CN215403308U - Bioelectrochemical electrode with arc-shaped structure and bioelectrochemical device for treating refractory wastewater - Google Patents
Bioelectrochemical electrode with arc-shaped structure and bioelectrochemical device for treating refractory wastewater Download PDFInfo
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Abstract
The utility model discloses a bioelectrochemical electrode with an arc structure and application thereof, comprising an anode and a cathode which are oppositely arranged, wherein at least one arc sub-electrode is respectively formed on the anode and the cathode; in the anode and the cathode, the central angle of each arc sub-electrode is independently 60-180 degrees; and a bioelectrochemical device for treating refractory wastewater, which adopts the bioelectrochemical electrode with the arc-shaped structure; this bioelectrochemical electrode with arc structure has not only promoted biocompatibility, can effectively get rid of dead and dead bacterial and foreign bacteria, discarded object under the effect of rivers moreover, and then promoted the formation and the stability of electrochemical activity bacterium biomembrane, its negative and positive poles of the earth can also set up more closely simultaneously, electron transfer efficiency between the electrode has been accelerated, obtain higher current density, thereby make this electrode can be applied to in the middle of the preliminary treatment of difficult degradation waste water, can promote the biodegradability of waste water effectively.
Description
Technical Field
The utility model relates to the technical field of microbial electrochemistry, in particular to a bioelectrochemical electrode with an arc-shaped structure and a bioelectrochemical device for treating refractory wastewater.
Background
As a sustainable development technology that combines wastewater treatment and energy generation, the bioelectrochemical system has shown great potential in pretreatment of refractory wastewater. The working principle is that the anode electrochemical activity bacteria of the system oxidize organic substrates in the wastewater to generate electrons, and then the electrons are transferred to the cathode through an external circuit to act on the reduction reaction of the refractory substances, so that the aim of efficiently removing the refractory pollutants is fulfilled. Meanwhile, when additional voltage is applied, the degradation of organic matters in the wastewater can be directionally strengthened. Therefore, the system has the advantages of low applied energy, high processing efficiency and the like.
The electrode is a key part of the structure and the function of a bioelectrochemical system, and can promote the electrochemically active bacteria to carry out electron transfer, thereby accelerating the degradation of pollutants which are difficult to degrade. The anode provides a site for metabolism of electrochemically active microorganisms and reduces the cathode potential through anode reaction, thereby indirectly affecting the degradation efficiency of the contaminants. The cathode acts as an electron donor, directly affecting the reduction efficiency of the refractory contaminants. Like the anode, the cathode also has a significant effect on the biofilm formed by the microbe-electrode interaction. In general, the electrode surface reactions depend to a large extent on the properties of the electrode material used. In the past decades, electrodes have been made mainly of carbon-based materials, such as carbon brushes, carbon cloth, carbon fiber felt, graphite particles, etc., which have characteristics of large specific surface area, corrosion resistance, good biocompatibility, and high stability. Meanwhile, many reports have been made on studies on changing the characteristics of stainless steel materials by using methods such as nitrogen doping, carbon nanotube loading, conductive polymer modification and the like. However, the traditional carbon-based material and the modified stainless steel electrode have the defects of poor economic feasibility and the like, so that the traditional carbon-based material and the modified stainless steel electrode are difficult to apply to the actual large-scale pretreatment of the refractory wastewater, and have the problems of low biological retentivity, poor treatment efficiency and the like.
SUMMERY OF THE UTILITY MODEL
The present invention is directed to overcoming the disadvantages of the prior art and providing an improved bioelectrochemical electrode having an arc structure capable of improving the biodegradability of refractory wastewater, which solves one or more of the problems of the prior art described above and provides at least one advantageous alternative or creation.
The utility model also provides a bioelectrochemical device for treating refractory wastewater, which comprises the bioelectrochemical electrode with the arc-shaped structure, wherein the anode and the cathode respectively extend along the vertical direction.
In order to achieve the purpose, the utility model adopts the technical scheme that:
a bioelectrochemical electrode with an arc-shaped structure comprises an anode and a cathode which are oppositely arranged, wherein at least one arc-shaped sub-electrode is respectively formed on the anode and the cathode; and in the anode and the cathode, the central angle of the arc sub-electrode is 60-180 degrees independently.
