CN115594355B - In-situ pollutant degradation photoelectrocatalysis water purification treatment system and method - Google Patents
In-situ pollutant degradation photoelectrocatalysis water purification treatment system and method Download PDFInfo
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Classifications
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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
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/46104—Devices therefor; Their operating or servicing
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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
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
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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
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/38—Organic compounds containing nitrogen
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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
- C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
- C02F2103/007—Contaminated open waterways, rivers, lakes or ponds
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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
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/005—Combined electrochemical biological processes
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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
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/32—Biological treatment of water, waste water, or sewage characterised by the animals or plants used, e.g. algae
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W10/00—Technologies for wastewater treatment
- Y02W10/30—Wastewater or sewage treatment systems using renewable energies
- Y02W10/37—Wastewater or sewage treatment systems using renewable energies using solar energy
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- Life Sciences & Earth Sciences (AREA)
- Hydrology & Water Resources (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
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Abstract
The invention belongs to the field of urban black and odorous water body and water environment restoration, eutrophication prevention and control and PPCPs (emerging pollutants) in-situ degradation, and particularly relates to a system and a method for in-situ degradation of pollutants by photocatalysis and water purification. The system consists of emergent aquatic plants, photocatalytic materials, a composite microbial fuel cell working principle and bioelectricity Fenton technology, and comprises a floating plate, a photocatalytic plate, a cathode and anode electrode, an external resistor, an iron-carbon micro-electrolysis filler and the like. According to the invention, emergent aquatic plants, photocatalytic materials and bioelectricity Fenton technology are introduced on the basis of the working principle of the MFC, and the MFC is used for in-situ restoration of water and synchronous electricity generation for pollutant removal. The three effects of synchronous power generation by pollutant removal, zero external energy supply by water treatment and in-situ water environment restoration are realized.
Description
Technical Field
The invention belongs to the field of urban black and odorous water body and water environment restoration, eutrophication prevention and control, PPCPs (emerging pollutants) in-situ degradation, and particularly relates to a system and a method for in-situ degradation of pollutants by photocatalysis and water purification.
Background
Along with the development of economy and the acceleration of urban process, a large amount of domestic sewage, industrial wastewater, agricultural non-point source pollution and the like are flushed into the river, so that more and more surface water bodies such as rivers, lakes and reservoirs completely lose specific ecological functions, urban black odor and water body eutrophication of the lakes and reservoirs occur to different degrees, the resource utilization of the water bodies is seriously hindered, the economic development of surrounding towns and the drinking safety of residents are restricted, and even the running of an aquatic ecological system is caused, so that the health of human beings and the environmental safety are seriously threatened. The main sources of pollutants in urban surface water bodies are exogenous and endogenous pollutants, wherein the endogenous pollutants are the exogenous pollutants which are discharged for a long time, so that a large amount of nitrogen and phosphorus organic matters, heavy metals and other toxic and harmful substances are accumulated in the sediment to become carriers and reservoirs for transferring and converting the pollutants, and in addition, dynamic balance relation exists between the river sediment and overlying water, material and energy exchange is carried out at any moment, the endogenous treatment is incomplete, and the urban water body pollution is difficult to thoroughly remove. In addition, the problem of huge energy sources caused by high energy consumption of conventional wastewater treatment is urgently needed, and a water treatment technology capable of effectively relieving double dilemma of water environment pollution and energy crisis is urgently needed.
Microbial Fuel Cell (MFC) technology is a water pollution control technology that can synchronously achieve in-situ degradation of contaminants and power generation. The technology can degrade the pollutants and realize the electricity generation conversion of potential energy sources in the pollutants at the same time, thereby conforming to the sustainable development concept of the resource utilization of the pollutants. But current individual MFCs are limited in practical applications by low power density. The MFC is coupled with other technologies, so that not only can the defect of the MFC be overcome and the in-situ application of electric quantity be realized, but also the water treatment capacity of the coupling system can be improved. But prior art has less research on coupling of MFCs to other technologies.
Disclosure of Invention
The invention aims to solve the problems, introduces emergent aquatic plants, photocatalytic materials and bioelectricity Fenton technology on the basis of the working principle of the MFC, and is used for synchronously generating electricity for in-situ restoration of water and pollutant removal. The three effects of synchronous power generation by pollutant removal, zero external energy supply by water treatment and in-situ water environment restoration are realized. The specific technical scheme is as follows:
the photoelectric catalytic water purification treatment system for in-situ degradation of pollutants comprises a floating plate, wherein the floating plate comprises a grid and a carrier planting groove, the carrier planting groove is a detachable floating bed planting basket, and the floating bed planting basket is filled with fixed filler and used for planting emergent aquatic plants; the outside of the floating plate is connected with a photocatalytic plate through a wire, a cathode is arranged under the photocatalytic plate, the cathode is immersed in the surface of the liquid level of the polluted water body and is connected with an anode through a wire and a resistor, and the anode is fixedly immersed in anaerobic bottom mud at the bottom of the polluted water body through a connecting wire; and iron-carbon micro-electrolysis hollowed-out filling balls are hung below the floating plate, and iron-carbon micro-electrolysis filling materials are arranged in the filling balls.
