CN113045063A - Water purifying device and method based on self-driven electrochemical Fenton-like flocculation reaction - Google Patents

Water purifying device and method based on self-driven electrochemical Fenton-like flocculation reaction Download PDF

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CN113045063A
CN113045063A CN202110283717.1A CN202110283717A CN113045063A CN 113045063 A CN113045063 A CN 113045063A CN 202110283717 A CN202110283717 A CN 202110283717A CN 113045063 A CN113045063 A CN 113045063A
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water
chamber
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purified
storage chamber
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CN113045063B (en
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张芳
吴玥
李广贺
侯德义
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Tsinghua University
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Tsinghua University
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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
    • C02F9/00—Multistage treatment of water, waste water or sewage
    • 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
    • C02F1/001—Processes for the treatment of water whereby the filtration technique is of importance
    • 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
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/46109—Electrodes
    • 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
    • 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
    • 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
    • C02F1/72—Treatment of water, waste water, or sewage by oxidation
    • C02F1/722—Oxidation by peroxides
    • 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
    • C02F1/72—Treatment of water, waste water, or sewage by oxidation
    • C02F1/725—Treatment of water, waste water, or sewage by oxidation by catalytic oxidation
    • 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
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/46109—Electrodes
    • C02F2001/46133—Electrodes characterised by the material
    • C02F2001/46138—Electrodes comprising a substrate and a coating
    • C02F2001/46142—Catalytic coating
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2101/00—Nature of the contaminant
    • C02F2101/10—Inorganic compounds
    • C02F2101/103—Arsenic compounds
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2305/00—Use of specific compounds during water treatment
    • C02F2305/02—Specific form of oxidant
    • C02F2305/026—Fenton's reagent

Abstract

The invention relates to a water purifying device and a water purifying method based on self-driven electrochemical Fenton-like flocculation reaction. The water purifying device comprises a water storage chamber, an oxygen reduction cathode and an iron anode. The oxygen reduction cathode and the iron anode are arranged in the water storage chamber. The water storage chamber is used for containing water to be purified. The oxygen reduction cathode is electrically connected with the iron anode and is used for contacting with the water body to be purified to generate the following reaction: o is2+2H2O+2e－→H2O2+2OH－. The iron anode is used for contacting with a water body to be purified to generate a reaction comprising the following steps: fe-2e‑→Fe2+. When the water purifying device is used for purifying water, the removal rate of pollutants can be effectively improved. Meanwhile, the water purifier performs self-driven reaction when purifying the water body, does not need external energy sources, and can effectively reduce the energy consumption of water body purification.

Description

Water purifying device and method based on self-driven electrochemical Fenton-like flocculation reaction
Technical Field
The invention relates to the field of water purification, in particular to a water purification device and method based on self-driven electrochemical Fenton-like flocculation reaction.
Background
With the development of industrialization, the problem of water pollution is increasingly severe. Water pollution can have serious adverse effects on human health. In the water treatment process, pollutants dissolved in water, such as metal elements, metalloid elements, organic matters and the like, are often difficult to remove, and the pollutants often have certain toxicity, so that the risk of pathological changes of human organs is increased. Therefore, the purification of water is of great significance. Electrolytic purification is a fast water purification method, which can achieve a certain water purification effect but consumes much energy.
Disclosure of Invention
Therefore, there is a need for a water purification apparatus and method based on self-driven electrochemical fenton-like flocculation reaction, which can effectively reduce energy consumption.
In order to solve the technical problems, the technical scheme of the invention is as follows:
a water purifying device based on self-driven electrochemical Fenton-like flocculation reaction comprises a water storage chamber, an oxygen reduction cathode and an iron anode; the oxygen reduction cathode and the iron anode are arranged in the water storage chamber; the water storage chamber is used for containing water to be purified; the oxygen reduction cathode is electrically connected with the iron anode and is used for contacting with the water body to be purified to generate a reaction comprising the following steps: o is2+2H2O+2e－→H2O2+2OH－(ii) a The iron anode is used for contacting with the water body to be purified to generate the following reaction: fe-2e-→Fe2+。
In one embodiment, the oxygen reduction cathode is capable of floating on the surface of the body of water to be purified.
In one embodiment, the water inlet of the water storage chamber is closer to the bottom of the water storage chamber than the oxygen reduction cathode so that the water to be purified enters the water storage chamber from the lower part of the oxygen reduction cathode.
In one embodiment, the iron anode can sink to the bottom of the body of water to be purified.
In one embodiment, the oxygen reduction cathode is an air cathode.
