CN117185436A - Electrodialysis-three-dimensional electrode reaction method for synchronous desalination and pollution reduction of high-salt landfill leachate - Google Patents
Electrodialysis-three-dimensional electrode reaction method for synchronous desalination and pollution reduction of high-salt landfill leachate Download PDFInfo
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- CN117185436A CN117185436A CN202311367542.8A CN202311367542A CN117185436A CN 117185436 A CN117185436 A CN 117185436A CN 202311367542 A CN202311367542 A CN 202311367542A CN 117185436 A CN117185436 A CN 117185436A
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- 238000000034 method Methods 0.000 title claims abstract description 17
- 239000000149 chemical water pollutant Substances 0.000 title claims abstract description 13
- 238000003411 electrode reaction Methods 0.000 title claims abstract description 12
- 238000010612 desalination reaction Methods 0.000 title description 8
- 230000001360 synchronised effect Effects 0.000 title description 6
- 230000009467 reduction Effects 0.000 title description 5
- 241001122767 Theaceae Species 0.000 claims abstract description 34
- 239000002245 particle Substances 0.000 claims abstract description 25
- 238000006243 chemical reaction Methods 0.000 claims abstract description 22
- 230000005291 magnetic effect Effects 0.000 claims abstract description 14
- 238000000909 electrodialysis Methods 0.000 claims abstract description 13
- 238000005273 aeration Methods 0.000 claims abstract description 11
- 239000007772 electrode material Substances 0.000 claims abstract description 6
- 238000011033 desalting Methods 0.000 claims abstract description 4
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 34
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N iron oxide Inorganic materials [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 claims description 20
- 229910052757 nitrogen Inorganic materials 0.000 claims description 17
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 16
- 239000012528 membrane Substances 0.000 claims description 13
- 230000000694 effects Effects 0.000 claims description 10
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 8
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 claims description 8
- 239000008367 deionised water Substances 0.000 claims description 8
- 229910021641 deionized water Inorganic materials 0.000 claims description 8
- 238000010438 heat treatment Methods 0.000 claims description 7
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 5
- 229910052760 oxygen Inorganic materials 0.000 claims description 5
- 239000001301 oxygen Substances 0.000 claims description 5
- 239000004793 Polystyrene Substances 0.000 claims description 4
- HJPBEXZMTWFZHY-UHFFFAOYSA-N [Ti].[Ru].[Ir] Chemical compound [Ti].[Ru].[Ir] HJPBEXZMTWFZHY-UHFFFAOYSA-N 0.000 claims description 4
- 238000004140 cleaning Methods 0.000 claims description 4
- 238000001816 cooling Methods 0.000 claims description 4
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- 239000003014 ion exchange membrane Substances 0.000 claims description 4
- RBTARNINKXHZNM-UHFFFAOYSA-K iron trichloride Chemical compound Cl[Fe](Cl)Cl RBTARNINKXHZNM-UHFFFAOYSA-K 0.000 claims description 4
- 238000002156 mixing Methods 0.000 claims description 4
- NDLPOXTZKUMGOV-UHFFFAOYSA-N oxo(oxoferriooxy)iron hydrate Chemical compound O.O=[Fe]O[Fe]=O NDLPOXTZKUMGOV-UHFFFAOYSA-N 0.000 claims description 4
- 238000007747 plating Methods 0.000 claims description 4
- 229920002223 polystyrene Polymers 0.000 claims description 4
- 230000001105 regulatory effect Effects 0.000 claims description 4
- 239000011780 sodium chloride Substances 0.000 claims description 4
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- 238000001914 filtration Methods 0.000 claims 1
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- 239000002957 persistent organic pollutant Substances 0.000 abstract description 10
- 150000003839 salts Chemical class 0.000 abstract description 9
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Abstract
The invention discloses an electrodialysis-three-dimensional electrode reaction method for synchronously desalting and reducing pollution of high-salt landfill leachate. The invention prepares a magnetic nitrogen-doped biochar particle electrode material by taking tea residues as raw materials, and places the magnetic nitrogen-doped biochar particle electrode material in a concentrated chamber of an electrodialysis reaction tank to construct a three-dimensional electrode reaction system, and the particle electrode is suspended in an aeration mode, so that organic pollutants in the concentrated chamber are degraded by utilizing the electrochemical performance of the particle electrode and the high-salt condition in the concentrated chamber in the electrifying process of a reactor. The electrodialysis-three-dimensional electrode reaction system constructed by the invention can efficiently degrade organic pollutants by utilizing the salt separated in the concentration chamber while separating the salt by electrodialysis, thereby ensuring the recycling utilization efficiency of high-salt organic wastewater.
Description
Technical Field
The invention relates to a synchronous desalination and pollution reduction method for a water body, in particular to an electrodialysis-three-dimensional electrode reaction system for synchronous desalination and pollution reduction of high-salt landfill leachate.
