CN103934260B - Method for repairing petroleum-polluted soil by using electrochemical device and synchronously generating electricity - Google Patents
Method for repairing petroleum-polluted soil by using electrochemical device and synchronously generating electricity Download PDFInfo
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- CN103934260B CN103934260B CN201410140586.1A CN201410140586A CN103934260B CN 103934260 B CN103934260 B CN 103934260B CN 201410140586 A CN201410140586 A CN 201410140586A CN 103934260 B CN103934260 B CN 103934260B
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Abstract
The invention discloses a method for repairing petroleum-polluted soil by using an electrochemical device and synchronously generating electricity. The method comprises the following steps: (1) assembling an electrochemical device; (2) mixing the petroleum-polluted soil with distilled water to obtain a mixture, then adding the mixture into the electrochemical device, separating four layers of soil respectively by carbon fiber cloth anodes, leading out by taking a titanium sheet as lead wire, and gathering the three paths of anodes; (3) injecting the water for sealing the layers, connecting compound PTFE (Polytetrafluoroethylene) air cathodes and the gathered carbon fiber cloth anodes respectively through the lead wire and external resistors to form a soil microbial fuel cell, and automatically recording voltages on the external resistors through an electrochemical collection card and a computer; and (4) operating the microbial fuel cell for 180 days at the temperature of 30 DEG C, repairing the petroleum-polluted soil and synchronously generating electric energy. The method has the advantages that the electrochemical device is simple in structure, convenient to operate and easy to implement, capable of degrading petroleum pollutants by using indigenous organisms in the soil and recycling the electric energy, and significant in technical effects and promotional value.
Description
Technical field
The present invention relates to the reparation of oil-polluted soils, particularly a kind of method adopting electrochemical appliance remedying oil-polluted soils synchronous electrogenesis.
Background technology
Along with the continuous increase of Petroleum Production and consumption figure, in its exploitation, process and utilize in process, the continuous entered environment of a large amount of petroleum substances, ecological safety in serious threat.According to estimates, about there is 6 × l0 in China every year
8kg oil entered environment by all means, ended for the end of the year 2003, and petroleum industry solid waste heap high-volume reaches 1.9 × lO
10kg, floor space is 1.8 × 1O about
6m
2, produce oil-polluted soils nearly 1 × 10 per year
8kg, accumulation heap high-volume reaches 5 × l0
8kg.Petroleum pollution is in soil, and spoiled soil structure, affects the permeability of soil, changes the Nomenclature Composition and Structure of Complexes of the soil organism, cause the change of soil microbial community quantity and structure, thus safety and the sustainability of the ecosystem in serious threat.
At present, the recovery technique of oil-polluted soils mainly comprises physical method, chemical method and microbial process.Employed physico-chemical techniques conventional at present comprises concentrated mummification method, solid-liquid isolation method, extraction separation method, douche, heat treatment and thermal desorption technology, chemical demulsification absorption method etc.These methods mainly reclaim for greasy filth Crude Oil and set up, and the application in soil remediation is also ripe not to the utmost.Microorganism remediation technology comprises dystopy process and the large class of in-situ treatment two.Dystopy microorganism remediation technology mainly comprises Anaerobic Treatment method, bioreactor, compost type process etc.; Original position microorganism remediation technology mainly comprises throws bacterium method, biological culture method, bioventing process, agro-farming method etc.This method is comparatively large by such environmental effects, and input cost is higher.
Summary of the invention
The object of the invention is for above-mentioned existing problems, a kind of method adopting electrochemical appliance remedying oil-polluted soils synchronous electrogenesis is provided, adopt this device to not adding any chemicals such as surfactant, nutrient and bacteria agent in oil-polluted soils reparation, utilize autochthons in soil by petroleum pollution degradation, and reclaim electric energy simultaneously.