In one embodiment, the water purification apparatus further comprises a filter chamber; the water inlet of the filtering chamber is connected with the water outlet of the water storage chamber, and the filtering chamber is used for filtering the water outlet of the water storage chamber.
In one embodiment, the filtering chamber is divided into a plurality of sub-filtering chambers; the sub-filtering chambers are distributed in sequence and the filtering degree of each sub-filtering chamber is gradually increased along with the distance from the water storage chamber.
In one embodiment, the filtering chamber is divided into a first sub-filtering chamber, a second sub-filtering chamber, and a third sub-filtering chamber; the first sub-filtering chamber, the second sub-filtering chamber and the third sub-filtering chamber are distributed in sequence along with the distance from the water storage chamber; the volume ratio of the first sub-filtration chamber, the second sub-filtration chamber and the third sub-filtration chamber is (4.5-5.5): (1.5-2.5): 2.5-3.5).
In one embodiment, the first sub-filter chamber is filled with a first filter medium, the second sub-filter chamber is filled with a second filter medium, and the third sub-filter chamber is filled with a third filter medium; the particle size of the first filter medium is 0.1-1 mm, the particle size of the second filter medium is 1-2 mm, and the particle size of the third filter medium is 4-7 mm.
A water purification method based on self-driven electrochemical Fenton-like flocculation reaction adopts the water purification device in any embodiment; the water purification method comprises the following steps:
and adding a water body to be purified into the water storage chamber, so that the oxygen reduction cathode and the iron anode are both in contact with the water body to be purified.
The water purifying device based on the self-driven electrochemical Fenton-like flocculation reaction comprises a water storage chamber, an oxygen reduction cathode and an iron anode. The oxygen reduction cathode and the iron anode are arranged in the water storage chamber. The water storage chamber is used for containing water to be purified. The oxygen reduction cathode is electrically connected with the iron anode and is used for contacting with the water body to be purified to generate the following reaction: o is2+2H2O+2e－→H2O2+2OH－. The iron anode is used for contacting with a water body to be purified to generate a reaction comprising the following steps: fe-2e-→Fe2+. When the water purifying device is used for purifying a water body, a certain amount of hydrogen peroxide and ferrous iron ions are generated in the water storage chamber, and then the Fenton-like reaction is generated, so that the efficient oxidation of pollutants in the water body is realized, and iron hydroxide floccules formed by hydrolyzing the iron ions have a good adsorption effect on the pollutants, so that the removal rate of the pollutants can be effectively improved. Meanwhile, the water purifier performs self-driven reaction when purifying the water body, does not need external energy sources, and can effectively reduce the energy consumption of water body purification.
The water purification method based on the self-driven electrochemical Fenton-like flocculation reaction adopts the water purification device. The water purification method comprises the following steps: and adding the water to be purified into the water storage chamber, so that the oxygen reduction cathode and the iron anode are both in contact with the water to be purified. At this time, reactions including: o is2+2H2O+2e－→H2O2+2OH－(ii) a The iron anode takes place by the following reactions: fe-2e-→Fe2+. Therefore, the water body can be purified in a self-driven reaction mode, and the removal rate of pollutants is improved. Meanwhile, in the water purification method, the self-driven reaction is adopted, external energy sources are not needed, and the energy consumption of water purification can be effectively reduced.
Drawings
Fig. 1 is a schematic structural diagram of a water purification apparatus based on a self-driven electrochemical fenton-like flocculation reaction according to an embodiment of the present invention.
The notation in the figure is:
100. a water purification device based on self-driven electrochemical Fenton-like flocculation reaction; 101. a water storage chamber; 102. an oxygen reduction cathode; 103. an iron anode; 104. a filtering chamber; 1041. a first sub-filtration chamber; 1042. a second sub-filtration chamber; 1043. a third sub-filtration chamber; 105. a secondary filtration chamber; 1051. a first sub-secondary filtration chamber; 1052. a second sub-secondary filtration chamber; 1053. a third sub-secondary filtering chamber; 106. a water outlet of the filter chamber; 107. a water outlet of the secondary filter chamber; 200. an arsenic-containing water.
Detailed Description
The present invention will be described in detail with reference to the following embodiments in order to make the aforementioned objects, features and advantages of the invention more comprehensible. In the following description, numerous specific details are set forth in order to provide a thorough understanding of the present invention. This invention may, however, be embodied in many different forms and should not be construed as limited to the embodiments set forth herein.
