CN117654231A - Three-dimensional electrode reactor and method for treating chlorobenzene by cooperation of three-dimensional electrode reactor and persulfate - Google Patents
Three-dimensional electrode reactor and method for treating chlorobenzene by cooperation of three-dimensional electrode reactor and persulfate Download PDFInfo
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- CN117654231A CN117654231A CN202311726779.0A CN202311726779A CN117654231A CN 117654231 A CN117654231 A CN 117654231A CN 202311726779 A CN202311726779 A CN 202311726779A CN 117654231 A CN117654231 A CN 117654231A
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- MVPPADPHJFYWMZ-UHFFFAOYSA-N chlorobenzene Chemical compound ClC1=CC=CC=C1 MVPPADPHJFYWMZ-UHFFFAOYSA-N 0.000 title claims abstract description 108
- 238000000034 method Methods 0.000 title claims abstract description 25
- JRKICGRDRMAZLK-UHFFFAOYSA-L peroxydisulfate Chemical compound [O-]S(=O)(=O)OOS([O-])(=O)=O JRKICGRDRMAZLK-UHFFFAOYSA-L 0.000 title claims abstract description 22
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical group [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 63
- 239000002245 particle Substances 0.000 claims abstract description 50
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims abstract description 46
- 239000003792 electrolyte Substances 0.000 claims abstract description 36
- 239000002912 waste gas Substances 0.000 claims abstract description 31
- 229910003460 diamond Inorganic materials 0.000 claims abstract description 23
- 239000010432 diamond Substances 0.000 claims abstract description 23
- 229910052759 nickel Inorganic materials 0.000 claims abstract description 23
- 238000006243 chemical reaction Methods 0.000 claims abstract description 21
- 238000003487 electrochemical reaction Methods 0.000 claims abstract description 13
- 239000007789 gas Substances 0.000 claims abstract description 13
- 238000005273 aeration Methods 0.000 claims abstract description 7
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical group [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 claims description 18
- 238000001354 calcination Methods 0.000 claims description 15
- 239000002904 solvent Substances 0.000 claims description 15
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 13
- 229910052799 carbon Inorganic materials 0.000 claims description 11
- LCPVQAHEFVXVKT-UHFFFAOYSA-N 2-(2,4-difluorophenoxy)pyridin-3-amine Chemical compound NC1=CC=CN=C1OC1=CC=C(F)C=C1F LCPVQAHEFVXVKT-UHFFFAOYSA-N 0.000 claims description 10
- KBJMLQFLOWQJNF-UHFFFAOYSA-N nickel(ii) nitrate Chemical compound [Ni+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O KBJMLQFLOWQJNF-UHFFFAOYSA-N 0.000 claims description 10
- CHQMHPLRPQMAMX-UHFFFAOYSA-L sodium persulfate Substances [Na+].[Na+].[O-]S(=O)(=O)OOS([O-])(=O)=O CHQMHPLRPQMAMX-UHFFFAOYSA-L 0.000 claims description 10
- 239000011780 sodium chloride Substances 0.000 claims description 9
- 239000000243 solution Substances 0.000 claims description 9
- 238000001027 hydrothermal synthesis Methods 0.000 claims description 8
- 239000011259 mixed solution Substances 0.000 claims description 8
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 7
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 7
- 239000004202 carbamide Substances 0.000 claims description 7
- VGBWDOLBWVJTRZ-UHFFFAOYSA-K cerium(3+);triacetate Chemical compound [Ce+3].CC([O-])=O.CC([O-])=O.CC([O-])=O VGBWDOLBWVJTRZ-UHFFFAOYSA-K 0.000 claims description 7
- UFMZWBIQTDUYBN-UHFFFAOYSA-N cobalt dinitrate Chemical compound [Co+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O UFMZWBIQTDUYBN-UHFFFAOYSA-N 0.000 claims description 7
- 229910001981 cobalt nitrate Inorganic materials 0.000 claims description 7
- 239000006185 dispersion Substances 0.000 claims description 7
- 238000002156 mixing Methods 0.000 claims description 7
- -1 polytetrafluoroethylene Polymers 0.000 claims description 7
- 239000004810 polytetrafluoroethylene Substances 0.000 claims description 7
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims description 7
- 238000002360 preparation method Methods 0.000 claims description 6