Technical scheme of the present invention:
Adopt a method for electrochemical appliance remedying oil-polluted soils synchronous electrogenesis, step is as follows:
1) assembling of electrochemical appliance
Electrochemical appliance is made up of lucite casing, carbon cloth anode and compound polytetrafluoroethylene (PTFE) (PTFE) air cathode assembly, lucite casing is the cuboid with flange frame bottom upper and lower opening also, bottom half is provided with base plate and is supported by four supporting legs, and the part that base plate connects with air cathode is evenly equipped with that diameter is 0.5cm, pitch of holes is the circular hole of 1cm, carbon cloth anode carbon cloth is placed in acetone to soak 8 hours, cleans 3 times obtain after taking-up with distilled water, compound polytetrafluoroethylene (PTFE) (PTFE) air cathode assembly is by compound polytetrafluoroethylene (PTFE) (PTFE) air cathode and its, the plastic pad combination that bottom is respectively equipped with is formed and is fixed by the bolt of surrounding, on, the square hole size at lower plastic pad center is identical with the lumenal cross-section of lucite casing, wherein compound polytetrafluoroethylene (PTFE) (PTFE) air cathode preparation method is: take conductive carbon black 4g and add in 200mL beaker, add 80mL absolute ethyl alcohol, stir and ultrasonic 5min, add the PTFE emulsion that 6.2mL density is 1.5g/mL, stir and ultrasonic 5min, then 40min is about in 80 DEG C of stirring in water bath, take out micelle gently to rub, it is 0.5mm electrode slice that roll squeezer is rolled into thickness with 60 order stainless (steel) wires, then at 340 DEG C, 25min is heated stand-by, taking electric capacity carbon dust 6g adds in 200mL beaker, add 45mL absolute ethyl alcohol, stir and ultrasonic 5min, add 0.670mL PTFE emulsion, stir again and ultrasonic 5min, be then about 3h in 80 DEG C of stirring in water bath, take out micelle and gently rub, be pressed in the opposite side of electrode slice after being rolled into film, final thickness of electrode is 0.6mm,
2) oil pollution soil is dried in the shade naturally, ground 2mm sieve, after taking 320.00g oil pollution soil powder mixing with 90mL distilled water, be divided into 6 parts, tile 1 part at the 4th layer of soil, 2 parts are tiled at the 3rd layer of soil, tile 2 parts at the 2nd layer of soil, tile 1 part at the 1st layer of soil, soil separates with carbon cloth anode between layers respectively, draw as wire by titanium sheet, three road carbon cloth anodes are converged;
3) with syringe 20mL distilled water injected on the 1st layer of soil and form water seal layer, compound polytetrafluoroethylene (PTFE) (PTFE) air cathode is connected with 1000 Ω external resistances respectively by wire with the carbon cloth anode converged, composition edaphon fuel cell, the voltage in external resistance is by electrochemistry capture card and the automatic record of computer;
4) make above-mentioned edaphon fuel cell run 180d at 30 DEG C under keeping water seal layer condition, complete the reparation of oil-polluted soils and produce electric energy simultaneously.
Advantage of the present invention is: this electrochemical appliance structure is simple, easy to operate, easy to implement, adopt this device to not adding any chemicals such as surfactant, nutrient and bacteria agent in oil-polluted soils reparation, utilize the autochthons in soil by petroleum pollution degradation and reclaim electric energy simultaneously, there is significant technique effect and promotional value.
Accompanying drawing explanation
Fig. 1 is electrochemical appliance structural representation.
Fig. 2 is electrochemical appliance sectional structure schematic diagram.
Fig. 3 is voltage pattern and the electricity figure of electrochemical appliance generation.
Fig. 4 is the degradation rate figure of total petroleum hydrocarbon in the soil after utilizing electrochemical appliance to repair.
Fig. 5 be in the soil after utilizing electrochemical appliance to repair 16 kinds of polycyclic aromatic hydrocarbons containing spirogram.
Fig. 6 is alkane (C in the soil after utilizing electrochemical appliance to repair
8-C
40) containing spirogram and degradation rate figure.
