CN102386431A - Soil microbial fuel cell and method for remediating petroleum hydrocarbon polluted soil - Google Patents
Soil microbial fuel cell and method for remediating petroleum hydrocarbon polluted soil Download PDFInfo
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Abstract
The invention provides a soil microbial fuel cell which is composed of a U-shaped tube and a membrane electrode wrapped on the outside surface of the U-shaped tube, wherein the U-shaped tube is a hollow tube and the tube wall is uniformly distributed with round holes; the membrane electrode comprises a diffusion layer, a carbon basic layer, a cathode, a catalysis layer, a glass fibrous membrane and an anode which are arranged from inside to outside and are wound to form a layered structure; the anode and cathode on the two sides of the U-shaped tube can be connected with each other by a conducting wire, the anode and the cathode are connected with an externally connected resistor through a conducting wire so as to form a cell, the U-shaped tube and the membrane electrode are adhered and sealed, the height of a straight tube section of the U-shaped tube, which is embedded in the polluted soil is same with thickness of the polluted soil. The invention has the following advantages: the fuel cell can provide an electron acceptor in situ for petroleum hydrocarbon degrading bacteria through an external circuit and an anode electrogenesis biomembrane, and thus the degradation of the petroleum hydrocarbon can be accelerated, the fuel cell has simple structure and is easy to put into effect; the polluted soil remediation method can be used for removing the petroleum hydrocarbon out of the soil and also can be used for removing other organic pollutants out of the soil without adding any microbes or exogenous chemical substances to the soil.
Description
Technical field
The present invention relates to the microbiological fuel cell technology, particularly a kind of edaphon fuel cell and the method for repairing petroleum hydrocarbon contaminated soil.
Background technology
Along with the aggravation of development of modern industry and energy demand, the oil demand amount is constantly soaring.In exploitation, transportation, conveying and the smelting process of oil, can't avoid the leakage of petroleum hydrocarbon, cause a large amount of soil by petroleum hydrocarbon contaminated.Contain a large amount of harmful materials in the petroleum hydrocarbon, like benzene series thing, polycyclic aromatic hydrocarbon and other difficult degradation poisonous and harmful substances.Therefore, the reparation of petroleum hydrocarbon contaminated soil has important practical significance.The removal method of petroleum hydrocarbon contaminant mainly comprises chemical method, physics method and bioanalysis at present.Because chemistry and physics method have the cost height and are prone to cause secondary pollution, the reparation of soil petroleum hydrocarbon to adopt bioanalysis to carry out usually.
The method of biological restoration mainly comprises two kinds of biological reinforced (bioaugmentaion) and biostimulations (biostimulation).Biological reinforced is to realize the degraded of pollutant through adding pre-incubated contaminant degradation microbe, and biostimulation then is through in soil, adding nutritive salt (like nitrogenous fertilizer, phosphate fertilizer etc.), biosurfactant, electron acceptor or regulating the biological removal that soil characteristic (like pH, moisture content etc.) realizes pollutant.There is limitation separately in above-mentioned technology: in the biological reinforced process, because microbe is not the indigenous microorganism of contaminated site, the contaminant degradation bacterium that adds after the long-time running might be substituted by other floras gradually and lose the characteristic of contaminant degradation; The biostimulation process need adds chemical agent or changes soil property in soil, there is potential threat in soil ecosystem.
Summary of the invention
The objective of the invention is to above-mentioned existing problems; The method that a kind of edaphon fuel cell is provided and repairs petroleum hydrocarbon contaminated soil provides electron acceptor through external circuit and anode electrogenesis biomembrane for the petroleum hydrocarbon degradation bacterium original position, quickens petroleum hydrocarbon degradation; When this method is used for the biological restoration of contaminated soil; Need in soil, not add any microbe or exogenous chemical substances, also have no energy consumption, be that a kind of brand-new efficient green soil pollution recovery technique obtains electric energy simultaneously.
