CN116550739A - Method for restoring petroleum hydrocarbon contaminated soil by adding elemental sulfur and synthesizing pyrite through in-situ microorganisms - Google Patents
Method for restoring petroleum hydrocarbon contaminated soil by adding elemental sulfur and synthesizing pyrite through in-situ microorganisms Download PDFInfo
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- CN116550739A CN116550739A CN202310524417.7A CN202310524417A CN116550739A CN 116550739 A CN116550739 A CN 116550739A CN 202310524417 A CN202310524417 A CN 202310524417A CN 116550739 A CN116550739 A CN 116550739A
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- soil
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- 239000002689 soil Substances 0.000 title claims abstract description 83
- 239000003209 petroleum derivative Substances 0.000 title claims abstract description 33
- 238000000034 method Methods 0.000 title claims abstract description 28
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 title claims abstract description 21
- 238000011065 in-situ storage Methods 0.000 title claims abstract description 14
- 229910052683 pyrite Inorganic materials 0.000 title claims abstract description 14
- NIFIFKQPDTWWGU-UHFFFAOYSA-N pyrite Chemical compound [Fe+2].[S-][S-] NIFIFKQPDTWWGU-UHFFFAOYSA-N 0.000 title claims abstract description 14
- 239000011028 pyrite Substances 0.000 title claims abstract description 14
- 244000005700 microbiome Species 0.000 title claims description 9
- 230000002194 synthesizing effect Effects 0.000 title claims description 6
- 239000003208 petroleum Substances 0.000 claims description 23
- 238000000227 grinding Methods 0.000 claims description 13
- 238000007873 sieving Methods 0.000 claims description 13
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 10
- 239000000843 powder Substances 0.000 claims description 9
- 239000000463 material Substances 0.000 claims description 8
- 238000005067 remediation Methods 0.000 claims description 7
- 238000005303 weighing Methods 0.000 claims description 7
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 6
- 239000010439 graphite Substances 0.000 claims description 6
- 229910002804 graphite Inorganic materials 0.000 claims description 6
- 229910001220 stainless steel Inorganic materials 0.000 claims description 6
- 239000010935 stainless steel Substances 0.000 claims description 6
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 5
- 239000010405 anode material Substances 0.000 claims description 5
- 230000015572 biosynthetic process Effects 0.000 claims description 5
- 239000010406 cathode material Substances 0.000 claims description 5
- 239000000203 mixture Substances 0.000 claims description 5
- 238000003786 synthesis reaction Methods 0.000 claims description 5
- NIXOWILDQLNWCW-UHFFFAOYSA-N acrylic acid group Chemical group C(C=C)(=O)O NIXOWILDQLNWCW-UHFFFAOYSA-N 0.000 claims description 2
- 230000000694 effects Effects 0.000 claims description 2
- 238000012986 modification Methods 0.000 claims description 2
- 230000004048 modification Effects 0.000 claims description 2
- 230000000813 microbial effect Effects 0.000 abstract description 18
- 238000005516 engineering process Methods 0.000 abstract description 10
- 238000002137 ultrasound extraction Methods 0.000 description 6
- 239000010802 sludge Substances 0.000 description 5
- 241000894006 Bacteria Species 0.000 description 4
- 238000002156 mixing Methods 0.000 description 4
- 239000002699 waste material Substances 0.000 description 4
- 230000008569 process Effects 0.000 description 3
- 230000027756 respiratory electron transport chain Effects 0.000 description 3
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 2
- 239000000370 acceptor Substances 0.000 description 2
- 230000015556 catabolic process Effects 0.000 description 2
- 238000010276 construction Methods 0.000 description 2
- 238000006731 degradation reaction Methods 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 238000002149 energy-dispersive X-ray emission spectroscopy Methods 0.000 description 2
- 229910052500 inorganic mineral Inorganic materials 0.000 description 2
- 230000004060 metabolic process Effects 0.000 description 2
- 239000011707 mineral Substances 0.000 description 2
- 230000003014 reinforcing effect Effects 0.000 description 2
- 230000008439 repair process Effects 0.000 description 2
- 230000004888 barrier function Effects 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000004020 conductor Substances 0.000 description 1
- 239000000356 contaminant Substances 0.000 description 1
- 230000002708 enhancing effect Effects 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 125000000524 functional group Chemical group 0.000 description 1
- 230000005251 gamma ray Effects 0.000 description 1
- 238000001727 in vivo Methods 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 239000013049 sediment Substances 0.000 description 1
- 239000010865 sewage Substances 0.000 description 1
- 238000000638 solvent extraction Methods 0.000 description 1
- 239000008223 sterile water Substances 0.000 description 1
- 230000001954 sterilising effect Effects 0.000 description 1