According to some preferred aspects of the present invention, the central angle of each of the arc type sub-electrodes is independently 120 ° to 180 °.
In the utility model, if the central angle of each arc-shaped sub-electrode is less than 60 degrees, the improvement on the biological retention is not obvious, meanwhile, the biocompatibility is poor, and the formation of an electrochemical active bacterial biofilm is difficult to promote well; if the central angle of each arc-shaped sub-electrode is larger than 180 degrees, dead strains, impurity bacteria, suspended particles and the like are accumulated, the enrichment of electrochemical active bacteria is hindered, and the electron transfer rate is seriously reduced.
According to some preferred aspects of the utility model, at least two arc-shaped sub-electrodes are respectively formed on the anode and the cathode, and a linear electrode is formed between every two adjacent arc-shaped sub-electrodes in the anode and the cathode, so that the linear electrode can avoid interference between the adjacent arc-shaped sub-electrodes, and meanwhile, the position can be reserved for fixing the anode and the cathode in the later period.
According to some preferred aspects of the utility model, the anode and the cathode are parallel to each other.
According to some preferred aspects of the utility model, the distance between the anode and the cathode is 0.001-3 mm.
According to some preferred aspects of the utility model, the bioelectrochemical electrode further comprises an insulating plastic barrier disposed between the anode and the cathode.
According to some preferred aspects of the utility model, the insulating plastic barrier layer has a thickness of 0.001-3 mm.
According to some preferred aspects of the utility model, the anode, the insulating plastic interlayer and the cathode are sequentially laminated.
In the utility model, the distance between the anode and the cathode can be determined by the thickness of the insulating plastic interlayer, namely when the anode, the insulating plastic interlayer and the cathode are sequentially superposed and attached, the distance between the anode and the cathode is the thickness of the insulating plastic interlayer; the insulating plastic interlayer can prevent the anode and the cathode from being directly short-circuited in the use process, and can improve the stability of the overall relative position relation.
According to some preferred aspects of the present invention, the bioelectrochemical electrode further comprises a fixing member for fixing the anode, the cathode and the insulating plastic barrier relatively, and the fixing member is made of an insulating material.
In some embodiments of the utility model, the fixing member may be an insulated plastic tie, which is fixed by punching holes in the insulated plastic tie.
According to some preferred aspects of the present invention, the anode and the cathode are made of stainless steel fiber felt, which is more economical and corrosion resistant than conventional carbon-based electrodes; compared with the common stainless steel mesh, the stainless steel mesh has better biocompatibility and conductivity; and the economy is good, the acquisition is simple, and the operability is strong. In some embodiments of the utility model, the stainless steel fiber mat may be a type 316 stainless steel fiber mat with a 400 μm filter fineness.
The utility model provides another technical scheme that: a bioelectrochemical device for treating refractory wastewater, which comprises the bioelectrochemical electrode with the arc-shaped structure, wherein the anode and the cathode respectively extend along the vertical direction.
According to some preferred aspects of the present invention, the bioelectrochemical electrode is disposed in an anaerobic reactor; more preferably, the anaerobic reactor is an up-flow anaerobic sludge bed with an aspect ratio of 5-15: 1.
Due to the application of the technical scheme, compared with the prior art, the utility model has the following advantages:
based on the problems of poor economic feasibility, poor biological retentivity, poor treatment efficiency and the like of the bioelectrochemical electrode in the prior art, the utility model innovatively provides an improved cathode and anode provided with arc-shaped sub-electrodes, limits the central angle of each arc-shaped sub-electrode to be 60-180 degrees independently, improves the biocompatibility of the electrode, can effectively remove dead bacteria, impurity bacteria and suspended particles under the action of water flow, further promotes the formation and stability of an electrochemically active bacterial biofilm, can be arranged closer to each other, accelerates the electron transfer efficiency between the electrodes, obtains higher current density, so that the electrode can be applied to the pretreatment of refractory wastewater, and can effectively improve the biodegradability of the wastewater, the burden of treatment is relieved for the back-end biological treatment stage.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings used in the description of the embodiments or the prior art will be briefly described below, and it is obvious that the drawings in the following description are only some embodiments of the present invention, and for those skilled in the art, other drawings can be obtained according to these drawings without inventive exercise.