Further, the photocatalytic plate is made of a metal semiconductor material, a nonmetal semiconductor material or a composite semiconductor material.
Further, the photocatalysis plate is one of a TiO2/Fe2O3 composite photoelectrode, a TiO2 photoelectrode, an In2TiO5 photoelectrode and a g-C3N4 photoelectrode.
Further, the emergent aquatic plant is canna, calamus or water spinach.
Further, the iron-carbon micro-electrolysis filler is wrapped by a stainless steel net and placed in the iron-carbon micro-electrolysis hollowed-out filler balls.
Further, the cathode and the anode are one or more of graphite felt, carbon felt or stainless steel wire mesh coated active carbon particles, and the thickness is 5 mm-20 mm.
Furthermore, the connection among the cathode, the anode, the lead and the external resistor uses crocodile clips or metal connectors; the lead wire connecting the cathode and the anode passes through the center of the cathode and anode materials; the lead is copper wire or titanium wire; the resistance value of the external resistor is 200 to 1000 omega.
The invention also provides a treatment method of the water purification treatment system, wherein the system is placed in a polluted water body to be repaired, and the anode is placed in anaerobic sediment at the position of 5 cm-8 cm at the bottom of the polluted water body.
Further, the planting density of the emergent aquatic plants is 8 plants/square meter to 15 plants/square meter.
According to the invention, the water environment restoration is carried out on urban black and odorous water bodies, lakes and the like by utilizing emergent aquatic plants, photocatalytic polymer materials, a microbial fuel cell working principle and a bioelectricity Fenton technology, so that the concentration of PPCPs in the water bodies is further degraded, and the water quality purification efficiency is improved. The emergent aquatic plants form an aerobic environment by conveying oxygen to the roots, and provide a proper environment for the growth of microorganisms, so that pollutants in the wastewater are degraded; under the excitation of sunlight, the photocatalytic material generates electrons and holes, the holes and hydroxyl groups are combined to generate hydroxyl free radicals, and the electrons and oxygen are combined to generate superoxide free radicals, and meanwhile, by improving the specific surface area of the photocatalytic material, a large amount of pollutants can be adsorbed, and the pollutants adsorbed on the surface of the photocatalytic material are oxidized into inorganic small molecules such as carbon dioxide, water and the like, so that the aim of purifying the environment is fulfilled; the bioelectric Fenton technology utilizes the anode microorganisms of the microbial fuel cell system to oxidize organisms to generate electrons, and directly converts biomass energy into electric energy to form a water body bioelectric Fenton environment, so that external energy input is not needed, and pollutants, PPCPs and the like in wastewater are removed. Finally, zero external energy supply for water treatment is realized, the in-situ restoration effect of the water environment is improved, and organic matters in pollutants are oxidized through biological metabolic processes.
Compared with the prior art, the invention has the beneficial effects that:
1. the in-situ pollutant degrading photoelectrocatalysis unpowered water purifying technology is constructed, and the pollutant removing rate in the damaged water body is improved. Compared with the traditional water treatment technology, the invention has the advantages that on the basis of the working principle of the MFC, through the synergistic effect of emergent aquatic plants, photocatalytic materials and bioelectricity Fenton principle, extracellular electrogenerating bacteria oxidize organisms in an anaerobic state to generate electrons and degrade organic pollutants at the same time, enzymes secreted by roots of emergent aquatic plants can promote pollutant degradation, and meanwhile, through the introduction of iron-carbon micro-electrolysis environment and photocatalytic high polymer materials, the high-efficiency degradation of persistent pollutants is realized, and finally, the synergistic purification function is realized. The method solves the problem of high energy consumption in water environment in-situ restoration and treatment, effectively reduces the concentration of pollutants and the content of PPCPs in the water body, and promotes the realization of renewable energy source utilization and sewage treatment zero-energy consumption technology.
2. By introducing emergent aquatic plants, photocatalytic materials and bioelectricity Fenton technology, the water quality purification efficiency and the energy utilization rate are effectively improved, the sunlight utilization rate is improved, and the degradation capacity is enhanced.
3. The emergent aquatic plants are used as floating bed plants, so that the ecological floating bed can cooperatively purify water, has no secondary pollution, increases landscape benefits and optimizes ecological environment. In the implementation process and the subsequent effects, the ecological environment and the human body are not damaged, the water area landscape can be beautified, and the promotion effect on aquatic organisms is also achieved.