- 229910001220 stainless steel Inorganic materials 0.000 claims description 6
- 239000010935 stainless steel Substances 0.000 claims description 6
- 150000001638 boron Chemical class 0.000 claims description 4
- 229910002804 graphite Inorganic materials 0.000 claims description 4
- 239000010439 graphite Substances 0.000 claims description 4
- PMZURENOXWZQFD-UHFFFAOYSA-L Sodium Sulfate Chemical compound [Na+].[Na+].[O-]S([O-])(=O)=O PMZURENOXWZQFD-UHFFFAOYSA-L 0.000 claims description 3
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 3
- 238000007598 dipping method Methods 0.000 claims description 3
- USHAGKDGDHPEEY-UHFFFAOYSA-L potassium persulfate Chemical compound [K+].[K+].[O-]S(=O)(=O)OOS([O-])(=O)=O USHAGKDGDHPEEY-UHFFFAOYSA-L 0.000 claims description 3
- 230000008569 process Effects 0.000 claims description 3
- 238000002791 soaking Methods 0.000 claims description 3
- 229910052938 sodium sulfate Inorganic materials 0.000 claims description 3
- 235000011152 sodium sulphate Nutrition 0.000 claims description 3
- 239000010936 titanium Substances 0.000 claims description 3
- 229910052719 titanium Inorganic materials 0.000 claims description 3
- 238000000746 purification Methods 0.000 abstract description 12
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- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 description 1
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Abstract
The invention provides a three-dimensional electrode reactor and a method for treating chlorobenzene by cooperating with persulfate, and belongs to the technical field of chlorobenzene waste gas treatment. The three-dimensional electrode reactor comprises an air inlet area and a reaction area; the tail end of the air inlet pipe of the air inlet area is provided with a microporous aeration head; the reaction zone is provided with a cathode plate, an anode plate and a three-dimensional particle electrode, wherein the three-dimensional particle electrode is activated carbon particles loaded with nickel cobaltate, and the anode plate is a modified boron-doped diamond electrode; the reaction zone and the gas inlet zone are separated by a porous screen plate. Electrolyte is injected into the three-dimensional electrode reactor, and chlorobenzene waste gas is introduced to carry out electrochemical reaction, so that the chlorobenzene treatment can be realized. According to the invention, the three-dimensional particle electrode and the anode plate are modified, so that the purification efficiency of chlorobenzene waste gas can be greatly improved.
Description
Technical Field
The invention relates to the technical field of chlorobenzene waste gas treatment, in particular to a three-dimensional electrode reactor and a method for treating chlorobenzene by cooperating with persulfate.
Background
Chlorobenzene is an important chemical raw material and is widely applied to the fields of dyes, medicines, rubber, coatings and the like, but has strong toxicity and toxic action on nervous systems and internal organs of human bodies. The human body is exposed to the environment polluted by chlorobenzene compounds, and can absorb the chlorobenzene compounds through inhalation, ingestion and skin, thereby affecting the central nervous system, having irritation to skin and mucous membrane, and causing anesthesia symptoms and even coma due to high-concentration contact.
Current methods for treating chlorobenzene waste gas include adsorption, catalytic combustion, biological methods, and the like. However, the adsorption method is not used for eliminating pollution, and the adsorption capacity of the adsorbent has a certain limit, and the adsorbent needs to be replaced frequently, so that the cost for treating chlorobenzene by the adsorption method is high. The catalytic combustion treatment of chlorobenzene waste gas has high energy consumption, and the tail gas purification device is required to be arranged, so that secondary pollution is very easy to cause. The biological method is adopted to treat the chlorobenzene for a longer period, the chlorobenzene is toxic to microorganisms, and the culture and breeding of strains are very difficult.