FIG. 1 is a schematic structural view of a bioelectrochemical electrode having an arc-shaped structure according to example 1 of the present invention;
FIG. 2 is an enlarged schematic view of FIG. 1 at A;
wherein, in example 1, an anode; 2. a cathode; 3. an insulating plastic barrier layer; 4. an insulating plastic tie; a1, arc-type sub-electrode of anode; a2, arc-type sub-electrode of cathode; b1, a linear electrode of the anode; b2, linear electrode of cathode; central angle, α;
FIG. 3 is a schematic structural view of a bioelectrochemical electrode having an arc-shaped structure according to example 2 of the present invention;
among them, example 2, 1', anode; 2', a cathode; 3', insulating plastic interlayer; 4', an insulating plastic ribbon; central angle, α';
FIG. 4 is a schematic structural view of a bioelectrochemical electrode having an arc-shaped structure according to example 3 of the present invention;
wherein, in example 2, 1 ", anode; 2', a cathode; 3', an insulating plastic interlayer; 4', an insulating plastic ribbon; central angle, α ".
Detailed Description
In order to make the aforementioned objects, features and advantages of the present invention comprehensible, embodiments accompanied with figures are described in detail below. 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, "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.
In the present application, unless expressly stated or limited otherwise, the first feature may be directly on or directly under the second feature or indirectly via intermediate members. Also, a first feature "on," "over," and "above" a second feature may be directly or diagonally above the second feature, or may simply indicate that the first feature is at a higher level than the second feature. A first feature being "under," "below," and "beneath" a second feature may be directly under or obliquely under the first feature, or may simply mean that the first feature is at a lesser elevation than the second feature.
It will be understood that when an element is referred to as being "secured to" or "disposed on" another element, it can be directly on the other element or intervening elements may also be present. When an element is referred to as being "connected" to another element, it can be directly connected to the other element or intervening elements may also be present.
Preferred embodiments of the present invention will be described in detail below with reference to the accompanying drawings.
Based on the problems of poor economic feasibility, poor biological retentivity, poor treatment efficiency and the like of the bioelectrochemical electrode in the prior art, the utility model innovatively provides a bioelectrochemical electrode with an arc-shaped structure, which comprises an anode and a cathode which are oppositely arranged, wherein at least one arc-shaped sub-electrode is respectively formed on the anode and the cathode; and the central angle of each arc-type sub-electrode in the anode and the cathode is independently 60-180 degrees, preferably 120-180 degrees.
In the utility model, if the central angle of each arc-shaped sub-electrode is less than 60 degrees, the improvement on the biological retention is not obvious, meanwhile, the biocompatibility is poor, and the formation of an electrochemical active bacterial biofilm is difficult to promote well; if the central angle of each arc-shaped sub-electrode is larger than 180 degrees, dead strains, impurity bacteria, waste and the like can be accumulated, the enrichment of electrochemical active bacteria is hindered, and the electron transfer rate can be seriously reduced.
Preferably, at least two arc-shaped sub-electrodes are respectively formed on the anode and the cathode, and a linear electrode is formed between every two adjacent arc-shaped sub-electrodes in the anode and the cathode, so that the linear electrode can avoid interference between the adjacent arc-shaped sub-electrodes, and meanwhile, the positions of the anode and the cathode can be reserved for later fixing.
Preferably, the anode and the cathode are parallel to each other, and the distance between the anode and the cathode is 0.001-3 mm.
Preferably, the bioelectrochemical electrode further comprises an insulating plastic interlayer arranged between the anode and the cathode, the thickness of the insulating plastic interlayer is 0.001-3mm, and the anode, the insulating plastic interlayer and the cathode are sequentially laminated.