Technical scheme of the present invention:
A kind of edaphon fuel cell; Constitute by U type pipe and the membrane electrode that is wrapped in U type pipe straight-tube portion outer surface; U type pipe is a hollow tube, and U type tube wall is uniformly distributed with circular hole, and membrane electrode comprises diffusion layer, carbon based layer, negative electrode, Catalytic Layer, glass fibre membrane and anode from inside to outside and twines forms layer structure; Wherein Catalytic Layer is carried on the lateral surface of negative electrode; Two anodes of U type pipe both sides are connected through lead respectively with two negative electrodes, connect and compose battery through lead and outer meeting resistance between anode and the negative electrode, adopt epoxy resin or water-proof silica-gel adhering and sealing between U type pipe and the membrane electrode; The straight-tube portion height that U type pipe is imbedded in the contaminated soil is identical with the pollution soil thickness, and the bent tube section of U type pipe is arranged in uncontaminated soil.
Said U type tubing matter is polymethyl methacrylate, plastics or stainless steel; The diameter of the circular hole of U type tube wall is 5 ㎜, and the spacing of circular hole is 5 ㎜.
Said anode is carbon cloth or the carbon felt that acetone is handled; Negative electrode is the carbon cloth or the carbon felt of polytetrafluoroethylene water-proofing treatment.
Outer meeting resistance is 1000 Ω between said the two poles of the earth.
Said diffusion layer is polytetrafluoroethylene or dimethyl silicone polymer.
Said carbon based layer is the mixture of ptfe emulsion and carbon black, and the mass percent concentration of ptfe emulsion is 40%, and the amount ratio of ptfe emulsion and carbon black is 10-15 μ L/mg.
Said Catalytic Layer is platinum or palladium.
A kind of said edaphon fuel cell is repaired the method for petroleum hydrocarbon contaminated soil, at first battery is imbedded in the contaminated soil, and the upper end of U type hollow tube straight-tube portion is positioned at pollutes outside the soil layer, anode and cathode is connected in the resistance two ends starts battery; When cell voltage stabilized, the rehabilitating soil process begins and makes the electrogenesis microbial enrichment in anode surface, and battery voltage range is 10-800mV; When cell voltage decayed to 5mV, the rehabilitating soil process finished.
Advantage of the present invention is: this U type edaphon fuel cell provides electron acceptor through external circuit and anode electrogenesis biomembrane for the petroleum hydrocarbon degradation bacterium original position, quickens petroleum hydrocarbon degradation, and is simple in structure, easy to implement; When this method is used for the biological restoration of contaminated soil; Need in soil, not add any microbe or exogenous chemical substances; Also has no energy consumption; Be that a kind of brand-new efficient green soil pollution recovery technique obtains electric energy simultaneously, not only can remove the petroleum hydrocarbon in the soil, also can be used for the removal of other organic pollutions in the soil.
Description of drawings
Fig. 1 is this edaphon fuel cell structure sketch map.
Fig. 2 is the film electrode structure enlarged diagram.
Fig. 3 is the ruuning situation of microbiological fuel cell under the different soils moisture content, Fig. 3 (a) for the different soils moisture content down the output electric weight and repair time curve, wherein: 1,2 and 3 to represent soil moisture content respectively be 33%, 28% and 23%; Fig. 3 (b) be in initial 100 hours cell voltage and repair time curve.
Fig. 4 is the degradation rate variation comparison diagram of 33% o'clock total petroleum hydrocarbon for the rehabilitating soil moisture content; 1,2 and 3 pedotheques represented respectively apart from anode surface 0-1cm, 1-2cm and 2-3cm wherein, C1, C 2 and C 3 representatives insert batteries but when not being connected battery circuit apart from the control soil sample of anode surface 0-1cm, 1-2cm and 2-3cm.
