CN102335553A - Reproduction method for sodium-base flue gas desulfurization liquid - Google Patents
Reproduction method for sodium-base flue gas desulfurization liquid Download PDFInfo
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- CN102335553A CN102335553A CN2010102320595A CN201010232059A CN102335553A CN 102335553 A CN102335553 A CN 102335553A CN 2010102320595 A CN2010102320595 A CN 2010102320595A CN 201010232059 A CN201010232059 A CN 201010232059A CN 102335553 A CN102335553 A CN 102335553A
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Abstract
The invention relates to a reproduction method for sodium-base flue gas desulfurization liquid, which is characterized in that the flue gas desulfurization liquid containing sodium sulphite and sodium bisulfite is oxidized to a solution containing sodium sulfate, the solution containing sodium sulfate is electrolyzed to a sodium hydroxide solution and a sulfuric acid solution by using bipolar membrane electrodialysis. According to the invention, the electrolytic conversion rate of sodium sulfate can reach more than 90%, the obtained sodium hydroxide solution can be used as absorption liquid for a flue gas desulfurization tower, the sulfuric acid by-product is produced simultaneously. By-product sulfuric acid can be used as sulfuric acid for treating high hardness and high alkalinity. The reproduction method for sodium-base flue gas desulfurization liquid is capable of achieving the purposes of strong brine zero-draining, comprehensive resource utilization and cost reduction.
Description
Technical field
The present invention relates to a kind of renovation process of flue gas desulfurization liquid, particularly a kind of renovation process of sodium base flue gas desulfurization liquid.
Background technology
The aerial existence of sulfur oxide can have a strong impact on people's physical and mental health.It also is an atmosphere pollution simultaneously, and the accumulation in atmosphere is a main cause that causes acid rain.Acid rain can make forest withered, soil and lake acidifying, and crop production reduction, metal and construction material are corroded.Therefore, the pollution problem of sulfur oxide is the World Health Organization and United Nations Environment Programme and each national attention day by day.How reduce sulfur oxide under the industrial situation and become problem demanding prompt solution not influencing to airborne discharging.
The flue gas desulfurization technique of countries in the world research and development hundreds of, but commercial application be no more than 20 kinds.Whether add the wet form of doing of water or desulfurization product by sweetening process, flue gas desulfurization can be divided into wet method, semidry method and three types of technologies of dry method again.
The wet desulphurization technology maturation, efficient is high, and is reliable, simple to operate, but the processing of desulfurization product is cumbersome, and floor space is bigger with investment; The desulfurization product of dry method, semidry method is a powdered, handles easily, and technology is simpler, and investment generally is lower than conventional wet, but does the dry method of desulfurizing agent, the Ca/S ratio height of semidry method with lime (lime stone), and the utilization rate of desulfuration efficiency and desulfurizing agent is low.
In recent years, although semidry method and desulfurization by dry method and application thereof have had bigger development, wet desulphurization is still uses maximum desulfur technologies at present in the world.In the wet processing, lime stone (lime)-gypsum method technology is the most ripe, uses also extensive, but the required liquid-gas ratio height of this technology, power consumption is big, and has the fouling and the blockage problem of equipment and pipeline.
Soda is faster than calcium alkali to the absorption rate of oxysulfide, and needed liquid-gas ratio is much lower, can save power consumption; And all compounds all can remain in the solution in the system; Can avoid the fouling and the blockage problem of equipment and pipeline, therefore, the soda absorption process more receives people's attention.But because the soda price is more expensive, causes operating cost high, and produce the high concentration brine waste, its discharging can impact environment equally.
Two alkaline process absorb sulfur in smoke with sodium carbonate or sodium hydroxide solution (first alkali); Generate sodium base flue gas desulfurization liquid-promptly the contain solution of sodium sulfite and sodium hydrogensulfite; With lime or lime stone (second alkali) NaOH of regenerating, so recycle again.Adopt the relatively cheap calcium alkali of the price soda of regenerating, reduced operating cost.But this technology is because the alkali lye after the regeneration is saturated calcium sulfite solution, and fouling in conveyance conduit and absorption tower easily influences system's long-term operation.Simultaneously, because the two alkali process long flow paths of Sodium, the control point is many in the actual moving process, causes control unstable easily, influences operational effect.In addition, in two alkaline process, inferior sulfate radical is easy to be oxidized into sulfate radical in the absorption tower; And sulfate radical poor removal effect in the calcium method regenerative process, thereby cause the accumulation of sulfate radical, therefore; In actual moving process, a certain amount of high slat-containing wastewater of still will draining can impact environment equally.
