CN108314149B - Method for integrating desulfurization wastewater electrolysis and product denitration - Google Patents
Method for integrating desulfurization wastewater electrolysis and product denitration Download PDFInfo
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- CN108314149B CN108314149B CN201810171586.6A CN201810171586A CN108314149B CN 108314149 B CN108314149 B CN 108314149B CN 201810171586 A CN201810171586 A CN 201810171586A CN 108314149 B CN108314149 B CN 108314149B
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/463—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrocoagulation
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/54—Nitrogen compounds
- B01D53/56—Nitrogen oxides
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/77—Liquid phase processes
- B01D53/78—Liquid phase processes with gas-liquid contact
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/467—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction
- C02F1/4672—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction by electrooxydation
- C02F1/4674—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction by electrooxydation with halogen or compound of halogens, e.g. chlorine, bromine
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
Abstract
The invention discloses a method for integrating electrolysis of desulfurization wastewater and denitration of products thereof, which utilizes a Ti-based oxide coating or a modified coating plate thereof as a dimensionally stable electrode, and a traditional aluminum/iron polar plate as a soluble electrode to form an electrochemical reactor together with a metal cathode, wherein when pollutants such as heavy metal, solid suspended matters and the like in the desulfurization wastewater are electroflocculated, chloride ions rich in the desulfurization wastewater are used as a chlorine source to generate the counter gas NO in flue gasxHypochlorous acid with strong oxidizing power for oxidizing NO insoluble in water in flue gas into soluble NO2And removed. Thereby achieving the multiple purposes of degrading the desulfurization waste water pollutant generated by the desulfurization process of the coal-fired boiler and removing the NO in the flue gas of the coal-fired boiler.
Description
Technical Field
The invention relates to tail end desulfurization waste water and tail gas NO of a coal-fired boiler flue gas purification processxThe technical field of comprehensive treatment.
Background
A great deal of dust and SO are generated in the use process of the coal-fired boiler2、NOxAnd the like gaseous contaminants. At present, the limestone-gypsum method is generally adopted in industry to better remove SO in coal-fired boiler flue gas2And NO in the flue gasxRemoval is achieved primarily by Selective Catalytic Reduction (SCR) and selective non-catalytic reduction (SNCR). The limestone-gypsum method has a disadvantage of generating a large amount of desulfurized wastewater in which the concentrations of Suspended Solids (SS), heavy metals and calcium, magnesium, chlorine plasma are high. The effluent quality of the traditional triple-box process for treating the desulfurization wastewater is unstable, a large amount of medicament needs to be added, the sludge production amount and the occupied area are large, the chloride ion degradation rate is very low, and certain harm can be caused to the environment if the wastewater is directly discharged. On the other hand, the SCR method has the defects of easy inactivation of the catalyst, narrow operating temperature range, ammonia leakage, high investment cost and the like; the SNCR method also has disadvantages of low denitration efficiency, high operation temperature, ammonia leakage, and the like. NO developed in recent yearsxThe oxidation wet absorption technology has the advantages of relatively simple process, low requirement on temperature and obviously reduced investment and operation cost. However, with ozoneNO represented by potassium permanganate, hydrogen peroxide and hypochlorous acidxStrong oxidizers have limited application due to their ubiquitous source, high energy consumption and high cost.
Disclosure of Invention
The invention aims to form an electrochemical reaction tank with the synergistic effect of electrocoagulation and electrocatalytic oxidation by utilizing the characteristics of high selectivity chlorine evolution, corrosion resistance and high activity of a dimensionally stable electrode and a traditional soluble sacrificial electrode Al or Fe. Through the electric flocculation, on one hand, pollutants such as heavy metal ions, suspended matters, Chemical Oxygen Demand (COD) and the like in the desulfurization wastewater are removed, and meanwhile, chloride ions in the desulfurization wastewater are separated out on a dimensionally stable electrode to generate NO in the flue gasxAlso available chlorine species such as hypochlorite, which have oxidizing power. The technology provides NO by taking the desulfurization wastewater as a chlorine source while carrying out electric flocculation treatment on various pollutants in the desulfurization wastewaterxStrong oxidant required by oxidation wet absorption technology so as to realize the desulfurization of waste water and flue gas NO of end product of coal-fired boilerxThe comprehensive synergistic removal of (1).