Fig. 5 is to use behind the battery concentration change of 4 kinds of main polycyclic aromatic hydrocarbons in the soil at 33% o'clock for the rehabilitating soil moisture content; 1,2 and 3 pedotheques represented respectively apart from anode surface 0-1cm, 1-2cm and 2-3cm wherein; C1, C 2 and C 3 representatives insert batteries but when not being connected battery circuit apart from the control soil sample of anode surface 0-1cm, 1-2cm and 2-3cm, 0 represents initial soil.
Fig. 6 is the variation of using petroleum hydrocarbon degradation bacterium quantity behind the battery at 33% o'clock for the rehabilitating soil moisture content; 1,2 and 3 pedotheques represented respectively apart from anode surface 0-1cm, 1-2cm and 2-3cm wherein, C1, C 2 and C 3 representatives insert batteries but when not being connected battery circuit apart from the control soil sample of anode surface 0-1cm, 1-2cm and 2-3cm.
Among the figure: 1.U type pipe 2. membrane electrodes 3. outer meeting resistances 4. contaminated soils
5. uncontaminated soil 6. diffusion layers 7. carbon based layer 8. negative electrodes 9. Catalytic Layer
10. glass fibre membrane 11. anodes 12. circular holes.
Embodiment
Embodiment:
A kind of edaphon fuel cell; Be made up of U type pipe 1 and the membrane electrode 2 that is wrapped in U type pipe straight-tube portion outer surface, U type pipe 1 is a hollow tube, and U type pipe 1 tube wall is uniformly distributed with circular hole 12; Membrane electrode 2 comprises diffusion layer 6, carbon based layer 7, negative electrode 8, Catalytic Layer 9, glass fibre membrane 10 and anode 11 from inside to outside and twines forms layer structure; Wherein Catalytic Layer 9 is carried on the lateral surface of negative electrode 8, and two anodes 11 of U type pipe 1 both sides are connected through lead respectively with two negative electrodes 8, connect and compose battery through lead and outer meeting resistance 3 between anode 11 and the negative electrode 8; Outer meeting resistance 3 is 1000 Ω; Adopt the adhering with epoxy resin sealing between U type pipe 1 and the membrane electrode 2, the straight-tube portion height that U type pipe 1 is imbedded in the contaminated soil 4 is identical with the pollution soil thickness, and the bent tube section of U type pipe 1 is arranged in uncontaminated soil 5.
Among this embodiment, U type tubing matter is polymethyl methacrylate, and the diameter of U type pipe is 3cm, and the straight-tube portion height is 15cm, and the centerline diameter of bent tube section is 6cm, and the diameter of the circular hole of U type tube wall is 5 ㎜, and the spacing of circular hole is 5 ㎜; Anode is the carbon cloth that acetone is handled; Negative electrode is the carbon cloth of polytetrafluoroethylene water-proofing treatment; Diffusion layer is a polytetrafluoroethylene; Carbon based layer is the mixture of carbon black and polytetrafluoroethylene; Catalyst is a platinum.
Among this embodiment, the preparation method of carbon based layer is: the consumption of carbon black is every square centimeter of negative electrode 1.56mg, and mass percent concentration is that 40% PTFE emulsion consumption is every milligram of carbon dust 12 μ L; PTFE and carbon dust are mixed, evenly be applied to cathode surface, air-dryly be placed in the Muffle furnace 370 ℃ of heating and promptly obtained carbon based layer in 30 minutes.The preparation method of diffusion layer is: with mass percent concentration is that 60% ptfe emulsion evenly is applied to cathode surface, air-dryly is placed on that 370 ℃ of heating promptly obtained diffusion layer in 30 minutes in the Muffle furnace.The preparation method of Catalytic Layer is: the consumption of platinum catalyst is every square centimeter of negative electrode 0.1mg; With mass percent concentration is that 5% perfluor sulfoacid resin solution and catalyst mix are even; Be coated on cathode surface; The consumption of perfluor sulfoacid resin solution is every milligram of catalyst 6.7 μ L, obtains Catalytic Layer after air-dry 24 hours.