Drawings
FIG. 1 is a schematic diagram of a small test device according to the present invention;
FIG. 2 is a top view of a pilot device of the present invention;
reference numerals: 1. the photocatalytic plate comprises a photocatalytic plate body, a cathode body, an iron-carbon micro-electrolysis hollow filling ball, a fixed value resistor, a lead, an anode, an emergent aquatic plant, a microorganism and anaerobic sediment, wherein the photocatalytic plate body comprises a photocatalytic plate body, a cathode body, an iron-carbon micro-electrolysis hollow filling ball, a fixed value resistor, a lead, an anode, an emergent aquatic plant body, a microorganism and an anaerobic sediment.
Detailed Description
The following description of the embodiments of the present invention will be made clearly and completely with reference to the accompanying drawings, in which it is apparent that the embodiments described are only some embodiments of the present invention, but not all embodiments. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
As shown in fig. 1-2, a pollutant in-situ degradation photocatalysis water purifying treatment system is characterized in that: the floating plate comprises a grid and a carrier planting groove, wherein the carrier planting groove is a detachable floating bed planting basket, and the floating bed planting basket is filled with fixed filler and planted with emergent aquatic plants 7; the outside of the floating plate is connected with a photocatalytic plate 1 by a wire, a cathode 2 is arranged under the photocatalytic plate, the cathode is immersed in the surface of the liquid level of the polluted water body and is connected with an anode 6 by a wire 5 and a resistor 4, and the anode is fixedly immersed in anaerobic bottom mud 9 at the bottom of the polluted water body by a connecting wire; an iron-carbon micro-electrolysis hollow filling ball 3 is hung below the floating plate, and iron-carbon micro-electrolysis filling materials are arranged in the filling ball.
The test was performed using a pilot test, a test device (cuboid, length 40, width 20, height 50 cm) was set, the average temperature of the test device run was 30.+ -. 5 ℃, sampling holes were established at a height of 5, 10, 20 and 30 cm from the bottom of the reactor, the entire container volume was 40L, and the entire test device was wrapped with black plastic to prevent algae growth.
Example 1
The method comprises the steps of loading 10cm of sludge into the bottom of a pilot reaction test device, adding wastewater into the pilot reaction test device for simulation, placing a grid and a carrier planting groove on the upper water surface, loading quartz sand into the carrier planting groove, planting emergent water in the floating carrier planting groove, arranging a high molecular photocatalytic material around emergent water plants, connecting the high molecular photocatalytic material through a connecting wire, placing the emergent water on the surface of a cathode, arranging an anode at the position of 5cm of the bottom sludge so as to enrich pollutants, enabling a wire to pass through the anode, connecting the wire to the cathode through an external resistor to realize a closed-loop circuit, and simultaneously suspending an iron-carbon micro-electrolysis grid and an iron-carbon micro-electrolysis filler under the cathode to construct an iron-carbon micro-electrolysis environment, wherein the iron-carbon micro-electrolysis filler is wrapped by stainless steel and is arranged in the iron-carbon micro-electrolysis grid. The emergent aquatic plants are mainly canna and calamus which are planted on the floating carrier planting groove according to the proportion of 2:1. The bottom mud is anaerobic nitrified sludge in pig farm, the bottom mud is collected and then evenly mixed, weeds, stones and the like are removed from the sludge, natural sedimentation is carried out for 24 hours, and the sludge is stored in a small scale reactor in a closed and light-shielding manner. The wastewater is sewage after anaerobic treatment of a biogas digester in a pig farm. The photocatalytic material is a composite semiconductor material (TiO 2 /Fe 2 O 3 Composite material). The cathode and anode are made of carbon felt. The external lead is titanium wire. The external resistor is a constant resistor of 1000 omega.
The water quality restoration is carried out by adopting the pilot scale, the concentration of COD, ammonia nitrogen, TP and PPCPs (oxytetracycline and tetracycline are selected as representative pollutants) in the wastewater is researched, and the initial concentration of COD in the wastewater is 324-708mg L -1 The initial concentration of ammonia nitrogen is 158-284mg L -1 Initial concentration of TP is 24-35mg L -1 The initial concentration of terramycin is 86-221mg L -1 Four (IV)The initial concentration of the cyclosporin is about 21-33.2mg L -1 To reduce the effect of daily variation on removal efficiency, samples were collected every two days at local time 10:00, while recording system operation, ambient temperature and weather. The wastewater treatment performance was determined by daily measurement of COD, ammonia nitrogen, TP, oxytetracycline, and tetracycline concentrations. Experimental results show that after the small test device is adopted, the COD concentration in the average effluent concentration is 102.7mg L after two days of stable treatment -1 The concentration of ammonia nitrogen is 56.8mg L -1 TP concentration was 1.73mg L -1 The average removal effect of the technology on COD is 80%, the ammonia nitrogen removal rate is about 74%, the TP removal rate is up to 94%, the terramycin removal effect is about 97.3%, and the tetracycline removal rate is about 98.3%.
