• 专利附录
  • 专利说明
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    • 专利摘要:
    The present disclosure relates to the field of microbial electrochemical technology, in particular to a working electrode for degrading petroleum hydrocarbons, and a device 5 for degrading petroleum hydrocarbons and application thereof. The working electrode for degrading petroleum hydrocarbons provided in the present disclosure, comprising a conductive substrate, the working surface of the conductive substrate is composed of a conductive region and an etched region; the conductive region and the conductive substrate are concentric circles, and the diameter of the conductive substrate is larger 10 than the diameter of the conductive region; the etched region is a circular ring; the sum of the diameter of the conductive region and the wall thickness of the etched region is the same as the diameter of the conductive substrate, the etched region includes a groove region and a non-groove region; the grooves in the groove region are arranged at intervals in a radial direction, an electroactive microorganism is grown on the surface of 15 the conductive region, and the electroactive microorganism includes petroleum hydrocarbon degrading microorganism, and the groove region is laid with magnetite. The application of the working electrode in MET eXpands the remediation range of electroactive microorganisms and further strengthens the degradation efficiency of degrading petroleum hydrocarbons. 20
    公开号:NL2029412A
    申请号:NL2029412
    申请日:2021-10-14
    公开日:2022-02-16
    发明作者:Zhou Qixing；Zhang Xiaolin；Li Tian；Li Ruixiang
    申请人:Univ Nankai；
    IPC主号:
    专利说明:

    [01] [01] The present disclosure relates to the field of microbial electrochemical technology, in particular to a working electrode for degrading petroleum hydrocarbons, and a device for degrading petroleum hydrocarbons and application thereof.BACKGROUND ART
    [02] [02] At present, the irrational exploitation and utilization of oil fields can lead to serious petroleum pollution problems.. The erosion of ground oil and the leakage of oil transportation pipelines have caused the pollution of petroleum to the soil. With the infiltration and migration of petroleum in the soil, petroleum will gradually pollute surface water and groundwater, resulting in a decrease in dissolved oxygen in water and causing a serious threat to aquatic ecosystems. Therefore, solving the pollution problem of petroleum hydrocarbon in water has become a research hotspot of general concern in various countries.
    [03] [03] Due to the anaerobic characteristics of water polluted by petroleum hydrocarbons, anaerobic microbial remediation technology has become one of the important technologies for the degradation of petroleum hydrocarbons. However, due to the lack of electron acceptors in the anaerobic environment, the enrichment of anaerobic microorganisms is slow, resulting in unsatisfactory degradation efficiency. However, with the rise of microbial electrochemical technology (MET) at the end of the last century, new methods have been provided to supplement electron acceptors in anaerobic environments to accelerate the enrichment of anaerobic microorganisms. In 2008, Morris and Jin et al. (Morris JM, Jin S. Feasibility of using microbial fuel cell technology for bioremediation of hydrocarbons in groundwater. Journal of Environmental Science and Health Part A, 2008, 43: 18-23.) used MET to complete the conversion of C8-C25 petroleum hydrocarbon into small molecules within 21 days in groundwater, and the remediation efficiency was increased by 51%, which provided the possibility of anaerobic microbial remediation of petroleum hydrocarbons in water. At the same time, it 1s found that the reason that MET can improve the remediation efficiency is that the enrichment of electroactive microorganisms can induce the enrichment of petroleum hydrocarbon degrading microorganisms.
    [04] [04] However, in the current MET, electroactive microorganisms are mainly enriched on the electrode, so the remediation range is greatly limited. Only petroleum hydrocarbon molecules around the electrode within 1 cm can be remediated because of the enrichment of electroactive microorganisms, and after a long time of enrichment of the electroactive microorganisms on the electrode, due to the thickening of the electroactive microbial film, the mass transfer 1s affected, and the electricity generation performance is also greatly affected, which further limits the degradation process of petroleum hydrocarbons.SUMMARY
    [05] [05] The purpose of the present disclosure is to provide a working electrode for degrading petroleum hydrocarbons, and a device for degrading petroleum hydrocarbons and application thereof. The application of the working electrode in MET expands the remediation range of electroactive microorganisms and further strengthens the degradation efficiency of degrading petroleum hydrocarbons.