Detailed description of the invention
Embodiment:
Adopt a method for electrochemical appliance remedying oil-polluted soils synchronous electrogenesis, step is as follows:
1) assembling of electrochemical appliance
Electrochemical appliance, as shown in Figure 1 and Figure 2, be made up of lucite casing, carbon cloth anode and compound polytetrafluoroethylene (PTFE) (PTFE) air cathode assembly, lucite casing is the cuboid with flange frame bottom upper and lower opening also, bottom half is provided with base plate and is supported by four supporting legs, and the part that base plate connects with air cathode is evenly equipped with that diameter is 0.5cm, pitch of holes is the circular hole of 1cm, carbon cloth anode carbon cloth is placed in acetone to soak 8 hours, cleans 3 times obtain after taking-up with distilled water, compound polytetrafluoroethylene (PTFE) (PTFE) air cathode assembly is by compound polytetrafluoroethylene (PTFE) (PTFE) air cathode and its, the plastic pad combination that bottom is respectively equipped with is formed and is fixed by the bolt of surrounding, on, the square hole size at lower plastic pad center is identical with the lumenal cross-section of lucite casing, wherein compound polytetrafluoroethylene (PTFE) (PTFE) air cathode preparation method is: take conductive carbon black 4g and add in 200mL beaker, add 80mL absolute ethyl alcohol, stir and ultrasonic 5min, add the PTFE emulsion that 6.2mL density is 1.5g/mL, stir and ultrasonic 5min, then 40min is about in 80 DEG C of stirring in water bath, take out micelle gently to rub, it is 0.5mm electrode slice that roll squeezer is rolled into thickness with 60 order stainless (steel) wires, then at 340 DEG C, 25min is heated stand-by, taking electric capacity carbon dust 6g adds in 200mL beaker, add 45mL absolute ethyl alcohol, stir and ultrasonic 5min, add 0.670mL PTFE emulsion, stir again and ultrasonic 5min, be then about 3h in 80 DEG C of stirring in water bath, take out micelle and gently rub, be pressed in the opposite side of electrode slice after being rolled into film, final thickness of electrode is 0.6mm,
2) oil pollution soil is dried in the shade naturally, ground 2mm sieve, after taking 320.00g oil pollution soil powder mixing with 90mL distilled water, be divided into 6 parts, tile 1 part at the 4th layer of soil, 2 parts are tiled at the 3rd layer of soil, tile 2 parts at the 2nd layer of soil, tile 1 part at the 1st layer of soil, soil separates with carbon cloth anode between layers respectively, draw as wire by titanium sheet, three road carbon cloth anodes are converged;
3) with syringe 20mL distilled water injected on the 1st layer of soil and form water seal layer, compound polytetrafluoroethylene (PTFE) (PTFE) air cathode is connected with 1000 Ω external resistances respectively by wire with the carbon cloth anode converged, composition edaphon fuel cell, the voltage in external resistance is by electrochemistry capture card and the automatic record of computer;
4) make above-mentioned edaphon fuel cell run 180d at 30 DEG C under keeping water seal layer condition, complete the reparation of oil-polluted soils and produce electric energy simultaneously.
Experiment detects:
1) laboratory sample prepares: taken out by layer soil of four in said apparatus, puts into the dry 24h of vacuum freeze drier, pulverizes 100 mesh sieves, and obtained powdered sample.
2) electrochemical appliance produce voltage pattern and electricity figure detect:
Adopt this electrochemical appliance in the repair process of 180d, the electric energy reclaimed as shown in Figure 3, show in figure: this edaphon fuel cell is maximum at the voltage of the 5th day, up to 366mV, maintain more than 360mV about 9h, within 30th day, voltage drop is to below 100mV, within the 82nd day, drops to below 50mV, after this continues to decline.At the end of the 180th day repairs, the electric energy that this soil battery is recovered to altogether is 918C.
3) total petroleum hydrocarbons content of soil adopts gravimetric detemination:
Take the dry soil samples after 6.00g reparation, put into filter paper packet, adopt 125mL carrene rope to carry 24h, rope extract is rotated evaporate to dryness under 0.02Mpa, 37 DEG C ± 1 DEG C condition, calculates the total petroleum hydrocarbons content in soil sample by weight difference.
Adopt this electrochemical appliance remedying oil-polluted soils, the degraded situation of total petroleum hydrocarbon as shown in Figure 4, show in figure: the total petroleum hydrocarbon degradation efficiency of the 4th layer of soil is the highest, be 18.3%, next is the 1st layer of soil 12.5%, is the 2nd layer of soil 9.7% again, is finally the 3rd layer of soil 8.2%, average degradation rate is 12.2%, and control group is only 6.6%.