In the utility model, the distance between the anode and the cathode can be determined by the thickness of the insulating plastic interlayer, namely when the anode, the insulating plastic interlayer and the cathode are sequentially superposed and attached, the distance between the anode and the cathode is the thickness of the insulating plastic interlayer; the insulating plastic interlayer can prevent the anode and the cathode from being directly short-circuited in the use process, and can improve the stability of the overall relative position relation.
Furthermore, the bioelectrochemical electrode also comprises a fixing piece used for relatively fixing the anode, the cathode and the insulating plastic interlayer, and the fixing piece is made of insulating materials. Specifically, the fixing piece can be an insulating plastic binding belt which is fixed through a perforation.
Preferably, the anode and the cathode are made of stainless steel fiber felts, and the stainless steel fiber felts are more economical and corrosion resistant compared with the traditional carbon-based electrode; compared with the common stainless steel mesh, the stainless steel mesh has better biocompatibility and conductivity; and the economy is good, the acquisition is simple, and the operability is strong. In some embodiments of the utility model, the stainless steel fiber mat may be a type 316 stainless steel fiber mat with a 400 μm filter fineness.
The utility model also provides application of the bioelectrochemical electrode with the arc-shaped structure, and the bioelectrochemical electrode is applied to a bioelectrochemical device for treating refractory wastewater, the device comprises the bioelectrochemical electrode, and the anode and the cathode respectively extend along the vertical direction.
Preferably, the bioelectrochemical electrode is disposed in an anaerobic reactor; more preferably, the anaerobic reactor is an upflow anaerobic sludge blanket with the height-diameter ratio of 5-15: 1, and the bioelectrochemical electrode with the arc-shaped structure can be matched with the upflow anaerobic sludge blanket with the larger height-diameter ratio, and the matching effect is more excellent.
Specifically, in the present invention, the bioelectrochemical electrode having the arc-shaped structure (hereinafter also referred to as a bioelectrochemical electrode formed with the arc-shaped sub-electrode) may be prepared by a conventional method, for example, by cutting a stainless steel fiber felt to a specific requirement, then pressing and roughly shaping by using a cylindrical roller to form a stainless steel fiber felt electrode having an arc-shaped side surface, and finally fixing the stainless steel fiber felt electrode with an insulating plastic interlayer and cutting an excess portion.
Meanwhile, the bioelectrochemical electrode with the arc-shaped sub-electrode is applied to a bioelectrochemical device for treating refractory wastewater by adopting the following method, and the method specifically comprises the following steps:
1) pretreating the bioelectrochemical electrode with the arc-shaped sub-electrode: firstly, washing surface impurities with deionized water, naturally drying, then placing in an acetone solution for soaking for 12 hours, after the electrode is dried in the air, placing in a 5% sulfuric acid solution for soaking for 2 hours, finally cleaning with deionized water, and placing in a clean place for later use.
2) Constructing a bioelectrochemical system: and (2) placing the bioelectrochemical electrode which is processed in the step (1) and is provided with the arc-shaped sub-electrode into a bioelectrochemical reactor such as an up-flow anaerobic sludge bed, leading out a section of lead by a titanium wire to be communicated with a direct current power supply, and arranging a constant-value resistor and a reference electrode.
3) Starting a bioelectrochemical system: inoculating anaerobic activated sludge into the reactor, pumping the refractory wastewater into the reactor by a peristaltic pump, and supplying voltage by a direct current power supply to achieve the purpose of improving the biodegradability of the refractory wastewater.
Preferably, the anaerobic activated sludge is obtained from the actual degradation-resistant wastewater UASB, and the sludge concentration is 2000-3000 mg/L; the hydraulic retention time controlled by the peristaltic pump is 12 h; the direct current power supply provides 0.5V voltage; biochemical BOD of the refractory wastewater5/COD＝0.1～0.2。
Specifically, the present invention is further illustrated below with reference to three examples.