    [06] [06] In order to achieve the above purpose of the disclosure, the present disclosure provides the following technical schemes:
    [07] [07] The present disclosure provides a working electrode for degrading petroleum hydrocarbons, wherein comprising a conductive substrate;
    [08] [08] The working surface of the conductive substrate is composed of a conductive region and an etched region; the conductive region and the conductive substrate are concentric circles, and the diameter of the conductive substrate is larger than the diameter of the conductive region;
    [09] [09] The etched region is a circular ring; the sum of the diameter of the conductive region and the wall thickness of the etched region is the same as the diameter of the conductive substrate;
    [10] [10] The etched region includes a groove region and a non-groove region; the grooves inthe groove region are arranged at intervals in a radial direction;
    [11] [11] An electroactive microorganism is grown on the surface of the conductive region, and the electroactive microorganism includes petroleum hydrocarbon degrading microorganism; the groove region is laid with magnetite.
    [12] [12] Preferably, the ratio of the diameter of the conductive substrate to the diameter of the conductive region is (1-4) : 1.
    [13] [13] Preferably, the number of grooves in the groove region is 8-10.
    [14] [14] Preferably, the diameter of the groove is 40-60 nm.
    [15] [15] Preferably, calculated according to the value of OD600, the enrichment of the electroactive microorganisms in the conductive region is 3.5-4.5.
    [16] [16] The present disclosure also provides a device for degrading petroleum hydrocarbons, comprising a working electrode, a counter electrode and a power source;
    [17] [17] The working electrode is the working electrode described in the above technical scheme.
    [18] [18] The present disclosure also provides the application of the device described in the above technical scheme in the field of degrading petroleum hydrocarbons.
    [19] [19] Preferably, the degradation of petroleum hydrocarbons includes degradation of sediments or petroleum hydrocarbons in sewage.
    [20] [20] Preferably, the application method comprises the following steps:
    [21] [21] After placing the deposits containing petroleum hydrocarbons in the etched region of the working electrode, placing the device for degrading petroleum hydrocarbons in a buffer solution, and energizing for degrading;
    [22] [22] Or placing the device for degrading petroleum hydrocarbons in sewage containing petroleum hydrocarbons, and energizing for degrading.
    [23] [23] Preferably, the energized voltage is 0.3-0.5 V.
    [24] [24] The present disclosure provides a working electrode for degrading petroleum hydrocarbons, comprising a conductive substrate; the working surface of the conductive substrate is composed of a conductive region and an etched region; the conductive region and the conductive substrate are concentric circles, and the diameter of the conductive substrate is larger than the diameter of the conductive region; the etched region is a circular ring; the sum of the diameter of the conductive region and the wall thickness of the etched region is the same as the diameter of the conductive substrate, the etched region includes a groove region and a non-groove region; the grooves in the groove region are arranged at intervals in a radial direction; an electroactive microorganism is grown on the surface of the conductive region, and the electroactive microorganism includes petroleum hydrocarbon degrading microorganism; the groove region is laid with magnetite. In the present disclosure, by designing the etched region, and setting a groove containing magnetite in the etched region, the enrichment and enrichment range of electroactive microorganisms can be enhanced by using the mediating effect of magnetite, so as to expand the degradation range, thus forming a long-distance electron transfer network, and achieving efficient degradation of petroleum hydrocarbons at the distal end of the electrode.BRIEF DESCRIPTION OF THE DRAWINGS
    [25] [25] FIG. 1 is a schematic diagram of the structure of the working electrode for degrading petroleum hydrocarbons according to the present disclosure; wherein, 1- conducting region, 2-etched region, and 3-groove;