In the description of the present invention, it is to be understood that the terms "central," "longitudinal," "lateral," "length," "width," "thickness," "upper," "lower," "front," "rear," "left," "right," "vertical," "horizontal," "top," "bottom," "inner," "outer," "clockwise," "counterclockwise," "axial," "radial," "circumferential," and the like are used in the orientations and positional relationships indicated in the drawings for convenience in describing the invention and to simplify the description, and are not intended to indicate or imply that the referenced device or element must have a particular orientation, be constructed and operated in a particular orientation, and are not to be considered limiting of the invention.
Furthermore, the terms "first", "second" and "first" are used for descriptive purposes only and are not to be construed as indicating or implying relative importance or implicitly indicating the number of technical features indicated. Thus, a feature defined as "first" or "second" may explicitly or implicitly include at least one such feature. In the description of the present invention, "a plurality" means at least two, e.g., two, three, etc., unless specifically limited otherwise.
In the present invention, unless otherwise expressly stated or limited, the terms "mounted," "connected," "secured," and the like are to be construed broadly and can, for example, be fixedly connected, detachably connected, or integrally formed; can be mechanically or electrically connected; they may be directly connected or indirectly connected through intervening media, or they may be connected internally or in any other suitable relationship, unless expressly stated otherwise. The specific meanings of the above terms in the present invention can be understood by those skilled in the art according to specific situations.
Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. The terminology used in the description of the invention herein is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention. As used herein, the term "and/or" includes any and all combinations of one or more of the associated listed items.
Referring to fig. 1, an embodiment of the present invention provides a water purifying apparatus 100 based on self-driven electrochemical fenton-like flocculation reaction. The water purifying device 100 based on the self-driven electrochemical Fenton-like flocculation reaction comprises a water storage chamber 101, an oxygen reduction cathode 102 and an iron anode 103; the oxygen reduction cathode 102 and the iron anode 103 are arranged in the water storage chamber 101; the water storage chamber 101 is used for containing water to be purified; the oxygen reduction cathode 102 is electrically connected with the iron anode 103, and the oxygen reduction cathode 102 is used for contacting with the water body to be purified to generate the following reaction: o is2+2H2O+2e－→H2O2+2OH－(ii) a The iron anode 103 is used for contacting with the water body to be purified to generate the following reactions: fe-2e-→Fe2+。
When the water purifying device in the embodiment is used for purifying a water body, a certain amount of hydrogen peroxide and ferrous iron ions are generated in the water storage chamber 101, and then the Fenton-like reaction is generated, so that the efficient oxidation of pollutants in the water body is realized, and iron hydroxide floccules formed by hydrolyzing the iron ions have a good adsorption effect on the pollutants, so that the removal rate of the pollutants can be effectively improved. Meanwhile, the water purifier performs self-driven reaction when purifying the water body, does not need external energy sources, and can effectively reduce the energy consumption of water body purification.
Specifically, the inventors of the present invention found in the research on the water purification process and the water purification apparatus that, by the combined action of the oxygen reduction cathode 102 and the iron anode 103 which are electrically connected, when in contact with the water body to be purified, there is a potential difference between the oxygen reduction cathode 102 and the iron anode 103, and the theoretical open circuit voltage thereof is 0.730V to 1.263V, so that the reaction is started and continued, and the self-driven reaction in the water storage chamber 101 is realized. When the oxygen reduction cathode 102 is in contact with the body of water to be purified, the oxygen reduction cathode 102 undergoes a reaction comprising: o is2+2H2O+2e－→H2O2+2OH－(ii) a When the iron anode 103 is in contact with the water body to be purified, the iron anode 103 reacts as follows: fe-2e-→Fe2+. At this time, hydrogen peroxide can react with divalent iron ions to excite generation of hydroxyl radicals (. OH) and/or higher valent iron radicals (. Fe (IV)) (H)2O2+Fe2++H+→Fe3++·OH/·Fe(IV)+H2O), the oxidation effect of the pollutants in the water body to be purified is enhanced, and the efficient oxidation of the pollutants in the water body to be purified is realized. Meanwhile, iron hydroxide floccules formed by hydrolyzing iron ions have a good adsorption effect on pollutants, and the removal rate of the pollutants can be effectively improved.