Example 1:
constructing a bioelectrochemical electrode formed with an arc-type sub-electrode: the method comprises the steps of selecting a 316-type stainless steel fiber felt with the filtering precision of 400 mu m, cutting the 316-type stainless steel fiber felt into two stainless steel fiber felt pieces with the size of L multiplied by B (length multiplied by width) being 133.8 multiplied by 40mm, pressing one stainless steel fiber felt piece to be roughly shaped by a cylindrical roller with the radius of 20mm, pressing the other stainless steel fiber felt piece to be roughly shaped by a cylindrical roller with the radius of 22mm to form an electrode with an arc-shaped sub-electrode, finally punching and fixing the electrode and an insulating plastic interlayer 3 by an insulating plastic binding belt 4, and further cutting redundant parts.
As shown in fig. 1-2, the overall electrode has 4 arc sub-electrodes (specifically, the anode 1 may be simply referred to as the arc sub-electrode a1 of the anode; and the cathode 2 may be simply referred to as the arc sub-electrode a2 of the cathode) with a radius of 20mm (the cathode 2 has), a radius of 22mm (the anode 1 has), and a central angle α of 60 °; in the anode or the cathode, a linear electrode (specifically, in the anode 1, the linear electrode b1 which can be simply called as the anode; in the cathode 2, the linear electrode b2 which can be simply called as the cathode) is formed between every two adjacent arc-shaped sub-electrodes, and the length of the linear electrode is set to be 10mm in the example; washing impurities on the surface of the electrode by using deionized water, naturally drying the electrode, soaking the electrode in an acetone solution for 12 hours, soaking the electrode in a 5% sulfuric acid solution for 2 hours after the electrode is dried, and finally cleaning the electrode by using the deionized water and placing the electrode in a clean place. Similarly, a piece of insulating plastic interlayer 3 with the thickness D of 2mm and the rest of the insulating plastic interlayer 3 with the same size parameter and the same configuration as the electrodes is placed between the anode and the cathode, and the two electrodes and the insulating plastic interlayer 3 are further fixed by punching holes of an insulating plastic binding belt 4, so that the contact between the electrodes is avoided.
Constructing a bioelectrochemical reactor: the shaped bioelectrochemical electrode formed with the arc-shaped sub-electrode is placed in a bioelectrochemical reactor, a section of lead is led out by a titanium wire with the diameter of 1mm and is communicated with a direct current power supply, and a constant value resistance of 10 omega and a saturated calomel reference electrode are arranged. Starting the bioelectrochemical reactor: inoculating anaerobic activated sludge into UASB (height-diameter ratio of 10) of reactor to make sludge concentration in the reactor reach about 2500mg/L, and using peristaltic pump to make BOD5The refractory wastewater with COD of 0.15 is pumped into a reactor, the hydraulic retention time is controlled to be 12h, and a direct current power supply supplies 0.5V of voltage.
Example 2:
the difference between this example and example 1 is that the size of the cut stainless steel fiber mat is 217.6 × 40mm, 4 arc sub-electrodes with a radius of 20mm and a radius of 22mm are formed in the electrode, and the other steps are the same as those in example 1 (specifically, as shown in fig. 3, the anode is marked with 1 ', the cathode is marked with 2 ', the insulating plastic interlayer is marked with 3 ', the insulating plastic band is marked with 4 ', and the central angle is marked with α ').
Example 3:
this example differs from example 1 in that the cut stainless steel fiber mat had dimensions L × B of 331.3 × 40mm, and the resulting electrode had 4 circular arcs of 20mm radius, 4 circular arcs of 22mm radius and 180 ° central angle; the other steps were as in example 1 (specifically, as shown in FIG. 4, the electrode was identified with an anode 1 ", a cathode 2", an insulating plastic spacer 3 ", an insulating plastic tie 4", and a circle center angle α ").
Monitoring experiment:
the current is recorded by the data recorder once every 10 min; BOD5The COD index monitors the bioelectrochemistry water inlet and outlet samples every day. After the operation of the embodiment 1, the embodiment 2 and the embodiment 3 reaches the stable state, the current is stabilized at 6.25 +/-0.31 mA, 8.47 +/-0.11 mA and 17.86 +/-0.30 mA respectively; BOD5The COD lifting values are stabilized at 0.24 +/-0.04, 0.28 +/-0.02 and 0.33 +/-0.02 respectively.
