CN109879402B - Bioelectrochemical device and method for coupling and purifying bottom mud and water body of aquaculture pond - Google Patents
Bioelectrochemical device and method for coupling and purifying bottom mud and water body of aquaculture pond Download PDFInfo
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- Y02A40/10—Adaptation technologies in agriculture, forestry, livestock or agroalimentary production in agriculture
- Y02A40/22—Improving land use; Improving water use or availability; Controlling erosion
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Abstract
The invention discloses a bioelectrochemical device for coupling and purifying bottom mud and a water body of an aquaculture pond. The device comprises: the bioelectrochemical anode is arranged in the bottom mud of the aquaculture pond, and the bioelectrochemical cathode floats on the water body of the aquaculture pond, and is connected with the bioelectrochemical cathode through a lead; wherein the bioelectrochemical anode comprises two metal meshes and an activated carbon felt sandwiched between the two metal meshes; the bioelectrochemical cathode comprises a metal supporting net, conductive cellucotton or conductive sponge is covered on the metal supporting net, and aquatic plants are planted on the metal supporting net. The invention also discloses a method for purifying the bottom mud and the water body of the aquaculture pond by using the device in a coupling manner. According to the invention, a bioelectrochemical system is constructed in the culture pond, and the degradation and mineralization of organic matters in the bottom mud are enhanced by utilizing the difference of oxidation-reduction potentials in the bottom mud and the water body, so that the denitrification of nitrate nitrogen in the water body and the removal of pollutants are promoted, and the reduction, harmlessness and water quality purification of the sludge are realized in situ.
Description
Technical Field
The invention belongs to the field of environmental protection, and particularly relates to a bioelectrochemical device and a bioelectrochemical method for coupling and purifying bottom mud and a water body of an aquaculture pond.
Background
China has wide water areas and rich aquatic resource types, and is one of the longest countries in the world engaged in aquaculture. In recent years, with the increasing economic level, the demand of the people on aquaculture products is increasing, so that the aquaculture industry is rapidly developed. However, the rapidly growing aquaculture industry is also associated with a number of environmental issues. The most typical environmental pollution sources are residual baits and aquatic animal metabolites in aquaculture, according to statistics, only 9.1 percent and 17.4 percent of nitrogen and phosphorus in the feed put in the fish culture process are assimilated by the fish, and a large amount of elements such as nitrogen and phosphorus in the residual baits and excretions are deposited in the bottom sediment or dissolved in the water body and are continuously converted in the bottom sediment and the water body. The putrefactive decomposition of the residual bait and excrement causes the reduction of dissolved oxygen in water, the reduction of pH, the increase of COD, the breeding of pathogenic bacteria and the generation of a large amount of bottom mud. Moreover, drugs are widely used or even abused in the aquaculture industry, and disinfectants, antibiotics, hormones, vaccines and the like are potential environmental pollutants. The medicines are difficult to biodegrade, so that the medicines are continuously enriched in water and bottom mud, the quality and the yield of aquatic products are influenced, and the medicines can enter a human body through a food chain to threaten the health and the safety of human beings. Aquaculture pollution is also influenced by human activities, and common difficultly-degradable pollutants in industry (such as polycyclic aromatic hydrocarbon, polychlorinated biphenyl and the like) and pesticides and fertilizers widely used in agriculture all enter aquaculture water areas through surface runoff and are deposited in soil and bottom mud, so that potential environmental risks are formed.
The bioelectrochemical system combines the characteristics of biotechnology and electrochemical oxidation/reduction technology, and converts the energy in substrates such as organic matters into electric energy by utilizing the extracellular electron transfer capacity of microorganisms. Recent research on bioelectrochemistry is always subject to lower coulombic efficiency and is difficult to be a better energy acquisition means, but the exhibited pollutant degradation capability allows researchers to have a new application field for the bioelectrochemical system. At the anode of bioelectrochemistry, microorganisms are in an anaerobic environment, and electrons generated by degradation of a substrate are transferred to the cathode through an external circuit and finally combined with an electron acceptor. While the cathode combines the electrons of the external circuit with a final electron acceptor, which may be oxygen or other oxidizing species. Due to the existence of different redox conditions of the cathode and the anode, the physiological and biochemical processes of the microorganisms at the two poles are continuously promoted. At present, artificial wetland microbial fuel cells, soil microbial fuel cells and the like are available as pollutant removal devices designed on the principle of bioelectrochemistry, and are used for removing heavy metals, refractory organic matters, water COD (chemical oxygen demand) and the like in the environment. At present, no report for treating bottom mud or water body of an aquaculture pond by using the principle exists.