The electrochemical activation persulfate process is an emerging organic waste gas treatment technology that combines the principles of electrochemical and chemical reactions. The method utilizes active species generated by electrochemical reaction to oxidize organic matters in the organic waste gas, thereby reducing the concentration of the organic matters in the waste gas and realizing environmental protection. The electrochemical oxidation method is divided into a traditional two-dimensional electrode method and a three-dimensional electrode method, and the traditional two-dimensional electrode method has the problems of high resistance, low conductivity, low current efficiency and poor stability when organic waste gas is treated, so that the purification efficiency of the organic waste gas is low. The three-dimensional electrode advanced oxidation technology has the advantages of high mass transfer efficiency, high current transmission efficiency and the like. Therefore, the research on a three-dimensional electrode reactor is of great significance in the treatment of chlorobenzene waste gas.
Disclosure of Invention
The invention aims to provide a three-dimensional electrode reactor and a method for processing chlorobenzene by cooperating with persulfate, so as to solve the problem of low purification efficiency of the electrochemical activation persulfate to process chlorobenzene waste gas in the prior art.
In order to achieve the above object, the present invention provides the following technical solutions:
the invention provides a three-dimensional electrode reactor, which comprises an air inlet area and a reaction area; the tail end of the air inlet pipe of the air inlet area is provided with a microporous aeration head; the reaction zone is provided with a cathode plate, an anode plate and a three-dimensional particle electrode, wherein the three-dimensional particle electrode is activated carbon particles loaded with nickel cobaltate, and the anode plate is a modified boron-doped diamond electrode; the reaction zone and the gas inlet zone are separated by a porous screen plate.
Preferably, the cathode plate is a titanium plate electrode, a graphite electrode, a stainless steel electrode or a carbon felt electrode; the spacing between the cathode plate and the anode plate is 3.0-5.0 cm.
Preferably, the preparation method of the nickel cobaltate-loaded activated carbon particles comprises the following steps:
(1) Mixing nickel nitrate, cobalt nitrate, urea and a solvent to obtain a mixed solution;
(2) And (3) immersing the activated carbon particles in the mixed solution, and then sequentially carrying out hydrothermal reaction and calcination treatment to obtain the nickel cobaltate-loaded activated carbon particles.
Preferably, in the step (1), the molar ratio of nickel nitrate, cobalt nitrate and urea is 1 to 3:2 to 6: 15-30; the molar volume ratio of the nickel nitrate to the solvent is 1-3 mmol: 50-80 mL; the solvent is formed by mixing water and absolute ethyl alcohol, wherein the volume ratio of the water to the absolute ethyl alcohol is 1:1 to 5.
Preferably, the mass volume ratio of the activated carbon particles to the solvent is 1g: 50-80 mL; the soaking time is 4-6 hours; the temperature of the hydrothermal reaction is 100-120 ℃ and the time is 8-12 h; the temperature of the calcination treatment is 400-500 ℃, and the time of the calcination treatment is 3-5 h.
Preferably, the preparation method of the modified boron-doped diamond electrode comprises the following steps: and sequentially dipping the boron-doped diamond electrode in cerium acetate solution and polytetrafluoroethylene dispersion, and calcining to obtain the modified boron-doped diamond electrode.
The invention also provides a method for treating chlorobenzene by using the three-dimensional electrode reactor, which comprises the following steps: electrolyte and persulfate are added into a three-dimensional electrode reactor, and chlorobenzene waste gas is introduced to carry out electrochemical reaction.
Preferably, the electrolyte consists of an electrolyte and water; in the electrolyte, the concentration of the electrolyte is 0.05-0.30 mol/L; after electrolyte and persulfate are added into a three-dimensional electrode reactor, the concentration of the persulfate is 1.0-4.0 mmol/L; the mass volume ratio of the active carbon particles loaded with nickel cobaltate to the electrolyte in the three-dimensional electrode reactor is 50-150 g:1L.