Background
The landfill leachate has certain difficulty in treatment due to the problems of high salt, serious organic pollution and the like. How to desalt landfill leachate and to treat organic pollution in high-salt environment is of great concern. Electrodialysis is a common desalination technology, has the advantage of being capable of being operated at normal temperature and normal pressure, not only avoids energy consumption caused by changing temperature and pressure, but also has low dependence on environmental temperature and moderate degree, and is an environment-friendly and efficient desalination technology. In the electrodialysis reaction tank, anions and cations are alternately arranged to form a plurality of separated reaction tanks. After a certain time, the reaction tank alternately forms a concentrated chamber for gathering anions and cations and a dilute chamber with lower ion concentration. Because the concentration chamber has high salt content, the treatment difficulty of organic pollutants in the subsequent concentration chamber is extremely high. How to utilize the electric energy and the salt in the concentration chamber in the electrodialysis reaction process to construct an electrochemical synchronous degradation system to reduce organic pollutants in the concentration chamber, and has practical value for pollution treatment of high-salt wastewater.
Three-dimensional electrode technology is a very potential electrochemical oxidation technology, which means that particle electrodes are selected to be filled between a cathode and an anode of a reactor on the basis of a traditional two-dimensional electrode. The particle electrode filled in the running process of the reactor has the characteristics of cathode and anode when being charged under the action of the current of an electric field, and forms an independent electrode unit. The reaction area of the traditional two-dimensional electrode is mainly formed on the surfaces of the two-side electrodes, but the three-dimensional electrode technology can expand the reaction area into the whole reactor, so that the utilization rate of the space of the reactor is increased under the condition of not increasing the volume of the reactor, and the reaction efficiency of the whole reactor is improved. The three-dimensional electrode has become a high-efficiency organic pollution repair technology, the water treatment effect is better than that of the two-dimensional electrode, and salt ions in high-salt wastewater can be used as electrolyte to improve the degradation effect of organic pollutants. Therefore, the electrodialysis-three-dimensional electrode electrochemical system constructed by adding the particle electrode into the concentration chamber is beneficial to degrading organic pollutants in the concentration chamber, and can meet the requirement of recycling the high-salt cultivation wastewater.
The biomass charcoal has wide application in the field of particle electrodes, and has the advantages of low price, wide sources, resource waste avoidance and the like. However, the poor treatment effect limits the application of biomass charcoal in three-dimensional electrode systems. The doping of nitrogen can lead the carbon framework to form asymmetric electron defect sites, the electronegativity of nitrogen atoms is larger than that of carbon atoms, electrons are transferred from the carbon atoms to the nitrogen atoms, and the conductivity and the catalytic performance of the particle electrode are improved. At present, the doping mode of the externally added nitrogen source is complex in operation, and the externally added medicament is easy to cause environmental pollution. China is the largest tea producing country worldwide, the annual tea yield can reach 210 ten thousand tons, and the annual tea yield accounts for about 44.7 percent of the world share, wherein more than 90 percent of tea leaves can be discarded after drinking. The tea residue has high carbon content, contains rich cellulose, hemicellulose, lignin and other substances, and can be used as biochar raw material. In addition, the tea slag has high nitrogen content, and the nitrogen doped biochar can be prepared under the condition of no external nitrogen source by utilizing nitrogen elements contained in the tea slag. At present, the ferromagnetic modification is a mode for effectively endowing the biochar with recycling performance, and the magnetic nitrogen-doped tea dreg biochar particle electrode is prepared by utilizing the ferromagnetic modification method, so that the recycling and the reutilization of the particle electrode are facilitated, and the treatment effect of a reaction system can be further improved. The tea dreg biochar is prepared into a magnetic nitrogen doped particle electrode, and the magnetic nitrogen doped particle electrode is placed in an electrodialysis concentration chamber to construct a three-dimensional electrode reaction system, so that the method is a method for effectively and synchronously reducing the salt content and organic pollutants of high-salt landfill leachate.
Disclosure of Invention
In order to solve the problem that organic pollution in a concentration chamber is difficult to remove in the electrodialysis treatment process of high-salt wastewater, the invention provides an electrodialysis-three-dimensional electrode reaction method capable of being used for synchronous desalination and pollution reduction of high-salt organic wastewater.
The technical scheme adopted by the invention is as follows.
The invention provides an electrodialysis-three-dimensional electrode reaction method for synchronously desalting and reducing pollution of high-salt landfill leachate, which comprises the following specific steps:
(1) Placing the tea residue in a tube furnace, and heating 1. 1 h in nitrogen environment at 400-600deg.C to obtain biochar.