This technology is applied to the biological restoration of petroleum hydrocarbon contaminated soil, can carry out according to following scheme.
At first measure the degree of depth and the area of petroleum hydrocarbon contaminated soil, the size of design U type microbiological fuel cell.Prepare membrane electrode with reference to above-mentioned manufacture method, be assembled into battery with U type pipe.Battery is imbedded in the contaminated soil, anode and cathode is connected to the outer meeting resistance two ends, keep higher moisture content in the soil, the minimum of moisture content is 23%.The voltage at periodic measurement resistance two ends is treated to repair when voltage drop is low to moderate 5mV and is finished, and analyzes repairing effect.
1) U type microbiological fuel cell is repaired the performance of different water cut rate soil:
Soil moisture content is the key factor that influences U type microbiological fuel cell performance.In order to investigate the performance of the present invention in different water cut rate soil, our parallel startup 8 the soil batteries of knowing clearly, the soil moisture content of setting is followed successively by 33% (soil saturation moisture content), 28% and 23%, 2 of every kind of parallel startups of battery.In addition, also open circuit operation 2 moisture content be that 33% battery is as contrast.Tried soil and take from the Dagang Oilfield, Tianjin City, be petroleum hydrocarbon contaminated topsoil, total petroleum hydrocarbons content is 28.3mg/kg, and soil texture classification results is a light clay.Fig. 3 (a) for the different soils moisture content down the output electric weight and repair time curve, wherein: 1,2 and 3 to represent soil moisture content respectively be 33%, 28% and 23%; Can be found out by Fig. 3 (a): along with the raising of soil moisture content, the electric weight of soil battery output significantly increases.In 25 days test process, the electric weight of battery output is followed successively by 125 ± 7C (moisture content 33%), 35 ± 3C (moisture content 28%) and 15 ± 2C (moisture content 23%).Fig. 3 (b) be in initial 100 hours cell voltage and repair time curve, show among the figure: the start battery process is shorter relatively, only needs just can to obtain about 50h stable voltage output (resistance 1000 Ω).
2) the degraded situation of petroleum hydrocarbon behind the use edaphon fuel cell:
Behind 25 days degradation experiment,, mix back testing total petroleum hydrocarbon degradation rate at each galvanic anode surface 0-1cm, 1-2cm and 2-3cm difference collection soil sample.Fig. 4 is the degradation rate variation comparison diagram of 33% o'clock total petroleum hydrocarbon for the rehabilitating soil moisture content; 1,2 and 3 pedotheques represented respectively apart from anode surface 0-1cm, 1-2cm and 2-3cm wherein, C1, C 2 and C 3 representative representatives insert batteries but when not being connected battery circuit apart from the control soil sample of anode surface 0-1cm, 1-2cm and 2-3cm.Show among the figure: near the total petroleum hydrocarbon degradation rate the anode in the soil is compared with the open circuit operation battery, is elevated to 15.2 ± 0.6 % by 6.9 ± 2.5 %, has improved 120%.Polycyclic aromatic hydrocarbon in the petroleum hydrocarbon (PAH) is a noxious substance the most representative in the petroleum hydrocarbon, and it is present in the petroleum hydrocarbon contaminated soil, has greatly threatened health.Fig. 5 is to use behind the battery concentration change of 4 kinds of main polycyclic aromatic hydrocarbons in the soil at 33% o'clock for the rehabilitating soil moisture content; Comprise fluorenes, phenanthrene, pyrene and in the wrong; 1,2 and 3 pedotheques represented respectively apart from anode surface 0-1cm, 1-2cm and 2-3cm wherein; C1, C 2 and C 3 representatives insert batteries but when not being connected battery circuit apart from the control soil sample of anode surface 0-1cm, 1-2cm and 2-3cm, 0 represents initial soil.Show among the figure: after using U type microbiological fuel cell that petroleum hydrocarbon contaminated soil is repaired, can see that the PAH near the soil of anode reduces significantly.This explanation the present invention not only can quicken the biological restoration of soil PetroChina Company Limited. hydrocarbon, also can effectively remove the noxious substance in the soil simultaneously.
