CN112661255B - Sleeve type bioelectrochemical reactor for in-situ remediation of chlorohydrocarbon pollution of shallow groundwater - Google Patents
Sleeve type bioelectrochemical reactor for in-situ remediation of chlorohydrocarbon pollution of shallow groundwater Download PDFInfo
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- CN112661255B CN112661255B CN202011477268.6A CN202011477268A CN112661255B CN 112661255 B CN112661255 B CN 112661255B CN 202011477268 A CN202011477268 A CN 202011477268A CN 112661255 B CN112661255 B CN 112661255B
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Abstract
The invention relates to a sleeve type bioelectrochemical reactor for in-situ remediation of shallow groundwater polluted by hydrochloric ether, in particular to a bioelectrochemical reactor for in-situ remediation of shallow groundwater polluted by the hydrochloric ether. The invention utilizes the bioelectrochemistry dehalogenation technology, provides electrons for the dehalogenation breathing bacteria through a biological cathode, promotes the completion of biological dehalogenation breathing, and solves the problem of insufficient exogenous electron donors in underground water. The cathode of the reactor comprises a stainless steel cylinder with uniformly distributed holes on the surface and a carbon felt; the upper section of the bottom cylinder is of a straight cylinder structure, the lower section of the bottom cylinder is of a conical cylinder structure, the edge of the upper section of the bottom cylinder is connected with the stainless steel cylinder, and the check ball is positioned in the lower section of the bottom cylinder; the anode is positioned in the stainless steel cylinder, the PVC pipe is positioned between the anode and the cathode, and the anode and the cathode are electrically connected through an external direct current power supply. The device can be arranged in an in-situ monitoring well with a small caliber, is simple and convenient to operate, and is suitable for the characteristics of complex underground water environment and inconvenient operation conditions.
Description
Technical Field
The invention relates to a sleeve type bioelectrochemical reactor for in-situ remediation of shallow groundwater polluted by chlorohydrocarbon, in particular to a bioelectrochemical reactor for in-situ remediation of shallow groundwater polluted by halohydrocarbon.
Background
Groundwater is an important source of fresh water, is widely distributed and convenient to use, has become a main drinking water source in most countries and regions, and is used as drinking water by more than 20 hundred million people. The population of China accounts for 20% of the total population of China, while the fresh water resource only accounts for 5-7% of the fresh water resource of China, and the underground water resource has important strategic significance on the economic development, social development and civil guarantee of China. In China, more than 400 cities take underground water as drinking water sources, and the underground water accounts for more than 60 percent of the total number of the cities. Particularly, in northern areas of China, about 30% of agricultural water, 50% of industrial water and 60% of domestic water come from underground water. For rural areas in China, domestic drinking water is mainly supplied by underground water. In recent years, the pollution of underground water halogenated hydrocarbons has received great attention worldwide, wherein chlorinated aliphatic hydrocarbons are the most common organic pollutants in underground water, and tetrachloroethylene, trichloroethylene and 1, 2-dichloroethylene are representative pollutants in underground water halogenated hydrocarbons. The geological environment monitoring institute of China investigated the halogenated hydrocarbon pollution conditions of 69 urban groundwater in China, and the investigation result shows that at least one volatile pollutant is detected in 71 percent of urban groundwater. In many cities in the north of China, serious halohydrocarbon pollution exists, wherein PCE (tetrachloroethylene) and TCE (trichloroethylene) are main pollutants. The halogenated hydrocarbons exist in the underground water for a long time and are difficult to naturally degrade, and the artificial treatment is necessary and urgent when the pollution situation of the halogenated hydrocarbons in the underground water is faced.