Disclosure of Invention
The purpose of the invention is as follows: aiming at the problems in the prior art, the invention provides a bioelectrochemical device which is novel in structure and utilizes a bioelectrochemical principle to couple and purify bottom mud and a water body of an aquaculture pond, and the invention also aims to provide a method for coupling and purifying the bottom mud and the water body of the aquaculture pond.
The technical scheme is as follows: the invention relates to a bioelectrochemical device for coupling and purifying bottom mud and a water body of an aquaculture pond, which comprises: the bioelectrochemical anode is arranged in the bottom mud of the aquaculture pond, and the bioelectrochemical cathode floats on the water body of the aquaculture pond, and is connected with the bioelectrochemical cathode through a lead; wherein the bioelectrochemical anode comprises two metal meshes and an activated carbon felt sandwiched between the two metal meshes; the bioelectrochemical cathode comprises a metal supporting net, conductive cellucotton or conductive sponge is covered on the metal supporting net, and aquatic plants are planted on the metal supporting net.
The bottom sludge of the aquaculture pond is in an anaerobic environment, is rich in organic matters and hydrophobic pollutants, and is beneficial to the degradation of the substrate by bioelectrochemistry anode microorganisms. Meanwhile, in the culture environment, an aeration and oxygenation device is arranged in the aquaculture water body, and dissolved oxygen in the water body is beneficial to the consumption of electrons in the bioelectrochemical system. According to the invention, the characteristic of environmental conditions of the aquaculture pond is ingeniously utilized to construct a bioelectrochemical system, microorganisms of the bioelectrochemical anode are subjected to anaerobic degradation in the bottom mud and are not subjected to electron accumulation, and oxygen molecules of the bioelectrochemical cathode are continuously combined with external circuit electrons, so that the bioelectrochemical anode is promoted to further degrade organic matters or pollutants to generate electrons. The bioelectrochemistry cathode is combined with the aquatic plant, the activity of cathode microorganisms can be promoted by the secretion of plant root systems and the oxygen secretion of the root systems, and pollutants in water can be removed while the combination of electrons and oxygen is accelerated.
The bioelectrochemical anodes are a plurality of bioelectrochemical anodes which are vertically arranged. The configuration of the plurality of anodes can, on the one hand, act on the degradation of the sludge contamination in a larger spatial area than a single anode of equal area; on the other hand, the multi-anode configuration has better mechanical strength and shearing force resistance characteristics, and facilitates the arrangement, recovery and transfer of the anodes in the substrate sludge. The number of the plurality of the bioelectrochemical anodes is more than or equal to 2, and the number of the bioelectrochemical anodes can be set according to the requirement of the actual treatment environment.
In the bioelectrochemistry cathode structure, the conductive cellucotton or the conductive sponge is in a porous structure, the porous structure is favorable for the large value increase of microorganisms, the water treatment effect is improved, the thickness of the conductive cellucotton or the conductive sponge is 2-5 cm, and the pore diameter is 20-50 PPI. The bioelectrochemistry cathode material in the range can better enrich electrochemically active microorganisms, quickly form a biological membrane in pores, and is favorable for catalyzing external circuit electrons to be combined with an electron acceptor (such as oxygen) by the microorganisms.
The bioelectrochemical cathode is arranged in the floating bed. The floating bed provides buoyancy for the floating of the bioelectrochemical cathode, so that the cathode is just immersed in the water surface and can be made of a PVC pipe or a foam pipe.
The ratio of the projection area of the cathode and the anode is 1: 1-1: 2. The biomass and metabolic activity of bipolar bioelectrochemically active microorganisms are one of the main influencing factors for setting the area ratio of the cathode and the anode. Anaerobic electrochemically active bacteria in the anode region consume the substrate to produce extracellular electrons that are transferred to the cathode via an external circuit. The system exhibits optimal contaminant removal efficiency when the rate at which electrons are bound to the electron acceptor on the cathode matches the rate at which electrons are produced at the anode.