(2) Mixing the tea dreg biochar in the step (1) with KOH in a ratio of 1:1, heating to 1 h in a nitrogen environment, and setting the temperature at 300-600 ℃. And (3) cleaning the tea residue with ultrapure water for 3 times to obtain the nitrogen-doped tea residue biochar.
(3) Placing the 1 g tea dreg biochar obtained in the step (2), 2 g ferric trichloride and 0.5 g ferric oxide in a 500 mL conical flask, adding 60 mL deionized water, and using 1 mol L -1 The pH was adjusted to 10 to precipitate iron oxide and stirred in a 80℃water bath for 1 h. And (3) standing and cooling to room temperature, respectively washing with ethanol and deionized water for 3 times, washing off the undeposited iron oxide, and drying at 80 ℃ for 24 h to obtain the magnetic tea dreg biochar.
(4) Placing the magnetic biochar 1-10 g obtained in the step (3) in a concentration chamber of an electrodialysis-three-dimensional electrode reactor, wherein the electrodialysis-three-dimensional electrode reactor adopts a membrane stack of 10-20 pairs of membranes, the electrodialysis membrane is made of polystyrene heterogeneous ion exchange membranes, and the effective area is 200-400 cm 2 The electrode materials at the two ends are ruthenium iridium titanium plating plate electrodes, and the flow rate of garbage leachate entering water is regulated to be 1-10L h -1 The reaction voltage is 5-20V, and the NaCl concentration is 10-30 g L -1 。
(5) The concentrated chamber is aerated to suspend the particle electrode, so as to avoid the particle electrode from sinking, and the aeration rate is 10-20L min -1 Aeration can also increase the oxygen content in the solution to improve the treatment effect.
Compared with the prior art, the invention has the beneficial effects that: according to the electrodialysis-three-dimensional electrode reaction method, the particle electrode is added into the electrodialysis concentration chamber, so that the salt of the concentration chamber and the electric energy of the electrodialysis desalination process can be utilized to synchronously reduce organic pollutants, the electric energy is saved, and the recycling of the water in the concentration chamber is facilitated.
Drawings
FIG. 1 is a schematic diagram of an electrodialysis-three-dimensional electrode reaction system.
FIG. 2 shows the chloride ion removal rate in the dilute chamber of the electrodialysis-three-dimensional electrode reactor for treating high-salt landfill leachate in example 1.
FIG. 3 is a graph showing the change in chemical oxygen demand in the electrodialysis-three-dimensional electrode reactor process high salt landfill leachate concentrating compartment in example 2.
Description of the embodiments
The technical scheme of the invention is described in detail below with reference to the accompanying drawings and examples.
As shown in fig. 1, fig. 1 is a schematic diagram of a reaction system, and landfill leachate enters an electrodialysis-three-dimensional electrode reactor through a peristaltic pump; the concentration chamber in the reactor is a reaction area in which anions and cations continuously enter in the reaction process and the concentration is continuously increased; the dilute chamber in the reactor is a reaction area in which anions and cations continuously flow out in the reaction process and the concentration is continuously reduced; the organic pollutants in the concentration chamber are difficult to treat, so that the particle electrode is added in the concentration chamber; the particle electrode is suspended by aeration in the reaction process, and the treatment effect can be improved.
Example 1
(1) The tea leaves residues are placed in a tube furnace, and heated to 1 h in a nitrogen environment at 500 ℃ to obtain the biochar.
(2) Mixing the tea dreg biochar in the step (1) with KOH in a ratio of 1:1, heating to 1 h in a nitrogen environment, and setting the temperature at 500 ℃. And (3) cleaning the tea residue with ultrapure water for 3 times to obtain the nitrogen-doped tea residue biochar.
(3) Placing the 1 g tea dreg biochar obtained in the step (2), 2 g ferric trichloride and 0.5 g ferric oxide in a 500 mL conical flask, adding 60 mL deionized water, and using 1 mol L -1 The pH was adjusted to 10 to precipitate iron oxide and stirred in a 80℃water bath for 1 h. And (3) standing and cooling to room temperature, respectively washing with ethanol and deionized water for 3 times, washing off the undeposited iron oxide, and drying at 80 ℃ for 24 h to obtain the magnetic tea dreg biochar.
(4) Placing the magnetic biochar obtained in the step (3) in a concentration chamber of an electrodialysis-three-dimensional electrode reactor, wherein the electrodialysis-three-dimensional electrode reactor adopts a membrane stack of 20 pairs of membranes, the electrodialysis membrane is made of polystyrene heterogeneous ion exchange membranes, and the effective area is 400 cm 2 The electrode materials at the two ends are ruthenium iridium titanium plating plate electrodes, and the water flow rate of landfill leachate is regulated to be 1L h -1 The reaction voltage was 5V and the NaCl concentration was 10 g L -1 。
(5) The concentrated chamber is aerated to suspend the particle electrode, so as to avoid the particle electrode from sinking, and the aeration rate is 10L min -1 Aeration can also increase the oxygen content in the solution to improve the treatment effect.