- 238000004659 sterilization and disinfection Methods 0.000 description 1
- 230000004936 stimulating effect Effects 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- 238000005979 thermal decomposition reaction Methods 0.000 description 1
- 238000005406 washing Methods 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
- B09C—RECLAMATION OF CONTAMINATED SOIL
- B09C1/00—Reclamation of contaminated soil
- B09C1/08—Reclamation of contaminated soil chemically
- B09C1/085—Reclamation of contaminated soil chemically electrochemically, e.g. by electrokinetics
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
- B09C—RECLAMATION OF CONTAMINATED SOIL
- B09C1/00—Reclamation of contaminated soil
- B09C1/10—Reclamation of contaminated soil microbiologically, biologically or by using enzymes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
- B09C—RECLAMATION OF CONTAMINATED SOIL
- B09C2101/00—In situ
Landscapes
- Engineering & Computer Science (AREA)
- Life Sciences & Earth Sciences (AREA)
- Environmental & Geological Engineering (AREA)
- Soil Sciences (AREA)
- Health & Medical Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Chemical & Material Sciences (AREA)
- Biomedical Technology (AREA)
- Biotechnology (AREA)
- General Health & Medical Sciences (AREA)
- Microbiology (AREA)
- Molecular Biology (AREA)
- Mycology (AREA)
- Processing Of Solid Wastes (AREA)
Abstract
The invention discloses a method for restoring petroleum hydrocarbon polluted soil by adding elemental sulfur into a soil microbial electrochemical system to synthesize pyrite in situ, which mainly aims at the problems of poor conductivity of soil, limited effective restoration range caused by difficult mass transfer and the like. The method obviously strengthens the restoration of the petroleum hydrocarbon polluted soil, promotes the bio-geochemical circulation, and is a green, safe, low-cost and promising organic polluted soil bioremediation technology.
Description
Technical Field
The invention relates to the field of pollutant remediation, in particular to a method for remedying petroleum hydrocarbon contaminated soil by synthesizing pyrite in situ by microorganisms in a microbial electrochemical system.
Background
Along with the promotion of ecological civilization construction in China, the petroleum industry develops rapidly. In the process of oil and gas exploitation, a large amount of low-concentration oil sludge can be formed, so that serious economic loss is caused for petroleum enterprises, and meanwhile, the problem of soil environmental pollution is increasingly outstanding, and the method has become one of the first ten important industries on the national level. In addition, the oil content in the sludge is high, which is a precious resource in the waste, and if the waste is not recycled, the waste of the material is also large. The treatment methods for the sludge include incineration treatment, solvent extraction, hot water washing treatment, thermal decomposition treatment, biological treatment, and the like. However, these methods have respective drawbacks, such as resource waste, secondary pollution, high treatment cost, and long time consumption, and thus a method for enhancing the treatment of the sludge is needed.
The microbial electrochemical technology is a novel repair technology which occurs in recent years, and the technology is used for completing the electron transfer process of cells by enriching some electroactive microorganisms existing in nature and transferring electrons generated by in vivo substrate metabolism to electron acceptors such as extracellular conductive materials and the like. Unlike conventional bioremediation techniques, it promotes the degradation and removal of organic contaminants by the stimulating action of microbial currents. This technique has been successfully applied to sewage and sediment remediation. Research shows that the soil microbial electrochemical technology is one new kind of in-situ petroleum hydrocarbon polluted soil repairing mode, and it transfers the extracellular electrons produced by the metabolism of electroactive bacteria near the anode to the air cathode via the external circuit to form O together with the anode 2 And H in soil + Reaction to produce H 2 O (for example, an air cathode) and forms a closed loop. This process can be carried out spontaneously (microbial fuel cells) or under external pressure (microbial cells). However, the effective restoration range is limited due to poor conductivity and mass transfer of the soil.
Disclosure of Invention
The invention aims at solving the actual problems, and develops a technology for reinforcing the restoration of petroleum hydrocarbon contaminated soil by adding elemental sulfur microorganism in-situ synthesized pyrite based on the microbial electrochemical principle for treating the low-concentration oil sludge. The method constructs a high-efficiency and low-cost technology for bioelectrochemistry treatment of low-concentration floor oil pollution, and has great application prospects in the aspects of green synthesis of conductive minerals, high-concentration organic load treatment, sustainable biocatalysis and the like.