At present, the technologies for removing halogenated hydrocarbons from underground water mainly comprise adsorption, aeration stripping, zero-valent iron reduction, advanced oxidation, conventional microbial reduction dehalogenation and removal of halogenated hydrocarbon organic matters by a novel bioelectrochemical system. The adsorption is used as a traditional method for removing the halogenated hydrocarbon in the water, the cost is low, the design and the operation are simple, but the adsorption capacity of the adsorbent is limited, and in addition, the adsorption is used as a physical removal method, so that the halogenated hydrocarbon cannot be harmlessly removed, and the subsequent treatment is required. Aeration stripping has a repairing effect on water bodies polluted by volatile organic compounds, but the aeration consumption is high, and tail gas treatment is required when pollutants are contained in the tail gas. At present, it is known that nano metal materials represented by nano zero-valent iron have a good dehalogenation effect on halogenated hydrocarbons, but have the problems of material agglomeration, poor stability, poor fluidity, short service life and the like in practical application. The advanced oxidation technology is mainly Fenton oxidation and ozone oxidation technology, but in the in-situ remediation of underground water, a large amount of chemical agents need to be added, the treatment cost is high, and the advanced oxidation technology is difficult to be applied to the treatment of underground water in a large range. The microbial reduction technology utilizes halogenated hydrocarbon as an electron acceptor in the metabolism process of certain microbes under the anaerobic condition to complete the dehalogenation process of the halogenated hydrocarbon. However, in groundwater, there is a problem of insufficient electron donor, and furthermore, methanogens and denitrifying bacteria and dehalogenating reducing bacteria have a competitive relationship, which greatly limits the effect of conventional microbial reductive dehalogenation. Accordingly, the present invention provides a bioelectrochemical reactor using a bioelectrochemical cathode as an external electron donor to supply electrons to dehalogenating respiring bacteria to promote biological dehalogenation and decomposition and conversion of halogenated hydrocarbons.
Disclosure of Invention
The invention aims to solve the technical problems and provides a preparation method of a sleeve type bioelectrochemical reactor directly applied to an underground water in-situ monitoring well.
The technical scheme of the invention is as follows:
a sleeve type bioelectrochemical reactor used for in-situ remediation of chlorohydrocarbon pollution of shallow groundwater comprises an anode 6, a cathode, a PVC pipe 5, a bottom cylinder 7 and a check ball 8, wherein the cathode comprises a stainless steel cylinder 2 with uniformly distributed holes on the surface and a carbon felt 3, and the carbon felt 3 is adhered to the inner wall of the stainless steel cylinder 2 through conductive adhesive; the bottom cylinder 7 is divided into an upper section and a lower section, the upper section is of a straight cylinder structure, the lower section is of a conical cylinder structure, the edge of the upper section of the bottom cylinder 7 is connected with the lower edge of the stainless steel cylinder 2, and the check ball 8 is positioned in the lower section of the bottom cylinder 7; the positive pole 6 is the brush-shaped structure that carbon fiber and titanium silk winding formed, and positive pole 6 is located stainless steel drum 2, and PVC pipe 5 is located between positive pole 6 and stainless steel drum 2, and positive pole 6 and negative pole realize the electricity through external DC power supply 9 and connect.
Further, the opening ratio of the stainless steel cylinder 2 was 30%.
Furthermore, the diameter of the stainless steel cylinder 2 is 4cm, the length of the stainless steel cylinder is 201cm, upper edge holes are circumferentially formed at positions 5mm away from the upper edge of the stainless steel cylinder 2, the hole diameter is 8mm, and 8 upper edge holes are uniformly distributed along the circumferential direction; a lower edge hole is circumferentially formed at a position 5mm away from the lower edge of the stainless steel cylinder 2, the aperture is 5mm, and 4 lower edge holes are uniformly distributed along the circumferential direction; the holes are uniformly distributed from the position 1.5cm away from the upper edge of the stainless steel cylinder 2 to the lower edge part of the stainless steel cylinder 2, the hole diameter is 1.5cm, 6 holes are uniformly distributed in each row along the circumferential direction, and the minimum distance between adjacent holes in the axial direction is 1cm.
Furthermore, the upper edge holes are used for fixing the reactor and connecting with the negative pole of an external direct current power supply 9, and the upper edge holes are connected in series by using titanium wires in order to ensure that the current distribution is uniform.
Further, the upper segment diameter of a bottom section of thick bamboo 7 is 4cm, highly is 5cm, and 5mm department circumference trompil apart from upper segment top edge, the aperture is 5mm, and along 4 holes of circumference equipartition, the upper segment trompil and the lower limb hole of a bottom section of thick bamboo 7 correspond, and use the titanium silk to pass upper segment trompil and lower limb hole with the connection of a bottom section of thick bamboo 7 and stainless steel drum 2.
Further, the height of the cone structure at the lower section of the bottom cylinder 7 is 5cm, the diameter of the inlet is 4cm, and the diameter of the outlet is 2cm.
Further, the check ball 8 has a diameter of 2.5cm.