Preferably, the electrolyte is sodium chloride or sodium sulfate; the persulfate comprises sodium persulfate and/or potassium persulfate.
Preferably, the concentration of chlorobenzene in the chlorobenzene waste gas is 2-8 g/m 3 The method comprises the steps of carrying out a first treatment on the surface of the The flow of the chlorobenzene waste gas is 0.1-0.6L/min; the current of the electrochemical reaction is 0.2-1.8A.
The invention has the beneficial effects that:
(1) According to the three-dimensional electrode reactor provided by the invention, the three-dimensional particle electrode adopts the activated carbon particles loaded with nickel cobaltate, the anode plate is the modified boron-doped diamond electrode, chlorobenzene is treated by adopting the three-dimensional electrode reactor, electrolyte consisting of persulfate, electrolyte and water is added for electrochemical reaction, and more high-activity sulfate radical and hydroxyl radical can be generated in the reaction process through the synergistic effect of the modified diamond electrode and the three-dimensional particle electrode loaded with the activated carbon particles of nickel cobaltate, so that the purification efficiency of the chlorobenzene is obviously improved.
(2) The invention utilizes the three-dimensional electrode reactor, and can improve the purification efficiency of chlorobenzene to 99.23% by adjusting the concentration of electrolyte in electrolyte, the distance between a cathode plate and an anode plate, the addition amount of three-dimensional particle electrodes and current.
Drawings
Fig. 1 is a schematic diagram of a three-dimensional electrode reactor and an external power supply according to the present invention, wherein 1 is an air inlet zone, 2 is a reaction zone, 3 is a cathode plate, 4 is an anode plate, 5 is a three-dimensional particle electrode, 6 is a microporous aeration head, 7 is an air inlet pipe, 8 is a porous screen plate, and 9 is an external power supply.
Detailed Description
The invention provides a three-dimensional electrode reactor, which comprises an air inlet area and a reaction area; the tail end of the air inlet pipe of the air inlet area is provided with a microporous aeration head; the reaction zone is provided with a cathode plate, an anode plate and a three-dimensional particle electrode, wherein the three-dimensional particle electrode is activated carbon particles loaded with nickel cobaltate, and the anode plate is a modified boron-doped diamond electrode; the reaction zone and the gas inlet zone are separated by a porous screen plate.
In the invention, the three-dimensional electrode reactor is made of organic glass, and has the dimensions of 120.0mm long, 120.0mm wide and 300.0mm high; when the three-dimensional electrode reactor is used, the cathode plate and the anode plate are connected with a direct current power supply through the electrode clamps.
In the invention, the cathode plate is a titanium plate electrode, a graphite electrode, a stainless steel electrode or a carbon felt electrode, preferably a graphite electrode or a stainless steel electrode, and more preferably a stainless steel electrode; the spacing between the cathode plate and the anode plate is 3.0 to 5.0cm, preferably 3.5 to 4.5cm, and more preferably 4.0cm.
In the invention, the preparation method of the nickel cobaltate-loaded activated carbon particles comprises the following steps:
(1) Mixing nickel nitrate, cobalt nitrate, urea and a solvent to obtain a mixed solution;
(2) And (3) immersing the activated carbon particles in the mixed solution, and then sequentially carrying out hydrothermal reaction and calcination treatment to obtain the nickel cobaltate-loaded activated carbon particles.
In the present invention, in the step (1), the molar ratio of nickel nitrate, cobalt nitrate and urea is 1 to 3:2 to 6:15 to 30, preferably 2:3 to 5:20 to 25, more preferably 2:4:25, a step of selecting a specific type of material; the molar volume ratio of the nickel nitrate to the solvent is 1-3 mmol: 50-80 mL, preferably 2mmol: 60-70 mL; the solvent is formed by mixing water and absolute ethyl alcohol, wherein the volume ratio of the water to the absolute ethyl alcohol is 1:1 to 5, preferably 1:2 to 4, more preferably 1:3.