    [26] [26] FIG. 2 is a schematic diagram of the structure of the device for degrading petroleum hydrocarbons according to the present disclosure; wherein, 4-working electrode according to the present disclosure, 5-counter electrode, and 6-power source;
    [27] [27] FIG. 3 is the current curve of the working electrode for degrading petroleum hydrocarbons described in Example 1 and Comparative Example 1;
    [28] [28] FIG. 4 shows the degradation rate of the working electrode for degrading petroleum hydrocarbons described in Example 1 and Comparative Example 1 during the degradation process;
    [29] [29] FIG. 5 is a schematic diagram of the working principle of the working electrode for degrading petroleum hydrocarbons according to the present disclosure, wherein, 7- electroactive microorganisms, 8-electrons, 9-petroleum hydrocarbon degrading 5 microorganism, and 10-petroleum hydrocarbons.DETAILED DESCRIPTION OF THE EMBODIMENTS
    [30] [30] The present disclosure provides a working electrode for degrading petroleum hydrocarbons, comprising a conductive substrate; [BI] The working surface of the conductive substrate is composed of a conductive region and an etched region; the conductive region and the conductive substrate are concentric circles, and the diameter of the conductive substrate is larger than the diameter of the conductive region;
    [32] [32] The etched region is a circular ring; the sum of the diameter of the conductive region and the wall thickness of the etched region is the same as the diameter of the conductive substrate;
    [33] [33] The etched region includes a groove region and a non-groove region; the grooves in the groove region are arranged at intervals in a radial direction;
    [34] [34] The electroactive microorganisms are grown on the surface of the conductive region, and the electroactive microorganism includes petroleum hydrocarbon degrading microorganism; the groove region is laid with magnetite.
    [35] [35] The present disclosure does not have any special restrictions on the material of the conductive substrate, and a material well known to those skilled in the art can be used. In an embodiment of the present disclosure, the conductive substrate is specifically conductive glass.
    [36] [36] In the present disclosure, the ratio of the diameter of the conductive substrate to the diameter of the conductive region is preferably (1-4) : 1, more preferably (2-3) : 1, and most preferably 2 : 1. The present disclosure does not have any special restrictions on the diameter of the conductive substrate, and those skilled in the art can adjust it according to the actual scale of the object to be processed.
    [37] [37] In the present disclosure, the number of grooves in the groove region is preferably 8-10, and more preferably 9. In the present disclosure, the grooves are preferably arranged uniformly. In the present disclosure, the diameter of the groove is preferably 40-60 nm, more preferably 45-55 nm, and most preferably 50 nm.
    [38] [38] In the present disclosure, calculated according to the value of OD600, the enrichment of the electroactive microorganisms in the conductive region is 3.5-4.5, more preferably 3.8-4.2, and most preferably 4.0.
    [39] [39] The present disclosure does not have any special restrictions on the electroactive microorganisms and petroleum hydrocarbon degrading microorganisms, a type well- known to those skilled in the art can be used.
    [40] [40] In the present disclosure, the magnetite is preferably nano-magnetite; the particle size of the nano-magnetite is preferably smaller than the diameter of the groove.
    [41] [41] In the present disclosure, the working electrode for degrading petroleum hydrocarbons degrades petroleum hydrocarbons on a principle that the electroactive microorganisms and petroleum hydrocarbon degrading microorganism that are enriched in the conductive region are coexisting. The petroleum hydrocarbon degrading microorganism can degrade the petroleum hydrocarbon macromolecules on the outer edge of the conductive region into small molecules through redox reactions, and the small molecules are used as a carbon source by the electroactive microorganisms to generate electric signals, and magnetite is laid on the etched region to form a conductive path. The electroactive microorganisms and petroleum hydrocarbon degrading microorganism will grow along the direction of magnetite. Through the process of long- distance electron transfer, the petroleum hydrocarbon molecules at the distal end are degraded for electricity generation (as shown in FIG. 5).