The purpose of the invention is realized by the following technical scheme: takes dimensionally stable electrodes (such as Ti-based oxide coating and modified coating plates thereof) with excellent performances in corrosion resistance, stability, electrocatalytic activity and the like as anodes, metal cathodes, and a plurality of Al plates or Fe plates are arranged between the cathodes and the anodes to be taken as soluble electrodes, thus forming the high-efficiency electrochemical reactor for treating the desulfurization wastewater. The desulfurization waste water after electrochemical treatment contains hypochlorite with a certain concentration, and is pumped into a spray tower through a high-pressure pump after air floatation, flocculation, precipitation and filtration, and the hypochlorite and the NO-containing wastewater are mixed from top to bottom through a self-nozzlexReverse contact of flue gas from top to bottom, NOxCan be fully absorbed and removed.
The effective area of the polar plate is 90cm2The above. A plurality of aluminum plates or iron plates are used as induction polar plates and are arranged between a cathode and an anode, the distance between the polar plates is 3-10 mm, the first polar plate and the last polar plate are connected with a positive pole and a negative pole of a switch direct current power supply, and a water sample in an electrolytic bath is uniformly stirred by a magnetic stirrer. Electrolyzing under the condition of constant current, and exchanging the polarity of a power supply every 15-20 min to prevent the electrode plate from being passivated.
In the specific technical method, the dimensionally stable electrode can adopt commercially available Ti/IrO2、Ti/RuO2、Ti/IrO2-RuO2And the prepared Ti/XO (X = Ir, Ru, Pt, Sn, Sb, Pb, Ce, Co and other metal oxide multi-element doped) material, and the metal electrode can adopt stainless steel, copper, white iron and the like.
In the electrochemical reactor with the above specification, the desulfurization wastewater enters from the bottom of the electrochemical reactor with the above specification at a flow rate of 40-60 ml/min, overflows under the condition of ensuring the effective area of the polar plate, and enters the sedimentation tank through the baffle plate.
The treated desulfurization wastewater is precipitated in a precipitation tank, the supernatant passes through a filter screen and a high-pressure pump and is pumped into a spray tower and NO in the flue gasxAnd fully contacting.
The volume ratio of the sedimentation tank to the electrochemical reaction tank is not less than 1.5:1, the diameter (phi) of the spray tower is 5cm, and the height (H) of the spray tower is 20 cm.
The voltage applied by the DC power supply is 20-60V, and the current is 1-5.4A, preferably 4-5.4A. The electrochemical action lasts for 25-60 min.
The flow rate of the desulfurization wastewater pumped by the high-pressure pump is 40-60 mL/min, the flue gas at the temperature of 100-150 ℃ is introduced into the spray tower, the flow rate is 100-200 mL/min, and the preferred flue gas temperature is 100-140 ℃.
In the invention, the pH environment of the desulfurization wastewater is 6-8.
The method has the advantages that the desulfurization waste water rich in chloride ions is used as a chlorine source, solid suspended matters, heavy metals and COD in the desulfurization waste water are degraded through an electrochemical treatment method, and meanwhile, chlorite containing the generated by electrolysis is sprayed into a spray tower and contains NOxThe flue gas is contacted and oxidized and absorbed, so that the pollutants in the desulfurization wastewater are degraded, and simultaneously, the NO in the flue gas is purifiedxThe purpose of (1). The technology provides a new path for comprehensive treatment of waste water and waste gas at the tail end of the coal-fired boiler.
Drawings
FIG. 1 is a schematic diagram of the electrochemical treatment of desulfurization wastewater and its product denitration system.
In the figure: 1-inlet of desulfurization waste water, 2-direct current power supply, 3-scum, 4-sedimentation tank, 5-sludge, 6-electrochemical tank, 7-flotation tank, 8-filter, 9-delivery pump of electrolysis desulfurization waste water, 10-spray tower, 11-liquid storage cabinet, 13-circulating pump of washing liquid, 14-raw flue gas and 15-clean flue gas.