The number of membrane stacks is increased in example 1, so that the desalting rate in the reaction process can be increased, and the method is suitable for a reaction system with higher salt content and low organic pollution degree.
Example 2
(1) The tea slag is placed in a tube furnace and heated to 1 h in a nitrogen environment at 500 ℃ to obtain the biochar.
(2) Mixing the tea dreg biochar in the step (1) with KOH in a ratio of 1:1, heating to 1 h in a nitrogen environment, and setting the temperature at 500 ℃. And (3) cleaning the tea residue with ultrapure water for 3 times to obtain the nitrogen-doped tea residue biochar.
(3) Placing the 1 g tea dreg biochar obtained in the step (2), 2 g ferric trichloride and 0.5 g ferric oxide in a 500 mL conical flask, adding 60 mL deionized water, and using 1 mol L -1 The pH was adjusted to 10 to precipitate iron oxide and stirred in a 80℃water bath for 1 h. And (3) standing and cooling to room temperature, respectively washing with ethanol and deionized water for 3 times, washing off the undeposited iron oxide, and drying at 80 ℃ for 24 h to obtain the magnetic tea dreg biochar.
(4) Placing 10 g of the magnetic biochar obtained in the step (3) in an average manner in a concentration chamber of each electrodialysis-three-dimensional electrode reactor, wherein the electrodialysis-three-dimensional electrode reactor adopts a membrane stack of 10 pairs of membranes, the electrodialysis membrane is made of polystyrene heterogeneous ion exchange membranes, and the effective area is 300 cm 2 The electrode materials at the two ends are ruthenium iridium titanium plating plate electrodes, and the water inlet flow rate is regulated to 3L h -1 The reaction voltage was 10V and the NaCl concentration was 20 g L -1 。
(5) The concentrated chamber is aerated to suspend the particle electrode, so as to avoid the particle electrode from sinking, and the aeration rate is 20L min -1 Aeration can also increase the oxygen content in the solution to improve the treatment effect.
As shown in fig. 2, the rice hull control group is the treatment effect of replacing the rice hull biochar with the magnetic nitrogen-doped tea residue biochar in the concentration chamber; wherein, the preparation conditions of the rice hull are as follows: the heating was performed under nitrogen conditions at 500℃for 2 h. In the embodiment 2, the addition amount and the aeration amount of the particle electrode in the concentration chamber are increased, so that the organic pollutants can be removed in the reaction process, and the method is suitable for high-salt wastewater with serious organic pollution.
The foregoing description of the preferred embodiments of the invention is not intended to limit the invention to the particular embodiments disclosed, but on the contrary, the intention is to cover all modifications, equivalents, and alternatives falling within the spirit and scope of the invention.
Claims (1)
1. An electrodialysis-three-dimensional electrode reaction method for synchronously desalting and reducing pollution of high-salt landfill leachate is characterized by comprising the following specific steps of:
placing tea leaves residues in a tube furnace, and heating 1 to h in a nitrogen environment at 400-600 ℃ to obtain biochar; mixing the prepared tea dreg biochar with KOH in a ratio of 1:1, heating to 1 h in a nitrogen environment, setting the temperature to 300-600 ℃, and cleaning with ultrapure water for 3 times to obtain nitrogen-doped tea dreg biochar; placing 1 g tea residue biochar, 2 g ferric trichloride and 0.5 g ferric oxide in 500 mL conical flask, adding 60 mL deionized water, and using 1 mol L -1 Adjusting the pH to 10 to precipitate iron oxide, and stirring in a water bath at 80 ℃ for 1 h; standing and cooling to room temperature, respectively filtering with ethanol and deionized water for 3 times to remove non-precipitated iron oxide, and drying at 80deg.C for 24 h to obtain magnetic tea residue biochar; placing the magnetic biochar prepared by 1-10 g into a concentrated chamber of an electrodialysis-three-dimensional electrode reactor, wherein the electrodialysis-three-dimensional electrode reactor adopts a membrane stack of 10-20 pairs of membranes, the electrodialysis membrane is made of polystyrene heterogeneous ion exchange membrane, and the effective area is 200-400 cm 2 The electrode materials at the two ends are ruthenium iridium titanium plating plate electrodes, and the flow rate of garbage leachate entering water is regulated to be 1-10L h -1 The reaction voltage is 5-20V, and the NaCl concentration is 10-30 g L -1 The method comprises the steps of carrying out a first treatment on the surface of the The concentrated chamber is aerated to suspend the particle electrode, so as to avoid the particle electrode from sinking, and the aeration rate is 10-20L min -1 Aeration can also increase the oxygen content in the solution to improve the treatment effect.
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