3) the edaphon fuel cell is to the influence of petroleum hydrocarbon degradation bacterium quantity:
Fig. 6 is the variation of using petroleum hydrocarbon degradation bacterium quantity behind the battery at 33% o'clock for the rehabilitating soil moisture content; 1,2 and 3 pedotheques represented respectively apart from anode surface 0-1cm, 1-2cm and 2-3cm wherein, C1, C 2 and C 3 representatives insert batteries but when not being connected battery circuit apart from the control soil sample of anode surface 0-1cm, 1-2cm and 2-3cm.Show among the figure: through 25 days degradation experiment, in connecting the reactor of circuit, near the soil of electrode (<1cm) PetroChina Company Limited.'s alkane degradation bacterium (HDB) quantity is 373 ± 56 * 10
3CFU/g-soil, comparison is according to exceeding 2 one magnitude, and the insertion that shows microbiological fuel cell can promote the growth of HDB, quickened the decomposition rate of soil petroleum hydrocarbon.
When implementing, the present invention can repair means, as adding nutrient, adding contaminant degradation bacterium etc. and the coupling of phytoremediation means with other microbes.
Claims (8)
1. edaphon fuel cell; It is characterized in that: constitute by U type pipe and the membrane electrode that is wrapped in U type pipe straight-tube portion outer surface; U type pipe is a hollow tube, and U type tube wall is uniformly distributed with circular hole, and membrane electrode comprises diffusion layer, carbon based layer, negative electrode, Catalytic Layer, glass fibre membrane and anode from inside to outside and twines forms layer structure; Wherein Catalytic Layer is carried on the lateral surface of negative electrode; Two anodes of U type pipe both sides are connected through lead respectively with two negative electrodes, connect and compose battery through lead and outer meeting resistance between anode and the negative electrode, adopt epoxy resin or water-proof silica-gel adhering and sealing between U type pipe and the membrane electrode; The straight-tube portion height that U type pipe is imbedded in the contaminated soil is identical with the pollution soil thickness, and the bent tube section of U type pipe is arranged in uncontaminated soil.
2. according to the said edaphon fuel cell of claim 1, it is characterized in that: said U type tubing matter is polymethyl methacrylate, plastics or stainless steel; The diameter of the circular hole of U type tube wall is 5 ㎜, and the spacing of circular hole is 5 ㎜.
3. according to the said edaphon fuel cell of claim 1, it is characterized in that: said anode is carbon cloth or the carbon felt that acetone is handled; Negative electrode is the carbon cloth or the carbon felt of polytetrafluoroethylene water-proofing treatment.
4. according to the said edaphon fuel cell of claim 1, it is characterized in that: outer meeting resistance is 1000 Ω between said the two poles of the earth.
5. according to the said edaphon fuel cell of claim 1, it is characterized in that: said diffusion layer is polytetrafluoroethylene or dimethyl silicone polymer.
6. according to the said edaphon fuel cell of claim 1; It is characterized in that: said carbon based layer is the mixture of ptfe emulsion and carbon black; The mass percent concentration of ptfe emulsion is 40%, and the amount ratio of ptfe emulsion and carbon black is 10-15 μ L/mg.
7. according to the said edaphon fuel cell of claim 1, it is characterized in that: said Catalytic Layer is platinum or palladium.
8. edaphon fuel cell method of repairing petroleum hydrocarbon contaminated soil according to claim 1; It is characterized in that: at first battery is imbedded in the contaminated soil; The upper end of U type hollow tube straight-tube portion is positioned at pollutes outside the soil layer, anode and cathode is connected in the resistance two ends starts battery; When cell voltage stabilized, the rehabilitating soil process begins and makes the electrogenesis microbial enrichment in anode surface, and battery voltage range is 10-800mV; When cell voltage decayed to 5mV, the rehabilitating soil process finished.
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