Bipolar Membrane is the swifter and more violent a kind of novel amberplex of development in recent years, and it is composited by cation exchange layer and anion exchange layer usually.Anode membrane contains electronegative active group usually, can see through cation, and anion is then stopped; And cavity block contains the active group of positively charged usually, can see through anion, but repels and stop cation.The selection permeability of Here it is amberplex.Bipolar Membrane is composited by the negative and positive film because of it, so have the characteristic of negative and positive film concurrently; Produced new characteristic simultaneously: under the effect of DC electric field, dissociating of water will take place in the interface of yin, yang rete, produces H
+And OH
-H
+Can be combined into acid with anion, OH
-Can be combined into alkali with cation.
The bipolar membrane electrodialysis technology is a kind of high performance membrane isolation technics, and its basic foundation is the directed movement of ion under electric field action and the selection permeability of amberplex, and the distinctive hydrolysis of Bipolar Membrane produces H
+, OH
-Ability.The bipolar membrane electrodialysis Study on Technology is carried out like a raging firely both at home and abroad, and being applied to large-scale production also has 20 years history nearly.The domestic in recent years research to Bipolar Membrane itself is deep to some extent, and the cost and the film resistance of film reduce gradually, and the film contamination resistance improves constantly, and the basis that the bipolar membrane electrodialysis technology is applied to flue gas desulfurization alkali regeneration technology has been arranged.
Chinese patent CN1302920A discloses and a kind ofly has been used for the flue gas desulfurization occasion, and is suitable for the sodium sulphate of anionic membrane electrolytic cell, the electrolytic method of niter cake, it is characterized in that going out NaOH through the anionic membrane electrolytic regeneration.This invention can effectively reduce electrolysis energy consumption; But still contain a large amount of sodium sulphate in the regenerated liquid that electrolysis obtains; And it is very low really oxysulfide to be had a sodium hydrate content of absorbability, and this kind regenerated liquid is back to the power consumption that flue gas desulphurization system can be strengthened in the absorption tower.
Summary of the invention
The inventor finds: earlier with the doctor solution oxidation, utilize the resultant oxidation liquid of bipolar membrane electrodialysis electrolysis again, can solve the problems referred to above that prior art exists.
The object of the present invention is to provide a kind of renovation process of sodium base flue gas desulfurization liquid, can obtain sodium hydroxide solution and sulfuric acid solution with this method, sodium hydroxide solution can be used as absorption liquid and is back to fume desulfurizing tower, and sulfuric acid solution can be used as byproduct.
For achieving the above object; The present invention provides a kind of renovation process of sodium base flue gas desulfurization liquid; Comprise that the flue gas desulfurization liquid that will contain sodium sulfite and sodium hydrogensulfite is oxidized to the solution of contains sodium sulfate, utilize bipolar membrane electrodialysis that the contains sodium sulfate electrolysis of solutions is sodium hydroxide solution and sulfuric acid solution.
Oxidation of the present invention is to use the oxygen-containing gas oxidation, preferably uses the air or oxygen oxidation, more preferably uses air oxidation.
The present invention preferably adopts the method oxidation sweetening liquid of logical oxygen-containing gas, and throughput is 0.5～5L/minL doctor solution, and the ventilation oxidization time is 1-5h.
The pH value that the present invention preferably controls doctor solution is 3-7.
Bipolar membrane electrodialysis of the present invention is accomplished in the Bipolar Membrane electrolytic cell, and the structure optimization of electrolytic cell is three cell structures, i.e. alkali chamber-salt chamber-sour cell structure.The present invention adopts the assembling mode of Bipolar Membrane-anion-exchange membrane-cation-exchange membrane-Bipolar Membrane that electrolytic cell is separated composition alkali chamber, salt chamber and sour chamber.