Detailed Description
The process of the present invention is described in further detail below by varying the electrolysis conditions, the denitration temperature, the gas-liquid ratio, and the gas-liquid contact manner.
Example 1:
charging 2L of desulfurized wastewater having pH = 6-8 into an electrochemical reactor having a volume of 200mm × 150mm × 100mm (length × width × height), with Ti/RuO of 100mm × 100mm × 0.15mm (length × width × thickness)2Is an anode plate, a stainless steel plate is a cathode, 3mm is taken as a space, and 5 aluminum plates with the thickness of 0.15mm are placed as soluble electrodes. Continuously introducing the desulfurization wastewater at a flow rate of 40-60 ml/min, respectively connecting the polar plates with the positive electrode and the negative electrode of a direct-current power supply, electrifying, and carrying out electrochemical treatment on the desulfurization wastewater for 60min under the conditions of about 30V of voltage and 4A of constant current. Pumping the treated desulfurization wastewater into a spray tower (phi =5cm, H =20 cm) at a flow rate of 40-60 ml/min, wherein the flow rate of the flue gas is 100ml/min at a flue gas temperature of 110 ℃, and the flow rate of NO-N2The denitration efficiency reaches 47.8 percent under the condition of simulating the NO content in the flue gas to be 800 ppm. The highest removal rate of suspended solid in the desulfurization wastewater is 81.4 percent, the highest removal rates of heavy metals Zn and Ni are 84.2 percent and 80.3 percent, and the highest removal rate of COD is 87.6 percent.
Example 2:
charging 2L of desulfurized wastewater having pH = 6-8 into an electrochemical reactor having a volume of 200mm × 150mm × 100mm (length × width × height), and charging Ti/IrO in an amount of 100mm × 100mm × 0.15mm (length × width × thickness)2The anode plate is a copper plate, the cathode plate is a copper plate, 6mm is taken as a distance, and 3 aluminum plates with the thickness of 0.15mm are placed as soluble electrodes. Continuously introducing the desulfurization wastewater at a flow rate of 40-60 ml/min, respectively connecting the polar plates with the positive electrode and the negative electrode of a direct current power supply, electrifying, and carrying out electrochemical treatment on the desulfurization wastewater for 40min under the conditions of about 20V of voltage and 1A of constant current. Pumping the treated desulfurization wastewater into a spray tower (phi =5cm, H =20 cm) at a flow rate of 40-60 ml/min, wherein the flow rate of the flue gas is 150ml/min at a flue gas temperature of 100 ℃, and the flow rate of NO-N2Simulating NO content in flue gas 8The denitration efficiency reaches 60.5% under the condition of 00 ppm. The highest removal rate of suspended solid in the desulfurization wastewater is 85.8 percent, the highest removal rates of heavy metal Zn and Ni are 86.7 percent and 83.6 percent, and the highest removal rate of COD is 88.2 percent.
Example 3:
charging 2L of desulfurized wastewater having pH = 6-8 into an electrochemical reactor having a volume of 200mm × 150mm × 100mm (length × width × height), and charging Ti/IrO in an amount of 100mm × 100mm × 0.15mm (length × width × thickness)2-RuO2Is an anode plate, a white iron plate is a cathode, and 5 aluminum plates with the thickness of 0.15mm are placed at intervals of 10mm to be soluble electrodes. Continuously introducing the desulfurization wastewater at a flow rate of 40-60 ml/min, respectively connecting the polar plates with the positive electrode and the negative electrode of a direct current power supply, electrifying, and carrying out electrochemical treatment on the desulfurization wastewater for 25min under the conditions of about 60V of voltage and 5.4A of constant current. Pumping the treated desulfurization wastewater into a spray tower (phi =5cm, H =20 cm) at a flow rate of 40-60 ml/min, wherein the flow rate of the flue gas is 200ml/min at a flue gas temperature of 140 ℃, and the flow rate of NO-N2The denitration efficiency reaches 68.3 percent under the condition of simulating the NO content in the flue gas to be 800 ppm. The highest removal rate of suspended solid in the desulfurization wastewater is 88.6 percent, the highest removal rates of heavy metals Zn and Ni are 89.5 percent and 85.2 percent, and the highest removal rate of COD is 84.2 percent.