The wires connecting the cathode and the anode of the bioelectrochemical system are wrapped by waterproof rubber sheets, and a resistor of 10-1000 omega is connected in a circuit to control the potential of the two electrodes and the flow rate of electrons so as to achieve the optimal oxidation-reduction potential.
The invention also provides a method for coupling and purifying the bottom mud and the water body of the aquaculture pond, which comprises the following steps: using said bioelectrochemical device;
(1) and (3) horizontally or vertically inserting the bioelectrochemical anode after gathering anaerobic microorganisms into the bottom mud of the culture pond, enabling the bioelectrochemical cathode to float on the water body of the culture pond, and connecting the bioelectrochemical anode and the bioelectrochemical cathode to construct a bioelectrochemical device.
(2) In the starting stage of the bioelectrochemical device, an external circuit (namely, the circuit connection between the cathode and the anode) is opened and placed for 2 to 3 days, so that the molecular oxygen in the bioelectrochemical anode area is fully consumed, a strict anaerobic environment is formed, and the growth and the metabolism of anode electrochemically active microorganisms are facilitated. And meanwhile, monitoring the open-circuit voltage, and when the open-circuit voltage reaches 500mV, closing the external circuit to transfer the generated extracellular electrons to the cathode region of the floating bed.
(3) And monitoring the concentration change of pollutants in the water body and the bottom mud of the culture pond to achieve the treatment target.
In the step (1), the bioelectrochemical anode is positioned below a muddy water interface by 15cm when horizontally placed; the bioelectrochemical anode is positioned below a muddy water interface by 10cm when vertically placed. When the anode is placed, the anode needs to be fixed in the bottom mud layer, so that the anode is not interfered by the disturbance of overlying water. And meanwhile, the inserting depth of the anode can ensure that the anode is fully contacted with pollutants deposited on the bottom mud. The above depth can satisfy the requirements.
The vertical placement mode is more favorable for arrangement, recovery and transfer of the bioelectrochemical anodes, and all the bioelectrochemical anodes are vertically inserted into the bottom mud of the aquaculture pond at equal intervals.
The bioelectrochemical cathode is adjacent to the aeration device of the aquaculture pond, can provide higher dissolved oxygen concentration for the cathode, and is beneficial to the cathode reaction.
When the potential difference between the two poles of the bioelectrochemical device is lower than 200mV in the treatment process, which indicates that the electricity generation performance of the electrochemically active microorganisms is reduced, the bioelectrochemical anode is preferably re-enriched with anaerobic microorganisms or moved to a new sediment area to be treated.
Has the advantages that:
according to the invention, by constructing a bioelectrochemical system in the culture pond, the degradation and mineralization of organic matters in the bottom mud are enhanced by utilizing the difference of oxidation-reduction potentials in the bottom mud and the water body, the denitrification of nitrate nitrogen in the water body and the removal of pollutants are promoted, the reduction, harmlessness and water purification of the sludge are realized in situ, the energy is saved, and the purification efficiency is improved.
The method of the invention can be used for degrading organic matters (including and not limited to humus, cellulose, starch and volatile fatty acid) deposited in the bottom sediment and pollutants which are difficult to degrade (such as polycyclic aromatic hydrocarbon, antibiotics and the like) and inhibiting the proliferation and diffusion of drug-resistant bacteria and pathogenic bacteria.
Drawings
FIG. 1 is a schematic structural diagram of a bioelectrochemical device for coupling and purifying bottom mud and a water body of an aquaculture pond according to the present invention;
FIG. 2 is a cross-sectional view of the bioelectrochemical device for coupling and purifying the bottom mud and the water body of the aquaculture pond.
Detailed Description
The present invention is further illustrated by the following examples, which are intended to be purely exemplary and are not intended to limit the scope of the invention, as various equivalent modifications of the invention will occur to those skilled in the art upon reading the present disclosure and fall within the scope of the appended claims.
As shown in fig. 1 and fig. 2, the bioelectrochemical device for coupling and purifying the bottom mud and the water body of the aquaculture pond in the embodiment includes: the biological electrochemical anode 1 is arranged in the bottom mud of the aquaculture pond, the biological electrochemical cathode 2 floats on the water body of the aquaculture pond, and the biological electrochemical anode is connected with the biological electrochemical cathode through a lead 3.