In the invention, the mass volume ratio of the activated carbon particles to the solvent is 1g:50 to 80mL, preferably 1g: 60-70 mL; the time of the soaking is 4-6 hours, preferably 5 hours; the temperature of the hydrothermal reaction is 100-120 ℃, preferably 110 ℃, and the time is 8-12 h, preferably 9-11 h, and more preferably 10h; the temperature of the calcination treatment is 400-500 ℃, preferably 450 ℃; the calcination treatment time is 3 to 5 hours, preferably 4 hours.
In the invention, the preparation method of the modified boron-doped diamond electrode comprises the following steps: and sequentially dipping the boron-doped diamond electrode in cerium acetate solution and polytetrafluoroethylene dispersion, and calcining to obtain the modified boron-doped diamond electrode.
In the present invention, the concentration of the cerium acetate solution is 0.1 to 0.8mol/L, preferably 0.2 to 0.7mol/L, and more preferably 0.3 to 0.6mol/L; the mass concentration of the polytetrafluoroethylene dispersion is 1-4%, preferably 2-3%.
In the present invention, the time of immersion in the cerium acetate solution or polytetrafluoroethylene dispersion is independently 15 to 25 minutes, preferably 18 to 22 minutes, and more preferably 20 minutes.
In the present invention, the boron doped diamond electrode is preferably dried after the completion of the impregnation in the cerium acetate solution and after the completion of the impregnation in the polytetrafluoroethylene dispersion, and the drying temperature is independently 80 to 120 ℃, preferably 90 to 110 ℃, further preferably 100 ℃, and the drying time is independently 1 to 2 hours, preferably 1.5 hours.
In the present invention, the temperature of the calcination is 200 to 300 ℃, preferably 220 to 280 ℃, and more preferably 240 to 260 ℃; the calcination time is 10 to 20 minutes, preferably 15 minutes.
The invention also provides a method for treating chlorobenzene by using the three-dimensional electrode reactor, which comprises the following steps: electrolyte and persulfate are added into a three-dimensional electrode reactor, and chlorobenzene waste gas is introduced to carry out electrochemical reaction.
In the present invention, the electrolyte consists of an electrolyte and water; the concentration of the electrolyte in the electrolyte is 0.05 to 0.30mol/L, preferably 0.10 to 0.25mol/L, and more preferably 0.15 to 0.20mol/L; after the electrolyte and the persulfate are added into the three-dimensional electrode reactor, the concentration of the persulfate is 1.0-4.0 mmol/L, preferably 1.5-3.5 mmol/L, and more preferably 2.0-3.0 mmol/L; the mass volume ratio of the active carbon particles loaded with nickel cobaltate to the electrolyte in the three-dimensional electrode reactor is 50-150 g:1L, preferably 80 to 120g:1L, more preferably 100g:1L.
In the present invention, the electrolyte is sodium chloride or sodium sulfate, preferably sodium chloride; the persulfate comprises sodium persulfate and/or potassium persulfate, preferably sodium persulfate.
In the invention, the concentration of chlorobenzene in the chlorobenzene waste gas is 2-8 g/m 3 Preferably 3 to 7g/m 3 More preferably 4 to 6g/m 3 The method comprises the steps of carrying out a first treatment on the surface of the The flow rate of the chlorobenzene waste gas is 0.1-0.6L/min, preferably 0.2-0.5L/min, and more preferably 0.3-0.4L/min; the current of the electrochemical reaction is 0.2 to 1.8A, preferably 0.4 to 1.5A, and more preferably 1A.
The technical solutions provided by the present invention are described in detail below with reference to examples, but they should not be construed as limiting the scope of the present invention.