The invention aims at realizing the following technical scheme: a method for restoring petroleum hydrocarbon contaminated soil by synthesizing pyrite in situ by microorganisms in a soil microbial electrochemical system comprises the following construction steps:
the reactor adopted by the soil microbial electrochemical system is composed of a rectangular chamber made of acrylic materials with the length of 8 cm, the width of 8 cm and the height of 7 cm, a graphite plate with the length of 7 cm, the height of 4 cm and the thickness of 0.2 cm is selected as an anode material, a stainless steel net with the length, the height of 0.3 cm and the thickness of 0.3 cm is selected as a cathode material and is arranged on the opposite side of the chamber in parallel, the distance between the anode and the cathode is 7 cm, and the anode and the cathode are respectively connected by a titanium wire to extend out of 4 cm as a lead. Grinding and sieving the collected petroleum raw soil, adding sublimed sulfur powder (3 g/kg of petroleum raw soil) after grinding and sieving to uniformly mix the petroleum raw soil, weighing 250 g, uniformly paving the mixed soil in a chamber, and keeping the anaerobic environment of a soil system at the upper layer by adopting a water seal 2-3 cm mode. A potentiostat with real-time current acquisition function developed in the laboratory was used to apply a voltage of 1.2V between the anode and cathode while acquiring a varying current signal. All reactors were run in a light-protected greenhouse at 25±1 ℃.
Advantageous effects
The application of the existing soil microbial electrochemical technology is generally limited by poor conductivity, difficult mass transfer, small effective restoration range and the like of the soil. The invention provides a method for reinforcing soil remediation by adding elemental sulfur powder into a microbial electrochemical system to synthesize pyrite in situ, which utilizes abundant electroactive bacteria, iron-reducing bacteria, elemental sulfur-reducing bacteria and petroleum hydrocarbon degradation functional groups in petroleum soil, firstly takes iron oxide with abundant content in the soil and artificially scattered sulfur powder as electron acceptors, and petroleum hydrocarbon as an electron donor to form a large number of mutually interweaved pyrite conductive networks, so that microorganisms far from electrodes are tightly aggregated, close-range electron transfer and long-range indirect electron transfer among microorganisms are accelerated, the barrier of excessive medium resistance in the soil is eliminated, the conductivity of the soil is greatly improved, the advantages of microbial electrochemical technology are combined, the petroleum hydrocarbon degradation-after 2 months-total petroleum hydrocarbon removal rate is up to 62%, the repair of petroleum hydrocarbon polluted soil is remarkably enhanced, and the bio-earth chemical circulation is promoted. In addition, the sulfur powder is cheap and easy to obtain, which is clearly a green, safe, low-cost and promising bioremediation technology for organic contaminated soil.
Drawings
FIG. 1 is a schematic diagram of a soil microbial electrochemical system: 1, a computer; 2, a constant potential rectifier for power supply and data acquisition; 3, a soil reactor; 4, stainless steel mesh cathode; 5 graphite plate anode; 6 petroleum soil layer; 7 water seal layer
FIG. 2 time-current diagram collected in the soil microbial electrochemical system of the present invention
FIG. 3 field emission electron scanning microscope (SEM) image of a black material of the sulphurized group
Removal of Total Petroleum Hydrocarbon (TPH) from soil within 60 days of each group of FIG. 4
Detailed Description
The invention is further described below with reference to the drawings and specific examples.
Example 1
The total petroleum hydrocarbon content in the petroleum raw soil is determined by using an ultrasonic extraction method.