The disclosed Bipolar Membrane of prior art all can be used for the present invention, and Bipolar Membrane of the present invention can be selected commercially available Bipolar Membrane for use, comprises but is not limited only to following: out-phase Bipolar Membrane (Shanghai Chemical Plant's production), BP-1 type Bipolar Membrane (production of Tokuyama company) etc.The disclosed anion-exchange membrane of prior art all can be used for the present invention; Anion-exchange membrane according to the invention can be selected commercially available anion-exchange membrane for use; Comprise but be not limited only to following: polyethylene out-phase anion-exchange membrane (Shanghai Chemical Plant's production), DF120 series homogeneous-phase anion exchange film (sky, Shandong dimension membrane technology Co., Ltd produces) etc.The disclosed cation-exchange membrane of prior art all can be used for the present invention; Cation-exchange membrane according to the invention can be selected commercially available cation-exchange membrane for use; Comprise but be not limited only to following: polyethylene out-phase cation-exchange membrane (Shanghai Chemical Plant's production); DF120 series homogeneous phase cation exchange film (sky, Shandong dimension membrane technology Co., Ltd produces), Nafion cation-exchange membrane (production of Dupont company), Aciplex-F cation-exchange membrane (Asahi KASEI company gives birth to) etc.
The electrode of the disclosed electrolytic cell of prior art all can be used for the present invention, as long as produce enough electric currents, as selecting titanium plating ruthenium electrode, stainless steel electrode etc., the preferred titanium plating of the present invention ruthenium electrode for use.
The operational factor of bipolar membrane electrodialysis is among the present invention:
A) importing concentration in salt chamber is the metabisulfite solution of 2-16%; It is the metabisulfite solution of 0.05-1% that concentration is derived in the salt chamber.
B) importing concentration in alkali chamber is the sodium hydroxide solution of 1-5%; It is the sodium hydroxide solution of 3-15% that concentration is derived in the alkali chamber.
C) sour chamber importing concentration is the sulfuric acid solution of 1-5%; It is the sulfuric acid solution of 5-25% that concentration is derived in the acid chamber.
D) the initial current density of electrolysis is 10-120mA/cm
2
E) solution of contains sodium sulfate is 2-15h in the time of staying of electrolytic cell.
The electrolysis conversion ratio of sodium sulphate of the present invention can reach more than 90%, and the sodium hydroxide solution that obtains can be used as absorption liquid and is back to fume desulfurizing tower, simultaneously by-product sulfuric acid.Accessory substance sulfuric acid can be used as the sulfuric acid that high hard high-alkali circulating water treatment is used.The purpose that can reach strong brine zero-emission, comprehensive utilization of resources and reduce cost with method of the present invention.
Description of drawings
Fig. 1 is the electrolytic cell configuration sketch map of bipolar membrane electrodialysis regeneration sodium hydroxide.
The specific embodiment
Specify the present invention below in conjunction with embodiment and accompanying drawing, but do not limit to its scope.
To contain 3.3% sodium sulfite and 0.37% sodium hydrogensulfite, volume is that the doctor solution of 2L is used the sulphur acid for adjusting pH value, and control pH value is 6.Through sudden and violent gas head blowing air in doctor solution, throughput is the 2.5L/minL doctor solution.The ventilation oxidization time keeps 3h, and oxygenation efficiency reaches 100%, obtains concentration and be 4% metabisulfite solution.According to accompanying drawing 1, adopt the assembling mode of out-phase Bipolar Membrane-polyethylene out-phase anion-exchange membrane-polyethylene out-phase cation-exchange membrane-out-phase Bipolar Membrane that electrolytic cell is separated composition alkali chamber, salt chamber and sour chamber, the used electrode of electrolytic cell is a titanium plating ruthenium electrode.With concentration is 4%, and volume is that the metabisulfite solution of 2L injects the salt chamber, and alkali chamber and sour chamber implantation concentration respectively are 2%, and volume is NaOH and the sulfuric acid solution of 0.5L, and circulating pump starts the back opening power, and initial current density is 20mA/cm
2Na
+And SO
4 2-Under the effect of voltage, see through anionic membrane and cationic membrane respectively and get into alkali chamber and sour chamber, Na
2SO
4Solution concentration reduces with the prolongation of conduction time.The hydrone of Bipolar Membrane interlayer is dissociated into H under the voltage effect
+And OH
-, OH
-The cation exchange layer that sees through Bipolar Membrane gets into the alkali chamber, with Na
+Form NaOH solution; H
+The anion exchange layer that sees through Bipolar Membrane gets into sour chamber, with SO
4 2-Form H
2SO
4Solution.Behind the energising 5.5h, the electrolysis conversion ratio of sodium sulphate reaches 73%, and the naoh concentration of alkali chamber is 3.8%, and the sulfuric acid concentration of sour chamber is 6%.