Example two
15cm of sludge is filled in the bottom of the pilot reaction test device, the sludge is taken from river bottom sludge after weeds and stones are removed, natural sedimentation is carried out for 24 hours, and the sludge is stored in the pilot reactor in a closed and shading mode. Adding domestic wastewater into the device for simulation, placing floating plate (including carrier planting groove and grid) on the surface of water body, planting rhizoma Acori Calami in the floating plate, and adding metal semiconductor material (TiO 2 ) The high molecular photocatalytic material is concentrated on the surface of the cathode, the anode is arranged at a position 5cm away from the upper end of the bottom mud, the graphite felt is used as a cathode-anode material, the titanium wire passes through the anode as a lead and is connected to the cathode through an external resistor (a fixed value resistor of 500 Ω), stable electricity generation is realized, and meanwhile, an iron-carbon micro-electrolysis environment is built under the cathode (the building mode is as described in the first embodiment).
By adopting the scheme, the water quality restoration of black and odorous water bodies formed by the direct-discharge riverway of domestic sewage is simulated, the typical pollutant concentration in the wastewater is studied, the concentration of sulfonamide antibiotics and tetracycline is mainly measured in PPCPs (emerging pollutants), and the concentration of COD in the sewage is 142-350mg L -1 The initial concentration of ammonia nitrogen is 23-48mg L -1 Initial concentration of TP is 3-6mg L -1 The initial concentration of sulfonamide antibiotic is 120-520ng L -1 The initial concentration of tetracycline is about 180-600ng L -1 In order to reduce the effect of daily variation on removal efficiency,samples were collected every two days at local time 8:00, while recording system operation, ambient temperature and weather. The wastewater treatment performance was determined by measuring the concentration of various substances daily. The experimental result shows that after the technology is adopted and is subjected to two-day stabilization treatment, the result shows that the average removal effect of COD is 89.67%, the ammonia nitrogen removal rate is about 78%, the TP removal rate is up to 97%, the removal effect of sulfonamide antibiotics is about 96% and the removal rate of tetracycline is about 97%.
While the preferred embodiments of the present patent have been described in detail, the present patent is not limited to the above embodiments, and various changes may be made without departing from the spirit of the present patent within the knowledge of one of ordinary skill in the art.
Claims (6)
1. A pollutant in-situ degradation photocatalysis water purification treatment system is characterized in that: the floating plate comprises a grid and a carrier planting groove, wherein the carrier planting groove is a detachable floating bed planting basket, and the floating bed planting basket is filled with fixed filler and used for planting emergent aquatic plants; a circle of photocatalysis plates connected by wires are arranged on the outer side of the floating plate, a cathode is arranged below the photocatalysis plates, the cathode is immersed at the surface of the liquid level of the polluted water body and is connected to an anode through wires and a resistor, and the anode is fixedly immersed in anaerobic bottom mud at the bottom of the polluted water body through a connecting wire; iron-carbon micro-electrolysis hollowed-out filling balls are hung below the floating plate, and iron-carbon micro-electrolysis filling materials are arranged in the filling balls; the photocatalysis plate is one of a TiO2/Fe2O3 composite photoelectrode, a TiO2 photoelectrode, an In2TiO5 photoelectrode and a g-C3N4 photoelectrode; the cathode and the anode are one or more of graphite felt, carbon felt or stainless steel wire mesh coated active carbon particles, and the thickness is 5 mm-20 mm.
2. The in situ pollutant-degrading photocatalytic water purification treatment system according to claim 1, wherein: the emergent aquatic plant is canna, calamus or water spinach.
3. The in situ pollutant-degrading photocatalytic water purification treatment system according to claim 1, wherein: the iron-carbon micro-electrolysis filler is wrapped by a stainless steel net and is placed in the iron-carbon micro-electrolysis hollowed-out filler ball.
4. The in situ pollutant-degrading photocatalytic water purification treatment system according to claim 1, wherein: the cathodes, the anodes, the wires and the external resistors are connected by crocodile clips or metal connectors; a lead wire connecting the cathode and the anode passes through the center of the cathode and anode materials; the lead is copper wire or titanium wire; the resistance value of the external resistor is 200 to 1000 omega.
5. A treatment method using the water purification treatment system as claimed in any one of claims 1 to 4, characterized in that: placing the system in a polluted water body to be repaired, and placing the anode in anaerobic sediment at the position of 5 cm-8 cm at the bottom of the polluted water body.
6. The process according to claim 5, wherein: the planting density of the emergent aquatic plants is 8 plants/square meter-15 plants/square meter.
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