The bioelectrochemical anode is in a sandwich type and comprises two metal meshes 101 and an activated carbon felt 102 clamped between the two metal meshes 101, wherein the two metal meshes can clamp and fix the activated carbon felt through a fixing piece such as a titanium wire. Because the strength of the activated carbon felt is not enough, the metal net plays a supporting role on one hand, so that the bioelectrochemical anode can be smoothly inserted into the bottom mud of the culture pond, and on the other hand, the metal net is used as a current collector to lead out the current of the bioelectrochemical anode, and the metal net can adopt a stainless steel metal net. The thickness of the activated carbon felt is 10 mm-20 mm, and the excessive thick carbon felt can cause that the internal activated microorganisms are difficult to fully contact with a substrate, so that an ineffective area exists in the anode, and the excessive thin carbon felt is difficult to enrich enough functional microorganisms, thereby limiting the efficiency of the anode. The activated carbon felt can be round, rectangular and the like, and can be enlarged or reduced according to actual conditions, for example, the radius or the side length is 10-100 cm. The anaerobic microorganism enrichment of the activated carbon felt adopts a conventional method, for example, after dust is washed by clean water, 1mol/L hydrochloric acid and 1mol/L sodium hydroxide are respectively used for soaking for 12 hours, then the activated carbon felt is cleaned by the clean water and dried in the air, and the activated carbon felt is cultured in a biased anaerobic reactor for more than 1 week, thus the anaerobic microorganism with electrochemical activity can be enriched. The bioelectrochemical anodes are vertically arranged and are 3 in the same size, are inserted into the bottom mud of the culture pond at equal intervals (the interval does not have a particularly strict requirement, and the phenomenon that the competition of microorganisms on substrates is unbalanced due to the fact that carbon felts are too close to each other is prevented), and are connected with the same bioelectrochemical cathode in a stacking mode. The bioelectrochemical anode can also be horizontally inserted into the bottom mud of the culture pond.
The bioelectrochemical cathode 2 comprises a metal supporting net 201, conductive cellucotton or conductive sponge 202 covered on the metal supporting net, and aquatic plants 203 are planted on the metal supporting net. The metal supporting net 201 plays a role of supporting and collecting fluid, and can be made of stainless steel materials, the thickness of the conductive fiber cotton or the conductive sponge 202 is more than 20mm, the pore diameter is about 30PPI, the conductive fiber cotton or the conductive sponge is provided with an opening, floating or emergent aquatic plants including but not limited to lettuce, cress, water spinach, ryegrass and the like can be planted, and holes are cut on the metal supporting net to enable the roots of the plants to grow. The projection area ratio of the bioelectrochemical cathode to the bioelectrochemical anode is 1:1, the bioelectrochemical cathode is arranged in a floating bed 4, and the floating bed can be a frame structure made of hollow plastic pipes wrapping foam.
The metal net of the bioelectrochemistry anode is connected with the metal supporting net of the bioelectrochemistry cathode through a lead 3, the lead is wrapped by a waterproof rubber, and is connected with a resistor 5 of 10-1000 omega in a circuit to form a closed loop, and the resistor controls the potential of two poles and the flow velocity of electrons to achieve the optimal oxidation-reduction potential.