Embodiment 2
Operating procedure is with embodiment 1; Operating condition is following: will contain 5.8% sodium sulfite and 0.65% sodium hydrogensulfite, volume is that the doctor solution use sulphur acid for adjusting pH value of 2L is 4, blowing air; Throughput is the 1L/minL doctor solution; The ventilation oxidization time keeps 2.5h, and oxygenation efficiency reaches 100%, obtains concentration and be 7% metabisulfite solution.With concentration is 7%, and volume is the salt chamber that the metabisulfite solution of 2L injects the Bipolar Membrane electrolytic cell, and alkali chamber and sour chamber implantation concentration respectively are 1.5%, and volume is NaOH and the sulfuric acid solution of 0.5L, energising, and initial current density is 35mA/cm
2Behind the electrolysis 3.5h, the electrolysis conversion ratio of sodium sulphate reaches 67%, and the naoh concentration of alkali chamber is 5.2%, and the sulfuric acid concentration of sour chamber is 8.9%.
Embodiment 3
Operating procedure is with embodiment 1; Operating condition is following: will contain 8.3% sodium sulfite and 0.92% sodium hydrogensulfite, volume is that the doctor solution use sulphur acid for adjusting pH value of 2L is 5, blowing air; Throughput is the 2L/minL doctor solution; The ventilation oxidization time keeps 1.5h, and oxygenation efficiency reaches 100%, obtains concentration and be 10% metabisulfite solution.With concentration is 10%, and volume is the salt chamber that the metabisulfite solution of 2L injects the Bipolar Membrane electrolytic cell, and alkali chamber and sour chamber implantation concentration respectively are 1%, and volume is NaOH and the sulfuric acid solution of 0.5L, energising, and initial current density is 50mA/cm
27.5h after, the electrolysis conversion ratio of sodium sulphate reaches 80%, and the naoh concentration of alkali chamber is 8.0%, and the sulfuric acid concentration of sour chamber is 14.3%.
Embodiment 4
Operating procedure is with embodiment 1; Operating condition is following: will contain 11.6% sodium sulfite and 1.3% sodium hydrogensulfite, volume is that the doctor solution use sulphur acid for adjusting pH value of 2L is 5, blowing air; Throughput is the 3L/minL doctor solution; The ventilation oxidization time keeps 2h, and oxygenation efficiency reaches 100%, obtains concentration and be 14% metabisulfite solution.With concentration is 14%, and volume is the salt chamber that the metabisulfite solution of 2L injects the Bipolar Membrane electrolytic cell, and alkali chamber and sour chamber implantation concentration respectively are 1%, and volume is NaOH and the sulfuric acid solution of 0.5L, energising, and initial current density is 70mA/cm
2Behind the electrolysis 10.5h, the electrolysis conversion ratio of sodium sulphate reaches 94%, and the naoh concentration of alkali chamber is 12.8%, and the sulfuric acid concentration of sour chamber is 23.25%.
The present invention is oxidized to sodium sulphate with sodium sulfite in the doctor solution and sodium hydrogensulfite earlier; Utilize the bipolar membrane electrodialysis electrolysis to be sulfuric acid and NaOH again; The sodium hydroxide solution that obtains can be used as absorption liquid and is back to fume desulfurizing tower (alkali absorption tower), simultaneously by-product sulfuric acid.The purpose that has reached comprehensive utilization of resources and reduced cost.
Claims (11)
1. the renovation process of a sodium base flue gas desulfurization liquid comprises the solution that the flue gas desulfurization liquid that contains sodium sulfite and sodium hydrogensulfite is oxidized to contains sodium sulfate, utilizes bipolar membrane electrodialysis that the contains sodium sulfate electrolysis of solutions is sodium hydroxide solution and sulfuric acid solution.
2. renovation process according to claim 1 is characterized in that described oxidation is to use the oxygen-containing gas oxidation, preferably uses the air or oxygen oxidation, more preferably uses air oxidation.
3. renovation process according to claim 1 and 2 is characterized in that the pH value of controlling flue gas desulfurization liquid is 3-7.