Furthermore, the diameter of the PVC pipe 5 is 2.5cm, the length of the PVC pipe is 200cm, holes are evenly distributed on the surface of the PVC pipe, rubber gaskets are respectively sleeved at two ends of the PVC pipe 5, and the PVC pipe 5 is fixed in the stainless steel net 2 through the rubber gaskets.
Further, the diameter of the anode 6 is 2cm, the length of the anode is 201cm, carbon fibers are not wound on the part 1cm away from the top end of the anode 6, and the titanium wires are bent to form holes and used for being connected with the positive electrode of the external direct current power supply 9.
Further, the cathode and anode may be interchanged.
The invention has the following beneficial effects: the invention utilizes the bioelectrochemistry dehalogenation technology, can provide electrons for the dehalogenation respiratory bacteria under the condition of limited electron donor, and promotes the completion of dehalogenation respiration. The reactor can be placed in a small monitoring well, has the characteristics of simple and convenient operation, suitability for complex underground water environment and unchanged operation conditions, does not need to add a large amount of chemical agents, has small voltage (about 1V) required by operation and extremely low energy consumption. When the reactor is operated, microorganisms can be subjected to biofilm formation on a cathode carbon felt, and halohydrocarbon pollutants can be reduced and dehalogenated in a cathode area through the synergistic effect of the electrodes and the microorganisms. The operation of the reactor can maintain the oxidation-reduction potential in the well in a lower range, and is more favorable for the enrichment and proliferation of dehalogenation respiratory microorganisms. In addition, the anode of the reactor can also be used for the oxidative decomposition of partial halohydrocarbon such as cis-1, 2-dichloroethylene and other halohydrocarbon reduction products to realize the complete mineralization of the halohydrocarbon.
Drawings
FIG. 1 is a view showing the structure of an axial section of a sleeve type bioelectrochemical reactor;
FIG. 2 is a schematic structural view of a cathode stainless steel cylinder 2;
FIG. 3 is a schematic view of the structure of the bottom cylinder;
FIG. 4 is a schematic view of an anode structure;
in the figure, 2-a stainless steel cylinder, 3-a carbon felt, 5-a PVC pipe, 6-an anode, 7-a bottom cylinder, 8-a check ball and 9-an external direct current power supply.
Detailed Description
The experimental procedures used in the following examples are conventional unless otherwise specified. The materials, reagents, methods and apparatus used, unless otherwise specified, are conventional in the art and are commercially available to those skilled in the art.
Embodiment mode 1:
as shown in fig. 1, the reactor comprises an anode 6, a cathode, a PVC pipe 5, a bottom cylinder 7 and a check ball 8, wherein the cathode comprises a stainless steel cylinder 2 with uniformly distributed holes on the surface and a carbon felt 3, and the carbon felt 3 is adhered to the inner wall of the stainless steel cylinder 2 through conductive adhesive; the bottom cylinder 7 is divided into an upper section and a lower section, the upper section is of a straight cylinder structure, the lower section is of a conical cylinder structure, the edge of the upper section of the bottom cylinder 7 is connected with the lower edge of the stainless steel cylinder 2, and the check ball 8 is positioned in the lower section of the bottom cylinder 7; the anode 6 is a brush-shaped structure formed by winding carbon fibers and titanium wires, the anode 6 is positioned in the stainless steel cylinder 2, the PVC pipe 5 is positioned between the anode 6 and the stainless steel cylinder 2, and the anode 6 and the cathode are electrically connected through an external direct current power supply 9. So set up, the reactor is the sleeve type, arranges in the water, is the unicompartment for the water, but has PVC between the negative and positive poles to cut off a section of thick bamboo, can see as the bicompartment again. The PVC pipe 5 ensures the relative independence of the cathode and the anode and ensures the diffusion of pollutants in the water body to the working electrode. And the reactor can change the design size according to the size of the underground water monitoring well and is put into the well for in-situ repair. Meanwhile, an external direct current power supply can adjust different voltages, so that the cathode and the anode reach different potentials, and the potentials and electrons are provided for degrading the halogenated hydrocarbon by the microorganisms.