Example 1
Mixing 20mmol of nickel nitrate, 40mmol of cobalt nitrate, 250mmol of urea and 700mL of solvent (deionized water and absolute ethyl alcohol are mixed according to the volume ratio of 1:3) to obtain a mixed solution; and immersing 10g of active carbon particles in the mixed solution for 5 hours, carrying out hydrothermal reaction at 110 ℃ for 10 hours, finally calcining the product of the hydrothermal reaction at 400 ℃ for 4 hours, and cooling the calcined product to room temperature to obtain the active carbon particles loaded with nickel cobaltate.
Preparation of modified boron-doped diamond electrode: the boron-doped diamond electrode is firstly immersed in cerium acetate solution (water is used as a solvent) with the concentration of 0.5mol/L for 15min, taken out, dried at the temperature of 100 ℃ for 1.5h, then immersed in polytetrafluoroethylene dispersion (water is used as a solvent) with the mass concentration of 2% for 20min, taken out, dried at the temperature of 100 ℃ for 1.5h, and finally calcined at the temperature of 250 ℃ for 15min, thus obtaining the modified boron-doped diamond electrode.
The three-dimensional electrode reactor comprises an air inlet area and a reaction area; the end of the air inlet pipe of the air inlet area is provided with a microporous aeration head, the reaction area is provided with a cathode plate, an anode plate and active carbon particles loaded with nickel cobaltate, the cathode plate is a stainless steel electrode, the anode plate is a modified boron doped diamond electrode, the cathode plate and the anode plate are respectively a sheet electrode with the thickness of 10.0cm multiplied by 2mm, the reaction area and the air inlet area are separated by a porous screen plate (made of sand core glass and provided with a pore of 1 mm), the distance between the anode plate and the cathode plate is 3.0cm, and the active carbon particles loaded with nickel cobaltate are arranged between the anode plate and the cathode plate and are contacted with the anode plate and the cathode plate.
Example 2
The difference from example 1 is that the distance between the anode plate and the cathode plate is 4.0cm, and the other conditions are the same.
Example 3
The difference from example 1 is that the distance between the anode plate and the cathode plate is 5.0cm, and the other conditions are the same.
Comparative example 1
The difference from example 1 is that the anode plate uses an unmodified boron doped diamond electrode, all other conditions being identical.
Comparative example 2
The difference from example 1 is that the three-dimensional particle electrode is an activated carbon particle, and the other conditions are the same.
Comparative example 3
The difference from example 1 is that the anode plate uses an unmodified boron doped diamond electrode, the three-dimensional particle electrode is activated carbon particles, and the other conditions are the same.
Chlorobenzene waste gas was treated by using the three-dimensional electrode reactors of examples 1 to 3 and comparative examples 1 to 3, and the inlet concentration and the outlet concentration of chlorobenzene waste gas were measured, according to the formula re= (C) in -C out )/C in 100% calculation, wherein: RE-purification efficiency (%), C in Chlorobenzene waste gas inlet concentration (mg/m) 3 )，C out Chlorobenzene waste gas outlet concentration (mg/m) 3 )。
Application example 1
1.8L of electrolyte (the concentration of sodium chloride in the electrolyte is 0.05 mol/L) and sodium persulfate are respectively injected into the three-dimensional electrode reactors of the examples 1-3 and the comparative examples 1-3, so that the concentration of the sodium persulfate is 3.0mmol/L after the electrolyte and the sodium persulfate are uniformly mixed, the addition amount of the nickel cobaltate-loaded active carbon particles is 90g, and the concentration of the introduced chlorobenzene is 5g/m 3 The flow of the chlorobenzene waste gas is 0.4L/min, a direct current power supply is connected, the current is controlled to be 1A, the electrochemical reaction is carried out for 50min, the concentration of chlorobenzene in the outlet gas is measured, and the purification efficiency is calculated.