4. according to claim 2 or 3 described renovation process, it is characterized in that adopting the method oxidation sweetening liquid of logical oxygen-containing gas, throughput is 0.5～5L/minL doctor solution, and the ventilation oxidization time is 1-5h.
5. according to each described renovation process of claim 1-4, it is characterized in that bipolar membrane electrodialysis accomplishes in the Bipolar Membrane electrolytic cell, the structure of electrolytic cell is three cell structures, i.e. alkali chamber-salt chamber-sour cell structure.
6. renovation process according to claim 5 is characterized in that adopting the assembling mode of Bipolar Membrane-anion-exchange membrane-cation-exchange membrane-Bipolar Membrane that electrolytic cell is separated composition alkali chamber, salt chamber and sour chamber.
7. renovation process according to claim 6 is characterized in that Bipolar Membrane is out-phase Bipolar Membrane, BP-1 type Bipolar Membrane; Anion-exchange membrane is polyethylene out-phase anion-exchange membrane, DF120 series homogeneous-phase anion exchange film; Cation-exchange membrane is polyethylene out-phase cation-exchange membrane, DF120 series homogeneous phase cation exchange film, Nafion cation-exchange membrane, Aciplex-F cation-exchange membrane.
8. according to each described renovation process of claim 1-7; It is characterized in that it is the metabisulfite solution of 2-16% that Bipolar Membrane electrolysis lake salt chamber imports concentration; It is the sodium hydroxide solution of 1-5% that Bipolar Membrane electrolytic cell alkali chamber imports concentration, and it is the sulfuric acid solution of 1-5% that Bipolar Membrane electrolytic cell acid chamber imports concentration.
9. according to each described renovation process of claim 1-8, the initial current density that it is characterized in that electrolysis is 10-120mA/cm
2
10. according to each described renovation process of claim 1-8, it is characterized in that contains sodium sulfate solution is 2-15h in the time of staying of electrolytic cell.
11., it is characterized in that the sodium hydroxide solution of gained is back to fume desulfurizing tower as absorption liquid according to each described renovation process of claim 1-10.
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| CN101878327A (en) * | 2008-12-23 | 2010-11-03 | 卡勒拉公司 | Low-energy electrochemical hydroxide system and method |
| US8834688B2 (en) | 2009-02-10 | 2014-09-16 | Calera Corporation | Low-voltage alkaline production using hydrogen and electrocatalytic electrodes |
| US8869477B2 (en) | 2008-09-30 | 2014-10-28 | Calera Corporation | Formed building materials |
| US8883104B2 (en) | 2009-03-02 | 2014-11-11 | Calera Corporation | Gas stream multi-pollutants control systems and methods |
| US8894830B2 (en) | 2008-07-16 | 2014-11-25 | Celera Corporation | CO2 utilization in electrochemical systems |
| CN104478141A (en) * | 2014-12-05 | 2015-04-01 | 杭州水处理技术研究开发中心有限公司 | Power plant flue gas desulfurization wastewater treatment process |
| CN104529016A (en) * | 2014-08-12 | 2015-04-22 | 华东理工大学 | Method for treating high-salinity wastewater |
| CN104857838A (en) * | 2015-04-09 | 2015-08-26 | 北京廷润膜技术开发有限公司 | System and method for flue gas desulfurization through bipolar membrane electrodialysis |
| CN105056763A (en) * | 2015-09-02 | 2015-11-18 | 河南工业大学 | Method for removing salt in water through double-membrane dialysis under no-voltage condition and reactor |
| CN105110521A (en) * | 2015-08-25 | 2015-12-02 | 杭州蓝然环境技术有限公司 | Cyclic utilization method of desulphurization waste water |
| US9260314B2 (en) | 2007-12-28 | 2016-02-16 | Calera Corporation | Methods and systems for utilizing waste sources of metal oxides |
| CN105330049A (en) * | 2014-08-08 | 2016-02-17 | 中国石油化工股份有限公司 | Pretreatment method for desulphurization solution |
| CN106731562A (en) * | 2015-11-19 | 2017-05-31 | 中国石油化工股份有限公司 | A kind of integrated conduct method and device of the chloride organic exhaust gas of high concentration |
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| CN110921718A (en) * | 2018-09-18 | 2020-03-27 | 旭化成株式会社 | Method for producing hydroxide and method for producing positive electrode active material |
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