    [42] [42] In the present disclosure, the preparation method of the working electrode for degrading petroleum hydrocarbon preferably includes the following steps:
    [43] [43] Providing a conductive substrate with a working surface including a conductive region and an etched region;
    [44] [44] Etching grooves in the etched region to obtain the electrode;
    [45] [45] Using the electrode as the working electrode, platinum sheet or steel mesh as the counter electrode, energizing in a suspension containing electroactive microorganisms, and after the electroactive microorganisms are enriched in the conductive region, laying magnetite in the groove to obtain the working electrode for degrading petroleum hydrocarbons.
    [46] [46] The present disclosure provides a conductive substrate with a working surface including a conductive region and an etched region; the present disclosure does not have any special restrictions on the source of the conductive substrate, and a source well known to those skilled in the art can be used. For example, after a circular substrate is selected, the conductive layer is deposited with the center of the substrate as the center in accordance with the size ratio of the conductive region to the substrate described in the above technical scheme.
    [47] [47] In the present disclosure, grooves are etched in the etched region to obtain electrodes; the present disclosure does not have any special restrictions on the process of etching the grooves, and a process well known to those skilled in the art can be used to achieve the requirements for the diameter and arrangement of the grooves in the above technical schemes. In a specific embodiment of the present disclosure, the etching method is specifically laser etching.
    [48] [48] In the present disclosure, after the electrode is obtained, the electrode is used as the working electrode, the platinum sheet or steel mesh is used as the counter electrode, energizing is carried out in a suspension containing electroactive microorganisms, and after the electroactive microorganisms are enriched in the conductive region, magnetite is laid in the groove to obtain the working electrode for degrading petroleum hydrocarbons.
    [49] [49] In the present disclosure, the working surfaces of the working electrode and the counter electrode are parallel to the horizontal plane.
    [50] [50] In the present disclosure, the suspension containing electroactive microorganisms includes 1 g / L sodium acetate, and the OD600 of the suspension containing electroactive microorganisms is 0.2-0.6.
    [51] [51] In the present disclosure, the energized voltage is preferably 0.3-0.5 V, and more preferably 0.4 V; the time is preferably 6-8 days, and more preferably 7 days.
    [52] [52] After the conductive region is enriched with electroactive microorganisms, the present disclosure also preferably includes a process of cleaning the groove. In the present disclosure, the cleaning solution used for cleaning the groove is preferably an ethanol solution; the present disclosure does not have any special restrictions on the ethanol solution, and an ethanol solution well known to those skilled in the art can be used.
    [53] [53] The present disclosure does not have any special limitations on the process of laying magnetite, and a process well known to those skilled in the art can be used.
    [54] [54] The present disclosure also provides a device for degrading petroleum hydrocarbons, including a working electrode, a counter electrode and a power source; [SS] The working electrode is the working electrode described in the above technical scheme.
    [56] [56] In the present disclosure, the counter electrode is preferably a platinum sheet or steel mesh.
    [57] [57] In the present disclosure, the power source is preferably a DC power source.
    [58] [58] The present disclosure also provides the application of the device described in the above technical scheme in the field of degrading petroleum hydrocarbons.
    [59] [59] Preferably, the degradation of petroleum hydrocarbons includes degradation of sediments or petroleum hydrocarbons in sewage.
    [60] [60] Preferably, the application method includes the following steps:
    [61] [61] After placing the deposits containing petroleum hydrocarbons in the etched region of the working electrode, placing the device for degrading petroleum hydrocarbons in a buffer solution, and energizing for degrading;
    [62] [62] Or placing the device for degrading petroleum hydrocarbons in sewage containing petroleum hydrocarbons, and energizing for degrading.
    [63] [63] In the present disclosure, after placing the deposits containing petroleum hydrocarbons in the etched region of the working electrode, placing the device for degrading petroleum hydrocarbons in a buffer solution, and energizing for degrading;
    [64] [64] In the present disclosure, the deposits containing petroleum hydrocarbons are preferably laid on the etched region of the working electrode; the thickness of the laying is preferably 0.2-0.8 cm, and more preferably 0.5 cm.