Application example 2
1.8L of electrolyte (the concentration of sodium chloride in the electrolyte is 0.10 mol/L) and sodium persulfate are added into the three-dimensional electrode reactor of the embodiment 2, the concentration of the sodium persulfate is 3.0mmol/L after the electrolyte and the sodium persulfate are uniformly mixed, the addition amount of the activated carbon particles loaded with nickel cobaltate is 90g, and the concentration of chlorobenzene is introduced into the reactor is 5g/m 3 The flow of the chlorobenzene waste gas is 0.4L/min, a direct current power supply is connected, the current is controlled to be 1A, the electrochemical reaction is carried out for 50min, the concentration of chlorobenzene in the outlet gas is measured, and the purification efficiency is calculated.
Application example 3
The difference from application example 2 is that the concentration of sodium chloride is 0.15mol/L, and the other conditions are the same.
Application example 4
The difference from application example 2 is that the concentration of sodium chloride is 0.20mol/L, and the other conditions are the same.
Application example 5
The difference from application example 2 is that the concentration of sodium chloride is 0.30mol/L, and the other conditions are the same.
Application example 6
The difference from application example 2 was that the amount of the nickel cobaltate-supported activated carbon particles added was 150g, and the other conditions were the same.
Application example 7
The difference from application example 2 was that the addition amount of the nickel cobaltate-supported activated carbon particles was 200g, and the other conditions were the same.
The purification efficiency of the p-chlorobenzene waste gas in each application example is shown in Table 1.
Table 1 application examples 1 to 7 purification efficiency of P-chlorobenzene waste gas
The calculation formula of the required energy consumption of the three-dimensional electrode reactor is as follows: e (E) sp ＝UI/{(C in -C out ) Q }; wherein E is sp Energy consumption (kW.h/kg), U-cell voltage (V), I-cell current (mA), C in Chlorobenzene waste gas inlet concentration (kg/m) 3 )，C out Chlorobenzene waste gas outlet concentration (kg/m) 3 ) Q-gas flow (m) 3 /h)。
Application example 8
The difference from application example 2 is that the current is controlled to 0.2A, and the other conditions are the same.
Application example 9
The difference from application example 2 is that the current is controlled to 0.4A, and the other conditions are the same.
Application example 10
The difference from application example 2 is that the current is controlled to 2A, and the other conditions are the same.
Application example 11
The difference from application example 2 is that the current is controlled to 3A, and the other conditions are the same.
The energy consumption of the three-dimensional electrode reactors of application example 2 and application examples 8 to 11 was calculated, and the calculation results were as follows: 172.2 (kW.h)/kg (0.2A)<181.5(kW·h)/kg(0.4A)<190.2(kW·h)/kg(1.0A)<306.3(kW·h)/kg(2.0A)<380.7(kW·h) As can be seen from the results of the treatment of chlorobenzene waste gas with the three-dimensional electrode reactor of the present invention, E was measured at 0.2A, 0.4A and 1.0A sp Substantially the same, but E at 2.0A and 3.0A sp The current is controlled to be 1.0A, which is suitable because of the low energy consumption of 1.0A.
From the above examples, the present invention provides a three-dimensional electrode reactor and a method for treating chlorobenzene by cooperating with persulfate, wherein the three-dimensional electrode reactor comprises an air inlet area and a reaction area; the tail end of the air inlet pipe of the air inlet area is provided with a microporous aeration head; the reaction zone is provided with a cathode plate, an anode plate and a three-dimensional particle electrode, wherein the three-dimensional particle electrode is activated carbon particles loaded with nickel cobaltate, and the anode plate is a modified boron-doped diamond electrode; the reaction zone and the gas inlet zone are separated by a porous screen plate. Electrolyte is injected into the three-dimensional electrode reactor, and chlorobenzene waste gas is introduced to carry out electrochemical reaction, so that the chlorobenzene treatment can be realized. According to the invention, the three-dimensional particle electrode and the anode plate are modified, so that the purification efficiency of chlorobenzene waste gas can be greatly improved.