As shown in fig. 2, the diameter of the stainless steel cylinder 2 is 4cm, the length is 201cm, the upper edge holes are circumferentially opened at a distance of 5mm from the upper edge of the stainless steel cylinder 2, the aperture is 8mm, and 8 upper edge holes are uniformly distributed along the circumferential direction, the upper edge holes are used for fixing the reactor and are connected with the negative pole of the external direct current power supply 9, and the upper edge holes are connected in series by using titanium wires to ensure that the current is uniformly distributed. Lower edge hole is opened to 5mm department circumference apart from the lower limb of stainless steel drum 2, and the aperture is 5mm, and along 4 lower edge holes of circumference equipartition, this lower limb is used for being connected with end section of thick bamboo 7. The holes are uniformly distributed from the position 1.5cm away from the upper edge of the stainless steel cylinder 2 to the lower edge part of the stainless steel cylinder 2, the aperture is 1.5cm, 6 holes are uniformly distributed in each row along the circumferential direction, and the minimum distance between adjacent holes in the axial direction is 1cm. So set up, when stainless steel drum 2 was as negative pole supporting material, reinforcing negative pole electric conductivity, and its inner wall surface passes through conducting resin adhesion carbon felt 3, utilizes the porosity and the better water permeability of its carbon felt 3, when increasing the negative pole surface, provides more attached area for the microorganism, and the negative pole top edge uses the titanium silk with carbon felt 3 and stainless steel drum 2 along a section of thick bamboo inboard winding together, makes electric current evenly distributed.
And the aperture ratio of the cathode stainless steel cylinder 2 is 30%, so that the influence on the electric conduction effect caused by overlarge resistance due to too many apertures is avoided while the internal water permeability is ensured.
As shown in figure 3, the diameter of the upper section of the bottom cylinder 7 is 4cm, the height is 5cm, the circumferential opening is arranged at the position 5mm away from the upper edge of the upper section, the aperture is 5mm, 4 holes are uniformly distributed along the circumferential direction, the upper section opening of the bottom cylinder 7 corresponds to the lower edge hole, a titanium wire penetrates through the upper section opening and the lower edge hole to connect the bottom cylinder 7 and the stainless steel cylinder 2, the height of the conical cylinder structure at the lower section of the bottom cylinder 7 is 5cm, the inlet diameter is 4cm, and the outlet diameter is 2cm. So set up, the reactor bottom is for dismantling end section of thick bamboo 7 and check ball 8, and the mud of subsiding and the biomembrane that drops can be stayed wherein, can also carry the water sample simultaneously, are convenient for survey water sample and microorganism growth condition.
The pipe diameter of PVC pipe 5 is 2.5cm, and length is 200cm, and evenly arranges the hole on its surface, the both ends of PVC pipe 5 suit packing ring respectively, PVC pipe 5 realizes its rigidity in stainless steel drum 2 through the packing ring, prevents that PVC pipe 5 from rocking in stainless steel drum 2. So set up, adopt foraminiferous PVC pipe 5 to cut off between the negative and positive poles to it is fixed to add the rubber washer, when guaranteeing negative and positive poles ion exchange, prevents the short circuit.
As shown in FIG. 4, the anode 6 is a brush-shaped structure formed by winding carbon fibers and titanium wires, the diameter of the structure is 2cm, the length of the structure is 201cm, the carbon fibers are not wound at the part 1cm away from the top end of the anode 6, and the titanium wires are bent to form a hole for connecting with the positive electrode of the external DC power supply 9. With the arrangement, the brush-shaped structure formed by winding the carbon fibers and the titanium wires on the anode 6 increases the surface area of the anode, enhances the conductive capacity and reduces the limitation of the anode on the working electrode. And the brush-shaped structure of the anode 6 has conductivity and can also load microorganisms, when needed, the cathode and the anode can be exchanged, the carbon felt is used as the anode, the carbon brush is used as the cathode, the surface area of the cathode is improved, and meanwhile, the PVC pipe 5 can reduce the leakage of sludge and ensure the contact of the microorganisms and the carbon brush.
When the reactor is operated, the microorganisms can carry out biofilm formation on the cathode carbon felt. The halocarbon contaminants are subjected to reductive dehalogenation in the cathodic region by the synergistic action of the electrodes and the microorganisms. The anode can also be used for the oxidative decomposition of partial halohydrocarbon such as cis-1, 2-dichloroethylene and other halohydrocarbon reduction products to realize the complete mineralization of pollutants.
The reactor is of a single-chamber structure, can be placed in a small monitoring well, is simple and convenient to operate, is suitable for the characteristics of complex underground water environment and unchanged operating conditions, does not need to add a large amount of chemical agents, and is low in voltage (about 1V) required by operation and extremely low in energy consumption.