    [65] [65] In the present disclosure, the buffer solution is preferably a phosphate buffer solution. The present disclosure does not have any special restrictions on the type of the buffer solution, and a type well known to those skilled in the art can be used to make the pH value of the system within the range of 6.8-7.2.
    [66] [66] In the present disclosure, the energized voltage is preferably 0.3-0.5 V, and more preferably 0.4 V.
    [67] [67] The device for degrading petroleum hydrocarbons is placed in sewage containing petroleum hydrocarbons, and is energized for degradation.
    [68] [68] In the present disclosure, the energized voltage is preferably 0.3-0.5 V, and more preferably 0.4 V.
    [69] [69] The working electrode for degrading petroleum hydrocarbon, the device for degrading petroleum hydrocarbon and application thereof provided by the present disclosure will be described in detail below with reference to the examples, but they should not be understood as limiting the protection scope of the present disclosure.
    [70] [70] Example 1
    [71] [71] According to the structure shown in FIG. 1:
    [72] [72] A conductive glass with a diameter of 5 cm containing a conductive region and an etched region was provided, wherein the diameter of the conductive region was 2.5cm;
    [73] [73] Using a laser, 10 columns of grooves were etched uniformly distributed in a radial direction in the etched region, the diameter of the grooves was 60 nm, and the distance between two adjacent grooves was 0.5 cm to obtain an electrode;
    [74] [74] Using the electrode as the working electrode and the platinum sheet as the counter electrode, the working electrode and the counter electrode were placed in a suspension containing electroactive microorganisms (including lg / L sodium acetate, OD600 =
    [75] [75] The suspension containing electroactive microorganisms was replaced with a phosphate buffer solution (pH = 7.0), the working electrode for degrading petroleum hydrocarbons and platinum sheet were put in the replaced solution, the system was energized, the voltage was adjusted to 0.4 V, and the electrical signals were captured by the wireless current acquisition card in the laboratory, the test results are shown in curve Ain FIG. 3. From the curve Ain FIG. 3, it can be seen that after the 14th day of operation, the current density reaches 8.3 A / m , indicating that the electroactive microorganisms are grown along the laying direction of magnetite, resulting in a greater current density.
    [76] [76] Comparative Example 1
    [77] [77] A conductive glass with a diameter of 5 cm containing a conductive region and an etched region was provided, wherein the diameter of the conductive region was 2.5 cm;
    [78] [78] Using a laser, 10 columns of grooves were etched uniformly distributed in a radial direction in the etched region, the diameter of the grooves was 60 nm, and the distance between two adjacent grooves was 0.5 cm to obtain an electrode;
    [79] [79] Using the electrode as the working electrode and the platinum sheet as the counter electrode, the working electrode and the counter electrode were placed in a suspension containing electroactive microorganisms (including lg / L sodium acetate, OD600 =
    [80] [80] The suspension containing electroactive microorganisms was replaced with a phosphate buffer solution (pH = 7.0), the working electrode for degrading petroleum hydrocarbons and the platinum sheet were put in the replaced solution, the system was energized, the voltage was adjusted to 0.4 V, and the electrical signals were captured by the wireless current acquisition card in the laboratory, the test results are shown in curve B in FIG. 3, it can be seen from the curve B in FIG. 3 that after the 14th day of operation, the current density reaches 7.1 A / m , indicating that without laying magnetite, the electroactive microorganisms are only grown in the conductive region, and the current density does not change anymore.