The foregoing is merely a preferred embodiment of the present invention and it should be noted that modifications and adaptations to those skilled in the art may be made without departing from the principles of the present invention, which are intended to be comprehended within the scope of the present invention.
Claims (10)
1. A three-dimensional electrode reactor, characterized in that the three-dimensional electrode reactor comprises an air inlet zone and a reaction zone; the tail end of the air inlet pipe of the air inlet area is provided with a microporous aeration head; the reaction zone is provided with a cathode plate, an anode plate and a three-dimensional particle electrode, wherein the three-dimensional particle electrode is activated carbon particles loaded with nickel cobaltate, and the anode plate is a modified boron-doped diamond electrode; the reaction zone and the gas inlet zone are separated by a porous screen plate.
2. The three-dimensional electrode reactor according to claim 1, wherein the cathode plate is a titanium plate electrode, a graphite electrode, a stainless steel electrode or a carbon felt electrode; the spacing between the cathode plate and the anode plate is 3.0-5.0 cm.
3. The three-dimensional electrode reactor according to claim 1 or 2, wherein the preparation method of the nickel cobaltate-loaded activated carbon particles comprises the steps of:
(1) Mixing nickel nitrate, cobalt nitrate, urea and a solvent to obtain a mixed solution;
(2) And (3) immersing the activated carbon particles in the mixed solution, and then sequentially carrying out hydrothermal reaction and calcination treatment to obtain the nickel cobaltate-loaded activated carbon particles.
4. The three-dimensional electrode reactor according to claim 3, wherein in the step (1), the molar ratio of nickel nitrate, cobalt nitrate and urea is 1 to 3:2 to 6: 15-30; the molar volume ratio of the nickel nitrate to the solvent is 1-3 mmol: 50-80 mL; the solvent is formed by mixing water and absolute ethyl alcohol, wherein the volume ratio of the water to the absolute ethyl alcohol is 1:1 to 5.
5. The three-dimensional electrode reactor according to claim 4, wherein the mass-to-volume ratio of the activated carbon particles and the solvent is 1g: 50-80 mL; the soaking time is 4-6 hours; the temperature of the hydrothermal reaction is 100-120 ℃ and the time is 8-12 h; the temperature of the calcination treatment is 400-500 ℃, and the time of the calcination treatment is 3-5 h.
6. The three-dimensional electrode reactor according to claim 1 or 2 or 4 or 5, wherein the modified boron doped diamond electrode is prepared by the following steps: and sequentially dipping the boron-doped diamond electrode in cerium acetate solution and polytetrafluoroethylene dispersion, and calcining to obtain the modified boron-doped diamond electrode.
7. A method for treating chlorobenzene by using the three-dimensional electrode reactor according to any one of claims 1 to 6 in combination with persulfate, comprising the steps of: electrolyte and persulfate are added into a three-dimensional electrode reactor, and chlorobenzene waste gas is introduced to carry out electrochemical reaction.
8. The method of claim 7, wherein the electrolyte consists of an electrolyte and water; in the electrolyte, the concentration of the electrolyte is 0.05-0.30 mol/L; after electrolyte and persulfate are added into a three-dimensional electrode reactor, the concentration of the persulfate is 1.0-4.0 mmol/L; the mass volume ratio of the active carbon particles loaded with nickel cobaltate to the electrolyte in the three-dimensional electrode reactor is 50-150 g:1L.
9. The method of claim 8, wherein the electrolyte is sodium chloride or sodium sulfate; the persulfate comprises sodium persulfate and/or potassium persulfate.
10. The process according to claim 8 or 9, wherein the chlorobenzene waste gas has a chlorobenzene concentration of 2 to 8g/m 3 The method comprises the steps of carrying out a first treatment on the surface of the The flow of the chlorobenzene waste gas is 0.1-0.6L/min; the current of the electrochemical reaction is 0.2-1.8A.
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