In one particular example, the oxygen reduction cathode 102 is used in contact with a body of water to be purified to cause reactions including: o is2+2H2O+2e－→H2O2+2OH－(ii) a Or the oxygen reduction cathode 102 is used to contact the body of water to be purified to cause reactions including: o is2+2H2O+2e－→H2O2+2OH－And O2+2H2O+4e－→4OH－. The iron anode 103 is used for contacting with the water body to be purified to generate the following reactions: fe-2e-→Fe2+。
In another specific example, the oxygen reduction cathode 102 is used in contact with a body of water to be purified to react: o is2+2H2O+2e－→H2O2+2OH－(ii) a Or the oxygen reduction cathode 102 is used to contact the body of water to be purified to react: o is2+2H2O+2e－→H2O2+2OH－And O2+2H2O+4e－→4OH－. The iron anode 103 is used for contacting with the water body to be purified to react as follows: fe-2e-→Fe2+。
In a preferred embodiment, the water purification apparatus 100 based on self-driven electrochemical fenton-like flocculation is suitable for purification of arsenic-containing water. Arsenic is a metalloid element widely distributed in nature, has a certain toxicity, increases the risk of cancer in human organs such as skin, lung, bladder, liver and kidney, and is identified as a carcinogen by the international agency for research on cancer (IARC). At present, high-arsenic underground water is widely existed in a plurality of countries and regions around the world, and the long-term use of the high-arsenic underground water has a larger health risk. The water purification device 100 based on the self-driven electrochemical Fenton-flocculation reaction in the embodiment is used for purifying arsenic-containing water, so that a good arsenic removal effect can be achieved. Meanwhile, the water purifying device 100 based on the self-driven electrochemical Fenton-like flocculation reaction has a simple structure and low manufacturing cost, and can well meet the requirements of small centralized water supply or distributed water supply users in rural areas on arsenic treatment.
In the preferred embodiment, the water purification device 100 based on self-driven electrochemical Fenton-like flocculation reaction is used for purifying arsenic-containing water, and comprises a water storage chamber 101, an oxygen reduction cathode 102 and an iron anode 103; the oxygen reduction cathode 102 and the iron anode 103 are arranged in the water storage chamber 101; the water storage chamber 101 is used for containing water to be purified; the oxygen reduction cathode 102 is electrically connected with the iron anode 103, and the oxygen reduction cathode 102 is used for contacting with the water body to be purified to generate the following reaction: o is2+2H2O+2e－→H2O2+2OH－(ii) a The iron anode 103 is used for contacting with the water body to be purified to generate the following reactions: fe-2e-→Fe2+. At this time, a certain amount of hydrogen peroxide and ferrous ions are generated in the water storage chamber 101, and further, fenton-like reaction occurs, thereby realizing efficient oxidation of arsenic in the water body. The reaction of arsenic in the water reservoir 101 includes: as (III) +. OH → As (V) + H2O and/or As (III) +. Fe (IV) → As (V) + Fe3 +. Meanwhile, iron hydroxide floccules formed by hydrolyzing iron ions have a good adsorption effect on arsenic, and the removal rate of arsenic can be effectively improved. In addition, trivalent arsenic is oxidized into pentavalent arsenic, which is greatly reducedThe toxicity of arsenic is reduced, so that the toxicity of arsenic-containing water can be further reduced.
In one particular example, the oxygen reduction cathode 102 can float on the surface of the body of water to be purified. The oxygen reduction cathode 102 can float on the surface of the water body to be purified, so that the side-wall type oxygen reduction cathode 102 can be effectively prevented from being damaged due to long-time water pressure influence in the purification process, the service life of the oxygen reduction cathode 102 can be prolonged, and the problem of leakage caused by damage of the oxygen reduction cathode 102 can be avoided. Meanwhile, the oxygen reduction cathode 102 floats on the surface of the water body to be purified, can fully contact with the air, and utilizes the oxygen in the air to react, thereby further strengthening the self-driving effect. It will be appreciated that floating oxygen-reducing cathode 102 may be assisted by using a buoyant material, such as foam, to float oxygen-reducing cathode 102 to the surface of the body of water to be purified and to maintain oxygen-reducing cathode 102 in contact with the body of water to be purified.
Further, the water inlet of the water storage chamber 101 is closer to the bottom of the water storage chamber 101 than the oxygen reduction cathode 102 so that the water to be purified enters the water storage chamber 101 from below the oxygen reduction cathode 102. At this time, the water inlet is located below the oxygen reduction cathode 102, so that the problem that the oxygen reduction cathode 102 is separated from the surface of the water body to be purified due to the influence of water flow during water inflow can be effectively avoided. Furthermore, the water outlet of the water storage chamber 101 is located at the bottom of the water storage tank, so that the water body can be discharged under the action of self gravity, and the energy consumption is further reduced.
As an example of a position of the iron anode 103, the iron anode 103 can be sunk to the bottom of the water body to be purified. When water is purified, the iron anode 103 sinks at the bottom of the water body to be purified, so that the reaction of the iron anode 103 is more sufficient, and the water purification efficiency of the water purification device is improved. More specifically, the iron anode 103 is fixed to the bottom of the water storage chamber 101.