    [81] [81] Test Example
    [82] [82] 100 g of soil particles with a particle size of 40-60 nm were dipped in an ethanol solution containing Philippines with a mass percentage of 40 % for 30 days to obtain the Philippines-containing soil particles;
    [83] [83] The Philippines-containing soil particles were laid on the etched region of the working electrode for degrading petroleum hydrocarbons described in Example 1 and Comparative Example 1, with a thickness of 0.5 cm, the working electrode for degrading petroleum hydrocarbons with Philippines-containing soil particles was used as the working electrode, the platinum sheet was used as the counter electrode, and in the buffer solution with the pH of 7.0, the system was energized, and the voltage was adjusted to
    [84] [84] During the degradation process, 1 mL of the solution was taken every two days, after passing through a 0.22 pum filter membrane, the absorbance of the solution was measured at a wavelength of 220 nm, and the concentration of the generated small molecule substances degraded Philippines contained in the solution was calculated from the absorbance value., and finally the degradation rate was calculated, wherein the calculation formula is: degradation rate = (initial concentration - final concentration) / initial concentration * 100 %, and remaining rate = 100 % - degradation rate;
    [85] [85] FIG. 4 shows the degradation rate of the working electrode for degrading petroleum hydrocarbons described in Example 1 (curve A) and Comparative Example 1 (curve B) during the degradation process; it can be seen from FIG. 4 that the degradation rate of the electrode for degrading petroleum hydrocarbons described in Example 1 to Philippines on the 2nd, 4th, 6th, 8th, 10th, 12th, 14th and 16th days are 25 %, 45 %, 55%, 58 %, 60 %, 61 %, 62 % and 62 %, respectively, the degradation rate of the working electrode for degrading petroleum hydrocarbons described in Comparative Example 1 to Philippines on the 2nd, 4th, 6th, 8th, 10th, 12th, 14th and 16th days are 10%, 18%, 24%, 27%, 29%, 30%, 30% and 31%, respectively.
    [86] [86] The above are only the preferred embodiments of the present disclosure. It should be pointed out that for those of ordinary skill in the art, without departing from the principle of the present disclosure, several improvements and modifications can be made, and these improvements and modifications should also be regarded as the protection scope of the present disclosure.
    权利要求:
    Claims (10)
    [1]
    Claims L Working electrode for degrading petroleum hydrocarbons, comprising a conductive substrate; wherein a working surface of the conductive substrate is composed of a conductive region and an etched region; wherein the conductive region and the conductive substrate are concentric circles, and a diameter of the conductive substrate is greater than the diameter of the conductive region; wherein the etched area is a circular ring; wherein the sum of the diameter of the conductive region and a wall thickness of the etched region is the same as the diameter of the conductive substrate; wherein the etched area includes a slot area and a non-slot area; wherein the slots in the slot region are arranged at intervals in a radial direction; an electroactive microorganism is grown on the surface of the conductive region, and the electroactive microorganism comprises a microorganism that degrades hydrocarbons from petroleum, wherein the slot region is laid with magnetite.
    [2]
    The working electrode according to claim 1, wherein the ratio of the diameter of the conductive substrate to the diameter of the conductive region (1 - 4): 1 µs.
    [3]
    The working electrode of claim 1, wherein the number of slots in the slot region is 8-101s.
    [4]
    The working electrode of claim 1 or 3, wherein the diameter of the slot is 40-60 nm.
    [5]
    The working electrode of claim 1, wherein, calculated according to the value of OD600, the enrichment of the electroactive microorganisms in the conductive region is 3.5-45.
    [6]
    An apparatus for degrading petroleum hydrocarbons, comprising a working electrode, a counter electrode and a power source;
    -14- wherein the working electrode is the working electrode according to any one of claims 1-5.
    [7]
    Use of the device according to claim 6 in the field of degrading petroleum hydrocarbons.
    [8]
    The use of claim 7, wherein the degradation of petroleum hydrocarbons comprises degradation of sediments or petroleum hydrocarbons in sewage.
    [9]
    The use of claim 8, wherein the application method comprises the steps of: after placing a deposit containing petroleum hydrocarbons in the etched region of the working electrode, placing the petroleum hydrocarbon degrader in a buffer solution, and empowering for degradation; or placing the device for degradation of petroleum hydrocarbons in sewage containing petroleum hydrocarbons, and energizing for degradation.
    [10]
    The use of claim 9, wherein the applied voltage is 0.3 - 0.5 V.
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