4) content detection of 16 kinds of polycyclic aromatic hydrocarbons in the soil after repairing:
Above-mentioned 3) in measured total petroleum hydrocarbon after sample in add 5ml n-hexane, then through silica gel alumina composite chromatography column purification, described silica gel alumina composite chromatography column internal diameter 1cm, 1cm anhydrous sodium sulfate from top to bottom, 6cm 2w% deactivates aluminium oxide and 12cm 2w% deactivated silica gel, use 20mL normal hexane, carrene/n-hexane (the 1:1 of 70mL, V/V) mixed liquor drip washing, the former is alkane leacheate, the latter is aromatic hydrocarbons leacheate, component leacheate is concentrated into about 1mL, be transferred to sample bottle, flow down at soft high pure nitrogen and dry up, be 10mL with chromatographically pure n-hexane constant volume, standby GC-MS analyzes.
After adopting this electrochemical appliance remedying oil-polluted soils, the content situation of 16 kinds of polycyclic aromatic hydrocarbons as shown in Figure 5, shows in figure: along with the increase of polycyclic aromatic hydrocarbon number of rings, and its amount be degraded reduces gradually.Naphthalene, acenaphthene and acenaphthene are relatively easily degraded because number of rings is less, so background values is very low in the soil adopted, however, the soil fuel cell of structure still facilitates residual degraded, particularly acenaphthene and acenaphthene, degradation rate is respectively 64.7% and 66.5%.Fluorenes, phenanthrene, anthracene and fluoranthene degradation rate reduce successively gradually, and the degradation rate of fluorenes is the highest, are 15.8%.Pyrene, benzo [a] anthracene, bend and benzo [b] fluoranthene in, benzo [a] anthracene degradation rate is the highest, is 13.7%.[in g, h, i] perylene, benzo [k] fluoranthene degradation rate is the highest, is 15.5% for benzo [k] fluoranthene, benzo [a] pyrene, indeno [1,2,3-cd] pyrene, dibenzo [a, h] anthracene and benzo.
5) alkane (C in the soil after repairing
8-C
40) content and degradation rate detect:
Method is with 4).After adopting this electrochemical appliance remedying oil-polluted soils, alkane (C
8-C
40) degraded situation as shown in Figure 6, show in figure: most high degradation rate is 69.3% (C
13), minimum degradation rate is 17.7% (C
21), total degradation rate is 28.7% (C
8-C
40summation), wherein light oil constituents (C
12-C
23) degradation rate be 24.5%, the degradation rate of heavy oil component is 31.4%.
Claims (1)
1. adopt a method for electrochemical appliance remedying oil-polluted soils synchronous electrogenesis, it is characterized in that step is as follows:
1) assembling of electrochemical appliance
Electrochemical appliance is made up of lucite casing, carbon cloth anode and compound polytetrafluoroethylene (PTFE) (PTFE) air cathode assembly, lucite casing is the cuboid with flange frame bottom upper and lower opening also, bottom half is provided with base plate and is supported by four supporting legs, and the part that base plate connects with air cathode is evenly equipped with that diameter is 0.5cm, pitch of holes is the circular hole of 1cm, carbon cloth anode carbon cloth is placed in acetone to soak 8 hours, cleans 3 times obtain after taking-up with distilled water, compound polytetrafluoroethylene (PTFE) (PTFE) air cathode assembly is by compound polytetrafluoroethylene (PTFE) (PTFE) air cathode and its, the plastic pad combination that bottom is respectively equipped with is formed and is fixed by the bolt of surrounding, on, the square hole size at lower plastic pad center is identical with the lumenal cross-section of lucite casing, wherein compound polytetrafluoroethylene (PTFE) (PTFE) air cathode preparation method is: take conductive carbon black 4g and add in 200mL beaker, add 80mL absolute ethyl alcohol, stir and ultrasonic 5min, add the PTFE emulsion that 6.2mL density is 1.5g/mL, stir and ultrasonic 5min, then 40min is about in 80 DEG C of stirring in water bath, take out micelle gently to rub, it is 0.5mm electrode slice that roll squeezer is rolled into thickness with 60 order stainless (steel) wires, then at 340 DEG C, 25min is heated stand-by, taking electric capacity carbon dust 6g adds in 200mL beaker, add 45mL absolute ethyl alcohol, stir and ultrasonic 5min, add 0.670mL PTFE emulsion, stir again and ultrasonic 5min, be then about 3h in 80 DEG C of stirring in water bath, take out micelle and gently rub, be pressed in the opposite side of electrode slice after being rolled into film, final thickness of electrode is 0.6mm,