In one particular example, the oxygen-reducing cathode 102 is an air cathode. The air cathode can directly utilize oxygen in the air to react without providing an additional oxygen source, so that the cost and the energy consumption in the water purification process can be further reduced.
Further, the air cathode comprises a current collector and a carbon catalytic layer, wherein the carbon catalytic layer is positioned on one surface of the current collector; the carbon catalyst layer faces the outside of the water storage chamber 101. That is, in the installation process of the air cathode, the carbon catalyst layer is directed to the outside of the water storage chamber 101, the carbon catalyst layer is contacted with the air, the surface of the current collector without the carbon catalyst layer is directed to the inside of the water storage chamber 101, and the current collector is contacted with the water in the water storage chamber 101. Higher reaction efficiency can be obtained at this time, and the water purification efficiency is improved. It is understood that the carbon catalyst layer may also face the inside of the water storage chamber 101, and the utilization of oxygen in the air can be realized.
Preferably, the current collector is a titanium mesh current collector. More preferably, the mesh number of the titanium mesh is 50 to 100. Still more preferably, the mesh number of the titanium mesh is 60 mesh.
As a method for preparing an air cathode, the method for preparing an air cathode comprises the steps of:
mixing carbon black and activated carbon according to the mass ratio of 1 (0.8-1.5) to obtain a mixed carbon material; mixing the mixed carbon material with a binder solution to obtain a coating material; and coating the coating material on one surface of the current collector to obtain the carbon catalytic layer.
It is understood that the mass ratio of carbon black to activated carbon in the preparation of the air cathode may be, but is not limited to, 1:0.8, 1:0.9, 1:1, 1:1.1, 1:1.2, 1:1.3, 1:1.4, or 1: 1.5. Preferably, the mass ratio of carbon black to activated carbon is 1:1, in which case a better balance of hydrogen peroxide production and electron transport can be achieved.
Preferably, the concentration of the binder in the binder solution is 70mg/L to 90 mg/L. For example, the concentration of the binder in the binder solution may be, but is not limited to, 70mg/L, 75mg/L, 80mg/L, 85mg/L, or 90mg/L, etc. Further preferably, the binder is polyvinylidene fluoride (PVDF) and the solvent of the binder solution is Dimethylacetamide (DMAC).
Specifically, the preparation method of the binder solution comprises the following steps: the binder is completely dissolved in the solvent. More specifically, the binder is added to the solvent and dissolved with stirring at room temperature. Optionally, the stirring time is 7h to 8 h.
In a specific example, when the coating material is coated on one surface of the current collector, the coating time is controlled to be 3min to 5 min. For example, the coating time can be controlled to be, but is not limited to, 3min, 3.5min, 4min, 4.5min, or 5 min.
It is understood that the step of applying the coating material to one surface of the current collector further comprises the steps of: and cleaning and drying the current collector in sequence. Through cleaning and drying treatment, the dirt on the surface of the current collector is removed, and the performance of the air cathode is improved. Specifically, the cleaning is ultrasonic cleaning, and the cleaning time is 10 min-20 min. The cleaning medium for ultrasonic cleaning is ultrapure water. Alternatively, the washing time may be, but is not limited to, 10min, 12min, 15min, 18min, or 20 min. Specifically, the drying treatment is air drying for 5-8 h. For example, the drying time may be, but is not limited to, 5h, 6h, 7h, or 8 h.
In a preferred embodiment, the step of coating the coating material on one surface of the current collector further comprises the following steps: and contacting one surface of the air cathode coated with the coating material with ultrapure water, standing for 10-20 min, and drying to obtain the carbon catalyst layer. Alternatively, the side of the air cathode 103 coated with the coating material is contacted with ultrapure water and left to stand for 10min, 12min, 15min, 18min or 20 min.
As another preparation method of the air cathode, the preparation method of the air cathode includes the steps of:
calcining carbon black at 550-650 ℃ for 50-70 min to obtain a carbon material; mixing a carbon material with a binder solution to obtain a coating material; and coating the coating material on one surface of the current collector to obtain the carbon catalytic layer. Preferably, the concentration of the binder in the binder solution is 110mg/L to 130 mg/L. For example, the concentration of the binder in the binder solution may be, but is not limited to, 110mg/L, 115mg/L, 120mg/L, 125mg/L, 130mg/L, or the like. Further preferably, the binder is polyvinylidene fluoride (PVDF) and the solvent of the binder solution is Dimethylacetamide (DMAC). It is understood that the preparation of the binder solution, the coating method, and the like are the same as in the previous preparation method of the air cathode.