The method for purifying the bottom mud and the water body of the aquaculture pond by adopting the device in a coupling way comprises the following steps:
(1) investigating an aquaculture field to be treated, and acquiring the pollution types and the pollution degrees of an aquaculture water body and bottom mud and the basic physicochemical properties of the bottom mud so as to determine the pollution amount;
(2) after being cleaned and cut, the activated carbon felt is put into an anode chamber of a double-chamber electrochemical anaerobic reactor, and functional bacteria such as enriched anaerobic electrogenesis bacteria and the like are cultured under the condition of a closed external circuit. Or the screening and enrichment speed of the microorganisms is accelerated by applying bias voltage (-400mV, vs. calomel electrode). In an enrichment reactor which runs stably, the enrichment can be completed within 1 to 2 weeks, and the bioelectrochemical anode of the device is manufactured with a metal mesh after the enrichment is completed;
(3) vertically inserting a bioelectrochemical anode into the bottom mud of the culture pond, wherein the bioelectrochemical anode is positioned 10cm below a mud-water interface, so that a bioelectrochemical cathode floats on the water body of the culture pond and is adjacent to an aeration device of the culture pond; connecting a wire with the bioelectrochemical anode and the bioelectrochemical cathode, and connecting a resistor to construct a bioelectrochemical device;
(4) in the starting stage of the bioelectrochemical device, an external circuit (namely, the circuit connection between the cathode and the anode) is placed in an open circuit for 2 to 3 days, the open-circuit voltage is monitored, and when the open-circuit voltage reaches 500mV, the external circuit is closed;
(5) monitoring the pollutant concentration change of the water body and the bottom mud of the culture pond, and removing the device when the treatment target is reached; when the potential difference between the two poles of the bioelectrochemical device is lower than 200mV, which indicates that the electricity generation performance of the electrochemically active microorganisms is reduced, the bioelectrochemical anode is preferably re-enriched with anaerobic microorganisms or moved to a new substrate sludge area to be treated.
Application example 1
The test device adopts organic glass, is configured into a hollow cylindrical single-chamber bioelectrochemical system, has an inner diameter of 24cm and a height of 150cm (including a base height of 200cm), is respectively filled with a bottom mud layer of 25cm and an upper water layer (of 25cm, 50cm and 75cm respectively) from bottom to top, adopts artificial water distribution according to the components of the water in the aquaculture pond, is vertically arranged, and simulates the longitudinal environment of the actual aquaculture pond. The structure of the bioelectrochemical device is as above, the bioelectrochemical anode material is an activated carbon felt (a circle with a diameter of 20 cm) wrapped by double-layer stainless steel wire meshes on two surfaces, and the monolithic bioelectrochemical anode is horizontally placed in the middle of the bottom mud layer and is 15cm below the mud-water interface. In the bioelectrochemical cathode, honeycomb activated carbon fiber cotton with the thickness of 20cm and the pore diameter of 30PPI is adopted, and a stainless steel metal mesh is used as a substrate. The cathode and the anode are connected by a titanium wire with the thickness of 1mm, and a 1000 omega resistor is connected.
Establishing a plurality of groups of treatment experiments, and analyzing the feasibility and key influence factors of the bioelectrochemical technical method for coupling and purifying the bottom sediment and the water body of the aquaculture pond through researches on the types of carbon sources in the bottom sediment, the conductivity characteristics of the overlying water, the starting method of the bioelectrochemical device and the like.
Glucose, sodium acetate, soluble starch and microcrystalline cellulose are respectively added into bottom mud of the device, 1g of substrate is added into each liter of bottom mud to be used as an energy substrate of the bioelectrochemical anode, and in the experiment, the depth of an overlying water layer is 25 cm. The result shows that the glucose and sodium acetate treatment group presents a high potential difference of 500-600 mV in the first 3 days and then rapidly drops, and the potential of the two poles of the glucose and sodium acetate treatment group slowly drops and is maintained between 200-300 mV in a continuous monitoring period lasting for 2 months; while the electricity production performance of the starch and cellulose treatment groups increased slowly and the potential difference was kept around 500mV for approximately 4 months. The experiment shows that the anode microorganism of the bioelectrochemical device can degrade and utilize a carbon source to generate electricity, open-circuit voltage between two electrodes of the device can be rapidly increased by additionally adding glucose or sodium acetate in the starting stage of the device, and the bioelectrochemical device is also beneficial to long-period electricity generation performance.
The proportion (mud-water ratio, namely depth ratio) of the overlying water to the bottom mud also has a remarkable influence on the bioelectrochemical performance, the potential difference between the cathode and the anode is monitored in real time under the condition of the thickness of 25cm of the bottom mud, the corresponding maximum potential differences are 603mV, 510mV and 369mV when the overlying water is 25cm, 50cm and 75cm in a period of continuous monitoring for 2 months, and the deeper the overlying water is, the larger the mass transfer resistance is, the lower the activity of electrochemically active microorganisms is, which means that the potential difference between the two poles is reduced and the electricity generation performance is reduced. However, the depth of the overlying water is not too shallow so as to prevent oxygen from entering the bioelectrochemical anode area to influence the anaerobic condition of the anode and inhibit the activity of microorganisms, and generally, the depth of the overlying water is not less than 15cm, so that the anaerobic environment of the bottom mud can be well maintained.