2) oil pollution soil is dried in the shade naturally, ground 2mm sieve, after taking 320.00g oil pollution soil powder mixing with 90mL distilled water, be divided into 6 parts, tile 1 part at the 4th layer of soil, 2 parts are tiled at the 3rd layer of soil, tile 2 parts at the 2nd layer of soil, tile 1 part at the 1st layer of soil, soil separates with carbon cloth anode between layers respectively, draw as wire by titanium sheet, three road carbon cloth anodes are converged;
3) with syringe 20mL distilled water injected on the 1st layer of soil and form water seal layer, compound polytetrafluoroethylene (PTFE) (PTFE) air cathode is connected with 1000 Ω external resistances respectively by wire with the carbon cloth anode converged, composition edaphon fuel cell, the voltage in external resistance is by electrochemistry capture card and the automatic record of computer;
4) make above-mentioned edaphon fuel cell run 180d at 30 DEG C under keeping water seal layer condition, complete the reparation of oil-polluted soils and produce electric energy simultaneously.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN105689387A (en) * | 2016-03-30 | 2016-06-22 | 中国石油大学(华东) | Method for restoring combined pollution soil through electrodynamic force-fuel cell coupling device |
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| CN104174646B (en) * | 2014-08-29 | 2017-01-25 | 东南大学 | System for purifying soil with pesticide degradation-resistant organic pollutants |
| CN105280941B (en) * | 2015-09-18 | 2018-01-16 | 南开大学 | A kind of method based on MFC technology in-situ immobilization oil-polluted soils and electricity production |
| CN108817076B (en) * | 2018-06-08 | 2023-05-05 | 广西博世科环保科技股份有限公司 | Method and system for enhanced restoration of petroleum-contaminated soil by using microbial electrochemical respirator |
| CN108996661A (en) * | 2018-08-07 | 2018-12-14 | 南开大学 | A method of improving the degradation property of deposition microbiological fuel cell |
| CN109772874B (en) * | 2018-12-29 | 2022-04-12 | 农业部环境保护科研监测所 | Device and method for recovering electric energy from petroleum hydrocarbon polluted saline-alkali soil and synchronously desalting |
| CN112474773B (en) * | 2020-11-06 | 2022-04-15 | 南开大学 | Device and method for strengthening soil remediation by combining plant microorganism electrochemistry and application |
| CN113578947B (en) * | 2021-07-20 | 2022-10-18 | 大连海事大学 | Bioelectrochemical method for repairing lead-polluted soil |
| CN114518398A (en) * | 2022-02-18 | 2022-05-20 | 南开大学 | Bioelectrochemical sensor and method for detecting oil content of sludge |
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| JP2006339132A (en) * | 2005-06-05 | 2006-12-14 | Toru Ueda | Method and apparatus for restoring electricity using soil fuel cell generation system |
| US7858243B2 (en) * | 2007-03-22 | 2010-12-28 | The University Of Wyoming Research Corporation | Influential fuel cell systems including effective cathodes and use with remediation efforts |
| US9045354B2 (en) * | 2010-09-21 | 2015-06-02 | Advanced Environmental Technologies, Llc | Methods for enhanced oxidative and reductive remediation |
| CN102386431B (en) * | 2011-10-24 | 2012-12-05 | 南开大学 | Soil microbe fuel cell and method for remediating petroleum hydrocarbon polluted soil |
| CN102655235B (en) * | 2012-03-09 | 2014-03-26 | 南开大学 | Microbial fuel cell air cathode and preparation method thereof |
| CN103611723B (en) * | 2013-12-16 | 2015-06-10 | 华北电力大学 | Method and device for restoring petroleum-polluted soil through composting by enhancing microbial fuel cells |
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| CN105689387A (en) * | 2016-03-30 | 2016-06-22 | 中国石油大学(华东) | Method for restoring combined pollution soil through electrodynamic force-fuel cell coupling device |
| CN105689387B (en) * | 2016-03-30 | 2018-08-31 | 中国石油大学(华东) | A kind of method that electric power-fuel cell coupling device repairs combined contamination soil |
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