Specifically, before calcining, the temperature is increased to 550-650 ℃ at the temperature rising speed of 5-8 ℃/min. Alternatively, the ramp rate can be, but is not limited to, 5 deg.C/min, 5.5 deg.C/min, 6 deg.C/min, 6.5 deg.C/min, 7 deg.C/min, 7.5 deg.C/min, or 8 deg.C/min. The calcination temperature may be, but is not limited to, 550 deg.C, 560 deg.C, 570 deg.C, 580 deg.C, 590 deg.C, 600 deg.C, 610 deg.C, 620 deg.C, 630 deg.C, 640 deg.C or 650 deg.C. The calcination time can be selected from 50min, 52min, 55min, 58min, 60min, 62min, 65min, 68min or 70 min. More specifically, the carbon black is placed in a muffle furnace, the temperature is raised to 550-650 ℃ at the temperature raising speed of 5-8 ℃/min, and then the carbon black is calcined at the temperature of 550-650 ℃ for 50-70 min. Preferably, the temperature rising speed is 5 ℃/min, the calcining temperature is 600 ℃, and the calcining time is 60 min.
As one arrangement of the oxygen-reducing cathode 102 and the iron anode 103, the oxygen-reducing cathode 102 is arranged in parallel with the iron anode 103. Specifically, the distance between the oxygen reduction cathode 102 and the iron anode 103 is 1cm to 5cm, for example, the distance between the oxygen reduction cathode 102 and the iron anode 103 may be, but is not limited to, 1cm, 1.5cm, 2cm, 2.5cm, 3cm, 3.5cm, 4cm, 4.5cm, or 5 cm. Preferably, the distance between the oxygen reduction cathode 102 and the iron anode 103 is 3cm, so that better reaction strength can be maintained, reaction is promoted, and water purification efficiency is improved. It will be appreciated that the distance between the oxygen reduction cathode 102 and the iron anode 103 may be controlled by the amount of water to be purified.
In one particular example, the water purification apparatus further comprises a filter chamber 104; the inlet of the filter chamber 104 is connected with the outlet of the water storage chamber 101, and the filter chamber 104 is used for filtering the outlet water of the water storage chamber 101. The purified water body can be filtered through the filter chamber 104, so that the filtered clear liquid can be recycled.
Specifically, filter chamber 104 is divided into a plurality of sub-filter chambers 104; the sub-filtering chambers are distributed in sequence and the filtering degree of each sub-filtering chamber is gradually increased along with the distance from the water storage chamber 101.
More specifically, filter chamber 104 is divided into first sub-filter chamber 1041, second sub-filter chamber 1042 and third sub-filter chamber 1043; the first sub-filtering chamber 1041, the second sub-filtering chamber 1042 and the third sub-filtering chamber 1043 are distributed in sequence as being far away from the water storage chamber 101; the volume ratio of the first sub-filtering chamber 1041, the second sub-filtering chamber 1042 and the third sub-filtering chamber 1043 is (4.5-5.5): (1.5-2.5): 2.5-3.5). Preferably, the volume ratio of the first sub-filtration chamber 1041, the second sub-filtration chamber 1042 and the third sub-filtration chamber 1043 is 5:2: 3. It will be appreciated that when the radial dimensions of the plenums 101 are uniform, the volumes of the first, second and third sub-filter chambers 1041, 1042 and 1043 are expressed as the heights of the first, second and third sub-filter chambers 1041, 1042 and 1043, which facilitates control of the volumes of the sub-filter chambers by height control.
It is understood that the first sub-filter chamber 1041 is filled with a first filter medium, the second sub-filter chamber 1042 is filled with a second filter medium, and the third sub-filter chamber 1043 is filled with a third filter medium; the grain size of the first filter medium is 0.1 mm-1 mm, the grain size of the second filter medium is 1 mm-2 mm, and the grain size of the third filter medium is 4 mm-7 mm. Can avoid the filter medium with small particle size from entering the water outlet pipeline of the filter chamber to cause pipeline blockage.
In one particular example, the first filter media is at least one of masonry and sand; and/or the second filter medium is at least one of masonry and sand; and/or the third filter medium is at least one of masonry and sand. The masonry and/or the sandstone with easily available sources and low price can be selected as the filter medium, so that the manufacturing cost of the water purifying device is reduced. In addition, the wide existence of masonry and/or grit in rural areas can be used for local materials, and the water purification device is suitable for popularization in rural areas.