The results demonstrate that:
in the aspect of output current: the results of the examples show that the bioelectrochemical electrode formed with the arc-type sub-electrode keeps the current output of the whole system at a high level due to the good conductivity and the excellent biological retentivity thereof. Meanwhile, the electrodes with different central angles show different current magnitudes. The bioelectrochemical electrode formed with the arc-shaped sub-electrodes has the inferior arc configurations with the central angles of 60 degrees and 120 degrees, and researches show that with the increase of the central angles, biomembranes formed by electrochemically active bacteria are less prone to be disturbed by water flow, so that the current output by the electrode with the inferior arc configuration increases with the increase of the central angles. While the electrode with the arc configuration of half arc shows the optimal output current (17.86 +/-0.30 mA) and current density (1.78 +/-0.03A/m)2) The semi-arc configuration not only has certain biological retention, but also relieves the problem of low electron transfer rate caused by sludge decay, disintegration and the like. BOD of inlet and outlet water5In the aspect of the COD change, the results of the examples show that the formation ofThe bioelectrochemical electrode of the arc-shaped sub-electrode can further improve the biodegradability of the refractory wastewater due to the good conductivity and the excellent biological retentivity of the bioelectrochemical electrode. Among them, examples 3 BOD exhibited by the bioelectrochemical electrode formed with the half arc type sub-electrode having a central angle of 180 °5the/COD rise value is optimally 0.33 ± 0.02, which is consistent with the high output current it exhibits. The boost values in the remaining embodiments appear to increase as the central angle increases.
In conclusion, the above experimental results show that the bioelectrochemical electrode formed with the arc-shaped sub-electrode has significant advantages in the method for improving biodegradability of refractory wastewater, and particularly, the bioelectrochemical electrode formed with the half-arc-shaped sub-electrode, in which the central angle is 180 °, has unexpected advantages.
The above embodiments are merely illustrative of the technical concept and features of the present invention, and the purpose thereof is to enable those skilled in the art to understand the content of the present invention and implement the utility model, and not to limit the scope of the utility model, and all equivalent changes or modifications made according to the spirit of the present invention should be covered by the scope of the present invention.
Claims (10)
1. A bioelectrochemical electrode with an arc-shaped structure comprises an anode and a cathode which are oppositely arranged, and is characterized in that at least one arc-shaped sub-electrode is respectively formed on the anode and the cathode; and in the anode and the cathode, the central angle of the arc sub-electrode is 60-180 degrees independently.
2. The bioelectrochemical electrode according to claim 1, wherein the central angle of each of the arc type sub-electrodes is independently 120 ° to 180 °.
3. The bioelectrochemical electrode according to claim 1, wherein at least two arc-shaped sub-electrodes are formed on each of the anode and the cathode, and a linear electrode is formed between each two adjacent arc-shaped sub-electrodes of the anode and the cathode.
4. The bioelectrochemical electrode according to claim 1, wherein the anode and the cathode are parallel to each other.
5. The bioelectrochemical electrode according to claim 4, wherein a distance between the anode and the cathode is 0.001 to 3 mm.
6. The bioelectrochemical electrode according to claim 1, 4 or 5, having an arc-shaped structure, further comprising an insulating plastic barrier disposed between the anode and the cathode.
7. The bioelectrochemical electrode according to claim 6, wherein the thickness of the insulating plastic barrier is 0.001 to 3 mm; and/or the anode, the insulating plastic interlayer and the cathode are sequentially superposed and attached.
8. The bioelectrochemical electrode according to claim 6, further comprising a fixing member for fixing the anode, the cathode and the insulating plastic barrier relatively, wherein the fixing member is made of an insulating material.
9. The bioelectrochemical electrode according to claim 1, wherein the anode and the cathode are made of stainless steel fiber felt.
10. A bioelectrochemical device for treatment of refractory wastewater, comprising the bioelectrochemical electrode having an arc-shaped structure according to any one of claims 1 to 9, wherein the anode and the cathode each extend in a vertical direction.
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| CN113023874B (en) * | 2021-04-26 | 2024-02-06 | 江苏苏净集团有限公司 | Bioelectrochemical electrode with arc-shaped structure and application thereof |
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