When the bottom sludge contains refractory organic matters (such as polycyclic aromatic hydrocarbon and the like), the pollutants accumulated in the bottom sludge can be efficiently degraded by the bioelectrochemical anode. Under the condition that 1:1 sludge-water ratio is adopted and 1g of soluble starch is added into each liter of bottom sludge to serve as a carbon source substance, three kinds of polycyclic aromatic hydrocarbons (naphthalene, acenaphthene and pyrene) are dissolved by acetone and mixed into the bottom sludge, the concentration of the polycyclic aromatic hydrocarbons is 1g/L, and the removal effect of the bioelectrochemical device on the three kinds of polycyclic aromatic hydrocarbons is researched. Experimental research shows that the bioelectrochemistry cathode-anode potential difference and the weak current of an external circuit can greatly promote the degradation of naphthalene, acenaphthene and pyrene in the sediment, compared with a processing group with an external circuit disconnected, a closed circuit with a 1000 omega resistor is connected to increase the removal rates of naphthalene, acenaphthene and pyrene from 35.1%, 15.1% and 13.7% to 76.1%, 65.3% and 56.2% respectively, so that the high-efficiency pollution purification capacity is presented, the high-efficiency removal of organic matters in the sediment, particularly refractory organic matters can reduce the water pollution caused by the diffusion of pollutants in the sediment. Meanwhile, the floating bed part can realize the nitrogen and phosphorus removal of the overlying water through the metabolism of aerobic microorganisms and the absorption of plants, and realize the coupling purification of the bottom mud and the overlying water.
Claims (1)
1. A method for coupling and purifying bottom mud and a water body of an aquaculture pond, which is characterized in that a bioelectrochemical device for coupling and purifying the bottom mud and the water body of the aquaculture pond is utilized, and the device comprises: the bioelectrochemical anode is arranged in the bottom mud of the aquaculture pond, and the bioelectrochemical cathode floats on the water body of the aquaculture pond, and is connected with the bioelectrochemical cathode through a lead; wherein the bioelectrochemical anode comprises two metal meshes and an activated carbon felt sandwiched between the two metal meshes; the bioelectrochemical cathode comprises a metal supporting net, conductive sponge is covered on the metal supporting net for planting aquatic plants, the bioelectrochemical anode is formed by stacking a plurality of anode monomers connected with resistors, the conductive sponge is of a porous structure, the thickness of the conductive sponge is 2-5 cm, the pore diameter of the conductive sponge is 20-50 PPI, the projection area ratio of the cathode to the anode is 1: 1-1: 2, and the bioelectrochemical cathode is arranged in a floating bed; the method comprises the following steps:
(1) the method comprises the following steps of (1) horizontally or vertically inserting a bioelectrochemical anode after anaerobic microorganisms are enriched into bottom mud of an aquaculture pond, enabling a bioelectrochemical cathode to float on a water body of the aquaculture pond, connecting the bioelectrochemical anode and the bioelectrochemical cathode, removing organic pollutants in the bottom mud of the aquaculture pond, and purifying the water body;
(2) in the starting stage of the bioelectrochemical device, an external circuit is placed for 2 to 3 days in an open circuit mode, the open circuit voltage is monitored, when the open circuit voltage reaches 500mV, the external circuit is closed, and in the starting stage of the device, the open circuit voltage between two electrodes of the device is increased by additionally adding glucose or sodium acetate;
(3) monitoring the concentration change of pollutants in the water body and the bottom mud of the culture pond, and removing the device when the treatment target is reached, wherein the bioelectrochemical anode is positioned below a mud-water interface by 15cm when horizontally placed; when the bioelectrochemical anode is vertically placed, the sludge interface is below 10cm, all the bioelectrochemical anodes are vertically inserted into the bottom sludge of the aquaculture pond at equal intervals, the bioelectrochemical cathode is adjacent to the aeration device of the aquaculture pond, and when the potential difference between the two poles of the bioelectrochemical device is lower than 200mV, the bioelectrochemical anode is used for re-enriching anaerobic microorganisms or moving to a new bottom sludge area to be treated.
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