liquid enters the external regeneration system and regenerates.
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