Those skilled in the art can make other changes and modifications within the spirit of the invention, which are suitable for various practical situations, and such changes and modifications within the spirit of the invention are intended to be included within the scope of the invention as claimed.
Claims (9)
1. A sleeve type bioelectrochemical reactor for in-situ remediation of chlorohydrocarbon pollution of shallow groundwater is characterized by comprising an anode (6), a cathode, a PVC pipe (5), a bottom cylinder (7) and check balls (8), wherein the cathode comprises a stainless steel cylinder (2) with uniformly distributed holes on the surface and a carbon felt (3), and the carbon felt (3) is adhered to the inner wall of the stainless steel cylinder (2) through conductive adhesive; the bottom cylinder (7) is divided into an upper section and a lower section, the upper section is of a straight cylinder structure, the lower section is of a conical cylinder structure, the edge of the upper section of the bottom cylinder (7) is connected with the lower edge of the stainless steel cylinder (2), and the check ball (8) is positioned in the lower section of the bottom cylinder (7); the anode (6) is a brush-shaped structure formed by winding carbon fibers and titanium wires, the anode (6) is positioned in the stainless steel cylinder (2), the PVC pipe (5) is positioned between the anode (6) and the cathode, and the anode (6) and the cathode are electrically connected through an external direct current power supply (9);
the PVC pipe (5) has a pipe diameter of 2.5cm and a length of 200cm, and holes are uniformly distributed on the surface;
the cathode and the anode (6) can work simultaneously, and an oxidation area and a reduction area are formed in the same system.
2. The sleeve type bioelectrochemical reactor according to claim 1, characterized in that said stainless steel cylinder (2) has an open area ratio of 30%.
3. The sleeve type bioelectrochemical reactor according to claim 1 or 2, wherein the diameter of the stainless steel cylinder (2) is 4cm, the length of the stainless steel cylinder is 201cm, an upper edge hole is formed in the position 5mm away from the upper edge of the stainless steel cylinder (2) along the circumferential direction, the hole diameter is 8mm, and 8 upper edge holes are uniformly distributed along the circumferential direction; a lower edge hole is circumferentially formed at a position 5mm away from the lower edge of the stainless steel cylinder (2), the aperture is 5mm, and 4 lower edge holes are uniformly distributed along the circumferential direction; the holes are uniformly distributed from the position 1.5cm away from the upper edge of the stainless steel cylinder (2) to the lower edge part of the stainless steel cylinder (2), the hole diameter is 1.5cm, 6 holes are uniformly distributed in each row along the circumferential direction, and the minimum distance between adjacent holes in the axial direction is 1cm.
4. The sleeve type bioelectrochemical reactor according to claim 3, characterized in that the upper edge holes are used for fixing the reactor and connecting with the negative electrode of an external DC power supply (9), and 8 upper edge holes are connected in series by using titanium wires to ensure uniform current distribution.
5. The sleeve type bioelectrochemical reactor according to claim 3, wherein the diameter of the upper section of the bottom cylinder (7) is 4cm, the height of the bottom cylinder is 5cm, a circumferential hole is formed at a position 5mm away from the upper edge of the upper section, the hole diameter is 5mm, 4 holes are uniformly distributed along the circumferential direction, the upper section of the bottom cylinder (7) corresponds to the lower edge hole, and a titanium wire is used for connecting the bottom cylinder (7) with the stainless steel cylinder (2) through the upper section of the hole and the lower edge hole.
6. The sleeve type bioelectrochemical reactor according to claim 3, characterized in that the height of the cone structure at the lower section of the bottom cylinder (7) is 5cm, the inlet diameter is 4cm, and the outlet diameter is 2cm.
7. The telescopic bioelectrochemical reactor for in-situ remediation of chlorinated hydrocarbon pollutants in shallow groundwater according to claim 3, characterized in that the diameter of the check ball (8) is 2.5cm.
8. The sleeve type bioelectrochemical reactor according to claim 3, wherein the two ends of the PVC pipe (5) are respectively sleeved with a rubber gasket, and the PVC pipe (5) is fixed in position in the stainless steel cylinder (2) through the rubber gaskets.
9. The sleeve type bioelectrochemical reactor according to claim 1, wherein the diameter of the anode (6) is 2cm, the length of the anode is 201cm, a part 1cm away from the top end of the anode (6) is not wound with carbon fiber, and a titanium wire is bent to form a hole for connecting with the anode of an external direct current power supply (9).
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