In a preferred embodiment, the filtering chamber 104 and the water storage chamber 101 are integrally formed. The filtering chamber 104 and the water storage chamber 101 are integrally formed, and water body reacted in the water storage chamber 101 can directly enter the filtering chamber 104 for filtering. With continued reference to fig. 1, in the same container, the upper part is a water storage chamber 101, and the lower part is a filtering chamber 104, and the water to be purified reacts in the water storage chamber 101 and then enters the filtering chamber 104 for filtering.
In another preferred aspect, the water purifying apparatus further comprises a secondary filtering chamber 105, the secondary filtering chamber 105 being divided into a first sub-secondary filtering chamber 1051, a second sub-secondary filtering chamber 1052 and a third sub-secondary filtering chamber 1053. The inlet of secondary filter chamber 105 is connected to outlet 106 of filter chamber and secondary filter chamber 105 is used to further filter the outlet water of filter chamber 104. It is understood that the secondary filtering chamber 105 and the filtering chamber 104 are identical in structure, and the first sub-secondary filtering chamber 1051, the second sub-secondary filtering chamber 1052 and the third sub-secondary filtering chamber 1053 are respectively identical to the first sub-filtering chamber 1041, the second sub-filtering chamber 1042 and the third sub-filtering chamber 1043. The filtered supernatant after filtration in the secondary filtration chamber 105 is discharged from the outlet 107 of the secondary filtration chamber.
In yet another embodiment of the present invention, a water purification method based on self-driven electrochemical fenton-like flocculation reaction is provided. The water purification method adopts the water purification device; the water purification method comprises the following steps: the water to be purified is added into the water storage chamber 101, so that the oxygen reduction cathode 102 and the iron anode 103 are both in contact with the water to be purified. At this time, reactions including: o is2+2H2O+2e－→H2O2+2OH－(ii) a The iron anode 103 undergoes a reaction comprising: fe-2e-→Fe2+. Therefore, the water body can be purified in a self-driven reaction mode, a certain amount of hydrogen peroxide and ferrous ions are generated in the water storage chamber 101, efficient oxidation and good adsorption of pollutants in the water body are realized, and the removal rate of the pollutants is effectively improved. Meanwhile, through self-driven reaction, external energy sources are not needed, and the energy consumption of water purification can be effectively reduced.
Preferably, when the oxygen reduction cathode 102 and the iron anode 103 are both in contact with the water body to be purified, the oxygen reduction cathode 102 is controlled to float on the surface of the water body to be purified. Further preferably, when the oxygen reduction cathode 102 and the iron anode 103 are both in contact with the water body to be purified, the iron anode 103 is controlled to sink to the bottom of the water body to be purified.
As some specific examples of the water inlet speed of the water to be purified in the water storage chamber 101, the water inlet speed of the water to be purified is 1mL/min to 10 mL/min. For example, the water inlet rate can be selected to be 1mL/min, 1.5mL/min, 1.8mL/min, 2mL/min, 2.5mL/min, 2.8mL/min, 3mL/min, 5mL/min, 8mL/min, 10 mL/min. As some specific examples of the water outlet speed of the water body in the water storage chamber 101, the water outlet speed of the water body is 1mL/min to 10 mL/min. For example, the water outlet rate can be selected to be 1mL/min, 1.5mL/min, 1.8mL/min, 2mL/min, 2.5mL/min, 2.8mL/min, 3mL/min, 5mL/min, 8mL/min, 10 mL/min. Preferably, the water inlet speed and the water outlet speed in the water storage chamber 101 are the same.
It can be understood that the size of the iron anode 103, the size of the oxygen reduction cathode 102, the water inlet speed, the water outlet speed, etc. can be selected according to the actual amount of water to be purified, so as to shorten the purification time and improve the purification efficiency.
The following are specific examples.
Example 1
In this example, the water purification apparatus shown in FIG. 1 was used to purify water containing arsenic. Before purification, the arsenic content in the arsenic-containing water to be purified was 500. mu.g/L. The oxygen reduction cathode 102 is an air cathode that floats on the surface of the water in the water storage chamber 101. The iron anode 103 sinks to the bottom of the water in the water storage chamber 101. The air cathode comprises a current collector and a carbon catalytic layer, wherein the carbon catalytic layer is positioned on one surface of the current collector; the carbon catalyst layer faces the outside of the water storage chamber 101. The volume of the water storage chamber 101 is 2L.
The preparation method of the air cathode comprises the following steps:
s101: the 60 mesh titanium mesh was ultrasonically cleaned in ultrapure water for 15min, and then dried. The dried titanium mesh served as the current collector.
S102: and adding polyvinylidene fluoride into dimethylacetamide, and stirring until the polyvinylidene fluoride is completely dissolved to obtain a binder solution.