Example 2
The soil microbial electrochemical system shown in fig. 1 is adopted, a graphite plate 5 with the length of 7 cm, the height of 4 cm and the thickness of 0.2 cm is selected as an anode material, a stainless steel net 4 with the length, the height of 0.3 cm and the thickness of 0.3 is selected as a cathode material and is arranged on the opposite side of the cavity in parallel, the distance between the anode and the cathode is 7 cm, and the anode and the cathode are respectively connected by a titanium wire and extend out of 4 cm to serve as leads. Grinding and sieving the collected petroleum raw soil, adding sublimed sulfur powder (3-g/kg of petroleum raw soil) after grinding and sieving to uniformly mix the petroleum raw soil, weighing the soil 6 after mixing 250-g, uniformly paving the soil in a chamber, and keeping the anaerobic environment of a soil system at the upper layer by adopting a water seal mode of 2-3 cm. A potentiostat 2 developed in the laboratory with a real-time current acquisition function was used to apply a voltage of 1.2V between the anode and cathode, while a varying current signal was acquired using a computer 1 as shown in fig. 2 oil-BES-S. All reactors were run in a light-protected greenhouse at 25±1 ℃. After 60 days, the total petroleum hydrocarbon content remained in the soil was measured by using an ultrasonic extraction method, and the total petroleum hydrocarbon removal rate was calculated to be 62% (fig. 4); and samples were taken and observed for the morphology of the black material using a field electron scanning microscope, the observed black material was found to consist of a regular needle-like mineral structure (fig. 3), while the black material was found to be FeS using energy dispersive X-ray spectroscopy (EDS) to observe the elemental composition (C: S: fe=43%: 29%: 28%) and calculating the ratio thereof.
Example 3
The soil microbial electrochemical system shown in fig. 1 is adopted, a graphite plate 5 with the length of 7 cm, the height of 4 cm and the thickness of 0.2 cm is selected as an anode material, a stainless steel net 4 with the length, the height of 0.3 cm and the thickness of 0.3 is selected as a cathode material and is arranged on the opposite side of the cavity in parallel, the distance between the anode and the cathode is 7 cm, and the anode and the cathode are respectively connected by a titanium wire and extend out of 4 cm to serve as leads. Grinding and sieving the collected petroleum raw soil, then carrying out gamma-ray irradiation sterilization, adding sublimated sulfur powder (3-g/kg of petroleum raw soil) after grinding and sieving, uniformly mixing, weighing the sterilized soil after mixing 250-g, uniformly paving the sterilized soil in a cavity, and injecting sterile water into the upper layer for 2-3 cm to maintain the anaerobic environment of a soil system. A potentiostat 2 developed in the laboratory with a real-time current acquisition function was used to apply a voltage of 1.2V between the anode and cathode while the computer 1 was used to acquire the varying current signal as shown in fig. 2 sterileSoil-BES-S. All reactors were run in a light-protected greenhouse at 25±1 ℃. The total petroleum hydrocarbon content remaining in the soil was measured after 60 days using ultrasonic extraction with little change (fig. 4).
Example 4
The soil microbial electrochemical system shown in fig. 1 is adopted, a graphite plate 5 with the length of 7 cm, the height of 4 cm and the thickness of 0.2 cm is selected as an anode material, a stainless steel net 4 with the length, the height of 0.3 cm and the thickness of 0.3 is selected as a cathode material and is arranged on the opposite side of the cavity in parallel, the distance between the anode and the cathode is 7 cm, and the anode and the cathode are respectively connected by a titanium wire and extend out of 4 cm to serve as leads. Weighing up to 250-g, uniformly paving the petroleum raw soil after grinding and sieving in a cavity, and keeping the anaerobic environment of a soil system on the upper layer by adopting a water seal mode of 2-3 cm. A potentiostat 2 developed in the laboratory with a real-time current acquisition function was used to apply a voltage of 1.2V between the anode and cathode, while a computer 1 was used to acquire the varying current signal as shown in fig. 2 oil-BES-CK. All reactors were run in a light-protected greenhouse at 25±1 ℃. After 60 days, the total petroleum hydrocarbon content remaining in the soil was measured using ultrasonic extraction, and the total petroleum hydrocarbon removal rate was calculated to be 27% (fig. 4). No blackening of the soil was observed in this group of reactors.
Example 5
After grinding and sieving the collected petroleum raw soil by adopting a reactor 3 shown in fig. 1, adding sublimed sulfur powder (3-g/kg petroleum raw soil) after grinding and sieving to uniformly mix the petroleum raw soil, then weighing the soil 6 after mixing 250-g, uniformly paving the soil in a chamber, and keeping the anaerobic environment of a soil system at the upper layer by adopting a water seal mode 2-3 cm. All reactors were run in a light-protected greenhouse at 25.+ -. 1 ℃ and designated as soil-S. After 60 days, the total petroleum hydrocarbon content remaining in the soil was measured using an ultrasonic extraction method, and the total petroleum hydrocarbon removal rate was calculated to be 20% (fig. 4). The set of reactors observed soil darkening.