Example 4:
charging 2L of desulfurized wastewater having pH = 6-8 into an electrochemical reactor having a volume of 200mm × 150mm × 100mm (length × width × height), with Ti/RuO of 100mm × 100mm × 0.15mm (length × width × thickness)2Is a cathode plate, a stainless steel plate is an anode, 3mm is taken as a space, and 5 aluminum plates with the thickness of 0.15mm are placed as soluble electrodes. Continuously introducing the desulfurization wastewater at a flow rate of 40-60 ml/min, respectively connecting the polar plates with the positive electrode and the negative electrode of a direct-current power supply, electrifying, and carrying out electrochemical treatment on the desulfurization wastewater for 60min under the conditions of about 40V of voltage and 5.0A of constant current. Taking 1L of clear liquid in a sedimentation tank, bubbling and introducing simulated flue gas NO-N with the flue gas temperature of 150 ℃, the flow rate of 100ml/min and the NO content of 800ppm2And the denitration efficiency reaches 74.8 percent.
Claims (5)
1. A method for integrating desulfurization wastewater electrolysis and product denitration is characterized in that: the dimensionally stable electrode and the metal electrode are respectively used for constituting current collection flocculation and electrocatalytic oxidationThe electrode can exchange the polarity of a power supply, and a plurality of Al plate or Fe plate soluble electrodes are arranged between the dimensionally stable electrode and the metal electrode; the dimensionally stable electrode adopts Ti/IrO2、Ti/RuO2、Ti/IrO2-RuO2One of (1); the metal electrode is made of one of stainless steel, copper and white iron;
the method comprises the following specific steps:
(1) continuously introducing desulfurization wastewater at a flow rate of 40-60 mL/min, respectively connecting a polar plate with a positive electrode and a negative electrode of a direct-current power supply, electrifying, carrying out electrochemical treatment on the desulfurization wastewater for 25-60 min under the conditions of a voltage of 20-60V and a constant current of 1-5.4A, wherein the water inlet direction and the water outlet direction are water inlet at the bottom, and the upper layer overflows;
(2) pumping the treated desulfurization wastewater into a spray tower at a flow rate of 40-60 mL/min to be in reverse spray contact with flue gas, or bubbling the treated desulfurization wastewater into the flue gas; the temperature of the introduced flue gas is 100-150 ℃, and the flow rate of the flue gas is 100-200 mL/min.
2. The integrated method for electrolysis of desulfurization waste water and denitration of desulfurization waste water according to claim 1, characterized in that: the distance between the polar plates is 3-10 mm.
3. The integrated method for electrolysis of desulfurization waste water and denitration of desulfurization waste water according to claim 1, characterized in that: and the pH environment of the desulfurization wastewater is 6-8.
4. The integrated method for electrolysis of desulfurization waste water and denitration of desulfurization waste water according to claim 1, characterized in that: the temperature of the flue gas is 100-140 ℃.
5. The integrated method for electrolysis of desulfurization waste water and denitration of desulfurization waste water according to claim 1, characterized in that: the constant current is 4-5.4A.
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| CN111135692A (en) * | 2018-11-05 | 2020-05-12 | 新疆硅基新材料创新中心有限公司 | Method and system for recycling waste slurry obtained by power plant boiler flue gas desulfurization and denitrating power plant boiler flue gas |
| CN111530254A (en) * | 2020-04-17 | 2020-08-14 | 苏州庚泽新材料科技有限公司 | Gas treatment method |
| CN113860645A (en) * | 2021-10-14 | 2021-12-31 | 江苏京源环保股份有限公司 | Method for treating high-concentration degradation-resistant organic wastewater |
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| JPH0839095A (en) * | 1994-08-03 | 1996-02-13 | Japan Organo Co Ltd | Water treatment apparatus |
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