S103: carbon black and activated carbon were mixed at a mass ratio of 1:1 to obtain a mixed carbon material.
S104: the mixed carbon material is mixed with a binder solution to obtain a coating material.
S105: the coating material is coated on one surface of the current collector. The coating time was 4 min.
S106: the side of the air cathode coated with the coating material was contacted with ultrapure water and left to stand for 15min, and then air-dried in a hood for 6 hours. After air drying, an air cathode was obtained.
The method for purifying the arsenic-containing water comprises the following steps:
s201: the water storage chamber 101 is added with the arsenic-containing water 200, and the water inlet speed and the water outlet speed of the water storage chamber 101 are 10 mL/min.
S202: the effluent of the water storage chamber 101 is filtered through the filter chamber 104 and the secondary filter chamber 105 in sequence to obtain filtered clear liquid.
In this example, the arsenic content in the filtrate was 29. mu.g/L, and the arsenic removal rate was 94.2%.
Example 2
The difference between this embodiment and embodiment 1 is that the water inlet speed of the water storage chamber 101 is 5 mL/min. In this example, the arsenic content in the filtrate was 100. mu.g/L, and the arsenic removal rate was 80%.
The technical features of the embodiments described above may be arbitrarily combined, and for the sake of brevity, all possible combinations of the technical features in the embodiments described above are not described, but should be considered as being within the scope of the present specification as long as there is no contradiction between the combinations of the technical features.
The above-mentioned embodiments only express several embodiments of the present invention, and the description thereof is more specific and detailed, but not construed as limiting the scope of the invention. It should be noted that, for a person skilled in the art, several variations and modifications can be made without departing from the inventive concept, which falls within the scope of the present invention. Therefore, the protection scope of the present patent shall be subject to the appended claims.

Claims (10)

1. A water purifying device based on self-driven electrochemical Fenton-like flocculation reaction is characterized by comprising a water storage chamber, an oxygen reduction cathode and an iron anode; the oxygen reduction cathode and the iron anode are arranged in the water storage chamber; the water storage chamber is used for containing water to be purified; the oxygen reduction cathode is electrically connected with the iron anode and is used for contacting with the water body to be purified to generate a reaction comprising the following steps: o is2+2H2O+2e－→H2O2+2OH－(ii) a The iron anode is used for contacting with the water body to be purified to generate the following reaction: fe-2e-→Fe2+。
2. The water purification apparatus of claim 1, wherein the oxygen reduction cathode is capable of floating on the surface of the body of water to be purified.
3. The water purification apparatus of claim 2, wherein the water inlet of the water storage chamber is closer to the bottom of the water storage chamber than the oxygen reduction cathode so that the water to be purified enters the water storage chamber from below the oxygen reduction cathode.
4. The water purification apparatus of claim 2, wherein the iron anode is capable of sinking to the bottom of the body of water to be purified.
5. The water purification apparatus of claim 1, wherein the oxygen reduction cathode is an air cathode.
6. The water purification apparatus of any one of claims 1 to 5, further comprising a filter chamber; the water inlet of the filtering chamber is connected with the water outlet of the water storage chamber, and the filtering chamber is used for filtering the water outlet of the water storage chamber.
7. The water purification apparatus of claim 6, wherein the filter chamber is divided into a plurality of sub-filter chambers; the sub-filtering chambers are distributed in sequence and the filtering degree of each sub-filtering chamber is gradually increased along with the distance from the water storage chamber.
8. The water purification apparatus of claim 7, wherein the filter chamber is divided into a first sub-filter chamber, a second sub-filter chamber, and a third sub-filter chamber; the first sub-filtering chamber, the second sub-filtering chamber and the third sub-filtering chamber are distributed in sequence along with the distance from the water storage chamber; the volume ratio of the first sub-filtration chamber, the second sub-filtration chamber and the third sub-filtration chamber is (4.5-5.5): (1.5-2.5): 2.5-3.5).
9. The water purification apparatus of claim 8, wherein the first sub-filter chamber is filled with a first filter medium, the second sub-filter chamber is filled with a second filter medium, and the third sub-filter chamber is filled with a third filter medium; the particle size of the first filter medium is 0.1-1 mm, the particle size of the second filter medium is 1-2 mm, and the particle size of the third filter medium is 4-7 mm.
10. A water purification method based on self-driven electrochemical fenton-like flocculation reaction, which is characterized in that the water purification device according to any one of claims 1-9 is adopted; the water purification method comprises the following steps:
and adding a water body to be purified into the water storage chamber, so that the oxygen reduction cathode and the iron anode are both in contact with the water body to be purified.
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