Example 6
The reactor 3 shown in fig. 1 is adopted, petroleum raw soil after weighing to 250 and g, grinding and sieving is evenly paved in a cavity, and the upper layer is used for keeping the anaerobic environment of a soil system in a water seal mode of 2-3 cm and is marked as soil-CK. All reactors were run in a light-protected greenhouse at 25±1 ℃. After 60 days, the total petroleum hydrocarbon content remaining in the soil was measured using an ultrasonic extraction method, and the total petroleum hydrocarbon removal rate was calculated to be 0.2% (fig. 4). No blackening of the soil was observed in this group of reactors.
The above-described embodiments are preferred modes of the present invention, and it should be noted that all modifications and improvements made without departing from the principle of the present invention fall within the scope of the protection of the present invention.
Claims (7)
1. The method for synthesizing pyrite by in-situ microorganisms by adding elemental sulfur for repairing petroleum hydrocarbon contaminated soil is characterized by comprising the following steps of:
the reactor is composed of a rectangular cavity made of acrylic material with the length of 8 cm, the width of 8 cm and the height of 7 cm, a graphite plate with the length of 7 cm, the height of 4 cm and the thickness of 0.2 cm is selected as an anode material, a stainless steel net with the length, the height of 0.3 cm and the thickness of the same size as that of the anode is selected as a cathode material and is arranged on the opposite side of the cavity in parallel, the distance between the anode and the cathode is 7 cm, and the anode and the cathode are respectively connected by a titanium wire to extend out 4 cm as a lead.
2. Grinding and sieving the collected petroleum raw soil, adding sublimed sulfur powder (3 g/kg of petroleum raw soil) after grinding and sieving to uniformly mix the petroleum raw soil, then weighing 150 g, uniformly paving the mixed soil in a chamber, and keeping the anaerobic environment of a soil system at the upper layer by adopting a water seal 2-3 cm mode. A potentiostat with real-time current acquisition function developed in the laboratory was used to apply a voltage of 1.2V between the anode and cathode while acquiring a varying current signal. All reactors were run in a light-protected greenhouse at 25±1 ℃.
3. The method for in-situ synthesis of pyrite by adding elemental sulfur for remediation of petroleum hydrocarbon contaminated soil according to claim 1, wherein the petroleum raw soil after grinding and sieving is uniformly mixed with sublimed sulfur powder.
4. The method for in-situ synthesis of pyrite by adding elemental sulfur for petroleum hydrocarbon contaminated soil remediation according to claim 1, wherein the upper layer maintains the anaerobic environment of the soil system by means of water seals 2-3 cm.
5. The method for in-situ synthesis of pyrite with addition of elemental sulfur for remediation of petroleum hydrocarbon contaminated soil according to claim 1, wherein a voltage of 1.2V is applied between the anode and the cathode, which is 42% higher than the total petroleum hydrocarbon removal rate when only sublimated elemental sulfur powder is added without applying the voltage.
6. The method for in-situ synthesis of pyrite by adding elemental sulfur for remediation of petroleum hydrocarbon contaminated soil according to claim 1, wherein the content of sublimed sulfur powder added by the method is not limited to 3 g/kg of petroleum original soil, and the amount of sublimed sulfur powder added can be optimized for different concentrations of petroleum hydrocarbon so as to obtain better petroleum hydrocarbon removal effect.
7. The method for restoring petroleum hydrocarbon contaminated soil by in-situ synthesizing pyrite according to claim 1, wherein the used reactor is not limited to the above-mentioned size and material, and all modifications and finishes made without departing from the principle of the invention are included in the scope of the protection of the invention.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202310524417.7A CN116550739A (en) | 2023-05-11 | 2023-05-11 | Method for restoring petroleum hydrocarbon contaminated soil by adding elemental sulfur and synthesizing pyrite through in-situ microorganisms |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202310524417.7A CN116550739A (en) | 2023-05-11 | 2023-05-11 | Method for restoring petroleum hydrocarbon contaminated soil by adding elemental sulfur and synthesizing pyrite through in-situ microorganisms |
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| Publication Number | Publication Date |
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| CN116550739A true CN116550739A (en) | 2023-08-08 |
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| Application Number | Title | Priority Date | Filing Date |
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| CN202310524417.7A Pending CN116550739A (en) | 2023-05-11 | 2023-05-11 | Method for restoring petroleum hydrocarbon contaminated soil by adding elemental sulfur and synthesizing pyrite through in-situ microorganisms |
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| CN (1) | CN116550739A (en) |
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2023
- 2023-05-11 CN CN202310524417.7A patent/CN116550739A/en active Pending
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